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1T-TiSe$_2$ hosts a $2 \times 2 \times 2$ charge density wave (CDW) that is known to form the state with localized domains separated by the domain walls upon Cu intercalation. The CDW state with the domain wall network has attracted significant interest due to its coexistence with superconductivity. Here we present a scanning tunneling microscopy, transport and magnetic susceptibility study of 1T-Ti$_{1-\text{x}}$Ta$_\text{x}$Se$_2$. Ta substitution for Ti atoms allows us to perform experiments over the wide range of doping ($ 0 \leqslant \text{x} \leqslant 0.2$), providing access to a significantly broader phase diagram than Cu intercalation experiments. At x = 0.02, we observe a complex network of domains and domain walls. We identify two distinct types of domain walls and show their structure with atomic resolution. Additionally, an elusive symmetry-breaking stripe CDW is found at the light substitution of x = 0.02. We also measure highly substituted x = 0.2 crystals that are superconducting despite the full collapse of the CDW order. Our results uncover rich CDW physics in Ta-substituted 1T-TiSe2 crystals and illuminate the interplay between the CDW and superconductivity., Comment: 10 pages, 4 figures

A systematic temperature dependent study of the femtosecond optical superconducting (SC) state destruction and recovery in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$ cuprate superconductor by means of the all-optical polarization-sensitive multi-pulse spectroscopy is presented. At low temperatures and a partial SC state suppression an anisotropic SC-gap recovery-timescale is suggested by the data. The SC state destruction and recovery dynamics are compared to the recent TR-ARPES-inferred SC-gap dynamics and a qualitative agreement is found. Using a phenomenological response function the experimental data are also compared to time dependent Ginzburg-Landau model simulations.

We investigated temperature and fluence dependent dynamics of the time resolved optical reflectivity in undoped spin-density-wave (SDW) and doped superconducting (SC) EuFe$_{2}$(As,P)$_{2}$ with emphasis on the ordered Eu$^{2+}$-spin temperature region. The data indicate that the SDW order coexists at low temperature with the SC and Eu$^{2+}$-ferromagnetic order. Increasing the excitation fluence leads to a thermal suppression of the Eu$^{2+}$-spin order due to the crystal-lattice heating while the SDW order is suppressed nonthermally at a higher fluence.

Temperature and fluence dependence of the 1.55-eV optical transient reflectivity in BaFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ was measured and analysed in the low and high excitation density limit. The effective magnitude of the superconducting gap of $\sim 5$ meV obtained from the low-fluence-data bottleneck model fit is consistent with the ARPES results for the $\gamma$-hole Fermi surface. The superconducting-state nonthermal optical destruction energy was determined from the fluence dependent data. The in-plane optical destruction energy scales well with T$_{\mathrm{c}}^{2}$ and is found to be similar in a number of different layered superconductors.

Ferromagnetism and superconductivity are antagonistic phenomena. Their coexistence implies either a modulated ferromagnetic order parameter on a lengthscale shorter than the superconducting coherence length or a weak exchange coupling between the itinerant superconducting electrons and the localized ordered spins. In some iron based pnictide superconductors the coexistence of ferromagnetism and superconductivity has been clearly demonstrated. The nature of the coexistence, however, remains elusive since no clear understanding of the spin structure in the superconducting state has been reached and the reports on the coupling strength are controversial. We show, by a direct optical pump-probe experiment, that the coupling is weak, since the transfer of the excess energy from the itinerant electrons to ordered localized spins is much slower than the electron-phonon relaxation, implying the coexistence without the short-lengthscale ferromagnetic order parameter modulation. Remarkably, the polarization analysis of the coherently excited spin wave response points towards a simple ferromagnetic ordering of spins with two distinct types of ferromagnetic domains.

We systematically investigate temperature- and spectrally-dependent optical reflectivity dynamics in AAs$_{2}$Fe$_{2}$, (A=Ba, Sr and Eu), iron-based superconductors parent spin-density-wave (SDW) compounds. Two different relaxation processes are identified. The behavior of the slower process, which is strongly sensitive to the magneto-structural transition, is analyzed in the framework of the relaxation-bottleneck model involving magnons. The results are compared to recent time resolved angular photoemission results (TR-ARPES) and possible alternative assignment of the slower relaxation to the magneto-structural order parameter relaxation is discussed.

