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# Nuclear matter hole spectral function in the Bethe-Brueckner-Goldstone approach

## 1 Introduction

One of the main features of nuclear systems is the relevance of short range correlations (SRC) due to the hard core part of the nucleon-nucleon (NN) potential. These are relevant for the binding energy of the nuclear system in general and are probed directly by the high momentum and energy region of the hole spectral function. In fact, SRC are entirely responsible for this region, where the mean field and the long range correlations can give only negligeable contributions. Spectral functions are extracted mainly from electron-nucleus scattering experiments. Theoretically, many approaches have been proposed for a quantitative description of SRC and the corresponding spectral functions. The many-body aspect appears essential for a correct understanding of the correlations, and Bethe-Brueckner  or variational  methods have been extensively applied. Although the main features of the spectral functions in the region relevant for SRC seem to have a similar trend within different approaches, discrepancies are still present and controversial interpretations of the experimental data exist in the literature. Recently  it was pointed out that the main features of the nucleon spectral function in nuclear matter can be understood in the framework of transport theory. In this approach the only ingredient is the in-medium nucleon-nucoleon cross section, which can be, in first approximation, schematized by a single parameter throughout the entire momentum and energy range. The self-consistent calculation of the single particle self-energy and strength function then provides the nucleon spectral function. Therefore, phase space effects seem to dominate the behaviour of the spectral function.

A close comparison among the results of different approaches appears necessary to extract the characteristics of SRC which determine the strength function. In particular, the dependence of the results on the particular many-body theory as well as on the specific nucleon-nucleon interaction used in the calculations should elucidate the structure of the SRC.

In this letter, we present calculations of the nucleon spectral function in nuclear matter within the Brueckner scheme using different realistic NN interactions and compare them with other approaches. We will concentrate the comparison mainly in the high energy region, where the effect of correlations is dominating.

## 2 Formalism

The hole spectral function in nuclear matter is defined as:

$$S(k,\omega )=\underset{f}{}\left|\mathrm{\Psi }_{A1}^f|a_k|\mathrm{\Psi }_A^0\right|^2\delta \left(\omega \left(E_{A1}^fE_A^0\right)\right)$$
(1)
where $`|\mathrm{\Psi }_A^0`$ is the ground state for $`A`$ nucleons with eigenvalue $`E_A^0`$, $`|\mathrm{\Psi }_{A1}^f`$ is a complete set of states for $`A1`$ nucleons with eigenvalues $`E_{A1}^f`$, and $`a_k`$ is the annihilation operator for the normalized plane wave at momentum $`k`$.

In a single-particle description of nuclei only states with $`k<k_F`$ are occupied and the final states involved in the sum are at most one hole states. In a correlated nucleus, the wave function of the ground state can have high momentum components, and the structure of the spectral function becomes more complicated.

In nuclear matter, the spectral function corresponding to the nucleon self-energy $`M(k,\omega )=V(k,\omega )+iW(k,\omega )`$, is given by the well known result :

$$S(k,\omega )=\frac{1}{\pi }\mathrm{Im}𝒢(k,\omega )=\frac{1}{\pi }\frac{W(k,\omega )}{(\omega \frac{k^2}{2m}V(k,\omega ))^2+W(k,\omega )^2}$$
(2)
where $`𝒢(k,\omega )`$ is the single–particle Green’s function:

$$𝒢(k,\omega )=\frac{1}{\omega \frac{k^2}{2m}V(k,\omega )\mathrm{i}W(k,\omega )}$$
(3)
The real and imaginary parts of the self-energy, $`V(k,\omega )`$ and $`W(k,\omega )`$, are highly off-shell in the considered energy and momentum ranges. In nuclear matter, according to the BBG expansion, the whole set of two-hole line contributions is summed up by the diagrams depicted in Fig. 13 , where the wavy lines indicate the Brueckner G-matrix. Since it is known that correlations with higher number of holes give a much smaller contribution to the ground state energy , it is reasonable to assume that their effect on the spectral function is also of minor relevance, producing mainly an additional background. The first diagram $`(1.a)`$ corresponds to the standard Brueckner approximation for the nucleon self-energy, and has the following expression

$$M_1(k,\omega )=\underset{k^{}<k_F}{}kk^{}|G(e(k^{})+\omega )|kk^{}_a$$
(4)
where $`e(k)`$ is the self-consistent single particle energy and the label $`a`$ means antisymmetrization. In the energy range relevant to the hole strength function and for $`k>k_F`$, this diagram contributes only to the real part $`V(k,\omega )`$ of the self-energy. Indeed, the imaginary part of $`M_1(k,\omega )`$ comes only from on-shell transitions from one-particle states ($`k>k_F`$) to two-particle one-hole states and this process is not allowed by momentum conservation. The diagram $`(1.b)`$ takes into account transitions to one-particle two-hole states. It contributes to both real and imaginary parts in the considered energy and momentum range. Explicitely, the imaginary part $`W(k,\omega )`$ is given by

$`W(k,\omega )=\frac{1}{2}{\displaystyle \underset{hh^{}p}{}}\mathrm{Im}{\displaystyle \frac{|kp|G\left(e(h)+e(h^{})\right)|hh^{}_a|^2}{Ee(p)+e(h)+e(h^{})\mathrm{i}\eta }}=`$
$`\frac{\pi }{2}_{hh^{}p}|kp|G\left(e(h)+e(h^{})\right)|hh^{}_a|^2\delta (\omega +e(p)e(h)e(h^{}))`$ (5)
where the sum is restricted to states $`h`$ and $`h^{}`$ with a momentum smaller than $`k_F`$ and $`p`$ with momentum larger than $`k_F`$.

Once the Brueckner calculation for nuclear matter is performed, the G-matrix and the corresponding self-consistent single particle spectrum are obtained. The G-matrix is then calculated off-shell for the entry energies needed in Eqs. (4,5), which provide the real and imaginary parts of the self-energy. Finally, the spectral function is calculated from Eq. (2).

Equation (5) is similar to the formula used in ref. . The main difference is the inclusion in the latter of the single particle strength functions in the phase space integral, which implies a self-consistent calculation. Furthermore, in that work the square of the in-medium scattering matrix is approximated by a constant average value, which simplifies the calculation considerably. The average scattering matrix is then adjusted in order to reproduce at best the results of ref. .

Equation (5) looks also similar to the formula for perturbative corrections introduced in ref.  within the variational scheme. In this case, the g-matrix is replaced by the residual interaction between hole states and two-hole one-particle states. The perturbative corrections are essential near the Fermi energy since they allow the hole states to acquire a width. However, in the high energy region, where we are focusing the analysis, their contribution is only marginal. In the variational scheme the main contribution comes from the two-hole one-particle orhtogonal correlated intermediate states, which cannot be cast in a formula like Equation (5). Therefore a formal comparison between the BBG and variational approach would be misleading.

As a consequence the numerical comparison among these many-body theories appears necessary.

## 3 Results

We performed calculations of the nuclear matter spectral function with three different two-body potentials, the Urbana v14 , the Argonne v14  and the Argonne v18 . Three-body forces were added, according to the Urbana IX model , and adjusted to reproduce the correct saturation point. We checked that the effect of the three-body force on the spectral function is negligeable. The Urbana potential was used only to compare with the results of ref.  and ref. .

In Figs. 2-a and 2-b we show the spectral function calculated at two values of the momentum, $`k=2.25`$ fm-1 and $`k=3.5`$ fm-1. The three lines indicate our BBG calculations with different potentials as described in the figure, while the full circles label the results of ref. , where the Urbana v14 was used. For both momenta the dependence on the nucleon-nucleon potential appears quite weak, only in some cases a discrepancy is present, which however does not exceed 20%. Larger deviations in the high energy region occur between the BBG results and those of ref. . We can conclude that these discrepancies in the high energy region are due to the many-body treatment and not to the interaction employed.

In Figs. 3-a and 3-b we compare our results (for the Urbana v14 potential) to the fully self consistent calculation of Lehr et al. . In this case the comparison can be more transparent. In fact, the first order calculations of ref. , indicated by the dotted lines in the figures, are exactly equivalent to our calculations if the G-matrix in Eq. (5) is replaced by a constant average value independent of momenta, directly related to in-medium nucleon-nucleon cross section . The discrepancy with the BBG calculations is, in this case, only due to this approximation, i.e. to the neglect of the G-matrix momentum dependence. This shows the relevance of the momentum dependent correlations for the determination of the single particle spectral function. The fact that the introduction of the self-consistency moves the high energy tail towards the BBG behaviour appears misleading, since in the BBG calculations no self-consistency has been used. This observation seems equally well applicable to the comparison with the variational calculations , where also no self-consistency procedure is included in the many-body scheme.

Of course these conclusions do not imply that the self-consistent procedure is not relevant, but only that it must be carried out with the full momentum dependence of the G-matrix.


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# Searching for Clusters of Galaxies with SUMSS

## 1. Introduction

Large numbers of distant ($`z>0.3`$) clusters are now being identified by the new generation of X-ray telescopes, such as Chandra and XMM-Newton (Allen et al. 2001; Fabian et al. 2001). This will allow the study of the evolution of gas and galaxies within massive dark-matter halos. However, because of the $`n^2`$ dependence of thermal bremsstrahlung, X-ray selection of clusters is inevitably biased towards relaxed systems. Other cluster selection techniques, which can also reach high redshifts, are needed to complement the X-ray work.

A different approach to cluster selection is to look for overdensities of radio sources. Such overdensities are known to be signposts for high-redshift clusters of galaxies containing several radio-loud AGN. These clusters will form a very different sample to that of the high-redshift X-ray clusters; plausibly it will be biased towards merging systems if, for example, AGN activity is triggered by mergers.

This search technique has been carried out on the NRAO VLA Sky Survey (NVSS) with a high success rate. Optical observations indicate that approximately $`65\%`$ of the overdensities of radio sources are indeed clusters of galaxies (Croft & Rawlings, private communication). Many $`z>0.3`$ clusters have been found; TOC J0233.3+3021, which has optical and infrared magnitudes implying $`z1`$, was mapped by the Ryle Telescope at Cambridge and was found to have a detectable Sunyaev-Zel’ dovich effect (Cotter et al. 2001).

## 2. Continuing the search in the Southern Hemisphere

The Sydney University Molonglo Sky Survey (SUMSS) is comparable to the NVSS survey. It has a resolution of 43 arcseconds at 843 MHz and identifies sources down to a level of 5 mJy. It follows that overdensities in this survey will also be signposts to clusters of galaxies.

We searched the SUMSS catalogue (Mauch, private communication) for overdensities of 5 or more radio sources inside a 7-arcminute radius. To weed out nearby clusters, we examine the SuperCOSMOS $`R`$-band data (Hambly et al. 2001). About $`5\%`$ of the radio source overdensities prove to be Abell clusters, and another $`35\%`$ have one or more optical identifications to the SuperCOSMOS limit of $`R=21.5`$. The remaining overdensities are robust candidate $`z>0.3`$ galaxy clusters. Sixty such candidates have been found to date; two are shown in Figure 1.

We will now embark on a detailed follow-up program that includes higher-resolution radio imaging at the ATCA, deeper imaging at the MSSSO 2.3-m and wide-field NIR imaging at the AAT. When we have assembled a sample of spectroscopically-confirmed clusters (using 8-m class telescopes for the most distant clusters), comparisons will be drawn between high-redshift X-ray- and radio source-selected samples. This will allow examination, for example, of the hypothesis that merging triggers multiple AGN activity in clusters.

