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Stephen D. Wilson

Publications and source records attributed to Stephen D. Wilson.

At least 145 records · Page 8Linked to original sources

Band Splitting and Long-lived Carrier Recombination in Ferromagnetic CrSiTe3 Nanosheets

Magnetic layered ternary chalcogenides hold great promise for future spin-optoelectronic devices in the two dimensional limit. Understanding how the properties of the materials are impacted by magnetic ordering and the spin-orbit interactions is critically needed information for the development of applications. Ultrafast transient reflectance (TR) and photocurrent (PC) spectroscopies are combined with ab initio density functional theory (DFT) calculations to investigate the band structure and photoresponse of a layered magnetic semiconductor CrSiTe3 (CST) nanosheet in the paramagnetic (PM, 300K) and ferromagnetic (FM, 10 K) phases. We observe both a decrease of the direct bandgap and emergence of a 120 meV splitting of the optical transition when the FM phase is present. DFT band structure calculations suggest that the band modifications are driven by a FM ordering-induced band splitting between the Te p and the Cr d states at the valence and conduction band edges. We find that the majority of carriers photoexcited at the direct gap recombine within picoseconds through defect-mediated recombination, but that 2-3 % of the electrons scatter into indirect conduction band valleys resulting in very long-lived electrons and holes. Those long-lived carriers contribute to the broadband PC response of CST devices that also features indirect absorption. These results provide critical insights into the dynamics and energy landscape of photoexcited electrons and holes, and how they are impacted by spin-ordering effects in layered ferromagnets.

cond-mat.mtrl-sci↗

Superconductivity modulated by structural phase transitions in pressurized vanadium-based kagome metals

The interplay of superconductivity with electronic and structural instabilities on the kagome lattice provides a fertile ground for the emergence of unusual phenomena. The vanadium-based kagome metals $A$V$_3$Sb$_5$ ($A=$ K, Rb, Cs) exhibit superconductivity on an almost ideal kagome lattice, with the superconducting transition temperature $T_{\rm c}$ forming two domes upon pressure-tuning. The first dome arises from the competition between superconductivity and a charge-density-wave, whereas the origin for the second dome remains unclear. Herein, we show that the appearance of the second superconducting dome in KV$_3$Sb$_5$ and RbV$_3$Sb$_5$ is associated with transitions from hexagonal $P6$/$mmm$ to monoclinic $P2$/$m$ structures, evidenced by splitting of structural peaks from synchrotron powder X-ray diffraction experiments and imaginary phonon frequencies in first-principles calculations. In KV$_3$Sb$_5$, transition to an orthorhombic $Pmmm$ structure is further observed for pressure $p\gtrsim20$ GPa, and is correlated with the strong suppression of $T_{\rm c}$ in the second superconducting dome. Our findings indicate distortions of the crystal structure modulates superconductivity in $A$V$_3$Sb$_5$ under pressure, providing a platform to study the emergence of superconductivity in the presence of multiple structural instabilities.

cond-mat.supr-con↗

Kagome superconductors AV$_3$Sb$_5$ (A=K, Rb, Cs)

The quasi two-dimensional (quasi-2D) kagome materials AV$_3$Sb$_5$ (A=K, Rb, Cs) were found to be a prime example of kagome superconductors, a new quantum platform to investigate the interplay between electron correlation effects, topology and geometric frustration. In this review, we report recent progress on the experimental and theoretical studies of AV$_3$Sb$_5$ and provide a broad picture of this fast-developing field in order to stimulate an expanded search for unconventional kagome superconductors. We review the electronic properties of AV$_3$Sb$_5$, the experimental measurements of the charge density wave state, evidence of time-reversal symmetry breaking, and other potential hidden symmetry breaking in these materials. A variety of theoretical proposals and models that address the nature of the time-reversal symmetry breaking are discussed. Finally, we review the superconducting properties of AV$_3$Sb$_5$, especially the potential pairing symmetries and the interplay between superconductivity and the charge density wave state.

cond-mat.supr-con↗

Magnetic properties and signatures of moment ordering in triangular lattice antiferromagnet KCeO$_2$

