SearcharxivSearch

arXiv subjects

Paul Tuemmler

Publications and source records attributed to Paul Tuemmler.

2 recordsLinked to original sources

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

Fast Simulation of Wide-Angle Coherent Diffractive Imaging

Single-shot coherent diffractive imaging (CDI) using intense XUV and soft X-ray pulses holds the promise to deliver information on the three dimensional shape as well as the optical properties of nano-scale objects in a single diffraction image. This advantage over conventional X-ray diffraction methods comes at the cost of a much more complex description of the underlying scattering process due to the importance of wide-angle scattering and propagation effects. The commonly employed reconstruction of the sample properties via iterative forward fitting of diffraction patterns requires an accurate and fast method to simulate the scattering process. This work introduces the propagation multi-slice Fourier transform method (pMSFT) and demonstrates its superior performance and accuracy against existing methods for wide-angle scattering. A derivation from first principles, a unified physical picture of the approximations underlying pMSFT and the existing methods, as well as a systematic benchmark that provides qualified guidance for the selection of the appropriate scattering method is presented.

physics.optics