### Acknowledgments.

HJB acknowledges a PPARC PhD studentship. GC acknowledges a PPARC Postdoctoral Research Fellowship.

## References

Allen, S. W. et al. 2001, MNRAS, 324, 842A

Fabian, A. C. et al. 2001, MNRAS, 322L, 11F

Cotter, G. et al. 2001, MNRAS in press, astro-ph/0109506

Hambly, N. C. et al. 2001, MNRAS, 326, 1279H


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# Spin Alignment of Heavy Meson Revisited

## Abstract

Using heavy quark effective theory a factorized form for inclusive production rate of a heavy meson can be obtained, in which the nonperturbative effect related to the heavy meson can be characterized by matrix elements defined in the heavy quark effective theory. Using this factorization, predictions for the full spin density matrix of a spin-1 and spin-2 meson can be obtained and they are characterized only by one coefficient representing the nonperturbative effect. Predictions for spin-1 heavy meson are compared with experiment performed at $`e^+e^{}`$ colliders in the energy range from $`\sqrt{s}=10.5`$GeV to $`\sqrt{s}=91`$GeV, a complete agreement is found for $`D^{}`$\- and $`B^{}`$-meson. There are distinct differences from the existing approach and they are discussed.

Heavy quark effective theory(HQET) is a powerful tool to study properties of heavy hadrons which contain one heavy quark $`Q`$. With HQET it allows such a study starting directly from QCD. HQET is widely used in studied of decays of heavy hadrons. In comparison, only in a few works it is used to study productions of heavy hadrons. In 1994 Falk and Peskin used HQET to predict spin alignment of a heavy hadron in its inclusive production. In this talk we will reexamine the subject and restrict ourself to the case of spin-1 meson.

A spin-1 heavy meson $`H^{}`$ is a bound state of a heavy quark $`Q`$ and a system of light degrees of freedom in QCD, like gluons and light quarks. In the work the total angular momentum $`j`$ of the light system is taken as $`1/2`$. In the heavy quark limit, the orbital angular momentum of $`Q`$ can be neglected and only the spin of $`Q`$ contributes to the total spin of $`H^{}`$. Once the heavy quark $`Q`$ is produced, it will combine the light system into $`H^{}`$. Because parity is conserved in QCD, the probabilities for the light system with positive- and negative helicity is the same. Therefore, one can predict the probabilities for production of $`H^{}`$ with a left-handed heavy quark $`Q`$ as:

$$P(\overline{B}^{}(\lambda =1)):P(\overline{B}^{}(\lambda =0)):P(\overline{B}^{}(\lambda =1))=\frac{1}{2}:\frac{1}{4}:0,$$
(1)
where $`\lambda `$ is the helicity of $`H^{}`$. These results are easily derived, however, three questions or comments can be made to them:

(a). In general the spin information is contained in a spin density matrix, probabilities are the diagonal part of the matrix. The question is how about the non-diagonal part. It should be noted that this part is also measured in experiment.

(b). It is possible that the light system can have the total angular momentum $`j=3/2`$ to form $`H^{}`$. One may argue that the production of such a system is suppressed. Is it possible to derive full spin density matrix without the assumption of $`j=1/2`$?

(c). How can we systematically add corrections to the approximation which lead to the results in Eq.(1)?

To make responses to these questions let us look at a inclusive production of $`H^{}`$ in detail. In its inclusive production a heavy meson is formed with a heavy quark $`Q`$ and with other light degrees of freedom, the light degrees can be a system of light quarks and gluons. Because its large mass $`m_Q`$ the heavy quark is produced by interactions at short distance. Therefore the production can be studied with perturbative QCD. The heavy quark, once produced, will combine light degrees of freedom to form a hadron, the formation is a long-distance process, in which momentum transfers are small, hence the formed hadron will carry the most momentum of the heavy quark. The above discussion implies the production rate can be factorized, in which the perturbative part is for the production of a heavy quark, while the nonperturbative part is for the formation. For the nonperturbative part an expansion in the inverse of $`m_Q`$ can systematically be performed in the framework of HQET. This type of the factorization was firstly used in parton fragmentation into a heavy hadron.

In this talk we will not discuss the factorization in detail, the details can be found in the work. We directly give our results and make a comparison with experiment. It should be noted that the factorization can be performed for any inclusive production of $`H^{}`$. Because the most experiments to measure spin alignment are performed at $`e^+e^{}`$-colliders, we present the results for the inclusive production at $`e^+e^{}`$-colliders. We consider the process

$$e^+(𝐩)+e^{}(𝐩)H^{}(𝐤)+X,$$
(2)
where the three momenta are given in the brackets. In the process we assume that the initial beams are unpolarized. We denote the helicity of $`H^{}`$ as $`\lambda `$ and $`\lambda =1,0,1`$. All information about the polarization of $`H^{}`$ is contained in a spin density matrix, which may be unnormalized or normalized, we will call them unnormalized or normalized spin density matrix, respectively. The unnormalized spin density matrix can be defined as

$$R(\lambda ,\lambda ^{},𝐩,𝐤)=\underset{X}{}H^{}(\lambda )X|𝒯|e^+e^{}H^{}(\lambda ^{})X|𝒯|e^+e^{}^{},$$
(3)
where the conservation of the total energy-momentum and the spin average of the initial state is implied. $`𝒯`$ is the transition operator. The cross-section with a given helicity $`\lambda `$ is given by:

$$\sigma (\lambda )=\frac{1}{2s}\frac{d^3k}{(2\pi )^3}R(\lambda ,\lambda ,𝐩,𝐤).$$
(4)
From Eq.(3) the normalized spin density matrix is defined by

$$\rho _{\lambda \lambda ^{}}(𝐩,𝐤)=\frac{R(\lambda ,\lambda ^{},𝐩,𝐤)}{_\lambda R(\lambda ,\lambda ,𝐩,𝐤)}.$$
(5)
It should be noted that the normalized spin density matrix is measured in experiment. It is straightforward to perform the mentioned factorization for the unnormalized spin density matrix in the rest frame of $`H^{}`$, which is related to the moving frame only by a Lorentz boost. In the rest frame we can define a creation operator for $`H^{}`$:

$$|H^{}(\lambda )=a^{}(\lambda )|0=\mathit{ϵ}(\lambda )𝐚^{}|0.$$
(6)
where $`\mathit{ϵ}(\lambda )`$ is the polarization vector. In the rest frame the field $`h_v`$ of the heavy quark $`Q`$ in HQET has two non-zero components. We denote them as:

$$h_v(x)=\left(\begin{array}{c}\psi (x)\\ 0\end{array}\right).$$
(7)
With these notations we define two operators:

$$O(H^{})=\frac{1}{6}\mathrm{Tr}\psi a_i^{}a_i\psi ^{},O_s(H^{})=\frac{i}{12}\mathrm{Tr}\sigma _i\psi a_j^{}a_k\psi ^{}\epsilon _{ijk},$$
(8)
where $`\epsilon _{ijk}`$ is the totally antisymmetric tensor and $`\sigma _i(i=1,2,3)`$ is the Pauli matrix. The results for the unnormalized spin density matrix read:

$`R(\lambda ,\lambda ^{},𝐩,𝐤)`$ $`=`$ $`{\displaystyle \frac{1}{3}}a(𝐩,𝐤)0|O(H^{})|0\mathit{ϵ}^{}(\lambda )\mathit{ϵ}(\lambda ^{})`$ (9)
$`+`$ $`{\displaystyle \frac{i}{3}}𝐛(𝐩,𝐤)[\mathit{ϵ}^{}(\lambda )\times \mathit{ϵ}(\lambda ^{})]0|O_s(H^{})|0+𝒪(m_Q^2).`$ (10)
The quantities $`a(𝐩,𝐤)`$ and $`𝐛(𝐩,𝐤)`$ characterize the spin density matrix of the heavy quark $`Q`$ produced in the inclusive process:

$$e^+(𝐩)+e^{}(𝐩)Q(𝐤,𝐬)+X$$
(11)
where $`𝐬`$ is the spin vector of $`Q`$ in its rest frame and the rest frame is related to the moving frame only by a Lorentz boost. The unnormalized spin density matrix $`R_Q(𝐬,𝐩,𝐤)`$ of $`Q`$ can be defined by replacing $`H^{}(\lambda )`$ with $`Q(𝐤,𝐬)`$ in Eq.(3). This matrix can be calculated with perturbative theory because of the heavy mass. The result in general takes the form

$$R_Q(𝐬,𝐩,𝐤)=a(𝐩,𝐤)+𝐛(𝐩,𝐤)𝐬$$
(12)
where $`a(𝐩,𝐤)`$ and $`𝐛(𝐩,𝐤)`$ are the same in Eq.(9). The physical interpretation for Eq.(9) is the following: The coefficients $`a(𝐩,𝐤)`$ and $`𝐛(𝐩,𝐤)`$ characterize the production of $`Q`$ and they can be calculated with perturbative QCD, while the two matrix elements defined in HQET characterize the nonperturbative effects of the formation of $`H^{}`$ with the heavy quark $`Q`$. With Eq.(9) we obtain:

$$\rho (𝐩,𝐤)=\frac{1}{3}\left(\begin{array}{ccc}1+P_3,& P_+,& 0\\ P_{},& 1,& P_+\\ 0,& P_{},& 1P_3\end{array}\right),$$
(13)
with

$$P_3=\frac{b_3(𝐩,𝐤)}{a(𝐩,𝐤)}\frac{0|O_s(H^{})|0}{0|O(H^{})|0},P_\pm =\frac{b_1(𝐩,𝐤)\pm ib_2(𝐩,𝐤)}{\sqrt{2}a(𝐩,𝐤)}\frac{0|O_s(H^{})|0}{0|O(H^{})|0},$$
(14)
The indices of the matrix in Eq.(12) run from -1 to 1. Without knowing the coefficients and the matrix elements we can already predict that $`\rho _{00}=1/3`$ and $`\rho _{11}=\rho _{11}=0`$.

With these results we are in position to compare with experiment. The experiments to measure the polarization of $`B^{}`$ are performed at LEP with $`\sqrt{s}=M_Z`$ by different experiments groups. To measure the polarization the dominant decay $`B^{}\gamma B`$ is used, where the polarization of the photon is not observed. Because the parity is conserved and the distribution of the angle between the moving directions of $`\gamma `$ and of $`B^{}`$ is measured, one can only determine the matrix element $`\rho _{00}`$. If we denote $`\theta `$ is the angle between the moving directions of $`B^{}`$ and of $`\gamma `$ in the $`B^{}`$-rest frame and $`\varphi `$ is the azimuthal angle of $`\gamma `$, then the angular distribution is given by $`W_{B^{}B\gamma }(\theta ,\varphi )_{\lambda \lambda ^{}}\rho _{\lambda \lambda ^{}}(\delta _{\lambda \lambda ^{}}Y_{1\lambda }(\theta ,\varphi )Y_{1\lambda ^{}}^{}(\theta ,\varphi ))`$. Integrating over $`\varphi `$ and using our result $`\rho _{00}=1/3`$, the distribution of $`\theta `$ is isotropic. In experiment one indeed finds that the distribution is isotropic in $`\theta `$. The experimental results at $`\sqrt{s}=M_Z`$ are:

$`\rho _{00}`$ $`=`$ $`0.32\pm 0.04\pm 0.03,\mathrm{DELPHI}`$ (15)
$`\rho _{00}`$ $`=`$ $`0.33\pm 0.06\pm 0.05,\mathrm{ALEPH},`$ (16)
$`\rho _{00}`$ $`=`$ $`0.36\pm 0.06\pm 0.07,\mathrm{OPAL}.`$ (17)
These results agree well with our prediction $`\rho _{00}=1/3`$.

