arXiv subjects

Lukas Bruder

Publications and source records attributed to Lukas Bruder.

At least 19 recordsLinked to original sources

arXiv2026

Size characterization of neutral rare-gas clusters based on time-resolved polarization anisotropy measurements

The size determination of neutral clusters is experimentally challenging. In particular, weakly-bound rare-gas clusters tend to fragment upon ionization, resulting in systematic errors in cluster size studies. In contrast, characterization of the temporal polarization anisotropy dephasing provides a soft detection scheme for cluster size estimation, which avoids fragmentation of the clusters. Here, we present a systematic experimental study of argon and neon clusters in the size range of 50 to 10.000 atoms using this technique. In order to extract the mean cluster sizes from the data, we present an efficient analytical model of the polarization anisotropy dephasing of an ensemble of doped clusters. The approach shows remarkable sensitivity to small changes in the mean cluster size of just a few tens of atoms and allows us to refine the widely used Hagena scaling law for the estimation of rare-gas cluster sizes.

physics.atm-clus↗

arXiv2026

Ultrafast configuration changes and anomalous diffusion of an aromatic adsorbate on rare-gas nanoparticles

Nanoparticles (NPs) exhibit tunable catalytic properties and serve as nanoreactors for controlled multimolecular chemistry. The kinetics and reactivity of such systems are critically governed by the surface binding configurations of adsorbates, their stochastic fluctuations, and the adsorbate mobility across the nanosurface. However, resolving these properties with sufficient structural, spatial, and temporal resolution remains a major experimental challenge. Here, we study phthalocyanine adsorbates on rare-gas clusters as a test case. By combining high-resolution two-dimensional electronic spectroscopy and molecular dynamics simulations, we reveal the configurational dynamics of the adsorbates and establish a direct relation between these dynamics and the nanoscale properties of the clusters. Our findings indicate sub-diffusive surface motion and trapping of the adsorbate within single surface facets. Such dynamical behavior seems unexpected considering the weak adsorbate-surface interaction and cluster temperatures close to the sublimation point. These results provide direct insight into the ultrafast binding dynamics of molecular adsorbates on nanoscale objects, which is critical for our understanding of the chemistry of such systems.

physics.chem-ph↗

arXiv2026

Impact of interference between two infrared pulses driving high harmonic generation

Extreme ultraviolet (XUV) interferometry is technically challenging to implement. One approach to generating interference between two XUV pulses relies on driving high-harmonic generation in a gas jet with two collinearly overlapping infrared laser pulses. We investigate this scheme through a combined experimental and theoretical study, with particular emphasis on the regime of temporal overlap between the driving pulses. A special phase-modulation interferometry technique is implemented to increase the sensitivity for the comprehensive mapping of the strong-field induced high-order nonlinear response. We find that the dynamics arising from the interference of the two electric fields can be adequately described by the non-perturbative model developed by Lewenstein and co-workers.

physics.optics↗

arXiv2025

Anisotropic fluorescence signals retarded dipole-dipole interactions in a thermal atomic cloud

We experimentally observe and theoretically explain anisotropic multiple quantum coherence signals in the fluorescence from dilute thermal potassium vapors, at room temperature and particle densities $\sim 10^8\ \rm{cm}^{-3}$. We identify the retarded part of the geometrically fully resolved inter-atomic, resonant dipole-dipole interaction as the crucial ingredient to theoretically reproduce all qualitative features of the experimental spectra.

quant-ph↗

arXiv2025

Low-dispersive phase-modulated rapid scanning interferometry

Time-domain interferometry is an important principle in Fourier transform (FT) and nonlinear femto- to attosecond spectroscopy. To optimize the resolution and sensitivity of this approach, various interferometer stabilization schemes have been developed. Among them, acousto-optical phase modulation (AOPM) of the interferometer arms combined with phase-synchronous lock-in detection has proven as a particular sensitive technique. However, the acousto-optical modulators (AOMs), required for this technique, introduce several disadvantages. Here, we demonstrate an alternative phase modulation scheme which omits AOMs, termed PM scheme here. As a benchmark, we directly compare the performance between the PM and the AOPM scheme in a linear FT spectroscopy experiment and find comparable sensitivity in both approaches.

