Photoelectron interferometry with femtosecond and attosecond light pulses is a powerful probe of the fast electron wave-packet dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain both high temporal and spectral resolution by stimulating Raman interferences with one light pulse and monitoring the modification of the electron yield in a separate step. Applying this spectroscopic approach to the autoionizing states of argon, we experimentally resolved its electronic composition and time evolution in exquisite detail. Theoretical calculations show remarkable agreement with the observations and shed light on the light-matter interaction parameters. Using appropriate Raman probing and delayed detection steps, this technique enables highly sensitive probing and control of electron dynamics in complex systems.
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http://dx.doi.org/10.1103/PhysRevLett.128.083001 | DOI Listing |
J Phys Chem A
December 2024
Radboud University Nijmegen, Institute for Molecules and Materials, Heijendaalseweg 135, 6525 AJ Nijmegen, The Netherlands.
In molecular beam scattering experiments, an important technique for measuring product energy and angular distributions is velocity map imaging following photoionization of one or more scattered species. For studies with cold molecular beams, the ultimate resolution of such a study is often limited by the product detection process. When state-selective ionization detection is used, excess energy from the ionization step can transfer to kinetic energy in the target molecular ion-electron pair, resulting in measurable cation recoil.
View Article and Find Full Text PDFPhys Rev Lett
October 2024
Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, 14195 Berlin, Germany.
Several diatomic transition metal oxides, rare-earth metal oxides, and fluorides have the unusual property that their bond dissociation energy is larger than their ionization energy. In these molecules, bound levels above the ionization energy can be populated via strong, resonant transitions from the ground state. The only relevant decay channel of these levels is autoionization; predissociation is energetically not possible and radiative decay is many orders of magnitude slower.
View Article and Find Full Text PDFPhys Rev Lett
September 2024
Laboratoire Kastler Brossel, Collège de France, CNRS, ENS-Université PSL, Sorbonne Université, 11, place Marcelin Berthelot, 75005 Paris, France.
Rydberg alkaline earth atoms are promising tools for quantum simulation and metrology. When one of the two valence electrons is promoted to long-lived circular states, the second valence electron can be optically manipulated without significant autoionization. We harness this feature to demonstrate laser slowing of a thermal atomic beam of circular strontium atoms.
View Article and Find Full Text PDFPhys Rev Lett
September 2024
5. Physikalisches Institut and Center for Integrated Quantum Science and Technology, Universität Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany.
J Chem Phys
June 2024
Department of Nuclear and Atomic Physics, Tata Institute of Fundamental Research, Dr. Homi Bhabha Road, Colaba, Mumbai 400005, India.
We present an experimental study of multiple-electron capture-induced fragmentation dynamics of Ar2m+ (4 ≤m≤ 7) dimer ions in 4 keV/u Ar8+-Ar2 collisions. The fragment recoil ion pairs and the charge-changing projectiles are coincidentally measured using a double coincidence technique. The branching ratios between the different charge-sharing fragmentation channels show an inherent enhancement of the asymmetric channels.
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