Over 10% Efficient Sb2(S,Se)3 Solar Cells Enabled by CsI-Doping Strategy.

Antimony selenosulfide (Sb2(S,Se)3) is an emerging quasi-1D photovoltaic semiconductor with exceptional photoelectric properties. The low-symmetry chain structure contains complex defects and makes it difficult to improve electrical properties via doping method. This article reports a doping strategy to enhance the efficiency of Sb2(S,Se)3 solar cells by using alkali halide (CsI) as the hydrothermal reaction precursor. It is found that the Cs and I ions are effectively doped and atomically coordinate with Sb ions and S/Se ions. The CsI-doping Sb2(S,Se)3 absorbers exhibit enhanced grain morphologies and reduced trap densities. The consequential CsI-doping Sb2(S,Se)3 based solar cells demonstrate favorable band alignment, suppressed carrier recombination, and improved device performance. An efficiency as high as 10.05% under standard AM1.5 illumination irradiance is achieved. This precursor-based alkali halide doping strategy provides a useful guidance for high-efficiency antimony selenosulfide solar cells.

Flexible All-in-one Quasi-Solid-State Batteries Enabled by Low-water-content Hydrogel Films.

The high conductivities and good mechanical properties of hydrogel electrolyte films are critical for energy storage devices with high flexibility, fast redox kinetics, and long life. Herein, a low water content (6.63 wt%) hydrogel film is prepared, and a favorable environment is created, with an electrochemical stability window of 2.26 V and a high ionic conductivity of 2.6 mS cm-1 . The hydrogel film exhibits good folding ability, low in-plane swelling, and anti-freezing abilities. These properties are benefitted by immobilizing free water molecules on the abundant oxygenic groups of polymer fibers in the hydrogel film, offering a unique 3D channel to allow Li+ to quickly transport along the polymer network. Therefore, the hydrogel film-based all-in-one flexible cell exhibits stable cycling performance with a retention of 81.8% of the initial capacity after 500 cycles at room temperature and 66.2% of capacity retention at -30 °C. Furthermore, the full cell with high cathode loading (≈21 mg cm-2 ) exhibits a high areal capacity of 2.5 mAh cm-2 (≈119 mAh g-1 ). The overall merits of flexible all-in-one quasi-solid-state batteries demonstrate high potential to be used for power wearable electronics.

Large-Grain Spanning Monolayer Cu2 ZnSnSe4 Thin-Film Solar Cells Grown from Metal Precursor.

The persistent double layer structure whereby two layers with different properties form at the front and rear of absorbers is a critical challenge in the field of kesterite thin-film solar cells, which imposes additional nonradiative recombination in the quasi-neutral region and potential limitation to the transport of hole carriers. Herein, an effective model for growing monolayer CZTSe thin-films based on metal precursors with large grains spanning the whole film is developed. Voids and fine grain layer are avoided successfully by suppressing the formation of a Sn-rich liquid metal phase near Mo back contact during alloying, while grain coarsening is greatly promoted by enhancing mass transfer during grain growth. The desired morphology exhibits several encouraging features, including significantly reduced recombination in the quasi-neutral region that contributes to the large increase of short-circuit current, and a quasi-Ohmic back contact which is a prerequisite for high fill factor. Though this growth mode may introduce more interfacial defects which require further modification, the strategies demonstrated remove a primary obstacle toward higher efficiency kesterite solar cells, and can be applicable to morphology control with other emerging chalcogenide thin films.

Encapsulation of Sulfur into N-Doped Porous Carbon Cages by a Facile, Template-Free Method for Stable Lithium-Sulfur Cathode.

Lithium-sulfur (Li-S) batteries with a high energy density and long lifespan are considered as promising candidates for next-generation electrochemical energy-storage devices. However, the sluggish redox kinetics of electrochemistry and high solubility of polysulfide during cycling render insufficient sulfur utilization and poor cycling stability. Herein, a facile, template-free procedure based on controlled pyrolysis of polydopamine vesicles is described to prepare N-doped porous carbon cages (NHSC) as a new sulfur host, which significantly improves both the sulfur utilization and cycling stability. As NHSC shows a high pore volume, continuous electron and ion transport paths, and good catalytic activity, encapsulation of S nanoparticles into NHSC endows the resulting S@NHSC electrode with a good energy storage capacity and exceptionally high electrochemical stability. Consequently, a Li-S cell with the S@NHSC as the cathode achieves a high initial capacity of 1280.7 mAh g-1 , and cycling stability over 500 cycles with the capacity decay as low as 0.0373% per cycle.

