Ultrafast spin dynamics in magnetic semiconductor quantum wells studied by magnetization modulation spectroscopy

1-x Mn_xTe quantum well structures at room temperature using time-resolved magnetization modulation spectroscopy. Access to the different electron and hole spin dynamics is obtained by carefully measuring the spectroscopic changes of the magneto-optical response during the first hundreds of femtoseconds after excitation. Experimental results are discussed in the framework of a simple model for a two-dimensional band structure. The spectroscopy is shown to be intimately related to the spectral band width of the applied ultrashort laser pulses. The general potential of the method for fundamental studies on other materials and systems is addressed. Received: 20 September 1998     

Ultrafast dynamics of carrier-induced absorption changes in highly-excited CdSe nanocrystals

We use femtosecond time-resolved transmission spectroscopy to study the density and time dependence of transient absorption changes of CdSe nanocrystals. Our data show pronounced absorption saturation up to complete bleaching of the lowest optical transition. At high carrier density the nonlinear spectra show several peaks that can be related to the two lowest quantized electron states. Thetime dependence of the carrier-induced absorption changes indicates an ultrafast relaxation process within the strongly broadened absorption lines.     

Ultrafast redistribution of vibrational excitation of CH-stretching modes probed via anti-Stokes Raman scattering

Resonant infrared femtosecond light pulses in the 3 μm region are used to excite specific CH-stretching modes of liquid 1,1,1-trichloroethane, cyclopentane, and cyclohexane. The ultrafast redistribution of vibrational excitation between different CH-stretching modes and the vibrational relaxation of these modes are monitored by spontaneous anti-Stokes Raman scattering of properly delayed and spectrally shaped probe pulses. The results are treated with a rate-equation system, yielding energy-redistribution and energy-relaxation times. Received: 16 December 1999 / Published online: 7 August 2000     

Ultrafast relaxation dynamics of electronic excitations in noble-metal clusters

We investigate non-equilibrium relaxation processes in optically excited large gold and silver clusters. Time-resolved pump-probe experiments and model calculations show that optical excitation of the clusters by femtosecond laser pulses results in a heating of the electron system, which is followed by electron cooling via phonon emission. The electron heating leads to an enhanced damping of the surface-plasmon resonance in the clusters. This enhanced damping is caused by an enhancement of the Landau damping and electron scattering rates at high electron temperatures. Furthermore, we find that the rate of electron cooling in the clusters changes with electron temperature; this is a consequence of the temperature-dependent specific heat of the conduction electrons. Finally, pump-probe experiments on ellipsoidal silver clusters show that the thermal expansion of the heated clusters triggers mechanical vibrations at the acoustic eigenfrequencies of the clusters. Received: 6 December 1999 / Published online: 7 August 2000     

Ultrafast motion of liquids C2H4Cl2 and C2H4Br2 studied with a femtosecond laser

Transient optical Kerr effect of liquids C₂H₄Cl₂ and C₂H₄Br₂ is investigated, for the first time to our knowledge, with a femtosecond (fs) probe laser delayed with respect to a coherent fs pump laser. Coherent coupling and electronic Kerr signals are observed around zero delay when pump and probe overlap. Persisting after the pump-probe overlap are Kerr signals arising from the torsional and other intramolecular vibrations of the trans and gauche conformations; Kerr signals arising from the intermolecular motion are also observed. Vibrational quantum interference is only observed in liquid C₂H₄Br₂ and the related beats data are fitted with the torsional vibrations, 91 cm⁻¹ (gauche) and 132 cm⁻¹ (trans), and the CCBr angle-bending vibrations, 231 cm⁻¹ (gauche) and 190 cm⁻¹ (trans), with dephasing times, 0.45 ps, 0.45 ps, 2 ps, and 1.5 ps, respectively. These vibrational frequencies agree with those obtained in the frequency-domain. That no vibrational mode is observed for C₂H₄Cl₂ might be attributed to ineffective Raman-pumping. Kerr signals observed after the pump-probe overlap are Fourier transformed to give the spectra of the intermolecular motion and the vibrational spectrum, which agrees with the one observed in the infrared absorption and/or Raman scattering heretofore.     

