Observation of Multi-Directional Energy Transfer in a Hybrid 
Plasmonic–Excitonic Nanostructure

Pincelli, Tommaso; Vasileiadis, Thomas; Dong, Shuo; Beaulieu, Samuel; Dendzik, Maciej Ramon; Zahn, Daniela; Lee, Sang-Eun; Seiler, Helene; Qi, Yingpeng; Xian, R. Patrick; Maklar, Julian; Coy, Emerson; Mueller, Niclas S.; Okamura, Yu; Reich, Stephanie; Wolf, Martin; Rettig, Laurenz; Ernstorfer, Ralph

doi:10.1002/adma.202209100

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Observation of Multi-Directional Energy Transfer in a Hybrid Plasmonic–Excitonic Nanostructure

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Pincelli, Tommaso
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons138038

Vasileiadis, Thomas
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons206871

Dong, Shuo
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons227651

Beaulieu, Samuel
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons205838

Dendzik, Maciej Ramon
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons195530

Zahn, Daniela
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons213525

Lee, Sang-Eun
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons222712

Seiler, Helene
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons245740

Qi, Yingpeng
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons136124

Xian, R. Patrick
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons232536

Maklar, Julian
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22250

Wolf, Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons104701

Rettig, Laurenz
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21497

Ernstorfer, Ralph
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Pincelli, T., Vasileiadis, T., Dong, S., Beaulieu, S., Dendzik, M. R., Zahn, D., et al. (2023). Observation of Multi-Directional Energy Transfer in a Hybrid Plasmonic–Excitonic Nanostructure. Advanced Materials, 35(9): 2209100. doi:10.1002/adma.202209100.

Cite as: https://hdl.handle.net/21.11116/0000-000C-44D0-C

Abstract

Hybrid plasmonic devices involve a nanostructured metal supporting localized surface plasmons to amplify light–matter interaction, and a non-plasmonic material to functionalize charge excitations. Application-relevant epitaxial heterostructures, however, give rise to ballistic ultrafast dynamics that challenge the conventional semiclassical understanding of unidirectional nanometal-to-substrate energy transfer. Epitaxial Au nanoislands are studied on WSe₂ with time- and angle-resolved photoemission spectroscopy and femtosecond electron diffraction: this combination of techniques resolves material, energy, and momentum of charge-carriers and phonons excited in the heterostructure. A strong non-linear plasmon–exciton interaction that transfers the energy of sub-bandgap photons very efficiently to the semiconductor is observed, leaving the metal cold until non-radiative exciton recombination heats the nanoparticles on hundreds of femtoseconds timescales. The results resolve a multi-directional energy exchange on timescales shorter than the electronic thermalization of the nanometal. Electron–phonon coupling and diffusive charge-transfer determine the subsequent energy flow. This complex dynamics opens perspectives for optoelectronic and photocatalytic applications, while providing a constraining experimental testbed for state-of-the-art modelling.