- Open Access
Predominant electronic order parameter for structural chirality: Role of spinless electronic toroidal multipoles in Te and Se
Phys. Rev. Research 7, 033250 – Published 15 September, 2025
DOI: https://doi.org/10.1103/1zq8-pqh8
Abstract
We discuss predominant order parameters for structural chirality and demonstrate that time-reversal-even axial quadrupole plays a key role in stabilizing a chiral structure. Using the symmetry-adapted closest Wannier model of the trigonal Te and Se, we quantify the evolution of the spin-independent (spinless) and spin-dependent (spinful) electric toroidal (ET) (axial) multipole moments across the transition from an achiral to a chiral structure. Our results clearly identify that a spin-independent off-diagonal real hopping between orbitals, which corresponds to the bond-cluster spinless ET quadrupole of type , is the predominant order parameter in stabilizing helical structures. We further elucidate that the above itinerant spinless ET quadrupole induces a monopolelike orbital angular momentum texture in the momentum space, which can be observed via circular dichroism in soft x-ray photoemission spectroscopy measurement. Our findings highlight a critical role of the orbital angular momentum in chiral materials rather than less dominant spin angular momentum arising from the relativistic spin-orbit coupling.
Physics Subject Headings (PhySH)
Article Text
References (82)
- L. D. Barron, Molecular Light Scattering and Optical Activity (Cambridge University Press, Cambridge, 2004), 2nd ed.
- L. D. Barron, True and false chirality and absolute enantioselection, Rend. Fis. Acc. Lincei 24, 179 (2013).
- M. Hirayama, R. Okugawa, S. Ishibashi, S. Murakami, and T. Miyake, Weyl node and spin texture in trigonal tellurium and selenium, Phys. Rev. Lett. 114, 206401 (2015).
- M. Sakano et al., Radial spin texture in elemental tellurium with chiral crystal structure, Phys. Rev. Lett. 124, 136404 (2020).
- L. E. Vorob’ev, E. L. Ivchenko, G. E. Pikus, I. I. Farbshten, V. A. Shalygin, and A. V. Shturbin, Optical activity in tellurium induced by a current, JETP Lett. 29, 441 (1979).
- T. Yoda, T. Yokoyama, and S. Murakami, Current-induced orbital and spin magnetizations in crystals with helical structure, Sci. Rep. 5, 12024 (2015).
- T. Yoda, T. Yokoyama, and S. Murakami, Orbital Edelstein effect as a condensed-matter analog of solenoids, Nano Lett. 18, 916 (2018).
- V. A. Shalygin, A. N. Sofronov, L. E. Vorob'ev, and I. I. Farbshtein, Current-induced spin polarization of holes in tellurium, Phys. Solid State 54, 2362 (2012).
- T. Furukawa, Y. Shimokawa, K. Kobayashi, and T. Itou, Observation of current-induced bulk magnetization in elemental tellurium, Nat. Commun. 8, 954 (2017).
- T. Furukawa, Y. Watanabe, N. Ogasawara, K. Kobayashi, and T. Itou, Current-induced magnetization caused by crystal chirality in nonmagnetic elemental tellurium, Phys. Rev. Res. 3, 023111 (2021).
- R. Oiwa and H. Kusunose, Rotation, electric-field responses, and absolute enantioselection in chiral crystals, Phys. Rev. Lett. 129, 116401 (2022).
- V. Gopalan and D. B. Litvin, Rotation-reversal symmetries in crystals and handed structures, Nat. Mater. 10, 376 (2011).
- D. M. Lipkin, Existence of a new conservation law in electromagnetic theory, J. Math. Phys. 5, 696 (1964).
- T. W. B. Kibble, Conservation laws for free fields, J. Math. Phys. 6, 1022 (1965).
- I. Proskurin, A. S. Ovchinnikov, P. Nosov, and J.-I. Kishine, Optical chirality in gyrotropic media: Symmetry approach, New J. Phys. 19, 063021 (2017).
- 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).
- S. Hayami, R. Yambe, and H. Kusunose, Analysis of photo-induced chirality and magnetic toroidal moment based on Floquet formalism, J. Phys. Soc. Jpn. 93, 043702 (2024).
- H. Kusunose, J.-I. Kishine, and H. M. Yamamoto, Emergence of chirality from electron spins, physical fields, and material-field composites, Appl. Phys. Lett. 124, 260501 (2024).
- D. Portigal and E. Burstein, Magneto-spatial dispersion effects on the propagation of electro-magnetic radiation in crystals, J. Phys. Chem. Solids 32, 603 (1971).
- G. L. J. A. Rikken and E. Raupach, Observation of magneto-chiral dichroism, Nature (London) 390, 493 (1997).
