arXiv subjects

Wolfgang Theis

Publications and source records attributed to Wolfgang Theis.

4 recordsLinked to original sources

arXiv2026

Near-Field Vibrational Energy Transfer for Mid-Infrared Upconversion in Plasmonic Nanogaps

Förster energy transfer underpins modern photonics, yet establishing an analogous vibrational pathway in the mid-infrared (MIR) remains highly challenging, as sub-picosecond intramolecular vibrational redistribution (IVR) suppresses intermolecular coupling. Here we demonstrate vibrational donor--acceptor transfer in the MIR and subsequent upconversion to visible luminescence enabled by sub-2 nm plasmonic nanogaps. The extreme lateral field confinement in metal--molecule--metal ring cavities defined by self-assembled molecular spacers couples efficiently to in-plane molecular dipoles. Continuous-wave MIR excitation selectively populates $-\mathrm{C}\equiv\mathrm{N}$ vibrational donors, and plasmon-enhanced near-field coupling transfers this energy to nearby electronic acceptors, generating anti-Stokes visible emission under low power densities. Upconversion efficiencies exceeding $0.3\%$ are observed, limited by competition between the plasmon-mediated transfer rate and IVR. These results show that extreme plasmonic confinement can redirect molecular vibrational relaxation pathways, opening a route toward vibrational nanophotonics, intermolecular interactions for bioimaging, and room-temperature MIR detection based on molecular degrees of freedom.

physics.optics↗

arXiv2023

Advanced Techniques in Automated High Resolution Scanning Transmission Electron Microscopy

Scanning transmission electron microscopy is a common tool used to study the atomic structure of materials. It is an inherently multimodal tool allowing for the simultaneous acquisition of multiple information channels. Despite its versatility, however, experimental workflows currently rely heavily on experienced human operators and can only acquire data from small regions of a sample at a time. Here, we demonstrate a flexible pipeline-based system for high-throughput acquisition of atomic-resolution structural data using a custom built sample stage and automation program. The program is capable of operating over many hours without human intervention improving the statistics of high-resolution experiments.

physics.ins-det↗

arXiv2022

Revealing 3-dimensional core-shell interface structures at the single-atom level

Nanomaterials with core-shell architectures are prominent examples of strain-engineered materials, where material properties can be designed by fine-tuning the misfit strain at the interface. Here, we elucidate the full 3D atomic structure of Pd@Pt core-shell nanoparticles at the single-atom level via atomic electron tomography. Full 3D displacement fields and strain profiles of core-shell nanoparticles were obtained, which revealed a direct correlation between the surface and interface strain. It also showed clear Poisson effects at the scale of the full nanoparticle as well as the local atomic bonds. The strain distributions show a strong shape-dependent anisotropy, whose nature was further corroborated by molecular statics simulations. From the observed surface strains, the surface oxygen reduction reaction activities were predicted. These findings give a deep understanding of structure-property relationships in strain-engineerable core-shell systems, which could pave a new way toward direct control over the resulting catalytic properties.

cond-mat.mtrl-sci↗

arXiv2016

Nanomaterial datasets to advance tomography in scanning transmission electron microscopy

Electron tomography in materials science has flourished with the demand to characterize nanoscale materials in three dimensions (3D). Access to experimental data is vital for developing and validating reconstruction methods that improve resolution and reduce radiation dose requirements. This work presents five high-quality scanning transmission electron microscope (STEM) tomography datasets in order to address the critical need for open access data in this field. The datasets represent the current limits of experimental technique, are of high quality, and contain materials with structural complexity. Included are tomographic series of a hyperbranched Co2P nanocrystal, platinum nanoparticles on a carbon nanofibre imaged over the complete 180° tilt range, a platinum nanoparticle and a tungsten needle both imaged at atomic resolution by equal slope tomography, and a through-focal tilt series of PtCu nanoparticles. A volumetric reconstruction from every dataset is provided for comparison and development of post-processing and visualization techniques. Researchers interested in creating novel data processing and reconstruction algorithms will now have access to state of the art experimental test data.

cond-mat.mes-hall↗