1. Introduction
The phenomenon of weak localization of conduction electrons, which manifests itself in the enhancement of backscattering of classical waves in disordered media, has attracted scientific interest in recent decades [
1,
2,
3,
4,
5,
6,
7,
8,
9]. Weak localization manifests itself mainly in an increase in the probability of elastic backscattering in a narrow range of solid angles, of the order of
, where
is the length of an electron or light wave, and
is the mean free path of electrons and photons. Coherent phenomena associated with the scattering of external particles (such as electrons or neutrons) with fixed excitation energies of a disordered medium were studied in [
10,
11,
12,
13], where weak localization was observed for electron beams with energies from 10 to 1000 electron volts. Neutron beams were also the subject of this work [
14]. According to these works, coherent phenomena can be observed in the enhancement of particle backscattering during elastic interaction with a disordered medium, despite the relatively high energies of the particle beams. The influence of inelastic processes on the conductivity under conditions of weak localization has been studied in many works [
15,
16,
17,
18]. In these cases, two basic assumptions are usually made. First, multiple scattering is represented as forward multiple scattering and single large-angle scattering [
19]. Second, the scattering by each individual diffuser is considered to be isotropic. It was shown that the role of inelastic processes at weak localization is secondary and negative, since inelastic collisions violate phase relations, thereby reducing the probability of coherent processes. However, there are cases when inelastic processes do not lead to the loss of phase memory by the system. It was shown for the first time in [
20]. In this case, in addition to the usual weak localization of the Anderson type, there is a weak localization of electrons of a new type or a new weak localization, which is essentially associated with inelastic processing. Moreover, the origin of inelasticity is not essential, for example, it can be a plasmon, photon, phonon, or exciton. Moreover, quantum coherence can exist even if the electron is exposed to an incoherent electromagnetic field. In these cases, the situation is considered when, in the case of an inelastic interaction, the particle loses a fixed energy and enters the inelastic channel, having an energy different from the initial value in the incident beam. In addition to inelastic collision, the particle can still participate in at least one elastic process, after which it leaves the medium and can be registered. This effect demonstrates itself in the scattering processes of high-energy electron beams, where electrons velocities are relativistic. The investigation of the process of the resonant spontaneous bremsstrahlung of ultrarelativistic electrons in the fields of a nucleus and a weak quasimonochromatic electromagnetic wave was done in [
21,
22]. There is a coherent scattering process of photons with inelastic interaction with ultrarelativistics electrons. In this case, a characteristic angular dependence with a frequency shift appears for photons. The process has been studied in a special kinematic region, where stimulated processes with correlated emission and absorption of photons of the first and second waves predominate (the effect of parametric interference). It is interesting that the described effect of a new type of weak localization for photons does not depend on the type of inelasticity, the creation of an electron-positron, or something else. The amount of energy loss is important. In this interference kinematics, correspondence is established between the emission angle and the energy of the final electron.
There are two ways to implement this process, so it can start or end with an inelastic collision. The interference of electron waves associated with these additional processes turns out to be constructive [
23]. This manifests itself in an increase in the scattering of electrons at an angle other than π, and this difference can be significant. There are certain differences in the localization of electrons for different mechanisms of inelastic scattering, but it turns out that the general features of this phenomenon prevail. The most striking difference between localization of a new type in the case of inelastic scattering from ordinary weak localization is the difference in the characteristic scattering angles. The scattering probability here is maximal in the range of scattering angles close to
, and the effect manifests itself in a much wider range of angles than in the case of traditional localization, in which the beam enhancement is observed in forward or backward scattering at an angle of π. As already mentioned, the main difference between conventional and new weak localization is the typical electron scattering angle. The angular distribution of particles and radiation in the case of ordinary weak localization in a disordered medium is usually described using the maximum cross (or so-called “fan”) diagrams, which are used to calculate the electron radiation cross-section. Regular weak localization, in particular, can be described by a simple graphical method [
24,
25], which gives an idea of this phenomenon and explains why the angle pi is specific for regular weak localization. This method takes into account that an electron with momentum
k is scattered through two complementary series of intermediate scattering states
and
to the state
−k. Momentum changes:
for the first scattering chain and
for the second. The amplitudes in the final state −
k are the same, and add up, and the waves in the forward and reverse directions are superimposed on each other constructively, reinforcing each other. This is due to the fact that the complementary scattering processes have the same changes in momentum, both in a straight line and in the opposite sequence. An explanation of why the coherent enhancement of electron scattering in the inelastic scattering channel occurs at angles other than π is proposed in [
25]. A simple kinematic model is used to determine the basic properties of weak localization of electrons in the inelastic scattering channel. It easily reproduces the range of scattering angles characteristic of weak localization of electrons with energy loss. The results are consistent with the results based on the dynamic theory associated with the calculation of crossed and ladder diagrams. It is possible to trace the transition from a new type of weak localization to the usual weak localization with a decrease in energy losses. The new type of weak localization is consistent with regular weak localization if the energy losses are approximately equal to zero.
