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Philip J. W. Moll

Publications and source records attributed to Philip J. W. Moll.

At least 37 records · Page 2Linked to original sources

Switchable chiral transport in charge-ordered Kagome metal CsV$_3$Sb$_5$

When electric conductors differ from their mirror image, unusual chiral transport coefficients appear that are forbidden in achiral metals, such as a non-linear electric response known as electronic magneto-chiral anisotropy (eMChA). While chiral transport signatures are by symmetry allowed in many conductors without a center of inversion, it reaches appreciable levels only in rare cases when an exceptionally strong chiral coupling to the itinerant electrons is present. So far, observations of chiral transport have been limited to materials in which the atomic positions strongly break mirror symmetries. Here, we report chiral transport in the centro-symmetric layered Kagome metal CsV$_3$Sb$_5$, observed via second harmonic generation under in-plane magnetic field. The eMChA signal becomes significant only at temperatures below $T'\sim$ 35 K, deep within the charge-ordered state of CsV$_3$Sb$_5$ ($T_{\mathrm{CDW}}\sim$ 94 K). This temperature dependence reveals a direct correspondence between electronic chirality, unidirectional charge order, and spontaneous time-reversal-symmetry breaking due to putative orbital loop currents. We show that the chirality is set by the out-of-plane field component and that a transition from left- to right-handed transport can be induced by changing the field sign. CsV$_3$Sb$_5$ is the first material in which strong chiral transport can be controlled and switched by small magnetic-field changes, in stark contrast to structurally chiral materials -- a prerequisite for their applications in chiral electronics.

cond-mat.str-el↗

3D Fermi surfaces from charge order in layered CsV$_3$Sb$_5$

The cascade of electronic phases in CsV$_3$Sb$_5$ raises the prospect to disentangle their mutual interactions in a clean, strongly interacting Kagome lattice. When the Kagome planes are stacked into a crystal, its electronic dimensionality encodes how much of the Kagome physics and its topological aspects survive. The layered structure of CsV$_3$Sb$_5$ reflects in Brillouin-zone-sized quasi-2D Fermi surfaces and a significant transport anisotropy. Yet here we demonstrate that CsV$_3$Sb$_5$ is a three-dimensional metal within the charge-density-wave (CDW) state. Small 3D pockets play a crucial role in its low-temperature magneto- and quantum transport. Their emergence at $T_{CDW}\sim 93$ K results in an anomalous sudden increase of the in-plane magnetoresistance by 4 orders of magnitude. The presence of these 3D pockets is further confirmed by quantum oscillations under in-plane magnetic fields - demonstrating their closed nature. These results emphasize the impact of interlayer coupling on the Kagome physics in 3D materials.

cond-mat.str-el↗

Hierarchy of quasi-symmetries and degeneracies in chiral crystal materials CoSi

In materials, certain approximated symmetry operations can exist in a lower-order approximation of the effective model but are good enough to influence the physical responses of the system, and these approximated symmetries were recently dubbed "quasi-symmetries" \cite{guo_arxiv_2021}. In this work, we reveal a hierarchy structure of the quasi-symmetries and the corresponding nodal structures that they enforce via two different approaches of the perturbation expansions for the effective model in the chiral crystal material CoSi. In the first approach, we treat the spin-independent linear momentum (k) term as the zero-order Hamiltonian. Its energy bands are four-fold degenerate due to an SU(2)$\times$SU(2) quasi-symmetry. We next consider both the k-independent spin-orbit coupling (SOC) and full quadratic-k terms as the perturbation terms and find that the first-order perturbation leads to a model described by a self-commuting "stabilizer code" Hamiltonian with a U(1) quasi-symmetry that can protect nodal planes. In the second approach, we treat the SOC-free linear-k term and k-independent SOC term as the zero-order. They exhibit an SU(2) quasi-symmetry, which can be reduced to U(1) quasi-symmetry by a choice of quadratic terms. Correspondingly, a two-fold degeneracy for all the bands due to the SU(2) quasi-symmetry is reduced to two-fold nodal planes that are protected by the U(1) quasi-symmetry. For both approaches, including higher-order perturbation will break the U(1) quasi-symmetry and induce a small gap $\sim$ 1 meV for the nodal planes. These quasi-symmetry protected near degeneracies play an essential role in understanding recent quantum oscillation experiments in CoSi.

