1. |
- 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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2. |
- 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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3. |
- Dong, Shuo, et al.
(författare)
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Direct measurement of key exciton properties: Energy, dynamics, and spatial distribution of the wave function
- 2021
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Ingår i: Natural Sciences. - : Wiley. - 2698-6248. ; 1:1
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Tidskriftsartikel (refereegranskat)abstract
- Excitons, Coulomb-bound electron–hole pairs, are the fundamental excitations governing the optoelectronic properties of semiconductors. Although optical signatures of excitons have been studied extensively, experimental access to the excitonic wave function itself has been elusive. Using multidimensional photoemission spectroscopy, we present a momentum-, energy-, and time-resolved perspective on excitons in the layered semiconductor WSe2. By tuning the excitation wavelength, we determine the energy–momentum signature of bright exciton formation and its difference from conventional single-particle excited states. The multidimensional data allow to retrieve fundamental exciton properties like the binding energy and the exciton–lattice coupling and to reconstruct the real-space excitonic distribution function via Fourier transform. All quantities are in excellent agreement with microscopic calculations. Our approach provides a full characterization of the exciton properties and is applicable to bright and dark excitons in semiconducting materials, heterostructures, and devices. Key points: The full life cycle of excitons is recorded with time- and angle-resolved photoemission spectroscopy. The real-space distribution of the excitonic wave function is visualized. Direct measurement of the exciton-phonon interaction.
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4. |
- 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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5. |
- Giorgianni, Flavio, et al.
(författare)
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Melting of magnetic order in NaOsO3 by femtosecond laser pulses
- 2022
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Ingår i: Physical Review B. - : American Physical Society. - 2469-9950 .- 2469-9969. ; 105:15
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Tidskriftsartikel (refereegranskat)abstract
- NaOsO3 has recently attracted significant attention for the strong coupling between its electronic band structure and magnetic ordering. Here, we used time-resolved magnetic x-ray diffraction to determine the timescale of the photoinduced antiferromagnetic dynamics in NaOsO3. Our measurements are consistent with a sub-100 fs melting of the antiferromagnetic long-range order that occurs significantly faster than the lattice dynamics as monitored by the transient change in intensity of selected Bragg structural reflections, which instead show a decrease of intensity on a timescale of several ps.
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6. |
- 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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7. |
- 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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