Biradicalic excited states of zwitterionic phenol-ammonia clusters
Phenol-ammonia clusters with more than five ammonia molecules are proton transferred species in the ground state. In the present work, the excited states of these zwitterionic clusters have been studied experimentally with two-color pump probe methods on the nanosecond time scale and by ab initio el...
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| Acceso en línea: | http://hdl.handle.net/20.500.12110/paper_00219606_v130_n2_p_Carrera |
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todo:paper_00219606_v130_n2_p_Carrera2023-10-03T14:24:16Z Biradicalic excited states of zwitterionic phenol-ammonia clusters Carrera, A. Nielsen, I.B. Çaŗabal, P. Dedonder, C. Broquier, M. Jouvet, C. Domcke, W. Sobolewski, A.L. Excited states Free radical reactions Ground state Hydrogen Ionic strength Phenols Ab initio Ab initio calculations Ammonia clusters Ammonia molecules Charge separation (CS) Electron transfer process (ETP) Pump probes Small clusters Structure calculations Time scaling Ammonia Phenol-ammonia clusters with more than five ammonia molecules are proton transferred species in the ground state. In the present work, the excited states of these zwitterionic clusters have been studied experimentally with two-color pump probe methods on the nanosecond time scale and by ab initio electronic-structure calculations. The experiments reveal the existence of a long-lived excited electronic state with a lifetime in the 50-100 ns range, much longer than the excited state lifetime of bare phenol and small clusters of phenol with ammonia. The ab initio calculations indicate that this long-lived excited state corresponds to a biradicalic system, consisting of a phenoxy radical that is hydrogen bonded to a hydrogenated ammonia cluster. The biradical is formed from the locally excited state of the phenolate anion via an electron transfer process, which neutralizes the charge separation of the ground state zwitterion. © 2009 American Institute of Physics. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_00219606_v130_n2_p_Carrera |
| institution |
Universidad de Buenos Aires |
| institution_str |
I-28 |
| repository_str |
R-134 |
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Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) |
| topic |
Excited states Free radical reactions Ground state Hydrogen Ionic strength Phenols Ab initio Ab initio calculations Ammonia clusters Ammonia molecules Charge separation (CS) Electron transfer process (ETP) Pump probes Small clusters Structure calculations Time scaling Ammonia |
| spellingShingle |
Excited states Free radical reactions Ground state Hydrogen Ionic strength Phenols Ab initio Ab initio calculations Ammonia clusters Ammonia molecules Charge separation (CS) Electron transfer process (ETP) Pump probes Small clusters Structure calculations Time scaling Ammonia Carrera, A. Nielsen, I.B. Çaŗabal, P. Dedonder, C. Broquier, M. Jouvet, C. Domcke, W. Sobolewski, A.L. Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| topic_facet |
Excited states Free radical reactions Ground state Hydrogen Ionic strength Phenols Ab initio Ab initio calculations Ammonia clusters Ammonia molecules Charge separation (CS) Electron transfer process (ETP) Pump probes Small clusters Structure calculations Time scaling Ammonia |
| description |
Phenol-ammonia clusters with more than five ammonia molecules are proton transferred species in the ground state. In the present work, the excited states of these zwitterionic clusters have been studied experimentally with two-color pump probe methods on the nanosecond time scale and by ab initio electronic-structure calculations. The experiments reveal the existence of a long-lived excited electronic state with a lifetime in the 50-100 ns range, much longer than the excited state lifetime of bare phenol and small clusters of phenol with ammonia. The ab initio calculations indicate that this long-lived excited state corresponds to a biradicalic system, consisting of a phenoxy radical that is hydrogen bonded to a hydrogenated ammonia cluster. The biradical is formed from the locally excited state of the phenolate anion via an electron transfer process, which neutralizes the charge separation of the ground state zwitterion. © 2009 American Institute of Physics. |
| format |
JOUR |
| author |
Carrera, A. Nielsen, I.B. Çaŗabal, P. Dedonder, C. Broquier, M. Jouvet, C. Domcke, W. Sobolewski, A.L. |
| author_facet |
Carrera, A. Nielsen, I.B. Çaŗabal, P. Dedonder, C. Broquier, M. Jouvet, C. Domcke, W. Sobolewski, A.L. |
| author_sort |
Carrera, A. |
| title |
Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| title_short |
Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| title_full |
Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| title_fullStr |
Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| title_full_unstemmed |
Biradicalic excited states of zwitterionic phenol-ammonia clusters |
| title_sort |
biradicalic excited states of zwitterionic phenol-ammonia clusters |
| url |
http://hdl.handle.net/20.500.12110/paper_00219606_v130_n2_p_Carrera |
| work_keys_str_mv |
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1782030028594216960 |