论文标题

通过几何预采样:液体水的应用中的电子停止的电子停止有效地计算。

Efficient ab initio calculation of electronic stopping in disordered systems via geometry pre-sampling: application to liquid water

论文作者

Gu, Bin, Cunningham, Brian, Muñoz-Santiburcio, Daniel, Da Pieve, Fabiana, Artacho, Emilio, Kohanoff, Jorge

论文摘要

对Swift离子的电子停止曲线的了解,$ S_E(V)$,尤其是在Bragg Peak附近,对于理解辐射损害很重要。然而,从实验上讲,对轻离子的这种特征非常具有挑战性,尤其是在液体水和生物组织等无序系统中。实时时间相关密度功能理论(RT-TDDFT)的最新发展使沿NM大小的轨迹对$ S_E(V)$的计算。但是,获得可以比较观测值的有意义的统计平均$ s_e(v)$仍然是一个挑战。 In this work, taking advantage of the correlation between the local electronic structure probed by the projectile and the distance from the projectile to the atoms in the target, we devise a trajectory pre-sampling scheme to select, geometrically, a small set of short trajectories to accelerate the convergence of the averaged $S_e(v)$ computed via rt-TDDFT.对于液态水中的质子,我们首先计算从质子到最接近氧原子的距离的参考概率分布函数(PDF),$ ϕ_R(r_ {p {\ rightarrow} o})$,对于与这些采样实验相似的长度的轨迹。然后,将短轨迹顺序选择,以便累积的PDF再现$ ϕ_R(r_ {p {\ rightarrow} o})$,以越来越高的精度。使用这些预采样的轨迹,我们证明了平均$ s_e(v_p)$在整个速度范围内收敛,少于八个轨迹,而其他使用随机和均匀分布的轨迹的平均方法则需要大约是计算工作的十倍。这使我们可以将$ S_E(V_P)$曲线与实验数据进行比较,并根据Bragg的规则评估广泛使用的经验表。

Knowledge of the electronic stopping curve for swift ions, $S_e(v)$, particularly around the Bragg peak, is important for understanding radiation damage. Experimentally, however, the determination of such feature for light ions is very challenging, especially in disordered systems such as liquid water and biological tissue. Recent developments in real-time time-dependent density functional theory (rt-TDDFT) have enabled the calculation of $S_e(v)$ along nm-sized trajectories. However, it is still a challenge to obtain a meaningful statistically averaged $S_e(v)$ that can be compared to observations. In this work, taking advantage of the correlation between the local electronic structure probed by the projectile and the distance from the projectile to the atoms in the target, we devise a trajectory pre-sampling scheme to select, geometrically, a small set of short trajectories to accelerate the convergence of the averaged $S_e(v)$ computed via rt-TDDFT. For protons in liquid water, we first calculate the reference probability distribution function (PDF) for the distance from the proton to the closest oxygen atom, $ϕ_R(r_{p{\rightarrow}O})$, for a trajectory of a length similar to those sampled experimentally. Then, short trajectories are sequentially selected so that the accumulated PDF reproduces $ϕ_R(r_{p{\rightarrow}O})$ to increasingly high accuracy. Using these pre-sampled trajectories, we demonstrate that the averaged $S_e(v_p)$ converges in the whole velocity range with less than eight trajectories, while other averaging methods using randomly and uniformly distributed trajectories require approximately ten times the computational effort. This allows us to compare the $S_e(v_p)$ curve to experimental data, and assess widely used empirical tables based on Bragg's rule.

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