Abstract An error in the author's previous treatment of the interaction of an absorber with high intensity light is noted. The correct development of Mower is applied to determine the amplitude of the initial state of the radiation‐matter system. Comparison of the quantum theory solution for a damped absorber exposed to a square light pulse with the results of semiclassical theories based on the undamped optical Bloch equations is effected by determining the effective in‐ and out‐of‐phase components of the transition dipole response. In general, the out‐of‐phase (or absorptive) part of the transition dipole is zero at the outset and strongly time‐dependent at short times, evolving to a steady‐state value at longer times. For resonance radiation the system exhibits either overdamped irreversible decay or underdamped oscillations, depending upon the relative magnitudes of the incident light intensity and the radiative damping rate. Specific results are presented for a variety of limiting values of the physical parameters, including light intensity, damping rate, and amount of off‐resonance.
Abstract An error in the author's previous treatment of the interaction of an absorber with high intensity light is noted. The correct development of Mower is applied to determine the amplitude of the initial state of the radiation‐matter system. Comparison of the quantum theory solution for a damped absorber exposed to a square light pulse with the results of semiclassical theories based on the undamped optical Bloch equations is effected by determining the effective in‐ and out‐of‐phase components of the transition dipole response. In general, the out‐of‐phase (or absorptive) part of the transition dipole is zero at the outset and strongly time‐dependent at short times, evolving to a steady‐state value at longer times. For resonance radiation the system exhibits either overdamped irreversible decay or underdamped oscillations, depending upon the relative magnitudes of the incident light intensity and the radiative damping rate. Specific results are presented for a variety of limiting values of the physical parameters, including light intensity, damping rate, and amount of off‐resonance.
Abstract A function analogue of the formal operator theory of Goldberger and Watson for the decay of prepared states is developed with a modification that permits treatment of degenerate, interacting intermediate states. The theory is applied to the problem of absorption of radiation by an absorber in a very intense monochromatic beam. In particular, a simple two‐level absorber in a resonant monochromatic beam of sufficient intensity to induce transitions from the ground state at a rate exceeding the spontaneous emission rate from the excited state, but still lying well below the optical frequency characterizing the transition, is investigated with the conclusion that the absorption cross‐section falls off with the one‐half power of the incident intensity. Conditions for the possible experimental verification of this result are presented.
Radiation can change the energy state of matter via three optical processes: spontaneous emission, absorption and stimulated emission. In spontaneous emission, an excited atomic or molecular state decays to a lower energy state with the emission of a photon of energy equal to the difference in the quantum state energies. Photon absorption is the reverse process, with a photon causing excitation from a lower to an excited quantum state. Stimulated emission was first proposed by Einstein in a paper published in 1917. He attempted to balance spontaneous emission and photon absorption, but could not get the correct balance without the postulated process of stimulated emission (see Section 4.2). With stimulated emission, an excited quantum state is stimulated to decay to a lower quantum state by an impinging photon. The existing photon survives with another identical photon being created (so that energy is conserved). The rates at which radiative transitions occur can be calculated using quantum mechanics. The time-dependent Schrodinger equation is used with the system wavefunction comprising time-varying linear combinations of the two wavefunctions for the lower and upper quantum states. In semi-classical treatments, an atom is treated quantum mechanically with the radiation field treated classically. There is a perturbation in energy associated with, say, the electric field of the radiation interacting with the electric dipole of the atom, though other interactions can be significant if the electric dipole interaction energy is small. In absorption, for example, a differential equation representing the change in ‘weighting’ of the wavefunction from the lower to upper state is obtained. A ‘time constant’ for the speed of change represents the rate of the radiative process. We examine the quantum mechanical nature of radiation absorption in Section 10.1 before discussing (Section 10.3) another important parameter arising with radiative transitions between discrete bound quantum states: the lineshape function. Quantum Theory of the Atom–Radiation Interaction An expression for the Einstein B-coefficient for photo-absorption is derived using quantum mechanics in this section. Einstein determined the detailed balance relationship between the rates of spontaneous emission, photo-absorption and stimulated emission when light interacts with an atom by considering an atomic system of two energy levels which are in equilibrium with a black-body radiation field. We use a semi-classical treatment where the atom is treated quantum mechanically and the radiation field is treated as a classical oscillating electric field.
Abstract The atom-field interaction is treated in semiclassical radiation theory, starting from the transformation from the minimal coupling Hamiltonian to the electric dipole form used extensively in quantum optics. The Heisenberg and density matrix approaches are developed and applied to two-state atoms, Bloch equations, Rabi oscillations, Maxwell-Bloch equations, and transition rates for absorption and emission. Einstein’s theory of blackbody radiation based on momentum fluctuations and dissipation is reviewed. The Einstein fluctuation formula is derived and used to introduce wave-particle duality, Hanbury Brown-Twiss correlations, and photon bunching.
