DataVXJournal of Materials ResearchPaper
journal article·2025-01-14Open access

Probing rapid solidification pathways in refractory complex concentrated alloys via multimodal synchrotron X-ray imaging and melt pool-scale simulation

Dillon K. Jobes, Yuanren Liu, Lucero Lopez, Seunghee Oh, Ashley Bucsek, Daniel Rubio-Ejchel, Christopher Tandoc, Yong-Jie Hu, Jerard V. Gordon

Journal of Materials Research· Volume 40· Issue 1
Publisher pageOpen full text
Source abstract

Abstract

Abstract Refractory complex concentrated alloys (RCCAs) show potential as the next-generation structural materials due to their superior strength in extreme environments. However, RCCAs processed by metal additive manufacturing (AM) typically suffer from process-related challenges surrounding laser material interaction defects and microstructure control. Multimodal in situ techniques (synchrotron X-ray imaging and diffraction and infrared imaging) and melt pool-level simulations were employed to understand rapid solidification pathways in two representative RCCAs: (i) multi-phase BCC + HCP Ti0.4Zr0.4Nb0.1Ta0.1 and (ii) single-phase BCC Ti0.486V0.375Cr0.111Ta0.028. As expected, laser material interaction defects followed similar systematic trends in process parameter space for both alloys. Additionally, both alloys formed a single-phase (BCC) microstructure after rapid solidification processing. However, significant differences in microstructure selection between these alloys were discovered, where Ti0.4Zr0.4Nb0.1Ta0.1 showed a mixture of equiaxed and columnar grains, while Ti0.486V0.375Cr0.111Ta0.028 was dominated by columnar growth. These behaviors were well described by the influence of undercooling effects on columnar-to-equiaxed transition (CET). Distinct microstructure formation in each alloy was verified through CET predictions via analytical melt pool simulations, which showed a ~ 5 × increase degrees in undercooling for Ti0.4Zr0.4Nb0.1Ta0.1 compared to Ti0.486V0.375Cr0.111Ta0.028. Overall, these results show that microstructure control based on modulating the freezing range must be balanced with process considerations which resist defect formation, such as solidification crack formation in RCCAs. Graphical abstract
Source: crossref · Quality: baseline

Research context

Metals & alloysCeramics & glassesMaterials processing

OpenAlex topics: Additive Manufacturing Materials and Processes · High Entropy Alloys Studies · Aluminum Alloy Microstructure Properties

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

References (60)

