Extended software development workshop in quantum dynamics

Basile was a co-organizer with Dr. Federica Agostini and Dr. Ari P. Seitsonen of the Extended Software Development Workshop (ESDW) in quantum dynamics, which took place in the “Maison de la Simulation” near Paris. Morning sessions were dedicated to the scientific presentations and HPC training, while coding sessions took place every afternoon. The central goal of this event was to further extend the E-CAM library of software for quantum dynamics, as well as to stimulate future developments in the field.

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Participants of the ESDW 2018.

More information about E-CAM software repositories can be found here.

 

How good are the approximations of Ab Initio Multiple Spawning?

Ab Initio Multiple Spawning (AIMS) is a method that allows for accurate yet efficient excited-state molecular dynamics. It portrays nuclear wavepackets as linear combinations of coupled Gaussian functions that follow classical trajectories. (See our recent review for a detailed discussion on this method.)

AIMS emerges from the (formally-exact) Full Multiple Spawning framework by invoking two central approximations related to the coupling between Gaussian functions. While AIMS has been successfully employed to simulate the photochemistry of numerous molecules, a detailed analysis of the strengths and weaknesses of its underlying approximations was missing in the literature.

Together with Dr. Benoît Mignolet (University of Liège), we investigated in great details the approximations in AIMS using a model molecule, LiH, photoexcited by an external electric field to generate interfering nuclear wavepackets. Interestingly, AIMS could capture the behavior of properties like electronic state populations and the more challenging time-dependent molecular dipole moment, even if this low-dimensional system constitutes one of the worst-case scenarios for the AIMS approximations. We furthermore proposed and validated strategies, compatible with the simulation of larger molecular systems, to overcome some potential shortcomings of these approximations.

(On a less serious note, this article is also the first one of the group fulfilling the requirements of the Palatinate Challenge.)

A walk through the approximations of ab initio multiple spawning, by Benoît Mignolet and Basile F. E. Curchod, J. Chem. Phys., 148, 134110 (2018).

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West Coast Theoretical Chemistry Symposium & TeraChem/FMS developer meeting

Basile attended the West Coast Theoretical Chemistry Symposium, organized at Stanford University for the 50th birthday of Todd J. Martínez.

This Symposium was directly followed by the first TeraChem/FMS developer meeting. TeraChem is a GPU-accelerated quantum chemical package that can be interfaced with the nonadiabatic dynamics method Full Multiple Spawning (FMS). Both codes are used in the ISP group and this developer meeting was an exciting opportunity to discuss their future directions and developments.

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Participants to the first TeraChem/FMS developer meeting, in front of the Old Chemistry Building at Stanford University.

 

CECAM School on Nonadiabatic Dynamics

From February 26 to March 2, Basile co-organized a CECAM School entitled “Nonadiabatic Molecular Dynamics in Three Different Flavors” with Todd Martínez (Stanford University), Graham Worth (University College London), and Ivano Tavernelli (IBM Zürich). The School took place at the CECAM Headquarter in Lausanne (Switzerland).

https://www.cecam.org/workshop-1396.html

The central idea of this School was to introduce the 40 participants to general concepts of computational photochemistry as well as three distinct methods for nonadiabatic molecular dynamics: Multiconfiguration Time-Dependent Hartree (MCTDH), Ab Initio Multiple Spawning (AIMS), and Trajectory Surface Hopping (TSH). The morning was dedicated to lectures for each method, and exercises on the computer were organized each afternoon. The main goal of these exercises was for the participants to play with each technique and to be able to use them, maybe, in their own research.

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Intensive coffee breaks
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Group picture on the last day of the School.

 

Review on nonadiabatic quantum dynamics methods

What happens to a molecule after it absorbs light? Have a look at our review freshly published in Chemical Reviews to discover different theoretical approaches that aim to answer this question. We focus our attention on nonadiabatic frameworks that can be derived from the time-dependent molecular Schrödinger equation and employ traveling Gaussian functions to describe nuclear wavefunctions. We discuss in details the different approximations used to produce methods that are compatible with an on-the-fly propagation of the Schrödinger equation for molecules in their full configuration space, such as Ab Initio Multiple Spawning (AIMS), MultiConfigurational Ehrenfest (MCE), or variational Multi-Configurational Gaussian (vMCG).

Ab Initio Nonadiabatic Quantum Molecular Dynamics, by Basile F. E. Curchod and Todd J. Martínez, Chemical Reviews (2018). DOI: 10.1021/acs.chemrev.7b00423

(No, this wasn’t a competition on the maximum number of adjectives one can we used to qualify “dynamics”.)

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COST Workshop on the interaction between light and molecules in interstellar space

Basile organized with Petr Slavíček, Eva Muchova, and Jean-Hugues Fillion, a workshop entitled “Formation and destruction of molecules by UV and X-ray radiation”, in the context of the COST Action “Our Astro-Chemical History“. This workshop took place at the University of Bristol and triggered very stimulating discussions between theoretical and experimental chemists on the effect of UV and X-ray radiations on molecules in interstellar space.

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Picture from http://cost.obs.ujf-grenoble.fr/outreach