arXiv subjects

P. J. W. Moll

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

16 recordsLinked to original sources

arXiv2026

Three-phonon mixing as a source of light-induced chirality

Mid- and far-infrared optical pulses have found wide applicability in experiments in which collective modes of solids are driven nonlinearly, as a means to manipulate functional properties of materials on ultrafast time scales. In the illustrative case of boron phosphate (BPO$_4$), mid-infrared excitation has been used to induce chirality in an otherwise achiral crystal. The pump frequency dependence of photo-induced chirality reveals that, while on-resonance excitation is understood in terms of the well-documented phonon rectification from two-phonon mixing, additional pathways become relevant when the pump pulse is detuned from resonance. We find that a three-mode mixing mechanism becomes important in this case, whereas the contributions from other impulsive Raman terms are negligible. The results reported here provide a quantitative foundation for nonlinear phononic lineshapes in transparent materials, and open up new opportunities for lattice control.

cond-mat.mtrl-sci↗

arXiv2026

Programmable superconducting diode from nematic domain control in FeSe

The superconducting diode effect (SDE) allows polarity-dependent critical currents when time-reversal and current-inverting spatial symmetries are broken. Superconducting diodes show promise for applications, but inversion asymmetry is usually encoded in sample geometry or non-centrosymmetric crystals, rendering them static circuit elements. Here we demonstrate a programmable superconducting diode whose functionality is encoded in correlated electronic domains. We use the nematic superconductor FeSe as a platform and report a large intrinsic SDE with efficiencies up to $η\sim 75\%$ due to vortices interacting with nematic twin boundaries. The domain wall configuration thus encodes the SDE of the device. Through intense microsecond current pulses to quench the nematic order at rates exceeding $10^7$ K/s, we modify the domain pattern and control the polarity and strength of the SDE. These results establish a new paradigm in which superconducting circuit elements can be programmed through patterns imprinted into correlated electronic states.

cond-mat.supr-con↗

arXiv2025

Electronic dimensionality of UTe2

Superconductivity in the heavy-fermion metal UTe2 survives the application of very high magnetic fields, presenting both an intriguing puzzle and an experimental challenge. The strong, non-perturbative influence of the magnetic field complicates the determination of superconducting order parameters in the high-field phases. Here, we report electronic transport anisotropy measurements in precisely aligned microbars in magnetic fields to 45 T applied along the b-axis. Our results reveal a highly directional vortex pinning force in the field-reinforced phase. The critical current is significantly suppressed for currents along the c direction, whereas the flux-flow voltage is reduced with slight angular misalignments--hallmarks of vortex lock-in transitions typically seen in quasi-2D superconductors like cuprates and pnictides. These findings challenge the assumption of nearly isotropic charge transport in UTe2 and point to enhanced two-dimensionality in the high-field state, consistent with a change in the order parameter. A pair-density-wave-like state at high fields could naturally induce a layered modulation of the superfluid density, forming planar structures that confine vortices and guide their sliding in the flux-flow regime.

cond-mat.supr-con↗

arXiv2025

Non-Fermi liquid quasiparticles in strain-tuned Sr2RuO4

Interacting electrons can form metallic states beyond the Fermi liquid paradigm, a conceptual frontier of many-body physics mainly explored via bulk thermodynamics and transport. In contrast, the microscopics of anomalous single-particle excitations underlying non-Fermi liquid properties have largely remained in the dark. Here we spectroscopically map such quantum-critical excitations in Sr$_2$RuO$_4$ under uniaxial pressure, an experimental challenge overcome by technical advances combining focused ion beam micro-milling with laser angle resolved photoemission. We show that quasiparticle excitations acquire a non-Fermi liquid scattering rate near the critical point but remain remarkably robust throughout the transition. These experiments serve as a benchmark for the theory of anomalous metals and settle the long-standing question if quantum-critical systems host quasiparticle excitations.

