Project acronym OMSQC
Project Orthogonalization Models in Semiempirical Quantum Chemistry
Researcher (PI) Walter Thiel
Host Institution (HI) MAX PLANCK INSTITUT FUER KOHLENFORSCHUNG
Call Details Advanced Grant (AdG), PE4, ERC-2013-ADG
Summary "The proposal aims at the development of a generally applicable semiempirical approach that goes beyond the current standard model by including explicit orthogonalization and dispersion terms into the semiempirical Hamiltonian. We have recently shown in preliminary work on organic molecules that such orthogonalization models (OMx = OM1, OM2, OM3) are significantly more accurate than standard semiempirical methods (AM1, PM3, PM6) both for ground-state and excited-state properties, at comparable computational costs. We plan to improve the OMx models by incorporating dispersion corrections (OMx-D) and by extending the formalism from an sp to an spd basis (OMx-DE). The resulting approaches will be parameterized for all chemically important main-group elements and transition metals to generate the next generation of generally applicable semiempirical methods. These methods are designed to fill the currently existing gap between density functional theory (DFT) and classical force field approaches. Being about 1,000 times faster than DFT, and being capable of treating electronic events (unlike classical force fields), OMx-based methods are expected to enable realistic electronic structure calculations, with useful accuracy, on large complex systems in all branches of chemistry. Especially when applied in a multi-method strategy, with synergistic use of different computational tools, this will allow the modelling of many chemically relevant systems that are currently beyond reach for computational chemistry. Proof-of-concept applications will address the reaction mechanisms of enzymatic reactions (biocatalysis) and electronically excited states (organic solar cells, photoactive proteins, excited-state dynamics in complex systems). The successful development of generally applicable OMx-based methods will provide a breakthrough in computational chemistry by opening up new areas of application."
Summary
"The proposal aims at the development of a generally applicable semiempirical approach that goes beyond the current standard model by including explicit orthogonalization and dispersion terms into the semiempirical Hamiltonian. We have recently shown in preliminary work on organic molecules that such orthogonalization models (OMx = OM1, OM2, OM3) are significantly more accurate than standard semiempirical methods (AM1, PM3, PM6) both for ground-state and excited-state properties, at comparable computational costs. We plan to improve the OMx models by incorporating dispersion corrections (OMx-D) and by extending the formalism from an sp to an spd basis (OMx-DE). The resulting approaches will be parameterized for all chemically important main-group elements and transition metals to generate the next generation of generally applicable semiempirical methods. These methods are designed to fill the currently existing gap between density functional theory (DFT) and classical force field approaches. Being about 1,000 times faster than DFT, and being capable of treating electronic events (unlike classical force fields), OMx-based methods are expected to enable realistic electronic structure calculations, with useful accuracy, on large complex systems in all branches of chemistry. Especially when applied in a multi-method strategy, with synergistic use of different computational tools, this will allow the modelling of many chemically relevant systems that are currently beyond reach for computational chemistry. Proof-of-concept applications will address the reaction mechanisms of enzymatic reactions (biocatalysis) and electronically excited states (organic solar cells, photoactive proteins, excited-state dynamics in complex systems). The successful development of generally applicable OMx-based methods will provide a breakthrough in computational chemistry by opening up new areas of application."
Max ERC Funding
1 996 000 €
Duration
Start date: 2014-01-01, End date: 2018-12-31
Project acronym OPERANDOCAT
Project In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Researcher (PI) Beatriz ROLDAN CUENYA
Host Institution (HI) MAX-PLANCK-GESELLSCHAFT ZUR FORDERUNG DER WISSENSCHAFTEN EV
Call Details Consolidator Grant (CoG), PE4, ERC-2016-COG
Summary Tailoring the chemical reactivity of nanomaterials at the atomic level is one of the most important challenges in catalysis research. In order to achieve this elusive goal, fundamental understanding of the structural and chemical properties of these complex systems must be obtained. Numerous studies have been devoted to understanding the properties that affect the catalytic performance of metal nanoparticles (NPs) such as their size, interaction with the support, and chemical state. The role played by the NP shape on catalytic performance is, however, less understood. Complicating the analysis is the fact that the former parameters cannot be considered independently, since the NP size as well as the support will have an impact on the most stable NP shapes. In addition, the dynamic nature of the NP catalysts and their response to the environment must be taken into consideration, since the working state of a NP catalyst might not be the state in which the catalyst was prepared, but rather a structural and/or chemical isomer that adapted to the particular reaction conditions. To address the complexity of real-world catalysts, a synergistic approach taking advantage of a variety of cutting-edge experimental methods must be undertaken.
