SearcharxivSearch

arXiv subjects

Daniel P. Shoemaker

Publications and source records attributed to Daniel P. Shoemaker.

At least 19 recordsLinked to original sources

High temperature Jahn-Teller distortion and short-range order in CsCuCl$_3$

CsCuCl$_3$, chiral and Jahn-Teller distorted at room temperature, takes a more symmetric structure above 423 K. Describing this 'simpler' high temperature structure is far from simple and has been the subject of many, sometimes contradicting, studies. Here we reinvestigate the high temperature structure of CsCuCl$_3$, its thermal stability, and its effect on room temperature chirality. In situ pair distribution function data from powder neutron diffraction confirms that CsCuCl$_3$ is Jahn-Teller distorted both below and above $T_\mathrm{c}$, and provides a quantitative view of short-range order in the high temperature structure. In situ powder x-ray diffraction shows that CsCuCl$_3$ does not undergo any additional structural changes above 423 K and is congruently melting. In situ single crystal x-ray diffraction experiments reveal that the phase transition induces domains of mixed handedness in originally homochiral crystals. These findings contribute to a better understanding of phase transitions in Jahn-Teller distorted compounds, and highlight the potential use of phase transitions to control chiral domains.

cond-mat.mtrl-sci

Dynamic competition between phason and amplitudon observed by ultrafast multimodal scanning tunneling microscopy

The intertwining between two ordered states that arise from the same interactions is reflected in the dynamics of their coupled collective excitations. While the equilibrium phase diagram resulting from such intertwined orders has been extensively studied, the dynamic competition between non-equilibrium modes is a largely unexplored territory. Here, we introduce a multimodal STM-based pump-probe technique, that combines ultrafast tunneling microscopy (USTM), ultrafast point-contact spectroscopy (UPC), and optical pump-probe reflectance (OPPR) on femtosecond timescale, all within a single instrument. Using this platform, we investigate the collective excitations of the unconventional charge density wave insulator (TaSe4)2I. Our UPC measurements reveal charge oscillations at 0.22 THz, with a temperature dependence that matches the theoretically predicted behavior of the long-sought massive phason gaining mass through the Anderson-Higgs mechanism. Unexpectedly, the data also reveals a second mode at 0.11 THz exhibiting similar temperature and polarization dependence with comparable mode intensity. These features, along with the robust 1/2 frequency ratio locking suggest that the 0.11 THz phason is a 'daughter mode' that arises from the splitting of the 0.22 THz massive phason into two massless phasons via parametric amplification, analogous to the decay of a neutral pion into two photons. Strikingly, comparison with OPPR data reveals that the daughter phason competes with and suppresses the amplitudon at proximate frequency. Our studies reveal an unexplored mechanism for the generation and extinction of collective excitations in quantum materials and pave the way for a microscopic understanding of ultrafast phenomena.

cond-mat.str-el

Applied-field magnetic structure and spectroscopy shifts of the effective spin-$\frac{1}{2}$, $XY$-like magnet Li$_2$CoCl$_4$

Insulators containing chains of magnetic transition metal cations provide platforms for probing spin-$\frac{1}{2}$ dynamics and quantum critical behavior. Li$_2$CoCl$_4$ contains edge-sharing CoCl$_6$ octahedra that form chains along the crystallographic $c$ axis and orders antiferromagnetically at zero field, but questions remain about its applied-field magnetic structure and the Co$^{2+}$ spin state. Here, we show with neutron diffraction on a polycrystalline sample how the anti-aligned chains of cobalt moments begin to transition to a ferromagnetic state above 1.6 T. Further, using magnetic resonance absorption measurements and noninteracting spin models, we reveal the strongly anisotropic nature of the Co$^{2+}$ ion's $XY$-like magnetic behavior ($g_{\parallel}=2.77$ and $g_{\perp}=5.23$) and its $J=\frac{1}{2}$ ground state. We, therefore, supply the magnetic structures and anisotropic description needed to explore the dynamics of the field-driven magnetic phases, laying the foundation for further experimental and theoretical studies.

cond-mat.str-el

Observation of a dynamic magneto-chiral instability in photoexcited tellurium

In a system of charged chiral fermions driven out of equilibrium, an electric current parallel to the magnetic field can generate a dynamic instability by which electromagnetic waves become amplified. Whether a similar instability can occur in chiral solid-state systems remains an open question. Using time-domain terahertz (THz) emission spectroscopy, we detect signatures of what we dub a ``dynamic magneto-chiral instability" in elemental tellurium, a structurally chiral crystal. Upon transient photoexcitation in a moderate external magnetic field, tellurium emits THz radiation consisting of coherent modes that amplify over time. An explanation for this amplification is proposed using a theoretical model based on a dynamic instability of electromagnetic waves interacting with infrared-active oscillators of impurity acceptor states in tellurium to form an amplifying polariton. Our work not only uncovers the presence of a magneto-chiral instability but also highlights its promise for THz-wave amplification in chiral materials.

