journal article·2024-09-12Open access

Accelerating multiscale electronic stopping power predictions with time-dependent density functional theory and machine learning

Logan Ward, Ben Blaiszik, Cheng-Wei Lee, Troy Martin, Ian Foster, André Schleife

npj Computational Materials· Volume 10· Issue 1

Abstract

Knowing the rate at which particle radiation releases energy in a material, the “stopping power,” is key to designing nuclear reactors, medical treatments, semiconductor and quantum materials, and many other technologies. While the nuclear contribution to stopping power, i.e., elastic scattering between atoms, is well understood in the literature, the route for gathering data on the electronic contribution has for decades remained costly and reliant on many simplifying assumptions, including that materials are isotropic. We establish a method that combines time-dependent density functional theory (TDDFT) and machine learning to reduce the time to assess new materials to hours on a supercomputer and provide valuable data on how atomic details influence electronic stopping. Our approach uses TDDFT to compute the electronic stopping from first principles in several directions and then machine learning to interpolate to other directions at a cost of 10 million times fewer core-hours. We demonstrate the combined approach in a study of proton irradiation in aluminum and employ it to predict how the depth of maximum energy deposition, the “Bragg Peak,” varies depending on the incident angle—a quantity otherwise inaccessible to modelers and far outside the scales of quantum mechanical simulations. The lack of any experimental information requirement makes our method applicable to most materials, and its speed makes it a prime candidate for enabling quantum-to-continuum models of radiation damage. The prospect of reusing valuable TDDFT data for training the model makes our approach appealing for applications in the age of materials data science.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Machine Learning in Materials Science · Molecular Junctions and Nanostructures · Advanced Memory and Neural Computing

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (67)

