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Orbital multiferroicity in pentalayer rhombohedral graphene

Tonghang Han, Zhengguang Lu, Giovanni Scuri, Jiho Sung, Jue Wang, Tianyi Han, Kenji Watanabe, Takashi Taniguchi, Liang Fu, Hongkun Park and Long Ju ()
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Tonghang Han: Massachusetts Institute of Technology
Zhengguang Lu: Massachusetts Institute of Technology
Giovanni Scuri: Harvard University
Jiho Sung: Harvard University
Jue Wang: Harvard University
Tianyi Han: Massachusetts Institute of Technology
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Liang Fu: Massachusetts Institute of Technology
Hongkun Park: Harvard University
Long Ju: Massachusetts Institute of Technology

Nature, 2023, vol. 623, issue 7985, 41-47

Abstract: Abstract Ferroic orders describe spontaneous polarization of spin, charge and lattice degrees of freedom in materials. Materials exhibiting multiple ferroic orders, known as multiferroics, have important parts in multifunctional electrical and magnetic device applications1–4. Two-dimensional materials with honeycomb lattices offer opportunities to engineer unconventional multiferroicity, in which the ferroic orders are driven purely by the orbital degrees of freedom and not by electron spin. These include ferro-valleytricity corresponding to the electron valley5 and ferro-orbital-magnetism6 supported by quantum geometric effects. These orbital multiferroics could offer strong valley–magnetic couplings and large responses to external fields—enabling device applications such as multiple-state memory elements and electric control of the valley and magnetic states. Here we report orbital multiferroicity in pentalayer rhombohedral graphene using low-temperature magneto-transport measurements. We observed anomalous Hall signals Rxy with an exceptionally large Hall angle (tanΘH > 0.6) and orbital magnetic hysteresis at hole doping. There are four such states with different valley polarizations and orbital magnetizations, forming a valley–magnetic quartet. By sweeping the gate electric field E, we observed a butterfly-shaped hysteresis of Rxy connecting the quartet. This hysteresis indicates a ferro-valleytronic order that couples to the composite field E · B (where B is the magnetic field), but not to the individual fields. Tuning E would switch each ferroic order independently and achieve non-volatile switching of them together. Our observations demonstrate a previously unknown type of multiferroics and point to electrically tunable ultralow-power valleytronic and magnetic devices.

Date: 2023
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DOI: 10.1038/s41586-023-06572-w

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