Show source-provided references
1. O.N. Senkov, D.B. Miracle, K.J. Chaput, J.P. Couzinie, Development and exploration of refractory high entropy alloys—a review. J. Mater. Res. 33, 3092–3128 (2018). https://doi.org/10.1557/jmr.2018.15310.1557/jmr.2018.153 ↗
2. O.N. Senkov, G.B. Wilks, J.M. Scott, D.B. Miracle, Mechanical properties of Nb25Mo25Ta25W25 and V20Nb20Mo20Ta20W20 refractory high entropy alloys. Intermetallics (Barking) 19, 698–706 (2011). https://doi.org/10.1016/J.INTERMET.2011.01.00410.1016/J.INTERMET.2011.01.004 ↗
3. S. Mooraj, G. Kim, X. Fan, S. Samuha, Y. Xie, T. Li, J.S. Tiley, Y. Chen, D. Yu, K. An, P. Hosemann, P.K. Liaw, W. Chen, W. Chen, Additive manufacturing of defect-free TiZrNbTa refractory high-entropy alloy with enhanced elastic isotropy via in-situ alloying of elemental powders. Commun Mater (2024). https://doi.org/10.1038/s43246-024-00452-010.1038/s43246-024-00452-0 ↗
4. A. Ostovari Moghaddam, N.A. Shaburova, M.N. Samodurova, A. Abdollahzadeh, E.A. Trofimov, Additive manufacturing of high entropy alloys: a practical review. J. Mater. Sci. Technol. 77, 131–162 (2021). https://doi.org/10.1016/j.jmst.2020.11.02910.1016/j.jmst.2020.11.029 ↗
5. Y. He, M. Zhong, N. Jones, J. Beuth, B. Webler, The columnar-to-equiaxed transition in melt pools during laser powder bed fusion of M2 steel. Metall. Mater. Trans. A Phys. Metall. Mater. Sci. 52, 4206–4221 (2021). https://doi.org/10.1007/S11661-021-06380-9/FIGURES/1110.1007/S11661-021-06380-9/FIGURES/11 ↗
6. M.A. Melia, S.R. Whetten, R. Puckett, M. Jones, M.J. Heiden, N. Argibay, A.B. Kustas, High-throughput additive manufacturing and characterization of refractory high entropy alloys. Appl. Mater. Today 19, 100560 (2020). https://doi.org/10.1016/J.APMT.2020.10056010.1016/J.APMT.2020.100560 ↗
7. C. Zhao, B. Shi, S. Chen, D. Du, T. Sun, B.J. Simonds, K. Fezzaa, A.D. Rollett, Laser melting modes in metal powder bed fusion additive manufacturing. Rev. Mod. Phys. (2022). https://doi.org/10.1103/RevModPhys.94.04500210.1103/RevModPhys.94.045002 ↗
8. D.H. Cook, P. Kumar, M.I. Payne, C.H. Belcher, P. Borges, W. Wang, F. Walsh, Z. Li, A. Devaraj, M. Zhang, M. Asta, A.M. Minor, E.J. Lavernia, D. Apelian, R.O. Ritchie, Kink bands promote exceptional fracture resistance in a NbTaTiHf refractory medium-entropy alloy. Science 384, 178–184 (2024). https://doi.org/10.1126/SCIENCE.ADN2428/SUPPL_FILE/SCIENCE.ADN2428_SM.PDF10.1126/SCIENCE.ADN2428/SUPPL_FILE/SCIENCE.ADN2428_SM.PDF ↗
9. S.A. Oh, R.E. Lim, J.W. Aroh, A.C. Chuang, B.J. Gould, B. Amin-Ahmadi, J.V. Bernier, T. Sun, P.C. Pistorius, R.M. Suter, A.D. Rollett, High speed synchrotron X-ray diffraction experiments resolve microstructure and phase transformation in laser processed Ti-6Al-4V. Mater Res Lett 9, 429–436 (2021). https://doi.org/10.1080/21663831.2021.196653710.1080/21663831.2021.1966537 ↗
10. S.Y. Chen, Y. Tong, K.K. Tseng, J.W. Yeh, J.D. Poplawsky, J.G. Wen, M.C. Gao, G. Kim, W. Chen, Y. Ren, R. Feng, W.D. Li, P.K. Liaw, Phase transformations of HfNbTaTiZr high-entropy alloy at intermediate temperatures. Scr. Mater. 158, 50–56 (2019). https://doi.org/10.1016/j.scriptamat.2018.08.03210.1016/j.scriptamat.2018.08.032 ↗
11. B. Luís Moreira Ribeiro, In-situ alloying by direct energy deposition for high-throughput screening of RCCA/RHEAs compositions (2023)
