Atomic-level passivation mechanism of ammonium salts enabling highly efficient perovskite solar cells.

The high conversion efficiency has made metal halide perovskite solar cells a real breakthrough in thin film photovoltaic technology in recent years. Here, we introduce a straightforward strategy to reduce the level of electronic defects present at the interface between the perovskite film and the hole transport layer by treating the perovskite surface with different types of ammonium salts, namely ethylammonium, imidazolium and guanidinium iodide. We use a triple cation perovskite formulation containing primarily formamidinium and small amounts of cesium and methylammonium. We find that this treatment boosts the power conversion efficiency from 20.5% for the control to 22.3%, 22.1%, and 21.0% for the devices treated with ethylammonium, imidazolium and guanidinium iodide, respectively. Best performing devices showed a loss in efficiency of only 5% under full sunlight intensity with maximum power tracking for 550 h. We apply 2D- solid-state NMR to unravel the atomic-level mechanism of this passivation effect

Multifunctional molecular modulators for perovskite solar cells with over 20% efficiency and high operational stability

Perovskite solar cells present one of the most prominent photovoltaic technologies, yet their stability, scalability, and engineering at the molecular level remain challenging. We demonstrate a concept of multifunctional molecular modulation of scalable and operationally stable perovskite solar cells that exhibit exceptional solar-to-electric power conversion efficiencies. The judiciously designed bifunctional molecular modulator SN links the mercapto-tetrazolium (S) and phenylammonium (N) moieties, which passivate the surface defects, while displaying a structure-directing function through interaction with the perovskite that induces the formation of large grain crystals of high electronic quality of the most thermally stable formamidinium cesium mixed lead iodide perovskite formulation. As a result, we achieve greatly enhanced solar cell performance with efficiencies exceeding 20% for active device areas above 1 cm(2) without the use of antisolvents, accompanied by outstanding operational stability under ambient conditions

Europium-Doped CsPbI2Br for Stable and Highly Efficient Inorganic Perovskite Solar Cells

All-inorganic perovskite films hold promise for improving the stability of perovskite solar cells (PSCs). However, the 3D alpha phase of narrow-bandgap inorganic perovskites is thermodynamically unstable at room temperature, limiting the development of high-performance inorganic PSCs. Here, we show that europium doping of CsPbI2Br stabilizes the alpha phase of this inorganic perovskite at room temperature. We rationalize it by using solid-state nuclear magnetic resonance and high-angle annular dark-field scanning transmission electron microscopy, which show that europium is incorporated into the perovskite lattice. We demonstrate amaximum power-conversion efficiency of 13.71% for an inorganic PSC with the CsPb0.95Eu0.05I2Br perovskite and alpha stable power output of 13.34%. Using electroluminescence we show that incorporation of europium reduces non-radiative recombination, resulting in high open-circuit voltage of 1.27 V. The devices retain 93% of the initial efficiency after 370 hr under 100 mW cm(-2) continuous white light illumination under maximum-power point-tracking measurement

Recent developments in perovskite-based precursor inks for scalable architectures of perovskite solar cell technology

Abstract The progressive enhancements in solar-to-electrical conversion within the past decade have allowed organic–inorganic lead halide perovskite-based solar cell (PSC) technology to become a competitive candidate for creating affordable and sustainable electricity. This review highlights the developments in fabricating advanced precursor inks of organic–inorganic lead halide perovskite-based light harvesters for large-area perovskite solar cell technology. One of the key characteristics of this promising photovoltaic technology includes solution processing, which offers possibilities to scale up lab-sized solar cell devices into large-area perovskite solar modules comprising unique device architectures. These have been realized in recent years for their deployment in various applications such as building-integrated photovoltaics or internet of things (IoT) devices. In this regard, the presented overview highlights the recent trends that have emerged in the research and development of novel perovskite precursor ink formulations, and it also discusses their contribution toward demonstrating efficient, scalable, and durable PSC technology to create electricity and energize futuristic applications. Various reports were included aiming to showcase the robust photovoltaic performance of large-area perovskite solar modules in a variety of device configurations, hence providing a brief overview of the role of state-of-the-art scalable precursor ink development in transforming unstable lab-sized solar cells into robust, low-cost perovskite solar cell technology that can be scaled up to cover much larger areas

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

Included in the dataset are detailed information into the crystallography, morphology, electronic properties, (photo)electrochemical and carrier dynamics of both single-crystal Cu2O thin films and polycrystalline Cu2O with favored crystal orientations. Multiple intruments, including Empyrean X-ray Diffractometer, Zeiss Merlin Scanning Electron Microscope, Tecnai Osiris Transmission Electron Micrisocope, Newport LCS-100 Solar Simulator, Biologic SP-200, GC9790plus Gas Chromatograph, Keithley 2450 SourceMeter, Shimadzu UV-3600 Plus Double-beam Spectrophotometer, were applied to collect the data. Abstract of associated publication: 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] orientation was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm−2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.European Research Council (HYPERION, grant 756962) Engineering and Physical Sciences Research Council (grant H2CAT, EP/V012932/1) Swiss National Science Foundation (P2ELP2_195109) Engineering and Physical Sciences Research Council (EP/ T001038/1) UK Research and Innovation (EP/X022986/1) St John’s College Cambridge (Title A) European Research Council (MatEnSAP, 682833) UK Research and Innovation (EP/X030563/1) National Natural Science Foundation of China (52072187, 22122903) National Key Research and Development Program of China (019YFE0123400) Royal Society and Tata Group (UF150033

High carrier mobility along the [111] orientation in Cu2O photoelectrodes

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3,4,5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. 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] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm−2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h.Correction in: Nature, vol. 629, article-ID E14DOI: 10.1038/s41586-024-07489-8</p

High carrier mobility along the [111] orientation in Cu2O photoelectrodes.

Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3-5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. 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] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm-2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h

High carrier mobility along the [111] orientation in Cu2O photoelectrodes.

Acknowledgements: The work was supported by funding from the European Research Council (ERC; HYPERION, grant 756962) and the Engineering and Physical Sciences Research Council (grant H2CAT, EP/V012932/1). L.P. acknowledges funding from the Swiss National Science Foundation under the Early Postdoc.Mobility fellowship (P2ELP2_195109). O.J.B. and S.H. acknowledge funding from the Engineering and Physical Sciences Research Council (EP/T001038/1). L.C. acknowledges funding from UK Research and Innovation-funded Postdoctoral Fellowships (Horizon Europe MSCA Postdoctoral Fellowships in the UK; EP/X022986/1). V.A. acknowledges financial support from St John’s College Cambridge (Title A Research Fellowship) and the Winton Programme for the Physics of Sustainability. A.A. acknowledges funding from the Royal Society. T.C.-J.Y acknowledges the support of the MSCA Individual Fellowship from the European Union’s Horizon 2020 (PeTSoC, No. 891205). E.R. was supported by an ERC Consolidator Grant (MatEnSAP, grant 682833) and a UK Research and Innovation–ERC Advanced Grant (EP/X030563/1). Y.Z. and H.S. acknowledge financial support from the EPSRC Centre for Doctoral Training in Graphene Technology, the Royal Society (RP/R1/201082) and the Engineering and Physical Sciences Research Council (EP/W017091/1). J.L. acknowledges funding from the National Natural Science Foundation of China (grant numbers 52072187 and 22122903) and the National Key Research and Development Program of China (grant number 2019YFE0123400). S.D.S. acknowledges the Royal Society and Tata Group (UF150033). We thank Y. Huang for assisting with the space-charge-limited current measurement, and Z. Liang for helping with the cross-sectional transmission electron microscopy imaging. For the purpose of open access, the authors have applied a Creative Commons Attribution (CC BY) licence to any author accepted manuscript version arising from this submission.Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3-5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. 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] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm-2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h

High carrier mobility along the [111] orientation in Cu2O photoelectrodes.

Acknowledgements: The work was supported by funding from the European Research Council (ERC; HYPERION, grant 756962) and the Engineering and Physical Sciences Research Council (grant H2CAT, EP/V012932/1). L.P. acknowledges funding from the Swiss National Science Foundation under the Early Postdoc.Mobility fellowship (P2ELP2_195109). O.J.B. and S.H. acknowledge funding from the Engineering and Physical Sciences Research Council (EP/T001038/1). L.C. acknowledges funding from UK Research and Innovation-funded Postdoctoral Fellowships (Horizon Europe MSCA Postdoctoral Fellowships in the UK; EP/X022986/1). V.A. acknowledges financial support from St John’s College Cambridge (Title A Research Fellowship) and the Winton Programme for the Physics of Sustainability. A.A. acknowledges funding from the Royal Society. T.C.-J.Y acknowledges the support of the MSCA Individual Fellowship from the European Union’s Horizon 2020 (PeTSoC, No. 891205). E.R. was supported by an ERC Consolidator Grant (MatEnSAP, grant 682833) and a UK Research and Innovation–ERC Advanced Grant (EP/X030563/1). Y.Z. and H.S. acknowledge financial support from the EPSRC Centre for Doctoral Training in Graphene Technology, the Royal Society (RP/R1/201082) and the Engineering and Physical Sciences Research Council (EP/W017091/1). J.L. acknowledges funding from the National Natural Science Foundation of China (grant numbers 52072187 and 22122903) and the National Key Research and Development Program of China (grant number 2019YFE0123400). S.D.S. acknowledges the Royal Society and Tata Group (UF150033). We thank Y. Huang for assisting with the space-charge-limited current measurement, and Z. Liang for helping with the cross-sectional transmission electron microscopy imaging. For the purpose of open access, the authors have applied a Creative Commons Attribution (CC BY) licence to any author accepted manuscript version arising from this submission.Solar fuels offer a promising approach to provide sustainable fuels by harnessing sunlight1,2. Following a decade of advancement, Cu2O photocathodes are capable of delivering a performance comparable to that of photoelectrodes with established photovoltaic materials3-5. However, considerable bulk charge carrier recombination that is poorly understood still limits further advances in performance6. 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] direction was found to be an order of magnitude higher than those along other orientations. Driven by these findings, we developed a polycrystalline Cu2O photocathode with an extraordinarily pure (111) orientation and (111) terminating facets using a simple and low-cost method, which delivers 7 mA cm-2 current density (more than 70% improvement compared to that of state-of-the-art electrodeposited devices) at 0.5 V versus a reversible hydrogen electrode under air mass 1.5 G illumination, and stable operation over at least 120 h