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At least 1,243 records · Page 69
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Nuclear Data Impact on Key Metrics for a Representative Molten Chloride Fast Reactor Model

Nuclear data are an essential component of the foundation on which all modeling and simulation methods and tools are relying upon, from the front end to the back end of the nuclear fuel cycle. In this study, the impact of uncertainties in nuclear data is investigated for a representative molten chloride fast reactor, for several important metrics, including eigenvalue, reactivity differences, and nuclide inventories in fuel at 5-yr irradiation. Uncertainty of keff for a full core model was found to be similar between the fresh fuel and the irradiated fuel states (1.7-1.8%), with its primary driver being the uncertainty in the 235U (n,γ) cross section. The results obtained for the reactivity differences show large uncertainties, of over 100%, in elastic scattering sensitivities of several nuclides, which led to large uncertainties of temperature reactivity differences for cladding and reflector. These results provide evidence that the currently applied methods may not be sufficiently adequate for ensuring the reliable determination of such metrics.

Procop, Germina [ORNL] (ORCID:0000000342226393)↗
DOE OSTI2026

Design optimization of MAPS-based detectors using a data-driven fast simulation approach

A parametric simulation tool for pixel sensors is presented. A realistic pixel response is simulated purely based on measurement input, without requiring detailed knowledge of the underlying manufacturing process. As such, it provides an efficient alternative to the use of Technology Computer-Aided Design simulations, which typically depend on proprietary process information. Due to its parametric approach, the package is fast and thus particularly useful for larger detector systems and high hit rate environments. This work presents measurements, simulation and its validation for the MALTA2 sensor. It is a small collection electrode monolithic active pixel sensor produced in the Tower 180 nm complementary metal-oxide-semiconductor imaging process. Modifications to the sensor’s periphery, mainly in the hit merger, are studied in order to optimize the performance for tracking and calorimetry. This optimization is of special interest as part of the MALTA3 sensor redesign in the 65 nm Tower Partners Semiconductor Co. process.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Tank 48H Phase 1 Initial Testing Using Sodium Permanganate to Decompose Tetraphenylborate: Simulant Studies with Shaker Oven and 2-L Vessel

Tank 48H currently holds legacy material including organic tetraphenylborate (TPB) compounds from the operation of the In-Tank Precipitation process. The large quantity of TPB is not compatible with the waste treatment facilities at SRS and must be removed or undergo treatment to oxidize the organic compounds before the tank can be returned to routine Tank Farm service. Tank 48H currently holds approximately 270,000 gallons of legacy material comprised of decontaminated salt solution, approximately 20,000 kilograms of TPB solids, 3,400 kilograms of sludge solids, and 1,800 kilograms of monosodium titanate (MST).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Issue Resolution During the Development of the Performance Assessment for the Savannah River Site Saltstone Disposal Facility - 20125

