Probing Spin Dynamics Across Magnetic Phase Transitions in CrCl3 Nanoflakes Using Nitrogen-Vacancy Microscopy

TL;DR

This study uses nitrogen-vacancy microscopy to probe spin dynamics in CrCl3 nanoflakes across magnetic phase transitions, revealing enhanced spin fluctuations and magnetic noise in the ferromagnetic regime, vital for 2D magnonics.

Contribution

It provides the first detailed measurement of spin fluctuations and magnetic noise across phase transitions in CrCl3 using NV center microscopy.

Findings

Spin fluctuations are intensified in the ferromagnetic regime.

NV relaxation rate G1 increases by two orders of magnitude in ferromagnetic phase.

Magnetic noise varies markedly across the magnetic phase diagram.

Abstract

CrCl3, a layered van der Waals (vdW) magnet, exhibits in-plane magnetic anisotropy and enhanced interlayer coupling upon stacking, making it an ideal platform to host exotic nanoscale magnetic phenomena such as magnon hydrodynamics and meron-like topological spin defects. When interfaced with other vdW materials, its antiferromagnetic-to-ferromagnetic and ferromagnetic-to-paramagnetic phase transitions and magnetic anisotropy can be tuned by voltage, strain, and layer stacking. Understanding the spin dynamics of CrCl3 at its magnetic phase transitions is crucial to its applications in magnonics. Here, we investigate the spin dynamics of CrCl3 nanoflakes using cryogenic diamond quantum sensing microscopy, based on measuring optically detected magnetic resonance, Rabi oscillations, and spin-lattice relaxation time (T1) of shallow nitrogen vacancy (NV) centers in diamond. In the ferromagnetic regime, we observe a pronounced reduction in the NV spin resonance contrast, a collapse of the Rabi oscillations, and a strong enhancement by two orders of magnitude of the relaxation rate, G1 = 1/T1. These observations indicate intensified spin fluctuations in the gigahertz range. Broadband ferromagnetic resonance spectroscopy on CrCl3 microcrystals reveals resonance frequencies in the 4-15 GHz range together with a linewidth of ~24 mT, further supporting the NV measurements. A phenomenological model of magnetic-noise-induced NV relaxation reproduces the temperature dependence of G1 by combining antiferromagnetic, ferromagnetic, and paramagnetic fluctuation channels, indicating that magnetic noise is strongest in the ferromagnetic regime and evolves markedly across the phase diagram. These results are crucial for using CrCl3 in 2D magnonics and hybrid quantum-magnon systems.