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Ferroelastic Altermagnetism

Rui Peng 1 , Shibo Fang 1 , Pin Ho 2 , Tong Zhou 3 , Junwei Liu 4, * , Yee Sin Ang 1, †

1 Science, Mathematics and Technology (SMT) Cluster, Singapore University of Technology and

Design (SUTD), Singapore 487372, Singapore. 2 Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and

Research (A*STAR), Singapore 138634, Singapore. 3 Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, Zhejiang 315200,

China 4 Hong Kong University of Science and Technology, Hong Kong, China SAR.

Emails: *[email protected], † [email protected]

Abstract

Combination of altermagnetism and ferroic orders, such as ferroelectric switchable

altermagnetism [Phys. Rev. Lett. 134, 106801 (2025) and Phys. Rev. Lett. 134, 106802

(2025)], offers a powerful route to achieve nonvolatile switching of altermagnetic spin

splitting. In this work, by synergizing altermagnetism and ferroelasticity, we propose the

concept of ferroelastic altermagnets in which the ferroelastic crystal reorientation can drive

multistate nonvolatile switching of the altermagnetic spin splitting via altermagnetoelastic

effect. Using monolayers RuF 4 and CuF 2 as material candidates, we demonstrate 2-state

and 3-state altermagnetic spin splitting switching as driven by ferroelastic strain states.

Transport calculation shows that multistate spin conductivities can be ferroelastically

encoded in an ferroelastic altermagnet, thus suggesting the potential of ferroelastic

altermagnetic as nonvolatile nanomechanical spin switches. The proposed concept of

ferroelastic altermagnetism enriches the emerging landscape of multiferroic altermagnetism

and shall pave a way towards straintronic-spintronic device applications.

1

1. Introduction

Together with ferromagnet (FM) and conventional antiferromagnet (AFM), altermagnet

represents an emerging new family of collinear magnetic materials [1-5]. Altermagnets

exhibit zero net magnetization like conventional AFM, but host nonrelativistic band spin

splitting like FM. Such FM-AFM dichotomy endows altermagnets with the advantages of

AFM such as robustness against external fields and compatible with ultrahigh-speed device

operation while still exhibiting broken spin degeneracy of FM, which are critical for spin

manipulation and information processing [6-21]. Altermagnets exhibit a plethora of intriguing

physical phenomena such as spin current generation [1-2], spin Hall effect [6], spin Nernst

effect [7], anomalous Hall effect [5], and tunneling magnetoresistance effects [6], which can

be harnessed for various device applications. A large variety of altermagnets have been

theoretically proposed [3-4,17,22], and some of them have been experimentally confirmed

[23-26].

The physics of altermagnets can be further enriched by multiferroicity. Multiferroics are

singular materials that exhibit two or more ferroic orders among (anti)ferromagnetism,

(anti)ferroelectricity and (anti)ferroelasticity [27-35]. For instance, the coupling between

ferroelectricity and magnetism yields magnetoelectric effect where ferroelectric polarization

and magnetization are coupled and can be mutually switched. Recent studies have unveiled

the altermagnetic counterpart of magnetoelectric effect, namely the altermagnetoelectric

effect [Fig. 1(a)] in which the altermagnetic spin splitting can be tuned by various forms of

ferroelectric switching [36-43], thus unveiling a route towards electrical-based nonvolatile

switching of altermagnetism. The multiferroic integration of ferroelectricity and

altermagnetism immediately raises the following question: Can altermagnetism be

integrated with ferroelasticity [44-48] – magnetoelastic effect – to achieve nonvolatile

nanomechanical deformation-induced switching of the altermagnetic spin splitting?

