arXiv subjects

Michael Meyer

Publications and source records attributed to Michael Meyer.

At least 19 recordsLinked to original sources

arXiv2026

X-ray Driven Trihydrogen Formation on Silica Nanosurfaces

The trihydrogen cation ($\mathrm{H_3^+}$) initiates the ion-molecule reactions that build molecular complexity in interstellar space. Whether its canonical formation reaction, $\mathrm{H_2^+ + H_2 \rightarrow H_3^+ + H}$, proceeds on inorganic surfaces under radiation-driven ionization has remained untested. Here we drive $\mathrm{H_3^+}$ formation on hydrated silica nanoparticles using intense 1.88 keV X-ray pulses, combining ion velocity map imaging, electron time-of-flight spectroscopy, and single-particle coherent diffractive imaging to resolve this chemistry on individual particles. The self-induced surface electric field on the V/nm scale drives interfacial charge transfer and water fragmentation. This field is the dominant parameter governing the relative yields of $\mathrm{H^+}$, $\mathrm{H_2^+}$, and $\mathrm{H_3^+}$ across particle size, composition, and aggregation. Density functional theory and nonadiabatic quantum molecular dynamics simulations trace this field-driven charge transfer, directly analogous to band bending at semiconductor photoelectrodes. These results establish surface-field-driven charge transfer as a unifying mechanism between radiation dominated astrophysical environments and field-driven surface catalysis.

physics.chem-ph↗

arXiv2026

Photoinduced enhancement of chemical shift sensitivity to local vibrations

The advent of novel free-electron laser sources enabling time-resolved x-ray photoelectron spectroscopy (tr-XPS) provides a unique opportunity to monitor local chemical environments in real time by measuring sub-eV shifts in core-electron binding energies. These shifts reflect the interplay between electronic excitation and nuclear motion, an interplay that remains largely unexplored. In our combined theoretical and experimental study of fluoropyridine (C$_5$H$_4$FN), we investigate this link by monitoring the evolving chemical environment at the N and F atomic sites as the photoexcited $S_1$ state relaxes to the ground state via a conical intersection. We find that the F site responds primarily to vibrational relaxation, showing minimal sensitivity to the electronic excited state. In contrast, excitation to $S_1$ induces a measurable energy shift at the N site and significantly enhances its sensitivity to local vibrations within the ring. This behavior arises from a photoinduced redistribution of charge, which also increases the Coulomb interaction between the 1s electron at the N atom and the atomic partial charge at an adjacent C atom. This insight opens new avenues for exploring ultrafast dynamics and conical intersection pathways in more complex systems, from photostable DNA bases to light-harvesting materials.

physics.chem-ph↗

arXiv2026

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics↗

arXiv2026

Two-colour coherent control of nuclear and electron dynamics in photoionization of molecular hydrogen with FEL pulses

The extension of coherent $\omega$-$2\omega$ control schemes, recently implemented in free-electron lasers (FELs), to molecular systems offers new opportunities to control chemical dynamics on the electronic timescale, potentially allowing for the steering of reactions along previously inaccessible pathways. We have implemented such a scheme at the seeded FERMI FEL to retrieve the relative phases between one-photon (frequency $2\omega$) and two-photon (frequency $\omega$) ionization paths in the hydrogen molecule as a function of photoelectron energy and emission angle. The narrow bandwidth of the XUV pulses enables selective excitation of vibrational levels of neutral intermediate H$_2$ states in the two-photon ionization path. Here we focus on $\omega$--$2\omega$ ionization of H$_2(X\,^{1}\Sigma_g^{+},\,v=0)$ into the H$_2^{+}(X\,^{2}\Sigma_g^{+},\,v_f)$ ground state involving the H$_2(B\,^{1}\Sigma_u^{+},\,v'=6)$ intermediate state. The relative phases of the $\omega$ and $2\omega$ interfering photoionization amplitudes exhibit a strong dependence on photoelectron energy, i.e.\ on the final vibrational state $v_f$ in the H$_2^{+}$ cation. With the help of accurate theoretical calculations, the observed phase jumps are assigned to the coupled electronic and nuclear dynamics at play in the two-photon process, significantly influenced by H$_2(^{1}\Sigma_g^{+}$ and $^{1}\Pi_g)$ autoionizing states and the mapping of the H$_2(B\,^{1}\Sigma_u^{+},\,v'=6)$ intermediate-state nuclear wavefunction into the final vibrational states of H$_2^{+}(X\,^{2}\Sigma_g^{+})$. The present work establishes the fundamental concepts required to access coupled electron--nuclear dynamics in molecules using $\omega$--$2\omega$ coherent control schemes currently available at free-electron laser facilities.

