Thomas Schnappinger
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View article: Selective excitation of molecular vibrations via a two-mode cavity Raman scheme
Selective excitation of molecular vibrations via a two-mode cavity Raman scheme Open
The experimental realization of strong light–matter coupling with molecules initiated the rapidly evolving field of molecular polaritonics. Most studies focus on how exciton polaritons, which combine electronic excitations with confined li…
View article: Selective excitation of molecular vibrations via a two-mode cavity Raman scheme
Selective excitation of molecular vibrations via a two-mode cavity Raman scheme Open
The experimental realization of strong light-matter coupling with molecules initiated the rapidly evolving field of molecular polaritonics. Most studies focus on how exciton polaritons, which combine electronic excitations with confined li…
View article: Attosecond spectroscopy of molecular charge transfer uncovers a 1.5-fs delay in population transfer
Attosecond spectroscopy of molecular charge transfer uncovers a 1.5-fs delay in population transfer Open
The transfer of population between two intersecting quantum states is the most fundamental event in many dynamical processes in physics, chemistry, biology, and material science. Any two-state description of such processes requires populat…
View article: Impact of Dark Polariton States on Collective Strong Light–Matter Coupling in Molecules
Impact of Dark Polariton States on Collective Strong Light–Matter Coupling in Molecules Open
Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the past few years. These exper…
View article: Molecular Polarizability under Vibrational Strong Coupling
Molecular Polarizability under Vibrational Strong Coupling Open
Polaritonic chemistry offers the possibility of modifying molecular properties and even influencing chemical reactivity through strong coupling between vibrational transitions and confined light modes in optical cavities. Despite considera…
View article: Analytic model reveals local molecular polarizability changes induced by collective strong coupling in optical cavities
Analytic model reveals local molecular polarizability changes induced by collective strong coupling in optical cavities Open
Despite recent numerical evidence, one of the fundamental theoretical mysteries of polaritonic chemistry is how and if collective strong coupling can induce local changes of the electronic structure to modify chemical properties. Here we p…
View article: Simulating nonadiabatic dynamics in benzophenone: Tracing internal conversion through photoelectron spectra
Simulating nonadiabatic dynamics in benzophenone: Tracing internal conversion through photoelectron spectra Open
Benzophenone serves as a prototype chromophore for studying the photochemistry of aromatic ketones, with applications ranging from biochemistry to organic light-emitting diodes. In particular, its intersystem crossing from the first single…
View article: Simulation of time-resolved site-selective X-ray spectroscopy tracing nonadiabatic dynamics in <i>meta</i> -methylbenzophenone
Simulation of time-resolved site-selective X-ray spectroscopy tracing nonadiabatic dynamics in <i>meta</i> -methylbenzophenone Open
Benzophenone derivatives are interesting photochemical systems. Quantum dynamics is used to simulate time-resolved X-ray absorption and Raman spectroscopy with core-level sensitivity at the carbonyl group of meta-methylbenzophenone.
View article: Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy
Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy Open
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical rea…
View article: Enhanced photoisomerization with hybrid metallodielectric cavities based on mode interference
Enhanced photoisomerization with hybrid metallodielectric cavities based on mode interference Open
The ability to control chemical reactions by coupling organic molecules to confined light in a cavity has recently attracted much attention. While most previous studies have focused on single-mode photonic or plasmonic cavities, here we in…
View article: Simulating Nonadiabatic Dynamics in Benzophenone: Tracing Internal Conversion Through Photoelectron Spectra
Simulating Nonadiabatic Dynamics in Benzophenone: Tracing Internal Conversion Through Photoelectron Spectra Open
Benzophenone serves as a prototype chromophore for studying the photochemistry of aromatic ketones, with applications ranging from biochemistry to organic light-emitting diodes. In particular, its intersystem crossing from the first single…
View article: Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy
Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy Open
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical rea…
View article: 1.5-Femtosecond Delay in Charge Transfer
1.5-Femtosecond Delay in Charge Transfer Open
The transfer of population between two intersecting quantum states is the most fundamental dynamical event that governs a broad variety of processes in physics, chemistry, biology and material science. Whereas any two-state description imp…
View article: Extending the Tavis–Cummings model for molecular ensembles—Exploring the effects of dipole self-energies and static dipole moments
Extending the Tavis–Cummings model for molecular ensembles—Exploring the effects of dipole self-energies and static dipole moments Open
Strong coupling of organic molecules to the vacuum field of a nanoscale cavity can be used to modify their chemical and physical properties. We extend the Tavis–Cummings model for molecular ensembles and show that the often neglected inter…
View article: Do Molecular Geometries Change Under Vibrational Strong Coupling?
