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DOE OSTI2016

Fukushima Daiichi Unit 1 Accident Progression Uncertainty Analysis and Implications for Decommissioning of Fukushima Reactors - Volume I.

Sandia National Laboratories (SNL) has conducted an uncertainty analysis (UA) on the Fukushima Daiichi unit (1F1) accident progression with the MELCOR code. The model used was developed for a previous accident reconstruction investigation jointly sponsored by the US Department of Energy (DOE) and Nuclear Regulatory Commission (NRC). That study focused on reconstructing the accident progressions, as postulated by the limited plant data. This work was focused evaluation of uncertainty in core damage progression behavior and its effect on key figures-of-merit (e.g., hydrogen production, reactor damage state, fraction of intact fuel, vessel lower head failure). The primary intent of this study was to characterize the range of predicted damage states in the 1F1 reactor considering state of knowledge uncertainties associated with MELCOR modeling of core damage progression and to generate information that may be useful in informing the decommissioning activities that will be employed to defuel the damaged reactors at the Fukushima Daiichi Nuclear Power Plant. Additionally, core damage progression variability inherent in MELCOR modeling numerics is investigated.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Multi-Physics Coupled Seismic Safety Analysis of Molten-Salt Reactors

Pool-type Molten Salt Reactors (MSRs) are a promising advanced nuclear reactor concept relying on passive physical behavior to provide increased safety characteristics. The high heat capacity, high boiling point, unpressurized liquid salt contains the nuclear fuel and as it passes through the vessel achieves criticality and produces nuclear power. The salt then carries away the heat produced along with the delayed neutron precursors towards heat exchangers and primary pumps before entering the core. This forms a highly coupled multiphysics problem between neutronics and fluid flow, which makes modeling these reactors challenging. The safety/licensing case heavily relies on modeling and simulation to prove their safety, and significant effort has been expanded by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program to develop the appropriate simulation tools. Their safety/licensing will require a thorough analysis of their behavior during earthquake-based transients. Earthquakes are a transient condition commonly experienced in many regions, and are safely survived by dozens of reactors every year. Nonetheless, significant conservatisms were introduced with limited predictive modeling and simulation available. The first-of-a-kind capability developed by this research will allow for engineers to analyze ranges of design-basis and beyond-design basis accident scenarios to assess the integrity of the reactor vessel and surrounding system, possibly allowing for limiting the costly conservatisms in the design. This projects uses MASTODON, Griffin, and Pronghorn in the NEAMS ecosystem to model the coupled multiphysics problem posed by an earthquake in a molten salt reactor. It marches through a number of number of coupling schemes, from uncoupled simulations to tightly two-way coupled simulations. The appropriate level of coupling for these simulations will then be determined based on the accuracy in the quantities of interest (QoI) and computational effort involved in each scheme. The QoIs chosen for this paper include the mass flow rate across the heat exchanger (for Pronghorn simulations), power output of the reactor (for Griffin simulations), and the maximum Von Mises stress (for MASTODON simulations). This summary paper reports on the current progress of this project, with 2D tightly coupled multiphysics results.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2016

Development of safety requirements for HTGRs design - 18467

The safety requirements for the design of High Temperature Gas-cooled Reactors (HTGRs), which is analogous to the IAEA specific safety requirements (SSR) for Light Water Reactor (LWR) design (IAEA SSR-2/1), has been developed by the research committee established in the Atomic Energy Society of Japan so as to incorporate the HTGR safety features demonstrated by High Temperature Engineering Test Reactor (HTTR), lessons learned from the accident of Fukushima Daiichi Nuclear Power Station and requirements for the coupling of the hydrogen production plants with nuclear plant. The safety design approach was determined to establish a high level of safety design standards by utilizing inherent safety features of HTGRs. The safety requirements is then developed using the objectives provisions tree methodology based on the safety design approach. The requirements for a structural integrity of fuel during accident conditions, for a confinement structure instead of a leak-tight pressure resistance containment vessel, for a passive residual heat removal from outside of reactor pressure vessel, etc., which are significantly different from those of LWR, are stated in the developed safety requirements. This paper describes overview of the proposed HTGR specific safety requirements. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2023

