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Title: Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20 cm –3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.
Authors:
 [1] ; ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6] ;  [3] ;  [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Technion - Israel Institute of Technology, Haifa (Israel)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States); Univ. of Oregon, Eugene, OR (United States)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; characterization and analytical techniques; high-harmonic generation; ultrafast photonics; X-rays
OSTI Identifier:
1374369
Alternate Identifier(s):
OSTI ID: 1408433

Zurch, Michael, Chang, Hung -Tzu, Borja, Lauren J., Kraus, Peter M., Cushing, Scott K., Gandman, Andrey, Kaplan, Christopher J., Oh, Myoung Hwan, Prell, James S., Prendergast, David, Pemmaraju, Chaitanya D., Neumark, Daniel M., and Leone, Stephen R.. Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium. United States: N. p., Web. doi:10.1038/ncomms15734.
Zurch, Michael, Chang, Hung -Tzu, Borja, Lauren J., Kraus, Peter M., Cushing, Scott K., Gandman, Andrey, Kaplan, Christopher J., Oh, Myoung Hwan, Prell, James S., Prendergast, David, Pemmaraju, Chaitanya D., Neumark, Daniel M., & Leone, Stephen R.. Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium. United States. doi:10.1038/ncomms15734.
Zurch, Michael, Chang, Hung -Tzu, Borja, Lauren J., Kraus, Peter M., Cushing, Scott K., Gandman, Andrey, Kaplan, Christopher J., Oh, Myoung Hwan, Prell, James S., Prendergast, David, Pemmaraju, Chaitanya D., Neumark, Daniel M., and Leone, Stephen R.. 2017. "Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium". United States. doi:10.1038/ncomms15734. https://www.osti.gov/servlets/purl/1374369.
@article{osti_1374369,
title = {Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium},
author = {Zurch, Michael and Chang, Hung -Tzu and Borja, Lauren J. and Kraus, Peter M. and Cushing, Scott K. and Gandman, Andrey and Kaplan, Christopher J. and Oh, Myoung Hwan and Prell, James S. and Prendergast, David and Pemmaraju, Chaitanya D. and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm–3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.},
doi = {10.1038/ncomms15734},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {6}
}

Works referenced in this record:

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999