| 1. |
- Beaulieu, S., et al.
(författare)
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Revealing Hidden Orbital Pseudospin Texture with Time-Reversal Dichroism in Photoelectron Angular Distributions
- 2020
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Ingår i: Physical Review Letters. - : American Physical Society (APS). - 0031-9007 .- 1079-7114. ; 125:21
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Tidskriftsartikel (refereegranskat)abstract
- We performed angle-resolved photoemission spectroscopy (ARPES) of bulk 2H-WSe2 for different crystal orientations linked to each other by time-reversal symmetry. We introduce a new observable called time-reversal dichroism in photoelectron angular distributions (TRDAD), which quantifies the modulation of the photoemission intensity upon effective time-reversal operation. We demonstrate that the hidden orbital pseudospin texture leaves its imprint on TRDAD, due to multiple orbital interference effects in photoemission. Our experimental results are in quantitative agreement with both the tight-binding model and state-of-the-art fully relativistic calculations performed using the one-step model of photoemission. While spin-resolved ARPES probes the spin component of entangled spin-orbital texture in multiorbital systems, we unambiguously demonstrate that TRDAD reveals its orbital pseudospin texture counterpart.
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| 2. |
- Beaulieu, Samuel, et al.
(författare)
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Ultrafast dynamical Lifshitz transition
- 2021
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Ingår i: Science Advances. - : American Association for the Advancement of Science (AAAS). - 2375-2548. ; 7:17
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Tidskriftsartikel (refereegranskat)abstract
- Fermi surface is at the heart of our understanding of metals and strongly correlated many-body systems. An abrupt change in the Fermi surface topology, also called Lifshitz transition, can lead to the emergence of fascinating phenomena like colossal magnetoresistance and superconductivity. While Lifshitz transitions have been demonstrated for a broad range of materials by equilibrium tuning of macroscopic parameters such as strain, doping, pressure, and temperature, a nonequilibrium dynamical route toward ultrafast modification of the Fermi surface topology has not been experimentally demonstrated. Combining time-resolved multidimensional photoemission spectroscopy with state-of-the-art TDDFT+U simulations, we introduce a scheme for driving an ultrafast Lifshitz transition in the correlated type-II Weyl semimetal T-d-MoTe2. We demonstrate that this nonequilibrium topological electronic transition finds its microscopic origin in the dynamical modification of the effective electronic correlations. These results shed light on a previously unexplored ultrafast scheme for controlling the Fermi surface topology in correlated quantum materials.Y
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| 3. |
- Beldowski, Piotr, et al.
(författare)
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Albumin-Hyaluronan Interactions : Influence of Ionic Composition Probed by Molecular Dynamics
- 2021
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Ingår i: International Journal of Molecular Sciences. - : MDPI AG. - 1661-6596 .- 1422-0067. ; 22:22
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Tidskriftsartikel (refereegranskat)abstract
- The lubrication mechanism in synovial fluid and joints is not yet fully understood. Nevertheless, intermolecular interactions between various neutral and ionic species including large macromolecular systems and simple inorganic ions are the key to understanding the excellent lubrication performance. An important tool for characterizing the intermolecular forces and their structural consequences is molecular dynamics. Albumin is one of the major components in synovial fluid. Its electrostatic properties, including the ability to form molecular complexes, are closely related to pH, solvation, and the presence of ions. In the context of synovial fluid, it is relevant to describe the possible interactions between albumin and hyaluronate, taking into account solution composition effects. In this study, the influence of Na+, Mg2+, and Ca2+ ions on human serum albumin-hyaluronan interactions were examined using molecular dynamics tools. It was established that the presence of divalent cations, and especially Ca2+, contributes mostly to the increase of the affinity between hyaluronan and albumin, which is associated with charge compensation in negatively charged hyaluronan and albumin. Furthermore, the most probable binding sites were structurally and energetically characterized. The indicated moieties exhibit a locally positive charge which enables hyaluronate binding (direct and water mediated).
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| 4. |
- Dendzik, Maciej, et al.
(författare)
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Observation of an Excitonic Mott Transition Through Ultrafast Core-cum-Conduction Photoemission Spectroscopy
- 2020
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Ingår i: Physical Review Letters. - : American Physical Society (APS). - 0031-9007 .- 1079-7114. ; 125:9
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Tidskriftsartikel (refereegranskat)abstract
- Time-resolved soft-x-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe2. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels clearly show a delayed core-hole renormalization due to screening by excited quasifree carriers resulting from an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectroscopy as a sensitive probe of subtle electronic many-body interactions and ultrafast electronic phase transitions.
