Electron tomography of (In,Ga)N insertions in GaN nanocolumns grown on semi-polar (11(2)over-bar2) GaN templates

We present results of scanning transmission electron tomography on GaN/(In,Ga)N/GaN nanocolumns (NCs) that grew uniformly inclined towards the patterned, semi-polar GaN( 112̄ 2 ) substrate surface by molecular beam epitaxy. For the practical realization of the tomographic experiment, the nanocolumn axis has been aligned parallel to the rotation axis of the electron microscope goniometer. The tomographic reconstruction allows for the determination of the three-dimensional indium distribution inside the nanocolumns. This distribution is strongly interrelated with the nanocolumn morphology and faceting. The (In,Ga)N layer thickness and the indium concentration differ between crystallographically equivalent and non-equivalent facets. The largest thickness and the highest indium concentration are found at the nanocolumn apex parallel to the basal planes.

Electrocatalytic oxidation enhancement at the surface of InGaN films and nanostructures grown directly on Si(111)

Pronounced electrocatalytic oxidation enhancement at the surface of InGaN layers and nanostructures directly grown on Si by plasma-assisted molecular beam epitaxy is demonstrated. The oxidation enhancement, probed with the ferro/ferricyanide redox couple increases with In content and proximity of nanostructure surfaces and sidewalls to the c-plane. This is attributed to the corresponding increase of the density of intrinsic positively charged surface donors promoting electron transfer. Strongest enhancement is for c-plane InGaN layers functionalized with InN quantum dots (QDs). These results explain the excellent performance of our InN/InGaN QD biosensors and water splitting electrodes for further boosting efficiency.

Femtosecond spectroscopy of molecular autoionization and fragmentation

Femtosecond laser pulses are applied to the study of the dynamics and the pathways of multiphoton-induced ionization, autoionization, and fragmentation of Na_2 in molecular-beam experiments. In particular, we report on first results obtained studying electronic autoionization (leading to Na_2{^+} + {e ^-}) and autoionization-induced fragmentation (leading to Na{^+} + Na + {e ^-}) of a bound doubly excited molecular state. The final continuum states are analyzed by photoelectron spectroscopy and by measuring the mass and the released kinetic energy of the corresponding ionic fragments with a time-of-flight arrangement.

Femtosecond time-resolved wave packet motion in molecular multiphoton ionization and fragmentation

The dynamics of molecular multiphoton ionization and fragmentation of a diatomic molecule (Na_2) have been studied in molecular beam experiments. Femtosecond laser pulses from an amplified colliding-pulse mode-locked (CPM) ring dye laser are employed to induce and probe the molecular transitions. The final continuum states are analyzed by photoelectron spectroscopy, by ion mass spectrometry and by measuring the kinetic energy of the formed ionic fragments. Pump-probe spectra employing 70-fs laser pulses have been measured to study the time dependence of molecular multiphoton ionization and fragmentation. The oscillatory structure of the transient spectra showing the dynamics on the femtosecond time scale can best be understood in terms of the motion of wave packets in bound molecular potentials. The transient Na_2^+ ionization and the transient Na^+ fragmentation spectra show that contributions from direct photoionization of a singly excited electronic state and from excitation and autoionization of a bound doubly excited molecular state determine the time evolution of molecular multiphoton ionization.

Femtosecond time-resolved molecular multiphoton ionization: the Na_2 system

We report here the first experimental study of femtosecond time-resolved molecular multiphoton ionization. Femtosecond pump-probe techniques are combined with time-of-flight spectroscopy to measure transient ionization spectra of Na_2 in a molecular-beam experiment. The wave-packet motions in different molecular potentials show that incoherent contributions from direct photoionization of a singly excited state and from excitation and autoionization of a bound doubly excited molecular state determine the observed transient ionization signal.

Molecular photochemistry with femtosecond laser pulses

Femtosecond laser pulses generated from an amplified coiliding pulse modelocked ring dye laser have been employed in molecular beam experiments to study the dynamics and the pathways of multiphoton induced ionization, autoionization and fragmentation of Na2 . Energy distributions of photoelectrons arising from these processes and the mass and released kinetic energy of the corresponding fragment ions are measured by time-of-flight spectroscopy.

