Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Dissociation”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 973 records · Page 54
All sourcesNASA NTRSDOE OSTI
NASA NTRS2012

The Influence of Large Solar Proton Events on the Atmosphere

Solar proton events (SPEs) can cause changes in constituents in the Earth s polar middle atmosphere. A number of large SPEs have occurred over the past 50 years and tend to happen most frequently near solar maximum. The highly energetic protons cause ionizations, excitations, dissociations, and dissociative ionizations of the background constituents. Complicated ion chemistry leads to HOx (H, OH, HO2) production and dissociation of N2 leads to NOy (N, NO, NO2, NO3, N2O5, HNO3, HO2NO2, ClONO2, BrONO2) production. Both the HOx and NOy increases can result in changes to ozone in the stratosphere and mesosphere. The HOx increases lead to short-lived (~days) ozone decreases in the mesosphere and upper stratosphere. The NOy increases lead to long-lived (~several months) stratospheric ozone changes because of the long lifetime of NOy constituents in this region. UARS HALogen Occultation Experiment (HALOE) instrument observations showed SPE-caused polar stratospheric NOx (NO+NO2) increases over 10 ppbv in September 2000 due to the very large SPE of July 2000, which are reasonably well simulated with the Whole Atmosphere Community Climate Model (WACCM). WACCM-computed SPE-caused polar stratospheric ozone decreases >10% continued for up to 5 months past the largest events in the past 50 years, however, SPE-caused total ozone changes were not found to be statistically significant. Small polar middle atmospheric temperature changes of <4 K have also been predicted to occur as a result of the larger SPEs. The polar atmospheric effects of large SPEs during solar cycle 23 and 24 will be emphasized in this presentation.

Jackman, Charles H.↗
NASA NTRS2018

Characterization of CO Thermochemistry in Incident Shockwaves

Incident shock waves in pure CO have been characterized in the Electric Arc Shock Tube facility at NASA Ames Research Center. Spectrally and spatially resolved emission spectra characterize radiative signatures from CO in the VUV (Vacuum Ultra-Violet) and mid-infrared and atomic carbon and C2 in the visible. CO absorption of a single vibrational line is also measured with a tunable diode laser. The experimental data analyzed here are at a pressure of 0.25 Torr in the driven section and span a shock velocity range from 3.4-9.5 km/s. The emission and absorption signals are analyzed to extract temperature relaxation behind the shock which is used to derive the rate of CO dissociation. The emission spectra are compared to results using different kinetic parameters for CO dissociation and C2 dissociation and exchange. Different rates from the literature are found to match the data from 3.4-6.6 km/s and 6.6-9.5 km/s. Areas for improvement in CO and C2 radiation modeling are suggested on the basis of the analysis.

Entry↗
NASA NTRS2018

Characterization of CO Thermochemistry in Incident Shockwaves

Incident shock waves in pure CO have been characterized in the Electric Arc ShockTube facility at NASA Ames Research Center. Spectrally and spatially resolved emissionspectra characterize radiative signatures from CO in the VUV and mid-infrared and atomiccarbon and C2 in the visible. CO absorption of a single vibrational line is also measuredwith a tunable diode laser. The experimental data analyzed here are at a pressure of 0.25Torr in the driven section and span a shock velocity range from 3.4-9.5 km/s. The emissionand absorption signals are analyzed to extract temperature relaxation behind the shockwhich is used to derive the rate of CO dissociation. The emission spectra are compared toresults using different kinetic parameters for CO dissociation and C2 dissociation andexchange. Different rates from the literature are found to match the data from 3.4-6.6 km/sand 6.6-9.5 km/s. Areas for improvement in CO and C2 radiation modeling are suggested onthe basis of the analysis.

