Optical microcavities are often proposed as platforms for spectroscopy in the single- and few-photon regime due to strong light-matter coupling. For classical-light spectroscopies, an empty microcavity simply acts as an optical filter. However, we find that in the single- or few-photon regime treating the empty microcavity as an optical filter does not capture the full effect on the quantum state of the transmitted photons. Focusing on the case of entangled photon-pair spectroscopy, we consider how the propagation of one photon through an optical microcavity changes the joint spectrum of a frequency-entangled photon pair. Using the input-output treatment of a Dicke model, we find that propagation through a strongly coupled microcavity above a certain coupling threshold enhances the entanglement entropy between the signal and idler photons. These results show that optical microcavities are not neutral platforms for quantum-light spectroscopies and their effects must be carefully considered when using change in entanglement entropy as an observable.
Optical microcavities are often proposed as platforms for spectroscopy in the single- and few-photon regime due to strong light-matter coupling. For classical-light spectroscopies, an empty microcavity simply acts as an optical filter. However, we find that in the single- or few-photon regime treating the empty microcavity as an optical filter does not capture the full effect on the quantum state of the transmitted photons. Focusing on the case of entangled photon-pair spectroscopy, we consider how the propagation of one photon through an optical microcavity changes the joint spectrum of a frequency-entangled photon pair. Using the input-output treatment of a Dicke model, we find that propagation through a strongly coupled microcavity above a certain coupling threshold enhances the entanglement entropy between the signal and idler photons. These results show that optical microcavities are not neutral platforms for quantum-light spectroscopies and their effects must be carefully considered when using change in entanglement entropy as an observable.
One of the most common approaches for coupling optical single-photon sources and photonic integrated circuits is to use a cavity. The cavity acts as a spectral filter that distorts the light spectrum and changes its statistical properties. But in the general case one should take into account not only spectral filtering of light but also the spectral filter influence on the single-photon source dynamics. We build an effective analytical model for description of the cavity influence on the photon statistics of light emitted by the single-photon source as spectral filtering only. We show that this model correctly describes the photon statistics even in a strong-coupling regime between the single-photon source and the spectral filter. Our results can be useful for analytical modeling of photon statistics of quantum emitters strongly coupled to various electromagnetic interfaces.
The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation. These applications aim at the controlled manipulation of the photonic degrees of freedom, and therefore rely on simple models of matter, where the analysis is simpler. Furthermore, quantum imaging with entangled light can achieve enhanced resolution, and quantum metrology can overcome the shot noise limit for classical light. This Account focuses on an entirely different emerging class of applications using quantum light as a powerful spectroscopic tool to reveal novel information about complex molecules. These applications utilize two appealing properties of quantum light: its distinct intensity fluctuations and its nonclassical bandwidth properties. These give rise to new and surprising behavior of nonlinear optical signals. Nonclassical intensity fluctuations can enhance nonlinear optical signals relative to linear absorption. For instance, the two-photon absorption of entangled photon pairs scales linearly (rather than quadratically) in the photon flux, just like a single photon absorption. This enables nonlinear quantum spectroscopy of photosensitive, for example, biological, samples at low light intensities. We will discuss how the two-photon absorption cross section becomes a function of the photonic quantum state, which can be manipulated by properties of the entangled photon pairs. In addition, the quantum correlations in entangled photon states further influence the nonlinear signals in a variety of ways. Apart from affecting the signal's scaling with intensity, they also constitute an entirely new approach to shaping and controlling excitation pathways in molecular aggregates in a way that cannot be achieved with shaped classical pulses. This is because between the two absorption events in entangled two-photon absorption, the light and material system are entangled. Classical constraints for the simultaneous time and frequency resolution can thus be circumvented, since the two are not Fourier conjugates. Here we review the simplest manifestation of quantum light spectroscopy, two-photon absorption spectroscopy with entangled photons. This will allow us to discuss exemplarily the impact of quantum properties of light on a nonlinear optical signal and explore the opportunities for future applications.
The strong-coupling regime of cavity-quantum-electrodynamics (cQED) represents the light-matter interaction at the fully quantum level. Adding a single photon shifts the resonance frequencies, a profound nonlinearity. cQED is a test-bed of quantum optics and the basis of photon-photon and atom-atom entangling gates. At microwave frequencies, success in cQED has had a transformative effect. At optical frequencies, the gates are potentially much faster; the photons can propagate over long distances; and the photons can be detected easily, ideal features for quantum networks. Following pioneering work on single atoms, solid-state implementations using semiconductor quantum dots are emerging, an important prospect for quantum technology. We present here a gated, ultralow-loss microcavity-device which forms a highly coherent photon−quantum-dot interface with a cooperativity of C=150. The gates allow both the quantum dot charge state and resonance frequency to be controlled electrically; crucially, they eliminate the noise-source which has complicated quantum dot cQED in the past − scattering from the bare microcavity mode even at the quantum dot-microcavity resonance. Even in the microcavity, the quantum dot has a linewidth close to the radiative limit. In addition to a very pronounced avoided-crossing in the spectral domain, we observe a clear coherent exchange of a single energy-quantum between the ``atom" and cavity in the time domain (vacuum Rabi-oscillations). Decoherence arises predominantly via the atom and photon loss-channels. The coherence is exploited to probe the transitions between the singly- and doubly-excited photon-atom system via photon-statistics spectroscopy. We propose this system as a platform for quantum technology, for instance a photon-photon entangling gate.
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.
Theoretical study on entangled photon generation from a quantum dot (QD) embedded in microcavity is briefly reviewed within a strong coupling regime. In this system, entangled photon pairs can be generated through the cascade photon emission via dressed states in the cavity quantum electrodynamics (CQED). Excitation levels of a QD are modeled by a V-type three-level system and four-level system including a biexciton. In contrast to the entangled-photon generation until now, all four Bell states can be generated from an identical cavity system by simply selecting applied-field polarizations and frequencies as characteristic features of the CQED. The CQED effects play a crucial role in providing a high degree of entanglement: (i) spectral fi ltering can be used to extract entangled photons due to the vacuum Rabi splitting and (ii) non-entangled co-polarized photons are strongly suppressed due to the photon blockade effect.
Semiconductor quantum dots (QDs) coupled with optical microcavities provide an excellent platform for generating high-performance single-photon sources. However, the current microcavity structures are difficult to solve the tradeoff between single-photon purity and indistinguishability without additional filtering, due to challenges in suppressing broad phonon sideband spectrum and two-photon emission in the practical experiments. To address these issues, we have developed a novel asymmetric microcavity that supports two nondegenerate polarized modes, both resonant with a single quantum dot. One cavity mode is broadband and is used for excitation to reduce two-photon emission intensity, while the other is narrowband and is used for collection to enhance the indistinguishability of single-photon sources. This asymmetric microcavity also has the ability to overcome at least half of the photon efficiency loss under polarization filtering. Moreover, our model has employed an excitation pulse that resonates with cavity modes eliminating spectral distortion of intracavity fields, and efficiently achieving deterministic population inversion of QDs compared to an elliptical cavity. Our scheme paves the way to develop the excellent performance single-photon sources with higher brightness, near-unity purity, and indistinguishability without any additional filtering in practical experiments.