Simulation of ultrafast excited-state dynamics and elastic x-ray scattering by quantum wavepacket dynamics

Pápai, Mátyás; Rozgonyi, Tamás; Penfold, Thomas J.; Nielsen, Martin Meedom; Møller, Klaus Braagaard

doi:10.1063/1.5115204

Cited by 19 publications

(43 citation statements)

References 70 publications

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“…Whereas these spectra simulations are based on the computed energy differences and transition matrix elements, simulation of time‐resolved X‐ray scattering requires only to know the nuclear coordinate data. Examples have been presented for ethylene and metal‐organic Fe complexes …”

Section: The Challenges In Nuclear Dynamics Theorymentioning

confidence: 99%

Molecular Photochemistry: Recent Developments in Theory

2020

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Photochemistry is a fascinating branch of chemistry that is concerned with molecules and light. However, the importance of simulating light‐induced processes is reflected also in fields as diverse as biology, material science, and medicine. This Minireview highlights recent progress achieved in theoretical chemistry to calculate electronically excited states of molecules and simulate their photoinduced dynamics, with the aim of reaching experimental accuracy. We focus on emergent methods and give selected examples that illustrate the progress in recent years towards predicting complex electronic structures with strong correlation, calculations on large molecules, describing multichromophoric systems, and simulating non‐adiabatic molecular dynamics over long time scales, for molecules in the gas phase or in complex biological environments.

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Section: The Challenges In Nuclear Dynamics Theorymentioning

confidence: 99%

Molecular Photochemistry: Recent Developments in Theory

2020

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“…Further advanced computational investigations, including high level calculations of excited states as well as quantum dynamics simulations, have also been carried out recently by several groups to elucidate different aspects of the excited state properties of the iron carbene reference compounds and related iron complexes, with a range of different ligands from regular polypyridyls to NHCs and other strong σ-donors, see e.g., [21,24,[69][70][71][72][73][74]. These studies provide fundamental insight into the difference of the FeNHC complexes compared to more traditional iron polypyridyl complexes such as [Fe(bpy) 3 ] 2+ , e.g., in terms of the role of intersystem crossing and transitions from CT to MC states.…”

Section: Hot Branching and Wave Packet Dynamicsmentioning

confidence: 99%

Photophysics and Photochemistry of Iron Carbene Complexes for Solar Energy Conversion and Photocatalysis

et al. 2020

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Earth-abundant first row transition metal complexes are important for the development of large-scale photocatalytic and solar energy conversion applications. Coordination compounds based on iron are especially interesting, as iron is the most common transition metal element in the Earth’s crust. Unfortunately, iron-polypyridyl and related traditional iron-based complexes generally suffer from poor excited state properties, including short excited-state lifetimes, that make them unsuitable for most light-driven applications. Iron carbene complexes have emerged in the last decade as a new class of coordination compounds with significantly improved photophysical and photochemical properties, that make them attractive candidates for a range of light-driven applications. Specific aspects of the photophysics and photochemistry of these iron carbenes discussed here include long-lived excited state lifetimes of charge transfer excited states, capabilities to act as photosensitizers in solar energy conversion applications like dye-sensitized solar cells, as well as recent demonstrations of promising progress towards driving photoredox and photocatalytic processes. Complementary advances towards photofunctional systems with both Fe(II) complexes featuring metal-to-ligand charge transfer excited states, and Fe(III) complexes displaying ligand-to-metal charge transfer excited states are discussed. Finally, we outline emerging opportunities to utilize the improved photochemical properties of iron carbenes and related complexes for photovoltaic, photoelectrochemical and photocatalytic applications.

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“…Hierzu finden sich in der Literatur Beispiele fürE thylen [167] und fürm etallorganische Eisenkomplexe. [208] Abbildung 6. BeispielhafteV ergleiche von experimentellen und simulierten zeitaufgelçsten Spektren.…”

Section: Simulation Von Observablenunclassified

“…Die genannten Spektrensimulationen basieren auf berechneten Energiedifferenzen und Übergangsmatrixelementen, wohingegen die Simulation von zeitaufgelösten Röntgenbeugungssignalen lediglich die Daten für die Kernkoordinaten erfordert. Hierzu finden sich in der Literatur Beispiele für Ethylen und für metallorganische Eisenkomplexe …”

Section: Die Herausforderungen Der Kerndynamikunclassified

Molekulare Photochemie: Moderne Entwicklungen in der theoretischen Chemie

Mai

González

2020

Angewandte Chemie

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Photochemie ist ein faszinierendes Teilgebiet der Chemie, das sich mit der Wechselwirkung von Molekülen und Licht befasst. Die Simulation von lichtinduzierten Prozessen spielt auch in anderen Forschungsgebieten wie Biologie, Materialwissenschaften oder Medizin eine bedeutende Rolle. Dieser Kurzaufsatz beleuchtet die jüngsten Entwicklungen in der theoretischen Chemie, die das Ziel haben, experimentelle Genauigkeit bei der Berechnung von elektronisch angeregten Zuständen von Molekülen und bei der Simulation von deren lichtinduzierten Dynamiken zu erreichen. Wir konzentrieren uns dabei auf neue, aufstrebende Methoden und zeigen ausgewählte Beispiele, welche die Fortschritte der letzten Jahre für folgende Themen aufzeigen: die Voraussage komplexer Elektronenstrukturen mit starker Korrelation, die Berechnung von großen Molekülen, die Beschreibung von multi‐chromophorischen Systemen und die Simulation nicht‐adiabatischer Moleküldynamik auf langen Zeitskalen; dies umfasst Moleküle sowohl in der Gasphase als auch in komplexer biologischer Umgebung.

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Simulation of ultrafast excited-state dynamics and elastic x-ray scattering by quantum wavepacket dynamics

Cited by 19 publications

References 70 publications

Molecular Photochemistry: Recent Developments in Theory

Molecular Photochemistry: Recent Developments in Theory

Photophysics and Photochemistry of Iron Carbene Complexes for Solar Energy Conversion and Photocatalysis

Molekulare Photochemie: Moderne Entwicklungen in der theoretischen Chemie

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