Twisted CrPS4 Layers Reveal Elusive Altermagnetic State

Physicists have long sorted the magnetic world into two familiar camps: ferromagnets, whose spins align in unison and produce the everyday magnetism of refrigerator doors, and antiferromagnets, whose spins cancel in opposing rows and leave the material outwardly silent. A third category, altermagnetism, has been racing through condensed matter theory over the past several years, promising the best of both worlds: the compensated, stray-field-free spin order of an antiferromagnet combined with the spin-split electronic bands normally associated with ferromagnets. Now, a team reporting in Nature Physics has delivered something theorists had proposed but experimentalists had not yet captured: direct signatures of altermagnetism in a twisted van der Waals material, created simply by stacking two flakes of the same magnetic crystal on top of one another at a right angle.

The material at the heart of the study is chromium thiophosphate, CrPS4, an air-stable, layered magnetic semiconductor that has become a workhorse of two-dimensional magnetism research. On its own, CrPS4 behaves conventionally depending on thickness: few-layer samples can show ferromagnetic order, while bulk crystals adopt an antiferromagnetic arrangement. Neither of these ground states, however, exhibits the hallmark of altermagnetism, which is a finite splitting between electronic states of opposite spin that does not arise from spin-orbit coupling but instead from the symmetry of the crystal and its magnetic arrangement. The researchers reasoned that if two CrPS4 flakes were stacked with their crystal axes rotated by ninety degrees, the interlayer symmetry would be altered in precisely the way theory predicts should generate an altermagnetic state.

The idea traces back to theoretical work suggesting that twisted magnetic van der Waals bilayers constitute an ideal platform for altermagnetism. In an ordinary antiferromagnet, time-reversal symmetry combined with a lattice translation protects the degeneracy of spin-up and spin-down bands, so the electronic structure shows no net spin splitting. When layers are rotated relative to one another, that combined symmetry operation is broken, and the spin degeneracy is lifted in a momentum-dependent fashion. The result is a material whose spins cancel macroscopically, avoiding the stray fields that plague ferromagnetic devices, yet whose electronic bands are split in a way that can carry spin-polarized currents. For spintronics, this combination is extraordinarily attractive: fast switching, dense packing, and robust spin information without the crosstalk that limits conventional magnetic memory.

To test the prediction, the team fabricated orthogonally twisted CrPS4/CrPS4 homostructures, stacking four-layer flakes rotated by ninety degrees relative to each other. They then interrogated the samples with a battery of optical probes, beginning with polarized Raman spectroscopy. In the twisted configuration, the Raman spectra revealed a splitting of phonon modes that is absent in untwisted controls. This vibrational fingerprint, the researchers show, arises from the interlayer coupling unique to the altermagnetic arrangement: the same symmetry breaking that splits the electronic bands also modifies the lattice dynamics, producing a spectroscopic signature that distinguishes the twisted state from any simple superposition of ferromagnetic and antiferromagnetic layers.

The more decisive evidence came from magneto-optical spectroscopy. Measuring the photoluminescence of the twisted homostructure under an applied magnetic field, the researchers tracked the degree of circular polarization of the emitted light. The twisted sample displayed a magnetic-field dependence that resembles the response of a ferromagnet, a striking result given that the underlying spin order is compensated. Even more telling was the observation of a pronounced Zeeman splitting in the photoluminescence spectra, with the sigma-plus and sigma-minus emission peaks separating as the field increased. Crucially, neither ferromagnetic nor antiferromagnetic CrPS4 samples show this splitting in the same configuration. Its emergence only in the twisted geometry indicates that the stack has entered a genuinely distinct magnetic ground state, one that carries the fingerprints of altermagnetism.

