Vibrational coherent control of localized d–d electronic excitation

Nature Physics 17, 368 - 373 (2021)

Vibrational coherent control of localized d–d electronic excitation

Alexandre Marciniak,Stefano Marcantoni,Francesca Giusti,Filippo Glerean,Giorgia Sparapassi , Tobia Nova,Andrea Cartella,Simone Latini,Francesco Valiera,Angel Rubio,Jeroen van den Brink, Fabio Benatti, Daniele Fausti

Addressing the role of quantum coherence in the interplay between the different matter constituents (electrons, phonons and spin) is a critical step towards understanding transition metal oxides and designing complex materials with new functionalities. Here we use coherent vibrational control of on-site d–d electronic transitions in a model edge-sharing insulating transition metal oxide (CuGeO3) to single out the effects of vibrational coherence in electron–phonon coupling. By comparing time-domain experiments based on high- and low-photon-energy ultrashort laser excitation pulses with a fully quantum description of phonon-assisted absorption, we could distinguish the processes associated with incoherent thermal lattice fluctuations from those driven by the coherent motion of the atoms. In particular, while thermal fluctuations of the phonon bath uniformly increase the electronic absorption, the resonant excitation of phonon modes also results in light-induced transparency that is coherently controlled by the vibrational motion.

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We thank A. Revcolevschi for providing the CuGeO3 samples and the critical reading of the manuscript and A. Cavalleri for his feedback on the manuscript and project. This work was mainly supported by the ERC grant INCEPT no. 677488. F. Glerean was supported by the Italian Ministry of Education, University and Research, MIUR (SIR project grant no. RBSI14ZIY2). This work was partially supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence AIM and SFB925. J.v.d.B. aknowledges support from the Deutsche Forschungsgemeinschaft (DFG) through the Würzburg-Dresden Cluster of Excellence ct.qmat (EXC 2147, project ID 390858490) and CRC 1143 (project no. A05, project ID 247310070). F.B. acknowledges that his research has been conducted within the framework of the Trieste Institute for Theoretical Quantum Technologies.

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