Giant and broadband circular dichroism from particle–hole symmetry breaking in Weyl semimetals
Source abstract
Abstract
Circular dichroism originates from symmetry breaking in a material structure and leads to differential absorption of left-handed and right-handed circularly polarized light. However, circular dichroism in most materials is inherently weak and spectrally narrow, especially in the mid-to-far infrared. Here we uncover giant infrared circular dichroism in the magnetic-field-forced Weyl semimetal Mn(Bi,Sb)2Te4 driven by extreme particle-hole symmetry breaking. Helicity-resolved magneto-infrared spectroscopy reveals circular dichroism exceeding 3,000 mdeg (~130 mdeg nm-1) with an above-degree response extending over the 6-13 μm spectral range. The optical resonances are enhanced by a strong band nesting effect intrinsic to the Landau levels of type-II Weyl dispersion. A symmetry-based k·p model reproduces these magneto-infrared responses and demonstrates that magnetization-induced asymmetric spin-orbit coupling generates particle-hole symmetry breaking, which suppresses spin-up, parity-even wavefunction components in the valence Landau band and thereby produces pronounced optical helicity-selectivity. Our findings establish particle-hole symmetry breaking as an effective route towards helicity-resolved optical control in quantum materials.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Topological Materials and Phenomena · Metamaterials and Metasurfaces Applications · 2D Materials and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (94)
Show source-provided references
1. Beaulieu, S. et al. Photoexcitation circular dichroism in chiral molecules. Nat. Phys. 14, 484–489 (2018).10.1038/s41567-017-0038-z ↗
2. Long, G. et al. Chiral-perovskite optoelectronics. Nat. Rev. Mater. 5, 423–439 (2020).10.1038/s41578-020-0181-5 ↗
3. Parrish, K. A. et al. Differential absorption of circularly polarized light by a centrosymmetric crystal. Science 388, 1194–1197 (2025).10.1126/science.adr5478 ↗
4. Ugras, T. J. et al. Transforming achiral semiconductors into chiral domains with exceptional circular dichroism. Science 387, eado7201 (2025).10.1126/science.ado7201 ↗
5. Rodgers, D. S. Circular Dichroism: Theory and Spectroscopy (Nova Science Publishers, 2012).
6. Mason, W. R. A Practical Guide to Magnetic Circular Dichroism Spectroscopy (Wiley-Interscience, 2007).10.1002/9780470139233 ↗
7. Busch, K. L. & Busch, M. A. Chiral Analysis (Elsevier, 2006).
8. Yang, R. Inherent circular dichroism of phonons in magnetic Weyl semimetal Co3Sn2S2. Phys. Rev. Lett. 134, 196905 (2025).10.1103/PhysRevLett.134.196905 ↗
9. Yu, R., Weng, H., Fang, Z., Ding, H. & Dai, X. Determining the chirality of Weyl fermions from circular dichroism spectra in time-dependent angle-resolved photoemission. Phys. Rev. B 93, 205133 (2016).10.1103/PhysRevB.93.205133 ↗
10. Bertrand, S., Parent, J.-M., Côté, R. & Garate, I. Complete optical valley polarization in Weyl semimetals in strong magnetic fields. Phys. Rev. B 100, 075107 (2019).10.1103/PhysRevB.100.075107 ↗
11. Li, J. et al. Magnetically controllable topological quantum phase transitions in the antiferromagnetic topological insulator MnBi2Te4. Phys. Rev. B 100, 121103 (2019).10.1103/PhysRevB.100.121103 ↗
12. Li, J. et al. Intrinsic magnetic topological insulators in van der Waals layered MnBi2Te4-family materials. Sci. Adv. 5, eaaw5685 (2019).10.1126/sciadv.aaw5685 ↗
13. Lee, S. H. et al. Evidence for a magnetic-field-induced ideal type-II Weyl state in antiferromagnetic topological insulator Mn(Bi1−xSbx)2Te4. Phys. Rev. X 11, 031032 (2021).