In 2019, Savannah River Remediation developed a revision to the performance assessment (PA) on behalf of the U.S. Department of Energy (DOE) Savannah River Operations Office (SR) for the near-surface disposal of low-level waste at the Savannah River Site (SRS) Saltstone Disposal Facility (SDF). Soluble waste from SRS Tank Farms undergoes salt processing to remove cesium and other high-activity constituents. The low-activity decontaminated salt solution (DSS) is then immobilized by mixing it into a cementitious waste form known as saltstone. After mixing, the saltstone is poured into leak-tight concrete vaults, known as saltstone disposal units (SDUs), where the waste form cures. By the time of facility closure, the SDF is expected to consist of 15 SDUs with a combined capacity of 1.06 E+09 L (280 Mgal) of cured saltstone. The facility operates under a Disposal Authorization Statement from DOE and a permit from the South Carolina Department of Health and Environmental Control (SCDHEC). Since the start of operations in 1990, the SDF has received almost 6.7 E+07 L (18 Mgal) of DSS, resulting in the safe disposal of 2.7 E+16 Bq (7.3 E+05 Ci) of activity. Due to the radioactive decay of short-lived contaminants, the total remaining activity in the disposed waste is estimated to be approximately 1.4 E+16 Bq (3.9 E+05 Ci), as of September 2018. The Disposal Authorization Statement requires a demonstration that the system of engineered and natural features of the disposal facility will limit releases from the facility and be protective of human health and the environment for at least the next 1,000 years. The long-term performance of the facility was evaluated under the requirements of the DoE's Radioactive Waste Management Manual (US DOE Manual 435.1-1). Simulations were performed to demonstrate that the disposal facility would meet performance objectives specified in the manual. The evaluation was based on numerical models that simulate the releases of contaminants from the saltstone waste form. Contaminants were transported through groundwater and air pathways to points of assessment to evaluate compliance (i.e., 100 m from the SDUs). In addition, the potential consequences of an inadvertent human intrusion (IHI) were also evaluated. A number of issues were overcome during the development of these simulations. These issues were identified as part of internal technical reviews. Simulations are developed by people and people make mistakes, so the internal technical review process is a vital step in PA development. Specific examples of resolved issues include a unit-conversion error, an inappropriate definition for a model boundary condition, a model time-stepping issue, and an error in the calculation for the buildup of contaminants in soil. Actions taken to address these issues resulted in an improved product with a better supported technical basis and more defensible results. The identification and correction of these issues are discussed. By understanding these issues, model developers and technical reviewers working on PAs in the future may avoid repeating these types of mistakes. Transparency with respect to these mistakes builds trust between waste management sites, regulators, and stakeholders. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1988

Simulation of proton-induced energy deposition in integrated circuits

A time-efficient simulation technique was developed for modeling the energy deposition by incident protons in modern integrated circuits. To avoid the excessive computer time required by many proton-effects simulators, a stochastic method was chosen to model the various physical effects responsible for energy deposition by incident protons. Using probability density functions to describe the nuclear reactions responsible for most proton-induced memory upsets, the simulator determines the probability of a proton hit depositing the energy necessary for circuit destabilization. This factor is combined with various circuit parameters to determine the expected error-rate in a given proton environment. An analysis of transient or dose-rate effects is also performed. A comparison to experimental energy-disposition data proves the simulator to be quite accurate for predicting the expected number of events in certain integrated circuits.

Fernald, Kenneth W.↗
DOE OSTI2020

Laboratory-Scale Melter Systems for Simulated and Real AP-107 Tank Waste - 20483

The Hanford Waste Treatment and Immobilization Plant (WTP) will process and stabilize waste that is stored in underground tanks on the Hanford Site. At the WTP, the tank waste will be combined with glass-forming and modifying additives to form an aqueous and solid mixture called melter feed, which will then be vitrified in joule-heated melters. A small-scale melter system, the continuous laboratory-scale melter (CLSM), is designed to operate with a continuous feeding process while periodically pouring glass product and collecting off-gas. Two CLSMs were constructed: one in a non-radioactive environment for processing waste simulants and another in a fume hood capable of handling radioactive material for processing actual Hanford tank waste. The waste sample received for vitrification in the CLSM was from Hanford tank 241-AP-107. Approximately 12 liters of melter-feed slurry was vitrified into 7 kilograms of glass product over the course of 10 hours of charging to the CLSM. The partitioning of technetium-99 in the product streams was used to calculate the technetium-99 recovery and help determine when the vitrification process had reached a steady state. The average single-pass retention of technetium-99 in the glass product was then calculated for the processing of AP-107 waste in the CLSM system. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Cold ion beam in a storage ring as a platform for large-scale quantum computers and simulators: Challenges and directions for research and development

The purpose of this paper is to evaluate the possibility of constructing a large-scale storage-ring-type ion-trap system capable of storing, cooling, and controlling a large number of ions as a platform for scalable quantum computing (QC) and quantum simulations. In such a trap, the ions form a crystalline beam moving along a circular path with a constant velocity determined by the frequency and intensity of the cooling lasers. In this paper, we consider a large leap forward in terms of the number of ions that serve as qubits in QC, from fewer than 100 available in state of the art linear ion-trap devices today to an order of 10 5 crystallized ions in the storage-ring setup. This new trap design unifies two different concepts: the storage rings of charged particles and the linear ion traps used for QC and mass spectrometry. In this paper, we use the language of particle accelerators to discuss the ion state and dynamics. We outline the differences between the above concepts, analyze challenges of the large ring with a revolving chain of ions, and propose goals for the research and development required to enable future quantum computers with 1000 times more qubits than available today. The challenge of creating such a large-scale quantum system while maintaining the necessary coherence of the qubits and the high fidelity of quantum logic operations is significant. Performing analog quantum simulations may be an achievable initial goal for such a device. Quantum calculations and simulations of complex quantum systems will move forward both the fundamental science and the applied research. Nuclear and particle physics, many-body quantum systems, lattice gauge theories, and nuclear structure calculations are just a few examples in which a large-scale quantum simulation system will become a very powerful tool to move forward our understanding of nature.

