Prof Henry Snaith FRS

Abstract:

We show that the use of 1,3-diaminopropane (DAP) as a chemical modifier at the perovskite/electron-transport layer (ETL) interface enhances the power conversion efficiency (PCE) of 1.7 eV band gap mixed-halide perovskite containing formamidinium and Cs single-junction cells, primarily by increasing the open-circuit voltage (VOC) from 1.06 to 1.15 V. We find that adding a postprocessing annealing step after C60 evaporation further improves device performance. Specifically, the fill factor (FF) increases by 20% in the DAP + postannealing devices compared to the control. Using hyperspectral photoluminescence microscopy, we demonstrate that annealing helps improve compositional homogeneity at the electron-transport layer (ETL) and hole-transport layer (HTL) interfaces of the solar cell, which prevents detrimental band gap pinning in the devices and improves C60 adhesion. Using time-of-flight secondary ion mass spectrometry, we show that DAP reacts with formamidinium (FA+) present at the surface of the perovskite structure to form a larger molecular cation, 1,4,5,6-tetrahydropyrimidinium (THP+), which remains at the interface. Combining the use of DAP and annealing the C60 interface, we fabricate Si-perovskite tandems with a PCE of 25.29%, compared to 23.26% for control devices. Our study underscores the critical role of the chemical reactivity of diamines at the surface and the thermal postprocessing of the C60/Lewis-base passivator interface in minimizing device losses and enhancing solar-cell performance of wide-band-gap mixed-cation mixed-halide perovskites for tandem applications.

Abstract:

Thanks to their superior bandgap tunability and high absorption coefficient, metal halide perovskites demonstrate high potential for fabricating multijunction photovoltaics capable of achieving power conversion efficiencies surpassing the radiative efficiency limit of single-junction solar cells[1],[2]. One of the key challenges currently facing all-perovskite multijunction photovoltaics is the low quality of the narrow bandgap (~1.25 eV) mixed tin-lead perovskite films used as the rear absorber. At this conference, we will present our recent investigations on the mixed tin−lead perovskites covering the control of the Sn(II) oxidation[3], interface carrier extraction[4], and in-situ surface reaction[5], as well as the understanding of the solution chemistry and resultant crystallization[6], aiming to generate a global picture toward the comprehensive understanding of this material and its photovoltaic devices. As a result, we have obtained efficiencies of over 23.9% for the single-junction tin−lead perovskite devices, with an open circuit voltage of up to 0.91 V. Building on optimizations of neat lead perovskites, we then showcase the successful integration of these improved mixed tin-lead perovskites into double-, triple-, and quadruple-junction tandem solar cells, achieving efficiencies exceeding 29%, 28%, and 27%, respectively. In addition, we will propose promising strategies for enhancing the light and temperature stability of the involved perovskite subcells, aiming to improve the reliability of efficient all-perovskite multijunction photovoltaics. Furthermore, we will also share insights and recent progress achieved in perovskite-on-silicon multijunction cells.

Abstract:

Photovoltaic cells are generally optimised for operation at 25 °C under the AM1.5 solar spectrum. This is useful for comparing different technologies, but ultimately energy yield (the energy output across a year of operation) is what we aim to maximise. This is generally estimated using the power conversion efficiency (PCE) of a cell at 25 °C and its temperature coefficient (how PCE changes with temperature). For monolithic tandem cells, this method is less accurate as current matching between each sub cell is required for maximum performance. To understand how to optimise tandems for energy yield, we fabricated perovskite/Si (30.8% PCE) and all-perovskite (25.4% PCE) tandems and tested them over a range of temperatures. Opposing temperature dependence with bandgap - perovskite bandgaps tend to widen with increasing temperature, whereas Si narrows - results in a worse temperature coefficient for perovskite/Si (-0.23%/°C) compared to all-perovskite tandems (-0.17%/°C). Increasing the Cs concentration at the perovskite A-site reduces the bandgap widening effect, resulting in an improved temperature coefficient (-0.19%/°C). Surprisingly, when estimating energy yields using real-world data, this improved temperature coefficient does not translate to increased yields. Instead, we find that the opposing temperature/bandgap correlation of perovskite/Si tandems is an advantage as the solar spectrum is blue-shifted compared to AM1.5 when cells are warmest and operate at their peak power output. Thus, we expect an increase in energy yield of up to 3% for optimised perovskite/Si tandems compared to other tandem technologies with the same PCE. Significantly, this equates to a full PCE point increase under standard conditions for optimised (> 30%) perovskite/Si tandems.

Abstract:

Despite significant advances in wide band gap perovskite solar cells over the past several years, non-radiative recombination at the perovskite-electron transport interface continues to be a critical obstacle limiting device performance. This study presents a solution utilizing a thin interlayer of blended fullerenes [6], [6]-phenyl C61 butyric acid methyl ester (PCBM) and indene-C60 bis-adduct (ICBA) between the 1.77 eV perovskite and evaporated C60. Optimizing the blend to a trace 2% by mass PCBM in ICBA results in a hybrid electron transport layer (ETL) with improved energetic alignment, stronger molecular ordering, an order of magnitude higher electron mobility compared to neat PCBM or ICBA. When combined with surface passivation, this approach resulted in devices with 19.5% steady state efficiency, a fill factor of 0.85 and open-circuit voltage (VOC) of 1.33 V, which is within 10% of the radiative limit of VOC for this bandgap. Here we highlight the complex nonlinear behavior with fullerene mixing, and how controlling the energetics and crystallinity as well as the electronic properties of these materials is vital in mitigating nonradiative recombination and achieving high performing wide band gap perovskite solar cells.