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Vibrational coherent control of localized d–d electronic excitation

Nature Physics volume 17, pages 368–373 (2021)Cite this article

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Abstract

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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Fig. 1: Coherent vibrational control of on-site d–d crystal field transitions between different Cu orbital states.
Fig. 2: Experimental evidence of coherent and incoherent phonon dressings of d–d crystal field transitions.
Fig. 3: Phonon-mediated crystal field absorption.

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Source data are provided with this paper. All other data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

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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Author notes

  1. These authors contributed equally: Alexandre Marciniak, Stefano Marcantoni.

Authors and Affiliations

  1. Department of Physics, University of Trieste, Trieste, Italy

    Alexandre Marciniak, Stefano Marcantoni, Francesca Giusti, Filippo Glerean, Giorgia Sparapassi, Francesco Valiera, Fabio Benatti & Daniele Fausti

  2. Elettra-Sincrotrone Trieste S.C.p.A., Trieste, Italy

    Alexandre Marciniak, Francesca Giusti, Filippo Glerean, Giorgia Sparapassi & Daniele Fausti

  3. National Institute for Nuclear Physics (INFN), Trieste Section, Trieste, Italy

    Stefano Marcantoni & Fabio Benatti

  4. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany

    Tobia Nova, Andrea Cartella, Simone Latini & Angel Rubio

  5. Leibniz Institute for Solid State and Materials Research IFW, Dresden, Germany

    Jeroen van den Brink

  6. Institut für Theoretische Physik and Würzburg-Dresden Cluster of Excellence ct.qmat, Technische Universität Dresden, Dresden, Germany

    Jeroen van den Brink

  7. Department of Chemistry, Princeton University, Princeton, NJ, USA

    Daniele Fausti

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Contributions

A.M. and F. Giusti performed the experiments with support from F. Glerean, G.S. and F.V. A.M. analysed the data. S.M., F.B. and F.V. developed the theoretical model. S.M. performed the analytical calculations with support from F.V. and F.B. S.M., S.L. and A.R. conceived and performed the DFT calculations. T.N. and A.C. performed the finite-difference time-domain calculations. J.v.d.B., D.F. and F.B. conceived the effective Hamiltonian model. A.M., S.M., F.B. and D.F. led the data interpretation and the drafting of the manuscript with contributions from all other authors. D.F. conceived and managed the project.

Corresponding author

Correspondence to Daniele Fausti.

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Peer review information Nature Physics thanks Venkatraman Gopalan and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–11, experimental details, complementary results, discussion, details about the theory and calculations, and Tables 1 and 2.

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Source Data Fig. 1

Source data for Fig. 1c.

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Marciniak, A., Marcantoni, S., Giusti, F. et al. Vibrational coherent control of localized d–d electronic excitation. Nat. Phys. 17, 368–373 (2021). https://doi.org/10.1038/s41567-020-01098-8

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