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Interesting emergent behavior in quantum materials arises when the interaction of electrons with the lattice leads to partial localization and ordering of charge at low temperatures. The triangular lattice of some transition metal dichalcogenides additionally presents an interesting case, where spin order is frustrated, leading to an additional complex interplay of interactions involving spin, charge and lattice degrees of freedom. Here we present a study of local symmetry breaking of the lattice structure in the layered dichalcogenide material 1T-TaS$_{2}$ using x-ray pair-distribution function measurements. Remarkably, we observe symmetry-breaking polaronic distortions of the lattice structure around individual localized electrons at temperatures well above any of the known long-range ordered phases. These characteristic polaronic signatures remain on cooling through the spin and charge ordered states, eventually revealing a new transition near 50 K to a state displaying partially restored symmetry and significant inter-layer dimerization. The order parameter associated with the observed local atomic displacements and symmetry-allowed polaron spin structure in the ground state suggests that charge ordering is driven by the crystallization of polarons, rather than conventional Fermi surface nesting. Symmetry analysis shows that the distorted structure is consistent with a breakup of the QSL phase at low temperature, concurrent with the disappearance of domains in the charge order., Comment: 16 pages, 4 figures

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS$_2$ upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Utilizing a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden phase are key for device applications., 17 pages, 13 figures

Ultrafast dynamics across the photoinduced three-dimensional Peierls-like insulator-metal (IM) transition in CuIr$_{2}$S$_{4}$ was investigated by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. The structural coherence of the low-$T$ broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence of $F_{\mathrm{c}}\approx3$ mJ/cm$^{2}$ (at 1.55-eV photon energy) resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the original low-$T$ state. The electronic order shows a transient gap filling at a significantly lower fluence threshold of $\sim0.6$~mJ/cm$^{2}$. The data suggest that the photoinduced-transition structural dynamics to the high-$T$ metallic phase is governed by first-order-transition nucleation kinetics that prevents the complete structural transition into the high-$T$ phase even at excitation fluences significantly larger than $F_{\mathrm{c}}$. In contrast, the dynamically-decoupled electronic order is suppressed rather independently due to a photoinduced Mott transition., By mistake resubmitted as 2104.03698

Ultrafast transient reflectivity across the unusual three-dimensional Peierls-like insulator-metal (IM) transition in CuIr_{2}S_{4} was measured as a function of temperature. The low-temperature insulating-phase transient response is dominated by broken-symmetry-induced coherent lattice oscillations that abruptly vanish at the IM transition. The coherent mode spectra are consistent with Raman spectra reported in literature. The origin of the broken-symmetry-induced is also briefly discussed.

The femtosecond transinet optical spectroscopy is employed to study the relaxation dynamics of the equilibrium and hidden metastable charge-density-wave states in single crystals of 1$T$-TaS$_{2-x}$Se$_{x}$ as a function of the Se doping $x$. Similarly to pristine 1$T$-TaS$_{2}$, the transition to a hidden phase is observed at low temperature after a quench with a single 50~fs laser pulse, in the commensurate Mott phase up to $x=0.6$. The photo-induced hidden-phase formation is accompanied by a notable change in the coherent phonon spectra, and particularly the collective amplitude mode. While the stability of the hidden phase with increased temperatures is only slightly dependent of the Se content the hidden-phase creation-treshold fluence strongly increases with the Se content from 1 to $\sim4$ mJ/cm$^{2}$.

A systematic temperature dependent study of the femtosecond optical superconducting (SC) state destruction and recovery in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+��}$ 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.

All optical femtosecond relaxation dynamics in a single crystal of mono-phosphate tungsten bronze (PO$_{2}$)$_{4}$(WO$_{3}$)$_{2m}$ with alternate stacking m=6 of WO$_{3}$ layers was studied through the three consequent charge density wave (CDW) transitions. Several transient coherent collective modes associated to the different CDW transitions were observed and analyzed in the framework of the time dependent Ginzburg-Landau theory. Remarkably, the interference of the modes leads to an apparent rectification effect in the transient reflectivity response. A saturation of the coherent-mode amplitudes with increasing pump fluence well below the CDWs destruction threshold fluence indicates a decoupling of the electronic and lattice parts of the order parameter under strong optical drive.

