A Stochastic Approach for Investigation Ultrafast Phenomena in Semiconductors

2002 Mathematics Subject Classification: 65C05

Mechanisms in fs-laser ablation in fused silica

A theoretical model is proposed to describe the microscopic processes involved in the ablation in fused silica induced by femtosecond-laser pulse. Conduction-band electron (CBE) can absorb laser energy, the rate is calculated by quantum mechanical method and classical method. CBE is produced via photoionization (PI) and impact ionization (II). The PI and II rates are calculated by using the Keldysh theory and double-flux model, respectively. Besides the CBE production, we investigate laser energy deposition and its distribution. The equation of energy diffusion in physical space is resolved numerically. Taking energy density E-dep=54 kJ/cm(3) as the criterion, we calculate damage threshold, ablation depth, and ablation volumes. It is found that if energy diffusion is considered, energy density near sample surface is reduced to 1/10, damage threshold is enhanced more than 30%, ablation depth is increased by a factor of 10. Our theoretical results agree well with experimental measurements. Several ultrafast phenomena in fused silica are also discussed. (C) 2004 American Institute of Physics.

Femtosecond laser-induced breakdown of multilayers and gold film

unavailable<br>H. Sun's e-mail address is shy780327@siom.ac.cn.

Nonradiative recombination effect on photoluminescence decay dynamics in GaInNAs/GaAs quantum wells - art. no. 61180Z

The nonradiative recombination effect on the photoluminescence (PL) decay dynamics in GaInNAs/GaAs quantum wells is studied by photoluminescence and time-resolved photoluminescence under various excitation intensities and temperatures. It is found that the PL decay dynamics strongly depends on the excitation intensity. In particular, under the moderate excitation levels the PL decay curves exhibit unusual non-exponential behavior and show a convex shape. By introducing a new concept of the effective concentration of nonradiative recombination centers into a rate equation, the observed results are well simulated. In the cw PL measurement, a rapid PL quenching is observed even at very low temperature and is of the excitation power dependence. These results further demonstrate that the non-radiative recombination process plays a very important role on the optical properties of GaInNAs/GaAs quantum wells.

Electron trapping materials for use in a picosecond infrared streak camera

We describe our research on the employment of an infrared upconversion screen made of electron trapping material (ETM) in combination with the high sensitivity of the S-20 photocathode responsive to visible radiation to produce a streak camera arrangement capable of viewing and recording infrared incident pulses. The ETM-based upconversion screen converts 800-1600 nm infrared radiation to visible light which is viewed or recorded by the S-20 photocathode. The peak values of the upconversion efficiency are located at 1165 nm for CaS:Eu, Sm and 1060 nm for CaS:Ce, Sm. The present experiment showed time resolution was 12.3 ps for a CaS:Eu, Sm screen and 8.4 ps for a CaS:Ce, Sm screen. The minimum detectability is 4.8 x 10(-9) J/mm(2) (minimum detectability of the coupled visible streak camera is 8.3x10(-10) J/mm(2)). Other parameters, such as spatial resolution and dynamic range, have also been measured and analyzed. The results show ETM can be used in the measurement of infrared ultrafast phenomena up to picosecond time domain. In consideration of the limited number of trapped electrons in ETM, the infrared-sensitive streak camera consisting of an ETM-based upconversion screen is suitable to operate in the single shot mode. (C) 1999 American Institute of Physics. [S0034-6748(99)00112-4].

Femtosecond dynamics of molecular and cluster ionization and fragmentation

The real-time dynamics of molecular (Na_2 . Na_3) and cluster Na_n (n=4-2l) multiphoton ionization and -fragmentation has been studied in beam experiments applying femtosecond pump-probe techniques in combination with ion and electron spectroscopy. Wave packet motion in the dimer Na_2 reveals two independent multiphoton ionization processes while the higher dimensional motion in the trimer Na_3 reflects the chaotic vibrational motion in this floppy system. The first studies of cluster properties (energy, bandwidth and lifetime of intermediate resonances Na^*_n) ) with femtosecond laser pulses give a striking illustration of the transition from "molecule-like" excitations to "surfaceplasma"-like resonances for increasing cluster sizes. Time-resolved fragmentation of cluster ions Na_n^* indicate that direct photo-induced fragmentation processes are more important at short times than the statistical unimolecular decay.

