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# Finite resolution measurement of the non-classical polarization statistics of entangled photon pairs

## I Introduction

Perhaps the most convincing proof of the non-classical nature of quantum statistics is the violation of Bell’s inequalities by a pair of entangled spin-1/2 particles . Several experimental tests of these inequalities have been performed on pairs of entangled photons generated either by two photon emission  or by parametric down conversion . These experimental tests compare the polarization correlations of photon pairs emitted at the same time for different sets of orthogonal polarizations. While no information about the relationship between non-orthogonal polarization directions of the single photon are revealed in such measurements, the statistics obtained correspond to the quantum theoretical prediction. Since the quantum formalism from which the violation of Bell’s inequalities is derived is widely accepted, one might wonder whether it should not be possible to obtain a clearer understanding of the origin of this non-classical effect by investigating the unique statistical connection between non-commuting quantum variables in more detail. In particular, finite resolution measurements can provide quantitative information about a quantum variable without destroying the quantum coherence between different eigenstate components of that variable . By applying finite resolution measurements, it is therefore possible to identify the non-classical correlations between non-commuting variables directly . In the following, an experiment is proposed to determine the correlations between non-orthogonal polarizations of entangled photon pairs. It is shown that the violation of Bell’s inequalities results from the negative joint probabilities arising from local non-classical correlations of the photon polarization. It is then possible to give a local interpretation of entanglement based on standard quantum mechanics.

The rest of the paper is organized as follows. In section II, the application of finite resolution measurements to the polarization of a single photon is discussed and fundamental non-classical correlations are derived. In section III, the experimental setup for a measurement of entangled photon pairs is presented and the statistical results of such a measurement are derived. In section IV, the non-classical features of the statistics are identified and the implications concerning the nature of entanglement are discussed. Finally, the conclusions are summarized in section V.

## II Finite resolution measurements

### A The generalized measurement postulate

A measurement assigns a quantity to a system property based on the observable action of the system on some measurement device. The uncertainty principle of quantum mechanics requires that this interaction between the system and the measurement setup introduces noise into properties that do not commute with the measured variable. Therefore, the classical ideal of a complete determination of all system properties is unattainable. Nevertheless it is possible to obtain quantitative information on the correlations between non-commuting variables by limiting the measurement resolution. Such a finite resolution measurement is described by the generalized measurement operator $`\widehat{P}_{\delta s}(s_m)`$, which assigns a continuous measurement value $`s_m`$ to the operator $`\widehat{s}`$. It reads

$$\widehat{P}_{\delta s}(s_m)=\left(2\pi \delta s^2\right)^{\frac{1}{4}}\mathrm{exp}\left(\frac{(s_m\widehat{s})^2}{4\delta s^2}\right).$$
(1)
For a given initial state $`\psi _{\text{in}}`$, the probability $`P(s_m)`$ of obtaining a measurement result $`s_m`$ and the state $`\psi _{\text{out}}`$ after the measurement are then given by

$`P(s_m)`$ $`=`$ $`\psi _{\text{in}}\widehat{P}_{\delta s}^2(s_m)\psi _{\text{in}}`$ (2)
$`\psi _{out}`$ $`=`$ $`{\displaystyle \frac{1}{\sqrt{P(s_m)}}}\widehat{P}_{\delta s}(s_m)\psi _{in}.`$ (3)
Note that this generalized measurement postulate does not restrict the values of an operator variable to the eigenvalues of that operator. Eigenvalues emerge only in infinitely precise measurements. One of the fundamental problems in the discussion of quantum mechanics is that eigenvalues are often identified with “elements of reality” regardless of the measurement context discussed. By assigning a continuous measurement value to the operator variable in a finite resolution measurement this identification is avoided, allowing a determination of quantitative results beyond the spectrum of its eigenvalues.

### B Finite resolution measurement of photon polarization

The polarization of a single photon can be described in terms of the Stokes parameters $`\widehat{s}_i`$. In terms of the circular polarization eigenstates $`R`$ and $`L`$, the operators of the three single photon Stokes parameters may be written as

$`\widehat{s}_1`$ $`=`$ $`LR+RL`$ (4)
$`\widehat{s}_2`$ $`=`$ $`iLRiRL`$ (5)
$`\widehat{s}_3`$ $`=`$ $`RRLL.`$ (6)
$`\widehat{s}_1`$ represents the intensity difference between the x and y polarizations, $`\widehat{s}_2`$ represents the intensity difference between the polarizations along the diagonals between the x and y axes, and $`\widehat{s}_3`$ represents the intensity difference between the circular polarizations. Since only one photon is considered, the eigenvalues of each Stokes parameter are $`\pm 1`$.

A finite resolution measurement of photon polarization can be realized by using a polarization sensitive beam displacer that shifts the x-polarization component relative to the y-polarization component of the light field. The displacement of the photon trajectory in the beam displacer can be interpreted as the action of the one-photon Stokes parameter $`\widehat{s}_1`$. The polarization of the photon is then described by a continuous value $`s_{1m}`$ of the Stokes parameter $`\widehat{s}_1`$ obtained from the measurement of the transversal photon position after the beam displacer. The measurement resolution depends on the ratio of the displacement and the width of the input beam. If the transversal profile of the light field is Gaussian, the generalized measurement postulate describes the single photon polarization statistics obtained by measuring the polarization dependent displacement of the photon. In terms of the circular polarization eigenstates, the measurement operator is given by

$`\widehat{P}_{\delta s}(s_{1m})=(2\pi \delta s^2)^{\frac{1}{4}}\mathrm{exp}\left({\displaystyle \frac{s_{1m}^2+1}{4\delta s^2}}\right)`$ (7)
$`\times (`$ $`\mathrm{cosh}\left({\displaystyle \frac{s_{1m}}{2\delta s^2}}\right)\left(RR+LL\right)`$ (9)
$`+\mathrm{sinh}\left({\displaystyle \frac{s_{1m}}{2\delta s^2}}\right)(RL+LR)).`$
This operator describes the changes in the quantum state of the single photon polarization conditioned by the finite resolution measurement of the Stokes parameter $`\widehat{s}_1`$.

### C Joint measurements of non-orthogonal polarizations

In order to measure the correlated non-orthogonal polarization components of a single photon, the finite resolution measurement can be combined with a fully resolved polarization measurement. By rotating the polarization by an angle of $`\pi /4`$ and separating the x and y components as shown in figure 1, the eigenvalues of the Stokes parameter $`\widehat{s}_2`$ are measured. Two spatial patterns emerge, corresponding to the conditional distributions of continuous measurement results $`s_{1m}`$ of the Stokes parameter $`\widehat{s}_1`$ associated with a final measurement of the eigenvalues $`+1`$ or $`1`$ of the Stokes parameter $`\widehat{s}_2`$. The positive valued operator measure (POM) describing the joint measurement of $`\widehat{s}_1`$ and $`\widehat{s}_2`$ is defined by projections onto the states

$$s_{1m};s_2=\pm 1=\widehat{P}_{\delta s}(s_{1m})\frac{1}{\sqrt{2}}\left(R\pm iL\right).$$
(10)
The joint probabilities $`P(s_{1m};s_2=\pm 1)`$ for measuring a finite resolution value of $`s_{1m}`$ for the Stokes parameter $`\widehat{s}_1`$ followed by an eigenvalue of $`s_2=\pm 1`$ for the Stokes parameter $`\widehat{s}_2`$ is then given by

$`P(s_{1m};s_2=\pm 1)`$ $`=`$ $`|s_{1m};s_2=\pm 1\psi _{\text{in}}|^2`$ (11)
$`=`$ $`{\displaystyle \frac{1}{2}}\left|R\widehat{P}_{\delta s}(s_{1m})\psi _{\text{in}}iL\widehat{P}_{\delta s}(s_{1m})\psi _{\text{in}}\right|^2,`$ (12)
where $`\psi _{\text{in}}`$ is an arbitrary initial state. This POM thus assigns quantitative results to both Stokes parameters, allowing a derivation of correlations between the polarization components of a single photon.

If the light field entering the measurement setup shown in figure 1 is polarized along the diagonal between the x and y axes, the initial photon state is given by

$$\psi _{\text{in}}=\frac{1}{\sqrt{2}}\left(R+iL\right).$$
(13)
The joint probabilities of the measurement results $`s_{1m}`$ and $`s_2`$ can then be determined using equation (11). In its most compact form, it reads

$`P(s_{1m};s_2=+1)`$ $`=`$ $`\left(2\pi \delta s^2\right)^{\frac{1}{2}}\mathrm{exp}\left({\displaystyle \frac{s_{1m}^2+1}{2\delta s^2}}\right)\mathrm{cosh}^2\left({\displaystyle \frac{s_{1m}}{2\delta s^2}}\right)`$ (14)
$`P(s_{1m};s_2=1)`$ $`=`$ $`\left(2\pi \delta s^2\right)^{\frac{1}{2}}\mathrm{exp}\left({\displaystyle \frac{s_{1m}^2+1}{2\delta s^2}}\right)\mathrm{sinh}^2\left({\displaystyle \frac{s_{1m}}{2\delta s^2}}\right).`$ (15)
Note that $`P(s_{1m}=0;s_2=1)`$ is always exactly equal to zero, even if $`\delta s`$ is larger than one. Obviously, this result is too exact to be explained in terms of a random measurement error superimposed on classical statistics. The result for a measurement resolution of $`\delta s=0.6`$ is illustrated in figure 2. The peaks in $`P(s_{1m};s_2=1)`$ are shifted to values of about $`\pm 1.1`$ and the asymmetry of the peaks seems to favor even higher values. These results can hardly be explained by statistics originating only from the eigenvalues of $`s_1=\pm 1`$.

