arXiv subjects

Girsh Blumberg

Publications and source records attributed to Girsh Blumberg.

17 recordsLinked to original sources

arXiv2026

Direct observation of phonon mode with an antisymmetric Raman tensor

Phonon angular momentum, characterized by circular or elliptical motion of atoms, plays a decisive role in diverse phenomena, ranging from the phonon Hall effect, phonon magnetic moment, Einstein-de Haas effect, Weyl phonons, and driven chiral phonons. The phonon modes with an antisymmetric Raman tensor, which carry an intrinsic phonon angular momentum in a pseudovector symmetry channel, have been overlooked in the past in the chiral phonon community. Here, we report the detection of this type of phonon mode using polarization-resolved Raman spectroscopy. We observe a phonon at 266cm$^{-1}$ in the antiferromagnetic chiral phase of Cr$_2$O$_3$ in the $A_2$-pseudovector symmetry channel. This $A_2$ mode's frequency and the elliptical motion are captured by first-principles phonon calculations, which treat both lattice and spins on an equal footing as 'slow' degrees of freedom. This mode gets Raman activity due to the presence of Cr vacancies in Cr$_2$O$_3$ that locally break the twofold rotational symmetry perpendicular to the threefold axis. Our results provide a new way to detect the novel symmetry-forbidden $A_2$ phonon modes with an antisymmetric Raman tensor in a pseudovector symmetry channel.

cond-mat.mtrl-sci↗

arXiv2026

Magnetic quantum defects in a uniaxial antiferromagnetic insulator

Point defects have been successfully utilized in various quantum technologies, serving as quantum qubits for quantum computation, single-photon emitters for quantum communication, and nanoscale sensors for quantum metrology. However, their further development faces key challenges, particularly in discovering and exploring suitable defect-host systems that meet the necessary criteria for quantum applications. Here, using polarization-resolved Raman spectroscopy and terahertz absorption spectroscopy, we discover three distinct chromium-vacancy-induced excitations in the uniaxial antiferromagnetic insulator, Cr$_2$O$_3$. These vacancy-induced excitations have an energy scale of a few tens of millielectronvolts and are twofold degenerate, and the lowest one at 64 $cm^{-1}$ is sharp and sensitive to the external magnetic field along the easy-axis direction, particularly close to the spin-flop regime around 6T, where the mode softens from 64 to 27$cm^{-1}$. Based on the defect supercell first-principles calculations, we interpret the mode at 64 $cm^{-1}$ as a local magnetic excitation of the local moment within the chromium vacancy state. Our results establish that the magnetic defect states in Cr$_2$O$_3$ have potential for quantum applications.

cond-mat.mtrl-sci↗

arXiv2025

Phonon anomalies within the polar charge density wave phase of the structurally chiral superconductor Mo$_3$Al$_2$C

We employ polarization-resolved Raman spectroscopy to study the lattice dynamics of the polar charge density wave phase of the superconductor Mo$_3$Al$_2$C with structural chirality. We show the phononic signatures of the charge density wave transition at $T^*$ = 155\,K in Mo$_3$Al$_2$C. The detailed temperature dependence of these phonon modes' frequency, half width at half maximum, and integrated area below $T^*$ reveal anomalies at an intermediate temperature $T' \sim$ 100\,K, especially for the low-energy modes at 130 and 180\,\cm-1. We discuss the origin of these phonon anomalies within the polar charge density wave phase of Mo$_3$Al$_2$C.

cond-mat.supr-con↗

arXiv2024

Polar charge density wave in a superconductor with crystallographic chirality

Symmetry plays an important role in determining the physical properties in condensed matter physics, as the symmetry operations of any physical property must include the symmetry operations of the point group of the crystal. As a consequence, crystallographic polarity and chirality are expected to have an impact on the Cooper pairing in a superconductor. While superconductivity with crystallographic polarity and chirality have both been found in a few crystalline phases separately; however, their coexistence and material realizations have not been studied. Here, by utilizing transport, Raman scattering, and transmission electron microscopy, we unveil a unique realization of superconductivity in single-crystalline Mo3Al2C (superconducting Tc=8K) with a polar charge-density-wave phase and well-defined crystallographic chirality. We show that the intriguing charge density wave order leads to a noncentrosymmetric-nonpolar to polar transition below T*=155K via breaking both the translational and rotational symmetries. Superconductivity emerges in this polar and chiral crystal structure below Tc=8K. Our results establish that Mo3Al2C is a superconductor with crystallographic polarity and chirality simultaneously, and motivate future studies of unconventional superconductivity in this category.

