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# X-ray Dichroism in Noncentrosymmetryc crystals

## I Introduction

### I.1 Pure electric transitions

Near-edge x-ray dichroism with synchrotron radiation is a powerful probe of electronic states in crystals. As is known, its effectiveness stems from two prominent features of inner-shell excitations

* site selectivity, resulting from the tuning of the x-ray energy at a given inner-shell threshold;
* electron angular momentum resolution, as enforced by the selection rules of pure electric multipole (E1, E=2, …) transitions, which raise an inner-shell electron to empty valence orbitals.

Linear or circular polarisations are employed in experiments, leading to linear or circular x-ray dichroism, respectively. The former implies a difference between radiations with linear polarisations parallel or perpendicular to a local symmetry axis and is sensitive to charge anisotropies. The latter measures the difference in absorption between right and left circularly polarised radiations and reflects magnetic properties of crystals.

Following the pioneering work of Templeton and Templeton TT80  and Schütz and coworkers Sch87 , a number of authors have recorded x-ray dichroic signals in a variety of samples, ranging across the periodic table from 3d transition metals to actinides.

In parallel with this experimental activity, theory has aimed at identifying the microscopic origin of the observed spectra. Working within an atomic model Tho92 ; Car93a ; Car93b  (a good approximation, as it was later demonstrated BCA00 ) a set of sum rules was obtained, which relate integrated dichroic intensities to the ground-state expectation value of effective one-electron operators (irreducible tensors) Note1 . Two classes of operators are obtained, which are identified by their transformation properties under space inversion ($`𝐱𝐱`$, $`I`$-transformation) and time reversal ($`tt`$, $`R`$-transformation). They correspond to charge ($`I`$-even, $`R`$-even) and magnetic ($`I`$-even, $`R`$-odd) order parameters of crystals. X-ray dichroism is thus sensitive to long-range crystalline orderings; and these are distinguished by photon polarisation and by the nature (E1 or E2) of the inner-shell excitation. Undoubtedly, the most important result of this theoretical analysis has been to show that, in a ferromagnet (or ferrimagnet), x-ray circular dichroism provides a direct and independent determination of orbital and spin contributions to the magnetic moment Tho92 ; Car93a .

It is important to observe that pure electric multipole transitions cannot probe electronic properties which stem from the breaking of space inversion: all order parameters revealed by pure E1 and E2 transitions are even under the transformation $`I`$.

### I.2 Interference

In the x-ray region, other classes of dichroic phenomena have recently been investigated by Goulon et al. who reported the observation of three effects:

* X-ray natural circular dichroism (XNCD), probed in Na3Nd(digly)$`{}_{3}{}^{}`$2NaBF$`{}_{4}{}^{}`$6H2O Ala98  and in $`\alpha `$-LiIO3 Gou98 . (The effect was observed near the Nd $`L_3`$ edge and near the iodine $`L`$ edges.)
* X-ray nonreciprocal linear dichroism (XNLD), detected near the vanadium $`K`$ edge in the low-temperature insulating phase of a Cr-doped V2O3 crystalGou00 .
* X-ray magnetochiral dichroism (XM$`\chi `$D), observed at the cromium K edge Gou02  in crystalline Cr2O3.

Here, inner-shell excitations are ascribed to the E1-E2 interference; detecting a nonvanishing signal thus requires an ordered structure and the breaking of space inversion.

In our view, the work of Goulon and his collaborators is of particular importance as it identifies new directions in the microscopic analysis of materials using x-ray absorption spectroscopy. In fact, symmetry considerations indicate that XNCD, XNLD and XM$`\chi `$D are sensitive to polar and magnetoelectric (ME) properties of crystals.

It is immediately obvious that the microscopic theory of integrated spectra previously mentioned does not apply to the E1-E2 interference. Broader symmetry considerations are required to identify order parameters probed by x-ray natural and non-reciprocal dichroism. Such an analysis is outlined in the current work. Our discussion will be restricted to spectra integrated over the energy range corresponding to the two partners of a spin-orbit split inner shell: $`j_\pm =l_c\pm \frac{1}{2}`$, where $`l_c`$ denotes the angular momentum of the inner electron. Only orbital degrees of freedom (no spin) are observed in this case.

It will be shown that the E1-E2 interference is described by $`I`$-odd microscopic operators, revealing the presence of parity nonconserving interactions. (We remind the reader that the expectation value of an $`I`$-odd operator vanishes in any state of definite parity.) As in the case of pure electric multipole transitions, such operators are further distinguished by their behaviour under time reversal. Two classes of order parameters are therefore identified

* $`R`$-even and $`I`$-odd operators corresponding to one-electron polar properties, which arise from a noncentrosymmetric distribution of charge.
* $`I`$-odd and $`R`$-odd operators, obviously invariant under the combined symmetry $`RI`$ and thus describing one-electron ME properties of crystals Dzy60 .

It is thus readily seen that E1-E2 x-ray dichroism is sensitive to additional charge and magnetic orderings, which manifest themselves when the crystal lacks space-inversion symmetry.

For convenience of the reader, a classification of order parameters as probed by various x-ray dichroisms is provided in Table 1. \[Notice that a class may contain more than one order parameter, as illustrated by the following example. Consider pure E2 absorption. Four irreducible tensors of rank $`k=0,1,\mathrm{},4`$ contribute to the integrated spectrum, for arbitrary polarisation Car93b . In this case, magnetic circular dichroism selects two order parameters: a vector ($`k=1`$) and an octapole ($`k=3`$).\]

## II E1-E2 x-ray dichroism

This Section discusses general features of E1-E2 x-ray absorption. As we have anticipated, we will consider integrated spectra and express them as a linear combination of ground-state expectation values of one-electron irreducible tensors (order parameters). These order parameters are obtained by implementing Racah-Wigner recoupling techniques VMK88 , a convenient framework for dealing with the angular part of matrix elements. The ensuing results will then be applied to x-ray natural and nonreciprocal dichroism. Our discussion focusses on the physical interpetation of dichroic spectra; algebraic details of the derivation will be given in an appendix.

### II.1  Space-odd order parameters

Central to our considerations is the absorption cross section

$$\sigma ^\mathit{ϵ}(\omega )=4\pi ^2\alpha \mathrm{}\omega [\frac{i}{2}\underset{f}{}\underset{\iota \iota ^{}}{}g\mathit{ϵ}^{}𝐫_\iota ff\mathit{ϵ}𝐫_\iota ^{}𝐤𝐫_\iota ^{}g+\mathrm{c}.\mathrm{c}.]\delta (E_fE_g\mathrm{}\omega ),$$
(1)
picking out the E1-E2 interference in the $`𝒑𝑨`$ interaction between x rays and and electrons. The notation is as follows: $`\mathrm{}\omega `$, $`𝐤`$ and $`\mathit{ϵ}`$ represent energy, wave vector and polarisation of the photon; $`g`$ and $`f`$ denote ground and final states of the electron system, with energies $`E_g`$ and $`E_f`$ respectively; electrons are labelled by $`\iota `$ and $`\iota ^{}`$; $`\alpha =e^2/\mathrm{}c`$.

The integrated intensityNote14 .

$$_{j_{}+j_+}\frac{\sigma ^\mathit{ϵ}(\omega )}{(\mathrm{}\omega )^2}d(\mathrm{}\omega ),$$
(2)
expands into a linear combinations of pairs of irreducible tensors of increasing rank, $`\mu =1,2,3`$. Each pair is given by the scalar product between a wave-vector and polarisation response (geometrical factor) and the ground-state expectation value of an effective one-electron operator

$$\underset{q}{}T_q^{(\mu ,\pm )}(\mathit{ϵ},\widehat{𝐤})g|𝒪_q^{(\mu ,\pm )}(l,l^{})|g.$$

In the second quantisation formalism, the latter is defined by

$$\underset{\iota }{}𝒪_q^{(\mu ,\pm )}(l,l^{})_\iota =\underset{mm^{}}{}l^{}m^{}|𝒪_q^{(\mu ,\pm )}|lma_{l^{}m^{}}^{}a_{lm}+\mathrm{c}.\mathrm{c}.,$$
(3)
where $`l^{}=l\pm 1`$ and $`|lm`$ stands for a spherical harmonic; $`a_{lm}^{}`$ and $`a_{l^{}m^{}}`$ create and annihilate valence electrons. All $`𝒪^{(\mu ,\pm )}(l,l^{})`$ are odd under space inversion; their behaviour (even or odd) under time reversal is denoted by the superscript $`\pm `$.

Four operators $`𝒪^{(\mu ,\pm )}`$ contribute to the E1-E2 absorption spectrum for arbitrary polarisation. They can all be written out in terms of three dimensionless order parameters: the familiar orbital angular momentum $`𝑳`$, an electric dipole $`𝒏=𝐫/r`$, and $`𝛀=(𝒏\times 𝑳𝑳\times 𝒏)/2`$, a ME vector.

By applying suitable recoupling transformations to Eq. (1), we obtain

$$𝒪^{(1,)}=𝛀,𝒪^{(2,+)}=[𝑳,𝛀]^{(2)},𝒪^{(2,)}=[𝑳,𝒏]^{(2)}\mathrm{and}𝒪^{(3,)}=[[𝑳,𝑳]^{(2)},𝛀]^{(3)},$$
(4)
where the couplings are defined via Clebsch-Gordan coefficients

$$[U^{(p)},V^{(\kappa )}]_q^{(k)}\underset{\mu ,\nu }{}C_{p\mu ;\kappa \nu }^{kq}U_\mu ^{(p)}V_\nu ^\kappa .$$

Equations (4) identify one-electron properties revealed by E1-E2 absorption in the x-ray domain. The corresponding geometrical factors are given in Table 2. \[As $`T^{(1,+)}(\mathit{ϵ},\widehat{𝐤})=T^{(3,+)}(\mathit{ϵ},\widehat{𝐤})0`$, the polar moments $`𝒪^{(1,+)}=𝒏`$ and $`𝒪^{(3,+)}=[[𝑳,𝑳]^{(2)},𝒏]^{(3)}`$ do not contribute to expression (2).\]

Our derivation is based on a localised model, which considers a single ion with a partially filled valence shell; all other shells filled. Inclusion of spin-orbit interactions and/or crystal fields results in a deformation of the electronic cloud. Its multipolar expansion will contain spin and orbital moments characteristic of the symmetry of the deformation and described by one-particle irreducible tensors. Valence states are hybridised in general, with the orbital part given as a superposition of two angular momenta: $`l`$ and $`l^{}=l\pm 1`$, corresponding to $`sp`$ or $`pd`$ hybridisation in the actual case. (In our formalism, valence electrons are labelled using uncoupled orbital and spin quantum numbers.)

As shown in previous work Tho92 ; Car93a ; Car93b , integrated dichroic spectra which stem from pure E1 or E2 transitions provide a measure of the ground-state expectation value of $`I`$-even irreducible tensors. Only the diagonal part (in the sense of $`\delta _{l,l^{}}`$) contributes to the ground-state matrix elements in this case. Angular momentum and parity are good quantum numbers; the known sum rules for linear and circular dichroism are recovered Note3 .

Integrated E1-E2 dichroic spectra are related to the ground-state expectation value of $`I`$-odd irreducible tensors. Only the off-diagonal part contributes to the ground-state matrix elements, in this case. Orbital angular momentum is not a good quantum number and electron states do not have definite parity. Hybridisation effects are now observable and described by the operators $`𝒪^{(\mu ,\pm )}`$.

Relations between XNCD, XNLD, XM$`\chi `$D and the order parameters given by Eqs. (4) will be provided below.