Fully Implicit Conjugate Heat Transfer Analysis of the ARC-Class Vacuum Vessel

The coupled simulation of fusion reactor blankets including neutronics, thermal-hydraulics and thermo-mechanics is expected to speed up the design cycle of fusion reactor design concepts. In this work we demonstrate tight implicit coupling of conjugate heat transfer using the open-source Computational Fluid Dynamics software OpenFOAM for thermo-fluid mechanics and Diablo for thermo-solid mechanics. The heat transfer analysis is augmented by volumetric energy deposition from neutronic calculations using the Monte Carlo N-particle code on both solid and fluid parts of the vacuum vessel. An additional heat flux is imposed on the first wall estimated from the design power of the reactor. The tight coupling is realized through the open-source coupling library, preCICE, and tested on the vacuum vessel of the affordable, robust, compact reactor design by Commonwealth Fusion Systems. The features of the coupling and the influence of different coupling parameters such as coupling schemes, acceleration techniques and convergence criterion are discussed. The coupled simulation results are compared to a thermal-hydraulics simulation which includes only the fluid domains (the liquid immersion molten salt blanket and cooling channel) to demonstrate usefulness of a coupled simulation. Further analysis is performed to identify regions of hot spots for subsequent design improvement. This introduces the outline for integrating conjugate electromagnetics and fluid/solid mechanics (e.g., allow for deformation of the cooling channel walls) with our present approach for future analysis.

Sircar, Arpan↗

DOE OSTI2024

Mass Optimization of a Multilayered Shield for Transportable Microreactors

The ability to easily transport microreactors is a major selling point for deploying microreactors to remote areas. However, this creates a unique shielding challenge, especially when the microreactor is being shipped after irradiation. A traditional reactor configuration utilizes a separate biological shield and pressure vessel to meet radiological shielding and pressure needs. The limited space available for transportable microreactors for both shielding and pressure vessels requires a revised assessment of separating out the biological shield and pressure vessel. To address these concerns, we examine a nuclear-grade sandwich composite (NGSC) that combines the reactor pressure vessel and biological shielding functions into a single component. Through a series of optimization problems for both transportation and operational use cases, the NGSC is able to minimize dose, minimize the vessel cost, and ensure that weight requirements are met for transportation. Initial results show that using a tungsten-tetraboride cermet in the first two layers of a six-layer NGSC provides adequate shielding for both use cases. These results show promise that an NGSC has enough overlap between operational and transportation cases to help reduce the design space for future analysis and assessment.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2014

Scanning tunneling microscope assembly, reactor, and system

An embodiment of a scanning tunneling microscope (STM) reactor includes a pressure vessel, an STM assembly, and three spring coupling objects. The pressure vessel includes a sealable port, an interior, and an exterior. An embodiment of an STM system includes a vacuum chamber, an STM reactor, and three springs. The three springs couple the STM reactor to the vacuum chamber and are operable to suspend the scanning tunneling microscope reactor within the interior of the vacuum chamber during operation of the STM reactor. An embodiment of an STM assembly includes a coarse displacement arrangement, a piezoelectric fine displacement scanning tube coupled to the coarse displacement arrangement, and a receiver. The piezoelectric fine displacement scanning tube is coupled to the coarse displacement arrangement. The receiver is coupled to the piezoelectric scanning tube and is operable to receive a tip holder, and the tip holder is operable to receive a tip.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2016

Wireless in-core acoustic telemetry and self-powered sensing

A promising wireless telemetry infrastructure based on acoustic transmission of in-pile measurements (information) is being developed at the Idaho National Laboratory for use in nuclear reactors. In this paper, we will demonstrate an approach to telemetry and sensing that exploits a reactor core's energy-rich environment to generate acoustic telemetry signals from self-powered telemeters that produce sounds. These sounds propagate through the reactor's coolant, whether it is gas, water, or liquid metal, through its mechanical structures (e.g., lattice work, pressure vessel, and piping), and can be detected outside the reactor. A thermo-acoustic (TAC) sensor was designed to be geometrically indistinguishable from the other Training Research Isotopes General Atomics (TRIGA) fuel elements in the Breazeale reactor's core. Heat was produced by fission of two Pathfinder {sup 235}UO{sub 2} fuel pellets contained within a finned heat exchanger. The acoustic signals from the TAC sensor can be picked up by hydro-phones and accelerometers anywhere in the reactor pool and from structures that penetrate the pool. Most of the signals we acquired had sufficient signal-to-noise ratios even with both the {sup 16}N diffusion pump and the pool coolant pump operating. The TAC sensor was tested during eight irradiation runs in the Breazeale Nuclear Reactor over the span of a week. We were able to show that the frequency of the thermo-acoustically generated sound provides an accurate determination of the reactor's coolant temperature. Such a sensor strategy might have provided useful information in a reactor accident like that which destroyed the Fukushima complex in March 2011.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2022

