Iodine Molecular Interferometer and Inversion Symmetry Mat Leonard Molecular Structure o Properties of electronic wave functions describe molecular structure o symmetry o spatial extent o localization
o energy eigenvalues o Traditional photoelectron spectroscopy focused on energy levels o Time-resolved photoelectron imaging allows insight into other properties of electron wave functions Davis I2 Experiment - o Time-resolved photoelectron spectrum of I2- experiment (Davis, et al J. Chem.
Phys. 118, 999 (2003)) o Ti:Sapphire laser, 90 fs pulses o Pump with IR, probe with 3h o Velocity Map Imaging Photoelectron Energy SpectrumProbe only o From energy conservation, photoelectron energy spectrum reveals information
about molecular states Time-Resolved Photoelectron Energy Probe only Spectrum Pump + Probe Photoelectron Angular Distribution Interesting information lies in the photoelectron angular distribution (PAD)
The PAD can be represented by: where, is the angle between the electron velocity and laser polarization vectors, 2nn is the anisotropy parameter associated with P2nn, the nth Legendre polynomial PAD Anisotropy o 2n varies in time, even after
dissociation is complete (~300 fs) o Increase in 2n after 350 fs is attributed to a shallow well in the long range potential o Decrease suggested to be related to localization of electron o |4|<0.1, negligibly small and no time dependence is observed Electron Localization
o Localization occurs due to mixing of g and u states (gerade and ungerade refer to states being even or odd under inversion, respectively) o In the absence of an external field, the overall electron wave function is of the the form (IA-IB + IAIB-) o The wave functions for localization on a particular I atom, i.e. IA-IB or IAIB-, are obtained from linear combinations
of g u states o External extraction field of 500 V/cm can induce the g/u mixing Sanov I2 Experiment - o Time-resolved photoelectron spectrum of I2- experiment (Sanov, et al J. Chem. Phys. 123, 054329 (2005))
o Ti:Sapphire laser, 100 fs pulses o Pump with IR, probe with 2h o Extraction field ~40-80 V/cm PAD Anisotropy Again, fitting the measured PADs to we see 2n change long after the dissociation is complete (~500 fs) Complete oscillation of the anisotropy
parameter in ~2.5 ps, R35 I2- Molecular Interferometer o Photoelectron with KE=0.12 eV has de Broglie wavelength =35.4 o Effective state mixing occurs when the field induced perturbation H=eER is comparable to the energy separation of the two unperturbed potential-energy curves
o Electron localization estimated at R35.6 , corresponding to ~2.5 ps delay o 2n varies as R(t)/, as expected for double source interference
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