### D Negative conditional probabilities and non-classical correlations in the polarization of single photons

The non-classical features of the joint probabilities $`P(s_{1m};s_2=\pm 1)`$ can be analyzed by expressing the result as a sum of shifted normalized Gaussian distributions

$$G_{\delta s}(s_{1m}d):=\left(2\pi \delta s^2\right)^{\frac{1}{2}}\mathrm{exp}\left(\frac{(s_{1m}^2d)^2}{2\delta s^2}\right).$$
(16)
In terms of these Gaussians, the joint probabilities read

$`P(s_{1m};s_2=+1)`$ $`=`$ $`{\displaystyle \frac{1}{4}}G_{\delta s}(s_{1m}+1)+\mathrm{exp}\left({\displaystyle \frac{1}{2\delta s^2}}\right){\displaystyle \frac{1}{2}}G_{\delta s}(s_{1m})+{\displaystyle \frac{1}{4}}G_{\delta s}(s_{1m}1)`$ (17)
$`P(s_{1m};s_2=1)`$ $`=`$ $`{\displaystyle \frac{1}{4}}G_{\delta s}(s_{1m}+1)\mathrm{exp}\left({\displaystyle \frac{1}{2\delta s^2}}\right){\displaystyle \frac{1}{2}}G_{\delta s}(s_{1m})+{\displaystyle \frac{1}{4}}G_{\delta s}(s_{1m}1).`$ (18)
Each Gaussian contribution to the joint probabilities given in equation (17) can be identified with elements of the density matrix of the original state in the eigenstate basis of the observable $`\widehat{s}_1`$. As discussed in a previous paper , the measurement of $`s_{1m}`$ modifies each matrix element by a decoherence factor given by the difference of the eigenvalues and an information factor depending on the difference between the measurement result $`s_{1m}`$ and the average of the eigenvalues.

The decoherence factor $`\mathrm{exp}(1/(2\delta s^2))`$ is a result of the quantum noise in the measurement required by the uncertainty principle. In the case of the beam displacer acting on single photons, it is the uncertainty of the wave vector dependent time the photon spends in the birefringent medium which randomly rotates the Stokes vector around the $`s_1`$ axis. Since this noisy interaction is statistically independent of the measurement result, it is possible to separate its effect from the information obtained about the system. A hypothetical noise free measurement then reveals negative probabilities of $`s_2=1`$ for measurement results $`s_{1m}`$ close to zero . These negative probabilities describe the non-classical correlations between non-commuting operator variables .

The information about $`\widehat{s}_1`$ obtained in the measurement modifies the statistical weight of each density matrix element by a Gaussian function of the difference between the measurement result $`s_{1m}`$ and the average of the two eigenvalues of the density matrix element. In particular, the Gaussians centered around $`s_{1m}=0`$ represent contributions from the quantum coherence between the $`s_1=+1`$ and the $`s_1=1`$ eigenstates conditioned by a measurement of $`s_{1m}`$. Measurement results close to $`s_{1m}=0`$ enhance the coherence and increase the probability of $`s_2=+1`$ to values above 1, while measurement results far away from $`s_{1m}=0`$ reduce the coherence, lowering the probability of $`s_2=+1`$ to values below 1. In order to explain this non-classical correlation between $`s_1`$ and $`s_2`$, some measure of reality must be attributed to $`s_1=0`$, even though it is not an eigenvalue of $`\widehat{s}_1`$ . Since the width of the Gaussians represents the effect of random noise in the readout of the finite resolution measurement, it is reasonable to identify each Gaussian contribution with its average value of $`s_{1m}`$. The continuum of measurement values $`s_{1m}`$ can then be represented by a discrete set of three values at $`s_1=\pm 1`$ and $`s_1=0`$. The joint probabilities for these three values of $`s_1`$ and the two eigenvalues of $`s_2`$ read

$`P(s_1=1;s_2=1)=1/4`$ $`P(s_1=1;s_2=+1)=1/4`$ (19)
$`P(s_1=0;s_2=1)=1/2`$ $`P(s_1=0;s_2=+1)=1/2`$ (20)
$`P(s_1=+1;s_2=1)=1/4`$ $`P(s_1=+1;s_2=+1)=1/4.`$ (21)
These joint probabilities explain the non-classical features of the quantum statistics obtained from the single photon polarization measurement setup shown in figure 1 for any value of the measurement resolution $`\delta s`$.

It should be noted that the measurement setup itself defines an asymmetry between $`\widehat{s}_1`$ and $`\widehat{s}_2`$ since the non-eigenvalue of zero appears only in the statistics of the initial finite resolution measurement of $`\widehat{s}_1`$. This dependence on the order of measurement is reflected in the operator order dependence of quantum mechanical expectation values. In order to identify the operator properties responsible for the appearance of negative probabilities in the statistical properties, it is useful to characterize the measurement statistics in terms of the correlation between $`s_{1m}^2`$ and $`s_2`$,

$`C(s_{1m}^2,s_2)`$ $`=`$ $`s_{1m}^2s_2s_{1m}^2s_2`$ (22)
$`=`$ $`2(s_{1m}^2\delta s^2)s_2`$ (23)
$`=`$ $`2\mathrm{exp}\left({\displaystyle \frac{1}{2\delta s^2}}\right),`$ (24)
where $``$ denotes statistical averages over actual measurement results. This correlation may be expressed in terms of the operator expectation values of $`\psi _{\text{in}}`$ as

$$C(s_1^2,s_2)=\mathrm{exp}\left(\frac{1}{2\delta s^2}\right)\left(\psi _{\text{in}}\widehat{s}_1\widehat{s}_2\widehat{s}_1\psi _{\text{in}}\psi _{\text{in}}\widehat{s}_1^2\psi _{\text{in}}\psi _{\text{in}}\widehat{s}_2\psi _{\text{in}}\right).$$
(25)
As explained above, the exponential factor expresses the randomization of $`\widehat{s}_2`$ induced by the measurement of $`\widehat{s}_1`$ according to the uncertainty principle. For $`\delta s\mathrm{}`$, the noise introduced in the measurement of $`\widehat{s}_1`$ goes to zero and the correlation is given by the operator expectation values of the initial state. Due to the operator ordering, the anti-correlation between $`s_1^2`$ and $`s_2`$ is an inherent statistical property of $`\psi _{\text{in}}`$ even though $`\psi _{\text{in}}`$ is an eigenstate of $`\widehat{s}_2`$. Thus operator ordering allows a correlation between fluctuating properties and seemingly well defined operator variables of the quantum state.

This property implies that even the eigenvalues of a quantum state do not represent “elements of reality”. Consequently, it is wrong to assign measurement values to physical properties before the measurement even if the measurement result can be predicted with certainty. Since the violation of Bell’s inequalities depends on the assignment of such “elements of reality” it is not surprising that it can be violated by quantum theory. In the following, it will be shown how the violation of Bell’s inequalities can be explained in terms of negative joint probabilities obtained from finite resolution measurements.

## III Measurement of polarization entanglement

### A Entangled photons

Entangled photon pairs can be created in two photon emission  or in parametric down conversion . The precise polarization statistics may vary depending on the geometry of the setup. In order to express the violation of Bell’s inequalities in terms of the Stokes parameters $`\widehat{s}_1`$ and $`\widehat{s}_2`$, it is useful to rotate the polarizations of the two photons in such a way that the quantum state is given by

$$\psi _{a,b}=\frac{1}{\sqrt{2}}\left(R;L+\mathrm{exp}\left(i\frac{\pi }{4}\right)L;R\right).$$
(26)
This state is an eigenstate of two polarization correlations,

$`{\displaystyle \frac{1}{\sqrt{2}}}\left(\widehat{s}_1(a)+\widehat{s}_2(a)\right)\widehat{s}_1(b)\psi _{a,b}`$ $`=`$ $`\psi _{a,b}`$ (27)
$`{\displaystyle \frac{1}{\sqrt{2}}}\left(\widehat{s}_1(a)\widehat{s}_2(a)\right)\widehat{s}_2(b)\psi _{a,b}`$ $`=`$ $`\psi _{a,b}.`$ (28)
The sum of these two eigenvalues violates a Bell’s inequality of the form

$$K=s_1(a)s_1(b)+s_2(a)s_1(b)s_1(a)s_2(b)+s_2(a)s_2(b)2.$$
(29)
It is therefore not possible to interpret the polarization statistics by assigning eigenvalues of $`\pm 1`$ to each Stokes parameter. However, as indicated by the results of finite resolution measurements on the polarization of single photons discussed in section II above, such an identification of physical properties with their eigenvalues is not even consistent with the correlated statistics of local single photon properties. The non-classical statistical properties responsible for the violation of Bell’s inequality (29) can be derived in detail by applying the finite resolution measurement setup introduced above to realize a polarization measurement on the entangled photon pairs given by equation (26).

