[en] A phase transition can drive the spontaneous emergence of chiral orders in crystals below a critical temperature. However, selecting either a right- or a left-handed phase with the aid of electromagnetic fields is challenging, particularly when intrinsic polar and axial moments are lacking. In this Letter, we show that purely chiral phases with opposite handedness, when both deriving from one degenerate instability, are linked by accessible transition states. While these states compete with the chirality under an electromagnetic field, a circularly polarized source can select the handedness of the system. This selection is mediated by a chiral monopole and may further result in a hysteresis process of the gyrotropic properties, namely, the optical activity, below the critical temperature. We suggest several materials, among which K_{3}NiO_{2}, as candidates for possible experimental observation.
Research Center/Unit :
Q-MAT - Quantum Materials - ULiège
Disciplines :
Physics
Author, co-author :
Fava, Mauro ; Université de Liège - ULiège > Département de physique > Physique théorique des matériaux
Romero, Aldo ; Université de Liège - ULiège > Département de physique > Physique des matériaux et nanostructures ; West Virginia University, Department of Physics and Astronomy, Morgantown, West Virginia 26505-6315, USA
Bousquet, Eric ; Université de Liège - ULiège > Département de physique > Physique théorique des matériaux
Language :
English
Title :
Handedness Selection and Hysteresis of Chiral Orders in Crystals.
Publication date :
03 October 2025
Journal title :
Physical Review Letters
ISSN :
0031-9007
eISSN :
1079-7114
Publisher :
American Physical Society, United States
Volume :
135
Issue :
14
Pages :
146102
Peer reviewed :
Peer Reviewed verified by ORBi
Tags :
CÉCI : Consortium des Équipements de Calcul Intensif
F.R.S.-FNRS - Fonds de la Recherche Scientifique DOE - United States. Department of Energy SDSC - San Diego Supercomputer Center NSF - National Science Foundation
Funding text :
The authors acknowledge E. McCabe for fruitful discussions. Computational resources have been provided by the Consortium des Aquipements de Calcul Intensif funded by the Fonds de la Recherche Scientifique (F.R.S.-FNRS) under Grant No. 5020.11. M.F. and E.B. acknowledge FNRS for support and the PDR project CHRYSALID No. 40003544. Work at West Virginia University was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0021375. This work used Bridges2 and Expanse at the Pittsburgh Supercomputer (Bridges2) and the San Diego Supercomputer Center (Expanse) through Allocation No. DMR140031 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support program, which the National Science Foundation supports via Grants No. 2138259, No. 2138286, No. 2138307, No. 2137603, and No. 2138296.The authors acknowledge E. McCabe for fruitful discussions. Computational resources have been provided by the Consortium des \u00C9quipements de Calcul Intensif funded by the Fonds de la Recherche Scientifique (F.R.S.-FNRS) under Grant No. 2.5020.11. M.\u2009F. and E.\u2009B. acknowledge FNRS for support and the PDR project CHRYSALID No. 40003544. Work at West Virginia University was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0021375. This work used Bridges2 and Expanse at the Pittsburgh Supercomputer (Bridges2) and the San Diego Supercomputer Center (Expanse) through Allocation No. DMR140031 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support program, which the National Science Foundation supports via Grants No. 2138259, No. 2138286, No. 2138307, No. 2137603, and No. 2138296.
