Kinetic equations for two-photon light in random media
Abstract.
We consider the propagation of light in a random medium of two-level atoms. We investigate the dynamics of the field and atomic probability amplitudes for a two-photon state and show that at long times and large distances, the corresponding average probability densities can be determined from the solutions to a system of kinetic equations.
1. Introduction
The propagation of light in random media is usually considered within the setting of classical optics [1]. However, there has been considerable recent interest in phenomena where quantum effects play a key role [2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15]. Of particular importance is understanding the impact of multiple scattering on entangled two-photon states, with an eye towards characterizing the transfer of entanglement from the field to matter [13, 16, 5, 17, 18, 19, 20]. Progress in this direction can be expected to lead to advances in spectroscopy [21], imaging [22, 23, 24, 25, 26, 27, 28, 29, 30, 31] and communications [32, 33, 34] .
The propagation of two-photon light is generally investigated either in free space or, in some cases, with account of diffraction [35, 36] or scattering [37]. In this paper, we consider the propagation of two-photon light in a random medium. A step in this direction was taken in [38], where a model in which the field is quantized and the medium is treated classically was investigated. The main drawback of that work is that it is does not allow for the transfer of entanglement between the field and the atoms or between the atoms themselves. Instead, we treat the problem from first principles, employing a model in which the field and the matter are both quantized. We show that for a medium consisting of two-level atoms, the field and atomic probability amplitudes for a two-photon state obey a system of nonlocal partial differential equations with random coefficients. Using this result, we find that at long times and large distances, the corresponding average probability densities in a random medium can be determined from the solutions to a system of kinetic equations. These equations follow from the multiscale asymptotics of the average Wigner transform of the amplitudes in a suitable high-frequency limit [39, 40, 41, 42]. This formulation of the problem builds on earlier research by the authors on collective emission of single photons in a random medium of two-level atoms [43]. In that work, we employed a formulation of quantum electrodynamics in which the field is quantized in real space, thus allowing for the field and atomic degrees of freedom to be treated on the same footing.
This paper is organized as follows. In section 2 we formulate our model for the propagation of two-photon light and derive the equations governing the dynamics of the field and atomic degrees of freedom. Section 3 is concerned with the application of the real-space formalism to the problem of stimulated emission by a single atom. In section 4 we study the dynamics of a two-photon state in a homogeneous medium. In section 5 we discuss the problem of stimulated emission in a random medium and obtain the governing kinetic equations. Section 6 takes up the general problem of two-photon transport in random media and presents the relevant kinetic equations. Our conclusions are formulated in section 7. The appendices contain the details of calculations.
2. Model
We consider the following model for the interaction between a quantized massless scalar field and a system of two-level atoms. The atoms are taken to be identical, stationary and sufficiently well separated that interatomic interactions can be neglected. The overall system is described by the Hamiltonian
(1) |
where is the Hamiltonian of the field, is the Hamiltonian of the atoms and is the interaction Hamiltonian. In order to treat the atoms and the field on the same footing, it is useful to introduce a real-space representation of [43]. The Hamiltonian of the field is of the form
(2) |
where is a Bose scalar field that obeys the commutation relations
(3) | ||||
(4) |
where we have neglected the zero-point energy. The nonlocal operator is defined by the Fourier integral
(5) | ||||
(6) |
We note that (2) is equivalent to the usual oscillator representation of .
To facilitate the treatment of random media, it will prove convenient to introduce a continuum model of the atomic degrees of freedom [43]. The Hamiltonian of the atoms is given by
(7) |
where is the atomic resonance frequency, is the number density of the atoms, and is a Fermi field that obeys the anticommutation relations
(8) | ||||
(9) |
The Hamiltonian describing the interaction between the field and the atoms is taken to be
(10) |
where is the strength of the atom-field coupling. Here we have made the Markovian approximation, in which the coupling constant is independent of the frequency of the photons or positions of the atoms, and have imposed the rotating wave approximation (RWA).
We suppose that the system is in a two-photon state of the form
(11) | ||||
where is the combined vacuum state of the field and the ground state of the atoms. Here the atomic amplitude is the probability amplitude for exciting two atoms at the points and at time , the one-photon amplitude is the probability amplitude for exciting an atom at and creating a photon at , and the two-photon amplitude is the probability amplitude for creating photons at and . The functions and are symmetric and antisymmetric, respectively:
(12) |
consistent with the bosonic and fermionic character of the corresponding fields.
