A Universal Approach for Solving Real-World Problems Using Quantum Dynamics: Coherent States for Molecular Simulations (COSMOS)
Lead Research Organisation:
UNIVERSITY COLLEGE LONDON
Department Name: Chemistry
Abstract
Experiments using modern laser technologies and new light sources look at quantum systems undergoing dynamic change to understand molecular function and answer fundamental questions relevant to chemistry, materials and quantum technologies. Typical questions are: How can molecules be engineered for maximum efficiency during energy harvesting, UV protection or photocatalysis? What happens when strong and rapidly changing laser fields act on electrons in atoms and molecules? How fast do qubits lose information due to interactions with the environment? Will an array of interacting qubits in future quantum computers remain stable over long time-scales?
Interpreting time-resolved experiments that aim to answer these questions requires Quantum Dynamics (QD) simulations, the theory of quantum motion. QD is on the cusp of being able to make quantitative predictions about large molecular systems, solving the time-dependent Schrödinger equation in a way that will help unravel the complicated signals from state-of-the-art experiments and provide mechanistic details of quantum processes. However, important methodological challenges remain, such as computational expense and accurate prediction of experimental observables, requiring a concerted team-effort. Addressing these will greatly benefit the wider experimental and computational QD communities.
In this programme grant we will develop transformative new QD simulation strategies that will uniquely deliver impact and insight for real-world applications across a range of technological and biological domains. The key to our vision is the development, dissemination, and wide adaptation of powerful new universal software for QD simulations, building on our collective work on QD methods exploiting trajectory-guided basis functions. Present capability is, however, held back by the typically fragmented approach to academic software development. This lack of unification makes it difficult to use ideas from one group to improve the methods of another group, and even the simple comparison of QD simulation methods is non-trivial. Here, we will combine a wide range of existing methods into a unified code suitable for use by both computational and experimental researchers to model fundamental photo-excited molecular behaviour and interpret state-of-the-art experiments. Importantly we will develop and implement new mathematical and numerical ideas within this software suite, with the explicit objective of pushing the system-size and time-scale limits beyond what is currently accessible within "standard" QD simulations. Our unified code will lead to powerful and reliable QD methods, simultaneously enabling easy adoption by non-specialists; for the first time, scientists developing and using QD simulations will be able to access, develop and deploy a common software framework, removing many of the inter- and intra-community barriers that exist within the current niche software set-ups across the QD domain.
The transformative impact of method development and code integration is powerfully illustrated by electronic structure and classical molecular dynamics packages, used routinely by thousands of researchers around the world and recognised by several Nobel Prizes in the last few decades. Our programme grant aims to deliver a similar step-change by improving accessibility for QD simulations. Success in our programme grant would be the demonstrated increase in adoption of advanced QD simulations across a broad range of end-user communities (e.g. spectroscopy, materials scientists, molecular designers). Furthermore, by supporting a large yet integrated cohort of early-career researchers, this programme grant will provide an enormous acceleration to developments in QD, positioning the UK as a global leader in this domain as we move from the era of classical computation and simulation into the quantum era of the coming decades.
Interpreting time-resolved experiments that aim to answer these questions requires Quantum Dynamics (QD) simulations, the theory of quantum motion. QD is on the cusp of being able to make quantitative predictions about large molecular systems, solving the time-dependent Schrödinger equation in a way that will help unravel the complicated signals from state-of-the-art experiments and provide mechanistic details of quantum processes. However, important methodological challenges remain, such as computational expense and accurate prediction of experimental observables, requiring a concerted team-effort. Addressing these will greatly benefit the wider experimental and computational QD communities.
In this programme grant we will develop transformative new QD simulation strategies that will uniquely deliver impact and insight for real-world applications across a range of technological and biological domains. The key to our vision is the development, dissemination, and wide adaptation of powerful new universal software for QD simulations, building on our collective work on QD methods exploiting trajectory-guided basis functions. Present capability is, however, held back by the typically fragmented approach to academic software development. This lack of unification makes it difficult to use ideas from one group to improve the methods of another group, and even the simple comparison of QD simulation methods is non-trivial. Here, we will combine a wide range of existing methods into a unified code suitable for use by both computational and experimental researchers to model fundamental photo-excited molecular behaviour and interpret state-of-the-art experiments. Importantly we will develop and implement new mathematical and numerical ideas within this software suite, with the explicit objective of pushing the system-size and time-scale limits beyond what is currently accessible within "standard" QD simulations. Our unified code will lead to powerful and reliable QD methods, simultaneously enabling easy adoption by non-specialists; for the first time, scientists developing and using QD simulations will be able to access, develop and deploy a common software framework, removing many of the inter- and intra-community barriers that exist within the current niche software set-ups across the QD domain.
The transformative impact of method development and code integration is powerfully illustrated by electronic structure and classical molecular dynamics packages, used routinely by thousands of researchers around the world and recognised by several Nobel Prizes in the last few decades. Our programme grant aims to deliver a similar step-change by improving accessibility for QD simulations. Success in our programme grant would be the demonstrated increase in adoption of advanced QD simulations across a broad range of end-user communities (e.g. spectroscopy, materials scientists, molecular designers). Furthermore, by supporting a large yet integrated cohort of early-career researchers, this programme grant will provide an enormous acceleration to developments in QD, positioning the UK as a global leader in this domain as we move from the era of classical computation and simulation into the quantum era of the coming decades.
Organisations
- UNIVERSITY COLLEGE LONDON (Lead Research Organisation)
- University Paris-Saclay (Project Partner)
- Imperial College London (Project Partner)
- University of Ottawa (Project Partner)
- Autonomous University of Madrid (Project Partner)
- University of Valencia (Project Partner)
- Institut Charles Gerhardt Montpellier (Project Partner)
- Goethe University Frankfurt (Project Partner)
- Swiss Federal Inst of Technology (EPFL) (Project Partner)
- University of St Andrews (Project Partner)
- University of Heidelberg (Project Partner)
- Ruder Boskovic Institute (Project Partner)
- Nantes University (Project Partner)
- CECAM (Euro Ctr Atomic & Molecular Comp) (Project Partner)
- University of Salamanca (Project Partner)
- Louisiana State University (Project Partner)
- University of Nebraska-Lincoln (Project Partner)
- University of Groningen (Project Partner)
- University of Sheffield (Project Partner)
- UNSW Canberra (Project Partner)
- Max Born Institute for Nonlinear Optics (Project Partner)
- Los Alamos National Laboratory (Project Partner)
- ETH Zurich (Project Partner)
- Brown University (Project Partner)
- Central Laser Facility (Project Partner)
- National Research Council (CNR) Italy (Project Partner)
- Kansas State University (Project Partner)
- University of Edinburgh (Project Partner)
- University of Toronto (Project Partner)
Publications