cond-mat.mes-hall

Narrow optical linewidths in stoichiometric layered rare-earth crystals

Rare-earth emitters in solids are well-suited for implementing efficient, long-lived quantum memory coupled to integrated photonics for scalable quantum technologies. They are typically introduced as dopants in a solid-state host, but this introduces disorder and limits the available density of emitters. Stoichiometric materials can offer high densities with narrow optical linewidths. The regular spacing of emitters also opens possibilities for quantum information processing and collective effects. Here we show narrow optical linewidths in a layered stoichiometric crystalline material, NaEu(IO$_3$)$_4$. We observed an inhomogeneous linewidth of 2.2(1) GHz and a homogeneous linewidth of 120(4) kHz. Using spectral hole-burning techniques, we observe a hyperfine spin lifetime of 1.9(4) s. Furthermore, we demonstrate an atomic frequency comb delay of up to 800 ns.

quant-ph

High-pressure characterization of Ag$_3$AuTe$_2$: Implications for strain-induced band tuning

Recent band structure calculations have suggested the potential for band tuning in a chiral semiconductor, Ag$_3$AuTe$_2$, to zero upon application of negative strain. In this study, we report on the synthesis of polycrystalline Ag$_3$AuTe$_2$ and investigate its transport, optical properties, and pressure compatibility. Transport measurements reveal the semiconducting behavior of Ag$_3$AuTe$_2$ with high resistivity and an activation energy $E_a$ of 0.2 eV. The optical band gap determined by diffuse reflectance measurements is about three times wider than the experimental $E_a$. Despite the difference, both experimental gaps fall within the range of predicted band gaps by our first-principles DFT calculations employing the PBE and mBJ methods. Furthermore, our DFT simulations predict a progressive narrowing of the band gap under compressive strain, with a full closure expected at a strain of -4% relative to the lattice parameter. To evaluate the feasibility of gap tunability at such substantial strain, the high-pressure behavior of Ag$_3$AuTe$_2$ was investigated by $in$ $situ$ high-pressure X-ray diffraction up to 47 GPa. Mechanical compression beyond 4% resulted in a pressure-induced structural transformation, indicating the possibilities of substantial gap modulation under extreme compression conditions.

cond-mat.mtrl-sci

Strong Chirality Suppression in 1-D correlated Weyl Semimetal (TaSe4)2I

The interaction of light with correlated Weyl semimetals (WSMs) provides a unique platform for exploring non-equilibrium phases and fundamental properties such as chirality. Here, we investigate the structural chirality of (TaSe4)2I, a correlated WSM, under weak optical pumping using Circular Photogalvanic Effect (CPGE) measurements and Raman spectroscopy. Surprisingly, we find that there is a loss of chirality in (TaSe4)2I above a threshold light intensity. We suggest that the loss of chirality is due to an optically driven phase transition into an achiral structure distinct from the ground state. This structural transformation is supported by fluence-dependent Raman spectra, revealing a new peak at low pump fluences that disappears above the threshold fluence. The loss of chirality even at low optical powers suggests that the system quickly transitions into a non WSM phase, and also highlights the importance of considering light-induced structural interactions in understanding the behavior of correlated systems. These studies showcase that even low excitation powers can be used to control the properties of correlated topological systems, opening up new avenues for low power optical devices.

cond-mat.mtrl-sci

Synthesis of layered gold tellurides AuSbTe and Au$_2$Te$_3$ and their semiconducting and metallic behavior

Previous studies on natural samples of pampaloite (AuSbTe) revealed the crystal structure of a potentially cleavable and/or exfoliable material, while studies on natural and synthetic montbrayite (Sb-containing Au$_2$Te$_3$) claimed various chemical compositions for this low symmetry compound. Few investigations of synthetic samples have been reported for both materials, leaving much of their chemical, thermal and electronic characteristics unknown. Here, we investigate the stability, electronic properties and synthesis of the gold antimony tellurides AuSbTe and Au$_{1.9}$Sb$_{0.46}$Te$_{2.64}$ (montbrayite). Differential thermal analysis and $\textit{in situ}$ powder x-ray diffraction revealed that AuSbTe is incongruently melting, while Au$_{1.9}$Sb$_{0.46}$Te$_{2.64}$ is congruently melting. Calculations of the band structures and four-point resistivity measurements showed that AuSbTe is a semiconductor and Au$_{1.9}$Sb$_{0.46}$Te$_{2.64}$ a metal. Various synthesis attempts confirmed the limited stable chemical composition of Au$_{1.9}$Sb$_{0.46}$Te$_{2.64}$, identified successful methods to synthesize both compounds, and highlighted the challenges associated with single crystal synthesis of AuSbTe.

