A Joined-up Approach for New Molecular Simulation Technologies To Harness Ultrafast Photochemistry
Lead Research Organisation:
Heriot-Watt University
Department Name: Sch of Engineering and Physical Science
Abstract
Light triggers many important chemical reactions. These include photosynthesis, which converts sunlight to chemical energy and powers most life on earth, human vision, where light is detected using the light-induced isomerisation of a molecule in our retinas, and new technologies such as photodynamic therapies for cancer, photocatalysis, molecular photonics, photovoltaics, and organic light-emitting diodes in displays. Ultrafast imaging experiments that study these types of processes rely on computational modelling to interpret and analyse data and extract chemical and physical insight from the observations. Yet, the computational modelling remains very challenging, in essence because the photon ('light-particle') absorbed by a molecule in a photochemical process carries a large amount of energy, which forces the electrons and nuclei into complex coupled motion described by quantum mechanics, making computations exponentially more difficult than the corresponding system described by classical mechanics. The necessary calculations are composed of two different types of computations, which both require great technical expertise: electronic structure calculations and quantum dynamics.
We will combine our expertise in electronic structure calculations and quantum dynamics, to create powerful new simulation methods. The team includes two world-leading experimentalists who are each expert in a complementary ultrafast imaging technique. As a team, we will push experiments and theory to achieve greater insight into complex light-activated dynamics in molecules. The project will provide a framework for interpreting multiple complementary state-of-the-art experiments. The long-term goal is to achieve simulations that are sufficiently powerful that we can use computers to design new photoactive molecules for new light-driven technologies. In the later stages of the project, we will tackle complex molecular systems well beyond the current cutting-edge of simulations, which will include exciting applications such as photosensitizers, photostabilizers, photoactive pro-drugs, photovoltaics, photocatalysts, and light-emitting diodes.
We will combine our expertise in electronic structure calculations and quantum dynamics, to create powerful new simulation methods. The team includes two world-leading experimentalists who are each expert in a complementary ultrafast imaging technique. As a team, we will push experiments and theory to achieve greater insight into complex light-activated dynamics in molecules. The project will provide a framework for interpreting multiple complementary state-of-the-art experiments. The long-term goal is to achieve simulations that are sufficiently powerful that we can use computers to design new photoactive molecules for new light-driven technologies. In the later stages of the project, we will tackle complex molecular systems well beyond the current cutting-edge of simulations, which will include exciting applications such as photosensitizers, photostabilizers, photoactive pro-drugs, photovoltaics, photocatalysts, and light-emitting diodes.
Publications
Broumidis E
(2023)
The Photochemical Mediated Ring Contraction of 4 H -1,2,6-Thiadiazines To Afford 1,2,5-Thiadiazol-3(2 H )-one 1-Oxides
in Organic Letters
Coe JP
(2022)
Efficient Computation of Two-Electron Reduced Density Matrices via Selected Configuration Interaction.
in Journal of chemical theory and computation
Craciunescu L
(2023)
Excited-state van der Waals potential energy surfaces for the NO A2S+ + CO2X1Sg+ collision complex
in The Journal of Chemical Physics
Craciunescu L
(2025)
Selected configuration interaction for high accuracy and compact wave functions: Propane as a case study.
in The Journal of chemical physics
Crane SW
(2023)
The Value of Different Experimental Observables: A Transient Absorption Study of the Ultraviolet Excitation Dynamics Operating in Nitrobenzene.
in The journal of physical chemistry. A
Gaensicke V
(2025)
New insights into bioactive Ga( iii ) hydroxyquinolinate complexes from UV-vis, fluorescence and multinuclear high-field NMR studies
in Dalton Transactions
Garrow M
(2025)
Excited state dynamics of azanaphthalenes reveal opportunities for the rational design of photoactive molecules
in Communications Chemistry
He H
(2024)
Ultra-fast laser pulses as a probe of electron dynamics: A next generation QTAIM perspective
in Chemical Physics Letters
Hutton L
(2024)
Using a multistate mapping approach to surface hopping to predict the ultrafast electron diffraction signal of gas-phase cyclobutanone.
in The Journal of chemical physics
Kotsina N
(2022)
Photochemical carbon-sulfur bond cleavage in thioethers mediated via excited state Rydberg-to-valence evolution.
in Physical chemistry chemical physics : PCCP
Leng JG
(2024)
Inelastic scattering of NO(A2S+) + CO2: rotation-rotation pair-correlated differential cross sections.
in Faraday discussions
Li Z
(2022)
Next generation quantum theory of atoms in molecules for the design of emitters exhibiting thermally activated delayed fluorescence with laser irradiation.