physics.chem-ph↗

arXiv2026

Probing the structure of cyclic hydrocarbon molecules with X-ray-induced Coulomb explosion imaging

Coulomb explosion imaging (CEI) is a powerful experimental technique that maps a molecule's geometric structure onto the momenta of ionic molecular fragments produced by rapid multiple ionization. Here, we apply CEI induced by pulses from an X-ray free-electron laser in order to image and distinguish complex hydrocarbon isomers with the chemical formula C7H8: toluene, cycloheptatriene, and 1,6-heptadiyne. The measured fragment-ion momentum distributions show discernible differences between the three isomers and provide signatures of specific carbon and hydrogen sites in the molecule. In contrast to previous work, we demonstrate that distinct 'marker atoms' are not strictly required for constructing a meaningful molecular frame of reference for the interpretation of the momentum-space data. Our work paves the way for tracking the ultrafast motion of nuclei during isomerization reactions in pure hydrocarbons.

physics.chem-ph↗

arXiv2026

Jupiter-like uniform metal enrichment in a system of multiple giant exoplanets

The accretion of icy and rocky solids during the formation of a gas giant planet is poorly constrained and challenging to model. Refractory species, like sulfur, are only present in solids in the protoplanetary disk where planets form. Measuring their abundance in planetary atmospheres is one of the most direct ways of constraining the extent and mechanism of solid accretion. Using the unprecedented sensitivity of NASA's James Webb Space Telescope (JWST), we measure a detailed chemical make-up of three massive gas giants orbiting the star HR~8799 including direct detections of H$_2$O, CO, CH$_4$, CO$_2$, H$_2$S, $^{13}$CO, and C$^{18}$O. We find these planets are uniformly and highly enriched in heavy elements compared to the star irrespective of their volatile (carbon and oxygen) or refractory (sulfur) nature, which strongly suggests efficient accretion of solids during their formation. This composition closely resembles that of Jupiter and Saturn and demonstrates that this enrichment also occurs in systems of multiple gas giant planets orbiting stars beyond the Solar System. This discovery hints at a shared origin for the heavy element enrichment of giant planets across a wider range of planet masses and orbital separations than previously anticipated.

astro-ph.EP↗

arXiv2025

Unraveling real-time chemical shifts in the ultrafast regime

Traditional x-ray photoelectron spectroscopy (XPS) relies upon a direct mapping between the photoelectron binding energies and the local chemical environment, which is well-characterized by an electrostatic partial charges model for systems in equilibrium. However, the extension of this technique to out-of-equilibrium systems has been hampered by the lack of x-ray sources capable of accessing multiple atomic sites with high spectral and temporal resolution, as well as the lack of simple theoretical procedures to interpret the observed signals. In this work we employ multi-site XPS with a narrowband femtosecond x-ray probe to unravel different ultrafast dissociation processes of a polyatomic molecule, fluoromethane (CH$_{3}$F). We show that XPS can follow the cleavage of both the C-F and C-H bonds in real time, despite these channels lying close in binding energy. Additionally, we apply the partial charges model to describe these dynamics, and verify this extension with both advanced ab-initio calculations and experimental data. These results enable the application of this technique to out-of-equilibrium systems of higher complexity, by correlating real-time information from multiple atomic sites and interpreting the measurements through a viable theoretical modelling.

physics.chem-ph↗

arXiv2025

Enhanced One-Color-Two-Photon Resonant Ionization in Highly Charged Ions by Fine-Structure Effects