The polarization measurement for $`D^{}`$-meson has been done with different $`\sqrt{s}`$, in some experiments the non-diagonal part of the spin density matrix has also been measured by measuring azimuthal angular distribution in $`D^{}`$ decay, where the decay mode into two pseudo-scalars, i.e., $`D^{}D\pi `$, is used. Denoting $`\theta `$ as the angle between the moving directions of $`D^{}`$ and of $`\pi `$ in the $`D^{}`$-rest frame and $`\varphi `$ as the azimuthal angle of $`\pi `$, then the angular distribution of $`\pi `$ is given by $`W_{D^{}D\pi }(\theta ,\varphi )_{\lambda \lambda ^{}}\rho _{\lambda \lambda ^{}}Y_{1\lambda }(\theta ,\varphi )Y_{1\lambda ^{}}^{}(\theta ,\varphi )`$. Integrating over $`\varphi `$ and using our result $`\rho _{00}=1/3`$, the distribution of $`\theta `$ is again isotropic. The experimental results are summarized in Table 1 and also partly summarized in .

From Table 1. we can see that the $`\rho _{00}`$ measured by all experimental groups is close to the prediction $`\rho _{00}=\frac{1}{3}`$, the most precise result is obtained by CLEO, its deviation from the prediction is $`2\%`$, the largest deviation of the prediction is from the result made by OPAL at $`\sqrt{s}=90`$GeV, it is $`20\%`$. In general, $`\rho _{00}`$ depends on the energy of $`H^{}`$. Our results in Eq.(17) give that $`\rho _{00}`$ is a constant in the heavy quark limit, or the energy dependence is suppressed by $`m_Q^2`$. In experiment only a very weak energy dependence is observed, e.g., in CLEO results. From our results $`\rho _{11}`$ is exactly zero in the heavy quark limit, the results from TPC and from HRS are in consistent with our result, a non zero value is obtained by OPAL, which has a $`3\sigma `$ deviation from zero. These deviations may be explained with effects of higher orders in $`m_c^1`$, these effects are expected to be substantial, because $`m_c`$ is not so large. It is interesting to note only results from OPAL at $`\sqrt{s}=91`$GeV have the largest deviations from our predictions, while results from other groups agree well with our predictions. At $`\sqrt{s}=10.5\mathrm{GeV}\mathrm{or}29`$GeV, the effect of the $`Z`$-boson exchange can be neglected, hence the parity is conserved. We obtain $`\rho _{10}=0`$. This prediction is also in agreement with the experimental result made by TPC and by HRS.

Table 1. Experimental Results for $`D^{}`$

| Collaboration | $`\sqrt{s}`$ in GeV | Results |
| --- | --- | --- |
| CLEO | 10.5 | $`\rho _{00}=0.327\pm 0.006`$ |
| HRS | 29 | $`\rho _{00}=0.371\pm 0.016`$ |
|  |  | $`\rho _{11}=0.04\pm 0.03`$ |
|  |  | $`\rho _{10}=0.00\pm 0.01`$ |
| TPC | 29 | $`\rho _{00}=0.301\pm 0.042\pm 0.007`$ |
|  |  | $`\rho _{11}=0.01\pm 0.03\pm 0.00`$ |
|  |  | $`\rho _{10}=0.03\pm 0.03\pm 0.00`$ |
| SLD | 91 | $`\rho _{00}=0.34\pm 0.08\pm 0.13`$ |
| OPAL | 91 | $`\rho _{00}=0.40\pm 0.02\pm 0.01`$ |
|  |  | $`\rho _{11}=0.039\pm 0.014`$ |

Since our results are derived without knowing the total angular momentum $`j`$ of the light degrees of freedom in the heavy meson, the agreement of our results with experiment can not be used to extract the information about $`j`$ from the experimental data in Eq.(19) and in Table 1., although $`\rho _{00}=1/3`$ can also be obtained by taking $`j=1/2`$. One way to extract $`j`$ may be to measure the difference between $`\rho _{11}\rho _{11}`$, but it seems not possible, because the polarization of $`H^{}`$ is measured through its parity-conserved decay and the polarization of decay products is not observed in experiment. In the heavy quark limit, the nondiagonal element $`\rho _{11}`$ and $`\rho _{11}`$ are zero, while the other nondiagonal matrix elements are nonzero if the parity is not conserved and the initial state is unpolarized. At higher orders in $`m_Q^1`$ this can be changed, e.g., $`H^{}`$ can have tensor polarization.

The factorization can also be done for inclusive productions of a spin-2 meson. The results can be found in the work. Experimentally only the spin alignment of $`D_2^{}(2460)`$ is measured with large errors. But the experimental results seem to be not in agreement with the predictions. The reason can be the large effect from corrections at higher orders of $`m_c^1`$.

To summarize: Using the approach of QCD factorization and employing HQET, we obtain predictions of full spin density matrices of spin-1- and spin-2 heavy meson. The leading order predictions for a spin-1 meson agree well with experiment. Within the approach the three questions asked before are answered. Although we have given in this talk detailed predictions for inclusive production of a spin-1 heavy meson at an $`e^+e^{}`$ collider, our approach can be easily generalized to other inclusive productions, testable predictions can be made without a detailed calculation, for example, in inclusive production of $`B^{}`$ at an electron-hadron- or a hadron-hadron collider we always have the prediction $`\rho _{00}=1/3`$ and $`\rho _{11}=\rho _{11}=0`$ in the heavy quark limit.


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# Single-electron control of Wigner crystallization

## Abstract

Wigner crystallization in mesoscopic quantum dots containing only few ($`N<50`$) electrons exhibits a number of interesting peculiarities: (i) there exist two distinct crystal phases, and (ii) the phase boundary sensitively depends on the precise particle number. In this paper we demonstrate that this behavior can be used to control the collective transport properties by adding or removing a single electron.

,

One of the most exciting properties of mesoscopic systems is the dependence of their properties on the particle number. Besides the familiar electron addition spectra in quantum dots, e.g. ashoori96 , recently, another example has been found, cf. bedanov ; afilinov-etal.01prl  and references therein: Wigner crystallization in mesoscopic electron clusters in two-dimensional quantum dots. Simulations of a small number of electrons confined in a spherically symmetric harmonic trap and interacting via the Coulomb potential afilinov-etal.01prl ; afilinov-etal.00pss  revealed that the location of the phase boundary of the Wigner crystal in the density-temperature plane sensitively depends on the precise particle number. In this paper we discuss principle possibilities of taking advantage of this behavior for applications.

The particle number sensitivity originates from the configuration symmetry of the cluster ground state. Minimization of the total energy computed from the hamiltonian

$`\widehat{H}={\displaystyle \underset{i=1}{\overset{N}{}}}{\displaystyle \frac{\mathrm{}^2_i^2}{2m_i^{}}}+{\displaystyle \underset{i=1}{\overset{N}{}}}{\displaystyle \frac{m_i^{}\omega _0^2r_i^2}{2}}+{\displaystyle \underset{i<j}{\overset{N}{}}}{\displaystyle \frac{e^2}{ϵ_b|𝐫_i𝐫_j|}},`$ (1)
($`m^{}`$ and $`ϵ_b`$ are the effective electron mass and background dielectric constant, respectively), yields a spherical shell structure details of which vary strongly with the particle number, see Fig. 1. “Magic” clusters (those with an integer ratio of particle numbers on the outer and inner shell - e.g. $`N=19`$) show a clear hexagonal crystal structure (Fig. 1, left part). In contrast, non-magic ones (e.g. $`N=20`$) are dominated by the spherical trap symmetry. This has a strong effect on the stability of the crystal phases, see Fig. 1, right part.

Generally, crystal-like behavior wc  is found below a critical temperature (of the order of a few $`K`$ in semiconductor quantum dots) in a finite density interval, see Fig. 1. If the density is reduced below a critical value $`n_1(T,N)`$, the system undergoes a transition to a state resembling a classical liquid. Similarly, above a second critical density $`n_2(T,N)`$ (with $`n_2n_1`$) a Fermi liquid-like state (in mesoscopic systems, sometimes referred to as Wigner molecule) is reached. While this general behavior is analogous to macroscopic systems, e.g. tanatar89 , crystallization in few-electron systems shows a number of interesting peculiarities spin : (i) strong $`N`$ dependence of the phase boundary and (ii), the existence of a second phase boundary which is embedded into the first one where the crystal structure is transformed from a completely ordered (“OO”, fully localized electrons) state into a partially (“RO”, radially) ordered one where electrons are rigidly confined to crystal shells which, as a whole, can rotate against each other. The phase boundary is determined by critical values of the coupling parameters: the low-density boundary by the classical parameter, $`\mathrm{\Gamma }e^2/(ϵ_br_0k_BT)`$, and the high-density limit by $`r_sr_0/a_B`$, cf. Fig. 1. Here, $`a_B`$ is the effective Bohr radius, $`a_B=\mathrm{}^2ϵ_b/(me^2)`$, and $`r_0`$ is the mean interparticle distance, approximately given by the balance of the repulsive Coulomb force and the radial confinement force of the harmonic potential with strength $`\omega _0`$: $`e^2/(ϵ_br_0^2)=m\omega _0^2r_0`$. A particularly strong N dependence is observed for the “OO” phase: “magic” clusters ($`N=12,19`$ etc.) are found to be much more stable than clusters having one electron more or less bedanov ; afilinov-etal.01prl . For example, the orientational melting parameters $`\mathrm{\Gamma }^{OM}`$ and $`r_s^{OM}`$ of the cluster with $`N=19`$ are 9 orders of magnitude lower than those for $`N=20`$, see Fig. 1.

This behavior can be exploited for a non-traditional control of crystallization. In addition to changing temperature or/and density (confinement strength), crystallization in mesoscopic systems can be achieved by variation of the particle number without change of $`T`$ and $`n`$. For example, choosing a point in the temperature-density plane, Fig. 1, which is located between the radial (orientational) melting curves of $`N=19`$ and $`N=20`$ and switching between the two particle numbers is equivalent to a crossover between crystal-like and liquid-like (OO and RO crystal) behavior. We will demonstrate this below for the orientational melting curves in the classical part of the phase diagram, i.e. we fix the classical coupling parameter $`\mathrm{\Gamma }`$ between $`\mathrm{\Gamma }_{20}^{OM}`$ and $`\mathrm{\Gamma }_{19}^{OM}`$, (see Fig. 1, right part).

