A large number of "molecules," which are taken to be angular momentum oscillators of frequency $\ensuremath{\nu}$, are considered to interact through their dipole moment with two electromagnetic cavity modes of frequencies ${\ensuremath{\omega}}_{1}$ and ${\ensuremath{\omega}}_{2}$, respectively, where $\ensuremath{\nu}={\ensuremath{\omega}}_{1}\ifmmode\pm\else\textpm\fi{}{\ensuremath{\omega}}_{2}$. The behavior of the combined system is analyzed up to fourth order in perturbation theory. Phenomena known as two-photon emission or absorption, parametric amplification, various types of Raman emission, and frequency conversion are exhibited. The analytical method used is applicable to both a quantum-mechanical and a classical description of the modes and molecules; it displays explicitly the resulting differences. Expressions for the rate of energy change of the modes and molecules indicate resonance in second and fourth order. The second-order results are the same for the classical and quantum-mechanical treatments, while the fourth-order results show certain differences, which are examined in detail. The conditions under which each of the above phenomena occurs are discussed in a self-consistent manner, both classically and quantum-mechanically. It is shown that the second-order expression and the most significant part of the fourth-order expression can be derived very simply from a resonance interaction Hamiltonian that consists of a sum of products of three variables---two referring to the two modes, and the third to the molecules. The relationship between this resonance Hamiltonian and the fundamental dipole-moment Hamiltonian is examined, and the approximations by which the resonance Hamiltonian may be derived are considered. Arguments concerning the applicability of perturbation theory to steady-state situations are presented; it is pointed out that the second-order expressions for the energy transfer between molecules and field may be applicable to such a situation, in which case the classical and quantum-mechanical treatments are equivalent.
A large number of "molecules," which are taken to be angular momentum oscillators of frequency \ensuremathν, are considered to interact through their dipole moment with two electromagnetic cavity modes of frequencies \ensuremathω1 and \ensuremathω2, respectively, where \ensuremathν=\ensuremathω1\ifmmode±\else\textpm\fi\ensuremathω2. The behavior of the combined system is analyzed up to fourth order in perturbation theory. Phenomena known as two-photon emission or absorption, parametric amplification, various types of Raman emission, and frequency conversion are exhibited. The analytical method used is applicable to both a quantum-mechanical and a classical description of the modes and molecules; it displays explicitly the resulting differences. Expressions for the rate of energy change of the modes and molecules indicate resonance in second and fourth order. The second-order results are the same for the classical and quantum-mechanical treatments, while the fourth-order results show certain differences, which are examined in detail. The conditions under which each of the above phenomena occurs are discussed in a self-consistent manner, both classically and quantum-mechanically. It is shown that the second-order expression and the most significant part of the fourth-order expression can be derived very simply from a resonance interaction Hamiltonian that consists of a sum of products of three variables---two referring to the two modes, and the third to the molecules. The relationship between this resonance Hamiltonian and the fundamental dipole-moment Hamiltonian is examined, and the approximations by which the resonance Hamiltonian may be derived are considered. Arguments concerning the applicability of perturbation theory to steady-state situations are presented; it is pointed out that the second-order expressions for the energy transfer between molecules and field may be applicable to such a situation, in which case the classical and quantum-mechanical treatments are equivalent.
