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Over the past decade, the proliferation of pulsed laser sources with high repetition rates has facilitated a merger of ultrafast time-resolved spectroscopy with imaging microscopy. In transient absorption microscopy (TAM), the excited-state dynamics of a system are tracked by measuring changes in the transmission of a focused probe pulse following photoexcitation of a sample. Typically, these experiments are done using a photodiode detector and lock-in amplifier synchronized with the laser and images highlighting spatial heterogeneity in the TAM signal are constructed by scanning the probe across a sample. Performing TAM by instead imaging a spatially defocused widefield probe with a multipixel camera could dramatically accelerate the acquisition of spatially resolved dynamics, yet approaches for such widefield imaging generally suffer from reduced signal-to-noise due to an incompatibility of multipixel cameras with high-frequency lock-in detection. Herein, we describe implementation of a camera capable of high-frequency lock-in detection, thereby enabling widefield TAM imaging at rates matching those of high repetition rate lasers. Transient images using a widefield probe and two separate pump pulse configurations are highlighted. In the first, a widefield probe was used to image changes in the spatial distribution of photoexcited molecules prepared by a tightly focused pump pulse, while in the second, a widefield probe detected spatial variations in photoexcited dynamics within a heterogeneous organic crystal excited by a defocused pump pulse. These results highlight the ability of high-sensitivity lock-in detection to enable widefield TAM imaging, which can be leveraged to further our understanding of excited-state dynamics and excitation transport within spatially heterogeneous systems.more » « lessFree, publicly-accessible full text available July 18, 2025
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Free, publicly-accessible full text available April 27, 2025
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Time-resolved spectroscopy of plasmonic nanoparticles is a vital technique for probing their ultrafast electron dynamics and subsequent acoustic and photothermal properties. Traditionally, these experiments are performed with spectrally broad probe beams on the ensemble level to achieve high signal amplitudes. However, the relaxation dynamics of plasmonic nanoparticles is highly dependent on their size, shape, and crystallinity. As such, the inherent heterogeneity of most nanoparticle samples can complicate efforts to build microscopic models for these dynamics solely on the basis of ensemble measurements. Although approaches for collecting time-resolved microscopy signals from individual nanoparticles at selected probe wavelengths have been demonstrated, acquiring time-resolved spectra from single objects remains challenging. Here, we demonstrate an alternate method that efficiently yields the time-resolved spectra of a single gold nanodisk in one measurement. By modulating the frequency-doubled output of a 96 MHz Ti:sapphire oscillator at 8 kHz, we are able to use a lock-in pixel-array camera to detect photoinduced changes in the transmission of a white light continuum probe derived from a photonic crystal fiber to produce broadband femtosecond transmission spectra of a single gold nanodisk. We also compare the performance of the lock-in camera for the same single nanoparticle to measurements with a single-element photodiode and find comparable sensitivities. The lock-in camera thus provides a major advantage due to its ability to multiplex spectral detection, which we utilize here to capture both the electronic dynamics and acoustic vibrations of a single gold nanodisk following ultrafast laser excitation.more » « lessFree, publicly-accessible full text available May 30, 2025
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Nancy Grace Roman Space Telescope will revolutionize our understanding of the Galactic Bulge with its Galactic Bulge Time Domain survey. At the same time, Rubin Observatories's Legacy Survey of Space and Time (LSST) will monitor billions of stars in the Milky Way. The proposed Roman survey of the Galactic Plane, with its NIR passbands and exquisite spacial resolution, promises groundbreaking insights for a wide range of time-domain galactic astrophysics. In this white paper, we describe the scientific returns possible from the combination of the Roman Galactic Plane Survey with the data from LSST.more » « lessFree, publicly-accessible full text available June 1, 2025
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Abstract. Air–water gas exchange is essential to understanding and quantifying many biogeochemical processes in streams and rivers, including greenhouse gas emissions and metabolism. Gas exchange depends on two factors, which are often quantified separately: (1) the air–water concentration gradient of the gas and (2) the gas exchange velocity. There are fewer measurements of gas exchange velocity compared to concentrations in streams and rivers, which limits accurate characterization of air–water gas exchange (i.e., flux rates). The National Ecological Observatory Network (NEON) conducts SF6 gas-loss experiments in 22 of their 24 wadeable streams using standardized methods across all experiments and sites, and publishes raw concentration data from these experiments on the NEON data portal. NEON also conducts NaCl injections that can be used to characterize hydraulic geometry at all 24 wadeable streams. These NaCl injections are conducted both as part of the gas-loss