This project focuses on model heterogeneous catalysts for reactions of tremendous societal and industrial relevance, namely the gas-phase hydrogenation and electrocatalytic reduction of CO2. Important components that are missing from existing studies, and that we propose to contribute, are a systematic design of catalytically active model NPs with narrow size and shape distributions and tunable oxidation state, and in situ and operando structural, chemical, and reactivity characterization of such model catalysts as a function of the reaction environment. The results are expected to open up new routes for the reutilization of CO2 through its direct conversion into valuable chemicals and fuels such as methanol, methane and ethylene.
Summary
Tailoring the chemical reactivity of nanomaterials at the atomic level is one of the most important challenges in catalysis research. In order to achieve this elusive goal, fundamental understanding of the structural and chemical properties of these complex systems must be obtained. Numerous studies have been devoted to understanding the properties that affect the catalytic performance of metal nanoparticles (NPs) such as their size, interaction with the support, and chemical state. The role played by the NP shape on catalytic performance is, however, less understood. Complicating the analysis is the fact that the former parameters cannot be considered independently, since the NP size as well as the support will have an impact on the most stable NP shapes. In addition, the dynamic nature of the NP catalysts and their response to the environment must be taken into consideration, since the working state of a NP catalyst might not be the state in which the catalyst was prepared, but rather a structural and/or chemical isomer that adapted to the particular reaction conditions. To address the complexity of real-world catalysts, a synergistic approach taking advantage of a variety of cutting-edge experimental methods must be undertaken.
This project focuses on model heterogeneous catalysts for reactions of tremendous societal and industrial relevance, namely the gas-phase hydrogenation and electrocatalytic reduction of CO2. Important components that are missing from existing studies, and that we propose to contribute, are a systematic design of catalytically active model NPs with narrow size and shape distributions and tunable oxidation state, and in situ and operando structural, chemical, and reactivity characterization of such model catalysts as a function of the reaction environment. The results are expected to open up new routes for the reutilization of CO2 through its direct conversion into valuable chemicals and fuels such as methanol, methane and ethylene.
Max ERC Funding
2 000 000 €
Duration
Start date: 2017-05-01, End date: 2022-04-30
Project acronym ORDERin1D
Project Order in one dimension: Functional hybrids of chirality-sorted carbon nanotubes
Researcher (PI) Sofie Cambré
Host Institution (HI) UNIVERSITEIT ANTWERPEN
Call Details Starting Grant (StG), PE4, ERC-2015-STG
Summary The hollow structure of carbon nanotubes (CNTs) with a wide range of diameters forms an ideal one-dimensional host system to study restricted diameter-dependent molecular transport and to achieve unique polar molecular order. For the ORDERin1D project, I will capitalize on my recent breakthroughs in the processing, filling, chiral sorting and high-resolution spectroscopic characterization of empty and filled CNTs, aiming for a diameter-dependent characterization of the filling with various molecules, which will pave the way for the rational design of ultraselective filtermembranes, sensors, nanofluidic devices and nanohybrids with unseen control over the structural order at the molecular scale. In particular, I recently found that dipolar molecules naturally align head-to-tail into a polar array inside the CNTs, after which their molecular directional properties such as their dipole moment and second-order nonlinear optical responses add up coherently, groundbreaking for the development of nanophotonics applications.
Summary
The hollow structure of carbon nanotubes (CNTs) with a wide range of diameters forms an ideal one-dimensional host system to study restricted diameter-dependent molecular transport and to achieve unique polar molecular order. For the ORDERin1D project, I will capitalize on my recent breakthroughs in the processing, filling, chiral sorting and high-resolution spectroscopic characterization of empty and filled CNTs, aiming for a diameter-dependent characterization of the filling with various molecules, which will pave the way for the rational design of ultraselective filtermembranes, sensors, nanofluidic devices and nanohybrids with unseen control over the structural order at the molecular scale. In particular, I recently found that dipolar molecules naturally align head-to-tail into a polar array inside the CNTs, after which their molecular directional properties such as their dipole moment and second-order nonlinear optical responses add up coherently, groundbreaking for the development of nanophotonics applications.
