arXiv subjects

Jan Vogelsang

Publications and source records attributed to Jan Vogelsang.

At least 19 recordsLinked to original sources

arXiv2026

Spatially-resolved multiphoton photoemission from a lateral transition metal dichalcogenide heterostructure

Transition metal dichalcogenides (TMDs) in their monolayer form offer a premier platform for next-generation optoelectronics, particularly through the local manipulation of their robust excitonic states using nanoscale electric fields. These localized states can be dynamically controlled through spatial structuring as well as through ultrafast field modulations driven by tailored optical pulses. Characterizing the resulting rapid, nanoscale charge carrier dynamics requires a technique with exceptional spatial and temporal resolution. Here, we report on the spatio-temporally resolved investigation of ground state and excited state photoemission from a lateral heterostructure built of monolayers of WSe$_2$ and MoSe$_2$ using few-cycle light pulses with a photon energy of 0.62 eV. We utilize photoemission electron microscopy to spatially resolve the highly nonlinear photoemission from the monolayer structure with few tens of nanometer resolution. By varying the laser pulse energy, we extract the nonlinearity of the photoemission process and thus the dynamic binding energy of the photoelectrons before and after optical excitation with high spatial and temporal resolution.

physics.optics↗

arXiv2026

NUMA balancing hampering performance of spiking network simulations

Computing centers today mostly operate conventional CPU- and GPU-based systems, where the direct way of decreasing energy consumption is a reduction in the applications' runtime. Neuromorphic computing promises an alternative architecture with improved energy efficiency for artificial intelligence. In this endeavor, code for the simulation of large-scale spiking networks on conventional supercomputers is the reference. We show that turning off automatic NUMA balancing may reduce energy consumption by 30%. This dwarfs other attempts of increasing the energy efficiency of a computing center with respect to cost effectiveness. The memory access pattern of spiking network simulation code dynamically interacts with automatic NUMA balancing. This does not affect the correctness of simulation results and thus goes unnoticed in day-to-day neuroscience research. In performance analysis, however, time measurements fluctuate obstructing attempts to optimize simulation technology. A new time- and compute-node resolved performance display exposes the fine-grained temporal variability of distributed spiking network simulations. The analysis uncovers that automatic NUMA balancing is of disadvantage and affects the jemalloc library for thread-aware memory allocation in a transient manner. The method also allows developers to detect perturbations of the HPC system and target specific improvements to simulation technology. As a consequence, we have equipped our supercomputers with an option to turn on or off automatic NUMA balancing on a per-job basis on the user level. This gives researchers the opportunity to find the best setting for the application at hand. There are indications in the literature that the effect has been observed before, yet it does not seem common knowledge in scientific computing. It remains to be investigated how widespread the phenomenon is among scientific codes.

cs.DC↗

arXiv2026

Continuous benchmarking: Keeping pace with an evolving ecosystem of models and technologies

Drawing on ideas from continuous integration, we present concepts of an automated benchmarking pipeline for high performance applications. Customization and collaboration have been key design goals owing to the requirements of research-software development as a continuous community effort. We have extended our previous conceptual work on systematic benchmarking workflows with the functionality of user-agnostic operations as well as continuous benchmarking. This fosters reproducibility and re-use of benchmarking results to ensure sustainable technological progress. We provide software-engineering solutions to keep pace with the rapid evolution of both large-scale models and high-performance computing systems with a view towards the scientific domains of neuroscience and artificial intelligence.

cs.DC↗

arXiv2024

Multiscale carrier-envelope phase characterization of 2-\mu m pulses delivered by a 200-kHz optical parametric amplifier

Light fields with a central wavelength of 2 um are very well suited for strong-field-driven charge carrier control: Their photon energy lies far below the band gap of many materials, while their oscillation period remains significantly shorter than the coherence time of charge carrier oscillations. The resulting potential for field-driven charge carrier control is contingent on the reproducibility of the field structure of such ultrashort laser pulses. Here, we present a compact 200-kHz laser system that delivers ultrashort pulses with a duration of less than 20 fs in the spectral range around 2 um and with a pulse energy of 25 uJ. The electric field structure of the 2-um pulses is characterized in detail. In particular, the carrier-envelope phase (CEP) is measured over a wide range of timescales, from microseconds to hours. Passive stabilization due to difference frequency generation results in a root mean square value of carrier-envelope phase noise of less than 70 mrad over all measured time scales. The applicability of the pulses is demonstrated by measuring CEP-dependent high-order harmonic spectra with energies of up to 160 eV.

physics.optics↗

arXiv2023

Time-resolved photoemission electron microscopy on a ZnO surface using an extreme ultraviolet attosecond pulse pair