experiments and separately. Here, we use these data to estimate gas exchange and water velocity using the reaRate R package. The dataset presented includes estimates of hydraulic parameters, cleaned raw concentration SF6 tracer-gas data (including removing outliers and failed experiments), estimated SF6 gas-loss rates, normalized gas exchange velocities (k600; m d−1) and normalized depth-dependent gas exchange rates (K600; d−1). This dataset provides one of the largest compilations of gas-loss experiments (n=339) in streams to date. This dataset is unique in that it contains gas exchange estimates from repeated experiments in geographically diverse streams across a range of discharges. In addition, this dataset contains information on the hydraulic geometry of all 24 NEON wadeable streams, which will support future research using NEON aquatic data. This dataset is a valuable resource that can be used to explore both within- and across-reach variability in the hydraulic geometry and gas exchange velocity in streams. The data are available at https://doi.org/10.6073/pasta/18dcc1871ee71cf0b69f2ee4082839d0 (Aho et al., 2024), and the reaRate R package code is available at https://doi.org/10.5281/zenodo.12786089 (Cawley et al., 2024).more » « less
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Materials that undergo singlet fission are of interest for their use in light-harvesting, photocatalysis, and quantum information science, but their ability to undergo fission can be sensitive to local variations in molecular packing. Herein we employ transient absorption microscopy, molecular dynamics simulations, and electronic structure calculations to interrogate how structures found at the edges of orthorhombic rubrene crystals impact singlet fission. Within a micrometer-scale spatial region at the edges of rubrene crystals, we find that the rate of singlet fission increases nearly 4-fold. This observation is consistent with formation of a region at crystal edges with reduced order that accelerates singlet fission by disrupting the symmetry found in rubrene’s orthorhombic crystal structure. Our work demonstrates that structural distortions of singlet fission materials can be used to control fission in time and in space, potentially offering a means of controlling this process in light harvesting and quantum information applications.more » « less
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Plant xylem colonization is the hallmark of vascular wilt diseases caused by phytopathogens within the Fusarium oxysporum species complex. Recently, xylem colonization has also been reported among endophytic F. oxysporum strains, resulting in some uncertainty. This study compares xylem colonization processes by pathogenic versus endophytic strains in Arabidopsis thaliana and Solanum lycopersicum, using Arabidopsis pathogen Fo5176, tomato pathogen Fol4287, and the endophyte Fo47, which can colonize both plant hosts. We observed that all strains were able to advance from epidermis to endodermis within 3 days postinoculation (dpi) and reached the root xylem at 4 dpi. However, this shared progression was restricted to lateral roots and the elongation zone of the primary root. Only pathogens reached the xylem above the primary-root maturation zone (PMZ). Related to the distinct colonization patterns, we also observed stronger induction of callose at the PMZ and lignin deposition at primary-lateral root junctions by the endophyte in both plants. This observation was further supported by stronger induction of Arabidopsis genes involved in callose and lignin biosynthesis during the endophytic colonization (Fo47) compared with the pathogenic interaction (Fo5176). Moreover, both pathogens encode more plant cell wall–degrading enzymes than the endophyte Fo47. Therefore, observed differences in callose and lignin deposition could be the combination of host production and the subsequent fungal degradation. In summary, this study demonstrates spatial differences between endophytic and pathogenic colonization, strongly suggesting that further investigations of molecular arm-races are needed to understand how plants differentiate friend from foe. [Formula: see text] Copyright © 2023 The Author(s). This is an open access article distributed under the CC BY-NC-ND 4.0 International license .more » « less
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Leibovich-Raveh, Tali (Ed.)Number-recognition tasks, such as the how-many task, involve set-to-word mapping, and number-creation tasks, such as the give-n task, entail word-to-set mapping. The present study involved comparing sixty 3-year-olds’ performance on the two tasks with collections of one to three items over three time points about 3 weeks apart. Inconsistent with the sparse evidence indicating equivalent task performance, an omnibus test indicated that success differed significantly by task (and set size but not by time). A follow-up analysis indicated that the hypothesis that success emerges first on the how-many task was, in general, significantly superior to the hypothesis of simultaneous development. It further indicated the how-many-first hypothesis was superior to a give-n- first hypothesis for sets of three. A theoretical implication is that set-to-word mapping appears to develop before word-to-set mapping, especially in the case of three. A methodological implication is that the give-n task may underestimate a key aspect of children’s cardinal understanding of small numbers. Another is that the traditional give-n task, which requires checking an initial response by one-to-one counting, confounds pre-counting and counting competencies.more » « less