Time resolved photoelectron spectroscopy of chemical dynamics

Lead Research Organisation: University of Southampton
Department Name: Sch of Chemistry

Abstract

The PhD project involves the experimental development and implementation of a state of the art XUV photoelectron spectroscopy experiment within our own laser lab and at international X-ray free electron laser facilities. The experiments aim to uncover some of the most fundamental aspects of photochemistry that underlie light initiated processes in chemistry and biology. The development of these sources will remove the limited observation window of most spectroscopy techniques and will allow us to uncover the full reaction pathway for the first time.

Publications

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Studentship Projects

Project Reference Relationship Related To Start End Student Name
EP/N509747/1 01/10/2016 30/09/2021
1839943 Studentship EP/N509747/1 01/01/2017 31/12/2019 Emily Warne
 
Description Our most significant achievements centre on the development of XUV photoelectron spectroscopy capabilities leading to the first UK demonstration of the measurement of a complete reaction pathway in carbon disulphide. Subsequent measurements of the wavelength dependent dynamics in methyl iodide have also resulted in previously unseen dynamics that have been missed in previous experiments. The results highlight the importance of measuring full reaction pathways and the extra information available and vital for a full understanding of what controls photochemical reactivity. The technique is still in its early stages of development but with advances in laser technology, particularly high repetition rate laser systems, there is a clear development pathway but one that requires investment.
Exploitation Route All experiments have been performed on conventional lab based laser systems with X-ray free electron laser experiments unfortunately not awarded beamtime. Significantly many experiments have involved extensive development work at the Artemis central laser facility meaning the work can directly benefit the wider chemical dynamics community. The methodology development is therefore available to the UK laser community through open call for access to Artemis. Specific results related to the chemical systems have also been picked up by international groups and have led to new collaborations based around relativistic electron diffraction measurements and X-ray free electron laser based coulomb explosion imaging measurements. The methodology developments and scientific results are therefore being taken forward by the international and national chemical dynamics community as we build our understanding towards larger chemical systems.
Sectors Chemicals

URL https://www.clf.stfc.ac.uk/Pages/Mapping-the-complete-reaction-.aspx
 
Description Frequency Upconversion using Hollow Core Fibre Sources for Ultrafast Chemistry and Microscopy
Amount £20,000 (GBP)
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 03/2020 
End 07/2020
 
Title CS2 data 
Description DOI: 10.5258/SOTON/D0455 Data associated with paper DOI: 10.1103/PhysRevLett.120.183003 
Type Of Material Database/Collection of data 
Year Produced 2018 
Provided To Others? Yes  
Impact Paper DOI: 10.1103/PhysRevLett.120.183003 
 
Title Methyl Iodide MPI data 
Description Data doi.org/10.5258/SOTON/D1273 associated with paper DOI:10.1039/c9cp01477b (Photodissociation dynamics of CH3I probed via multiphoton ionisation photoelectron spectroscopy) 
Type Of Material Database/Collection of data 
Year Produced 2020 
Provided To Others? Yes  
Impact Paper: "Photodissociation dynamics of CH3I probed via multiphoton ionisation photoelectron spectroscopy" 
URL https://doi.org/10.5258/SOTON/D1273
 
Description Adam Kirrander - Edinburgh 
Organisation University of Edinburgh
Country United Kingdom 
Sector Academic/University 
PI Contribution Experimental data: time-resolved photoelectron spectra
Collaborator Contribution Computational results: potential energy surfaces and wavepacket trajectories
Impact DOI:10.1103/PhysRevLett.120.183003
Start Year 2017
 
Description Artemis Central Laser Facility 
Organisation Rutherford Appleton Laboratory
Department Central Laser Facility
Country United Kingdom 
Sector Academic/University 
PI Contribution The Artemis central laser facility houses the UK femtosecond XUV laser facility for scientific applications. We have worked with the Artemis team to develop gas phase photo electron spectroscopy capabilities and molecular frame measurements. This has involved input into the design and development of the facility and hands on optimisation and commissioning of new experimental processes. We are also starting to work on the use of hollow core fiber sources for UV pulse generation.
Collaborator Contribution The Artemis team manage and maintain the facility and provide input into feasibility and design of experiments as well as experimental support during beamtime and commissioning phases.
Impact to do
Start Year 2011
 
Description Poster: Development of time-resolved XUV photoelectron capabilities in Southampton and at Artemis 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact I presented a poster about "Development of time-resolved XUV photoelectron capabilities in Southampton and at Artemis" at a number of conferences, to an audience of other researchers in the field. The conferences were: Artemis User Meeting, September 2017; Spectroscopy and Dynamics Group conference, January 2018; PALM International School - Attosecond Science: From Ultrafast Sources to Applications, May 2018
Year(s) Of Engagement Activity 2017,2018
 
Description Poster: Using UV and XUV Time Resolved Photoelectron Spectroscopy to Probe the Dissociation Dynamics of Methyl Iodide 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Other audiences
Results and Impact I presented a poster on "Using UV and XUV Time Resolved Photoelectron Spectroscopy to Probe the Dissociation Dynamics of Methyl Iodide" at the 2019 International Symposium of Molecular Beams.
Year(s) Of Engagement Activity 2019
 
Description Talk: Mapping the Dissociation Dynamics of Methyl Iodide 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Other audiences
Results and Impact I gave a talk on "Mapping the Dissociation Dynamics of Methyl Iodide" at the 2019 Spectroscopy and Dynamics Group conference, to an audience of researchers in the field.
Year(s) Of Engagement Activity 2019