arXiv subjects

N. P. Armitage

Publications and source records attributed to N. P. Armitage.

At least 37 records · Page 2Linked to original sources

arXiv2024

Anomalous electronic energy relaxation and soft phonons in the Dirac semimetal Cd$_3$As$_2$

We have used a combination of linear response time-domain THz spectroscopy (TDTS) and high-field non-linear THz spectroscopy to separately probe the electronic momentum and energy relaxation rates respectively of the Dirac semimetal Cd$_3$As$_2$. We find, consistent with prior measurements, that Cd$_3$As$_2$ has an enormous nonlinearities in the THz frequency range. We extract the momentum relaxation rate of Cd$_3$As$_2$ using Drude fits to the optical conductivity. We also conduct THz range 2D coherent spectroscopy. The dominant response is a pump-probe signal, which allow us to separately extract the energy relaxation rate. We find that the rate of energy relaxation decreases down to the lowest measured temperatures. We connect this to Cd$_3$As$_2$ anomalous lattice dynamics, evidence for which is found in its low thermal conductivity and soft phonons in Raman scattering. The lack of a peak in the energy relaxation rate as a function of T can be connected to the linear in T dependence of the current relaxation e.g. the phonon scattering is elastic down to the lowest measured temperatures approximately 120 K.

cond-mat.str-el↗

arXiv2024

Revealing novel aspects of light-matter coupling in terahertz two-dimensional coherent spectroscopy: the case of the amplitude mode in superconductors

Recently developed terahertz (THz) two-dimensional coherent spectroscopy (2DCS) is a powerful technique to obtain materials information in a fashion qualitatively different from other spectroscopies. Here, we utilized THz 2DCS to investigate the THz nonlinear response of conventional superconductor NbN. Using broad-band THz pulses as light sources, we observed a third-order nonlinear signal whose spectral components are peaked at twice the superconducting gap energy $2Δ$. With narrow-band THz pulses, a THz nonlinear signal was identified at the driving frequency $Ω$ and exhibited a resonant enhancement at temperature when $Ω= 2Δ$. General theoretical considerations show that such a resonance can only arise from a disorder-activated paramagnetic coupling between the light and the electronic current. This proves that the nonlinear THz response can access processes distinct from the diamagnetic Raman-like density fluctuations, which are believed to dominate the nonlinear response at optical frequencies in metals. Our numerical simulations reveal that even for a small amount of disorder, the $Ω=2Δ$ resonance is dominated by the superconducting amplitude mode over the entire investigated disorder range. This is in contrast to other resonances, whose amplitude-mode contribution depends on disorder. Our findings demonstrate the unique ability of THz 2DCS to explore collective excitations inaccessible in other spectroscopies.

cond-mat.supr-con↗

arXiv2024

Coupled metamaterial-phonon terahertz range polaritons in a topological insulator

We report terahertz time-domain spectroscopy (TDTS) experiments demonstrating strong light-matter coupling in a terahertz (THz) LC-metamaterial in which the phonon resonance of a topological insulator (TI) thin film is coupled to the photonic modes of an array of electronic split-ring resonators. As we tune the metamaterial resonance frequency through the frequency of the low frequency $α$ mode of (Bi$_x$Sb$_{1-x}$)$_2$Te$_3$ (BST), we observe strong mixing and level repulsion between phonon and metamaterial resonance. This hybrid resonance is a phonon polariton. We observe a normalized coupling strength, $η$ = $Ω_R$/$ω_c$ $\approx$ 0.09, using the measured vacuum Rabi frequency and cavity resonance. Our results demonstrate that one can tune the mechanical properties of materials by changing their electromagnetic environment and therefore modify their magnetic and topological degrees of freedom via coupling to the lattice in this fashion.

cond-mat.mes-hall↗

arXiv2024

Anomalous frequency and temperature dependent scattering in the dilute metallic phase in lightly doped-SrTiO$_3$

