B07 - Momentum-resolved dynamics of relaxation processes and control of spins and pseudospins in two-dimensional spintronic heterostructures
A range of semiconducting transition metal dichalcogenides (TMDCs) exhibits a unique electronic structure governed by spin-polarized electronic states localized both in momentum and real space. These materials open new perspectives in view of spintronic applications, for instance as source of spin currents in heterostructures. For example, spin- and valley-selective excitation localized in a TMDC layer can be induced by circular polarized light leading to ultrafast scattering processes in momentum space followed by charge and spin transfer to adjacent layers via electronic states which are delocalized across a heterostructure interface. This project employs femtosecond time-, energy- and momentum-resolved XUV photoemission spectroscopy (trARPES) to probe spin-, valley- and layer-dependent electronic excitations, ultrafast excited state carrier scattering and spin transfer processes in TMDCs and TMDC-based heterostructures with ferro- and paramagnetic metals. These processes will be initiated by ultrashort optical laser pulses with selected (linear/circular) polarization. Our goal is obtaining a microscopic understanding of excited state scattering dynamics, relaxation phenomena and spin-transfer processes across various heterostructure interfaces. Furthermore, we will study the dependence of the dynamics on external parameters like strain, electric fields, and interfacial coupling in TMDC-metal heterostructures. These studies will be performed in close collaboration with the projects B08 (Bolotin / Gahl) and B09 (Marques). The long-term goal of our work is to elucidate the potential of TMDCs for ultrafast spintronics and to reveal the underlying fundamental processes of spin- and charge transfer and energy dissipation.
Publications (2nd Funding Period 2022 - 2025)
- Ultrafast optical control of Rashba interactions in TMDC heterostructure
H. Mittenzwey, A. M. Kumar, R. Dhingra, K. Watanabe, T. Taniguchi, C. Gahl, K. I. Bolotin, M. Selig, and A. Knorr
Phys. Rev. Lett. 134, 026901 (2025) - DOI: 10.1103/PhysRevLett.134.026901
- Berry curvature signatures in chiroptical excitonic transitions
S. Beaulieu, S. Dong, V. Christiansson, P. Werner, T. Pincelli, J. D. Ziegler, T. Taniguchi, K. Watanabe, A. Chernikov, M. Wolf, L. Rettig, R. Ernstorfer, and M. Schüler
Sci. Adv. 10, eadk3897 (2024) - DOI: 10.1126/sciadv.adk3897
- Ultrafast spin transfer and its impact on the electronic structure
K. Bobowski, X. Zheng, B. Frietsch, D. Lawrenz, W. Bronsch, C. Gahl, B. Andres, C. Strüber, R. Carley, M. Teichmann, A. Scherz, S. Molodtsov, C. Cacho, R. T. Chapman, E. Springate, and M. Weinelt
Sci. Adv. 10, eadn4613 (2024) - DOI: 10.1126/sciadv.adn4613
- Strain fingerprinting of exciton valley character in 2D semiconductors
A. M. Kumar, D. Yagodkin, R. Rosati, D. J. Bock, C. Schattauer, S. Tobisch, J. Hagel, B. Höfer, J. N. Kirchhof, P. Hernández López, K. Burfeindt, S. Heeg, C. Gahl, F. Libisch, E. Malic, and K. I. Bolotin
Nat. Commun. 15: 7546 (2024) - DOI: 10.1038/s41467-024-51195-y
