Gamache Robert R.
Department of Environmental, Earth, and Atmospheric Sciences, University of Massachusetts Lowell, 1 University Avenue, Lowell, Massachusetts, 01854
J Mol Spectrosc. 2001 Jul;208(1):79-86. doi: 10.1006/jmsp.2001.8359.
For the first time the half-width within the complex Robert-Bonamy (CRB) formalism is calculated without making the mean relative thermal velocity approximation. The application is to the nitrogen-broadened half-width of the 500.4-GHz transition (34(2 32)<--34(1 33)) of the ground vibrational state of ozone. For each state of the perturber, the optical cross sections are determined at a number of velocities with the intermolecular potential taken as a sum of electrostatic contributions and Lennard-Jones (6-12) atom-atom components. The dynamics of the collision process are correct to second order in time. Using a nonlinear least-squares fitting method, the optical cross sections are fit to a double power law, which allows the velocity integral for the half-width to be done analytically. The results are compared with the mean relative thermal velocity complex Robert-Bonamy calculations and with measurement. The temperature dependence of the half-width, which is necessary for reduction of remotely sensed data, is determined from both methods and compared with experiment. Copyright 2001 Academic Press.
首次在不采用平均相对热速度近似的情况下，计算了复杂的罗伯特 - 博纳米（CRB）形式体系内的半高宽。应用于臭氧基振动态500.4 - GHz跃迁（34(2 32)<--34(1 33)）的氮加宽半高宽。对于微扰体的每个状态，在多个速度下确定光学截面，分子间势取为静电贡献和伦纳德 - 琼斯（6 - 12）原子 - 原子分量之和。碰撞过程的动力学在时间上精确到二阶。使用非线性最小二乘法拟合方法，将光学截面拟合为双幂律，这使得半高宽的速度积分能够解析进行。将结果与平均相对热速度复杂罗伯特 - 博纳米计算结果以及测量结果进行比较。从两种方法确定了遥感数据反演所需的半高宽的温度依赖性，并与实验进行比较。版权所有2001年学术出版社。
