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Many different photovoltaic technologies are being developed for large-scale solar energy conversion. The wafer-based first-generation photovoltaic devices have been followed by thin-film solid semiconductor absorber layers sandwiched between two charge-selective contacts and nanostructured (or mesostructured) solar cells that rely on a distributed heterojunction to generate charge and to transport positive and negative charges in spatially separated phases. Although many materials have been used in nanostructured devices, the goal of attaining high-efficiency thin-film solar cells in such a way has yet to be achieved. Organometal halide perovskites have recently emerged as a promising material for high-efficiency nanostructured devices. Here we show that nanostructuring is not necessary to achieve high efficiencies with this material: a simple planar heterojunction solar cell incorporating vapour-deposited perovskite as the absorbing layer can have solar-to-electrical power conversion efficiencies of over 15 per cent (as measured under simulated full sunlight). This demonstrates that perovskite absorbers can function at the highest efficiencies in simplified device architectures, without the need for complex nanostructures. [ABSTRACT FROM AUTHOR]

The article discusses a study which examines the flexible platform of perovskite semiconductors for wavelength-selective sensing and colour imaging. Topics include the production of colour imaging arrays, the comparison between photodiodes and solar cells, and control of switch off and onset wavelengths of photodiodes.

The efficiency and longevity of metal-halide perovskite solar cells are typically dictated by nonradiative defect-mediated charge recombination. In this work, we demonstrate a vapor-based amino-silane passivation that reduces photovoltage deficits to around 100 millivolts (>90% of the thermodynamic limit) in perovskite solar cells of bandgaps between 1.6 and 1.8 electron volts, which is crucial for tandem applications. A primary-, secondary-, or tertiary-amino–silane alone negatively or barely affected perovskite crystallinity and charge transport, but amino-silanes that incorporate primary and secondary amines yield up to a 60-fold increase in photoluminescence quantum yield and preserve long-range conduction. Amino-silane–treated devices retained 95% power conversion efficiency for more than 1500 hours under full-spectrum sunlight at 85°C and open-circuit conditions in ambient air with a relative humidity of 50 to 60%. [ABSTRACT FROM AUTHOR]

Owing to the bandgap‐bowing effect, mixed lead‐tin halide perovskites provide ideal bandgaps for the bottom subcell of all‐perovskite tandem photovoltaic devices that offer fundamentally elevated power‐conversion efficiencies. However, these materials suffer from degradation in ambient air, which worsens their optoelectronic properties and hinders their usability for photovoltaic applications. Such degradation pathways are not yet fully understood, especially for the perovskites in the middle of the APbxSn1‐xI3 solid solution line, which offer the narrowest bandgaps across the range. This study unravels the degradation mechanisms of APbxSn1‐xI3 perovskites, reporting clear differences between mixed lead‐tin (x = 0.5) and tin‐only (x = 0) perovskites. The dynamic optoelectronic properties, electronic structure, crystal structure, and decomposition products of the perovskite thin films are examined in situ during air exposure. Both perovskite compositions suffer from the formation of defects over the timescale of hours, as indicated by a significant reduction in their charge‐carrier diffusion lengths. For tin‐only perovskite, degradation predominantly causes the formation of energetically shallow tin vacancies and hole doping. However, for mixed lead‐tin perovskite, deep trap states are formed that significantly accelerate charge‐carrier recombination, yet leave mobilities relatively unaffected. These findings highlight the need for passivation strategies tailored specifically to mixed lead‐tin iodide perovskites. [ABSTRACT FROM AUTHOR]

Mixed lead‐tin (Pb:Sn) halide perovskites are promising absorbers with narrow‐bandgaps (1.25–1.4 eV) suitable for high‐efficiency all‐perovskite tandem solar cells. However, solution processing of optimally thick Pb:Sn perovskite films is notoriously difficult in comparison with their neat‐Pb counterparts. This is partly due to the rapid crystallization of Sn‐based perovskites, resulting in films that have a high degree of roughness. Rougher films are harder to coat conformally with subsequent layers using solution‐based processing techniques leading to contact between the absorber and the top metal electrode in completed devices, resulting in a loss of VOC, fill factor, efficiency, and stability. Herein, this study employs a non‐continuous layer of alumina nanoparticles distributed on the surface of rough Pb:Sn perovskite films. Using this approach, the conformality of the subsequent electron‐transport layer, which is only tens of nanometres in thickness is improved. The overall maximum‐power‐point‐tracked efficiency improves by 65% and the steady‐state VOC improves by 28%. Application of the alumina nanoparticles as an interfacial buffer layer also results in highly reproducible Pb:Sn solar cell devices while simultaneously improving device stability at 65 °C under full spectrum simulated solar irradiance. Aged devices show a six‐fold improvement in stability over pristine Pb:Sn devices, increasing their lifetime to 120 h. [ABSTRACT FROM AUTHOR]