CO↗
NASA NTRSDate not supplied

TEMPERATURE CONSTRAINT OF THE MISTASTIN LAKE IMPACT STRUCTURE IMPACT MELT ROCKS

Impact melt is a product of hypervelocity cratering events formed by the instantaneous melting of near-surface target rocks. The temperatures of impact melt upon formation are believed to be superheated, vastly exceeding the liquidus temperature of igneous rocks formed via endogenic processes. However, quantitative understanding of the formation and duration of superheated temperatures remains incomplete. To date, only one datum on the hottest post-shock temperature (>2370 °C) has been derived by Timms et al. (2017) [1]. These authors studied the microstructures and crystallographic orientations preserved within a rim of vermicular ZrO2 of a zircon grain entrained within impact glass at the Mistastin Lake impact structure, Canada. Diagnostic crystallographic orientation indicated the presence of cubic zirconia, requiring a minimum temperature for the impact melt of >2370°C from the dissociation of zircon to cubic zirconia and liquid SiO2. With only one temperature datum, it cannot be stated whether the temperature of the impact melt sheet was homogenous across the entire structure or if the thermal history of the melt varied with spatial distribution. In this study, we present a preliminary investigation of 70 zircon grains, 22 of which exhibit rims of vermicular ZrO2 dissociation textures, similar to those studied by Timms et al. (2017). To acquire a more accurate temperature profile representative of impact melt, zircon crystals were collected from different types of impact melt bearing units, including additional samples of the impact glass studied by Timms et al. (2017). Of the 22 zircon grains with dissociation textures, at least 4 grains in the impact glass show diagnostic evidence of pre-existing cubic zirconia, and 1 grain from a glass-bearing breccia exhibits granular zircon textures, possible evidence of a transition from high-P to high-T conditions. These results show the heterogeneous post-shock temperature distribution of superheated impact melt within the Mistastin impact structure. [1] Timms, N.E., Erickson, T.M., Zanetti, M.R., Pearce, M.A., Cayron, C., Cavosie, A.J., Reddy, S.M., Wittmann, A. and Carpenter, P.K., 2017. Cubic zirconia in> 2370° C impact melt records Earth's hottest crust. Earth and Planetary Science Letters, 477, pp.52-58.

rock↗
NASA NTRSDate not supplied

Experimental and Theoretical Needs for the JWST Early Release Science Program on Radiative Feedback from Massive Stars (PDRs4ALL): III. A Quantum Chemistry Perspective

Massive stars disrupt their natal molecular cloud material by dissociating molecules, ionizing atoms and molecules, and heating the gas and dust. These processes drive the evolution of interstellar matter in our Galaxy and throughout the Universe from the era of vigorous star formation at z=1-3 to the present day. Much of this interaction occurs in Photo- Dissociation Regions (PDRs) where far-ultraviolet photons of these stars create a largely neutral, but warm region of gas and dust. PDR emission dominates the IR spectra of starforming galaxies and provides a unique tool to study the physical and chemical processes that are relevant for inter- and circumstellar media including diffuse clouds, molecular cloud and protoplanetary disk surfaces, and starburst galaxies. The ERS program ID1288 is dedicated to provide template data as well as data processing and analysis tools for PDRs. To this end, it will observe the Orion Bar, the proto-typical PDR situated in the nearby Orion Nebula, using NIRSpec IFU, MIRI IFU, and NIRCAM and MIRI imaging. These observations will, for the first time, spatially resolve and perform a tomography of the PDR, revealing the individual IR spectral signatures from the key zones and sub-regions within the ionized gas, the PDR, and the molecular cloud. Quantum chemistry can be used to determine molecular data such as ionization potentials, chemical reaction rates, electronic spectra, dissociation energies, channels, and branching ratios, etc. These are often used in synergy with experiment to take advantage of the strengths of each approach. An area of active research is modeling the infrared (IR) emission spectra produced by PAH molecules, including the effects of anharmonicity. This will be important in the interpretation of JWST data which will yield higher-resolution spectral data compared to Spitzer or ISO. Quantum chemistry methods can compute accurate anharmonic IR absorption spectra of PAH molecules up to about 25 C atoms, and the results have been benchmarked against high-resolution experimental spectra. These feed into a quantum Monte Carlo (QMC) approach to generate temperature-dependent anharmonic IR emission spectra and then used to generate fully anharmonic cascade emission IR spectra of PAH molecules -- the very type of spectra that JWST will observe. Work continues to extend these methods to larger PAH molecules. We will discuss the current state of this work, as well as

Timothy Lee↗
DOE OSTI2021

Excited state management

Arrangements and techniques for providing organic emissive layers are provided, in which the emissive layer includes a first dopant having a dissociative energy level. A second dopant in the emissive layer provides a solid state sink energy level, to which doubly excited excitons and/or polarons may transition instead of to the dissociative energy level, thereby decreasing the undesirable effects of transitions to the dissociative energy level.