Show source-provided references
1. Bragg, W. H. & Kleeman, R. On the α particles of radium, and their loss of range in passing through various atoms and molecules. Lond. Edinb. Dublin Philos. Mag. J. Sci. 10, 318–340 (1905).10.1080/14786440509463378 ↗
2. Bohr, N. On the theory of the decrease of velocity of moving electrified particles on passing through matter. Lond. Edinb. Dublin Philos. Mag. J. Sci. 25, 10–31 (1913).10.1080/14786440108634305 ↗
3. Ziegler, J. F., Ziegler, M. D. & Biersack, J. P. SRIM—the stopping and range of ions in matter (2010). Nucl. Instrum. Methods Phys. Res. Sect. B 268, 1818–1823 (2010).10.1016/j.nimb.2010.02.091 ↗
4. Stoller, R. E. et al. On the use of SRIM for computing radiation damage exposure. Nucl. Instrum. Methods Phys. Res. Sect. B 310, 75–80 (2013).10.1016/j.nimb.2013.05.008 ↗
5. Berger, M. ESTAR, PSTAR, and ASTAR: Computer Programs For Calculating Stopping-power and Range Tables for Electrons, Protons, and Helium Ions. NIST Interagency/Internal Report (NISTIR) (National Institute of Standards and Technology, Gaithersburg, MD, 1992).
6. Paul, H. & Schinner, A. Empirical stopping power tables for ions from 3Li to 18Ar and from 0.001 to 1000 MeV/nucleon in solids and gases. At. Data Nucl. Data Tables 85, 377–452 (2003).10.1016/j.adt.2003.08.003 ↗
7. Schinner, A. & Sigmund, P. Expanded pass stopping code. Nucl. Instrum. Methods Phys. Res. Sect. B 460, 19–26 (2019).10.1016/j.nimb.2018.10.047 ↗
8. Schiwietz, G. & Grande, P. Stopping of protons—improved accuracy of the UCA model. Nucl. Instrum. Methods Phys. Res. Sect. B 273, 1–5 (2012).10.1016/j.nimb.2011.07.023 ↗
9. Wittmaack, K. Misconceptions impairing the validity of the stopping power tables in the SRIM library and suggestions for doing better in the future. Nucl. Instrum. Methods Phys. Res. Sect. B 380, 57–70 (2016).10.1016/j.nimb.2016.04.057 ↗
10. Kang, K. et al. Pushing the frontiers of modeling excited electronic states and dynamics to accelerate materials engineering and design. Comput. Mater. Sci. 160, 207–216 (2019).10.1016/j.commatsci.2019.01.004 ↗
11. Guinan, M. & Kinney, J. Molecular dynamic calculations of energetic displacement cascades. J. Nucl. Mater. 104, 1319–1323 (1981).10.1016/0022-3115(82)90782-6 ↗
12. Gross, E. K. U. & Kohn, W. Time-dependent density-functional theory. Adv. Quantum Chem. 21, 287–323 (1990).
13. Correa, A. A. Calculating electronic stopping power in materials from first principles. Comput. Mater. Sci. 150, 291–303 (2018).10.1016/j.commatsci.2018.03.064 ↗
14. Lee, C.-W., Stewart, J. A., Dingreville, R., Foiles, S. M. & Schleife, A. Multiscale simulations of electron and ion dynamics in self-irradiated silicon. Phys. Rev. B 102, 024107 (2020).10.1103/PhysRevB.102.024107 ↗
15. Mishin, Y. Machine-learning interatomic potentials for materials science. Acta Mater. 214, 116980 (2021).10.1016/j.actamat.2021.116980 ↗
16. van der Giessen, E. et al. Roadmap on multiscale materials modeling. Model. Simul. Mater. Sci. Eng. 28, 043001 (2020).10.1088/1361-651X/ab7150 ↗
17. Maulik, R., Egele, R., Lusch, B. & Balaprakash, P. Recurrent neural network architecture search for geophysical emulation. In SC20: International Conference for High Performance Computing, Networking, Storage and Analysis (Cuicchi C, Qualters I. & Kramer W) (IEEE, 2020).10.1109/SC41405.2020.00012 ↗
18. Rasp, S., Pritchard, M. S. & Gentine, P. Deep learning to represent subgrid processes in climate models. Proc. Natl Acad. Sci. USA 115, 9684–9689 (2018).10.1073/pnas.1810286115 ↗
19. Roberts, M. et al. Common pitfalls and recommendations for using machine learning to detect and prognosticate for COVID-19 using chest radiographs and CT scans. Nat. Mach. Intell. 3, 199–217 (2021).10.1038/s42256-021-00307-0 ↗
20. Guo, X. et al. Development of an electronic stopping power model based on deep learning and its application in ion range prediction. Chin. Phys. B 31, 073402 (2022).10.1088/1674-1056/ac4e0c ↗
21. Anderson, B., Hy, T.-S. & Kondor, R. Cormorant: covariant molecular neural networks. In 33rd International Conference on Neural Information Processing Systems (eds Wallach, H. et al.) 14537–14546 (Curran Associates Inc., Red Hook, NY, USA, 2019).
