Henry J Snaith

Two dimensional/three‐dimensional (2D/3D) metal halide perovskite heterostructures have attracted great interest in photovoltaic and light‐emitting diode (LEDs) applications. In both, their implementation results in an improvement in device efficiency yet the understanding of these heterostructures remains incomplete. In this work the role of organic cations, essential for the formation of 2D perovskite structures is unraveled, in a range of metal halide perovskite heterostructures. These heterostructures are used to fabricate efficient green perovskite LEDs and a strong dependence between cation content and device performance is shown. The crystal structure, charge‐carrier transport and dynamics, and the electronic structure of these heterostructures are studied and it is shown that the presence of crystalline 2D perovskite inhibits electron injection and ultimately lowers device performance. This work highlights the …

All‐perovskite tandem solar cells show great potential to enable the highest performance at reasonable costs for a viable market entry in the near future. In particular, wide‐bandgap (WBG) perovskites with higher open‐circuit voltage (VOC) are essential to further improve the tandem solar cells’ performance. Here, a new 1.8 eV bandgap triple‐halide perovskite composition in conjunction with a piperazinium iodide (PI) surface treatment is developed. With structural analysis, it is found that the PI modifies the surface through a reduction of excess lead iodide in the perovskite and additionally penetrates the bulk. Constant light‐induced magneto‐transport measurements are applied to separately resolve charge carrier properties of electrons and holes. These measurements reveal a reduced deep trap state density, and improved steady‐state carrier lifetime (factor 2.6) and diffusion lengths (factor 1.6). As a result, WBG …

All-perovskite tandem solar cells are attracting considerable interest in photovoltaics research, owing to their potential to surpass the theoretical efficiency limit of single-junction cells, in a cost-effective sustainable manner. Thanks to the bandgap-bowing effect, mixed tin−lead (Sn−Pb) perovskites possess a close to ideal narrow bandgap for constructing tandem cells, matched with wide-bandgap neat lead-based counterparts. The performance of all-perovskite tandems, however, has yet to reach its efficiency potential. One of the main obstacles that need to be overcome is the─oftentimes─low quality of the mixed Sn−Pb perovskite films, largely caused by the facile oxidation of Sn(II) to Sn(IV), as well as the difficult-to-control film crystallization dynamics. Additional detrimental imperfections are introduced in the perovskite thin film, particularly at its vulnerable surfaces, including the top and bottom interfaces as well …

Surface defects of metal halide perovskite nanocrystals (PNCs) substantially compromise the optoelectronic performances of the materials and devices via undesired charge recombination. However, those defects, mainly the vacancies, are structurally entangled with each other in the PNC lattice, necessitating a delicately designed strategy for effective passivation. Here, a synergistic metal ion doping and surface ligand exchange strategy is proposed to passivate the surface defects of CsPbBr3 PNCs with various divalent metal (e.g., Cd2+, Zn2+, and Hg2+) acetate salts and didodecyldimethylammonium (DDA+) via one‐step post‐treatment. The addition of metal acetate salts to PNCs is demonstrated to suppress the defect formation energy effectively via the ab initio calculations. The developed PNCs not only have near‐unity photoluminescence quantum yield and excellent stability but also show luminance of …

Organic–inorganic halide perovskite semiconductors have revolutionized next‐generation photovoltaics (PV) due to several characteristics such as solution‐processability, gap tunability, and excellent charge generation and transport properties. This has made them very adaptable for various applications in light harvesting and photodetection. One such rapidly growing application is indoor photovoltaics (IPV) which have the potential to power standalone Internet of Things devices. IPV requires wider optimal bandgaps than solar cells (1.8 vs 1.3 eV) due to the differences between the spectra of artificial lights versus solar radiation. For IPV applications, the active layer wide‐gap perovskite must be developed systemically considering all other components of the device, such as interlayers, electrodes, and scaling. This perspective provides an overview of the potential and challenges facing perovskite‐based IPV …

Quaternary copper‐silver‐bismuth‐iodide compounds represent a promising new class of wide‐bandgap (2 eV) semiconductors for photovoltaic and photodetector applications. In this study, vapor phase co‐evaporation is utilized to fabricate Cu2AgBiI6 thin films and photovoltaic devices. The findings show that the properties of vapor‐deposited films are highly dependent upon processing temperature, exhibiting increased pinhole density and transforming into a mixture of quaternary, binary, and metallic phases depending on the post‐deposition annealing temperature. This change in phase is accompanied by an enhancement in photoluminescence (PL) intensity and charge‐carrier lifetime, along with the emergence of an additional absorption peak at high energy (≈3 eV). Generally, increased PL is a desirable property for a solar absorber material, but this change in PL is ascribed to the formation of CuI impurity …

The developing Internet of Things market is attracting the indoor photovoltaic (IPV) as an essential power source. Perovskite photovoltaics (PPVs) are a fascinating candidate for IPV in solution-processable photovoltaics. Recent developments in PPVs can deliver power conversion efficiency (PCE) up to 25% outdoor (AM 1.5 G) and over 40% under indoor (1000 lux) light. The selection of charge transport layers (CTLs) has played an essential role in improving PPVs indoor performance. Herein, formamidinium-caesium-based mixed-cation (FACsPb (I, Br) 3) PPV devices are fabricated, and evaluated their outdoor and indoor performances by changing the different CTL combinations such as PTAA-PCBM and SAM-C 60. Outdoor PCEs were 13.76% and 15.27% achieved for PTAA-PCBM and SAM-C 60-based devices, respectively. Meanwhile, under LED (4000 K) 1000 lux, the PCEs were 26.32% and 31.92% for …

Monolithic all-perovskite triple-junction solar cells have the potential to deliver power conversion efficiencies beyond those of state-of-art double-junction tandems and well beyond the detailed-balance limit for single junctions. Today, however, their performance is limited by large deficits in open-circuit voltage and unfulfilled potential in both short-circuit current density and fill factor in the wide-bandgap perovskite sub cell. Here we find that halide heterogeneity—present even immediately following materials synthesis—plays a key role in interfacial non-radiative recombination and collection efficiency losses under prolonged illumination for Br-rich perovskites. We find that a diammonium halide salt, propane-1,3-diammonium iodide, introduced during film fabrication, improves halide homogenization in Br-rich perovskites, leading to enhanced operating stability and a record open-circuit voltage of 1.44 V in an …

Metal halide perovskites are promising light absorbers for multijunction photovoltaic applications because of their remarkable bandgap tunability, achieved through compositional mixing on the halide site. However, poor energy‐level alignment at the interface between wide‐bandgap mixed‐halide perovskites and charge‐extraction layers still causes significant losses in solar‐cell performance. Here, the origin of such losses is investigated, focusing on the energy‐level misalignment between the valence band maximum and the highest occupied molecular orbital (HOMO) for a commonly employed combination, FA0.83Cs0.17Pb(I1‐xBrx)3 with bromide content x ranging from 0 to 1, and poly[bis(4‐phenyl)(2,4,6‐trimethylphenyl)amine] (PTAA). A combination of time‐resolved photoluminescence spectroscopy and numerical modeling of charge‐carrier dynamics reveals that open‐circuit voltage (VOC) losses …

