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Darius H. Torchinsky

Publications and source records attributed to Darius H. Torchinsky.

15 recordsLinked to original sources

Second Harmonic Generation Spectroscopy of the Surface Charge Density Wave in the Weyl Semimetal CoSi

Using temperature-dependent rotational anisotropy second harmonic generation (RA-SHG), we identify a charge density wave (CDW) instability on the CoSi (001) face with an onset temperature at $90.0 \pm 0.8$ K. The SHG response tracks the order parameter amplitude, dominated by two nonlinear tensor elements, whose background-subtracted intensity evolves with temperature as a power law. The extracted critical exponent $\beta = 0.30 \pm 0.03$ is consistent with the 3D XY universality class, an unexpected result for a nominally two-dimensional surface layer. No corresponding anomaly is observed in the bulk response, establishing the transition as a purely surface-driven phase transition. We attribute this unexpected scaling to the coupling between surface Fermi-arc states and the bulk topology they are tied to, grounded in a previously observed intra-unit-cell phase relationship between surface sublayers that gives the order parameter intrinsic three-dimensional structure.

cond-mat.str-el

Evidence for ferroaxial order in 1T-TiSe$_2$ via elastoresistivity measurements

The study of spontaneous symmetry breaking and electronic order is fundamental in condensed matter physics. Hidden order, symmetry-breaking states that elude conventional probes, potentially plays a crucial role in understanding complex quantum phases in a wide range of materials. Ferroaxial order, a state characterized by broken mirror symmetries while maintaining time-reversal and inversion symmetries, is one of the hidden orders that have proven most challenging to detect experimentally. Here, we demonstrate a new approach for investigating both the ferroaxial order parameter and ferroaxial susceptibility using elastoresistivity measurements. We do this for 1T-TiSe$_{2}$, a material that exhibits charge density wave order that has eluded comprehensive understanding for a long time. These measurements reveal an anomalous off-diagonal linear elastoresistivity in the CDW state. We discuss why this provides a smoking gun for ferroaxial order. Furthermore, we construct an appropriate combination of the symmetry-breaking strains $\epsilon_{x^2-y^2}$ and $\epsilon_{xy}$ that acts as an effective conjugate field for the ferroaxial order, and demonstrate how sweeping this effective field in the CDW state results in a hysteretic behavior of the elastoresistivity, associated with the movement of ferroaxial domain walls. Finally, we reveal a divergence of certain nonlinear elastoresistivity coefficients above the critical temperature, and discuss how this is consistent with a divergence of the ferroaxial susceptibility near T$_{\rm{CDW}}$ $\sim$ 200K. Our study also includes detailed elastocaloric measurements, which reveal the presence of an additional phase transition several tens of Kelvin below T$_{\rm{CDW}}$. Our results provide new insight into the symmetry of the ordered state in 1T-TiSe$_2$ and establish elastoresistivity as a powerful probe of hidden order and its symmetry.

cond-mat.str-el

Topological spiral magnetism in the Weyl semimetal SmAlSi

Weyl electrons are intensely studied due to novel charge transport phenomena such as chiral anomaly, Fermi arcs, and photogalvanic effect. Recent theoretical works suggest that Weyl electrons can also participate in magnetic interactions, and the Weyl-mediated indirect exchange coupling between local moments is proposed as a new mechanism of spiral magnetism that involves chiral electrons. Despite reports of incommensurate and non-collinear magnetic ordering in Weyl semimetals, an actual spiral order has remained hitherto undetected. Here, we present evidence of Weyl-mediated spiral magnetism in SmAlSi from neutron diffraction, transport, and thermodynamic data. We show that the spiral order in SmAlSi results from the nesting between topologically non-trivial Fermi pockets and weak magnetocrystalline anisotropy, unlike related materials (Ce,Pr,Nd)AlSi, where a strong anisotropy prevents the spins from freely rotating. We map the magnetic phase diagram of SmAlSi and reveal an A-phase where topological magnetic excitations may exist. This is corroborated by the observation of a topological Hall effect within the A-phase.

