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Shusen Ye

Publications and source records attributed to Shusen Ye.

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Eight-unit-cell electronic modulations in cuprates originating from local molecular orbitals

The pair density wave (PDW) state with eight-unit-cell (8a0) periodicity has been widely regarded as the primary order in cuprates, yet its existence and origin remain subjects of intense debate. Using spectroscopic imaging scanning tunneling microscopy, we observe spatial modulations of the electronic states with approximately 8a0 periodicity in both the superconducting and insulating regimes of hole-doped Ca2CuO2Cl2 cuprate. We find that the 8a0 spatial patterns are generated by the formation of molecular orbitals by doped holes, which organize into 4a0*4a0 plaquettes as the basic unit. Our results identify the 4a0 molecular orbital as the fundamental electronic building block in cuprates, while the 8a0 PDW represents a spatial subharmonic that emerges at sufficiently high doping.

cond-mat.supr-con

Mott-Derived Local Moments and Kondo Hybridization in a d-electron Kagome lattice

Unlike canonical Kondo lattices in f-electron systems, where localized f orbitalsnaturally provide local moments, d-electron Kondo lattices require a distinct mechanism for local-moment formation. However, the study of d-electron Kondo lattices in bulk materials remains far from settled, particularly with regard to the microscopic origin of the local moments. Here, we report a microscopic mechanism for this process in the bilayer kagome metal CsCr6Sb6, where strong correlations drive a Mott splitting of the kagome flat band to supply the requisite local moments. By combining STM/STS and ARPES, we resolve a spectroscopic hierarchy between high-energy correlation effects and low temperature hybridization. Low-temperature STS reveals a robust asymmetric suppression of the density of states near EF that is well captured phenomenologically by a Fano-type lineshape, while ARPES detects a sharp quasiparticlepeak near EF. These low-energy signatures evolveon the same temperature scale and disappear upon warming, consistent with the onset of Kondo hybridization. At the same time, STS resolves symmetric humps at approximately +-50 mV and ARPES identifies a weakly dispersive feature around 50 meV below EF; unlike the near-EF hybridization signatures, these features persist to substantially higher temperatures. This separation of energy and temperature scales supports a two-stage picture in which a kagome flat band first undergoes correlation-driven splitting into lower and upper Hubbard bands, and the occupied lower Hubbard band supplies the local moments that later hybridize with itinerant electrons at lower temperature. Our results therefore move beyond the phenomenology of a kagome Kondo lattice candidate and instead provide a microscopic spectroscopic picture linking Mottness to Kondo hybridization in a frustrated d-electron system.

cond-mat.str-el

Half-filled metal and molecular-orbital-mediated pairing in cuprate

The cuprates exhibit anomalous momentum-space structure with antinodal gap and nodal arc in the underdoped regime, which evolves into a complete hole-type Fermi surface with a large Luttinger volume in the overdoped regime. The real-space electronic structure is also quite complex, as characterized by microscopic inhomogeneities and intertwined density wave orders. Here we show that doped holes in cuprate form localized electronic molecules consisting of 4a0 plaquettes, and each plaquette contains approximately two holes. The effective local doping level is thus around 1/8, which is sufficient to destroy the underlying AF order and more importantly, recovers the half-filled metallic state of the original CuO2 plane. The restored Fermi surface, hosting one hole per unit cell, is consistent with experimental results and satisfies the Luttinger theorem. We then construct the momentum-space structure of the half-filled metal by considering the real-space configuration of electronic molecules. We show that the electronic potential with 4a0 periodicity imposed by the plaquettes and the quantum size effect of electronic molecules obliterate the nested antinodal Fermi surface sheets, leaving behind short arcs with coherent quasiparticles around the node. We propose that two doped holes in each plaquette occupy the shared molecular orbital and form a spin singlet, which can mediate the pairing of itinerant holes on the remnant Fermi surface of the half-filled metal. The electric dipole moment between the molecular orbitals and the dopant ions may also provide a novel attractive interaction between itinerant holes. This phenomenological model for pair formation between itinerant holes on the half-filled Fermi surface mediated by localized molecular orbitals resolves several core issues concerning the mechanism of superconductivity in cuprates.

cond-mat.supr-con

Visualizing the Zhang-Rice singlet, molecular orbitals and pair formation in cuprate

