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Anshul Kogar

Publications and source records attributed to Anshul Kogar.

33 records · Page 2Linked to original sources

Second harmonic generation as a probe of broken mirror symmetry

The notion of spontaneous symmetry breaking has been used to describe phase transitions in a variety of physical systems. In crystalline solids, the breaking of certain symmetries, such as mirror symmetry, is difficult to detect unambiguously. Using 1$T$-TaS$_2$, we demonstrate here that rotational-anisotropy second harmonic generation (RA-SHG) is not only a sensitive technique for the detection of broken mirror symmetry, but also that it can differentiate between mirror symmetry-broken structures of opposite planar chirality. We also show that our analysis is applicable to a wide class of different materials with mirror symmetry-breaking transitions. Lastly, we find evidence for bulk mirror symmetry-breaking in the incommensurate charge density wave phase of 1$T$-TaS$_2$. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role.

cond-mat.mtrl-sci↗

Amplitude dynamics of charge density wave in LaTe$_3$: theoretical description of pump-probe experiments

We formulate a dynamical model to describe a photo-induced charge density wave (CDW) quench transition and apply it to recent multi-probe experiments on LaTe$_3$ [A. Zong et al., Nat. Phys. 15, 27 (2019)]. Our approach relies on coupled time-dependent Ginzburg-Landau equations tracking two order parameters that represent the modulations of the electronic density and the ionic positions. We aim at describing the amplitude of the order parameters under the assumption that they are homogeneous in space. This description is supplemented by a three-temperature model, which treats separately the electronic temperature, temperature of the lattice phonons with stronger couplings to the electronic subsystem, and temperature of all other phonons. The broad scope of available data for LaTe$_3$ and similar materials as well as the synergy between different time-resolved spectroscopies allow us to extract model parameters. The resulting calculations are in good agreement with ultra-fast electron diffraction experiments, reproducing qualitative and quantitative features of the CDW amplitude evolution during the initial few picoseconds after photoexcitation.

cond-mat.mes-hall↗

Optical detection and manipulation of spontaneous gyrotropic electronic order in a transition-metal dichalcogenide semimetal

The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels. Examples range from parity violation in the subatomic weak force to the homochirality in essential biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order, where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal $1T$-TiSe$_2$. We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe$_2$. Such chiral induction provides a new way of optical control over novel orders in quantum materials.

cond-mat.mes-hall↗

Light-Induced Charge Density Wave in LaTe$_3$

When electrons in a solid are excited with light, they can alter the free energy landscape and access phases of matter that are beyond reach in thermal equilibrium. This accessibility becomes of vast importance in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by light. Here, we study a layered compound, LaTe$_3$, where a small in-plane (a-c plane) lattice anisotropy results in a unidirectional charge density wave (CDW) along the c-axis. Using ultrafast electron diffraction, we find that after photoexcitation, the CDW along the c-axis is weakened and subsequently, a different competing CDW along the a-axis emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for unleashing similar states of matter that are "trapped" under equilibrium conditions.

cond-mat.mtrl-sci↗

Dynamical slowing down in an ultrafast photo-induced phase transition

Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photo-induced transition of a model charge-density-wave (CDW) compound, LaTe$_3$. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be quantitatively captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.

cond-mat.str-el↗

Ultrafast manipulation of mirror domain walls in a charge density wave

Domain walls (DWs) are singularities in an ordered medium that often host exotic phenomena such as charge ordering, insulator-metal transition, or superconductivity. The ability to locally write and erase DWs is highly desirable, as it allows one to design material functionality by patterning DWs in specific configurations. We demonstrate such capability at room temperature in a charge density wave (CDW), a macroscopic condensate of electrons and phonons, in ultrathin 1T-TaS$_2$. A single femtosecond light pulse is shown to locally inject or remove mirror DWs in the CDW condensate, with probabilities tunable by pulse energy and temperature. Using time-resolved electron diffraction, we are able to simultaneously track anti-synchronized CDW amplitude oscillations from both the lattice and the condensate, where photo-injected DWs lead to a red-shifted frequency. Our demonstration of reversible DW manipulation may pave new ways for engineering correlated material systems with light.

cond-mat.mtrl-sci↗

Disentangling amplitude and phase dynamics of a charge density wave in a photo-induced phase transition

