Electron dynamics in extended systems within real-time time-dependent density-functional theory

被引:25
作者
Kononov, Alina [1 ]
Lee, Cheng-Wei [2 ]
dos Santos, Tatiane Pereira [3 ]
Robinson, Brian [3 ]
Yao, Yifan [3 ]
Yao, Yi [4 ,5 ]
Andrade, Xavier [6 ]
Baczewski, Andrew David [1 ]
Constantinescu, Emil [7 ]
Correa, Alfredo A. [6 ]
Kanai, Yosuke [5 ]
Modine, Normand [8 ]
Schleife, Andre [3 ,9 ,10 ]
机构
[1] Sandia Natl Labs, Ctr Comp Res, Albuquerque, NM 87123 USA
[2] Colorado Sch Mines, Golden, CO 80401 USA
[3] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA
[4] Duke Univ, Thomas Lord Dept Mech Engn & Mat Sci, Durham, NC 27708 USA
[5] Univ N Carolina, Dept Chem, Chapel Hill, NC 27595 USA
[6] Lawrence Livermore Natl Lab, Quantum Simulat Grp, Livermore, CA 94551 USA
[7] Argonne Natl Lab, Math & Comp Sci, Lemont, IL 60439 USA
[8] Sandia Natl Labs, Mat Phys & Chem Sci Ctr, Albuquerque, NM 87123 USA
[9] Univ Illinois, Mat Res Lab, Urbana, IL 61801 USA
[10] Univ Illinois, Natl Ctr Supercomp Applicat, Urbana, IL 61801 USA
基金
美国国家科学基金会;
关键词
SPACE; IMPLEMENTATION; SIMULATION; LIFETIMES;
D O I
10.1557/s43579-022-00273-7
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
Due to a beneficial balance of computational cost and accuracy, real-time time-dependent density-functional theory has emerged as a promising first-principles framework to describe electron real-time dynamics. Here we discuss recent implementations around this approach, in particular in the context of complex, extended systems. Results include an analysis of the computational cost associated with numerical propagation and when using absorbing boundary conditions. We extensively explore the shortcomings for describing electron-electron scattering in real time and compare to many-body perturbation theory. Modern improvements of the description of exchange and correlation are reviewed. In this work, we specifically focus on the Qb@ll code, which we have mainly used for these types of simulations over the last years, and we conclude by pointing to further progress needed going forward.
引用
收藏
页码:1002 / 1014
页数:13
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