Materials capable of sustaining high radiation doses at a high temperature are required for next-generation fission and future fusion energy. To date, however, even the most promising structural materials cannot withstand the demanded radiation environment due to irreversible radiation-driven microstructure degradation. Here we report a counterintuitive strategy to achieve exceptionally high radiation tolerance at high temperatures by enabling reversible local disordering–ordering transition of the introduced superlattice nanoprecipitates in metallic materials. As particularly demonstrated in martensitic steel containing a high density of B2-ordered superlattices, no void swelling was detected even after ultrahigh-dose radiation damage at 400–600 °C. The reordering process of the low-misfit superlattices in highly supersaturated matrices occurs through the short-range reshuffling of radiation-induced point defects and excess solutes right after rapid, ballistic disordering. This dynamic process stabilizes the microstructure, continuously promotes in situ defect recombination and efficiently prevents the capillary-driven long-range diffusion process. The strategy can be readily applied into other materials and pave the pathway for developing materials with high radiation tolerance.
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Zinkle, S. J. & Busby, J. T. Structural materials for fission & fusion energy. Mater. Today 12, 12–19 (2009).
Zinkle, S. J. & Was, G. S. Materials challenges in nuclear energy. Acta Mater. 61, 735–758 (2013).
Zinkle, S. J. & Snead, L. L. Designing radiation resistance in materials for fusion energy. Ann. Rev. Mater. Res. 44, 241–267 (2014).
Kenik, E. A. & Busby, J. T. Radiation-induced degradation of stainless steel light water reactor internals. Mater. Sci. Eng. R Rep. 73, 67–83 (2012).
Busby, J. T. Economic benefits of advanced materials in nuclear power systems. J. Nucl. Mater. 392, 301–306 (2009).
Chen, T. et al. Microstructural changes and void swelling of a 12Cr ODS ferritic-martensitic alloy after high-dpa self-ion irradiation. J. Nucl. Mater. 467, 42–49 (2015).
Heald, P. T. The preferential trapping of interstitials at dislocations. Philos. Mag. J. Theor. Exp. Appl. Phys. 31, 551–558 (1975).
Gigax, J. G. et al. Radiation response of alloy T91 at damage levels up to 1000 peak dpa. J. Nucl. Mater. 482, 257–265 (2016).
Ackland, G. Controlling radiation damage. Science 327, 1587–1588 (2010).
Han, W. Z. et al. Design of radiation tolerant materials via interface engineering. Adv. Mater. 25, 6975–6979 (2013).
Field, K. G. et al. Dependence on grain boundary structure of radiation induced segregation in a 9 wt.% Cr model ferritic/martensitic steel. J. Nucl. Mater. 435, 172–180 (2013).
Chen, T. et al. Temperature dependent dispersoid stability in ion-irradiated ferritic-martensitic dual-phase oxide-dispersion-strengthened alloy: coherent interfaces vs. incoherent interfaces. Acta Mater. 116, 29–42 (2016).
Wharry, J. P., Swenson, M. J. & Yano, K. H. A review of the irradiation evolution of dispersed oxide nanoparticles in the b.c.c. Fe-Cr system: current understanding and future directions. J. Nucl. Mater. 486, 11–20 (2017).
Zinkle, S. J. et al. Development of next generation tempered and ODS reduced activation ferritic/martensitic steels for fusion energy applications. Nucl. Fusion 57, 092005 (2017).
Yamashita, S., Akasaka, N., Ukai, S. & Ohnuki, S. Microstructural development of a heavily neutron-irradiated ODS ferritic steel (MA957) at elevated temperature. J. Nucl. Mater. 367-370, 202–207 (2007).
Boothby, R. M. in Comprehensive Nuclear Materials: Radiation Efects in Nickel-based Alloys Vol. 4 (ed. Konings, R. J. M.) 123–150 (Elsevier, 2012).
Yamashita, S., Oka, K., Ohnuki, S., Akasaka, N. & Ukai, S. Phase stability of oxide dispersion-strengthened ferritic steels in neutron irradiation. J. Nucl. Mater. 307, 283–288 (2002).
Allen, T. R. et al. The stability of 9Cr-ODS oxide particles under heavy-ion irradiation. Nucl. Sci. Eng. 151, 305–312 (2005).
Aydogan, E. et al. Stability of nanosized oxides in ferrite under extremely high dose self ion irradiations. J. Nucl. Mater. 486, 86–95 (2017).