12. A.F. Andreoli, R.G. Mendes, V.T. Witusiewicz, O. Shuleshova, M.A. van Huis, K. Nielsch, I. Kaban, Phase constitution and microstructure of the NbTiVZr refractory high-entropy alloy solidified upon different processing. Acta Mater. 221, 117416 (2021). https://doi.org/10.1016/J.ACTAMAT.2021.11741610.1016/J.ACTAMAT.2021.117416 ↗
13. J.O. Andersson, T. Helander, L. Höglund, P. Shi, B. Sundman, Thermo-Calc & DICTRA, computational tools for materials science. Calphad 26, 273–312 (2002). https://doi.org/10.1016/S0364-5916(02)00037-810.1016/S0364-5916(02)00037-8 ↗
14. Y.J. Hu, A. Sundar, S. Ogata, L. Qi, Screening of generalized stacking fault energies, surface energies and intrinsic ductile potency of refractory multicomponent alloys. Acta Mater. (2021). https://doi.org/10.1016/j.actamat.2021.11680010.1016/j.actamat.2021.116800 ↗
15. D. Jobes, D. Rubio-Ejchel, L. Lopez, W. Jenkins, A. Sundar, C. Tandoc, J. Hochhalter, A. Misra, L. Qi, Y.-J. Hu, J. Gordon, Computationally guided alloy design and microstructure-property relationships for non-equiatomic Ti-Zr-Nb-Ta-V-Cr alloys with tensile ductility made by laser powder bed fusion. Under Review (n.d.).
16. D. Rosenthal, The theory of moving sources of heat and its application to metal treatments. J. Fluids Eng. 68, 849–865 (1946). https://doi.org/10.1115/1.401862410.1115/1.4018624 ↗
17. P. Promoppatum, S.C. Yao, P.C. Pistorius, A.D. Rollett, A comprehensive comparison of the analytical and numerical prediction of the thermal history and solidification microstructure of Inconel 718 products made by laser powder-bed fusion. Engineering 3, 685–694 (2017). https://doi.org/10.1016/J.ENG.2017.05.02310.1016/J.ENG.2017.05.023 ↗
18. M. Tang, P.C. Pistorius, J.L. Beuth, Prediction of lack-of-fusion porosity for powder bed fusion. Addit. Manuf. 14, 39–48 (2017). https://doi.org/10.1016/j.addma.2016.12.00110.1016/j.addma.2016.12.001 ↗
19. J. Kim, A. Wakai, A. Moridi, Materials and manufacturing renaissance: additive manufacturing of high-entropy alloys (2020). https://doi.org/10.1557/jmr.2020.14010.1557/jmr.2020.140 ↗
20. D. Dobranich, R. Dykhuizen, Scoping thermal calculations of the LENS process (Sandia National Laboratories Internal Report, 1998)
21. Z. Xiang, M. Yin, G. Dong, X. Mei, G. Yin, Modeling of the thermal physical process and study on the reliability of linear energy density for selective laser melting. Results Phys 9, 939–946 (2018). https://doi.org/10.1016/J.RINP.2018.03.04710.1016/J.RINP.2018.03.047 ↗
22. Z. Wu, G. Tang, S.J. Clark, A. Meshkov, S. Roychowdhury, B. Gould, V. Ostroverkhov, T. Adcock, S.J. Duclos, K. Fezzaa, C. Immer, A.D. Rollett, High frequency beam oscillation keyhole dynamics in laser melting revealed by in-situ x-ray imaging. Commun Mater. 4, 1–10 (2023). https://doi.org/10.1038/s43246-023-00332-z10.1038/s43246-023-00332-z ↗
23. N.P. Calta, V. Thampy, D.R.C. Lee, A.A. Martin, R. Ganeriwala, J. Wang, P.J. Depond, T.T. Roehling, A.Y. Fong, A.M. Kiss, C.J. Tassone, K.H. Stone, J. Nelson Weker, M.F. Toney, A.W. Van Buuren, M.J. Matthews, Cooling dynamics of two titanium alloys during laser powder bed fusion probed with in situ X-ray imaging and diffraction. Mater. Des. 195, 108987 (2020). https://doi.org/10.1016/J.MATDES.2020.10898710.1016/J.MATDES.2020.108987 ↗
