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# Four-wave mixing at maximum coherence and eliminated Doppler broadening controlled with the driving fields

## 1 Introduction

The concept of quantum coherence and interference plays an important role in resonant nonlinear optics and spectroscopy . Coherent coupling of laser radiation with multilevel quantum schemes has been used to manipulate energy level populations, nonlinear-optical response, refraction and absorption of a resonance medium . Much attention has been shown to four-wave mixing (FWM) processes with maximal coherence on a Raman transition  based on the effect of coherence population trapping (CPT) , which allows a dramatic increase of conversion efficiency. In far-from-degenerate schemes, substantial Doppler broadening of the resonant quantum transitions gives rise to inhomogeneous coupling of the driving fields with the atoms in different velocity intervals. Therefore, under relatively low intensities, only a small fraction of the atoms can be concurrently coupled with both the fields driving the Raman transition and, as a consequence, the CPT conditions can not be fulfilled for the entire thermal velocity interval. This fundamental limitation in resonant nonlinear optics of gases substantially reduces the efficiency of the corresponding processes. The common methods of Doppler-free (DF) nonlinear spectroscopy entail ladder energy level schemes and equal frequency counter-propagating beams. This usually leads to large detunings from the intermediate resonance and consequently a decrease of the nonlinear susceptibility. Besides that, the method can not be applied to FWM processes in ladder schemes, due to the phase-matching requirements, and in Raman-type schemes due to the difference in frequencies of the coupled fields.

The technique, allowing one to overcome this obstacle by compensating for Doppler frequency shifts with light-induced ac-Stark shifts and thus enabling one to couple a wide velocity interval concurrently, has been proposed in . This was developed in further publications  and most recently in publications  addressing FWM under conditions where CPT is not possible. Related effects in the absorption index were also investigated recently .

We further mean CPT as the process where two driving fields form nearly equal velocity-averaged populations of the levels at Raman transitions, while the velocity-averaged population of the intermediate state is much less. Along with this absorption and amplification indices for the couple fields reach minimum. On the other hand coherence in the Raman transition, which is origin of FWM, approaches maximum. That allows one to accomplish a maximum of the conversion efficiency. The conditions to achieve CPT may differ from those required for the DF Raman-type resonance. This present paper is aimed at investigating what are the most favorable conditions to accomplish effective FWM frequency conversion of radiation at a low fundamental radiation level. This also addresses the problem “nonlinear optics at the level a few photons per atom” .

## 2 Theoretical

### 2.1 Atomic coherence and energy level populations

Consider a Raman-type scheme of FWM, $`\omega _S=\omega _1\omega _2+\omega _3`$, depicted in Fig. 1, where $`E_1`$ and $`E_2`$ with frequencies $`\omega _1`$ and $`\omega _2`$ are traveling waves of the driving fields. The field $`E_3`$ with the frequency $`\omega _3`$ and generated radiation $`E_S`$ with the frequency $`\omega _S`$ are assumed weak (i.e., not changing the level populations). All waves are co-propagated. Initially, only the lower level $`\mathit{0}`$ is populated. The steady-state solution for the off-diagonal elements of the density matrix (atomic coherence) can be found in the same form of traveling waves as the the resonant driving radiations. Then the equations for the density matrix amplitudes to the lowest order in $`E_{3,S}`$ can be written as

$`P_{01}r_{01}=i\left[G_{01}(r_1r_0)G_{21}r_{02}\right],P_{21}r_{21}=i\left[G_{21}(r_1r_2)G_{01}r_{20}\right],`$
$`P_{02}r_{02}=i\left[G_{01}r_{12}G_{12}r_{01}\right];`$ (1)
$`\mathrm{\Gamma }_1r_1=2\text{Re }[iG_{12}r_{21}+iG_{10}r_{01}],\mathrm{\Gamma }_2r_2=2\text{Re }[iG_{12}r_{21}]+\gamma _2r_1,`$
$`r_0+r_1+r_2=1;`$ (2)
$`P_{23}r_{23}=i\left[G_{23}r_2+G_{21}r_{13}G_{03}r_{20}\right],`$
$`P_{03}r_{03}=i\left[G_{03}r_0+G_{01}r_{13}G_{23}r_{02}\right],`$
$`P_{13}r_{13}=i\left[G_{12}r_{23}G_{23}r_{12}+G_{10}r_{03}G_{03}r_{10}\right]`$ (3)
Here $`r_{ij}`$ and $`r_i`$ are the amplitudes of the off-diagonal and diagonal elements of the density matrix, $`P_{ij}=\mathrm{\Gamma }_{ij}+i(\mathrm{\Omega }_lk_lv)`$, $`\mathrm{\Omega }_l`$ is the resonance detuning for the corresponding resonant field (e.g., $`\mathrm{\Omega }_1=\omega _1\omega _{01}`$), $`\mathrm{\Gamma }_{ij}`$ are homogeneous half-widths of the transitions (coherence relaxation rates), $`v`$ is the projection of the atom velocity on the direction of the wave vectors $`𝐤_l`$, $`\gamma _{1,2}`$ are relaxation rates from level $`\mathit{1}`$ to $`\mathit{0}`$ and from $`\mathit{1}`$ to $`\mathit{2}`$, accordingly, $`\mathrm{\Gamma }_1,\mathrm{\Gamma }_2`$ are relaxation rates of the populations of the levels $`\mathit{1}`$ and $`\mathit{2}`$ accordingly, $`G_{ij}=E_jd_{ij}/2\mathrm{}`$ are the Rabi frequencies, and $`d_{ij}`$ are the electric dipole momenta of the transitions. Only the resonant couplings are accounted for.