The main difference between the orientationally ordered (with $`N=19`$) and disordered ($`N=20`$) state will be that the latter is able to support inter-shell rotational excitations. This should give rise to macroscopic currents and magnetic fields. To estimate this effect, we compute the total angular current created by N electrons confined to one of M shells of radius $`R_k`$ rotating with angular frequency $`\omega _k`$ (positive or negative depending on the direction), $`I_\varphi =e_{k=1}^MN_k\omega _kR_k`$. The associated magnetic field on the symmetry axis in a distance $`z`$ above the cluster plane is directed normal to the plane: $`B_z(z,t)=\frac{\mu e}{2}_{k=1}^MN_k\omega _k(t)\left[1+\left(z/R_k\right)^2\right]^{3/2}`$ For example, for $`N=20`$, we have $`N_1=7`$, $`N_2=12`$, $`R_22R_12r_0`$, so that $`I_\varphi ^{20}er_0(7\omega _1+24\omega _2)`$. The relation between $`\omega _1`$ and $`\omega _2`$ depends on the excitation conditions. For example, if the total angular momentum of the excitation is zero, one readily finds $`\omega _1/\omega _24N_2/N_1`$, i.e. the inner shell rotates approximately 7 times faster. Alternatively, rotation of some shells may be inhibited due to defects (pinning). For definiteness, in the following we consider the cluster $`N=20`$ with the outer shell pinned.

At a given coupling $`\mathrm{\Gamma }`$ and confinement energy $`m\omega _0r_0^2/2`$, thermal fluctuations spontaneously excite rotational and vibrational degrees of freedom both, in radial and angular direction. The thermal energy per particle is $`k_BT`$ and is $`\mathrm{\Gamma }`$ times smaller than the confinement energy. As our simulations show (see below), approximately half of it is converted into angular kinetic energy (rotations and oscillations), i.e. $`E_{rot}\frac{1}{4}m\omega _0^2R_1^2/\mathrm{\Gamma }`$. Depending on the excitation conditions, this gives rise to rotations of the inner shell electrons with $`\omega _{1max}\omega _0/\sqrt{2\mathrm{\Gamma }}`$. Inserting this result into the expression for $`B_z`$ and averaging over the fast vibrations, we obtain $`B_z(z)_{max}{\displaystyle \frac{\mu e^2}{2ϵ_br_0}}{\displaystyle \frac{N_1}{\sqrt{mr_0\mathrm{\Gamma }}}}\left[1+\left(z/r_0\right)^2\right]^{3/2}.`$ Interestingly, the current and the magnetic field increase as the square root of temperature. In contrast, the cluster of 19 electrons does not support intershell rotations. Here, the excitation energy is completely converted into vibrations.

We have verified this concept by performing classical molecular dynamics simulations for $`N=19`$ and $`N=20`$ in a wide range of $`\mathrm{\Gamma }`$ values vova01 ; anim . As expected, the cluster with $`N=19`$ (pinned to suppress the trivial rotation of the whole system) supports, at $`\mathrm{\Gamma }=500>\mathrm{\Gamma }_{19}^{OM}`$, no intershell rotations, and only vibrations are excited, even for purely rotational initial fluctuations anim . In contrast, for $`N=20`$, strong collective rotational motion of the inner shell electrons is excited, see Fig. 2. In all cases, we found that, in the spectrum, the vibrational excitations are well separated from the rotations – the former occur at significantly higher frequency, dominantly at frequency $`\omega _0`$ (and $`\omega _0/4`$). After averaging over $`4T_0`$, with $`T_0=2\pi /\omega _0`$, a “persistent” collective current $`j_{in}`$ of the inner shell is observed which exceeds the averaged fluctuating signal $`j_{out}`$ of the pinned outer shell by at least two orders of magnitude. The direction of the shell rotation and its slow time-dependence of $`j_{in}`$ are determined by the (random) excitation conditions and is not relevant. As an independent test we computed the potential barriers for intershell rotation using Quantum Monte Carlo simulations afilinov-etal.01prl . These simulations effectively average over the random excitations and yield, for $`N=20`$ at $`\mathrm{\Gamma }=500`$, potential barriers which are practically zero.

For practical applications, one may think of designing a suitable external rotational excitation in such a way that it is sufficiently weak so it does not overcome the barrier of the $`N=19`$ cluster. If applied to the $`N=20`$ cluster, the same excitation will easily give rise to intershell rotations. Such an excitation could be e.g. a constant or pulsed circularly polarized electric field. Based on our simulations, we expect that the response of a (pinned) $`N=20`$ cluster will be a nearly dissipationless rotation of the inner shell which stops after removal of one electron anim . This allows for a completely new kind of single-electron controlled devices. Such collective rotations of a group of electrons can be easily transmitted, e.g. in a system of multiple layers afilinov-etal.01cpp  and may find applications for quantum computing. Naturally, realization of this concept will require very clean samples, and detection of the weak circular currents is another important issue to be solved. At the same time, high sensitivity of these few-electron clusters to very weak rotational excitations could be of interest for applications by itself.

M.B. acknowledges stimulating discussions with participants of NPMS-5, in particular, J. Barker on quantum computing and K. von Klitzing on experimental verification issues.

This work has been supported by the Deutsche Forschungsgemeinschaft (grant BO-1366/2) and by a grant for CPU time at the NIC Jülich.


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# Electron scattering on disordered double barrier GaAs-AlxGa1-xAs heterostructures

## I Introduction

Resonant tunneling (RT) through double-barrier structures (DBS) make these systems very promising candidates for a new generation of ultra-high speed electronic devices. For instance, a GaAs-Ga1-xAlxAs DBS operating at THz frequencies has been reported in the literature. The basic reason for RT to arise in DBS is a quantum phenomenon whose fundamental characteristics are by now well understood: There exists a dramatic increase of the electron transmission whenever the energy of the incident electron is close to one of the unoccupied quasi-bound-states inside the well. In practice, a bias voltage is applied to shift the energy of this quasi-bound-state of nonzero width so that its center matches the Fermi level. Consequently, the $`jV`$ characteristics present negative differential resistance when the quasi-bound-state lies well below the Fermi level.

In actual samples, however, the situation is much more complex than this simple picture. Scattering by phonons, electrons or defects reduces the required quantum coherence and, in fact, deviations from the above simple description are observed. These scattering mechanisms explain the occurrence of side-band resonant peaks due to the interaction with phonons and photons, hysteresis in the $`jV`$ characteristics due to many body effects, and the decrease of electron mobility due to rough surfaces even in good-quality heterostructures. While one-dimensional models successfully describe scattering by electrons and phonons, they obviously cannot account for all interface roughness effects. So far, there are analytical results concerning the propagation of wave packets in a randomly layered medium when the potential is a random function of only one coordinate, but for a small number of layers, as in DBS, in-plane disorder becomes important and one expects such approaches to fail. Realistic models of in-plane disorder, including power-like or exponential spatial correlations observed by transmission electron microscopy, usually lead to intractable analytical models; hence the importance of numerically solvable models to bridge this gap. An important contribution was already provided by Henrickson et al., who applied the tight-binding Green function method to interface roughness in DBS. In this paper transmission was studied for a DBS with a rather simple model of disorder (periodic roughness with random relative phases at the interfaces). A level splitting was found for narrow well DBS and a dependence on the roughness lateral size was observed.

In this work we present a simple two-dimensional model that allowed us to carry out an extensive study of electron scattering by interface roughness and how it manifests trough vertical transport properties of the DBS. In particular, we aim to elucidate the relationship between macroscopic properties of the DBS (e.g. conductance) with microscopic parameters of the model (e.g. correlation length of the surface disorder). The paper is organized as follows: The body of the paper is Sec. II, where we present our model based, on the effective-mass approximation, describing a disordered sample (e.g. an imperfect DBS) connected to two perfectly ohmic leads. The Ben Daniel-Duke equation is discretized, boundary conditions are discussed and scattering solutions are found by means of the transfer-matrix method for any arbitrary heterostructure made of wide gap semiconductors. Afterwards, expressions for two-terminal conductance and current for unintentionally disordered DBS are provided. The model is worked out in a two-dimensional space for computational limitations, although it will be clear that generalization to three dimensions is rather straightforward. Section III describes the various models of disorder we have used to mimic structural data obtained by transmission electron microscopy and X-ray scattering. In Sec. IV we present the numerical results and, in particular, the relationship between macroscopic properties of the DBS with microscopic parameters of the model. Finally, in Sec. V we discuss our results and the main conclusions of the work.

## II Model

### A Discrete equation

We consider the single-electron two-dimensional Schrödinger equation within the framework of the one-band effective-mass approximation. Close to the $`\mathrm{\Gamma }`$ valley, this approach leads to the Ben Daniel-Duke equation for the envelope function

$$\left[\frac{\mathrm{}^2}{2m^{}}\left(\frac{^2}{y^2}+\frac{^2}{z^2}\right)+U(y,z)\right]\psi (y,z)=E\psi (y,z).$$
(1)
where $`z`$ denotes the coordinate along the growth direction (see Fig. 1). Notice that we have taken a constant effective mass $`m^{}`$ at the $`\mathrm{\Gamma }`$ valley although this is not a serious limitation as the model can be easily generalized to include a position-dependent effective mass. We then consider a mesh with lattice spacings $`a_y`$ and $`a_z`$ in the $`y`$ and $`z`$ directions, respectively. Defining $`t_y\mathrm{}^2/(2m^{}a_y^2)`$ and $`t_z\mathrm{}^2/(2m^{}a_z^2)`$, we arrive at the following discretized version of Eq. (1)

$$t_z(\psi _{n+1,m}+\psi _{n1,m})+t_y(\psi _{n,m+1}+\psi _{n,m1})+(U_{n,m}2t_z2t_y)\psi _{n,m}=E\psi _{n,m}.$$
(2)
The potential term $`U_{n,m}`$ in Eq. (2) is given by the conduction-band edge energy at the point $`(na_y,ma_z)`$ which, in turn, depends on the Al mole fraction in the vicinity of that position. Consequently, both kinds of disorder (lateral and compositional) are taken into account through this diagonal term (diagonal disorder).

