Themed collection Festschrift Wolfgang E. Ernst: Electronic & Nuclear Dynamics in Molecules, Clusters, and on Surfaces
Festschrift for Wolfgang E. Ernst – electronic and nuclear dynamics and their interplay in molecules, clusters and on surfaces
Guest editors, Andreas W. Hauser, Martina Havenith, Markus Koch and Martin Sterrer, introduce this themed issue dedicated to Professor Wolfgang E. Ernst on the occasion of his 70th birthday.
Four modifications of the Jahn–Teller effects. The problem of observables: spin–orbit interaction, tunneling splitting, and orientational polarization of solids
Four kinds of electronic degeneracy or pseudodegeneracy leading to the Jahn-Teller effects.
Perspectives on weak interactions in complex materials at different length scales
Weak interactions are essential in modern research and technologies, such as nanocomposite materials, nanometer-sized quantum objects embedded in a host material or van der Waals heterostructures. Various fields address their characterisations and descriptions.
Superfluid helium droplet-mediated surface-deposition of neutral and charged silver atomic species
High-level ab initio theory, combined with a full quantum description of the superfluid helium nanodroplet motion, provides evidence for the fundamental mechanism of soft-deposition of Ag and Ag+, being the soft-landing favored as the helium nanodroplet size increases.
Photodissociation dynamics and UV absorption spectrum of acetone oxide (CH3)2COO
The photodynamics and B1A′ ← X1A′ absorption spectrum of acetone oxide, (CH3)2COO, are studied theoretically from first principles.
The stochastic wave function method for diffusion of alkali atoms on metallic surfaces
The stochastic wave function method is proposed to study the diffusion regimes of alkali atoms on metallic surfaces and, in general, surface diffusion.
Carrier envelope phase sensitivity of photoelectron circular dichroism
The PECD of methyloxirane molecules fragmenting along the laser propagation direction (left) shows a strong modulation by the CEP (top) due to the CEP-dependence of the ionization probability from different areas of specific orbitals (bottom right).
Relaxation dynamics of 3He and 4He clusters and droplets studied using near infrared and visible fluorescence excitation spectroscopy
The relaxation dynamics of electronically excited 3He and 4He clusters and droplets is investigated using time-correlated near-infrared and visible (NIR/VIS) fluorescence excitation spectroscopy.
Tautomerization of single asymmetric oxahemiporphycene molecules on Cu(111)
We have studied 22-oxahemiporphycene molecules by a combination of scanning tunneling microscopy at low temperatures and density functional theory calculations.
How does tuning the van der Waals bonding strength affect adsorbate structure?
The binding and structure of an ordered pyrazine overlayer on graphite are studied with neutron scattering and DFT. We find increased van der Waals bonding and stability of the overlayer compared to benzene, due to the nitrogen atoms in the ring.
Relaxation dynamics in excited helium nanodroplets probed with high resolution, time-resolved photoelectron spectroscopy
The ultrafast relaxation dynamics of excited helium nanodroplets were studied using time-resolved photoelectron spectroscopy. We observed an efficient population of triplet atomic states as well as the formation of the first excimer state of He2*.
Charge and adsorption height dependence of the self-metalation of porphyrins on ultrathin MgO(001) films
While the self-metalation of 2H-TPP on MgO(001) thin films is mediated by charge transfer, 2H-P self-metalates irrespective of its charge state. The different reactivity is explained based on the molecule-substrate distance.
Electron diffraction of 1,4-dichlorobenzene embedded in superfluid helium droplets
Electron diffraction of 1,4-dichlorobenzene (C6H4Cl2) clusters embedded in superfluid helium droplets, resulting in the structure evolution of cluster growth.
Q-Band relaxation in chlorophyll: new insights from multireference quantum dynamics
The ultrafast relaxation within the Q-bands of chlorophyll plays a crucial role in photosynthetic light-harvesting. We investigate this process via nuclear and electronic quantum dynamics on multireference potential energy surfaces.
The quantum mean square displacement of thermalized CO on Cu(100) in the short time approximation
The mean square displacement of a thermalized CO molecule moving on a copper substrate is evaluated on the basis of a new quantum dynamical approach (Mol. Phys. 119, e1971315, 2021); results at 190 K, the Cu(100) lattice constant a ≈ 256 pm.
Nonadiabatic excited-state dynamics of ReCl(CO)3(bpy) in two different solvents
Hybrid QM/MM nonadiabatic dynamics of the complex ReCl(CO)3(bpy) (bpy = 2,2-bipyridine) on spin-mixed potential energy surfaces was carried out in acetonitrile and dimethylsulfoxide.
Non-adiabatic dynamics in collisions of sodium and chlorine atoms and their ions
Collisions of sodium atoms with chlorine atoms and sodium cations with chloride anions are studied by non-adiabatic dynamics. Rate coefficients for mutual neutralisation, chemiionisation, and radiative association are calculated up to 5300 K.
Dimer photofragmentation and cation ejection dynamics in helium nanodroplets
We present femtosecond pump–probe photoionization experiments with indium dimers (In2) solvated in helium nanodroplets (HeN), and identify an ionization pathway leading to ion ejection from the droplet, enabling ion-electron correlation.
Simulation of the photodetachment spectra of the nitrate anion (NO3−) in the 2E′ energy range and non-adiabatic electronic population dynamics of NO3
Quantum dynamics simulations demonstrate the presence of ultra-fast non-statistical and slow statistical non-radiative decay and the presence of active and inactive conical intersections in NO3.
Reaction of lithium hexamethyldisilazide (LiHMDS) with water at ultracold conditions
The reaction of LiHMDS with water was investigated at ultra-cold conditions (0.37 K) in superfluid helium nanodroplets using mid IR radiation.
