Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. Although strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, because of the lack of pulse-shaping technologies in the extreme ultraviolet (XUV) and X-ray domain.
View Article and Find Full Text PDFWe present a method for the reconstruction of ion kinetic energy distributions from ion time-of-flight mass spectra through ion trajectory simulations. In particular, this method is applicable to complicated spectrometer geometries with largely anisotropic ion collection efficiencies. A calibration procedure using a single ion mass peak allows the accurate determination of parameters related to the spectrometer calibration, experimental alignment, and instrument response function, which improves the agreement between simulations and experiment.
View Article and Find Full Text PDFCareful control of quantum states is a gateway to research in many areas of science such as quantum information, quantum-controlled chemistry, and astrophysical processes. Precise optical control of molecular ions remains a challenge due to the scarcity of suitable level schemes, and direct laser cooling has not yet been achieved for either positive or negative molecular ions. Using a cryogenic wire trap, we show how the internal quantum states of C_{2}^{-} anions can be manipulated using optical pumping and inelastic quenching collisions with H_{2} gas.
View Article and Find Full Text PDFIn the literature, the chemi-ionization of Li in the 2S ground level by He in a metastable state is typically described as an electron transfer process in which an electron from the 2s orbital of Li is transferred to the 1s orbital of He while an electron from the 2s orbital of He is ejected. Therefore, one would not assume that the orbital of the valence electron of He strongly influences the coupling strength of the collision complex to the ionization continuum. However, we observe that the chemi-ionization rate is decreased when He is laser-excited from the metastable 2S level to the 2P level (with = 0, 1, 2).
View Article and Find Full Text PDFFemtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. A setup for phase modulation spectroscopy is used to probe the 3S-2P transition in an 800K-cold sample of Li atoms confined in a magneto-optical trap. The observation of a double quantum coherence response, a signature of interparticle interactions, paves the way for detailed investigations of few- and many-body effects in ultracold gases using this technique.
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