期刊
JOURNAL OF PHYSICAL CHEMISTRY B
卷 119, 期 14, 页码 4857-4864出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.5b00744
关键词
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资金
- NSF [CAREER CHE-0847707, CHE-0923360]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0847707] Funding Source: National Science Foundation
Ultrafast transient absorption spectroscopy is used to investigate the radiationless relaxation dynamics of CuCl42- and IrBr62- complexes directly promoted into their lowest energy excited metal centered states upon near infrared femtosecond excitation at 2000 nm. Both the excited CuCl42- E-2 and IrBr62- 2Ug'(T-2g) states undergo internal conversion to the ground electronic states, yet with significantly different lifetimes (55 Is and 360 ps, respectively) despite the fact that the E-2 and 2Ug'(T-2g) states are separated by the same energy gap (similar to 5000 cm(-1)) from the respective ground state. This difference likely arises from the predominance of the Jahn-Teller effect in a Cu2+ ion and the spin-orbit coupling effect in an Ir4+ ion. The approach documented in this work may be used for elucidating the role of low energy metal-centered states in relaxation cascades of a number of coordination compounds, allowing for design of efficient light-triggered metal complexes.
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