The magnetic ground state and the crystalline electric field level scheme of the triangular lattice antiferromagnet KCeO$_2$ are investigated. Below $T_N =$ 300 mK, KCeO$_2$ develops signatures of magnetic order in specific heat measurements and low energy inelastic neutron scattering data. Trivalent Ce$^{3+}$ ions in the $D_{3d}$ local environment of this compound exhibit large splittings among the lowest three $4f^1$ Kramers doublets defining for the free ion the $J = 5/2$ sextet and a ground state doublet with dipole character, consistent with recent theoretical predictions in M. S. Eldeeb et al. Phys. Rev. Materials 4, 124001 (2020). An unexplained, additional local mode appears, and potential origins of this anomalous mode are discussed.

cond-mat.str-el↗

Evaluating the Effects of Structural Disorder on the Magnetic Properties of Nd$_{2}$Zr$_{2}$O$_{7}$

Motivated by the variation in reported lattice parameters of floating-zone-grown Nd$_{2}$Zr$_{2}$O$_{7}$ crystals, we have performed a detailed study of the relationship between synthesis environment, structural disorder, and magnetic properties. Using a combination of polycrystalline standards, electron-probe microanalysis and scattering techniques, we show that crystals grown under atmospheric conditions have a reduced lattice parameter - relative to pristine polycrystalline powders - due to occupation of the Nd-site by excess Zr (i.e. "negative" stuffing). In contrast, crystals grown under high-pressure Ar are nearly stoichiometric with an average lattice parameter approaching the polycrystalline value. While minimal disorder of the oxygen sublattices is observed on the scale of the average structure, neutron pair-distribution function analysis indicates a highly local disorder of the oxygen coordination, which is only weakly dependent on growth environment. Most importantly, our magnetization, heat capacity and single-crystal neutron scattering data show that the magnetic properties of crystals grown under high-pressure Ar match closely with those of stoichiometric powders. Neutron scattering measurements reveal that the signature of magnetic moment fragmentation - the coexistence of all-in-all-out (AIAO) magnetic Bragg peaks and diffuse pinch-point scattering due to spin-ice correlations - persists in these nearly stoichiometric crystals. However, in addition to an increased AIAO transition temperature, the diffuse signal is seemingly stabilized and remains nearly unchanged upon warming to 800 mK. This behavior indicates that both the AIAO magnetic order and spin-ice correlations are sensitive to deviations of the Nd stoichiometry.

cond-mat.mtrl-sci↗

Intrinsic nature of chiral charge order in the kagome superconductor RbV3Sb5

Superconductors with kagome lattices have been identified for over 40 years, with a superconducting transition temperature TC up to 7K. Recently, certain kagome superconductors have been found to exhibit an exotic charge order, which intertwines with superconductivity and persists to a temperature being one order of magnitude higher than TC. In this work, we use scanning tunneling microscopy (STM) to study the charge order in kagome superconductor RbV3Sb5. We observe both a 2x2 chiral charge order and nematic surface superlattices (predominantly 1x4). We find that the 2x2 charge order exhibits intrinsic chirality with magnetic field tunability. Defects can scatter electrons to introduce standing waves, which couple with the charge order to cause extrinsic effects. While the chiral charge order resembles that discovered in KV3Sb5, it further interacts with the nematic surface superlattices that are absent in KV3Sb5 but exist in CsV3Sb5.

cond-mat.str-el↗

Magnetoentropic mapping and computational modeling of cycloids and skyrmions in the lacunar spinels GaV$_4$S$_8$ and GaV$_4$Se$_8$

We report the feasibility of using magnetoentropic mapping for the rapid identification of magnetic cycloid and skyrmion phases in uniaxial systems, based on the GaV4S8 and GaV4Se8 model skyrmion hosts with easy-axis and easy-plane anisotropies respectively. We show that these measurements can be interpreted with the help of a simple numerical model for the spin Hamiltonian to yield unambiguous assignments for both single phase regions and phase boundaries. In the two lacunar spinel chemistries, we obtain excellent agreement between the measured magnetoentropic features and a minimal spin Hamiltonian built on Heisenberg exchange, single-ion anisotropy, and anisotropic Dzyaloshinskii-Moriya interactions. In particular, we identify characteristic high-entropy behavior in the cycloid phase that serves as a precursor to the formation of skyrmions at elevated temperatures and is a readily-measurable signature of this phase transition. Our results demonstrate that rapid magnetoentropic mapping guided by numerical modeling is an effective means of understanding the complex magnetic phase diagrams innate to skyrmion hosts. One notable exception is the observation of an anomalous, low-temperature high-entropy state in the easy-plane system GaV$_4$Se$_8$, which is not captured in the numerical model. Possible origins of this state are discussed.