### B Transfer matrix formalism

In order to solve the tight binding-like equation (2) we use the transfer matrix method based on the solutions calculated for each slide of the system along the $`z`$ direction. To this end, we define

$$\varphi _n\left(\begin{array}{c}\psi _{n,1}\\ \psi _{n,2}\\ \mathrm{}\\ \psi _{n,M}\end{array}\right),n=0,1,\mathrm{},N+1,$$
(4)
and

$$_\mathrm{n}=\left(\begin{array}{ccccc}\mathrm{U}_{\mathrm{n},1}2\mathrm{t}_\mathrm{z}2\mathrm{t}_\mathrm{y}& \mathrm{t}_\mathrm{y}& 0& \mathrm{}& \mathrm{t}_\mathrm{y}\\ \mathrm{t}_\mathrm{y}& \mathrm{U}_{\mathrm{n},2}2\mathrm{t}_\mathrm{z}2\mathrm{t}_\mathrm{y}& \mathrm{t}_\mathrm{y}& \mathrm{}& 0\\ 0& \mathrm{t}_\mathrm{y}& \mathrm{U}_{\mathrm{n},3}2\mathrm{t}_\mathrm{z}2\mathrm{t}_\mathrm{y}& \mathrm{}& 0\\ \mathrm{}& \mathrm{}& \mathrm{}& \mathrm{}& \mathrm{}\\ \mathrm{t}_\mathrm{y}& 0& 0& \mathrm{}& \mathrm{U}_{\mathrm{n},\mathrm{M}}2\mathrm{t}_\mathrm{z}2\mathrm{t}_\mathrm{y}\end{array}\right).$$
(5)
Here $`M`$ and $`N+1`$ are the number of mesh divisions in the $`y`$ and $`z`$ directions, respectively. Note that periodic boundary conditions have been taken into account on each slide. With these definitions, Eq. (2) can be cast in a more compact form

$$\left(\begin{array}{c}\varphi _{n1}\\ \varphi _n\end{array}\right)=\left(\begin{array}{cc}t_z^1(E_\mathrm{n})& \\ & 𝒪\end{array}\right)\left(\begin{array}{c}\varphi _n\\ \varphi _{n+1}\end{array}\right)$$
(6)
where $``$ and $`𝒪`$ are the $`M\times M`$ identity and null matrices respectively. This expression allows us to relate by iteration the envelope function amplitudes at non-consecutive slides. In particular, we can obtain the expression of the envelope function amplitudes in the left contact as a function of the amplitudes in the right one

$$\left(\begin{array}{c}\varphi _0\\ \varphi _1\end{array}\right)=𝒯^{(N)}\left(\begin{array}{c}\varphi _N\\ \varphi _{N+1}\end{array}\right),$$
(8)
where

$$𝒯^{(N)}\underset{n=1}{\overset{N}{}}\left(\begin{array}{cc}t_z^1(E_\mathrm{n})& \\ & 𝒪\end{array}\right).$$
(9)
is the transfer matrix for the heterostructure.

### C Scattering solutions

We are interested in the scattering of electrons incident from the left contact. The envelope functions within the contacts will be determined by the boundary conditions. These boundary conditions are open in the $`z`$ direction, and periodic on each slide, that is in the $`y`$ direction. The former imply plane wave solutions in the $`z`$ axis, and the latter yield an energy discretization on $`y`$. As a consequence, this discretization results in a number of transverse channels equal to the number of points in the transverse mesh direction. Considering by the moment $`U_{n,m}=0`$ at the contacts and setting $`\psi _{n,1}=\psi _{n,M+1}`$, a particular solution of Eq. (2) is given by

$$\psi _{n,m}^l=\frac{1}{\sqrt{𝒩_l}}\mathrm{exp}\left(i\frac{2\pi l}{M}m\right)\mathrm{exp}\left(ik_la_zn\right),l=1,2,\mathrm{},M.$$
(10)
Here $`𝒩_l`$ is a normalization constant that is needed for the different propagating modes to carry the same current all of them. This normalization constant is given by

$$𝒩_l=\frac{1}{a_y^2}\mathrm{sin}^2\left(\frac{2\pi l}{M}\right)+\frac{1}{a_z^2}\mathrm{sin}^2\left(k_la_z\right)$$
(11)
Note that we consider a dependence on the index $`l`$ of the momentum in the $`z`$ direction. This is a consequence of the implicit assumption that all the scattering processes in region II are elastic, so energy is conserved. Thus, for a given energy

$$k_l=\frac{1}{a_z}\mathrm{cos}^1\left\{\frac{1}{2t_z}\left[E2t_y\left(\mathrm{cos}\frac{2\pi l}{M}1\right)\right]+1\right\}.$$
(12)
Finally we can write a general solution of the scattering problem for an electron of energy $`E`$ impinging on the scattering region on the $`l`$ transverse mode. On the left contact the solution will be of the form

$`\psi _{n,m}^l`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{𝒩_l}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi l}{M}}m\right)\mathrm{exp}\left(ik_la_zn\right)`$ (14)
$`+`$ $`{\displaystyle \underset{j=1}{\overset{M}{}}}\widehat{r}_{lj}{\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right)\mathrm{exp}\left(ik_ja_zn\right),(m,n)\mathrm{I}.`$ (15)
On the right contact we have

$$\psi _{n,m}^l=\underset{j=1}{\overset{M}{}}\widehat{t}_{lj}\frac{1}{\sqrt{𝒩_j}}\mathrm{exp}\left(i\frac{2\pi j}{M}m\right)\mathrm{exp}\left(ik_ja_zn\right),(m,n)\mathrm{III}.$$
(16)
The matrices $`\widehat{r}`$ and $`\widehat{t}`$ appearing in these two solutions are the reflection and transmission matrices and they are responsible for the channel mixing due to scattering events. Thus, $`\widehat{r}_{ij}`$ represents the probability amplitude for an electron impinging in channel $`i`$ to be reflected into the chanel $`j`$. Similarly $`\widehat{t}_{ij}`$ represents the probability amplitude for an electron impinging in chanel $`i`$ to be transmited through the scattering region II into the channel $`j`$. Note that the solution within region II is unknown. Actually, we are not interested in this solution since all the physics of the scattering problem is contained in the mixing matrices $`\widehat{t}`$ and $`\widehat{r}`$. In the following, our main goal will be to relate the elements of $`\widehat{t}`$ and $`\widehat{r}`$ to those of $`𝒯^{(N)}`$ in Eq. (8).

We start by re-writting formally Eq. (2) as $`\psi =E\psi `$. Now we perform the following transformation upon the envelope functions

$$\stackrel{~}{\psi }=\widehat{t}^1\psi .$$
(17)
It is easy to see that the Hamiltonian is invariant under such a transformation, that is, $`\stackrel{~}{}\widehat{t}^1\widehat{t}=`$. This is clear since $`\widehat{t}`$ and $``$ formally commute as they act upon different vector spaces. The fact that $``$ is invariant implies that $`𝒯^{(N)}`$ is not affected by transformation (17) so it remains unchanged. In addition, equations (14) and (16) are transformed into

$`\stackrel{~}{\psi }_{n,m}^l`$ $`=`$ $`{\displaystyle \underset{j=1}{\overset{M}{}}}\widehat{a}_{lj}{\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right)\mathrm{exp}\left(ik_ja_zn\right)`$ (19)
$`+`$ $`{\displaystyle \underset{j=1}{\overset{M}{}}}\widehat{b}_{lj}{\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right)\mathrm{exp}\left(ik_ja_zn\right),(m,n)\mathrm{I}`$ (20)
and

$$\stackrel{~}{\psi }_{n,m}^l=\frac{1}{\sqrt{𝒩_l}}\mathrm{exp}\left(i\frac{2\pi l}{M}m\right)\mathrm{exp}\left(ik_la_zn\right),(m,n)\mathrm{III},$$
(21)
respectively, where we have defined $`\widehat{b}_{lj}_{s=1}^M\widehat{t}_{ls}^1\widehat{r}_{sj}`$ and $`\widehat{a}_{lj}\widehat{t}_{lj}^1`$. For each channel $`l`$ we can write the transform of Eq. (8) as

$$\left(\begin{array}{c}\stackrel{~}{\varphi }_0^l\\ \stackrel{~}{\varphi }_1^l\end{array}\right)=𝒯^{(N)}\left(\begin{array}{c}\stackrel{~}{\varphi }_N^l\\ \stackrel{~}{\varphi }_{N+1}^l\end{array}\right).$$
(22)
Now, introducing the definitions

$`𝒜^0`$ $``$ $`A_{jm}^0={\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right),`$ (23)
$`^0`$ $``$ $`𝒜^0,`$ (24)
$`𝒜^1`$ $``$ $`A_{jm}^1={\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right)\mathrm{exp}\left(ik_ja_z\right),`$ (25)
$`^1`$ $``$ $`B_{jm}^1={\displaystyle \frac{1}{\sqrt{𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi j}{M}}m\right)\mathrm{exp}\left(ik_ja_z\right),`$ (26)
$`\widehat{a}^l`$ $`=`$ $`\left(\begin{array}{c}\widehat{a}_{l1}\\ \widehat{a}_{l2}\\ \mathrm{}\\ \widehat{a}_{lM}\end{array}\right),\widehat{b}^l=\left(\begin{array}{c}\widehat{b}_{l1}\\ \widehat{b}_{l2}\\ \mathrm{}\\ \widehat{b}_{lM}\end{array}\right),`$ (35)
we arrive at the following transform of Eq. (22) in terms of the elements of the mixing matrices

$$\left(\begin{array}{c}\stackrel{~}{\varphi }_0^l\\ \stackrel{~}{\varphi }_1^l\end{array}\right)=\left(\begin{array}{cc}𝒜^0& ^0\\ 𝒜^1& ^1\end{array}\right)\left(\begin{array}{c}\widehat{a}^l\\ \widehat{b}^l\end{array}\right)=𝒯^{(N)}\left(\begin{array}{c}\stackrel{~}{\varphi }_{N1}^l\\ \stackrel{~}{\varphi }_N^l\end{array}\right),$$
(36)
and, finally, we have

$$\left(\begin{array}{c}\widehat{a}^l\\ \widehat{b}^l\end{array}\right)=\left(\begin{array}{cc}𝒜^0& ^0\\ 𝒜^1& ^1\end{array}\right)^1𝒯^{(N)}\left(\begin{array}{c}\stackrel{~}{\varphi }_{N1}^l\\ \stackrel{~}{\varphi }_N^l\end{array}\right),$$
(37)
that give us the matrix elements $`\widehat{a}_{lj}`$ and $`\widehat{b}_{lj}`$ with $`j=1,2,\mathrm{},M`$ for each channel $`l`$ in terms of the product of two known matrices and the transformed solutions (21) at the right contact for the $`l`$ channel. It is worth noticing that all the scattering information is contained in the transfer matrix $`𝒯^{(N)}`$. Thus, this quantity turns out to be the fundamental object in the resolution of the scattering problem.

### D Conductance and current

Once $`\widehat{a}`$ and $`\widehat{b}`$ have been calculated, obtaining $`\widehat{t}`$ and $`\widehat{r}`$ is an easy task. However, the matrices calculated this way are the response matrices that contains some non-physical information. This non-physical information comes from the fact that we have been considering all the mathematical solutions of the scattering problem, including those diverging at infinity. These solutions are those for which momentum in Eq. (12) is an imaginary number. In order to avoid the unphysical solutions we will cancel out all the elements on $`\widehat{t}`$ for which the incoming and/or the outgoing transverse quantum number $`l`$ satisfy the following condition

$$E<2t_y\left(\mathrm{cos}\frac{2\pi l}{M}1\right).$$
(38)
Once the physical mixing matrices are known, particularly the transmission matrix $`\widehat{t}`$, we can use them to calculate different physical quantities like the conductance or the electric current. From the Landauer-Büttiker formalism, the zero temperature two-leads multichannel conductance can be calculated using de Fisher-Lee formula

$$G=\frac{2e^2}{h}\text{Tr}(\widehat{t}^{}\widehat{t}).$$
(39)
In order to calculate the electric current due to an applied field $`F`$ we have to modify slightly our equations and further approximations are needed. First of all, we consider perfect leads, so no voltage drop occurs within the contacts. Besides, we will not consider the contribution to the current of electrons impinging from the right contact. This is a good approximation provided $`eV>E_F`$, where $`V`$ is the voltage drop along the region I and $`E_F`$ is the electron Fermi level on the contacts. Finally, we will assume zero temperature so no carrier statistics will be taken into account.

