arXiv subjects

Frank Stienkemeier

Publications and source records attributed to Frank Stienkemeier.

At least 37 records · Page 2Linked to original sources

arXiv2022

Time-resolved Ultrafast Interatomic Coulombic Decay in Superexcited Sodium-doped Helium Nanodroplets

The autoionization dynamics of superexcited superfluid He nanodroplets doped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electron spectroscopy. Following excitation into the higher-lying droplet absorption band, the droplet relaxes into the lowest metastable atomic $1s2s$ $^{1,\,3}$S states from which Interatomic Coulombic Decay (ICD) takes places either between two excited He atoms or between an excited He atom and a Na atom attached to the droplet surface. Four main ICD channels are identified and their time constants are determined by varying the delay between the XUV pulse and a UV pulse that ionizes the initial excited state and thereby quenches ICD. The time constants for the different channels all fall in the range $\sim$1~ps indicating that the ICD dynamics are mainly determined by the droplet environment. A periodic modulation of the transient ICD signals is tentatively attributed to the oscillation of the bubble forming around the localized He excitation. The ICD efficiency depends on the total number of excited states in a droplet rather than the density of excited states pointing to a collective enhancement of ICD.

physics.atm-clus↗

arXiv2022

Excitation dynamics in polyacene molecules on rare-gas clusters

Laser-induced fluorescence spectra and excitation lifetimes of anthracene, tetracene, and pentacene molecules attached to the surface of solid argon clusters have been measured with respect to cluster size, density of molecules and excitation density. Results are compared to previous studies on the same sample molecules attached to neon clusters. A contrasting lifetime behavior of anthracene on neon and argon clusters is discussed, and mechanisms are suggested to interpret the results. Although both neon and argon clusters are considered to be weakly interacting environments, we find that the excitation decay dynamics of the studied acenes depends significantly on the cluster material. Moreover, we find even qualitative differences regarding the dependence on the dopant density. Based on these observations, previous assignments of collective radiative and non-radiative decay mechanisms are discussed in the context of the new experimental findings.

physics.chem-ph↗

arXiv2021

Improved stabilization scheme for extreme ultraviolet quantum interference experiments

Interferometric pump-probe experiments in the extreme ultraviolet (XUV) domain are experimentally very challenging due to the high phase stability required between the XUV pulses. Recently, an efficient phase stabilization scheme was introduced for seeded XUV free electron lasers (FELs) combining shot-to-shot phase modulation with lock-in detection. This method stabilized the seed laser beampath on the fundamental ultraviolet wavelength to a high degree. Here, we extend this scheme including the stabilization of the XUV beampath, incorporating phase fluctuations from the FEL high gain harmonic generation process. Our analysis reveals a clear signal improvement with the new method compared to the previous stabilization scheme.

physics.atom-ph↗

arXiv2021

Dynamics of photo-excited Cs atoms attached to helium nanodroplets

We present an experimental study of the dynamics following the photo-excitation and subsequent photo-ionization of single Cs atoms on the surface of helium nanodroplets. The dynamics of excited-Cs-atom desorption and re-adsorption as well as CsHe exciplex formation are measured using femtosecond pump-probe velocity-map-imaging spectroscopy and ion-time-of-flight spectrometry. The timescales for the desorption of excited Cs atoms off helium nanodroplets as well as the timescales for CsHe exciplex formation are experimentally determined for the 6p states of Cs. For the 6p $^2Π_ {1/2}$ state, our results confirm that the excited Cs atoms only desorb from the nanodroplet when the excitation wavenumber is blue-shifted from the $6p\,^2Π_ {1/2} \leftarrow 6s\,^2Σ_ {1/2}$ resonance. Our results suggest that the dynamics following excitation to the 6p $^2Π_ {3/2}$ state can be described by an evaporation-like desorption mechanism, whereas the dynamics arising from excitation to the 6p $^2Σ_ {1/2}$ state is indicative for a more impulsive desorption process. Furthermore, our results suggest a helium-induced spin-orbit relaxation from the the 6p $^2Σ_ {1/2}$ state to the 6p $^2Π_ {1/2}$ state. Our findings largely agree with the results of time-dependent $^4$He-density-functional theory (DFT) simulations published earlier [Coppens et al., Eur. Phys. J. D 73, 94 (2019)].

