ORCID Profile
0000-0003-1140-8485
Current Organisation
Monash University
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In Research Link Australia (RLA), "Research Topics" refer to ANZSRC FOR and SEO codes. These topics are either sourced from ANZSRC FOR and SEO codes listed in researchers' related grants or generated by a large language model (LLM) based on their publications.
Functional Materials | Condensed Matter Physics | Electronic and Magnetic Properties of Condensed Matter; Superconductivity | Atomic, Molecular, Nuclear, Particle and Plasma Physics | Materials Engineering | Nanochemistry and Supramolecular Chemistry | Quantum Optics | Surfaces and Structural Properties of Condensed Matter | Nanoscale Characterisation | Degenerate Quantum Gases and Atom Optics | Lasers and Quantum Electronics | Plasma Physics; Fusion Plasmas; Electrical Discharges | Nanoelectronics | Atomic and Molecular Physics
Expanding Knowledge in the Physical Sciences | Commercial Energy Conservation and Efficiency | Management of Greenhouse Gas Emissions from Information and Communication Services | Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in Engineering | Integrated Circuits and Devices | Expanding Knowledge in Technology |
Publisher: Springer Science and Business Media LLC
Date: 19-03-2020
DOI: 10.1038/S42005-020-0317-3
Abstract: Scanning probe microscopy (SPM) has revolutionized the fields of materials, nano-science, chemistry, and biology, by enabling mapping of surface properties and surface manipulation with atomic precision. However, these achievements require constant human supervision fully automated SPM has not been accomplished yet. Here we demonstrate an artificial intelligence framework based on machine learning for autonomous SPM operation (DeepSPM). DeepSPM includes an algorithmic search of good s le regions, a convolutional neural network to assess the quality of acquired images, and a deep reinforcement learning agent to reliably condition the state of the probe. DeepSPM is able to acquire and classify data continuously in multi-day scanning tunneling microscopy experiments, managing the probe quality in response to varying experimental conditions. Our approach paves the way for advanced methods hardly feasible by human operation (e.g., large dataset acquisition and SPM-based nanolithography). DeepSPM can be generalized to most SPM techniques, with the source code publicly available.
Publisher: Springer Science and Business Media LLC
Date: 02-2007
Publisher: The Optical Society
Date: 14-11-2016
Publisher: American Chemical Society (ACS)
Date: 20-11-2017
Publisher: Springer Science and Business Media LLC
Date: 06-10-2015
DOI: 10.1038/NCOMMS9312
Abstract: Organic semiconductor devices rely on the movement of charge at and near interfaces, making an understanding of energy level alignment at these boundaries an essential element of optimizing materials for electronic and optoelectronic applications. Here we employ low temperature scanning tunneling microscopy and spectroscopy to investigate a model system: two-dimensional nanostructures of the prototypical organic semiconductor, PTCDA (3,4,9,10-perylenetetracarboxylic dianhydride) adsorbed on NaCl (2 ML)/Ag(111). Pixel-by-pixel scanning tunneling spectroscopy allows mapping of occupied and unoccupied electronic states across these nanoislands with sub-molecular spatial resolution, revealing strong electronic differences between molecules at the edges and those in the centre, with energy level shifts of up to 400 meV. We attribute this to the change in electrostatic environment at the boundaries of clusters, namely via polarization of neighbouring molecules. The observation of these strong shifts illustrates a crucial issue: interfacial energy level alignment can differ substantially from the bulk electronic structure in organic materials.
