A5046747864- Advanced Photocatalysis Techniques
- CO2 Reduction Techniques and Catalysts
- Crystallization and Solubility Studies
- X-ray Diffraction in Crystallography
- Electrocatalysts for Energy Conversion
- Photochemistry and Electron Transfer Studies
- Porphyrin and Phthalocyanine Chemistry
- Metal complexes synthesis and properties
- Machine Learning in Materials Science
- Nanocluster Synthesis and Applications
- Advanced biosensing and bioanalysis techniques
- Electrochemical Analysis and Applications
- Organic Light-Emitting Diodes Research
- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Radical Photochemical Reactions
- Luminescence and Fluorescent Materials
- Lanthanide and Transition Metal Complexes
- Advanced Nanomaterials in Catalysis
- Laser-Matter Interactions and Applications
- Polyoxometalates: Synthesis and Applications
- Metalloenzymes and iron-sulfur proteins
- Organic Chemistry Cycloaddition Reactions
- Perovskite Materials and Applications
- Electronic and Structural Properties of Oxides
Friedrich-Alexander-Universität Erlangen-Nürnberg
2023-2025
University of Luxembourg
2023-2024
Robert Bosch (Germany)
2023
Helmholtz Institute Jena
2017-2022
Friedrich Schiller University Jena
2017-2022
Leibniz Institute of Photonic Technology
2020-2022
Schott (Germany)
2020
Institute of Materials Research of the Slovak Academy of Sciences
2020
Institute of Physical Chemistry
2019
We present a comprehensive analysis of the capabilities modern machine learning force fields to simulate long-term molecular dynamics at near-ambient conditions for molecules, molecule-surface interfaces, and materials within TEA Challenge 2023.
Assessing the performance of modern machine learning force fields across diverse chemical systems to identify their strengths and limitations within TEA Challenge 2023.
Herein, we present KiMoPack, an analysis tool for the kinetic modeling of transient spectroscopic data. KiMoPack enables a state-of-the-art routine including data preprocessing and standard fitting (global analysis), as well complex (target) models, interactive viewing (fit) results, multiexperiment via user accessible functions graphical interface (GUI) enhanced interface. To facilitate its use, this paper guides through typical operations covering wide range tasks, establishes workflow is...
Unequivocal assignment of rate-limiting steps in supramolecular photocatalysts is utmost importance to rationally optimize photocatalytic activity. By spectroscopic and catalytic analysis a series three structurally similar [(tbbpy)2Ru-BL-Rh(Cp*)Cl]3+ just differing the central part (alkynyl, triazole or phenazine) bridging ligand (BL) we are able derive design strategies for improved activity this class compounds (tbbpy = 4,4´-tert-butyl-2,2´-bipyridine, Cp* pentamethylcyclopentadienyl)....
Significance Laser-induced electron diffraction is a molecular-scale microscopy that captures clean snapshots of molecule’s geometry with subatomic picometer and attosecond spatiotemporal resolution. We induce unambiguously identify the stretching bending linear triatomic molecule following excitation to an excited electronic state bent stretched geometry. show we can directly retrieve structure electronically molecules otherwise possible through indirect retrieval methods such as pump–probe...
Synthetic models of the active site [FeFe]-hydrogenase containing naphthalene monoimide (NMI) peri-substituted dichalcogenides as bridging linkers have been prepared and characterized using different spectroscopic methods. The influence imide functionality chalcogen atoms on redox properties catalytic behaviour complexes 7-10 was studied cyclic voltammetry. results revealed that has improved chemical stability reduced species replacement S by Se caused a cathodic shift in oxidation peaks....
S pai NN employs ch N et P ack to train electronic properties across various potential energy curves, including energies, gradients, and couplings, while integrating with SHARC for excited state molecular dynamics simulations.
The production of hydrogen by efficient, low-cost, and integrated photoelectrochemical water splitting processes represents an important target for the ecological transition. This challenge can be addressed thanks to bioinspired chemistry artificial photosynthesis approaches designing dye-sensitized photocathodes production, incorporating first-row transition metal-based catalysts. present work describes preparation characterization a NiO photocathode sensitized with phosphonate-derivatized...
In recent years, dyads in which molecular donor and acceptor moieties are chemically linked by a bridging ligand have emerged as attractive systems for light-driven catalysis. Their modular structure, controllable donor-acceptor distance, their ability to undergo charge transfer, is not limited diffusion, render such promising charge-transfer reactions redox Copper-catalyzed alkyne azide cycloaddition (CuAAC) particularly popular synthetic strategy coupling moieties. This CLICK chemistry...
We present the second part of rigorous evaluation state-of-the-art machine learning force fields (MLFFs) within TEA Challenge 2023. This study provides an in-depth analysis performance MACE, SO3krates, sGDML, SOAP/GAP, and FCHL19* in modeling molecules, molecule-surface interfaces, periodic materials. compare observables obtained from molecular dynamics (MD) simulations using different MLFFs under identical conditions. Where applicable, density-functional theory (DFT) or experiment serves as...
Atomistic simulations are routinely employed in academia and industry to study the behavior of molecules, materials, their interfaces. Central these force fields (FF), whose development is challenged by intricate interatomic interactions at different spatio-temporal scales vast expanse chemical space. Machine learning (ML) FFs, trained on quantum-mechanical energies forces, have shown capacity achieve sub-kcal/(mol*A) accuracy while maintaining computational efficiency. The TEA Challenge...