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| 5. |
- Dong, Shuo, et al.
(författare)
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Observation of ultrafast interfacial Meitner-Auger energy transfer in a Van der Waals heterostructure
- 2023
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 14:1
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Tidskriftsartikel (refereegranskat)abstract
- Atomically thin layered van der Waals heterostructures feature exotic and emergent optoelectronic properties. With growing interest in these novel quantum materials, the microscopic understanding of fundamental interfacial coupling mechanisms is of capital importance. Here, using multidimensional photoemission spectroscopy, we provide a layer- and momentum-resolved view on ultrafast interlayer electron and energy transfer in a monolayer-WSe2/graphene heterostructure. Depending on the nature of the optically prepared state, we find the different dominating transfer mechanisms: while electron injection from graphene to WSe2 is observed after photoexcitation of quasi-free hot carriers in the graphene layer, we establish an interfacial Meitner-Auger energy transfer process following the excitation of excitons in WSe2. By analysing the time-energy-momentum distributions of excited-state carriers with a rate-equation model, we distinguish these two types of interfacial dynamics and identify the ultrafast conversion of excitons in WSe2 to valence band transitions in graphene. Microscopic calculations find interfacial dipole-monopole coupling underlying the Meitner-Auger energy transfer to dominate over conventional Förster- and Dexter-type interactions, in agreement with the experimental observations. The energy transfer mechanism revealed here might enable new hot-carrier-based device concepts with van der Waals heterostructures.
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| 6. |
- Grubisic-Cabo, Antonija, et al.
(författare)
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In Situ Exfoliation Method of Large-Area 2D Materials
- 2023
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Ingår i: Advanced Science. - : Wiley. - 2198-3844. ; 10:22
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Tidskriftsartikel (refereegranskat)abstract
- 2D materials provide a rich platform to study novel physical phenomena arising from quantum confinement of charge carriers. Many of these phenomena are discovered by surface sensitive techniques, such as photoemission spectroscopy, that work in ultra-high vacuum (UHV). Success in experimental studies of 2D materials, however, inherently relies on producing adsorbate-free, large-area, high-quality samples. The method that yields 2D materials of highest quality is mechanical exfoliation from bulk-grown samples. However, as this technique is traditionally performed in a dedicated environment, the transfer of samples into vacuum requires surface cleaning that might diminish the quality of the samples. In this article, a simple method for in situ exfoliation directly in UHV is reported, which yields large-area, single-layered films. Multiple metallic and semiconducting transition metal dichalcogenides are exfoliated in situ onto Au, Ag, and Ge. The exfoliated flakes are found to be of sub-millimeter size with excellent crystallinity and purity, as supported by angle-resolved photoemission spectroscopy, atomic force microscopy, and low-energy electron diffraction. The approach is well-suited for air-sensitive 2D materials, enabling the study of a new suite of electronic properties. In addition, the exfoliation of surface alloys and the possibility of controlling the substrate-2D material twist angle is demonstrated.
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| 7. |
- Guo, Qinda, et al.
(författare)
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A narrow bandwidth extreme ultra-violet light source for time- and angle-resolved photoemission spectroscopy
- 2022
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Ingår i: Structural Dynamics. - : AIP Publishing. - 2329-7778. ; 9:2
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Tidskriftsartikel (refereegranskat)abstract
- Here, we present a high repetition rate, narrow bandwidth, extreme ultraviolet photon source for time- and angle-resolved photoemission spectroscopy. The narrow bandwidth pulses Δ E = 9, 14, and 18 meV for photon energies h ν = 10.8, 18.1, and 25.3 eV are generated through high harmonic generation using ultra-violet drive pulses with relatively long pulse lengths (461 fs). The high harmonic generation setup employs an annular drive beam in tight focusing geometry at a repetition rate of 250 kHz. Photon energy selection is provided by a series of selectable multilayer bandpass mirrors and thin film filters, thus avoiding any time broadening introduced by single grating monochromators. A two stage optical-parametric amplifier provides < 100 fs tunable pump pulses from 0.65 μm to 9 μm. The narrow bandwidth performance of the light source is demonstrated through angle-resolved photoemission measurements on a series of quantum materials, including high-temperature superconductor Bi-2212, WSe2, and graphene.