Publisher: Wiley
Date: 12-02-2021
Abstract: Metalated phthalocyanines (Pc's) are robust and versatile molecular complexes, whose properties can be tuned by changing their functional groups and central metal atom. The electronic structure of magnesium Pc (MgPc)—structurally and electronically similar to chlorophyll—adsorbed on the Ag(100) surface is investigated by low‐temperature scanning tunneling microscopy and spectroscopy, non‐contact atomic force microscopy, and density functional theory. Single, isolated MgPc's exhibit a flat, fourfold rotationally symmetric morphology, with doubly degenerate, partially populated (due to surface‐to‐molecule electron transfer) lowest unoccupied molecular orbitals (LUMOs). In contrast, MgPc's with neighbouring molecules in proximity undergo a lift of LUMOs degeneracy, with a near‐Fermi local density of states with reduced twofold rotational symmetry, indicative of a long‐range attractive intermolecular interaction. The latter is assigned to a surface‐mediated two‐step electronic hybridization process. First, LUMOs interact with Ag(100) conduction electrons, forming hybrid molecule‐surface orbitals with enhanced spatial extension. Then, these delocalized molecule‐surface states further hybridize with those of neighbouring molecules. This work highlights how the electronic structure of molecular adsorbates—including orbital degeneracies and symmetries—can be significantly altered via surface‐mediated intermolecular hybridization, over extended distances (beyond 3 nm), having important implications for prospects of molecule‐based solid‐state technologies.
Publisher: Springer Science and Business Media LLC
Date: 10-08-2018
DOI: 10.1038/S41467-018-05543-4
Abstract: Coordination chemistry relies on harnessing active metal sites within organic matrices. Polynuclear complexes—where organic ligands bind to several metal atoms—are relevant due to their electronic/magnetic properties and potential for functional reactivity pathways. However, their synthesis remains challenging few geometries and configurations have been achieved. Here, we synthesise—via supramolecular chemistry on a noble metal surface—one-dimensional metal-organic nanostructures composed of terpyridine (tpy)-based molecules coordinated with well-defined polynuclear iron clusters. Combining low-temperature scanning probe microscopy and density functional theory, we demonstrate that the coordination motif consists of coplanar tpyʼs linked via a quasi-linear tri-iron node in a mixed (positive-)valence metal–metal bond configuration. This unusual linkage is stabilised by local accumulation of electrons between cations, ligand and surface. The latter, enabled by bottom-up on-surface synthesis, yields an electronic structure that hints at a chemically active polynuclear metal centre, paving the way for nanomaterials with novel catalytic/magnetic functionalities.
Publisher: American Chemical Society (ACS)
Date: 08-11-2008
DOI: 10.1021/NL802995U
Abstract: We employed temperature-controlled fast-scanning tunneling microscopy to monitor the diffusion of tetrapyridylporphyrin molecules on the Cu(111) surface. The data reveal unidirectional thermal migration of conformationally adapted monomers in the 300-360 K temperature range. Surprisingly equally oriented molecules spontaneously form dimers that feature a drastically increased one-dimensional diffusivity. The analysis of the bonding and mobility characteristics indicates that this boost is driven by a collective transport mechanism of a metallosupramolecular complex.
Publisher: Wiley
Date: 12-09-2021
Abstract: 2D and layered electronic materials characterized by a kagome lattice, whose valence band structure includes two Dirac bands and one flat band, can host a wide range of tunable topological and strongly correlated electronic phases. While strong electron correlations have been observed in inorganic kagome crystals, they remain elusive in organic systems, which benefit from versatile synthesis protocols via molecular self‐assembly and metal‐ligand coordination. Here, direct experimental evidence of local magnetic moments resulting from strong electron–electron Coulomb interactions in a 2D metal–organic framework (MOF) is reported. The latter consists of di‐cyano‐anthracene (DCA) molecules arranged in a kagome structure via coordination with copper (Cu) atoms on a silver surface [Ag(111)]. Temperature‐dependent scanning tunneling spectroscopy reveals magnetic moments spatially confined to DCA and Cu sites of the MOF, and Kondo screened by the Ag(111) conduction electrons. By density functional theory and mean‐field Hubbard modeling, it is shown that these magnetic moments are the direct consequence of strong Coulomb interactions between electrons within the kagome MOF. The findings pave the way for nanoelectronics and spintronics technologies based on controllable correlated electron phases in 2D organic materials.
