Homogeneous and polymorphic transformations to ordered intermetallics in nanostructured Au–Cu multilayer thin films
Source abstract
Abstract
Atomic arrangements in the nanostructured grains and interfaces of thermally evaporated Au/Cu multilayer thin films on polycrystalline Si substrate have been explored through GIXRD, HRTEM, simulation, and direct structure imaging. GIXRD pattern conforms to cF4 solid solution of Au and Cu with peak broadening and shift. Comparative analysis with simulation indicated the presence of cP4, tP4, oP8, and oI40 phases in the multilayer. The Cu layer is amorphous. Localized amorphous phase forms at the Cu–Si interface due to the impingement of Cu atoms during deposition. Interfaces of Au–Cu are wavy. The Au layer is polycrystalline and columnar with some twin-like defects present in them. At the Cu–Au interface, diffusionally grown cP4, tP4, oI40, and oP8 phases could be observed. Adatom mobility, concurrent growth, and coalescence of growth islands lead to columnar growth. Ordered intermetallic phases could be related with the cF4 solid solution phase through polymorphism. The strain associated with the polymorphs and the solid solution phase is quite small. Faceted semi-coherent interfaces of the ordered phases with the solid solution phase have been resolved. The ordered phases grow into the solid solution matrix by homogeneous transformation. Structure imaging of the ordered phases indicated that most of the time a cluster of atoms is imaged in these structures. The interfaces are likely to be chemically diffused in nature. Polymorphism and homogeneous nature of the transformation at low temperature allows local transformation to ordered phases, that explain the phase field ambiguity in the binary phase diagram. Such structural details are critical in understanding the novel properties in these nanostructured alloys.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: nanoparticles nucleation surface interactions · Solidification and crystal growth phenomena · Microstructure and mechanical properties
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (70)
Show source-provided references
1. Garcia-Gonzalez M, Van Petegem S, Baluc N, Dupraz M, Honkimaki V, Lalire F, Van Swygenhoven H (2020) Influence of thermo-mechanical history on the ordering kinetics in 18 carat Au alloys. Acta Mater 191:186–197. https://doi.org/10.1016/j.actamat.2020.03.03210.1016/j.actamat.2020.03.032 ↗
2. Critchley K, Khanal BP, Górzny ML, Vigderman L, Evans SD, Zubarev ER, Kotov NA (2010) Near-bulk conductivity of gold nanowires as nanoscale interconnects and the role of atomically smooth interface. Adv Mater 22:2338–2342. https://doi.org/10.1002/adma.20100023610.1002/adma.201000236 ↗
3. Liu K, Ma M, Wu L, Valenti M, Cardenas-Morcoso D, Hofmann JP, Bisquert J, Gimenez S, Smith WA (2019) Electronic effects determine the selectivity of planar Au–Cu bimetallic thin films for electrochemical CO2 reduction. ACS Appl Mater Interfaces 11:16546–16555. https://doi.org/10.1021/acsami.9b0155310.1021/acsami.9b01553 ↗
4. Fratoddi I, Venditti I, Battocchio C, Carlini L, Amatori S, Porchia M, Tisato F, Bondino F, Magnano E, Pellei M, Santini C (2019) Highly hydrophilic gold nanoparticles as carrier for anticancer copper(I) complexes: loading and release studies for biomedical applications. Nanomaterials 9:772. https://doi.org/10.3390/nano905077210.3390/nano9050772 ↗
5. El Mel AA, Boukli-Hacene F, Molina-Luna L, Bouts N, Chauvin A, Thiry D, Gautron E, Gautier N, Tessier PY (2015) Unusual dealloying effect in gold/copper alloy thin films: the role of defects and column boundaries in the formation of nanoporous gold. ACS Appl Mater Interfaces 7:2310–2321. https://doi.org/10.1021/am506581610.1021/am5065816 ↗