physics.atm-clus↗

arXiv2021

Effects of high pulse intensity and chirp in two-dimensional electronic spectroscopy of an atomic vapor

The effects of high pulse intensity and chirp on two-dimensional electronic spectroscopy signals are experimentally investigated in the highly non-perturbative regime using atomic rubidium vapor as clean model system. Data analysis is performed based on higher-order Feynman diagrams and non-perturbative numerical simulations of the system response. It is shown that higher-order contributions may lead to a fundamental change of the static appearance and beating-maps of the 2D spectra and that chirped pulses enhance or suppress distinct higher-order pathways. We further give an estimate of the threshold intensity beyond which the high-intensity effects become visible for the system under consideration.

physics.optics↗

arXiv2021

Development and characterization of high-frequency sources for supersonic beams of fluorine radicals

We present and compare two high-pressure, high-frequency electric-discharge sources for the generation of supersonic beams of fluorine radicals. The sources are based on dielectric-barrier-discharge (DBD) and plate-discharge units attached to a pulsed solenoid valve. The corrosion-resistant discharge sources were operated with fluorine gas seeded in helium up to backing pressures as high as 30 bar. We employed a (3+1) resonance-enhanced multiphoton ionization combined with velocity-map imaging for the optimization, characterization and comparison of the fluorine beams. Additionally, universal femtosecond-laser-ionization detection was used for the characterization of the discharge sources at experimental repetition rates up to 200 Hz. Our results show that the plate discharge is more efficient in F$_{2}$ dissociation than the DBD by a factor of 8-9, whereas the DBD produces internally colder fluorine radicals.

physics.chem-ph↗

arXiv2021

A flexible and scalable, fully software-based lock-in amplifier for nonlinear spectroscopy

We demonstrate a cost-effective, fully software-based lock-in amplifier (LIA) implemented on a commercial computer. The device is designed for application in nonlinear spectroscopy, such as transient absorption and coherent multidi-mensional spectroscopy, but may be also used in any other application. The performance of our device is compared to a state-of-the-art commercial LIA with nearly identical results for both devices. Advantages of our device over commercial hardwired electronic lock-in amplifiers is the improved flexibility in the data analysis and the possibility of arbitrary up-scaling of the number of LIA channels.

physics.ins-det↗

arXiv2021

Single-Source, Collinear Merged-Beam Experiment for the Study of Reactive Neutral-Neutral Collisions

We present two methods for studying reactive collisions between two atomic or molecular species: a collinear merged-beam method, in which two gas pulses from a single supersonic beam source are coalesced, and an intrabeam-scattering technique, in which a single gas pulse is used. Both approaches, which rely on the laser cooling and deceleration of a laser-coolable species inside a Zeeman slower, can be used for a wide range of scattering studies. Possible experimental implementations of the proposed methods are outlined for autoionizing collisions between helium atoms in the metastable $2^3\mathrm{S}_1$ state and a second, atomic or molecular species. Using numerical trajectory calculations, we provide estimates of the expected on-axis detection efficiency, collision-energy range and collision-energy resolution of the approach. We have experimentally tested the feasibility of such an experiment by producing two gas pulses at very short time intervals, and the results of these measurements are detailed as well.

physics.atom-ph↗

arXiv2021

Sensitive detection of metastable NO and \ce{N2} by reactive collisions with laser-excited Li