cond-mat.str-el↗

arXiv2024

Breaking symmetry with light: photo-induced chirality in a non-chiral crystal

Chirality is a pervasive form of symmetry that is intimately connected to the physical properties of solids, as well as the chemical and biological activity of molecular systems. However, its control with light is challenging, because inducing chirality in a non-chiral material requires that all mirrors and all roto-inversions be simultaneously broken. Electromagnetic fields exert only oscillatory forces that vanish on average, mostly leading to entropy increase that does not break symmetries, per se. Here, we show that chirality of either handedness can be generated in the non-chiral piezoelectric material BPO$_4$, in which two compensated sub-structures of opposite handedness coexist within the same unit cell. By resonantly driving either one of two orthogonal, doubly degenerate vibrational modes at Terahertz frequency, we rectify the lattice distortion and exert a displacive force onto the crystal. The staggered chirality is in this way uncompensated in either direction, inducing chiral structure with either handedness. The rotary power of the photo-induced phases is comparable to the static value of prototypical chiral alpha-quartz, limited by the strength of the pump laser pulse.

cond-mat.mtrl-sci↗

arXiv2023

Controlling crystal cleavage in Focused Ion Beam shaped specimens for surface spectroscopy

Our understanding of quantum materials is commonly based on precise determinations of their electronic spectrum by spectroscopic means, most notably angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). Both require atomically clean and flat crystal surfaces which traditionally are prepared by in-situ mechanical cleaving in ultrahigh vacuum chambers. We present a new approach that addresses three main issues of the current state-of-the-art methods: 1) Cleaving is a highly stochastic and thus inefficient process; 2) Fracture processes are governed by the bonds in a bulk crystal, and many materials and surfaces simply do not cleave; 3) The location of the cleave is random, preventing data collection at specified regions of interest. Our new workflow is based on Focused Ion Beam (FIB) machining of micro-stress lenses in which shape (rather than crystalline) anisotropy dictates the plane of cleavage, which can be placed at a specific target layer. As proof-of-principle we show ARPES results from micro-cleaves of Sr$_2$RuO$_4$ along the ac plane and from two surface orientations of SrTiO$_3$, a notoriously difficult to cleave cubic perovskite.

cond-mat.mtrl-sci↗

arXiv2020

Tuning the structural and antiferromagnetic phase transitions in UCr$_{2}$Si$_2$: hydrostatic pressure and chemical substitution

Structural phase transitions in $f$-electron materials have attracted sustained attention both for practical and basic science reasons, including that they offer an environment to directly investigate relationships between structure and the $f$-state. Here we present results for UCr$_2$Si$_2$, where structural (tetragonal $\rightarrow$ monoclinic) and antiferromagnetic phase transitions are seen at $T_{\rm{S}}$ $=$ 205 K and $T_{\rm{N}}$ $=$ 25 K, respectively. We also provide evidence for an additional second order phase transition at $T_{\rm{X}}$ = 280 K. We show that $T_{\rm{X}}$, $T_{\rm{S}}$, and $T_{\rm{N}}$ respond in distinct ways to the application of hydrostatic pressure and Cr $\rightarrow$ Ru chemical substitution. In particular, hydrostatic compression increases the structural ordering temperature, eventually causes it to merge with $T_{\rm{X}}$ and destroys the antiferromagnetism. In contrast, chemical substitution in the series UCr$_{2-x}$Ru$_x$Si$_2$ suppresses both $T_{\rm{S}}$ and $T_{\rm{N}}$, causing them to approach zero temperature near $x$ $\approx$ 0.16 and 0.08, respectively. The distinct $T-P$ and $T-x$ phase diagrams are related to the evolution of the rigid Cr-Si and Si-Si substructures, where applied pressure semi-uniformly compresses the unit cell and Cr $\rightarrow$ Ru substitution results in uniaxial lattice compression along the tetragonal $c$-axis and an expansion in the $ab$-plane. These results provide insights into an interesting class of strongly correlated quantum materials where degrees of freedom associated with $f$-electron magnetism, strong electronic correlations, and structural instabilities are readily controlled.

