Chemical Applications of Velocity and Spatial Imaging
Lead Research Organisation:
University of Bristol
Department Name: Chemistry
Abstract
Ion imaging, first demonstrated just 25 years ago, is already having a major impact on the way we explore molecular change (the very essence of chemistry) in many gas phase systems. The technique has features in common with mass spectrometry (MS). Both start by removing an electron from the target species, generating ions, i.e. charged molecules or fragments, which are then 'sorted' by their mass. In traditional MS, the species of interest is characterised by its spectrum of ion yield versus mass. Electron removal in most ion imaging experiments is induced by a short pulse of laser light; the resulting ions are then accelerated towards a time and position sensitive detector. Heavier ions travel more slowly, so one can image ions of just one particular mass by ensuring that the detector is only 'on' at the appropriate time. The spatial pattern of ion impacts that builds up on the detector when the experiment is repeated many times is visually intuitive, and provides quantitative energetic information about the reaction(s) that yields the monitored product. However, the read out time of current ion imaging detectors is too slow to allow imaging of ions with different mass formed in the same laser shot, and many species are not readily amenable to ionisation in current ion imaging schemes. Imaging all products from a given reaction is therefore time consuming (at best) and, at worst, impossible.
We seek to solve both these limitations. Two of the team have already demonstrated new, much faster, time and position sensitive sensors capable of imaging multiple masses in a single shot experiment. This multimass imaging capability will be developed further and rolled-out for use and refinement across the team. We also propose new multiphoton ionization schemes as well as 'universal' ion formation methods based on use of shorter laser wavelengths or short duration pulses of energy selected electrons. The following over-arching scientific ambitions will proceed in parallel, and exploit the foregoing advances in ion imaging technology at the earliest possible opportunity:
(i) We will use the latest ion imaging methods to explore molecular change in the gas phase, focusing on key families of (photo)chemical reactions: addition, dissociation, cyclisation and ring opening reactions of organic molecules, and metal-ligand and metal-cluster interactions. These choices reflect the importance of such reactions in synthesis, catalysis, etc., their amenability to complementary high level theory, and our ability to explore the same reactions in solution (using a new ultrafast pump-probe laser spectroscopy facility). Determining the extent to which the mechanisms and energetics of reactions established through exquisitely detailed gas phase studies can inform our understanding of reactivity in the condensed phase is a current 'hot' issue in chemical science, which the team is ideally placed to address.
(ii) We will develop and exploit new multi-dimensional analytical methods with combined mass, structural and spatial resolution. Mass spectra usually show many peaks attributable to fragment ions, but the paths by which these are formed are often unclear. Imaging MS is proposed as a novel means of unravelling different routes to forming a given fragment ion; distinguishing and characterising such pathways can offer new insights into, for example, peptide structure. Yet more ambitious, we propose to combine multimass and spatial map imaging with existing laser desorption/ionisation methods to enable spatially resolved compositional analysis of surfaces and of samples on surfaces. Such a capability will offer new opportunities in diverse activities like tissue imaging (e.g. detection of metal ions within tissue specimens of relevance to understanding the failure of some metal-on-metal hip implants), forensic analysis (e.g. 'chemical' imaging of fingerprints, inks, dyes, pollens, etc) and parallel mass spectrometric sampling (e.g. of blood samples).
We seek to solve both these limitations. Two of the team have already demonstrated new, much faster, time and position sensitive sensors capable of imaging multiple masses in a single shot experiment. This multimass imaging capability will be developed further and rolled-out for use and refinement across the team. We also propose new multiphoton ionization schemes as well as 'universal' ion formation methods based on use of shorter laser wavelengths or short duration pulses of energy selected electrons. The following over-arching scientific ambitions will proceed in parallel, and exploit the foregoing advances in ion imaging technology at the earliest possible opportunity:
(i) We will use the latest ion imaging methods to explore molecular change in the gas phase, focusing on key families of (photo)chemical reactions: addition, dissociation, cyclisation and ring opening reactions of organic molecules, and metal-ligand and metal-cluster interactions. These choices reflect the importance of such reactions in synthesis, catalysis, etc., their amenability to complementary high level theory, and our ability to explore the same reactions in solution (using a new ultrafast pump-probe laser spectroscopy facility). Determining the extent to which the mechanisms and energetics of reactions established through exquisitely detailed gas phase studies can inform our understanding of reactivity in the condensed phase is a current 'hot' issue in chemical science, which the team is ideally placed to address.
(ii) We will develop and exploit new multi-dimensional analytical methods with combined mass, structural and spatial resolution. Mass spectra usually show many peaks attributable to fragment ions, but the paths by which these are formed are often unclear. Imaging MS is proposed as a novel means of unravelling different routes to forming a given fragment ion; distinguishing and characterising such pathways can offer new insights into, for example, peptide structure. Yet more ambitious, we propose to combine multimass and spatial map imaging with existing laser desorption/ionisation methods to enable spatially resolved compositional analysis of surfaces and of samples on surfaces. Such a capability will offer new opportunities in diverse activities like tissue imaging (e.g. detection of metal ions within tissue specimens of relevance to understanding the failure of some metal-on-metal hip implants), forensic analysis (e.g. 'chemical' imaging of fingerprints, inks, dyes, pollens, etc) and parallel mass spectrometric sampling (e.g. of blood samples).
