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arXiv:2609.33714

Placement-driven reversal of preferred spin alignment in monolayer hBN vacancy pairs

Daniel Hashemi

cond-mat.mtrl-scicond-mat.mes-hallquant-phSubmitted Sep 27, 2026• Announced Sep 29, 2026
v1 · Sep 27, 2026v2 · Oct 14, 2026
arXivHTMLPDF

Abstract

The negatively charged boron vacancy is an optically addressable spin centre in hexagonal boron nitride (hBN), but bringing two vacancies together introduces electronic interactions absent from the isolated-defect picture. Here we use density-functional theory at total charge q = -2 to show that atomic-scale placement reverses the preferred collinear spin alignment in monolayer hBN. Among seven configurations, the closest pair, separated by 4.3 angstrom, favours parallel alignment by 27.6 meV within the semilocal approximation. Moving one vacancy by a single lattice vector reverses the preference, and a 7.5 angstrom pair favours antiparallel alignment by 50.7 meV. Numerical controls change these two reference splittings by less than 1 meV; hybrid-functional calculations retain their signs while substantially changing their magnitudes. Local distortions connect the antiparallel preference at 7.5 angstrom to changes in vacancy-state hybridization along an intervening atomic chain. The closest pair instead exhibits a contact-localized spin-density contrast and constrained angular energies that depart from the bilinear Heisenberg form. These results identify a placement-sensitive regime of interacting defects and provide a microscopic foundation for investigating coupled spin centres in atomically thin materials.

Comments
15-page main text, 4 main figures; 72-page Supplementary Information included in the same PDF

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The negatively charged boron vacancy ($\VB$) in hexagonal boron nitride (\hBN{}) was the first optically addressable spin qubit identified inside a van der Waals crystal, allowing atomically defined placement relative to a target. Its coherence in bulk \hBN{} is limited by the boron nuclei of the layers flanking the defect plane, which a thin flake removes. Here, we use a generalized cluster-correlation expansion with an extended central-spin block to calculate the Hahn-echo coherence time of $\VB$ in h11^{11}11B15^{15}15N as a function of layer number. Our results show that T2T_2T2​ rises from $199\ns$ in the bulk limit to $653\ns$ in a monolayer, a factor of 3.33.33.3 that is already saturated at three layers and that a sublattice decomposition attributes entirely to boron. The enhancement is confined to low field, is insensitive to stacking registry and twist angle, and requires alignment to within about two degrees, an onset we reproduce with no free parameters. Under dynamical decoupling, a 1/e1/e1/e threshold returns $206\ns$ for every thickness, but this is a zero of the first-shell modulation rather than a decay: measured without a threshold, the layer contrast survives and reaches a factor of 170170170. Layer number thus emerges as a design parameter for $\VB$-based sensing.
Spin defects in two-dimensional materials hold significant potential for quantum information technologies and sensing applications. The negatively charged boron vacancy (VB-) in hexagonal boron nitride (hBN) has attracted considerable attention as a quantum sensor due to its demonstrated sensitivity to temperature, magnetic fields, and pressure.1 However, its applications have thus far been limited by inherently dim photoluminescence (PL). By fabricating a van der Waals heterostructure with a sensitizing donor layer, lead iodide (PbI2), we effectively enhance the PL intensity from the VB- by 5-45x, while maintaining compatibility with other heterostructures and vdW optoelectronic platforms. The type-I band alignment at the heterojunction enables efficient exciton migration while suppressing back-electron transfer, and the strong spectral overlap between the PbI2 emission and defect absorption supports efficient fluorescence resonance energy transfer. Ab initio density functional theory (DFT) predicts a photon-ratcheting mechanism that boosts absorption and emission while maintaining magnetic resonance (ODMR) contrast through minimal hybridization. Experimentally, the heterostructure exhibits enhanced continuous-wave ODMR sensitivity and functions as a precise probe of external magnetic fields. This work establishes a proof-of-concept for amplifying weak defect signals in nanomaterials, highlighting a new strategy for engineering their optical and magnetic responses.
The negatively charged boron vacancy center in hexagonal boron nitride is a premier candidate for quantum sensing, yet its performance is critically limited by longitudinal spin-lattice relaxation time (T1T_1T1​). A microscopic understanding of spin relaxation in the high magnetic field regime remains elusive, as the relevant Zeeman transitions lie far below the optical phonon energies typically invoked to describe the relaxation process. Here, we apply an \textit{ab initio} acoustic mode spin-phonon relaxation theory to this problem and quantitatively reproduce the experimental magnetic field and temperature dependence of T1T_1T1​ without empirical fitting parameters. We demonstrate that the relaxation dynamics are driven by a direct one-phonon emission and absorption process resonant with the Zeeman splitting. Furthermore, we identify the out-of-plane flexural phonon branch which is unique to two-dimensional hosts, as the primary source of decoherence, creating a distinct low-energy spectral function that facilitates spin relaxation. Our results provide a microscopic interpretation of the experimentally observed non-monotonic field and temperature dependence in two-dimensional quantum defect centers.
Boron nitride is a layered crystal whose properties depend on how its atomic sheets are stacked. Its negatively charged boron vacancy is a well-established magnetic defect that can be prepared and read out optically, but in the common hexagonal form it emits very little light, because the symmetry of the surrounding lattice forbids the relevant optical transition. Here we show, using first-principles calculations, that stacking the sheets in the rhombohedral sequence instead removes this restriction and increases the emitted intensity by one to two orders of magnitude, while the magnetic properties remain comparable or improve. We predict that the resulting emission is bright enough for a single defect to be addressed at room temperature, and that a sharp emission line, absent in the hexagonal form, should appear on cooling. Stacking order therefore acts as a design parameter for tailoring the quantum properties of defects embedded in layered materials.
Boron vacancies (VB−V_B^-VB−​) in hexagonal boron nitride (hBN) have emerged as a promising platform for two-dimensional quantum sensors capable of operating at atomic-scale proximity. However, the mechanisms responsible for photoluminescence quenching in thin hBN sensing layers when placed in contact with absorptive materials remain largely unexplored. In this Letter, we investigate non-radiative Förster resonance energy transfer (FRET) between VB−V_B^-VB−​ centers and either monolayer graphene or 2D semiconductors. Strikingly, we find that the FRET rate is negligible for hBN sensing layers thicker than 3 nm, highlighting the potential of VB−V_B^-VB−​ centers for integration into ultra-thin quantum sensors within van der Waals heterostructures. Furthermore, we experimentally extract the intrinsic radiative decay rate of VB−V_B^-VB−​ defects.
Negatively charged boron vacancy (VB−\mathrm{V_B^-}VB−​) in hexagonal boron nitride (hBN) is the most extensively studied room-temperature quantum spin system in two-dimensional (2D) materials. Nevertheless, the current effective readout of VB−\mathrm{V_B^-}VB−​ spin states is carried out by systematically optical methods. This limits their exploitation in compact and miniaturized quantum devices, which would otherwise hold substantial promise to address quantum sensing and quantum information tasks. In this study, we demonstrated a photoelectric spin readout technique for VB−\mathrm{V_B^-}VB−​ spins in hBN. The observed photocurrent signals stem from the spin-dependent ionization dynamics of boron vacancies, mediated by spin-dependent non-radiative transitions to a metastable state. We further extend this electrical detection technique to enable the readout of dynamical decoupling sequences, including the Carr-Purcell-Meiboom-Gill (CPMG) protocols, and of nuclear spins via electron-nuclear double resonance. These results provide a pathway toward on-chip integration and real-field exploitation of quantum functionalities based on 2D material platforms.