Research data supporting" High carrier mobility along the [111] orientation in Cu2O photoelectrodes"

SI Data contains all synthesis details (including 1H NMR, UV-vis, MS), photocatalysis, product quantification, Transmission IR spectra for 13C, in-situ UV-vis spectroscopy, FT-IR, Photoluminescence quenching, electrochemistry and image data related to the Supplementary Information sorted by respective figure.

Advanced Materials

High‐performance perovskite solar cells (PSCs) typically require interfacial passivation, yet this is challenging for the buried interface, owing to the dissolution of passivation agents during the deposition of perovskites. Here, this limitation is overcome with in situ buried‐interface passivation—achieved via directly adding a cyanoacrylic‐acid‐based molecular additive, namely BT‐T, into the perovskite precursor solution. Classical and ab initio molecular dynamics simulations reveal that BT‐T spontaneously may self‐assemble at the buried interface during the formation of the perovskite layer on a nickel oxide hole‐transporting layer. The preferential buried‐interface passivation results in facilitated hole transfer and suppressed charge recombination. In addition, residual BT‐T molecules in the perovskite layer enhance its stability and homogeneity. A power‐conversion efficiency (PCE) of 23.48% for 1.0 cm2 inverted …

Nature Energy

The stabilization of grain boundaries and surfaces of the perovskite layer is critical to extend the durability of perovskite solar cells. Here we introduced a sulfonium-based molecule, dimethylphenethylsulfonium iodide (DMPESI), for the post-deposition treatment of formamidinium lead iodide perovskite films. The treated films show improved stability upon light soaking and remains in the black α phase after two years ageing under ambient condition without encapsulation. The DMPESI-treated perovskite solar cells show less than 1% performance loss after more than 4,500 h at maximum power point tracking, yielding a theoretical T80 of over nine years under continuous 1-sun illumination. The solar cells also display less than 5% power conversion efficiency drops under various ageing conditions, including 100 thermal cycles between 25 °C and 85 °C and an 1,050-h damp heat test.

Nature

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight,. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials, –. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111 …

Materials Science in Semiconductor Processing

We investigate the reproducibility of repeated intercalation of hydrogen in graphene/Ge (110) and the formation of H2 nanobubbles after thermal treatments. By exploiting high-resolution electron energy loss, we obtain direct spectroscopic fingerprints of H2 trapped gas in the samples when nanobubbles are present and we are able to track the effectiveness of H intercalation via the Ge–H vibrational mode. We correlate the effectiveness of interface re-hydrogenation to the presence of structural defects in graphene as highlighted by Raman spectroscopy. The π-plasmon mode of graphene on Ge (110) is investigated as a function of the hydrogen presence at the interface, revealing that, independent of the hydrogen intercalation status, graphene is weakly interacting on Ge (110).

Small

Metal halide perovskites are multifunctional semiconductors with tunable structures and properties. They are highly dynamic crystals with complex octahedral tilting patterns and strongly anharmonic atomic behavior. In the higher temperature, higher symmetry phases of these materials, several complex structural features are observed. The local structure can differ greatly from the average structure and there is evidence that dynamic 2D structures of correlated octahedral motion form. An understanding of the underlying complex atomistic dynamics is, however, still lacking. In this work, the local structure of the inorganic perovskite CsPbI3 is investigated using a new machine learning force field based on the atomic cluster expansion framework. Through analysis of the temporal and spatial correlation observed during large‐scale simulations, it is revealed that the low frequency motion of octahedral tilts implies a …

Nature

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight,. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials, –. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111 …

Nature Energy

The stabilization of grain boundaries and surfaces of the perovskite layer is critical to extend the durability of perovskite solar cells. Here we introduced a sulfonium-based molecule, dimethylphenethylsulfonium iodide (DMPESI), for the post-deposition treatment of formamidinium lead iodide perovskite films. The treated films show improved stability upon light soaking and remains in the black α phase after two years ageing under ambient condition without encapsulation. The DMPESI-treated perovskite solar cells show less than 1% performance loss after more than 4,500 h at maximum power point tracking, yielding a theoretical T80 of over nine years under continuous 1-sun illumination. The solar cells also display less than 5% power conversion efficiency drops under various ageing conditions, including 100 thermal cycles between 25 °C and 85 °C and an 1,050-h damp heat test.

