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Halide perovskites with bandgaps of 1.70–1.85 eV are of interest for multijunction photovoltaics. Mixing halides on the X site of the ABX3-structured perovskite system is a common way to reach thes...

The effect of carrier-carrier and carrier-phonon interactions are presented in n = 1 (2D) (BA)2PbI4 Ruddlesden-Popper thin films and their effect compared to that of conventional MAPbI3. While temp...

Cesium-containing all-inorganic perovskites have received considerable interest in photovoltaics research because of their potential for improved stability compared to their organic–inorganic hybri...

Two different single junction mixed organic-inorganic halide perovskite solar cells (PSCs) were assessed for their tolerance to high energy proton radiation. Both the narrow band gap mixed tin-lead iodide and wide band gap lead iodide-bromide show remarkable tolerance for fluences up to 1x1011 p/cm2. Both materials show a retention of open circuit voltage and decrease in dark current densities indicating minimal effect on SRH recombination that typically plagues traditional III-V based solar cells. Additionally, a control device that was processed without the perovskite absorber layer showed better diode characteristics and lower dark current densities after proton irradiation. The tolerance of these perovskite as a class of materials is promising for multijunction tandem flexible photovoltaic devices.

Summary Multijunction all-perovskite solar cells offer a route toward efficiencies of III-V materials at low cost by combining the advantages of low thermalization loss in multijunction architectures with the beneficial properties of perovskites—namely, low processing cost, high-throughput fabrication, and compatibility with flexible substrates. However, there are two main challenges for enabling high-efficiency tandems: (1) design of a recombination layer to efficiently combine two perovskite subcells while also preventing bottom cell damage during top cell processing and (2) achieving high open-circuit voltage of the wide-gap subcell. Herein, we overcome both of these challenges. First, we demonstrate a nucleation layer consisting of an ultra-thin polymer with nucleophilic hydroxyl and amine functional groups for nucleating a conformal, low-conductivity aluminum zinc oxide layer by atomic layer deposition (ALD). This method enables ALD-grown recombination layers that reduce shunting as well as solvent degradation from solution processing on top of existing perovskite active layers. Next, we demonstrate a band-gap tuning strategy based on A-site cations of mismatched size (dimethylammonium and cesium) to enable a 1.7 eV perovskite with high, stable voltages. By combining these advances, we fabricate two-terminal all-perovskite tandem solar cells with 23.1% power conversion efficiency on rigid substrates and 21.3% on flexible plastic substrates.

Mixed-cation-based perovskite solar cells are investigated under conditions consistent with those found in orbit around Mars, Jupiter, and Saturn. Temperature dependent photoluminescence spectra sh...

Here we use time-resolved and steady-state optical spectroscopy on state-of-the-art low- and high-bandgap perovskite films for tandems to quantify intrinsic recombination rates and absorption coefficients. We apply these data to calculate the limiting efficiency of perovskite-silicon and all-perovskite two-terminal tandems employing currently available bandgap materials as 42.0 % and 40.8 % respectively. By including luminescence coupling between sub-cells, i.e. the re-emission of photons from the high-bandgap sub-cell and their absorption in the low-bandgap sub-cell, we reveal the stringent need for current matching is relaxed when the high-bandgap sub-cell is a luminescent perovskite compared to calculations that do not consider luminescence coupling. We show luminescence coupling becomes important in all-perovskite tandems when charge carrier trapping rates are < 10$^{6}$ s$^{-1}$ (corresponding to carrier lifetimes longer than 1 $��$s at low excitation densities) in the high-bandgap sub-cell, which is lowered to 10$^{5}$ s$^{-1}$ in the better-bandgap-matched perovskite-silicon cells. We demonstrate luminescence coupling endows greater flexibility in both sub-cell thicknesses, increased tolerance to different spectral conditions and a reduction in the total thickness of light absorbing layers. To maximally exploit luminescence coupling we reveal a key design rule for luminescent perovskite-based tandems: the high-bandgap sub-cell should always have the higher short-circuit current. Importantly, this can be achieved by reducing the bandgap or increasing the thickness in the high-bandgap sub-cell with minimal reduction in efficiency, thus allowing for wider, unstable bandgap compositions (>1.7 eV) to be avoided. Finally, we experimentally visualise luminescence coupling in an all-perovskite tandem device stack through cross-section luminescence images., 20 pages, 5 figures

