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R. D. Averitt

Publications and source records attributed to R. D. Averitt.

At least 19 recordsLinked to original sources

Magnetic Order Driven Ultrafast Phase Transition in NdNiO$_3$

Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO$_3$ (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an IMT. During the course of the photoinduced insulator to metal transition (IMT) with above gap excitation, we observe an ultrafast ($<$ 180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by X-ray absorption and THz transmission (~ 450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory (DFT) calculations reveal a consistent scenario where optically driven inter-site charge transfer (ICT) drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide new modalities for control of electronic phase transitions in quantum materials based on ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation.

cond-mat.str-el

Decoupling of static and dynamic criticality in a driven Mott insulator

Dynamically driven interacting quantum many-body systems have the potential to exhibit properties that defy the laws of equilibrium statistical mechanics. A widely studied model is the impulsively driven antiferromagnetic Mott insulator, which is predicted to realize exotic transient phenomena including dynamical phase transitions into thermally forbidden states and highly non-thermal magnon distributions. However such far-from-equilibrium regimes, where conventional time-dependent Ginzburg-Landau descriptions fail, are experimentally challenging to prepare and to probe especially in solid state systems. Here we use a combination of time-resolved second harmonic optical polarimetry and coherent magnon spectroscopy to interrogate $n$-type photo-doping induced ultrafast magnetic order parameter dynamics in the Mott insulator Sr$_2$IrO$_4$. We uncover an unusual far-from-equilibrium critical regime in which the divergences of the magnetic correlation length and relaxation time are decoupled. This violation of conventional thermal critical behavior arises from the interplay of photo-doping and non-thermal magnon population induced demagnetization effects. Our findings, embodied in a non-equilibrium "phase diagram", provide a blueprint for engineering the out-of-equilibrium properties of quantum matter, with potential applications to terahertz spintronics technologies.

cond-mat.str-el

Magneto-Elastic Coupling to Coherent Acoustic Phonon Modes in Ferrimagnetic Insulator GdTiO$_3$

In this work we investigate single crystal GdTiO$_{3}$, a promising candidate material for Floquet engineering and magnetic control, using ultrafast optical pump-probe reflectivity and magneto-optical Kerr spectroscopy. GdTiO${}_{3}$ is a Mott-Hubbard insulator with a ferrimagnetic and orbitally ordered ground state (\textit{T${}_{C}$} = 32 K). We observe multiple signatures of the magnetic phase transition in the photoinduced reflectivity signal, in response to above band-gap 660 nm excitation. Magnetic dynamics measured via Kerr spectroscopy reveal optical perturbation of the ferrimagnetic order on spin-lattice coupling timescales, highlighting the competition between the Gd${}^{3+}$ and Ti${}^{3+}$ magnetic sub-lattices. Furthermore, a strong coherent oscillation is present in the reflection and Kerr dynamics, attributable to an acoustic strain wave launched by the pump pulse. The amplitude of this acoustic mode is highly dependent on the magnetic order of the system, growing sharply in magnitude at \textit{T${}_{C}$}, indicative of strong magneto-elastic coupling. The driving mechanism, involving strain-induced modification of the magnetic exchange interaction, implies an indirect method of coupling light to the magnetic degrees of freedom and emphasizes the potential of GdTiO${}_{3}$ as a tunable quantum material.

cond-mat.str-el

Influence of spin and orbital fluctuations on Mott-Hubbard exciton dynamics in LaVO${}_{3}$ Thin Films

Recent optical conductivity measurements reveal the presence of Hubbard excitons in certain Mott insulators. In light of these results, it is important to revisit the dynamics of these materials to account for excitonic correlations. We investigate time-resolved excitation and relaxation dynamics as a function of temperature in perovskite-type LaVO${}_{3}$ thin films using ultrafast optical pump-probe spectroscopy. LaVO${}_{3}$ undergoes a series of phase transitions at roughly the same critical temperature $T_C\cong 140\ K$, including a second-order magnetic phase transition (PM $\xrightarrow{}$ AFM) and a first-order structural phase transition, accompanied by \textit{C}-type spin order (SO) and \textit{G}-type orbital order (OO). Ultrafast optical pump-probe spectroscopy at 1.6 eV monitors changes in the spectral weight of the Hubbard exciton resonance which serves as a sensitive reporter of spin and orbital fluctuation dynamics. We observe dramatic slowing down of the spin, and orbital dynamics in the vicinity of $T_C\cong 140$ K, reminiscent of a second-order phase transition, despite the (weakly) first-order nature of the transition. We emphasize that since it is spectral weight changes that are probed, the measured dynamics are not reflective of conventional exciton generation and recombination, but are related to the dynamics of Hubbard exciton formation in the presence of a fluctuating many-body environment.

