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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). 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. https://doi.org/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. https://doi.org/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 = {Fri Mar 24 00:00:00 EDT 2017},
month = {Fri Mar 24 00:00:00 EDT 2017}
}

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Cited by: 33 works
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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

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