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Abstract Helical spin structures are expressions of magnetically induced chirality, entangling the dipolar and magnetic orders in materials1–4. The recent discovery of helical van der Waals multiferroics down to the ultrathin limit raises prospects of large chiral magnetoelectric correlations in two dimensions5,6. However, the exact nature and magnitude of these couplings have remained unknown so far. Here we perform a precision measurement of the dynamical magnetoelectric coupling for an enantiopure domain in an exfoliated van der Waals multiferroic. We evaluate this interaction in resonance with a collective electromagnon mode, capturing the impact of its oscillations on the dipolar and magnetic orders of the material with a suite of ultrafast optical probes. Our data show a giant natural optical activity at terahertz frequencies, characterized by quadrature modulations between the electric polarization and magnetization components. First-principles calculations further show that these chiral couplings originate from the synergy between the non-collinear spin texture and relativistic spin–orbit interactions, resulting in substantial enhancements over lattice-mediated effects. Our findings highlight the potential for intertwined orders to enable unique functionalities in the two-dimensional limit and pave the way for the development of van der Waals magnetoelectric devices operating at terahertz speeds.
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This content will become publicly available on February 1, 2026
Dispersive Dark Excitons in van der Waals Ferromagnet CrI3
Spin-flip dark excitons are optical-dipole-forbidden quasiparticles with remarkable potential in optoelectronics, especially when they are realized within cleavable van der Waals materials. Despite this potential, dark excitons have not yet been definitively identified in ferromagnetic van der Waals materials. Here, we report two dark excitons in a model ferromagnetic material CrI3 using high-resolution resonant inelastic x-ray scattering and show that they feature narrower linewidths compared to the bright excitons previously reported in this material. These excitons are shown to have spin-flip character, to disperse as a function of momentum, and to change through the ferromagnetic transition temperature. Given the versatility of van der Waals materials, these excitons hold promise for new types of magneto-optical functionality.
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- Award ID(s):
- 2441874
- PAR ID:
- 10657270
- Publisher / Repository:
- American Physical Society (APS)
- Date Published:
- Journal Name:
- Physical Review X
- Volume:
- 15
- Issue:
- 1
- ISSN:
- 2160-3308
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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