cond-mat.str-el↗

arXiv2019

Probing intraband excitations in ZrTe$_5$: a high-pressure infrared and transport study

Zirconium pentatetelluride, ZrTe5, shows remarkable sensitivity to hydrostatic pressure. In this work we address the high-pressure transport and optical properties of this compound, on samples grown by flux and charge vapor transport. The high-pressure resistivity is measured up to 2 GPa, and the infrared transmission up to 9 GPa. The dc conductivity anisotropy is determined using a microstructured sample. Together, the transport and optical measurements allow us to discern band parameters with and without the hydrostatic pressure, in particular the Fermi level, and the effective mass in the less conducting, out-of-plane direction. The results are interpreted within a simple two-band model characterized by a Dirac-like, linear in-plane band dispersion, and a parabolic out-of-plane dispersion.

cond-mat.mtrl-sci↗

arXiv2019

Orbital effect and weak localization physics in the longitudinal magnetoresistance of the Weyl semimetals NbP, NbAs, TaP and TaAs

Weyl semimetals such as the TaAs family (TaAs, TaP, NbAs, NbP) host quasiparticle excitations resembling the long sought after Weyl fermions at special band-crossing points in the band structure denoted as Weyl nodes. They are predicted to exhibit a negative longitudinal magnetoresistance (LMR) due to the chiral anomaly if the Fermi energy is sufficiently close to the Weyl points. However, current jetting effects, i.e. current inhomogeneities caused by a strong, field-induced conductivity anisotropy in semimetals, have a similar experimental signature and therefore have hindered a determination of the intrinsic LMR in the TaAs family so far. This work investigates the longitudinal magnetoresistance of all four members of this family along the crystallographic $a$ and $c$ direction. Our samples are of similar quality as those previously studied in the literature and have a similar chemical potential as indicated by matching quantum oscillation (QO) frequencies. Care was taken to ensure homogeneous currents in all measurements. As opposed to previous studies where this was not done, we find a positive LMR that saturates in fields above 4 T in TaP, NbP and NbAs for $B||c$. Using Fermi-surface geometries from band structure calculations that had been confirmed by experiment, we show that this is the behaviour expected from a classical purely orbital effect, independent on the distance of the Weyl node to the Fermi energy. The TaAs family of compounds is the first to show such a simple LMR without apparent influences of scattering anisotropy. In configurations where the orbital effect is small, i.e. for $B||a$ in NbAs and NbP, we find a non-monotonous LMR including regions of negative LMR. We discuss a weak antilocalisation scenario as an alternative interpretation than the chiral anomaly for these results, since it can fully account for the overall field dependence.

cond-mat.str-el↗

arXiv2017

Single crystal growth, structure and electronic properties of metallic delafossite PdRhO_{2}

We report growth of single crystals of the non-magnetic metallic delafossite PdRhO_{2}, comparing the results from three different methods. Complete crystallographic data were obtained from single crystal X-ray diffraction, and electronic structure calculations made using the refined structural parameters. Focused-ion beam microstructuring was used to prepare a sample for measurements of the in- and out-of-plane electrical resistivity, and the large observed anisotropy is qualitatively consistent with the cylindrical Fermi surface predicted by the calculations.

cond-mat.mes-hall↗

arXiv2017

Electronic in-plane symmetry breaking at field-tuned quantum criticality in CeRhIn5

