Pascal Heim
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View article: Real-time tracking of energy flow in cluster formation
Real-time tracking of energy flow in cluster formation Open
Femtosecond time-resolved spectroscopy has shaped our understanding of light-matter interaction at the atomic level. However, the photoinduced formation of chemical bonds, especially for larger aggregates, has evaded observation due to dif…
View article: Real-time tracking the energy flow in cluster formation
Real-time tracking the energy flow in cluster formation Open
While photodissociation of molecular systems has been extensively studied, the photoinduced formation of chemical bonds remains largely unexplored. Especially for larger aggregates, the electronic and nuclear dynamics involved in the clust…
View article: Transient absorption microscopy setup with multi-ten-kilohertz shot-to-shot subtraction and discrete Fourier analysis
Transient absorption microscopy setup with multi-ten-kilohertz shot-to-shot subtraction and discrete Fourier analysis Open
Recording of transient absorption microscopy images requires fast detection of minute optical density changes, which is typically achieved with high-repetition-rate laser sources and lock-in detection. Here, we present a highly flexible an…
View article: Transient absorption microscopy setup with multi-ten-kilohertz\n shot-to-shot subtraction and discrete Fourier analysis
Transient absorption microscopy setup with multi-ten-kilohertz\n shot-to-shot subtraction and discrete Fourier analysis Open
Recording of transient absorption microscopy images requires fast detection\nof minute optical density changes, which is typically achieved with\nhigh-repetition-rate laser sources and lock-in detection. Here, we present a\nhighly flexible…
View article: Observation of laser-assisted electron scattering in superfluid helium
Observation of laser-assisted electron scattering in superfluid helium Open
Measured and simulated electron spectra for the study entitled "Observation of laser-assisted electron scattering in superfluid helium". Figure 1a (fig1_a.csv) column 1: simulated electron energy in eV column 2: log_10(simulated electron …
View article: Observation of laser-assisted electron scattering in superfluid helium
Observation of laser-assisted electron scattering in superfluid helium Open
Measured and simulated electron spectra for the study entitled "Observation of laser-assisted electron scattering in superfluid helium". Figure 1a (fig1_a.csv) column 1: simulated electron energy in eV column 2: log_10(simulated electron …
View article: Observation of laser-assisted electron scattering in superfluid helium
Observation of laser-assisted electron scattering in superfluid helium Open
Laser-assisted electron scattering (LAES), a light-matter interaction process that facilitates energy transfer between strong light fields and free electrons, has so far been observed only in gas phase. Here we report on the observation of…
View article: Long-Lived Nuclear Coherences inside Helium Nanodroplets
Long-Lived Nuclear Coherences inside Helium Nanodroplets Open
Much of our knowledge about dynamics and functionality of molecular systems has been achieved with femtosecond time-resolved spectroscopy. Despite extensive technical developments over the past decades, some classes of systems have eluded …
View article: Revealing Ultrafast Population Transfer between Nearly Degenerate Electronic States
Revealing Ultrafast Population Transfer between Nearly Degenerate Electronic States Open
The response of a molecule to photoexcitation is governed by the coupling of its electronic states. However, if the energetic spacing between the electronically excited states at the Franck-Condon window becomes sufficiently small, it is i…
View article: Bayesian Analysis of Femtosecond Pump-Probe Photoelectron-Photoion Coincidence Spectra with Fluctuating Laser Intensities
Bayesian Analysis of Femtosecond Pump-Probe Photoelectron-Photoion Coincidence Spectra with Fluctuating Laser Intensities Open
This paper employs Bayesian probability theory for analyzing data generated in femtosecond pump-probe photoelectron-photoion coincidence (PEPICO) experiments. These experiments allow investigating ultrafast dynamical processes in photoexci…
View article: Femtosecond solvation dynamics of indium dimers inside superfluid helium nanodroplets
Femtosecond solvation dynamics of indium dimers inside superfluid helium nanodroplets Open
Indium dimers (In 2 ) solvated inside helium nanodroplets are studied with femtosecond photoelectron and photoion spectroscopy. The solvation dynamics triggered by photoexcitation of the In 2 include expansion of the solvation shell and do…
View article: Bayesian probability theory to identify false coincidences in coincidence experiments
Bayesian probability theory to identify false coincidences in coincidence experiments Open
We describe a Bayesian formalism to analyse femtosecond pump-probe photoionization experiments with photoelectron-photoion coincidence (PEPICO) detection. This approach overcomes the drawback of extraordinary long data acquisition times of…
View article: Femtosecond dopant-to-solvent energy transfer inside helium nanodroplets
Femtosecond dopant-to-solvent energy transfer inside helium nanodroplets Open
Photoexcitation of atoms solvated inside superfluid helium nanodroplets is investigated with femtosecond photoelectron spectroscopy. Expansion of the solvation shell within about 600 fs is observed as transient photoelectron peak shift. Fo…
View article: Femtosecond photoexcitation dynamics inside a quantum solvent
Femtosecond photoexcitation dynamics inside a quantum solvent Open
The observation of chemical reactions on the time scale of the motion of electrons and nuclei has been made possible by lasers with ever shortened pulse lengths. Superfluid helium represents a special solvent that permits the synthesis of …
View article: Analysis of femtosecond pump-probe photoelectron-photoion coincidence measurements applying Bayesian probability theory
Analysis of femtosecond pump-probe photoelectron-photoion coincidence measurements applying Bayesian probability theory Open
Ultrafast dynamical processes in photoexcited molecules can be observed with\npump-probe measurements, in which information about the dynamics is obtained\nfrom the transient signal associated with the excited state. Background signals\npr…
View article: The Role of Rydberg–Valence Coupling in the Ultrafast Relaxation Dynamics of Acetone
The Role of Rydberg–Valence Coupling in the Ultrafast Relaxation Dynamics of Acetone Open
The electronic structure of excited states of acetone is represented by a Rydberg manifold that is coupled to valence states which provide very fast and efficient relaxation pathways. We observe and characterize the transfer of population …
View article: Direct observation of a photochemical activation energy: a case study of acetone photodissociation
Direct observation of a photochemical activation energy: a case study of acetone photodissociation Open
The ability to observe and quantify the conversion of electronic potential energy to vibrational kinetic energy in a molecule after photoexcitation is essential to understand and control the outcome of photoinduced molecular fragmentation.…