Profluorescent protease substrates: intramolecular dimers described by the exciton model.

Xanthene dyes are known to form dimers with spectral characteristics that have been interpreted in terms of exciton theory. A unique aspect of H-type dimers is the fluorescence quenching that accompanies their formation. Using the principles of exciton theory as a guide, a series of protease substrates was synthesized with a xanthene dye on each side of the cleavage site. To bring the attached dyes into spatial proximity to form a dimer, the molecular design included structure determinant regions in the amino acid sequence. In addition, chromophores were chosen such that changes in absorption spectra indicative of exciton splitting were anticipated. Cleavage of the peptides by a protease resulted in disruption of the dimers and indeed significant absorption spectral changes were observed. Furthermore, substrate cleavage was accompanied by at least an order of magnitude increase in fluorescence intensity. This has allowed determination of intracellular elastase activity using a fluorescence microscope equipped with standard optics.

Polarized interacting exciton gas in quantum wells and bulk semiconductors

We develop a theory to calculate exciton binding energies of both two- and three-dimensional spin polarized exciton gases within a mean field approach. Our method allows the analysis of recent experiments showing the importance of the polarization and intensity of the excitation light on the exciton luminescence of GaAs quantum wells. We study the breaking of the spin degeneracy observed at high exciton density (5×1010 cm2). Energy level splitting between spin +1 and spin -1 is shown to be due to many-body interexcitonic exchange while the spin relaxation time is controlled by intraexciton exchange. © 1996 The American Physical Society.

Spin splitting in a polarized quasi-two-dimensional exciton gas

We have observed a large spin splitting between "spin" +1 and -1 heavy-hole excitons, having unbalanced populations, in undoped GaAs/AlAs quantum wells in the absence of any external magnetic field. Time-resolved photoluminescence spectroscopy, under excitation with circularly polarized light, reveals that, for high excitonic density and short times after the pulsed excitation, the emission from majority excitons lies above that of minority ones. The amount of the splitting, which can be as large as 50% of the binding energy, increases with excitonic density and presents a time evolution closely connected with the degree of polarization of the luminescence. Our results are interpreted on the light of a recently developed model, which shows that, while intraexcitonic exchange interaction is responsible for the spin relaxation processes, exciton-exciton interaction produces a breaking of the spin degeneracy in two-dimensional semiconductors.

Single-exciton spectroscopy of semimagnetic quantum dots

A photoexcited II-VI semiconductor quantum dots doped with a few Mn spins is considered. The effects of spin-exciton interactions and the resulting multispin correlations on the photoluminescence are calculated by numerical diagonalization of the Hamiltonian, including exchange interaction between electrons, holes, and Mn spins, as well as spin-orbit interaction. The results provide a unified description of recent experiments on the photoluminesnce of dots with one and many Mn atoms as well as optically induced ferromagnetism in semimagnetic quantum dots.

Single-exciton spectroscopy of single Mn doped InAs quantum dots

The optical spectroscopy of a single InAs quantum dot doped with a single Mn atom is studied using a model Hamiltonian that includes the exchange interactions between the spins of the quantum dot electron-hole pair, the Mn atom, and the acceptor hole. Our model permits linking the photoluminescence spectra to the Mn spin states after photon emission. We focus on the relation between the charge state of the Mn, A0 or A−, and the different spectra which result through either band-to-band or band-to-acceptor transitions. We consider both neutral and negatively charged dots. Our model is able to account for recent experimental results on single Mn doped InAs photoluminescence spectra and can be used to account for future experiments in GaAs quantum dots. Similarities and differences with the case of single Mn doped CdTe quantum dots are discussed.

Spin degree of freedom in two dimensional exciton condensates

We present a theoretical analysis of a spin-dependent multicomponent condensate in two dimensions. The case of a condensate of resonantly photoexcited excitons having two different spin orientations is studied in detail. The energy and the chemical potentials of this system depend strongly on the spin polarization. When electrons and holes are located in two different planes, the condensate can be either totally spin polarized or spin unpolarized, a property that is measurable. The phase diagram in terms of the total density and electron-hole separation is discussed.

Coherent-light emission from exciton condensates in semiconductor quantum wells

We show that a quasi-two dimensional condensate of optically active excitons emits coherent light even in the absence of population inversion. This allows an unambiguous and clear experimental detection of the condensed phase. We prove that, due to the exciton–photon coupling, quantum and thermal fluctuations do not destroy condensation at finite temperature. Suitable conditions to achieve condensation are temperatures of a few K for typical exciton densities and the use of a pulsed and preferably circularly polarized, laser.

Exciton beats in GaAs quantum wells: bosonic representation and collective effects

We discuss light–heavy hole beats observed in transient optical experiments in GaAs quantum wells in terms of a free-boson coherent state model. This approach is compared with descriptions based on few-level representations. Results lead to an interpretation of the beats as due to classical electromagnetic interference. The boson picture correctly describes photon excitation of extended states and accounts for experiments involving coherent control of the exciton density and Rayleigh scattering beating.

Carrier lifetime and exciton saturation in a strain-balanced InGaAs/InAsP multiple-quantum-well

The bleaching of the n = 1 heavy-hole and light-hole exciton absorption has been studied at room temperature and zero bias in a strain-balanced InGaAs/InAsP multiple quantum well. Pump-probe spectroscopy was used to measure the decay of the light-hole absorption saturation, giving a hole lifetime of only 280 ps. As only 16 meV separates the light- and heavy-hole bands, the short escape time can be explained by thermalization between these bands followed by thermionic emission over the heavy-hole barrier. The saturation density was estimated to be 1 × 1016 cm-3; this is much lower than expected for tensile-strained wells where both heavy and light holes have large in-plane masses. © 1998 American Institute of Physics.