### B Experimental setup and measurement statistics

Figure 3 shows the experimental setup for a measurement of the correlations in the Bell’s inequality (29). The detector arrays record coincidence counts between the right and left hand side. Each detector array corresponds to an eigenvalue measurement of $`\widehat{s}_2`$. The spatial coordinate at which the photon is registered corresponds to the continuous measurement value $`s_{1m}`$ of $`\widehat{s}_1`$. Each measurement result can then be identified with a point in one of four two dimensional graphs. The probability distribution for the measurement outcomes of the joint measurements may be determined by projections onto the non-orthogonal, non-normalized set of states

$`s_{1m}(a);s_{1m}(b);s_2(a)=\pm 1;s_2(b)=\pm 1=`$ (31)
$`\widehat{P}_{\delta s}(s_{1m}(a))\widehat{P}_{\delta s}(s_{1m}(b)){\displaystyle \frac{1}{2}}\left(R;R+s_2(a)iL;R+s_2(b)iR;Ls_2(a)s_2(b)L;L\right).`$
In their most compact form, the joint probabilities of the measurement results $`s_{1m}(a)`$, $`s_{1m}(b)`$, $`s_2(a)`$, and $`s_2(b)`$ for the entangled input state $`\psi (a,b)`$ given by equation (26) read

$`P(s_{1m}(a);s_{1m}(b);s_2(a)=\pm 1;s_2(b)=\pm 1)=`$ (32)
$`{\displaystyle \frac{\sqrt{2}}{16\pi \delta s^2}}\mathrm{exp}\left({\displaystyle \frac{s_{1m}(a)^2+s_{1m}(b)^2+2}{2\delta s^2}}\right)`$ (36)
$`\times (2\mathrm{sinh}\left({\displaystyle \frac{s_{1m}(a)s_2(b)s_{1m}(b)s_2(a)}{2\delta s^2}}\right)\mathrm{cosh}\left({\displaystyle \frac{s_{1m}(a)s_2(b)+s_{1m}(b)s_2(a)}{2\delta s^2}}\right)`$
$`+\left(\sqrt{2}+s_2(a)s_2(b)\right)\mathrm{cosh}^2\left({\displaystyle \frac{s_{1m}(a)s_2(b)+s_{1m}(b)s_2(a)}{2\delta s^2}}\right)`$
$`+(\sqrt{2}s_2(a)s_2(b))\mathrm{sinh}^2\left({\displaystyle \frac{s_{1m}(a)s_2(b)s_{1m}(b)s_2(a)}{2\delta s^2}}\right)).`$
Figure 4 shows the results for a measurement resolution of $`\delta s=0.6`$. At this intermediate resolution, quantum mechanical interference effects are especially visible . In particular, separate peaks can be resolved clearly, but quantum interference effects are visible in the asymmetric peak shapes and in the zero probability valleys in the $`s_{1m}0`$ regions separating the peaks. As in the single photon case discussed in section II above, it is indeed possible to interpret these features entirely in terms of Gaussian distributions. However, negative probability contributions centered around values of $`s_{1m}=0`$ have to be included in order to explain the asymmetries and the regions of extremely low probabilities near $`s_{1m}=0`$ separating the peaks corresponding to quantized results around $`s_{1m}=\pm 1`$.

### C Violation of Bell’s inequality by the finite resolution measurement statistics

As in the one photon case, the regions of low probability at values of $`s_{1m}(a/b)=0`$ can be traced back to negative joint probabilities. The measurement probabilities given by equation (32) may be expressed as a sum of shifted normalized Gaussian distributions

$$G_{\delta s}(s_{1m}(a)d_a;s_{1m}(b)d_b):=\left(2\pi \delta s^2\right)^1\mathrm{exp}\left(\frac{(s_{1m}(a)^2d_a)^2+(s_{1m}(b)^2d_b)^2}{2\delta s^2}\right).$$
(37)
Since the shifts $`d_a`$ and $`d_b`$ may be $`1`$, $`0`$ or $`+1`$, respectively, each of the four sums has nine components associated with joint probabilities of the four Stokes parameters. The probability distribution of the measurement results is then given by the sum

$`P(s_{1m}(a);s_{1m}(b);s_2(a)=\pm 1;s_2(b)=\pm 1)=`$ (38)
$`{\displaystyle \frac{\sqrt{2}+1}{16\sqrt{2}}}\left(G_{\delta s}(s_{1m}(a)+1;s_{1m}(b)+1)+G_{\delta s}(s_{1m}(a)1;s_{1m}(b)1)\right)`$ (43)
$`+{\displaystyle \frac{\sqrt{2}1}{16\sqrt{2}}}\left(G_{\delta s}(s_{1m}(a)+1;s_{1m}(b)1)+G_{\delta s}(s_{1m}(a)1;s_{1m}(b)+1)\right)`$
$`+\mathrm{exp}\left({\displaystyle \frac{1}{2\delta s^2}}\right){\displaystyle \frac{1}{8\sqrt{2}}}s_2(b)\left(G_{\delta s}(s_{1m}(a)+1;s_{1m}(b))G_{\delta s}(s_{1m}(a)1;s_{1m}(b))\right)`$
$`\mathrm{exp}\left({\displaystyle \frac{1}{2\delta s^2}}\right){\displaystyle \frac{1}{8\sqrt{2}}}s_2(a)\left(G_{\delta s}(s_{1m}(a);s_{1m}(b)+1)G_{\delta s}(s_{1m}(a);s_{1m}(b)1)\right)`$
$`+\mathrm{exp}\left({\displaystyle \frac{1}{\delta s^2}}\right){\displaystyle \frac{1}{4\sqrt{2}}}s_2(a)s_2(b)G_{\delta s}(s_{1m}(a);s_{1m}(b)).`$
Using this decomposition, it is a straightforward matter to determine the averages corresponding to the correlations of the Bell’s inequality (29) by summing over $`s_2(a)`$ and $`s_2(b)`$ and integrating over the continuous results $`s_{1m}(a)`$ and $`s_{1m}(b)`$. The result reads

$$K=\frac{1}{\sqrt{2}}\left(1+\mathrm{exp}\left(\frac{1}{2\delta s^2}\right)\right)^2.$$
(44)
This expectation value exceeds the maximal value of 2 allowed by inequality (29) for measurement resolutions of $`\delta s>1.143`$. The violation of Bell’s inequality can therefore be obtained directly from the measurement statistics for sufficiently low resolutions of the $`\widehat{s}_1`$ measurements. An example for this direct violation of Bell’s inequality is shown in figure 5 for a measurement resolution of $`\delta s=2`$. At this low resolution, quantization effects are not resolved. The non-classical properties of the statistics are observable in the shift of the peak maxima for $`s_2(a)=s_2(b)`$ to values greater than $`s_{1m}=+1`$ or lower than $`s_{1m}=1`$. Specifically, the maximum probability density for $`s_2(a)=+1`$ and $`s_2(b)=1`$ is at $`s_{1m}(a)==s_{1m}(a)=1.383`$ and the maximum for $`s_2(a)=1`$ and $`s_2(b)=+1`$ is at $`s_{1m}(a)==s_{1m}(a)=1.383`$. The value of $`K`$ at these points would be equal to 3.68.

While it might be tempting to interpret the statistics in terms of polarization components greater than $`+1`$ or smaller than $`1`$, the high resolution results of figure 4 and the analysis of single photon polarization in section II suggests that the true reason for the shifted peaks are negative probabilities around $`s_{1m}(a)=s_{1m}(b)=0`$. In order to obtain a consistent interpretation of the measurement results for both high and low resolutions, it is necessary to identify the decoherence factor $`\mathrm{exp}(1/(2\delta s^2))`$ with the quantum noise induced reduction of the expectation values of $`\widehat{s}_2(a)`$ and $`\widehat{s}_2(b)`$. It is then possible to remove the effects of noise and of finite measurement resolution from the measurement statistics, tracing the violation of Bell’s inequality directly to the appearance of negative probabilities in the joint probabilities for $`s_1(a)`$,$`s_2(a)`$,$`s_1(b)`$, and $`s_2(b)`$.

## IV Disentangling entanglement: interpretation of the non-classical statistics

### A Negative conditional probabilities in photon entanglement

As in the case of single photon polarization discussed in section II, the sum of Gaussians given in equation (38) can be interpreted in terms of joint probabilities for $`s_1(a)`$,$`s_2(a)`$,$`s_1(b)`$, and $`s_2(b)`$ by identifying the average of each Gaussian with the appropriate value of $`s_1`$. The joint probabilities for all 36 combinations of the six contributions from $`s_1(a)`$ and $`s_2(a)`$ with the six contributions from $`s_1(b)`$ and $`s_2(b)`$ characterizing the statistics of the entangled state $`\psi _{a,b}`$ are shown in table I. From these probabilities, the statistical weight of different contributions to the sum correlation $`K`$ in inequality (29) can be determined.