Mixed‐halide perovskites offer ideal bandgaps for tandem solar cells, but photoinduced halide segregation compromises photovoltaic device performance. This study explores the influence of a hole‐transport layer, necessary for a full device, by monitoring halide segregation through in situ, concurrent X‐ray diffraction and photoluminescence measurements to disentangle compositional and optoelectronic changes. This work demonstrates that top coating FA0.83Cs0.17Pb(Br0.4I0.6)3 perovskite films with a poly(triaryl)amine (PTAA) hole‐extraction layer surprisingly leads to suppression of halide segregation because photogenerated charge carriers are rapidly trapped at interfacial defects that do not drive halide segregation. However, the generation of iodide‐enriched regions near the perovskite/PTAA interface enhances hole back‐transfer from the PTAA layer through improved energy level offsets, increasing radiative recombination losses. It is further found that while passivation with a piperidinium salt slows halide segregation in perovskite films, the addition of a PTAA top‐coating accelerates such effects, elucidating the specific nature of trap types that are able to drive the halide segregation process. This work highlights the importance of selective passivation techniques for achieving efficient and stable wide‐bandgap perovskite photovoltaic devices. [ABSTRACT FROM AUTHOR]

Mixed tin‐lead halide perovskites are promising low‐bandgap absorbers for all‐perovskite tandem solar cells that offer higher efficiencies than single‐junction devices. A significant barrier to higher performance and stability is the ready oxidation of tin, commonly mitigated by various additives whose impact is still poorly understood for mixed tin‐lead perovskites. Here, the effects of the commonly used SnF2 additive are revealed for FA0.83Cs0.17SnxPb1−xI3 perovskites across the full compositional lead‐tin range and SnF2 percentages of 0.1–20% of precursor tin content. SnF2 addition causes a significant reduction in the background hole density associated with tin vacancies, yielding longer photoluminescence lifetimes, decreased energetic disorder, reduced Burstein–Moss shifts, and higher charge‐carrier mobilities. Such effects are optimized for SnF2 addition of 1%, while for 5% SnF2 and above, additional nonradiative recombination pathways begin to appear. It is further found that the addition of SnF2 reduces a tetragonal distortion in the perovskite structure deriving from the presence of tin vacancies that cause strain, particularly for high tin content. The optical phonon response associated with inorganic lattice vibrations is further explored, exhibiting a shift to higher frequency and significant broadening with increasing tin fraction, in accordance with lower effective atomic metal masses and shorter phonon lifetimes. [ABSTRACT FROM AUTHOR]

Trap‐related charge‐carrier recombination fundamentally limits the performance of perovskite solar cells and other optoelectronic devices. While improved fabrication and passivation techniques have reduced trap densities, the properties of trap states and their impact on the charge‐carrier dynamics in metal‐halide perovskites are still under debate. Here, a unified model is presented of the radiative and nonradiative recombination channels in a mixed formamidinium‐cesium lead iodide perovskite, including charge‐carrier trapping, de‐trapping and accumulation, as well as higher‐order recombination mechanisms. A fast initial photoluminescence (PL) decay component observed after pulsed photogeneration is demonstrated to result from rapid localization of free charge carriers in unoccupied trap states, which may be followed by de‐trapping, or nonradiative recombination with free carriers of opposite charge. Such initial decay components are shown to be highly sensitive to remnant charge carriers that accumulate in traps under pulsed‐laser excitation, with partial trap occupation masking the trap density actually present in the material. Finally, such modelling reveals a change in trap density at the phase transition, and disentangles the radiative and nonradiative charge recombination channels present in FA0.95Cs0.05PbI3, accurately predicting the experimentally recorded PL efficiencies between 50 and 295 K, and demonstrating that bimolecular recombination is a fully radiative process. [ABSTRACT FROM AUTHOR]

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 FROM AUTHOR]

Mixed‐halide perovskites are essential for use in all‐perovskite or perovskite–silicon tandem solar cells due to their tunable bandgap. However, trap states and halide segregation currently present the two main challenges for efficient mixed‐halide perovskite technologies. Here photoluminescence techniques are used to study trap states and halide segregation in full mixed‐halide perovskite photovoltaic devices. This work identifies three distinct defect species in the perovskite material: a charged, mobile defect that traps charge‐carriers in the perovskite, a charge‐neutral defect that induces halide segregation, and a charged, mobile defect that screens the perovskite from external electric fields. These three defects are proposed to be MA+ interstitials, crystal distortions, and halide vacancies and/or interstitials, respectively. Finally, external quantum efficiency measurements show that photoexcited charge‐carriers can be extracted from the iodide‐rich low‐bandgap regions of the phase‐segregated perovskite formed under illumination, suggesting the existence of charge‐carrier percolation pathways through grain boundaries where phase‐segregation may occur. [ABSTRACT FROM AUTHOR]