We demonstrate the critical role of surface recombination in mixed-cation, mixed-halide perovskite, FA0.83Cs0.17Pb(I0.85Br0.15)3. By passivating non-radiative defects with the polymerizable Lewis base (3-aminopropyl)trimethoxysilane (APTMS) we transform these thin films. We demonstrate average minority carrier lifetimes > 4 ��s, nearly single exponential monomolecular PL decays, and concomitantly high external photoluminescence quantum efficiencies (>20%, corresponding to ~97% of the maximum theoretical quasi-Fermi-level splitting) at low excitation fluence. We confirm both the composition and valence band edge position of the FA0.83Cs0.17Pb(I0.85Br0.15)3 perovskite using multi-institution, cross-validated, XPS and UPS measurements. We extend the APTMS surface passivation to higher bandgap double cation (FA,Cs) compositions (1.7 eV, 1.75 eV and 1.8 eV) as well as the widely used triple cation (FA,MA,Cs) composition and observe significant PL and PL lifetime improvements after surface passivation. Finally, we demonstrate that the average surface recombination velocity (SRV) decreases from ~1000 cm/s to ~10 cm/s post APTMS passivation for FA0.83Cs0.17Pb(I0.85Br0.15)3. Our results demonstrate that surface-mediated recombination is the primary non-radiative loss pathway in MA-free mixed-cation mixed-halide films with a range of different bandgaps, which is a problem observed for a wide range of perovskite active layers and reactive electrical contacts. This study indicates that surface passivation and contact engineering will enable near-theoretical device efficiencies with these materials.

We use time-resolved photoluminescence measurements to determine the biexciton Auger recombination rate in both hybrid organic-inorganic and fully inorganic halide perovskite nanocrystals as a function of nanocrystal volume. We find that the volume scaling of the biexciton Auger rate in the hybrid perovskites, containing a polar organic A-site cation, is significantly shallower than in the fully inorganic Cs-based nanocrystals. As the nanocrystals become smaller, the Auger rate in the hybrid nanocrystals increases even less than expected, compared to the fully inorganic nanocrystals, which already show a shallower volume dependence than other material systems such as chalcogenide quantum dots. This finding suggests there may be differences in the strength of Coulombic interactions between the fully inorganic and hybrid perovskites, which may prove to be crucial in selecting materials to obtain the highest performing devices in the future, and hints that there could be something "special" about the hybrid materials.

Funder: European Research Council; Id: http://dx.doi.org/10.13039/501100000781, Funder: Engineering and Physical Sciences Research Council; Id: http://dx.doi.org/10.13039/501100000266, Funder: European Union's Horizon 2020, Radiation‐resistant but cost‐efficient, flexible, and ultralight solar sheets with high specific power (W g−1) are the “holy grail” of the new space revolution, powering private space exploration, low‐cost missions, and future habitats on Moon and Mars. Herein, this study investigates an all‐perovskite tandem photovoltaic (PV) technology that uses an ultrathin active layer (1.56 µm) but offers high power conversion efficiency, and discusses its potential for high‐specific‐power applications. This study demonstrates that all‐perovskite tandems possess a high tolerance to the harsh radiation environment in space. The tests under 68 MeV proton irradiation show negligible degradation (22%. Using high spatial resolution photoluminescence (PL) microscopy, it is revealed that defect clusters in GaAs are responsible for the degradation of current space‐PV. By contrast, negligible reduction in PL of the individual perovskite subcells even after the highest dose studied is observed. Studying the intensity‐dependent PL of bare low‐gap and high‐gap perovskite absorbers, it is shown that the VOC, fill factor, and efficiency potentials remain identically high after irradiation. Radiation damage of all‐perovskite tandems thus has a fundamentally different origin to traditional space PV.

