Abstract
Supramolecular photoinduced electron transfer dynamics between coumarin 153 (C153) and 4,4′-dimethyl viologen dichloride (MV2+) across the molecular barrier of a host molecule, octa acid (OA), has been investigated with femtosecond time resolution. The ultrafast electron transfer from C153 to MV2+ followed excitation with 150 fs laser pulses at a wavelength of 390 nm despite the fact that C153 was incarcerated within an OA2 capsule. As a result, the photoexcited coumarin did not show any of the typical relaxation dynamics that is usually observed in free solution. Instead, the excited electron was transferred across the molecular wall of the capsuleplex within 20 ps. Likewise, the lifetime of the charge transfer state was short (724 ps), and electron back-transfer reestablished the ground state of the system within 1 ns, showing strong electronic coupling among the excited electron donor, host, and acceptor. When the donor was encapsulated into the host molecule, the electron transfer process showed significantly accelerated dynamics and essentially no solvent relaxation compared with that in free solution. The study was also extended to N-methylpyridinium iodide as the acceptor with similar results.
| Original language | English |
|---|---|
| Pages (from-to) | 14718-14721 |
| Number of pages | 4 |
| Journal | Journal of the American Chemical Society |
| Volume | 134 |
| Issue number | 36 |
| DOIs | |
| State | Published - Sep 12 2012 |
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ASJC Scopus subject areas
- Chemistry(all)
- Catalysis
- Biochemistry
- Colloid and Surface Chemistry
Cite this
Ultrafast photoinduced electron transfer between an incarcerated donor and a free acceptor in aqueous solution. / Porel, Mintu; Chuang, Chi Hung; Burda, Clemens; Ramamurthy, Vaidhyanathan.
In: Journal of the American Chemical Society, Vol. 134, No. 36, 12.09.2012, p. 14718-14721.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Ultrafast photoinduced electron transfer between an incarcerated donor and a free acceptor in aqueous solution
AU - Porel, Mintu
AU - Chuang, Chi Hung
AU - Burda, Clemens
AU - Ramamurthy, Vaidhyanathan
PY - 2012/9/12
Y1 - 2012/9/12
N2 - Supramolecular photoinduced electron transfer dynamics between coumarin 153 (C153) and 4,4′-dimethyl viologen dichloride (MV2+) across the molecular barrier of a host molecule, octa acid (OA), has been investigated with femtosecond time resolution. The ultrafast electron transfer from C153 to MV2+ followed excitation with 150 fs laser pulses at a wavelength of 390 nm despite the fact that C153 was incarcerated within an OA2 capsule. As a result, the photoexcited coumarin did not show any of the typical relaxation dynamics that is usually observed in free solution. Instead, the excited electron was transferred across the molecular wall of the capsuleplex within 20 ps. Likewise, the lifetime of the charge transfer state was short (724 ps), and electron back-transfer reestablished the ground state of the system within 1 ns, showing strong electronic coupling among the excited electron donor, host, and acceptor. When the donor was encapsulated into the host molecule, the electron transfer process showed significantly accelerated dynamics and essentially no solvent relaxation compared with that in free solution. The study was also extended to N-methylpyridinium iodide as the acceptor with similar results.
AB - Supramolecular photoinduced electron transfer dynamics between coumarin 153 (C153) and 4,4′-dimethyl viologen dichloride (MV2+) across the molecular barrier of a host molecule, octa acid (OA), has been investigated with femtosecond time resolution. The ultrafast electron transfer from C153 to MV2+ followed excitation with 150 fs laser pulses at a wavelength of 390 nm despite the fact that C153 was incarcerated within an OA2 capsule. As a result, the photoexcited coumarin did not show any of the typical relaxation dynamics that is usually observed in free solution. Instead, the excited electron was transferred across the molecular wall of the capsuleplex within 20 ps. Likewise, the lifetime of the charge transfer state was short (724 ps), and electron back-transfer reestablished the ground state of the system within 1 ns, showing strong electronic coupling among the excited electron donor, host, and acceptor. When the donor was encapsulated into the host molecule, the electron transfer process showed significantly accelerated dynamics and essentially no solvent relaxation compared with that in free solution. The study was also extended to N-methylpyridinium iodide as the acceptor with similar results.
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U2 - 10.1021/ja3067594
DO - 10.1021/ja3067594
M3 - Article
C2 - 22931120
AN - SCOPUS:84866353934
VL - 134
SP - 14718
EP - 14721
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 36
ER -