cond-mat.mtrl-sci

Magnetic anisotropy in single-crystalline antiferromagnetic Mn$_2$Au

Multiple recent studies have identified the metallic antiferromagnet Mn$_2$Au to be a candidate for spintronic applications due to apparent in-plane anisotropy, preserved magnetic properties above room temperature, and current-induced N\'eel vector switching. Crystal growth is complicated by the fact that Mn$_2$Au melts incongruently. We present a bismuth flux method to grow millimeter-scale bulk single crystals of Mn$_2$Au in order to examine the intrinsic anisotropic electrical and magnetic properties. Flux quenching experiments reveal that the Mn$_2$Au crystals precipitate below 550{\deg}C, about 100{\deg}C below the decomposition temperature of Mn$_2$Au. Bulk Mn$_2$Au crystals have a room-temperature resistivity of 16-19 $\mu\Omega$-cm and a residual resistivity ratio of 41. Mn$_2$Au crystals have a dimensionless susceptibility on the order of 10$^{-4}$, comparable to calculated and experimental reports on powder samples. Single-crystal neutron diffraction confirms the in-plane magnetic structure. The tetragonal symmetry of Mn$_2$Au constrains the $ab$-plane magnetic susceptibility to be constant, meaning that $\chi_{100}=\chi_{110}$ in the low-field limit, below any spin-flop transition. We find that three measured magnetic susceptibilities $\chi_{100}$, $\chi_{110}$, and $\chi_{001}$ are the same order of magnitude and agree with the calculated prediction, meaning the low-field susceptibility of Mn$_2$Au is quite isotropic, despite clear differences in $ab$-plane and $ac$-plane magnetocrystalline anisotropy. Mn$_2$Au is calculated to have an extremely high in-plane spin-flop field above 30 T, which is much larger than that of another in-plane antiferromagnet Fe$_2$As (less than 1 T). The subtle anisotropy of intrinsic susceptibilities may lead to dominating effects from shape, crystalline texture, strain, and defects in devices that attempt spin readout in Mn$_2$Au.

cond-mat.mtrl-sci

Disorder and diffuse scattering in single-chirality (TaSe$_4$)$_2$I crystals

The quasi-one-dimensional chiral compound (TaSe$_4$)$_2$I has been extensively studied as a prime example of a topological Weyl semimetal. Upon crossing its phase transition temperature $T_\textrm{CDW}$ $\approx$ 263 K, (TaSe$_4$)$_2$I exhibits incommensurate charge density wave (CDW) modulations described by the well-defined propagation vector $\sim$(0.05, 0.05, 0.11), oblique to the TaSe$_4$ chains. Although optical and transport properties greatly depend on chirality, there is no systematic report about chiral domain size for (TaSe$_4$)$_2$I. In this study, our single-crystal scattering refinements reveal a bulk iodine deficiency, and Flack parameter measurements on multiple crystals demonstrate that separate (TaSe$_4$)$_2$I crystals have uniform handedness, supported by direct imaging and helicity dependent THz emission spectroscopy. Our single-crystal X-ray scattering and calculated diffraction patterns identify multiple diffuse features and create a real-space picture of the temperature-dependent (TaSe$_4$)$_2$I crystal structure. The short-range diffuse features are present at room temperature and decrease in intensity as the CDW modulation develops. These transverse displacements, along with electron pinning from the iodine deficiency, help explain why (TaSe$_4$)$_2$I behaves as an electronic semiconductor at temperatures above and below $T_\textrm{CDW}$, despite a metallic band structure calculated from density functional theory of the ideal structure.

cond-mat.str-el

Zero-field magnetic structure and metamagnetic phase transitions of the cobalt chain compound Li$_2$CoCl$_4$

