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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American Physical Society
2018
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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 |
first_indexed | 2024-09-23T11:05:58Z |
format | Article |
id | mit-1721.1/118327 |
institution | Massachusetts Institute of Technology |
language | English |
last_indexed | 2024-09-23T11:05:58Z |
publishDate | 2018 |
publisher | American Physical Society |
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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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