Electrons photoemitted by extreme ultraviolet attosecond pulses derive spatially from the first few atomic surface layers and energetically from the valence band and highest atomic orbitals. As a result, it is possible to probe the emission dynamics from a narrow two-dimensional region in the presence of optical fields as well as obtain elemental specific information. However, combining this with spatially-resolved imaging is a long-standing challenge because of the large inherent spectral width of attosecond pulses as well as the difficulty of making them at high repetition rates. Here we demonstrate an attosecond interferometry experiment on a zinc oxide (ZnO) surface using spatially and energetically resolved photoelectrons. We combine photoemission electron microscopy with near-infrared pump - extreme ultraviolet probe laser spectroscopy and resolve the instantaneous phase of an infrared field with high spatial resolution. Our results show how the core level states with low binding energy of ZnO are well suited to perform spatially resolved attosecond interferometry experiments. We observe a distinct phase shift of the attosecond beat signal across the laser focus which we attribute to wavefront differences between the pump and the probe fields at the surface. Our work demonstrates a clear pathway for attosecond interferometry with high spatial resolution at atomic scale surface regions opening up for a detailed understanding of nanometric light-matter interaction.

physics.optics↗

arXiv2020

Picosecond time-resolved antibunching measures nanoscale exciton motion, annihilation, and true number of chromophores

The particle-like nature of light becomes evident in the photon statistics of fluorescence of single quantum systems as photon antibunching. In multichromophoric systems, exciton diffusion and subsequent annihilation occurs. These processes also yield photon antibunching but cannot be interpreted reliably. Here, we develop picosecond time-resolved antibunching (psTRAB) to identify and decode such processes. We use psTRAB to measure the true number of chromophores on well-defined multichromophoric DNA-origami structures, and precisely determine the distance-dependent rates of annihilation between excitons. Further, psTRAB allows us to measure exciton diffusion in mesoscopic H- and J-type conjugated-polymer aggregates. We distinguish between one-dimensional intra-chain and three-dimensional inter-chain exciton diffusion at different times after excitation and determine the disorder-dependent diffusion lengths. Our method provides a new lens through which excitons can be studied at the single-particle level, enabling the rational design of improved excitonic probes such as ultra-bright fluorescent nanoparticles, and materials for optoelectronic devices.

physics.chem-ph↗

arXiv2020

Characterizing ultrashort laser pulses with second harmonic dispersion scans

The dispersion scan (d-scan) technique has emerged as a simple-to-implement characterization method for ultrashort laser pulses. D-scan traces are intuitive to interpret and retrieval algorithms that are both fast and robust have been developed to obtain the spectral phase and the temporal pulse profile. Here, we give a review of the d-scan technique based on second harmonic generation. We describe and compare recent implementations for the characterization of few- and multi-cycle pulses as well as two different approaches for recording d-scan traces in single-shot, thus showing the versatility of the technique.

physics.optics↗

arXiv2020

A high-repetition rate attosecond light source for time-resolved coincidencespectroscopy

Attosecond pulses, produced through high-order harmonic generation in gases, have been successfully used for observing ultrafast, sub-femtosecond electron dynamics in atoms, molecules and solid state systems. Today's typical attosecond sources, however, are often impaired by their low repetition rate and the resulting insufficient statistics, especially when the number of detectable events per shot is limited. This is the case for experiments where several reaction products must be detected in coincidence, and for surface science applications where space-charge effects compromise spectral and spatial resolution. In this work, we present an attosecond light source operating at 200 kHz, which opens up the exploration of phenomena previously inaccessible to attosecond interferometric and spectroscopic techniques. Key to our approach is the combination of a high repetition rate, few-cycle laser source, a specially designed gas target for efficient high harmonic generation, a passively and actively stabilized pump-probe interferometer and an advanced 3D photoelectron/ion momentum detector. While most experiments in the field of attosecond science so far have been performed with either single attosecond pulses or long trains of pulses, we explore the hitherto mostly overlooked intermediate regime with short trains consisting of only a few attosecond pulses.e also present the first coincidence measurement of single-photon double ionization of helium with full angular resolution, using an attosecond source. This opens up for future studies of the dynamic evolution of strongly correlated electrons.

physics.atom-ph↗

arXiv2020

Few-cycle lightwave-driven currents in a semiconductor at high repetition rate

When an intense, few-cycle light pulse impinges on a dielectric or semiconductor material, the electric field will interact nonlinearly with the solid, driving a coherent current. An asymmetry of the ultrashort, carrier-envelope-phase-stable waveform results in a net transfer of charge, which can be measured by macroscopic electric contact leads. This effect has been pioneered with extremely short, single-cycle laser pulses at low repetition rate, thus limiting the applicability of its potential for ultrafast electronics. We investigate lightwave-driven currents in gallium nitride using few-cycle laser pulses of nearly twice the duration and at a repetition rate two orders of magnitude higher than in previous work. We successfully simulate our experimental data with a theoretical model based on interfering multiphoton transitions, using the exact laser pulse shape retrieved from dispersion-scan measurements. Substantially increasing the repetition rate and relaxing the constraint on the pulse duration marks an important step forward towards applications of lightwave-driven electronics.