cond-mat.mtrl-sci

Mapping Domain Wall Topology in the Magnetic Weyl Semimetal CeAlSi

We report full vector mapping of local magnetization in CeAlSi, a Weyl semimetal in which both inversion and time-reversal symmetries are broken. The vector maps reveal unanticipated features both within domains and at their boundaries. Boundaries between domains form two kinds of walls with distinct topology and therefore different interactions with Weyl fermions. Domain walls aligned along the tetragonal axes, e.g. (100), exhibit emergent chirality forbidden by the bulk space group, while diagonal walls are non-chiral. Within the domains, we observe that the previously reported set of four easy axes aligned along the in-plane diagonals of the tetragonal structure actually split to form an octet with decreasing temperature below the magnetic transition. All the above phenomena are ultimately traced to the noncollinear magnetic structure of CeAlSi.

cond-mat.str-el

A new noncollinear ferromagnetic Weyl semimetal with anisotropic anomalous Hall effect

A developing frontier in condensed matter physics is the emergence of novel electromagnetic responses, such as topological and anomalous Hall effect (AHE), in ferromagnetic Weyl semimetals (FM-WSMs). Candidates of FM-WSM are limited to materials that preserve inversion symmetry and generate Weyl crossings by breaking time-reversal symmetry. These materials share three common features: a centrosymmetric lattice, a collinear FM ordering, and a large AHE observed when the field is parallel to the magnetic easy-axis. Here, we present CeAlSi as a new type of FM-WSM, where the Weyl nodes are stabilized by breaking inversion symmetry, but their positions are tuned by breaking time-reversal symmetry. Unlike the other FM-WSMs, CeAlSi has a noncentrosymmetric lattice, a noncollinear FM ordering, and a novel AHE that is anisotropic between the easy- and hard-axes. It also exhibits large FM domains that are promising for both device applications and an interplay between the Weyl nodes and FM domain walls.

cond-mat.mtrl-sci

Direct Measurement of Helicoid Surface States in RhSi using Nonlinear Optics

Despite the fundamental nature of the edge state in topological physics, direct measurement of electronic and optical properties of the Fermi arcs of topological semimetals has posed a significant experimental challenge, as their response is often overwhelmed by the metallic bulk. However, laser-driven currents carried by surface and bulk states can propagate in different directions in nonsymmorphic crystals, allowing for the two components to be easily separated. Motivated by a recent theoretical prediction \cite{chang20}, we have measured the linear and circular photogalvanic effect currents deriving from the Fermi arcs of the nonsymmorphic, chiral Weyl semimetal RhSi over the $0.45 - 1.1$ eV incident photon energy range. Our data are in good agreement with the predicted magnitude of the circular photogalvanic effect as a function of photon energy, although the direction of the surface photocurrent departed from the theoretical expectation over the energy range studied. Surface currents arising from the linear photogalvanic effect were observed as well, with the unexpected result that only two of the six allowed tensor element were required to describe the measurements, suggesting an approximate emergent mirror symmetry inconsistent with the space group of the crystal.

cond-mat.mes-hall

Suppression of second-harmonic generation from linear bands in the topological multifold semimetal RhSi

Recent experiments in the topological Weyl semimetal TaAs have observed record-breaking second-harmonic generation, a non-linear optical response at $2ω$ generated by an incoming light source at $ω$. However, whether second-harmonic generation is enhanced in topological semimetals in general is a challenging open question because their band structure entangles the contributions arising from trivial bands and topological band crossings. In this work, we circumvent this problem by studying RhSi, a chiral topological semimetal with a simple band structure with topological multifold fermions close to the Fermi energy. We measure second-harmonic generation (SHG) in a wide frequency window, $ω\in [0.27,1.5]$eV and, using first principle calculations, we establish that, due to their linear dispersion, the contribution of multifold fermions to SHG is subdominant as compared with other regions in the Brillouin zone. Our calculations suggest that parts of the bands where the dispersion is relatively flat contribute significantly to SHG. As a whole, our results suggest avenues to enhance SHG responses.

