Ultrasonic Pulverization of an Aerosol: A Versatile Tool for the Deposition of Sol–Gel Thin Films

  • M. Langlet
Living reference work entry


Fine droplets with a narrow size distribution are generated from a liquid stream, when an ultrasonic or pneumatic spraying device is used. The liquid containing the sol–gel precursors breaks into droplets that are directed at a substrate, in some cases using a DC voltage for electrospraying. The process of spray deposition encompasses several techniques and many variables. By adjusting the variables, high quality optical films can be achieved. The advantages and disadvantages of these processes are discussed in detail.



The author is warmly grateful toward the following collaborators for their close participation in the aforementioned researches and for rereading the present chapter: M. Burgos, C. Coutier, C. Jimenez, P. Jenouvrier, P. Marage, M. Trejo Valdez, and C. Vautey.


  1. Albin DS, Risbud SH. Spray pyrolysis processing of optoelectronic materials. Adv Ceram Mater. 1987;2:243–52.CrossRefGoogle Scholar
  2. Bellessa J, Rabaste S, Plenet JC, Dumas J, Mugnier J, Marty O. Eu3+ doped microcavities fabricated by sol–gel process. Appl. Phys. Lett. 2001;79:2142–4.CrossRefGoogle Scholar
  3. Biehl S, Danzebrink R, Oliveira P, Aegerter MA. Refractive microlens fabrication by ink-jet process. J. Sol–Gel Sci. Tech. 1998;13:177–82.CrossRefGoogle Scholar
  4. Blandenet G, Court M, Lagarde Y. Thin layers deposited by the pyrosol process. Thin Solid Films. 1981;77:81–90.CrossRefGoogle Scholar
  5. Bornand V, Papet P, Philippot EA. Study of the effects of process variables on the synthesis of PZT thin films by the pyrosol process. Eur. J. Solid State. Inorg. Chem. 1998;35:607–18.CrossRefGoogle Scholar
  6. Bornand V, Huet I, Paper P. LiNbO3 thin films deposited on Si substrates: a morphological development study, Mat. Chem. Phys. 2002;77:571–7.Google Scholar
  7. Brinker CJ, Scherer GW. Sol–gel science. In: The physics and chemistry of sol–gel processing. San Diego: Academic; 1990.Google Scholar
  8. Brite-Euram project 7765, contract no. BRE2-CT94-0985, 1994–1998.Google Scholar
  9. Burgos M. PhD thesis, Grenoble. 2001.Google Scholar
  10. Chamberlin RR, Skarman JS. Chemical spray deposition process for inorganic films. J. Electrochem. Soc. 1966;113:86–9.CrossRefGoogle Scholar
  11. Chen CH, Kelder EM, Schoonman J. Unique porous LiCoO2 thin layers prepared by electrostatic spray deposition. J. Mater. Sci. 1996;31:5437–42.CrossRefGoogle Scholar
  12. Chen CH, Kelder EM, Schoonman J. Electrostatic sol-spray deposition (ESSD) and characterisation of nanostructured TiO2 thin films. Thin Solid Films. 1999a;342:35–41.CrossRefGoogle Scholar
  13. Chen KM, Sparks AW, Luan HC, Lim DR, Wada K, Kimerling LC. SiO2/TiO2 omnidirectional reflector and microcavity resonator via the sol–gel method. Appl. Phys. Lett. 1999b;75:3805–7.CrossRefGoogle Scholar
  14. Chu J, Lu J, Wu Y, Huang W, Maeda R, Itoh T, Suga T. Micro sensors and actuators array based on Pb(Zr, Ti)O3 thin film for AFM data-storage. SPIE Proc. 2001;4601:379–83.CrossRefGoogle Scholar
  15. Coutier C. PhD thesis, Grenoble. 2001.Google Scholar
  16. Coutier C, Audier M, Fick J, Rimet R, Langlet M. Aerosol–gel deposition of optically active layers in the system Er/SiO2–TiO2. Thin Solid Films. 2000;372:177–89.CrossRefGoogle Scholar
  17. Coutier C, Meffre W, Jenouvrier P, Fick J, Audier M, Rimet R, Jacquier B, Langlet M. The effects of phosphorus on the crystallisation and photoluminescence behaviour of aerosol–gel deposited SiO2–TiO2–Er2O3–P2O5 thin films. Thin Solid Films. 2001;392:40–9.CrossRefGoogle Scholar
  18. Danzebrink R, Aegerter MA. Deposition of micropatterned coating using an ink-jet technique. Thin Solid Films. 1999;351:115–8.CrossRefGoogle Scholar
