Double-side 2D/3D heterojunctions for inverted perovskite solar cells.

Defects at the top and bottom interfaces of three-dimensional (3D) perovskite photoabsorbers diminish the performance and operational stability of perovskite solar cells owing to charge recombination, ion migration and electric-field inhomogeneities1-5. Here we demonstrate that long alkyl amine ligands can generate near-phase-pure 2D perovskites at the top and bottom 3D perovskite interfaces and effectively resolve these issues. At the rear-contact side, we find that the alkyl amine ligand strengthens the interactions with the substrate through acid-base reactions with the phosphonic acid group from the organic hole-transporting self-assembled monolayer molecule, thus regulating the 2D perovskite formation. With this, inverted perovskite solar cells with double-side 2D/3D heterojunctions achieved a power conversion efficiency of 25.6% (certified 25.0%), retaining 95% of their initial power conversion efficiency after 1,000 h of 1-sun illumination at 85 °C in air.

Two-dimensional Perovskitoids Enhance Stability in Perovskite Solar Cells.

Two-dimensional (2D)/three-dimensional (3D) perovskite heterostructures have played a key role in advancing the performance of perovskite solar cells (PSCs)1,2. However, the migration of cations between 2D and 3D layers results in the disruption of octahedral networks that leads to degradation in performance over time3,4. We hypothesized that perovskitoids, with robust organic-inorganic networks enabled by edge- and face-sharing, could impede ion migration. We explored a set of perovskitoids of varying dimensionality, and found that cation migration within perovskitoid/perovskite heterostructures was suppressed compared to the 2D/3D perovskite case. Increasing the dimensionality of perovskitoids improves charge transport when they are interfaced with 3D perovskite surfaces - this the result of enhanced octahedral connectivity and out-of-plane orientation. The 2D perovskitoid (A6BfP)8Pb7I22 (A6BfP: N-aminohexyl-benz[f]-phthalimide) provides efficient passivation of perovskite surfaces and enables uniform large-area perovskite films. Devices based on perovskitoid/perovskite heterostructures achieve a certified quasi-steady-state power conversion efficiency of 24.6% for centimeter-area PSCs. We removed the fragile hole transport layers and showed stable operation of the underlying perovskitoid/perovskite heterostructure at 85°C for 1,250 hours for encapsulated large-area devices in an air ambient.

Enhanced optoelectronic coupling for perovskite/silicon tandem solar cells.

Monolithic perovskite/silicon tandem solar cells are of great appeal as they promise high power conversion efficiencies (PCEs) at affordable cost. In state-of-the-art tandems, the perovskite top cell is electrically coupled to a silicon heterojunction bottom cell by means of a self-assembled monolayer (SAM), anchored on a transparent conductive oxide (TCO), which enables efficient charge transfer between the subcells1-3. Yet reproducible, high-performance tandem solar cells require energetically homogeneous SAM coverage, which remains challenging, especially on textured silicon bottom cells. Here, we resolve this issue by using ultrathin (5-nm) amorphous indium zinc oxide (IZO) as the interconnecting TCO, exploiting its high surface-potential homogeneity resulting from the absence of crystal grains and higher density of SAM anchoring sites when compared with commonly used crystalline TCOs. Combined with optical enhancements through equally thin IZO rear electrodes and improved front contact stacks, an independently certified PCE of 32.5% was obtained, which ranks among the highest for perovskite/silicon tandems. Our ultrathin transparent contact approach reduces indium consumption by approximately 80%, which is of importance to sustainable photovoltaics manufacturing4.

Regulating surface potential maximizes voltage in all-perovskite tandems.

The open-circuit voltage (VOC) deficit in perovskite solar cells is greater in wide-bandgap (over 1.7 eV) cells than in perovskites of roughly 1.5 eV (refs. 1,2). Quasi-Fermi-level-splitting measurements show VOC-limiting recombination at the electron-transport-layer contact3-5. This, we find, stems from inhomogeneous surface potential and poor perovskite-electron transport layer energetic alignment. Common monoammonium surface treatments fail to address this; as an alternative, we introduce diammonium molecules to modify perovskite surface states and achieve a more uniform spatial distribution of surface potential. Using 1,3-propane diammonium, quasi-Fermi-level splitting increases by 90 meV, enabling 1.79 eV perovskite solar cells with a certified 1.33 V VOC and over 19% power conversion efficiency (PCE). Incorporating this layer into a monolithic all-perovskite tandem, we report a record VOC of 2.19 V (89% of the detailed balance VOC limit) and over 27% PCE (26.3% certified quasi-steady state). These tandems retained more than 86% of their initial PCE after 500 h of operation.

