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

Title: Anisotropic thermal transport in bulk hexagonal boron nitride

Abstract

Hexagonal boron nitride (h-BN) has received great interest in recent years as a wide band-gap analog of graphene-derived systems along with its potential in a wide range of applications, for example, as the dielectric layer for graphene devices. However, the thermal transport properties of h-BN, which can be critical for device reliability and functionality, are little studied both experimentally and theoretically. The primary challenge in the experimental measurements of the anisotropic thermal conductivity of h-BN is that typically the sample size of h-BN single crystals is too small for conventional measurement techniques, as state-of-the-art technologies synthesize h-BN single crystals with lateral sizes only up to 2.5 mm and thicknesses up to 200 μm. Recently developed time-domain thermoreflectance (TDTR) techniques are suitable to measure the anisotropic thermal conductivity of such small samples, as it only requires a small area of 50 × 50 μm 2 for the measurements. Accurate atomistic modeling of thermal transport in bulk h-BN is also challenging due to the highly anisotropic layered structure. Here we conduct an integrated experimental and theoretical study on the anisotropic thermal conductivity of bulk h-BN single crystals over the temperature range of 100–500 K using TDTR measurements with multiple modulation frequencies andmore » a full-scale numerical calculation of the phonon Boltzmann transport equation starting from first principles. Our experimental and numerical results compare favorably for both the in-plane and the through-plane thermal conductivities. We observe unusual temperature dependence and phonon-isotope scattering in the through-plane thermal conductivity of h-BN and elucidate their origins. Here, this article not only provides an important benchmark of the anisotropic thermal conductivity of h-BN, but also develops fundamental insight into the nature of phonon transport in this highly anisotropic layered material.« less

Authors:
 [1];  [1];  [1];  [2]
  1. Univ. of Colorado, Boulder, CO (United States). Dept. of Mechanical Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1458358
Alternate Identifier(s):
OSTI ID: 1457208
Grant/Contract Number:  
AC05-00OR22725; 1511195; AR0000743
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 2; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Jiang, Puqing, Qian, Xin, Yang, Ronggui, and Lindsay, Lucas. Anisotropic thermal transport in bulk hexagonal boron nitride. United States: N. p., 2018. Web. doi:10.1103/PhysRevMaterials.2.064005.
Jiang, Puqing, Qian, Xin, Yang, Ronggui, & Lindsay, Lucas. Anisotropic thermal transport in bulk hexagonal boron nitride. United States. doi:10.1103/PhysRevMaterials.2.064005.
Jiang, Puqing, Qian, Xin, Yang, Ronggui, and Lindsay, Lucas. Tue . "Anisotropic thermal transport in bulk hexagonal boron nitride". United States. doi:10.1103/PhysRevMaterials.2.064005. https://www.osti.gov/servlets/purl/1458358.
@article{osti_1458358,
title = {Anisotropic thermal transport in bulk hexagonal boron nitride},
author = {Jiang, Puqing and Qian, Xin and Yang, Ronggui and Lindsay, Lucas},
abstractNote = {Hexagonal boron nitride (h-BN) has received great interest in recent years as a wide band-gap analog of graphene-derived systems along with its potential in a wide range of applications, for example, as the dielectric layer for graphene devices. However, the thermal transport properties of h-BN, which can be critical for device reliability and functionality, are little studied both experimentally and theoretically. The primary challenge in the experimental measurements of the anisotropic thermal conductivity of h-BN is that typically the sample size of h-BN single crystals is too small for conventional measurement techniques, as state-of-the-art technologies synthesize h-BN single crystals with lateral sizes only up to 2.5 mm and thicknesses up to 200 μm. Recently developed time-domain thermoreflectance (TDTR) techniques are suitable to measure the anisotropic thermal conductivity of such small samples, as it only requires a small area of 50 × 50 μm2 for the measurements. Accurate atomistic modeling of thermal transport in bulk h-BN is also challenging due to the highly anisotropic layered structure. Here we conduct an integrated experimental and theoretical study on the anisotropic thermal conductivity of bulk h-BN single crystals over the temperature range of 100–500 K using TDTR measurements with multiple modulation frequencies and a full-scale numerical calculation of the phonon Boltzmann transport equation starting from first principles. Our experimental and numerical results compare favorably for both the in-plane and the through-plane thermal conductivities. We observe unusual temperature dependence and phonon-isotope scattering in the through-plane thermal conductivity of h-BN and elucidate their origins. Here, this article not only provides an important benchmark of the anisotropic thermal conductivity of h-BN, but also develops fundamental insight into the nature of phonon transport in this highly anisotropic layered material.},
doi = {10.1103/PhysRevMaterials.2.064005},
journal = {Physical Review Materials},
number = 6,
volume = 2,
place = {United States},
year = {2018},
month = {6}
}

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

Citation Metrics:
Cited by: 6 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Large-Scale Growth of High-Quality Hexagonal Boron Nitride Crystals at Atmospheric Pressure from an Fe–Cr Flux
journal, August 2017


Electron Tunneling through Ultrathin Boron Nitride Crystalline Barriers
journal, February 2012