The solution for the coherence $`r_{02}`$ and for those at the allowed transitions, which determine absorption and refraction at the frequencies $`\omega _1`$, $`\omega _2`$, $`\omega _3`$, are found in the form

$`r_{02}={\displaystyle \frac{G_{01}G_{12}}{\stackrel{~}{P}_{02}}}\left\{{\displaystyle \frac{\mathrm{\Delta }r_{10}}{P_{01}}}{\displaystyle \frac{\mathrm{\Delta }r_{21}}{P_{21}^{}}}\right\}={\displaystyle \frac{G_{01}G_{12}}{P_{01}P_{21}^{}}}R_{02},`$
$`r_{01}=i{\displaystyle \frac{G_{01}}{P_{01}}}\left\{\mathrm{\Delta }r_{10}{\displaystyle \frac{|G_{12}|^2}{\stackrel{~}{P}_{02}}}\left({\displaystyle \frac{\mathrm{\Delta }r_{10}}{P_{01}}}{\displaystyle \frac{\mathrm{\Delta }r_{21}}{P_{21}^{}}}\right)\right\}=i{\displaystyle \frac{G_{01}}{P_{01}}}R_1,`$
$`r_{12}=i{\displaystyle \frac{G_{12}}{P_{21}^{}}}\left\{\mathrm{\Delta }r_{21}+{\displaystyle \frac{|G_{01}|^2}{\stackrel{~}{P}_{02}}}\left({\displaystyle \frac{\mathrm{\Delta }r_{10}}{P_{01}}}{\displaystyle \frac{\mathrm{\Delta }r_{21}}{P_{21}^{}}}\right)\right\}=i{\displaystyle \frac{G_{12}}{P_{21}^{}}}R_2,`$
$`r_{23}=i{\displaystyle \frac{G_{23}}{P_{23}}}\left\{r_2\left(1{\displaystyle \frac{|G_{12}|^2}{P_{23}\stackrel{~}{P}_{13}}}\right){\displaystyle \frac{|G_{01}G_{12}|^2}{P_{03}\stackrel{~}{P}_{13}}}{\displaystyle \frac{R_{02}}{P_{01}P_{21}^{}}}{\displaystyle \frac{|G_{12}|^2}{P_{21}^{}\stackrel{~}{P}_{13}}}R_2\right\},`$
where $`\mathrm{\Delta }r_{ij}`$ are intensity-dependent population differences, and $`\stackrel{~}{P}_{02}`$ and $`\stackrel{~}{P}_{13}`$ are two-photon denominators “dressed” by the driving fields:

$`\stackrel{~}{P}_{02}=P_{02}+{\displaystyle \frac{|G_{01}|^2}{P_{21}^{}}}+{\displaystyle \frac{|G_{12}|^2}{P_{01}}},\stackrel{~}{P}_{13}=P_{13}+{\displaystyle \frac{|G_{01}|^2}{P_{03}}}+{\displaystyle \frac{|G_{12}|^2}{P_{23}}}.`$ (4)
The coherence $`r_{03}`$ consists of two terms. One, $`\overline{r}_{03}`$, determines absorption and refraction at the frequency $`\omega _S`$, and the other, $`\stackrel{~}{r}_{03}`$, determines FWM at $`\omega _1\omega _2+\omega _3=\omega _S`$:

$`\overline{r}_{03}=i{\displaystyle \frac{G_{03}}{P_{03}}}\left\{r_0\left(1{\displaystyle \frac{|G_{01}|^2}{P_{03}\stackrel{~}{P}_{13}}}\right){\displaystyle \frac{|G_{01}G_{12}|^2}{P_{23}\stackrel{~}{P}_{13}}}{\displaystyle \frac{R_{02}^{}}{P_{01}^{}P_{21}}}+{\displaystyle \frac{|G_{01}|^2}{P_{01}^{}\stackrel{~}{P}_{13}}}R_1^{}\right\},`$ (5)
$`\stackrel{~}{r}_{03}=i{\displaystyle \frac{G_{01}G_{12}G_{23}}{P_{01}P_{21}^{}P_{03}}}\left\{R_{02}\left({\displaystyle \frac{|G_{01}|^2}{P_{03}\stackrel{~}{P}_{13}}}1\right)+{\displaystyle \frac{P_{01}P_{21}^{}}{\stackrel{~}{P}_{13}}}\left({\displaystyle \frac{r_2}{P_{23}}}+{\displaystyle \frac{R_2}{P_{21}^{}}}\right)\right\},`$ (6)
where $`P_{03}=\mathrm{\Gamma }_{03}+i(\mathrm{\Omega }_1\mathrm{\Omega }_2+\mathrm{\Omega }_3k_Sv)`$ and $`k_S=k_1k_2+k_3.`$

Making use of the above equations, the solution for the populations can be found from (2) as

$`r_2={\displaystyle \frac{Y_1W_{02}Y_3W_{01}}{Y_1Y_4Y_3Y_2}},r_1={\displaystyle \frac{Y_4W_{01}Y_2W_{02}}{Y_1Y_4Y_3Y_2}},r_0=1r_1r_2,`$ (7)
where

$`Y_1=2W_{01}W_{02}+\gamma _1,Y_2=W_{02}+W_{01}+\mathrm{\Gamma }_2,`$
$`Y_3=W_{02}W_{21}\gamma _2,Y_4=W_{02}+W_{21}+\mathrm{\Gamma }_2,`$
and

$`W_{01}=2|G_{01}|^2\text{Re }\left\{\left(1{\displaystyle \frac{|G_{12}|^2}{P_{01}\stackrel{~}{P}_{02}}}\right)/P_{01}\right\},`$
$`W_{21}=2|G_{12}|^2\text{Re }\left\{\left(1{\displaystyle \frac{|G_{01}|^2}{P_{21}^{}\stackrel{~}{P}_{02}}}\right)/P_{21}^{}\right\},`$
$`W_{02}=2|G_{01}|^2|G_{12}|^2\text{Re }\left\{1/P_{01}P_{21}^{}\stackrel{~}{P}_{02}\right\}.`$
### 2.2 Coherence-induced Doppler-free resonance

