论文标题
与交换的无限级扰动处理量子进化
Infinite-order perturbative treatment for quantum evolution with exchange
论文作者
论文摘要
生物化学，材料科学和催化中的许多重要应用正好位于量子和统计力学之间的界面：连贯的演化被离散事件（例如底物的结合或异构化的结合）中断。这种动力学的理论模型通常会截断这些事件将这些事件的掺入到线性响应极限上，从而需要小的步骤尺寸。在这里，我们完全重新评估了化学交换模型的基础，并重新设计了对扰动理论中所有秩序准确的主方程处理。最终结果是对传统图片的惊人简单纠正，它极大地改善了收敛性，而没有增加计算成本。我们证明，这种方法可以准确有效地从高度复杂的实验数据中提取物理参数，例如磁共振中的相干超极化动力学，并且适用于广泛的其他系统。
Many important applications in biochemistry, materials science, and catalysis sit squarely at the interface between quantum and statistical mechanics: coherent evolution is interrupted by discrete events, such as binding of a substrate or isomerization. Theoretical models for such dynamics usually truncate the incorporation of these events to the linear-response limit, thus requiring small step sizes. Here, we completely re-assess the foundations of chemical exchange models and redesign a master equation treatment accurate to all orders in perturbation theory. The net result is an astonishingly simple correction to the traditional picture which vastly improves convergence with no increased computational cost. We demonstrate that this approach accurately and efficiently extracts physical parameters from highly complex experimental data, such as coherent hyperpolarization dynamics in magnetic resonance, and is applicable to a wide range of other systems.