cond-mat.supr-con↗

arXiv2024

Symmetry breaking and ascending in the magnetic kagome metal FeGe

Spontaneous symmetry breaking-the phenomenon where an infinitesimal perturbation can cause the system to break the underlying symmetry-is a cornerstone concept in the understanding of interacting solid-state systems. In a typical series of temperature-driven phase transitions, higher temperature phases are more symmetric due to the stabilizing effect of entropy that becomes dominant as the temperature is increased. However, the opposite is rare but possible when there are multiple degrees of freedom in the system. Here, we present such an example of a symmetry-ascending phenomenon in a magnetic kagome metal FeGe by utilizing neutron Larmor diffraction and Raman spectroscopy. In the paramagnetic state at 460K, we confirm that the crystal structure is indeed hexagonal kagome lattice. On cooling to TN, the crystal structure changes from hexagonal to monoclinic with in-plane lattice distortions on the order of 10^(-4) and the associated splitting of the double degenerate phonon mode of the pristine kagome lattice. Upon further cooling to TCDW, the kagome lattice shows a small negative thermal expansion, and the crystal structure becomes more symmetric gradually upon further cooling. Increasing the crystalline symmetry upon cooling is unusual, it originates from an extremely weak structural instability that coexists and competes with the CDW and magnetic orders. These observations are against the expectations for a simple model with a single order parameter, hence can only be explained by a Landau free energy expansion that takes into account multiple lattice, charge, and spin degrees of freedom. Thus, the determination of the crystalline lattice symmetry as well as the unusual spin-lattice coupling is a first step towards understanding the rich electronic and magnetic properties of the system and sheds new light on intertwined orders where the lattice degree of freedom is no longer dominant.

cond-mat.str-el↗

arXiv2024

Spin-orbit interaction enabled electronic Raman scattering from charge collective modes

Electronic Raman scattering in the fully symmetric channel couples to the charge excitations in the system, including the plasmons. However, the plasmon response has a spectral weight of $\sim q^2$, where $q$, the momentum transferred by light, is small. In this work, we show that in inversion symmetry broken systems where Rashba type spin-orbit coupling affects the states at the Fermi energy (which is a known low energy effect) as well as the transition elements to other states (a high energy effect), there is an additional coupling of the plasmons to the Raman vertex, even at zero momentum transfer, that results in a spectral weight that is proportional to the spin-orbit coupling. The high energy effect is due to the breaking of SU(2) spin invariance in the spin-flip transitions to the intermediate state. We present a theory for this coupling near the resonant regime of Raman scattering and show that in giant Rashba systems it can dominate over the conventional $q^2$ weighted coupling. We also provide experimental support along with a symmetry based justification for this spin-mediated coupling by identifying a prominent c-axis plasmon peak in the fully symmetric channel of the resonant Raman spectrum of the giant Rashba material BiTeI. This new coupling could lead to novel ways of manipulating coherent charge excitations in inversion-broken systems. This process is also relevant for spectroscopic studies in ultrafast spectroscopies, certain driven Floquet systems and topologically non-trivial phases of matter where strong inversion-breaking spin-orbit coupling plays a role.

cond-mat.mes-hall↗

arXiv2022

Charge density wave order in kagome metal AV$_3$Sb$_5$ (A= Cs, Rb, K)

We employ polarization-resolved electronic Raman spectroscopy and density functional theory to study the primary and secondary order parameters, as well as their interplay, in the charge density wave (CDW) state of the kagome metal AV3Sb5. Previous x-ray diffraction data at 15K established that the CDW order in CsV3Sb5 comprises of a 2x2x4 structure: one layer of inverse-star-of-David and three consecutive layers of star-of-David pattern. We analyze the lattice distortions based the 2x2x4 structure at 15K, and find that U lattice distortion is the primary order parameter while M and L distortions are secondary order parameters for Vanadium displacements. This conclusion is confirmed by the calculation of bare susceptibility that shows a broad peak at around qz=0.25 along the hexagonal Brillouin zone face central line (U-line). We also identify several phonon modes emerging in the CDW state, which are lattice vibration modes related to V and Sb atoms as well as alkali atoms. The detailed temperature evolution of these modes' frequencies, HWHM, and integrated intensities support a phase diagram with two successive structural phase transitions in CsV3Sb5: the first one with a primary order parameter appearing at TS=94K and the second isostructural one appearing at around 70K.

