Control and Imaging of processes triggered by X-ray pulses in multi-center molecules

Lead Research Organisation: University College London
Department Name: Physics and Astronomy

Abstract

Attoscience is one of the great scientific challenges of the 21st century. While femtosecond laser pulses provided a candid camera into the world of nuclear motion, attosecond laser pulses will bring a revolution in our understanding of electron dynamics. Attoseconds and sub-femtoseconds are the natural time scale for multi-electron effects during complete ionization and break-up of atoms and molecules.
Attosecond ``steering" of electrons in chemical bonds using ultra-short pulses is a fundamental way of manipulating
the molecular structure. Controlling the electronic motion in small molecules will pave the way for modifying
the structure of complex biomolecules, thus impacting such diverse fields as physics, chemistry and biology.


The overall aim of the proposed work is to harness the properties of ultra-short and ultra-strong laser pulses to time-resolve and control attosecond phenomena triggered by intense X-ray laser pulses in multi-center molecular systems. The rapid experimental advances make urgent the quest for new theoretical tools that will address the challenges facing Attoscience.
The main intellectual weapon that I bring is my expertise on novel, non-mainstream quasiclassical techniques that are much faster than quantum-mechanical ones and that allow for significant insights into the physical mechanisms. These techniques are appropriate for ionization processes through long range Coulomb forces. I propose to deliver sophisticated and efficient techniques for tackling some of the most fundamental problems facing Attoscience. My objectives are:

1)Explore the correlated dynamics of two-electron escape during the break-up of multi-center molecules triggered by intense and ultra-fast X-ray pulses.
2)Explore pump-probe schemes for coherent control and transfer of electrons in multi-center molecules.
3)Use infrared laser pulses as an ``attosecond clock" to accurately map the properties of the observed spectra of the final fragments to the temporal evolution of correlated electron escape dynamics during the break-up, by X-rays, of molecules.

Planned Impact

The proposed research is on exploring multi-electron effects on an attosecond time-scale during the complete ionization
and break-up of multi-center molecules. Understanding the electronic motion on an attosecond time-scale in atomic and
molecular systems will be of importance in the future for a number of industries that closely work with applied researchers in order to enhance the industries' capabilities.
My results will be communicated to these applied researchers through academic dissemination but most importantly through direct interaction with them at the London Center for Nanotechnology (LCN). LCN aims to provide the nanoscience and nanotechnology needed to solve major problems in information processing, health care, and energy and environment.
In the sense mentioned above, my research will contribute in addressing the first two of the above strategic areas of LCN---such potential applications of attoscience are well-acknowledged and identified.

Namely, the density of information flow, such as operations performed by a computer, is determined by how fast the electron current can be switched on and off in a digital chip.
The current state-of-the-art in electronic circuits dictates a switching time within a fraction of a nanosecond. To achieve higher density of information, faster switching times need to be achieved, such as attoseconds. The latter is the natural time-scale for electronic motion in neighbouring atoms in a crystal lattice or in a small molecule. Thus, understanding and controlling the attosecond electronic
motion in molecules (one of the goals of the proposed research) and solid state structures opens up the way for researching technologies that may lead to speeding up current electronics
by several orders of magnitude. In addition, controlling the electronic motion in small molecules using ultrashort laser pulses (one of the goals of the proposed research) will pave the way for ``steering" electronic motion and thus affecting the structure of biomolecules. This will lead to a better understanding of how to control radiation damage in biological systems and thus how to achieve the best effect in radiation therapies, significantly impacting the technology associated with health care.