Second Annual Report on Development of Microwave Resonant Cavity Transducer for Fluid Flow Sensing

We are investigating a microwave resonant cavity transducer for flow sensing in the vessel of a high temperature fluid advanced reactor (AR), such as a molten salt cooled reactor (MSCR) or a sodium fast reactor (SFR). This transducer is a hollow metallic cylindrical cavity, with the flat wall of the cylinder flexible enough to undergo microscopic deflection due to dynamic fluid pressure. Membrane deflection leads to a shift in the resonant frequency, which can be detected with a spectrum analyzer. Because the transducer is intended for immersion in a high temperature corrosive fluid, understanding of material degradation is crucial for estimation of transducer performance lifetime, and development of measurement interpretation algorithms. We conducted a preliminary computational investigation of relevant damage mechanisms of a stainless steel 316 cylindrical resonator in FLiBe salt. The two main damage mechanisms, creep and corrosion, were modeled using multiphysics COMSOL software. Degradation was modeled for a temperature range 500°C to 700°C. Coupling of the damage mechanisms was not considered. These models predict significant inelastic deformation at most temperatures due to creep, and qualitatively predict chromium depletion both along the liquid/solid interface and along the grain boundaries. An algorithmic approach for compensation of these degradation effects during fluid flow measurements will be developed in the future work. To validate sensor physics, we have performed proof-of-principle test of flow sensing in water. For this test, we have developed a cylindrical resonator for K-band, which was machined from brass. The cavity was excited through WR-42 waveguide through a subwavelength hole on the side of the wall of the cylinder. To increase the spectral signal visibility, we developed a signal processing method for baseline subtraction. A flow loop for proof-of-principle test of transducer performance in water was assembled. A commercial flow meter was installed in the loop for reference measurements. Cylindrical cavity was excited in the TE 011 mode with resonant frequency f ≈ 17.8GHz. Frequency shift of cavity spectral response was obtained by gradually increasing water flow rate from 0 to 60gpm. Corresponding monotonic increase of resonant frequency shift by several MHz was observed. Approximate figure of merit of sensitivity to flow rate is 100KHz/GPM. In addition, we have identified an existing liquid sodium experimental setup for demonstration of flow sensing in environment similar to that of an advanced reactor. The setup consists of a cylindrical vessel and center feed line, where transducer inserted through the lid will measure velocity of the impinging liquid jet. As a calibration experiment, we have assembled a water vessel with center feed with the same dimensions as those of the liquid sodium setup. We have also developed and insertion probe consisting of a 50cm brass waveguide enclosed in protective SS316 tube. Using the water loop, we have demonstrated feasibility of sensing the impinging liquid jet in the vessel.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2016

US Efforts in Support of Examinations at Fukushima Daiichi – 2016 Evaluations

Although it is clear that the accident signatures from each unit at the Fukushima Daiichi Nuclear Power Station (NPS) [Daiichi] differ, much is not known about the end-state of core materials within these units. Some of this uncertainty can be attributed to a lack of information related to cooling system operation and cooling water injection. There is also uncertainty in our understanding of phenomena affecting: a) in-vessel core damage progression during severe accidents in boiling water reactors (BWRs), and b) accident progression after vessel failure (ex-vessel progression) for BWRs and Pressurized Water Reactors (PWRs). These uncertainties arise due to limited full scale prototypic data. Similar to what occurred after the accident at Three Mile Island Unit 2, these Daiichi units offer the international community a means to reduce such uncertainties by obtaining prototypic data from multiple full-scale BWR severe accidents. Information obtained from Daiichi is required to inform Decontamination and Decommissioning activities, improving the ability of the Tokyo Electric Power Company Holdings (TEPCO) to characterize potential hazards and to ensure the safety of workers involved with cleanup activities. This document reports recent results from the US Forensics Effort to use information obtained by TEPCO to enhance the safety of existing and future nuclear power plant designs. This Forensics Effort, which is sponsored by the Reactor Safety Technologies Pathway of the Department of Energy Office of Nuclear Energy Light Water Reactor (LWR) Sustainability Program, consists of a group of US experts in LWR safety and plant operations that have identified examination needs and are evaluating TEPCO information from Daiichi that address these needs. Examples presented in this report demonstrate that significant safety insights are being obtained in the areas of component performance, fission product release and transport, debris end-state location, and combustible gas generation and transport. In addition to reducing uncertainties related to severe accident modeling progression, these insights are being used to update guidance for severe accident prevention, mitigation, and emergency planning. Furthermore, reduced uncertainties in modeling the events at Daiichi will improve the realism of reactor safety evaluations and inform future D&D activities by improving the capability for characterizing potential hazards to workers involved with cleanup activities.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

