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DOE OSTI2022

Enhancement of radiation detection performance with reduction of EH 6/7 deep levels in n-type 4H–SiC through thermal oxidation

We report the effect of EH 6/7 electron trap centers alone on the performance of high-resolution radiation detectors fabricated on n-type 4H–SiC epitaxial layers. A Schottky barrier detector (SBD) and a metal-oxide-semiconductor (MOS) capacitor detector fabricated using two sister samples derived from the same 50 μm 4H–SiC parent wafer exhibited widely different energy resolutions of 0.4% and 0.9% for 5486 keV alpha particles. An equivalent noise charge model analysis ruled out the effect of the detector capacitance and the leakage current on the resolution of the detectors. Deep level transient spectroscopic studies revealed the presence of two trapping centers in each detector within the temperature scan range 240–800 K. The Z 1/2 center, a potential electron trap, was detected in both the detectors in equal concentration, which suggested that the observed difference in the energy resolution is due to the presence of the other defect, the EH 6/7 center, in the SBD. The capture cross section of the EH 6/7 center was calculated to be three orders of magnitude higher than the second defect [a carbon antisite vacancy (CAV) center] observed in the MOS detector with an activation energy of 1.10 eV, which accounted for the enhanced electronic trapping in the SBD leading to its poor energy resolution. It has been proposed that the EH 6/7 centers in the SBD have likely been reconfigured to CAV pairs during the thermal growth of the silicon dioxide layer in the MOS detector. The proposed formation mechanism of CAV, a stable qubit state for quantum information processing, addresses the outstanding questions related to the role of defect dynamics in their formation.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2025

Active deep kernel learning of molecular properties from structural embeddings

As vast databases of chemical identities become increasingly available, the challenge shifts to how we effectively explore and leverage these resources to study molecular properties. This paper presents an active learning approach for molecular discovery using deep kernel learning (DKL), demonstrated on the QM9 dataset. DKL links structural embeddings directly to properties, creating organized latent spaces that prioritize relevant property information. By iteratively recalculating embedding vectors in alignment with target properties, DKL uncovers concentrated maxima representing key molecular properties and reveals unexplored regions with potential for innovation. This approach underscores DKL’s potential in advancing molecular research and discovery.

Artificial neural networks↗

DOE OSTI2025

Mechanism of shape symmetry breaking in surfactant-mediated crystal growth

We present a dynamical model of crystal growth, in which it is possible to reliably achieve asymmetric products, beginning from symmetric initial conditions and growing within an isotropic environment. The asymmetric growth is the result of a positive feedback mechanism that amplifies the effect of thermal fluctuations in the coverage of surfactants on the growing crystalline facets. Within our simple model, we are able to understand the kinetic and thermodynamic factors involved in both the onset of symmetry breaking and the persistence of anisotropic growth. We demonstrate that the mechanism is general by studying models with increasing complexity. We argue that this mechanism of symmetry breaking underpins observations of colloidal, seed-mediated syntheses of single crystalline metal nanorods capped with strongly interacting surfactants. The parameters within our model are related to experimental observables such as the concentration, hydrophobicity, and binding strength of the surfactants, which suggests a potential route to optimize the yield of asymmetric products in colloidal nanoparticle syntheses.

Oaks-Leaf, Sam↗

DOE OSTI2022

Dynamic Earth Energy Storage: Terawatt-year, Grid-scale Energy Storage Using Planet Earth as a Thermal Battery (GeoTES): Phase I Project (Final Report)