The joint probabilities can be classified according to whether the values of $`s_1(a)`$ and $`s_1(b)`$ are zero or not. There are sixteen contributions with both $`s_1(a)`$ and $`s_1(b)`$ non-zero. These cases correspond to the classical expectation that the values of $`s_1`$ should be equal to the eigenvalues observed in high resolution measurements. Consequently, they are the only contributions that are not diminished by the decoherence factor for small $`\delta s`$. Moreover, their probabilities are all positive. In eight of these sixteen cases, three of the four correlations in inequality (29) are equal to $`+1`$ and one is equal to $`1`$, for a total of $`K=2`$. The reverse is true for the remaining eight cases, resulting in a total of $`K=2`$ for the sum of correlations in inequality (29). The probability of each case is equal to $`(2+s_1(a)s_1(b)\sqrt{2})/32`$. Summing up the probability of the eight cases with $`K=2`$ thus results in a total probability of $`(4+\sqrt{2})/8`$ or roughly 67.7 %. The eight cases with $`K=2`$ have a total probability of $`(4\sqrt{2})/8`$, or 32.3 %. The average value of $`K`$ for these “classical” contributions to the joint probability is therefore equal to $`1/\sqrt{2}`$, as evidenced by the limit of equation (44) for $`\delta s0`$. Obviously, the violation of Bell’s inequality must originate from the remaining twenty contributions with at least one value of $`s_1`$ equal to zero.

There are sixteen contributions with one value of $`s_1`$ equal to zero and the other value non-zero. Two of the four correlations in the inequality (29) are then equal to zero, while the other two may be either plus or minus one each. In four cases, they are both equal to plus one ($`K=2`$), in eight cases, they have opposite sign ($`K=0`$), and in the remaining four cases, they are both equal to minus one ($`K=2`$). The probabilities for these cases are $`\pm \sqrt{2}/16`$. As a result, the total probability for the four cases with $`K=2`$ is equal to $`\sqrt{2}/4`$ or 35.4%, the total probabilities for the eight cases with $`K=0`$ cancel to zero, and the total probability for $`K=2`$ is $`\sqrt{2}/4`$ or -35.4%. This negative probability more than outweighs the 32.3 % of the classical contributions, explaining the increase of the expectation value of $`K`$ beyond the limit of 2. However, the effect is further enhanced by the contributions from $`s_1(a)=s_1(b)=0`$.

There are four contributions with $`s_1(a)=s_1(b)=0`$. Only the correlation $`s_2(a)s_2(b)`$ is non-zero in these cases. Two cases have $`K=1`$ and a positive probability of $`\sqrt{2}/8`$, and two cases have $`K=1`$ and a negative probability of $`\sqrt{2}/8`$. This adds a total probability of 35.4 % for $`K=1`$ and -35.4 % for $`K=1`$.

The probability distribution over values of $`K`$ can be summarized as follows:

$`P(K=2)=103.1\%`$ $`P(K=2)=3.1\%`$ (45)
$`P(K=1)=35.4\%`$ $`P(K=1)=35.4\%`$ (46)
$`P(K=0)=0\%.`$ (47)
The high expectation value of $`K`$ is a result of the negative probabilities for combinations of $`s_1(a)`$,$`s_2(a)`$,$`s_1(b)`$, and $`s_2(b)`$ with $`K<0`$. In the measured probability distributions described by equations (32) and (38), these negative probabilities appear as a suppression of the probability for values of $`s_1`$ close to zero, pushing the peak of the probability distribution beyond the eigenvalue limit of $`\pm 1`$. Since $`s_{1m}`$ is not restricted to eigenvalues of $`\widehat{s}_1`$, the contributions to the expectation value of $`K`$ taken from the measured distribution (32) shown in figure 4 may exceed the classical limit. Even though a direct observation of the negative probabilities is of course impossible, the continuous distribution of finite resolution measurement results thus reveals clear evidence of these non-classical statistical features.

### B Quantum noise and negative probabilities in entangled systems

The negative conditional probabilities shown in table I allow an interpretation of the measurement statistics in terms of individual measurement results observed separately in branch $`a`$ and in branch $`b`$. There is neither a need for action at a distance, nor for non-local properties. The non-classical feature required to explain the violation of Bell’s inequalities is expressed in the negative probabilities which are possible even in individual quantum systems because the uncertainty principle does not allow an isolated measurement of a joint probability of non-commuting variables.

Once the relationship between uncertainty and negative conditional probabilities is understood, the problem of non-locality in entangled systems can be resolved by introducing local decompositions of the entangled state density matrix based on negative probability components of the local density matrices. For the state discussed above, one possible decomposition reads

$`\psi _{a,b}\psi _{a,b}`$ $`=`$ $`{\displaystyle \frac{1}{4}}\widehat{1}(a)\widehat{1}(b)+{\displaystyle \frac{1}{4\sqrt{2}}}(\widehat{s}_1(a)+\widehat{s}_2(a))\widehat{s}_1(b)`$ (49)
$`+{\displaystyle \frac{1}{4\sqrt{2}}}(\widehat{s}_1(a)\widehat{s}_2(a))\widehat{s}_2(b){\displaystyle \frac{1}{4}}\widehat{s}_3(a)\widehat{s}_3(b).`$
All by themselves, the Stokes parameter operators $`\widehat{s}_i`$ would not qualify as density matrices because of their negative eigenvalues. Once negative eigenvalue components are permitted, however, the decomposition given above can be interpreted as a separation of the entangled density matrix into products of local density matrices. The reason why density matrices with negative probability eigenvalues may be used in the decomposition of entangled states is that any measurement performed on system $`a`$ mixes contributions to the density matrix of system $`b`$ in such a way that the information required to isolate the negative conditional probabilities represented by the negative eigenvalues is lost.

Effectively, the uncertainty in system $`a`$ necessarily “covers up” the negative eigenvalues of the density matrix components of system $`b`$ by mixing them with positive components. Entanglement can therefore be explained by the local properties of quantum measurements described previously . In the light of this result, it is not surprising that some applications of quantum mechanics such as quantum computation can work without entanglement . The most fundamental property of quantum mechanics is not entanglement, but local non-classical correlations represented by the operator-ordering dependence of expectation values and the negative conditional probabilities obtained from finite resolution measurements.

## V Conclusions

The interpretation of quantum statistics cannot be based on the assumption that potential measurement results represent “elements of reality” whether the actual measurement is performed or not. This is not only true for entangled systems, but also for combinations of finite resolution measurements performed to obtain the correlations between non-commuting operator variables in a single quantum system. As a result, concepts such as photon polarization have to be reviewed critically in order to understand the relationship between eigenvalues and operator variables.

The experimental approach proposed above allows a direct determination of the non-classical features of the polarization statistics for both single photons and entangled pairs. Its application to the violation of Bell’s inequalities reveals details of the statistical relationships between all four polarization components. A full set of conditional probabilities can be obtained from the statistics of a single measurement, revealing the negative conditional probabilities that are responsible for the violation of Bell’s inequalities. A comparison with the single photon polarization statistics reveals that such negative probabilities are also observable in the polarization of a single photon. The property responsible for the violation of Bell’s inequalities is therefore a local feature of quantum statistics. Once the implications of the operator formalism are accepted, entanglement can be understood as a special case of the non-classical features observable in local correlations.

## Acknowledgment

The author would like to acknowledge support from the Japanese Society for the Promotion of Science, JSPS, and thank Dr. Takao Fuji for helpful discussions of the experimental aspects.


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# Inversionless gain in a three-level system driven by a strong field and collisions 1footnote 11footnote 1Project supported in part by the Russian Fundation for Basic Research (Grant No.96-02-00010c), by the National Sciences Foundation of China (Grant No. 19911121500) and the Science and Technology Foundation of Jilin Province, China (Grant No. 980526).

## I  Introduction

Light amplification without population inversion (AWI) has been studied in a number of theoretical and experimental papers po  \- mes  because of its potential application in producing high-power lasers in the regions of electromagnetic spectrum which are difficult to reach with traditional laser system. Although population inversion between the laser levels is not necessary in inversionless light amplification system, it is required to pump a fraction of population to the upper level incoherently. Possible AWI at the transitions between excited states of noble gases, pumped by discharge, was shown in po ; am . The incoherent pump by discharge may not always provide necessary population, and the direct excitation by laser with broad linewidth may introduce additional atomic coherence. Another approach to possible AWI assisted by the collisional population transfer between fine structure levels of alkali atoms was proposed in cr ; fl ; wod  and based on successful experiments atu ; mov  proved that wide range manipulation by population of the levels (up to population inversion) can be provided with this mechanism. Successful experiments on AWI in potassium vapors based on such mechanism were reported in str . (The theory and estimates for sodium atoms, underlying cr ; fl ; wod  were presented in wel ; izv  too). Hyperfine structure of D-lines in alkalies and degeneracy of the coupled levels require multilevel model in order to consider complex of quantum nonlinear coherence and interference effects, which are origin of AWI. However experiments with sodium gu  and potassium str  atoms showed, that major behavior and requirements for AWI (especially at detuning of the driving field from the resonance) may be studied with the aid of simple three-level V-configuration. In this paper, the mechanism of incoherent pump by a strong laser beam and collisional population transfer induced by buffer gas pressure is further analyzed. In order to fit better experimental conditions degeneracy are taken into account. We derived simple and explicit formulae, describing process. With the aid of these expressions we compare various alkalies and buffer gases in order to show that strong competition between population transfer and loss of coherence may be optimize by the proper choice of the transitions and buffer gases. The idea developed here for incoherent pump could be generalized to other systems.

