Ultrafast X-ray spectroscopy of conical intersections
NRC publication: Yes
Gespeichert in:
| Veröffentlicht in: | Physical review letters Jg. 120; H. 24; S. 243001 |
|---|---|
| Hauptverfasser: | , , , |
| Format: | Journal Article |
| Sprache: | Englisch |
| Veröffentlicht: |
United States
American Physical Society
12.06.2018
|
| Schlagworte: | |
| ISSN: | 0031-9007, 1079-7114, 1079-7114 |
| Online-Zugang: | Volltext |
| Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
| Abstract | NRC publication: Yes Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S2(ππ∗) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections. |
|---|---|
| AbstractList | Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S_{2}(ππ^{*}) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections.Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S_{2}(ππ^{*}) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections. Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S2(ππ*) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections. Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by general electronic degeneracies termed conical intersections, which play a key role, analogous to that of a transition state, in the electronic-nuclear dynamics of excited molecules. Using high-level ab initio quantum dynamics simulations, we studied time-resolved x-ray absorption (TRXAS) and photoelectron spectroscopy (TRXPS) of the prototypical unsaturated organic chromophore, ethylene, following excitation to its S_{2}(ππ^{*}) state. The TRXAS, in particular, is highly sensitive to all aspects of the ensuing dynamics. These x-ray spectroscopies provide a clear signature of the wave packet dynamics near conical intersections, related to charge localization effects driven by the nuclear dynamics. Given the ubiquity of charge localization in excited state dynamics, we believe that ultrafast x-ray spectroscopies offer a unique and powerful route to the direct observation of dynamics around conical intersections. NRC publication: Yes |
| ArticleNumber | 243001 |
| Author | Chergui, Majed Stolow, Albert Schuurman, Michael S Neville, Simon P |
| Author_xml | – sequence: 1 fullname: Neville, Simon P – sequence: 2 fullname: Chergui, Majed – sequence: 3 fullname: Stolow, Albert – sequence: 4 fullname: Schuurman, Michael S |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/29956989$$D View this record in MEDLINE/PubMed |
| BookMark | eNqFkEFrHCEUx6WkNJukXyEM9NLLbN7TGXWglxLSJLDQUhrITRzHoYZZnaob2G8ft5OGkEsvPp_-_k_5nZAjH7wl5BxhjQjs4sfvffppHzc25zVSWNOGAeA7skIQXS0QmyOyAmBYdwDimJyk9ACFoFx-IMe061reyW5F2rspRz3qlKv7Oup9lWZrcgzJhHlfhbEywTujp8r5bGMqdy74dEbej3pK9uNzPSV3365-Xd7Um-_Xt5dfN7VpUeZajghc4GiktHrA3kLLqKCDlVxo6Pu252UPPQ6UswF5Q8e2G6QVtG0Ysy07JZ-XuXMMf3Y2ZbV1ydhp0t6GXVIUOJVMCA4F_fQGfQi76MvvFEUqGkobpIU6f6Z2_dYOao5uq-Ne_RNSAL4ApjhI0Y4vCII6mFevzKtiXi3mS_DLm6BxWR9sFb9u-n_8Zon7aIz2etAvDwftyqyUnXKHogqhzN9FL-d-1qWjZU6DrGNPVDWnEg |