The mechanism of superconductivity in materials with aborted ferroelectricity and the emergence of a dilute metallic phase in systems like doped-SrTiO$_3$ are outstanding issues in condensed matter physics. This dilute metal has features both similar and different to those found in the normal state of other unconventional superconductors. We have investigated the optical properties of the dilute metallic phase in doped-SrTiO$_3$ using THz time-domain spectroscopy. At low frequencies the THz response exhibits a Drude-like form as expected for typical metal-like conductivity. We observed the frequency and temperature dependencies to the low energy scattering rate $Γ(ω, T) \propto (\hbarω)^2 + (p πk_BT)^2 $ expected in a conventional Fermi liquid, despite the fact that densities are too small to allow current decay through electron-electron scattering. However we find the lowest known $p$ values of 0.39-0.72. As $p$ is 2 in a canonical Fermi liquid and existing models based on energy dependent elastic scattering bound $p$ from below to 1, our observation lies outside current explanation. Our data also gives insight into the high temperature regime and shows that the temperature dependence of the resistivity derives in part from strong T dependent mass renormalizations.

cond-mat.str-el↗

arXiv2024

Continuum of magnetic excitations in the Kitaev honeycomb iridate D$_3$LiIr$_2$O$_6$

Inelastic neutron scattering (INS) measurements of powder D$_3(^{7}$Li)($^{193}$Ir)$_2$O$_6$ reveal low energy magnetic excitations with a scattering cross section that is broad in $|Q|$ and consistent with a Kitaev spin-liquid (KSL) state. The magnetic nature of the excitation spectrum is demonstrated by longitudinally polarized neutron studies. The total magnetic moment of 1.7(2)$μ_B$/Ir inferred from the total magnetic scattering cross section is consistent with the effective moment inferred from magnetic susceptibility data and expectations for the $J_{\rm eff}=1/2$ single ion state. The rise in the dynamic correlation function ${\cal S}(Q,ω)$ for $\hbarω<5~$meV can be described by a nearest-neighbor Kitaev model with interaction strength $K\approx-13(5)$~meV. Exchange disorder associated with the mixed D-Li site could play an important role in stabilizing the low $T$ quantum fluctuating state.

cond-mat.str-el↗

arXiv2024

Electrodynamics of the quantum anomalous Hall state in a magnetically doped topological insulator

Magnetically doped topological insulators have been extensively studied over the past decade as a material platform to exhibit quantum anomalous Hall effect. Most material realizations are magnetically doped and despite material advances suffer from large disorder effects. In such systems, it is believed that magnetic disorder leads to a spatially varying Dirac mass gap and chemical potential fluctuations, and hence quantized conductance is only observed at very low temperatures. Here, we use a recently developed high-precision time-domain terahertz (THz) polarimeter to study the low-energy electrodynamic response of Cr-doped (Bi,Sb)$_2$Te$_3$ thin films. These films have been recently shown to exhibit a dc quantized anomalous Hall response up to T = 2 K at zero gate voltage. We show that the real part of the THz range Hall conductance $σ_{xy}(ω)$ is slightly smaller than $e^2/h$ down to T = 2 K with an unconventional decreasing dependence on frequency. The imaginary (dissipative) part of $σ_{xy}(ω)$ is small, but increasing as a function of omega. We connect both aspects of our data to a simple model for effective magnetic gap disorder. Our work highlights the different effect that disorder can have on the dc vs. ac quantum anomalous Hall effect.

cond-mat.mes-hall↗

arXiv2023

Energy Relaxation and dynamics in the correlated metal Sr$_2$RuO$_4$ via THz two-dimensional coherent spectroscopy

Separating out the contributions of different scattering channels in strongly interacting metals is crucial in identifying the mechanisms that govern their properties. While momentum or current relaxation rates can be readily probed via \textit{dc} resistivity or optical/THz spectroscopy, distinguishing different kinds of inelastic scattering can be more challenging. Using nonlinear THz 2D coherent spectroscopy, we measure the rates of energy relaxation after THz excitation in the strongly interacting Fermi liquid, Sr$_2$RuO$_4$. Energy relaxation is a bound on the total scattering and specifically a measure of contributions to the electron self-energy that arise from {\it inelastic} coupling to a bath. We observe two distinct energy relaxation channels: a fast process that we interpret as energy loss to the phonon system and a much slower relaxation that we interpret as arising from a non-equilibrium phonon effects and subsequent heat loss through diffusion. Interestingly, even the faster energy relaxation rate is at least an order of magnitude slower than the overall momentum relaxation rate, consistent with strong electron interactions and the dominance of energy-conserving umklapp or interband electron-electron scattering in momentum relaxation. The slowest energy relaxation rate decays on a sub-GHz scale, consistent with the relaxation dynamics of non-equilibrium phonons. Our observations reveal the versatility of nonlinear THz spectroscopy to measure the energy relaxation dynamics in correlated metals. Our work also highlights the need for improved theoretical understanding of such processes in interacting metals.