Publisher: Springer Science and Business Media LLC
Date: 05-02-2012
DOI: 10.1038/NPHYS2214
Publisher: Proceedings of the National Academy of Sciences
Date: 27-03-2007
Abstract: The engineering of complex architectures from functional molecules on surfaces provides new pathways to control matter at the nanoscale. In this article, we present a combined study addressing the self-assembly of the amino acid l -methionine on Ag(111). Scanning tunneling microscopy data reveal spontaneous ordering in extended molecular chains oriented along high-symmetry substrate directions. At intermediate coverages, regular biomolecular gratings evolve whose periodicity can be tuned at the nanometer scale by varying the methionine surface concentration. Their characteristics and stability were confirmed by helium atomic scattering. X-ray photoemission spectroscopy and high-resolution scanning tunneling microscopy data reveal that the l -methionine chaining is mediated by zwitterionic coupling, accounting for both lateral links and molecular dimerization. This methionine molecular recognition scheme is reminiscent of sheet structures in amino acid crystals and was corroborated by molecular mechanics calculations. Our findings suggest that zwitterionic assembly of amino acids represents a general construction motif to achieve biomolecular nanoarchitectures on surfaces.
Publisher: American Chemical Society (ACS)
Date: 16-10-2017
Publisher: Inderscience Publishers
Date: 2008
Publisher: American Chemical Society (ACS)
Date: 15-06-2009
DOI: 10.1021/JP900593G
Publisher: IEEE
Date: 10-2017
Publisher: American Chemical Society (ACS)
Date: 04-10-2019
Abstract: Quantum dots (QD) with electric-field-controlled charge state are promising for electronics applications,
Publisher: American Chemical Society (ACS)
Date: 14-02-2008
DOI: 10.1021/JP076961I
Publisher: American Chemical Society (ACS)
Date: 21-01-2010
DOI: 10.1021/NN901669P
Abstract: We present a combined study of the adsorption and ordering of the l-tyrosine amino acid on the close-packed Ag(111) noble-metal surface in ultrahigh vacuum by means of low-temperature scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) spectroscopy. On this substrate the biomolecules self-assemble at temperatures exceeding 320 K into linear structures primarily following specific crystallographic directions and evolve with larger molecular coverage into two-dimensional nanoribbons which are commensurate with the underlying atomic lattice. Our high resolution topographical STM data reveal noncovalent molecular dimerization within the highly ordered one-dimensional nanostructures, which recalls the geometrical pattern already seen in the l-methionine/Ag(111) system and supports a universal bonding scheme for amino acids on smooth and unreactive metal surfaces. The molecules desorb for temperatures above 350 K, indicating a relatively weak interaction between the molecules and the substrate. XPS measurements reveal a zwitterionic adsorption, whereas NEXAFS experiments show a tilted adsorption configuration of the phenol moiety. This enables the interdigitation between aromatic side chains of adjacent molecules via parallel-displaced pi-pi interactions which, together with the hydrogen-bonding capability of the hydroxyl functionality, presumably mediates the emergence of the self-assembled supramolecular nanoribbons.
Publisher: Wiley
Date: 04-01-2008
Abstract: We present a molecular-level study of the geometric and electronic properties of Co(II) tetraphenylporphyrin molecules adsorbed on the Cu(111) surface. A combination of low-temperature scanning tunneling microscopy and near-edge X-ray absorption fine structure observations reveals how the metal substrate induces a conformational adaptation into a distorted saddle-shaped geometry. By scanning tunneling spectroscopy we identified the discrete energy levels of the molecule and mapped their spatial electron-density distributions. These results, along with a simple theoretical description, provide a direct correlation between the shape of frontier molecular orbitals and intramolecular structural features.
