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

Title: Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales

Abstract

Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4D evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.

Authors:
 [1];  [2];  [2];  [2];  [3]; ORCiD logo [4];  [4];  [4];  [1];  [1];  [5]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Science Dept.; Univ. College London, London (United Kingdom). London Center for Nanotechnology
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  5. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1376176
Report Number(s):
BNL-114155-2017-JA
Journal ID: ISSN 2045-2322; R&D Project: PO011; KC0201060
Grant/Contract Number:
SC0012704; AC02-06CH11357; AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Materials science; Nanoscale materials; Techniques and instrumentation

Citation Formats

Ulvestad, A., Cherukara, M. J., Harder, R., Cha, W., Robinson, I. K., Soog, S., Nelson, S., Zhu, D., Stephenson, G. B., Heinonen, O., and Jokisaari, A. Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales. United States: N. p., 2017. Web. doi:10.1038/s41598-017-09999-0.
Ulvestad, A., Cherukara, M. J., Harder, R., Cha, W., Robinson, I. K., Soog, S., Nelson, S., Zhu, D., Stephenson, G. B., Heinonen, O., & Jokisaari, A. Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales. United States. doi:10.1038/s41598-017-09999-0.
Ulvestad, A., Cherukara, M. J., Harder, R., Cha, W., Robinson, I. K., Soog, S., Nelson, S., Zhu, D., Stephenson, G. B., Heinonen, O., and Jokisaari, A. 2017. "Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales". United States. doi:10.1038/s41598-017-09999-0. https://www.osti.gov/servlets/purl/1376176.
@article{osti_1376176,
title = {Bragg Coherent Diffractive Imaging of Zinc Oxide Acoustic Phonons at Picosecond Timescales},
author = {Ulvestad, A. and Cherukara, M. J. and Harder, R. and Cha, W. and Robinson, I. K. and Soog, S. and Nelson, S. and Zhu, D. and Stephenson, G. B. and Heinonen, O. and Jokisaari, A.},
abstractNote = {Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct study with x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4D evolution of the acoustic phonons in a single zinc oxide rod with a spatial resolution of 50 nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. Lastly, we find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.},
doi = {10.1038/s41598-017-09999-0},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = 2017,
month = 8
}

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

Save / Share:
  • Mesoscale thermal transport is of fundamental interest and practical importance in materials such as thermoelectrics. Coherent lattice vibrations (acoustic phonons) govern thermal transport in crystalline solids and are affected by the shape, size, and defect density in nanoscale materials. The advent of hard x-ray free electron lasers (XFELs) capable of producing ultrafast x-ray pulses has significantly impacted the understanding of acoustic phonons by enabling their direct studywith x-rays. However, previous studies have reported ensemble-averaged results that cannot distinguish the impact of mesoscale heterogeneity on the phonon dynamics. Here we use Bragg coherent diffractive imaging (BCDI) to resolve the 4D evolutionmore » of the a coustic phonons in a single zinc oxide rod with a spatial resolution of 50nm and a temporal resolution of 25 picoseconds. We observe homogeneous (lattice breathing/rotation) and inhomogeneous (shear) acoustic phonon modes, which are compared to finite element simulations. We investigate the possibility of changing phonon dynamics by altering the crystal through acid etching. We find that the acid heterogeneously dissolves the crystal volume, which will significantly impact the phonon dynamics. In general, our results represent the first step towards understanding the effect of structural properties at the individual crystal level on phonon dynamics.« less
  • Coherent control of electronic and phononic excitations in solids, as well as chemical and biological systems on ultrafast time scales is of current research interest. In semiconductors, coherent control of phonons has been demonstrated for acoustic and optical phonons generated in superlattice structures. The bandwidth of these approaches is typically fully utilized by employing a 1-D geometry where the laser spot size is much larger than the superlattice repeat length. In this article we demonstrate coherent control of optically generated picosecond surface acoustic phonons using sub-optical wavelength absorption gratings. The generation and detection characteristics of two material systems are investigatedmore » (aluminum absorption gratings on Si and GaAs substrates). Constructive and complete destructive interference conditions are demonstrated using two pump pulses derived from a single Michelson interferometer.« less
  • Using a strain-rosette, we demonstrate the existence of transverse strain using time-resolved x-ray diffraction from multiple Bragg reflections in laser-excited bulk gallium arsenide. We find that anisotropic strain is responsible for a considerable fraction of the total lattice motion at early times before thermal equilibrium is achieved. Our measurements are described by a new model where the Poisson ratio drives transverse motion, resulting in the creation of shear waves without the need for an indirect process such as mode conversion at an interface. Finally, using the same excitation geometry with the narrow-gap semiconductor indium antimonide, we detected coherent transverse acousticmore » oscillations at frequencies of several GHz.« less
  • Using a strain-rosette, we demonstrate the existence of transverse strain using time-resolved x-ray diffraction from multiple Bragg reflections in laser-excited bulk gallium arsenide. We find that anisotropic strain is responsible for a considerable fraction of the total lattice motion at early times before thermal equilibrium is achieved. Here, our measurements are described by a new model where the Poisson ratio drives transverse motion, resulting in the creation of shear waves without the need for an indirect process such as mode conversion at an interface. Using the same excitation geometry with the narrow-gap semiconductor indium antimonide, we detected coherent transverse acousticmore » oscillations at frequencies of several GHz.« less