You can find the new paper describing the OpenMolcas package in JCTC – OpenMolcas: From source code to insight. OpenMolcas represents the open-source release of the previously commercially distributed Molcas package. Use OpenMolcas to gain access to powerful multireference methods for free and to have full control if you need to modify the source.
My own contributions to Molcas are concerned with the implementation of the wavefunction analysis module &WFA , as described in JCTC 13, 5343 (2017), and the interface to Columbus. Let me know if you have any questions about these.
Our paper “Strong Influence of Decoherence Corrections and Momentum Rescaling in Surface Hopping Dynamics of Transition Metal Complexes” was just accepted in JCTC. In this work we investigated the reliability of the surface hopping method in the case of a transition metal complex described using a linear vibronic coupling model. We found that various seemingly unimportant parameters can have a strong influence on the results.
Our new paper Effect of Symmetric and Asymmetric Substitution on the Optoelectronic Properties of 9,10-Dicyanoanthracene, written in collaboration with colleagues from Imperial College London, TU Vienna, University of Geneva, and the Polish Academy of Sciences just appeared in the new RSC journal Molecular Systems Design & Engineering. The paper illustrates design principles relevant for strong two-photon absorbers. The best two-photon absorption is obtained by using a symmetric D-A-D arrangement with sufficiently strong donors.
The challenge about running photodynamics simulations is that the computational cost is often so high that one might have to compromise in terms of the electronic structure method used. One is tempted to just check the vertical excitations at one geometry and run the dynamics if those look alright. How this can go wrong is investigated in the paper “The Influence of the Electronic Structure Method on Intersystem Crossing Dynamics. The Case of Thioformaldehyde” that just appeared in JCTC. Take a look if you are interested.
Copyright 2019 American Chemical Society.
Small modifications can make a big difference. Swapping anthraquinone for a thiophene based acceptor in a donor-acceptor-donor system produces the desired red shift in the emission but limits its quantum efficiency. This conclusion was drawn from a recent paper lead by Stephanie Montanaro and Iain Wright at Loughborough: Red-shifted delayed fluorescence at the expense of photoluminescence quantum efficiency – an intramolecular charge-transfer molecule based on a benzodithiophene-4,8-dione acceptor which just a appeared in PCCP.
Computations reveal that the reason for the reduced emission quantum efficiency lies in the presence of low-lying locally excited states (4 triplets and one singlet) on the central unit.
A joint experimental and computational study with groups from Vienna and Geneva just appeared in Sci. Rep.: “Wavelength-optimized Two-Photon Polymerization Using Initiators Based on Multipolar Aminostyryl-1,3,5-triazines.” In this paper, the two-photon absorption properties of a new class of aminostyryl-triazines were investigated showing good agreement between experiment and computation. Furthermore, the practical applicability of these molecules for 3D-printing was shown.
Another paper working on improving the efficiency of surface hopping dynamics just appeared, this time in JCTC: “Surface hopping within an exciton picture – An electrostatic embedding scheme.” authored by M. F. S. J. Menger, F. Plasser, B. Mennucci, and L. González. In this paper, we explored the possibility of running nonadiabatic dynamics simulations within an exciton model. The main challenge in this endeavour was to derive a consistent energy expression for combining QM/MM electrostatic embedding calculations of the different chromophores.
To test the implementation, we ran simulations on a molecular dyad, where full TDDFT nonadiabatic dynamics simulations were available. Good agreement was found.
The method was implemented in the SHARC molecular dynamics package.
A new paper co-authored by F. Plasser just appeared in PCCP: “Highly efficient surface hopping dynamics using a linear vibronic coupling model.” The paper shows that it is possible to perform photodynamics simulations of nonadiabatic processes, such as internal conversion and intersystem crossing, at virtually no cost.
The book chapter “General Trajectory Surface Hopping Method for Ultrafast Nonadiabatic Dynamics” written by S. Mai, F. Plasser, P. Marquetand, and L. González of the book Attosecond Molecular Dynamics edited by M. J. J. Vrakking and F. Lepine just appeared online. Download and read it if you are interested in getting an introduction into nonadiabatic surface hopping dynamics.