The hydrogen-bond collective dynamics in liquid methanol

被引:19
作者
Bellissima, Stefano [1 ]
De Panfilis, Simone [2 ]
Bafile, Ubaldo [3 ]
Cunsolo, Alessandro [4 ]
Gonzalez, Miguel Angel [5 ]
Guarini, Eleonora [1 ]
Formisano, Ferdinando [6 ]
机构
[1] Univ Florence, Dipartimento Fis, I-50019 Sesto Fiorentino, Italy
[2] Ist Italiano Tecnol, Ctr Life Nanosci, I-00161 Rome, Italy
[3] CNR, Ist Sistemi Complessi, I-50019 Sesto Fiorentino, Italy
[4] Brookhaven Natl Lab, Natl Synchrotron Light Source 2, Upton, NY 11973 USA
[5] Inst Laue Langevin, F-38042 Grenoble, France
[6] CNR, Ist Off Mat, Operat Grp Grenoble, F-38042 Grenoble, France
关键词
1ST COORDINATION SHELL; NORMAL-MODE ANALYSIS; NEUTRON-SCATTERING; HEAVY-WATER; FAST SOUND; EXCITATIONS; SPECTROSCOPY; SPECTRUM; PRESSURES; MOTIONS;
D O I
10.1038/srep39533
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 relatively simple molecular structure of hydrogen-bonded (HB) systems is often belied by their exceptionally complex thermodynamic and microscopic behaviour. For this reason, after a thorough experimental, computational and theoretical scrutiny, the dynamics of molecules in HB systems still eludes a comprehensive understanding. Aiming at shedding some insight into this topic, we jointly used neutron Brillouin scattering and molecular dynamics simulations to probe the dynamics of a prototypical hydrogen-bonded alcohol, liquid methanol. The comparison with the most thoroughly investigated HB system, liquid water, pinpoints common behaviours of their THz microscopic dynamics, thereby providing additional information on the role of HB dynamics in these two systems. This study demonstrates that the dynamic behaviour of methanol is much richer than what so far known, and prompts us to establish striking analogies with the features of liquid and supercooled water. In particular, based on the strong differences between the structural properties of the two systems, our results suggest that the assignment of some dynamical properties to the tetrahedral character of water structure should be questioned. We finally highlight the similarities between the characteristic decay times of the time correlation function, as obtained from our data and the mean lifetime of hydrogen bond known in literature.
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页数:10
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