### II.2 Interpretation of experiments

#### II.2.1 XNCD

In this case, a recoupling of Eq. (1) leads to the following integral relation

$$_{j_{}+j_+}\frac{\sigma _\mathrm{X}^{\mathit{ϵ}^+}(\omega )\sigma _\mathrm{X}^\mathit{ϵ}^{}(\omega )}{(\mathrm{}\omega )^2}d(\mathrm{}\omega )=\frac{16\pi ^2\alpha }{3\mathrm{}c}(2l_c+1)\underset{\genfrac{}{}{0pt}{}{l=l_c\pm 1}{l^{}=l\pm 1}}{}\underset{\iota ,q}{}R_{l_cl}^{(1)}R_{l_cl^{}}^{(2)}a_l^{}^{(2,+)}(l_c,l)\sqrt{\frac{3}{2}}T_q^{(2,+)}(\mathit{ϵ}^{},\mathit{ϵ}^+,\widehat{𝐤})g|[𝑳_\iota ,𝛀_\iota ]_q^{(2)}(l,l^{})|g,$$
(5)
which reveals the microscopic origin of XNCD spectra. Here, $`\mathit{ϵ}^\pm =(i/\sqrt{2})(\mathit{ϵ}_1\pm i\mathit{ϵ}_2)`$ define circular polarisation states; the index $`\iota `$ runs over valence electrons Note4 . Furthermore,

$$a_l^{}^{(2,+)}(l_c,l)=\frac{2(2l+1)(2l^{}+1)[6+3l_c(l_c+1)2l(l+1)l^{}(l^{}+1)]}{(l+l^{}+1)(l_c3l^{}+2l)(l_c+3l^{}2l+1)(l_c+l)^2(l_c+l+2)^2}.$$
(6)
The XNCD experiment of Goulon et al. on $`\alpha `$-LiIO3 Gou98 , whose crystal structure (space group $`P6_3`$) is depicted in Fig. 1, is readily interpreted with the help of Eq. (5).

We focus on charge properties stemming from $`sp`$ hybridisation. (The $`4d`$ shell of iodine is filled and the crystal displays no magnetism.) At the iodine sites the symmetry is $`C_3`$. Notice that $`𝒪^{(2,+)}=[𝑳,𝛀]^{(2)}`$, known as pseudodeviator or gyration tensor, is totally symmetric in this point group i.e., it is invariant under all $`C_3`$ transformations. It yields therefore a nonvanishing ground-state expectation value at each iodine site. The threefold axes of all the iodate groups are parallel in the unit cell of $`\alpha `$-LiIO3 ($`P6_3`$ is noncentrosymmetric). As a consequence, all the microscopic pseudodeviators add up upon absorption of circularly polarised x rays. This contribution to the E1-E2 absorption profile is selected by circular dichroism (see Table 2) yielding the observed XNCD spectrum. The effect can thus be viewed as the $`I`$-odd analog of ferroquadrupolar ordering, which is probed by pure E1 x-ray linear dichroism Car93b .

#### II.2.2 XNLD

In the case of XNLD, the integral relation reads

$`{\displaystyle _{j_{}+j_+}}{\displaystyle \frac{\sigma _\mathrm{X}^{}(\omega )\sigma _\mathrm{X}^{}(\omega )}{(\mathrm{}\omega )^2}}d(\mathrm{}\omega )={\displaystyle \frac{8\pi ^2\alpha }{\mathrm{}c}}(2l_c+1){\displaystyle \underset{\genfrac{}{}{0pt}{}{l=l_c\pm 1}{l^{}=l\pm 1}}{}}R_{l_cl}^{(1)}R_{l_cl^{}}^{(2)}{\displaystyle \underset{q}{}}\{\sqrt{{\displaystyle \frac{2}{3}}}a_l^{}^{(2,)}(l_c,l)i(T_q^{(2,)}(\mathit{ϵ}^{},\widehat{𝐤})T_q^{(2,)}(\mathit{ϵ}^{},\widehat{𝐤}))`$
$`g|{\displaystyle \underset{\iota }{}}[𝑳_\iota ,𝒏_\iota ]_q^{(2)}(l,l^{})|g2a_l^{}^{(3,)}(l_c,l)(T_q^{(3,)}(\mathit{ϵ}^{},\widehat{𝐤})T_q^{(3,)}(\mathit{ϵ}^{},\widehat{𝐤}))g|{\displaystyle \underset{\iota }{}}[[𝑳_\iota ,𝑳_\iota ]^2,𝛀_\iota ]_q^{(3)}(l,l^{})|g\},`$ (7)
where $``$ and $``$ denote two orthogonal linear-polarisation states. The expansion coefficients are given by

$$a_l^{}^{(3,)}(l_c,l)=\frac{a_l^{}^{(2,+)}(l_c,l)}{6+3l_c(l_c+1)2l(l+1)l^{}(l^{}+1)}$$
(8)
and

$$a_l^{}^{(2,)}(l_c,l)=\frac{(l+l^{}+1)(l^{}l)}{2}a_l^{}^{(2,+)}(l_c,l),$$
(9)
with $`a_l^{}^{(2,+)}(l_c,l)`$ defined by Eq. (6).

Equation (7) reveals the microscopic ME nature of XNLD. (Notice the peculiarity of this form of linear dichroism: it changes sign upon reversal of an external applied magnetic fieldNote17 . The result implies that Goulon and his co-workers have probed ME properties of (V1-xCrx)2O3.

V2O3 is characterised by a strongly destructive first-order transition from a paramagnetic metallic phase (corundum structure) to an antiferromagnetic (AFM) insulating phase (monoclinic) at T$`{}_{N}{}^{}150^{}`$K. The unit cells of pure V2O3 are depicted in Fig. 2.

Substitution of Cr3+ in the V2O3 lattice results in a Mott metal-to-insulator transition. At room temperature, charge properties of the compound can be deduced from structural studies, which have been reported by Dernier and Marezio DaM70 ; Der70 . These authors ascribe the Cr-induced metal-to-insulator transition to an increase in the nearest neighbour vanadium-vanadium distances, which is accompanied by an ’umbrella-like’ distortion of the oxygen octahedra. Crystal-structure refinements indicate that at each vanadium site the point group is C3v Der70 . Formation of an electric-dipole moment is thus permitted by symmetry. Crystallography also suggests that nearest-neighbour pairs of vanadium atoms are antiferroeletrically ordered along the hexagonal c axis (the symmetry of a pair is D3h Der70 ), as shown in Fig. 3. We can thus argue that, at about $`300^{}`$K in the insulating phase, (V1-xCrx)2O3 is an antiferroelectric (AFE) crystal Note19 .

At $`T=T_N`$, the crystal makes a nearly second-order transition to an AFM monoclinic phase Mon70 . The driving mechanism of this transition is not fully understood Yet87 . The lattice space group lowers to $`I2/a`$, with magnetic point group $`C_{2h}R`$ DiM02 . Notice that this symmetry is incompatible with the observation of XNLD. However, a reduction of magnetic symmetry leading to $`C_{2h}(C_{1h})`$ or $`C_{2h}(C_2)`$ might take placeNote20 .

A lowering of magnetic symmetry could occur as follows. The structural change to the monoclinic phase eliminates the three-fold axis, which characterises the corundum structure. It probably involves a co-operative Jahn-Teller distortion, which tilts the electric moments. A tilting with the pattern depicted in Fig. 4 would render (V1-xCrx)2O3 an AFM, AFE, and ME crystal, thus explaining the observations of Goulon and his collaborators.

A physical interpretation of Eq. (7) is obtained by expanding the ”energy” function $`W(𝒏,𝑳)`$Bar82 . The $`m`$th term in the MacLaurin formula reads: $`\frac{1}{m!}\left(n_\alpha _{n_\alpha }+L_\beta _{L_\beta }\right)^mW(0,0);`$ here, greek letters denote cartesian components and repeated indexes are summed over. It is readily seen that $`[𝑳,𝒏]^{(2)}`$ stems from the $`m=2`$ term and describes a linear ME effect. The contribution $`[[𝑳,𝑳]^2,𝛀]^{(3)}`$ is found in the $`m=4`$ term and accounts for a trilinear ME effect.

#### II.2.3 XM$`\chi `$D

The third form of E1-E2 x-ray dichroism, namely XM$`\chi `$D, was probed by Goulon and co-workers Gou02  at the cromium K-edge in Cr2O3 by implementing a new experimental technique: the dichroism of unpolarised x rays. A microscopic description of this spectroscopy, which is readily obtained from our theory of integrated spectra, is reported in the current subsection.

As is known Car93b , the following integral relationship holds for pure E1 transitions

$$_{j_++j_{}}\frac{(\sigma ^{\mathit{ϵ}^+}+\sigma ^\mathit{ϵ}^{})_{E1}}{(\mathrm{}\omega )^2}d(\mathrm{}\omega )=4\pi ^2\alpha \underset{l}{}\left[\frac{2}{3}\frac{n_h(l)}{2l+1}+b^{(2,+)}(l_c,l)g|\underset{\iota }{}(3L_z^2𝑳^2)_\iota |g\right][P_{l_cl}^{(1)}]^2,$$
(10)
where $`n_h(l)=4l+2g|n|g`$ denotes the number of holes in the valence $`l`$ shell, and $`P_{l_cl}^{(1)}=c\sqrt{4\pi /3}𝐘^{(1)}lR_{l_c,l}^{(1)}`$. Furthermore,

$$b^{(2,+)}(l_c,l)=\frac{l(l+1)[3l(l+1)+16l_c(l_c+1)]+3l_c(l_c+1)[l_c(l_c+1)3]}{6l(2l1)(2l+1)(l+1)(2l+3)}$$
(11)
In the case of a magnetoelectric crystal, E1-E2 corrections to Eq. (10) need to be taken into account. They read

$`{\displaystyle _{j_++j_{}}}{\displaystyle \frac{(\sigma ^{\mathit{ϵ}^+}+\sigma ^\mathit{ϵ}^{})_{E1E2}}{(\mathrm{}\omega )^2}}d(\mathrm{}\omega )`$ $`=`$ $`{\displaystyle \frac{2\pi ^2\alpha }{\mathrm{}c}}(2l_c+1){\displaystyle \underset{\genfrac{}{}{0pt}{}{l=l_c\pm 1}{l^{}=l\pm 1}}{}}R_{l_cl}^{(1)}R_{l_cl^{}}^{(2)}[{\displaystyle \frac{2}{5}}a_l^{}^{(1,)}(l_c,l)k_zg|{\displaystyle \underset{\iota }{}}𝛀_\iota (l,l^{})_z|g`$ (12)
$``$ $`{\displaystyle \frac{16}{\sqrt{10}}}a_l^{}^{(3,)}(l_c,l)k_zg|{\displaystyle \underset{\iota }{}}[[𝑳_\iota ,𝑳_\iota ]^2,𝛀_\iota ]_z^{(3)}(l,l^{})|g]`$
with

$$a_l^{}^{(1,)}(l_c,l)=\frac{(l_c+l+1)(l_c+l2l^{})h_1(l_c,l,l^{})}{(l_c+l)(l_c+l+2)(l+l^{}+1)^2},$$
(13)
where $`h_1(l_c,l,l^{})=l_c+2l^{}l+1`$ and $`l^{}=l\pm 1`$. We have set $`𝐤=k_z\widehat{𝐳}`$ in Eqs. (10 \- 12).

Eqs. (10 \- 12) indicate that XM$`\chi `$D is observed as follows. Record the $`\sigma ^{\mathit{ϵ}^+}+\sigma ^\mathit{ϵ}^{}`$ spectrum in a magnetoeletric cystal annealed in the parallel configuration. Ditto for antiparallel annealing. Subtract the two spectra.

It goes without saying that such a dichroic spectrum, which is described by Eq. (12), reflects ME properties of crystals.

## III Discussion and outlook

To provide a theoretical interpretation of recent x-ray experiments, which have detected XNCD, XNLD and XM$`\chi `$D respectively in $`\alpha `$-LiIO3, (V.972Cr.028)2O3 and Cr2O3, the current paper has presented a theoretical analysis of near-edge absorption of polarised x rays in noncentrosymmetric crystals. Our work has centred on the derivation of integral relations for dichroic effects which stem from E1-E2 inner-shell excitations. Such relations are written out in terms of one-electron effective operators (order parameters), which identify crystalline microscopic properties revealed by the observed spectra. Two classes of parity-breaking order parameters have been found, which correspond to polar and magnetoelectric moments of valence electrons. Only orbital degrees of freedom have been considered in our derivation; inclusion of spin would be straightforward.