Jiang, S. et al. Ultrastrong steel via minimal lattice misfit and high-density nanoprecipitation. Nature 544, 460–464 (2017).
Chen, Y. R. Irradiation effects of HT-9 martensitic steel. Nucl. Eng. Technol. 45, 311–322 (2013).
Zinkle, S. J. & Snead, L. L. Opportunities and limitations for ion beams in radiation effects studies: bridging critical gaps between charged particle and neutron irradiations. Scr. Mater. 143, 154–160 (2018).
Certain, A., Kuchibhatla, S., Shutthanandan, V., Hoelzer, D. T. & Allen, T. R. Radiation stability of nanoclusters in nano-structured oxide dispersion strengthened (ODS) steels. J. Nucl. Mater. 434, 311–321 (2013).
Lescoat, M. L. et al. Radiation-induced Ostwald ripening in oxide dispersion strengthened ferritic steels irradiated at high ion dose. Acta Mater. 78, 328–340 (2014).
Parish, C. M., White, R. M., LeBeau, J. M. & Miller, M. K. Response of nanostructured ferritic alloys to high-dose heavy ion irradiation. J. Nucl. Mater. 445, 251–260 (2014).
Xu, Q., Watanabe, H. & Yoshida, N. Microstructural evolution in Fe–Cr–Ni alloy irradiated with Ni ion under varying temperature. J. Nucl. Mater. 233, 1057–1061 (1996).
Hunn, J. D., Lee, E. H., Byun, T. S. & Mansur, L. K. Ion-irradiation-induced hardening in Inconel 718. J. Nucl. Mater. 296, 203–209 (2001).
Russell, K. C. Phase instability under cascade damage irradiation. J. Nucl. Mater. 206, 129–138 (1993).
Robino, C. V., Cieslak, M. J., Hochanadel, P. W. & Edwards, G. R. Heat treatment of investment cast PH 13-8 Mo stainless steel: part II. Isothermal aging kinetics. Metall. Mater. Trans. A 25, 697–704 (1994).
Mirzadeh, H. & Najafizadeh, A. Aging kinetics of 17-4 PH stainless steel. Mater. Chem. Phys. 116, 119–124 (2009).
Dimmler, G., Weinert, P., Kozeschnik, E. & Cerjak, H. Quantification of the Laves phase in advanced 9–12% Cr steels using a standard SEM. Mater. Charact. 51, 341–352 (2003).
Monnet, I. et al. Microstructural investigation of the stability under irradiation of oxide dispersion strengthened ferritic steels. J. Nucl. Mater. 335, 311–321 (2004).
He, L., Tan, L., Yang, Y. & Sridharan, K. Evolution of B2 and Laves phases in a ferritic steel under Fe2+ ion irradiation at 475 °C. J. Nucl. Mater. 525, 102–110 (2019).
Ferreirós, P. A., Alonso, P. R. & Rubiolo, G. H. Coarsening process and precipitation hardening in Fe2AlV-strengthened ferritic Fe76Al12V12 alloy. Mater. Sci. Eng. A 684, 394–405 (2017).
Sencer, B. H. et al. Microstructural alteration of structural alloys by low temperature irradiation with high energy protons and spallation neutrons. in Symposium on Effects of Radiation on Materials: 20th International Symposium (eds. Rosinski, S. T., Grossbeck, M. L., Allen, T. R. & Kumar, A. S.), ASTM STP 1405, 588–611 (ASTM International, 2001).
Cabet, C., Dalle, F., Gaganidze, E., Henry, J. & Tanigawa, H. Ferritic-martensitic steels for fission and fusion applications. J. Nucl. Mater. 523, 510–537 (2019).
Yeli, G. et al. The stability of γ′ precipitates in a multi-component FeCoNiCrTi0.2 alloy under elevated-temperature irradiation. J. Nucl. Mater. 540, 152364 (2020).
Brinkman, J. A. Production of atomic displacements by high-energy particles. Am. J. Phys. 24, 246–267 (1956).
Yang, T.-n et al. The effect of injected interstitials on void formation in self-ion irradiated nickel containing concentrated solid solution alloys. J. Nucl. Mater. 488, 328–337 (2017).
Yang, T.-n et al. Influence of irradiation temperature on void swelling in NiCoFeCrMn and NiCoFeCrPd. Scr. Mater. 158, 57–61 (2019).
Zhang, Y. et al. Influence of chemical disorder on energy dissipation and defect evolution in concentrated solid solution alloys. Nat. Commun. 6, 8736 (2015).
