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arXiv:2106.04171 · The Journal of Chemical Physics

Optimization of selective two-photon absorption in cavity polaritons

Edoardo G. Carnio, Andreas Buchleitner, Frank Schlawin

Published Jun 7, 2021• 11 citations
arXivHTMLPDF

Abstract

We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs separable states of light. Interference between excitation pathways as well as the presence of nearby states may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem and enhance the achievable "selectivity" between two energy levels, i.e., the relative difference in population transferred into each of them. We find that the added value of optimal entangled states of light increases with broadening linewidths of the target states.

DOI
10.1063/5.0049863

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We investigate optimal states of photon pairs to excite a target transition in a multilevel quantum system. With the help of coherent control theory for two-photon absorption with quantum light, we infer the maximal population achievable by optimal entangled vs separable states of light. Interference between excitation pathways as well as the presence of nearby states may hamper the selective excitation of a particular target state, but we show that quantum correlations can help to overcome this problem and enhance the achievable "selectivity" between two energy levels, i.e., the relative difference in population transferred into each of them. We find that the added value of optimal entangled states of light increases with broadening linewidths of the target states.
We investigate how entanglement can enhance two-photon absorption in a three-level system. First, we employ the Schmidt decomposition to determine the entanglement properties of the optimal two-photon state to drive such a transition, and the maximum enhancement which can be achieved in comparison to the optimal classical pulse. We then adapt the optimization problem to realistic experimental constraints, where photon pairs from a down-conversion source are manipulated by local operations such as spatial light modulators. We derive optimal pulse shaping functions to enhance the absorption efficiency, and compare the maximal enhancement achievable by entanglement to the yield of optimally shaped, separable pulses.
We investigate the excitation of a three-level ladder-type atom by a unidirectional field with a pair of indistinguishable photons. Starting from an analytical expression for the two-photon absorption probability, we determine the two-photon state that maximizes the population of the upper atomic state at a chosen time and show that in the limit of an infinitely long pulse, perfect excitation is possible. The optimal state is identified as the time-reversed counterpart of the two-photon state emitted in spontaneous cascade decay. We then compare this ideal excitation strategy with experimentally accessible families of states, including symmetrized Gaussian product states, temporally correlated Gaussian states, and coherent pulses. We analyze how the optimal excitation conditions depend on the ratio of atomic decay rates and on the separation of the atomic transition frequencies. For indistinguishable photons, quantum interference may shift the maxima of the marginal spectral distribution away from the atomic resonances and qualitatively modify the optimal excitation strategy. Our results clarify the role of indistinguishability and correlations in two-photon absorption and provide guidance for designing realistic excitation schemes in quantum-optical light-matter interfaces.
This work discusses the problem of optimal excitation of a three-level atom of ladder configuration by light in the two-photon state and coherent light carrying an average of two photons. The applied atom-light interaction model is based on the Wigner-Weisskopf approximation. We characterize the properties of the optimal two-photon state that excites an atom perfectly, i.e., with probability equal to one. We find that the spectrotemporal shape of the optimal state of light is determined by the lifetimes of the atomic states, with the degree of photonic entanglement in the optimal state depending on the lifetime ratio. In consequence, two distinct interaction regimes can be identified in which the entanglement of the input state of light has a qualitatively different impact. As the optimal states may be challenging to prepare in general, we compare the results with those obtained for photon pairs of selected experimentally relevant pulse shapes. As these shapes are optimized for maximal atomic excitation probability, the results can be interpreted in terms of the overlap between the optimal and investigated pulse shapes.
We propose and analyze a scheme for controlling coherent photon transmission and reflection in a cavity-quantum-electrodynamics (CQED) system consisting of an optical resonator coupled with three-level atoms coherently prepared by a control laser from free space. When the control laser is off and the cavity is excited by two identical light fields from two ends of the cavity, the two input light fields can be completely absorbed by the CQED system and the light energy is converted into the excitation of the polariton states, but no light can escape from the cavity. Two distinct cases of controlling the perfect photon absorption are analyzed: (a) when the control laser is tuned to the atomic resonance and creates electromagnetically induced transparency, the perfect photon absorption is suppressed and the input light fields are nearly completely transmitted through the cavity; (b) when the control laser is tuned to the polariton state resonance and inhibits the polariton state excitation, the perfect photon absorption is again suppressed and the input light fields are nearly completely reflected from the cavity. Thus, the CQED system can act as a perfect absorber or near-perfect transmitter and/or reflector by simply turning the control laser off or on. Such interference control of the coherent photon-atom interaction in the CQED system should be useful for a variety of applications in optical logical devices.