We remind the reader that two irreducible tensors, namely $`𝒪^{(1,+)}=𝒏`$ and $`𝒪^{(3,+)}=[[𝑳,𝑳]^{(2)},𝒏]^{(3)}`$ (see Section II.1), have not entered our discussion of integrated XNCD, XNLD and XM$`\chi `$D spectra. As previously observed, $`𝒪^{(1,+)}`$ and $`𝒪^{(3,+)}`$ have vanishing geometrical factors and do not appear in our coupled expansion of expression (2). They do contribute however to x-ray resonant diffaction, as can be verified by extending the work of Luo et al. Luo93  to include E1-E2 processes. (Such a lengthy derivation will not be reported here.) The result is of interest as it indicates the possibiity of detecting Bragg peaks from ferrolectric and AFE structures with x rays at resonance.

In conclusion, the pioneering experiments of Goulon and his collaborators appear to have paved the way for new investigations of electronic states in noncentrosymmetric crystals using x-ray absorption and resonant scattering. As shown by our work, a variety of one-electron properties, which result from parity-nonconserving electron interactions, can be measured, yielding valuable information in condensed matter physics and material science.

###### Acknowledgements.

Stimulating discussions with F. de Bergevin, P. J. Brown, J. Goulon, and E. Katz are gratefully acknowledged. We would like to thank S. di Matteo for pointing out an error in an earlier version of Eq. (7). We are indebted to B. G. Searle for providing the computer program that generated Fig. 1.

*

## Appendix A Symmetry Analysis

Lie groups (or, alternatively, Lie algebras) furnish a powerful tool for interpreting x-ray dichroism in non-centrosymmetric crystals. In fact, effective microscopic operators, which express electronic properties revealed by the spectra, are readily deduced from the pertinent group generators. Our approach hinges therefore on spectrum-generating algebras, a concept originally introduced in nuclear GoL59  and particle physics DGN65 ; DaN66 .

We follow Carra and BenoistCaB00  and consider the general framework of a de Sitter algebra: $`so(3,2)`$ GoL59 ; Eng72 . A realisation of such an algebra is provided by the operators:

$$𝑨^{}=i(𝑨𝑨^{})/2,𝑨^+=(𝑨+𝑨^{})/2,$$
(14)
$$𝑳\mathrm{and}N_0,$$
(15)
where $`𝑳`$ denotes the orbital angular momentum (in units of $`\mathrm{}`$) and $`N_0|lm=(l+\frac{1}{2})|lm`$, with $`|lm`$ a spherical harmonic. Furthermore,

$$𝑨=𝒏f_1(N_0)+\mathbf{}_\mathrm{\Omega }f_2(N_0),$$
(16)
with $`𝒏=𝐫/r`$, $`\mathbf{}_\mathrm{\Omega }=i𝒏\times 𝑳`$ and

$$f_1(N_0)=(N_01/2)f_2(N_0),$$
(17)
$$f_2(N_0)=\sqrt{(N_01)/N_0}.$$
(18)
$`𝑨`$ and $`𝑨^{}`$ are known as shift operators as their action on $`|lm`$ changes $`l`$ into $`l\pm 1`$.

A physical interpretation of $`𝑨^{}`$ is provided by the relation

$$𝛀=(𝒏\times 𝑳𝑳\times 𝒏)/2=i[𝒏,𝑳^2]/2=\frac{i}{2}\left(\mathbf{}_\mathrm{\Omega }\mathbf{}_\mathrm{\Omega }^{}\right)=\frac{1}{2}\frac{1}{\sqrt{N_0}}[N_0,𝑨^{}]_+\frac{1}{\sqrt{N_0}},$$
(19)
where $`[\mathrm{}]_+`$ denotes an anticommutator. Eq. (19) defines the (purely angular) orbital anapole Zel57 ; FaK80 ; BaB97 .

A physical representation of the generator $`𝑨^+`$ is provided by

$$𝑨^+=\sqrt{N_0}𝒏\sqrt{N_0}.$$
(20)
$`𝑳,𝒏`$ and $`𝛀`$ provide the building blocks of our derivation. They form a triad of mutually orthogonal dimensionless vectors. Their nature (magnetic, electric and magnetoelectric, respectively) is readily inferred from behaviour under space inversion and time reversal.

Notice that $`𝑳`$ (rotations) and $`𝛀`$ (boosts) generate a homogeneous Lorentz group: SO(3,1). Also $`𝑳`$ and $`\sqrt{N_0}𝒏\sqrt{N_0}`$, where $`N_0|lm=(l+\frac{1}{2})|lm`$, generate SO(3,1). The homogeneous Lorentz group enters our derivation of $`I`$-odd operators in a natural way, given its deep interweaving with chirality. Notice that $`𝑳`$, $`𝛀`$ and $`\sqrt{N_0}𝒏\sqrt{N_0}`$ provide a realisation of the $`so(3,2)`$ de Sitter algebra. This is the required symmetry extension, with respect to pure E1 or E2 transitions, that was mentioned in the Introduction.


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# The Rigged Hilbert Space of the Free Hamiltonian

## 1 Introduction

There is a growing realization that the Rigged Hilbert Space (RHS) provides the methods needed to handle Dirac’s bra-ket formalism and continuous spectrum. Moreover, there is an increasing number of Quantum Mechanics textbooks that include the RHS as part of their contents  (this list is non-exhaustive). However, there is still a lack of simple examples for which the RHS is explicitly constructed (one exception is Ref. ). Especially important is to construct the RHS generated by the Schrödinger equation, because claiming that Quantum Mechanics needs the RHS is tantamount to claiming that the solutions of the Schrödinger equation lie in a RHS (when continuous spectrum is present). The task of constructing the RHS generated by the Schrödinger equation was undertaken in Ref. . The method proposed in  has been applied to two simple potentials . In this paper, we shall apply this method to the simplest example possible: the free Hamiltonian.

We note that the results of this paper follow immediately from those in Refs. , by making the value of the potential zero. Nevertheless, we think that the example of the free Hamiltonian provides a very transparent way to understand the essentials of the method of , because the calculations are reduced to the minimum.

The time-independent Schrödinger equation for the free Hamiltonian $`H_0`$ reads, in the position representation, as

$$\stackrel{}{x}|H_0|E=\frac{\mathrm{}^2}{2m}^2\stackrel{}{x}|E=E\stackrel{}{x}|E,$$
(1.1)
where $`^2`$ is the three-dimensional Laplacian. In spherical coordinates $`\stackrel{}{x}(r,\theta ,\varphi )`$, Eq. (1.1) has the following form:

$$r,\theta ,\varphi |H_0|E,l,m=\left(\frac{\mathrm{}^2}{2m}\frac{1}{r}\frac{^2}{r^2}r+\frac{\mathrm{}^2l(l+1)}{2mr^2}\right)r,\theta ,\varphi |E,l,m=Er,\theta ,\varphi |E,l,m.$$
(1.2)
By separating the radial and angular dependences,

$$r,\theta ,\varphi |E,l,mr|E_l\theta ,\varphi |l,m\frac{1}{r}\chi _l(r;E)Y_{l,m}(\theta ,\varphi ),$$
(1.3)
where $`Y_{l,m}(\theta ,\varphi )`$ are the spherical harmonics, we obtain for the radial part

$$\left(\frac{\mathrm{}^2}{2m}\frac{d^2}{dr^2}+\frac{\mathrm{}^2l(l+1)}{2mr^2}\right)\chi _l(r;E)=E\chi _l(r;E).$$
(1.4)
In this paper, we shall restrict ourselves to the case of zero orbital angular momentum (the higher-order case can be treated analogously). We then write $`\chi _{l=0}(r;E)\chi (r;E)`$ and obtain

$$\frac{\mathrm{}^2}{2m}\frac{d^2}{dr^2}\chi (r;E)=E\chi (r;E).$$
(1.5)
We shall write this equation as

$$h_0\chi (r;E)=E\chi (r;E),$$
(1.6)
where

$$h_0\frac{\mathrm{}^2}{2m}\frac{d^2}{dr^2}$$
(1.7)
is the formal differential operator corresponding to the free Hamiltonian (for $`l=0`$). Our goal is to solve Eq. (1.6) and show that its solutions lie in a RHS rather than just in a Hilbert space.

The basic tool necessary to solve Eq. (1.6) is the Sturm-Liouville theory . This theory provides the Hilbert space methods. As shown in many publications (cf.  and references therein), the Hilbert space methods do not provide us with all the tools needed in Quantum Mechanics when continuous spectrum is present. In particular, the Hilbert space cannot incorporate Dirac’s bra-ket formalism. Therefore, an extension of the Hilbert space is needed. The extension that seems to be most suitable is the RHS (cf.  and references therein). In particular, the RHS incorporates Dirac’s bra-ket formalism.

The structure of the paper is as follows. In Section 2, we construct the domain and the self-adjoint extension of the differential operator (1.7). In Section 3, we obtain the free Green function, whose expression is used in Section 4 to calculate the spectrum of $`H_0`$. Section 5 is devoted to the eigenfunction expansion and the direct integral decomposition of the Hilbert space. In Section 6, we construct the RHS of $`H_0`$. The Dirac basis vector expansion for $`H_0`$ is obtained in Section 7, and the energy representation of the RHS of $`H_0`$ is constructed in Section 8. Finally, the results of the paper are summarized in the diagram of Eq. (8).

## 2 Self-Adjoint Extension

The first step is to define a linear operator on a Hilbert space corresponding to the formal differential operator (1.7). In the radial position representation, the Hilbert space that belongs to the RHS of the free Hamiltonian is realized by the space $`L^2([0,\mathrm{}),dr)`$ of square integrable functions $`f(r)`$ defined on the interval $`[0,\mathrm{})`$ (see the diagram (8) below).

The domain $`𝒟(H_0)`$ of the free Hamiltonian must be a proper dense linear subspace of $`L^2([0,\mathrm{}),dr)`$. The action of $`h_0`$ must be well defined on $`𝒟(H_0)`$, and this action must remain in $`L^2([0,\mathrm{}),dr)`$. We need also a boundary condition that assures the self-adjointness of the Hamiltonian. The boundary conditions that select the possible self-adjoint extensions of $`h_0`$ are given by (see , page 1306)

$$f(0)+\alpha f^{}(0)=0,\mathrm{}<\alpha \mathrm{}.$$
(2.1)
Among all these boundary conditions, we choose $`f(0)=0`$. Therefore, the requirements that are to be fulfilled by the elements of the domain of $`H_0`$ are

$`f(r)L^2([0,\mathrm{}),dr),`$ (2.2a)
$`h_0f(r)L^2([0,\mathrm{}),dr),`$ (2.2b)
$`f(r)AC^2[0,\mathrm{}),`$ (2.2c)
$`f(0)=0,`$ (2.2d)
where $`AC^2[0,\mathrm{})`$ denotes the space of functions whose derivative is absolutely continuous (for details on absolutely continuous functions, consult Refs. ). The requirements in Eq. (2.2) yield the domain of $`H_0`$:

$$𝒟(H_0)=\{f(r)|f(r),h_0f(r)L^2([0,\mathrm{}),dr),f(r)AC^2[0,\mathrm{}),f(0)=0\}.$$
(2.3)
On $`𝒟(H_0)`$ the formal differential operator $`h_0`$ is self-adjoint. In choosing (2.3) as the domain of our formal differential operator $`h_0`$, we define a linear operator $`H_0`$ by

$$H_0f(r):=h_0f(r)=\frac{\mathrm{}^2}{2m}\frac{d^2}{dr^2}f(r),f(r)𝒟(H_0).$$
(2.4)
## 3 Resolvent and Green Function

The expression of the free Green function $`G_0(r,s;E)`$ is given in terms of eigenfunctions of the differential operator $`h_0`$ subject to certain boundary conditions (cf. Theorem 1 in Appendix A). We shall divide the complex energy plane in three regions, and calculate $`G_0(r,s;E)`$ for each region separately. In all our calculations, we shall use the following branch of the square root function:

$$\sqrt{}:\{E|\pi <\mathrm{arg}(E)\pi \}\{E|\pi /2<\mathrm{arg}(E)\pi /2\}.$$
(3.1)
### 3.1 Region $`\text{Re}(E)<0`$, $`\text{Im}(E)0`$