Here we propose the concept of ferroelastic altermagnetism in which altermagnetism

and ferroelasticity are synergized. As ferroelastic switching is equivalent to a rotation

operation on the lattice, such lattice rotation changes the spin-momentum coupling in a

ferroelastic altermagnetism, thus enabling an altermagnetoelastic effect in which the

altermagnetic spin splitting can be mechanically switched [Figs. 1(b,c)]. Ferroelastic 2 altermagnetism represents a mechanical multiferroic counterpart of the recently proposed

ferroelectric altermagnetism [36-40]. Using monolayers RuF 4 [49] and CuF 2 as proof-of-

concept, 2-state and 3-state nonvolatile switching of the altermagnetic spin splitting are

demonstrated, respectively, via first-principles calculations. We further show that the

multistate ferroelastic switching lead to nonvolatile switchable spin transport. These findings

reveal a previously unexplored mechanism to achieve nonvolatile strain-based

altermagnetic switching that enables multistate nonvolatile information encoding. This

concept of ferroelastic altermagnet shall serve as a harbinger of straintronic-spintronic

devices uniquely enabled by the union of altermagnetism and ferroelasticity.

Fig.1. Concept of ferroelastic altermagnetism. (a) Ferroelastic altermagnet arises in a material where altermagnetism and ferroelasticity are simultaneously present. Schematic diagram of (b) 2-state and (c) 3- state nonvolatile mechanical switching of the altermagnetic spin splitting two-dimensional ferroelastic altermagnets. M is the mirror symmetry axis of the systems.

2. Results and Discussion

2.1 Ferroelastic-driven altermagnetic spin switching and material candidates Two-dimensional (2D) materials can be classified according to layer groups [50], and those

belonging to layer groups L 8 –L 48 may host ferroelasticity due to their rectangular 2D Bravais

lattices. Altermagnetic monolayers within these layer groups may thus exhibit coexisting

ferroelasticity and altermagnetism [18]. To illustrate the concept of ferroelastic

altermagnetism, we use monolayers RuF 4 and CuF 2 (layer group L 17 ) as a proof-of-concept

3 material platform for achieving 2-state and 3-state ferroelastic-driven altermagnetic spin

switching. Monolayers RuF 4 and CuF 2 can potentially be mechanically exfoliated from bulks

RuF 4 and CuF 2 due to their layered structures [51-52]. As shown in Fig. 2(a), the crystal

lattice of monolayer RuF 4 has a rectangular lattice with a space group of P2 1 /c. The Ru

atoms are encapsulated in a distorted RuF 6 octahedron, and each Ru atom is connected to

six F atoms. The optimized lattice constants of monolayer RuF 4 is a = 5.42 Å and b = 5.08

Å. The crystal structure of monolayer CuF 2 shares the same space group P2 1 /c with

monolayer RuF 4 [Fig. 2(b)]. Also, the Cu atoms are encapsulated in a distorted CuF 6

octahedron, and each Cu atom is connected to six F atoms. The difference is that the

adjacent RuF 6 octahedrons are connected via the corner-sharing manner. The optimized

lattice constants of monolayer CuF 2 is a = 5.32 Å and b = 3.56 Å. The stability of monolayers

RuF 4 and CuF 2 are confirmed by phonon and ab initio molecular dynamics simulations (Fig.

S1 [53]). Fig. 2. Crystal and electronic structures of 2D ferroelastic altermagnets. Crystal structures of (a) RuF4 and (b) CuF2 from top and side views. Spin charge densities of monolayers (c) RuF4 and (d) CuF2 . Red and blue shading represent spin up and down, respectively. Band structures of monolayers (e) RuF4 and (f) CuF2 . Insets are two highest valence bands, and alternating spin splitting ΔE between them in the hole Brillouin zone. Density of states of monolayers (g) RuF4 and (h) CuF2 . Fermi level is set to zero in (e) to (h).

Under the octahedral crystal field, the d orbitals split into t 2g triplets and e g doublets. In

monolayer RuF 4 , Ru atoms lose four electrons and transform into Ru 4+ ions with four 4d

electrons. Two of them occupy one t 2g orbital, one of them occupy another t 2g orbital, and 4 one of them occupy the remaining t 2g orbital, giving rise to a local magnetic moment of 2 μ B .

