Electronic Structure Manipulation of the Mott Insulator RuCl3via Single‐Crystal to Single‐Crystal Topotactic Transformation

Author:

Lu Weiqun1ORCID,Lee Hyungseok12ORCID,Cha Joonil12,Zhang Jian13ORCID,Chung In12ORCID

Affiliation:

1. School of Chemical and Biological Engineering and Institute of Chemical Processes Seoul National University Seoul 08826 Republic of Korea

2. Center for Correlated Electron Systems Institute for Basic Science (IBS) Seoul 08826 Republic of Korea

3. Key Lab of Photovoltaic and Energy Conservation Materials Institute of Solid State Physics HFIPS Chinese Academy of Sciences Hefei 230031 China

Abstract

AbstractThe 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 RuCl3employing a facile and reversible single‐crystal to single‐crystal intercalation process. The resulting product (NH4)0.5RuCl3⋅1.5 H2O forms a new hybrid superlattice of alternating RuCl3monolayers with NH4+and H2O 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 103folds. 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.

Funder

National Research Foundation of Korea

Institute for Basic Science

Publisher

Wiley

Subject

General Medicine

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