Electronic Structure Manipulation of the Mott Insulator RuCl3 via Single‐Crystal to Single‐Crystal Topotactic Transformation. Issue 17 (20th March 2023)

• Record Type: Journal Article
• Authors: Lu, Weiqun; Lee, Hyungseok; Cha, Joonil; Zhang, Jian; Chung, In
• Is Part Of: Angewandte Chemie international edition. Volume 62:Issue 17(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2023-03-20
• Subjects: Charge Carrier Transport -- Electronic Structures -- Intercalation -- Mott Insulators -- RuCl3; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202219344
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: The core task for Mott insulators includes how rigid distributions of electrons evolve and how these induce exotic physical phenomena. However, it is highly challenging to chemically dope Mott insulators to tune properties. Herein, we report how to tailor electronic structures of the honeycomb Mott insulator RuCl3 employing a facile and reversible single‐crystal to single‐crystal intercalation process. The resulting product (NH4 )0.5 RuCl3 ⋅1.5 H2 O forms a new hybrid superlattice of alternating RuCl3 monolayers with NH4 + and H2 O molecules. Its manipulated electronic structure markedly shrinks the Mott–Hubbard gap from 1.2 to 0.7 eV. Its electrical conductivity increases by more than 10 3 folds. This arises from concurrently enhanced carrier concentration and mobility in contrary to the general physics rule of their inverse proportionality. We show topotactic and topochemical intercalation chemistry to control Mott insulators, escalating the prospect of discovering exotic physical phenomena. Abstract : The electronic structures of the honeycomb Mott‐insulator RuCl3 are tailored by employing a facile and reversible single‐crystal to single‐crystal intercalation strategy. The resulting product forms a new hybrid superlattice of alternating RuCl3 monolayers, displaying distinct optical and electronic properties and dramatically boosted charge carrier transport characteristics.