The appearance of a DF resonance and therefore the coupling of molecules from a wide velocity interval can be understood as follows. Ac-Stark shifts $`\text{Im }\left\{|G_{01}|^2/P_{21}^{}\right\}`$ and $`\text{Im }\left\{|G_{12}|^2/P_{01}\right\}`$ in (4), originating from the coherence $`\textcolor[rgb]{1,0,0}{r}_{\textcolor[rgb]{1,0,0}{02}}`$, depend on the radiation intensity and frequency detunings. The later ones, in turn, depend on Doppler shifts. This allows one, by making judicious choice of the intensities and detunings of the driving fields, to “draw” into the dressed two-photon resonance all the molecules, independent of their velocities. In the limiting case, when the detuning from the intermediate resonance is much greater than the Doppler HWHM of the allowed optical transitions, the modified two-photon resonance described by the denominator $`\stackrel{~}{P}_{02}`$ can be presented in the lowest order in $`k_{1,2}v/\mathrm{\Omega }_{1,2}`$ as

$$\stackrel{~}{P}_{02}=\stackrel{~}{\mathrm{\Gamma }}_{02}+i\stackrel{~}{\mathrm{\Omega }}_{02}i\left\{\left(1+\frac{|G_{12}|^2}{\mathrm{\Omega }_1^2}\right)k_1\left(1+\frac{|G_{01}|^2}{\mathrm{\Omega }_2^2}\right)k_2\right\}v,$$
(8)
where $`\stackrel{~}{\mathrm{\Gamma }}_{02}=\mathrm{\Gamma }_{02}+{\displaystyle \frac{|G_{01}|^2}{\mathrm{\Omega }_2^2}}\mathrm{\Gamma }_{12}+{\displaystyle \frac{|G_{12}|^2}{\mathrm{\Omega }_1^2}}\mathrm{\Gamma }_{01},\stackrel{~}{\mathrm{\Omega }}_{02}=\mathrm{\Omega }_1\mathrm{\Omega }_2+{\displaystyle \frac{|G_{01}|^2}{\mathrm{\Omega }_2}}{\displaystyle \frac{|G_{12}|^2}{\mathrm{\Omega }_1}}`$ are the power broadened HWHM and ac-Stark shifted two-photon resonance detuning. From (8) it follows that the requirements for the induced Doppler-free resonance to be achieved are $`\stackrel{~}{\mathrm{\Omega }}_{02}=0`$ and $`\stackrel{~}{k_1}=\stackrel{~}{k_2}`$, where
$`\stackrel{~}{k_1}v=\left(1+{\displaystyle \frac{|G_{12}|^2}{\mathrm{\Omega }_1^2}}\right)k_1v`$ and $`\stackrel{~}{k_2}v=\left(1+{\displaystyle \frac{|G_{01}|^2}{\mathrm{\Omega }_2^2}}\right)k_2v`$
are intensity-dependent Doppler shifts. Eventually the equations take form

$`k_1\left(1+{\displaystyle \frac{|G_{12}|^2}{\mathrm{\Omega }_1^2}}\right)k_2\left(1+{\displaystyle \frac{|G_{01}|^2}{\mathrm{\Omega }_2^2}}\right)=0,`$ (9)
$`\mathrm{\Omega }_1\left(1{\displaystyle \frac{|G_{12}|^2}{\mathrm{\Omega }_1^2}}\right)\mathrm{\Omega }_2\left(1{\displaystyle \frac{|G_{01}|^2}{\mathrm{\Omega }_2^2}}\right)=0.`$ (10)
From (9)-(10) follows a cubic equation as $`\mathrm{\Omega }_2`$:

$$\mathrm{\Omega }_{2r}^3(2K)\mathrm{\Omega }_{2r}^2\mathrm{\Omega }_1\mathrm{\Omega }_{2r}|G_{01}|^2+K\mathrm{\Omega }_1|G_{01}|^2=0,K=k_2/k_1,$$
(11)
which determines the detuning of field $`E_2`$, corresponding to the induced resonance, under given values of the Rabi frequency and detuning of field $`E_1`$. Here, the Rabi frequency of $`E_2`$ must be

$$|G_{12}|^2=\mathrm{\Omega }_1^2\left\{K\left(1+\frac{|G_{01}|^2}{\mathrm{\Omega }_{2r}^2}\right)1\right\}.$$
(12)
One of the roots of the equation (11) corresponds to the dressed DF two-photon resonance,

$$\mathrm{\Omega }_{2r}=(A^{1/3}+9B+2\mathrm{\Omega }_1\mathrm{\Omega }_1K)/3,$$
(13)
where $`A=9\mathrm{\Omega }_1|G_{01}|^2(12K)+\mathrm{\Omega }_1^3(812K+6K^2K^3)+3[3\mathrm{\Omega }_1^2|G_{01}|^4\times `$

$`\times (18K+11K^2)+3\mathrm{\Omega }_1^4|G_{01}|^2(8K+12K^26K^3+K^4)3|G_{01}|^6]^{1/2}`$,

$`B=(|G_{01}|^2+4\mathrm{\Omega }_1^24\mathrm{\Omega }_1^2K+\mathrm{\Omega }_1^2K^2)/3A^{1/3},K=k_2/k_1.`$

The conditions for the CPT and DF resonances may fit each other or differ, depending on the specific case. This and corresponding outcomes regarding FWM will be investigated below numerically for the most optimum situations, where the analytical solution can not be obtained.

## 3 Numerical analysis

The graphs presented below are computed numerically based on averages over the velocity equations (5), (6) and (7). For the numerical analysis we have used the parameters of the sodium dimer transition with the following wavelengths : $`X^1\mathrm{\Sigma }_g^+(v^{\prime \prime }=3,J^{\prime \prime }=43)`$$`B^1\mathrm{\Pi }_u(6,43)(\lambda _{01}=488`$ nm) – $`X^1\mathrm{\Sigma }_g^+(13,43)`$ $`(\lambda _{21}=525`$ nm) – $`A^1\mathrm{\Sigma }_u^+(24,44)(\lambda _{23}=655`$ nm) – $`X^1\mathrm{\Sigma }_g^+(3,43)(\lambda _{13}=598`$ nm). The corresponding homogeneous half-widths of the transition are 20.69, 23.08, 18.30 and 15.92 MHz, whereas the Doppler half-widths $`\mathrm{\Delta }\omega _{iD}`$ are equal to 0.92, 0.85, 0.68 and 0.75 GHz. The numerical simulations allow us to analyze the velocity-averaged equation for the detunings, where the approximation taken in (8) is not valid.

