Enhancement Luminescence and Applications of Rare Earth Fluoride

doi:10.7536/PC190330

Rare earth fluoride upconversion nanomaterials have immense potential applications for biological imaging and photothermal therapy, biosensing, solar cell and anti-counterfeiting technology, due to its high chemical stability, large anti-stokes shifts, no photobleaching, long fluorescence life, narrow emission band and deep penetration, which is a promising fluorescent material. However,such materials are limited in practical application due to their low upconversion luminescence efficiency and small absorption cross-section of activator. Based on the above problems, upconversion luminescence enhancement of rare earth doped fluoride materials such as ion co-doping, core shell structure, surface plasmon coupling, photonic crystal, broadband sensitization and thermal effect are expounded herein, and the mechanisms of enhancement of upconversion luminescence are analyzed. In addition, the research status in the fields of biological imaging and photothermal therapy, biosensing, solar cell and anti-counterfeiting technology is elaborated. Moreover, the limitations and development directions for future are also prospected.

Key words: rare earth fluoride, upconversion luminescence, luminescence enhancment, biological application

Fig. 1 Schematic diagram of rare earth doped upconversion nanomaterials

Fig. 2 The changes of the doping of a host atom with a dopant of varied size:crystal lattice contraction(left) and expansion(right)[1]

Table 1 Ion-induced upconversion enhancement

Upconversion materials	Synthesis method	Enhancement factors	ref
NaYF₄: Yb³⁺/Er³⁺/10%Sc³⁺	Hydrothermal	5	21
NaYF₄: Yb³⁺/Er³⁺/1.57%Ti⁴⁺	Hydrothermal	6(521 nm)	22
NaYF₄: Yb³⁺/Er³⁺/15%Cr³⁺	Hydrothermal	16(G), 7(R)	23
LiYF₄: Yb³⁺/Er³⁺/10%Mn²⁺	Thermal decomposition	15(G), 22(R)	24
NaGdF₄: Yb³⁺/Er³⁺/30%Fe³⁺	Hydrothermal	34(G), 30(R)	25
NaYF₄: Yb³⁺/Er³⁺/15%Co²⁺	Thermal decomposition	114(G), 84(R)	26
LiYF₄: Yb³⁺/Er³⁺/10%Cd²⁺	Thermal decomposition	2.2(G)	27
NaYF₄: Yb³⁺/Er³⁺/20%Ni²⁺	Hydrothermal	32.8(G), 20.99(R)	28
NaGdF₄: Yb³⁺/Er³⁺/13.5%Mg²⁺	Solvothermal	9(R), 6(G)	29
KMnF₃: Yb³⁺/Er³⁺/30%Mg²⁺	Solvothermal	20.8(R)	30
NaYF₄: Yb³⁺/Er³⁺/60%Cu²⁺	Hydrothermal	37(G), 25(R)	31
NaYF₄: Yb³⁺/Er³⁺/5%Zn²⁺	Hydrothermal	<2	32
KLaF₄:Yb³⁺/Er³⁺/10%Al³⁺	Hydrothermal	5.9(G), 7.3(R)	33
NaGdF₄: Yb³⁺/Er³⁺/25%Bi³⁺	Hydrothermal	60(802 nm), 160(B)	34