For $`\text{Re}(E)<0`$, $`\text{Im}(E)0`$, the free Green function (see Theorem 1 in Appendix A) is given by

$$G_0(r,s;E)=\{\begin{array}{cc}\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\frac{\stackrel{~}{\chi }(r;E)\stackrel{~}{f}(s;E)}{2}\hfill & r<s\hfill \\ \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\frac{\stackrel{~}{\chi }(s;E)\stackrel{~}{f}(r;E)}{2}\hfill & r>s\hfill \end{array}\text{Re}(E)<0,\text{Im}(E)0.$$
(3.2)
The eigenfunction $`\stackrel{~}{\chi }(r;E)`$ satisfies the Schrödinger equation, Eq. (1.6), and the boundary conditions

$`\stackrel{~}{\chi }(0;E)=0,`$ (3.3a)
$`\stackrel{~}{\chi }(r;E)\mathrm{is}\mathrm{square}\mathrm{integrable}\mathrm{at}0,`$ (3.3b)
which yield

$$\stackrel{~}{\chi }(r;E)=e^{\sqrt{\frac{2m}{\mathrm{}^2}E}r}e^{\sqrt{\frac{2m}{\mathrm{}^2}E}r},0<r<\mathrm{}.$$
(3.4)
The eigenfunction $`\stackrel{~}{f}(r;E)`$ satisfies the Schrödinger equation, Eq. (1.6), and the boundary condition

$$\stackrel{~}{f}(r;E)\mathrm{is}\mathrm{square}\mathrm{integrable}\mathrm{at}\mathrm{},$$
(3.5)
which yield

$$\stackrel{~}{f}(r;E)=e^{\sqrt{\frac{2m}{\mathrm{}^2}E}r},0<r<\mathrm{}.$$
(3.6)
The Wronskian of $`\stackrel{~}{\chi }`$ and $`\stackrel{~}{f}`$ can be easily calculated:

$$W(\stackrel{~}{\chi },\stackrel{~}{f})=2\sqrt{\frac{2m}{\mathrm{}^2}E}.$$
(3.7)
### 3.2 Region $`\text{Re}(E)>0`$, $`\text{Im}(E)>0`$

When $`\text{Re}(E)>0`$, $`\text{Im}(E)>0`$, the expression of the free Green function is

$$G_0(r,s;E)=\{\begin{array}{cc}\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\chi (r;E)f^+(s;E)\hfill & r<s\hfill \\ \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\chi (s;E)f^+(r;E)\hfill & r>s\hfill \end{array}\text{Re}(E)>0,\text{Im}(E)>0.$$
(3.8)
The eigenfunction $`\chi (r;E)`$ satisfies Eq. (1.6) and the boundary conditions (3.3), which yield

$$\chi (r;E)=\mathrm{sin}(\sqrt{\frac{2m}{\mathrm{}^2}E}r),0<r<\mathrm{}.$$
(3.9)
The eigenfunction $`f^+(r;E)`$ satisfies Eq. (1.6) subject to the boundary condition (3.5), which yield

$$f^+(r;E)=e^{i\sqrt{\frac{2m}{\mathrm{}^2}E}r},0<r<\mathrm{}.$$
(3.10)
The expression of the Wronskian of $`\chi `$ and $`f^+`$ follows immediately from Eqs. (3.9) and (3.10):

$$W(\chi ,f^+)=\sqrt{\frac{2m}{\mathrm{}^2}E}.$$
(3.11)
### 3.3 Region $`\text{Re}(E)>0`$, $`\text{Im}(E)<0`$

In the region $`\text{Re}(E)>0`$, $`\text{Im}(E)<0`$, the free Green function reads

$$G_0(r,s;E)=\{\begin{array}{cc}\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\chi (r;E)f^{}(s;E)\hfill & r<s\hfill \\ \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\chi (s;E)f^{}(r;E)\hfill & r>s\hfill \end{array}\text{Re}(E)>0,\text{Im}(E)<0.$$
(3.12)
The eigenfunction $`\chi (r;E)`$ is given by (3.9), although now $`E`$ belongs to the fourth quadrant of the energy plane. The eigenfunction $`f^{}(r;E)`$ satisfies Eq. (1.6) and the boundary condition (3.5), which yield

$$f^{}(r;E)=e^{i\sqrt{\frac{2m}{\mathrm{}^2}E}r},0<r<\mathrm{}.$$
(3.13)
The Wronskian of $`\chi `$ and $`f^{}`$ is given by

$$W(\chi ,f^{})=\sqrt{\frac{2m}{\mathrm{}^2}E}.$$
(3.14)
## 4 Spectrum of $`H_0`$

In this section, we obtain the spectrum of $`H_0`$, which we shall denote by $`\mathrm{Sp}(H_0)`$. We know that $`H_0`$ is self-adjoint, and therefore its spectrum is real. In order to obtain the set of real numbers that belong to $`\mathrm{Sp}(H_0)`$, we apply Theorem 4 of Appendix A. From Theorem 4 and from the previous section, it is clear that we should study the positive and the negative real lines separately. As expected, we shall obtain that $`\mathrm{Sp}(H_0)=[0,\mathrm{})`$.

### 4.1 Subset $`\mathrm{\Lambda }=(\mathrm{},0)`$

We first take $`\mathrm{\Lambda }`$ from Theorem 4 of Appendix A to be $`(\mathrm{},0)`$. We choose a basis for the space of solutions of the equation $`h_0\sigma =E\sigma `$ as

$`\stackrel{~}{\sigma }_1(r;E)=e^{\sqrt{\frac{2m}{\mathrm{}^2}E}r},`$ (4.1a)
$`\stackrel{~}{\sigma }_2(r;E)=\stackrel{~}{f}(r;E).`$ (4.1b)
Obviously,

$$\stackrel{~}{\chi }(r;E)=\stackrel{~}{\sigma }_1(r;E)\stackrel{~}{\sigma }_2(r;E),$$
(4.2)
which along with Eq. (3.2) leads to

$$G_0(r,s;E)=\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\frac{1}{2}\left[\stackrel{~}{\sigma }_1(r;E)\stackrel{~}{\sigma }_2(r;E)\right]\stackrel{~}{\sigma }_2(s;E),r<s,\text{Re}(E)<0,\text{Im}(E)0.$$
(4.3)
Because

$$\overline{\stackrel{~}{\sigma }_2(s;\overline{E})}=\stackrel{~}{\sigma }_2(s;E),$$
(4.4)
we can write Eq. (4.3) as

$`G_0(r,s;E)={\displaystyle \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}}{\displaystyle \frac{1}{2}}\left[\stackrel{~}{\sigma }_1(r;E)\overline{\stackrel{~}{\sigma }_2(s;\overline{E})}\stackrel{~}{\sigma }_2(r;E)\overline{\stackrel{~}{\sigma }_2(s;\overline{E})}\right],`$
$`r<s,\text{Re}(E)<0,\text{Im}(E)0.`$ (4.5)
On the other hand, by Theorem 4 in Appendix A we have

$$G_0(r,s;E)=\underset{i,j=1}{\overset{2}{}}\theta _{ij}^{}(E)\stackrel{~}{\sigma }_i(r;E)\overline{\stackrel{~}{\sigma }_j(s;\overline{E})},r<s.$$
(4.6)
By comparing Eqs. (4.5) and (4.6) we see that

$$\theta _{ij}^{}(E)=\left(\begin{array}{cc}0& \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\frac{1}{2}\\ 0& \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\frac{1}{2}\end{array}\right),\text{Re}(E)<0,\text{Im}(E)0.$$
(4.7)
The functions $`\theta _{ij}^{}(E)`$ are analytic in a neighborhood of $`\mathrm{\Lambda }=(\mathrm{},0)`$. Therefore, the interval $`(\mathrm{},0)`$ is in the resolvent set, $`\mathrm{Re}(H_0)`$, of the operator $`H_0`$.

### 4.2 Subset $`\mathrm{\Lambda }=(0,\mathrm{})`$

In this case, we choose the following basis for the space of solutions of $`h_0\sigma =E\sigma `$:

$`\sigma _1(r;E)=\chi (r;E),`$ (4.8a)
$`\sigma _2(r;E)=\mathrm{cos}(\sqrt{{\displaystyle \frac{2m}{\mathrm{}^2}}E}r).`$ (4.8b)
Eqs. (3.10), (3.13) and (4.8) lead to

$$f^+(r;E)=i\sigma _1(r;E)+\sigma _2(r;E)$$
(4.9)
and to

$$f^{}(r;E)=i\sigma _1(r;E)+\sigma _2(r;E).$$
(4.10)
By substituting Eq. (4.9) into Eq. (3.8) we get to

$$G_0(r,s;E)=\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\sigma _1(s;E)\left[i\sigma _1(r;E)+\sigma _2(r;E)\right],r>s,\text{Re}(E)>0,\text{Im}(E)>0.$$
(4.11)
By substituting Eq. (4.10) into Eq. (3.12) we get to

$$G_0(r,s;E)=\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\sigma _1(s;E)\left[i\sigma _1(r;E)+\sigma _2(r;E)\right],r>s,\text{Re}(E)>0,\text{Im}(E)<0.$$
(4.12)
Because

$$\overline{\sigma _1(s;\overline{E})}=\sigma _1(s;E),$$
(4.13)
Eq. (4.11) leads to

$`G_0(r,s;E)={\displaystyle \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}}\left[i\sigma _1(r;E)\overline{\sigma _1(s;\overline{E})}+\sigma _2(r;E)\overline{\sigma _1(s;\overline{E})}\right],`$
$`\text{Re}(E)>0,\text{Im}(E)>0,r>s,`$ (4.14)
whereas Eq. (4.12) leads to

$`G_0(r,s;E)={\displaystyle \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}}\left[i\sigma _1(r;E)\overline{\sigma _1(s;\overline{E})}+\sigma _2(r;E)\overline{\sigma _1(s;\overline{E})}\right],`$
$`\text{Re}(E)>0,\text{Im}(E)<0,r>s.`$ (4.15)
The expression of the resolvent in terms of the basis $`\sigma _1,\sigma _2`$ can be written as (see Theorem 4 in Appendix A)

$$G_0(r,s;E)=\underset{i,j=1}{\overset{2}{}}\theta _{ij}^+(E)\sigma _i(r;E)\overline{\sigma _j(s;\overline{E})},r>s.$$
(4.16)
By comparing (4.16) to (4.14) we get to

$$\theta _{ij}^+(E)=\left(\begin{array}{cc}\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}i& \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\\ 0& 0\end{array}\right),\text{Re}(E)>0,\text{Im}(E)>0.$$
(4.17)
By comparing (4.16) to (4.15) we get to

$$\theta _{ij}^+(E)=\left(\begin{array}{cc}\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}i& \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}\\ 0& 0\end{array}\right),\text{Re}(E)>0,\text{Im}(E)<0.$$
(4.18)
From Eqs. (4.17) and (4.18) we can see that the measures $`\varrho _{12}`$, $`\varrho _{21}`$ and $`\varrho _{22}`$ in Theorem 4 of Appendix A are zero, and that the measure $`\varrho _{11}`$ is given by

$`\varrho _{11}((E_1,E_2))`$ $`=`$ $`\underset{\delta 0}{lim}\underset{\epsilon 0+}{lim}{\displaystyle \frac{1}{2\pi i}}{\displaystyle _{E_1+\delta }^{E_2\delta }}\left[\theta _{11}^+(Ei\epsilon )\theta _{11}^+(E+i\epsilon )\right]𝑑E`$ (4.19)
$`=`$ $`{\displaystyle _{E_1}^{E_2}}{\displaystyle \frac{1}{\pi }}{\displaystyle \frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}}}𝑑E,`$
which leads to

$$\varrho (E)\varrho _{11}(E)=\frac{1}{\pi }\frac{2m/\mathrm{}^2}{\sqrt{2m/\mathrm{}^2E}},E(0,\mathrm{}).$$
(4.20)
The function $`\theta _{11}^+(E)`$ has a branch cut along $`(0,\mathrm{})`$, and therefore $`(0,\mathrm{})`$ is included in $`\mathrm{Sp}(H_0)`$. Because $`\mathrm{Sp}(H_0)`$ is a closed set, $`\mathrm{Sp}(H_0)=[0,\mathrm{})`$.

