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

Observation of a metal-to-insulator transition with both Mott-Hubbard and Slater characteristics in Sr_2IrO_4 from time-resolved photocarrier dynamics

We perform a time-resolved optical study of Sr_2IrO_4 to understand the influence of magnetic ordering on the low energy electronic structure of a strongly spin-orbit coupled J_(eff) = 1/2 Mott insulator. By studying the recovery dynamics of photoexcited carriers, we find that upon cooling through the Néel temperature T_N the system evolves continuously from a metal-like phase with fast (∼50 fs) and excitation density independent relaxation dynamics to a gapped phase characterized by slower (∼500 fs) excitation density-dependent bimolecular recombination dynamics, which is a hallmark of a Slater-type metal-to-insulator transition. However our data indicate that the high energy reflectivity associated with optical transitions into the unoccupied J_(eff) = 1/2 band undergoes the sharpest upturn at TN, which is consistent with a Mott-Hubbard type metal-to-insulator transition involving spectral weight transfer into an upper Hubbard band. These findings show Sr_2IrO_4 to be a unique system in which Slater- and Mott-Hubbard-type behaviors coexist and naturally explain the absence of anomalies at T_N in transport and thermodynamic measurements

Nonlinear optical probe of tunable surface electrons on a topological insulator

We use ultrafast laser pulses to experimentally demonstrate that the second-order optical response of bulk single crystals of the topological insulator Bi$_2$Se$_3$ is sensitive to its surface electrons. By performing surface doping dependence measurements as a function of photon polarization and sample orientation we show that second harmonic generation can simultaneously probe both the surface crystalline structure and the surface charge of Bi$_2$Se$_3$. Furthermore, we find that second harmonic generation using circularly polarized photons reveals the time-reversal symmetry properties of the system and is surprisingly robust against surface charging, which makes it a promising tool for spectroscopic studies of topological surfaces and buried interfaces

α\alpha-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 $\alpha$ 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

Tracking Cooper Pairs in a Cuprate Superconductor by Ultrafast Angle-Resolved Photoemission

In high-temperature superconductivity, the process that leads to the formation of Cooper pairs, the fundamental charge carriers in any superconductor, remains mysterious. We use a femtosecond laser pump pulse to perturb superconducting Bi2Sr2CaCu2O8+{\delta}, and study subsequent dynamics using time- and angle-resolved photoemission and infrared reflectivity probes. Gap and quasiparticle population dynamics reveal marked dependencies on both excitation density and crystal momentum. Close to the d-wave nodes, the superconducting gap is sensitive to the pump intensity and Cooper pairs recombine slowly. Far from the nodes pumping affects the gap only weakly and recombination processes are faster. These results demonstrate a new window into the dynamical processes that govern quasiparticle recombination and gap formation in cuprates.Comment: 22 pages, 9 figure

Theoretical and experimental study of second harmonic generation from the surface of the topological insulator Bi_2Se_3

We develop a theoretical model that describes the second harmonic generation of light from the surface of the topological insulator Bi_2Se_3 and experimentally demonstrate that the technique is sensitive to the surface electrons. By performing a crystal symmetry analysis of Bi_2Se_3 (111) we determine the nonlinear electric susceptibility tensor elements that give rise to second harmonic generation. Using these results, we present a phenomenological model that shows that the relative magnitudes of these tensor elements can be determined by measuring the polarization and intensity of the radiated second harmonic light as a function of the in-plane crystal orientation and incident laser polarization. We describe optical techniques capable of isolating second harmonic light and, using these techniques, we measure the first-order linear optical and second-order nonlinear optical responses as a function of crystal orientation and laser polarization on bulk single crystals of Bi_2Se_3 (111). The experimental results are consistent with our theoretical description. By comparing the data to our theoretical model we determine that a portion of the measured second harmonic light originates from the accumulation region of Bi_2Se_3 (111), which we confirm by performing surface doping-dependent studies. Our results show that second harmonic generation is a promising tool for spectroscopic studies of topological surfaces and buried interfaces

Stress distribution and the fragility of supercooled melts

We formulate a minimal ansatz for local stress distribution in a solid that includes the possibility of strongly anharmonic short-length motions. We discover a broken-symmetry metastable phase that exhibits an aperiodic, frozen-in stress distribution. This aperiodic metastable phase is characterized by many distinct, nearly degenerate configurations. The activated transitions between the configurations are mapped onto the dynamics of a long range classical Heisenberg model with 6-component spins and anisotropic couplings. We argue the metastable phase corresponds to a deeply supercooled non-polymeric, non-metallic liquid, and further establish an order parameter for the glass-to-crystal transition. The spin model itself exhibits a continuous range of behaviors between two limits corresponding to frozen-in shear and uniform compression/dilation respectively. The two regimes are separated by a continuous transition controlled by the anisotropy in the spin-spin interaction, which is directly related to the Poisson ratio $\sigma$ of the material. The latter ratio and the ultra-violet cutoff of the theory determine the liquid configurational entropy. Our results suggest that liquid's fragility depends on the Poisson ratio in a non-monotonic way. The present ansatz provides a microscopic framework for computing the configurational entropy and relaxational spectrum of specific substances.Comment: 11 pages, 5 figures, Final version published in J Phys Chem

Giant phonon anomalies and central peak due to charge density wave formation in YBa2_2Cu3_3O6.6_{6.6}

The electron-phonon interaction is a major factor influencing the competition between collective instabilities in correlated-electron materials, but its role in driving high-temperature superconductivity in the cuprates remains poorly understood. We have used high-resolution inelastic x-ray scattering to monitor low-energy phonons in YBa$_2$Cu$_3$O$_{6.6}$ (superconducting $\bf T_c = 61$ K), which is close to a charge density wave (CDW) instability. Phonons in a narrow range of momentum space around the CDW ordering vector exhibit extremely large superconductivity-induced lineshape renormalizations. These results imply that the electron-phonon interaction has sufficient strength to generate various anomalies in electronic spectra, but does not contribute significantly to Cooper pairing. In addition, a quasi-elastic "central peak" due to CDW nanodomains is observed in a wide temperature range above and below $\bf T_c$, suggesting that the gradual onset of a spatially inhomogeneous CDW domain state with decreasing temperature is a generic feature of the underdoped cuprates