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Nicholas P. Butch

Publications and source records attributed to Nicholas P. Butch.

At least 19 recordsLinked to original sources

Origin of High-Temperature Antiferromagnetic Order in a van der Waals Material

While Van der Waals (vdW) itinerant antiferromagnets with high Neel temperatures (TN) are highly desirable for spintronics, they remain relatively scarce. Here, we unravel the physical origin of the unusually high TN (= 250 K) in the newly identified vdW compound (Fe0.65Co0.35)4GeTe2. The substitution of Co in Fe4GeTe2 induces layer-selective Fe-Co ordering and stabilizes a robust antiferromagnetic (AFM) state primarily driven by Co moments. The AFM order is further strengthened by enhanced electronic correlations of quasi-localized Co 3d-states at the Fermi level, giving rise to an itinerant-localized duality of the 3d electrons. This interplay generates strong magnetic correlations well above TN and stabilizes low-temperature spin canting with a possible nontrivial Berry curvature. Our results establish (Fe0.65Co0.35)4GeTe2 as a rare material bridging fundamental magnetic interactions with potential applications in AFM spintronics.

cond-mat.mtrl-sci

Field-direction sensitivity of Kondo hybridization in UTe$_2$

Neutron scattering experiments on the spin-triplet superconductor UTe$_2$ have established that the dominant low-energy magnetic response is along Brillouin zone boundaries, resembling the magnetic susceptibility of narrow-gap interband excitations. We report a study of the sensitivity of these excitations to magnetic field along the crystallographic $\hat{a}$-axis. Up to fields of $\mu_0 H$=13 T, the maximal inelastic neutron spectral weight increases in energy transfer, with a pronounced increase in $d\hbar\omega_{peak}/dH$ near $\mu_0 H$=7 T. This behavior parallels the field and temperature dependent features of the electrical resistivity that are associated with Kondo hybridization. Our measurements suggest that $\hat{a}$-axis fields near $\mu_0 H$=7~T induce a change in the hybridization between heavy $f$-electrons and the bare conduction band.

cond-mat.str-el

Limited coincidence between ultrahigh-field superconductivity and line of metamagnetic endpoints in UTe$_2$

The field-dependent magnetization of UTe$_2$ was measured through the metamagnetic transition at a variety of field angles, tracking how the step in magnetization evolves with fields tilted away from the $b$ axis. For fields oriented within the $ab$ plane, jumps in both $M_a$ and $M_b$ vanish approximately 18{\deg} away from the $b$ axis. From contactless conductivity measurements, we find that the halo-like high-field superconducting region extends to the $ab$ plane, where it exists only within a very narrow ($<$1{\deg}) angular range near the termination of the metamagnetic phase boundary and extends beyond the highest measured field of 73 T. As the field orientation tilts towards the $c$ axis, the superconducting and metamagnetic phase boundaries no longer coincide and exhibit distinct trends.

cond-mat.supr-con

Visualizing the low-energy electronic structure of the triplet superconductor UTe$_2$ through quasiparticle interference

The identification, control and theoretical modelling of spin-triplet superconductors (STC) remain a central theme in quantum materials research. Intrinsic STC are rare but offer rich condensate properties and unique surface properties allowing insights into the nature of the spin-triplet order, and promising applications in quantum technologies. Owing to interactions, the order parameter in STCs can often be intertwined with other symmetry breaking orders like charge/spin density waves (CDW/SDW) or pair density waves (PDW) complicating their phase diagrams. UTe2 stands out as the only known odd-parity, STC that harbors such intertwined orders on the surface and possible topological surface states composed of Majorana fermions. While the (0-11) facet is the most heavily studied, the fermiology of this surface that gives rise to such exotic phenomena is still lacking and continues to be an area of active interest. Here, we employ low-temperature spectroscopic imaging to reveal the Fermi surface of UTe2 through quasiparticle interference. We find scattering originating from the uranium-derived bands that play a major role in the formation of the CDW and the PDW phases. Tunneling spectroscopy further reveals spectral signatures of the CDW gap, corroborating its onset temperature. Suppressing the CDW with a magnetic field, highlights the presence of small, circular Fermi pockets that disperse strongly near the Fermi energy. We discuss the nature of the interference patterns and the origin of the small Fermi pockets in the context of the calculated band structure and the unconventional CDW phase.

