Water-soluble porphyrin, 5,10,15,20-tetraphenyl- 21H,23H-porphine-tetrasulfonic acid (TPPS), forms J-aggregate in aqueous solution depending on experimental conditions such as pH, dye concentration, and/or ionic strength. The steady-state fluorescence and picosecond single-photon timing spectroscopy were applied for protonated monomer and J-aggregate in aqueous solution and in thin films to reveal the dynamics in the S_{2} and S_{1} states. The S_{2} fluorescence spectra from the protonated monomer and J-aggregate were observed in addition to the normal S_{1} fluorescence. The lifetime of the S_{2} state was estimated to be ≈5 ps for J-aggregate, whereas the lifetime is shorter than 1 ps for protonated TPPS monomer. The mesoscopic structures of J-aggregate in thin film with and without polymer on the glass surface were examined by scanning near-field optical microscopy. With the surface topography and scanning near-field optical microscopy transmission images, TPPS J-aggregate was found to form a long and narrow tube-like structure which has a few μm length, 0.2-0.5 μm width, and 5-30 nm height. An unidirectional orientation of the structure was also found, which may be originated from the spin-coating process.
Transient pump-probe reflectance measurements on La_{0.67}Ca_{0.33}MnO_3/MgO and La_{0.67} Ca_{0.33}MnO_3/SrTiO_3 thin films reveal a hitherto unknown magnetization-dependent energy gap that determines the relaxation process of the optically excited charge carriers on the picosecond time scale. In the case of La_{0.67}Ca_{0.33}MnO_3/SrTiO_3, the subsequent reflectance dynamics at low temperatures is determined to be substrate-induced strain that drives the sample into a metastable state characterized by an increased number of paramagnetic domains.
We study theoretically the nonlinear four-wave mixing response of an ensemble of coupled pairs of quantum dots (quantum dot molecules). We discuss the shape of the echo signal depending on the parameters of the ensemble: the statistics of transition energies and the degree of size correlations between the dots forming the molecules.
By using the femtosecond and picosecond transient absorption measurement techniques, we have investigated diphenylacetylene, diphenylbutadiyne, and their methoxy and cyano derivatives in the solution phase. Both the rapid S_{2} → S_{1} internal conversion in the subpicosecond time scale and the triplet formation in the tens of picosecond region were observed for diphenylbutadiyne and its methoxy derivatives, while the dynamic behavior of dimethoxy-diphenylacetylene was quite similar to that of diphenyl acetylene. The level inversion of the lowest excited singlet states of dicyano-diphenylbutadiyne was observed. The thermally activated S_{2} ← S_{1} internal conversion was not negligible and the sum of the rate constants of S_{2} → S_{1} and S_{2} ← S_{1} internal conversions was estimated to be about 5 × 10^{11} s^{-1} at room temperature.
We have used an all-optical photoluminescence-imaging technique to measure excitonic transport in three types of GaAs structures in which the excitonic transitions vary from allowed direct-gap excitons to forbidden, doubly-indirect Type-II excitons. We f nd remarkable differences in the transport properties of these excitons. Our studies show that bulk free-exciton transport exhibits an anomalous laser power-dependent diffusivity, whereas quasi-2D interfacial excitons and Type-II cross-interface excitons do not. Additionally, we observe localization of cross-interface excitons at the potential disorder induced by the heterointerface roughness.
We apply time-resolved photocurrent and differential electroreflectance spectroscopy to study the evolution of the internal field in a GaAs/AlGaAs superlattice after pulsed optical excitation at low temperature. The electric field dynamics is investigated by tracing the spectral position of the Wannier-Stark transitions as a function of delay time. We determine the electron sweep-out time, extract detailed information about the picosecond-time-scale drift of the charge carriers by comparing the measured data with the results of semi-classical self-consistent model calculations, and evaluate the two experimental techniques with respect to their ability to provide information about the carrier and field dynamics.
Ultrafast spatio-temporal effects in optically excited semiconductors are investigated by solving the coupled semiconductor Maxwell-Bloch equations which include the relevant relaxation phenomena. The analysis is used to describe transport of electronic excitations on nano- to micrometer scales with a dynamic range on the femto- to picosecond time scale.
Measurement of photoluminescence as a function of temperature and of magnetic field in p-type phosphorus doped Cd_{1-x}Mn_{x}Te is reported. From the conduction band-acceptor level transition, the ionization energy of P-acceptors is obtained to be 54ą1 meV. The photoluminescence spectrum in the band edge region exhibits three maxima connected with the recombination of excitons bound to neutral acceptors (A^{0}, X), excitons bound to neutral donors (D^{0},X), and free excitons (X) at energies E_{(A^{0},X)}=1.606, E_{(D^{0},X)}=1.610, and E_{X}=1.614 eV, respectively. At T=1.4 K a strong increase in PL intensity of (A^{0}, X) line 8-fold as a function of magnetic field is found and shown to originate from the magnetic field-induced lowering of the acceptor binding energy and increase in the hole effective volume.
Ultrafast excited-state relaxation process has been studied with zinc porphyrin dimers and circular trimer. Following 80 fs excitation at Soret band (420 nm) or Q band (580 nm) of zinc porphyrin, the fluorescence decay curves exhibit ultrafast decays with lifetimes of 80 fs in o-dimer, 450 fs in trimer and 540 fs in m-dimer. The timeresolved fluorescence spectra show that the fast decay process correspond to disappearance of monomer-like emission followed by red-shifted and broaden spectra. These ultrafast processes are assigned as due to excitation transfer among monomers and delocalization of excitation yielding excitonic states.
