arXiv subjects

Thomas Feurer

Publications and source records attributed to Thomas Feurer.

At least 19 recordsLinked to original sources

arXiv2026

Time-resolved THz Stark spectroscopy of molecules in water

Stark spectroscopy is a powerful method for probing molecular dipole moment changes, charge transfer dynamics, and polarizability under applied electric fields. Time-Resolved Terahertz Stark Spectroscopy (TRTSS), which employs intense single-cycle terahertz (THz) pulses to induce transient Stark shifts, overcomes key limitations of conventional approaches. Unlike static or low-frequency fields, THz pulses oscillate much faster than typical molecular rotation times, effectively preventing dipole reorientation and enabling measurements in solutions at ambient conditions. Here, we extend TRTSS to molecules dissolved in water, the most important polar solvent for chemical and biological systems and report the first demonstration of Stark spectroscopy in water at room temperature. Using Malachite Green and Methyl Orange as model systems, we observe clear THz-induced spectral modulations, demonstrating that TRTSS can successfully reveal THz Stark responses even in highly polar, hydrogen-bonded environments. Measured signals exhibit a combination of linear (dipole-driven) and quadratic (polarizability-driven) Stark effects in both systems, consistent with time-dependent density functional theory (TD-DFT) calculations. Comparison with TD-DFT further suggests that conformational effects can influence the extracted Stark parameters in solvated molecules.

physics.chem-ph↗

arXiv2026

Anharmonic phonon coupling enabled by local inversion symmetry breaking at domain walls in ferroelastics

In ferroelastic materials, spontaneous symmetry breaking leads to the formation of twin domains. Although the bulk crystal typically remains centrosymmetric, inversion symmetry can be locally broken at the domain walls, potentially changing phonon selection rules and enabling local anharmonic phonon coupling. Here we report direct evidence of such anharmonic coupling in ferroelastic LaAlO$_3$ using two-dimensional Raman-terahertz spectroscopy. We attribute the cross-peaks observed in the two-dimensional spectra to both mechanical and electrical anharmonicity between the $A_{1g}$ Raman-active phonon and the $E_g$ phonon, which acquires finite infrared activity through local inversion symmetry breaking at ferroelastic domain walls. These findings provide new insight into the complex lattice dynamics of ferroelastic materials and highlight the potential of two-dimensional Raman-terahertz spectroscopy to uncover subtle symmetry breaking through the detection of intrinsically weak anharmonic signals.

cond-mat.mtrl-sci↗

arXiv2026

An accurate theoretical framework for the optical and electronic properties of paracyclophanes

Aromatic $\pi$-stacking interactions play an important role in both natural and artificial systems, influencing processes such as charge separation in photosynthesis and charge transport in organic semiconductors. Controlling the geometry and distance between aromatic units is therefore crucial for tuning intermolecular interactions and charge-transfer efficiency. Due to their well-defined stacking geometry, paracyclophanes (PCPs) composed of two or more aromatic units connected by rigid linkers, provide an ideal platform for a systematic study of such effects. Despite extensive experimental studies of PCPs, a comprehensive and quantitatively validated theoretical description linking the structure with the electronic and optical properties is still missing. Here, we present an extensive computational and experimental investigation of the electronic and optical properties of homo-PCPs containing naphthalene diimide (NDI) or pyrene chromophores linked by bridges of varying length and rigidity. We introduce a robust methodology for an accurate simulation of the absorption and fluorescence spectra of PCPs based on a combined TD-DFT and CC2 approach, achieving excellent quantitative agreement with experiment. We also present and validate a fragment-based description of PCPs using the Frenkel exciton model. Such approach is valuable not only for interpretation of the electronic and optical properties of PCPs, but it can also significantly reduce the cost of the calculation while maintaining the accuracy of the supermolecular approach. This work establishes a quantitatively reliable framework linking structure, excitonic coupling, and charge-transfer interactions in PCPs with optical properties, providing design principles for next-generation optoelectronic materials.