Planned Impact
Five technical work packages (TWPs) underpinning four substantial scientific work packages (SWPs) are proposed. The TWPs centre on new and improved methods of (i) creating charged particles, (ii) detecting/imaging them with improved velocity, spatial and/or time resolution and (iii) integrated high-level modelling of the results of experiments (photodissociation or photoionization processes, bimolecular reactions, surface desorptions, etc) which depend on such measurements. Short term beneficiaries include the economy (e.g. companies developing and manufacturing improved fast charged particle imaging detectors/sensors, with several of whom consortium members already collaborate). Such devices already find many applications of benefit to society (e.g. monitoring bioluminescence, corona imaging, fluorescence lifetime imaging, time resolved imaging, high speed and/or low light level imaging, security detection systems, threat detection systems, missile warning systems, space science, etc), but the quest for new and improved performance is unending. On the longer term (but within the timescale of the PG), fast sensors of the type envisaged here should offer new opportunities in mass spectrometry (e.g. imaging mass spectrometry) - a pivotal research and analysis tool in broad areas of physical and life science - and more widely (e.g. in neutron science, electron microscopy, etc). Interest in new and improved neutron detectors has soared as a result of the current world shortage of 3He.
Apart from Instrument Development, the proposed SWP activities are envisaged to have longer term impact in several other areas of the EPSRC Portfolio: Healthcare Technologies (e.g. chemical analysis of bioarrays and tissue analysis, enabled by new high fidelity, mass selective, spatially resolved imaging methods), Energy (e.g. via improved understanding of catalytic sites and surfaces from gas phase, gas-surface and condensed phase studies), Manufacturing for the Future (e.g. improved understanding and application of condensed phase (photo)chemical reactivity). The latter SWP also impacts on the Dial-a-Molecule Grand Challenge in Chemistry - by providing a deeper understanding of chemical reactivity and the promise of greater control. Such science boosts the pool of knowledge available to synthetic chemists, the pharmaceutical industry, etc; the strength of associated synthetic chemistry and biochemistry groups at Bristol (which hosts the CDT in Chemical Synthesis) and at Oxford will help ensure efficient knowledge transfer.
Longer term benefits for society in general, the knowledge base and people will be delivered through the training of a new generation of research leaders skilled in quantitative, cutting edge experimental and theoretical physical chemistry/chemical physics, capable of identifying and solving problems of global importance, and by the development and application of novel instrumentation coupled with integrated high-level computational modelling. Recent destinations for group members include academia (e.g. new appointees at UC Irvine, Heriot Watt, Newcastle), post-doctoral research (e.g. UC Berkeley, VU Amsterdam, Berlin, Lausanne, Space Science Group and Diamond Synchrotron at RAL) and industry (e.g. Du Pont, Malvern Instruments, AWE, Shell International).
Apart from Instrument Development, the proposed SWP activities are envisaged to have longer term impact in several other areas of the EPSRC Portfolio: Healthcare Technologies (e.g. chemical analysis of bioarrays and tissue analysis, enabled by new high fidelity, mass selective, spatially resolved imaging methods), Energy (e.g. via improved understanding of catalytic sites and surfaces from gas phase, gas-surface and condensed phase studies), Manufacturing for the Future (e.g. improved understanding and application of condensed phase (photo)chemical reactivity). The latter SWP also impacts on the Dial-a-Molecule Grand Challenge in Chemistry - by providing a deeper understanding of chemical reactivity and the promise of greater control. Such science boosts the pool of knowledge available to synthetic chemists, the pharmaceutical industry, etc; the strength of associated synthetic chemistry and biochemistry groups at Bristol (which hosts the CDT in Chemical Synthesis) and at Oxford will help ensure efficient knowledge transfer.
Longer term benefits for society in general, the knowledge base and people will be delivered through the training of a new generation of research leaders skilled in quantitative, cutting edge experimental and theoretical physical chemistry/chemical physics, capable of identifying and solving problems of global importance, and by the development and application of novel instrumentation coupled with integrated high-level computational modelling. Recent destinations for group members include academia (e.g. new appointees at UC Irvine, Heriot Watt, Newcastle), post-doctoral research (e.g. UC Berkeley, VU Amsterdam, Berlin, Lausanne, Space Science Group and Diamond Synchrotron at RAL) and industry (e.g. Du Pont, Malvern Instruments, AWE, Shell International).
Organisations
- University of Bristol (Lead Research Organisation)
- Complutense University of Madrid (Collaboration)
- Deutsches Electronen-Synchrotron (DESY) (Collaboration)
- University of Innsbruck (Collaboration)
- University of Warwick (Collaboration)
- University of Kyoto (Collaboration)
- University of Maryland, College Park (Collaboration)
- Max Planck Society (Collaboration)
- Johns Hopkins University (Collaboration)
- Stanford University (Collaboration)
- Radboud University Nijmegen (Collaboration)
- Rosalind Franklin Institute (Collaboration)
- University of Santiago de Compostela (Collaboration)
- Aarhus University (Collaboration)
- Technical University Berlin (Collaboration)
- Dalian Institute of Chemical Physics (Collaboration)
- University of Gothenburg (Collaboration)
- Hokkaido University (Collaboration)
- University of Louisiana at Lafayette (Collaboration)
- Sandia Laboratories (Collaboration)
- National Research Council - Ottawa (Collaboration)
- Lomonosov Moscow State University (Collaboration)
- Kansas State University (Collaboration)
- Scientific Analysis Instruments Ltd (Project Partner)
- Photek (United Kingdom) (Project Partner)
Publications
Cunningham EM
(2017)
Infrared Signature of Structural Isomers of Gas-Phase M+(N2O)n (M = Cu, Ag, Au) Ion-Molecule Complexes.