cond-mat.str-el↗

Strain-sensitive superconductivity in kagome metals KV$_3$Sb$_5$ and CsV$_3$Sb$_5$ probed by point-contact spectroscopy

The kagome lattice is host to flat bands, topological electronic structures, Van Hove singularities and diverse electronic instabilities, providing an ideal platform for realizing highly tunable electronic states. Here, we report soft- and mechanical- point-contact spectroscopy (SPCS and MPCS) studies of the kagome superconductors KV$_3$Sb$_5$ and CsV$_3$Sb$_5$. Compared to the superconducting transition temperature $T_{\rm c}$ from specific heat measurements (2.8~K for CsV$_3$Sb$_5$ and 1.0~K for KV$_3$Sb$_5$), significantly enhanced values of $T_{\rm c}$ are observed via the zero-bias conductance of SPCS ($\sim$4.2~K for CsV$_3$Sb$_5$ and $\sim$1.8~K for KV$_3$Sb$_5$), which become further enhanced in MPCS measurements ($\sim$5.0~K for CsV$_3$Sb$_5$ and $\sim$3.1~K for KV$_3$Sb$_5$). While the differential conductance curves from SPCS are described by a two-gap $s$-wave model, a single $s$-wave gap reasonably captures the MPCS data, likely due to a diminishing spectral weight of the other gap. The enhanced superconductivity probably arises from local strain caused by the point-contact, which also leads to the evolution from two-gap to single-gap behaviors in different point-contacts. Our results demonstrate highly strain-sensitive superconductivity in kagome metals CsV$_3$Sb$_5$ and KV$_3$Sb$_5$, which may be harnessed in the manipulation of possible Majorana zero modes.

cond-mat.supr-con↗

Visualizing nematic transition and nanoscale suppression of superconductivity in Fe(Te,Se)

The interplay of different electronic phases underlies the physics of unconventional superconductors. One of the most intriguing examples is a high-Tc superconductor FeTe1-xSex: it undergoes both a topological transition, linked to the electronic band inversion, and an electronic nematic phase transition, associated with rotation symmetry breaking, around the same critical composition xc where superconducting Tc peaks. At this regime, nematic fluctuations and symmetry-breaking strain could have an enormous impact, but this is yet to be fully explored. Using spectroscopic-imaging scanning tunneling microscopy, we study the electronic nematic transition in FeTe1-xSex as a function of composition. Near xc, we reveal the emergence of electronic nematicity in nanoscale regions. Interestingly, we discover that superconductivity is drastically suppressed in areas where static nematic order is the strongest. By analyzing atomic displacement in STM topographs, we find that small anisotropic strain can give rise to these strongly nematic localized regions. Our experiments reveal a tendency of FeTe1-xSex near x~0.45 to form puddles hosting static nematic order, suggestive of nematic fluctuations pinned by structural inhomogeneity, and demonstrate a pronounced effect of anisotropic strain on superconductivity in this regime.

cond-mat.supr-con↗

Distinct band reconstructions in kagome superconductor CsV$_3$Sb$_5$

The new two-dimensional (2D) kagome superconductor CsV$_3$Sb$_5$ has attracted much recent attention due to the coexistence of superconductivity, charge order, topology and kagome physics. A key issue in this field is to unveil the unique reconstructed electronic structure, which successfully accommodates different orders and interactions to form a fertile ground for emergent phenomena. Here, we report angle-resolved photoemission spectroscopy (ARPES) evidence for two distinct band reconstructions in CsV$_3$Sb$_5$. The first one is characterized by the appearance of new electron energy band at low temperature. The new band is theoretically reproduced when the three dimensionality of the charge order is considered for a band-folding along the out-of-plane direction. The second reconstruction is identified as a surface induced orbital-selective shift of the electron energy band. Our results provide the first evidence for the three dimensionality of the charge order in single-particle spectral function, highlighting the importance of long-range out-of-plane electronic correlations in this layered kagome superconductor. They also point to the feasibility of orbital-selective control of the band structure via surface modification, which would open a new avenue for manipulating exotic phenomena in this system, including superconductivity.

cond-mat.str-el↗

Imaging antiferromagnetic domain fluctuations and the effect of atomic-scale disorder in a doped spin-orbit Mott insulator