- T. Yokouchi, N. Kanazawa, A. Kikkawa, D. Morikawa, K. Shibata, T. Arima, Y. Taguchi, F. Kagawa, and Y. Tokura, Electrical magnetochiral effect induced by chiral spin fluctuations, Nat. Commun. 8, 866 (2017).
- G. L. J. A. Rikken and N. Avarvari, Strong electrical magnetochiral anisotropy in tellurium, Phys. Rev. B 99, 245153 (2019).
- R. Aoki, Y. Kousaka, and Y. Togawa, Anomalous nonreciprocal electrical transport on chiral magnetic order, Phys. Rev. Lett. 122, 057206 (2019).
- H. Ishizuka and N. Nagaosa, Anomalous electrical magnetochiral effect by chiral spin-cluster scattering, Nat. Commun. 11, 2986 (2020).
- M. Atzori, C. Train, E. A. Hillard, N. Avarvari, and G. L. J. A. Rikken, Magneto-chiral anisotropy: From fundamentals to perspectives, Chirality 33, 844 (2021).
- M. Suárez-Rodríguez, B. Martín-García, F. Calavalle, S. S. Tsirkin, I. Souza, F. de Juan, A. Fert, M. Gobbi, L. E. Hueso, and F. Casanova, Symmetry origin and microscopic mechanism of electrical magnetochiral anisotropy in tellurium, Phys. Rev. B 111, 024405 (2025).
- R. Naaman and D. H. Waldeck, Chiral-induced spin selectivity effect, J. Phys. Chem. Lett. 3, 2178 (2012).
- D. H. Waldeck, R. Naaman, and Y. Paltiel, The spin selectivity effect in chiral materials, APL Mater. 9, 040902 (2021).
- F. Evers et al., Theory of chirality induced spin selectivity: Progress and challenges, Adv. Mater. 34, 2106629 (2022).
- B. P. Bloom, Y. Paltiel, R. Naaman, and D. H. Waldeck, Chiral induced spin selectivity, Chem. Rev. 124, 1950 (2024).
- K. Ray, S. P. Ananthavel, D. H. Waldeck, and R. Naaman, Asymmetric scattering of polarized electrons by organized organic films of chiral molecules, Science 283, 814 (1999).
- B. Göhler, V. Hamelbeck, T. Z. Markus, M. Kettner, G. F. Hanne, Z. Vager, R. Naaman, and H. Zacharias, Spin selectivity in electron transmission through self-assembled monolayers of double-stranded DNA, Science 331, 894 (2011).
- O. Ben Dor, S. Yochelis, A. Radko, K. Vankayala, E. Capua, A. Capua, S.-H. Yang, L. T. Baczewski, S. S. P. Parkin, R. Naaman, and Y. Paltiel, Magnetization switching in ferromagnets by adsorbed chiral molecules without current or external magnetic field, Nat. Commun. 8, 14567 (2017).
- K. Michaeli, D. N. Beratan, D. H. Waldeck, and R. Naaman, Voltage-induced long-range coherent electron transfer through organic molecules, Proc. Natl. Acad. Sci. USA 116, 5931 (2019).
- R. Naaman, Y. Paltiel, and D. H. Waldeck, Chiral induced spin selectivity gives a new twist on spin-control in chemistry, Acc. Chem. Res. 53, 2659 (2020).
- M. Suda, Y. Thathong, V. Promarak, H. Kojima, M. Nakamura, T. Shiraogawa, M. Ehara, and H. M. Yamamoto, Light-driven molecular switch for reconfigurable spin filters, Nat. Commun. 10, 2455 (2019).
- S. Miwa, K. Kondou, S. Sakamoto, A. Nihonyanagi, F. Araoka, Y. Otani, and D. Miyajima, Chirality-induced effective magnetic field in a phthalocyanine molecule, Appl. Phys. Express 13, 113001 (2020).
- A. Kato, H. M. Yamamoto, and J.-I. Kishine, Chirality-induced spin filtering in pseudo Jahn-Teller molecules, Phys. Rev. B 105, 195117 (2022).
- K. Kondou, M. Shiga, S. Sakamoto, H. Inuzuka, A. Nihonyanagi, F. Araoka, M. Kobayashi, S. Miwa, D. Miyajima, and Y. Otani, Chirality-induced magnetoresistance due to thermally driven spin polarization, J. Am. Chem. Soc. 144, 7302 (2022).
- S. Miwa, T. Yamamoto, T. Nagata, S. Sakamoto, K. Kimura, M. Shiga, W. Gao, H. M. Yamamoto, K. Inoue, T. Takenobu, T. Nozaki, and T. Ohto, Spin polarization driven by molecular vibrations leads to enantioselectivity in chiral molecules, arXiv:2412.03082.