physics.optics↗

arXiv2025

High-resolution rapid-scanning Fourier-transform spectroscopy of ultracold atoms

Femtosecond interferometry combined with acousto-optical phase modulation is an effective approach to implement various types of coherent nonlinear and multidimensional spectroscopy schemes. The high sensitivity of this method has recently enabled the study of highly dilute gaseous and ultracold quantum systems for which the attainable spectral resolution is of particular interest. Here, we directly compare the performance and spectral resolution between two experimental implementations, that are step-wise and continuous rapid scanning of the underlying Fourier transform interferometers. We show the performance advantage of the rapid-scanning approach and demonstrate a spectral resolution of 250 MHz in the spectroscopy of laser-cooled Li atoms. This is a 10-fold resolution improvement compared to previous experiments.

physics.atom-ph↗

arXiv2024

Strong-field quantum control in the extreme ultraviolet using pulse shaping

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. While 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, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

physics.atom-ph↗

arXiv2024

Non-adiabatic electronic relaxation of tetracene from its brightest singlet excited state

The ultrafast relaxation dynamics of tetracene following UV excitation to a bright singlet state S6 has been studied with time-resolved photoelectron spectroscopy. With the help of high-level ab-initio multireference perturbation theory calculations, we assign photoelectron signals to intermediate dark electronic states S3, S4 and S5 as well as a to a low-lying electronic state S2. The energetic structure of these dark states has not been determined experimentally previously. The time-dependent photoelectron yields assigned to the states S6, S5 and S4 have been analyzed and reveal the depopulation of S6 within 50 fs, while S5 and S4 are populated with delays of about 50 and 80 fs. The dynamics of the lower-lying states S3 and S2 seem to agree with a delayed population coinciding with the depopulation of the higher-lying states S4-S6, but could not be elucidated in full detail due to the low signal levels of the corresponding two-photon ionization probe processes.

physics.chem-ph↗

arXiv2023

Two-dimensional electronic spectroscopy of an ultracold gas

Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. For this, a setup for phase modulation spectroscopy is used to probe the $3^2\mathrm{S}_{1/2} - 2^2\mathrm{P}_{1/2, 3/2}$ transition in an 800 $μ$K-cold sample of $^7$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 atomic and molecular gases using this technique. The experiment combines a frequency resolution of 3 GHz with a potential time resolution of 200 fs, which allows for high-resolution studies of ultracold atoms and molecules both in the frequency and in the time domain.

physics.atom-ph↗

arXiv2022

Pulse overlap ambiguities in multiple quantum coherence spectroscopy

Coherent two-dimensional electronic spectroscopy probes ultrafast dynamics using femtosecond pulses. In case the timescale of the studied dynamics become comparable to the pulse duration, pulse overlap effects may compromise the experimental data. Here, we perform one-dimensional coherence scans and study pulse overlap effects in clean two-level systems. We find parasitic multiple-quantum coherence signals as a consequence of the arbitrary time ordering during the temporal pulse overlap. Surprisingly, the signal lifetimes exceed the temporal pulse overlap by a factor of 1.8. These findings have important implications for the interpretation of higher-order coherent two-dimensional and related spectroscopy experiments.

physics.chem-ph↗

arXiv2022

High-resolution two-dimensional electronic spectroscopy reveals homogeneous line profiles in isolated nanoparticles

Doped clusters in the gas phase provide nanoconfined model systems for the study of system-bath interactions. To gain insight into interaction mechanisms between chromophores and their environment, the ensemble inhomogeneity has to be lifted and the homogeneous line profile must be accessed. However, such measurements are very challenging at the low particle densities and low signal levels in cluster beam experiments. Here, we dope cryogenic rare-gas clusters with phthalocyanine molecules and apply action-detected two-dimensional electronic spectroscopy to gain insight into the local molecule-cluster environment for solid and superfluid cluster species. The high-resolution homogeneous linewidth analysis provides a benchmark for the theoretical modelling of binding configurations and shows a promising route for high-resolution molecular two-dimensional spectroscopy.

physics.chem-ph↗

arXiv2022

Extreme ultraviolet wave packet interferometry of the autoionizing HeNe dimer

Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant inter-atomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process. A Fourier analysis reveals the molecular absorption spectrum with high resolution. The demonstrated experiment shows a promising route for the real-time analysis of ultrafast ICD processes with both high temporal and spectral resolution.

physics.atm-clus↗

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↗

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

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

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

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↗