## II Theoretical model and equations

We consider a model as shown in Fig.1 which consists of three levels labeled $`|1`$, $`|2`$ and $`|3`$. A strong driving field with frequency $`\omega `$ produces coherent coupling between levels $`|1`$ and $`|2`$, while the weak probe field with frequency $`\omega _p`$ is scanned around the transition between levels $`|3`$ and $`|1`$. We express the probe and driving fields in the form:

$`E_p(t)`$ $`=`$ $`{\displaystyle \frac{1}{2}}[E_{p0}e^{i\omega _pt}+c.c.]`$ (1)
$`E(t)`$ $`=`$ $`{\displaystyle \frac{1}{2}}[E_0e^{i\omega t}+c.c.]`$ (2)
where $`E_{p0}`$ and $`E_0`$ are the complex amplitudes. The Hamiltonian of the system including the interaction between the atom and the two fields can be written as:

$`H`$ $`=`$ $`H_a+H_b`$
$`H_a`$ $`=`$ $`\mathrm{}\omega _pa_3^+a_3+\mathrm{}\omega a_2^+a_2`$ (3)
$`H_b`$ $`=`$ $`\mathrm{}\delta _pa_3^+a_3\mathrm{}\delta a_2^+a_2\mathrm{}[g_pa_3^+a_1e^{i\omega _pt}+ga_2^+a_1e^{i\omega t}+c.c.],`$
where $`\delta _p=\omega _p\omega _{31}`$, $`\delta =\omega \omega _{21}`$; $`\omega _{31}`$ and $`\omega _{21}`$ denote the transition frequencies from $`|3`$ to $`|1`$ and $`|2`$ to $`|1`$, respectively; $`g=\mu _{21}E_0/2\mathrm{}`$, $`g_p=\mu _{31}E_{p0}/2\mathrm{}`$ are the Rabi frequencies of the probe and the driving fields, respectively; $`\mu _{31}`$ and $`\mu _{21}`$ are the dipole matrix elements of optical transitions from $`|3`$ to $`|1`$ and $`|2`$ to $`|1`$, respectively. In the interaction picture, the master equation for density operator is

$`{\displaystyle \frac{dr}{dt}}={\displaystyle \frac{i}{\mathrm{}}}[\stackrel{~}{H_b},r]+\text{incoherent term},`$ (4)
where $`r=e^{iH_at/\mathrm{}}\rho e^{iH_at/\mathrm{}}`$, $`\stackrel{~}{H}_b=e^{iH_at/\mathrm{}}H_be^{iH_at/\mathrm{}}`$. According to the equation (4), the matrix elements of density operator can be expressed as follows:

$`{\displaystyle \frac{dr_{31}}{dt}}=ig_p(r_1r_3)(\mathrm{\Gamma }_{31}i\delta _p)r_{31}igr_{32}`$
$`{\displaystyle \frac{dr_{32}}{dt}}=igr_{21}^{}ig^{}r_{31}[\mathrm{\Gamma }_{23}i(\delta _p\delta )]r_{32}`$
$`{\displaystyle \frac{dr_{21}}{dt}}=ig(r_1r_2)(\mathrm{\Gamma }_{21}i\delta )r_{21}ig_pr_{32}^{}`$ (5)
$`{\displaystyle \frac{dr_3}{dt}}=2Im(g_p^{}r_{31})\mathrm{\Gamma }_3r_3+w_{23}r_2`$
$`{\displaystyle \frac{dr_2}{dt}}=2Im(g^{}r_{21})\mathrm{\Gamma }_2r_2+w_{32}r_3`$
$`r_1+r_2+r_3=1.`$ (6)
Here $`r_{ij}=r_{ji}^{}`$, $`r_{ii}=r_i`$, $`\mathrm{\Gamma }_2=A_{21}+w_{23}`$, $`\mathrm{\Gamma }_3=A_{31}+w_{32}`$, where $`A_{21}`$ and $`A_{31}`$ are the decay rates of populations in levels $`|2`$ and $`|3`$ to the ground state $`|1`$ due to the common spontaneous transition, respectively; $`w_{23}`$ and $`w_{32}`$ are the collision transfer relaxation rates of the populations in level $`|2`$ to level $`|3`$ and in level $`|3`$ to level $`|2`$ due to collision; $`\mathrm{\Gamma }_{21}`$, $`\mathrm{\Gamma }_{31}`$, $`\mathrm{\Gamma }_{23}`$ — are the polarization decay rates between levels $`|1`$ and $`|2`$, levels $`|3`$ and $`|1`$, levels $`|3`$ and $`|2`$, respectively ($`\mathrm{\Gamma }_{ij}=\mathrm{\Gamma }_{ji}`$).

Absorption and refractive indices at the frequency $`\omega _p`$ are determined by the complex susceptibility $`\chi (\omega _p)`$ which is proportional to the off-diagonal element $`r_{31}`$: $`\chi (\omega _p)=(r_{31}\mu _{13})/(E_p/2).`$ In the liner approximation of probe field, the steady state solution of equations (5) for $`r_{31}`$ is:

$`r_{31}=i{\displaystyle \frac{g_p(r_1r_3)gr_{32}}{\mathrm{\Gamma }_{31}i\delta _p}}`$ (7)
The coherence $`r_{32}`$ itself is dependent on $`r_{31}`$ and $`r_{21}`$. By substituting solution for $`r_{32}`$ to equation(7) one obtains:

$`{\displaystyle \frac{\chi }{\chi _0}}=f(\delta _p)=i\mathrm{\Gamma }_{31}{\displaystyle \frac{[\mathrm{\Gamma }_{23}i(\delta _p\delta )](r_1r_3)igr_{21}^{}}{[\mathrm{\Gamma }_{23}i(\delta _p\delta )](\mathrm{\Gamma }_{31}i\delta _p)+|g|^2}},`$ (8)
where

$$r_{21}=ig(r_1r_2)/(\mathrm{\Gamma }_{21}i\delta ).$$
(9)
Eventually from (8),(9) we obtain:

$`f(\delta _p)=i\mathrm{\Gamma }_{31}{\displaystyle \frac{[\mathrm{\Gamma }_{23}i(\delta _p\delta )](r_1r_3)|g|^2(r_1r_2)/(\mathrm{\Gamma }_{21}+i\delta )}{[\mathrm{\Gamma }_{23}i(\delta _p\delta )](\mathrm{\Gamma }_{31}i\delta _p)+|g|^2}},`$ (10)
$`\alpha _p/\alpha _{p0}=Imf(\delta _p),(n_p1)/(n_{pmax}1)=Ref(\delta _p)`$
## III  Mechanism of power and collision driven $`AWI`$

Optimum conditions for $`AWI`$ in three-level $`V`$ configuration, assuming possible manipulating by populations of the coupled levels with incoherent pump were analyzed in po . Classification of the effects of a strong field on the spectral line shape at an adjacent transition for various $`V`$, $`\mathrm{\Lambda }`$ and $`H`$ configurations of coupled transitions was given in po ; sok  (see also rus (e),he ): dependencies of $`r_{i,j}`$ and of the denominator in (8) on $`g`$ refer to saturation of populations and energy-level splitting effects, correspondingly; $`r_{21}`$– represents nonlinear interference effects ($`NIEF`$). As it was shown in sok ,rus (e) NIEF bring about change of a line shape but not an integral intensity:

$$𝑑\delta _pf(\delta _p,|E|^2)=\pi \mathrm{\Gamma }_{31}(r_1r_3),$$
(11)
which depends only on saturation effects.

Indeed, NIEF represent the origin of sign-changing spectral line shapes and AWI at the probe transition. One can regard (8) as the difference between acts of pure emission (associated with the $`r_3`$, assuming $`r_1=r_2=0`$), and pure absorption (the rest terms). Both of them are positive but depend in a different way on detunings, because of NIEF. This was emphasized in sok  (see also rus (e),po ; he ).

Thus, in the schematic under consideration $`AWI`$ originates from the coherence at the transition $`|3|2`$, induced by the strong field, coupled to the auxiliary level $`|2`$ in combination with the probe field, which consequently gives rise to factor $`r_{21}`$ in (8). The larger is maximum value of $`r_{21}`$ compared to $`r_1r_3`$ the more pronounced is the effect of $`AWI`$. At $`\delta =0,`$ maximum of absorption (gain) corresponds to $`\delta _p=0.`$

$`f(0)={\displaystyle \frac{(r_1r_3)(r_1r_2)S}{1+S}},`$ (12)
where $`S=|g|^2/\mathrm{\Gamma }_{21}\mathrm{\Gamma }_{32}`$. Therefore, even at $`(r_1r_3)>0`$, $`(r_1r_2)>0,`$ negative absorption (gain) occurs if

$`(r_1r_2)S>r_1r_3.`$ (13)
The less is coherence decay rate $`\mathrm{\Gamma }_{32}`$ at the two-photon transition $`|3|2`$, compared to that at the coupled one-photon transitions, the more favorable are the conditions for AWI. At $`S>1`$ large splitting of the level $`|1`$ on two quasi levels significantly reduces interference and, therefore, the magnitude of AWI at the center of the transition $`|3|1`$. Optimal value of strength of driving field for $`AWI`$ in the probe line center was analyzed in po .