The ability to characterise perovskite phases non-destructively is key on the route to ensuring their long-term stability in operando. Raman spectroscopy holds the promise to play an important role in this task. Among all perovskites, formamidinium lead iodide (FAPbI3) has emerged as one of the most promising candidates for single-junction photovoltaic cells. However, Raman spectroscopy of FAPbI3 remains challenging as is evidenced by conflicting reports in the literature. Here, we demonstrate that due to the vulnerability of FAPbI3 to laser-induced degradation, the detected Raman spectrum depends strongly on the experimental conditions. This can lead to conflicting results and is revealed as the origin of discrepancies in the literature. We overcome this issue by deploying defocused Raman spectroscopy, preventing laser-induced damage to the sample and simultaneously improving the signal-to-noise ratio …

Three‐photon‐pumped (3PP) excitonic lasing in inorganic semiconductor quantum dots (QDs) is of particular importance for near‐infrared biophotonics and optical communications. However, the implementation of such lasers has been hindered severely by the required high pump thresholds. Here, 3PP excitonic lasing of all‐inorganic cesium lead bromide perovskite QDs (CsPbBr3 PQDs) embedded in a whispering‐gallery microcavity is demonstrated, and achieving a record low threshold of 3 mJ cm−2 by tuning the 3P pump energy in resonance with the S exciton state. Wavelength‐dispersive Z‐scan spectroscopy reveals that such reduced lasing threshold is attributed to the exciton resonance enhanced multiphoton absorption, which, as disclosed by the kinetics analysis of transient absorption spectroscopy (TAS), leads to the appearance of net gain at a pump fluence as low as 2.2 mJ cm−2, corresponding to …

Perovskite solar cells (PSCs) comprise a solid perovskite absorber sandwiched between several layers of different charge-selective materials, ensuring unidirectional current flow and high voltage output of the devices 1, 2. A ‘buffer material’between the electron-selective layer and the metal electrode in p-type/intrinsic/n-type (pin) PSCs (also known as inverted PSCs) enables electrons to flow from the electron-selective layer to the electrode 3, 4, 5. Furthermore, it acts as a barrier inhibiting the inter-diffusion of harmful species into or degradation products out of the perovskite absorber 6, 7, 8. Thus far, evaporable organic molecules 9, 10 and atomic-layer-deposited metal oxides 11, 12 have been successful, but each has specific imperfections. Here we report a chemically stable and multifunctional buffer material, ytterbium oxide (YbO x), for pin PSCs by scalable thermal evaporation deposition. We used this YbO x …

The limited conductivity of existing transparent conducting oxide (TCO) greatly restricts the further performance improvement of perovskite solar cells (PSCs), especially for large‐area devices. Herein, buried‐metal‐grid tin‐doped indium oxide (BMG ITO) electrodes are developed to minimize the power loss caused by the undesirable high sheet resistance of TCOs. By burying 140‐nm‐thick metal grids into ITO using a photolithography technique, the sheet resistance of ITO is reduced from 15.0 to 2.7 Ω sq−1. The metal step of BMG over ITO has a huge impact on the charge carrier transport in PSCs. The PSCs using BMG ITO with a low metal step deliver power conversion efficiencies (PCEs) significantly better than that of their counterparts with higher metal steps. Moreover, compared with the pristine ITO‐based PSCs, the BMG ITO‐based PSCs show a smaller PCE decrease when scaling up the active area of …

The presence of mobile ions in metal halide perovskites has been shown to adversely affect the intrinsic stability of perovskite solar cells (PSCs). However, the actual contribution of mobile ions to the total degradation loss compared with other factors such as trap-assisted recombination remains poorly understood. Here we reveal that mobile ion-induced internal field screening is the dominant factor in the degradation of PSCs under operational conditions. The increased field screening leads to a decrease in the steady-state efficiency, often owing to a large reduction in the current density. Instead, the efficiency at high scan speeds (>1,000 V s−1), where the ions are immobilized, is much less affected. We also show that the bulk and interface quality do not degrade upon ageing, yet the open-circuit voltage decreases owing to an increase in the mobile ion density. This work reveals the importance of ionic losses for …

The invention provides an optoelectronic device comprising a porous material, which porous material comprises a semiconductor comprising a perovskite. The porous material may comprise a porous perovskite. Thus, the porous material may be a perovskite material which is itself porous. Additionally or alternatively, the porous material may comprise a porous dielectric scaffold material, such as alumina, and a coating disposed on a surface thereof, which coating comprises the semiconductor comprising the perovskite. Thus, in some embodiments the porosity arises from the dielectric scaffold rather than from the perovskite itself. The porous material is usually infiltrated by a charge transporting material such as a hole conductor, a liquid electrolyte, or an electron conductor. The invention further provides the use of the porous material as a semiconductor in an optoelectronic device. Further provided is the use of the …

The continued development of renewable energy is clearly critical for eliminating the use of fossil fuels. There is no possibility of a sustainable, stable future for humanity or the broader environment and ecosystem on Earth without making this transition to renewables over the next few decades. The renewable power generation technologies are numerous, and many will play a role in our future power generation network, but there exist some clear front runners. Hydroelectric power (HEP) is well established, but the capacity is geographically dependent and the large dams required for HEP can have severe consequences to the local environment. Wind power is widespread and will continue to expand and generate a significant fraction of our future power demands, although the predominant requirement to create off-shore wind farms, rather than on-shore, has and will continue to slow down the price reduction. At some point however, the potential for larger and larger off-shore wind turbines, enabled

The present invention relates to a semiconductor device comprising a semiconducting material, wherein the semiconducting material comprises a compound comprising:(i) one or more first monocations [A];(ii) one or more second monocations [B “;(iii) one or more trications [B “); and (iv) one or more halide anions| X]. The invention also relates to a process for producing a semiconductor device comprising said semiconducting material. Also described is a compound comprising:(i) one or more first monocations [A];(ii) one or more second monocations [B"| selected from Cu", Ag" and Au";(iii) one or more trications [B “); and (iv) one or more halide anions [X].

The present invention relates to a process for producing a layer of a crystalline A/M/X material, which crystalline A/M/X material comprises a compound of formula [A] a [M] b [X] c, wherein:[M] comprises one or more first cations, which one or more first cations are metal or metalloid cations;[A] comprises one or more second cations;[X] comprises one or more halide anions; a is an integer from 1 to 6; b is an integer from 1 to 6; and c is an integer from 1 to 18, wherein the process comprises disposing on a substrate a precursor composition comprising:(a) a first precursor compound comprising a first cation (M), which first cation is a metal or metalloid cation; and (b) a solvent, and wherein the solvent comprises:(i) a non-polar organic solvent which is a hydrocarbon solvent, a chlorohydrocarbon solvent or an ether solvent; and (ii) a first organic amine comprising at least three carbon atoms. Also described are compositions …

Understanding the kinetic competition between charge extraction and recombination, and how this is impacted by mobile ions, remains a key challenge in perovskite solar cells (PSCs). Here, this issue is addressed by combining operando photoluminescence (PL) measurements, which allow the measurement of real‐time PL spectra during current–voltage (J–V) scans under 1‐sun equivalent illumination, with the results of drift‐diffusion simulations. This operando PL analysis allows direct comparison between the internal performance (recombination currents and quasi‐Fermi‐level‐splitting (QFLS)) and the external performance (J–V) of a PSC during operation. Analyses of four PSCs with different electron transport materials (ETMs) quantify how a deeper ETM LUMO induces greater interfacial recombination, while a shallower LUMO impedes charge extraction. Furthermore, it is found that a low ETM mobility leads …

