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  1. Free, publicly-accessible full text available November 1, 2024
  2. 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. 
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    Free, publicly-accessible full text available October 1, 2024
  3. 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. 
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    Free, publicly-accessible full text available October 1, 2024
  4. 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. 
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    Free, publicly-accessible full text available September 25, 2024
  5. Abstract

    Charge density waves (CDWs) in kagome metals have been tied to many exotic phenomena. Here, using spectroscopic-imaging scanning tunneling microscopy and angle-resolved photoemission spectroscopy, we study the charge order in kagome metal ScV6Sn6. The similarity of electronic band structures of ScV6Sn6and TbV6Sn6(where charge ordering is absent) suggests that charge ordering in ScV6Sn6is unlikely to be primarily driven by Fermi surface nesting of the Van Hove singularities. In contrast to the CDW state of cousin kagome metals, we find no evidence supporting rotation symmetry breaking. Differential conductance dI/dVspectra show a partial gapΔ1CO ≈ 20 meV at the Fermi level. Interestingly, dI/dVmaps reveal that charge modulations exhibit an abrupt phase shift as a function of energy at energy much higher thanΔ1CO, which we attribute to another spectral gap. Our experiments reveal a distinctive nature of the charge order in ScV6Sn6with fundamental differences compared to other kagome metals.

     
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  6. Free, publicly-accessible full text available June 1, 2024
  7. Abstract

    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.

     
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  8. Abstract In high-temperature ( T c ) cuprate superconductors, many exotic phenomena are rooted in the enigmatic pseudogap state, which has been interpreted as consisting of preformed Cooper pairs or competing orders or a combination thereof. Observation of pseudogap phenomenologically in electron-doped Sr 2 IrO 4 —the 5d electron counterpart of the cuprates, has spurred intense interest in the strontium iridates as a testbed for exploring the exotic physics of the cuprates. Here, we examine the pseudogap state of electron-doped Sr 2 IrO 4 by angle-resolved photoemission spectroscopy (ARPES) and parallel theoretical modeling. Our analysis demonstrates that the pseudogap state of Sr 2 IrO 4 appears without breaking the particle–hole symmetry or inducing spectral broadening which are telltale signatures of competing orders in the cuprates. We find quasiparticle dispersion and its temperature dependence in the pseudogap state of Sr 2 IrO 4 to point to an electronic order with a zero scattering wave vector and limited correlation length. Particle–hole symmetric preformed Cooper pairs are discussed as a viable mechanism for such an electronic order. The potential roles of incommensurate density waves are also discussed. 
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