  19. Danzebrink R, Aegerter MA. Deposition of optical microlens arrays by ink-jet processes. Thin Solid Films. 2001;392:223–5.CrossRefGoogle Scholar
  20. Fink-Straube C., Kalleder A., Koch T., Mennig M., Schmidt H. Method for the production of optical layers having uniform layer thickness, DE Patent 19840525 Al. 2000.Google Scholar
  21. Garcia-Hipolito M, Alvarez-Fregoso O, Martinez E, Falcony C, Aguilar-Frutis MA. Characterization of ZrO2:Mn,Cl luminescent coatings synthesized by the pyrosol technique. Opt. Mater. 2002;20:113–8.CrossRefGoogle Scholar
  22. Gershenzon EL, Eknadiosyants OK. On the mechanism of atomization of liquid in an ultrasonic fountain. Sov. Phys. Acoust. 1964;10:156–62.Google Scholar
  23. Gomez A, Tang K. Charge and fission of droplets in electrostatic sprays. Phys. Fluids. 1994;6:404–14.CrossRefGoogle Scholar
  24. Gurav A, Kodas T, Pluym T, Xiong Y. Aerosol processing of materials. Aerosol Sci. Tech. 1993;19:411–52.CrossRefGoogle Scholar
  25. Hong BS, Han JH, Kim ST, Cho YJ, Park MS, Dolukhanyan T, Sung C. Endurable water-reppelent glass for automobiles. Thin Solid Films. 1999;351:274–8.CrossRefGoogle Scholar
  26. Huffman M. Liquid source misted chemical deposition (LSMCD) – a critical review. Integr. Ferroelectr. 1995;10:39–53.CrossRefGoogle Scholar
  27. Jang GW, Chen C, Gumbs RW. Large-area electrochromic coatings. J. Electrochem. Soc. 1996;143:2591–6.CrossRefGoogle Scholar
  28. Jenouvrier P, Cela E, Coutier C, Langlet M, Rimet R, Fick J. Photoluminescence of terbium-organic complex in aerosol–gel-derived planar waveguides. Appl. Phys. B. 2001;73:463–6.CrossRefGoogle Scholar
  29. Jenouvrier P, Langlet M, Fick J. High photoluminescence in a new nano-crystalline active phase: YETO. SPIE Proc. 2002;4808:52–9.CrossRefGoogle Scholar
  30. Jenouvrier P, Langlet M, Rimet R, Fick J. Influence of crystallisation on the photoluminescence properties of Y2–xErxTi2O7 sol–gel thin films. Appl. Phys. A. 2003;77:687–92.CrossRefGoogle Scholar
  31. Jergel M, Gallardo AC, Guajardo CF, Strbik V. Tl-based superconductors for high-current, high-field applications. Supercond. Sci. Technol. 1996;9:427–46.CrossRefGoogle Scholar
  32. Jimenez C, Langlet M. Formation of TiN by nitridation of TiO2 films deposited by ultrasonically assisted sol–gel technique. Surf. Coat. Tech. 1994;68–69:249–52.CrossRefGoogle Scholar
  33. Kang YC, Park SB. Preparation of nanometre size oxide particles using filter expansion aerosol generator. J. Mater. Sci. 1996;31:2409–16.CrossRefGoogle Scholar
  34. Kang YC, Seup YS, Park SB. Preparation of YAG: europium red phosphors by spray pyrolysis using a filter-expansion aerosol generator. J. Am. Ceram. Soc. 1999;82:2056–60.CrossRefGoogle Scholar
  35. Kim HH, Kim KB. Ruthenium oxide thin film electrodes for supercapacitors. Electrochem. Solid-State Lett. 2001;4:A62–4.CrossRefGoogle Scholar
  36. Kololuoma T, Haatainen T. Plastic integrated optoelectronics. SPIE Proc. 2002;4647:52–9.CrossRefGoogle Scholar
  37. Kololuoma T, Oksanen JAI, Raerinne P, Rantala JT. Dye-doped sol–gel coatings for near-infrared laser protection. J. Mater. Res. 2001;16:2186–8.CrossRefGoogle Scholar
  38. Lang RJ. Ultrasonic atomization of liquids. J. Acoust. Soc. Am. 1962;34:6–8.CrossRefGoogle Scholar
  39. Langlet M. Optically active coatings deposited from an ultrasonically generated aerosol. Thin Solid Films. 2001;398–9:71–7.CrossRefGoogle Scholar
  40. Langlet M., Joubert J.C. Procédé sol gel de dépôt en couches minces par pulvérisation ultrasonore, FR Patent 9014312, 1990; EU Patent 0486393. 1991.Google Scholar
  41. Langlet M, Joubert JC. The pyrosol process or the pyrolysis of an aerosol. In: Chemistry of Advanced Materials. Oxford: IUPAC-Blackwell; 1992. p. 55–79.Google Scholar