The state is the most general two-photon state within the RWA. In addition, is normalized so that . It follows from (3) and (8) that the amplitudes obey the normalization condition
(13) |
If the amplitudes , and are factorizable as functions of and , then there are no quantum correlations and the state is not entangled. Otherwise is entangled. If alone is not factorizable, we say that is an entangled two-photon state.
The dynamics of is governed by the Schrodinger equation
(14) |
Projecting onto the states and and making use of (3) and (8), we arrive at the following system of equations obeyed by , and :
(15) | ||||
(16) | ||||
(17) |
The overall factors of in the above will be cancelled as necessary. The details of the calculation are presented in Appendix A.
The above model views the atomic degrees of freedom as fermionic. In Appendix D we consider the bosonic case.
3. Single-Atom Stimulated Emission
In this section we consider the problem of stimulated emission by a single atom. We assume that the atom is located at the origin and put . Thus the system (2)–(17) becomes
(18) | |||
(19) |
where the term does not contribute due to the antisymmetry of . We assume that initially there is only one photon present in the system, which means that the initial conditions for the amplitudes and are given by
where is the wavevector of the photon. Note that the amplitude of is set to unity for convenience. To proceed, we take the Laplace transform with respect to and the Fourier transforms with respect to and of (18) and (19). We thus obtain
(20) | ||||
(21) |
Here we have defined the Laplace transform by
(22) |
where we denote a function and its Laplace transform by the same symbol. Solving (20) and (21) leads to an integral equation for of the form
(23) |
where
(24) |
with . In order to evaluate the integral in (23), we make the pole approximation where we replace with . We note that this quantity is independent of and , and so we will denote it by . For consistency, we also replace by under the integral in (23). Note that this approximation arises in the Wigner-Weisskopf theory of spontaneous emission. In addition, we split into its real and imaginary parts:
(25) | ||||
(26) |
We can calculate and by making use of the identity
(27) |
We find that
(28) | ||||
(29) |
and
(30) |
where we have introduced a high-frequency cutoff to regularize the divergent integral. Using the above results, (23) becomes
(31) |
Since appears on both the left- and right-hand sides of (31), upon iteration we obtain an infinite series for , which to order is given by
(32) | ||||
(33) |
Inverting the Laplace transform, we find that is given by
(34) |
Note that decays exponentially at long times () and that can be obtained from (20).
4. Constant Density
In this section we consider the case of a homogeneous medium and set , where is constant. It is useful to define the function and write (17) as a symmetric system. If we further define the vector
(35) |
then (17) can be written as
(36) |
where
(37) |
This definition of has the advantage that the matrix is symmetric. The Fourier transform of (36) with respect to the variables and is given by
(38) |
where
(39) |
The matrix has eigenvalues
where
(40) | ||||
(41) | ||||
(42) |
The components of the associated eigenvectors are given by
(43) | ||||
(44) | ||||
(45) | ||||
(46) |
It follows that the solution to (38) is
(47) |
where the values are solutions to the linear system
(48) |
In order to study the emission of photons, we assume that initially there are two localized volumes of excited atoms of linear size centered at the points and . The initial amplitudes are taken to be
(49) | ||||
(50) | ||||
(51) |
Figure 1 illustrates the time dependence of and , where we have set the dimensionless quantities . Note that the atomic amplitude is antisymmetric, consistent with (8) and that it corresponds to an entangled state. We observe that the amplitudes oscillate and decay in time. Moreover, the atomic and one-photon amplitudes are out of phase with one another, and the two-photon amplitude is an order of magnitude smaller.
