Dynamical Chemical Processes

Lead Research Organisation: Heriot-Watt University
Department Name: Sch of Engineering and Physical Science

Abstract

The field of chemical dynamics is concerned with the detailed atomic-level events that lie at the heart of all chemical and photochemical processes. We are studying these phenomena through a combination of sophisticated experiments, based on laser and vacuum technology, and advanced theoretical methods. The understanding that we provide is crucial to the enhanced exploitation or modelling of a wide range of natural or man-made phenomena, from chemistry in the atmosphere, combustion, catalysis, natural photoprotection and the design of sunscreens, through to photodynamic therapy.
The purpose of this Platform is to provide stability and greater flexibility in the use of postdoctoral-level personnel across a group of five academic investigators with an established record of working together in areas spanning the interaction of molecules with liquid surfaces; chemical reactions and the transfer of energy in the gas-phase; and the chemical and physical processes initiated in molecules by the absorption of light.
The Platform will allow us to retain key staff, and to deploy them in ways that are not possible with standard proposals. In particular, we will be able to accelerate our ability to grasp immediate opportunities based on our existing collaborations, both among the group and with external partners, by carrying out critical proof-of-concept studies. We will tackle larger, more complex, multi-stranded projects that will require us to work together in new combinations. We can see the potential for exciting developments in a number of areas, but currently we don't have funds to carry out the groundwork necessary to underpin successful joint proposals. In particular, we aim to expand the areas in which we have close integration between experiment and theory. We will also have the scope to carry out high-risk but adventurous pilot studies to expand into new areas beyond the boundaries of existing work, with potential new collaborators.
The PDRAs employed will benefit greatly from the enhanced career development under the Platform. We will broaden their experience through research exchanges; engage them in proposals to win new funding; support them in applications for personal fellowships with dedicated funds for their own short proof-of-concept projects; and involve them in management of the Platform.

Planned Impact

Much of the work that will be enabled by the Platform is fundamentally motivated. The potential for societal and economic benefits is also substantial. The impacts are of three main types: the output of skilled personnel; more direct economic benefits of the results of the research that we expect to be realised primarily in the longer term; and improved public awareness.
Absolutely central to the philosophy of the Platform Grant scheme is the output of highly trained personnel, skilled in the use of modern laser, vacuum, electronic-data capture and data processing technologies, or in forefront computational chemical methods. They will also have well-developed generic and transferable communication, presentation and problem-solving skills. In some cases they will be exposed to financial management on the Operational Management Group. An integral part of our programme is to engage in research exchanges of personnel, in both directions, with existing and proposed new collaborators. Involvement in these interactions, and in the wider group under the Platform, will enhance the skills and experience of the PDRAs. They will be ideally suited to contribute to the growth or creation of high-technology companies, enhancing innovative capacity and consequently increasing business revenues.
The potential direct economic impacts of the results of the research span a wide range of applications. Our gas-liquid work has major implications for gas uptake and sequestration and multiphase catalysis, particularly based on ionic liquids; heterogeneous chemistry on atmospheric aerosol particles; combustion of liquid fuels; through to biological respiration. Our gas-phase collision studies also impact on atmospheric chemistry, combustion, technological plasmas and astrochemistry. We will provide quantitative constraints on, and in some cases new mechanisms that need to be included in, numerical models of these complex collisional environments. The improvements in spectroscopic detection that we will develop, and the greater understanding of the effects of collisional quenching that we will provide, will broaden the range and increase the quantitative accuracy of methods of detection of trace-species concentrations. These will be adopted by applied scientists and engineers investigating either the atmosphere itself or combustion systems that are the potential sources of pollutants. The ultimate societal benefit will result from consequent regulatory changes. Our studies of electronic excitation, photophysics and photochemistry will inform scientists and engineers working in more applied areas including the rapidly emerging fields of biophysics, molecular switches and photochromic polymers, photoprotective compounds such as sunscreens, and photodynamic therapy. Ultimately, uptake of this research has the potential to yield health benefits in medical therapies and disease prevention. Although not the primary aim of this proposal, a secondary benefit may be the development of new technical methods or techniques that generate commercial interest. Any such intellectual property will be protected and exploited in consultation with HWU Research & Enterprise Services.
We will also continue to enhance public awareness of science. We will involve the PDRAs in the dissemination of the aims and results of this work to the wider public, at a suitable level, extending our group's on-going contributions to Open Days, careers events, a resident Chemistry Teachers Week, and external events such as Science and the Parliament and the Edinburgh Science Festival.

Publications

10 25 50
 
Description A significant number of proof-of-concept studies have been carried out by PDRA staff employed on the grant, supporting independent bids for funding, including personal fellowships for the PDRAs. Substantial onward funding has been secured as a direct result of some of this proof-of-concept work. A substantial volume of papers have been published in high-profile international journals.
Exploitation Route The award is still in progress - there will be further on-going findings.

