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At least 73 records · Page 4

GMRES with embedded ensemble propagation for the efficient solution of parametric linear systems in uncertainty quantification of computational models

In a previous work, embedded ensemble propagation was proposed to improve the efficiency of sampling-based uncertainty quantification methods of computational models on emerging computational architectures. It consists of simultaneously evaluating the model for a subset of samples together, instead of evaluating them individually. A first approach introduced to solve parametric linear systems with ensemble propagation is ensemble reduction. In Krylov methods for example, this reduction consists in coupling the samples together using an inner product that sums the sample contributions. Ensemble reduction has the advantages of being able to use optimized implementations of BLAS functions and having a stopping criterion which involves only one scalar. However, the reduction potentially decreases the rate of convergence due to the gathering of the spectra of the samples. In this paper, we investigate a second approach: ensemble propagation without ensemble reduction in the case of GMRES. This second approach solves each sample simultaneously but independently to improve the convergence compared to ensemble reduction. This raises two new issues which are solved in this paper: the fact that optimized implementations of BLAS functions cannot be used anymore and that ensemble divergence, whereby individual samples within an ensemble must follow different code execution paths, can occur. We tackle those issues by implementing a high-performing ensemble GEMV and by using masks. The proposed ensemble GEMV leads to a similar cost per GMRES iteration for both approaches, i.e. with and without reduction. For illustration, we study the performances of the new linear solver in the context of a mesh tying problem. Furthermore, this example demonstrates improved ensemble propagation speed-up without reduction.

BLAS↗

Oxidation Dynamics of Supported Catalytic Cu Clusters: Coupling to Fluxionality

Copper oxide nanoclusters have a wide range of catalytic applications, such as the selective oxidation of hydrocarbons. O 2 binding to the catalyst, activation, and release upon reagent oxidation are key events in these catalytic chemistries. Furthermore, these events are expected to be accompanied by significant structural changes of the Cu clusters, because O atoms integrate into the cluster, rather than bind to its surface. Topping the complexity of the problem, partially oxidized Cu clusters are known to exhibit strong fluxionality and feature diverse and interconverting structures and oxygen contents in conditions of oxidative dehydrogenation (ODH). Hence, a significant dynamic coupling between the “hot” O 2 molecule impacting the cluster at reaction temperatures and the cluster fluxionality can be expected. In this work, we focus on the dynamics of dioxygen integration into a partially oxidized Cu cluster supported on hydroxylated amorphous alumina–a system recently reported to be an exceptionally selective catalyst for cyclohexane ODH with very little CO produced, whose mechanistic underpinnings are of utmost interest. The statistics over a swarm of adsorption and scattering trajectories where O 2 hits various sites on the cluster at reaction temperature shows that the O 2 binding does not only follow the minimal energy paths. O 2 also rarely integrates into the cluster in a single step and instead first binds to a single Cu atom via either an η 1 -O 2 or an η 2 -O 2 mode. Surprisingly, this step often has a higher barrier than the subsequent O 2 integration and dissociation, which in turn take multiple steps and complete the oxidation process. Dynamic trajectories starting from the key transition state of integration of the adsorbed O 2 can also lead to different intermediate structures during or right after the dissociation, due to the energy released from the transition state and the thermal intracluster effects. From these activated O 2 chemisorbed structures, O 2 dissociation occurs with moderate barriers (~0.5 eV), producing multiple final oxidized Cu 4 O 4 states. Hence, a diversity of reaction profiles for the attack of supported Cu cluster by O 2 emerges due to the dynamic effects, with implications for mechanisms, kinetic models, and catalyst design principles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Effect of Strength of Soluble and Solid Acid Catalysts on Selectivity in Aldol Reactions