| CitedBy_id | crossref_primary_10_1073_pnas_2015988117 crossref_primary_10_1063_4_0000093 crossref_primary_10_1063_4_0000070 crossref_primary_10_1002_ange_202007192 crossref_primary_10_1038_s41467_020_17745_w crossref_primary_10_1063_1_5097653 crossref_primary_10_1063_1_5085011 crossref_primary_10_1038_s41566_024_01436_9 crossref_primary_10_1063_4_0000076 crossref_primary_10_1126_science_abf1656 crossref_primary_10_1063_4_0000215 crossref_primary_10_1039_D0SC00840K crossref_primary_10_1126_science_aax0076 crossref_primary_10_1002_anie_202000940 crossref_primary_10_1021_jacs_4c06035 crossref_primary_10_3367_UFNr_2021_10_039078 crossref_primary_10_1002_anie_202007192 crossref_primary_10_1063_1_5113798 crossref_primary_10_1038_s42005_025_02175_1 crossref_primary_10_1038_s41467_021_27908_y crossref_primary_10_1021_jacs_3c01800 crossref_primary_10_1021_jacs_4c03033 crossref_primary_10_1146_annurev_physchem_082820_020236 crossref_primary_10_3367_UFNe_2021_10_039078 crossref_primary_10_1038_s41566_019_0549_5 crossref_primary_10_1063_4_0000146 crossref_primary_10_1021_acs_jctc_5c00457 crossref_primary_10_1038_s41467_023_40628_9 crossref_primary_10_1002_wcms_70012 crossref_primary_10_1002_nadc_20244143084 crossref_primary_10_1039_D0SC06328B crossref_primary_10_1002_ange_202000940 crossref_primary_10_1016_j_cpc_2023_109016 crossref_primary_10_1002_lpor_202200588 crossref_primary_10_1038_s41467_020_16480_6 crossref_primary_10_1073_pnas_2321343121 |
| Cites_doi | 10.1063/1.4921841 10.1021/ja1114002 10.1063/1.4938561 10.1016/0301-0104(77)85131-8 10.1002/0471264318 10.1021/jp0723665 10.1021/acs.jpca.5b06094 10.1021/cr020683w 10.1103/PhysRevA.86.053406 10.1063/1.3697760 10.1088/0953-4075/48/21/214001 10.1103/PhysRevLett.115.193003 10.1063/1.4933007 10.1126/science.aaj2198 10.1063/1.3604007 10.1038/nature13252 10.1021/ja00496a005 10.1021/jp312559h 10.1021/jp9063565 10.1039/C6FD00117C 10.1103/PhysRevA.26.2395 10.1021/jz200168m 10.1063/1.4939220 10.1126/science.1165733 10.1021/acs.chemrev.7b00081 10.1142/5406 10.1021/jp2097185 10.1063/1.4964369 10.1063/1.4964821 |
| ContentType | Journal Article |
| Copyright | Copyright American Physical Society Jun 15, 2018 |
| Copyright_xml | – notice: Copyright American Physical Society Jun 15, 2018 |
| DBID | -LJ GXV AAYXX CITATION NPM 7U5 8FD H8D L7M 7X8 |
| DOI | 10.1103/PhysRevLett.120.243001 |
| DatabaseName | National Research Council Canada Archive CISTI Source CrossRef PubMed Solid State and Superconductivity Abstracts Technology Research Database Aerospace Database Advanced Technologies Database with Aerospace MEDLINE - Academic |
| DatabaseTitle | CrossRef PubMed Aerospace Database Solid State and Superconductivity Abstracts Technology Research Database Advanced Technologies Database with Aerospace MEDLINE - Academic |
| DatabaseTitleList | MEDLINE - Academic Aerospace Database PubMed |
| Database_xml | – sequence: 1 dbid: NPM name: PubMed url: http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed sourceTypes: Index Database – sequence: 2 dbid: 7X8 name: MEDLINE - Academic url: https://search.proquest.com/medline sourceTypes: Aggregation Database |
| DeliveryMethod | fulltext_linktorsrc |
