text:
# The 𝑄²-dependence of the Generalised Gerasimov-Drell-Hearn Integral for the Proton

(August 17, 2000)

## Abstract

The dependence on $`Q^2`$ (the negative square of the 4-momentum of the exchanged virtual photon) of the generalised Gerasimov-Drell-Hearn integral for the proton has been measured in the range 1.2 GeV$`{}_{}{}^{2}<Q^2<12`$ GeV2 by scattering longitudinally polarised positrons on a longitudinally polarised hydrogen gas target. The contributions of the nucleon-resonance and deep-inelastic regions to this integral have been evaluated separately. The latter has been found to dominate for $`Q^2>3`$ GeV2, while both contributions are important at low $`Q^2`$. The total integral shows no significant deviation from a 1/$`Q^2`$ behaviour in the measured $`Q^2`$ range, and thus no sign of large effects due to either nucleon-resonance excitations or non-leading twist.

HERMES Collaboration

A. Airapetian$`^{\text{ ae}}`$, N. Akopov$`^{\text{ ae}}`$, I. Akushevich$`^{\text{ g}}`$, M. Amarian$`^{\text{ w,z,ae}}`$, J. Arrington$`^{\text{ b}}`$, E.C. Aschenauer$`^{\text{ g,m,w}}`$, H. Avakian$`^{\text{ k}}`$, R. Avakian$`^{\text{ ae}}`$, A. Avetissian$`^{\text{ ae}}`$, E. Avetissian$`^{\text{ ae}}`$, P. Bailey$`^{\text{ o}}`$, B. Bains$`^{\text{ o}}`$, C. Baumgarten$`^{\text{ u}}`$, M. Beckmann$`^{\text{ l}}`$, S. Belostotski$`^{\text{ x}}`$, S. Bernreuther$`^{\text{ i}}`$, N. Bianchi$`^{\text{ k}}`$, H. Böttcher$`^{\text{ g}}`$, A. Borissov$`^{\text{ f,n}}`$, M. Bouwhuis$`^{\text{ o}}`$, J. Brack$`^{\text{ e}}`$, S. Brauksiepe$`^{\text{ l}}`$, B. Braun$`^{\text{ i,u}}`$, W. Brückner$`^{\text{ n}}`$, A. Brüll$`^{\text{ n,r}}`$, P. Budz$`^{\text{ i}}`$, H.J. Bulten$`^{\text{ q,w,ad}}`$, G.P. Capitani$`^{\text{ k}}`$, P. Carter$`^{\text{ d}}`$, P. Chumney$`^{\text{ v}}`$, E. Cisbani$`^{\text{ z}}`$, G.R. Court$`^{\text{ p}}`$, P.F. Dalpiaz$`^{\text{ j}}`$, R. De Leo$`^{\text{ c}}`$, L. De Nardo$`^{\text{ a}}`$, E. De Sanctis$`^{\text{ k}}`$, D. De Schepper$`^{\text{ b,r}}`$, E. Devitsin$`^{\text{ t}}`$, P.K.A. de Witt Huberts$`^{\text{ w}}`$, P. Di Nezza$`^{\text{ k}}`$, V. Djordjadze$`^{\text{ g}}`$, M. Düren$`^{\text{ i}}`$, A. Dvoredsky$`^{\text{ d}}`$, G. Elbakian$`^{\text{ ae}}`$, J. Ely$`^{\text{ e}}`$, A. Fantoni$`^{\text{ k}}`$, A. Fechtchenko$`^{\text{ h}}`$, M. Ferro-Luzzi$`^{\text{ w,ad}}`$, K. Fiedler$`^{\text{ i}}`$, B.W. Filippone$`^{\text{ d}}`$, H. Fischer$`^{\text{ l}}`$, B. Fox$`^{\text{ e}}`$, J. Franz$`^{\text{ l}}`$, S. Frullani$`^{\text{ z}}`$, Y. Gärber$`^{\text{ g}}`$, F. Garibaldi$`^{\text{ z}}`$, E. Garutti$`^{\text{ w}}`$, G. Gavrilov$`^{\text{ x}}`$, V. Gharibyan$`^{\text{ ae}}`$, A. Golendukhin$`^{\text{ f,u,ae}}`$, G. Graw$`^{\text{ u}}`$, O. Grebeniouk$`^{\text{ x}}`$, P.W. Green$`^{\text{ a,ab}}`$, L.G. Greeniaus$`^{\text{ a,ab}}`$, A. Gute$`^{\text{ i}}`$, W. Haeberli$`^{\text{ q}}`$, M. Hartig$`^{\text{ ab}}`$, D. Hasch$`^{\text{ g,k}}`$, D. Heesbeen$`^{\text{ w}}`$, F.H. Heinsius$`^{\text{ l}}`$, M. Henoch$`^{\text{ i}}`$, R. Hertenberger$`^{\text{ u}}`$, W.H.A. Hesselink$`^{\text{ w,ad}}`$, P. Hoffmann-Rothe$`^{\text{ w}}`$, G. Hofman$`^{\text{ e}}`$, Y. Holler$`^{\text{ f}}`$, R.J. Holt$`^{\text{ o}}`$, B. Hommez$`^{\text{ m}}`$, G. Iarygin$`^{\text{ h}}`$, M. Iodice$`^{\text{ z}}`$, A. Izotov$`^{\text{ x}}`$, H.E. Jackson$`^{\text{ b}}`$, A. Jgoun$`^{\text{ x}}`$, P. Jung$`^{\text{ g}}`$, R. Kaiser$`^{\text{ g,aa,ab}}`$, J. Kanesaka$`^{\text{ ac}}`$, E. Kinney$`^{\text{ e}}`$, A. Kisselev$`^{\text{ x}}`$, P. Kitching$`^{\text{ a}}`$, H. Kobayashi$`^{\text{ ac}}`$, N. Koch$`^{\text{ i}}`$, K. Königsmann$`^{\text{ l}}`$, H. Kolster$`^{\text{ u,w}}`$, V. Korotkov$`^{\text{ g}}`$, E. Kotik$`^{\text{ a}}`$, V. Kozlov$`^{\text{ t}}`$, V.G. Krivokhijine$`^{\text{ h}}`$, G. Kyle$`^{\text{ v}}`$, L. Lagamba$`^{\text{ c}}`$, A. Laziev$`^{\text{ w,ad}}`$, P. Lenisa$`^{\text{ j}}`$, T. Lindemann$`^{\text{ f}}`$, W. Lorenzon$`^{\text{ s}}`$, N.C.R. Makins$`^{\text{ b,o}}`$, J.W. Martin$`^{\text{ r}}`$, H. Marukyan$`^{\text{ ae}}`$, F. Masoli$`^{\text{ j}}`$, M. McAndrew$`^{\text{ p}}`$, K. McIlhany$`^{\text{ d,r}}`$, R.D. McKeown$`^{\text{ d}}`$, F. Menden$`^{\text{ l,ab}}`$, A. Metz$`^{\text{ u}}`$, N. Meyners$`^{\text{ f}}`$, O. Mikloukho$`^{\text{ x}}`$, C.A. Miller$`^{\text{ a,ab}}`$, R. Milner$`^{\text{ r}}`$, V. Mitsyn$`^{\text{ h}}`$, V. Muccifora$`^{\text{ k}}`$, R. Mussa$`^{\text{ j}}`$, A. Nagaitsev$`^{\text{ h}}`$, E. Nappi$`^{\text{ c}}`$, Y. Naryshkin$`^{\text{ x}}`$, A. Nass$`^{\text{ i}}`$, K. Negodaeva$`^{\text{ g}}`$, W.-D. Nowak$`^{\text{ g}}`$, T.G. O’Neill$`^{\text{ b}}`$, R. Openshaw$`^{\text{ ab}}`$, J. Ouyang$`^{\text{ ab}}`$, B.R. Owen$`^{\text{ o}}`$, S.F. Pate$`^{\text{ r,v}}`$, S. Potashov$`^{\text{ t}}`$, D.H. Potterveld$`^{\text{ b}}`$, G. Rakness$`^{\text{ e}}`$, V. Rappoport$`^{\text{ x}}`$, R. Redwine$`^{\text{ r}}`$, D. Reggiani$`^{\text{ j}}`$, A.R. Reolon$`^{\text{ k}}`$, R. Ristinen$`^{\text{ e}}`$, K. Rith$`^{\text{ i}}`$, D. Robinson$`^{\text{ o}}`$, M. Ruh$`^{\text{ l}}`$, D. Ryckbosch$`^{\text{ m}}`$, Y. Sakemi$`^{\text{ ac}}`$, I. Savin$`^{\text{ h}}`$, C. Scarlett$`^{\text{ s}}`$, A. Schäfer$`^{\text{ y}}`$, C. Schill$`^{\text{ l}}`$, F. Schmidt$`^{\text{ i}}`$, G. Schnell$`^{\text{ v}}`$, K.P. Schüler$`^{\text{ f}}`$, A. Schwind$`^{\text{ g}}`$, J. Seibert$`^{\text{ l}}`$, B. Seitz$`^{\text{ a}}`$ T.-A. Shibata$`^{\text{ ac}}`$, T. Shin$`^{\text{ r}}`$, V. Shutov$`^{\text{ h}}`$, C. Simani$`^{\text{ j,w,ad}}`$, A. Simon$`^{\text{ l,v}}`$, K. Sinram$`^{\text{ f}}`$, E. Steffens$`^{\text{ i}}`$, J.J.M. Steijger$`^{\text{ w}}`$, J. Stewart$`^{\text{ p,ab}}`$, U. Stösslein$`^{\text{ g}}`$, K. Suetsugu$`^{\text{ ac}}`$, M. Sutter$`^{\text{ r}}`$, H. Tallini$`^{\text{ p}}`$, S. Taroian$`^{\text{ ae}}`$, A. Terkulov$`^{\text{ t}}`$, S. Tessarin$`^{\text{ j}}`$, E. Thomas$`^{\text{ k}}`$, B. Tipton$`^{\text{ d,r}}`$, M. Tytgat$`^{\text{ m}}`$, G.M. Urciuoli$`^{\text{ z}}`$, J.F.J. van den Brand$`^{\text{ w,ad}}`$, G. van der Steenhoven$`^{\text{ w}}`$, R. van de Vyver$`^{\text{ m}}`$, J.J. van Hunen$`^{\text{ w}}`$, M.C. Vetterli$`^{\text{ aa,ab}}`$, V. Vikhrov$`^{\text{ x}}`$, M.G. Vincter$`^{\text{ a,ab}}`$, J. Visser$`^{\text{ w}}`$, E. Volk$`^{\text{ n}}`$, C. Weiskopf$`^{\text{ i}}`$, J. Wendland$`^{\text{ aa,ab}}`$, J. Wilbert$`^{\text{ i}}`$, T. Wise$`^{\text{ q}}`$, S. Yen$`^{\text{ ab}}`$, S. Yoneyama$`^{\text{ ac}}`$, H. Zohrabian$`^{\text{ ae}}`$