Grid-scale energy storage has been identified by the U.S. Department of Energy’s (DOE) Energy Storage Grand Challenge as a necessary technology to support the continued build-out of intermittent renewable energy resources required to attain a carbon-free energy future. To meet this goal, the 2018 Department of Energy Research and Innovation Act mandated the creation of a comprehensive program to accelerate the development and commercialization of next-generation energy storage technologies. One of numerous energy storage technology options is the storage of excess energy as heated geothermal brine in suitable geologic formations. This concept, known as reservoir thermal energy storage (RTES), geologic thermal energy storage (GeoTES), aquifer thermal energy storage (ATES), etc., relies on the storage of thermal energy in geologic formations for recovery and use in large-scale direct use geothermal (e.g., district heating, industrial processes, etc.) and electrical power generation applications. This thermal energy is derived from excess or waste heat from any high-temperature heat source, such as concentrated solar or from conventional thermal/nuclear generation. As such, RTES can potentially play a significant role in meeting the energy storage shortfall in the coming decades. RTES can provide energy arbitrage through both the storage and production of thermal energy stored in geologic formations for direct use applications and can serve as a source of hot fluids that can be used to generate electricity to support peak demand ramping, thus easing stress on transmission and distribution. This energy storage option has geographic benefits in that energy can be stored locally or regionally depending on the various needs/loads. RTES can also be located across an enormous geographic area, without the need for a traditional hydrothermal resource but where thermal gradients and hydrogeology allow economic exploitation of subsurface heat. The work conducted for this project includes (1) a review of lessons learned from past high-temperature RTES international projects; (2) geochemical experimental investigation and numerical simulations of potential domestic sedimentary reservoirs and (3) development of a thermo-hydrological-mechanical (THM) numerical simulation tool for optimizing formation properties and design parameters to maximize thermal energy storage performance.

15 GEOTHERMAL ENERGY↗

DOE OSTI2023

Investigation of encapsulin nanocompartment systems as ascaffold for biomaterials synthesis in Rhodococcus species (DOE ECRP Annual Report 2023)

Engineered protein compartmentalization systems hold significant promise to enhance reaction efficiencies through co-localization, concentration, and sequestration of biosynthetic pathways. As such, they have the potential to enable the bioproduction of next generation bioproducts and biomaterials in genetically engineered microbes in support of DOE’s mission to build a strong bioeconomy. Among systems of particular interest are protein nanocompartment systems called encapsulins that are natively produced by a variety of bacteria including those with a high potential for bioproduction. This ECRP project is focused on understanding how encapsulins can be used to enhance the biosynthesis of next-generation biomaterials in Rhodococcus species. Specifically, we seek: (1) to probe the mechanistic basis for how these compartments are regulated, biosynthesized, and maintained, and (2) to engineer these systems to achieve new biosynthetic functions (e.g., CdS nanoparticle biosynthesis). We anticipate that this work will establish encapsulin compartmentalization systems as a means of improving yields and enabling biosynthetic routes toward new biomaterials, thus advancing the U.S. bioeconomy.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Investigation of encapsulin nanocompartment systems as a scaffold for biomaterials synthesis in Rhodococcus species

Engineered protein compartmentalization systems hold significant promise to enhance reaction efficiencies through co-localization, concentration, and sequestration of biosynthetic pathways. As such, they have the potential to enable the bioproduction of next generation bioproducts and biomaterials in genetically engineered microbes in support of DOE’s mission to build a strong bioeconomy. Among systems of particular interest are protein nanocompartment systems called encapsulins that are natively produced by a variety of bacteria including those with a high potential for bioproduction. This ECRP project is focused on understanding how encapsulins can be used to enhance the biosynthesis of next-generation biomaterials in Rhodococcusspecies. Specifically, we seek: (1) to probe the mechanistic basis for how these compartments are regulated, biosynthesized, and maintained, and (2) to engineer these systems to achieve new biosynthetic functions (e.g., CdS nanoparticle biosynthesis). We anticipate that this work will establish encapsulin compartmentalization systems as a means of improving yields and enabling biosynthetic routes toward new biomaterials, thus advancing the U.S. bioeconomy.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2025

Investigation of encapsulin nanocompartment systems as a scaffold for biomaterials synthesis in Rhodococcus species (Annual Report 2025)

Engineered protein compartmentalization systems hold significant promise to enhance reaction efficiencies through co-localization, concentration, and sequestration of biosynthetic pathways. As such, they have the potential to enable the bioproduction of next generation bioproducts and biomaterials in genetically engineered microbes in support of DOE’s mission to build a strong bioeconomy. Among systems of particular interest are protein nanocompartment systems called encapsulins that are natively produced by a variety of bacteria including those with a high potential for bioproduction. This ECRP project is focused on understanding how encapsulins can be used to enhance the biosynthesis of next-generation biomaterials in Rhodococcus species. Specifically, we seek: (1) to probe the mechanistic basis for how these compartments are regulated, biosynthesized, and maintained, and (2) to engineer these systems to achieve new biosynthetic functions (e.g., alkene, inorganic nanoparticle biosynthesis). We anticipate that this work will establish encapsulin compartmentalization systems as a means of improving yields and enabling biosynthetic routes toward new biomaterials, thus advancing the U.S. bioeconomy.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2026

