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P. Bucksbaum

Publications and source records attributed to P. Bucksbaum.

3 recordsLinked to original sources
arXiv2016

Probing ultrafast \pi\pi*/n\pi* internal conversion in organic chromophores via K-edge resonant absorption

Organic chromophores with heteroatoms possess an important excited state relaxation channel from an optically allowed {\pi}{\pi}* to a dark n{\pi}*state. We exploit the element and site specificity of soft x-ray absorption spectroscopy to selectively follow the electronic change during the {\pi}{\pi}*/n{\pi}* internal conversion. As a hole forms in the n orbital during {\pi}{\pi}*/n{\pi}* internal conversion, the near edge x-ray absorption fine structure (NEXAFS) spectrum at the heteroatom K-edge exhibits an additional resonance. We demonstrate the concept with the nucleobase thymine, a prototypical heteroatomic chromophore. With the help of time resolved NEXAFS spectroscopy at the oxygen K-edge, we unambiguously show that {\pi}{\pi}*/n{\pi}* internal conversion takes place within (60 \pm 30) fs. High-level coupled cluster calculations on the isolated molecules used in the experiment confirm the superb electronic structure sensitivity of this new method for excited state investigations.

physics.chem-ph↗
arXiv2014

Transient Impulsive Giant Electronic Raman Redistribution

Resonant Raman excitation by ultrafast vacuum ultraviolet laser pulses is a powerful means to study electron dynamics in molecules, but experiments must contend with linear background ionization: frequencies high enough to reach resonant core-valence transitions will usually ionize all occupied orbitals as well, and the ionization cross sections are usually dominant. Here we show that attosecond pulses can induce a process, transient impulsive stimulated Raman scattering, which can overwhelm valence ionization. Calculations are performed for atomic sodium, but the principal is valid for many molecular systems. This approach opens the path for high fidelity multidimensional spectroscopy with attosecond pulses.

physics.chem-ph↗
arXiv2010

Teravolt-per-meter plasma wakefields from low-charge, femtosecond electron beams

Recent initiatives in ultra-short, GeV electron beam generation have focused on achieving sub-fs pulses for driving X-ray free-electron lasers (FELs) in single-spike mode. This scheme employs very low charge beams, which may allow existing FEL injectors to produce few-100 as pulses, with high brightness. Towards this end, recent experiments at SLAC have produced ~2 fs rms, low transverse emittance, 20 pC electron pulses. Here we examine use of such pulses to excite plasma wakefields exceeding 1 TV/m. We present a focusing scheme capable of producing ~200 nm beam sizes, where the surface Coulomb fields are also ~TV/m. These conditions access a new regime for high field atomic physics, allowing frontier experiments, including sub-fs plasma formation for wake excitation.

physics.plasm-ph↗