Full quantum dynamics of the interparticle Coulombic electron capture

在范德华力和氢键系统以及量子点阵列中，ICEC已被理论预测。在这些工作中采用的理论方法范围从分析模型从头计算电子结构和动力学计算。这些方法中的一个共同假设是，在ICEC期间，细胞核保持固定。然而，基于对相关粒子间库仑衰变（ICD）的观测，核动力学应该在改变效率和/或影响系统的最终状态方面发挥重要作用。因此，我们的项目的目的是开发，实施和应用原始的量子动力学方法，以提供一个完整的描述ICEC。为了实现这一雄心勃勃的目标，我们将联合收割机我们的团队互补的专业知识：我们将开发ICEC模型，将（数值）精确解决使用多配置时间相关哈特里（MCTDH）方法。我们将逐步降低这种模型系统的近似程度，从而使现实的原子和分子系统的研究成为可能。此外，我们将开发分析方法，这将提供深入了解核动力学在ICEC的影响，并帮助解释的数值模拟。最后，通过这些经过验证的方法收集的信息将导致基于R矩阵方法的有效工具的开发。由于电子捕获过程的普遍存在，我们的项目将在从辐射损伤到天体化学/物理学的广泛应用中产生重大影响。此外，我们的研究结果将奠定基础的预期，不久的将来的实验ICEC的解释，并在同一时间，刺激理论-实验协同作用的预测有前途的ICEC目标系统。

ICEC has been predicted theoretically in van-der-Waals and hydrogen bonded systems as well as in quantum dot arrays. The theoretical approaches employed in these works range from analytical models to ab-initio electronic structure and dynamical calculations. A common assumption in these approaches is that nuclei remain fixed during ICEC. However, based on observations on the related inter-particle Coulombic decay (ICD), nuclear dynamics should play an important role changing the efficiency and/or influencing the final state of the system. The aim of our project is therefore to develop, implement, and apply original quantum-dynamical methods to provide a complete description of ICEC. To achieve this ambitious goal, we will combine the complementary expertise of our groups: we will develop ICEC models that will be (numerically) exactly solved using the multiconfiguration time-dependent Hartree (MCTDH) method. We will gradually lower the degree of approximation in such model systems, thus enabling the study of realistic atomic and molecular systems. Furthermore, we will develop analytical approaches which will provide insights into the impact of nuclear dynamics in ICEC and help the interpretation of the numerical simulations. Finally, the information gathered through these validated methods will lead to the development of efficient tools based on the R-matrix approach. Owing to the ubiquity of electron capture processes, our project will have a significant impact in a broad range of applications from radiation damage, to astro-chemistry/physics. Furthermore, our results will lay the groundwork for the interpretation of expected, near-future experiments on ICEC and at the same time, stimulating a theory-experiment synergy for the prediction of promising ICEC target systems.