  42. Langlet M, Vautey C. Influence of the deposition parameters on the characteristics of aerosol–gel deposited thin films. J. Sol–gel Sci. Tech. 1997;8:347–51.Google Scholar
  43. Langlet M, Walz D, Marage P, Joubert JC. SiO2 thin films deposited by a new sol–gel technique. J. Non-Cryst. Sol. 1992;147–8:488–92.CrossRefGoogle Scholar
  44. Langlet M, Marage P, Joubert JC. Aerosol–gel deposition of oxide films in the system SiO2–TiO2. Adv. Sci. Tech. 1995;5:267–74.Google Scholar
  45. Langlet M, Vautey C, Mazeas N. Some aspects of the aerosol–gel process. Thin Solid Films. 1997;299:25–32.CrossRefGoogle Scholar
  46. Langlet M, Burgos M, Coutier C, Jimenez C, Morant C, Manso M. Preparation of sol–gel TiO2 thin films at low temperature for AR coating applications. J. Sol–gel Sci. Tech. 2001a;22:139–50.CrossRefGoogle Scholar
  47. Langlet M, Coutier C, Fick J, Audier M, Meffre W, Jacquier B, Rimet R. Sol–gel thin film deposition and characterization of a new optically active compound: Er2Ti2O7. Opt. Mater. 2001b;16:463–73.CrossRefGoogle Scholar
  48. Langlet M, Jenouvrier P, Fick J, Rimet R. Aerosol–gel deposition of optically active thin films in the system Y2Ti2O7–Er2Ti2O7. J. Sol–gel Sci. Tech. 2003a;26:985–8.CrossRefGoogle Scholar
  49. Langlet M, Jenouvrier P, Fick J, Rimet R. Aerosol–gel deposition and spectroscopic characterization of pyrochlore films heavily doped with erbium ions. Opt. Mater. 2003b;25:141–7.CrossRefGoogle Scholar
  50. Lin Y, Wu C. The properties of antimony-doped tin oxide thin films from the sol–gel process. Surf. Coat. Tech. 1997;88:239–47.CrossRefGoogle Scholar
  51. Lu J, Chu J, Huang W, Ping Z. Preparation of thick Pb(Zr,Ti)O3 (PZT) films by electrostatic spray deposition (ESD) for applications in micro-system technology. Jpn. J. Appl. Phys. 2002;41:4317–20.CrossRefGoogle Scholar
  52. Manso M, Langlet M, Jimenez C, Martinez-Duart JM. Hydroxyapatite coatings obtained by the thermal activation of polymeric sols. Int. J. Inorg. Mater. 2001;3:1153–5.CrossRefGoogle Scholar
  53. Manso M, Martinez-Duart JM, Langlet M, Jimenez C, Herrero P, Million E. Aerosol–gel-derived microcrystalline hydroxyapatite coatings. J. Mater. Res. 2002a;17:1482–9.CrossRefGoogle Scholar
  54. Manso M, Ogueta S, Garcia P, Perez-Rigueiro J, Jimenez C, Martinez-Duart JM, Langlet M. Mechanical and in vitro testing of aerosol–gel deposited titania coatings for biocompatible applications. Biomaterials. 2002b;23:349–56.CrossRefGoogle Scholar
  55. Manso M, Ogueta S, Herrero P, Vazquez L, Langlet M, Garcia P. Biological evaluation of aerosol–gel-derived hydroxyapatite coatings with human mesenchymal stem cells. Biomaterials. 2002c;23:3985–90.CrossRefGoogle Scholar
  56. Manso M, Herrero P, Fernández M, Langlet M, Martínez-Duart JM. Textured hydroxyapatite interface onto biomedical Ti based coatings. J. Biomed. Mater. Res. A. 2003a;64:600–5.CrossRefGoogle Scholar
  57. Manso M, Langlet M, Fernández M, Vázquez L, Martinez-Duart JM. Surface and interface analysis of hydroxyapatite/TiO2 biocompatible structures. Mater. Sci. Eng. C. 2003b;23:451–4.CrossRefGoogle Scholar
  58. Marage R, Langlet M, Joubert JC. A new route for the deposition of SiO2 sol–gel coatings. Thin Solid Films. 1994a;238:218–27.CrossRefGoogle Scholar
  59. Marage P, Langlet M, Joubert JC. Understanding and improving the deposition conditions of SiO2 thin films obtained by ultrasonic sol–gel procedure. J. Sol–Gel Sci. Tech. 1994b;2:615–8.CrossRefGoogle Scholar
  60. Mennig M, Kalleder A, Jonschker G, Schmidt H. Sol–gel coatings for the substitution of fluoride or lead containing white decoration on glass. J. Non-Cryst. Sol. 1997;218:395–8.CrossRefGoogle Scholar
