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Morphology-modified contributions of electronic transitions to the optical response of plasmonic nanoporous gold metamaterial
Umeå University, Faculty of Science and Technology, Department of Physics.ORCID iD: 0000-0002-0839-4556
Umeå University, Faculty of Science and Technology, Department of Physics.
Umeå University, Faculty of Science and Technology, Department of Physics.ORCID iD: 0000-0003-0992-9871
Umeå University, Faculty of Science and Technology, Department of Physics.ORCID iD: 0009-0004-6538-126X
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2026 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 17, no 1, article id 829Article in journal (Refereed) Published
Abstract [en]

Nanoporous metals have emerged as promising functional architectures with tunable optical and electronic properties, high surface areas, and applicability in sensing, catalysis, and biomedicine. While their linear optical behavior and morphological properties have been extensively studied, the electronic properties, and in particular how they are affected by morphology, remain not fully understood. Here we combine experimental and theoretical studies of electronic excitation and relaxation in a nanoporous gold metamaterial. Optical pump–probe experiments show slower electron relaxation dynamics compared to the continuous film, consistent with a higher transient electronic temperature and stronger smearing of the Fermi–Dirac distribution, well reproduced by an extended two-temperature model. Furthermore, cathodoluminescence measurements reveal broadband localized plasmon resonances, and atomistic simulations disentangle intra- and interband effects, demonstrating that nanoscale porosity fundamentally reshapes the electronic response. These findings support nanoporosity as a key design parameter for controlling steady-state and ultrafast optical behavior in plasmonic materials.

Place, publisher, year, edition, pages
Springer Nature, 2026. Vol. 17, no 1, article id 829
National Category
Condensed Matter Physics
Identifiers
URN: urn:nbn:se:umu:diva-249344DOI: 10.1038/s41467-026-68506-0ISI: 001667080400001PubMedID: 41559066Scopus ID: 2-s2.0-105028321894OAI: oai:DiVA.org:umu-249344DiVA, id: diva2:2034663
Funder
Swedish Research Council, 2021-05784Swedish Research Council, 2025-04734Knut and Alice Wallenberg Foundation, 2023.0089EU, European Research Council, 101116253EU, Horizon 2020, 101147248EU, Horizon 2020, 101099125EU, Horizon 2020, 101072818Available from: 2026-02-02 Created: 2026-02-02 Last updated: 2026-02-02Bibliographically approved
In thesis
1. Fast and furious: ultrafast electron dynamics in disordered nanostructures
Open this publication in new window or tab >>Fast and furious: ultrafast electron dynamics in disordered nanostructures
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Alternative title[sv]
Fast and furious : ultrasnabb elektrondynamik i oregelbundna nanostrukturer
Abstract [en]

This thesis investigates ultrafast charge carrier dynamics in disordered nanostructures using femtosecond optical pump probe spectroscopy. The main aim is to understand how photoexcited electronic distributions evolve on femtosecond to picosecond timescales and how nanoscale morphology reshapes the transient optical response and the associated relaxation pathways. Broadband pump probe measurements are combined with optical modelling to relate time dependent changes in transmission to transient modifications of the complex permittivity, electronic damping, and energy transfer to the lattice. 

Ultrafast dynamics are studied in two plasmonic metal systems. For nanoporous gold, the transient transmission response is strongly enhanced and broadened compared with a continuous film. The broadband negative signal extends below the equilibrium interband onset, consistent with higher transient electron temperatures in the porous network that increase Fermi smearing and enable additional 5d to 6sp excitation pathways at lower photon energies. The relaxation is slower than in bulk gold, and modelling with an extended two temperature description combined with an effective medium optical treatment captures both the broadened spectra and the modified recovery, linking the response to morphology-controlled energy deposition and electron to lattice energy flow. 

For disordered copper nano island films, the transient transmission is strongly dispersive in the visible range, with negative and positive contributions that evolve in time due to the interplay of pump induced absorption and bleaching. In both Au and Cu, the measurements show that disorder and nanoscale connectivity reshape the spectral line shape and modify the apparent relaxation dynamics by changing the effective optical response and the effective metal volume involved in energy deposition. 

A complementary case study on polycrystalline NiO thin films extends the investigation to a transition metal oxide under sub band gap excitation, The transient reflectivity shows a prompt negative response followed by recovery that is well described by a biexponential model with a fast component on the order of a few tens of femtoseconds and a slower sub picosecond component. In addition, the thesis documents the generation and characterization of few-cycle structured light pulses carrying orbital angular momentum with controlled polarization states, providing an experimental platform for future ultrafast studies with tailored excitation fields 

Place, publisher, year, edition, pages
Umeå University, 2026. p. 71
Keywords
ultrafast spectroscopy, pump probe, plasmonics, nanoporous gold, copper nano islands, hot carriers, structured light, orbital angular momentum.
National Category
Condensed Matter Physics
Identifiers
urn:nbn:se:umu:diva-249345 (URN)978-91-8070-929-3 (ISBN)978-91-8070-930-9 (ISBN)
Public defence
2026-02-27, NAT.D.410 + Zoom, Umeå University, Umeå, 09:00 (English)
Opponent
Supervisors
Funder
Swedish Research Council, 2021-05784
Note

Link to participate via Zoom: https://umu.zoom.us/j/9817313817

Available from: 2026-02-06 Created: 2026-02-02 Last updated: 2026-02-02Bibliographically approved

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Tapani, TlekHenriksson, NilsBrunner, Carla M.Zimmermann, Ann CélineZäll, ErikHauff, Nils V.Das, Lakshmide Andres, AitorMaccaferri, Nicolò

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Tapani, TlekHenriksson, NilsBrunner, Carla M.Zimmermann, Ann CélineZäll, ErikHauff, Nils V.Das, Lakshmide Andres, AitorGiovannini, TommasoGaroli, DenisMaccaferri, Nicolò
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