24. C. Zhao, N.D. Parab, X. Li, K. Fezzaa, W. Tan, A.D. Rollett, T. Sun, Critical instability at moving keyhole tip generates porosity in laser melting (n.d.). https://www.science.org
25. R. Jiang, Z. Ren, J. Aroh, A. Mostafaei, B. Gould, T. Sun, A.D. Rollett, Quantifying equiaxed vs epitaxial solidification in laser melting of CMSX-4 single crystal superalloy. Metall. Mater. Trans. A Phys. Metall. Mater. Sci. 54, 808–822 (2023). https://doi.org/10.1007/s11661-022-06929-210.1007/s11661-022-06929-2 ↗
26. Y. Lian, Z. Gan, C. Yu, D. Kats, W.K. Liu, G.J. Wagner, A cellular automaton finite volume method for microstructure evolution during additive manufacturing. Mater. Des. 169, 107672 (2019). https://doi.org/10.1016/J.MATDES.2019.10767210.1016/J.MATDES.2019.107672 ↗
27. C. Zhao, K. Fezzaa, R.W. Cunningham, H. Wen, F. De Carlo, L. Chen, A.D. Rollett, T. Sun, Real-time monitoring of laser powder bed fusion process using high-speed X-ray imaging and diffraction. Sci. Rep. (2017). https://doi.org/10.1038/s41598-017-03761-210.1038/s41598-017-03761-2 ↗
28. C. Jasien, A. Saville, C.G. Becker, J. Klemm-Toole, K. Fezzaa, T. Sun, T. Pollock, A.J. Clarke, In situ X-ray radiography and computational modeling to predict grain morphology in β-titanium during simulated additive manufacturing. Metals 12, 1217 (2022). https://doi.org/10.3390/MET1207121710.3390/MET12071217 ↗
29. I. Weiss, S.L. Semiatin, Thermomechanical processing of beta titanium alloys—an overview. Mater. Sci. Eng. A 243, 46–65 (1998). https://doi.org/10.1016/S0921-5093(97)00783-110.1016/S0921-5093(97)00783-1 ↗
30. S. Huang, R.L. Narayan, J.H.K. Tan, S.L. Sing, W.Y. Yeong, Resolving the porosity-unmelted inclusion dilemma during in-situ alloying of Ti34Nb via laser powder bed fusion. Acta Mater. 204, 116522 (2021). https://doi.org/10.1016/J.ACTAMAT.2020.11652210.1016/J.ACTAMAT.2020.116522 ↗
31. B. Schuh, B. Völker, J. Todt, N. Schell, L. Perrière, J. Li, J.P. Couzinié, A. Hohenwarter, Thermodynamic instability of a nanocrystalline, single-phase TiZrNbHfTa alloy and its impact on the mechanical properties. Acta Mater. 142, 201–212 (2018). https://doi.org/10.1016/J.ACTAMAT.2017.09.03510.1016/J.ACTAMAT.2017.09.035 ↗
32. N.D. Stepanov, N.Y. Yurchenko, S.V. Zherebtsov, M.A. Tikhonovsky, G.A. Salishchev, Aging behavior of the HfNbTaTiZr high entropy alloy (2017). https://doi.org/10.1016/j.matlet.2017.09.09410.1016/j.matlet.2017.09.094 ↗
33. T. Li, S. Wang, W. Fan, Y. Lu, T. Wang, T. Li, P.K. Liaw, CALPHAD-aided design for superior thermal stability and mechanical behavior in a TiZrHfNb refractory high-entropy alloy. Acta Mater. 246, 118728 (2023). https://doi.org/10.1016/J.ACTAMAT.2023.11872810.1016/J.ACTAMAT.2023.118728 ↗
34. H.H. König, N.H. Pettersson, A. Durga, S. Van Petegem, D. Grolimund, A.C. Chuang, Q. Guo, L. Chen, C. Oikonomou, F. Zhang, G. Lindwall, Solidification modes during additive manufacturing of steel revealed by high-speed X-ray diffraction. Acta Mater. 246, 118713 (2023). https://doi.org/10.1016/j.actamat.2023.11871310.1016/j.actamat.2023.118713 ↗
35. S.S. Babu, J.W. Elmer, J.M. Vitek, S.A. David, Time-resolved X-ray diffraction investigation of primary weld solidification in Fe-C-Al-Mn steel welds. Acta Mater. 50, 4763–4781 (2002). https://doi.org/10.1016/S1359-6454(02)00317-810.1016/S1359-6454(02)00317-8 ↗
