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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

A simple and accurate model of collectively enhanced optical non-linearities

Martin Cordier, Max Schemmer, Philipp Schneeweiß, Jürgen Volz, Arno Rauschenbeutel

Published Jun 21, 2021• 0 citations
Publisher

Abstract

The investigation of resonance fluorescence of two-level systems has played a fundamental role in the development of quantum optics. Pioneering experiments have demonstrated that the fluorescence of a single emitter exhibits many interesting features such as the Mollow triplet, photon-antibunching as well as squeezing.
DOI
10.1109/cleo/europe-eqec52157.2021.9542656

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Field quantization is fundamental to quantum optics and polaritonic chemistry, enabling exploration of light–matter interactions at the quantum level. We report resonant coupling between the two-level excitation of a dinickel (Ni₂) complex and its locally recycled scattering field under ambient, cavity-free conditions. This Ni₂ system exhibits hallmark resonance-fluorescence features, including Rabi doublets and Mollow triplets, with strong coupling achieved under weak, non-resonant excitation. The Ni₂ unit functions as a diatomic resonator, enhancing photon scattering and forming a Jaynes–Cummings molecule. Simulations of second-order correlation functions confirm photon antibunching and underdamped Rabi oscillations. Collective coupling strength scales linearly with the number of molecules (N), surpassing Tavis–Cummings model predictions and reaching the ultrastrong coupling regime. These findings establish Ni₂ complexes as robust molecular quantum systems, offering a chemically tunable platform for quantum information processing and coherent chemical control at the molecular scale.
Field quantization is fundamental to quantum optics and polaritonic chemistry, enabling exploration of light–matter interactions at the quantum level. We report resonant coupling between the two-level excitation of a dinickel (Ni₂) complex and its locally recycled scattering field under ambient, cavity-free conditions. This Ni₂ system exhibits hallmark resonance-fluorescence features, including Rabi doublets and Mollow triplets, with strong coupling achieved under weak, non-resonant excitation. The Ni₂ unit functions as a diatomic resonator, enhancing photon scattering and forming a Jaynes–Cummings molecule. Simulations of second-order correlation functions confirm photon antibunching and underdamped Rabi oscillations. Collective coupling strength scales linearly with the number of molecules (N), surpassing Tavis–Cummings model predictions and reaching the ultrastrong coupling regime. These findings establish Ni₂ complexes as robust molecular quantum systems, offering a chemically tunable platform for quantum information processing and coherent chemical control at the molecular scale.
The coherent interaction between a two-level system and electromagnetic fields serves as a foundation for fundamental quantum physics and modern photonic quantum technology. A profound example is resonance fluorescence, where the non-classical photon emission appears in the form of a Mollow-triplet when a two-level system is continuously driven by a resonant laser. Pushing resonance fluorescence from a static to dynamic regime by using short optical pulses generates on-demand emissions of highly coherent single photons. Further increasing the driving strength in the dynamical regime enables the pursuit of exotic non-classical light emission in photon number superposition, photon number entanglement, and photon bundle states. However, the long-sought-after spectrum beyond the Mollow-triplet, a characteristic of dynamic resonance fluorescence under strong driving strength, has not been observed yet. Here we report the direct observation and systematic investigations of dynamic resonance fluorescence spectra beyond the Mollow-triplet in a solid-state cavity quantum electrodynamic system. The dynamic resonance fluorescence spectra with up to five pairs of side peaks, excitation detuning induced spectral asymmetry, and cavity filtering effect are observed and quantitatively modeled by a full quantum model with phonon scattering included. Time-resolved measurements further reveal that the multiple side peaks originate from interference of the emission associated with different temporal positions of the excitation pulses. Our work facilitates the generation of a variety of exotic quantum states of light with dynamic driving of two-level systems.