Below we shall consider opportunities and specific experimental schematic to control shape of absorption and refraction indexes without external incoherent pump. Necessary for $`AWI`$ distribution of populations is ensured by collisions.

Consider alkali atoms, immersed into buffer gas. Strong field couples $`P_{3/2}`$ and ground $`S`$ levels. Fast collision exchange ensures population transfer from the $`P_{3/2}`$ to the lower $`P_{1/2}`$ level. In order to understand main mechanism giving rise to $`AWI`$, suppose for simplicity, that pressure of the buffer gas is so strong, that Boltzmann population distribution between the fine structure levels is established. This brings about the means to control population difference at the probe transition in a wide range by increasing intensity of the strong field. Even population inversion at the $`P_{1/2}S`$ transition can be provided due to the saturation effect at $`P_{3/2}S`$ transition (similar to that in Ruby laser). Such a feasibility to produce population inversion at the transition $`P_{1/2}S`$ has been demonstrated experimentally for potassium mov  and sodium atu  vapors admixed to helium at about atmospheric pressure. Possible $`AWI`$, the required driving field strength and buffer gas pressure can be estimated as follows. One can find from the equation system (6):

$$r_2=\frac{\mathrm{\Gamma }_3}{2\mathrm{\Gamma }_3+w_{23}}\frac{\text{æ}^{}}{1+\text{æ}^{}},r_3=\frac{w_{23}}{\mathrm{\Gamma }_3}r_2,r_1=(1+\frac{\mathrm{\Gamma }_3\text{æ}^{}}{2\mathrm{\Gamma }_3+w_{23}})\frac{1}{1+\text{æ}^{}};$$
(14)
$$r_1r_2=\frac{1}{1+\text{æ}^{}},r_1r_3=(1+\frac{\mathrm{\Gamma }_3w_{23}}{2\mathrm{\Gamma }_3+w_{23}}\text{æ}^{})\frac{1}{1+\text{æ}^{}}.$$
(15)
Here

$`\text{æ}^{}={\displaystyle \frac{2+(w_{23}/\mathrm{\Gamma }_3)}{[1(w_{32}w_{23}/\mathrm{\Gamma }_3\mathrm{\Gamma }_2)}}\text{æ},`$ (16)
$`\text{æ}=2\mathrm{\Gamma }|g|^2/\mathrm{\Gamma }_2(\mathrm{\Gamma }^2+\delta ^2)`$ (17)
Consider high pressure limit, assuming that $`A_{31}A_{21}`$, and the buffer gas pressure is so high, that $`(w_{23}w_{32})>>A_{31},A_{21}`$. Then taking into account that in the given conditions $`w_{32}=w_{23}\mathrm{exp}(\mathrm{\Delta }E/k_BT)`$, where $`\mathrm{\Delta }E=E_2E_3`$ is the fine splitting energy, $`k_B`$ and $`T`$ are Boltzmann’s constant and temperature, we obtain:

$`r_1r_3=\left[1\text{æ}^{}{\displaystyle \frac{1\mathrm{exp}(\mathrm{\Delta }E/k_BT)}{1+2\mathrm{exp}(\mathrm{\Delta }E/k_BT)}}\right]{\displaystyle \frac{1}{1+\text{æ}^{}}};`$ (18)
$`\text{æ}^{}={\displaystyle \frac{1+2\mathrm{exp}(\mathrm{\Delta }E/k_BT)}{1+\mathrm{exp}(\mathrm{\Delta }E/k_BT)}}{\displaystyle \frac{2|g|^2\mathrm{\Gamma }_{21}/A_{21}}{\mathrm{\Gamma }_{21}^2+\delta ^2}}.`$ (19)
For sodium $`\mathrm{\Delta }E=17.2\text{cm}\text{-1}\text{ and at }T=550K`$ the estimates give

$$\mathrm{\Delta }E/k_BT=4.310^2,\text{æ}^{}3|g|^2/\mathrm{\Gamma }\mathrm{\Gamma }_29\lambda ^3I/64\pi ^3ϵ_0\mathrm{}c\mathrm{\Gamma }_{21},$$

$$r_1r_3\frac{1}{1+\text{æ}^{}}[11.310^2\text{æ}^{}]$$
(20)
Here $`\lambda `$ and I are strong field wavelength and energy flux density, $`ϵ_0`$ is primitivity of free space. From the equations (12),(18),(19) one can see that the potentially attainable AWI grows with the increase of $`\mathrm{\Delta }E`$ (for example, in $`K`$ and $`Rb)`$. But on the other hand with the increase of fine splitting population transferring collision crossection decreases. That must be compensated with increase of buffer gas pressure. Later brings loss of coherence. These dependencies will be investigated numerically in the next section.

Inelastic collision crossection of sodium and helium for the transition $`3P_{3/2}3P_{1/2}`$ is $`\sigma _{23}410^{15}`$ cm2 11 . For T= 550K and atmospheric pressure of helium we estimate $`w_{23}=N_{He}\overline{v}\sigma _{23}7.510^9`$ sec-1. Since $`A_{31}A_{21}6.210^7`$ sec-1, requirements for the approximations (18),(19) are met. Taking the data of ref.12  for the collision broadening of sodium $`D`$ lines by helium, we estimate collision halfwidth as $`\mathrm{\Gamma }_{21}510^{10}`$ sec-1, which exceeds measured Doppler halfwidth of this transition $`\mathrm{\Delta }\omega _D/2=4.710^9`$ sec-1 $`(\mathrm{\Delta }\nu _D/2=0.75`$ GHz). So we can neglect inhomogeneous broadening of the transition.

For the conditions under consideration we estimate $`\text{æ}^{}510^9I`$ (where I is in W/cm2), $`|g|^2/\mathrm{\Gamma }_{21}\mathrm{\Gamma }_{32}|g|^2/\mathrm{\Gamma }_{31}\mathrm{\Gamma }_{32}\text{æ}^{}\mathrm{\Gamma }_2/3\mathrm{\Gamma }_{32}`$. For the laser power $`0.1`$ W focused to the spot $`A=10^5\text{cm}\text{2}`$ (confocal parameter $`b1`$ cm) we obtain $`|g|3.6`$ GHz, $`\text{æ}^{}510^2`$, $`|g|^2/\mathrm{\Gamma }_{21}\mathrm{\Gamma }_{32}0.1`$. These magnitudes are about optimal ones and correspond to the estimated values, required to vary population difference at the probe transition $`r_1r_3`$ around zero. Above presented estimates for the intensity $`(110)\text{kW/cm}\text{2}`$, required to achieve appreciated change of the line shape under the conditions considered, compares well with the experimental data obtained for the significant change of the ratio of population differences at the coupled transitions at the similar conditions atu .

The magnitude of AWI at $`r_1r_3=0`$ is estimated as $`\alpha _p(0)/\alpha _{p0}\mathrm{\Gamma }_2/3\mathrm{\Gamma }_{32}`$. Assuming $`\mathrm{\Gamma }_{32}w_{23}`$, it may yield about $`0.3\%`$ of the absorption in the absence of the strong field. It is seen that this quantity is very sensitive to the decay rate of the coherence at the Raman-like transition $`|3|2`$.

## IV  Numerical analysis of power and collision induced AWI at the transition between degenerate levels of alkalies

We shall consider such frequency detunings and collision broadening of the transitions, that hyperfine splitting of the levels can be neglected. However, account for degenerating of the levels may occur important for the quantitative analysis of the optimum conditions for $`AWI`$.

Assume that both driving and probe fields are linear and in the same way polarized. Then we assume that collisions can transfer only populations but not coherence. By that we can consider equations (5) for off-diagonal elements of density matrix as referred to the transitions between the same Zeeman sublevels of the upper and lower energy levels, which are not coupled. Unlike that equations for populations of the sublevels are coupled by the collisions. We assume that collisions are so strong, that populations of all sublevels within a same level are equal. Consequently we shall consider populations of any sublevel $`r_{iM}`$ and of the level $`R_i`$ to be related as $`r_{iM}=R_i/g_i`$, where $`g_i`$ is degenerating factor of the level. Equations for the populations take the form:

$`R_2=({\displaystyle \frac{g_2}{g_1}}R_1R_2)\text{æ}+R_3{\displaystyle \frac{w_{32}}{\mathrm{\Gamma }_2}};R_3=R_2{\displaystyle \frac{w_{23}}{\mathrm{\Gamma }_3}};R_1+R_2+R_3=1,`$ (21)
where æ is given by (17). Solution of (21) is:

$`R_2={\displaystyle \frac{g_2/g_1}{1+(g_2/g_1)[1+(w_{23}/\mathrm{\Gamma }_3)]}}{\displaystyle \frac{\text{æ}^{}}{1+\text{æ}^{}}};R_3=R_2{\displaystyle \frac{w_{23}}{\mathrm{\Gamma }_3}};`$
$`R_1=\left[1+{\displaystyle \frac{\text{æ}^{}}{1+(g_2/g_1)[1+(w_{23}/\mathrm{\Gamma }_3)]}}\right]{\displaystyle \frac{1}{1+\text{æ}^{}}},`$ (22)
$`{\displaystyle \frac{R_1}{g_1}}{\displaystyle \frac{R_2}{g_2}}={\displaystyle \frac{1}{g_1}}{\displaystyle \frac{1}{1+\text{æ}^{}}},`$ (23)
$`{\displaystyle \frac{R_1}{g_1}}{\displaystyle \frac{R_3}{g_3}}={\displaystyle \frac{1}{g_1}}\left\{1+{\displaystyle \frac{[1(g_2w_{23}/g_3\mathrm{\Gamma }_3)]\text{æ}^{}}{1+(g_2/g_1)[1+(w_{23}/\mathrm{\Gamma }_3)]}}\right\}{\displaystyle \frac{1}{1+\text{æ}^{}}}.`$ (24)
It is seen from (24) that population inversion at the probe transition is impossible until buffer gas number density $`N_b`$ meets requirement:

$$N_bv(g_2\sigma _{23}g_3\sigma _{32})<g_3A_{31}$$
(25)
Here $`v`$ and $`\sigma _{ij}`$ are averaged relative collision velocity and fine structure population transfer crossections with the buffer atom.

