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383 records · Page 22

High-Performance Semiempirical Excited-State Molecular Dynamics Powered by Graphics Processing Units

Here, this Letter introduces excited-state molecular dynamics in PYSEQM, a GPU-accelerated semiempirical quantum chemistry engine implemented in PyTorch. The new module enables Born–Oppenheimer molecular dynamics (BOMD) using configuration-interaction singles and random phase approximation for excited states, allowing long trajectories and large statistical ensembles to be simulated efficiently on a single GPU. We also implement an extended Lagrangian excited-state BOMD (XL-ESMD) scheme that propagates auxiliary electronic variables, enabling relaxed ground and excited-state convergence thresholds without compromising energy conservation. The excited-state BOMD implementation scales smoothly from small chromophores to a nearly 900-atom dendrimer (taking 6.5 s per MD step). PYSEQM also supports batched execution, allowing many geometries or trajectories to be evaluated in a single GPU launch, substantially increasing throughput and making ensemble-based protocols routine. As a demonstration, we compute absorption, emission, and infrared spectra from trajectories propagated on the ground and first excited states. The XL-ESMD scheme yields identical spectra at significantly lower computational cost, establishing the role of extended Lagrangian based dynamics for efficient excited-state BOMD simulations. Beyond raw performance, PYSEQM’s PyTorch foundation provides automatic differentiation for forces, efficient GPU batching, and seamless interfacing with machine learning models. These capabilities position PYSEQM as a practical platform for machine learning-augmented excited-state dynamics and lay the foundation for future data-driven nonadiabatic excited-state dynamics modeling of ultrafast spectroscopic probes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-Consistent Relativistic Electron Scattering using the Sherlock Scattering Model for X-ray Diagnostics

We present on a new, self-consistent, arbitrary-temperature Romberg integration scheme for modeling electron scattering in materials in a LANL Lagrangian Shock Hydro (LSH) code. Electron beam-target interactions are fundamental to a wide range of scientific and technological applications. When high-energy electron beams hit their target, they may scatter, deposit energy, or ionize the source. These processes govern the behavior and outcomes in nanotechnology manufacturing, electron microscopy, and modern X-ray diagnostics. Simulating these interactions is essential for interpreting experimental results, predicting material responses, and designing efficient tools and experiments. At Los Alamos, this is done using a LSH code, which is a multi-dimension, multi-material, massively parallel, multi-physics code used to simulate applications from asteroid impacts to electron beam interactions. By effectively and efficiently modeling the way that electrons scatter from the beam we can bolster these simulations and more accurately predict experimental outcomes. The model currently implemented in the LSH of interest is based on work by Papp and does not self-consistently preserve momentum in the slightly relativistic regime; here we adopt a model proposed by Braams and Karney and implement a Romberg integration scheme to compute the diffusion tensor. In this paper we will provide background on the Braams-Karney diffusion tensor as well as the Romberg integration scheme we employed to numerically solve for it. We will show that our integration scheme is accurate in solving for the set of scalar potentials used to re-express the diffusion tensor in differential form, and in solving for the diffusion coefficients in the larger LSH code. By using this diffusion tensor rather than the existing Papp one, and numerically integrating it with a Romberg method, we produce much more accurate, self-consistent results.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Finite deformation implementation of a mixed-mode single-integral type cohesive zone with reorienting surfaces of separation

To model material ductile failure and crack propagation, cohesive zone elements can be embedded along potential fracture paths in a finite element simulation. When damage criteria are met, elements in the mesh decohere, simulating the formation and propagation of a crack. In this paper, we present a novel computational algorithm based on finite deformation theory, essential to modeling crack initiation and growth in solids undergoing large deformations. This new algorithm was formulated within a Lagrangian frame of reference to extend previous cohesive zone algorithms to include modeling crack growth in finite deformation contexts. The local coordinate system, necessary for defining an embedded cohesive zone, is constructed based upon the current configuration and is updated within the nonlinear iteration process, thereby resulting in the convergence of the solution for a growing crack in a large deformation quasi-static setting. The model’s accuracy was demonstrated by comparing finite element model simulation results with the analytic case of a constant surface separation, as shown in the verification examples. The power and efficacy of the algorithm to capture large deformations during crack growth were then demonstrated with a double cantilever beam example case. It indicates that the model can be applied to a variety of physical circumstances for predicting crack initiation and growth with delamination and fracture.

