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At least 847 records · Page 47

Range-separated thermal hybrid exchange-correlation density functional for accurate band-gap calculations of warm dense matter

Here, in this study, we present a range-separated thermal hybrid exchange-correlation (XC) functional, termed RS-KDT0, which provides highly accurate band-gap predictions at elevated temperature while reducing the computational cost relative to thermal global hybrid functionals. At zero temperature, RS-KDT0 recovers the widely used ground-state range-separated hybrid functional HSE06. To assess its performance across temperature regimes, we conducted static calculations of electronic pressure, band gaps, and band structures. RS-KDT0 exhibits the same level of accuracy as HSE06 in the low-temperature regime and demonstrates improved agreement with finite-temperature GW calculations at elevated temperatures when compared to other thermal XC functionals such as the generalized gradient approximation (GGA)-level KDT16 and the global hybrid KDT0.

density functional theory↗

Density functional based methods for light harvesting molecules

The goal of the proposal was to computationally study the photoinduced charge transfer excited states of organic molecules. The systems of interest are the large organic supramolecules that have potential for photovoltaic applications. The simulation of the charge transfer excited states in large supramolecular assemblies require quantum mechanical methods that can be applied to systems with hundreds of atoms. Through this project we have implemented a perturbative delta-self-consistent field method that can easily describe the charge transfer excited states with regular density functionals without range separation. The cost of the calculations of an excited state is similar to that of the ground state. The method also allows for calculation of the energy gradients of the excited state. The developed method was applied to study a number of different supramolecular systems containing hundreds of atoms with excellent agreement with experiment. The absorption characteristics and the influence of density functional approximations were also examined. These led to several studies on the variety of organic electron donor and acceptor molecules. Apart from these developments through this project we also improved the code capabilities by implementing new meta-GGA functionals. This was a major step since the code is purely density functional and earlier the functional capabilities were limited only to generalized gradient approximations. A total of 23 peer-reviewed publications in top chemical physics journals resulted from this grant.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-Resolved Measurements Of Laser Far-Field Patterns

Computer-controlled scanning photometric instrumentation system measures intensity pattern in far field of pulsed laser as function of time during each pulse (provided that pulse is at least 1 ns long). Such measurements important in studying dynamics of laser operation: they reveal such previously unobservable phenomena as oscillations of undesired spatial modes of radiation pattern during pulse, steering of beam during pulse, and instability of intensity of laser beam. Principal advantages of system are its relatively low cost and its ability to function under normal lighting conditions without incurring damage.

Forrest, Kathrine↗

GW with hybrid functionals for large molecular systems

A low-cost approach for stochastically sampling static exchange during time-dependent Hartree–Fock-type propagation is presented. This enables the use of an excellent hybrid density functional theory (DFT) starting point for stochastic GW quasiparticle energy calculations. Generalized Kohn–Sham molecular orbitals and energies, rather than those of a local-DFT calculation, are used for building the Green function and effective Coulomb interaction. The use of an optimally tuned hybrid diminishes the starting point dependency in one-shot stochastic GW, effectively avoiding the need for self-consistent GW iterations.

Chemistry↗

A framework and tool for designing cost-effective, resilient, and circular net-zero supply chains under uncertainty with an application to multilayer plastic films

While 55% of Fortune 500 companies have committed to achieving net-zero emissions and/or zero-waste operations by 2035, only 2% are currently on track, revealing a critical gap between ambition and action. Designing supply chains that reduce both emissions and waste is a complex non-intuitive, multi-objective challenge, compounded by the high costs of new technologies and the need for resilient, profitable solutions. This paper aims to address this challenge by presenting a generic framework and multi-objective optimization formulation for designing cost-effective, circular, and resilient supply chains under uncertainty, implemented through a user-friendly decision-support tool with intuitive data visualization capabilities, enabling communication of results to both technical and non-technical stakeholders. We demonstrate the application of this framework in the context of multilayer plastic films (barrier films), which are widely used in food packaging and composite materials. The model quantifies trade-offs across three objectives: minimizing global warming potential, maximizing circularity, and minimizing cost. A key contribution of this work is the explicit modeling of technological resilience, the ability of supply chains to maintain function under disruption. In the cost-minimization case, the resilience constraint makes the design approximately three times more expensive in the short-term metric, but shifts the system from relying on a single recovery pathway to a portfolio of four recovery pathways, improving the robustness of the optimization solution under uncertainty. Lastly, we introduce TranZero, a decision-support tool that integrates material flow analysis, hotspot identification, and optimization-based scenario planning to support net-zero and circularity decisions.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Bismuth-Functionalized Silica Aerogels for Iodine Capture

