Computational screening of 2D pentagonal materials with room-temperature altermagnetism, multiferroicity, and topological states

Two-dimensional planar pentagonal crystals, long pursued for their geometrically frustrated lattice configurations and emergent quantum phenomena, have remained challenging to realize due to the intrinsic incompatibility of regular pentagons with Euclidean tiling. Here, we unveil 37 dynamically stable binary planar pentagonal monolayers through high-throughput computational screening of 1470 stoichiometric candidates. These materials exhibit room-temperature magnetism, including ferromagnetic (Curie temperature (TC) up to 521 K), antiferromagnetic (Néel temperature (TN) up to 761 K), and altermagnetic (TN = 984 K) ground states, alongside unprecedented electronic states: Dirac semimetals, Dirac half-metal, nodal-loop semimetal, nodal-loop half-metal, and altermagnetic semiconductors (Mn4N2) with giant spin splitting (0.78 eV). The latter achieves pure spin-polarized transport windows (−0.04 to 0.36 eV) and strain-tunable valley splitting (18.2 meV under 4% uniaxial strain). Intrinsic type-II multiferroicity emerges in Fe4C2 and Mn4C2, featuring in-plane electric polarization (1.4 and 1.6 pC/m), ferroelasticity (0.8% and 1.2% reversible strain), and reversal chirality. Topological band analysis identifies chiral edge states in Dirac semimetal pentagons, alongside a magnetic topological insulator with Chern number |C| = 2 in Mo2S4 and W2Te4. Temperature-driven structural transitions in Os2S4 and Tc2S4 from pentagonal to Lieb lattices accompany topological state switching and metal-to-semiconductor transitions. This work establishes pentagonal lattices as a platform for symmetry-driven multifunctionality, bridging geometric frustration with applications in spintronics, nanoelectronics, and quantum devices.