非平衡量子核动力学的原子模拟

Francesco Libbi, Anders Johansson, Lorenzo Monacelli, Boris Kozinsky
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摘要

然而,在晶格激发相互作用的系统中,由于存在复杂的非线性响应,解释这些实验极具挑战性,特别是在由轻原子组成的晶体中或在离子的量子性质变得非常重要的低温条件下。在这项工作中,我们从第一性原理出发,研究单平衡量子离子动力学。我们的方法具有通用性,可以结合电子的第一性原理处理或外部机器学习势来模拟任何晶体。该方法利用非平衡态时空自洽近似(TD-SCHA),采用稳定、能量守恒、相关的随机积分方案,精度达到 $\mathcal{O}(dt^3)$。我们用一个简单的一维模型和一个太赫兹激光泵浦下真实的40原子SrTiO3晶胞对该方法进行了基准测试,为模拟超快太赫兹-X射线泵浦探针光谱(如在同步加速器设施中进行的模拟)铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Atomistic simulations of out-of-equilibrium quantum nuclear dynamics
The rapid advancements in ultrafast laser technology have paved the way for pumping and probing the out-of-equilibrium dynamics of nuclei in crystals. However, interpreting these experiments is extremely challenging due to the complex nonlinear responses in systems where lattice excitations interact, particularly in crystals composed of light atoms or at low temperatures where the quantum nature of ions becomes significant. In this work, we address the nonequilibrium quantum ionic dynamics from first principles. Our approach is general and can be applied to simulate any crystal, in combination with a first-principles treatment of electrons or external machine-learning potentials. It is implemented by leveraging the nonequilibrium time-dependent self-consistent harmonic approximation (TD-SCHA), with a stable, energy-conserving, correlated stochastic integration scheme that achieves an accuracy of $\mathcal{O}(dt^3)$. We benchmark the method with both a simple one-dimensional model to test its accuracy and a realistic 40-atom cell of SrTiO3 under THz laser pump, paving the way for simulations of ultrafast THz-Xray pump-probe spectroscopy like those performed in synchrotron facilities.
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