The U.S. Department of Energy is looking into alternative sorbents for the removal of radioiodine from off-gas streams in a used nuclear fuel reprocessing plant. One class of sorbents considered are bismuth-functionalized silica aerogels which offer an efficient capture of iodine from off-gas streams and are environmentally friendly and lower cost when compared to silver-functionalized sorbents. Two types of bismuth-functionalized silica aerogels were successfully manufactured using a hierarchical synthesis approach:1) The Bi 3+ -aerogel with bismuth oxide nitrate hydroxide hydrate particles and 2) Bi-aerogel with bismuth metal and bismuth sulfide nanoparticles. Both sorbents exhibited high sorption capacity for iodine. However, presence of particles of different composition, size, and distribution on aerogel support resulted in different iodine loadings. The Bi 3+ -aerogel exhibited sorption capacity of 289 mg/g. In contrast, Bi-aerogel exhibited more that 20% higher sorption capacity. The heat-treatment of Bi 3+ -aerogel at 225? under hydrogen atmosphere increased iodine loading capacity to 351 mg/g.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Mechanical properties of zeolite-templated carbons from approximate density functional theory calculations

Zeolite-templated carbon (ZTC) is a unique porous carbonaceous material whose structure is ordered at the nanometre scale, enabling a representative periodic description at the atomistic level. Utilizing an existing, well-defined reference model for ZTCs, a structural library of varying compositions was developed by refinement using density-functional tight-binding (DFTB) potentials parameterized for materials science applications. We first determined the quantum chemical-refined structures of models with CH, CHO, CHON, CHOB, and CHOBN compositions with various degrees of heteroatom substitution. These structural models comprise the characteristic morphological features of highly porous carbon materials, such as open-blade surfaces, edges, saddles, and closed-strut formations, spanning a range of curvatures and characteristic sizes. Second, we carried out alternating compression and expansion of the CHO model unit cell to determine the lowest energy structure as well as to obtain its bulk modulus in order to demonstrate a close connection between macroscopic observations and atomic-scale structures. Further, the agreement between experimental measurements and the computational model is remarkable and demonstrates the power of approximate density functional theory as a cost-effective computational tool with chemical accuracy for the investigation of structure/property relationships in real-world carbon-based solids.

03 NATURAL GAS↗

Design and dispatch optimization of packaged ice storage systems within a connected community

The traditional implementation of cool thermal energy storage (CTES) must be reimagined within the context of a dynamic grid and smart buildings operating as connected communities. As most buildings do not operate central chillers or connect to district cooling loops, this necessitates a broader use of packaged CTES. Our objective is to begin answering the question of how such packaged CTES should be implemented within a connected community. We do so by presenting a simulation–optimization workflow employing building energy modeling software and a mixed-integer linear program to design and dispatch a packaged CTES technology to achieve minimum total annual cost. We demonstrate this methodology on a seven-building case study using current utility rates and find that total annual cooling energy costs can be reduced by 17.8% compared to baseline, after accounting for the cost of storage. We perform three parametric sensitivity studies to evaluate modeling assumptions and obtain the prioritization of storage procurement as a function of annualized life-cycle cost of storage. We find that a community optimization approach provides significantly different results than individual building optimizations and provides greater savings compared to baseline.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

The symmetric quasi-classical model using on-the-fly time-dependent density functional theory within the Tamm–Dancoff approximation

