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Physical Review

Quantum Theory of a Gas Laser

C. R. Willis

Published Apr 10, 1967• 14 citations
Publisher

Abstract

We derive the equation of motion for the quantum-mechanical radiation density matrix of a gas laser to lowest order in the dimensionless coupling constant. Our derivation is fully quantum mechanical and we can calculate the coherence properties from the radiation density matrix. Our model consists of $N$ two-level systems interacting with radiation in a cavity in the presence of dissipation, pumping, and collisions. The method we use is a generalization of the Bogoliubov derivation of the kinetic equation for a small parameter. Our derivation holds for any physically realizable pump power, and near threshold reduces to Lamb's near-threshold theory. With the equation of motion for the radiation density matrix, we obtain solutions both for when the average field is nonzero and for when it is zero. The steady-state electromagnetic density is the same in both cases except for a small spontaneous-emission term. We show that the reason gas lasers do not satisfy rate equations is the existence of zeroth-order correlations between the internal atomic variables and atomic center-of-mass variables. It is these same zeroth-order correlations which are responsible for the Lamb dip. Our derivation includes collisions and reduces the calculations of their effect to quadrature.

DOI
10.1103/physrev.156.320

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We derive the equation of motion for the quantum-mechanical radiation density matrix of a gas laser to lowest order in the dimensionless coupling constant. Our derivation is fully quantum mechanical and we can calculate the coherence properties from the radiation density matrix. Our model consists of NNN two-level systems interacting with radiation in a cavity in the presence of dissipation, pumping, and collisions. The method we use is a generalization of the Bogoliubov derivation of the kinetic equation for a small parameter. Our derivation holds for any physically realizable pump power, and near threshold reduces to Lamb's near-threshold theory. With the equation of motion for the radiation density matrix, we obtain solutions both for when the average field is nonzero and for when it is zero. The steady-state electromagnetic density is the same in both cases except for a small spontaneous-emission term. We show that the reason gas lasers do not satisfy rate equations is the existence of zeroth-order correlations between the internal atomic variables and atomic center-of-mass variables. It is these same zeroth-order correlations which are responsible for the Lamb dip. Our derivation includes collisions and reduces the calculations of their effect to quadrature.
We derive the kinetic equations for the coupled single-particle density matrix $\ensuremath{\rho}$ and the electromagnetic density matrix RRR to lowest order in the dimensionless coupling constant ${\ensuremath{\beta}}^{2}\ensuremath{\equiv}{(\frac{{\ensuremath{\omega}}_{L}}{{\ensuremath{\omega}}_{D}})}^{2}$. The laser frequency ${\ensuremath{\omega}}_{L}$ is ${(4\ensuremath{\pi})}^{\ensuremath{-}\frac{1}{2}}{(\mathfrak{N}{r}_{0}{\ensuremath{\lambda}}^{2})}^{\frac{1}{2}}{\ensuremath{\omega}}_{0}$ where N\mathfrak{N}N is the number of two-level systems per unit volume, r0{r}_{0}r0​ is the classical electron radius, $\ensuremath{\lambda}$ is the wavelength of the radiation, and $k{\ensuremath{\omega}}_{0}$ is the two-level energy difference. The Doppler frequency ${\ensuremath{\omega}}_{D}$ characterizes the center-of-mass motion. For gas lasers ${\ensuremath{\beta}}^{2}$ is much less than 1 and, consequently, we generalize and use the Bogoliubov derivation of kinetic equations for weak interactions. We find solutions when the average field vanishes and which include spontaneous emission correctly. The single-particle density matrix and the radiation density matrix are coupled through their second moments. When we substitute the solution of the second-moment equations into the density-matrix equations, we find that each density matrix satisfies an uncoupled linear equation with known time-dependent coefficients. We introduce and discuss dissipation from the density-matrix point of view. With the use of the density-matrix formalism we indicate that the correct expansion parameter for higher order kinetic equations is ${\ensuremath{\beta}}^{2}$.
A quantum theory of two-photon correlated-spontaneous-emission lasers (CEL's) is developed, starting from the exact atom-field interaction Hamiltonian for cascade three-level atoms interacting with a single-mode radiation field. We consider the situation where the active atoms are prepared initially in a coherent superposition of three atomic levels and derive a master equation for the field-density operator by using a quantum theory for coherently pumped lasers. The master equation is transformed into a Fokker-Planck equation for the antinormal-ordering Q function. The drift coefficients of the Fokker-Planck equation enable us to study the steady-state operation of the two-photon CEL's analytically. We have studied both resonant two-photon CEL for which there is no threshold, and off-resonant two-photon CEL for which there exists a threshold. In both cases the initial atomic coherences provide phase locking, and squeezing in the phase quadrature of the field is found. The off-resonant two-photon CEL can build up from a vacuum when its linear gain is larger than the cavity loss (even without population inversion). Maximum squeezing is found in the no-population-inversion region with the laser intensities far below saturation in both cases, which are more than 90% for the resonant two-photon CEL and nearly 50% for the off-resonant one. Approximate steady-state Q functions are obtained for the resonant two-photon CEL and, in certain circumstances, for the off-resonant one.