The results obtained so far have been instrumental in a successful application for follow-on funding in the form of a major EPSRC Programme Grant (EP/T00732X/1) between the majority of the Co-Inverstigators on this grant and three new Co-Investigators at University of Oxford, and further additional EPSRC responsive-mode funding (EP/T03114X/1) between two of the investigators and collaborators at University of York plus international partners in Germany and USA.
Sectors Chemicals,Energy,Environment,Healthcare

URL http://dynamics.eps.hw.ac.uk/index.php
 
Description Out put of highly trained personnel who have gone on to future employment on other research projects (3), high technology industry (2) and education (secondary level) (1).
First Year Of Impact 2018
Sector Aerospace, Defence and Marine,Digital/Communication/Information Technologies (including Software),Education
Impact Types Economic

 
Description A Joined-up Approach for New Molecular Simulation Technologies To Harness Ultrafast Photochemistry
Amount £524,400 (GBP)
Funding ID EP/V006746/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 02/2021 
End 07/2024
 
Description Carnegie Collaborative Research Grant
Amount £60,000 (GBP)
Funding ID Photochemistry to the next level: combining state-of-the-art ab-initio and quantum dynamics 
Organisation Carnegie Trust 
Sector Charity/Non Profit
Country United Kingdom
Start 04/2018 
End 03/2019
 
Description Chemical Structure and Dynamics at the Gas-Liquid Interface
Amount £12,718 (GBP)
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 06/2020 
End 05/2021
 
Description Cirrus funding; MD of hydrocarbon liquid surfaces
Amount £6,389 (GBP)
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 02/2019 
End 02/2020
 
Description DTP studentship
Amount £65,000 (GBP)
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 10/2017 
End 09/2020
 
Description EPSRC Grant
Amount £588,864 (GBP)
Funding ID EP/R030448/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 04/2018 
End 10/2021
 
Description Ionic-Liquid Mixtures: from Surface Structure to Catalytic Performance
Amount £680,203 (GBP)
Funding ID EP/T03114X/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 08/2020 
End 08/2024
 
Description James Watt Scholarship for Adam Knight
Amount £65,000 (GBP)
Organisation Heriot-Watt University 
Sector Academic/University
Country United Kingdom
Start 09/2020 
End 09/2023
 
Description James Watt Scholarship for Malcolm Garrow
Amount £65,000 (GBP)
Organisation Heriot-Watt University 
Sector Academic/University
Country United Kingdom
Start 09/2020 
End 08/2023
 
Description James-Watt Studentship
Amount £75,000 (GBP)
Organisation Heriot-Watt University 
Sector Academic/University
Country United Kingdom
Start 10/2022 
End 03/2026
 
Description James-Watt Studentship (Clément Soulie)
Amount £65,000 (GBP)
Organisation Heriot-Watt University 
Sector Academic/University
Country United Kingdom
Start 10/2018 
End 09/2021
 
Description New Directions in Molecular Scattering
Amount £5,880,172 (GBP)
Funding ID EP/T021675/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 06/2020 
End 05/2025
 
Description Unified Quantum Dynamics of Nuclei and Electrons
Amount £348,859 (GBP)
Funding ID RPG-2020-208 
Organisation The Leverhulme Trust 
Sector Charity/Non Profit
Country United Kingdom
Start 02/2021 
End 01/2024
 
Title AIR Network 
Description Many charged particle imaging measurements rely on the inverse Abel transform (or related methods) to reconstruct three-dimensional (3D) photoproduct distributions from a single two-dimensional (2D) projection image. This technique allows for both energy- and angle-resolved information to be recorded in a relatively inexpensive experimental setup, and its use is now widespread within the field of photochemical dynamics. There are restrictions, however, as cylindrical symmetry constraints on the overall form of the distribution mean that it can only be used with a limited range of laser polarization geometries. The more general problem of reconstructing arbitrary 3D distributions from a single 2D projection remains open. Here, we demonstrate how artificial neural networks can be used as a replacement for the inverse Abel transform and-more importantly-how they can be used to directly "reinflate" 2D projections into their original 3D distributions, even in cases where no cylindrical symmetry is present. This is subject to the simulation of appropriate training data based on known analytical expressions describing the general functional form of the overall anisotropy. Our arbitrary image reinflation (AIR) neural network can be utilized for a range of different examples, potentially offering a simple and flexible alternative to more expensive and complicated 3D imaging techniques 
Type Of Material Data analysis technique 
Year Produced 2022 
Provided To Others? Yes  
Impact Only just published - still to be determined 
URL https://github.com/HWQuantum/AIR
 