The primary computational challenge when simulating nonadiabatic ab initio molecular dynamics is the unfavourable compute costs of electronic structure calculations with molecular size. Simple electronic structure theories, like time-dependent density functional theory within the Tamm–Dancoff approximation (TDDFT/TDA), alleviate this cost for moderately sized molecular systems simulated on realistic time scales. Although TDDFT/TDA does have some limitations in accuracy, an appealing feature is that, in addition to including electron correlation through the use of a density functional, the cost of calculating analytic nuclear gradients and nonadiabatic coupling vectors is often computationally feasible even for moderately sized basis sets. Here in this work, some of the benefits and limitations of TDDFT/TDA are discussed and analysed with regard to its applicability as a ‘back-end’ electronic structure method for the symmetric quasi-classical Meyer–Miller model (SQC/MM). In order to investigate the benefits and limitations of TDDFT/TDA, SQC/MM is employed to predict and analyse a prototypical example of excited-state hydrogen transfer in gas-phase malonaldehyde. Then, the ring-opening dynamics of selenophene are simulated, which highlight some of the deficiencies of TDDFT/TDA. Additionally, some new algorithms are proposed that speed up the calculation of analytic nuclear gradients and nonadiabatic coupling vectors for a set of excited electronic states.

molecular dynamics↗

A deformation-dependent coupled Lagrangian/semi-Lagrangian meshfree hydromechanical formulation for landslide modeling

Abstract The numerical modelling of natural disasters such as landslides presents several challenges for conventional mesh-based methods such as the finite element method (FEM) due to the presence of numerically challenging phenomena such as severe material deformation and fragmentation. In contrast, meshfree methods such as the reproducing kernel particle method (RKPM) possess unique features conducive to modelling extreme events such as the absence of a structured mesh and the ease of adaptive refinement, among others. While the semi-Lagrangian reproducing kernel (SL-RK) shape functions of RKPM defined in the current configuration have proven to be effective in extreme event modelling, the computational cost for the re-evaluation of the shape functions at every time step is costly. In this work, a deformation-dependent coupling of the Lagrangian reproducing kernel (L-RK) and SL-RK approximations is proposed for the solution of a hydro-mechanical formulation for effective simulations of landslides. The ramp function is constructed based on an equivalent plastic strain as a deformation-dependent transition from L-RK shape functions to SL-RK ones as the deformation progresses. The particular focus of the paper will be on modelling seepage-induced landslides with a mixed $$u$$ u – $$p$$ p formulation to couple the solid and fluid phases. Examples are presented to examine the effectiveness of this coupled Lagrangian/semi-Lagrangian reproducing kernel (L–SL RK) formulation and to highlight its performance in landslide modelling.

Baek, Jonghyuk↗

Elements of designing for cost

During recent history in the United States, government systems development has been performance driven. As a result, systems within a class have experienced exponentially increasing cost over time in fixed year dollars. Moreover, little emphasis has been placed on reducing cost. This paper defines designing for cost and presents several tools which, if used in the engineering process, offer the promise of reducing cost. Although other potential tools exist for designing for cost, this paper focuses on rules of thumb, quality function deployment, Taguchi methods, concurrent engineering, and activity-based costing. Each of these tools has been demonstrated to reduce cost if used within the engineering process.

Dean, Edwin B.↗

Efficient Quantum Gate Discovery with Optimal Control

Optimal control theory provides a framework for numerical discovery of device controls that implement quantum logic gates, but common objective functions used for optimization often assign arbitrarily high costs to otherwise useful controls. We propose a framework for designing objective functions that permit novel gate designs such as echo pulses or locally-equivalent gates. We use numerical simulations to demonstrate the efficacy of the new objective functions by designing microwave-only pulses that act as entangling gates for superconducting transmon architectures. We observe that the proposed objective functions lead to higher fidelity controls in fewer optimization iterations than obtainable by traditional objective functions.

