Infrared spectroscopic study of hydrogen bonding topologies in the smallest ice cube

Li，Gang1; Zhang，Yang Yang2; Li，Qinming1,3; Wang，Chong1,3; Yu，Yong1,3; Zhang，Bingbing1; Hu，Han Shi2; Zhang，Weiqing1; Dai，Dongxu1; Wu，Guorong1; Zhang，Dong H.1; Li，Jun2,4; Yang，Xueming1,4; Jiang，Ling1

2020-12-01

10.1038/s41467-020-19226-6

Nature Communications   影响因子和分区

2041-1723

2041-1723

The water octamer with its cubic structure consisting of six four-membered rings presents an excellent cluster system for unraveling the cooperative interactions driven by subtle changes in the hydrogen-bonding topology. Despite prediction of many distinct structures, it has not been possible to extract the structural information encoded in their vibrational spectra because this requires size-selectivity of the neutral clusters with sufficient resolution to identify the contributions of the different isomeric forms. Here we report the size-specific infrared spectra of the isolated cold, neutral water octamer using a scheme based on threshold photoionization using a tunable vacuum ultraviolet free electron laser. A plethora of sharp vibrational bands features are observed. Theoretical analysis of these patterns reveals the coexistence of five cubic isomers, including two with chirality. The relative energies of these structures are found to reflect topology-dependent, delocalized multi-center hydrogen-bonding interactions. These results demonstrate that even with a common structural motif, the degree of cooperativity among the hydrogen-bonding network creates a hierarchy of distinct species. The implications of these results on possible metastable forms of ice are speculated.

SCI

英语

NI论文

通讯

National Natural Science Foundation of China[21688102][21673231][21590792][91645203] ; Strategic Priority Research Program of Chinese Academy of Sciences (CAS)[XDB17000000] ; International Partnership Program of CAS[121421KYSB20170012] ; Dalian Institute of Chemical Physics[DICP DCLS201701][DCLS201702] ; CAS[GJJSTD20190002] ; Science Challenge Project[TZ2016004]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000588060400006

NATURE RESEARCH

2-s2.0-85094187567

Scopus

1.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
2.Key Laboratory of Organic Optoelectronics & Molecular Engineering of the Ministry of Education,Department of Chemistry,Tsinghua University,Beijing,100084,China
3.University of Chinese Academy of Sciences,Beijing,19A Yuquan Road,100049,China
4.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China

Li，Gang,Zhang，Yang Yang,Li，Qinming,et al. Infrared spectroscopic study of hydrogen bonding topologies in the smallest ice cube[J]. Nature Communications,2020,11(1).

Li，Gang.,Zhang，Yang Yang.,Li，Qinming.,Wang，Chong.,Yu，Yong.,...&Jiang，Ling.(2020).Infrared spectroscopic study of hydrogen bonding topologies in the smallest ice cube.Nature Communications,11(1).

Li，Gang,et al."Infrared spectroscopic study of hydrogen bonding topologies in the smallest ice cube".Nature Communications 11.1(2020).