Quantum Beat Photoelectron Imaging Spectroscopy of Xe in the VUV

Quantum Beat Photoelectron Imaging Spectroscopy of Xe in the VUV

New on arXiv

Time-resolved pump-probe measurements of Xe, pumped at 133~nm and probed at 266~nm, are presented. The pump pulse prepared a long-lived hyperfine wavepacket, in the Xe 5p5(2P1/2)6s 2[1/2]1 manifold (E=77185 cm1=9.57 eV). The wavepacket was monitored via single-photon ionization, and photoelectron images measured. The images provide angle- and time-resolved data which, when obtained over a large time-window (900~ps), constitute a precision quantum beat spectroscopy measurement of the hyperfine state splittings. Additionally, analysis of the full photoelectron image stack provides a quantum beat imaging modality, in which the Fourier components of the photoelectron images correlated with specific beat components can be obtained. This may also permit the extraction of isotope-resolved photoelectron images in the frequency domain, in cases where nuclear spins (hence beat components) can be uniquely assigned to specific isotopes (as herein), and also provides phase information. The information content of both raw, and inverted, image stacks is investigated, suggesting the utility of the Fourier analysis methodology in cases where images cannot be inverted.

Also available on Authorea.

Full data, code & analysis notes on OSF.

Bootstrapping (Ultrafast) Photoionization Dynamics – PQE 2018 (extended) video

Bootstrapping (Ultrafast) Photoionization Dynamics – PQE 2018 (extended) video

Bootstrapping (Ultrafast) Photoionization Dynamics – PQE 2018 (extended) from femtolab.ca on Vimeo.

Talk originally given as a 20min presentation at PQE 2018 (Snowbird, Utah, http://pqeconference.com/pqe2018/program). The original talk was not recorded; this is an extended version using the same slides, but with rather more introductory discussion. The abstract is given below, along with links to additional material.

More details of the work discussed in the main part of the talk can be found in:
Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry.
Marceau et. al., Physical Review Letters, 119(8), 83401 (2017).
http://doi.org/10.1103/PhysRevLett.119.083401

PQE 2018 Abstract

Bootstrapping (Ultrafast) Photoionization Dynamics
Slot: Tuesday Morning Invited Session 1
Session: Ultrafast photoionization dynamics

Photoionization is an interferometric process, in which multiple paths can contribute to the final continuum photoelectron state. At the simplest level, interferences between different final angular momentum states are clearly manifest in the energy and angle resolved photoelectron spectra; metrology schemes making use of these interferograms are thus phase-sensitive, and provide a powerful route to detailed understanding of photoionization.

The high information content of angle-resolved interferograms, combined with geometric control over the photoionization dynamics, can provide sufficient data for reconstruction of the continuum state, in terms of the constituent partial waves and phases. This has recently been explored for a range of cases, including the use of ultrafast pump-probe schemes with a bootstrapping analysis methodology: aspects of this work will be presented.

DOI: 10.6084/m9.figshare.5645509

Refs
Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry
Marceau, C., Makhija, V., Platzer, D., Naumov, A. Y., Corkum, P. B., Stolow, A., Villeneuve, D. M., Hockett, P. (2017). Physical Review Letters, 119(8), 83401. http://doi.org/10.1103/PhysRevLett.119.083401

Coherent control of photoelectron wavepacket angular interferograms.
Hockett, P., Wollenhaupt, M., & Baumert, T. (2015). Journal of Physics B: Atomic, Molecular and Optical Physics, 48(21), 214004. http://doi.org/10.1088/0953-4075/48/21/214004

Complete Photoionization Experiments via Ultrafast Coherent Control with Polarization Multiplexing.
Hockett, P., Wollenhaupt, M., Lux, C., & Baumert, T. (2014). Physical Review Letters, 112(22), 223001. http://doi.org/10.1103/PhysRevLett.112.223001

Coherent imaging of an attosecond electron wave packet.
Villeneuve, D. M., Hockett, P., Vrakking, M. J. J., & Niikura, H. (2017). Science, 356(6343), 1150–1153. http://doi.org/10.1126/science.aam8393