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Title: Thermal acoustic excitations with atomic-scale wavelengths in amorphous silicon

Abstract

The vibrational properties of glasses remain a topic of intense interest due to several unresolved puzzles, including the origin of the Boson peak and the mechanisms of thermal transport. Inelastic scattering measurements have revealed that amorphous solids support collective acoustic excitations with low THz frequencies despite the atomic disorder, but these frequencies are well below most of the thermal vibrational spectrum. Here, we report the observation of acoustic excitations with frequencies up to 10 THz in amorphous silicon. The excitations have atomic-scale wavelengths as short as 6 Å and exist well into the thermal vibrational frequencies. Simulations indicate that these high-frequency waves are supported due to the high group velocity and monatomic composition of a-Si, suggesting that other glasses with these characteristics may also exhibit such excitations. Furthermore, our findings demonstrate that a substantial portion of thermal vibrational modes in amorphous materials can still be described as a phonon gas despite the lack of atomic order.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [2];  [3];  [3];  [1]
  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Div. of Engineering and Applied Science
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Material Science and Technology Div.
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1526377
Alternate Identifier(s):
OSTI ID: 1524118; OSTI ID: 1526967
Grant/Contract Number:  
[AC05-00OR22725; AC02-06CH11357]
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
[ Journal Volume: 3; 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

Moon, Jaeyun, Hermann, Raphaël P., Manley, Michael E., Alatas, Ahmet, Said, Ayman H., and Minnich, Austin J. Thermal acoustic excitations with atomic-scale wavelengths in amorphous silicon. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.065601.
Moon, Jaeyun, Hermann, Raphaël P., Manley, Michael E., Alatas, Ahmet, Said, Ayman H., & Minnich, Austin J. Thermal acoustic excitations with atomic-scale wavelengths in amorphous silicon. United States. doi:10.1103/PhysRevMaterials.3.065601.
Moon, Jaeyun, Hermann, Raphaël P., Manley, Michael E., Alatas, Ahmet, Said, Ayman H., and Minnich, Austin J. Mon . "Thermal acoustic excitations with atomic-scale wavelengths in amorphous silicon". United States. doi:10.1103/PhysRevMaterials.3.065601.
@article{osti_1526377,
title = {Thermal acoustic excitations with atomic-scale wavelengths in amorphous silicon},
author = {Moon, Jaeyun and Hermann, Raphaël P. and Manley, Michael E. and Alatas, Ahmet and Said, Ayman H. and Minnich, Austin J.},
abstractNote = {The vibrational properties of glasses remain a topic of intense interest due to several unresolved puzzles, including the origin of the Boson peak and the mechanisms of thermal transport. Inelastic scattering measurements have revealed that amorphous solids support collective acoustic excitations with low THz frequencies despite the atomic disorder, but these frequencies are well below most of the thermal vibrational spectrum. Here, we report the observation of acoustic excitations with frequencies up to 10 THz in amorphous silicon. The excitations have atomic-scale wavelengths as short as 6 Å and exist well into the thermal vibrational frequencies. Simulations indicate that these high-frequency waves are supported due to the high group velocity and monatomic composition of a-Si, suggesting that other glasses with these characteristics may also exhibit such excitations. Furthermore, our findings demonstrate that a substantial portion of thermal vibrational modes in amorphous materials can still be described as a phonon gas despite the lack of atomic order.},
doi = {10.1103/PhysRevMaterials.3.065601},
journal = {Physical Review Materials},
number = [6],
volume = [3],
place = {United States},
year = {2019},
month = {6}
}

Journal Article:
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Works referenced in this record:

Acoustic-like dynamics of amorphous drugs in the THz regime
journal, August 2013

  • Pogna, E. A. A.; Rodríguez-Tinoco, C.; Krisch, M.
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02518

Spectroscopy with meV energy resolution
journal, August 2001


Thermal conductivity accumulation in amorphous silica and amorphous silicon
journal, April 2014


Thermal conductivity of a -Si:H thin films
journal, September 1994


Heat transport in amorphous silicon: Interplay between morphology and disorder
journal, April 2011

  • He, Yuping; Donadio, Davide; Galli, Giulia
  • Applied Physics Letters, Vol. 98, Issue 14
  • DOI: 10.1063/1.3574366

Neutron Brillouin and Umklapp Scattering from Glassy Selenium
journal, September 1998


Vibrational instability, two-level systems, and the boson peak in glasses
journal, August 2007


An instrument with very high energy resolution in X-ray scattering
journal, April 1983


Nondynamic Origin of the High-Frequency Acoustic Attenuation in Glasses
journal, December 1999


Interatomic potential for Si–O systems using Tersoff parameterization
journal, April 2007


Phonon spectroscopy by inelastic x-ray scattering
journal, January 2000


Empirical interatomic potential for silicon with improved elastic properties
journal, November 1988


Universal link between the boson peak and transverse phonons in glass
journal, October 2008

  • Shintani, Hiroshi; Tanaka, Hajime
  • Nature Materials, Vol. 7, Issue 11
  • DOI: 10.1038/nmat2293

New developments in fabrication of high-energy-resolution analyzers for inelastic X-ray spectroscopy
journal, March 2011

