Time-reversal (T) symmetry breaking is a fundamental physics concept underpinning a broad science and technology area, including topological magnets, axion physics, dissipationless Hall currents, or spintronic memories. A best known conventional model of macroscopic T-symmetry breaking is a ferromagnetic order of itinerant Bloch electrons with an isotropic spin interaction in momentum space. Anisotropic electron interactions, on the other hand, have been a domain of correlated quantum phases, such as the T-invariant nematics or unconventional superconductors. Here we report discovery of a broken-T phase of itinerant Bloch electrons with an unconventional anisotropic spin-momentum interaction, whose staggered nature leads to the formation of two ferromagnetic-like valleys in the momentum space with opposite spin splittings. We describe qualitatively the effect by deriving a non-relativistic single-particle Hamiltonian model. Next, we identify the unconventional staggered spin-momentum interaction by first-principles electronic structure calculations in a four-sublattice antiferromagnet Mn5Si3 with a collinear checkerboard magnetic order. We show that the staggered spin-momentum interaction is set by nonrelativistic spin-symmetries which were previously omitted in relativistic physics classifications of spin interactions and topological quasiparticles. Our measurements of a spontaneous Hall effect in epilayers of antiferromagnetic Mn5Si3 with vanishing magnetization are consistent with our theory predictions. Bloch electrons with the unconventional staggered spin interaction, compatible with abundant low atomic-number materials, strong spin-coherence, and collinear antiferromagnetic order open unparalleled possibilities for realizing T-symmetry broken spin and topological quantum phases.
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