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Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales…
We demonstrate the breakdown of molecular-frame dynamics induced by the uncoupling of molecular rotation from electronic motion in molecular Rydberg states. We observe this non-Born-Oppenheimer regime in the time domain through…
The temporal evolution of an atomic wave packet interacting with object and reference electromagnetic waves is investigated beyond the weak perturbation of the initial state. It is shown that the diffraction of an ultracold atomic beam by…
We observe and control a molecular vibrational wave packet in an electronically excited state of the neutral hydrogen molecule. In an extreme-ultraviolet (XUV) transient-absorption experiment we launch a vibrational wave packet in the $D…
We report the optical imaging of a single atom with nanometer resolution using an adaptive optical alignment technique that is applicable to general optical microscopy. By decomposing the image of a single laser-cooled atom, we identify and…
We show that two-particle interferences can be used to probe the nuclear motion in a doubly-excited hydrogen molecule. The dissociation of molecular hydrogen by electron impact involves several decay channels, associated to different…
We report optical absorption imaging of ultracold neutral plasmas.Images are used to measure the ion absorption spectrum, which is Doppler-broadened. Through the spectral width, we monitor ion equilibration in the first 250ns after plasma…
Established x-ray diffraction methods allow for high-resolution structure determination of crystals, crystallized protein structures or even single molecules. While these techniques rely on coherent scattering, incoherent processes like…
We measure molecular vibrations with femtometer precision using time-resolved x-ray absorption spectroscopy. For a demonstration, a Raman process excites the A$_{1g}$ mode in gas-phase SF$_6$ molecules with an amplitude of $\approx50$ fm,…
The two-dimensional spectroscopy has recently revealed oscillatory behavior of excitation dynamics in molecular systems. However, in the majority of cases it is strongly debated if excitonic or vibrational wavepackets, or evidences of…
We report absolute frequency measurements of 81 hyperfine components of the rovibrational transitions of molecular iodine at 578 nm using the second harmonic generation of an 1156-nm external-cavity diode laser and a fiber-based optical…
Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. We present the direct experimental recording of very-high-resolution and -fidelity molecular…
This study introduces a novel method to investigate in-situ light transport within optically thick ensembles of cold atoms, exploiting the internal structure of alkaline-earth metals. A method for creating an optical excitation at the…
Control over various fragmentation reactions of a series of polyatomic molecules (acetylene, ethylene, 1,3-butadiene) by the optical waveform of intense few-cycle laser pulses is demonstrated experimentally. We show both experimentally and…
The chemical and physical properties of molecular clusters can heavily depend on their size, which makes them very attractive for the design of new materials with tailored properties. Deriving the structure and dynamics of clusters is…
A model based on the strong-field and Born-Oppenheimer approximations qualitatively describes the distribution over vibrational states formed in a diatomic molecular ion following ionization of the neutral molecule by intense laser pulses.…
Ultrafast processes in matter, such as the electron emission following light absorption, can now be studied using ultrashort light pulses of attosecond duration ($10^{-18}$s) in the extreme ultraviolet spectral range. The lack of spectral…
Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…
Among polycyclic aromatic hydrocarbons, pyrene is widely used as an optical probe thanks to peculiar ultraviolet absorption and infrared emission features. Interestingly, this molecule is also an abundant component of the interstellar…
The time-dependent Schr\"{o}dinger equation for the hydrogen atom and its interaction with coherent intense high-frequency short laser pulses is solved numerically exactly by propagating the single-electron wave packets. Thereby, the…