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Bo Hao

Publications and source records attributed to Bo Hao.

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Enhanced and robust superconductivity in La0.8Sr0.2NiO2 membranes compressed up to 210 GPa

The discovery of superconductivity in infinite-layer nickelate thin films has opened a new frontier for exploring unconventional oxide superconductors beyond the copper oxide family. However, the presence of substrate hampers investigations under very high pressure. Recently, this problem was circumvented by a study of freestanding Nd0.85Sr0.15NiO2 membranes, which revealed that superconducting transition temperature kept increasing as the pressure was ramped up to 91 GPa, without showing signs of saturation. Naturally, one wonders what would happen at even higher pressures. Here, we report that superconductivity in a freestanding La0.8Sr0.2NiO2 membrane persists under applied ultrahigh pressures up to 210 GPa. The superconducting transition onset temperature exhibits a continuous dome-like evolution, increasing from 16 K at ambient pressure to a peak of 74.5 K at 146 GPa, and then gradually decreasing to 57.4 K at 210 GPa. Such robustness of superconductivity against ultrahigh pressure has not been observed in high-Tc oxide superconductors before.

cond-mat.supr-con

Pauli-limited upper critical field and anisotropic depairing effect of La2.82Sr0.18Ni2O7 superconducting thin film

We investigate the upper critical field and superconducting anisotropy of epitaxial La2.82Sr0.18Ni2O7 thin films, which show a sharp superconducting transition at Tc=31.6 K. Near Tc, superconductivity exhibits thickness-limited two-dimensional characteristics. Upon cooling, the out-of-plane coherence length decreases below the sample thickness of 6 nm, corresponding to a 3-unit-cell film, indicating a crossover to intrinsic three-dimensional bulk superconductivity. High-field transport measurements reveal large upper critical fields with a small anisotropy ratio gama~1.34, comparable to bulk Ruddlesden-Popper nickelates. At low temperatures, the in-plane (ab) upper critical field Hc2(ab) is strongly suppressed by spin-paramagnetic pair breaking and approaches the Pauli limit (Hc2(Pauli)=58 T), while Hc2(c) remains largely unaffected. This anisotropic Pauli limitation accounts for the reduced upper critical field anisotropy and supports the conclusion that superconductivity in these films is fundamentally three-dimensional bulk like. Our results highlight the essential role of spin-paramagnetic effects in shaping the high-field superconducting phase diagram of Ruddlesden-Popper nickelates.

cond-mat.supr-con

Doping evolution of spin excitations in La$_{3-x}$Sr$_{x}$Ni$_2$O$_7$/SrLaAlO$_4$ superconducting thin films

Ambient-pressure superconductivity in compressively strained bilayer nickelate films provides a unique platform to test pairing scenarios, yet the evolution of magnetism with carrier doping remains largely unexplored. Here, we utilize Ni $L_3$-edge resonant inelastic x-ray scattering to systematically track the evolution of spin and electronic excitations in coherently strained La$_{3-x}$Sr$_x$Ni$_2$O$_7$/SrLaAlO$_4$ thin films, spanning the superconducting ($x \le 0.21$) and overdoped non-superconducting ($x = 0.38$) regimes. We reveal that dispersive spin excitations, characterized by double-stripe correlations and nearly doping-independent exchange scales, persist robustly throughout the entire superconducting dome. In stark contrast, upon entering the overdoped non-superconducting state, this coherent magnetic framework undergoes an abrupt collapse, melting into a heavily damped, low-spectral-weight continuum. We show that this magnetic breakdown is fundamentally driven by a selective doping-induced orbital reconstruction. While the invariant $\sim\!1.0$~eV intra-atomic $dd$ peak confirms an intact local octahedral crystal field, the concurrent quenching of the $\sim\!0.4$~eV and $\sim\!1.6$~eV features signifies a severe degradation of the apical-oxygen-mediated $d_{z^2}$--$p_z$--$d_{z^2}$ singlet sector and bilayer charge-transfer coherence. The synchronized demise of coherent spin excitations and macroscopic pairing establishes a direct, doping-controlled link, underscoring that maintaining the localized $d_{z^2}$ magnetic framework and robust apical-oxygen coupling is the fundamental prerequisite for high-$T_c$ superconductivity in bilayer nickelates.

