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arXiv:2505.04786

Resonant pump intensity dependence of luminescence achieved via Floquet engineering

I. S. Pashkevich, Iliya V. Doronin, A. A. Zyablovsky, E. S. Andrianov

Published May 7, 2025• 0 citations
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Abstract

We discover an unexpected behavior in a hybrid system composed of cavity strongly coupled to molecules and subjected to high intensity coherent pumping. We show that if the frequency of the pumping wave is close to polariton transitions in the hybrid system, non monotone dependence of fluorescence and scattering amplitudes on pump intensity with a narrow resonance-like response occurs. We demonstrate that this phenomenon occurs due to hybridization of lower and upper polaritons with substantially different excitation numbers caused by the pumping affecting polariton states of the system. This occurs when the Rabi interaction with coherent field is comparable to the field-matter coupling constant which in turn needs to be sufficient for the manifestation of strong coupling. This non-monotonic dependence of the fluorescence and scattering amplitudes on pump rate intensity pave the way for creation of nonlinear optical devices.

DOI
10.48550/arxiv.2505.04786

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We discover an unexpected behavior in a hybrid system composed of cavity strongly coupled to molecules and subjected to high intensity coherent pumping. We show that if the frequency of the pumping wave is close to polariton transitions in the hybrid system, non monotone dependence of fluorescence and scattering amplitudes on pump intensity with a narrow resonance-like response occurs. We demonstrate that this phenomenon occurs due to hybridization of lower and upper polaritons with substantially different excitation numbers caused by the pumping affecting polariton states of the system. This occurs when the Rabi interaction with coherent field is comparable to the field-matter coupling constant which in turn needs to be sufficient for the manifestation of strong coupling. This non-monotonic dependence of the fluorescence and scattering amplitudes on pump rate intensity pave the way for creation of nonlinear optical devices.
Light-matter strong coupling has been the subject of much attention in recent decades, giving optical systems unique features. However, properties of a system with strong coupling are determined by the properties of its components and are thus difficult to control. Here, we propose Floquet engineering, a technique of controlling the energy levels of a quantum system using external fields, as a method of manipulating a hybrid system of a molecule strongly coupled to a single-mode resonator. We show that an external field can change the relative positions of levels in an open strongly coupled system, leading to a change in the rates of transitions between them. We demonstrate that if the frequency of the pumping wave is close to polariton transitions in the hybrid system, nonmonotonic dependence of fluorescence and scattering amplitudes on pump intensity with a narrow resonance-like response occurs. We show that this phenomenon occurs due to hybridization of the lower and upper polaritons with substantially different excitation numbers caused by the pumping affecting polariton states of the system. This occurs when the Rabi interaction with the coherent field is comparable to the field-matter coupling constant, which in turn needs to be sufficient for the manifestation of strong coupling. This nonmonotonic dependence of the fluorescence and scattering amplitudes on pump rate intensity paves the way for the creation of nonlinear optical devices.
We explore the nonlinear response of tailor-cut light-matter hybrid states in a novel regime, where both the Rabi frequency induced by a coherent driving field and the vacuum Rabi frequency set by a cavity field are comparable to the carrier frequency of light. In this previously unexplored strong-field limit of ultrastrong coupling, subcycle pump-probe and multiwave mixing nonlinearities between different polariton states violate the normal-mode approximation while ultrastrong coupling remains intact, as confirmed by our mean-field model. We expect such custom-cut nonlinearities of hybridized elementary excitations to facilitate nonclassical light sources, quantum phase transitions, or cavity chemistry with virtual photons.
Bloch equations for the atomic population and the polarization/coherence and the equation of motion for the photon number in a laser are solved in steady state as a function of the pump rate. Two level atom and two modes of three levels atom are investigated. Close to threshold the usual linear dependence of the intensity on the pump rate in found for all cases. However, far above threshold strongly nonlinear dependence is encountered. In the cases for which the pump connects the lower lasing state to one of the excited states the character of the non-linearity differs crucially from the cases when the pump in not related directly to the lower lasing state. Non-monotonic dependence of laser intensity upon the pump rate is predicted. Detailed discussion of the nonlinear behavior is presented, including saturation and depletion effects.
The resonant Raman scattering in a three level system produces an optical pumping of molecules from the initial to the final states which are radiatively coupled to the intermediate resonant state. We consider the pumping that is produced by an intense, pulsed, monochromatic radiation field that is near-resonant with the initial resonance frequency. The Heitler–Ma damping theory is solved exactly for the case when the resonance fluorescence is weak compared to the Raman scattering, or any other processes which might cause irreversible decay of the resonant state. In particular, we examine the usefulness of dressed states to describe the intense field limit. The spectral line shape for the Raman scattering is obtained. The transient behavior following the onset of the laser pulse is examined and a careful analysis of the pumping rate and its relationship to both weak and strong field theories is presented.
We investigate the nonlinearities of custom-tailored ultrastrongly light-matter coupled states by driving them with both the vacuum electromagnetic field and strong coherent THz waveforms. In this novel regime, where both the Rabi frequency induced by the coherent field and the vacuum Rabi frequency set by the cavity field are on the order of the carrier frequency of light, we observe strong subcycle pump-probe and multiwave mixing nonlinearities and nonlinear polariton correlations, violating the normal-mode approximation. Such custom-cut nonlinearities of hybridized excitations set the stage for nonlinear optical control of deep-strong coupling, exploring quantum phase transitions or nonclassical light sources.
The nonstationary pump-probe interaction between short laser pulses propagating in a resonant optically dense coherent medium is considered. Special attention is paid to the case where the density of two-level particles is high enough that a considerable part of the energy of relatively weak external laser fields can be coherently absorbed and reemitted by the medium. Thus, the field of the medium reaction plays a key role in the interaction processes, which leads to collective behavior of an atomic ensemble in the strongly coupled light-matter system. Such behavior results in fast excitation interchanges between the field and a medium in the form of optical ringing, which is analogous to polariton beating in solid-state optics. This collective oscillating response, which can be treated as successive beats between light wave packets of different group velocities, is shown to significantly affect the propagation and amplification of the probe field under its nonlinear interaction with a nearly copropagating pump pulse. Depending on the probe-pump time delay, the probe transmission spectra show the appearance of either a specific doublet or coherent dip. The widths of these features are determined by the density-dependent field-matter coupling coefficient and increase during the propagation. Besides that, the widths of the coherent features, which appear close to resonance in the broadband probe spectrum, exceed the absorption-line width, since under the strong-coupling regime, the frequency of optical ringing exceeds the rate of incoherent relaxation. Contrary to stationary strong-field effects, the density- and coordinate-dependent transmission spectra of the probe manifest the importance of collective oscillations and cannot be obtained in the framework of a single-atom model.