Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane
We employ few-cycle pulses to strong-field-ionize di-iodomethane (CH2I2) and femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to investigate the subsequent ultrafast dissociative ionization and vibrational wave packet dynamics. Probing in the spectral region of the I 4d core-l...
Հիմնական հեղինակներ: | , , , , , |
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Այլ հեղինակներ: | |
Ձևաչափ: | Journal Article |
Լեզու: | English |
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2020
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Առցանց հասանելիություն: | https://hdl.handle.net/10356/143149 |
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author | Wei, Zhengrong Li, Jialin Zhang, Huimin Lu, Yunpeng Yang, Minghui Loh, Zhi-Heng |
author2 | School of Physical and Mathematical Sciences |
author_facet | School of Physical and Mathematical Sciences Wei, Zhengrong Li, Jialin Zhang, Huimin Lu, Yunpeng Yang, Minghui Loh, Zhi-Heng |
author_sort | Wei, Zhengrong |
collection | NTU |
description | We employ few-cycle pulses to strong-field-ionize di-iodomethane (CH2I2) and femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to investigate the subsequent ultrafast dissociative ionization and vibrational wave packet dynamics. Probing in the spectral region of the I 4d core-level transitions, the time-resolved XUV differential absorption spectra reveal the population of several electronic states of CH2I2+ by strong-field ionization. Global analysis reveals three distinct time scales for the observed dynamics: 20 ± 2 fs, 49 ± 6 fs, and 157 ± 9 fs, ascribed to relaxation of the CH2I2+ parent ion from the Franck-Condon region, dissociation of high-lying excited states of CH2I2+ to I+ (3P2), CH2I, and I2+ (2Π3/2,g), and dissociation of CH2I2+ to I (2P3/2) and CH2I+, respectively. Oscillatory features in the time-resolved XUV differential absorption spectra point to the generation of vibrational wave packets in both the residual CH2I2 and the CH2I2+ parent ion. Analysis of the oscillation frequencies and phases reveals, in the case of neutral CH2I2, C-I symmetric stretching induced by bond softening and I-C-I bending driven by a combination of bond softening and R-selective depletion. In the case of CH2I2+, both the fundamental and first overtone frequencies of the I-C-I bending mode are observed, indicating large-amplitude I-C-I bending motion, in good agreement with results obtained from ab initio simulations of the XUV transition energy along the I-C-I bend coordinate. These results show that femtosecond XUV absorption spectroscopy is well-suited for studying ultrafast photodissociation and vibrational wave packet dynamics. |
first_indexed | 2024-10-01T03:02:23Z |
format | Journal Article |
id | ntu-10356/143149 |
institution | Nanyang Technological University |
language | English |
last_indexed | 2024-10-01T03:02:23Z |
publishDate | 2020 |
record_format | dspace |
spelling | ntu-10356/1431492023-10-24T01:23:10Z Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane Wei, Zhengrong Li, Jialin Zhang, Huimin Lu, Yunpeng Yang, Minghui Loh, Zhi-Heng School of Physical and Mathematical Sciences Centre for Optical Fibre Technology The Photonics Institute Science::Chemistry Photodissociation Quantum Coherence We employ few-cycle pulses to strong-field-ionize di-iodomethane (CH2I2) and femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to investigate the subsequent ultrafast dissociative ionization and vibrational wave packet dynamics. Probing in the spectral region of the I 4d core-level transitions, the time-resolved XUV differential absorption spectra reveal the population of several electronic states of CH2I2+ by strong-field ionization. Global analysis reveals three distinct time scales for the observed dynamics: 20 ± 2 fs, 49 ± 6 fs, and 157 ± 9 fs, ascribed to relaxation of the CH2I2+ parent ion from the Franck-Condon region, dissociation of high-lying excited states of CH2I2+ to I+ (3P2), CH2I, and I2+ (2Π3/2,g), and dissociation of CH2I2+ to I (2P3/2) and CH2I+, respectively. Oscillatory features in the time-resolved XUV differential absorption spectra point to the generation of vibrational wave packets in both the residual CH2I2 and the CH2I2+ parent ion. Analysis of the oscillation frequencies and phases reveals, in the case of neutral CH2I2, C-I symmetric stretching induced by bond softening and I-C-I bending driven by a combination of bond softening and R-selective depletion. In the case of CH2I2+, both the fundamental and first overtone frequencies of the I-C-I bending mode are observed, indicating large-amplitude I-C-I bending motion, in good agreement with results obtained from ab initio simulations of the XUV transition energy along the I-C-I bend coordinate. These results show that femtosecond XUV absorption spectroscopy is well-suited for studying ultrafast photodissociation and vibrational wave packet dynamics. Published version 2020-08-05T08:04:30Z 2020-08-05T08:04:30Z 2019 Journal Article Wei, Z., Li, J., Zhang, H., Lu, Y., Yang, M., & Loh, Z.-H. (2019). Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized Di-iodomethane. The Journal of Chemical Physics, 151(21), 214308-. doi:10.1063/1.5132967 0021-9606 https://hdl.handle.net/10356/143149 10.1063/1.5132967 31822095 2-s2.0-85076224194 21 151 en The Journal of Chemical Physics 10.21979/N9/WVRVOP © 2019 Author(s). All rights reserved. This paper was published by AIP Publishing in The Journal of Chemical Physics and is made available with permission of Author(s). application/pdf |
spellingShingle | Science::Chemistry Photodissociation Quantum Coherence Wei, Zhengrong Li, Jialin Zhang, Huimin Lu, Yunpeng Yang, Minghui Loh, Zhi-Heng Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title | Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title_full | Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title_fullStr | Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title_full_unstemmed | Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title_short | Ultrafast dissociative ionization and large-amplitude vibrational wave packet dynamics of strong-field-ionized di-iodomethane |
title_sort | ultrafast dissociative ionization and large amplitude vibrational wave packet dynamics of strong field ionized di iodomethane |
topic | Science::Chemistry Photodissociation Quantum Coherence |
url | https://hdl.handle.net/10356/143149 |
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