Lanczos subspace time-independent wave packet calculations of S(D-1)+H-2 reactive scattering

In this paper. we present the results of quantum dynamical simulations of the S (D-1) + H-2 insertion reaction on a newly developed potential energy surface (J. Chem. Phys. 2001, 114, 320). State-to-state reaction probabilities. product state distributions, and initial-state resolved cumulative reaction probabilities from a given incoming reactant channel are obtained from a time-independent wave packet analysis, performed within a single Lanczos subspace. Integral reaction cross sections are then estimated by J-shifting method and compared with the results from molecular beam experiment and QCT calculations.

Prediction of absolute rate coefficients and product branching ratios for the C(P-3) plus allene reaction system

Complex chemical reactions in the gas phase can be decomposed into a network of elementary (e.g., unimolecular and bimolecular) steps which may involve multiple reactant channels, multiple intermediates, and multiple products. The modeling of such reactions involves describing the molecular species and their transformation by reaction at a detailed level. Here we focus on a detailed modeling of the C(P-3)+allene (C3H4) reaction, for which molecular beam experiments and theoretical calculations have previously been performed. In our previous calculations, product branching ratios for a nonrotating isomerizing unimolecular system were predicted. We extend the previous calculations to predict absolute unimolecular rate coefficients and branching ratios using microcanonical variational transition state theory (mu-VTST) with full energy and angular momentum resolution. Our calculation of the initial capture rate is facilitated by systematic ab initio potential energy surface calculations that describe the interaction potential between carbon and allene as a function of the angle of attack. Furthermore, the chemical kinetic scheme is enhanced to explicitly treat the entrance channels in terms of a predicted overall input flux and also to allow for the possibility of redissociation via the entrance channels. Thus, the computation of total bimolecular reaction rates and partial capture rates is now possible. (C) 2002 American Institute of Physics.

Neutral C60 effusive source for atomic collisions with fullerene

Review of scientific instruments, Vol.72, Nº9

Photothermal deflection measurement on heat transport in GaAs epitaxial layers

In this paper, we report the in-plane and cross-plane measurements of the thermal diffusivity of double epitaxial layers of n-type GaAs doped with various concentrations of Si and a p-type Be-doped GaAs layer grown on a GaAs substrate by the molecular beam epitaxial method, using the laser-induced nondestructive photothermal deflection technique. The thermal diffusivity value is evaluated from the slope of the graph of the phase of the photothermal deflection signal as a function of pump-probe offset. Analysis of the data shows that the cross-plane thermal diffusivity is less than that of the in-plane thermal diffusivity. It is also seen that the doping concentration has a great influence on the thermal diffusivity value. Measurement of p-type Be-doped samples shows that the nature of the dopant also influences the effective thermal diffusivity value. The results are interpreted in terms of a phonon-assisted heat transfer mechanism and the various scattering process involved in the propagation of phonons.

Photothermal deflection measurement on heat transport in GaAs epitaxial layers

In this paper, we report the in-plane and cross-plane measurements of the thermal diffusivity of double epitaxial layers of n-type GaAs doped with various concentrations of Si and a p-type Be-doped GaAs layer grown on a GaAs substrate by the molecular beam epitaxial method, using the laser-induced nondestructive photothermal deflection technique. The thermal diffusivity value is evaluated from the slope of the graph of the phase of the photothermal deflection signal as a function of pump-probe offset. Analysis of the data shows that the cross-plane thermal diffusivity is less than that of the in-plane thermal diffusivity. It is also seen that the doping concentration has a great influence on the thermal diffusivity value. Measurement of p-type Be-doped samples shows that the nature of the dopant also influences the effective thermal diffusivity value. The results are interpreted in terms of a phonon-assisted heat transfer mechanism and the various scattering process involved in the propagation of phonons

