Imperial College London

Dr Alex Ganose

Faculty of Natural SciencesDepartment of Chemistry

Lecturer in Chemistry
 
 
 
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Contact

 

a.ganose Website

 
 
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Location

 

301EMolecular Sciences Research HubWhite City Campus

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Summary

 

Publications

Publication Type
Year
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72 results found

Moore GC, Horton MK, Linscott E, Ganose AM, Siron M, O'Regan DD, Persson KAet al., 2024, High-throughput determination of Hubbard U and Hund J values for transition metal oxides via the linear response formalism, Physical Review Materials, Vol: 8

DFT+U provides a convenient, cost-effective correction for the self-interaction error (SIE) that arises when describing correlated electronic states using conventional approximate density functional theory (DFT). The success of a DFT+U(+J) calculation hinges on the accurate determination of its Hubbard U and Hund J parameters, and the linear response (LR) methodology has proven to be computationally effective and accurate for calculating these parameters. This study provides a high-throughput computational analysis of the U and J values for transition metal d-electron states in a representative set of over 1000 magnetic transition metal oxides (TMOs), providing a frame of reference for researchers who use DFT+U to study transition metal oxides. In order to perform this high-throughput study, an atomate workflow is developed for calculating U and J values automatically on massively parallel supercomputing architectures. To demonstrate an application of this workflow, the spin-canting magnetic structure and unit cell parameters of the multiferroic olivine LiNiPO4 are calculated using the computed Hubbard U and Hund J values for Ni-d and O-p states, and are compared with experiment. Both the Ni-dU and J corrections have a strong effect on the Ni-moment canting angle. Additionally, including a O-pU value results in a significantly improved agreement between the computed lattice parameters and experiment.

Journal article

Wu R, Ganose AM, 2024, Tilt-induced charge localisation in phosphide antiperovskite photovoltaics, JPhys Materials, Vol: 7

Antiperovskites are a rich family of compounds with applications in battery cathodes, superconductors, solid-state lighting, and catalysis. Recently, a novel series of antimonide phosphide antiperovskites (A 3SbP, where A = Ca, Sr Ba) were proposed as candidate photovoltaic absorbers due to their ideal band gaps, small effective masses and strong optical absorption. In this work, we explore this series of compounds in more detail using relativistic hybrid density functional theory. We reveal that the proposed cubic structures are dynamically unstable and instead identify a tilted orthorhombic Pnma phase as the ground state. Tilting is shown to induce charge localisation that widens the band gap and increases the effective masses. Despite this, we demonstrate that the predicted maximum photovoltaic efficiencies remain high (24%-31% for 200 nm thin films) by bringing the band gaps into the ideal range for a solar absorber. Finally, we assess the band alignment of the series and suggest hole and electron contact materials for efficient photovoltaic devices.

Journal article

Hu X, Borowiec J, Zhu Y, Liu X, Wu R, Ganose AM, Parkin IP, Boruah BDet al., 2023, Dendrite-free zinc anodes enabled by exploring polar-face-rich 2D ZnO interfacial layers for rechargeable Zn-ion batteries, Small, ISSN: 1613-6810

Zinc metal is a promising candidate for anodes in zinc-ion batteries (ZIBs), but its widespread implementation is hindered by dendrite growth in aqueous electrolytes. Dendrites lead to undesirable side reactions, such as hydrogen evolution, passivation, and corrosion, causing reduced capacity during prolonged cycling. In this study, an approach is explored to address this challenge by directly growing 1D zinc oxide (ZnO) nanorods (NRs) and 2D ZnO nanoflakes (NFs) on Zn anodes, forming artificial layers to enhance ZIB performance. The incorporation of ZnO on the anode offers both chemical and thermal stability and leverages its n-type semiconductor nature to facilitate the formation of ohmic contacts. This results in efficient electron transport during Zn ion plating and stripping processes. Consequently, the ZnO NFs-coated Zn anodes demonstrate significantly improved charge storage performance, achieving 348 mAh g-1 , as compared to ZnO NRs (250 mAh g-1 ) and pristine Zn (160 mAh g-1 ) anodes when evaluated in full cells with V2 O5 cathodes. One significant advantage of ZnO NFs lies in their highly polar surfaces, promoting strong interactions with water molecules and rendering them exceptionally hydrophilic. This characteristic enhances the ability of ZnO NFs to desolvate Zn2+ ions, leading to improved charge storage performance.