Aldol reactions can follow the classical condensation path and produce an α,β-unsaturated carbonyl compound and water, however in some cases, aldol chemistry may be steered towards a fission that gives an olefin and a carboxylic acid. This investigation examines how the strength of Brønsted acid sites—both in homogeneous and heterogeneous catalysis—controls these two pathways and their kinetics. The cross-aldol reaction between benzaldehyde and 3-pentanone served as test case. Batch reactions, conducted in toluene as solvent at a temperature of 140 °C under autogenous pressure, were analyzed by GC and in situ ATR-FTIR spectroscopy to determine product distributions and rate constants for condensation and fission pathways. A series of soluble acids including a family of sulfonic acids mostly favored the condensation pathway, with formic acid as the weakest in the series by its pKa being inactive for aldol chemistry. Significant amounts of fission products were rare except for the known selectivity of phosphoric acid, and the circumstances were difficult to delineate. For the sulfonic acid family, the logarithm of the first-order condensation rate constants scaled only roughly with pKa (water) values, whereas a good correlation was obtained with calculated deprotonation Gibbs energies in toluene. A series of H-forms of isomorphously substituted beta zeolites, HESiBEA with E = Al, Ga, Fe, or B, favored the fission pathway. Site density and site strength were characterized by calorimetric measurements of the heats of adsorption of isopropylamine, which decreased in the order Al > Ga, Fe > B. The logarithm of the site-normalized first-order fission rate constants scaled roughly with the heats of adsorption and correlated excellently with reported deprotonation energies. In conclusion, acid strength mainly affects activity and can be seen as a pre-requisite for either aldol condensation or fission chemistry, whereas additional, yet to be full clarified catalyst properties and reaction conditions are required to steer aldol chemistry towards fission selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Transition between protein-like and polymer-like dynamic behavior: Internal friction in unfolded apomyoglobin depends on denaturing conditions

Equilibrium dynamics of different folding intermediates and denatured states is strongly connected to the exploration of the conformational space on the nanosecond time scale and might have implications in understanding protein folding. For the first time, the same protein system apomyoglobin has been investigated using neutron spin-echo spectroscopy in different states: native-like, partially folded (molten globule) and completely unfolded, following two different unfolding paths: using acid or guanidinium chloride (GdmCl). While the internal dynamics of the native-like state can be understood using normal mode analysis based on high resolution structural information of myoglobin, for the unfolded and even for the molten globule states, models from polymer science are employed. The Zimm model accurately describes the slowly-relaxing, expanded GdmCl-denaturated state, ignoring the individuality of the different aminoacid side chain. The dynamics of the acid unfolded and molten globule state are similar in the framework of the Zimm model with internal friction, where the chains still interact and hinder each other: the first Zimm relaxation time is as large as the internal friction time. Transient formation of secondary structure elements in the acid unfolded and presence of α-helices in the molten globule state lead to internal friction to a similar extent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Foreword Special issue on the Kilopower Project, Kilowatt Reactor Using Stirling TechnologY (KRUSTY) Test

This special issue of Nuclear Technology contains full-length, peer-reviewed papers describing the design work leading up to and the results of the Kilowatt Reactor Using Stirling TechnologY (KRUSTY) test. KRUSTY was the centerpiece of the National Aeronautics and Space Administration (NASA) Kilopower Project to design, build, and test a space nuclear reactor. This test was the first such test since the end of the Space Nuclear Auxiliary Power (SNAP) project at the end of the 1960s. In this issue, the introduction paper presents the goals of the Kilopower Project and the potential missions this reactor concept could serve in NASA. Kilopower was intended to serve both human exploration needs on planetary surfaces as well as science needs for deep-space exploration. The design work for the experiment by Poston and the power conversion development by Gibson present the pre-work required to perform the eventual KRUSTY test. A paper on regulatory analysis follows, to show the path used to gain approval of the proposed experiment. Then, the early zero-power critical experiments are presented by Sanchez and Grove. These experiments were essential data used to enhance model predictions prior to the high-temperature test. Next, Poston presents the three experiments (warm criticals) that increase the temperature in an incremental fashion prior to the final experiment. These experiments were used to achieve final regulatory approval of the final high-temperature experiment. The last paper by Poston presents the results of the steady-state and transient testing of the reactor at full power and at the design temperature. These results show that the reactor design and as-built experiment met all of the requirements that NASA had developed for the system. Any experiment of this magnitude was accomplished only because of the hard work and dedication of a large number of people at multiple institutions, including the NASA Glenn Research Center, NASA Marshall Space Flight Center, Y-12 National Security Site, Los Alamos National Laboratory, and the Nevada National Security Site prime contractor (formerly National Security Technologies and now the Mission Support and Test Services). The project was jointly funded by the Space Technology Mission Directorate at NASA and the Criticality Safety Program at the National Nuclear Security Administration (NNSA). A special thanks to Jerry McKamy and Angela Chambers at the NNSA and Lee Mason and Don Palac at NASA for their support and guidance. For the authors and multitude of staff that performed this work, the passion for space nuclear reactors was the key to making this experiment a reality.