Forrest, Stephen R.↗
DOE OSTI2023

Excited state management

Arrangements and techniques for providing organic emissive layers are provided, in which the emissive layer includes a first dopant having a dissociative energy level. A second dopant in the emissive layer provides a solid state sink energy level, to which doubly excited excitons and/or polarons may transition instead of to the dissociative energy level, thereby decreasing the undesirable effects of transitions to the dissociative energy level.

Forrest, Stephen R.↗
DOE OSTI2023

Acid–Base Chemistry of a Model IrO 2 Catalytic Interface

Iridium oxide (IrO 2 ) is one of the most efficient catalytic materials for the oxygen evolution reaction (OER), yet the atomic scale structure of its aqueous interface is largely unknown. Herein, the hydration structure, proton transfer mechanisms and acid-base properties of the rutile IrO 2 (110)-water interface are investigated using ab-initio based deep neural-network potentials and enhanced sampling simulations. The proton affinities of the different surface sites are characterized by calculating their acid dissociation constants, which yield a point of zero-charge in good agreement with experiments. A large fraction (≈ 80%) of adsorbed water dissociation is observed, together with a short lifetime (≈ 0.5 ns) of the resulting terminal hydroxy groups, due to rapid proton exchanges between adsorbed H 2 O and adjacent OH species. As a result, this rapid surface proton transfer supports the suggestion that the rate-determining step in the OER may not involve proton transfer across the double layer into solution, as indicated by recent experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

A deep learning-guided automated workflow in LipidOz for detailed characterization of fungal fatty acid unsaturation by ozonolysis

Understanding fungal lipid biology and metabolism is critical for antifungal target discovery as lipids play central roles in cellular processes. Nuances in lipid structural differences can significantly impact their functions, making it necessary to characterize lipids in detail to enable and understanding of their roles in these complex systems. In particular, lipid double bond (DB) locations are an important component of lipid structure that can only be determined using a few specialized analytical techniques. Ozone-induced dissociation mass spectrometry (OzID-MS) is one such technique that uses ozone to break lipid DBs, producing pairs of characteristic fragments that allow the determination of DB positions. In this work we apply OzID-MS and LipidOz software to analyze the complex lipids of Saccharomyces cerevisiae yeast strains transfected with different fatty acid desaturases from Histoplasma capsulatum to determine the specific unsaturated lipids produce. The automated data analysis in LipidOz made the determination of DB positions from this large dataset more practical, but manual verification for all targets was still time-consuming. The DL model reduces manual involvement in data analysis, but since it was trained using mammalian lipid extracts, the prediction accuracy on yeast-derived data was reduced. We addressed both shortcomings by retraining the DL model to act as a pre-filter to prioritize targets for automated analysis, providing confident manually verified results but requiring less computational time and manual effort. Our workflow resulted in the determination of novel DB positions and enzymatic specificity.

mass spectrometry, deep learning, Lipidomics, doub↗
DOE OSTI2025

Initiation of dusting corrosion in high-temperature alloys under CO exposure

Carbon monoxide is commonly encountered in energy systems, yet its reactivity with structural alloys—critical heat-resistant components in these systems—has been largely overlooked compared to the well-documented effects of oxidizing gases. In contrast, we demonstrate the high-temperature reaction of CO with NiAl using in-situ low-energy electron microscopy and X-ray photoemission electron microscopy. Our results show that CO dissociates into atomic oxygen and carbon, resulting in two concurrent reactions: selective oxidation of aluminum to form Al 2 O 3 and the initiation of dusting corrosion through carbon dissolution into the alloy and subsequent carbon deposition on the surface. These reactions produce spatially distinct surface products, preventing the formation of a continuous protective Al oxide layer. These results reveal a preference for the dissociative pathway of CO over the classic Boudouard disproportionation reaction that forms CO 2 . These insights not only advance our understanding of CO-induced alloy degradation but also highlight the practical implications for managing alloy stability and optimizing catalysis in carbon-rich environments, such as those in petrochemical processing and hydrocarbon combustion.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Silica modulated palladium catalyst with superior activity for the selective catalytic reduction of nitrogen oxides with hydrogen

