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arXiv:1701.08228 · Physical Review A

Atomically thin semiconductors as nonlinear mirrors

Sina Zeytinoǧlu, Charlaine Roth, Sebastian D. Huber, Ataç İmamoğlu

Published Sep 12, 2017• 33 citations
arXivHTMLPDF

Abstract

We show that a transition-metal dichalcogenide monolayer with a radiatively broadened exciton resonance would exhibit perfect extinction of the transmitted field. This result holds for $s$- or $p$-polarized weak resonant light fields at any incidence angle, due to the conservation of the in-plane momentum of excitons and photons in a flat defect-free two-dimensional crystal. In contrast to extinction experiments with single quantum emitters, exciton-exciton interactions lead to an enhancement of reflection with increasing power for incident fields that are blue detuned with respect to the exciton resonance. By taking into account quantum fluctuations, we show that the extinction of such a nonlinear mirror is limited; for light intensities leading to maximal reflection, the transmitted field is in a multimode squeezed state.

DOI
10.1103/physreva.96.031801

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We show that a transition-metal dichalcogenide monolayer with a radiatively broadened exciton resonance would exhibit perfect extinction of the transmitted field. This result holds for sss- or ppp-polarized weak resonant light fields at any incidence angle, due to the conservation of the in-plane momentum of excitons and photons in a flat defect-free two-dimensional crystal. In contrast to extinction experiments with single quantum emitters, exciton-exciton interactions lead to an enhancement of reflection with increasing power for incident fields that are blue detuned with respect to the exciton resonance. By taking into account quantum fluctuations, we show that the extinction of such a nonlinear mirror is limited; for light intensities leading to maximal reflection, the transmitted field is in a multimode squeezed state.
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A theoretical investigation is reported of the coherent nonlinear response of excitons and biexcitons in a thin semiconductor film subjected to resonant laser radiation. It is shown that saturation of an exciton transition results in an abrupt qualitative change in the nature of film transmission from total reflection of the incident pulse at low pump amplitudes to oscillatory reflection at high amplitudes. A new area theorem is derived for ultrashort pulses: it establishes a correspondence between the areas of the incident, transmitted, and reflected pulses. Anomalous transmission and reflection (area 'quantisation') is predicted for large values of the nonlinear parameter. The equations of state, describing bistable behaviour of the amplitudes of the fields of the transmitted and reflected radiation, are derived for quasi-cw operation.
A theoretical investigation is reported of the coherent nonlinear response of excitons and biexcitons in a thin semiconductor film subjected to resonant laser radiation. It is shown that saturation of an exciton transition results in an abrupt qualitative change in the nature of film transition from the regime of total reflection of the incident pulse at low pump amplitudes to oscillatory reflection at high amplitudes. A new area theorem is derived for ultrashort pulses: it establishes a correspondence between the areas of the incident, transmitted and reflected pulses. Anomalous transmission and reflection is predicted for large values of the nonlinear parameter. The equations of the state, describing bistable behavior of the amplitudes of the fields of the transmitted and reflected radiation, are derived for quasi-cw operation.
The peculiarities of nonlinear transmission of ultrashort pulses of resonance laser radiation by a semiconductor thin film in the excitonic spectral region have been studied, taking into account the exciton-phonon interaction and concentration gain of the dipole moment of the excitonic transition. It has been shown that under exact resonance conditions the film transmits only the leading edge of the incident rectangular pulse and completely reflects the remaining part. For a nonzero off-resonance, a residual transmission occurs. A series of possibilities for transforming Gaussian pulses is predicted. The state equations for steady-state bistable transmission (reflection) have been derived, and the stability of the solutions has been studied. A theorem of areas, which predicts area restriction of the transmitted pulses, has been stated; namely, the transmitted pulse area cannot exceed π/2.
The emergence of photonic quantum correlations is typically associated with emitters strongly coupled to a photonic mode. Here, we show that semiconductor Rydberg excitons, which are only weakly coupled to a free-space light mode can produce strongly antibunched fields, i.e., quantum light. This effect is fueled by a micron-scale excitation blockade between Rydberg excitons inducing pair-wise polariton scattering events. Photons incident on an exciton resonance are scattered into blue- and red-detuned pairs, which enjoy relative protection from absorption and thus dominate the transmitted light. We demonstrate that this effect persists in the presence of additional phonon coupling, strong nonradiative decay, and across a wide range of experimental parameters. Our results pave the way for the observation of quantum statistics from weakly coupled semiconductor excitons.