Coherent Spins in van der Waals Semiconductor GeS2 at Ambient Conditions

TL;DR

This paper reports the discovery and room-temperature coherent control of spin defects in GeS2, a 2D vdW semiconductor, demonstrating extended coherence times and potential for quantum sensing applications.

Contribution

First observation of optically active spin defects in GeS2 at room temperature with extended coherence times using dynamical decoupling.

Findings

Spin defects exhibit spin-1/2 behavior.

Dynamical decoupling extends T2 by 20 times.

DFT estimates possible defect structures.

Abstract

Optically active spin defects in van der Waals (vdW) materials have recently emerged as versatile quantum sensors, enabling applications from nanoscale magnetic field detection to the exploration of novel quantum phenomena in condensed matter systems. Their ease of exfoliation and compatibility with device integration make them promising candidates for future quantum technologies. Here we report the observation and room-temperature coherent control of spin defects in the high-temperature crystalline phase of germanium disulfide ($\beta$-GeS2), a two-dimensional (2D) semiconductor with low nuclear spin density. The observed spin defects exhibit spin-1/2 behavior, and their spin dynamics can be explained by a weakly coupled spin-pair model. We implement dynamical decoupling techniques to extend the spin coherence time (T$_2$) by a factor of 20. Finally, we use density functional theory (DFT) calculations to estimate the structure and spin densities of two possible spin defect candidates. This work will help expand the field of quantum sensing with spin defects in van der Waals materials.