Max ERC Funding
1 499 425 €
Duration
Start date: 2016-05-01, End date: 2021-04-30
Project acronym P-MEM-NMR
Project Structure of paramagnetic integral membrane metalloproteins by MAS-NMR
Researcher (PI) Guido Pintacuda
Host Institution (HI) CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE CNRS
Call Details Consolidator Grant (CoG), PE4, ERC-2014-CoG
Summary Integral membrane metalloproteins are involved in the transport and homeostasis of metal ions, as well as in key redox reactions that have a tremendous impact on many fields within life sciences, environment, energy, and industry.
Most of our understanding of fine details of biochemical processes derives from atomic or molecular structures obtained by diffraction methods on single crystal samples. However, in the case of integral membrane systems, single crystals large enough for X-ray diffraction cannot be easily obtained, and the problem of structure elucidation is largely unsolved.
We have recently pioneered a breakthrough approach using Magic-Angle Spinning Nuclear Magnetic Resonance (MAS-NMR) for the atomic-level characterization of paramagnetic materials and complex biological macromolecules. The proposed project aims to leverage these new advances through a series of new concepts i) to improve the resolution and sensitivity of MAS-NMR from nuclei surrounding a paramagnetic metal ion, such as e.g. cobalt, nickel and iron, and ii) to extend its applicability to large integral membrane proteins in lipid membrane environments. With these methods, we will enable the determination of structure-activity relationships in integral membrane metalloenzymes and transporters, by combining the calculation of global structure and dynamics with measurement of the electronic features of metal ions.
These goals require a leap forward with respect to today’s protocols, and we propose to achieve this through a combination of innovative NMR experiments and isotopic labeling, faster MAS rates and high magnetic fields. As outlined here, the approaches go well beyond the frontier of current research. The project will yield a broadly applicable method for the structural characterization of essential cellular processes and thereby will provide a powerful tool to solve challenges at the forefront of molecular and chemical sciences today.
Summary
Integral membrane metalloproteins are involved in the transport and homeostasis of metal ions, as well as in key redox reactions that have a tremendous impact on many fields within life sciences, environment, energy, and industry.
Most of our understanding of fine details of biochemical processes derives from atomic or molecular structures obtained by diffraction methods on single crystal samples. However, in the case of integral membrane systems, single crystals large enough for X-ray diffraction cannot be easily obtained, and the problem of structure elucidation is largely unsolved.
We have recently pioneered a breakthrough approach using Magic-Angle Spinning Nuclear Magnetic Resonance (MAS-NMR) for the atomic-level characterization of paramagnetic materials and complex biological macromolecules. The proposed project aims to leverage these new advances through a series of new concepts i) to improve the resolution and sensitivity of MAS-NMR from nuclei surrounding a paramagnetic metal ion, such as e.g. cobalt, nickel and iron, and ii) to extend its applicability to large integral membrane proteins in lipid membrane environments. With these methods, we will enable the determination of structure-activity relationships in integral membrane metalloenzymes and transporters, by combining the calculation of global structure and dynamics with measurement of the electronic features of metal ions.
These goals require a leap forward with respect to today’s protocols, and we propose to achieve this through a combination of innovative NMR experiments and isotopic labeling, faster MAS rates and high magnetic fields. As outlined here, the approaches go well beyond the frontier of current research. The project will yield a broadly applicable method for the structural characterization of essential cellular processes and thereby will provide a powerful tool to solve challenges at the forefront of molecular and chemical sciences today.
