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Related Experiment Video

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Correlative Light- and Electron Microscopy Using Quantum Dot Nanoparticles

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Published on: August 7, 2016

Cavity-Correlated Electron-Nuclear Dynamics from First Principles.

Johannes Flick¹, Prineha Narang¹

¹John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA.

Physical Review Letters

|September 29, 2018

Summary

We developed a new time-dependent density-functional theory to model light-matter interactions. This approach enables accurate predictions of polaritonic chemistry and quantum optics phenomena with atomic precision.

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Area of Science:

Quantum optics
Polaritonic chemistry
Theoretical chemistry

Background:

Strongly correlated light-matter interactions are crucial in polaritonic chemistry and quantum optics.
Existing methods lack atomic-scale resolution for these complex systems.

Purpose of the Study:

To develop a unified theoretical framework for studying electron, nuclear, and photon interactions.
To enable ab initio calculations of correlated light-matter systems.

Main Methods:

Introduced a general time-dependent density-functional theory (TDDFT) for quantized light-matter interactions.
Performed the first ab initio calculation of a correlated electron-nuclear-photon system.

Main Results:

Calculated infrared spectra for CO2 in an optical cavity, showing Rabi splitting.
Observed quantum-electrodynamical observables like the electric displacement field.
Demonstrated cavity-modulated molecular motion.

Conclusions:

The new TDDFT approach provides atomic-scale resolution for light-matter interactions.
This work introduces ab initio methods to the field of collective strong vibrational light-matter interactions.