Ultrafast energy transfer between π-stacked aromatic rings upon inner-valence ionization
Non-covalently bound aromatic systems are ubiquitous and govern the physicochemical properties of various organic materials. They are important to many phenomena of biological and technological relevance, such as protein folding, base-pair stacking in nucleic acids, molecular recognition and self-as...
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| Veröffentlicht in: | Nature chemistry 2022-02, Vol.14 (2), p.232-238 |
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| creator | Ren, Xueguang Zhou, Jiaqi Wang, Enliang Yang, Tao Xu, Zhongfeng Sisourat, Nicolas Pfeifer, Thomas Dorn, Alexander |
| description | Non-covalently bound aromatic systems are ubiquitous and govern the physicochemical properties of various organic materials. They are important to many phenomena of biological and technological relevance, such as protein folding, base-pair stacking in nucleic acids, molecular recognition and self-assembly, DNA–drug interactions, crystal engineering and organic electronics. Nevertheless, their molecular dynamics and chemical reactivity, particularly in electronic excited states, are not fully understood. Here, we observe intermolecular Coulombic decay in benzene dimers, (C
6
H
6
)
2
—the simplest prototypes of noncovalent
π
–
π
interactions between aromatic systems. Intermolecular Coulombic decay is initiated by a carbon 2
s
vacancy state produced by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules. As a result, the dimer relaxes with the emission of a further low-energy electron ( |
| doi_str_mv | 10.1038/s41557-021-00838-4 |
| format | Article |
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6
H
6
)
2
—the simplest prototypes of noncovalent
π
–
π
interactions between aromatic systems. Intermolecular Coulombic decay is initiated by a carbon 2
s
vacancy state produced by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules. As a result, the dimer relaxes with the emission of a further low-energy electron (<10 eV) and a pair of C
6
H
6
+
cations undergoing Coulomb explosion. Coincident fragment-ion and electron momentum spectroscopy, accompanied by ab initio calculations, enables us to elucidate the dynamical details of this ultrafast relaxation process.
Aromatic systems that interact non-covalently are important in many settings, such as base-pair stacking and DNA–drug interactions; however, their excited-state molecular dynamics are not fully understood. Now, intermolecular Coulombic decay in benzene dimers has been observed. The process is initiated by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules.</description><identifier>ISSN: 1755-4330</identifier><identifier>EISSN: 1755-4349</identifier><identifier>DOI: 10.1038/s41557-021-00838-4</identifier><identifier>PMID: 34931045</identifier><language>eng</language><publisher>London: Nature Publishing Group UK</publisher><subject>639/638/440/94 ; 639/638/440/948 ; 639/638/440/949 ; 639/638/440/950 ; Analytical Chemistry ; Aromatic compounds ; Benzene ; Biochemistry ; Cations ; Chemical reactions ; Chemistry ; Chemistry and Materials Science ; Chemistry/Food Science ; Decay ; Deoxyribonucleic acid ; Dimers ; DNA ; Drug interactions ; Electron impact ; Electrons ; Energy transfer ; Excitation ; Hydrocarbons ; Inorganic Chemistry ; Ionization ; Molecular dynamics ; Nucleic acids ; Organic Chemistry ; Organic materials ; Physical Chemistry ; Physicochemical properties ; Protein folding ; Self-assembly ; Spectroscopy ; Stacking</subject><ispartof>Nature chemistry, 2022-02, Vol.14 (2), p.232-238</ispartof><rights>The Author(s), under exclusive licence to Springer Nature Limited 2021</rights><rights>2021. The Author(s), under exclusive licence to Springer Nature Limited.</rights><rights>The Author(s), under exclusive licence to Springer Nature Limited 2021.