physics.chem-ph↗

arXiv2026

Spin waves excited by hard x-ray transient gratings

Recent progress in ultrafast x-ray sources helped establish x-rays as an important tool for probing lattice and magnetic dynamics initiated by femtosecond optical pulses. Here, we explore the potential of ultrashort hard x-ray pulses for driving magnetic dynamics. We use a transient grating technique in which a spatially periodic x-ray excitation pattern gives rise to material excitations at a well-defined wave vector, whose dynamics are monitored via diffraction of an optical probe pulse. The excitation of a ferrimagnetic gadolinium bismuth iron garnet film placed in an external tilted magnetic field by x-rays at the Gd L3 edge results in both magnetic and non-magnetic transient gratings whose contributions to the diffracted signal are separated by polarization analysis. We observe the magnetization precession at both longitudinal acoustic and spin wave frequencies. An analysis with the Landau-Lifshitz-Gilbert equation indicates that the magnetization precession is driven by strain resulting from thermal expansion induced by absorbed x-rays. The results establish x-ray transient gratings as a tool for driving coherent phonons and magnons, with the potential of accessing wave vectors across the entire Brillouin zone.

physics.optics↗

arXiv2024

Coherent all X-ray four wave mixing at core shell resonances

Nonlinear wave mixing in the X-ray range can provide valuable insights into the structural and electron dynamics of atomic and molecular systems on ultrafast time scales, with state- and site-selectivity and atomic resolution. This promising experimental toolbox was so far limited by requiring at least one near-visible laser, thus preventing core-shell two-dimensional X-ray spectroscopy. In this work, we demonstrate the generation of background-free all-X-ray four-wave mixing (XFWM) signals from a dilute gaseous sample (Ne). The measured and simulated two-dimensional spectral maps ($\omega_{\text{in}},\omega_{\text{out}}$) show multiple contributions involving the coherent response from core electrons. Notably, two-color resonant XFWM signals, essential for generalized multi-color schemes that allow to locally probe the electronic excitation of matter, are observed in neutral Ne. Moreover, stimulated Ne$^+$ emission in each of the propagating X-ray pulses leads to an increase of the temporal coherence in a narrow-bandwidth, which results in the coherent mixing of three X-ray lasers. Preliminary X-ray excitation experiments making use of multi-color time-delayed X-ray pulses demonstrate temporal resolution capability and show a time dependency consistent with a signal dominated by resonant XFWM processes. This first all-X-ray four-wave-mixing approach represents a major breakthrough towards multidimensional X-ray correlation spectroscopy and the general application of nonlinear all-X-ray wave-mixing.

physics.optics↗

arXiv2022

Time-resolved THz Stark spectroscopy

We introduce THz Stark spectroscopy by using intense single-cycle terahertz pulses as the electric field source and monitoring the induced spectral response of an isotropic molecular ensemble with a coincident femtosecond supercontinuum pulse. THz Stark spectroscopy offers several advantages over conventional Stark spectroscopy and opens previously inaccessible perspectives. Most importantly, THz pulses oscillate faster than typical molecular rotations and consequently eliminate the requirement to freeze the samples to prevent poling effects. Hence, THz Stark spectroscopy allows for time-resolved studies at arbitrary temperatures, specifically ambient conditions more relevant to physiological or operative conditions. Moreover, dynamical field effects, e.g., higher order Stark contributions or hysteresis effects (non-Markovian behavior), can be studied on the time scales of molecular vibrations or rotations. We demonstrate THz Stark spectroscopy for two judiciously selected molecular systems and compare the results to conventional Stark spectroscopy and first principle calculations.

physics.optics↗

arXiv2022

Wideband dispersion-free THz waveguide platform

We present an integrated THz spectroscopy and sensing platform featuring low loss, vacuum-like dispersion, and strong field confinement in the fundamental mode. Its performance was characterized experimentally for frequencies between 0.1 THz and 1.5 THz. While linear THz spectroscopy and sensing gain mostly from low loss and an extended interaction length, nonlinear THz spectroscopy would also profit from the field enhancement associated to strong mode confinement. Moreover, the vacuum-like dispersion allows for a reshaping-free propagation of broadband single- to few-cycle pulses in gas-phase samples or velocity matching between THz pump and visible to infrared probe pulses. Our platform is based on a metallic structure and falls in the category of double ridged waveguides. We characterize essential waveguide properties, for instance, propagation and bending losses, but also demonstrate junctions and interferometers, essentially because those elements are prerequisites for integrated THz waveform synthesis, and hence, for coherently controlled linear and nonlinear interactions.

