N ILICO HOTOCHEMISTRY ROUP - WordPress.comelusive excited-dynamics of organic molecules and metal...
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I N S ILICO P HOTOCHEMISTRY G ROUP B ASILE F. E. C URCHOD BASILE . F . CURCHOD @ DURHAM . AC . UK D EPARTMENT OF C HEMISTRY ,D URHAM U NIVERSITY RESEARCH INTERESTS Our research focuses on the development and the applications of theoretical methods for simulating the dynamics of molecules beyond the Born-Oppenheimer approximation, i.e., when the coupling between electronic and nuclear motion cannot be neglected and leads to the appearance of the so-called nonadiabatic effects. The breakdown of the Born-Oppenheimer approximation is common for photoinduced and electron-transfer processes, e.g. photochemical reactions, photosynthesis, solar cells, retinal isomerization in the primary step of vision, chemiluminescence, or in atmospheric chemistry, and leads to fascinating phenomena. In fact, nonadiabatic effects are ubiquitous as soon as a given chemical process requires more than one electronic state for its descrip- tion, but their theoretical description remains an important and arduous challenge due to the necessity of revisiting several critical approximations commonly employed in theoretical chemistry. The main pillars of our scientific research are the development and the application of theoretical methods for studying the dynamics of molecules in their electronically excited states. In Silico P HOTOCHEMISTRY –A PPLICATIONS FROM E NERGY -R ELATED D EVICES TO A TMOSPHERIC C HEMISTRY One important component of a more responsible energy consumption pol- icy is saving energy, which can only be achieved via the development and use of more efficient technologies in domains such as light produc- tion, for example. Organic light-emitting diodes (OLEDs) are a good example of a highly efficient lighting source. However, this technology still suffers from important limitations – notably related to internal degra- dation events – preventing its general usage as an efficient and reliable lighting device, as compared to LED for example. In this project, we will combine different theoretical and computational methodologies to investigate the elusive excited-dynamics of organic molecules and metal complexes that comprise OLEDs. Earth’s atmosphere is a massive photochemical reactor, and human activities are changing its chemical composition, impacting both climate change and air pollution. Interestingly, the reactions of volatile organic compound (VOC) in- termediates upon light absorption remain largely unexplored, even though an important number of key reactions in atmospheric chemistry implies photo- chemical processes, or generates intermediates that are potential photoactive molecules. In this project, we will study the role of nonadiabatic effects in the excited- state reaction dynamics of oxidation intermediates in atmospheric VOC chemistry, in close collaboration with experimental atmospheric groups. THEORETICAL DEVELOPMENTS We are working on a newly- introduced theory, coined Exact Factorization, which goes beyond the concept of nuclear wavepackets evolving on potential energy surfaces. We focus on understanding how the Exact Factorization alters our BO representation of photochemistry. METHODS DEVELOPMENT One of the main interests of the group is the development of new methods for nonadiabatic molecular dynamics, for example based on the Full Multiple Spawning framework, which describes nuclear wavepack- ets as a combination of coupled traveling Gaussians. We also use graphical processing units (GPUs) for accelerating the electronic structure calculations re- quired for ab initio nonadiabatic dy- namics. COLLABORATIONS Todd J. Martínez (Stanford U.), Fed- erica Agostini (U. Paris-Sud), Benoît Mignolet (U. Liège), Tom Penfold (U. Newcastle), Bristol Dynamics Group. KEY REFERENCES T: J. Phys. Chem. Lett., 8, 831 (2017). D: J. Chem. Phys., 144, 101102 (2016). A: Angew. Chem. Int. Ed., 55, 14993 (2016). OPENINGS A fully-funded PhD position in Theo- retical and Computational Chemistry is available in the group, starting ide- ally in September 2018. FURTHER INFO www.in-silico-photochem.com T: +44 (0) 191 334 4065 CG301, Department of Chemistry Durham University
Transcript of N ILICO HOTOCHEMISTRY ROUP - WordPress.comelusive excited-dynamics of organic molecules and metal...
