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.
Microlasers have emerged as a promising approach for the detection or identification of different biomolecules. Most lasers were designed to reflect changes of molecular concentration within the cavity, without being able to characterize biophysical changes in the gain medium. Here, we report a strategy to extract and amplify polarized laser emissions from small molecules and demonstrate how molecular rotation interplays with lasing at the nanoscale. The concept of molecular lasing polarization was proposed and was first evidenced to increase accordingly as the fluorophore binds to larger biomolecules in a microcavity. By detecting the molecular rotational correlation time through stimulated emission, small molecules could be distinguished while conventional fluorescence polarization cannot. Theoretical models were developed to elucidate the underlying mechanisms. Finally, different types of small molecules were analyzed by adopting a Fabry-Pérot optofluidic laser. The results suggest an entirely new tool to quantify small molecules and guidance for laser emissions to characterize biophysical properties down to the molecular level.
Liquid droplets offer a great number of opportunities in biochemical and physical research studies in which droplet-based microlasers have come into play over the past decade. While the recent emergence of droplet lasers has demonstrated their powerful capabilities in amplifying subtle molecular changes inside the cavity, the optical interactions between droplet resonators and an interface remain unclear. We revealed the underlying mechanism of droplet lasers when interacting with a droplet–solid interface and explored its correlation with intermolecular forces. A vertically oriented oscillation mode—arc-like mode—was discovered, where the number of lasing modes and their Q-factors increase with the strength of interfacial hydrophobicity. Both experimental and theoretical results demonstrated that hydrophobicity characterized by contact angle and interfacial tension plays a significant role in the geometry of droplet cavity and laser mode characteristics. Finally, we demonstrated how tiny forces induced by proteins and peptides could strongly modulate the lasing output in droplet resonators. Our findings illustrate the potential of exploiting optical resonators to amplify intermolecular force changes, providing comprehensive insights into lasing actions modulated by interfaces and applications in biophysics.
Optical barcodes have demonstrated a great potential in multiplexed bioassays and cell tracking for their distinctive spectral fingerprints. The vast majority of optical barcodes were designed to identify a specific target by fluorescence emission spectra, without being able to characterize dynamic changes in response to analytes through time. To overcome these limitations, the concept of the bioresponsive dynamic photonic barcode was proposed by exploiting interfacial energy transfer between a microdroplet cavity and binding molecules. Whispering-gallery modes resulting from cavity-enhanced energy transfer were therefore converted into photonic barcodes to identify binding activities, in which more than trillions of distinctive barcodes could be generated by a single droplet. Dynamic spectral barcoding was achieved by a significant improvement in terms of signal-to-noise ratio upon binding to target molecules. Theoretical studies and experiments were conducted to elucidate the effect of different cavity sizes and analyte concentrations. Time-resolved fluorescence lifetime was implemented to investigate the role of radiative and non-radiative energy transfer. Finally, microdroplet photonic barcodes were employed in biodetection to exhibit great potential in fulfilling biomedical applications.
Electrostatics plays a critical function in most biomolecules, therefore monitoring subtle biomolecular bindings and dynamics via the electrostatic changes of biomolecules at biointerfaces has been an attractive topic recently and has provided the basis in diagnosis and biomedical science. Here we present a bioelectrostatic responsive microlaser based on liquid crystal (LC) droplet and explored its application for ultrasensitive detection of negatively charged biomolecules. Whispering gallery mode (WGM) lasing from positively charged LC microdroplets was applied as the optical resonator, where the lasing wavelength shift was employed as a sensing parameter. With the dual impacts from whispering-gallery mode and liquid crystal, molecular binding signals will be amplified in such LC droplet sensors. It is found that molecular electrostatic changes at the biointerface of droplet triggered wavelength shift in lasing spectra. The total wavelength shift increased proportionally with the adhering target concentrations. Compared to a conventional polarized optical microscope, significant improvements in sensitivity and dynamic range by four orders of magnitude were achieved. Our work indicated that the surface-to-volume ratio plays a critical role in the detection sensitivity in WGM laser-based microsensors. Finally, bovine serum albumin and specific biosensing using streptavidin and biotin were exploited to demonstrate the potential applications of microlasers with a detection limit on the order of 1 pM. We anticipate this approach will open new possibilities for the ultrasensitive label-free detection of charged biomolecules and molecular interactions by providing a lower detection limit than conventional methods.
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