The range of angles in the elastic channel is of the order of
, and in the inelastic channel is of the order
, where
γ is the electron collision frequency,
E is its energy, and
is the energy transferred to the medium. It is assumed that the energy of an electron incident on the medium is high enough to excite plasmons or atoms. However, this energy should not be too large so that the de Broglie wavelength of electrons was less but remained comparable to the distance between the centers of scattering, so that constructive interference of waves of scattered electrons inside condensed media could exist. The corresponding energy values for electron beams are in the range from hundreds of eV to keV. Moreover, the above statements remain valid both for the case of a small number of elastic collisions, and for a sufficiently large number; the main thing in this case is only one inelastic collision [
23]. The main reason for the difficulty of fixing the indicated effect in a solid is that the very phenomenon of the new weak localization and all possible measurable parameters have been considered and calculated for an infinite three-dimensional medium, while the role of surface effects at a boundary of a condensed medium is large.
Taking into account the principle of indistinguishability of electrons in a beam and a medium, as was shown for a neutral atomic medium [
26], but also takes place in a solid, this shifts the scattering enhancement to the parameters of an ordinary weak localization. As it is shown in [
26], the scattering intensity includes the electron exchange terms varying directly as cosχ, where χ is a scattering angle. The expression for intensity contains two main terms, the first one is specific for the new weak localization, and the exchange interaction here contributes as an increasing pre-factor. The second term is entirely produced by electron exchange and is proportional to cosχ. Despite the obtained interesting exchange effect in a new type of weak localization for hydrogen scatterers, there was no systematic method allowing the principle of indistinguishability and permutation symmetry to be taken into account when describing scattering processes in the general case. The exchange effect considered in [
24] is a good example of the importance of developing a general formalism that makes it possible to take into account the permutation symmetry of a many-electron system in the scattering problem in general and for weak localization, in particular.
In the presented work, we discuss how exchange affects the scattering of electrons in a disordered medium in a general case. We will take into account the identity of the incident electrons and electrons belonging to multielectron scatterer atoms. An invariant exchange perturbation theory method [
27,
28] is applied for the development of the cross-section for the weak localization scattering process while taking into account exchange effects. It is shown that, in spite of isotropic scattering by each individual scatterer, the number of electrons and their spin state in the open shell of the atom radically affect the resulting angular dependence of the scattering cross-section of incident electrons. In this case, the electrons themselves of the open shell of the scattering atom can be in the s-state, that is, the shell of the atom remains spherically symmetric. An additional angular dependence of the scattering cross-section appears, which is proportional to cosχ and does not depend on the number and state of the spin of electrons with an open or closed shell. The main difference, depending on the number of electrons and their spin states, is the coefficient in front of cosχ.
2. Probability of Plasmon Emission with Atom Excitation and Electron Exchange
We consider the interaction of electrons with a medium, accompanying the excitation of atoms when electrons are scattered by them, by the same way as in [
20] by using the interaction operator in the form of the sum of two contributions:
where the operator
describes electron interaction with atoms of medium, numbered by indexes
l:
and
describes the interaction of the moving electron with the electric polarization field of the medium electrons, which arises under this action. Then, let the process of inelastic scattering of an electron be associated with the loss of energy on the plasmon:
where
is the operator of the electric field potential due to plasma oscillation and
is the charge density operator.
