Nonlinear Optical Response in Layer‐Stacked Gallenene with Ferroelectric Polarization

M Muhammad Yunusa (Physical Intelligence Department Max Planck Institute for Intelligent Systems 70569 Stuttgart Germany) A Andrew K. Schulz (Max Planck Institute for Intelligent Systems 70569 Stuttgart Germany) T Tim Parker (Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany) F Felix Schneider K Kenan Elibol (Max Planck Institute for Solid State Research 70569 Stuttgart Germany) M Marius Predel (Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria) J Jana Dzíbelová (Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria) M Michel Rebmann (Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany) T Taylan Gorkan (UNAM‐National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology Bilkent University Ankara 06800 Turkey) J Jiahao Ye J Jin‐Chong Tan (Multifunctional Materials and Composites (MMC) Laboratory Department of Engineering Science University of Oxford Oxford OX1 3PJ UK) W Wenbin Kang P Peter A. van Aken (Max Planck Institute for Solid State Research, Heisenbergstr. 1, Stuttgart 70569, Germany) A Alfred J. Meixner (Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany) E Engin Durgun (UNAM‐National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology Bilkent University Ankara 06800 Turkey) J Jani Kotakoski (Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria) D Dai Zhang M Metin Sitti

Abstract

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.

Article Details

Volume / Issue Vol. 37, Issue 44
Published November 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (18)

M

Muhammad Yunusa

Physical Intelligence Department Max Planck Institute for Intelligent Systems 70569 Stuttgart Germany

A

Andrew K. Schulz

Max Planck Institute for Intelligent Systems 70569 Stuttgart Germany

T

Tim Parker

Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany

F

Felix Schneider

K

Kenan Elibol

Max Planck Institute for Solid State Research 70569 Stuttgart Germany

M

Marius Predel

Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria

J

Jana Dzíbelová

Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria

M

Michel Rebmann

Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany

T

Taylan Gorkan

UNAM‐National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology Bilkent University Ankara 06800 Turkey

J

Jiahao Ye

J

Jin‐Chong Tan

Multifunctional Materials and Composites (MMC) Laboratory Department of Engineering Science University of Oxford Oxford OX1 3PJ UK

W

Wenbin Kang

P

Peter A. van Aken

Max Planck Institute for Solid State Research, Heisenbergstr. 1, Stuttgart 70569, Germany

A

Alfred J. Meixner

Institute of Physical and Theoretical Chemistry Eberhard Karls University of Tübingen Auf der Morgenstelle 15 72076 Tübingen Germany

E

Engin Durgun

UNAM‐National Nanotechnology Research Center and Institute of Materials Science and Nanotechnology Bilkent University Ankara 06800 Turkey

J

Jani Kotakoski

Faculty of Physics University of Vienna Boltzmanngasse 5 Vienna 1090 Austria

D

Dai Zhang

M

Metin Sitti