Shortcut to Self-Consistent Light-Matter Interaction and Realistic Spectra from First Principles

Area of Science:

• Quantum Chemistry
• Theoretical Physics
• Computational Electromagnetism

Background:

• Accurately modeling light-matter interactions is crucial for understanding quantum phenomena.
• Existing methods for embedding electromagnetic environments can be computationally expensive.
• There is a need for efficient and accessible approaches to simulate these interactions.

Purpose of the Study:

• To introduce a simple and efficient method for embedding electromagnetic environments into electronic structure calculations.
• To demonstrate the capability of this method to capture various light-matter interaction phenomena.
• To showcase the seamless integration of this approach into existing computational frameworks.

Main Methods:

• The study introduces radiation-reaction forces as a means to represent the electromagnetic environment.
• This approach is integrated into state-of-the-art electronic structure methods.
• The method is demonstrated using time-dependent density-functional theory (TDDFT).

Main Results:

• The method self-consistently provides access to radiative emission and natural linewidth.
• It accurately captures phenomena such as Lamb shifts and strong coupling.
• Electromagnetically induced transparency, Purcell-enhanced, and superradiant emission are also demonstrated.

Conclusions:

• The proposed method offers an efficient way to include electromagnetic environments in electronic structure calculations.
• Its seamless integration into TDDFT incurs virtually no additional computational cost.
• This work presents a convenient shortcut for studying complex light-matter interactions.