论文标题
一种用于核心激发的跨蒙特卡洛方法
A variational Monte Carlo approach for core excitations
论文作者
论文摘要
我们提出了一种系统不足的方法，用于变异蒙特卡洛的核心激发。在兴奋状态特异性蒙特卡洛的最新工作的基础上，我们展示了从量子化学猜测开始的直接方案如何能够捕获核心状态的强轨道松弛，在这些放松期间保持近核区域的准确性，并明确平衡地面和核心激发状态之间的准确性。在水，氨和甲烷中，它们分别用作氧，氮和碳核状态的典型代表，即使使用相对较小的波浪功能扩展，这种方法即使在最佳的理论方法上也可以提供准确的理论方法。
We present a systematically-improvable approach to core excitations in variational Monte Carlo. Building on recent work in excited-state-specific Monte Carlo, we show how a straightforward protocol, starting from a quantum chemistry guess, is able to capture core state's strong orbital relaxations, maintain accuracy in the near-nuclear region during these relaxations, and explicitly balance accuracy between ground and core excited states. In water, ammonia, and methane, which serve as prototypical representatives for oxygen, nitrogen, and carbon core states, respectively, this approach delivers accuracies on par with the best available theoretical methods even when using relatively small wave function expansions.