J. Hlinka, Eight types of symmetrically distinct vectorlike physical quantities, Phys. Rev. Lett. 113, 165502 (2014). PRLTAO 0031-9007 10.1103/PhysRevLett.113.165502
K. C. Erb and J. Hlinka, Symmetry guide to chiroaxial transitions, Phase Transitions 91, 953 (2018). PHTRDP 0141-1594 10.1080/01411594.2018.1498498
K. Kimura, M. Sera, and T. Kimura, (Equation presented) cation control of chiral domain formation in a (Equation presented), Inorg. Chem. 55, 1002 (2016). INOCAJ 0020-1669 10.1021/acs.inorgchem.5b02622
P. Huang, Z. Xia, X. Gao, J. M. Rondinelli, X. Zhang, H. Zhang, K. R. Poeppelmeier, and A. Zunger, Ferri-chiral compounds with potentially switchable dresselhaus spin splitting, Phys. Rev. B 102, 235127 (2020). PRBMDO 2469-9950 10.1103/PhysRevB.102.235127
T. Hayashida, K. Kimura, D. Urushihara, T. Asaka, and T. Kimura, Observation of ferrochiral transition induced by an antiferroaxial ordering of antipolar structural units in (Equation presented), J. Am. Chem. Soc. 143, 3638 (2021). JACSAT 0002-7863 10.1021/jacs.1c00391
T. Hayashida, K. Kimura, and T. Kimura, Switching crystallographic chirality in (Equation presented) by laser irradiation, J. Phys. Chem. Lett. 13, 3857 (2022). JPCLCD 1948-7185 10.1021/acs.jpclett.2c00606
M. Fava, W. Lafargue-Dit-Hauret, A. H. Romero, and E. Bousquet, Large and tunable spin-orbit effect of (Equation presented) orbitals through structural cavities in crystals, Phys. Rev. B 108, L201112 (2023). PRBMDO 2469-9950 10.1103/PhysRevB.108.L201112
M. Fava, W. Lafargue-Dit-Hauret, A. H. Romero, and E. Bousquet, Ferroelectricity and chirality in the (Equation presented) crystal, Phys. Rev. B 109, 024113 (2024). PRBMDO 2469-9950 10.1103/PhysRevB.109.024113
R. Oiwa and H. Kusunose, Rotation, electric-field responses, and absolute enantioselection in chiral crystals, Phys. Rev. Lett. 129, 116401 (2022). PRLTAO 0031-9007 10.1103/PhysRevLett.129.116401
V. Dubovik and V. Tugushev, Toroid moments in electrodynamics and solid-state physics, Phys. Rep. 187, 145 (1990). PRPLCM 0370-1573 10.1016/0370-1573(90)90042-Z
S. Prosandeev, I. Ponomareva, I. Kornev, I. Naumov, and L. Bellaiche, Controlling toroidal moment by means of an inhomogeneous static field: An ab initio study, Phys. Rev. Lett. 96, 237601 (2006). PRLTAO 0031-9007 10.1103/PhysRevLett.96.237601
J. Hlinka, J. Privratska, P. Ondrejkovic, and V. Janovec, Symmetry guide to ferroaxial transitions, Phys. Rev. Lett. 116, 177602 (2016). PRLTAO 0031-9007 10.1103/PhysRevLett.116.177602
S. Hoshino, M.-T. Suzuki, and H. Ikeda, Spin-derived electric polarization and chirality density inherent in localized electron orbitals, Phys. Rev. Lett. 130, 256801 (2023). PRLTAO 0031-9007 10.1103/PhysRevLett.130.256801
D. D. Khalyavin, R. D. Johnson, F. Orlandi, P. G. Radaelli, P. Manuel, and A. A. Belik, Emergent helical texture of electric dipoles, Science 369, 680 (2020). SCIEAS 0036-8075 10.1126/science.aay7356
C. P. Romao and D. M. Juraschek, Phonon-induced geometric chirality, ACS Nano 18, 29550 (2024). ANCAC3 1936-0851 10.1021/acsnano.4c05978
P. Behera, Electric field control of chirality, Sci. Adv. 8, eabj8030 (2022). SACDAF 2375-2548 10.1126/sciadv.abj8030
