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Title: Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields

Abstract

Nanoscale phonon transport is a key process that governs thermal conduction in a wide range of materials and devices. Creating controlled phonon populations by resonant excitation at terahertz (THz) frequencies can drastically change the characteristics of nanoscale thermal transport and allow a direct real-space characterization of phonon mean-free paths. Using metamaterial-enhanced terahertz excitation, we tailored a phononic excitation by selectively populating low-frequency phonons within a nanoscale volume in a ferroelectric BaTiO 3 thin film. Real-space time-resolved x-ray diffraction microscopy following THz excitation reveals ballistic phonon transport over a distance of hundreds of nm, two orders of magnitude longer than the averaged phonon mean-free path in BaTiO 3. On longer length scales, diffusive phonon transport dominates the recovery of the transient strain response, largely due to heat conduction into the substrate. The measured real-space phonon transport can be directly compared with the phonon mean-free path as predicted by molecular dynamics modeling. In conclusion, this time-resolved real-space visualization of THz-matter interactions opens up opportunities to engineer and image nanoscale transient structural states with new functionalities.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [1];  [1];  [1];  [1];  [1];  [4];  [1];  [3];  [5];  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Univ. of Wisconsin, Madison, WI (United States)
  4. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (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:
1420052
Alternate Identifier(s):
OSTI ID: 1409131; OSTI ID: 1420068
Grant/Contract Number:  
SC0012375; AC02-06CH11357; AC02-05CH11231; AC02-76SF00515; FG02-04ER46147; W911NF-14-1-0104
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 1; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Zhu, Yi, Chen, Frank, Park, Joonkyu, Sasikumar, Kiran, Hu, Bin, Damodaran, Anoop R., Jung, Il Woong, Highland, Matthew J., Cai, Zhonghou, Tung, I-Cheng, Walko, Donald A., Freeland, John W., Martin, Lane W., Sankaranarayanan, Subramanian K. R. S., Evans, Paul G., Lindenberg, Aaron M., and Wen, Haidan. Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields. United States: N. p., 2017. Web. doi:10.1103/physrevmaterials.1.060601.
Zhu, Yi, Chen, Frank, Park, Joonkyu, Sasikumar, Kiran, Hu, Bin, Damodaran, Anoop R., Jung, Il Woong, Highland, Matthew J., Cai, Zhonghou, Tung, I-Cheng, Walko, Donald A., Freeland, John W., Martin, Lane W., Sankaranarayanan, Subramanian K. R. S., Evans, Paul G., Lindenberg, Aaron M., & Wen, Haidan. Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields. United States. doi:10.1103/physrevmaterials.1.060601.
Zhu, Yi, Chen, Frank, Park, Joonkyu, Sasikumar, Kiran, Hu, Bin, Damodaran, Anoop R., Jung, Il Woong, Highland, Matthew J., Cai, Zhonghou, Tung, I-Cheng, Walko, Donald A., Freeland, John W., Martin, Lane W., Sankaranarayanan, Subramanian K. R. S., Evans, Paul G., Lindenberg, Aaron M., and Wen, Haidan. Thu . "Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields". United States. doi:10.1103/physrevmaterials.1.060601. https://www.osti.gov/servlets/purl/1420052.
@article{osti_1420052,
title = {Structural imaging of nanoscale phonon transport in ferroelectrics excited by metamaterial-enhanced terahertz fields},
author = {Zhu, Yi and Chen, Frank and Park, Joonkyu and Sasikumar, Kiran and Hu, Bin and Damodaran, Anoop R. and Jung, Il Woong and Highland, Matthew J. and Cai, Zhonghou and Tung, I-Cheng and Walko, Donald A. and Freeland, John W. and Martin, Lane W. and Sankaranarayanan, Subramanian K. R. S. and Evans, Paul G. and Lindenberg, Aaron M. and Wen, Haidan},
abstractNote = {Nanoscale phonon transport is a key process that governs thermal conduction in a wide range of materials and devices. Creating controlled phonon populations by resonant excitation at terahertz (THz) frequencies can drastically change the characteristics of nanoscale thermal transport and allow a direct real-space characterization of phonon mean-free paths. Using metamaterial-enhanced terahertz excitation, we tailored a phononic excitation by selectively populating low-frequency phonons within a nanoscale volume in a ferroelectric BaTiO3 thin film. Real-space time-resolved x-ray diffraction microscopy following THz excitation reveals ballistic phonon transport over a distance of hundreds of nm, two orders of magnitude longer than the averaged phonon mean-free path in BaTiO3. On longer length scales, diffusive phonon transport dominates the recovery of the transient strain response, largely due to heat conduction into the substrate. The measured real-space phonon transport can be directly compared with the phonon mean-free path as predicted by molecular dynamics modeling. In conclusion, this time-resolved real-space visualization of THz-matter interactions opens up opportunities to engineer and image nanoscale transient structural states with new functionalities.},
doi = {10.1103/physrevmaterials.1.060601},
journal = {Physical Review Materials},
number = 6,
volume = 1,
place = {United States},
year = {2017},
month = {11}
}

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Figures / Tables:

Figure 1 Figure 1: Schematic of the experiment. The vertically polarized THz pulses are focused onto the sample surface. The THz field is enhanced near the horizontal gold gaps (red-colored ellipses) of the split-ring resonators shown by the gold color. An x-ray beam is focused by a Fresnel zone plate to probemore » locally in the vicinity of the field-enhanced regions and the diffracted x-ray beam is collected by an area detector. The inset shows the unit cell of BaTiO3.« less

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