Max ERC Funding
2 499 375 €
Duration
Start date: 2015-09-01, End date: 2020-08-31
Project acronym PARAMIR
Project Investigating micro-RNA Dynamics using Paramagnetic NMR Spectroscopy
Researcher (PI) Loic SALMON
Host Institution (HI) CENTRE NATIONAL DE LA RECHERCHE SCIENTIFIQUE CNRS
Call Details Starting Grant (StG), PE4, ERC-2018-STG
Summary Over the last decades, new discoveries have revealed an ever-increasing diversity of RNA functions, profoundly modifying the conceptual framework of molecular biology. This is the case of micro-RNAs (miRNA), a fascinating class of small non-coding RNA that play essential roles in RNA induced gene silencing and are estimated to target up to 60% of protein-coding genes in humans.
RNA functional diversity is often triggered by conformational changes, so capturing the dynamics of these molecules is key to a precise understanding of their function, which in turn is essential to control their activity. Nuclear Magnetic Resonance (NMR) spectroscopy is extremely well suited to investigate dynamical processes. However, the sparsity of measureable NMR data in a RNA sample represents a major bottleneck, preventing so far an accurate description of RNA conformational fluctuations.
This project aims to overcome this barrier by developing paramagnetic NMR for RNA. By chemically modifying an RNA, I will introduce paramagnetic tags to strategic positions so as to acquire NMR data from otherwise silent substrate. Adequate computational and analytical models will be developed to decode the experimental data into an atomic-level description of dynamics.
These goals require a leap forward with respect to today’s approaches. I propose to achieve this by combining innovative sample preparation strategies and NMR experiments, high magnetic fields, and MD simulations. With these methods, I will enable the determination of the dynamic landscape of let-7, the first miRNA discovered in humans, involved in cell proliferation and differentiation and oncogenesis.
This project will yield a broadly applicable method for the structural and dynamic characterization of RNA with unprecedented details. This knowledge will improve our fundamental biochemical and biophysical conception of RNA, opening new avenues for bioengineering and establishing the bases for rational RNA-oriented drug discovery.
Summary
Over the last decades, new discoveries have revealed an ever-increasing diversity of RNA functions, profoundly modifying the conceptual framework of molecular biology. This is the case of micro-RNAs (miRNA), a fascinating class of small non-coding RNA that play essential roles in RNA induced gene silencing and are estimated to target up to 60% of protein-coding genes in humans.
RNA functional diversity is often triggered by conformational changes, so capturing the dynamics of these molecules is key to a precise understanding of their function, which in turn is essential to control their activity. Nuclear Magnetic Resonance (NMR) spectroscopy is extremely well suited to investigate dynamical processes. However, the sparsity of measureable NMR data in a RNA sample represents a major bottleneck, preventing so far an accurate description of RNA conformational fluctuations.
This project aims to overcome this barrier by developing paramagnetic NMR for RNA. By chemically modifying an RNA, I will introduce paramagnetic tags to strategic positions so as to acquire NMR data from otherwise silent substrate. Adequate computational and analytical models will be developed to decode the experimental data into an atomic-level description of dynamics.
These goals require a leap forward with respect to today’s approaches. I propose to achieve this by combining innovative sample preparation strategies and NMR experiments, high magnetic fields, and MD simulations. With these methods, I will enable the determination of the dynamic landscape of let-7, the first miRNA discovered in humans, involved in cell proliferation and differentiation and oncogenesis.
This project will yield a broadly applicable method for the structural and dynamic characterization of RNA with unprecedented details. This knowledge will improve our fundamental biochemical and biophysical conception of RNA, opening new avenues for bioengineering and establishing the bases for rational RNA-oriented drug discovery.
Max ERC Funding
1 633 500 €
Duration
Start date: 2019-02-01, End date: 2024-01-31
Project acronym pcCell
Project Physicochemical principles of efficient information processing in biological cells
Researcher (PI) Frank Noe
Host Institution (HI) FREIE UNIVERSITAET BERLIN
Call Details Starting Grant (StG), PE4, ERC-2012-StG_20111012
Summary Biological cellular function relies on the coordination of many information processing steps in which specific biomolecular complexes are formed. But how can proteins and ligands find their targets in extremely crowded cellular membranes or cytosol? Here, I propose that intracellular signal processing depends upon the spatiotemporal order of molecules arising from “dynamical sorting”, i.e. no stable structure may exist at any time and yet the molecules might be ordered at all times. I propose to investigate the existence and the physicochemical driving forces of such dynamical sorting mechanisms in selected neuronal synaptic membrane proteins that must be tightly coordinated during neurotransmission and recovery. To this end, massive atomistic and coarse-grained molecular simulations will be combined with statistical mechanical theory, producing predictions to be experimentally validated through our collaborators.
