Nonlinear Optical Response in Layer-Stacked Gallenene with Ferroelectric Polarization

Author(s)
Muhammad Yunusa, Andrew K. Schulz, Tim Parker, Felix Schneider, Kenan Elibol, Marius Predel, Jana Dzíbelová, Michel Rebmann, Taylan Gorkan, Jiahao Ye, Jin Chong Tan, Wenbin Kang, Peter A. van Aken, Alfred J. Meixner, Engin Durgun, Jani Kotakoski, Dai Zhang, Metin Sitti
Abstract

Polar metals are very rare and challenging to realize due to the incompatibility of ferroelectricity and metallicity. Mobile electrons in polar metals effectively screen the static electric field and dipoles. Recent studies show that 2D van der Waals metals without an inversion center can have polar order due to specific layer stacking. However, room temperature reversible ferroelectricity and nonlinear second harmonic generation in non-centrosymmetric polar metals remain unrealized. Here, the experimental realization of AB-stacked gallenene (a100) nanocrystals with a room temperature ferroelectric polarization in a liquid gallium environment is reported. Using first-principles calculations, the origin of spontaneous polarization (Ps) due to a broken symmetry in multilayer gallenene structures, resulting in P1 (space group) and C1 (point group) symmetry is explained. The reversible polarization switching is characterized using piezoresponse force microscopy. This results demonstrate the reversible nonlinear optical response of the AB-stacked gallenene crystal through second harmonic generation (SHG) microscopy. The intensities of SHG signals are controlled via angular rotations and thermal heating, which indicate a phase transition at high temperatures. Furthermore, electrical perturbation enables the tunability of SHG intensity. Bipolar resistive switching is demonstrated in a two-terminal device. These findings open avenues for advancements in 2D ferroelectricity, piezoelectricity, and topological superconductivity.

Organisation(s)
Physics of Nanostructured Materials
External organisation(s)
Max Planck Institute for Intelligent Systems, Eberhard Karls Universität Tübingen, Max-Planck-Institut für Festkörperforschung, Bilkent University, University of Oxford, City University of Hong Kong (CityU), Koc University
Journal
Advanced Materials
Volume
37
No. of pages
14
ISSN
0935-9648
DOI
https://doi.org/10.1002/adma.202501058
Publication date
11-2025
Peer reviewed
Yes
Austrian Fields of Science 2012
103018 Materials physics
Keywords
ASJC Scopus subject areas
General Materials Science, Mechanics of Materials, Mechanical Engineering
Portal url
https://ucrisportal.univie.ac.at/en/publications/92f84842-01ee-4c71-abcb-40f1502a3299