Table 1 Ion-induced upconversion enhancement

Upconversion materials	Synthesis method	Enhancement factors	ref
NaYF₄: Yb³⁺/Er³⁺/10%Sc³⁺	Hydrothermal	5	21
NaYF₄: Yb³⁺/Er³⁺/1.57%Ti⁴⁺	Hydrothermal	6(521 nm)	22
NaYF₄: Yb³⁺/Er³⁺/15%Cr³⁺	Hydrothermal	16(G), 7(R)	23
LiYF₄: Yb³⁺/Er³⁺/10%Mn²⁺	Thermal decomposition	15(G), 22(R)	24
NaGdF₄: Yb³⁺/Er³⁺/30%Fe³⁺	Hydrothermal	34(G), 30(R)	25
NaYF₄: Yb³⁺/Er³⁺/15%Co²⁺	Thermal decomposition	114(G), 84(R)	26
LiYF₄: Yb³⁺/Er³⁺/10%Cd²⁺	Thermal decomposition	2.2(G)	27
NaYF₄: Yb³⁺/Er³⁺/20%Ni²⁺	Hydrothermal	32.8(G), 20.99(R)	28
NaGdF₄: Yb³⁺/Er³⁺/13.5%Mg²⁺	Solvothermal	9(R), 6(G)	29
KMnF₃: Yb³⁺/Er³⁺/30%Mg²⁺	Solvothermal	20.8(R)	30
NaYF₄: Yb³⁺/Er³⁺/60%Cu²⁺	Hydrothermal	37(G), 25(R)	31
NaYF₄: Yb³⁺/Er³⁺/5%Zn²⁺	Hydrothermal	<2	32
KLaF₄:Yb³⁺/Er³⁺/10%Al³⁺	Hydrothermal	5.9(G), 7.3(R)	33
NaGdF₄: Yb³⁺/Er³⁺/25%Bi³⁺	Hydrothermal	60(802 nm), 160(B)	34

Fig. 3 Red emission upnconversion fluorescence spectra of Mn2+ doped NaYF4:Yb3+,Er3+[35]

Fig. 4 Basic functions of a shell around Ln3+ doped nanoparticles[36]

Fig. 5 The mechanism and spectrogram of the upconversion nanocrystals enhanced by activated shell.(a) Schematic diagram. (b)Upconversion luminescence spectra(The insert illustrated the comparison of the luminescence intensity of nanoparticles coated with inert and activated shells under the same excitation density).(c) Mechanism of enhanced luminescence[45].(d) The upconversion emission spectra and phtographs of nanoparticles coated with active shell and uncoated: BaGdF5:Yb3+, Er3+@BaGdF5:x%Yb3+(left), core、core@active shell、core@active shell@active shell(right)[46]

Fig. 6 (a) The upconversion luminscence and quantum yield of NaYF4:Yb3+,Er3+ nanoparticles coated with heterogeneous shell[47].(b)Emission spectra of NaYF4:Yb3+,Er3+@mNaYF4(m=0,1,2,3,4,5)nanoparticles by 980 nm excitation[49]

Fig. 7 Schematic illustration showing the plausible mechamism of enhancement of upconversion luminescence by plasmon resonance[1]

Fig. 8 (a) Upconversion luminescence spectra of Ag NP-Al2O3-NaYF4:Yb3+,Er3+ UCNPs,the inset is its schematic structure[58].(b)Luminscence enhancement through use of a disk-coupled dot-on-pillar antenna array(D2PA)[59].(c) PL enhancement factor as a function of SiO2 spacer layer thickness[60].(d) The center field intensity [E/Eo] [2]z=d/2. The inset table is the numerical Efupc of the NaGdF4: Yb3+,Er3+ under 980 nm excitation[61]

Table 2 Core-shell system for plasmonic enhancement luminscence of rare earth fluoride

Upconversion materials	Space	Plasmonic material	Enchancement factors	ref
NaYF₄: Yb³⁺/Er³⁺	——	Ag	green/red↑	64
NaYF₄: Yb³⁺/Tm³⁺	——	Au(≈10 nm)	109.0(345 nm)	65
NaYF₄: Yb³⁺/Er³⁺/Gd³⁺	——	Au(sphere)	3.8(540 nm), 4.0(660 nm)	66
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺	——	Au shell(4~8 nm)	8(646 nm)	67
NaYF₄: Yb³⁺/Tm³⁺	PAA^①/PAH	Au	≈2.5(452 nm,476 nm)	68
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺	PAMAM^②	Ag(20 nm) Au(20 nm)	20(413 nm), 22(452 nm) 20(518 nm), 21(540 nm)	69
NaYF₄: Yb³⁺/Tm³⁺	PAMAM	Au rod	27(805 nm), 6(470,550 nm)	70
NaYF₄: Yb³⁺/Er³⁺	SiO₂(10 nm)	Ag(15 nm) Ag(30 nm)	14.4(542 nm), 12.2(656 nm) 9.5(542 nm), 10.8(656 nm)	71
NaGdF₄: Yb³⁺/Er³⁺	SiO₂(8 nm)	Au rod	9(540 nm)	72
NaYF₄:Nd³⁺/Yb³⁺/Ho³⁺	SiO₂(10 nm)	Ag	15(540 nm), 7.5(655 nm)	73
NaGdF₄: Yb³⁺/Er³⁺	NaGdF₄	Ag	2.0(540 nm), 2.51(650 nm)	74
Ag/graphene	SiO₂(10 nm)	NaLuF₄: Yb³⁺/Gd³⁺/Er³⁺	52(520~550 nm)	75
Au rod	SiO₂(19 nm)	CaF₂: Yb³⁺Er³⁺	2.0(540 nm), 2.0(650 nm)	76
Au	SiO₂(28 nm)	NaGdF₄:Yb³⁺,Nd³⁺@NaGdF₄:Yb³⁺,Er³⁺@NaGdF₄	18.9(545 nm), 4.9(660 nm)	77
Ag-Au nanocage	NaYF₄	NaYF₄: Yb³⁺/Er³⁺	25	78