14. Jiang, Q. et al. Revealing Fermi surface evolution and Berry curvature in an ideal type-II Weyl semimetal. Nat. Commun. 15, 2310 (2024).10.1038/s41467-024-46633-w ↗
15. Ma, H.-Y. et al. Multifunctional antiferromagnetic materials with giant piezomagnetism and noncollinear spin current. Nat. Commun. 12, 2846 (2021).10.1038/s41467-021-23127-7 ↗
16. Berciu, M. et al. Origin of magnetic circular dichroism in GaMnAs: giant Zeeman splitting versus spin dependent density of states. Phys. Rev. Lett. 102, 247202 (2009).10.1103/PhysRevLett.102.247202 ↗
17. Zhang, H. et al. Topological insulators in Bi2Se3, Bi2Te3 and Sb2Te3 with a single Dirac cone on the surface. Nat. Phys. 5, 438–442 (2009).10.1038/nphys1270 ↗
18. Zhang, D. et al. Topological axion states in the magnetic insulator MnBi2Te4 with the quantized magnetoelectric effect. Phys. Rev. Lett. 122, 206401 (2019).10.1103/PhysRevLett.122.206401 ↗
19. Wu, W. et al. The discovery of three-dimensional Van Hove singularity. Nat. Commun. 15, 2313 (2024).10.1038/s41467-024-46626-9 ↗
20. Santos-Cottin, D. et al. EuCd2As2: a magnetic semiconductor. Phys. Rev. Lett. 131, 186704 (2023).10.1103/PhysRevLett.131.186704 ↗
21. Schmutz, L. E., Dresselhaus, G. & Dresselhaus, M. S. Optical absorption of EuTe in high magnetic fields. Solid State Commun. 28, 597–600 (1978).10.1016/0038-1098(78)90588-4 ↗
22. Xu, B. et al. Infrared study of the multiband low-energy excitations of the topological antiferromagnet MnBi2Te4. Phys. Rev. B 103, L121103 (2021).10.1103/PhysRevB.103.L121103 ↗
23. Yu, Z.-M., Yao, Y. & Yang, S. A. Predicted unusual magnetoresponse in type-II Weyl semimetals. Phys. Rev. Lett. 117, 077202 (2016).10.1103/PhysRevLett.117.077202 ↗
24. Carvalho, A., Ribeiro, R. M. & Castro Neto, A. H. Band nesting and the optical response of two-dimensional semiconducting transition metal dichalcogenides. Phys. Rev. B 88, 115205 (2013).10.1103/PhysRevB.88.115205 ↗
25. Rodger, A. & Norden, B. Circular Dichroism and Linear Dichroism (Oxford Univ. Press, 1997).10.1093/oso/9780198558972.001.0001 ↗
26. Barron, L. D. Molecular Light Scattering and Optical Activity (Cambridge Univ. Press, 2004).10.1017/CBO9780511535468 ↗
27. Jiang, Y. et al. Landau-level spectroscopy of massive Dirac fermions in single-crystalline ZrTe5 thin flakes. Phys. Rev. B 96, 041101 (2017).10.1103/PhysRevB.96.041101 ↗
28. Orlita, M. et al. Magneto-optics of massive Dirac fermions in bulk Bi2Se3. Phys. Rev. Lett. 114, 186401 (2015).10.1103/PhysRevLett.114.186401 ↗
29. Ma, Q. et al. Direct optical detection of Weyl fermion chirality in a topological semimetal. Nat. Phys. 13, 842–847 (2017).10.1038/nphys4146 ↗
30. Ma, J. et al. Nonlinear photoresponse of type-II Weyl semimetals. Nat. Mater. 18, 476–481 (2019).10.1038/s41563-019-0296-5 ↗
31. Xu, B. et al. Temperature-tunable Fano resonance induced by strong coupling between Weyl fermions and phonons in TaAs. Nat. Commun. 8, 14933 (2017).10.1038/ncomms14933 ↗
32. Mukherjee, S. P. & Carbotte, J. P. Absorption of circular polarized light in tilted type-I and type-II Weyl semimetals. Phys. Rev. B 96, 085114 (2017).10.1103/PhysRevB.96.085114 ↗
