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Fast and furious: ultrafast electron dynamics in disordered nanostructures
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Institutionen för fysik. (Ultrafast Nanoscience)ORCID-id: 0000-0002-0839-4556
2026 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)Alternativ titel
Fast and furious : ultrasnabb elektrondynamik i oregelbundna nanostrukturer (Svenska)
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 

Ort, förlag, år, upplaga, sidor
Umeå University, 2026. , s. 71
Nyckelord [en]
ultrafast spectroscopy, pump probe, plasmonics, nanoporous gold, copper nano islands, hot carriers, structured light, orbital angular momentum.
Nationell ämneskategori
Den kondenserade materiens fysik
Identifikatorer
URN: urn:nbn:se:umu:diva-249345ISBN: 978-91-8070-929-3 (tryckt)ISBN: 978-91-8070-930-9 (digital)OAI: oai:DiVA.org:umu-249345DiVA, id: diva2:2034697
Disputation
2026-02-27, NAT.D.410 + Zoom, Umeå University, Umeå, 09:00 (Engelska)
Opponent
Handledare
Forskningsfinansiär
Vetenskapsrådet, 2021-05784
Anmärkning

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

Tillgänglig från: 2026-02-06 Skapad: 2026-02-02 Senast uppdaterad: 2026-02-02Bibliografiskt granskad
Delarbeten
1. Morphology-modified contributions of electronic transitions to the optical response of plasmonic nanoporous gold metamaterial
Öppna denna publikation i ny flik eller fönster >>Morphology-modified contributions of electronic transitions to the optical response of plasmonic nanoporous gold metamaterial
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2026 (Engelska)Ingår i: Nature Communications, E-ISSN 2041-1723, Vol. 17, nr 1, artikel-id 829Artikel i tidskrift (Refereegranskat) 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.

Ort, förlag, år, upplaga, sidor
Springer Nature, 2026
Nationell ämneskategori
Den kondenserade materiens fysik
Identifikatorer
urn:nbn:se:umu:diva-249344 (URN)10.1038/s41467-026-68506-0 (DOI)001667080400001 ()41559066 (PubMedID)2-s2.0-105028321894 (Scopus ID)
Forskningsfinansiär
Vetenskapsrådet, 2021-05784Vetenskapsrådet, 2025-04734Knut och Alice Wallenbergs Stiftelse, 2023.0089EU, Europeiska forskningsrådet, 101116253EU, Horisont 2020, 101147248EU, Horisont 2020, 101099125EU, Horisont 2020, 101072818
Tillgänglig från: 2026-02-02 Skapad: 2026-02-02 Senast uppdaterad: 2026-02-02Bibliografiskt granskad
2. Disordered plasmonic system with dense copper nano-island morphology
Öppna denna publikation i ny flik eller fönster >>Disordered plasmonic system with dense copper nano-island morphology
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2025 (Engelska)Ingår i: Nanophotonics, ISSN 2192-8606, E-ISSN 2192-8614, Vol. 14, nr 12, s. 2151-5160Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Dry synthesis is a highly versatile method for the fabrication of nanoporous metal films, since it enables easy and reproducible deposition of single or multi-layers of nanostructured materials that can find intriguing applications in plasmonics, photochemistry and photocatalysis, to name a few. Here, we extend the use of this methodology to the preparation of copper nano-islands that represent an affordable and versatile example of disordered plasmonic substrates. Although the island morphology is disordered, the high density of these nanostructures with large surface area results in a good homogeneity on a macroscale, which is beneficial for plasmonic applications such as bio-sensing and photo-catalysis. With cathodoluminescence and electron-energy-loss spectroscopies we confirm the nano-islands as sources of the local field enhancement and identify the plasmonic resonance bands in the visible and near-infrared spectral range. The decay dynamics of the plasmonic signal are slower in the nano-island as compared to bulk copper films, which can be rationalized by a reduced energy dissipation in the nano-island films. Our study demonstrates a robust and lithography-free fabrication pathway to obtain nanostructured plasmonic copper substrates that represent a highly versatile low-cost alternative for future applications ranging from sensing to photochemistry and photocatalysis.

