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Title: Probing and controlling terahertz-driven structural dynamics with surface sensitivity

Abstract

Intense, single-cycle terahertz (THz) pulses are powerful tools to understand and control material properties through low-energy resonances, such as phonons. Combining this with optical second harmonic generation (SHG) makes it possible to observe the resulting ultrafast structural changes with surface sensitivity. This makes SHG an ideal method to probe phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a phonon mode in the TI Bi 2Se 3with THz pulses and use SHG to separate the resulting symmetry changes at the surface from the bulk. Furthermore, we coherently control the lattice vibrations with a pair of THz pulses. Lastly, our work demonstrates a versatile, table-top tool to probe and control phonon dynamics in a range of systems, particularly at surfaces and interfaces.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [3];  [4];  [4];  [1];  [1];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. The Ohio State Univ., Columbus, OH (United States). Center for Emergent Materials, Dept. of Physics
  3. Peac Inst. of Multiscale Sciences, Chengdu (China)
  4. Univ. of Notre Dame, IN (United States). Dept. of Physics
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1351229
Report Number(s):
LA-UR-16-27580
Journal ID: ISSN 2334-2536
Grant/Contract Number:  
AC52-06NA25396; DMR14-00432
Resource Type:
Accepted Manuscript
Journal Name:
Optica
Additional Journal Information:
Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2334-2536
Publisher:
Optical Society of America
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Material Science

Citation Formats

Bowlan, Pamela Renee, Bowlan, J., Trugman, S. A., Valdés Aguilar, R., Qi, J., Liu, X., Furdyna, J., Dobrowolska, M., Taylor, A. J., Yarotski, D. A., and Prasankumar, R. P. Probing and controlling terahertz-driven structural dynamics with surface sensitivity. United States: N. p., 2017. Web. doi:10.1364/OPTICA.4.000383.
Bowlan, Pamela Renee, Bowlan, J., Trugman, S. A., Valdés Aguilar, R., Qi, J., Liu, X., Furdyna, J., Dobrowolska, M., Taylor, A. J., Yarotski, D. A., & Prasankumar, R. P. Probing and controlling terahertz-driven structural dynamics with surface sensitivity. United States. doi:10.1364/OPTICA.4.000383.
Bowlan, Pamela Renee, Bowlan, J., Trugman, S. A., Valdés Aguilar, R., Qi, J., Liu, X., Furdyna, J., Dobrowolska, M., Taylor, A. J., Yarotski, D. A., and Prasankumar, R. P. Fri . "Probing and controlling terahertz-driven structural dynamics with surface sensitivity". United States. doi:10.1364/OPTICA.4.000383. https://www.osti.gov/servlets/purl/1351229.
@article{osti_1351229,
title = {Probing and controlling terahertz-driven structural dynamics with surface sensitivity},
author = {Bowlan, Pamela Renee and Bowlan, J. and Trugman, S. A. and Valdés Aguilar, R. and Qi, J. and Liu, X. and Furdyna, J. and Dobrowolska, M. and Taylor, A. J. and Yarotski, D. A. and Prasankumar, R. P.},
abstractNote = {Intense, single-cycle terahertz (THz) pulses are powerful tools to understand and control material properties through low-energy resonances, such as phonons. Combining this with optical second harmonic generation (SHG) makes it possible to observe the resulting ultrafast structural changes with surface sensitivity. This makes SHG an ideal method to probe phonon dynamics in topological insulators (TI), materials with unique surface transport properties. Here, we resonantly excite a phonon mode in the TI Bi2Se3with THz pulses and use SHG to separate the resulting symmetry changes at the surface from the bulk. Furthermore, we coherently control the lattice vibrations with a pair of THz pulses. Lastly, our work demonstrates a versatile, table-top tool to probe and control phonon dynamics in a range of systems, particularly at surfaces and interfaces.},
doi = {10.1364/OPTICA.4.000383},
journal = {Optica},
number = 3,
volume = 4,
place = {United States},
year = {2017},
month = {3}
}

Journal Article:
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Cited by: 5 works
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Figures / Tables:

Fig. 1 Fig. 1: Setup for THz pump, SHG-probe experiments and phonon properties of Bi2Se3. (a) The P-polarized THz excitation pulse (ETHz) is incident on the sample at θ ∼ 30°. A collinear, co-polarized 1.55 eV probe pulse (Eω) arrives at a delay $τ$ after the THz pulse. The P-polarized reflected SHGmore » signal, E, at 2ω 3.1 eV, is collected with a PMT. We also rotated the crystal about the azimuthal angle ϕ to measure the static SHG symmetry (when blocking the THz pump pulse) or the symmetry of the THz-induced changes. (b) Real (green) and imaginary (blue) parts of the linear susceptibility (χ(1)) of Bi2Se3 in the THz spectral range, clearly showing the E$^1_u$ IR-active phonon at 1.95 THz. (c) Schematic of the crystal structure of a quintuple layer of Bi2Se3 in the ab plane and a side view along the c-axis; the arrows illustrate the lattice displacements associated with the E$^1_u$ phonon (adapted from [15,30]).« less

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    Works referencing / citing this record:

    Probing and controlling terahertz-driven structural dynamics with surface sensitivity [Supplemental Data]
    dataset, March 2017

    • Bowlan, P.; Bowlan, J.; Trugman, S. A.
    • figshare-Supplementary information for journal article at DOI: 10.1364/OPTICA.4.000383, 1 PDF file (775.05 kB)
    • DOI: 10.6084/m9.figshare.c.3756653

      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.