33. Li, H. et al. Collective chiroptical activity through the interplay of excitonic and charge-transfer effects in localized plasmonic fields. Nat. Commun. 15, 4846 (2024).10.1038/s41467-024-49086-3 ↗
34. Albano, G., Pescitelli, G. & Di Bari, L. Chiroptical properties in thin films of π-conjugated systems. Chem. Rev. 120, 10145–10243 (2020).10.1021/acs.chemrev.0c00195 ↗
35. Ma, S. et al. Elucidating the origin of chiroptical activity in chiral 2D perovskites through nano-confined growth. Nat. Commun. 13, 3259 (2022).10.1038/s41467-022-31017-9 ↗
36. Chen, C. et al. Circularly polarized light detection using chiral hybrid perovskite. Nat. Commun. 10, 1927 (2019).10.1038/s41467-019-09942-z ↗
37. Kim, R. M. et al. Enantioselective sensing by collective circular dichroism. Nature 612, 470–476 (2022).10.1038/s41586-022-05353-1 ↗
38. Gansel, J. K. et al. Gold helix photonic metamaterial as broadband circular polarizer. Science 325, 1513–1515 (2009).10.1126/science.1177031 ↗
39. Xie, H. et al. Twist engineering of the two-dimensional magnetism in double bilayer chromium triiodide homostructures. Nat. Phys. 18, 30–36 (2022).10.1038/s41567-021-01408-8 ↗
40. Srivastava, A. et al. Valley Zeeman effect in elementary optical excitations of monolayer WSe2. Nat. Phys. 11, 141–147 (2015).10.1038/nphys3203 ↗
41. Li, J. et al. Spontaneous valley polarization of interacting carriers in a monolayer semiconductor. Phys. Rev. Lett. 125, 147602 (2020).10.1103/PhysRevLett.125.147602 ↗
42. Kim, J. et al. Observation of ultralong valley lifetime in WSe2/MoS2 heterostructures. Sci. Adv. 3, e1700518 (2017).10.1126/sciadv.1700518 ↗
43. Du, M.-H., Yan, J., Cooper, V. R. & Eisenbach, M. Tuning Fermi levels in intrinsic antiferromagnetic topological insulators MnBi2Te4 and MnBi4Te7 by defect engineering and chemical doping. Adv. Funct. Mater. 31, 2006516 (2021).10.1002/adfm.202006516 ↗
44. Yan, J.-Q. et al. Evolution of structural, magnetic, and transport properties in MnBi2−xSbxTe4. Phys. Rev. B 100, 104409 (2019).10.1103/PhysRevB.100.104409 ↗
45. Riberolles, S. X. M. et al. Evolution of magnetic interactions in Sb-substituted MnBi2Te4. Phys. Rev. B 104, 064401 (2021).10.1103/PhysRevB.104.064401 ↗
46. Jiang, Q.-D., Jiang, H., Liu, H., Sun, Q.-F. & Xie, X. C. Chiral wave-packet scattering in Weyl semimetals. Phys. Rev. B 93, 195165 (2016).10.1103/PhysRevB.93.195165 ↗
47. Liang, T. et al. Ultrahigh mobility and giant magnetoresistance in the Dirac semimetal Cd3As2. Nat. Mater. 14, 280–284 (2015).10.1038/nmat4143 ↗
48. Otrokov, M. M. et al. Unique thickness-dependent properties of the van der Waals interlayer antiferromagnet MnBi2Te4 films. Phys. Rev. Lett. 122, 107202 (2019).10.1103/PhysRevLett.122.107202 ↗
49. Lin, W. et al. Direct visualization of edge state in even-layer MnBi2Te4 at zero magnetic field. Nat. Commun. 13, 7714 (2022).10.1038/s41467-022-35482-0 ↗
50. Li, Y. et al. Giant nonlocal edge conduction in the axion insulator state of MnBi2Te4. Sci. Bull. 68, 1252–1258 (2023).10.1016/j.scib.2023.05.011 ↗
