Coherent Manipulation of Molecular Spins Using Wideband Chirped Pulses at High Fields

This presentation will provide an overview of a range of new applications in the area of molecular quantum spin science that are now possible at the US National High Magnetic Field Laboratory (MagLab) as a result of the development of a wideband, high-power 94 GHz pulsed EPR spectrometer [1]. This instrument allows true Fourier-transform detection spanning a 1 GHz instantaneous bandwidth, akin to what has been possible in NMR for several decades. The presentation will begin by describing acquisition of single-shot, frequency-domain EPR spectra using chirped pulses, thus providing a very efficient and convenient means to measure time-resolve processes in molecules and solids, e.g., spin-lattice and spin-spin relaxation. This will be followed by a discussion of a coherent population transfer protocol involving the 2S + 1 = 8 Zeeman levels associated with the spin S = ⁷/₂ Gd(III) qudit (see Figure 1), potentially paving the way towards implementation of well-known quantum search algorithms. It will also be shown how the use of chirped pulses provides a route to achieving highly non-thermal spin populations, suggesting novel qubit initialization schemes [2].