Kairys, Paul↗

Identification of an educational production function for diverse technologies

Production function analysis used to estimate the cost effectiveness of three alternative technologies in higher education: traditional instruction, instructional television, and computer-assisted instruction is presented. Criteria and selection of a functional form are outlined and a general discussion of variable selection and measurement is presented.

Mcclung, R. L.↗

Comparison of Separation Shock for Explosive and Nonexplosive Release Actuators on a Small Spacecraft Panel

Functional shock, safety, overall system costs, and emergence of new technologies, have raised concerns regarding continued use of pyrotechnics on spacecraft. NASA Headquarters-Office of Chief Engineer requested Langley Research Center (LaRC) study pyrotechnic alternatives using non-explosive actuators (NEA's), and LARC participated with Lockheed Martin Missile and Space Co. (LMMSC)-Sunnyvale, CA in objectively evaluating applicability of some NEA mechanisms to reduce small spacecraft and booster separation event shock. Comparative tests were conducted on a structural simulator using five different separation nut mechanisms, consisting of three pyrotechnics from OEA-Aerospace and Hi-Shear Technology and two NEA's from G&H Technology and Lockheed Martin Astronautics (LMA)-Denver, CO. Multiple actuations were performed with preloads up to 7000 pounds, 7000 being the comparison standard. All devices except LMA's NEA rotary flywheel-nut concept were available units with no added provisions to attenuate shock. Accelerometer measurements were recorded, reviewed, processed into Shock Response Spectra (SRS), and comparisons performed. For the standard preload, pyrotechnics produced the most severe and the G&H NEA the least severe functional shock levels. Comparing all results, the LMA concept produced the lowest levels, with preload limited to approximately 4200 pounds. Testing this concept over a range of 3000 to 4200 pounds indicated no effect of preload on shock response levels. This report presents data from these tests and the comparative results.

Lucy, M. H.↗

Cyclic olefin copolymer-based reinforced anion exchange membranes for water electrolyzers

Anion exchange membranes (AEMs) have emerged as a promising technology for water electrolysis in hydrogen production since they offer significant cost reduction in choices of electrocatalysts and bipolar plates. However, AEMs satisfying multiple requirements of high ionic conductivity, good chemical stability, robust mechanical properties, scalable synthesis, and low manufacturing costs are rare. Herein, we introduce quaternary ammonium functionalized cyclic olefin copolymers (COCs) as a new class of chemically stable and low-cost AEM materials. To further enhance the mechanical robustness, we prepared reinforced composite AEMs by impregnating the ionically functionalized COC into a mechanically robust matrix. The resulting reinforced composite membrane exhibits a high hydroxide conductivity of 127 mS cm −1 and excellent mechanical strength. In water electrolyzers, the MEA demonstrated outstanding performance, achieving a current density of 2.24 A cm −2 at 1.8 V, attributable to high conductivity, enhanced mechanical properties, and good alkaline stability of the composite membrane. These results indicate that the COC-based AEMs demonstrate good potential for application in AEM electrolyzers.

08 HYDROGEN↗

Earth Observatory Satellite system definition study. Report no. 4: Management approach recommendations

A management approach for the Earth Observatory Satellite (EOS) which will meet the challenge of a constrained cost environment is presented. Areas of consideration are contracting techniques, test philosophy, reliability and quality assurance requirements, commonality options, and documentation and control requirements. The various functional areas which were examined for cost reduction possibilities are identified. The recommended management approach is developed to show the primary and alternative methods.