Title Image de-noising using machine learning 
Description Artificial neural networks transform noisy charged particle images unsuitable for quantitative analysis into statistically reliable data in excellent agreement with benchmark references. The approach has significant potential use within the field of chemical dynamics, particularly for the extraction of subtle features originating from photofragment vector correlations or photoelectron circular dichroism. 
Type Of Material Data analysis technique 
Year Produced 2021 
Provided To Others? Yes  
Impact Still to be determined 
URL https://github.com/HWQuantum/Charged-Particle-Denoising
 
Description Experiment - Dave Chandler 
Organisation Sandia Laboratories
Department Combustion Research Facility
Country United States 
Sector Public 
PI Contribution The PDRA, Dr T. R. Sharples, employed on the project visited the laboratory of Dr David Chandler at Sandia National Lab, Livermore for a 4 week period in Jan/Feb 2014. The primary aim of the visit was to learn about the technique of velocity-map imaging and in particular its application in minature crossed-molecular beam systems. Dr Sharples contributed to on-going experiments in Dr Chandler's laboratory during the visit. Dr Chandler has subsequently visited Heriot-Watt for 1 week (Sept 2016) during which we performed the first proof of concept measurements for a 4-vector correlation in inelastic rotational energy transfer, this lead to a publication in Nature Chemistry.
Collaborator Contribution Dr David Chandler is a world-expert on the application of imaging techniques in molecular dynamics, having introduced the idea of ion-imaging itself in the 1980s. He is also an expert in crossed-molecular beam experiments, and designed the first miniature apparatus to include velocity-map imaging. Previous collaboration with him lead to the proof-of-concept publications that were instrumental in the funding of this project. In this particular collaboration, he has provided training for the PDRA in crossed-beam VMI techniques, and provided valuable technical insight into the design of the new apparatus at Heriot-Watt.
Impact Steill et al. Journal of Physical Chemistry A, 117, 8163 (2013) Sharples et al. Journal of Chemical Physics 143 204301(2015) Luxford et al. Journal of Chemical Physics 145 084312 (2016) Luxford et al. Journal of Chemical Physics 145 174304 (2016) Luxford et al. Journal of Chemical Physics 147 013912 (2017) Sharples et al. Nature Chemistry 10 1148 (2018)
Start Year 2013
 
Description Jérôme Loreau QM scattering calculations for NH3 + D2 
Organisation University Libre Bruxelles (Université Libre de Bruxelles ULB)
Department Department of Quantum and Photophysical Chemistry
Country Belgium 
Sector Academic/University 
PI Contribution We conducted an analysed crossed molecular beam scattering experiments to study the collisions between NH3 and D2. The analysis produced differential cross sections that could be compared to the theoretical calculations of Dr Loreau.
Collaborator Contribution Time independent quantum scattering calculations on the NH3 + D2 system to produce differential scattering cross sections for comparison with experiment.
Impact paper submitted to the Journal of Physical Chemistry - currently under review.
Start Year 2017
 
Description Minton (MSU) on NSF/EPSRC jointly funded project 
Organisation Montana State University
Country United States 
Sector Academic/University 
PI Contribution Linked funding was obtained from NSF and EPSRC for a joint project between Minton (MSU, Montana, USA) and Slattery and Bruce (York) with Costen and McKendrick (HWU).
Collaborator Contribution Complementary experiments and theory at MSU. Chemical synthesis and complementary neutron, X-ray and physical prperty measurements at York.
Impact Outputs are linked to the award.
Start Year 2013
 
Description Minton (MSU) on NSF/EPSRC jointly funded project 
Organisation University of York
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution Linked funding was obtained from NSF and EPSRC for a joint project between Minton (MSU, Montana, USA) and Slattery and Bruce (York) with Costen and McKendrick (HWU).
Collaborator Contribution Complementary experiments and theory at MSU. Chemical synthesis and complementary neutron, X-ray and physical prperty measurements at York.
Impact Outputs are linked to the award.
Start Year 2013
 
Description Stark deflection for molecular cluster separation 
Organisation University of Hamburg
Country Germany 
Sector Academic/University 
PI Contribution Secondment of Dr Thomas Sharples to the group of Prof Jochen Kupper at DESY/U. of Hamburg to develop the application of Stark deflection methods to the separation of weakly bound molecular clusters. Dr Sharples has proposed the experiments to Prof Kupper, and performed experiments at U. of Hamburg with Prof Kupper's research group. Dr Sharples has subsequently helped develop the theoretical modelling of the deflection.
Collaborator Contribution Prof Kupper provided the experimental apparatus and hosted Dr Sharples' visit. He has subsequently provided computing resources and manpower towards the interpretation of the experimental results.
Impact None to date.
Start Year 2018
 