in The journal of physical chemistry. A
Eland JH
(2016)
Dissociation of multiply charged ICN by Coulomb explosion.
in The Journal of chemical physics
Essafi S
(2017)
The Dynamics of the Reaction of FeO + and H 2 : A Model for Inorganic Oxidation
in Angewandte Chemie
Essafi S
(2017)
The Dynamics of the Reaction of FeO+ and H2 : A Model for Inorganic Oxidation.
in Angewandte Chemie (International ed. in English)
Essafi S
(2018)
Rates of Molecular Vibrational Energy Transfer in Organic Solutions.
in The journal of physical chemistry. A
Figueira Nunes JP
(2024)
Monitoring the Evolution of Relative Product Populations at Early Times during a Photochemical Reaction.
in Journal of the American Chemical Society
Forbes R
(2017)
Time-resolved multi-mass ion imaging: Femtosecond UV-VUV pump-probe spectroscopy with the PImMS camera.
in The Journal of chemical physics
Forbes R
(2020)
Time-resolved site-selective imaging of predissociation and charge transfer dynamics: the CH 3 I B-band
in Journal of Physics B: Atomic, Molecular and Optical Physics
Description | This is a 5 year programme grant award; a detailed (~20 page) end of year 2 progress report was sent to external advisory board members and EPSRC at the start of 2016. In summary: PImMS1 cameras are now installed in the labs of 4 of the lead investigators. After a few teething issues, two of these have been upgraded to the PImMS2 sensor and are running well. We were able to recruit excellent PDRAs to the PG. One - resigned in 9/2015 to take a permanent scientist position at the Norwegian Institute for Energy Technology. Another has secured an Assistant Professorship at Fort Lewis College, Colorado, starting in summer 2016. Two others left in 2016 to start Teaching Fellow positions at the Universities of St Andrew and Warwick, respectively. The search for their successors attracted a very strong pool of applicants; and two new PDRAs joined the PG in early 2016. Another 2-year PDRA position is currently being advertised. Much high quality science has been performed - addressing technique development, unimolecular gas phase molecular photophysics, bimolecular collisions and gas phase reactivity, new developments in mass spectrometry and imaging material on surfaces. Since the start of 2014, the team have published >50 peer reviewed articles on topics within the remit of the PG, in most of the leading journals for work in this area (J. Chem. Phys., J. Phys. Chem. A, J. Phys. Chem. Letts., Chem. Sci., Phys. Chem. Chem. Phys., Phys. Rev. Lett., Phys. Rev. A, Rev. Sci. Instrum., etc. Roughly one third of these publications are authored by more than one of the lead investigators; a similar fraction reports collaborative work with groups outside of the PG. The lead investigators have given >50 invited conference lectures and a further 30 research seminars on work within the PG remit during the period 2014-16. Each has further invitations lined up for 2017. The PDRAs and associated PhD students have also been excellent drivers of, and ambassadors for, the PG activities. Expenditure on staff, equipment and consumables is running largely as planned, though the purchase of some equipment items has been delayed. The original proposal identified a number of milestones within the 4 scientific work packages (SWPs) and 5 technical work packages (TWPs). Some have already been achieved in full, some (as expected) remain work in progress, implementation of a few have been delayed, while other ambitions have emerged (or been moved forward) as a result of new opportunities enabled by the flexibility of the PG. Noteworthy examples in the latter category include the PImMS-driven collaborations with scientists at Aarhus and at DESY (Hamburg), the demonstration of using PImMS sensors in neutron imaging, and computational chemistry collaborations with groups in Munich and in Hokkaido. The possibility of ambient pressure SMI-MS is now being explored with two companies. The complementarity of many of the PG activities with the ERC funded condensed phase photophysics research programme in Bristol is proving every bit as rewarding as anticipated at the time of the PG submission. Each lead investigator has sought to make significant contributions in one or more advocacy, leadership and/or outreach areas during the first two years of the PG. The mid-term review of the PG (Nov 2016) returned the very positive outcome: 5; this is a strong grant that broadly meets all assessment criteria. Following the review, the PG Team produced a set of additional milestones for years 4 and 5, focusing on the development and application of Coulomb-explosion covariance-map imaging methods to explore molecular structure and (photoinduced) dynamics in the gas phase. The team met with the (expanded) External Advisory Board in 9/2017, for which meeting an updated progress report was prepared and circulated. Key advances reported at that time included the successful installation of fsec lasers for Coulomb-explosion imaging studies at both Oxford and Bristol, and many further publications and invited conference presentations describing recent progress in all of the scientific work packages outlined in the original application. By end of grant (Sept 2019), Coulomb explosion imaging experiments had been established in both Bristol and Oxford, ex PDRA Dr Michael Burt had secured an EPSRC Fellowship to drive future activity in this area in Oxford, many further publications reporting pioneering activities in all areas of the original application (and more) are continuing to appear and all lead investigators continue to be in demand as invited speakers at international conferences in the general area of chemical reaction dynamics. |
