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Title: Ultrafast time-resolved extreme ultraviolet (XUV) photoelectron spectroscopy of hole transfer in a Zn/n-GaP Schottky junction

Abstract

The addition of a metal overlayer to a semiconductor photocatalyst is a frequently used synthetic route to passivate the surface and, via the formation of a Schottky barrier, to enhance catalytic activity of the photocatalyst material. While it is known that Schottky junctions decrease recombination by charge separation, measurements of the depletion region dynamics have remained elusive. Here, we use ultrafast pump-probe transient photoelectron spectroscopy to measure material-specific dynamics of the Zn/n-GaP(100) system. Through photoemission measurements the Schottky barrier height is determined to be 2.1± 0.1eV at 10 monolayers of total Zn deposition. Transient photoemission measurements utilizing a 400 nm pump pulse show that, after excitation, holes are transferred from n-GaP(100) to the Zn overlayer within a few ps, as evidenced by shifts of the Zn 3d and Ga 3d core levels to higher binding energies. Within the timescale of the experiment (130 ps) no carrier recombination is observed in the junction. Furthermore, a long-lived surface photovoltage signal is observed at times >1 ms after photoexcitation. This work further exemplifies the potential of transient extreme ultraviolet photoelectron spectroscopy as a material-specific technique for the study of heterojunctions.

Authors:
 [1];  [2];  [3]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States); Purdue Univ., West Lafayette, IN (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1616966
Grant/Contract Number:  
AC02-05CH11231; FA9550-14-1-0154
Resource Type:
Accepted Manuscript
Journal Name:
Structural Dynamics
Additional Journal Information:
Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2329-7778
Publisher:
American Crystallographic Association/AIP
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Marsh, Brett M., Lamoureux, Bethany R., and Leone, Stephen R. Ultrafast time-resolved extreme ultraviolet (XUV) photoelectron spectroscopy of hole transfer in a Zn/n-GaP Schottky junction. United States: N. p., 2018. Web. doi:10.1063/1.5046776.
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Marsh, Brett M., Lamoureux, Bethany R., & Leone, Stephen R. Ultrafast time-resolved extreme ultraviolet (XUV) photoelectron spectroscopy of hole transfer in a Zn/n-GaP Schottky junction. United States. https://doi.org/10.1063/1.5046776
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Marsh, Brett M., Lamoureux, Bethany R., and Leone, Stephen R. Mon . "Ultrafast time-resolved extreme ultraviolet (XUV) photoelectron spectroscopy of hole transfer in a Zn/n-GaP Schottky junction". United States. https://doi.org/10.1063/1.5046776. https://www.osti.gov/servlets/purl/1616966.
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@article{osti_1616966,
title = {Ultrafast time-resolved extreme ultraviolet (XUV) photoelectron spectroscopy of hole transfer in a Zn/n-GaP Schottky junction},
author = {Marsh, Brett M. and Lamoureux, Bethany R. and Leone, Stephen R.},
abstractNote = {The addition of a metal overlayer to a semiconductor photocatalyst is a frequently used synthetic route to passivate the surface and, via the formation of a Schottky barrier, to enhance catalytic activity of the photocatalyst material. While it is known that Schottky junctions decrease recombination by charge separation, measurements of the depletion region dynamics have remained elusive. Here, we use ultrafast pump-probe transient photoelectron spectroscopy to measure material-specific dynamics of the Zn/n-GaP(100) system. Through photoemission measurements the Schottky barrier height is determined to be 2.1± 0.1eV at 10 monolayers of total Zn deposition. Transient photoemission measurements utilizing a 400 nm pump pulse show that, after excitation, holes are transferred from n-GaP(100) to the Zn overlayer within a few ps, as evidenced by shifts of the Zn 3d and Ga 3d core levels to higher binding energies. Within the timescale of the experiment (130 ps) no carrier recombination is observed in the junction. Furthermore, a long-lived surface photovoltage signal is observed at times >1 ms after photoexcitation. This work further exemplifies the potential of transient extreme ultraviolet photoelectron spectroscopy as a material-specific technique for the study of heterojunctions.},
doi = {10.1063/1.5046776},
journal = {Structural Dynamics},
number = 5,
volume = 5,
place = {United States},
year = {Mon Oct 22 00:00:00 EDT 2018},
month = {Mon Oct 22 00:00:00 EDT 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1063/1.5046776
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Cited by: 3 works
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Figures / Tables:

FIG. 1 FIG. 1: (a) Photoemission spectrum and band structure of n-GaP(100). (b) Photoemission spectrum and band structure of 10 ML Zn/n-GaP(100). (c) Enlarged view of the valence regions of n-GaP and 10 ML Zn/n-GaP. Dashed lines show the linear fit of n-GaP as well as the Fermi-Dirac fit for 10 MLmore » Zn/n-GaP(100). (d) Measured barrier height as a function of Zn coverage.« less
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Intrinsic Optical Absorption of Gallium Phosphide between 2.33 and 3.12 eV
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Ultrafast time resolution in scanned probe microscopies: Surface photovoltage on Si(111)–(7×7)
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Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation
journal, May 2014

Femtosecond time-resolved core-level photoelectron spectroscopy tracking surface photovoltage transients on p –GaAs
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Photo-Electrochemical Behaviors of Semiconductor Electrodes Coated with thin Metal Films
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