Upon excitation with an intense ultrafast laser pulse, a symmetry-broken ground state can undergo a non-equilibrium phase transition through pathways dissimilar from those in thermal equilibrium. Determining the mechanism underlying these photo-induced phase transitions (PIPTs) has been a long-standing issue in the study of condensed matter systems. To this end, we investigate the light-induced melting of a unidirectional charge density wave (CDW) material, LaTe$_3$. Using a suite of time-resolved probes, we independently track the amplitude and phase dynamics of the CDW. We find that a quick ($\sim\,$1$\,$ps) recovery of the CDW amplitude is followed by a slower reestablishment of phase coherence. This longer timescale is dictated by the presence of topological defects: long-range order (LRO) is inhibited and is only restored when the defects annihilate. Our results provide a framework for understanding other PIPTs by identifying the generation of defects as a governing mechanism.

cond-mat.mtrl-sci↗

Signatures of exciton condensation in a transition metal dichalcogenide

Bose condensation has shaped our understanding of macroscopic quantum phenomena, having been realized in superconductors, atomic gases, and liquid helium. Excitons are bosons that have been predicted to condense into either a superfluid or an insulating electronic crystal. Using the recently developed momentum-resolved electron energy-loss spectroscopy (M-EELS), we study electronic collective modes in the transition metal dichalcogenide semimetal, 1T-TiSe$_2$. Near the phase transition temperature, T$_c$ = 190 K, the energy of the electronic mode falls to zero at nonzero momentum, indicating dynamical slowing down of plasma fluctuations and crystallization of the valence electrons into an exciton condensate. Our study provides compelling evidence for exciton condensation in a three-dimensional solid and establishes M-EELS as a versatile technique sensitive to valence band excitations in quantum materials.

cond-mat.str-el↗

Measurement of the dynamic charge response of materials using low-energy, momentum-resolved electron energy-loss spectroscopy (M-EELS)

One of the most fundamental properties of an interacting electron system is its frequency- and wave-vector-dependent density response function, $χ({\bf q},ω)$. The imaginary part, $χ''({\bf q},ω)$, defines the fundamental bosonic charge excitations of the system, exhibiting peaks wherever collective modes are present. $χ$ quantifies the electronic compressibility of a material, its response to external fields, its ability to screen charge, and its tendency to form charge density waves. Unfortunately, there has never been a fully momentum-resolved means to measure $χ({\bf q},ω)$ at the meV energy scale relevant to modern elecronic materials. Here, we demonstrate a way to measure $χ$ with quantitative momentum resolution by applying alignment techniques from x-ray and neutron scattering to surface high-resolution electron energy-loss spectroscopy (HR-EELS). This approach, which we refer to here as "M-EELS," allows direct measurement of $χ''({\bf q},ω)$ with meV resolution while controlling the momentum with an accuracy better than a percent of a typical Brillouin zone. We apply this technique to finite-q excitations in the optimally-doped high temperature superconductor, Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$ (Bi2212), which exhibits several phonons potentially relevant to dispersion anomalies observed in ARPES and STM experiments. Our study defines a path to studying the long-sought collective charge modes in quantum materials at the meV scale and with full momentum control.

cond-mat.supr-con↗

Observation of a Charge Density Wave Incommensuration Near the Superconducting Dome in CuxTiSe2

X-ray diffraction was employed to study the evolution of the charge density wave (CDW) in CuxTiSe2 as a function of copper intercalation in order to clarify the relationship between the CDW and superconductivity. The results show a CDW incommensuration arising at an intercalation value coincident with the onset of superconductivity at around x=0.055(5). Additionally, it was found that the charge density wave persists to higher intercalant concentrations than previously assumed, demonstrating that the CDW does not terminate inside the superconducting dome. A charge density wave peak was observed in samples up to x=0.091(6), the highest copper concentration examined in this study. The phase diagram established in this work suggests that charge density wave incommensuration may play a role in the formation of the superconducting state.

cond-mat.supr-con↗

Quasiparticle Interference and Strong Electron-Mode Coupling in the Quasi-One-Dimensional Bands of Sr$_2$RuO$_4$

The single-layered ruthenate Sr$_2$RuO$_4$ has attracted a great deal of interest as a spin-triplet superconductor with an order parameter that may potentially break time reversal invariance and host half-quantized vortices with Majorana zero modes. While the actual nature of the superconducting state is still a matter of controversy, it has long been believed that it condenses from a metallic state that is well described by a conventional Fermi liquid. In this work we use a combination of Fourier transform scanning tunneling spectroscopy (FT-STS) and momentum resolved electron energy loss spectroscopy (M-EELS) to probe interaction effects in the normal state of Sr$_2$RuO$_4$. Our high-resolution FT-STS data show signatures of the β-band with a distinctly quasi-one-dimensional (1D) character. The band dispersion reveals surprisingly strong interaction effects that dramatically renormalize the Fermi velocity, suggesting that the normal state of Sr$_2$RuO$_4$ is that of a 'correlated metal' where correlations are strengthened by the quasi 1D nature of the bands. In addition, kinks at energies of approximately 10meV, 38meV and 70meV are observed. By comparing STM and M-EELS data we show that the two higher energy features arise from coupling with collective modes. The strong correlation effects and the kinks in the quasi 1D bands may provide important information for understanding the superconducting state. This work opens up a unique approach to revealing the superconducting order parameter in this compound.