IN SILICO PHOTOCHEMISTRY GROUPBASILE F. E. CURCHOD
DEPARTMENT OF CHEMISTRY, DURHAM UNIVERSITY
RESEARCH INTERESTS
Our research focuses on the development and the applications of theoretical methodsfor simulating the dynamics of molecules beyond the Born-Oppenheimer approximation, i.e.,when the coupling between electronic and nuclear motion cannot be neglected and leadsto the appearance of the so-called nonadiabatic effects.The breakdown of the Born-Oppenheimer approximation is common for photoinducedand electron-transfer processes, e.g. photochemical reactions, photosynthesis, solar cells,retinal isomerization in the primary step of vision, chemiluminescence, or in atmosphericchemistry, and leads to fascinating phenomena. In fact, nonadiabatic effects are ubiquitousas soon as a given chemical process requires more than one electronic state for its descrip-tion, but their theoretical description remains an important and arduous challenge due tothe necessity of revisiting several critical approximations commonly employed in theoreticalchemistry.
The main pillars of our scientific research are the development and the application of theoretical methods for studyingthe dynamics of molecules in their electronically excited states.
In Silico PHOTOCHEMISTRY – APPLICATIONS FROM ENERGY-RELATED DEVICES TO ATMOSPHERIC CHEMISTRY
One important component of a more responsible energy consumption pol-icy is saving energy, which can only be achieved via the developmentand use of more efficient technologies in domains such as light produc-tion, for example. Organic light-emitting diodes (OLEDs) are a goodexample of a highly efficient lighting source. However, this technologystill suffers from important limitations – notably related to internal degra-dation events – preventing its general usage as an efficient and reliablelighting device, as compared to LED for example. In this project, we willcombine different theoretical and computational methodologies to investigate theelusive excited-dynamics of organic molecules and metal complexes that compriseOLEDs.
Earth’s atmosphere is a massive photochemical reactor, and human activitiesare changing its chemical composition, impacting both climate change and airpollution. Interestingly, the reactions of volatile organic compound (VOC) in-termediates upon light absorption remain largely unexplored, even though animportant number of key reactions in atmospheric chemistry implies photo-chemical processes, or generates intermediates that are potential photoactivemolecules. In this project, we will study the role of nonadiabatic effects in the excited-state reaction dynamics of oxidation intermediates in atmospheric VOC chemistry, inclose collaboration with experimental atmospheric groups.
THEORETICAL DEVELOPMENTS
We are working on a newly-introduced theory, coined ExactFactorization, which goes beyondthe concept of nuclear wavepacketsevolving on potential energy surfaces.We focus on understanding howthe Exact Factorization alters our BOrepresentation of photochemistry.
METHODS DEVELOPMENT
One of the main interests of thegroup is the development of newmethods for nonadiabatic moleculardynamics, for example based on theFull Multiple Spawning framework,which describes nuclear wavepack-ets as a combination of coupledtraveling Gaussians.We also use graphical processingunits (GPUs) for accelerating theelectronic structure calculations re-quired for ab initio nonadiabatic dy-namics.
COLLABORATIONS
Todd J. Martínez (Stanford U.), Fed-erica Agostini (U. Paris-Sud), BenoîtMignolet (U. Liège), Tom Penfold (U.Newcastle), Bristol Dynamics Group.
KEY REFERENCES
T: J. Phys. Chem. Lett., 8, 831 (2017).D: J. Chem. Phys., 144, 101102 (2016).A: Angew. Chem. Int. Ed., 55, 14993(2016).
OPENINGS
A fully-funded PhD position in Theo-retical and Computational Chemistryis available in the group, starting ide-ally in September 2018.
FURTHER INFO
www.in-silico-photochem.comT: +44 (0) 191 334 4065CG301, Department of ChemistryDurham University