5. Stimulated Emission in Random Media
5.1. Kinetic equations
In this section we consider stimulated emission in a random medium. We suppose that there is at most one atomic excitation and that there are at most two photons present in the field. Thus we set the and study the dynamics of and . The system (17) then becomes
(52) |
which can be rewritten as the pair of equations
(53) |
We will assume that the number density is of the form
(54) |
where is a constant and is a real-valued random field. We assume that the correlations of are given by
(55) | ||||
(56) |
where is the two-point correlation function and denotes statistical averaging. We further assume that the medium is statistically homogeneous and isotropic, so that depends only upon the quantity . If we define
(57) |
then the above system of equation can be rewritten as
(58) |
where
(59) | ||||
(60) |
To derive a kinetic equation in the high-frequency limit, we rescale the variables , , and . Additionally, we assume that the randomness is sufficiently weak so that the correlation function is . Eq. (58) thus becomes
(61) |
where
(62) |
Next we introduce the scaled Wigner transform, which provides a phase space representation of the correlation functions of the various amplitudes. The Wigner transform is defined by
(63) |
where denotes the hermitian conjugate. The Wigner transform is real-valued and its diagonal elements are related to the probability densities and by
(64) | |||
(65) |
The above factor of two is due to the symmetry of the function . The off diagonal elements are related to correlations between the amplitudes:
(66) |
As shown in Appendix B, the Wigner transform satisfies the Liouville equation
(67) |
where
(68) |
and the Fourier transform is defined as
(69) |
We study the behavior of in the high frequency limit . To this end, we introduce a multiscale expasion of the Wigner transform of the form
(70) |
where and are fast variables and is assumed to be both deterministic and independent of the fast variables. We treat the variables and as independent and make the replacements
(71) |
Hence the Liouville equation becomes
(72) |
where
(73) | ||||
(74) |
and the Fourier transform is defined as
(75) |
Substituting (5.1) into (5.1) and equating terms of the same order in leads to a hierarchy of equations. At we have
(76) |
Since is symmetric it can be diagonalized by a unitary transformation. The eigenvalues and eigenvectors of are given by
(77) | ||||
(78) |
where
(79) |
Evidently is also diagonal in this basis and can be expanded as
(80) |
At order we have
(81) |
We can then decompose as
(82) |
Multiplying (5.1) on the left by and the right by , we arrive at
(83) |
where is a small positive regularizing parameter and
(84) |
At order we find that
(85) |
where
(86) |
In order to obtain an equation satisfied by , we multiply this equation on the left by () and on the right by () and take the average. Additionally, we assume that is identically zero, which corresponds to being statistically stationary with respect to the fast variables and . This relation closes the hierarchy of equations and leads to the kinetic equation
(87) |
where the scattering coefficients , the scattering kernel , and the functions are defined as
(88) | ||||
(89) | ||||
(90) | ||||
(91) |
Some details of the derivation of (5.1) are included in Appendix C.
5.2. Diffusion approximation
We now consider the diffusion limit of the kinetic equation (5.1). The diffusion approximation (DA) to a kinetic equation of the form
(92) |
is obtained by expanding into spherical harmonics as
(93) |
where
(94) | ||||
(95) | ||||
(96) |
Integrating (5.2) with respect to and we arrive at
(97) |
If instead we multiply by and integrate we obtain
(98) |
where
(99) |
and
(100) | ||||
(101) |
Similarly, multiplying (5.2) by and carrying out the indicated integrals leads to
(102) |
where
(103) |
and
(104) |
Next we substitute (93) into (100), (101), and (104) and carry out the indicated integrations. We find that
(105) | ||||
(106) | ||||
(107) |
Using the above results, (98) and (102) become
(108) | |||
(109) |
At long times (), the first terms on the right-hand sides of (108) and (109) can be neglected. Substituting the resulting expressions for and into (97), we obtain the diffusion equation obeyed by :
(110) |
Here the diffusion coefficients are defined by
(111) |
In the case of white noise disorder, where the correlation function , with constant , the phase functions , which corresponds to isotropic scattering.
The solution to (110) for an infinite medium is given by
(112) |
Making use of the above results, we see that each of the modes satisfy (5.1) and thus their first angular moments, which are defined by
(113) |
satisfy the equations
(114) |
where
(115) |
We assume that initially there are two photons present in the field localized around the points and in a volume of linear size . The corresponding initial conditions are given by
(116) | ||||
(117) |
Note that corresponds to an entangled two-photon state. These initial conditions imply initial conditions for the Wigner transform from (5.1), which in turn imply initial conditions for the modes from (80):
(118) |
(119) |
where
(120) |
The initial conditions for the first angular moments are then found using (113):
(121) |
(122) |
The above initial conditions are then inserted into (112) and the Gaussian integrals carried out. This results in the following formulas for the angular moments :
(123) | |||
(124) |
(125) | |||
(126) |
Finally, combining the above with (64), (80) and (113), we see that the average probability densities are given by
(127) |
where we have introduced the notation for , and the coefficients and are defined by
(128) | ||||
(129) |
It is readily seen that long times, and decay algebraically according to the formulas
(130) | ||||
(131) |
where the constants for are given by
(132) |
(133) | ||||
(134) |
(135) |
To illustrate the above results, we consider the case of isotropic scattering and set the dimensionless quantities . In addition, we choose , , and , so that the distances from the points of excitation ( and ) to the points of detection are equal to . In Figure 2 we plot the time dependence of the probability densities and . We note that is monotonically decreasing while has a peak near . A comparison of these results with the asymptotic formulas (130) and (131) is shown in Figures 3 and 4 . There is good agreement at long times.