Quantum dynamics of the Br2 (B-excited state) photodissociation in superfluid helium nanodroplets: importance of the recombination process
The photodissociation dynamics of Br2 (B ← X excitation) in helium nanodroplets is much more complex than that of Cl2, showing very large differences in several key properties. This is the second system investigated theoretically in this context.
Ionization potentials of MgN (N = 7–56) clusters formed by spontaneous collapse of magnesium foam in helium nanodroplets
Ultracold helium nandroplets are doped by Mg atoms in order to extract ionization potentials of magnesium clusters MgN in the size range N = 7–56.
Electronic spectroscopy of cationic adamantane clusters and dehydrogenated adamantane in helium droplets
We report the first helium-tagged electronic spectra of cationic adamantane clusters, along with its singly, doubly, and triply dehydrogenated analogues embedded in helium droplets.
The ultrafast vibronic dynamics of ammonia's state
Ultrafast internal vibrational relaxation is observed in ammonia's state on a timescale of less than 100 fs. This is a highly surprising observation, and has been revealed through vibronically sensitive time-resolved photoelectron measurements.
The role of high-energy phonons in electron–phonon interaction at conducting surfaces with helium-atom scattering
The Debye–Waller exponent for Helium atom specular reflection from a conducting surface, when measured as a function of temperature in the linear high-temperature regime, allows for the determination of the surface electron–phonon coupling.
Magnetic exchange and valence delocalization in a mixed valence [Fe2+Fe3+Te2]+ complex: insights from theory and interpretations of magnetic and spectroscopic data
A mixed valence tellurium bridged Fe(II)–Fe(III) complex was studied using correlated ab initio methods. Spectroscopic and magnetic properties have been rationalized considering coupling between spins and vibrations.
Electronic spectroscopy of phthalocyanine in a supersonic jet revisited
Rotationally resolved electronic spectroscopy of phthalocyanine in a supersonic jet has revealed detailed information on the configuration of both electronic states and the corresponding transition dipole moment.
Stable excited dication: trapping on the S1 state of formaldehyde dication after strong field ionization
Unusual trapping of an excited state of a dication observed after strong field ionization. Symmetry is responsible for forbidden nonradiative and radiative decay.
A neural network potential energy surface and quantum dynamics studies for the Ca+(2S) + H2 → CaH+ + H reaction
A globally accurate PES and dynamics studies for the Ca+(2S) + H2 → CaH+ + H reaction.
Analysis of measured high-resolution doublet rovibronic spectra and related line lists of 12CH and 16OH
Understanding the energy-levels and rovibronic spectra of the ethylidyne (CH) and the hydroxyl (OH) radicals is mandatory for a multitude of modelling efforts within multiple chemical, combustion, astrophysical, and atmospheric environments.
Performance of the nitrogen reduction reaction on metal bound g-C6N6: a combined approach of machine learning and DFT
DFT calculations assisted by machine-learning models predict tantalum (Ta) to be a suitable single-atom catalyst (SAC) for the nitrogen reduction reaction (NRR).
Mode selective chemistry for the dissociation of methane on efficient Ni/Pt-bimetallic alloy catalysts
Dissociation probability of CH4 dissociation on a surface depends on the symmetry of the minimum energy path, which in turn depends on the surface alloy compositions. The reaction path is symmetric, if the top layer is replaced by the guest metals.
Size-dependent H and H2 formation by infrared multiple photon dissociation spectroscopy of hydrated vanadium cations, V+(H2O)n, n = 3–51
Infrared multiple photon dissociation spectra of V+(H2O)n depend on experiment conditions, with strong kinetic shift effects for large clusters.
Representing globally accurate reactive potential energy surfaces with complex topography by combining Gaussian process regression and neural networks
A scheme for representing globally accurate reactive potential energy surfaces by combining Gaussian process regression and neural networks is proposed.
Ultrafast proton transfer of the aqueous phenol radical cation
Ultrafast spectroscopy and quantum dynamics simulations elucidate the ∼0.1 ps ultrafast proton transfer of photoionized aqueous phenol.
(De)localization dynamics of molecular excitons: comparison of mixed quantum-classical and fully quantum treatments
Exciton (de)localization dynamics in molecular dimers are analyzed using surface hopping and quantum dynamical calculations.
Optical absorption and shape transition in neutral SnN clusters with N ≤ 40: a photodissociation spectroscopy and electric beam deflection study
Quantum-chemically supported electric beam deflection and photodissociation spectroscopy reveal the shape evolution and optical absorption of small Sn clusters with focus on the rotational, vibrational, multiphoton and dissociation characteristics.
Atomistic simulation of the FEBID-driven growth of iron-based nanostructures
Irradiation-driven molecular dynamics simulations provide atomistic insights into the structure and morphology of metal deposits grown during the FEBID process.
About this collection
The focus of this Festschrift themed collection is dedicated to the recent studies of electronic and nuclear features of molecules and new materials, their structure and dynamics, interplay and coupling mechanisms in honour of Professor Wolfgang Ernst. The field of electronic and nuclear dynamics has grown rapidly in recent years due to the possibility of real-time observations through ultrafast laser technologies as well as improvements in theoretical and method development. The understandings of structural and dynamic properties of molecular systems, paired with new experimental possibilities in the time domain and femtosecond chemistry, help in the development of technologies in fields such as renewable energies and energy conversion, data processing and storage, or chemical sensing and catalysis.
Guest Edited by: Martina Havenith (Ruhr-Universität Bochum), Martin Sterrer (University of Graz), Andreas W. Hauser (Graz University of Technology), Markus Koch (Graz University of Technology)