Beyond time constants: Quantifying interactions in correlated materials by complementary ultrafast time-domain approaches
Final Report Abstract
Correlated materials are characterized by a variety of interactions between the elementary degrees of freedom, leading to novel ground states with broken symmetries and often intriguing properties. Goal of this project was to combine several ultrafast time-resolved techniques to quantify these interactions, and unravel their relevance in various complex quantum materials. Charge-Density wave (CDW) materials were chosen as model system for electron-phonon (eph) coupling. In the CDW material TbTe3, we quantified based on time-resolved photoemission and diffraction experiments the transient CDW energy surface, extracted the ultrafast CDW trajectories after a photoinduced phase transition, and demonstrated a transient CDW stabilization due to transiently suppressed lattice fluctuations. Furthermore, the CDW dependence of fundamental interactions such as e-ph and electron-electron coupling was studied on the level of individual bands and modes. In TaS2, coherent control of the transition into a metastable, hidden state was demonstrated. Magnetic interactions and exchange coupling were studied in various antiferromagnetic (AFM) materials by time-resolved photoemission and time-resolved resonant x-ray diffraction. Based on a systematic study of magnetization dynamics in intermetallics of type LnRh2Si2 (Ln=rare earth atom), we uncovered a fundamental relation between angular momentum transfer between AFM sublattices, and interlayer exchange coupling, which also depends sensitively on the conduction electron properties. In addition, the energy flow between the different subsystems was systematically studied. In GdRh2Si2, optical control of the direction of the AFM order as well as excitation of coherent magnons could be demonstrated, allowing us to quantify the magnetic-field dependent magnetic anisotropy energy. Finally, the interaction between spin and lattice degrees of freedom in the Mott insulator NiO has been investigated by time-resolved electron diffraction, highlighting the relevance of exchange striction for a long-lasting nonthermal lattice state. In addition, charge order has been identified as dominant order parameter in the charge- and orbitally-ordered mixed-valence manganite Pr0.5Ca0.5MnO3. Overall, the project has shed light on the microscopic interactions driving complex phase transitions in various quantum materials, with promising results for applications e.g. in future information technology.
Publications
-
Disentangling transient charge order from structural dynamics contributions during coherent atomic motion studied by ultrafast resonant x-ray diffraction. Physical Review B, 99(13).
Rettig, L.; Caviezel, A.; Mariager, S. O.; Ingold, G.; Dornes, C.; Huang, S.-W.; Johnson, J. A.; Radovic, M.; Huber, T.; Kubacka, T.; Ferrer, A.; Lemke, H. T.; Chollet, M.; Zhu, D.; Glownia, J. M.; Sikorski, M.; Robert, A.; Nakamura, M.; Kawasaki, M. ... & Staub, U.
-
A quantitative comparison of time-of-flight momentum microscopes and hemispherical analyzers for time- and angle-resolved photoemission spectroscopy experiments. Review of Scientific Instruments, 91(12).
Maklar, J.; Dong, S.; Beaulieu, S.; Pincelli, T.; Dendzik, M.; Windsor, Y. W.; Xian, R. P.; Wolf, M.; Ernstorfer, R. & Rettig, L.
-
Deterministic control of an antiferromagnetic spin arrangement using ultrafast optical excitation. Communications Physics, 3(1).
Windsor, Y. W.; Ernst, A.; Kummer, K.; Kliemt, K.; Schüßler-Langeheine, Ch.; Pontius, N.; Staub, U.; Chulkov, E. V.; Krellner, C.; Vyalikh, D. V. & Rettig, L.
-
Exchange-Striction Driven Ultrafast Nonthermal Lattice Dynamics in NiO. Physical Review Letters, 126(14).
Windsor, Y. W.; Zahn, D.; Kamrla, R.; Feldl, J.; Seiler, H.; Chiang, C.-T.; Ramsteiner, M.; Widdra, W.; Ernstorfer, R. & Rettig, L.
-
Nonequilibrium charge-density-wave order beyond the thermal limit. Nature Communications, 12(1).
Maklar, J.; Windsor, Y. W.; Nicholson, C. W.; Puppin, M.; Walmsley, P.; Esposito, V.; Porer, M.; Rittmann, J.; Leuenberger, D.; Kubli, M.; Savoini, M.; Abreu, E.; Johnson, S. L.; Beaud, P.; Ingold, G.; Staub, U.; Fisher, I. R.; Ernstorfer, R.; Wolf, M. & Rettig, L.
-
Coherent Modulation of Quasiparticle Scattering Rates in a Photoexcited Charge-Density-Wave System. Physical Review Letters, 128(2).
Maklar, J.; Schüler, M.; Windsor, Y. W.; Nicholson, C. W.; Puppin, M.; Walmsley, P.; Fisher, I. R.; Wolf, M.; Ernstorfer, R.; Sentef, M. A. & Rettig, L.
-
Exchange scaling of ultrafast angular momentum transfer in 4f antiferromagnets. Nature Materials, 21(5), 514-517.
Windsor, Y. W.; Lee, S.-E.; Zahn, D.; Borisov, V.; Thonig, D.; Kliemt, K.; Ernst, A.; Schüßler-Langeheine, C.; Pontius, N.; Staub, U.; Krellner, C.; Vyalikh, D. V.; Eriksson, O. & Rettig, L.
-
Robust Magnetic Order Upon Ultrafast Excitation of an Antiferromagnet. Advanced Materials Interfaces, 9(36).
Lee, Sang‐Eun; Windsor, Yoav William; Fedorov, Alexander; Kliemt, Kristin; Krellner, Cornelius; Schüßler‐Langeheine, Christian; Pontius, Niko; Wolf, Martin; Atxitia, Unai; Vyalikh, Denis V. & Rettig, Laurenz
-
Ultrafast Momentum-Resolved Hot Electron Dynamics in the Two-Dimensional Topological Insulator Bismuthene. Nano Letters, 22(13), 5420-5426.
Maklar, Julian; Stühler, Raúl; Dendzik, Maciej; Pincelli, Tommaso; Dong, Shuo; Beaulieu, Samuel; Neef, Alexander; Li, Gang; Wolf, Martin; Ernstorfer, Ralph; Claessen, Ralph & Rettig, Laurenz
-
Coherent light control of a metastable hidden state. Science Advances, 9(47).
Maklar, Julian; Sarkar, Jit; Dong, Shuo; Gerasimenko, Yaroslav A.; Pincelli, Tommaso; Beaulieu, Samuel; Kirchmann, Patrick S.; Sobota, Jonathan A.; Yang, Shuolong; Leuenberger, Dominik; Moore, Robert G.; Shen, Zhi-Xun; Wolf, Martin; Mihailovic, Dragan; Ernstorfer, Ralph & Rettig, Laurenz
-
Controlling 4f antiferromagnetic dynamics via itinerant electronic susceptibilityy. Physical Review Research, 6(4).
Lee, Sang-Eun; Windsor, Yoav William; Zahn, Daniela; Kraiker, Alexej; Kummer, Kurt; Kliemt, Kristin; Krellner, Cornelius; Schüßler-Langeheine, Christian; Pontius, Niko; Staub, Urs; Vyalikh, Denis V.; Ernst, Arthur & Rettig, Laurenz