Exploring the uncharacterized magnetic phases of Co$^{2+}$ chain compounds is critical for finding new low-dimensional magnets hosting quantized excitations. We map the unexplored magnetic phases of the Co$^{2+}$ chain compound Li$_2$CoCl$_4$. Magnetometry reveals magnetic ordering below 7 K with a metamagnetic transition near 16.5 kOe and a gradual transition to a field-aligned paramagnetic state above 31 kOe. Curie-Weiss fits to the high temperature susceptibility reveal a high-spin (spin-$\frac{3}{2}$) state for cobalt. Heat capacity data, though, give a magnetic entropy change of 5.46 J/mol, consistent with cobalt effective spin-$\frac{1}{2}$ systems. To characterize the zero-field antiferromagnetic ordering, we separately calculated the energy of proposed magnetic structures with density functional theory and collected 3.5 K neutron diffraction data, finding that Li$_2$CoCl$_4$ has ferromagnetic chains with antiferromagnetic interactions between them. Increasing field rotates these spin chains, producing the antiferromagnetic to intermediate to paramagnetic transition sequence.

cond-mat.str-el

Angstrom-Scale Imaging of Magnetization in Antiferromagnetic Fe$_2$As via 4D-STEM

We demonstrate a combination of computational tools and experimental 4D-STEM methods to image the local magnetic moment in antiferromagnetic Fe$_2$As with 6 angstrom spatial resolution. Our techniques utilize magnetic diffraction peaks, common in antiferromagnetic materials, to create imaging modes that directly visualize the magnetic lattice. Using this approach, we show that center-of-mass analysis can determine the local magnetization component in the plane perpendicular to the path of the electron beam. Moreover, we develop Magnstem, a quantum mechanical electron scattering simulation code, to model electron scattering of an angstrom-scale probe from magnetic materials. Using these tools, we identify optimal experimental conditions for separating weak magnetic signals from the much stronger interactions of an angstrom-scale probe with electrostatic potentials. Our techniques should be useful for characterizing the local magnetic order in systems such in thin films, interfaces, and domain boundaries of antiferromagnetic materials, which are difficult to probe with existing methods.

cond-mat.mtrl-sci

Ultrafast x-ray scattering reveals composite amplitude collective mode in the Weyl charge density wave material (TaSe$_4$)$_2$I

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe$_4$)$_2$I following photoexcitation with femtosecond infrared laser pulses. From the time-dependent diffraction signal at the CDW sidebands we identify an amplitude mode derived primarily from the transverse acoustic component of the CDW static distortion. The dynamics of this acoustic amplitude mode are described well by a model of a displacive excitation, which we interpret as mediated through a coupling to the optical phonon component associated with the tetramerization of the Ta chains.

cond-mat.mtrl-sci

Observation of the massive Lee-Fukuyama phason in a charge density wave insulator

The lowest-lying fundamental excitation of an incommensurate charge density wave (CDW) material is widely believed to be a massless phason -- a collective modulation of the phase of the CDW order parameter. However, as first pointed out by Lee and Fukuyama, long-range Coulomb interactions should push the phason energy up to the plasma energy of the CDW condensate, resulting in a massive phason and a fully gapped spectrum. Whether such behavior occurs in a CDW system has been unresolved for more than four decades. Using time-domain THz emission spectroscopy, we investigate this issue in the material (TaSe$_4$)$_2$I, a classical example of a quasi-one-dimensional CDW insulator. Upon transient photoexcitation at low temperatures, we find the material strikingly emits coherent, narrow-band THz radiation. The frequency, polarization and temperature-dependence of the emitted radiation imply the existence of a phason that acquires mass by coupling to long-range Coulomb interaction. Our observations constitute the first direct evidence of the massive "Lee-Fukuyama" phason and highlight the potential applicability of fundamental collective modes of correlated materials as compact and robust sources of THz radiation.

cond-mat.str-el

A new quasi-one-dimensional transition metal chalcogenide semiconductor (Nb$_4$Se$_{15}$I$_2$)I$_2$

The discovery of new low-dimensional transition metal chalcogenides is contributing to the already prosperous family of these materials. In this study, needle-shaped single crystals of a new quasi-one-dimensional material (Nb$_4$Se$_{15}$I$_2$)I$_2$ were grown by chemical vapor transport, and the structure was solved by single crystal X-ray diffraction (XRD). The new structure has one-dimensional (Nb$_4$Se$_{15}$I$_2$)$_n$ chains along the [101] direction, with two I$^-$ ions per formula unit directly bonded to Nb$^{5+}$. The other two I$^-$ ions are loosely coordinated and intercalate between the chains. Individual chains are chiral, and stack along the $b$ axis in opposing directions, giving space group $P2_1/c$. The phase purity and crystal structure was verified by powder XRD. Density functional theory calculations show (Nb$_4$Se$_{15}$I$_2$)I$_2$ to be a semiconductor with a direct band gap of around 0.6 eV. Resistivity measurements of bulk crystals and micro-patterned devices demonstrate that (Nb$_4$Se$_{15}$I$_2$)I$_2$ has an activation energy of around 0.1 eV, and no anomaly or transition was seen upon cooling. (Nb$_4$Se$_{15}$I$_2$)I$_2$ does not undergo structural phase transformation from room temperature down to 8.2 K, based on cryogenic temperature single crystal XRD. This compound represents a well-characterized and valence-precise member of a diverse family of anisotropic transition metal chalcogenides.