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.

The functionality of logic and memory elements in current electronics is based on multi-stability, driven either by manipulating local concentrations of electrons in transistors, or by switching between equivalent states of a material with a degener- ate ground state in magnetic or ferroelectric materials. Another possibility is offered by phase transitions with switching between metallic and insulating phases, but classical phase transitions are limited in speed by slow nucleation, proliferation of domains and hysteresis. We can in principle avoid these problems by using quantum states for switching, but microscopic systems suffer from decoherence which prohibits their use in everyday devices. Macroscopic quantum states, such as the superconducting ground state have the advantage that on a fundamental level they do not suffer from decoherence plaguing microscopic systems. Here we demonstrate for the first time ultrafast non-thermal switching between different metastable electronically ordered states by pulsed electrical charge injection. The macroscopic nature of the many-body quantum states(1-4) - which are not part of the equilibrium phase diagram - gives rise to unprecedented stability and remarka- bly sharp switching thresholds. Fast sub-50 ps switching, large associated re- sistance changes, 2-terminal operation and demonstrable high fidelity of bi-stability control suggest new opportunities for the use of macroscopic quantum states in electronics, particularly for an ultrafast non-volatile quantum charge-order resistive random access memory (QCOR-RAM)., 12 pages, 3 figures

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.

Hidden states of matter with novel and unusual properties may be created if a system out of equilibrium can be induced to follow a trajectory to a state which is inaccessible or does not even exist under normal equilibrium conditions. Here we report on the discovery of a hidden (H) topologically protected electronic state in a layered dichalcogenide 1T-TaS2 crystal reached as a result of a quench caused by a single 35 fs laser pulse. The properties of the H state are markedly different from any other state of the system: it exhibits a large drop of electrical resistance, strongly modified single particle and collective mode spectra and a marked change of optical reflectivity. Particularly important and unusual, the H state is stable for an arbitrarily long time until a laser pulse, electrical current or thermal erase procedure is applied, causing it to revert to the thermodynamic ground state. Major observed events can be reproduced by a kinetic model describing the conversion of photo excited electrons and holes into an electronically ordered crystal, thus converting a Mott insulator to a conducting H state. Its long-time stability follows from the topological protection of the number of periods in the electronic crystal., 21 pages and 5 figures, separate supplementary material

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$_{8+��}$ (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 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

The anharmonic response of charge-density wave (CDW) order to strong laser-pulse perturbations in 1T-TaS_2 and TbTe_3 is investigated by means of a multiple-pump-pulse time-resolved femtosecond optical spectroscopy. We observe remarkable anharmonic effects hitherto undetected in the systems exhibiting collective charge ordering. The efficiency for additional excitation of the amplitude mode by a laser pulse becomes periodically modulated after the mode is strongly excited into a coherently oscillating state. A similar effect is observed also for some other phonons, where the cross-modulation at the amplitude-mode frequency indicates anharmonic interaction of those phonons with the amplitude mode. By analyzing the observed phenomena in the framework of time-dependent Ginzburg-Landau theory we attribute the effects to the anharmonicity of the mode potentials inherent to the broken symmetry state of the CDW systems.

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=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

Temperature and fluence dependence of the transient photoinduced reflectivity and the magnetooptical Kerr angle was measured in two Pr0.6Ca0.4MnO3 thin films subject to tensile and compressive substrate-induced strain. A photoinduced transient ferromagnetic metallic (TFM) phase is found to form below ~60K and ~40K in the substrate-strained and substrate-compressed film, respectively. From the hysteresis loops a difference in the TFM cluster sizes and amount of photomodulation is observed at low temperatures and low excitation fluences in the films with different strain. Surprisingly, the characteristic timescale for the TFM phase photomodulation is virtually strain independent. At high excitation fluences, the cluster sizes and amount of photomodulation are independent on the substrate-induced strain.