Publications

10 25 50
 
Description In the first two years of this award we have explored single photon processes in multi-electron atoms. Specifically we have shown that for the ground state of Be the four electrons, for a photon energy close to the fragmentation threshold of Be, escape on the apexes of a triangular pyramid. This is an unexpected pattern since according to the famous Wannier law (1950s) we expect the four electrons to escape on the apexes of a regular tetrahedron. Moreover, we verified, with a fully quantum-mecha
Exploitation Route As explained above we have developed a powerful and novel computational toolkit that can be used by other AMO scientists to explore the fragmentation of multi-center molecules when driven by strong-fields.
Sectors Digital/Communication/Information Technologies (including Software),Education,Energy

 
Description We have developed computer algorithms and models to describe strongly driven multi-center molecules and non-dipole effects in strongly-driven atoms
Sector Digital/Communication/Information Technologies (including Software),Education
Impact Types Economic

 
Description Semi-classical models for ultra-fast multi-electron phenomena in intense electro-magnetic laser fields
Amount £336,665 (GBP)
Funding ID EP/N031326/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 10/2016 
End 09/2020
 
Title Two-electron dynamics in ultra-short and intense electromagnetic fields 
Description The last few months we have developed in my group a new state-of-the-art theoretical and computational tool to describe the two-electron dynamics in intense and ultra-short laser pulses. The innovative aspect and strength of this theoretical technique and computational tool is that it allows one to account for non-dipole effects, i.e. the effect of the magnetic field, in strongly-driven molecules. The vast majority of strong-field studies use the dipole approximation to describe strongly-driven molecules and in most studies the nuclei are fixed. This powerful computational tool will allow our group to perform the first studies of magnetic field effects during the break-up of strongly driven diatomic and triatomic molecules. In the next few months we will investigate the effect of the magnetic field in the different mechanisms of Rydberg formation, we have introduced the latter a few years ago, as well as the magnetic effects on non-sequential double ionization. This tool along with the magnetic field effects will be published in the next few months. 
Type Of Material Improvements to research infrastructure 
Year Produced 2020 
Provided To Others? No  
Impact This tool will have significant impact on studies of magnetic field effects during the break-up of strongly-driven multi-centre molecules. It will also allow to perform studies of magnetic field effects on non-sequential double ionization, which have never been performed before. 
 
Title Quantum mechanical method for obtaining countinuum orbitals in molecules 
Description We produced in my group a previously developed (by another group) model for obtaining continuum orbitals in molecules. This will allow us to compute Auger rates in molecules and thus study Free-Electron Laser (FEL) processes in molecular systems 
Type Of Material Computer model/algorithm 
Provided To Others? No  
Impact In the future it will allow us to study FEL processes in molecules 
 
Title Qunatum-mechanical tool for FEL-driven atoms 
Description We have developed a set of quantum mechanical tools to describe the interaction of Free-Electron Lasers with complex atoms. 
Type Of Material Computer model/algorithm 
Provided To Others? No  
Impact papers and invitations to conferences 
 
Title Semiclassical Toolkit for strongly-driven molecules 
Description We developed a semiclassical set of tools to describe in three-dimensions the break-up of molecules driven by intense and infrared laser pulses 
Type Of Material Computer model/algorithm 
Year Produced 2014 
Provided To Others? Yes  
Impact papers and invitations to conferences 
 
Title Semiclassical tool and method to account for non-dipole effects in strongly-driven molecules 
Description The last few months we have developed a new theoretical and computational tool to account for magnetic field effects in molecules driven by intense laser fields. This new tool will have big impact in the attoscience and strong field community since almost all studies up to now do not include magnetic field effects. 
Type Of Material Computer model/algorithm 
Year Produced 2019 
Provided To Others? No  
Impact This theoretical and computational tool we have developed in 2020, we will soon be published in an appropriate journal to effectively disseminate the results. We will use this technique to perform ground-breaking studies of magnetic field effects during the break-up of strongly-driven diatomic and triatomic molecules. 
 