Correlated oxides can exhibit complex magnetic patterns, characterized by domains with vastly different size, shape and magnetic moment spanning the material. Understanding how magnetic domains form in the presence of chemical disorder and their robustness to temperature variations has been of particular interest, but atomic-scale insight into this problem has been limited. We use spin-polarized scanning tunneling microscopy to image the evolution of spin-resolved modulations originating from antiferromagnetic (AF) ordering in a spin-orbit Mott insulator Sr3Ir2O7 as a function of chemical composition and temperature. We find that replacing only several percent of La for Sr leaves behind nanometer-scale AF puddles clustering away from La substitutions preferentially located in the middle SrO layer within the unit cell. Thermal erasure and re-entry into the low-temperature ground state leads to a spatial reorganization of the AF modulations, indicating multiple stable AF configurations at low temperature. Interestingly, regardless of this rearrangement, the AF puddles maintain scale-invariant fractal geometry in each configuration. Our experiments reveal spatial fluctuations of the AF order in electron doped Sr3Ir2O7, and shed light on its sensitivity to different types of atomic-scale disorder.

cond-mat.str-el↗

Interplay between charge order and superconductivity in the kagome metal KV$_3$Sb$_5$

The kagome metal KV$_3$Sb$_5$ hosts charge order, topologically nontrivial Dirac band crossings, and a superconducting ground state with unconventional characteristics, providing an ideal platform to investigate the interplay between different electronic states on the kagome lattice. Here we study the evolution of charge order and superconductivity in KV$_3$Sb$_5$ under hydrostatic pressure using electrical resistivity measurements. With the application of pressure, the superconducting transition temperature $T_{\rm c}=0.9$ K under ambient pressure quickly increases to 3.1 K at $p=0.4$ GPa, as charge order progressively weakens. Upon further increasing pressure, signatures of charge order disappears at $p_{\rm c1}\approx0.5$ GPa and $T_{\rm c}$ is gradually suppressed, forming a superconducting dome that terminates at $p\approx10$ GPa. Beyond $p\approx10$ GPa, a second superconducting dome emerges with maximum $T_{\rm c}\approx1.0$ K at $p_{\rm c2}\approx22$ GPa, which becomes fully suppressed at $p\approx28$ GPa. The suppression of superconductivity for the second superconducting dome is associated with the appearance of a unique high-pressure phase , possibly a distinct charge order.

cond-mat.supr-con↗

Discovery of unconventional chiral charge order in kagome superconductor KV3Sb5

Intertwining quantum order and nontrivial topology is at the frontier of condensed matter physics. A charge density wave (CDW) like order with orbital currents has been proposed as a powerful resource for achieving the quantum anomalous Hall effect in topological materials and for the hidden phase in cuprate high-temperature superconductors. However, the experimental realization of such an order is challenging. Here we use high-resolution scanning tunnelling microscopy (STM) to discover an unconventional charge order in a kagome material KV3Sb5, with both a topological band structure and a superconducting ground state. Through both topography and spectroscopic imaging, we observe a robust 2x2 superlattice. Spectroscopically, an energy gap opens at the Fermi level, across which the 2x2 charge modulation exhibits an intensity reversal in real-space, signaling charge ordering. At impurity-pinning free region, the strength of intrinsic charge modulations further exhibits chiral anisotropy with unusual magnetic field response. Theoretical analysis of our experiments suggests a tantalizing unconventional chiral CDW in the frustrated kagome lattice, which can not only lead to large anomalous Hall effect with orbital magnetism, but also be a precursor of unconventional superconductivity.

cond-mat.supr-con↗

Rotation symmetry breaking in the normal state of a kagome superconductor KV3Sb5

Recently discovered kagome superconductors AV3Sb5 (A=K, Rb, Cs) provide a fresh opportunity to realize and study correlation-driven electronic phenomena on a kagome lattice. The observation of a 2a0 by 2a0 charge density wave (CDW) in the normal state of all members of AV3Sb5 kagome family has generated an enormous amount of interest, in an effort to uncover the nature of this CDW state, and identify any "hidden" broken symmetries. We use spectroscopic-imaging scanning tunneling microscopy to reveal a pronounced intensity anisotropy between different 2a0 CDW directions in KV3Sb5. In particular, by examining the strength of ordering wave vectors as a function of energy in Fourier transforms of differential conductance maps, we find that one of the CDW directions is distinctly different compared to the other two. This observation points towards an intrinsic rotation symmetry broken electronic ground state, where the symmetry is reduced from C6 to C2. Furthermore, in contrast to previous reports, we find that the CDW phase is insensitive to magnetic field direction, regardless of the presence or absence of atomic defects. Our experiments, combined with earlier observations of a stripe 4a0 charge ordering in CsV3Sb5, establish correlation-driven rotation symmetry breaking as a unifying feature of AV3Sb5 kagome superconductors.

