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

Nature

Published On 2024/4/25

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 …

Journal

Nature

Published On

2024/4/25

Volume

628

Issue

8,009

Page

765-770

Authors

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Position

Professor

H-Index(all)

299

H-Index(since 2020)

170

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Solar energy conversion

Anders Hagfeldt

Anders Hagfeldt

École Polytechnique Fédérale de Lausanne

Position

Professor of Physical Chemistry EPFL

H-Index(all)

170

H-Index(since 2020)

113

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

solar cells

photoelectrochemistry

solar fuel

dye-sensitized

perovskite solar cells

Professor Sam Stranks

Professor Sam Stranks

University of Cambridge

Position

University Lecturer in Energy

H-Index(all)

86

H-Index(since 2020)

79

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Perovskite Solar Cells

Light-Emitting Diodes

Organic Photovoltaics

Time-Resolved Spectroscopy

Carbon Nanotubes

University Profile Page

Erwin Reisner

Erwin Reisner

University of Cambridge

Position

Department of Chemistry

H-Index(all)

85

H-Index(since 2020)

67

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Artificial Photosynthesis

Solar-driven Chemistry

Solar Fuels

Photosynthesis

Hybrid photocatalysis

University Profile Page

Stephan Hofmann

Stephan Hofmann

University of Cambridge

Position

Professor of Nanotechnology UK

H-Index(all)

77

H-Index(since 2020)

54

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Nanomaterials

Materials Science

Semiconductor Engineering

In-situ Metrology

Electronic Material Synthesis

University Profile Page

Jingshan Luo

Jingshan Luo

Nankai University

Position

Professor

H-Index(all)

69

H-Index(since 2020)

57

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Solar energy conversion

Electrocatalysis

Photoelectrocatalysis

University Profile Page

Kyle Frohna

Kyle Frohna

University of Cambridge

Position

H-Index(all)

21

H-Index(since 2020)

21

I-10 Index(all)

0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Materials Science

Nanoscience

Photovoltaics

DFT

University Profile Page

Virgil Andrei

Virgil Andrei

University of Cambridge

Position

Research Fellow

H-Index(all)

21

H-Index(since 2020)

20

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0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

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0

Research Interests

Solar Fuels

Photovoltaics

Thermoelectrics

University Profile Page

Linfeng Pan

Linfeng Pan

University of Cambridge

Position

H-Index(all)

19

H-Index(since 2020)

19

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0

I-10 Index(since 2020)

0

Citation(all)

0

Citation(since 2020)

0

Cited By

0

Research Interests

Solar Fuels

Solar Cells

Electrocatalysis

Spectroscopy

University Profile Page

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Erwin Reisner

Erwin Reisner

University of Cambridge

Research data supporting" Photocatalytic CO2 Reduction using Homogeneous Carbon Dots with a Molecular Cobalt Catalyst"

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.

Michael Graetzel

Michael Graetzel

École Polytechnique Fédérale de Lausanne

Advanced Materials

Buried‐Interface Engineering Enables Efficient and 1960‐Hour ISOS‐L‐2I Stable Inverted Perovskite Solar Cells

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 …

Anders Hagfeldt

Anders Hagfeldt

École Polytechnique Fédérale de Lausanne

Nature Energy

Multifunctional sulfonium-based treatment for perovskite solar cells with less than 1% efficiency loss over 4,500-h operational stability tests

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.

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Nankai University

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Phenyltrimethylammonium Chloride Additive for Highly Efficient and Stable FAPbI3 Perovskite Solar Cells

Formamidinium lead triiodide (FAPbI3)-rich perovskite absorbers have emerged as the frontrunners for the development of perovskite solar cells (PSCs), but pristine FAPbI3 absorber exhibits phase instability because of external stressors during device manufacture and operation. In this work, we systematically study the function of a trace amount of phenyltrimethylammonium chloride (PTAC) additive in FAPbI3-based perovskites. The introduced PTAC have a strong electrostatic interaction with perovskite because of the coordination of electron-rich benzene ring unit and under-coordinated Pb2+, which leads to the decrease of the trap density and the release of the lattice strain. Simultaneously, the increased work function of modulated film optimizes the band alignment, promoting carrier transport and reducing nonradiative recombination, thereby improving the open-circuit voltages and fill factors. Consequently, the …

Erwin Reisner

Erwin Reisner

University of Cambridge

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

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.

Stephan Hofmann

Stephan Hofmann

University of Cambridge

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Probing post-growth hydrogen intercalation and H2 nanobubbles formation in graphene on Ge (110)

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).

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University of Cambridge

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Dynamic local structure in caesium lead iodide: Spatial correlation and transient domains

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 …

Professor Sam Stranks

Professor Sam Stranks

University of Cambridge

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Multifunctional sulfonium-based treatment for perovskite solar cells with less than 1% efficiency loss over 4,500-h operational stability tests

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.

