Project acronym ABACUS
Project Ab-initio adiabatic-connection curves for density-functional analysis and construction
Researcher (PI) Trygve Ulf Helgaker
Host Institution (HI) UNIVERSITETET I OSLO
Call Details Advanced Grant (AdG), PE4, ERC-2010-AdG_20100224
Summary Quantum chemistry provides two approaches to molecular electronic-structure calculations: the systematically refinable but expensive many-body wave-function methods and the inexpensive but not systematically refinable Kohn Sham method of density-functional theory (DFT). The accuracy of Kohn Sham calculations is determined by the quality of the exchange correlation functional, from which the effects of exchange and correlation among the electrons are extracted using the density rather than the wave function. However, the exact exchange correlation functional is unknown—instead, many approximate forms have been developed, by fitting to experimental data or by satisfying exact relations. Here, a new approach to density-functional analysis and construction is proposed: the Lieb variation principle, usually regarded as conceptually important but impracticable. By invoking the Lieb principle, it becomes possible to approach the development of approximate functionals in a novel manner, being directly guided by the behaviour of exact functional, accurately calculated for a wide variety of chemical systems. In particular, this principle will be used to calculate ab-initio adiabatic connection curves, studying the exchange correlation functional for a fixed density as the electronic interactions are turned on from zero to one. Pilot calculations have indicated the feasibility of this approach in simple cases—here, a comprehensive set of adiabatic-connection curves will be generated and utilized for calibration, construction, and analysis of density functionals, the objective being to produce improved functionals for Kohn Sham calculations by modelling or fitting such curves. The ABACUS approach will be particularly important in cases where little experimental information is available—for example, for understanding and modelling the behaviour of the exchange correlation functional in electromagnetic fields.
Summary
Quantum chemistry provides two approaches to molecular electronic-structure calculations: the systematically refinable but expensive many-body wave-function methods and the inexpensive but not systematically refinable Kohn Sham method of density-functional theory (DFT). The accuracy of Kohn Sham calculations is determined by the quality of the exchange correlation functional, from which the effects of exchange and correlation among the electrons are extracted using the density rather than the wave function. However, the exact exchange correlation functional is unknown—instead, many approximate forms have been developed, by fitting to experimental data or by satisfying exact relations. Here, a new approach to density-functional analysis and construction is proposed: the Lieb variation principle, usually regarded as conceptually important but impracticable. By invoking the Lieb principle, it becomes possible to approach the development of approximate functionals in a novel manner, being directly guided by the behaviour of exact functional, accurately calculated for a wide variety of chemical systems. In particular, this principle will be used to calculate ab-initio adiabatic connection curves, studying the exchange correlation functional for a fixed density as the electronic interactions are turned on from zero to one. Pilot calculations have indicated the feasibility of this approach in simple cases—here, a comprehensive set of adiabatic-connection curves will be generated and utilized for calibration, construction, and analysis of density functionals, the objective being to produce improved functionals for Kohn Sham calculations by modelling or fitting such curves. The ABACUS approach will be particularly important in cases where little experimental information is available—for example, for understanding and modelling the behaviour of the exchange correlation functional in electromagnetic fields.
Max ERC Funding
2 017 932 €
Duration
Start date: 2011-03-01, End date: 2016-02-29
Project acronym BIO2CHEM-D
Project Biomass to chemicals: Catalysis design from first principles for a sustainable chemical industry
Researcher (PI) Nuria Lopez
Host Institution (HI) FUNDACIO PRIVADA INSTITUT CATALA D'INVESTIGACIO QUIMICA
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary The use of renewable feedstocks by the chemical industry is fundamental due to both the depletion of fossil
resources and the increasing pressure of environmental concerns. Biomass can act as a sustainable source of
organic industrial chemicals; however, the establishment of a renewable chemical industry that is
economically competitive with the present oil-based one requires the development of new processes to
convert biomass-derived compounds into useful industrial materials following the principles of green
chemistry. To achieve these goals, developments in several fields including heterogeneous catalysis are
needed. One of the ways to accelerate the discovery of new potentially active, selective and stable catalysts is
the massive use of computational chemistry. Recent advances have demonstrated that Density Functional
Theory coupled to ab initio thermodynamics, transition state theory and microkinetic analysis can provide a
full view of the catalytic phenomena.