6. Kinetic Equations for Two-Photon Light
In this section, we consider the general problem of two photons interacting with a random medium. That is, we will study the the time evolution of the amplitudes , and and derive the related kinetic equations. We begin with the system (17), where we have canceled overall factors of :
(136) | ||||
Here the number density is a random field of the form (54). Eq. (6) can now be rewritten as
(137) |
where is defined by (35) and
(138) | ||||
(139) |
As before. to derive a kinetic equation in the high-frequency limit, we rescale according to , and . Additionally, we assume that the randomness is sufficiently weak so that the correlations of are . Eq. (137) thus becomes
(140) |
where
(141) |
To proceed further, we introduce the matrix Wigner transform which is defined by (5.1). The diagonal elements of are related to the probability densities by
(142) | |||
(143) | |||
(144) |
while the off diagonal elements of are related to correlations between the amplitudes. It can be seen by direct calculation that the Wigner transform satisfies the Liouville equation
(145) |
where is given by (39), and the Fourier transform is defined by
(146) |
Once again we study the behavior of in the high-frequency limit and introduce a multiscale expansion of the Wigner transform of the form
(147) |
where and are fast variables and is both deterministic and independent of the fast variables. We will treat the slow and fast variables and (respectively and ) as independent and make the replacement (71). Hence (6) becomes
(148) |
where the Fourier transform is defined by (5.1). Next we substitute (6) into (5.1) and collect terms at each order of . At order we have
(149) |
Since is symmetric it can be diagonalized. We then define , be the eigenvector-eigenvalue pairs given by (4) and (4). It follows from (149) that is also diagonal in this basis and can be expanded as
(150) |
At order we find that
(151) |
Although is not diagonal, we can still decompose its Fourier transform as
(152) |
Multiplying (6) on the left by and the right by , we obtain
(153) |
where
(154) | ||||
(155) |
Here is a regularizing parameter. At order we find that
(156) |
where
(157) |
and
(158) |
In order to obtain the equations satisfied by the , we multiply (6) on the left by and the right by , and take the ensemble average. In order to close the hierarchy of equations, we assume that , which corresponds to the assumption that is statistically stationary with respect to the fast variables and . Following procedures similar to those in Appendix C, we find that
(159) |
where
(160) | ||||
(161) | ||||
(162) | ||||
(163) | ||||
(164) |
6.1. Diffusion approximation
In this section we consider the diffusion limit of the kinetic equation (6). We again specialize to the case of white-noise correlations, which leads to the phase function , corresponding to isotropic scattering. Making use of the diffusion approximation developed in section 5.2, we see that the first angular moments
(165) |
satisfy the equations
(166) |
where
(167) | ||||
(168) |
Suppose that initially there are two photons in the field localized around the points and in a volume of linear size . The corresponding initial conditions are given by
(169) | ||||
(170) |
where
(171) |
Note that this corresponds to an entangled two-photon state.
The above initial conditions imply initial conditions for the Wigner transform . The initial conditions for the modes are determined by solving the linear system
(172) |
where
(173) |
It follows that the initial conditions for the first angular moments are given by
(174) |
The diffusion equations (166) can then be solved using (112). Combining this result with (142)–(144), (150) and (165) we see that the average probability densities are given by
(175) |
(176) |
(177) |
We note that at long times, the average probability densities decay algebraically according to
(178) | ||||
(179) | ||||
(180) |
where the constants and , are given by
(181) | ||||
(182) | ||||
(183) |
In order to illustrate the above results, we consider the case of isotropic scattering and set the dimensionless quantities . In addition, we choose , , and , so that the distances from the points of excitation ( and ) to the points of detection are equal to . In Figure 5 we plot the time dependence of the probability densities , and . We note that the negative values of these quantities are due to the breakdown of the diffusion approximation at short times. We observe that the two-photon probability density increases before eventually decaying. A comparison of these results with the asymptotic formulas (178), (179) and (180) is shown in Figures 6, 7 and 8. There is good agreement at long times.