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c342t-d44908e48673f9dec11568d8e242b6db825415fd9c4ccadf4d9bc6b2c64c915b3</citedby><cites>FETCH-LOGICAL-c342t-d44908e48673f9dec11568d8e242b6db825415fd9c4ccadf4d9bc6b2c64c915b3</cites><orcidid>0000-0002-8024-224X ; 0000-0001-6132-092X ; 0000-0002-5312-3747 ; 0000-0002-5703-6501</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.1038/s41557-021-00838-4$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.1038/s41557-021-00838-4$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,776,780,27901,27902,41464,42533,51294</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/34931045$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Ren, Xueguang</creatorcontrib><creatorcontrib>Zhou, Jiaqi</creatorcontrib><creatorcontrib>Wang, Enliang</creatorcontrib><creatorcontrib>Yang, Tao</creatorcontrib><creatorcontrib>Xu, Zhongfeng</creatorcontrib><creatorcontrib>Sisourat, Nicolas</creatorcontrib><creatorcontrib>Pfeifer, Thomas</creatorcontrib><creatorcontrib>Dorn, Alexander</creatorcontrib><title>Ultrafast energy transfer between π-stacked aromatic rings upon inner-valence ionization</title><title>Nature chemistry</title><addtitle>Nat. Chem</addtitle><addtitle>Nat Chem</addtitle><description>Non-covalently bound aromatic systems are ubiquitous and govern the physicochemical properties of various organic materials. They are important to many phenomena of biological and technological relevance, such as protein folding, base-pair stacking in nucleic acids, molecular recognition and self-assembly, DNA–drug interactions, crystal engineering and organic electronics. Nevertheless, their molecular dynamics and chemical reactivity, particularly in electronic excited states, are not fully understood. Here, we observe intermolecular Coulombic decay in benzene dimers, (C
6
H
6
)
2
—the simplest prototypes of noncovalent
π
–
π
interactions between aromatic systems. Intermolecular Coulombic decay is initiated by a carbon 2
s
vacancy state produced by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules. As a result, the dimer relaxes with the emission of a further low-energy electron (<10 eV) and a pair of C
6
H
6
+
cations undergoing Coulomb explosion. Coincident fragment-ion and electron momentum spectroscopy, accompanied by ab initio calculations, enables us to elucidate the dynamical details of this ultrafast relaxation process.
Aromatic systems that interact non-covalently are important in many settings, such as base-pair stacking and DNA–drug interactions; however, their excited-state molecular dynamics are not fully understood. Now, intermolecular Coulombic decay in benzene dimers has been observed. The process is initiated by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules.</description><subject>639/638/440/94</subject><subject>639/638/440/948</subject><subject>639/638/440/949</subject><subject>639/638/440/950</subject><subject>Analytical Chemistry</subject><subject>Aromatic compounds</subject><subject>Benzene</subject><subject>Biochemistry</subject><subject>Cations</subject><subject>Chemical reactions</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Chemistry/Food Science</subject><subject>Decay</subject><subject>Deoxyribonucleic acid</subject><subject>Dimers</subject><subject>DNA</subject><subject>Drug interactions</subject><subject>Electron impact</subject><subject>Electrons</subject><subject>Energy transfer</subject><subject>Excitation</subject><subject>Hydrocarbons</subject><subject>Inorganic Chemistry</subject><subject>Ionization</subject><subject>Molecular dynamics</subject><subject>Nucleic acids</subject><subject>Organic Chemistry</subject><subject>Organic materials</subject><subject>Physical Chemistry</subject><subject>Physicochemical properties</subject><subject>Protein folding</subject><subject>Self-assembly</subject><subject>Spectroscopy</subject><subject>Stacking</subject><issn>1755-4330</issn><issn>1755-4349</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid>BENPR</sourceid><recordid>eNp9kM1OAyEURonR2Fp9AReGxDUKA0yZpWn8S5q4sQtXhIE7zdSWqTCjqSvf0FeSOlV3roBwvu_mHoROGb1glKvLKJiUY0IzRihVXBGxh4ZsLCURXBT7v3dOB-goxgWlueQsP0SD9M0ZFXKInmbLNpjKxBaDhzDf4PT0sYKAS2jfADz-_CCxNfYZHDahWZm2tjjUfh5xt248rn3KkVezBG8B142v3xPS-GN0UJllhJPdOUKzm-vHyR2ZPtzeT66mxHKRtcQJUVAFQuVjXhUOLGMyV05BJrIyd6XKZFqzcoUV1hpXCVeUNi8zmwtbMFnyETrve9eheekgtnrRdMGnkTrLt2GuCpGorKdsaGIMUOl1qFcmbDSjemtT9zZ1sqm_bept6GxX3ZUrcL-RH30J4D0Q11sjEP5m_1P7BaYngao</recordid><startdate>20220201</startdate><enddate>20220201</enddate><creator>Ren, Xueguang</creator><creator>Zhou, Jiaqi</creator><creator>Wang, Enliang</creator><creator>Yang, Tao</creator><creator>Xu, Zhongfeng</creator><creator>Sisourat, Nicolas</creator><creator>Pfeifer, Thomas</creator><creator>Dorn, Alexander</creator><general>Nature Publishing Group UK</general><general>Nature Publishing Group</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>3V.