Exploitation Route | Work is ongoing. |
Sectors | Aerospace Defence and Marine Creative Economy Education Environment Healthcare Manufacturing including Industrial Biotechology |
URL | http://dynamics.chem.ox.ac.uk/ |
Description | Impacts in industry: Bristol-based velocity map imaging research supported by this EPSRC Programme Grant (PG) and a previous award (EP/G00224X), various EU network grants and a KTP award with Photek Ltd (KTP008481) led to an ion optics design - detailed in Marchetti et al, J Chem Phys 142, 224303 (2015) - that was key to the launch of Velocitas VMI as a new activity within Photek. The Velocity Map Imaging (VMI) Spectrometers | Velocitas VMI | Photek (velocitas-vmi.com) website describes the ongoing reach and significance of this extension to Photek's traditional activities. Building directly on PG-enabled work - see e.g. Guo et al, J Am Soc Mass Spec 31, 1903 (2020) - the Oxford team have a Rosalind Franklin Institute (RFI)-funded project with Ionoptika Ltd (Home - Ionoptika Ltd) to develop a secondary ion mass spectrometry (SIMS) microscope mode imaging instrument. This work sits within the Biological mass spectrometry theme of the RFI (https://www.rfi.ac.uk/projects/microscope-mode-msi/). Impacts on wider science: 1. Sunscreens and 'molecular heaters to boost plant growth. The organic components in commercial sunscreens must absorb UV light efficiently and be 'photostable' (i.e. following photoexcitation, the sunscreen molecules must decay back to their ground state, releasing the photon energy in the form of localised heating, and be ready to repeat the excitation-decay cycle over and over again, with high efficiency and fidelity). PG enabled research by Karsili et al. (J Phys Chem A 118, 11999 (2014)) established the underlying photophysics in the case of oxybenzone (and other sunscreen molecules), which inspired collaboration with the Stavros group (University of Warwick) and joint experimental studies (e.g. Baker et al, J Phys Chem Letts 6, 1383 (2015)) that not only validated the theoretical picture but led to the realisation that molecules displaying similar photophysics might find use as molecular heaters for plants, thereby enhancing crop growth under cold and freezing stress. This led to a patent filing and an EU H2020 FET-Open award 'Boostcrop' (boostcrop.eu) led by Warwick, involving other photophysicists (Bristol, Amsterdam), 'green' synthetic chemists (AgroParisTech), theoretical chemists (Marseille), plant biologists and breeders, in academia (Bristol, Amsterdam) and in industry (GAB Consulting), and experts in food safety, toxicology, etc (German Federal Institute for Risk Assessment (BfR)). This project is ongoing and showing much promise (see e.g. Abiola et al, Chem Sci 12, 15239 (2021)), though plant trials have been slowed by the covid pandemic. 2. Stimulating activity at international facilities Research collaborations and programmes at international facilities/free electron lasers (e.g. FLASH (Hamburg), EU XFEL (Hamburg), SLAC (USA), SACLA (Japan), DCLS (China), Brookhaven (USA), Artemis (UK)) have been enabled and enhanced by access to contemporary time and position sensitive detectors like the PImMS camera that underpinned this PG - see e.g. Allum et al, J Chem Phys 149, 204313 (2018). PG science has also had a significant impact on driving aspects of the scientific agenda within the communities exploiting such facilities. Examples include (i) studies of photoinduced ring opening reactions using time resolved photoelectron spectroscopy at FERMI, Trieste (Pathak et al, Nature Chem 12, 795 (2020)) and time resolved ultrafast diffraction methods (at SLAC), inspired by earlier PG studies on thiophenone (Murdock et al, Phys Chem Chem Phys 16 21271 (2014)) and halothiophenes (Marchetti et al, J Chem Phys 142, 224303 (2015)) and (ii) efforts to develop covariance methods beyond 3-fold covariance and to compare the outputs with coincidence methods (Allum et al, J Phys Chem Lett 12, 8302 (2021)). 3. Impacts on higher education and training: As well as training high quality PhD students to think and function as professional scientists, the PG also supported the career progression of many early career researchers. ECRs associated with this PG who have now progressed to independent academic careers within and beyond the UK include Simon-John King, UEA; Rebecca Ingle, UCL; Michael Grubb, Fort Collins, Colorado; Tolga Karsili, Univ of Louisiana at Lafayette and Chris Hansen, Univ of New South Wales. Longer term impact: This point has been made many times before (by me, and by many others), but impacts from physical chemistry/chemical physics activities often take much longer than 2-3 years to acquire real significance. This PG succeeded an earlier award (EP/G00224X). The investigators associated with that earlier award included Manby (Bristol), Clary (Oxford) and Western (Bristol). Research undertaken by these individuals in the previous award has since contributed to, respectively: the foundation of ENTOS in 2019, with headquarters in San Diego and Manby as Chief Technical Officer (Entos | Breakthrough AI-driven chemistry for medicine); one of the Oxford Chemistry impact case studies submitted to REF2021 (a classified case study addressing the destruction of chemical nerve agents); and PGOPHER, the most versatile, powerful, and user-friendly software package available anywhere for molecular spectroscopy simulation and analysis (Western, J Quant Spectrosc Rad Trans 186 221 (2017)). More than 100 publications, spanning fields like combustion, plasmas, planetary atmospheres and interstellar space and with authors drawn from all continents of the world, cited PGOPHER in 2021. One output from the recently concluded PG used PGOPHER to demonstrate how OH emission measurements could offer a route to identifying high oxygen exoplanetary atmospheres (Chang et al, J Phys Chem Letts 11 (2020) 9086 (2020)). Again, potentially very impactful, but since such observations require a dedicated spacecraft platform, not the sort of science that can be expected to generate immediate impact! |