### 3.1 Nonlinear resonances in FWM polarizations, in absorption indices and in the level populations

Figure 2, plots 1 illustrate the coherence-induced compensation of Doppler shifts with ac-Stark shifts resulting in the resonance narrowing in the squared module of the velocity-averaged reduced nonlinear FWM polarizations

$`|\stackrel{~}{P}_4|^2=(|\stackrel{~}{\chi }_4|^2/|\stackrel{~}{\chi }_{40}|^2)|g_{01}|^2|g_{12}|^2`$ \[Fig.2 (a)\] and $`|\stackrel{~}{P}_3|^2=(|\stackrel{~}{\chi }_3|^2/|\stackrel{~}{\chi }_{40}|^2)|g_{01}|^2|g_{12}|^2`$ \[Fig.2 (b)\]. The nonlinear susceptibility is reduced by its maximum value in the same frequency range, but for negligibly-weak $`E_1`$ and $`E_2`$ fields, $`g_{01}=G_{01}/\mathrm{\Delta }\omega _{1D}`$, $`g_{12}=G_{12}/\mathrm{\Delta }\omega _{2D}`$. A substantial narrowing is seen from comparison with the subplot, presenting the spectral dependence of the velocity-averaged squared module of the same susceptibility, but in the negligibly weak fields, normalized to unity. The HWHM of the resonance in the subplot is approximately 70 MHz, which corresponds to the Doppler width of the nonperturbated Raman transition, whereas the HWHM of the resonance in plots 1 is 15 MHz. This indicates some power and residual Doppler broadening. The Rabi frequencies of the fields $`E_1`$ and $`E_2`$ are equal to 157 MHz and 85 MHz. The detuning of $`E_1`$ is equal to 413.8 MHz ($`0.45\mathrm{\Delta }\omega _{1D}`$), and detuning of $`E_3`$ is equal to -695.5 MHz ($`1.02\mathrm{\Delta }\omega _{3D}`$). Plots 2 display the same dependences, but related to the CPT conditions (the half-width of this resonance in $`|\stackrel{~}{P}_4|^2`$ is 200 MHz). In this case, the required Rabi frequencies of $`E_1`$ and $`E_2`$ are equal to 351 MHz and 332 MHz, respectively, while the detunings are identical to those in plots 1. Plots 3 display the same dependence, but under the intensities, that provide narrowing in the intermediate range (HWHM of resonance is 70 MHz). In this case, the Rabi frequencies of the fields $`E_1`$ and $`E_2`$ are equal to 222 MHz and 235 MHz, respectively, whereas the detunings are the same as in the previous plots. The important outcome is that in the Doppler-free regime, larger FWM polarizations can be accomplished under lower driving fields. Also, we want to stress the substantial difference in magnitudes of the nonlinear susceptibilities $`\chi _4`$ and $`\chi _3`$, which follows from the interference of contributions of molecules in different velocity intervals to the macroscopic nonlinear polarizations.

Figure 3(a) shows dependence of the velocity integrated populations on the detuning of the field $`E_2`$, while the Rabi frequencies of $`E_1`$ and $`E_2`$ are equal to 351 MHz and 332 MHz, respectively so that the CPT conditions can be fulfilled under appropriate detuning. The subplot displays the distribution of the populations over velocities, whereas the detuning corresponds to the CPT regime for the velocity-integrated populations. Here $`u`$ is the thermal velocity with Maxwell envelope removed. The subplot indicates CPT for molecules in $`\textcolor[rgb]{1,0,0}{v}\textcolor[rgb]{1,0,0}{=}\textcolor[rgb]{1,0,0}{0}`$; however, even inversion of the populations occurs in a relatively wide velocity intervals.

Figure 3(b) is computed for the Rabi frequencies of the fields $`E_1`$ and $`E_2`$ equal to 157 MHz and 85 MHz, respectively. The inset displays the distribution of the populations over velocities at the detuning corresponding to DF. The distribution is even more complicated compared to that in the previous case.

Figure 4 displays velocity-averaged absorption indices vs detuning of the field $`E_2`$.

The intensities of the fields are the same as in the corresponding graphs given above. The graph 4 (a) shows a substantially decreased absorption index for the first field due to saturation effects, which is almost independent of the detuning of the second field because of its relative weakness. The second field experiences Stokes gain. The plot for the generated beam (reduced by 10) displays a nonlinear resonance in the absorption index. With growth of the second field intensity, so that CPT becomes possible, both absorption of the first and gain of the second driving field experience substantial decrease in the CPT regime. Absorption of the generated field dramatically changes as well (Figure 4 (a)).

A linear approximation in $`k_{1,2}v/\mathrm{\Omega }_{1,2}`$ (see equation (8)) is valid for large detunings from the intermediate resonance. While for tuning close to the resonance, the concurrently coupled velocity interval decreases, the nonlinear response of the molecules grows. At the same time, absorption of the coupled radiations increases as well.

The output FWM generated radiation is determined by the interplay of the above considered processes. Moreover, resonant FWM may not be viewed as a sequence of the independent elementary acts of absorption, gain and FWM. Interference of these elementary processes plays a crucial role, even for a qualitative prediction of the spatial dynamics of the generated field . Therefore, appropriate optimization is required in order to achieve the maximum FWM-generation output. In the next section, relevant results are presented based on the above analyzed dependencies.