The inequivalent distribution of the electrons on the three t 2g orbitals leads to the

compressed Jahn–Teller distortions of the crystal structure, which further splits the t 2g and

e g orbitals (Fig. S2 [53]). In monolayer CuF 2 , Cu atoms lose two electrons and transform into Cu 2+ ions with nine 3d electrons. Six of them occupy the three t 2g orbitals, two of them occupy

one e g orbital, and one of them occupy the other e g orbital, giving rise to a local magnetic

moment of 1 μ B . The inequivalent distribution of the electrons on the two e g orbitals leads to

the elongated Jahn–Teller distortions of the crystal structure, making t 2g and e g orbitals split

in a different way with those in monolayer RuF 4 (Fig. S2 [53]). The calculated magnetic

moments on Ru and Cu atoms are 1.67 and 0.64 μ B , respectively, which is consistent with

the above analysis.

The ground states of monolayers RuF 4 and CuF 2 are determined by comparing the

energy among three magnetic configurations: FM, Néel antiferromagnetic (AFM-Néel), and

stripe antiferromagnetic (AFM-stripe) (Fig. S3 [53]). It is found that the energies of FM and

AFM-stripe are 30.28 (7.47) and 11.69 (4.27) meV/unit cell higher than the AFM-Néel in

monolayer RuF 4 (CuF 2 ), respectively, thus indicating AFM-Néel is the energetically most

favorable state for both RuF 4 and CuF 2 . The spin charge densities of AFM-Néel RuF 4 and

CuF 2 are shown in Figs. 2(c-d). After considering magnetism, the two opposite-spin

sublattices in RuF 4 and CuF 2 can only be transformed to each other by screw or glide

symmetry, which is typical for altermagnets.

Monolayer RuF 4 has an indirect band gap of 0.82 eV, with CBM located at M/M’ point

and VBM located along Γ-M/M’ line [Fig. 2(e)]. The spin-up and spin-down states are

degenerate along M-X-Γ-Y-M, while an alternating spin splitting appears along M’-Γ-M,

forming a spin-momentum locking physics. We also plotted the two highest valence bands

and the amplitude of the spin splitting ΔE between them over the entire Brillouin zone. The

spin-momentum locking physics can also be observed at generic k points. The amplitude of

the spin splitting reaches up to 205 meV. For monolayer CuF 2 , its indirect band gap is 0.69

eV, with CBM located at X point and VBM located at M/M’ point [Fig. 2(f)]. Similarly, the spin-

up and spin-down states are degenerate along M-X-Γ-Y-M, while an alternating spin splitting

appears along M’-Γ-M. The amplitude of the spin splitting reaches up to 98 meV. The spin-

up and spin-down density of states of RuF 4 and CuF 2 are equal [Figs. 2(g-h)].

5 2.2 Symmetry analysis The underlying mechanism of the spin-momentum locking in monolayers RuF 4 and CuF 2

can be elucidated through symmetry analysis. When omitting the nonmagnetic F atoms, the

systems have PT and t 1/2 T symmetry, thus guaranteeing that the band structures are spin-

degenerate over the entire Brillouin zone. The F atoms in the noncentrosymmetric sites

break the PT and t 1/2 T symmetry, yielding spin splitting in the band structures. The space

group of monolayers RuF 4 and CuF 2 , P2 1 /c, contains four symmetry operations: {E, P, t 1/2 M y ,

t 1/2 C 2y }. The former two connects the same-spin sublattices, while the latter two connects

the opposite-spin sublattices. Considering the crystal and spin rotation symmetries remain

decoupled when considering AFM coupling in the absence of spin-orbital coupling, the

symmetry connecting two opposite-spin sublattices can be represented as [C 2 ||R], where

the transformations on the left (right) of the double vertical bar act only on the spin (real)

space. When the [C 2 ||t 1/2 M y ] and [C 2 ||t 1/2 C 2y ] is operated on monolayer CuF 2 , respectively,

we obtain:

!𝐶! | |𝑡" /!𝑀 $ &E(𝑘% , 𝑘$ , ↑, = E(𝑘% , −𝑘$ , ↓, !𝐶! | |𝑡" /!𝐶 ! $ &E(𝑘% , 𝑘$ , ↑, = E(−𝑘% , 𝑘$ , ↓,

(1)

Consequently, we have

E(𝑘% , 𝑘$ , ↑, = E(𝑘% , −𝑘$ , ↓, E(𝑘% , 𝑘$ , ↑, = E(−𝑘% , 𝑘$ , ↓,

(2)

This explains the emergence of alternating spin-split bands along M’-Γ-M and at generic k

points. We also have

E(𝑘% , 0, ↑) = E(𝑘% , 0, ↓) E(0, 𝑘$ , ↑, = E(0, 𝑘$ , ↓,

(3)

6 After considering the Bloch theorem, the bands are spin-degenerate when k x = mπ and k y =

nπ, thus explaining the spin-degenerate bands along high-symmetry paths M-X-Γ-Y-M.

