Experimental study on the vibrational relaxation mechanism of N2(X1Σg+, v = 6) molecules in collision with N2, O2, and CO

doi:10.1088/1674-1056/adf82e

Abstract This study employed time-resolved coherent anti-Stokes Raman scattering to investigate the vibrational relaxation mechanism of N$_{2}$ ($v = 6$) molecules in N$_{2}$-$M$ systems, where $M$ denotes N$_{2}$, O$_{2}$, or CO. At 297 K, the relaxation rate coefficients for collisions between N$_{2}$ ($v = 6$) and N$_{2}$, O$_{2}$, and CO were determined to be $(2.85 \pm 0.07)\times 10^{-14}$ cm$^{3}\cdot$s$^{-1}$, $(6.29 \pm 0.12)\times 10^{-14}$ cm$^{3}\cdot$s$^{-1}$, and $(11.21 \pm 0.20)\times 10^{-14}$ cm$^{3}\cdot$s$^{-1}$, respectively. The results demonstrated that the relaxation rate coefficient for N$_{2}$ ($v = 6$)-CO collisions was 1.8 times higher than that for N$_{2}$-O$_{2}$ collisions and 3.9 times greater than that for homonuclear N$_{2}$-N$_{2}$ collisions, indicating that CO significantly enhances the vibrational relaxation of N$_{2}$ ($v = 6$). Furthermore, by analyzing the time-resolved population evolution of N$_{2}$ ($v \le 6$) in N$_{2}$-O$_{2}$ and N$_{2}$-CO systems under varying buffer gas molar ratios and integrating these data with kinetic analysis, the vibrational relaxation mechanism of N$_{2}$ ($v = 6$) in different collisional environments was systematically elucidated. The findings indicate that in the N$_{2}$-O$_{2}$ system, increasing the molar ratio of acceptor molecules leads to a gradual shift from single-quantum to multi-quantum relaxation dominance, whereas the N$_{2}$-CO system exhibits a transition from multi-quantum to single-quantum dominance. In addition, a systematic study examined the vibrational relaxation mechanism of N$_{2}$ ($v = 6$) in two gas mixtures between 297 K and 573 K. The results indicate that elevated temperature significantly enhances the efficiency of near-resonance energy transfer associated with the dominant relaxation pathway.

Keywords: collision relaxation rate coefficients vibrational energy near-resonance quantum exchange multi-quantum relaxation mechanism temperature dependence

Received: 02 July 2025
Revised: 01 August 2025
Accepted manuscript online: 06 August 2025

PACS:	34.50.Ez	(Rotational and vibrational energy transfer)
	34.20.-b	(Interatomic and intermolecular potentials and forces, potential energy surfaces for collisions)
	33.80.-b	(Photon interactions with molecules)
	42.65.Dr	(Stimulated Raman scattering; CARS)

Fund: Project supported by the Natural Science Foundation of Xinjiang Uygur Autonomous Region of China (Grant No. 2024D01C51).

Corresponding Authors: Jing Liu
E-mail: xdlj@xju.edu.cn

Cite this article:

Yaqi Zhang(张亚琦), Yuhao Wu(武宇豪), Jing Liu(刘静), Jiaxin Lin(林佳欣), and Maofu Yu(于茂福) Experimental study on the vibrational relaxation mechanism of N₂(X¹Σ_g⁺, v = 6) molecules in collision with N₂, O₂, and CO 2026 Chin. Phys. B 35 033401

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Experimental study on the vibrational relaxation mechanism of N2(X1Σg+, v = 6) molecules in collision with N2, O2, and CO

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Experimental study on the vibrational relaxation mechanism of N₂(X¹Σ_g⁺, v = 6) molecules in collision with N₂, O₂, and CO