The initial state of the system corresponding to an incident electron and an atom of the medium (for example, a Zi-Ni alloy doped with Ca, Mg, or hydrogen or He) is described by the wave vector
, antisymmetric taking into account the electronic permutations between the atom and the incident electron. Here,
n is the set of quantum numbers of atoms in the initial state, and
p is the momentum of the incident electron. Regarding the exchange perturbation theory method [
27,
28], the final state of the whole system can be described by the non-symmetric wave function
, which is a simple product of the atomic function
, antisymmetrized with internal electron permutations, and a free electron function
, where
Q is the total momentum transferred to the medium. It should be underlined that the operator (2) describing electron interaction with atoms has a non-symmetric form regarding the interatomic electron permutations (the exchange of numbered atomic electrons with the free electron of incident):
where
is the antisymmetrization operator [
27,
28]. Acting on a non-symmetric wave function, operator
performs antisymmetrization:
where
is the parity of the
permutation,
are the normalization condition and a normalization factor,
is the wave vector of the zeroth permutation with the initial arrangement of the electrons, and the subindex shows that the number of the permutation is ν = 0. Here, we deal with the antisymmetric non-orthogonal basis, while
is the same as for
, but this set meet a completeness property:
where
is the total number of electron permutations. The proof of completeness property (6) is described in detail in
Appendix A. Generally speaking, both the “zero” Hamiltonian
describing a multicentre many-electron system without interatomic interaction, and the perturbation operator
describing this interatomic interaction are not invariant to the operation of antisymmetrization, taking into account the rearrangement of electrons between the two subsystems:
. At the same time, the complete Hamiltonian of the system
retains its invariance:
. This discrepancy means a serious problem related to the fact that the zero-order wave function, antisymmetrized with respect to center-to-center electron permutations, is not an eigenfunction of the non-invariant Hamiltonian
[
27], and the corrections are obtained by applying an asymmetric operator of interactions containing non-physical contributions. In [
27,
28], a special symmetric form of the perturbation operator and zeroth Hamiltonian were developed. It allows corrections of the wave functions, properly antisymmetrised, and the energy corrections to be obtained by using the correct antisymmetric basis of the wavefunctions:
where
denotes a projector onto an asymmetric state, corresponding to the
permutation
and
, and
, as mentioned before, is the total number of permutations. In this case, the Hamiltonian
describing a system without the interaction of two subsystems has an eigenvector, which has an antisymmetric form taking into account the electronic permutations between these subsystems:
In our case, the second term of the perturbation operator (1)
has a symmetric form with respect to the permutations of electrons. It is important to emphasize that after obtaining all the corrections to the energy and the wave vector in all orders of the perturbation theory in the general formalism, all matrix elements containing the complex symmetric form (6) of the perturbation operator can be analytically reduced to a simple form. This is a symmetry-adapted form that includes the usual asymmetric perturbation operator corresponding to the initial zero permutation of electrons. Such a form is more convenient for practical applications. We transform all matrix elements in the following way:
The probability of a transition of the system in unit time from one state to another with transfer of momentum
Q from the incident electron to the medium and with transition of the medium from state n to state m has the form obtained in [
27,
28], taking into account electron exchange
where operator
is the operator of transition on the energy surface [
27,
28,
29], the general operator equation for which with taking into account electron permutations between subsystems is:
where
η is the relaxation frequency in the general case. We rewrite it as a series:
In the matrix element
in Equation (9), the
bra-vector has an antisymmetric form with respect to electronic permutations, and the
ket-vector has a simple non-symmetric form. Then, a transition amplitude will be:
where we denote the normalized (indexed
) resolvent operator
(or the Green’s function for the coordinate representation) and the operator equation taking into account an antisymmetric nonorthogonal basis:
Since the plasmon excitation is small, we can consider this process in the Born approximation. We do not fix our attention on the features of plasmon excitation in different situations, as it was done in detail in [
22,
30], where the excitation and propagation of bulk and surface plasma waves by incident electrons were analyzed. The motion of electrons was considered both in vacuum when approaching the surface of the metal, and inside the metal, the boundary of which elastically and specularly reflected the internal nonequilibrium electrons. The effect of electron boundary scattering parameters on the structure of bulk and surface plasmon resonances was analyzed in [
31]. The probability of transition radiation of bulk plasmon by an electron moving in vacuum was examined.
