arXiv subjects

Wieland Schöllkopf

Publications and source records attributed to Wieland Schöllkopf.

12 recordsLinked to original sources

arXiv2026

Non-equilibrium state during proton-deuteron exchange at a liquid-liquid interface

Proton-deuteron exchange is a very fast process, even across macroscopic length scales. Here we directly and quantitatively measure the formation of HDO within the first 100 microseconds of the reaction at the liquid-liquid interface between D$_2$O and H$_2$O, using a fast-flowing liquid flat jet combined with infrared spectroscopic imaging. We demonstrate that, at early stages HDO formation is reaction-limited, set by the low concentration of the hydroxide and hydronium ions that mediate the exchange. As the ion concentration rises, the rate rapidly approaches the diffusion limit. The reaction rate constant we extract is consistent with the picosecond timescale of the elementary proton-deuteron exchange. Access to these microsecond kinetics reveals a non-equilibrium state in the early H$_2$O/D$_2$O interface: the two liquids are fully mixed by diffusion, yet the HDO concentration remains well below equilibrium. Quantitative imaging of reactant and product concentrations at well-defined liquid-liquid interfaces, as introduced here, will enable the study of fast kinetics across a wide range of chemical reactions.

physics.chem-ph↗

arXiv2026

A two-color dual-oscillator infrared free-electron laser

We report on the design and performance of a two-color dual-oscillator infrared free-electron laser (FEL). The mid-infrared (MIR) FEL at the Fritz Haber Institute (FHI FEL) has been upgraded to include a second oscillator FEL beamline that permits lasing in the far-infrared (FIR) regime from 4.5 μm to 175 μm. In addition, a 500 MHz kicker cavity has been installed downstream of the electron accelerator. It allows to deflect electron bunches of up to 50 MeV energy alternately left and right by an angle of {\pm}2°. It can, thus, split the high-repetition-rate (1 GHz) electron bunch train from the accelerator into two bunch trains of 500 MHz repetition rate each; one is steered to the MIR FEL and the other one to the new FIR FEL. In this two-color mode of simultaneous, synchronized operation the wavelengths in both FELs can be tuned independently over wide ranges of up to a factor of four each by undulator-gap variation. In addition, two-color operation is also available at reduced repetition rates (e.g. 55.6 MHz of both MIR and FIR pulses), as needed for some applications. This unique two-color mode opens up a wealth of novel user applications such as, MIR-FIR pump-probe experiments.

physics.acc-ph↗

arXiv2026

Controlling isomer population using a dual-oscillator infrared free-electron laser

We report on the control and characterization of the isomer population of ions inside superfluid helium nanodroplets, using two-color operation of a dual-oscillator infrared free-electron laser. The timing of both lasers is highly synchronized, and their frequencies (or "colors") can be tuned independently over a wide range. Interaction of the singly deuterated proton-bound dimer of dihydrogen phosphate and formate inside helium nanodroplets with both colors enables the control over its isomer population and the recording of - one-color hidden - infrared spectra of individual isomers.

physics.chem-ph↗

arXiv2024

Comprehensive peak-width analysis in matter-wave diffraction under grazing incidence conditions

Thermal energy atom scattering at a surface with grazing incidence conditions is an innovative method for investigating dispersive atom-surface interactions with potential application in quantum sensing interferometry. The complete establishment of this technique would require a detailed peak analysis, which has yet to be achieved. We examined peak-width fluctuations in atomic and molecular beams diffracted by a grating under grazing incidence conditions. Careful measurements and analyses of the diffraction patterns of He atoms and D$_2$ molecules from three square-wave gratings with different periods and radii of curvature enabled the identification of factors influencing the variations in the width as a function of the grazing incidence angle. The effects of macroscopic surface curvature, grating magnification, and beam emergence are substantial under these conditions but negligible for incidence angles close to the normal. Our results shed light on the phenomena occurring in grazing incidence thermal energy atom scattering.

physics.atom-ph↗

arXiv2021

Infrared super-resolution wide-field microscopy using sum-frequency generation

Super-resolution microscopy in the visible is an established powerful tool in several disciplines. In the infrared (IR) spectral range, however, no comparable schemes have been demonstrated to date. In this work, we experimentally demonstrate super-resolution microscopy in the IR range ($λ_{IR}\approx 10-12\,μ$m) using IR-visible sum-frequency generation. We operate our microscope in a wide-field scheme and image localized surface phonon polaritons in 4H-SiC nanostructures as a proof-of-concept. With this technique, we demonstrate an enhanced spatial resolution of $\simλ_{IR}/9$, enabling to resolve the polariton resonances in individual sub-diffractional nanostructures with sub-wavelength spacing. Furthermore we show, that this resolution allows to differentiate between spatial patterns associated with different polariton modes within individual nanostructures.

physics.optics↗

arXiv2018

Second-harmonic phonon spectroscopy of $α$-quartz

We demonstrate midinfrared second-harmonic generation as a highly sensitive phonon spectroscopy technique that we exemplify using $α$-quartz (SiO$_2$) as a model system. A midinfrared free-electron laser provides direct access to optical phonon resonances ranging from $350\ \mathrm{cm}^{-1}$ to $1400\ \mathrm{cm}^{-1}$. While the extremely wide tunability and high peak fields of an free-electron laser promote nonlinear spectroscopic studies---complemented by simultaneous linear reflectivity measurements---azimuthal scans reveal crystallographic symmetry information of the sample. Additionally, temperature-dependent measurements show how damping rates increase, phonon modes shift spectrally and in certain cases disappear completely when approaching $T_c=846\ \mathrm{K}$ where quartz undergoes a structural phase transition from trigonal $α$-quartz to hexagonal $β$-quartz, demonstrating the technique's potential for studies of phase transitions.