### 3.2 Coherent quantum control of FWM in a double-$`\mathrm{\Lambda }`$ Doppler broadened medium

The solution of the Maxwell equations for the coupled traveling waves can be found in the form

$$E^j(z,t)=\text{Re }\{E_j(z)\mathrm{exp}[\mathrm{i}(\omega _jtk_jz)]\},$$
(14)
where $`k_j`$ are complex wave number at the corresponding frequencies, $`k_j=k_j^{}\mathrm{i}\alpha _j/2`$. The set of the equations for the amplitudes, relevant to the case under consideration, is

$`{\displaystyle \frac{dE_1}{dz}}={\displaystyle \frac{\alpha _1}{2}}E_1,{\displaystyle \frac{dE_2}{dz}}={\displaystyle \frac{\alpha _2}{2}}E_2,`$ (15)
$`{\displaystyle \frac{dE_3}{dz}}={\displaystyle \frac{\alpha _3}{2}}E_3+\sigma _3E_1^{}E_2E_S\mathrm{exp}\{i\mathrm{\Delta }kz\},`$ (16)
$`{\displaystyle \frac{dE_S}{dz}}={\displaystyle \frac{\alpha _S}{2}}E_S+\sigma _SE_1E_2^{}E_3\mathrm{exp}\{i\mathrm{\Delta }kz\},`$ (17)
where $`\sigma _3=i2\pi k_3\stackrel{~}{\chi _3}`$ and $`\sigma _S=i2\pi k_S\stackrel{~}{\chi _S}`$ are cross coupling parameters, $`\stackrel{~}{\chi _3}`$ and $`\stackrel{~}{\chi _S}`$ are intensity-dependent nonlinear susceptibilities for the FWM processes $`\omega _S\omega _1\omega _2+\omega _3`$ and $`\mathrm{\Delta }k=k_Sk_1+k_2k_3`$. The boundary conditions are $`E_l(z=0)=E_{0l}`$ ($`l=1,2,3`$) and $`E_S(z=0)=0`$. We assume that intensities of the weak waves with frequencies $`\omega _3`$ and $`\omega _S`$ are weak enough so that the change of the strong fields $`E_{1,2}`$ due to FWM conversion can be neglected. The quantum efficiency of conversion QEC of the radiation $`E_3`$ in $`E_S`$ is defined by the equation

$$\eta _\mathrm{q}=(\omega _3/\omega _S)|E_S(z)/E_3(0)|^2\mathrm{exp}(\alpha _Sz).$$
(18)
Assuming that the condition of phase matching $`\mathrm{\Delta }k^{}=0`$ can be ensured (e.g., with a buffer gas), the solution for QEC of the above given equations can be expressed as

$`\eta _q={\displaystyle \frac{\omega _3}{\omega _S}}|{\displaystyle \frac{\sigma _S}{g_0}}|^2|E_{01}E_{02}|^2\mathrm{exp}\left[(\text{Re }g_0{\displaystyle \frac{\alpha }{2}})z\right]|1\mathrm{exp}(g_0z)|^2,`$
$`g_0=[\left[(\alpha _1+\alpha _2+\alpha _3\alpha _S/2)\right]^2+4\sigma _S\sigma _3|E_{01}E_{02}|^2]^{1/2},\alpha =\alpha _3+\alpha _S.`$
These formulas account for nonlinear resonances both in FWM nonlinear polarizations and in absorption indices. In order to compute the absolute magnitude of QEC (under the assumption of $`\mathrm{\Delta }k^{}=0`$) we have used the data for the Frank-Condon factors of 0.068, 0.142, 0.02 and 0.036 for the transition with wavelengths $`\lambda _{01}`$, $`\lambda _{21}`$, $`\lambda _{23}`$ and $`\lambda _{03}`$ accordingly.

Figure 5 presents a numerical simulation of the evolution of QEC along the vapor cell. The distance is scaled to the resonance optical density $`\alpha _{01}z`$ with the driving fields being turned off. The plot 1 corresponds to the case where the conditions for Doppler compensation at the transition 0–2 are fulfilled on the entrance of the cell. The Doppler-free resonance would be narrower if one of the coupled fields were weak. However, that would give rise to larger absorption and to decreased nonlinear FWM polarization. The optimization accounting for the change of the driving fields along the medium also shows that it does not substantially change the optimum input intensity values for the plots presented in Fig. 5. Plot 2 displays the same dependence, but for the optimum CPT conditions. Alternatively, they are not optimum for the elimination of Doppler broadening.

The maxima of these two curves are comparable, but in the Doppler- free regime, quite lower intensities of the fundamental radiations are required. Plot 3 displays a similar dependence in the intermediate case. All intensities and detunings are identical to those used for computing the previous figures.

For the transitions under consideration, the Rabi frequency on the level of 100 MHz corresponds to powers of about 100 mW focused on a spot on the order of $`10^4`$ cm<sup>2</sup>, which can be realized with common cw lasers with the confocal parameter of focusing of about 2.5 cm. At a temperature of about 700 K, the optimum optical density of the dimers is achievable for vapor lengths of about 2 cm. This is in accord with the parameters of typical cw FWM experiments (see, e.g. ).

The above indicated intensity corresponds to about $`10^{11}`$ photons per cubic centimeter. Accounting for the molecule number density at the indicated temperature, which is on the order on $`10^{13}`$ cm<sup>-3</sup>, we have about $`\textcolor[rgb]{1,0,0}{10}^\textcolor[rgb]{1,0,0}{}\textcolor[rgb]{1,0,0}{2}`$ photon/molecule.

## 4 Conclusion

Coherent control of populations  and of four-wave mixing  with pulses shorter than the dephasing time $`T_2`$ has proven to be a powerful tool for manipulating nonlinear-optical and chemical properties of free atoms and molecules. In these cases, maximum coherence can be achieved as a result of Rabi oscillations of the two-photon transition, and the required driving intensity is much higher than that proposed in this paper. Consequently, Doppler broadening of the coupled transitions does not play an important role.

On the contrary, this paper considers coherent quantum control of resonant four-wave mixing processes, where Doppler-broadening of a double-$`\mathrm{\Lambda }`$ medium is the factor of crucial importance. An approach enabling one to enhance the efficiency of nonlinear optical conversion and, at the same time, to decrease the required intensity for the fundamental pump beams is proposed. This approach is based on the elimination of Doppler broadening of the resonant two-photon transition. The advantages of the proposed method as compared to those based on coherent population trapping, where inhomogeneous broadening may play important role too, are illustrated with numerical simulations for realistic experimental schemes. The results obtained contribute to the field of nonlinear optics at the level of several photons per atom, which is currently attracting growing interest.