Suppressed phase segregation for triple-junction perovskite solar cells.

The tunable bandgaps and facile fabrication of perovskites make them attractive for multi-junction photovoltaics1,2. However, light-induced phase segregation limits their efficiency and stability3-5: this occurs in wide-bandgap (>1.65 electron volts) iodide/bromide mixed perovskite absorbers, and becomes even more acute in the top cells of triple-junction solar photovoltaics that require a fully 2.0-electron-volt bandgap absorber2,6. Here we report that lattice distortion in iodide/bromide mixed perovskites is correlated with the suppression of phase segregation, generating an increased ion-migration energy barrier arising from the decreased average interatomic distance between the A-site cation and iodide. Using an approximately 2.0-electron-volt rubidium/caesium mixed-cation inorganic perovskite with large lattice distortion in the top subcell, we fabricated all-perovskite triple-junction solar cells and achieved an efficiency of 24.3 per cent (23.3 per cent certified quasi-steady-state efficiency) with an open-circuit voltage of 3.21 volts. This is, to our knowledge, the first reported certified efficiency for perovskite-based triple-junction solar cells. The triple-junction devices retain 80 per cent of their initial efficiency following 420 hours of operation at the maximum power point.

Oxygen Vacancy Mediation in SnO2 Electron Transport Layers Enables Efficient, Stable, and Scalable Perovskite Solar Cells.

Previous findings have suggested a close association between oxygen vacancies in SnO2 and charge carrier recombination as well as perovskite decomposition at the perovskite/SnO2 interface. Underlying the fundamental mechanism holds great significance in achieving a more favorable balance between the efficiency and stability. In this study, we prepared three SnO2 samples with different oxygen vacancy concentrations and observed that a low oxygen vacancy concentration is conducive to long-term device stability. Iodide ions were observed to easily diffuse into regions with high oxygen vacancies, thereby speeding up the deprotonation of FAI, as made evident by the detection of the decomposition product formamide. In contrast, a high oxygen vacancy concentration in SnO2 could prevent hole injection, leading to a decrease in interfacial recombination losses. To suppress this decomposition reaction and address the trade-off, we designed a bilayer SnO2 structure to ensure highly efficient carrier transport still while maintaining a chemically inert surface. As a result, an enhanced efficiency of 25.06% (certified at 24.55% with an active area of 0.09 cm2 under fast scan) was achieved, and the extended operational stability maintained 90% of their original efficiency (24.52%) after continuous operation for nearly 2000 h. Additionally, perovskite submodules with an active area of 14 cm2 were successfully assembled with a PCE of up to 22.96% (20.09% with an aperture area).

Molecular Orientation Regulation of Hole Transport Semicrystalline-Polymer Enables High-Performance Carbon-Electrode Perovskite Solar Cells.

Carbon-based perovskite solar cells (PSCs) coupled with solution-processed hole transport layers (HTLs) have shown potential owing to their combination of low cost and high performance. However, the commonly used poly(3-hexylthiophene) (P3HT) semicrystalline-polymer HTL dominantly shows edge-on molecular orientation, in which the alkyl side chains directly contact the perovskite layer, resulting in an electronically poor contact at the perovskite/P3HT interface. The study adopts a synergetic strategy comprising of additive and solvent engineering to transfer the edge-on molecular orientation of P3HT HTL into 3D molecular orientation. The target P3HT HTL possesses improved charge transport as well as enhanced moisture-repelling capability. Moreover, energy level alignment between target P3HT HTL and perovskite layer is realized. As a result, the champion devices with small (0.04 cm2) and larger areas (1 cm2) deliver notable efficiencies of 20.55% and 18.32%, respectively, which are among the highest efficiency of carbon-electrode PSCs.

