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Physical Review

Field-Correlation Effects in Two-Photon Processes

P. Lambropoulos

Published Apr 25, 1968• 51 citations
Publisher

Abstract

The rate of two-photon absorption from an arbitrary state of the radiation field, and its dependence on the statistical properties of the field, are studied. It is found that when the density operator of the field factors into a product of single-mode density operators (in which case the modes are statistically independent), the rate depends on the spectral composition of the field. When the density operator is nonfactorable, the process depends on a photon doublet density. Therefore, the information obtained from two-photon experiments in the first case can, in principle, also be obtained from single-photon counting, while in the second case it would require coincidence counting.

DOI
10.1103/physrev.168.1418

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Physical Review•Nov 1, 1968•212 citations
The rate of two-photon absorption from an arbitrary state of the radiation field, and its dependence on the statistical properties of the field, are studied. It is found that when the density operator of the field factors into a product of single-mode density operators (in which case the modes are statistically independent), the rate depends on the spectral composition of the field. When the density operator is nonfactorable, the process depends on a photon doublet density. Therefore, the information obtained from two-photon experiments in the first case can, in principle, also be obtained from single-photon counting, while in the second case it would require coincidence counting.
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 nthn\mathrm{th}nth-order time-dependent perturbation theory, that the multiphoton absorption probability depends on the (n,n)th(n, n)\mathrm{th}(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 nnn! 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 nnn-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 relation between the two-quantum photocounting distribution p(n, T) and the intensity fluctuations of the radiation incident on the detector is obtained and compared with the one-quantum results. The actual statistics are evaluated for several cases of interest, including a chaotic source, an amplitude-stabilized wave, and the output of a single-mode laser (Van der Pol oscillator). The two-quantum count rate 〈n〉/T is found to depend on the mean-square intensity of the radiation, in contrast to the one-quantum count rate which is proportional to the mean intensity. The effects of photon correlations in the radiation beam become apparent since the two-quantum distributions manifest a distinctly more positive second derivative than the corresponding one-quantum distributions. Both the low-and the high-count probabilities are therefore increased at the expense of counts near the mean. The quantum-theoretical treatment is found to be equivalent to the semiclassical treatment for density operators possessing a positive-definite weight function in the P-representation. Some possible experiments to verify the theory are discussed and shown to be feasible.
A theory of a quantum amplifier based on two-photon transitions is presented. The model consists of an assemblage of atoms interacting with a single mode of the light field via two-photon absorption and emission. The treatment is quantum mechanical, and the emphasis is on the photon-statistical aspects of the problem. Difference-differential equations for the density matrix of the field mode are derived. The equations are solved for a special case. Differential equations for the expectation vaues of the number of photons and of the field amplitudes, and for their higher statistical moments, are also obtained. Approximate solutions for the average number of photons are found, and the effect of the amplification process on the statistical fluctuations of the number of photons and the field amplitudes is discussed. The results of this study suggest that such an amplifier does not have the coherence properties of a laser amplifier because it tends to increase the statistical fluctuations of the field.
The two-photon absorption process is discussed using a density matrix formalism. The electromagnetic field is described by means of coherent states, a technique that permits a simple evaluation of the effect of coherence on the transition probability. It is concluded that the latter is the same for a coherent and an incoherent pulse of radiation. In the case of a stationary field containing many modes, the transition probability is nearly the same in the coherent and incoherent cases, whereas for a single mode the transition probability is twice as high for the incoherent field. These conclusions are independent of the multipole expansion of the interaction Hamiltonian and are valid for electric dipole and higher multipole transitions.
The probability of an atom undergoing a transition to a given final state by means of two-photon absorption is expressed for arbitrary field states in terms of the second-order normally-ordered field correlation function, evaluated at the position of the atom. In the case of stationary fields, an expression for the absorption rate is found which reduces to a particularly simple form for narrow-bandwidth fields near resonance. The effect of field statistics is illustrated by comparing the absorption rate w2(ch)w_{2}^{}{}_{}{}^{(\mathrm{ch})}w2​​(ch) for chaotic or Gaussian light to the rate w2(l)w_{2}^{}{}_{}{}^{(l)}w2​​(l) for laser light. The rate for laser light is calculated within the context of a particular model based on the assumption of fixed field amplitude and random frequency modulation, and the chaotic light to which it is compared is assumed to have the same (Lorentzian) power spectrum. When the width ${\ensuremath{\kappa}}_{f}$ of the final atomic level is much greater than the bandwidth bbb of the field, we obtain the previously derived result w2(ch)w2(l)=2\frac{w_{2}^{}{}_{}{}^{(\mathrm{ch})}}{w_{2}^{}{}_{}{}^{(l)}}=2w2​​(l)w2​​(ch)​=2. When ${\ensuremath{\kappa}}_{f}\ensuremath{\ll}b$, on the other hand, the ratio between the two rates depends on the (mean) frequency of the field, and assumes the (maximum) value 4 when the field is exactly on resonance.