Improved Quantum-Classical Treatment of N<sub>2</sub>-N<sub>2</sub> Inelastic Collisions: Effect of the Potentials and Complete Rate Coefficient Data Sets

doi:10.1021/acs.jctc.3c01103

CORC > 力学研究所 > 中国科学院力学研究所 > 高温气体动力学国家重点实验室

	Improved Quantum-Classical Treatment of N₂-N₂ Inelastic Collisions: Effect of the Potentials and Complete Rate Coefficient Data Sets
	Hong QZ(洪启臻)4; Storchi, Loriano 5; Sun QH(孙泉华)3,4; Bartolomei, Massimiliano 2; Pirani, Fernando 1; Coletti, Cecilia 5
刊名	JOURNAL OF CHEMICAL THEORY AND COMPUTATION
	2023-11-26
卷号	19 期号:23 页码:8557-8571
ISSN号	1549-9618
DOI	10.1021/acs.jctc.3c01103
通讯作者	Coletti, Cecilia(ccoletti@unich.it)
英文摘要	In this study, complete (i.e., including all vibrational quantum numbers in an N-2 vibrational ladder) data sets of vibration-to-vibration and vibration-to-translation rate coefficients for N-2-N-2 collisions are explicitly computed along with transport properties (shear and bulk viscosity, thermal conductivity, and self-diffusion) in the temperature range 100-9000 K. To reach this goal, we improved a mixed quantum-classical (MQC) dynamics approach by lifting the constraint of a Morse treatment of the vibrational wave function and intramolecular potential and permitting the use of more realistic and flexible representations. The new formulation has also allowed us to separately analyze the role of intra- and intermolecular potentials on the calculated rates and properties. Ab initio intramolecular potentials are indispensable for highly excited vibrational states, though the Morse potential still gives reasonable values up to v = 20. An accurate description of the long-range interaction and the van der Waals well is a requisite for the correct reproduction of qualitative and quantitative rate coefficients, particularly at low temperatures, making physically meaningful analytical representations still the best choice compared to currently available ab initio potential energy surfaces. These settings were used to directly compute the MQC rates corresponding to a large number of initial vibrational quantum numbers, and the missing intermediate values were predicted using a machine learning technique (i.e., the Gaussian process regression approach). The obtained values are reliable in the wide temperature range employed and are therefore valuable data for many communities dealing with nonlocal thermal equilibrium conditions in different environments.
分类号	一类
资助项目	Chinese Academy of Sciences[XDA17030100] ; Strategic Priority Research Program of Chinese Academy of Sciences[2022M723233] ; China Postdoctoral Science Foundation[12302391] ; China Postdoctoral Science Foundation[PID2020-114654GB-I00] ; National Natural Science Foundation of China ; Spanish Ministerio de Ciencia e Innovacion
WOS关键词	THERMAL-CONDUCTIVITY ; ROTATIONAL RELAXATION ; VIBRATIONAL TRANSITIONS ; TRANSPORT-COEFFICIENTS ; TEMPERATURE-RANGE ; ENERGY SURFACE ; RATE CONSTANTS ; NITROGEN ; VISCOSITY ; GASES
WOS研究方向	Chemistry ; Physics
语种	英语
WOS记录号	WOS:001124992500001
资助机构	Chinese Academy of Sciences ; Strategic Priority Research Program of Chinese Academy of Sciences ; China Postdoctoral Science Foundation ; National Natural Science Foundation of China ; Spanish Ministerio de Ciencia e Innovacion
其他责任者	Coletti, Cecilia
内容类型	期刊论文
源URL	[http://dspace.imech.ac.cn/handle/311007/93743]
专题	力学研究所_高温气体动力学国家重点实验室
作者单位	1.Univ Perugia, Dipartimento Chim Biol & Biotecnol, I-06123 Perugia, Italy 2.CSIC, Inst Fis Fundamental, Madrid 28006, Spain; 3.Univ Chinese Acad Sci, Sch Engn Sci, Beijing 100049, Peoples R China; 4.Chinese Acad Sci, Inst Mech, State Key Lab High Temp Gas Dynam, Beijing 100190, Peoples R China; 5.Univ Gabriele Annunzio Chieti Pescara, Dipartimento Farm, I-66100 Chieti, Italy;
推荐引用方式 GB/T 7714	Hong QZ,Storchi, Loriano,Sun QH,et al. Improved Quantum-Classical Treatment of N₂-N₂ Inelastic Collisions: Effect of the Potentials and Complete Rate Coefficient Data Sets[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2023,19(23):8557-8571.
APA	洪启臻,Storchi, Loriano,孙泉华,Bartolomei, Massimiliano,Pirani, Fernando,&Coletti, Cecilia.(2023).Improved Quantum-Classical Treatment of N₂-N₂ Inelastic Collisions: Effect of the Potentials and Complete Rate Coefficient Data Sets.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,19(23),8557-8571.
MLA	洪启臻,et al."Improved Quantum-Classical Treatment of N₂-N₂ Inelastic Collisions: Effect of the Potentials and Complete Rate Coefficient Data Sets".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 19.23(2023):8557-8571.