A significant promotion effect of colloidal SiO 2 on Pd/TiO 2 catalyst for improving the activity and N 2 selectivity in the selective catalytic reduction of NO with H 2 (H 2 -SCR) was reported, both before and after hydrothermal aging. The SiO 2 addition not only benefited the formation of more oxygen vacancies but also increased Pd dispersion and created rich Pd-SiO 2 interfaces on Pd-SiO 2 /TiO 2 catalyst. The H 2 -SCR of NO on both Pd/TiO 2 and Pd-SiO 2 /TiO 2 followed a Langmuir-Hinshelwood mechanism, in which the adsorbed bridging bidentate nitrates on TiO 2 could react with dissociated H 2 species on Pd sites at Pd-TiO 2 interface. Particularly, on the promoted Pd-SiO 2 /TiO 2 , the Pd-TiO 2 interface could facilitate NO adsorption and activation, and the created Pd-SiO 2 interface could benefit H 2 adsorption and dissociation, thus contributing to its significantly improved H 2 -SCR activity. Additionally, the active Pd species (which should be Pd0 under reaction condition with higher surface concentration) within Pd-SiO 2 /TiO 2 could be well stabilized during long-term hydrothermal aging process through the formation of rich Pd-SiO 2 interfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Resolving SPARC–HSA binding kinetics with an ultrasensitive photonic sensor based on bound states in the continuum

Secreted protein acidic and rich in cysteine (SPARC) is critical in cell-matrix interactions and tissue remodeling. It influences tumor progression through its affinity for human serum albumin (HSA) - the most abundant plasma protein, which also plays a crucial role in drug delivery. Strong molecular binding leads to a dissociation constant KD in the nanomolar range. Thus, determining KD requires detecting sub-nanomolar concentrations with ultrasensitive methods. This may be crucial for elucidating the nature of SPARC-HSA binding, as their interaction remains a subject of debate. Capturing these interactions accurately requires a platform capable of resolving rapid binding kinetics at extremely low analyte concentrations. In this work, we report on a microfluidics-integrated photonic nanostructure that supports bound states in the continuum (BICs) and is optimized for studying the fast kinetics of high-affinity protein-protein interactions. The unprecedented capability of detecting sub-nanomolar concentrations allows quantifying KD between SPARC and HSA beyond the state of the art. We leverage an all-dielectric photonic crystal slab (PhCS) sustaining two BIC branches arising from gapped Dirac cone dispersion. HSA is covalently immobilized on the PhCS bonded to a PDMS microfluidic chamber. SPARC dissociation is carried out using PBS buffer (pH 7.4), ensuring complete protein release through precise control of the flow rate and continuous spectral monitoring of the BICs. The measured KD=8.2±0.8 nM confirms the strong affinity of SPARC for HSA. This study highlights the potential of BIC-based sensing as a versatile tool for investigating protein interactions. These results also have implications for the optimization of drug delivery systems and cancer treatment strategies.

Albumin↗
DOE OSTI2022

Re-evaluation of rate constants for the reaction N 2 H 4 (+ M) $^→_←$ NH 2 + NH 2 (+ M)

Rate constants for the dissociation/recombination reaction N 2 H 4 (+ M) $^→_←$ NH 2 + NH 2 (+ M) are determined by a combination of quantum-chemical calculations and statistical unimolecular rate theory. Between 1100 and 2500 K, limiting low-pressure rate constants for hydrazine dissociation in the bath gas Ar of k 0 = [Ar] 6.1 × 10 20 (T/1000 K) –7.3 exp (-34490 K/T) cm 3 mol –1 s –1 , limiting high-pressure rate constants of k ∞ = 7.6 × 10 16 (T/1000 K) –1.0 exp(-33600 K/T) s –1 , and center broadening factors of the falloff curves (between 1100 and 1600 K in Ar) of F cent = 0.71 exp(- T/1460 K) + 0.29 exp(- T/21 K) + exp(-13400 K/T) were calculated. Using equilibrium constants K C = 1.7 × 10 3 (T/1000 K) –1.5 exp(-33,460 K/T) mol cm –3 , between 300 and 600 K limiting low-pressure rate constants for the reverse recombination of NH 2 radicals in the bath gas N 2 of k rec,0 = [N 2 ] 4.4 × 10 20 (T/400 K) –6.9 exp (-1630 K/T) cm 6 mol –2 s –1 , limiting high-pressure rate constants of k rec,∞ = 4.4 × 10 13 (T/1000 K) 0.44 exp(-140 K/T) cm 3 mol -1 s –1 , and center broadening factors (between 300 and 600 K in N 2 ) of F cent = exp(- T/1130 K) + exp (-10340 K/T) were obtained. A comparison with experimental results for hydrazine dissociation from the literature suggests incomplete falloff extrapolations toward k ∞ and experimental problems in the determination of k 0 at temperatures above about 1600 K. Finally, implications of the present re-evaluated rate constants for the modeling of high temperature ammonia oxidation kinetics are discussed, showing an only small influence of their precise values on the overall properties of the process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Challenges in Kinetic modeling of ammonia pyrolysis

