Several calculations have been carried out using the transition operator technique. The radiative decay in a two-level quantum system with excited state coupled by an external perturbation has been investigated and an expression obtained for P(t), the probability of finding the atom in its excited state at time t. This is seen to possess a steady value for yt >> 1 and a third term which decays at nearly half the rate of its second. Next radiative decay of an atom with two close-lying excited states is considered and |bq| 2 , the spectral density for spontaneous emission from the uppermost level, calculated. This shows that the proximity of the upper two levels makes the line-shape non-Lorentxian. Heisenberg equations of motion were then derived for the transitions operators of an ℓ-level atom undergoing radiative decay, the possibility of overlapping pairs of levels being ignored. These master equations were then used to obtain the spectral profiles of certain atomic lines, employing the so-far avoided Markoff approximation. First the spectral density of the scattered radiation was found for transitions between levels 5P3/2 and 4S (ground state), and 6S and 5P 3/2, in the potassium atom when driving fields of arbitrary strength coupled levels 6S and 4P3/2, and 4P 3/2 and 4S. Triple-peaked profiles were obtained. Spectral profiles for emission were then derived for transitions between levels 3P and (ground state), and 3P and in the hydrogen atom when a driving field of arbitrary strength coupled levels The former profile was double the latter quadruple-peaked. Lastly master equations were derived for an atom, with two excited levels undergoing radiative decay, when allowance was made for thepossibility of their overlapping. A driving field of arbitrary magnitude coupled the uppermost and ground states. The spectrum for the scattered light resulting from transitions between the uppermost and ground state was found and graphs computed for various field strengths and separations of the excited states.
A two-state atom in a perturber gas is irradiated by intense light with an arbitrary spectral profile. The authors derive a general expression for the fluorescence spectrum in terms of the conventional low-intensity absorption profile and the spectral density of the incident light. This result, which contains previous results as special limiting cases, describes the transition from the three-line fluorescence spectrum excited by intense monochromatic light and the power-broadened Lorentzian spectrum produced by broad-band excitation.
The spectral densities of Einstein coefficients for absorption and stimulated emission in a two-level quantum system are not equal to each other beyond the absorption (emission) line if the homogeneous broadening caused by interaction with a thermostat is much larger than the natural width. In this study, a relationship between these coefficients is derived on the basis of general thermodynamic requirements. This relationship is associated with new effects such as population inversion upon the nonresonant absorption of continuous radiation and radiation amplification without population inversion.
Abstract The development with time of the excitation of a transition between two atomic or molecular energy levels under the influence of monochromatic laser radiation is examined under conditions of strictly homogeneous line-broadening. The ratio of the number of atoms or molecules, N2, in an excited state to the total number, N, is calculated for various ratios of the intensity parameter β ═ E0μ/ħ to the half line-width γ. E0 is the amplitude of the electric field in the incident radiation and the dipole moment matrix element for the transition. Exact expressions for N2/N as a function of time are given for the situation when the frequency ω/2π of the radiation is exactly equal to that of the transition ω0/2π. Numerical calculations are made for the situation when the ‘detuning’ δ ═ ω — ω0 is not equal to zero. Approximate expressions are also derived in terms of δ for use in a later paper which deals with mixed homogeneous and inhomogeneous line-broadening.
A general theory of spontaneous emission was developed in Papers I and II of this series. In the present paper, the mastre equation describing spontaneous emission from
N identical two-level atoms is investigated further. It is shown that the equation of motion for the
p(<N)-atom density matrix is coupled to the (
p+1)-atom density matrix. We first consider the initial excitation of the system to state $|{\ensuremath{\theta}}_{0},{\ensuremath{\phi}}_{0}〉$ (${\ensuremath{\theta}}_{0}<\ensuremath{\pi}$) and solve the hierarchy of equations so obtained in the "uncorrelated approximation." It is found that the presence of other atoms is equivalent to an external field which is determined from a self-consistent analysis. It is also found that in this approximation the state of the atom at time
t can be described by a single parameter $\ensuremath{\theta}(t)$ ($\ensuremath{\theta}<\ensuremath{\pi}$), with ${sin}^{2}\frac{1}{2}\ensuremath{\theta}$ giving the probability that the atom is to be found in the excited state. Next, some improvements over the uncorrelated approximation are given. This is done by decoupling the equation of motion for higher-order mean values. It is found that the fluctuation $〈({S}_{i}^{Z}\ensuremath{-}〈{S}_{i}^{Z}〉)({S}_{j}^{Z}\ensuremath{-}〈{S}_{j}^{Z}〉)〉$ for any pair of atoms is of the order of
N1. The case when ${\ensuremath{\theta}}_{0}=\ensuremath{\pi}$ is considered separately and we obtain an expression for the radiation rate by making a "Hartree-Fock" type of approximation on the two-particle mean values. In this case, the behavior of the radiation rate is found to differ markedly from the "sech" behavior. It is then shown that the entire dynamics of two-level atoms emitting spontaneously can be described by a set of
2N coupled first-order equations which clearly exhibit the type of nonlinearity (which is the analog of the van der Pol type of nonlinearity) for this problem and provide a better understanding of spontaneous emission. Finally in Sec. V, the theory is extended to include the effects of inhomogeneous broadening, and the functional dependence of the radiation rate on the atomic-line-shape factor is obtained.