cond-mat.mes-hall↗

Quasi-symmetry protected topology in a semi-metal

The crystal symmetry of a material dictates the type of topological band structures it may host, and therefore symmetry is the guiding principle to find topological materials. Here we introduce an alternative guiding principle, which we call 'quasi-symmetry'. This is the situation where a Hamiltonian has an exact symmetry at lower-order that is broken by higher-order perturbation terms. This enforces finite but parametrically small gaps at some low-symmetry points in momentum space. Untethered from the restraints of symmetry, quasi-symmetries eliminate the need for fine-tuning as they enforce that sources of large Berry curvature will occur at arbitrary chemical potentials. We demonstrate that a quasi-symmetry in the semi-metal CoSi stabilizes gaps below 2 meV over a large near-degenerate plane that can be measured in the quantum oscillation spectrum. The application of in-plane strain breaks the crystal symmetry and gaps the degenerate point, observable by new magnetic breakdown orbits. The quasi-symmetry, however, does not depend on spatial symmetries and hence transmission remains fully coherent. These results demonstrate a class of topological materials with increased resilience to perturbations such as strain-induced crystalline symmetry breaking, which may lead to robust topological applications as well as unexpected topology beyond the usual space group classifications.

cond-mat.mtrl-sci↗

Temperature dependence of quantum oscillations from non-parabolic dispersions

The phase offset of quantum oscillations is commonly used to experimentally diagnose topologically non-trivial Fermi surfaces. This methodology, however, is inconclusive for spin-orbit-coupled metals where $π$-phase-shifts can also arise from non-topological origins. Here, we show that the linear dispersion in topological metals leads to a $T^2$-temperature correction to the oscillation frequency that is absent for parabolic dispersions. We confirm this effect experimentally in the Dirac semi-metal Cd$_3$As$_2$ and the multiband Dirac metal LaRhIn$_5$. Both materials match a tuning-parameter-free theoretical prediction, emphasizing their unified origin. For topologically trivial Bi$_2$O$_2$Se, no frequency shift associated to linear bands is observed as expected. However, the $π$-phase shift in Bi$_2$O$_2$Se would lead to a false positive in a Landau-fan plot analysis. Our frequency-focused methodology does not require any input from ab-initio calculations, and hence is promising for identifying correlated topological materials.

cond-mat.str-el↗

Controlling superconductivity of CeIrIn$_5$ microstructures by substrate selection

Superconductor/metal interfaces are usually fabricated in heterostructures that join these dissimilar materials. A conceptually different approach has recently exploited the strain sensitivity of heavy-fermion superconductors, selectively transforming regions of the crystal into the metallic state by strain gradients. The strain is generated by differential thermal contraction between the sample and the substrate. Here, we present an improved finite-element model that reliably predicts the superconducting transition temperature in CeIrIn$_5$ even in complex structures. Different substrates are employed to tailor the strain field into the desired shapes. Using this approach, both highly complex and strained as well as strain-free microstructures are fabricated to validate the model. This enables full control over the microscopic strain fields, and forms the basis for more advanced structuring of superconductors as in Josephson junctions.

cond-mat.supr-con↗

Glass-like Electronics in Vanadium Dioxide

Functional materials can offer new paradigms for miniaturized and energy-efficient electronics, providing a complementary or even alternative platform to metal-oxide-semiconductors. Here we report on electronically accessible long-lived structural states in Vanadium Dioxide that can offer a scheme for data storage and processing. We show that such states can be electrically manipulated and tracked beyond 10,000 seconds after excitation, exhibiting similar features of glasses, which are beyond the classic metastability in Mott systems. Glass-like electronics can potentially overcome some of the fundamental limitations in conventional metal-oxide-semiconductor electronics, and open avenues for neuromorphic computation and multi-level memories.

cond-mat.mes-hall↗

Ionic liquid gating of SrTiO$_3$ lamellas fabricated with a focused ion beam

In this work, we combine two previously-incompatible techniques for defining electronic devices: shaping three-dimensional crystals by focused ion beam (FIB), and two-dimensional electrostatic accumulation of charge carriers. The principal challenge for this integration is nanometer-scale surface damage inherent to any FIB-based fabrication. We address this by using a sacrificial protective layer to preserve a selected pristine surface. The test case presented here is accumulation of 2D carriers by ionic liquid gating at the surface of a micron-scale SrTiO$_3$ lamella. Preservation of surface quality is reflected in superconductivity of the accumulated carriers. This technique opens new avenues for realizing electrostatic charge tuning in materials that are not available as large or exfoliatable single crystals, and for patterning the geometry of the accumulated carriers.

cond-mat.mtrl-sci↗

Low-symmetry non-local transport in microstructured squares of delafossite metals