Bi(benz)imidazoles (b(b)im) acting as N,N-chelates in ruthenium complexes represent a unique class of ligands. They do not harbor metal-to-ligand charge-transfer (MLCT) excited states polypyridyl upon visible-light excitation provided that no substitution is introduced at the N atoms. Hence, they can be used to steer light-driven electron-transfer pathways desired direction. Nonetheless, free atoms are susceptible protonation and, hence, introduce highly pH-dependent properties into...
Transition-metal-based donor–acceptor systems can produce long-lived excited charge-transfer states by visible-light irradiation. The novel ruthenium(II) polypyridyl type complexes Ru1 and Ru2 based on the dipyridophenazine ligand (L0) directly linked to 4-hydroxythiazoles of different donor strengths were synthesized photophysically characterized. excited-state dynamics investigated femtosecond-to-nanosecond transient absorption nanosecond emission spectroscopy complemented time-dependent...
To optimize light-driven catalytic processes, light-mediated multi-electron transfer dynamics in molecular dyads need to be studied and correlated with structural changes focusing on the catalytically active metastable intermediates. Here, spectro-electrochemistry has been employed investigate structure-dependent photoelectron kinetics intermediates of two Ru-Rh catalysts for NAD+ reduction. The excited-state reactivity short-lived was along different photoreaction pathways by resonance...
Using the extended QM7-X dataset, it is shown that polarizabilty and HOMO–LUMO gap are uncorrelated in chemical compound space. The lack of correlation enables design novel materials, demonstrated through organic photodetector candidates.
The excited state properties of three heteroleptic copper(I) xantphos 4H-imidazolate complexes are investigated by means femtosecond and nanosecond time-resolved transient absorption spectroscopy in dichloromethane solution. subpicosecond spectral changes observed after excitation into the MLCT band interpreted as intersystem crossing from singlet to triplet manifold. This interpretation is corroborated DFT TD-DFT results, indicating a comparable molecular geometry ground (and hence...
The impact of the electronic structure a series 4H-imidazolate ligands in neutral, heteroleptic Cu(I) complexes is investigated. Remarkable broad and strong ligand-dependent absorption visible range electromagnetic spectrum renders studied promising photosensitizers for photocatalytic applications. localization photoexcited states Franck-Condon region are unraveled by means UV-vis resonance Raman (rR) spectroscopy supported time-dependent density functional theory (TD-DFT) calculations....
Abstract An implementation of real‐time time‐dependent density functional theory (RT‐TDDFT) within the TURBOMOLE program package is reported using Gaussian‐type orbitals as basis functions, second and fourth order Magnus propagator, self‐consistent field well predictor–corrector time integration schemes. The Coulomb contribution to Kohn–Sham matrix calculated combining fitting approximation continuous fast multipole method. Performance benchmarked for molecular systems with different sizes...
Ruthenium(II) complexes, like [(tbbpy)2Ru(dppz)]2+ (Ru-dppz; tbbpy = 4,4′-di-tert-butyl-2,2′-bipyridine, dppz dipyrido-[3,2-a:2′,3′-c]phenazine), have emerged as suitable photosensitizers in photoredox catalysis. Since then, there has been ongoing interest the design of π-extended Ru-dppz systems with red-shifted visible absorption maxima and sufficiently long-lived excited states independent solvent or pH value. Herein, we explore photophysical properties protonation isomers linearly...
Exact determination of the electronic density molecules and materials would provide direct access to accurate bonded non-bonded interatomic interactions by virtue Hellman-Feynman theorem. However, density-functional approximations (DFA) -- workhorse methods for structure atomistic systems only approximate sometimes unreliable electron densities. Here we show that long-range van der Waals (vdW) dispersion can visibly modify charge density, scale nontrivially with system size, in some cases...
Abstract Cyclometalated Iridium(III) complexes, i. e . [Ir(C N) 2 (dppz)][PF 6 ], bearing either two or four ‐CH PO(OH) anchoring groups ( IrP dppz 4 ) are explored as photosensitizers for p‐type dye sensitized solar cell (DSSC). The synthetic route is described and the iridium(III) complexes characterized with respect to their electrochemical photophysical properties. modified ligand geometry exploited in this work not only alters electronic nature of complex (that by destabilizing LUMO...
The design of photoactive systems capable storing and relaying multiple electrons is highly demanded in the field artificial photosynthesis, where transformations interest rely on multielectronic redox processes. photophysical properties ruthenium photosensitizer [(bpy)2 Ru(oxim-dppqp)]2+ (Ru), two coupled to protons π-extended oxim-dppqp ligand under light-driven conditions, are investigated by means excitation wavelength-dependent resonance Raman transient absorption spectroscopies,...
Multifunctional supramolecular systems are a central research topic in light-driven solar energy conversion. Here, we report polyoxometalate (POM)-based dyad, where two platinum-complex hydrogen evolution catalysts covalently anchored to an Anderson polyoxomolybdate anion. Supramolecular electrostatic coupling of the system iridium photosensitizer enables visible evolution. Combined theory and experiment demonstrate multifunctionality POM, which acts as photosensitizer/catalyst-binding-site