Shaped optimal control pulses for increased excitation bandwidth in EPR

► Optimal control theory pulses have been applied for the first time in EPR. ► A fast amplitude and phase modulation unit has been implemented into a commercial pulse EPR spectrometer. ► Broadband excitation has been achieved for FT-EPR on radicals in liquid solution. ► The concept of dead-time compensated prefocused pulses has been tested. ► The spectrometer response function has been taken into account for the design of pulses with improved performance.