Investigation of encapsulin nanocompartment systems as a scaffold for biomaterials synthesis in Rhodococcus species (Annual Report 2025)

Engineered protein compartmentalization systems hold significant promise to enhance reaction efficiencies through co-localization, concentration, and sequestration of biosynthetic pathways. As such, they have the potential to enable the bioproduction of next generation bioproducts and biomaterials in genetically engineered microbes in support of DOE’s mission to build a strong bioeconomy. Among systems of particular interest are protein nanocompartment systems called encapsulins that are natively produced by a variety of bacteria including those with a high potential for bioproduction. This ECRP project is focused on understanding how encapsulins can be used to enhance the biosynthesis of next-generation biomaterials in Rhodococcus species. Specifically, we seek: (1) to probe the mechanistic basis for how these compartments are regulated, biosynthesized, and maintained, and (2) to engineer these systems to achieve new biosynthetic functions (e.g., alkene, inorganic nanoparticle biosynthesis). We anticipate that this work will establish encapsulin compartmentalization systems as a means of improving yields and enabling biosynthetic routes toward new biomaterials, thus advancing the U.S. bioeconomy.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Geometric and Material Variability Influences Stress States Relevant to Coastal Permafrost Bluff Failure

Scientific knowledge and engineering tools for predicting coastal erosion are largely confined to temperate climate zones that are dominated by non-cohesive sediments. The pattern of erosion exhibited by the ice-bonded permafrost bluffs in Arctic Alaska, however, is not well-explained by these tools. Investigation of the oceanographic, thermal, and mechanical processes that are relevant to permafrost bluff failure along Arctic coastlines is needed. We conducted physics-based numerical simulations of mechanical response that focus on the impact of geometric and material variability on permafrost bluff stress states for a coastal setting in Arctic Alaska that is prone to toppling mode block failure. Our three-dimensional geomechanical boundary-value problems output static realizations of compressive and tensile stresses. We use these results to quantify variability in the loci of potential instability. We observe that niche dimension affects the location and magnitude of the simulated maximum tensile stress more strongly than the bluff height, ice wedge polygon size, ice wedge geometry, bulk density, Young's Modulus, and Poisson's Ratio. Our simulations indicate that variations in niche dimension can produce radically different potential failure areas and that even relatively shallow vertical cracks can concentrate displacement within ice-bonded permafrost bluffs. These findings suggest that stability assessment approaches, for which the geometry of the failure plane is delineated a priori, may not be ideal for coastlines similar to our study area and could hamper predictions of erosion rates and nearshore sediment/biogeochemical loading.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Mercury Speciation via Diffusive Gradients Thin-Films Technology

Objectives: Develop and test various diffusive gradient in thin films (DGT) samplers for mercury - SRNL is developing reactive DGTS (rDGTs). Test chemistry to differentiate methylmercury from total and/or inorganic mercury in environmental samples. Fabricate and test rDGT samplers for deployment. Deploy the rDGTs in variable settings. Mercury is a persistent-bioaccumulative-toxic environmental pollutant. Mercury exists in different species such as elemental, inorganic, and methyl. Mercury speciation determine mercury behavior and toxicity. For example, methylmercury strongly accumulates in biota such as fish resulting in potential human health impacts. DGTs are innovative samplers to measure water concentration by diffusion and capture. Types of Hg DGTs used: Total Hg, Inorganic Hg, and Methyl Hg. Deployment Sites: Upper Three Runs, Lower Three Runs, Steele Creek, East Fork Poplar Creek (SRNL Sites), Horizons Creek, NOA Creek, Bruners Creek (ORNL Sites). DGT concentration estimates closely matched alternative measurements for soluble mercury at each Oak Ridge site - DGTs did not respond to particulate mercury. DGTs provide a representative measure for biota uptake since they are left out longer which allows for an average exposure concentration. DMA-80 provided an efficient and quick analysis. Variability in site location made a difference in Hg species. DGT preparations and sampling wasn't as quick and simple as microcolumn technology. Copper reagent degraded agarose gel - more work and cleaner data are needed to assess speciation in rDGTs. Future Work: Use cross-linked polyacrylamide for the collection layer for a stronger plastic. Make a copper diffusion layer without agarose. Test copper separation in lab using realistic stream conditions such as high organic carbon.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Flammable Gas Generation and Control at the Idaho Completion Project Legacy Combustible Gas Generation - 20191

