Using novel methods of directly simulating the effects of molecular dynamics on magnetic resonance spectra, EPR spectra of perdeuterated N15-substituted nitroxide tempone spin probes generated over 1-250 GHz and Brownian rotational correlation times 10-11 to 10-5 seconds. Simulations are in good agreement with less versatile techniques. Both experimental (W-band) and simulated spectra confirm predictions that VHF-EPR at higher frequencies show greater sensitivity in the faster motional regime (i.e. less than 0.1 ns).