- A. Inui, R. Aoki, Y. Nishiue, K. Shiota, Y. Kousaka, H. Shishido, D. Hirobe, M. Suda, J.-I. Ohe, J.-I. Kishine, H. M. Yamamoto, and Y. Togawa, Chirality-induced spin-polarized state of a chiral crystal , Phys. Rev. Lett. 124, 166602 (2020).
- Y. Nabei, D. Hirobe, Y. Shimamoto, K. Shiota, A. Inui, Y. Kousaka, Y. Togawa, and H. M. Yamamoto, Current-induced bulk magnetization of a chiral crystal , Appl. Phys. Lett. 117, 052408 (2020).
- H. Shishido, R. Sakai, Y. Hosaka, and Y. Togawa, Detection of chirality-induced spin polarization over millimeters in polycrystalline bulk samples of chiral disilicides and , Appl. Phys. Lett. 119, 182403 (2021).
- K. Shiota, A. Inui, Y. Hosaka, R. Amano, Y. Ōnuki, M. Hedo, T. Nakama, D. Hirobe, J.-I. Ohe, J.-I. Kishine, H. M. Yamamoto, H. Shishido, and Y. Togawa, Chirality-induced spin polarization over macroscopic distances in chiral disilicide crystals, Phys. Rev. Lett. 127, 126602 (2021).
- R. Nakajima, D. Hirobe, G. Kawaguchi, Y. Nabei, T. Sato, T. Narushima, H. Okamoto, and H. M. Yamamoto, Giant spin polarization and a pair of antiparallel spins in a chiral superconductor, Nature (London) 613, 479 (2023).
- K. Ohe, H. Shishido, M. Kato, S. Utsumi, H. Matsuura, and Y. Togawa, Chirality-induced selectivity of phonon angular momenta in chiral quartz crystals, Phys. Rev. Lett. 132, 056302 (2024).
- J.-I. Kishine, H. Kusunose, and H. M. Yamamoto, On the definition of chirality and enantioselective fields, Isr. J. Chem. 62, e202200049 (2022).
- A. Inda, R. Oiwa, S. Hayami, H. M. Yamamoto, and H. Kusunose, Quantification of chirality based on electric toroidal monopole, J. Chem. Phys. 160, 184117 (2024).
- T. Miki, H. Ikeda, M.-T. Suzuki, and S. Hoshino, Quantification of electronic asymmetry: Chirality and axiality in solids, Phys. Rev. Lett. 134, 226401 (2025).
- S. S. Tsirkin, P. A. Puente, and I. Souza, Gyrotropic effects in trigonal tellurium studied from first principles, Phys. Rev. B 97, 035158 (2018).
- A. Roy, F. T. Cerasoli, A. Jayaraj, K. Tenzin, M. B. Nardelli, and J. Sławińska, Long-range current-induced spin accumulation in chiral crystals, npj Comput. Mater. 8, 243 (2022).
- Q. Yang, J. Xiao, I. Robredo, M. G. Vergniory, B. Yan, and C. Felser, Monopole-like orbital-momentum locking and the induced orbital transport in topological chiral semimetals, Proc. Natl. Acad. Sci. USA 120, e2305541120 (2023).
- S. S. Brinkman, X. L. Tan, B. Brekke, A. C. Mathisen, O. Finnseth, R. J. Schenk, K. Hagiwara, M.-J. Huang, J. Buck, M. Kalläne, M. Hoesch, K. Rossnagel, K.-H. Ou Yang, M.-T. Lin, G.-J. Shu, Y.-J. Chen, C. Tusche, and H. Bentmann, Chirality-driven orbital angular momentum and circular dichroism in CoSi, Phys. Rev. Lett. 132, 196402 (2024).
- Y. Yen, J. A. Krieger, M. Yao, I. Robredo, K. Manna, Q. Yang, E. C. McFarlane, C. Shekhar, H. Borrmann, S. Stolz, R. Widmer, O. Gröning, V. N. Strocov, S. S. P. Parkin, C. Felser, M. G. Vergniory, M. Schüler, and N. B. M. Schröter, Controllable orbital angular momentum monopoles in chiral topological semimetals, Nat. Phys. 20, 1912 (2024).
- S. Hayami and H. Kusunose, Microscopic description of electric and magnetic toroidal multipoles in hybrid orbitals, J. Phys. Soc. Jpn. 87, 033709 (2018).
- S. Hayami, M. Yatsushiro, Y. Yanagi, and H. Kusunose, Classification of atomic-scale multipoles under crystallographic point groups and application to linear response tensors, Phys. Rev. B 98, 165110 (2018).
- H. Watanabe and Y. Yanase, Group-theoretical classification of multipole order: Emergent responses and candidate materials, Phys. Rev. B 98, 245129 (2018).
