Vibrationally Induced Resonances in Lasing

TL;DR

This paper investigates how vibrational structures influence lasing in nanoscopic, few-molecule plasmonic cavities, revealing resonances dependent on vibrational effects and challenging common approximations.

Contribution

It introduces a first-principles approach to account for vibrational effects in molecular nanolasers, highlighting their impact on lasing resonances and limitations of traditional models.

Findings

Vibrational structure causes resonances in laser intensity.

Resonances depend on Stokes shift, drive strength, and emitter number.

Challenges the validity of the 'incoherent drive' approximation.

Abstract

Optical circuits and light sources, such as lasers, undergo continuous miniaturization. In its extreme, nanolasers might be comprised of only a few molecules confined in plasmonic nanoresonators. Few-emitter lasers promise low energy requirements and fast responses in a footprint that can be inserted into any device or biological tissue. Utilizing the recently developed stacked hierarchy approach, informed from first principles, we demonstrate the impact of vibrational structure on lasing, using the example of few-molecule lasing in plasmonic cavities. Explicitly accounting for the entire vibrational manifold unveils resonances in the laser intensity that depend on the Stokes shift, drive strength, and the number of emitters. Our work identifies the limits of the omnipresent "incoherent drive"-approximation and paves the way for the understanding of nanolasers at the molecular scale.