Ultrafast Symmetry Control in Photoexcited Quantum Dots
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.
Authors
- Thomas R. Hopper
- Benjamin L. Cotts (ORCID: https://orcid.org/0000-0002-6988-5762)
- Richard D. Schaller (ORCID: https://orcid.org/0000-0001-9696-8830)
- Burak Güzeltürk (ORCID: https://orcid.org/0000-0003-1977-6485)
- Jihong Ma (ORCID: https://orcid.org/0000-0001-9142-8528)
- Ming‐Fu Lin (ORCID: https://orcid.org/0000-0001-8086-2484)
- Olaf J. Borkiewicz (ORCID: https://orcid.org/0000-0003-2370-3393)
- Patrick L. Kramer (ORCID: https://orcid.org/0000-0001-8589-1540)
- Xiaozhe Shen (ORCID: https://orcid.org/0000-0002-6844-608X)
- Dmitri V. Talapin (ORCID: https://orcid.org/0000-0002-6414-8587)
- Duan Luo (ORCID: https://orcid.org/0000-0001-5926-9870)
- Joshua Portner (ORCID: https://orcid.org/0000-0002-5926-6503)
- Aaron M. Lindenberg (ORCID: https://orcid.org/0000-0003-3233-7161)
- Ahhyun Jeong (ORCID: https://orcid.org/0000-0002-5362-0700)
- Justin C. Ondry (ORCID: https://orcid.org/0000-0001-9113-3420)
- Alexander H. Reid (ORCID: https://orcid.org/0000-0002-7587-295X)
- Uta Ruett
- Nicolas E. Watkins (ORCID: https://orcid.org/0000-0002-0417-7909)
- Xiaoyi Zhang (ORCID: https://orcid.org/0000-0001-9732-1449)
- Jin Yu (ORCID: https://orcid.org/0000-0003-2845-957X)
- Xinxin Cheng (ORCID: https://orcid.org/0000-0002-1077-809X)
- Thomas Field
- Eliza Wieman
- Mia Tarantola
- Samira Ghanbarzadeh
- Alicia M. Chandler
Institutions
- University of Vermont (US)
- Northwestern University (US)
- Argonne National Laboratory (US)
- Middlebury College (US)
- Brown University (US)
- SLAC National Accelerator Laboratory (US)
- University of Chicago (US)
- Stanford University (US)
Publication Details
- Journal
- Advanced Materials
- Published
- 2024-11-25
- DOI
- https://doi.org/10.1002/adma.202414196
- Citations
- 4
- Primary Topic
- Quantum Dots Synthesis And Properties
- Type
- article
- Field-Weighted Citation Impact
- 0.47
Funders
- National Science Foundation
- U.S. Department of Energy
- Kwanjeong Educational Foundation
- Office of Science
- TomKat Center for Sustainable Energy, Stanford University
- Division of Materials Research
- Division of Chemistry
- Basic Energy Sciences
- Workforce Development for Teachers and Scientists
- SLAC National Accelerator Laboratory
- Division of Materials Sciences and Engineering