Ultrafast Intra-Molecular Electron Dynamics
Lead Research Organisation:
Queen's University Belfast
Department Name: Sch of Mathematics and Physics
Abstract
The study of dynamic processes in nature continues to breach new frontiers as the timescales and dimensions under investigation shrink. These advances have gone hand-in-hand with generation of ever shorter light pulses from conventional laser and accelerator based sources, which are exploited as ultrafast strobes for observing the dynamics of matter. While the motion of atoms can now be tracked with femtosecond pulses of light, the recent advent of attosecond pulses (a billion billionth of a second) has the potential to capture the movement of electrons. The ability to observe and control this quantum electronics will be essential for the future understanding and exploitation of electrical, chemical, and biological processes in natural and synthetic nano-structures.
In this project, coherent charge dynamics in some exemplar biological frameworks, amino acids and small peptides, will be generated and observed using a state-of-the-art attosecond laser. These laboratory measurements will probe the ultrafast movement of charge created by ionising radiation from which some of the remarkable electrical properties of these complex biological molecules will be discerned. Ultimately, the pathways for understanding the role of the underlying molecular structures and methods for quantum control of the electrons will be investigated.
In this project, coherent charge dynamics in some exemplar biological frameworks, amino acids and small peptides, will be generated and observed using a state-of-the-art attosecond laser. These laboratory measurements will probe the ultrafast movement of charge created by ionising radiation from which some of the remarkable electrical properties of these complex biological molecules will be discerned. Ultimately, the pathways for understanding the role of the underlying molecular structures and methods for quantum control of the electrons will be investigated.
Planned Impact
The results and outcomes of the research from this project will have a direct impact in number of UK and EU networks and laser infrastructures in which the project researchers are already participating, e.g. EPSRC Grand Challenge Networks, the STFC Central Laser Facility, COST Actions, and the European Extreme Light Infrastructure. The research methodology will instigate state-of-the-art training in a range of emerging technologies for participating PhD students which will include development of public dissemination skills through production of videos, websites and animations on the research.
Organisations
- Queen's University Belfast (Lead Research Organisation)
- European Cooperation in Science and Technology (COST) (Collaboration)
- Case Western Reserve University (Collaboration)
- Heriot-Watt University (Collaboration)
- University of Bordeaux (Collaboration)
- Uppsala University (Collaboration)
- Polytechnic University of Milan (Collaboration)
- Politecnico di Milano (Project Partner)
Publications
Calegari F
(2016)
Charge migration induced by attosecond pulses in bio-relevant molecules
in Journal of Physics B: Atomic, Molecular and Optical Physics
Calegari F
(2015)
Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses
in IEEE Journal of Selected Topics in Quantum Electronics
Calegari F.
(2018)
Attosecond spectroscopy of bio-chemically relevant molecules
in RIVISTA DEL NUOVO CIMENTO
Comby A
(2020)
Using photoelectron elliptical dichroism (PEELD) to determine real-time variation of enantiomeric excess.
in Chirality
Comby A
(2018)
Real-time determination of enantiomeric and isomeric content using photoelectron elliptical dichroism.
in Nature communications
Crane SW
(2019)
Dynamics of electronically excited states in the eumelanin building block 5,6-dihydroxyindole.
in Physical chemistry chemical physics : PCCP
De Camillis S
(2015)
Ultrafast non-radiative decay of gas-phase nucleosides.
in Physical chemistry chemical physics : PCCP
Ghafur O
(2018)
Ultraviolet relaxation dynamics in uracil: Time-resolved photoion yield studies using a laser-based thermal desorption source.
in The Journal of chemical physics
Lara-Astiaso M
(2018)
Attosecond Pump-Probe Spectroscopy of Charge Dynamics in Tryptophan.
in The journal of physical chemistry letters
Miles J
(2015)
Detection limits of organic compounds achievable with intense, short-pulse lasers.