Charge transport measurements on flexible Mo$_{6}$S$_{3}$I$_{6}$ (MoSI) nanowires with different diameters in highly imperfect 2-terminal circuits reveal systematic power law behaviour of the conductivity $\sigma(T,V)$ as a function of temperature and voltage. On the basis of measurements on a number of circuits we conclude that the behaviour in \emph{thin} wires can be most convincingly described by tunneling through Tomonaga-Luttinger liquid (TLL) segments of MoSI wire, which is in some cases modified by environmental Coulomb blockade (ECB). The latter are proposed to arise from deformations or imperfections of the MoSI wires, which - in combination with their recognitive terminal sulfur-based connectivity properties - might be useful for creating sub-nanometer scale interconnects as well as non-linear elements for molecular electronics., Comment: 7 pages, 8 figures

We measured the temperature and fluence dependence of the time-resolved photoinduced optical reflectivity in a decagonal Al_{71.9}Ni_{11.1}Co_{17.0} quasicrystal. We find no evidence for the relaxation of a hot thermalized electron gas as observed in metals. Instead, a quick diffusion of the hot nonthermal carries ~40 nm into the bulk is detected enhanced by the presence of a broad ~1 eV pseudogap. From the relaxation dynamics we find an evidence for the presence of a fine structure in the electronic density of states around ~13 meV from the Fermi energy. The structure is related to a weak bottleneck for the carrier relaxation observed at low temperatures., The sample composition was corrected

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., 10 pages, 15 figures

Self-organization of charged particles on a 2D lattice, subject to an anisotropic Jahn-Teller-type interaction and 3D Coulomb repulsion is investigated. In the mean-field approximation without Coulomb interaction, the system displays a phase transition of first order. In the presence of the Coulomb repulsion the global phase separation becomes unfavorable and the system shows a mesoscopic phase separation, where the size of the charged regions is determined by the competition between the ordering energy and the Coulomb energy. The phase diagram of the system as a function of particle density and temperature is obtained by systematic Monte Carlo simulations. With decreasing temperature a crossover from a disordered state to a state composed from mesoscopic charged clusters is observed. In the phase separated state charged clusters with even number of particles are more stable than those with odd number of particles in a large range of particle densities. With increasing particle density at low temperatures a series of crossovers between states with different cluster sizes is observed. Above half filling in addition to the low temperature clustering another higher temperature scale, which corresponds to orbital ordering of particles, appears. We suggest that the diverse functional behaviour - including superconductivity - observed in transition metal oxides can be thought to arise from the self-organization of this type., 9 pages, 7 figures

The properties of Mo_6S_3I_6 nanowires were investigated with ab initio calculations based on the density-functional theory. The molecules build weakly coupled one-dimensional chains with three sulfur atoms in the bridging planes between the Mo octahedra, each dressed with six iodines. Upon uniaxial strain along the wires, each bridging plane shows two energy minima, one in the ground state with the calculated Young modulus Y=82 GPa, and one in the stretched state with Y=94 GPa. Both values are at least four times smaller than the experimental values and the origin of the discrepancy remains a puzzle. The ideal tensile strength is about 8.4 GPa, the chains break in the Mo-Mo bonds within the octahedra and not in the S bridges. The charge-carrier conductivity is strongly anisotropic and the Mo_6S_3I_6 nanowires behave as quasi-one-dimensional conductors in the whole range of investigated strains. The conductivity is extremely sensitive to strain, making this material very suitable for stain gauges. Very clean nanowires with good contacts may be expected to behave as ballistic quantum wires over lengths of several $\mu $m. On the other hand, with high-impedance contacts they are good candidates for the observation of Luttinger liquid behaviour. The pronounced 1D nature of the Mo_6S_3I_6 nanowires makes them a uniquely versatile and user-friendly system for the investigation of 1D physics., Comment: 7 pages, 8 figures included

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 temperature dependence of ultrafast photoinduced reflectivity transients is reported in Nd$_{0.5}$Sr$_{0.5}$MnO$_{3}$ thin film. The photoinduced reflectivity shows a complex response with very different temperature dependences on different timescales. The response on the sub-ps timescale appears to be only weakly sensitive to the 270K-metal-insulator phase transition. Below $\sim 160$ K the sub-ps response displays a two component behavior indicating inhomogeneity of the film resulting from the substrate induced strain. On the other hand, the slower response on the 10-100 ps timescale is sensitive only to the metal-insulator phase transition and is in agreement with some previously published results. The difference in the temperature dependences of the responses on nanosecond and $\mu $s timescales indicates that thermal equilibrium between the different degrees of fredom is established relatively slowly - on a nanosecond timescale.

