X-ray photoemission and absorption study of the pyrochlore iridates (Eu1-xBix)2Ir2O7, 0 ⩽x ⩽ 1.

The pyrochlore iridates (Eu1-xBix)2Ir2O7(0⩽x⩽1) undergo an anomalous negative lattice expansion for small Bi-doping (x⩽0.035) (region I) and a normal lattice expansion forx⩾0.1(region II); this is accompanied by a transition from an insulating (and magnetically ordered) to a metallic (and with no magnetic ordering) ground state. Here, we investigate (Eu1-xBix)2Ir2O7(0⩽x⩽1) using hard x-ray photoemission spectroscopy and x-ray absorption fine structure (XAFS) spectroscopy. By analyzing the Eu-L3, Ir-L3and Bi-L2&L3edges x-ray absorption near edge structure spectra and Eu-3dcore-level XPS spectra, we show that the metal cations retain their nominal valence, namely, Ir4+, Bi3+and Eu3+, respectively, throughout the series. The Ir-4fand Bi-4fcore-level XPS spectra consist of screened and unscreened doublets. The unscreened component is dominant In the insulating range (x⩽0.035), and in the metallic region (x⩾0.1), the screened component dominates the spectra. The Eu-3dcore-level spectra remain invariant under Bi doping. The extended XAFS data show that the coordination around the Ir remains well preserved throughout the series. The evolution of the valence band spectra near the Fermi energy with increasing Bi doping indicates the presence of strong Ir(5d)-Bi(6p) hybridization which drives the metal-to-insulator transition.

Imaging the coherent propagation of collective modes in the excitonic insulator Ta2NiSe5 at room temperature.

Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta2NiSe5 Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of ~105 m/s, which we attribute to the hybridization between phonon modes and the phase mode of the condensate. We develop a theoretical framework to support this explanation and propose that electronic interactions provide a substantial contribution to the ordered phase in Ta2NiSe5 These results allow us to understand how the condensate's collective modes transport energy and interact with other degrees of freedom. Our study provides a unique paradigm for the investigation and manipulation of these properties in strongly correlated materials.

Ultrafast melting and recovery of collective order in the excitonic insulator Ta2NiSe5.

The layered chalcogenide Ta2NiSe5 has been proposed to host an excitonic condensate in its ground state, a phase that could offer a unique platform to study and manipulate many-body states at room temperature. However, identifying the dominant microscopic contribution to the observed spontaneous symmetry breaking remains challenging, perpetuating the debate over the ground state properties. Here, using broadband ultrafast spectroscopy we investigate the out-of-equilibrium dynamics of Ta2NiSe5 and demonstrate that the transient reflectivity in the near-infrared range is connected to the system's low-energy physics. We track the status of the ordered phase using this optical signature, establishing that high-fluence photoexcitations can suppress this order. From the sub-50 fs quenching timescale and the behaviour of the photoinduced coherent phonon modes, we conclude that electronic correlations provide a decisive contribution to the excitonic order formation. Our results pave the way towards the ultrafast control of an exciton condensate at room temperature.