physics.optics↗

arXiv2022

Structure, Organization and Heterogeneity of Water-Containing Deep Eutectic Solvents

The spectroscopy and structural dynamics of a deep eutectic mixture (KSCN/acetamide) with varying water content is investigated from 2D IR (with the C-N stretch vibration of the SCN$^-$ anions as the reporter) and THz spectroscopy. Molecular dynamics simulations correctly describe the non-trivial dependence of both spectroscopic signatures depending on water content. For the 2D IR spectra, the MD simulations relate the steep increase in the cross relaxation rate at high water content to parallel alignment of packed SCN$^-$ anions. Conversely, the non-linear increase of the THz absorption with increasing water content is mainly attributed to the formation of larger water clusters. The results demonstrate that a combination of structure sensitive spectroscopies and molecular dynamics simulations provides molecular-level insights into emergence of heterogeneity of such mixtures by modulating their composition.

physics.chem-ph↗

arXiv2022

Metastable defects decrease the fill factor of solar cells

Cu(In,Ga)Se2 based solar cells exceed power conversion efficiencies of 23 %. Yet, the fill factor of these solar cells, with best values around 80 %, is relatively low (Si reaches 84.9%) mostly due to diode factors greater than one. Recently, we proposed metastable defects, a general feature of the Cu(In,Ga)Se2 alloy, to be the origin of the increased diode factor. We measure the diode factor of the bare absorber layers by excitation-dependent photoluminescence. For high quality and thus high luminescent polycrystalline absorbers, we evaluate the diode factor excitation dependence over four orders of magnitude. Using simulations and the model of metastable defects, we can well describe the experimental findings on n- and p-type epitaxial films as well as the polycrystalline absorbers, providing additional evidence for this model. We find that the diode factors measured optically by photoluminescence impose a lower limit for the diode factor measured electrically on a finished solar cell. Interestingly, the lowest diode factor (optical and electrical) and consequently highest fill factor of 81.0 % is obtained by Ag alloying, i.e. an (Ag,Cu)(In,Ga)Se2 absorber. This finding hints to a pathway to increase fill factors and thus efficiencies for Cu(In,Ga)Se2-based solar cells.

cond-mat.mtrl-sci↗

arXiv2020

Generalized spectral phase-only time-domain ptychographic phase reconstruction applied in nonlinear microscopy

Nonlinear microscopy has evolved over the last few decades to become a powerful tool for imaging and spectroscopic applications in biological sciences. In this study, I$^2$PIE, a novel spectral phase control technique, was implemented in order to compress broad-bandwidth supercontinuum light pulses generated in an all-normal-dispersion (ANDi) photonic crystal fiber (PCF). The technique, based on time-domain ptychography, is demonstrated here in a nonlinear microscopy application for the first time, to the best of our knowledge. The first real-world application of this technique for second-harmonic generation and two-photon excitation fluorescence microscopies in biological samples is presented. We further show that in our implementation, I$^2$PIE leads to improved contrast and signal-to-noise ratios in the generated images, compared to conventional compression techniques used in nonlinear microscopy.

physics.optics↗

arXiv2020

Implementation of temporal ptychography algorithm, I$^2$PIE, for improved single-beam coherent anti-Stokes Raman scattering measurements

We present an improvement on the signal-to-background of single-beam coherent anti-Stokes Raman scattering (SB-CARS) spectroscopy measurements for systems employing ultrafast supercontinuum sources based on all-normal dispersion photonic crystal fibers. Improvements to the signal-to-background arise in the use of a new pulse-reconstruction algorithm based on temporal ptychography, I$^2$PIE. A simple SB-CARS strategy is used to measure the spectrum of para-xylene, where the supercontinuum pulses used are compressed using multiphoton intrapulse interference phase scan (MIIPS) and, for the first time to the best of our knowledge, I$^2$PIE using the same single-beam setup. With the I$^2$PIE implementation, the signal-to-background is improved by nearly a factor of 4 in comparison with MIIPS. More notably, the integrated SB-CARS spectral intensity is increased by a factor of 6.5.