DOE OSTI2015

FHR Process Instruments

Fluoride salt-cooled High temperature Reactors (FHRs) are entering into early phase engineering development. Initial candidate technologies have been identified to measure all of the required process variables. The purpose of this paper is to describe the proposed measurement techniques in sufficient detail to enable assessment of the proposed instrumentation suite and to support development of the component technologies. This paper builds upon the instrumentation chapter of the recently published FHR technology development roadmap. Locating instruments outside of the intense core radiation and high-temperature fluoride salt environment significantly decreases their environmental tolerance requirements. Under operating conditions, FHR primary coolant salt is a transparent, low-vapor-pressure liquid. Consequently, FHRs can employ standoff optical measurements from above the salt pool to assess in-vessel conditions. For example, the core outlet temperature can be measured by observing the fuel s blackbody emission. Similarly, the intensity of the core s Cerenkov glow indicates the fission power level. Short-lived activation of the primary coolant provides another means for standoff measurements of process variables. The primary coolant flow and neutron flux can be measured using gamma spectroscopy along the primary coolant piping. FHR operation entails a number of process measurements. Reactor thermal power and core reactivity are the most significant variables for process control. Thermal power can be determined by measuring the primary coolant mass flow rate and temperature rise across the core. The leading candidate technologies for primary coolant temperature measurement are Au-Pt thermocouples and Johnson noise thermometry. Clamp-on ultrasonic flow measurement, that includes high-temperature tolerant standoffs, is a potential coolant flow measurement technique. Also, the salt redox condition will be monitored as an indicator of its corrosiveness. Both electrochemical techniques and optical spectroscopy are candidate fluoride salt redox measurement methods. Coolant level measurement can be performed using radar-level gauges located in standpipes above the reactor vessel. While substantial technical development remains for most of the instruments, industrially compatible instruments based upon proven technology can be reasonably extrapolated from the current state of the art.

FHR↗

DOE OSTI2024

Comparison of PM-HIP to forged SA508 pressure vessel steel under high-dose neutron irradiation

Not Available

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

NASA NTRS1971

A mini-cavity probe reactor.

The mini-cavity reactor is a rocket engine concept which combines the high specific impulse from a central gaseous fueled cavity (0.6 m diam) and NERVA type fuel elements in a driver region that is external to a moderator-reflector zone to produce a compact light weight reactor. The overall dimension including a pressure vessel that is located outside of the spherical reactor is approximately 1.21 m in diameter. Specific impulses up to 2000 sec are obtainable for 220 to 890 N of thrust with pressures less than 1000 atm. Powerplant weights including a radiator for disposing of the power in the driver region are between 4600 and 32,000 kg - less than payloads of the shuttle. This reactor could also be used as a test reactor for gas-core, MHD, breeding and materials research.

Hyland, R. E.↗

DOE OSTI2017

A Cyclic-Plasticity-Based Mechanistic Approach for Fatigue Evaluation of 316 Stainless Steel Under Arbitrary Loading

In this paper, a cyclic-plasticity based fully mechanistic fatigue modeling approach is presented. This is based on time-dependent stress-strain evolution of the material over the entire fatigue life rather than just based on the end of live information typically used for empirical S~N curve based fatigue evaluation approaches. Previously we presented constant amplitude fatigue test based related material models for 316 SS base, 508 LAS base and 316 SS- 316 SS weld which are used in nuclear reactor components such as pressure vessels, nozzles, and surge line pipes. However, we found that constant amplitude fatigue data based models have limitation in capturing the stress-strain evolution under arbitrary fatigue loading. To address the above mentioned limitation, in this paper, we present a more advanced approach that can be used for modeling the cyclic stress-strain evolution and fatigue life not only under constant amplitude but also under any arbitrary (random/variable) fatigue loading. The related material model and analytical model results are presented for 316 SS base metal. Two methodologies (either based on time/cycle or based on accumulated plastic strain energy) to track the material parameters at a given time/cycle are discussed and associated analytical model results are presented. From the material model and analytical cyclic plasticity model results, it is found that the proposed cyclic plasticity model can predict all the important stages of material behavior during the entire fatigue life of the specimens with more than 90% accuracy