99 GENERAL AND MISCELLANEOUS↗

Graphene-based analog of single-slit electron diffraction

In this study, we report on the experimental demonstration of single-slit diffraction exhibited by electrons propagating in encapsulated graphene with an effective de Broglie wavelength corresponding to their attributes as massless Dirac fermions. Nanometer-scale device designs were implemented to fabricate a single-slit followed by five detector paths. Predictive calculations were also utilized to readily understand the observations reported. These calculations required the modeling of wave propagation in ideal case scenarios of the reported device designs to more accurately describe the observed single-slit phenomenon. This experiment was performed at room temperature and 190 K, where data from the latter highlighted the exaggerated asymmetry between electrons and holes, recently ascribed to slightly different Fermi velocities near the K point. This observation and device concept may be used for building diffraction switches with versatile applicability.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Leveraging Multiple Connected Traffic Light Signals in an Energy-Efficient Speed Planner

Connecting automated vehicles to traffic lights can lead to significant energy savings by enabling them to pass through intersections in an energy-efficient way without unnecessary stops. A cellular-based communication system connecting multiple traffic lights can help realize the full potential of energy-efficient driving at intersections. Thus, we propose a hierarchical speed planner that can leverage information from multiple connected traffic lights. The proposed speed planner consists of two modules: a green window selector and a reference trajectory generator. The green window selector, based on Dijkstra’s algorithm, finds a series of "green windows" for connected traffic lights that builds an energy-optimal path for vehicles to follow. The reference trajectory generator finds optimal entering times, based on the selected green window at each intersection, and then computes reference trajectories. Deriving and using analytical optimal entering speeds as a function of entering times allows us to guarantee the computational simplicity suitable for real-time implementation. We also demonstrate how to balance energy and traffic flow perspectives in the reference trajectory generator. Lastly, a high-fidelity simulation framework is used to evaluate the proposed speed planner and quantify the extent to which it can save energy in various real-world urban route scenarios.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Commissioning, Performance, and Effect of the Quench Current-Boosting Device on a Dedicated Superconducting Magnet

Superconducting magnet training is one of the accelerator related issues attracting attention due to significant operational costs and time budget associated to it. It is especially worrisome that magnets based on the “next-generation” Nb 3 Sn technology are affected by long training. While various efforts are underway to better understand and resolve the problem a parallel path could also be investigated, a path bypassing the issue. Following the concept of fast induced over-current during magnet powering, FNAL has developed an upgradable capacitor-based device to discharge through a superconducting magnet at quench detection or operator chosen time. The 0.4 F/1 kV device has been tested on a 1-m-long dipole-coil in a “mirror” magnet configuration and conclusive results on magnet training elimination have been observed. Here in this paper we discuss the main characteristics of the device, compare simulated response and actual performance, elaborate on test drivers and outcomes. Next steps and perspectives for future use are debated.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

SmartFlower Renewable Energy Program (Final Technical Report)

The SmartFlower Renewable Energy Programming project brings renewable energy education to K-12 youth in the region. The motivation of the project was to pair an educational curriculum with Girl Scouts of the Colonial Coast’s newly acquired SmartFlower. A SmartFlower is a solar energy device shaped like a flower in which each petal is a solar panel. The ‘stem’ of the SmartFlower rotates throughout the day, so the petal panels follow the sun’s path and maximize sunlight absorption. The goal of the project was to create an educational curriculum for K-12 youth that centered the SmartFlower and other renewable energy related topics. The Girl Scouts of Colonial Coast team created two educational curriculums; each designed for a specific age group (K-5 and 6 th -12 th grade). Both curriculums walk participants through hands-on activities about the sun, renewable energy, and sustainability. The project adds to educational opportunities in the region and for Girl Scouts. As renewable energy becomes more prevalent and essential, youth must be informed on its’ mechanics and application. The project provides an age-appropriate educational tool that welcomes youth to visit the SmartFlower, understand its larger purpose, and consider the importance of renewable energy. The project was achieved on a modest budget of $16,672 and its sustainability beyond the project period has low to no cost for participants. The curriculum is free and accessible on our website and can be used as an evergreen educational tool. The SmartFlower Renewable Energy Programming project benefits the public as it provides a free, easily accessible education tool to children, families, caregivers, and local educators that is scientifically based and relevant to our energy landscape.