cond-mat.supr-con

Superconducting Dome in $\mathrm{La}_{3-x}\mathrm{Sr}_{x}\mathrm{Ni}_{2}\mathrm{O}_{7-\delta}$ Thin Films

The ambient-pressure superconductivity in $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films via compressive epitaxial strain provides a highly accessible platform for diverse characterization techniques, facilitating the studies of high-temperature superconductivity. Here, we systematically map the phase diagram and reveal the superconducting dome with an electron-hole crossover in compressively strained $\mathrm{La}_{3-x}\mathrm{Sr}_{x}\mathrm{Ni}_{2}\mathrm{O}_{7-\delta}$ thin films by simultaneously tuning Sr doping and oxygen content. The maximum transition temperature (${T}_{c}$) coincides with an anomalous sign change in the Hall coefficient (${R}_{H}$), reminiscent of electron-doped cuprates, which may signal a Fermi surface reconstruction. Beyond the superconducting dome, a $\ln1/T$ insulating regime and a $T$-linear resistivity regime are also resolved, resembling behaviors observed in cuprates and infinite-layer nickelates. This work reveals a dome-shaped relationship between ${T}_{c}$ and ${R}_{H}$ and establishes a key framework for understanding unconventional superconductivity in nickelate systems.

cond-mat.supr-con

Observation of superconductivity-induced leading-edge gap in Sr-doped $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films

The discovery of high-temperature superconductivity in pressurized bulk $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ has ignited significant interest in nickelate superconductors. Unlike cuprates, where superconductivity predominantly originates from the $\mathrm{3}d_{x^2-y^2}$ orbital, nickelates exhibit additional complexities involving contributions from the $\mathrm{3}d_{z^2}$ orbital, prompting fundamental questions about their pairing mechanisms. Despite recent progress in stabilizing superconductivity in $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films at ambient pressure, direct spectroscopic evidence of the superconducting gap opening remains elusive. Here, we present an in-situ angle-resolved photoemission spectroscopy study of Sr-doped superconducting $\mathrm{La}_{3}\mathrm{Ni}_{2}\mathrm{O}_{7}$ thin films. Fermi surface mapping reveals Ni-$\mathrm{3}d_{x^2-y^2}$-derived $\alpha$ and $\beta$ pockets, with orbital fillings of 0.11$\pm$0.02 electrons and 0.66$\pm$0.03 holes per Ni, respectively, resulting in a total of 0.45$\pm$0.04 electrons for each Ni. These bands exhibit moderate electron correlations, characterized by a band renormalization factor of 3-4. Notably, both $\alpha$ and $\beta$ bands exhibit leading-edge shifts across the superconducting transition, with gap magnitude of ~1-2 meV at Fermi momenta along the Brillouin zone diagonal and slightly away from the zone diagonal, deviating from the conventional $d_{x^2-y^2}$-wave gap structure. Additionally, the Ni-$\mathrm{3}d_{z^2}$-derived $\gamma$ band lies ~75 meV below the Fermi level, indicating a $\mathrm{3}d_{x^2-y^2}$-dominated fermiology in this compound.

cond-mat.supr-con

Superconductivity and phase diagram in Sr-doped La$_{3-x}$Sr$_{x}$Ni$_2$O$_7$ thin films