in The Analyst
Description | We have developed an experimental techniques which has been able to make the first direct measurements of electron motion within large molecules . Such charge transfer is believed to be crucial to many processes in biology and its understanding will be crucial in understanding charge behaviour in nano-scale devices. We are currently working with our collaborators to develop new sources of ultrashort ultraviolet light which will help progress our understanding of these processes. |
Exploitation Route | Our results have already inspired many theoretical groups to model the behaviour of electrons in complex systems as evidenced by the already high number of citations for our recent paper published in Science. The techniques we have developed are also likely to inspire new developments in ultrashort light sources with wavelengths from the infrared to X-rays. |
Sectors | Electronics,Pharmaceuticals and Medical Biotechnology |
URL | http://ultrafastbelfast.com |
Description | The main impact of the project which goes beyond the academic output, is that it has stimulated the development of a new field of research - attosecond chemistry. This has led to creation of a large COST Action - AttoChem which is currently active and many collaborators have gone on to form high profile research groups in this field - https://attochem.qui.uam.es/. In particular, two groups (Calegari - experiment, Rubio - theory) have been set up at the Centre for Free Electron Science at DESY, Hamburg. This has stimulated a drive to develop attosecond pulses from Free Electron Lasers. As a result the PI - Jason Greenwood was part of the team writing the case for an X-ray Free Electron Laser facility in the UK - https://www.clf.stfc.ac.uk/Pages/UK-XFEL-science-case.aspx. This submission is currently being considered by the UK government to move to the design stage of this facility (~£1B cost). |
First Year Of Impact | 2020 |
Sector | Pharmaceuticals and Medical Biotechnology |
Impact Types | Policy & public services |
Description | Paul Instrument Fund |
Amount | £74,778 (GBP) |
Funding ID | PI170043 |
Organisation | The Royal Society |
Sector | Charity/Non Profit |
Country | United Kingdom |
Start | 02/2018 |
End | 01/2020 |
Title | Chiral mass spectrometer |
Description | This is a new device which is capable of identifying the handedness of chiral molecules and the chemical composition of samples at the same time. It is based on a new chiral phenomenon of photoelectric circular dichroism which shows an asymmetry in the electron emission from photoionised chiral molecules. An innovate experimental setup has been used to measure this phenomenon. |
Type Of Material | Improvements to research infrastructure |
Year Produced | 2017 |
Provided To Others? | Yes |
Impact | Interest from the academic community but also from some commercial companies. |
Description | Attosecond Electron Dynamics |
Organisation | Polytechnic University of Milan |
Country | Italy |
Sector | Academic/University |
PI Contribution | This collaboration was initiated in 2012 through a beamtime application to Laserlab-Europe to use the Attosecond Laser Facility in Milan. We have been on several experimental campaigns at this facility using our apparatus. Our techniques for volatilising biomolecules have allowed the partnership to study electron dynamics in a complex molecule for the first time. |
Collaborator Contribution | The group of Mauro Nisoli have set up the brightest source of attosecond laser pulses in the world and an ultrafast pump-probe scheme with a time resolution approaching attosecond timescales. In combination with our molecular target techniques, we have been the first to directly observe electron motion in a complex structure. |