## 5 Acknowledgments

TFG and AKP thank U.S. National Research Council - National Academy of Sciences for support of this research through the international Collaboration in Basic Science and Engineering (COBASE) program. AKP and ASB acknowledge funding support from the International Association of the European Community for the promotion of co-operation with scientists from the New Independent States of the former Soviet Union (INTAS) (grant INTAS-99-19) and Russian Foundations for Basic Research (grant 99-02-39003) and from the Center on Fundamental Natural Sciences at St. Petersburg University (grant 97-5.2-61).


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# On the Jones polynomials of checkerboard colorable virtual knots

## 1 Introduction

In 1996, L. H. Kauffman introduced the notion of a virtual knot, which is motivated by study of knots in a thickened surface and abstract Gauss codes, cf. . M. Goussarov, M. Polyak, and O. Viro  proved that the natural map from the category of classical knots to the category of virtual knots is injective; namely, if two classical knot diagrams are equivalent as virtual knots, then they are equivalent as classical knots. Thus, virtual knot theory is a generalization of knot theory. It is also found in their paper  that the notion of a virtual knot is helpful to study of finite type invariants.

Kauffman defined the Jones polynomial of a virtual knot, which is also called the normalized bracket polynomial or the $`f`$-polynomial (cf. ). In this paper, according to , we call it the $`f`$-polynomial instead of the Jones polynomial, since the definition is different from Jones’ in . Finite type invariants derived from the $`f`$-polynomials are studied in , and it is proved that a certain property of them (Corollary 14 of ) is hold in the category of virtual knots.

The $`f`$-polynomial (Jones polynomial) of a virtual link is quite different from $`f`$-polynomials of classical links. For a Laurent polynomial $`f`$ on valuable $`A`$, we denote by $`\mathrm{EXP}(f)`$ the set of integers appearing as exponents of $`f`$. For example, if $`f=3A^2+6A7A^5`$, then $`\mathrm{EXP}(f)=\{2,1,5\}`$. It is well-known that for a classical link $`L`$ with $`n`$ components, the $`f`$-polynomial satisfies that $`\mathrm{EXP}(f)4𝐙`$ if $`n`$ is odd, and $`\mathrm{EXP}(f)4𝐙+2`$ if $`n`$ is even. However, this is not true for a virtual knot/link in general. In this paper we introduce the notion of checkerboard coloring of a virtual link diagram as a generalization of checkerboard coloring of a classical link diagram.

###### Theorem 1

Let $`f`$ be the $`f`$-polynomial of a virtual link $`L`$ with $`n`$ components. Suppose that $`L`$ has a virtual link diagram which admits a checkerboard coloring. Then $`\mathrm{EXP}(f)4𝐙`$ if $`n`$ is odd, and $`\mathrm{EXP}(f)4𝐙+2`$ if $`n`$ is even.

For example the virtual knot diagram illustrated in Figure 1 (a) admits a checkerboard coloring and the $`f`$-polynomial is $`A^4+A^{12}A^{16}`$. So $`\mathrm{EXP}(f)4𝐙`$. On the other hand, virtual knot diagram illustrated in Figure 1 (b) does not admit a checkerboard coloring and the $`f`$-polynomial is $`A^{10}+A^6+A^4`$. Theorem 1 implies that this diagram is never equivalent to a diagram that admits a checkerboard coloring.

If a virtual link diagram is alternating (the definition is given later), then the diagram admits a checkerboard coloring. Thus we have the following.

###### Corollary 2

Let $`f`$ be the $`f`$-polynomial of a virtual link $`L`$ with $`n`$ components. Suppose that $`L`$ has an alternating virtual link diagram. Then $`\mathrm{EXP}(f)4𝐙`$ if $`n`$ is odd, and $`\mathrm{EXP}(f)4𝐙+2`$ if $`n`$ is even.

By this corollary, we see that the virtual knot represented by Figure 1 (b) is not equivalent to an alternating diagram.

## 2 Virtual link diagram and abstract link diagram

A virtual link diagram is a closed oriented 1-manifold generically immersed in $`𝐑^2`$ such that each double point has information of a crossing (as in classical knot theory) or a virtual crossing which is indicated by a small circle around the double point. The moves of virtual link diagrams illustrated in Figure 2 are called generalized Reidemeister moves. Two virtual link diagrams are said to be equivalent if they are related by a finite sequence of generalized Reidemeister moves. We call the equivalence class of a virtual link diagram a virtual link.

A pair $`P=(\mathrm{\Sigma },D)`$ of a compact oriented surface $`\mathrm{\Sigma }`$ and a link diagram $`D`$ in $`\mathrm{\Sigma }`$ is called an abstract link diagram (ALD) if $`|D|`$ is a deformation retract of $`\mathrm{\Sigma }`$, where $`|D|`$ is a graph obtained from $`D`$ by replacing each real/virtual crossing point with a vertex. For an ALD, $`P=(\mathrm{\Sigma },D)`$, if there is an orientation preserving embedding $`f:\mathrm{\Sigma }F`$ into a closed oriented surface $`F`$, $`f(D)`$ is a link diagram in $`F`$. We call it a link diagram realization of $`P`$ in $`F`$. In Figure 3, we show two abstract link diagrams and their link diagram realizations. Two ALDs $`P=(\mathrm{\Sigma },D)`$, $`P^{}=(\mathrm{\Sigma }^{},D^{})`$ are related by an abstract Reidemeister move (of type I, II or III) if there is a closed oriented surface $`F`$ and link diagram realizations of $`P`$ and $`P^{}`$ in $`F`$ which are related by a Reidemeister move (of type I, II or III) in $`F`$. Two ALDs are equivalent if they are related by a finite sequence of abstract Reidemeister moves. We call the equivalence class of an ALD an abstract link.

In  a map

$$\varphi :\{\text{virtual link diagrams}\}\{\text{ALDs}\}$$

was defined. The idea of this map is illustrated in Figure 4. Refer to  for the definition. We call $`\varphi (D)`$ an ALD associated with a virtual link diagram $`D`$. The ALDs in Figure 3 (a) and (b) are ALDs associated with the virtual link diagrams in Figure 1 (a) and (b) respectively.