## 5 Diagonalization and Eigenfunction Expansion

In the present section, we diagonalize $`H_0`$ and construct the expansion of the wave functions in terms of the eigenfunctions of the differential operator $`h_0`$.

By Theorem 2 of Appendix A, there is a unitary map $`\stackrel{~}{U}_0`$ defined by

$`\stackrel{~}{U}_0:L^2([0,\mathrm{}),dr)`$ $``$ $`L^2((0,\mathrm{}),\varrho (E)dE)`$
$`f(r)`$ $``$ $`\stackrel{~}{f}(E)=\stackrel{~}{U}_0f(E)={\displaystyle _0^{\mathrm{}}}𝑑rf(r)\overline{\chi (r;E)},`$ (5.1)
that brings $`𝒟(H_0)`$ onto the space

$$𝒟(\stackrel{~}{H}_0)=\{\stackrel{~}{f}(E)L^2((0,\mathrm{}),\varrho (E)dE)|_0^{\mathrm{}}𝑑EE^2|\stackrel{~}{f}(E)|^2\varrho (E)<\mathrm{}\}.$$
(5.2)
The unitary operator $`\stackrel{~}{U}_0`$ provides a $`\varrho `$-normalization (cf. Ref. ). In order to obtain a $`\delta `$-normalization, the measure $`\varrho (E)`$ must be absorbed in the definition of the eigenfunctions (cf. Ref. ). This is why we define

$$\sigma (r;E):=\sqrt{\varrho (E)}\chi (r;E),$$
(5.3)
which is the $`\delta `$-normalized eigensolution of the differential operator $`h_0`$. If we define

$$\widehat{f}(E):=\sqrt{\varrho (E)}\stackrel{~}{f}(E),\stackrel{~}{f}(E)L^2((0,\mathrm{}),\varrho (E)dE),$$
(5.4)
and construct the unitary operator

$`\widehat{U}_0:L^2((0,\mathrm{}),\varrho (E)dE)`$ $``$ $`L^2((0,\mathrm{}),dE)`$
$`\stackrel{~}{f}`$ $``$ $`\widehat{f}(E)=\widehat{U}_0\stackrel{~}{f}(E):=\sqrt{\varrho (E)}\stackrel{~}{f}(E),`$ (5.5)
then the operator that $`\delta `$-diagonalizes our Hamiltonian is $`U_0:=\widehat{U}_0\stackrel{~}{U}_0`$,

$`U_0:L^2([0,\mathrm{}),dr)`$ $``$ $`L^2((0,\mathrm{}),dE)`$
$`f`$ $``$ $`U_0f:=\widehat{f}.`$ (5.6)
The action of $`U_0`$ can be written as an integral operator:

$$\widehat{f}(E)=U_0f(E)=_0^{\mathrm{}}𝑑rf(r)\overline{\sigma (r;E)},f(r)L^2([0,\mathrm{}),dr).$$
(5.7)
The image of $`𝒟(H_0)`$ under the action of $`U_0`$ is

$$𝒟(\widehat{H}_0):=U𝒟(H_0)=\{\widehat{f}(E)L^2((0,\mathrm{}),dE)|_0^{\mathrm{}}E^2|\widehat{f}(E)|^2𝑑E<\mathrm{}\}.$$
(5.8)
Therefore, we have constructed a unitary operator

$`U_0:𝒟(H)L^2([0,\mathrm{}),dr)`$ $``$ $`𝒟(\widehat{H}_0)L^2((0,\mathrm{}),dE)`$
$`f`$ $``$ $`\widehat{f}=U_0f`$ (5.9)
that transforms from the position representation into the energy representation (see diagram (8) below). The operator $`U_0`$ diagonalizes the free Hamiltonian in the sense that $`\widehat{H}_0U_0H_0U_0^1`$ is the multiplication operator. The inverse operator of $`U_0`$ is given by (see Theorem 3 of Appendix A)

$$f(r)=U_0^1\widehat{f}(r)=_0^{\mathrm{}}𝑑E\widehat{f}(E)\sigma (r;E),\widehat{f}(E)L^2((0,\mathrm{}),dE).$$
(5.10)
The operator $`U_0^1`$ transforms from the energy representation into the position representation (see diagram (8) below). The expressions (5.7) and (5.10) provide the eigenfunction expansion of any square integrable function in terms of the $`\delta `$-normalized eigensolutions $`\sigma (r;E)`$ of $`h_0`$.

## 6 Construction of the RHS of the Free Hamiltonian

The Sturm-Liouville theory only provides a domain $`𝒟(H_0)`$ on which the Hamiltonian $`H_0`$ is self-adjoint and a unitary operator $`U_0`$ that diagonalizes $`H_0`$. This unitary operator induces a direct integral decomposition of the Hilbert space (cf. Ref.  and references therein),

$``$ $``$ $`U_0\widehat{}={\displaystyle _{\mathrm{Sp}(H_0)}}(E)𝑑E`$
$`f`$ $``$ $`U_0f\{\widehat{f}(E)\},\widehat{f}(E)(E).`$ (6.1)
As shown in Refs. , the direct integral decomposition does not provide us with all the tools needed in Quantum Mechanics. This is why we extend the Hilbert space to the RHS.

We first need to construct a dense invariant domain $`𝚽_0`$ on which all the powers and all the expectation values of $`H_0`$ are well defined, and on which the Dirac kets act as antilinear functionals. Before building $`𝚽_0`$, we need to build the maximal invariant subspace $`𝒟_0`$ of $`H_0`$,

$$𝒟_0:=\underset{n=0}{\overset{\mathrm{}}{}}𝒟(H_0^n).$$
(6.2)
It is easy to check that

$`𝒟_0=\{\phi L^2([0,\mathrm{}),dr)|`$ $`h_0^n\phi (r)L^2([0,\mathrm{}),dr),h_0^n\phi (0)=0,n=0,1,2,\mathrm{},`$ (6.3)
$`\phi (r)C^{\mathrm{}}([0,\mathrm{}))\}.`$
We can now construct the subspace $`𝚽_0`$ on which the eigenkets $`|E`$ of $`H_0`$ are well defined as antilinear functionals. This subspace is given by

$$𝚽_0=\{\phi 𝒟_0|_0^{\mathrm{}}𝑑r\left|(r+1)^n(h_0+1)^m\phi (r)\right|^2<\mathrm{},n,m=0,1,2,\mathrm{}\}.$$
(6.4)
On $`𝚽_0`$, we define the family of norms

$$\phi _{n,m}:=\sqrt{_0^{\mathrm{}}𝑑r\left|(r+1)^n(h_0+1)^m\phi (r)\right|^2},n,m=0,1,2,\mathrm{}$$
(6.5)
The quantities (6.5) fulfill the conditions to be a norm (see Proposition 1 of Appendix B), and can be used to define a countably normed topology $`\tau _{𝚽_0}`$ on $`𝚽_0`$ (for the definition of a countably normed topology, consult Ref.  and references therein),

$$\phi _\alpha \underset{\alpha \mathrm{}}{\overset{\tau _{𝚽_0}}{-⟶}}\phi \mathrm{iff}\phi _\alpha \phi _{n,m}\underset{\alpha \mathrm{}}{-⟶}\mathrm{\hspace{0.17em}0},n,m=0,1,2,\mathrm{}$$
(6.6)
The space $`𝚽_0`$ is stable under the action of $`H_0`$, and $`H_0`$ is $`\tau _{𝚽_0}`$-continuous (see Proposition 2 of Appendix B).

Once we have constructed the space $`𝚽_0`$, we can construct its topological dual $`𝚽_0^\times `$ as the space of $`\tau _{𝚽_0}`$-continuous antilinear functionals on $`𝚽_0`$ and therewith the RHS of the free Hamiltonian (see diagram (8) below):

$$𝚽_0L^2([0,\mathrm{}),dr)𝚽_0^\times .$$
(6.7)
For each $`E\mathrm{Sp}(H_0)`$, we can now associate a ket $`|E`$ to the generalized eigenfunction $`\sigma (r;E)`$ through

$`|E:𝚽_0`$ $``$ $``$
$`\phi `$ $``$ $`\phi |E:={\displaystyle _0^{\mathrm{}}}\overline{\phi (r)}\sigma (r;E)𝑑r=\overline{(U_0\phi )(E)}.`$ (6.8)
The ket $`|E`$ in Eq. (6.8) is a well-defined antilinear functional on $`𝚽_0`$, i.e., $`|E`$ belongs to $`𝚽_0^\times `$ (see Proposition 3 of Appendix B). The ket $`|E`$ is a generalized eigenvector of the free Hamiltonian $`H_0`$ (see Proposition 3 of Appendix B):

$$H_0^\times |E=E|E;$$
(6.9)
that is,

$$\phi |H_0^\times |E=H_0^{}\phi |E=E\phi |E,\phi 𝚽_0.$$
(6.10)
## 7 The Dirac Basis Vector Expansion for $`H_0`$

We are now in a position to derive the Dirac basis vector expansion for the free Hamiltonian. This derivation consists of the restriction of the Weyl-Kodaira expansions (5.7) and (5.10) to the space $`𝚽_0`$. If we denote $`r|\phi \phi (r)`$ and $`E|r\overline{\sigma (r;E)}`$, and if we define the action of the bra $`E|`$ on $`\phi 𝚽_0`$ as $`E|\phi :=\widehat{\phi }(E)`$, then Eq. (5.7) becomes

$$E|\phi =_0^{\mathrm{}}𝑑rE|rr|\phi ,\phi 𝚽_0.$$
(7.1)
If we denote $`r|E\sigma (r;E)`$, then Eq. (5.10) becomes

$$r|\phi =_0^{\mathrm{}}𝑑Er|EE|\phi ,\phi 𝚽_0.$$
(7.2)
This equation is the Dirac basis vector expansion of the wave function $`\phi `$ in terms of the free eigenkets $`|E`$. We can also prove the Nuclear Spectral Theorem for the free Hamiltonian (see Proposition 4 of Appendix B),

$$(\phi ,H_0^n\psi )=_0^{\mathrm{}}𝑑EE^n\phi |EE|\psi ,\phi ,\psi 𝚽_0,n=1,2,\mathrm{}$$
(7.3)
## 8 Energy Representation of the RHS of $`H_0`$

We have already seen that in the energy representation, the Hamiltonian $`H_0`$ acts as the multiplication operator $`\widehat{H}_0`$. The energy representation of the space $`𝚽_0`$ is defined as

$$\widehat{𝚽}_0:=U_0𝚽_0.$$
(8.1)
Obviously $`\widehat{𝚽}_0`$ is a linear subspace of $`L^2([0,\mathrm{}),dE)`$. In oder to endow $`\widehat{𝚽}_0`$ with a topology $`\tau _{\widehat{𝚽}_0}`$, we carry the topology on $`𝚽_0`$ into $`\widehat{𝚽}_0`$,

$$\tau _{\widehat{𝚽}_0}:=U_0\tau _{𝚽_0}.$$
(8.2)
With this topology, the space $`\widehat{𝚽}_0`$ is a linear topological space. If we denote the dual space of $`\widehat{𝚽}_0`$ by $`\widehat{𝚽}_0^\times `$, then we have

$$U_0^\times 𝚽_0^\times =(U_0𝚽_0)^\times =\widehat{𝚽}_0^\times .$$
(8.3)
If we denote $`|\widehat{E}U_0^\times |E`$, then we can prove that $`|\widehat{E}`$ is the antilinear Schwartz delta functional (see Proposition 5 of Appendix B),

$`|\widehat{E}:\widehat{𝚽}`$ $``$ $``$
$`\widehat{\phi }`$ $``$ $`\widehat{\phi }|\widehat{E}:=\overline{\widehat{\phi }(E)}.`$ (8.4)
It is very helpful to show the different realizations of the RHS through the following diagram:

$$\begin{array}{cccccccccccc}H_0;& \phi (r)& & 𝚽_0\hfill & & L^2([0,\mathrm{}),dr)& & 𝚽_0^\times \hfill & & |E& & \mathrm{position}\mathrm{repr}.\hfill \\ & & & U_0\hfill & & U_0& & U_0^\times \hfill & & & & \\ \widehat{H}_0;& \widehat{\phi }(E)& & \widehat{𝚽}_0\hfill & & L^2([0,\mathrm{}),dE)& & \widehat{𝚽}_0^\times \hfill & & |\widehat{E}& & \mathrm{energy}\mathrm{repr}.\hfill \end{array}$$

On the top line, we have the position representation of the Hamiltonian, the wave functions, the kets, and the RHS. On the bottom line, we have their energy representation counterparts.