Understanding performance losses in all‐perovskite tandem photovoltaics is crucial to accelerate advancements toward commercialization, especially since these tandem devices generally underperform in comparison to what is expected from isolated layers and single junction devices. Here, the individual sub‐cells in all‐perovskite tandem stacks are selectively characterized to disentangle the various losses. It is found that non‐radiative losses in the high‐gap subcell dominate the overall recombination in the baseline system, as well as in the majority of literature reports. Through a multi‐faceted approach, the open‐circuit voltage (VOC) of the high‐gap perovskite subcell is enhanced by 120 mV. Employing a novel (quasi) lossless indium oxide interconnect, this enables all‐perovskite tandem solar cells with 2.00 V VOC and 23.7% stabilized efficiency. Reducing transport losses as well as imperfect energy …

Inverted‐structure metal halide perovskite solar cells (PSCs) have attractive advantages like low‐temperature processability and outstanding device stability. The two‐step sequential deposition method shows the benefits of easy fabrication and decent performance repeatability. Nevertheless, it is still challenging to achieve high‐performance inverted PSCs with similar or equal power conversion efficiencies (PCEs) compared to the regular‐structure counterparts via this deposition method. Here, an improved two‐step sequential deposition technique is demonstrated via treating the bottom organic hole‐selective layer with the binary modulation system composed of a polyelectrolyte and an ammonium salt. Such improved sequential deposition method leads to the spontaneous refinement of up and buried interfaces for the perovskite films, contributing to high film quality with significantly reduced defect density and …

High temperature post‐deposition annealing of hybrid lead halide perovskite thin films—typically lasting at least 10 min—dramatically limits the maximum roll‐to‐roll coating speed, which determines solar module manufacturing costs. While several approaches for “annealing‐free” perovskite solar cells (PSCs) have been demonstrated, many are of limited feasibility for scalable fabrication. Here, this work has solvent‐engineered a high vapor pressure solvent mixture of 2‐methoxy ethanol and tetrahydrofuran to deposit highly crystalline perovskite thin‐films at room temperature using gas‐quenching to remove the volatile solvents. Using this approach, this work demonstrates p‐i‐n devices with an annealing‐free MAPbI3 perovskite layer achieving stabilized power conversion efficiencies (PCEs) of up to 18.0%, compared to 18.4% for devices containing an annealed perovskite layer. This work then explores the …

In article number 2303472, Do-Hoon Hwang, Bo Ram Lee, and co-workers design crosslinked poly (FCA 60-co-BFCA 20-co-VFCA 20) as a temperature-dependent hole transport layer for perovskite nanocrystal light-emittingdiodes (LEDs), balancing charge injection, reducing interface exciton quenching and Joule heating. The effective thermal management of the working device results in a 2-fold increase in ex-ternal quantum efficiency (EQE) and a remarkable 150-fold extension of the operational lifetime compared to LEDs with poly (4-butyl-phenyl-diphenyl-amine)(poly-TPD) as the hole transport layer.

The invention relates to perovskite compounds which have surprisingly good emission properties, particularly photoluminescent emission properties, in the blue region of the visible spectrum. These perovskites contain a mixture of cations or a mixture of halides, or both. The invention also relates to a photoactive material containing the perovskite species of the invention; to an optoelectronic device containing the photoactive material of the invention; to a method of producing blue light; and to the use of the photoactive material of the invention to emit blue light or as a phosphor.

Formamidinium lead trioiodide (FAPbI3) is a promising perovskite for single-junction solar cells. However, FAPbI3 is metastable at room temperature and can cause intrinsic quantum confinement effects apparent through a series of above-bandgap absorption peaks. Here, we explore three common solution-based film-fabrication methods, neat N,N-dimethylformamide (DMF)–dimethyl sulfoxide (DMSO) solvent, DMF-DMSO with methylammonium chloride, and a sequential deposition approach. The latter two offer enhanced nucleation and crystallization control and suppress such quantum confinement effects. We show that elimination of these absorption features yields increased power conversion efficiencies (PCEs) and short-circuit currents, suggesting that quantum confinement hinders charge extraction. A meta-analysis of literature reports, covering 244 articles and 825 photovoltaic devices incorporating FAPbI …

Lead Mixed Halide Perovskites (LMHPs), CsPbBrI2, have attracted significant interest as promising candidates for wide bandgap absorber layers in tandem solar cells due to their relative stability and red-light emission with a bandgap ∼1.7 eV. However, these materials segregate into Br-rich and I-rich domains upon continuous illumination, affecting their optical properties and compromising the operational stability of devices. Herein, we track the microscopic processes occurring during halide segregation by using combined spectroscopic measurements at room and cryogenic temperatures. We also evaluate a passivation strategy to mitigate the halide migration of Br/I ions in the films by overcoating with cyclic olefin copolymer (COC). Our results explain the correlation between grain size, intensity dependencies, phase segregation, activation energy barrier, and their influence on photoinduced carrier lifetimes …

Light-emitting diodes (LEDs) are ubiquitous in modern society, with applications spanning from lighting and displays to medical diagnostics and data communications. Metal-halide perovskites are promising materials for LEDs because of their excellent optoelectronic properties and solution processability. Although research has progressed substantially in optimizing their external quantum efficiency, the modulation characteristics of perovskite LEDs remain unclear. Here we report a holistic approach for realizing fast perovskite photonic sources on silicon based on tailoring alkylammonium cations in perovskite systems. We reveal the recombination behaviour of charged species at various carrier density regimes relevant for their modulation performance. By integrating a Fabry–Pérot microcavity on silicon, we demonstrate perovskite devices with efficient light outcoupling. We achieve device modulation bandwidths …

Semiconducting lead halide perovskite nanocrystals (PNCs) are regarded as promising candidates for next‐generation optoelectronic devices due to their solution processability and outstanding optoelectronic properties. While the field of light‐emitting diodes (LEDs) and photovoltaics (PVs), two prime examples of optoelectronic devices, has recently seen a multitude of efforts toward high‐performance PNC‐based devices, realizing both devices with high efficiencies and stabilities through a single PNC processing strategy has remained a challenge.  In this work, diphenylpropylammonium (DPAI) surface ligands, found through a judicious ab‐initio‐based ligand search, are shown to provide a solution to this problem. The universal PNC ink with DPAI ligands presented here, prepared through a solution‐phase ligand‐exchange process, simultaneously allows single‐step processed LED and PV devices with peak …

Interfaces in thin‐film photovoltaics play a pivotal role in determining device efficiency and longevity. In this work, the top surface treatment of mixed tin–lead (≈1.26 eV) halide perovskite films for p–i–n solar cells is studied. Charge extraction is promoted by treating the perovskite surface with piperazine. This compound reacts with the organic cations at the perovskite surface, modifying the surface structure and tuning the interfacial energy level alignment. In addition, the combined treatment with C60 pyrrolidine tris‐acid (CPTA) reduces hysteresis and leads to efficiencies up to 22.7%, with open‐circuit voltage values reaching 0.90 V, ≈92% of the radiative limit for the bandgap of this material. The modified cells also show superior stability, with unencapsulated cells retaining 96% of their initial efficiency after >2000 h of storage in N2 and encapsulated cells retaining 90% efficiency after >450 h of storage in air …

