arXiv subjects

Sebastian Kaiser

Publications and source records attributed to Sebastian Kaiser.

4 recordsLinked to original sources

arXiv2026

Efficient purely organic phosphorescent emitters for programmable luminescent tags: from building blocks to donor-acceptor-donor structures

Purely organic room-temperature phosphorescence (RTP) emitters are key components of programmable luminescent tags (PLTs), photonic devices for rewritable information storage and UV dosimetry. In this work, we systematically explore the design space of donor-acceptor and donor-acceptor-donor organic phosphorescent emitters in symmetric and asymmetric architectures. Phenoxathiine (PX) is introduced as an alternative donor to thianthrene (TA), combined with benzophenone (BP) or pyridine (Py) as acceptors. Through photophysical characterization, quantum chemical simulations, and PLT device testing, we identify structure-property relationships and, in particular, investigate the impact of the individual moieties on the emission properties and stability. The RTP emission wavelength is primarily tunable through the donor moiety: PX-based emitters emit sky-blue ({\lambda}_P = 480 nm), while TA-based emitters emit in the green ({\lambda}_P = 520 nm) due to an increased Stokes shift. The acceptor unit strongly influences the phosphorescence quantum yield, with Py-based emitters systematically outperforming BP-based ones. All newly synthesized PX-containing emitters show sufficient performance in PLT devices, though with reduced photostability compared to TA-based counterparts. Together, these results demonstrate that systematic donor-acceptor design enables predictable control over RTP emission properties, advancing the rational development of high-performance RTP-based photonic devices.

cond-mat.mtrl-sci↗

arXiv2023

On-Surface Carbon Nitride Growth from Polymerization of 2,5,8-Triazido-s-heptazine

Carbon nitrides have recently come into focus for photo- and thermal catalysis, both as support materials for metal nanoparticles as well as photocatalysts themselves. While many approaches for the synthesis of three-dimensional carbon nitride materials are available, only top-down approaches by exfoliation of powders lead to thin film flakes of this inherently two-dimensional material. Here, we describe an in situ on-surface synthesis of monolayer 2D carbon nitride films, as a first step towards precise combination with other 2D materials. Starting with a single monomer precursor, we show that 2,5,8-triazido-s-heptazine (TAH) can be evaporated intact, deposited on a single crystalline Au(111) or graphite support, and activated via azide decomposition and subsequent coupling to form a covalent polyheptazine network. We demonstrate that the activation can occur in three pathways, via electrons (X-ray illumination), photons (UV illumination) and thermally. Our work paves the way to coat materials with extended carbon nitride networks which are, as we show, stable under ambient conditions.

cond-mat.mtrl-sci↗

arXiv2023

Does cluster encapsulation inhibit sintering? Stabilization of size-selected Pt clusters on Fe$_3$O$_4$(001) by SMSI

The metastability of supported metal nanoparticles limits their application in heterogeneous catalysis at elevated temperatures due to their tendency to sinter. One strategy to overcome these thermodynamic limits on reducible oxide supports is encapsulation via strong metal-support interaction (SMSI). While annealing-induced encapsulation is a well-explored phenomenon for extended nanoparticles, it is as yet unknown whether the same mechanisms hold for sub-nanometer clusters, where concomitant sintering and alloying might play a significant role. In this article, we explore the encapsulation and stability of size-selected Pt$_5$, Pt$_{10}$ and Pt$_{19}$ clusters deposited on Fe$_3$O$_4$(001). In a multimodal approach using temperature-programmed desorption (TPD), x-ray photoelectron spectroscopy (XPS) and scanning tunneling microscopy (STM), we demonstrate that SMSI indeed leads to the formation of a defective, FeO-like conglomerate encapsulating the clusters. By stepwise annealing up to 1023 K, we observe the succession of encapsulation, cluster coalescence and Ostwald ripening, resulting in square-shaped crystalline Pt particles, independent of the initial cluster sizes. The respective sintering onset temperatures scale with the cluster footprint and thus size. Remarkably, while small encapsulated clusters can still diffuse as a whole, atom detachment and thus Ostwald ripening are successfully suppressed up to 823 K, i.e. 200 K above the H\"uttig temperature that indicates the thermodynamic stability limit.

cond-mat.mtrl-sci↗

arXiv2021

Cluster Catalysis with Lattice Oxygen: Tracing Oxygen Transport from a Magnetite(001) Support onto Small Pt Clusters

Oxidation catalysis on reducible oxide-supported small metal clusters often involves lattice oxygen. In the present work, we trace the path of lattice oxygen from Fe3O4(001) onto small Pt clusters during the CO oxidation, aiming at differentiating whether the reaction takes place at the cluster/support interface or on the cluster. While oxygen vacancies form on many other supports, magnetite maintains its surface stoichiometry upon reduction thanks to a high cation mobility. In order to investigate whether size-dependent oxygen affinities play a role, we study two specific cluster sizes, Pt5 and Pt19. By separating different reaction steps in our experiment, lattice oxygen can be accumulated on the clusters. Temperature programmed desorption (TPD) and sophisticated pulsed valve experiments indicate that the CO oxidation takes place on the Pt clusters rather than at the interface. Scanning tunneling microscopy (STM) shows a decrease in apparent height of the clusters, which density functional theory (DFT) explains as a restructuring following lattice oxygen reverse spillover.

cond-mat.mtrl-sci↗