$`^\text{a}`$Department of Physics, University of Alberta, Edmonton, Alberta T6G 2J1, Canada
$`^{\text{ b}}`$Physics Division, Argonne National Laboratory, Argonne, Illinois 60439-4843, USA
$`^{\text{ c}}`$Istituto Nazionale di Fisica Nucleare, Sezione di Bari, 70124 Bari, Italy
$`^{\text{ d}}`$W.K. Kellogg Radiation Laboratory, California Institute of Technology, Pasadena, California 91125, USA
$`^{\text{ e}}`$Nuclear Physics Laboratory, University of Colorado, Boulder, Colorado 80309-0446, USA
$`^{\text{ f}}`$DESY, Deutsches Elektronen Synchrotron, 22603 Hamburg, Germany
$`^{\text{ g}}`$DESY Zeuthen, 15738 Zeuthen, Germany
$`^{\text{ h}}`$Joint Institute for Nuclear Research, 141980 Dubna, Russia
$`^{\text{ i}}`$Physikalisches Institut, Universität Erlangen-Nürnberg, 91058 Erlangen, Germany
$`^{\text{ j}}`$Istituto Nazionale di Fisica Nucleare, Sezione di Ferrara and Dipartimento di Fisica, Università di Ferrara, 44100 Ferrara, Italy
$`^{\text{ k}}`$Istituto Nazionale di Fisica Nucleare, Laboratori Nazionali di Frascati, 00044 Frascati, Italy
$`^{\text{ l}}`$Fakultät für Physik, Universität Freiburg, 79104 Freiburg, Germany
$`^{\text{ m}}`$Department of Subatomic and Radiation Physics, University of Gent, 9000 Gent, Belgium
$`^{\text{ n}}`$Max-Planck-Institut für Kernphysik, 69029 Heidelberg, Germany
$`^{\text{ o}}`$Department of Physics, University of Illinois, Urbana, Illinois 61801, USA
$`^{\text{ p}}`$Physics Department, University of Liverpool, Liverpool L69 7ZE, United Kingdom
$`^{\text{ q}}`$Department of Physics, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA
$`^{\text{ r}}`$Laboratory for Nuclear Science, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA
$`^{\text{ s}}`$Randall Laboratory of Physics, University of Michigan, Ann Arbor, Michigan 48109-1120, USA
$`^{\text{ t}}`$Lebedev Physical Institute, 117924 Moscow, Russia
$`^{\text{ u}}`$Sektion Physik, Universität München, 85748 Garching, Germany
$`^{\text{ v}}`$Department of Physics, New Mexico State University, Las Cruces, New Mexico 88003, USA
$`^{\text{ w}}`$Nationaal Instituut voor Kernfysica en Hoge-Energiefysica (NIKHEF), 1009 DB Amsterdam, The Netherlands
$`^{\text{ x}}`$Petersburg Nuclear Physics Institute, St. Petersburg, Gatchina, 188350 Russia
$`^{\text{ y}}`$Institut für Theoretische Physik, Universität Regensburg, 93040 Regensburg, Germany
$`^{\text{ z}}`$Istituto Nazionale di Fisica Nucleare, Sezione Sanità and Physics Laboratory, Istituto Superiore di Sanità, 00161 Roma, Italy
$`^{\text{ aa}}`$Department of Physics, Simon Fraser University, Burnaby, British Columbia V5A 1S6, Canada
$`^{\text{ ab}}`$TRIUMF, Vancouver, British Columbia V6T 2A3, Canada
$`^{\text{ ac}}`$Department of Physics, Tokyo Institute of Technology, Tokyo 152, Japan
$`^{\text{ ad}}`$Department of Physics and Astronomy, Vrije Universiteit, 1081 HV Amsterdam, The Netherlands
$`^{\text{ ae}}`$Yerevan Physics Institute, 375036, Yerevan, Armenia

The Gerasimov-Drell-Hearn (GDH) sum rule  relates the anomalous contribution $`\kappa `$ in the nucleon magnetic moment to an energy-weighted integral of the difference of the nucleon’s total spin-dependent photoabsorption cross sections:

$$_{\nu _0}^{\mathrm{}}[\sigma _{\frac{1}{2}}(\nu )\sigma _{\frac{3}{2}}(\nu )]\frac{d\nu }{\nu }=\frac{2\pi ^2\alpha }{M^2}\kappa ^2,$$
(1)
where $`\sigma _{\frac{1}{2}(\frac{3}{2})}`$ is the photoabsorption cross section for total helicity of the photon-nucleon system equal to $`\frac{1}{2}`$ ($`\frac{3}{2}`$), $`\nu `$ is the photon energy in the target rest frame, $`\nu _0`$ is the pion production threshold and $`M`$ is the nucleon mass. For the proton ($`\kappa _\mathrm{p}=+1.79`$) the GDH sum rule prediction is $`204\mu `$b. The importance of this sum rule is due to the fact that it is based mostly on very general principles of causality, unitarity, crossing symmetry, and Lorentz and gauge invariance. It has never been directly tested, due to the need for a circularly polarised beam with a longitudinally polarised target, and a wide range of photon energies that has to be covered. There are available several predictions for the contribution of nucleon resonance excitation to the GDH integral , derived from multipole analyses of data for unpolarised single-pion photoproduction, and a prediction for the contribution of high energy multi-hadron production , based on a multiple-Reggeon exchange analysis of deep-inelastic asymmetries. The estimate from multipole analysis was confirmed by preliminary results from the GDH experiment at Mainz , which covered the photon energy range from 200 MeV up to 800 MeV.

The GDH integral can be generalised to the case of absorption of polarised transverse virtual photons with squared four-momentum $`Q^2`$ :

$`I_{GDH}(Q^2){\displaystyle _{\nu _0}^{\mathrm{}}}[\sigma _{\frac{1}{2}}(\nu ,Q^2)\sigma _{\frac{3}{2}}(\nu ,Q^2)]{\displaystyle \frac{d\nu }{\nu }}`$ (2)
$`=16\pi ^2\alpha {\displaystyle _0^{x_0}}{\displaystyle \frac{g_1(x,Q^2)\gamma ^2g_2(x,Q^2)}{Q^2\sqrt{1+\gamma ^2}}}𝑑x`$ (3)
$`={\displaystyle \frac{8\pi ^2\alpha }{M}}{\displaystyle _0^{x_0}}{\displaystyle \frac{A_1(x,Q^2)F_1(x,Q^2)}{K}}{\displaystyle \frac{dx}{x}},`$ (4)
where $`g_1`$ and $`g_2`$ are the polarised structure functions of the nucleon, $`\gamma ^2=Q^2/\nu ^2=(2Mx)^2/Q^2`$, $`x=Q^2/2M\nu `$ and $`x_0=Q^2/2M\nu _0`$. The quantity $`A_1`$ is the longitudinal asymmetry for virtual photoabsorption, while $`F_1`$ is the unpolarised structure function of the nucleon. The Gilman notation  for the virtual photon flux factor $`K=\nu \sqrt{1+\gamma ^2}`$ has been used. It should be noted that elastic scattering occurring at $`x=1`$ does not contribute to the generalised integral. Other generalisations of the GDH integral also have been considered . They differ from the definition given in Eq. 2 by terms in the integral that are proportional to $`\gamma ^2`$ and which therefore vanish in both the real-photon ($`Q^2`$ = 0) and the deep-inelastic ($`Q^21`$ GeV2 and $`\gamma ^20`$) limits. Since $`\gamma ^2`$ is not small in the nucleon-resonance region and at moderate $`Q^2`$ (e.g. $`\gamma ^2`$ is larger than unity for the $`P_{33}(1232)`$-resonance for 0.2 GeV$`{}_{}{}^{2}<Q^2<2`$ GeV2), these generalisations are equivalent for finite values of $`Q^2`$ only if the contributions of the nucleon-resonance excitations are small.

The generalisation of the GDH integral to non-zero photon virtuality $`Q^2`$ provides a way to study the transition from polarised lepton scattering from the nucleon, which is dominated by deep-inelastic scattering (DIS) at large photon-nucleon centre of mass energy $`W=\sqrt{M^2+2M\nu Q^2}`$, to the polarised real photon absorption on the nucleon, which is dominated by nucleon-resonance excitation at low $`W`$. In leading twist (e.g. for $`Q^2\mathrm{}`$), Eq. 3 simplifies: the elastic contribution excluded from the integral is of higher twist, the factor $`1/\sqrt{1+\gamma ^2}`$ is 1+$`𝒪(1/Q^2)`$, and in leading twist approximation it is generally believed (though not formally proven) that the Burkhardt-Cottingham sum rule $`_0^1g_2(x,Q^2)𝑑x=0`$ holds. This leads to:

$$I_{GDH}(Q^2)_{\gamma ^20}=\frac{16\pi ^2\alpha }{Q^2}\mathrm{\Gamma }_1,$$
(5)
where $`\mathrm{\Gamma }_1_0^1g_1(x)𝑑x`$ is predicted to have only the weak $`Q^2`$-dependence due to QCD evolution. As $`Q^20`$, $`I_{GDH}(Q^2)`$ must change sign in order to reach the negative value predicted by the GDH sum rule at $`Q^2=0`$.

Several phenomenological models have been proposed to describe the dependence of the generalised GDH integral on $`Q^2`$ . Some of these models predict large effects from nucleon-resonance excitation  or from higher twist , even for $`Q^2`$ up to a few GeV2. Other models based on chiral perturbation theory have been proposed but their application is limited to $`Q^21`$ GeV2 .

The contribution of the region $`W^23.24`$ GeV2 to the GDH integral defined in Eq. 2 was recently measured  for the proton and the neutron in the range 0.8 GeV$`{}_{}{}^{2}Q^212`$ GeV2, showing that higher-twist effects do not appear to be significant in the measured region. This paper presents a measurement of the contribution of the resonance region to the GDH integral for the proton in a similar $`Q^2`$-range (1.2 GeV$`{}_{}{}^{2}Q^212`$ GeV2). In combination with the analysis at higher $`W^2`$, this provides the first experimental determination of essentially the complete GDH integral for the proton over a range of $`Q^2`$ values.

The measurement was performed in 1997 with a 27.56 GeV beam of longitudinally polarised positrons incident on a longitudinally polarised 1H gas target internal to the HERA storage ring at DESY. The beam polarisation was measured continuously using Compton backscattering of circularly polarised laser light . The average beam polarisation for the analysed data was $`0.55`$.

The HERMES polarised target  consists of polarised atomic 1H gas confined in a storage cell, which is a 40 cm long open-ended thin-walled elliptical tube located on the beam axis inside the HERA vacuum pipe. It is fed by an atomic-beam source of nuclear-polarised hydrogen based on Stern-Gerlach separation . It provides an areal target density of about $`7\times 10^{13}`$ atoms/cm2. The nuclear polarisation of atoms and the atomic fraction are continuously measured with a Breit-Rabi polarimeter and a target gas analyser . The average value of the target polarisation for the analysed data was $`0.88`$ . The fractional systematic uncertainties of the beam and target polarisations were 3.4% and 4.5%, respectively. The integrated luminosity for this data set was 70 pb-1.

Scattered positrons were detected by the HERMES forward spectrometer, which is described in detail elsewhere . The kinematic requirements on the scattered positrons for the analysis in the nucleon-resonance region were: 1 GeV$`{}_{}{}^{2}<W^2<4.2`$ GeV2, 1.2 GeV$`{}_{}{}^{2}<Q^2<12`$ GeV2. After applying data quality criteria, about 0.13 million events were selected.

For all detected positrons the angular resolution was better than 0.6 mrad, the momentum resolution was better than 1.6% aside from bremsstrahlung tails and the $`Q^2`$-resolution was better than 2.2%. The limited $`W^2`$-resolution (about 840 MeV2, or $`\mathrm{\Delta }W`$ 240 MeV) in the resonance region did not allow the contributions of the individual nucleon resonances to be distinguished. To evaluate the smearing corrections and the contaminations intruding into the resonance region from the elastic and deep-inelastic regions, events were simulated using a Monte-Carlo code that includes elastic, deep-inelastic and resonance contributions. The description of the resonance contribution was based on the model of Ref. . The deep-inelastic region was modelled using the parameterisation of Ref.  while the elastic form factors were taken from Ref. . In Fig. 1 the distribution of events as a function of $`W^2`$ is presented in comparison with the simulation. It is apparent that the shape of the simulated distribution agrees well with that of the data. It was found that the relative contaminations from the elastic and DIS regions in the yield of the resonance region range from 10% to 2% and from 7% to 16% respectively, as $`Q^2`$ increases from 1.2 GeV2 up to 12 GeV2.

