非平衡初始条件在分子转动中的表现：广义J-扩散模型
Manifestation of nonequilibrium initial conditions in molecular rotation: the generalized J-diffusion model
摘要：
为了充分描述远离平衡的分子旋转，我们通过允许旋转弛豫速率与角动量相关来推广J-扩散模型。计算的非平衡转动关联函数（CFs）的衰减速度比它们的平衡对应物慢得多，热分子的取向CFs表现出相干的行为，它持续了几个旋转周期。与标准理论的结果不同，转动和取向的CF被发现强烈依赖于分子系综的非平衡制备。我们预测的Arbriius能量依赖的旋转弛豫时间和违反哈伯德关系的取向弛豫时间。标准和广义J-扩散模型被证明是几乎不可区分的平衡条件下。他们的预测远非均衡，可能大相径庭。
英文摘要：
In order to adequately describe molecular rotation far from equilibrium, we have generalized the J-diffusion model by allowing the rotational relaxation rate to be angular momentum dependent. The calculated nonequilibrium rotational correlation functions (CFs) are shown to decay much slower than their equilibrium counterparts, and orientational CFs of hot molecules exhibit coherent behavior, which persists for several rotational periods. As distinct from the results of standard theories, rotational and orientational CFs are found to dependent strongly on the nonequilibrium preparation of the molecular ensemble. We predict the Arrhenius energy dependence of rotational relaxation times and violation of the Hubbard relations for orientational relaxation times. The standard and generalized J-diffusion models are shown to be almost indistinguishable under equilibrium conditions. Far from equilibrium, their predictions may differ dramatically.
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