Photovoltaics (PVs) are a critical technology for curbing growing levels of anthropogenic greenhouse gas emissions, and meeting increases in future demand for low-carbon electricity. In order to fulfil ambitions for net-zero carbon dioxide equivalent (CO2eq) emissions worldwide, the global cumulative capacity of solar PVs must increase by an order of magnitude from 0.9 TWp in 2021 to 8.5 TWp by 2050 according to the International Renewable Energy Agency, which is considered to be a highly conservative estimate. In 2020, the Henry Royce Institute brought together the UK PV community to discuss the critical technological and infrastructure challenges that need to be overcome to address the vast challenges in accelerating PV deployment. Herein, we examine the key developments in the global community, especially the progress made in the field since this earlier roadmap, bringing together experts primarily from the UK across the breadth of the photovoltaics community. The focus is both on the challenges in improving the efficiency, stability and levelized cost of electricity of current technologies for utility-scale PVs, as well as the fundamental questions in novel technologies that can have a significant impact on emerging markets, such as indoor PVs, space PVs, and agrivoltaics. We discuss challenges in advanced metrology and computational tools, as well as the growing synergies between PVs and solar fuels, and offer a perspective on the environmental sustainability of the PV industry. Through this roadmap, we emphasize promising pathways forward in both the short- and long-term, and for communities working on technologies across …

Outstanding optoelectronic properties of mixed tin‐lead perovskites are the cornerstone for the development of high‐efficiency all‐perovskite tandems. However, recombination losses in Sn‐Pb perovskites still limit the performance of these perovskites, necessitating more fundamental research. Here, rubidium iodide is employed as an additive for methylammonium‐free Sn‐Pb perovskites. It is first investigated the effect of the RbI additive on the perovskite composition, crystal structure, and element distribution. Quasi‐Fermi level splitting and transient photoluminescence measurements reveal that the RbI additive reduces recombination losses and increases carrier lifetime of the perovskite films. This finding is attributed to an approximately ten‐fold reduction in the defect density following RbI treatment, as probed using constant final state yield photoelectron spectroscopy. Additionally, the concentration of Sn …

Metal halide perovskite based tandem solar cells are promising to achieve power conversion efficiency beyond the theoretical limit of their single‐junction counterparts. However, overcoming the significant open‐circuit voltage deficit present in wide‐bandgap perovskite solar cells remains a major hurdle for realizing efficient and stable perovskite tandem cells. Here, a holistic approach to overcoming challenges in 1.8 eV perovskite solar cells is reported by engineering the perovskite crystallization pathway by means of chloride additives. In conjunction with employing a self‐assembled monolayer as the hole‐transport layer, an open‐circuit voltage of 1.25 V and a power conversion efficiency of 17.0% are achieved. The key role of methylammonium chloride addition is elucidated in facilitating the growth of a chloride‐rich intermediate phase that directs crystallization of the desired cubic perovskite phase and …

Over the past decade, the performance of solar cells based on metal halide perovskite semiconductors has skyrocketed, now rivalling established technologies such as crystalline silicon. The most promising implementation of these perovskites is in tandem solar cells, which have delivered far higher power conversion efficiencies than single-junction devices alone. Given their tunable bandgap, perovskites are uniquely placed to act as both narrow-bandgap and wide-bandgap absorbers in tandem devices. Methylammonium-free wide-bandgap perovskites perform particularly poorly in tandem devices compared with their methylammonium-containing and narrower bandgap counterparts, illustrating considerable scope for improvement. In this Review, we highlight the challenges related to methylammonium-free perovskites, including the energy-loss pathways that currently constrain their open-circuit voltage and …

We report that device architecture engineering has a substantial impact on the reverse bias instability that has been reported as a critical issue in commercializing perovskite solar cells. We demonstrate breakdown voltages exceeding -15 V in typical pin structured perovskite solar cells via two steps: i) using polymer hole transporting materials; ii) using a more electrochemically stable gold electrode. While device degradation can be exacerbated by higher reverse bias and prolonged exposure, our as-fabricated perovskite solar cells completely recover their performance even after stressing at -7 V for 9 hours both in the dark and under partial illumination. Following these observations, we systematically discuss and compare the reverse bias driven degradation pathways in perovskite solar cells with different device architectures. Our model highlights the role of electrochemical reaction rates and species in dictating the reverse bias stability of perovskite solar cells.

In the last decade, perovskite semiconductors have triggered a revolution in solar cell research. However, critical issues remain concerning the stability of metal-halide perovskites, which need to be overcome to enable a large scale commercialisation of perovskite photovoltaics (PV). While the rather poor environmental stability of these perovskites is usually attributed to their ionic nature rendering them sensitive to moisture and oxygen, the actual contribution of mobile ions to the total degradation loss under different environmental conditions is poorly understood. In this work, we reveal that the initial degradation of perovskite semiconductors is largely the result of mobile ion-induced internal field screening-a phenomenon that has not been previously discussed in relation to the degradation of perovskite solar cells. The increased field screening leads to a decrease in the steady-state power conversion efficiency mainly due to a large reduction in current density, while the efficiency at high scan speeds (> 1000 V/s) where the ions are immobilized is much less affected. We also show that interfacial recombination does not increase upon ageing, yet the open-circuit voltage (VOC) decreases as the result of an increase in the mobile ion density upon ageing. Furthermore, similar ionic losses appear under different external stressors, in particular when there are free charges present in the absorber layer. This work reveals a key degradation mechanism, providing new insights into initial device degradation before chemical or extrinsic mechanical device degradation effects manifest, and it highlights the critical role mobile ions play therein.

In this work, we couple theoretical and experimental approaches to understand and reduce the losses of wide bandgap Br-rich perovskite pin devices at open-circuit voltage (VOC) and short-circuit current (JSC) conditions. A mismatch between the internal quasi-Fermi level splitting (QFLS) and the external VOC is detrimental for these devices. We demonstrate that modifying the perovskite top-surface with guanidinium-Br and imidazolium-Br forms a low-dimensional perovskite phase at the n-interface, suppressing the QFLS-VOC mismatch, and boosting the VOC. Concurrently, the use of an ionic interlayer or a self-assembled monolayer at the p-interface reduces the inferred field screening induced by mobile ions at JSC, promoting charge extraction and raising the JSC. The combination of the n- and p-type optimizations allows us to approach the thermodynamic potential of the perovskite absorber layer, resulting in …

The present invention relates to devices comprising metal halide perovskites and organic passivating agents. In particular, the invention relates to photovoltaic and optoelectronic devices comprising passivated metal halide perovskites. The device according to the invention comprises:(a) a metal halide perovskite; and (b) a passivating agent which is an organic compound; wherein molecules of the passivating agent are chemically bonded to anions or cations in the metal halide perovskite. The invention also provides a process for producing a photovoltaic device, which photovoltaic device comprises:(a) a metal halide perovskite; and (b) a passivating agent which is an organic compound; wherein molecules of the passivating agent are chemically bonded to anions or cations in the metal halide perovskite,(Continued)

Formamidinium lead triiodide (FAPbI3) is the leading candidate for single-junction metal–halide perovskite photovoltaics, despite the metastability of this phase. To enhance its ambient-phase stability and produce world-record photovoltaic efficiencies, methylenediammonium dichloride (MDACl2) has been used as an additive in FAPbI3. MDA2+ has been reported as incorporated into the perovskite lattice alongside Cl–. However, the precise function and role of MDA2+ remain uncertain. Here, we grow FAPbI3 single crystals from a solution containing MDACl2 (FAPbI3-M). We demonstrate that FAPbI3-M crystals are stable against transformation to the photoinactive δ-phase for more than one year under ambient conditions. Critically, we reveal that MDA2+ is not the direct cause of the enhanced material stability. Instead, MDA2+ degrades rapidly to produce ammonium and methaniminium, which subsequently …

An embodiment of the present invention relates to an optoelectronic device comprising an optoelectronic component, a waveguide having an optical waveguide section and an electrical conductor section, the optical waveguide section being transparent for radiation of a given wavelength or a given wavelength range and capable of guiding the radiation along the longitudinal axis of the waveguide, wherein the optical waveguide section is optically butt-coupled to an optical surface section of the optoelectronic component, and wherein the electrical conductor section is mechanically butt-coupled to an electrical contact of the optoelectronic component.