Data were divided into six bins in $`Q^2`$, but only one bin in $`W^2`$. In each $`Q^2`$-bin the average longitudinal asymmetry $`A_1`$ for virtual photoabsorption was calculated using the formula

$$A_1=\frac{A_{}}{D}\eta A_2,$$
(6)
where $`D`$ and $`\eta `$ are factors  that depend on kinematic variables. The quantity $`D`$ depends also on $`R=\sigma _L/\sigma _T`$, the ratio of the absorption cross sections for longitudinal and transverse virtual photons. $`A_2`$ is related to longitudinal-transverse interference. The cross section asymmetry $`A_{}`$ is given by :

$$A_{}=\frac{N^{\stackrel{}{}}L^{\stackrel{}{}}N^{\stackrel{}{}}L^{\stackrel{}{}}}{N^{\stackrel{}{}}L_P^{\stackrel{}{}}+N^{\stackrel{}{}}L_P^{\stackrel{}{}}}.$$
(7)
Here, $`N^{\stackrel{}{}}`$($`N^{\stackrel{}{}}`$) is the number of scattered positrons for target spin parallel (anti-parallel) to the beam spin orientation. The deadtime-corrected luminosities for each target spin state are $`L^{\stackrel{}{}(\stackrel{}{})}`$ and $`L_P^{\stackrel{}{}(\stackrel{}{})}`$, the latter being weighted by the product of beam and target polarisations. The cross section asymmetry $`A_{}^{res}`$ in the resonance region was corrected for contaminations originating from elastic and deep-inelastic scattering, as discussed above. The asymmetry for the elastic contribution was taken from , while for the DIS region a parameterisation  based on world data has been used. Model dependent uncertainties due to these asymmetries and contributions from the Monte Carlo simulation are negligible, as this correction is less than 5% for $`Q^2<`$ 5 GeV2. Radiative corrections were calculated using the codes described in Ref. , and were found not to exceed 2% of the asymmetry $`A_{}^{res}`$. The values for $`A_1^{res}+\eta A_2^{res}`$ for the measured range of $`Q^2`$ values are presented in Table 1. The asymmetry $`A_1`$ was evaluated using Eq. 6 under the assumption that $`A_2=0.06`$  in the whole resonance region, and with an average depolarisation factor $`D`$ weighted by the event distribution.

The contribution $`I_{GDH}^{res}`$ of the resonance region to the GDH integral was determined in each $`Q^2`$-bin from the asymmetry $`A_1`$, according to Eq. 4, in which the integration limits were determined by the 1 GeV$`{}_{}{}^{2}<W^2<4.2`$ GeV2 range. The unpolarised structure function $`F_1=F_2(1+\gamma ^2)/(2x(1+R))`$ was calculated from a modification of the parameterisation of $`F_2`$ given in Ref.  that accounts for nucleon-resonance excitation assuming $`R=\sigma _L/\sigma _T`$ is constant and equal to 0.18 in the whole resonance region. It is worth noting that due to cancellation between the R–dependences of $`F_1`$ and $`D`$ at low $`y`$, the final result is insensitive to the choice of $`R`$. In the integration the $`W^2`$ dependence of the integrand $`F_1/K`$ within the individual bins was fully accounted for.

The results for $`I_{GDH}^{res}`$ are presented in Fig. 2. The integral strongly decreases with $`Q^2`$ over the entire measured range. The magnitude of the systematic uncertainty is indicated by the band. The dominant contribution to the systematic uncertainty is due to the lack of knowledge of $`A_2`$. This contribution (up to 15%) was evaluated from the total error quoted for a measurement in the resonance region: $`A_2=0.06\pm 0.16`$ . This range is consistent with two other possible assumptions for $`A_2`$: $`A_2=0`$, or $`A_2=0.53Mx/\sqrt{Q^2}`$, which describes the behaviour in the deep-inelastic region . Other contributions are uncertainties from the beam and target polarisations (5.3%), from the spectrometer geometry (2.5%), from the combined smearing and radiative effects (up to 10%) and from the knowledge of $`F_2`$ (2%). The smearing contribution to the systematic uncertainty was evaluated by comparing simulated results from two very different assumptions for $`A_1`$: a power law ($`A_1=x^{0.727}`$) that smoothly extends the DIS behaviour for the asymmetry into the resonance region , and a step function ($`A_1=0.5`$ for $`W^2<1.8`$ GeV2 and $`A_1=+1.0`$ for 1.8 GeV$`{}_{}{}^{2}<W^2<4.2`$ GeV2) that is suggested by the hypothesis of the possible dominance of the $`P_{33}`$-resonance at low $`W^2`$ and of the $`S_{11}`$-resonance at higher $`W^2`$.

The results for $`I_{GDH}^{res}`$ are compared in Fig. 2 with two predictions for the contribution of nucleon-resonance excitation to the integral defined in Eq. 2. Burkert and Li  parameterised the experimental $`Q^2`$-evolution of the main nucleon resonances ($`P_{33}`$(1232), $`P_{11}`$(1440), $`S_{11}`$(1535), $`D_{13}`$(1520), $`F_{15}`$(1680)), and assumed single-quark transitions to evaluate the contributions from other resonances. Aznauryan  described the resonance excitation in the approximation of infinitely narrow resonances, and included a contribution from one-pion exchange in the near-threshold region. Both models predict a sudden decline in $`I_{GDH}^{res}`$ as $`Q^2`$ falls below 1.5 GeV2, due to a large negative contribution at low $`Q^2`$ by the helicity structure of the $`P_{33}`$-resonance. At higher $`Q^2`$ the $`P_{33}`$-resonance magnetic form factor strongly decreases with increasing $`Q^2`$, and the positive contribution to $`I_{GDH}^{res}`$ arising from the excitation of higher-mass resonances becomes dominant. Neither of these models includes the non-resonant multi-hadron production channels, which should provide an additional positive contribution for the region $`W^2`$ 4.2 GeV2. Comparison with the data suggests that for $`Q^2`$ 1.5 GeV2, the resonance-excitation models are not sufficient to fully explain the experimental result for $`I_{GDH}^{res}`$. Other predictions exist for the resonance-excitation contribution to generalised GDH integrals, but they are limited to regions of lower $`Q^2`$ .

To complete the evaluation of the full integral $`I_{GDH}`$, data from the DIS region (4.2 GeV$`{}_{}{}^{2}<W^2<45`$ GeV2) were reanalysed in the same $`Q^2`$-bins as for the kinematically more restricted resonance region, following the procedure described in a previous HERMES publication . A total of 1.52 million events were selected in this $`W^2`$-range. The systematic uncertainty for this region is the same as published in . The systematic uncertainty on $`A_2`$ in DIS region does not contribute significantly.

In Table 1 the resonance region contribution $`I_{GDH}^{res}`$, the integrals $`I_{GDH}^{meas}`$ in the full measured region and the full GDH integrals are reported. The latter was calculated in each $`Q^2`$-interval by adding to $`I_{GDH}^{meas}`$ an estimate of the unmeasured contribution for $`W^2>45`$ GeV2. This was calculated using a multiple-Reggeon exchange parameterisation  for $`\sigma _{\frac{1}{2}}(\nu ,Q^2)\sigma _{\frac{3}{2}}(\nu ,Q^2)`$ at high energy, and amounted to about $`3.5\mu `$b for all $`Q^2`$-bins. A parameterisation for $`g_1`$  based on a NLO-QCD analysis provided within 5% the same results as the multiple-Reggeon exchange analysis. This difference was taken as the systematic uncertainty of the high energy contribution. It is worth noting that for the low $`Q^2`$-bins, both the statistical and the systematic uncertainties of $`I_{GDH}`$ are dominated by those from the resonance region. In this region, these uncertainties are large due to the smallness of $`D`$ and to the large size of $`\eta `$, respectively.

In Fig. 3a) the total GDH integral is shown together with the partial integrals for $`W^2<4.2`$ GeV2 and for $`W^2<45`$ GeV2. The contribution of the resonance region to the full GDH integral is small for $`Q^2`$ values above 3 GeV2.

Fig. 3a) also shows a prediction  based on a $`Q^2`$-evolution of the two polarised structure functions $`g_1`$ and $`g_2`$, without consideration of any explicit nucleon-resonance contribution. This prediction is in good agreement with the experimental data.

In the whole energy range, $`I_{GDH}`$ is consistent within the uncertainties ($`\chi ^2/N_{df}=0.4`$) with a simple 1/$`Q^2`$ power law. This is demonstrated in Fig. 3b where the results for $`I_{GDH}`$ are multiplied by $`Q^2/(16\pi ^2\alpha )`$. In the deep-inelastic limit, this quantity is equivalent to $`\mathrm{\Gamma }_1`$ (see Eq. 5). The present results are in agreement with the measurements of $`\mathrm{\Gamma }_1=0.120\pm 0.016`$ at $`Q^2=10`$ GeV2  and $`\mathrm{\Gamma }_1=0.129\pm 0.010`$ at $`Q^2=5`$ GeV2 . In addition, values of $`\mathrm{\Gamma }_1`$ extracted from the present data are also consistent with a measurement of $`\mathrm{\Gamma }_1=0.104\pm 0.017`$ at $`Q^2=1.2`$ GeV2  in which the structure function $`g_1`$ was measured in the resonance region.

In summary, the $`Q^2`$-dependence of the generalised Gerasimov-Drell-Hearn integral for the proton was determined for the first time in both the resonance and the deep-inelastic regions, covering the $`Q^2`$-range from 1.2 to 12 GeV2. In the resonance region, the data suggest that for $`Q^2`$ 1.5 GeV2, existing resonance-excitation models are not sufficient to fully explain the experimental result for $`I_{GDH}^{res}`$. Above $`Q^2=3`$ GeV2 the DIS contribution to the generalised GDH integral is dominant. The $`Q^2`$-behaviour of $`I_{GDH}`$ suggests that there are no large effects from either resonances or non-leading-twist, and indicates that the sign change of $`I_{GDH}`$ to meet the real photon limit occurs at $`Q^2`$ lower than 1.2 GeV2.

We thank S. Gerasimov, V. Burkert and I.G. Aznauryan for useful discussions and I.G.A. for providing the curves of her calculations. We gratefully acknowledge the DESY management for its support, the staffs at DESY and the collaborating institutions for their significant effort, and our funding agencies for financial support.


format: text

text:
# Coherent control using adaptive learning algorithms

## I Introduction

An original impetus for coherent control was mode-selective laser photochemistry. This dream of exciting a specific bond with a laser has dimmed for various reasons. Control is hampered by fast relaxation, complicated mode structure, imperfect knowledge of the inter-nuclear potentials along arbitrary coordinates, and the distorting influence of the strong external light fields. Recent theoretical  and experimental advances have led to successful control of molecular ionization and dissociation , atomic and molecular fluorescence , and excitations or electrical currents in semiconductors . Control has been predicted and demonstrated in several systems that have only two interfering pathways .

Strongly coupled systems such as large molecules in condensed phase are so complicated that it is nearly impossible to calculate optimal pulse shapes in advance. Recent efforts have used experimental feedback as suggested by Judson and Rabitz  to determine the optimal optical pulse shape to achieve a particular control goal . In the absence of detailed knowledge of the system Hamiltonian, an algorithm must be used for selecting new pulse shapes inside the feedback loop.

This paper presents a detailed investigation of a learning strategy incorporating a modified genetic algorithm (GA) in order to discover control pathways in complicated physical systems. Experiments have been carried out in a variety of molecular systems whose common feature is the existence of observable physical properties that depended on the incident (shaped) light. Several systems are described. In the gas phase we explore nonlinear control of ionization channels in diatomic sodium. Several liquid phase experiments are also described, including control of self-phase modulation in $`CCl_4`$ and excitation of vibrational modes in methanol and benzene.

In addition to traditional GA search strategies, we incorporate other search methods that all run concurrently. The algorithm adapts itself during a run in order to search the phase space most efficiently. Because of this, it is possible to obtain physical insight into the problem under investigation not only through the pulse-shape solutions, but also by how the algorithm arrived at those solutions. We demonstrate that our adaptive evolutionary algorithm is capable of controlling a diverse array of systems.