cond-mat.str-el

Multi-messenger nano-probes of hidden magnetism in a strained manganite

The ground state properties of correlated electron systems can be extraordinarily sensitive to external stimuli, such as temperature, strain, and electromagnetic fields, offering abundant platforms for functional materials. We present a metastable and reversible photoinduced ferromagnetic transition in strained films of the doped manganite La(2/3)Ca(1/3)MnO3. Using the novel multi-messenger combination of atomic force microscopy, cryogenic scanning near-field optical microscopy, magnetic force microscopy, and ultrafast laser excitation, we demonstrate both "writing" and "erasing" of a metastable ferromagnetic metal phase with nanometer-resolved finesse. By tracking both optical conductivity and magnetism at the nano-scale, we reveal how spontaneous strain underlies the thermal stability, persistence, and reversal of this photoinduced metal. Our first-principles electronic structure calculations reveal how an epitaxially engineered Jahn-Teller distortion can stabilize nearly degenerate antiferromagnetic insulator and ferromagnetic metal phases. We propose a Ginzburg-Landau description to rationalize the co-active interplay of strain, lattice distortion, and magnetism we resolve in strained LCMO, thus guiding future functional engineering of epitaxial oxides like manganites into the regime of phase-programmable materials.

cond-mat.mes-hall

Ultrafast enhancement of ferromagnetic spin exchange induced by ligand-to-metal charge transfer

Directly modifying spin exchange energies in a magnetic material with light can enable ultrafast control of its magnetic states. Current approaches rely on tuning charge hopping amplitudes that mediate exchange by optically exciting either virtual or real charge-transfer transitions (CT) between magnetic sites. Here we show that when exchange is mediated by a non-magnetic ligand, it can be substantially enhanced by optically exciting a real CT transition from the ligand to magnetic site, introducing lower order virtual hopping contributions. We demonstrate sub-picosecond enhancement in a superexchange dominated ferromagnet CrSiTe3 through this mechanism using phase-resolved coherent phonon spectroscopy. This technique can also be applied in the paramagnetic phase to disentangle light induced exchange modification from other ultrafast effects that alter the magnetization. This protocol can potentially be broadly applied to engineer thermally inaccessible spin Hamiltonians in superexchange dominated magnets.

cond-mat.str-el

Ultrafast Polaron Dynamics in Layered and Perovskite Manganites: 2D and 3D Polarons

We have studied the sub-picosecond quasiparticle dynamics in the perovskite manganite La0.7Ca0.3MnO3 and the layered manganite La1.4Sr1.6Mn2O7 using ultrafast optical spectroscopy. We found that for T > TC, initial relaxation proceeds on the time scale of several hundred femtoseconds and corresponds to the redressing of a photoexcited electron to its polaronic ground state. The temperature and dimensionality dependence of this polaron redressing time provides insight into the relationship between polaronic motion and spin dynamics on a sub-picosecond time scale. We also observe a crossover to a more conventional electron-phonon relaxation in the ferromagnetic metallic phase below Tc.

cond-mat.str-el

Ultrafast THz Field Control of Electronic and Structural Interactions in Vanadium Dioxide

Vanadium dioxide, an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally-driven physics. Using ultrafast optical spectroscopy and x-ray scattering we show that these processes can be disentangled in the time domain. Specifically, following intense sub-picosecond electric-field excitation, a partial collapse of the insulating gap occurs within the first ps. Subsequently, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a novel method to control electronic interactions in correlated materials on an ultrafast timescale.

cond-mat.str-el

Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors

We present a comparative study of ultrafast photo-conversion dynamics in tetracene (Tc) and pentacene (Pc) single crystals and Pc films using optical pump-probe spectroscopy. Photo-induced absorption in Tc and Pc crystals is activated and temperature-independent respectively, demonstrating dominant singlet-triplet exciton fission. In Pc films (as well as C$_{60}$-doped films) this decay channel is suppressed by electron trapping. These results demonstrate the central role of crystallinity and purity in photogeneration processes and will constrain the design of future photovoltaic devices.

cond-mat.other

Magnetic exchange interaction between rare-earth and Mn ions in multiferroic hexagonal manganites

We report a study of magnetic dynamics in multiferroic hexagonal manganite HoMnO3 by far-infrared spectroscopy. Low-temperature magnetic excitation spectrum of HoMnO3 consists of magnetic-dipole transitions of Ho ions within the crystal-field split J=8 manifold and of the triangular antiferromagnetic resonance of Mn ions. We determine the effective spin Hamiltonian for the Ho ion ground state. The magnetic-field splitting of the Mn antiferromagnetic resonance allows us to measure the magnetic exchange coupling between the rare-earth and Mn ions.

cond-mat.mtrl-sci

Detection of coherent magnons via ultrafast pump-probe reflectance spectroscopy in multiferroic Ba0.6Sr1.4Zn2Fe12O22

