Inverse Problems in Pump–Probe Spectroscopy
Ultrafast pump–probe spectroscopic studies allow for deep insights into the mechanisms and timescales of photophysical and photochemical processes. Extracting valuable information from these studies, such as reactive intermediates’ lifetimes and coherent oscillation frequencies, is an example of the...
| Main Authors: | , , |
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| Format: | Article |
| Language: | English |
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MDPI AG
2024-01-01
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| Series: | Photochem |
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| Online Access: | https://www.mdpi.com/2673-7256/4/1/5 |
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| author | Denis S. Tikhonov Diksha Garg Melanie Schnell |
| author_facet | Denis S. Tikhonov Diksha Garg Melanie Schnell |
| author_sort | Denis S. Tikhonov |
| collection | DOAJ |
| description | Ultrafast pump–probe spectroscopic studies allow for deep insights into the mechanisms and timescales of photophysical and photochemical processes. Extracting valuable information from these studies, such as reactive intermediates’ lifetimes and coherent oscillation frequencies, is an example of the inverse problems of chemical kinetics. This article describes a consistent approach for solving this inverse problem that avoids the common obstacles of simple least-squares fitting that can lead to unreliable results. The presented approach is based on the regularized Markov Chain Monte-Carlo sampling for the strongly nonlinear parameters, allowing for a straightforward solution of the ill-posed nonlinear inverse problem. The software to implement the described fitting routine is introduced and the numerical examples of its application are given. We will also touch on critical experimental parameters, such as the temporal overlap of pulses and cross-correlation time and their connection to the minimal reachable time resolution. |
| first_indexed | 2024-04-24T17:54:33Z |
| format | Article |
| id | doaj.art-01885d03d536474ea27c1b6a1716eaa7 |
| institution | Directory Open Access Journal |
| issn | 2673-7256 |
| language | English |
| last_indexed | 2024-04-24T17:54:33Z |
| publishDate | 2024-01-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Photochem |
| spelling | doaj.art-01885d03d536474ea27c1b6a1716eaa72024-03-27T13:59:58ZengMDPI AGPhotochem2673-72562024-01-01415711010.3390/photochem4010005Inverse Problems in Pump–Probe SpectroscopyDenis S. Tikhonov0Diksha Garg1Melanie Schnell2Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, GermanyDeutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, GermanyDeutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, GermanyUltrafast pump–probe spectroscopic studies allow for deep insights into the mechanisms and timescales of photophysical and photochemical processes. Extracting valuable information from these studies, such as reactive intermediates’ lifetimes and coherent oscillation frequencies, is an example of the inverse problems of chemical kinetics. This article describes a consistent approach for solving this inverse problem that avoids the common obstacles of simple least-squares fitting that can lead to unreliable results. The presented approach is based on the regularized Markov Chain Monte-Carlo sampling for the strongly nonlinear parameters, allowing for a straightforward solution of the ill-posed nonlinear inverse problem. The software to implement the described fitting routine is introduced and the numerical examples of its application are given. We will also touch on critical experimental parameters, such as the temporal overlap of pulses and cross-correlation time and their connection to the minimal reachable time resolution.https://www.mdpi.com/2673-7256/4/1/5pump–probe spectroscopyinverse problemsMonte-Carlo sampling |
| spellingShingle | Denis S. Tikhonov Diksha Garg Melanie Schnell Inverse Problems in Pump–Probe Spectroscopy Photochem pump–probe spectroscopy inverse problems Monte-Carlo sampling |
| title | Inverse Problems in Pump–Probe Spectroscopy |
| title_full | Inverse Problems in Pump–Probe Spectroscopy |
| title_fullStr | Inverse Problems in Pump–Probe Spectroscopy |
| title_full_unstemmed | Inverse Problems in Pump–Probe Spectroscopy |
| title_short | Inverse Problems in Pump–Probe Spectroscopy |
| title_sort | inverse problems in pump probe spectroscopy |
| topic | pump–probe spectroscopy inverse problems Monte-Carlo sampling |
| url | https://www.mdpi.com/2673-7256/4/1/5 |
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