6. Xing W, Kalidindi AR, Amram D, Schuh CA (2018) Solute interaction effects on grain boundary segregation in ternary alloys. Acta Mater 161:285–294. https://doi.org/10.1016/j.actamat.2018.09.00510.1016/j.actamat.2018.09.005 ↗
7. Amin KR, Kundu S, Biswas S, Roy A, Singh AK, Ravishankar N, Bid A (2016) Effect of ambient on electrical transport properties of ultra-thin Au nanowires. Appl Phys Lett 109:25310810.1063/1.4972843 ↗
8. Yan K, Yao W, Cao J, Li Y, Zhu Y, Cao L (2015) Electron migration behavior of Au/Cu multilayer films on Si substrates under UV radiation. Phys Chem Chem Phys 17:5057–5062. https://doi.org/10.1039/c4cp04124k10.1039/c4cp04124k ↗
9. Kim H, Choi C, Khamwannah J, Young Noh S, Zhang Y, Seong TY, Jin S (2013) Plasmonic Au nanoparticles on 8 nm TiO2 nanotubes for enhanced photocatalytic water splitting. J Renew Sustain Energy 5:053104. https://doi.org/10.1063/1.482117710.1063/1.4821177 ↗
10. Okamoto H, Chakrabarti DJ, Laughlin DE, Massalski TB (1987) The Au–Cu (Gold-Copper) system. Bull Alloy Ph Diagr 8:454–47310.1007/BF02893155 ↗
11. Jaumot FE, Charles SH (1954) Order-disorder in Cu–Au alloys II. The nature of the order-disorder transformation and long-range order. Acta Metall 2:63–74. https://doi.org/10.1016/0001-6160(54)90095-410.1016/0001-6160(54)90095-4 ↗
12. Golosov NS, Popov LE, Pudan LY (1973) Theory of order-disorder transformation in binary systems of the Cu–Au type-II. J Phys Chem Solids 34:1157–1163. https://doi.org/10.1016/S0022-3697(73)80205-710.1016/S0022-3697(73)80205-7 ↗
13. Howe JM, Gautam ARS, Chatterjee K, Phillipp F (2007) Atomic-level dynamic behavior of a diffuse interphase boundary in an Au–Cu alloy. Acta Mater 55:2159–2171. https://doi.org/10.1016/j.actamat.2006.11.01610.1016/j.actamat.2006.11.016 ↗
14. Guisbiers G, Mejia-Rosales S, Khanal S, Ruiz-Zepeda F, Whetten RL, José-Yacaman M (2014) Gold-copper nano-alloy, “tumbaga”, in the era of nano: phase diagram and segregation. Nano Lett 14:6718–6726. https://doi.org/10.1021/nl503584q10.1021/nl503584q ↗
15. Marcinkowski MJ, Zwell L (1963) Transmission electron microscopy study of the off-stoichiometric Cu3Au superlattices. Acta Metall 11:373–390. https://doi.org/10.1016/0001-6160(63)90162-710.1016/0001-6160(63)90162-7 ↗
16. Williams RO (1980) Long-period superlattices in the copper-gold system as two-phase mixtures. Metall Trans A 11:247–253. https://doi.org/10.1007/BF0266062910.1007/BF02660629 ↗
17. Yakel HL (1962) High-temperature X-ray diffraction study of the order-disorder transition in a Cu-32.2 atomic percent gold alloy. J Appl Phys 33:2439–2443. https://doi.org/10.1063/1.172898910.1063/1.1728989 ↗
18. Tissot P, Dallenbach R (1978) Study of order-disorder transformation of copper-gold alloys by means of differential thermal analysis. Thermochim Acta 25:143–153. https://doi.org/10.1016/0040-6031(78)85002-310.1016/0040-6031(78)85002-3 ↗
19. Kundu P, Turner S, Van Aert S, Ravishankar N, Van Tendeloo G (2014) Atomic structure of quantum gold nanowires: quantification of the lattice strain. ACS Nano 8:599–606. https://doi.org/10.1021/nn405231510.1021/nn4052315 ↗
20. Stadelmann PA (1987) EMS–a software package for electron diffraction analysis and HREM image simulation in materials science. Ultramicroscopy 21:131–145. https://doi.org/10.1016/0304-3991(87)90080-510.1016/0304-3991(87)90080-5 ↗
