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Title: VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments

Abstract

An open-source program named VeloxChem has been developed for the calculation of electronic real and complex linear response functions at the levels of Hartree–Fock and Kohn–Sham density functional theories. With an object-oriented program structure written in a Python/C++ layered fashion, VeloxChem enables time-efficient prototyping of novel scientific approaches without sacrificing computational efficiency, so that molecular systems involving up to and beyond 500 second-row atoms (or some 10,000 contracted and in part diffuse Gaussian basis functions) can be routinely addressed. In addition, VeloxChem is equipped with a polarizable embedding scheme for the treatment of the classical electrostatic interactions with an environment that in turn is modeled by atomic site charges and polarizabilities. The underlying hybrid message passing interface (MPI)/open multiprocessing (OpenMP) parallelization scheme makes VeloxChem suitable for execution in high-performance computing cluster environments, showing even slightly beyond linear scaling for the Fock matrix construction with use of up to 16,384 central processing unit (CPU) cores. An efficient—with respect to convergence rate and overall computational cost—multifrequency/gradient complex linear response equation solver enables calculations not only of conventional spectra, such as visible/ultraviolet/X-ray electronic absorption and circular dichroism spectra, but also time-resolved linear response signals as due to ultra-short weak laser pulses.

Authors:
 [1];  [2];  [2];  [2]; ORCiD logo [2];  [2];  [3];  [4];  [4];  [4]; ORCiD logo [2]
  1. KTH Royal Inst. of Technology, Stockholm (Sweden); Kaunas Univ. of Technology (Lithuania)
  2. KTH Royal Inst. of Technology, Stockholm (Sweden)
  3. Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  4. Ruprecht‐Karls Univ., Heidelberg (Germany)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1591634
Grant/Contract Number:  
AC02-76SF00515; COSINE; 274918; 2018‐4343; VKR023371
Resource Type:
Accepted Manuscript
Journal Name:
Wiley Interdisciplinary Reviews: Computational Molecular Science
Additional Journal Information:
Journal Name: Wiley Interdisciplinary Reviews: Computational Molecular Science; Journal ID: ISSN 1759-0876
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
circular dichroism; density functional theory (DFT); ECD; high‐performance computing (HPC); MPI; OpenMP; response theory; UV/vis

Citation Formats

Rinkevicius, Zilvinas, Li, Xin, Vahtras, Olav, Ahmadzadeh, Karan, Brand, Manuel, Ringholm, Magnus, List, Nanna Holmgaard, Scheurer, Maximilian, Scott, Mikael, Dreuw, Andreas, and Norman, Patrick. VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments. United States: N. p., 2019. Web. doi:10.1002/wcms.1457.
Rinkevicius, Zilvinas, Li, Xin, Vahtras, Olav, Ahmadzadeh, Karan, Brand, Manuel, Ringholm, Magnus, List, Nanna Holmgaard, Scheurer, Maximilian, Scott, Mikael, Dreuw, Andreas, & Norman, Patrick. VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments. United States. doi:10.1002/wcms.1457.
Rinkevicius, Zilvinas, Li, Xin, Vahtras, Olav, Ahmadzadeh, Karan, Brand, Manuel, Ringholm, Magnus, List, Nanna Holmgaard, Scheurer, Maximilian, Scott, Mikael, Dreuw, Andreas, and Norman, Patrick. Wed . "VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments". United States. doi:10.1002/wcms.1457. https://www.osti.gov/servlets/purl/1591634.
@article{osti_1591634,
title = {VeloxChem: A Python-driven density-functional theory program for spectroscopy simulations in high-performance computing environments},
author = {Rinkevicius, Zilvinas and Li, Xin and Vahtras, Olav and Ahmadzadeh, Karan and Brand, Manuel and Ringholm, Magnus and List, Nanna Holmgaard and Scheurer, Maximilian and Scott, Mikael and Dreuw, Andreas and Norman, Patrick},
abstractNote = {An open-source program named VeloxChem has been developed for the calculation of electronic real and complex linear response functions at the levels of Hartree–Fock and Kohn–Sham density functional theories. With an object-oriented program structure written in a Python/C++ layered fashion, VeloxChem enables time-efficient prototyping of novel scientific approaches without sacrificing computational efficiency, so that molecular systems involving up to and beyond 500 second-row atoms (or some 10,000 contracted and in part diffuse Gaussian basis functions) can be routinely addressed. In addition, VeloxChem is equipped with a polarizable embedding scheme for the treatment of the classical electrostatic interactions with an environment that in turn is modeled by atomic site charges and polarizabilities. The underlying hybrid message passing interface (MPI)/open multiprocessing (OpenMP) parallelization scheme makes VeloxChem suitable for execution in high-performance computing cluster environments, showing even slightly beyond linear scaling for the Fock matrix construction with use of up to 16,384 central processing unit (CPU) cores. An efficient—with respect to convergence rate and overall computational cost—multifrequency/gradient complex linear response equation solver enables calculations not only of conventional spectra, such as visible/ultraviolet/X-ray electronic absorption and circular dichroism spectra, but also time-resolved linear response signals as due to ultra-short weak laser pulses.},
doi = {10.1002/wcms.1457},
journal = {Wiley Interdisciplinary Reviews: Computational Molecular Science},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {12}
}

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