期刊
ANNUAL REVIEW OF PHYSICAL CHEMISTRY
卷 60, 期 -, 页码 21-38出版社
ANNUAL REVIEWS
DOI: 10.1146/annurev-physchem-073108-112712
关键词
solute-solvent complex dynamics; carbon-carbon single-bond isomerization dynamics; protein structural substate switching dynamics
资金
- Air Force Office of Scientific Research [F49620-01-1-0018]
- National Science Foundation [DMR 0652232]
- National Institutes of Health [2 R01 GM-061137-05]
- NATIONAL INSTITUTE OF GENERAL MEDICAL SCIENCES [R01GM061137] Funding Source: NIH RePORTER
A wide variety of molecular systems undergo fast structural changes under thermal equilibrium conditions. Such transformations are involved in a vast array of chemical problems. Experimentally measuring equilibrium dynamics is a challenging problem that is at the forefront of chemical research. This review describes ultrafast 2D IR vibrational echo chemical exchange experiments and applies them to several types of molecular systems. The formation and dissociation of organic solute-solvent complexes are directly observed. The dissociation times of 13 complexes, ranging from 4 ps to 140 ps, are shown to obey a relationship that depends on the complex's formation enthalpy. The rate of rotational gauche-trans isomerization around a carbon-carbon single bond is determined for a substituted ethane at room temperature in a low viscosity solvent. The results are used to obtain an approximate isomerization rate for ethane. Finally, the time dependence of a well-defined single structural transformation of a protein is measured.
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