21. Zhang W, Brongersma SH, Richard O, Brijs B, Palmans R, Froyen L, Maex K (2004) Microstructure and resistivity characterization of CuAu I superlattice formed in Cu/Au thin films. J Vac Sci Technol B Microelectron Nanom Struct 22:2715–2718. https://doi.org/10.1116/1.181989910.1116/1.1819899 ↗
22. Czigany Z, Radrhczi G (1999) Columnar growth structure and evolution of wavy interface morphology in amorphous multilayered thin films. Thin Solid Films 343–344:5–810.1016/S0040-6090(98)01558-2 ↗
23. Spaepen F (2000) Interfaces and stresses in thin films. Acta Mater 48:31–42. https://doi.org/10.1016/S1359-6454(99)00286-410.1016/S1359-6454(99)00286-4 ↗
24. De Veirman AEM, Hakkens FJG, Dirks AG (1993) Cross-sectional transmission electron microscopy studies of metallic multilayers. Ultramicroscopy 51:306–315. https://doi.org/10.1016/0304-3991(93)90156-R10.1016/0304-3991(93)90156-R ↗
25. Brückl H, Vancea J, Lecheler R, Reiss G, Hoffmann H (1994) Growth and structure of polycrystalline Cr/Au multilayered thin films. Thin Solid Films 250:56–60. https://doi.org/10.1016/0040-6090(94)90165-110.1016/0040-6090(94)90165-1 ↗
26. Norton MG, Carter CB (1995) Moiré patterns and their application to the study of the growth of YBa2Cu3O7-δ thin films. J Mater Sci 30:381–389. https://doi.org/10.1007/BF0035440010.1007/BF00354400 ↗
27. Schneider MM, Howe JM (2017) Observation of interface dynamics and Cu island formation at a crystalline Si/liquid Al-alloy interface. Acta Mater 133:224–229. https://doi.org/10.1016/j.actamat.2017.05.02310.1016/j.actamat.2017.05.023 ↗
28. Jeon ID, Barnes MC, Kim DY, Hwang NM (2003) Origin of positive charging of nanometer-sized clusters generated during thermal evaporation of copper. J Cryst Growth 247:623–630. https://doi.org/10.1016/S0022-0248(02)02058-410.1016/S0022-0248(02)02058-4 ↗
29. Baxter CS, Stobbs WM (1985) TEM methods for the characterization of fine metal multilayers. Ultramicroscopy 16:216–226. https://doi.org/10.1016/0304-3991(85)90075-010.1016/0304-3991(85)90075-0 ↗
30. Ali M, Knowles KM, Mallinson PM, Fernie JA (2016) Interfacial reactions between sapphire and Ag–Cu–Ti-based active braze alloys. Acta Mater 103:859–869. https://doi.org/10.1016/j.actamat.2015.11.01910.1016/j.actamat.2015.11.019 ↗
31. Paulson WM, Hilliard JE (1977) Interdiffusion in composition-modulated copper-gold thin films. J Appl Phys 48:2117–2123. https://doi.org/10.1063/1.32402710.1063/1.324027 ↗
32. Jin M, Cao P, Short MP (2020) Achieving exceptional radiation tolerance with crystalline-amorphous nanocrystalline structures. Acta Mater 186:587–596. https://doi.org/10.1016/j.actamat.2019.12.05810.1016/j.actamat.2019.12.058 ↗
33. Pelaz L, Marqús LA, Barbolla J (2004) Ion-beam-induced amorphization and recrystallization in silicon. J Appl Phys 96:5947–5976. https://doi.org/10.1063/1.180848410.1063/1.1808484 ↗
34. Broddin D, Van Tendeloo G, Van Landuyt J, Amelinckx S, De Graef M (1989) The long-period antiphase-boundary-modulated structures in Cu3+xAl1−x. Philos Mag A 59:979–998. https://doi.org/10.1080/0141861890820983210.1080/01418618908209832 ↗
35. Venkateswaran SP, Nuhfer NT, De Graef M (2007) Anti-phase boundaries and magnetic domain structures in Ni2MnGa-type Heusler alloys. Acta Mater 55:2621–2636. https://doi.org/10.1016/j.actamat.2006.12.00310.1016/j.actamat.2006.12.003 ↗
36. Han K, Hirth JP, Embury JD (2001) Modeling the formation of twins and stacking faults in the Ag–Cu system. Acta Mater 49:1537–1540. https://doi.org/10.1016/S1359-6454(01)00057-X10.1016/S1359-6454(01)00057-X ↗
37. Lu Q, You Z, Huang X, Hansen N, Lu L (2017) Dependence of dislocation structure on orientation and slip systems in highly oriented nanotwinned Cu. Acta Mater 127:85–97. https://doi.org/10.1016/j.actamat.2017.01.01610.1016/j.actamat.2017.01.016 ↗