- Controlling 4f antiferromagnetic dynamics via itinerant electronic susceptibility
S.-E. Lee, Y. W. Windsor, D. Zahn, A. Kraiker, K. Kummer, K. Kliemt, C. Krellner, C. Schüßler-Langeheine, N. Pontius, U. Staub, D. V. Vyalikh, A. Ernst, and L. Rettig
Phys. Rev. Research 6, 043019 (2024) - DOI: 10.1103/PhysRevResearch.6.043019
- Observation of ultrafast interfacial Meitner-Auger energy transfer in a Van der Waals heterostructure
S. Dong, S. Beaulieu, Malte Selig, P. Rosenzweig, D. Christiansen, T. Pincelli, M. Dendzik, J. D. Ziegler, J. Maklar, R P. Xian, A. Neef, A. Mohammed, A. Schulz, M. Stadler, M. Jetter, P. Michler, T. Taniguchi, K. Watanabe, H. Takagi, U. Starke, A. Chernikov, M. Wolf, H. Nakamura, A. Knorr, L. Rettig, and R. Ernstorfer
Nat. Commun. 14, 5057 (2023) - DOI: 10.1038/s41467-023-40815-8
- Observation of multi-directional energy transfer in a hybrid plasmonic–excitonic nanostructure
T. Pincelli, T. Vasileiadis, S. Dong, S. Beaulieu, M. Dendzik, D. Zahn, S.-E. Lee, H. Seiler, Y. Qi, R. P. Xian, J. Maklar, E. Coy, N. S. Mueller, Y. Okamura, S. Reich, M. Wolf, L. Rettig, and R. Ernstorfer
Adv. Mater. 35, 2209100 (2023) - DOI: 10.1002/adma.202209100
- Probing the formation of dark interlayer excitons via ultrafast photocurrent
D. Yagodkin, A. Kumar, E. Ankerhold, J. Richter, K. Watanabe, T. Taniguchi, C. Gahl, and K. I. Bolotin
Nano Lett. 23, 9212 (2023) - DOI: 10.1021/acs.nanolett.3c01708
- Robust magnetic order upon ultrafast excitation of an antiferromagnet
S.-E. Lee, Y. W. Windsor, A. Fedorov, K. Kliemt, C. Krellner, C. Schüßler-Langeheine, N. Pontius, M. Wolf, U. Atxitia, D. V. Vyalikh, and L. Rettig
Adv. Mater. Interfaces 9, 2201340 (2022) - DOI: 10.1002/admi.202201340
- Polarization-modulated angle-resolved photoemission spectroscopy: toward circular dichroism without circular photons and Bloch wave-function reconstruction
M. Schüler, T. Pincelli, S. Dong, T. P. Devereaux, M. Wolf, L. Rettig, R. Ernstorfer, and S. Beaulieu
Phys. Rev. X 12, 011019 (2022) - DOI: 10.1103/PhysRevX.12.011019
- Exchange scaling of ultrafast angular momentum transfer in 4f antiferromagnets
Y.W. Windsor, S.-E. Lee, D. Zahn, V. Borisov, D. Thonig, K. Kliemt, A. Ernst, C. Schüßler-Langeheine, N. Pontius, U. Staub, C. Krellner, D.V. Vyalikh, O. Eriksson, and L. Rettig
Nat. Mater. 21, 514 (2022) - DOI: 10.1038/s41563-022-01206-4
- Intrinsic energy flow in laser-excited 3d ferromagnets
D. Zahn, F. Jakobs, H. Seiler, T. A. Butcher, D. Engel, J. Vorberger, U. Atxitia, Y. W. Windsor, and R. Ernstorfer
Phys. Rev. Res. 4, 013104 (2022) - DOI: 10.1103/PhysRevResearch.4.013104
Publications (1st Funding Period 2018 - 2021)
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Direct measurement of key exciton properties: Energy, dynamics and spatial distribution of the wave function
S. Dong, M. Puppin, T. Pincelli, S. Beaulieu, D. Christiansen, H. Hubener, C. W. Nicholson, R. P. Xian, M. Dendzik, Y. Deng, Y. W. Windsor, M. Selig, E. Malic, A. Rubio, A. Knorr, M. Wolf, L. Rettig, and R. Ernstorfer
Nat. Sci. 1, e10010 (2021) - DOI: 10.1002/ntls.10010 -
Ultrafast dynamical Lifshitz transition
S. Beaulieu, S. Dong, N. Tancogne-Dejean, M. Dendzik, T. Pincelli, J. Maklar, R. P. Xian, M. A. Sentef, M. Wolf, A. Rubio, L. Rettig, and R. Ernstorfer
