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Cavity-free plasmonic nanolasing enabled by dispersionless stopped light.

ABSTRACT: When light is brought to a standstill, its interaction with gain media increases dramatically due to a singularity in the density of optical states. Concurrently, stopped light engenders an inherent and cavity-free feedback mechanism, similar in effect to the feedback that has been demonstrated and exploited in large-scale disordered media and random lasers. Here we study the spatial, temporal and spectral signatures of lasing in planar gain-enhanced nanoplasmonic structures at near-infrared frequencies and show that the stopped-light feedback mechanism allows for nanolasing without a cavity. We reveal that in the absence of cavity-induced feedback, the subwavelength lasing mode forms dynamically as a phase-locked superposition of quasi dispersion-free waveguide modes. This mechanism proves remarkably robust against interface roughness and offers a new route towards nanolasing, the experimental realization of ultra-thin surface emitting lasers, and cavity-free active quantum plasmonics.

SUBMITTER: Pickering T

PROVIDER: S-EPMC4199200 | biostudies-literature | 2014 Sep

REPOSITORIES: biostudies-literature

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Cavity-free plasmonic nanolasing enabled by dispersionless stopped light.

Pickering Tim T Hamm Joachim M JM Page A Freddie AF Wuestner Sebastian S Hess Ortwin O

Nature communications 20140917

When light is brought to a standstill, its interaction with gain media increases dramatically due to a singularity in the density of optical states. Concurrently, stopped light engenders an inherent and cavity-free feedback mechanism, similar in effect to the feedback that has been demonstrated and exploited in large-scale disordered media and random lasers. Here we study the spatial, temporal and spectral signatures of lasing in planar gain-enhanced nanoplasmonic structures at near-infrared fre ...[more]

PMID: 25230337

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Project description:Harnessing visible light as the driving force for chemical transformations generally offers a more environmentally friendly alternative compared with classical synthetic methodology. The transition metal-based photocatalysts commonly employed in photoredox catalysis absorb efficiently in the visible spectrum, unlike most organic substrates, allowing for orthogonal excitation. The subsequent excited states are both more reducing and more oxidizing than the ground state catalyst and are competitive with some of the more powerful single-electron oxidants or reductants available to organic chemists yet are simply accessed via irradiation. The benefits of this strategy have proven particularly useful in radical chemistry, a field that traditionally employs rather toxic and hazardous reagents to generate the desired intermediates. In this Account, we discuss our efforts to leverage visible light photoredox catalysis in radical-based bond-forming and bond-cleaving events for which few, if any, environmentally benign alternatives exist. Mechanistic investigations have driven our contributions in this field, for both facilitating desired transformations and offering new, unexpected opportunities. In fact, our total synthesis of (+)-gliocladin C was only possible upon elucidating the propensity for various trialkylamine additives to elicit a dual behavior as both a reductive quencher and a H-atom donor. Importantly, while natural product synthesis was central to our initial motivations to explore these photochemical processes, we have since demonstrated applicability within other subfields of chemistry, and our evaluation of flow technologies demonstrates the potential to translate these results from the bench to pilot scale. Our forays into photoredox catalysis began with fundamental methodology, providing a tin-free reductive dehalogenation that exchanged the gamut of hazardous reagents previously employed for such a transformation for visible light-mediated, ambient temperature conditions. Evolving from this work, a new avenue toward atom transfer radical addition (ATRA) chemistry was developed, enabling dual functionalization of both double and triple bonds. Importantly, we have also expanded our portfolio to target clinically relevant scaffolds. Photoredox catalysis proved effective in generating high value fluorinated alkyl radicals through the use of abundantly available starting materials, providing access to libraries of trifluoromethylated (hetero)arenes as well as intriguing gem-difluoro benzyl motifs via a novel photochemical radical Smiles rearrangement. Finally, we discuss a photochemical strategy toward sustainable lignin processing through selective C-O bond cleavage methodology. The collection of these efforts is meant to highlight the potential for visible light-mediated radical chemistry to impact a variety of industrial sectors.

Dataset Information

Cavity-free plasmonic nanolasing enabled by dispersionless stopped light.

Publications

Cavity-free plasmonic nanolasing enabled by dispersionless stopped light.

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