7. Discussion
We have investigated the propagation of two-photon light in a random medium of two-level atoms. Our main results are kinetic equations that govern the behavior of the field and atomic probability densities. Several topics for further research are apparent. An alternative derivation of these equations may be possible using diagrammatic perturbation theory rather than multiscale asymptotic analysis. This is the case for the classical theory of wave propagation in random media, where a comparative exposition of the two approaches has been presented in [41]. It would be of some interest to quantify the evolution of the entanglement of a two-photon state as it propagates through the medium. One approach to this problem is to introduce a suitable measure of entanglement such as the entropy defined by the singular values of the two-photon amplitude [37]. Here the evolution of the entanglement of an initially entangled state is of particular importance, especially in applications to communications and imaging. Finally, accounting for atomic motion is a challenging problem. One possible approach is to view the density as a quantum field whose dynamics must be taken into account.
Appendix A Derivation of the System (17)
Here we derive the system (17). We begin by computing both sides of the time-dependent Schrodinger equation (14), employing the Hamiltonian and the state (11). The left-hand side is equal to
(184) |
while the right-hand side is given by
Using the commutation and anticommutation relations (3) and (8) we arrive at
(185) |
Computing the inner products
(186) | ||||
(187) |
yields (2). The inner products
(188) | ||||
(189) |
give (16), while
(190) | ||||
(191) |
gives (17).
Appendix B Derivation of the Liouville Equation (5.1)
Here we derive (5.1). We first define
(192) |
The Wigner transform is defined by
(193) |
We begin by computing :
(194) |
The first term becomes
(195) |
where
(196) |
Likewise, the second term becomes
(197) |
Finally, the third term becomes
(198) |
Appendix C Derivation of the Kinetic Equation (5.1)
Here we derive the kinetic equation (5.1) which is satisfied by the quantity . The first two terms are elementary and so we must compute
(199) |
We compute each of the above in two steps. The first term is
Next we substitute the expression using equation (5.1) to arrive at
We separate the above into two terms and use the orthogonality of the basis to see that in the first term. We thus obtain
(200) |
As the above converges to
(201) | |||
(202) |
which follows from the Riemann-Lebesgue Lemma and the fact that is independent of the fast variables and . Similarly the other three terms become
(203) |
Making use of the identity
(204) |
we see that we must have , to ensure that the support of the delta function is nonempty since and are never equal. Thus the above equation simplifies as
(205) |
Putting everything together, we see that satisfies the equation
(206) | ||||
(207) |
The delta function can be simplified using the identity
(208) |
where has a single real root at . Thus
(209) |
Hence (C) becomes
(210) |
as desired.
Appendix D Bosonic Model
Here we consider the bosonic analog of the model described in section 2. The physical implications of the bosonic model will be explored elsewhere.
We suppose that the atomic field satisfies the bosonic commutation relations
(211) | ||||
(212) |
The Hamiltonian (1) remains unchanged. As in section 2, we assume that the state is of the form
(213) | ||||
The amplitudes and are now both taken to be symmetric,
(214) |
consistent with the bosonic character of the fields. Making use of the Schrodinger equation (14), we find that , , and satisfy the system of equations
(215) | ||||
(216) | ||||
(217) |
Note that there is a difference in the equations of motion for the bosonic and fermionic cases. Namely, a single term in each of (16), (17) and (216), (217) changes sign. We also note that there is no corresponding change in the single excitation theory of [43].
The bosonic model allows more than one atomic excitation to be present at the same point in space. To address this difficulty, the Hamiltonian is modified by adding an interaction term of the form
(218) |
where the number operator and the repulsion is a large positive number. The above term penalizes the creation of an excitation at a point where another is present. A similar term arises in the Hubbard model for fermionic systems.
Acknowledgments
This work was performed when the authors were members of the Department of Mathematics at University of Michigan. We thank Nick Read for valuable discussions. This work was supported in part by the NSF grant DMS-1912821 and the AFOSR grant FA9550-19-1-0320. J.E.K. was supported, in part, by Simons Foundation Math + X Investigator Award No. 376319 (Michael I. Weinstein).
Author Declarations
Conflict of Interest
The authors have no conflicts to disclose.
Data Sharing
Data sharing is not applicable to this article as no new data were created or analyzed in this study.
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