42 ENGINEERING↗

Dividing the Concentrator Target From the Genesis Mission

The Genesis spacecraft, launched in 2001, traveled to a Lagrangian point between the Earth and Sun to collect particles from the solar wind and return them to Earth. However, during the return of the spacecraft in 2004, the parachute failed to open during descent, and the Genesis spacecraft crashed into the Utah desert. Many of the solar wind collectors were broken into smaller pieces, and the field team rapidly collected the capsule and collector pieces for later assessment. On each of the next few days, the team discovered that various collectors had survived intact, including three of four concentrator targets. Within a month, the team had imaged more than 10,000 fragments and packed them for transport to the Astromaterials Acquisition and Curation Office within the ARES Directorate at JSC. Currently, the Genesis samples are curated along with the other extraterrestrial sample collections within ARES. Although they were broken and dirty, the Genesis solar wind collectors still offered the science community the opportunity to better understand our Sun and the solar system as a whole. One of the more highly prized concentrator collectors survived the crash almost completely intact. The Genesis Concentrator was designed to concentrate the solar wind by a factor of at least 20 so that solar oxygen and nitrogen isotopes could be measured. One of these materials was the Diamond-on-Silicon (DoS) concentrator target. Unfortunately, the DoS concentrator broke on impact. Nevertheless, the scientific value of the DoS concentrator target was high. The Genesis Allocation Committee received a request for approximately 1 cm(sup 2) of the DoS specimen taken near the focal point of the concentrator for the analysis of solar wind nitrogen isotopes. The largest fragment, Genesis sample 60000, was designated for this allocation and needed to be precisely cut. The requirement was to subdivide the designated sample in a manner that prevented contamination of the sample and minimized the risk of losing or breaking the precious requested sample fragment. The Genesis curator determined that the use of laser scribing techniques to "cut" a precise line and subsequently cleave the sample (in a controlled break of the sample along that line) was the best method for accomplishing the sample subdivision. However, there were risks, including excess heating of the sample, that could cause some of the implanted solar wind to be lost via thermal diffusion. Accidentally breaking the sample during the handling and cleaving process was an additional risk. Early in fiscal year 2013, to address this delicate, complicated task, the ARES Directorate assembled its top scientists to develop a cutting plan that would ensure success when applied to the actual concentrator target wafer; i.e., to produce an approximately 1 cm(sup 2) piece from the requested area of the wafer. The team, subsequently referred to as the JSC Genesis Tiger Team, spent months researching and testing parameters and techniques related to scribing, cleaving, transporting, handling, and holding (i.e., mounting) the specimen. The investigation required considerable "thinking outside the box," and many, many trials using nonflight wafer analogs. After all preliminary testing, the following method was adopted as the final cutting plan. It was used in two final end-to-end practice runs before being used on the actual flight target wafer. The wafer was oriented on the laser cutting stage with the 100 and 010 directions of the wafer parallel to the corresponding X and Y directions of the cutting stage. The laser was programed to scribe 31 lines of the appropriate length along the Y stage direction. The programed scribe lines were separated by 5 micron in the X direction. The laser parameters were set as follows: (1) The laser power was 0.5 watts; (2) each line consisted of 50 passes, with the Z position being advanced 5 micron per pass; and (3) 30 s would elapse before the next line was scribed to allow for wafer cool down from any possible heating via the laser. The ablated material that "stuck" in the "scribe-cut" was removed from the "cut" using an ultrasonic micro-tool. After all the ablated silicon was removed from the wafer, the wafer was repositioned in exactly the same orientation on the laser stage. The laser was focused using the bottom of the wafer channel, and the 31-line scribing pattern described above was reprogrammed using the Z position of the groove bottom as the starting Z value instead of the top wafer surface, which was used previously. Upon completion of the second set of scribes, the ultrasonic micro-tool was again used to clean out the cut. The wafer was remounted on the stage in exactly the same orientation as before. The laser was again focused on the bottom of the groove. This time, however, the laser was.programed to scribe only one line down the exact center of the channel. The final scribe line consisted of 100 passes with a Z advance of 5 micron per pass and with the laser power set at 0.5 watts. As mentioned above, the final cutting plan was practiced in two end-to-end trials using non-flight, triangular-shaped silicon wafers similar in size and orientation to the actual DOS 60000 target sample. The actual scribing of the triangular-shaped wafers required scribing two lines and cleaving (i.e. scribe-cleave, then scribe-cleave) to obtain the piece requested for allocation. Early in December 2012, after many months of experiments and practicing and perfecting the techniques and procedures, the team successfully subdivided the Genesis DoS 60000 target sample, one of the most scientifically important samples from the Genesis mission (figure 2). On December 17, 2012, the allocated piece of concentrator target sample was delivered to the requesting principal investigator.The cutting plan developed for the subdivision of this sample will be used as the model for subdividing future requested Genesis flight wafers (appropriately modified for different wafer types).

