Ionic 2D Materials for Designable Organic-Inorganic Interfaces
Abstract
Two-dimensional (2D) materials with ionic layered structures represent an emerging class of highly tunable systems that bridge conventional van der Waals materials with hybrid organic–inorganic metal halides. In this dissertation, design principles inspired by amphiphilic molecular organization. analogous to biological membranes. are applied to construct crystalline ionic 2D materials comprising functionalized organic ammonium cations and diverse metal halide anions. These materials form neutral trilayer architectures with well-defined van der Waals galleries, enabling their exfoliation into few-layer or monolayer sheets.
Building on earlier studies of chiral and luminescent hybrid metal halides, this work systematically investigates the synthesis, structural chemistry, and optoelectronic behavior of newly developed ionic 2D systems. Mild solution-based synthetic routes were established using tailored amines and metal halides, allowing precise control over supramolecular interactions and crystal formation. By varying the organic cations and metal halide motifs, the resulting structures exhibit tunable band gaps, adjustable dipole moments, and, in specific cases, chiroptical activity.
Particular attention is devoted to photophysical processes arising from reduced structural dimensionality. Several synthesized compounds display broadband white-light emission dominated by self-trapped excitons (STEs), reflecting strong electron–phonon coupling and lattice softness characteristic of low-dimensional halides. Exfoliated few-layer sheets further reveal thickness-dependent quantum confinement, confirming the feasibility of tuning optical responses via dimensional control.
This work demonstrates that ionic 2D materials offer a versatile design platform for tailoring organic–inorganic interfaces at the molecular level. Their modularity enables the integration of programmable structural, electronic, and optical properties, opening pathways toward multifunctional layered heterostructures and future optoelectronic, chiral, or ferroelectric devices.
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