Journal article

Lu Y, Andersen H, Wu R, Ganose AM, Wen B, Pujari A, Wang T, Borowiec J, Parkin IP, De Volder M, Boruah BDet al., 2023, Hydrogenated V2 O5 with Improved Optical and Electrochemical Activities for Photo-Accelerated Lithium-Ion Batteries., Small

Solar power represents an abundant and readily available source of renewable energy. However, its intermittent nature necessitates external energy storage solutions, which can often be expensive, bulky, and associated with energy conversion losses. This study introduces the concept of a photo-accelerated battery that seamlessly integrates energy harvesting and storage functions within a single device. In this research, a novel approach for crafting photocathodes is presented using hydrogenated vanadium pentoxide (H:V2 O5 ) nanofibers. This method enhances optical activity, electronic conductivity, and ion diffusion rates within photo-accelerated Li-ion batteries. This study findings reveal that H:V2 O5 exhibits notable improvements in specific capacity under both dark and illuminated conditions. Furthermore, it demonstrates enhanced diffusion kinetics and charge storage performance when exposed to light, as compared to pristine counterparts. This strategy of defect engineering holds great promise for the development of high-performance photocathodes in future energy storage applications.

Journal article

Wang X, Li Z, Kavanagh SR, Ganose AM, Walsh Aet al., 2023, Correction: Lone pair driven anisotropy in antimony chalcogenide semiconductors, Physical Chemistry Chemical Physics, Vol: 25, Pages: 25055-25055, ISSN: 1463-9076

Correction for 'Lone pair driven anisotropy in antimony chalcogenide semiconductors' by Xinwei Wang et al., Phys. Chem. Chem. Phys., 2022, 24, 7195-7202, https://doi.org/10.1039/D1CP05373F.

Journal article

Wu R, Ganose AM, 2023, Relativistic electronic structure and photovoltaic performance of K<inf>2</inf>CsSb, Journal of Materials Chemistry A, Vol: 11, Pages: 21636-21644, ISSN: 2050-7488

The discovery of an efficient and cost-effective photovoltaic absorber is urgently needed to meet global emission targets. Antimony-based materials have emerged as promising non-toxic and earth-abundant candidates with similar electronic properties to the lead hybrid perovskites. The full-Heusler K2CsSb has been widely studied as a photocathode and thermoelectric material but has not been evaluated as a potential photovoltaic absorber. Here, using relativistic hybrid density functional theory, we demonstrate that K2CsSb exhibits ideal properties for use in photovoltaic applications, based on its bandgap, dispersive conduction band, and strong optical absorption. Using a detailed balance approach, we reveal the maximum theoretical efficiency to be competitive with other state-of-the-art photovoltaics, reaching over 28 percent at a thickness of 200 nm. Additionally, we perform band-alignment calculations to provide recommendations for suitable device architectures that will minimise contact losses.

Journal article

Wu R, Ganose AM, 2023, Relativistic electronic structure and photovoltaic performance of K<sub>2</sub>CsSb, JOURNAL OF MATERIALS CHEMISTRY A, ISSN: 2050-7488

Journal article

Woods-Robinson R, Xiong Y, Shen J-X, Winner N, Horton MK, Asta M, Ganose AM, Hautier G, Persson KAet al., 2023, Designing transparent conductors using forbidden optical transitions, MATTER, Vol: 6, Pages: 3021-3039, ISSN: 2590-2393

Journal article

Huang J, Shin S-J, Tolborg K, Ganose A, Krenzer G, Walsh Aet al., 2023, Room-temperature stacking disorder in layered covalent-organic frameworks from machine-learning force fields, MATERIALS HORIZONS, Vol: 10, Pages: 2883-2891, ISSN: 2051-6347

Journal article

Li Z, Park J-S, Ganose AMM, Walsh Aet al., 2023, From Cubic to Hexagonal: Electronic Trends across Metal Halide Perovskite Polytypes, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 127, Pages: 12695-12701, ISSN: 1932-7447

Journal article

Jackson AJ, Parrett BJ, Willis J, Ganose AM, Leung WWW, Liu Y, Williamson BAD, Kim TK, Hoesch M, Veiga LSI, Kalra R, Neu J, Schmuttenmaer CA, Lee T-L, Regoutz A, Lee T-C, Veal TD, Palgrave RG, Perry R, Scanlon DOet al., 2022, Computational Prediction and Experimental Realization of Earth-Abundant Transparent Conducting Oxide Ga-Doped ZnSb2O6, ACS ENERGY LETTERS, Vol: 7, Pages: 3807-3816, ISSN: 2380-8195

