Direct Spectroscopic Observation of Berry Phase Interference in the Ni$_4$ Single-Molecule Magnet

TL;DR

This paper reports direct spectroscopic observation of Berry phase interference in a Ni4 single-molecule magnet, demonstrating how quantum interference affects tunneling between spin states, with experimental data aligning with theoretical models.

Contribution

First direct spectroscopic measurement of Berry phase interference in a Ni4 SMM using electron-spin resonance with in situ sample rotation.

Findings

Berry phase interference causes observable splitting in ESR transitions.

Experimental results match theoretical predictions.

Data reveals effects of dipolar interactions and sample misalignment.

Abstract

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 four-fold symmetric SMM. Specifically, we measure transitions between tunnel-split excited states in the 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 \textit{in situ} so that 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 theoretical predictions, and fitting of the data provides information about the effects of dipolar interactions and sample misalignment.