2.3 Multistate nonvolatile ferroelastic-altermagnetic spin splitting switching

Interestingly, RuF 4 and CuF 2 are also ferroelastic monolayers. RuF 4 has two energy-

equivalent states F1 (a > b) and F2 (a < b), and one paraelastic state P (a = b) [Fig. 3(a)].

The ferroelastic switching from F1 to F2 is equivalent to a π/2 rotation of the lattice. In

contrast, CuF 2 has three ferroelastic states. For convenience, we choose the deformed

hexagon to be the structure unit. The three energy-equivalent ferroelastic phases can be

described as F1 (a 1 > a 2 /a 3 ), F2 (a 2 > a 1 /a 3 ) and F3 (a 3 > a 1 /a 2 ), where a 1 , a 2 and a 3 are the

diagonal lines of the deformed hexagon [Fig. 3(b)]. The paraelastic phase P is the T-phase

CuF 2 with a 1 = a 2 = a 3 . The ferroelastic switching from F1 to F2 (F3) is equivalent to a 2π/3

(4π/3) lattice rotation. The ferroelastic reversible strain of RuF 4 and CuF 2 , which are defined

as (a/b - 1) × 100% and (a i /a j - 1) × 100%, are calculated to be 6.8% and 11.4%, respectively,

7 which are larger than those of SnS (4.9%) and SnSe (2.1%) [44]. Fig. 3. Ferroelastic switching in RuF4 and CuF2 . Schematic diagram of 2-state and 3-state ferroelastic switching in (a) monolayer RuF4 and (b) monolayer CuF2 , respectively. Here a1 , a2 and a3 are three diagonal lines of the deformed hexagon of CuF2 . Energy profiles of the ferroelastic transition for (c) RuF4 and (d) CuF2 as a function of step number in nudged elastic band (N EB) calculations. Insets show the spin-momentum locking in different ferroelastic phases at −0.1 eV below the Fermi level.

We simulate the ferroelastic switching process of RuF 4 and CuF 2 using the nudged

elastic band (NEB) method. The overall switching barrier of RuF 4 and CuF 2 are 4 and 54

meV/atom [Figs. 3(c-d)], respectively, which is lower than those of phosphorene (200

meV/atom) [44] and borophane (100 meV/atom) [45]. The low switching barrier suggests

that monolayers RuF 4 and CuF 2 are potentially compatible with fast and low-energy

ferroelastic switching operation. Upon ferroelastic switching, the reoriented lattice changes

spin-momentum locking fashion, thus realizing multistate nonvolatile switching of the

altermagnetic spin splitting [see insets in Figs. 3(c-d)]. Fig.4. Transport properties in RuF4 and CuF2 . (a) Schematic diagram of the direction of the external in-plane electric field. (b) Schematic diagram of a four-terminal Hall-bar-like device. (c) Longitudinal and (d) transverse spin conductivities of monolayer RuF4 as a function of φ. (e) Longitudinal and (f) transverse spin conductivities of monolayer CuF2 as a function of φ. Fermi level is set to -0.1 eV in (c-f).