Journal article

Andreasen JW, Bowers JW, Breternitz J, Dale PJ, Dimitrievska M, Fermin DJ, Ganose A, Gurieva G, Hages CJ, Hawkins C, Hobson TDC, Jaramillo R, Kavanagh SR, Major JD, Mandati S, Mitzi DB, Naylor MC, Bjorkman CP, Scanlon DO, Schorr S, Scragg JJS, Shin B, Siebentritt S, Sood M, Sopiha K, Sutton M, Tiwari D, Unold T, Valdes M, Wang M, Weiss TP, Woods-Robinson Ret al., 2022, Indium-free CIGS analogues: general discussion, FARADAY DISCUSSIONS, Vol: 239, Pages: 85-111, ISSN: 1359-6640

Journal article

Agbenyeke R, Andreasen JW, Benhaddou N, Bowers JW, Breternitz J, Bar M, Dimitrievska M, Fermin DJ, Ganose A, Hawkins C, Jaramillo R, Kavanagh SR, Kondrotas R, Major JD, Mandati S, Nicolson A, Bjorkman CP, Savory C, Scanlon DO, Schorr S, Scragg JJS, Sheppard A, Shin B, Siebentritt S, Sood M, Sopiha K, Spalatu N, Tang J, Walsh A, Weiss TP, Woods-Robinson R, Yetkin HAet al., 2022, Materials design and bonding: general discussion, FARADAY DISCUSSIONS, Vol: 239, Pages: 375-404, ISSN: 1359-6640

Journal article

Andreasen JW, Arca E, Bowers JW, Bar M, Breternitz J, Dale PJ, Dimitrievska M, Fermin DJ, Ganose A, Hages CJ, Hobson T, Jaramillo R, Kavanagh SR, Kayastha P, Kondrotas R, Lee J, Major JD, Mandati S, Mitzi DB, Scanlon DO, Schorr S, Scragg JJS, Shin B, Siebentritt S, Smiles M, Sood M, Sopiha K, Spalatu N, Sutton M, Unold T, Valdes M, Walsh A, Wang M, Wang X, Weiss TP, Woo YW, Woods-Robinson R, Tiwari Det al., 2022, Novel chalcogenides, pnictides and defect-tolerant semiconductors: general discussion, FARADAY DISCUSSIONS, Vol: 239, Pages: 287-316, ISSN: 1359-6640

Journal article

Tolborg K, Klarbring J, Ganose AM, Walsh Aet al., 2022, Free energy predictions for crystal stability and synthesisability, Digital Discovery, Vol: 1, Pages: 586-595

What is the likelihood that a hypothetical material—the combination of a composition and crystal structure—can be formed? Underpinning the reliability of predictions for local or global crystal stability is the choice of thermodynamic potential. Here, we discuss recent advances in free energy descriptions for crystals including both harmonic and anharmonic phonon contributions to the vibrational entropy. We critically discuss some of the techniques and descriptors, including data-driven machine learning approaches, being developed to assess the stability and synthesisability of solids. Avenues are highlighted that deserve further attention including thermodynamic and kinetic factors that govern the accessibility of metastable structures away from equilibrium.

Journal article

Wang X, Ganose AM, Kavanagh SR, Walsh Aet al., 2022, Band versus Polaron: Charge Transport in Antimony Chalcogenides, ACS ENERGY LETTERS, Vol: 7, Pages: 2954-2960, ISSN: 2380-8195

Journal article

Ganose A, Scanlon D, Walsh A, Hoye Ret al., 2022, The defect challenge of wide-bandgap semiconductors for photovoltaics and beyond, Nature Communications, Vol: 13, ISSN: 2041-1723

The optoelectronic performance of wide-bandgap semiconductors often cannot compete with that of their defect-tolerant small-bandgap counterpart. Here, the authors outline three main challenges to overcome for mitigating the impact of defects in wide-bandgap semiconductors.