Nature

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight,. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials, –. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance. Here we demonstrate performance of Cu2O photocathodes beyond the state-of-the-art by exploiting a new conceptual understanding of carrier recombination and transport in single-crystal Cu2O thin films. Using ambient liquid-phase epitaxy, we present a new method to grow single-crystal Cu2O samples with three crystal orientations. Broadband femtosecond transient reflection spectroscopy measurements were used to quantify anisotropic optoelectronic properties, through which the carrier mobility along the [111 …

Nature Photonics

Perovskite light-emitting diodes (LEDs) show promises for next-generation displays owing to their excellent luminescent properties and low cost. Despite substantial progress with green- and red-emitting devices, the development of efficient blue perovskite LEDs has lagged behind. Here we demonstrate efficient blue perovskite LEDs based on a mixed two-dimensional–three-dimensional perovskite and a multifunctional ionic additive that enables control over the reduced-dimensional phases, non-radiative recombination channels and spectral stability. We report a series of devices that emit efficient electroluminescence from mixed bromide/chloride quasi-three-dimensional regions, with external quantum efficiencies of up to 21.4% (at a luminance of 22 cd m–2 and emission peak at 483 nm), 13.2% (at a luminance of 2.0 cd m–2 and emission peak at 474 nm) and 7.3% (at a luminance of 6 cd m–2 and …

Nature Communications

Bifacial perovskite solar cells have shown great promise for increasing power output by capturing light from both sides. However, the suboptimal optical transmittance of back metal electrodes together with the complex fabrication process associated with front transparent conducting oxides have hindered the development of efficient bifacial PSCs. Here, we present a novel approach for bifacial perovskite devices using single-walled carbon nanotubes as both front and back electrodes. single-walled carbon nanotubes offer high transparency, conductivity, and stability, enabling bifacial PSCs with a bifaciality factor of over 98% and a power generation density of over 36%. We also fabricate flexible, all-carbon-electrode-based devices with a high power-per-weight value of 73.75 W g−1 and excellent mechanical durability. Furthermore, we show that our bifacial devices have a much lower material cost than …

The adverse environmental impacts of greenhouse gas emissions and persistent waste accumulation are driving the demand for sustainable approaches to clean-energy production and waste recycling. By coupling the thermodynamically favourable oxidation of waste-derived organic carbon streams with fuel-forming reduction reactions suitable for producing clean hydrogen or converting CO2 to fuels, solar reforming simultaneously valorizes waste and generates useful chemical products. With appropriate light harvesting, catalyst design, device configurations and waste pre-treatment strategies, a range of sustainable fuels and value-added chemicals can already be selectively produced from diverse waste feedstocks, including biomass and plastics, demonstrating the potential of solar-powered upcycling plants. This Review highlights solar reforming as an emerging technology that is currently transitioning from …

Advanced Functional Materials

Perovskite solar cells have led the new surge of solar energy research. However, their instability is a pressing issue mostly attributed to the perovskite interface with charge‐selective transport layers. In this work, diethylammonium iodide (DEAI) surface treatment is used to mitigate interfacial non‐radiative recombination losses by forming a mixed phase of layered perovskite on the surface. This results in enhanced device performance with the power conversion efficiency of 23.3% and improved operational stability under thermal stress. Moreover, the DEAI treatment facilitates interfacial hole transfer, enabling a carbon‐based hole transport layer‐free perovskite solar cell with a power conversion efficiency of 15.6%.

Journal of Materials Chemistry B

The Editors-in-Chief for Journal of Materials Chemistry A, B and C look back at the 10th anniversary year and the celebratory activities that took place.

Advanced Materials

Efficient and robust n‐i‐p perovskite solar cells necessitate superior organic hole‐transport materials with both mechanical and electronic prowess. Deciphering the structure−property relationship of these materials is crucial for practical perovskite solar cell applications. Through direct arylation, we synthesized two high glass transition temperature molecular semiconductors, DBC‐ETPA (202 °C) and TPE‐ETPA (180 °C), using dibenzo[g,p]chrysene (DBC) and 1,1,2,2‐tetraphenylethene (TPE) tetrabromides with triphenylene–ethylenedioxythiophene‐dimethoxytriphenylamine (ETPA). In comparison to spiro‐OMeTAD, both semiconductors exhibit shallower HOMO energy levels, resulting in increased hole densities (generated by air oxidation doping) and accelerated hole extraction from photoexcited perovskite. Experimental and theoretical studies highlight the more rigid DBC core, enhancing hole mobility due to …

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A simple and precious‐metal free photosystem for the reduction of aqueous CO2 to syngas (CO and H2) is reported consisting of carbon dots (CDs) as the sole light harvester together with a molecular cobalt bis(terpyridine) CO2 reduction co‐catalyst. This homogeneous photocatalytic system operates in the presence of a sacrificial electron donor (triethanolamine) in DMSO/H2O solution at ambient temperature. The photocatalytic system exhibits an activity of 7.7 ± 0.2 mmolsyngas gCDs−1 (3.6 ± 0.2 mmolCO gCDs−1 and 4.1 ± 0.1 mmolH2 gCDs−1) after 24 hours of full solar spectrum irradiation (AM 1.5G). Spectroscopic and electrochemical characterization supports that this photocatalytic performance is attributed to a favorable association between CDs and the molecular cobalt catalyst, which results in improved interfacial photoelectron transfer and catalytic mechanism. This work provides a scalable and …