arXiv subjects

F. Stienkemeier

Publications and source records attributed to F. Stienkemeier.

At least 37 records · Page 2Linked to original sources

arXiv2015

Enhanced ionization of embedded clusters by Electron Transfer Mediated Decay in helium nanodroplets

Here, we report the observation of electron transfer mediated decay (ETMD) involving Mg clusters embedded in helium nanodroplets which is initiated by the ionization of helium followed by removal of two electrons from the Mg clusters of which one is transferred to the He environment neutralizing it while the other electron is emitted into the continuum. The process is shown to be the dominant ionization mechanism for embedded clusters for photon energies above the ionization potential of He. The photoelectron spectrum reveals a low energy ETMD peak. For Mg clusters larger than 5 atoms we observe stable doubly-ionized clusters. We argue that ETMD provides a new pathway to the formation of doubly-ionized cold species.

physics.chem-ph↗

arXiv2015

Predissociation dynamics of lithium iodide

The predissociation dynamics of lithium iodide (LiI) in the first excited A-state is investigated for molecules in the gas phase and embedded in helium nanodroplets, using femtosecond pump-probe photoionization spectroscopy. In the gas phase, the transient Li+ and LiI+ ion signals feature damped oscillations due to the excitation and decay of a vibrational wave packet. Based on high-level ab initio calculations of the electronic structure of LiI and simulations of the wave packet dynamics, the exponential signal decay is found to result from predissociation predominantly at the lowest avoided X-A potential curve crossing, for which we infer a coupling constant V=650(20) reciprocal cm. The lack of a pump-probe delay dependence for the case of LiI embedded in helium nanodroplets indicates fast droplet-induced relaxation of the vibrational excitation.

physics.atm-clus↗

arXiv2014

Desorption Dynamics of Heavy Alkali Metal Atoms (Rb, Cs) off the Surface of Helium Nanodroplets

We present a combined ion imaging and density functional theory study of the dynamics of the desorption process of rubidium and cesium atoms off the surface of helium nanodroplets upon excitation of the perturbed $6s$ and $7s$ states, respectively. Both experimental and theoretical results are well represented by the pseudodiatomic model for effective masses of the helium droplet in the desorption reaction of m_eff/m_He~10 (Rb) and 13 (Cs). Deviations from this model are found for Rb excited to the 6p state. Photoelectron spectra indicate that the dopant-droplet interaction induces relaxation into low-lying electronic states of the desorbed atoms in the course of the ejection process.

physics.atm-clus↗

arXiv2014

Photoionizaton of Pure and Doped Helium Nanodroplets

Helium nanodroplets, commonly regarded as the "nearly ideal spectroscopic matrix", are being actively studied for more than two decades now. While they mostly serve as cold, weakly perturbing and transparent medium for high-resolution spectroscopy of embedded molecules, their intrinsic quantum properties such as microscopic superfluidity still are subject-matter of current research. This article reviews recent work on pure and doped He nanodroplets using PI spectroscopy, an approach which has greatly advanced in the past years. While the notion of the ideal spectroscopic matrix mostly no longer holds in this context, photoionization techniques provide detailed insights into the photo-physical properties of pure and doped He nanodroplets and their relaxation dynamics following electronic excitation. Exploiting nowadays available high laser fields, even highly ionized states of matter on the nanoscale can be formed. Our particular focus lies on recent experimental progress including fs time-resolved spectroscopy, photoion and electron imaging, and novel sources of highly energetic radiation.

physics.atm-clus↗

arXiv2013

Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields.

physics.atm-clus↗

arXiv2013

EUV ionization of pure He nanodroplets: Mass-correlated photoelectron imaging, Penning ionization and electron energy-loss spectra

The ionization dynamics of pure He nanodroplets irradiated by EUV radiation is studied using Velocity-Map Imaging PhotoElectron-PhotoIon COincidence (VMI-PEPICO) spectroscopy. We present photoelectron energy spectra and angular distributions measured in coincidence with the most abundant ions He+, He2+, and He3+. Surprisingly, below the autoionization threshold of He droplets we find indications for multiple excitation and subsequent ionization of the droplets by a Penning-like process. At high photon energies we evidence inelastic collisions of photoelectrons with the surrounding He atoms in the droplets.