Solitons in Exciton-Polariton System: Reduced Modelling, Analysis, and Numerical Studies

In this dissertation, we study the behavior of exciton-polariton quasiparticles in semiconductor microcavities, under the sourceless and lossless conditions.

First, we simplify the original model by removing the photon dispersion term, thus effectively turn the PDEs system to an ODEs system,

and investigate the behavior of the resulting system, including the equilibrium points and the wave functions of the excitons and the photons.

Second, we add the dispersion term for the excitons to the original model and prove that the band of the discontinuous solitons now become dark solitons.

Third, we employ the Strang-splitting method to our sytem of PDEs and prove the first-order and second-order error bounds in the $H^1$ norm and the $L_2$ norm, respectively.

Using this numerical result, we analyze the stability of the steady state bright soliton solution. This solution revolves around the $x$-axis as time progresses

and the perturbed soliton also rotates around the $x$-axis and tracks closely in terms of amplitude but lags behind the exact one. Our numerical result shows orbital

stability but no $L_2$ stability.

EXCITON ENGINEERING THROUGH TUNALBLE FLUORESCENT QUANTUM DEFECTS

This thesis demonstrates exciton engineering in semiconducting single-walled carbon nanotubes through tunable fluorescent quantum defects. By introducing different functional moieties on the sp2 lattice of carbon nanotubes, the nanotube photoluminescence is systematically tuned over 68 meV in the second near-infrared window. This new class of quantum emitters is enabled by a new chemistry that allows covalent attachment of alkyl/aryl functional groups from their iodide precursors in aqueous solution. Using aminoaryl quantum defects, we show that the pH and temperature of complex fluids can be optically measured through defect photoluminescence that encodes the local environment information. Furthermore, defect-bound trions, which are electron-hole-electron tri-carrier quasi-particles, are observed in alkylated single-walled carbon nanotubes at room temperature with surprisingly high photoluminescence brightness. Collectively, the emission from defect-bound excitons and trions in (6,5)-single walled carbon nanotubes is 18-fold brighter than that of the native exciton. These findings pave the way to chemical tailoring of the electronic and optical properties of carbon nanostructures with fluorescent quantum defects and may find applications in optoelectronics and bioimaging.

Exciton-mediated photothermal cooling in GaAs membranes

Cooling of the mechanical motion of a GaAs nano-membrane using the photothermal effect mediated by excitons was recently demonstrated by some of the authors (Usami et al 2012 Nature Phys. 8 168) and provides a clear example of the use of thermal forces to cool down mechanical motion. Here, we report on a single-free-parameter theoretical model to explain the results of this experiment which matches the experimental data remarkably well.

Hybrid light-emitting diodes based on ZnO nanowires

ZnO is a wide band-gap semiconductor that has several desirable properties for optoelectronic devices. With its large exciton binding energy of ~60 meV, ZnO is a promising candidate for high stability, room-temperature luminescent and lasing devices [1]. Ultraviolet light-emitting diodes (LEDs) based on ZnO homojunctions had been reported [2,3], while preparing stable p-type ZnO is still a challenge. An alternative way is to use other p-type semiconductors, ether inorganic or organic, to form heterojunctions with the naturally n-type ZnO. The crystal structure of wurtzite ZnO can be described as Zn and O atomic layers alternately stacked along the [0001] direction. Because of the fastest growth rate over the polar (0001) facet, ZnO crystals tend to grow into one-dimensional structures, such as nanowires and nanobelts. Since the first report of ZnO nanobelts in 2001 [4], ZnO nanostructures have been particularly studied for their potential applications in nano-sized devices. Various growth methods have been developed for growing ZnO nanostructures, such as chemical vapor deposition (CVD), Metal-organic CVD (MOCVD), aqueous growth and electrodeposition [5]. Based on the successful synthesis of ZnO nanowires/nanorods, various types of hybrid light-emitting diodes (LEDs) were made. Inorganic p-type semiconductors, such as GaN, Si and SiC, have been used as substrates to grown ZnO nanorods/nanowires for making LEDs. GaN is an ideal material that matches ZnO not only in the crystal structure but also in the energy band levels. However, to prepare Mg-doped p-GaN films via epitaxial growth is still costly. In comparison, the organic semiconductors are inexpensive and have many options to select, for a large variety of p-type polymer or small-molecule semiconductors are now commercially available. The organic semiconductor has the limitation of durability and environmental stability. Many polymer semiconductors are susceptible to damage by humidity or mere exposure to oxygen in the air. Also the carrier mobilities of polymer semiconductors are generally lower than the inorganic semiconductors. However, the combination of polymer semiconductors and ZnO nanostructures opens the way for making flexible LEDs. There are few reports on the hybrid LEDs based on ZnO/polymer heterojunctions, some of them showed the characteristic UV electroluminescence (EL) of ZnO. This chapter reports recent progress of the hybrid LEDs based on ZnO nanowires and other inorganic/organic semiconductors. We provide an overview of the ZnO-nanowire-based hybrid LEDs from the perspectives of the device configuration, growth methods of ZnO nanowires and the selection of p-type semiconductors. Also the device performances and remaining issues are presented.