Coherent ultrafast dynamics in the quantum Hall effect regime

We review recent investigations of the femtosecond non-linear optical response of the two-dimensional electron gas (2DEG) in the quantum Hall effect regime. We find that the time and frequency profile of the four-wave-mixing non-linear optical spectrum is strongly influenced by Coulomb correlations between the photoexcited electron-hole pairs and the 2DEG collective excitations. We discuss experimental and theoretical results showing non-Markovian memory effects in the polarization dephasing, and an optically induced time-dependent coupling between the two lowest Landau level magnetoexcitons.     

Theory of photoinduced phase transitions in itinerant electron systems

Theoretical progress in the research of photoinduced phase transitions is reviewed with closely related experiments. After a brief introduction of stochastic evolution in statistical systems and domino effects in localized electron systems, we treat photoinduced dynamics in itinerant-electron systems. Relevant interactions are required in the models to describe the fast and ultrafast charge-lattice-coupled dynamics after photoexcitations. First, we discuss neutral-ionic transitions in the mixed-stack charge-transfer complex, TTF-CA. When induced by intrachain charge-transfer photoexcitations, the dynamics of the ionic-to-neutral transition are characterized by a threshold behavior, while those of the neutral-to-ionic transition by an almost linear behavior. The difference originates from the different electron correlations in the neutral and ionic phases. Second, we deal with halogen-bridged metal complexes, which show metal, Mott insulator, charge-density-wave, and charge–polarization phases. The latter two phases have different broken symmetries. The charge-density-wave to charge–polarization transition is much more easily achieved than the reverse transition. This is clarified by considering microscopic charge-transfer processes. The transition from the charge-density-wave to Mott insulator phases and that from the Mott insulator to metal phases proceed much faster than those between the low-symmetry phases. Next, we discuss ultrafast, inverse spin-Peierls transitions in an organic radical crystal and alkali-TCNQ from the viewpoint of intradimer and interdimer charge-transfer excitations. Then, we study photogenerated electrons in the quantum paraelectric perovskite, SrTiO₃, which are assumed to couple differently with soft-anharmonic phonons and breathing-type high-energy phonons. The different electron–phonon couplings result in two types of polarons, a “super-paraelectric large polaron” with a quasi-global parity violation, and an “off-center-type self-trapped polaron” with only a local parity violation. The former is equivalent to a charged and conductive ferroelectric domain, which greatly enhances both the quasi-static electric susceptibility and the electric conductivity. Finally, we outline the development of time-resolved X-ray diffraction experiments, which directly accesses the dynamics of electronic, atomic and molecular motions in photoexcited materials. They are extremely useful when a three-dimensional structural long-range order is established and changes the symmetry.     

SHG studies of plasmon dephasing in nanoparticles

2 . The necessary high SHG efficiency is obtained by nanoparticles produced by an electron beam lithographic method, which enables us to fabricate a two-dimensional array of nearly identical, parallel oriented particles of designed shape without centrosymmetry, essential for high SHG efficiency and the tuning of the plasmon resonance to the driving laser wavelength of 780 nm. Received: 14 October 1998 / Revised version: 4 January 1999     

Ultrafast carrier dynamics in laser-excited materials: subpicosecond optical studies

2 , MgO and Al₂O₃) irradiated by short laser pulses (70 fs to 1.3 ps) at intensities below and above breakdown threshold. This is achieved with the help of time-resolved interferometry in the frequency domain, which was successfully used to study the dynamics of photoexcited carriers in insulators. The results obtained under different experimental conditions, distance from the surface, pump intensities and duration, during or after the pump pulse, are discussed and compared to the models recently developed to explain optical breakdown. Received: 20 September 1998     

The determination of the lifetime of hot electrons in metals by time-resolved two-photon photoemission: the role of transport effects, virtual states, and transient excitons

Experience has shown that theoretically determined lifetimes of bulk states of hot electrons in real metals agree quantitatively with the experimental ones, if theory fully takes into account the crystal structure and many-body effects of the investigated metal, i.e., if the Dyson equation is solved at the ab initio level and the effective electron–electron interaction is determined beyond the plasmon-pole approximation. Therefore the hitherto invoked transport effect [Knoesel et al.: Phys. Rev. B 57, 12812 (1998)] does not seem to exist. In this paper we show that likewise neither virtual states [Hertel: et al. Phys. Rev. Lett. 76, 535 (1996)] nor damped band-gap states [Ogawa: et al.: Phys. Rev. B 55, 10869 (1997)] exist, but that the hitherto unexplained d-band catastrophe in Cu [Cu(111), Cu(110)] can be naturally resolved by the concept of the transient exciton. This is a new quasiparticle in metals, which owes its existence to the dynamical character of dielectric screening at the microscopic level. This means that excitons, though they do not exist under stationary conditions, can be observed under ultrafast experimental conditions. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