Recent studies have demonstrated ambient pressure superconductivity in compressively strained La$_{3}$Ni$_{2}$O$_{7}$ thin films, yet the phase diagram of heterovalent doping$-$critical for advancing the field$-$remains unexplored. Here, we report superconductivity in Sr$^{2+}$-doped La$_{3-x}$Sr$_{x}$Ni$_2$O$_7$ films synthesized via molecular beam epitaxy with ozone-assisted post-annealing. The superconducting transition temperature ($T_{\mathrm{c}}$) follows an asymmetric dome-like profile, persisting across a wide doping range ($0 \leq x \leq 0.21$) before diminishing at $x \approx 0.38$. Optimally doped films ($x = 0.09$) achieve $T_{\mathrm{c}}$ of $\sim$ 42 K, with high critical current ($J_{\mathrm{c}} > 1.4$ $\mathrm{kA/cm^{2}}$ at 2 K) and upper critical fields ($\mu_{0}H_{\mathrm{c,\parallel}}(0)= 83.7$ $\mathrm{T}$, $\mu_{0}H_{\mathrm{c,\perp}}(0)= 110.3$ $\mathrm{T}$), comparable to reported La$_{3-x}$Pr$_{x}$Ni$_2$O$_7$ films. Scanning transmission electron microscopy reveals oxygen vacancies predominantly occupy at planar NiO$_{2}$ sites$-$unlike apical-site vacancies in bulk samples$-$due to Coulomb repulsion destabilizing planar oxygen under compressive strain. Additionally, the elongated out-of-plane Ni-O bonds, exceeding those in pressurized bulk samples by $4\%$, likely weaken the interlayer $d_{z^2}$ coupling, thus contributing to the reduced $T_{\mathrm{c}}$ in strained films. This work establishes heterovalent Sr$^{2+}$ doping as a robust tuning parameter for nickelate superconductivity, unveiling a unique phase diagram topology.

cond-mat.supr-con

Spin correlations in La$_3$Ni$_2$O$_7$ thin films

The discovery of ambient-pressure superconductivity with $T_{c,\text{onset}} > 40$ K in La$_3$Ni$_2$O$_7$ (LNO) thin films grown on the SrLaAlO$_4$ (SLAO) substrate with compressive ($\varepsilon\approx-2\%$) epitaxial strain provides a unique platform for investigating the superconducting mechanism in nickelate superconductors. Here, we use resonant inelastic X-ray scattering (RIXS) to unveil the dispersive spin excitations in the LNO/SLAO thin film and establish the strain dependence of the electronic and spin excitations in LNO thin films with strain ranging from $\varepsilon\approx-2\%$ to $+1.9\%$. Compared with bulk LNO, LNO/SLAO exhibits similar $dd$ excitations and spin dynamics, but with a larger spin-excitation bandwidth, whereas tensile-strained LNO/SrTiO$_3$ exhibits a marked suppression of both the spin excitations and the Ni $3d_{z^2}$-derived $dd$ excitations. This evolution reflects a strain-tuned interlayer exchange interaction $J_z$ and Ni $3d_{z^2}$-O 2$p_z$ hybridization. Our results demonstrate how epitaxial strain modulates the interlayer magnetic coupling and are consistent with scenarios in which the interlayer antiferromagnetic superexchange interaction promotes interlayer pairing in bilayer nickelates.

cond-mat.supr-con

Electronic Structure of Superconducting Infinite-Layer Lanthanum Nickelates

Revealing the momentum-resolved electronic structure of infinite-layer nickelates is essential for understanding this new class of unconventional superconductors, but has been hindered by the formidable challenges in improving the sample quality. In this work, we report for the first time the angle-resolved photoemission spectroscopy of superconducting La$_{0.8}$Sr$_{0.2}$NiO$_{2}$ films prepared by molecular beam epitaxy and ${\mathrm{\textit{in situ}}}$ atomic-hydrogen reduction. The measured Fermi topology closely matches theoretical calculations, showing a large Ni-$d_{x^2-y^2}$ derived Fermi sheet that evolves from hole-like to electron-like along $k_{z}$, and a three-dimensional (3D) electron pocket centered at Brillouin zone corner. The Ni-$d_{x^2-y^2}$ derived bands show a mass enhancement ($m^*/m_{\rm{DFT}}$) of 2-3,while the 3D electron band shows negligible band renormalization. Moreover, the Ni-$d_{x^2-y^2}$ derived states also display a band dispersion anomaly at higher binding energy, reminiscent of the waterfall feature and kinks observed in cuprates.

cond-mat.supr-con

${\mathrm{\textit{In situ}}}$ preparation of superconducting infinite-layer nickelate thin films with atomically flat surface

