VeloxChem: Large-Scale DFT Calculations of Geometric Derivatives up to Second Order for Simulation of IR Spectra
Josefine H. Andersen, Iulia Emilia Brumboiu, Manuel Hodecker, Xin Li, Patrick Norman, Zilvinas Rinkevicius
TL;DR
VeloxChem enables efficient large-scale DFT calculations for simulating IR spectra, including second-order geometric derivatives and GPU acceleration.
Contribution
Implementation of analytic second-order geometric derivatives for IR spectra simulations in DFT using GPU acceleration and efficient parallelization.
Findings
Gradient calculations scale efficiently and are computationally cheaper than SCF optimizations.
Hessian calculations scale as N^3.5 and benefit from GPU acceleration for solving perturbed Kohn–Sham equations.
Successful simulation of IR spectrum for ubiquitin with 1,152 atoms shows excellent agreement with experimental amide I band.
Abstract
A software implementation of analytic geometric derivatives of electron-repulsion integrals up to second order is presented for the modeling of vibrational spectroscopies at the level of first-principles Kohn–Sham density functional theory (DFT). In line with the general goals of the VeloxChem program, it targets efficient execution in high-performance computing environments with a hybrid MPI/OpenMP parallelization model and is based on the technique of automatic C++ code generation for high versatility. Gradient calculations scale identically with conventional Fock matrix constructions, and also with the prefactor taken into account, the computational cost of the gradient is significantly lower than that of the self-consistent field (SCF) optimization of the reference state. The Hessian calculation shows a scaling of N 3.5 with N being the number of contracted Gaussian basis functions.…
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Taxonomy
TopicsSpectroscopy and Quantum Chemical Studies · Advanced Chemical Physics Studies · Photosynthetic Processes and Mechanisms