cond-mat.str-el↗

A reexamination of the effective fine structure constant of graphene, as measured in graphite

We present a refined and improved study of the influence of screening on the effective fine structure constant of graphene, $α^*$, as measured in graphite using inelastic x-ray scattering. This follow-up to our previous study [J. P. Reed, et al., Science 330, 805 (2010)] was carried out with two times better energy resolution, five times better momentum resolution, and improved experimental setup with lower background. We compare our results to RPA calculations and evaluate the relative importance of interlayer hopping, excitonic corrections, and screening from high energy excitations involving the $σ$ bands. We find that the static, limiting value of $α^*$ falls in the range 0.25 to 0.35, which is higher than our previous result of 0.14, but still below the value expected from RPA. We show the reduced value is not a consequence of interlayer hopping effects, which were ignored in our previous analysis, but of a combination of excitonic effects in the $π\rightarrow π^*$ particle-hole continuum, and background screening from the $σ$-bonded electrons. We find that $σ$-band screening is extremely strong at distances of the order of a few nm, and should be highly effective at screening out short-distance, Hubbard-like interactions in graphene, as well as other carbon allotropes.

cond-mat.str-el↗

Temperature-resolution anomalies in the reconstruction of time dynamics from energy-loss experiments

Inelastic scattering techniques provide a powerful approach to studying electron and nuclear dynamics, via reconstruction of a propagator that quantifies the time evolution of a system. There is now growing interest in applying such methods to very low energy excitations, such as lattice vibrations, but in this limit the cross section is no longer proportional to a propagator. Significant deviations occur due to the finite temperature Bose statistics of the excitations. Here we consider this issue in the context of high-resolution electron energy loss experiments on the copper-oxide superconductor Bi$_2$Sr$_2$CaCu$_2$O$_{8+x}$. We find that simple division of a Bose factor yields an accurate propagator on energy scales greater than the resolution width. However, at low energy scales, the effects of resolution and finite temperature conspire to create anomalies in the dynamics at long times. We compare two practical ways for dealing with such anomalies, and discuss the range of validity of the technique in light of this comparison.

cond-mat.str-el↗

Crystallographic refinement of collective excitations using standing wave inelastic x-ray scattering

We propose a method for realizing true, real-space imaging of charge dynamics in a periodic system, with angstrom spatial resolution and attosecond time resolution. In this method, inelastic x-ray scattering (IXS) is carried out with a coherent, standing wave source, which provides the off-diagonal elements of the generalized dynamic structure factor, S(q_1,q_2,ω), allowing complete reconstruction of the inhomogeneous response function of the system, χ(x_1,x_2,t). The quantity χhas the physical meaning of a propagator for charge, so allows one to observe - in real time - the disturbance in the electron density created by a point source placed at a specified location, x_1 (on an atom vs. between atoms, for example). This method may be thought of as a generalization of x-ray crystallography that allows refinement of the excited states of a periodic system, rather than just its ground state.

cond-mat.str-el↗

Adsorption properties and third sound propagation in superfluid $^4$He films on carbon nanotubes

We consider the adsorption properties of superfluid $^4$He films on carbon nanotubes. One major factor in the adsorption is the surface tension force arising from the very small diameter of the nanotubes. Calculations show that surface tension keeps the film thickness on the tubes very thin even when the helium vapor is increased to the saturated pressure. The weakened Van der Waals force due to the cylindrical geometry also contributes to this. Both of these effects act to lower the predicted velocity of third sound propagation along the tubes. It does not appear that superfluidity will be possible on single-walled nanotubes of diameter about one nm, since the film thickness is less than 3 atomic layers even at saturation. Superfluidity is possible on larger-diameter nanotube bundles and multi-walled nanotubes, however. We have observed third sound signals on nanotube bundles of average diameter 5 nm which are sprayed onto a Plexiglass surface, forming a network of tubes.

cond-mat.mtrl-sci↗