Publisher: Optica Publishing Group
Date: 16-04-2010
DOI: 10.1364/OE.18.009173
Publisher: American Chemical Society (ACS)
Date: 11-11-2022
DOI: 10.1021/JACS.2C10154
Abstract: Selective activation and controlled functionalization of C-H bonds in organic molecules is one of the most desirable processes in synthetic chemistry. Despite progress in heterogeneous catalysis using metal surfaces, this goal remains challenging due to the stability of C-H bonds and their ubiquity in precursor molecules, h ering regioselectivity. Here, we examine the interaction between 9,10-dicyanoanthracene (DCA) molecules and Au adatoms on a Ag(111) surface at room temperature (RT). Characterization via low-temperature scanning tunneling microscopy, spectroscopy, and noncontact atomic force microscopy, supported by theoretical calculations, revealed the formation of organometallic DCA-Au-DCA dimers, where C atoms at the ends of the anthracene moieties are bonded covalently to single Au atoms. The formation of this organometallic compound is initiated by a regioselective cleaving of C-H bonds at RT. Hybrid quantum mechanics/molecular mechanics calculations show that this regioselective C-H bond cleaving is enabled by an intermediate metal-organic complex which significantly reduces the dissociation barrier of a specific C-H bond. Harnessing the catalytic activity of single metal atoms, this regioselective on-surface C-H activation reaction at RT offers promising routes for future synthesis of functional organic and organometallic materials.
Publisher: American Chemical Society (ACS)
Date: 18-06-2018
Abstract: Supramolecular chemistry protocols applied on surfaces offer compelling avenues for atomic-scale control over organic-inorganic interface structures. In this approach, adsorbate-surface interactions and two-dimensional confinement can lead to morphologies and properties that differ dramatically from those achieved via conventional synthetic approaches. Here, we describe the bottom-up, on-surface synthesis of one-dimensional coordination nanostructures based on an iron (Fe)-terpyridine (tpy) interaction borrowed from functional metal-organic complexes used in photovoltaic and catalytic applications. Thermally activated diffusion of sequentially deposited ligands and metal atoms and intraligand conformational changes lead to Fe-tpy coordination and formation of these nanochains. We used low-temperature scanning tunneling microscopy and density functional theory to elucidate the atomic-scale morphology of the system, suggesting a linear tri-Fe linkage between facing, coplanar tpy groups. Scanning tunneling spectroscopy reveals the highest occupied orbitals, with dominant contributions from states located at the Fe node, and ligand states that mostly contribute to the lowest unoccupied orbitals. This electronic structure yields potential for hosting photoinduced metal-to-ligand charge transfer in the visible/near-infrared. The formation of this unusual tpy/tri-Fe/tpy coordination motif has not been observed for wet chemistry synthetic methods and is mediated by the bottom-up on-surface approach used here, offering pathways to engineer the optoelectronic properties and reactivity of metal-organic nanostructures.
Publisher: AIP Publishing
Date: 17-05-2006
DOI: 10.1063/1.2194541
Abstract: We present a low-temperature scanning tunneling microscopy (STM) study on the supramolecular ordering of tetrapyridyl-porphyrin (TPyP) molecules on Ag(111). Vapor deposition in a wide substrate temperature range reveals that TPyP molecules easily diffuse and self-assemble into large, highly ordered chiral domains. We identify two mirror-symmetric unit cells, each containing two differently oriented molecules. From an analysis of the respective arrangement it is concluded that lateral intermolecular interactions control the packing of the layer, while its orientation is induced by the coupling to the substrate. This finding is corroborated by molecular mechanics calculations. High-resolution STM images recorded at 15K allow a direct identification of intramolecular features. This makes it possible to determine the molecular conformation of TPyP on Ag(111). The pyridyl groups are alternately rotated out of the porphyrin plane by an angle of 60°.
