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Synopsis
Attosecond pulses are produced by nonlinear-optical high-harmonic generation of focused few-cycle phase-stabilized femtosecond laser light in a rare gas target. These pulses are used to illuminate the quantum dynamics and correlated motion of electrons in various systems, including atoms, molecules, clusters and nanoparticles.
See also: Leone group, attosecond dynamics in atoms/molecules and semiconductors
Molecules studied:
atoms (He, Kr, Xe), diatomics (N2, IBr, O2), fundamental organic systems (alkyl bromides and iodides), and solid materials (Si, Ge)
Information obtained:
Time-resolved wavefunctions of electrons
Project members:
Dylan Cleveland
Josh Edwards
John Hack
Patrick Rupprecht
Recent publications:
"Coherent vibrational dynamics in molecular bond breaking: Methyl radical umbrella mode probed by femtosecond x-ray spectroscopy" C. A. Schröder, J. H. Hack, J. L. Edwards, Z. Zhang, J. T. Kenyon, Q. Wang, H. Wang, D. M. Neumark, S. R. Leone, Phys. Rev. Research, 8, L022033 (2026). pdf
"All-optical logic gates for extreme ultraviolet switching via attosecond four-wave mixing" P. Rupprecht, D. M. Neumark, S. R. Leone, Opt. Express, 34, 4079–4091 (2026). pdf
"Tracing long-lived atomic coherences generated via molecular conical intersections" P. Rupprecht, F. Montorsi, L. Xu, N. G. Puskar, M. Garavelli, S. Mukamel, N. Govind, D. M. Neumark, D. Keefer, S. R. Leone, Phys. Rev. Lett., 135, 233201 (2025). pdf
"Probing autoionization decay lifetimes of the 4d−16ℓ core-excited states in xenon using attosecond noncollinear four-wave-mixing spectroscopy" N. G. Puskar, P. Rupprecht, J. Dvořák, Y.-C. Lin, A. E. Greene, R. R. Lucchese, C. W. McCurdy, S. R. Leone, D. M. Neumark, J. Chem. Phys., 163, 184302 (2025). pdf
"Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy" P. Rupprecht, N. G. Puskar, D. M. Neumark, S. R. Leone, Phys. Rev. Research, 6, 043100 (2024). pdf
"Femtosecond symmetry breaking and coherent relaxation of methane cations via x-ray spectroscopy" E. Ridente, D. Hait, E. A. Haugen, A. D. Ross, D. M. Neumark, M. Head-Gordon, S. R. Leone, Science, 380, 713–717 (2023). pdf
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