When an electric field applied along the growth direction is considered, the potential $`U(y,z)`$ in Eq. (1) has to be replaced by $`U(y,z)+U_F(z)`$, where $`U_F`$ is constant in the contacts ($`U_F(z)=0`$ in region I and $`U_F(z)=eV`$ in region III) and behaves linearly in region II, namely $`U_F(z)=eFz`$. Here $`F`$ is the applied electric field and $`V=FL`$ is the voltage drop across the scattering region whose length is $`L`$. The electron momentum on the right contact now reads

$$q_l=\frac{1}{a_z}\mathrm{cos}^1\left\{\frac{1}{2t_z}\left[E+eV2t_y\left(\mathrm{cos}\frac{2\pi l}{M}1\right)\right]+1\right\},(m,n)\mathrm{III}$$
(40)
and solution in region III changes to

$$\psi _{n,m}^l=\underset{j=1}{\overset{M}{}}\widehat{t}_{lj}\frac{1}{\sqrt{𝒩_j}}\mathrm{exp}\left(i\frac{2\pi j}{M}m\right)\mathrm{exp}\left(iq_ja_zn\right).$$
(41)
Bearing in mind all the approximations considered so far, a new transfer matrix $`𝒯^{(N)}`$ can be calculated for a each value of $`F`$. Inserting solution (41) in Eq. (37) we can obtain the mixing matrices for a given applied field and then calculate using them the electric current induced by that field. From the expression for the probability current we can write the discretized version of the electronic current density contribution of chanel $`l`$ along the applied field direction across the right lead (calculated on a slide $`n`$ within the region III) as

$$j_z^l=i\frac{et_za_z}{\mathrm{}a_y}\frac{1}{M}\underset{m=1}{\overset{M}{}}\left[(\psi _{n,m}^l)^{}\psi _{n+1,m}^l\psi _{n,m}^l(\psi _{n+1,m}^l)^{}\right].$$
(42)
In order to calculate the total density current across the sample, we just need to sum up over all the allowed transverse states below the Fermi level at the left contact, that is

$$j_z=i\frac{et_za_z}{2\pi \mathrm{}a_y}\frac{1}{M}\underset{m=1}{\overset{M}{}}\underset{l=1}{\overset{M}{}}_0^{k_F^l}\left[(\psi _{n,m}^l)^{}\psi _{n+1,m}^l\psi _{n,m}^l(\psi _{n+1,m}^l)^{}\right]𝑑k.$$
(43)
Notice that the electron momentum in the $`z`$ direction, $`k`$, varies continously as the energy for an incident electron can take values from $`0`$ to $`E_F`$. Here, $`k_F^l`$ is the component of the electron momentum along the $`z`$ direction for an incident electron with transverse quantum number $`l`$ and an incident energy $`E_F`$. Using the transmission matrix elements we finally arrive at

$`j_z`$ $`=`$ $`i{\displaystyle \frac{et_za_z}{2\pi \mathrm{}a_y}}{\displaystyle \frac{1}{M}}{\displaystyle \underset{m=1}{\overset{M}{}}}{\displaystyle \underset{l=1}{\overset{M}{}}}{\displaystyle _0^{k_F^l}}{\displaystyle \underset{j=1}{\overset{M}{}}}{\displaystyle \underset{s=1}{\overset{M}{}}}\widehat{t}_{lj}^{}\widehat{t}_{ls}{\displaystyle \frac{1}{\sqrt{𝒩_s𝒩_j}}}\mathrm{exp}\left(i{\displaystyle \frac{2\pi (sj)}{M}}m\right)`$ (44)
$`\times `$ $`\mathrm{exp}\left[i(q_sq_j)a_zn\right]\left[\mathrm{exp}\left(iq_sa_z\right)\mathrm{exp}\left(iq_ja_z\right)\right]dk.`$ (45)
The results we have obtained so far provide an exact, although nonclosed, analytical description of any two-dimensional heterostructure based on wide-gap semiconductors, whenever the Ben Daniel-Duke holds valid. Let us stress that the generalization to three-dimensional heterostructures is fairly straightforward. With these results at hand, we can compute the transport magnitudes we mentioned above. All expressions are very simple and suitable for an efficient numerical treatment for any specific case. We will now evaluate them for unintentionally disordered DBS to describe the relevant features of the model.

## III Models of disorder

Unintentional disorder appearing during growth in actual heterostructures depends critically on the growth conditions. There exist several techniques, like scanning tunneling microscopy  and X-ray scattering,  which have been applied in recent years to quantitatively determine structural properties of multilayers and superlattices. Precise information about the nature and extend of defects at interfaces is now available. Following Mäder et al., disorder in a heterostructure can be classified into two categories, namely lateral and vertical. Lateral disorder occurs whenever one semiconductor protrudes into the other, forming chemically intermixed interfaces, steps and islands. As a consequence, the interface is not flat and translational symmetry in the plane perpendicular to the growth direction is broken. On the other side, vertical disorder is observed whenever layer thicknesses fluctuate around their nominal values. Compositional disorder due to different local Al concentration in each Ga1-xAlxAs layer can be viewed as mixing of vertical and lateral disorder.

### A Lateral disorder

In order to treat lateral disorder we have considered the formation of islands on the interface between two consecutive layers having identical lateral sizes all of them and being consecutive one to each other. In our model islands have heights that are randomly distributed (see Fig. 2). It is possible to express the rough profile of the interface between two consecutive layers defining the following height function

$$h(y)=\eta \underset{n}{}w_n\{\mathrm{\Theta }(yn\zeta )+\mathrm{\Theta }[(n+1)\zeta y]1\}.$$
(46)
Here $`h(y)`$ represents the deviation from the flat surface at position $`y`$, $`\mathrm{\Theta }`$ is the Heavyside theta function, $`\zeta `$ is the island width, $`w_n`$ is a random variable associated to the $`\mathrm{n}`$th island that controls the fluctuation around the mean value, and $`\eta `$ is the largest deviation —in absolute value— assuming that the $`w_n`$’s are uniformly distributed between $`1`$ and $`1`$. Hereafter $`\eta `$ will be referred to as degree of lateral disorder. In the following, two models will be introduced. First of all, uncorrelated disorder will be considered, for which the random variables $`w_n`$ take values from $`1`$ to $`1`$ uniformly, satisfying the following correlator $`w_nw_m=\delta _{nm}/3`$. However, experimental data and theoretical models of molecular-beam-epitaxy growth processes indicate that the heigths of the surface at distant points are strongly correlated. To mimic this situation, we will consider a second model of lateral disorder where the $`w_n`$’s are normally distributed with zero mean satisfying the exponential correlator $`w_nw_m=\mathrm{exp}(|nm|/\xi )/3`$, where $`\xi `$ is the correlation length of the disorder.

### B Compositional disorder

Compositional disorder in GaAs-AlxGa1-xAs heterostructures is due to the lack of spatial uniformity of the Al mole fraction during the heterostructure growth process. We will simulate compositional disorder by defining a spatial two-dimensional mesh over the AlxGa1-xAs barriers, as shown in Fig. 3. We will associate a value $`x_{ij}`$ for the Al mole fraction to each region of the mesh. This value will fluctuate randomly around the nominal value of the aluminum fraction on the barrier $`\overline{x}`$. Thus we can write

$$x_{ij}=\overline{x}+\mathrm{\Omega }w_{ij}$$
(47)
where $`\mathrm{\Omega }`$ is the maximum fluctuation of the Al mole fraction, and $`w_{ij}`$ is a random variable related to the $`(i,j)`$ point of the mesh, taking values uniformly between $`1`$ and $`1`$. Note that the overall averaged mole fraction is equal to $`\overline{x}`$.

## IV Results

We have performed several numerical calculations in order to study the effect of both lateral and compositional disorder over the transport properties of DBS made of GaAs-AlxGa1-xAs heterostructures.

### A Uncorrelated lateral disorder

We start by considering the effect of the interface roughness, characterized by the degree of lateral disorder $`\eta `$ given in (46), on the conductance. Figure 4 shows the conductance calculated for different values of $`\eta `$. Here $`a_y=10`$nm, $`a_z=0.3`$nm, $`\zeta =20`$nm, $`M=50`$, and $`N=38`$. The barrier widths are $`2.1`$nm for both the emitter and the collector, their heights are also the same, $`0.3`$eV, and the well width is $`4.8`$nm. The curves correspond to an ensemble average of the conductance curves over $`100`$ different realizations of the lateral disorder. Three different values of $`\eta `$ were studied, namely $`\eta =0`$ (perfect DBS), $`\eta =0.3`$nm (largest fluctuation of the order of one monolayer) and $`\eta =0.6`$nm (largest fluctuation of the order of two monolayers). As a main result, it can be seen in Fig. 4 that increasing the degree of lateral disorder, $`\eta `$, results in a decrease of the conductance at the resonant energy.

Notice that the resonant conductance peak slightly widens due to the fluctuations of its energy for each realization of the disorder. Besides, an additional effect can be seen, that is, as the degree of lateral disorder $`\eta `$ increases the conductance peak shifts to smaller energies. This effect will be important in order to explain the $`jV`$ characteristics later. Regarding the effect of the size of the islands, $`\zeta `$, we have observed that it can be neglected unless this size is of the order of the electron wavelength, that is, for $`\zeta \lambda _e`$ the conductance does not depend on $`\zeta `$. As expected, when $`\zeta \lambda _e`$ the electron starts to see the disorder and then the conductance increases as $`\zeta `$ decreases, as shown in Fig. 5. For energies about $`0.1`$eV this transition takes place at sizes $`\zeta 10`$nm .

Current as a function of the applied bias is depicted in Fig. 6. For this calculation we have chosen $`a_y=10`$nm, $`a_z=0.1`$nm, $`\zeta =10`$nm, $`M=20`$ and $`N=77`$. The barrier widths are $`2.1`$nm for both the emitter and the collector and their heights are also the same, $`0.25`$eV. The well width is $`2.9`$nm. Curves show in Fig. 6 correspond to an average over $`50`$ different realizations of the lateral disorder. The Fermi level was fixed at $`20`$meV, the maximum applied bias was $`0.5`$eV, and $`\eta =0.3`$ nm. Surprisingly, current in disordered DBS is larger than that measured in ordered DBS. This counterintuitive result can be explained recalling that conductance peak shifted to lower energies, as mentioned above. The lowering of the conductance peak can be understood assuming that surface roughness makes the effective width of the quantum well larger than its nominal value. This would imply a lower transmission resonance so the current peak shifts toward lower bias. But an effective wider well implies a higher current too, so in some statistical sense the current for the disordered DBS will be higher.

