Data from: Dimensionality-controlled confinement effects for tunable optoelectronic properties in quasi-1D hybrid perovskites

Hybrid perovskite dimensional engineering enables the creation of one- to three-dimensional (1D to 3D) networks of corner-sharing metal halide octahedra interspersed by organic cations, offering opportunities to tailor semiconducting properties through quantum- and dielectric-confinement effects. Beyond the discrete options, intermediate dimensionality has been introduced in the form of quasi-2D phases with varying thickness inorganic layers. The current study extends this approach to quasi-1D lead-iodide systems with variable ribbon widths from 2 to 6 octahedra, stabilized by flexible molecular configurations, cation mixing of organic cations, or guest molecule selection. This family of quasi-1D structures adopts unique well-like configurations, with intra-octahedral distortion increasing from the core to the edges. First-principles density-functional theory (DFT) calculations and optical characterizations—i.e., temperature-dependent UV-visible absorption, electro-absorption, photoluminescence, and circular dichroism—collectively demonstrate lower bandgap and exciton binding energy with increased ribbon width due to tailorable quantum confinement and structural distortions. Access to two ribbon widths within a single well-ordered structure yields distinguishable bandgaps and excitonic properties, opening a category of dual-quantum confinement materials in the perovskite family. Our study serves as a starting point, showcasing a paradigm to stabilize increased ribbon widths through further tuning of organic templating effects. This continuum between 2D and 1D structures presents a new approach for fine-tuning the dimensionality and optoelectronic properties of hybrid perovskites.

The dataset provided here is the FHIaims input and output files for all density-functional theory calculations included in this work. This includes five quasi-1D perovskite structures as well as one 2D perovskite structure used as a comparison benchmark within the work itself. The included calculations include band structure calculations demonstrating the regular decrease in band gap correlated to increasing ribbon width as well as geometry optimizations. Further computational details can be found within this dataset.

This work was primarily supported as part of the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) an Energy Frontier Research Center funded by the Office of Basic Energy Sciences, Office of Science within the U.S. Department of Energy. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231 using NERSC awards BES-ERCAP0024246 and BES-ERCAP0029145. The views expressed in the article do not necessarily represent the views of the DOE or the U.S. Government. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this work or allow others to do so, for U.S. Government purposes. KB was supported by the REU Program "Engineering Materials for a Healthy World”, which was funded through the National Science Foundation through EEC-2244546.