Ammonia pyrolysis reactions have implications for its ignition and oxidation in engines and gas turbines. In the present work, the chemistry of ammonia pyrolysis is investigated by kinetic modeling and theory. Rate constants for key reactions are carefully evaluated based on available experimental and theoretical results. The high pressure limit k1,∞ for NH 2 + H (+M) &rlarr; NH 3 (+M) (R1) is calculated to be essentially the collision frequency, indicating that dissociation of ammonia in combustion processes will be at or close to the low pressure limit even at engine and gas turbine conditions. The chemical kinetic model is validated against reported shock tube measurements of NH 3 , NH 2 , and NH in ammonia pyrolysis. Predictions are in good agreement with observations for dilute conditions (≤ 0.5% NH 3 ), but the model appears to underpredict the NH 3 consumption rate at longer times in less dilute mixtures. At short reaction times, thermal dissociation of NH3, together with the NH 3 + H reaction, controls conversion. At longer times, secondary reactions involving NH 2 and NH become important due to their impact on the radical pool. Predictions become sensitive to formation and consumption of diazene (tHNNH and cHNNH). Several of the key steps in the ammonia pyrolysis mechanism are radical-radical reactions that are difficult to measure accurately and challenging to calculate theoretically, and a more comprehensive experimental characterization is desirable to support further model development.

10 SYNTHETIC FUELS↗
DOE OSTI2023

Solvation dynamics of choline fluoride in ethylene glycol – Water mixtures

Due to their favorable physical properties, deep eutectic solvents (DESs) have been of interest in many applications in the energy and industry sectors. In this study, we investigate the new deep eutectic solvent ethalineF (a 1:2 M ratio of choline fluoride:ethylene glycol) and the effect of water addition on the solvation dynamics compared to the better known ethaline (a 1:2 M ratio of choline chloride:ethylene glycol). Femtosecond transient absorption spectroscopy and NMR diffusometry were used to study the solvation dynamics. 19 F NMR spectra were obtained for ethalineF solutions with different water additions. The 19 F NMR spectra show two fluorine signals; one can be assigned to fluoride anions solvated by EG and the other signal to fluoride anions associated with the much heavier and less mobile choline cation. Density, viscosity, conductivity, and E T (30) polarity measurements are also provided for ethalineF. The nuclear spin nature of fluorine atom permits to measure the self-diffusion coefficient of the negative ion in addition of the cation diffusion in a choline halide based deep eutectic solvent system. This allows to calculate the NMR-predicted conductivities σ NMR . The obtained ion dissociation coefficients α D at different water concentrations suggest a partial ion dissociation which was commensurate with the relatively low ion conductivity. Furthermore, the observed modest conductivity of ethalineF is explained in terms of ion association as well as the gradual increase in conductivity caused by the addition of water.

19F NMR↗
DOE OSTI2022

Numerical Simulations in Support of a Long-Term Test of Gas Production from Hydrate Accumulations on the Alaska North Slope: Reservoir Response to Interruptions of Production (Shut-Ins)

