Photoelectron interferometry as a structural and dynamical probe

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

Abstract

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Publications

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Razmus WO (2022) Multichannel photodissociation dynamics in CS2 studied by ultrafast electron diffraction. in Physical chemistry chemical physics : PCCP

 
Description Through the course of the grant we have worked to develop tools for the detailed measurement and analysis of photoelectron spectra. We have measured time-resolved photoelectron images and spectra of quantum chemical dynamics and, developed and implemented the tools and techniques to align molecules or varying degrees of complexity around a particular axis in space and then ionised these molecules using both single and multiple photon absorption. The experimental results allow us to obtain much more detailed measurements of the underlying electronic structure of molecules through comparison to advanced theoretical simulations. Through the project we have developed a new photoelectron imaging spectrometer and also developed a workflow for the analysis of molecular frame measurements that will in the future allow for more accurate, quantitative analysis of the obtained photoelectron angular distributions. The results of recent experiments are still being analysed but will be published in due course.
The work has expanded and we have developed further collaborations in the field with international academics and international facilities that we are now actively working with to develop the field further.
Exploitation Route The research sets a protocol and toolbox for analysis of photoelectron images. We are continuing this research with collaborators in Europe and North America to standardise the representation of data and simulations, to improve communication between the different research fields impacted and remove some of the ambiguity present in much of the data in the literature. This will allow the molecular control community, the chemical dynamics community and the photoelectron spectroscopy community to talk in a common language when discussing data of this type. We hope this will allow for the different scientific communities to overcome critical barriers to the future development of quantitative modelling of photoelectron spectra which will truly transform the field. The data we have obtained will provide the first input data for this development.
The delays cause by these two effects meant the most challenging aspect of the project - performing time-resolved measurements of the photochemical dynamics of aligned molecules could not be attempted during the project.
Sectors Other

 
Description Next Generation Experiment and Theory for Photoelectron Spectroscopy
Amount £1,500,000 (GBP)
Funding ID EP/X027635/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 06/2023 
End 12/2026
 
Title Extreme ultraviolet photoelectron imaging endstation 
Description We have designed and built a new velocity map imaging (VMI) spectrometer optimised for the detection of high energy photoelectrons. The spectrometer is attached to a high harmonic generation source allowing for universal chemical detection. 
Type Of Material Improvements to research infrastructure 
Year Produced 2021 
Provided To Others? No  
Impact The development of the instrument was significantly delayed by the pandemic which shut our internal workshops and then reduced capacity for work. The instrument is now commissioned and we have attracted further funding to use the system moving forward. 
 
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 ELI Beamlines studentship 
Organisation Extreme Light Infrastructure Beamlines
Country Czech Republic 
Sector Public 
PI Contribution We have contributed both manpower and scientific expertise to the development of the MAC endstation. This has fed into the experimental development and development plans of the facility.
Collaborator Contribution ELI beamllnes have provided several weeks of access to the facility for the development of the MAC endstation for photoelectron spectroscopy measurements. To this end they have supported travel costs and experimental costs associated with the running, maintanance and development of the facility. They have also provided cofunding for a PhD studentship starting October 2022 for three and a half years.
Impact none to date
Start Year 2019
 
Description General Public talks - molecular movies 
Form Of Engagement Activity A talk or presentation
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Public/other audiences
Results and Impact General public lectures held in the evening at schools in Bournemouth area. On average about 30 people attended with large numbers of questions at the end. The presentation is about how we can use technology to obtain detailed views of chemical structure and reactions as they happen. The talk cover many aspects of chemistry that are not often discussed and shows that chemists work in a variety of environments, not just wet chemistry labs.
The feedback has been excellent with many students from chemistry, biology and physics attending.
Year(s) Of Engagement Activity 2022