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| 8. |
- Jørgensen, Jakob Holm, et al.
(författare)
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Symmetry-Driven Band Gap Engineering in Hydrogen Functionalized Graphene
- 2016
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 10:12, s. 10798-10807
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Tidskriftsartikel (refereegranskat)abstract
- Band gap engineering in hydrogen functionalized graphene is demonstrated by changing the symmetry of the functionalization structures. Small differences in hydrogen adsorbate binding energies on graphene on Ir(111) allow tailoring of highly periodic functionalization structures favoring one distinct region of the moiré supercell. Scanning tunneling microscopy and X-ray photoelectron spectroscopy measurements show that a highly periodic hydrogen functionalized graphene sheet can thus be prepared by controlling the sample temperature (Ts) during hydrogen functionalization. At deposition temperatures of Ts = 645 K and above, hydrogen adsorbs exclusively on the HCP regions of the graphene/Ir(111) moiré structure. This finding is rationalized in terms of a slight preference for hydrogen clusters in the HCP regions over the FCC regions, as found by density functional theory calculations. Angle-resolved photoemission spectroscopy measurements demonstrate that the preferential functionalization of just one region of the moiré supercell results in a band gap opening with very limited associated band broadening. Thus, hydrogenation at elevated sample temperatures provides a pathway to efficient band gap engineering in graphene via the selective functionalization of specific regions of the moiré structure.
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| 9. |
- Li, Cong, et al.
(författare)
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Coexistence of two intertwined charge density waves in a kagome system
- 2022
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Ingår i: Physical Review Research. - : American Physical Society (APS). - 2643-1564. ; 4:3
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Tidskriftsartikel (refereegranskat)abstract
- Materials with a kagome lattice structure display a wealth of intriguing magnetic properties due to their geometric frustration and intrinsically flat band structure. Recently, topological and superconducting states have also been observed in kagome systems. The kagome lattice may also host a "breathing" mode that leads to charge density wave (CDW) states, if there is strong electron-phonon coupling, electron-electron interaction, or external excitation of the material. This "breathing" mode can give rise to candidate distortions such as the star of David (SoD) or its inverse structure [trihexagonal (TrH)]. To date, in most materials, only a single type of distortion has been observed. Here, we present angle-resolved photoemission spectroscopy measurements on the kagome superconductor CsV3Sb5 at multiple temperatures and photon energies to reveal the nature of the CDW in this material. It is shown that CsV3Sb5 displays two intertwined CDW orders corresponding to the SoD and TrH distortions. These two distinct types of distortions are stacked along the c direction to form a three-dimensional CDW order where the two 2-fold CDWs are phase shifted along the c axis. The presented results provide not only key insights into the nature of the unconventional CDW order in CsV3Sb5, but also an important reference for further studies on the relationship between the CDW and superconducting order.
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| 10. |
- Li, Cong, et al.
(författare)
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Emergence of Weyl fermions by ferrimagnetism in a noncentrosymmetric magnetic Weyl semimetal
- 2023
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 14:1
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Tidskriftsartikel (refereegranskat)abstract
- Condensed matter physics has often provided a platform for investigating the interplay between particles and fields in cases that have not been observed in high-energy physics. Here, using angle-resolved photoemission spectroscopy, we provide an example of this by visualizing the electronic structure of a noncentrosymmetric magnetic Weyl semimetal candidate NdAlSi in both the paramagnetic and ferrimagnetic states. We observe surface Fermi arcs and bulk Weyl fermion dispersion as well as the emergence of new Weyl fermions in the ferrimagnetic state. Our results establish NdAlSi as a magnetic Weyl semimetal and provide an experimental observation of ferrimagnetic regulation of Weyl fermions in condensed matter.
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| 11. |
- Majchrzak, Paulina, et al.
