Multiple anti-counterfeiting strategy by integrating up-conversion, down-shifting luminescence, phosphorescence and photochromism into NaYTiO4: Bi/Er phosphors

doi:10.1016/j.jmst.2022.05.030

Abstract

Abstract:

With the rapid development of science and technology, the high-security-level anti-counterfeiting technique is essential for ensuring property or information security. In this work, we prepared micron NaYTiO₄: Bi/Er (NYT: Bi/Er) phosphors with integrating up-conversion (UC) photoluminescence, down-shifting (DS) emission, phosphorescence and photochromism (PC) performances for advanced multiple anti-counterfeiting application. Owing to the abundant energy levels of Er³⁺ ions, the UC and DS luminescence behaviors are anticipated. Specifically, the yellow-green emission of Er³⁺ ions can be observed upon 980 nm excitation, and the bright green emission is demonstrated under 281 or 254 nm excitation due to the energy transitions of Er³⁺ ions and the energy transfer process from Bi³⁺ to Er³⁺ ions. Besides, the introduction of Bi³⁺ ions generates defect levels in the matrix and thus leads to phosphorescence. Furthermore, the repeatable PC performance could be triggered by the 365 nm irradiation and vanished with 450 nm illumination or thermal stimulation. To verify the practical usability of NYT: Bi/Er phosphors on anti-counterfeiting applications, some experiments are designed and successfully executed. It is believed that the NYT: Bi/Er phosphors can be a promising candidate for high-security-level multiple anti-counterfeiting.

Key words: Anti-counterfeiting, Up-conversion, Down shifting, Phosphorescence, Photochromism, NaYTiO₄, Bi/Er

Yuzhen Wang, Xuanyi Yuan, Yongge Cao, Chaoyang Ma. Multiple anti-counterfeiting strategy by integrating up-conversion, down-shifting luminescence, phosphorescence and photochromism into NaYTiO₄: Bi/Er phosphors[J]. J. Mater. Sci. Technol., 2022, 130: 219-226.

Figures/Tables 8

Fig. 1. (a) XRD patterns of NYT: 5 mol% Er doped with various concentration of Bi3+ ions (0-5.0 mol%) and enlarged view of (100) peak. (b) Rietveld refinement XRD patterns of NYT: 5 mol% Er/1 mol% Bi. (c) The crystal structure and Bi/Er ions substitution diagram in NYT host. (d) SEM image and element mappings of NYT: 1.0 mol% Bi/ 5 mol% Er. (e) XPS spectra of NYT: 1.0 mol% Bi/ 5 mol % Er in survey range and enlarged range for Bi 4d5 and Er 4p3.

Table 1. Rietveld refinement results of NYT: 1 mol% Bi (NYTB), NYT: 5 mol% Er (NYTE) and NYT: 5 mol% Er/1 mol% Bi (NYTBE).

Empty Cell	NYTB	NYTE	NYTBE
Space group	Pbcm	Pbcm	Pbcm
a (Å)	12.24276(14)	12.23716(23)	12.23737(12)
b (Å)	5.36043(15)	5.35952(14)	5.36013(12)
c (Å)	5.35595(13)	5.35479(13)	5.35457(11)
α=β=γ (degree)	90	90	90
V (Å³)	351.492(14)	351.180(14)	351.227(12)
R_wp	12.52%	10.06%	11.06%
R_p	8.52%	7.13%	7.72%
GOF	2.72	2.27	2.50

Fig. 2. Up-conversion luminescence properties of NYT: Bi/Er phosphors. (a) UC spectra and (b) relative intensity of green, red and total emission varies with different Bi3+ concentration. (c) UC luminescence at various pumping power, (d) log-log plot of pumping power vs UC intensity under 980 nm irradiation, and (e) the energy level diagrams and possible energy transition mechanism of Er3+ ions. And the insert photos are corresponding luminescence photos of NYT: Bi/Er samples under 980 nm irradiations.

Fig. 3. DS luminescence properties of NYT: Bi/Er phosphors. (a) Absorption of NYT host matrix, comparison of PL and PLE spectra of NYT: Bi, NYT: Er and NYT: Bi/Er phosphors. (b) Decay curves of Bi3+ ions emission at 470 nm of NYT: Bi samples doped with and without Er3+ ions. (c) PL spectra excited by 281 nm. (d) PLE monitored at 551 nm emission, and (e) integral emission intensity at blue, green and whole region of NYT: Er doped with different concentration of Bi3+ ions. (f) Possible energy transfer process of NYT: Bi/Er phosphors.

Fig. 4. Phosphorescence properties of NYT: Bi/Er samples. (a) Phosphorescence spectra of NYT: 1 mol% Bi/ 5 mol% Er phosphors with 254 nm irradiation for 2 min. (b) Logarithmic decay curves of various Bi ions doped NYT: 5 mol% Er, excited at 254 nm and monitored at 551 nm. (c) Normalized TL curves of samples. (d) Possible energy transfer mechanism of phosphorescence process.

Fig. 5. PC performance of NYT: Bi/Er phosphors. (a) UV-vis reflectance spectra of NYT: 1 mol% Bi/5 mol% Er samples irradiated by 365 nm with various time. (b) and (c) Bleaching by operations of heating and 450 nm irradiation, respectively. (d) O 1s XPS spectra before and after 365 nm irradiation. (e) Reflectivity modulation under alternate cycles between 365 nm irradiation and thermal stimulation. (f) Diagram of coloration and bleaching of photochromism.

Fig. 6. Schematic diagram of multimode advanced anti-counterfeiting application based on NYT: Bi/Er phosphors. Various wavelength light irradiated samples of (a) NYT: 1 mol% Bi/5 mol% Er, (b) NYT: 1 mol% Bi and NYT: 5 mol% Er. (c) Multimode advanced anti-counterfeiting experiments of NYT: Bi/Er samples by employing PC, DS, phosphorescence, and UC luminescence.

Fig. 7. Schematic diagram of advanced anti-counterfeiting application based on NYT: 1 mol% Bi/5 mol% Er and NYT: 1 mol% Bi phosphors. (a) the abridged general irradiation view of NYT: Bi and NYT: Bi/Er phosphors by various light sources. “0” shape is for NYT: Bi/Er and “1” shape is for NYT: Bi. (b-f) the corresponding luminescence photos of PC, UC, DS and phosphorescence performances, respectively.

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Multiple anti-counterfeiting strategy by integrating up-conversion, down-shifting luminescence, phosphorescence and photochromism into NaYTiO₄: Bi/Er phosphors

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