Exciton Control in a Room-Temperature Bulk Semiconductor with Coherent Strain Pulses

The coherent manipulation of excitons in bulk semiconductors via the lattice degrees of freedom is key to the development of acousto-optic and acousto-excitonic devices. Wide-bandgap transition metal oxides exhibit strongly bound excitons that are interesting for applications in the deep-ultraviolet, but their properties have remained elusive due to the lack of efficient generation and detection schemes in this spectral range. Here, we perform ultrafast broadband deep-ultraviolet spectroscopy on anatase TiO$_2$ single crystals at room temperature, and reveal a dramatic modulation of the exciton peak amplitude due to coherent acoustic phonons. This modulation is comparable to those of nanostructures where exciton-phonon coupling is enhanced by quantum confinement, and is accompanied by a giant exciton shift of 30-50 meV. We model these results by many-body perturbation theory and show that the deformation potential coupling within the nonlinear regime is the main mechanism for the generation and detection of the coherent acoustic phonons. Our findings pave the way to the design of exciton control schemes in the deep-ultraviolet with propagating strain pulses

The Effect Of Stationary UV Excitation On The Optical Behavior Of Electrochemically Self-Assembled Semiconductor Nanowires

In this work, we investigate the optical response of the semiconductor quantum wire array when excited by stationary UV light. The array is synthesized by selectively electro-depositing the semiconductor material in electrochemically self-assembled porous alumina templates. Our studies are based on the optical behavioral changes in CdS, ZnO, ZnSe and CdSe quantum wires of 50-, 25- and 10-nm diameters. We use a set of generalized Bloch equations to solve the interband polarization function of the semiconductors derived within the Hartree-Fock approximation, and theoretically model the UV excitation effect on the quantum wires. The solutions which consider the effects of screening, Coulomb interaction between the carriers and many body effects on excitons are generated for a quasi-equilibrium regime using a devised accelerated fixed point method. The solution technique is developed in Mathematica to iteratively solve this complex set of equations. The optical constants generated for individual quantum wires are incorporated into a finite-element electromagnetic wave simulator, HFSS, to investigate the full behavior of the array of wires. Theoretically calculated values of the dielectric permittivity of the un-excited quantum wires are shown to decrease progressively as the wire diameter reduces. We perform the experimental analysis using a pump-probe excitation scheme incorporated in a sensitive Michelson interferometer in a homodyne setup. We measure extremely small changes in the phase shift between the interfering IR probe beams and hence measure the refractive index changes caused by the UV pump. While the decreasing filling factor acts to reduce the optical activity in narrower wire arrays, the shifting of the DOS function with additional quantum confinement serves to increase it. These competing effects give rise to the size-dependent non-monotonic optical activity experimentally observed in ZnO, CdS and ZnSe nanowire arrays. The simulation results show a rapid increase in the changes in effective permittivity values of the individual quantum wires as diameter decreases. The substantial changes observed in the refractive index for the whole thin film array at intermediate wire diameter sizes may be suitable for optical phase shifting, intensity modulation and switching applications in integrated optical devices

Radiative Recombination Of Spatially Extended Excitons In (znse/cds)/cds Heterostructured Nanorods

We report on organometallic synthesis of luminescent (ZnSe/CdS)/CdS semiconductor heterostructured nanorods (hetero-NRs) that produce an efficient spatial separation of carriers along the main axis of the structure (type II carrier localization). Nanorods were fabricated using a seeded-type approach by nucleating the growth of 20-100 nm CdS extensions at [000 +/- 1] facets of wurtzite ZnSe/CdS core/shell nanocrystals. The difference in growth rates of CdS in each of the two directions ensures that the position of ZnSe/CdS seeds in the final structure is offset from the center of hetero-NRs, resulting in a spatially asymmetric distribution of carrier wave functions along the heterostructure. Present work demonstrates a number of unique properties of (ZnSe/CdS)/CdS hetero-NRs, including enhanced magnitude of quantum confined Stark effect and subnanosecond switching of absorption energies that can find practical applications in electroabsorption switches and ultrasensitive charge detectors

Multiphoton Absorption and Multiphoton Excited Photoluminescence in Transition Metal Doped ZnSe/ZnS Quantum Dots

Ph.DDOCTOR OF PHILOSOPH

Exciton-photon hybridisation in ZnSe based microcavities

This thesis presents the design, fabrication and experimental analysis of ZnSe based microcavities. Semiconductor microcavities are micro-structures in which the exciton ground state of a semiconductor is coupled to a photonic mode of an optical cavity. The strong light matter coupling mixes the character of excitons and photons, giving rise to the lower and upper cavity polaritons, quasiparticles with an unusual dispersion due to the extreme mass contrast between the composite exciton and photon. In particular, the dispersion of the lower polariton forms a dip around the lowest energy state with zero in-plane momentum. In this dip, which can be seen as a trap in momentum space, the polaritons are efficiently isolated from dephasing mechanisms involving phonons. The features of these quasiparticles promise a variety of applications, for instance lasing without inversion and micro-optical parametric amplifiers, and an environment to study fundamental physics, such as Bose-Einstein condensation in the solid state. By overcoming the longstanding fabrication problems of ZnSe-based microcavities, the enlarged exciton binding energy in combination with the use of highly reflective dielectric mirrors makes this material system ideally suited to the realisation of polariton-based devices operating at room temperature. An epitaxial liftoff technology is developed that relies on the high etch selectively between the ZnSe heterostructure and a novel II-VI release layer, MgS. Three hybrid microcavities are fabricated with the liftoff technique and spectroscopically characterised. Angle resolved transmission experiments reveal strong hybridization of the ZnSe/Zn0:9Cd0:1Se quantum well excitons and cavity photons in a fixed microcavity. A completely length tunable microcavity is presented and shown to exhibit similar dispersion as for the fixed microcavity, with the addition of evidencing the cavity polariton bottleneck effect. The nonlinear optical features are discussed. Photoluminescence data is presented that evidences the first observation of the build up of cavity polaritons at the edge of the momentum space trap in the lower polariton branch, the bottleneck effect, in a ZnSe based microcavity. Finally, lasing at room temperature in the blue spectral region is presented for a metal/dielectric hybrid microcavity

Enhanced carrier multiplication in engineered quasi-type-II quantum dots

Sem informaçãoOne process limiting the performance of solar cells is rapid cooling (thermalization) of hot carriers generated by higher-energy solar photons. In principle, the thermalization losses can be reduced by converting the kinetic energy of energetic carriers into additional electron-hole pairs via carrier multiplication (CM). While being inefficient in bulk semiconductors this process is enhanced in quantum dots, although not sufficiently high to considerably boost the power output of practical devices. Here we demonstrate that thick-shell PbSe/CdSe nanostructures can show almost a fourfold increase in the CM yield over conventional PbSe quantum dots, accompanied by a considerable reduction of the CM threshold. These structures enhance a valence-band CM channel due to effective capture of energetic holes into long-lived shell-localized states. The attainment of the regime of slowed cooling responsible for CM enhancement is indicated by the development of shell-related emission in the visible observed simultaneously with infrared emission from the core.518Sem informaçãoSem informaçãoSem informaçãoC. M. C., L. A. P., K. A. V., I. R., J.M.P. and V. I. K acknowledge support of the Center for Advanced Solar Photophysics (CASP), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES). N.S.M. is a CASP member supported by LANL Director's Postdoctoral Fellowship. Q. L. and H. L. are CASP affiliates supported by the New Mexico Consortium and Los Alamos National Laboratory