The dynamics of excitations with different symmetry is investigated in the superconducting (SC) and normal state of the high-temperature superconductor Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+\delta}$ (Bi2212) using optical pump-probe (Pp) experiments with different light polarizations at different doping levels. The observation of distinct selection rules for SC excitations, present in A$_{{\rm 1g}}$ and B$_{{\rm 1g}}$ symmetries, and for the PG excitations, present in A$_{{\rm 1g}}$ and B$_{{\rm 2g}}$ symmetries, by the probe and absence of any dependence on the pump beam polarization leads to the unequivocal conclusion of the existence of a spontaneous spatial symmetry breaking in the pseudogap (PG) state.

We investigate temperature and fluence dependent dynamics of the photoexcited quasi-particle relaxation and low-energy electronic structure in electron-doped 1111-structure Sm(Fe_{0.93}Co_{0.07})AsO single crystal. We find that the behavior is qualitatively identical to the 122-structure Ba(Fe,Co)_{2}As_{2} including the presence of a normal state pseudogap and a marked 2-fold symmetry breaking in the tetragonal phase that we relate to the electronic nematicity. The 2-fold symmetry breaking appears to be a general feature of the electron doped iron pnictides.

Systems which rapidly evolve through symmetry-breaking transitions on timescales comparable to the fluctuation timescale of the single-particle excitations may behave very differently than under controlled near-ergodic conditions. A real-time investigation with high temporal resolution may reveal new insights into the ordering through the transition that are not available in static experiments. We present an investigation of the system trajectory through a normal-to-superconductor transition in a prototype high-temperature superconducting cuprate in which such a situation occurs. Using a multiple pulse femtosecond spectroscopy technique we measure the system trajectory and time-evolution of the single-particle excitations through the transition in La$_{1.9}$Sr$_{0.1}$CuO$_{4}$ and compare the data to a simulation based on time-dependent Ginzburg-Landau theory, using laser excitation fluence as an adjustable parameter controlling the quench conditions in both experiment and theory. The comparison reveals the presence of significant superconducting fluctuations which precede the transition on short timescales. By including superconducting fluctuations as a seed for the growth of superconducting order we can obtain a satisfactory agreement of the theory with the experiment. Remarkably, the pseudogap excitations apparently play no role in this process.

We use femtosecond optical spectroscopy to systematically measure the primary energy relaxation rate k1 of photoexcited carriers in cuprate and pnictide superconductors. We find that k1 increases monotonically with increased negative strain in the crystallographic a-axis. Generally, the Bardeen-Shockley deformation potential theorem and, specifically, pressure-induced Raman shifts reported in the literature suggest that increased negative strain enhances electron-phonon coupling, which implies that the observed direct correspondence between a and k1 is consistent with the canonical assignment of k1 to the electron-phonon interaction. The well-known non-monotonic dependence of the superconducting critical temperature Tc on the a-axis strain is also reflected in a systematic dependence Tc on k1, with a distinct maximum at intermediate values (~16 ps-1 at room temperature). The empirical non-monotonic systematic variation of Tc with the strength of the electron-phonon interaction provides us with unique insight into the role of electron-phonon interaction in relation to the mechanism of high-Tc superconductivity as a crossover phenomenon., Comment: manuscript as accepted in PRX, main paper (20 pages, 3 figures) plus supplementary material (25 pages, 19 figures)

The processes leading to nonthermal condensate vaporization and charge-density wave (CDW) melting with femtosecond laser pulses is systematically investigated in different materials. We find that vaporization is relatively slow (tau_v ~ 1 ps) and inefficient in superconductors, exhibiting a strong systematic dependence of the vaporization energy Uv on Tc. In contrast, melting of CDW order proceeds rapidly (tau_m = 50 ~ 200 fs) and more efficiently. A quantitative model describing the observed systematic behavior in superconductors is proposed based on a phonon-mediated quasi-particle (QP) bottleneck mechanism. In contrast, Fermi surface disruption by hot QPs is proposed to be responsible for CDW state melting.

