| 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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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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| 4. |
- Dürr, Hermann A., et al.
(författare)
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Revealing momentum-dependent electron-phonon and phonon-phonon coupling in complex materials with ultrafast electron diffuse scattering
- 2021
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Ingår i: MRS bulletin. - : Springer Nature. - 0883-7694 .- 1938-1425. ; 46:8, s. 731-737
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Tidskriftsartikel (refereegranskat)abstract
- Despite their fundamental role in determining many important properties of materials, detailed momentum-dependent information on the strength of electron–phonon and phonon–phonon coupling across the entire Brillouin zone has remained elusive. Ultrafast electron diffuse scattering (UEDS) is a recently developed technique that is making a significant contribution to these questions. Here, we describe both the UEDS methodology and the information content of ultrafast, photoinduced changes in phonon-diffuse scattering from single-crystal materials. We present results obtained from Ni, WSe2, and TiSe2, materials that are characterized by a complex interplay between electronic (charge, spin) and lattice degrees of freedom. We demonstrate the power of this technique by unraveling carrier–phonon and phonon–phonon interactions in both momentum and time and following nonequilibrium phonon dynamics in detail on ultrafast time scales. By combining ab initio calculations with ultrafast diffuse electron scattering, insights into electronic and magnetic dynamics that impact UEDS indirectly can also be obtained.
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| 5. |
- Miller, R. J. Dwayne, et al.
(författare)
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'Making the molecular movie': first frames
- 2010
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Ingår i: Acta crystallographica. Section A, Foundations of crystallography. - 0108-7673. ; 66, s. 137-156
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Tidskriftsartikel (refereegranskat)abstract
- Recent advances in high-intensity electron and X-ray pulsed sources now make it possible to directly observe atomic motions as they occur in barrier-crossing processes. These rare events require the structural dynamics to be triggered by femtosecond excitation pulses that prepare the system above the barrier or access new potential energy surfaces that drive the structural changes. In general, the sampling process modifies the system such that the structural probes should ideally have sufficient intensity to fully resolve structures near the single-shot limit for a given time point. New developments in both source intensity and temporal characterization of the pulsed sampling mode have made it possible to make so-called 'molecular movies', i.e. measure relative atomic motions faster than collisions can blur information on correlations. Strongly driven phase transitions from thermally propagated melting to optically modified potential energy surfaces leading to ballistic phase transitions and bond stiffening are given as examples of the new insights that can be gained from an atomic level perspective of structural dynamics. The most important impact will likely be made in the fields of chemistry and biology where the central unifying concept of the transition state will come under direct observation and enable a reduction of high-dimensional complex reaction surfaces to the key reactive modes, as long mastered by Mother Nature.
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| 6. |
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| 7. |
- 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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| 8. |
- 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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