Sniegowski, J. J. & Wolfer, W. G. On the Physical Basis for the Swelling Resistance of Ferritic Steels (The Metallurgical Society, 1984).
Little, E. A. & Stow, D. A. Void-swelling in irons and ferritic steels: II. An experimental survey of materials irradiated in a fast reactor. J. Nucl. Mater. 87, 25–39 (1979).
Garner, F. A., Toloczko, M. B. & Sencer, B. H. Comparison of swelling and irradiation creep behavior of fcc-austenitic and bcc-ferritic/martensitic alloys at high neutron exposure. J. Nucl. Mater. 276, 123–142 (2000).
Little, E. A., Bullough, R., Wood, M. H. & Marshall, W. C. On the swelling resistance of ferritic steel. Proc. R. Soc. Lond. A 372, 565–579 (1980).
Ribis, J. & Leprêtre, F. Interface roughening in irradiated oxide dispersion strengthened steels. Appl. Phys. Lett. 111, 261602 (2017).
Kashinath, A., Misra, A. & Demkowicz, M. J. Stable storage of helium in nanoscale platelets at semicoherent interfaces. Phys. Rev. Lett. 110, 086101 (2013).
Pickering, E. J. et al. High-entropy alloys for advanced nuclear applications. Entropy 23, 98 (2021).
Zhang, Z., Armstrong, D. E. J. & Grant, P. S. The effects of irradiation on CrMnFeCoNi high-entropy alloy and its derivatives. Prog. Mater. Sci. 123, 100807 (2022).
Zhang, Y., Osetsky, Y. N. & Weber, W. J. Tunable chemical disorder in concentrated alloys: defect physics and radiation performance. Chem. Rev. 122, 789–829 (2022).
Foreman, A. J. E., Von Harrach, H. S. & Saldin, D. K. The TEM contrast of faceted voids. Philos. Mag. A 45, 625–645 (1982).
Toloczko, M. B. et al. Ion-induced swelling of ODS ferritic alloy MA957 tubing to 500 dpa. J. Nucl. Mater. 453, 323–333 (2014).
Shao, L. et al. Effect of defect imbalance on void swelling distributions produced in pure iron irradiated with 3.5 MeV self-ions. J. Nucl. Mater. 453, 176–181 (2014).
Short, M. P., Gaston, D. R., Jin, M., Shao, L. & Garner, F. A. Modeling injected interstitial effects on void swelling in self-ion irradiation experiments. J. Nucl. Mater. 471, 200–207 (2016).
Doyle, P. J., Benensky, K. M. & Zinkle, S. J. Modeling the impact of radiation-enhanced diffusion on implanted ion profiles. J. Nucl. Mater. 509, 168–180 (2018).
Ziegler, J. F., Ziegler, M. D. & Biersack, J. P. SRIM—the stopping and range of ions in matter (2010). Nucl. Instrum. Methods Phys. Res. B: Beam Interact. Mater. At. 268, 1818–1823 (2010).
Stoller, R. E. et al. On the use of SRIM for computing radiation damage exposure. Nucl. Instrum. Methods Phys. Res. B: Beam Interact. Mater. At. 310, 75–80 (2013).
Agarwal, S., Lin, Y., Li, C., Stoller, R. E. & Zinkle, S. J. On the use of SRIM for calculating vacancy production: quick calculation and full-cascade options. Nucl. Instrum. Methods Phys. Res. B: Beam Interact. Mater. At. 503, 11–29 (2021).
Weber, W. J. & Zhang, Y. Predicting damage production in monoatomic and multi-elemental targets using stopping and range of ions in matter code: challenges and recommendations. Curr. Opin. Solid State Mater. Sci. 23, 100757 (2019).
Doyle, P. J., Benensky, K. M. & Zinkle, S. J. A set of MATLAB routines and associated files for prediction of radiation-enhanced diffusion in ion irradiated materials. Data Br. 21, 83–85 (2018).
