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Title: Ultrafast laser dynamics and interactions in complex materials

Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
OSTI Identifier:
Report Number(s):
IS-T 3212
DOE Contract Number:
Resource Type:
Country of Publication:
United States

Citation Formats

Patz, Aaron. Ultrafast laser dynamics and interactions in complex materials. United States: N. p., 2017. Web. doi:10.2172/1417983.
Patz, Aaron. Ultrafast laser dynamics and interactions in complex materials. United States. doi:10.2172/1417983.
Patz, Aaron. Sat . "Ultrafast laser dynamics and interactions in complex materials". United States. doi:10.2172/1417983.
title = {Ultrafast laser dynamics and interactions in complex materials},
author = {Patz, Aaron},
abstractNote = {},
doi = {10.2172/1417983},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sat May 06 00:00:00 EDT 2017},
month = {Sat May 06 00:00:00 EDT 2017}

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  • This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.
  • Lasers having picosecond and shorter pulse duration are receiving much attention due to their capabilities for direct-write micromachining on many materials with minimal substrate damage. Substantial progress has been made in the understanding of laser ablation processes, particularly the creation of plasmas that often shield the target and reduce the material processing efficiency at nanosecond time scales. However, a considerable challenge that still remains is the understanding of the underlying mechanisms during picosecond laser interactions with electronic solids. In this work we first study picosecond laser-induced electron emission from semiconductor surfaces. A theoretical model was set up based on carriermore » transport inside the semiconductor material during picosecond laser-semiconductor interactions. We demonstrate that nonequilibrium carrier dynamics plays a significant role for picosecond, as well as short nanosecond, laser induced electron emission from semiconductors. Photoelectric effect is found to be responsible for electron emission at low incident laser fluences, whereas thermionic emission is dominant at higher fluences. We have also performed experimental and theoretical studies on the formation and subsequent evolution of plasmas during laser-metal interactions at the picosecond time scale. Using picosecond time-resolved shadowgrams ahd interferograms, a novel type of plasma is observed, which has an electron density on the order of 1020cm -3.The origin of this picosecond plasma is attributed to gas breakdown, which is caused by laser-induced electron emission fi-om the target surface. After the laser pulse is completed, the longitudinal expansion of the plasma is suppressed. This suppression is found to result from an electric field above the target that prevents, after laser irradiation, fbrther movement of the electrons inside the plasma. Measurements of lateral plasma expansion indicate that the picosecond plasma may absorb substantial amount of incident laser energy during laser irradiation. This result is consistent with the measurements of laser ablation efficiency, which levels off when the laser fluence exceeds a certain threshold. The information provided in this work would be essential for precise control of laser energy coupling with materials, particularly for machining at microscale depth.« less
  • Many laser ablation applications such as laser drilling and micromachining generate cavity structures. The study of laser ablation inside a cavity is of both fundamental and practical significance. In this dissertation, cavities with different aspect ratios (depth/diameter) were fabricated in fused silica by laser micromachining. Pulsed laser ablation in the cavities was studied and compared with laser ablation on a flat surface. The formation of laser-induced plasmas in the cavities and the effects of the cavities on the ablation processes were investigated. The temperatures and electron number densities of the resulting laser-induced plasmas in the cavities were determined from spectroscopicmore » measurements. Reflection and confinement effects by the cavity walls and plasma shielding were discussed to explain the increased temperature and electron number density with respect to increasing cavity aspect ratio. The temporal variations of the plasma temperature and electron number density inside the cavity decreased more rapidly than outside the cavity. The effect of laser energy on formation of a plasma inside a cavity was also investigated. Propagation of the shock wave generated during pulsed laser ablation in cavities was measured using laser shadowgraph imaging and compared with laser ablation on a flat surface. It is found that outside the cavity, after about 30 ns the radius of the expanding shock wave was proportional to t2/5, which corresponds to a spherical blast wave. The calculated pressures and temperatures of the shocked air outside of the cavities were higher than those obtained on the flat surface. Lasers with femtosecond pulse duration are receiving much attention for direct fabrication of microstructures due to their capabilities of high-precision ablation with minimal damage to the sample. We have also performed experimental studies of pulsed femtosecond laser ablation on the flat surface of silicon samples and compared results with pulsed nanosecond laser ablation at a ultraviolet wavelength (266 nm). Crater depth measurements indicated that ablation efficiency was enhanced for UV femtosecond laser pulses. The electron number densities and temperatures of femtosecond-pulse plasmas decreased faster than nanosecond-pulse plasmas due to different energy deposition mechanisms. Plasma expansion in both the perpendicular and the lateral directions were studied.« less
