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Physical Review

Two-Photon Absorption and Coherence

Salvatore Carusotto, G. Fornaca, ERSEO POLACCO

Published May 25, 1967• 34 citations
Publisher

Abstract

We study the probabilities for two-photon absorption processes induced by both coherent and thermal light when acting on an atomic system. Calculations are performed with quantum electrodynamics, and we find results similar to those obtained with semiclassical methods; that is, the two-photon absorption probability depends on the statistical properties of the light used. This probability assumes its maximum value for coherent light.

DOI
10.1103/physrev.157.1207

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The Two-photon absorption processes (TPA) is of great interest due to its variety of technical applications. Two-photon transitions can be excited using light with different statistical properties, such as laser light (coherent light), pseudo-thermal light and entangled photons-pairs (ETPA). For a TPA process driven with entangled photons (ETPA), a linear dependence of the signal with the photon flux has been theoretically predicted and experimentally demonstrated by various groups. The main motivation for studying ETPA relies on the capability of inducing TPA with a low photon flux. This is advantageous to analyze, among other things, biological samples with a reduced probability of destroying them in the process. However, ETPA experiments developed to date raise many questions regarding the difficulty of isolating a signal in organic molecules. One of the main problems in these experiments is the difficulty to study independently all the systematic effects due to the complex structure of organic molecules. An alternative to clarify the origin of the signal is to study the ETPA process in atomic systems. In this case, the possibility to excite narrow band transitions with tunable single frequency lasers can provide a clear signature of the ETPA process. To achieve this objective, the first step consists of understanding TPA with coherent light, or classical TPA, and measuring the corresponding cross-section in atomic systems. Once the classical regime is characterized, the ETPA process can be studied considering decoherence effects and coherence between intermediate states. For this, the ETPA cross section must be calculated and measured. In this work we present a theoretical calculation of the ETPA transition probability and cross-section with the density operator formalism for the transition 62S1/2 →82S1/2. The theoretical results will be complemented with an experiment with atomic Cesium based in a coincidence detection scheme.

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We study the probabilities for two-photon absorption processes induced by both coherent and thermal light when acting on an atomic system. Calculations are performed with quantum electrodynamics, and we find results similar to those obtained with semiclassical methods; that is, the two-photon absorption probability depends on the statistical properties of the light used. This probability assumes its maximum value for coherent light.
We study the probability for multiphoton absorption processes induced by both laser and thermal light acting on an atomic system. When the thermal radiation, suitably filtered, has the same frequency spectrum and the same total energy as the laser packet, we find that the ratio between the relative probabilities for sss-photon absorption can be expressed by ${(4\ensuremath{\pi})}^{\frac{\ensuremath{-}1}{2(s\ensuremath{-}1)}}s!{s}^{\frac{1}{2}}{(\frac{{\ensuremath{\tau}}_{c}}{\ensuremath{\tau}})}^{s\ensuremath{-}1},$ where $\ensuremath{\tau}$ is the time during which the atomic system is illuminated by thermal radiation with coherence time ${\ensuremath{\tau}}_{c}$. This shows that multiphoton absorption processes depend on the statistical properties of the incident light, and that the probability induced by the laser packet is certainly greater than that induced by the thermal light if $s<\frac{\ensuremath{\tau}}{{\ensuremath{\tau}}_{c}}$.
The effects of two-photon absorption from a single beam of light on the statistical properties of the beam are considered. Simple expressions are obtained for the initial rates of change and limiting steady-state values of the mean photon number and degree of second-order coherence of the beam. The general time dependences of these properties of the light and of the complete photon probability distribution are evaluated for several initial types of beam. The physical significance of the results is described, and their relationship to calculations which use a classical representation of the light is discussed.
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.
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 .
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 Two-photon absorption processes (TPA) is of great interest due to its variety of technical applications. Two-photon transitions can be excited using light with different statistical properties, such as laser light (coherent light), pseudo-thermal light and entangled photons-pairs (ETPA). For a TPA process driven with entangled photons (ETPA), a linear dependence of the signal with the photon flux has been theoretically predicted and experimentally demonstrated by various groups. The main motivation for studying ETPA relies on the capability of inducing TPA with a low photon flux. This is advantageous to analyze, among other things, biological samples with a reduced probability of destroying them in the process. However, ETPA experiments developed to date raise many questions regarding the difficulty of isolating a signal in organic molecules. One of the main problems in these experiments is the difficulty to study independently all the systematic effects due to the complex structure of organic molecules. An alternative to clarify the origin of the signal is to study the ETPA process in atomic systems. In this case, the possibility to excite narrow band transitions with tunable single frequency lasers can provide a clear signature of the ETPA process. To achieve this objective, the first step consists of understanding TPA with coherent light, or classical TPA, and measuring the corresponding cross-section in atomic systems. Once the classical regime is characterized, the ETPA process can be studied considering decoherence effects and coherence between intermediate states. For this, the ETPA cross section must be calculated and measured. In this work we present a theoretical calculation of the ETPA transition probability and cross-section with the density operator formalism for the transition 62S1/2 →82S1/2. The theoretical results will be complemented with an experiment with atomic Cesium based in a coincidence detection scheme.