Towards reliable references for electron paramagnetic resonance parameters based on quantum chemistry: the case of verdazyl radicals

Physical Chemistry Chemical Physics : PCCP
Anja MassolleJohannes Neugebauer

Abstract

We present an efficient and accurate computational procedure to calculate properties measurable by EPR spectroscopy. We simulate a molecular dynamics (MD) trajectory by employing the quantum mechanically derived force field (QMDFF) [S. Grimme, J. Chem. Theory Comput., 2014, 10, 4497] and sample the trajectory at different time steps. For each snapshot EPR properties are calculated with a hybrid density functional theory (DFT) method. EPR spectra are simulated based on the averaged results. We applied the strategy to a number of previously published and novel verdazyl radicals, for which we recorded EPR spectra. The resulting simulated spectra are compatible with experiment already before employing an additional fitting step, in contrast to those from single point electronic-structure calculations. After the refinement, the experimental data are excellently reproduced, and the fitted EPR parameters do not deviate much from the calculated ones. This provides confidence in ascribing a direct physical meaning to the refined data in terms of experimental EPR parameters rather than merely considering them as mathematical fit parameters. We also find that couplings to hydrogen nuclei have a significant influence on the spectra of verd...Continue Reading

References

Jan 11, 2005·The Journal of Chemical Physics·Vincenzo Barone
Sep 29, 2005·Journal of Magnetic Resonance·Stefan Stoll, Arthur Schweiger
Jan 6, 2006·The Journal of Chemical Physics·Johannes NeugebauerEvert Jan Baerends
Sep 25, 2007·The Journal of Organic Chemistry·Joe B GilroyRobin G Hicks
Jan 5, 2008·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Brendan C Mort, Jochen Autschbach
Oct 19, 2010·The Journal of Chemical Physics·Remigius MastalerzMarkus Reiher
Nov 11, 2010·Physical Chemistry Chemical Physics : PCCP·Xing ChenHans Agren
Mar 4, 2011·Journal of Computational Chemistry·Stefan GrimmeLars Goerigk
Jun 29, 2011·The Journal of Organic Chemistry·Matthew Bancerz, Michael K Georges
Aug 19, 2011·Chemical Society Reviews·Imma Ratera, Jaume Veciana
Nov 21, 2015·Journal of Chemical Theory and Computation·Stefan Grimme
Oct 11, 2011·Journal of Chemical Theory and Computation·Zilvinas RinkeviciusHans Ågren
Jan 31, 2017·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Stephan EhrlichStefan Grimme
Jun 13, 2017·Physical Chemistry Chemical Physics : PCCP·S EusterwiemannA Studer
Aug 1, 2015·Chemical Science·David MatuschekArmido Studer

❮ Previous
Next ❯

Citations

Jun 10, 2018·The Journal of Chemical Physics·Michael GlasbrennerChristian Ochsenfeld
Jan 23, 2021·Physical Chemistry Chemical Physics : PCCP·Jessica ExnerArmido Studer
May 22, 2021·Journal of the American Chemical Society·Evgeny V TretyakovVictor I Ovcharenko

❮ Previous
Next ❯

Methods Mentioned

BETA
ENDOR

Software Mentioned

Orca
garlic
SP
COSMO
Matlab
QMDFF
EasySpin
Amsterdam Density Functional 2014 ( ADF )

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.