Ultrafast hydrogen-bond dynamics in the infrared spectroscopy of water

被引：864

作者：

Fecko, CJ

Eaves, JD

Loparo, JJ

Tokmakoff, A ^{[1
]}

Geissler, PL

机构：

[1] MIT, Dept Chem, Cambridge, MA 02139 USA

[2] MIT, George R Harrison Spect Lab, Cambridge, MA 02139 USA

来源：

SCIENCE | 2003年 / 301卷 / 5640期

关键词：

D O I：

10.1126/science.1087251

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：

We investigated rearrangements of the hydrogen-bond network in water by measuring fluctuations in the OH-stretching frequency of HOD in liquid D2O with femtosecond infrared spectroscopy. Using simulations of an atomistic model of water, we relate these frequency fluctuations to intermolecular dynamics. The model reveals that OH frequency shifts arise from changes in the molecular electric field that acts on the proton. At short times, vibrational dephasing reflects an underdamped oscillation of the hydrogen bond with a period of 170 femtoseconds. At longer times, vibrational correlations decay on a 1.2-picosecond time scale because of collective structural reorganizations.

引用

页码：1698 / 1702

页数：5

共 29 条

[1] THEORY OF THE TIME DEVELOPMENT OF THE STOKES SHIFT IN POLAR MEDIA
BAGCHI, B
OXTOBY, DW
FLEMING, GR
[J]. CHEMICAL PHYSICS, 1984, 86 (03) : 257 - 267
[2] Transient absorption of vibrationally excited water
Bakker, HJ
Nienhuys, HK
Gallot, G
Lascoux, N
Gale, GM
Leicknam, JC
Bratos, S
[J]. JOURNAL OF CHEMICAL PHYSICS, 2002, 116 (06) : 2592 - 2598
[3] THE MISSING TERM IN EFFECTIVE PAIR POTENTIALS
BERENDSEN, HJC
GRIGERA, JR
STRAATSMA, TP
[J]. JOURNAL OF PHYSICAL CHEMISTRY, 1987, 91 (24) : 6269 - 6271
[4] THE INTERMOLECULAR DYNAMICS OF LIQUID WATER
CASTNER, EW
CHANG, YJ
CHU, YC
WALRAFEN, GE
[J]. JOURNAL OF CHEMICAL PHYSICS, 1995, 102 (02) : 653 - 659
[5] INSTANTANEOUS NORMAL-MODE ANALYSIS OF LIQUID WATER
CHO, M
FLEMING, GR
SAITO, S
OHMINE, I
STRATT, RM
[J]. JOURNAL OF CHEMICAL PHYSICS, 1994, 100 (09) : 6672 - 6683
[6] The integrated photon echo and solvation dynamics
Cho, MH
Yu, JY
Joo, TH
Nagasawa, Y
Passino, SA
Fleming, GR
[J]. JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (29) : 11944 - 11953
[7] Ultrafast solvation dynamics explored by femtosecond photon echo spectroscopies
de Boeij, WP
Pshenichnikov, MS
Wiersma, DA
[J]. ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 1998, 49 : 99 - 123
[8] Relationship between structural order and the anomalies of liquid water
Errington, JR
Debenedetti, PG
[J]. NATURE, 2001, 409 (6818) : 318 - 321
[9] Femtosecond dynamics of hydrogen bonds in liquid water: A real time study
Gale, GM
Gallot, G
Hache, F
Lascoux, N
Bratos, S
Leicknam, JC
[J]. PHYSICAL REVIEW LETTERS, 1999, 82 (05) : 1068 - 1071
[10] Possible mechanism of OH frequency shift dynamics in water
Georgievskii, Y
Marcus, RA
[J]. JOURNAL OF PHYSICAL CHEMISTRY A, 2001, 105 (11) : 2281 - 2284

← 1 2 3 →