Linear-response time-dependent density functional theory approach to warm dense matter with adiabatic exchange-correlation kernels
Linear-response time-dependent density functional theory approach to warm dense matter with adiabatic exchange-correlation kernels
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DOI：
10.1103/physrevresearch.5.023089
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发表时间：
2023-02
影响因子：
4.2
通讯作者：
Z. Moldabekov;M. Pavanello;Maximilian P. Boehme;J. Vorberger;T. Dornheim
中科院分区：
文献类型：
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作者：
Z. Moldabekov;M. Pavanello;Maximilian P. Boehme;J. Vorberger;T. Dornheim
我们提出了一种用于在绝热近似下计算温稠密物质动态密度响应函数的线性响应含时密度泛函理论（LR - TDDFT）的新方法，该方法可与雅各布天梯（Jacob's Ladder）上任何可用的交换关联（XC）泛函以及不同温度范围一起使用。所提出方法的主要新颖之处在于，它能够超越绝热局域密度近似（ALDA）和广义局域密度近似（AGGA），同时在扩展体系中保持科恩 - 沈（Kohn - Sham，KS）响应函数与绝热XC核之间的自洽性。所提出方法的关键要素是将直接微扰方法中的绝热XC核与使用KS轨道的标准LR - TDDFT方法中的宏观动态KS响应相结合。我们以温稠密氢为例展示了该方法的应用，并对KS密度响应函数、无规相近似（RPA）结果、总密度响应函数以及绝热XC核进行了详细分析。该分析使用了针对XC效应的局域密度近似（LDA）、广义梯度近似（GGA）和超广义梯度近似（meta - GGA）层级的近似。所提出的方法可直接应用于无序体系，如液态金属、温稠密物质和稠密等离子体。
We present a new methodology for the linear-response time-dependent density functional theory (LR-TDDFT) calculation of the dynamic density response function of warm dense matter in an adiabatic approximation that can be used with any available exchange-correlation (XC) functional across Jacob's Ladder and across temperature regimes. The main novelty of the presented approach is that it can go beyond the adiabatic local density approximation (ALDA) and generalized LDA (AGGA) while preserving the self-consistence between the Kohn-Sham (KS) response function and adiabatic XC kernel for extended systems. The key ingredient for the presented method is the combination of the adiabatic XC kernel from the direct perturbation approach with the macroscopic dynamic KS response from the standard LR-TDDFT method using KS orbitals. We demonstrate the application of the method for the example of warm dense hydrogen, for which we perform a detailed analysis of the KS density response function, the RPA result, the total density response function and of the adiabatic XC kernel. The analysis is performed using LDA, GGA, and meta-GGA level approximations for the XC effects. The presented method is directly applicable to disordered systems such as liquid metals, warm dense matter, and dense plasmas.