Mixed organic-inorganic halide perovskite solar cells (PSCs) have received considerable attention in recent years for their impressive solar to electrical power efficiency gains and potentially lower material and processing costs for optoelectronic applications. In addition to terrestrial applications, PSCs are of interest to the space power markets for their low cost, low weight, adaptability to flexible architectures, and tolerance to high energy particle irradiation (mainly protons and electrons). Here we investigate the properties of mixed formamidinium-methylammonium tin-lead iodide (FASn)0.6(MAPb)0.4I3 perovskites which lower the lead content as well as the bandgap, making them attractive for the low bandgap absorber material in tandem PSCs. Through current density-voltage (JV) characterization at lower temperatures, majority carrier transport is hindered and a barrier to photogenerated carrier extraction is evident. This is attributed to the thermally induced change of the bandgap of the absorber layer relative to the energy selective contacts in the device. We find that although the architecture used here hinders the performance at temperatures below 225 K, the tolerance to high energy (3.7 MeV) protons is impressive, considerably out-performing commercially available thin-film CIGS. These results suggest further improvements to structural and interface stability as well as lightweight encapsulation could lead to all perovskite flexible tandem arrays deployed for power generation on missions to low Earth orbit, the moon, Mars, and beyond.

We demonstrate exchange of the B-site metal cation in hybrid organic–inorganic halide perovskite thin films. We exchange tin in formamidinium tin triiodide (CH(NH2)2SnI3, or FASnI3) with lead at controllable levels, forming CH(NH2)2SnxPb1–xI3 alloys with partial substitution and fully converting the film to CH(NH2)2PbI3 with a large excess of Pb2+. We observe no evidence for phase segregation or bilayered films, indicating that conversion is uniform throughout the film. This facile technique provides a new way to control composition independently from the crystallization processes, allowing formation of the black phase of CH(NH2)2PbI3 at much lower temperatures than those previously reported while also opening the door to new morphology–composition combinations. The surprising observation that the B-site metal cations are mobile may also provide insight into the nature of transient processes in these materials, suggesting that they may be involved in ionic conduction, and will be a critical consideration ...

Perovskite solar cells have shown phenomenal progress and have great potential to be manufactured as low‐cost large area modules. However, perovskite films often suffer from pinholes and the resulting contact between hole‐ and electron transporting layers provides lower resistance (shunt) pathways, leading to decreased open‐circuit voltage and fill factor. This problem is even more severe in large area cells and especially in the case of neutral color semitransparent cells, where a large absorber‐free area is required to provide the desired transparency. Herein, a simple, inexpensive, and scalable wet chemical method is presented to block these “shunting paths” via deposition of transparent, insulating molecular layers, which preferentially bind to the uncovered surface of the electron collecting oxide, without hindering charge extraction from the perovskite to the charge collection layers. It is shown that this method improves the performance in semitransparent cells, where the enhancement in open‐circuit voltage is up to 30% without negatively impacting the photocurrent. Using this method, we achieved an efficiency of 6.1% for a neutral color semitransparent perovskite cell with 38% average visible transmittance. This simple shunt blocking technique has applications in improving the yield as well as efficiency of large area perovskite solar cells and light emitting devices.

Tin-lead perovskites have low band gaps (1.2 eV – 1.4 eV) that offer complementary absorption spectra to mixed halide perovskites with band gaps in the range of 1.6 eV – 1.85 eV. In combination, tin-lead and mixed halide perovskites can be used to make efficient all-perovskite tandem solar cells. While these can achieve high efficiency, they are hampered by the unproven longterm stability of tin-containing perovskites. We make the first demonstration of tin-lead perovskite solar cells that pass benchmark 1000-hour tests of stability under stressors of heat, light, and atmospheric exposure. We identify that mixed tin-lead perovskites oxidise by a different chemical pathway, one that is much less favourable, than the oxidation pathway followed by pure tin perovskites, making them significantly more stable. Fortuitously, mixed tin-lead perovskites also have band gaps that are close to ideal for the rear cell of an all-perovskite monolithic two-junction tandem. Beyond selecting the composition of the perovskite to be one that has inherently suppressed tendency to oxidise, we also fabricate a novel heterojunction-based architecture that eliminates the commonly used acidic PEDOT:PSS layer, which leads to enhanced stability. By packaging the resulting solar cell in a glass-on-glass package with a pliable low-elastic-modulus polyolefin encapsulant and a butyl rubber edge seal, we also demonstrate that the low band gap perovskite solar cell that passes the IEC damp heat test for thin film solar cells – a milestone that demonstrates the removal of a significant impediment to the commercialization of high efficiency perovskite tandem solar cells.

