title: Anharmonic Infrared Spectroscopy through the Fourier Transform of Time Correlation Function Formalism in ONETEP.
abstract: Density functional theory molecular dynamics (DFT-MD) provides an efficient framework for accurately computing several types of spectra. The major benefit of DFT-MD approaches lies in the ability to naturally take into account the effects of temperature and anharmonicity, without having to introduce any ad hoc or a posteriori corrections. Consequently, computational spectroscopy based on DFT-MD approaches plays a pivotal role in the understanding and assignment of experimental peaks and bands at finite temperature, particularly in the case of floppy molecules. Linear-scaling DFT methods can be used to study large and complex systems, such as peptides, DNA strands, amorphous solids, and molecules in solution. Here, we present the implementation of DFT-MD IR spectroscopy in the ONETEP linear-scaling code. In addition, two methods for partitioning the dipole moment within the ONETEP framework are presented. Dipole moment partitioning allows us to compute spectra of molecules in solution, which fully include the effects of the solvent, while at the same time removing the solvent contribution from the spectra.
authors.affiliation: School of Chemistry, University of Southampton , Southampton, United Kingdom.|Institute of Complex Systems Simulation, University of Southampton , Southampton, United Kingdom.
authors.forename: Valerio
authors.initials: V
authors.lastname: Vitale
authors.affiliation: School of Chemistry, University of Southampton , Southampton, United Kingdom.|Faculty of Applied Physics and Mathematics, Gdańsk University of Technology , Gdańsk, Poland.
authors.forename: Jacek
authors.initials: J
authors.lastname: Dziedzic
authors.affiliation: Institut de la Matière Condenseée et des Nanosciences, Universitè Catholique de Louvain B-1348 Louvain-la-Neuve, Belgium.
authors.forename: Simon M-M
authors.initials: SM
authors.lastname: Dubois
authors.affiliation: Engineering and the Environment, University of Southampton , Southampton, United Kingdom.|Institute of Complex Systems Simulation, University of Southampton , Southampton, United Kingdom.
authors.forename: Hans
authors.initials: H
authors.lastname: Fangohr
authors.affiliation: School of Chemistry, University of Southampton , Southampton, United Kingdom.
authors.forename: Chris-Kriton
authors.initials: CK
authors.lastname: Skylaris