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.
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.
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.
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