All-Inorganic CsPbI2Br Perovskite Solar Cells with High Efficiency Exceeding 13.

All-inorganic perovskite solar cells provide a promising solution to tackle the thermal instability problem of organic-inorganic perovskite solar cells (PSCs). Herein, we designed an all-inorganic perovskite solar cell with novel structure (FTO/NiO x/CsPbI2Br/ZnO@C60/Ag), in which ZnO@C60 bilayer was utilized as the electron-transporting layers that demonstrated high carrier extraction efficiency and low leakage loss. Consequently, the as-fabricated all-inorganic CsPbI2Br perovskite solar cell yielded a power conversion efficiency (PCE) as high as 13.3% with a Voc of 1.14 V, Jsc of 15.2 mA·cm-2, and FF of 0.77. The corresponding stabilized power output (SPO) of the device was demonstrated to be ∼12% and remarkably stable within 1000 s. Importantly, the obtained all-inorganic PSCs without encapsulation exhibited only 20% PCE loss with thermal treatment at 85 °C for 360 h, which largely outperformed the organic-species-containing PSCs. The present study demonstrates potential in overcoming the intractable issue concerning the thermal instability of perovskite solar cells.

Controllable Synthesis and Properties of Sb2Se3 Nanorods Synthesized by Hot-Injection Method.

Antimony selenide (Sb2Se3) is an interesting p-type semiconductor with a proper bandgap for photovoltaic devices. In this work, Sb2Se3 nanorods with controllable length-width ratios were synthesized via hot-injection method, where selenium powder was used as selenium sources and oleylamine was selected as reducing agent and high-point solvent. X-ray diffraction (XRD) patterns and high resolution Transmission electron microscope (HRTEM) results demonstrate that nanorods are wellcrystallized single crystalline and grow along the [110] direction. The reaction temperatures were found to have a noticeable influence on the morphologies of Sb2Se3 nanorods. The growth mechanism of the nanorods was discussed based on scanning electron microscope (SEM) observations. Vis-NIR absorption spectra reveal that the bandgaps of nanorods were between 0.75 eV and 1.1 eV. Electrical conductivities in dark and light were also investigated.

Controllable Grain Morphology of Perovskite Absorber Film by Molecular Self-Assembly toward Efficient Solar Cell Exceeding 17%.

The highly developed crystallization process with respect to perovskite thin films is favorable for efficient solar cells. Here, an innovative intermolecular self-assembly approach was employed to retard the crystallization of PbI2 in dimethylformamide (DMF) by additional solvent of dimethyl sulfoxide (DMSO), which was proved to be capable of coordinating with PbI2 by coordinate covalent bond. The obtained PbI2(DMSO)x (0 ≤ x ≤ 1.86) complexes tend to be closely packed by means of intermolecular self-assembly. Afterward, an intramolecular exchange of DMSO with CH3NH3I (MAI) enabled the complexes to deform their shape and finally to reorganize to be an ultraflat and dense thin film of CH3NH3PbI3. The controllable grain morphology of perovskite thin film allows obtaining a power conversion efficiency (PCE) above 17% and a stabilized power output above 16% within 240 s by controlling DMSO species in the complex-precursor system (CPS). The present study gives a reproductive and facile strategy toward high quality of perovskite thin films and efficient solar cells.

Ultraviolet C upconversion fluorescence of trivalent erbium in BaGd2ZnO5 phosphor excited by a visible commercial light-emitting diode.

Multiple ultraviolet (UV) emission bands have been obtained in Er3+ doped BaGd2ZnO5 phosphor under the excitation of a 532 nm solid-state laser, and the emission peaks at 217, 254, 278, 296, 314, 348, 374 and 394 nm were determined to stem from the high-energy states 4D(1/2), 4D(7/2), 2H(9/2), 2P(1/2), 2P(3/2), 4G(7/2), 4G(11/2), 4H(9/2) of trivalent erbium, respectively. Some UV emission bands in the UVC region can be observed when the sample was excited by commercial green (529 nm) and blue (460 nm) LED. In view of the small size, low-drive voltage and price of LED, UVC upconversion phosphor BaGd2ZnO5:Er3+ excited by visible LED has potential application in environmental sciences.

Efficient and Stable Perovskite Solar Cells and Modules Enabled by Tailoring Additive Distribution According to the Film Growth Dynamics.