The tight-binding approach to the dielectric response in the multiband systems

Starting from the random phase approximation for the weakly coupled multiband tightly-bounded electron systems, we calculate the dielectric matrix in terms of intraband and interband transitions. The advantages of this representation with respect to the usual planewave decomposition are pointed out. The analysis becomes particularly transparent in the long wavelength limit, after performing the multipole expansion of bare Coulomb matrix elements. For illustration, the collective modes and the macroscopic dielectric function for a general cubic lattice are derived. It is shown that the dielectric instability in conducting narrow band systems proceeds by a common softening of one transverse and one longitudinal mode. Furthermore, the self-polarization corrections which appear in the macroscopic dielectric function for finite band systems, are identified as a combined effect of intra-atomic exchange interactions between electrons sitting in different orbitals and a finite inter-atomic tunneling.     

Development of high-throughput combinatorial terahertz time-domain spectrometer and its application to ternary composition-spread film

We have developed a high-throughput combinatorial terahertz (THz) time-domain spectrometer (CTTDS) and applied to a ternary composition-spread film. This technique has possibilities to reveal a variety of physical properties such as complex refractive index, complex dielectric constant, and complex electrical conductivity. Further, this method is a non-contact and non-destructive way to map those physical properties. The demonstration of THz transmittance mapping of ternary composition-spread film, with a spatial resolution of 1 mm, reveals metallic behavior in specific range of film compositions. This prospective technique may serve as a convenient tool for the high-throughput, non-contact, non-destructive, and spatially resolved characterization suited for combinatorial composition-spread films.     

Dynamic correlation function for the propagation of light in disordered medium

We have calculated the time autocorrelation function of the intensity of light multiply scattered in the medium with dynamical properties. A new asimptotic for larget is found.     

A Method for Quantitative Analysis of Chemical Mixtures with THz Time Domain Spectroscopy

A method for analysing chemical mixtures quantitatively with terahertz time domain spectroscopy is proposed. The experimental results demonstrate the feasibility of this technique. Transmission coefficient of THz wave at the sample surface is taken into account to improve the analytic precision, lsomer mixtures are chosen as the experimental samples. Compared to similar techniques, the analytic precision could be improved evidently in this method.     

Mechanisms of femtosecond laser-induced breakdown and damage in MgO

Single-shot laser damage threshold of MgO for 40-986 fs, 800 nm laser pulses is reported. The pump-probe measurements with femtosecond pulses were carried out to investigate the time-resolved electronic excitation processes. A theoretical model including conduction band electrons (CBE) production and laser energy deposition was applied to discuss the roles of multiphoton ionization (MPI) and avalanche ionization in femtosecond laser-induced dielectric breakdown. The results indicate that avalanche ionization plays the dominant role in the femtosecond laser-induced breakdown in MgO near the damage threshold.     

Studies on 2,4-DNT Mixtures Using Reflection Terahertz Time Domain Spectroscopy for Explosives Detection

Absorption spectra （0.2-1.8 THz） of the mixtures of explosive 2,4-DNT and polyethylene（PE） at different ratios are obtained using reflection terahertz time domain spectroscopy （THz-TDS）. The pronounced absorption peak of 2,4-DNT at 1.08 THz is always observed for the mixtures with 2,4-DNT ratios above 20%. Experimental results demonstrate that more applicable and realistic THz-TDS in reflection geometry can be used to distinguish explosive mixed with other material having no THz fingerprints, and has a high potential in the detection of explosives.     

Time-resolved photo-induced nonlinear magneto-optical Kerr effect for the study of spin dynamics at a GaAs(001) surface

Received: 20 September 1998     

Optical anisotropy and pinning of the linear polarization of light in semiconductor microcavities

We report strong experimental evidence of the optical anisotropy in a CdTe-based microcavity: the polarization of light is pinned to one of the crystallographic axes independently of the polarization of the excitation. The polarization degree depends strongly on the excitation power, reaching almost 100% in the stimulated regime. The relaxation time of the polarization is about 1 ns. We argue that all of this is an effect of a splitting of the polariton doublet at k=0. We consider different sources for the splitting and conclude that the most likely one is optical birefringence in the mirrors and/or the cavity.     

