ORCID Profile
0000-0001-8337-1066
Current Organisation
University of Queensland
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Theory and Design of Materials | Condensed Matter Physics | Condensed Matter Modelling and Density Functional Theory |
Expanding Knowledge in the Physical Sciences | Expanding Knowledge in Technology
Publisher: Springer Science and Business Media LLC
Date: 18-01-2018
DOI: 10.1038/S41467-017-02670-2
Abstract: Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with material stoichiometry, is still poorly understood. Here we show that bimolecular charge-carrier recombination in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. By correctly accounting for contributions to the absorption from excitons and electron-hole continuum states, we are able to utilise the van Roosbroeck–Shockley relation to determine bimolecular recombination rate constants from absorption spectra. We show that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy. Our findings provide vital understanding of band-to-band recombination processes in this hybrid perovskite, which comprise direct, fully radiative transitions between thermalized electrons and holes.
Publisher: Wiley
Date: 22-02-2023
Abstract: Understanding collective phenomena in quantum materials from first principles is a promising route toward engineering materials properties and designing new functionalities. This work examines the quantum paraelectric state, an elusive state of matter characterized by the smooth saturation of the ferroelectric instability at low temperature due to quantum fluctuations associated with anharmonic phonon effects. The temperature‐dependent evolution of the soft ferroelectric phonon mode in the quantum paraelectric KTaO 3 in the range 0–300 K is modeled by combining density functional theory (DFT) calculations with the stochastic self‐consistent harmonic approximation assisted by an on‐the‐fly machine‐learned force field. The calculated data show that including anharmonic terms is essential to stabilize the spurious imaginary ferroelectric phonon predicted by DFT in the harmonic approximation, in agreement with experiments. Augmenting the DFT workflow with machine‐learned force fields allows for efficient stochastic s ling of the configuration space using large supercells in a wide temperature range, inaccessible to conventional ab initio protocols. This work proposes a robust computational workflow capable of accounting for collective behaviors involving different degrees of freedom and occurring at large time/length scales, paving the way for precise modeling and control of quantum effects in materials.
Publisher: American Chemical Society (ACS)
Date: 29-10-2015
Publisher: Springer Science and Business Media LLC
Date: 02-04-2020
DOI: 10.1038/S42005-020-0330-6
Abstract: Many transition metal oxides (TMOs) are Mott insulators due to strong Coulomb repulsion between electrons, and exhibit metal-insulator transitions (MITs) whose mechanisms are not always fully understood. Unlike most TMOs, minute doping in CaMnO 3 induces a metallic state without any structural transformations. This material is thus an ideal platform to explore band formation through the MIT. Here, we use angle-resolved photoemission spectroscopy to visualize how electrons delocalize and couple to phonons in CaMnO 3 . We show the development of a Fermi surface where mobile electrons coexist with heavier carriers, strongly coupled polarons. The latter originate from a boost of the electron-phonon interaction (EPI). This finding brings to light the role that the EPI can play in MITs even caused by purely electronic mechanisms. Our discovery of the EPI-induced dichotomy of the charge carriers explains the transport response of Ce-doped CaMnO 3 and suggests strategies to engineer quantum matter from TMOs.
Publisher: American Physical Society (APS)
Date: 25-02-2022
Publisher: Springer Science and Business Media LLC
Date: 08-06-2017
DOI: 10.1038/NCOMMS15769
Abstract: Transition metal oxides host a wealth of exotic phenomena ranging from charge, orbital and magnetic order to nontrivial topological phases and superconductivity. In order to translate these unique materials properties into device functionalities these materials must be doped however, the nature of carriers and their conduction mechanism at the atomic scale remain unclear. Recent angle-resolved photoelectron spectroscopy investigations provided insight into these questions, revealing that the carriers of prototypical metal oxides undergo a transition from a polaronic liquid to a Fermi liquid regime with increasing doping. Here, by performing ab initio many-body calculations of angle-resolved photoemission spectra of titanium dioxide, we show that this transition originates from non-adiabatic polar electron–phonon coupling, and occurs when the frequency of plasma oscillations exceeds that of longitudinal-optical phonons. This finding suggests that a universal mechanism may underlie polaron formation in transition metal oxides, and provides a pathway for engineering emergent properties in quantum matter.
Publisher: Springer Science and Business Media LLC
Date: 30-09-2021
DOI: 10.1038/S41524-021-00630-5
Abstract: Machine-learned interatomic potentials enable realistic finite temperature calculations of complex materials properties with first-principles accuracy. It is not yet clear, however, how accurately they describe anharmonic properties, which are crucial for predicting the lattice thermal conductivity and phase transitions in solids and, thus, shape their technological applications. Here we employ a recently developed on-the-fly learning technique based on molecular dynamics and Bayesian inference in order to generate an interatomic potential capable to describe the thermodynamic properties of zirconia, an important transition metal oxide. This machine-learned potential accurately captures the temperature-induced phase transitions below the melting point. We further showcase the predictive power of the potential by calculating the heat transport on the basis of Green–Kubo theory, which allows to account for anharmonic effects to all orders. This study indicates that machine-learned potentials trained on the fly offer a routine solution for accurate and efficient simulations of the thermodynamic properties of a vast class of anharmonic materials.