The aim of the present project is thus to employ these well-tested computational techniques to the
development of a theoretical framework that can accelerate the identification of new catalysts for the
conversion of biomass derived target compounds into useful chemicals. Since compared to petroleum-based
materials-biomass derived ones are multifuncionalized, the search for new catalytic materials and processes
has a strong requirement in the selectivity of the chemical transformations. The main challenges in the
project are related to the high functionalization of the molecules, their liquid nature and the large number of
potentially competitive reaction paths. The requirements of specificity and selectivity in the chemical
transformations while keeping a reasonably flexible framework constitute a major objective. The work will
be divided in three main work packages, one devoted to the properties of small molecules or fragments
containing a single functional group; the second addresses competition in multiple functionalized molecules;
and third is dedicated to the specific transformations of two molecules that have already been identified as
potential platform generators. The goal is to identify suitable candidates that could be synthetized and tested
in the Institute facilities.
Summary
The use of renewable feedstocks by the chemical industry is fundamental due to both the depletion of fossil
resources and the increasing pressure of environmental concerns. Biomass can act as a sustainable source of
organic industrial chemicals; however, the establishment of a renewable chemical industry that is
economically competitive with the present oil-based one requires the development of new processes to
convert biomass-derived compounds into useful industrial materials following the principles of green
chemistry. To achieve these goals, developments in several fields including heterogeneous catalysis are
needed. One of the ways to accelerate the discovery of new potentially active, selective and stable catalysts is
the massive use of computational chemistry. Recent advances have demonstrated that Density Functional
Theory coupled to ab initio thermodynamics, transition state theory and microkinetic analysis can provide a
full view of the catalytic phenomena.
The aim of the present project is thus to employ these well-tested computational techniques to the
development of a theoretical framework that can accelerate the identification of new catalysts for the
conversion of biomass derived target compounds into useful chemicals. Since compared to petroleum-based
materials-biomass derived ones are multifuncionalized, the search for new catalytic materials and processes
has a strong requirement in the selectivity of the chemical transformations. The main challenges in the
project are related to the high functionalization of the molecules, their liquid nature and the large number of
potentially competitive reaction paths. The requirements of specificity and selectivity in the chemical
transformations while keeping a reasonably flexible framework constitute a major objective. The work will
be divided in three main work packages, one devoted to the properties of small molecules or fragments
containing a single functional group; the second addresses competition in multiple functionalized molecules;
and third is dedicated to the specific transformations of two molecules that have already been identified as
potential platform generators. The goal is to identify suitable candidates that could be synthetized and tested
in the Institute facilities.
Max ERC Funding
1 496 200 €
Duration
Start date: 2010-10-01, End date: 2015-09-30
Project acronym C3ENV
Project Combinatorial Computational Chemistry A new field to tackle environmental problems
Researcher (PI) Thomas Heine
Host Institution (HI) JACOBS UNIVERSITY BREMEN GGMBH
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary Combinatorial Computational Chemistry is developed as a standard tool to tackle complex problems in chemistry and materials science. The method employs a series of state-of-the-art methods, ranging from empirical molecular mechanics to first principles calculations, as well as of mathematical (graph theoretical and combinatorial) methods. The process is similar as in experimental combinatorial chemistry: First, a large set of candidate structures is generated which is complete in the sense that the best possible structure for a particular purpose must be found among the set. This structure is then identified using computational chemistry. We will apply methodologies at different stages in hierarchical order and successively screen the set of candidate structures. Screening criteria are based on the computer simulations and include geometry, stability and properties of the candidate structures. Detailed characteristics of the final materials will be simulated, including the X-ray diffraction pattern, the electronic structure, and the target properties. We will apply C3 to two important problems of environmental science. (i) We will optimise nanoporous materials to act as molecular sieves to separate water from ethanol, an important task for the production of biofuels. Here, materials are optimised to transport ethanol, but not water (or vice versa). The tuning parameters are the channel size of the material and its polarity. (ii) We will optimise nanoporous materials to transport protons, an important task for the design of energy-efficient fuel cells, by distributing flexible functional groups, acting as hopping sites for the protons, in the framework.