On April 11, 2018, four drums containing transuranic waste at the Idaho National Laboratory underwent over-pressurization, ejecting their lids and spreading radiological waste within a facility. An investigation has found that waste in the drums generated methane gas, which contributed to the event. Subsequent to the investigation, the potential for drums to have methane and other flammable analytes whose concentrations could approach or exceed the lower flammability limit (LFL) and the adequacy of the controls to prevent or mitigate a possible deflagration was evaluated. An extensive review of the historical records was performed to determine how many drums exceed the LFL. The historical record identified a small quantity of drums that exceeded the LFL for xylene, hydrogen, and methane. The primary codified applicable code or standard for handling drums is 29 CFR 1910.120 (j) 'Handling Drums and Containers.' It is used throughout the commercial and government sector. This code is integrated throughout the Fluor Idaho safety management programs and procedures to control the Standard Industrial Hazards (SIHs) associated with drum and container handling. Example requirements include: - Drums and containers are inspected, and their integrity assured prior to being moved. - Site operations are organized to minimize the amount of drum or container movement. - When there is a reasonable possibility of flammable atmospheres being present, material handling equipment and hand tools are of the type to prevent sources of ignition. Drums and containers under pressure, as evidenced by bulging or swelling, are not moved until the cause for excess pressure is determined and appropriate containment procedures have been implemented to protect employees from explosive relief of the drum. Drums which exceed the WIPP FGA limit have NCRs associated with them. Once a drum fails flammable gas sampling, an NCR is initiated. The NCR drives placement into NCR dense pack rows. A standing order drives placement of the FGA failures to a single planer segregation location. These drums are not allowed for further processing or shipment until the NCR has been cleared. Once in the single planer rows, follow-up FGA testing is performed by CCP. The NCR is dispositioned by follow-up sampling occurring after adequate time has been provided for the gas to diffuse through the filter assembly, or, in some cases, the drums are repackaged into additional drums to reduce the source term. To date, the ICP project has performed approximately 1.5 million drums moves without a deflagration event due to combustible gas generation. Flammable gas generation in a transuranic waste drum is not unique to the ICP but is common across the DOE complex. Based on the experience at Idaho, application of industry standards is sufficient to control the risk of drum deflagration due to drum movements. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Considerations for Regulation and Practical Implementation of Analyses of Inadvertent Human Intrusion - 20169

Recommendations from the International Commission for Radiological Protection (ICRP) and the International Atomic Energy Agency (IAEA) identify the need to consider potential inadvertent human intrusion into a near-surface radioactive waste disposal facility when developing limits for radionuclide concentrations that can be disposed. The recommendations also provide perspective on expectations for performance criteria and general assumptions for such analyses. Inadvertent human intrusion analyses are conducted to address the potential failure of institutional controls and loss of memory of a disposal facility. The analyses consider potential consequences of human actions that result in unknowingly bringing waste to the surface. Inadvertent human intrusion scenarios consider potential impacts to someone involved in an activity that actually disturbs the waste (e.g., drilling or excavation of a basement) or that exposes the person to emanations from the waste (e.g., radioactive gases) and also for the case where there may be longer term exposures to waste that has been brought to the surface. In practice, inadvertent human intrusion analyses have proven to be a critical consideration for the development of waste classification systems and for the determination of disposal requirements and limitations on wastes that can be disposed at shallow depths. The IAEA implemented a project on Human Intrusion in the context of Disposal of Radioactive waste (HIDRA) to further explore the regulatory expectations and practical implementation of analyses of potential inadvertent human intrusion. The paper begins with a discussion of international recommendations related to consideration of inadvertent human intrusion and then summarizes examples of some topical considerations related to addressing inadvertent human intrusion that are being discussed as part of the second phase of the HIDRA project. The topical considerations are planned to be addressed in a formal IAEA publication. All information in this paper simply reflects on-going project discussions and no formal recommendations are implied for these topical considerations at this time. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Investigating the Effects of Copper Impurity Deposition on the Structure and Electrochemical Behavior of Hydrogen Evolution Electrocatalyst Materials

