# Comment on ”Quantum Theory of Dispersive Electromagnetic Fields”

## Abstract

Recently Drummond and Hillery \[Phys. Rev. A 59, 691 (1999)\] presented a quantum theory of dispersion based on the analysis of a coupled system of the electromagnetic field and atoms in the multipolar QED formulation. The theory has led to the explicit mode-expansions for various field-operators in a homogeneous medium characterized by an arbitrary number of resonant transitions with different frequencies. In this Comment, we drawn attention to a similar multipolar study by Juzeliūnas \[Phys. Rev. A 53, 3543 (1996); A 55, 929 (1997)\] on the field quantization in a discrete molecular (or atomic) medium. A comparative analysis of the two approaches is carried out highlighting both common and distinctive features.

Recently Drummond and Hillery  have presented a quantum theory of dispersive electromagnetic modes in a medium characterized by an arbitrary number of resonant transitions with different frequencies. The radiation field and the matter was assumed to constitute a single dynamical system. In the homogeneous (plane wave) case, explicit expansions have been obtained for the field-operators in terms of the operators for creation and annihilation of polaritons (elementary excitations of a combined system containing the radiation and the matter).Yet, the authors of the paper  have overlooked a closely related study  that also provides explicit mode-expansions for various quantized fields, such as the macroscopic displacement field, given by (in the Heisenberg picture) :

$$\overline{𝐝}^{}(𝐫,t)=\underset{𝐤,m}{}\overline{𝐝}_{𝐤,m}^{}(𝐫,t);$$
(1)   
with

$$\overline{𝐝}_{𝐤,m}^{}(𝐫,t)=i\underset{\lambda =1}{\overset{2}{}}\left(\frac{\epsilon _0\mathrm{}kv_g^{\left(m\right)}}{2V_0}\right)^{1/2}n^{\left(m\right)}𝐞^{\left(\lambda \right)}\left(𝐤\right)\left[e^{i\left(𝐤.𝐫\omega _k^{\left(m\right)}t\right)}P_{𝐤,m,\lambda }e^{i\left(𝐤.𝐫\omega _k^{\left(m\right)}t\right)}P_{𝐤,m,\lambda }^+\right]$$
(2)   
where $`P_{k,m,\lambda }^+`$ ($`P_{k,m,\lambda }`$) is the Bose operator for creation (annihilation) of a polariton characterized by a wave-vector $`k`$, a polarization index $`\lambda `$, and also an extra index $`m`$ $`=1,2,\mathrm{},M+1`$ that labels branches of polariton dispersion, $`M`$ being a number of excitation frequencies accommodated by each molecule forming the medium. Here also $`𝐞^{\left(\lambda \right)}\left(𝐤\right)`$ is a unit polarization vector, $`V_0`$ is the quantization volume, $`\omega _k^{\left(m\right)}=ck/n^{\left(m\right)}`$ is the polariton frequency, $`n^{\left(m\right)}n\left(\omega _k^{\left(m\right)}\right)`$ is the refractive index (calculated at $`\omega _k^{\left(m\right)}`$), and $`v_g^{\left(m\right)}=d\omega _k^{\left(m\right)}/dk`$ is the branch-dependent group velocity.

In what follows we compare the formalism by Drummond and Hillery  to that by Juzeliūnas  highlighting common and distinctive features of the two approaches. Both studies consider a similar coupled system of the radiation field and the matter, exploiting the same multipolar formulation of Quantum Electrodynamics (QED). (Yet, different techniques have been employed to represent the operators of interest in terms of the normal polariton modes.) Moreover, in either approach an arbitrary number of transition frequencies (of electronic or vibrational origin) has been included for the material medium. As a result, the above mode-expansion (1)-(2) reproduces the same functional dependence on the group velocity and the refractive index as the corresponding expansion for the macroscopic displacement field in the one-dimensional case, given by Eq.(5.17) of ref.. Such a functional dependence is also consistent with earlier narrow-band Langrangian approach by Drummond . Furthermore, the mode-expansion (1)-(2) is equivalent to the three-dimensional displacement operator derived by Drummond and Hillery , as long as the spatial dispersion is neglected in the corresponding Eq. (8.24) of ref.. The same holds for other field-operators, such as the operator for the transverse electric field whose mode-components are related to Eq.(2) via a relationship of the classical type : $`\overline{𝐝}_{𝐤,m}^{}\left(𝐫\right)=\epsilon _0\epsilon _r^{\left(m\right)}\overline{𝐞}_{𝐤,m}^{}\left(𝐫\right)`$, the emerging relative dielectric permittivity $`\epsilon _r^{\left(m\right)}\left(n^{\left(m\right)}\right)^2`$ being a branch-dependent quantity. This is also in agreement with the ref. .