Description Ionization in multi-electron atoms and molecules by intense laser pulses 
Organisation National Research Council of Canada
Country Canada 
Sector Public 
PI Contribution My collaboration with experimentalists Prof. P.B. Corkum and A.Staudte has resulted in four publications
Collaborator Contribution Provide experimental feedback on strongly-driven processes in atoms and molecules
Impact 4 co-authored papers
Start Year 2009
 
Description LMU Munich 
Organisation Ludwig Maximilian University of Munich (LMU Munich)
Country Germany 
Sector Academic/University 
PI Contribution We provided the theory for non-sequential double ionization of Ar for a range of intensities triggered by near-single cycle pulses. This collaboration resulted in 1 publication. In addition, we have collaborated on identifying a new mechanism of non-sequential double ionization for low intensities. Mainly we have identified the slingshot non-sequential double ionization, where two electrons escape opposite to each other. The main reason for the anti-correlation pattern is that one electron undergoes a slingshot motion around the nucleus as is the case in the gravitational slingshot motion of a spacecraft. The nucleus assists the electron in escaping in conjunction to the laser field. That is the change in momentum is in the same direction as the force from the field thus resulting in the electron absorbing the energy needed to escape.
Collaborator Contribution The group of Prof. M. F. Kling provided the experimental results for the above project. Moreover, in the second project Prof. M. Kling and B. Bergues contributed to formulating the new mechanism of non-sequential double ionization.
Impact This collaboration resulted in a very accurate theoretical description of the ultra-fast phenomena underlying non-sequential double ionization in atoms triggered by ultra-short laser pulses and the theory we provided explained very well the experimental results of Prof. M. F. Kling. Moreover, this collaboration resulted in identifying and formulating a new mechanism in strong field physics, namely, slingshot non-sequential double ionization which is the analog of the gravitational slingshot motion in strong field physics.
Start Year 2017
 
Description National Research Council in Ottawa and University of Ottawa 
Organisation National Research Council - Ottawa
Country Canada 
Sector Public 
PI Contribution My team was the main contributor in a collaboration with experimentalist Prof. P. B Corkum that resulted to the identification of a new non-dipole effect in non-sequential double ionization of strongly-driven He, namely, to non-dipole re-collision gated ionization In 2018, we collaborated with the group of Prof. Paul Corkum and Dr. Andre Staudte to control double ionization of Ar. To do so, we employed two-colour laser fields, one at 800 nm and the other at 2400 nm.
Collaborator Contribution Prof. P. B. Corkum discussed with me the signatures of non-dipole effects in single ionization of atoms which his attoscience experimental group has identified in 2011, and then we were then able to investigate new effects in double ionization of atoms. In 2019, my experimental collaborators have provided the experiments for strongly-driven Ar by two-colour laser fields, while my group has provided the theory. The work from this latter project has resulted in a publication where we identify how to streak the ionization times of two electrons in double ionization when Ar is strongly driven by a two-colour laser field.
Impact This collaboration has resulted in the identification of a new non-dipole effect and the publication of two journal papers. The collaboration is multi-disciplinary in the sense that Prof. Corkum is an experimentalist in the field of attoscience and my group is a theoretical and computational group in attosecond and strong-field science. Our joint work in 2018,. will result in an experimental scheme of identifying the ionization time of electrons in non-sequential double ionization of atoms driven by intense fields.
Start Year 2008
 
Description Open to the public talk for Attoscience by P.B. Corkum 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? Yes
Geographic Reach International
Primary Audience Public/other audiences
Results and Impact 100 people attended the talk on Attoscience

Undergraduate students contacted me to do a research project with me over the summer at UCL.
Year(s) Of Engagement Activity 2014
 
Description Seminar Series : Frontiers of Ultafast Science UK 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach National
Primary Audience Other audiences
Results and Impact Starting in 2017, I have initiated a seminar series "Frontiers of Ultafast Science UK". This seminar series takes place in different Institutions and Universities across the UK. Up to now I have organised 5 such seminars up to now. The goal is to bring together scientists working in different ultrafast-science fields such as, atomic and molecular physics, condensed matter physics, quantum optics, ultrafast chemistry and so on.
Year(s) Of Engagement Activity 2017,2018,2019,2020