36 MATERIALS SCIENCE↗
DOE OSTI2022

The Feasibility and the Benefits of the Advanced Nuclear Fuel Pellet Designs with Radially Varying Fuel Zoning and Burnable Poison Concentration (Final Summary Report)

As part of the work supported by the US Department of Energy (DOE) Office of Nuclear Energy (NE) Gateway for Accelerated Innovation in Nuclear (GAIN) FY 2021 Voucher, Exelon Generation, now Constellation, and Oak Ridge National Laboratory (ORNL) entered into a cooperative research and development agreement (CRADA) to evaluate and assess the feasibility and impact of various conceptual advanced nuclear fuel pellet designs (ANFPDs). The objective of this project was to perform modeling and simulation and analyses using the advanced modeling and simulation capabilities of VERA/BISON, developed by DOE, to determine the viability and benefits of numerous advanced nuclear fuel pellet design concepts in terms of fuel cycle costs, operational safety, and margin improvement. Whereas the detailed coupled neutronic and thermal hydraulic analyses performed using VERA provided in-depth knowledge in terms of fuel cycle performance, the detailed VERA results were used in subsequent fuel performance analyses using BISON. These subsequent analyses focused on several key fuel performance criteria, such as peak fuel centerline temperature (FCT), fission gas release (FGR), gap closure, plenum pressure, and cladding hoop stress. These key fuel performance criteria were analyzed for some of the conceptual fuel designs and were compared with the results obtained for UO 2 fuel. The results provided detailed information to enable better understanding of the performance of the fuel types analyzed. Understanding the advantage of loading these conceptual fuel designs into the core is important not only to Constellation but also to the entire light-water reactor (LWR) fleet in the United States.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Correlation between time and angular alignment in molecular dynamics simulations of heavy ion collisions

Neutron-proton equilibration is a process which has been used to study the density dependence of the symmetry energy term in the nuclear equation-of-state. Here, this study utilizes constrained molecular dynamics (CoMD) simulations of 70 Zn + 70 Zn with collision energies of 35 and 45 MeV/nucleon. An algorithm is used which searches through CoMD events and identifies the PLF* after it separates from the target and determines its lifetime, Δt. It also determines the fragments that the PLF* breaks apart into and determines their angular alignment. This technique gives an opportunity to explore how the average alignment of dynamically produced fragments, $\langle$α $\rangle$ dyn , evolves with PLF* lifetime. An approximately linear relationship was determined with d$\langle$α $\rangle$ dyn /dΔt = 0.98 ± 0.08 rad / zs and 1.06 ± 0.09 rad / zs for the 35 and 45 MeV / nucleon, respectively, indicating a correlation with magnitude consistent with classically determined values which were used for prior experimental studies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1984

The climatic effects of nuclear war

The effects of various US-USSR nuclear-exchange scenarios on global climate are investigated by means of computer simulations, summarizing the results of Turco et al. (1983) and follow-up studies using 3D global-circulation models. A nuclear-scenario model is used to determine the amounts of dust, smoke, radioactivity, and pyrotoxins generated by a particular type of nuclear exchange (such as a general 5,000-Mt exchange, a 1,000-Mt limited exchange, a 5,000-Mt hard-target counterforce attack, and a 100-Mt attack on cities only): a particle-microphysics model predicts the evolution of the dust and smoke particles; and a radiative-convective climate model estimates the effects of the dust and smoke clouds on the global radiation budget. The findings are presented in graphs, diagrams, and a table. Thick clouds blocking most sunlight over the Northern Hemisphere midlatitudes for weeks or months and producing ground-temperature reductions of 20-40 C, disruption of global circulation patterns, and rapid spread of clouds to the Southern Hemisphere are among the 'nuclear-winter' effects predicted for the 5,000-Mt baseline case. The catastrophic consequences for plant, animal, and human populations are considered, and the revision of superpower nuclear strategies is urged.