in Journal of computational chemistry
Li Z
(2021)
Control of chirality, bond flexing and anharmonicity in an electric field
in International Journal of Quantum Chemistry
Liu J
(2023)
A Concerted Redox- and Light-Activated Agent for Controlled Multimodal Therapy against Hypoxic Cancer Cells
in Advanced Materials
Lomas J
(2024)
A multimass velocity-map and covariance-map imaging study of the dissociative electron ionisation dynamics of carbonyl sulphide (OCS)
in Journal of Physics B: Atomic, Molecular and Optical Physics
Luxford TFM
(2023)
Differential Cross Sections for Pair-Correlated Rotational Energy Transfer in NO(A2S+) + N2, CO, and O2: Signatures of Quenching Dynamics.
in The journal of physical chemistry. A
Malcomson T
(2022)
Protocols for Understanding the Redox Behavior of Copper-Containing Systems.
in ACS omega
Mi XP
(2024)
Response of the mechanical and chiral character of ethane to ultra-fast laser pulses.
in Journal of computational chemistry
Moreno Carrascosa A
(2022)
Towards high-resolution X-ray scattering as a probe of electron correlation.
in Physical chemistry chemical physics : PCCP
Plackett E
(2024)
Structural dynamics around a hydrogen bond: Investigating the effect of hydrogen bond strengths on the excited state dynamics of carboxylic acid dimers.
in The Journal of chemical physics
Prentice AW
(2023)
Modular Approach to Selected Configuration Interaction in an Arbitrary Spin Basis: Implementation and Comparison of Approaches.
in Journal of chemical theory and computation
Robertson C
(2024)
Correction: Velocity map images from surface-hopping; reactive scattering of OH (2S+) + H2 (1S+g).
in Chemical communications (Cambridge, England)
Robertson C
(2022)
Velocity map images from surface-hopping; reactive scattering of OH (2S+) + H2 (1S+g).
in Chemical communications (Cambridge, England)
Saalbach L
(2021)
Ultraviolet Excitation Dynamics of Nitrobenzenes.
in The journal of physical chemistry. A
Shi H
(2021)
DNA-Intercalative Platinum Anticancer Complexes Photoactivated by Visible Light
in Chemistry - A European Journal
Soulié C
(2022)
Molecular properties and excited state van der Waals potentials in the NO A2S+ + O2 XSg- collision complex.
in Physical chemistry chemical physics : PCCP
Soulié C
(2022)
Multistate electronic quenching: Nonadiabatic pathways in NO A 2S+ + O2X 3Sg - scattering.
in The Journal of chemical physics
Taylor D
(2022)
4,7-Diarylbenzo[ c ][1,2,5]thiadiazoles as fluorophores and visible light organophotocatalysts
in Organic Chemistry Frontiers
Taylor D
(2023)
Regioselective electrophilic aromatic borylation as a method for synthesising sterically hindered benzothiadiazole fluorophores.
in RSC advances
Taylor D
(2024)
Immobilisation of benzo[ c ][1,2,5]thiadiazole (BTZ) within polymers of intrinsic microporosity (PIMs) for use in flow photochemistry
in Journal of Materials Chemistry A
Walker SE
(2021)
Steric control of sorting regimes in self-assembled cages.
in Chemical communications (Cambridge, England)
Xu T
(2021)
Chirality without Stereoisomers: Insight from the Helical Response of Bond Electrons.
in Chemphyschem : a European journal of chemical physics and physical chemistry
Xu T
(2022)
Corrigendum: Chirality without Stereoisomers: Insight from the Helical Response of Bond Electrons.
in Chemphyschem : a European journal of chemical physics and physical chemistry
Xue X
(2021)
Photoactivated Osmium Arene Anticancer Complexes.
in Inorganic chemistry
Zhou X
(2024)
Chirality reversal with the carrier-envelope phase: A next generation QTAIM interpretation
in Chemical Physics Letters
| Description | James-Watt Studentship |
| Amount | £75,000 (GBP) |
| Organisation | Heriot-Watt University |
| Sector | Academic/University |
| Country | United Kingdom |
| Start | 09/2022 |
| End | 03/2026 |
| Title | GeneralSCI |
| Description | A general selected configuration interaction (GeneralSCI 1.0) program which can construct variational wavefunctions based on various selection protocols. Please note that this is a development version. |
| Type Of Technology | Software |
| Year Produced | 2023 |
| Impact | Too early to identify impacts. |
| URL | https://zenodo.org/doi/10.5281/zenodo.10203394 |