A step-like emission is observed for CdTe/CdMnTe structures δ-doped with In. The new photoluminescence cannot be explained by neither the Raman process nor by the "ordinary" hot photoluminescence. We propose that magnetic interactions are responsible for the new photoluminescence appearing due to a dramatic increase in a thermalization time of hot excitons.
An influence of doping level on exciton properties in n-doped multiple quantum well structures of CdTe/CdMnTe is studied for multiple quantum well structures prepared in the way that donor (indium) concentration changes within the length of the sample. We show that the formation scenario for neutral donor bound excitons in low-dimensional structures can be different from that observed in bulk samples. We further show that in the case of such quantum well structures we can selectively excite either photoluminescence emission of localized or donor bound excitons, which is a consequence of surprisingly weak energy transfer link between two types of excitonic transitions.
The direct evidence for the efficient transfer of excitons from 4 nm and 6 nm to 10 nm wide CdTe quantum wells is presented based on the results of photoluminescence and photoluminescence excitation investigation. Efficient transfer is observed for quantum wells separated by thick (50 nm) CdMnTe barriers containing 10% or 30% Mn fraction. A new mechanism of the transfer is proposed, which involves long range dynamic magnetic interactions between free/bound excitons and Mn ions in the CdMnTe barrier regions of the structure.
In this work we evaluate optical properties of cubic phase GaN epilayers grown on top of (001) silicon substrate prepared by a new process. Prior to the growth Si substrate was annealed at 1300-1400°C in propane. The so-prepared substrate is covered with a thin (≈ 4 nm) SiC wafer, which allowed a successful growth of good morphological quality cubic phase GaN epilayers. The present results confirm recent suggestion on smaller ionization energies of acceptors in cubic phase GaN epilayers.
On the example of an explicitly solvable model of a semiconductor with alloy disorder in the conduction band, it is shown that a slowly varying exciting light pulse can be treated in an adiabatic approximation, that is, the self-energy of an electron can be taken as a continuously evolving series of snapshots of self-energies corresponding to a steady illumination with the instantaneous value of the light strength.
The hyperpolarizabilities of several pseudoazulenes are evaluated using a semiempirical quantum chemistry package MOPAC-93 and compared with hyperpolarizabilities of simple molecules like chloroform, benzene, naphthalene and azulene. The third-order hyperpolarizability γ is measured for a derivative of 1,2-5,6 dibenzoxalene using a femtosecond Z-scan method at 800 nm. The resulting hyperpolarizability of 1.7×10-34 esu corroborates the theoretical prediction that pseudoazulene structures behave similar to other aromatic molecules provided the experiments are carried out in a non-resonant regime.
We report on optical orientation of excitons and trions (singly charged exciton) in individual charge-tunable self-assembled InAs/GaAs quantum dots. When the number of electrons varies from 0 to 2, the trion photoluminescence under quasi-resonant excitation gets progressively polarized from zero to ≈100%. We discuss this behavior as the efficient quenching of exciton spin quantum beats in anisotropic quantum dots due to the trion formation. This result indicates a long hole-spin relaxation time larger than the radiative lifetime, confirmed by time-resolved photoluminescence measurements carried out on a quantum dots ensemble.
The properties of small-sized high density InAs/GaAs quantum dots (emitting at 1.25 eV) are studied by means of optically detected microwave resonance spectroscopy and time resolved photoluminescence techniques. The results are discussed in terms of trapping and thermal escape of the carriers as well as their relaxation and recombination in quantum dots. The data are compared with those recently obtained on shallowly formed InAs quantum dot structures.
We show that at low carrier energies and densities the carriers in a two-dimensional Coulomb gas interact via classical unscreened carrier-carrier collisions. This allows us to calculate exactly the thermalization due to the two-dimensional carrier-carrier collisions in a nonthermal low-density (≈10^{10} cm^{-2}) two-dimensional plasma excited near the band edge of an undoped GaAs quantum well. The thermalization is found to be 10-15 times slower than the 200 fs thermalization deduced from the previous spectral-hole burning measurements, which means that the spectral hole does not reflect the thermalization process. We also show that the Born approximation fails in describing such carrier-carrier collisions.
In this work we evaluate structural and optical properties of ZnO nanoparticles grown by wet chemistry method. Light emission properties of these nanoparticles are studied with cathodoluminescence and micro-photoluminescence. Even at the room temperature excitonic emission is well resolved, due to high exciton binding energy of ZnO. Decay kinetics of photoluminescence emissions and efficiency of inter-nanoparticles energy migration is evaluated from maps of in-plane variations of photoluminescence decay times measured in microphotoluminescence setup.
We present time-resolved photoluminescence measurements of GaN/AlGaN low dimensional structures showing very characteristic changes of dynamics related to strong electric field. Strong piezoelectric and spontaneous polarizations built-in in nitride structures lead to the changes in spatial separation of carriers which leads to changes in recombination energies and radiative lifetimes of the carriers. The observed effect can be well described by a simple exponential relation. The observed dependence can be explained by an approximated model of quantum-confined Stark effect based on the Airy functions.
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