Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Super-diffusion of excited carriers in semiconductors

Abstract

The ultrafast spatial and temporal dynamics of excited carriers are important to understanding the response of materials to laser pulses. Here we use scanning ultrafast electron microscopy to image the dynamics of electrons and holes in silicon after excitation with a short laser pulse. We find that the carriers exhibit a diffusive dynamics at times shorter than 200 ps, with a transient diffusivity up to 1,000 times higher than the room temperature value, D0≈30 cm2s–1. The diffusivity then decreases rapidly, reaching a value of D0 roughly 500 ps after the excitation pulse. We attribute the transient super-diffusive behaviour to the rapid expansion of the excited carrier gas, which equilibrates with the environment in 100–150 ps. Numerical solution of the diffusion equation, as well as ab initio calculations, support our interpretation. Lastly, our findings provide new insight into the ultrafast spatial dynamics of excited carriers in materials.

Authors:
 [1];  [2];  [1];  [3]
+ Show Author Affiliations
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Physical Biology Center for Ultrafast Science and Technology, Arthur Noyes Lab. of Chemical Physics
  2. California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Applied Physics and Materials Science and Dept. of Physics
  3. California Inst. of Technology (CalTech), Pasadena, CA (United States). Dept. of Applied Physics and Materials Science
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1489371
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Najafi, Ebrahim, Ivanov, Vsevolod, Zewail, Ahmed, and Bernardi, Marco. Super-diffusion of excited carriers in semiconductors. United States: N. p., 2017. Web. doi:10.1038/ncomms15177.
Copy to clipboard
Najafi, Ebrahim, Ivanov, Vsevolod, Zewail, Ahmed, & Bernardi, Marco. Super-diffusion of excited carriers in semiconductors. United States. https://doi.org/10.1038/ncomms15177
Copy to clipboard
Najafi, Ebrahim, Ivanov, Vsevolod, Zewail, Ahmed, and Bernardi, Marco. Thu . "Super-diffusion of excited carriers in semiconductors". United States. https://doi.org/10.1038/ncomms15177. https://www.osti.gov/servlets/purl/1489371.
Copy to clipboard
@article{osti_1489371,
title = {Super-diffusion of excited carriers in semiconductors},
author = {Najafi, Ebrahim and Ivanov, Vsevolod and Zewail, Ahmed and Bernardi, Marco},
abstractNote = {The ultrafast spatial and temporal dynamics of excited carriers are important to understanding the response of materials to laser pulses. Here we use scanning ultrafast electron microscopy to image the dynamics of electrons and holes in silicon after excitation with a short laser pulse. We find that the carriers exhibit a diffusive dynamics at times shorter than 200 ps, with a transient diffusivity up to 1,000 times higher than the room temperature value, D0≈30 cm2s–1. The diffusivity then decreases rapidly, reaching a value of D0 roughly 500 ps after the excitation pulse. We attribute the transient super-diffusive behaviour to the rapid expansion of the excited carrier gas, which equilibrates with the environment in 100–150 ps. Numerical solution of the diffusion equation, as well as ab initio calculations, support our interpretation. Lastly, our findings provide new insight into the ultrafast spatial dynamics of excited carriers in materials.},
doi = {10.1038/ncomms15177},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {Thu May 11 00:00:00 EDT 2017},
month = {Thu May 11 00:00:00 EDT 2017}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/ncomms15177
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 48 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Schematic of scanning ultrafast electron microscopy (SUEM) imaging. In our SUEM measurements, the optical pump pulse excites electron-hole pairs in silicon, which undergo super-diffusion until they equilibrate with the environment. Electron probe pulses with a known delay raster-scan the surface, resulting in the emission of secondary electrons (SEs)more » employed to image the carrier dynamics. The right panel schematically shows carrier dynamical processes mapped onto the bandstructure of Si. Shown are the carrier optical excitation (green arrow), as well as energy gain and recombination (upward and downward oriented red arrows, respectively) due to carrier scattering processes. The SEs preferentially observed by SUEM (blue dot) are emitted from the high-energy tail of the carrier distribution.« less
All figures and tables (4 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Pump–Probe Microscopy: Spatially Resolved Carrier Dynamics in ZnO Rods and the Influence of Optical Cavity Resonator Modes
journal, November 2012

  • Mehl, Brian P.; Kirschbrown, Justin R.; Gabriel, Michelle M.
  • The Journal of Physical Chemistry B, Vol. 117, Issue 16
  • DOI: 10.1021/jp307089h