First Year Of Impact | 2017 |
Sector | Aerospace, Defence and Marine,Agriculture, Food and Drink,Chemicals,Digital/Communication/Information Technologies (including Software),Education,Energy,Environment,Security and Diplomacy,Other |
Impact Types | Societal Economic |
Description | Advised on the RSC's policy on the Plan S open access policy in my capacity as a member of the RSC's Member Communities Board. |
Geographic Reach | National |
Policy Influence Type | Participation in a guidance/advisory committee |
URL | http://www.rsc.org/globalassets/04-campaigning-outreach/policy/research-policy/royal-society-of-chem... |
Description | Chair of Chemistry sub-panel in REF2021 |
Geographic Reach | National |
Policy Influence Type | Contribution to a national consultation/review |
Description | Chair of RSC Faraday Division Council |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
URL | http://www.rsc.org/Membership/Networking/InterestGroups/FaradayDivision/Council.asp |
Description | Member of Council of Royal Societyl |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
Description | Member of RSC Faraday Division Council |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
URL | http://www.rsc.org/Membership/Networking/InterestGroups/FaradayDivision/Council.asp |
Description | Member of the STFC Physical Sciences and Engineering Adivisor Panel |
Geographic Reach | National |
Policy Influence Type | Participation in a guidance/advisory committee |
Description | On behalf of RSC |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
Impact | RSC is the learned society for Chemists with a worldwide membership >50000. |
URL | http://www.rsc.org/about-us/our-structure/#council |
Description | RSC Heads of Chemistry Standing Committee |
Geographic Reach | National |
Policy Influence Type | Participation in a guidance/advisory committee |
Impact | Through the RSC HCUK, influenced RSC policy in areas of education, research, and the economy. |
Description | RSC Member Communities Board |
Geographic Reach | Multiple continents/international |
Policy Influence Type | Membership of a guideline committee |
Impact | Development of RSC's response to Plan S proposals on open-access publishing. Development of RSC's advice on freedom of movement for individuals in the context of Brexit. |
Description | chair of SP8 for REF2021 |
Geographic Reach | National |
Policy Influence Type | Contribution to a national consultation/review |
Description | membership of Council of Royal Society |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
Impact | Royal Society is premier learned society in UK. Council members advise on RS activities and are the trustees of this charity. |
Description | EPSRC DTP - CASE conversion incentivisation scheme |
Amount | ÂŁ73,000 (GBP) |
Funding ID | EP/N509711/1 |
Organisation | University of Oxford |
Sector | Academic/University |
Country | United Kingdom |
Start | 08/2017 |
End | 09/2021 |
Description | EPSRC DTP - CASE conversion incentivisation scheme |
Amount | ÂŁ73,000 (GBP) |
Funding ID | D4T00130 |
Organisation | University of Oxford |
Sector | Academic/University |
Country | United Kingdom |
Start | 08/2018 |
End | 09/2022 |
Description | EPSRC Impact Acceleration Account Award |
Amount | ÂŁ95,512 (GBP) |
Funding ID | EP/R511742/1 |
Organisation | University of Oxford |
Sector | Academic/University |
Country | United Kingdom |
Start | 08/2018 |
End | 03/2020 |
Description | EU FET-OPEN |
Amount | € 4,900,000 (EUR) |
Funding ID | 828753 |
Organisation | EU-T0 |
Sector | Public |
Country | European Union (EU) |
Start | 01/2019 |
End | 12/2022 |
Description | New Directions in Molecular Scattering: Multiple Pathways and Products |
Amount | ÂŁ5,880,172 (GBP) |
Funding ID | EP/T021675/1 |
Organisation | Engineering and Physical Sciences Research Council (EPSRC) |
Sector | Public |
Country | United Kingdom |
Start | 05/2020 |
End | 05/2026 |
Description | Oxford Berlin Research Partnership |
Amount | € 18,000 (EUR) |
Organisation | University of Oxford |
Department | Oxford–Berlin Research Partnership |
Sector | Academic/University |
Country | United Kingdom |
Start | 01/2019 |
End | 12/2020 |
Description | Ultrafast Photochemical Dynamics in Complex Environments |
Amount | ÂŁ8,055,185 (GBP) |
Funding ID | EP/V026690/1 |
Organisation | Engineering and Physical Sciences Research Council (EPSRC) |
Sector | Public |
Country | United Kingdom |
Start | 08/2021 |
End | 08/2027 |
Title | Improvements to covariance analysis methods and simulation techniques used in Coulomb explosion ion imaging |
Description | In collaboration with groups in Stanford, Stony Brook, and elsewhere, we have developed covariance methods to analyse velocity map ion imaging data, in particular those arising from the Coulomb explosion of isolated molecules in the gas phase. This includes work developing 2-, 3- and higher-fold covariance methods, and also simulation methods to interpret such correlated ion images. |
Type Of Material | Improvements to research infrastructure |
Year Produced | 2014 |
Provided To Others? | Yes |