  61. Moon WS, Chung HJ, Park SB, Woo SI. Effect of lead acetate concentration on the droplet size in liquid source misted chemical deposition. Thin Solid Films. 2000a;358:86–9.CrossRefGoogle Scholar
  62. Moon WS, Woo SI, Park SB. preparation and characterization of lead zirconate titanate thin films by liquid source misted chemical deposition. Thin Solid Films. 2000b;359:77–81.CrossRefGoogle Scholar
  63. Morse TF, Kilian A, Reinhart L, Risen Jr W, Cipolla Jr JW. Aerosol techniques for glass formation. J. Non-Cryst. Sol. 1991;129:93–100.CrossRefGoogle Scholar
  64. Olding T, Sayer M, Barrow D. Ceramic sol–gel composite coatings for electrical insulation. Thin Solid Films. 2001;398–9:581–6.CrossRefGoogle Scholar
  65. Ortiz A, Alonso JC, Pankov V, Huanosta A, Andrade E. Characterization of amorphous aluminium oxide films prepared by the pyrosol process. Thin Solid Films. 2000;368:74–9.CrossRefGoogle Scholar
  66. Primeau N, Vautey C, Langlet M. The effect of thermal annealing on aerosol–gel deposited SiO2 films: a FTIR deconvolution study. Thin Solid Films. 1997;310:47–56.CrossRefGoogle Scholar
  67. Sauvet AL, Guindet J, Fouletier J. La0.8Sr0.2Cr0.95Ru0.05O3 (LSCRu) as a new anode material for SOFC using natural gas. Ionics. 1999;5:150–5.CrossRefGoogle Scholar
  68. Solayappan N, Derbenwick GF, McMillan LD, Paz de Araujo CA, Hayashi S, Conformal LSMCD. deposition of SrBi2(Ta1–xNbx)2O9. Integr. Ferroelectr. 1997;14:237–46.CrossRefGoogle Scholar
  69. Tokumoto MS, Smith A, Santilli CV, Pulcinelli SH, Craievich AF, Elkaim E, Traverse A, Briois V. Structural electrical and optical properties of undoped and indium doped ZnO thin films prepared by the pyrosol process at different temperatures. Thin Solid Films. 2002;416:284–93.CrossRefGoogle Scholar
  70. Tourtin F, Armand P, Ibanez A, Tourillon G, Philippot E. Gallium phosphate thin solid films: structural and chemical determination of oxygen surroundings by XANES and XPS. Thin Solid Films. 1998;322:85–92.CrossRefGoogle Scholar
  71. Trejo-Valdez M., Jenouvrier P., Fick J., Langlet M. Characterization of optically active and photocurable ORMOSIL thin films deposited using the Aerosol process. J. Mat. Sci. 2004;39:2801–2810.CrossRefGoogle Scholar
  72. Vasiliev RB, Rumyantseva MN, Ryabova LI, Akimov BA, Labeau M, Langlet M, Gaskov AM. Memory effect and its switching by electric field in solid-state gas sensors. J. Mater. Sci. Eng. B. 2000;77:106–9.CrossRefGoogle Scholar
  73. Vautey C. PhD thesis, Grenoble. 1998.Google Scholar
  74. Vautey C, Burgos M, Langlet M. Aerosol–gel deposition and low temperature post-treatment of SiO2 layers. Thin Solid Films. 1999;347:184–94.CrossRefGoogle Scholar
  75. Viguié JC, Spitz J. Chemical vapor deposition at low temperature. J. Electrochem. Soc. 1975;122:585–8.CrossRefGoogle Scholar
  76. Viitala RI, Langlet M, Simola J, Linden M, Rosenholm JB. Aerosol–gel deposition of doped titania thin films. Thin Solid Films. 2000;368:35–40.CrossRefGoogle Scholar
  77. Viitala RI, Simola J, Peltola T, Rahiala H, Langlet M, Rosenholm JB. vitro bioactivity of aerosol–gel deposited TiO2 thin coatings. J. Biomed. Mater. Res. 2001;54:109–14.CrossRefGoogle Scholar
  78. Wang J, Curtis CJ, Schulz DL, Ji-Guang Z. Spray deposited V2O3nH2O xerogel films as cathodes in rechargeable lithium batteries. Proc. Symp. Lithium Batteries (Electrochem. Soc. Proc.). 1999;98:374–82.Google Scholar
  79. Wilson S, Hawthorne HM, Yang Q, Troczynski T. Scale effects in abrasive wear of composite sol–gel alumina coated light alloys. Wear. 2001;251:1042–50.CrossRefGoogle Scholar

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© Springer International Publishing AG 2017

Authors and Affiliations

  1. 1.Grenoble INP – MinatecGrenoble Cedex 1France

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