cond-mat.str-el↗

arXiv2023

High-precision measurements of terahertz polarization states with a fiber coupled time-domain THz spectrometer

We present a new method for high precision measurements of polarization rotation in the frequency range from 0.2 to 2.2 THz using a fiber coupled time-domain THz spectrometer. A free standing wire-grid polarizer splits THz light into orthogonal components which are then measured by two separate detectors simultaneously. We theoretically model the uncertainties introduced by optical component non-idealities and predict that we may expect to achieve precisions of order 2.3 $μ$rad (0.13 mdeg) and accuracies of 0.8$\%$ when anti-symmetrizing the response with respect to an applied field. Anti-symmetrization improves precision by more than four orders of magnitude. We demonstrate this method on a 2D electron gas in magnetic field and show that we achieve a precision of 20 $μ$rad (1.1 mdeg) for small polarization rotation angles. A detailed description of the technique and data analysis procedure is provided, demonstrating its capability to precisely measure polarization states in the 0.2 to 2.2 THz range.

physics.optics↗

arXiv2022

Evolution of the cyclotron mass with doping in La$_{2-x}$Sr$_x$CuO$_4$

The recent observation of cyclotron resonance in optimally-doped La$_{2-x}$Sr$_x$CuO$_4$ using time-domain THz spectroscopy in high magnetic field has given new possibilities for the study of cuprate superconductors. One can measure the cyclotron mass in more disordered cuprates possesing short scattering times therefore expanding the study to materials and dopings in which quantum oscillations have not been observed. Here we present the measurement of the carrier mass of the hole doped cuprate La$_{2-x}$Sr$_x$CuO$_4$ across a a range of dopings spanning the slightly underdoped ($x=0.13$) to highly overdoped ($x=0.26$), near to the termination of the superconducting dome. These results reveal a systematic increase of $m_c$ with doping, up to values greater than thirteen times the bare electron mass. This is in contrast with those masses extracted from the heat capacity, which show a peak near the pseudogap critical point $p^*$ and/or Lifshitz transition. The cyclotron frequency is linear in field up to 31 T for all dopings giving no evidence for field induced Fermi surface reconstructions. The cyclotron mass is found to be positive for all dopings, but with a magnitude systematically below the heat capacity mass for under and optimally doped samples, while exceeding it for overdoped samples. Among other aspects, these results are surprising as photoemission reveals a Lifshitz transition in the middle of our doping range and the sign of the cyclotron mass determined from a finite frequency resonance is -- in conventional theories -- a {\it topological quantity} only sensitive to whether or not the Fermi surface is closed around holes or electrons. We see no sign of a divergence of the mass near $p^*$ nor near the Lifshitz transition, showing that any singularity -- if it exists -- is not strong enough to affect the cyclotron mass.

cond-mat.supr-con↗

arXiv2022

Disorder-enhanced effective masses and deviations from Matthiessen's rule in PdCoO$_2$ thin films

The observation of hydrodynamic transport in the metallic delafossite PdCoO$_2$ has increased interest in this family of highly conductive oxides, but experimental studies so far have mostly been confined to bulk crystals. In this work, the development of high-quality thin films of PdCoO$_2$ has enabled a thorough study of the conductivity as a function of film thickness using both dc transport and time-domain THz spectroscopy. With increasing film thickness from 12 nm to 102 nm, the residual resistivity decreases and we observe a large deviation from Matthiessen's rule (DMR) in the temperature dependence of the resistivity. We find that the complex THz conductivity is well fit by a single Drude term. We fit the data to extract the spectral weight and scattering rate simultaneously. The temperature dependence of the Drude scattering rate is found to be nearly independent of the residual resistivity and cannot be the primary mechanism for the observed DMR. Rather, we observe large changes in the spectral weight as a function of disorder, changing by a factor of 1.5 from the most disordered to least disordered films. We believe this corresponds to a mass enhancement of $\geq 2$ times the value of the bulk effective mass which increases with residual disorder. This suggests that the mechanism behind the DMR observed in dc resistivity is primarily driven by changes in the electron mass. We discuss the possible origins of this behavior including the possibility of disorder-enhanced electron-phonon scattering, which can be systematically tuned by film thickness.