physics.atm-clus↗

arXiv2013

Penning ionization of doped helium nanodroplets following EUV excitation

Helium nanodroplets are widely used as a cold, weakly interacting matrix for spectroscopy of embedded species. In this work we excite or ionize doped He droplets using synchrotron radiation and study the effect onto the dopant atoms depending on their location inside the droplets (rare gases) or outside at the droplet surface (alkali metals). Using photoelectron-photoion coincidence imaging spectroscopy at variable photon energies (20-25 eV), we compare the rates of charge-transfer to Penning ionization of the dopants in the two cases. The surprising finding is that alkali metals, in contrast to the rare gases, are efficiently Penning ionized upon excitation of the (n=2)-bands of the host droplets. This indicates rapid migration of the excitation to the droplet surface, followed by relaxation, and eventually energy transfer to the alkali dopants.

physics.atm-clus↗

arXiv2012

Quantum rainbow scattering at tunable velocities

Elastic scattering cross sections are measured for lithium atoms colliding with rare gas atoms and SF6 molecules at tunable relative velocities down to ~50 m/s. Our scattering apparatus combines a velocity-tunable molecular beam with a magneto-optic trap that provides an ultracold cloud of lithium atoms as a scattering target. Comparison with theory reveals the quantum nature of the collision dynamics in the studied regime, including both rainbows as well as orbiting resonances.

physics.atom-ph↗

arXiv2012

Formation and relaxation of RbHe exciplexes on He nanodroplets studied by femtosecond pump and picosecond probe spectroscopy

Vibrationally resolved photoionization spectra of RbHe exciplexes forming on He nanodroplets are recorded using femtosecond pump-probe spectroscopy with amplitude-shaped probe pulses. The time-evolution of the spectra reveals an exciplex formation time ~10ps followed by vibrational relaxation extending up to >1ns. This points to an indirect, time-delayed desorption process of RbHe off the He surface.

physics.atm-clus↗

arXiv2012

Spectroscopy of PTCDA attached to rare gas samples: clusters vs. bulk matrices. I. Absorption spectroscopy

The interaction between PTCDA (3,4,9,10-perylene-tetracarboxylic-dianhydride) and rare gas or para-hydrogen samples is studied by means of laser-induced fluorescence excitation spectroscopy. The comparison between spectra of PTCDA embedded in a neon matrix and spectra attached to large neon clusters shows that these large organic molecules reside on the surface of the clusters when doped by the pick-up technique. PTCDA molecules can adopt different conformations when attached to argon, neon and para-hydrogen clusters which implies that the surface of such clusters has a well-defined structure and has not liquid or fluxional properties. Moreover, a precise analysis of the doping process of these clusters reveals that the mobility of large molecules on the cluster surface is quenched, preventing agglomeration and complex formation.

physics.atm-clus↗

arXiv2012

Spectroscopy of PTCDA attached to rare gas samples: clusters vs. bulk matrices. II. Fluorescence emission spectroscopy

The interaction between PTCDA (3,4,9,10-perylene-tetracarboxylic-dianhydride) molecules and solid rare gas samples is studied by means of fluorescence emission spectroscopy. On the one hand, laser-excited PTCDA-doped large argon, neon and para-hydrogen clusters in comparison with PTCDA embedded in helium nanodroplets are spectroscopically characterized with respect to line broadening and shifting. A fast non-radiative relaxation is observed before a radiative decay in the electronic ground state takes place. On the other hand, fluorescence emission studies of PTCDA embedded in bulk neon and argon matrices results in much more complex spectral signatures characterized by a splitting of the different emission lines. These can be assigned to the appearance of site isomers of the surrounding matrix lattice structure.