| Discipline | Sciences Physics |
| EISSN | 1079-7114 |
| ExternalDocumentID | 29956989 10_1103_PhysRevLett_120_243001 oai_cisti_icist_nrc_cnrc_ca_cistinparc_23004139 |
| Genre | Journal Article |
| GroupedDBID | --- -DZ -LJ -~X 123 2-P 29O 3MX 5VS 85S ABSSX ABUFD ACBEA ACGFO ACNCT AECSF AENEX AEQTI AFFNX AFGMR AGDNE AJQPL ALMA_UNASSIGNED_HOLDINGS APKKM AUAIK CS3 D0L DU5 EBS EJD ER. F5P GXV MVM N9A NPBMV OK1 P2P ROL S7W SJN TN5 UBE WH7 XSW YNT ZPR ~02 186 3O- 41~ 6TJ 8NH 8WZ 9M8 A6W AAYJJ AAYXX ACKIV ADXHL AETEA CITATION H~9 NEJ NHB OHT P0- RNS T9H UBC VOH XOL YYP ZCG ZY4 NPM UCJ VQA 7U5 8FD H8D L7M 7X8 |
| ID | FETCH-LOGICAL-c518t-8f10671fc88ead1be053272de867a0bb5b6de80b1d263d1642f59d8e725433e53 |
| IEDL.DBID | 3MX |
| ISICitedReferencesCount | 92 |
| ISICitedReferencesURI | http://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=Summon&SrcAuth=ProQuest&DestLinkType=CitingArticles&DestApp=WOS_CPL&KeyUT=000434937000007&url=https%3A%2F%2Fcvtisr.summon.serialssolutions.com%2F%23%21%2Fsearch%3Fho%3Df%26include.ft.matches%3Dt%26l%3Dnull%26q%3D |
| ISSN | 0031-9007 1079-7114 |
| IngestDate | Thu Jul 10 23:28:04 EDT 2025 Mon Nov 03 04:26:41 EST 2025 Thu Jan 02 23:12:10 EST 2025 Sat Nov 29 01:46:56 EST 2025 Tue Nov 18 22:00:44 EST 2025 Fri Nov 21 15:59:20 EST 2025 |
| IsDoiOpenAccess | false |
| IsOpenAccess | true |
| IsPeerReviewed | true |
| IsScholarly | true |
| Issue | 24 |
| Language | English |
| LinkModel | DirectLink |
| MergedId | FETCHMERGED-LOGICAL-c518t-8f10671fc88ead1be053272de867a0bb5b6de80b1d263d1642f59d8e725433e53 |
| Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23 |
| OpenAccessLink | http://infoscience.epfl.ch/record/260249 |
| PMID | 29956989 |
| PQID | 2127422412 |
| PQPubID | 2048222 |
| ParticipantIDs | proquest_miscellaneous_2062837760 proquest_journals_2127422412 pubmed_primary_29956989 crossref_primary_10_1103_PhysRevLett_120_243001 crossref_citationtrail_10_1103_PhysRevLett_120_243001 nrccanada_primary_oai_cisti_icist_nrc_cnrc_ca_cistinparc_23004139 |
| PublicationCentury | 2000 |
| PublicationDate | 2018-06-12 |
| PublicationDateYYYYMMDD | 2018-06-12 |
| PublicationDate_xml | – month: 06 year: 2018 text: 2018-06-12 day: 12 |
| PublicationDecade | 2010 |
| PublicationPlace | United States |
| PublicationPlace_xml | – name: United States – name: College Park |
| PublicationTitle | Physical review letters |
| PublicationTitleAlternate | Phys Rev Lett |
| PublicationYear | 2018 |
| Publisher | American Physical Society |
| Publisher_xml | – name: American Physical Society |
| References | PhysRevLett.120.243001Cc25R1 PhysRevLett.120.243001Cc27R1 PhysRevLett.120.243001Cc26R1 PhysRevLett.120.243001Cc21R1 PhysRevLett.120.243001Cc20R1 PhysRevLett.120.243001Cc9R1 PhysRevLett.120.243001Cc8R1 PhysRevLett.120.243001Cc29R1 PhysRevLett.120.243001Cc6R1 PhysRevLett.120.243001Cc28R1 J. Schirmer (PhysRevLett.120.243001Cc34R1) 1996 PhysRevLett.120.243001Cc5R1 PhysRevLett.120.243001Cc4R1 PhysRevLett.120.243001Cc3R1 PhysRevLett.120.243001Cc2R1 PhysRevLett.120.243001Cc30R1 PhysRevLett.120.243001Cc14R1 PhysRevLett.120.243001Cc13R1 PhysRevLett.120.243001Cc16R1 PhysRevLett.120.243001Cc35R1 PhysRevLett.120.243001Cc15R1 PhysRevLett.120.243001Cc10R1 PhysRevLett.120.243001Cc32R1 PhysRevLett.120.243001Cc33R1 PhysRevLett.120.243001Cc31R1 PhysRevLett.120.243001Cc12R1 PhysRevLett.120.243001Cc11R1 W. Domcke (PhysRevLett.120.243001Cc1R1) 2004 PhysRevLett.120.243001Cc18R1 PhysRevLett.120.243001Cc17R1 B. O. Roos (PhysRevLett.120.243001Cc22R1) 1995 |
