Cavity-Induced Quantum Interference and Collective Interactions in van der Waals Systems

TL;DR

This paper predicts how optical cavities can modify van der Waals interactions, inducing many-body effects, altering distance scaling, and potentially leading to new structural orders in molecular systems.

Contribution

It introduces a theoretical framework for cavity-induced modifications of vdW interactions, including many-body corrections and altered distance dependencies, revealing new avenues for controlling molecular order.

Findings

Cavity-induced quantum fluctuations generate 3-body and 4-body vdW interactions.

Single-molecule energy shifts and pair interactions scale as R^{-3} instead of R^{-6}.

Enhanced interaction range due to cavity effects may lead to new structural phases.

Abstract

The central topic of this letter is to show that light-matter hybridization not only gives rise to novel dynamic responses but can also modify intermolecular interactions and induce new structural order. Using the van der Waals (vdW) system in an optical cavity as an example, we predict the effects of interference and collectivity in cavity-induced many-body dispersion interactions. Specifically, the leading order correction due to cavity-induced quantum fluctuations leads to 3-body and 4-body vdW interactions, which can align intermolecular vectors and are not pairwise additive. In addition, the cavity-induced dipole leads to a single-molecule energy shift that aligns individual molecules, and a pair-wise interaction that scales as $R^{-3}$ instead of the standard $R^{-6}$ distance scaling. The coefficients of all these cavity-induced corrections depend on the cavity frequency and are renormalized by the effective Rabi frequency, which in turn depends on the particle density. Finally, we study the interaction of the vdW system in a cavity with an external object and find a significant enhancement in the interaction range due to modified distance scaling laws. These theoretical predictions suggest the possibility of cavity-induced nematic or smectic order and may provide an essential clue to understanding intriguing phenomena observed in optical cavities, such as strongly-modified ground-state reactivity, ion transport and solvent polarity.