physics.atm-clus↗

arXiv2012

Evolution of dopant-induced helium nanoplasmas

Two-component nanoplasmas generated by strong-field ionization of doped helium nanodroplets are studied in a pump-probe experiment using few-cycle laser pulses in combination with molecular dynamics simulations. High yields of helium ions and a pronounced, droplet size-dependent resonance structure in the pump-probe transients reveal the evolution of the dopant-induced helium nanoplasma. The pump-probe dynamics is interpreted in terms of strong inner ionization by the pump pulse and resonant heating by the probe pulse which controls the final charge states detected via the frustration of electron-ion recombination.

physics.atm-clus↗

arXiv2011

Imaging spectroscopy of rubidium atoms attached to helium nanodroplets

Highly excited states of rubidium (Rb) atoms attached to helium (He) nanodroplets are studied by two-photon ionization spectroscopy in combination with electron and ion imaging. Photoion spectra and angular distributions are in good agreement with a pseudodiatomic model for the RbHe_N complex. Repulsive interactions in the excited states entail fast dissociation followed by ionization of free Rb atoms as well as of RbHe and RbHe_2 exciplexes. Nonresonant excitation generates Rb atoms in low-lying electronic levels by statistical evaporation-like desorption.

physics.atm-clus↗

arXiv2011

Guiding slow polar molecules with a charged wire

We demonstrate experimentally the guiding of cold and slow ND3 molecules along a thin charged wire over a distance of ~0.34 m through an entire molecular beam apparatus. Trajectory simulations confirm that both linear and quadratic high-field-seeking Stark states can be efficiently guided from the beam source up to the detector. A density enhancement up to a factor 7 is reached for decelerated beams with velocities ranging down to ~50 m/s generated by the rotating nozzle technique.

physics.atm-clus↗

arXiv2011

Dopant induced ignition of helium nanodroplets in intense few-cycle laser pulses

We demonstrate ultrafast resonant energy absorption of rare-gas doped He nanodroplets from intense few-cycle (~10 fs) laser pulses. We find that less than 10 dopant atoms "ignite" the droplet to generate a non-spherical electronic nanoplasma resulting ultimately in complete ionization and disintegration of all atoms, although the pristine He droplet is transparent for the laser intensities applied. Our calculations at those intensities reveal that the minimal pulse length required for ignition is about 9 fs.

physics.atm-clus↗

arXiv2009

Improved setup for producing slow beams of cold molecules using a rotating nozzle

Intense beams of cold and slow molecules are produced by supersonic expansion out of a rapidly rotating nozzle, as first demonstrated by Gupta and Herschbach. An improved setup is presented that allows to accelerate or decelerate cold atomic and molecular beams by up to 500 m/s. Technical improvements are discussed and beam parameters are characterized by detailed analysis of time of flight density distributions. The possibility of combining this beam source with electrostatic fields for guiding polar molecules is demonstrated.

physics.atom-ph↗

arXiv2009

High-resolution spectroscopy of triplet states of Rb2 by femtosecond pump-probe photoionization of doped helium nanodroplets

The dynamics of vibrational wave packets in triplet states of rubidium dimers (Rb2) formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited Rb2 molecules off the droplets and due to their low internal temperature, wave packet oscillations can be followed up to very long pump-probe delay times >1.5ns. In the first excited triplet state (1)^3Σ_g^+, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations.

physics.atm-clus↗

arXiv2009

Alkali-helium snowball complexes formed on helium nanodroplets

We systematically investigate the formation and stability of snowballs formed by femtosecond photo-ionization of small alkali clusters bound to helium nanodroplets. For all studied alkali species Ak=(Na, K, Rb, Cs) we observe the formation of snowballs (AkHe_N)^+ when multiply doping the droplets. Fragmentation of clusters Ak_N upon ionization appears to enhance snowball formation. In the case of Na and Cs we also detect snowballs (Ak_2He_N)^+ formed around Ak dimer ions. While the snowball progression for Na and K is limited to less than 11 helium atoms, the heavier atoms Rb and Cs feature wide distributions at least up to (AkHe_41)^+. Characteristic steps in the mass spectra of Cs-doped helium droplets are found at positions consistent with predictions on the closure of the 1st shell of helium atoms around the Ak^+ ion based on variational Monte Carlo simulations.

physics.atm-clus↗