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.

Ultrafast Chemical Dynamics in Time Domain Through Fluorescence Spectroscopy

While absorption and emission spectroscopy have always been used to detect and characterize molecules and molecular complexes, the availability of ultrashort laser pulses and associated computer-aided optical detection techniques allowed study of chemical processes directly in the time domain at unprecedented time scales, through appearance and disappearance of fluorescence from participating chemical species. Application of such techniques to chemical dynamics in liquids, where many processes occur with picosecond and femtosecond time scales lead to the discovery of a host of new phenomena that in turn led to the development of many new theories. Experiment and theory together provided new and valuable insight into many fundamental chemical processes, like isomerization dynamics, electron and proton transfer reactions, vibrational energy and phase relaxation, photosynthesis, to name just a few. In this article, we shall review a few of such discoveries in attempt to provide a glimpse of the fascinating research employing fluorescence spectroscopy that changed the field of chemical dynamics forever.

Ablation and ultrafast dynamics of zinc selenide under femtosecond laser irradiation

The ablation in zinc selenide (ZnSe) crystal is studied by using 150-fs, 800-nm laser system. The images of the ablation pit measured by scanning electronic microscope (SEM) show no thermal stress and melting dynamics. The threshold fluence is measured to be 0.7 J/cm2. The ultrafast ablation dynamics is studied by using pump and probe method. The result suggests that optical breakdown and ultrafast melting take place in ZnSe irradiated under femtosecond laser pulses.

Ultrafast double pulses ablation of Cr film on glass

Ultrafast lasers ablation of Cr film was investigated by using double-pulse method. Experimental results show that there exists a temporal ablation window effect with each of the double pulses adjusted just smaller than the threshold. When the delay between the double pulses is within the order of 400 ps, the ablation of Cr film could happen. When the delay between the double pulses is beyond the order of 400 ps, the ablation of Cr film would not happen, and the reflectivity from the surface of the Cr film shows a sharp rise at the same time. The two-temperature model was developed into the form of double pulses to explain the experimental phenomena. Furthermore, microbump structures were formed on the surface of Cr film after ablation by ultrafast double pulses. Their heights exhibit an obvious drop between 1 and 10 ps double pulses delay, which is involved with the electron-phonon coupling process according to the numerical simulation. These results should be helpful for understanding the dynamic processes during ultrafast lasers ablation of metal films. (C) 2008 Elsevier B.V. All rights reserved.

Evidence of ultrafast energy exchange-induced soft'mode of phonons and lattice instability: a nanotime effect

With a series of supportive experimental phenomena as induced by ion beam bombardment, energetic beaminduced athermal activation process in Si is demonstrated. This is correlated with phenomena induced by ultrafast energy exchange in condensed matter in general. A critical modelling is presented on the above process and a universal concept: the ultrafast energy exchange-induced soft mode of phonons and the lattice instability in condensed matter are proposed.

Ultrafast diffraction and structural dynamics: The nature of complex molecules far from equilibrium

Studies of molecular structures at or near their equilibrium configurations have long provided information on their geometry in terms of bond distances and angles. Far-from-equilibrium structures are relatively unknown—especially for complex systems—and generally, neither their dynamics nor their average geometries can be extrapolated from equilibrium values. For such nonequilibrium structures, vibrational amplitudes and bond distances play a central role in phenomena such as energy redistribution and chemical reactivity. Ultrafast electron diffraction, which was developed to study transient molecular structures, provides a direct method for probing the nature of complex molecules far from equilibrium. Here we present our ultrafast electron diffraction observations of transient structures for two cyclic hydrocarbons. At high internal energies of ≈4 eV, these molecules display markedly different behavior. For 1,3,5-cycloheptatriene, excitation results in the formation of hot ground-state structures with bond distances similar to those of the initial structure, but with nearly three times the average vibrational amplitude. Energy is redistributed within 5 ps, but with a negative temperature characterizing the nonequilibrium population. In contrast, the ring-opening reaction of 1,3-cyclohexadiene is shown to result in hot structures with a C—C bond distance of over 1.7 Å, which is 0.2 Å away from any expected equilibrium value. Even up to 400 ps, energy remains trapped in large-amplitude motions comprised of torsion and asymmetric stretching. These studies promise a new direction for studying structural dynamics in nonequilibrium complex systems.