Real-Time Extension of TAO-DFT

• Published in: Molecules Vol. 28; no. 21; p. 7247
• Main Authors: Tsai, Hung-Yi, Chai, Jeng-Da
• Format: Journal Article
• Language: English
• Published: Basel MDPI AG 01.11.2023
• Subjects: Accuracy; Approximation; Density functionals; Electrons; Energy; Equilibrium; high-order harmonic generation; multi-reference character; real-time electron dynamics; RT-TAO-DFT; TAO-DFT; time-dependent properties
• ISSN: 1420-3049; 1433-1373; 1420-3049; 1433-1373
• DOI: 10.3390/molecules28217247

Thermally assisted occupation density functional theory (TAO-DFT) has been an efficient electronic structure method for studying the ground-state properties of large electronic systems with multi-reference character over the past few years. To explore the time-dependent (TD) properties of electronic systems (e.g., subject to an intense laser pulse), in this work, we propose a real-time (RT) extension of TAO-DFT, denoted as RT-TAO-DFT. Moreover, we employ RT-TAO-DFT to study the high-order harmonic generation (HHG) spectra and related TD properties of molecular hydrogen H2 at the equilibrium and stretched geometries, aligned along the polarization of an intense linearly polarized laser pulse. The TD properties obtained with RT-TAO-DFT are compared with those obtained with the widely used time-dependent Kohn–Sham (TDKS) method. In addition, issues related to the possible spin-symmetry breaking effects in the TD properties are discussed.