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|a (TOE)ost1465130
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|a (TOE)1465130
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|a E 1.99:1465130
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|a E 1.99:1465130
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|a Ultrabroadband 2D electronic spectroscopy with high-speed, shot-to-shot detection
|h [electronic resource]
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|a Washington, D.C. :
|b United States. Department of Energy. Office of Basic Energy Sciences ;
|a Oak Ridge, Tenn. :
|b distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
|c 2017.
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|a p. 18950-18962 :
|b digital, PDF file.
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|a text
|b txt
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|a computer
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|2 rdamedia.
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|a online resource
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|a Published through SciTech Connect.
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|a 07/27/2017.
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|a Optics Express 25 16 ISSN 1094-4087; OPEXFF AM.
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|a Minjung Son; Sandra Mosquera-Vázquez; Gabriela S. Schlau-Cohen.
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|a Two-dimensional electronic spectroscopy (2DES) is an incisive tool for disentangling excited state energies and dynamics in the condensed phase by directly mapping out the correlation between excitation and emission frequencies as a function of time. Despite its enhanced frequency resolution, the spectral window of detection is limited to the laser bandwidth, which has often hindered the visualization of full electronic energy relaxation pathways spread over the entire visible region. Here, we describe a high-sensitivity, ultrabroadband 2DES apparatus. We report a new combination of a simple and robust setup for increased spectral bandwidth and shot-to-shot detection. We utilize 8-fs supercontinuum pulses generated by gas filamentation spanning the entire visible region (450 - 800 nm), which allows for a simultaneous interrogation of electronic transitions over a 200-nm bandwidth, and an all-reflective interferometric delay system with angled nanopositioner stages achieves interferometric precision in coherence time control without introducing wavelength-dependent dispersion to the ultrabroadband spectrum. To address deterioration of detection sensitivity due to the inherent instability of ultrabroadband sources, we introduce a 5-kHz shot-to-shot, dual chopping acquisition scheme by combining a high-speed line-scan camera and two optical choppers to remove scatter contributions from the signal. Comparison of 2D spectra acquired by shot-to-shot detection and averaged detection shows a 15-fold improvement in the signal-to-noise ratio. In conclusion, this is the first direct quantification of detection sensitivity on a filamentation-based ultrabroadband 2DES apparatus.
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|b SC0001088.
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|a Other Instrumentation.
|2 edbsc.
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|a Inorganic, Organic, Physical, And Analytical Chemistry.
|2 edbsc.
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| 710 |
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|a Massachusetts Institute of Technology.
|4 res.
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|a United States.
|b Department of Energy.
|b Office of Basic Energy Sciences.
|4 spn.
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| 710 |
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|a United States.
|b Department of Energy.
|b Office of Scientific and Technical Information.
|4 dst.
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|u http://www.osti.gov/scitech/biblio/1465130
|z Online Access (via OSTI)
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| 907 |
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|a .b105023553
|b 03-09-23
|c 05-17-19
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| 998 |
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|a web
|b 05-17-19
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|f eng
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|s 7d39475e-9efb-57c9-a02e-74629504ed63
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| 952 |
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|p Can circulate
|a University of Colorado Boulder
|b Online
|c Online
|d Online
|e E 1.99:1465130
|h Superintendent of Documents classification
|i web
|n 1
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