Polaron Self-localization in White-light Emitting Hybrid Perovskites

Two-dimensional (2D) perovskites with general formula $APbX_4$ are attracting increasing interest as solution processable, white-light emissive materials. Recent studies have shown that their broadband emission is related to the formation of intra-gap color centers; however, the nature and dynamics of the emissive species have remained elusive. Here we show that the broadband photoluminescence of the 2D perovskites $(EDBE)PbCl_4$ and $(EDBE)PbBr_4$ stems from the localization of small polarons within the lattice distortion field. Using a combination of spectroscopic techniques and first-principles calculations, we infer the formation of ${Pb_2}^{3+}$, $Pb^{3+}$, and ${X_2}^-$ (where X=Cl or Br) species confined within the inorganic perovskite framework. Due to strong Coulombic interactions, these species retain their original excitonic character and form self-trapped polaron-excitons acting as radiative color centers. These findings are expected to be applicable to a broad class of white-light emitting perovskites with large polaron relaxation energy.Comment: 34 pages, 15 figures, 3 table

Computational Study of Halide Perovskite-Derived A2_2BX6_6 Inorganic Compounds: Chemical Trends in Electronic Structure and Structural Stability

The electronic structure and energetic stability of A$_2$BX$_6$ halide compounds with the cubic and tetragonal variants of the perovskite-derived K$_2$PtCl$_6$ prototype structure are investigated computationally within the frameworks of density-functional-theory (DFT) and hybrid (HSE06) functionals. The HSE06 calculations are undertaken for seven known A$_2$BX$_6$ compounds with A = K, Rb and Cs, and B = Sn, Pd, Pt, Te, and X = I. Trends in band gaps and energetic stability are identified, which are explored further employing DFT calculations over a larger range of chemistries, characterized by A = K, Rb, Cs, B = Si, Ge, Sn, Pb, Ni, Pd, Pt, Se and Te and X = Cl, Br, I. For the systems investigated in this work, the band gap increases from iodide to bromide to chloride. Further, variations in the A site cation influences the band gap as well as the preferred degree of tetragonal distortion. Smaller A site cations such as K and Rb favor tetragonal structural distortions, resulting in a slightly larger band gap. For variations in the B site in the (Ni, Pd, Pt) group and the (Se, Te) group, the band gap increases with increasing cation size. However, no observed chemical trend with respect to cation size for band gap was found for the (Si, Sn, Ge, Pb) group. The findings in this work provide guidelines for the design of halide A$_2$BX$_6$ compounds for potential photovoltaic applications

Vacuum-processed metal halide perovskite light-emitting diodes: prospects and challenges

In less than a decade, organic-inorganic metal halide perovskites (MHPs) have shown tremendous progress in the field of light-emitting applications. Perovskite light-emitting diodes (PeLEDs) have reached external quantum efficiencies (EQE) exceeding 20 % and they have been recognized as a potential contender of the commercial display technologies. However, perovskite thin films in PeLEDs are generally deposited via a spin-coating process, which is not favourable for large area device fabrication. Despite the great success of solution-processed PeLEDs, very few articles have been reported on vacuum processed PeLEDs and the improvements in their optoelctronic performances are also progressing slowly. On the other hand, vacuum processing techniques are mostly used in organic LED technology as they can guarantee (i) the absence of solvent during thin-film growth, (ii) process scalability over large area substrates, and (iii) precise thin-film thickness control. This thin-film growth process is suitable for application in the advancement of a large variety of display technologies. In this Review, we present an overview of current research advances in the field of perovskite thin films grown via vacuum techniques, a study of their photophysical properties, and integration in PeLEDs for the generation of different colors. We also highlight the current challenges and future prospects for the further development of vacuum processed PeLEDs

Transparent, conducting Nb:SnO2 for host-guest photoelectrochemistry

Many candidate materials for photoelectrochemical water splitting will be better employed by decoupling optical absorption from carrier transport. A promising strategy is to use multiple thin absorber layers supported on transparent, conducting materials; however there are limited such materials that are both pH stable and depositable on arbitrary high surface area substrates. Here we present the first 3D porous niobium doped tin oxide (NTO) electrodes fabricated by atomic layer deposition. After high temperature crystallization the NTO is transparent, conductive, and stable over a wide range of pH. The optimized films have high electrical conductivity up to 37 S/cm concomitant with a low optical attenuation coefficient of 0.99 mu m(-1) at 550 nm. NTO was deposited onto high surface area templates that were subsequently coated with hematite Fe2O3 for the photoelectrochemical water splitting. This approach enabled near-record water splitting photocurrents for hematite electrodes employing a host-guest strategy

Tunable electroluminescence for pure white emission from a perovskite-based LED

Raw data for project titled &quot;Tunable electroluminescence for pure white emission from a perovskite-based LED&quot;</span

New donor-pi-acceptor sensitizers containing 5H-[1,2,5]thiadiazolo [3,4-f]isoindole-5,7(6H)-dione and 6H-pyrrolo[3,4-g]quinoxaline-6,8(7H)-dione units

Two new D-pi-A sensitizers (L101 and L102) incorporating 5H-[1,2,5]thiadiazolo [3,4-f] isoindole-5,7(6H)-dione and 6H-pyrrolo[3,4-g]quinoxaline-6,8(7H)-dione core structures were synthesized and tested in liquid dye-sensitized solar cells (DSCs). L102 achieved a promising power conversion efficiency (PCE) of 6.2% (AM 1.5, 100 mW cm(-2))

Pentacene organic field effect transistors on flexible substrates with polymer dielectrics

Pentacene Organic Field Effect Transistors are fabricated using polymethyl methacrylate (PMMA) as a gate dielectric on flexible polymeric substrates like the Indium tin oxide coated polyethylene terephthalate (ITO coated PET), and polyethylene napthalate (PEN) in top contact configuration. The ITO and aluminium (evaporated on PEN) act as the gate materials for the OFETs. The devices on ITO coated PET show electron mobility up to 0.07 cm/V-s and the on/off ratios in the order of 10