51. Liu, C. et al. Robust axion insulator and Chern insulator phases in a two-dimensional antiferromagnetic topological insulator. Nat. Mater. 19, 522–527 (2020).10.1038/s41563-019-0573-3 ↗
52. Deng, Y. et al. Quantum anomalous Hall effect in intrinsic magnetic topological insulator MnBi2Te4. Science 367, 895–900 (2020).10.1126/science.aax8156 ↗
53. Lian, Z. et al. Antiferromagnetic quantum anomalous Hall effect under spin flips and flops. Nature 641, 70–75 (2025).10.1038/s41586-025-08860-z ↗
54. Zhang, C. et al. Zero-field chiral edge transport in an intrinsic magnetic topological insulator MnBi2Te4. Nat. Commun. 16, 5587 (2025).10.1038/s41467-025-59160-z ↗
55. Wang, Y. et al. Towards the quantized anomalous Hall effect in AlOx-capped MnBi2Te4. Nat. Commun. 16, 1727 (2025).10.1038/s41467-025-57039-7 ↗
56. Bai, Y. et al. Quantized anomalous Hall resistivity achieved in molecular beam epitaxy-grown MnBi2Te4 thin films. Natl Sci. Rev. 11, nwad189 (2024).10.1093/nsr/nwad189 ↗
57. Ghosh, B. et al. Probing quantum geometry through optical conductivity and magnetic circular dichroism. Sci. Adv. 10, eado1761 (2024).10.1126/sciadv.ado1761 ↗
58. Gao, A. et al. Layer Hall effect in a 2D topological axion antiferromagnet. Nature 595, 521–525 (2021).10.1038/s41586-021-03679-w ↗
59. Qiu, J.-X. et al. Axion optical induction of antiferromagnetic order. Nat. Mater. 22, 583–590 (2023).10.1038/s41563-023-01493-5 ↗
60. Ahn, J., Xu, S.-Y. & Vishwanath, A. Theory of optical axion electrodynamics and application to the Kerr effect in topological antiferromagnets. Nat. Commun. 13, 7615 (2022).10.1038/s41467-022-35248-8 ↗
61. Wu, L. et al. Quantized Faraday and Kerr rotation and axion electrodynamics of a 3D topological insulator. Science 354, 1124–1127 (2016).10.1126/science.aaf5541 ↗
62. Lei, C. & MacDonald, A. H. Kerr, Faraday, and magnetoelectric effects in MnBi2Te4 thin films. Phys. Rev. B 108, 125424 (2023).10.1103/PhysRevB.108.125424 ↗
63. Ge, J. et al. High-Chern-number and high-temperature quantum Hall effect without Landau levels. Natl Sci. Rev. 7, 1280–1287 (2020).10.1093/nsr/nwaa089 ↗
64. Cai, J. et al. Electric control of a canted-antiferromagnetic Chern insulator. Nat. Commun. 13, 1668 (2022).10.1038/s41467-022-29259-8 ↗
65. Chong, S. K. et al. Anomalous Landau quantization in intrinsic magnetic topological insulators. Nat. Commun. 14, 4805 (2023).10.1038/s41467-023-40383-x ↗
66. Liu, C. et al. Magnetic-field-induced robust zero Hall plateau state in MnBi2Te4 Chern insulator. Nat. Commun. 12, 4647 (2021).10.1038/s41467-021-25002-x ↗
67. Bac, S.-K. et al. Probing Berry curvature in magnetic topological insulators through resonant infrared magnetic circular dichroism. Phys. Rev. Lett. 134, 016601 (2025).10.1103/PhysRevLett.134.016601 ↗
68. Otrokov, M. M. et al. Prediction and observation of an antiferromagnetic topological insulator. Nature 576, 416–422 (2019).10.1038/s41586-019-1840-9 ↗
69. Li, H. et al. Dirac surface states in intrinsic magnetic topological insulators EuSn2As2 and MnBi2nTe3n+1. Phys. Rev. X 9, 041039 (2019).