- H. Kusunose, R. Oiwa, and S. Hayami, Complete multipole basis set for single-centered electron systems, J. Phys. Soc. Jpn. 89, 104704 (2020).
- S. Hayami and H. Kusunose, Unified description of electronic orderings and cross correlations by complete multipole representation, J. Phys. Soc. Jpn. 93, 072001 (2024).
- H. Kusunose, R. Oiwa, and S. Hayami, Symmetry-adapted modeling for molecules and crystals, Phys. Rev. B 107, 195118 (2023).
- R. Oiwa, A. Inda, S. Hayami, T. Nomoto, R. Arita, and H. Kusunose, Symmetry-adapted closest Wannier modeling based on complete multipole basis set, Phys. Rev. B 112, 035116 (2025).
- T. Ishitobi and K. Hattori, Purely electronic chirality without structural chirality, arXiv:2502.13977.
- K. Nakazawa, T. Yamaguchi, and A. Yamakage, Nonlinear charge transport properties in chiral tellurium, Phys. Rev. Mater. 8, L091601 (2024).
- W. D. Teuchert, R. Geick, G. Landwehr, H. Wendel, and W. Weber, Lattice dynamics of trigonal selenium. I. Phonon spectra, J. Phys. C: Solid State Phys. 8, 3725 (1975).
- M. Cheng, S. Wu, Z.-Z. Zhu, and G.-Y. Guo, Large second-harmonic generation and linear electro-optic effect in trigonal selenium and tellurium, Phys. Rev. B 100, 035202 (2019).
- P. Giannozzi et al., quantum espresso: A modular and open-source software project for quantum simulations of materials, J. Phys.: Condens. Matter 21, 395502 (2009).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- D. R. Hamann, Optimized norm-conserving Vanderbilt pseudopotentials, Phys. Rev. B 88, 085117 (2013).
- M. van Setten, M. Giantomassi, E. Bousquet, M. Verstraete, D. 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).
- P. Ghosh, J. Bhattacharjee, and U. V. Waghmare, The origin of stability of helical structure of tellurium, J. Phys. Chem. C 112, 983 (2008).
- H. Ning, O. Mehio, C. Lian, X. Li, E. Zoghlin, P. Zhou, B. Cheng, S. D. Wilson, B. M. Wong, and D. Hsieh, Light-induced weyl semiconductor-to-metal transition mediated by Peierls instability, Phys. Rev. B 106, 205118 (2022).
- P. Tangney and S. Fahy, Density-functional theory approach to ultrafast laser excitation of semiconductors: Application to the phonon in tellurium, Phys. Rev. B 65, 054302 (2002).
- A. M.-T. Kim, C. A. D. Roeser, and E. Mazur, Modulation of the bonding-antibonding splitting in Te by coherent phonons, Phys. Rev. B 68, 012301 (2003).
- S. L. Johnson, E. Vorobeva, P. Beaud, C. J. Milne, and G. Ingold, Full reconstruction of a crystal unit cell structure during coherent femtosecond motion, Phys. Rev. Lett. 103, 205501 (2009).
- A. Decker, G. A. Landrum, and R. Dronskowski, Structural and electronic Peierls distortions in the elements (a): The crystal structure of tellurium, Z. Anorg. Allg. Chem. 628, 295 (2002).
- C. Hejny, S. Falconi, L. F. Lundegaard, and M. I. McMahon, Phase transitions in tellurium at high pressure and temperature, Phys. Rev. B 74, 174119 (2006).
- C. Marini, D. Chermisi, M. Lavagnini, D. Di Castro, C. Petrillo, L. Degiorgi, S. Scandolo, and P. Postorino, High-pressure phases of crystalline tellurium: A combined Raman and ab initio study, Phys. Rev. B 86, 064103 (2012).
- P. P. Ewald, Die Berechnung optischer und elektrostatischer Gitterpotentiale, Ann. Phys. 369, 253 (1921).
- T. Ozaki, Closest Wannier functions to a given set of localized orbitals, Phys. Rev. B 110, 125115 (2024).
- S. Hayami, Y. Yanagi, and H. Kusunose, Bottom-up design of spin-split and reshaped electronic band structures in antiferromagnets without spin-orbit coupling: Procedure on the basis of augmented multipoles, Phys. Rev. B 102, 144441 (2020).
- R. Oiwa and H. Kusunose, Systematic analysis method for nonlinear response tensors, J. Phys. Soc. Jpn. 91, 014701 (2022).
- K. Ishito, H. Mao, Y. Kousaka, Y. Togawa, S. Iwasaki, T. Zhang, S. Murakami, J.-I. Kishine, and T. Satoh, Truly chiral phonons in -HgS, Nat. Phys. 19, 35 (2023).