Abstract

Magnetic proximity effects in Co/hBN/graphene heterostructures are systematically analyzed via first-principles calculations, demonstrating a pronounced localized spatial variation of the induced spin polarization of graphene’s Dirac states. The proximity-induced exchange coupling, magnetic moments, and tunneling spin polarization (TSP) are shown to depend sensitively on the atomic registry at the interfaces. We analyze more than twenty distinct stackings—including high- and low-symmetry configurations—and reveal that the spin splittings of graphene’s Dirac bands span a wide range from 1 to 100 meV, depending on the local hybridization of Co dz2, hBN pz, and graphene pz orbitals. The strongest proximity effects emerge at geometric resonances, or “proximity hot spots,” where the three orbital states overlap maximally. The local spin polarization also depends sensitively on energy: Dirac states aligned with resonant Co orbitals experience the most pronounced exchange interaction. At these energies, the pseudospin Hamiltonian description of magnetic proximity effects breaks down. Outside these resonances, the pseudospin picture is restored. Our findings highlight the intrinsically local nature of proximity effects, governed by the spectral resonance and interlayer wavefunction overlap. We further quantify how additional hBN layers, interlayer twist, and multilayer graphene modify the proximity exchange and TSP, offering microscopic insight for designing spintronic van der Waals heterostructures with engineered interfaces and optimized spin transport.

Abstract

Magnetic proximity effects in Co/hBN/graphene heterostructures are systematically analyzed via first-principles calculations, demonstrating a pronounced localized spatial variation of the induced spin polarization of graphene’s Dirac states. The proximity-induced exchange coupling, magnetic moments, and tunneling spin polarization (TSP) are shown to depend sensitively on the atomic registry at the interfaces. We analyze more than twenty distinct stackings—including high- and low-symmetry configurations—and reveal that the spin splittings of graphene’s Dirac bands span a wide range from 1 to 100 meV, depending on the local hybridization of Co dz2, hBN pz, and graphene pz orbitals. The strongest proximity effects emerge at geometric resonances, or “proximity hot spots,” where the three orbital states overlap maximally. The local spin polarization also depends sensitively on energy: Dirac states aligned with resonant Co orbitals experience the most pronounced exchange interaction. At these energies, the pseudospin Hamiltonian description of magnetic proximity effects breaks down. Outside these resonances, the pseudospin picture is restored. Our findings highlight the intrinsically local nature of proximity effects, governed by the spectral resonance and interlayer wavefunction overlap. We further quantify how additional hBN layers, interlayer twist, and multilayer graphene modify the proximity exchange and TSP, offering microscopic insight for designing spintronic van der Waals heterostructures with engineered interfaces and optimized spin transport.

Abstract

Magnetic proximity effects in Co/hBN/graphene heterostructures are systematically analyzed via first-principles calculations, demonstrating a pronounced localized spatial variation of the induced spin polarization of graphene’s Dirac states. The proximity-induced exchange coupling, magnetic moments, and tunneling spin polarization (TSP) are shown to depend sensitively on the atomic registry at the interfaces. We analyze more than twenty distinct stackings—including high- and low-symmetry configurations—and reveal that the spin splittings of graphene’s Dirac bands span a wide range from 1 to 100 meV, depending on the local hybridization of Co dz2, hBN pz, and graphene pz orbitals. The strongest proximity effects emerge at geometric resonances, or “proximity hot spots,” where the three orbital states overlap maximally. The local spin polarization also depends sensitively on energy: Dirac states aligned with resonant Co orbitals experience the most pronounced exchange interaction. At these energies, the pseudospin Hamiltonian description of magnetic proximity effects breaks down. Outside these resonances, the pseudospin picture is restored. Our findings highlight the intrinsically local nature of proximity effects, governed by the spectral resonance and interlayer wavefunction overlap. We further quantify how additional hBN layers, interlayer twist, and multilayer graphene modify the proximity exchange and TSP, offering microscopic insight for designing spintronic van der Waals heterostructures with engineered interfaces and optimized spin transport.

Abstract

Magnetic proximity effects in Co/hBN/graphene heterostructures are systematically analyzed via first-principles calculations, demonstrating a pronounced localized spatial variation of the induced spin polarization of graphene’s Dirac states. The proximity-induced exchange coupling, magnetic moments, and tunneling spin polarization (TSP) are shown to depend sensitively on the atomic registry at the interfaces. We analyze more than twenty distinct stackings—including high- and low-symmetry configurations—and reveal that the spin splittings of graphene’s Dirac bands span a wide range from 1 to 100 meV, depending on the local hybridization of Co dz2, hBN pz, and graphene pz orbitals. The strongest proximity effects emerge at geometric resonances, or “proximity hot spots,” where the three orbital states overlap maximally. The local spin polarization also depends sensitively on energy: Dirac states aligned with resonant Co orbitals experience the most pronounced exchange interaction. At these energies, the pseudospin Hamiltonian description of magnetic proximity effects breaks down. Outside these resonances, the pseudospin picture is restored. Our findings highlight the intrinsically local nature of proximity effects, governed by the spectral resonance and interlayer wavefunction overlap. We further quantify how additional hBN layers, interlayer twist, and multilayer graphene modify the proximity exchange and TSP, offering microscopic insight for designing spintronic van der Waals heterostructures with engineered interfaces and optimized spin transport.