cond-mat.str-el↗

arXiv2022

Anisotropy of Kondo-lattice coherence in momentum space for CeCoIn5

We study the electronic and phononic excitations of heavy-fermion metal CeCoIn$_5$ by polarization-resolved Raman spectroscopy to explore the Kondo-lattice coherence. Below the coherence temperature T*\,=\,45\,K, the continuum of electronic excitations in the XY scattering geometry is suppressed at frequencies below 50\,cm$^{-1}$, whereas the low-frequency continuum in the X'Y' geometry exhibits no change across T*. We relate the suppression to the reduced electron-electron scattering rate resulting from the coherence effect. The presence of suppression in the XY geometry and absence of it in the X'Y' geometry implies that the $α$ and $β$ bands become coherent below T*, whereas the $γ$ band remains largely incoherent down to 10\,K. Moreover, two optical phonon modes exhibit anomalies in their temperature dependence of the frequency and linewidth below T*, which results from developing coherent spectral weight near the Fermi level and reduced electron-phonon scattering rate. Our results further support the key role of anisotropic hybridization in CeCoIn$_5$.

cond-mat.str-el↗

arXiv2021

Failed excitonic quantum phase transition in Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$

We study the electronic phase diagram of the excitonic insulator candidates Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ [x=0, ... ,1] using Raman spectroscopy. Critical excitonic fluctuations are observed, that diminish with $x$ and ultimately shift to high energies, characteristic of a quantum phase transition. Nonetheless, a symmetry-breaking transition at finite temperatures is detected for all $x$, exposing a cooperating lattice instability that takes over for large $x$. Our study reveals a failed excitonic quantum phase transition, masked by a preemptive structural order.

cond-mat.str-el↗

arXiv2021

Lattice dynamics of the excitonic insulator Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$

Recently, we employed electronic polarization-resolved Raman spectroscopy to reveal the strongly correlated excitonic insulator (EI) nature of Ta2NiSe5, Volkov et al. [arXiv:2007.07344], and also showed that for Ta$_2$Ni(Se$_{1-x}$S$_x$)$_5$ alloys the critical excitonic fluctuations diminish with sulfur concentration x exposing a cooperating lattice instability that takes over for large x, Volkov et al. [arXiv:2104.07032]. Here we focus on the lattice dynamics of this EI family. We identify all Raman-active optical phonons of fully symmetric and ac-quadrupole-like symmetries and study their evolution with temperature and sulfur concentration. We demonstrate the change of selection rules at temperatures below the orthorhombic-to-monoclinic transition at Tc(x) that is related to the EI phase. We find that Tc(x) decrease monotonically from 328 K for Ta2NiSe5 to 120 K for Ta2NiS5 and that the magnitude of lattice distortion also decreases with the sulfur concentration x. For x < 0.7, the two lowest-frequency B2g phonon modes show strongly asymmetric lineshapes at high temperatures due to Fano interference with the broad excitonic continuum present in a semimetallic state. Within the framework of extended Fano model, we develop a quantitative description of the interacting exciton-phonon excitation lineshape, enabling us to derive the intrinsic phonon parameters and determine the exciton-phonon interaction strength, that affects the transition temperature Tc(x). We also observe signatures of the acoustic mode scattered assisted by the structural domain walls formed below Tc. Based on our results, we additionally present a consistent interpretation of the origin of oscillations observed in time-resolved pump-probe experiments.

cond-mat.str-el↗

arXiv2021

Critical charge fluctuations and emergent coherence in a strongly correlated excitonic insulator

Excitonic insulator is a coherent electronic phase that results from the formation of a macroscopic population of bound particle-hole pairs - excitons. With only a few candidate materials known, the collective excitonic behavior is challenging to observe, being obscured by crystalline lattice effects. Here we use polarization-resolved Raman spectroscopy to reveal the quadrupolar excitonic mode in the candidate zero-gap semiconductor Ta$_2$NiSe$_5$ disentangling it from the lattice phonons. The excitonic mode pronouncedly softens close to the phase transition, showing its electronic character, while its coupling to non-critical lattice modes is shown to enhance the transition temperature. On cooling, we observe the gradual emergence of coherent superpositions of band states at the correlated insulator gap edge, with strong departures from mean-field theory predictions. Our results demonstrate the realization of a strongly correlated excitonic state in an equilibrium bulk material.

cond-mat.str-el↗

arXiv2021

Crystal-field excitations and vibronic modes in triangular-lattice spin-liquid candidate TbInO$_3$