First-principles calculations reinforced the interpretation. Using density functional theory with an on-site Coulomb correction to treat the correlated chromium d electrons, the team computed the electronic structure of the orthogonally twisted bilayer and found large spin-split bands in an antiferromagnetic configuration. The pattern of the splitting matches the theoretical expectations for altermagnets: opposite-spin bands separate in momentum space in a way dictated by crystal rotation symmetry, while the net magnetization remains zero. The agreement between the computed band structure and the optical measurements provides a coherent picture in which twisting acts as a symmetry-breaking knob that switches on spin splitting without introducing any net magnetic moment.

The significance of the result extends beyond confirming a theoretical prediction. Van der Waals homostructures, in which the same material is stacked with controlled twist angles, have already revolutionized research on graphene and transition metal dichalcogenides, giving rise to moiré physics, flat bands, and correlated electronic phases. The present work shows that the same stacking engineering can serve as a design principle for magnetism itself. Rather than searching for new chemical compounds that happen to be altermagnets, researchers can now, in principle, manufacture altermagnetic states from well-characterized magnetic layers by choosing the twist angle. Because the twist angle is a continuously tunable parameter, it opens a route to systematically exploring how altermagnetic spin splitting evolves with interlayer symmetry, something no fixed crystal structure can offer.

The experimental signatures reported here also add to a growing toolbox for identifying altermagnets. Earlier confirmations of altermagnetic band splitting relied on techniques such as spin-resolved and angle-resolved photoemission spectroscopy, x-ray magnetic circular dichroism, and magneto-optical Kerr effect measurements in compounds like CrSb, MnTe, and RuO2. The CrPS4 study demonstrates that circularly polarized photoluminescence and Raman spectroscopy, both accessible table-top optical methods, can detect altermagnetism in atomically thin devices. This accessibility matters: optical probes can be applied to microscopic samples inside cryostats, under magnetic fields, and across device geometries, accelerating the pace at which candidate altermagnetic structures can be screened and characterized.

For applications, the appeal of altermagnets lies in their potential to combine the speed and stability of antiferromagnetic spintronics with the readout convenience of ferromagnets. Antiferromagnetic memory elements are immune to external fields and can in principle switch at terahertz frequencies, but their vanishing net moment makes them hard to read. Altermagnets solve the readout problem because their spin-split bands allow spin-polarized transport and magneto-optical signals even without net magnetization. A twisted van der Waals altermagnet adds another dimension: the state exists in an atomically thin, air-stable semiconductor that can be integrated into heterostructures with other two-dimensional materials, potentially enabling spin filters, tunnel junctions, and valleytronic devices in which spin and momentum are locked by design.

Challenges remain before such devices materialize. The reported signatures are spectroscopic rather than transport-based, and future work will need to demonstrate electrical readout and manipulation of the altermagnetic state, quantify the magnitude and temperature stability of the spin splitting, and explore how different twist angles and layer numbers tune the effect. Still, the demonstration that a simple ninety-degree rotation of identical CrPS4 flakes produces a magnetic phase absent from either constituent marks a conceptual milestone. It establishes twisted van der Waals homostructures as an experimental platform for altermagnetism, transforming a theoretical proposal into a tangible, measurable state of matter and handing the spintronics community a new material class to engineer.

Subject of Research: Experimental observation of altermagnetism in orthogonally twisted CrPS4 van der Waals homostructures

Article Title: Altermagnetism in twisted van der Waals homostructures

Article References: Chen, J., Xie, X., Li, S., Zhang, S., Hou, S., Zhang, X., He, J., Liu, Z., Wang, J.-T., & Liu, Y. (2026). Altermagnetism in twisted van der Waals homostructures. Nature Physics. https://doi.org/10.1038/s41567-026-03440-y

Image Credits: AI Generated

DOI: 10.1038/s41567-026-03440-y

Keywords: altermagnetism, CrPS4, van der Waals heterostructures, twisted bilayers, spintronics, magneto-optical spectroscopy, Zeeman splitting, Raman spectroscopy, 2D magnets, spin splitting, antiferromagnetism, first-principles calculations