Solar-Powered Gram-Scale Ammonia Production from Nitrate.

The photoelectrochemical (PEC) method has the potential to be an attractive route for converting and storing solar energy as chemical bonds. In this study, a maximum NH3 production yield of 1.01 g L-1 with a solar-to-ammonia conversion efficiency of 8.17% through the photovoltaic electrocatalytic (PV-EC) nitrate (NO3 -) reduction reaction (NO3 -RR) is achieved, using silicon heterojunction solar cell technology. Additionally, the effect of tuning the operation potential of the PV-EC system and its influence on product selectivity are systematically investigated. By using this unique external resistance tuning approach in the PV-EC system, ammonia production through nitrate reduction performance from 96 to 360 mg L-1 is enhanced, a four-fold increase. Furthermore, the NH3 is extracted as NH4Cl powder using acid stripping, which is essential for storing chemical energy. This work demonstrates the possibility of tuning product selectivity in PV-EC systems, with prospects toward pilot scale on value-added product synthesis.

Intrinsic efficiency limits in low-bandgap non-fullerene acceptor organic solar cells.

In bulk heterojunction (BHJ) organic solar cells (OSCs) both the electron affinity (EA) and ionization energy (IE) offsets at the donor-acceptor interface should equally control exciton dissociation. Here, we demonstrate that in low-bandgap non-fullerene acceptor (NFA) BHJs ultrafast donor-to-acceptor energy transfer precedes hole transfer from the acceptor to the donor and thus renders the EA offset virtually unimportant. Moreover, sizeable bulk IE offsets of about 0.5 eV are needed for efficient charge transfer and high internal quantum efficiencies, since energy level bending at the donor-NFA interface caused by the acceptors' quadrupole moments prevents efficient exciton-to-charge-transfer state conversion at low IE offsets. The same bending, however, is the origin of the barrier-less charge transfer state to free charge conversion. Our results provide a comprehensive picture of the photophysics of NFA-based blends, and show that sizeable bulk IE offsets are essential to design efficient BHJ OSCs based on low-bandgap NFAs.

Acene Ring Size Optimization in Fused Lactam Polymers Enabling High n-Type Organic Thermoelectric Performance.

Three n-type fused lactam semiconducting polymers were synthesized for thermoelectric and transistor applications via a cheap, highly atom-efficient, and nontoxic transition-metal free aldol polycondensation. Energy level analysis of the three polymers demonstrated that reducing the central acene core size from two anthracenes (A-A), to mixed naphthalene-anthracene (A-N), and two naphthalene cores (N-N) resulted in progressively larger electron affinities, thereby suggesting an increasingly more favorable and efficient solution doping process when employing 4-(2,3-dihydro-1,3-dimethyl-1H-benzimidazol-2-yl)-N,N-dimethylbenzenamine (N-DMBI) as the dopant. Meanwhile, organic field effect transistor (OFET) mobility data showed the N-N and A-N polymers to feature the highest charge carrier mobilities, further highlighting the benefits of aryl core contraction to the electronic performance of the materials. Ultimately, the combination of these two factors resulted in N-N, A-N, and A-A to display power factors (PFs) of 3.2 µW m-1 K-2, 1.6 µW m-1 K-2, and 0.3 µW m-1 K-2, respectively, when doped with N-DMBI, whereby the PFs recorded for N-N and A-N are among the highest reported in the literature for n-type polymers. Importantly, the results reported in this study highlight that modulating the size of the central acene ring is a highly effective molecular design strategy to optimize the thermoelectric performance of conjugated polymers, thus also providing new insights into the molecular design guidelines for the next generation of high-performance n-type materials for thermoelectric applications.

CH(3)NH(3)PbI(3) perovskite / silicon tandem solar cells: characterization based optical simulations.

In this study we analyze and discuss the optical properties of various tandem architectures: mechanically stacked (four-terminal) and monolithically integrated (two-terminal) tandem devices, consisting of a methyl ammonium lead triiodide (CH(3)NH(3)PbI(3)) perovskite top solar cell and a crystalline silicon bottom solar cell. We provide layer thickness optimization guidelines and give estimates of the maximum tandem efficiencies based on state-of-the-art sub cells. We use experimental complex refractive index spectra for all involved materials as input data for an in-house developed optical simulator CROWM. Our characterization based simulations forecast that with optimized layer thicknesses the four-terminal configuration enables efficiencies over 30%, well above the current single-junction crystalline silicon cell record of 25.6%. Efficiencies over 30% can also be achieved with a two-terminal monolithic integration of the sub-cells, combined with proper selection of layer thicknesses.