2023-02-01 Assigned to OXFORD UNIVERSITY INNOVATION LIMITED reassignment OXFORD UNIVERSITY INNOVATION LIMITED ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: WENGER, BERNARD, SAKAI, NOBUYA, SNAITH, HENRY JAMES

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 …

Perovskite/silicon tandems have smashed through the 30% efficiency barrier, which represents a promising step towards high efficiency solar modules. However, the processing used to fabricate high efficiency devices is not compatible with mass production. For this technology to be impactful in the urgent fight against climate change and be scalable to the multi-terawatt (TW) level, a shift in mindset is required when designing the silicon bottom cell. In this work, we outline the design requirements for the silicon cell, with a particular focus on the constraints imposed by industrial processing. In doing so, we discuss the type of silicon wafers used, the surface treatment, the most appropriate silicon cell architecture and the formation of metal contacts. Additionally, we frame this discussion in the context of multi-TW markets, which impose additional constraints on the processing relating to the sustainability of the materials …

Although significant progress has been made in the development of green, red, and near-infrared perovskite light-emitting diodes (PeLEDs), blue PeLEDs exhibit inferior performance, owing to various defects and poor carrier injection in solution-processed perovskite films. Thus, this study incorporates dual-passivation additive diphenylphosphinamide (DPPA) into perovskite films, and through density functional theory calculations and experimental characterizations, DPPA has been proven to be an effective passivator. Its phosphine oxide group coordinates with unsaturated lead ions, passivating perovskite defects, while the amino group forms hydrogen bonds with adjacent halide ions, suppressing their migration and further strengthening the passivation effect. Blue quasi-two-dimensional PeLEDs based on DPPA-modified perovskite films achieved an external quantum efficiency of 12.31% with an emission peak …

Halide perovskite light-emitting diodes (PeLEDs) exhibit great potential for use in next-generation display technologies. However, scale-up will be challenging due to the requirement of very thin transport layers for high efficiencies, which often present spatial inhomogeneities from improper wetting and drying during solution processing. Here, we show how a thin Al2O3 layer grown by atomic layer deposition can be used to preferentially cover regions of imperfect hole transport layer deposition and form an intermixed composite with the organic transport layer, allowing hole conduction and injection to persist through the organic hole transporter. This has the dual effect of reducing nonradiative recombination at the heterojunction and improving carrier selectivity, which we infer to be due to the inhibition of direct contact between the indium tin oxide and perovskite layers. We observe an immediate improvement in …

Tin-containing metal halide perovskites have enormous potential as photovoltaics, both in narrow band gap mixed tin–lead materials for all-perovskite tandems and for lead-free perovskites. The introduction of Sn(II), however, has significant effects on the solution chemistry, crystallization, defect states, and other material properties in halide perovskites. In this perspective, we summarize the main hurdles for tin-containing perovskites and highlight successful attempts made by the community to overcome them. We discuss important research directions for the development of these materials and propose some approaches to achieve a unified understanding of Sn incorporation. We particularly focus on the discussion of charge carrier dynamics and nonradiative losses at the interfaces between perovskite and charge extraction layers in p-i-n cells. We hope these insights will aid the community to accelerate the …

Inside Front Cover In article number 2300095, Hesjedal and co-workers demonstrate that the substitution of Co2+ ions into the halide perovskite imparts magnetic behavior to the material while maintaining photovoltaic performance. We utilize the Co2+ ions (shown as robots) themselves as probes to sense the local electronic environment of lead in the perovskite, thereby opening the substitution gateway for developing novel functional perovskite materials and devices for future technologies.

Ultranarrow bandwidth single-photon sources operating at room-temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud-based quantum information processing networks, and quantum metrology. Here we show a room-temperature ultranarrow bandwidth single-photon source generating single-mode photons at a rate of 5 MHz based on an inorganic CsPbI3 perovskite quantum dot embedded in a tunable open-access optical microcavity. When coupled to an optical cavity mode, the quantum dot room-temperature emission becomes single-mode, and the spectrum narrows down to just ∼1 nm. The low numerical aperture of the optical cavities enables efficient collection of high-purity single-mode single-photon emission at room-temperature, offering promising performance for photonic and quantum technology applications. We measure 94 …

Metal halide perovskite (MHP) semiconductors have driven a revolution in optoelectronic technologies over the last decade, in particular for high‐efficiency photovoltaic applications. Low‐dimensional MHPs presenting electronic confinement have promising additional prospects in light emission and quantum technologies. However, the optimisation of such applications requires a comprehensive understanding of the nature of charge carriers and their transport mechanisms. This study employs a combination of ultrafast optical and terahertz spectroscopy to investigate phonon energies, charge‐carrier mobilities, and exciton formation in 2D (PEA)2PbI4 and (BA)2PbI4 (where PEA is phenylethylammonium and BA is butylammonium). Temperature‐dependent measurements of free charge‐carrier mobilities reveal band transport in these strongly confined semiconductors, with surprisingly high in‐plane mobilities …

A photovoltaic device comprises plural layers separated into plural cells, each comprising a region of a photoactive layer and electrodes on opposite sides thereof. Each of the regions of the photoactive layer are formed comprising a first part that comprises photoactive material and a second part that is not photoactive and that has a greater transmittance of visible light than the light absorbing photoactive material, in pre-selected locations, or in a pre-selected distribution of locations, across the region of the photoactive layer. One of the first and second parts are located in plural separate areas within the other of the first and second parts. The transparency of the photovoltaic device is increased by the transmission of light through the second part that is not photoactive.

Achieving the long-term stability of perovskite solar cells is arguably the most important challenge required to enable widespread commercialization. Understanding the perovskite crystallization process and its direct impact on device stability is critical to achieving this goal. The commonly employed dimethyl-formamide/dimethyl-sulfoxide solvent preparation method results in a poor crystal quality and microstructure of the polycrystalline perovskite films. In this work, we introduce a high-temperature dimethyl-sulfoxide-free processing method that utilizes dimethylammonium chloride as an additive to control the perovskite intermediate precursor phases. By controlling the crystallization sequence, we tune the grain size, texturing, orientation (corner-up versus face-up) and crystallinity of the formamidinium (FA)/caesium (FA)yCs1–yPb(IxBr1–x)3 perovskite system. A population of encapsulated devices showed improved …

Despite the well-established defect tolerance of metal halide perovskites (MHPs), there are multiple sources of defects in MHPs, such as grain boundaries in thin films, colloidal nanocrystal surfaces, and a heterointerface formed with the charge-transport layer, all of which play a crucial role in determining the efficiency and stability of light-emitting diodes (LEDs). Defect passivation strategies have become essential tools for improving device performance. Here, we analyzed and correlated the origins of the defects in MHPs to their influence on the optical and charge-carrier transport properties and systematically reviewed mechanistic principles of promising passivation strategies to either eliminate or suppress various defects that undermine the potential of perovskite LEDs. Several challenges and prospects for the future development of MHP LEDs have been identified. This review could provide a valuable reference …