In this work, we investigate by means of numerical simulation a planned year-long field test of depressurization-induced production from a permafrost-associated hydrate reservoir on the Alaska North Slope at the site of the recently drilled Hydrate-01 Stratigraphic Test Well. The main objective of this study is to assess quantitatively the impact of temporary interruptions (well shut-ins) on the expected fluid production performance from the B1 Sand of the stratigraphic Unit B during controlled depressurization over different time scales, as well as on other relevant aspects of the system response that have the potential to significantly affect the design of the field test. We consider eight different cases of depressurization, including (a) rapid depressurization over a 60-day period to a terminal bottomhole pressure P W of 2.8 MPa and (b) a slower depressurization rate to a final P W of 0.6 MPa at the end of the year-long production test, in addition to (c) a multi-step depressurization regime and (d) a quasi-linear continuous depressurization strategy. The results of the study indicate that shut-ins obviously reduce gas release and production during and immediately after their occurrence, but their longer-term effects are strongly dependent on the depressurization regime and on the time of observation, covering the entire range of potential outcomes. Shut-ins (a) have a universally strong negative effect when quasi-linear depressurization is involved regardless of the length of the production period, and (b) have a strong positive effect in multi-step depressurization schemes that becomes apparent earlier for large initial pressure drops, but (c) can also appear to have practically no effect for slow stepwise depressurization at the end of the year-long production test. Shut-ins lead to a rapid reformation of hydrates, even to the point of disappearance of a free gas phase in the reservoir. Rapid depressurization regimes lead to early maximum rates of hydrate dissociation and gas production, while the maximum rates occur at the end of the production test for the cases of slower depressurization. Shut-ins do not appear to have a significant impact on water production, as the cessation of production is followed by higher rates production when depressurization resumes. Similarly, (a) the fraction of produced CH 4 originating from exsolution from the water, (b) the water-to-gas ratio, and (c) the rate of replenishment of produced water by boundary inflows do not appear significantly affected by shut-ins, the effects of which seem to be temporary in the majority of the cases. The study confirmed the superiority of multi-step depressurization methods as the most effective strategies for hydrate dissociation and gas production and showed that two observation wells (located at distances of 30 and 50 m from the production well) are appropriately positioned and both able to capture the P, T, and S G behavior during the fluid production and shut-ins in any of the eight cases we investigated.

03 NATURAL GAS↗
DOE OSTI2023

Molecular Simulation of Lithium Carbonate Reactive Vapor–Liquid Equilibria Using a Deep Potential Model

We developed a first-principles machine learning model for the reactive vapor–liquid phase behavior of molten Li 2 CO 3 . The model was trained on ab initio electronic density functional theory data using the Deep Potential (DP) methodology, and its accuracy was evaluated by comparing model predictions of density and viscosity to experimental measurements. Direct coexistence simulations with the DP model over time scales of tens of nanoseconds were used to observe equilibrium dissociation of Li 2 CO 3 into CO 2 residing primarily in the vapor phase and Li 2 O which remains dissolved in the liquid. The simulations covered a range of temperatures, overall system sizes, and vapor-to-liquid volume ratios. Results were analyzed in terms of the observed chemical composition of the liquid and vapor phases, product structure, and CO 2 partial pressures. In addition, we calculated equilibrium constants for the dissociation reaction by assuming ideal-solution behavior for the liquid. As expected on the basis of thermodynamic arguments and prior experiments for this system, the observed partial pressure of CO 2 in the gas phase depends on both the temperature and the ratio of vapor to liquid volumes, while the calculated equilibrium constants only depend on temperature. DP model predictions for the equilibrium constant of the reaction are generally consistent with the available experimental measurements. Furthermore, the present study establishes the validity of the DP methodology for the description of reactive, multiphase equilibria from first principles, with possible applications to many other systems of scientific and technological interest even in the absence of relevant experimental measurements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Photoionization and Photofragmentation Dynamics of I 2 in Intense Laser Fields: A Velocity-Map Imaging Study

The photoionization and photofragmentation dynamics of I 2 in intense femtosecond near-infrared laser fields were studied using velocity-map imaging of cations, electrons, and anions. A series of photofragmentation pathways originating from different cationic electronic states were observed following single ionization, leading to I + fragments with distinct kinetic energies, which could not be resolved in previous studies. Photoelectron spectra indicate that these high-lying dissociative states are primarily produced through nonresonant ionization from several molecular orbitals (MO) of the neutral. The photoelectron spectra also show clear signatures of resonant ionization pathways (Freeman resonances) to low-lying bound ionic states via Rydberg states of the neutral moiety. To investigate the role of these Rydberg states further, we imaged anionic products (I – ) formed through ion-pair dissociations of neutral molecules excited to these Rydberg states by the intense femtosecond laser pulse. Collectively, these results shed significant new light on the complex dynamics of I 2 molecules in intense laser fields and on the important role of neutral Rydberg states in a full description of strong-field phenomena in molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