We sincerely thank S. J. Zinkle, L. Shao, F. A. Garner and F. Gao for the fruitful and valuable discussions. We also thank J. Zhang, Z. J. Zhou, T. D. Shen, K. Y. Yu, Y. Liu, S. Y. Hu, P. Wang, S. D. Yao, H. H. Zhu, J. M. Zhang, Z. M. Wu, Z. Y. Hu, Y. B. Zhao, Z. F. Wu, S.K. Shen and L. Y. Hao for help in the experiments. This work was supported by the National Magnetic Confinement Fusion Energy Research Project from the Ministry of Science and Technology of China (grant nos. 2019YFE03120003 (E.F.), 2018YFE0307100 (E.F.) and 2022YEF03030000 (J.D.)), the National Natural Science Foundation of China (NSFC) (grant nos. 11921006 (E.F.), 11975034 (E.F.), 11375018 (E.F.), 51921001 (Z.L.), 51671018 (S.J.), 11790293 (Z.L.), U20B2025 (Z.L.), U21B2082 (C.X.) and 51871016 (Y.W.)) and Beijing Municipal Natural Science Foundation (grant no. 1222023 (E.F.)). E.F. acknowledges support from the Science Fund for Creative Research Groups (NSFC), the Ion Beam Materials Laboratory (IBML) at Peking University and Collaborative Innovation Center of Quantum Matter at Peking University. Z.L. and S.J. acknowledge financial support from the 111 Project (B07003 (Z.L.)), the Fundamental Research Fund for the Central Universities of China (FRF-MP_20-43Z (S.J.) and National Postdoctoral Program for Innovative Talents (BX20180035 (S.J.)).
The authors declare no competing interests.
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a, STEM micrograph. b, High-resolution HAADF-STEM micrograph of the steel specimen taken along the 001 zone axis. The contrast in the HAADF imaging originates from different atomic numbers (Z), and dark columns arise from the partitioning of Al atoms. c, Combined elemental mapping of the APT datasets. d, NPs highlighted by an isoconcentration surface encompassing regions containing more than 50 at% of Al and Ni combined.
a, SRIM simulation (using the Kinchin-Pease method56,57) showing the radiation damage (dpa) profile and injected ion distribution along the ion penetration depth for 6 MeV Au3+ with a dose of 3×1017 cm−2. Inset is the corresponding cross-sectional HAADF-STEM image of the Au ion-irradiated superlattice steel. b, Energy dispersive X-ray spectrometer (EDS) profiles along radiation depth of the samples subjected to 84, 840 and 2350 dpa at 500 °C. The error bars are the standard deviation of the mean. c, Enlarged EDS profiles’ image labeled by violet dashed rectangle. d, The temperature-dependent void denuded zone near the surface and the injected ion-affected region for the 6 MeV Au ion-irradiated superlattice steel. Safe analysis region for void swelling is shown between two regions.
Extended Data Fig. 3 Cross-sectional TEM images of the superlattice steel subjected to 2350 dpa at a, 400 °C and b, 600 °C under different objective lens (OL) focus conditions.
No voids were observed in both cases. (a1, b1) Cross-sectional TEM images showing the radiation damage along the radiation depth. The investigated layer (200 ~ 320 nm) was indicated by two vertical dashed lines. (a2-a4) Cross-sectional TEM images of the investigated layer (200 ~ 320 nm deep) of the superlattice steel irradiated at 400 °C taken at a2, underfocus, a3, in focus, and a4 overfocus conditions. (b2-b4) Cross-sectional TEM images of the investigated layer (200 ~320 nm deep) in the superlattice steel irradiated at 600 °C taken at b2, underfocus, b3, in focus, and b4, overfocus conditions. The defocus distance is ±2 μm.
Extended Data Fig. 4 Cross-sectional HAADF-STEM images of the superlattice steel irradiated with different dpa at varied temperatures.
a, 84 dpa, 400 °C. b, 84 dpa, 500 °C. c, 420 dpa, 500 °C. d, 84 dpa, 600 °C. e-f, 84 dpa, 700 °C. g, 84 dpa, 400 °C. Insets are the corresponding SAED or FFT images. h, NPs density and diameter evolution versus radiation temperature up to 84 dpa. i, NPs density and diameter evolution versus radiation damage at 500 °C. j, Composition evolution of NPs versus radiation damage at 500 °C. The error bars represent the standard deviation of the mean.
a, NP labeled by the red arrow in Fig. 2b, which is highlighted by the isoconcentration surface encompassing regions containing more than a 50 at.% combination of Al and Ni. b, Proximity histogram showing the composition change across the selected NPs, especially the Mo profile. c, The solute-enriched region labeled by the blue arrow in Fig. 2b, which is highlighted by the isoconcentration surface encompassing regions containing more than a 50 at.% combination of Al and Ni; Additionally, more than 23 at.% Al and 28 at.% Ni show an inhomogeneous distribution of Ni and Al in the solute-enriched regions. d, Proximity histogram showing the composition change across the selected solute-enriched regions, revealing the rejection of Mo atoms out of the precipitates and reformation of NPs inside the solute-enriched regions. The error bars represent the standard deviation of the mean.
