| Summary: | The current generation of quantum sensing technologies using color centers in diamond crystals is primarily based on the principle that the resonant microwave frequency of the luminescence between quantum levels of the nitrogen-vacancy (NV) center varies with temperature and electric and magnetic fields. This principle enables us to measure, for instance, magnetic and electric fields, as well as local temperature with nanometer resolution in conjunction with a scanning probe microscope (SPM). However, the time resolution of conventional quantum sensing technologies has been limited to microseconds due to the limited luminescence lifetime. Here, we investigate ultrafast opto-magnetic effects in diamond crystals containing NV centers to improve the time resolution of quantum sensing to sub-picosecond time scales. The spin ensemble from diamond NV centers induces an inverse Cotton–Mouton effect (ICME) in the form of a sub-picosecond optical response in a femtosecond pump–probe measurement. The helicity and quadratic power dependence of the ICME can be interpreted as a second-order opto-magnetic effect in which ensembles of NV electron spins act as a source for the ICME. The results provide fundamental guidelines for enabling high-resolution spatial-time quantum sensing technologies when combined with SPM techniques.
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