Abstract
This paper offers new insights into the physical phenomena in light emission from ZnO. The effect of the annealing atmosphere and temperature on defect-related emission in ZnO thin films prepared by the sol–gel method and nonpolar ZnO bulk substrates is investigated by photoluminescence spectroscopy, transmission electron microscopy, and DC electrical measurements. It is demonstrated that the post-annealing treatment is a powerful tool to modify intrinsic/extrinsic defects in ZnO and that the defect-related emission can be accurately tailored in a wide range from blue to red by changing the post-deposition processing parameters. Accurate tailoring of the deep-level emission wavelength in ZnO is of great importance in optoelectronics, particularly in white-light-emitting diodes, display devices, or biological labeling.

Graphical abstract
Highlights
-
New insights into the physical phenomena in light emission from ZnO were introduced.
-
Defect related emission of ZnO was accurately tailored in a wide range from blue to red.
-
The formation of willemite and its effect on the optical properties was discussed.
This is a preview of subscription content, access via your institution.






References
Djurišić AB, Ng AMC, Chen XY (2010) ZnO nanostructures for optoelectronics: material properties and device applications. Prog Quantum Electron 34:191–259
Yatskiv R, Tiagulskyi S, Grym J, Vaniš J, Bašinová N, Horak P, Torrisi A, Ceccio G, Vacik J, Vrňata M (2020) Optical and electrical characterization of CuO/ZnO heterojunctions. Thin Solid Films 693:137656
Ong CB, Ng LY, Mohammad AW (2018) A review of ZnO nanoparticles as solar photocatalysts: synthesis, mechanisms and applications. Renew Sustain Energy Rev 81:536–551
Xiong H-M (2013) ZnO nanoparticles applied to bioimaging and drug delivery. Adv Mater 25:5329–5335
Ozgur U, Alivov YI, Liu C, Teke A, Reshchikov MA, Dogan S, Avrutin V, Cho SJ, Morkoc H (2005) A comprehensive review of ZnO materials and devices. J Appl Phys 98:041301
Sekiguchi T, Ohashi N, Terada Y (1997) Effect of Hydrogenation on ZnO Luminescence. Jpn J Appl Phys 36:L289–L291
Yatskiv R, Grym J (2016) Luminescence properties of hydrothermally grown ZnO nanorods. Superlattice Microst 99:214–220
Chen C, He H, Lu Y, Wu K, Ye Z (2013) Surface passivation effect on the photoluminescence of ZnO nanorods. ACS Appl Mater Interfaces 5:6354–6359
Richters J-P, Voss T, Wischmeier L, Rückmann I, Gutowski J (2008) Influence of polymer coating on the low-temperature photoluminescence properties of ZnO nanowires. Appl Phys Lett 92:011103
Belhaj M, Dridi C, Yatskiv R, Grym J (2020) The improvement of UV photodetection based on polymer/ZnO nanorod heterojunctions. Org Electron 77:105545
Cho J, Park JH, Kim JK, Schubert EF (2017) White light-emitting diodes: History, progress, and future. Laser Photonics Rev 11:1600147
Wang Y, Zhu G, Xin S, Wang Q, Li Y, Wu Q, Wang C, Wang X, Ding X, Geng W (2015) Recent development in rare earth doped phosphors for white light emitting diodes. J Rare Earths 33:1–12
Yang Z, Gao M, Wu W, Yang X, Sun XW, Zhang J, Wang H-C, Liu R-S, Han C-Y, Yang H, Li W (2019) Recent advances in quantum dot-based light-emitting devices: challenges and possible solutions. Mater Today 24:69–93
Willander M, Nur O, Sadaf JR, Qadir MI, Zaman S, Zainelabdin A, Bano N, Hussain I (2010) Luminescence from zinc oxide nanostructures and polymers and their hybrid devices. Materials 3:2643–2667
Barnett CJ, Mourgelas V, McGettrick JD, Maffeis TGG, Barron AR, Cobley RJ (2019) The effects of vacuum annealing on the conduction characteristics of ZnO nanorods. Mater Lett 243:144–147
Zeng J-L, Zhang X-W, Yie Tan JZ, Bian J-C, Li Z, Chen Z-D, Peng R-Q, He H-Y, Wang J, Yang F (2013) Full-color photoluminescence of ZnO nanorod arrays based on annealing processes. J Lumin 135:201–205
Tsakonas C, Cranton W, Li F, Abusabee K, Flewitt A, Koutsogeorgis D, Ranson R (2013) Intrinsic photoluminescence from low temperature deposited zinc oxide thin films as a function of laser and thermal annealing. J Phys D Appl Phys 46:095305
Yatskiv R, Tiagulskyi S, Grym J, Cernohorsky O (2018) Electrical and optical properties of rectifying ZnO homojunctions fabricated by wet chemistry methods. Phys Status Solidi A 215:1700592
Meyer BK, Alves H, Hofmann DM, Kriegseis W, Forster D, Bertram F, Christen J, Hoffmann A, Strassburg M, Dworzak M, Haboeck U, Rodina AV (2004) Bound exciton and donor-acceptor pair recombinations in ZnO. Phys Status Solidi B-Basic Solid State Phys 241:231–260
