Hydrogen-induced tunable remanent polarization in a perovskite nickelate

Yifan Yuan; Michele Kotiuga; Tae Joon Park; Ranjan Kumar Patel; Yuanyuan Ni; Arnob Saha; Hua Zhou; Jerzy T Sadowski; Abdullah Al-Mahboob; Haoming Yu; Kai Du; Minning Zhu; Sunbin Deng; Ravindra S Bisht; Xiao Lyu; Chung-Tse Michael Wu; Peide D Ye; Abhronil Sengupta; Sang-Wook Cheong; Xiaoshan Xu; Karin M Rabe; Shriram Ramanathan

doi:10.1038/s41467-024-49213-0

Hydrogen-induced tunable remanent polarization in a perovskite nickelate

Nat Commun. 2024 Jun 3;15(1):4717. doi: 10.1038/s41467-024-49213-0.

Authors

Yifan Yuan^#¹, Michele Kotiuga^#², Tae Joon Park^#³, Ranjan Kumar Patel⁴, Yuanyuan Ni⁵, Arnob Saha⁶, Hua Zhou⁷, Jerzy T Sadowski⁸, Abdullah Al-Mahboob⁸, Haoming Yu⁹, Kai Du¹⁰, Minning Zhu⁴, Sunbin Deng⁹, Ravindra S Bisht⁴, Xiao Lyu¹¹, Chung-Tse Michael Wu⁴, Peide D Ye¹¹, Abhronil Sengupta⁶, Sang-Wook Cheong¹⁰, Xiaoshan Xu⁵, Karin M Rabe¹⁰, Shriram Ramanathan¹²

Affiliations

¹ Department of Electrical & Computer Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ, USA. yifan.yuan10@gmail.com.
² Theory and Simulation of Materials (THEOS), National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland. mkotiuga@materialsdesign.com.
³ School of Materials Engineering, Purdue University, West Lafayette, IN, USA. tjp059@gmail.com.
⁴ Department of Electrical & Computer Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ, USA.
⁵ Department of Physics and Astronomy, University of Nebraska-Lincoln, Lincoln, NE, USA.
⁶ School of Electrical Engineering and Computer Science, The Pennsylvania State University, University Park, State College, PA, USA.
⁷ X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Lemont, IL, USA.
⁸ Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY, USA.
⁹ School of Materials Engineering, Purdue University, West Lafayette, IN, USA.
¹⁰ Department of Physics and Astronomy, Rutgers, The State University of New Jersey, Piscataway, NJ, USA.
¹¹ School of Electrical and Computer Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, IN, USA.
¹² Department of Electrical & Computer Engineering, Rutgers, The State University of New Jersey, Piscataway, NJ, USA. shriram.ramanathan@rutgers.edu.

^# Contributed equally.

Abstract

Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO₃ into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second which is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing ferroelectric materials and electrets using light-ion doping.