Petascale Orbital-Free Density Functional Theory Enabled by Small-Box Algorithms

详细信息    查看全文

• 作者：Mohan Chen ; Xiang-Wei Jiang ; Houlong Zhuang ; Lin-Wang Wang ; Emily A. Carter
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2016
• 出版时间：June 14, 2016
• 年：2016
• 卷：12
• 期：6
• 页码：2950-2963
• 全文大小：699K
• 年卷期：0
• ISSN：1549-9626

文摘

Orbital-free density functional theory (OFDFT) is a quantum-mechanics-based method that utilizes electron density as its sole variable. The main computational cost in OFDFT is the ubiquitous use of the fast Fourier transform (FFT), which is mainly adopted to evaluate the kinetic energy density functional (KEDF) and electron–electron Coulomb interaction terms. We design and implement a small-box FFT (SBFFT) algorithm to overcome the parallelization limitations of conventional FFT algorithms. We also propose real-space truncation of the nonlocal Wang–Teter KEDF kernel. The scalability of the SBFFT is demonstrated by efficiently simulating one full optimization step (electron density, energies, forces, and stresses) of 1,024,000 lithium (Li) atoms on up to 65,536 cores. We perform other tests using Li as a test material, including calculations of physical properties of different phases of bulk Li, geometry optimizations of nanocrystalline Li, and molecular dynamics simulations of liquid Li. All of the tests yield excellent agreement with the original OFDFT results, suggesting that the OFDFT-SBFFT algorithm opens the door to efficient first-principles simulations of materials containing millions of atoms.