Light-responsive organic polaritons from first principles

Area of Science:

• Photonics
• Organic Chemistry
• Quantum Optics

Background:

• Controlling optical properties of organic molecules is crucial for photonics.
• Light-responsive organic molecules, such as trans-azobenzene and tetraphenyl porphyrin (H2TPP), are key components.

Purpose of the Study:

• To demonstrate the use of light-responsive organic polaritons within an optical cavity to modify molecular optical properties.
• To investigate the effects of weak to strong light-matter coupling on molecular behavior.

Main Methods:

• First-principles calculations were employed to study molecular behavior.
• Optical cavity effects on trans-azobenzene and H2TPP were simulated under varying coupling strengths.

Main Results:

• Optical cavities were shown to modulate the dispersion and absorption properties of organic molecules.
• Anomalous dispersion in trans-azobenzene was suppressed by the cavity, with suppression decreasing as coupling strength increased.
• Switching between Lorentz and Fano line shapes for H2TPP polaritons was achieved by tuning light-matter coupling.
• The Purcell effect was utilized to control spontaneous radiation of organic molecules.

Conclusions:

• Optical cavities provide a method to manipulate the optical dipole trap of organic molecules.
• Strong light-matter coupling offers significant control over molecular spectral features and radiation.
• This research presents a novel approach for controlling optical properties of light-responsive organic molecules for photonic applications.