Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level
We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the gr...
Gespeichert in:
| Veröffentlicht in: | The Journal of chemical physics 2024-04, Vol.160 (16) |
|---|---|
| Hauptverfasser: | , , , , , , , , |
| Format: | Artikel |
| Sprache: | eng |
| Schlagworte: | |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| container_end_page | |
|---|---|
| container_issue | 16 |
| container_start_page | |
| container_title | The Journal of chemical physics |
| container_volume | 160 |
| creator | Jaiswal, V. K. Montorsi, F. Aleotti, F. Segatta, F. Keefer, Daniel Mukamel, Shaul Nenov, A. Conti, I. Garavelli, M. |
| description | We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state. |
| doi_str_mv | 10.1063/5.0203624 |
| format | Article |
| fullrecord | <record><control><sourceid>proquest_pubme</sourceid><recordid>TN_cdi_proquest_journals_3049019312</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>3049721030</sourcerecordid><originalsourceid>FETCH-LOGICAL-c343t-a08bf96b7f98709aee5356584172483f1f6ee59fe9f7a861b7ac82baba4f88d83</originalsourceid><addsrcrecordid>eNp9kc2KFDEUhYM4OO3owheQgJsZocabSlUqWcrgHwwMiLMuUqkbu4Z0Uiapxn4BH8CN7-eTTNpuZ-FC7uLC4eNwzz2EvGBwyUDwN-0l1MBF3TwiKwZSVZ1Q8JisAGpWKQHilDxN6Q4AWFc3T8gpl6IMUyvy69blqK1Omc7rkINZ42ZKOe6o9iNFhybH4KtxsjZqk6fgaZr3oqaTp57-_vGTnvN0QT_vxgHjV4rfzZRxpGZnXBiWrH3wSCOm4LZF1pnmNdLN4vIU0WJEb5DOGPMSB52nLVKHW3TPyInVLuHz4z4jt-_ffbn6WF3ffPh09fa6MrzhudIgB6vE0FklO1AaseWtaGWzDyq5ZVYUSVlUttNSsKHTRtaDHnRjpRwlPyPnB985hm8LptyX-Aad0x7DknoOjepqBhwK-uof9C4s0Zfr_lDAFGd1oS4OlIkhpRKxn-O00XHXM-j3bfVtf2yrsC-PjsuwwfGB_FtPAV4fgFSeqvff_4_bPf0gn-Q</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>3049019312</pqid></control><display><type>article</type><title>Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level</title><source>AIP Journals Complete</source><creator>Jaiswal, V. K. ; Montorsi, F. ; Aleotti, F. ; Segatta, F. ; Keefer, Daniel ; Mukamel, Shaul ; Nenov, A. ; Conti, I. ; Garavelli, M.</creator><creatorcontrib>Jaiswal, V. K. ; Montorsi, F. ; Aleotti, F. ; Segatta, F. ; Keefer, Daniel ; Mukamel, Shaul ; Nenov, A. ; Conti, I. ; Garavelli, M.</creatorcontrib><description>We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state.</description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/5.0203624</identifier><identifier>PMID: 38686819</identifier><identifier>CODEN: JCPSA6</identifier><language>eng</language><publisher>United States: American Institute of Physics</publisher><subject>Diffraction ; Photochemistry ; Rydberg states ; Spectra</subject><ispartof>The Journal of chemical physics, 2024-04, Vol.160 (16)</ispartof><rights>Author(s)</rights><rights>2024 Author(s). Published under an exclusive license by AIP Publishing.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c343t-a08bf96b7f98709aee5356584172483f1f6ee59fe9f7a861b7ac82baba4f88d83</cites><orcidid>0000-0002-1058-4770 ; 0000-0002-7176-5305 ; 0000-0003-4150-6676 ; 0000-0002-5090-7984 ; 0000-0003-3071-5341 ; 0000-0001-7982-4480 ; 0000-0002-6015-3135 ; 0000-0001-5941-5567 ; 0000-0002-0796-289X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://pubs.aip.org/jcp/article-lookup/doi/10.1063/5.0203624$$EHTML$$P50$$Gscitation$$H</linktohtml><link.rule.ids>314,776,780,790,4497,27903,27904,76130</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/38686819$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Jaiswal, V. K.