physics.optics↗

arXiv2019

Interchromophoric Interactions Determine the Maximum Brightness Density in DNA Origami Structures

An ideal point light source is as small and as bright as possible. For fluorescent point light sources, homogeneity of the light sources is important as well as that the fluorescent units inside the light source maintain their photophysical properties which is compromised by dye aggregation. Here we propose DNA origami as a rigid scaffold to arrange dye molecules in a dense pixel array with high control of stoichiometry and dye-dye interactions. In order to find the highest labeling density in a DNA origami structure without influencing dye photophysics we alter the distance of two ATTO647N dyes in single base pair steps and probe the dye-dye interactions on the single-molecule level. For small distances strong quenching in terms of intensity and fluorescence lifetime is observed. With increasing distance, we observe reduced quenching and molecular dynamics. However, energy transfer processes in the weak coupling regime still have a significant impact and can lead to quenching by singlet-dark-state-annihilation. Our study fills a gap of studying the interactions of dyes relevant for superresolution microscopy with dense labeling and for single-molecule biophysics. Incorporating these findings in a 3D DNA origami object will pave the way to bright and homogeneous DNA origami nanobeads.

physics.chem-ph↗

arXiv2019

Controlling the Photoelectric Effect in the Time Domain

When an atom or molecule absorbs a high-energy photon, an electron is emitted with a well-defined energy and a highly-symmetric angular distribution, ruled by energy quantization and parity conservation. These rules seemingly break down when small quantum systems are exposed to short and intense light pulses, which raise the question of their universality for the simplest case of the photoelectric effect. Here we investigate the photoionization of helium by a sequence of attosecond pulses in the presence of a weak infrared dressing field. We continuously control the energy and introduce an asymmetry in the emission direction of the photoelectrons, thus contradicting well established quantum-mechanical predictions. This control is possible due to an extreme temporal confinement of the light-matter interaction. Our work extends time-domain coherent control schemes to one of the fastest processes in nature, the photoelectric effect.

physics.atom-ph↗

arXiv2018

Spatio-temporal coupling of attosecond pulses

The shortest light pulses produced to date are of the order of a few tens of attoseconds, with central frequencies in the extreme ultraviolet range and bandwidths exceeding tens of eV. They are often produced as a train of pulses separated by half the driving laser period, leading in the frequency domain to a spectrum of high, odd-order harmonics. As light pulses become shorter and more spectrally wide, the widely-used approximation consisting in writing the optical waveform as a product of temporal and spatial amplitudes does not apply anymore. Here, we investigate the interplay of temporal and spatial properties of attosecond pulses. We show that the divergence and focus position of the generated harmonics often strongly depend on their frequency, leading to strong chromatic aberrations of the broadband attosecond pulses. Our argumentation uses a simple analytical model based on Gaussian optics, numerical propagation calculations and experimental harmonic divergence measurements. This effect needs to be considered for future applications requiring high quality focusing while retaining the broadband/ultrashort characteristics of the radiation.

physics.optics↗

arXiv2018

Role of Triplet-State Shelving in Organic Photovoltaics: Single-Chain Aggregates of Poly(3-hexylthiophene) versus Mesoscopic Multichain Aggregates

Triplet excitons have been the focus of considerable attention with regards to the functioning of polymer solar cells, because these species are long-lived and quench subsequently generated singlet excitons in their vicinity. The role of triplets in poly(3-hexylthiophene) (P3HT) has been investigated extensively with contrary conclusions regarding their importance. We probe the various roles triplets can play in P3HT by analyzing the photoluminescence (PL) from isolated single-chain aggregates and multi-chain mesoscopic aggregates. Solvent vapor annealing allows deterministic growth of P3HT aggregates consisting of ~20 chains, which exhibit red-shifted and broadened PL compared to single-chain aggregates. The multi-chain aggregates exhibit a decrease of photon antibunching contrast compared to single-chain aggregates, implying rather weak interchain excitonic coupling and energy transfer. Nevertheless, the influence of triplet-quenching oxygen on PL and a photon correlation analysis of aggregate PL reveal that triplets are quenched by intermolecular interactions in the bulk state.

physics.chem-ph↗

arXiv2018

Determining the True Optical Gap in a High-Performance Organic Photovoltaic Polymer Using Single-Molecule Spectroscopy