The main methodological challenge of this proposal is the infamous sampling problem: Even with immense computational effort, unbiased molecular dynamics trajectory lengths are at most microseconds for the protein systems considered here. This is insufficient to calculate relevant states, probabilities, and rates for these systems. Based on recent mathematical and computational groundwork developed by us and others, I propose to develop enhanced sampling methods that will yield an effective speedup of at least 4 orders of magnitude over current simulations. This will allow protein-ligand and protein-protein interactions to be sampled efficiently using atomistic models, thus having far reaching impact on the field.
The proposed project is at the forefront of an interdisciplinary field, spanning traditional areas such as physical chemistry, computer science, mathematics, and biology. The project claims fundamental advances in both simulation techniques and in the understanding of the physicochemical principles that govern the functionality of the cell
Summary
Biological cellular function relies on the coordination of many information processing steps in which specific biomolecular complexes are formed. But how can proteins and ligands find their targets in extremely crowded cellular membranes or cytosol? Here, I propose that intracellular signal processing depends upon the spatiotemporal order of molecules arising from “dynamical sorting”, i.e. no stable structure may exist at any time and yet the molecules might be ordered at all times. I propose to investigate the existence and the physicochemical driving forces of such dynamical sorting mechanisms in selected neuronal synaptic membrane proteins that must be tightly coordinated during neurotransmission and recovery. To this end, massive atomistic and coarse-grained molecular simulations will be combined with statistical mechanical theory, producing predictions to be experimentally validated through our collaborators.
The main methodological challenge of this proposal is the infamous sampling problem: Even with immense computational effort, unbiased molecular dynamics trajectory lengths are at most microseconds for the protein systems considered here. This is insufficient to calculate relevant states, probabilities, and rates for these systems. Based on recent mathematical and computational groundwork developed by us and others, I propose to develop enhanced sampling methods that will yield an effective speedup of at least 4 orders of magnitude over current simulations. This will allow protein-ligand and protein-protein interactions to be sampled efficiently using atomistic models, thus having far reaching impact on the field.
The proposed project is at the forefront of an interdisciplinary field, spanning traditional areas such as physical chemistry, computer science, mathematics, and biology. The project claims fundamental advances in both simulation techniques and in the understanding of the physicochemical principles that govern the functionality of the cell
Max ERC Funding
1 397 328 €
Duration
Start date: 2013-01-01, End date: 2017-12-31
Project acronym PhotoMutant
Project Rational Design of Photoreceptor Mutants with Desired Photochemical Properties
Researcher (PI) Igor Schapiro
Host Institution (HI) THE HEBREW UNIVERSITY OF JERUSALEM
Call Details Starting Grant (StG), PE4, ERC-2015-STG
Summary From a technological viewpoint photoreceptor proteins, the light-sensitive proteins involved in the sensing and response to light in a variety of organisms, represent biological light converters. Hence they are successfully utilized in a number of technological applications, e.g. the green-fluorescent protein used to visualize spatial and temporal information in cells. However, despite the ground-breaking nature of this utilization in life science and other disciplines, the attempts to design a photoreceptor for a particular application by protein mutation remains an open challenge. This is exactly the scope of my research proposal: the application of multi-scale modelling for the systematic design of biological photoreceptor mutants.
With this target in mind I will study representatives of two prominent photoreceptor proteins subfamilies which are of towering interest to experimentalists: proteorhodopsins and cyanobacteriochromes. Computer models of these proteins will be constructed using accurate multi-scale modeling. Their excitation energies and other properties (e.g. excited-state reactivity and efficiency) will be calculated using multireference methods that were shown to have an accuracy of <3 kcal/mol. The insights gained from simulations of the wild-type proteins will provide the basis for proposing mutations with altered photochemical properties: in essence to predict absorption and emission spectra, excited-state lifetime and quantum yields.