  • Britnell, Liam; Gorbachev, Roman V.; Jalil, Rashid
  • Nano Letters, Vol. 12, Issue 3
  • DOI: 10.1021/nl3002205

Calculation of the lattice constant of solids with semilocal functionals
journal, February 2009


Intrinsic lattice thermal conductivity of semiconductors from first principles
journal, December 2007

  • Broido, D. A.; Malorny, M.; Birner, G.
  • Applied Physics Letters, Vol. 91, Issue 23
  • DOI: 10.1063/1.2822891

Ab initio thermal transport in compound semiconductors
journal, April 2013


Normal Modes in Hexagonal Boron Nitride
journal, June 1966


Two-channel model for nonequilibrium thermal transport in pump-probe experiments
journal, October 2013


Strongly anisotropic in-plane thermal transport in single-layer black phosphorene
journal, February 2015

  • Jain, Ankit; McGaughey, Alan J. H.
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep08501

Graphene-hexagonal boron nitride resonant tunneling diodes as high-frequency oscillators
journal, September 2015

  • Gaskell, J.; Eaves, L.; Novoselov, K. S.
  • Applied Physics Letters, Vol. 107, Issue 10
  • DOI: 10.1063/1.4930230

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

Mechanics and Mechanically Tunable Band Gap in Single-Layer Hexagonal Boron-Nitride
journal, July 2013


Role of Low-Energy Phonons in Thermal Conduction
journal, August 1954


Thermal conductivity of bulk and monolayer MoS 2
journal, February 2016


Analysis of heat flow in layered structures for time-domain thermoreflectance
journal, December 2004

  • Cahill, David G.
  • Review of Scientific Instruments, Vol. 75, Issue 12
  • DOI: 10.1063/1.1819431

Pulse accumulation, radial heat conduction, and anisotropic thermal conductivity in pump-probe transient thermoreflectance
journal, November 2008

  • Schmidt, Aaron J.; Chen, Xiaoyuan; Chen, Gang
  • Review of Scientific Instruments, Vol. 79, Issue 11
  • DOI: 10.1063/1.3006335

Uncertainty analysis of thermoreflectance measurements
journal, January 2016

  • Yang, Jia; Ziade, Elbara; Schmidt, Aaron J.
  • Review of Scientific Instruments, Vol. 87, Issue 1
  • DOI: 10.1063/1.4939671

Enhanced thermal conductivity and isotope effect in single-layer hexagonal boron nitride
journal, October 2011


Temperature Dependence of Anisotropic Thermal-Conductivity Tensor of Bulk Black Phosphorus
journal, November 2016


Graphene Field-Effect Transistors Based on Boron–Nitride Dielectrics
journal, July 2013


Thermal Conductivity of Graphene and Graphite: Collective Excitations and Mean Free Paths
journal, October 2014

  • Fugallo, Giorgia; Cepellotti, Andrea; Paulatto, Lorenzo
  • Nano Letters, Vol. 14, Issue 11
  • DOI: 10.1021/nl502059f

Negative Coulomb Drag in Double Bilayer Graphene
journal, July 2016


Ab initio calculation of phonon dispersions in II-VI semiconductors
journal, February 1993


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

Light scattering study of boron nitride microcrystals
journal, June 1981

  • Nemanich, R. J.; Solin, S. A.; Martin, Richard M.
  • Physical Review B, Vol. 23, Issue 12, p. 6348-6356
  • DOI: 10.1103/PhysRevB.23.6348

Time-domain thermoreflectance (TDTR) measurements of anisotropic thermal conductivity using a variable spot size approach
journal, July 2017

  • Jiang, Puqing; Qian, Xin; Yang, Ronggui
  • Review of Scientific Instruments, Vol. 88, Issue 7
  • DOI: 10.1063/1.4991715

Far-ultraviolet plane-emission handheld device based on hexagonal boron nitride
journal, September 2009

  • Watanabe, Kenji; Taniguchi, Takashi; Niiyama, Takahiro
  • Nature Photonics, Vol. 3, Issue 10
  • DOI: 10.1038/nphoton.2009.167

Ultrafast relaxation of hot phonons in graphene-hBN heterostructures
journal, May 2017

  • Golla, Dheeraj; Brasington, Alexandra; LeRoy, Brian J.
  • APL Materials, Vol. 5, Issue 5
  • DOI: 10.1063/1.4982738

Thermal conductivity and phonon linewidths of monolayer MoS 2 from first principles
journal, December 2013

  • Li, Wu; Carrete, J.; Mingo, Natalio
  • Applied Physics Letters, Vol. 103, Issue 25
  • DOI: 10.1063/1.4850995

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965


Coulomb drag in graphene–boron nitride heterostructures: Effect of virtual phonon exchange
journal, September 2012


Light-emitting diodes by band-structure engineering in van der Waals heterostructures
journal, February 2015

  • Withers, F.; Del Pozo-Zamudio, O.; Mishchenko, A.
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4205

High performance vertical tunneling diodes using graphene/hexagonal boron nitride/graphene hetero-structure
journal, February 2014

  • Hwan Lee, Seung; Sup Choi, Min; Lee, Jia
  • Applied Physics Letters, Vol. 104, Issue 5
  • DOI: 10.1063/1.4863840