cond-mat.supr-con↗

Charge-order-assisted topological surface states and flat bands in the kagome superconductor CsV$_3$Sb$_5$

The diversity of emergent phenomena in quantum materials often arises from the interplay between different physical energy scales or broken symmetries. Cooperative interactions among them are rare; however, when they do occur, they often stabilize fundamentally new ground states or phase behaviors. For instance, a pair density wave can form when the superconducting order parameter borrows spatial periodical variation from charge order; a topological superconductor can arise when topologically nontrivial electronic states proximitize with or participate in the formation of the superconducting condensate. Here, we report spectroscopic evidence for a unique synergy of topology and correlation effects in the kagome superconductor CsV$_3$Sb$_5$ - one where topologically nontrivial surface states are pushed below the Fermi energy (E$_F$) by charge order, making the topological physics active near E$_F$ upon entering the superconducting state. Flat bands are observed, indicating that electron correlation effects are also at play in this system. Our results reveal the peculiar electronic structure of CsV$_3$Sb$_5$, which holds the potential for realizing Majorana zero modes and anomalous superconducting states in kagome lattices. They also establish CsV$_3$Sb$_5$ as a unique platform for exploring the cooperation between the charge order, topology, correlation effects and superconductivity.

cond-mat.supr-con↗

Bulk superconductivity in FeTe$_{1-x}$Se$_{x}$ via physicochemical pumping of excess iron

The iron-based superconductor FeTe$_{1-x}$Se$_{x}$ has attracted considerable attention as a candidate topological superconductor owing to a unique combination of topological surface states and bulk high-temperature superconductivity. The superconducting properties of as-grown single crystals, however, are highly variable and synthesis dependent due to excess interstitial iron impurities incorporated during growth. Here we report a novel physicochemical process for pumping this interstitial iron out of the FeTe$_{1-x}$Se$_{x}$ matrix and achieving bulk superconductivity. Our method should have significant value for the synthesis of high-quality single crystals of FeTe$_{1-x}$Se$_{x}$ with large superconducting volume fractions.

cond-mat.supr-con↗

Coherent phonon spectroscopy and interlayer modulation of charge density wave order in the kagome metal CsV$_3$Sb$_5$

The recent discovery of the $A$V$_3$Sb$_5$ ($A=$ K, Rb, Cs) material family offers an exciting opportunity to investigate the interplay of correlations, topology, and superconductivity in kagome metals. The low energy physics of these materials is dominated by an unusual charge density wave phase, but little is understood about the true nature of the order parameter. In this work, we use a combination of ultrafast coherent phonon spectroscopy and first-principles density functional theory calculations to investigate the charge density wave order in CsV$_3$Sb$_5$. We find that the charge density wave is the result of a simultaneous condensation of three optical phonon modes at one $M$ and two $L$ points. This distortion can be described as tri-hexagonal ordering with an interlayer modulation along the $c$ axis. It breaks the $C_6$ rotational symmetry of the crystal and may offer a natural explanation for reports of uniaxial order at lower temperatures in this material family.

cond-mat.str-el↗

Nodeless superconductivity in the kagome metal CsV$_3$Sb$_5$

The recently discovered kagome metal series $A$V$_3$Sb$_5$ ($A$=K, Rb, Cs) exhibits topologically nontrivial band structures, chiral charge order and superconductivity, presenting a unique platform for realizing exotic electronic states. The nature of the superconducting state and the corresponding pairing symmetry are key questions that demand experimental clarification. Here, using a technique based on the tunneling diode oscillator, the magnetic penetration depth $Δλ(T)$ of CsV$_3$Sb$_5$ was measured down to 0.07 K. A clear exponential behavior in $Δλ(T)$ with marked deviations from a $T$ or $T^2$ temperature dependence is observed at low temperatures, indicating a deficiency of nodal quasiparticles. Temperature dependence of the superfluid density and electronic specific heat can be described by two-gap $s$-wave superconductivity, consistent with the presence of multiple Fermi surfaces in CsV$_3$Sb$_5$. These results evidence nodeless superconductivity in CsV$_3$Sb$_5$ under ambient pressure, and constrain the allowed pairing symmetry.

cond-mat.supr-con↗