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arXiv:2207.10420 · Physical review. B./Physical review. B

Bichromatic four-wave mixing and quadrature-squeezing from biexcitons in atomically thin semiconductor microcavities

Emil V. Denning, Andreas Knorr, Florian Katsch, Marten Richter

Published Nov 28, 2022• 5 citations
arXivHTMLPDF

Abstract

Nonlinear optical effects such as four-wave mixing and generation of squeezed light are ubiquitous in optical devices and light sources. For new devices operating at low optical power, the resonant nonlinearity arising from the two-photon sensitive bound biexciton in a semiconductor microcavity is an interesting prospective platform. Due to the particularly strong Coulomb interaction in atomically thin semiconductors, these materials have strongly bound biexcitons and operate in the visible frequency range of the electromagnetic spectrum. To remove the strong pump laser from the generated light in optical devices or to simultaneously excite nondegenerate polaritons, a bichromatic-pump configuration with two spectrally separated pump lasers is desirable. In this paper, we theoretically investigate spontaneous four-wave mixing and quadrature-squeezing in a bichromatically pumped atomically thin semiconductor microcavity. We explore two different configurations that support degenerate and nondegenerate scattering from polaritons into bound biexcitons, respectively. We find that these configurations lead to the generation of strongly single- and two-mode quadrature-squeezed light.

DOI
10.1103/physrevb.106.195307

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Nonlinear optical effects such as four-wave mixing and generation of squeezed light are ubiquitous in optical devices and light sources. For new devices operating at low optical power, the resonant nonlinearity arising from the two-photon sensitive bound biexciton in a semiconductor microcavity is an interesting prospective platform. Due to the particularly strong Coulomb interaction in atomically thin semiconductors, these materials have strongly bound biexcitons and operate in the visible frequency range of the electromagnetic spectrum. To remove the strong pump laser from the generated light in optical devices or to simultaneously excite nondegenerate polaritons, a bichromatic-pump configuration with two spectrally separated pump lasers is desirable. In this paper, we theoretically investigate spontaneous four-wave mixing and quadrature-squeezing in a bichromatically pumped atomically thin semiconductor microcavity. We explore two different configurations that support degenerate and nondegenerate scattering from polaritons into bound biexcitons, respectively. We find that these configurations lead to the generation of strongly single- and two-mode quadrature-squeezed light.
Modification of electromagnetic quantum fluctuations in the form of quadrature squeezing is a central quantum resource, which can be generated from nonlinear optical processes. Such a process is facilitated by coherent two-photon excitation of the strongly bound biexciton in atomically thin semiconductors. We show theoretically that interfacing an atomically thin semiconductor with an optical cavity makes it possible to harness this two-photon resonance and use the biexcitonic parametric gain to generate squeezed light with input power an order of magnitude below current state-of-the-art devices with conventional third-order nonlinear materials that rely on far off-resonant nonlinearities. Furthermore, the squeezing bandwidth is found to be in the range of several meV. These results identify atomically thin semiconductors as a promising candidate for on-chip squeezed-light sources.
Summary form only given. In a recent paper [1] it has been shown how a bichromatic fast driving of optomechanical (optical domain) and superconducting circuit systems (microwave domain), operating in a limit where they present a non-linear Kerr-type interaction, can give rise to very strong vacuum squeezing. The driving with two close frequencies of a Kerr cavity changes the usual bistability bifurcation behaviour that takes place under monochromatic driving, into a degenerate four-wave mixing bifurcation, where a phase-bistable component starts oscillating spontaneously at a frequency that lies halfway between the two driving frequencies [2]. This resembles the physics of the optical parametric oscillator threshold, devices that has produced experimentally the strongest squeezing up to now. Associated to this bifurcation there is a strong reduction of the quantum fluctuations for a given quadrature of the electromagnetic field, resulting in vacuum squeezing, the reduction takes place at the central non-injected frequency.Here we show the application of this bichromatic driving protocol to a semiconductor micro-cavity system [3,4], where the nonlinear interaction between photons is caused through the excitons induced at the semiconductor embedded in the optical cavity.
Using a general Hamiltonian treatment, we theoretically study the generation of degenerate quadrature squeezing in a dual-pumped integrated microring resonator coupled to a waveguide. Considering a dual-pump four-wave mixing configuration in an integrated Si3N4{\text{Si}}_{3}{\text{N}}_{4}Si3​N4​ platform, and following the coupled-mode theory approach, we investigate the effects of parasitic quantum nonlinear optical processes on the generation of squeezed light. Considering five resonance modes in this approach allows us to include the most important four-wave mixing processes involved in such a configuration. We theoretically explore the effects of the pump detunings on different nonlinear processes and show that the effects of some of the parasitic processes are effectively neutralized by symmetrically detuning the two pumps. This yields a significant enhancement in the output squeezing quality without physically changing the structure, but suffers from the trade-off of requiring substantially higher pump power for a fixed target level of squeezing.
Summary form only given. Four-particle correlation mediated by the Coulomb interaction has been found to play a major role in the nonlinear optical response at the semiconductor band edge at low excitation density. The attractive interaction of the excitons with opposite spins result in the formation of bound (bi-exciton) and unbound (scattered) two-exciton states. In this paper we report on the first to our knowledge, comparison of the contributions to the coherent nonlinearity from the bound and unbound two-exciton states. The polarization-sensitive four wave mixing experiment is performed in the high-Q semiconductor microcavity, in which the incoherent effects are suppressed due to strong exciton-photon coupling. The semiconductor microcavity has a single 12-nm-thick GaAs quantum well.
Investigations of quantum effects in semiconductor quantum-well microcavities interacting with laser light in the strong-coupling regime are presented. Modifications of quantum fluctuations of the outgoing light are expected due to the non-linearity originating from coherent exciton–exciton scattering. In the strong-coupling regime, this scattering translates into a four-wave mixing interaction between the mixed exciton–photon states, the polaritons. Squeezing and giant amplification of the polariton field and of the outgoing light field fluctuations are predicted. However, polariton–phonon scattering is shown to yield excess noise in the output field, which may destroy the non-classical effects. Experiments demonstrate evidence for giant amplification due to coherent four-wave mixing of polaritons. Noise reduction below the thermal noise level was also observed.
We report squeezed polariton generation using parametric polariton four-wave mixing in semiconductor microcavities in thestrong coupling regime. The geometry of the experiment corresponds to degenerate four-wave mixing, which gives rise to abistability threshold. Spatial effects in the nonlinear regime are evidenced, and spatial filtering is required in orderto optimize the measured squeezing. By measuring the noise of the outgoing light, we infer a 9 percent squeezing on thepolariton field close to the bistability turning point.