36. R.W. Armstrong, Engineering science aspects of the Hall-Petch relation. Acta Mech. 225, 1013–1028 (2014). https://doi.org/10.1007/s00707-013-1048-210.1007/s00707-013-1048-2 ↗
37. J.V. Gordon, S.P. Narra, R.W. Cunningham, H. Liu, H. Chen, R.M. Suter, J.L. Beuth, A.D. Rollett, Defect structure process maps for laser powder bed fusion additive manufacturing. Addit. Manuf. 36, 101552 (2020). https://doi.org/10.1016/J.ADDMA.2020.10155210.1016/J.ADDMA.2020.101552 ↗
38. T. Mukherjee, J.W. Elmer, H.L. Wei, T.J. Lienert, W. Zhang, S. Kou, T. DebRoy, Control of grain structure, phases, and defects in additive manufacturing of high-performance metallic components. Prog. Mater. Sci. 138, 101153 (2023). https://doi.org/10.1016/J.PMATSCI.2023.10115310.1016/J.PMATSCI.2023.101153 ↗
39. A.T. Polonsky, W.C. Lenthe, M.P. Echlin, V. Livescu, G.T. Gray, T.M. Pollock, Solidification-driven orientation gradients in additively manufactured stainless steel. Acta Mater. 183, 249–260 (2020). https://doi.org/10.1016/J.ACTAMAT.2019.10.04710.1016/J.ACTAMAT.2019.10.047 ↗
40. A.T. Polonsky, N. Raghavan, M.L.P. Echlin, M.M. Kirka, R.R. Dehoff, T.M. Pollock, 3D Characterization of the columnar-to-equiaxed transition in additively manufactured Inconel 718. Miner Metals Mater Ser (2014). https://doi.org/10.1007/978-3-030-51834-9_97/FIGURES/810.1007/978-3-030-51834-9_97/FIGURES/8 ↗
41. M.S.K.K.Y. Nartu, B.A. Welk, S.A. Mantri, N.L. Taylor, G.B. Viswanathan, N.B. Dahotre, R. Banerjee, H.L. Fraser, Underlying factors determining grain morphologies in high-strength titanium alloys processed by additive manufacturing. Nat. Commun. 14, 1–6 (2023). https://doi.org/10.1038/s41467-023-38885-910.1038/s41467-023-38885-9 ↗
42. M. Gäumann, C. Bezençon, P. Canalis, W. Kurz, Single-crystal laser deposition of superalloys: processing–microstructure maps. Acta Mater. 49, 1051–1062 (2001). https://doi.org/10.1016/S1359-6454(00)00367-010.1016/S1359-6454(00)00367-0 ↗
43. J.D. Hunt, Steady state columnar and equiaxed growth of dendrites and eutectic. Mater. Sci. Eng. 65, 75–83 (1984). https://doi.org/10.1016/0025-5416(84)90201-510.1016/0025-5416(84)90201-5 ↗
44. M. Haines, A. Plotkowski, C.L. Frederick, E.J. Schwalbach, S.S. Babu, A sensitivity analysis of the columnar-to-equiaxed transition for Ni-based superalloys in electron beam additive manufacturing. Comput. Mater. Sci. 155, 340–349 (2018). https://doi.org/10.1016/J.COMMATSCI.2018.08.06410.1016/J.COMMATSCI.2018.08.064 ↗
45. D.A. Porter, K.E. Easterling, M.Y. Sherif, Phase Transformations in Metals and Alloys, 3rd edn. (CPC Press, 2009)
46. B. Dovgyy, M. Simonelli, M.S. Pham, Alloy design against the solidification cracking in fusion additive manufacturing: an application to a FeCrAl alloy. Mater Res Lett 9, 350–357 (2021). https://doi.org/10.1080/21663831.2021.192294510.1080/21663831.2021.1922945 ↗
47. G. Tang, B.J. Gould, A. Ngowe, A.D. Rollett, An updated index including toughness for hot-cracking susceptibility. Metall. Mater. Trans. A Phys. Metall. Mater. Sci. 53, 1486–1498 (2022). https://doi.org/10.1007/s11661-022-06612-610.1007/s11661-022-06612-6 ↗
48. J.H. Martin, B.D. Yahata, J.M. Hundley, J.A. Mayer, T.A. Schaedler, T.M. Pollock, 3D printing of high-strength aluminium alloys. Nature 549, 365–369 (2017). https://doi.org/10.1038/nature2389410.1038/nature23894 ↗