Impact | The impact has been mainly in the form of publications, demonstrating these new developments and applying the methods to femtosecond time-resolved studies of a wide variety of photochemical processes. |
Title | CEI perspective for PCCP |
Description | Ultrafast electron diffraction data |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
Impact | New method to determine structural changes in photoexcited molecules and how they lead to different products of a photochemical reaction. |
URL | https://data.bris.ac.uk/data/dataset/1c14gl3i484312c6h6lr4nttz9 |
Title | Data for Norrish calculations |
Description | Results from calculations of singlet only contributions to Norrish type I and II reactions. |
Type Of Material | Database/Collection of data |
Year Produced | 2019 |
Provided To Others? | Yes |
Title | Effects of Ring Fluorination on the Ultraviolet Photodissociation Dynamics of Phenol |
Description | Results from Bristol HRA-PTS experiments on photodissociation dynamics of fluorophenols |
Type Of Material | Database/Collection of data |
Year Produced | 2020 |
Provided To Others? | Yes |
URL | https://data.bris.ac.uk/data/dataset/28frhrmwllnx42l7irrypuhng3/ |
Title | Experimental and computational data supporting the findings published in the article 'Side-impact collisions of Ar with NO' |
Description | Stereodynamical data concerning collision or oriented NO molecules with Ar. The data set includes both experimental and theoretical results associated with the Nature Chemistry publication. |
Type Of Material | Database/Collection of data |
Year Produced | 2019 |
Provided To Others? | Yes |
Impact | The data presented and the methods developed enabled subsequent work to study the oriented collisions of more complex systems, which is the topic of the EPSRC programme grant 'New directions in molecular scattering: Multiple Pathways and Products'. |
URL | http://ora.ox.ac.uk/objects/uuid:6767458b-ef8d-453e-949e-4ce9df0f343c |
Title | Inelastic scattering of NO with methane |
Description | Velocity map imaging data for the inelastic scattering of NO with methane, using a crossed molecular beam apparatus. |
Type Of Material | Database/Collection of data |
Year Produced | 2019 |
Provided To Others? | Yes |
Title | Monitoring the evolution of relative product populations at early times during a photochemical reaction |
Description | Identifying multiple rival reaction products and transient species formed during ultrafast photochemical reactions and determining their time-evolving relative populations are key steps towards understanding and predicting photochemical outcomes. Yet, most contemporary ultrafast studies struggle with clearly identifying and quantifying competing molecular structures/species amongst the emerging reaction products. Here, we show that mega-electronvolt ultrafast electron diffraction in combination with ab initio molecular dynamics calculations offers a unique route to determine time-resolved populations of the various isomeric products formed after UV (266 nm) excitation of the five-membered heterocyclic molecule thiophenone. This strategy reveals an unexpectedly high (~50%) yield of an episulfide isomer containing a strained 3-membered ring within ~1 ps at early times and rapid interconversions between the rival photoproducts. |
Type Of Material | Database/Collection of data |
Year Produced | 2023 |
Provided To Others? | Yes |
Impact | New method to study structural changes leading to different products in photochemical reactions. |
URL | http://datadryad.org/stash/dataset/doi:10.5061/dryad.nzs7h44wm |
Title | Photodissociation of Methimazole |
Description | Results from photodissociation studies on methimazole for the paper "Photofragment Translational Spectroscopy Studies of H Atom Loss Following Ultraviolet Photoexcitation of Methimazole in the Gas Phase" |
Type Of Material | Database/Collection of data |
Year Produced | 2018 |
Provided To Others? | Yes |
Title | Photoinduced C-H bond fission |
Description | Perspective on photoinduced C-H bond fission in prototypical organic molecules and radicals |
Type Of Material | Database/Collection of data |
Year Produced | 2018 |
Provided To Others? | Yes |
Title | Quantifying Rival Bond Fission Probabilities following photoexcitation: C-S bond fission in t-butylmethylsulfide |
Description | Experimental data sets for the uv photodissociation of t-butylmethylsulfide measured by single photon ionisation coupled to multi-mass VMI. Theoretical calculations of cuts along relevant coordinates of potential energy surfaces and single point vibrational calculations of asymptotic products and parent molecules. |
Type Of Material | Database/Collection of data |
Year Produced | 2019 |
Provided To Others? | Yes |
Description | Academic collaborations |
Organisation | Aarhus University |
Country | Denmark |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Complutense University of Madrid |
Country | Spain |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Dalian Institute of Chemical Physics |
Country | China |
Sector | Private |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Deutsches Electronen-Synchrotron (DESY) |
Country | Germany |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Hokkaido University |
Country | Japan |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Johns Hopkins University |
Country | United States |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Kansas State University |
Country | United States |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Max Planck Society |
Department | Fritz Haber Institute |
Country | Germany |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Moscow State University |