Low-Temperature-Low-Intensity (LILT) conditions consistent with those found in orbit around the outer planets are applied on mixed-cation-based perovskite solar cells. Stability under low temperature is supported by no evidence of a phase change in the temperature dependent photoluminescence spectra. Under 1-sun AM0 conditions at low temperature a barrier is apparent that impedes current flow and reduces the fill factor. However, under low intensity and low temperature, where the photogenerated current is less than the thermionic emission rate the carrier extraction, fill factor and efficiency are recovered; indicating perovskites are promising candidates for CubeSat and SmallSat outer planetary missions.

We demonstrate four-and two-terminal perovskite-perovskite tandem solar cells with ideally matched band gaps. We develop an infrared-absorbing 1.2-electron volt band-gap perovskite, FA(0.75)Cs(0.25)Sn(0.5)Pb(0.5)I(3), that can deliver 14.8% efficiency. By combining this material with a wider-band gap FA(0.83)Cs(0.17)Pb(I0.5Br0.5)(3) material, we achieve monolithic two-terminal tandem efficiencies of 17.0% with > 1.65-volt open-circuit voltage. We also make mechanically stacked four-terminal tandem cells and obtain 20.3% efficiency. Notably, we find that our infrared-absorbing perovskite cells exhibit excellent thermal and atmospheric stability, not previously achieved for Sn-based perovskites. This device architecture and materials set will enable "all-perovskite" thin-film solar cells to reach the highest efficiencies in the long term at the lowest costs. We thank M. T. Horantner for performing the Shockley-Queisser calculation. The research leading to these results has received funding from the Graphene Flagship (Horizon 2020 grant no. 696656 - GrapheneCore1), the Leverhulme Trust (grant RL-2012-001), the UK Engineering and Physical Sciences Research Council (grant EP/J009857/1 and EP/M020517/1), and the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement nos. 239578 (ALIGN) and 604032 (MESO). T.L. is funded by a Marie Sklodowska Curie International Fellowship under grant agreement H2O2IF-GA-2015-659225. A.B. is financed by IMEC (Leuven) in the framework of a joint Ph.D. program with Hasselt University. B.C. is a postdoctoral research fellow of the Research Fund Flanders (FWO). We also acknowledge the U.S. Office of Naval Research for support. We acknowledge the use of the University of Oxford Advanced Research Computing (ARC) facility (http://dx.doi.org/10.5281/zenodo.22558) and the ARCHER UK National Super-computing Service under the "AMSEC" Leadership project. We thank the Global Climate and Energy Project (GCEP) at Stanford University. All data pertaining to the conclusions of this work can be found in the main paper and the supplementary materials.

We use high-resolution, spatially resolved, laser beam induced current, confocal photoluminescence, and photoconductive atomic force microscopy (pcAFM) measurements to correlate local solar cell performance with spatially heterogeneous local material properties in methylammonium lead triiodide (CH3NH3PbI3) perovskite solar cells. We find that, for this material and device architecture, the photocurrent heterogeneity measured via pcAFM on devices missing a top selective contact with traditional Au-coated tips is significantly larger than the photocurrent heterogeneity observed in full devices with both electron- and hole-selective extraction layers, indicating that extraction barriers at the Au/perovskite interface are ameliorated by deposition of the organic charge extraction layer. Nevertheless, in completed, efficient device structures (PCE ≈ 16%) with state-of-the-art nickel oxide and [6,6]-phenyl-C61-butyric acid (PCBM) methyl ester contacts, we observe that the local photoluminescence (PL) is weakly ...

Semitransparent solar cells can open new applications in many areas, such as integration into buildings, and may also be important for construction of efficient multi-junction solar cells. Herein, ...