  • The complete description of a chemical reaction in solution depends upon an understanding of the reactive molecule as well as its interactions with the surrounding solvent molecules. Using ultrafast infrared spectroscopy it is possible to observe both the solute-solvent interactions and the rearrangement steps which determine the overall course of a chemical reaction. The topics addressed in these studies focus on reaction mechanisms which require the rearrangement of complex ligands and the spectroscopic techniques necessary for the determination of these mechanisms. Ligand rearrangement is studied by considering two different reaction mechanisms for which the rearrangement of a complex ligand constitutesmore » the most important step of the reaction. The first system concerns the rearrangement of a cyclopentadienyl ring as the response of an organometallic complex to a loss of electron density. This mechanism, commonly referred to as ''ring slip'', is frequently cited to explain reaction mechanisms. However, the ring slipped intermediate is too short-lived to be observed using conventional methods. Using a combination of ultrafast infrared spectroscopy and electronic structure calculations it has been shown that the intermediate exists, but does not form an eighteen-electron intermediate as suggested by traditional molecular orbital models. The second example examines the initial steps of alkyne polymerization. Group 6 (Cr, Mo, W) pentacarbonyl species are generated photolytically and used to catalyze the polymerization of unsaturated hydrocarbons through a series of coordination and rearrangement steps. Observing this reaction on the femto- to millisecond timescale indicates that the initial coordination of an alkyne solvent molecule to the metal center results in a stable intermediate that does not rearrange to form the polymer precursor. This suggests that polymerization requires the dissociation of additional carbonyl ligands before rearrangement can occur. Overall, this research demonstrates the importance of examining reaction dynamics on the ultrafast timescale. In the case of both ring slip and alkyne polymerization, early time dynamics have been invaluable in understanding the exact reaction mechanisms which show important differences from previously accepted models.« less
  • Femtosecond time- and angle-resolved two-photon photoemission spectroscopy has been used to study fundamental aspects of excited electron dynamics at metal-dielectric interfaces, including layer-by-layer evolution of electronic structure and two-dimensional electron localization. On bare Ag(111), the lifetimes of image states are dominated by their position with respect to the projected bulk band structure. The n = 2 state has a shorter lifetime than the n = 1 state due to degeneracy with the bulk conduction band. As the parallel momentum of the n = 1 image electron increases, the lifetime decreases. With decreasing temperatures, the n = 1 image electrons, withmore » zero or nonzero parallel momentum, all become longer lived. Adsorption of one to three layers of n-heptane results in an approximately exponential increase in lifetime as a function of layer thickness. This results from the formation of a tunneling barrier through which the interfacial electrons must decay, consistent with the repulsive bulk electron affinity of n-alkanes. The lifetimes of the higher quantum states indicate that the presence of the monolayer significantly reduces coupling of the image states to the bulk band structure. These results are compared with predictions of a dielectric continuum model. The study of electron lateral motion shows that optical excitation creates interfacial electrons in quasifree states for motion parallel to the n-heptane/Ag(111) interface. These initially delocalized electrons decay into a localized state within a few hundred femtoseconds. The localized electrons then decay back to the metal by tunneling through the adlayer potential barrier. The localization time depends strongly on the electron's initial parallel momentum and exhibits a non-Arrhenius temperature dependence. The experimental findings are consistent with a 2-D self-trapping process in which electrons become localized by interacting with the topmost plane of the alkane layer. The energy dependence of the self-trapping rate has been modeled with an electron transfer theory. This analysis shows that self-trapping involves inter- and intramolecular vibrational modes of the overlayer and the non-Arrhenius temperature dependence is a result of a strong quantum contribution from the intramolecular modes. These results for a model interface contribute to the fundamental understanding of electron behavior at the interface between metals and molecular solids.« less