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To resolve why isoelectronic chromium monopnictides exhibit vastly disparate ground states ranging from altermagnetism to complete absence of long-range order, the authors construct a unified spin-fermion model mapped via first-principles calculations in the non-collinear paramagnetic state. They reveal that across CrSb, CrAs, and CrP, a common nominal high-spin Cr$^{1+}$ ($d^5$) configuration couples to itinerant pnictogen bands, with chemical pressure systematically enhancing ligand itinerancy and driving structural transitions from NiAs- to distorted MnP-type lattices. This lattice distortion reconstructs competing Cr-Cr exchange interactions, cleanly explaining the evolution from A-type antiferromagnetism in CrSb to double-helical order in CrAs and magnetic frustration in CrP.
Identical high-spin electron configurations can span the spectrum from high-temperature altermagnetism to frustrated quantum disorder purely through chemical-pressure-driven exchange pathway reconstruction.
Isoelectronic compounds are generally expected to exhibit related electronic, structural, and magnetic behavior. Chromium monopnictides CrX (X= Sb, As, P), however, display a striking evolution from high-temperature altermagnetism in NiAs-type CrSb, through double-helical antiferromagnetism in MnP-type CrAs, to the absence of resolved long-range magnetic order in MnP-type CrP. Here, combining first-principles calculations in the non-collinear Curie-paramagnetic state, structural analysis, magnetic phase-diagram calculations, and exchange-parameter extraction, we establish a unified microscopic framework for this evolution. All three compounds share a formal high-spin $d^5$ configuration, nominally Cr$^{1+}$, coupled to itinerant states of predominantly pnictogen character. From Sb to P, chemical pressure enhances ligand itinerancy and drives the structural evolution from the high-symmetry NiAs lattice to increasingly distorted MnP-type networks. The accompanying reconstruction of competing Cr-Cr exchanges favors A-type antiferromagnetism in CrSb and double-helical order in CrAs, while placing CrP near a frustrated regime with closely competing magnetic tendencies. Our results establish chemical-pressure-driven exchange reconstruction as a general mechanism through which a common spin-fermion electronic structure can generate contrasting magnetic phases in strongly correlated materials.