Applying a space translation operation, the Schrodinger equation for an atom in an electromagnetic field is solved with sufficient accuracy to obtain probabilities for multiple absorption of photons from a monochromatic laser beam of arbitrary intensity or frequency. It is shown that the derived expression for the N-photon T-matrix contains the usual single photon matrix elements given by the perturbation theory and that the perturbative result is obtained in the limit of low intensity. Other explicit examples are considered. The conditions of applicability of the method are specified.
Applying a space translation operation, the Schrodinger equation for an atom in an electromagnetic field is solved with sufficient accuracy to obtain probabilities for multiple absorption of photons from a monochromatic laser beam of arbitrary intensity or frequency. It is shown that the derived expression for the N-photon T-matrix contains the usual single photon matrix elements given by the perturbation theory and that the perturbative result is obtained in the limit of low intensity. Other explicit examples are considered. The conditions of applicability of the method are specified.
The dependence of the multiphoton absorption probability for an atomic system on the statistical properties of the incident light is investigated. It is shown, by means of nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the (n,n)th normally ordered correlation functions of the electromagnetic field. For stationary fields, the transition probability per unit time is constant and is directly related to the reduced cross-spectral correlation function of the electromagnetic field. This expression for the transition probability is then analyzed under various conditions of coherence. Explicit calculations are carried out for thermal light and for laser light, and the transition rates are compared when each has a Lorentzian spectrum. In particular, when the width of the final atomic level is much larger than the bandwidth of the field, the transition rate for thermal light is n! times higher than with laser light of the same mean intensity. The other extreme case, i.e., when the width of the final atomic level is much smaller than the bandwidth of the field, is also considered in detail. An equation for the density operator of the field is derived; this equation governs the change in the statistical properties of the photon system in n-photon absorption processes. On the basis of this equation, the time-dependent properties of the photon system are then studied and some physical consequences of these equations are discussed. Some numerical solutions relating to the time dependence of the factorial moments in two-photon absorption processes are presented.
The physics of the two-photon absorption process is investigated for a three-state system. The density-matrix equations for the two-photon interaction are solved in the steady-state limit assuming that the pump laser radiation is monochromatic. Collisional broadening, saturation, and Stark shifting of the two-photon resonance are investigated in detail by numerical solution of the steady-state density-matrix equations. Analytical expressions for the saturation intensity and the Stark shift are derived for the case where the single-photon transitions between the intermediate state and the initial and final states are far from resonance with the pump laser. For this case, it is found that the direction of the Stark shift is dependent on the relative magnitudes of the dipole-moment matrix elements for the single-photon transitions that couple the intermediate state with the initial and final states. Saturation and Stark shifting are also investigated for the case where the single-photon transitions between the intermediate state and the initial and final states are close to resonance with the pump laser.
The interaction is considered between N stationary two-level atoms and a radiation field described by a single cavity mode. The state vector for the complete system of atoms plus radiation is expressed as a linear superposition of states constructed from a product of photon states in the n representation and products of Pauli spin eigenstates describing all combinations of atoms in the lower and upper energy levels. Equations for the corresponding probability amplitudes are derived by substituting this superposition into the Schr\"odinger equation. The resulting equations are combined into bilinear form and phenomenological damping contributions are added. After the neglect of certain of the bilinear quantities, a master equation is derived which governs the probability Pmn of having m atoms in the lower level and n photons in the mode. This master equation takes account of multiple single-quantum absorption and emission processes but not of simultaneous multiple processes involving two or more atoms at a time. The equation which governs the expected number of photons 〈n〉 derived from the master equation bears a close resemblance to a rate equation. The effect of radiation loss from the cavity is incorporated into the master equation. Numerical calculations for a Q-spoiled laser show that the statistics of the number of photons in the mode bear a qualitative resemblance to Poisson statistics.
Two-photon absorption is theoretically analyzed within the semiclassical formalism of radiation-matter interaction. We consider an ensemble of inhomogeneously broadened three-level atoms subjected to the action of two counterpropagating fields of the same frequency. By concentrating in the limit of large detuning in one-photon transitions, we solve perturbatively the Bloch equations in a non-usual way. In this way we derive an analytical expression for the width of the two-photon resonance that makes evident sub-Doppler two--photon spectroscopy. We also derive an analytical expression for the Stark shift of the two-photon resonance.
Abstract The quantum mechanical description of the interaction of light with atoms treats absorption, gain, and recombination as upward and downward induced transitions of electrons between two states by perturbation due to the optical electric field. This provides the basis for a quantitative theory of diode lasers. The chapter begins with Einstein’s description of absorption, stimulated emission, and spontaneous emission, setting the scene for calculation of the transition probability by solving the time-dependent Schrödinger equation for a coherent superposition of the wavefunctions of two states. The resulting absorption spectrum has a Lorentzian lineshape due to dephasing of these wavefunctions. Expressions for the optical absorption cross section and Einstein coefficients are derived in terms of the dipole matrix element, and the dipole is illustrated using a hypothetical one-dimensional atom. Fermi’s Golden Rule for transitions to a continuum of states (as in quantum wells) is introduced in terms of the momentum matrix element.
The rate of absorption and emission of radiation is calculated for two laser fields interacting with a homogeneously broadened, three-level molecular system. The time-dependent Schrödinger equation is used in the density matrix formalism and the laser fields are treated classically. The laser fields, at frequencies ωpand ωs, are off resonance by δpand δs, respectively, such that|\delta_{p}|, |\delta_{s}| \ll \omega_{p}, \omega_{s}. Analytic expressions are derived for the imaginary part of the electric susceptibility,\chi"(\omega_{p})and\chi"(\omega_{s}). The present work differs from previous calculations in that the laser fields may have arbitrary values of field strength and each field may be on or off resonance. A discussion is presented of the properties of the solutions for\chi"(\omega_{p})and\chi"(\omega_{s}), for both strong and weak laser fields, based on computer evaluation of the general analytic expressions. It is shown that the solutions may be divided into single-photon and two-photon, or Raman, contributions. Conditions for optimizingdI(\omega_{s})/dzand the photon conversion efficiency are derived. These results may be applied to analyzing the pulsed, optically pumped submillimeter laser and to studying two-photon absorption in a gas.