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Efficient Intramolecular Vibrational Excitonic Energy Transfer in Ru-3(CO)(12) Cluster Revealed by Two-Dimensional Infrared Spectroscopy
Dong, Xueqian; Yang, Fan; Zhao, Juan; Wang, Jianping
JAN 25 2018
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY B
Volume122Issue:3Pages:1296-1305
AbstractTrinuclear transition-metal carbonyl complex dodecacarbonyl triruthenium (Ru-3(CO)(12)) is considered as one of the paradigms in cluster chemistry, which plays an important role in photocatalysis, photoenergy conversion, and synthetic chemistry. Due to structural symmetry (D-3h point group), 12 carbonyl (C O) groups in the Ru-3(CO)(12) complex contribute to mainly three excitonic carbonyl stretching modes: E ' (radial), A(2)'' (axial), and E ' (axial). In this work, efficient intramolecular vibrational energy redistribution (IVR) processes among the three modes in this RuCO complex were observed to occur on the time scale of tens of picoseconds. The IVR processes were characterized in detail using a kinetic model and fitting to the waiting-time-dependent diagonal and off-diagonal signals of ultrafast two-dimensional infrared spectroscopy. In addition, the diagonal anharmonicities of the three C O stretching modes were determined to be quite close to one another, and the coupling-induced cross peaks were invariant because this Ru-3(CO)(12) cluster does not show picosecond fluxionality and hence their contributions were neglected in modeling the IVR processes. Our results provide a benchmark for understanding the excitonic nature of the vibrational excited states of the carbonyl vibrators and the associated efficient vibrational energy-flow pathways, in such multicentered transition-metal complexes, which are of key importance to their functions.
WOS IDWOS:000423652900032
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Cited Times:3[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/38824
Collection其它
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GB/T 7714
Dong, Xueqian,Yang, Fan,Zhao, Juan,et al. Efficient Intramolecular Vibrational Excitonic Energy Transfer in Ru-3(CO)(12) Cluster Revealed by Two-Dimensional Infrared Spectroscopy[J]. JOURNAL OF PHYSICAL CHEMISTRY B,JAN ,122(3):1296-1305.
APA Dong, Xueqian,Yang, Fan,Zhao, Juan,&Wang, Jianping.(JAN ).Efficient Intramolecular Vibrational Excitonic Energy Transfer in Ru-3(CO)(12) Cluster Revealed by Two-Dimensional Infrared Spectroscopy.JOURNAL OF PHYSICAL CHEMISTRY B,122(3),1296-1305.
MLA Dong, Xueqian,et al."Efficient Intramolecular Vibrational Excitonic Energy Transfer in Ru-3(CO)(12) Cluster Revealed by Two-Dimensional Infrared Spectroscopy".JOURNAL OF PHYSICAL CHEMISTRY B 122.3(JAN ):1296-1305.
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