Turco, R. P.↗
DOE OSTI2024

Thermal and hydraulic performance of volumetrically heated triply periodic minimal surface heaters

Advanced heat transfer surfaces, mainly Triply Periodic Minimal Surfaces (TPMSs) have great potential to increase heat transfer performance over traditional heat transfer surfaces due to their tortuous flow path and higher surface area-volume ratio. The emergence of additive manufacturing of nuclear fuel motivates experimental investigation of such advanced geometries in the context of a nuclear reactor core. Here, this study employed a novel method to explore the performance of gyroid and diamond TPMS geometries. Volumetrically heated heaters were additively manufactured from conductive polymer filament, and airflow was used to simulate the convective heat transfer from the core within a nuclear reactor. The mass flow and volumetric generation rates were varied, local Nusselt number correlations were obtained using embedded thermocouples to measure the solid and fluid temperature, and friction factor correlations were developed using differential pressure measurements. The gyroid TPMS presented a friction factor 1.5 times higher than the diamond TPMS and 90 times that of the rod bundle. TPMS geometries showed Nusselt numbers 8–10 times higher than that of the rod bundle, also maintaining colder internal temperatures, which suggested that they could sustain 250–275 % higher power density than the rod bundle for a given centerline temperature. Hence, having the potential to greatly increase the safety margins and power output of a nuclear reactor core with similar volume.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRSDate not supplied

Effects of Simulated Microgravity and LINC-Complex on Chromosome 8 of Human Mammary Cells

Previously, human breast epithelial cells were studied under simulated microgravity to determine the role of the LINC-complex in maintaining nuclear morphology and gene expression. Data from that study was used in this project to understand how the LINC-complex influences gene expression at chromosome 8 under simulated microgravity. Differentially expressed genes found in clusters typically indicate a molecular relationship amongst them. Visual and data analyses (GO, pathways) identified 51 genes within clusters on chromosome 8 across various simulated microgravity conditions that did not share any molecular relationship. Additional results also determined that cells with a disrupted LINC-complex experienced more differential gene expression than the control, and that extended periods of simulated microgravity exacerbated differential gene expression in chromosome 8 of LINC-disrupted cells. These results suggest that the stressful simulated microgravity environment coupled with disrupted biological processes, such as in the case of the LINC-complex, can increase differential gene expression in chromosomes. Future studies where additional analyses are performed to further analyze gene expression of clusters under simulated microgravity could potentially elucidate the molecular relationship amongst affected genes.

Simulated microgravity↗
DOE OSTI2021

Assessment of Fast Reactor Hot Channel Factor Calculation Capability in Griffin and NekRS

The DOE-NE Advanced Modeling and Simulation (NEAMS) program develops, demonstrates, and deploys predictive computational modeling tools for nuclear reactor design and analysis. Under the Fast Reactor Applications activity within the Application Drivers Technical Area of NEAMS, the ability to perform high fidelity “hot channel factor” (HCF) coupled multiphysics simulations has been identified as a valuable simulation capability.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Tool for Developing Integrated Strategies for Decontamination and Waste Management - 20291

