arXiv subjects

Muhammad Ejaz Khan

Publications and source records attributed to Muhammad Ejaz Khan.

4 recordsLinked to original sources

arXiv2022

Quantum hybridization negative differential resistance from non-toxic halide perovskite nanowire heterojunctions and its strain control

While low-dimensional organometal halide perovskites are expected to open up new opportunities for a diverse range of device applications, like in their bulk counterparts, the toxicity of Pb-based halide perovskite materials is a significant concern that hinders their practical use. We recently predicted that lead triiodide (PbI$_3$) columns de-rived from trimethylsulfonium (TMS) lead triiodide (CH$_3$)$_3$SPbI$_3$ (TMSPbI$_3$) by stripping off TMS ligands should be semimetallic, and additionally ultrahigh negative differential resistance (NDR) can arise from the heterojunction composed of a TMSPbI$_3$ channel sandwiched by PbI$_3$ electrodes. Herein, we computationally explore whether similar material and device characteristics can be obtained from other one-dimensional halide perovskites based on non-Pb metal elements, and in doing so deepen the understanding of their mechanistic origins. First, scanning through several candidate metal halide inorganic frameworks as well as their parental form halide perovskites, we find that the germanium triiodide (GeI$_3$) column also assumes a semimetallic character by avoiding the Peierls distortion. Next, adopting the bundled nanowire GeI$_3$-TMSGeI$_3$-GeI$_3$ junction configuration, we obtain a drastically high peak current density and ultrahigh NDR at room temperature. Furthermore, the robustness and controllability of NDR signals under strain are revealed, establishing its potential for flexible electronics applications. It will be emphasized that, despite the performance metrics notably enhanced over those from the PbI$_3$-TMSPbI$_3$-PbI$_3$ case, these device characteristics still arise from the identical quantum hybridization NDR mechanism.

cond-mat.mes-hall↗

arXiv2020

Strain-induced metallization and defect suppression at zipper-like interdigitated atomically thin interfaces enabling high-efficiency halide perovskite solar cells

Halide perovskite light absorbers have great advantages for photovoltaics such as efficient solar energy absorption, but charge accumulation and recombination at the interface with an electron transport layer (ETL) remains a major challenge in realizing their full potential. Here we report the experimental realization of a zipper-like interdigitated interface between a Pb-based halide perovskite light absorber and an oxide ETL by the PbO capping of the ETL surface, which produces an atomically thin two-dimensional metallic layer that can significantly enhance the perovskite/ETL charge extraction process. As the atomistic origin of the emergent two-dimensional interfacial metallicity, first-principles calculations performed on the representative MAPbI$_3$/TiO$_2$ interface identify the interfacial strain induced by the simultaneous formation of stretched I-substitutional Pb bonds (and thus Pb-I-Pb bonds bridging MAPbI$_3$ and TiO$_2$) and contracted substitutional Pb-O bonds. Direct and indirect experimental evidences for the presence of interfacial metallic states are provided, and a non-conventional defect-passivating nature of the strained interdigitated perovskite/ETL interface is emphasized. It is experimentally demonstrated that the PbO capping method is generally applicable to other ETL materials including ZnO and SrTiO$_3$, and that the zipper-like interdigitated metallic interface leads to about two-fold increase in charge extraction rate. Finally, in terms of the photovoltaic efficiency, we observe a volcano-type behavior with the highest performance achieved at the monolayer-level PbO capping. The method established here might prove to be a general interface engineering approach to realize high-performance perovskite solar cells.

cond-mat.mtrl-sci↗

arXiv2020

First-principles-derived effective mass approximation for the improved description of quantum nanostructures

The effective mass approximation (EMA) could be an efficient method for the computational study of semiconductor nanostructures with sizes too large to be handled by first-principles calculations, but the scheme to accurately and reliably introduce EMA parameters for given nanostructures remains to be devised. Herein, we report on an EMA approach based on first-principles-derived data, which enables accurate predictions of the optoelectronic properties of quantum nanostructures. For the CdS/ZnS core/shell quantum rods, for which we recently reported its experimental synthesis, we first carry out density functional theory (DFT) calculations for an infinite nanowire to obtain the nanoscopic dielectric constant, effective mass, and Kohn-Sham potential. The DFT-derived data are then transferred to the finite nanorod cases to set up the EMA equations, from which we estimate the photoluminescence (PL) characteristics. Compared with the corresponding method based on bulk EMA parameters and abrupt potential, we confirm that our EMA approach more accurately describes the PL properties of nanorods. We find that, in agreement with the experimentally observed trends, the optical gap of nanorods is roughly determined by the nanorod diameter and the PL intensity is reduced with increasing the nanorod length. The developed methodology is additionally applied to CdSe nanoplatelets, where reliable experimental data became recently available. Here, we again obtain excellent agreements between calculated and measured optical gap values, confirming the generality of our approach. It is finally shown that the abrupt confinement potential approximation most adversely affects the accuracy of EMA simulations.

cond-mat.mes-hall↗

arXiv2018

Semimetallicity and Negative Differential Resistance from Hybrid Halide Perovskite Nanowires

In the rapidly progressing field of organometal halide perovskites, the dimensional reduction could open up new opportunities for device applications. Herein, taking the recently synthesized trimethylsulfonium lead triiodide (CH$_3$)$_3$SPbI$_3$ perovskite as a representative example, we carry out first-principles calculations and study the nanostructuring and device application of halide perovskite nanowires. We find that the one-dimensional (1D) (CH$_3$)$_3$SPbI$_3$ structure is structurally stable, and the electronic structures of higher-dimensional forms are robustly determined at the 1D level. Remarkably, due to the face-sharing [PbI$_6$] octahedral atomic structure, the organic ligand-removed 1D PbI$_3$ frameworks are also found to be stable. Moreover, the PbI$_3$ columns avoid the Peierls distortion and assume a semimetallic character, contradicting the conventional assumption of semiconducting metal-halogen inorganic frameworks. Adopting the bundled nanowire junctions consisting of (CH$_3$)$_3$SPbI$_3$ channels with sub-5 nm dimensions sandwiched between PbI$_3$ electrodes, we finally obtain high current densities and large room-temperature negative differential resistance (NDR). It will be emphasized that the NDR originates from the combination of the near-Ohmic character of (CH$_3$)$_3$SPbI$_3$-PbI$_3$ contacts and a novel NDR mechanism that involves the quantum-mechanical hybridization between channel and electrode states. Our work demonstrates the great potential of low-dimensional hybrid perovskites toward advanced electronic devices beyond actively-pursued photonic applications.

cond-mat.mes-hall↗