Tracking Electron, Proton, and Solvent Motion in Proton-Coupled Electron Transfer with Ultrafast X-rays
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| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Preprint |
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2025
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| author | Kahraman, Abdullah Sachs, Michael Ghosh, Soumen Poulter, Benjamin I. Sucre-Rosales, Estefanía Ryland, Elizabeth S. Garratt, Douglas Raj, Sumana L. Powers-Riggs, Natalia Kundu, Subhradip Hampton, Christina Y. Hoffman, David J. Coslovich, Giacomo Dakovski, Georgi L. Kramer, Patrick L. Chollet, Matthieu Mori, Roberto A. van Driel, Tim B. Lee, Sang-Jun Kunnus, Kristjan Cordones, Amy A. Schoenlein, Robert W. Vauthey, Eric Andersen, Amity Govind, Niranjan Larsen, Christopher Biasin, Elisa |
| author_facet | Kahraman, Abdullah Sachs, Michael Ghosh, Soumen Poulter, Benjamin I. Sucre-Rosales, Estefanía Ryland, Elizabeth S. Garratt, Douglas Raj, Sumana L. Powers-Riggs, Natalia Kundu, Subhradip Hampton, Christina Y. Hoffman, David J. Coslovich, Giacomo Dakovski, Georgi L. Kramer, Patrick L. Chollet, Matthieu Mori, Roberto A. van Driel, Tim B. Lee, Sang-Jun Kunnus, Kristjan Cordones, Amy A. Schoenlein, Robert W. Vauthey, Eric Andersen, Amity Govind, Niranjan Larsen, Christopher Biasin, Elisa |
| contents | Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge. We combine femtosecond optical spectroscopy, site-specific ultrafast soft X-ray absorption spectroscopy, and time-resolved X-ray scattering with advanced calculations to disentangle the elementary steps of PCET in solution. Using a ruthenium polypyridyl model complex, we directly resolve photoinduced electron redistribution, ligand-site protonation within 100 ps, and the accompanying solvent reorganization. This unified multi-modal approach provides an orbital-level, atomistic picture of PCET, showing how electronic, nuclear, and solvation degrees of freedom can be separated experimentally. Our results establish a general X-ray framework for understanding and ultimately controlling PCET in catalysis, artificial photosynthesis, and biological energy flow. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2510_03693 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Tracking Electron, Proton, and Solvent Motion in Proton-Coupled Electron Transfer with Ultrafast X-rays Kahraman, Abdullah Sachs, Michael Ghosh, Soumen Poulter, Benjamin I. Sucre-Rosales, Estefanía Ryland, Elizabeth S. Garratt, Douglas Raj, Sumana L. Powers-Riggs, Natalia Kundu, Subhradip Hampton, Christina Y. Hoffman, David J. Coslovich, Giacomo Dakovski, Georgi L. Kramer, Patrick L. Chollet, Matthieu Mori, Roberto A. van Driel, Tim B. Lee, Sang-Jun Kunnus, Kristjan Cordones, Amy A. Schoenlein, Robert W. Vauthey, Eric Andersen, Amity Govind, Niranjan Larsen, Christopher Biasin, Elisa Chemical Physics Proton-coupled electron transfer (PCET) is foundational to catalysis, bioenergetics, and energy conversion, yet capturing and disentangling the coupled motions of electrons, protons, and solvent has remained a major experimental challenge. We combine femtosecond optical spectroscopy, site-specific ultrafast soft X-ray absorption spectroscopy, and time-resolved X-ray scattering with advanced calculations to disentangle the elementary steps of PCET in solution. Using a ruthenium polypyridyl model complex, we directly resolve photoinduced electron redistribution, ligand-site protonation within 100 ps, and the accompanying solvent reorganization. This unified multi-modal approach provides an orbital-level, atomistic picture of PCET, showing how electronic, nuclear, and solvation degrees of freedom can be separated experimentally. Our results establish a general X-ray framework for understanding and ultimately controlling PCET in catalysis, artificial photosynthesis, and biological energy flow. |
| title | Tracking Electron, Proton, and Solvent Motion in Proton-Coupled Electron Transfer with Ultrafast X-rays |
| topic | Chemical Physics |
| url | https://arxiv.org/abs/2510.03693 |