We report the detection of a magnetic resonance mode in multiferroic Ba0.6Sr1.4Zn2Fe12O22 using time domain pump-probe reflectance spectroscopy. Magnetic sublattice precession is coherently excited via picosecond thermal modification of the exchange energy. Importantly, this precession is recorded as a change in reflectance caused by the dynamic magnetoelectric effect. Thus, transient reflectance provides a sensitive probe of magnetization dynamics in materials with strong magnetoelectric coupling, such as multiferroics, revealing new possibilities for application in spintronics and ultrafast manipulation of magnetic moments.

cond-mat.other

Highly-flexible wide angle of incidence terahertz metamaterial absorber

We present the design, fabrication, and characterization of a metamaterial absorber which is resonant at terahertz frequencies. We experimentally demonstrate an absorptivity of 0.97 at 1.6 terahertz. Importantly, this free-standing absorber is only 16 microns thick resulting in a highly flexible material that, further, operates over a wide range of angles of incidence for both transverse electric and transverse magnetic radiation.

cond-mat.mtrl-sci

Terahertz metamaterials on free-standing highly-flexible polyimide substrates

We have fabricated resonant terahertz metamaterials on free standing polyimide substrates. The low-loss polyimide substrates can be as thin as 5.5 micron yielding robust large-area metamaterials which are easily wrapped into cylinders with a radius of a few millimeters. Our results provide a path forward for creating multi-layer non-planar metamaterials at terahertz frequencies.

cond-mat.mtrl-sci

Softening of the insulating phase near Tc for the photo-induced insulator-to-metal phase transition in vanadium dioxide

We use optical-pump terahertz-probe spectroscopy to investigate the near-threshold behavior of the photoinduced insulator-to-metal (IM) transition in vanadium dioxide thin films. Upon approaching Tc a reduction in the fluence required to drive the IM transition is observed, consistent with a softening of the insulating state due to an increasing metallic volume fraction (below the percolation limit). This phase coexistence facilitates the growth of a homogeneous metallic conducting phase following superheating via photoexcitation. A simple dynamic model using Bruggeman effective medium theory describes the observed initial condition sensitivity.

cond-mat.str-el

Coupling Between An Optical Phonon and the Kondo Effect

We explore the ultra-fast optical response of Yb_{14}MnSb_{11}, providing further evidence that this Zintl compound is the first ferromagnetic, under-screened Kondo lattice. These experiments also provide the first demonstration of coupling between an optical phonon mode and the Kondo effect.

cond-mat.str-el

Observation of Competing Order in a High-$T_{c}$ Superconductor with Femtosecond Optical Pulses

We present studies of the photoexcited quasiparticle dynamics in Tl$_{2}$Ba$_{2}$Ca$_{2}$Cu$_{3}$O$_{y}$ (Tl-2223) using femtosecond optical techniques. Deep into the superconducting state (below 40 K), a dramatic change occurs in the temporal dynamics associated with photoexcited quasiparticles rejoining the condensate. This is suggestive of entry into a coexistence phase which, as our analysis reveals, opens a gap in the density of states (in addition to the superconducting gap), and furthermore, competes with superconductivity resulting in a depression of the superconducting gap.

cond-mat.supr-con

Time-Resolved Quasiparticle Dynamics in the Spin-Density-Wave State

Time-resolved photoinduced reflectivity is measured in the spin-density-wave (SDW) phase using itinerant antiferromagnets UMGa$_{5}$ (M=Ni, Pt). For UNiGa$_{5}$ [$T_{N}$=85 K, $Q$=($π$,$π$,$π$)], the relaxation time $τ$ shows a sharp increase at $T_{N}$ consistent with the opening of a SDW gap. For UPtGa$_{5}$ [$T_{N}$=26 K, $Q$=(0,0,$π$)], no change in $τ$ is observed at $T_{N}$ or at the lowest temperatures. We attribute this to the absence of the SDW gap at the Fermi level, due to a different modulation vector $Q$, which leads to a gapless quasiparticle spectrum. Our results challenge the conventional wisdom that a SDW phase necessarily implies a SDW gap at the Fermi level.

cond-mat.str-el

Quasiparticle Relaxation Across a Spin Gap in the Itinerant Antiferromagnet UNiGa5

Ultrafast time-resolved photoinduced reflectivity is measured for the itinerant antiferromagnet UNiGa$_{5}$ ($T_{N} \approx$85 K) from room temperature to 10 K. The relaxation time $τ$ shows a sharp increase at $T_{N}$ consistent with the opening of a spin gap. In addition, the temperature dependence of $τ$ below $T_{N}$ is consistent with the opening of a spin gap leading to a quasiparticle recombination bottleneck as revealed by the Rothwarf-Taylor model. This contrasts with canonical heavy fermions such as CeCoIn$_{5}$ where the recombination bottleneck arises from the hybridization gap.

cond-mat.str-el