Impact | Ultrafast Electron Dynamics in Phenylalanine Initiated by Attosecond Pulses F. Calegari, D. Ayuso, A. Trabattoni, L. Belshaw, S. De Camillis, S. Anumula, F. Frassetto, L. Poletto, A. Palacios, P. Decleva, J.B. Greenwood, F. Martín, and M. Nisoli Science, 346, 336-339 (2014), DOI: 10.1126/science.1254061 Observation of Ultrafast Charge Migration in an Amino Acid L. Belshaw, F. Calegari, M.J. Duffy, A. Trabattoni, L. Poletto, M. Nisoli and J.B. Greenwood Journal of Chemical Physics Letters, 3, 3751-3754 (2012) Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses Francesca Calegari, David Ayuso, Andrea Trabattoni, Louise Belshaw, Simone De Camillis, Fabio Frassetto, Luca Poletto, Alicia Palacios, Piero Decleva, Jason B. Greenwood, Fernando Martin, and Mauro Nisoli IEEE Journal of Selected Topics in Quantum Electronics, 21, 8700512 (2015) Charge migration induced by attosecond pulses in biorelevant molecules Francesca Calegari, Andrea Trabattoni, Alicia Palacios, Davis Ayuso, Jason B. Greenwood, Piero Decleva, Fernando Martin and Mauro Nisoli Journal of Physics B, 49, 142001 (2016) |
Start Year | 2012 |
Description | Attosecond Electron Dynamics - Theory |
Organisation | Case Western Reserve University |
Department | Department of Chemistry |
Country | United States |
Sector | Academic/University |
PI Contribution | We have acquired attosecond pump-probe data of electron dynamics in the amino acid phenylalanine. This has stimulated interest from this group in calculating the evolution of the electron wavepacket in this molecule. |
Collaborator Contribution | Fernando Martin's group has performed state-of-the-art calculations to simulate the ultrafast intra-molecular dynamics we have observed in our experiments. |
Impact | Ultrafast Electron Dynamics in Phenylalanine Initiated by Attosecond Pulses F. Calegari, D. Ayuso, A. Trabattoni, L. Belshaw, S. De Camillis, S. Anumula, F. Frassetto, L. Poletto, A. Palacios, P. Decleva, J.B. Greenwood, F. Martín, and M. Nisoli Science, 346, 336-339 (2014), DOI: 10.1126/science.1254061 Charge migration induced by attosecond pulses in biorelevant molecules Francesca Calegari, Andrea Trabattoni, Alicia Palacios, Davis Ayuso, Jason B. Greenwood, Piero Decleva, Fernando Martin and Mauro Nisoli Journal of Physics B, 49, 142001 (2016) Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses Francesca Calegari, David Ayuso, Andrea Trabattoni, Louise Belshaw, Simone De Camillis, Fabio Frassetto, Luca Poletto, Alicia Palacios, Piero Decleva, Jason B. Greenwood, Fernando Martin, and Mauro Nisoli IEEE Journal of Selected Topics in Quantum Electronics, 21, 8700512 (2015) |
Start Year | 2013 |
Description | Chiral Photoelectron Spectroscopy |
Organisation | University of Bordeaux |
Department | Center for Intense Lasers and Applications |
Country | France |
Sector | Academic/University |
PI Contribution | Participation in joint and complementary experiments |
Collaborator Contribution | Joint experiments in July 2018 in Bordeaux, results obtained in Belfast for a joint publication, successful proposal for laser beamtime at CELIA via Laserlan Europe Infrastructure written by me. |
Impact | Publication in preparation |
Start Year | 2018 |
Description | Gas Phase Molecular Dynamics |
Organisation | Heriot-Watt University |
Department | School of Engineering & Physical Sciences |
Country | United Kingdom |
Sector | Academic/University |
PI Contribution | This was a collaborative project with Dr. David Townsend funded by the Leverhulme Trust to develop techniques for studying the ultrafast dynamics of non-volatile molecules in the gas phase. Although this project finished in 2016 there is a continuing collaboration. |
Collaborator Contribution | Development of new technique to volatilise labile molecules. Use of a femtosecond laser to test instrumentation and measure ultrafast dyanamics. |
Impact | Ultrafast Non-Radiative Decay of Gas-Phase Nucleosides Simone De Camillis, Jordan Miles, Grace Alexander, Omair Ghafur, Ian D. Williams, Dave Townsend, Jason B. Greenwood Physical Chemistry Chemical Physics, 17, 23643-23650 (2015) |
Start Year | 2013 |
Description | Photoelectron Elliptical Dichroism |
Organisation | University of Bordeaux |
Department | Center for Intense Lasers and Applications |
Country | France |
Sector | Academic/University |
PI Contribution | We have performed joint, complementary experiments in Bordeaux and Belfast to study a new phenomenon in photoelectron spectroscopy. |
Collaborator Contribution | The CELIA lab has a suit of high spec laser facilities at which we performed experiments. This facility is part of the Laserlab Europe EU infrastructure and we have successfully applied for beamtime to perform experiments there. |
