Real-time time-dependent density functional theory (RT-TDDFT) is a powerful approach for investigating various ultrafast phenomena in materials. However, most existing RT-TDDFT studies rely on adiabatic local or semi-local approximations, which suffer from several shortcomings, including the inability to accurately capture excitonic effects in periodic systems. Combining RT-TDDFT with range-separated hybrid (RSH) functionals has emerged as an effective strategy to overcome these limitations. The RT-TDDFT-RSH implementation for periodic systems requires careful treatment of the Coulomb singularity and choosing proper gauges for the incorporation of external fields. We benchmark two schemes for treating the Coulomb singularity - the truncated Coulomb potential and the auxiliary-function correction - and find that the latter shows better convergence behavior and numerical stability for long-range corrected hybrid functions. Additionally, we assess the impact of gauge choice in simulations using numerical atomic orbitals and show that the recently proposed hybrid gauge incorporating position-dependent phases provides a more accurate description of excitonic absorption than the conventional velocity gauge. Our implementation significantly improves the accuracy of RT-TDDFT-RSH for modeling ultrafast excitonic dynamics in periodic systems.
Automated Workflow for Non-Empirical Wannier-Localized Optimal Tuning of Range-Separated Hybrid Functionals
University of California Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Université catholique de Louvain (UCLouvain)（天主教鲁汶大学）；Matgenix SRL（Matgenix有限责任公司）；Weizmann Institute of Science（魏茨曼科学研究所）；University of Massachusetts Amherst（马萨诸塞大学阿默斯特分校）；Kavli Energy NanoScience Institute at Berkeley（加州大学伯克利分校卡弗里能源纳米科学研究所）
Electronic and Optical Excitations in van der Waals Materials from a Non-Empirical Wannier-Localized Optimally-Tuned Screened Range-Separated Hybrid Functional
Resolving Contradictory Estimates of Band Gaps of Bulk PdSe$_2$: A Wannier-Localized Optimally-Tuned Screened Range-Separated Hybrid Density Functional Theory Study
Use of local density approximation within range separated hybrid exchange-correlation functional to investigate Pb doped SnO$_2$ as an electron transport layer
Accurate and efficient prediction of the band gaps and optical spectra of chalcopyrite semiconductors from a non-empirical range-separated dielectric-dependent hybrid: Comparison with many-body perturbation theory
An Investigation into the Thermoelectric Characteristics of Silver-based Chalcopyrites Utilizing a Non-empirical Range-separated Dielectric-dependent Hybrid Approach
Faster Exact Exchange for Solids via occ-RI-K: Application to Combinatorially Optimized Range-Separated Hybrid Functionals for Simple Solids with Pseudopotentials Near the Basis Set Limit
In this work, we developed and showcased the occ-RI-K algorithm to compute the exact exchange contribution in density functional calculations of solids near the basis set limit. Within the gaussian planewave (GPW) density fitting, our algorithm achieves a 1-2 orders of magnitude speedup compared to conventional GPW algorithms. Since our algorithm is well-suited for simulations with large basis sets, we applied it to 12 hybrid density functionals with pseudopotentials and a large uncontracted basis set to assess their performance on band gaps of 25 simple solids near the basis set limit. The la…
Accurate non-empirical range-separated hybrid van der Waals density functional for complex molecular problems, solids, and surfaces
我们在非经验vdW-DF方法中引入了一种新的通用范围分离混合范德华密度\ph{functional, termed vdW-DF-ahbr,} [JPCM 32，393001（2020）]。它将vdW-DF 2的相关性与由\ph{a new model of exchange effects}在密度显式vdW-DF 2-b86 r函数中固定的筛选Fock交换相结合[PRB 89，121103（R）（2014）]。新的vdW-DF 2-ahbr防止虚假的交换绑定，并有一个小的密度梯度形式集从多体微扰分析。它是准确的\ph{bulk as well as layered materials}，它系统地和显着地提高了目前的vdw-DF的性能的分子问题。重要的是，vdW-DF 2-ahbr也优于目前的标准（色散校正）范围分离的杂交广泛收集的非共价相互作用的基准集，而在同一时间成功地减轻密度驱动的错误，往往影响分子过渡态和异构化计算的描述。vdW-DF 2-ahbr还通过1）正确预测Pt（111）上CO吸附的基底结构和位点偏好，2）在描述CO $_2$在官能化和简单金属-有机骨架中的吸附方面优于现有的非经验vdW-DF，和3）在DNA装配模型中是高度精确的碱基对相互作用的\ph{for the}集合。
Electronic structure and optical properties of halide double perovskites from a Wannier-localized optimally-tuned screened range-separated hybrid functional
MaPBI3 and 2D hybrid organic inorganic perovskite based microcavities employing periodic, aperiodic and disordered photonic structures and with the possibility of light-induced tuning
Fast and Scalable GPU-Accelerated Quantum Chemistry for Periodic Systems with Gaussian Orbitals: Implementation and Hybrid Density Functional Theory Calculations
