Wave packet dynamics in atoms and molecules Eva Heesel Corinne Glendinning Helen Fielding Department of Chemistry University College London UCL Progress.

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Presentation transcript:

Wave packet dynamics in atoms and molecules Eva Heesel Corinne Glendinning Helen Fielding Department of Chemistry University College London UCL Progress Report at RAL Attomeeting on

Interferometer Stabilisation program completed Breadboard under investigation Ramsey Fringe Experiment Filter for wavelength selection under way Need kHz gas jet, TOF chamber, full beam line Can generate high-order harmonics from each interferometer beam + observe fringes (XUV SPIDER - Oxford report). Can also characterise bandwidth. Interferometer and Ramsey Fringes

Krypton experiment (Corinne) Use time-resolved photoelectron spectroscopy to look at low n Rydberg states Excitation of Kr + 4s 2 4p 5 ( 2 P 3/2 ) 6s, 7s and 5d Rydberg states from the ground state via 5p intermediate A VUV pulse will then ionise the Kr core further or ionise the Rydberg electron Relate different core excitations to core- Rydberg electron distances Double ionisation of Kr core – opportunity to study the dynamics of the Rydberg electron in the presence of a doubly charged core If photoelectrons are detected by imaging, the l- character of the Rydberg states can be reconstructed

Energy (eV) Kr + 4s 2 4p 5 ( 2 P 3/2 ) 5p 2[3/2] J= Kr + ( 2 P 3/2 ) LIMIT Kr + 4s 2 4p 5 ( 2 P 3/2 ) 5d 2[7/2] J=3 ; 2[3/2] J=2,1 ; 2[5/2] J=2,3 Kr + 4s 2 4p 5 ( 2 P 1/2 ) 6s 2[1/2] J=1 ; Kr + 4s 2 4p 5 ( 2 P 3/2 ) 7s 2[3/2] J=2,1 (range eV) Kr + ( 2 P 1/2 ) LIMIT Kr ++ ( 3 P 2,1,0 ) LIMITS , , Kr ++ ( 1 D 2 ) LIMIT Kr ++ ( 1 S 0 ) LIMIT S01S0 Kr ++ 4s4p 5 ( 3 P 2,1,0 ) LIMITS , , Kr ++ (4s 2 4p 3 4 S)4d ( 5 D 0,1,2,3,4 ) LIMITS , , , , Kr ++ 4s4p 5 ( 1 P 1 ) LIMIT nm 800 nm VUV ~6 fs OPA HHG Kr Energy levels

Two-stage plan for Kr experiment At UCL: Measure frequency-resolved spectrum Narrowband: Use ns beams: 214 nm and 800 nm Can do experiment both field-free and with static field (Stark splitting) Photoionise Rydberg states with 400/800 nm photon Field-free: apply field with 20 ns rise time to extract ions With static field: investigate Stark shifts (good test for imaging) (detect electrons) At IC: Measure electron dynamics + image photoelectrons Use 214 nm ns beam (OPO) and 200 nm fs beam (FHG from few-cycle pulse) Need static field for imaging.

Benzene experiment (Eva) Monitor ultrafast dynamics of benzene molecule using time- resolved photoelectron spectroscopy Excitation of benzene molecules from the ground state S 0 to the S 2 state with 200 nm photons (pulse duration as short as possible) The S 2 state decays very fast (< 50 fs) by internal conversion to high vibrational levels of the S 1 and S 0 states. Time-delayed probe photon (~ eV) can ionise populations from all electronic states: Detect photoelectrons with different kinetic energy Energy resolution given by a) pulse duration (bandwidth) eV for 5 fs pulse b) resolution of photoelectron spectrometer (1%)

Benzene Energy levels S0S0 S1S1 S2S2 I.P. Energy (eV) 200 nm (6.2 eV) VUV (e.g eV) VUV probe has the advantage of being able to ionise all intermediates and products

Plans/work in progress Generation/Characterisation of 200 nm –Generation: Fourth-harmonic of 800 nm –Characterisation: cross-correlation, two-photon ionisation,…. Calculations –Mike’s Robb group (IC chemistry) –Wave packet moves through conical intersection