49. G. Dai, Z. Sun, Y. Li, J. Jain, A. Bhowmik, J. Shinjo, J. Lu, C. Panwisawas, Grain refinement and columnar-to-equiaxed transition of Ti6Al4V during additive manufacturing via different laser oscillations. Int. J. Mach. Tools Manuf 189, 104031 (2023). https://doi.org/10.1016/J.IJMACHTOOLS.2023.10403110.1016/J.IJMACHTOOLS.2023.104031 ↗
50. L. Zhu, Q. Zhang, Z. Chen, C. Wei, G.M. Cai, L. Jiang, Z. Jin, J.C. Zhao, Measurement of interdiffusion and impurity diffusion coefficients in the bcc phase of the Ti–X (X = Cr, Hf, Mo, Nb, V, Zr) binary systems using diffusion multiples. J. Mater. Sci. 52, 3255–3268 (2017). https://doi.org/10.1007/S10853-016-0614-0/FIGURES/1410.1007/S10853-016-0614-0/FIGURES/14 ↗
51. K. Wang, X. Liu, T. Liu, C. He, J. Liu, Investigation on diffusion kinetics of Ti-X binary systems at 1300–1500 °C. J. Market. Res. 25, 1684–1695 (2023). https://doi.org/10.1016/J.JMRT.2023.06.05410.1016/J.JMRT.2023.06.054 ↗
52. Y. Gu, X. He, D. Han, On the phase-field modeling of rapid solidification. Comput. Mater. Sci. 199, 110812 (2021). https://doi.org/10.1016/J.COMMATSCI.2021.11081210.1016/J.COMMATSCI.2021.110812 ↗
53. J. Gockel, J. Beuth, K. Taminger, Integrated control of solidification microstructure and melt pool dimensions in electron beam wire feed additive manufacturing of Ti-6Al-4V. Addit. Manuf. 1–4, 119–126 (2014). https://doi.org/10.1016/J.ADDMA.2014.09.00410.1016/J.ADDMA.2014.09.004 ↗
54. A.T. Polonsky, N. Raghavan, M.P. Echlin, M.M. Kirka, R.R. Dehoff, T.M. Pollock, Scan strategies in EBM-printed IN718 and the physics of bulk 3D microstructure development. Mater Charact 190, 112043 (2022). https://doi.org/10.1016/J.MATCHAR.2022.11204310.1016/J.MATCHAR.2022.112043 ↗
55. N. Kouraytem, P.J. Chiang, R. Jiang, C. Kantzos, J. Pauza, R. Cunningham, Z. Wu, G. Tang, N. Parab, C. Zhao, K. Fezzaa, T. Sun, A.D. Rollett, Solidification crack propagation and morphology dependence on processing parameters in AA6061 from ultra-high-speed x-ray visualization. Addit. Manuf. 42, 101959 (2021). https://doi.org/10.1016/J.ADDMA.2021.10195910.1016/J.ADDMA.2021.101959 ↗
56. R. Cunningham, C. Zhao, N. Parab, C. Kantzos, J. Pauza, K. Fezzaa, T. Sun, A.D. Rollett, Keyhole threshold and morphology in laser melting revealed by ultrahigh-speed x-ray imaging, 2019. https://www.science.org.10.1126/science.aav4687 ↗
57. B. Gould, S. Wolff, N. Parab, C. Zhao, M.C. Lorenzo-Martin, K. Fezzaa, A. Greco, T. Sun, In situ analysis of laser powder bed fusion using simultaneous high-speed infrared and x-ray imaging. JOM 73, 201–211 (2021). https://doi.org/10.1007/S11837-020-04291-5/FIGURES/810.1007/S11837-020-04291-5/FIGURES/8 ↗
58. J.V. Bernier, R.M. Suter, A.D. Rollett, J.D. Almer, High-energy X-ray diffraction microscopy in materials science (2020). https://doi.org/10.1146/annurev-matsci-07061610.1146/annurev-matsci-070616 ↗
59. R.M. Digilov, Solid–liquid interfacial tension in metals: correlation with the melting point. Physica B Condens Matter 352, 53–60 (2004). https://doi.org/10.1016/J.PHYSB.2004.06.05410.1016/J.PHYSB.2004.06.054 ↗
60. D.J.S. Ferreira, B.N. Bezerra, M.N. Collyer, A. Garcia, I.L. Ferreira, The use of computational thermodynamics for the determination of surface tension and Gibbs-Thomson coefficient of multicomponent alloys. Continuum Mech. Thermodyn. 30, 1145–1154 (2018). https://doi.org/10.1007/S00161-018-0670-6/METRICS10.1007/S00161-018-0670-6/METRICS ↗