The effect of solvent relaxation in the ultrafast time-resolved spectroscopy of solvated benzophenone
Benzophenone (BP) despite its relatively simple molecular structure is a paradigmatic sensitizer, featuring both photocatalytic and photobiological effects due to its rather complex photophysical properties. In this contribution we report an original theoretical approach to model realistic, ultra-fa...
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| Veröffentlicht in: | Photochemical & photobiological sciences 2018, Vol.17 (3), p.323-331 |
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| creator | Zvereva, Elena Segarra-Martí, Javier Marazzi, Marco Brazard, Johanna Nenov, Artur Weingart, Oliver Léonard, Jérémie Garavelli, Marco Rivalta, Ivan Dumont, Elise Assfeld, Xavier Haacke, Stefan Monari, Antonio |
| description | Benzophenone (BP) despite its relatively simple molecular structure is a paradigmatic sensitizer, featuring both photocatalytic and photobiological effects due to its rather complex photophysical properties. In this contribution we report an original theoretical approach to model realistic, ultra-fast spectroscopy data, which requires describing intra- and intermolecular energy and structural relaxation. In particular we explicitly simulate time-resolved pump-probe spectra using a combination of state-of-the art hybrid quantum mechanics/molecular mechanics dynamics to treat relaxation and vibrational effects. The comparison with experimental transient absorption data demonstrates the efficiency and accuracy of our approach. Furthermore the explicit inclusion of the solvent, water for simulation and methanol for experiment, allows us, despite the inherent different behavior of the two, to underline the role played by the H-bonding relaxation in the first hundreds of femtoseconds after optical excitation. Finally we predict for the first time the two-dimensional electronic spectrum (2DES) of BP taking into account the vibrational effects and hence modelling partially symmetric and asymmetric ultrafast broadening. |
| doi_str_mv | 10.1039/c7pp00439g |
| format | Article |
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In this contribution we report an original theoretical approach to model realistic, ultra-fast spectroscopy data, which requires describing intra- and intermolecular energy and structural relaxation. In particular we explicitly simulate time-resolved pump-probe spectra using a combination of state-of-the art hybrid quantum mechanics/molecular mechanics dynamics to treat relaxation and vibrational effects. The comparison with experimental transient absorption data demonstrates the efficiency and accuracy of our approach. Furthermore the explicit inclusion of the solvent, water for simulation and methanol for experiment, allows us, despite the inherent different behavior of the two, to underline the role played by the H-bonding relaxation in the first hundreds of femtoseconds after optical excitation. Finally we predict for the first time the two-dimensional electronic spectrum (2DES) of BP taking into account the vibrational effects and hence modelling partially symmetric and asymmetric ultrafast broadening.</description><identifier>ISSN: 1474-905X</identifier><identifier>EISSN: 1474-9092</identifier><identifier>DOI: 10.1039/c7pp00439g</identifier><identifier>PMID: 29383356</identifier><language>eng</language><publisher>Cham: Springer International Publishing</publisher><subject>Benzophenone ; Biochemistry ; Biomaterials ; Chemical bonds ; Chemical Sciences ; Chemistry ; Computer simulation ; Molecular structure ; Physical Chemistry ; Plant Sciences ; Quantum mechanics ; Solvents ; Spectroscopy ; Spectrum analysis</subject><ispartof>Photochemical & photobiological sciences, 2018, Vol.17 (3), p.323-331</ispartof><rights>The Royal Society of Chemistry and Owner Societies 2018</rights><rights>Copyright Royal Society of Chemistry 2018</rights><rights>Distributed under a Creative Commons Attribution 4.0 International