Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Fragment approach to constrained density functional theory calculations using Daubechies wavelets

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4922378· OSTI ID:1392510
 [1];  [2];  [2];  [2]
  1. Argonne National Lab. (ANL), Lemont, IL (United States). Argonne Leadership Computing Facility (ALCF); Univ. de Grenoble Alpes (France)
  2. Univ. de Grenoble Alpes (France)
+ Show Author Affiliations
In a recent paper, we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions are optimized in situ and therefore adapted to the chemical properties of the molecular system. Thanks to the systematically controllable accuracy of the underlying basis set, this approach is able to provide an optimal contracted basis for a given system: accuracies for ground state energies and atomic forces are of the same quality as an uncontracted, cubic scaling approach. This basis set offers, by construction, a natural subset where the density matrix of the system can be projected. In this paper, we demonstrate the flexibility of this minimal basis formalism in providing a basis set that can be reused as-is, i.e., without reoptimization, for charge-constrained DFT calculations within a fragment approach. Support functions, represented in the underlying wavelet grid, of the template fragments are roto-translated with high numerical precision to the required positions and used as projectors for the charge weight function. Furthermore, we demonstrate the interest of this approach to express highly precise and efficient calculations for preparing diabatic states and for the computational setup of systems in complex environments.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1392510
Alternate ID(s):
OSTI ID: 22415983
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 23 Vol. 142; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (64)

