Growth of Germanium Quantum Dots on Oxidized Silicon Surface

Russian Physics Journal - Epitaxial growth of germanium quantum dots on an oxidized silicon surface is considered. A kinetic model of the nucleation and growth of three-dimensional islands by the...     

Electron capture by tetra- and di-chlorobenzene molecules. Comparative studies by position annihilation and ODESR methods

Experiments on inhibition and anti-inhibition of Ps formation and also on optical detection of ESR spectra in squalene solutions with 1,2,4,5-C₆H₂Cl₄ and p-C₆H₄Cl₂ have demonstrated the presence of short-lived molecular radical-anions (products of the spur electron capture by additives), their lifetimes being longer than roughly 10 ps and shorter than 10–30 ns. The cross section of electron capture by p-C₆H₄Cl₂ in squalane is nearly one-tenth of that by 1,2,4,5-C₆H₂Cl₄ and CCl₄ at concentration ? 0.02 M, while 10% of the electrons cannot be trapped even at 0.25 M p-C₆H₄Cl₂. Probably the electrons in the high-electric-field (0.3–3 MV/cm) regions of the spurs cannot be effectively captured by p-C₆H₄Cl₂, which is a shallow electron trap. Similar effects of the high electric fields of the charged spur series seem to influence the Ps formation appreciably, along with the other effects discussed in previous papers. Several new results can be predicted, by use of this interpretation. Both methods employed are emphasized to be selective with respect to geminate spur particles.     

Heterostructures with self-organized quantum dots of Ge on Si for optoelectronic devices

In this paper an analysis of tendencies of Ge on Si quantum dots nanoheterostructures’ usage in different optoelectronic devices such as, for example, solar cells and photodetectors of visible and infra-red regions is carried out; a complex mathematical model for calculation of dependency on growth conditions of self-organized quantum dots of Ge on Si grown using the method of molecular beam epitaxy parameters is described. Ways of segregation effect and underlying layers’ influence are considered. It is shown that for realization of good device characteristics quantum dots should have high density, small sizes, uniformity, and narrow size distribution function. The desirable parameters of arrays of square and rectangular quantum dots for device application are attainable under certain growth conditions.     

Control of molecular fragmentation using shaped femtosecond pulses

The possibility that chemical reactions may be controlled by tailored femtosecond laser pulses has inspired recent studies that take advantage of their short pulse duration, comparable to intramolecular dynamics, and high peak intensity to fragment and ionize molecules. In this article, we present an experimental quest to control the chemical reactions that take place when isolated molecules interact with shaped near-infrared laser pulses with peak intensities ranging from 1013 to 1016 W/cm2. Through the exhaustive evaluation of hundreds of thousands of experiments, we methodically evaluated the molecular response of 16 compounds, including isomers, to the tailored light fields, as monitored by time-of-flight mass spectrometry. Analysis of the experimental data, taking into account its statistical significance, leads us to uncover important trends regarding the interaction of isolated molecules with an intense laser field. Despite the energetics involved in fragmentation and ionization, the integrated second-harmonic generation of a given laser pulse (ISHG), which was recorded as an independent diagnostic parameter, was found to be linearly proportional to the total ion yield (IMS) generated by that pulse in all of our pulse shaping measurements. Order of magnitude laser control over the relative yields of different fragment ions was observed for most of the molecules studied; the fragmentation yields were found to vary monotonically with IMS and/or ISHG. When the extensive changes in fragmentation yields as a function of IMS were compared for different phase functions, we found essentially identical results. This observation implies that fragmentation depends on a parameter that is responsible for IMS and independent from the particular time-frequency structure of the shaped laser pulse. With additional experiments, we found that individual ion yields depend only on the average pulse duration, implying that coherence does not play a role in the observed changes in yield as a function of pulse shaping. These findings were consistently observed for all molecules studied (p-, m-, o-nitrotoluene, 2,4-dinitrotoluene, benzene, toluene, naphthalene, azulene, acetone, acetyl chloride, acetophenone, p-chrolobenzonitrile, N,N-dimethylformamide, dimethyl phosphate, 2-chloroethyl ethyl sulfide, and tricarbonyl-[eta5-1-methyl-2,4-cyclopentadien-1-yl]-manganese). The exception to our conclusion is that the yield of small singly-charged fragments resulting from a multiple ionization process in a subset of molecules, were found to be highly sensitive to the phase structure of the intense pulses. This coherent process plays a minimal role in photofragmentation; therefore, we consider it an exception rather than a rule. Changes in the fragmentation process are dependent on molecular structure, as evidenced in a number of isomers, therefore femtosecond laser fragmentation could provide a practical dimension to analytical chemistry techniques.     