License</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c499t-9b9f34ea4ec58031aef37a2323f6e99c2b89ada7b00262fbbdc1decc25559b33</citedby><cites>FETCH-LOGICAL-c499t-9b9f34ea4ec58031aef37a2323f6e99c2b89ada7b00262fbbdc1decc25559b33</cites><orcidid>0000-0001-9464-1463 ; 0000-0002-0796-289X ; 0000-0002-6969-4667 ; 0000-0002-2359-111X ; 0000-0002-9374-2323 ; 0000-0003-4227-6825 ; 0000-0002-1208-602X ; 0000-0003-1809-3543 ; 0000-0001-7158-7994</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1039/c7pp00439g$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1039/c7pp00439g$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>230,314,776,780,881,27901,27902,41464,42533,51294</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/29383356$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://hal.science/hal-02184642$$DView record in HAL$$Hfree_for_read</backlink></links><search><creatorcontrib>Zvereva, Elena</creatorcontrib><creatorcontrib>Segarra-Martí, Javier</creatorcontrib><creatorcontrib>Marazzi, Marco</creatorcontrib><creatorcontrib>Brazard, Johanna</creatorcontrib><creatorcontrib>Nenov, Artur</creatorcontrib><creatorcontrib>Weingart, Oliver</creatorcontrib><creatorcontrib>Léonard, Jérémie</creatorcontrib><creatorcontrib>Garavelli, Marco</creatorcontrib><creatorcontrib>Rivalta, Ivan</creatorcontrib><creatorcontrib>Dumont, Elise</creatorcontrib><creatorcontrib>Assfeld, Xavier</creatorcontrib><creatorcontrib>Haacke, Stefan</creatorcontrib><creatorcontrib>Monari, Antonio</creatorcontrib><title>The effect of solvent relaxation in the ultrafast time-resolved spectroscopy of solvated benzophenone</title><title>Photochemical & photobiological sciences</title><addtitle>Photochem Photobiol Sci</addtitle><addtitle>Photochem Photobiol Sci</addtitle><description>Benzophenone (BP) despite its relatively simple molecular structure is a paradigmatic sensitizer, featuring both photocatalytic and photobiological effects due to its rather complex photophysical properties. 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Finally we predict for the first time the two-dimensional electronic spectrum (2DES) of BP taking into account the vibrational effects and hence modelling partially symmetric and asymmetric ultrafast broadening.</description><subject>Benzophenone</subject><subject>Biochemistry</subject><subject>Biomaterials</subject><subject>Chemical bonds</subject><subject>Chemical Sciences</subject><subject>Chemistry</subject><subject>Computer simulation</subject><subject>Molecular structure</subject><subject>Physical Chemistry</subject><subject>Plant Sciences</subject><subject>Quantum mechanics</subject><subject>Solvents</subject><subject>Spectroscopy</subject><subject>Spectrum analysis</subject><issn>1474-905X</issn><issn>1474-9092</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNptkUlLBDEQhYMoLqMXf4A0eHGhNVsvOYq4wYCXOXgL6XTFaelJ2iQt6q83OjqCeEqR-upV8h5C-wSfEczEua6GAWPOxOMa2ia84rnAgq6v6uJhC-2E8IQxKXhZbaItKljNWFFuI5jNIQNjQMfMmSy4_gVszDz06lXFztmss1lMzNhHr4wKMYvdAnIPX2ibhSGNehe0G95-FFRMjQbsuxvmYJ2FXbRhVB9g7_ucoNn11ezyNp_e39xdXkxzzYWIuWiEYRwUB13UmBEFhlWKMspMCUJo2tRCtapqMKYlNU3TatKC1rQoCtEwNkHHS9m56uXgu4Xyb9KpTt5eTOXnHaak5iWnLySxR0t28O55hBDlogsa-l5ZcGOQRAiGcV0kXyfo8A_65EZv00ckxYRVNLlaJ-pkSenkRvBgVi8gWH7mJH9zSvDBt-TYLKBdoT_BJOB0CYTUso_gf3f-I_cBKcaddg</recordid><startdate>2018</startdate><enddate>2018</enddate><creator>Zvereva, Elena</creator><creator>Segarra-Martí, Javier</creator><creator>Marazzi, Marco</creator><creator>Brazard, Johanna</creator><creator>Nenov, Artur</creator><creator>Weingart, Oliver</creator><creator>Léonard, Jérémie</creator><creator>Garavelli, Marco</creator><creator>Rivalta, Ivan</creator><creator>Dumont, Elise</creator><creator>Assfeld, Xavier</creator><creator>Haacke, Stefan</creator><creator>Monari, Antonio</creator><general>Springer International Publishing</general><general>Royal Society of