We present a density fitted local configuration interaction singles (CIS) method for calculating optical bandgaps in 3D-periodic systems. We employ an Ewald technique to carry out infinite lattice summations for the exciton-exciton interaction, and robust product-density specific local density fitting in direct space for the electron-hole interaction. Moreover, we propose an alternative to the usual cyclic model with Born-von Karman periodic boundary conditions, the so called Wigner-Seitz supercell truncated infinite model, which exhibits much improved convergence of the CIS excitation energy with respect to the size of the supercell. Test calculations on a series of prototypical systems demonstrate that the method at the present stage can be used to calculate the excitonic bandgaps of 3D periodic systems with up to a dozen atoms in the unit cell, ranging from wide-gap insulators to semiconductors.

Local ab initio methods for calculating optical bandgaps in periodic systems. II. Periodic density fitted local configuration interaction singles method for solids

MASCHIO, LORENZO;
2012

Abstract

We present a density fitted local configuration interaction singles (CIS) method for calculating optical bandgaps in 3D-periodic systems. We employ an Ewald technique to carry out infinite lattice summations for the exciton-exciton interaction, and robust product-density specific local density fitting in direct space for the electron-hole interaction. Moreover, we propose an alternative to the usual cyclic model with Born-von Karman periodic boundary conditions, the so called Wigner-Seitz supercell truncated infinite model, which exhibits much improved convergence of the CIS excitation energy with respect to the size of the supercell. Test calculations on a series of prototypical systems demonstrate that the method at the present stage can be used to calculate the excitonic bandgaps of 3D periodic systems with up to a dozen atoms in the unit cell, ranging from wide-gap insulators to semiconductors.
137
204119
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http://jcp.aip.org/resource/1/jcpsa6/v137/i20/p204119_s1
ab initio calculations; convergence; density functional theory; electron-hole recombination; excitons; optical constants; periodic structures
Marco Lorenz; Lorenzo Maschio; Martin Schütz; Denis Usvyat
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2318/126972
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