We systematically investigate the photoexcited (PE) quasi-particle (QP) relaxation and low-energy electronic structure in electron doped Ba(Fe_{1-x}Co_{x})_{2}As_{2} single crystals as a function of Co doping, 0<= x <=0.11. The evolution of the photoinduced reflectivity transients with $x$ proceeds with no abrupt changes. In the orthorhombic spin-density-wave (SDW) state a bottleneck associated with a partial charge-gap opening is detected, similar to previous results in different SDW iron-pnictides. The relative charge gap magnitude decreases with increasing x. In the superconducting (SC) state an additional relaxational component appears due to a partial (or complete) destruction of the SC state proceeding on a sub-0.5-picosecond timescale. From the SC component saturation behavior the optical SC-state destruction energy, U_p/k_B=0.3 K/Fe, is determined near the optimal doping. The subsequent relatively slow recovery of the SC state indicates clean SC gaps. The T-dependence of the transient reflectivity amplitude in the normal state is consistent with the presence of a pseudogap in the QP density of states. The polarization anisotropy of the transients suggests that the pseudogap-like behavior might be associated with a broken point symmetry resulting from nematic electronic fluctuations persisting up to T~200 K at any x. The second moment of the Eliashberg function, obtained from the relaxation rate in the metallic state at higher temperatures, indicates a moderate electron phonon coupling, lambda <~0.3, that decreases with increasing doping.

We investigate the quasiparticle relaxation and low-energy electronic structure in undoped SrFe_2As_2 exhibiting spin-density wave (SDW) ordering using optical pump-probe femtosecond spectroscopy. A remarkable critical slowing down of the quasiparticle relaxation dynamics at the SDW transition temperature T_SDW = 200K is observed. From temperature dependence of the transient reflectivity amplitude we determine the SDW-state charge gap magnitude, 2Delta_SDW/k_BT_SDW=7.2+-1. The second moment of the Eliashberg function, lambda<(hbar omega)^2>=110+-10meV^2, determined from the relaxation time above T_SDW, is similar to SmFeAsO and BaFe_2As_2 indicating a rather small electron phonon coupling constant unless the electron-phonon spectral function (alpha^2F(omega) is strongly enhanced in the low-energy phonon region.

The 2D lattice gas model with competing short and long range interactions is appliedused for calculation of the incoherent charge transport in the classical strongly-correlated charge segregated polaronic state. We show, by means of Monte-Carlo simulations, that at high temperature the transport is dominated by hopping of the dissociated correlated polarons, where with thetheir mobility is inversely proportional to the temperature. At the temperatures below the clustering transition temperature the bipolaron transport becomes dominant. The energy barrier for the bipolaron hopping is determined by the Coulomb effects and is found to be lower than the barrier for the single-polaron hopping. This leads to drastically different temperature dependencies of mobilities for polarons and bipolarons at low temperatures.

We investigate the quasiparticle relaxation and low-energy electronic structure in undoped SmFeAsO and near-optimally doped SmFeAsO_{0.8}F_{0.2} single crystals - exhibiting spin-density wave (SDW) ordering and superconductivity respectively - using pump-probe femtosecond spectroscopy. In the undoped single crystals a single relaxation process is observed, showing a remarkable critical slowing down of the QP relaxation dynamics at the SDW transition temperature T_{SDW}\simeq125{K}. In the superconducting (SC) crystals multiple relaxation processes are present, with distinct SC state quasiparticle recombination dynamics exhibiting a BCS-like T-dependent superconducting gap, and a pseudogap (PG)-like feature with an onset above 180K indicating the existence of a pseudogap of magnitude 2\Delta_{\mathrm{PG}}\simeq120 meV above T_{\mathrm{c}}. From the pump-photon energy dependence we conclude that the SC state and PG relaxation channels are independent, implying the presence of two separate electronic subsystems. We discuss the data in terms of spatial inhomogeneity and multi-band scenarios, finding that the latter is more consistent with the present data., Comment: Replaced by the correct version

We determined electronic relaxation times via pump-probe optical spectroscopy using sub-15 fs pulses for the normal state of two different cuprate superconductors.We show that the primary relaxation process is the electron-phonon interaction and extract a measure of its strength, the second moment of the Eliashberg function\lambda<\omega^{2}>=800\pm200 meV^{2} for La_{1.85}Sr_{0.15}CuO_{4} and \lambda<\omega^{2}>=400\pm100 meV^{2} for YBa_{2}Cu_{3}O_{6.5}. These values suggest a possible fundamental role of the electron-phonon interaction in the superconducting pairing mechanism., Comment: As published in PRL