Both studies take special care in making sure that the (equal-time) commutation relationships preserve between various operators in their diagonal (polariton) representation. The study  has checked the commutation relationships involving the field-operators $`\overline{𝐝}^{}`$, $`𝐞^{}`$, $`\overline{𝐚}^{}`$, $`\overline{𝐩}^{}`$ and $`\overline{𝐡}^{}`$. Their correctness appears to be ensured by the following equalities :

$$\begin{array}{ccc}\underset{m}{}v_g^{\left(m\right)}n^{\left(m\right)}=c\hfill & \text{and}\hfill & \underset{m}{}v_g^{\left(m\right)}/n^{\left(m\right)}=c\hfill \end{array}$$
(3)   
Drummond and Hillery  have also exploited one of the these equalities in analyzing the commutation relationships. In addition, a few more complex equalities have been presented when dealing with the material operators.

A distinctive feature of the approach by Drummond and Hillery  is inclusion of spatial dispersion, i.e. dependence of the dielectric permittivity not only on the frequency, but also the wave-vector . This does not alter the form of the above relationships, as well as the mode-expansions of other macroscopic field-operators presented earlier , yet the meaning of group velocity is to be modified . It is noteworthy that the spatial dispersion has been included in the ’effective mass’ approximation through an extra differential term featured in Eqs.(6.2) and (6.8) of ref. : The term represents the coupling between infinitely close dipole-oscillators comprising the continuous dielectric medium. One might argue that such an approach is not fully consistent with the spirit of multipolar QED formulation in which there is no direct coupling between the dipole-oscillators . However, this is perhaps the only way to include the spatial dispersion within the continuous model of the dielectric considered.

On the other hand, the approach  assumes the matter to be discrete, the constituent molecules (dipole-oscillators) forming a cubic lattice. Here the effects of spatial dispersion (as well as other intermolecular coupling) are contained in the initial multipolar Hamiltonian for the radiation field coupled to the discrete medium, all interatomic coupling being mediated exclusively via the transverse virtual photons . As a result, the spatial dispersion is implicit in the general analysis of ref.  up to Eq.(3.40). The effect has been omitted in the subsequent long wave-length approximation made in Eq.(4.1) of ref.  followed by the explicit results. In fact, the spatial dispersion does play a minor role for the optical (photon-like) modes characterized by small wave-vectors. One can recover the spatial dispersion in a relatively straightforward manner using the discrete model , however this is out of the scope of the present Comment. Note that in contrast to the continuous approach , the spatial dispersion is characterized exclusively by the microscopic parameters of a discrete system, there being no need to introduce an extra parameter describing the effect.

Using a discrete approach, one can also recover the local field effects from first principles. In doing this, the theory  treats systematically the Umklapp processes playing an important role in the multipolar QED formulation. As a result, the required local-field corrections emerge intrinsically in the refractive index and the group velocity entering the mode-expansions of the field-operators . Furthermore, the discrete approach allows us to consider not only the macroscopic operators , but also the operators for the local  and microscopic  fields. For instance, the mode-components of the local displacement operator are related to those for the macroscopic displacement operator as : $`𝐝_{𝐤,m}^{}\left(𝐫_\zeta \right)=\left(\epsilon _r^{\left(m\right)}\right)^1\left[\left(\epsilon _r^{\left(m\right)}+2\right)/3\right]\overline{𝐝}_{𝐤,m}^{}\left(𝐫_\zeta \right)`$. This appears to be very helpful for the analysis of various molecular-radiation processes in dielectric media , such as the spontaneous emission.

Finally, Drummond and Hillery  have pointed out that the solution to the eigenvalue equation $`\omega ^2=c^2k^2/n^2`$ given by Eq.(7.5), ’is unique for any given modal frequency, but has forbidden regions which indicate a resonance, or absorption, band’. This would be absolutely true for the spatially non-dispersive media, as illustrated in fig.2 of ref.. However Eq.(7.5) of ref. contains the spatial dispersion (in the ’effective mass’ approximation), so that $`n=n(\omega ,k)`$. Inclusion of such a spatial dispersion yields more than one value of $`k`$ for certain frequencies , the additional solutions representing the exciton-like modes characterized by much larger $`k`$.