Electronic nematics are exotic states of matter where electronic interactions break a rotational symmetry of the underlying lattice, in analogy to the directional alignment without translational order in nematic liquid crystals. Intriguingly such phases appear in the copper- and iron-based superconductors, and their role in establishing high-temperature superconductivity remains an open question. Nematicity may take an active part, cooperating or competing with superconductivity, or may appear accidentally in such systems. Here we present experimental evidence for a phase of nematic character in the heavy fermion superconductor CeRhIn5. We observe a field-induced breaking of the electronic tetragonal symmetry of in the vicinity of an antiferromagnetic (AFM) quantum phase transition at Hc~50T. This phase appears in out-of-plane fields of H*~28T and is characterized by substantial in-plane resistivity anisotropy. The anisotropy can be aligned by a small in-plane field component, with no apparent connection to the underlying crystal structure. Furthermore no anomalies are observed in the magnetic torque, suggesting the absence of metamagnetic transitions in this field range. These observations are indicative of an electronic nematic character of the high field state in CeRhIn5. The appearance of nematic behavior in a phenotypical heavy fermion superconductor highlights the interrelation of nematicity and unconventional superconductivity, suggesting nematicity to be a commonality in such materials.

cond-mat.str-el↗

arXiv2015

Nearly-free electrons in a 5d delafossite oxide metal

Understanding the role of electron correlations in strong spin-orbit transition-metal oxides is key to the realisation of numerous exotic phases including spin-orbit assisted Mott insulators, correlated topological solids, and prospective new high-temperature superconductors. To date, most attention has been focussed on the $5d$ iridium-based oxides. Here, we instead consider the Pt-based delafossite oxide PtCoO$_2$. Our transport measurements, performed on single-crystal samples etched to well-defined geometries using focussed ion-beam techniques, yield a room-temperature resistivity of only 2.1~$μΩ$cm, establishing PtCoO$_2$ as the most conductive oxide known. From angle-resolved photoemission and density-functional theory, we show that the underlying Fermi surface is a single cylinder of nearly hexagonal cross-section, with very weak dispersion along k$_z$. Despite being predominantly composed of $d$-orbital character, the conduction band is remarkably steep, with an average effective mass of only 1.14$m_e$. Moreover, the sharp spectral features observed in photoemission remain well-defined with little additional broadening for over 500~meV below E$_F$, pointing to suppressed electron-electron scattering. Together, our findings establish PtCoO$_2$ as a model nearly-free electron system in a $5d$ delafossite transition-metal oxide.

cond-mat.str-el↗

arXiv2013

High-pressure flux growth, structural, and superconducting properties of LnFeAsO (Ln = Pr, Nd, Sm) single crystals

Single crystals of the LnFeAsO (Ln1111, Ln = Pr, Nd, and Sm) family with lateral dimensions up to 1 mm were grown from NaAs and KAs flux at high pressure. The crystals are of good structural quality and become superconducting when O is partially substituted by F (PrFeAsO1-xFx and NdFeAsO1-xFx) or when Fe is substituted by Co (SmFe1-xCoxAsO). From magnetization measurements, we estimate the temperature dependence and anisotropy of the upper critical field and the critical current density of underdoped PrFeAsO0.7F0.3 crystal with Tc = 25 K. Single crystals of SmFe1-xCoxAsO with maximal Tc up to 16.3 K for x = 0.08 were grown for the first time. From transport and magnetic measurements we estimate the critical fields and their anisotropy, and find these superconducting properties to be quite comparable to the ones in SmFeAsO1-xFx with a much higher Tc of = 50 K. The magnetically measured critical current densities are as high as 109 A/m2 at 2 K up to 7 T, with indication of the usual fishtail effect. The upper critical field estimated from resistivity measurements is anisotropic with slopes of -8.7 T/K (H // ab-plane) and -1.7 T/K (H // c-axis). This anisotropy (= 5) is similar to that in other Ln1111 crystals with various higher Tc s.

cond-mat.supr-con↗

arXiv2011

Interplay of composition, structure, magnetism, and superconductivity in SmFeAs1-xPxO1-y

