Quantum Chemistry on Graphical Processing Units. 2. Direct Self-Consistent-Field Implementation.

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• High-Performance Computing

Background:

• Self-consistent-field (SCF) calculations are fundamental in quantum chemistry for determining molecular electronic structure.
• Scaling SCF calculations to large molecular systems (e.g., >400 atoms) presents significant computational challenges on traditional hardware.
• Existing quantum chemistry software often relies on central processing units (CPUs), limiting computational speed for complex problems.

Purpose of the Study:

• To demonstrate the efficacy of graphical processing units (GPUs) for accelerating complete SCF calculations.
• To assess the performance gains of GPU-accelerated SCF methods compared to established CPU-based quantum chemistry programs.
• To explore parallelization strategies for SCF calculations on multiple GPUs.

Main Methods:

• Implementation of SCF calculations utilizing GPU hardware for accelerating computationally intensive steps.
• Comparison of GPU-based SCF performance against the GAMESS quantum chemistry program running on CPUs.
• Development and application of both coarse-grained and fine-grained parallelism across three GPUs.

Main Results:

• Achieved substantial speedups, ranging from 28x to 650x, for SCF calculations on molecules up to 453 atoms (2131 basis functions).
• Demonstrated the feasibility of complete SCF calculations on large molecular systems using GPUs.
• Successfully implemented parallel SCF calculations across multiple GPUs, combining different parallelism strategies.

Conclusions:

• GPUs offer a powerful and efficient platform for accelerating quantum chemistry calculations, particularly SCF methods.
• GPU acceleration significantly reduces the computational time for large molecular systems, enabling larger and more complex studies.
• Parallel GPU computing architectures provide a viable approach for further enhancing computational throughput in theoretical chemistry.