We use femtosecond spectroscopy to investigate the quasiparticle relaxation and low-energy electronic structure in a near-optimally doped pnictide superconductor with T_c=49.5 K. Multiple relaxation processes are evident, with distinct superconducting state quasiparticle (QP) recombination dynamics exhibiting a T-dependent superconducting (SC) gap, and a clear "pseudogap" (PG) -like feature with an onset around 200K indicating the existence of a temperature-independent gap of magnitude \Delta_PG= 61 +- 9 meV above T_c. Both the SC and PG components show saturation as a function of fluence with distinct saturation thresholds ~0.15 \muJ/cm^2 and 1.5 \muJ/cm^2, respectively.

We use ultrashort intense laser pulses to study superconducting state vaporization dynamics in La(2-x)Sr(x)CuO4 (x=0.1 and 0.15) on the femtosecond timescale. We find that the energy density required to vaporize the superconducting state is 2+- 0.8 K/Cu and 2.6 +- 1 K/Cu for x=0.1 and 0.15 respectively. This is significantly greater than the condensation energy density, indicating that the quasiparticles share a large amount of energy with the boson glue bath on this timescale. Considering in detail both spin and lattice energy relaxation pathways which take place on the relevant timescale of picoseconds, we rule out purely spin-mediated pair-breaking in favor of phonon-mediated mechanisms, effectively ruling out spin-mediated pairing in cuprates as a consequence., Comment: 5 pages of article plus 4 pages of supplementary material

Magnetic properties of high purity stoichiometric La$_2$CuO$_4$ nanoparticles are systematically investigated as a function of particle size. Ferromagnetic single-domain spin clusters are shown to spontaneously form at the surface of fine grains as well as paramagnetic defects. Hysteresis loops and thermomagnetic irreversibility are observed in a wide temperature range $5 - 350$ K with the remnant moment and coercivity gradually decreasing with increasing temperature. Possible origins of the spontaneous surface ferromagnetic clusters and the relation of our data to the appearance of unusual magnetic phenomena and phase separation of doped cuprates are discussed., Comment: 10 pages, 15 figures

In a recent letter [1] Pilgram, Rice and Sigrist (PRS) propose to perform oxygen isotope dependent conductivity measurements along the c-axis of the cuprate superconductor BSSCO. In Raman isotope data for vibrations along the c-axis from 1988 [2], and in site selective susceptibility experiments determining Tc, no isotope effects were observed for oxygen ions in the insulating layer [3]. Based on these earlier not by PRS quoted experiments, we argue that the suggestion made in Ref. 1 is not worth to be undertaken, and if it is carried through, no effect will be seen. From the meanwhile 12 years old site selective data [3] the observed isotope effects stem to nearly 100% from oxygen ions in the CuO2-planes. These results evidence polaronic behavior in these planes [4]., Comment: 3 pages, 1 figure

Time-resolved optical experiments can give unique information on the characteristic length scales of dynamic charge inhomogeneity on femtosecond timescales. From data on the effective quasiparticle relaxation time r in La2-xSrxCuO4 and Nd2-xCexCuO4 we derive the temperature- and doping- dependence of the intrinsic phonon escape length le, which, under certain circumstances, can be shown to be a direct measure of charge inhomogeneity. Remarkably, a common feature of both p and n-type cuprates - which has important consequences for superconductivity - is that as T  Tc from above, the escape length approaches the zero-temperature superconducting coherence length, le  s(0). In close vicinity of Tc, le appears to follow the critical behaviour of the Ginsburg-Landau coherence length, GL(T). In the normal state le is found to be in excellent agreement with the mean free path lm obtained from the resistivity data. The data on le also agree well with the data on structural coherence lengths ls obtained from neutron scattering experiments, implying the existence of complex intrinsic textures on different length scales which may have a profound effect on the functional properties of these materials., Comment: To appear in Physical Review Letters

The properties of a system of charged particles on a 2D lattice, subject to an anisotropic Jahn-Teller-type interaction and 3D Coulomb repulsion are investigated. In the mean-field approximation without Coulomb interaction, the system displays a phase transition of first order. When the long range Coulomb interaction is included, Monte Carlo simulations show that the system displays very diverse mesoscopic textures, ranging from spatially disordered pairs to ordered arrays of stripes, or charged clusters, depending only on the ratio of the two interactions (and the particle density). Remarkably, charged objects with even number of particles are more stable than with odd number of particles. We suggest that the diverse functional behaviour - including superconductivity - observed in oxides can be thought to arise from the self-organization of this type., Comment: To appera in PRL

