Spectroscopic study of energy transfer in collisions between vibrational excited H2 and CO2.

IF 3.1 2区 化学 Q3 CHEMISTRY, PHYSICAL
Chu Qin, Xiaofang Zhao, Shuying Wang, Yifan Shen
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引用次数: 0

Abstract

The collisional energy transfer between vibrational excited H2(1, 7) and CO2 was investigated by exciting H2 to a vibrational excited state of v = 1, J = 7 by the stimulated Raman scattering technique. The coherent anti-Stokes Raman spectroscopy (CARS) technique determined that H2 was excited to the H2(1, 7) state. Varying the cuvette temperature, the number of H2(1, 7) particles was found to increase with the increase in H2 molar ratio α by scanning the intensity of the CARS spectrum, with peaks at different α at a temperature of 363 ± 15 K, but the peak temperature was not sensitive to α. Scanning CARS spectra after H2 collisions yielded that the energies of the excited states of H2 were mainly distributed in the vibrational and translational states, proving that the collisions between the excited states of H2 were linear collisions. The collisional transfer rate coefficients of H2(1, 7) and CO2 were obtained by fitting the Stern-Volmer equation as kv(H2) = (2.89 ± 0.30) × 10-13 cm3 s-1 and kv(CO2) = (8.23 ± 0.42) × 10-13 cm3 s-1. Exciting H2 to different states, it was found that the collisional transfer rate coefficient of CO2 was less affected by the energy of the vibrational excited H2. The rotational temperature was obtained from the Boltzmann distribution of the rotational dynamics, and it was found that the rotational temperature of CO2(0000, J) was about 3.4 times higher than that of CO2(0001, J), which proved that the energy of the vibrational excited H2 was mainly allocated to the higher rotational state of CO2(0000).

振动激发H2与CO2碰撞中能量传递的光谱研究。
利用受激拉曼散射技术,将H2激发至v = 1, J = 7的振动激发态,研究了H2(1,7)与CO2之间的碰撞能量传递。相干反斯托克斯拉曼光谱(CARS)技术确定H2被激发到H2(1,7)态。通过对CARS光谱强度的扫描,发现H2(1,7)颗粒的数量随着H2摩尔比α的增加而增加,在363±15 K的温度下出现不同α的峰,但峰温度对α不敏感。H2碰撞后的CARS光谱扫描结果表明,H2的激发态能量主要分布在振动和平动态,证明H2的激发态之间的碰撞是线性碰撞。根据Stern-Volmer方程拟合得到H2(1,7)与CO2的碰撞传递速率系数分别为kv(H2) =(2.89±0.30)× 10-13 cm3 s-1和kv(CO2) =(8.23±0.42)× 10-13 cm3 s-1。将H2激发到不同的状态,发现CO2的碰撞传递速率系数受振动激发H2能量的影响较小。由旋转动力学的玻尔兹曼分布得到旋转温度,发现CO2(0000, J)的旋转温度比CO2(0001, J)的旋转温度高约3.4倍,这证明了振动激发H2的能量主要分配给了CO2(0000)较高的旋转状态。
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来源期刊
Journal of Chemical Physics
Journal of Chemical Physics 物理-物理:原子、分子和化学物理
CiteScore
7.40
自引率
15.90%
发文量
1615
审稿时长
2 months
期刊介绍: The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.
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