Intense work studying the ballistic regime of electron transport in two dimensional systems based on semiconductors and graphene had been thought to have established most of the key experimental facts of the field. In recent years, however, new forms of ballistic transport have become accessible in the quasi-two-dimensional delafossite metals, whose Fermi wavelength is a factor of 100 shorter than those typically studied in the previous work, and whose Fermi surfaces are nearly hexagonal in shape, and therefore strongly faceted. This has some profound consequences for results obtained from the classic ballistic transport experiment of studying bend and Hall resistances in mesoscopic squares fabricated from delafossite single crystals. We observe pronounced anisotropies in bend resistances and even a Hall voltage that is strongly asymmetric in magnetic field. Although some of our observations are non-intuitive at first sight, we show that they can be understood within a non-local Landauer-Büttiker analysis tailored to the symmetries of the square/hexagonal geometries of our combined device/Fermi surface system. Signatures of non-local transport can be resolved for squares of linear dimension of nearly 100 $μ$m, approximately a factor of 15 larger than the bulk mean free path of the crystal from which the device was fabricated.

cond-mat.mes-hall↗

Layered Metals as Polarized Transparent Conductors

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Transparent conductors are compromises between electrical conductivity, requiring mobile electrons, and optical transparency based on immobile charges to avoid screening of visible light. Technological solutions reflect this trade-off, achieving the desired transparencies by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. Materials with a quasi-two-dimensional electronic structure have a plasma edge well below the range of visible light while maintaining excellent in-plane conductivity. We demonstrate that slabs of the layered oxides Sr$_2$RuO$_4$ and Tl$_2$Ba$_2$CuO$_{6+δ}$ are optically transparent even at macroscopic thicknesses >2$μ$m for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens, that advancements in a-axis thin film growth will enable.

cond-mat.mtrl-sci↗

Finite-size effects of electron transport in PdCoO$_2$

A wide range of unconventional transport phenomena have recently been observed in single-crystal delafossite metals. Here, we present a theoretical framework to elucidate electron transport using a combination of first-principles calculations and numerical modeling of the anisotropic Boltzmann transport equation. Using PdCoO$_2$ as a model system, we study different microscopic electron and phonon scattering mechanisms and establish the mean free path hierarchy of quasiparticles at different temperatures. We treat the anisotropic Fermi surface explicitly to numerically obtain experimentally-accessible transport observables, which bridge between the "diffusive", "ballistic", and "hydrodynamic" transport regime limits. We illustrate that distinction between the "quasi-ballistic", and "quasi-hydrodynamic" regimes is challenging and often needs to be quantitative in nature. From first-principles calculations, we populate the resulting transport regime plots, and demonstrate how the Fermi surface orientation adds complexity to the observed transport signatures in micro-scale devices. Our work provides key insights into microscopic interaction mechanisms on open hexagonal Fermi surfaces and establishes their connection to the macroscopic electron transport in finite-size channels.

cond-mat.mtrl-sci↗

Evidence of a coupled electron-phonon liquid in NbGe$_2$

Whereas electron-phonon scattering typically relaxes the electron's momentum in metals, a perpetual exchange of momentum between phonons and electrons conserves total momentum and can lead to a coupled electron-phonon liquid with unique transport properties. This theoretical idea was proposed decades ago and has been revisited recently, but the experimental signatures of an electron-phonon liquid have been rarely reported. We present evidence of such a behavior in a transition metal ditetrelide, NbGe$_2$, from three different experiments. First, quantum oscillations reveal an enhanced quasiparticle mass, which is unexpected in NbGe$_2$ due to weak electron-electron correlations, hence pointing at electron-phonon interactions. Second, resistivity measurements exhibit a discrepancy between the experimental data and calculated curves within a standard Fermi liquid theory. Third, Raman scattering shows anomalous temperature dependence of the phonon linewidths which fits an empirical model based on phonon-electron coupling. We discuss structural factors, such as chiral symmetry, short metallic bonds, and a low-symmetry coordination environment as potential sources of coupled electron-phonon liquids.

cond-mat.mtrl-sci↗

Directional ballistic transport in the two-dimensional metal PdCoO2

In an idealized infinite crystal, the material properties are constrained by the symmetries of its unit cell. Naturally, the point-group symmetry is broken by the sample shape of any finite crystal, yet this is commonly unobservable in macroscopic metals. To sense the shape-induced symmetry lowering in such metals, long-lived bulk states originating from anisotropic Fermi surfaces are needed. Here we show how strongly facetted Fermi surfaces and long quasiparticle mean free paths present in microstructures of PdCoO2 yield an in-plane resistivity anisotropy that is forbidden by symmetry on an infinite hexagonal lattice. Bar shaped transport devices narrower than the mean free path are carved from single crystals using focused ion beam (FIB) milling, such that the ballistic charge carriers at low temperatures frequently collide with both sidewalls defining a channel. Two symmetry-forbidden transport signatures appear: the in-plane resistivity anisotropy exceeds a factor of 2, and transverse voltages appear in zero magnetic field. We robustly identify the channel direction as the source of symmetry breaking via ballistic Monte- Carlo simulations and numerical solution of the Boltzmann equation.

