Materials Simulation and Modelling, Department of Applied Physics, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.
Center for Computational Energy Research, Department of Applied Physics, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.
J Chem Inf Model. 2021 Sep 27;61(9):4415-4424. doi: 10.1021/acs.jcim.1c00432. Epub 2021 Aug 20.
In recent years, metal halide perovskites (MHPs) for optoelectronic applications have attracted the attention of the scientific community due to their outstanding performance. The fundamental understanding of their physicochemical properties is essential for improving their efficiency and stability. Atomistic and molecular simulations have played an essential role in the description of the optoelectronic properties and dynamical behavior of MHPs, respectively. However, the complex interplay of the dynamical and optoelectronic properties in MHPs requires the simultaneous modeling of electrons and ions in relatively large systems, which entails a high computational cost, sometimes not affordable by the standard quantum mechanics methods, such as density functional theory (DFT). Here, we explore the suitability of the recently developed density functional tight binding method, GFN1-xTB, for simulating MHPs with the aim of exploring an efficient alternative to DFT. The performance of GFN1-xTB for computing structural, vibrational, and optoelectronic properties of several MHPs is benchmarked against experiments and DFT calculations. In general, this method produces accurate predictions for many of the properties of the studied MHPs, which are comparable to DFT and experiments. We also identify further challenges in the computation of specific geometries and chemical compositions. Nevertheless, we believe that the tunability of GFN1-xTB offers opportunities to resolve these issues and we propose specific strategies for the further refinement of the parameters, which will turn this method into a powerful computational tool for the study of MHPs and beyond.
近年来，金属卤化物钙钛矿（MHPs）作为光电应用材料引起了科学界的关注，因为它们具有出色的性能。深入了解其物理化学性质对于提高其效率和稳定性至关重要。原子和分子模拟分别在描述 MHPs 的光电性质和动力学行为方面发挥了重要作用。然而，MHPs 中动力学和光电性质的复杂相互作用需要在相对较大的系统中同时对电子和离子进行建模，这需要很高的计算成本，有时标准的量子力学方法（如密度泛函理论（DFT））无法负担。在这里，我们探索了最近开发的密度泛函紧束缚方法 GFN1-xTB 用于模拟 MHPs 的适用性，旨在探索 DFT 的有效替代方法。通过与实验和 DFT 计算对比，对 GFN1-xTB 计算几种 MHPs 的结构、振动和光电性质的性能进行了基准测试。总的来说，该方法对所研究的 MHPs 的许多性质都能做出准确的预测，与 DFT 和实验结果相当。我们还确定了在计算特定几何形状和化学成分时存在的进一步挑战。然而，我们相信 GFN1-xTB 的可调性为解决这些问题提供了机会，我们提出了特定的策略来进一步细化参数，这将使该方法成为研究 MHPs 及其它领域的强大计算工具。
