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. Timeresolved 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.

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. 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.

Phycobiliproteins are a class of light-harvesting fluorescent proteins existing in cyanobacteria and microalgae, which harvest light and convert it into electricity. Owing to recent demands on environmental-friendly and renewable apparatuses, phycobiliproteins have attracted substantial interest in bioenergy and sustainable devices. However, converting energy from biological materials remains challenging to date. Herein, we report a novel scheme to enhance biological light-harvesting through light–matter interactions at the biointerface of whispering-gallery modes (WGMs), where phycobiliproteins were employed as the active gain material. By exploiting microdroplets as a carrier for light-harvesting biomaterials, strong local electric field enhancement and photon confinement at the cavity interface resulted in significantly enhanced bio-photoelectricity. A threshold-like behavior was discovered in photocurrent enhancement and the WGM modulated fluorescence. Systematic studies of biologically produced photoelectricity and optical mode resonance were carried out to illustrate the impact of the cavity quality factor, structural geometry, and refractive indices. Finally, a biomimetic system was investigated by exploiting cascade energy transfer in phycobiliprotein assembly composed of three light-harvesting proteins. The key findings not only highlight the critical role of optical cavity in light-harvesting but also offer deep insights into light energy coupling in biomaterials.

No abstract