Summary
Combinatorial Computational Chemistry is developed as a standard tool to tackle complex problems in chemistry and materials science. The method employs a series of state-of-the-art methods, ranging from empirical molecular mechanics to first principles calculations, as well as of mathematical (graph theoretical and combinatorial) methods. The process is similar as in experimental combinatorial chemistry: First, a large set of candidate structures is generated which is complete in the sense that the best possible structure for a particular purpose must be found among the set. This structure is then identified using computational chemistry. We will apply methodologies at different stages in hierarchical order and successively screen the set of candidate structures. Screening criteria are based on the computer simulations and include geometry, stability and properties of the candidate structures. Detailed characteristics of the final materials will be simulated, including the X-ray diffraction pattern, the electronic structure, and the target properties. We will apply C3 to two important problems of environmental science. (i) We will optimise nanoporous materials to act as molecular sieves to separate water from ethanol, an important task for the production of biofuels. Here, materials are optimised to transport ethanol, but not water (or vice versa). The tuning parameters are the channel size of the material and its polarity. (ii) We will optimise nanoporous materials to transport protons, an important task for the design of energy-efficient fuel cells, by distributing flexible functional groups, acting as hopping sites for the protons, in the framework.
Max ERC Funding
1 500 000 €
Duration
Start date: 2011-02-01, End date: 2016-04-30
Project acronym CCCAN
Project Characterizing and Controlling Carbon Nanomaterials
Researcher (PI) Janina Maultzsch
Host Institution (HI) TECHNISCHE UNIVERSITAT BERLIN
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary The aim of this project is to understand and control the fundamental physical properties of novel carbon nanomaterials:
carbon nanotubes and graphene. By a combination of complementary methods, i.e. vibrational spectroscopy, scanning probe microscopy, and theoretical modelling, a comprehensive understanding of the electronic, vibrational, optical properties, and their connection with the material’s structure will be obtained. A diagnostics “toolbox” will be established on the materials in
their most unperturbed, ideal states. Taking the results as reference, the materials will be studied under conditions relevant when incorporated into devices. These include imperfections of the materials and interaction with different environments, with other carbon nanotubes/graphene, and with extrinsic materials introduced during device processing. The gained insight and understanding on a fundamental level will also advance technological routes for scaling up carbon-nanomaterial electronic device fabrication, which is still lacking sufficient control over selectivity towards the desired physical properties. Control over the electronic and optical properties will be sought through deliberately induced interactions and chemical functionalization
of the materials. The project benefits from close collaborations between experimental and theoretical physics, chemistry, and materials science.
Summary
The aim of this project is to understand and control the fundamental physical properties of novel carbon nanomaterials:
carbon nanotubes and graphene. By a combination of complementary methods, i.e. vibrational spectroscopy, scanning probe microscopy, and theoretical modelling, a comprehensive understanding of the electronic, vibrational, optical properties, and their connection with the material’s structure will be obtained. A diagnostics “toolbox” will be established on the materials in
their most unperturbed, ideal states. Taking the results as reference, the materials will be studied under conditions relevant when incorporated into devices. These include imperfections of the materials and interaction with different environments, with other carbon nanotubes/graphene, and with extrinsic materials introduced during device processing. The gained insight and understanding on a fundamental level will also advance technological routes for scaling up carbon-nanomaterial electronic device fabrication, which is still lacking sufficient control over selectivity towards the desired physical properties. Control over the electronic and optical properties will be sought through deliberately induced interactions and chemical functionalization
of the materials. The project benefits from close collaborations between experimental and theoretical physics, chemistry, and materials science.
Max ERC Funding
1 468 960 €
Duration
Start date: 2010-12-01, End date: 2015-11-30
Project acronym CHEMHEAT
Project Chemical Control of Heating and Cooling in Molecular Junctions: Optimizing Function and Stability
Researcher (PI) Gemma Solomon
Host Institution (HI) KOBENHAVNS UNIVERSITET
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary Nanoscale systems binding single molecules, or small numbers of molecules, in conducting junctions show considerable promise for a range of technological applications, from photovoltaics to rectifiers to sensors. These environments differ significantly from the traditional domain of chemical studies involving molecules in solution and the gas phase, necessitating renewed efforts to understand the physical properties of these systems. The objective of this proposal concerns one particular class of physical processes: understanding and controlling local heating in molecular junctions in terms of excitation, dissipation and transfer.
