Lund University From Rydberg to Atto physic Is matter a wave ?

Lund University Big Bang 1897/ 1911 Joseph John Thomson: Characterization of the electron as an elementary particle Max Planck: Explication of the Black body radiation - Planck constant Albert Einstein: Explication of the Photoelectric effect Ernest Rutherford : Discovery of nucleus 1884/ 1888 Johan Jakob Balmer & Johannes Rydberg: Discrete spectral lines in vapour lamp

Lund University Big Bang 1897/ 1911 Louis de Broglie: Wave-particle duality Werner Heisenberg: uncertainty principle Rudolf Schrödinger: Quantum mechanics Wolgan Pauli: Exclusion principle Paul Dirac: Relativistic Quantum mechanics Niels Bohr: First atomic model Joseph John Thomson / Max Planck / Albert Einstein Ernest Rutherford 1884/ 1888 Johan Jakob Balmer / Johannes Rydberg / 19

Lund University Modern theory Atoms,Molecules,Solid,Surface 2010 Experiences on atoms 1950 Experiences on molecules Experiences on surface Laser visible (CW, ns, ps, fs) Synchrotron X-ray (ns, ps) XUV X-ray (fs, as) Experiences on nano Louis de Broglie Werner Heisenberg Rudolf Schrodinger Wolgan Pauli Paul Dirac Louis de Broglie Werner Heisenberg Rudolf Schrodinger Wolgan Pauli Paul Dirac

Lund University Natural time scale

Lund University Dynamics in real time To capture a moving object we need... an exposure time /shutter faster than the motion ! Stroboscope Sequential

Lund University Electron dynamics – attosecond timescale electron XUV source with temporal coherence ion +  t 2 eV Heisenberg uncertainties

Lund University step-wise direct Photoionization dynamics 1 photon 2 photon direct step-wise Because everything is a wave, we can assign a phase to everything… Interference between different ionization pathways arise from phase differences

Lund University Experimental background

Lund University Harmonic generation in a gas generation Gas (Ar) focusing optic 4 mJ, 35 fs 800 nm Ti:Saph Attosecond pulses filter wheel

Lund University Harmonic generation in a gas Corkum and Krausz, Nature physics 3, 381 (2007)

Lund University Harmonics : Attosecond pulse trains coupled, well-known phase! Filtering one-two harmonics  100 meV bandwidth/harmonic  fs timescale Without filtering  eV bandwidth  260 as/pulse

Lund University Pump-Probe experiments IR Probe focusing mirror recombination mirror delay stage <30nm 4 mJ, 35 fs 800 nm Ti:Saph Electron detection XUV Pump

Lund University Ionization with Harmonics + IR probe IpIp harmonics IR probe sidebands It is complicated… XUV pump mainlines

Lund University Ionization in valence shell

Lund University Helium ionization Harmonic order Delay (fs) IpIp harmonics He + h H19-H27  He + + e - (  s  ) + h IR  d 1D Electron spectrometer Paul et al., Science (2001) RABITT

Lund University Helium ionization Delay (fs) Freq. Amplitude DC comp. 2w FT(  ) He + h H19-H21  He + + e - (  s  ) + h IR  d FT(  )

Lund University Helium ionization Amplitude DC comp. 2w FT(  ) He + h H19-H21  He + + e - (  s  ) + h IR  d Argon Helium  offset (rad) Helium 3p Helium 1s What is happening? Harmonic 15 Harmonic 17

Lund University What do we measure? i kaka k Measured: XUV + IR ionization 1 keke Measured: XUV

Lund University Resonant ionization of helium tuning to red Ionization threshold Swodoba et al. Phys Rev Lett 104, (2010)

Lund University Ionization in valence and inner valence shells

Lund University Unbound states free particle: with r E potential present: shift δ with respect to free particle δ carries information about core region

Lund University δ for different potentials short range potential: V=0, r > r 0 matching conditions real potential:, r > r 0 0 V r0r0 r => 0 V r0r0 r scattering phase

Lund University Scattering phase and photoemission time delay One-Photon ionization: phase of complex amplitude is scattering phase Group delay of an electron wave packet during photoemission optics: pulse propagationelectron propagation: Wigner time delay 1s k

Lund University Measurement principle Ar S modulated with harmonic-IR delay:

Lund University What do we measure? i kaka k keke Wigner time delay Interference: Measured: XUV + IR ionization

Lund University Compare experiment and approximation Wigner time delay Continuum- continuum contribution Approximation Experiment