journal article·2011-11

Mechanism of film growth of pulsed electrodeposition of nanocrystalline copper in presence of thiourea

K. Shravan Kumar, Krishanu Biswas, R. Balasubramaniam

Journal of Nanoparticle Research· Volume 13· Issue 11
Publisher page

Abstract

This article reports the effect of addition of small amount of thiourea on mechanism of film growth, levelling and grain refinement of pulsed electrodeposition of nanocrystalline copper on stainless steel substrate using simple aqueous acidic copper sulphate solution prepared from 0.25 M CuSO4·5H2O and 0.5 M H2SO4. The amount of thiourea used in the electrolyte is 0 and 36 mg/l. The results indicate the change in morphology of the deposits with addition of thiourea leading to dendrite free copper deposits. The growth mechanism of the copper deposition is found to change from Volmer–Weber type to Frank-Vander Merwe type making the deposits smoother when deposited with thiourea addition. A small amount (36 mg/l) of thiourea addition leads to decrease in the average grain size of copper from 1160 nm to 14 nm. The results clearly reveal the formation of nanocrystalline copper by addition of thiourea with three orders of magnitude reduction in grain size as compared to the sample deposited without thiourea. Preferential segregation of sulphur (present in thiourea) along the grain boundaries of nanocrystalline copper is shown by energy filter imaging using ultra high resolution transmission electron microscope (TEM), thereby restricting the growth of copper grains during pulsed electrodeposition.
Source: openaire · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Electrodeposition and Electroless Coatings · Corrosion Behavior and Inhibition · Copper Interconnects and Reliability

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

References (21)

Show source-provided references
1. Alodan M, Smyrl W (1998) Effect of thiourea on copper dissolution and deposition. Electrochim Acta 44:299–30910.1016/S0013-4686(98)00060-7 ↗
2. Bolzan AE, Haseeb ASMA, Schilardi PL, Piatti RCV, Salvarezza RC, Arvia AJ (2001a) Anodisation of copper in thiourea- and formamidine disulphide-containing acid solution. Part I. Identification of products and reaction pathway. J Electroanal Chem 500:533–54210.1016/S0022-0728(00)00217-5 ↗
3. Bolzan AE, Wakenge IB, Piatti RCV, Salvarezza RC, Arvia AJ (2001b) The behavior of copper anodes in aqueous thiourea-containing sulphuric acid solutions. Open circuit potentials and electrochemical kinetics. J Electroanal Chem 501:241–25210.1016/S0022-0728(00)00535-0 ↗
4. Bonou L, Eyraud M, Denoyel R, Massiani Y (2002) Influence of additives on Cu electrodeposition mechanisms in acid solution: direct current study supported by non-electrochemical measurements. Electrochim Acta 47:4139–414810.1016/S0013-4686(02)00356-0 ↗
5. Braun AE (1999) Copper electroplating enters mainstream processing. Semicond Int 22:58–66
6. Fabricius G, Kontturi K, Sundholm G (1996) Influence of thiourea and thiourea ageing on the electrodeposition of copper from acid sulfate solutions studied by the ring-disc technique. J Appl Electrochem 26:1179–118310.1007/BF00243743 ↗
7. Grubac Z, Metikos-Hukovic M (2007) Nucleation of copper on an assembly of carbon microelectrodes. Mater Lett 61:794–79810.1016/j.matlet.2006.05.062 ↗
8. Hu C-C, Wu C-M (2003) Effects of deposition modes on the microstructure of copper deposits from an acidic sulfate bath. Surf Coat Tech 176:75–8310.1016/S0257-8972(03)00004-5 ↗
9. Huang L, Lee E-S, Kim K-B (2005) Electrodeposition of monodisperse copper nanoparticles on highly oriented pyrolytic graphite electrode with modulation potential method. Colloids Surf A 262:125–13110.1016/j.colsurfa.2005.03.023 ↗
10. Kang MS, Kim S-K, Kim K, Kim JJ (2008) The influence of thiourea on copper electrodeposition: adsorbate identification and effect on electrochemical nucleation. Thin Solid Films 516:3761–376610.1016/j.tsf.2007.06.069 ↗
11. Koch CC (2002) Nanostructured materials: processing, properties and applications. William Andrew Publishing, New York
12. Kruglikov SS, Kudriavtsev NT, Vorobiova GF, Antonov AYA (1965) On the mechanism of leveling by addition agents in electrodeposition of metals. Electrochim Acta 10:253–26110.1016/0013-4686(65)87023-2 ↗
13. Magali Q, Fabrice L, Laurence R, Jean-Yves H, Patrick D (2010) Adsorption of thiourea on polycrystalline platinum: Influence on electrodeposition of copper. Surf Coat Tech 204:3108–311710.1016/j.surfcoat.2010.01.025 ↗
14. Natter H, Hempelmann R (2003) Tailor-made nanomaterials designed by electrochemical methods. Electrochim Acta 49:51–6110.1016/j.electacta.2003.04.004 ↗
15. Ohring M (2002) Materials science of thin films, 2nd edn. Academic Press, San Diego
16. Paunovic Milan (2006) Fundamentals of electrochemical deposition, 2nd edn. Wiley, New York10.1002/0470009403 ↗
17. Plieth W (1992) Additives in the electrocrystallization process. Electrochim Acta 37:2115–212110.1016/0013-4686(92)85101-P ↗
18. San Martin V, Sanllorente S, Palmero S (1998) Optimization of influent factors on nucleation process of copper in solutions containing thiourea using an experimental design. Electrochim Acta 44:579–58510.1016/S0013-4686(98)00188-1 ↗
19. Suarez DF, Olson FA (1992) Nodulation of electrodeposited copper in the presence of thiourea. J Appl Electrochem 22:1002–101010.1007/BF01029577 ↗
20. Tantavichet N, Pritzker MD (2005) Effect of plating mode, thiourea and chloride on the morphology of copper deposits produced in acidic sulphate solutions. Electrochim Acta 50:1849–186110.1016/j.electacta.2004.08.045 ↗
21. Upadhyay DN, Yegnaraman V (2000) Effect of thiourea and substituted thioureas on copper underpotential deposition on gold. Mater Chem Phy 62:247–25310.1016/S0254-0584(99)00185-6 ↗