We study the ground state properties, the electronic excitations and lattice dynamics in spin-liquid candidate TbInO$_3$. By employing polarization resolved Raman spectroscopy we define the inter- and intra-multiplet excitations, and establish the low-energy crystal-field (CF) level scheme. In particular, we demonstrate that the ground state of the Tb$^{3+}$ ions is a non-Kramers doublet, and relate the enhanced linewidth of the CF modes to the magnetic fluctuations near the spin-liquid ground state. We identify all 38 allowed Raman-active phonon modes at low temperature. Moreover, we observe hybrid vibronic excitations involving coupled CF and low-lying phonon modes, suggesting strong spin-lattice dynamics. We develop a model for vibronic states and obtain the parameters of the bare responses and coupling strength. We further demonstrate that the obtained CF level scheme is consistent with specific heat data.

cond-mat.str-el↗

arXiv2018

Covalency-driven collapse of strong spin-orbit coupling in face-sharing iridium octahedra

We report $\textit{ab-initio}$ density functional theory calculation and Raman scattering results to explore the electronic structure of Ba$_5$CuIr$_3$O$_{12}$ single crystals. This insulating iridate, consisting of face-sharing IrO$_6$ octahedra forming quasi-one-dimensional chains, cannot be described by the local $j_{\rm eff}$=1/2 moment picture commonly adopted for discussing electronic and magnetic properties of iridate compounds with IrO$_6$ octahedra. The shorter Ir-Ir distance in the face-sharing geometry, compared to corner- or edge-sharing structures, leads to strong covalency between neighboring Ir. Then this strong covalency results in the formation of molecular orbitals (MO) at each Ir trimers as the low-energy electronic degree of freedom. The theoretically predicted three-peak structure in the joint density of states, a distinct indication of deviation from the $j_{\rm eff}$=1/2 picture, is verified by observing the three-peak structure in the electronic excitation spectrum by Raman scattering.

cond-mat.str-el↗

arXiv2015

Diffraction limited focusing and routing of gap plasmons by a metal-dielectric-metal lens

Passive optical elements can play key roles in photonic applications such as plasmonic integrated circuits. Here we experimentally demonstrate passive gap-plasmon focusing and routing in two-dimensions. This is accomplished using a high numerical-aperture metal-dielectric-metal lens incorporated into a planar-waveguide device. Fabrication via metal sputtering, oxide deposition, electron- and focused-ion- beam lithography, and argon ion-milling is reported on in detail. Diffraction-limited focusing is optically characterized by sampling out-coupled light with a microscope. The measured focal distance and full-width-half-maximum spot size agree well with the calculated lens performance. The surface plasmon polariton propagation length is measured by sampling light from multiple out-coupler slits.

physics.optics↗

arXiv2014

Ultracompact Nano-Mechanical Plasmonic Phase Modulators

Dielectrics' refractive index limits photonics miniaturization. By coupling light to metal's free electrons, plasmonic devices achieve deeper localization, which scales with the device geometric size. However, when localization approaches the skin depth, energy shifts from the dielectric into the metal, hindering active modulation. Here we propose a nano-electromechanical phase modulation principle exploiting the extraordinarily strong dependence of the phase velocity of metal-insulator-metal(MIM) gap plasmons on dynamically variable gap size. We demonstrate a 23 μm long non-resonant modulator having 1.5 π rad range with 1.7 dB excess loss at 780 nm. Analysis shows an ultracompact 1 μm$^{2}$ footprint π rad phase modulator can be realized, more than an order of magnitude smaller than any previously shown. Remarkably, this size reduction is achieved without incurring extra loss, since the nanobeam-plasmon coupling strength increases at a similar rate as the loss. Such small, high density electrically controllable components may find applications in optical switch fabrics and reconfigurable flat plasmonic optics.

physics.optics↗

arXiv2010

Screening of the Raman response in multiband superconductors -- application to iron-pnictides

We performed model calculations of Raman responses for multiband 2D superconductors. The multiband effects of screening in the A_{1g} symmetry channel were investigated analytically and numerically for a band structure model mimicing ARPES data on iron-pnictide materials. An acceptable agreement between our model calculations and recent experimental data is demonstrated by modification of the band structure parameters.

cond-mat.supr-con↗

arXiv1999

Electronic Raman Scattering in Superconducting Cuprates

We show that the novel features observed in Raman experiments on optimally doped and underdoped Bi-2212 compounds in $B_{1g}$ geometry can be explained by a strong fermionic self-energy due to the interaction with spin fluctuations. We compute the Raman intensity $R(ω)$ both above and below $T_c$, and show that in both cases $R(ω)$ progressively deviates, with decreasing doping, from that in a Fermi-gas due to increasing contribution from the fermionic self-energy. We also show that the final state interaction increases with decreasing doping and gradually transforms the $2Δ$ peak in the superconducting state into a pseudo resonance mode below $2Δ$. We argue that these results agree well with the experimental data for Bi-2212.

cond-mat↗