Ahmad S
(2024)
Conformational Control of Donor-Acceptor Molecules Using Non-covalent Interactions
in The Journal of Physical Chemistry A

Ahmad S
(2024)
Towards the accurate simulation of multi-resonance emitters using mixed-reference spin-flip time-dependent density functional theory
in Organic Electronics

Barlow K
(2024)
Tracking nuclear motion in single-molecule magnets using femtosecond X-ray absorption spectroscopy
in Nature Communications

Bennett O
(2024)
Prediction through quantum dynamics simulations: Photo-excited cyclobutanone.
in The Journal of chemical physics

Brook R
(2024)
Full wave function cloning for improving convergence of the multiconfigurational Ehrenfest method: Tests in the zero-temperature spin-boson model regime.
in The Journal of chemical physics

Cigrang L
(2024)
Modeling Photodissociation: Quantum Dynamics Simulations of Methanol
in The Journal of Physical Chemistry A

Cooper J
(2024)
Valence shell electronically excited states of norbornadiene and quadricyclane
in The Journal of Chemical Physics

Curchod B
(2024)
Perspective on Theoretical and Experimental Advances in Atmospheric Photochemistry
in The Journal of Physical Chemistry A

Dey D
(2024)
On the multiphoton ionisation photoelectron spectra of phenol.
in Physical chemistry chemical physics : PCCP