Schirra M, Schneider R, Reiser A, Prinz GM, Feneberg M, Biskupek J, Kaiser U, Krill CE, Sauer R, Thonke K (2007) Acceptor-related luminescence at 3.314eV in zinc oxide confined to crystallographic line defects. Phys B: Condens Matter 401-402:362–365
Frodason YK, Johansen KM, Galeckas A, Vines L (2019) Broad luminescence from donor-complexed LiZn and NaZn acceptors in ZnO. Phys Rev B 100:184102
Fang Z, Wang Y, Xu D, Tan Y, Liu X (2004) Blue luminescent center in ZnO films deposited on silicon substrates. Optical Mater 26:239–242
Sekiguchi T, Ohashi N, Terada Y (1997) Effect of hydrogenation on ZnO luminescence. Jpn J Appl Phys 36:L289–L291
Alvi NH, ul Hasan K, Nur O, Willander M (2011) The origin of the red emission in n-ZnO nanotubes/p-GaN white light emitting diodes. Nanoscale Res Lett 6:130
Thompson CV (2000) Structure evolution during processing of polycrystalline films. Annu Rev Mater Sci 30:159–190
Guillemin S, Consonni V, Masenelli B, Bremond G (2013) Extended-defect-related photoluminescence line at 3.33 eV in nanostructured ZnO thin films. Appl Phys Express 6:111101
Yuk JM, Shin JW, Lee JY, Son DI, Jung JH, Kim TW, Kim JY, Choi WK (2007) Effect of thermal annealing on the formation of preferential c-axis orientation and an interfacial layer for ZnO thin films grown on an n-Si (001) substrate. J Korean Phy Soc 50:608–611
Xu X, Guo C-x, Qi Z, Liu H, Xu J, Shi C, Chong C, Huang W, Zhou Y, Xu C-m (2002) Annealing effect for surface morphology and luminescence of ZnO film on silicon. Chem Phys Lett 364:57–63
Guillemin S, Sarigiannidou E, Appert E, Donatini F, Renou G, Bremond G, Consonni V (2015) Spontaneous shape transition of thin films into ZnO nanowires with high structural and optical quality. Nanoscale 7:16994–17003
Xie Q, Zhan P, Wang W, Li Z, Zhang Z (2015) Enhanced ultraviolet and visible photoluminescence of ZnO/Zn2SiO4/SiO2/Si multilayer structure. J Alloy Compd 642:131–135
Allen MW, Swartz CH, Myers TH, Veal TD, McConville CF, Durbin SM (2010) Bulk transport measurements in ZnO: the effect of surface electron layers. Phys Rev B 81:075211
Natsume Y, Sakata H (2000) Zinc oxide films prepared by sol-gel spin-coating. Thin Solid Films 372:30–36
Fay S, Steinhauser J, Nicolay S, Ballif C (2010) Polycrystalline ZnO: B grown by LPCVD as TCO for thin film silicon solar cells. Thin Solid Films 518:2961–2966
Seto JYW (1975) Electrical properties of polycrystalline silicon films. J Appl Phys 46:5247–5254
Fang ZB, Yan ZJ, Tan YS, Liu XQ, Wang YY (2005) Influence of post-annealing treatment on the structure properties of ZnO films. Appl Surf Sci 241:303–308
Allen MW, Heinhold R, Miller P, Henseler MJH, Mendelsberg RJ, Durbin SM, Reeves RJ (2013) Polarity effects in the optical properties of hydrothermal ZnO. Appl Phys Lett 103:231109
Janotti A, Van de Walle CG (2009) Fundamentals of zinc oxide as a semiconductor. Rep Prog Phys 72:126501
Garces NY, Wang L, Bai L, Giles NC, Halliburton LE, Cantwell G (2002) Role of copper in the green luminescence from ZnO crystals. Appl Phys Lett 81:622–624
Johansen KM, Haug H, Lund E, Monakhov EV, Svensson BG (2010) Thermal stability of the OH–Li complex in hydro-thermally grown single crystalline ZnO. Appl Phys Lett 97:211907
Funding
This work was supported by the Czech Science Foundation, Project No. 20-24366S.
Author information
Authors and Affiliations
Contributions
Conceptualization: RY and JG; writing original draft preparation: RY and JG; thin film preparation: NB and OC; optical characterization: RY; electrical characterization: ST; TEM characterization: SK and JV; visualization: RY and SK; project administration: RY; funding acquisition: RY and JG. All authors have read and agreed to the published version of the manuscript.
Corresponding author
Ethics declarations
Conflict of interest
The authors declare no competing interests.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Rights and permissions
About this article
Cite this article
Yatskiv, R., Grym, J., Kučerová, Š. et al. Tunable visible emission in nanostructured thin films and bulk ZnO. J Sol-Gel Sci Technol 102, 447–453 (2022). https://doi.org/10.1007/s10971-022-05779-z
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10971-022-05779-z
Keywords
- Zinc oxide
- Photoluminescence
- Electrical properties
- Annealing