Polycrystalline samples and single crystals of SmFeAs1-xPxO1-y were synthesized and grown employing different synthesis methods and annealing conditions. Depending on the phosphorus and oxygen content, the samples are either magnetic or superconducting. In the fully oxygenated compounds the main impact of phosphorus substitution is to suppress the Néel temperature TN of the spin density wave (SDW) state, and to strongly reduce the local magnetic field in the SDW state, as deduced from muon spin rotation measurements. On the other hand the superconducting state is observed in the oxygen deficient samples only after heat treatment under high pressure. Oxygen deficiency as a result of synthesis at high pressure brings the Sm-O layer closer to the superconducting As/P-Fe-As/P block and provides additional electron transfer. Interestingly, the structural modifications in response to this variation of the electron count are significantly different when phosphorus is partly substituting arsenic. Point contact spectra are well described with two superconducting gaps. Magnetic and resistance measurements on single crystals indicate an in-plane magnetic penetration depth of 200 nm and an anisotropy of the upper critical field slope of 4-5. PACS number(s): 74.70.Xa, 74.62.Bf, 74.25.-q, 81.20.-n

cond-mat.supr-con↗

arXiv2011

Interplay between magnetism and superconductivity in EuFe(2-x)Co(x)As2 studied by 57Fe and 151Eu Mössbauer spectroscopy

The compound EuFe(2-x)Co(x)As2 was investigated by means of the 57Fe and 151Eu Moessbauer spectroscopy versus temperature (4.2 - 300 K) for x=0 (parent), x=0.34 - 0.39 (superconductor) and x=0.58 (overdoped). It was found that spin density wave (SDW) is suppressed by Co-substitution, however it survives in the region of superconductivity, but iron spectra exhibit some non-magnetic component in the superconducting region. Europium orders anti-ferromagnetically regardless of the Co concentration with the spin re-orientation from the a-axis in the parent compound toward c-axis with the increasing replacement of iron by cobalt. The re-orientation takes place close to the a-c plane. Some trivalent europium appears in EuFe(2-x)Co(x)As2 versus substitution due to the chemical pressure induced by Co-atoms and it experiences some transferred hyperfine field from Eu2+. Iron experiences some transferred field due to the europium ordering for substituted samples in the SDW and non-magnetic state both, while the transferred field is undetectable in the parent compound. Superconductivity coexists with the 4f-europium magnetic order within the same volume. It seems that superconductivity has some filamentary character in EuFe(2-x)Co(x)As2 and it is confined to the non-magnetic component seen by the iron Moessbauer spectroscopy.

cond-mat.supr-con↗

arXiv2011

{Rearrangement of the antiferromagnetic ordering at high magnetic fields in SmFeAsO and SmFeAsO$_{0.9}$F$_{0.1}$ single crystals

The low-temperature antiferromagnetic state of the Sm-ions in both nonsuperconducting SmFeAsO and superconducting SmFeAsO$_{0.9}$F$_{0.1}$ single crystals was studied by magnetic torque, magnetization, and magnetoresistance measurements in magnetic fields up to 60~T and temperatures down to 0.6~K. We uncover in both compounds a distinct rearrangement of the antiferromagnetically ordered Sm-moments near $35-40$~T. This is seen in both, static and pulsed magnetic fields, as a sharp change in the sign of the magnetic torque, which is sensitive to the magnetic anisotropy and hence to the magnetic moment in the $ab$-plane, ({\it i.e.} the FeAs-layers), and as a jump in the magnetization for magnetic fields perpendicular to the conducting planes. This rearrangement of magnetic ordering in $35-40$~T is essentially temperature independent and points towards a canted or a partially polarized magnetic state in high magnetic fields. However, the observed value for the saturation moment above this rearrangement, suggests that the complete suppression of the antiferromagnetism related to the Sm-moments would require fields in excess of 60~T. Such a large field value is particularly remarkable when compared to the relatively small Néel temperature $T_{\rm N}\simeq5$~K, suggesting very anisotropic magnetic exchange couplings. At the transition, magnetoresistivity measurements show a crossover from positive to negative field-dependence, indicating that the charge carriers in the FeAs planes are sensitive to the magnetic configuration of the rare-earth elements. This is indicates a finite magnetic/electronic coupling between the SmO and the FeAs layers which are likely to mediate the exchange interactions leading to the long range antiferromagnetic order of the Sm ions.

cond-mat.supr-con↗