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This Perspective features the newly emerged AIO-type Cu( i )X-based hybrid semiconductors and showcases their structural diversity, solution-processability, framework stability, important photophysical properties and related potential applications.
We copolymerize a norbornene monomer bearing a pendant naphthalene diimide with a norbornene bearing a cinnamate pendant moiety to synthesize a crosslinkable electron-transporting polymer and study its use in solution-processed n–i–p perovskite solar cells. The crosslinked material exhibits over 90% transparency in the visible region and higher thermal stability (>300 °C) and lower surface energy than the corresponding homopolymer of the naphthalene diimide functionalized norbornene. Coating an ITO surface with the photo-crosslinked copolymer yields a slightly lower work function than homopolymer-coated ITO. We show that the morphologies of the perovskite films deposited on both polymers are similar (~300 nm features) based upon scanning electron microscopy. Our solar-cell device results show that the crosslinked naphthalene diimide polymer gives a higher open-circuit voltage (1.08 vs 1.05 V), fill factor (average 64.43 vs 58.77%), and stabilized power conversion efficiency (12.28 vs 10.33%) compared to its non-crosslinked homopolymer counterpart, as well as reduced hysteresis. As a result, we attribute the improved performance to decreased work function, reduced nonradiative recombination, and higher shunt resistance.
Proton-conducting electrochemical cells (PCECs) are promising for efficient hydrogen production, but achieving dense, uniform, thin electrolyte layers remains a key challenge, particularly for scalable fabrication. Here, we present a solution-processed deposition approach with a mechanistically optimized slurry for uniform electrolyte formation. By tailoring particle size distribution, solid loading, and solvent/additive balance, we regulated wetting behavior and evaporation kinetics of the electrolyte slurry to promote homogeneous electrolyte particle packing. These features facilitate tight grain boundary contact and early stage neck growth during sintering, eliminating residual porosity, and improving mechanical integrity. The resulting ∼15 μm thick electrolyte shows high density, strong electrode adhesion, and stable interfaces outperforming the previously reported spray-based fabricated electrolyte by about 31% at 600 °C in FC mode. Single cells deliver 0.962 W cm –2 at 600 °C in fuel cell mode and 1.31 A cm –2 at 1.3 V in electrolysis mode, maintaining robust performance over 100 h with negligible degradation (≤0.02% h –1 ) in each mode. Scale-up to 2.5 cm diameter substrates confirmed reproducible densification and geometric stability. This work demonstrates a cost-effective, scalable route where control over particle-fluid interactions and drying dynamics enables a superior electrolyte microstructure and high PCEC performance.
Conjugated polymers functionalized with oligoether (OE)-based side chains are a key class of materials for various organic electronic applications, including transparent electrodes, thermoelectrics, electrochromic displays, and electrochemical transistors. Herein, we report a highly soluble OE-functionalized poly(3,4-ethylenedioxythiophene) (PEDOT) homopolymer, prepared by direct (hetero)arylation polymerization, which allows solution processing to yield films with comparable redox properties to oxidatively polymerized PEDOT. This polymer, PEDOT(OE3), when optimally oxidatively doped, reaches among the highest electrical conductivities of any OE-functionalized polymer and is comparable to more synthetically complex OE-functionalized polymers. X-ray scattering and spectroscopy were utilized to rationalize the transport properties resulting from varying the doping level. Comparison of PEDOT(OE3) to a series of OE-functionalized dioxythiophenes with varying amounts of 3,4-ethylenedioxythiophene units allows for a deeper understanding of structure–property relationships through charge-transport models. Ultimately, PEDOT(OE3) is shown to be a material with exceptional charge-transport properties and is promising for various applications.
Thermography detects mid-infrared radiation from surfaces based on the Stefan-Boltzmann law, mapping surface temperatures and potentially revealing subsurface thermal activity. Recent developments offer an alternative strategy to traditional camera-based improvements: a thermal imaging sensitizer (TIS) coating whose emissivity increases sharply with local temperature, amplifying small thermal variations into high-contrast signals. Existing TIS structures are nanofabricated solid membranes and face significant challenges in fabrication complexity. Here, in this study, we present a solution-processed, liquid form of TIS, termed temperature-adaptive radiative paint (TARP), to address these limitations. TARP offers drastically reduced fabrication costs, scalability to large areas, applicability to curved surfaces, and an extended operating temperature range, while maintaining the function of temperature amplification. Application of TARP enhances small temperature contrast by more than 3 times, substantially improving ambient thermography and enabling broader applications such as detection of structural defects and hot spots in electronic components.