Ultrafast all-optical polarization switching based on “virtual excitation” of InGaAs(P) MQWs

All-optical polarization switches based on near-resonant excitation have been demonstrated recently, which operate without significant real carriers excited in MQWs so as to avoid carriers accumulation. In this paper, we focus our investigation on the switch adopting InGaAsP MQWs because it could be compatible with the optical communication system. Our theoretical analysis is restricted to χ³ regime (i.e., the lowest-order nonlinear regime) and based on the dynamics-controlled truncation (DCT) scheme which provides a formalism for studying the coherent dynamics in weakly-nonlinear coherent optics of semiconductors. By using the theoretical model based on DCT theory, the switching action was simulated. With this theoretical model, we study the respective contributions of phase space filling and Hartree-Fock mean field as main terms of the optical Stark effect to the switching process, then exhibit the influence of delay time and control intensity for the switching response.     

On the theory of relaxation of electrons excited by femtosecond laser pulses in thin metallic films

Received: 14 October 1998 / Revised version: 21 December 1998     

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     

Ultrafast magnetization dynamics of Nickel

Received: 28 November 1998 / Revised version: 14 December 1998     

Ultrafast dynamics in ZnO thin films irradiated by femtosecond lasers

The damage morphologies, threshold fluences in ZnO films were studied with femtosecond laser pulses. Time-resolved reflectivity and transmissivity have been measured by the pump-probe technique at different pump fluences and wavelengths. The results indicate that two-phase transition is the dominant damage mechanism, which is similar to that in narrow band gap semiconductors. The estimated energy loss rate of conduction electrons is 1.5 eV/ps.     

Ultrafast optical nonlinear properties of metal nanoparticles

The physical origin and the dynamics of the ultrafast optical nonlinear response of noble metal nanoparticles are analyzed around the surface plasmon resonance frequency using extension of the bulk metal electron kinetics and band structure models. The computed spectral and temporal responses are found to be in very good agreement with the measured ones in silver when taking into account the impact of electron excitation on both the interband absorption and electron optical scattering rate. A good reproduction of the strong excitation regime experimental results is also obtained in the case of gold, with a dominant contribution of the interband effect. Received: 4 July 2001 / Published online: 10 October 2001     

Dephasing of optically induced excitonic coherences in semiconductor heterostructures

Resonant optical excitation of a direct bandgap semiconductor below the band edge induces excitonic coherences. Experiments based on transient four-wave mixing or cw spectral-hole burning provide an excellent approach to eliminate inhomogeneous broadening and enable determination of the time scale and origin of the decay of the optically induced quantum coherence. Such measurements are of interest in basic physics since they reflect fundamental interactions between the exciton and the surrounding environment including, for example, lattice vibrations and interface fluctuations. They also relate to potential applications of these excitations such as in coherent control or quantum information processing. Received: 30 March 2000 / Accepted: 2 September 2000 / Published online: 12 October 2000     

High-resolution nonlinear laser spectroscopy of exciton relaxation in GaAs quantum wells

This paper describes measurements of exciton relaxation in GaAs/AlGaAs quantum well structures based on high resolution nonlinear laser spectroscopy. The nonlinear optical measurements show that low energy excitons can be localized by monolayer disorder of the quantum well interface. We show that these excitons migrate between localization sites by phonon assisted migration, leading to spectral diffusion of the excitons. The frequency domain measurements give a direct measure of the quasi-equilibrium exciton spectral redistribution due to exciton energy relaxation, and the temperature dependence of the measured migration rates confirms recent theoretical predictions. The observed line shapes are interpreted based on solutions we obtain to modified Bloch equations which include the effects of spectral diffusion.     

Time-resolved UV absorption of polyimide

The 355-nm transient absorption of polyimide thin films has been measured following excitation withsubablative, 24-ps long, 355-nm laser pulses. The 355-nm absorption increases by 25% following 355-nm, 20 mJ/cm² excitation and recovers with a fast time constant 34 ps, and a slow time constant which is much longer than 6 ns. The data are fitted by a three-level rate equation model incorporating the temperature dependence of the ground state absorption coefficient. The fast component is attributed to the decay ofS ₁ and the slow component results from increased ground state absorption caused by a laser-induced temperature rise. The nonlinear intensity dependence is attributed to excited state (S ₁) absorption. These results indicate the importance of considering the dynamic absorption in modelling ablation.     

Four-wave mixing in coupled semiconductor quantum dots

We present a theoretical analysis of four-wave mixing in coupled quantum dots subject to inhomogeneous broadening. For the biexciton transitions, a clear signature of interdot-coupling appears in the spectra. The possibility of experimental observation is discussed.     

