Kavli Affiliate: Long Zhang
| First 5 Authors: , , , ,
| Summary:
Spin splitting in emerging altermagnets is non-relativistic and
momentum-dependent, yet energy-independent, and localized in momentum space,
posing challenges for practical applications. Here, we propose an
intercalation-driven paradigm for altermagnets to attain ameliorative
electronic structures, multiferroic characteristics, and anomalous and spin
transport functionalities. As a representative system, we investigate
electrochemistry- and self-intercalated V2Se2O bilayers, building on the
recently reported room-temperature K- and Rb-intercalated V2Se2O family [Nat.
Phys. 2025, 21, 754; Nat. Phys. 2025, 21, 760], utilizing density functional
theory, Wannier function analyses, Monte Carlo simulations, and non-equilibrium
Green function methods. Intercalation induces room-temperature intralayer
ferrimagnetic and interlayer ferromagnetic order (358 K for Li-intercalation
and 773 K for V-intercalation), ferroelasticity (~1 % signal intensity),
in-plane uniaxial magnetic anisotropy, and metallization, while also modifying
the anomalous Hall effect. Notably, Li- and V-intercalated V2Se2O bilayers
exhibit enhanced spin splitting and half-metallic behavior, respectively,
yielding near-perfect spin filtering efficiency. Intercalation substantially
enhances spin transport in V2Se2O-based devices, enabling giant
magnetoresistance (877 %), ultra-high thermal tunneling magnetoresistance
(~12000 %), and observable spin Seebeck and temperature negative differential
resistance effects. This intercalation-driven paradigm expands altermagnetic
functionalities through multifunctional integration, offering promising avenues
for advanced, miniaturized, room-temperature exploitation of anomalous,
electron, and spin transport properties.
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