Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1021/acs.nanolett.7b05223 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Rapid Synthesis of Carbon-Supported Ru-RuO₂ Heterostructures for Efficient Electrochemical Water Splitting.
Adv Sci (Weinh)
January 2025
Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California, 95064, USA.
Development of high-performance electrocatalysts for water splitting is crucial for a sustainable hydrogen economy. In this study, rapid heating of ruthenium(III) acetylacetonate by magnetic induction heating (MIH) leads to the one-step production of Ru-RuO₂/C nanocomposites composed of closely integrated Ru and RuO₂ nanoparticles. The formation of Mott-Schottky heterojunctions significantly enhances charge transfer across the Ru-RuO interface leading to remarkable electrocatalytic activities toward both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1 m KOH.
View Article and Find Full Text PDFInfluence of Photoemission Geometry on Timing and Efficiency in 4D Ultrafast Electron Microscopy.
Chemphyschem
January 2025
University of Minnesota Twin Cities, Chemical Engineering and Materials Science, 421 Washington Avenue SE, 55455, Minneapolis, UNITED STATES OF AMERICA.
Broader adoption of 4D ultrafast electron microscopy (UEM) for the study of chemical, materials, and quantum systems is being driven by development of new instruments as well as continuous improvement and characterization of existing technologies. Perhaps owing to the still-high barrier to entry, the full range of capabilities of laser-driven 4D UEM instruments has yet to be established, particularly when operated at extremely low beam currents (~fA). Accordingly, with an eye on beam stability, we have conducted particle tracing simulations of unconventional off-axis photoemission geometries in a UEM equipped with a thermionic-emission gun.
View Article and Find Full Text PDFCo-Atomic Interface Minimizing Charge Transfer Barrier in Polytypic Perovskites for CO Photoreduction.
Adv Sci (Weinh)
January 2025
School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu, 611731, China.
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr-CsPbBr polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface.
View Article and Find Full Text PDFComputational microscopy with coherent diffractive imaging and ptychography.
Nature
January 2025
Department of Physics and Astronomy, University of California, Los Angeles, Los Angeles, CA, USA.
Microscopy and crystallography are two essential experimental methodologies for advancing modern science. They complement one another, with microscopy typically relying on lenses to image the local structures of samples, and crystallography using diffraction to determine the global atomic structure of crystals. Over the past two decades, computational microscopy, encompassing coherent diffractive imaging (CDI) and ptychography, has advanced rapidly, unifying microscopy and crystallography to overcome their limitations.
View Article and Find Full Text PDFAnnealing Effect on Linear and Ultrafast Nonlinear Optical Properties of BiTe Thin Films.
Materials (Basel)
December 2024
Department of Optical Science and Engineering, Shanghai Ultra-Precision Optical Manufacturing Engineering Center, Fudan University, Shanghai 200433, China.
In recent years, the fabrication of materials with large nonlinear optical coefficients and the investigation of methods to enhance nonlinear optical performance have been in the spotlight. Herein, the bismuth telluride (BiTe) thin films were prepared by radio-frequency magnetron sputtering and annealed in vacuum at various temperatures. The structural and optical properties were characterized and analyzed using X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, spectroscopic ellipsometry, and UV/VIS/NIR spectrophotometry.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!