22. Rupp, M. Machine learning for quantum mechanics in a nutshell. Int. J. Quantum Chem. 115, 1058–1073 (2015).10.1002/qua.24954 ↗
23. Schleife, A., Kanai, Y. & Correa, A. A. Accurate atomistic first-principles calculations of electronic stopping. Phys. Rev. B 91, 014306 (2015).10.1103/PhysRevB.91.014306 ↗
24. Schleife, A., Kanai, Y. & Correa, A. A. Accurate Atomistic First-principles Calculations of Electronic Stopping (Materials Data Facility, 2023).
25. Blaiszik, B. et al. The Materials Data Facility: data services to advance materials science research. J. Mater. 68, 2045–2052 (2016).
26. Jarrin, T., Richard, N., Teunissen, J., Da Pieve, F. & Hémeryck, A. Integration of electronic effects into molecular dynamics simulations of collision cascades in silicon from first-principles calculations. Phys. Rev. B 104, 195203 (2021).10.1103/PhysRevB.104.195203 ↗
27. Jain, A., Persson, K. A. & Ceder, G. Research update: the Materials Genome Initiative: data sharing and the impact of collaborative ab initio databases. APL Mater. 4, 053102 (2016).10.1063/1.4944683 ↗
28. Himanen, L., Geurts, A., Foster, A. S. & Rinke, P. Data-driven materials science: status, challenges, and perspectives. Adv. Sci. 6, 1900808 (2019).10.1002/advs.201900808 ↗
29. Suhr, B., Dungl, J. & Stocker, A. Search, reuse and sharing of research data in materials science and engineering—a qualitative interview study. PLoS ONE 15, e0239216 (2020).10.1371/journal.pone.0239216 ↗
30. Brinson, L. C. et al. Community action on FAIR data will fuel a revolution in materials research. MRS Bull. 49, 12–16 (2024).10.1557/s43577-023-00498-4 ↗
31. Schleife, A., Draeger, E. W., Kanai, Y. & Correa, A. A. Plane-wave pseudopotential implementation of explicit integrators for time-dependent Kohn–Sham equations in large-scale simulations. J. Chem. Phys. 137, 22A546 (2012).10.1063/1.4758792 ↗
32. Draeger, E. W. et al. Massively parallel first-principles simulation of electron dynamics in materials. J. Parallel Distr. Com. 106, 205–214 (2017).10.1016/j.jpdc.2017.02.005 ↗
33. Marx, D. & Jurg, H. Ab Initio Molecular Dynamics: Basic Theory and Advanced Methods (Cambridge University Press, 2009).10.1017/CBO9780511609633 ↗
34. Westermayr, J. & Marquetand, P. Machine learning for electronically excited states of molecules. Chem. Rev. 121, 9873–9926 (2020).10.1021/acs.chemrev.0c00749 ↗
35. Lindhard, J. & Winther, A. Stopping power of electron gas and equipartition rule. Mat. Fys. Medd. Dan. Vid. Selsk. 34, 24 (1964).
36. Firsov, O. B. A qualitative interpretation of the mean electron excitation energy in atomic collisions. J. Exp. Theor. Phys. 36, 1076 (1959).
37. Faber, F., Lindmaa, A., von Lilienfeld, O. A. & Armiento, R. Crystal structure representations for machine learning models of formation energies. Int. J. Quantum Chem. 115, 1094–1101 (2015).10.1002/qua.24917 ↗
38. Ewald, P. P. Die berechnung optischer und elektrostatischer gitterpotentiale. Ann. Phys. 369, 253–287 (1921).10.1002/andp.19213690304 ↗
39. Botu, V., Batra, R., Chapman, J. & Ramprasad, R. Machine learning force fields: construction, validation, and outlook. J. Phys. Chem. C 121, 511–522 (2017).10.1021/acs.jpcc.6b10908 ↗
40. Ward, L. et al. Software and Datasets for “Accelerating Electronic Stopping Power Predictions by 10 Million Times With a Combination of Time-dependent Density Functional Theory and Machine Learning" (Materials Data Facility, 2023).10.1038/s41524-024-01374-8 ↗
41. Kononov, A., Hentschel, T. W., Hansen, S. B. & Baczewski, A. D. Trajectory sampling and finite-size effects in first-principles stopping power calculations. npj Comput Mater 9, 205 (2023).10.1038/s41524-023-01157-7 ↗
42. Sillanpää, J., Nordlund, K. & Keinonen, J. Electronic stopping of Si from a three-dimensional charge distribution. Phys. Rev. B 62, 3109–3116 (2000).10.1103/PhysRevB.62.3109 ↗
43. Gygi, F. Architecture of Qbox: a scalable first-principles molecular dynamics code. IBM J. Res. Dev. 52, 137–144 (2008).10.1147/rd.521.0137 ↗
44. Piessens, R., de Doncker-Kapenga, E., Überhuber, C. W. & Kahaner, D. K. Quadpack (Springer, Berlin, Heidelberg, 1983).10.1007/978-3-642-61786-7 ↗