cond-mat.supr-con

Enhancement of antiferromagnetic spin fluctuations in UTe$_2$ under pressure revealed by $^{125}$Te NMR

Characterizing magnetic fluctuations is one of the keys to understanding the origin of superconductivity in the spin-triplet superconductor UTe$_2$ which exhibits two superconducting (SC) phases (SC1 and SC2) under pressure: SC1 where a superconducting transition temperature of $T_{\rm c}$ decreases with pressure while $T_{\rm c}$ of SC2 rises with pressure. Previously, D. Ambika et al. [Phys. Rev. B 105, L220403 (2022)] have reported the possible coexistence of ferromagnetic (FM) and antiferromagnetic (AFM) spin fluctuations in UTe$_2$ under pressure from their nuclear magnetic resonance (NMR) measurements. To delve the relationship between the magnetic fluctuations and the two SC phases, we have carried out detailed $^{125}$Te NMR measurements on a single crystal of UTe$_2$ with $T_{\rm c}$ = 1.6 K at various pressures ranging from 0 to 2.05 GPa. By comparing the temperature $T$ dependence of nuclear spin-lattice relaxation rates divided by temperature 1/$T_1T$ with that of the Knight shift $K$ for magnetic fields along the $a$, $b$, and $c$ directions, we evidence the enhancement of AFM spin fluctuations with increasing pressure. Based on the results, we suggest that FM spin fluctuations are more favorable for SC1 and AFM spin fluctuations are crucial for SC2. Our findings will inspire further study on this material to understand the peculiar SC phases in detail.

cond-mat.supr-con

Giant transverse magnetic fluctuations at the edge of re-entrant superconductivity in UTe$_{2}$

UTe$_{2}$ exhibits the remarkable phenomenon of re-entrant superconductivity, whereby the zero-resistance state reappears above 40 tesla after being suppressed with a field of around 10 tesla. One potential pairing mechanism, invoked in the related re-entrant superconductors UCoGe and URhGe, involves transverse fluctuations of a ferromagnetic order parameter. However, the requisite ferromagnetic order - present in both UCoGe and URhGe - is absent in UTe$_{2}$, and magnetization measurements show no sign of strong fluctuations. Here, we measure the magnetotropic susceptibility of UTe$_{2}$ across two field-angle planes. This quantity is sensitive to the magnetic susceptibility in a direction transverse to the applied magnetic field - a quantity that is not accessed in conventional magnetization measurements. We observe a very large decrease in the magnetotropic susceptibility over a broad range of field orientations, indicating a large increase in the transverse magnetic susceptibility. The three superconducting phases of UTe$_{2}$, including the high-field re-entrant phase, surround this region of enhanced susceptibility in the field-angle phase diagram. The strongest transverse susceptibility is found near the critical end point of the high-field metamagnetic transition, suggesting that quantum critical fluctuations of a field-induced magnetic order parameter may be responsible for the large transverse susceptibility, and may provide a pairing mechanism for field-induced superconductivity in UTe$_{2}$.

cond-mat.str-el

Odd-Parity Quasiparticle Interference in the Superconductive Surface State of UTe2

Although no known material exhibits intrinsic topological superconductivity, wherein spin-triplet odd-parity electron pairing occurs, UTe2 is now the leading representative of this class. Conventionally, the parity of the superconducting order parameter may be established by using Bogoliubov quasiparticle interference (QPI) imaging. However, odd-parity superconductors should support a topological quasiparticle surface band (QSB) at energies within the maximum superconducting energy gap. QPI would then be dominated by the electronic structure of the QSB and only reveal the characteristics of the bulk order parameter excursively. Here, we visualize quasiparticle interference patterns of UTe2 and find that, at the (0-11) cleave surface, a new band of Bogoliubov quasiparticles appears only in the superconducting state. QPI visualization then allows study of dispersion of states within this QSB, which we demonstrate exists only within the range of Fermi momenta projected onto the (0-11) surface. Finally, we develop a theoretical framework to predict the QPI signatures of such a QSB at the (0-11) surface of UTe2. Its predictions are most consistent with the experimental results if the bulk superconducting gap function exhibits time-reversal conserving, odd-parity, a-axis nodal, B3u symmetry.

cond-mat.supr-con

Revealing isotropic abundant low-energy excitations in UTe$_2$ through complex microwave surface impedance