In altermagnets, the spin-polarized current can be generated by an external in-plane

electric field due to the anisotropic spin splitting [1,2,40]. In ferroelastic altermagnets, the

spin transport current can be mechanically switched via different ferroelastic states. We

calculate the transport current in RuF 4 and CuF 2 when driven by an external field [53]. The 8 longitudinal and transverse spin conductivities exhibit an angular dependence on φ with a

period of π, where φ is the direction of the in-plane electric field relative to x axis [Fig. 4(a)]

and φ can be experimentally controlled by changing the relative angle between the source-

drain electrode axis [see Fig. 4(b) for a device schematic] and the crystal structure of

ferroelastic altermagnet sample. Upon a ferroelastic switching, the lattice re-orientation

changes the relative orientation between the altermagnetic spin-split band structure and the

electric field, thus leading to spin current switching effect. In RuF 4 , the carrier transport under

F1 and F2 states exhibits equal but opposite transverse and longitudinal spin conductivities

[Figs. 4(c-d)]. The 2-state ferroelastic switching between F1 and F2 states thus lead to spin

reversal. For CuF 2 , the spin conductivities exhibit even richer switching effect via the three

ferroelastic states F1, F2 and F3. For instance, when the electric field is directed at φ=0, the

longitudinal spin conductivities under F1, F2 and F3 states can be switched between positive,

zero and negative magnitudes, respectively [Figs. 4(e-f)]. The ferroelastic altermagnetic

broaden the application scenario of altermagnets, enabling nonvolatile spin information

encoding and hybrid straintronic-spintronic device application.

3. Conclusion

In summary, we have proposed the concept of ferroelastic altermagnets that synergizes ferroelasticity with altermagnetism. The switchable ferroelastic states in ferroelastic altermagnets drive multistate nonvolatile switching of the altermagnetic spin splitting, leading to an altermagnetoelastic effect. Using monolayers RuF 4 and CuF 2 as proof-ofconcept, 2-state and 3-state nonvolatile switching of the altermagnetic spin splitting are demonstrated. We further show that the multistate ferroelastic phase transitions are accompanied by a switching of the spin current associated with the altermagnetic spin splitting. We note that the ferroelastic altermagnetism can also be achieved in other 2D ferroelastic altermagnets such as the two-state ferroelastic monolayers of VF 4 [11,13,54,55] and OsF 4 [13], and the three-state ferroelastic monolayer AgF 2 [13,56,57].

4. Experimental Section

First-principles calculations are performed based on density functional theory (DFT) [58] as implemented in Vienna ab initio simulation package (VASP) [59]. Exchange-correlation interaction is described by the Perdew-Burke-Ernzerhof (PBE) parametrization of 9 generalized gradient approximation (GGA) [60]. Structures are relaxed until the force on each atom is less than 0.01 eV/Å. The cutoff energy and electronic iteration convergence criterion are set to 600 eV and 10 −6 eV, respectively. To sample the 2D Brillouin zone, Monkhorst–Pack (MP) k-grid messes [61] of 7 × 7 × 1 and 5 × 9 × 1 are used for monolayers RuF 4 and CuF 2 , respectively. To avoid the interaction between adjacent layers, a vacuum space of 20 Å is added. Phonon calculations are carried out using the PHONOPY code with a 4 × 5 × 1 and 4 × 4 × 1 supercell for monolayers RuF 4 and CuF 2 , respectively [62]. Ab initio molecular dynamics (AIMD) simulations are performed at 300 K for 5 ps with a time step of 1 fs with a 4 × 5 × 1 and 4 × 4 × 1 supercell for monolayers RuF 4 and CuF 2 , respectively. Ferroelastic switching barrier is obtained by nudged elastic band (NEB) method [63]. The spin-resolved transport properties are calculated using a housing-made code, in which the electron energy and electron group velocity are evaluated from the Wannier-based tight binding Hamiltonian [64].

Acknowledgement

This work is supported by the Singapore Ministry of Education Academic Research Fund

(AcRF) Tier 2 under the Project ID MOE-000834-00 (Proposal ID T2EP50224-0006). P.H.

acknowledges the supports by the RIE2025 Manufacturing, Trade and Connectivity (MTC)

Individual Research Grants (Grant No. M23M6c0101) and (Grant No. M24N7c0086),

administered by A*STAR. T.Z. acknowledges the supports by the National Natural Science

Foundation of China (12474155) and the Zhejiang Provincial Natural Science Foundation of

China (LR25A040001). The computational work for this article was performed on resources

of the National Supercomputing Centre, Singapore (https://www.nscc.sg).

10

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material

of this article.

Keywords

Altermagnetism, Ferroelasticity, Multiferroicity, First-principles calculation, Nonvolatile

switching 11

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