We develop a fully quantum-mechanical theory for the organic-dye-solution laser, obtain density-matrix equations of motion for the single-mode radiation-density operator and the matter-density operator, and solve and investigate the steady-state case. We generalize the usual Born-Markoff approximation master equation for two matter states to include four matter states, each one of which interacts with the laser radiation field. This allows us to treat exactly the organic-dye molecular triplet-state levels which participate in the laser operation in an essential way. For experimentally realizable conditions the steady-state solution contains features which are qualitatively different from nondye lasers. These effects are directly attributable to intensity-dependent triplet-state radiation absorption losses. At threshold the diagonal matrix elements of the radiation photon distribution (Rn{R}_{n}Rn​) can be a decreasing function of the photon number nnn with an inflection point rather than the usual truncated Gaussian. This necessitates redefinition of threshold. For pumping just above threshold there may be both a maximum and a minimum in Rn{R}_{n}Rn​ rather than just a maximum as in usual laser theories. We also specify the effect of triplets on the narrowing of Rn{R}_{n}Rn​ for pumping above threshold and the subsequent widening of Rn{R}_{n}Rn​ for pumping well above threshold. Many of our results require photon-counting experiments for verification. Also, our equations are easily reducible to a semiclassical theory, where our treatment of the triplets variables is an improvement over the usual rate equations.
We generalize the method of deriving a kinetic equation for a gas laser developed in the first paper of this series to include radiation-matter correlations. As a consequence, we are able to show that the first Born approximation with asymptotic conditions which contain radiation-matter correlations is sufficient to explain the nonthermal photon distribution observed in photon-counting experiments. Our derivation includes the spatial and velocity effects of the motion of the gas atoms. After adiabatically eliminating the matter variables, we obtain a master equation for the radiation density matrix RRR with nonlinear coefficients. Our radiation master equation for stationary atoms without spatial effects is the same as the generalized Fokker-Planck equation of the Langevin-noise-equation treatment of lasers. We show that the generalized Fokker-Planck equation is the result of the first-Born-approximation treatment of the j\ifmmode\cdot\else\textperiodcentered\fi{}A interaction and is not dependent upon the microscopic structure of the reservoirs. In the first Born approximation, the diagonal and off-diagonal matrix elements of RRR do not interact with each other. Consequently, an initially diagonal radiation density matrix remains diagonal. However, we show that even though the stationary state is diagonal it is necessary to know the propagator of the off-diagonal part of RRR to answer time-dependent questions about quantities, such as the line shape, that depend on phase.
A quantum statistical analysis of an optical maser is presented in generalization of the recent semiclassical theory of Lamb. Equations of motion for the density matrix of the quantized electromagnetic field are derived. These equations describe the irreversible dynamics of the laser radiation in all regions of operation (above, below, and at threshold). Nonlinearities play an essential role in this problem. The diagonal equations of motion for the radiation are found to have an apparent physical interpretation. At steady state, these equations may be solved via detailed-balance considerations to yield the photon statistical distribution ${\ensuremath{\rho}}_{n,n}$. The resulting distribution has a variance which is significantly larger than that for coherent light. The off-diagonal elements of the radiation density matrix describe the effects of phase diffusion in general and provide the spectral profile ${| E(\ensuremath{\omega}) |}^{2}$ as a special case. A detailed discussion of the physics involved in this paper is given in the concluding sections. The theory of the laser adds another example to the short list of solved problems in irreversible quantum statistical mechanics.
This paper presents a semiclassical theory of a single-mode gas laser valid for essentially arbitrary values of field intensity. The theory is formulated in terms of an ensemble-averaged form of the density-matrix equations of motion involving a single set of coordinates. The polarization and the population-inversion density are expanded in spatial Fourier components. One obtains a set of coupled difference equations in the Fourier coefficients yn{y}_{n}yn​, which may be solved subject to appropriate boundary conditions on yn{y}_{n}yn​ for large nnn. The solutions may be expressed in terms of continued fractions in the general case, and in closed form in important special cases. Quantities of interest are evaluated by computer. The steady-state laser intensity and frequency are obtained from the coupled electromagnetic field equations as functions of the cavity parameters and the linear gain of the amplifying medium. At moderate values of field intensity, the velocity distribution of the space-averaged population inversion density exhibits a fine structure for low-velocity atoms superimposed on the usual broader depletion. This structure is a manifestation of the coherent ringing of the amplifying medium. The results are compared with those obtained in the rate-equation approximation, and with the recent work of Stenholm and Lamb. Discrepancies with the latter paper are explained.