Management of waste from chemical, biological, and radiological incidents is complicated by the fact that decontamination decisions have a profound impact on the characteristics of resulting waste streams. Wide-area biological and radiological incidents could produce massive quantities of waste that may need to be treated on-site and sent for subsequent disposal as non-contaminated materials, or else be directly disposed of as contaminated materials. The EPA has developed the Waste Estimation Support Tool (WEST) for characterizing and quantifying biological and radiological waste that may be generated from decontamination efforts. This paper focuses on the WEST's uses for radiological incidents. WEST combines Geographic Information System (GIS)-based analysis of externally-supplied plume data, infrastructure databases derived from the Federal Emergency Management Agency's (FEMA's) Hazus tool [1], and satellite imagery surface recognition algorithms to combine the composition and square footage of the buildings in the plume with estimates of the materials between the buildings in the plume. The resulting GIS data files are then imported into a Microsoft Access database application, where they are combined with information about the nature and concentration of contaminants, and then subjected to decontamination strategies for different contaminated surfaces. The tool provides estimates of the type and quantities of potential wastes resulting from simulated decontamination and/or demolition activities and includes estimates of the remaining contamination levels including residual contamination contained within each waste stream. Estimates are presented at several levels of detail, allowing users to obtain needed data at the desired resolution. These include estimates for the total affected area, estimates by contamination zone, estimates by decontamination method(s), and estimates by building type (occupancy classification). EPA is currently developing the next version of WEST which will include several substantial enhancements. The most significant improvement for the next version of WEST will include the ability for users to develop contamination scenarios and waste estimates based on previously developed, readily available, and geographically specific infrastructure data. Instead of using WEST's default infrastructure data based on FEMA's Hazus tool, users will be able to import their own building data specific to the geographically affected area. This capability may substantially decrease uncertainties in the resulting waste estimates because the results will be based on actual building data (numbers of each type, square footage, building height, etc.). Two other significant enhancements will be the ability to generate waste estimates for vehicles and biomass. In addition to building debris and building decontamination waste, vehicles and biomass will likely constitute a significant percentage of the total waste which may result from wide area contamination events. This presentation will present the most recent version of WEST, which includes such considerations as affected biomass (e.g., trees), vehicles, and the ability to replace the default Hazus infrastructure databases with custom infrastructure databases. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Need for advanced research reactors for the next-generation reactor physics, analysis tools, and technology

Full text of publication follows. There is an urgent need for design and deployment of advanced research and test reactors in support of design, licensing and operation of advanced power reactors and education of next generation nuclear workforce. Existing research reactors mostly were designed and constructed decades ago with the main objectives of training operators, performing reactor physics experiments, and educating nuclear engineers and scientists. There are already gaps and significant concern about future capabilities for the existing research reactor facilities to address modern instrumentation and/or flexible environments for: performing reactor physics studies for advanced designs which have significantly different core materials forms and compositions, reactor shapes and size; validation of advanced high-fidelity software; development of machine learning algorithms for enhancement of human-machine collaboration in support of reactor monitoring, operation and safeguards; and, effective education of the next-generation workforce. The authors will focus on the need for advanced research reactors to improve and validate fast and accurate simulation tools for high-fidelity modeling and analysis of nuclear reactors in support of their design, optimization, licensing, operation, and monitoring. In the past, simulation tools were limited to relatively coarse models using approximate methodologies that benefited from two main factors: i) allowance for large margins and tolerances; ii) ability to construct prototype (e.g., zero power) reactors for adjustment of approximate methodologies. The next generation reactors have to be designed mainly by using novel high-fidelity computational tools that are accurate and fast, and therefore can be used for parametric studies and uncertainty quantification. To sufficiently demonstrate the accuracy of these tools, advanced research reactors are needed. The authors argue the need for new computational paradigms such as the MRT (Multistage, Response- function Transport) methodology which has resulted in the development of the novel high-fidelity RAPID (Real-time Analysis for Particle-transport and In-situ Detection) code system. Such code systems have to be robust in modeling any complex system, and should be fast and accurate, henceforth their uncertainties can be quantified at reasonable costs. Again, advanced research reactors are needed for the validation of the fidelity and accuracy of new computational tools. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2020

Use of Micro-Gravity Sensors for External Fluid Level Monitoring in Waste and Nuclear Related Applications - 20315