cond-mat.mtrl-sci↗

arXiv2017

Second Harmonic Generation from Critically Coupled Surface Phonon Polaritons

Mid-infrared nanophotonics can be realized using sub-diffractional light localization and field enhancement with surface phonon polaritons in polar dielectric materials. We experimentally demonstrate second harmonic generation due to the optical field enhancement from critically coupled surface phonon polaritons at the 6H-SiC-air interface, employing an infrared free-electron laser for intense, tunable, and narrowband mid-infrared excitation. Critical coupling to the surface polaritons is achieved using a prism in the Otto geometry with adjustable width of the air gap, providing full control over the excitation conditions along the polariton dispersion. The calculated reflectivity and second harmonic spectra reproduce the full experimental data set with high accuracy, allowing for a quantification of the optical field enhancement. We also reveal the mechanism for low out-coupling efficiency of the second harmonic light in the Otto geometry. Perspectives on surface phonon polariton-based nonlinear sensing and nonlinear waveguide coupling are discussed.

physics.optics↗

arXiv2016

Resonant enhancement of second harmonic generation in the mid-infrared using localized surface phonon polaritons in sub-diffractional nanostructures

We report on strong enhancement of mid-infrared second harmonic generation (SHG) from SiC nanopillars due to the resonant excitation of localized surface phonon-polaritons within the Reststrahlen band. The magnitude of the SHG peak at the monopole mode experiences a strong dependence on the resonant frequency beyond that described by the field localization degree and the dispersion of linear and nonlinear-optical SiC properties. Comparing the results for the identical nanostructures made of 4H and 6H SiC polytypes, we demonstrate the interplay of localized surface phonon polaritons with zone-folded weak phonon modes of the anisotropic crystal. Tuning the monopole mode in and out of the region where the zone-folded phonon is excited in 6H-SiC, we observe a prominent increase of the already monopole-enhanced SHG output when the two modes are coupled. Envisioning this interplay as one of the showcase features of mid-infrared nonlinear nanophononics, we discuss its prospects for the effective engineering of nonlinear-optical materials with desired properties in the infrared spectral range.

physics.optics↗

arXiv2015

Observation of the Efimov state of the helium trimer

Quantum theory dictates that upon weakening the two-body interaction in a three-body system, an infinite number of three-body bound states of a huge spatial extent emerge just before these three-body states become unbound. Three helium atoms have been predicted to form a molecular system that manifests this peculiarity under natural conditions without artificial tuning of the attraction between particles by an external field. Here we report experimental observation of this long predicted but experimentally elusive Efimov state of $^{4}$He$_{3}$ by means of Coulomb explosion imaging. We show spatial images of an Efimov state, confirming the predicted size and a typical structure where two atoms are close to each other while the third is far away.

physics.atm-clus↗

arXiv2010

Coherent reflection of He atom beams from rough surfaces at near-grazing incidence

We here report coherent reflection of thermal He atom beams from various microscopically rough surfaces at grazing incidence. For a sufficiently small normal component $k_z$ of the incident wave-vector of the atom the reflection probability is found to be a function of $k_z$ only. This behavior is explained by quantum-reflection at the attractive branch of the Casimir-van der Waals interaction potential. For larger values of $k_z$ the overall reflection probability decreases rapidly and is found to also depend on the parallel component $k_x$ of the wave-vector. The material specific $k_x$ dependence for this classical reflection at the repulsive branch of the potential is explained qualitatively in terms of the averaging-out of the surface roughness under grazing incidence conditions.

physics.atom-ph↗

arXiv2010

Emerging beam resonances in atom diffraction from a reflection grating

We report on the observation of emerging beam resonances, well known as Rayleigh-Wood anomalies and threshold resonances in photon and electron diffraction, respectively, in an atom-optical diffraction experiment. Diffraction of He atom beams reflected from a blazed ruled grating at grazing incidence has been investigated. The total reflectivity of the grating as well as the intensities of the diffracted beams reveal anomalies at the Rayleigh angles of incidence, i.e., when another diffracted beam merges parallel to the grating surface. The observed anomalies are discussed in terms of the classical wave-optical model of Rayleigh and Fano.

physics.atom-ph↗

arXiv2008

Quantum reflection of helium atom beams from a microstructured grating

We observe high-resolution diffraction patterns of a thermal-energy helium-atom beam reflected from a microstructured surface grating at grazing incidence. The grating consists of 10-$μ$m-wide Cr strips patterned on a quartz substrate and has a periodicity of 20 $μ$m. Fully-resolved diffraction peaks up to the $7^{\rm th}$ order are observed at grazing angles up to 20 mrad. With changes in de Broglie wavelength or grazing angle the relative diffraction intensities show significant variations which shed light on the nature of the atom-surface interaction potential. The observations are explained in terms of quantum reflection at the long-range attractive Casimir-van der Waals potential.

physics.atom-ph↗