Country | Russian Federation |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | National Research Council - Ottawa |
Country | Canada |
Sector | Public |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Radboud University Nijmegen |
Country | Netherlands |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | Sandia Laboratories |
Country | United States |
Sector | Private |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Gothenburg |
Country | Sweden |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Innsbruck |
Country | Austria |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Kyoto |
Country | Japan |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Louisiana at Lafayette |
Country | United States |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Maryland, College Park |
Country | United States |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Santiago de Compostela |
Country | Spain |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Academic collaborations |
Organisation | University of Warwick |
Department | University of Warwick Research Students Skills Programme |
Country | United Kingdom |
Sector | Academic/University |
PI Contribution | Numerous scientific collaborations, most of which have already yielded joint publications. |
Collaborator Contribution | Intellectual input, combining and sharing of knowledge and/or of scientific capability. |
Impact | See list of outputs |
Start Year | 2014 |
Description | Exploring non-adiabatic coupling in excited state molecules using ultrafast pump-probe laser techniques |
Organisation | University of Kyoto |
Country | Japan |
Sector | Academic/University |
PI Contribution | PhD student Rebecca Ingle contributed to on-going research in the Suzuki group and acquired new skills and expertise as a result |
Collaborator Contribution | Prof Suzuki hosted student Rebecca Ingle in his well-equipped laboratory. |
Impact | One scientific publication, T. Horio, R. Spesyvtsev, K. Nagashima, R. A. Ingle, Y. Suzuki and T. Suzuki, J. Chem. Phys., 2016, 145, 044306. |
Start Year | 2014 |
Description | Microscope mode imaging mass spectrometry |
Organisation | Rosalind Franklin Institute |
Country | United Kingdom |
Sector | Charity/Non Profit |
PI Contribution | Development of a microscope imaging mass spectrometer using secondary ion mass spectrometry (SIMS), using C60 and water cluster ion guns. This is a collaborative project involving the Rosalind Franklin Institute (RFI) and the company Ionoptika Ltd |
Collaborator Contribution | The RFI are providing the Phase 1 funding through PDRA support and equipment costs. Ionoptika are providing the C60 ion gun system and water cluster ion gun development, and we are providing the secondary ion time of flight detection capabilities. |
Impact | None as yet |
Start Year | 2019 |
Description | Oxford-Berlin partnership (with TU, Berlin and FHI, Berlin) "nitrogen oxide reduction at metal centres" |
Organisation | Max Planck Society |
Department | Fritz Haber Institute |
Country | Germany |
Sector | Academic/University |
PI Contribution | Expertise, intellectual input, access to unique facilities and instrumentation in a projcet designed to better understand nitrogen oxide reduction at metal centres |
Collaborator Contribution | Expertise, intellectual input, access to unique facilities and instrumentation |
Impact | SRM visited Berlin in Febuary 2019 for kick-off meeting and seminar |
Start Year | 2019 |
Description | Oxford-Berlin partnership (with TU, Berlin and FHI, Berlin) "nitrogen oxide reduction at metal centres" |
Organisation | Technical University Berlin |
Country | Germany |
Sector | Academic/University |
PI Contribution | Expertise, intellectual input, access to unique facilities and instrumentation in a projcet designed to better understand nitrogen oxide reduction at metal centres |
Collaborator Contribution | Expertise, intellectual input, access to unique facilities and instrumentation |
Impact | SRM visited Berlin in Febuary 2019 for kick-off meeting and seminar |
Start Year | 2019 |
Description | Use of X-ray free electron lasers in the USA, Germany, Switzerland and Japan |
Organisation | Kansas State University |
Country | United States |
Sector | Academic/University |
PI Contribution | Andrew Orr-Ewing, Mark Brouard, Claire Vallance, Basile Curchod emeritus Professor Mike Ashfold are partners in an international collaboration with scientists from Stanford University / SLAC, Kansas State University, Brown University, University of Nebraska and elsewhere to study photochemical dynamics using ultrafast X-ray scattering, ultrafast electron diffraction, time-resolved photoelectron spectroscopy and related techniques. We have contributed many of the scientific ideas to successful beamtime proposals, and have carried out experiments in our Bristol and Oxford laboratories to provide proof-of-principle data to underpin successful proposals, thereby securing beam time at these international facilities. |
Collaborator Contribution | Writing proposals for beamtime, participation in beam time at international facilities, data analysis, preparation of publications. |
