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Title: Phonon engineering of boron nitride via isotopic enrichment

Abstract

Phonon polaritons (PhPs) enable a variety of applications, yet it requires PhPs supported in the desired frequency range. The two BN allotropes (cubic and hexagonal, cBN and hBN) are of particular interest, as their optic phonons fall within the so-called molecular-fingerprint region (~ 1000–1610 cm-1). However, there remains a spectral gap between PhPs covered by these two, limiting applications. Thus, we isotopically engineered hBN and cBN and examined the optic phonons. Furthermore, for hBN, enhancement of the optic phonon lifetimes and shifted frequencies are observed. However, lifetimes are observed to decrease with the enrichment of cBN by 10B, 11B, and 15N. We propose that the reduced lifetimes are not due to intrinsic loss, but rather increased defect concentrations resulting from the modified growth, supported by first-principles calculations. Thus, reducing the extrinsic defects in isotopically engineered cBN may present a path toward overcoming these restrictions for applications in the molecular-fingerprint region.

Authors:
 [1]; ORCiD logo [2];  [3];  [4];  [1];  [5];  [6];  [6];  [6];  [7]; ORCiD logo [1]
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States). Center for Integrated Nanotechnologies (CINT)
  4. Vanderbilt Univ., Nashville, TN (United States); Univ. of Iowa, Iowa City, IA (United States)
  5. National Institute for Materials Science (NIMS), Tsukuba (Japan). Research Center for Functional Materials
  6. Fisk Univ., Nashville, TN (United States). Center for Photonic Materials and Devices
  7. National Institute for Materials Science (NIMS), Tsukuba (Japan). International Center for Materials Nanoarchitectonics
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); MEXT
OSTI Identifier:
1833973
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231; NA0003525; 1904793; JPMXP0112101001; JP20H00354
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Research
Additional Journal Information:
Journal Volume: 36; Journal Issue: 21; Journal ID: ISSN 0884-2914
Publisher:
Materials Research Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

He, Mingze, Lindsay, Lucas, Beechem, Thomas E., Folland, Thomas, Matson, Joseph, Watanabe, Kenji, Zavalin, Andrey, Ueda, Akira, Collins, Warren. E., Taniguchi, Takashi, and Caldwell, Joshua D. Phonon engineering of boron nitride via isotopic enrichment. United States: N. p., 2021. Web. doi:10.1557/s43578-021-00426-9.
He, Mingze, Lindsay, Lucas, Beechem, Thomas E., Folland, Thomas, Matson, Joseph, Watanabe, Kenji, Zavalin, Andrey, Ueda, Akira, Collins, Warren. E., Taniguchi, Takashi, & Caldwell, Joshua D. Phonon engineering of boron nitride via isotopic enrichment. United States. https://doi.org/10.1557/s43578-021-00426-9
He, Mingze, Lindsay, Lucas, Beechem, Thomas E., Folland, Thomas, Matson, Joseph, Watanabe, Kenji, Zavalin, Andrey, Ueda, Akira, Collins, Warren. E., Taniguchi, Takashi, and Caldwell, Joshua D. Tue . "Phonon engineering of boron nitride via isotopic enrichment". United States. https://doi.org/10.1557/s43578-021-00426-9. https://www.osti.gov/servlets/purl/1833973.
@article{osti_1833973,
title = {Phonon engineering of boron nitride via isotopic enrichment},
author = {He, Mingze and Lindsay, Lucas and Beechem, Thomas E. and Folland, Thomas and Matson, Joseph and Watanabe, Kenji and Zavalin, Andrey and Ueda, Akira and Collins, Warren. E. and Taniguchi, Takashi and Caldwell, Joshua D.},
abstractNote = {Phonon polaritons (PhPs) enable a variety of applications, yet it requires PhPs supported in the desired frequency range. The two BN allotropes (cubic and hexagonal, cBN and hBN) are of particular interest, as their optic phonons fall within the so-called molecular-fingerprint region (~ 1000–1610 cm-1). However, there remains a spectral gap between PhPs covered by these two, limiting applications. Thus, we isotopically engineered hBN and cBN and examined the optic phonons. Furthermore, for hBN, enhancement of the optic phonon lifetimes and shifted frequencies are observed. However, lifetimes are observed to decrease with the enrichment of cBN by 10B, 11B, and 15N. We propose that the reduced lifetimes are not due to intrinsic loss, but rather increased defect concentrations resulting from the modified growth, supported by first-principles calculations. Thus, reducing the extrinsic defects in isotopically engineered cBN may present a path toward overcoming these restrictions for applications in the molecular-fingerprint region.},
doi = {10.1557/s43578-021-00426-9},
journal = {Journal of Materials Research},
number = 21,
volume = 36,
place = {United States},
year = {Tue Nov 09 00:00:00 EST 2021},
month = {Tue Nov 09 00:00:00 EST 2021}
}

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