Description Visit to ETH Zurich 
Organisation ETH Zurich
Country Switzerland 
Sector Academic/University 
PI Contribution PDRA (N. Kotsina) conducted a short visit to the group of Prof. H.-J. Worner to exchange ideas relating to high-harmonic generation, thin liquid jet set-ups, and the use of hollow-core capillaries for short-pulses UV/VUV generation with a view to developing future proposals and fellowship applications.
Collaborator Contribution Exchange of ideas relating to high-harmonic generation, thin liquid jet set-ups, and the use of hollow-core capillaries for short-pulses UV/VUV generation with a view to developing future proposals and fellowship applications.
Impact None as yet
Start Year 2021
 
Description van de Meerakker (Nijmegen) 
Organisation Radboud University Nijmegen
Department Institute for Molecules and Materials
Country Netherlands 
Sector Academic/University 
PI Contribution We have sent a PDRA (Dr T. Sharples) to Prof. Meekakker's laboratory to learn about (1) their work on electric discharge radical molecular beam sources and (2) hexapole state selection.
Collaborator Contribution Prof Meerakker hosted the visit of Dr T Sharples, and has provided information related to the design of (1) electric discharge radical molecular beam sources and (2) hexapole state selectors.
Impact None so far.
Start Year 2016
 
Description Bristol Talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact Invited research talk at University of Bristol (April 2017)
Year(s) Of Engagement Activity 2017
 
Description Chairman, International Symposium on Molecular Beams 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Organised the 28th edition of the recurrent conference series: International Symposium on Molecular Beams
Year(s) Of Engagement Activity 2019
URL http://ismbedinburgh2019.eps.hw.ac.uk/index.html
 
Description Invited Talk at APS Meeting 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Invited talk by Dave Townsend at APS meeting, held Chicago, IL, USA, March 2022 (Special Session: 25 years of Velocity Map Imaging)
Year(s) Of Engagement Activity 2021,2022
 
Description Invited Talk at ISMS Meeting 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact Invited talk by Dave Townsend at International Symposium on Molecular Spectroscopy, Urbana-Champaign, IL, USA, June 2022 (designated Journal of Molecular Spectroscopy Special Review Lecture).
Year(s) Of Engagement Activity 2022
 
Description Invited participation in WE-Heraeus-Seminar: Surface and Interface of Ionic Liquids, Bad Honnef, Germany 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Invited participation by Dr Simon Purcell in WE-Heraeus-Seminar: Surface and Interface of Ionic Liquids, 4th to 6th Dec, 2017, Bad Honnef, Germany. Poster presentation and flash 1 minute talk.
Year(s) Of Engagement Activity 2017
URL http://www.we-heraeus-stiftung.de/index.php?option=com_icagenda&view=list&layout=event&id=238&Itemid...
 
Description Leicester talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact Invited departmental seminar at University of Leicester, November 2019
Year(s) Of Engagement Activity 2019
 
Description New Horizons in Chemical Physics talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Invited talk by Dave Townsend at New Horizons in Chemical Physics meeting, held Oxford, April 2019
Year(s) Of Engagement Activity 2019
 
Description Open University Talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact Invited research talk at the Open University (October 2017)
Year(s) Of Engagement Activity 2017
 
Description Organising Faraday Discussion: New Directions in Molecular Scattering 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact I chaired the Scientific Committee which has made a succesful bid to RSC to organise a Faraday Discussion on the topic New Directions in Molecular Scattering. Invited speakers have been identified and accepted and the meeting is being marketed by RSC, to take place in May 2024.
Year(s) Of Engagement Activity 2022
 
Description Physical Chemistry Research seminar University of Edinburgh 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Postgraduate students
Results and Impact Research seminar - Studying collisions at liquid surfaces may be interesting, but is it useful?
Year(s) Of Engagement Activity 2017
 
Description Ultrafast Scotland Talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Postgraduate students
Results and Impact Invited speaker talk at inaugural "Ultrafast Scotland" regional meeting (held 19th March 2018)
Year(s) Of Engagement Activity 2018
 
Description Virtual visit to Sandia National Lab, Livermore (Chemical Sciences, Geosciences and Biological Sciences Division). 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Invited talk to Sandia National Lab, Livermore (Chemical Sciences, Geosciences and Biological Sciences Division). Part of developing strategic links with Dr David Chandler, who has been given Honorary status at Heriot-Watt University and at Oxford University (collaborators under New Directions in Moleclar Scattering grant).
Year(s) Of Engagement Activity 2022
 
Description Visit to EPFL, Lausanne, Switzerland 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Professional Practitioners
Results and Impact Research visit to EPFL. Gave a research seminar, visited several research labs. Carried out a PhD examination.
Year(s) Of Engagement Activity 2022
 
Description York Talk 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Local
Primary Audience Postgraduate students
Results and Impact Invited talk at Department of Chemistry, University of York (21st November 2018)
Year(s) Of Engagement Activity 2018