Markus Kowalewski
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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: 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: 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: Ultrafast Mapping of Electronic and Nuclear Structure in the Photo Dissociation of Nitrogen Dioxide
Ultrafast Mapping of Electronic and Nuclear Structure in the Photo Dissociation of Nitrogen Dioxide Open
We investigate the photoinduced dissociation reaction of NO2 → NO + O upon electronic excitation of the X̃2A1 (D0) to the Ã2B2 (D1) state by femtosecond X-ray absorption spectroscopy at the nitrogen K-edge. We obtain key insight into the ch…
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: Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets
Supercritical density fluctuations and structural heterogeneity in supercooled water-glycerol microdroplets Open
Recent experiments and theoretical studies strongly indicate that water exhibits a liquid-liquid phase transition (LLPT) in the supercooled domain. An open question is how the LLPT of water can affect the properties of aqueous solutions. H…
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: Distinguishing Organomagnesium Species in the Grignard Addition to Ketones with X‐Ray Spectroscopy
Distinguishing Organomagnesium Species in the Grignard Addition to Ketones with X‐Ray Spectroscopy Open
The addition of Grignard reagents to ketones is a well‐established textbook reaction. However, a comprehensive understanding of its mechanism has only recently begun to emerge. X‐ray spectroscopy, because of its high selectivity and sensit…
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: Coherent x-ray spontaneous emission spectroscopy of conical intersections
Coherent x-ray spontaneous emission spectroscopy of conical intersections Open
Conical intersections are known to play a vital role in many photochemical processes. The breakdown of the Born–Oppenheimer approximation in the vicinity of a conical intersection causes exciting phenomena, such as the ultrafast radiationl…
View article: Raman Spectroscopy of Conical Intersections Using Entangled Photons
Raman Spectroscopy of Conical Intersections Using Entangled Photons Open
Ultrafast Raman spectroscopy with attosecond pulses in the extreme ultraviolet and X-ray regime has been proposed theoretically for tracking the non-adiabatic dynamics of molecules in great detail. The large bandwidth of these pulses, whic…
View article: Multidimensional high-harmonic echo spectroscopy: Resolving coherent electron dynamics in the EUV regime
Multidimensional high-harmonic echo spectroscopy: Resolving coherent electron dynamics in the EUV regime Open
We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electronvolts. Using our recently develop…
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: Multidimensional high-harmonic echo spectroscopy: resolving coherent electron dynamics in the EUV regime
Multidimensional high-harmonic echo spectroscopy: resolving coherent electron dynamics in the EUV regime Open
We theoretically propose a multidimensional high-harmonic echo spectroscopy technique which utilizes strong optical fields to resolve coherent electron dynamics spanning an energy range of multiple electron Volts. Using our recently develo…
View article: Cavity-Modified Chemiluminescent Reaction of Dioxetane
Cavity-Modified Chemiluminescent Reaction of Dioxetane Open
Chemiluminescence is a thermally activated chemical process that emits a photon of light by forming a fraction of products in the electronic excited state. A well-known example of this spectacular phenomenon is the emission of light in the…
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: The role of dephasing for dark state coupling in a molecular Tavis–Cummings model
The role of dephasing for dark state coupling in a molecular Tavis–Cummings model Open
The collective coupling of an ensemble of molecules to a light field is commonly described by the Tavis–Cummings model. This model includes numerous eigenstates that are optically decoupled from the optically bright polariton states. Acces…
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: The role of dephasing for dark state coupling in a molecular Tavis-Cummings model
The role of dephasing for dark state coupling in a molecular Tavis-Cummings model Open
Collective coupling of an ensemble of particles to a light field is commonly described by the Tavis--Cummings model. This model includes numerous eigenstates which are optically decoupled from the optically bright polariton states. To acce…