We report a new technique for tuning the bandgap of hybrid organic–inorganic halide perovskite materials. By dipping films of methylammonium or formamidinium lead triiodide (MAPbI3 or FAPbI3) in solutions of formamidinium or methylammonium iodide (FAI or MAI) at room temperature, we are able to inter-convert through cation exchange between perovskite materials, allowing us to carefully tune the bandgap between 1.57 and 1.48 eV. We observe uniform conversion through the entirety of the bulk film, with no evidence for a “bi-layered” or graded structure. By applying this technique to solar cell devices, we are able to enhance the performance of the single cation devices. Furthermore, we demonstrate that this technique allows us to form pure black phase FAPbI3 infiltrated into mesoporous scaffolds; this is normally infeasible since the pores confine the FAPbI3 in a yellow non-perovskite phase with a much wider bandgap, which is not of practical use in solar cells or other optoelectronic devices. Additionally, this work provides evidence for molecular cation mobility in the halide perovskites, indicating that the cations play a role in ionic conduction as well as the mobile anions.

The family of organic-inorganic halide perovskite materials has generated tremendous interest in the field of photovoltaics due to their high power conversion efficiencies. There has been intensive development of cells based on the archetypal methylammonium (MA)and recently introduced formamidinium (FA) materials, however, there is still considerable controversy over their fundamental electronic properties. Two of the most important parameters are the binding energy of the exciton (R$^{*}$) and its reduced effective mass $\mu$. Here we present extensive magneto optical studies of Cl assisted grown MAPbI$_{3}$ as well as MAPbBr$_{3}$ and the FA based materials FAPbI$_{3}$ and FAPbBr$_{3}$. We fit the excitonic states as a hydrogenic atom in magnetic field and the Landau levels for free carriers to give R$^{*}$ and $\mu$. The values of the exciton binding energy are in the range 14 - 25 meV in the low temperature phase and fall considerably at higher temperatures for the tri-iodides, consistent with free carrier behaviour in all devices made from these materials. Both R$^{*}$ and $\mu$ increase approximately proportionally to the band gap, and the mass values, 0.09-0.117 m$_{0}$, are consistent with a simple \textbf{k.p} perturbation approach to the band structure which can be generalized to predict values for the effective mass and binding energy for other members of this perovskite family of materials.

Despite rapid developments in both photovoltaic and light-emitting device performance, the understanding of the optoelectronic properties of hybrid lead halide perovskites is still incomplete. In particular, the polarizability of the material, the presence of molecular dipoles, and their influence on the dynamics of the photoexcitations remain an open issue to be clarified. Here, we investigate the effect of an applied external electric field on the photoexcited species of CH3NH3PbI3 thin films, both at room temperature and at low temperature, by monitoring the photoluminescence (PL) yield and PL decays. At room temperature we find evidence for electric-field-induced reduction of radiative bimolecular carrier recombination together with motion of charged defects that affects the nonradiative decay rate of the photoexcited species. At low temperature (190 K), we observe a field-induced enhancement of radiative free carrier recombination rates that lasts even after the removal of the field. We assign this to field-induced alignment of the molecular dipoles, which reduces the vibrational freedom of the lattice and the associated local screening and hence results in a stronger electron-hole interaction.

Metal halide perovskites (MHPs) have transfixed the photovoltaic (PV) community due to their outstanding and tunable optoelectronic properties coupled to demonstrations of high-power conversion efficiencies (PCE) at a range of bandgaps. This has motivated the field to push perovskites to reach the highest possible performance. One way to increase the efficiency is by fabricating multijunction solar cells, which can split the solar spectrum, reducing thermalization loss. Low-cost all-perovskite tandems have a real chance to soon exceed 30% PCE, which could transform the PV industry. Achieving this goal requires the identification of perovskite sub-cells that are both highly efficient and can be effectively integrated. Herein, it is discussed how to navigate the multiple-choice adventure in choosing between the myriad of options and considerations present when deciding what perovskite materials, contact layers, and processing tools to use. Some of the potential fabrication pitfalls often encountered in MHP based tandem PVs are highlighted, so that they can hopefully be avoided in the future.