| References_xml | – ident: PhysRevLett.120.243001Cc32R1 doi: 10.1063/1.4921841 – ident: PhysRevLett.120.243001Cc15R1 doi: 10.1021/ja1114002 – ident: PhysRevLett.120.243001Cc16R1 doi: 10.1063/1.4938561 – ident: PhysRevLett.120.243001Cc20R1 doi: 10.1016/0301-0104(77)85131-8 – ident: PhysRevLett.120.243001Cc27R1 doi: 10.1002/0471264318 – ident: PhysRevLett.120.243001Cc18R1 doi: 10.1021/jp0723665 – ident: PhysRevLett.120.243001Cc30R1 doi: 10.1021/acs.jpca.5b06094 – ident: PhysRevLett.120.243001Cc14R1 doi: 10.1021/cr020683w – ident: PhysRevLett.120.243001Cc21R1 doi: 10.1103/PhysRevA.86.053406 – ident: PhysRevLett.120.243001Cc31R1 doi: 10.1063/1.3697760 – volume-title: Quantum Mechanical Electronic Structure Calculations with Chemical Accuracy year: 1995 ident: PhysRevLett.120.243001Cc22R1 – ident: PhysRevLett.120.243001Cc8R1 doi: 10.1088/0953-4075/48/21/214001 – ident: PhysRevLett.120.243001Cc11R1 doi: 10.1103/PhysRevLett.115.193003 – ident: PhysRevLett.120.243001Cc12R1 doi: 10.1063/1.4933007 – ident: PhysRevLett.120.243001Cc6R1 doi: 10.1126/science.aaj2198 – ident: PhysRevLett.120.243001Cc25R1 doi: 10.1063/1.3604007 – ident: PhysRevLett.120.243001Cc4R1 doi: 10.1038/nature13252 – ident: PhysRevLett.120.243001Cc35R1 doi: 10.1021/ja00496a005 – ident: PhysRevLett.120.243001Cc3R1 doi: 10.1021/jp312559h – ident: PhysRevLett.120.243001Cc26R1 doi: 10.1021/jp9063565 – ident: PhysRevLett.120.243001Cc9R1 doi: 10.1039/C6FD00117C – ident: PhysRevLett.120.243001Cc33R1 doi: 10.1103/PhysRevA.26.2395 – ident: PhysRevLett.120.243001Cc5R1 doi: 10.1021/jz200168m – ident: PhysRevLett.120.243001Cc29R1 doi: 10.1063/1.4939220 – ident: PhysRevLett.120.243001Cc2R1 doi: 10.1126/science.1165733 – ident: PhysRevLett.120.243001Cc13R1 doi: 10.1021/acs.chemrev.7b00081 – volume-title: Conical Intersections: Electronic Structure, Dynamics and Spectroscopy year: 2004 ident: PhysRevLett.120.243001Cc1R1 doi: 10.1142/5406 – ident: PhysRevLett.120.243001Cc28R1 doi: 10.1021/jp2097185 – ident: PhysRevLett.120.243001Cc10R1 doi: 10.1063/1.4964369 – ident: PhysRevLett.120.243001Cc17R1 doi: 10.1063/1.4964821 – volume-title: VUV and Soft X-Ray Photoionization year: 1996 ident: PhysRevLett.120.243001Cc34R1 |
| SSID | ssj0001268 |
| Score | 2.5754745 |
| Snippet | NRC publication: Yes Ongoing developments in ultrafast x-ray sources offer powerful new means of probing the complex nonadiabatically coupled structural and electronic dynamics of... |
| SourceID | proquest pubmed crossref nrccanada |
| SourceType | Aggregation Database Index Database Enrichment Source Publisher |
| StartPage | 243001 |
