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使用从头算、基于密度泛函理论(DFT)和半经验方法对C富勒烯中的高次谐波产生进行建模。

Modeling of High-Harmonic Generation in the C Fullerene Using Ab Initio, DFT-Based, and Semiempirical Methods.

作者信息

Woźniak Aleksander P, Moszyński Robert

机构信息

Faculty of Chemistry, University of Warsaw, Pasteura 1, Warsaw 02-093, Poland.

出版信息

J Phys Chem A. 2024 Apr 11;128(14):2683-2702. doi: 10.1021/acs.jpca.3c07865. Epub 2024 Mar 27.

Abstract

We report calculations of the high-harmonic generation spectra of the C fullerene molecule carried out by employing a diverse set of real-time time-dependent quantum chemical methods. All methodologies involve expanding the propagated electronic wave function in bases consisting of the ground and singly excited time-independent eigenstates obtained through the solution of the corresponding linear-response equations. We identify the correlation and exchange effect in the spectra by comparing the results from methods relying on the Hartree-Fock reference determinant with those obtained using approaches based on the density functional theory with different exchange-correlation functionals. The effect of the full random-phase approximation treatment of the excited electronic states is also analyzed and compared with the configuration interaction singles and the Tamm-Dancoff approximation. We also showcase the fact that the real-time extension of the semiempirical method INDO/S can be effectively applied for an approximate description of laser-driven dynamics in large systems.

摘要

我们报告了通过采用多种实时含时量子化学方法对C富勒烯分子的高次谐波产生光谱进行的计算。所有方法都涉及在由通过求解相应线性响应方程获得的基态和单激发非含时本征态组成的基组中展开传播的电子波函数。我们通过比较基于Hartree-Fock参考行列式的方法与使用基于不同交换相关泛函的密度泛函理论的方法所得到的结果,来确定光谱中的关联和交换效应。还分析了对激发电子态进行完全随机相位近似处理的效果,并与组态相互作用单重态和Tamm-Dancoff近似进行了比较。我们还展示了半经验方法INDO/S的实时扩展可以有效地应用于对大型系统中激光驱动动力学的近似描述这一事实。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/fe5e/11017253/12a78dee9bb6/jp3c07865_0001.jpg

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