Publisher: Wiley
Date: 18-12-2015
Publisher: Springer Science and Business Media LLC
Date: 05-12-2012
DOI: 10.1038/NATURE11567
Abstract: The time it takes to switch on and off electric current determines the rate at which signals can be processed and s led in modern information technology. Field-effect transistors are able to control currents at frequencies of the order of or higher than 100 gigahertz, but electric interconnects may h er progress towards reaching the terahertz (10(12) hertz) range. All-optical injection of currents through interfering photoexcitation pathways or photoconductive switching of terahertz transients has made it possible to control electric current on a subpicosecond timescale in semiconductors. Insulators have been deemed unsuitable for both methods, because of the need for either ultraviolet light or strong fields, which induce slow damage or ultrafast breakdown, respectively. Here we report the feasibility of electric signal manipulation in a dielectric. A few-cycle optical waveform reversibly increases--free from breakdown--the a.c. conductivity of amorphous silicon dioxide (fused silica) by more than 18 orders of magnitude within 1 femtosecond, allowing electric currents to be driven, directed and switched by the instantaneous light field. Our work opens the way to extending electronic signal processing and high-speed metrology into the petahertz (10(15) hertz) domain.
Publisher: American Chemical Society (ACS)
Date: 18-08-2007
DOI: 10.1021/JA071572N
Abstract: We present a combined low-temperature scanning tunneling microscopy and near-edge X-ray adsorption fine structure study on the interaction of tetrapyridyl-porphyrin (TPyP) molecules with a Cu(111) surface. A novel approach using data from complementary experimental techniques and charge density calculations allows us to determine the adsorption geometry of TPyP on Cu(111). The molecules are centered on "bridge" sites of the substrate lattice and exhibit a strong deformation involving a saddle-shaped macrocycle distortion as well as considerable rotation and tilting of the meso-substituents. We propose a bonding mechanism based on the pyridyl-surface interaction, which mediates the molecular deformation upon adsorption. Accordingly, a functionalization by pyridyl groups opens up pathways to control the anchoring of large organic molecules on metal surfaces and tune their conformational state. Furthermore, we demonstrate that the affinity of the terminal groups for metal centers permits the selective capture of in idual iron atoms at low temperature.
Publisher: Springer Science and Business Media LLC
Date: 12-01-2014
Publisher: Springer Science and Business Media LLC
Date: 08-11-2022
DOI: 10.1038/S41524-022-00918-0
Abstract: Two-dimensional (2D) metal-organic frameworks (MOFs) with a kagome lattice can exhibit strong electron-electron interactions, which can lead to tunable quantum phases including many exotic magnetic phases. While technological developments of 2D MOFs typically take advantage of substrates for growth, support, and electrical contacts, investigations often ignore substrates and their dramatic influence on electronic properties. Here, we show how substrates alter the correlated magnetic phases in kagome MOFs using systematic density functional theory and mean-field Hubbard calculations. We demonstrate that MOF-substrate coupling, MOF-substrate charge transfer, strain, and external electric fields are key variables, activating and deactivating magnetic phases in these materials. While we consider the ex le of kagome-arranged 9,10-dicyanoanthracene molecules coordinated with copper atoms, our findings should generalise to any 2D kagome material. This work offers useful predictions for tunable interaction-induced magnetism in surface-supported 2D (metal-)organic materials, opening the door to solid-state electronic and spintronic technologies based on such systems.
Publisher: AIP Publishing
Date: 02-12-2008
DOI: 10.1063/1.3021291
Abstract: We present a combined scanning tunneling microscopy (STM), near-edge x-ray-absorption fine-structure, and x-ray photoemission spectroscopy (XPS) study on the bonding and ordering of tetrapyridyl-porphyrin molecules on the Cu(111) surface in the 300–500 K temperature range. Following deposition at 300 K the molecules are adsorbed with a pronounced conformational adaptation of the anchored species featuring a saddle-shaped macrocycle and terminal groups pointing toward the substrate. Upon moderate annealing supramolecular chains evolve that are stabilized by metal-ligand interactions between the mesopyridyl substituents and copper adatoms resulting in twofold copper coordination. Annealing to temperatures exceeding 450 K strongly alters the molecular appearance in high-resolution STM data. This modification was also induced by controlled voltage pulses and related to a deprotonation of the molecule by XPS. Under appropriate conditions a novel binding motif leads to honeycomb structures coexisting with the chain segments. The conformation withstands annealing without large modification.
