Free electron laser-powered pulsed electron paramagnetic resonance (EPR) experiments performed at 240 GHz / 8.56 T on the crystalline organic radical BDPA reveal a tip-angle dependent resonant frequency. Frequency shifts as large as 11 MHz (45 ppm) are observed during a single Rabi oscillation. We attribute the frequency shifts to a "dressing" of the nutation by spin-spin interactions. A nonlinear semi-classical model which includes a temperature- and sample-geometry-dependent demagnetizing field reproduces experimental results. Because experiments are performed without a cavity, radiation damping -- the most common nonlinear interaction in magnetic resonance -- is negligible in our experiments.
@article{arxiv.1904.03578,
title = {Dressed Rabi oscillation in a crystalline organic radical},
author = {C. Blake Wilson and Devin T. Edwards and Jessica A. Clayton and Songi Han and Mark S. Sherwin},
journal= {arXiv preprint arXiv:1904.03578},
year = {2020}
}