Search

The normal state of high-Tc cuprates has been considered one of the essential topics in high-temperature superconductivity research. However, compared to the high magnetic fields study of it, understanding a photoinduced normal state remains elusive. Here, we explore a photoinduced normal state of YBa$_2$Cu$_3$O$_{6.67}$ (YBCO) through a charge density wave (CDW) with time-resolved resonant soft x-ray scattering, as well as a high-magnetic field x-ray scattering. In the non-equilibrium state in which people predict a quenched superconducting state based on the previous optical spectroscopies, we experimentally observed a similar analogy to the competition between superconductivity and CDW shown in the equilibrium state. We further observe that the broken pairing states in the superconducting CuO$_2$ plane via the optical pump lead to nucleation of three-dimensional CDW precursor correlation, revealing that the photoinduced CDW is similar to phenomena shown under magnetic fields. Ultimately, these findings provide a critical clue that the characteristics of the photoinduced normal state show a solid resemblance to those under magnetic fields in equilibrium conditions., Comment: 22 pages, 5 figures and Supplementary Materials with 6 pages, 9 figures

Investigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang-Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin-correlations in the frustrated spin chain material CuGeO3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.

Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO$_3$ (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an IMT. During the course of the photoinduced insulator to metal transition (IMT) with above gap excitation, we observe an ultrafast ($<$ 180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by X-ray absorption and THz transmission (~ 450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory (DFT) calculations reveal a consistent scenario where optically driven inter-site charge transfer (ICT) drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide new modalities for control of electronic phase transitions in quantum materials based on ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation., Comment: 9 pages, 5 figures, major revision and title change from previous version

Superconductivity and charge density waves (CDW) are competitive, yet coexisting orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scales is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ following the quench of superconductivity by an infrared laser pulse. We observe a non-thermal response of the CDW order characterized by a near doubling of the correlation length within $\approx$ 1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDW manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations., Comment: Accepted version. 34 pages, 11 figures, Main text and Supplementary Materials

In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced $d^{1}d^{0}$ $\xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant x-ray diffraction and optical reflectivity -- to demonstrate that the orbital response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($\it{x}$ = 2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical $d^{1}d^{0}$ $\xrightarrow{}$ $d^{0}d^{1}$ transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the $d^{0}$ $ \xrightarrow{}$ $d^{1}L$, where $\it{L}$ denotes a hole in the oxygen band. This novel finding may pave a new avenue for selectively manipulating specific types of order in complex materials of this class.

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa2Cu3O6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO2 planes. The empty chain Cu dy2-z2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these calculations, we predict changes in the soft x-ray absorption spectra at the Cu L-edge. Femtosecond x-ray pulses from a free electron laser are used to probe these changes in absorption at two photon energies along this spectrum, and provide data consistent with these predictions., Comment: 20 pages with 6 figures

Ultrafast broadband transient reflectivity experiments are performed to study the interplay between the non-equilibrium dynamics of the pseudogap and the superconducting phases in Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+\delta}$. Once superconductivity is established the relaxation of the pseudogap proceeds $\sim$ 2 times faster than in the normal state, and the corresponding transient reflectivity variation changes sign after $\sim$ 0.5 ps. The results can be described by a set of coupled differential equations for the pseudogap and for the superconducting order parameter. The sign and strength of the coupling term suggest a remarkably weak competition between the two phases, allowing their coexistence., Comment: 12 pages, 5 figures. Accepted for publication in Physical Review Letters

The dynamics of an order parameter's amplitude and phase determines the collective behaviour of novel states emerged in complex materials. Time- and momentum-resolved pump-probe spectroscopy, by virtue of its ability to measure material properties at atomic and electronic time scales and create excited states not accessible by the conventional means can decouple entangled degrees of freedom by visualizing their corresponding dynamics in the time domain. Here, combining time-resolved femotosecond optical and resonant x-ray diffraction measurements on striped La1.75Sr0.25NiO4, we reveal unforeseen photo-induced phase fluctuations of the charge order parameter. Such fluctuations preserve long-range order without creating topological defects, unlike thermal phase fluctuations near the critical temperature in equilibrium10. Importantly, relaxation of the phase fluctuations are found to be an order of magnitude slower than that of the order parameter's amplitude fluctuations, and thus limit charge order recovery. This discovery of new aspect to phase fluctuation provides more holistic view for the importance of phase in ordering phenomena of quantum matter., Comment: 23 pages, 6 figures. Published version can be found at Nature Communications 3, 838 (2012)

Here we report extensive ultrafast time-resolved reflectivity experiments on overdoped Bi$_{2}$Sr$_{2}$Ca$_{1-x}$Y$_x$Cu$_{2}$O$_{8+\delta}$ single crystals (T$_C$=78 K) aimed to clarify the nature of the superconducting-to-normal-state photoinduced phase transition. The experimental data show the lack of the quasiparticles decay time divergence at the fluence required to induce this phase transition, in contrast to the thermally-driven phase transition observed at T$_C$ and at variance with recently reported photoinduced charge-density-wave and spin-density-wave to metal phase transitions. Our data demonstrate the non-thermal character of the superconducting-to-normal-state photoinduced phase transition. The data have been analyzed using an ad-hoc developed time-dependent Rothwarf-Taylor model, opening the question on the order of this non-equilibrium phase transition., Comment: 10 pages, 6 figures