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Andrew P. Mackenzie

Publications and source records attributed to Andrew P. Mackenzie.

At least 19 recordsLinked to original sources

Thermodynamics of $T_{\rm c}$ suppression in far-overdoped Tl$_2$Ba$_2$CuO$_6$

The physical origin of the suppression of superconductivity with hole doping in overdoped cuprates remains unclear. We measure the electronic specific heat of microgram-scale Tl$_2$Ba$_2$CuO$_6$ crystals and find sharp superconducting anomalies persisting far into the overdoped regime. A weak-coupling BCS-like framework incorporating the known Fermi surface and cation disorder quantitatively reproduces the observed anomalies for $T_{\rm c}=14$-$25$ K and their weak doping dependence. The results show $T_{\rm c}(p)$ to be driven predominantly by a smoothly decreasing pairing strength.

cond-mat.supr-con

Entropy mapping under uniaxial pressure utilizing the elastocaloric effect

Uniaxial pressure is a powerful tuning parameter for quantum materials, but conventional thermodynamic probes such as specific heat are difficult to realize in the constrained geometries of strain apparatus. We develop a quantitative analysis framework for a.c. elastocaloric effect measurements that enable the reconstruction of the absolute entropy and hence specific heat across complex phase diagrams. The absolute accuracy is achieved by combining measurements in the strong coupling regime at low frequencies with high signal-to-noise measurements in the quasi-adiabatic regime at high frequencies. Applying the approach to the correlated superconductor Sr$_2$RuO$_4$, we obtain an absolute entropy map across the phase diagram including across phase transitions deep into the superconducting state. We demonstrate that from such data one can derive the absolute specific heat which is currently not possible through other approaches. This data reinforces the finding that the quenching of entropy within the superconductor Sr$_2$RuO$_4$ is strongest at the critical strain consistent with the superconducting gap being maximized at the Van Hove singularity (VHs). Furthermore, we demonstrate that, although $\Delta c /(\gamma T) $ does increase at the VH strain, this increase is much weaker than previously inferred from more indirect caloric experiments.

cond-mat.supr-con

Cryogenic focused-ion-beam microstructuring enabling quantitative $c$-axis transport measurements in Tl$_2$Ba$_2$CuO$_{6+\delta}$

Absolute transport measurements in correlated quantum materials are often limited by disorder, inhomogeneity, geometric uncertainty, and small crystal size. Focused ion beam (FIB) technology offers a route to overcome many of these limitations by enabling transport devices with precisely defined geometry to be fabricated from lamellae extracted from carefully selected regions of a crystal, but its application to cuprate superconductors has been hindered by ion-beam-induced damage. Here we study the clean overdoped cuprate Tl2201 and show that conventional FIB processing causes thermally driven oxygen loss, while cryogenic FIB microstructuring largely suppresses this degradation and preserves the crystal structure from the bulk to the atomic scale. Microstructured devices quantitatively reproduce established in-plane resistivity and Hall carrier density measurements without rescaling. Applying this approach to $c$-axis transport, we obtain absolute $\rho_c(T)$ values approximately three times larger than previously reported, bringing the transport anisotropy into quantitative agreement with the known Fermi surface geometry within an isotropic relaxation-time approximation. These results resolve a long-standing discrepancy between transport and quantum oscillation measurements in overdoped Tl2201 and establish cryogenic FIB microstructuring as a route to reliable quantitative transport measurements in quantum materials where disorder, inhomogeneity, geometry, or small crystal size have previously limited experimental accuracy.

cond-mat.supr-con

Quantum Oscillations of $\mathrm{Sr}_2\mathrm{RuO}_4$ under c-Axis Uniaxial Stress

Uniaxial stress has now been widely used to study correlated electron materials. However, Fermi surface-resolved experimental data on the evolution of the electronic structure under piezoelectrically applied stress are sparse, with no reports of de Haas-van Alphen (dHvA) effects under uniaxial stress. Here we present dHvA measurements under $c$-axis uniaxial stress on the unconventional superconductor $\mathrm{Sr}_2\mathrm{RuO}_4$. This allows us to study the evolution of the electronic structure directly and to gain insight into the contradicting behavior of the predicted enhancement of the electronic density of states and the observed suppression of $T_\text{c}$. We are able to follow all Fermi surfaces for stress up to $-1.8$~GPa and find that the cross-sectional areas of the hole-like $\alpha$ sheet increase and electron-like $\beta$ sheet decrease. At the same time, the area of the electron-like $\gamma$ sheet increases. Therefore, in contrast to in-plane uniaxial stress, charge transfer is the mechanism for approaching the electron-to-hole Lifshitz transition and the associated Van Hove singularity. Additionally, we find that the effective masses on all three Fermi sheets are slightly enhanced as the Lifshitz transition is approached. We compare the dHvA results with quantum oscillations in the magnetostriction and band structure calculations, and find good agreement. At a more general level, our findings show that quantum oscillation measurements under uniaxial stress, combined with band-structure calculations, offer a promising new route for studying quantum materials.