In a proof-of-principle experiment, we demonstrate that metastable nitric oxide molecules, NO(a$^4Π_i$), generated inside a pulsed, supersonic beam, can be detected by reactive gas-phase collisions with electronically excited Li atoms in the $2^2$P$_{3/2}$ state. Since the internal energy of NO(a$^4Π_i$, $v \leq 4$) is lower than the ionization potential of Li in the $2^2$S$_{1/2}$ electronic ground state, we observe that the product ion yield arising from autoionizing NO(a$^4Π_i$)+Li($2^2$S$_{1/2}$) collisions is a factor of 21 lower than the ion yield from NO(a$^4Π_i$)+Li($2^2$P$_{3/2}$) collisions. We also compare our findings with measurements of relative rates for collisions of metastable \ce{N2}+Li($2^2$S$_{1/2}$) and metastable \ce{N2}+Li($2^2$P$_{3/2}$) reactive collisions. Using this detection method, we infer densities of $\approx 600$ NO(a$^4Π_i$) molecules/cm$^3$ and $\approx 6 \cdot 10^{4}$ metastable \ce{N2} molecules/cm$^3$ in the interaction region. Our results also allow for an estimate of the fractional population of NO(a$^4Π_i$, $v \geq 5$) prior to the collision process. The production of NO(a$^4Π_i$) in selected vibrational states using laser excitation from the X$^2Π_r$ ground state will open possibilities for the detailed study of vibrational-state-selected NO(a$^4Π_i$)-Li($2^2$P$_{3/2}$) collisions.

physics.atom-ph↗

arXiv2021

Preparation of individual magnetic sub-levels of $^4$He($2^3$S$_1$) in a supersonic beam using laser optical pumping and magnetic hexapole focusing

We compare two different experimental techniques for the magnetic-sub-level preparation of metastable $^4$He in the $2^3$S$_1$ level in a supersonic beam, namely magnetic hexapole focusing and optical pumping by laser radiation. At a beam velocity of $v = 830\,$m/s, we deduce from a comparison with a particle trajectory simulation that up to $99\,$\% of the metastable atoms are in the $M_{J^{''}} = +1$ sub-level after magnetic hexapole focusing. Using laser optical pumping via the $2^3$P$_2-2^3$S$_1$ transition, we achieve a maximum efficiency of $94\pm3\,$\% for the population of the $M_{J^{''}} = +1$ sub-level. For the first time, we show that laser optical pumping via the $2^3$P$_1-2^3$S$_1$ transition can be used to selectively populate each of the three $M_{J^{''}}$ sub-levels ($M_{J^{''}} = $ -1, 0, +1). We also find that laser optical pumping leads to higher absolute atom numbers in specific $M_{J^{''}}$ sub-levels than magnetic hexapole focusing.

physics.atom-ph↗

arXiv2021

Unravelling the Full Relaxation Dynamics of Superexcited Helium Nanodroplets

The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: Droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product of both droplet autoionization and photoionization is He$_2^+$, whereas the delayed appearance of He$^+$ is indicative of the ejection of excited He atoms from the droplets. The state-resolved time-dependent photoelectron spectra reveal that intermediate excited states of the droplets are populated in the course of the relaxation, terminating in the lowest-lying metastable singlet and triplet He atomic states. The slightly faster relaxation of the triplet state compared to the singlet state is in agreement with the simulation showing faster formation of a bubble around a He atom in the triplet state.

physics.atm-clus↗

arXiv2020

Tracking Attosecond Electronic Coherences Using Phase-Manipulated Extreme Ultraviolet Pulses

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths.

physics.atom-ph↗

arXiv2020

Phase cycling of extreme ultraviolet pulse sequences generated in rare gases

The development of schemes for coherent nonlinear time-domain spectroscopy in the extreme-ultraviolet regime (XUV) has so far been impeded by experimental difficulties that arise at these short wavelengths. In this work we present a novel experimental approach, which facilitates the timing control and phase cycling of XUV pulse sequences produced by harmonic generation in rare gases. The method is demonstrated for the generation and high spectral resolution characterization of narrow-bandwidth harmonics ($\approx14\,$eV) in argon and krypton. Our technique simultaneously provides high phase stability and a pathway-selective detection scheme for nonlinear signals - both necessary prerequisites for all types of coherent nonlinear spectroscopy.

physics.atom-ph↗

arXiv2020

High-Gain Harmonic Generation with temporally overlapping seed pulses and application to ultrafast spectroscopy

Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). High-order fringe-resolved autocorrelation and wave-packet interferometry experiments at photon energies > $23\,$eV are performed, accompanied by numerical simulations. It turns out that both the autocorrelation and the wave-packet interferometry data are very sensitive to saturation effects and can thus be used to characterize saturation in the HGHG process. Our results further imply that time-resolved spectroscopy experiments are feasible even for time delays smaller than the seed pulse duration.

physics.atom-ph↗

arXiv2020

Suppression of Penning ionization by orbital angular momentum conservation

The efficient suppression of Penning-ionizing collisions is a stringent requirement to achieve quantum degeneracy in metastable rare gases. Thus far, such loss processes have been avoided by electron-spin polarizing the collision partners. Here, we report on the efficient suppression of Penning ionization in collisions between metastable He and laser-excited Li atoms. The results illustrate that not only the electron spin, but also $Λ$ - the projection of the total molecular orbital angular momentum along the internuclear axis - is conserved during the ionization process. Our findings suggest that $Λ$ conservation can be used as a more general means of reaction control, for example, to improve schemes for the simultaneous laser cooling and trapping of metastable He and alkali atoms.

physics.chem-ph↗

arXiv2020

Time-resolved formation of excited atomic and molecular states in XUV-induced nanoplasmas in ammonia clusters

High intensity XUV radiation from a free-electron (FEL) was used to create a nanoplasma inside ammonia clusters with the intent of studying the resulting electron-ion interactions and their interplay with plasma evolution. In a plasma-like state, electrons with kinetic energy lower than the local collective Coulomb potential of the positive ionic core are trapped in the cluster and take part in secondary processes (e.g. electron-impact excitation/ionization and electron-ion recombination) which lead to subsequent excited and neutral molecular fragmentation. Using a time-delayed UV laser, the dynamics of the excited atomic and molecular states are probed from -0.1 ps to 18 ps. We identify three different phases of molecular fragmentation that are clearly distinguished by the effect of the probe laser on the ionic and electronic yield. We propose a simple model to rationalize our data and further identify two separate channels leading to the formation of excited hydrogen.

physics.atm-clus↗

arXiv2019

Coherent multidimensional spectroscopy in the gas phase

Recent work applying multidimentional coherent electronic spectroscopy at dilute samples in the gas phase is reviewed. The development of refined phase-cycling approaches with improved sensitivity has opened-up new opportunities to probe even dilute gas-phase samples. In this context, first results of 2-dimensional spectroscopy performed at doped helium droplets reveal the femtosecond dynamics upon electronic excitation of cold, weakly-bound molecules, and even the induced dynamics from the interaction with the helium environment. Such experiments, offering well-defined conditions at low temperatures, are potentially enabling the isolation of fundamental processes in the excitation and charge transfer dynamics of molecular structures which so far have been masked in complex bulk environments.

physics.atm-clus↗

arXiv2019

Deep neural networks for classifying complex features in diffraction images

Intense short-wavelength pulses from free-electron lasers and high-harmonic-generation sources enable diffractive imaging of individual nano-sized objects with a single x-ray laser shot. The enormous data sets with up to several million diffraction patterns represent a severe problem for data analysis, due to the high dimensionality of imaging data. Feature recognition and selection is a crucial step to reduce the dimensionality. Usually, custom-made algorithms are developed at a considerable effort to approximate the particular features connected to an individual specimen, but facing different experimental conditions, these approaches do not generalize well. On the other hand, deep neural networks are the principal instrument for today's revolution in automated image recognition, a development that has not been adapted to its full potential for data analysis in science. We recently published in Langbehn et al. (Phys. Rev. Lett. 121, 255301 (2018)) the first application of a deep neural network as a feature extractor for wide-angle diffraction images of helium nanodroplets. Here we present the setup, our modifications and the training process of the deep neural network for diffraction image classification and its systematic benchmarking. We find that deep neural networks significantly outperform previous attempts for sorting and classifying complex diffraction patterns and are a significant improvement for the much-needed assistance during post-processing of large amounts of experimental coherent diffraction imaging data.

physics.data-an↗