Local heating and dissipation in molecular junctions has long been a concern due to the possibly detrimental impact on device stability and function. More recently there has been increased interest, as these processes underlie both spectroscopic techniques and potential technological applications. Together these issues make an investigation of ways to chemically control local heating in molecular junctions timely and important.
The proposal objective will be addressed through the investigation of three challenges:
- Developing chemical control of local heating in molecular junctions.
- Developing chemical control of heat dissipation in molecular junctions.
- Design of optimal thermoelectric materials.
These three challenges constitute distinct, yet complementary, avenues for investigation with progress in each area supporting the other two. All three challenges build on existing theoretical methods, with the important shift of focus to methods to achieve chemical control. The combination of state-of-the-art computational methods with careful chemical studies promises significant new developments for the area.
Summary
Nanoscale systems binding single molecules, or small numbers of molecules, in conducting junctions show considerable promise for a range of technological applications, from photovoltaics to rectifiers to sensors. These environments differ significantly from the traditional domain of chemical studies involving molecules in solution and the gas phase, necessitating renewed efforts to understand the physical properties of these systems. The objective of this proposal concerns one particular class of physical processes: understanding and controlling local heating in molecular junctions in terms of excitation, dissipation and transfer.
Local heating and dissipation in molecular junctions has long been a concern due to the possibly detrimental impact on device stability and function. More recently there has been increased interest, as these processes underlie both spectroscopic techniques and potential technological applications. Together these issues make an investigation of ways to chemically control local heating in molecular junctions timely and important.
The proposal objective will be addressed through the investigation of three challenges:
- Developing chemical control of local heating in molecular junctions.
- Developing chemical control of heat dissipation in molecular junctions.
- Design of optimal thermoelectric materials.
These three challenges constitute distinct, yet complementary, avenues for investigation with progress in each area supporting the other two. All three challenges build on existing theoretical methods, with the important shift of focus to methods to achieve chemical control. The combination of state-of-the-art computational methods with careful chemical studies promises significant new developments for the area.
Max ERC Funding
1 499 999 €
Duration
Start date: 2010-12-01, End date: 2015-11-30
Project acronym COMPSELF
Project Self-Organisation: From Molecules to Matter
Researcher (PI) David John Wales
Host Institution (HI) THE CHANCELLOR MASTERS AND SCHOLARSOF THE UNIVERSITY OF CAMBRIDGE
Call Details Advanced Grant (AdG), PE4, ERC-2010-AdG_20100224
Summary This research proposal concerns the theory and computer simulation of self-organisation to predict properties and to design systems with specified characteristics. The key computational challenge is to explore the energy landscape for complex systems and make predictions to characterise efficient self-organisation on experimental time and length scales. Novel methodology is required to overcome the problems of broken ergodicity and rare events. The theoretical framework exploits stationary points of the potential energy landscape to access the required time and length scales. Applications include self-assembly of mesoscopic structures from coarse-grained building blocks and all-atom simulations of conformational changes in specific proteins and nucleic acids.
We aim to establish design principles for efficient self-assembly by developing novel tools for visualising and exploration of the corresponding landscape. Here, a key issue is how the interactions between the constituent particles determine the organisation of the energy landscape. Identifying which features lead to successful self-assembly and which disrupt such ordering will lead to a wide range of important applications, ranging from design of new materials to identifying new anti-viral drugs. The same methodology will be applied to detailed models of specific biomolecules, where self-organisation into alternative structures is associated with disease. Global optimisation will be employed in structure prediction for variable pathogens, such as human influenza virus. Pathways for folding and misfolding of specific proteins and nucleic acids will be characterised using novel rare events methodology, providing insight into intermediates that could serve as potential drug targets.
Summary
This research proposal concerns the theory and computer simulation of self-organisation to predict properties and to design systems with specified characteristics. The key computational challenge is to explore the energy landscape for complex systems and make predictions to characterise efficient self-organisation on experimental time and length scales. Novel methodology is required to overcome the problems of broken ergodicity and rare events. The theoretical framework exploits stationary points of the potential energy landscape to access the required time and length scales. Applications include self-assembly of mesoscopic structures from coarse-grained building blocks and all-atom simulations of conformational changes in specific proteins and nucleic acids.
