Molim Working Group 3:

Ab-Initio Modelling of Molecular Processes Under Confinement


We cordially invite members of MOLIM's Working Group 3 (COST Action CM1405) as well as all interested parties to Madrid, for the second Working Group 3 meeting. It will be dedicated to a better understanding and recognition of issues relevant to the development of novel computational approaches for the simulation of nuclear motion under spatial, optical, electric or magnetic confinement. It is an opportunity for active networking between action members with complementary and highly diverse expertise in fields such as spectroscopy, the modelling of weak inter-molecular interactions, quantum dynamics and large-scale molecular dynamics. The participants will be given a chance to present their research through introductory talks at the meeting, but large amounts of time will also be reserved to the active discussion of interdisciplinary models which extend the currently available tools and approaches.

The meeting will take place in Madrid, Spain, at the Centro de Física Miguel Antonio Catalán (CSIC, Serrano 123, 28006 Madrid). It will start on the 3rd of December in the morning and end on Wednesday, the 5th of December before lunch. Presentation time is 30 minutes (25+5 min) for invited lectures and 20 minutes (17+3 min) for invited contributed talks. Additionally, a poster session is planned for Tuesday afternoon.

The meeting includes the discussion of work in progress on the following MoU issues:

  1. 1. Nuclear Embedding: Work is in progress on a static DFT code to describe superfluid helium nanodroplets, having incorporated a tool to generate an embedding potential. The idea is to interface it with QMC, FCI-NO, or alternative methods which allow an accurate treatment of molecular motion for systems embedded in a superfluid He environment, with an emphasis on the microscopic molecular superfluidity response. The dynamic time-dependent form of He-DFT will also be discussed.

  2. 2. Ab-initio characterization of dynamic processes such as chemical reactions (oxidation, dehydrogenation, combustion processes and coking), electronic excitation, diffusion and alloying in nanomaterials. Work is in progress on ab-initio schemes to study the reactivity of molecular oxygen and other small molecules with metallic and mixed-metallic nanoparticles, including unsupported as well as surface-deposited clusters or nanoparticles in solution. This proposition is directly linked to the evaluation of current approaches towards accurate thermochemistry data, i.e., to the calculation of Gibbs energies as a function of (e.g. oxygen) pressure and temperature for any stationary point on the relevant energy landscapes, also including transition states for a realistic prediction of chemical reactivity.

  3. 3.Ab-initio modelling of the new generation of Angstrom-sized catalysts and photocatalysts based on bare metal clusters. The theory developed for metal nanoparticles and bulk materials does not apply at the bottom scale of nanotechnology. This molecular-like species has extraordinary and unexpected stability, which is still to be understood.

  4. 4. Ab-initio (classical and semiclassical) molecular dynamics (MD) simulations of molecular reactivity within helium nanodroplets (and other liquids) as well as that induced by laser pulses, with an emphasis on non-adiabatic processes. A mid-term goal will be to interface large-scale MD codes with open source electronic structure codes.

  5. 5. Studying the influence of light-matter interaction on molecular motion. Interaction with NIR to UV light can affect molecular motion through a direct promotion into an electronically excited state followed by a significantly different interaction with its local environment and/or the excitation of higher vibrational modes (overtones) of the electronic ground state, opening the possibility to redistribute energy over different degrees of freedom in the system via internal energy relaxation processes. Particularly interesting challenges could be the description of directional forces acting on chiral molecules through light in the context of racemic separation.

  6. 6. Accurate spectroscopic characterization of molecular complexes as a first step toward the understanding of intermolecular interactions in condensed phase.

  7. 7. Simplified physical models combined with accurate quantum-chemical approaches to quantitatively describe and interpret electronic, structural and vibrational properties of solid compounds as a function of temperature.

  8. 8.Enhancement and tailoring of photocatalytic and photovoltaic behaviour of semiconductors surfaces such as TiO2 by means of metallic nanocluster and atomcluster decoration. Charge transfer between the metallic adsorbates and the substrate alters strongly the electronic band structure of the system with a remarkable influence in the photo-excitation response. We will discuss computationally feasible approaches to calculate relevant properties such as light absorption and photo-mobilities.

  9. 9. Quantum coherent control strategies of molecular processes in complexes aiming at reaching the condensed phase limit.

  10. 10. Molecular dynamics simulations have become an essential tool to investigate biological problems. However, the latter still propose a large challenge in terms of the necessary meso-scaling approaches.

  11. 11. Simultaneous treatments of electrons and atomic nuclei. A goal is to reflect on rigorous non-BO methods which can be implemented in existing codes of standard packages and remain applicable also to larger systems, including molecular systems under confinement.


Second Working Group 3 Meeting: Ab-Initio Modelling of Molecular Processes Under Confinement

C.S.I.C. (Madrid , Spain) Dec 3-5 2018