Ultrafast Electron Transfer from Upper Excited State of Encapsulated Azulenes to Acceptors across an Organic Molecular Wall
In the context of generating reactive organic radical cations within a confined capsule and exploring photoinduced electron transfer from encapsulated organic molecules to organic and inorganic acceptors through an organic molecular wall, we have investigated electron transfer from the upper excited...
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| Published in | Journal of physical chemistry. C Vol. 121; no. 37; pp. 20205 - 20216 |
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| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
21.09.2017
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| Online Access | Get full text |
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| Abstract | In the context of generating reactive organic radical cations within a confined capsule and exploring photoinduced electron transfer from encapsulated organic molecules to organic and inorganic acceptors through an organic molecular wall, we have investigated electron transfer from the upper excited state (S2) of azulene (Az) and guaiazulene (GAz) enclosed within an octa acid (OA) capsule to water-soluble 4,4′-dimethyl viologen2+ (MV2+) and pyridinium+ (Py+) salts or colloidal TiO2. S2 fluorescence of OA encapsulated Az and GAz was quenched by electron acceptors such as MV2+ and Py+ salts. That electron transfer is responsible for S2 fluorescence quenching was established by recording the transient absorption spectrum of the MV●+ in the femtosecond time regime. Femtosecond time-resolved fluorescence experiments suggested that the time constant for the forward and reverse electron transfer from encapsulated Az and GAz to MV2+ is 4 and 3.6 ps, and 55.7 and 36.9 ps, respectively. The observed S2 fluorescence quenching by colloidal TiO2 in aqueous buffer solution is attributed to electron transfer from encapsulated Az and GAz to TiO2. Lack of quenching by the wider band gap material ZrO2 supported the above conclusion. FT-IR-ATR experiments confirmed that OA capsules containing Az and GAz can be adsorbed on TiO2 films, and excitation of these resulted in S2 fluorescence quenching. The observations presented here are important in the context of establishing the value of OA type cavitands where charge separation and donor shielding are critical. |
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| AbstractList | In the context of generating reactive organic radical cations within a confined capsule and exploring photoinduced electron transfer from encapsulated organic molecules to organic and inorganic acceptors through an organic molecular wall, we have investigated electron transfer from the upper excited state (S2) of azulene (Az) and guaiazulene (GAz) enclosed within an octa acid (OA) capsule to water-soluble 4,4′-dimethyl viologen2+ (MV2+) and pyridinium+ (Py+) salts or colloidal TiO2. S2 fluorescence of OA encapsulated Az and GAz was quenched by electron acceptors such as MV2+ and Py+ salts. That electron transfer is responsible for S2 fluorescence quenching was established by recording the transient absorption spectrum of the MV●+ in the femtosecond time regime. Femtosecond time-resolved fluorescence experiments suggested that the time constant for the forward and reverse electron transfer from encapsulated Az and GAz to MV2+ is 4 and 3.6 ps, and 55.7 and 36.9 ps, respectively. The observed S2 fluorescence quenching by colloidal TiO2 in aqueous buffer solution is attributed to electron transfer from encapsulated Az and GAz to TiO2. Lack of quenching by the wider band gap material ZrO2 supported the above conclusion. FT-IR-ATR experiments confirmed that OA capsules containing Az and GAz can be adsorbed on TiO2 films, and excitation of these resulted in S2 fluorescence quenching. The observations presented here are important in the context of establishing the value of OA type cavitands where charge separation and donor shielding are critical. |
| Author | Raj, A. Mohan Choudhury, Rajib Ma, Xiuyuan Mukherjee, Puspal Ramamurthy, V Porel, Mintu Galoppini, Elena Sen, Pratik |
| AuthorAffiliation | Department of Chemistry Chemistry Department Indian Institute of Technology University of Miami Department of Physical Sciences |
| AuthorAffiliation_xml | – name: Indian Institute of Technology – name: Department of Chemistry – name: University of Miami – name: Chemistry Department – name: Department of Physical Sciences |
| Author_xml | – sequence: 1 givenname: A. Mohan surname: Raj fullname: Raj, A. Mohan organization: University of Miami – sequence: 2 givenname: Mintu surname: Porel fullname: Porel, Mintu organization: University of Miami – sequence: 3 givenname: Puspal surname: Mukherjee fullname: Mukherjee, Puspal organization: Indian Institute of Technology – sequence: 4 givenname: Xiuyuan surname: Ma fullname: Ma, Xiuyuan organization: Chemistry Department – sequence: 5 givenname: Rajib surname: Choudhury fullname: Choudhury, Rajib organization: Department of Physical Sciences – sequence: 6 givenname: Elena surname: Galoppini fullname: Galoppini, Elena email: galoppin@newark.rutgers.edu organization: Chemistry Department – sequence: 7 givenname: Pratik orcidid: 0000-0002-8202-1854 surname: Sen fullname: Sen, Pratik email: psen@iitk.ac.in organization: Indian Institute of Technology – sequence: 8 givenname: V orcidid: 0000-0002-3168-2185 surname: Ramamurthy fullname: Ramamurthy, V email: murthy1@miami.edu organization: University of Miami |
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| Title | Ultrafast Electron Transfer from Upper Excited State of Encapsulated Azulenes to Acceptors across an Organic Molecular Wall |
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