Vibrationally Induced Resonances in Lasing
: Müller, Kai; Luoma, Kimmo; Schäfer, Christian
Publisher: American Chemical Society (ACS)
: 2026
Journal of Physical Chemistry Letters
: 1948-7185
DOI: https://doi.org/10.1021/acs.jpclett.5c04028
: https://doi.org/10.1021/acs.jpclett.5c04028
: https://research.utu.fi/converis/portal/detail/Publication/523160501
Optical circuits and light sources, such as lasers, undergo continuous miniaturization. In its extreme, nanolasers might be composed 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 the 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 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.
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The authors thank Walter Strunz and Alexander Eisfeld for insightful discussions. C.S. acknowledges support from the Swedish Research Council through Grant 2016-06059, the FWF Cluster of Excellence MECS, and funding from the Horizon Europe Research and Innovation Program of the European Union under the Marie Skłodowska-Curie Grant Agreement 101065117. The authors gratefully acknowledge the computing time made available to them on the high-performance computer at the NHR Center of TU Dresden. This center is jointly supported by the Federal Ministry of Research, Technology and Space of Germany and the state governments participating in the NHR (www.nhr-verein.de/unsere-partner). The authors acknowledge the TU Wien Bibliothek for financial support through its Open Access Funding Programme.
