Magnetic-Texture Control of Charge and Spin Dynamics in Curved CrI3 Nanotubes

Curvature provides a unique route to stabilize noncollinear spin textures and regulate excited-state dynamics in low-dimensional magnets. Here, using noncollinear time-dependent density functional theory combined with nonadiabatic molecular dynamics, we investigate magnetic-configuration-dependent charge and spin dynamics in a CrI3 nanotube by comparing collinear ferromagnetic magnetization (FM) and radial magnetization (RM) configurations. We show that the magnetic configuration acts as an active control variable rather than a passive background of the curved lattice. Relative to FM, RM suppresses hole energy relaxation and spin relaxation but accelerates nonradiative electron-hole recombination. This contrasting behavior arises from weakened phonon-driven electronic fluctuations in RM. During intraband relaxation, reduced fluctuations decrease nonadiabatic couplings and slow phonon-assisted hole and spin relaxation. During interband recombination, weaker elastic scattering prolongs the pure-dephasing time and accelerates recombination in decoherence-dominated regime. These results establish magnetic-texture engineering as an effective strategy for tuning coupled charge-spin dynamics in curved magnetic nanostructures.