Metal-insulator-semiconductor heterostructures for plasmonic hot-carrier optoelectronics

Plasmonic hot-electron devices are attractive candidates for light-energy harvesting and photodetection applications. For solid state devices, the most compact and straightforward architecture is the metalsemiconductor Schottky junction. However convenient, this structure introduces limitations such as the elevated dark current associated to thermionic emission, or constraints for device design due to the finite choice of materials. In this work we theoretically consider the metalinsulator-semiconductor heterojunction as a candidate for plasmonic hotcarrier photodetection and solar cells. The presence of the insulating layer can significantly reduce the dark current, resulting in increased device performance with predicted solar power conversion efficiencies up to 9%. For photodetection, the sensitivity can be extended well into the infrared by a judicious choice of the insulating layer, with up to 300-fold expected enhancement in detectivity.Peer ReviewedPostprint (published version

Large-Area Plasmonic-Crystal−Hot-Electron-Based Photodetectors

In view of their exciting optoelectronic light− matter interaction properties, plasmonic−hot-electron devices have attracted significant attention during the last few years as a novel route for photodetection and light-energy harvesting. Herein we report the use of quasi-3D large-area plasmonic crystals (PC) for hot-electron photodetection, with a tunable response across the visible and near-infrared. The strong interplay between the different PC modes gives access to intense electric fields and hot-carrier generation confined to the metal− semiconductor interface, maximizing injection efficiencies with responsivities up to 70 mA/W. Our approach, compatible with large-scale manufacturing, paves the way for the practical implementation of plasmonic−hot-electron optoelectronic devices.Peer ReviewedPostprint (published version

Inorganic Tin Perovskites with Tunable Conductivity Enabled by Organic Modifiers

Achieving control over the transport properties of charge-carriers is a crucial aspect of realizing high-performance electronic materials. In metal-halide perovskites, which offer convenient manufacturing traits and tunability for certain optoelectronic applications, this is challenging: The perovskite structure itself, poses fundamental limits to maximum dopant incorporation. Here, we demonstrate an organic modifier incorporation strategy capable of modulating the electronic density of states in halide tin perovskites without altering the perovskite lattice, in a similar fashion to substitutional doping in traditional semiconductors. By incorporating organic small molecules and conjugated polymers into cesium tin iodide (CsSnI3) perovskites, we achieve carrier density tunability over 2.7 decades, transition from a semiconducting to a metallic nature, and high electrical conductivity exceeding 200 S/cm. We leverage these tunable and enhanced electronic properties to achieve a thin-film, lead free, thermoelectric material with a near room-temperature figure-of-merit (ZT) of 0.21, the highest amongst all halide perovskite thermoelectrics. Our strategy provides an additional degree of freedom in the design of halide perovskites for optoelectronic and energy applications

Advances in solution-processed near-infrared light-emitting diodes

Near-infrared light-emitting diodes based on solution-processed semiconductors, such as organics, halide perovskites and colloidal quantum dots, have emerged as a viable technological platform for biomedical applications, night vision, surveillance and optical communications. The recently gained increased understanding of the relationship between materials structure and photophysical properties has enabled the design of efficient emitters leading to devices with external quantum efficiencies exceeding 20%. Despite considerable strides made, challenges remain in achieving high radiance, reducing efficiency roll-off and extending operating lifetime. This Review summarizes recent advances on emissive materials synthetic methods and device key attributes that collectively contribute to improved performance of the fabricated light-emitting devices

Edge stabilization in reduced-dimensional perovskites

Reduced-dimensional perovskites are attractive light-emitting materials due to their efficient luminescence, color purity, tunable bandgap, and structural diversity. A major limitation in perovskite light-emitting diodes is their limited operational stability. Here we demonstrate that rapid photodegradation arises from edge-initiated photooxidation, wherein oxidative attack is powered by photogenerated and electrically-injected carriers that diffuse to the nanoplatelet edges and produce superoxide. We report an edge-stabilization strategy wherein phosphine oxides passivate unsaturated lead sites during perovskite crystallization. With this approach, we synthesize reduced-dimensional perovskites that exhibit 97 ± 3% photoluminescence quantum yields and stabilities that exceed 300 h upon continuous illumination in an air ambient. We achieve green-emitting devices with a peak external quantum efficiency (EQE) of 14% at 1000 cd m-2; their maximum luminance is 4.5 × 104 cd m-2 (corresponding to an EQE of 5%); and, at 4000 cd m-2, they achieve an operational half-lifetime of 3.5 h.This publication is based in part on work supported by an award (KUS-11-009-21) from the King Abdullah University of Science and Technology (KAUST), by the Ontario Research Fund Research Excellence Program, by the Ontario Research Fund (ORF), by the Natural Sciences and Engineering Research Council (NSERC) of Canada, and by the US Department of Navy, Office of Naval Research (Grant Award No. N00014-17-1-2524). H.Y. acknowledges the Research Foundation-Flanders (FWO Vlaanderen) for a postdoctoral fellowship. E.B. gratefully acknowledges financial support by the Research Foundation-Flanders (FWO Vlaanderen). S.B. acknowledges financial support from European Research Council (ERC Starting Grant #815128-REALNANO). M.B.J.R. and J.H. acknowledge the Research Foundation-Flanders (FWO, Grants G.0962.13, G.0B39.15, AKUL/11/14 and G0H6316N), KU Leuven Research Fund (C14/15/053) and the European Research Council under the European Union’s Seventh Framework Programme (FP/2007-2013)/ERC Grant Agreement No. [307523], ERC-Stg LIGHT to M.B.J.R. DFT calculations were performed on the IBM BlueGene Q supercomputer with support from the Southern Ontario Smart Computing Innovation Platform (SOSCIP). M.I.S. acknowledges the Banting Postdoctoral Fellowship program from the Natural Sciences and Engineering Research Council of Canada (NSERC). H.T. acknowledges the Netherlands Organisation for Scientific Research (NWO) for a Rubicon grant (680-50-1511)

Solution-processed semiconductors for next-generation photodetectors

Efficient light detection is central to modern science and technology.Current photodetectors mainly use photodiodes based on crystalline inorganic elementalsemiconductors, such as silicon, or compounds such as III–V semiconductors. Photodetectorsmade of solution-processed semiconductors — which include organic materials, metal-halideperovskites and quantum dots — have recently emerged as candidates for next-generation lightsensing. They combine ease of processing, tailorable optoelectronic properties, facile integrationwith complementary metal–oxide–semiconductors, compatibility with flexible substrates andgood performance. Here, we review the recent advances and the open challenges in the field ofsolution-processed photodetectors, examining the topic from both the materials and the deviceperspective and highlighting the potential of the synergistic combination of materials and deviceengineering. We explore hybrid phototransistorsand their potential to overcome trade-offsin noise, gain and speed, as well as the rapid advances in metal-halide perovskite photodiodesand their recent application in narrowband filterless photodetection