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Direct Observation of Sub-Poissonian Temporal Statistics in a Continuous Free-Electron Beam with Subpicosecond Resolution.
Phys Rev Lett
March 2024
Department of Applied Physics, Eindhoven University of Technology, Groene Loper 19, 5612 AP, Eindhoven, The Netherlands.
We present a novel method to measure the arrival time statistics of continuous electron beams with subpicosecond resolution, based on the combination of an rf deflection cavity and fast single electron imaging. We observe Poissonian statistics within time bins from 100 to 2 ns and increasingly pronounced sub-Poissonian statistics as the time bin decreases from 2 ps to 340 fs. This 2D streak camera, in principle, enables femtosecond-level arrival time measurements, paving the way to observing Pauli blocking effects in electron beams and thus serving as an essential diagnostic tool toward degenerate electron beam sources for free-electron quantum optics.
View Article and Find Full Text PDFPhotochemistry Journey to Multielectron and Multiproton Chemical Transformation.
J Am Chem Soc
September 2022
Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, The Chinese Academy of Sciences, Beijing 100190, P. R. China.
The odyssey of photochemistry is accompanied by the journey to manipulate "electrons" and "protons" in time, in space, and in energy. Over the past decades, single-electron (1e) photochemical transformations have brought marvelous achievements. However, as each photon absorption typically generates only one exciton pair, it is exponentially challenging to accomplish multielectron and proton photochemical transformations.
View Article and Find Full Text PDFToward Å-fs-meV resolution in electron microscopy: systematic simulation of the temporal spread of single-electron packets.
Phys Chem Chem Phys
October 2021
Department of Chemical Engineering and Materials Science, University of Minnesota, 421 Washington Avenue SE, Minneapolis, MN, 55455, USA.
Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å-fs-meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform - attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales.
View Article and Find Full Text PDFOptical Properties and Excited-State Dynamics of Atomically Precise Gold Nanoclusters.
Annu Rev Phys Chem
April 2021
Department of Chemistry, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, USA; email:
Understanding the excited-state dynamics of nanomaterials is essential to their applications in photoenergy storage and conversion. This review summarizes recent progress in the excited-state dynamics of atomically precise gold (Au) nanoclusters (NCs). We first discuss the electronic structure and typical relaxation pathways of Au NCs from subpicoseconds to microseconds.
View Article and Find Full Text PDFMulticolor femtosecond pump-probe system with single-electron sensitivity at low temperatures and high magnetic fields.
Rev Sci Instrum
December 2019
Department of Physics and Center for Applied Photonics, University of Konstanz, D-78464 Konstanz, Germany.
We present an ultrafast spectroscopy system designed for temporal and spectral resolution of transient transmission changes after excitation of single electrons in solid-state quantum structures. The system is designed for optimum long-term stability, offering the option of hands-off operation over several days. Pump and probe pulses are generated in a versatile Er:fiber laser system where visible photon energies may be tuned independently from 1.
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