## II Experimental Setup

The control light field is made with a Kerr lens mode-locked (KLM) titanium sapphire laser that produces $`100`$ fs pulses with about $`5`$ nJ of energy at a central wavelength of $`790`$ nm (see Fig. 1). The pulses are temporally dispersed to $`150`$ ps in a single grating expander and amplified to $`2`$ mJ in a regenerative amplifier at $`10`$ Hz. The output of the amplifier is split to form two beams. One beam is sent to the pulse shaper, and the other is used as an unshaped reference for spectral interferometry measurements of the shaped pulses . The pulse shaper consists of a zero dispersion stretcher with an acousto-optic modulator (AOM) in the Fourier plane, where different colors in the light pulse map to different positions on the modulator . The AOM carries a shaped acoustic traveling wave, which diffracts different colors with different phases and amplitudes. These colors are reassembled at the output of the pulse shaper, yielding a temporally shaped laser pulse. In order to compensate for the low efficiency of the pulse shaper ($`1015\%`$), we reamplify the shaped pulses in a low-gain multipass amplifier. The pulses are then compressed in a single grating compressor. The resulting shaped laser pulses are then directed into the molecular sample to be studied, and a predetermined feedback signal is monitored.

## III The Learning Algorithm

### A Constructing the Algorithm

In previous work we demonstrated control of simple quantum systems using feedback . Now we wish to control more complex systems where the optimal pulse shape is not known a priori. The pulse shaper has 8 bit control over the amplitude and phase of 100 different frequency components, so there are $`2^{1600}`$ different pulse shapes. The physical system couples different frequencies, so they cannot each be optimized independently. This presents a vast phase space for the search algorithm. The search must also be robust in the face of experimental noise, and capable of escaping local maxima in a rough potential energy landscape.

These requirements led us to consider a genetic algorithm, which fulfills all of these conditions: It does not rely on any local information about the search space, such as derivatives, and it is capable of handling a multidimensional phase space in the presence of noise. Previous work with adaptive feedback found genetic algorithms (or similar evolutionary strategies ) adept at solving similar problems . A GA provides a general, robust approach to optimization, requiring little prior information about the problem to be solved. Furthermore, the GA can generate new pulse shapes that differ radically from the previous pulse shapes, to quickly sample different sections of the phase space. Our GA implementation is derived from the Handbook of Genetic Algorithms, a standard treatise on the subject .

Genetic algorithms are a class of search and optimization algorithms inspired by biological evolution. In evolution, natural selection links a string of genes to the structures that it represents. The gene string carries all of the information, while a structure’s success determines its chance of reproducing. Nature knows nothing about the problem to be solved; gene strings encoding successful structures merely reproduce more often. During reproduction, the algorithm has no regard for the structure represented by the gene string. Offspring have new gene strings representing new, and possibly more successful, structures. By incorporating these ideas, a GA can solve surprisingly difficult problems. Each possible solution (structure) in the search space is given a representation (gene string). This representation is called an individual, and a group of individuals is called a population.

A basic example of a GA’s implementation is shown in Fig. 2. Each individual in the population is evaluated on a given molecular sample. The individuals are ranked from most to least fit based on a predetermined single-valued feedback function (the fitness). These individuals (parents) then reproduce according to some protocol, called mating. The most fit individuals reproduce more than the least fit ones. The offspring (children) form a new population (the second generation). This reproduction and evaluation process repeats itself until terminated. The fittest current members of the population survive until the end.

In our experiments, each individual corresponds to a pulse shape, which is encoded as a string of floating point numbers specifying the phase and amplitude at the various frequency components of the laser pulse. The algorithm typically controls the phases for $`20`$ to $`60`$ colors, linearly interpolating the phases for colors between the specified frequencies. Unlike the phases, which vary continuously, the amplitudes are set at discrete levels (between $`3`$ and $`40`$). The actual number of amplitude genes was usually less than the number of phase genes (between $`10`$ and $`20`$). For some of the experiments, the learning algorithm is only allowed to vary the phases of the frequency components. This fixes the energy in each pulse shape, and the algorithm simply determines how to best distribute this energy in time.

Our population normally consists of $`60`$ individual pulse shapes. The first generation is composed of random individuals. Each pulse shape in the population interacts with the physical system under investigation and is evaluated for fitness. Our learning algorithm implements a process known as roulette wheel selection, in which an individual’s chances of reproduction are proportional to its fitness, so that more fit individuals reproduce more often. In addition, a given number of the most fit parents are passed on to the next generation. This technique, known as elitism, ensures that good genetic material is not lost if by chance one of the best individuals is not chosen for reproduction or does not reproduce fruitfully.

### B Operators

The protocol for the production of new children is carried out by mathematically defined operators that act on the gene strings of the pulse shapes. A traditional GA uses a mixture of crossover and mutation operators, both of which are described below. We have incorporated new operators to include many different methods for searching the available phase space. The algorithm then combines the entire set of mating operators into a pool, and the various operators are allowed to compete against each other for the chance to produce new pulse shapes. This learning strategy determines which combination of methods is best for solving the particular problem.

We can categorize our operators as traditional GA operators (crossovers and mutations), or nontraditional operators. Traditional operators generate new pulse shapes from old ones on a strictly statistical basis. Traditional operators that we use include two-point crossover, average crossover, mutation, and creep. Nontraditional operators generally search the phase space by modifying the pulse shapes in a way that is guided by the physics of the system. Examples of these operators that we use include smoothing, time-domain crossover, and polynomial phase mutation. A well-chosen set of operators can greatly enhance the performance of the learning algorithm. Our learning algorithm is general and not limited to the operators listed above. As has been discussed elsewhere, it is possible to add other operators to the pool, even including entirely new search algorithms, such as simulated annealing . If simulated annealing happens to be the method best suited to the particular problem, the learning algorithm will discover this, and allow simulated annealing to control the reproduction process.

Appendix A gives the mathematical form of each of the operators that we use. A basic operator employed in most traditional GA’s is known as n-point crossover. This operator selects a portion of the gene string from each of two (or more) parent pulse shapes, and then exchanges this section of the gene string between the two parents. The resulting pair of gene strings are the two new children pulse shapes. We use a two-point crossover, which snips the gene string at two random locations and exchanges the genetic information of the two parents between these two locations in order to produce two children. Average crossover also selects two parent gene strings, but rather than exchange genetic information between them, it averages the values of all the genes from the two parents to produce a single child. One important difference between average crossover and two-point crossover is that average crossover can introduce new gene values that were not present in either parent, while two-point crossover simply exchanges values between the two parents.

Another traditional operator that we employ is mutation. This creates a single child from a single parent by randomly reassigning the values of a group of randomly selected genes. Creep, an operator similar to mutation, reassigns values for selected genes incrementally, adjusting the previous values by a small but random amount. Like average crossover, both creep and mutation can introduce new gene values into the population.

Our nontraditional operators only act on the phase genes of the pulses, leaving the amplitudes fixed. One of the nontraditional operators we use is smoothing. The smoothing operator creates a new pulse from a single parent by performing a three-point windowed average over the phase values in the gene string. This operator works very well for problems that require smooth phase profiles across the bandwidth, and it also aids in the interpretation of the results because it produces pulses that are not plagued as much by the entropically driven variations in gene values that sometimes arise from the GA. The action of smoothing as seen in the time domain is to shorten the pulse and reduce structure at long time.

Time-domain crossover is a variation of two-point crossover that first transforms the gene string into a time domain representation of the pulse by performing an inverse fast Fourier transform (IFFT). It then performs a standard two-point crossover on the time domain pulse representation and transforms the pulse back to the frequency domain via a FFT. This operator is useful for problems that involve time domain correlations in the pulse. High order processes that depend sensitively on $`I\left(t\right)`$ are examples of such problems, and we have shown that the time domain crossover operator performs well in these situations.

Polynomial-phase mutation produces children by replacing a portion of a gene string with a polynomial phase function with a small degree of random variation. The resulting phase profile resembles a polynomial curve over a section of the spectrum. This operator and smoothing work well in conjunction to produce pulses with smooth polynomial phase, which have simpler interpretations in a time-frequency (i.e., Wigner or Husimi) representation .

### C Adaptive Operators

The adaptive algorithm determines how to best solve a problem by evaluating “operator fitnesses”. Like the individual pulse shapes, each of the operators in the pool is evaluated to form a basis for operator selection; each operator is chosen to produce new pulse shapes with a probability proportional to its own fitness. The operator fitnesses are controlled by compiling an operator geneology to keep track of the operators responsible for creating each individual, and assigning a “credit” anytime an operator produces a very fit new pulse shape. Thus, operators that produce good pulses are given the opportunity to produce more children. Specifically, credit is assigned when either (1) an individual pulse shape in the current generation is more fit than the best pulse shape of the previous generation, or (2) an individual was an ancestor of a pulse shape that is more fit than the best pulse shape of the previous generation. Passing credit back more than one generation is important, since some operators tend to act in concert. For example, mutation may change genes in ways that are not beneficial until combined with certain other genes in the gene string. By combining the changes made by mutation, two-point crossover may be able to produce fitter children. Passing the credit back a generation or two insures that the mutation operator is also rewarded for its contribution.

We begin our algorithm by assigning each operator an initial normalized fitness, or weighting. The initial weightings are determined by various methods, including empirically (from both experiments and simulations) or through prior knowledge of typical algorithm performances. After the first three generations, the operator fitnesses are allowed to evolve. At this point, the weight for each operator has two parts: a base weight (the value of the operator’s fitness during the previous generation) and an adaptive weight (the operator’s fraction of the total credit assigned to all individuals during the previous three generations). After each subsequent generation, each operator’s new fitness is a weighted sum of its current base weight ($`85\%`$) and its current adaptive weight ($`15\%`$). Adaptive weighting allows the operators that produce better children to increase their operator fitness. This serves two functions. First, this process speeds up the convergence of the algorithm, since the operators that are not producing better children, and therefore not helping the evolution, are prevented from dominating the reproduction process. Second, the fitnesses of the different operators can yield insight into the dynamics of the learning algorithm and also into the physical system itself by monitoring each operator’s fitness as a function of the generation. Possible control mechanisms can be tested by introducing new physically motivated operators and evaluating their success. However, the reproductive process is not required to “know” about the particular goal for the problem. The success of the algorithm relies on the fact that the adaptive pool of operators searches vast regions of phase space efficiently, finding successful individuals without any prior knowledge.

The full power of the learning algorithm is best put to use in problems where the experimental knobs are all coupled - when the different degrees of freedom are not independent of each other. In our experiments, the phases and amplitudes of the individual colors are coupled by the system Hamiltonian. In a completely decoupled basis, the problem is reduced to a series of simple one-dimensional searches for each of the genes. However, one does not know what this basis is in general. In a coupled basis, crossover has been demonstrated to be a very valuable operator in selecting new pulse shapes that out perform their parents.

## IV Experiments

### A Preliminary Test of Learning Feedback: Second Harmonic Generation in BBO

Many of the characteristics of adaptive learning are demonstrated by the simple control experiment of second-harmonic generation (SHG). Feedback experiments using SHG have previously been carried out with the goal of targeted pulse compression or shaping . Our primary goal was to investigate the dynamics of our algorithm and the learning process in a well-characterized and well-studied system. Frequency doubling in a noncentrosymmetric crystal with a large $`\chi ^{\left(2\right)}`$ provided us with this opportunity. Even though the interaction of the light field with this system can be described classically, this experiment illustrates features that are relevant to all the experiments described in this paper. In addition we are able to simulate the experimental feedback signal, which allows us to compare learning algorithms on the model with experiment.

In the low-intensity regime, the interaction of the laser pulses with the crystal can be described by a nonlinear polarization that is proportional to the square of the input light field:

$$P_{NL}\left(2\omega \right)=\chi ^{\left(2\right)}E\left(\omega \right)^2.$$
(1)
This nonlinear polarization acts as a source or driving term in the wave equation for a field at $`2\omega `$. The experimental feedback signal is the integrated second-harmonic intensity:

$$Signal=𝑑tE_{2\omega }^2\left(t\right)𝑑tE_\omega ^4\left(t\right).$$
(2)
If the input field strength is not too large, this description of the interaction gives accurate predictions for the second-harmonic generation without including other nonlinear effects. For all of the frequency doubling experiments and simulations, the amplitude of each frequency component in the pulse is kept fixed. Only the phases may vary. The laser pulse energy is therefore constant, and the algorithm determines how to distribute this energy in time.

