Simone Peli

Mottness at finite doping and charge instabilities in cuprates

The influence of the Mott physics on the doping-temperature phase diagram of copper oxides represents a major issue that is subject of intense theoretical and experimental effort. Here, we investigate the ultrafast electron dynamics in prototypical single-layer Bi-based cuprates at the energy scale of the O-2p→Cu-3d charge-transfer (CT) process. We demonstrate a clear evolution of the CT excitations from incoherent and localized, as in a Mott insulator, to coherent and delocalized, as in a conventional metal. This reorganization of the high-energy degrees of freedom occurs at the critical doping pcr ≈0.16 irrespective of the temperature, and it can be well described by dynamical mean field theory calculations. We argue that the onset of the low-temperature charge instabilities is the low-energy manifestation of the underlying Mottness that characterizes the p < pcr region of the phase diagram. This discovery sets a new framework for theories of charge order and low-temperature phases in underdoped copper oxides.

Tracking local magnetic dynamics via high-energy charge excitations in a relativistic Mott insulator

We use time- and energy-resolved optical spectroscopy to investigate the coupling of electron-hole excitations to the magnetic environment in the relativistic Mott insulator Na

Discrimination of molecular thin films by surface-sensitive time-resolved optical spectroscopy

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Collapse of superconductivity in cuprates via ultrafast quenching of phase coherence

IrO

Dynamics of correlation-frozen antinodal quasiparticles in superconducting cuprates

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Ultrafast orbital manipulation and Mott physics in multi-band correlated materials

. We show that, on the picosecond timescale, the photoinjected electron-hole pairs delocalize on the hexagons of the Ir lattice via the formation of quasi-molecular orbital (QMO) excitations and the exchange of energy with the short-range-ordered zig-zag magnetic background. The possibility of mapping the magnetic dynamics, which is characterized by typical frequencies in the THz range, onto high-energy (1-2 eV) charge excitations provides a new platform to investigate, and possibly control, the dynamics of magnetic interactions in correlated materials with strong spin-orbit coupling, even in the presence of complex magnetic phases.

A Route Towards Surface-Sensitive Ultrafast Spectroscopy

An optical discrimination technique, tailored to nanometric-sized, low optical absorbance molecular complexes adhering to thin metal films, is proposed and demonstrated. It is based on a time-resolved evanescent-wave detection scheme in conjunction with hierarchical cluster analysis and principal value decomposition. The present approach aims to differentiate among molecular films based on statistical methods, without using previous detailed knowledge of the physical mechanisms responsible for the detected signal. The technique is open to integration in lab-on-a-chip architectures and nanoscopy platforms for applications ranging from medical screening to material diagnostics.

Crystallization and second harmonic generation in potassium―sodium niobiosilicate glasses

The possibility of driving phase transitions in low-density condensates through the loss of phase coherence alone has far-reaching implications for the study of quantum phases of matter. This has inspired the development of tools to control and explore the collective properties of condensate phases via phase fluctuations. Electrically gated oxide interfaces1,2, ultracold Fermi atoms3,4 and cuprate superconductors5,6, which are characterized by an intrinsically small phase stiffness, are paradigmatic examples where these tools are having a dramatic impact. Here we use light pulses shorter than the internal thermalization time to drive and probe the phase fragility of the Bi2Sr2CaCu2O8+δ cuprate superconductor, completely melting the superconducting condensate without affecting the pairing strength. The resulting ultrafast dynamics of phase fluctuations and charge excitations are captured and disentangled by time-resolved photoemission spectroscopy. This work demonstrates the dominant role of phase coherence in the superconductor-to-normal state phase transition and offers a benchmark for non-equilibrium spectroscopic investigations of the cuprate phase diagram.Pump–probe, time-resolved ARPES experiments with underdoped cuprates reveal the transient enhancement of the density of phase fluctuations, eventually leading to the collapse of superconductivity.

Mechanical Properties of Ag Nanoparticle Thin Films Synthesized by Supersonic Cluster Beam Deposition

A novel ultrafast photoemission technique unveils the Mottness of antinodal quasiparticles in superconducting copper oxides. Many puzzling properties of high–critical temperature (Tc) superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wave vector parallel to the Cu–O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities, and they host the maximum of the anisotropic superconducting gap and pseudogap. We use time-resolved extreme-ultraviolet photoemission with proper photon energy (18 eV) and time resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a nonthermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. Whereas the nodal quasiparticle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2p bands, thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu–O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-Tc superconductivity and other exotic phases of HTSC cuprates.

The room temperature prodrome of charge-order in copper oxides

Multiorbital correlated materials are often on the verge of multiple electronic phases (metallic, insulating, superconducting, charge and orbitally ordered), which can be explored and controlled by small changes of the external parameters. The use of ultrashort light pulses as a mean to transiently modify the band population is leading to fundamentally new results. In this paper we will review recent advances in the field and we will discuss the possibility of manipulating the orbital polarization in correlated multi-band solid state systems. This technique can provide new understanding of the ground state properties of many interesting classes of quantum materials and offers a new tool to induce transient emergent properties with no counterpart at equilibrium. We will address: the discovery of high-energy Mottness in superconducting copper oxides and its impact on our understanding of the cuprate phase diagram; the instability of the Mott insulating phase in photoexcited vanadium oxides; the manipulation of orbital-selective correlations in iron-based superconductors; the pumping of local electronic excitons and the consequent transient effective quasiparticle cooling in alkali-doped fullerides. Finally, we will discuss a novel route to manipulate the orbital polarization in a a k-resolved fashion.