Singh Aditi, Jana Subrata, Constantin Lucian A, Della Sala Fabio, Samal Prasanjit, Śmiga Szymon
Institute of Physics, Faculty of Physics, Astronomy and Informatics, Nicolaus Copernicus University, Grudziadzka 5, 87-100 Toruń, Poland.
Institute of Physics, Faculty of Physics, Astronomy and Informatics, Nicolaus Copernicus University in Toruń, ul. Grudzia̧dzka 5, 87-100 Toruń, Poland.
J Phys Chem Lett. 2025 Aug 14;16(32):8198-8208. doi: 10.1021/acs.jpclett.5c01441. Epub 2025 Aug 4.
Range-separated hybrid (RSH) functionals with "ionization energy" and/or "optimal tuning" of the screening parameter have proven to be among the most practical and accurate approaches for describing excited-state properties across a wide range of systems, including condensed matter. However, this method typically requires multiple self-consistent calculations and can become computationally expensive and unstable, particularly for extended systems. In this work, we propose a very simple and efficient alternative approach to determine the screening parameter for RSH functionals solely on the basis of the total electron density of the system and the compressibility sum rule of density functional theory (DFT). This effective screening parameter achieves remarkable accuracy, particularly for charge-transfer excitations, surpassing the performance of previously suggested alternatives. Because it relies on only the electron density, the proposed approach is physically transparent and highly practical to automate DFT calculations in large and complex systems, including bulk solids, where "tuning" is not possible.
具有“电离能”和/或筛选参数“最优调谐”的范围分离杂化(RSH)泛函已被证明是描述包括凝聚态物质在内的广泛体系激发态性质的最实用且准确的方法之一。然而,该方法通常需要多次自洽计算,并且可能在计算上变得昂贵且不稳定,特别是对于扩展体系。在这项工作中,我们提出了一种非常简单且有效的替代方法,仅基于体系的总电子密度和密度泛函理论(DFT)的压缩性求和规则来确定RSH泛函的筛选参数。这个有效的筛选参数具有显著的准确性,特别是对于电荷转移激发,超过了先前提出的替代方法的性能。由于它仅依赖于电子密度,所提出的方法在物理上是透明的,并且对于在大型复杂体系(包括无法进行“调谐”的块状固体)中自动化DFT计算非常实用。