Ultra-fast optical spectroscopy of micelle-suspended single-walled carbon nanotubes

We present results of wavelength-dependent ultra-fast pump–probe experiments on micelle-suspended single-walled carbon nanotubes. The linear absorption and photoluminescence spectra of the samples show a number of chirality-dependent peaks and, consequently, the pump–probe results sensitively depend on the wavelength. In the wavelength range corresponding to the second van Hove singularities (VHSs) we observe subpicosecond decays, as has been seen in previous pump–probe studies. We ascribe these ultra-fast decays to intraband carrier relaxation. On the other hand, in the wavelength range corresponding to the first VHSs, we observe two distinct regimes in ultra-fast carrier relaxation: fast (0.3–1.2 ps) and slow (5–20 ps). The slow component, which has not been observed previously, is resonantly enhanced whenever the pump photon energy resonates with an interband absorption peak, and we attribute it to interband carrier recombination. Finally, the slow component is dependent on the pH of the solution, which suggests an important role played by H⁺ ions surrounding the nanotubes. PACS 78.47.+p; 78.67.Ch; 73.22.-f     

Landau-level lifetimes in PbTe nipi superlattices, PbTe/PbEuTe and InAs/AlSb quantum wells

Landau-level lifetimes are determined from saturation cyclotron resonance (CR) in wide parabolic wells, quantum wells and bulk PbTe–Pb_1−xEu_xTe systems. These narrow gap structures exhibit strong band non-parabolicity necessary to terminate the normally equi-spaced Landau-level ladder. It was not possible to saturate the bulk sample, but short lifetimes, of between 1.5 and 8 ps, were obtained for the wide parabolic well and the quantum well, respectively, utilising a multi-level rate equation model. We also report the first pump–probe cyclotron resonance result in an InAs–AlSb quantum structure. The pump–probe experiment provides a direct determination of the lifetime, giving τ=40 ps in this InAs–AlSb sample. This shows good agreement with an 8×8k·p calculation.     

Optical orientation and spin relaxation of resident electrons in n-doped InAs/GaAs self-assembled quantum dots

We report on optical orientation of electrons in n-doped InAs/GaAs quantum dots. Under non-resonant cw optical pumping, we measure a negative circular polarization of the luminescence of charged excitons (or trions) at low temperature (T=10 K). The dynamics of the recombination and of the circular polarization is studied by time-resolved spectroscopy. We discuss a simple theoretical model for the trion relaxation, that accounts for this remarkable polarization reversal. The interpretation relies on the bypass of Pauli blocking allowed by the anisotropic electron–hole exchange. Eventually, the spin relaxation time of doping electrons trapped in quantum dots is measured by a non-resonant pump–probe experiment.     

On the origin of time-resolved pump–probe differential signal from excitons in quantum wells

We investigate the origin and nature of femtosecond time-resolved (TR) pump–probe differential (PPD) signal from the exciton resonance in semiconductor quantum wells (QWs) in the coherent regime. The excitonic PPD signal is expressed as a sum of interferences of the excitonic nonlinear polarization with the incident probe field and the linear polarization induced by the probe. A nonzero excitonic TR-PPD signal from QWs can occur for time t larger than the pulse width (t_p) when the exciton dephasing time is longer than t_p, and this signal can originate only from the second interference term for both the negative and positive pump–probe delays, the contribution from the first interference term being zero for t>t_p. This is in contrast with the case of PPD signal in the spectral domain where the first interference term plays a major role. We discuss the effects of many body interactions on the TR-PPD signal. It is shown that excitation-induced dephasing can cause a significant increase in the rise time of the TR-PPD signal.     

