Ultrafast Symmetry Control in Photoexcited Quantum Dots

Ultrafast Symmetry Control in Photoexcited Quantum Dots

© 2024 UChicago Argonne, LLC, Operator of Argonne National Laboratory and The Author(s). Advanced Materials published by Wiley‐VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - (2024) vom: 25. Nov., Seite e2414196
1. Verfasser: Guzelturk, Burak (VerfasserIn)
Weitere Verfasser: Portner, Joshua, Ondry, Justin, Ghanbarzadeh, Samira, Tarantola, Mia, Jeong, Ahhyun, Field, Thomas, Chandler, Alicia M, Wieman, Eliza, Hopper, Thomas R, Watkins, Nicolas E, Yu, Jin, Cheng, Xinxin, Lin, Ming-Fu, Luo, Duan, Kramer, Patrick L, Shen, Xiaozhe, Reid, Alexander H, Borkiewicz, Olaf, Ruett, Uta, Zhang, Xiaoyi, Lindenberg, Aaron M, Ma, Jihong, Schaller, Richard D, Talapin, Dmitri V, Cotts, Benjamin L
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2024
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article PbS photoexcitation quantum dots symmetry ultrafast
Beschreibung
Zusammenfassung:© 2024 UChicago Argonne, LLC, Operator of Argonne National Laboratory and The Author(s). Advanced Materials published by Wiley‐VCH GmbH.
Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales
Beschreibung:Date Revised 25.11.2024
published: Print-Electronic
Citation Status Publisher
ISSN:1521-4095
DOI:10.1002/adma.202414196