cond-mat.str-el

Uniaxial-Stress-Induced Magnetic Transitions in the Triangular-Lattice Antiferromagnet PdCrO2

Uniaxial stress is a promising method to tune magnetic frustration, allowing its effects to be studied in a precise way. In this work, uniaxial stress is applied to the triangular-lattice antiferromagnet PdCrO2. The Cr-Cr magnetic interaction is very sensitive to interatomic separation, so laboratory-achievable stress can induce substantial changes in magnetic structure. Results from three types of measurement are presented: X-ray diffraction, the stress-strain relationship, and neutron diffraction. The combined data show that the elastic moduli of PdCrO2 are strongly affected by stress-induced changes in magnetic structure. A new, first-order stress-induced magnetic transition is observed, at which the lattice constant shrinks by 0.21%. The lattice stiffens dramatically across this transition: the Young's modulus increases by about 80 GPa, and the Poisson ratio falls from about 1 to about 0.4. This stiffening indicates that the magnetic order "locks," that is, becomes insensitive to lattice strain. This locking might occur because the new stress-induced magnetic order nests the Fermi surface of the Pd sheets. Other frustrated magnets, including candidate spin liquids, may show similarly strong coupling between magnetic and elastic degrees of freedom.

cond-mat.str-el

Disentangling bulk and surface electronic structure using targeted cleave planes in RuO$_2$

Rutile RuO$_2$ has attracted significant interest due to its putative unconventional electronic and magnetic properties and its proximity to superconductivity. However, the measurement and interpretation of its electronic structure has been complicated by a strongly three-dimensional crystal structure. Here, we demonstrate how the preparation of targeted $(110)$ and $(100)$ surfaces via focused ion beam (FIB)-engineered cleaving allows the acquisition of high-quality measurements of the electronic structure using angle-resolved photoemission spectroscopy. Our results demonstrate that ARPES spectra of RuO$_2$ are, in fact, largely dominated by signatures of distinct surface electronic states. From comparison with density-functional theory, we resolve a surface termination-dependent variation of these, and disentangle them from highly-three-dimensional bulk states and surface resonances. Moreover, we find a marked role of the substantial spin-orbit coupling of the Ru 4$d$ orbitals in the surface region, where a breaking of spatial inversion symmetry leads to significant Rashba-type spin splittings of the surface bands.

cond-mat.str-el

A correlated insulator at the surface of the polar metal Ca$_3$Ru$_2$O$_7$

We investigate the electronic structure at the surface of the correlated oxide Ca$_3$Ru$_2$O$_7$, a low-symmetry ruthenate oxide which hosts an unconventional polar-metal phase. From a combination of angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy measurements, we demonstrate that the surface hosts an insulating phase, a distinct departure from metallicity within the bulk. Utilizing quantitative low-energy electron diffraction in conjunction with electronic structure calculations, we show how this results from a combined surface structure relaxation and the impact of marked electronic correlations in this system. Our findings highlight the proximity of Ca$_3$Ru$_2$O$_7$ to an insulating metallic state, and illustrate how subtle structural distortions can control its emergent electronic phases.

cond-mat.str-el

Probing multipolar order in the candidate altermagnet MnF$_2$ through the elastocaloric effect under strain

Altermagnets break a combination of time-reversal and rotational symmetries without generating a net magnetization. As such, the order parameter of $d$-wave altermagnets has the same symmetry as magnetic multipoles, and couples to the product of a magnetic field and uniaxial strain. We combine elastocaloric experiments, free-energy modeling, and first-principles calculations on MnF$_2$ to establish a thermodynamic probe of the predicted finite-temperature altermagnetic critical point. These results pave the way to explore altermagnetic quantum criticality in $d$-wave materials and beyond.

cond-mat.str-el

Adsorbate-induced formation of a surface-polarity-driven nonperiodic superstructure