Density functional theory for systems of very many atoms journal November 1995
Valence and core photoelectron spectroscopy of C60, buckminsterfullerene journal January 1991
Single-photon ionization of C60- and C70-fullerene with synchrotron radiation: determination of the ionization potential of C60 journal January 1992
Structure of C60 fullerene in water: spectroscopic data journal January 2004
Theoretical calculations of the structure and UV–vis absorption spectra of hydrated C60 fullerene journal November 2006
Implicit solvation models in a multiresolution multiwavelet basis journal March 2013
An efficient numerical quadrature for the calculation of the potential energy of wavefunctions expressed in the Daubechies wavelet basis journal September 2006
Toward Fast and Accurate Evaluation of Charge On-Site Energies and Transfer Integrals in Supramolecular Architectures Using Linear Constrained Density Functional Theory (CDFT)-Based Methods journal April 2015
Molecular Interactions in Solution: An Overview of Methods Based on Continuous Distributions of the Solvent journal November 1994
Constrained Density Functional Theory journal November 2011
Constrained Density Functional Theory and Its Application in Long-Range Electron Transfer journal May 2006
Linear Scaling Constrained Density Functional Theory in CONQUEST journal March 2011
Robust and Efficient Constrained DFT Molecular Dynamics Approach for Biochemical Modeling journal January 2012
Failure of Time-Dependent Density Functional Theory for Long-Range Charge-Transfer Excited States:  The Zincbacteriochlorin−Bacteriochlorin and Bacteriochlorophyll−Spheroidene Complexes journal March 2004
Absolute Rates of Hole Transfer in DNA
  • Senthilkumar, Kittusamy; Grozema, Ferdinand C.; Guerra, Célia Fonseca
  • Journal of the American Chemical Society, Vol. 127, Issue 42 https://doi.org/10.1021/ja054257e
journal October 2005
Band Gap and Density of States of the Hydrated C 60 Fullerene System at Finite Temperature journal June 2007
Accurate and efficient linear scaling DFT calculations with universal applicability journal January 2015
C60 fullerene aggregation in aqueous solution journal January 2013
Charge transport in columnar stacked triphenylenes: Effects of conformational fluctuations on charge transfer integrals and site energies journal November 2003
Introducing ONETEP : Linear-scaling density functional simulations on parallel computers journal February 2005
A molecular-dynamics simulation study of solvent-induced repulsion between C60 fullerenes in water journal November 2005
A unified electrostatic and cavitation model for first-principles molecular dynamics in solution journal February 2006
A molecular dynamics simulation study of buckyballs in water: Atomistic versus coarse-grained models of C60 journal July 2006
Extracting electron transfer coupling elements from constrained density functional theory journal October 2006
Daubechies wavelets as a basis set for density functional pseudopotential calculations journal July 2008
Neutral and charged excitations in carbon fullerenes from first-principles many-body theories journal August 2008
Charge constrained density functional molecular dynamics for simulation of condensed phase electron transfer reactions journal January 2009
Electronic coupling matrix elements from charge constrained density functional theory calculations using a plane wave basis set journal December 2010
‘‘Magic number’’ carbon clusters: Ionization potentials and selective reactivity journal March 1991
Density‐functional thermochemistry. III. The role of exact exchange journal April 1993
Efficient and accurate solver of the three-dimensional screened and unscreened Poisson's equation with generic boundary conditions journal October 2012
A challenge for density functionals: Self-interaction error increases for systems with a noninteger number of electrons journal August 1998
High resolution photoelectron spectroscopy of C60− journal May 1999
Molecular dynamics study of self-agglomeration of charged fullerenes in solvents journal January 2013
Daubechies wavelets for linear scaling density functional theory journal May 2014
Nearsightedness of electronic matter journal August 2005
Calculations for millions of atoms with density functional theory: linear scaling shows its potential journal February 2010
Inhomogeneous Electron Gas journal November 1964
Self-Consistent Equations Including Exchange and Correlation Effects journal November 1965
Direct optimization method to study constrained systems within density-functional theory journal August 2005
Self-interaction correction to density-functional approximations for many-electron systems journal May 1981
Relativistic separable dual-space Gaussian pseudopotentials from H to Rn journal August 1998
Constrained-DFT method for accurate energy-level alignment of metal/molecule interfaces journal October 2013
Short-Range to Long-Range Charge-Transfer Excitations in the Zincbacteriochlorin-Bacteriochlorin Complex: A Bethe-Salpeter Study journal October 2012
Ground State of the Electron Gas by a Stochastic Method journal August 1980
Density-Functional Theory for Time-Dependent Systems journal March 1984
Ground States of Constrained Systems: Application to Cerium Impurities journal December 1984
Density Functional and Density Matrix Method Scaling Linearly with the Number of Atoms journal April 1996
Sparsity of the Density Matrix in Kohn-Sham Density Functional Theory and an Assessment of Linear System-Size Scaling Methods journal November 1997
Locality of the Density Matrix in Metals, Semiconductors, and Insulators journal March 1999
Exponential Decay Properties of Wannier Functions and Related Quantities journal June 2001
Density-functional theory for time-dependent systems journal January 1987
Inhomogeneous Electron Gas journal March 1973
A discussion of the solution for the best rotation to relate two sets of vectors journal September 1978
Ten Lectures on Wavelets book January 1992
A Least Squares Estimate of Satellite Attitude journal July 1965
Minimal parameter implicit solvent model for ab initio electronic-structure calculations journal July 2011
Exponential Decay Properties of Wannier Functions and Related Quantities text January 2001
Daubechies wavelets as a basis set for density functional pseudopotential calculations text January 2008
Efficient and accurate solver of the three-dimensional screened and unscreened Poisson's equation with generic boundary conditions text January 2012
Constrained-DFT method for accurate energy level alignment of metal/molecule interfaces text January 2013
Accurate and efficient linear scaling DFT calculations with universal applicability text January 2015
Nearsightedness of Electronic Matter text January 2005
A unified electrostatic and cavitation model for first-principles molecular dynamics in solution text January 2005

Cited By (5)

Molecular dynamics and charge transport in organic semiconductors: a classical approach to modeling electron transfer journal January 2017
Linear scaling DFT calculations for large Tungsten systems using an optimized local basis text January 2017
Challenges in large scale quantum mechanical calculations: Challenges in large scale quantum mechanical calculations journal November 2016
Optimization of constrained density functional theory journal July 2016
Challenges in Large Scale Quantum Mechanical Calculations text January 2016

Similar Records

Fragment approach to constrained density functional theory calculations using Daubechies wavelets
Journal Article · Sun Jun 21 00:00:00 EDT 2015 · Journal of Chemical Physics · OSTI ID:22415983
Daubechies wavelets for linear scaling density functional theory
Journal Article · Wed May 28 00:00:00 EDT 2014 · Journal of Chemical Physics · OSTI ID:22304330
Periodized Daubechies wavelets
Technical Report · Thu Feb 29 23:00:00 EST 1996 · OSTI ID:211651

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY