A Unified Heterogeneous Implementation of Numerical Atomic Orbitals-Based Real-Time TDDFT within the ABACUS Package

Abstract

We present a unified heterogeneous computing framework for real-time time-dependent density functional theory (RT-TDDFT) based on numerical atomic orbitals (NAOs), implemented in the ABACUS package. We introduce three co-designed abstraction layers, including unified data containers, unified linear algebra operators, and unified grid integration interfaces. These layers collectively accelerate the two most demanding parts of NAO-based RT-TDDFT: explicit real-time wavefunction propagation and real-space grid operations such as Hamiltonian construction and force evaluation under external fields. We validate the method by computing optical properties for systems ranging from finite molecules to periodic solids, showing excellent agreement with standard benchmarks. Performance evaluations on bulk silicon demonstrate that a single GPU can achieve substantial wall-clock speedup over a fully utilized dual-socket CPU node. Furthermore, distributed multi-GPU strong-scaling tests confirm high parallel efficiency over tens of GPUs. This work establishes a high-performance, portable platform for large-scale first-principles simulations of ultrafast electron dynamics.

References in corpus (20)

• CP2K: An Electronic Structure and Molecular Dynamics Software Package -- Quickstep: Efficient and Accurate Electronic Structure Calculations
• Optimized norm-conserving Vanderbilt pseudopotentials
• Quantum ESPRESSO toward the exascale
• Optimization Algorithm for the Generation of ONCV Pseudopotentials
• Recent developments in the PySCF program package
• Real-space grids and the Octopus code as tools for the development of new simulation approaches for electronic systems
• Impact of the electronic band structure in high-harmonic generation spectra of solids
• GPAW: An open Python package for electronic-structure calculations
• Adaptive local basis set for Kohn-Sham density functional theory in a discontinuous Galerkin framework I: Total energy calculation
• DGDFT: A Massively Parallel Method for Large Scale Density Functional Theory Calculations
• Accurate ionic forces and geometry optimisation in linear scaling density-functional theory with local orbitals
• Velocity-gauge real-time TDDFT within a numerical atomic orbital basis set
• Coupling of Nonlocal Potentials to Electromagnetic Fields
• Nonadiabatic Ehrenfest molecular dynamics within the projector augmented-wave method
• $\text{Ab initio}$ evidence for nonthermal characteristics in ultrafast laser melting
• Cooperative evolution of intraband and interband excitations for high harmonic generation in strained MoS2
• Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory
• Ab initio simulation of attosecond transient absorption spectroscopy in two-dimensional materials
• All-electron full-potential implementation of real-time TDDFT in exciting
• GPU Acceleration of Collinear and Noncollinear DFT Using a Numerical Atomic Orbital-Based DFT Code