This research requires interactions across the disciplines, as the best candidates will be synthesized and characterized experimentally by collaborators. The outcome of these experiments will provide feedback to improve both the properties of the mutants and the simulation methodology. Ultimately this high-risk/high gain project should derive a comprehensive understanding that would result in novel biotechnological applications, e.g. optogenetic tools, fluorescent probes and biosensors.
Summary
From a technological viewpoint photoreceptor proteins, the light-sensitive proteins involved in the sensing and response to light in a variety of organisms, represent biological light converters. Hence they are successfully utilized in a number of technological applications, e.g. the green-fluorescent protein used to visualize spatial and temporal information in cells. However, despite the ground-breaking nature of this utilization in life science and other disciplines, the attempts to design a photoreceptor for a particular application by protein mutation remains an open challenge. This is exactly the scope of my research proposal: the application of multi-scale modelling for the systematic design of biological photoreceptor mutants.
With this target in mind I will study representatives of two prominent photoreceptor proteins subfamilies which are of towering interest to experimentalists: proteorhodopsins and cyanobacteriochromes. Computer models of these proteins will be constructed using accurate multi-scale modeling. Their excitation energies and other properties (e.g. excited-state reactivity and efficiency) will be calculated using multireference methods that were shown to have an accuracy of <3 kcal/mol. The insights gained from simulations of the wild-type proteins will provide the basis for proposing mutations with altered photochemical properties: in essence to predict absorption and emission spectra, excited-state lifetime and quantum yields.
This research requires interactions across the disciplines, as the best candidates will be synthesized and characterized experimentally by collaborators. The outcome of these experiments will provide feedback to improve both the properties of the mutants and the simulation methodology. Ultimately this high-risk/high gain project should derive a comprehensive understanding that would result in novel biotechnological applications, e.g. optogenetic tools, fluorescent probes and biosensors.
Max ERC Funding
1 397 475 €
Duration
Start date: 2016-02-01, End date: 2021-01-31
Project acronym PINNACLE
Project Perovskite Nanocrystal-Nanoreactors for Enhanced Light Emission
Researcher (PI) Alexander URBAN
Host Institution (HI) LUDWIG-MAXIMILIANS-UNIVERSITAET MUENCHEN
Call Details Starting Grant (StG), PE4, ERC-2017-STG
Summary The unprecedented advancement of halide perovskite photovoltaics and light-emission applications has far outpaced the basic scientific research necessary to understand this fascinating yet perplexing material and to optimize material quality and device integration. Additionally, the intricate nature of the perovskite is susceptible to degradation from environmental stress, such as moisture and heat, currently deterring commercialization.
This research project will realize a novel synthesis for perovskite nanocrystals (NCs) by means of block copolymer nanoreactors. These will enable an unprecedented control over size and dimensionality of the NCs into the quantum-confinement regime. Using these NCs, we will determine the fundamental optical, electrical, and phononic properties of perovskite, mainly by means of temperature-controlled transient optical spectroscopy.
Elucidation of the degradation mechanisms through controlled subjecting to external stress, will lead to strategies for designing the nanoreactor to shield the NCs, mitigating these effects. Additionally, we will investigate the high mobility of (halide) ions in perovskites, and likewise design the polymeric nanoreactor to deter ion migration and enable NC implementation into existing optoelectronic applications and currently unattainable architectures, such as hetero-structures and exciton funnels.
We will create stable, high-quality NC-films, enabling the formation of multilayers for exciton funnelling by means of Förster resonance energy transfer (FRET). We will highlight the NC potential by integrating them into LEDs of various architectures, by demonstrating low-threshold ASE and realizing unprecedented perovskite-laser geometries, e.g. vertical cavity surface emitting lasers (VCSELs) and plasmonic nanopatch lasers.
PINNACLE will greatly further the understanding of halide perovskites, benefitting the research community, and lead to novel optoelectronic devices and exciting new applications.
Summary
The unprecedented advancement of halide perovskite photovoltaics and light-emission applications has far outpaced the basic scientific research necessary to understand this fascinating yet perplexing material and to optimize material quality and device integration. Additionally, the intricate nature of the perovskite is susceptible to degradation from environmental stress, such as moisture and heat, currently deterring commercialization.
