Large Angular Jump Mechanism Observed for Hydrogen Bond Exchange in Aqueous Perchlorate Solution

被引：181
|
作者：
Ji, Minbiao [1 ,2 ]
Odelius, Michael [3 ]
Gaffney, K. J. [1 ]
机构：
[1] Stanford Univ, SLAC Natl Accelerator Lab, PULSE Inst Ultrafast Energy Sci, Stanford, CA 94305 USA
[2] Stanford Univ, Dept Phys, Stanford, CA 94305 USA
[3] Stockholm Univ, AlbaNova Univ Ctr, SE-10691 Stockholm, Sweden
来源：
SCIENCE | 2010年 / 328卷 / 5981期
基金：
瑞典研究理事会;
关键词：
INFRARED-SPECTROSCOPY; ULTRAFAST DYNAMICS; MOLECULAR-DYNAMICS; LIQUID WATER; 2D IR; REORIENTATION; 3RD-ORDER; 2D-IR; TIME;
D O I：
10.1126/science.1187707
中图分类号：
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号：
07 ; 0710 ; 09 ;
摘要：
The mechanism for hydrogen bond (H-bond) switching in solution has remained subject to debate despite extensive experimental and theoretical studies. We have applied polarization-selective multidimensional vibrational spectroscopy to investigate the H-bond exchange mechanism in aqueous NaClO(4) solution. The results show that a water molecule shifts its donated H-bonds between water and perchlorate acceptors by means of large, prompt angular rotation. Using a jump-exchange kinetic model, we extracted an average jump angle of 49 +/- 4 degrees, in qualitative agreement with the jump angle observed in molecular dynamics simulations of the same aqueous NaClO(4) solution.
引用
收藏
页码：1003 / 1005
页数：3
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