Journal article

Huang J, Golomb MJ, Kavanagh SR, Tolborg K, Ganose AM, Walsh Aet al., 2022, Band gap opening from displacive instabilities in layered covalent-organic frameworks, Journal of Materials Chemistry A, Vol: 10, Pages: 13500-13507, ISSN: 2050-7488

Covalent organic frameworks (COFs) offer a high degree of chemical and structural flexibility. There is a large family of COFs built from 2D sheets that are stacked to form extended crystals. While it has been common to represent the stacking as eclipsed with one repeating layer (“AA”), there is growing evidence that a more diverse range of stacking sequences is accessible. Herein, we report a computational study using density functional theory of layer stacking in two prototypical COFs, Tp-Azo and DAAQ-TFP, which have shown high performance as Li-ion battery electrodes. We find a striking preference for slipped structures with horizontal offsets between layers ranging from 1.7 Å to 3.5 Å in a potential energy minimum that forms a low energy ring. The associated symmetry breaking results in a pronounced change in the underlying electronic structure. A band gap opening of 0.8–1.4 eV is found due to modifications of the underlying valence and conduction band dispersion as explained from changes in the π orbital overlap. The implications for the screening and selection of COF for energy applications are discussed.

Journal article

Tolborg K, Klarbring J, Ganose AM, Walsh Aet al., 2022, Free energy predictions for crystal stability and synthesisability

<jats:p>What is the likelihood that a hypothetical material - the combination of a composition and crystal structure - can be formed? Underpinning the reliability of predictions for local or global crystal stability is the choice of thermodynamic potential. Here, we discuss recent advances in free energy descriptions for crystals including both harmonic and anharmonic phonon contributions to the vibrational entropy. We critically discuss some of the techniques and descriptors, including data-driven machine learning approaches, being developed to assess the stability and synthesisability of solids. Avenues are highlighted that deserve further attention including thermodynamic and kinetic factors that govern the accessibility of metastable structures away from equilibrium.</jats:p>

Journal article

Toriyama MY, Ganose AM, Dylla M, Anand S, Park J, Brod MK, Munro JM, Persson KA, Jain A, Snyder GJet al., 2022, How to analyse a density of states, Materials Today Electronics, Vol: 1

The density of states of electrons is a simple, yet highly-informative, summary of the electronic structure of a material. Here, some remarkable features of the electronic structure that are perceptible from the density of states are concisely reviewed, notably the analytical E vs. k dispersion relation near the band edges, effective mass, Van Hove singularities, and the effective dimensionality of the electrons, all of which have a strong influence on physical properties of materials. We emphasize that appropriate parameters in electronic structure calculations are necessary to obtain even a sufficient-quality density of states exhibiting fine features of the electronic structure.

Journal article

Wang X, Li Z, Kavanagh S, Ganose A, Walsh Aet al., 2022, Lone pair driven anisotropy in antimony chalcogenide semiconductors, Physical Chemistry Chemical Physics, Vol: 2022, ISSN: 1463-9076

Antimony sulfide (Sb2S3) and selenide (Sb2Se3) have emerged as promising earth-abundant alternatives among thin-film photovoltaic compounds. A distinguishing feature of these materials is their anisotropic crystal structures, which are composed of quasi-one-dimensional (1D) [Sb4X6]n ribbons. The interaction between ribbons has been reported to be van der Waals (vdW) in nature and Sb2X3 are thus commonly classified in the literature as 1D semiconductors. However, based on first-principles calculations, here we show that inter-ribbon interactions are present in Sb2X3 beyond the vdW regime. The origin of the anisotropic structures is related to the stereochemical activity of the Sb 5s lone pair according to electronic structure analysis. The impacts of structural anisotropy on the electronic, dielectric and optical properties relevant to solar cells are further examined, including the presence of higher dimensional Fermi surfaces for charge carrier transport. Our study provides guidelines for optimising the performance of Sb2X3-based photovoltaics via device structuring based on the underlying crystal anisotropy.

