Effects of phase-breaking on long-range charge transfer in DNA: Partially-coherent-tunneling model study

The mechanism of hole charge transfer in DNA of various lengths and sequences is investigated based on a partially coherent tunneling theory (Zhang et al., J Chem Phys 117:4578, 2002), where the effects of phase-breaking in adenine-thymine and guanine-cytosine base pairs are treated on equal foot. This work aims at providing a self-consistent microscopic interpretation for rate experiments on various DNA systems. We will also clarify the condition under which the simple superexchange-mediated-hopping picture is valid, and make some comments on the further development of present theory.

Role of different cap layers tuning the wavelength of self-assembled InAs/GaAs quantum dots

We have investigated the effect of different cap layers on the photoluminescence (PL) of self-assembled InAs/GaAs quantum dots (QDs). Based upon different cap layers, the wavelength of InAs QDs can be tuned to the range from 1.3 to 1.5 mum. An InAlAs and InGaAs combination layer can enlarge the energy separation between the ground and first excited radiative transition. GaAs/InAs short period superlattices (SLs) make the emission wavelength shift to 1.53 mum. The PL intensity of InAs QDs capped with GaAs/InAs SLs shows an anomalous increase with increasing temperature. We attribute this to the transfer of carriers between different QDs.

Study of optical properties in GaAs1-xSbx/GaAs single quantum wells

GaAsSb/GaAs single quantum wells (SQWs) grown by molecular beam epitaxy are studied by selectively-excited photoluminescence (SEPL) measurement. For the first time, we have simultaneously observed the PL, from both type I and type II transitions in GaAsSb/GaAs heterostructure in the SEPL. The two transitions exhibit different PL, behaviours under different excitation energy. As expected, the peak energy of type I emission remains constant in the whole excitation energy range we used, while type U transition shows a significant blue shift with increasing excitation energy. The observed blue shift is well explained in terms of electron-hole charge separation model at the interface. Time-resolved(TR) PL exhibits more type 11 characteristic of GaAsSb/GaAs QW. Moreover, the results of the excitation-power-dependent PL and TRPL provide more direct information on the type-II nature of the band alignment in GaAsSb/GaAs quantum-well structures. By combining the experimental results with some simple calculations, we have obtained the strained and unstrained valence band offsets of Q(v) = 1.145 and Q(v)(0) = 0. 76 in our samples, respectively.

Anomalous temperature dependence of photoluminescence in GaInNAs/GaAs multiple quantum wells

Photoluminescence (PL) spectra of GaInNAs/GaAs multiple quantum wells grown on a GaAs substrate by molecular beam epitaxy are measured in a range of temperatures and excitation power densities. The energy position of the dominant PL peak shows an anomalous S-shape temperature dependence instead of the Varshni relation. By careful inspection, especially for the PL under lower excitation power density, two near bandedge peaks are well identified. These are assigned to carriers localized in nitrogen-induced bound states and interband excitonic recombinations, respectively. It is suggested that the temperature-induced switch of such two luminescence peaks in relative intensity causes a significant mechanism responsible for the S-shape shift observed in GaInNAs. A quantitative model based on the thermal depopulation of carriers is used to explain the temperature dependence of the PL peak related to N-induced bound states.

A partially incoherent rate theory of long-range charge transfer in deoxyribose nucleic acid

A quantum chemistry based Green's function formulation of long-range charge transfer in deoxyribose nucleic acid (DNA) double helix is proposed. The theory takes into account the effects of DNA's electronic structure and its incoherent interaction with aqueous surroundings. In the implementation, the electronic tight-binding parameters for unsolvated DNA molecules are determined at the HF/6-31G* level, while those for individual nucleobase-water couplings are at a semiempirical level by fitting with experimental redox potentials. Numerical results include that: (i) the oxidative charge initially at the donor guanine site does hop sequentially over all guanine sites; however, the revealed rates can be of a much weaker distance dependence than that described by the ordinary Ohm's law; (ii) the aqueous surroundings-induced partial incoherences in thymine/adenine bridge bases lead them to deviate substantially from the superexchange regime; (iii) the time scale of the partially incoherent hole transport through the thymine/adenine pi stack in DNA is about 5 ps. (C) 2002 American Institute of Physics.

Interplay between partial incoherence, partial inelasticity, resonance, and heterogeneity in long-range electron transfer and transport

A generalized scattering matrix formalism is constructed to elucidate the interplay of electron resonance, coherence, dephasing, inelastic scattering, and heterogeneity, which play important roles in the physics of long-range electron transfer/transport. The theory consists of an extension of the standard Buttiker phase-breaking model and an analytical expression of the electron transmission coefficient for donor-bridge-acceptor systems with arbitrary length and sequence. The theory incorporates the following features: Dephasing-assisted off-resonance enhancement, inelasticity-induced turnover, resonance enhancement and its dephasing-induced suppression, dephasing-induced smooth superexchange-hopping transition, and heterogeneity effects. (C) 2002 American Institute of Physics.

The PL "violet shift" of cerium dioxide on silicon

CeO2 thin film was fabricated by dual ion beam epitaxial technique. The phenomenon of PL violet shift at room temperature was observed, and the distance of shift was about 65 nm. After the analysis of crystal structure and valence in the compound were carried out by XRD and XPS technique, it was concluded that the PL shift was related with valence of cerium ion in the oxides. When the valence of cerium ion varied front tetravalence to trivalence, the PL peak position would move from blue region to violet region and the phenomenon of "violet shift" was observed.

