Deconstructing vibrational motions on the potential energy surfaces of hydrogen-bonded complexes

Zhang，Bingbing1; Yang，Shuo1,4; Huang，Qian Rui2; Jiang，Shukang1; Chen，Rongjun1,4; Yang，Xueming1,3; Zhang，Dong H.1; Zhang，Zhaojun1; Kuo，Jer Lai2; Jiang，Ling1

2021

10.31635/ccschem.020.202000230

CCS Chemistry   影响因子和分区

2096-5745

2096-5745

Internal vibrations underlie transient structure formation, spectroscopy, and dynamics. However, at least two challenges exist when aiming to elucidate the contributions of vibrational motions on the potential energy surfaces. One is the acquisition of well-resolved experimental infrared spectra, and the other is the development of efficient theoretical methodologies that reliably predict band positions, relative intensities, and substructures. Here, we report size-specific infrared spectra of ammonia clusters to address these two challenges. Unprecedented agreement between experiment and state-of-the-art quantum simulations reveals that the vibrational spectra are mainly contributed by proton-donor ammonia. A striking Fermi resonance observed at approximately 3210 and 3250 cm originates from the coupling of NH symmetric stretch fundamentals with overtones of free and hydrogen-bonded NH bending, respectively. These novel, intriguing findings contribute to a better understanding of vibrational motions in a large variety of hydrogen-bonded complexes with orders of magnitude improvements in spectral resolution, efficiency, and specificity.

Ammonia cluster Anharmonic algorithm calculation Fermi resonance Hydrogen bonding Infrared spectroscopy Potential energy surface Quantum simulation Vibrational motion

ESCI

英语

其他

National Natural Science Foundation of China[21673231,21688102] ; Strategic Priority Research Program of the Chinese Academy of Sciences (CAS)[XDB17000000] ; Dalian Institute of Chemical Physics[DICP DCLS201702] ; K.C. Wong Education Foundation[GJTD-2018-06] ; Ministry of Science and Technology of Taiwan["MOST-106-2811-M-001-051","MOST-107-2628-M-001-002-MY4"]

Chemistry

Chemistry, Multidisciplinary

WOS:000794135600014

CHINESE CHEMICAL SOC

2-s2.0-85107618597

Scopus

1.State Key Laboratory of Molecular Reaction Dynamics,Collaborative Innovation Center of Chemistry for Energy and Materials,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
2.Institute of Atomic and Molecular Sciences,Academia Sinica,Taipei,10617,Taiwan
3.Department of Chemistry,School of Science,Southern University of Science and Technology,Shenzhen,518055,China
4.University of Chinese Academy of Sciences,Beijing,100049,China

Zhang，Bingbing,Yang，Shuo,Huang，Qian Rui,et al. Deconstructing vibrational motions on the potential energy surfaces of hydrogen-bonded complexes[J]. CCS Chemistry,2021,3(1):829-835.

Zhang，Bingbing.,Yang，Shuo.,Huang，Qian Rui.,Jiang，Shukang.,Chen，Rongjun.,...&Jiang，Ling.(2021).Deconstructing vibrational motions on the potential energy surfaces of hydrogen-bonded complexes.CCS Chemistry,3(1),829-835.

Zhang，Bingbing,et al."Deconstructing vibrational motions on the potential energy surfaces of hydrogen-bonded complexes".CCS Chemistry 3.1(2021):829-835.