Gas quenching and vacuum quenching process are widely applied to accelerate solvent volatilization to induce nucleation of perovskites in blade-coating method. In this work, we found these two pre-crystallization processes lead to different order of crystallization dynamics within the perovskite thin film, resulting in the differences of additive distribution. We then tailor-designed an additive molecule named 1,3-bis(4-methoxyphenyl)thiourea to obtain films with fewer defects and holes at the buried interface, and prepared perovskite solar cells with a certified efficiency of 23.75%. Furthermore, this work also demonstrates an efficiency of 20.18% for the large-area perovskite solar module (PSM) with an aperture area of 60.84 cm2. The PSM possesses remarkable continuous operation stability for maximum power point tracking of T90 > 1000 h in ambient air.

Investigation of the driving voltage on the high performance flexible ATF-ECDs based on PET/ITO/NiOX/LiTaO3/WO3/ITO.

High performance flexible all-thin-film electrochromic devices (ATF-ECDs) have been fabricated and systematically investigated by operating with different driving voltages during the electrochromic processes. The device structure (cross-section) and material properties of some main functional layers were presented and analysed. The electrochromic properties including kinetic and spectral tests were systematically investigated through combining chronoamperometry, cyclic voltammetry measurements and optical measurements. In addition, the open circuit memory measurement was also carried out. A much higher driving voltage might lead to a current leakage inside the device during coloring process. A proper driving voltage is needed for achieving high device performances. More details were widely described and deeply discussed.

Phenanthroline-Based Low-Cost and Efficient Small-Molecule Cathode Interfacial Layer Enables High-Performance Inverted Perovskite Solar Cells via Doctor-Blade Coating.

Perovskite solar cells (PSCs) have recently emerged as highly efficient and cutting-edge photovoltaic technology. In inverted PSCs, challenges are focused on the insufficient interface contact and energy level misalignment between the electron transport layer (ETL) and the metal electrode. Hence, the cathode interfacial layer (CIL) plays a crucial role in regulating energy levels and enabling charge extraction in PSCs. In this study, a low-cost phenanthroline derivative, 4,7-dimethoxy-1,10-phenanthroline (Phen-OMe), is developed as an efficient CIL between the PCBM and Ag electrodes. The incorporation of Phen-OMe not only improves the interfacial contact but also effectively reduces the work function (WF) of the Ag electrode, thus promoting charge dissociation and transport at the interface. Through utilizing a wide-band-gap perovskite with the band gap of 1.77 eV as the active layer by a simple, high-throughput, and low-cost doctor-blade coating process, the power conversion efficiency (PCE) is enhanced significantly from 16.11% of the control device to 18.61% of the device with Phen-OMe as the CIL. Interestingly, Phen-OMe shows a broad application as the CIL in PSCs and tandem solar cells (TSCs), resulting in a boosted efficiency of 22.29% in intermediate-band-gap PSCs and a PCE of 22.05% with a high open-circuit voltage (VOC) of 2.12 V in the perovskite/organic TSC. This achievement shows that Phen-OMe would be a potential candidate as low-cost and efficient CILs for PSCs.

Ligand Homogenized Br-I Wide-Bandgap Perovskites for Efficient NiOx-Based Inverted Semitransparent and Tandem Solar Cells.

Phase heterogeneity of bromine-iodine (Br-I) mixed wide-bandgap (WBG) perovskites has detrimental effects on solar cell performance and stability. Here, we report a heterointerface anchoring strategy to homogenize the Br-I distribution and mitigate the segregation of Br-rich WBG-perovskite phases. We find that methoxy-substituted phenyl ethylammonium (x-MeOPEA+) ligands not only contribute to the crystal growth with vertical orientation but also promote halide homogenization and defect passivation near the buried perovskite/hole transport layer (HTL) interface as well as reduce trap-mediated recombination. Based on improvements in WBG-perovskite homogeneity and heterointerface contacts, NiOx-based opaque WBG-perovskite solar cells (WBG-PSCs) achieved impressive open-circuit voltage (Voc) and fill factor (FF) values of 1.22 V and 83%, respectively. Moreover, semitransparent WBG-PSCs exhibit a PCE of 18.5% (15.4% for the IZO front side) and a high FF of 80.7% (79.4% for the IZO front side) for a designated illumination area (da) of 0.12 cm2. Such a strategy further enables 24.3%-efficient two-terminal perovskite/silicon (double-polished) tandem solar cells (da of 1.159 cm2) with a high Voc of over 1.90 V. The tandem devices also show high operational stability over 1000 h during T90 lifetime measurements.

Large Orientation Angle Buried Substrate Enables Efficient Flexible Perovskite Solar Cells and Modules.