Journal article

Spooner KB, Ganose AM, Leung WWW, Buckeridge J, Williamson BAD, Palgrave RG, Scanlon DOet al., 2021, BaBi<sub>2</sub>O<sub>6</sub>: A Promising n-Type Thermoelectric Oxide with the PbSb<sub>2</sub>O<sub>6</sub> Crystal Structure, CHEMISTRY OF MATERIALS, Vol: 33, Pages: 7441-7456, ISSN: 0897-4756

Journal article

Pan H, Ganose AM, Horton M, Aykol M, Persson K, Zimmermann NER, Jain Aet al., 2021, Benchmarking Coordination Number Prediction Algorithms on Inorganic Crystal Structures (vol 60, pg 1590, 2021), INORGANIC CHEMISTRY, Vol: 60, Pages: 7590-7590, ISSN: 0020-1669

Journal article

Shi X, Zhang X, Ganose A, Park J, Sun C, Chen Z, Lin S, Li W, Jain A, Pei Yet al., 2021, Compromise between band structure and phonon scattering in efficient n-Mg<sub>3</sub>Sb<sub>2-<i>x</i></sub>Bi<i><sub>x</sub></i> thermoelectrics, MATERIALS TODAY PHYSICS, Vol: 18, ISSN: 2542-5293

Journal article

Ganose AM, Park J, Faghaninia A, Woods-Robinson R, Persson KA, Jain Aet al., 2021, Efficient calculation of carrier scattering rates from first principles, Nature Communications, Vol: 12, Pages: 1-9, ISSN: 2041-1723

The electronic transport behaviour of materials determines their suitability for technological applications. We develop a computationally efficient method for calculating carrier scattering rates of solid-state semiconductors and insulators from first principles inputs. The present method extends existing polar and non-polar electron-phonon coupling, ionized impurity, and piezoelectric scattering mechanisms formulated for isotropic band structures to support highly anisotropic materials. We test the formalism by calculating the electronic transport properties of 23 semiconductors, including the large 48 atom CH3NH3PbI3 hybrid perovskite, and comparing the results against experimental measurements and more detailed scattering simulations. The Spearman rank coefficient of mobility against experiment (rs = 0.93) improves significantly on results obtained using a constant relaxation time approximation (rs = 0.52). We find our approach offers similar accuracy to state-of-the art methods at approximately 1/500th the computational cost, thus enabling its use in high-throughput computational workflows for the accurate screening of carrier mobilities, lifetimes, and thermoelectric power.

Journal article

Toriyama MY, Ganose AM, Dylla M, Anand S, Park J, Brod MK, Munro J, Persson KA, Jain A, Snyder GJet al., 2021, Comparison of the tetrahedron method to smearing methods for the electronic density of states, Publisher: arXiv

The electronic density of states (DOS) highlights fundamental properties ofmaterials that oftentimes dictate their properties, such as the band gap andVan Hove singularities. In this short note, we discuss how sharp features ofthe density of states can be obscured by smearing methods (such as the Gaussianand Fermi smearing methods) when calculating the DOS. While the common approachto reach a "converged" density of states of a material is to increase thediscrete k-point mesh density, we show that the DOS calculated by smearingmethods can appear to converge but not to the correct DOS. Employing thetetrahedron method for Brillouin zone integration resolves key features of thedensity of states far better than smearing methods.

Working paper

Pan H, Ganose AM, Horton M, Aykol M, Persson KA, Zimmermann NER, Jain Aet al., 2021, Benchmarking Coordination Number Prediction Algorithms on Inorganic Crystal Structures, INORGANIC CHEMISTRY, Vol: 60, Pages: 1590-1603, ISSN: 0020-1669

Journal article

Pohls J-H, Chanakian S, Park J, Ganose AM, Dunn A, Friesen N, Bhattacharya A, Hogan B, Bux S, Jain A, Mar A, Zevalkink Aet al., 2021, Experimental validation of high thermoelectric performance in RECuZnP<sub>2</sub> predicted by high-throughput DFT calculations, MATERIALS HORIZONS, Vol: 8, Pages: 209-215, ISSN: 2051-6347

Journal article

Mattei GS, Dagdelen JM, Bianchini M, Ganose AM, Jain A, Suard E, Fauth F, Masquelier C, Croguennec L, Ceder G, Persson KA, Khalifah PGet al., 2020, Enumeration as a Tool for Structure Solution: A Materials Genomic Approach to Solving the Cation-Ordered Structure of Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>2</sub>F<sub>3</sub>, CHEMISTRY OF MATERIALS, Vol: 32, Pages: 8981-8992, ISSN: 0897-4756

Journal article

Dunn A, Wang Q, Ganose A, Dopp D, Jain Aet al., 2020, Benchmarking materials property prediction methods: the Matbench test set and Automatminer reference algorithm (Sep, 10.1038/s41524-020-00406-3, 2020), NPJ COMPUTATIONAL MATERIALS, Vol: 6

Journal article

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