Superconducting state dynamics following excitation of a superconductor with a femtosecond optical pulse is studied in terms of a phenomenological Rothwarf and Taylor model. Analytical solutions for various limiting cases are obtained. The model is found to account for the intensity and temperature dependence of both photoinduced quasiparticle density, as well as pair-breaking and superconducting state recovery dynamics in conventional as well as cuprate superconductors., Comment: revised version - accepted for publication in Phys. Rev. Lett

The experimental and theoretical challenges posed by the study of dynamically inhomogeneous systems are outlined in the context of cuprates and other oxides. Considering the pitfalls in the single-component approach to the analysis of inhomogeneous systems, the effect of either temporal or spatial averaging by different experiments is discussed. A group-theoretical symmetry analysis of the observed inhomogeneities in real space and k-space observed in the cuprates is shown to lead to a quantitatively verifiable description of the inhomogeneous state, comprising of bound singlet pairs in the ground state and unbound fermions in the excited state. The predicted symmetry breaking associated with pairing is shown to be verifiable experimentally., Comment: 6 pages, 5 figures

Femtosecond pump probe experiments are reported on quasiparticle relaxation and recombination in YBa2Cu4O8 as a function of temperature and polarization. The data show a 2-component relaxation similar to YBa2Cu3O7-\delta, one component being assocated with the superconducting transition, and the other with the pseudogap below T* The relaxation time tau_p associated with the pseudogap is found to be T-independent, while the relaxation time tau_g of the component obseved only below Tc exhibits a clear divergence near Tc. A strong polarisation anisotropy of the picosecond transient is observed below Tc which is attributed to the anisotropy of the probe transition matrix elements., Comment: 4 pages, 4 figures

Time-resolved optical spectroscopy of collective and single-particle excitations of 1T-TaS2 and 2H-TaSe2 reveals the presence of a large gap in the excitation spectrum on the femtosecond timescale, associated with the formation of various degrees of CDW order. In common with superconducting cuprates, excitations with energies less than the full gap show much slower relaxation. This separation of timescales cannot be explained in a quasi-2D Fermi-Liquid picture with an anisotropic gap but rather suggests the formation of a fluctuating spatially inhomogeneous state eventually forming a long-range ordered state at low temperatures., Comment: to appear in Phys. Rev.B Rapid Comm

The onset of macroscopic phase coherence in superconducting cuprates is considered to be determined by random percolation between mesoscopic Jahn-Teller pairs, stripes or clusters. The model is found to predict the onset of superconductivity near 6% doping, maximum Tc near 15% doping and Tc= T* at optimum doping, and accounts for the destruction of superconductivity by Zn doping near 7%. The model also predicts a relation between the pairing (pseudogap) energy and Tc in terms of experimentally measurable quantities., Comment: 3 pages + 3 postscript figures

Measurements of the temperature dependence of the quasiparticle (QP) dynamics in Hg1223 with femtosecond time-resolved optical spectroscopy are reported. From the temperature dependence of the amplitude of the photoinduced reflection, the existence of two gaps is deduced, one temperature dependent Dc that closes at Tc, and another temperature independent ''pseudogap'' Dp. The zero-temperature magnitudes of the two gaps are Dc/kTc = 6 +/- 0.5 and Dp/kTc = 6.4 +/- 0.5 respectively. The quasiparticle lifetime is found to exhibit a divergence as T -> Tc from below, which is attributed to the existence of a superconducting gap which closes at Tc. Above Tc the relaxation time is longer than expected for metallic relaxation, which is attributed to the presence of the ''pseudogap''. The QP relaxation time is found to increase significantly at low temperatures. This behavior is explained assuming that at low temperatures the relaxation of photoexcited quasiparticles is governed by a bi-particle recombination process., Comment: accepted for publication in Phys.Rev.B