Tin-lead (Sn-Pb) narrow bandgap (NBG) perovskites show great potential in both single-junction and all-perovskite tandem solar cells. Sn-Pb perovskite solar cells (PSCs) are still limited by low charge collection efficiency and poor stability. Here, we report a ternary Sn (II) alloy of SnOCl as the hole-transport material (HTM) with a work function of 4.95 eV for Sn-Pb PSCs. The solution processed SnOCl layer has a texture structure which not only reduces the optical loss of the devices but also changes grain growth of Sn-Pb perovskites and boosts the carrier diffusion length to 3.63 μm. The formation of small perovskite grains at the HTM/perovskite interface is suppressed. These result in an almost constant internal quantum efficiency of 96 ± 2% across the absorption spectrum of Sn-Pb perovskites. The SnOCl HTM significantly enhances the stability of Sn-Pb PSCs with 87% of its initial efficiency retained after 1-sun illumination for 1,200 h, and keep 85% efficiency under 85°C thermal stress for 1,500 h. Furthermore, the hybrid HTM further improve the stabilized efficiencies of single-function Sn-Pb PSCs and all-perovskite tandem solar cells to 23.2% and 25.9%, respectively. This discovery opens an avenue to the multi-component metal alloys as HTM in PSCs.
Single photons are cornerstones of quantum technologies. The need for an ultrafast, bright, and stable photon source emitting in the telecom-band at ∼1550 nm, ideally operating at room temperature, has resulted in a decades-long quest. However, to date, telecom sources are hampered by inherently long radiative lifetimes that severely limit brightness and speed, material instability, or the need for cryogenic operation. Here, in this study, stable colloidal PbS/CdS quantum dots emitting at 1550 nm (C-band) or 1350 nm (O-band) are embedded in a solution-synthesized nanoparticle-on-mirror cavity. Single cavity-coupled quantum dots experience extreme Purcell factors up to 10,700, resulting in ultrafast emission lifetimes of 65 ps, along with near-complete blinking suppression. As a result, 12 million single photons are emitted per second affording a single photon source at 1550 nm that is more than two orders of magnitude brighter than previously possible at room-temperature. These telecom-band single photon sources are solution-processable and lithography-free and may leverage mature colloidal fabrication technologies for future quantum applications.
A critical issue in developing high-performance organic light-emitting transistors (OLETs) is to balance the trade-off between charge transport and light emission in a semiconducting material. Although traditional materials for organic light-emitting diodes (OLEDs) or organic field-effect transistors (OFETs) have shown modest performance in OLET devices, design strategies towards high-performance OLET materials and the crucial structure–performance relationship remain unclear. Our research effort in developing cross-conjugated weak acceptor-weak donor copolymers for luminescent properties lead us to an unintentional discovery that these copolymers form coiled foldamers with intramolecular H-aggregation, leading to their exceptional OLET properties. An impressive external quantum efficiency (EQE) of 6.9% in solution-processed multi-layer OLET devices was achieved.
The chalcogenide perovskite family has been steadily gaining increasing attention from the research community due to its optoelectronic properties and potential for diverse applications. While BaZrS 3 and BaTiS 3 have been the most extensively studied, other promising compounds in this family, such as Sr x TiS 3 (1.05 < x < 1.22), are now being explored for various optical, optoelectronic, and energy storage applications. However, challenges remain in achieving the low-temperature synthesis of Sr x TiS 3 . In this study, we report, for the first time, the synthesis of Sr x TiS 3 nanocrystals at temperatures below 400 °C. The synthesized nanocrystals exhibit a rod-like morphology. Additionally, we have developed solution-processing routes to synthesize phase-pure Sr x TiS 3 thin films, marking the first reported instance of such films, at temperatures below 600 °C. We also demonstrate the solid-state synthesis of Sr x TiS 3 powder below 600 °C. Our work paves the way for new and exciting application avenues for Sr x TiS 3 .
A series of copper halide based inorganic–organic hybrid semiconductors have been synthesized. Structural analysis confirms that all compounds are composed of one-dimensional Cu 4 X 6 2- anionic chains that coordinate to cationic ligands via Cu–N dative bonds. Different coordination affinities of the ligands lead to two types of ligand arrangements with various structural distortions. All compounds are highly resistant to heat and moisture as a result of the combination of coordinate and ionic bonds. Low energy emission with high efficiency is achieved for these compounds and the emission energy (~552–615 nm) and color (yellow-orange) can be tuned by varying the ligand and halogen element. The electronic structure and luminescence mechanism are examined by both experimental and theoretical methods. More importantly, all compounds demonstrate good solubility in polar aprotic solvents, a desired property that is absent in all other CuX hybrid families of extended structures, which is attributed primarily to the ionic nature of this material class. Furthermore, the good solution-processability, and cost effective and easily scalable synthesis coupled with high quantum efficiencies and framework stability make these hybrid materials promising phosphors for general lighting applications.
Although back-surface passivation plays an important role in high-efficiency photovoltaics, it has not yet been definitively demonstrated for CdTe. Here, we present a solution-based process, which achieves passivation and improved electrical performance when very small amounts of oxidized Al 3+ species are deposited at the back surface of CdTe devices. The open circuit voltage (V oc ) is increased and the fill factor (FF) and photoconversion efficiency (PCE) are optimized when the total amount added corresponds to ~1 monolayer, suggesting that the passivation is surface specific. Addition of further Al 3+ species, present in a sparse alumina-like layer, causes the FF and PCE to drop as the interface layer becomes blocking to current flow. The optimized deposit increases the average baseline PCE for both Cu-free devices and devices where Cu is present as a dopant. The greatest improvement is found when the Al 3+ species are deposited prior to the CdCl 2 activation step and Cu is employed. In this case, the best-cell efficiency was improved from 12.6 to 14.4%. Furthermore, time-resolved photoluminescence measurements at the back surface and quantum efficiency measurements performed at the maximum power point indicate that the performance enhancement is due to a reduction in the interface recombination current at the back surface.