316 Stainless Steel↗

DOE OSTI2022

TCR Central Shutdown Rod Fine Motion Control

Transformational Challenge Reactor (TCR) is a Helium cooled 3 MWt test reactor that leverages advances in materials and manufacturing, computing, and AI in its design. Classical design of a shutdown rod uses either gravity, pneumatic, or springs to quickly release the Central Shutdown Rod (CSR) containing neutron absorber into the reactor core stopping nuclear reaction. Generally, the motor/actuator resides outside the reactor, but the motion is transmitted through a penetration into the pressure vessel. There are also designs where the control rod drive incorporates magnetic latches with coil residing outside the pressure boundary for precise position control of the rod. We are proposing a magnetic coupling to position the shutdown rod without any penetration into the pressure vessel for the entire drive length of TCR shutdown rod. Electromagnets are currently used in non-power nuclear reactors for shutdown rods, but these electromagnets are resident inside the reactor pressure vessel. This paper will describe the use of an electromagnet outside the pressure vessel to position and release the shutdown rod. A prototype was developed at ORNL to demonstrate the concept, and a design optimization of the ferritic core and material was conducted to maximize the lift force of the electromagnet. An elevated temperature testing was also performed to ensure that the system will perform under the temperature conditions inside an operating reactor.

Fountain, Eliott J.↗

DOE OSTI2023

Demonstration of Microwave Cavity Transducer Performance in High Temperature Fluid Flow Sensing: Development of Microwave Cavity Flow Meter for Advanced Reactor High Temperature Fluids

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2026

Integrated Simulation of Weld Residual Stress Evolution and Crack Propagation Using XFEM

Nuclear power plant components operate in environments that promote multiple degradation mecha- nisms, several of which involve crack initiation and growth. An ongoing effort in the U.S. Department of Energy’s Nuclear Energy Advanced Modeling and Simulation (NEAMS) program is developing a general capability within the Multiphysics Object Oriented Simulation Environment (MOOSE) framework for simulating three-dimensional crack growth under a range of driving conditions, including fatigue, stress corrosion cracking (SCC), brittle fracture, and stress-relaxation cracking. This report demonstrates an end-to-end workflow that uses this capability to model weld-residual-stress-driven SCC in the J-groove weld of a pressurized-water reactor control rod drive mechanism penetration in the vessel head. The workflow consists of a thermomechanical welding simulation with temperature-dependent plasticity, followed by cooldown to ambient conditions, and a restart of the simulation using the MOOSE extended finite element method (XFEM) module to propagate a three-dimensional crack through the residual stress field. New welding capabilities were developed to properly initialize newly activated elements in the weld region, and robustness improvements were made to the mesh-based algorithm for defining cutting planes in the 3D XFEM algorithm, allowing it to handle complex crack fronts and stress fields. Together these advances allowed the simulated SCC crack to grow from an initial elliptical flaw in the weld, across the weld, through the tube wall, and almost to the triple point (where the weld, tube, and reactor pressure vessel head intersect) over roughly 36 years of simulated service. These results demonstrate a workflow that can be extended to fully three-dimensional welding simulations and more complex crack interaction problems.