physics.optics↗

arXiv2019

Low noise all-fiber amplification of a coherent supercontinuum at 2 μm and its limits imposed by polarization noise

We report the amplification of an all-normal dispersion supercontinuum pulse in a Thulium / Holmium co-doped all-fiber chirped pulse amplification system. With a -20 dB bandwidth of more than 300 nm in the range 1800-2100 nm the system delivers high quality 66 fs pulses with more than 70 kW peak power directly from the output fiber. The coherent seeding of the entire emission bandwidth of the doped fiber and the stability of the supercontinuum generation dynamics in the silicate glass all-normal dispersion photonic crystal fiber result in excellent noise characteristics of the amplified ultrashort pulses.

physics.optics↗

arXiv2019

Flexible perovskite/Cu(In,Ga)Se2 monolithic tandem solar cells

We report a proof-of-concept two-terminal perovskite/Cu(In, Ga)Se2 (CIGS) monolithic thin-film tandem solar cell grown on ultra-thin (30-microns thick), light-weight, and flexible polyimide foil with a steady-state power conversion efficiency of 13.2% and a high open-circuit voltage over 1.75 V under standard test condition.

physics.app-ph↗

arXiv2019

Extending time-domain ptychography to generalized phase-only transfer functions

We extend the time-domain ptychographic iterative engine to generalized spectral phase-only transfer functions. The modified algorithm, i$^2$PIE, is described and its robustness is demonstrated by different numeric simulations. The concept is experimentally verified by reconstruction of a complex supercontinuum pulse from an all normal dispersion fiber.

eess.SP↗

arXiv2018

Dispersion Measurement of Ultra-High Numerical Aperture Fibers covering Thulium, Holmium, and Erbium Emission Wavelengths

We present broadband group velocity dispersion (GVD) measurements of commercially available ultra-high numerical aperture fibers (UHNA1, UHNA3, UHNA4, UHNA7 and PM2000D from Coherent-Nufern). Although these fibers are attractive for dispersion management in ultrafast fiber laser systems in the 2 μm wavelength region, experimental dispersion data in literature is scarce and inconsistent. Here we demonstrate the measurements using the spectral interferometry technique covering the typically used erbium, thulium and holmium emission bands. The results are characterized in terms of the standard-deviation uncertainty and compared with previous literature reports. Fitting parameters are provided for each fiber allowing for the straightforward replication of the measured dispersion profiles. This work is intended to facilitate the design of ultrafast fiber laser sources and the investigations of nonlinear optical phenomena.

physics.ins-det↗

arXiv2016

Measurement of complex supercontinuum light pulses using time domain ptychography

We demonstrate that time-domain ptychography, a recently introduced ultrafast pulse reconstruction modality, has properties ideally suited for the temporal characterization of complex light pulses with large time-bandwidth products as it achieves temporal resolution on the scale of a single optical cycle using long probe pulses, low sampling rates, and an extremely fast and robust algorithm. In comparison to existing techniques, ptychography minimizes the data to be recorded and processed, and drastically reduces the computational time of the reconstruction. Experimentally we measure the temporal waveform of an octave-spanning, 3.5~ps long supercontinuum pulse generated in photonic crystal fiber, resolving features as short as 5.7~fs with sub-fs resolution and 30~dB dynamic range using 100~fs probe pulses and similarly large delay steps.

physics.optics↗

arXiv2016

All optical implementation of a time-domain ptychographic pulse reconstruction set-up

An all optical implementation of pulse reconstruction using time-domain ptychography is demonstrated showing excellent results. Setup and reconstruction are easy to implement and a number of drawbacks found in other second order techniques are removed, such as the beam splitter modifying the pulse under consideration, the time ambiguity, or the strict correspondence between time delay increment and temporal resolution. Ptychography generally performs superior to algorithms based on general projections, requires considerable less computational effort and is much less susceptible to noise.

physics.optics↗

arXiv2015

Time-domain ptychography

Through dedicated measurements in the optical regime we demonstrate that ptychography can be applied to reconstruct complex-valued object functions that vary with time from a sequence of spectral measurements. A probe pulse of approximately 1 ps duration, time delayed in increments of 0.25 ps is shown to recover dynamics on a ten times faster time scale with an experimental limit of approximately 5 fs.

physics.optics↗