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Overview of New Programme Grant

Overview of New Programme Grant. A 6 Year Programme Commencing ~ June 2011 It will be the main (but not the only) activity within the Consortium over this period. It unifies the current activities in Attosecond Technology, HHG Spectroscopy, Multi-Colour Control, Molecular Dynamics & Theory.

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Overview of New Programme Grant

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  1. Overview of New Programme Grant A 6 Year Programme Commencing ~ June 2011 It will be the main (but not the only) activity within the Consortium over this period. It unifies the current activities in Attosecond Technology, HHG Spectroscopy, Multi-Colour Control, Molecular Dynamics & Theory.

  2. Overview of Science Objectives The programme, comprising four interlinked projects, will exploit two new types of measurements that we have already begun to develop: high harmonic generation (HHG) spectroscopy (project 1)and attosecondpump-probe spectroscopy (project 2), and will apply them to the measurement of attosecond electron dynamics in large molecules (project 3) and the condensed phase (project 4). This programme ultimately will: Address the coupling of charge migration to chemistry We will address, in experiments and theory on prototypical molecular systems, the coupling of coherent electron excitation to the pathways of chemical change. Observe the evolution of hole states in matter We will conduct time-domain measurements in molecules and condensed phase systems to probe the propagation of holes and observe their evolution, delocalisation and decay on unprecedented time scales. Understand electron transport in biomolecules We will apply our techniques to discovering the mechanisms of charge migration in the building blocks of biomolecules in order to understand the fastest timescales of the electronic energy transport vital to the functioning of all living systems.

  3. Project 1: HHG Spectroscopy 1a extend our PACER structural imaging technique to image nuclear re-arrangements induced by localized hole excitations at the time-scales from 0.5 fsec to 4-5 fsec; 1b use strong-field ionization to create localized hole excitations and study their attosecond dynamics in polyatomic molecules; 1c achieve selective imaging of hole dynamics induced by the removal of e.g. inner-valence electrons using the XUV initiated HHG technique; 1d develop multi-dimensional HHG spectroscopy capable of following energy flow between different molecular modes over multiple fsec time-scale;

  4. Project 2: Attosecondpump-probe spectroscopy 2a development of a high-power ~1 fs VUV source to directly, and selectively, excite specific chromophores; 2b generation of isolated attosecond pulses extending to the carbon K-edge for initiating inner shell dynamics and performing time resolved soft X-ray spectroscopy; 2c pioneer attosecond X-ray absorption techniques for gas and condensed phase systems; 2d break new ground in attosecond XUV photoelectron spectroscopy of isolated molecules.

  5. Project 3: Coupling of charge migration and nuclear dynamics 3a develop single-ionization ADC(3) theory for the solution of the time-dependent electronic Schroedinger equation and the energy gradients needed for classical nuclear dynamics; 3b develop the CASSCFEhrenfest dynamics code to include the ionised molecular state as an initial condition; 3c measure the effects of charge migration using ~ 1fs resolution chromophore specific VUV pump + IR-field probe, and VUV pump + XUV probe in medium-sized organic molecules and in biomolecular building blocks; 3d measure the effects of charge migration using an Auger marker method to start localized site-specific dynamics.

  6. Project 4: Probing attosecond dynamics in the condensed phase 4a demonstrate attosecond transient absorption spectroscopy in the condensed phase; 4b introduce and exploit new high transmission and low-dispersion micro and nanoscale targets for attosecond science; 4c develop high harmonic spectroscopy on surfaces; 4d test and exploit ‘infrared-field-streaked’ nonlinear spectroscopy in bulk.

  7. June 2011 June 2017

  8. Frasinski Frasinski

  9. Priorities for Science Programme over next 18 months • HHG from larger molecules using the mid-IR OPG sources (coupled to heated jet and ablation plume techniques) • Develop “phase” measurements for molecular HHG (including MQPI & RABBITT) • Demonstration of XUV initiated HHG in atoms • Development of sub-fs 10-20eV source • Gas phase absorption based attosecond pump-probe spectroscopy • Continuing development of attosecond source • Surface HHG studies (including in nanoplasmonic arrays) • Commissioning of electron VMI and molecular beam • Propagation included in molecular HHG codes

  10. Enabling technical developments over the next year • Red Dragon energy up-grade to ~10 mJ/pulse • Installation of HE TOPAS OPG for ~40 fs mid-IR pulses • Completion of few-cycle DFG-OPG (extra £18 k promised by College for this) • Energy up-grade of Femtolaser to ~ 4mJ/pulse • Robust ablation plume rig for fullerenes, nanoparticles and larger molecules

  11. Next Steps • Kick off meeting in early June • Appointment of Postdocs by middle of year • Arranging tenders for laser up-grades etc. • Discussions with all members of the Consortium about their roles

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