Vibrational Spectroscopy

Vibrational Spectroscopy

In my research, I am developing methods to predict vibrational spectra of condensed phase systems from ab initio simulations (no empirical parameters or experimental input required). During the last years, my co-workers and me were able to publish the first-ever ab initio pre­diction of a liquid phase Raman Optical Activity (ROA) spectrum as well as of a liquid phase resonance Raman spectrum, which are both based on novel approaches we have developed.

Are you interested in the algorithms behind computing spectra from molecular dynamics simulations? Some of them are explained in Section V of our recent open access article about the TRAVIS program package. Please have a look:

M. Brehm, M. Thomas, S. Gehrke, B. Kirchner:
“TRAVIS – A Free Analyzer for Trajectories from Molecular Simulation”,
J. Chem. Phys. 2020, 152 (16), 164105, DOI 10.1063/5.0005078.

Our methods for computing spectra rely heavily on the Voronoi integration approach which we have developed in 2015. It yields molecular electromagnetic properties (such as the electric dipole vector) via integration of the total electron density within Voronoi cells.

Tutorial on Computing Spectra

Below, I present a new version of our tutorial on computing vibrational spectra of bulk phase systems with CP2k and TRAVIS. The tutorial gives a step-by-step explanation of how to install the software, decide for a system, and compute the infrared, Raman, VCD, and ROA spectra on the basis of AIMD simulations. Please download:

FileType / SizeLast Changed
Computing Bulk Phase Vibrational Spectra with CP2k and TRAVIS (2018) .pdf, 2.1 MiB Oct 22 2018
Collection of input files
from the appendix
.tar.gz, 6.3 kiB Oct 22 2018
Slides from my presentation
in Paderborn (Aug 2018)
.pdf, 7.6 MiB Aug 29 2018

An updated version of the tutorial which also covers our newly published method to predict resonance Raman spectra will be uploaded in the next weeks.

Please also see the homepage of the bqb file format and bqbtool.

— Related Publications —

8 of my publications are related to vibrational spectroscopy:

40M. Brehm, M. Thomas, S. Gehrke, B. Kirchner:
"TRAVIS – A Free Analyzer for Trajectories from Molecular Simulation"
J. Chem. Phys. 2020, 152 (16), 164105.     (16 citations, DOI 10.1063/5.0005078 ) ⭳Bib
Open Access
36M. Brehm, M. Thomas:
"Computing Bulk Phase Resonance Raman Spectra from ab initio Molecular Dynamics and Real-Time TDDFT"
J. Chem. Theory Comput. 2019, 15 (7), 3901–3905.     (3 citations, DOI 10.1021/acs.jctc.9b00512 ) ⭳Bib
31M. Brehm, D. Sebastiani:
"Simulating Structure and Dynamics in Small Droplets of 1-Ethyl-3-Methylimidazolium Acetate"
J. Chem. Phys. 2018, 148, 193802.     (12 citations, DOI 10.1063/1.5010342 ) ⭳Bib
26M. Brehm, M. Thomas:
"Computing Bulk Phase Raman Optical Activity Spectra from ab initio Molecular Dynamics Simulations"
J. Phys. Chem. Lett. 2017, 8 (14), 3409–3414.     (10 citations, DOI 10.1021/acs.jpclett.7b01616 ) ⭳Bib
23M. Thomas, M. Brehm, B. Kirchner:
"Voronoi Dipole Moments for the Simulation of Bulk Phase Vibrational Spectra"
Phys. Chem. Chem. Phys. 2015, 17, 3207–3213.     (49 citations, DOI 10.1039/C4CP05272B ) ⭳Bib
19M. Thomas, M. Brehm, O. Hollóczki, Z. Kelemen, L. Nyulászi, T. Pasinszki, B. Kirchner:
"Simulating the Vibrational Spectra of Ionic Liquid Systems: 1-Ethyl-3-Methylimidazolium Acetate and its Mixtures"
J. Chem. Phys. 2014, 141, 024510.     (46 citations, DOI 10.1063/1.4887082 ) ⭳Bib
14M. Thomas, M. Brehm, R. Fligg, P. Vöhringer, B. Kirchner:
"Computing Vibrational Spectra from ab initio Molecular Dynamics"
Phys. Chem. Chem. Phys. 2013, 15, 6608–6622.     (220 citations, DOI 10.1039/C3CP44302G ) ⭳Bib
Cover Art
9K. Wendler, M. Brehm, F. Malberg, B. Kirchner, L. Delle Site:
"Short Time Dynamics of Ionic Liquids in AIMD-Based Power Spectra"
J. Chem. Theory Comput. 2012, 8 (5), 1570–1579.     (49 citations, DOI 10.1021/ct300152t ) ⭳Bib