Liquid-state paramagnetic relaxation from first principles
|Author:||Rantaharju, Jyrki1; Vaara, Juha1|
1NMR Research Unit, P.O. Box 3000, FIN-90014 University of Oulu, Finland
|Online Access:||PDF Full Text (PDF, 0.8 MB)|
|Persistent link:|| http://urn.fi/urn:nbn:fi-fe201801021023
American Physical Society,
|Publish Date:|| 2018-01-02
We simulate nuclear and electron spin relaxation rates in a paramagnetic system from first principles. Sampling a molecular dynamics trajectory with quantum-chemical calculations produces a time series of the instantaneous parameters of the relevant spin Hamiltonian. The Hamiltonians are, in turn, used to numerically solve the Liouville–von Neumann equation for the time evolution of the spin density matrix.We demonstrate the approach by studying the aqueous solution of the Ni2+ ion. Taking advantage of Kubo’s theory, the spin-lattice (T1) and spin-spin (T2) relaxation rates are extracted from the simulations of the time dependence of the longitudinal and transverse magnetization, respectively. Good agreement with the available experimental data is obtained by the method.
Physical review. A
|Type of Publication:||
A1 Journal article – refereed
|Field of Science:||
114 Physical sciences
The research leading to these results has received funding from the People Programme (Marie Curie Actions) of the European Union’s Seventh Framework Programme (No. FP7/2007-2013) under REA Grant Agreement No. 317127. Further financial support has been obtained from the Exactus doctoral program of the University of Oulu Graduate School (J.R.), and the Academy of Finland. Computational resources due to CSC-IT Center for Science (Espoo, Finland) and the Finnish Grid Initiative project, were used.
|EU Grant Number:||
(317127) PNMR - Pushing the Envelope of Nuclear Magnetic Resonance Spectroscopy for Paramagnetic Systems. A Combined Experimental and Theoretical Approach
© 2016 American Physical Society. Published in this repository with the kind permission of the publisher.