The chemical and electronic properties of surfaces and interfaces are important for many technologically relevant processes, be it in information processing, where interfacial electronic properties are crucial for device performance, or in catalytic processes, which depend on the types and densities of active nucleation sites for chemical reactions. Quasi-periodic and nonperiodic crystalline surfaces offer new opportunities because of their inherent inhomogeneity, resulting in localisation and properties vastly different from those of surfaces described by conventional Bravais lattices. Here, we demonstrate the formation of a nonperiodic tiling structure on the surface of the frustrated antiferromagnet PdCrO2 due to hydrogen adsorption. The tiling structure exhibits no long-range periodicity but comprises few-atom hexagonally packed domains covering large terraces. Measurement of the local density of states by tunnelling spectroscopy reveals adsorption-driven modifications to the quasi-2D electronic structure of the surface layer, showing exciting opportunities arising from electron localisation.

cond-mat.mtrl-sci

Disorder-induced suppression of superconductivity in infinite-layer nickelates

The pairing symmetry of superconducting infinite-layer nickelates is a fundamental yet experimentally challenging question. We employ high-energy electron irradiation to induce disorder in superconducting Nd$_{0.825}$Sr$_{0.175}$NiO$_2$ thin films and examine the impact of pair-breaking defects on superconductivity and elucidate the nature of the superconducting gap. Our measurements reveal a complete suppression of superconductivity with increasing disorder, suggesting an unconventional, sign-changing order parameter.

cond-mat.supr-con

Directional ballistic magnetotransport in the delafossite metals PdCoO$_2$ and PtCoO$_2$

Studies of electronic transport in width-restricted channels of PdCoO$_2$ have recently revealed a novel `directional ballistic' regime, in which ballistic propagation of electrons on an anisotropic Fermi surface breaks the symmetries of bulk transport. Here we introduce a magnetic field to this regime, in channels of PdCoO$_2$ and PtCoO$_2$ along two crystallographically distinct directions and over a wide range of widths. We observe magnetoresistance distinct from that in the bulk, with features strongly dependent on channel orientation and becoming more pronounced the narrower the channel. Comparison to semi-classical theory establishes that magnetoresistance arises from field-induced modification of boundary scattering, and helps connect features in the data with specific electronic trajectories. However, the role of bulk scattering in our measurements is yet to be fully understood. Our results demonstrate that finite-size magnetotransport is sensitive to the anisotropy of Fermi surface properties, motivating future work to fully understand and exploit this sensitivity.

cond-mat.mes-hall

Dichotomy of electron-phonon interactions in the delafossite PdCoO$_2$: From weak bulk to polaronic surface coupling

The metallic delafossites host ultra-high mobility carriers in the bulk, while at their polar surfaces, intrinsic electronic reconstructions stabilise markedly distinct electronic phases, from charge-disproportionated insulators, to Rashba-split heavy-hole gases and ferromagnetic metals. The understanding of these phases has been strongly informed by surface spectroscopic measurements, but previous studies have been complicated by the presence of spatially varying terminations of the material surface. Here, we demonstrate the potential of microscopic-area angle-resolved photoemission to overcome these challenges. Our measurements of the model compound PdCoO$_2$ yield extremely high-quality spectra of the electronic structure, which allows us to place new experimental constraints on the weak electron-phonon coupling in the bulk of PdCoO$_2$, while revealing much stronger interactions at its surfaces. While the CoO$_2$-terminated surface exhibits a conventional weak-coupling behavior, our measurements reveal surprising spectroscopic signatures of polaron formation at the Pd-terminated surface, despite its pronounced metallicity. Together, our findings reveal how mode and symmetry-selective couplings can markedly tune the electron-phonon interactions in a single host material, here opening routes to stabilise surprisingly persistent polaronic quasiparticles.

cond-mat.mtrl-sci

Hydride superconductivity: here to stay

The field of hydride superconductivity has recently been mired in a controversy that might divert attention from the question of central importance: do hydrides support genuine superconductivity or not? We examine some key papers from the field, and conclude that hydride superconductivity is real.

cond-mat.supr-con

Avoided metallicity in a hole-doped Mott insulator on a triangular lattice

Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO$_2$ layer of the delafossite PdCrO$_2$, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.

cond-mat.str-el

$T_c$ and the elastocaloric effect of Sr$_2$RuO$_4$ under $\langle 110 \rangle$ uniaxial stress: no indications of transition splitting