Femtosecond electron and spin dynamics probed by nonlinear optics

Received: 20 September 1998     

Single-pulse time- and fluence-resolved optical measurements at femtosecond excited surfaces

We describe a new technique for optical pump–probe measurements at femtosecond excited surfaces. By combining time-resolved microscopy with cylindrical focusing of the pump, complete mapping of the time and fluence dependence of laser-induced optical changes becomes possible in a single-pulse experiment. Received: 16 August 1999 / Accepted: 17 August 1999 / Published online: 30 September 1999     

Friedel oscillations in a two dimensional Fermi liquid

Within linear response the long range oscillations caused by short or long ranged impurities embedded in an otherwise homogeneous electron gas reflect the singularities of the static response function. By making use of the theory of the many-body local fields and the results of recent quantum Monte Carlo studies we have calculated the exact dependence of the amplitude of these oscillations on the density in a two dimensional electron Fermi liquid.     

Nonlinear Bragg structures based on ZnS/ZnSe superlattices

Nonlinear optical response of periodic ZnSe/ZnS heterostructures is reported using interband excitation of a ZnSe sublattice by nano-, pico- and femtosecond laser pulses. A considerable shift of the reflection spectrum and large relative reflection changes were observed in a wide spectral range corresponding to the transparency region of ZnSe far from the intrinsic absorption onset. Evaluated refraction-index change is about −0.05 with the relaxation time being about 3 ps. In the case of femtosecond excitation, a wide-band nonlinear response is observed for both one-photon near-UV and two-photon near-IR excitation. The nonlinear refraction is supposed to be controlled by population-induced absorption changes in ZnSe single crystals and relevant refraction-index modification via Kramers–Kronig relations. The nonlinearity relaxation time is supposed to trace a transition from a non-equilibrium to a quasi-equilibrium distribution of electrons and holes within ZnSe conduction and valence bands, respectively, rather than the electron–hole recombination time. The nonlinearity mechanism does not reduce to just population-dependent absorption saturation, but essentially results from the specific distribution function in the first instance after excitation.     

Quantum charge density fluctuations and the phase transition in Ce

We have calculated the quantum quadrupolar interaction due to charge density fluctuations of localized 4f-electrons in Ce by taking into account the angular dependence, the degeneracy of the localized 4f -orbitals and the spin-orbit coupling. The calculated crystal field of 4 f electronic states is in good agreement with neutron diffraction measurements. We show that orientational ordering of quantum quadrupoles drives a phase transition at K which we assign with the transformation. In the phase the centers of mass of the Ce atoms still form a face centered cubic lattice. The theory accounts for the first order character of the transition and for the cubic lattice contraction which accompanies the transition. The transition temperature increases linearly with pressure. Our approach does not involve Kondo spin fluctuations as the significant process for the phase transition. Received 19 October 1998     

Modification of the charge ordering transition in the quasi-one-dimensional conductor (TMTTF)2SbF6 under pressure

We have measured the temperature dependences of the conductance G and the dielectric permittivity ε′ of the (TMTTF)₂SbF₆ compound under a moderate pressure. The maximum of G(T) associated with the Mott-Hubbard localization disappears under pressure. With increasing pressure the peak in ε′(T), corresponding to the charge ordering (CO) phase transition, shifts to lower temperatures and broadens. At pressures above 0.24 GPa, ε′(T) becomes strongly frequency dependent. These modifications are explained in the frame of the extended Hubbard model and a slowing down behavior.     

Exchange-correlation and layer-thickness effects in quasi-two dimensional electron liquids

We demonstrate a replacement of the non-uniform sub-band density of quasi-2D electron layers by an effective uniform-slab density. Exchange, correlation and Fermi-liquid properties are determined via a mapping of the electron liquid to a classical fluid, using the hyper-netted-chain equation inclusive of bridge corrections, (i.e. the CHNC), as a function of the density, spin-polarization, layer width and the temperature. Our parameters-free theory is in good accord with quantum simulations, with effective-mass and spin-susceptibility results for 2D layers found in GaAs/AlGaAs structures.