English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

All-electron, real-space perturbation theory for homogeneous electric fields: theory, implementation, and application within DFT

MPS-Authors
/persons/resource/persons39373

Shang,  Honghui
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons200437

Raimbault,  Nathaniel
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22064

Scheffler,  Matthias
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21421

Rossi,  Mariana
Theory, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21413

Carbogno,  Christian
Theory, Fritz Haber Institute, Max Planck Society;

External Resource
No external resources are shared
Fulltext (restricted access)
There are currently no full texts shared for your IP range.
Fulltext (public)

Shang_2018_New_J._Phys._20_073040.pdf
(Publisher version), 2MB

Supplementary Material (public)
There is no public supplementary material available
Citation

Shang, H., Raimbault, N., Rinke, P., Scheffler, M., Rossi, M., & Carbogno, C. (2018). All-electron, real-space perturbation theory for homogeneous electric fields: theory, implementation, and application within DFT. New Journal of Physics, 20(7): 073040. doi:10.1088/1367-2630/aace6d.


Cite as: https://hdl.handle.net/21.11116/0000-0001-E7B6-D
Abstract
Within density-functional theory, perturbation theory (PT) is the state-of-the-art formalism for assessing the response to homogeneous electric fields and the associated material properties, e.g., polarizabilities, dielectric constants, and Raman intensities. Here, we derive a real-space formulation of PT and present an implementation within the all-electron, numeric atom-centered orbitals electronic structure code FHI-aims that allows for massively parallel calculations. As demonstrated by extensive validation, we achieve a rapid computation of accurate response properties of molecules and solids. As an application showcase, we present harmonic and anharmonic Raman spectra, the latter obtained by combining hundreds of thousands of PT calculations with ab initio molecular dynamics. By using the PBE exchange-correlation functional with many-body van der Waals corrections, we obtain spectra in good agreement with experiment especially with respect to lineshapes for the isolated paracetamol molecule and two polymorphs of the paracetamol crystal.