Sci. Adv. 7 : eabd9275 (2021) - DOI: 10.1126/sciadv.abd9275 -
Exchange-striction driven ultrafast nonthermal lattice dynamics in NiO
Y. W. Windsor, D. Zahn, R. Kamrla, J. Feldl, H. Seiler, C.-T. Chiang, M. Ramsteiner, W. Widdra, R. Ernstorfer, and L. Rettig
Phys. Rev. Lett. 126, 147202 (2021) - DOI: 10.1103/PhysRevLett.126.147202 -
Lattice dynamics and ultrafast energy flow between electrons, spins, and phonons in a 3d ferromagnet
D. Zahn, F. Jakobs, Y. W. Windsor, H. Seiler, T. Vasileiadis, T. A. Butcher, Y. Qi, D. Engel, U. Atxitia, J. Vorberger, and R. Ernstorfer
Phys. Rev. Res. 3, 023032 (2021) - DOI: 10.1103/PhysRevResearch.3.023032 -
Terahertz spin-to-charge conversion by interfacial skew scattering in metallic bilayers
O. Gueckstock, L. Nádvorník, M. Gradhand, T. S. Seifert, G. Bierhance, R. Rouzegar, M. Wolf, M. Vafaee, J. Cramer, M. A. Syskaki, G. Woltersdorf, I. Mertig, G. Jakob, M. Kläui, and T. Kampfrath
Adv. Mater. 33, 2006281 (2021) - DOI: 10.1002/adma.202006281 -
A quantitative comparison of time-of-flight momentum microscopes and hemispherical analyzers for time- and angle-resolved photoemission spectroscopy experiments
J. Maklar, S. Dong, S. Beaulieu, T. Pincelli, M. Dendzik, Y. W. Windsor, R. P. Xian, M. Wolf, R. Ernstorfer, and L. Rettig
Rev. Sci. Instrum. 91, 123112 (2020) - DOI: 10.1063/5.0024493 -
An open-source, end-to-end workflow for multidimensional photoemission spectroscopy
R. P. Xian, Y. Acremann, S. Y. Agustsson, M. Dendzik, K. Bühlmann, D. Curcio, D. Kutnyakhov, F. Pressacco, M. Heber, S. Dong, T. Pincelli, J. Demsar, W. Wurth, P. Hofmann, M. Wolf, M. Scheidgen, L. Rettig, and R. Ernstorfer
Sci. Data 7, 442 (2020) - DOI: 10.1038/s41597-020-00769-8 -
Revealing hidden orbital pseudospin texture with time-reversal dichroism in photoelectron angular distributions
S. Beaulieu, J. Schusser, S. Dong, M. Schüler, T. Pincelli, M. Dendzik, J. Maklar, A. Neef, H. Ebert, K. Hricovini, M. Wolf, J. Braun, L. Rettig, J. Minár, and R. Ernstorfer
Phys. Rev. Lett. 125, 216404 (2020) - DOI: 10.1103/PhysRevLett.125.216404 -
Observation of an excitonic Mott transition through ultrafast core-cum-conduction photoemission spectroscopy
M. Dendzik, R. P. Xian, E. Perfetto, D. Sangalli, D. Kutnyakhov, S. Dong, S. Beaulieu, T. Pincelli, F. Pressacco, D. Curcio, S. Y. Agustsson, M. Heber, J. Hauer, W. Wurth, G. Brenner, Y. Acremann, P. Hofmann, M. Wolf, A. Marini, G. Stefanucci, L. Rettig, and R. Ernstorfer
Phys. Rev. Lett. 125, 096401 (2020) - DOI: 10.1103/PhysRevLett.125.096401 -
Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser
D. Kutnyakhov, R. P. Xian, M. Dendzik, M. Heber, F. Pressacco, S. Y. Agustsson, L. Wenthaus, H. Meyer, S. Gieschen, G. Mercurio, A. Benz, K. Bühlman, S. Däster, R. Gort, D. Curcio, K. Volckaert, M. Bianchi, Ch. Sanders, J. A. Miwa, S. Ulstrup, A. Oelsner, C. Tusche, Y.-J. Chen, D. Vasilyev, K. Medjanik, G. Brenner, S. Dziarzhytski, H. Redlin, B. Manschwetus, S. Dong, J. Hauer, L. Rettig, F. Diekmann, K. Rossnagel, J. Demsar, H.-J. Elmers, Ph. Hofmann, R. Ernstorfer, G. Schönhense, Y. Acremann, and W. Wurth
Rev. Sci. Instr. 91, 013109 (2020) - DOI: 10.1063/1.5118777