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In heavily hole-doped cuprates, superconductivity does not die by simply dissolving into a uniform metal due to the lack of pairing, but rather survives by shattering into nanoscale superconducting puddles. 

Angle-resolved photoemission spectroscopy (ARPES) is a powerful tool for probing the momentum-resolved single-particle spectral function of materials. Historically, in situ magnetic fields have been carefully avoided as they are detrimental to the control of photoelectron trajectory during the photoelectron detection process. However, magnetic field is an important experimental knob for both probing and tuning symmetry-breaking phases and electronic topology in quantum materials. In this paper, we introduce an easily implementable method for realizing an in situ tunable magnetic field at the sample position in an ARPES experiment and analyze magnetic-field-induced artifacts in the ARPES data. Specifically, we identified and quantified three distinct extrinsic effects of a magnetic field: constant energy contour rotation, emission angle contraction, and momentum broadening. We examined these effects in three prototypical quantum materials, i.e., a topological insulator (Bi2Se3), an iron-based superconductor (LiFeAs), and a cuprate superconductor (Pb-Bi2Sr2CuO6+x), and demonstrate the feasibility of ARPES measurements in the presence of a controllable magnetic field. Our studies lay the foundation for the future development of the technique and interpretation of ARPES measurements of field-tunable quantum phases. 

The Fe intercalated transition metal dichalcogenide (TMD), Fe 1 / 3 NbS 2 , exhibits remarkable resistance switching properties and highly tunable spin ordering phases due to magnetic defects. We conduct synchrotron x-ray scattering measurements on both underintercalated ( x = 0.32 ) and overintercalated ( x = 0.35 ) samples. We discover a new charge order phase in the overintercalated sample, where the excess Fe atoms lead to a zigzag antiferromagnetic order. The agreement between the charge and magnetic ordering temperatures, as well as their intensity relationship, suggests a strong magnetoelastic coupling as the mechanism for the charge ordering. Our results reveal the first example of a charge order phase among the intercalated TMD family and demonstrate the ability to stabilize charge modulation by introducing electronic correlations, where the charge order is absent in bulk 2 H − NbS 2 compared to other pristine TMDs. 

We examine key aspects of the theory of the Bardeen–Cooper–Schrieffer (BCS) to Bose–Einstein condensation (BEC) crossover, focusing on the temperature dependence of the chemical potential,μ. We identify an accurate method of determining the change ofμin the cuprate high temperature superconductors from angle-resolved-photoemission data (along the ‘nodal’ direction), and show thatμvaries by less than a few percent of the Fermi energy over a range of temperatures from far below to several times above the superconducting transition temperature,T_c. This shows, unambiguously, that not only are these materials always on the BCS side of the crossover (which is a phase transition in thed-wave case), but are nowhere near the point of the crossover (where the chemical potential approaches the band bottom).

 

Electron-hole bound pairs, or excitons, are common excitations in semiconductors. They can spontaneously form and condense into a new insulating ground state—the so-called excitonic insulator—when the energy of electron-hole Coulomb attraction exceeds the band gap. In the presence of electron-phonon coupling, a periodic lattice distortion often concomitantly occurs. However, a similar structural transition can also be induced by electron-phonon coupling itself, therefore hindering the clean identification of bulk excitonic insulators (e.g., which instability is the driving force of the phase transition). Using high-resolution synchrotron x-ray diffraction and angle-resolved photoemission spectroscopy, we identify key electron-phonon coupling effects in a leading excitonic insulator candidate Ta 2 NiSe 5 . These include an extensive unidirectional lattice fluctuation and an electronic pseudogap in the normal state, as well as a negative electronic compressibility in the charge-doped broken-symmetry state. In combination with first principles and model calculations, we use the normal state electronic spectra to quantitatively determine the electron-phonon interaction vertex g and interband Coulomb interaction V in the minimal lattice model, the solution to which captures the experimental observations. Moreover, we show how the Coulomb and electron-phonon coupling effects can be unambiguously separated based on the solution to quantified microscopic models. Finally, we discuss how the strong lattice fluctuations enabled by low dimensionality relate to the unique electron-phonon interaction effects beyond the textbook Born-Oppenheimer approximation. 

Electron-doped cuprates consistently exhibit strong antiferromagnetic correlations, leading to the prevalent belief that antiferromagnetic spin fluctuations mediate Cooper pairing in these unconventional superconductors. However, early investigations showed that although antiferromagnetic spin fluctuations create the largest pseudogap at hot spots in momentum space, the superconducting gap is also maximized at these locations. This presented a paradox for spin-fluctuation-mediated pairing: Cooper pairing is strongest at momenta where the normal-state low-energy spectral weight is most suppressed. Here we investigate this paradox and find evidence that a gossamer—meaning very faint—Fermi surface can provide an explanation for these observations. We study Nd2–xCexCuO4 using angle-resolved photoemission spectroscopy and directly observe the Bogoliubov quasiparticles. First, we resolve the previously observed reconstructed main band and the states gapped by the antiferromagnetic pseudogap around the hot spots. Within the antiferromagnetic pseudogap, we also observe gossamer states with distinct dispersion, from which coherence peaks of Bogoliubov quasiparticles emerge below the superconducting critical temperature. Moreover, the direct observation of a Bogoliubov quasiparticle permits an accurate determination of the superconducting gap, yielding a maximum value an order of magnitude smaller than the pseudogap, establishing the distinct nature of these two gaps. We propose that orientation fluctuations in the antiferromagnetic order parameter are responsible for the gossamer states. 

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$${d}_{{x}^{2}-{y}^{2}}$$$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 CuL₃and PrM₅resonant x-ray scattering and first-principles calculations, we report a highly correlated three-dimensional charge order in Pr-substituted YBa₂Cu₃O₇, where the Prf-electrons create a direct orbital bridge between CuO₂planes. With this we demonstrate that interplanar orbital engineering can be used to surgically control electronic phases in correlated oxides and other layered materials.