Ultraintense pulses from X-ray free-electron lasers can drive, within femtoseconds, multiple processes in the inner shells of atoms and molecules in all phases of matter. The ensuing complex ionization pathways of outer-shell electrons from the neutral to the final highly charged states make a comparison with theory enormously difficult. We resolve these pathways by preparing highly charged ions in an electron beam ion trap before exposing them to the pulsed radiation. This reveals how relativistic fine-structure effects shift electronic energies, largely compensate the core-screening potential, and enable the consecutive, resonant absorption of two quasi-monochromatic X-ray photons that would generally be unfeasible. This doubly-resonant channel enhances the efficiency of two-photon ionization by more than two orders of magnitude, dominating in this regime the nonlinear interaction of light and matter with possible application for future precision X-ray metrology.

physics.atom-ph↗

arXiv2025

Generative Modeling Enables Molecular Structure Retrieval from Coulomb Explosion Imaging

Capturing the structural changes that molecules undergo during chemical reactions in real space and time is a long-standing dream and an essential prerequisite for understanding and ultimately controlling femtochemistry. A key approach to tackle this challenging task is Coulomb explosion imaging, which benefited decisively from recently emerging high-repetition-rate X-ray free-electron laser sources. With this technique, information on the molecular structure is inferred from the momentum distributions of the ions produced by the rapid Coulomb explosion of molecules. Retrieving molecular structures from these distributions poses a highly non-linear inverse problem that remains unsolved for molecules consisting of more than a few atoms. Here, we address this challenge using a diffusion-based Transformer neural network. We show that the network reconstructs unknown molecular geometries from ion-momentum distributions with a mean absolute error below one Bohr radius, which is half the length of a typical chemical bond.

physics.chem-ph↗

arXiv2025

The Ethical and Sustainable Concerns Triangle: A Framework for Navigating Discourses in Mathematics and Its Education

The literature on ethics and sustainability in mathematics and its education is increasingly complex and fragmented, potentially leading to communication breakdowns between different scholarly traditions. To address this, the paper introduces the "Ethical and Sustainable Concerns Triangle," a framework that maps discourses based on their relative concern for three areas (represented as three vertices in the triangle): "Mathematics", "Community", and "Society/Planet". By integrating a systems theoretic perspective, we analyse discourses as dynamic systemic reactions to external irritations. Our analysis reveals that the field's fragmentation can be explained by the "location effect": the phenomenon whereby a discourse's position within the triangle shapes its perception and acceptance of other scholarship. By mapping key discourses and educator archetypes, the framework functions as a meta-heuristic tool. Ultimately, it serves not only to facilitate critical reflection but also as a call for the epistemic humility and dialogue needed to advance the field.

math.HO↗

arXiv2025

Wavefront Error Recovery and Companion Identification with the James Webb Space Telescope

The James Webb Space Telescope is orders of magnitude more sensitive than any other facility across the near to mid-infrared wavelengths. Many approved programs take advantage of its highly stable point spread function (PSF) to directly detect faint companions using diverse high-contrast imaging (HCI) techniques. However, periodic re-phasing of the Optical Telescope Element (OTE) is required due to slow thermal drifts distorting to the primary mirror backplane along with stochastic tilt events on individual mirror segments. Many programs utilize observations of a reference star to remove the stellar contribution within an image which can typically take half of the total allocated time. We present a high-contrast imaging technique for the NIRISS instrument that uses the measured wavefront error (WFE) from a phase calibration observation (performed roughly every 48 hours) as prior information in a Bayesian analysis with nested sampling. This technique estimates the WFE of a given observation and simultaneously searches for faint companions, without using a reference star. We estimate the wavefront error for both full aperture and aperture masking interferometry (AMI) imaging modes using three low order Zernike coefficients per mirror segment, using the Hexike basis, to generate synthetic PSFs and compare to simulations. We compare our technique to traditional interferometric analysis in realistic NIRISS F430M simulations both relative to the photon noise limit, and through recovering an injected companion with $\Delta$F430M= 8 mag at 0.2''. With future testing, this technique may save significant amounts of observing time given the results of our current implementation on NIRISS simulations.

