Direct calculation of (1)H(2)O T(1) NMRD profiles and EPR lineshapes for the electron spin quantum numbers S = 1, 3/2, 2, 5/2, 3, 7/2, based on the stochastic Liouville equation combined with Brownian dynamics simulation.
Direct calculation of electron spin relaxation and EPR lineshapes, based on Brownian dynamics simulation techniques and the stochastic Liouville equation approach (SLE-L) [Mol. Phys., 2004, 102, 1085-1093], is here generalized to high spin systems with spin quantum number S = 3/2, 2, 5/2, 3 and 7/2. A direct calculation method is demonstrated for electron spin-spin and spin-lattice relaxation, S-, X- and Q-band EPR-lineshapes and paramagnetic enhanced water proton T(1)- NMRD profiles. The main relaxation mechanism for the electron spin system is a stochastic second rank zero field splitting (ZFS). Brownian dynamics simulation techniques are used in describing a fluctuating ZFS interaction which comprises two parts namely the "permanent" part which is modulated by isotropic reorientation diffusion, and the transient part which is modulated by fast local distortion, which is also modelled by the isotropic rotation diffusion model. The SLE-L approach present is applicable both in the perturbation (Redfield) regime as well as outside the perturbation regime, in the so called slow motion regime.
Aman
Ken
K
Department of Chemistry, Biophysical Chemistry, Umeå University, S-901 87, Umeå, Sweden.
Westlund
Per-Olof
PO
D003198:Computer Simulation; D004578:Electron Spin Resonance Spectroscopy / Q000379:methods; D009682:Magnetic Resonance Spectroscopy / Q000379:methods*; D008956:Models, Chemical; D011789:Quantum Theory; D012680:Sensitivity and Specificity; D013269:Stochastic Processes; D014867:Water / Q000737:chemistry
D014867:Water