</scope><scope>7QR</scope><scope>7X7</scope><scope>7XB</scope><scope>88E</scope><scope>8AO</scope><scope>8FD</scope><scope>8FE</scope><scope>8FG</scope><scope>8FH</scope><scope>8FI</scope><scope>8FJ</scope><scope>8FK</scope><scope>ABJCF</scope><scope>ABUWG</scope><scope>AEUYN</scope><scope>AFKRA</scope><scope>AZQEC</scope><scope>BBNVY</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>BHPHI</scope><scope>CCPQU</scope><scope>D1I</scope><scope>DWQXO</scope><scope>FR3</scope><scope>FYUFA</scope><scope>GHDGH</scope><scope>GNUQQ</scope><scope>HCIFZ</scope><scope>K9.</scope><scope>KB.</scope><scope>LK8</scope><scope>M0S</scope><scope>M1P</scope><scope>M7P</scope><scope>P64</scope><scope>PDBOC</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><orcidid>https://orcid.org/0000-0002-8024-224X</orcidid><orcidid>https://orcid.org/0000-0001-6132-092X</orcidid><orcidid>https://orcid.org/0000-0002-5312-3747</orcidid><orcidid>https://orcid.org/0000-0002-5703-6501</orcidid></search><sort><creationdate>20220201</creationdate><title>Ultrafast energy transfer between π-stacked aromatic rings upon inner-valence ionization</title><author>Ren, Xueguang ; 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Chem</stitle><addtitle>Nat Chem</addtitle><date>2022-02-01</date><risdate>2022</risdate><volume>14</volume><issue>2</issue><spage>232</spage><epage>238</epage><pages>232-238</pages><issn>1755-4330</issn><eissn>1755-4349</eissn><abstract>Non-covalently bound aromatic systems are ubiquitous and govern the physicochemical properties of various organic materials. They are important to many phenomena of biological and technological relevance, such as protein folding, base-pair stacking in nucleic acids, molecular recognition and self-assembly, DNA–drug interactions, crystal engineering and organic electronics. Nevertheless, their molecular dynamics and chemical reactivity, particularly in electronic excited states, are not fully understood. Here, we observe intermolecular Coulombic decay in benzene dimers, (C
6
H
6
)
2
—the simplest prototypes of noncovalent
π
–
π
interactions between aromatic systems. Intermolecular Coulombic decay is initiated by a carbon 2
s
vacancy state produced by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules. As a result, the dimer relaxes with the emission of a further low-energy electron (<10 eV) and a pair of C
6
H
6
+
cations undergoing Coulomb explosion. Coincident fragment-ion and electron momentum spectroscopy, accompanied by ab initio calculations, enables us to elucidate the dynamical details of this ultrafast relaxation process.
Aromatic systems that interact non-covalently are important in many settings, such as base-pair stacking and DNA–drug interactions; however, their excited-state molecular dynamics are not fully understood. Now, intermolecular Coulombic decay in benzene dimers has been observed. The process is initiated by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules.</abstract><cop>London</cop><pub>Nature Publishing Group UK</pub><pmid>34931045</pmid><doi>10.1038/s41557-021-00838-4</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0002-8024-224X</orcidid><orcidid>https://orcid.org/0000-0001-6132-092X</orcidid><orcidid>https://orcid.org/0000-0002-5312-3747</orcidid><orcidid>https://orcid.org/0000-0002-5703-6501</orcidid></addata></record> |
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| subjects | 639/638/440/94 639/638/440/948 639/638/440/949 639/638/440/950 Analytical Chemistry Aromatic compounds Benzene Biochemistry Cations Chemical reactions Chemistry Chemistry and Materials Science Chemistry/Food Science Decay Deoxyribonucleic acid Dimers DNA Drug interactions Electron impact Electrons Energy transfer Excitation Hydrocarbons Inorganic Chemistry Ionization Molecular dynamics Nucleic acids Organic Chemistry Organic materials Physical Chemistry Physicochemical properties Protein folding Self-assembly Spectroscopy Stacking |
| title | Ultrafast energy transfer between π-stacked aromatic rings upon inner-valence ionization |
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