Scattering matrix approach to electronic dephasing in long-range electron transfer

Based on the Buttiker dephasing model, we propose an analytical scattering matrix approach to the long-range electron transfer phenomena. The present efficient scheme smoothly interpolates between the superexchange and the sequential hopping mechanisms. Various properties such as the drastic dephasing-assisted enhancement and turnover behaviors are demonstrated in good agreement with those obtained via the dynamical reduced density-matrix methods. These properties are further elucidated as results of the interplay among the dephasing strength, the tunneling parameter, and the bridge length of the electron transfer system. (C) 2001 American Institute of Physics.

Blue-violet photoluminescence from large-scale highly aligned boron carbonitride nanofibers

We report on the strong blue-violet photoluminescence (PL) at room temperature from the large-scale highly aligned boron carbonitride (BCN) nanofibers synthesized by bias-assisted hot filament chemical vapor deposition. The photoluminescence peak wavelength shifts in the range of 470-390 nm by changing the chemical composition of the BCN nanofibers, which shows an interesting blue and violet-light-emitting material with adjustable optical properties. The mechanism for the shift of the PL peaks at room temperature is also discussed. (C) 2000 American Institute of Physics. [S0003-6951(00)04427-2].

Raman scattering of nanocrystalline silicon embedded in SiO2

Raman scattering of nanocrystalline silicon embedded in SiO2 matrix is systematically investigated. It is found that the Raman spectra can be well fitted by 5 Lorentzian lines in the Raman shift range of 100-600 cm(-1). The two-phonon scattering is also observed in the range of 600-1100 cm(-1) The experimental results indicate that the silicon crystallites in the films consist of nanocrystalline phase and amorphous phase; both can contribute to the Raman scattering. Besides the red-shift of the first order optical phonon modes with the decreasing size of silicon nanocrystallites, we have also found an enhancement effect on the second order Raman scattering, and the size effect on their Raman shift.

Absorption spectra of nanocrystalline silicon embedded in SiO2 matrix

Nanocrystalline silicon (nc-Si) embedded SiO2 matrix has been formed by annealing the SiOx films fabricated by plasma-enhanced chemical vapor deposition (PECVD) technique. Absorption coefficient and photoluminescence of the films have been measured at room temperature. The experimental results show that there is an "aUrbach-like" b exponential absorption in the spectral range of 2.0-3.0 eV. The relationship of (alpha hv)(1/2) proportional to(hv - E-g) demonstrates that the luminescent nc-Si have an indirect band structure. The existence of Stokes shift between photoluminescence and absorption edge indicates that radiative combination can take place not only between electron states and hole states but also between shallow trap states of electrons and holes. (C) 2000 Elsevier Science B.V. All rights reserved.

Investigation of absorption of nanocrystalline silicon

Nanocrystalline silicon embedded SiO2 matrix is formed by annealing the SiO2 films fabricated by plasma enhanced chemical vapor deposition technique. In conjunction with the micro-Ramam spectra, the absorption spectra of the films have been investigated. The blue-shift of absorption edge with decreasing size of silicon crystallites is due to quantum confinement effect. It is found that nanocrystalline silicon is of an indirect band structure, and that the absorption presents an exponential dependance absorption coefficient on photon energy ii! the range of 2.0-3.0 eV, and a sub-band appears in the the range of 1.0-1.5 eV. We believe that the exponential absorption is due to the indirect band-to-band transition of electrons in silicon nanocrystallites, while the Sub-band absorption is ascribed to transitions between the amorphous silicon states existing in the films.

Optical properties of nanocrystalline silicon embedded in SiO2

Nanocrystalline silicon embedded SiO2 matrix has been formed by annealing the a-SiOx films fabricated by plasma enhanced chemical vapor deposition technique. Absorption and photoluminescence spectra of, the films have been studied in conjunction with micro-Raman scattering spectra. It is found that absorption presents an exponential dependence of absorption coefficient to photon energy in the range of 1.5-3.0 eV, and a sub-band appears in the range of 1.0-1.5 eV. The exponential absorption is due to the indirect band-to-band transition of electrons in silicon nanocrystallites, while the sub-band absorption is ascribed to transitions between surfaces and/or defect states of the silicon nanocrystallites. The existence of Stokes shift between absorption and photoluminescence suggests that the phonon-assisted luminescence would he enhanced due to the quantum confinement effects.

Observation of field-driven blue shift in delta-doped Si n-i-p-i multiple quantum wells

We report the observation of the field-driven blue shift at near absorption edge in the photo-current response spectra of delta-doped Si n-i-p-i multiple quantum wells due to the widening of the effective energy gap. This phenomenon differs from the observed results in GaAs/AlGaAs and GeSi/Si superlattices, because the physical mechanisms of forming energy band in these superlattice samples are different. Our experimental results are interpreted satisfactorily by the theoretical calculation. (C) 1999 Elsevier Science Ltd. All rights reserved.

A Raman scattering study of GaAs: As films lifted off GaAs substrate

We performed Raman scattering investigations on low-temperature-grown (LTG) films of GaAs that had been lifted off the GaAs substrate. The Raman measurements unambiguously show the effects of excess arsenic on phonon scattering from LTG films of GaAs. The larger downwards shift of the LO phonon frequency for unannealed free-standing films is explained by invoking the elimination of mismatch strain. The Raman signal due to precipitates of elemental arsenic in the annealed GaAs : As films is determined. It is confirmed that the arsenic clusters formed by rapid thermal annealing are mainly amorphous, giving rise a broad Raman peak in the range 180-260 cm(-1).