期刊
JOURNAL OF PHYSICAL CHEMISTRY A
卷 118, 期 36, 页码 7788-7795出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp505188y
关键词
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资金
- National Natural Science Foundation of China [61177017]
- National Science Center of Poland [2012/04/A/ST2/00100]
- Deutsche Forschungsgemeinschaft
- DFG cluster of excellence Munich Centre for Advanced Photonics
It has recently been shown that low-lying dark charge-separated singlet excited states of n pi* and pi pi* character exist in the hydrogen-bonded pyridine-water complex in addition to the familiar n pi* and pi pi* excited states of the pyridine chromophore. The former have been shown to promote the transfer of a proton from water to pyridine, resulting in the pyridinyl-hydroxyl radical pair. In the present work, the potential-energy surfaces of the triplet excited states of the pyridine-water complex have been explored with the same ab initio electronicstructure methods (ADC(2), CASPT2). Minimum-energy reaction paths for excited-state H atom transfer, energy surfaces in the vicinity of the barrier for H atom transfer, as well as multistate surface crossings have been characterized. The photochemical reaction mechanisms on the singlet and triplet potential-energy surfaces are compared, and their relevance for photoinduced water oxidation with the pyridine chromophore are discussed.
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