astro-ph.IM↗

arXiv2025

Model-free pattern separation of two-color ultrafast X-ray diffraction

Two-color X-ray imaging with Free Electron Laser pulses offers a powerful approach for probing ultrafast structural dynamics in nanoscale systems, combining (near-)atomic spatial resolution with femtosecond temporal precision. The first X-ray pulse captures the object's initial state, while the second, time-delayed pulse records its subsequent evolution. A key challenge lies in disentangling the two patterns simultaneously recorded by the same detector. We demonstrate the realization of this approach on structurally varying nanoscale particles using two X-ray pulses of different photon energies, 1 and 1.2 keV. Sub-micrometer helium nanodroplets generated in vacuum are irradiated by the two X-ray pulses separated in time by up to 750 femtoseconds. Taking advantage of the high photon-energy resolution of the imaging detector, we separate the overlapping diffraction signals by analyzing individual pixel counts and applying pattern recognition. The helium nanodroplets' spherical shape allows us to cross-validate this approach by fitting the radial scattering profiles with Mie solutions for abichromatic field. The excellent agreement between the two methods, particularly in the sparsely illuminated outer regions of the diffraction patterns where high-resolution structural information is encoded, highlights the quality of this approach and its potential for future advanced X-ray movie techniques.

physics.optics↗

arXiv2025

Dichography: Two-frame Ultrafast Imaging from a Single Diffraction Pattern

We experimentally demonstrate that pairs of time-delayed ultrabright and ultrashort X-ray pulses of two different colors, delivered by modern X-ray Free Electron Lasers, can provide two time-delayed snapshots of a sample. We introduce Dichography, a method that algorithmically separates the diffraction signals overlapping on the detector and independently retrieves the two images of the specimen. We employ Dichography to reconstruct two views of individual xenon-doped helium nanodroplets with 20 nm spatial resolution. The consistency of structures observed in both images at delays up to 750 fs provides evidence that, under these illumination conditions, significant structural damage only occurs at longer timescales. We further validate the method by imaging pairs of silver nanoparticles intercepted by the same light pulse. Dichography enables a new class of experiments across physics, chemistry, and materials science, making a significant step toward the original promise of X-ray free-electron lasers to capture ultrafast movies of nanomatter.

physics.optics↗

arXiv2025

MIRAC-5 on the MMT with MAPS: annular groove phase mask N-band coronagraphic upgrade

We describe the coronagraphic upgrade underway for the Mid-Infrared Array Camera-5 (MIRAC-5) to be used with the 6.5-m MMT telescope utilizing the new MMT Adaptive optics exoPlanet characterization System (MAPS). Mid-IR ground-based coronagraphic adaptive-optics-assisted imaging can be a powerful tool for characterizing exoplanet atmospheres and studying protoplanets in formation within circumstellar disks around young stars. In addition to enabling ground-based observations of bright targets in the background limit, high actuator density 1-2 kHz adaptive optics systems can be competitive with JWST in the contrast limit. We have procured an annular groove phase mask (AGPM) and performed preliminary characterization of its on-axis source rejection as a function of wavelength. We present an optimized Lyot Stop design for use with the AGPM using the High-contrast End-to-End Performance Simulator (HEEPS). Future work includes implementing the Quadrant Analysis of Coronagraphic Images for Tip-tilt Sensing (QACITS) control loop algorithm with MAPS. We present the system overview, pupil mask design, and expected performance metrics aligned with our scientific goals, building upon recent advances with MIRAC-5 (Bowens et al. 2025) and MAPS.

astro-ph.IM↗

arXiv2025

Dichroic Electron Emission Patterns from Oriented Helium Ions

We report a joint experimental and theoretical study using a combination of polarization-controlled free-electron-laser (FEL) and near-infra\-red (NIR) pulses in a synchronized two-color photo\-ionization scheme. Excited He$^+$ ions, created by extreme ultraviolet (XUV) circularly polarized radiation from the XUV-FEL FERMI in the oriented $3p\, (m\!=\!+1)$ state, are exposed to circularly polarized 784-nm NIR radiation with peak intensities from $10^{12}\,\rm W/cm^2$ to $\rm 10^{13}\,W/cm^2$. The angular distribution of the ejected electrons exhibit a strong dichroism depending on the NIR intensity. While the co-rotating case is defined by a single path, for the counter-rotating case, there are two dominant pathways whose relative strength and phase difference are determined.

physics.atom-ph↗

arXiv2025

Assessing robustness and bias in 1D retrievals of 3D Global Circulation Models at high spectral resolution: a WASP-76 b simulation case study in emission