45. Quashie, E. E., Saha, B. C. & Correa, A. A. Electronic band structure effects in the stopping of protons in copper. Phys. Rev. B 94, 155403 (2016).10.1103/PhysRevB.94.155403 ↗
46. Yao, Y., Yost, D. C. & Kanai, Y. k-shell core-electron excitations in electronic stopping of protons in water from first principles. Phys. Rev. Lett. 123, 066401 (2019).10.1103/PhysRevLett.123.066401 ↗
47. Ullah, R., Artacho, E. & Correa, A. A. Core electrons in the electronic stopping of heavy ions. Phys. Rev. Lett. 121, 116401 (2018).10.1103/PhysRevLett.121.116401 ↗
48. Clevert, D.-A., Unterthiner, T. & Hochreiter, S. Fast and accurate deep network learning by exponential linear units (ELUs). In Proc. 4th International Conference on Learning Representations (eds Bengio Y. & LeCun Y.) (2015).
49. Krasheninnikov, A. V. & Nordlund, K. Ion and electron irradiation-induced effects in nanostructured materials. J. Appl. Phys. 107, 071301 (2010).10.1063/1.3318261 ↗
50. Haume, K. et al. Gold nanoparticles for cancer radiotherapy: a review. Cancer Nanotechnol. 7, 8 (2016).10.1186/s12645-016-0021-x ↗
51. Lee, C.-W. & Schleife, A. Hot-electron-mediated ion diffusion in semiconductors for ion-beam nanostructuring. Nano Lett. 19, 3939–3947 (2019).10.1021/acs.nanolett.9b01214 ↗
52. Wolfowicz, G. et al. Quantum guidelines for solid-state spin defects. Nat. Rev. Mater. 6, 906–925 (2021).10.1038/s41578-021-00306-y ↗
53. Ortiz, C., Souidi, A., Becquart, C., Domain, C. & Hou, M. Recent radiation damage studies and developments of the Marlowe code. Radiat. Eff. Defects Solids 169, 592–602 (2014).10.1080/10420150.2014.920018 ↗
54. Posselt, M. Crystal-trim and its application to investigations on channeling effects during ion implantation. Radiat. Eff. Defects Solids null, 87–119 (1994).10.1080/10420159408219774 ↗
55. Hinks, J. A. et al. Effects of crystallographic and geometric orientation on ion beam sputtering of gold nanorods. Sci. Rep. 8, 512 (2018).10.1038/s41598-017-17424-9 ↗
56. Sand, A. E., Ullah, R. & Correa, A. A. Heavy ion ranges from first-principles electron dynamics. npj Comput. Mater. 5, 43 (2019).10.1038/s41524-019-0180-5 ↗
57. Averback, R. & de la Rubia, T. D. Displacement damage in irradiated metals and semiconductors. In Solid State Physics Vol. 51 (eds Ehrenreich, H., Spaepen, F.) 281–402 (Academic Press, 1998).10.1016/S0081-1947(08)60193-9 ↗
58. Andrade, X. et al. Inq, a modern GPU-accelerated computational framework for (time-dependent) density functional theory. J. Chem. Theory Comput. 17, 7447–7467 (2021).10.1021/acs.jctc.1c00562 ↗
59. Pruneda, J. M., Sánchez-Portal, D., Arnau, A., Juaristi, J. I. & Artacho, E. Electronic stopping power in LiF from first principles. Phys. Rev. Lett. 99, 235501 (2007).10.1103/PhysRevLett.99.235501 ↗
60. Larsen, A. H. et al. The atomic simulation environment—a Python library for working with atoms. J. Phys.: Condens. Matter 29, 273002 (2017).
61. Ward, L. et al. Matminer: an open source toolkit for materials data mining. Comput. Mater. Sci. 152, 60–69 (2018).10.1016/j.commatsci.2018.05.018 ↗
62. Ong, S. P. et al. Python Materials Genomics (pymatgen): a robust, open-source Python library for materials analysis. Comput. Mater. Sci. 68, 314–319 (2013).10.1016/j.commatsci.2012.10.028 ↗
63. Pedregosa, F. et al. Scikit-learn: machine learning in Python. J. Mach. Learn. Res. 12, 2825–2830 (2011).
64. Abadi, M. et al. TensorFlow: Large-scale Machine Learning on Heterogeneous Systems. Software available from tensorflow.org (2015).
65. Babuji, Y. et al. Parsl: pervasive parallel programming in Python. In 28th International Symposium on High-Performance Parallel and Distributed Computing (eds Weissman J. et al.) 25–36 (Association for Computing Machinery, 2019).10.1145/3307681.3325400 ↗
66. Dormand, J. & Prince, P. A family of embedded Runge–Kutta formulae. J. Comput. Appl. Math. 6, 19–26 (1980).10.1016/0771-050X(80)90013-3 ↗
67. Schleife, A., Ward, L., Blaiszik, B. & Foster, I. Time-dependent Density Functional Theory Calculations of Proton Radiation in Aluminum (Materials Data Facility, 2023).