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Physical Review A

Aspects of two-photon absorption of squeezed light: The continuous-wave limit

Christian Drago, John E. Sipe

Published Aug 22, 2022• 27 citations
Publisher

Abstract

The authors present a theoretical analysis of two-photon absorption of classical and squeezed light that is valid for arbitrary intensity, both pulsed and cw light, and absorption both resonant and far-off-resonance from an intermediate state. Among other results, they find closed-form expressions for the cross sections and the scaling of the absorption with intensity.

DOI
10.1103/physreva.106.023115

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The authors present a theoretical analysis of two-photon absorption of classical and squeezed light that is valid for arbitrary intensity, both pulsed and cw light, and absorption both resonant and far-off-resonance from an intermediate state. Among other results, they find closed-form expressions for the cross sections and the scaling of the absorption with intensity.
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.
Squeezing in both intracavity and travelling-wave multiphoton absorption is investigated theoretically for incident intense nearly coherent light. It is shown that after sufficiently strong travelling-wave k-photon absorption (k=2,3...) a squeezed state of the radiation field is reached that is not a minimum uncertainty state. In this state the inphase and quadrature variances of the normalized electric field strength approach the asymptotic values k/(4(2k-1)) and k/4, respectively. With the help of an approximate Heisenberg picture treatment of a continuous mode field travelling through a broad-band k-photon absorber an analytical expression is obtained for the evolution of the squeezing spectrum in dependence on the degree of absorption. For intracavity multiphoton absorption the spectrum of output squeezing is investigated with the help of the usual Langevin equation approach. It turns out that the squeezing bandwidth in intracavity and travelling-wave multiphoton absorption is determined by the cavity bandwidth and the absorber linewidth, respectively.
An unconventional perturbation treatment of the theory of two-photon absorption in a four-level atomic system close to two-photon resonance is developed on the basis of the optical Bloch equations. The results for the longtime populations of the intermediate and upper states are valid in low- and medium-intensity regimes. In both regimes the upper state population shows a lorentzian resonance centred on zero two-photon detuning with a width equal to the natural linewidth of the upper state. The intermediate state population shows a similar behaviour in the intermediate regime only, with no significant dependence on two-photon detuning in the low-intensity regime. However, in both regimes the population of the virtual intermediate state is at least comparable to that of the resonant upper state. The perturbation theory results have been checked by direct numerical calculations based on the Bloch equations. Numerical calculations confirm the presence of a high-intensity regime characterized by power shifts, broadening and saturation effects.
Two-photon absorption (TPA) is of fundamental importance in super-resolution imaging and spectroscopy. Its nonlinear character allows for the prospect of using quantum resources, such as entanglement, to improve measurement precision or to gain new information on, e.g., ultrafast molecular dynamics. Here, we establish the metrological properties of nonclassical squeezed light sources for precision measurements of TPA cross sections. We find that the Cram\'er-Rao bound does not provide a fundamental limit for the precision achievable with squeezed states in the limit of very small cross sections. Considering the most relevant measurement strategies---namely, photon-counting and quadrature measurements---we determine the quantum advantage provided by squeezed states as compared to coherent states. We find that squeezed states outperform the precision achievable by coherent states when performing quadrature measurements, which provide improved scaling of the Fisher information with respect to the mean photon number $\ensuremath{\sim}{n}^{4}$. Due to the interplay of the incoherent nature and the nonlinearity of the TPA process, unusual scaling can also be obtained with coherent states, which feature an $\ensuremath{\sim}{n}^{3}$ scaling in both quadrature and photon-counting measurements.
Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs have been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This Tutorial presents a detailed theoretical study of one- and two-photon absorption by molecules, focusing on how to treat the quantum nature of light. We review some basic quantum optics theory and then we review the density-matrix (Liouville) derivation of molecular optical response, emphasizing how to incorporate quantum states of light into the treatment. For illustration, we treat in detail the TPA of photon pairs created by spontaneous parametric down conversion, with an emphasis on how quantum light TPA differs from that with classical light. In particular, we treat the question of how much enhancement of the TPA rate can be achieved using entangled states. This Tutorial includes a review of known theoretical methods and results as well as some extensions, especially the comparison of TPA processes that occur via far-off-resonant intermediate states only and those that involve off-resonant intermediate states by virtue of dephasing processes. A brief discussion of the main challenges facing experimental studies of entangled two-photon absorption is also given.