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Simon Bettler

Publications and source records attributed to Simon Bettler.

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Tuning Incommensurate Charge Order in Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$

The BaAl$_4$-type structure family is home to a vast landscape of interesting and exotic properties, with descendant crystal structures hosting a variety of electronic ground states including magnetic, superconducting and strongly correlated electron phenomena. BaAl$_4$ itself hosts a non-trivial topological band structure, but is otherwise a paramagnetic metal. However, the other members of the $A$Al$_4$ family ($A$= alkali earth), including SrAl$_4$ and EuAl$_4$, exhibit symmetry-breaking ground states including charge density wave (CDW) and magnetic orders. Here we investigate the properties of the solid solution series Ba$_{1-x}$Sr$_x$Al$_4$ and Ba$_{1-y}$Eu$_y$Al$_4$ using transport, thermodynamic and scattering experiments to study the evolution of the charge-ordered state as it is suppressed with Ba substitution to zero near 50% substitution in both systems. Neutron and x-ray diffraction measurements reveal an incommensurate CDW state in SrAl$_4$ with $c$-axis-oriented ordering vector (0, 0, 0.097) that evolves with Ba substitution toward a shorter wavelength. A similar progression is observed in the Ba$_{1-y}$Eu$_y$Al$_4$ series that also scales with the ordering temperature, revealing a universal correlation between charge-order transition temperature and ordering vector that points to a critical wavevector that stabilizes CDW order in both systems. We study the evolution of the phonon band structure in the Ba$_{1-x}$Sr$_x$Al$_4$ system, revealing the suppression of the CDW phase matches the suppression of a phonon instability at precisely the same momentum as observed in experiments, confirming the electron-phonon origin of charge order in this system.

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

Consistency between reflection M-EELS and optical spectroscopy measurements of the long-wavelength density response of Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$

The density fluctuation spectrum captures many fundamental properties of strange metals. Using momentum-resolved electron energy-loss spectroscopy (M-EELS), we recently showed that the density response of the strange metal Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi-2212) at large momentum, $q$, exhibits a constant-in-frequency continuum [Mitrano, PNAS $\textbf{115}$, 5392 (2018); Husain, PRX $\textbf{9}$, 041062 (2019)] reminiscent of the marginal Fermi liquid (MFL) hypothesis of the late 1980s [Varma, PRL $\textbf{63}$, 1996 (1989)]. However, reconciling this observation with infrared (IR) optics experiments, which show a well-defined plasmon excitation at $q \sim 0$, has been challenging. Here we report M-EELS measurements of Bi-2212 using 4$\times$ improved momentum resolution, allowing us to reach the optical limit. For momenta $q<0.04$ r.l.u., the M-EELS data show a plasmon feature that is quantitatively consistent with IR optics. For $q>0.04$ r.l.u., the spectra become incoherent with an MFL-like, constant-in-frequency form. We speculate that, at finite frequency, $ω$, and nonzero $q$, some attribute of this Planckian metal randomizes the probe electron, causing it to lose information about its own momentum.

cond-mat.str-el

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

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

Anharmonic multiphonon origin of the valence plasmon in SrTi1-xNbxO3

Doped SrTi1-xNbxO3 exhibits superconductivity and a mid-infrared optical response reminiscent of copper-oxide superconductors. Strangely, its plasma frequency, omega_p, increases by a factor of ~3 when cooling from 300 K to 20 K, without any accepted explanation. Here, we present momentum-resolved electron energy loss spectroscopy (M-EELS) measurements of SrTi1-xNbxO3 at nonzero momentum, q. We find that the infrared feature previously identified as a plasmon is present at large q in insulating SrTiO3, where it exhibits the same temperature dependence and may be identified as an anharmonic, multiphonon background. Doping with Nb increases its peak energy and total spectral weight, drawing this background to lower q where it becomes visible in IR optics experiments. We conclude that the "plasmon" in doped SrTi1-xNbxO3 is not a free-carrier mode, but a composite excitation that inherits its unusual properties from the lattice anharmonicity of the insulator.

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

Transport and optical properties of the chiral semiconductor Ag3AuSe2

Previous band structure calculations predicted Ag3AuSe2 to be a semiconductor with a band gap of approximately 1 eV. Here, we report single crystal growth of Ag3AuSe2 and its transport and optical properties. Single crystals of Ag3AuSe2 were synthesized by slow-cooling from the melt, and grain sizes were confirmed to be greater than 2 mm using electron backscatter diffraction. Optical and transport measurements reveal that Ag3AuSe2 is a highly resistive semiconductor with a band gap of and activation energy around 0.3 eV. Our first-principles calculations show that the experimentally-determined band gap lies between the predicted band gaps from GGA and hybrid functionals. We predict band inversion to be possible by applying tensile strain. The sensitivity of the gap to Ag/Au ordering, chemical substitution, and heat treatment merit further investigation.

cond-mat.mtrl-sci

Sign-switching of dimer correlations in SrCu$_2$(BO$_3$)$_2$ under hydrostatic pressure

Magnetic and vibrational excitations in SrCu$_2$(BO$_3$)$_2$ are studied using Raman spectroscopy at hydrostatic pressures up to 34 kbar and temperatures down to 2.6 K. The frequency of a particular optical phonon, the so-called pantograph mode, shows a very strong anomalous temperature dependence below about 40 K. We link the magnitude of the effect to the magnetic exchange energy on the dimer bonds in the Sutherland-Shastry spin lattice in this material. The corresponding dimer spin correlations are quantitatively estimated and found to be strongly pressure dependent. At around P$_2\sim$22 kbar they switch from antiferromagnetic to being predominantly ferromagnetic.

cond-mat.str-el

High pressure Raman study of the quantum magnet (C$_4$H$_{12}$N$_2$)Cu$_2$Cl$_6$

Magnetic and lattice excitations in the quantum antiferromagnet (C$_4$H$_{12}$N$_2$)Cu$_2$Cl$_6$ (PHCC) are studied across two pressure-induced phase transition at $P_c=4.3~\mathrm{kbar}$ and $P_1=13.4~\mathrm{kbar}$ using Raman spectroscopy. It is confirmed that neither transition is a result of a structural transformation. Magnetic scattering is detected. It shows a pronounced pressure dependence and undergoes substantial changes at both transitions. The results are in clear contradiction with previous neutron studies, which detected only minor changes of the magnon spectrum at $P_1$. A number of phonons show anomalous frequency shifts at low temperatures. This effect is pressure dependent and for two of the observed phonons dramatically reverses sign at around $P_1$. The anomalous behavior is attributed to strong magnetoelastic coupling in PHCC.

cond-mat.str-el

Magnetic structure and spin waves in the frustrated ferro-antiferromagnet Pb$_2$VO(PO$_4$)$_2$

Single crystal neutron diffraction, inelastic neutron scattering and electron spin resonance experiments are used to study the magnetic structure and spin waves in Pb$_2$VO(PO$_4$)$_2$, a prototypical layered $S=1/2$ ferromagnet with frustrating next nearest neighbor antiferromagnetic interactions. The observed excitation spectrum is found to be inconsistent with a simple square lattice model previously proposed for this material. At least four distinct exchange coupling constants are required to reproduce the measured spin wave dispersion. The degree of magnetic frustration is correspondingly revised and found to be substantially smaller than in all previous estimates.

cond-mat.str-el