14 SOLAR ENERGY↗

Advancing the quantification of aerosol-cloud interactions with the CALIPSO-CloudSat-Aqua/MODIS record

Aerosol-cloud-precipitation interactions are assessed over the non-polar ocean using more than 11 years of combined Aqua-MODIS, CALIPSO-CALIOP, and CloudSat products. The analysis first shows the benefit of incorporating vertically resolved aerosol extinction coefficient (σext) in aerosol-cloud interactions (ACI) assessments, demonstrating that: σext vertically collocated with the cloud layer () correlates best with cloud droplet number concentration (Nd), column-integrated aerosol optical depth (AOD) cannot explain the Nd variability in the extratropics, and the S-shape of the AOD-Nd relationship reported in previous studies is not replicated when using instead of AOD, with a Nd- linearity more consistent with in-situ studies over the ocean. ACI metric, estimated as the log-scale regression between CALIOP and MODIS Nd reveals that the eastern Pacific is the region with the strongest ACI, followed by the Southern Ocean. The susceptibility of clouds to changes in their liquid water path (LWP) and frequency of precipitation followed a 2-step calculation by combining the Nd- regression (ACI) with the regression between these macrophysical variables and Nd. LWP susceptibility is negative (LWP decreases with aerosol loading) and statistically significant over the eastern Pacific, eastern Atlantic, and extratropics. In contrast, vast areas of the tropical and subtropical ocean feature negligible changes in LWP with aerosol. Precipitation frequency susceptibility is negative, but the values are only significant over the coastal eastern Pacific and Atlantic. The findings suggest that previous modeling assessments relying on AOD may need to be revisited by taking advantage of the synergy between passive and active sensors.

Li, Zhujun↗

Adaptive Variational Quantum Imaginary Time Evolution Approach for Ground State Preparation

Abstract An adaptive variational quantum imaginary time evolution (AVQITE) approach is introduced that yields efficient representations of ground states for interacting Hamiltonians on near‐term quantum computers. It is based on McLachlan's variational principle applied to imaginary time evolution of variational wave functions. The variational parameters evolve deterministically according to equations of motions that minimize the difference to the exact imaginary time evolution, which is quantified by the McLachlan distance. Rather than working with a fixed variational ansatz, where the McLachlan distance is constrained by the quality of the ansatz, the AVQITE method iteratively expands the ansatz along the dynamical path to keep the McLachlan distance below a chosen threshold. This ensures the state is able to follow the quantum imaginary time evolution path in the system Hilbert space rather than in a restricted variational manifold set by a predefined fixed ansatz. AVQITE is used to prepare ground states of H 4 , H 2 O, and BeH 2 molecules, where it yields compact variational ansätze and ground state energies within chemical accuracy. Polynomial scaling of circuit depth with system size is shown through a set of AVQITE calculations of quantum spin models. Finally, quantum Lanczos calculations are demonstrated alongside AVQITE without additional quantum resource costs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effect of realistic routing on the social burden metric

The distance people travel to reach critical services is a key input to the Social Burden metric used by Sandia’s Resilient Node Cluster Analysis Tool (ReNCAT) in the optimization’s objective function. By default, ReNCAT utilizes Euclidian distances between population blocks and critical facilities when calculating Social Burden. However, these straight-line distances do not reflect how most residents or goods would travel throughout the area. As distance is a vital input to the burden calculation, a more realistic distance calculation will yield more realistic burden values. This work uses real road networks and calculates the shortest distance path between population centers and critical facilities using a standard graph theory approach. These realistic route distances are then used to compute Social Burden for four areas of study. It was found that distances using real road routes are generally, but not always, longer than the Euclidean distance. The increased length increases the final Social Burden metric, however, the overall burden percent change ranged between 17% and 52%, which means the impact of realistic routes relies heavily upon the area’s road topology. It was found that rural locations within an area may have larger burden increases than urban areas as more dense road networks allow routes to more closely follow a straight-line path. Additionally, using the most straight forward routing algorithms requires high computational effort for areas with large road networks. While it is believed this process can be made more performant, that task is beyond this scope of work.

