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During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators - an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta2Ni(Se,S)5. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta2NiSe5, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems.

The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the [Formula: see text] orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu L3 and Pr M5 resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa2Cu3O7, where the Pr f-electrons create a direct orbital bridge between CuO2 planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.

Charge order has been a central focus in the study of cuprate high-temperature superconductors due to its intriguing yet not fully understood connection to superconductivity. Recent advances in resonant inelastic x-ray scattering (RIXS) in the soft x-ray regime have enabled the first momentum-resolved studies of dynamic charge order correlations in the cuprates. This progress has opened a window for a more nuanced investigation into the mechanisms behind the formation of charge order (CO) correlations. This review provides an overview of RIXS-based measurements of dynamic CO correlations in various cuprate materials. It specifically focuses on electron-doped cuprates and Bi-based hole-doped cuprates, where the CO-related RIXS signals may reveal signatures of the effective Coulomb interactions. This aims to explore a connection between two central phenomena in the cuprates: strong Coulomb correlations and CO-forming tendencies. Finally, we discuss current open questions and potential directions for future RIXS studies as the technique continues to improve and mature, along with other probes of dynamic correlations that would provide a more comprehensive picture. [ABSTRACT FROM AUTHOR]

During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators – an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta2Ni(Se,S)5. A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta2NiSe5, but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems. The presence of excitonic instability and its relationship with a structural transition in Ta2NiSe5 has been debated. Chen et al. map out the electronic bands and lattice distortion across the semimetal-to-semiconductor transition with sulfur doping, revealing the crucial role of electron-phonon coupling. [ABSTRACT FROM AUTHOR]

The shape of 3d-orbitals often governs the electronic and magnetic properties of correlated transition metal oxides. In the superconducting cuprates, the planar confinement of the d x 2 − y 2 orbital dictates the two-dimensional nature of the unconventional superconductivity and a competing charge order. Achieving orbital-specific control of the electronic structure to allow coupling pathways across adjacent planes would enable direct assessment of the role of dimensionality in the intertwined orders. Using Cu L3 and Pr M5 resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa2Cu3O7, where the Pr f-electrons create a direct orbital bridge between CuO2 planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials. External perturbations can induce 3D charge order in cuprates, but the 3D correlation length is limited and the mechanism is not well understood. Ruiz et al. show that Pr substitution in YBa2Cu3O7 enhances interplanar orbital coupling and stabilizes coherent 3D charge order that coexists with superconductivity. [ABSTRACT FROM AUTHOR]