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

Optical experiments on calf thymus DNA films subjected to different buffer environments are reported. The optical conductivity is that of a disordered or lightly doped semiconductor with a well-defined band-gap for charge excitations and low frequency transport determined by a small number of strongly localized electron states., Comment: 5 pages, 3 figures submitted to PRL

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., accepted for publication in Phys.Rev.B

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

Photoinduced IR absorption was measured in undoped (LaMn)_{1-\delta}O_{3} and (NdMn)_{1-\delta}O_{3}. We observe broadening and a ~44% increase of the midinfrared anti-Jahn-Teller polaron peak energy when La^{3+} is replaced with smaller Nd^{3+}. The absence of any concurent large frequency shifts of the observed PI phonon bleaching peaks and the Brillouin-zone-center internal perovskite phonon modes measured by Raman and infrared spectroscopy indicate that the polaron peak energy shift is mainly a consequence of an increase of the electron phonon coupling constant with decreasing ionic radius on the perovskite A site. This indicates that the dynamical lattice effects strongly contribute to the electronic band narrowing with decreasing in doped giant magnetoresistance manganites., Comment: RevTex, 2 postscript figures

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., 3 postscript figures are included, will be published in Phys. Rev. B

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., 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-��} 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 $��_{p}$ and the other is a T-dependent collective gap $��_{c}(T)$ 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 $��_{c}(T)$ 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., 4 pages, 4 figures, accepted for publication in Phys.Rev.Lett

Photoinduced IR absorption was measured in (La(1-x)Sr(x)Mn)(1-��)O3. A midinfrared peak centered at ~ 5000 cm$^{-1}$ was observed in the x=0 antiferromagnetic sample. The peak diminishes and softens as hole doping is increased. The origin of the photoinduced absorption peak is atributted to the photon assisted hopping of anti-Jahn-Teller polarons formed by photoexcited charge carriers, whose binding energy decreases with increasing hole doping. The shape of the peak indicates that the polarons are small., 5 pages, 3 figures, submitted to PRB

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

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

Ultrafast transient reflectivity changes caused by collective and single particle excitations in the quasi one-dimensional charge-density wave (CDW) semiconductor K0.3MoO3 are investigated with optical pump-probe spectroscopy. The temperature-dependence of non-equilibrium single particle excitations across the CDW gap and their recombination dynamics are reported for the first time. In addition, amplitude mode reflectivity oscillations are observed in real time. A T-dependent overdamped response is also observed which is attributed to relaxation of the phason mode., Comment: 5 pages, 4 figures, accepted for publication in Phys.Rev.Lett

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

We report new time-resolved data of quasiparticle relaxation and Cooper pair recombination dynamics in YBa_2Cu_3O_{7-��}, measured as a function of temperature and doping ��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 ��_s with ��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 ��_s is observed at T_c. From the sum rule, both observations signify that no gap opens at T_c in underdoped YBCO for ��>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, ��~ 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., 5 pages, 4 figures

Photoexcited quasiparticle relaxation dynamics are investigated in a $YBa_{2}Cu_{3}O_{7-��}$ superconductor as a function of doping $��$ 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 $��{\cal T}/{\cal T}$ and relaxation time $��$ for three different superconducting gaps: (i) a temperature-dependent collective gap such that ${\bf ��}(T)\to 0$ 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 $| ��{\cal T}/{\cal T} |$, reflection $| Delta{\cal R}/{\cal R}|$ and quasiparticle recombination time $��$ in $YBa_{2}Cu_{3}O_{7-��}$ over a very wide range of doping ($0.1 < ��, 12 pages, 7 ps figures, to be published in Phys. Rev. B

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., 9 pages, 6 figures (ps)