Near-Field Vibrational Energy Transfer for Mid-Infrared Upconversion in Plasmonic Nanogaps
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| Format: | Preprint |
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2026
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| _version_ | 1866909056153681920 |
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| author | Pal, Avisekh Sajan, Anju Sumner, Christopher Alharbi, Eman Theis, Wolfgang Chikkaraddy, Rohit |
| author_facet | Pal, Avisekh Sajan, Anju Sumner, Christopher Alharbi, Eman Theis, Wolfgang Chikkaraddy, Rohit |
| contents | Förster energy transfer underpins modern photonics, yet establishing an analogous vibrational pathway in the mid-infrared (MIR) remains highly challenging, as sub-picosecond intramolecular vibrational redistribution (IVR) suppresses intermolecular coupling. Here we demonstrate vibrational donor--acceptor transfer in the MIR and subsequent upconversion to visible luminescence enabled by sub-2 nm plasmonic nanogaps. The extreme lateral field confinement in metal--molecule--metal ring cavities defined by self-assembled molecular spacers couples efficiently to in-plane molecular dipoles. Continuous-wave MIR excitation selectively populates $-\mathrm{C}\equiv\mathrm{N}$ vibrational donors, and plasmon-enhanced near-field coupling transfers this energy to nearby electronic acceptors, generating anti-Stokes visible emission under low power densities. Upconversion efficiencies exceeding $0.3\%$ are observed, limited by competition between the plasmon-mediated transfer rate and IVR. These results show that extreme plasmonic confinement can redirect molecular vibrational relaxation pathways, opening a route toward vibrational nanophotonics, intermolecular interactions for bioimaging, and room-temperature MIR detection based on molecular degrees of freedom. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2605_19498 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Near-Field Vibrational Energy Transfer for Mid-Infrared Upconversion in Plasmonic Nanogaps Pal, Avisekh Sajan, Anju Sumner, Christopher Alharbi, Eman Theis, Wolfgang Chikkaraddy, Rohit Optics Mesoscale and Nanoscale Physics Applied Physics Förster energy transfer underpins modern photonics, yet establishing an analogous vibrational pathway in the mid-infrared (MIR) remains highly challenging, as sub-picosecond intramolecular vibrational redistribution (IVR) suppresses intermolecular coupling. Here we demonstrate vibrational donor--acceptor transfer in the MIR and subsequent upconversion to visible luminescence enabled by sub-2 nm plasmonic nanogaps. The extreme lateral field confinement in metal--molecule--metal ring cavities defined by self-assembled molecular spacers couples efficiently to in-plane molecular dipoles. Continuous-wave MIR excitation selectively populates $-\mathrm{C}\equiv\mathrm{N}$ vibrational donors, and plasmon-enhanced near-field coupling transfers this energy to nearby electronic acceptors, generating anti-Stokes visible emission under low power densities. Upconversion efficiencies exceeding $0.3\%$ are observed, limited by competition between the plasmon-mediated transfer rate and IVR. These results show that extreme plasmonic confinement can redirect molecular vibrational relaxation pathways, opening a route toward vibrational nanophotonics, intermolecular interactions for bioimaging, and room-temperature MIR detection based on molecular degrees of freedom. |
| title | Near-Field Vibrational Energy Transfer for Mid-Infrared Upconversion in Plasmonic Nanogaps |
| topic | Optics Mesoscale and Nanoscale Physics Applied Physics |
| url | https://arxiv.org/abs/2605.19498 |