Ultrafast Intra-Molecular Electron Dynamics

Lead Research Organisation: Queen's University of 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.

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.

Publications

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Calegari F (2016) Charge migration induced by attosecond pulses in bio-relevant molecules in Journal of Physics B: Atomic, Molecular and Optical Physics

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Calegari F (2015) Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses in IEEE Journal of Selected Topics in Quantum Electronics

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De Camillis S (2015) Ultrafast non-radiative decay of gas-phase nucleosides. in Physical chemistry chemical physics : PCCP

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Lara-Astiaso M (2018) Attosecond Pump-Probe Spectroscopy of Charge Dynamics in Tryptophan. in The journal of physical chemistry letters

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Månsson EP (2017) Ultrafast dynamics in the DNA building blocks thymidine and thymine initiated by ionizing radiation. in Physical chemistry chemical physics : PCCP

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Poully JC (2015) Proton irradiation of DNA nucleosides in the gas phase. in Physical chemistry chemical physics : PCCP

 
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 Paul Instrument Fund
Amount £74,778 (GBP)
Funding ID PI170043 
Organisation The Royal Society 
Sector Academic/University
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 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