Already exhibiting solar to electrical power conversion efficiencies of over 17%, organic-inorganic lead halide perovskite solar cells are one of the most promising emerging contenders in the drive to provide a cheap and clean source of energy. One concern however, is the potential toxicology issue of lead, a key component in the archetypical material. The most likely substitute is tin, which like lead, is also a group 14 metal. While organic-inorganic tin halide perovskites have shown good semiconducting behaviour, the instability of tin in its 2+ oxidation state has thus far proved to be an overwhelming challenge. Here, we report the first completely lead-free, CH3NH 3SnI3 perovskite solar cell processed on a mesoporous TiO2 scaffold, reaching efficiencies of over 6% under 1 sun illumination. Remarkably, we achieve open circuit voltages over 0.88 V from a material which has a 1.23 eV band gap. This journal is © the Partner Organisations 2014.

We report the fabrication of monolithic all-perovskite tandem solar cells with a stabilized power conversion efficiency of 19.1% and demonstrate improved thermal, atmospheric, and operational stability of the tin–lead perovskite (FA0.75Cs0.25Sn0.5Pb0.5I3) used as the low gap absorber. To achieve a high matched current density in the two-terminal tandem, we develop a route to fabricate uniform and thick tin–lead perovskites that enable the two-terminal tandem to attain external quantum efficiencies >80% in the near infrared. By post-processing the as-deposited tin–lead perovskite films with methylammonium chloride vapor, we increase grain sizes to over a micron and boost solar cell open circuit voltage and fill factor. Tin–lead perovskite solar cells made by this method exhibit the most stable operation at maximum power under simulated sunlight of any reported small bandgap perovskite solar cell to date. We show that an unencapsulated tin–lead perovskite solar cell maintains its full performance after 150 hours at 85C in air, which is substantially better than has been observed previously. This work identifies strategies for attaining highly efficient all-perovskite tandem solar cells while maintaining thermal and operational stability.

We study the spontaneous polarization of the archetypal semiconducting halide perovskite methylammonium lead triiodide (CH3NH3PbI3) that is currently being investigated for use in thin film solar cells and light-emitting diodes. Using both lateral and vertical piezoresponse force microscopy (PFM) to image polycrystalline thin films, we observed domains in the piezoresponse that reversibly appear and disappear below and above the tetragonal-to-cubic phase transition temperature. Importantly, we observe these domains to exhibit a piezoresponse that is predominantly in-plane for films with the (110) plane oriented parallel to the substrate, providing a measure of the polarization associated with specific crystal planes. We characterize the polarization and its temporal response using both local switching spectroscopy and time-dependent PFM spectra. These data show hysteresis loops with the polarization switching with bias but relaxing back on time scales of several minutes. Our results suggest the existence ...

A significant fraction of global electricity demand is for lighting. Enabled by the realization and development of efficient GaN blue light-emitting diodes (LEDs), phosphor-based solid-state white LEDs provide a much higher efficiency alternative to incandescent and fluorescent lighting, which are being broadly implemented. However, a key challenge for this industry is to achieve the right photometric ranges and application-specific emission spectra via cost-effective means. Here, we synthesize organic–inorganic lead halide-based perovskite crystals with broad spectral tuneability. By tailoring the composition of methyl and octlyammonium cations in the colloidal synthesis, meso- to nanoscale 3D crystals (5–50 nm) can be formed with enhanced photoluminescence efficiency. By increasing the octlyammonium cations content, we observe platelet formation of 2D layered perovskite sheets; however, these platelets appear to be less emissive than the 3D crystals. We further manipulate the halide composition of the p...

Moisture, in the form of ambient humidity, has a significant impact on methylammonium lead halide perovskite films. In particular, due to the hygroscopic nature of the methylammonium component, moisture plays a significant role during film formation. This issue has so far not been well understood and neither has the impact of moisture on the physical properties of resultant films. Herein, we carry out a comprehensive and well-controlled study of the effect of moisture exposure on methylammonium lead halide perovskite film formation and properties. We find that films formed in higher humidity atmospheres have a less continuous morphology but significantly improved photoluminescence, and that film formation is faster. In photovoltaic devices, we find that exposure to moisture, either in the precursor solution or in the atmosphere during formation, results in significantly improved open-circuit voltages and hence overall device performance. We then find that by post-treating dry films with moisture exposure, we can enhance photovoltaic performance and photoluminescence in a similar way. The enhanced photoluminescence and open-circuit voltage imply that the material quality is improved in films that have been exposed to moisture. We determine that this improvement stems from a reduction in trap density in the films, which we postulate to be due to the partial solvation of the methylammonium component and "self-healing" of the perovskite lattice. This work highlights the importance of controlled moisture exposure when fabricating high-performance perovskite devices and provides guidelines for the optimum environment for fabrication. Moreover, we note that often an unintentional water exposure is likely responsible for the high performance of solar cells produced in some laboratories, whereas careful synthesis and fabrication in a dry environment will lead to lower-performing devices.

