.png){kind=icon}
返回
Pushing the limits: Efficient wavefunction methods for excited states in complex systems using frozen-density embedding
.png){kind=icon}
PRE
AI
DOI：10.1063/5.0100393.png)
.png){kind=icon}
原文求助.png){kind=icon}
分享.png){kind=icon}
收藏
摘要
En 中文
Frozen density embedding (FDE) is an embedding method for complex environments that is simple for users to set up. It reduces the computation time by dividing the total system into small subsystems and approximating the interaction by a functional of their densities. Its combination with wavefunction methods is, however, limited to small- or medium-sized molecules because of the steep scaling in computation time of these methods. To mitigate this limitation, we present a combination of the FDE approach with pair natural orbitals (PNOs) in the TURBOMOLE software package. It combines the uncoupled FDE (FDEu) approach for excitation energy calculations with efficient implementations of second-order correlation methods in the ricc2 and pnoccsd programs. The performance of this combination is tested for tetraazaperopyrene (TAPP) molecular crystals. It is shown that the PNO truncation error on environment-induced shifts is significantly smaller than the shifts themselves and, thus, that the local approximations of PNO-based wavefunction methods can without the loss of relevant digits be combined with the FDE method. Computational wall times are presented for two TAPP systems. The scaling of the wall times is compared to conventional supermolecular calculations and demonstrates large computational savings for the combination of FDE-and PNO-based methods. Additionally, the behavior of excitation energies with the system size is investigated. It is found that the excitation energies converge quickly with the size of the embedding environment for the TAPPs investigated in the current study.
Keyword:
CONSTRAINED ELECTRON-DENSITY
KOHN-SHAM EQUATIONS
BASIS-SETS
RESPONSE THEORY
KINETIC-ENERGY
APPROXIMATION
SIMULATIONS
MOLECULES
CONTINUUM
VALENCE
期刊
IF:
3.1
论文数:
7.2W
被引数:
23.2W
机构
引用论文
Self-assembly of five new organic–inorganic hybrids based on two new flexible tricationic templates基于两个新的柔性三阳离子模板的五个新的有机-无机杂化物的自组装
.png){kind=icon}
PREAI
分享收藏Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases用于精确计算气相和凝聚相分子系统的高斯基集
OAAI
OAAI分享收藏Assessment of the Perdew-Burke-Ernzerhof exchange-correlation functionalPerdew-burke-ernzerhof交换相关功能的评估
PREAI
分享收藏Coupled cluster response theory for solvated molecules in equilibrium and nonequilibrium solvation
PREAI
分享收藏A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu94元素h-pu的密度泛函色散校正 (dft-d) 的一致且精确的从头算参数化
PREAI
分享收藏
查看更多内容