Electrolysis of impure water (such as seawater) has recently garnered research interest as it may enable hydrogen production at reduced costs. However, the tendency of impurity ions and other species to degrade electrocatalysts and membranes within an electrolyzer is a serious challenge. Here, we investigate the effects of copper impurities of varying concentrations on the hydrogen evolution reaction (HER) using platinum electrocatalysts. A decrease of current density is observed with an increasing copper concentration. By comparing the effect of ionic impurities on current density at different concentrations, we gain insight into how impurities can interfere with the HER at different potentials. Surface characterization of the electrodes reveals differences in the morphology and extent of copper deposition on HER-active platinum vs inactive gold electrodes. This enables an improved understanding of how copper nucleates and grows on the two types of electrodes under different electrochemical conditions while also confirming deposition in low-concentration cases, as present in seawater. The results indicate that copper electrodeposition competes with the HER, and the nature of copper electrodeposition varies depending on the electrocatalytic activity of the electrode. This study provides insight toward catalyst design that can withstand the effects of impurity-induced degradation over extended use.

08 HYDROGEN↗

DOE OSTI2022

Feasibility of enhancing carbon sequestration and stock capacity in temperate and boreal European forests via changes to management regimes

Forest management practices might act as nature-based methods to remove CO 2 from the atmosphere and slow anthropogenic climate change and thus support an EU forest-based climate change mitigation strategy. However, the extent to which diversified management actions could lead to quantitatively important changes in carbon sequestration and stocking capacity at the tree level remains to be thoroughly assessed. To that end, we used a state-of-the-science bio-geochemically based forest growth model to simulate effects of multiple forest management scenarios on net primary productivity (NPP) and potential carbon woody stocks (pCWS) under twenty scenarios of climate change in a suite of observed and virtual forest stands in temperate and boreal European forests. Previous modelling experiments indicated that the capacity of forests to assimilate and store atmospheric CO 2 in woody biomass is already being attained under business-as-usual forest management practices across a range of climate change scenarios. Nevertheless, we find that on the long-term, with increasing atmospheric CO 2 concentration and warming, managed forests show both higher productivity capacity and a larger potential pool size of stored carbon than unmanaged forests as long as thinning and tree harvesting are of moderate intensity.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Manganese Oxidation States in Volcanic Soils across Annual Rainfall Gradients

Manganese (Mn) exists as Mn(II), Mn(III), or Mn(IV) in soils, and the Mn oxidation state controls the roles of Mn in numerous environmental processes. However, the variations of Mn oxidation states with climate remain unknown. Here we determined the Mn oxidation states in highly weathered bulk volcanic soils (primary minerals free) across two rainfall gradients covering mean annual precipitation (MAP) of 0.25–5 m in the Hawaiian Islands. With increasing MAP, the soil redox conditions generally shifted from oxic to suboxic and to anoxic despite fluctuating at each site; concurrently, the proportions of Mn(IV) and Mn(II) decreased and increased, respectively. Mn(III) was low at both low and high MAP, but accumulated substantially, up to 80% of total Mn, in soils with prevalent suboxic conditions at intermediate MAP. Mn(III) was likely hosted in Mn(III,IV) and iron(III) oxides or complexed with organic matter, and its distribution among these hosts varied with soil redox potentials and soil pH. Soil redox conditions and rainfall-driven leaching jointly controlled exchangeable Mn(II) in soils, with its concentration peaking at intermediate MAP. The Mn redox chemistry was at disequilibrium, with the oxidation states correlating with long-term average soil redox potentials better than with soil pH. The soil redox conditions likely fluctuated between oxic and anoxic conditions more frequently at intermediate than at low and high MAP, creating biogeochemical hot spots where Mn, Fe, and other redox-sensitive elements may be actively cycled.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Dehydration-Driven Ion Aggregation and the Onset of Gelation in ZnCl2 Solution

A minimal model of ionic aggregation in concentrated ZnCl2 is developed, guided by molecular dynamics simulations with a machine-learned potential. It explicitly incorporates solvent-site depletion, correlated chloride binding, and allows for loops within Zn–Cl clusters. Dehydration drives two coordination-controlled structural changes: a crossover at Z=2 from predominantly isolated Zn-containing species to Cl-bridged clusters and the onset of gelation near Z≈3. The model reproduces the concentration-dependent trends observed in the molecular dynamics simulations with two fitted parameters, while the cluster-size distribution at the highest concentration is consistent with three-dimensional percolation scaling over the accessible range of cluster sizes.