A model interaction is proposed in which pairing is caused by a non-local Jahn-Teller (JT) -like instability due to the coupling between planar O states and knot equal to 0 phonons. Apart from pairing, the interaction is found to naturally allow metallic stripe formation. The consequences of the model for superconductivity in the cuprates are discussed. The model is shown to be consistent with numerous sets of experimental data in quite some detail., Comment: 20 pages, 6 ps figures

We consider finite-k electron-phonon coupling appropriate for a superconductor with a very short coherence length and local intersite pairs. From group theoretical analyis we find that phonons with nonzero k can couple to degenerate electronic states in LaSrCuO and a Jahn-Teller-like distortion is found to be operative for E_u and E_g -symmetry O states. Experimentally observed anomalies in inelastic neutron scattering, ESR and EXAFS are found to be consistent with such an interaction of the tau_1 symmetry Sigma point mode with the planar O p_x and p_y states. The proposed interaction is found to naturally facilitate symmetry breaking associated with pairing and/or stripe formation., Comment: 8 pages postscript figures are included

A model is developed for photoinduced absorption from localized states observed in femtosecond pump-probe experiments in high-Tc superconductors and other materials. The dynamics of localized carriers are described in terms of phenomenological approach similar to that originaly proposed by Rothwarf and Taylor. Expanding the relaxation rate in powers of the order parameter we have shown that density of localized carriers is sensitive to Tc. From the analysis of the experimental data on YBa2Cu3O(7-x) and K0.3MoO3 we conclude that significant intra-gap density of localized states exists in these materials. Temperature dependence of the density of photoexcited localized carriers in underdoped YBa2Cu3O(7-x) and in K0.3MoO3 is consistent with the observation of the pseudogap above Tc., Comment: 4 pages, 2 figures, acepted for publication in Physica C, invited poster presented at M2S, Feb. 20 - 25, 2000, Houston, USA

We show that low-energy spectral features in the cuprates can be separated into different components by the measurement of the recombination dynamics of different low-energy excitations in real-time using femtosecond laser spectroscopy. Quasiparticle (QP) recombination across the gap and intra-gap localized state relaxation processes exhibit qualitatively different time- and temperature-dependences. The relaxation measurements also show the existence of two distinct coexisting energy gaps near optimum doping and in the overdoped region, one more or less temperature independent (which exists above and below Tc) and one which closes at Tc in a mean-field like fashion. Thus systematic studies of QP recombination as a function of doping and temperature suggest that the ground state of the cuprates is a mixed Boson-Fermion system with localised states present over the entire region of the phase diagram., Comment: 4 pages, acepted for publication in Physica C, invited paper given at M2S, Feb. 20 - 25, 2000, Houston, USA

Following recent progress in understanding the relaxation dynamics of photoexcited carriers in materials exhibiting a small gap in the low-energy excitation spectrum we have performed pump-probe measurements on near optimally doped Hg-1223. We show that the behavior is very similar as in optimally-doped YBCO, where the data can be interpreted with the coexisting presence of two energy gaps: normal state T-independent pseudogap and a mean-field-like collective gap, associated with intrinsic spatially inhomogeneous ground state. An important difference between the two compounds is found in the low temperature relaxation time, which in Hg-1223 is found to be strongly temperature and photoexcitation intensity dependent., Comment: 2 pages, acepted for publication in Physica C, Proccedings of M2S 2000, Feb. 20 - 25, 2000, Houston, Texas, USA

The unusual slow carrier relaxation dynamics - observed in femtosecond pump-probe experiments on high-temperature superconductors and recently also in a charge-density-wave system - is analyzed in terms of a model for relaxation of carriers in intra-gap states. The data on YBa_2Cu_3O_7-delta near optimum doping and K_0.3$MoO_3 are found to be described very well with the model using a BCS-like gap which closes at T_c. From the analysis of the data we conclude that a significant intra-gap density of localized states exists in these materials, which can be clearly distinguished from quasiparticle states by the time-resolved optical experiments because of the different time- and temperature-dependences of the photoinduced transmission or reflection. Localized charges are suggested to be the most likely origin of the intra-gap states, while the similarity of the response in the two materials appear to exclude spin and vortex excitations., Comment: 3 postscript figures are included, will be published in Phys. Rev. B