Traps limit the photovoltaic efficiency and affect the charge transport of optoelectronic devices based on hybrid lead halide perovskites. Understanding the nature and energy scale of these trap states is therefore crucial for the development and optimization of solar cell and laser technology based on these materials. Here, the low-temperature photoluminescence of formamidinium lead triiodide (HC(NH2)2PbI3) is investigated. A power-law time dependence in the emission intensity and an additional low-energy emission peak that exhibits an anomalous relative Stokes shift are observed. Using a rate-equation model and a Monte Carlo simulation, it is revealed that both phenomena arise from an exponential trap-density tail with characteristic energy scale of ≈3 meV. Charge-carrier recombination from sites deep within the tail is found to cause emission with energy downshifted by up to several tens of meV. Hence, such phenomena may in part be responsible for open-circuit voltage losses commonly observed in these materials. In this high-quality hybrid perovskite, trap states thus predominantly comprise a continuum of energetic levels (associated with disorder) rather than discrete trap energy levels (associated, e.g., with elemental vacancies). Hybrid perovskites may therefore be viewed as classic semiconductors whose band-structure picture is moderated by a modest degree of energetic disorder. [ABSTRACT FROM AUTHOR]

Hybrid metal-halide perovskites are promising new materials for use in solar cells; however, their chemical stability in the presence of moisture remains a significant drawback. Quasi two-dimensional (2D) perovskites that incorporate hydrophobic organic interlayers offer improved resistance to degradation by moisture, currently still at the cost of overall cell efficiency. To elucidate the factors affecting the optoelectronic properties of these materials, we have investigated the charge transport properties and crystallographic orientation of mixed methylammonium (MA)-phenylethylammonium (PEA) lead iodide thin films as a function of the MA-to-PEA ratio and, thus, the thickness of the "encapsulated" MA lead-halide layers. We find that monomolecular charge-carrier recombination rates first decrease with increasing PEA fraction, most likely as a result of trap passivation, but then increase significantly as excitonic effects begin to dominate for thin confined layers. Bimolecular and Auger recombination rate constants are found to be sensitive to changes in electronic confinement, which alters the density of states for electronic transitions. We demonstrate that effective charge-carrier mobilities remain remarkably high (near 10 cm²V−1s−1) for intermediate PEA content and are enhanced for preferential orientation of the conducting lead iodide layers along the probing electric field. The trade-off between trap reduction, electronic confinement, and layer orientation leads to calculated charge-carrier diffusion lengths reaching a maximum of 2.5 μm for intermediate PEA content (50%). [ABSTRACT FROM AUTHOR]

Highest reported efficiency cesium lead halide perovskite solar cells are realized by tuning the bandgap and stabilizing the black perovskite phase at lower temperatures. CsPbI2Br is employed in a planar architecture device resulting in 9.8% power conversion efficiency and over 5% stabilized power output. Offering substantially enhanced thermal stability over their organic based counterparts, these results show that all‐inorganic perovskites can represent a promising next step for photovoltaic materials. [ABSTRACT FROM AUTHOR]

Organic-inorganic metal halide perovskite solar cells have emerged in the past few years to promise highly efficient photovoltaic devices at low costs. Here, temperature-sensitive core-shell Ag@TiO2 nanoparticles are successfully incorporated into perovskite solar cells through a low-temperature processing route, boosting the measured device efficiencies up to 16.3%. Experimental evidence is shown and a theoretical model is developed which predicts that the presence of highly polarizable nanoparticles enhances the radiative decay of excitons and increases the reabsorption of emitted radiation, representing a novel photon recycling scheme. The work elucidates the complicated subtle interactions between light and matter in plasmonic photovoltaic composites. Photonic and plasmonic schemes such as this may help to move highly efficient perovskite solar cells closer to the theoretical limiting efficiencies. [ABSTRACT FROM AUTHOR]

The performance of perovskite solar cells has been progressing over the past few years and efficiency is likely to continue to increase. However, a negative aspect for the integration of perovskite solar cells in the built environment is that the color gamut available in these materials is very limited and does not cover the green-to-blue region of the visible spectrum, which has been a big selling point for organic photovoltaics. Here, we integrate a porous photonic crystal (PC) scaffold within the photoactive layer of an opaque perovskite solar cell following a bottom-up approach employing inexpensive and scalable liquid processing techniques. The photovoltaic devices presented herein show high efficiency with tunable color across the visible spectrum. This now imbues the perovskite solar cells with highly desirable properties for cladding in the built environment and encourages design of sustainable colorful buildings and iridescent electric vehicles as future power generation sources. [ABSTRACT FROM AUTHOR]

Halide perovskites are currently one of the most heavily researched emerging photovoltaic materials. Despite achieving remarkable power conversion efficiencies, perovskite solar cells have not yet achieved their full potential, with the interfaces between the perovskite and the charge‐selective layers being where most recombination losses occur. In this study, a fluorinated ionic liquid (IL) is employed to modify the perovskite/SnO2 interface. Using Kelvin probe and photoelectron spectroscopy measurements, it is shown that depositing the perovskite onto an IL‐treated substrate results in the crystallization of a perovskite film which has a more n‐type character, evidenced by a decrease of the work function and a shift of the Fermi level toward the conduction band. Photoluminescence spectroscopy and time‐resolved microwave conductivity are used to investigate the optoelectronic properties of the perovskite grown on neat and IL‐modified surfaces and it is found that the modified substrate yields a perovskite film which exhibits an order of magnitude lower trap density than the control. When incorporated into solar cells, this interface modification results in a reduction in the current–voltage hysteresis and an improvement in device performance, with the best performing devices achieving steady‐state PCEs exceeding 20%. [ABSTRACT FROM AUTHOR]