Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase

Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. The direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic ins...

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Main Authors: Shin, Taeho, Cheng, Yu-Hsiang, Teitelbaum, Samuel Welch, Wolfson, Johanna W., Porter, Ilana J., Kandyla, Maria, Nelson, Keith Adam
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:English
Published: American Physical Society 2018
Online Access:http://hdl.handle.net/1721.1/118327
https://orcid.org/0000-0002-0812-9832
https://orcid.org/0000-0001-7804-5418
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author Shin, Taeho
Cheng, Yu-Hsiang
Teitelbaum, Samuel Welch
Wolfson, Johanna W.
Porter, Ilana J.
Kandyla, Maria
Nelson, Keith Adam
author2 Massachusetts Institute of Technology. Department of Chemistry
author_facet Massachusetts Institute of Technology. Department of Chemistry
Shin, Taeho
Cheng, Yu-Hsiang
Teitelbaum, Samuel Welch
Wolfson, Johanna W.
Porter, Ilana J.
Kandyla, Maria
Nelson, Keith Adam
author_sort Shin, Taeho
collection MIT
description Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. The direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases, photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This requirement precludes conventional ultrafast spectroscopy, in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we are able to observe the photoinduced phase transition from the semimetallic, low-symmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities is predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10  mJ/cm[superscript 2] in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for several picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration. Subject Areas: Condensed Matter Physics, Materials Science, Physical Chemistry
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spelling mit-1721.1/1183272022-09-27T17:08:20Z Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase Shin, Taeho Cheng, Yu-Hsiang Teitelbaum, Samuel Welch Wolfson, Johanna W. Porter, Ilana J. Kandyla, Maria Nelson, Keith Adam Massachusetts Institute of Technology. Department of Chemistry Teitelbaum, Samuel Welch Wolfson, Johanna W. Porter, Ilana J. Kandyla, Maria Nelson, Keith Adam Excursions far from their equilibrium structures can bring crystalline solids through collective transformations including transitions into new phases that may be transient or long-lived. The direct spectroscopic observation of far-from-equilibrium rearrangements provides fundamental mechanistic insight into chemical and structural transformations and a potential route to practical applications, including ultrafast optical control over material structure and properties. However, in many cases, photoinduced transitions are irreversible or only slowly reversible, or the light fluence required exceeds material damage thresholds. This requirement precludes conventional ultrafast spectroscopy, in which optical excitation and probe pulses irradiate the sample many times, each measurement providing information about the sample response at just one probe delay time following excitation, with each measurement at a high repetition rate and with the sample fully recovering its initial state in between measurements. Using a single-shot, real-time measurement method, we are able to observe the photoinduced phase transition from the semimetallic, low-symmetry phase of crystalline bismuth into a high-symmetry phase whose existence at high electronic excitation densities is predicted based on earlier measurements at moderate excitation densities below the damage threshold. Our observations indicate that coherent lattice vibrational motion launched upon photoexcitation with an incident fluence above 10  mJ/cm[superscript 2] in bulk bismuth brings the lattice structure directly into the high-symmetry configuration for several picoseconds, after which carrier relaxation and diffusion restore the equilibrium lattice configuration. Subject Areas: Condensed Matter Physics, Materials Science, Physical Chemistry United States. Office of Naval Research (Grant N00014-12-1- 0530) United States. Office of Naval Research (Grant N00014-16-1-2090) National Science Foundation (U.S.) (Grant CHE-1111557) 2018-10-01T19:52:23Z 2018-10-01T19:52:23Z 2018-09 2018-03 2018-09-26T18:00:20Z Article http://purl.org/eprint/type/JournalArticle 2160-3308 http://hdl.handle.net/1721.1/118327 Teitelbaum, Samuel W., et al. “Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase.” Physical Review X, vol. 8, no. 3, Sept. 2018. © 2018 American Physical Society https://orcid.org/0000-0002-0812-9832 https://orcid.org/0000-0001-7804-5418 en http://dx.doi.org/10.1103/PhysRevX.8.031081 Physical Review X Creative Commons Attribution http://creativecommons.org/licenses/by/3.0 application/pdf American Physical Society American Physical Society
spellingShingle Shin, Taeho
Cheng, Yu-Hsiang
Teitelbaum, Samuel Welch
Wolfson, Johanna W.
Porter, Ilana J.
Kandyla, Maria
Nelson, Keith Adam
Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title_full Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title_fullStr Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title_full_unstemmed Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title_short Real-Time Observation of a Coherent Lattice Transformation into a High-Symmetry Phase
title_sort real time observation of a coherent lattice transformation into a high symmetry phase
url http://hdl.handle.net/1721.1/118327
https://orcid.org/0000-0002-0812-9832
https://orcid.org/0000-0001-7804-5418
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