论文标题

碰撞引起的三体极化氦

Collision-induced three-body polarizability of helium

论文作者

Lang, Jakub, Lesiuk, Michal, Przybytek, Michal, Jeziorski, Bogumil

论文摘要

我们提出了三体极化性和第三个介电病毒系数的第一原理理论测定。耦合群集理论和完整的配置交互过程用于执行所需的电子结构计算。使用外推技术确定了三体极化张量张量的痕迹的平均绝对相对不确定性。使用完整的配置相互作用计算估计了由于三重近似处理和忽略更高激发的额外不确定性。开发了一种分析功能来描述极化性及其渐近衰变对三原子和原子 - diatom碎裂通道的行为。我们还开发了一个分析函数,描述了计算总体不确定性的局部行为。使用这两种拟合,我们使用经典和半经典的Feynman-Hibbs方法计算了第三个介电病毒系数及其不确定性。将我们的计算结果与可用的实验数据进行了比较,以及最近采用了三体极化性的所谓叠加近似近似值的近期路径综合蒙特卡洛(PIMC)计算。对于高于200 K的温度,我们观察到使用叠加近似或从头算的极化性获得的经典结果之间的显着差异。这项工作中报告的理论数据消除了光压标准发展的主要准确性瓶颈,并有望促进量子热量学领域的进一步进步

We present first-principles theoretical determination of the three-body polarizability and the third dielectric virial coefficient of helium. Coupled-cluster theory and the full configuration interaction procedure were used to perform required electronic structure calculations. The mean absolute relative uncertainty of the trace of the three-body polarizability tensor, resulting from the incompleteness of orbital basis set, was determined using extrapolation techniques. Additional uncertainty due to approximate treatment of triple and the neglect of higher excitations was estimated using full configuration interaction calculations. An analytic function was developed to describe the behavior of the polarizability and its asymptotic decay to three-atomic and atom-diatom fragmentation channels. We also developed an analytic function describing the local behavior of the total uncertainty of our calculations. Using both fits we calculated the third dielectric virial coefficient and its uncertainty using the classical and semiclassical Feynman-Hibbs approaches. The results of our calculations were compared with available experimental data and with recent Path-Integral Monte Carlo (PIMC) calculations employing the so-called superposition approximation of the three-body polarizability. For temperatures above 200 K we observed significant discrepancy between the classical results obtained using either the superposition approximation or the ab initio computed polarizability. The theoretical data reported in this work eliminate the main accuracy bottleneck of the development of optical pressure standard and are expected to facilitate further progress in the field of quantum thermal metrology

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