Time-resolved optical measurements give information on the quasiparticle relaxation dynamics in YBCO, from which the evolution of the gap with doping and temperature can be systematically deduced. In this paper these optical charge-channel `pseudogap' data are compared with the `pseudogap' obtained from the NMR Knight shift Ks, spin polarized neutron scattering (SPNS) and single particle tunneling measurements. A simple energy level diagram is proposed to explain the different `gap' magnitudes observed by different spectroscopies in Y1-xCaxBa2Cu3O7-y, whereby the spin gap Delta_s in NMR and SPNS corresponds to a triplet local pair state, while Delta_p in the charge excitation spectrum corresponds to the pair dissociation energy. At optimum doping and in the overdoped state, an additional T-dependent gap becomes evident, which closes at T_c, suggesting a cross-over to a more conventional BCS-like superconductivity scenario., Comment: 9 pages, 4 figures. Presented in HTS99, Miami, January 99

A systamatic quantitative comparison of ''pseudogap'' values obtained from the analysis of charge and spin excitation spectroscopies in underdoped YBa2Cu3O7-x using a temperature-independent gap shows two distinct excitations, one visible in spin-flip spectroscopies like NMR and spin polarized neutron scattering, and the other in charge excitation spectoscopies like single particle tunneling and time-resolved quasiparticle relaxation. Both appear to decrease with doping x approximately as 1/x and are T-independent, existing above and below Tc. We suggest that the charge excitation can be attributed to a pair-breaking local gap, while the spin excitation can be explained by an intra-gap local triplet state., Comment: 4 pages and 3 postscript figures, to be published in Phys. Rev.B (Rapid. Comm), Figure 1 is corrected

The low-energy electronic excitation spectrum and gap structure in optimally doped and overdoped Y_{1-x}Ca_{x}Ba_{2}Cu_{3}O_{7-\delta} single crystals are investigated by real-time measurements of the quasiparticle relaxation dynamics with femtosecond optical spectroscopy. From the amplitude of the photoinduced reflectivity as a function of time, temperature and doping x we find clear evidence for the coexistence of two distinct gaps in the entire overdoped phase. One is a temperature-independent pseudogap $\Delta_{p}$ and the other is a T-dependent collective gap $\Delta_{c}(T)$ which has a BCS-like T-dependence closing at Tc. From quasiparticle relaxation time measurements above Tc we ascertain that fluctuations associated with the collective gap $\Delta_{c}(T)$ are limited to a few K, consistent with time-dependent Ginzburg-Landau theory and are distinct from the pseudogap whose presence is apparent well above Tc for all x., Comment: 4 pages, 4 figures, accepted for publication in Phys.Rev.Lett

Ultrafast time-resolved optical spectroscopy in high-temperature superconductors enables the direct real-time measurement of non-equilibrium quasiparticle recombination dynamics. In addition, it also gives detailed information about the symmetry of the superconducting gap and the "pseudogap", their doping dependence and their temperature dependence. Experimental data, together with theoretical models on the photoinduced transmission amplitude and relaxation time as a function of temperature and doping in YBa2Cu3O7-d gives a consistent picture of the evolution of low-energy structure, where a temperature-independent gap is shown to exist in the underdoped state which evolves with doping into a two-component state near optimum doping, where the dominant response is from a T-dependent BCS-like superconducting gap., Comment: 15 pages, to be published in "Spectroscopy of Superconducting Materials", ACS Symposium Series Volume 730, 1999, Ed. E. Faulques

Time resolved measurements of quasiparticle (QP) relaxation dynamics on the femtosecond timescale are reported as a function of temperature and doping in YBa2Cu3O(7-x) for (0.48 < x < 0.1). In the underdoped state (x > 0.15), there is no evidence for any changes in the low-energy gap structure at Tc from either photoinduced QP absorption or QP relaxation time data. In combination with the sum rule, this implies the existence of pre-formed pairs up to a much higher temperature T*. Near x = 0.1 a rapid cross-over is observed, to a state where the QP recombination time diverges and the photoinduced QP density falls to zero at Tc, indicating the existence of a temperature-dependent superconducting gap which closes at Tc., Comment: 4 pages, 3 figures, accepted for publication in Europhysics Letters