Heat capacity and thermal conductivity of hexagonal pyrolytic boron nitride
journal, May 1976


The thermal conductivity of highly oriented pyrolytic boron nitride
journal, September 1971


Flexible and Transparent MoS 2 Field-Effect Transistors on Hexagonal Boron Nitride-Graphene Heterostructures
journal, August 2013

  • Lee, Gwan-Hyoung; Yu, Young-Jun; Cui, Xu
  • ACS Nano, Vol. 7, Issue 9
  • DOI: 10.1021/nn402954e

Thermal Conductivity and Phonon Transport in Suspended Few-Layer Hexagonal Boron Nitride
journal, January 2013

  • Jo, Insun; Pettes, Michael Thompson; Kim, Jaehyun
  • Nano Letters, Vol. 13, Issue 2, p. 550-554
  • DOI: 10.1021/nl304060g

Lattice parameters and anisotropic thermal expansion of hexagonal boron nitride in the 10?297.5�K temperature range
journal, September 2002

  • Paszkowicz, W.; Pelka, J. B.; Knapp, M.
  • Applied Physics A: Materials Science & Processing, Vol. 75, Issue 3
  • DOI: 10.1007/s003390100999

Phonons and related crystal properties from density-functional perturbation theory
journal, July 2001

  • Baroni, Stefano; de Gironcoli, Stefano; Dal Corso, Andrea
  • Reviews of Modern Physics, Vol. 73, Issue 2
  • DOI: 10.1103/RevModPhys.73.515

Theory of resonant tunneling in bilayer-graphene/hexagonal-boron-nitride heterostructures
journal, March 2015

  • de la Barrera, Sergio C.; Feenstra, Randall M.
  • Applied Physics Letters, Vol. 106, Issue 9
  • DOI: 10.1063/1.4914324

Thermal conductivity of half-Heusler compounds from first-principles calculations
journal, September 2011


Deep Ultraviolet Light-Emitting Hexagonal Boron Nitride Synthesized at Atmospheric Pressure
journal, August 2007


Measurement Techniques for Thermal Conductivity and Interfacial Thermal Conductance of Bulk and Thin Film Materials
journal, October 2016

  • Zhao, Dongliang; Qian, Xin; Gu, Xiaokun
  • Journal of Electronic Packaging, Vol. 138, Issue 4
  • DOI: 10.1115/1.4034605

Layer thickness-dependent phonon properties and thermal conductivity of MoS 2
journal, February 2016

  • Gu, Xiaokun; Li, Baowen; Yang, Ronggui
  • Journal of Applied Physics, Vol. 119, Issue 8
  • DOI: 10.1063/1.4942827

Inhomogeneous Electron Gas
journal, November 1964


Thermal Conductivity of Monolayer MoSe 2 and MoS 2
journal, November 2016

  • Hong, Yang; Zhang, Jingchao; Zeng, Xiao Cheng
  • The Journal of Physical Chemistry C, Vol. 120, Issue 45
  • DOI: 10.1021/acs.jpcc.6b07262

Vibrational Properties of Hexagonal Boron Nitride: Inelastic X-Ray Scattering and Ab Initio Calculations
journal, March 2007


Enhanced Photon Tunneling by Surface Plasmon–Phonon Polaritons in Graphene/hBN Heterostructures
journal, October 2016

  • Zhao, B.; Zhang, Z. M.
  • Journal of Heat Transfer, Vol. 139, Issue 2
  • DOI: 10.1115/1.4034793

Boron nitride as a lubricant additive
journal, October 1999


Field-Effect Tunneling Transistor Based on Vertical Graphene Heterostructures
journal, February 2012


Towards Thermoconductive, Electrically Insulating Polymeric Composites with Boron Nitride Nanotubes as Fillers
journal, June 2009

  • Zhi, Chunyi; Bando, Yoshio; Terao, Takeshi
  • Advanced Functional Materials, Vol. 19, Issue 12, p. 1857-1862
  • DOI: 10.1002/adfm.200801435

First Principles Peierls-Boltzmann Phonon Thermal Transport: A Topical Review
journal, April 2016


Phonon thermal transport in strained and unstrained graphene from first principles
journal, April 2014


Graphene/h-BN/GaAs sandwich diode as solar cell and photodetector
journal, January 2016

  • Li, Xiaoqiang; Lin, Shisheng; Lin, Xing
  • Optics Express, Vol. 24, Issue 1
  • DOI: 10.1364/OE.24.000134

Frequency dependence of the thermal conductivity of semiconductor alloys
journal, August 2007


Phonon hydrodynamics in two-dimensional materials
journal, March 2015

  • Cepellotti, Andrea; Fugallo, Giorgia; Paulatto, Lorenzo
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7400

Bilayer Graphene-Hexagonal Boron Nitride Heterostructure Negative Differential Resistance Interlayer Tunnel FET
journal, April 2015

  • Kang, Sangwoo; Fallahazad, Babak; Lee, Kayoung
  • IEEE Electron Device Letters, Vol. 36, Issue 4
  • DOI: 10.1109/LED.2015.2398737