| SubjectTerms | Chromophores Dynamic structural analysis Dynamics Intersections Localization Spectrum analysis X ray absorption X ray sources X ray spectra X-ray spectroscopy |
| Title | Ultrafast X-ray spectroscopy of conical intersections |
| URI | https://nrc-publications.canada.ca/eng/view/object/?id=265c3b7c-5d67-4daa-b8bd-bfd3cd2019ab https://www.ncbi.nlm.nih.gov/pubmed/29956989 https://www.proquest.com/docview/2127422412 https://www.proquest.com/docview/2062837760 |
| Volume | 120 |
| WOSCitedRecordID | wos000434937000007&url=https%3A%2F%2Fcvtisr.summon.serialssolutions.com%2F%23%21%2Fsearch%3Fho%3Df%26include.ft.matches%3Dt%26l%3Dnull%26q%3D |
| hasFullText | 1 |
| inHoldings | 1 |
| isFullTextHit | |
| isPrint | |
| journalDatabaseRights | – providerCode: PRVABR databaseName: American Physical Society Journals customDbUrl: eissn: 1079-7114 dateEnd: 99991231 omitProxy: false ssIdentifier: ssj0001268 issn: 1079-7114 databaseCode: 3MX dateStart: 20020101 isFulltext: true titleUrlDefault: https://journals.aps.org/ providerName: American Physical Society – providerCode: PRVIAO databaseName: SCOAP3 Journals (Open Access) customDbUrl: eissn: 1079-7114 dateEnd: 99991231 omitProxy: false ssIdentifier: ssj0001268 issn: 1079-7114 databaseCode: ER. dateStart: 20180101 isFulltext: true titleUrlDefault: https://scoap3.org/ providerName: SCOAP3 (Sponsoring Consortium for Open Access Publishing in Particle Physics) |
| link | http://cvtisr.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwlV1LS-0wEB5EFO_Gx9Wr9UUvuK2mSZvHUkRxoSKi0F1I0xQEaQ-nVfDfm0lrUVDETVvapKTzyqSZ-QbgSJmKcVOmCbVemzJra69SCPrp_ORQscyQMnD6StzcyKJQtwtAvt7BTwk7wUjIO_eC2S3HKSXHNGNkSNiSGQo2uy4m05tSPphehnEHRIwpwd-_5tNstNLMbQi1Mt-7m2HauVj7_YDXYXV0MePTQSY2YME1f2E5hHrabhPyh6d-bmrT9XGR3JnXGEvQ9whq2c5e47aOz9qQKxmHn4VdCNVqui14uDi_P7tMxuIJic1T2SeyRnC4tLZSemFJy1ACQtDKSS48A8q85P6alGlFOav8oonWuaqkE5gdz1zO_sFi0zZuB-IqM9LwmnNpy8woZYTkeVWXnrGGWMUjyN-JqO2ILI4FLp50WGEQpj-QRHuS6IEkEZxM_WYDtsaPPU4nHk1dECDbokHUj3jSvoW24WCG-83M2wxNA7YYUxHsv_NWj_raacS5z9CboRH8nx57TcPtE9O49tm3wXRTJgQnEWwPMjGNgWKCsJJq99eftAd_vA8mk1AOaR8W-_mzO4Al-9I_dvPDIN7-KAr5BnZz-g0 |
| linkProvider | American Physical Society |
| openUrl | ctx_ver=Z39.88-2004&ctx_enc=info%3Aofi%2Fenc%3AUTF-8&rfr_id=info%3Asid%2Fsummon.serialssolutions.com&rft_val_fmt=info%3Aofi%2Ffmt%3Akev%3Amtx%3Ajournal&rft.genre=article&rft.atitle=Ultrafast+X-Ray+Spectroscopy+of+Conical+Intersections&rft.jtitle=Physical+review+letters&rft.au=Neville%2C+Simon+P&rft.au=Chergui%2C+Majed&rft.au=Stolow%2C+Albert&rft.au=Schuurman%2C+Michael+S&rft.date=2018-06-12&rft.eissn=1079-7114&rft.volume=120&rft.issue=24&rft.spage=243001&rft_id=info:doi/10.1103%2FPhysRevLett.120.243001&rft_id=info%3Apmid%2F29956989&rft.externalDocID=29956989 |
| thumbnail_l | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/lc.gif&issn=0031-9007&client=summon |
| thumbnail_m | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/mc.gif&issn=0031-9007&client=summon |
| thumbnail_s | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/sc.gif&issn=0031-9007&client=summon |