## 9 Conclusions

We have constructed the RHS of $`H_0`$ (for the zero angular momentum case), and its energy representation. We have associated an eigenket $`|E`$ to each energy $`E`$ in the spectrum of $`H_0`$, and shown that $`|E`$ belongs to $`𝚽_0^\times `$. We have seen that the energy representation of $`|E`$ is given by the antilinear Schwartz delta functional. We have also shown that the Dirac basis vector expansion holds within the RHS of $`H_0`$.

Thus, we conclude that the natural setting for the solutions of the Schrödinger equation of $`H_0`$ is the Rigged Hilbert Space rather than just the Hilbert space.

## Acknowledgment

C. Koeninger’s advise on English style is gratefully acknowledged. This work was financially supported by the E.U. TMR Contract No. ERBFMRX-CT96-0087 “The Physics of Quantum Information.”

## Appendix A Appendix A: The Sturm-Liouville Theory

The following theorem provides the procedure to compute the Green function of $`H_0`$ (cf. Theorem XIII.3.16 of Ref.  and also Refs.  for some applications):

Theorem 1 Let $`H_0`$ be the self-adjoint operator (2.4) derived from the real formal differential operator (1.7) by the imposition of the boundary condition (2.2d). Let $`\text{Im}(E)0`$. Then there is exactly one solution $`\chi (r;E)`$ of $`(h_0E)\sigma =0`$ square-integrable at $`0`$ and satisfying the boundary condition (2.2d), and exactly one solution $`f(r;E)`$ of $`(h_0E)\sigma =0`$ square-integrable at infinity. The resolvent $`(EH_0)^1`$ is an integral operator whose kernel $`G_0(r,s;E)`$ is given by

$$G_0(r,s;E)=\{\begin{array}{cc}\frac{2m}{\mathrm{}^2}\frac{\chi (r;E)f(s;E)}{W(\chi ,f)}\hfill & r<s\hfill \\ \frac{2m}{\mathrm{}^2}\frac{\chi (s;E)f(r;E)}{W(\chi ,f)}\hfill & r>s,\hfill \end{array}$$
(A.1)
where $`W(\chi ,f)`$ is the Wronskian of $`\chi `$ and $`f`$

$$W(\chi ,f)=\chi f^{}\chi ^{}f.$$
(A.2)
The theorem that provides the operator $`U_0`$ that diagonalizes $`H_0`$ is the following (cf. Theorem XIII.5.13 of Ref.  and also Refs.  for some applications):

Theorem 2 (Weyl-Kodaira) Let $`h_0`$ be the formally self-adjoint differential operator (1.7) defined on the interval $`[0,\mathrm{})`$. Let $`H_0`$ be the self-adjoint operator (2.4). Let $`\mathrm{\Lambda }`$ be an open interval of the real axis, and suppose that there is given a set $`\{\sigma _1(r;E),\sigma _2(r;E)\}`$ of functions, defined and continuous on $`(0,\mathrm{})\times \mathrm{\Lambda }`$, such that for each fixed $`E`$ in $`\mathrm{\Lambda }`$, $`\{\sigma _1(r;E),\sigma _2(r;E)\}`$ forms a basis for the space of solutions of $`h_0\sigma =E\sigma `$. Then there exists a positive $`2\times 2`$ matrix measure $`\{\varrho _{ij}\}`$ defined on $`\mathrm{\Lambda }`$, such that

1. the limit

$$(U_0f)_i(E)=\underset{c0}{lim}\underset{d\mathrm{}}{lim}\left[_c^df(r)\overline{\sigma _i(r;E)}𝑑r\right]$$
(A.3)
exists in the topology of $`L^2(\mathrm{\Lambda },\{\varrho _{ij}\})`$ for each $`f`$ in $`L^2([0,\mathrm{}),dr)`$ and defines an isometric isomorphism $`U_0`$ of $`𝖤(\mathrm{\Lambda })L^2([0,\mathrm{}),dr)`$ onto $`L^2(\mathrm{\Lambda },\{\varrho _{ij}\})`$, where $`𝖤(\mathrm{\Lambda })`$ is the spectral projection associated with $`\mathrm{\Lambda }`$;
2. for each Borel function $`G`$ defined on the real line and vanishing outside $`\mathrm{\Lambda }`$,

$$U_0𝒟(G(H_0))=\{[f_i]L^2(\mathrm{\Lambda },\{\varrho _{ij}\})|[Gf_i]L^2(\mathrm{\Lambda },\{\varrho _{ij}\})\}$$
(A.4)
and

$$(U_0G(H_0)f)_i(E)=G(E)(U_0f)_i(E),i=1,2,E\mathrm{\Lambda },f𝒟(G(H_0)).$$
(A.5)

The theorem that provides the inverse of the operator $`U_0`$ is the following (cf. Theorem XIII.5.14 of Ref.  and also Refs.  for some applications):

Theorem 3 (Weyl-Kodaira) Let $`H_0`$, $`\mathrm{\Lambda }`$, $`\{\varrho _{ij}\}`$, etc., be as in Theorem 2. Let $`E_0`$ and $`E_1`$ be the end points of $`\mathrm{\Lambda }`$. Then

1. the inverse of the isometric isomorphism $`U_0`$ of $`𝖤(\mathrm{\Lambda })L^2([0,\mathrm{}),dr)`$ onto $`L^2(\mathrm{\Lambda },\{\varrho _{ij}\})`$ is given by the formula

$$(U_0^1F)(r)=\underset{\mu _0E_0}{lim}\underset{\mu _1E_1}{lim}_{\mu _0}^{\mu _1}\left(\underset{i,j=1}{\overset{2}{}}F_i(E)\sigma _j(r;E)\varrho _{ij}(dE)\right)$$
(A.6)
where $`F=[F_1,F_2]L^2(\mathrm{\Lambda },\{\varrho _{ij}\})`$, the limit existing in the topology of $`L^2([0,\mathrm{}),dr)`$;
2. if $`G`$ is a bounded Borel function vanishing outside a Borel set $`e`$ whose closure is compact and contained in $`\mathrm{\Lambda }`$, then $`G(H_0)`$ has the representation

$$G(H_0)f(r)=_0^{\mathrm{}}f(s)K(H_0,r,s)𝑑s,$$
(A.7)
where

$$K(H_0,r,s)=\underset{i,j=1}{\overset{2}{}}_eG(E)\overline{\sigma _i(s;E)}\sigma _j(r;E)\varrho _{ij}(dE).$$
(A.8)

The spectral measures are provided by the following theorem (cf. Theorem XIII.5.18 of Ref.  and also Refs.  for some applications):

Theorem 4 (Titchmarsh-Kodaira) Let $`\mathrm{\Lambda }`$ be an open interval of the real axis and $`O`$ be an open set in the complex plane containing $`\mathrm{\Lambda }`$. Let $`\mathrm{Re}(H_0)`$ be the resolvent set of $`H_0`$. Let $`\{\sigma _1(r;E),\sigma _2(r;E)\}`$ be a set of functions which form a basis for the solutions of the equation $`h_0\sigma =E\sigma `$, $`EO`$, and which are continuous on $`(0,\mathrm{})\times O`$ and analytically dependent on $`E`$ for $`E`$ in $`O`$. Suppose that the kernel $`G_0(r,s;E)`$ for the resolvent $`(EH_0)^1`$ has a representation

$$G_0(r,s;E)=\{\begin{array}{ccc}_{i,j=1}^2\theta _{ij}^{}(E)\sigma _i(r;E)\overline{\sigma _j(s;\overline{E})},\hfill & & r<s,\hfill \\ _{i,j=1}^2\theta _{ij}^+(E)\sigma _i(r;E)\overline{\sigma _j(s;\overline{E})},\hfill & & r>s,\hfill \end{array}$$
(A.9)
for all $`E`$ in $`\mathrm{Re}(H_0)O`$, and that $`\{\varrho _{ij}\}`$ is a positive matrix measure on $`\mathrm{\Lambda }`$ associated with $`H_0`$ as in Theorem 2. Then the functions $`\theta _{ij}^\pm `$ are analytic in $`\mathrm{Re}(H_0)O`$, and given any bounded open interval $`(E_1,E_2)\mathrm{\Lambda }`$, we have for $`1i,j2`$,

$$\begin{array}{ccc}\varrho _{ij}((E_1,E_2))\hfill & =\hfill & lim_{\delta 0}lim_{\epsilon 0+}\frac{1}{2\pi i}_{E_1+\delta }^{E_2\delta }[\theta _{ij}^{}(Ei\epsilon )\theta _{ij}^{}(E+i\epsilon )]𝑑E\hfill \\ & =\hfill & lim_{\delta 0}lim_{\epsilon 0+}\frac{1}{2\pi i}_{E_1+\delta }^{E_2\delta }[\theta _{ij}^+(Ei\epsilon )\theta _{ij}^+(E+i\epsilon )]𝑑E.\hfill \end{array}$$
(A.10)
## Appendix B Appendix B: Auxiliary Propositions

In this appendix, we list the propositions invoked throughout the paper.

Proposition 1 The quantities

$$\phi _{n,m}:=\sqrt{_0^{\mathrm{}}𝑑r\left|(r+1)^n(h_0+1)^m\phi (r)\right|^2},\phi 𝚽_0,n,m=0,1,2,\mathrm{},$$
(B.1)
are norms.

Proof It is very easy to show that the quantities (B.1) fulfill the conditions to be a norm:

$`\phi +\psi _{n,m}\phi _{n,m}+\psi _{n,m},`$ (B.2a)
$`\alpha \phi _{n,m}=|\alpha |\phi _{n,m},`$ (B.2b)
$`\phi _{n,m}0,`$ (B.2c)
$`\mathrm{If}\phi _{n,m}=0,\mathrm{then}\phi =0.`$ (B.2d)
The only condition that is somewhat difficult to prove is (B.2d): if $`\phi _{n,m}=0`$, then

$$(1+r)^n(h_0+1)^m\phi (r)=0,$$
(B.3)
which yields

$$(h_0+1)^m\phi (r)=0.$$
(B.4)
If $`m=0`$, then Eq. (B.4) implies $`\phi (r)=0`$. If $`m=1`$, then Eq. (B.4) implies that $`1`$ is an eigenvalue of $`H_0`$ whose corresponding eigenvector is $`\phi `$. Since $`1`$ is not an eigenvalue of $`H_0`$, $`\phi `$ must be the zero vector. If $`m>1`$, the proof is similar.

Proposition 2 The space $`𝚽_0`$ is stable under the action of $`H_0`$, and $`H_0`$ is $`\tau _{𝚽_0}`$-continuous.

Proof In order to see that $`H_0`$ is $`\tau _{𝚽_0}`$-continuous, we just have to realize that

$`H_0\phi _{n,m}`$ $`=`$ $`(H_0+I)\phi \phi _{n,m}`$ (B.5)
$``$ $`(H_0+I)\phi _{n,m}+\phi _{n,m}`$
$`=`$ $`\phi _{n,m+1}+\phi _{n,m}.`$
We now prove that $`𝚽_0`$ is stable under the action of $`H_0`$. Let $`\phi 𝚽_0`$. Saying that $`\phi 𝚽_0`$ is equivalent to saying that $`\phi 𝒟_0`$ and that the norms $`\phi _{n,m}`$ are finite for every $`n,m=0,1,2,\mathrm{}`$ Since $`H_0\phi `$ is also in $`𝒟_0`$, and since the norms $`H_0\phi _{n,m}`$ are also finite (see Eq. (B.5)), the vector $`H_0\phi `$ is also in $`𝚽_0`$.

Proposition 3 The function

$`|E:𝚽_0`$ $``$ $``$
$`\phi `$ $``$ $`\phi |E:={\displaystyle _0^{\mathrm{}}}\overline{\phi (r)}\sigma (r;E)𝑑r=\overline{(U_0\phi )(E)}.`$ (B.6)
is an antilinear functional on $`𝚽_0`$ and a generalized eigenvector of (the restriction to $`𝚽_0`$ of) $`H_0`$.

