Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy

Abstract

Understanding of the precise mechanisms of high-temperature superconductivity is elusive. In particular, in order to solve the puzzle of the pairing mechanism, it is important to understand the detailed nature of the excitations at energies around the superconducting gap. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy for the first time to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 - 60 meV. These results reveal the correlation between high and low energy excitations, and indicate that the interplay between many-body states on different energy scales conserves phase coherence. In revealing these dynamics we demonstrate that multidimensional coherent spectroscopy can address electronic correlations and interrogate many-body quantum systems in unprecedented ways.

References in corpus (23)

• Angle-resolved photoemission spectroscopy of the cuprate superconductors
• Conventional superconductivity at 203 K at high pressures
• Complexity in Strongly Correlated Electronic Systems
• A Common Thread: the pairing interaction for the unconventional superconductors
• Inelastic Light Scattering From Correlated Electrons
• Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: a non-equilibrium approach
• Higgs Amplitude Mode in BCS Superconductors Nb${}_{1-x}$Ti${}_x$N induced by Terahertz Pulse Excitation
• Steep anomalous dispersion in coherently prepared Rb vapor
• Phonon Assisted Multimagnon Optical Absorption and Long Lived Two-Magnon States in Undoped Lamellar Copper Oxides
• Femtosecond Quasiparticle and Phonon Dynamics in Superconducting YBa2Cu3O7 Studied by Wideband Terahertz Spectroscopy
• Diffusion of Nonequilibrium Quasiparticles in a Cuprate Superconductor
• Chirality density wave of the 'hidden order' phase in URu${}_2$Si${}_2$
• Apical oxygens and correlation strength in electron and hole doped copper oxides
• Snapshots of the retarded interaction of charge carriers with ultrafast fluctuations in cuprates
• Energy dissipation in the time domain governed by bosons in a correlated material
• Witnessing the formation and relaxation of massive quasi-particles in a strongly correlated electron system
• Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects
• Optical Weights and Waterfalls in Doped Charge Transfer Insulators: an LDA+DMFTStudy of LSCO
• Thermal conductivity of lightly Sr- and Zn-doped La${}_2$CuO${}_4$ single crystals
• Isolating quantum coherence with pathway-selective coherent multi-dimensional spectroscopy
• Strain-induced enhancement of the electron energy relaxation in strongly correlated superconductors
• Probing ultrafast spin-relaxation and precession dynamics in a cuprate Mott insulator with 7-fs optical pulses
• Nature of Bosonic Excitations revealed by high-energy charge carriers

Cited by in corpus (5)

• Exciton-polaron interactions in monolayer WS${}_2$
• Two-dimensional polaron spectroscopy of Fermi superfluids
• Direct and ultrafast probing of quantum many-body interaction and Mott-insulator transition through coherent two-dimensional spectroscopy
• Unlocking Quantum Control and Multi-Order Correlations via Terahertz Two-Dimensional Coherent Spectroscopy
• Fundamentals of heterodyne wave mixing spectroscopy: a tutorial