42 - ENGINEERING↗

DOE OSTI2015

COUPLING OF RELAP5-SCDAP MOD4.0 AND NEUTRONIC CODES

High-fidelity and accurate nuclear system codes play a key role in the design and analysis of complex nuclear power plants, which consist of multiple subsystems, such as the reactor core (and its fuel, burnable poisons, control elements, etc.), the reactor internal structures, the vessel, and the energy conversion subsystem and beyond to grid demand. Most commonly the interplay between these various subsystems is modeled using coupled codes, each of which represents one of the subsystems. And the most common direct coupling is that of thermal-hydraulics and neutronics codes. The subject of this paper is the coupling of codes that model not only thermal-hydraulics and neutronics, but also structural components damage. Furthermore, the neutronic component is not limited to the sole core solver. The coupled code system encompasses thermal-hydraulics, material performance of the fuel, neutronic solver, and neutronic data preparation. Thus, this paper presents a framework for coupling RELAP5/SCDAPSIM/MOD4.0 with a suite of neutron kinetics codes that includes NESTLE, DRAGON and a version of the ENDF library. The version of the RELAP5/SCDAPSIM/MOD4.0 code used in this work is one developed by Innovate System Software (ISS) as part of the international SCDAP Development and Training Program (SDTP) for best-estimate analysis to model reactor transients including severe accident phenomena. This RELAP5/SCDAPSIM/MOD4.0 code version is also capable of predicting nuclear fuel performance. It uses nodal power distributions to calculate mechanical and thermal parameters such as heat-up, oxidation and meltdown of fuel rods and control rods, the ballooning and rupture of fuel rod cladding, the release of fission products from fuel rods, and the disintegration of fuel rods into porous debris and molten material. On the neutronics side, this work uses the NESTLE and DRAGON codes. NESTLE is a multi-dimensional static and kinetic neutronic code developed at North Carolina State University. It solves up to four energy groups neutron diffusion equations utilizing the Nodal Expansion Method (NEM) in Cartesian or hexagonal geometry. The DRAGON code, developed at Ecole Polytechnique de Montreal, performs lattice physics calculations based on the neutron transport equation and is capable of using very fine energy group structures. In this work, we have developed a coupling approach to exchange data among the various modules. In the coupling process, the generated nuclear data (in fine multigroup energy structure) are collapsed down into two- or four-group energy structures for use in NESTLE. The neutron kinetics and thermal-hydraulics modules are coupled at each time step by using the cross-section data. The power distribution results of the neutronic calculations are transmitted to the thermal-hydraulics code. The spatial distribution of coolant density and the fuel-moderator temperature, which result from the thermal-hydraulic calculations, are transmitted back to the neutron kinetics codes and then the loop is closed using new neutronics results. Details of the actual data transfers will be described in the full length paper.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2016

In situ secondary organic aerosol formation from ambient pine forest air using an oxidation flow reactor

Abstract. An oxidation flow reactor (OFR) is a vessel inside which the concentration of a chosen oxidant can be increased for the purpose of studying SOA formation and aging by that oxidant. During the BEACHON-RoMBAS (Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen–Rocky Mountain Biogenic Aerosol Study) field campaign, ambient pine forest air was oxidized by OH radicals in an OFR to measure the amount of SOA that could be formed from the real mix of ambient SOA precursor gases, and how that amount changed with time as precursors changed. High OH concentrations and short residence times allowed for semicontinuous cycling through a large range of OH exposures ranging from hours to weeks of equivalent (eq.) atmospheric aging. A simple model is derived and used to account for the relative timescales of condensation of low-volatility organic compounds (LVOCs) onto particles; condensational loss to the walls; and further reaction to produce volatile, non-condensing fragmentation products. More SOA production was observed in the OFR at nighttime (average 3 µg m−3 when LVOC fate corrected) compared to daytime (average 0.9 µg m−3 when LVOC fate corrected), with maximum formation observed at 0.4–1.5 eq. days of photochemical aging. SOA formation followed a similar diurnal pattern to monoterpenes, sesquiterpenes, and toluene+p-cymene concentrations, including a substantial increase just after sunrise at 07:00 local time. Higher photochemical aging (> 10 eq. days) led to a decrease in new SOA formation and a loss of preexisting OA due to heterogeneous oxidation followed by fragmentation and volatilization. When comparing two different commonly used methods of OH production in OFRs (OFR185 and OFR254-70), similar amounts of SOA formation were observed. We recommend the OFR185 mode for future forest studies. Concurrent gas-phase measurements of air after OH oxidation illustrate the decay of primary VOCs, production of small oxidized organic compounds, and net production at lower ages followed by net consumption of terpenoid oxidation products as photochemical age increased. New particle formation was observed in the reactor after oxidation, especially during times when precursor gas concentrations and SOA formation were largest. Approximately 4.4 times more SOA was formed in the reactor from OH oxidation than could be explained by the VOCs measured in ambient air. To our knowledge this is the first time that this has been shown when comparing VOC concentrations with SOA formation measured at the same time, rather than comparing measurements made at different times. Several recently developed instruments have quantified ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) that were not detected by a proton transfer reaction time-of-flight mass spectrometer (PTR-TOF-MS). An SOA yield of 18–58 % from those compounds can explain the observed SOA formation. S/IVOCs were the only pool of gas-phase carbon that was large enough to explain the observed SOA formation. This work suggests that these typically unmeasured gases play a substantial role in ambient SOA formation. Our results allow ruling out condensation sticking coefficients much lower than 1. These measurements help clarify the magnitude of potential SOA formation from OH oxidation in forested environments and demonstrate methods for interpretation of ambient OFR measurements.

54 ENVIRONMENTAL SCIENCES↗