Z. Zeng, M. Först, M. Fechner, M. Buzzi, E. B. Amuah, C. Putzke, P. J. W. Moll, D. Prabhakaran, P. G. Radaelli, and A. Cavalleri, Photo-induced chirality in a nonchiral crystal, Science 387, 431 (2025). SCIEAS 0036-8075 10.1126/science.adr4713
S.-Y. Xu, Q. Ma, Y. Gao, A. Kogar, A. Zong, A. M. Mier Valdivia, T. H. Dinh, S.-M. Huang, B. Singh, C.-H. Hsu, T.-R. Chang, J. P. C. Ruff, K. Watanabe, T. Taniguchi, H. Lin, G. Karapetrov, D. Xiao, P. Jarillo-Herrero, and N. Gedik, Spontaneous gyrotropic electronic order in a transition-metal dichalcogenide, Nature (London) 578, 545 (2020). NATUAS 0028-0836 10.1038/s41586-020-2011-8
K. Crossed D signuriš, U. Müller, and M. Jansen, (Equation presented) revisited, phase transition and crystal structure refinement, Z. Anorg. Allg. Chem. 638, 737 (2012). ZAACAB 0044-2313 10.1002/zaac.201100511
D. Yamamoto, T. Sakurai, R. Okuto, S. Okubo, H. Ohta, H. Tanaka, and Y. Uwatoko, Continuous control of classical-quantum crossover by external high pressure in the coupled chain compound (Equation presented), Nat. Commun. 12, 4263 (2021). NCAOBW 2041-1723 10.1038/s41467-021-24542-6
S. Hirotsu, Jahn-Teller induced phase transition in (Equation presented): Structural phase transition with helical atomic displacements, J. Phys. C 10, 967 (1977). JPSOAW 0022-3719 10.1088/0022-3719/10/7/008
M. Isobe and Y. Ueda, Observation of phase transition from metal to spin-singlet insulator in (Equation presented) with (Equation presented) pyrochlore lattice, J. Phys. Soc. Jpn. 71, 1848 (2002). JUPSAU 0031-9015 10.1143/JPSJ.71.1848
M. Schmidt, W. Ratcliff, P. G. Radaelli, K. Refson, N. M. Harrison, and S. W. Cheong, Spin singlet formation in (Equation presented): Evidence of a helical dimerization pattern, Phys. Rev. Lett. 92, 056402 (2004). PRLTAO 0031-9007 10.1103/PhysRevLett.92.056402
S. Di Matteo, G. Jackeli, C. Lacroix, and N. B. Perkins, Valence-bond crystal in a pyrochlore antiferromagnet with orbital degeneracy, Phys. Rev. Lett. 93, 077208 (2004). PRLTAO 0031-9007 10.1103/PhysRevLett.93.077208
D. I. Khomskii and T. Mizokawa, Orbitally induced peierls state in spinels, Phys. Rev. Lett. 94, 156402 (2005). PRLTAO 0031-9007 10.1103/PhysRevLett.94.156402
N. R. Keskar and J. R. Chelikowsky, Structural properties of nine silica polymorphs, Phys. Rev. B 46, 1 (1992). PRBMDO 0163-1829 10.1103/PhysRevB.46.1
V. Dmitriev, V. Torgashev, P. Tolédano, and E. K. H. Salje, Theory of (Equation presented) polymorphs, Europhys. Lett. 37, 553 (1997). EULEEJ 0295-5075 10.1209/epl/i1997-00190-3
A. J. Leadbetter and A. F. Wright, The (Equation presented) transition in the cristobalite phases of (Equation presented) and (Equation presented) I. x-ray studies, Philos. Mag. 33, 105 (1976). PHMAA4 0031-8086 10.1080/14786437608221095
D. M. Hatch and S. Ghose, The (Equation presented) phase transition in cristobalite, (Equation presented), Phys. Chem. Miner. 17, 554 (1991). PCMIDU 0342-1791 10.1007/BF00202234
H. T. Stokes, D. M. Hatch, B. J. Campbell, and D. E. Tanner, Isodisplace: A web-based tool for exploring structural distortions, J. Appl. Crystallogr. 39, 607 (2006). JACGAR 0021-8898 10.1107/S0021889806014075
See Supplemental Material at http://link.aps.org/supplemental/10.1103/c4v9-nd4b for additional information about simulation parameters and the herein discussed theoretical model.
