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The Journal of Physical Chemistry Letters

Manipulating Two-Photon-Absorption of Cavity Polaritons by Entangled Light

Bing Gu, Shaul Mukamel

Published Sep 2, 2020• 34 citations
Publisher

Abstract

We demonstrate that two-photon excitations to bipolariton states created by placing several molecules in an optical cavity can be manipulated by quantum light. Entangled photons can access classically dark bipolariton states by modifying the quantum interferences of two-photon transition pathways involving different single-polariton intermediate states and time-ordering of the two photon beams.

DOI
10.1021/acs.jpclett.0c02282

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We demonstrate that two-photon excitations to bipolariton states created by placing several molecules in an optical cavity can be manipulated by quantum light. Entangled photons can access classically dark bipolariton states by modifying the quantum interferences of two-photon transition pathways involving different single-polariton intermediate states and time-ordering of the two photon beams.
We theoretically investigate entangled-photon generation via a biexciton in a planar microcavity. Owing to strong exciton-photon coupling, the biexciton in the cavity produces a bound two-cavity-polariton state (cavity bipolariton). Entangled photons are generated by the cascade decay of the cavity bipolariton. We propose a novel scheme for highly efficient entangled-photon generation by controlling the cavity bipolariton states. It is shown that highly efficient generation can be achieved when a weak cavity bipolariton, formed by a biexciton and unbound cavity polaritons, is realized.
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.
The use of quantum light to probe exciton properties in semiconductor and molecular nanostructures typically occurs in the low-intensity regime. A substantial enhancement of exciton-photon coupling can be achieved with photonic cavities, where excitons hybridize with cavity modes to form polariton states. To provide a theoretical framework for interpreting emerging experimental efforts in this direction, we develop a scattering theory describing the interaction of frequency-entangled photon pairs with cavity polariton and bipolariton states under various coupling regimes. Employing the Tavis-Cummings model in combination with our scattering approach, we present a quantitative analysis of how the interaction of the entangled photon pair with the polariton/bipolariton modifies its joint spectral amplitude (JSA). Specifically, we examine the effects of the cavity-mode steady-state population, exciton-cavity coupling strength, and different forms of the input photon JSA. Our results show that the entanglement entropy of the scattered photons is highly sensitive to the interplay between the input JSA and the spectral line shapes of the polariton resonances, emphasizing the cavity filtering effects. We suggest that biphoton scattering quantum light spectroscopy best serves as a sensitive probe of polariton and bipolariton states in the photon-vacuum cavity state. Our approach is not only robust to various regimes of cavity-exciton coupling, but also amenable to extensions beyond the Tavis-Cummings model, enabling the representation of a broad class of molecular systems and solid state quantum materials.
Nonlinear optical response of cavity polaritons formed in high-g semiconductor microcavities has attracted much attention because of their potential applications to entangled-photon sources and other quantum information technologies. Theoretical ideas of entangled-photon generation, e.g., biexcitonic cavity quantum electrodynamics and polariton-polariton scattering, have been suggested, however these theories are limited in scope of target because they restrict two-exciton states to either biexciton or unbound two-exciton states. As for exciton system with small binding energy of biexciton, it is likely that the interplay between the biexciton and unbound two-exciton states have much impact on generation efficiency of entangled photons. The authors introduces a general model including both biexciton and unbound two-exciton states and discuss generation efficiency of entangled photons.
It has been shown that perfect photon absorption can occur in the linear excitation regime of cavity quantum electrodynamics (CQED), in which photons from two identical light fields coupled into two ends of the cavity are completely absorbed and result in excitation of the polariton state of the CQED system. The output light from the cavity is totally suppressed by destructive interference and the polariton state can only decay incoherently back to the ground state. Here we analyze perfect photon absorption and the onset of optical bistability in the nonlinear regime of the CQED and show that perfect photon absorption persists in the nonlinear regime of the CQED below the threshold of optical bistability. Therefore perfect photon absorption is a phenomenon that can be observed in both linear and nonlinear regimes of CQED. Furthermore, our study reveals that optical bistability is influenced by input-light interference and can be manipulated by varying the relative phase of the two input fields.