The parent compound of cuprates is a charge-transfer-type Mott insulator with strong hybridization between the Cu $3d_{\mathrm x^2-y^2}$ and O $2p$ orbitals. A key question concerning the pairing mechanism is the behavior of doped holes in the antiferromagnetic (AF) Mott insulator background, which is a prototypical quantum many-body problem. It was proposed that doped hole on the O site tends to form a singlet, known as Zhang-Rice singlet (ZRS), with the unpaired Cu spin. But experimentally little is known about the properties of a single hole and the interplay between them that leads to superconductivity. Here we use scanning tunneling microscopy to visualize the electronic states in hole-doped $\mathrm{Ca_2CuO_2Cl_2}$, aiming to establish the atomic-scale local basis for pair formation. A single doped hole is shown to have an in-gap state and a clover-shaped spatial distribution that can be attributed to a localized ZRS. When the dopants are close enough, they develop delocalized molecular orbitals with characteristic stripe- and ladder-shaped patterns, accompanied by the opening of a small gap around the Fermi level ($E_{\mathrm F}$). With increasing doping, the molecular orbitals proliferate in space and gradually form densely packed plaquettes, but the stripe and ladder patterns remain nearly the same. The low-energy electronic states of the molecular orbitals are intimately related to the local pairing properties, thus play a vitally important role in the emergence of superconductivity. We propose that the Cooper pair is formed by two holes occupying the stripe-like molecular orbital, while the attractive interaction is mediated by the AF spin background.

cond-mat.supr-con

Emergent normal fluid in the superconducting ground state of overdoped cuprates

The microscopic mechanism for the disappearance of superconductivity in overdoped cuprates is still under heated debate. Here we use scanning tunneling spectroscopy to investigate the evolution of quasiparticle interference phenomenon in $\rm Bi_2Sr_2CuO_{6+δ}$ over a wide range of hole densities. We find that when the system enters the overdoped regime, a peculiar quasiparticle interference wavevector with quarter-circle pattern starts to emerge even at zero bias, and its intensity grows with increasing doping level. Its energy dispersion is incompatible with the octet model for d-wave superconductivity, but is highly consistent with the scattering interference of gapless normal carriers. The weight of the gapless quasiparticle interference is mainly located at the antinodes and is independent of temperature. We propose that the normal fluid emerges from the pair-breaking scattering between flat antinodal bands in the quantum ground state, which is the primary cause for the reduction of superfluid density and suppression of superconductivity in overdoped cuprates.

cond-mat.supr-con

The emergence of global phase coherence from local pairing in underdoped cuprates

In conventional metal superconductors such as aluminum, the large number of weakly bounded Cooper pairs become phase coherent as soon as they start to form. The cuprate high critical temperature ($T_c$) superconductors, in contrast, belong to a distinctively different category. To account for the high $T_c$, the attractive pairing interaction is expected to be strong and the coherence length is short. Being doped Mott insulators, the cuprates are known to have low superfluid density, thus are susceptible to phase fluctuations. It has been proposed that pairing and phase coherence may occur separately in cuprates, and $T_c$ corresponds to the phase coherence temperature controlled by the superfluid density. To elucidate the microscopic processes of pairing and phase ordering in cuprates, here we use scanning tunneling microscopy to image the evolution of electronic states in underdoped $\rm Bi_2La_xSr_{2-x}CuO_{6+δ}$. Even in the insulating sample, we observe a smooth crossover from the Mott insulator to superconductor-type spectra on small islands with chequerboard order and emerging quasiparticle interference patterns following the octet model. Each chequerboard plaquette contains approximately two holes, and exhibits a stripy internal structure that has strong influence on the superconducting features. Across the insulator to superconductor boundary, the local spectra remain qualitatively the same while the quasiparticle interferences become long-ranged. These results suggest that the chequerboard plaquette with internal stripes plays a crucial role on local pairing in cuprates, and the global phase coherence is established once its spatial occupation exceeds a threshold.

cond-mat.supr-con

Particle-hole asymmetric superconducting coherence peaks in overdoped cuprates

To elucidate the superconductor to metal transition at the end of superconducting dome, the overdoped regime has stepped onto the center stage of cuprate research recently. Here, we use scanning tunneling microscopy to investigate the atomic-scale electronic structure of overdoped trilayer Bi-2223 and bilayer Bi-2212 cuprates. At low energies the spectroscopic maps are well described by dispersive quasiparticle interference patterns. However, as the bias increases to the superconducting coherence peak energy, a virtually non-dispersive pattern with sqrt(2)*sqrt(2) periodicity emerges. Remarkably, the position of the coherence peaks exhibits evident particle-hole asymmetry which also modulates with the same period. We propose that this is an extreme quasiparticle interference phenomenon, caused by pairing-breaking scattering between flat anti-nodal Bogoliubov bands, which is ultimately responsible for the superconductor to metal transition.

cond-mat.supr-con

Imaging the atomic-scale electronic states induced by a pair of hole dopants in Ca2CuO2Cl2 Mott insulator

We use scanning tunneling microscopy to visualize the atomic-scale electronic states induced by a pair of hole dopants in Ca2CuO2Cl2 parent Mott insulator of cuprates. We find that when the two dopants approach each other, the transfer of spectral weight from high energy Hubbard band to low energy in-gap state creates a broad peak and nearly V-shaped gap around the Fermi level. The peak position shows a sudden drop at distance around 4 a0 and then remains almost constant. The in-gap states exhibit peculiar spatial distributions depending on the configuration of the two dopants relative to the underlying Cu lattice. These results shed important new lights on the evolution of low energy electronic states when a few holes are doped into parent cuprates.