Conceptual problems in quantum optics are investigated by a study of the physical significance of various types of description of the field of a single mode. The descriptions are examined through the effect of the field on matter. Both undamped and damped modes are considered, the descriptions being those of various degrees of precision in classical and quantum-mechanical formalisms. The matter consists of a large number of "molecules," and the interaction is studied by means of low-order perturbation theory. Formal expressions are obtained for the energy interchange between field and molecules in terms of the zeroth-order (uncoupled) operators, with the effect of the commutation properties of the field variables explicitly separated from that of the excitation of the field, in second order. The significance of taking expectation values of the operator results is discussed, and it is concluded that this procedure is justified only when the experiment under consideration involves an averaging process; thus, the molecular variables should be averaged, but not necessarily those of the field. Conditions under which the averaging process is justified are considered, and it is reasoned that, when such a process is not justified, a statistical description of the field can result only in a statistical description of the interaction process. Results of various field descriptions are compared, and it is shown that for induced emission and for spontaneous emission from coherently oscillating molecules, classical and quantum-mechanical fields are equivalent. However, for a self-consistent theory of spontaneous emission from molecules that are not oscillating coherently, the quantum-mechanical commutation properties of the field are essential if the molecules are treated quantum-mecahnically, and the field must be treated classically if the molecules are treated classically; the type of description used for the excitation of the field is inconsequential. Photoelectric emission is examined, and, within the approximation framework used, shown to be accurately described by a classical treatment of the field. It is pointed out that there does not necessarily exist a connection between "photon statistics," that is, the statistics associated with an ensemble of fields, and photocurrent fluctuations in one or more detectors coupled to the same field.
The theory developed in the first two articles of this series, dealing with the interaction between the electromagnetic field in a cavity resonator and a number of two-level molecules, is generalized to include a Gaussian spread in the molecular frequency. The center of the molecular frequency distribution coincides with the cavity resonant frequency. There is a coherent driving field in the cavity at the same frequency, and cavity loss is taken into account.Using the formalism previously developed for a quantum-mechanical field in a lossy cavity, expressions are obtained by means of second-order perturbation theory for the expectation values of the field strength and field energy in the cavity, and of the power loss by the molecules. It is shown that the parts of the field energy resulting from induced and spontaneous emission, respectively, initially increase as the square of the time and approach steady-state values after (different, in general) transient periods, each of which is determined by two time constants: cavity relaxation time and inverse molecular frequency spread.It is also shown that both the induced and spontaneous emission power radiated by the molecules increase initially linearly with the time and approach steady-state values after transient periods. For the induced emission power, the transient period is determined by only one time constant, the inverse molecular frequency spread, while for the spontaneous emission power it is determined both by the inverse molecular frequency spread and the cavity relaxation time. The ratio of induced to spontaneous emission is initially n, and approaches a steady-state value $n{[\mathrm{exp}({r}^{2})(1\ensuremath{-}\mathrm{erf}r)]}^{\ensuremath{-}1},$ where n is the driving field energy in units of the photon energy, and r is the ratio of the cavity resonance width to molecular frequency spread. The seeming inconsistency of this value with the classical value of the ratio of the Einstein coefficients is discussed.
The isolation usually encountered in optics between the part of a field that is of interest and its source motivates the consideration of a radiation mode weakly coupled to a quantum-mechanical source. After the introduction of some refinements into the quantum mechanics of a damped radiation mode, the field is expressed as the sum of two parts, one due to the source (the source field) and the other due to the loss mechanism (the "vacuum" field). The characteristic function for the field is calculated up to second order in perturbation theory. This function is then compared with the characteristic function for the field in the presence of a classical source. A method is exhibited by which a classical source can be found such that the two characteristic functions are identical when averaged over a half cycle. In particular, the two sources yield the same expectation values for the instantaneous amplitude and energy of the field. The description of the equivalent classical source must be given in statistical terms, in general, and requires only a knowledge of 〈S(0)(t)〉 and 〈S(0)(t1)S(0)(t2)〉, where S(0) is the dipole-moment operator of the quantum-mechanical source unperturbed by the mode under consideration (but otherwise arbitrarily complex, with the possibility of strong coupling to other modes). The theory is illustrated by a consideration of several simple sources---a two-level system, a harmonic oscillator, and a blackbody---for which equivalent classical sources are found. The two-time correlation functions for the field obtained with the two types of sources are compared and are shown to be the same up to first order in $\ensuremath{\xi}\ensuremath{\tau}$, where $\ensuremath{\tau}$ is the difference between the two times and $\ensuremath{\xi}$ is the inverse of the field relaxation time; the physical meaning of the second-order difference in the correlation functions is discussed. A limiting process, in which both the coupling to the source and the damping become small, is suggested as a method of adapting the results to free fields, but it is pointed out that for discussion of a single mode, a free field is physically less satisfactory than a damped field. It is concluded that, within a reasonable approximation scheme, the source field may be described classically (the "vacuum" field furnishing all the necessary quantum-mechanical properties of the total field).