Photoexcited quasiparticle relaxation dynamics are investigated in a $YBa_{2}Cu_{3}O_{7-\delta}$ superconductor as a function of doping $\delta$ and temperature $T$ using ultrafast time-resolved optical spectroscopy. A model calculation is presented which describes the temperature dependence of the photoinduced quasiparticle population $n_{pe}$, photoinduced transmission $\Delta{\cal T}/{\cal T}$ and relaxation time $\tau $ for three different superconducting gaps: (i) a temperature-dependent collective gap such that ${\bf \Delta}(T)\to 0$ as $T\to T_{c}$, (ii) a temperature-independent gap, which might arise for the case of a superconductor with pre-formed pairs and (iii) an anisotropic (e.g. d-wave) gap with nodes. Comparison of the theory with data of photoinduced transmission $| \Delta{\cal T}/{\cal T} |$, reflection $| Delta{\cal R}/{\cal R}|$ and quasiparticle recombination time $\tau$ in $YBa_{2}Cu_{3}O_{7-\delta}$ over a very wide range of doping ($0.1 < \delta <0.48)$ is found to give good quantitative agreement with a temperature-dependent BCS-like isotropic gap near optimum doping ($\delta <0.1)$ and a temperature-independent isotropic gap in underdoped $YBa_{2}Cu_{3}O_{7-\delta}$ ($0.15<\delta <0.48$). A pure d-wave gap was found to be inconsistent with the data., Comment: 12 pages, 7 ps figures, to be published in Phys. Rev. B

We report new time-resolved data of quasiparticle relaxation and Cooper pair recombination dynamics in YBa_2Cu_3O_{7-\delta}, measured as a function of temperature and doping \delta using femtosecond optical spectroscopy. The data show the existence of a normal state pseudo-gap for in-plane charge excitations below T* and an unusual divergence of the quasiparticle relaxation time in the superconducting state \tau_s with \delta towards optimum doping. In the underdoped state, no change in the amplitude of the induced transmission (which is proportional to the DOS at E_F), or relaxation time \tau_s is observed at T_c. From the sum rule, both observations signify that no gap opens at T_c in underdoped YBCO for \delta >0.15. T_c in this case only signifies the onset of phase coherence. The presented data thus suggest pair formation with an associated redistribution of the DOS starting at T* and the establishment of phase coherence at T_c consistent with Bose-Einstein condensation. In the optimally doped material, \delta ~ 0.1, on the other hand, both a divergence in lifetime and a change of the DOS occur at T_c, signifying the opening of a gap and the occurence of pairing takes place simultaneously., Comment: 5 pages, 4 figures

Analysis of the a-b plane optical conductivity $\sigma_{ab}$ for both twinned and untwinned YBa$_{2}$Cu$_{3}$O$_{7-\delta}$ as a function of temperature and doping shows that below a well defined temperature T*, a dip in the spectrum systematically appears separating the infrared charge excitation spectrum into two components with distinct energy scales. The change from monotonic behaviour in $\sigma_{ab}$ is found to be concurrent with the onset of phonon anomalies in Raman and infrared spectra below T*. The optical data are suggested to be evidence for the appearance of an inhomogeneous distribution of carriers rather than the opening of a simple gap for charge excitations below T*, an interpretation wich is consistent with recent angle-resoved photoemission and electronic Raman spectra. We find that the behaviour below T* and the absence of any anomalies at Tc can be interpreted assuming a Bose-Einstein condensation of preformed pairs., Comment: 6 pages, 4 figures

The temperature dependence of the energy relaxation of photoexcited (PE) carriers is used as a probe of the electronic structure of YBa_2Cu_3O_(7-d) in the insulating d~0.8 and metallic d~0.1 phases. The energy relaxation rate to phonons is obtained by measuring the non-equilibrium phonon occupation number, n_neq, with pulsed Raman Stokes/anti-Stokes spectroscopy using 1.5 and 70 ps long laser pulses. We can distinguish between relaxation via extended band states and localized states, since theoretically in the former, the relaxation is expected to be virtually T-independent, while in the latter it is strongly T-dependent. From the experiment - which shows strong temperature dependence of n_neq - we deduce that at least part of the PE carrier relaxation proceeds via hopping between localized states and we propose a simple theoretical model of the relaxation process. In addition, we compare the coupling of different vibrational modes to the carriers to find that the apical O vibrational mode is significantly more involved in the energy relaxation process that the in-plane 340 cm^(-1}) mode. This implies that the localized states are mainly (but not entirely) coupled to out-of plane vibrations., Comment: 9 pages, 6 figures (ps)