Perovskite solar cells represent an emerging and highly promising renewable energy technology. However, the most efficient perovskite solar cells critically depend on the use of lead. This represents a possible environmental concern potentially limiting the technologies’ commercialization. Here, we demonstrate a facile recycling process for PbI2, the most common lead-based precursor in perovskite absorber material. The process uses only hot water to effectively extract lead from synthetic precursor mixes, plastic- and glass-based perovskites (92.6 – 100% efficiency after two extractions). When the hot extractant is cooled, crystalline PbI2 in high purity (> 95.9%) precipitated with a high yield: from glass-based perovskites, the first cycle of extraction / precipitation was sufficient to recover 94.4 ± 5.6% of Pb, whereas a second cycle yielded another 10.0 ± 5.2% Pb, making the recovery quantitative. The solid extraction …

XDXWNHPWWKGTKO-UHFFFAOYSA-N 207739-72-8 Chemical compound C1= CC (OC)= CC= C1N (C= 1C= C2C3 (C4= CC (= CC= C4C2= CC= 1) N (C= 1C= CC (OC)= CC= 1) C= 1C= CC (OC)= CC= 1) C1= CC (= CC= C1C1= CC= C (C= C13) N (C= 1C= CC (OC)= CC= 1) C= 1C= CC (OC)= CC= 1) N (C= 1C= CC (OC)= CC= 1) C= 1C= CC (OC)= CC= 1) C1= CC= C (OC) C= C1 XDXWNHPWWKGTKO-UHFFFAOYSA-N 0.000 description 6

A multi-junction photovoltaic device comprising a layer of metal oxynitride between a first sub-cell and a second sub-cell is disclosed, the first sub-cell having a layer comprising a perovskite light absorber material. In addition, a method of manufacturing said multi junction photovoltaic device is disclosed. The metal oxynitride is preferably titanium oxynitride. Advantageously, the device may be produced in a simple, fast, consistent and inexpensive manner, whilst the properties of the titanium oxynitride layer may be tuned to avoid the occurrence of local shunt paths and to reduce reflection losses.

Ultranarrow bandwidth single-photon sources operating at room-temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud based quantum information processing networks, and quantum metrology. Here we show a room-temperature ultranarrow bandwidth single-photon source generating polarised photons at a rate of 5MHz based on an inorganic CsPbI3 perovskite quantum dot embedded in a tunable open-access optical microcavity. When coupled to an optical cavity mode, the quantum dot room-temperature emission becomes single-mode and the spectrum narrows down to just 1 nm. The low numerical aperture of the optical cavities enables efficient collection of high-purity single-mode single-photon emission at room-temperature, offering promising performance for photonic and quantum technology applications. We measure 94% pure single-photon emission into a single-mode under pulsed and continuous-wave (CW) excitation.

Mobile ions play a significant role in perovskite photovoltaics (PV), yet their impact on the overall performance and stability of tandem solar cells (TSCs) remains largely unexplored. Moreover, the effects of hysteresis in the current-voltage (JV) characteristic and ionic field screening are usually not considered to be a major problem anymore in high-performance tandem cells due to the introduction of comparatively stable and well-performing pin-type perovskite cells. This conclusion is based on the established practice of using a relatively slow JV scanning rate for the characterization of these devices. Here, based on recent work,[1-4] I will present a comprehensive study that combines an experimental analysis of ionic losses in Si/perovskite and all-perovskite TSCs during device aging with drift-diffusion simulations. Our findings demonstrate that mobile ions have a significant influence on the hysteresis of both …

The use of layered, 2D perovskites can improve the stability of metal halide perovskite thin films and devices. However, the charge carrier transport properties in layered perovskites are still not fully understood. Here, the sum of the electron and hole mobilities (Σμ) in thin films of the 2D perovskite PEA2PbI4, through transient electronically contacted nanosecond‐to‐millisecond photoconductivity measurements, which are sensitive to long‐time, long‐range (micrometer length scale) transport processes is investigated. After careful analysis, accounting for both early‐time recombination and the evolution of the exciton‐to‐free‐carrier population, a long‐range mobility of 8.0 +/− 0.6 cm2 (V s)–1, which is ten times greater than the long‐range mobility of a comparable 3D material FA0.9Cs0.1PbI3 is determined. These values are compared to ultra‐fast transient time‐resolved THz photoconductivity measurements, which …

We report process improvements for the fabrication of single-walled carbon nanotube ethylene-vinyl acetate transparent conductive films. CNT: EVA films demonstrate high resilience against folding and can replace the external dopant in a spiro-OMeTAD based hole selective contact of nip perovskite solar cells achieving a steady-state efficiency of 16.3%. The adapted process is fully scalable, and compared to previous reports (Mazzotta et al., 2018) lowers the material cost dramatically and improves DC to optical conductivity ratio by two orders of magnitude to σ d c/σ o p= 3. 6 for pristine and σ d c/σ o p= 15 for chemically doped films. We analyse the microstructure of our films via small angle neutron scattering and find a positive correlation between the long range packing density of the CNT: EVA films and the σ d c/σ o p performance. Increasing monomer ratio and chain length of the EVA polymer improves …

As perovskite-based photovoltaics near commercialization, it is imperative to develop industrial-scale defect-passivation techniques. Vapor deposition is a solvent-free fabrication technique that is widely implemented in industry and can be used to fabricate metal-halide perovskite thin films. We demonstrate markably improved growth and optoelectronic properties for vapor-deposited [CH(NH2)2]0.83Cs0.17PbI3 perovskite solar cells by partially substituting PbI2 for PbCl2 as the inorganic precursor. We find the partial substitution of PbI2 for PbCl2 enhances photoluminescence lifetimes from 5.6 ns to over 100 ns, photoluminescence quantum yields by more than an order of magnitude, and charge-carrier mobility from 46 cm2/(V s) to 56 cm2/(V s). This results in improved solar-cell power conversion efficiency, from 16.4% to 19.3% for the devices employing perovskite films deposited with 20% substitution of PbI2 for …

The present invention relates to a semiconductor device comprising a semiconducting material, wherein the semi conducting material comprises a halometallate compound comprising:(a) cesium;(b) palladium; and (c) one or more halide anions [X]. The invention also relates to a layer comprising the semiconducting material. The invention fur ther relates to a process for producing a halometallate compound of formula (IV):[A] 2 [M'][X]., which process uses a H [X] and a compound comprising a sulfoxide group.

The present invention relates to an optoelectronic device comprising:(a) a substrate comprising at least one first electrode, which at least one first electrode comprises a first electrode material, and at least one second electrode, which at least one second electrode comprises a second electrode material; and (b) a photoactive material disposed on the substrate, which photoactive material is in contact with the at least one first electrode and the at least one second electrode, wherein the substrate comprises: a layer of the first electrode material; and, disposed on the layer of the first electrode material, a layer of an insulating material, which layer of an insulating material partially covers the layer of the first electrode material; and, disposed on the layer of the insulating material, the second electrode material, and wherein the photoactive material comprises a crystalline compound, which crystalline compound comprises …

We employ terahertz radiation to investigate the impact of phase segregation on the charge-carrier dynamics and transport properties of mixed halide perovskite films. We reveal negligible impact on charge-carrier mobilities, and preservation of Drude-like transport. We demonstrate enhanced lattice anharmonicity that underlines the ionic migration mechanisms. We show how minimal structural transformations have a dramatic effect on the charge-carrier dynamics as a result of charge funnelling.