25 ENERGY STORAGE↗

DOE OSTI2020

Oxaliplatin–DNA Adducts as Predictive Biomarkers of FOLFOX Response in Colorectal Cancer: A Potential Treatment Optimization Strategy

FOLFOX is one of the most effective treatments for advanced colorectal cancer (CRC). However, cumulative oxaliplatin neurotoxicity often results in halting the therapy. Oxaliplatin functions predominantly via the formation of toxic covalent drug-DNA adducts. We hypothesize that oxaliplatin-DNA adduct levels formed in vivo in peripheral blood mononuclear cells (PBMC) are proportional to tumor shrinkage caused by FOLFOX therapy. We further hypothesize that adducts induced by sub-therapeutic "diagnostic microdoses" are proportional to those induced by therapeutic doses and are also predictive of response to FOLFOX therapy. These hypotheses were tested in CRC cell lines and a pilot clinical study. Four CRC cell lines were cultured with therapeutically relevant (100 µM) or diagnostic microdose (1 µM) concentrations of [ 14 C]oxaliplatin. The C-14 label enabled quantification of oxaliplatin-DNA adduct level with accelerator mass spectrometry (AMS). Oxaliplatin-DNA adduct formation was correlated with oxaliplatin cytotoxicity for each cell line as measured by the MTT viability assay. Six CRC patients received by IV a diagnostic microdose containing [ 14 C]oxaliplatin prior to treatment, as well as a second [ 14 C]oxaliplatin dose during FOLFOX chemotherapy, termed a "therapeutic dose." Oxaliplatin-DNA adduct levels from PBMC correlated significantly to mean tumor volume change of evaluable target lesions (5 of the 6 patients had measurable disease). Finally, oxaliplatin-DNA adduct levels were linearly proportional between microdose and therapeutically relevant concentrations in cell culture experiments and patient samples, as was plasma pharmacokinetics, indicating potential utility of diagnostic microdosing.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

Multi-century dynamics of the climate and carbon cycle under both high and net negative emissions scenarios

Abstract. Future climate projections from Earth system models (ESMs) typically focus on the timescale of this century. We use a set of five ESMs and one Earth system model of intermediate complexity (EMIC) to explore the dynamics of the Earth's climate and carbon cycles under contrasting emissions trajectories beyond this century to the year 2300. The trajectories include a very-high-emissions, unmitigated fossil-fuel-driven scenario, as well as a mitigation scenario that diverges from the first scenario after 2040 and features an “overshoot”, followed by a decrease in atmospheric CO2 concentrations by means of large net negative CO2 emissions. In both scenarios and for all models considered here, the terrestrial system switches from being a net sink to either a neutral state or a net source of carbon, though for different reasons and centered in different geographic regions, depending on both the model and the scenario. The ocean carbon system remains a sink, albeit weakened by carbon cycle feedbacks, in all models under the high-emissions scenario and switches from sink to source in the overshoot scenario. The global mean temperature anomaly is generally proportional to cumulative carbon emissions, with a deviation from proportionality in the overshoot scenario that is governed by the zero emissions commitment. Additionally, 23rd century warming continues after the cessation of carbon emissions in several models in the high-emissions scenario and in one model in the overshoot scenario. While ocean carbon cycle responses qualitatively agree in both globally integrated and zonal mean dynamics in both scenarios, the land models qualitatively disagree in zonal mean dynamics, in the relative roles of vegetation and soil in driving C fluxes, in the response of the sink to CO2, and in the timing of the sink–source transition, particularly in the high-emissions scenario. The lack of agreement among land models on the mechanisms and geographic patterns of carbon cycle feedbacks, alongside the potential for lagged physical climate dynamics to cause warming long after CO2 concentrations have stabilized, points to the possibility of surprises in the climate system beyond the 21st century time horizon, even under relatively mitigated global warming scenarios, which should be taken into consideration when setting global climate policy.

54 ENVIRONMENTAL SCIENCES↗