There are a number of applications in nuclear energy and hazardous waste disposal that require monitoring of fluids under extreme environments, including high levels of temperature, pressure, toxicity and radioactivity. Many of these applications will benefit from a monitoring technique that is external and non-invasive. Currently the sensors used are invasive, must reside inside the pressurized vessels and must penetrate the vessel walls, which can create a weakness in the vessel. Additionally, instruments that are used inside such containers must be exceptionally hardened to the environment. Information Systems Laboratories (ISL) has developed an external mass (gravimetric) measuring technique for monitoring nuclear coolant in Small Modular Reactors (SMRs), which will also work for measuring fluid levels in waste tanks, that avoids the problems inherent in invasive sensors. It utilizes a COTS gravitational sensor of unprecedented accuracy, leveraged via proper sensor placement geometry, to detect fluid changes of small amplitude from an outside position, obviating the need to penetrate the vessel. The technique is called Gravisense{sup TM}. ISL has proven via simulation and experiment that this concept can be usefully applied to monitoring fluid levels in both nuclear reactors and large waste tanks. Numerical simulation algorithms were developed to calculate the gravity effect of small changes in water level, which were verified by experiments at the NIST Physical Simulator facility at the Oregon State University. The measured ultralow noise levels of the superconducting gravimeter type which utilizes a Niobium sphere suspended in a magnetic field to attain its phenomenal accuracy, demonstrated that fluid levels in SMRs can be measured at least to within 3 cm. Furthermore, the method can distinguish between a contained leak (from reactor to containment vessel) from an external leak (from reactor to outside of containment). Additionally, simulations of waste canisters that hold spent fuel rods show that the fluid level measuring accuracy can potentially do better than 1 cm accuracy by measuring from below the vessel, and judicious placement of sensors on top of large waste tanks can potentially achieve a very impressive 2 mm measurement accuracy. These encouraging results prove that the Gravisense{sup TM} technique for fluid determination can be very useful in nuclear energy generation, testing, and research, as well as in waste monitoring situations that are difficult to monitor via traditional sensing technology. We believe that the next step should be to test the technique on canisters of the type that are currently storing waste in various DOE locations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

High-burnup fuel stress analysis prior to and during a LOCA transient

High-burnup fuel fragmentation and pulverization have been experimentally observed during simulated loss-of-coolant accident (LOCA) transient testing of high-burnup (>62 GWd/tU) nuclear fuel. The cause of this phenomenon is generally accepted to be the formation of stresses arising from the off-normal conditions. However, the primary mechanism(s) contributing to the stress formation is/are still being debated. Leading hypotheses suggest that the concurrence of fission gas bubbles and high burnup structure on the pellet periphery (i.e., the rim) leave the fuel susceptible to pulverization. Other hypotheses suggest that pulverization is artificially inflated during externally heated tests that do not reproduce prototypic fuel stresses and radial temperature profiles as the fuel transitions from full-power nuclear heating to decay heating. This work performs finite element analyses of fuel pellet temperatures and macroscopic stresses prior to and during a LOCA transient to identify (1) operating conditions that may exacerbate the fuel pellet stress state, (2) differences in predicted stresses with nuclear vs. furnace heating, and (3) how fuel cracking impacts the subsequent stress state in the pellet fragments. Analyses predict that macroscopic transient fuel stresses resulting from constrained thermal expansion will remain below the fracture stress of fresh UO 2 once the fragment size reaches ~4 mm or less. Calculated fuel stresses from simulated LOCA tests performed with representative nuclear vs. electrical heating rates are shown to be equal within 5% and essentially unchanged for all times after the first 27 seconds of the transients. Because the fuel stresses do not change once the temperature profile becomes uniform, macroscopic transient stresses would be no different than those following a normal shutdown. Because pulverization of high burnup fuel does not occur prior to a LOCA test, pulverization of high burnup UO 2 cannot be initiated by differential thermal stresses.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Signatures of electronic and nuclear coherences in ultrafast molecular x-ray and electron diffraction

Femtosecond x-ray and electron diffraction hold promise to image the evolving structures of single molecules. We present a unified quantum-electrodynamical formulation of diffraction signals, based on the exact many-body nuclear + electronic wavefunction that can be extracted from quantum chemistry simulations. This gives a framework for analyzing various approximate molecular dynamics simulations. We show that the complete description of ultrafast diffraction signals contains interesting contributions involving mixed elastic and inelastic scattered photons that are usually masked by other larger contributions and are neglected. These terms include overlaps of nuclear wavepackets between different electronic states that provide an electronic decoherence mechanism and are important for the time-resolved imaging of conical intersections.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