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Physical Review

Two-Photon Absorption and Field Correlation Functions

B. R. Mollow

Published Nov 1, 1968• 212 citations
Publisher

Abstract

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 $w_{2}^{}{}_{}{}^{(\mathrm{ch})}$ for chaotic or Gaussian light to the rate $w_{2}^{}{}_{}{}^{(l)}$ 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 $b$ of the field, we obtain the previously derived result $\frac{w_{2}^{}{}_{}{}^{(\mathrm{ch})}}{w_{2}^{}{}_{}{}^{(l)}}=2$. 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.

DOI
10.1103/physrev.175.1555

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•Jan 1, 1980•1 citation
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 \ensuremathκf{\ensuremath{\kappa}}_{f}\ensuremathκf​ 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 \ensuremathκf\ensuremath≪b{\ensuremath{\kappa}}_{f}\ensuremath{\ll}b\ensuremathκf​\ensuremath≪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.
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.
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Under usual laboratory conditions the absorption of a beam of light by a dilute two-level medium depends on the intensity and spectrum of the incident light. If the incident photon flux is small compared to the decay rate of the absorber’s excited state, saturation effects can be neglected and only the spectrum of the light is important; thus, weak-field absorption depends only on the firstorder correlation function of the incident light. This result relies, however, on a requirement that the incident beam cross-section be much larger than the absorption cross-section of an atom. Then individual atoms act as low efficiency scatterers and the statistics of the scattering process is governed by the law of large numbers applied to many scattering sites. In contrast, if it is arranged that just one atom significantly absorbs (scatters) a beam of photons, correlation functions of the incident light beyond the first-order must be considered. For a beam that is focused within an absorption cross-section, we might naively predict that every photon will be scattered and none transmitted. In fact, even for a very weak beam there is a finite probability for two photons to arrive at the atom within the excited state lifetime, and in this event at least one of them will be transmitted (statistical saturation). In this paper we calculate the transmitted photon flux for a weak beam of photons focussed strongly onto a single, resonant two-state atom. We study the dependence of the transmitted flux on the statistics of the incident photons. Photon beams derived from sources of coherent, chaotic, squeezed, coherent-antibunched, and broadband-antibunched light are considered. our calculations are based on a recently developed theory of cascaded open systems,1,2 and serve to illustrate the usefulness of this theory.
Experimental evidence of field-correlation effects on weak-field two-photon absorption in atomic sodium is presented. In the case of a nearly Lorentzian laser power spectrum the absorption profile has four times the spectral width of the exciting field, in agreement with predictions by Mollow. The measurement is carried out with counterpropagating laser beams to cancel Doppler broadening. The width of the two-photon absorption spectrum is decreased by partially decorrelating the counterpropagating laser beams. Increasing the correlation time of the frequency fluctuations, resulting in a nearly Gaussian laser power spectrum, has also been observed to decrease the width of the absorption spectrum. An extension of the time-dependent second-order perturbation theory to these additional cases yields good agreement.
Two-photon absorption and emission for a collection of two level atoms from a single mode beam of light are considered and the statistical proper- ties of the field after the interaction are investigated without placing any restriction of the population of the atomic levels . The dynamical behaviour of the field is described by assuming the atomic levels maintained with a nearly fixed popula- tion distribution . By applying iteration methods the time development for the density operator of the field is written and an expression for the coherent component is obtained . This component appears to be present only when there is a coherent component in the field before the interaction . The statistical properties of the field after the interaction, when the mean photon number is large initially, are then discussed and explicit calculations are carried out for some special cases of initial fields . Finally, it is shown that two-photon spontaneous emission field can be expressed as a superposition of chaotic fields .