###### Theorem 3

() The map $`\varphi `$ induces a bijection

$$\mathrm{\Phi }:\{\text{virtual links}\}\{\text{abstract links}\}$$

.

Let $`P=(\mathrm{\Sigma },D)`$ be a pair of a compact oriented surface $`\mathrm{\Sigma }`$ and a link diagram $`D`$ in $`\mathrm{\Sigma }`$. A checkerboard coloring is a coloring of the all components of $`\mathrm{\Sigma }|D|`$ by two colors, say black and white, such that two components of $`\mathrm{\Sigma }|D|`$ which are adjacent by an edge of $`D`$ have always distinct colors.

We say that a virtual link diagram admits a checkerboard coloring or it is checkerboard colorable if the associated ALD admits a checkerboard coloring.

## 3 The $`f`$-polynomials of abstract link diagrams

An ALD, $`P=(\mathrm{\Sigma },D)`$, is said to be unoriented if the diagram $`D`$ is unoriented. There is a unique map

$$<>:\{\text{unoriented ALDs}\}\mathrm{\Lambda }=𝐙[A,A^1]$$

satisfying the following rules.

1. $`<T>_F=1`$ where $`T`$ is a one-component trivial ALD,
2. $`<TD>=(A^2A^2)<D>`$ if $`D`$ is not empty, where $``$ means the disjoint union, and
3. $`<\text{}>=A<\text{}>+A^1<\text{}>`$.

Then $`<>`$ is an invariant under abstract Reidemeister moves II and III. We call it the Kauffman bracket polynomial of ALD, cf. .

Let $`P=(\mathrm{\Sigma },D)`$ be an unoriented ALD. Replacing the neighborhood of a double point as in Figure 5, we have another unoriented ALD. We call it an unoriented ALD obtained from $`D`$ by doing an A-splice  or B-splice  at the crossing point. An unoriented trivial ALD obtained from $`P`$ by doing an A-splice or B-splice at each crossing point is said to be a state  of $`P`$. From the definition of $`<>`$, we see

$$<P>=\underset{S}{}A^{\mathrm{}(S)}(A^2A^2)^{\mathrm{}(S)1},$$

where $`S`$ runs over all of states of $`D`$, $`\mathrm{}(S)`$ is the number of A-splice minus that of B-splice used for obtaining $`S`$ and $`\mathrm{}(S)`$ is the number of components of $`S`$.

For an ALD, $`P=(\mathrm{\Sigma },D)`$, the writhe $`\omega (P)`$ is defined by the number of positive crossings minus the number of negative crossings. Then we define the normalized bracket polynomial or the $`f`$-polynomial of $`P`$ by

$$f_P(A)=(A^3)^{\omega (P)}<P>.$$

By normalizing by $`(A^3)^{\omega (P)}`$, this value is preserved under abstract Reidemeister moves of type I. Thus this is an invariant of an abstract link. This invariant was defined in , where it is called the Jones polynomial of $`P`$. It should be noted that the bijection $`\mathrm{\Phi }`$ preserves the $`f`$-polynomial.

## 4 Proof of Theorem 1

Let $`p`$ be a crossing point of an ALD, $`P=(\mathrm{\Sigma },D)`$. Let $`P_0=(\mathrm{\Sigma }_0,D_0)`$ and $`P_{\mathrm{}}=(\mathrm{\Sigma }_{\mathrm{}},D_{\mathrm{}})`$ be ALDs obtained from $`P`$ by splicing at $`p`$ orientation coherently and orientation incoherently, respectively. Note that $`D_{\mathrm{}}`$ does not inherit an orientation from $`D`$. The crossing point $`p`$ is either (i) a self-intersection of an immersed loop of $`D`$ or (ii) an intersection of two immersed loops. Let $`\alpha `$ and $`\alpha ^{}`$ be the immersed open arcs obtained from the loop (in case (i)) or from the two loops (in case (ii)) by cutting at $`p`$. Choose one of them, say $`\alpha `$, and we give an orientation to $`D_{\mathrm{}}`$ which is induced from that of $`D`$ except $`\alpha `$ (and hence the orientation is reversed on $`\alpha `$). Let $`C`$ be the set of crossing points of $`D`$, except $`p`$, such that the sign of the crossing point does not change in $`D`$ and $`D_{\mathrm{}}`$; in other word, at each crossing point belonging to $`C`$, both of the two intersecting arcs are contained in $`D\alpha `$ or both of them are in $`\alpha `$. Let $`C^{}`$ be the set of crossing points of $`D`$, except $`p`$, such that the sign of the crossing point changes in $`D`$ and $`D_{\mathrm{}}`$; in other word, at each crossing point belonging to $`C^{}`$, one of the two intersecting arcs is contained in $`D\alpha `$ and the other is in $`\alpha `$. Let $`k`$ (or $`\mathrm{}`$, resp.) be the number of positive crossings of $`C`$ (resp. $`C^{}`$) minus the number of negative crossings of $`C`$ (resp. $`C^{}`$).

###### Lemma 4

In the above situation, let $`f`$, $`f_0`$ and $`f_{\mathrm{}}`$ be the $`f`$-polynomials of $`P`$, $`P_0`$ and $`P_{\mathrm{}}`$, respectively. Then we have

$$f=\{\begin{array}{cc}A^2f_0(A^3)^2\mathrm{}A^4f_{\mathrm{}},\hfill & \text{if }p\text{ is a positive crossing,}\hfill \\ A^{+2}f_0(A^3)^2\mathrm{}A^{+4}f_{\mathrm{}},\hfill & \text{if }p\text{ is a negative crossing.}\hfill \end{array}$$

Proof. If $`p`$ is a positive crossing, then the writhes are $`\omega (D)=k+\mathrm{}+1`$, $`\omega (D_0)=k+\mathrm{}`$ and $`\omega (D_{\mathrm{}})=k\mathrm{}`$. Since $`<P>=A<P_0>+A^1<P_{\mathrm{}}>`$, we have the result. The case that $`p`$ is a negative crossing is similar. $`\mathrm{}`$

Remark. In the remark of Section 5 of (page 677), an equation which is similar to Lemma 4 is given. However, it seems to be forgotten there to take account of the term $`(A^3)^2\mathrm{}`$. In consequence, the recursion formula of Theorem 13 of  is as follows:

$$v_n(G_{})=\underset{k=0}{\overset{n1}{}}\frac{2^{nk}}{(nk)!}\{(1(1)^{nk})v_k(G_0)+\{(23\mathrm{})^{nk}(23\mathrm{})^{nk}\}v_k(G_{\mathrm{}})\}.$$

By this formula, Corollary 14 of  is still true.

