Bernard Wenger

Abstract:

We present a crystallographic and optoelectronic study of the double perovskite Cs2AgBi1–xInxBr6. From structural characterization we determine that the indium cation shrinks the lattice and shifts the cubic-to-tetragonal phase transition point to lower temperatures. The absorption onset is shifted to shorter wavelengths upon increasing the indium content, leading to wider band gaps, which we rationalize through first-principles band structure calculations. Despite the unfavorable band gap shift, we observe an enhancement in the steady-state photoluminescence intensity, and n-i-p photovoltaic devices present short-circuit current greater than that of neat Cs2AgBiBr6 devices. In order to evaluate the prospects of this material as a solar absorber, we combine accurate absorption measurements with thermodynamic modeling and identify the fundamental limitations of this system. Provided radiative efficiency can be increased and the choice of charge extraction layers are specifically improved, this material could prove to be a useful wide band gap solar absorber.

Abstract:

We present the synthesis of formamidinium lead tribromide (FAPbBr3) perovskite nanocrystals through a phosphine oxide route, where in comparison to more traditional syntheses oleylamine is replaced with trioctylphosphine oxide (TOPO). This route has previously been shown to be successful for the inorganic cesium lead tribromide perovskite nanocrystals. We examine the interactions between the precursors via nuclear magnetic resonance spectroscopy (NMR). We confirm the existence of an interaction between FA-oleate and TOPO and use this to guide the optimization of our synthesis. When the reaction is conducted at room temperature, we observe the formation of nanoparticles with high photoluminescence quantum yield (PLQY, ∼70%) at 2.39 eV (518 nm) with little ripening or size defocusing over time. Although we obtain narrow emission peaks, the crystals are irregular in shape—a testament to the impact of the FA-oleate:TOPO interaction. Despite a drop in PLQY in the washed solutions, films made maintain a high PLQY of ∼50% at 2.33 eV (532 nm), which is fortuitously the ideal wavelength for the green emission channel in displays, and we demonstrate 532 nm electroluminescence in light-emitting diodes with an EQE of 3.7%.

Abstract:

Longevity has been a long-standing concern for hybrid perovskite photovoltaics. We demonstrate high-resilience positive-intrinsic-negative perovskite solar cells by incorporating a piperidiniumbased ionic-compound into the formamidinium-cesium lead-trihalide perovskite absorber. With the band gap tuned to be well suited for perovskite-on-silicon tandem cells, this piperidinium additive enhances the open-circuit voltage and cell efficiency. This additive also retards compositional segregation into impurity phases and pinhole formation in the perovskite absorber layer during aggressive aging. Under full-spectrum simulated sunlight in ambient atmosphere, our Confidential unencapsulated and encapsulated cells retain 80% and 95% of their peak and “post-burn-in” efficiencies for 1010 and 1200 hours at 60 and 85 degree Celsius, respectively. Our analysis reveals detailed degradation routes that contribute to the failure of aged cells.

Abstract:

Longevity has been a long-standing concern for hybrid perovskite photovoltaics. We demonstrate high-resilience positive-intrinsic-negative perovskite solar cells by incorporating a piperidinium-based ionic compound into the formamidinium-cesium lead-trihalide perovskite absorber. With the bandgap tuned to be well suited for perovskite-on-silicon tandem cells, this piperidinium additive enhances the open-circuit voltage and cell efficiency. This additive also retards compositional segregation into impurity phases and pinhole formation in the perovskite absorber layer during aggressive aging. Under full-spectrum simulated sunlight in ambient atmosphere, our unencapsulated and encapsulated cells retain 80 and 95% of their peak and post-burn-in efficiencies for 1010 and 1200 hours at 60° and 85°C, respectively. Our analysis reveals detailed degradation routes that contribute to the failure of aged cells.

Abstract:

Light-emitting diodes (LEDs) made from metal halide perovskites have demonstrated external electroluminescent quantum efficiencies (EQEEL) in excess of 20%. However, their poor operational stability, resulting in lifetimes of only tens to hundreds of hours, needs to be dramatically improved prior to commercial use. There is little consensus in the community upon which factors limit the stability of these devices. Here, we investigate the role played by ammonium cations on the operational stability. We vary the amount of phenylethylammonium bromide, a widely used alkylammonium salt, that we add to a precursor solution of CsPbBr3 and track changes in stability and EQEEL. We find that while phenylethylammonium bromide is beneficial in achieving high efficiency, it is highly detrimental to operational stability. We investigate material properties and electronic characteristics before and after degradation and find that both a reduction in the radiative efficiency of the emitter and significant changes in current–voltage characteristics explain the orders of magnitude drop in the EQEEL, which we attribute to increased ionic mobility. Our results suggest that engineering new contacts and further investigation into materials with lower ionic mobility should yield much improved stability of perovskite LEDs.