Proof From the definition (B.6), it is pretty easy to see that $`|E`$ is an antilinear functional. In order to show that $`|E`$ is continuous, we define

$$(E):=\underset{r[0,\mathrm{})}{sup}\left|\sigma (r;E)\right|.$$
(B.7)
Because

$`|\phi |E|`$ $`=`$ $`|\overline{U\phi (E)}|`$ (B.8)
$`=`$ $`\left|{\displaystyle _0^{\mathrm{}}}𝑑r\overline{\phi (r)}\sigma (r;E)\right|`$
$``$ $`{\displaystyle _0^{\mathrm{}}}𝑑r|\overline{\phi (r)}||\sigma (r;E)|`$
$``$ $`(E){\displaystyle _0^{\mathrm{}}}𝑑r|\phi (r)|`$
$`=`$ $`(E){\displaystyle _0^{\mathrm{}}}𝑑r{\displaystyle \frac{1}{1+r}}(1+r)|\phi (r)|`$
$``$ $`(E)\left({\displaystyle _0^{\mathrm{}}}𝑑r{\displaystyle \frac{1}{(1+r)^2}}\right)^{1/2}\left({\displaystyle _0^{\mathrm{}}}𝑑r\left|(1+r)\phi (r)\right|^2\right)^{1/2}`$
$`=`$ $`(E)\left({\displaystyle _0^{\mathrm{}}}𝑑r{\displaystyle \frac{1}{(1+r)^2}}\right)^{1/2}\phi _{1,0}`$
$`=`$ $`(E)\phi _{1,0},`$
the functional $`|E`$ is continuous when $`𝚽_0`$ is endowed with the $`\tau _{𝚽_0}`$ topology.

In order to prove that $`|E`$ is a generalized eigenvector of $`H_0`$, we make use of the conditions (6.3) and (6.5) satisfied by the elements of $`𝚽_0`$:

$`\phi |H_0^\times |E`$ $`=`$ $`H_0^{}\phi |E`$ (B.9)
$`=`$ $`{\displaystyle _0^{\mathrm{}}}𝑑r\left({\displaystyle \frac{\mathrm{}^2}{2m}}{\displaystyle \frac{d^2}{dr^2}}\overline{\phi (r)}\right)\sigma (r;E)`$
$`=`$ $`{\displaystyle \frac{\mathrm{}^2}{2m}}\left[{\displaystyle \frac{d\overline{\phi (r)}}{dr}}\sigma (r;E)\right]_0^{\mathrm{}}+{\displaystyle \frac{\mathrm{}^2}{2m}}\left[\overline{\phi (r)}{\displaystyle \frac{d\sigma (r;E)}{dr}}\right]_0^{\mathrm{}}`$
$`+{\displaystyle _0^{\mathrm{}}}𝑑r\overline{\phi (r)}\left({\displaystyle \frac{\mathrm{}^2}{2m}}{\displaystyle \frac{d^2}{dr^2}}\sigma (r;E)\right)`$
$`=`$ $`E\phi |E.`$
Similarly, one can also prove that

$$\phi |(H_0^\times )^n|E=E^n\phi |E.$$
(B.10)
Proposition 4 (Nuclear Spectral Theorem) Let

$$𝚽_0L^2([0,\mathrm{}),dr)𝚽_0^\times $$
(B.11)
be the RHS of $`H_0`$ such that $`𝚽_0`$ remains invariant under $`H_0`$ and $`H_0`$ is a $`\tau _{𝚽_0}`$-continuous operator on $`𝚽_0`$. Then, for each $`E`$ in the spectrum of $`H_0`$ there is a generalized eigenvector $`|E`$ such that

$$H_0^\times |E=E|E$$
(B.12)
and such that

$$(\phi ,\psi )=_{\mathrm{Sp}(H_0)}𝑑E\phi |EE|\psi ,\phi ,\psi 𝚽_0,$$
(B.13)
and

$$(\phi ,H_0^n\psi )=_{\mathrm{Sp}(H_0)}𝑑EE^n\phi |EE|\psi ,\phi ,\psi 𝚽_0,n=1,2,\mathrm{}$$
(B.14)
Proof Let $`\phi `$ and $`\psi `$ be in $`𝚽_0`$. Since $`U_0`$ is unitary,

$$(\phi ,\psi )=(U_0\phi ,U_0\psi )=(\widehat{\phi },\widehat{\psi }).$$
(B.15)
The wave functions $`\widehat{\phi }`$ and $`\widehat{\psi }`$ are in particular elements of $`L^2([0,\mathrm{}),dE)`$. Therefore their scalar product is well defined,

$$(\widehat{\phi },\widehat{\psi })=_{\mathrm{Sp}(H_0)}𝑑E\overline{\widehat{\phi }(E)}\widehat{\psi }(E).$$
(B.16)
Because $`\phi `$ and $`\psi `$ belong to $`𝚽_0`$, the action of each eigenket $`|E`$ on them is well defined,

$`\phi |E=\overline{\widehat{\phi }(E)},`$ (B.17a)
$`E|\psi =\widehat{\psi }(E).`$ (B.17b)
By plugging Eq. (B.17) into Eq. (B.16) and Eq. (B.16) into Eq. (B.15), we obtain Eq. (B.13). The proof of (B.14) is similar:

$`(\phi ,H_0^n\psi )`$ $`=`$ $`(U_0\phi ,U_0H_0^nU_0^1U_0\psi )`$ (B.18)
$`=`$ $`(\widehat{\phi },\widehat{H}_0^n\widehat{\psi })`$
$`=`$ $`{\displaystyle _{\mathrm{Sp}(H_0)}}𝑑E\overline{\widehat{\phi }(E)}(\widehat{H}_0^n\widehat{\psi })(E)`$
$`=`$ $`{\displaystyle _{\mathrm{Sp}(H_0)}}𝑑EE^n\overline{\widehat{\phi }(E)}\widehat{\psi }(E)`$
$`=`$ $`{\displaystyle _{\mathrm{Sp}(H_0)}}𝑑EE^n\phi |EE|\psi .`$
Proposition 5 The energy representation of the eigenket $`|E`$ is the antilinear Schwartz delta functional $`|\widehat{E}`$.

Proof Because

$`\widehat{\phi }|U_0^\times |E`$ $`=`$ $`U_0^1\widehat{\phi }|E`$ (B.19)
$`=`$ $`\phi |E`$
$`=`$ $`{\displaystyle _0^{\mathrm{}}}\overline{\phi (r)}\sigma (r;E)𝑑r`$
$`=`$ $`\overline{\widehat{\phi }(E)},`$
the functional $`U_0^\times |E=|\widehat{E}`$ is the antilinear Schwartz delta functional.


text:
# New physics scales and anomalous magnetic moment

## 1 Introduction

The recen t BNL measurement of the anomalous magnetic moment of the muon $`a_\mu =\frac{g2}{2}`$ has confirmed an excess on the calculation of standard model contributions of

$$\mathrm{\Delta }a_\mu 2\times 10^9$$
(1)
at a $`2\sigma `$ level .

This is an indication of possible new physics at an energy scale $`\mathrm{\Lambda }.`$ It is interesting to estimate the order of the correction of $`a_\mu `$ in powers of $`\frac{m_\mu }{\mathrm{\Lambda }}`$ , where $`m_\mu `$ is the muon mass. This is related  to the validity or breaking of the chiral symmetry of leptons together with the change of sign of $`m_\mu `$. If this symmetry, which we will call of Weinberg, is respected $`\mathrm{\Delta }a_\mu \left(m_\mu /\mathrm{\Lambda }\right)^2`$ whereas if it is broken $`\mathrm{\Delta }a_\mu m_\mu /\mathrm{\Lambda }`$ . This is important because in the latter case the explanation of Eq. (1) may be given by new physics at a relatively high energy whereas in the former it should appear at a scale close to the electroweak one.

## 2 Weinberg symmetry and Standard Model

Since the mass term breaks chiral symmetry, one can make it invariant changing the mass sign

$$\mu \gamma _5\mu ,m_\mu m_\mu .$$
(2)
The effective interaction for the anomalous magnetic moment has a similar chiral form

$$_{\mathrm{𝐞𝐟𝐟}}=a_\mu \frac{e}{4m_\mu }\overline{\mu }\sigma ^{\alpha \beta }\mu F_{\alpha \beta },$$
(3)
so that if the symmetry Eq. (2) is valid the corrections to $`a_\mu `$ must be of even powers of the ratio of $`m_\mu `$ to a larger scale $`\mathrm{\Lambda }`$

$$a_\mu =c_o\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^0+c_2\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^2+\mathrm{}.$$
(4)
This is what happens in the Standard Model (SM) since, to be invariant in it, Eq. (3) must be written as

$$_{\mathrm{𝐞𝐟𝐟}}=a_\mu \frac{e}{4m_\mu }(\overline{l}_L\sigma ^{\alpha \beta }\mu _R\frac{f\phi _V}{m_\mu }+h.c.)F_{\alpha \beta },$$
(5)
with a doublet Higgs field $`\phi =\phi _V+\left(\begin{array}{c}0\\ h/\sqrt{2}\end{array}\right)`$ such that

$$\overline{l}_L=\left(\begin{array}{c}\nu _L\\ \mu _L\end{array}\right),\phi _V=\left(\begin{array}{c}0\\ \frac{\upsilon }{\sqrt{2}}\end{array}\right),f\frac{\upsilon }{\sqrt{2}}=m_\mu .$$
(6)
To have the transformations Eq. (2) one must perform

$$l_L\gamma _5l_L=l_L,\mu _R\gamma _5\mu _R=\mu _R,\phi \phi .$$
(7)
The Weinberg symmetry (WS) is respected in SM since the charged weak interactions

$$\overline{\nu }_L\gamma ^\alpha \mu _LW_\alpha ,$$

neutral and electromagnetic

$$\overline{\mu }\gamma ^\alpha (g_\upsilon +g_a\gamma ^5)\mu Z_\alpha ,\overline{\mu }\gamma ^\alpha \mu A_\alpha $$

and Yukawa one

$$\overline{\mu }\mu h,$$

are invariant under Eq. (7) .
Therefore the corrections to $`a_\mu `$ are of the type of Eq. (4) with the electroweak scale $`\mathrm{\Lambda }_{EW}`$ , corresponding the first term to the electromagnetic contributions $`c_o=\frac{\alpha }{2\pi }+\mathrm{}`$ and the second to the weak ones $`10^9`$ .

## 3 Grand Unification Theories

In principle, if there is a second  Higgs doublet $`\phi \stackrel{´}{}`$ wich breaks at a scale $`\mathrm{\Lambda }`$ higher than that of SM and is not directly related to the muon mass, it is possible to have an additional effective interaction of new physics

$$_{\mathrm{𝐞𝐟𝐟}}\frac{1}{\mathrm{\Lambda }^2}(\overline{l}_L\sigma ^{\alpha \beta }\mu _R\phi \stackrel{´}{}_V+h.c.)F_{\alpha \beta }.$$
(8)
Being $`\phi \stackrel{´}{}_V\mathrm{\Lambda }`$ , Eq. (8) is of the form

$$_{\mathrm{𝐞𝐟𝐟}}=\mathrm{\Delta }a_\mu \frac{e}{4m_\mu }\overline{\mu }\sigma ^{\alpha \beta }\mu F_{\alpha \beta }$$
(9)
with $`\mathrm{\Delta }a_\mu =O\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)`$ which breaks the Weinberg symmetry.

Regarding Grand Unification Theories(GUT) it is not obvious that a particular model has interactions which violate this symmetry and therefore produce an effective interaction like Eq. (8).