###### Corollary 5

(cf. Theorem 13 of ) Let $`f`$ be the $`f`$-polynomial of an ALD with $`n`$ components. Then $`f(1)=(2)^{n1}`$. In particular, $`f`$-polynomials of ALDs are not zero.

Proof. It follows from Lemma 4 by induction on the number of (real) crossing points. $`\mathrm{}`$

Since $`\mathrm{\Phi }`$ preserves the $`f`$-polynomials, Theorem 1 is equivalent to the following theorem.

###### Theorem 6

Let $`f`$ be the $`f`$-polynomial of an ALD, $`P=(\mathrm{\Sigma },D)`$, with $`n`$ components. Suppose that $`P`$ admits a checkerboard coloring. Then $`\mathrm{EXP}(f)4𝐙`$ if $`n`$ is odd, and $`\mathrm{EXP}(f)4𝐙+2`$ if $`n`$ is even.

Proof. For a state $`S`$ of $`P`$, we define $`I(S)`$ by

$$I(S)=A^{\mathrm{}(S)}(A^2A^2)^{\mathrm{}(S)1}$$

so that the bracket polynomial of $`P`$ is the sum of $`I(S)`$ for all states $`S`$. Let $`\mathrm{ind}(S)`$ be a value in $`𝐙_4=\{0,1,2,3\}`$ such that $`I(S)4𝐙+\mathrm{ind}(S)`$.

Every state of $`P`$ has a unique checkerboard coloring induced from the checkerboard coloring of $`P`$, see Figure 6. (Figure 7 is an example of an ALD with a checkerboard coloring and a state with the induced checkerboard coloring.) Using this fact, we prove that $`\mathrm{ind}(S)=\mathrm{ind}(S^{})`$ for any states $`S`$ and $`S^{}`$ of $`P`$. It is sufficient to prove this in a special case that $`S`$ and $`S^{}`$ are the same state except a crossing point, say $`p`$, of $`D`$ where $`S`$ and $`S^{}`$ are as in Figure 8. For this state $`S`$, there are two cases (A) and (B) as in Figure 9. The case (C) does not occur, because a state as in (C) does not have a checkerboard coloring induced from the checkerboard coloring of $`P`$. In both cases (A) and (B), we have $`I(S^{})=A^{\mathrm{}(S)\pm 2}(A^2A^2)^{\mathrm{}(S)1\pm 1}`$ and $`\mathrm{ind}(S)=\mathrm{ind}(S^{})`$.

Now we have that $`\mathrm{EXP}(f)4+i`$ where $`i=\mathrm{ind}(S)`$ for any state $`S`$ of $`P`$. We denote this number $`i`$ by $`\mathrm{ind}(f)`$. The remaining task is to prove this index is $`0`$ if $`n`$ is odd, and $`2`$ if $`n`$ is even. This is proved by induction on the number of (real) crossing points of $`P`$. If $`P`$ has no real crossing points, then this is obvious by the definition of the $`f`$-polynomial. If there is a crossing point, say $`p`$, apply Lemma 4. Note that $`P_0`$ and $`P_{\mathrm{}}`$ have checkerboard colorings, and $`\mathrm{EXP}(f_0)4𝐙+\mathrm{ind}(f_0)`$ and $`\mathrm{EXP}(f_{\mathrm{}})4𝐙+\mathrm{ind}(f_{\mathrm{}})`$. Since $`f0`$ and $`f_00`$ (Corollary 5), it follows from the equation in Lemma 4 that $`\mathrm{ind}(f)=\mathrm{ind}(f_0)+2𝐙_4`$. The ALD $`P_0`$ has fewer crossing points than $`P`$ and has a checkerboard coloring. By induction hypothesis, $`\mathrm{ind}(f_0)`$ is $`0`$ if $`n^{}`$ is odd, and $`2`$ if $`n^{}`$ is even, where $`n^{}`$ is the number of components of $`P_0`$. Since $`n^{}=n\pm 1`$, we have that $`\mathrm{ind}(f)`$ is $`0`$ if $`n`$ is odd, and $`2`$ if $`n`$ is even. $`\mathrm{}`$

## 5 Alternating virtual link diagrams and ALDs

An ALD or a virtual link diagram is alternating if we meet over and under crossing points alternatively when we travel along each component of the diagram twice.

###### Lemma 7

For an ALD, $`P=(\mathrm{\Sigma },D)`$, the following conditions are equivalent.

* By applying crossing changes, $`P`$ changes into an alternating ALD.
* $`P`$ has a checkerboard coloring.

Proof of Lemma 7. If $`P`$ has a checkerboard coloring, change each real crossing according to the coloring as in the most left figure of Figure 6. Conversely if $`P`$ is an alternating ALD, then give a checkerboard coloring near each crossing point as in the picture, which is extended to a checkerboard coloring of $`P`$. $`\mathrm{}`$

Proof of Corollary 2. It follows from Theorem 1 and Lemma 7. $`\mathrm{}`$

Remark. M. B. Thistlethwaite  and K. Murasugi  showed that the $`f`$-polynomial (Jones polynomial) of a non-split alternating link is alternating, namely it is in a form of $`A^\alpha c_iA^{4i}`$ such that $`c_ic_j0`$ for $`ij(mod\mathrm{\hspace{0.33em}2})`$ and $`c_ic_j0`$ for $`ij(mod\mathrm{\hspace{0.33em}2})`$. This does not hold in virtual knot theory. The $`f`$-polynomial of a virtual knot in Figure 10 is $`A^{12}+3A^{16}4A^{20}+3A^{24}4A^{28}+4A^{32}3A^{36}+A^{40}`$.