Vacuum deposition is a solvent-free method suitable for growing thin films of metal halide perovskite (MHP) semiconductors. However, most reports of high-efficiency solar cells based on such vacuum-deposited MHP films incorporate solution-processed hole transport layers (HTLs), thereby complicating prospects of industrial upscaling and potentially affecting the overall device stability. In this work, we investigate organometallic copper phthalocyanine (CuPc) and zinc phthalocyanine (ZnPc) as alternative, low-cost, and durable HTLs in all-vacuum-deposited solvent-free formamidinium-cesium lead triodide [CH(NH2)2]0.83Cs0.17PbI3 (FACsPbI3) perovskite solar cells. We elucidate that the CuPc HTL, when employed in an “inverted” p–i–n solar cell configuration, attains a solar-to-electrical power conversion efficiency of up to 13.9%. Importantly, unencapsulated devices as large as 1 cm2 exhibited excellent long …

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Halogen mixing in lead-halide perovskites is an effective route for tuning the band gap in light emission and multijunction solar cell applications. Here we report the effect of halogen mixing on the optoelectronic properties of lead-halide perovskites from theory and experiment. We applied the virtual crystal approximation within density functional theory, the GW approximation, and the Bethe–Salpeter equation to calculate structural, vibrational, and optoelectronic properties for a series of mixed halide perovskites. We separately perform spectroscopic measurements of these properties and analyze the impact of halogen mixing on quasiparticle band gaps, effective masses, absorption coefficients, charge-carrier mobilities, and exciton binding energies. Our joint theoretical–experimental study demonstrates that iodide–bromide mixed-halide perovskites can be modeled as homovalent alloys, and local structural …

The invention provides an optoelectronic device compris ing:(i) a porous dielectric scaffold material; and (ii) a semiconductor having a band gap of less than or equal to 3.0 eV, in contact with the scaffold material. Typically the semiconductor, which may be a perovskite, is disposed on the surface of the porous dielectric scaffold material, so that it is supported on the surfaces of pores within the scaffold. In one embodiment, the optoelectronic device is an opto electronic device which comprises a photoactive layer, wherein the photo-active layer comprises:(a) said porous dielectric scaffold material;(b) said semiconductor; and (c) a charge transporting material. The invention further pro vides the use, as a photoactive material in an optoelectronic device, of:(i) a porous dielectric scaffold material; and (ii) a semi-conductor having a band gap of less than or equal to (Continued)

The performance of single-junction solar cells in thermal equilibrium is limited by the conversion of excess photon energy to heat through hot-carrier—phonon interactions [1]. However, hot-carrier photovoltaic devices, a future-generation technology for solar power conversion, could overcome this limitation. If the temperature of the charge-carrier gas is elevated compared to that of the crystal lattice, extraction of the photoexcited charge carriers with above-bandgap energies may be possible, boosting the energy conversion efficiency. Metal-halide perovskites, and in particular tin-iodide perovskite semiconductors, have been investigated in recent years as potential candidates for such technology, owing to the long hot-carrier cooling times observed in these materials [2]. Reported nanosecond-long cooling dynamics could allow for efficient extraction of hot carriers high above the bandgap, pushing the efficiency limit …

The invention relates to a process for chemically etching the surface of a metal halide perovskite, the process comprising treating the metal halide perovskite with one or more multidentate ligands, wherein the one or more multidentate ligands comprise an organic compound or a salt thereof, which organic compound comprises three or more binding groups. A chemically etched metal halide perovskite, a process for producing a semiconductor device, a composition and a semiconductor device are also described.

Successful manipulation of halide perovskite surfaces is typically achieved via the interactions between modulators and perovskites. Herein, it is demonstrated that a strong‐interaction surface modulator is beneficial to reduce interfacial recombination losses in inverted (p‐i‐n) perovskite solar cells (IPSCs). Two organic ammonium salts are investigated, consisting of 4‐hydroxyphenethylammonium iodide and 2‐thiopheneethylammonium iodide (2‐TEAI). Without thermal annealing, these two modulators can recover the photoluminescence quantum yield of the neat perovskite film in contact with fullerene electron transport layer (ETL). Compared to the hydroxyl‐functionalized phenethylammonium moiety, the thienylammonium facilitates the formation of a quasi‐2D structure onto the perovskite. Density functional theory and quasi‐Fermi level splitting calculations reveal that the 2‐TEAI has a stronger interaction with …

2D halide perovskites are among intensely studied materials platforms profiting from solution-based growth and chemical flexibility. They feature exceptionally strong interactions among electronic, optical, as well as vibrational excitations and hold a great potential for future optoelectronic applications. A key feature for these materials is the occurrence of structural phase transitions that can impact their functional properties, including the electronic band gap and optical response dominated by excitons. However, to what extent the phase transitions in 2D perovskites alter the fundamental exciton properties remains barely explored so far. Here, we study the influence of the phase transition on both exciton binding energy and exciton diffusion, demonstrating their robust nature across the phase transition. These findings are unexpected in view of the associated substantial changes of the free carrier masses, strongly …

Direct bandgap perovskite and indirect bandgap Si, which form the two active layers in a tandem solar cell configuration, have different optoelectronic properties and thicknesses. The charge-carrier dynamics of the two-terminal perovskite-on-Si tandem solar cell in response to a supercontinuum light pulse is studied using transient photocurrent (TPC) measurements. Spectral dependence of TPC lifetime is observed and can be classified into two distinct timescales based on their respective carrier generation regions. The faster timescale ($500 ns) corresponding to the spectral window (300–750nm) represents the top-perovskite sub-cell, while the slower timescale regime of $25 ls corresponds to the bottom-Si sub-cell (> 700 nm). Additionally, under light-bias conditions, the transient carrier dynamics of the perovskite sub-cell is observed to be coupled with that of the Si sub-cell. A sharp crossover from the fast …

Having captivated the research community with simple fabrication processes and staggering device efficiencies, perovskite-based optoelectronics are already on the way to commercialization. However, one potential obstacle to this commercialization is the almost exclusive use of toxic, highly coordinating, high boiling point solvents to make perovskite precursor inks. Herein, we demonstrate that nonpolar organic solvents, such as toluene, can be combined with butylamine to form an effective solvent for alkylammonium-based perovskites. Beyond providing broader solvent choice, our finding opens the possibility of blending perovskite inks with a wide range of previously incompatible materials, such as organic molecules, polymers, nanocrystals, and structure-directing agents. As a demonstration, using this solvent, we blend the perovskite ink with 6,6-phenyl-C-61-butyric acid methyl ester and show improved …

Despite the incredible progress made, the highest efficiency perovskite solar cells are still restricted to small areas (<1 cm2). In large part, this stems from a poor understanding of the widespread spatial heterogeneity in devices. Conventional techniques to assess heterogeneities can be time consuming, operate only at microscopic length scales, and demand specialized equipment. We overcome these limitations by using luminescence imaging to reveal large, millimeter-scale heterogeneities in the inferred electronic properties. We determine spatially resolved maps of “charge collection quality”, measured using the ratio of photoluminescence intensity at open and short circuit. We apply these methods to quantify the inhomogeneities introduced by a wide range of transport layers, thereby ranking them by suitability for upscaling. We reveal that top-contacting transport layers are the dominant source of heterogeneity …