Femtosecond vibrational nuclear dynamics in the electronically excited state of the I2 molecule

Dynamics of the nuclear motion in the bound electronic B-state of the I₂ molecule was studied in the real time scale. Experiments were performed by the femtosecond pump-probe technique, which measured the dependence of the intensity of fluorescenceP(t) in the highly excited f-state on the time delay between pump and probe pulses. TheP(t) dependence observed has an oscillating character with a period of –300 fs. The pump pulse was generated by a femtosecond dye laser and amplified in a pulse dye laser amplifier; its spectral width was 5.6 nm, the wavelength in the center of the spectrum was 614 nm, and the duration was 90 fs. The probe pulse was generated in a KDP crystal due to duplication of the light frequency; its spectral width was 1.2 nm, the wavelength in the center of the spectrum was 307 nm, and the duration was 120 fs. TheP(t) dependence on the parameters of the probe and pump pulses was theoretically analyzed in terms of the quantum model based on the known energies of electronic vibrational-rotational states in the X-, B-, and f-terms of the iodine molecule. Experimental and calculatedP(t) plots at time delays of up to l.5 ps and time resolution of less than 100 fs were compared. Values of potentials in the X-, B-, and f-terms of the iodine molecule, spectra, and durations of pump and probe pulses are sufficient data for quantitative calculation of the experimentally obtainedP(t) plot.Translated fromIzvestiya Akademii Nauk. Seriya Khimicheskaya, No. 3, pp. 594–600, March, 1996.     

Mechanism elucidation for nonstochastic femtosecond laser-induced ionization/dissociation: from amino acids to peptides

Femtosecond laser-induced ionization/dissociation (fs-LID) has been demonstrated as a novel ion activation method for use in tandem mass spectrometry. The technique opens the door to unique structural information about biomolecular samples that is not easily accessed by traditional means. fs-LID is able to cleave strong bonds while keeping weaker bonds intact. This feature has been found to be particularly useful for the mapping of post-translational modifications such as phosphorylation, which is difficult to achieve by conventional proteomic studies. Here we investigate the laser-ion interaction on a fundamental level through the characterization of fs-LID spectra for the protonated amino acids and two series of derivatized samples. The findings are used to better understand the fs-LID spectra of synthetic peptides. This is accomplished by exploring the effects of several single-residue substitutions.     

Systematic control of nonlinear optical processes using optimally shaped femtosecond pulses.

This article reviews experimental efforts to control multiphoton transitions using shaped femtosecond laser pulses, and it lays out the systematic study being followed by us for elucidating the effect of phase on nonlinear optical laser-molecule interactions. Starting with a brief review of nonlinear optics and how nonlinear optical processes depend on the electric field inducing them, a number of conclusions can be drawn directly from analytical solutions of the equations. From a Taylor expansion of the phase in the frequency domain, we learn that nonlinear optical processes are affected only by the second- and higher-order terms. This simple result has significant implications on how pulse-shaping experiments are to be designed. If the phase is allowed to vary arbitrarily as a continuous function, then an infinite redundancy that arises from the addition of a linear phase function across the spectrum with arbitrary offset and slope could prevent us from carrying out a closed-loop optimization experiment. The early results illustrate how the outcome of a nonlinear optical transition depends on the cooperative action of all frequencies in the bandwidth of a laser pulse. Maximum constructive or destructive interference can be achieved by programming the phase using only two phase values, 0 and pi. This assertion has been confirmed experimentally, where binary phase shaping (BPS) was shown to outperform other alternative functions, sometimes by at least on order of magnitude, in controlling multiphoton processes. Here we discuss the solution of a number of nonlinear problems that range from narrowing the second harmonic spectrum of a laser pulse to optimizing the competition between two- and three-photon transitions. This Review explores some present and future applications of pulse shaping and coherent control.     

Modeling the formation kinetics of wedge-shaped germanium quantum dots on silicon

A mathematical model for calculating the dependences of the parameters of self-organized germanium quantum dots (QDs) on silicon on the conditions of growth in molecular beam epitaxy is described. The energies of formation for pyramidal and wedge-shaped islands in the Ge/Si(001) system are calculated with allowance for the contributions from surface energy and elastic stress relaxation, and the drop in the energy of attraction between atoms and the substrate.