cond-mat.mtrl-sci

Incommensurate magnetism mediated by Weyl fermions in NdAlSi

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect, and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a new Weyl semimetal, NdAlSi that offers an example. Using neutron diffraction, we report a long-wavelength magnetic order in NdAlSi whose periodicity is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. Our work provides a rare example of Weyl fermions driving collective magnetism.

cond-mat.str-el

Observation of Topological Photocurrents in the Chiral Weyl Semimetal RhSi

Weyl semimetals are crystals in which electron bands cross at isolated points in momentum space. Associated with each crossing point (or Weyl node) is an integer topological invariant known as the Berry monopole charge. The discovery of new classes of Weyl materials is driving the search for novel properties that derive directly from the Berry charge. The circular photogalvanic effect (CPGE), whereby circular polarized light generates a current whose direction depends on the helicity of the absorbed photons, is a striking example of a macroscopic property that emerges from Weyl topology. Recently, it was predicted that the rate of current generation associated with optical transitions near a Weyl node is proportional to its monopole charge and independent of material-specific parameters. In Weyl semimetals that retain mirror symmetry this universal photogalvanic current is strongly suppressed by opposing contributions from energy equivalent nodes of opposite charge. However, when all mirror symmetries are broken, as in chiral Weyl systems, nodes with opposite topological charge are no longer degenerate, opening a window of photon energies where the topological CPGE can emerge. In this work we test this theory through measurement of the photon-energy dependence of the CPGE in the chiral Weyl semimetal RhSi. The spectrum is fully consistent with a topological CPGE, as it reveals a response in a low-energy window that closes at 0.65 eV, in quantitative agreement with the theoretically-derived bandstucture.

cond-mat.mes-hall

Fast Reflective Optic-Based Rotational Anisotropy Nonlinear Harmonic Generation Spectrometer

We present a novel Rotational Anisotropy Nonlinear Harmonic Generation (RA-NHG) apparatus based primarily upon reflective optics. The data acquisition scheme used here allows for fast accumulation of RA-NHG traces, mitigating low frequency noise from laser drift, while permitting real-time adjustment of acquired signals with significantly more data points per unit angle rotation of the optics than other RA-NHG setups. We discuss the design and construction of the optical and electronic components of the device and present example data taken on a GaAs test sample at a variety of wavelengths. The RA-second harmonic generation data for this sample show the expected four-fold rotational symmetry across a broad range of wavelengths, while those for RA-third harmonic generation exhibit evidence of cascaded nonlinear processes possible in acentric crystal structures.

physics.ins-det

Fourier Domain Rotational Anisotropy Second Harmonic Generation

We describe a novel scheme of detecting rotational anisotropy second harmonic generation (RA-SHG) signals using a lock-in amplifier referenced to a fast scanning RA-SHG apparatus. The method directly measures the $n^{th}$ harmonics of the scanning frequency corresponding to SHG signal components of $C_n$ symmetry that appear in a Fourier series expansion of a general RA-SHG signal. GaAs was used as a test sample allowing comparison of point-by-point averaging with the lock-in based method. When divided by the $C_\infty$ signal component, the lock-in detected data allowed for both self-referenced determination of ratios of $C_n$ components of up to 1 part in 10$^4$ and significantly more sensitive measurement of the relative amount of different $C_n$ components when compared with conventional methods.