We leave only the first two terms in Equation (12), where the scattering process begins or ends with plasmon excitation, and omit all other terms where the inelastic process with a plasmon occurs between the processes of elastic scattering by atoms. This is because we are not interested in small-angle scattering by the medium as a whole. The mentioned two terms we shall write out in the form:
where the first two matrix elements describe the process of plasmon excitation without atomic scattering. However, the exchange coefficients:
mean the exchange density due to the entanglement of electronic states. The third term of Equation (14) corresponds to a process that begins with scattering by atoms and ends with excitation of plasmons. The fourth term corresponds to the process in which the events occur in the opposite order. Since we are not interested in small-angle scattering by the medium as a whole, as mentioned earlier, we can omit the first two terms.
Dividing the result of Equation (9) by the flux density of incident particles (
, where
is the wavevector of the relative movement of the incident electrons and
me is their mass), we obtain an expression for the cross-section of scattering events and reactions. Then, we multiply this expression for the cross-section by the number of final states in the volume per unit energy interval for scattering along the unit vector
into a solid angle element
dΩ,
, because the final state is within the continuous spectrum. Then, for the differential cross-section summed over the final states of the medium, it has the form:
For electrons, we take into account the disorder of the medium, and for the plasmon electric field, we assume that the medium is completely homogeneous. Therefore, we can assume that the matrix elements in Equation (14) are approximately equal to each other:
and the exchange coefficients
and
have the same order and are proportional to
, then we can rewrite Equation (16) in the form:
which is illustrated in
Figure 1 by the set of so-called fan diagrams determining the effect of new angle dependence of the effective cross-section.
As usual, in the diagrams that match Equation (17), we will use the dotted line to connect two vertices belonging to the same atom. The lower parts of the diagrams correspond to the analytic expression, which is the complex conjugation of the expression equivalent to the upper parts. The wavy line corresponds to the plasmon. The set of ladder diagrams, correspondent to the terms contributed to the cross-section (17), are independent of the electron-scattering angle. The relation of the crossed diagram contributions and ladder diagrams determine a so-called coherency degree [
25]:
Neglecting exchange effects, in the resulting expression (17), both
bra- and
ket- vectors become non symmetric, and we obtain the well-known result obtained in [
25,
26,
27]. In contrast to the usual weak localization, one of the crossed lines in the new type of weak localization corresponds to inelastic scattering, while the others correspond to elastic interaction with randomly distributed power centers. According to formula (18), crossed diagrams together with the corresponding ladder diagrams contribute to the scattering probability factor
[
20]:
It was shown in [
24,
25,
26] that the angular dependence characteristic of a new weak localization arises due to the term in the integrand, which describes the contribution of the interference of two electron waves propagating along the same path in opposite directions:
where
γ is the electron collision frequency.
This means that weak localization occurs due to such collisions of electrons in which each subsequent scattering begins earlier than the end of the previous one. Thus, a new weak localization is realized when two conditions are met simultaneously:
If we denote
, then a simple kinematic approach explains the range of the scattering angle
typical for the new type of weak localization:
For more details, [
24,
25], where it is explained why the ang1es typical of the new type of weak localization differ from
π, and by using the simple kinematic approach, these angles can be estimated very accurately.
Considering Equation (18) taking into account the exchange contributions, we can write the following:
In the case of an antisymmetric basis, the calculation of matrix elements
requires additional comments. Instead of the resolvent operator
, we will use a one-electron Green function
taking into account that exchange contributions influence the one-particle system:
where:
Integration over the conductor volume
V means averaging over randomly distributed scatterers. Here, we used the completeness property (6). In the same way, we rewrite the matrix element of another resolvent operator:
The spectral density
of the cross-section (23) of the process of inelastic scattering of electrons on disordered media consisting of atomic defects in a metal alloy (metal alloy doped with di- or trivalent atoms), taking into account exchange effects, has the form:
Using the obtained general expression for the cross-section (18) for the case considered in [
24], the alloy doped by hydrogen atoms as disordered centers, we obtain the same expression for the Green functions and for the scattering probability. It proves a limit transition of the obtained general expression (18) for the cross-section to the known case described in [
24].