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Title: Carrier-Specific Femtosecond XUV Transient Absorption of PbI 2 Reveals Ultrafast Nonradiative Recombination

Femtosecond carrier recombination in PbI 2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative recombination converts the initial electronic excitation to thermal excitation within picoseconds. Ultrafast electron diffraction (UED) is used to measure the lattice temperature and confirm the recombination mechanism. Lastly, the XUV and UED results support a 2nd-order recombination model with a rate constant of 2.5x10 -9 cm 3/s.
Authors:
 [1] ;  [2] ;  [3] ;  [2] ;  [2] ;  [2] ;  [4] ;  [5] ;  [5] ;  [6] ;  [7] ;  [5] ; ORCiD logo [8] ; ORCiD logo [2]
  1. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Chemistry; SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  2. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Chemistry
  3. Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Materials Science and Engineering
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  8. Univ. of Illinois, Urbana-Champaign, IL (United States). Frederick Seitz Materials Research Lab., National Center for Supercomputing Applications, and Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
FA9550-14-1-0314; CBET-1437230; AC02-76SF00515; SC00014607
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 50; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; High-Harmonic Generation; Carrier Dynamics; Extreme Ultraviolet; Semiconductor; Electron Diffraction
OSTI Identifier:
1425349

Lin, Ming-Fu, Verkamp, Max A., Leveillee, Joshua, Ryland, Elizabeth S., Benke, Kristin, Zhang, Kaili, Weninger, Clemens, Shen, Xiaozhe, Li, Renkai, Fritz, David, Bergmann, Uwe, Wang, Xijie, Schleife, André, and Vura-Weis, Josh. Carrier-Specific Femtosecond XUV Transient Absorption of PbI2 Reveals Ultrafast Nonradiative Recombination. United States: N. p., Web. doi:10.1021/acs.jpcc.7b11147.
Lin, Ming-Fu, Verkamp, Max A., Leveillee, Joshua, Ryland, Elizabeth S., Benke, Kristin, Zhang, Kaili, Weninger, Clemens, Shen, Xiaozhe, Li, Renkai, Fritz, David, Bergmann, Uwe, Wang, Xijie, Schleife, André, & Vura-Weis, Josh. Carrier-Specific Femtosecond XUV Transient Absorption of PbI2 Reveals Ultrafast Nonradiative Recombination. United States. doi:10.1021/acs.jpcc.7b11147.
Lin, Ming-Fu, Verkamp, Max A., Leveillee, Joshua, Ryland, Elizabeth S., Benke, Kristin, Zhang, Kaili, Weninger, Clemens, Shen, Xiaozhe, Li, Renkai, Fritz, David, Bergmann, Uwe, Wang, Xijie, Schleife, André, and Vura-Weis, Josh. 2017. "Carrier-Specific Femtosecond XUV Transient Absorption of PbI2 Reveals Ultrafast Nonradiative Recombination". United States. doi:10.1021/acs.jpcc.7b11147.
@article{osti_1425349,
title = {Carrier-Specific Femtosecond XUV Transient Absorption of PbI2 Reveals Ultrafast Nonradiative Recombination},
author = {Lin, Ming-Fu and Verkamp, Max A. and Leveillee, Joshua and Ryland, Elizabeth S. and Benke, Kristin and Zhang, Kaili and Weninger, Clemens and Shen, Xiaozhe and Li, Renkai and Fritz, David and Bergmann, Uwe and Wang, Xijie and Schleife, André and Vura-Weis, Josh},
abstractNote = {Femtosecond carrier recombination in PbI2 is measured using tabletop high-harmonic extreme ultraviolet (XUV) transient absorption spectroscopy and ultrafast electron diffraction. XUV absorption from 45 eV to 62 eV measures transitions from the iodine 4d core level to the conduction band density of states. Photoexcitation at 400 nm creates separate and distinct transient absorption signals for holes and electrons, separated in energy by the 2.4 eV band gap of the semiconductor. The shape of the conduction band and therefore the XUV absorption spectrum is temperature dependent, and nonradiative recombination converts the initial electronic excitation to thermal excitation within picoseconds. Ultrafast electron diffraction (UED) is used to measure the lattice temperature and confirm the recombination mechanism. Lastly, the XUV and UED results support a 2nd-order recombination model with a rate constant of 2.5x10-9 cm3/s.},
doi = {10.1021/acs.jpcc.7b11147},
journal = {Journal of Physical Chemistry. C},
number = 50,
volume = 121,
place = {United States},
year = {2017},
month = {11}
}