### B Correlated lateral disorder

Up to now we have been considering only lateral uncorrelated roughness at the heterojunctions. We have also calculated the conductance for a DBS in which interface roughness is an exponentially correlated random variable, as described previously. Figure 7 shows the conductance at a given energy about the conductance resonance for the ordered case (where fluctuations are lower), $`E_c=0.1025`$ eV, when the correlation length varies several orders of magnitude. Physical parameters of the DBS are the same as in Fig. 4. The size of the islands is $`20`$nm and the degree of lateral disorder is $`\eta =0.3`$nm. An average over 50 realizations of the disorder has been performed. It can be observed that the conductance increases as the correlation length increases. Two asymptotic regimes are clearly observed for small and large correlation lengths, respectively. The former limit, $`\xi 0`$, can be understood as the situation previously studied where lateral disorder is uncorrelated. From a closed inspection of Fig. 7 we come to the remarkable result that this uncorrelated limit correctly describes transport properties whenever the correlation length do not exceed $`10`$nm. Then we are led to an important conclusion, namely those models of electron transport in disordered DBS based on the assumption that disorder is uncorrelated would yield right values of the conductance even if the correlation length is not vanishing but fairly large. There is no need to mention that uncorrelated disordered models are much more convenient for analytical work than correlated ones. The size of the plateau for which correlations in the disorder do not play an essential role is governed by the size of the islands, $`\zeta `$, as might be expected. This is due to the fact that only correlations of the lateral disorder whose correlation length is greater than the size of the islands affect electron motion. For these sizes, the conductance increases as the correlation length becomes larger. This trend is observed up to sizes of the order of $`100`$nm, namely the system size in the $`y`$ direction, and then the second regime appears. In this regime the limiting value of the conductance can be calculated as an average over different ordered DBS, each one having barrier widths distributed normally.

### C Compositional disorder

Having discussed the effects of interface roughness, let us now present our results regarding compositional disorder. To clarify the effects of local fluctuations of the Al mole fraction, we assume that the interfaces are perfectly flat and that the width of the different semiconductor layers are exactly their nominal values, i.e., we neglect fluctuations of their widths. We show typical results in Fig. 8, where physical parameters are the same as in Fig. 4. The espatial extend of the region where the Al mole fraction can be assumed locally constant was taken to be $`a=10`$nm and $`b=1`$nm (see Fig. 3). It can be observed that, for fluctuations as large as $`\mathrm{\Omega }=0.14`$, that is, height fluctuations of about $`0.1`$ eV, when averaging over $`100`$ realizations the conductance is almost unchanged (only 3% variation). This behavior is a consequence of the small electron probability amplitudes within the barriers, where compositional disorder is considered to appear. In other words, even moderately high spatial inhomogeneities in the barriers scarcely affect the electron envelope function. Thus we can conclude that the effects of compositional disorder can be disregarded as they are much smaller than those of lateral disorder.

## V Conclusions

In this paper we have presented a method to study electron transport in unintentionally disordered DBS when translational symmetry along the normal plane to the growth direction is broken by structural imperfections. Two different kinds of disorder leading to electron scattering has been presented, namely lateral disorder and compositional disorder. Lateral disorder appears as a consequence of the roughness present at the interfaces between GaAs and AlxGa1-xAs. Compositional disorder is due to the inhomogeneity of the Al mole fraction occurring during the growth process of AlxGa1-xAs epilayers. We have shown that the main effect of the lateral disorder is to decrease the DBS conductance. When correlations are introduced, conductance starts improving, the larger the correlation length, the higher the conductance. However, current shows a surprising behavior, as it is higher in the disordered case than in the ordered one. We attributed it to an energy shift of the transmission resonance of the DBS. Another important conclusion regards the validity of uncorrelated disordered models; they provide right values of the conductance whenever the actual correlation length does not exceed the system size, thus allowing a simpler theoretical description. Finally we have shown that the effect of compositional disorder can be disregarded as it is much smaller than the effect of lateral disorder.

###### Acknowledgements.

The authors want to thank V. A. Malyshev for the critical reading of the manuscript. Work in Madrid was supported by DGI-MCyT (Project MAT2000-0734) and CAM (Project 07N/0075/2001). P. Orellana would like to thank Milenio ICM P99-135-F and Cátedra Presidencial de Ciencias for financial support.


text:
# Enrichment of nuclear spin isomers by molecular coherent control

## I Introduction

Nuclear spin isomers were discovered in the late 1920s when ortho and para H2 were separated by deep cooling of hydrogen gas Farkas35 . This technique was successful because of extremely large gap between the ortho and para states in H2. Investigations of heavier isomers were not possible to perform until recently because of the lack of appropriate enrichment methods. First separation of heavy molecules (CH3F) was achieved using the Light-Induce Drift effect Krasnoperov84JETPL . Later, the isomers of H2O Konyukhov86JETPL , H2CO Kern89CPL , Li2 Bernheim90JCP , and C2H4 Chap00CPL  were enriched. A few practical applications of spin isomer are already known. For example, isomers can affect chemical reactions Quack77MP ; Uy97PRL , can significantly enhance NMR signals Bowers86PRL ; Bargon93ZPC , or can be used as spin labels in NMR based techniques.

Further investigations of nuclear spin isomers and progress in their applications need new enrichment methods. This is rather difficult and challenging task because physical and chemical properties of spin isomers are almost identical. Recently new approach to the isomer enrichment based on molecular excitation by strong electromagnetic field was proposed Ilichov98CPL ; Shalagin99JETPL ; Chap01PRA2 ; Chap01JPB . In this paper we discuss the isomer enrichment based on the coherent control by strong infrared radiation. We make emphasis on the conditions necessary for the experimental observation of the phenomenon.

## II Level scheme

The level scheme is shown in Fig. 1. We assume that test molecules have only two nuclear spin states, ortho and para. This is very often the case, e.g., in CH3F Landau81 ; Chap99ARPC . Each of the two vibrational states (ground and excited) has one ortho-para level pair mixed by intramolecular perturbation. Molecules are embedded into a “nonmagnetic” gaseous environment characterized by zero cross-section for collisional ortho-para transition. The infrared radiation is resonant to the rovibrational transition $`mn`$ of the ortho molecules.

The molecular Hamiltonian in our problem consists of four terms,

$$\widehat{H}=\widehat{H}_0+\mathrm{}\widehat{H}_{rad}+\mathrm{}\widehat{V}+\mathrm{}\widehat{V}^{}.$$
(1)
The main part, $`\widehat{H}_0`$, has the eigen ortho and para states shown in Fig. 1. $`\mathrm{}\widehat{H}_{rad}`$ describes the molecular interactions with the external radiation that will be taken in the form of monochromatic travelling wave,

$$\widehat{H}_{rad}=2\widehat{G}\mathrm{cos}(\omega _Lt\mathrm{𝐤𝐫});\widehat{G}=𝐄_0\widehat{𝐝}/2\mathrm{},$$
(2)
where $`𝐄_0`$; $`\omega _L`$ and $`𝐤`$ are the amplitude, frequency and wave vector of the electromagnetic wave, respectively; $`\widehat{𝐝}`$ is the molecular electric dipole moment operator. $`\widehat{V}`$ and $`\widehat{V}^{}`$ are the intramolecular perturbations that mix the ortho and para states in excited and ground vibrational states, respectively. These perturbations originate from the nuclear spin-spin and spin-rotation interactions Curl67JCP ; Chap91PRA ; Guskov95JETP ; Ilisca98PRA .

Suppose that a test molecule is placed initially in the ortho subspace of the ground vibrational state. Due to collisions the molecule will undergo fast rotational and velocity relaxation inside the ortho subspace. This will proceed until the molecule jumps to the state $`m^{}`$, which is mixed with the para state $`k^{}`$ by the intramolecular perturbation $`\widehat{V}^{}`$ (see Fig. 1), or to the state $`n`$ which is mixed with the para state $`k`$ by the combined action of the external field and intramolecular perturbation $`\widehat{V}`$. Admixture of a para state implies that the next collision can move the molecule to another para states and thus localize it inside the para subspace. The spin conversion occurs.

The molecular center-of-mass motion affects the process because of the Doppler effect. Vibrational degree of freedom plays an important role too. After ortho-para transition in upper vibrational state the molecule relaxes to the ground vibrational state. Consequently, back conversion can only occur through the unperturbed $`m^{}k^{}`$ channel. It is essential that conversion through the $`mk`$ channel can be substantially affected by electromagnetic radiation.

Quantitative description of the isomer conversion can be done using the perturbation theory Chap01MP . The zeroth-order theory neglects the intramolecular ortho-para state mixing by $`\widehat{V}`$ and $`\widehat{V}^{}`$ and thus contains no ortho-para conversion. In this approximation an external field does not affect the population of para states. The populations of ortho states in the model of strong collisions read,

$`\rho _o(e,j,𝐯)`$ $`=`$ $`\rho _o\{p(\mathrm{\Omega })\tau _{ev}w_jf(𝐯)+p(\mathrm{\Omega },𝐯)[\tau _{et}w_j+\tau _e\delta _{jm}]\},`$
$`\rho _o(g,j,𝐯)`$ $`=`$ $`\rho _ow_jf(𝐯)\rho _o\{p(\mathrm{\Omega })\tau _{gv}w_jf(𝐯)+p(\mathrm{\Omega },𝐯)[\tau _{gt}w_j+\tau _g\delta _{jn}]\}.`$ (3)
Here $`\rho _o`$ is the total concentration of ortho molecules; $`e,g`$ designate the excited and ground vibrational states, respectively; $`j`$ is the rotational quantum number; $`w_j`$ is the Boltzmann distribution; $`f(𝐯)`$ is the Maxwell distribution and $`𝐯`$ is the molecular center-of-mass velocity. The level populations in Eq. (3) are split into the terms nonequilibrium in $`j`$ and v, nonequilibrium only in v, and equilibrium in $`j`$ and v. The magnitudes of these terms are proportional to specific relaxation parameters $`\tau `$’s (see Ref. Chap01MP  for more details). The function $`p(\mathrm{\Omega },𝐯)`$ is the excitation probability of molecules with particular velocity v and $`p(\mathrm{\Omega })=p(\mathrm{\Omega },𝐯)𝑑𝐯`$,

$`Y(\mathrm{\Omega })`$ $`=`$ $`{\displaystyle \frac{\mathrm{\Gamma }_B^2f(𝐯)d𝐯}{\mathrm{\Gamma }_B^2+(\mathrm{\Omega }\mathrm{𝐤𝐯})^2}},`$
$`p(\mathrm{\Omega })`$ $`=`$ $`{\displaystyle \frac{w_n}{\tau _1}}{\displaystyle \frac{Y(\mathrm{\Omega })}{1+\kappa ^1+Y(\mathrm{\Omega })\tau _2\tau _1^1}},p(\mathrm{\Omega },𝐯)={\displaystyle \frac{p(\mathrm{\Omega })}{Y(\mathrm{\Omega })}}{\displaystyle \frac{\mathrm{\Gamma }_B^2f(𝐯)}{\mathrm{\Gamma }_B^2+(\mathrm{\Omega }\mathrm{𝐤𝐯})^2}}.`$ (4)
Here $`\mathrm{\Omega }=\omega _L\omega `$ and $`\omega \omega _{mk}`$ is the gap between the states $`m`$ and $`k`$. The function $`p(\mathrm{\Omega })`$ is the Foigt profile of the absorption line having the homogeneous linewidth $`\mathrm{\Gamma }_B=\mathrm{\Gamma }\sqrt{1+\kappa }`$, where $`\kappa `$ is the saturation parameter, $`\kappa =2|G|^2\tau _1\mathrm{\Gamma }^1`$; $`|G|=E_0|d_{mn}|/2\mathrm{}`$ is the Rabi frequency; $`\mathrm{\Gamma }`$ is the collisional linewidth of the absorbing transition; $`\tau _1=\tau _{et}w_m+\tau _{gt}w_n+\tau _e+\tau _g`$ and $`\tau _2=\tau _{ev}w_m+\tau _{gv}w_n`$.