99 GENERAL AND MISCELLANEOUS↗

Pathways to IEC Standards for Heliostat Design Qualification and Site Acceptance in Central Receiver CSP Applications

This paper surveys the existing landscape of standards relevant to heliostats, identifies their gaps, and proposes a path forward to a comprehensive set of heliostat guidelines, technical specifications, and standards under the framework of International Electrotechnical Commission (IEC) TC 117. Gaps in existing guidelines and standards are surveyed using a three-tiered taxonomy: component-level, heliostat-level, and field-level. At each level, the gap analysis is followed by a proposal for a coordinated path forward on the development of standards. At the component level, advances in the understanding of wind loading should inform a technical specification for drives and structures. Reflectors require consolidation of measurement guidelines into existing standards documents. Communications & controls require technical standards to inform their selection and secure implementation. At the heliostat level, IEC 62817 (solar trackers) adequately characterizes drive systems, structures, and electronics, but requires adaptation to heliostats' use patterns, operating modes, and expected life cycles. IEC 62817 does not address heliostat beam quality and pointing accuracy, but the process for determining both is elaborated in the SolarPACES Guideline for Heliostat Performance Testing. This SolarPACES document requires two main modifications: adaptation to IEC language and inclusion of testing after heliostats which have undergone accelerated weathering and mechanical cycling (to understand performance degradation). At the field level, IEC 62862-4-2 addresses the function and control of heliostat fields but does not cover the statistically rigorous testing of heliostat groups, or field performance factors like security and soiling. The addition of documents under IEC-62862-4 is proposed to address this gap.

beam↗

Reaction Evolution Flow Chart - The Critical Path to DDT [Slides]

Purpose (and limitations): The following flow-chart identifies and organizes a generalized, and simplified, sequence of necessary conditions for accidental ignition and reaction growth in a consolidated, polymer-bonded explosive (PBX) charge that has been insulted. A ‘yes’ answer to each question will lead down the critical path and produce violent, explosive reactions, up to and possibly including transition to detonation. Alternatively, any ‘no’ answer will serve as an off-ramp from the path resulting in less violent responses. It is important to note that this flow-chart is a high-level tool to flag potential operational vulnerabilities, but lacks the details needed to stand alone as a sole-source for risk determination. Each question represents a significant area of study and, therefore, the flow chart is intended to be supplemented by subject matter expert elicitations.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Adsorption and Surface Diffusion of Metals on α-Al2O3 for Advanced Manufacturing Applications

Abstract The adsorption and diffusion of Mo and Nb adatoms on the $$\alpha$$ α -Al 2 O 3 (0001) surface were explored using density functional theory-based methods. Adsorption energies of Mo and Nb adatoms at minima sites on the surface were determined. Mo and Nb adatoms prefer to adsorb to the same locations on the surface, and larger adsorption energies calculated for Nb compared to Mo indicate that Nb adatom-surface interactions are stronger than Mo. Using minima adsorption sites as initial and final locations for surface diffusion, energy barriers for diffusion were calculated using the nudged elastic band method. Overall, Mo and Nb follow roughly the same diffusion paths. The diffusion pre-factors for Mo and Nb are similar; however, Mo diffusion has a lower energy barrier and thus a larger diffusion coefficient compared with Nb. These results provide insight into the role of surface diffusion of Mo and Nb adatoms during advanced manufacturing processes.

Biaggne, Austin (ORCID:0000000328074960)↗

An optimization-based approach to tailor the mechanical response of soft metamaterials undergoing rate-dependent instabilities

An optimization-based design framework is proposed to tune the response of soft metamaterials involving both geometric instabilities and nonlinear viscoelastic material behavior. Designing the response of soft metamaterials to harness instabilities and undergo large, tailored configuration changes will enable advancements in soft robotics, shock and vibration mitigation, and flexible electronics. In line with the metamaterial concept, the response of these materials is governed to a large extent by the geometric and topological makeup of their small-scale features. However, the link between structure and response is less intuitive for soft metamaterials due to their reliance upon highly nonlinear responses triggered by geometric instabilities. This is further complicated by the effects of viscoelastic relaxation, which recent studies have shown to alter the emergence of instabilities in non-intuitive ways. Here, these effects are accounted for in our framework to achieve various design objectives, including tailored force–displacement response and maximized energy absorption from both geometric and material effects. To fully automate this process, it is essential to have a completely robust equation solver for forward problems involving instabilities and viscoelastic relaxation. We achieve this by casting the search for stable mechanical equilibrium — i.e. the forward problem — as a minimization problem and utilize a trust region algorithm to robustly handle instabilities and follow energetically-favorable equilibrium paths through critical points.