Low-gap conjugated polymers have enabled an impressive increase in the efficiencies of organic solar cells, primarily due to their red absorption which allows harvesting of that part of the solar spectrum. Here, we report that the true optical gap of one prototypical material, PTB7, is in fact at significantly higher energy than has previously been reported, indicating that the red absorption utilized in these materials in solar cells is entirely due to chain aggregation. Using single-molecule spectroscopy we find that PL from isolated nanoscale aggregates consists of multiple independently emitting chromophores. At the single-molecule level, however, straight single chains with a high degree of emission polarization are observed. The PL is found to be ~0.4 eV higher in energy, with a longer lifetime than the red aggregates, and is attributed to single chromophores. Our findings indicate that the impressive light-harvesting abilities of PTB7 in the red spectral region arises solely from chain aggregation.

physics.chem-ph↗

arXiv2018

Watching charge separation in nanoantennas by ultrafast point-projection electron microscopy

Watching the motion of electrons on their natural nanometre length- and femtosecond time scales is a fundamental goal and an open challenge of contemporary ultrafast science. Optical techniques and electron microscopy currently mostly provide either ultrahigh temporal or spatial resolution, yet, microscopy techniques with combined space-time resolution need further development. Here we create an ultrafast electron source by plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used, in an optical pump - electron probe experiment, to study ultrafast photoemission from a nanometer-sized plasmonic antenna. We show that the real space motion of the photoemitted electrons and residual holes in the metal is probed with 20-nm spatial resolution and 25-fs time resolution. This is a step forward towards time-resolved microscopy of electronic motion in nanostructures.

physics.optics↗

arXiv2017

Spectral focusing of broadband silver electroluminescence in nanoscopic FRET-LEDs

Few inventions have shaped the world like the incandescent bulb. While Edison used thermal radiation from ohmically heated conductors, some noble metals exhibit "cold" electroluminescence (EL) in percolation films, tunnel diodes, electromigrated nanoparticle aggregates, optical antennae, or scanning-tunnelling microscopy (STM). The origin of this radiation, which is spectrally broad and depends on applied bias, is controversial given the low radiative yields of electronic transitions. Nanoparticle EL is particularly intriguing since it involves localized surface-plasmon resonances with large dipole moments. Such plasmons enable very efficient non-radiative fluorescence resonance energy transfer (FRET) coupling to proximal resonant dipole transitions. We demonstrate nanoscopic FRET-LEDs which exploit the opposite process, energy transfer from silver nanoparticles to exfoliated monolayers of transition-metal dichalcogenides (TMDCs). In diffraction-limited hotspots showing pronounced photon bunching, broadband silver EL is focused into the narrow excitonic resonance of the atomically thin overlayer. Such devices may offer alternatives to conventional nano-LEDs in on-chip optical interconnects.

physics.optics↗

arXiv2016

Mesoscopic Quantum Emitters from Deterministic Aggregates of Conjugated Polymers

An appealing definition of the term "molecule" arises from consideration of the nature of fluorescence, with discrete molecular entities emitting a stream of single photons. We address the question of how large a molecular object may become by growing deterministic aggregates from single conjugated polymer chains. Even particles containing dozens of individual chains still behave as single quantum emitters due to efficient excitation energy transfer, while the brightness is raised due to the increased absorption cross-section of the suprastructure. Excitation energy can delocalize between individual polymer chromophores in these aggregates by both coherent and incoherent coupling, which are differentiated by their distinct spectroscopic fingerprints. Coherent coupling is identified by a ten-fold increase in excited-state lifetime and a corresponding spectral red shift. Exciton quenching due to incoherent FRET becomes more significant as aggregate size increases, resulting in single-aggregate emission characterized by strong blinking. This mesoscale approach allows us to identify intermolecular interactions which do not exist in isolated chains and are inaccessible in bulk films where they are present but masked by disorder.

physics.chem-ph↗

arXiv2016

Differentiation between shallow and deep charge trap states on single poly(3-hexylthiophene) chains through fluorescence photon statistics

Blinking of the photoluminescence (PL) emitted from individual conjugated polymer chains is one of the central observations made by single-molecule spectroscopy (SMS). Important information, e.g., regarding excitation energy transfer, can be extracted by evaluating dynamic quenching. However, the nature of trap states, which are responsible for PL quenching, often remains obscured. We present a detailed investigation of the photon statistics of single poly(3-hexylthiophene) (P3HT) chains obtained by SMS. The photon statistics provide a measure of the number and brightness of independently emitting areas on a single chain. These observables can be followed during blinking. A decrease in PL intensity is shown to be correlated with either (i) a decrease in the average brightness of the emitting sites; or (ii) a decrease in the number of emitting regions. We attribute these phenomena to the formation of (i) shallow charge traps, which can weakly affect all emitting areas of a single chain at once; and (ii) deep traps, which have a strong effect on small regions within the single chains.

physics.chem-ph↗