physics.optics

Resonance-enhanced optical nonlinearity in the Weyl semimetal TaAs

While all media can exhibit first-order conductivity describing current linearly proportional to electric field, $E$, the second-order conductivity, $σ^{(2)}$ , relating current to $E^2$, is nonzero only when inversion symmetry is broken. Second order nonlinear optical responses are powerful tools in basic research, as probes of symmetry breaking, and in optical technology as the basis for generating currents from far-infrared to X-ray wavelengths. The recent surge of interest in Weyl semimetals with acentric crystal structures has led to the discovery of a host of $σ^{(2)}$ -related phenomena in this class of materials, such as polarization-selective conversion of light to dc current (photogalvanic effects) and the observation of giant second-harmonic generation (SHG) efficiency in TaAs at photon energy 1.5 eV. Here, we present measurements of the SHG spectrum of TaAs revealing that the response at 1.5 eV corresponds to the high-energy tail of a resonance at 0.7 eV, at which point the second harmonic conductivity is approximately 200 times larger than seen in the standard candle nonlinear crystal, GaAs. This remarkably large SHG response provokes the question of ultimate limits on $σ^{(2)}$ , which we address by a new theorem relating frequency-integrated nonlinear response functions to the third cumulant (or "skewness") of the polarization distribution function in the ground state. This theorem provides considerable insight into the factors that lead to the largest possible second-order nonlinear response, specifically showing that the spectral weight is unbounded and potentially divergent when the possibility of next-neighbor hopping is included.

cond-mat.mtrl-sci

Direct Test of Supercooled Liquid Scaling Relations

Diverse material classes exhibit practically identical behavior when made viscous upon cooling toward the glass transition, suggesting a common theoretical basis. The first-principles scaling laws that have been proposed to describe the evolution with temperature have yet to be appropriately tested due to the extraordinary range of time scales involved. We used seven different measurement methods to determine the structural relaxation kinetics of a prototype molecular glass former over a temporal range of 13 decades and over a temperature range spanning liquid to glassy states. For the material studied, our results comprise a comprehensive validation of the two scaling relations that are central to the fundamental question of whether supercooled liquid dynamics can be described universally. The ultrabroadband mechanical measurements demonstrated have fundamental and practical applications in polymer science, geophysics, multifunctional materials, and other areas.

cond-mat.soft

Fluctuating charge density waves in a cuprate superconductor

Cuprate materials hosting high-temperature superconductivity (HTS) also exhibit various forms of charge and/or spin ordering whose significance is not fully understood. To date, static charge-density waves (CDWs) have been detected by diffraction probes only at special doping or in an applied external field. However, dynamic CDWs may also be present more broadly and their detection, characterization and relationship with HTS remain open problems. Here, we present a new method, based on ultrafast spectroscopy, to detect the presence and measure the lifetimes of CDW fluctuations in cuprates. In an underdoped La1.9Sr0.1CuO4 film (Tc = 26 K), we observe collective excitations of CDW that persist up to 100 K. This dynamic CDW fluctuates with a characteristic lifetime of 2 ps at T = 5 K which decreases to 0.5 ps at T = 100 K. In contrast, in an optimally doped La1.84Sr0.16CuO4 film (Tc = 38.5 K), we detect no signatures of fluctuating CDWs at any temperature, favoring the competition scenario. This work forges a path for studying fluctuating order parameters in various superconductors and other materials.

cond-mat.supr-con

$α$-Scale Decoupling of the Mechanical Relaxation and Diverging Shear Wave Propagation Lengthscale in Triphenylphosphite

We have performed depolarized Impulsive Stimulated Scattering experiments to observe shear acoustic phonons in supercooled triphenylphosphite (TPP) from $\sim$10 - 500 MHz. These measurements, in tandem with previously performed longitudinal and shear measurements, permit further analyses of the relaxation dynamics of TPP within the framework of the mode coupling theory (MCT). Our results provide evidence of $α$ coupling between the shear and longitudinal degrees of freedom up to a decoupling temperature $T_c$ = 231 K. A lower bound length scale of shear wave propagation in liquids verified the exponent predicted by theory in the vicinity of the decoupling temperature.

cond-mat.dis-nn