We aim to establish design principles for efficient self-assembly by developing novel tools for visualising and exploration of the corresponding landscape. Here, a key issue is how the interactions between the constituent particles determine the organisation of the energy landscape. Identifying which features lead to successful self-assembly and which disrupt such ordering will lead to a wide range of important applications, ranging from design of new materials to identifying new anti-viral drugs. The same methodology will be applied to detailed models of specific biomolecules, where self-organisation into alternative structures is associated with disease. Global optimisation will be employed in structure prediction for variable pathogens, such as human influenza virus. Pathways for folding and misfolding of specific proteins and nucleic acids will be characterised using novel rare events methodology, providing insight into intermediates that could serve as potential drug targets.
Max ERC Funding
2 069 374 €
Duration
Start date: 2011-03-01, End date: 2016-02-29
Project acronym DYNAMO
Project Dynamical processes in open quantum systems: pushing the frontiers of theoretical spectroscopy
Researcher (PI) Angel Secades Rubio
Host Institution (HI) UNIVERSIDAD DEL PAIS VASCO/ EUSKAL HERRIKO UNIBERTSITATEA
Call Details Advanced Grant (AdG), PE4, ERC-2010-AdG_20100224
Summary "Scope ""Energy Materials. In this project we develop new concepts for building a novel theoretical framework (the ab-initio non-equilibrium dynamical modelling tool”) for understanding, identifying, and quantifying the different contributions to energy harvesting and storage as well as describing transport mechanisms in natural light harvesting complexes, photovoltaic materials, fluorescent proteins and artificial (nanostructured) devices by means of theories of open quantum systems, non-equilibrium processes and electronic structure. We address cutting-edge applications along three major scientific challenges: i) characterize matter out of equilibrium, ii) control material processes at the electronic level and tailor material properties, iii) master energy and information on the nanoscale. The long-term goal is developing a set of theoretical tools for the quantitative prediction of energy transfer phenomena in real systems.
We will provide answers to the following questions: What are the design principles from the environment-assisted quantum transport in photosynthetic organisms that can be transferred to nanostructured materials such as organic photovoltaic materials and biomimetic materials? What are the fundamental limits of excitonic transport properties such as exciton diffusion lengths and recombination rates? What is the role of quantum coherence in the energy transport in photosynthetic complexes and photovoltaic materials? What is the role of spatial confinement in water and proton transfer through porous membranes (nano-capillarity)?
The ground-breaking nature of the project lies in being the first systematic development and application of the theories of open quantum systems and quantum optimal control within an ab-initio framework (time-dependent-density functional theory). The project will open new methodological, applicative and theoretical horizons of research."
Summary
"Scope ""Energy Materials. In this project we develop new concepts for building a novel theoretical framework (the ab-initio non-equilibrium dynamical modelling tool”) for understanding, identifying, and quantifying the different contributions to energy harvesting and storage as well as describing transport mechanisms in natural light harvesting complexes, photovoltaic materials, fluorescent proteins and artificial (nanostructured) devices by means of theories of open quantum systems, non-equilibrium processes and electronic structure. We address cutting-edge applications along three major scientific challenges: i) characterize matter out of equilibrium, ii) control material processes at the electronic level and tailor material properties, iii) master energy and information on the nanoscale. The long-term goal is developing a set of theoretical tools for the quantitative prediction of energy transfer phenomena in real systems.
We will provide answers to the following questions: What are the design principles from the environment-assisted quantum transport in photosynthetic organisms that can be transferred to nanostructured materials such as organic photovoltaic materials and biomimetic materials? What are the fundamental limits of excitonic transport properties such as exciton diffusion lengths and recombination rates? What is the role of quantum coherence in the energy transport in photosynthetic complexes and photovoltaic materials? What is the role of spatial confinement in water and proton transfer through porous membranes (nano-capillarity)?
The ground-breaking nature of the project lies in being the first systematic development and application of the theories of open quantum systems and quantum optimal control within an ab-initio framework (time-dependent-density functional theory). The project will open new methodological, applicative and theoretical horizons of research."