The optimal pulse shapes are best viewed as Husimi distributions. The Husimi distribution, $`Q(t,\omega )`$ is calculated from the measured field $`E(\omega )`$ in the frequency domain:

$$Q(t,\nu )=𝑑t^{}𝑑\nu ^{}S(t^{},\nu ^{})e^{(\nu \nu ^{})^2(tt^{})^2},$$
(3)
$$S(t,\nu )=E(\nu +\nu ^{})E^{}(\nu \nu ^{})e^{2i\nu ^{}t}𝑑\nu ^{}.$$
(4)
$`S(t,\nu )`$ is the Wigner function whose marginals represent the power spectrum $`P(\nu )`$ and the temporal intensity $`I(t)`$ of the laser pulse:

$$𝑑\nu ^{}S(t,\nu ^{})=I(t),$$
(5)
$$𝑑t^{}S(t^{},\nu )=P(\nu ).$$
(6)
Husimi distributions are generated using the values of the phase and amplitude that the pulse shaper programs onto each individual pulse shape. We use spectral interferometry on a limited number of pulse shapes to verify the correspondence between the phase and amplitude profile of the pulse and its representation on our pulse shaper. Since each convergence run of the algorithm has the potential to provide a vast amount of information regarding the problem under study, we monitor not only the optimal pulse shape solution, but also compare this solution to other competing solutions from individual generations throughout the run.

Figure 3 shows the Husimi distributions for pulses optimized to either maximize or minimize frequency doubling in BBO. The results of both simulations and experiments are shown for comparison. Comparison of panels a and c reveals that experiment and simulation arrive at the same result for maximizing SHG, except for a small amount of quadratic dispersion (chirp) evident in the experimental result that is within our measurement resolution of the laser pulse.

When the algorithm minimizes the SHG, solutions from both the simulation and experiment contain structure in $`I\left(t\right)`$. We initially expected the solutions for the spectral phase $`\varphi \left(\omega \right)`$ would contain only the lowest nontrivial order ($`\varphi \left(\omega \right)=k\omega ^2`$). Given the AOM’s constraint of a maximum allowed phase change between adjacent frequencies in the light pulse, quadratic phase is the most efficient single-order phase variation, since it allows for the greatest amount of total phase variation across the spectrum. However, the algorithm finds that a single order of phase is not the most efficient way to minimize $`I\left(t\right)`$ . We evaluated pulses that were simply chirped in time by programming them with the maximum amount of quadratic-only phase allowed by the resolution of our pulse shaper, and found that they did not perform as well as the solutions found by the learning algorithm (see Fig. 3).

Simulations provide rapid testing of the performance of many possible operators. For instance, Fig. 4 shows the best fitness as a function of generation for three different runs of the SHG simulation, both with and without the smoothing operator. The addition of the smoothing operator allows the algorithm to achieve higher fitness more rapidly and converge sooner. In the absence of noise, the best fitness increases monotonically as a function of generation, as guaranteed by elitism.

When the intensity of the light increases, our simple model is no longer adequate to describe the doubling process. Figure 5 shows the changing optimal pulse shape for maximization of SHG as the energy of the input pulse is increased. The optimal pulse in the high-energy solutions acquires large third- and fourth-order dispersion. The shaped pulse spectrum at high intensities shows significant self-phase modulation (SPM), whereas in the low intensity limit there is no evidence of SPM. Simulations are also consistent with SPM in the crystal, which contributes to variations in the solutions as the intensity is increased . At higher pulse energies, SPM is no longer negligible. Evidently, SPM distorts the phase matching for the SHG process, so that a transform limited input pulse is no longer optimal for maximum SHG.

The interplay of multiple operators during the algorithm can yield further insight into the learning process. Figure 6 shows the operator fitness as a function of generation for several of our common operators during the frequency doubling experiment. The operators are initialized in a traditional GA configuration, with two-point crossover dominant. For the first few generations, the operators create children in proportion to their initially assigned fitnesses, but after the third generation their fitnesses are allowed to freely change in accordance with the procedure described earlier. As Fig. 6 demonstrates, the algorithm finds that two-point crossover and simple mutation are not always the best operators, and at different points during the evolution, different combinations of operators become optimal for producing the best children. Polynomial phase mutation, smoothing, and average crossover each produce very fit children at different stages of the run.

This example shows that operators cannot be evaluated in isolation, because they affect each other. For example, smoothing is more important when other operators tend to introduce unnecessary phase variations across the pulse. Also, the performance of the operators cannot be evaluated instantaneously, but must be evaluated over the course of several generations. An operator that is not performing well at one point during the run may become more useful later on. Since some operators that perform poorly at the beginning of the algorithm often perform very well toward the end (e.g., average crossover), their fitness is not allowed to fall below some minimum value ($`5\%`$). This lower bound ensures that every operator always has some chance of being used during reproduction. Finally, the performance of each operator depends on the problem. Performance of a given operator can help determine whether its action on an individual is physically relevant.

The fitness function assigns each individual pulse shape a single-valued number, reflecting that individual’s ability to achieve the goal. Since an individual’s fitness is used in parent selection (see Appendix B for details), its determination is an important step in the performance of the algorithm. For the frequency doubling experiment, the fitness assigned to each individual was simply the integrated blue light intensity as measured by a photodiode in a regime where the response of the diode was linear. The frequency doubling experiment, therefore, provides a clear testing ground for the learning algorithm. In other experiments, it is not always so clear how to assign a fitness to each individual, given the nature of the measurement to evaluate the success of each pulse.

### B Controlling Dissociative Ionization in Diatomic Sodium

We next explore nonlinear control mechanisms for ionization of diatomic sodium. This experiment provides further opportunities to understand the learning algorithm. However, unlike second-harmonic generation, which can be described classically, this is strictly a quantum system. Here, the adaptive algorithm and pulse shaper must control higher-order nonlinearities. The multiphoton ionization of this system was previously studied using low-energy laser pulses with a single photon resonance enhancement . Our experiments use lower-energy laser photons that are below this resonance.

The shaped pulses were focused into a molecular beam of sodium, causing the molecules to undergo multiphoton ionization. A time-of-flight mass spectrometer allowed identification of molecules that dissociatively ionized and those that did not. The fitness function was a normalized ratio of the ion yield for the two channels. The learning algorithm then worked to optimize either dissociative or nondissociative ionization. As in the doubling experiment, we restricted the algorithm to control only the phases of the colors, with the amplitudes fixed. The algorithm was able to find pulse shapes that could maximize either channel. In the case of maximizing the nondissociative channel, the optimal pulse yielded $`88\%`$ nondissociative ionization. When we optimized the other channel, we found $`73\%`$ dissociative ionization.

Figure 7 shows the Husimi distributions for pulses optimized to either nondissociatively or dissociatively ionize the sodium molecules. In addition, the ion yield as a function of the laser energy for an unshaped laser pulse is plotted for both of the channels. The solutions resemble the optimal pulse shapes for the second-harmonic generation experiment (see Fig. 3). For the dissociative channel, the pulse shape is similar to the short-pulse, high-intensity solution of SHG maximization, while for the nondissociative channel, the pulse shape is similar to the long-pulse, low-intensity solution of SHG minimization. These results are consistent with the fact that the two channels in log-log plot have different slopes, and that the branching ratio is a function of intensity.

The sodium experiment demonstrates the importance of the choice of basis for encoding pulse shapes. The learning algorithm incorporates the time-domain crossover operator, which allows it to choose the basis best suited to the problem. Figure 8 shows the operator fitnesses as a function of generation when optimizing the nondissociative channel. There are five operators - four in the usual frequency basis, and the time-domain crossover operator in the time basis. As Fig. 8 shows, the time-domain crossover operator increases its fitness at the expense of the operators working in the frequency basis. Correlations in the time domain are an important control parameter for this problem, as expected.

Another possible control mechanism involves the parity of the phase profile of the pulse: Is the phase as a function of frequency an even function, an odd function, or neither about the central frequency? Parity control in nonlinear atomic absorption was previously demonstrated by Meshulach and Silberberg . The amount and sign of chirp on the pulse is another possible way to control the population dynamics . We investigated both possibilities using our pulse shaper and feedback, but saw no conclusive dependence on the dissociation fraction with either method. The adaptive pool of operators performs a more effective search of the phase space.

### C Controlling Molecular Liquids

Molecular liquids pose a greater challenge for learning control, because of rapid relaxation and inhomogeneous broadening. Our initial goal was to control molecular vibrations in liquids through impulsive stimulated Raman scattering. Impulsive scattering occurs when the laser pulse is shorter than the vibrational period of the molecule. In the frequency domain, this means that the bandwidth of the laser is broad compared to the vibrational energy spacing of the mode in question. The result is that a stimulated Stokes wave can be seeded with light that is already present in the laser and does not have to build up from noise, thereby making the process much more efficient than the nonimpulsive case. Shaped laser pulses should allow selective control over excitation of Raman modes since the pulse shaper can modulate the spectrum of $`E^2(\omega )`$, the driving term in Raman excitation . In the time domain, this corresponds to resonantly driving some modes but not others.

#### 1 Controlling SPM in Liquids

Impulsive scattering in a multimode molecular liquid was studied in $`CCl_4`$ because it has several low frequency modes with relatively high cross sections. We discovered, however, that it also has a large polarizability, and therefore, most of the light that was scattered near the laser bandwidth in the forward direction was a result of SPM. We found that we had a significant degree of control over the spectrum of the forward scattered light, and so as an initial demonstration of the capabilities of the apparatus, we studied the nonlinear frequency shift of intense light propagating in $`CCl_4`$. Early results of this investigation were previously published . Here, we describe the learning process and analyze the solutions in more detail.

Feedback goals for SPM are based upon small features that are barely visible in the spectra of the forward scattered radiation after unshaped pulses illuminate the sample. These modulations are typical spectral features for pulses that have undergone SPM . The learning algorithm is able to control their frequency and phase by altering the shape of the driving pulse. Only phase modulation is used, so that the pulse energy is fixed. Figure 9 shows the spectra of four different pulses after propagating through the $`CCl_4`$ sample. The first panel shows the spectrum for an unshaped pulse, and the following three panels show spectra for pulses that are shaped to control the spectral modulations.

Model calculations can determine whether SPM is responsible for the observed spectra. The simplest description of SPM, which doesn’t include spatial effects such as self focusing, characterizes the nonlinear interaction between the laser and the medium through a intensity-dependent index of refraction:

$$n(t)=n_0+n_2I(t)$$
(7)
where $`n_0`$ is the field free index, I is the instantaneous laser intensity, and $`n_2`$ is an empirically determined coefficient. The calculated power spectra for laser pulses that have acquired a phase proportional to their instantaneous intensity show intensity modulations with the same dependence on pulse shape that we found in the experiment (see Fig. 9).

#### 2 Controlling Vibrations in Multimode Molecular Liquids

The learning algorithm can also control the interaction between the driving laser pulse and the vibrational modes of a multimode molecule without making use of impulsive scattering. In order to avoid confusion between Stokes light and light generated by SPM alone, we chose a molecule with a much larger Stokes shift, since there is much less light generated through SPM further from the central laser frequency. Methanol ($`CH_3OH`$) is ideal because it has two closely spaced modes with large Stokes shifts and large cross sections. Forward scattered radiation is the feedback for the algorithm. There is no backwards scattered Stokes radiation because of the short duration of the shaped pump pulse ($`1ps`$). The forward-backward symmetry of the scattering is broken for a short pump pulse because the backward traveling Stokes wave passes through the pump wave before any appreciable buildup .