The complex surface impedance is a well-established tool to study the super- and normal-fluid responses of superconductors. Fundamental properties of the superconductor, such as the pairing mechanism, Fermi surface, and topological properties, also influence the surface impedance. We explore the microwave surface impedance of spin-triplet UTe$_2$ single crystals as a function of temperature using resonant cavity perturbation measurements employing a novel multi-modal analysis to gain insight into these properties. We determine a composite surface impedance of the crystal for each mode using resonance data combined with the independently measured normal state dc resistivity tensor. The normal state surface impedance reveals the weighting of current flow directions in the crystal of each resonant mode. For UTe$_2$, we find an isotropic $\Delta \lambda(T) \sim T^\alpha$ power-law temperature dependence for the magnetic penetration depth for $T\le T_c/3$ with $\alpha < 2$, which is inconsistent with a single pair of point nodes on the Fermi surface under weak scattering. We also find a similar power-law temperature dependence for the low-temperature surface resistance $R_s(T) \sim T^{\alpha_R}$ with $\alpha_R < 2$. We observe a strong anisotropy of the residual microwave loss across these modes, with some modes showing loss below the universal line-nodal value, to those showing substantially more. We compare to predictions for topological Weyl superconductivity in the context of the observed isotropic power-laws, and anisotropy of the residual loss.

cond-mat.supr-con

Pair Wavefunction Symmetry in UTe2 from Zero-Energy Surface State Visualization

Although nodal spin-triplet topological superconductivity appears probable in UTe2, its superconductive order-parameter $\Delta_k$ remains unestablished. In theory, a distinctive identifier would be the existence of a superconductive topological surface band (TSB), which could facilitate zero-energy Andreev tunneling to an s-wave superconductor, and also distinguish a chiral from non-chiral $\Delta_k$ via enhanced s-wave proximity. Here we employ s-wave superconductive scan-tips and detect intense zero-energy Andreev conductance at the UTe2 (0-11) termination surface. Imaging reveals sub-gap quasiparticle scattering interference signatures with a-axis orientation. The observed zero-energy Andreev peak splitting with enhanced s-wave proximity, signifies that $\Delta_k$ of UTe2 is a non-chiral state: B1u, B2u or B3u. However, if the quasiparticle scattering along the a-axis is internodal, then a non-chiral B3u state is the most consistent for UTe2.

cond-mat.supr-con

Field-angle evolution of the superconducting and magnetic phases of UTe$_2$ around the $b$ axis

We experimentally determine the bounds of the magnetic-field-induced superconducting and magnetic phases near the crystalline $b$ axis of uranium ditelluride (UTe$_2$). By measuring the magnetoresistance as a function of rotation angle and field strength in magnetic fields as large as 41.5 T, we have studied these boundaries in three dimensions of magnetic field direction. The phase boundaries in all cases obey crystallographic symmetries and no additional symmetries, evidence against any symmetry-breaking quadrupolar or higher magnetic order. We find that the upper critical field of the zero-field superconducting state is well-described by an anisotropic mass model. In contrast, the angular boundaries of the $b$-axis-oriented field-reentrant superconducting phase are nearly constant as a function of field up to the metamagnetic transition, with anisotropy between the $ab$ and $bc$ planes that is comparable to the angular anisotropy of the metamagnetic transition itself. We discuss the relationship between the observed superconducting boundaries and the underlying $\mathbf{d}$ vector that represents the spin-triplet order parameter. Additionally, we report an unexplained normal-state feature in resistance and track its evolution as a function of field strength and angle.

cond-mat.supr-con

Connection between f-electron correlations and magnetic excitations in UTe2

The detailed anisotropy of the low-temperature, low-energy magnetic excitations of the candidate spin-triplet superconductor UTe$_2$ is revealed using inelastic neutron scattering. The magnetic excitations emerge from the Brillouin zone boundary at the high symmetry $Y$ and $T$ points and disperse along the crystallographic $\hat{b}$-axis. In applied magnetic fields to at least $\mu_0 H=11$~T along the $\hat{c}-$axis, the magnetism is found to be field-independent in the $(hk0)$ plane. The scattering intensity is consistent with that expected from U$^{3+}$/U$^{4+}$ $f$-electron spins with preferential orientation along the crystallographic $\hat{a}$-axis, and a fluctuating magnetic moment of 2.3(7) $\mu_B$. These characteristics indicate that the excitations are due to intraband spin excitons arising from $f$-electron hybridization.

