Non‐Markovian effects having a strong influence on far‐wing intensities of spectroscopic signatures by molecular gases are analyzed theoretically with the use of a non‐Markovian relaxation matrix derived for rapidly colliding linear rotators (J. Chem. Phys. 149, 044305 [2018]) for the benchmark case of rototranslational Raman spectra of molecular nitrogen recorded at high densities up to very far wings (Phys. Lett. A 157, 44 [1991]). This matrix is built here on the base of the translational‐spectrum model of Birnbaum and Cohen and the recently computed, from known potential energy surfaces, two leading classical spectral moments (J. Ram. Spectrosc. 2020, DOI: 10.1002/jrs.5923). Theoretical intensity computations, going beyond the commonly used impact approximation, give much less overestimated values in the far wing and constitute a promising tool for getting accurate theoretical description of broad‐band spectra.

中文翻译：

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从超前光谱矩预测的N2-N2旋转平移拉曼光谱上的压力效应

从分子气体对光谱特征的远翼强度产生重大影响的非马尔可夫效应通过理论上使用非马尔可夫弛豫矩阵进行分析，该矩阵用于快速碰撞的线性旋转器（J. Chem。Phys。149，044305 [2018 ]）作为分子氮的旋转翻译拉曼光谱的基准案例，以高密度记录到非常远的机翼（Phys。Lett。A 157，44 [1991]）。这个矩阵是在Birnbaum和Cohen的平移光谱模型以及最近从已知势能面计算出的两个主要经典光谱矩的基础上建立的（J.Ram.Spectrosc.2020，DOI：10.1002 / jrs.5923 ）。理论强度计算超出了常用的冲击近似法，