(författare)
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Spectroscopic view of ultrafast charge carrier dynamics in single- and bilayer transition metal dichalcogenide semiconductors
- 2021
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Ingår i: Journal of Electron Spectroscopy and Related Phenomena. - : Elsevier BV. - 0368-2048 .- 1873-2526. ; 250
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Tidskriftsartikel (refereegranskat)abstract
- The quasiparticle spectra of atomically thin semiconducting transition metal dichalcogenides (TMDCs) and their response to an ultrafast optical excitation critically depend on interactions with the underlying substrate. Here, we present a comparative time- and angle-resolved photoemission spectroscopy (TR-ARPES) study of the transient electronic structure and ultrafast carrier dynamics in the single- and bilayer TMDCs MoS2 and WS2 on three different substrates: Au(111), Ag(111) and graphene/SiC. The photoexcited quasiparticle bandgaps are observed to vary over the range of 1.9-2.5 eV between our systems. The transient conduction band signals decay on a sub-50 fs timescale on the metals, signifying an efficient removal of photoinduced carriers into the bulk metallic states. On graphene, we instead observe a fast timescale on the order of 170 fs, followed by a slow dynamics for the conduction band decay in MoS2. These timescales are explained by Auger recombination involving MoS2 and in-gap defect states. In bilayer TMDCs on metals we observe a complex redistribution of excited holes along the valence band that is substantially affected by interactions with the continuum of bulk metallic states.
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| 12. |
- Maklar, J., et al.
(författare)
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A quantitative comparison of time-of-flight momentum microscopes and hemispherical analyzers for time- and angle-resolved photoemission spectroscopy experiments
- 2020
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 91:12
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Tidskriftsartikel (refereegranskat)abstract
- Time-of-flight-based momentum microscopy has a growing presence in photoemission studies, as it enables parallel energy- and momentum-resolved acquisition of the full photoelectron distribution. Here, we report table-top extreme ultraviolet time- and angle-resolved photoemission spectroscopy (trARPES) featuring both a hemispherical analyzer and a momentum microscope within the same setup. We present a systematic comparison of the two detection schemes and quantify experimentally relevant parameters, including pump- and probe-induced space-charge effects, detection efficiency, photoelectron count rates, and depth of focus. We highlight the advantages and limitations of both instruments based on exemplary trARPES measurements of bulk WSe2. Our analysis demonstrates the complementary nature of the two spectrometers for time-resolved ARPES experiments. Their combination in a single experimental apparatus allows us to address a broad range of scientific questions with trARPES.
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| 13. |
- Pincelli, Tommaso, et al.
(författare)
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Observation of Multi-Directional Energy Transfer in a Hybrid Plasmonic–Excitonic Nanostructure
- 2023
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Ingår i: Advanced Materials. - : Wiley. - 0935-9648 .- 1521-4095. ; 35:9
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Tidskriftsartikel (refereegranskat)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.
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| 14. |
- Wang, Yang, et al.
(författare)
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Recent progress in angle-resolved photoemission spectroscopy
- 2024
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Ingår i: Measurement science and technology. - : IOP Publishing. - 0957-0233 .- 1361-6501. ; 35:4
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Forskningsöversikt (refereegranskat)abstract
- Angle-resolved photoemission spectroscopy (ARPES) is a well-established experimental technique that allows probing of the electronic structure of quantum materials using relatively high-energy photons. ARPES has been extensively used to study important classes of materials such as topological insulators, high-temperature superconductors, two-dimensional materials or interface systems. Although the technique was originally developed over 60 years ago, the last decade has witnessed significant advancements in instrumentation. In this review, we survey recent progress in ARPES, with a focus on developments in novel light sources and electron detection methods, which enable the expansion of ARPES into spin-, time-, or space-resolved domains. Important examples of ARPES results are presented, together with an outlook for the field.
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| 15. |
- Xian, R. Patrick, et al.
(författare)
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A machine learning route between band mapping and band structure
- 2023
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Ingår i: Nature Computational Science. - : Springer Nature. - 2662-8457. ; 3:1, s. 101-114
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Tidskriftsartikel (refereegranskat)abstract
- The electronic band structure and crystal structure are the two complementary identifiers of solid-state materials. Although convenient instruments and reconstruction algorithms have made large, empirical, crystal structure databases possible, extracting the quasiparticle dispersion (closely related to band structure) from photoemission band mapping data is currently limited by the available computational methods. To cope with the growing size and scale of photoemission data, here we develop a pipeline including probabilistic machine learning and the associated data processing, optimization and evaluation methods for band-structure reconstruction, leveraging theoretical calculations. The pipeline reconstructs all 14 valence bands of a semiconductor and shows excellent performance on benchmarks and other materials datasets. The reconstruction uncovers previously inaccessible momentum-space structural information on both global and local scales, while realizing a path towards integration with materials science databases. Our approach illustrates the potential of combining machine learning and domain knowledge for scalable feature extraction in multidimensional data.
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