The time scales for the interaction between the molecules and the laser pulse are set by the vibrational period of the active modes and their coherence time. Stimulated scattering with pulses that are longer than the coherence time reaches a steady state and exhibits a strong dependence on pulse duration because it is a stimulated process: The more photons that interact with the molecules within the coherence time, the more likely the molecule will be stimulated to absorb a laser photon and emit a Stokes photon. Scattering with pulses that are shorter than the coherence time but longer than the vibrational period (transient Raman scattering) exhibits little dependence on the duration of the laser pulse . Scattering with pulses that are shorter than the vibrational period (impulsive scattering) results in very efficient stimulated scattering as discussed above .

With an unshaped laser pulse focused into $`10cm`$ of methanol, the spectrum shown in Fig. 10 a is obtained. The two small peaks in the spectrum correspond to Stokes light for $`\delta \nu =1`$ for the symmetric and asymmetric C-H stretch modes. The lens focal length is $`40cm`$. The first feedback goal is to maximize the contrast between the two Stokes peaks and the background light resulting from SPM. The forward scattered spectrum in the spectral range of the Stokes radiation is collected for each laser pulse. The number of Stokes photons at a particular frequency is a measure of the number of molecules excited in that particular mode; however, since SPM is present and the bandwidth of the shaped laser pulses is large, the forward scattered spectrum also contains some misleading information. The feedback function must filter this out. Different fitness functions work best, depending on which peak(s)are optimized. A typical fitness function is:

$$\underset{\omega _r<\omega _i<\omega _b}{}\frac{NC\left(\omega _i\right)}{\omega _b\omega _r}\underset{\omega _i>\omega _b,\omega _i<\omega _r}{}\frac{C\left(\omega _i\right)}{\mathrm{\Delta }\omega \left(\omega _b\omega _r\right)}.$$
(8)
Here, $`C\left(\omega _i\right)`$ is the number of spectrometer counts at $`\omega _i`$, $`\mathrm{\Delta }\omega `$ is the bandwidth of the spectrometer, $`\omega _r`$ is the low-frequency limit for the desired peak, $`\omega _b`$ is the high-frequency limit for the desired peak and N is an empirically determined integer. We set the values of $`\omega _r`$ and $`\omega _b`$ by narrowing the bandwidth of shaped laser pulse and measuring the width of the Stokes peaks in the forward scattered spectrum. We find that $`N=2`$ and $`N=3`$ work well. A pulse solution that optimizes the contrast between the two Stokes peaks and the background is shown in Fig. 10 b.

The next goal is to generate spectra with each peak separately. These spectra, shown in Fig. 10 c, correspond to exciting symmetric or antisymmetric modes alone. The Stokes shift for these modes is large compared to the bandwidth of the driving laser pulse. This is equivalent to saying that the Raman excitation is nonimpulsive, and therefore, one cannot seed the Stokes radiation directly with the laser light. Our final feedback goal is to eliminate all forward scattered light at either of the two Stokes frequencies, with the resulting spectrum shown in Fig. 10 d.

#### 3 Using the Adaptive Algorithm to Investigate Possible Control Mechanisms for SRS in Methanol

The Stokes shift for the C-H stretch is almost $`3000cm^1`$and the laser bandwidth is roughly $`100cm^1`$, so the scattering is definitely nonimpulsive. Another possible mechanism that could account for our ability to selectively excite the symmetric or asymmetric stretch mode of methanol is a coupling between the electronic polarizability of the atoms and the vibrational modes. The results with $`CCl_4`$ have shown that the light generated from SPM of the pump beam is very sensitive to the input pulse shape. A large contribution to SPM, particularly for femtosecond pulses, is the atomic polarizability . Perhaps the atomic polarizability generates SPM to seed one of the two Raman modes but not the other.

This hypothesis was tested by replacing the methanol with a mixture of benzene ($`C_6H_6`$) and deuterated benzene ($`C_6D_6`$). Similar control experiments were attempted, except now the two modes of vibration were in two different molecules. The ring breathing mode of benzene $`\left(\nu =992cm^1\right)`$ has a large Raman cross section making excitation easy. Deuterated benzene has a frequency of $`\nu _D=945cm^1`$ which is shifted by $`47cm^1`$, similar to the mode splitting in methanol. Initially, an unshaped laser pulse was focused into the experimental cell with pure $`C_6H_6`$, and we measured no forward scattered Stokes light. We then used the learning algorithm to find a shaped pulse that generates the forward scattered Stokes radiation shown in Fig. 11 (top panel, left curve). The deuterated benzene ($`C_6D_6`$) generates the spectrum shown in Fig. 11 (top panel, right curve), demonstrating the expected shift of the mode frequency. Finally, a $`50/50`$ mixture of $`C_6H_6`$ and $`C_6D_6`$ is placed in the cell and we ask the algorithm to selectively drive each of the two modes. Figure 11(bottom panel) shows the learning algorithm can select the $`C_6H_6`$ mode but not the $`C_6D_6`$ mode. This demonstration of a lack of control is consistent with the idea that the mode selection is an intramolecular effect that relies on coupling between the two modes inside each molecule, rather than seeding of one of the modes with light from SPM.

Another experiment supports this conclusion: Experiments conducted in $`CO_2`$ gas show that light generated by SPM more than a few hundred $`cm^1`$ away from the laser frequency is extremely noisy and not reproducible . The reproducibility of SPM spectra increases nearer the frequency of the driving laser. Figure 9 shows that SPM produces stable spectra very near the laser frequency. However, far from the laser at the frequency of the Stokes light from the C-H stretch mode, the light produced by SPM would be too noisy to reproducibly seed one of the two Raman modes but not the other.

Another possible control mechanism is suggested by analyzing the optimal pulse shape solutions for exciting each of the two modes. Figure 12 shows the Husimi distribution for pulses that were optimized for excitation of the asymmetric stretch mode in methanol, while Fig. 13 shows the Husimi distribution for pulses optimized for excitation of the symmetric stretch mode. The structure of the optimal pulse shape for the symmetric stretch mode suggests a “quasi-impulsive” model, where the frequency separation of the two subpulses is exactly the beat frequency between the symmetric and asymmetric modes. The term “quasi-impulsive” is used, since although the laser bandwidth is narrow compared to the Stokes shift of each mode, it is wide in comparison to the spacing between the modes. This is equivalent to saying that in the time domain, the laser pulse is long compared to the vibrational period of the modes, but short compared to the beat note between them. The beat note period is $`285`$ fs, while the time duration of the unshaped laser pulse is $`150`$ fs. Therefore, energy could be transferred between the two modes by engineering temporal structure in the driving pulse at the coupling frequency between the two modes. Once an initial vibrational population is established in some combination of the two modes, the population could be redistributed by the shaped pulse through an impulsive coupling of the two levels.

General trends in an entire population can provide valuable information, since looking at a single individual, even if it is the very best pulse shape of the group, does not give information about which features are necessary and which are merely sufficient. One cannot tell whether a feature in the pulse shape plays some physical role in the process under investigation, or whether the algorithm simply did not remove the feature since its presence did not degrade the fitness. We test this by repeating a convergence sequence of the learning algorithm with different random initial populations. If the best solution has similar structure multiple times, it is likely that the structure is physically necessary.

Statistical variations among gene values of individuals in a population also reveals which genes are important for a given problem and which are not. Figure 14 shows the genetic variation as a function of generation for a run of the algorithm during the methanol experiment. Light shading represents a large degree of variation among individuals for the value of a given gene, while dark shading represents low variation. The variation is the normalized sum of the absolute values of the differences between all of the genes’ values in a given location on the gene string:

$$\underset{i,j>i}{\overset{N}{}}|g_ig_j|,$$
(9)
where $`g_{i,j}`$ is the value of gene $`g`$ for the $`i^{th},j^{th}`$ individual. Since the genes are randomly initialized, all the genes begin with a light shading. As the algorithm converges, all gene values become more similar through mating. The plots verify the intuitive idea that near convergence, frequency components whose amplitudes are large have smaller variation in their programmed phase values than frequency components whose amplitudes are zero. The power spectra shown at right match with the darker regions (smaller variation) in the plots.

## V Conclusions

We have demonstrated control over a variety of systems using an adaptive learning algorithm. The algorithm uses a variety of searching methods and adapts itself in order to arrive at an optimal solution. This learning technique is general and can be applied to other systems since the interaction does not require specific resonances and no prior knowledge of the system Hamiltonian is required. The adaptive approach provides information about the physical system through examination of the solutions, the operator dynamics, and the choice of basis. Future goals include controlling bond excitation to drive reactions in bimolecular solutions.

## Acknowledgements

The authors would like to acknowledge very helpful and informative discussions with Marcus Motzkus, Ronnie Kosloff, Misha Ivanov, and Robert Levis, as well as Daniel Morris for technical assistance. This work was supported by the National Science Foundation under Grant No. $`9987916`$.

## A Definitions of Operators

$`\text{r}_i=rand(),P=parent,C=child`$

Two Point Crossover
$`P1`$ $`=`$ $`[\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)],P2=[\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)]`$
$`C1`$ $`=`$ $`\left\{\begin{array}{c}[\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)],j<i<k\\ [\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)],\text{all other i}\end{array}\right\},C2=\left\{\begin{array}{c}[\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)],j<i<k\\ [\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)],\text{all other i}\end{array}\right\}`$
Average Crossover
$`P1`$ $`=`$ $`[\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)],P2=[\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)]`$
$`C`$ $`=`$ $`\left\{\begin{array}{c}[\frac{\mathrm{\Phi }_{p1}\left(\omega _i\right)+\mathrm{\Phi }_{p2}\left(\omega _i\right)}{2},\frac{A_{p1}\left(\omega _i\right)+A_{p2}\left(\omega _i\right)}{2}],j<i<k\hfill \\ [\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)],\text{all other i}\hfill \end{array}\right\}`$
Mutation
$`P`$ $`=`$ $`[\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)]`$
$`C`$ $`=`$ $`\left\{\begin{array}{c}[2\pi r_i,r_i],\text{i}>\text{k}\\ [\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)],\text{all other i}\end{array}\right\}`$
Polynomial Phase Mutation
$`P`$ $`=`$ $`[\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)]`$
$`C`$ $`=`$ $`\left\{\begin{array}{c}[\omega _i^n+r_i,A_p\left(\omega _i\right)],j<i\text{ or }i<k\hfill \\ [\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)],\text{all other i}\hfill \end{array}\right\}\text{ where }n=(int)6r_i`$
Creep
$`P`$ $`=`$ $`[\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)]`$
$`C`$ $`=`$ $`\left\{\begin{array}{c}[\mathrm{\Phi }_p\left(\omega _i\right)+0.25rand(),A_p\left(\omega _i\right)+A_{level}(\pm 1,0)],\text{ }r_i<0.10\text{ }\hfill \\ [\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)],r_i0.10\hfill \end{array}\right\}`$
Smooth
$`P`$ $`=`$ $`[\mathrm{\Phi }_p\left(\omega _i\right),A_p\left(\omega _i\right)]`$
$`C`$ $`=`$ $`[{\displaystyle \frac{\mathrm{\Phi }_p\left(\omega _i\right)+\mathrm{\Phi }_p\left(\omega _{i+1}\right)+\mathrm{\Phi }_p\left(\omega _{i1}\right)}{3}},A_p\left(\omega _i\right)]`$
Time Domain Crossover
$`P1`$ $`=`$ $`[\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)],P2=[\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)]`$
$`P1^{^{}}`$ $`=`$ $`IFFT[\mathrm{\Phi }_{p1}\left(\omega _i\right),A_{p1}\left(\omega _i\right)]=E_1\left(t_i\right),P2^{^{}}=IFFT[\mathrm{\Phi }_{p2}\left(\omega _i\right),A_{p2}\left(\omega _i\right)]=E_2\left(t_i\right)`$
$`C1^{}`$ $`=`$ $`\left\{\begin{array}{c}\left[E_1\left(t_i\right)\right],j<i\text{ or }i<k\hfill \\ \left[E_2\left(t_i\right)\right],\text{all other i}\hfill \end{array}\right\},C2^{}=\left\{\begin{array}{c}\left[E_2\left(t_i\right)\right],j<i\text{ or }i<k\hfill \\ \left[E_1\left(t_i\right)\right],\text{all other i}\hfill \end{array}\right\}`$
$`C1`$ $`=`$ $`IFFT\left(C1^{}\right),C2=IFFT\left(C2^{}\right)\text{but original amplitudes are kept since}A\left(\omega _i\right)1`$
## B Details of Fitness Function

