Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy

The conventional ultrafast pump-probe spectroscopy has primarily focused on examining the formation and decay of the excited state intermediates, but it is very difficult to detect those intermediates while the formation is slow and dissipation is much fast because of the limited concentration durin...

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Main Authors: Guo, Yuanyuan, Feng, Minjun, Kuang, Zhuoran, Abeywickrama, Chathura S., Pang, Yi, Xia, Andong
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/171373
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1713732023-10-26T07:07:16Z Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy Guo, Yuanyuan Feng, Minjun Kuang, Zhuoran Abeywickrama, Chathura S. Pang, Yi Xia, Andong School of Physical and Mathematical Sciences Science::Physics Science::Mathematics Excited-States Pyrene Derivatives The conventional ultrafast pump-probe spectroscopy has primarily focused on examining the formation and decay of the excited state intermediates, but it is very difficult to detect those intermediates while the formation is slow and dissipation is much fast because of the limited concentration during the intrinsic photocycle. To address this issue, a multipulse ultrafast pump-dump-probe spectroscopy was employed to generate and probe the short-lived ground state intermediates (GSIs) in an electronic push-pull pyrene derivative (EPP). This particular derivative undergoes planarized intramolecular charge transfer (PICT) in the excited state upon initial femtosecond pulse excitation. After applying the dump pulse once the PICT was formed, the blue-shifted transient absorption GSIs with the ground state dynamics of the structure recovery was directly observed. It is found that GSIs undergo slower reorganization than the PICT formation in the excited state of EPP due to the solvation effect with different dipole moments of ground states and excited states. These findings provide a comprehensive understanding of the full photocycle dynamics of both the ground and excited states, shedding light on the presence of hidden ground state behaviors. This work was supported by the National Natural Science Foundation of China (NSFCs, grant nos. 21827803, 22133001), the Beijing Municipal Natural Science Foundation (grant no. 2232012), the Project for High-grade, Precision, and Advance in Beijing (BUPT). 2023-10-26T07:07:16Z 2023-10-26T07:07:16Z 2023 Journal Article Guo, Y., Feng, M., Kuang, Z., Abeywickrama, C. S., Pang, Y. & Xia, A. (2023). Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy. Journal of Physical Chemistry B, 127(36), 7764-7771. https://dx.doi.org/10.1021/acs.jpcb.3c05450 1520-6106 https://hdl.handle.net/10356/171373 10.1021/acs.jpcb.3c05450 37656037 2-s2.0-85171309886 36 127 7764 7771 en Journal of Physical Chemistry B © 2023 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Physics
Science::Mathematics
Excited-States
Pyrene Derivatives
spellingShingle Science::Physics
Science::Mathematics
Excited-States
Pyrene Derivatives
Guo, Yuanyuan
Feng, Minjun
Kuang, Zhuoran
Abeywickrama, Chathura S.
Pang, Yi
Xia, Andong
Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
description The conventional ultrafast pump-probe spectroscopy has primarily focused on examining the formation and decay of the excited state intermediates, but it is very difficult to detect those intermediates while the formation is slow and dissipation is much fast because of the limited concentration during the intrinsic photocycle. To address this issue, a multipulse ultrafast pump-dump-probe spectroscopy was employed to generate and probe the short-lived ground state intermediates (GSIs) in an electronic push-pull pyrene derivative (EPP). This particular derivative undergoes planarized intramolecular charge transfer (PICT) in the excited state upon initial femtosecond pulse excitation. After applying the dump pulse once the PICT was formed, the blue-shifted transient absorption GSIs with the ground state dynamics of the structure recovery was directly observed. It is found that GSIs undergo slower reorganization than the PICT formation in the excited state of EPP due to the solvation effect with different dipole moments of ground states and excited states. These findings provide a comprehensive understanding of the full photocycle dynamics of both the ground and excited states, shedding light on the presence of hidden ground state behaviors.
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Guo, Yuanyuan
Feng, Minjun
Kuang, Zhuoran
Abeywickrama, Chathura S.
Pang, Yi
Xia, Andong
format Article
author Guo, Yuanyuan
Feng, Minjun
Kuang, Zhuoran
Abeywickrama, Chathura S.
Pang, Yi
Xia, Andong
author_sort Guo, Yuanyuan
title Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
title_short Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
title_full Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
title_fullStr Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
title_full_unstemmed Unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
title_sort unveiling solvation dynamics of excited and ground states via ultrafast pump–dump–probe spectroscopy
publishDate 2023
url https://hdl.handle.net/10356/171373
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