Since their discovery, the infinite-layer nickelates have been regarded as an appealing system for gaining deeper insights into high temperature superconductivity (HTSC). However, the synthesis of superconducting samples has been proved to be challenging. Here, we develop an ultrahigh vacuum (UHV) ${\mathrm{\textit{in situ}}}$ reduction method using atomic hydrogen as reducing agent and apply it in lanthanum nickelate system. The reduction parameters, including the reduction temperature (${\mathrm{\textit{T}_{R}}}$) and hydrogen pressure (${\mathrm{\textit{P}_{H}}}$), are systematically explored. We found that the reduction window for achieving superconducting transition is quite wide, reaching nearly 80$^\circ$C in ${\mathrm{\textit{T}_{R}}}$ and 3 orders of magnitude in ${\mathrm{\textit{P}_{H}}}$ when the reduction time is set to 30 mins. And there exists an optimal ${\mathrm{\textit{P}_{H}}}$ for achieving the highest ${\mathrm{\textit{T}_{c}}}$ if both ${\mathrm{\textit{T}_{R}}}$ and reduction time are fixed. More prominently, as confirmed by atomic force microscopy and scanning transmission electron microscopy, the atomically flat surface can be preserved during the ${\mathrm{\textit{in situ}}}$ reduction process, providing advantages over the ${\mathrm{\textit{ex situ}}}$ CaH$_2$ method for surface-sensitive experiments.

cond-mat.supr-con

Superconductivity in freestanding infinite-layer nickelate membranes

The observation of superconductivity in infinite-layer nickelates has attracted significant attention due to its potential as a new platform for exploring high $ \mathrm{\textit{T}}_{c} $ superconductivity. However, thus far, superconductivity has only been observed in epitaxial thin films, which limits the manipulation capabilities and modulation methods compared to two-dimensional exfoliated materials. Given the exceptionally giant strain tunability and stacking capability of freestanding membranes, separating superconducting nickelates from the as-grown substrate is a novel way to engineer the superconductivity and uncover the underlying physics. Herein, we report the synthesis of the superconducting freestanding $ \mathrm{La}_{0.8}\mathrm{Sr}_{0.2}\mathrm{Ni}\mathrm{O}_{2} $ membranes ($ \mathrm{\textit{T}}_{c}\mathrm{=}\mathrm{10.9}\;\mathrm{K} $), emphasizing the crucial roles of the interface engineering in the precursor phase film growth and the quick transfer process in achieving superconductivity. Our work offers a new versatile platform for investigating the superconductivity in nickelates, such as the pairing symmetry via constructing Josephson tunneling junctions and higher $ \mathrm{\textit{T}}_{c} $ values via high-pressure experiments.

cond-mat.supr-con

Spontaneous gap opening and potential excitonic states in an ideal Dirac semimetal Ta$_2$Pd$_3$Te$_5$

The opening of an energy gap in the electronic structure generally indicates the presence of interactions. In materials with low carrier density and short screening length, long-range Coulomb interaction favors the spontaneous formation of electron-hole pairs, so-called excitons, opening an excitonic gap at the Fermi level. Excitonic materials host unique phenomenons associated with pair excitations. However, there is still no generally recognized single-crystal material with excitonic order, which is, therefore, awaited in condensed matter physics. Here, we show that excitonic states may exist in the quasi-one-dimensional material Ta$_2$Pd$_3$Te$_5$, which has an almost ideal Dirac-like band structure, with Dirac point located exactly at Fermi level. We find that an energy gap appears at 350 K, and it grows with decreasing temperature. The spontaneous gap opening is absent in a similar material Ta$_2$Ni$_3$Te$_5$. Intriguingly, the gap is destroyed by the potassium deposition on the crystal, likely due to extra-doped carriers. Furthermore, we observe a pair of in-gap flat bands, which is an analog of the impurity states in a superconducting gap. All these observations can be properly explained by an excitonic order, providing Ta$_2$Pd$_3$Te$_5$ as a new and promising candidate realizing excitonic states.

cond-mat.mtrl-sci