Flexible perovskite solar cells (f-PSCs) have emerged as potential candidates for specific mechanical applications owing to their high foldability, efficiency, and portability. However, the power conversion efficiency (PCE) of f-PSC remains limited by the inferior contact between perovskite and flexible buried substrate. Here, an asymmetric π-extended self-assembled monolayer (SAM) (4-(9H-dibenzo[a,c]carbazol-9-yl)butyl)phosphonic acid (A-4PADCB) is reported as a buried substrate for efficient inverted f-PSCs. Employing this design strategy, A-4PADCB exhibits a significant orientation angle away from the surface normal, homogenizing the distribution of contact potentials. This enhancement improves the SAM/perovskite interface quality, controlling the growth of favorable perovskite films with low defect density and slight tensile stress. Integration of A-4PADCB into small-area f-PSCs and large-area flexible perovskite solar modules with an aperture area of 20.84 cm2 achieves impressive PCEs of up to 25.05% and 20.64% (certified 19.51%), respectively. Moreover, these optimized A-4PADCB-based f-PSCs possess enhanced light, thermal, and mechanical stability. This research paves a promising avenue toward the design of SAM-buried substrates with a large orientation angle, regulating perovskite growth, and promoting the commercialization of large-area flexible perovskite photovoltaics.

Operando monitoring of dendrite formation in lithium metal batteries via ultrasensitive tilted fiber Bragg grating sensors.

Lithium (Li) dendrite growth significantly deteriorates the performance and shortens the operation life of lithium metal batteries. Capturing the intricate dynamics of surface localized and rapid mass transport at the electrolyte-electrode interface of lithium metal is essential for the understanding of the dendrite growth process, and the evaluation of the solutions mitigating the dendrite growth issue. Here we demonstrate an approach based on an ultrasensitive tilted fiber Bragg grating (TFBG) sensor which is inserted close to the electrode surface in a working lithium metal battery, without disturbing its operation. Thanks to the superfine optical resonances of the TFBG, in situ and rapid monitoring of mass transport kinetics and lithium dendrite growth at the nanoscale interface of lithium anodes have been achieved. Reliable correlations between the performance of different natural/artificial solid electrolyte interphases (SEIs) and the time-resolved optical responses have been observed and quantified, enabling us to link the nanoscale ion and SEI behavior with the macroscopic battery performance. This new operando tool will provide additional capabilities for parametrization of the batteries' electrochemistry and help identify the optimal interphases of lithium metal batteries to enhance battery performance and its safety.

Efficient and Stable Perovskite Solar Modules Enabled by Inhibited Escape of Volatile Species.

The intrinsically weak bonding structure in halide perovskite materials makes components in the thin films volatile, leading to the decomposition of halide perovskite materials. The reactions within the perovskite film are reversible provided that components do not escape the thin films. Here, a holistic approach is reported to improve the efficiency and stability of PSMs by preventing the effusion of volatile components. Specifically, a method for in situ generation of channel barrier layers for perovskite photovoltaic modules is developed. The resulting PSMs attain a certified aperture PCE of 21.37%, and possess remarkable continuous operation stability for maximum power point tracking (MPPT) of T90 > 1100 h in ambient air, and damp heat (DH) tracking of T93 > 1400 h.

Crystallization Kinetics of Perovskite Films by a Green Mixture Antisolvent for Efficient NiOx-Based Inverted Solar Cells.

Environment-friendly antisolvents are critical for obtaining highly efficient, reproducible, and sustainable perovskite solar cells (PSCs). Here, we introduced a green mixture antisolvent of ethyl acetate-isopropanol (EA/IPA) to finely regulate the crystal grain growth and related film properties, including the morphology, crystal structure, and chemical composition of the perovskite thin film. The IPA with suitable content in EA plays a key role in achieving a smooth and compact high-quality perovskite thin film, leading to the suppression of film defect-induced nonradiative recombination. As a result, the PSCs based on the EA/IPA (5:1) antisolvent showed a power conversion efficiency of 22.9% with an open-circuit voltage of 1.17 V.

Slow-Release Effect Assisted Crystallization for Sequential Deposition Realizes Efficient Inverted Perovskite Solar Cells.