Nyckelord
EELS, cathodoluminescence, SHG, pump-probe, nano islands, nanoporous
Nationell ämneskategori
Den kondenserade materiens fysik
Identifikatorer
urn:nbn:se:umu:diva-238190 (URN)10.1515/nanoph-2024-0743 (DOI)2-s2.0-105003834365 (Scopus ID)
Forskningsfinansiär
EU, Horisont 2020
Tillgänglig från: 2025-04-25 Skapad: 2025-04-25 Senast uppdaterad: 2026-02-02Bibliografiskt granskad
3. NiO thin films fabricated using spray-pyrolysis technique: structural and optical characterization and ultrafast charge dynamics studies
Öppna denna publikation i ny flik eller fönster >>NiO thin films fabricated using spray-pyrolysis technique: structural and optical characterization and ultrafast charge dynamics studies
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2024 (Engelska)Ingår i: Journal of Physics D: Applied Physics, ISSN 0022-3727, E-ISSN 1361-6463, Vol. 57, nr 38, artikel-id 385303Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Nickel (II) oxide, NiO, is a wide band gap Mott insulator characterized by strong Coulomb repulsion between d-electrons and displays antiferromagnetic order at room temperature. NiO has gained attention in recent years as a very promising candidate for applications in a broad set of areas, including chemistry and metallurgy to spintronics and energy harvesting. Here, we report on the fabrication of polycrystalline NiO using spray-pyrolysis technique, which is a deposition technique able to produce quite uniform films of pure and crystalline materials without the need of high vacuum or inert atmospheres. The composition and structure of the NiO thin films were then studied using x-ray diffraction, and atomic force and scanning electron microscopies (SEM). The phononic and magnonic properties of the NiO thin films were also studied via Raman spectroscopy, and the ultrafast electron dynamics by using optical pump probe spectroscopy. We found that the NiO samples display the same phonon and magnon excitations expected for single crystal NiO at room temperature, and that electron dynamics in our system is like those of previously reported NiO mono- and polycrystalline systems synthesized using different techniques. These results prove that spray-pyrolysis can be used as affordable and large-scale fabrication technique to synthesize strongly correlated materials for a large set of applications.

Ort, förlag, år, upplaga, sidor
Institute of Physics Publishing (IOPP), 2024
Nyckelord
materials structure characterization, nickel oxide, polycrystalline thin film, spray-pyrolysis, ultrafast spectroscopy
Nationell ämneskategori
Den kondenserade materiens fysik
Identifikatorer
urn:nbn:se:umu:diva-227871 (URN)10.1088/1361-6463/ad584a (DOI)001260085400001 ()2-s2.0-85197633731 (Scopus ID)
Forskningsfinansiär
Wenner-Gren Stiftelserna, UPD2022-0074Vetenskapsrådet, 2021-05784Stiftelsen för strategisk forskning (SSF), 2030-PUSHKempestiftelserna, JCK-2132Carl Tryggers stiftelse för vetenskaplig forskning , CTS 21-1581
Tillgänglig från: 2024-07-15 Skapad: 2024-07-15 Senast uppdaterad: 2026-02-02Bibliografiskt granskad
4. Vortex plate retarder-based approach for the generation of sub-20 fs light pulses carrying orbital angular momentum
Öppna denna publikation i ny flik eller fönster >>Vortex plate retarder-based approach for the generation of sub-20 fs light pulses carrying orbital angular momentum
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2024 (Engelska)Ingår i: Journal of Optics, ISSN 2040-8978, E-ISSN 2040-8986, Vol. 26, nr 4, artikel-id 045502Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

We use a vortex retarder-based approach to generate few optical cycles light pulses carrying orbital angular momentum (OAM) (known also as twisted light or optical vortex) from a Yb:KGW oscillator pumping a noncollinear optical parametric amplifier generating sub-10 fs linearly polarized light pulses in the near infrared spectral range (central wavelength 850 nm). We characterize such vortices both spatially and temporally by using astigmatic imaging technique and second harmonic generation-based frequency resolved optical gating, respectively. The generation of optical vortices is analyzed, and its structure reconstructed by estimating the spatio-spectral field and Fourier transforming it into the temporal domain. As a proof of concept, we show that we can also generate sub-20 fs light pulses carrying OAM and with arbitrary polarization on the first-order Poincaré sphere.

Ort, förlag, år, upplaga, sidor
Institute of Physics (IOP), 2024
Nyckelord
optical vortex, orbital angular momentum, twisted light, ultrashort light pulses, vortex plate retarder
Nationell ämneskategori
Atom- och molekylfysik och optik
Identifikatorer
urn:nbn:se:umu:diva-222577 (URN)10.1088/2040-8986/ad2e1f (DOI)001183679100001 ()2-s2.0-85187554162 (Scopus ID)
Forskningsfinansiär
Vetenskapsrådet, 2021-05784Kempestiftelserna, JCK-3122EU, Horisont 2020, 801505
Tillgänglig från: 2024-04-08 Skapad: 2024-04-08 Senast uppdaterad: 2026-02-02Bibliografiskt granskad

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