This research project will realize a novel synthesis for perovskite nanocrystals (NCs) by means of block copolymer nanoreactors. These will enable an unprecedented control over size and dimensionality of the NCs into the quantum-confinement regime. Using these NCs, we will determine the fundamental optical, electrical, and phononic properties of perovskite, mainly by means of temperature-controlled transient optical spectroscopy.
Elucidation of the degradation mechanisms through controlled subjecting to external stress, will lead to strategies for designing the nanoreactor to shield the NCs, mitigating these effects. Additionally, we will investigate the high mobility of (halide) ions in perovskites, and likewise design the polymeric nanoreactor to deter ion migration and enable NC implementation into existing optoelectronic applications and currently unattainable architectures, such as hetero-structures and exciton funnels.
We will create stable, high-quality NC-films, enabling the formation of multilayers for exciton funnelling by means of Förster resonance energy transfer (FRET). We will highlight the NC potential by integrating them into LEDs of various architectures, by demonstrating low-threshold ASE and realizing unprecedented perovskite-laser geometries, e.g. vertical cavity surface emitting lasers (VCSELs) and plasmonic nanopatch lasers.
PINNACLE will greatly further the understanding of halide perovskites, benefitting the research community, and lead to novel optoelectronic devices and exciting new applications.
Max ERC Funding
1 498 188 €
Duration
Start date: 2018-03-01, End date: 2023-02-28
Project acronym PORPHDYN
Project STRUCTURE AND DYNAMICS OF PORPHYRIN-BASED MATERIALS IN SOLUTION vs. INTERFACES
Researcher (PI) Emad Flear Aziz Bekhit
Host Institution (HI) HELMHOLTZ-ZENTRUM BERLIN FUR MATERIALIEN UND ENERGIE GMBH
Call Details Starting Grant (StG), PE4, ERC-2011-StG_20101014
Summary The goal of the proposed project is to perform a systematic study of the electronic structure and the dynamic behaviour of specifically selected metalloporphyrin materials in solution, and at liquid-solid interfaces, with a time resolution covering the range from sub-femtosecond up to picoseconds which is fundamental for their biochemical properties. Metalloporphyrins play a key role in a wide range of processes, such as the light energy conversion in photosynthesis, or in haem proteins performing the transport of small ligands like oxygen. Because of their peculiar optical, electronic and magnetic properties, they are potential candidates for technological applications like in molecular electronics. It is of fundamental importance to gain a detailed understanding of the structural and dynamic properties of these materials under realistic conditions (i.e. ambient pressure, room temperature, and in heterogeneous environments). Soft X-ray spectroscopy is an ideal tool for this purpose, which has recently been implemented by the PI for the investigation of applied materials in the liquid phase, drawing on international recognition of his achievements. Taking advantage from his broad expertise, the PI extended the soft X-ray spectroscopy to biochemical systems in solutions for the first time. Since last year the PI became the youngest group leader at HZB, and Junior Professor at the Freie Universität Berlin. Here, the PI proposes to use the laser pump / soft X-ray probe spectroscopy at first in the sub-picosecond domain. The experiments will extended to femtosecond resolution at the X-ray Free Electron Laser facility. To address sub-femtosecond processes, the systematic scanning of the systems with core-clock spectroscopy is intended. The study will provide fundamental knowledge about the electronic structure and dynamics of metalloporphyrin materials which are essential for different applications, thus helping significantly to enhance their performance.
Summary
The goal of the proposed project is to perform a systematic study of the electronic structure and the dynamic behaviour of specifically selected metalloporphyrin materials in solution, and at liquid-solid interfaces, with a time resolution covering the range from sub-femtosecond up to picoseconds which is fundamental for their biochemical properties. Metalloporphyrins play a key role in a wide range of processes, such as the light energy conversion in photosynthesis, or in haem proteins performing the transport of small ligands like oxygen. Because of their peculiar optical, electronic and magnetic properties, they are potential candidates for technological applications like in molecular electronics. It is of fundamental importance to gain a detailed understanding of the structural and dynamic properties of these materials under realistic conditions (i.e. ambient pressure, room temperature, and in heterogeneous environments). Soft X-ray spectroscopy is an ideal tool for this purpose, which has recently been implemented by the PI for the investigation of applied materials in the liquid phase, drawing on international recognition of his achievements. Taking advantage from his broad expertise, the PI extended the soft X-ray spectroscopy to biochemical systems in solutions for the first time. Since last year the PI became the youngest group leader at HZB, and Junior Professor at the Freie Universität Berlin. Here, the PI proposes to use the laser pump / soft X-ray probe spectroscopy at first in the sub-picosecond domain. The experiments will extended to femtosecond resolution at the X-ray Free Electron Laser facility. To address sub-femtosecond processes, the systematic scanning of the systems with core-clock spectroscopy is intended. The study will provide fundamental knowledge about the electronic structure and dynamics of metalloporphyrin materials which are essential for different applications, thus helping significantly to enhance their performance.