For numerical analysis we use data presented in Table 1 (with $`He`$ as buffer gas).

Fig.2 (curves a) shows dependence of threshold value of the saturation parameter $`\text{æ}_0`$, required for population inversion to be achieved, on the buffer gas pressure above this limit (equation $`(R_1/g_1)(R_3/g_3)=0`$). Curves b show dependence of threshold value of the saturation parameter $`\text{æ}_0`$, required in order to achieve inversion of sign of $`\alpha _p`$ ($`AWI`$), on the buffer gas pressure (equation $`[(R_1/g_1)(R_3/g_3)][(R_1/g_1)(R_2/g_2)]S=0`$). Both dependencies are drown for atoms at $`v=0`$ and at $`\delta =\delta _p=0`$. $`\text{æ}_0`$ is resonant value for saturation parameter at collisionless limit ($`\text{æ}_0=4|g|^2/A_{21}^2`$). In the range between curves (a) and (b) change of sign of $`\alpha _p`$ occurs without changing of sign of population difference $`(R_1/g_1)(R_3/g_3)`$. Minimum value of the saturation parameter $`\text{æ}_0`$, required in order to achieve AWI is $`\text{æ}_0=92`$ ($`P_b3.1`$Torr), $`\text{æ}_0=848`$ ($`P_b12.4`$Torr) and $`\text{æ}_0=4971`$ ($`P_b640.5`$Torr) for $`K`$, $`Na`$ and $`Rb`$ respectively. Such values of the saturation parameter lead to considerable change of level populations which becomes $`R_1=0.28`$, $`R_2=0.5`$, $`R_3=0.22`$ for $`K`$, $`R_1=0.264`$, $`R_2=0.51`$, $`R_3=0.226`$ for $`Na`$ and $`R_1=0.324`$, $`R_2=0.462`$, $`R_3=0.214`$ for $`Rb`$.

One can manipulate the shape of the absorption/gain spectral line, position and bandwidth of the absorption and gain frequency-intervals. Analysis is given in ref. po . Line shape is quite sensitive to the intensity and frequency detunings of the strong field from the resonance. Bandwidth of the gain grows and the maximum value decreases with the increase of the intensity of the strong field above a certain magnitude. Saturation of the population difference at the strong field transition and splitting of the common energy level oppose AWI effect, so that it can be optimize by the proper choice of intensity and detunings of the strong field. In the case under consideration inelastic collision frequency is important parameter to be optimized as well.

Fig.3 demonstrate dependencies of absorption/gain of probe field at frequency $`\omega _p`$ vs scaled detuning $`\delta _p/\mathrm{\Gamma }_{31}`$ ($`\delta =0`$) under optimal values of the buffer gas pressure and of the driving field intensity. Maximum values of the AWI index are: $`\alpha _p=0.002`$ for $`Na`$ ($`\text{æ}_0=8700,P=170`$ Torr); $`\alpha _p=0.01`$ for $`K`$ ($`\text{æ}_0=370,P=16`$ Torr) and $`\alpha _p=1.310^4`$ for $`Rb`$ ($`\text{æ}_0=12300,P=1800`$ Torr). Corresponding population differences $`(R_1/g_1)(R_3/g_3)`$ are $`210^5`$, $`310^4`$ and $`1.210^4`$.

Taking the data of ref.lew  for the collision broadening of $`D`$ lines by helium, we estimate collision halfwidth as $`\mathrm{\Gamma }_{21}8.810^9`$ sec-1, $`\mathrm{\Gamma }_{21}0.7310^9`$ sec-1 and $`\mathrm{\Gamma }_{21}79.810^9`$ sec-1 for $`Na`$, $`K`$ and $`Rb`$ respectively, which exceeds measured Doppler halfwidth of this transition for $`Na`$ ($`\mathrm{\Delta }\omega _D/2=5.610^9`$ sec-1) and $`Rb`$ ($`\mathrm{\Delta }\omega _D/2=2.1510^9`$ sec-1). So in this case we can neglect inhomogeneous broadening of the transition. But in the case of $`K`$ $`\mathrm{\Gamma }_{21}\mathrm{\Delta }\omega _D/2=3.110^9`$ and it is necessary to perform averaging over velocities of atoms.

Fig.4 shows velocity-averaged absorption indices (for $`K`$) at inhomogeneously broadened $`|1|3`$ transition in the presence of strong field at $`|1|2`$ transition (1 — $`\text{æ}_0=3400`$, $`\delta =0`$, 2 — $`\text{æ}_0=610^4`$, $`\delta =3\mathrm{\Delta }\omega _D/2`$).

The shape of the refraction index (dispersion) is described by the $`Ref(\delta _p,|E|^2)`$. In the scope of the discussed experiment one can manipulate by the shape of both absorption (gain) and refraction indexes so, that maxima and minima of the refraction would fall to the spectrum range of the near vanishing absorption.

In summary, this work considers a model of interference and collision driven $`V`$ – type three degenerate-level system which, provides gain without population inversion and resonance-enhanced refraction at vanishing absorption. Explicit formulas for analyzing of the optimal conditions are presented. Comparative analysis of use of various alkalies relative to potential experiment is qualitatively discussed in details. Coherence destroying collision decrease the AWI and ERWA effects compared to that in atomic beams. However the decrease may be comparable to that due to the Doppler broadening in metal vapors. The advantages are simplicity of the experiment, feasibilities to manipulate the population differences at the coupled transitions and to avoid some side effects. These make the experiment conformable to the simple common accepted theoretical model.


text:
# Semi-classical theory of magnetic quantum oscillations in a two-dimensional multiband canonical Fermi liquid.

\[

## Abstract

The semi-classical Lifshitz-Kosevich (LK) description of quantum oscillations is extended to a multiband two-dimensional Fermi liquid with a constant number of electrons. The amplitudes of novel oscillations with combination frequencies, recently predicted and observed experimentally, are analytically derived and compared with the single-band amplitudes. The combination amplitudes decay with temperature exponentially faster than the standard harmonics, and this provides a valuable tool for their experimental identification.

\]

It has been shown  that the magnetic quantum oscillations in a multiband $`2D`$ metal with a fixed electron density (canonical ensemble ($`CE`$)) are qualitatively different from those in an open system where the chemical potential is fixed (grand canonical ensemble ($`GCE`$)). There is a mechanism for different bands to ’talk’ to each other in $`CE`$ producing a dHvA signal with the combination frequencies, $`f=f_1+f_2`$  and $`f=f_1f_2`$ in addition to the ordinary dHvA frequencies, $`f_{1,2}`$, of the individual bands in $`GCE.`$ Numerical studies of novel oscillations showed that their amplitudes are comparable with the standard components, and they are robust with respect to a background (non-quantized) density of states .

The novel frequencies have been recently observed  in quantum well structures. These additional components in the dHvA frequency spectrum of low-dimensional metals may provide a unique information on the Fermi surface and carrier density if detailed analytical theory is available. In this paper we develop such a theory in the framework of the semiclassical LK approach . The equations (12) and (14) are the main results of the present paper.

We first derive a convenient expression for a multiband two-dimensional thermodynamic potential in an external magnetic field $`H`$,

$$\mathrm{\Omega }=T𝑑ϵN(ϵ,B)\mathrm{ln}\left[1+\mathrm{exp}\left(\frac{\mu ϵ}{T}\right)\right]$$
(1)
where

$$N(ϵ,B)=\underset{\alpha }{}\underset{n=0}{\overset{\mathrm{}}{}}\rho _\alpha \omega _\alpha \delta (ϵϵ_{\alpha n})$$
(2)
is the quantized density of states, $`\rho _\alpha `$ is the zero-field density of states in the band $`\alpha `$, $`ϵ_{\alpha n}=\mathrm{\Delta }_{\alpha 0}+\omega _\alpha (n+1/2)+g_\alpha \sigma \mu _BB`$, $`\omega _\alpha =eB/m_\alpha `$ the cyclotron frequency with the cyclotron mass $`m_\alpha `$, $`B=H+4\pi M`$ the magnetic field, $`\mathrm{\Delta }_{\alpha 0}`$ the band edge in zero magnetic field, $`\mu `$ the chemical potential, $`g_\alpha `$ the electron $`g`$-factor, $`\sigma =\pm 1/2`$, $`\mu _B`$ the Bohr magneton, and $`\mathrm{}=c=k_B=1`$. The band index $`\alpha `$ includes the electron spin. In actual experiments on 2DEG $`BH`$ and magnetic coupling between subbands was negligible.

