Resolving length-scale-dependent transient disorder through an ultrafast phase transition

Griffiths, Jack; Suzana, Ana F.; Wu, Longlong; Marks, Samuel D.; Esposito, Vincent; Boutet, Sébastien; Evans, Paul G.; Mitchell, J. F.; Dean, Mark P. M.; Keen, David A.; Robinson, Ian; Billinge, Simon J. L.; Bozin, Emil S.

doi:10.1038/s41563-024-01927-8

Resolving length-scale-dependent transient disorder through an ultrafast phase transition

Journal Article · Thu Jun 13 00:00:00 EDT 2024 · Nature Materials

DOI:https://doi.org/10.1038/s41563-024-01927-8· OSTI ID:2403576

; ; ; Marks, Samuel D.; ; Boutet, Sébastien; ; ; ; ; Robinson, Ian; ;

Abstract

Material functionality can be strongly determined by structure extending only over nanoscale distances. The pair distribution function presents an opportunity for structural studies beyond idealized crystal models and to investigate structure over varying length scales. Applying this method with ultrafast time resolution has the potential to similarly disrupt the study of structural dynamics and phase transitions. Here we demonstrate such a measurement of CuIr ₂ S ₄ optically pumped from its low-temperature Ir-dimerized phase. Dimers are optically suppressed without spatial correlation, generating a structure whose level of disorder strongly depends on the length scale. The redevelopment of structural ordering over tens of picoseconds is directly tracked over both space and time as a transient state is approached. This measurement demonstrates the crucial role of local structure and disorder in non-equilibrium processes as well as the feasibility of accessing this information with state-of-the-art XFEL facilities.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; FG02-04ER46147; SC0012704

OSTI ID:: 2403576

Alternate ID(s):: OSTI ID: 2367440
OSTI ID: 2440139

Report Number(s):: BNL--225635-2024-JAAM; PII: 1927

Journal Information:: Nature Materials, Journal Name: Nature Materials; ISSN 1476-1122

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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