In addition to the level population change, an external radiation creates a coherence (off-diagonal density matrix element) on the $`mn`$ transition,

$$\rho _o(n|m;𝐯)=i\rho _o\frac{p(\mathrm{\Omega },𝐯)}{2G\mathrm{\Gamma }}[\mathrm{\Gamma }i(\mathrm{\Omega }\mathrm{𝐤𝐯})]e^{i(\mathrm{\Omega }t\mathrm{𝐤𝐫})}.$$
(5)
## III Enrichment

The first-order theory takes the intramolecular perturbations $`\widehat{V}`$ and $`\widehat{V}^{}`$ into account. In this approximation the spin conversion appears and it can be affected by the radiation. An external radiation changes the concentration of ortho molecules from the equilibrium value, $`\rho _o(0)`$, to the steady-state value, $`\overline{\rho }_o`$. Because the total concentration of the test molecules is conserved, one has steady-state enrichment of para molecules Chap01MP ,

$$\beta \frac{\overline{\rho }_p}{\rho _p(0)}1=1\frac{\gamma _{free}}{\gamma },\gamma =\gamma _{free}\gamma _n^{}+\gamma _n+\gamma _{coh}.$$
(6)
Here an equal concentrations of ortho and para molecules in equilibrium gas has been assumed that, implies $`w_m^{}=w_k^{}`$. The conversion rate $`\gamma `$ has four terms of different origin. The first one,

$$\gamma _{free}=\frac{2\mathrm{\Gamma }|V^{}|^2}{\mathrm{\Gamma }^2+\omega ^2}[w_k^{}+w_m^{}],$$
(7)
is the conversion rate without an external electromagnetic field; $`\omega ^{}\omega _{m^{}k^{}}`$ is the gap between the states $`m^{}`$ and $`k^{}`$. One can see from Eq. (6) that the light-induced enrichment is enhanced by small $`\gamma _{free}`$. The second term is due to the light-induced level depopulation in the ground vibrational state,

$$\gamma _n^{}=\frac{2\mathrm{\Gamma }|V^{}|^2}{\mathrm{\Gamma }^2+\omega ^2}p(\mathrm{\Omega })w_m^{}(\tau _{gv}+\tau _{gt})=\frac{1}{2}\gamma _{free}p(\mathrm{\Omega })(\tau _{gv}+\tau _{gt}).$$
(8)
The last two terms in $`\gamma `$ is convenient to present in a form that can be easily obtained from Chap01MP . The “noncoherent” contribution to the rate,

$$\gamma _n=\frac{2\mathrm{\Gamma }|V|^2}{\mathrm{\Gamma }^2+\omega ^2}p(\mathrm{\Omega })\tau +2|V|^2Re\left(1\frac{\mathrm{\Gamma }_1+i\omega _1}{\mathrm{\Gamma }+i\omega }\right)\frac{\rho _o^1\rho _o(e,m,𝐯)d𝐯}{\mathrm{\Gamma }_1+i(\mathrm{\Omega }+\omega _1\mathrm{𝐤𝐯})}.$$
(9)
Here $`\tau =\tau _{ev}w_m+\tau _{et}w_m+\tau _e`$. The “coherent” part, $`\gamma _{coh}`$, originates from the light-induced coherence (5),

$$\gamma _{coh}=\frac{|V|^2p(\mathrm{\Omega })}{\mathrm{\Gamma }^2+\omega ^2}+\frac{|V|^2}{\mathrm{\Gamma }}Re\frac{\mathrm{\Gamma }+\mathrm{\Gamma }_1+i\omega _1}{\mathrm{\Gamma }+i\omega }\frac{p(\mathrm{\Omega },𝐯)d𝐯}{\mathrm{\Gamma }_1+i(\mathrm{\Omega }+\omega _1\mathrm{𝐤𝐯})}.$$
(10)
The new homogeneous width, $`\mathrm{\Gamma }_1`$, and the ortho-para level gap, $`\omega _1`$, are

$$\mathrm{\Gamma }_1=\mathrm{\Gamma }\left(1+\frac{|G|^2}{\mathrm{\Gamma }^2+\omega ^2}\right),\omega _1=\omega \left(1\frac{|G|^2}{\mathrm{\Gamma }^2+\omega ^2}\right).$$
(11)
One can see from Eqs. (8), (9), and (10) that the conversion rate, $`\gamma `$, has two peaks. The peak at the absorption line center ($`\mathrm{\Omega }=0`$) appears because the excitation probabilities, $`p(\mathrm{\Omega })`$ and $`p(\mathrm{\Omega },𝐯)`$, have maximum at $`\mathrm{\Omega }=0`$. The homogeneous width of this peak is equal to $`\mathrm{\Gamma }_B`$ that can be very large in molecular systems due to the slow rotational, velocity, and vibrational relaxations. The peak at $`\mathrm{\Omega }=\omega _1`$ is due to the light-induced crossing of $`m`$ and $`k`$ states (see Ref. Chap01PRA2 ; Chap01JPB ; Chap01MP ) and appears formally because of the resonant denominators in the integrands in Eq. (9) and (10). The homogeneous width of the peak at $`\mathrm{\Omega }=\omega _1`$ is equal to $`\mathrm{\Gamma }_1`$.

Coherent control allows to achieve substantial enrichment if the mixing in ground and vibrationally excited states has the same order of magnitude Chap01MP . On the other hand, close coincidences between ortho and para states in molecules are rather rare. Consequently, such close level pairs in excited vibrational state may be absent, or they cannot be accessible by the available radiation. Below we estimate the enrichment in the case of large ortho-para gap in excited state, $`\omega kv_0\mathrm{\Gamma }`$, where $`kv_0`$ is the Doppler parameter and $`v_0`$ is the molecular thermal velocity, $`v_0=\sqrt{2k_BT/M}`$. For moderate radiation intensities, $`|G|\omega `$, the field-dependent terms at the absorption line center, $`\mathrm{\Omega }=0`$, are

$$\gamma _n^{}(0)0.5\gamma _{free}p(0)(\tau _{gv}+\tau _{gt});\gamma _n(0)\frac{2|V|^2}{\omega ^2}p(0)\tau \mathrm{\Gamma };\gamma _{coh}(0)\frac{|V|^2}{\omega ^2}p(0).$$
(12)
The terms $`\gamma _n(0)`$ and $`\gamma _{coh}(0)`$ have the “off-resonant” nature which manifests itself by the large ortho-para gap, $`\omega `$, in the denominators. At large $`\omega `$, the conversion rate, $`\gamma (0)`$, is determined mainly by $`\gamma _n^{}(0)`$ and the radiation depletes the para molecules,

$$\beta (0)0.5p(0)(\tau _{gv}+\tau _{gt}).$$
(13)
This is analogous to the enrichment by light-induced population change Ilichov98CPL ; Shalagin99JETPL . Maximum of $`\beta (0)`$ is achieved at sufficiently strong field, $`\mathrm{\Gamma }_Bkv_0`$. In this case, $`Y(0)1`$, $`p(0)w_n/(\tau _1+\tau _2)`$ and enrichment reaches the value,

$$\beta _{max}(0)w_n\frac{\tau _{gv}+\tau _{gt}}{\tau _1+\tau _2}.$$
(14)
Depending on the relaxation scheme and the origin of the relaxation “bottle neck”, one can achieve different level of enrichment. In the most favorable situation of fast velocity and rotational relaxations the enrichment reaches -1/4.

Larger enrichment can be achieved at the level-crossing resonance. The field-dependent rates at the $`\mathrm{\Omega }=\omega _1`$ can be readily estimated if $`\mathrm{\Gamma }_Bkv_0`$. In this case $`p(\omega _1,𝐯)p(\omega _1)f(𝐯)`$ and one has,

$`\gamma _n^{}(\omega _1)`$ $``$ $`0.5\gamma _{free}p(\omega _1)(\tau _{gv}+\tau _{gt}),`$
$`\gamma _n(\omega _1)`$ $``$ $`{\displaystyle \frac{2\sqrt{\pi }|V|^2}{kv_0}}{\displaystyle \frac{|G|^2}{\omega ^2}}p(\omega _1)\tau ,\gamma _{coh}(\omega _1){\displaystyle \frac{\sqrt{\pi }|V|^2}{kv_0}}p(\omega _1)\mathrm{\Gamma }^1.`$ (15)
The terms, $`\gamma _n(\omega _1)`$ and $`\gamma _{coh}(\omega _1)`$ are due to the light-induced crossing of the $`m`$ and $`k`$ states that has an efficient width equal $`kv_0/\sqrt{\pi }`$ (compare with the level crossing in molecules being at rest Chap01JPB ). The main contribution to $`\gamma (\omega _1)`$ comes from $`\gamma _{coh}(\omega _1)`$ if $`|G|\omega `$.

The results (12) and (15) allows to determine which peak, $`\mathrm{\Omega }=0`$, or $`\mathrm{\Omega }=\omega `$, should be used for enrichment. At low radiation intensity larger enrichment is achieved at $`\mathrm{\Omega }=0`$ because $`p(0)p(\omega _1)`$ if $`\mathrm{\Gamma }_B\omega `$. If radiation intensity is high, $`\mathrm{\Gamma }_B\omega `$, larger enrichment is obtained at $`\mathrm{\Omega }=\omega _1`$. The ratio of the two peaks reads,

$$\frac{\gamma (\omega _1)}{\gamma (0)}\frac{\gamma _{coh}(\omega _1)}{\gamma _n^{}(0)}\frac{2\sqrt{\pi }|V|^2}{\gamma _{free}kv_0}\mathrm{\Gamma }^1(\tau _{gv}+\tau _{gt})^1.$$
(16)
The amplitude of the enrichment peak at $`\mathrm{\Omega }=\omega _1`$ as a function of $`|G|`$ and various values of $`\omega `$ are shown in Fig. 2. The calculations were done using the exact expressions for the conversion rates, (7)–(10). In this numerical example the following parameters were used Chap01MP , $`V=3`$ kHz, $`V^{}=5`$ kHz, $`\mathrm{\Gamma }=2`$ MHz, $`\omega ^{}=130`$ MHz, $`kv_0=30`$ MHz; $`\tau _1=5`$ MHz-1; $`\tau _2=1`$ MHz-1 and all Boltzmann factors equal, $`w_m=w_n=w_k=w_m^{}=w_k^{}=10^2`$.

## IV Discussion

Conditions necessary for the experimental observation of the light-induced enrichment are not easy to fulfil. First of all, the field free conversion rate, $`\gamma _{free}`$, of the molecules under consideration should be low in order to enhance the role of light-induced changes in the total rate, $`\gamma `$. Note that the rate $`\gamma _{free}`$ should combine all significant contributions, e.g., caused by the molecular collisions with the walls of the gas container. At present, only in a few rare cases (see the Introduction) the rates $`\gamma _{free}`$ are known.

Next task is to determine the target ortho-para level pair in the excited vibrational state. For this, one has to know rather accurately the relative positions of ortho and para states and the intramolecular ortho-para mixing efficiency as well.

Perhaps, the most difficult problem is to find powerful radiation having right frequency. The most promising sources of such radiation are the powerful Free Electron Lasers.

## Acknowledgments

This work was made possible by financial support from the Russian Foundation for Basic Research (RFBR), grant No. 01-03-32905 and from The Institute of Physical and Chemical Research (RIKEN), Japan.