Ultra-fast spectroscopy and extreme nonlinear optics by few-optical-cycle laser pulses

Many fundamental processes of radiation–matter interaction, which take place on the ultra-short time scale, can now be directly investigated by using few-optical-cycles light pulses with duration <10 fs. We discuss two techniques for generating such pulses: broad-band parametric amplification, which allows the generation of pulses in the visible range suitable for spectroscopy, and compression of high-energy light pulses in a hollow fiber. As an example of application in time-resolved spectroscopy we report results of pump–probe experiments in a prototypical conjugated molecule, namely sexithiophene. The new laser sources, due to their characteristics of peak power and coherence, also allow the exploration of new fields of experimental physics, such as extreme nonlinear optics. We focus on high-order harmonics, showing that a high-energy bunch of photons, up to the X-ray-energy region, with coherence typical of laser radiation and time duration comparable to or shorter than the exciting pulses, can be generated. Received: 31 July 2000 / Revised version: 19 September 2000 / Published online: 8 November 2000     

Direct nanosecond Nd→Ce nonradiative energy transfer in cerium trifluoride laser crystals

Using third harmonics of LiF:F₂⁺ tunable color center laser excitation and selective fluorescence detection the temperature and concentration dependencies of fluorescence decay curves of the high-lying manifold of the Nd³⁺ ion were measured in CeF₃ crystals. As a result the temperature dependence of energy transfer kinetics from the manifold of the Nd³⁺ donor ions to the manifold of the acceptor Ce³⁺ ions in the ordered practically 100% filled crystal lattice was determined for 13-. Based on the temperature dependence the mechanisms and the channels of the Nd→Ce nonradiative energy transfer have been recognized. The net growth of the resonance Nd→Ce energy transfer rate in the temperature range from 25 to is found to be almost 3 orders of magnitude from 9.0×10⁴ to .In a crystal a significant contribution of the Nd→Nd resonance energy transfer to the manifold quenching is found for 20- and its channel and mechanism are suggested.Discussion of the possibility of subpicosecond and picosecond nonradiative energy transfer in rare-earth doped laser crystals is provided.     

Study of photo-induced phenomena in VO2 by terahertz pump-probe spectroscopy

The ultrafast terahertz response to the photoexcitation in vanadium dioxide was investigated using the optical-pump terahertz-probe technique at room temperature. The optical excitation at 790 nm induced an ultrafast decrease of the transmittance of the terahertz pulses corresponding to the increase of the electronic conductivity within 0.7 ps, and then the transmittance decreases gradually up to 100 ps. This two-step behavior is very similar to the previous reports of the time resolved X-ray and electron diffractions. This fact indicates that the increase of the electronic conductivity and the change of the lattice structure proceed in parallel, and the photo-induced insulator-metal phase transition is of the Peierls type.     

Ultrafast Energy Transfer and Enhanced Two-Photon Absorption in a Novel Porphyrin Side-Chain Polymer

Ultrafast relaxation processes and transient two-photon absorption are studied in a novel porphyrin side-chain polymer, 5-hydroxy-10,15,20-triphenyl-porphyrin-poly(glycidyl methacrylate) (HTPP-PGMA), by using picosecond luminescence spectroscopy and femtosecond pump--probe techniques. HTPP-PGMA exhibits the ultrafast initial luminescence decay (～300ps), which is absent in the conventional porphyrin monomer such as TPP. Enhanced two-photon absorption was observed in HTPP-PGMA; the corresponding Im x⁽³⁾ is about 2.8× 10¹¹esu, which is almost one order of magnitude larger than that of the conventional porphyrin monomer (TPP) (～1.3×10¹²esu). The ultrafast energy transfer plays an important role in the excited-state relaxation dynamics observed in HTPP-PGMA. The potential application of HTPP-PGMA in optical switching is discussed.     

Micro-photoluminescence study of electron-spin injection in self-assembled semiconductor quantum dots

We present a micro-photoluminescence (m-PL) study of electron-spin injection under magnetic fields in self-assembled semiconductor quantum dots (QDs) of CdSe. A characteristic band line-up of the CdSe QDs coupled with a diluted magnetic semiconductor quantum well (DMS-QW) of ZnCdMnSe through a ZnSe barrier layer enabled us to inject the electron spins from the DMS-QW into QDs. An experimental evidence of the electron-spin injection was provided by observations of circularly polarized m-PL spectra from individual QDs in this coupled QD structure. We find anti-correlation of PL intensity in between the DMS-QW (spin injector) and the individual QDs (spin receiver).