Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory
We present time-resolved X-ray absorption spectra of ionized liquid water and demonstrate that OH radicals, H3O+ ions, and solvated electrons all leave distinct X-ray-spectroscopic signatures. Particularly, this allows us to characterize the electron solvation process through a tool that focuses on...
| Main Authors: | , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/179940 |
| _version_ | 1811679933807722496 |
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| author | Moros, Arturo Sopena Li, Shuai Li, Kai Doumy, Gilles Southworth, Stephen H. Otolski, Christopher Schaller, Richard D. Kumagai, Yoshiaki Rubensson, Jan-Erik Simon, Marc Dakovski, Georgi Kunnus, Kristjan Robinson, Joseph S. Hampton, Christina Y. Hoffman, David J. Koralek, Jake Loh, Zhi-Heng Santra, Robin Inhester, Ludger Young, Linda |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Moros, Arturo Sopena Li, Shuai Li, Kai Doumy, Gilles Southworth, Stephen H. Otolski, Christopher Schaller, Richard D. Kumagai, Yoshiaki Rubensson, Jan-Erik Simon, Marc Dakovski, Georgi Kunnus, Kristjan Robinson, Joseph S. Hampton, Christina Y. Hoffman, David J. Koralek, Jake Loh, Zhi-Heng Santra, Robin Inhester, Ludger Young, Linda |
| author_sort | Moros, Arturo Sopena |
| collection | NTU |
| description | We present time-resolved X-ray absorption spectra of ionized liquid water and demonstrate that OH radicals, H3O+ ions, and solvated electrons all leave distinct X-ray-spectroscopic signatures. Particularly, this allows us to characterize the electron solvation process through a tool that focuses on the electronic response of oxygen atoms in the immediate vicinity of a solvated electron. Our experimental results, supported by ab initio calculations, confirm the formation of a cavity in which the solvated electron is trapped. We show that the solvation dynamics are governed by the magnitude of the random structural fluctuations present in water. As a consequence, the solvation time is highly sensitive to temperature and to the specific way the electron is injected into water. |
| first_indexed | 2024-10-01T03:17:02Z |
| format | Journal Article |
| id | ntu-10356/179940 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T03:17:02Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1799402024-09-06T15:31:43Z Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory Moros, Arturo Sopena Li, Shuai Li, Kai Doumy, Gilles Southworth, Stephen H. Otolski, Christopher Schaller, Richard D. Kumagai, Yoshiaki Rubensson, Jan-Erik Simon, Marc Dakovski, Georgi Kunnus, Kristjan Robinson, Joseph S. Hampton, Christina Y. Hoffman, David J. Koralek, Jake Loh, Zhi-Heng Santra, Robin Inhester, Ludger Young, Linda School of Chemistry, Chemical Engineering and Biotechnology School of Physical and Mathematical Sciences Chemistry Cavity formation Electron solvation We present time-resolved X-ray absorption spectra of ionized liquid water and demonstrate that OH radicals, H3O+ ions, and solvated electrons all leave distinct X-ray-spectroscopic signatures. Particularly, this allows us to characterize the electron solvation process through a tool that focuses on the electronic response of oxygen atoms in the immediate vicinity of a solvated electron. Our experimental results, supported by ab initio calculations, confirm the formation of a cavity in which the solvated electron is trapped. We show that the solvation dynamics are governed by the magnitude of the random structural fluctuations present in water. As a consequence, the solvation time is highly sensitive to temperature and to the specific way the electron is injected into water. Ministry of Education (MOE) Published version A.S.M., L.I., and R.S. acknowledge support from DESY(Hamburg, Germany), a member of the Helmholtz Association HGF, and also acknowledge the scientific exchange and support of the Centre for Molecular Water Science (CMWS).R.S. and L.I. acknowledge support from the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)-EXC 2056-project ID 390715994. This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Science, Chemical Sciences, Geosciences and Biosciences Division, which supported the Argonne group under contract numberDE-AC02-06CH11357. Z.-H.L. is supported by the Ministry of Education, Singapore (grants MOE-T2EP50221-0004, RG1/20, and RG1/22). J.-E.R. acknowledges support from Swedish Research Council, Project No. 2021-04017. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, and resources of the Center for Nanoscale Materials (CNM), Argonne National Laboratory are supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES) under Contracts DE-AC02-76SF00515 and DE-AC02-06CH11357. 2024-09-04T02:02:16Z 2024-09-04T02:02:16Z 2024 Journal Article Moros, A. S., Li, S., Li, K., Doumy, G., Southworth, S. H., Otolski, C., Schaller, R. D., Kumagai, Y., Rubensson, J., Simon, M., Dakovski, G., Kunnus, K., Robinson, J. S., Hampton, C. Y., Hoffman, D. J., Koralek, J., Loh, Z., Santra, R., Inhester, L. & Young, L. (2024). Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory. Journal of the American Chemical Society, 146(5), 3262-3269. https://dx.doi.org/10.1021/jacs.3c11857 0002-7863 https://hdl.handle.net/10356/179940 10.1021/jacs.3c11857 38270463 2-s2.0-85184523068 5 146 3262 3269 en MOE-T2EP50221-0004 RG1/20 RG1/22 Journal of the American Chemical Society © 2024 The Authors. Published by American Chemical Society. This article is licensed under CC-BY 4.0. application/pdf |
| spellingShingle | Chemistry Cavity formation Electron solvation Moros, Arturo Sopena Li, Shuai Li, Kai Doumy, Gilles Southworth, Stephen H. Otolski, Christopher Schaller, Richard D. Kumagai, Yoshiaki Rubensson, Jan-Erik Simon, Marc Dakovski, Georgi Kunnus, Kristjan Robinson, Joseph S. Hampton, Christina Y. Hoffman, David J. Koralek, Jake Loh, Zhi-Heng Santra, Robin Inhester, Ludger Young, Linda Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title | Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title_full | Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title_fullStr | Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title_full_unstemmed | Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title_short | Tracking cavity formation in electron solvation: insights from x‑ray spectroscopy and theory |
| title_sort | tracking cavity formation in electron solvation insights from x ray spectroscopy and theory |
| topic | Chemistry Cavity formation Electron solvation |
| url | https://hdl.handle.net/10356/179940 |
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