Berry-phase effects in spin systems lead to the suppression of tunneling effects when different tunneling paths interfere destructively. Such effects have been seen in several single-molecule magnets (SMMs) through measurements of magnetization dynamics, where the experimental signal may arise from the contributions of numerous energy levels. Here we present experimental measurements of Berry-phase interference effects that are determined through electron-spin resonance on a fourfold symmetric SMM. Specifically, we measure transitions between tunnel-split excited states in the ${\mathrm{Ni}}_4$ SMM in the presence of a transverse field in the hard plane of the crystalline sample. By using a home-built rotation apparatus, the direction of the sample can be changed in situ so that the field direction can be swept through the entire hard plane of the sample. When the field is in certain directions in the plane, we observe a splitting of the transition, a hallmark of Berry-phase interference. The experimental results are well reproduced by numerical simulations, and fitting of the data provides information about the effects of dipolar interactions and sample misalignment.

• Received 1 October 2020
• Revised 1 December 2020
• Accepted 7 December 2020

DOI:https://doi.org/10.1103/PhysRevB.102.224428