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Title: Electron‐Doping Mottronics in Strongly Correlated Perovskite
Abstract

The discovery of hydrogen‐induced electron localization and highly insulating states in d‐band electron correlated perovskites has opened a new paradigm for exploring novel electronic phases of condensed matters and applications in emerging field‐controlled electronic devices (e.g., Mottronics). Although a significant understanding of doping‐tuned transport properties of single crystalline correlated materials exists, it has remained unclear how doping‐controlled transport properties behave in the presence of planar defects. The discovery of an unexpected high‐concentration doping effect in defective regions is reported for correlated nickelates. It enables electronic conductance by tuning the Fermi‐level in Mott–Hubbard band and shaping the lower Hubbard band state into a partially filled configuration. Interface engineering and grain boundary designs are performed for HxSmNiO3/SrRuO3heterostructures, and a Mottronic device is achieved. The interfacial aggregation of hydrogen is controlled and quantified to establish its correlation with the electrical transport properties. The chemical bonding between the incorporated hydrogen with defective SmNiO3is further analyzed by the positron annihilation spectroscopy. The present work unveils new materials physics in correlated materials and suggests novel doping strategies for developing Mottronic and iontronic devices via hydrogen‐doping‐controlled orbital occupancy in perovskite heterostructures.

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Award ID(s):
1706815
NSF-PAR ID:
10458693
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Materials
Volume:
32
Issue:
6
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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    References

    Lee, D. H.; Park, H.; Clevenger, M.; Kim, H.; Kim, C. S.; Liu, M.; Kim, G.; Song, H. W.; No, K.; Kim, S. Y.; Ko, D.-K.; Lucietto, A.; Park, H.; Lee, S., High-Performance Oxide-Based p–n Heterojunctions Integrating p-SnOx and n-InGaZnO.ACS Applied Materials & Interfaces2021,13(46), 55676-55686.

    Hautier, G.; Miglio, A.; Ceder, G.; Rignanese, G.-M.; Gonze, X., Identification and design principles of low hole effective mass p-type transparent conducting oxides.Nat Commun2013,4.

    Yim, K.; Youn, Y.; Lee, M.; Yoo, D.; Lee, J.; Cho, S. H.; Han, S., Computational discovery of p-type transparent oxide semiconductors using hydrogen descriptor.npj Computational Materials2018,4(1), 17.

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