All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane
In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d5/2-σ∗ transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-defined exci...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2022
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| Online Access: | https://hdl.handle.net/10356/154041 |
| _version_ | 1826129873657135104 |
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| author | Rebholz, M. Ding, T. Despré, V. Aufleger, L. Hartmann, M. Meyer, K. Stooß, V. Magunia, A. Wachs, D. Birk, P. Mi, Y. Borisova, G. D. Castanheira, C. D. C. Rupprecht, P. Schmid, G. Schnorr, K. Schröter, C. D. Moshammer, R. Loh, Zhi-Heng Attar, A. R. Leone, S. R. Gaumnitz, T. Wörner, H. J. Roling, S. Butz, M. Zacharias, H. Düsterer, S. Treusch, R. Brenner, G. Vester, J. Kuleff, A. I. Ott, C. Pfeifer, T. |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Rebholz, M. Ding, T. Despré, V. Aufleger, L. Hartmann, M. Meyer, K. Stooß, V. Magunia, A. Wachs, D. Birk, P. Mi, Y. Borisova, G. D. Castanheira, C. D. C. Rupprecht, P. Schmid, G. Schnorr, K. Schröter, C. D. Moshammer, R. Loh, Zhi-Heng Attar, A. R. Leone, S. R. Gaumnitz, T. Wörner, H. J. Roling, S. Butz, M. Zacharias, H. Düsterer, S. Treusch, R. Brenner, G. Vester, J. Kuleff, A. I. Ott, C. Pfeifer, T. |
| author_sort | Rebholz, M. |
| collection | NTU |
| description | In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d5/2-σ∗ transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-defined excited state. We subsequently measure the time-dependent absorption change of the molecule with the FEL probe spectrum centered on the same I: 4d resonance. Using ab initio calculations of absorption spectra of a transient isomerization pathway observed in earlier studies, our time-resolved measurements allow us to assign the timescales of the previously reported direct and indirect dissociation pathways. The presented method is thus sensitive to excited-state molecular geometries in a time-resolved manner, following a core-resonant site-specific trigger. |
| first_indexed | 2024-10-01T07:47:39Z |
| format | Journal Article |
| id | ntu-10356/154041 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T07:47:39Z |
| publishDate | 2022 |
| record_format | dspace |
| spelling | ntu-10356/1540412023-02-28T19:59:45Z All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane Rebholz, M. Ding, T. Despré, V. Aufleger, L. Hartmann, M. Meyer, K. Stooß, V. Magunia, A. Wachs, D. Birk, P. Mi, Y. Borisova, G. D. Castanheira, C. D. C. Rupprecht, P. Schmid, G. Schnorr, K. Schröter, C. D. Moshammer, R. Loh, Zhi-Heng Attar, A. R. Leone, S. R. Gaumnitz, T. Wörner, H. J. Roling, S. Butz, M. Zacharias, H. Düsterer, S. Treusch, R. Brenner, G. Vester, J. Kuleff, A. I. Ott, C. Pfeifer, T. School of Physical and Mathematical Sciences Science::Chemistry Atomic Physics Molecular Physics In this work, we use an extreme-ultraviolet (XUV) free-electron laser (FEL) to resonantly excite the I: 4d5/2-σ∗ transition of a gas-phase di-iodomethane (CH2I2) target. This site-specific excitation generates a 4d core hole located at an iodine site, which leaves the molecule in a well-defined excited state. We subsequently measure the time-dependent absorption change of the molecule with the FEL probe spectrum centered on the same I: 4d resonance. Using ab initio calculations of absorption spectra of a transient isomerization pathway observed in earlier studies, our time-resolved measurements allow us to assign the timescales of the previously reported direct and indirect dissociation pathways. The presented method is thus sensitive to excited-state molecular geometries in a time-resolved manner, following a core-resonant site-specific trigger. Ministry of Education (MOE) Published version For their support during the experiment, we thankfully acknowledge the technical and scientific staff at FLASH. We gratefully acknowledge C. Kaiser and B. Knape for their technical support. We acknowledge funding from the European Research Council (ERC) (X-MuSiC-616783). Z.-H. L. acknowledges support from the Ministry of Education, Singapore (RG105/17 and RG1/20). V. D. and A. I. K. acknowledge the financial support of DFG through QUTIF Priority Programme. S. R. L. acknowledges the support of the GPCP and AMOS programs of the Division of Chemical Sciences, Geosciences, and Biosciences of the U.S. Department of Energy at LBNL underContract No. DEAC02-05CH11231 and the National Science Foundation underGrant No.CHE-1660417. H. Z. acknowledges support by the BMBF (Project No. 05K13PM2). 2022-02-08T08:22:45Z 2022-02-08T08:22:45Z 2021 Journal Article Rebholz, M., Ding, T., Despré, V., Aufleger, L., Hartmann, M., Meyer, K., Stooß, V., Magunia, A., Wachs, D., Birk, P., Mi, Y., Borisova, G. D., Castanheira, C. D. C., Rupprecht, P., Schmid, G., Schnorr, K., Schröter, C. D., Moshammer, R., Loh, Z., ...Pfeifer, T. (2021). All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane. Physical Review X, 11(3), 031001-. https://dx.doi.org/10.1103/PhysRevX.11.031001 2160-3308 https://hdl.handle.net/10356/154041 10.1103/PhysRevX.11.031001 2-s2.0-85110547820 3 11 031001 en RG105/17 RG1/20 Physical Review X © 2021 The Author(s). Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Open access publication funded by the Max Planck Society. application/pdf |
| spellingShingle | Science::Chemistry Atomic Physics Molecular Physics Rebholz, M. Ding, T. Despré, V. Aufleger, L. Hartmann, M. Meyer, K. Stooß, V. Magunia, A. Wachs, D. Birk, P. Mi, Y. Borisova, G. D. Castanheira, C. D. C. Rupprecht, P. Schmid, G. Schnorr, K. Schröter, C. D. Moshammer, R. Loh, Zhi-Heng Attar, A. R. Leone, S. R. Gaumnitz, T. Wörner, H. J. Roling, S. Butz, M. Zacharias, H. Düsterer, S. Treusch, R. Brenner, G. Vester, J. Kuleff, A. I. Ott, C. Pfeifer, T. All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title | All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title_full | All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title_fullStr | All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title_full_unstemmed | All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title_short | All-XUV pump-probe transient absorption spectroscopy of the structural molecular dynamics of di-iodomethane |
| title_sort | all xuv pump probe transient absorption spectroscopy of the structural molecular dynamics of di iodomethane |
| topic | Science::Chemistry Atomic Physics Molecular Physics |
| url | https://hdl.handle.net/10356/154041 |
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