Controlling photophysics and photochemistry via quantum superpositions of electronic states: towards attochemistry

Lead Research Organisation: Imperial College London
Department Name: Physics


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Barnard JCT (2022) Delivery of stable ultra-thin liquid sheets in vacuum for biochemical spectroscopy. in Frontiers in molecular biosciences

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English J (2022) Mercury Liquid Embrittlement Failure of 5083-O Aluminum Alloy Piping in Journal of Failure Analysis and Prevention

Description The laboratory work in my laboratory just started (Jan 2021) with the appointment of a PDRA (Jonathan Tobit Barnard) who has begun work on setting up the ultrafast pump pulses (UV/deep UV) in collaboration with two PhD students (Jacob Lee and Timur Avni). In the meantime earlier experimental work using high harmonic generation (HHG) spectroscopy that is part of this project was published in Scientific Reports. This demonstrates how ultrafast molecular nuclear dynamics can be extracted from HHG spectra using a laser intensity self-referencing scheme. Further work on molecular dynamics measured by HHG spectroscopy of benzene and substituted benzene has been submitted.
A new experimental set-up for pump-probe x-ray spectroscopy with sub-10 fs temporal resolution has been commissioned and validated. New experiments on glycine have been completed at the FLASH FEL and are under analysis. Proposals for beamtime at LCLS to investigate charge migration in glycine, phenylalinine and tryptophan have been submitted.

Close collaboration with our theory colleagues is leading to new insights and developing further experiments.
Exploitation Route Other academic users in chemical physics and reaction dynamics may be able to use this result in there research. Our methodology for measuring charge migration via x-ray absorption spectroscopy registered via Auger decay has been adopted by other laboratories.
Sectors Chemicals


Description Enhancements of standard quantum chemistry packages, informed by this research, are in progress. Generation and delivery of few femtosecond tuneable Vis-UV sources anticipated to find wider impact in technology and science.
First Year Of Impact 2021
Sector Chemicals,Electronics,Energy,Pharmaceuticals and Medical Biotechnology
Description Science Lead UK XFEL Project 2019-2025
Geographic Reach National 
Policy Influence Type Contribution to a national consultation/review
Description Attosecond Electronic Dynamics of the Valence States in Matter Measured with XFELs
Amount £834,035 (GBP)
Funding ID EP/X026094/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 04/2023 
End 04/2026
Description Ultrafast Photochemical Dynamics in Complex Environments
Amount £8,055,186 (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 Proving of utility of attosecond X-ray pulses from XFELs 
Description We have used the XLEAP (attosecond pulse mode) in both single colour and two-colour format to demonstrate new capability in X-ray non-linear optics, X-ray pump-probe spectroscopy and time resolving photoelectron emission. 
Type Of Material Improvements to research infrastructure 
Year Produced 2020 
Provided To Others? Yes  
Impact So far a number of high profile publications in PRX, PRL and Science 
Description Bucksbaum Group - Stanford University 
Organisation Stanford University
Country United States 
Sector Academic/University 
PI Contribution We have provided ideas and expertise to progress research in ultrafast X-ray science by leading and participating in a number of joint beamtimes.
Collaborator Contribution Through this collaboration we have been able to efficiently engage in X-ray free electron laser research at the LCLS facility SLAC through their local resources and manpower. It has enabled around 10 separate beam-times.
Impact A number of research papers including 1 PRL, 2 Nature Communications and more in preparation.
Start Year 2011
Description SLAC Photon Sciences 
Organisation Stanford University
Department SLAC National Accelerator Laboratory
Country United States 
Sector Public 
PI Contribution We are a member of an international collaboration, the "Attosecond Campaign" coordinated by SLAC (Dr Agostino Marinelli and Dr James Cryan SLAC leads) aimed at developing attosecond measurements of electron dynamics using newly proven X-ray FEL capabilities.
Collaborator Contribution They provide the support of X-ray FEL beamtime and run the experimental endstation
Impact A papers published in PRL, Nature Photonics, Science
Start Year 2020