cond-mat.str-el

Itinerant A-type Antiferromagnetic Order in Co$_{0.25}$TaSe$_2$

We present the magnetic behavior and resulting transport properties of TaSe$_2$ when intercalated by magnetically active cobalt cations. Acting as the layered host, TaSe$_2$ is a transition metal dichalcogenide (TMD) that adopts the 2H-polytype. We find through our single crystal and powder diffraction studies that we can prepare the stoichiometry Co$_{0.25}$TaSe$_2$, which crystallizes in the centrosymmetric space group $P6_3/mmc$. From magnetic susceptibility and x-ray photoelectron spectroscopy measurements, we find a transition consistent with antiferromagnetic order below the temperature $T_N$ = 173 K and Co$^{2+}$ in the high-spin state. Neutron powder diffraction and specific heat measurements, however, point to a much smaller than anticipated ordered moment in this sample. From the neutron results, the magnetic structure can be described as an A-type antiferromagnet with an ordered moment size of 1.35(11) $\mu_B$ per Co cation. The direction of the moments are all long the c-axis, which is consistent with the magnetization and susceptibility studies showing this direction to be the easy axis. Interestingly, we find that a weak and subtle ferromagnetic component appears to exist along the $ab$-plane of the Co$_{0.25}$TaSe$_2$ crystals. We place the results of this work in the context of other magnetic-ion intercalated TMDs, especially those of Ta and Nb.

cond-mat.str-el

Synthesis and characterization of the novel breathing pyrochlore compound Ba3Tm2Zn5O11

In this study, a novel material from the rare-earth based breathing pyrochlore family, Ba3Tm2Zn5O11, was successfully synthesized. Powder x-ray diffraction and high-resolution powder neutron diffraction confirmed phase purity and the F-43m breathing pyrochlore crystal structure, while thermogravimetric analysis revealed incongruent melting behavior compared to its counterpart, Ba3Yb2Zn5O11. High-quality single crystals of Ba3Tm2Zn5O11 were grown using the traveling solvent floating zone technique and assessed using Laue x-ray diffraction and single crystal x-ray diffraction. Thermodynamic characterization indicated paramagnetic behavior down to 0.05 K, and inelastic neutron scattering measurements identified distinct dispersionless crystal electric field energy bands, with the fitted crystal electric field model predicting a single-ion singlet ground state and an energy gap of ~9 meV separating it from the first excited (singlet) state. Additional low-energy excitation studies on single crystals revealed dispersionless bands at 0.8 and 1 meV. Computed phonon dispersions from first-principles calculations ruled out phonons as the origin of these modes, further illustrating the puzzling and unique properties of Ba3Tm2Zn5O11.

cond-mat.str-el

Absence of a bulk charge density wave signature in x-ray measurements of UTe$_2$

The long-sought pair density wave (PDW) is an exotic phase of matter in which charge density wave (CDW) order is intertwined with the amplitude or phase of coexisting, superconducting order \cite{Berg2009,Berg2009b}. Originally predicted to exist in copper-oxides, circumstantial evidence for PDW order now exists in a variety of materials. Recently, scanning tunneling microscopy (STM) studies have reported evidence for a three-component charge density wave (CDW) at the surface of the heavy-fermion superconductor, UTe$_2$, persisting below its superconducting transition temperature. Here, we use hard x-ray diffraction measurements on crystals of UTe$_2$ at $T = 1.9$ K and $12$ K to search for a bulk signature of this CDW. Using STM measurements as a constraint, we calculate the expected locations of CDW superlattice peaks, and sweep a large volume of reciprocal space in search of a signature. We failed to find any evidence for a CDW near any of the expected superlattice positions in many Brillouin zones. We estimate an upper bound on the CDW lattice distortion of $u_{max} \lesssim 4 \times 10^{-3} \mathrm{\AA}$. Our results suggest that the CDW observed in STM is either purely electronic, somehow lacking a signature in the structural lattice, or is restricted to the material surface.