Second harmonic generation in In2O3–SiON films doped by Al and Sn

Photoinduced optical and second-order non-linear optical effects in the interfaces separating In₂O₃–SiON (O/N ratio equals 1) films doped with A1, Sn and glass substrates were investigated using the photoinduced optical second harmonic generation. The photoinduced effective second-order optical susceptibility d_eff (at λ=1.76 μm) shows a good correlation with the linear optical susceptibility, particularly with the shift of the absorption edge. The maximal response of the photoinduced optical response signal was observed for the pump–probe delaying time of 34 ps. The performed experimental measurements indicate that the observed effects are mainly caused by the interface potential gradients on the border glass–In₂O₃–SiON film and by additional polarization due to insertion of the Al and Sn atoms. The observed phenomenon may be proposed as a sensitive tool for investigation of thin semiconducting interfacial layers and simultaneously such films may be used as materials for non-linear optical devices.     

Optically induced gate voltage spectroscopy in a GaAs/AlGaAs heterostructure

We report on measurements of optically induced gate voltage spectroscopy in a GaAs/AlGaAs heterostructure with a high mobility 2-dimensional electron gas (2DEG) in a thin (55 nm) GaAs layer. The optically induced gate voltage between the front gate and the 2DEG is sensitive to excess electron concentrations below 10⁷ cm⁻². In the gate voltage spectrum we observe a peak below the bandgap energy of GaAs, which is not observed in the photocurrent, luminescence or excitation spectra. Due to the extremely high sensitivity of this technique we attribute this below bandgap signal to very weak absorption lines below the GaAs bandgap energy by impurity bands or defect absorption. The fall-off of the below bandgap signal varies as exp (hω/E₀), where E₀ is an indicative for the quality of the heterostructure.     

Femtosecond pump and probe measurement of all-optical modulation based on intersubband transition in n-doped quantum wells

An all-optical modulation of interband-resonant light (near-infrared signal light: 800 nm) by intersubband-resonant light (mid-infrared control light: 4–7 μm) in n-doped AlGaAs/GaAs multiple quantum wells is investigated by two-color femtosecond pump–probe experiments at room temperature. The modulation of the near-infrared signal light with an ultrafast recovery as short as 1 ps is successfully observed when the quantum wells are pumped by the mid-infrared control light pulse (4 fJ/μm²). The dependence of the modulation depth on the wavelength of the control light is also measured, which is shown to be consistent with the intersubband absorption spectrum of the quantum wells. The results indicate that the utilization of the intersubband transition is promising for the ultrafast all-optical modulation and switching.     

Optical generation of spin coherence in single-charged (In,Ga)As/GaAs self-assembled quantum dots

The generation of electron spin coherence has been studied in n-modulation-doped (In,Ga)As/GaAs self-assembled quantum dots (QDs) which contain on average a single electron per dot. The doping has been confirmed by pump–probe Faraday rotation experiments in a magnetic field parallel to the heterostructure growth direction. For studying spin coherence, the magnetic field was rotated by 90° to the Voigt geometry, and the precession of the electron spin about the field was monitored. The coherence is generated by resonant excitation of the QDs with circularly polarized laser pulses, creating a coherent superposition of an electron, and a trion state. The efficiency of the generation can be controlled by the pulse intensity, being most efficient for (2n+1)π pulses.     

Extremely narrow luminescence linewidth in GaAs single quantum wells by insertion of thin AlAs smoothing layers

We propose a new method to considerably reduce the overall growth interruption for high-quality GaAs single quantum wells during molecular beam epitaxy. The insertion of ultrathin AlAs smoothing layers at the constituent GaAs/Al _x Ga_1–x As heterointerfaces and growth interruptions of not more than 15 s yields an improvement of the luminescence linewidth (FWHM) to 0.56 meV for a 13 nm wide GaAs well and to a value as low as 0.195 meV for a 27 nm wide GaAs well. In addition, no Stokes shift between absorption and emission and no line splitting due to monolayer fluctuations in the well width is observed.     