Organic-inorganic halide perovskite/crystalline silicon four-terminal tandem solar cells.

Tandem solar cells constructed from a crystalline silicon (c-Si) bottom cell and a low-cost top cell offer a promising way to ensure long-term price reductions of photovoltaic modules. We present a four-terminal tandem solar cell consisting of a methyl ammonium lead triiodide (CH3NH3PbI3) top cell and a c-Si heterojunction bottom cell. The CH3NH3PbI3 top cell exhibits broad-band transparency owing to its design free of metallic components and yields a transmittance of >55% in the near-infrared spectral region. This allows the generation of a short-circuit current density of 13.7 mA cm(-2) in the bottom cell. The four-terminal tandem solar cell yields an efficiency of 13.4% (top cell: 6.2%, bottom cell: 7.2%), which is a gain of 1.8%abs with respect to the reference single-junction CH3NH3PbI3 solar cell with metal back contact. We employ the four-terminal tandem solar cell for a detailed investigation of the optical losses and to derive guidelines for further efficiency improvements. Based on a power loss analysis, we estimate that tandem efficiencies of ∼28% are attainable using an optically optimized system based on current technology, whereas a fully optimized, ultimate device with matched current could yield up to 31.6%.

Radiative cooling for vertical solar panels.

Radiative cooling presents a method for reducing the operational temperature of solar panels without additional energy consumption. However, its applicability to PV modules has been limited by the thermal properties of existing materials. To overcome these challenges, we introduce a V-shaped design that enhances cooling in vertical PV modules by effectively harnessing thermal radiation from both the front and rear sides, resulting in a substantial temperature reduction of 10.6°C under 1 sun illumination in controlled laboratory conditions. Field tests conducted in warm and humid conditions, specifically in Thuwal, Saudi Arabia, demonstrate a remarkable 15% increase in efficiency while maintaining an operating temperature 0.2°C lower than that of conventional horizontal PV modules, corresponding to a significant 16.8% increase in power output. Our innovative V-shaped design offers a promising thermal strategy suitable for diverse climates, contributing to improved performance and reduced module temperatures, thereby supporting the global pursuit of carbon neutrality.

Impact of the TCO Microstructure on the Electronic Properties of Carbazole-Based Self-Assembled Monolayers.

Carbazole-based self-assembled monolayers (PACz-SAMs), anchored via their phosphonic acid group on a transparent conductive oxide (TCO), have demonstrated excellent performance as hole-selective layers in perovskite/silicon tandem solar cells. Yet, whereas different PACz-SAMs have been explored, the role of the TCO, and specifically its microstructure, on the hole transport properties of the TCO/PACz-SAMs stack has been largely overlooked. Here, we demonstrate that the TCO microstructure directly impacts the work function (WF) shift after SAM anchoring and is responsible for WF variations at the micro/nanoscale. Specifically, we studied Sn-doped In2O3 (ITO) substrates with amorphous and polycrystalline (featuring either nanoscale- or microscale-sized grains) microstructures before and after 2PACz-SAMs and NiOx/2PACz-SAMs anchoring. With this, we established a direct correlation between the ITO crystal grain orientation and 2PACz-SAMs local potential distribution, i.e., the WF. Importantly, these variations vanish for amorphous oxides (either in the form of amorphous ITO or when adding an amorphous NiOx buffer layer), where a homogeneous surface potential distribution is found. These findings highlight the importance of TCO microstructure tuning, to enable both high mobility and broadband transparent electrodes while ensuring uniform WF distribution upon application of hole transport SAMs, both critical for enhanced device performance.

Moisture-Resilient Perovskite Solar Cells for Enhanced Stability.