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In materials science, chiral perovskites stand out due to their exceptional optoelectronic properties and the versatility in their structure and composition, positioning them as crucial in the advances of technologies in spintronics and chiroptical systems. This review underlines the critical role of synthesizing and growing these materials, a process integral to leveraging their complex interplay between structural chirality and distinctive optoelectronic properties, including chiral-induced spin selectivity and chiroptical activity. The paper offers a comprehensive summary and discussion of the methods used in the synthesis and growth of chiral perovskites, delving into extensive growth techniques, fundamental mechanisms, and strategic approaches for the engineering of low-dimensional perovskites, alongside the creation of novel chiral ligands. The necessity of developing new synthetic approaches and maintaining precise control during the growth of chiral perovskites is emphasized, aiming to enhance their structural chirality and boost their efficiency in spin and chiroptical selectivity.
The engineering of mixed-solvent formulations and their evaporation conditions are key to reproducible perovskite coatings for high-performance photovoltaics. Here, we report a lumped-parameter evaporation model to predict the evolution of a perovskite ink liquid film over time (solvent ratio, solute concentration, and film thickness). The drying-rate model is validated via in situ film-thickness measurements, and the predicted transient liquid film state is mapped as a process path. These methods allow for the prediction of process sensitivity to local environmental factors and the understanding and visualization of a broader processing parameter space enabled through the coupling of process and ink engineering. Process maps are applied to create a new framework for scalable perovskite coating development with a goal of improving the reproducibility and transferability of perovskite fabrication. This approach is demonstrated with blade-coated FA 0.83 Cs 0.17 PbI 3 photovoltaic devices, improving the photovoltaic conversion efficiency from 17.5% ± 1.7% to 20.3% ± 0.6%.
In this study, we demonstrated for the first time that a metal-containing semicrystalline polymer was used as an additive to mediate the thin film morphology of solution-grown, small-molecule organic semiconductors. By mixing polyferrocenylsilane (PFS) with an extensively-studied organic semiconductor 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene), PFS as a semicrystalline polymer independently forms nucleation and crystallization while simultaneously ameliorating diffusivity of the blend system and tuning the surface energies as a result of its partially amorphous property. We discovered that the resultant blend film exhibited a 6-fold reduction in crystal misorientation angle and a 3-fold enlargement in average grain width. Enhanced crystal orientation considerably reduces mobility variation, while minimized defects and trap centers located at grain boundaries lessen the adverse impact on the charge transport. Consequently, bottom-gate, top-contact organic thin film transistors (OTFTs) based on the TIPS pentacene/PFS mixture yielded a 40% increase in performance consistency (represented by the ratio of average mobility to the standard deviation of mobility). The PFS semicrystalline polymer-controlled crystallization can be used to regulate the thin film morphology of other high-performance organic semiconductors and shed light on applications in organic electronic devices.
Industrial decarbonization is a key area that must be accelerated, to foster the removal of fossil fuels from the provision of heat, especially at low temperatures less than 300 degrees C. This paper looks at the results of two case studies for understanding the economics and potential for renewable thermal energy systems (RTES), particularly in hybrid configurations to provide industrial process heat (IPH). The first case study looks at heat pumps for district heating, and the second, the use of linear Fresnel collectors (LFCs) coupled with phase change material (PCM) thermal energy storage (TES) for direct steam generation (DSG). Using district heat as an input for the heat pump, three cases were run harvesting energy from ambient water (5 degrees C), sewage water (20 degrees C), and a solar collector (35 degrees C). Accounting for elevated costs of infrastructure for each heat source, the levelized cost of heat (LCOH) of the first case study ranged from $4-$15 per million British Thermal Units (MMBTU). For the second case study modeling LFCs with PCM and TES, the results show that a LCOH of $9-$15 per MMBTU is possible, depending on the direct normal irradiance.
Industrial decarbonization is a key area that must be accelerated, to foster the removal of fossil fuels from the provision of heat, especially at low temperatures less than 300 degrees C. This paper looks at the results of two case studies for understanding the economics and potential for renewable thermal energy systems (RTES), particularly in hybrid configurations to provide industrial process heat (IPH). The first case study looks at heat pumps for district heating, and the second, the use of linear Fresnel collectors (LFCs) coupled with phase change material (PCM) thermal energy storage (TES) for direct steam generation (DSG). Using district heat as an input for the heat pump, three cases were run harvesting energy from ambient water (5 degrees C), sewage water (20 degrees C), and a solar collector (35 degrees C). Accounting for elevated costs of infrastructure for each heat source, the levelized cost of heat (LCOH) of the first case study ranged from $4-$10 per million British Thermal Units (MMBTU). For the second case study modeling LFCs with PCM and TES, the results show that a LCOH of $9-$15 per MMBTU is possible, depending on the direct normal irradiance.