Going toward the grains Great strides have been made in improving the efficiency of organic-inorganic perovskite solar cells. Further improvements are likely to depend on understanding the role of film morphology on charge-carrier dynamics. de Quilettes et al. correlated confocal fluorescence microscopy images with those from scanning electron microscopy to spatially resolve the photoluminescence and carrier decay dynamics from films of organic-inorganic perovskites. Carrier lifetimes varied widely even between grains, and chemical treatments could improve lifetimes Science , this issue p. 683

Photovoltachromic devices combine photovoltaic and electrochromic behaviours to enable adjustable transparency glazing, where the photovoltaic component supplies the power to drive the coloration. Such stand-alone, self-powered devices are of commercial interest for integration into windows and surfaces of buildings and vehicles. Here, we report for the first time a perovskite-based photovoltachromic device with self-adaptive transparency. This multifunctional device is capable of producing electrical power by solar energy conversion as well as undergoing a chromic transition from neutral-color semi-transparent to dark blue-tinted when irradiated with solar light, without any additional external bias. The combination of semi-transparent perovskite photovoltaic and solid-state electrochromic cells enables fully solid-state photovoltachromic devices with 26% (or 16%) average visible transmittance and 3.7% (or 5.5%) maximum light power conversion efficiency. Upon activating the self-tinting, the average visible transmittance drops to 8.4% (or 5.5%). These results represent a significant step towards the commercialization of photovoltachromic building envelopes.

Efficient, neutral-colored semitransparent solar cells are of commercial interest for incorporation into the windows and surfaces of buildings and automobiles. Here, we report on semitransparent perovskite solar cells that are both efficient and neutral-colored, even in full working devices. Using the microstructured architecture previously developed, we achieve higher efficiencies by replacing methylammonium lead iodide perovskite with formamidinium lead iodide. Current-voltage hysteresis is also much reduced. Furthermore, we apply a novel transparent cathode to the devices, enabling us to fabricate neutral-colored semitransparent full solar cells for the first time. Such devices demonstrate over 5% power conversion efficiency for average visible transparencies of almost 30%, retaining impressive color-neutrality. This makes these devices the best-performing single-junction neutral-colored semitransparent solar cells to date. These microstructured perovskite solar cells are shown to have a significant advantage over silicon solar cells in terms of performance at high incident angles of sunlight, making them ideal for building integration.

Metal halide perovskite semiconductors offer rapid, low-cost deposition of solar cell active layers with a wide range of band gaps, making them ideal candidates for multijunction solar cells. Here, we combine optical and electrical models using experimental inputs to evaluate the feasible performances of all-perovskite double-junction (2PJ), triple-junction (3PJ), and perovskite-perovskite-silicon triple-junction (2PSJ) solar cells. Using parameters and design constraints from the current state-of-the-art generation of perovskite solar cells, we find that 2PJs can feasibly approach 32% power conversion efficiency, 3PJs can reach 33%, and 2PSJs can surpass 35%. We also outline pathways to improve light harvesting and demonstrate that it is possible to raise the performances to 34%, 37%, and 39% for the three architectures. Additionally, we discuss important future directions of research. Finally, we perform energy yield modeling to demonstrate that the multijunction solar cells should not suffer from reduced operational performances due to discrepancies between the AM1.5G and real-world spectrum over the course of a year.

The current decay in response to a sudden change of applied bias up to 1 V has been measured on a methylammonium lead triiodide perovskite solar cell with titania and spiro-OMeTAD transport layers, for temperatures between 258 and 308 K. These measurements are highly reproducible, in contrast to most other techniques used to investigate perovskite cells. A drift-diffusion model that accounts for slow moving ions as well as electrons and holes acting as charge carriers was used to predict the current transients. The close fit of the model predictions to the measurements shows that mobile ions in the perovskite layer influence transient behaviour on timescales of up to 50 s. An activation energy of 0.55 eV is inferred from fitting simulations to measurements made at room temperature.

