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Updated: Sep 20, 2025
08:04
Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
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Frequency-Dependent Sternheimer Linear-Response Formalism for Strongly Coupled Light-Matter Systems
Davis M Welakuh1,2, Johannes Flick3, Michael Ruggenthaler1
1Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science & Department of Physics, Luruper Chaussee 149, Hamburg 22761, Germany.
Journal of Chemical Theory and Computation
|June 8, 2022
Summary
We developed a new quantum electrodynamical density-functional theory (QEDFT) method to efficiently calculate how molecules change when interacting with light. This approach accurately models strong light-matter interactions, revealing spectral shifts like Fano resonances.
Area of Science:
- Quantum Optics and Cavity Quantum Electrodynamics
- Nanoplasmonics and Light-Matter Interactions
- Computational Chemistry and Physics
Background:
- Experimental advances in cavity quantum electrodynamics and nanoplasmonics enable control over matter properties via quantized fields.
- Quantum electrodynamical density-functional theory (QEDFT) provides a first-principles approach for studying strongly coupled light-matter systems.
- Efficient ab initio methods are needed to study large systems interacting with numerous photon modes.
Purpose of the Study:
- To extend the linear-response Sternheimer approach within QEDFT for efficient computation of excited-state properties.
- To investigate the effects of strong light-matter coupling on molecular dispersion and absorption properties.
- To provide an efficient computational method for large molecular systems interacting with quantized electromagnetic fields.
Main Methods:
- Extension of the linear-response Sternheimer approach within the QEDFT framework.
- Computation of excited-state properties for strongly coupled light-matter systems.
- Coupling a molecular system to cavity modes and the continuum of an electromagnetic field.
Main Results:
- Successfully captured features of strong light-matter coupling in molecular dispersion and absorption spectra.
- Observed spectral changes from Lorentzian line shapes to Fano resonances upon strong interaction with the electromagnetic field continuum.
- Demonstrated the efficiency of the Sternheimer approach for modeling light-matter interactions.
Conclusions:
- The extended Sternheimer QEDFT approach efficiently computes excited-state properties of strongly coupled light-matter systems.
- This method accurately models spectral modifications, including the emergence of Fano resonances, due to strong light-matter interactions.
- Presents a viable computational alternative for analyzing large molecular systems interacting with quantized fields.
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