</creatorcontrib><creatorcontrib>Montorsi, F.</creatorcontrib><creatorcontrib>Aleotti, F.</creatorcontrib><creatorcontrib>Segatta, F.</creatorcontrib><creatorcontrib>Keefer, Daniel</creatorcontrib><creatorcontrib>Mukamel, Shaul</creatorcontrib><creatorcontrib>Nenov, A.</creatorcontrib><creatorcontrib>Conti, I.</creatorcontrib><creatorcontrib>Garavelli, M.</creatorcontrib><title>Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level</title><title>The Journal of chemical physics</title><addtitle>J Chem Phys</addtitle><description>We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state.</description><subject>Diffraction</subject><subject>Photochemistry</subject><subject>Rydberg states</subject><subject>Spectra</subject><issn>0021-9606</issn><issn>1089-7690</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNp9kc2KFDEUhYM4OO3owheQgJsZocabSlUqWcrgHwwMiLMuUqkbu4Z0Uiapxn4BH8CN7-eTTNpuZ-FC7uLC4eNwzz2EvGBwyUDwN-0l1MBF3TwiKwZSVZ1Q8JisAGpWKQHilDxN6Q4AWFc3T8gpl6IMUyvy69blqK1Omc7rkINZ42ZKOe6o9iNFhybH4KtxsjZqk6fgaZr3oqaTp57-_vGTnvN0QT_vxgHjV4rfzZRxpGZnXBiWrH3wSCOm4LZF1pnmNdLN4vIU0WJEb5DOGPMSB52nLVKHW3TPyInVLuHz4z4jt-_ffbn6WF3ffPh09fa6MrzhudIgB6vE0FklO1AaseWtaGWzDyq5ZVYUSVlUttNSsKHTRtaDHnRjpRwlPyPnB985hm8LptyX-Aad0x7DknoOjepqBhwK-uof9C4s0Zfr_lDAFGd1oS4OlIkhpRKxn-O00XHXM-j3bfVtf2yrsC-PjsuwwfGB_FtPAV4fgFSeqvff_4_bPf0gn-Q</recordid><startdate>20240428</startdate><enddate>20240428</enddate><creator>Jaiswal, V. K.</creator><creator>Montorsi, F.</creator><creator>Aleotti, F.</creator><creator>Segatta, F.</creator><creator>Keefer, Daniel</creator><creator>Mukamel, Shaul</creator><creator>Nenov, A.</creator><creator>Conti, I.</creator><creator>Garavelli, M.</creator><general>American Institute of Physics</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>8FD</scope><scope>H8D</scope><scope>L7M</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-1058-4770</orcidid><orcidid>https://orcid.org/0000-0002-7176-5305</orcidid><orcidid>https://orcid.org/0000-0003-4150-6676</orcidid><orcidid>https://orcid.org/0000-0002-5090-7984</orcidid><orcidid>https://orcid.org/0000-0003-3071-5341</orcidid><orcidid>https://orcid.org/0000-0001-7982-4480</orcidid><orcidid>https://orcid.org/0000-0002-6015-3135</orcidid><orcidid>https://orcid.org/0000-0001-5941-5567</orcidid><orcidid>https://orcid.org/0000-0002-0796-289X</orcidid></search><sort><creationdate>20240428</creationdate><title>Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level</title><author>Jaiswal, V. K. ; Montorsi, F. ; Aleotti, F. ; Segatta, F. ; Keefer, Daniel ; Mukamel, Shaul ; Nenov, A. ; Conti, I. ; Garavelli, M.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c343t-a08bf96b7f98709aee5356584172483f1f6ee59fe9f7a861b7ac82baba4f88d83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Diffraction</topic><topic>Photochemistry</topic><topic>Rydberg states</topic><topic>Spectra</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Jaiswal, V. K.</creatorcontrib><creatorcontrib>Montorsi, F.</creatorcontrib><creatorcontrib>Aleotti, F.</creatorcontrib><creatorcontrib>Segatta, F.</creatorcontrib><creatorcontrib>Keefer, Daniel</creatorcontrib><creatorcontrib>Mukamel, Shaul</creatorcontrib><creatorcontrib>Nenov, A.</creatorcontrib><creatorcontrib>Conti, I.</creatorcontrib><creatorcontrib>Garavelli, M.