skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Effects of Interlayer Coupling on Hot-Carrier Dynamics in Graphene-Derived van der Waals Heterostructures

Abstract

Graphene exhibits promise as a plasmonic material with high mode confinement that could enable efficient hot carrier extraction. The lifetimes and mean free paths of energetic carriers have been investigated in free-standing graphene, graphite, and a heterostructure consisting of alternating graphene and hexagonal boron nitride layers using ab initio calculations of electron–electron and electron–phonon scattering in these materials. It is found that the extremely high lifetimes (3 ps) of low-energy carriers near the Dirac point in graphene, which are a 100 times larger than that in noble metals, are reduced by an order of magnitude due to interlayer coupling in graphite, but enhanced in the heterostructure due to phonon mode clamping. However, these lifetimes drop precipitously with increasing carrier energy and are smaller than those in noble metals at energies exceeding 0.5 eV. By analyzing the contribution of different scattering mechanisms and interlayer interactions, desirable spacer layer characteristics—high dielectric constant and heavy atoms—that could pave the way for plasmonic heterostructures with improved hot carrier transport have been identified.

Authors:
 [1];  [2];  [2];  [2]
  1. Harvard Univ., Cambridge, MA (United States)
  2. Rensselaer Polytechnic Inst., Troy, NY (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1543462
Alternate Identifier(s):
OSTI ID: 1401286
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Optical Materials
Additional Journal Information:
Journal Volume: 5; Journal Issue: 15; Journal ID: ISSN 2195-1071
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Materials Science; Optics

Citation Formats

Narang, Prineha, Zhao, Litao, Claybrook, Steven, and Sundararaman, Ravishankar. Effects of Interlayer Coupling on Hot-Carrier Dynamics in Graphene-Derived van der Waals Heterostructures. United States: N. p., 2017. Web. doi:10.1002/adom.201600914.
Narang, Prineha, Zhao, Litao, Claybrook, Steven, & Sundararaman, Ravishankar. Effects of Interlayer Coupling on Hot-Carrier Dynamics in Graphene-Derived van der Waals Heterostructures. United States. doi:10.1002/adom.201600914.
Narang, Prineha, Zhao, Litao, Claybrook, Steven, and Sundararaman, Ravishankar. Fri . "Effects of Interlayer Coupling on Hot-Carrier Dynamics in Graphene-Derived van der Waals Heterostructures". United States. doi:10.1002/adom.201600914. https://www.osti.gov/servlets/purl/1543462.
@article{osti_1543462,
title = {Effects of Interlayer Coupling on Hot-Carrier Dynamics in Graphene-Derived van der Waals Heterostructures},
author = {Narang, Prineha and Zhao, Litao and Claybrook, Steven and Sundararaman, Ravishankar},
abstractNote = {Graphene exhibits promise as a plasmonic material with high mode confinement that could enable efficient hot carrier extraction. The lifetimes and mean free paths of energetic carriers have been investigated in free-standing graphene, graphite, and a heterostructure consisting of alternating graphene and hexagonal boron nitride layers using ab initio calculations of electron–electron and electron–phonon scattering in these materials. It is found that the extremely high lifetimes (3 ps) of low-energy carriers near the Dirac point in graphene, which are a 100 times larger than that in noble metals, are reduced by an order of magnitude due to interlayer coupling in graphite, but enhanced in the heterostructure due to phonon mode clamping. However, these lifetimes drop precipitously with increasing carrier energy and are smaller than those in noble metals at energies exceeding 0.5 eV. By analyzing the contribution of different scattering mechanisms and interlayer interactions, desirable spacer layer characteristics—high dielectric constant and heavy atoms—that could pave the way for plasmonic heterostructures with improved hot carrier transport have been identified.},
doi = {10.1002/adom.201600914},
journal = {Advanced Optical Materials},
number = 15,
volume = 5,
place = {United States},
year = {2017},
month = {3}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

Figures / Tables:

FIG. 1 FIG. 1: (a) Schematic structures of 2D materials and graphene-derived vdW heterostructures in which we investigate hot carrier relaxation dynamics. (b) Feynman diagrams for the intrinsic carrier relaxation mechanisms: electronphonon (e-ph) scattering and and electron-electron (e-e) scattering. (c) Roles of the two mechanisms in energy and momentum relaxation: both processesmore » randomize the momentum component along the original propagation direction, $\vec{p}$ · $\hat{p}$0 in a single scatter, while energy relaxation due to a single scattering event is substantial only in e-e scattering because the overall energy-scale of phonons is much smaller than the typical scale of excited electron energies.« less

Save / Share:

Works referenced in this record:

Plasmon-induced hot carrier science and technology
journal, January 2015

  • Brongersma, Mark L.; Halas, Naomi J.; Nordlander, Peter
  • Nature Nanotechnology, Vol. 10, Issue 1
  • DOI: 10.1038/nnano.2014.311

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Mixed-dimensional van der Waals heterostructures
journal, August 2016

  • Jariwala, Deep; Marks, Tobin J.; Hersam, Mark C.
  • Nature Materials, Vol. 16, Issue 2
  • DOI: 10.1038/nmat4703

Two-dimensional material nanophotonics
journal, November 2014


Carrier Transport in Two-Dimensional Graphene Layers
journal, May 2007


First-Principles Study of Electron Linewidths in Graphene
journal, February 2009


Ultrafast Carrier Dynamics in Graphite
journal, February 2009


Ultrafast graphene photodetector
journal, October 2009

  • Xia, Fengnian; Mueller, Thomas; Lin, Yu-ming
  • Nature Nanotechnology, Vol. 4, Issue 12, p. 839-843
  • DOI: 10.1038/nnano.2009.292