Femtosecond dynamics of dielectric films in the pre-ablation regime

The ultra-fast dynamics of dielectric oxide materials excited close to the laser-damage threshold is studied by performing transient reflection and transmission pump–probe measurements on TiO₂, Ta₂O₅, and HfO₂ films. The time-dependent dielectric constant is retrieved taking into account standing-wave effects of both pump and probe. A sub-100-fs transient is followed by a 1-ps transient, during which a sign reversal from negative to positive is observed in the real part of the induced change in the dielectric function, indicating the formation of deep defect states, possibly self-trapped excitons. PACS  78.47.+p; 61.80.-x; 72.20.Jv     

Polaritons in anisotropic semiconductors

We show how to compute the optical properties (reflection and absorption) of anisotropic semiconductors in the exciton energy region, taking into account polariton and electron-hole coherence effects. The method is applied to a GaAs/Ga_1–x Al _x As superlattice, and the modifications in the optical properties with respect to GaAs are related to the anisotropy.     

Dependence on temperature of homogeneous broadening of InGaAs/InAs/GaAs quantum dot fundamental transitions

We report systematic temperature-dependent measurements of photoluminescence spectra in self-assembled InGaAs/InAs/GaAs quantum dots (QDs). We have studied the rise in temperature of the ground-state homogeneous linewidth.A theoretical model is presented and accounts for the phonon-assisted broadening of this transition in individual QD. We have estimated the homogeneous linewidth of an individual QD from PL spectra of self-organized InAs/GaAs QDs by isolating the PL of each individual QD and fitting the narrow line associated with self-organized QDs through a Lorentzian convoluted by a Gaussian. We have observed a strong exciton–LO–phonon coupling (γ_LO) which becomes the dominating contribution to the linewidth above the temperature of 45 K. We have also derived the activation energy (ΔE) of the exciton–LO–phonon coupling, zero temperature linewidth (Γ₀) and the exciton-LA-phonon coupling parameter (γ_Ac). We report that our values are close to the values found in the literature for single InGaAs QD and InAs QD.     

Optical properties of Stranski–Krastanov grown three-dimensional Si/Si1−xGex nanostructures

Detailed Raman and photoluminescence (PL) measurements are reported for Si/Si_1−xGe_x nanostructures grown by molecular beam epitaxy under near Stranski–Krastanov (S–K) growth mode conditions. In samples with x ranging from 0.096 to 0.53, we observe that an increase in the Raman signal related to Ge–Ge vibrations correlates with (i) a red shift in the PL peak position, (ii) an increase in the activation energy of PL thermal quenching, and (iii) an increase in the PL quantum efficiency. The results indicate that for x>0.5 Ge atoms form nanometer size clusters with a nearly pure Ge core surrounded by a SiGe shell. Time-resolved PL measurements reveal a stretched-exponential long-lived PL component that is associated with compositional and dimensional fluctuations in the SiGe dots.     

Femtosecond response from two copolymers with intense two-photon absorption

Under excitation of femtosecond laser pulses at 800 nm, intense two-photon absorption induced fluorescence was observed from two copolymers, linear structure copolymer M2 and tri-branched copolymer M3. In a one-color pump–probe experiment at 800 nm, an ultrafast transient absorption was observed, which was mainly from the simultaneous absorption of the one photon from the pump beam and another photon from the probe beam. This analysis was further confirmed by a two-color pump–probe measurement with a pump at 800 nm and a probe at 556 nm, respectively. The other two decaying processes in transient absorption have a lifetime of about 14 and 126 ps, which reflects the intraband relaxation and the decay of the excited state via intersystem crossing or the solvation effect, respectively.     

Electron spin lifetimes in Hg0.78Cd0.22 Te and InSb

We have made direct pump–probe measurements of spin lifetimes in long wavelength narrow-gap semiconductors at wavelengths between 4 and 10 μm and from 4 to 300 K. In particular, we measure remarkably long spin lifetimes, τ_s300 ps, even at 300 K for epilayers of degenerate n-type InSb. In this material the mobility is approximately constant between 77 and 300 K, and we find that τ_s is approximately constant in this temperature range. In order to determine the dominant spin relaxation mechanism we have investigated the temperature dependence of τ_s in non-degenerate lightly n-type Hg_0.78Cd_0.22Te of approximately the same band gap as InSb, and find that τ_s varies from 356 ps at 150 K to 24 ps at 300 K. Our results, both in magnitude and temperature dependence of τ_s, imply that the Elliott–Yafet model dominates in these materials.     

Photo production of surface recombination centers in gallium arsenide

The near band edge photoluminescence (–870 nm) at 300 K of semi-insulating and p-type GaAs, a potentially useful tool for GaAs wafer mapping, decreases with time under illumination from the 514 nm line of an Ar⁺ laser. The photoluminescence bleaching has been studied by optical and photo Hall-effect techniques. It recovers only partially on a time scale of days and does not show a distinct intensity threshold behavior. From lifetime measurements and experiments on samples covered with epitaxial layers of GaAs _x P_1–x or Si₃N₄ it is concluded that creation of surface recombination centers causes the PL bleaching.     

Growth by molecular beam epitaxy and electrical characterization of GaAs nanowires

We report on structural and electrical properties of GaAs nanowires (NWs) grown by molecular beam epitaxy (MBE) on GaAs and SiO₂ substrates using Au as growth catalyst. Au–Ga particles are observed on the top of the NWs by transmission electron microscopy (TEM). In most of the observed cases, individual particles contain two Au–Ga compositions, in particular orthorhombic AuGa and β′ hexagonal Au₇Ga₂. The wires grown on GaAs are regularly shaped and tidily oriented on both (1 0 0) and (1 1 1)B substrates. TEM also reveals that the NWs have a wurtzite lattice structure. Electrical transport measurements indicate that nominally undoped NWs are weakly n-type while both Be- and Si-doped wires show p-type behaviour. The effect of the lattice structure on impurity incorporation is briefly discussed.     

Ultrafast dynamics and temperature effects on the quantum efficiency of the ring-opening reaction of a photochromic indolylfulgide

The ultrafast ring-opening reaction of the molecular switch 1,2-Dimethyl-3-indolylfulgide dissolved in acetonitrile is investigated by temperature dependent quantum efficiency measurements and time-resolved transient absorption spectroscopy in the ultraviolet and visible spectral range. The photoreaction is found to be thermally activated with an activation energy of about 1640 cm^− 1. The transient absorption signal is bi-exponential with the time constants τ₁ = 0.7 ps and τ₂ = 12 ps. The fast time constant is due to solvation dynamics, while the main component τ₂ is attributed to the excited state lifetime and product formation. A long-lived intermediate state in the photoreaction can be excluded.     

Selectively dopedn-AlxGa1−xAs/GaAs heterostructures with high-mobility two-dimensional electron gas for field effect transistors

In selectively dopedn-Al_xGa_1–xAs/GaAs heterostructures with high-mobility two-dimensional electron gas (2 DEG) at the heterointerface a second conductive channel exists, if the Al_xGa_1–xAs layer is not totally depleted from free carries. The occurrence of parallel conductance has a deleterious effect on the performance of high-electron mobility transistors (HEMTs) fabricated from this material. Although in principle computable, parallel conductance depends on a large number of design parameters to be chosen for the heterostructure, which are additionally affected by the presence of deep electron traps inn-Al_xGa_1–xAs of composition 0.25n-Al_xGa_1–xAs/GaAs heterostructures is shown.     

Excitonic polarons in quasi-two-dimensional structures

A theory of excitonic polarons in semiconductor quantum wells is presented. Using a unitary transformation, we have diagonalized the exciton-phonon interaction operator in a quasi-two-dimensional system partially and then calculated the ground-state energy of an excitonic polaron. We have numerically evaluated the energy gap shift and effective mass of an excitonic polaron. We have numerically evaluated the energy gap shift and effective mass of an excitonic polaron in GaAs-Al _x Ga_1–x As systems. The results obtained here indicate that the polaronic effect is significant in the case of the light hole excitons in quantum wells of small well widths.