In the previous articles of this series, dealing with the interaction between a number of molecules and the electromagnetic field in a resonant cavity, both the molecules and the field were treated by perturbation theory. The perturbation restriction on the field is removed in the present article, allowing large changes in the field, but the molecules are still assumed to undergo a small change during the time under consideration. The justification for this type of analysis, involving the generalization of the conventional concepts of induced and spontaneous emission, the applicability to a molecular amplifier during the buildup period, and the re-examination of a calculation by Serber and Townes concerning the fundamental limits of molecular amplification, is discussed.Two different molecular distributions are considered. In one (the resonant case) all molecules have the same frequency as the cavity, and in the other (the nonresonant case) there is a uniform frequency distribution. The molecules are assumed to be initially in an emissive state. Several types of driving fields are considered. Expressions are obtained for the field operators by the solution of a Volterra integral equation, and expectation values are obtained for the field strength and field energy.In the resonant case, both the coherent and incoherent fields increase exponentially after a sufficiently long time, no matter how small the initial gain is. Their ratio becomes constant and is equal to the number of photons in the driving field only in the absence of dissipation. An interesting related result is the fact that the signal-to-noise ratio for constant signal input power increases as the cavity dissipation increases. An estimate of the total time for which the theory is valid is obtained from a consideration of the energy emitted by the molecules. Contact is made with perturbation theory for sufficiently small gain and short time.In the nonresonant case the effect of the molecules is shown to be that of a negative dissipation. In contrast to the resonant case, the gain becomes exponential only if the negative dissipation exceeds, in absolute value, the true dissipation. The ratio of induced to spontaneous emission is, in this case also, equal to the number of photons in the driving field only in the absence of disipation. However, the signal-to-noise ratio for constant input power drops with increasing cavity dissipation.
The multiple-linear-time-scale method is used to construct a perturbation theory for N-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2), the approximate solution is valid for many thousands of Rabi cycles.
Fock states and coherent states have been widely applied in analyses of quantum-optics experiments. In this paper, the application of a set of basis functions that consist of a product of displaced harmonic-oscillator states for the electromagnetic field and atomic states that are eigenfunctions of the momentum operator will be explored. For the case of a single mode, these states are the exact eigenfunctions in the limiting case where the electromagnetic-field mode frequency is much larger than the atomic transition frequency. This choice of basis functions will be used to analyze the interaction of a nonrelativistic, ``two-level'' atom with a single-frequency, quantized electromagnetic-field mode. Since in this basis the sign of the displacement of the electromagnetic-field state depends on the state of the atom, these new basis wave functions exhibit explicitly some aspects of atom-field correlations that are intrinsically quantum mechanical in nature. The analysis will be performed in the electric-dipole approximation for an atomic system that obeys the \ensuremath{\Delta}m=0 selection rule. The rotating-wave-approximation (RWA) terms cannot be made negligible through judicious choice of the field polarization for this system. The diamagnetic term, e2A2/2mc2, which is of the same order of magnitude as the RWA terms, is taken into account exactly by slightly modifying the traditional approach to quantizing the electromagnetic field. In this way the physical effects of the diamagnetic term are absorbed into a new electromagnetic cavity mode frequency.An approximate expression for the combined system's energy eigenvalues is found up to third order in the ratio of one-half the atomic transition frequency to the mode frequency. This expression indicates that inclusion of the RWA terms adds a small ``ripple'' on top of the smoothly varying energy eigenvalues when they are plotted as a function of the atom-field coupling constant. The ripple is interpreted as ``interference'' between two displaced oscillator-field states that represent the unperturbed state. When the Fock states are used as the basis for expanding the wave function of this system, a formidable five-term recurrence relation results. However, expanding the wave function in terms of the displaced harmonic-oscillator basis results in a less formidable three-term recurrence relation for the quantum coefficients.