cond-mat.supr-con

Evolution of Charge and Pair Density Modulations in Overdoped Bi2Sr2CuO6+delta

One of the central issues concerning the mechanism of high temperature superconductivity in cuprates is the nature of the ubiquitous charge order and its implications to superconductivity. Here we use scanning tunneling microscopy to investigate the evolution of charge order from the optimally doped to strongly overdoped Bi2Sr2CuO6+δ cuprates. We find that with increasing hole concentration, the long-range checkerboard order gradually evolves into short-range glassy patterns consisting of diluted charge puddles. Each charge puddle has a unidirectional nematic internal structure, and exhibits clear pair density modulations as revealed by the spatial variations of superconducting coherence peak and gap depth. Both the charge puddles and the nematicity vanish completely in the strongly overdoped non-superconducting regime, when another type of short-range order with root2 * root2 periodicity emerges. These results shed important new lights on the intricate interplay between the intertwined orders and the superconducting phase of cuprates.

cond-mat.supr-con

Anomalous doping evolution of superconductivity and quasiparticle interference in Bi2Sr2Ca2Cu3O10+δ trilayer cuprates

We use scanning tunneling microscopy to investigate Bi2Sr2Ca2Cu3O10+δ trilayer cuprates from the optimally doped to overdoped regime. We find that the two distinct superconducting gaps from the inner and outer CuO2 planes both decrease rapidly with doping, in sharp contrast to the nearly constant Tc. Spectroscopic imaging reveals the absence of quasiparticle interference in the antinodal region of overdoped samples, showing an opposite trend to that in single- and double-layer compounds. We propose that the existence of two types of inequivalent CuO2 planes and the intricate interaction between them are responsible for these highly anomalous observations in trilayer cuprates.

cond-mat.supr-con

Zero-energy bound states in the high-temperature superconductors at the two-dimensional limit

Majorana zero modes (MZMs) that obey the non-Abelian statistics have been intensively investigated for potential applications in topological quantum computing. The prevailing signals in tunneling experiments "fingerprinting" the existence of MZMs are the zero-energy bound states (ZEBSs). However, nearly all of the previously reported ZEBSs showing signatures of the MZMs are observed in difficult-to-fabricate heterostructures at very low temperatures and additionally require applied magnetic field. Here, by using in-situ scanning tunneling spectroscopy, we detect the ZEBSs upon the interstitial Fe adatoms deposited on two different high-temperature superconducting one-unit-cell-thick iron chalcogenides on SrTiO3(001). The spectroscopic results resemble the phenomenological characteristics of the MZMs inside the vortex cores of topological superconductors. Our experimental findings may extend the MZM explorations in connate topological superconductors towards an applicable temperature regime and down to the two-dimensional limit. While a concrete understanding of the observations is lacking, possible explanations involving novel 2D superconducting states with spin-orbit coupling, spontaneous nucleation of anomalous vortices at the magnetic sites, and noncoplanar magnetic ordering may further stimulate theoretical understandings of the scarcely captured ZEBSs in strongly correlated systems with multiband Cooper pairing.

cond-mat.supr-con

Effect of structural supermodulation on superconductivity in tri-layer cuprate Bi2Sr2Ca2Cu3O10+x

We investigate the spatial and doping evolutions of the superconducting properties of tri-layer cuprate Bi2Sr2Ca2Cu3O10+x by using scanning tunneling microscopy and spectroscopy. Both the superconducting coherence peak and gap size exhibit periodic variations with the structural supermodulation, but the effect is much more pronounced in the underdoped regime than at optimal doping. Moreover, a new type of tunneling spectrum characterized by two superconducting gaps emerges with increasing doping, and the two-gap features also correlate with the supermodulation. We propose that the interaction between the inequivalent outer and inner CuO2 planes is responsible for these novel features that are unique to tri-layer cuprates.

cond-mat.supr-con

Detection of bosonic mode as a signature of magnetic excitation in one unit cell FeSe on SrTiO3

We report an in situ scanning tunneling spectroscopy study of one-unit-cell (1-UC) FeSe film on SrTiO3(001) (STO) substrate. In quasiparticle density of states, bosonic excitation mode characterized by the "dip-hump" structure is detected outside the larger superconducting gap with energy comparable with phonon and spin resonance modes in heavily electron-doped iron selenides. Statistically, the excitation mode, which is intimately correlated with superconductivity, shows an anticorrelation with pairing strength and yields an energy scale upper-bounded by twice the superconducting gap coinciding with the characteristics of magnetic resonance in cuprates and iron-based superconductors. The local response of tunneling spectra to magnetically different Se defects all exhibits the induced in-gap quasiparticle bound states, indicating an unconventional sign-reversing pairing. These results support the magnetic nature of the excitation mode and possibly reveal a signature of electron-magnetic-excitation coupling in high-temperature superconductivity of 1-UC FeSe/STO.

cond-mat.supr-con