Ultrastrong coupling is a distinct regime of electromagnetic interaction that enables a rich variety of intriguing physical phenomena. Traditionally, this regime has been reached by coupling intersubband transitions of multiple quantum wells, superconducting artificial atoms, or two-dimensional electron gases to microcavity resonators. However, employing these platforms requires demanding experimental conditions such as cryogenic temperatures, strong magnetic fields, and high vacuum. Here, we use a plasmonic nanorod array positioned at the antinode of a resonant optical Fabry-Pérot microcavity to reach the ultrastrong coupling (USC) regime at ambient conditions and without the use of magnetic fields. From optical measurements we extract the value of the interaction strength over the transition energy as high as g/ω ~ 0.55, deep in the USC regime, while the nanorod array occupies only ∼4% of the cavity volume. Moreover, by comparing the resonant energies of the coupled and uncoupled systems, we indirectly observe up to ∼10% modification of the ground-state energy, which is a hallmark of USC. Our results suggest that plasmon-microcavity polaritons are a promising platform for room-temperature USC realizations in the optical and infrared ranges, and may lead to the long-sought direct visualization of the vacuum energy modification.

We propose a geometry-specific, mode-selective quantization scheme in coupled field-emitter systems which makes it easy to include material and geometrical properties, intrinsic losses as well as the positions of an arbitrary number of quantum emitters. The method is presented through the example of a spherically symmetric, non-magnetic, arbitrarily layered system. We follow it up by a framework to project the system on simpler, effective cavity QED models. Maintaining a well-defined connection to the original quantization, we derive the emerging effective quantities from the full, mode-selective model in a mathematically consistent way. We discuss the uses and limitations of these effective models.

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