38. Xue S, Fan Z, Chen Y, Li J, Wang H, Zhang X (2015) The formation mechanisms of growth twins in polycrystalline Al with high stacking fault energy. Acta Mater 101:62–70. https://doi.org/10.1016/j.actamat.2015.08.04610.1016/j.actamat.2015.08.046 ↗
39. Yu KY, Bufford D, Chen Y, Liu Y, Wang H, Zhang X (2013) Basic criteria for formation of growth twins in high stacking fault energy metals. Appl Phys Lett 103:181903. https://doi.org/10.1063/1.482691710.1063/1.4826917 ↗
40. Chopra KL, Randlett MR (1968) Influence of deposition parameters on the coalescence stage of growth of metal films. J Appl Phys 39:1874. https://doi.org/10.1017/S174392130802721X10.1017/S174392130802721X ↗
41. Ranganathan S, Divakar R, Raghunathan VS (2001) Interface structures in nanocrystalline materials. Scr Mater 44:1169–1174. https://doi.org/10.1016/S1359-6462(01)00678-910.1016/S1359-6462(01)00678-9 ↗
42. Rodney D (2007) Activation enthalpy for kink-pair nucleation on dislocations: comparison between static and dynamic atomic-scale simulations. Phys Rev B 76:144108. https://doi.org/10.1103/PhysRevB.76.14410810.1103/PhysRevB.76.144108 ↗
43. Perez-Bergquist AG, Cerreta EK, Trujillo CP, Gray GT, Brandl C, Germann TC (2012) Transmission electron microscopy study of the role of interface structure at 1 0 0/1 1 1 boundaries in a shocked copper multicrystal. Scr Mater 67:412–415. https://doi.org/10.1016/j.scriptamat.2012.05.03510.1016/j.scriptamat.2012.05.035 ↗
44. Ågren J (2002) On the classification of phase transformations. Scr Mater 46:893–898. https://doi.org/10.1016/S1359-6462(02)00083-010.1016/S1359-6462(02)00083-0 ↗
45. Pradeepkumar MS, Pal AS, Singh A, Basu J, Ahmad MI (2020) Phase separation in wurtzite CuInxGa1−xS2 nanoparticles. J Mater Sci 55:11841–11855. https://doi.org/10.1007/s10853-020-04844-810.1007/s10853-020-04844-8 ↗
46. Singh MK, Basu J, Mukherjee B, Mandal RK (2019) Determination of symmetry breaking transitions and polymorphism in AuCu nanostructures by nano-beam electron diffraction. Mater Charact 154:437–448. https://doi.org/10.1016/j.matchar.2019.06.02610.1016/j.matchar.2019.06.026 ↗
47. Singh MK, Mukherjee B, Basu J, Mandal RK (2018) Vacancy-mediated structural changes in Au–Cu nanoparticles. Philos Mag Lett 98:97–106. https://doi.org/10.1080/09500839.2018.147725810.1080/09500839.2018.1477258 ↗
48. Singh MK, Chettri P, Basu J, Tripathi A, Mukherjee B, Tiwari A, Mandal RK (2019) Synthesis of rod-shaped Au–Cu intermetallic nanoparticles and SERS detection. Mater Lett 249:33–3610.1016/j.matlet.2019.04.065 ↗
49. Raj R, Dehm G, Scheu C, Ru M (1998) Growth and structure of internal Cu/Al2O3 and Cu/Ti/Al2O3 interfaces. Acta Metall 46:759–772
50. Rohrer GS (2005) Influence of interface anisotropy on grain growth and coarsening. Annu Rev Mater Res 35:99–126. https://doi.org/10.1146/annurev.matsci.33.041002.09465710.1146/annurev.matsci.33.041002.094657 ↗
51. Levinstein H (1992) The growth and structure of thin metallic films. J Appl Phys 306:306–315. https://doi.org/10.1063/1.169836210.1063/1.1698362 ↗
52. Malis O, Ludwig KF (1999) Kinetics of phase transitions in equiatomic CuAu. Phys Rev B 60:14675–14682. https://doi.org/10.1103/PhysRevB.60.1467510.1103/PhysRevB.60.14675 ↗
53. Beyerlein IJ, Demkowicz MJ, Misra A, Uberuaga BP (2015) Defect-interface interactions. Prog Mater Sci 74:125–210. https://doi.org/10.1016/j.pmatsci.2015.02.00110.1016/j.pmatsci.2015.02.001 ↗
