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Single spin resonance in a van der Waals embedded paramagnetic defect

Published 13 Jun 2019 in cond-mat.mes-hall and physics.optics | (1906.05903v1)

Abstract: Spins constitute a group of quantum objects forming a key resource in modern quantum technology. Two-dimensional (2D) van der Waals materials are of fundamental interest for studying nanoscale magnetic phenomena. However, isolating singular paramagnetic spins in 2D systems is challenging. We report here on a quantum emitting source embedded within hexgonal boron nitride (h-BN) exhibiting optical magnetic resonance (ODMR). We extract an isotropic $g$ factor close to 2 and derive an upper bound for a zero field splitting (ZFS) ($\leq$ 4 MHz). Photoluminescence (PL) behavior under temperature cycling using different excitations is presented, assigning probable zero phonon lines (ZPLs) / phonon side band (PSBs) to emission peaks, compatible with h-BN's phonon density of states, indicating their intrinsic nature. Narrow and inhomogeneous broadened ODMR lines differ significantly from monoatomic vacancy defect lines known in literature. We derive a hyperfine coupling of around 10 MHz. Its angular dependence indicates an unpaired electron in an out-of-plane $\pi$-orbital, probably originating from an additional substitutional carbon impurity or other low mass atom. We determine the spin relaxation time $T_1$ to be around 17 $\mu$s.

Citations (163)

Summary

Overview of Single Spin Resonance in a van der Waals Embedded Paramagnetic Defect

The paper "Single Spin Resonance in a van der Waals Embedded Paramagnetic Defect" represents an investigation into the quantum emitting capabilities of hexagonal boron nitride (h-BN) within the framework of optically detected magnetic resonance (ODMR). This study targets the challenging task of isolating singular paramagnetic spins in two-dimensional (2D) van der Waals materials, focusing on defects embedded in h-BN.

Examination of Quantum Emitters in h-BN

The authors present an analysis of quantum emitters (QE) embedded in h-BN, emphasizing optical magnetic resonance characteristics. An isotropic g-factor close to 2 was identified, along with an upper bound zero field splitting (ZFS) of ≤4 MHz. The study elaborates on photoluminescence (PL) behaviors noted during temperature cycling under diverse excitations. Emission peaks were attributed to probable zero phonon lines (ZPLs) or phonon side bands (PSBs), aligning with h-BN's phonon density of states. These findings suggest an intrinsic nature of PL features.

Notably, ODMR lines were observed to be narrow yet inhomogeneously broadened, differing significantly from monoatomic vacancy defect lines found in existing literature. A hyperfine coupling of around 10 MHz was derived, with angular dependence pointing to an unpaired electron originating from an out-of-plane π-orbital, possibly due to additional substitutional carbon impurities or other low mass atoms. Spin relaxation time T1 was determined to be approximately 17 μs, indicative of the potential quantum technological applications of h-BN defects.

Spin Properties and Optical Behavior

The exploration of the spin properties of h-BN emitters unfolds through several optical behaviors, such as confinement of wave functions and electron spin interactions. Hanbury Brown and Twiss autocorrelation measurements revealed how the metastable state is significant in observing ODMR. The study delineates specific emission peaks that couple to distinct phonon energies within h-BN's optical phonon scope, revealing detailed phonon maps and the PSB spectrum juxtaposed against ZPL.

ODMR Analysis and Implications

This work marks the first demonstration of ODMR concerning paramagnetic defects in 2D van der Waals materials. By employing continuous wave (CW) laser excitation and magnetic field modulation, ODMR peaks with Voigt functions were fitted, indicating interactions significantly dominated by hyperfine coupling. Analysis reveals narrow ODMR line widths (<100 MHz), parallel to electron paramagnetic resonance (EPR) studies, implicating defect structures involve vacancy alongside impurity atoms such as carbon.

Given the isotropic g-factor and the hyperfine tensor behavioral insights, the study provides a robust framework to understand defect structures in h-BN, facilitating advancements in quantum emitter technologies. Recognizing the emission characteristics of the spectrum, specifically at >800 nm (peak 7), offers potential pathways for future research to enhance emitter identification or isolation efforts in h-BN.

Future Directions and Conclusion

The findings embodied in this publication reflect nuanced understandings of spin-orbit interactions, defect-bound charactistics, and their magneto-optic responses of h-BN quantum emitters. Future investigations should explore angular-dependent magnetic field variations and closely monitor hyperfine satellites in different ODMR configurations, which could unravel more precise chemical identities and broader applications in quantum computing and sensing technologies. By elucidating defect-emitter behaviors and interactions within a 2D material context, this paper lays the groundwork for significant advancements in optical quantum technologies.

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