Lauer, H. V., Jr.↗

Shock-Layer Radiation Insights Available Through Flowfield Property Binning

This paper introduces a method for assessing similarity between available shock-layer radiation measurements and the radiative heating to a vehicle of interest. This method will be referred to as the flowfield property binning (FPB) approach. The challenge in developing this approach is that radiometer measurements from a surface normal line of sight, observed radiation measurements of the entire shock-layer from a distance, or measured shock-tube nonequilibrium profiles are notably different geometrically than the radiative flux to a vehicle surface. Therefore, the relative contributions of various regions of the shock-layer to the measurement, and how these relative contributions compare with the radiative heating to a vehicle of interest, are unclear. By tracking the radiation contribution from each flowfield location, and then grouping this contribution based on two local flowfield properties, these geometric differences are removed. This provide a two dimensional group, or bin, distribution that represents the radiation environment in the same format for various types of radiation simulations, such as observed radiation or radiative flux to a vehicle surface. In the limits of optically-thin radiation transport and thermochemical equilibrium flow, the choice of pressure and temperature as the binning flowfield properties is shown to provide a bin distribution that uniquely defines the radiation simulation. This concept is found to be sufficient for establishing similarity between two cases even when the optically-thin radiation transport and thermochemical equilibrium assumptions are not satisfied. A simple metric of comparison between bin distributions from different cases is provided by the histogram intersection algorithm. This algorithm results in a histogram intersection factor (H) between 0 and 1, which represents the fraction of the radiation that is similar between the two cases. Therefore, if H evaluated between bin distributions for two completely different radiation problems is near 1, then they represent essentially the same radiation problem. This means that they depend on the same weighting of various radiation modeling parameters evaluated at the same pressure and temperature. If one of these cases agrees well with a radiation measurement, then the matching bin distributions provide justification for applying this experimental validation to the other case. Even for H values as low as 0.2, the measurement case could be considered relevant if there are no other useful measurements. This approach allows observed radiation measurements to directly inform radiative heating simulations, which allows NASA’s past and future investments in observed radiation measurements to directly inform the radiative heating uncertainty or margins for future vehicle design. This FPB approach is also used to determine shock-tube conditions for informing backshell radiative heating simulations, where the normal shock velocity and Lagrangian time from the shock is used for the binning variables instead of pressure and temperature.

Shock Layer Radiation↗