Many-body correlation effects in complex quantum systems often lead to phase transitions that bear great technological potential. However, the underlying microscopic driving mechanisms or even the quantum-mechanical properties of the novel ground state often remain elusive. Here we employ phase-locked ultrabroadband terahertz (THz) pulses to disentangle two coexisting orders in the charge density wave phase 1T-TiSe2 via their individual non-equilibrium multi- THz dynamics. Furthermore, we demonstrate that few-cycle THz pulses can project out the matter part of a transient cold exciton-polariton condensate, providing novel insights into the very nature of this macroscopic quantum state.
In numerous solids exhibiting broken symmetry ground states, changes in electronic (spin) structure are accompanied by structural changes. Femtosecond time-resolved techniques recently contributed many important insights into the origin of their ground states by tracking dynamics of the electronic subsystem with femtosecond light pulses. Moreover, several studies of structural dynamics in systems with periodic lattice modulation (PLD) were performed. Since intensities of the super-lattice diffraction peaks are in the first approximation proportional to the square of the PLD amplitude, their temporal dynamics provides access to cooperative atomic motion. This process takes place on a fraction of a period of the corresponding lattice vibration (typically 100 fs timescale). However, since energy transfer from the excited electronic system to the lattice takes place on a comparable timescale, contribution of the incoherent lattice motion on diffraction intensities has to be taken into account. Furthermore we demonstrate an ultrafast transmission electron diffraction set-up, where relative changes in individual diffraction peaks of less than 1% can be studied. Here we show, that by simultaneously tracking the dynamics of intensities in super-lattice peaks, lattice peaks and in the incoherent background over multiple diffraction orders the two processes can be effectively disentangled.
Ultrashort pulses in the terahertz (THz) spectral range allow us to study and control spin dynamics on time scales faster than a single oscillation cycle of light. In a first set of experiments, we harness an optically triggered coherent lattice vibration to induce a transient spin-density wave in BaFe2As2, the parent compound of pnictide superconductors. The time-dependent multi-THz response of the non-equilibrium phases shows that the ordering quasi-adiabatically follows a coherent lattice oscillation at a frequency as high as 5.5 THz. The results suggest important implications for unconventional superconductivity. In a second step, we utilize the magnetic field component of intense THz transients to directly switch on and off coherent spin waves in the antiferromagnetic nickel oxide NiO. A femtosecond optical probe traces the magnetic dynamics in the time domain and verifies that the THz field addresses spins selectively via Zeeman interaction. This concept provides a universal ultrafast handle on magnetic excitations in the electronic ground state.
In this report we review recent experimental results on photoexcited carrier relaxation dynamics on high temperature superconductors (HTSC) probed by a femtosecond time-resolved optical spectroscopy, and compare the results with the data obtained on quasi two dimensional charge density waves. In these experiments, a femtosecond laser pump pulse excites electron-hole pairs via an inter-band transition in the material. These hot carriers rapidly release their energy via electron-electron and electron-phonon collisions reaching states near the Fermi energy within ~100 fs. If an energy gap is present in the low-energy density of states (DOS), it inhibits the final relaxation step and photoexcited carriers accumulate above the gap causing a transient change in reflectivity arising from excited state absorption. The relaxation and recombination processes of photoexcited quasiparticles, governed by the magnitude, anisotropy and the T-dependence of the low energy gap, are monitored by measuring the resulting photoinduced absorption as a function of time after the photoexcitation. This way, the studies of carrier relaxation dynamics give us direct information of the T-dependent changes in the low energy DOS. The technique is particularly useful to probe the systems with spatial inhomogeneities, where different local environments give rise to different relaxation rates. The data on series of HTSC-s show evidence for the coexistence of two distinct relaxation processes, whose T-dependences seem to be governed by two different energy scales: a T-independent pseudogap and a mean-field-like T-dependent gap that opens at Tc. The data suggest the origin of the two-gap behavior is in the intrinsic microscopic spatial inhomogeneity of these materials.
Femtosecond optical reflectivity measurements of La2-xSrxCuO4, La2CuO4+y, Bi2Sr2CuO6+z and Bi2Sr2CaCu2O8+δ thin films and single crystal samples indicate qualitative changes with fluence. At the lowest fluencies, there is a power law divergence in the relaxation time. The divergence has an onset temperature of 55±15K, independent of whether the sample is in the superconducting or normal states. At slightly higher fluencies, still perturbative, the additional response does not exhibit this power law divergence. At quite high fluencies- no longer perturbative- the metallic samples exhibit oscillations in the reflectivity amplitude. The period of these oscillations varies with the probe wavelength but not with the pump wavelength. The oscillations exhibit a decay time as long as 10 nsec.
Temperature dependence of the relaxation of photoexcited (PE) carriers is used as a probe of the electronic structure of the high-temperature superconductor YBa2Cu3O7- (delta ) ((delta) approximately equals 0.1). The relaxation process is studied by 'counting' -- through measurement of the Raman scattering Stokes/anti-Stokes intensity ratio -- the phonons emitted in the process of carrier energy relaxation. The phonon 'shake-off' is found to be strongly temperature dependent, implying that the PE carrier relaxation proceeds via a temperature activated process, which can be understood in terms of hopping between localized states. The long PE carrier lifetime and temperature dependence of the relaxation process implies the existence of localized states within 2 eV of the Fermi energy in optimally doped high-Tc superconductor.