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Laser Resonators, Microresonators, and Beam Control

Stimulated chiral light-matter interactions in biological microlasers

Zhiyi Yuan, Yunke Zhou, Yucheng Chen

Published Mar 4, 2021• 2 citations
Publisher

Abstract

Chiral light-matter interactions have emerged as a promising area in biophysics and quantum optics. Remarkable progress in enhancing chiral light-matter interactions have been investigated through passive resonators or spontaneous emission. Nevertheless, the interaction between chiral biomolecules and stimulated emission remains unexplored. Here we introduce the concept of a biological chiral laser by amplifying chiral light-matter interactions in an active resonator through stimulated emission process. Green fluorescent proteins or chiral biomolecules encapsulated in Fabry-Perot microcavity served as the gain material while excited by either left-handed or righthanded circularly polarized pump laser. Owing to the nonlinear pump energy dependence of stimulated emission, significant enhancement of chiral light-matter interactions was demonstrated. Detailed experiments and theory revealed that lasing dissymmetry factor is determined by molecular absorption dissymmetry factor at its excitation wavelength. Finally, chirality transfer was investigated under stimulated emission process through Forster resonance energy transfer. Our findings elucidate the mechanism of stimulated chiral light-matter interactions, providing new prospects for understanding light-matter interaction in biophysics, chiral sensing, and quantum photonics.

DOI
10.1117/12.2593443

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Chiral light-matter interactions have emerged as a promising area in biophysics and quantum optics. Remarkable progress in enhancing chiral light-matter interactions have been investigated through passive resonators or spontaneous emission. Nevertheless, the interaction between chiral biomolecules and stimulated emission remains unexplored. Here we introduce the concept of a biological chiral laser by amplifying chiral light-matter interactions in an active resonator through stimulated emission process. Green fluorescent proteins or chiral biomolecules encapsulated in Fabry-Perot microcavity served as the gain material while excited by either left-handed or righthanded circularly polarized pump laser. Owing to the nonlinear pump energy dependence of stimulated emission, significant enhancement of chiral light-matter interactions was demonstrated. Detailed experiments and theory revealed that lasing dissymmetry factor is determined by molecular absorption dissymmetry factor at its excitation wavelength. Finally, chirality transfer was investigated under stimulated emission process through Forster resonance energy transfer. Our findings elucidate the mechanism of stimulated chiral light-matter interactions, providing new prospects for understanding light-matter interaction in biophysics, chiral sensing, and quantum photonics.
Chiral light-matter interactions have emerged as a promising area in biophysics and quantum optics. Great progress in enhancing chiral light-matter interactions have been investigated through passive resonators or spontaneous emission. Nevertheless, the interaction between chiral biomolecules and stimulated emission remains unexplored. Here we introduce the concept of a biological chiral laser by amplifying chiral light-matter interactions in an active resonator through stimulated emission process. Green fluorescent proteins or chiral biomolecules encapsulated in Fabry-Perot microcavity served as the gain material while excited by either left-handed or right-handed circularly polarized pump laser. Owing to the nonlinear pump energy dependence of stimulated emission, significant enhancement of chiral light-matter interactions was demonstrated. Detailed experiments and theory revealed that a lasing dissymmetry factor is determined by molecular absorption dissymmetry factor at its excitation wavelength. Finally, chirality transfer was investigated under a stimulated emission process through resonance energy transfer. Our findings elucidate the mechanism of stimulated chiral light-matter interactions, providing better understanding of light-matter interaction in biophysics, chiral sensing, and quantum biophotonics.
Electromagnetically induced transparency and lasing without inversion are optical manifestations of quantum coherence control. Here we theoretically investigate these effects in a chiral molecule, coherently driven by an optical pump, finding that signal fields can undergo chiroptical absorption quenching or amplification within particular spectral windows at pump intensities as low as ≈ 1kW/cm 2 . Our calculations reveal that molecular chirality has the capacity to dramatically alter quantum coherence phenomena at peculiar wavelength ranges, modulating efficiently circular dichroism depending on the polarisation state of both pump and signal fields and the molecular orientation. We find that, for a given molecular orientation, the dissymmetry factor probed upon right/left-circular polarisation excitation by the signal can get maximised by pump polarisation tuning and the signal direction. By averaging over impinging signal orientations, we find that the orientation-averaged dissymmetry factor can diverge owing to electromagnetically induced transparency producing vanishing averaged absorption cross-sections.
This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.
Recent development of spectroscopic techniques based on quantum states of light can precipitate many breakthroughs in observing and controlling light-matter interactions in biological materials on a fundamental quantum level. For this reason, the generation of entangled light in biologically produced fluorescent proteins would be promising because of their biocompatibility. Here we demonstrate the generation of polarization-entangled two-photon state through spontaneous four-wave mixing in enhanced green fluorescent proteins. The reconstructed density matrix indicates that the entangled state is subject to decoherence originating from two-photon absorption. However, the prepared state is less sensitive to environmental decoherence because of the protective β-barrel structure that encapsulates the fluorophore in the protein. We further explore the quantumness, including classical and quantum correlations, of the state in the decoherence environment. Our method for photonic entanglement generation may have potential for developing quantum spectroscopic techniques and quantum-enhanced measurements in biological materials.
Summary form only given. Controlling the interaction of light and matter is the basis for diverse applications ranging from light technology to quantum information processing. Nowadays, many of these applications are based on nanophotonic structures. It turns out that the confinement of light in such nanostructures imposes an inherent link between its local polarization and its propagation direction, also referred to as spin-momentum locking of light [1]. Remarkably, this leads to chiral, i.e., propagation direction-dependent effects in the emission and absorption of light, and elementary processes of light-matter interaction are fundamentally altered. For example, when coupling plasmonic particles or atoms to evanescent fields, the intrinsic mirror symmetry of the particles' emission can be broken. In our group, we observed this effect in the interaction between single rubidium atoms and the evanescent part of a light field that is confined by continuous total internal reflection in a whispering-gallery-mode microresonator [2]. In the following, this allowed us to realize chiral nanophotonic interfaces in which the emission direction of light into the structure is controlled by the polarization of the excitation light [3] or by the internal quantum state of the emitter [4], respectively. Moreover, we employed this chiral interaction to demonstrate an integrated optical isolator [5] as well as an integrated optical circulator [6] which operate at the single-photon level and which exhibit low loss. The latter are the first two examples of a new class of nonreciprocal nanophotonic devices which exploit the chiral interaction between single quantum emitters and transversally confined photons.