cond-mat.mes-hall↗

Scanning SQUID microscopy in a cryogen-free dilution refrigerator

We report a scanning superconducting quantum interference device (SQUID) microscope in a cryogen-free dilution refrigerator with a base temperature at the sample stage of at least 30 mK. The microscope is rigidly mounted to the mixing chamber plate to optimize thermal anchoring of the sample. The microscope housing fits into the bore of a superconducting vector magnet, and our design accommodates a large number of wires connecting the sample and sensor. Through a combination of vibration isolation in the cryostat and a rigid microscope housing, we achieve relative vibrations between the SQUID and sample that allow us to image with micrometer resolution over a 150 $μ$m range while the sample stage temperature remains at base temperature. To demonstrate the capabilities of our system, we show images acquired simultaneously of the static magnetic field, magnetic susceptibility, and magnetic fields produced by a current above a superconducting micrometer-scale device.

cond-mat.mes-hall↗

Sondheimer oscillations as a probe of non-ohmic flow in type-II Weyl semimetal WP$_2$

As conductors in electronic applications shrink, microscopic conduction processes lead to strong deviations from Ohm's law. Depending on the length scales of momentum conserving ($l_{MC}$) and relaxing ($l_{MR}$) electron scattering, and the device size ($d$), current flows may shift from ohmic to ballistic to hydrodynamic regimes and more exotic mixtures thereof. So far, an in situ, in-operando methodology to obtain these parameters self-consistently within a micro/nanodevice, and thereby identify its conduction regime, is critically lacking. In this context, we exploit Sondheimer oscillations, semi-classical magnetoresistance oscillations due to helical electronic motion, as a method to obtain $l_{MR}$ in micro-devices even when $l_{MR}\gg d$. This gives information on the bulk $l_{MR}$ complementary to quantum oscillations, which are sensitive to all scattering processes. We extract $l_{MR}$ from the Sondheimer amplitude in the topological semi-metal WP$_2$, at elevated temperatures up to $T\sim 50$~K, in a range most relevant for hydrodynamic transport phenomena. Our data on micrometer-sized devices are in excellent agreement with experimental reports of the large bulk $l_{MR}$ and thus confirm that WP$_2$ can be microfabricated without degradation. Indeed, the measured scattering rates match well with those of theoretically predicted electron-phonon scattering, thus supporting the notion of strong momentum exchange between electrons and phonons in WP$_2$ at these temperatures. These results conclusively establish Sondheimer oscillations as a quantitative probe of $l_{MR}$ in micro-devices in studying non-ohmic electron flow.

cond-mat.mes-hall↗

Non-monotonic pressure dependence of high-field nematicity and magnetism in CeRhIn$_5$

CeRhIn$_5$ provides a textbook example of quantum criticality in a heavy fermion system: Pressure suppresses local-moment antiferromagnetic (AFM) order and induces superconductivity in a dome around the associated quantum critical point (QCP) near $p_{c} \approx 23\,$kbar. Strong magnetic fields also suppress the AFM order at a field-induced QCP at $B_{\rm c}\approx 50\,$T. In its vicinity, a nematic phase at $B^*\approx 28\,$T characterized by a large in-plane resistivity anisotropy emerges. Here, we directly investigate the interrelation between these phenomena via magnetoresistivity measurements under high pressure. As pressure increases, the nematic transition shifts to higher fields, until it vanishes just below $p_{\rm c}$. While pressure suppresses magnetic order in zero field as $p_{\rm c}$ is approached, we find magnetism to strengthen under strong magnetic fields due to suppression of the Kondo effect. We reveal a strongly non-mean-field-like phase diagram, much richer than the common local-moment description of CeRhIn$_5$ would suggest.

cond-mat.str-el↗

Scale-Invariance of a Spin Liquid in High Magnetic Fields

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$.

cond-mat.str-el↗

Scale-invariant magnetic anisotropy in RuCl$_3$ at high magnetic fields

In RuCl$_3$, inelastic neutron scattering and Raman spectroscopy reveal a continuum of non-spin-wave excitations that persists to high temperature, suggesting the presence of a spin liquid state on a honeycomb lattice. In the context of the Kitaev model, magnetic fields introduce finite interactions between the elementary excitations, and thus the effects of high magnetic fields - comparable to the spin exchange energy scale - must be explored. Here we report measurements of the magnetotropic coefficient - the second derivative of the free energy with respect to magnetic field orientation - over a wide range of magnetic fields and temperatures. We find that magnetic field and temperature compete to determine the magnetic response in a way that is independent of the large intrinsic exchange interaction energy. This emergent scale-invariant magnetic anisotropy provides evidence for a high degree of exchange frustration that favors the formation of a spin liquid state in RuCl$_3$.

cond-mat.str-el↗