The invention provides an optoelectronic device comprising a mixed-anion perovskite, wherein the mixed-anion perovskite comprises two or more different anions selected from halide anions and chalcogenide anions. The invention further provides a mixed-halide perovskite of the formula (I)[A][B][X] 3 wherein:[A] is at least one organic cation;[B] is at least one divalent metal cation; and [X] is said two or more different halide anions. In another aspect, the invention provides the use of a mixed-anion perovskite as a sensitizer in an optoelectronic device, wherein the mixed-anion perovskite comprises two or more different anions selected from halide anions and chalcogenide anions. The invention also provides a photosensitizing material for an optoelectronic device comprising a mixed-anion perovskite wherein the mixed-anion perovskite comprises two or more different anions selected from halide anions and …

Ultra narrow bandwidth single-photon sources operating at room temperature are of vital importance for viable optical quantum technologies at scale, including quantum key distribution, cloud-based quantum information processing networks, and quantum metrology. Here we show a room-temperature single-photon source generating polarised photons at a rate of 5 MHz based on an inorganic CsPbI3 perovskite quantum dot embedded in a tunable open optical microcavity. When coupled to the mode of the optical cavity, the quantum dot room-temperature emission becomes single-mode and the spectrum narrows down to just∼ 1 nm. The excellent directionality of the optical modes enables high single-mode collection at RT, offering promising performance for photonic and quantum technology applications. We measure 94% single-photon purity under pulsed and continuous-wave (CW) excitation.

Tainter_Joule_data. opj-Origin project file containing data underlying figures presented in the article. Original figures are presented and named as presented in the paper, as well as corresponding worksheets containing raw and smoothed data.Detailed origin worksheet breakdown:" Fig2Adata" and" Fig2Bdata"-data underlying scanning photocurrent measurements presented in figure 2, presenting position of measurement (relative to junction) and normalised current or characteristic rise time." trplGlass, trplNiOx, trplSnO2"-time-resolved photoluminescence data performed on perovskites films deposited over glass, NiOx, and SnO2, respectively. Data for time delay and number of counts is presented, which is presented in figure 3A." Fig3Boutput"-modeled charge density vs position as presented in figure 3b, details of model in the supporting information." Fig4Cdata"-forward and reverse JV data given in V and mAcm-2 which is presented in Figures 4C and S8." Fig4Ddata"-scanning photocurrent and scanning photoluminescence microscopy data as presented in figure 4D. Data is presented for position of measurement and photocurrent amplitude and PL intensity (norm.)." FigS2data"-Photoluminescence spectra obtained over the two materials in the active area of a device. Data is presented as wavelength vs counts (au)." FigS9data"-Peak short-circuit currents obtained for varying device pitch distance.

The invention relates to an optoelectronic device comprising:(a) a layer comprising a crystalline A/M/X material, wherein the crystalline A/M/X material comprises a compound of formula:[A] a [M] b [X] c wherein:[A] comprises one or more A cations;[M] comprises one or more M cations which are metal or metalloid cations;[X] comprises one or more X anions; a is a number from 1 to 6; b is a number from 1 to 6; and c is a number from 1 to 18; and (b) an ionic liquid which is a salt comprising an organic cation and a counter anion, wherein the organic cation is present within the layer comprising the crystalline A/M/X material. The invention also relates to processes for producing an ionic liquid-modified film of a crystalline A/M/X material and a process for producing an optoelectronic device comprising an ionic-liquid modified film of a crystalline A/M/X material.

The invention provides a process for producing a passivated semiconductor, which process comprises treating a semiconductor with a passivating agent, wherein: the semiconductor comprises a crystalline compound comprising:(i) one or more first cations (A);(ii) one or more metal cations (M); and (iii) one or more anions (X); and the passivating agent comprises a compound comprising an oxygen-oxygen single bond. A composition and the use of a passivating agent are also provided.

Efficient and stable perovskite solar cells rely on the use of Pb species potentially challenging the technologies’ commercialisation. In this study, the fate of Pb derived from two common perovskite precursors is compared to cationic lead in soil-water microcosm experiments under various biogeochemical conditions. The rapid and efficient removal of Pb from the aqueous phase is demonstrated by inductively coupled plasma mass spectrometry. Sequential soil extraction results reveal that a substantial amount of Pb is associated with immobile fractions, whereas a minor proportion of Pb may become available again in the long term, when oxygen is depleted (e.g. during water logging). X-ray absorption spectroscopy results reveal that the sorption of Pb on mineral phases represents the most likely sequestration mechanism. The obtained results suggest that the availability of leached Pb from perovskite solar cells is …

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 …

We show that adding ethylenediamine (EDA) to perovskite precursor solutions improves the photovoltaic device performance and material stability of high-bromide-content, methylammonium-free, formamidinium cesium lead halide perovskites FA1–xCsxPb(I1–yBry)3, which are currently of interest for perovskite-on-Si tandem solar cells. Using spectroscopy and hyperspectral microscopy, we show that the additive improves film homogeneity and suppresses the phase instability that is ubiquitous in high-Br perovskite formulations, producing films that remain stable for over 100 days in ambient conditions. With the addition of 1 mol % EDA, we demonstrate 1.69 eV-gap perovskite single-junction p-i-n devices with a VOC of 1.22 V and a champion maximum-power-point-tracked power conversion efficiency of 18.8%, comparable to the best reported methylammonium-free perovskites. Using nuclear magnetic resonance …

Challenges in fabricating all-perovskite tandem solar cells as modules rather than as single-junction configurations include growing high-quality wide-bandgap perovskites and mitigating irreversible degradation caused by halide and metal interdiffusion at the interconnecting contacts. We demonstrate efficient all-perovskite tandem solar modules using scalable fabrication techniques. By systematically tuning the cesium ratio of a methylammonium-free 1.8–electron volt mixed-halide perovskite, we improve the homogeneity of crystallization for blade-coated films over large areas. An electrically conductive conformal “diffusion barrier” is introduced between interconnecting subcells to improve the power conversion efficiency (PCE) and stability of all-perovskite tandem solar modules. Our tandem modules achieve a certified PCE of 21.7% with an aperture area of 20 square centimeters and retain 75% of their initial …

Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady‐state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via “fast‐hysteresis” measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (1000 V s−1). The “ion‐free” PCE is between 1% and 3% higher than the steady‐state PCE, demonstrating the importance of ion‐induced losses, even in cells with low levels of hysteresis at typical scan speeds (100 mV s−1). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the …

Charge carrier mobility is a fundamental property of semiconductor materials that governs many electronic device characteristics. For metal halide perovskites, a wide range of charge carrier mobilities have been reported using different techniques. Mobilities are often estimated via transient methods assuming an initial charge carrier population after pulsed photoexcitation and measurement of photoconductivity via non-contact or contact techniques. For nanosecond to millisecond transient methods, early-time recombination and exciton-to-free-carrier ratio hinder accurate determination of free-carrier population after photoexcitation. By considering both effects, we estimate long-range charge carrier mobilities over a wide range of photoexcitation densities via transient photoconductivity measurements. We determine long-range mobilities for FA0.83Cs0.17Pb(I0.9Br0.1)3, (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 …