70. Ma, X.-M. et al. Realization of a tunable surface Dirac gap in Sb-doped MnBi2Te4. Phys. Rev. B 103, L121112 (2021).10.1103/PhysRevB.103.L121112 ↗
71. Zhang, E. et al. Observation of edge supercurrent in topological antiferromagnet MnBi2Te4-based Josephson junctions. Sci. Adv. 11, eads8730 (2025).10.1126/sciadv.ads8730 ↗
72. Shi, Z. et al. A high-flux and high-efficiency setup for magneto-infrared spectroscopy. Rev. Sci. Instrum. 96, 113902 (2025).10.1063/5.0296925 ↗
73. Kliger, D. S., Lewis, J. W. & Randall, C. E. Polarized Light in Optics and Spectroscopy (Academic, 1990).10.1016/B978-0-08-057104-1.50011-9 ↗
74. Kobayashi, N., Muranaka, A. & Mack, J. Circular Dichroism and Magnetic Circular Dichroism Spectroscopy for Organic Chemists (Royal Society of Chemistry, 2011).10.1039/9781849732932 ↗
75. Višňovský, Š. & Krishnan, R. Complex Faraday effect in multilayer structures. J. Opt. Soc. Am. 71, 315 (1981).10.1364/JOSA.71.000315 ↗
76. Silverman, M. P. & Sohn, R. B. Effects of circular birefringence on light propagation and reflection. Am. J. Phys. 54, 69–76 (1986).10.1119/1.14745 ↗
77. Dillon, J. F. Origin and uses of the Faraday rotation in magnetic crystals. J. Appl. Phys. 39, 922–929 (1968).10.1063/1.1656335 ↗
78. Kuzmenko, A. B. Kramers–Kronig constrained variational analysis of optical spectra. Rev. Sci. Instrum. 76, 083108 (2005).10.1063/1.1979470 ↗
79. Hayashi, M. et al. Magneto-optical Kerr rotation spectra in Fe ultrathin film on noble metals. J. Magn. Magn. Mater. 126, 547–549 (1993).10.1016/0304-8853(93)90684-T ↗
80. Yan, B. Structural chirality and electronic chirality in quantum materials. Annu. Rev. Mater. Res. 54, 97–115 (2024).10.1146/annurev-matsci-080222-033548 ↗
81. Chen, B. et al. Intrinsic magnetic topological insulator phases in the Sb doped MnBi2Te4 bulks and thin flakes. Nat. Commun. 10, 4469 (2019).10.1038/s41467-019-12485-y ↗
82. Ai, M. et al. Spin selection in atomic-level chiral metal oxide for photocatalysis. Nat. Commun. 14, 4562 (2023).10.1038/s41467-023-40367-x ↗
83. Chen, T.-L. et al. A 2D chiral microcavity based on apparent circular dichroism. Nat. Commun. 15, 3072 (2024).10.1038/s41467-024-47411-4 ↗
84. Hentschel, M., Schäferling, M., Duan, X., Giessen, H. & Liu, N. Chiral plasmonics. Sci. Adv. 3, e1602735 (2017).10.1126/sciadv.1602735 ↗
85. Kim, K. et al. Chiral-phonon-activated spin Seebeck effect. Nat. Mater. 22, 322–328 (2023).10.1038/s41563-023-01473-9 ↗
86. Kimura, K., Otake, Y. & Kimura, T. Visualizing rotation and reversal of the Néel vector through antiferromagnetic trichroism. Nat. Commun. 13, 697 (2022).10.1038/s41467-022-28215-w ↗
87. Li, S. et al. Large exchange-driven intrinsic circular dichroism of a chiral 2D hybrid perovskite. Nat. Commun. 15, 2573 (2024).10.1038/s41467-024-46851-2 ↗
88. Sun, R. et al. Colossal anisotropic absorption of spin currents induced by chirality. Sci. Adv. 10, eadn3240 (2024).10.1126/sciadv.adn3240 ↗
89. Yao, Z.-F. et al. Lattice-guided assembly of optoelectronically active π-conjugated peptides on 1D van der Waals single crystals. Sci. Adv. 10, eadl2402 (2024).10.1126/sciadv.adl2402 ↗
90. Ahn, J. et al. Chiral 2D organic inorganic hybrid perovskite with circular dichroism tunable over wide wavelength range. J. Am. Chem. Soc. 142, 4206–4212 (2020).10.1021/jacs.9b11453 ↗
91. Gao, X. et al. Detecting electronic structure evolution of semiconductor nanocrystals by magnetic circular dichroism spectroscopy. Nanoscale 11, 19380–19386 (2019).10.1039/C9NR03630J ↗
92. Gromova, Y. A. et al. Magnetic circular dichroism in 2D colloidal semiconductor nanocrystals. Opt. Spectrosc. 125, 698–702 (2018).10.1134/S0030400X18110139 ↗
93. Parashar, N. D., Chiu, P. T. & Wessels, B. W. Reflectance magnetic circular dichroism studies at the Γ-point in InMnAs semiconductor films. Phys. E 41, 1147–1150 (2009).10.1016/j.physe.2008.12.027 ↗
94. Ando, K. & Akinaga, H. Optical study of the magnetic phase transition in Cd1−xMnxTe. J. Magn. Magn. Mater. 140–144, 2029–2030 (1995).10.1016/0304-8853(94)00712-8 ↗