Each individual is evaluated, and a single-valued fitness is returned to the algorithm. Each individual’s fitness is transformed into a scaled fitness used for parent selection during reproduction. The fitness scaling helps to ensure there is an adequate degree of “selection pressure”, which is a measure of how much successful pulse shapes are rewarded. Maintaining selection pressure becomes difficult when the range of fitness values decreases as the algorithm converges. Without fitness scaling the algorithm can stagnate since more fit pulse shapes receive little reward. Specifically, we use a linear scaling technique:

$`ScaledFitness={\displaystyle \frac{BestFitnessUnscaledFitness}{AverageFitnessBestFtiness}}+2`$

Any scaled fitnesses less than zero are reset to zero. With this scaling method the best pulse shape is selected as a parent twice as often as the average pulse shape.


text:
# Nonlinearity of Acoustic Effects and High-Frequency Electrical Conductivity in GaAs/AlGaAs Heterostructures under Conditions of the Integer Quantum Hall Effect

## I Introduction

Studies of the kinetic effects in GaAs/AlGaAs heterostructures with two-dimensional (2D) electron gas in strong constant electric fields  show that nonlinear effects are adequately accounted for by heating of electron gas. The main issue of controversy in the interpretation of the above results is related to identification of the relevant mechanism of electron-energy relaxation. The theory of electron-gas heating and the energy-relaxation mechanisms in the 2D case were considered in Ref. . In Ref. , the dependence of the coefficient of absorption of a surface acoustic wave (SAW) by 2D electron gas in a GaAs/AlGaAs heterostructure on the SAW intensity was also explained by heating of 2D electron gas by the SAW alternating electric field; it was also shown that the electron-energy relaxation time is controlled by energy dissipation at the piezoelectric potential of acoustic phonons under conditions of strong screening.

In the magnetic-field range where electrons are localized (i.e.. under the conditions of IQHE), kinetic effects were also actively studied in a strong constant electric field . However, notwithstanding the fact that nonlinear dependences of current on voltage were similar in all cases, these dependences have not been unambiguously interpreted so far. Thus, these nonlinearities were explained by the heating of 2D electron gas . by impurity breakdown in homogeneous electric field , and by resonance tunneling of electrons between the Landau levels ; still another explanation was based on the theory of variable-range hopping conduction in a strong electric field . In Ref. , in order to explain the nonlinearities in the dependence of the width of the IQHE step on the current density in a GaAs/AlGaAs heterostructure at $`T`$ = 2.05 K. the model of heating of 2D electron gas was used. It was found that the dependence of electron temperature $`T_e`$ on the current $`I`$ coincided with $`T_e(I)`$ measured in the absence of a magnetic field. As a plausible reason for this behavior, the authors of Ref.  could only suggest that it arose from the injection of hot charge carriers from near-contact regions where the Hall voltage was shorted out by the current contacts.

In connection with the above, the acoustic method seems to hold considerable promise for studying the nonlinear effects under the conditions of IQHE; this method is particularly convenient owing to the fact that there is no need for electrical contacts in such measurements.

In this work, we studied the dependences of absorptivity $`\mathrm{\Gamma }`$ and variations $`\mathrm{\Delta }V/V`$ in the velocity of SAWs in a piezoelectric due to the interaction of SAWs with 2D electron gas in GaAs/AlGaAs heterostructures on the SAW power $`W`$ absorbed in the sample (or on the SAW electric field $`E`$) under the conditions of IQHE ($`T`$ = 1.5 K), which corresponds to the carrier-localization domain. The experimental dependences $`\mathrm{\Gamma }`$(E) and $`\mathrm{\Delta }V/V(E)`$ were used to calculate the real and imaginary components of high-frequency electrical conductivity $`\sigma _1(E)`$ and $`\sigma _2(E)`$), as the high-frequency conductivity is written in the complex form  $`\sigma (E)=\sigma _1(E)i\sigma _2(E)`$ under the electron-localization conditions. The mechanisms of the nonlinearities were studied by analyzing the dependences of the components of the high-frequency electrical conductivity on the strength (i.e., on absorbed power) of a high-frequency electric field.

## II EXPERIMENTAL METHODS AND RESULTS

In this work, the effect of the SAW power introduced into sample ($`f`$= 30 MHz) on the absorption coefficient $`\mathrm{\Gamma }`$ and on the relative variation in the SAW velocity $`\mathrm{\Delta }V/V`$ was measured at $`T`$=1.5K in magnetic fields corresponding to the midpoint of the Hall plateau (i.e., under the conditions of IQHE). We used the GaAs/AlGaAs heterostructures $`\delta `$-doped with silicon; the density of electrons in 2D gas in the channel was $`n=(1.32.7)\times 10^{11}cm^2`$ and their mobility was $`\mu 2\times 10^5cm^2/(Vs)`$. The heterostructures were grown by molecular-beam epitaxy and involved a spacer layer $`4\times 10^6`$cm in width. The experimental procedure was described in detail elsewhere . Here, we only note that the structure with 2D electron gas was grown on the piezoelectric (lithium niobate) surface over which the SAWs propagated. An alternating electric field having the frequency of SAW and accompanying the strain wave penetrates into the channel with 2D electron gas, induces electric currents and, correspondingly, introduces ohmic losses. As a result of such an interaction, the wave energy is absorbed. Experimentally, we measured the absorption coefficient $`\mathrm{\Gamma }`$ and the relative variation in the SAW velocity $`\mathrm{\Delta }V/V`$ in relation to the magnetic induction. Since the measured quantities $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }V/V`$ are defined by the electric conductivity of 2D electron gas, electron-spectrum quantization resulting in the Shubnikov-de Haas oscillations brings about oscillations in the above effects as well.

Figure 1 shows the dependences of $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }V/V`$ on the power $`P`$ at the output of the RF generator (for a frequency of $`f`$= 30 MHz) for the filling numbers $`\nu `$ = 2; 4 and 6 for a sample with the 2D-electron gas density of $`n=2.7\times 10^{11}cm^2`$ Here, $`\nu =nch/eH`$, where $`H`$ is the magnetic field strength. In the insert in Fig. 1, the dependences of $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }V/V`$ on the magnetic field are shown for several values of the SAW power at a temperature of 1.5K. The form of the dependences of $`\mathrm{\Gamma }`$ on the magnetic field is analyzed in detail in Ref. : positions of the peaks in the $`\mathrm{\Gamma }`$(H) and $`\mathrm{\Delta }V/V(H)`$ curves are equidistant in $`1/H`$, and the splitting of the $`\mathrm{\Gamma }()`$ peaks under the IQHE conditions is related to its relaxation origin. It can be seen from Fig. 1 that an increase in the supplied SAW power results invariably in a decrease in $`\mathrm{\Delta }V/V`$ irrespective of the filling number, which corresponds to an increase in electrical conductivity . The form of dependences $`\mathrm{\Gamma }(H)`$ for dissimilar filling numbers is different: absorption increases with increasing $`P`$ for $`\nu `$ = 2, whereas, for $`\nu `$ = 4 and 6, $`\mathrm{\Gamma }`$ increases initially as the SAW power increases, attains a maximum, and then decreases. The smaller the filling number, the higher the power corresponding to the maximum in $`\mathrm{\Gamma }`$. It is also evident from Fig. 1 that the higher the magnetic field (the smaller the filling number), the higher is power $`P`$ corresponding to the onset of the dependences $`\mathrm{\Gamma }`$(P) and $`\mathrm{\Delta }V/V(P)`$.

## III DISCUSSION OF THE RESULTS

In the experimental configuration of this work, the quantities $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }V/V`$ are defined  by the formulas

$`\mathrm{\Gamma }=8.68{\displaystyle \frac{K^2}{2}}qA{\displaystyle \frac{(\frac{4\pi \sigma _1}{\epsilon _sV})t(q)}{[1+(\frac{4\pi \sigma _2}{\epsilon _sV})t(q)]^2+[(\frac{4\pi \sigma _1}{\epsilon _sV})t(q)]^2}},{\displaystyle \frac{dB}{cm}}`$ (1)
$$A=8b(q)(\epsilon _1+\epsilon _0)\epsilon _0^2\epsilon _se^{(2q(a+d))},$$

$$\frac{\mathrm{\Delta }V}{V}=\frac{K^2}{2}A\frac{(\frac{4\pi \sigma _2}{\epsilon _sV})t(q)+1}{[1+(\frac{4\pi \sigma _2}{\epsilon _sV})t(q)]^2+[(\frac{4\pi \sigma _1}{\epsilon _sV})t(q)]^2},$$

$$b(q)=[b_1(q)[b_2(q)b_3(q)]]^{1,}$$

$$t(q)=[b_2(q)b_3(q)]/[2b_1(q)],$$

$$b_1(q)=(\epsilon _1+\epsilon _0)(\epsilon _s+\epsilon _0)(\epsilon _1\epsilon _0)(\epsilon _s\epsilon _0)e^{(2qa)},$$

$$b_2(q)=(\epsilon _1+\epsilon _0)(\epsilon _s+\epsilon _0)+(\epsilon _1+\epsilon _0)(\epsilon _s\epsilon _0)e^{(2qd)},$$

$`b_3(q)=(\epsilon _1\epsilon _0)(\epsilon _s\epsilon _0)e^{(2qa)}+(\epsilon _1\epsilon _0)(\epsilon _s+\epsilon _0)\times `$ (2)
$`\times e^{[2q(a+d)]},`$ (3)
where the absorption coefficient $`\mathrm{\Gamma }`$ is expressed in dB/cm; $`K^2`$ is the piezoelectric constant of $`LiNbO_3`$; $`q`$ and $`V`$ are the wave vector and the velocity of SAW, respectively; $`a`$ is the distance between the dielectric and the heterostructure under consideration; $`d`$ is the depth of the position of the 2D electron-gas layer; $`\epsilon _1`$, $`\epsilon _0`$ and $`\epsilon _s`$ are the permittivities of lithium niobate, vacuum, and gallium arsenide, respectively; and $`\sigma _1`$ and $`\sigma _2`$ are the components of the complex high-frequency electri-cal conductivity of 2D electron gas: $`\sigma =\sigma _1i\sigma _2`$. The necessity of considering both components of high-frequency conductivity was demonstrated in  and was related to localization of electrons under the conditions of IQHE. These formulas make it possible to determine $`\sigma _1`$ and $`\sigma _2`$ from the quantities $`\mathrm{\Gamma }`$ and $`\mathrm{\Delta }V/V`$ measured experimentally.

Figure 2 shows the dependences of $`\sigma _1`$ and $`\sigma _2`$ on the strength of high-frequency electric field $`E`$ accompanying the SAW for the sample with $`n=1.3\times 10^{11}cm^2`$ and the filling numbers $`\nu `$ = 2 and 1. It can be seen from Fig. 2 that, for $`\nu `$ = 2 (orbital splitting), $`\sigma _1`$ and $`\sigma _2`$ initially increase with increasing electric field and, beginning with a certain $`E`$, $`\sigma _2`$ decreases rapidly while $`\sigma _1`$ continues to increase. In magnetic fields corresponding to the spin splitting ($`\nu `$ = 1), $`\sigma _1`$ increases and $`\sigma _2`$ decreases with increasing $`E`$.