With the rapid rise in device performance of perovskite solar cells (PSCs), overcoming instabilities under outdoor operating conditions has become the most crucial obstacle toward their commercialization. Among stressors such as light, heat, voltage bias, and moisture, the latter is arguably the most critical, as it can decompose metal-halide perovskite (MHP) photoactive absorbers instantly through its hygroscopic components (organic cations and metal halides). In addition, most charge transport layers (CTLs) commonly employed in PSCs also degrade in the presence of water. Furthermore, photovoltaic module fabrication encompasses several steps, such as laser processing, subcell interconnection, and encapsulation, during which the device layers are exposed to the ambient atmosphere. Therefore, as a first step toward long-term stable perovskite photovoltaics, it is vital to engineer device materials toward maximizing moisture resilience, which can be accomplished by passivating the bulk of the MHP film, introducing passivation interlayers at the top contact, exploiting hydrophobic CTLs, and encapsulating finished devices with hydrophobic barrier layers, without jeopardizing device performance. Here, existing strategies for enhancing the performance stability of PSCs are reviewed and pathways toward moisture-resilient commercial perovskite devices are formulated.

Pathways toward commercial perovskite/silicon tandem photovoltaics.

Perovskite/silicon tandem solar cells offer a promising route to increase the power conversion efficiency of crystalline silicon (c-Si) solar cells beyond the theoretical single-junction limitations at an affordable cost. In the past decade, progress has been made toward the fabrication of highly efficient laboratory-scale tandems through a range of vacuum- and solution-based perovskite processing technologies onto various types of c-Si bottom cells. However, to become a commercial reality, the transition from laboratory to industrial fabrication will require appropriate, scalable input materials and manufacturing processes. In addition, perovskite/silicon tandem research needs to increasingly focus on stability, reliability, throughput of cell production and characterization, cell-to-module integration, and accurate field-performance prediction and evaluation. This Review discusses these aspects in view of contemporary solar cell manufacturing, offers insights into the possible pathways toward commercial perovskite/silicon tandem photovoltaics, and highlights research opportunities to realize this goal.

Capillary Manganese Halide Needle-Like Array Scintillator with Isolated Light Crosstalk for Micro-X-Ray Imaging.

The exacerbation of inherent light scattering with increasing scintillator thickness poses a major challenge for balancing the thickness-dependent spatial resolution and scintillation brightness in X-ray imaging scintillators. Herein, a thick pixelated needle-like array scintillator capable of micrometer resolution is fabricated via waveguide structure engineering. Specifically, this involves integrating a straightforward low-temperature melting process of manganese halide with an aluminum-clad capillary template. In this waveguide structure, the oriented scintillation photons propagate along the well-aligned scintillator and are confined within individual pixels by the aluminum reflective cladding, as substantiated from the comprehensive analysis including laser diffraction experiments. Consequently, thanks to isolated light-crosstalk channels and robust light output due to increased thickness, ultrahigh spatial resolutions of 60.8 and 51.7 lp mm-1 at a modulation transfer function (MTF) of 0.2 are achieved on 0.5 mm and even 1 mm thick scintillators, respectively, which both exceed the pore diameter of the capillary arrays' template (Φ = 10 µm). As far as it is known, these micrometer resolutions are among the highest reported metal halide scintillators and are never demonstrated on such thick scintillators. Here an avenue is presented to the demand for thick scintillators in high-resolution X-ray imaging across diverse scientific and practical fields.

Enhanced cation interaction in perovskites for efficient tandem solar cells with silicon.

To achieve the full potential of monolithic perovskite/silicon tandem solar cells, crystal defects and film inhomogeneities in the perovskite top cell must be minimized. We discuss the use of methylenediammonium dichloride as an additive to the perovskite precursor solution, resulting in the incorporation of in situ-formed tetrahydrotriazinium (THTZ-H+) into the perovskite lattice upon film crystallization. The cyclic nature of the THTZ-H+ cation enables a strong interaction with the lead octahedra of the perovskite lattice through the formation of hydrogen bonds with iodide in multiple directions. This structure improves the device power conversion efficiency (PCE) and phase stability of 1.68 electron volts perovskites under prolonged light and heat exposure under 1-sun illumination at 85°C. Monolithic perovskite/silicon tandems incorporating THTZ-H+ in the perovskite photo absorber reached a 33.7% independently certified PCE for a device area of 1 square centimeter.