Controlling photophysics and photochemistry via quantum superpositions of electronic states: towards attochemistry
Lead Research Organisation:
Imperial College London
Department Name: Physics
Abstract
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Publications
Alexander O
(2024)
Attosecond impulsive stimulated X-ray Raman scattering in liquid water.
in Science advances
Barillot T
(2021)
Correlation-Driven Transient Hole Dynamics Resolved in Space and Time in the Isopropanol Molecule
in Physical Review X
Barnard JCT
(2022)
Delivery of stable ultra-thin liquid sheets in vacuum for biochemical spectroscopy.
in Frontiers in molecular biosciences
Danilov D
(2023)
Coherent Mixing of Singlet and Triplet States in Acrolein and Ketene: A Computational Strategy for Simulating the Electron-Nuclear Dynamics of Intersystem Crossing.
in The journal of physical chemistry letters
Danilov D
(2022)
How electronic superpositions drive nuclear motion following the creation of a localized hole in the glycine radical cation.
in The Journal of chemical physics
Deumal M
(2024)
Using 'designer' coherences to control electron transfer in a model bis(hydrazine) radical cation: can we still distinguish between direct and superexchange mechanisms?
in Journal of Physics B: Atomic, Molecular and Optical Physics
Deumal M
(2024)
Real-Time CASSCF (Ehrenfest) Modeling of Electron Dynamics in Organic Semiconductors. Dynamics Reaction Paths Driven by Quantum Coherences. Application to a Radical Organic Semiconductor
in The Journal of Physical Chemistry A
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. In particular a collaboration with Morgane Vacher at University of Nantes where we could confirm a theoretical prediction for the ultrafast evolution of the electronic and nuclear states in fluorobenzene was confirmed by measurements in our laboratory. |
| 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 Energy |
| 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 |
| URL | https://www.xfel.ac.uk/ |
| 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 |
| Title | Attosecond impulsive stimulated x-ray raman scattering in liquid water |
| Description | We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket, which comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to a valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a non-linear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarisation response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density. |
| Type Of Material | Database/Collection of data |
| Year Produced | 2024 |
| Provided To Others? | Yes |
| URL | https://datadryad.org/stash/dataset/doi:10.5061/dryad.dv41ns26m |
| Title | Raw data for Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser |
| Description | There are 4 Jupyter notebooks in this folder:Generate_Correlation_Map_for_Delay _Analysis.ipynb: It generates the correlation map used in the delay analysis.Draw_Differential_Map.ipynb: It loads the raw data of streaked images with similar streaking directions and generates an average sorted streaked image. It also draws the differential map between the average sorted streaked image and the average unstreaked image.Draw_Strongly_Streaked_Shots.ipynb: It loads the raw data of some good streaked images. This notebook also plots two shots with different streaking directions.Covariance_Demonstration_of_attosecond_Xray_FEL_pump_probe.ipynb: This is a Jupyter notebook that uses the Run24 file to process the data, perform covariance analysis, and extract the binding energy of a carbon 1s photoelectron feature. |
| Type Of Material | Database/Collection of data |
| Year Produced | 2024 |
| Provided To Others? | Yes |
| URL | https://figshare.com/articles/dataset/Raw_data_of_angular_streaking_measurement/23232350/2 |
| Title | Raw data for Experimental Demonstration of Attosecond Pump-Probe Spectroscopy with an X-ray Free-Electron Laser |
| Description | There are 4 Jupyter notebooks in this folder:Generate_Correlation_Map_for_Delay _Analysis.ipynb: It generates the correlation map used in the delay analysis.Draw_Differential_Map.ipynb: It loads the raw data of streaked images with similar streaking directions and generates an average sorted streaked image. It also draws the differential map between the average sorted streaked image and the average unstreaked image.Draw_Strongly_Streaked_Shots.ipynb: It loads the raw data of some good streaked images. This notebook also plots two shots with different streaking directions.Covariance_Demonstration_of_attosecond_Xray_FEL_pump_probe.ipynb: This is a Jupyter notebook that uses the Run24 file to process the data, perform covariance analysis, and extract the binding energy of a carbon 1s photoelectron feature. |
| Type Of Material | Database/Collection of data |
| Year Produced | 2024 |
| Provided To Others? | Yes |
| URL | https://figshare.com/articles/dataset/Raw_data_of_angular_streaking_measurement/23232350 |
| 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 |