This study presents a prediction of the yearly energy production and visual comfort benefits deriving from the adoption of building integrated semitransparent photovoltaic windows. Measured electrical and optical properties of neutral-colored solid-state planar heterojunction perovskite cells, characterized by promising transparency and photovoltaic conversion efficiency, were applied to a hypothetic photovoltaic glazing. Such experimental data were used as input to estimate annual energy production and visual comfort effects. The effect of different climate conditions was also investigated. A south-oriented test-room was modelled, assuming two window-to-wall ratios (WWRs) for office buildings, 19% and 32%, respectively. Energy yield was calculated at different locations showing figures between 20 and 30 kWh/m2 per year, with negligible reduction (not exceeding 3% in the hottest climates) when cell temperature was taken into account. Visual comfort assessment was carried out using two typical metrics: Useful Daylight Illuminance (UDI) and Daylight Glare Probability (DGP), comparing the performances of a photovoltaic glass with those of a commercial solar control glass and of a clear glass, acting as a reference. We found that the use of photovoltaic glass, independent of the location latitude, showed a significant increase in UDI values respect to clear glasses and performances comparable to solar control glasses. With reference to DGP, the use of photovoltaic glass allowed the reduction of occurrence of high DGP values (>0.45) of about 12–23%, depending on the location. Finally, we compared the annual energy production of building integrated photovoltaic cells to the annual use of electric energy for artificial lighting, finding that in most of the cases the annual energy production overcomes the amount of electric energy used for artificial lighting.

Building integration of innovative photovoltaic technologies, defined by high efficiency and optical properties allowing their use as a replacement of solar control films, offers new opportunities for energy saving. In order to estimate this potential under real world conditions, we have carried out simulations for this scenario based on an existing office building located in Bari (Italy). The building has a significant amount of transparent surfaces combined with transparent shades, while office layout corresponds to a typical Mediterranean configuration with several single/double offices (2.9 m by 6.6 m). We investigate the effect of the replacement of standard clear glass windows with new windows integrating perovskite-based semi-transparent photovoltaic modules, and the replacement of the original transparent shading system with high performance opaque perovskite-perovskite tandem cells. In particular, the attributes that were directly influenced by the proposed modifications were investigated in detail, including overall energy consumption for heating, air conditioning, and artificial lighting, evaluated against the overall energy yield given by building-integrated photovoltaic modules. Results showed that under ideal conditions (no obstructing buildings) yearly savings up to 18% could be obtained. In presence of nearby buildings savings dropped to 14%. Considering that fabrication costs for this technology are promisingly low and that this is currently the only neutral colored semi-transparent photovoltaic, the above results are promising, particularly for buildings with large window-to-wall ratios.

Solution-processed organometal trihalide perovskite solar cells are attracting increasing interest, leading to high performances over 15% in thin film architectures. Here, we probe the presence of sub gap states in both solid and mesosuperstructured perovskite films and determine that they strongly influence the photoconductivity response and splitting of the quasi-Fermi levels in films and solar cells. We find that while the planar perovskite films are superior to the mesosuperstructured films in terms of charge carrier mobility (in excess of 20 cm(2) V(-1) s(-1)) and emissivity, the planar heterojunction solar cells are limited in photovoltage by the presence of sub gap states and low intrinsic doping densities.

Unrestricted Travel in Solar Cells In the past 2 years, organolead halide perovskites have emerged as a promising class of light-harvesting media in experimental solar cells, but the physical basis for their efficiency has been unclear (see the Perspective by Hodes ). Two studies now show, using a variety of time-resolved absorption and emission spectroscopic techniques, that these materials manifest relatively long diffusion paths for charge carriers energized by light absorption. Xing et al. (p. 344 ) independently assessed (negative) electron and (positive) hole diffusion lengths and found them well-matched to one another to the ~100-nanometer optical absorption depth. Stranks et al. (p. 341 ) uncovered a 10-fold greater diffusion length in a chloride-doped material, which correlates with the material's particularly efficient overall performance. Both studies highlight effective carrier diffusion as a fruitful parameter for further optimization.