Publisher: American Physical Society (APS)
Date: 21-10-2015
Publisher: American Physical Society (APS)
Date: 16-02-2022
Publisher: American Physical Society (APS)
Date: 19-06-2019
Publisher: American Physical Society (APS)
Date: 16-09-2022
Publisher: American Chemical Society (ACS)
Date: 05-04-2023
Publisher: Elsevier BV
Date: 12-2016
Publisher: Springer International Publishing
Date: 2018
Publisher: American Physical Society (APS)
Date: 09-04-2018
Publisher: Springer Science and Business Media LLC
Date: 13-06-2018
DOI: 10.1038/S41467-018-04749-W
Abstract: Strong many-body interactions in solids yield a host of fascinating and potentially useful physical properties. Here, from angle-resolved photoemission experiments and ab initio many-body calculations, we demonstrate how a strong coupling of conduction electrons with collective plasmon excitations of their own Fermi sea leads to the formation of plasmonic polarons in the doped ferromagnetic semiconductor EuO. We observe how these exhibit a significant tunability with charge carrier doping, leading to a polaronic liquid that is qualitatively distinct from its more conventional lattice-dominated analogue. Our study thus suggests powerful opportunities for tailoring quantum many-body interactions in solids via dilute charge carrier doping.
Publisher: American Physical Society (APS)
Date: 29-09-2022
Publisher: American Physical Society (APS)
Date: 17-02-2023
Publisher: AIP Publishing
Date: 03-2029
DOI: 10.1063/5.0036097
Abstract: The hydration free energy of atoms and molecules adsorbed at liquid–solid interfaces strongly influences the stability and reactivity of solid surfaces. However, its evaluation is challenging in both experiments and theories. In this work, a machine learning aided molecular dynamics method is proposed and applied to oxygen atoms and hydroxyl groups adsorbed on Pt(111) and Pt(100) surfaces in water. The proposed method adopts thermodynamic integration with respect to a coupling parameter specifying a path from well-defined non-interacting species to the fully interacting ones. The atomistic interactions are described by a machine-learned inter-atomic potential trained on first-principles data. The free energy calculated by the machine-learned potential is further corrected by using thermodynamic perturbation theory to provide the first-principles free energy. The calculated hydration free energies indicate that only the hydroxyl group adsorbed on the Pt(111) surface attains a hydration stabilization. The observed trend is attributed to differences in the adsorption site and surface morphology.
Publisher: AIP Publishing
Date: 15-06-2020
DOI: 10.1063/5.0009491
Abstract: When determining machine-learning models for inter-atomic potentials, the potential energy surface is often described as a non-linear function of descriptors representing two- and three-body atomic distribution functions. It is not obvious how the choice of the descriptors affects the efficiency of the training and the accuracy of the final machine-learned model. In this work, we formulate an efficient method to calculate descriptors that can separately represent two- and three-body atomic distribution functions, and we examine the effects of including only two- or three-body descriptors, as well as including both, in the regression model. Our study indicates that non-linear mixing of two- and three-body descriptors is essential for an efficient training and a high accuracy of the final machine-learned model. The efficiency can be further improved by weighting the two-body descriptors more strongly. We furthermore examine a sparsification of the three-body descriptors. The three-body descriptors usually provide redundant representations of the atomistic structure, and the number of descriptors can be significantly reduced without loss of accuracy by applying an automatic sparsification using a principal component analysis. Visualization of the reduced descriptors using three-body distribution functions in real-space indicates that the sparsification automatically removes the components that are less significant for describing the distribution function.
Publisher: American Physical Society (APS)
Date: 19-06-2019
Publisher: American Physical Society (APS)
Date: 16-03-2023
Publisher: Springer Science and Business Media LLC
Date: 26-05-2016
DOI: 10.1038/NCOMMS11755
Abstract: Phonon scattering limits charge-carrier mobilities and governs emission line broadening in hybrid metal halide perovskites. Establishing how charge carriers interact with phonons in these materials is therefore essential for the development of high-efficiency perovskite photovoltaics and low-cost lasers. Here we investigate the temperature dependence of emission line broadening in the four commonly studied formamidinium and methylammonium perovskites, HC(NH 2 ) 2 PbI 3 , HC(NH 2 ) 2 PbBr 3 , CH 3 NH 3 PbI 3 and CH 3 NH 3 PbBr 3 , and discover that scattering from longitudinal optical phonons via the Fröhlich interaction is the dominant source of electron–phonon coupling near room temperature, with scattering off acoustic phonons negligible. We determine energies for the interacting longitudinal optical phonon modes to be 11.5 and 15.3 meV, and Fröhlich coupling constants of ∼40 and 60 meV for the lead iodide and bromide perovskites, respectively. Our findings correlate well with first-principles calculations based on many-body perturbation theory, which underlines the suitability of an electronic band-structure picture for describing charge carriers in hybrid perovskites.
Publisher: American Physical Society (APS)
Date: 06-10-2014
Publisher: American Physical Society (APS)
Date: 24-05-2021
Location: United Kingdom of Great Britain and Northern Ireland
Start Date: 01-2023
End Date: 01-2026
Amount: $407,600.00
Funder: Australian Research Council
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