Max ERC Funding
1 877 497 €
Duration
Start date: 2011-04-01, End date: 2016-03-31
Project acronym ENERGYBIOCATALYSIS
Project Understanding and Exploiting Biological Catalysts for Energy Cycling: Development of Infrared Spectroelectrochemistry for Studying Intermediates in Metalloenzyme Catalysis
Researcher (PI) Kylie Alison Vincent
Host Institution (HI) THE CHANCELLOR, MASTERS AND SCHOLARS OF THE UNIVERSITY OF OXFORD
Call Details Starting Grant (StG), PE4, ERC-2010-StG_20091028
Summary Advanced catalysts for energy cycling will be essential to a future sustainable energy economy. Interconversion of water and hydrogen allows solar and other green electricity to be stored in transportable form as H2 - a fuel for electricity generation on demand. Precious metals (Pt) are the best catalysts currently available for H2 oxidation in fuel cells. In contrast, readily available Ni/Fe form the catalytic centres of robust enzymes used by micro-organisms to oxidise or produce H2 selectively, at rates rivalling platinum. Metalloenzymes also efficiently catalyse redox reactions of the nitrogen and carbon cycles. Electrochemistry of enzyme films on a graphite electrode provides a direct route to studying and exploiting biocatalysis, for example a fuel cell that produces electricity from dilute H2 in air using an electrode modified with hydrogenase. Understanding structures and complex chemistry of enzyme active sites is now an important challenge that underpins exploitation of enzymes and design of future catalysts. This project develops sensitive IR methods for metalloenzymes on conducting surfaces or particles. Ligands with strong InfraRed vibrational signatures (CO, CN-) are exploited as probes of active site chemistry for hydrogenases and carbon-cycling enzymes. The proposal unites physical techniques (surface vibrational spectroscopy, electrochemistry), microbiology (mutagenesis, microbial energy cycling), inorganic chemistry (reactions at unusual organometallic centres) and technology development (energy-catalysis) in addressing enzyme chemistry. Understanding the basis for the extreme catalytic selectivity of enzymes will contribute to knowledge of biological energy cycling and provide inspiration for new catalysts.
Summary
Advanced catalysts for energy cycling will be essential to a future sustainable energy economy. Interconversion of water and hydrogen allows solar and other green electricity to be stored in transportable form as H2 - a fuel for electricity generation on demand. Precious metals (Pt) are the best catalysts currently available for H2 oxidation in fuel cells. In contrast, readily available Ni/Fe form the catalytic centres of robust enzymes used by micro-organisms to oxidise or produce H2 selectively, at rates rivalling platinum. Metalloenzymes also efficiently catalyse redox reactions of the nitrogen and carbon cycles. Electrochemistry of enzyme films on a graphite electrode provides a direct route to studying and exploiting biocatalysis, for example a fuel cell that produces electricity from dilute H2 in air using an electrode modified with hydrogenase. Understanding structures and complex chemistry of enzyme active sites is now an important challenge that underpins exploitation of enzymes and design of future catalysts. This project develops sensitive IR methods for metalloenzymes on conducting surfaces or particles. Ligands with strong InfraRed vibrational signatures (CO, CN-) are exploited as probes of active site chemistry for hydrogenases and carbon-cycling enzymes. The proposal unites physical techniques (surface vibrational spectroscopy, electrochemistry), microbiology (mutagenesis, microbial energy cycling), inorganic chemistry (reactions at unusual organometallic centres) and technology development (energy-catalysis) in addressing enzyme chemistry. Understanding the basis for the extreme catalytic selectivity of enzymes will contribute to knowledge of biological energy cycling and provide inspiration for new catalysts.
Max ERC Funding
1 373 322 €
Duration
Start date: 2011-02-01, End date: 2016-01-31
Project acronym ENERGYSURF
Project Surfaces of Energy Functional Metal Oxides
Researcher (PI) Geoffrey Thornton
Host Institution (HI) University College London
Call Details Advanced Grant (AdG), PE4, ERC-2010-AdG_20100224
Summary Many important interactions near the surfaces of energy functional metal oxide surfaces are yet to be established at the atomic level. How bonds are formed and broken in photocatalysis, the role of the metal and oxide in a supported metal catalyst, the mechanism of energy flow from atom to atom after photoexcitation in a photovoltaic device are just some of the open questions. The underlying motivation to generate answers is clear: it provides an opportunity to improve technology associated with light harvesting and energy-related catalysis. But the fundamental science required is extremely challenging and is only just starting to yield some detailed answers. In this highly ambitious project we will tackle three major issues associated with the surface chemistry of energy functional metal oxides-- three grand challenges. In doing so, we will make use of a unique range of experimental techniques. One will focus on solid-gas interactions in studies of Au on CeO2, employing scanning tunneling microscopy (STM), scanning tunnelling spectroscopy and STM-inelastic electron tunnelling spectroscopy to answer questions about the active site of water gas shift catalysis and the mechanism by which the substrate reversibly exchanges oxygen. The second challenge will probe the structures of interfaces between water and ZnO and TiO2, using surface X-ray diffraction and STM. This will include the adsorption of dye mimics from solution. In the third challenge, femtosecond time resolved photoemission using pump probe will be used to unravel the details of energy dissipation following a UV pulse absorption by ZnO and TiO2 substrates and their interaction with water. This is directly related to processes associated with photocatalysis. We expect that this ERC project will revolutionise our understanding of energy functional surfaces based on metal oxides and ultimately lead to key breakthroughs in the design of advanced devices.
