We have implemented pseudospectral density-functional theory (DFT) with long-range corrected DFT functionals (PS-LRC) in quantum mechanics package Jaguar, and applied it in the calculations of geometry optimizations, dimmer interaction energies, polarizabilities and first-order hyperpolarizabilities, harmonic vibrational frequencies, S₁ and T₁ excitation energies, singlet-triplet gaps, charge transfer numbers, oscillator strengths, reaction barrier heights, electron-transfer couplings, and charge-transfer excitation energies. From our accuracy benchmark analysis, PS grids, PS dealiasing functions, PS atomic corrections, PS multigrid strategy, PS length scales, and PS cutoff scheme perform well in PS DFT with LRC density functionals with very small and ignorable deviations when compared to the conventional spectral (CS) method. The timing benchmark study of S₁ excitation energy calculations of fullerenes (C_n, n up to 540) demonstrates that PS-LRC achieves 1.4–8.4-fold speedups in SCF, 22–32-fold speedups in Tamm-Dancoff approximation, and 6–15-fold speedups in total wall clock time with an average error 0.004 eV of excitation energies compared to the CS method.

中文翻译：

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长程校正密度泛函理论的伪谱实现

我们在量子力学包 Jaguar 中实现了具有长程校正 DFT 泛函 (PS-LRC) 的伪谱密度泛函理论 (DFT)，并将其应用于几何优化、调光相互作用能、极化率和一阶超极化率的计算，谐波振动频率，S ₁和 T ₁激发能、单线态-三线态间隙、电荷转移数、振荡器强度、反应势垒高度、电子转移耦合和电荷转移激发能。从我们的精度基准分析来看，PS 网格、PS 去混叠函数、PS 原子校正、PS 多重网格策略、PS 长度尺度和 PS 截止方案在具有 LRC 密度函数的 PS DFT 中表现良好，与传统光谱相比，具有非常小且可忽略的偏差(CS) 方法。富勒烯( C _n , n ) S ₁激发能计算的时序基准研究 高达 540）表明 PS-LRC 在 SCF 中实现了 1.4-8.4 倍的加速，在 Tamm-Dancoff 近似中实现了 22-32 倍的加速，以及在总挂钟时间上实现了 6-15 倍的加速，平均误差为 0.004 eV激发能量与 CS 方法相比。