Source record↗

Enabling Affordable Communications for the Burgeoning Deep Space Cubesat Fleet

The low costs of development and launch, coupled with new propulsive technologies, have made CubeSats increasingly popular for use in science investigations beyond geosynchronous orbit. As this deep space CubeSat fleet grows in size, the challenge of trying to provide affordable communications for it grows commensurately. The mass, power, and volume constraints inherent to CubeSats limit the antenna size and transmit power that they can use to close the deep space link. As a consequence, CubeSats need to rely more heavily on ground antennas that are characterized by large aperture, low noise temperatures, and relatively high-power transmitters. Such antennas are not in great abundance, nor are they inexpensive to build. For this reason, NASA’s Deep Space Network has been advocating a three-pronged approach to meeting anticipated CubeSat demand: development of simultaneous, shared-beam multi-spacecraft communications capabilities, development of large-antenna cross-support arrangements with other agencies and universities, and development of less uplink-intensive navigation techniques. This paper focuses on the pursuit of simultaneous, shared-beam multi-spacecraft communications capabilities. While the Multiple Spacecraft per Antenna (MSPA) technique has existed for over a decade, it has generally been limited to supporting downlink for just two in-beam spacecraft at a time. This limitation has largely been a function of the number and cost of available receivers. A relatively new technique that potentially overcomes this limitation is Opportunistic MSPA (OMSPA). Instead of relying on additional receivers, OMSPA makes use of a digital recorder at each ground station that is capable of capturing the intermediate frequency (IF) signals from every spacecraft in the antenna beam within the frequency bands of interest. When CubeSat projects see one or more opportunities for their CubeSat(s) to intercept the traditionally scheduled antenna beam of a “host” spacecraft, they can arrange for the CubeSat(s) to transmit open loop during those opportunities. Via a secure Internet site, the CubeSat mission operators can then retrieve the time- and frequency-relevant portions of the digital recording for subsequent demodulation and decoding, or subscribe to a service that does it for them. This “opportunistic” use of a host spacecraft’s ground antenna beam potentially enables CubeSat projects to make use of large ground antennas for downlink without having to compete with bigger, better-funded missions for antenna time in the formal scheduling process. In so doing, it also potentially enables CubeSat projects to avoid the aperture fees associated with formally scheduled downlink time - fees that factor into the “bottom-line” of competitively-bid NASA missions and that actually get charged to non-NASA missions. Taking advantage of these potential OMSPA benefits, however, will require CubeSat projects to pursue mission designs that ensure at least periodic in-beam operations relative to a “host” spacecraft. In the case of a constellation of CubeSats with inter-spacecraft distances that do not extend outside of the beam-width of the desired ground antenna at the given range, one CubeSat can serve as the “host” and have a formally scheduled downlink while the rest of the CubeSats can downlink essentially for “free” via OMSPA. Deep space CubeSats, of course, will need uplink in addition to downlink. Beyond commanding, this need is driven by the use of two-way ranging and Doppler for navigation. While OMSPA may not directly facilitate uplink, it does have the potential to free up antennas for those spacecraft that periodically require formally scheduled links for commanding and two-way radio metrics. NASA is also exploring the physical feasibility of an in-beam, simultaneous multi-spacecraft uplink technique. As with OMSPA, if successful, it will require little new equipment, further enabling affordable deep space CubeSat communications.

Abraham, Douglas S.↗

A deep potential model with long-range electrostatic interactions

Machine learning models for the potential energy of multi-atomic systems, such as the deep potential (DP) model, make molecular simulations with the accuracy of quantum mechanical density functional theory possible at a cost only moderately higher than that of empirical force fields. However, the majority of these models lack explicit long-range interactions and fail to describe properties that derive from the Coulombic tail of the forces. To overcome this limitation, we extend the DP model by approximating the long-range electrostatic interaction between ions (nuclei + core electrons) and valence electrons with that of distributions of spherical Gaussian charges located at ionic and electronic sites. The latter are rigorously defined in terms of the centers of the maximally localized Wannier distributions, whose dependence on the local atomic environment is modeled accurately by a deep neural network. In the DP long-range (DPLR) model, the electrostatic energy of the Gaussian charge system is added to short-range interactions that are represented as in the standard DP model. The resulting potential energy surface is smooth and possesses analytical forces and virial. Missing effects in the standard DP scheme are recovered, improving on accuracy and predictive power. By including long-range electrostatics, DPLR correctly extrapolates to large systems the potential energy surface learned from quantum mechanical calculations on smaller systems. We illustrate the approach with three examples: the potential energy profile of the water dimer, the free energy of interaction of a water molecule with a liquid water slab, and the phonon dispersion curves of the NaCl crystal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