Giant chiral magnetoelectric oscillations in a van der Waals multiferroic

Frank Y. Gao, Xinyue Peng, Xinle Cheng, Emil Viñas Boström, Dong Seob Kim, Ravish K. Jain, Deepak Vishnu, Kalaivanan Raju, Raman Sankar, Shang-Fan Lee, Michael A. Sentef, Takashi Kurumaji, Xiaoqin Li, Peizhe Tang, Angel Rubio () and Edoardo Baldini ()
Additional contact information
Frank Y. Gao: The University of Texas at Austin
Xinyue Peng: The University of Texas at Austin
Xinle Cheng: Max Planck Institute for the Structure and Dynamics of Matter
Emil Viñas Boström: Max Planck Institute for the Structure and Dynamics of Matter
Dong Seob Kim: The University of Texas at Austin
Ravish K. Jain: Academia Sinica
Deepak Vishnu: Academia Sinica
Kalaivanan Raju: Academia Sinica
Raman Sankar: Academia Sinica
Shang-Fan Lee: Academia Sinica
Michael A. Sentef: Max Planck Institute for the Structure and Dynamics of Matter
Takashi Kurumaji: California Institute of Technology
Xiaoqin Li: The University of Texas at Austin
Peizhe Tang: Max Planck Institute for the Structure and Dynamics of Matter
Angel Rubio: Max Planck Institute for the Structure and Dynamics of Matter
Edoardo Baldini: The University of Texas at Austin

Nature, 2024, vol. 632, issue 8024, 273-279

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41586-024-07678-5

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