Figure 3 shows the dependences of $`\sigma _1`$ and $`\sigma _2`$ on the strength of high-frequency electric field E for the sample with $`n=2.7\times 10^{11}cm^2`$ for the filling numbers of $`\nu `$= 2; 4 and 6. It can be seen from Fig. 3 that, in the magnetic field $`H`$ amounting to 5.5T ($`\nu `$=2), both components of high-frequency conductivity are independent of $`E`$ in a wide range of electric fields; for fields higher than a certain value $`E_1`$ these components increase with $`E`$. In a magnetic field of $`H`$ = 2.7 T ($`\nu `$= 4), an increase in $`\sigma _1`$ and $`\sigma _2`$ sets in an electric field $`E_2<E_1`$, and, for $`H`$ = 1.8T ($`\nu `$ = 6), $`\sigma _2`$ increases initially with increasing $`E`$, attains a maximum, and then decreases (similarly to what is shown in Fig. 2 for $`H`$= 2.7 T in the case of $`\nu `$ = 2).

The high-frequency electric field of SAW is calculated here with the formula reported in Ref. . The only difference is that we have $`\sigma =\sigma _1i\sigma _2`$ i.e.,

$`|E|^2=K^2{\displaystyle \frac{32\pi }{V}}(\epsilon _1+\epsilon _0){\displaystyle \frac{zqe^{(2q(a+d))}}{(1+\frac{4\pi \sigma _2}{\epsilon _sV}t)^2+(\frac{4\pi \sigma _1}{\epsilon _sV}t)^2}}W,`$ (4)
$`z=[(\epsilon _1+\epsilon _0)(\epsilon _s+\epsilon _0)e^{(2qa)}(\epsilon _1\epsilon _0)`$ (5)
$`\times (\epsilon _s\epsilon _0)]^2,`$ (6)
In order to explain the above dependences of $`\sigma _1`$ and $`\sigma _2`$ on E, we should rely on the fact that, as was shown in Ref. , electrical conduction in the temperature range of $`T`$= 1.5-4.2 K is simultaneously governed by the following two mechanisms: (i) the Arrhenius-type mechanism related to activation of charge carriers from the Fermi level, where these carriers are in localized states, to the percolation level and (ii) the mechanism of hop-ping over localized states in the vicinity of the Fermi level. For $`T`$ = 1.5 K, the contributions of these two mechanisms vary in relation to the filling number (the magnetic field). The smaller the filling number (the higher the magnetic field), the larger the activation energy defined by the value of $`0.5\mathrm{}\omega _c`$ ($`\omega _c`$ is the cyclotron frequency) and the smaller the Arrhenius contribution to the conductivity. In the case of hopping high-frequency conduction, the imaginary component has the value of $`\sigma _210\sigma _1\sigma _1`$  and begins to decrease with an increasing number of delocalized electrons as a result of the activation process. Thus, the ratio $`\sigma _1/\sigma _1`$ is a quantity characterizing the contribution of the above two mechanisms to conduction: if $`\sigma _1/\sigma _11`$, the hopping conduction is dominant, whereas, if $`\sigma _1/\sigma _11`$, the Arrhenius-law conduction is dominant and the hop-ping conduction may be ignored.

In view of the above, the nonlinearities should be analyzed separately for two different domains.

### A Nonlinearities in the Region of Arrhenius-Type Conduction ($`\sigma _1/\sigma _21`$)

The influence of a strong constant electric field on electrical conductivity stemming from activation of charge carriers to the percolation level of the conduction band distorted by random fluctuation potential of charged impurities was considered by Shklovskii in Ref. . In fact, we study here the influence of a strong electric field on conduction over the percolation level, with the role of the electric field limited to a reduction of activation energy, which may be interpreted as a lowering of the percolation threshold.

In this case, an increase in electrical conductivity in a strong electric field with decreasing activation energy is given by

$$\sigma _1/\sigma _1^0=exp[(CeElV_0)^{1/(1+\gamma )}/kT],$$
(7)
where $`\sigma _1^0`$ is the conductivity in the linear mode, $`E`$ is the electric field strength, $`T`$ is temperature, is a numerical coefficient, $`V_0`$ is the amplitude of fluctuations in the potential-relief pattern (the characteristic spatial scale of a potential), and $`\gamma `$ is the coefficient that depends on dimensionality: $`\gamma `$= 0.9 for the three-dimensional (3D) case and $`\gamma `$= 4/3 for the 2D case .

Thus, in the 2D case under consideration, formula 7 can be rewritten as

$$\sigma _1/\sigma _1^0=exp(\alpha E^{3/7}/kT),$$
(8)
where

$$\alpha =(Cel_{sp}V_0)^{3/7},$$
(9)
and $`l_{sp}`$ is the characteristic spatial scale of the potential, which may be taken as equal to the spacer thickness  in the heterostructures we studied ($`l_{sp}=4\times 10^6cm`$).

In the experiment we performed, the following conditions were satisfied:

$$ql_{sp}1,\omega \tau 1.$$
(10)
Here, $`q`$ and $`\omega `$ are the wave vector and frequency of SAW, respectively, and $`\tau `$ is the electron-momentum relaxation time. Therefore, we may regard the wave as standing and we can use the formulas obtained for the constant electric field in the analysis of dependences of high-frequency conductivity on the alternating SAW electric field.

Figure 4 shows the dependences of $`\sigma _1/\sigma _2`$ on electric-field strength $`E`$ calculated according to 4 for two samples in different magnetic fields. It can be seen from Fig. 4 that the condition $`\sigma _1/\sigma _2`$ is met for sample AG106 alone; therefore, the dependences $`\sigma _1/\sigma _1^0`$ on $`E`$ can be analyzed on the basis of  only for this sample. Figure 5 shows the dependence of $`\mathrm{ln}\sigma _1/\sigma _1^0`$ on $`E^{3/7}`$. It can be seen that the dependence is linear; the slope of the corresponding straight line makes it possible to determine (to within a numerical factor) $`V_0`$ i.e., the amplitude of fluctuations in the potential relief pattern. We found that $`V_01.5meV`$.

Calculation of the fluctuation amplitude by the formula

$$V_0=(e^2/\epsilon _s)/\sqrt{n},$$
(11)
where $`n`$ is the density of ionized impurities equal in our case to the carrier density in the 2D channel with $`n=1.3\times 10^{11}cm^2`$ yields $`V_0`$ = 4.5 meV, which coincides by an order of magnitude with $`V_0`$ determined experimentally to within a numerical factor.

It is stated in Ref.  that the electric-field range in which formula 7 is valid is limited by the inequalities

$$V_0eEl_{sp}kT(kT/V_0)^{4/3}.$$
(12)
Using the experimental value of $`V_0`$, we can estimate the quantities in this inequality:

$`1.5meV3\times 10^3meV5\times 10^3meV`$ at the threshold of nonlinearities; and

$`1.5meV7\times 10^3meV>5\times 10^3meV`$ at the upper limit in our measurements.

Taking into account that the fluctuation amplitude is determined to within a numerical factor, we may consider that the inequality holds and we can use the theory  to interpret nonlinearities arising in the case where the conductivity obeys the Arrhenius law.

It is worth noting here that the nonlinearities under a constant electric field $`E`$ were studied for $`E>`$ 5-10 V/cm.

The results reported here were obtained for electric fields lower than 2 V/cm. Thus, the following general pattern emerges. In electric fields $`E`$ 1 V/cm corresponding to the prebreakdown region, electrical conductivity increases owing to an increase in concentration in the empty Landau band due to activation of localized electrons from the Fermi level; in this case, the activation energy depends on the electric field (the higher the electric field, the lower the activation energy). In electric fields $`E`$ 10 V/cm, a sharp increase in electron concentration in the empty Landau band due to the impurity breakdown sets in (this phenomenon was clearly observed, for example, in Ref. ). Electrons brought into delocalized states of the Landau band are heated in a strong electric field applied to the sample.

### B Nonlinearities in the Region of High-Frequency Hopping Conduction ($`\sigma _1/\sigma _20.1`$)

In the case of electrical conductivity limited by activation, we could use the nonlinearity theory developed for constant fields to interpret the nonlinearities in high-frequency conductivity, because this theory described the influence of a strong electric field on the motion of quasi-free electrons activated to the percolation level. The mechanism of conduction in a constant electric field and that in a high-frequency field are found to be the same. However, in the case where the electrons are localized, the mechanisms of high-frequency hopping conduction and dc hopping conduction are different: in the dc mode, the conduction is accomplished by hops of electrons between two edges of the sample, whereas, in a high-frequency electric field with electrons localized at separate impurity atoms, conduction can be effected by hops of electrons between two impurity atoms separated by a distance smaller than the average one (within an impurity pair with a single electron); in this case, transitions of electrons between different pairs do not occur (a neighbor-site model). Therefore, it is understandable that the theory developed for nonlinearities in the mode of dc hopping conduction  cannot be used to interpret the nonlinearities we observed in high-frequency hopping conduction (Figs. 2,3).

The dependences of resistivities $`\rho _{xx}`$ and $`\rho _{xy}`$, on the current density in a GaAs/AlGaAs heterostructure were observed under the IQHE conditions in the region of variable-range hopping conduction at $`T<`$1K . These dependences were analyzed using the theory  for variable-range hopping conduction in a strong electric field for 2D electron gas under conditions of the quantum Hall effect. An introduction of effective temperature for hopping conduction in terms of Ref.  makes it possible to use the above measurements to determine the value of localization length. However, it was found that the value thus obtained was by almost an order of magnitude larger than the localization length deter-mined from the temperature dependence of $`\rho _{xx}`$ in a linear conduction mode. This fact was related  to non-uniformity in the distribution of the electric field.

The theory of nonlinear high-frequency electrical conduction was developed in Ref.  for the 3D case. However, the dependences $`\mathrm{\Delta }\sigma _{1,2}^{nl}/\sigma _{1,2}^0W^2`$ we observed are stronger than those predicted in Ref.  ($`\mathrm{\Delta }\sigma W`$). Here, $`\sigma _{1,2}^0`$ is the conductivity in linear mode, $`\mathrm{\Delta }\sigma _{1,2}^{nl}=\sigma _{1,2}(E)\sigma _{1,2}^0`$, $`\sigma _{1,2}(E)`$ is the conductivity measured experimentally, and $`W`$ is the SAW power absorbed in the sample. At present, the absence of a theory for the 2D case prevents us from analyzing the obtained results. The dependences of or,$`\sigma _1`$ and $`\sigma _2`$ on the SAW electric field under conditions of hopping conduction set in under the electric field, which becomes lower as the magnetic-field increases; this fact is qualitatively well explained by assuming that the magnetic field affects the overlap integral for localized states at different impurities and, thus, brings about a depression of hopping conduction and a decrease in the relative nonlinear component .

Dependence of absorpitivity of SAW by 2D electron gas on the SAW power in GaAs/AlGaAs heterostructures was previously observed  in magnetic fields corresponding to small integer filling numbers when the Fermi level was in midposition between the neighboring Landau levels and when the electrons were localized. However, it is hardly possible to accept the interpretation  of these dependences as due to the heating of 2D electron gas, which, as was mentioned above, manifests itself only in the case where the electrons in 2D configuration are delocalized.

## IV Conclusion

We studied nonlinear dependences of absorptivity and variation in the SAW velocity induced by 2D electron gas on the intensity of sound under the conditions of the integer quantum Hall effect in GaAs/AlGaAs heterostructures.

The nonlinearities were analyzed on the basis of high-frequency electrical conductivity that had a complex form and was calculated from experimental data.

It is shown that the electric-field range corresponding to nonlinearities can be divided into two domains.

In the electric-field domain where $`Re\sigma =\sigma _1Im\sigma =\sigma _2`$, The dependence $`\sigma _1(E)`$ is not only adequately accounted for by the Shklovskii dc nonlinearity theory  describing the influence of a strong electric field on the motion of quasi-free electrons activated to the percolation level, but also makes it possible to evaluate the magnitude of the fluctuation impurity potential.

In the electric-field domain where $`Im\sigma =\sigma _2Re\sigma =\sigma _1`$. the 2D high-frequency hopping conduction apparently takes place; as of yet, the nonlinearity theory for this type of conduction has not been developed.

## V Acknowledgments

We thank V.D. Kagan for his helpful participation in discussions of the results.

This work was supported by the Russian Foundation for Basic Research (project No. 98-02-18280) and the Ministry of Science (project No. 97-1043).