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|a E 1.99:1810824
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|a E 1.99:1810824
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|a Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy
|h [electronic resource]
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|a Washington, D.C. :
|b United States. Department of Energy. Office of Science ;
|a Oak Ridge, Tenn. :
|b Distributed by the Office of Scientific and Technical Information, U.S. Department of Energy,
|c 2021.
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| 300 |
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|a Size: Article No. 044301 :
|b digital, PDF file.
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|a text
|b txt
|2 rdacontent.
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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 07/08/2021.
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|a "Journal ID: ISSN 2329-7778."
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|a "Other: ark:/13030/qt0nk0m6bk."
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|a ": US2213102."
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|a Brausse, Felix ; Borgwardt, Mario ; Mahl, Johannes ; Fraund, Matthew ; Roth, Friedrich ; Blum, Monika ; Eberhardt, Wolfgang ; Gessner, Oliver ;
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|a USDOE.
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|a Lawrence Berkeley National Laboratory, E-Scholarship Repository, Berkeley, CA (United States)
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|a We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump-probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump-probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.
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|b AC02-05CH11231.
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|a 72 physics of elementary particles and fields
|2 local.
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|a Xray photoelectron spectroscopy
|2 local.
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| 650 |
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|a Timeresolved photoemission spectroscopy
|2 local.
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| 650 |
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|a Time resolved xray spectroscopy
|2 local.
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| 650 |
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|a Surface dynamics
|2 local.
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|a Interface dynamics
|2 local.
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|a Chemical dynamics
|2 local.
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| 650 |
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|a X ray photon correlation spectroscopy
|2 local.
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| 650 |
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|a Correlation spectroscopy
|2 local.
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| 650 |
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|a X-ray photoelectron spectroscopy
|2 local.
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| 650 |
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|a Time-resolved photoemission spectroscopy
|2 local.
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| 650 |
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|a Physics of elementary particles and fields
|2 local.
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| 650 |
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|a Time resolved x-ray spectroscopy
|2 local.
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| 710 |
2 |
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|a Lawrence Berkeley National Laboratory.
|4 res.
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| 710 |
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|a United States.
|b Department of Energy.
|b Office of Science.
|4 spn.
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| 710 |
2 |
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|a Lawrence Berkeley National Laboratory, E-Scholarship Repository, Berkeley, CA (United States).
|f res.
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| 710 |
1 |
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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 https://www.osti.gov/servlets/purl/1810824
|z Full Text (via OSTI)
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|a .b119267196
|b 02-28-23
|c 08-27-21
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|a web
|b 12-08-22
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|p Can circulate
|a University of Colorado Boulder
|b Online
|c Online
|d Online
|e E 1.99:1810824
|h Superintendent of Documents classification
|i web
|n 1
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