Impact | Awarded beamtimes include: SwissFEL 20230065, December 2023: Probing Norrish Type-I Reactions of Cyclic Ketones via Femtosecond X-Ray Absorption and X-Ray Photoelectron Spectroscopy, 12 shifts on ATHOS-Maloja beamline. PI Dr D. Rolles, Kansas State University. LCLS L-10227 CXI (time-resolved hard X-ray scattering) experiment, November 2023: Structural Imaging of Competing Ultrafast Reaction Pathways in the Photoinduced Wolff Rearrangement. PI Felix Allum (SLAC). LCLS L-10060 CXI (time-resolved hard X-ray scattering) experiment, October 2023: Structural Insight into Norrish Type-I Reactions of Cyclic Ketones. PI Alice Green (SLAC, Stanford University). LCLS MeV Ultrafast Electron Diffraction U108: Photodissociation and ring-opening dynamics in 2- and 3-iodothiophene. PI Ruaridh Forbes (SLAC, Stanford University). Beamtime Nov 14 - 19 2023. LCLS Run 20 award of ultrafast X-ray scattering beamtime: LX93 - Competing reaction pathways: ring-opening versus bond cleavage in cyclic molecular systems (June 2022). PI: Dr R.J.G. Forbes (SLAC, Stanford University). EuXFEL, project 5680, Imaging the Ultrafast Photochemistry of a Prototypical Carbonyl. PI. Dr Alice Green (SLAC, Stanford University). 4 days of beamtime in May 2024. FLASH2, Time-resolved C K-edge XPS of the Wolff Rearrangement in Ethyl Diazoacetate (EDA) and Ethyl Diazoacetoacetate (EDAA). PI Dr Felix Allum (SLAC, Stanford University). May 2024. |
Start Year | 2021 |
Description | Use of X-ray free electron lasers in the USA, Germany, Switzerland and Japan |
Organisation | Stanford University |
Country | United States |
Sector | Academic/University |
PI Contribution | Andrew Orr-Ewing, Mark Brouard, Claire Vallance, Basile Curchod emeritus Professor Mike Ashfold are partners in an international collaboration with scientists from Stanford University / SLAC, Kansas State University, Brown University, University of Nebraska and elsewhere to study photochemical dynamics using ultrafast X-ray scattering, ultrafast electron diffraction, time-resolved photoelectron spectroscopy and related techniques. We have contributed many of the scientific ideas to successful beamtime proposals, and have carried out experiments in our Bristol and Oxford laboratories to provide proof-of-principle data to underpin successful proposals, thereby securing beam time at these international facilities. |
Collaborator Contribution | Writing proposals for beamtime, participation in beam time at international facilities, data analysis, preparation of publications. |
Impact | Awarded beamtimes include: SwissFEL 20230065, December 2023: Probing Norrish Type-I Reactions of Cyclic Ketones via Femtosecond X-Ray Absorption and X-Ray Photoelectron Spectroscopy, 12 shifts on ATHOS-Maloja beamline. PI Dr D. Rolles, Kansas State University. LCLS L-10227 CXI (time-resolved hard X-ray scattering) experiment, November 2023: Structural Imaging of Competing Ultrafast Reaction Pathways in the Photoinduced Wolff Rearrangement. PI Felix Allum (SLAC). LCLS L-10060 CXI (time-resolved hard X-ray scattering) experiment, October 2023: Structural Insight into Norrish Type-I Reactions of Cyclic Ketones. PI Alice Green (SLAC, Stanford University). LCLS MeV Ultrafast Electron Diffraction U108: Photodissociation and ring-opening dynamics in 2- and 3-iodothiophene. PI Ruaridh Forbes (SLAC, Stanford University). Beamtime Nov 14 - 19 2023. LCLS Run 20 award of ultrafast X-ray scattering beamtime: LX93 - Competing reaction pathways: ring-opening versus bond cleavage in cyclic molecular systems (June 2022). PI: Dr R.J.G. Forbes (SLAC, Stanford University). EuXFEL, project 5680, Imaging the Ultrafast Photochemistry of a Prototypical Carbonyl. PI. Dr Alice Green (SLAC, Stanford University). 4 days of beamtime in May 2024. FLASH2, Time-resolved C K-edge XPS of the Wolff Rearrangement in Ethyl Diazoacetate (EDA) and Ethyl Diazoacetoacetate (EDAA). PI Dr Felix Allum (SLAC, Stanford University). May 2024. |
Start Year | 2021 |
Title | Molecular Heaters |
Description | The invention relates to the use of molecular photon to heat convertors (also known as "molecular heaters") to warm plants, parts of plants or seeds of plants, to methods of using such molecular heaters to warm plants, to plants producing such molecular heaters and to compositions containing such molecular heaters. |
IP Reference | GB1715528.4 |
Protection | Patent application published |
Year Protection Granted | 2017 |
Licensed | No |
Impact | N/A |
Description | Career and research talk to the Oxford Women in Chemistry society. |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | Local |
Primary Audience | Postgraduate students |
Results and Impact | Talk on my career and research areas I've worked in for the Oxford Women in Chemistry society. |
Year(s) Of Engagement Activity | 2021 |
Description | Departmental seminar |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Professional Practitioners |
Results and Impact | Online departmental seminar for physical chemists at the University of Cambridge. |
Year(s) Of Engagement Activity | 2021 |
Description | Departmental seminar |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Online research talk on my work to the Department of Chemistry at Wayne State University in the USA. |
Year(s) Of Engagement Activity | 2020 |
Description | Oxford Impact short film |
Form Of Engagement Activity | A broadcast e.g. TV/radio/film/podcast (other than news/press) |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Public/other audiences |
Results and Impact | See url below |
Year(s) Of Engagement Activity | 2016 |
URL | https://www.youtube.com/watch?v=z6e21GXwnBY&feature=youtu.be |
Description | SUSDG meetings |
Form Of Engagement Activity | Participation in an activity, workshop or similar |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Postgraduate students |
Results and Impact | Launch of ESR-led Southern Universities Spectroscopy and Dynamics Group series of 2-day meetings (Bristol, Oxford, Nottingham, ) |
Year(s) Of Engagement Activity | 2014 |
URL | http://vallance.chem.ox.ac.uk/SUSDG2015/SUSDG%202015%20Talk%20Titles.pdf |