Van der Waals heterostructures
journal, July 2013

  • Geim, A. K.; Grigorieva, I. V.
  • Nature, Vol. 499, Issue 7459, p. 419-425
  • DOI: 10.1038/nature12385

Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004


Anisotropic behaviours of massless Dirac fermions in graphene under periodic potentials
journal, February 2008

  • Park, Cheol-Hwan; Yang, Li; Son, Young-Woo
  • Nature Physics, Vol. 4, Issue 3
  • DOI: 10.1038/nphys890

Photoexcitation cascade and multiple hot-carrier generation in graphene
journal, February 2013

  • Tielrooij, K. J.; Song, J. C. W.; Jensen, S. A.
  • Nature Physics, Vol. 9, Issue 4
  • DOI: 10.1038/nphys2564

Theoretical predictions for hot-carrier generation from surface plasmon decay
journal, December 2014

  • Sundararaman, Ravishankar; Narang, Prineha; Jermyn, Adam S.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6788

First-principles calculation of hot-electron scattering in metals
journal, December 2004


Hot Electron Cooling by Acoustic Phonons in Graphene
journal, August 2012


Plasmonics in graphene at infrared frequencies
journal, December 2009


Disorder-Assisted Electron-Phonon Scattering and Cooling Pathways in Graphene
journal, September 2012


Plasmonic hot carrier dynamics in solid-state and chemical systems for energy conversion
journal, January 2016

  • Narang, Prineha; Sundararaman, Ravishankar; Atwater, Harry A.
  • Nanophotonics, Vol. 5, Issue 1
  • DOI: 10.1515/nanoph-2016-0007

Atomic layers of hybridized boron nitride and graphene domains
journal, February 2010

  • Ci, Lijie; Song, Li; Jin, Chuanhong
  • Nature Materials, Vol. 9, Issue 5, p. 430-435
  • DOI: 10.1038/nmat2711

Observation of Ultrafast Carrier Dynamics and Phonon Relaxation of Graphene from the Deep-Ultraviolet to the Visible Region
journal, March 2014

  • Oum, Kawon; Lenzer, Thomas; Scholz, Mirko
  • The Journal of Physical Chemistry C, Vol. 118, Issue 12
  • DOI: 10.1021/jp4072197

Relaxation of optically excited carriers in graphene
journal, August 2011


Four-Dimensional Electron Microscopy
journal, April 2010


Ultrafast core-loss spectroscopy in four-dimensional electron microscopy
journal, March 2015

  • van der Veen, Renske M.; Penfold, Thomas J.; Zewail, Ahmed H.
  • Structural Dynamics, Vol. 2, Issue 2
  • DOI: 10.1063/1.4916897

The rise of graphene
journal, March 2007

  • Geim, A. K.; Novoselov, K. S.
  • Nature Materials, Vol. 6, Issue 3, p. 183-191
  • DOI: 10.1038/nmat1849

Graphene photonics and optoelectronics
journal, August 2010


The electronic properties of graphene
journal, January 2009

  • Castro Neto, A. H.; Guinea, F.; Peres, N. M. R.
  • Reviews of Modern Physics, Vol. 81, Issue 1, p. 109-162
  • DOI: 10.1103/RevModPhys.81.109

Boron nitride substrates for high-quality graphene electronics
journal, August 2010

  • Dean, C. R.; Young, A. F.; Meric, I.
  • Nature Nanotechnology, Vol. 5, Issue 10, p. 722-726
  • DOI: 10.1038/nnano.2010.172

Theory of electron-plasmon coupling in semiconductors
journal, September 2016


Optimization algorithm for the generation of ONCV pseudopotentials
journal, November 2015


Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry
journal, December 2015

  • Brown, Ana M.; Sundararaman, Ravishankar; Narang, Prineha
  • ACS Nano, Vol. 10, Issue 1
  • DOI: 10.1021/acsnano.5b06199

Femtosecond pump–probe nondestructive examination of materials (invited)
journal, January 2003

  • Norris, Pamela M.; Caffrey, Andrew P.; Stevens, Robert J.
  • Review of Scientific Instruments, Vol. 74, Issue 1
  • DOI: 10.1063/1.1517187

Substrate-induced band gap in graphene on hexagonal boron nitride: Ab initio density functional calculations
journal, August 2007


Supercollision cooling in undoped graphene
journal, December 2012

  • Betz, A. C.; Jhang, S. H.; Pallecchi, E.
  • Nature Physics, Vol. 9, Issue 2
  • DOI: 10.1038/nphys2494

Quantum Transport of Massless Dirac Fermions
journal, February 2007


Maximally localized Wannier functions for entangled energy bands
journal, December 2001


Carrier Relaxation in Epitaxial Graphene Photoexcited Near the Dirac Point
journal, November 2011


Ab initio phonon coupling and optical response of hot electrons in plasmonic metals
journal, August 2016


Femtosecond carrier dynamics in bulk graphite and graphene paper
journal, February 2011


Hot electron relaxation and phonon dynamics in graphene
journal, November 2007

  • Butscher, S.; Milde, F.; Hirtschulz, M.
  • Applied Physics Letters, Vol. 91, Issue 20
  • DOI: 10.1063/1.2809413

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.