Abstract
The creation of low-dimensional heterostructures for intelligent devices is a challenging research topic; however, macro- and atomic-scale connections in one-dimensional (1D) electronic systems have not been achieved yet. Herein, we synthesize a heterostructure comprising a 1D Mott insulator [Ni(chxn)2Br]Br2 (1; chxn = 1R-2R-diaminocyclohexane) and a 1D Peierls or charge-density-wave insulator [Pd(chxn)2Br]Br2 (2) using stepwise electrochemical growth. It can be considered as the first example of electrochemical liquid-phase epitaxy applied to molecular-based heterostructures with a macroscopic scale. Moreover, atomic-resolution scanning tunneling microscopy images reveal a modulation of the electronic state in the heterojunction region with a length of five metal atoms (~ 2.5 nm), that is a direct evidence for the atomic-scale connection of 1 and 2. This is the first time that the heterojunction in the 1D chains has been shown and examined experimentally at macro- and atomic-scale. This study thus serves as proof of concept for heterojunctions in 1D electronic systems.
Highlights
The creation of low-dimensional heterostructures for intelligent devices is a challenging research topic; macro- and atomic-scale connections in one-dimensional (1D) electronic systems have not been achieved yet
After removing the crystals from the anode, the crystals were cleaved with the utmost care along the bc-plane using a razor blade in order to observe the 1–2 heterojunction
The modulations of the electronic structure and the band bending have been reported to occur at the sub-nanometer to ~2 nm scale at the heterojunction of the graphene nanoribbons[14,15], which is comparable to the modulation distance in this study (~2.5 nm)
Summary
The creation of low-dimensional heterostructures for intelligent devices is a challenging research topic; macro- and atomic-scale connections in one-dimensional (1D) electronic systems have not been achieved yet. Organic–inorganic hybrids and molecule-based heterostructures have attracted great attention[1–9], as their structures and properties can be precisely tuned through crystal and molecular design In these heterostructures, bulk[1–6] or planar heterojunctions[7–9] have been developed to obtain high performance; connection at the atomic scale has remained elusive so far. Have synthesized and examined a heterojunction in a twodimensional (2D) material, using graphene and hexagonal boron–nitride sheets, at the atomic scale using high-resolution transmission electron microscopy[10] This sophisticated study demonstrated that low-dimensional heterostructures are attractive materials that show non-linear properties based on the quantum effect[11–13]. As the unit cell parameters for [Ni(chxn)2Br]Br2 (1) and [Pd(chxn)2Br]Br2 (2) are almost identical (Fig. 1 and Supplementary Table 1)[21,28,29], these compounds can be mixed in any ratio to produce solid solutions Combinations of these MX-Chains represent the most desirable candidate to realize a 1D heterojunction material composed of a Ni Mott insulator and a Pd Peierls insulator. The 1D heterojunction was unequivocally observed using optical and scanning electron microscope energy dispersive X-ray spectroscopy (SEM-EDS) and scanning tunneling microscopy (STM), which is the first time that a macro- and atomic-scale heterojunction in a 1D electron system has been examined experimentally
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