Max ERC Funding
1 499 000 €
Duration
Start date: 2011-09-01, End date: 2016-08-31
Project acronym PPOLAH
Project Predicting Properties of Large Heterogeneous Systems with Optimally-Tuned Range-Separated Hybrid Functionals
Researcher (PI) Leeor Kronik
Host Institution (HI) WEIZMANN INSTITUTE OF SCIENCE
Call Details Starting Grant (StG), PE4, ERC-2011-StG_20101014
Summary I propose to develop a broadly applicable, quantitatively reliable, computationally simple approach to the study of large heterogeneous systems, and to apply it to important problems in molecular and organic electronics and photovoltaics. This will be based on a radically different approach to the development and application of density functional theory (DFT) - determining an optimally yet non-empirically tuned system-specific functional, instead of seeking a universally applicable one.
Large heterogeneous systems are vital to several of the most burning challenges facing materials science. Perhaps most notably, this includes materials systems relevant for basic energy sciences, e.g., for photovoltaics or photocatalysis, but also includes, e.g., organic/inorganic interfaces that are crucial for molecular, organic, and hybrid organic/inorganic (opto)electronic systems. Theory and modelling of such systems face many challenges and would benefit greatly from accurate first principles calculations. However, the “work-horse” of such large-scale calculations – DFT – faces multiple, serious challenges when applied to such systems. This includes treating systems with components of different chemical nature, predicting energy level alignment, predicting charge transfer, handling weak interactions, and more. Solving all these problems within conventional DFT is extremely difficult, and even if at all possible the result will likely be too computationally complex for many applications.
Instead, I propose a completely different strategy - sacrifice the quest for an all-purpose functional and focus on per-system physical criteria that can fix system-specific parameters without recourse to empiricism. The additional flexibility would help us gain tremendously in simplicity and applicability without loss of predictive power. I propose a practical scheme based on tunable range-separated hybrid functionals and a plan for its application to a wide range of practical systems.
Summary
I propose to develop a broadly applicable, quantitatively reliable, computationally simple approach to the study of large heterogeneous systems, and to apply it to important problems in molecular and organic electronics and photovoltaics. This will be based on a radically different approach to the development and application of density functional theory (DFT) - determining an optimally yet non-empirically tuned system-specific functional, instead of seeking a universally applicable one.
Large heterogeneous systems are vital to several of the most burning challenges facing materials science. Perhaps most notably, this includes materials systems relevant for basic energy sciences, e.g., for photovoltaics or photocatalysis, but also includes, e.g., organic/inorganic interfaces that are crucial for molecular, organic, and hybrid organic/inorganic (opto)electronic systems. Theory and modelling of such systems face many challenges and would benefit greatly from accurate first principles calculations. However, the “work-horse” of such large-scale calculations – DFT – faces multiple, serious challenges when applied to such systems. This includes treating systems with components of different chemical nature, predicting energy level alignment, predicting charge transfer, handling weak interactions, and more. Solving all these problems within conventional DFT is extremely difficult, and even if at all possible the result will likely be too computationally complex for many applications.
Instead, I propose a completely different strategy - sacrifice the quest for an all-purpose functional and focus on per-system physical criteria that can fix system-specific parameters without recourse to empiricism. The additional flexibility would help us gain tremendously in simplicity and applicability without loss of predictive power. I propose a practical scheme based on tunable range-separated hybrid functionals and a plan for its application to a wide range of practical systems.
Max ERC Funding
1 500 000 €
Duration
Start date: 2011-09-01, End date: 2016-08-31