E.g. starting with SU(5), the only new interaction which contributes to $`a_\mu `$ is that due to leptoquarks $`X^\alpha `$ i.e. $`\overline{\mu }\gamma ^\alpha qX_\alpha `$ which changes muon into quarks but respects chiral symmetry $`\mu \gamma _5\mu `$ , $`q\gamma _5q.`$ Since the Yukawa interaction is unchanged because the Higgs which breaks $`SU(5)`$ does not affect the muon mass, the WS is still valid, the effective interaction is of the type of Eq. (5) and

$$\mathrm{\Delta }a_\mu ^{SU(5)}\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^2,$$
(10)
which is negligible for the GUT scale $`10^{15}GeV.`$

In the case of $`SO(10),`$ the only change is that the high-scale Higgs $`\phi \stackrel{´}{}`$ gives mass to $`\nu _R`$ with a Majorana term. Then the low scale Higgs $`\phi `$ gives also to $`\nu `$ a Dirac mass. The diagonalization of the mass matrix produces the see-saw mechanism which involves a mixture of $`\nu _L`$ and $`\nu _R`$. But this only means that also the charged weak interactions have a small right-lepton contribution. Since $`\overline{\nu }\gamma ^\alpha \mu W_\alpha `$ is chiral invariant and the Yukawa muon term $`\overline{\mu }\mu h`$ is unchanged, the WS is preserved and again

$$\mathrm{\Delta }a_\mu ^{SO(10)}\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^2.$$

The substantial difference of the exceptional group $`E_6`$ is that it has 11 additional superheavy fermions among which a charged lepton $`M`$ that can mix with $`\mu .`$

If the breakings of symmetry are due to  a 351 of $`E_6`$ , when GUT is broken the mass eigenstates $`\mu _o`$ (massless) and $`\widehat{M}`$ (superheavy) are determined by the expectation values of the $`(SO(10),SU(5))`$ multiplets $`\phi \stackrel{´}{}(\mathrm{𝟓𝟒},\mathrm{𝟐𝟒})`$ and $`\phi \stackrel{´}{}(\mathrm{𝟏𝟒𝟒},\mathrm{𝟐𝟒})`$ through a large mixture of left components

$$\mu _L^o=\mu _L\mathrm{cos}\theta _L+M_L\mathrm{sin}\theta _L,\widehat{M}_L=M_L\mathrm{cos}\theta _L\mu _L\mathrm{sin}\theta _L$$
(12)
with the same mixing of $`\nu _L`$ and the neutral exotic lepton $`N_L.`$

The small mass of ordinary muon is due to the appearance of an expectation value of a Higgs $`H(10,\overline{\mathrm{𝟓}})`$ which in terms of the doublet $`\phi `$ gives

$$\overline{l}_L\mu _Rf\phi +h.c.=\frac{f}{\sqrt{2}}(\upsilon +h)(\overline{\mu }_R\mu _L+h.c.).$$
(13)
Since the right components were not mixed at the GUT scale, the mass term from Eq. (13) is

$$\frac{f}{\sqrt{2}}\upsilon (\overline{\mu }_R^o\mu _L^o\mathrm{cos}\theta _L\overline{\mu }_R^o\widehat{M}_L\mathrm{sin}\theta _L+h.c.).$$

Diagonalizing the whole mass matrix to give the physical state $`\widehat{\mu }`$ there will be also a mixture of $`\mu _R^o`$ with $`\widehat{M}_R`$ which will be small due to the very different GUT and EW scales, but with a relevant contribution to the muon mass. Therefore it will not be possible to argue that the transformation $`\phi \phi `$ will assure the change $`m_\mu m_\mu `$ .

Regarding the interaction with the light Higgs $`h`$ , there will be a “flavour-changing” term approximately equal to

$$_{\mathrm{𝐞𝐟𝐟}}=\frac{fh}{\sqrt{2}}(\overline{\widehat{\mu }}_R\widehat{M}_L\mathrm{sin}\theta _L+h.c.),$$
(14)
due to the slight difference between $`\mu ^o`$ and the physical state $`\widehat{\mu }.`$ This interaction does not respect WS because even though it is invariant under

$$\widehat{\mu }\gamma _5\widehat{\mu },\widehat{M}\gamma _5\widehat{M},hh,$$
(15)
as said above the last transformation does not imply $`m_\mu m_\mu `$ . As a consequence one may expect a linear correction of the muon magnetic moment. In fact the explicit calculation  of the one-loop contribution caused by Eq. (14) gives

$$\mathrm{\Delta }a_\mu ^{FCh}\frac{1}{16\pi ^2}\kappa ^2\frac{m_\mu }{M_M},$$
(16)
where, being $`\kappa =\frac{1}{\sqrt{2}}f\mathrm{sin}\theta _L1`$ and here $`f`$ not necessarily as small as $`\sqrt{2}\frac{m_\mu }{\upsilon }`$, to explain the discrepancy Eq. (1) one needs $`M_M10^6`$ $`GeV.`$ Even though this mass value seems small for a GUT particle, it is not unreasonable considering the strong mixture of exotic and ordinary fermions. The interaction Eq.(14) we have deduced from a particular scheme of mixture of muon with exotic lepton of $`E_6`$ is equivalent to the one of a singlet charged heavy lepton with the muonic and light Higgs doublets .

The mixture of $`\mu `$ and $`M`$ produces additional corrections to $`a_\mu `$ of electroweak type . If the scheme of breakings is based on the multiplet 351 as said above, the equal mixings for $`\mu _L`$ and $`\nu _L`$ avoid any correction in the charged current interaction. The same happens for the neutral charge interaction with $`Z`$ if only the left mixtures are considered. But if the small right mixture is included, a coupling $`\overline{\widehat{\mu }}\gamma ^\alpha \widehat{M}Z_\alpha `$ appears which is however chiral invariant and gives

$$\mathrm{\Delta }a_\mu ^{FCZ}\frac{\alpha }{\pi }\left(\mathrm{sin}\theta _R\mathrm{cos}\theta _R\right)^2\left(\frac{m_\mu }{M_Z}\right)^2,$$
(17)
where $`\left(\mathrm{sin}\theta _R\mathrm{cos}\theta _R\right)^2<10^2`$ not to spoil the experimental $`\mu \mu Z`$ coupling , so that $`\mathrm{\Delta }a_\mu ^{FCZ}10^{11}`$ i.e. irrelevant.

For the correction given by a loop with exchange of a heavy neutral boson $`Z\stackrel{´}{},`$ with different charges of the corresponding abelian group for $`\mu `$ and $`M`$ , there will be a “flavour changing” contribution

$$\mathrm{\Delta }a_\mu ^{FCZ\stackrel{´}{}}\frac{\alpha }{\pi }\left(\mathrm{sin}\theta _L\mathrm{cos}\theta _L\right)^2\left(\frac{m_\mu }{M_{Z\stackrel{´}{}}}\right)^2+\frac{\alpha }{\pi }\mathrm{sin}\theta _L\mathrm{cos}\theta _L\mathrm{sin}\theta _R\mathrm{cos}\theta _R\frac{m_\mu }{M_{Z\stackrel{´}{}}}$$
(18)
where the first chiral conserving term depends only on the large left mixture and is quadratic in the new physics scale, whereas the second chiral interference term needs the small right mixture reflecting the two-scales building of mass states and is linear in $`m_\mu /M_{Z\stackrel{´}{}}`$ .

But, compared with Eq. (16), even if $`M_{Z\stackrel{´}{}}`$ is so low as $`10^6GeV`$ this linear term gives again $`\mathrm{\Delta }a_\mu 10^{11}`$ i.e. negligible.

## 4 Other theories beyond the Standard Model

One of the most obvious is the Minimal Supersymmetric Standard Model (MSSM) which has two Higgs doublets with a ratio of expectation values $`\mathrm{tan}\beta =\frac{H\stackrel{´}{}}{H}`$ where $`H`$ gives mass to electron and quark $`d`$, and $`H\stackrel{´}{}`$ to quark $`u`$.

The interaction of muon with the chargino $`\stackrel{~}{W}`$ , $`\overline{\mu }\stackrel{~}{W}\stackrel{~}{\nu }`$ , in a way similar to Eq. (18), gives  the correction of $`a_\mu `$

$$\mathrm{\Delta }a_\mu ^{\stackrel{~}{W}}\frac{\alpha }{\pi }\left(\frac{m_\mu }{M_{\stackrel{~}{W}}}\right)^2+\frac{\alpha }{\pi }\frac{m_\mu }{M_{\stackrel{~}{W}}}O\left(\frac{m_\mu \mathrm{tan}\beta }{M_W}\right),$$
(19)
for large $`\mathrm{tan}\beta ,`$ where the first quadratic term corresponds to conservation of chirality and the second linear one is due to the chiral violation in internal line caused by the coupling of the two Higgs .

An analogous correction $`\mathrm{\Delta }a_\mu ^{\stackrel{~}{Z}}`$ comes from the coupling $`\overline{\mu }\stackrel{~}{Z}\stackrel{~}{\mu }`$ replacing in Eq. (19) $`M_{\stackrel{~}{W}}`$ by $`M_{\stackrel{~}{Z}}.`$ Since one expects $`M_{\stackrel{~}{W}}`$ $`M_{\stackrel{~}{Z}}1`$ $`TeV`$ , it is possible that these two chiral violating contributions add to $`\mathrm{\Delta }a_\mu ^{SUSY}10^9.`$

The hypothesis of a large extra dimension, and a simple Higgs doublet, gives way to a strong gravitation exchange producing for a relevant number of Kaluza-Klein states

$$_{\mathrm{𝐞𝐟𝐟}}^{ED}\left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^2\frac{e}{4m_\mu }\overline{\mu }\sigma ^{\alpha \beta }\mu F_{\alpha \beta },$$
(20)
that to satisfy the discrepancy Eq. (1) would require $`\mathrm{\Lambda }TeV`$ which seems excluded by astrophysical observations. An analogous contribution may come from the exchange of an antisymmetric tensor field encountered in string theory .

It is interesting that a model  of breaking of SUSY through boundary conditions in a 5th dimension of radius $`RTeV^1`$ allows to use only one Higgs doublet which would modify the contribution to $`a_\mu `$ given by Eq. (19).

The possibility of a new abelian gauge symmetry felt by muon and tauon but not by electron  would give an additional quadratic contribution to $`a_\mu `$ similar to that of the exchange of $`Z`$ of the second term of Eq. (4) which might be $`10^9`$. Mixing of the two neutral gauge bosons may produce  a linear correction of $`a_\mu .`$

Finally, the models of substructure of muons are different in the sense that they do not correspond simply to add new particles to those of the SM. Their effect to $`a_\mu `$ depends on the model assumptions.

One reasoning  is that since the terms of mass and anomalous magnetic moment of muon have the same chiral structure, the scale of substructure should enter into them as $`\mathrm{\Lambda }\overline{\mu }\mu `$ and $`\frac{e}{\mathrm{\Lambda }}\overline{\mu }\sigma ^{\alpha \beta }\mu F_{\alpha \beta }`$ , respectively. One would expect that in the same way as a decreasing factor $`\frac{m_\mu }{\mathrm{\Lambda }}`$ perhaps related to a chiral symmetry must be introduced in the former, a similar one in the latter should give $`\mathrm{\Delta }a_\mu \left(\frac{m_\mu }{\mathrm{\Lambda }}\right)^2.`$

However, a specific model  which assumes the appearance at a scale $`\mathrm{\Lambda }`$ of a Yukawa-type vertex $`\mu ^{}\pi ^{}N`$ , with a heavy neutrino $`N,`$ gives a linear correction $`\mathrm{\Delta }a_\mu \frac{m_\mu }{\mathrm{\Lambda }}`$ since the WS is violated because the pion field has nothing to do with $`m_\mu .`$

## 5 Conclusion

We have seen that interactions which break chiral symmetry together with change of sign of muon mass favour the contribution of new physics to the anomalous magnetic moment $`a_\mu .`$ In this way, parameter regions of MSSM, additional neutral gauge interactions, particular models of muon substructure, or even a GUT alternative of strong mixing of ordinary left lepton doublet with the exotic one of $`E_6`$ together with a small mixture of the corresponding right charged component, may explain the discrepancy between the recent experimental measurement of $`a_\mu `$ and its calculation within Standard Model. It is obviously too soon to say that the need of physics beyond the SM has been proved since the above discrepancy is so far only a 2$`\sigma `$ effect.

> Acknowledgements

The authors thank Ernest Ma for interesting discussions. The work of H. Ch. was financially supported by CNPq of Brazil.