Extended Data Fig. 6 Radiation-induced dissolution and thermally activated reprecipitation of NPs in the superlattice steel.
a, The number density of NPs versus radiation damage at room temperature (RT). b, Cross-sectional STEM image of the specimen subjected to 5 dpa at room temperature. The inset is the corresponding SAED pattern. c, Cross-sectional STEM image of the specimen irradiated to 5 dpa at room temperature followed by aging at 500 °C for 3 h. d, APT characterization of the superlattice steel irradiated to 5 dpa at room temperature. e, Proximity histogram showing the composition profiles across the selected nanopreccipitates shown in 40 at.% Ni+Al isosurface image (labeled by the red rectangular box). f, Proximity histogram showing the composition profiles across the selected nanoprecipitate shown in 40 at.% Ni+Al isosurface image (labeled by the blue rectangular box). The error bars are the standard deviation of the mean.
Extended Data Fig. 7 Room temperature radiation induced disordering of NPs in the superlattice steel and MEA.
a-f, APT characterization of the superlattice steel for a, As-prepared, b, 1 dpa, c, 2 dpa, and d, 5 dpa of the ion-irradiated sample followed by aging. The steel was radiated by Fe ion with doses of 1, 2 and 5 dpa at room temperature. The ion-irradiated steel with a dose of 5 dpa was aged at 500 °C for 3 h. e, The nearest neighbor distribution of Ni. f, The nearest neighbor distribution of Al. g-i. APT characterization of the designed MEA experienced 5 dpa radiation at room temperature, indicating fully dissolution of the L12-ordered phase. g, The tomographic reconstruction from one of the APT datasets, revealing complete dissolution of NPs after 5 dpa radiation at room temperature. h, The corresponding Ni elemental mapping. i, The nearest neighbor distribution of Ni, Ti and Al. The error bars are the standard deviation of the mean.
a-c, Schematic figures showing the atomic structures of a, α-iron, b, B2-Ni:(Fe,Al), and c, L21-Fe2AlV. d-f, Evolution of L21 nanoprecipitation in Fe-12Cr4Al10V0.7Nb0.01B alloy before and after ion irradiation. d, As-prepared sample, showing the L21 NPs. e, Irradiated by Au ions up to 10 dpa at 500 °C, and SAED patterns show the dissolution of L21 NPs. f, Irradiated by Au ions up to 50 dpa at 600 °C, and SAED pattern shows the dissolution of L21 NPs, accompanied with formation of voids.
Extended Data Fig. 9 Mechanical properties, STEM characterizations and dynamic evolution of NPs of the superlattice steels with different Al contents and density of NPs.
a, Nanoindentation hardness evolution of the superlattice steels with different density of NPs as a function of radiation damage at 500 °C. The value without NPs is plotted by yellow dashed line and the line width indicates the corresponding error bar. Detailed description of the NPs in the superlattice steels with different NP density is provided in Supplementary Table S3. b, Nanoindentation hardness evolution of the superlattice steels and solution-annealed steel subjected to ion irradiation at 500 °C. c-e, STEM characterization of the 2Al superlattice steel with lower NPs density before and after ion irradiation; c, As-prepared. d, 84 dpa, 500 °C. e, 840 dpa, 500 °C. No NPs were observed in the ion-irradiated samples. f, Atomic resolved cross-sectional HAADF-STEM image of the steel with low NP density (that is, the 2Al steel) after 840 dpa ion irradiation at 500 °C. The inset is the corresponding FFT image showing weak spots of B2 structure. g, Inverse FFT image showing the B2 reordered regions (several are circled). h, Vickers hardness versus aging time revealing nanoprecipitation kinetics of the superlattice steels with different Al contents.The error bars are the standard deviation of the mean.
a, SEM image of 9Cr ODS steel. b, STEM image of 9Cr ODS steel containing nanoparticles labeled by red arrows and EDS mappings of one typical nanoparticle, in which rich Y and Ti can be detected.
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Du, J., Jiang, S., Cao, P. et al. Superior radiation tolerance via reversible disordering–ordering transition of coherent superlattices. Nat. Mater. 22, 442–449 (2023). https://doi.org/10.1038/s41563-022-01260-y
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