The two-step sequential deposition strategy has been widely recognized in promoting the research and application of perovskite solar cells, but the rapid reaction of organic salts with lead iodide inevitably affects the growth of perovskite crystals, accompanied by the generation of more defects. In this study, the regulation of crystal growth was achieved in a two-step deposition method by mixing 1-naphthylmethylammonium bromide (NMABr) with organic salts. The results show that the addition of NMABr effectively delays the aggregation and crystallization behavior of organic salts; thereby, the growth of the optimal crystal (001) orientation of perovskite is promoted. Based on this phenomenon of delaying the crystallization process of perovskite, the "slow-release effect assisted crystallization" is defined. Moreover, the incorporation of the Br element expands the band gap of perovskite and mitigates material defects as nonradiative recombination centers. Consequently, the power conversion efficiency (PCE) of the enhanced perovskite solar cells (PSCs) reaches 20.20%. It is noteworthy that the hydrophobic nature of the naphthalene moiety in NMABr can enhance the humidity resistance of PSCs, and the perovskite phase does not decompose for more than 3000 h (30-40% RH), enabling it to retain 90% of its initial efficiency even after exposure to a nitrogen environment for 1200 h.

Dendrimer Modification Strategy Based on the Understanding of the Photovoltaic Mechanism of a Perovskite Device under Full Sun and Indoor Light.

The wide-band-gap inorganic CsPbI2Br perovskite material provides a highly matched absorption range with the indoor light spectrum and is expected to be used in the fabrication of highly efficient indoor photovoltaic cells (IPVs) and self-powered low-power Internet of Things (IoT) sensors. However, the defects that cause nonradiative recombination and ion migration are assumed to form leakage loss channels, resulting in a severe impact on the open-circuit voltage (VOC) and the fill factor (FF) of IPVs. Herein, we introduce poly(amidoamine) (PAMAM) dendrimers with multiple passivation sites to fully repair the leakage channels in the devices, taking into account the characteristics of IPVs that are extremely sensitive to nonradiative recombination and shunt resistance. The as-optimized IPVs demonstrate a promising PCE of 35.71% under a fluorescent light source (1000 lux), with VOC increased from 0.99 to 1.06 V and FF improved from 75.21 to 84.39%. The present work provides insight into the photovoltaic mechanism of perovskites under full sun and indoor light, which provides guidance for perovskite photovoltaic technology with industrialization prospects.

Impermeable Atomic Layer Deposition for Sputtering Buffer Layer in Efficient Semi-Transparent and Tandem Solar Cells via Activating Unreactive Substrate.

Atomic layer deposition (ALD) turns out to be particularly attractive technology for the sputtering buffer layer when preparing the semi-transparent (ST) perovskite solar cells (PSCs) and the tandem solar cells. ALD process turns to be island growth when the substrate is unreactive with the ALD reactants, resulting in the pin-hole layer, which causes an adverse effect on anti-sputtering. Here, p-i-n structured PSCs with ALD SnOx as sputtering buffer layer are conducted. The commonly used electron transportation layer (ETL) PCBM in the p-i-n structured PVK solar cell is an unreactive substrate that prevents the layer-by-layer growth for the ALD SnOx . PCBM layer is activated by introducing reaction sites to form impermeable ALD layers. By introducing reaction sites/ALD SnOx as sputtering buffer layer, the authors succeed to fabricate ST-PSCs and perovskite/silicon (double-side polished) tandem solar cells with power conversion efficiency (PCE) of 20.25% and 23.31%, respectively. Besides, the unencapsulated device with reaction sites maintains more than 99% of the initial PCE after aging over 5100 h. This work opens a promising avenue to prepare impermeable layer for stable PSCs, ST-PSCs, tandem solar cells, and the related scale-up solar cells.

Hole-Transport Management Enables 23%-Efficient and Stable Inverted Perovskite Solar Cells with 84% Fill Factor.

NiOx-based inverted perovskite solar cells (PSCs) have presented great potential toward low-cost, highly efficient and stable next-generation photovoltaics. However, the presence of energy-level mismatch and contact-interface defects between hole-selective contacts (HSCs) and perovskite-active layer (PAL) still limits device efficiency improvement. Here, we report a graded configuration based on both interface-cascaded structures and p-type molecule-doped composites with two-/three-dimensional formamidinium-based triple-halide perovskites. We find that the interface defects-induced non-radiative recombination presented at HSCs/PAL interfaces is remarkably suppressed because of efficient hole extraction and transport. Moreover, a strong chemical interaction, halogen bonding and coordination bonding are found in the molecule-doped perovskite composites, which significantly suppress the formation of halide vacancy and parasitic metallic lead. As a result, NiOx-based inverted PSCs present a power-conversion-efficiency over 23% with a high fill factor of 0.84 and open-circuit voltage of 1.162 V, which are comparable to the best reported around 1.56-electron volt bandgap perovskites. Furthermore, devices with encapsulation present high operational stability over 1,200 h during T90 lifetime measurement (the time as a function of PCE decreases to 90% of its initial value) under 1-sun illumination in ambient-air conditions.