cond-mat.str-el↗

arXiv2022

Magnetic phase crossover in strongly correlated EuMn2P2

Strong electron correlations underlie a plethora of electronic and magnetic components and devices and are often used to identify and probe novel ground states in quantum materials. Herein we report a magnetic phase crossover in EuMn2P2, an insulator which shows Eu antiferromagnetism at TN=17K, but no phase transition attributed to Mn magnetism. The absence of a Mn magnetic phase transition contrasts with the formation of long-range Mn order at T=130K in isoelectronic EuMn2Sb2 and EuMn2As2. Temperature-dependent specific heat and 31P NMR measurements provide evidence for the development of Mn magnetic correlations from T=250-100 K. Density functional theory calculations demonstrate an unusual sensitivity of the band structure to the details of the imposed Mn and Eu magnetic order, with antiferromagnetic Mn order required to recapitulate an insulating state. Our results imply a picture in which long range Mn magnetic order is suppressed by chemical pressure, but that magnetic correlations persist, narrowing bands and producing an insulating state.

cond-mat.str-el↗

arXiv2022

Magnetic Excitations and Interactions in the Kitaev Hyperhoneycomb Iridate $β$-Li$_2$IrO$_3$

We present a thorough experimental study of the three-dimensional hyperhoneycomb Kitaev magnet $β$-Li$_2$IrO$_3$, using a combination of inelastic neutron scattering (INS), time-domain THz spectroscopy, and heat capacity measurements. The main results include a massive low-temperature reorganization of the INS spectral weight that evolves into a broad peak centered around 12 meV, and a distinctive peak in the THz data at 2.8(1) meV. A detailed comparison to powder-averaged spin-wave theory calculations reveals that the positions of these two features are controlled by the anisotropic $Γ$ coupling and the Heisenberg exchange $J$, respectively. The refined microscopic spin model places $β$-Li$_2$IrO$_3$ in close proximity to the Kitaev spin liquid phase.

cond-mat.str-el↗

arXiv2022

Quantum Critical Magnetic Excitations in Spin-1/2 and Spin-1 Chain Systems

The study of CoNb$_2$O$_6$ sits at the confluence of simplicity and complexity: on one hand, the model for Ising chains -- the building blocks of CoNb$_2$O$_6$ -- in a transverse field, can be exactly solved and, thus, serves as an archetype of quantum criticality; on the other hand, the weak but nonzero interchain coupling adds geometric frustration to the stage, substantially complicating the phase diagram. Here we utilize low-temperature specific heat and thermal conductivity measurements to study the low-lying magnetic excitations in CoNb$_2$O$_6$ and its spin-1 analogue NiNb$_2$O$_6$. The thermal conductivity is found to be suppressed around the quantum critical point, where the specific heat is enhanced due to gapless magnetic excitations, pointing to the localized nature of the latter. These results highlight the predominant role of frustration in determining the quantum critical magnetic excitations of spin chains, which may furthermore underlie the remarkable similarities between the phenomenology of these spin-1/2 and spin-1 systems.

cond-mat.str-el↗

arXiv2022

A magnetic continuum observed by terahertz spectroscopy in a quantum spin liquid candidate BaCo$_2$(AsO$_4$)$_2$

Quantum spin liquids (QSLs) are topologically ordered exotic states of matter that host fractionalized excitations. Kitaev proposed a particular route towards a QSL via strongly bond-dependent interactions on the hexagonal lattice. A number of candidate Kitaev QSL materials have been pursued, but all have appreciable non-Kitaev interactions, which put these systems far from the QSL regime. Using time-domain terahertz spectroscopy (TDTS) we observed a broad magnetic continuum over a wide range of temperature and field in the honeycomb cobalt-based magnet, BaCo$_2$(AsO$_4$)$_2$, which has been proposed to be more ideal versions of a Kitaev QSL. Applying a small in-plane magnetic field of $\sim$ 0.5 T suppresses the magnetic order and at at even higher fields gives rise to a spin-polarized state. With 4T magnetic field oriented principally out-of-plane, a broad magnetic continuum was observed that could be consistent with a field induced QSL. Our results indicate BaCo$_2$(AsO$_4$)$_2$ to be a promising QSL candidate.