High-resolution spectroscopy (HRS) of exoplanet atmospheres has successfully detected many chemical species and is quickly moving toward detailed characterization of the chemical abundances and dynamics. HRS is highly sensitive to the line shape and position, thus, it can detect three-dimensional (3D) effects such as winds, rotation, and spatial variation of atmospheric conditions. At the same time, retrieval frameworks are increasingly deployed to constrain chemical abundances, pressure-temperature (P-T) structures, orbital parameters, and rotational broadening. To explore the multidimensional parameter space, they need computationally fast models that are consequently mostly one-dimensional (1D). However, this approach risks introducing interpretation bias since the planet's true nature is 3D. We investigate the robustness of this methodology at high spectral resolution by running 1D retrievals on simulated observations in emission within an observational framework using 3D Global Circulation Models of the quintessential HJ WASP-76 b. We find that the retrieval broadly recovers conditions present in the atmosphere, but that the retrieved P-T and chemical profiles are not a homogeneous average of all spatial and phase-dependent information. Instead, they are most sensitive to spatial regions with large thermal gradients, which do not necessarily coincide with the strongest emitting regions. Our results further suggest that the choice of parameterization for the P-T and chemical profiles, as well as Doppler offsets among opacity sources, impact retrieval results. These factors should be carefully considered in future retrieval analyses.

astro-ph.EP↗

arXiv2025

Nonlinear reversal of photo-excitation on the attosecond time scale improves ultrafast x-ray diffraction images

The advent of isolated and intense sub-femtosecond X-ray pulses enables tracking of quantummechanical motion of electrons in molecules and solids. The combination of X-ray spectroscopy and diffraction imaging is a powerful approach to visualize non-equilibrium dynamics in systems beyond few atoms. However, extreme x-ray intensities introduce significant electronic damage, limiting material contrast and spatial resolution. Here we show that newly available intense subfemtosecond (sub-fs) x-ray FEL pulses can outrun most ionization cascades and partially reverse x-ray damage through stimulated x-ray emission in the vicinity of a resonance. In our experiment, we compared thousands of coherent x-ray diffraction patterns and simultaneously recorded ion spectra from individual Ne nanoparticles injected into the FEL focus. Our experimental results and theoretical modeling reveal that x-ray diffraction increases and the average charge state decreases in particles exposed to sub-fs pulses compared to those illuminated with 15-femtosecond pulses. Sub-fs exposures outrun most Auger decays and impact ionization processes, and enhance nonlinear effects such as stimulated emission, which cycle bound electrons between different states. These findings demonstrate that intense sub-fs x-ray FEL pulses are transformative for advancing high-resolution imaging and spectroscopy in chemical and material sciences, and open the possibilities of coherent control of the interaction between x-rays and complex specimen beyond few atoms.

physics.optics↗

arXiv2025

Evaluation of Modular Polynomials from Supersingular Elliptic Curves

We present several new algorithms to evaluate modular polynomials of level $\ell$ modulo a prime $p$ on an input $j$. More precisely, we introduce two new generic algorithms, sharing the following similarities: they are based on a CRT approach; they make use of supersingular curves and the Deuring correspondence; and, their memory requirements are optimal. The first algorithm combines the ideas behind a hybrid algorithm of Sutherland in 2013 with a recent algorithm to compute modular polynomials using supersingular curves introduced in 2023 by Leroux. The complexity (holding around several plausible heuristic assumptions) of the resulting algorithm matches the $\Tilde{O}(\ell^3 \log^{3} \ell + \ell \log p)$ time complexity of the best known algorithm by Sutherland, but has an optimal memory requirement. Our second algorithm is based on a sub-algorithm that can evaluate modular polynomials efficiently on supersingular $j$-invariants defined over $\Fp$, and achieves heuristic complexity quadratic in both $\ell$ and $\log j$, and linear in $\log p$. In particular, it is the first generic algorithm with optimal memory requirement to obtain a quadratic complexity in~$\ell$. Additionally, we show how to adapt our method to the computation of other types of modular polynomials such as the one stemming from Weber's function. Finally, we provide an optimised implementation of the two algorithms detailed in this paper, though we emphasise that various modules in our codebase may find applications outside their use in this paper.

math.NT↗