Photothermal deflection measurement on heat transport in GaAs epitaxial layers

In this paper, we report the in-plane and cross-plane measurements of the thermal diffusivity of double epitaxial layers of n-type GaAs doped with various concentrations of Si and a p-type Be-doped GaAs layer grown on a GaAs substrate by the molecular beam epitaxial method, using the laser-induced nondestructive photothermal deflection technique. The thermal diffusivity value is evaluated from the slope of the graph of the phase of the photothermal deflection signal as a function of pump-probe offset. Analysis of the data shows that the cross-plane thermal diffusivity is less than that of the in-plane thermal diffusivity. It is also seen that the doping concentration has a great influence on the thermal diffusivity value. Measurement of p-type Be-doped samples shows that the nature of the dopant also influences the effective thermal diffusivity value. The results are interpreted in terms of a phonon-assisted heat transfer mechanism and the various scattering process involved in the propagation of phonons

Photoacoustic measurement of transport properties in doped GaAs epitaxial layers

The photoacoustic technique under heat transmission configuration is used to determine the effect of doping on both the thermal and transport properties of p- and n-type GaAs epitaxial layers grown on GaAs substrate by the molecular beam epitaxial method. Analysis of the data is made on the basis of the theoretical model of Rosencwaig and Gersho. Thermal and transport properties of the epitaxial layers are found by fitting the phase of the experimentally obtained photoacoustic signal with that of the theoretical model. It is observed that both the thermal and transport properties, i.e. thermal diffusivity, diffusion coefficient, surface recombination velocity and nonradiative recombination time, depend on the type of doping in the epitaxial layer. The results clearly show that the photoacoustic technique using heat transmission configuration is an excellent tool to study the thermal and transport properties of epitaxial layers under different doping conditions.

Femtosecond real-time probing of reactions. 12. Vectorial dynamics of transition states

Femtosecond time-resolved techniques with KETOF (kinetic energy time-of-flight) detection in a molecular beam are developed for studies of the vectorial dynamics of transition states. Application to the dissociation reaction of IHgI is presented. For this system, the complex [I---Hg---I](++)* is unstable and, through the symmetric and asymmetric stretch motions, yields different product fragments: [I---Hg---I](++)* -> HgI(X^2/sigma^+) + I(^2P_3/2) [or I*(^2P_l/2)] (1a); [I---Hg---I](++)* -> Hg(^1S_0) + I(^2P_3/2) + I(^2P_3/2) [or I* (^2P_1/2)] (1 b). These two channels, (1a) and (1b), lead to different kinetic energy distributions in the products. It is shown that the motion of the wave packet in the transition-state region can be observed by MPI mass detection; the transient time ranges from 120 to 300 fs depending on the available energy. With polarized pulses, the vectorial properties (transition moments alignment relative to recoil direction) are studied for fragment separations on the femtosecond time scale. The results indicate the nature of the structure (symmetry properties) and the correlation to final products. For 311-nm excitation, no evidence of crossing between the I and I* potentials is found at the internuclear separations studied. (Results for 287-nm excitation are also presented.) Molecular dynamics simulations and studies by laser-induced fluorescence support these findings.

Femtosecond real-time probing of reactions. 13. Multiphoton dynamics of IHgI

Real-time studies of the dynamics were performed on the reaction of HgI_2 in a molecular beam. Excitation was by either one or multi pump photons (311 nm), leading to two separate sets of dynamics, each of which could be investigated by a time-delayed probe laser (622 nm) that ionized the parent molecule and the fragments by REMPI processes. These dynamics were distinguished by combining the information from transients taken at each mass (HgI_2, HgI, I_2, Hg, and I) with the results of pump (and probe) power dependence studies on each mass. A method of plotting the slope of the intensity dependence against the pump-probe time delay proved essential. In the preceding publication, we detailed the dynamics of the reaction initiated by a one photon excitation to the A-continuum. Here, we present studies of higher-energy states. Multiphoton excitation accesses predissociative states of HgI_2, for which there are crossings into the symmetric and asymmetric stretch coordinates. The dynamics of these channels, which lead to atomic (I or Hg) and diatomic (HgI) fragments, are discussed and related to the nature of the intermediates along the reaction pathway.