cond-mat.mtrl-sci

Spin-Resolved Topology and Partial Axion Angles in Three-Dimensional Insulators

Symmetry-protected topological crystalline insulators (TCIs) have primarily been characterized by their gapless boundary states. However, in time-reversal- ($\mathcal{T}$-) invariant (helical) 3D TCI$\unicode{x2014}$termed higher-order TCIs (HOTIs)$\unicode{x2014}$the boundary signatures can manifest as a sample-dependent network of 1D hinge states. We here introduce nested spin-resolved Wilson loops and layer constructions as tools to characterize the intrinsic bulk topological properties of spinful 3D insulators. We discover that helical HOTIs realize one of three spin-resolved phases with distinct responses that are quantitatively robust to large deformations of the bulk spin-orbital texture: 3D quantum spin Hall insulators (QSHIs), "spin-Weyl" semimetals, and $\mathcal{T}$-doubled axion insulator (T-DAXI) states with nontrivial partial axion angles indicative of a 3D spin-magnetoelectric bulk response and half-quantized 2D TI surface states originating from a partial parity anomaly. Using ab-initio calculations, we demonstrate that $\beta$-MoTe$_2$ realizes a spin-Weyl state and that $\alpha$-BiBr hosts both 3D QSHI and T-DAXI regimes.

cond-mat.mes-hall

Tuning cryogenic Jahn-Teller transition temperatures in magnetoelectric rare earth vanadates

Few materials undergo cooperative Jahn-Teller (JT) transitions at low temperatures, but zircon-type oxides are one class that includes DyVO$_4$, which transforms from a tetragonal to an orthorhombic structure at around 13.6 K, with a narrow transition temperature range within 0.5 K. Since many rare-earth ions can be accommodated in the structure, there should be ample routes to vary the transition temperature and structural effects of the transition. We have synthesized pure DyVO$_4$ and solid solutions Dy$_{1-x}$Tm$_x$VO$_4$ ($x$ = 0.05, 0.1, 0.15, 0.2, and 0.5) and Dy$_{1-y}$Pr$_y$VO$_4$ ($y$ = 0.03, 0.05, 0.1, 0.2, and 0.5), all by solution precipitation. X-ray diffraction shows a systematic peak shift and a linear change of lattice parameters with increasing substitution. We demonstrate through heat capacity measurements that both Tm$^{3+}$ and Pr$^{3+}$ substitutions cause a depression of the cooperative JT transition temperature. When the substitution level increases, the JT transition is eventually suppressed. We examine a mean-field approximation model that can explain the both the JT transition temperature shift and its eventual disappearance. The cooperative JT effect in these zircon-type oxides is known to exhibit a large magnetoelectric response, which should follow from the mean-field behavior. The structural transformation can be easily detected via diffraction and can be used as a temperature calibration in low temperature experiments.

cond-mat.mtrl-sci

High-resolution diffraction reveals magnetoelastic coupling and coherent phase separation in tetragonal CuMnAs

Tetragonal CuMnAs was the first antiferromagnet where reorientation of the N\'eel vector was reported to occur by an inverse spin galvanic effect. A complicating factor in the formation of phase-pure tetragonal CuMnAs is the formation of an orthorhombic phase with nearly the same stoichiometry. Pure-phase tetragonal CuMnAs has been reported to require an excess of Cu to maintain a single phase in traditional solid state synthesis reactions. Here we show that subtle differences in diffraction patterns signal pervasive inhomogeneity and phase separation, even in Cu-rich Cu$_{1.18}$Mn$_{0.82}$As. From calorimetry and magnetometry measurements, we identify two transitions corresponding to the N\'eel temperature (T$_N$) and an antiferromagnet to weak ferromagnet transition in Cu$_{1.18}$Mn$_{0.82}$As and CuMn$_{0.964}$As$_{1.036}$. These transitions have clear crystallographic signatures, directly observable in the lattice parameters upon in-situ heating and cooling. The immiscibility and phase separation could arise from a spinoidal decomposition that occurs at high temperatures, and the presence of a ferromagnetic transition near room temperature warrants further investigation of its effect on the electrical switching behavior.

cond-mat.mtrl-sci