Photoinduced Fano-resonance of coherent phonons in zinc

Utilizing femtosecond optical pump-probe technique, we have studied transient Fano-resonance in zinc. At high excitation levels the Fourier spectrum of the coherent E$_{2g}$ phonon exhibits strongly asymmetric line shape, which is well modeled by the Fano function. The Fano parameter (1/Q) was found to be strongly excitation fluence dependent while depending weakly on the initial lattice temperature. We attribute the origin of the Fano-resonance to the coupling of coherent phonon to the electronic continuum, with their transition probabilities strongly renormalized in the vicinity of the photoinduced structural transition.Comment: 5 pages, 3 figures, to be published in Physical Review

Photoexcited electron dynamics in Kondo insulators and heavy fermions

We have studied the photoexcited carrier relaxation dynamics in the Kondo insulator SmB6 and the heavy fermion metal YbAgCu4 as a function of temperature and excitation level. The dynamic response is found to be both strongly temperature dependent and nonlinear. The data are analyzed with a Rothwarf-Taylor bottleneck model, where the dynamics are governed by the presence of a narrow gap in the density of states near the Fermi level. The remarkable agreement with the model suggests that carrier relaxation in a broad class of heavy electron systems (both metals and insulators) is governed by the presence of a (weakly temperature dependent) hybridization gap.Comment: accepted for publication in Physical Review Letter

Combined investigation of collective amplitude and phase modes in a quasi-one-dimensional charge-density-wave system over a wide spectral range

We investigate experimentally both the amplitude and phase channels of the collective modes in the quasi-1D charge-density-wave (CDW) system, K0.3MoO3, by combining (i) optical impulsive-Raman pump-probe and (ii) terahertz time-domain spectroscopy (THz-TDS), with high resolution and a detailed analysis of the full complex-valued spectra in both cases. This allows an unequivocal assignment of the observed bands to CDW modes across the THz range up to 9 THz. We revise and extend a time-dependent Ginzburg-Landau model to account for the observed temperature dependence of the modes, where the combination of both amplitude and phase modes allows one to robustly determine the bare-phonon and electron-phonon coupling parameters. While the coupling is indeed strongest for the lowest-energy phonon, dropping sharply for the immediately subsequent phonons, it grows back significantly for the higher-energy phonons, demonstrating their important role in driving the CDW formation. We also include a reassessment of our previous analysis of the lowest-lying phase modes, whereby assuming weaker electronic damping for the phase channel results in a qualitative picture more consistent with quantum-mechanical treatments of the collective modes, with a strongly coupled amplitudon and phason as the lowest modes

Highly anisotropic transient optical response of charge density wave order in ZrTe3_3

Low dimensionality in CDW systems leads to anisotropic optical properties, in both equilibrium and non-equilibrium conditions. Here we perform polarized two-color pump probe measurements on a quasi-1D material ZrTe$_3$, in order to study the anisotropic transient optical response in the CDW state. Profound in-plane anisotropy is observed with respect to polarization of probe photons. Below $T_\mathrm{CDW}$ both the quasi-particle relaxation signal and amplitude mode (AM) oscillation signal are much larger with $\mathbf{E}_\mathrm{pr}$ nearly parallel to $a$ axis ($\mathbf{E}_\mathrm{pr} \parallel a$) than for $\mathbf{E}_\mathrm{pr}$ parallel to $b$ axis ($\mathbf{E}_\mathrm{pr} \parallel b$). This reveals that $\mathbf{E}_\mathrm{pr} \parallel a$ signal is much more sensitive to the variation of the CDW gap. Interestingly, the lifetime of the AM oscillations observed with $\mathbf{E}_\mathrm{pr} \parallel b$ is longer than $\mathbf{E}_\mathrm{pr} \parallel a$. Moreover, at high pump fluence where the electronic order melts and the AM oscillations vanish for $\mathbf{E}_\mathrm{pr} \parallel a$ , the AM oscillatory response still persists for $\mathbf{E}_\mathrm{pr} \parallel b$. We discuss possible origins that lead to such unusual discrepancy between the two polarizations.Comment: 6 pages, 4 figure

Ultrafast dynamics of coherent optical phonons and nonequilibrium electrons in transition metals