4D Electron Microscopy: Principles and Applications
journal, August 2012

  • Flannigan, David J.; Zewail, Ahmed H.
  • Accounts of Chemical Research, Vol. 45, Issue 10
  • DOI: 10.1021/ar3001684

Fast ions and hot electrons in the laser–plasma interaction
journal, January 1986

  • Gitomer, S. J.; Jones, R. D.; Begay, F.
  • Physics of Fluids, Vol. 29, Issue 8
  • DOI: 10.1063/1.865510

4D Electron Microscopy: Principles and Applications
journal, August 2012

  • Flannigan, David J.; Zewail, Ahmed H.
  • Accounts of Chemical Research, Vol. 45, Issue 10
  • DOI: 10.1021/ar3001684

Pump–Probe Microscopy: Spatially Resolved Carrier Dynamics in ZnO Rods and the Influence of Optical Cavity Resonator Modes
journal, November 2012

  • Mehl, Brian P.; Kirschbrown, Justin R.; Gabriel, Michelle M.
  • The Journal of Physical Chemistry B, Vol. 117, Issue 16
  • DOI: 10.1021/jp307089h

4D Scanning Ultrafast Electron Microscopy: Visualization of Materials Surface Dynamics
journal, May 2011

  • Mohammed, Omar F.; Yang, Ding-Shyue; Pal, Samir Kumar
  • Journal of the American Chemical Society, Vol. 133, Issue 20
  • DOI: 10.1021/ja2031322

Exciton Radiative Lifetimes in Two-Dimensional Transition Metal Dichalcogenides
journal, March 2015

  • Palummo, Maurizia; Bernardi, Marco; Grossman, Jeffrey C.
  • Nano Letters, Vol. 15, Issue 5
  • DOI: 10.1021/nl503799t

Surface photovoltage phenomena: theory, experiment, and applications
journal, December 1999

Quantum coherence controls the charge separation in a prototypical artificial light-harvesting system
journal, March 2013

  • Andrea Rozzi, Carlo; Maria Falke, Sarah; Spallanzani, Nicola
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2603

Two-photon spectroscopy of silicon using femtosecond pulses at above-gap frequencies
journal, January 1990

  • Reitze, D. H.; Zhang, T. R.; Wood, Wm. M.
  • Journal of the Optical Society of America B, Vol. 7, Issue 1
  • DOI: 10.1364/JOSAB.7.000084

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

A new examination of secondary electron yield data
journal, January 2005

  • Lin, Yinghong; Joy, David C.
  • Surface and Interface Analysis, Vol. 37, Issue 11
  • DOI: 10.1002/sia.2107

Characterization of the spatiotemporal evolution of laser-generated plasmas
journal, January 2008

  • Kanter, E. P.; Santra, R.; Höhr, C.
  • Journal of Applied Physics, Vol. 104, Issue 7
  • DOI: 10.1063/1.2991339

Ab initio study of hot electrons in GaAs
journal, April 2015

  • Bernardi, Marco; Vigil-Fowler, Derek; Ong, Chin Shen
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 17
  • DOI: 10.1073/pnas.1419446112

Ab Initio Study of Hot Carriers in the First Picosecond after Sunlight Absorption in Silicon
journal, June 2014

4D Scanning Ultrafast Electron Microscopy: Visualization of Materials Surface Dynamics
journal, May 2011

  • Mohammed, Omar F.; Yang, Ding-Shyue; Pal, Samir Kumar
  • Journal of the American Chemical Society, Vol. 133, Issue 20
  • DOI: 10.1021/ja2031322

Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals
journal, June 2015

  • Bernardi, Marco; Mustafa, Jamal; Neaton, Jeffrey B.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8044

Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals
journal, June 2015

  • Bernardi, Marco; Mustafa, Jamal; Neaton, Jeffrey B.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms8044

Four-dimensional imaging of carrier interface dynamics in p-n junctions
journal, January 2015

Real-Space Visualization of Energy Loss and Carrier Diffusion in a Semiconductor Nanowire Array Using 4D Electron Microscopy
journal, April 2016

Ultrafast spin transport as key to femtosecond demagnetization
journal, January 2013

  • Eschenlohr, A.; Battiato, M.; Maldonado, P.
  • Nature Materials, Vol. 12, Issue 4
  • DOI: 10.1038/nmat3546

Diffusion coefficient of electrons in silicon
journal, November 1981

  • Brunetti, R.; Jacoboni, C.; Nava, F.
  • Journal of Applied Physics, Vol. 52, Issue 11
  • DOI: 10.1063/1.328622