Publisher: American Physical Society (APS)
Date: 15-07-2008
Publisher: IEEE
Date: 05-2011
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2NA00385F
Abstract: Non-covalent intermolecular hybridization in a 2D molecular self-assembly gives rise to a narrow electronic energy band, a promising prospect for organic nanoelectronics.
Publisher: Wiley
Date: 26-01-2007
Abstract: We report a bottom-up approach for the fabrication of metallo-porphyrin compounds and nanoarchitectures in two dimensions. Scanning tunneling microscopy and tunneling spectroscopy observations elucidate the interaction of highly regular porphyrin layers self-assembled on a Ag(111) surface with iron monomers supplied by an atomic beam. The Fe is shown to be incorporated selectively in the porphyrin macrocycle whereby the template structure is strictly preserved. The immobilization of the molecular reactants allows the identification of single metalation events in a novel reaction scheme. Because the template layers provide extended arrays of reaction sites, superlattices of coordinatively unsaturated and magnetically active metal centers are obtained. This approach offers novel pathways to realize metallo-porphyrin compounds, low-dimensional metal-organic architectures and patterned surfaces which cannot be achieved by conventional means.
Publisher: IOP Publishing
Date: 08-02-2023
Abstract: Two-dimensional (2D) nanostructures and nanomaterials offer potential for a wide range of technological applications in electronics, optoelectronics, data storage, sensing and catalysis. On-surface molecular self-assembly – where organic molecules act as building blocks and where surfaces play the role of supporting templates – allows for the bottom-up synthesis of such 2D systems with tuneable atomically precise morphologies and tailored electronic properties. These self-assembly protocols are well established on metal surfaces, but remain limited on electronically gapped substrates (insulators, semiconductors). The latter are useful for preventing electronic coupling (that is, hybridization between molecular assembly and underlying surface) and for avoiding quenching of optical processes, necessary for prospective electronic and optoelectronic applications. In particular, molecular self-assembly on surfaces other than weakly interacting metals can be challenging due to substrate reactivity, defects and inhomogeneities, resulting in intricate energy landscapes that limit the growth kinetically and h ers the synthesis of large-area defect-free 2D systems. Here, we demonstrate the self-assembly of a 2D, atomically thin organic molecular film on a model wide bandgap 2D insulator, single-layer hexagonal boron nitride (hBN) on Cu(111). The molecular film consists of flat, aromatic 9,10-di-cyano-anthracene (DCA) molecules. Our low-temperature scanning tunnelling microscopy and spectroscopy measurements revealed mesoscopic ( 100 x 100 nm^2), topographically homogeneous crystalline molecular domains resulting from flat molecular adsorption and noncovalent in-plane cyano-ring bonding, with electronically decoupled molecular orbitals (MOs) lying within the hBN electronic gap. These MOs exhibit an energy level spatial modulation (~300 meV) that follows the moiré work function variation of hBN on Cu(111). This work paves the way for large-area, atomically precise, highly crystalline 2D organic (and metal-organic) nanomaterials on electronically functional wide bandgap insulators.
Start Date: 04-2017
End Date: 06-2019
Amount: $600,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 06-2017
End Date: 06-2024
Amount: $33,400,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 06-2020
End Date: 12-2022
Amount: $744,000.00
Funder: Australian Research Council
View Funded ActivityStart Date: 06-2016
End Date: 12-2022
Amount: $679,352.00
Funder: Australian Research Council
View Funded Activity