54. Hirth JP, Pond RC (1996) Steps, dislocations and disconnections as interface defects relating to structure and phase transformations. Acta Mater 44:4749–4763. https://doi.org/10.1016/S1359-6454(96)00132-210.1016/S1359-6454(96)00132-2 ↗
55. Chopra KL (1969) Thin film phenomena. McGraw-Hill Book Company, New York
56. Dehm G, Nadarzinski K, Ernst F, Rühle M (1996) Quantification of irradiation damage generated during HRTEM with 1250 keV electrons. Ultramicroscopy 63:49–55. https://doi.org/10.1016/0304-3991(96)00025-310.1016/0304-3991(96)00025-3 ↗
57. Menon ESK, Huang P, Kraitchman M, Hoyt JJ, Chow P, De Fontaine D (1993) Nonlinear diffusion in Cu–Au multilayer thin films. J Appl Phys 73:142–149. https://doi.org/10.1063/1.35389110.1063/1.353891 ↗
58. Hao T, Ono M, Okayasu S, Sakai S, Narumi K, Hiraiwa Y, Naramoto H, Maeda Y (2010) RBS study of diffusion under strong centrifugal force in bimetallic Au/Cu thin films. Nucl Instrum Methods Phys Res B 268:1867–1870. https://doi.org/10.1016/j.nimb.2010.02.03010.1016/j.nimb.2010.02.030 ↗
59. Morral JE, Jin C, Engström A, Ågren J (1996) Three types of planar boundaries in multiphase diffusion couples. Scr Mater 34:1661–1666. https://doi.org/10.1016/1359-6462(96)00038-310.1016/1359-6462(96)00038-3 ↗
60. Scott RE (1960) New complex phase in the copper-gold system. J Appl Phys 31:2112–2117. https://doi.org/10.1063/1.173550910.1063/1.1735509 ↗
61. Vronka M, Straka L, De Graef M, Heczko O (2020) Antiphase boundaries, magnetic domains, and magnetic vortices in Ni–Mn–Ga single crystals. Acta Mater 184:179–186. https://doi.org/10.1016/j.actamat.2019.11.04310.1016/j.actamat.2019.11.043 ↗
62. Gu XF, Furuhara T, Chen L, Yang P (2020) Domain structures and the transitional state of ordering in long-period stacking ordered (LPSO) structures in Mg–Al–Gd alloy. Scr Mater 187:19–23. https://doi.org/10.1016/j.scriptamat.2020.05.05510.1016/j.scriptamat.2020.05.055 ↗
63. Wang B, Jesanis AT, Berry DC, Rickman JM (2013) L1 FePt: ordering, anisotropy constant and their relation to film composition. IEEE Trans Magn 49:3284–3291. https://doi.org/10.1109/TMAG.2013.224244510.1109/TMAG.2013.2242445 ↗
64. Lee SB, Rickman JM, Barmak K (2003) Phase transformation kinetics and self-patterning in misfitting thin films. Acta Mater 51:6415–6427. https://doi.org/10.1016/j.actamat.2003.08.02110.1016/j.actamat.2003.08.021 ↗
65. Hutchinson CR, Ringer SP (2000) Precipitation processes in Al–Cu–Mg alloys microalloyed with Si. Metall Mater Trans A 31:2721–2733. https://doi.org/10.1007/BF0283033110.1007/BF02830331 ↗
66. Lu S, Ågren J, Vitos L (2018) Ab initio study of energetics and structures of heterophase interfaces: from coherent to semicoherent interfaces. Acta Mater 156:20–30. https://doi.org/10.1016/j.actamat.2018.06.03010.1016/j.actamat.2018.06.030 ↗
67. Schwartz LH, Cohen JB (1965) Nature of long-range order in Cu3Au and Cu72Au28. J Appl Phys 36:598–61610.1063/1.1714037 ↗
68. Lord NW (1953) On the kinetics of the disorder-order transformation in Cu3Au. J Chem Phys 21:692–699. https://doi.org/10.1063/1.169899210.1063/1.1698992 ↗
69. Seethalekshmi S, Mangalampalli KSRN, Hareesh UNS, Ramamurty U, Varughese S (2016) Structural snapshots of metastable intermediates reveals sequential addition of growth units in the formation of an archetypal coordination complex: anisotropic layer migration and solid-state thermochromic transitions. Cryst Growth Des 16:7271–7277. https://doi.org/10.1021/acs.cgd.6b0142910.1021/acs.cgd.6b01429 ↗
70. Odqvist J, Sundman B, Ågren J (2003) A general method for calculating deviation from local equilibrium at phase interfaces. Acta Mater 51:1035–1043. https://doi.org/10.1016/S1359-6454(02)00507-410.1016/S1359-6454(02)00507-4 ↗