Do Molecular Geometries Change Under Vibrational Strong Coupling? Open
As pioneering experiments have shown, strong coupling between molecular vibrations and light modes in an optical cavity can significantly alter molecular properties and even affect chemical reactivity. However, the current theoretical desc…
View article: Unraveling a Cavity-Induced Molecular Polarization Mechanism from Collective Vibrational Strong Coupling
Unraveling a Cavity-Induced Molecular Polarization Mechanism from Collective Vibrational Strong Coupling Open
We demonstrate that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. We do so by first showing that the full nonrelativistic …
View article: Electronic Fingerprint of the Protonated Imidazole Dimer Probed by X-ray Absorption Spectroscopy
Electronic Fingerprint of the Protonated Imidazole Dimer Probed by X-ray Absorption Spectroscopy Open
Protons in low-barrier superstrong hydrogen bonds are typically delocalized between two electronegative atoms. Conventional methods to characterize such superstrong hydrogen bonds are vibrational spectroscopy and diffraction techniques. We…
View article: Ab Initio Vibro-Polaritonic Spectra in Strongly Coupled Cavity-Molecule Systems
Ab Initio Vibro-Polaritonic Spectra in Strongly Coupled Cavity-Molecule Systems Open
Recent experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling, can modify reaction ra…
View article: Ab-Initio Vibro-Polaritonic Spectra in Strongly Coupled Cavity-Molecule Systems
Ab-Initio Vibro-Polaritonic Spectra in Strongly Coupled Cavity-Molecule Systems Open
Recent experiments have revealed the profound effect of strong light-matter interactions in optical cavities on the electronic ground state of molecular systems. This phenomenon, known as vibrational strong coupling (VSC), can modify react…
View article: Cavity Born–Oppenheimer Hartree–Fock Ansatz: Light–Matter Properties of Strongly Coupled Molecular Ensembles
Cavity Born–Oppenheimer Hartree–Fock Ansatz: Light–Matter Properties of Strongly Coupled Molecular Ensembles Open
Experimental studies indicate that optical cavities can affect chemical reactions through either vibrational or electronic strong coupling and the quantized cavity modes. However, the current understanding of the interplay between molecule…
View article: Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles
Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles Open
Experimental studies indicate that optical cavities can affect chemical reactions, through either vibrational or electronic strong coupling and the quantized cavity modes. However, the current understanding of the interplay between molecul…
View article: Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling
Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling Open
We demonstrate that collective vibrational strong coupling of molecules in thermal equilibrium can give rise to significant local electronic polarizations in the thermodynamic limit. We do so by first showing that the full non-relativistic…
View article: Nonadiabatic Wave Packet Dynamics with Ab Initio Cavity-Born-Oppenheimer Potential Energy Surfaces
Nonadiabatic Wave Packet Dynamics with Ab Initio Cavity-Born-Oppenheimer Potential Energy Surfaces Open
Strong coupling of molecules with quantized electromagnetic fields can reshape their potential energy surfaces by forming dressed states. In such a scenario, it is possible to manipulate the dynamics of the molecule and open new photochemi…
View article: Time-resolved X-ray and XUV based spectroscopic methods for nonadiabatic processes in photochemistry
Time-resolved X-ray and XUV based spectroscopic methods for nonadiabatic processes in photochemistry Open
Novel spectroscopic techniques based on ultra-short laser pulses in the X-ray regime are reviewed, capable of observing clear signatures of conical intersections.
View article: Photo-Induced Coupled Nuclear and Electron Dynamics in the Nucleobase Uracil
Photo-Induced Coupled Nuclear and Electron Dynamics in the Nucleobase Uracil Open
Photo-initiated processes in molecules often involve complex situations where the induced dynamics is characterized by the interplay of nuclear and electronic degrees of freedom. The interaction of the molecule with an ultrashort laser pul…
View article: Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study
Ultrafast strong-field dissociation of vinyl bromide: An attosecond transient absorption spectroscopy and non-adiabatic molecular dynamics study Open
Attosecond extreme ultraviolet (XUV) and soft x-ray sources provide powerful new tools for studying ultrafast molecular dynamics with atomic, state, and charge specificity. In this report, we employ attosecond transient absorption spectros…
View article: Coupled nuclear and electron dynamics in the vicinity of a conical intersection
Coupled nuclear and electron dynamics in the vicinity of a conical intersection Open
Ultrafast optical techniques allow us to study ultrafast molecular dynamics involving both nuclear and electronic motion. To support interpretation, theoretical approaches are needed that can describe both the nuclear and electron dynamics…
View article: Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals
Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals Open
Significance The capabilities of modern X-ray sources have substantially increased the temporal and spectral resolutions for the observation of elementary molecular events. Theoretically, it has been shown that these unique features can be…
View article: Photoprotecting Uracil by Coupling with Lossy Nanocavities
Photoprotecting Uracil by Coupling with Lossy Nanocavities Open
We analyze how the photorelaxation dynamics of a molecule can be controlled by modifying its electromagnetic environment using a nanocavity mode. In particular, we consider the photorelaxation of the RNA nucleobase uracil, which is the nat…