Summary
Many important interactions near the surfaces of energy functional metal oxide surfaces are yet to be established at the atomic level. How bonds are formed and broken in photocatalysis, the role of the metal and oxide in a supported metal catalyst, the mechanism of energy flow from atom to atom after photoexcitation in a photovoltaic device are just some of the open questions. The underlying motivation to generate answers is clear: it provides an opportunity to improve technology associated with light harvesting and energy-related catalysis. But the fundamental science required is extremely challenging and is only just starting to yield some detailed answers. In this highly ambitious project we will tackle three major issues associated with the surface chemistry of energy functional metal oxides-- three grand challenges. In doing so, we will make use of a unique range of experimental techniques. One will focus on solid-gas interactions in studies of Au on CeO2, employing scanning tunneling microscopy (STM), scanning tunnelling spectroscopy and STM-inelastic electron tunnelling spectroscopy to answer questions about the active site of water gas shift catalysis and the mechanism by which the substrate reversibly exchanges oxygen. The second challenge will probe the structures of interfaces between water and ZnO and TiO2, using surface X-ray diffraction and STM. This will include the adsorption of dye mimics from solution. In the third challenge, femtosecond time resolved photoemission using pump probe will be used to unravel the details of energy dissipation following a UV pulse absorption by ZnO and TiO2 substrates and their interaction with water. This is directly related to processes associated with photocatalysis. We expect that this ERC project will revolutionise our understanding of energy functional surfaces based on metal oxides and ultimately lead to key breakthroughs in the design of advanced devices.
Max ERC Funding
2 364 681 €
Duration
Start date: 2011-10-01, End date: 2017-09-30
Project acronym FCC
Project Functional Coordination Chemistry
Researcher (PI) David Parker
Host Institution (HI) UNIVERSITY OF DURHAM
Call Details Advanced Grant (AdG), PE4, ERC-2010-AdG_20100224
Summary To address critical problems in the natural sciences by developing the chemistry of metal coordination complexes, harnessing the unique ground and excited state properties of the lanthanide (III) ions to impart the required function into the complexes and their conjugates. This requires PI-led collaborative work in molecular design and instrumentation development.
Objectives
1. To measure changes in the concentration of essential bioactive species in particular compartments of plant and animal cells, including chiral species. This requires the creation of targeted luminescent probes that relay an optical signal to the observer, signalling changes in the concentration of these species, with high spatial and temporal control. In parallel, circularly polarised emission microscopy will be pioneered.
2. To enable 19F magnetic resonance studies to be undertaken much more widely by devising functional paramagnetic 19F-magnetic resonance probes, with fast relaxation and enhanced chemical shift dispersion.
Summary
To address critical problems in the natural sciences by developing the chemistry of metal coordination complexes, harnessing the unique ground and excited state properties of the lanthanide (III) ions to impart the required function into the complexes and their conjugates. This requires PI-led collaborative work in molecular design and instrumentation development.
Objectives
1. To measure changes in the concentration of essential bioactive species in particular compartments of plant and animal cells, including chiral species. This requires the creation of targeted luminescent probes that relay an optical signal to the observer, signalling changes in the concentration of these species, with high spatial and temporal control. In parallel, circularly polarised emission microscopy will be pioneered.
2. To enable 19F magnetic resonance studies to be undertaken much more widely by devising functional paramagnetic 19F-magnetic resonance probes, with fast relaxation and enhanced chemical shift dispersion.
Max ERC Funding
2 498 552 €
Duration
Start date: 2011-06-01, End date: 2016-05-31