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University of Cambridge

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Professor Sam Stranks

University of Cambridge

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

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.

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Michael Graetzel

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École Polytechnique Fédérale de Lausanne

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Ulsan National Institute of Science and Technology

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Nature

Multisensory gamma stimulation promotes glymphatic clearance of amyloid

The glymphatic movement of fluid through the brain removes metabolic waste, , –. Noninvasive 40 Hz stimulation promotes 40 Hz neural activity in multiple brain regions and attenuates pathology in mouse models of Alzheimer’s disease, , –. Here we show that multisensory gamma stimulation promotes the influx of cerebrospinal fluid and the efflux of interstitial fluid in the cortex of the 5XFAD mouse model of Alzheimer’s disease. Influx of cerebrospinal fluid was associated with increased aquaporin-4 polarization along astrocytic endfeet and dilated meningeal lymphatic vessels. Inhibiting glymphatic clearance abolished the removal of amyloid by multisensory 40 Hz stimulation. Using chemogenetic manipulation and a genetically encoded sensor for neuropeptide signalling, we found that vasoactive intestinal peptide interneurons facilitate glymphatic clearance by regulating arterial pulsatility. Our findings …

Ashot Margaryan

Ashot Margaryan

Københavns Universitet

Nature

Population genomics of post-glacial western Eurasia

Western Eurasia witnessed several large-scale human migrations during the Holocene, , , –. Here, to investigate the cross-continental effects of these migrations, we shotgun-sequenced 317 genomes—mainly from the Mesolithic and Neolithic periods—from across northern and western Eurasia. These were imputed alongside published data to obtain diploid genotypes from more than 1,600 ancient humans. Our analyses revealed a ‘great divide’ genomic boundary extending from the Black Sea to the Baltic. Mesolithic hunter-gatherers were highly genetically differentiated east and west of this zone, and the effect of the neolithization was equally disparate. Large-scale ancestry shifts occurred in the west as farming was introduced, including near-total replacement of hunter-gatherers in many areas, whereas no substantial ancestry shifts happened east of the zone during the same period. Similarly, relatedness …

Clary Clish

Clary Clish

Harvard University

Nature

Reverse metabolomics for the discovery of chemical structures from humans

Determining the structure and phenotypic context of molecules detected in untargeted metabolomics experiments remains challenging. Here we present reverse metabolomics as a discovery strategy, whereby tandem mass spectrometry spectra acquired from newly synthesized compounds are searched for in public metabolomics datasets to uncover phenotypic associations. To demonstrate the concept, we broadly synthesized and explored multiple classes of metabolites in humans, including N-acyl amides, fatty acid esters of hydroxy fatty acids, bile acid esters and conjugated bile acids. Using repository-scale analysis,, we discovered that some conjugated bile acids are associated with inflammatory bowel disease (IBD). Validation using four distinct human IBD cohorts showed that cholic acids conjugated to Glu, Ile/Leu, Phe, Thr, Trp or Tyr are increased in Crohn’s disease. Several of these compounds and …

Mingyao Li

Mingyao Li

University of Pennsylvania

Nature

An atlas of epithelial cell states and plasticity in lung adenocarcinoma

Understanding the cellular processes that underlie early lung adenocarcinoma (LUAD) development is needed to devise intervention strategies. Here we studied 246,102 single epithelial cells from 16 early-stage LUADs and 47 matched normal lung samples. Epithelial cells comprised diverse normal and cancer cell states, and diversity among cancer cells was strongly linked to LUAD-specific oncogenic drivers. KRAS mutant cancer cells showed distinct transcriptional features, reduced differentiation and low levels of aneuploidy. Non-malignant areas surrounding human LUAD samples were enriched with alveolar intermediate cells that displayed elevated KRT8 expression (termed KRT8+ alveolar intermediate cells (KACs) here), reduced differentiation, increased plasticity and driver KRAS mutations. Expression profiles of KACs were enriched in lung precancer cells and in LUAD cells and signified poor survival …

Esther García-Domínguez

Esther García-Domínguez

Universidad de Valencia

Nature

Multimodal cell atlas of the ageing human skeletal muscle

Muscle atrophy and functional decline (sarcopenia) are common manifestations of frailty and are critical contributors to morbidity and mortality in older people. Deciphering the molecular mechanisms underlying sarcopenia has major implications for understanding human ageing. Yet, progress has been slow, partly due to the difficulties of characterizing skeletal muscle niche heterogeneity (whereby myofibres are the most abundant) and obtaining well-characterized human samples,. Here we generate a single-cell/single-nucleus transcriptomic and chromatin accessibility map of human limb skeletal muscles encompassing over 387,000 cells/nuclei from individuals aged 15 to 99 years with distinct fitness and frailty levels. We describe how cell populations change during ageing, including the emergence of new populations in older people, and the cell-specific and multicellular network features (at the transcriptomic …