</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Technology Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>MEDLINE - Academic</collection><jtitle>The Journal of chemical physics</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Jaiswal, V. K.</au><au>Montorsi, F.</au><au>Aleotti, F.</au><au>Segatta, F.</au><au>Keefer, Daniel</au><au>Mukamel, Shaul</au><au>Nenov, A.</au><au>Conti, I.</au><au>Garavelli, M.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level</atitle><jtitle>The Journal of chemical physics</jtitle><addtitle>J Chem Phys</addtitle><date>2024-04-28</date><risdate>2024</risdate><volume>160</volume><issue>16</issue><issn>0021-9606</issn><eissn>1089-7690</eissn><coden>JCPSA6</coden><abstract>We study the ultrafast time evolution of cyclobutanone excited to the singlet n → Rydberg state through non-adiabatic surface-hopping simulationsperformed at extended multi-state complete active space second-order perturbation (XMS-CASPT2) level of theory. These dynamics predict relaxation to the ground-state with a timescale of 822 ± 45 fs with minimal involvement of the triplets. The major relaxation path to the ground-state involves a three-state degeneracy region and leads to a variety of fragmented photoproducts. We simulate the resulting time-resolved electron-diffraction spectra, which track the relaxation of the excited state and the formation of various photoproducts in the ground state.</abstract><cop>United States</cop><pub>American Institute of Physics</pub><pmid>38686819</pmid><doi>10.1063/5.0203624</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0002-1058-4770</orcidid><orcidid>https://orcid.org/0000-0002-7176-5305</orcidid><orcidid>https://orcid.org/0000-0003-4150-6676</orcidid><orcidid>https://orcid.org/0000-0002-5090-7984</orcidid><orcidid>https://orcid.org/0000-0003-3071-5341</orcidid><orcidid>https://orcid.org/0000-0001-7982-4480</orcidid><orcidid>https://orcid.org/0000-0002-6015-3135</orcidid><orcidid>https://orcid.org/0000-0001-5941-5567</orcidid><orcidid>https://orcid.org/0000-0002-0796-289X</orcidid><oa>free_for_read</oa></addata></record> |
| fulltext | fulltext |
| identifier | ISSN: 0021-9606 |
| ispartof | The Journal of chemical physics, 2024-04, Vol.160 (16) |
| issn | 0021-9606 1089-7690 |
| language | eng |
| recordid | cdi_proquest_journals_3049019312 |
| source | AIP Journals Complete |
| subjects | Diffraction Photochemistry Rydberg states Spectra |
| title | Ultrafast photochemistry and electron-diffraction spectra in n → (3s) Rydberg excited cyclobutanone resolved at the multireference perturbative level |
| url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-25T02%3A05%3A03IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_pubme&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Ultrafast%20photochemistry%20and%20electron-diffraction%20spectra%20in%20n%20%E2%86%92%20(3s)%20Rydberg%20excited%20cyclobutanone%20resolved%20at%20the%20multireference%20perturbative%20level&rft.jtitle=The%20Journal%20of%20chemical%20physics&rft.au=Jaiswal,%20V.%20K.&rft.date=2024-04-28&rft.volume=160&rft.issue=16&rft.issn=0021-9606&rft.eissn=1089-7690&rft.coden=JCPSA6&rft_id=info:doi/10.1063/5.0203624&rft_dat=%3Cproquest_pubme%3E3049721030%3C/proquest_pubme%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=3049019312&rft_id=info:pmid/38686819&rfr_iscdi=true |