Tutorial Review
Review of the foundations of time-dependent density-functional theory (TDDFT)
At present, TDDFT is based entirely on the mathematical Runge–Gross mapping theorems, not backed by a variational or stationarity principle. Contrary to the prevailing view, this does not provide a valid foundation of the theory.
Paper
The density-based many-body expansion for poly-peptides and proteins
By combining the MFCC fragmentation scheme with dimer interactions as well as a density-based correction, we are able to devise a fragmentation scheme for polypeptides and proteins that reaches chemical accuracy across different structural motifs.
Paper
Analyzing spectral distributions of charge transfer character in ensembles: a case study on the reaction center of photosystem II
Mixing and reordering of electronic states in a nuclear ensemble is resolved with analysis in a unified basis of reference states. Application to the reaction center of photosystem II identifies the pigments responsible for primary charge separation.
Paper
Density functional benchmark for quadruple hydrogen bonds
Hydrogen-bonding strengths of quadruply bonded self-complementary dimers are calculated using 152 density functional approximations and compared to high-level coupled-cluster energies.
Low-lying excited states of linear all-trans polyenes: the σ–π electron correlation and the description of ionic states
Accurately describing ionic states requires addressing basis-set effects, size-extensivity errors, and, most importantly, σ–π electron correlation.
Paper
Substituted acridones: simple deep blue HIGHrISC emitters in an aprotic environment
The properties of N-methylacridone as a potential deep blue OLED emitter are strongly improved by donating substituents at positions 2 and 7.
Carotenoid radical formation after multi-photon excitation of 8′-apo-β-carotenal
Excitation of 8′-apo-β-carotenal by 1300 nm ultrashort pulses leads to a four-photon excitation of a dark state, which is a precursor of carotenoid radical formation in a polar solvent.
Paper
Accurate incorporation of hyperfine coupling in diabatic potential models using the effective relativistic coupling by asymptotic representation approach
The accurate treatment of relativistic couplings like spin–orbit (SO) coupling into diabatic potential models is highly desirable.
Paper
Energy transfer booster: how a leaving group controls the excited state pathway within a caging BASHY–BODIPY dyad
A leaving group (LG) enhances excitation energy transfer (EET) in a dyad from the donor BASHY to the acceptor BODIPY. In the photoproduct, absence of the LG strongly reduces EET efficiency, resulting in fluorescence primarily from the donor moiety.
Photoinduced formation of a platina-α-lactone – a carbon dioxide complex of platinum. Insights from femtosecond mid-infrared spectroscopy
The oxalate precursor, oxaliplatin, is used to generate a carbon dioxide complex of platinum – a species, which can be regarded as a metalla-α-lactone.
Paper
Energy decomposition analysis for excited states: an extension based on TDDFT
Energy decomposition analysis (EDA) is extended by the excited state EDA (exc-EDA) using time-dependent density functional theory (TDDFT). Validated through studies on exciplexes, it demonstrates utility by singlet fission in pentacene.
Impact of solvation on the electronic resonances in uracil
Two types of electronic resonances are formed in uracil, by attaching an electron to the ground or excited states. Bulk and microsolvation effects on these resonances are examined.
Paper
Ultra-wide band near-infrared (NIR) optical thermometry (12–673 K) performance enhanced by Stark sublevel splitting in Er3+ ions near the first biological window in the PbZr0.53Ti0.47O3:Er3+/Yb3+ phosphor
NIR optical thermometry across a broad temperature range (12–673 K) was explored using FWHM and FIR as sensing parameters. Stark splitting in Er3+ ions was analyzed through parametric modelling and Gaussian distribution to deconvolute NIR emissions.
Control of electronic and exchange coupling by bridge substituents in donor acceptor triads with triptycene bridges
Triptycene-bridged dyads as ideal systems to prove inverse bridge energy dependence of electron transfer coupling.
About this collection
The themed collection ‘Festschrift for Christel Marian: The role of electron spin in molecular photochemical and photophysical processes: Theory and experiment’ brings together a broad range of studies, including both recent methodological developments and novel applications.
The focus of this Festschrift themed collection is dedicated to recent developments of (i) quantum mechanical methods for excited electronic state properties (e.g. energies, gradients, non-adiabatic, spin-spin, and spin-orbit couplings), (ii) theoretical strategies to study excited-state dynamics ranging from full-dimensional semiclassical on-the-fly dynamics to full quantum dynamics in reduced dimensionality, (iii) embedding methods to describe excited-state processes complex environments, as well as (iv) experimental and theoretical studies on a wide range of applications, e.g. excited-state processes and quantum effects in biological systems, organic light emitting diodes, metal organic frameworks, and renewable energy devices.
Guest Edited by Prof. Dr Shirin Faraji (Heinrich Heine University Düsseldorf), Prof. Dr Andreas Dreuw (University of Heidelberg), Prof. Dr Bernd Engels (University of Würzburg), Dr Martin Kleinschmidt (Heinrich Heine University Düsseldorf).