Deborah Doroshow

Deborah Doroshow

Yale University

Nature

An IL-4 signalling axis in bone marrow drives pro-tumorigenic myelopoiesis

Myeloid cells are known to suppress antitumour immunity. However, the molecular drivers of immunosuppressive myeloid cell states are not well defined. Here we used single-cell RNA sequencing of human and mouse non-small cell lung cancer (NSCLC) lesions, and found that in both species the type 2 cytokine interleukin-4 (IL-4) was predicted to be the primary driver of the tumour-infiltrating monocyte-derived macrophage phenotype. Using a panel of conditional knockout mice, we found that only deletion of the IL-4 receptor IL-4Rα in early myeloid progenitors in bone marrow reduced tumour burden, whereas deletion of IL-4Rα in downstream mature myeloid cells had no effect. Mechanistically, IL-4 derived from bone marrow basophils and eosinophils acted on granulocyte-monocyte progenitors to transcriptionally programme the development of immunosuppressive tumour-promoting myeloid cells …

Guofan Shao

Guofan Shao

Purdue University

Nature

Urban trees: how to maximize their benefits for humans and the environment

EconPapers: Urban trees: how to maximize their benefits for humans and the environment EconPapers Economics at your fingertips EconPapers Home About EconPapers Working Papers Journal Articles Books and Chapters Software Components Authors JEL codes New Economics Papers Advanced Search EconPapers FAQ Archive maintainers FAQ Cookies at EconPapers Format for printing The RePEc blog The RePEc plagiarism page Urban trees: how to maximize their benefits for humans and the environment Lina Tang (), Guofan Shao and Peter M. Groffman Nature, 2024, vol. 626, issue 7998, 261-261 Abstract: Letter to the Editor Keywords: Policy; Sustainability; Environmental sciences (search for similar items in EconPapers) Date: 2024 References: Add references at CitEc Citations: Track citations by RSS feed Downloads: (external link) https://www.nature.com/articles/d41586-024-00300-8 Abstract (text/…

Benjamin Z. Houlton

Benjamin Z. Houlton

Cornell University

Nature

Fertilizer management for global ammonia emission reduction

Crop production is a large source of atmospheric ammonia (NH 3), which poses risks to air quality, human health and ecosystems 1, 2, 3, 4, 5. However, estimating global NH 3 emissions from croplands is subject to uncertainties because of data limitations, thereby limiting the accurate identification of mitigation options and efficacy 4, 5. Here we develop a machine learning model for generating crop-specific and spatially explicit NH 3 emission factors globally (5-arcmin resolution) based on a compiled dataset of field observations. We show that global NH 3 emissions from rice, wheat and maize fields in 2018 were 4.3±1.0 Tg N yr− 1, lower than previous estimates that did not fully consider fertilizer management practices 6, 7, 8, 9. Furthermore, spatially optimizing fertilizer management, as guided by the machine learning model, has the potential to reduce the NH 3 emissions by about 38%(1.6±0.4 Tg N yr− 1 …

Benjamin Z. Houlton

Benjamin Z. Houlton

Cornell University

Nature

Reply to: Model uncertainty obscures major driver of soil carbon

Understanding the formation and stabilization mechanisms of soil organic carbon (SOC) is important for managing land carbon (C) and mitigating climate change. Tao et al. 1 reported that microbial C use efficiency (CUE) is the primary determinant of global SOC storage and that the relative impact of plant C inputs on SOC is minor. Although soil microbes undoubtedly play an important role in SOC cycling, we are concerned about the robustness of the approach taken by Tao et al. 1. The potential biases in their analyses may lead to misleading, model-dependent results.An important piece of evidence in support of an empirical relationship between CUE and SOC stems from a meta-analysis based on 132 paired CUE and SOC measurements. Tao et al. 1 applied a linear mixed-effects model to this dataset that included CUE, mean annual temperature (MAT), soil depth and random effects and explained 55% of the …

Patricia Rios Mendoza

Patricia Rios Mendoza

Universidad Autónoma de Madrid

Nature

Population genomics of post-glacial western Eurasia

Western Eurasia witnessed several large-scale human migrations during the Holocene, , , –. Here, to investigate the cross-continental effects of these migrations, we shotgun-sequenced 317 genomes—mainly from the Mesolithic and Neolithic periods—from across northern and western Eurasia. These were imputed alongside published data to obtain diploid genotypes from more than 1,600 ancient humans. Our analyses revealed a ‘great divide’ genomic boundary extending from the Black Sea to the Baltic. Mesolithic hunter-gatherers were highly genetically differentiated east and west of this zone, and the effect of the neolithization was equally disparate. Large-scale ancestry shifts occurred in the west as farming was introduced, including near-total replacement of hunter-gatherers in many areas, whereas no substantial ancestry shifts happened east of the zone during the same period. Similarly, relatedness …