This paper has two purposes: 1) to clarify the relationship between the quantum theory of radiation, where the electromagnetic field-expansion coefficients satisfy commutation relations, and the semiclassical theory, where the electromagnetic field is considered as a definite function of time rather than as an operator; and 2) to apply some of the results in a study of amplitude and frequency stability in a molecular beam maser. In 1), it is shown that the semiclassical theory, when extended te take into account both the effect of the field on the molecules and the effect of the molecules on the field, reproduces almost quantitatively the same laws of energy exchange and coherence properties as the quantized field theory, even in the limit of one or a few quanta in the field mode. In particular, the semiclassical theory is shown to lead to a prediction of spontaneous emission, with the same decay rate as given by quantum electrodynamics, described by the Einstein A coefficients. In 2), the semiclassical theory is applied to the molecular beam maser. Equilibrium amplitude and frequency of oscillation are obtained for an arbitrary velocity distribution of focused molecules, generalizing the results obtained previously by Gordon, Zeiger, and Townes for a singel-velocity beam, and by Lamb and Helmer for a Maxwellian beam. A somewhat surprising result is obtained; which is that the measurable properties of the maser, such as starting current, effective molecular Q, etc., depend mostly on the slowest 5 to 10 per cent of the molecules. Next we calculate the effect of amplitude and frequency of oscillation, of small systematic perturbations. We obtain a prediction that stability can be improved by adjusting the system so that the molecules emit all their energy h Ω to the field, then reabsorb part of it, before leaving the cavity. In general, the most stable operation is obtained when the molecules are in the process of absorbing energy from the radiation as they leave the cavity, most unstable when they are still emitting energy at that time. Finally, we consider the response of an oscillating maser to randomly time-varying perturbations. Graphs are given showing predicted response to a small superimposed signal of a frequency near the oscillation frequency. The existence of "noise enhancing" and "noise quieting" modes of operation found here is a general property of any oscillating system in which amplitude is limited by nonlinearity.
The spontaneous-emission rate of a radiating atom reaches its time-independent equilibrium value after an initial transient regime. In this paper, we consider the associated relaxation effects of the spontaneous-decay rate of atoms in dispersive and absorbing dielectric media for atomic-transition frequencies near material resonances. A quantum mechanical description of such media is furnished by a damped-polariton model in which absorption is taken into account through coupling to a bath. We show how all field and matter operators in this theory can be expressed in terms of the bath operators at an initial time. The consistency of these solutions for the field and matter operators are found to depend on the validity of certain velocity sum rules. The transient effects in the spontaneous-decay rate are studied with the help of several specific models for the dielectric constant, which are shown to follow from the general theory by adopting particular forms of the bath coupling constant.
We model the response of a molecular medium to an intense pulse of light. We begin by reducing the Maxwell-Bloch equations for a multilevel molecular model system to a set of simplified propagation equations. We thereby obtain expressions for the frequency, temperature, and field intensity dependence of the ground and excited electronic state absorption cross sections, and the emission cross section, as well as the temperature dependence of the decay rate of the excited state. The phenomena of saturation, excited-state absorption, optically induced dichroism and birefringence, vibronic energy transfer, induced molecular alignment, decay of the matter-field interaction energy, and rotational diffusion are considered within the general formalism for describing the propagation of an intense pulse of light in the molecular medium. We find that the cross section for absorption (emission) of a photon is not identical to the cross section for molecular excitation (deexcitation) via the matter-field interaction. This is explained in terms of an energy balance between the matter, radiation, the matter-radiation interaction, and the bath responsible for the broadening of the molecular transitions. The inequality of these cross sections determines whether the system supplies or draws energy from the thermal bath. The rise in the vibrational temperature of molecules subjected to an intense short pulse is shown to significantly affect propagation of the pulse. The alignment of the molecular system resulting from saturation of the ground-state transition by a polarized laser pulse and the effects of the orientational dependence of the matter-field interaction including effects of rotational diffusion are determined. As an example of the formalism we consider pulse propagation in a Rhodamine 6G solution. We fit the parameters of the model to determine the frequency dependence of the ground- and excited-state absorption cross sections and the emission cross section and compare with experimentally determined cross sections. We describe the propagation of a pulse whose temporal width is comparable to the rotational diffusion time of the molecules in the dye solution and calculate polarization pulse probe signals.