G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999). PRBMDO 0163-1829 10.1103/PhysRevB.59.1758
J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996). PRLTAO 0031-9007 10.1103/PhysRevLett.77.3865
S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, and A. P. Sutton, Electron-energy-loss spectra and the structural stability of nickel oxide: An (Equation presented) study, Phys. Rev. B 57, 1505 (1998). PRBMDO 0163-1829 10.1103/PhysRevB.57.1505
M. Cococcioni and S. de Gironcoli, Linear response approach to the calculation of the effective interaction parameters in the (Equation presented) method, Phys. Rev. B 71, 035105 (2005). PRBMDO 1098-0121 10.1103/PhysRevB.71.035105
M. Fava, E. McCabe, A. H. Romero, and E. Bousquet, Phonon-driven mechanism for the chiral phase transition of (Equation presented), Phys. Rev. B 111, 174102 (2025). PRBMDO 2469-9950 10.1103/PhysRevB.111.174102
A. Togo and I. Tanaka, First principles phonon calculations in materials science, Scr. Mater. 108, 1 (2015). SCMAF7 1359-6462 10.1016/j.scriptamat.2015.07.021
A. Togo, F. Oba, and I. Tanaka, First-principles calculations of the ferroelastic transition between rutile-type and (Equation presented)-type (Equation presented) at high pressures, Phys. Rev. B 78, 134106 (2008). PRBMDO 1098-0121 10.1103/PhysRevB.78.134106
D. M. Hatch and H. T. Stokes, INVARIANTS: Program for obtaining a list of invariant polynomials of the order-parameter components associated with irreducible representations of a space group, J. Appl. Crystallogr. 36, 951 (2003). JACGAR 0021-8898 10.1107/S0021889803005946
D. M. Juraschek, M. Fechner, and N. A. Spaldin, Ultrafast structure switching through nonlinear phononics, Phys. Rev. Lett. 118, 054101 (2017). PRLTAO 0031-9007 10.1103/PhysRevLett.118.054101
S. Bhowal and N. A. Spaldin, Electric toroidal dipole order and hidden spin polarization in ferroaxial materials, Phys. Rev. Res. 6, 043141 (2024). PPRHAI 2643-1564 10.1103/PhysRevResearch.6.043141
F. Thöle, M. Fechner, and N. A. Spaldin, First-principles calculation of the bulk magnetoelectric monopole density: Berry phase and Wannier function approaches, Phys. Rev. B 93, 195167 (2016). PRBMDO 2469-9950 10.1103/PhysRevB.93.195167
Y. Tang and A. E. Cohen, Optical chirality and its interaction with matter, Phys. Rev. Lett. 104, 163901 (2010). PRLTAO 0031-9007 10.1103/PhysRevLett.104.163901
X. Gonze, The Abinit project: Impact, environment and recent developments, Comput. Phys. Commun. 248, 107042 (2020). CPHCBZ 0010-4655 10.1016/j.cpc.2019.107042
M. Van Setten, M. Giantomassi, E. Bousquet, M. J. Verstraete, D. R. Hamann, X. Gonze, and G.-M. Rignanese, The pseudodojo: Training and grading a 85 element optimized norm-conserving pseudopotential table, Comput. Phys. Commun. 226, 39 (2018). CPHCBZ 0010-4655 10.1016/j.cpc.2018.01.012
G. Wagner and R. Hoppe, Oxydation intermetallischer phasen: (Equation presented) aus NaAu und (Equation presented), Z. Anorg. Allg. Chem. 549, 26 (1987). ZAACAB 0044-2313 10.1002/zaac.19875490604
I. Souza, J. Íñiguez, and D. Vanderbilt, First-principles approach to insulators in finite electric fields, Phys. Rev. Lett. 89, 117602 (2002). PRLTAO 0031-9007 10.1103/PhysRevLett.89.117602
A. Zabalo and M. Stengel, Natural optical activity from density-functional perturbation theory, Phys. Rev. Lett. 131, 086902 (2023). PRLTAO 0031-9007 10.1103/PhysRevLett.131.086902
K. Crossed D signuriš, O. V. Magdysyuk, and M. Jansen, Syntheses, structures and magnetic properties of the alkali oxonickelates (i) (Equation presented) ((Equation presented), Rb, Cs), Solid State Sci. 14, 1399 (2012). SSSCFJ 1293-2558 10.1016/j.solidstatesciences.2012.06.006
V. M. Talanov and V. B. Shirokov, Atomic order in the spinel structure-A group-theoretical analysis, Acta Crystallogr. Sect. A 70, 49 (2014). ACACEQ 0108-7673 10.1107/S2053273313027605
S. Marin, M. O'Keeffe, and D. Partin, Structures and crystal chemistry of ordered spinels: (Equation presented), (Equation presented), and (Equation presented), J. Solid State Chem. 113, 413 (1994). JSSCBI 0022-4596 10.1006/jssc.1994.1389
J. Liu, X. Wang, O. J. Borkiewicz, E. Hu, R.-J. Xiao, L. Chen, and K. Page, Unified view of the local cation-ordered state in inverse spinel oxides, Inorg. Chem. 58, 14389 (2019). INOCAJ 0020-1669 10.1021/acs.inorgchem.9b01685
V. Stevanović, M. d'Avezac, and A. Zunger, Simple point-ion electrostatic model explains the cation distribution in spinel oxides, Phys. Rev. Lett. 105, 075501 (2010). PRLTAO 0031-9007 10.1103/PhysRevLett.105.075501
M. Fava, A. H. Romero, and E. Bousquet, Handedness selection and hysteresis of chiral orders in crystals, v1, Zenodo, 2025, 10.5281/zenodo.17099265.