There is considerable evidence that the superconductivity of Sr2RuO4 has two components. Among this evidence is a jump in the shear elastic modulus $c_{66}$ at the critical temperature $T_c$, observed in ultrasound measurements. Such a jump is forbidden for homogeneous single-component order parameters, and implies that $T_c$ should develop as a cusp under the application of shear strain with $\langle 110 \rangle$ principal axes. This shear strain should split the onset temperatures of the two components, if they coexist, or select one component if they do not. Here, we report measurements of $T_c$ and the elastocaloric effect of Sr2RuO4 under uniaxial stress applied along the $[110]$ lattice direction. Within experimental resolution, we resolve neither a cusp in the stress dependence of $T_c$, nor any second transition in the elastocaloric effect data. We show that reconciling these null results with the observed jumps in $c_{66}$ requires extraordinarily fine tuning to a triple point of the Ginzburg-Landau parameter space. In addition, our results are inconsistent with homogeneous time reversal symmetry breaking at a temperature $T_2 \leq T_c$ as identified in muon spin relaxation experiments.

cond-mat.supr-con

Determination of the dynamic Young's modulus of quantum materials in piezoactuator-driven uniaxial pressure cells using a low-frequency a.c. method

We report on a new technique for measuring the dynamic Young's modulus, $E$, of quantum materials at low temperatures as a function of static tuning strain, $ε$, in piezoactuator-driven pressure cells. In addition to a static tuning of stress and strain, we apply a small-amplitude, finite-frequency a.c. (1 Hz$ \lesssim ω\lesssim $1000 Hz) uniaxial stress, $σ_{ac}$, to the sample and measure the resulting a.c. strain, $ε_{ac}$, using a capacitive sensor to obtain the associated modulus $E$. We demonstrate the performance of the new technique through proof-of-principle experiments on the unconventional superconductor Sr$_2$RuO$_4$, which is known for its rich temperature-strain phase diagram. In particular, we show that the magnitude of $E$, measured using this a.c. technique at low frequencies, exhibits a pronounced nonlinear elasticity, which is in very good agreement with previous Young's modulus measurements on Sr$_2$RuO$_4$ under [100] strain using a d.c. method (Noad et al., Science 382, 447-450 (2023)). By combining the new a.c. Young's modulus measurements with a.c. elastocaloric measurements in a single measurement, we demonstrate that these a.c. techniques are powerful in detecting small anomalies in the elastic properties of quantum materials. Finally, using the case of Sr$_2$RuO$_4$ as an example, we demonstrate how the imaginary component of the modulus can provide additional information about the nature of ordered phases.

cond-mat.mtrl-sci

Controllable suppression of the unconventional superconductivity in bulk and thin-film Sr$_{2}$RuO$_{4}$ via high-energy electron irradiation

In bulk Sr$_{2}$RuO$_{4}$, the strong sensitivity of the superconducting transition temperature $T_{\text{c}}$ to nonmagnetic impurities provides robust evidence for a superconducting order parameter that changes sign around the Fermi surface. In superconducting epitaxial thin-film Sr$_{2}$RuO$_{4}$, the relationship between $T_{\text{c}}$ and the residual resistivity $ρ_0$, which in bulk samples is taken to be a proxy for the low-temperature elastic scattering rate, is far less clear. Using high-energy electron irradiation to controllably introduce point disorder into bulk single-crystal and thin-film Sr$_{2}$RuO$_{4}$, we show that $T_{\text{c}}$ is suppressed in both systems at nearly identical rates. This suggests that part of $ρ_0$ in films comes from defects that do not contribute to superconducting pairbreaking, and establishes a quantitative link between the superconductivity of bulk and thin-film samples.

cond-mat.supr-con

Superconducting Penetration Depth Through a Van Hove Singularity: Sr$_2$RuO$_4$ Under Uniaxial Stress

In the unconventional superconductor Sr$_2$RuO$_4$, uniaxial stress along the $[100]$ direction tunes the Fermi level through a Van Hove singularity (VHS) in the density of states, causing a strong enhancement of the superconducting critical temperature $T_\textrm{c}$. Here, we report measurements of the London penetration depth $λ$ as this tuning is performed. We find that the zero-temperature superfluid density, here defined as $λ(0)^{-2}$, increases by $\sim$15%, with a peak that coincides with the peak in $T_\textrm{c}$. We also find that the low temperature form of $λ(T)$ is quadratic over the entire strain range. Using scanning tunneling microscopy, we find that the gap increases from $Δ_0 \approx 350~μ$eV in unstressed Sr$_2$RuO$_4$ to $Δ_0 \approx 600~μ$eV in a sample strained to near the peak in $T_c$. With a nodal order parameter, an increase in the superconducting gap could bring about an increase in the superfluid density through reduced sensitivity to defects and through reduced non-local effects in the Meissner screening. Our data indicate that tuning to the VHS increases the gap throughout the Brillouin zone, and that non-local effects are likely more important than reduced scattering.

cond-mat.supr-con