  • Said, Ayman H.; Sinn, Harald; Divan, Ralu
  • Journal of Synchrotron Radiation, Vol. 18, Issue 3
  • DOI: 10.1107/S0909049511001828

Evidence of High Frequency Propagating Modes in Vitreous Silica
journal, October 1996


Elastic modulus of supercooled liquid and hot solid silicon measured by inelastic X-ray scattering
journal, December 2005


Role of Disorder in the Thermodynamics and Atomic Dynamics of Glasses
journal, January 2014


Equivalence of the Boson Peak in Glasses to the Transverse Acoustic van Hove Singularity in Crystals
journal, May 2011


Glass-Specific Behavior in the Damping of Acousticlike Vibrations
journal, January 2006


Boson peak and Ioffe-Regel criterion in amorphous siliconlike materials: The effect of bond directionality
journal, February 2016


Coherent Dynamic Structure Factor of Liquid Lithium by Inelastic X-Ray Scattering
journal, March 1997


Computer simulation of local order in condensed phases of silicon
journal, April 1985


High-frequency dynamics of vitreous GeSe 2
journal, September 2010


Numerical study of anharmonic vibrational decay in amorphous and paracrystalline silicon
journal, June 2003


An inelastic X-ray spectrometer with 2.2meV energy resolution
journal, July 2001

  • Sinn, H.; Alp, E. E.; Alatas, A.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 467-468
  • DOI: 10.1016/S0168-9002(01)00755-0

A method for distinguishing between propagons, diffusions, and locons
journal, July 2016

  • Seyf, Hamid Reza; Henry, Asegun
  • Journal of Applied Physics, Vol. 120, Issue 2
  • DOI: 10.1063/1.4955420

High-quality continuous random networks
journal, August 2000


High Frequency Sound Waves in Vitreous Silica
journal, February 1998


High-frequency dynamics of glass-forming polybutadiene
journal, April 1999


Structural properties of amorphous silicon nitride
journal, October 1998


Fitting the Stillinger–Weber potential to amorphous silicon
journal, April 2001


Thermal Conductivity and Specific Heat of Thin-Film Amorphous Silicon
journal, February 2006


The origin of the boson peak and thermal conductivity plateau in low-temperature glasses
journal, February 2003

  • Lubchenko, V.; Wolynes, P. G.
  • Proceedings of the National Academy of Sciences, Vol. 100, Issue 4
  • DOI: 10.1073/pnas.252786999

Soft potential model and universal properties of glasses
journal, January 1993


Zur Theorie der spezifischen Wärmen
journal, January 1912


Improved focusing capability for inelastic X-ray spectrometer at 3-ID of the APS: A combination of toroidal and Kirkpatrick-Baez (KB) mirrors
journal, September 2011

  • Alatas, A.; Leu, B. M.; Zhao, J.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1
  • DOI: 10.1016/j.nima.2010.11.068

Modeling solid-state chemistry: Interatomic potentials for multicomponent systems
journal, March 1989


Structure and physical properties of paracrystalline atomistic models of amorphous silicon
journal, November 2001

  • Voyles, P. M.; Zotov, N.; Nakhmanson, S. M.
  • Journal of Applied Physics, Vol. 90, Issue 9
  • DOI: 10.1063/1.1407319

High Frequency Dynamics in a Monatomic Glass
journal, January 2004


Diffusons, locons and propagons: Character of atomie yibrations in amorphous Si
journal, November 1999

  • Allen, Philip B.; Feldman, Joseph L.; Fabian, Jaroslav
  • Philosophical Magazine B, Vol. 79, Issue 11-12
  • DOI: 10.1080/13642819908223054

Specific heat and thermal conductivity of low-stress amorphous Si–N membranes
journal, January 2004


Thermal conductivity of disordered harmonic solids
journal, November 1993


Propagating elastic vibrations dominate thermal conduction in amorphous silicon
journal, January 2018


High Thermal Conductivity of a Hydrogenated Amorphous Silicon Film
journal, January 2009


Characterization of the elastic properties of amorphous silicon carbide thin films by acoustic microscopy
journal, February 1997


Phonon interpretation of the ‘boson peak’ in supercooled liquids
journal, March 2003

  • Grigera, T. S.; Martín-Mayor, V.; Parisi, G.
  • Nature, Vol. 422, Issue 6929
  • DOI: 10.1038/nature01475

Six-reflection meV-monochromator for synchrotron radiation
journal, May 2011


Microscopic Dynamics of Liquid Aluminum Oxide
journal, March 2003


High-Frequency Dynamics in Metallic Glasses
journal, April 2006


Low-frequency vibrational excitations in vitreous silica: the Ioffe-Regel limit
journal, January 1999


Direct calculation of modal contributions to thermal conductivity via Green–Kubo modal analysis
journal, January 2016


The Local Structure of Amorphous Silicon
journal, February 2012


Breakdown of the Debye approximation for the acoustic modes with nanometric wavelengths in glasses
journal, February 2009

  • Monaco, G.; Giordano, V. M.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 10
  • DOI: 10.1073/pnas.0808965106

Inhomogeneous Elastic Response of Silica Glass
journal, July 2006