The femtosecond optical pump-probe technique was used to study dynamics of photoexcited electrons and coherent optical phonons in transition metals Zn and Cd as a function of temperature and excitation level. The optical response in time domain is well fitted by linear combination of a damped harmonic oscillation because of excitation of coherent $E_{2g}$ phonon and a subpicosecond transient response due to electron-phonon thermalization. The electron-phonon thermalization time monotonically increases with temperature, consistent with the thermomodulation scenario, where at high temperatures the system can be well explained by the two-temperature model, while below $\approx$ 50 K the nonthermal electron model needs to be applied. As the lattice temperature increases, the damping of the coherent $E_{2g}$ phonon increases, while the amplitudes of both fast electronic response and the coherent $E_{2g}$ phonon decrease. The temperature dependence of the damping of the $E_{2g}$ phonon indicates that population decay of the coherent optical phonon due to anharmonic phonon-phonon coupling dominates the decay process. We present a model that accounts for the observed temperature dependence of the amplitude assuming the photoinduced absorption mechanism, where the signal amplitude is proportional to the photoinduced change in the quasiparticle density. The result that the amplitude of the $E_{2g}$ phonon follows the temperature dependence of the amplitude of the fast electronic transient indicates that under the resonant condition both electronic and phononic responses are proportional to the change in the dielectric function.Comment: 10 pages, 9 figures, to appear in Physical Review

Collective modes in the charge-density wave state of K0.3_{0.3}MoO3_3: The role of long-range Coulomb interactions revisited

We re-examine the effect of long-range Coulomb interactions on the collective amplitude and phase modes in the incommensurate charge-density wave ground state of quasi-one-dimensional conductors. Using an effective action approach we show that the longitudinal acoustic phonon protects the gapless linear dispersion of the lowest phase mode in the presence of long-range Coulomb interactions. Moreover, in Gaussian approximation amplitude fluctuations are not affected by long-range Coulomb interactions. We also calculate the collective mode dispersions at finite temperatures and compare our results with the measured energies of amplitude and phase modes in K$_{0.3}$MoO$_3$. With the exception of the lowest phase mode, the temperature dependence of the measured mode energies can be quantitatively described within a multi-phonon Fr\"{o}hlich model neglecting long-range Coulomb interactions

Dynamics of collective modes in an unconventional charge density wave system BaNi2As2

BaNi 2As 2 is a non-magnetic analogue of BaFe2 As2 , the parent compound of a prototype pnictide high-temperature superconductor, displaying superconductivity already at ambient pressure. Recent diffraction studies demonstrated the existence of two types of periodic lattice distortions above and below the triclinic phase transition, suggesting the existence of an unconventional charge-density-wave (CDW) order. The suppression of CDW order upon doping results in a sixfold increase in the superconducting transition temperature and enhanced nematic fluctuations, suggesting CDW is competing with superconductivity. Here, we apply time-resolved optical spectroscopy to investigate collective dynamics in BaNi 2 As 2. We demonstrate the existence of several CDW amplitude modes. Their smooth evolution through the structural phase transition implies the commensurate CDW order in the triclinic phase evolves from the high-temperature unidirectional incommensurate CDW, and may indeed trigger the structural phase transition. Excitation density dependence reveals excep- tional resilience of CDW against perturbation, implying an unconventional origin of the underlying electronic instability

Tracking the surface atomic motion in a coherent phonon oscillation

X-ray photoelectron diffraction is a powerful tool for determining the structure of clean and adsorbate-covered surfaces. Extending the technique into the ultrafast time domain will open the door to studies as diverse as the direct determination of the electron-phonon coupling strength in solids and the mapping of atomic motion in surface chemical reactions. Here we demonstrate time-resolved photoelectron diffraction using ultrashort soft X-ray pulses from the free electron laser FLASH. We collect Se 3d photoelectron diffraction patterns over a wide angular range from optically excited Bi$_2$Se$_3$ with a time resolution of 140 fs. Combining these with multiple scattering simulations allows us to track the motion of near-surface atoms within the first 3 ps after triggering a coherent vibration of the A$_{1g}$ optical phonons. Using a fluence of 4.2 mJ/cm$^2$ from a 1.55 eV pump laser, we find the resulting coherent vibrational amplitude in the first two interlayer spacings to be on the order of 1 pm