Erratum: “Probing ultrafast carrier and phonon dynamics in semiconductors” [J. Appl. Phys. 83, 1789 (1998)]
journal, August 1998

  • Othonos, Andreas
  • Journal of Applied Physics, Vol. 84, Issue 3
  • DOI: 10.1063/1.368243

Self-consistent optical parameters of intrinsic silicon at 300K including temperature coefficients
journal, November 2008

Mapping Carrier Dynamics on Material Surfaces in Space and Time using Scanning Ultrafast Electron Microscopy
journal, March 2016

  • Sun, Jingya; Adhikari, Aniruddha; Shaheen, Basamat S.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 6
  • DOI: 10.1021/acs.jpclett.5b02908

Quantum coherence controls the charge separation in a prototypical artificial light harvesting system
conference, May 2013

  • Falke, Sarah M.; Rozzi, Carlo A.; Spallanzani, Nicola
  • 2013 Conference on Lasers & Electro-Optics Europe & International Quantum Electronics Conference CLEO EUROPE/IQEC
  • DOI: 10.1109/cleoe-iqec.2013.6801895

Probing ultrafast carrier and phonon dynamics in semiconductors
journal, February 1998

  • Othonos, Andreas
  • Journal of Applied Physics, Vol. 83, Issue 4
  • DOI: 10.1063/1.367411

Coherent ultrafast magnetism induced by femtosecond laser pulses
journal, May 2009

  • Bigot, Jean-Yves; Vomir, Mircea; Beaurepaire, Eric
  • Nature Physics, Vol. 5, Issue 7
  • DOI: 10.1038/nphys1285

Kinetics of Materials
book, September 2005

Ab initio study of hot electrons in GaAs
journal, April 2015

  • Bernardi, Marco; Vigil-Fowler, Derek; Ong, Chin Shen
  • Proceedings of the National Academy of Sciences, Vol. 112, Issue 17
  • DOI: 10.1073/pnas.1419446112

QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials
journal, September 2009

  • Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola
  • Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502
  • DOI: 10.1088/0953-8984/21/39/395502

Efficient pseudopotentials for plane-wave calculations
journal, January 1991

Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique
journal, December 2016

  • Adhikari, Aniruddha; Eliason, Jeffrey K.; Sun, Jingya
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 1
  • DOI: 10.1021/acsami.6b12301

Ultrafast Spectroscopy of Semiconductors and Semiconductor Nanostructures
book, January 1999

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    Imaging of nonlocal hot-electron energy dissipation via shot noise
    journal, March 2018

    Scanning ultrafast electron microscopy: Four-dimensional imaging of materials dynamics in space and time
    journal, July 2018

    • Yang, Ding-Shyue; Liao, Bolin; Mohammed, Omar F.
    • MRS Bulletin, Vol. 43, Issue 7
    • DOI: 10.1557/mrs.2018.149

    Plasmonics Yields Efficient Electron Transport via Assembly of Shell-Insulated Au Nanoparticles
    journal, October 2018

    Photo-excited hot carrier dynamics in hydrogenated amorphous silicon imaged by 4D electron microscopy
    journal, July 2017

    Ultrafast imaging of surface-exclusive carrier dynamics in silicon
    journal, May 2019

    • Najafi, Ebrahim; Jafari, Amir
    • Journal of Applied Physics, Vol. 125, Issue 18
    • DOI: 10.1063/1.5074198

    Tracking ultrafast hot-electron diffusion in space and time by ultrafast thermomodulation microscopy
    journal, May 2019

    Engineering Ultrafast Carrier Dynamics at the Graphene/GaAs Interface by Bulk Doping Level
    journal, June 2019

    • Yang, Jinghuan; Sun, Quan; Liu, Wei
    • Advanced Optical Materials, Vol. 7, Issue 19
    • DOI: 10.1002/adom.201900580

    Nanoscale thermal diffusion during the laser interference ablation using femto-, pico-, and nanosecond pulses in silicon
    journal, January 2018

    • Gedvilas, Mindaugas; Indrišiūnas, Simonas; Voisiat, Bogdan
    • Physical Chemistry Chemical Physics, Vol. 20, Issue 17
    • DOI: 10.1039/c7cp08458g
      Sort by:
      [ × clear filter / sort ]

      Figures / Tables found in this record:

      Figure 1 (p. 2)figure
      Figure 2 (p. 3)figure
      Figure 3 (p. 4)figure
      Figure 4 (p. 4)figure
        [ × clear filter / sort ]
        Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

        Similar Records in DOE PAGES and OSTI.GOV collections: