Proposal of structures possessing high exciton concentration

The possibility of achievement of high exciton concentrations is analyzed. It is shown that high concentrations can be achieved in a three-layer thin molecular film due to the autoreduction processes taking place in it. Shortly, the appearance of high concentrations is the consequence of boundary conditions in film and of the magnitude of matrix elements of dipol-dipol interactions. The autoreduction takes place in the cases when matrix elements characterizing exciton transfer are less than statistical matrix elements. Based on numerical analysis, it was found that optical quanta concentrations of a three-layer film can achieve values of about 5×10⁻². The structures possessing so high concentration do not exist in nature, thus they have to be synthesised. For the current state of nanotechnology, it is not a problem. Fortunately achieving high concentrations requires only certain ratios of relevant characteristics of the film with a two-level exciton scheme, but not their single values.     

Secondary peak in the optical absorption spectra: A possible criterion for Bose condensation of excitons

By solving the BCS and Bethe-Salpeter equations, we confirm the result by Chu and Chang that a secondary peak appears in the optical absorption spectrum immediately after the 1S-exciton peak in the presence of a condensed phase. The observation of the secondary peak indicates the presence of exciton condensate.     

Exciton formation with interchain couplings in organic polymers

Based on the framework of the tight binding approach and the nonadiabatic dynamics, the formation of an exciton in inter-coupled polymer chains is studied. Both a localized exciton in one single chain and a spread exciton between chains are obtained. It is found that an excited electron-hole pair is more inclined to evolve into a localized exciton, and the long range Coulomb e-e interaction is favorable to the exciton formation. By calculating the formation time of an exciton, we show that the optical response time is faster in a dilute solution than that in a solid film of polymer molecules.     

Electron-hole diagrams versus exciton diagrams: the simplest problem on interacting excitons

We study the interaction of an exciton with a distant metal, which is the simplest problem on interacting excitons: The semiconductor and metal electrons being “different” species, we do not have to worry about the tricky consequences of Pauli exclusion between identical carriers, which appear in any other problem on interacting excitons. We show how the exciton absorption, in the presence of semiconductor-metal interaction, can be derived in a very simple and transparent way from an exciton diagram procedure, provided that we use the appropriate exciton-metal interaction vertex, which contains the scattering from an exciton state to another exciton state under a Coulomb excitation. We also show that the resolution of this problem using standard electron-hole diagrams is dreadfully complicated at the lowest order in the semiconductor-metal interaction already, preventing a full calculation of the exciton-metal coupling from this usual technique. Received 26 February 2001     

Stability of singlet and triplet trions in carbon nanotubes

We investigate singlet and triplet trion states in semiconducting carbon nanotubes using a one-dimensional model. It is concluded that singlet trion states in bind up to 13.6% stronger than exciton states, and that they lower the optical transition energy with up to 50% of the tight binding band gap energy.     

Exciton condensation in coupled quantum wells

Bound electron-hole pairs—excitons—are Bose particles with small mass. Exciton Bose-Einstein condensation is expected to occur at a few degrees Kelvin—a temperature many orders of magnitude higher than for atoms. Experimentally, an exciton temperature well below 1 K is achieved in coupled quantum well (CQW) semiconductor nanostructures. In this contribution, we review briefly experiments that signal exciton condensation in CQWs: a strong enhancement of the indirect exciton mobility consistent with the onset of exciton superfluidity, a strong enhancement of the radiative decay rate of the indirect excitons consistent with exciton condensate superradiance, strong fluctuations of the indirect exciton emission consistent with critical fluctuations near the phase transition, and a strong enhancement of the exciton scattering rate with increasing concentration of the indirect excitons revealing bosonic stimulation of exciton scattering. Novel experiments with exciton condensation in potential traps, pattern formation in exciton system and macroscopically ordered exciton state will also be reviewed briefly.     

The trion as an exciton interacting with a carrier

The X⁻ trion is essentially an electron bound to an exciton. However, due to the composite nature of the exciton, there is no way to write an exciton-electron interaction potential. We can overcome this difficulty by using a commutation technique similar to the one we introduced for excitons interacting with excitons, which allows to take exactly into account the close-to-boson character of the excitons. From it, we can obtain the X⁻ trion creation operator in terms of excitons and electrons. We can also derive the X⁻ trion ladder diagram between an exciton and an electron. These are the basic tools for future works on many-body effects involving trions.     

Optical absorption in compact and extended dendrimers

Dendrimers are highly branched molecules, which are expected to be useful, for example, as efficient artificial light harvesting systems, in nano-technological or in medical applications. There are two different classes of dendrimers: compact dendrimers with constant distance between neighboring branching points throughout the macromolecule and extended dendrimers, where this distance increases from the system periphery to the center. We investigate the linear optical absorption spectra of these dendrimer types using the Frenkel exciton concept. The electron-phonon interaction is taken into account by introducing a heat bath that interacts with the exciton in a stochastic manner. We discuss compact dendrimers with equal excitation energies at all molecules, dendrimers with a functionalized core as well as with a whole branch functionalized. Furthermore the line shape of a compact dendrimer is discussed when neighboring molecules at the periphery interact and when all molecules have randomly distributed excitation energies due to disorder. Finally, we discuss two models for extended dendrimers.     

Temperature-Dependent Defect-Induced New Emission in ZnSe Crystal

The temperature-dependent photoluminescence behaviour of chemical vapour transport （CVT）-grown ZnSe crystal is investigated. A new emission band appears when temperature is reduced to 155K. It is shown that the new emission band is strongly related to defect emission peaked at around 2.1 eV. The emergence of the new emission band is accompanied by decreasing emission intensity of free exciton, as well as redshiR of defect emission with temperature decreases. The activated energy of the defect state is estimated to be 60.6 meV, which is approximately equal to the energy difference between the new emission and the free exciton emission at 155K.     

Signatures of stimulated bosonic exciton-scattering in semiconductor luminescence

We observe signatures of stimulated bosonic scattering of excitons, a precursor of Bose-Einstein-Condensation (BEC), in the photoluminescence of semiconductor quantum wells. The optical decay of a spinless molecule of two excitons (biexciton) into an exciton and a photon with opposite angular momenta is subject to bosonic enhancement in the presence of other excitons. In a gas of biexcitons and spin polarized excitons the bosonic enhancement breaks the symmetry of two equivalent biexciton decay channels leading to circularly polarized luminescence of the biexciton with the sign opposite to the circularly polarized exciton luminescence. Comparison of experiment and many body theory clearly indicates the existence of stimulated exciton-scattering, but excludes the presence of a fully condensed BEC-like state.     

Theory of dressed-excitons

We show that the exciton optical Stark effect is basically a dressed-exciton effect: excitons are dressed by the electromagnetic field in a way similar to the way atoms are dressed. The situation appears, however, much richer in semiconductor than in atomic physics due to both the complexity of the band structure and the Coulomb interaction between excitons. We show that the dressed-exciton effect can appear as either a blue or a red shift of the exciton line as well as a splitting of exciton levels, with an interesting dimensional effect in the absorption strength. We also relate the dressed-exciton to the polariton effect.     

Anisotropy of photoconductivity and nonlinear effects in GaSe monocrystals at high optical excitation

In this work, the photoelectric properties of gallium selenide (GaSe) monocrystals in the edge absorption region, with various configurations of current contacts, at low and high optical excitation levels are investigated. The photoconductivity spectrum behavior is determined by localized electronic and excitonic states along c-axis. It is shown that the localization of electronic and excitonic states in one-dimensional fluctuation potential along c-axis results to an anisotropy in photoconductivity spectrum at various current contacts configurations. At E⊥c the photoconductivity is observed in the hν < E_g and hν > E_g regions. In the case of hv < E_g, the maximum photoconductivity, in the impurity and exciton absorption region are observed at 1.975 eV and 2.102 eV, respectively. With rising of excitation energy level, suppression of photoconductivity in the exciton absorption region and increases in impurity absorption region is observed. At E||c contact configuration, the considerable photoconductivity is observed only in the impurity absorption region, which also increases with rising of excitation level. It is supposed that, suppression of photoconductivity in the exciton absorption region at high excitation levels is connected with exciton-exciton interaction, which results to a nonlinear light absorption. The results are compared with the absorption and photoluminescence measurements.     

Electron-phonon effects on Stark shifts of excitons in parabolic quantum wells: Fractional-dimension variational approach

Electron-phonon effects on Stark shifts of excitons in parabolic quantum wells are studied theoretically by using a fractional dimension method in combination with a Lee-Low-Pines-like transformation and a perturbation theory. The numerical results for the exciton binding energies and electron-phonon contributions to the binding energies as functions of the well width and the electric field in the Al_0.3Ga_0.7As parabolic quantum well structure are obtained. It is shown that both exciton binding energy and electron-phonon contributions have a maximum with increasing the well width. The binding energy and electron-phonon contribution decrease significantly with increasing the electric-field strength, in special in the wide-well case.     

Excitation relaxation and structure of TPPS4 J-aggregates

The energy relaxation kinetics and the structure of the J-aggregates of water-soluble porphyrin 5,10,15,20-tetrasulphonatophenyl porphine (TPPS₄) were investigated in aqueous medium by means of time-resolved fluorescence spectroscopy and confocal laser-scanning fluorescence microscopy. The excitation of the J-aggregates, at excitation intensities higher than ∼10¹⁵ photons/cm² per pulse, results in a remarkable decrease of the fluorescence quantum yield and in the appearance of an additional, non-exponential energy relaxation channel with a decay constant that depends on the excitation intensity. This relaxation mechanism was attributed to the exciton single-singlet annihilation. The exciton lifetime in the absence of the annihilation was calculated to be ∼150 ps. Using exciton annihilation theory, the exciton migration within the J-aggregates could be characterized by determining the exciton diffusion constant (1.8±0.9)  10⁻³ cm²/s and the hopping time (1.2±0.6) ps. Using the experimental data, the size of the J-aggregate could be evaluated and was seen to yield at least 20 TPPS₄ molecules per aggregate. It was shown by means of confocal fluorescence laser scanning microscopy that TPPS₄ does self-associate in polyvinyl alcohol (PVA) at acidic pH forming molecular macro-assemblies on a scale of ∼1 μm in PVA matrices.     

Phase diagram of electron-hole systems: Interplay between exciton Mott transition and quantum pair condensation

Quasi-thermal-equilibrium states of electron-hole (e-h) systems in photoexcited insulators are studied from a theoretical viewpoint, stressing the exciton Bose-Einstein condensation (BEC), the e-h BCS-type pair-condensed state, and the exciton Mott transition between an insulating exciton/biexciton gas phase and a metallic e-h plasma phase. We determine the quasi-equilibrium phase diagram of the e-h system at zero and finite temperatures with applying the dynamical mean-field theory (DMFT) to the e-h Hubbard model with both repulsive and attractive on-site interactions. Effects of inter-site interactions on the exciton Mott transition are also clarified with applying the extended DMFT to the extended e-h Hubbard model.     

Polaronic exciton in quantum wells wires and nanotubes

We investigate the effect of the longitudinal-optical phonon field on the binding energies of excitons in quantum wells, well-wires and nanotubes based on ionic semiconductors. We take into account the exciton-phonon interaction by using the Aldrich-Bajaj effective potential for Wannier excitons in a polarizable medium. We extend the fractional-dimensional method developed previously for neutral and negatively charged donors to calculate the exciton binding energies in these heterostructures. In this method, the exciton wave function is taken as a product of the ground state functions of the electron polaron and hole polaron with a correlation function that depends only on the electron-hole separation. Starting from the variational principle we derive a one-dimensional differential equation, which is solved numerically by using the trigonometric sweep method. We find that the potential that takes into account polaronic effects always give rise to larger exciton binding energies than those obtained using a Coulomb potential screened by a static dielectric constant. This enhancement of the binding energy is more considerable in quantum wires and nanotubes than in quantum wells. Our results for quantum wells are in a good agreement with previous variational calculations. Also, we present novel curves of the exciton binding energies as a function of the wire and nanotubes radii for different models of the confinement potential.     

Biexcitonic effects in the time integrated four-wave mixing with picosecond pulses

We propose a simple method to estimate the biexcitonic contribution to the excitonic non-linearity. The method is based on the time integrated four-wave mixing (TI FWM) with picosecond pulses. The TI FWM signal, which is measured as a function of the delay between pump and test pulses, shows shift towards positive and negative time delay when the laser is tuned at the exciton and biexciton resonance, respectively. We show theoretically that the magnitude of the shift allows us to estimate the biexcitonic contribution to the third-order non-linearity at the fundamental band edge.     

Exciton dynamics in nanostar dendritic systems using a quantum master equation approach: core monomer effects and possibility of energy transport control

The directional energy transport, i.e. exciton migration, in nanostar dendritic systems composed of two-state monomer units is studied using a quantum master equation approach. We examine the effects of the variation in the excitation energy of the monomer in the core region (core monomer) on the multistep exciton migration from the periphery to the core based on the relaxation factors among exciton states originating in weak exciton-phonon coupling. It turns out that when the core monomer possesses both an excitation energy slightly lower than that of the first generation and a partial exciton overlap with the first generation, more efficient and rapid exciton migration to the core is expected as compared with other core monomer cases with the energy level closer to or much lower than that of the first generation.     

Dependence of the heavy-hole exciton reduced mass on quantum-well size in InGaAs/GaAs heterostructures

We present low temperature photoluminescence investigations of the exciton ground state of In_0.14Ga_0.86As/GaAs quantum wells (QW) in the presence of pulsed magnetic fields up to 50 T. The exciton in-plane reduced mass and the heavy-hole in-plane mass are determined from the best fit of theoretical calculations to the magnetic field dependence of PL peaks. When the QW thickness decreases, their masses increases due to valence-band mixing effect.     

Exciton states and interband optical transitions in ZnO/MgZnO quantum dots

Within the framework of the effective-mass approximation, the exciton states confined in wurtzite ZnO/MgZnO quantum dot (QD) are calculated using a variational procedure, including three-dimensional confinement of carriers in the QD and the strong built-in electric field effect due to the piezoelectricity and spontaneous polarizations. The exciton binding energy and the electron-hole recombination rate as functions of the height (or radius) of the QD are studied. Numerical results show that the strong built-in electric field leads to a remarkable electron-hole spatial separation, and this effect has a significant influence on the exciton states and optical properties of wurtzite ZnO/MgZnO QD.