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Physical Review Letters

Two-photon absorption of nonclassical light

Julio R. Gea-Banacloche

Published Apr 3, 1989• 215 citations
Publisher

Abstract

Two-photon absorption of light with nonclassical (squeezed) fluctuations is considered. Several unique effects are predicted for various possible regimes. These include a linear (instead of quadratic) growth of the absorption rate with the light intensity for weak fields, the possibility of a decreasing absorption with increasing intensity, and orders-or-magnitude differences between absorption rates for phase- and amplitude-squeezed beams of the same intensity.

DOI
10.1103/physrevlett.62.1603

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Two-photon absorption of light with nonclassical (squeezed) fluctuations is considered. Several unique effects are predicted for various possible regimes. These include a linear (instead of quadratic) growth of the absorption rate with the light intensity for weak fields, the possibility of a decreasing absorption with increasing intensity, and orders-or-magnitude differences between absorption rates for phase- and amplitude-squeezed beams of the same intensity.
The two-photon interaction process of N identical three-level atoms with squeezed light is considered. The dependence of the absorption process on the squeezed fluctuations of light is studied. It is shown that the absorption rate of phase squeezed light is larger than the absorption rate of amplitude squeezed light. If the amplitude of the fluctuations is approximately equal to the average value of the electromagnetic field intensity, the quantum fluctuations can stop the two-photon nutation in the system. The possibility of a first-order phase transition in the system composed by the atoms and the external electromagnetic field is discussed.
We investigate the dynamical evolution of nonclassical states of light undergoing a two-photon absorption process. We consider two distinct cases of initial states, a squeezed coherent state and an eigenstate of the two-photon annihilation operator (a superposition of macroscopically distinct coherent states). We analyze the fluctuations in the photon-number operator and in the quadrature components of the field. Whereas one-photon linear damping rapidly destroys quantum features such as squeezing, we demonstrate that substantial coherence is retained when such light interacts with a two-photon-absorbing reservoir. This surviving coherence is responsible for the preservation of squeezing in the steady state despite the effect of dissipation. We relate the origin of squeezing of initially unsqueezed light interacting with two-photon absorbers with the squeezing generated by simple superposition states of light.
The present report deals with the condition under which an ensemble of atoms goes over into a regime of collective two-photon nutation, and with the behavior of Rabi frequency as function of external light. To simplify this problem, we consider a system of Λ-type atoms that enters into two-photon resonance with an external squeezed electromagnetic field relative to the forbidden transition ∣1> ∣2> , where ∣1> and ∣2> are ground and first exited states [1,2] The situation is examining, when the values of quantum fluctuations of electromagnetic field intensity have the same value as the mean value of electromagnetic field intensity. This is one of main difference between the our paper and [2]. The proposed mathematical model permits to take into account all the two-photon diagrams. These diagrams describe not only resonance two-photon transitions but two-photon scattering processes between ∣1> and ∣2> levels too. Using mathematical method which is proposed in [1,2] it is obtained the master equation for the atom subsystem. Two stationary solutions for the case when Rabi frequency is larger than the inverse value of the collective two-photon decay time and the case when external light is coherent are examined. It is showing that the absorption rate of an phase squeezed field is larger than the absorption rate of an amplitude squeezed light. We also obtained the behavior of inversion between the levels ∣1> and ∣2>, when the collective of atoms enters into two-photon resonance with external field.
We present a theoretical analysis of two-photon absorption of classical and squeezed light valid when one-photon absorption to an intermediate state is either resonant or far-detuned from resonance, and in both the low and high intensity regimes. In this paper we concentrate on continuous-wave excitation, although the approach we develop is more general. We calculate the energy removed from an incident field for typical experimental parameters and consider the limiting cases when the photon pairs are narrowband or broadband compared to the molecular linewidths. We find an enhancement of the two-photon absorption due to resonant contributions from the large squeezed light bandwidth and due to photon bunching in the low intensity regime. However, in both cases, for the parameters we choose, the one-photon absorption is the dominant process in the region of parameter space where a large enhancement of the two-photon absorption is possible.
We describe how a two-mode, above-threshold, optical parametric oscillator can generate nonclassical states of light with a large average number of photons: the fluctuation spectrum of the various fields is calculated, and several quantities are shown to have squeezed fluctuations. In particular, a perfect quantum noise suppression is predicted on the difference between the intensities of the two generated beams. We describe an experiment designed to demonstrate such an effect and show how it can be used to generate high-intensity amplitude-squeezed states.
We consider a single two-level atom in an optical cavity, in which the system is driven by a coherent driving field. In the bad-cavity limit, when the cavity loss rate is taken to be large compared to the atomic decay rate and atom-field coupling, the cavity field can be adiabatically eliminated from the equations of motion for the atomic operators. The main effect of the cavity in this limit is the enhancement of spontaneous emission into the cavity mode. For this model, the second-order intensity correlation function g(2)() has been shown to exhibit photon antibunching, sub-Poissonian photon number distributions, and other nonclassical effects.1 In this paper, analytic results are presented for g(2)() for both the transmitted and fluorescent light fields when broadband squeezed light is injected into the cavity. Effects of the squeezing on nonclassical behavior is examined.