Sustainability pathways for perovskite photovoltaics.

Solar energy is the fastest-growing source of electricity generation globally. As deployment increases, photovoltaic (PV) panels need to be produced sustainably. Therefore, the resource utilization rate and the rate at which those resources become available in the environment must be in equilibrium while maintaining the well-being of people and nature.

Towards linking lab and field lifetimes of perovskite solar cells.

Metal halide perovskite solar cells (PSCs) represent a promising low-cost thin-film photovoltaic technology, with unprecedented power conversion efficiencies obtained for both single-junction and tandem applications. To push PSCs towards commercialization, it is critical, albeit challenging, to understand device reliability under real-world outdoor conditions where multiple stress factors (for example, light, heat and humidity) coexist, generating complicated degradation behaviours. To quickly guide PSC development, it is necessary to identify accelerated indoor testing protocols that can correlate specific stressors with observed degradation modes in fielded devices.

Origins of Photoluminescence Instabilities at Halide Perovskite/Organic Hole Transport Layer Interfaces.

Metal halide perovskites are promising for optoelectronic device applications; however, their poor stability under solar illumination remains a primary concern. While the intrinsic photostability of isolated neat perovskite samples has been widely discussed, it is important to explore how charge transport layers─employed in most devices─impact photostability. Herein, we study the effect of organic hole transport layers (HTLs) on light-induced halide segregation and photoluminescence (PL) quenching at perovskite/organic HTL interfaces.

Electrochemical Doping of Halide Perovskites by Noble Metal Interstitial Cations.

Metal halide perovskites are an attractive class of semiconductors, but it has proven difficult to control their electronic doping by conventional strategies due to screening and compensation by mobile ions or ionic defects. Noble-metal interstitials represent an under-studied class of extrinsic defects that plausibly influence many perovskite-based devices. In this work, doping of metal halide perovskites is studied by electrochemically formed Au interstitial ions, combining experimental data on devices with a computational analysis of Au interstitial defects based on density functional theory (DFT).

Surface reaction for efficient and stable inverted perovskite solar cells.

Perovskite solar cells (PSCs) with an inverted structure (often referred to as the p-i-n architecture) are attractive for future commercialization owing to their easily scalable fabrication, reliable operation and compatibility with a wide range of perovskite-based tandem device architectures. However, the power conversion efficiency (PCE) of p-i-n PSCs falls behind that of n-i-p (or normal) structure counterparts. This large performance gap could undermine efforts to adopt p-i-n architectures, despite their other advantages.

Complexities of Contact Potential Difference Measurements on Metal Halide Perovskite Surfaces.

Understanding the stability of metal halide perovskite (MHP) surfaces is of considerable interest for the development of devices based on these materials. We present here a vacuum-based study of the surface potential and response to illumination of two different types of perovskite films, methylammonium lead bromide (MAPbBr) and the 2D Ruddlesden-Popper phase butylammonium lead iodide (BAPbI, n = 1), using Kelvin probe-based contact potential difference and surface photovoltage measurements. We show that supraband gap light irradiation can induce the loss of halide species, which adsorb on the Kelvin probe tip, inducing quasi-irreversible changes of the MHP surface and tip work functions.

Ionic-Electronic Ambipolar Transport in Metal Halide Perovskites: Can Electronic Conductivity Limit Ionic Diffusion?

Ambipolar transport describes the nonequilibrium, coupled motion of positively and negatively charged particles to ensure that internal electric fields remain small. It is commonly invoked in the semiconductor community where the motion of excess electrons and holes drift and diffuse together. However, the concept of ambipolar transport is not limited to semiconductor physics.

Mixed-Halide Perovskites with Stabilized Bandgaps.

One merit of organic-inorganic hybrid perovskites is their tunable bandgap by adjusting the halide stoichiometry, an aspect critical to their application in tandem solar cells, wavelength-tunable light emitting diodes (LEDs), and lasers. However, the phase separation of mixed-halide perovskites caused by light or applied bias results in undesirable recombination at iodide-rich domains, meaning open-circuit voltage (V) pinning in solar cells and infrared emission in LEDs. Here, we report an approach to suppress halide redistribution by self-assembled long-chain organic ammonium capping layers at nanometer-sized grain surfaces.

Linking Chemistry at the TiO/CHNHPbI Interface to Current-Voltage Hysteresis.

We demonstrate that reversible chemical reactions occur at TiO/gas and CHNHPbI/gas interfaces on a time scale of seconds to minutes. The chemisorption strongly affects their electronic properties, mainly acting to deplete TiO of free electrons and passivate surface traps on the perovskite. Although the chemistry is not directly probed, we infer that reversible chemistry occurs at the solid-state TiO/CHNHPbI interface.

In Situ Preparation of Metal Halide Perovskite Nanocrystal Thin Films for Improved Light-Emitting Devices.

Hybrid organic-inorganic halide perovskite semiconductors are attractive candidates for optoelectronic applications, such as photovoltaics, light-emitting diodes, and lasers. Perovskite nanocrystals are of particular interest, where electrons and holes can be confined spatially, promoting radiative recombination. However, nanocrystalline films based on traditional colloidal nanocrystal synthesis strategies suffer from the use of long insulating ligands, low colloidal nanocrystal concentration, and significant aggregation during film formation.

Valence and Conduction Band Densities of States of Metal Halide Perovskites: A Combined Experimental-Theoretical Study.

We report valence and conduction band densities of states measured via ultraviolet and inverse photoemission spectroscopies on three metal halide perovskites, specifically methylammonium lead iodide and bromide and cesium lead bromide (MAPbI3, MAPbBr3, CsPbBr3), grown at two different institutions on different substrates. These are compared with theoretical densities of states (DOS) calculated via density functional theory. The qualitative agreement achieved between experiment and theory leads to the identification of valence and conduction band spectral features, and allows a precise determination of the position of the band edges, ionization energy and electron affinity of the materials.

Diode-Pumped Organo-Lead Halide Perovskite Lasing in a Metal-Clad Distributed Feedback Resonator.

Organic-inorganic lead halide perovskite semiconductors have recently reignited the prospect of a tunable, solution-processed diode laser, which has the potential to impact a wide range of optoelectronic applications. Here, we demonstrate a metal-clad, second-order distributed feedback methylammonium lead iodide perovskite laser that marks a significant step toward this goal. Optically pumping this device with an InGaN diode laser at low temperature, we achieve lasing above a threshold pump intensity of 5 kW/cm(2) for durations up to ∼25 ns at repetition rates exceeding 2 MHz.

Real-Time Tracking of Singlet Exciton Diffusion in Organic Semiconductors.

Exciton diffusion in organic materials provides the operational basis for functioning of such devices as organic solar cells and light-emitting diodes. Here we track the exciton diffusion process in organic semiconductors in real time with a novel technique based on femtosecond photoinduced absorption spectroscopy. Using vacuum-deposited C_{70} layers as a model system, we demonstrate an extremely high diffusion coefficient of D≈3.