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Geometry optimization of large molecules with quantum Monte Carlo

利用量子蒙特卡罗对大分子进行几何优化

基本信息

批准号：
414171116
负责人：
Dr. Jonas Feldt
金额：
--
依托单位：
Faculteit Technische Natuurwetenschappen
依托单位国家：
德国
项目类别：
Research Fellowships
财政年份：
2018
资助国家：
德国
起止时间：
2017-12-31 至 2020-12-31
项目状态：
已结题

来源：
https://gepris.dfg.de/gepris/projekt/414171116?language=en
关键词：
Geometry optimization large molecules quantum

项目摘要

The availability of advanced computational tools to accurately and efficiently describe light-induced processes in complex systems is key to the development of new technologies for artificial photosynthesis, photo-catalysis, bio-imaging, and photo-medical applications. Computing excited states, however, is highly demanding for electronic structure methods, which often struggle to ensure accuracy or to treat the large, relevant system sizes. To overcome these limitations, we will work in the alternative framework of quantum Monte Carlo methods which use stochastic algorithms to solve the Schrödinger equation, scale well with system size, and offer a balanced description of the ground and electronic excited states. Here, we intend to further push this methodology and extend its applicability to the computation of structural properties of large molecular systems in the ground and excite states. To this aim, we will accelerate the computation of interatomic forces required to determine optimal structures and reaction pathways, by developing improved estimators characterized by small fluctuations and reduced bias. This will allow for considerably shorter Monte Carlo simulations and equally accurate structures with the use of simpler wave functions and, therefore, open the possibility to treat significantly larger systems. Furthermore, we plan to extend and explore the use of the more accurate and robust diffusion Monte Carlo method to structural relaxation. The advances achieved via these developments will be demonstrated on the study of the photoinduced switching mechanism of donor-acceptor Stenhouse adduct molecules, a novel class of synthetic photoswitches with promising applications in material science and biological systems.

利用先进的计算工具来准确有效地描述复杂系统中的光诱导过程是人工光合作用、光催化、生物成像和光医学应用新技术发展的关键。然而，计算激发态对电子结构方法的要求很高，这些方法通常难以确保准确性或处理大的相关系统尺寸。为了克服这些局限性，我们将在量子蒙特卡罗方法的替代框架下工作，该方法使用随机算法来求解薛定谔方程，随着系统尺寸的变化而变化，并提供基态和电子激发态的平衡描述。在这里，我们打算进一步推动这种方法，并将其适用性扩展到计算大分子系统的基态和激发态的结构性质。为了这个目标，我们将加快计算所需的原子间的力量，以确定最佳的结构和反应途径，通过开发改进的估计，其特点是小波动和减少偏见。这将允许相当短的蒙特卡罗模拟和同样准确的结构，使用更简单的波函数，因此，打开的可能性，以治疗显着更大的系统。此外，我们计划扩展和探索使用更准确和更强大的扩散蒙特卡罗方法的结构松弛。通过这些发展所取得的进展将证明对供体-受体Stenhouse加合物分子的光诱导开关机制的研究，一类新型的合成光开关，在材料科学和生物系统中具有广阔的应用前景。