97 MATHEMATICS AND COMPUTING↗

Development of thin-gap GEM- μ RWELL hybrid detectors

Micro Pattern Gaseous Detectors (MPGDs) are used for tracking in High Energy Physics and Nuclear Physics because of their large area, excellent spatial resolution capabilities and low cost. However, for high energy charged particles impacting at a large angle with respect to the axis perpendicular to detector plane, the spatial resolution degrades significantly because of the long trail of ionization charges produced in clusters all along the track in the drift region of the detector. The long ionization charge trail results in registering hits from large number of strips in the readout plane which makes it challenging to precisely reconstruct the particle’s position using simple center of gravity algorithm. As a result, the larger the drift gap, the more severe the deterioration of spatial resolution for inclined tracks. For the same reason, the position resolution is also severely degraded in a large magnetic field, where the Lorentz E x B effect causes the ionization charges to follow a curved and longer path in the detector gas volume. In this paper, we report on the development of thin-gap MPGDs as a way to maintain excellent spatial resolution capabilities of MPGD detectors over a wide angular range of incoming particles. In a thin-gap MPGD, the thickness of the gas volume in the drift region is reduced from typically 3 mm to 1 mm or less. We present preliminary test beam results demonstrating the improvement in spatial resolution from 400 m with a standard 3 mm gap μ RWELL prototype to ~140 μ m with a double amplification GEM- μ RWELL thin-gap hybrid detector. Here, we also discuss the impact of a thin-gap drift volume on other aspects of the performance of MPGD technologies such as the efficiency and detector stability.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Ab Initio Direct Dynamics

The reactivity and dynamics of molecular systems can be explored computationally by classical trajectory calculations. The traditional approach involves fitting a functional form of a potential energy surface (PES) to the energies from a large number of electronic structure calculations and then integrating numerous trajectories on this fitted PES to model the molecular dynamics. The ever-decreasing cost of computing and continuing advances in computational chemistry software have made it possible to use electronic structure calculations directly in molecular dynamics simulations without first having to construct a fitted PES. In this “on-the-fly” approach, every time the energy and its derivatives are needed for the integration of the equations of motion, they are obtained directly from quantum chemical calculations. This approach started to become practical in the mid-1990s as a result of increased availability of inexpensive computer resources and improved computational chemistry software. The application of direct dynamics calculations has grown rapidly over the last 25 years and would require a lengthy review article. The present Account is limited to some of our contributions to methods development and various applications. To improve the efficiency of direct dynamics calculations, we developed a Hessian-based predictor-corrector algorithm for integrating classical trajectories. Hessian updating made this even more efficient. Furthermore, this approach was also used to improve algorithms for following the steepest descent reaction paths. For larger molecular systems, we developed an extended Lagrangian approach in which the electronic structure is propagated along with the molecular structure. Strong field chemistry is a rapidly growing area, and to improve the accuracy of molecular dynamics in intense laser fields, we included the time-varying electric field in a novel predictor-corrector trajectory integration algorithm. Since intense laser fields can excite and ionize molecules, we extended our studies to include electron dynamics. Specifically, we developed code for time-dependent configuration interaction electron dynamics to simulate strong field ionization by intense laser pulses. Our initial application of ab initio direct dynamics in 1994 was to CH 2 O → H 2 + CO; the calculated vibrational distributions in the products were in very good agreement with experiment. In the intervening years, we have used direct dynamics to explore energy partitioning in various dissociation reactions, unimolecular dissociations yielding three fragments, reactions with branching after the transition state, nonstatistical dynamics of chemically activated molecules, dynamics of molecular fragmentation by intense infrared laser pulses, selective activation of specific dissociation channels by aligned intense infrared laser fields, angular dependence of strong field ionization, and simulation of sequential double ionization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