cond-mat.str-el

Field-dependent Magnons in a Honeycomb Antiferromagnet CoTiO$_3$

We report field-dependent high-resolution inelastic neutron scattering (INS) measurements on the honeycomb lattice magnet, CoTiO$_3$, to study the evolution of its magnon excitations across a spin reorientation transition driven by an in-plane magnetic field. By carrying out elastic neutron scattering in a magnetic field, we show that the sample transitions from a collinear antiferromagnetic state with multiple magnetic domains at a low field to a mono-domain state with a canted magnetic structure at a high field. Concurrent with this transition, we observed significant changes in both the energy and the width of the zone center magnon peak. The observed width change is argued to be consistent with an unusual zero-field state with extended domain walls. On the other hand, the magnon spectra near the $\mathbf{K}$ point of the Brillouin zone boundary are found to be largely insensitive to the changes in the ordered moment directions and the domain configuration. We argue that this observation is difficult to explain within the framework of the bond-dependent model proposed in a recent INS study [Elliot \textit{et\,al}, Nat. Commun., \textbf{12}, 3936 (2021)]. Our study therefore calls for alternative explanations for the observed $\mathbf{K}$-point gap in CoTiO$_3$.

cond-mat.str-el

Robust nodal behavior in the thermal conductivity of superconducting UTe$_2$

The superconducting state of the heavy-fermion metal UTe$_2$ has attracted considerable interest because of evidence for spin-triplet Cooper pairing and non-trivial topology. Progress on these questions requires identifying the presence or absence of nodes in the superconducting gap function and their dimension. In this article we report a comprehensive study of the influence of disorder on the thermal transport in the superconducting state of UTe$_2$. Through detailed measurements of the magnetic field dependence of the thermal conductivity in the zero-temperature limit, we obtain clear evidence for the presence of point nodes in the superconducting gap for all samples with transition temperatures ranging from 1.6~K to 2.1~K obtained by different synthesis methods, including a refined self-flux method. This robustness implies the presence of symmetry-imposed nodes throughout the range studied, further confirmed via disorder-dependent calculations of the thermal transport in a model with a single pair of nodes. In addition to capturing the temperature dependence of the thermal conductivity up to $T_c$, this model allows us to limit the possible locations of the nodes, suggesting a B$_{1u}$ or B$_{2u}$ symmetry for the superconducting order parameter. Additionally, comparing the new, ultra-high conductivity samples to older samples reveals a crossover between a low-field and a high field regime at a single value of the magnetic field in all samples. In the high field regime, the thermal conductivity at different disorder levels differ from each other by a simple offset, suggesting that some simple principle determines the physics of the mixed state, a fact which may illuminate trends observed in other clean nodal superconductors.

cond-mat.supr-con

High-Field Superconducting Halo in UTe$_2$

Heavy fermion UTe$_2$ is a promising candidate for topological superconductivity that also exhibits multiple high-field superconducting phases. The SC$_{\rm{FP}}$ phase has only been observed in off-axis magnetic fields in the $bc$ plane at fields greater than 40 teslas, a striking scale given its critical temperature of only 2 kelvins. Here, we extend measurements of this unique superconducting state outside of the $bc$ plane and reveal its core structure. The SC$_{\rm{FP}}$ phase is not confined to fields in the $bc$ plane and in fact wraps around the $b$ axis in a halo-like fashion. In other words, this superconducting state, which exists in fields above 73 teslas, is stabilized by a field component perpendicular to the magnetic easy axis. These remarkable field scales further underscore UTe$_2$'s unique magnetophilic superconducting tendencies and suggest an underlying pairing mechanism that is qualitatively distinct from known theories for field-enhanced superconductivity. Phenomenological modeling points to a two-component, non-unitary spin triplet order parameter with finite orbital momentum of the Cooper pairs as a natural explanation for the field-angle dependence of the upper critical field of the SC$_{\rm{FP}}$ phase.

cond-mat.supr-con

A review of UTe$_2$ at high magnetic fields

Uranium ditelluride (UTe$_2$) is recognized as a host material to unconventional spin-triplet superconductivity, but it also exhibits a wealth of additional unusual behavior at high magnetic fields. One of the most prominent signatures of the unconventional superconductivity is a large and anisotropic upper critical field that exceeds the paramagnetic limit. This superconductivity survives to 35 T and is bounded by a discontinuous magnetic transition, which itself is also field-direction-dependent. A different, reentrant superconducting phase emerges only on the high-field side of the magnetic transition, in a range of angles between the crystallographic $b$ and $c$ axes. This review discusses the current state of knowledge of these high-field phases, the high-field behavior of the heavy fermion normal state, and other phases that are stabilized by applied pressure.

cond-mat.supr-con