cond-mat.str-el↗

arXiv2022

Anomalous Residual Surface Conductivity in a Superconductor with Strong Spin-Orbit Coupling

Conventional BCS superconductors are expected to exhibit a conductivity with vanishing dissipation with decreasing temperature. While bulk physical properties measurements indicate PdPb$_{2}$ is a conventional superconductor with a $T_c$ of 3.0 K, measurements of surface impedance through the microwave cavity perturbation technique indicate a large, non-vanishing dissipative component below $T_c$ that is at odds with conventional superconductivity. We demonstrate PdPb$_2$ to be a possible topological superconductor with a fully gapped bulk and a dissipative Majorana fluid surface.

cond-mat.supr-con↗

arXiv2022

Anomalous high-temperature THz nonlinearity in superconductors near the metal-insulator transition

The interplay of strong disorder and superconductivity is a topic of long-term interest in condensed matter physics. Here we explore the nonlinear THz response of superconducting NbN films close to the 3D metal-insulator transition. For the least disordered samples, the magnitude of the nonlinear $χ^{(3)}$ response follows the temperature dependence of the superfluid density as expected. In contrast, for high disorder samples near the metal-insulator transition the $χ^{(3)}$ nonlinearity persists to temperatures as high as even 4 times the $T_c$ of the cleanest sample. We discuss the possible origins of this remarkably large nonlinearity, including the possibility that it arises in an enhancement of the temperature scales of superconductivity close to localization. Our work highlights the importance of finite frequency nonlinear THz experiments in detecting superconducting correlations even into regions where long-range ordered superconductivity does not persist.

cond-mat.supr-con↗

arXiv2022

Effect of radiation-induced defects on the superfluid density and optical conductivity of overdoped La$_{2-x}$Sr$_x$CuO$_4$

Using a combination of time-domain THz spectroscopy (TDTS) and mutual inductance measurements, we have investigated the low-energy electrodynamic response of overdoped La$_{2-x}$Sr$_x$CuO$_4$ films that have been exposed to ion irradiation. Films went through three rounds of irradiation (2, 4, and 6 $\times 10^{13}$ ions/cm$^2$) and mutual inductance and TDTS experiments were performed between each step. Together with the as-grown film, this gives four different levels of disorder. The transport scattering rate that is measured directly in the THz experiments is an approximately linear function of the radiation dose at all temperatures. This is consistent with a proportionate increase in elastic scattering. In the superconducting state we find that the relation between $T_c$, the superfluid density, and the scattering rates are quantitatively at odds with the predictions based on the extant theory of Abrikosov-Gorkov-like pair breaking in a dirty $d$-wave superconductor. Increasing disorder causes only a small change in the superconducting transition temperature for the overdoped films, but the changes to the $ω\sim 0$ superfluid density are much larger.

cond-mat.supr-con↗

arXiv2022

Measurements of cyclotron resonance of the interfacial states in strong spin-orbit coupled 2D electron gases proximitized with aluminum

Two-dimensional electron gasses (2DEG) in InAs quantum wells proximitized by aluminum are promising platforms for topological qubits based on Majorana zero modes. However, there are still substantial uncertainties associated with the nature of the electronic states at the interfaces of these systems. It is challenging to probe the properties of these hybridized states as they are buried under a relatively thick aluminum layer. In this work, we have investigated a range of InAs/In$ _{1-\text{x}} $Ga$ _\text{x} $As heterostructures with Al overlayers using high precision time-domain THz spectroscopy. Despite the thick metallic overlayer, we observe a prominent cyclotron resonance in the magnetic field that can be associated with the response of the interfacial states. Measurements of the THz range complex Faraday rotation allow the extraction of the sign and magnitude of the effective mass, the density of charge carriers, and scattering times of the 2DEG despite the close proximity of the aluminum layer. We discuss the extracted band parameters and connect their values to the known physics of these materials.

cond-mat.mes-hall↗