By applying the Poisson formula  to the sum over $`n`$ in the thermodynamic potential

$$\mathrm{\Omega }=T\underset{\alpha }{}\rho _\alpha \omega _\alpha \underset{n=0}{\overset{\mathrm{}}{}}\mathrm{ln}\left[1+\mathrm{exp}\left(\frac{\mu _\alpha \omega _\alpha (n+1/2)}{T}\right)\right]$$
(3)
with $`\mu _\alpha =\mu \mathrm{\Delta }_\alpha `$ and $`\mathrm{\Delta }_\alpha =\mathrm{\Delta }_{\alpha 0}+g_\alpha \sigma \mu _BB`$, we obtain

$$\mathrm{\Omega }=\mathrm{\Omega }_0+\stackrel{~}{\mathrm{\Omega }},$$
(4)
where

$$\mathrm{\Omega }_0=T_0^{\mathrm{}}𝑑ϵ\underset{\alpha }{}\rho _\alpha \mathrm{ln}\left[1+\mathrm{exp}\left(\frac{\mu _\alpha ϵ}{T}\right)\right]$$
(5)
is the ’classical’ part. In $`GCE`$ it does not oscillate as a function of $`1/B`$, and contains the contribution due to spin susceptibility (Pauli paramagnetism). The second part is

$$\stackrel{~}{\mathrm{\Omega }}=\frac{1}{24}\underset{\alpha }{}\rho _\alpha \omega _\alpha ^2+2\underset{\alpha }{}\underset{r=1}{\overset{\mathrm{}}{}}A_\alpha ^r\mathrm{cos}\left(\frac{rf_\alpha }{B}+\varphi _\alpha ^r\right),$$
(6)
where the first term produces the Landau diamagnetism and the second oscillatory term is responsible for the de Haas-van Alphen effect. It is small compared with the ’classical’ part as $`\stackrel{~}{\mathrm{\Omega }}/\mathrm{\Omega }_0(\omega /\mu )^2`$. The Fourier components appear with frequencies $`rf_\alpha rS_\alpha /e`$, where $`S_\alpha =2\pi m_\alpha (\mu \mathrm{\Delta }_{\alpha 0})`$ is the Fermi surface zero-field cross-section. The amplitudes of the Fourier harmonics are

$$A_\alpha ^r=\frac{T\rho _\alpha \omega _\alpha }{2r\mathrm{sinh}(2\pi ^2rT/\omega _\alpha )},$$
(7)
and the phase $`\varphi _\alpha ^r=r\pi (1+g_\alpha \sigma )`$.

Differently from $`GCE`$, the chemical potential oscillates in $`CE`$. Hence, the ’classical’ part of $`\mathrm{\Omega }`$ contributes to oscillations as well. The relevant thermodynamic potential of $`CE`$ is the free energy $`F=\mathrm{\Omega }+\mu N`$, with a fixed number of electrons, $`N=\mathrm{\Omega }/\mu `$. At low temperatures we find

$$\mathrm{\Omega }_0=\underset{\alpha }{}\rho _\alpha \mu _\alpha ^2/2,$$
(8)
so that

$$\mu =\frac{1}{\rho }\left(N+\underset{\alpha }{}\rho _\alpha \mathrm{\Delta }_\alpha +\frac{\stackrel{~}{\mathrm{\Omega }}}{\mu }\right),$$
(9)
where $`\rho =_\alpha \rho _\alpha `$ is the total density of states. Substituting this expression into $`\mathrm{\Omega }_0`$, Eq.(8), we obtain

$$F=F_0+\stackrel{~}{F},$$
(10)
where the smooth non-oscillatory part of the free energy is given by

$$F_0=\frac{1}{2\rho }\left(N+\underset{\alpha }{}\rho _\alpha \mathrm{\Delta }_\alpha \right)^2\frac{1}{2}\underset{\alpha }{}\rho _\alpha \mathrm{\Delta }_\alpha ^2,$$
(11)
while the most essential oscillatory part is

$$\stackrel{~}{F}=\stackrel{~}{\mathrm{\Omega }}\frac{1}{2\rho }\left(\frac{\stackrel{~}{\mathrm{\Omega }}}{\mu }\right)^2.$$
(12)
In a more explicit form we obtain

$`\stackrel{~}{F}`$ $`=`$ $`{\displaystyle \frac{1}{24}}{\displaystyle \underset{\alpha }{}}\rho _\alpha \omega _\alpha ^2+2{\displaystyle \underset{\alpha ,r}{}}A_\alpha ^r\mathrm{cos}\left({\displaystyle \frac{rf_\alpha }{B}}+\varphi _\alpha ^r\right)`$ (13)
$``$ $`4{\displaystyle \underset{\alpha ,\alpha ^{},r,r^{}}{}}C_{\alpha \alpha ^{}}^{rr^{}}\mathrm{sin}\left({\displaystyle \frac{rf_\alpha }{B}}+\varphi _\alpha ^r\right)\mathrm{sin}\left({\displaystyle \frac{r^{}f_\alpha ^{}}{B}}+\varphi _\alpha ^{}^r^{}\right).`$ (14)
It is the last term, which yields combination Fourier harmonics with the combination frequencies $`f=rf_\alpha \pm r^{}f_\alpha ^{}`$. Their amplitudes,

$$C_{\alpha \alpha ^{}}^{rr^{}}=2\pi ^2\frac{rr^{}A_\alpha ^rA_\alpha ^{}^r^{}}{\rho \omega _\alpha \omega _\alpha ^{}}$$
(15)
are comparable with the standard single-band harmonics at low temperatures, $`T<\omega _\alpha /2\pi ^2r`$, as also found in the numerical analysis  and in the experiment . For example, the ratio of the combination amplitude to a single-band one for $`r=r^{}=1`$ and $`T=0`$ in a metal with two parabolic bands ($`\rho _\alpha =m_\alpha /2\pi `$) is

$$\frac{2C_{\alpha \alpha ^{}}^{11}}{A_\alpha ^1}=\frac{m_\alpha }{m_\alpha +m_\alpha ^{}}.$$
(16)
Differentiating $`\stackrel{~}{\mathrm{\Omega }}`$ in $`GCE`$ and $`\stackrel{~}{F}`$ in $`CE`$ with respect to $`H`$ one obtains the ratio of the combination and single band amplitudes of magnetization as

$$\frac{M_{\alpha \alpha ^{}}^{11}}{M_\alpha ^1}=\frac{2C_{\alpha \alpha ^{}}^{11}}{A_\alpha ^1}\frac{f}{f_\alpha }=\frac{m_\alpha }{m_\alpha +m_\alpha ^{}}\frac{f}{f_\alpha },$$
(17)
Differentiating twice the ratio in susceptibility is ($`T=0`$)

$$\frac{\chi _{\alpha \alpha ^{}}^{11}}{\chi _\alpha ^1}=\frac{2C_{\alpha \alpha ^{}}^{11}}{A_\alpha ^1}\left(\frac{f}{f_\alpha }\right)^2=\frac{m_\alpha }{m_\alpha +m_\alpha ^{}}\left(\frac{f}{f_\alpha }\right)^2.$$
(18)
Last two ratios may be even larger than unity for the ’plus’ combination harmonic ($`f=f_\alpha ^{}+f_\alpha `$) while the ’minus’ one ($`f=f_\alpha ^{}f_\alpha `$) is suppressed in magnetization and susceptibility, Fig.1. At higher temperatures the combination harmonics are exponentially small compared with the single-band ones, as shown in Fig.1.

We note that according to Eq.(14) the difference between the second (and higher) Fourier amplitudes for open and closed systems should be seen even in a simplest single-band metal. On the other hand in three (and higher)- band metals a mixture of more than two different frequencies can be observed due to non-parabolic band dispersion giving rise to cubic and higher powers of the chemical potential in the expression for $`\mathrm{\Omega }_0`$, Eq.(8). In very high magnetic fields the usual magnetic breakdown and the non-linear field dependence of magnetic subbands due to non-parabolicity of the band dispersion could also lead to combination frequencies.

In conclusion we have developed the analytical semiclassical theory of magnetic quantum oscillations in multi-band two-dimensional metals. We have found the amplitudes of the novel combination Fourier harmonics, which are comparable with the single-band harmonics at low temperatures and exponentially small at higher temperatures. Their frequencies and the temperature dependence of amplitudes provide additional information on the band structure and carrier densities of a multiband canonical Fermi liquid. Essentially different temperature dependence of the combination amplitudes compared with the standard harmonics, Fig.1, should allow to distinguish them experimentally.

We thank A.P. Levanyuk for enlightening comments on the relationship between different statistical ensembles.