Impact | The work undertaken so far has been published in Nature Communications. |
Start Year | 2017 |
Description | UK representative on management board of the MD-GAS (Molecular Dynamics in the Gas Phase) EU COST Action |
Organisation | European Cooperation in Science and Technology (COST) |
Country | Belgium |
Sector | Public |
PI Contribution | I am the Uk representative on the management board of this network |
Collaborator Contribution | This COST action supports conferences, training and networking events for members, and funds short term scientific missions to labs within the network |
Impact | None so far |
Start Year | 2019 |
Description | Ultrafast catalytic dynamics |
Organisation | Uppsala University |
Country | Sweden |
Sector | Academic/University |
PI Contribution | This is a collaboration with Jacinto Sa (former at Swiss Light Source, Zurich) who studies fundamental ultrafast processes in catalytic systems. Through our collaboration we have introduced Jacinto the ultrafast pump-probe experiments which has resulted in a successful application for beamtime by him at the Attosecond Laser Facility in Milan to study charge separation in TiO2 catalysts. |
Collaborator Contribution | Jacinto has introduced to our research group the importance of electron processes such as charge separation in catalysts and possibilities for light induced reduction of water and CO2 in futrue fuel cells. |
Impact | Femtosecond lasers for mass spectrometry: Proposed application to catalytic hydrogenation of butadiene Orla Kelly, Martin J. Duffy, Raymond B. King, Louise Belshaw, Ian D. Williams, Jacinto Sa, Chris R. Calvert and Jason B. Greenwood Analyst, 137, 64 (2012) |
Start Year | 2012 |
Description | Institute of Physcis in Ireland Lecture Tour |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | Regional |
Primary Audience | Undergraduate students |
Results and Impact | This was a general talk on my attosecond science research |
Year(s) Of Engagement Activity | 2016 |
Description | Invited Talk at Kassel University |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | There were around 30 researchers in the audience. The talk was also streamed to 3 other institutions involved in a long term research project with Kassel. |
Year(s) Of Engagement Activity | 2018 |
URL | http://www.uni-kassel.de/cinsat/en/projekte/sp5-chirale-systeme.html |
Description | Invited Talk at XLIC COST Action Annual Meeting, Prague, April 2017 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | This was presented to a academics, researchers and postgraduate students engaged in the COST Action. It was an opportunity to disseminate a new technique we have developed along with our first results. This has since stimulated a collaboration with the University of Bordeaux |
Year(s) Of Engagement Activity | 2017 |
URL | http://www.qub.ac.uk/mp/ampr/ultrafastbelfast/Homepage.htm |
Description | Northern Ireland Science Festival |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | Regional |
Primary Audience | Public/other audiences |
Results and Impact | I gave lectures as part of the Northern Ireland Science Festival and Open Day organised in conjunction with the Ulster Museum. These lectures were on Lasers in Medicine and Lasers in the Movies. |
Year(s) Of Engagement Activity | 2010,2015 |
Description | Research Talk in the Chemistry Dept of Uppsala University |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Postgraduate students |
Results and Impact | This was an invited talk about recent research given to about 30 members of the Chemistry Dept at Uppsala Unversity |
Year(s) Of Engagement Activity | 2017 |
Description | Talk as the International Conference on Spectral Line Shapes - Dublin, July 2018 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | This was an invited talk on chiral photoelectron spectroscopy at an international conference. |
Year(s) Of Engagement Activity | 2018 |
Description | Talk at the Frontiers in Physical Science Workshop (Imperial College, Nov 2019) for Developing a Science Case for a UK Free Electron Laser |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | This workshop was the basis for developing a science case for building an X-ray Free Electron Laser in the UK. |
Year(s) Of Engagement Activity | 2019 |