Probing the fluctuating magnetic field of Fe-triazole spin-crossover thin-layers with nitrogen-vacancy centers in diamond

Abstract: Fe$^{\mathrm{II}}$ spin-crossover (SCO) complexes are materials that change their magnetic properties upon temperature variation, exhibiting a thermal hysteresis. Particularly interesting for magnetic-memory applications are thin layers of SCO complexes, where practical magnetic probing techniques are required. While conventional magnetometry on SCO complexes employs cryogenic temperatures, nitrogen-vacancy (NV) centers are quantum magnetometers that can operate at room temperature with high spatial resolution and magnetic-field sensitivity. In this work, we apply thin layers of Fe-triazole SCO complexes directly onto a single-crystal diamond with shallow NV centers working as magnetic sensors and probe the fluctuating magnetic field. Using temperature-dependent NV-center $T_1$ measurements and a widefield technique, we find that the complexes are paramagnetic in the investigated temperature range from 20 {\deg}C to 80 {\deg}C. We quantitatively describe the $T_1$ time by a model considering the fluctuating magnetic field of the Fe$^{\mathrm{II}}$ ions. We see signatures of a local change of spin state in the $T_1$ relaxometry data, but structural changes in the SCO material dominate the local magnetic environment of the NV centers. Moreover, we conduct a Hahn echo to measure the $T_2$ time, which contrasts the findings of the $T_1$ times for the SCO complexes. We attribute this to different NV detection sensitivities towards Fe$^{\mathrm{II}}$ and Fe$^{\mathrm{III}}$ of the protocols. Our results on the magnetic properties of SCO materials highlight the capabilities of the NV center as a susceptible sensor for fluctuating magnetic fields. At the same time, a spin switching of the complexes cannot be observed due to the systematic challenges when working on nanometer distances to the SCO thin layers.