Chemistry</general><general>Springer</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7QO</scope><scope>8FD</scope><scope>FR3</scope><scope>P64</scope><scope>7X8</scope><scope>1XC</scope><orcidid>https://orcid.org/0000-0001-9464-1463</orcidid><orcidid>https://orcid.org/0000-0002-0796-289X</orcidid><orcidid>https://orcid.org/0000-0002-6969-4667</orcidid><orcidid>https://orcid.org/0000-0002-2359-111X</orcidid><orcidid>https://orcid.org/0000-0002-9374-2323</orcidid><orcidid>https://orcid.org/0000-0003-4227-6825</orcidid><orcidid>https://orcid.org/0000-0002-1208-602X</orcidid><orcidid>https://orcid.org/0000-0003-1809-3543</orcidid><orcidid>https://orcid.org/0000-0001-7158-7994</orcidid></search><sort><creationdate>2018</creationdate><title>The effect of solvent relaxation in the ultrafast time-resolved spectroscopy of solvated benzophenone</title><author>Zvereva, Elena ; Segarra-Martí, Javier ; Marazzi, Marco ; Brazard, Johanna ; Nenov, Artur ; Weingart, Oliver ; Léonard, Jérémie ; Garavelli, Marco ; Rivalta, Ivan ; Dumont, Elise ; Assfeld, Xavier ; Haacke, Stefan ; Monari, Antonio</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c499t-9b9f34ea4ec58031aef37a2323f6e99c2b89ada7b00262fbbdc1decc25559b33</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Benzophenone</topic><topic>Biochemistry</topic><topic>Biomaterials</topic><topic>Chemical bonds</topic><topic>Chemical Sciences</topic><topic>Chemistry</topic><topic>Computer simulation</topic><topic>Molecular structure</topic><topic>Physical Chemistry</topic><topic>Plant Sciences</topic><topic>Quantum mechanics</topic><topic>Solvents</topic><topic>Spectroscopy</topic><topic>Spectrum analysis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zvereva, Elena</creatorcontrib><creatorcontrib>Segarra-Martí, Javier</creatorcontrib><creatorcontrib>Marazzi, Marco</creatorcontrib><creatorcontrib>Brazard, Johanna</creatorcontrib><creatorcontrib>Nenov, Artur</creatorcontrib><creatorcontrib>Weingart, Oliver</creatorcontrib><creatorcontrib>Léonard, Jérémie</creatorcontrib><creatorcontrib>Garavelli, Marco</creatorcontrib><creatorcontrib>Rivalta, Ivan</creatorcontrib><creatorcontrib>Dumont, Elise</creatorcontrib><creatorcontrib>Assfeld, Xavier</creatorcontrib><creatorcontrib>Haacke, Stefan</creatorcontrib><creatorcontrib>Monari, Antonio</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Biotechnology Research Abstracts</collection><collection>Technology Research Database</collection><collection>Engineering Research Database</collection><collection>Biotechnology and BioEngineering Abstracts</collection><collection>MEDLINE - Academic</collection><collection>Hyper Article en Ligne (HAL)</collection><jtitle>Photochemical & photobiological sciences</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zvereva, Elena</au><au>Segarra-Martí, Javier</au><au>Marazzi, Marco</au><au>Brazard, Johanna</au><au>Nenov, Artur</au><au>Weingart, Oliver</au><au>Léonard, Jérémie</au><au>Garavelli, Marco</au><au>Rivalta, Ivan</au><au>Dumont, Elise</au><au>Assfeld, Xavier</au><au>Haacke, Stefan</au><au>Monari, Antonio</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The effect of solvent relaxation in the ultrafast time-resolved spectroscopy of solvated benzophenone</atitle><jtitle>Photochemical & photobiological sciences</jtitle><stitle>Photochem Photobiol Sci</stitle><addtitle>Photochem Photobiol Sci</addtitle><date>2018</date><risdate>2018</risdate><volume>17</volume><issue>3</issue><spage>323</spage><epage>331</epage><pages>323-331</pages><issn>1474-905X</issn><eissn>1474-9092</eissn><abstract>Benzophenone (BP) despite its relatively simple molecular structure is a paradigmatic sensitizer, featuring both photocatalytic and photobiological effects due to its rather complex photophysical properties. 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| subjects | Benzophenone Biochemistry Biomaterials Chemical bonds Chemical Sciences Chemistry Computer simulation Molecular structure Physical Chemistry Plant Sciences Quantum mechanics Solvents Spectroscopy Spectrum analysis |
| title | The effect of solvent relaxation in the ultrafast time-resolved spectroscopy of solvated benzophenone |
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