Table 2 Core-shell system for plasmonic enhancement luminscence of rare earth fluoride

Upconversion materials	Space	Plasmonic material	Enchancement factors	ref
NaYF₄: Yb³⁺/Er³⁺	——	Ag	green/red↑	64
NaYF₄: Yb³⁺/Tm³⁺	——	Au(≈10 nm)	109.0(345 nm)	65
NaYF₄: Yb³⁺/Er³⁺/Gd³⁺	——	Au(sphere)	3.8(540 nm), 4.0(660 nm)	66
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺	——	Au shell(4~8 nm)	8(646 nm)	67
NaYF₄: Yb³⁺/Tm³⁺	PAA^①/PAH	Au	≈2.5(452 nm,476 nm)	68
NaYF₄:Yb³⁺/Er³⁺/Tm³⁺	PAMAM^②	Ag(20 nm) Au(20 nm)	20(413 nm), 22(452 nm) 20(518 nm), 21(540 nm)	69
NaYF₄: Yb³⁺/Tm³⁺	PAMAM	Au rod	27(805 nm), 6(470,550 nm)	70
NaYF₄: Yb³⁺/Er³⁺	SiO₂(10 nm)	Ag(15 nm) Ag(30 nm)	14.4(542 nm), 12.2(656 nm) 9.5(542 nm), 10.8(656 nm)	71
NaGdF₄: Yb³⁺/Er³⁺	SiO₂(8 nm)	Au rod	9(540 nm)	72
NaYF₄:Nd³⁺/Yb³⁺/Ho³⁺	SiO₂(10 nm)	Ag	15(540 nm), 7.5(655 nm)	73
NaGdF₄: Yb³⁺/Er³⁺	NaGdF₄	Ag	2.0(540 nm), 2.51(650 nm)	74
Ag/graphene	SiO₂(10 nm)	NaLuF₄: Yb³⁺/Gd³⁺/Er³⁺	52(520~550 nm)	75
Au rod	SiO₂(19 nm)	CaF₂: Yb³⁺Er³⁺	2.0(540 nm), 2.0(650 nm)	76
Au	SiO₂(28 nm)	NaGdF₄:Yb³⁺,Nd³⁺@NaGdF₄:Yb³⁺,Er³⁺@NaGdF₄	18.9(545 nm), 4.9(660 nm)	77
Ag-Au nanocage	NaYF₄	NaYF₄: Yb³⁺/Er³⁺	25	78

Fig. 9 (a)The schematic of the formation of PMMA OPCs/NaYF4:Yb3+,Tm3+ UCNP composites.(b)A comparision of UCL spectra of NaYF4:Yb3+,Tm3+ UCNP and PMMA OPCs/NaYF4:Yb3+,Tm3+ composites. Inset:UC population and emission process of NaYF4:Yb3+,Tm3+.(c) Dependence of the UC enhancement factor as a funciton of PSB of PMMA OPCs[81]

Fig. 10 Schematic illustrations of dye sensitized upconversion in(a) Core(S: sensitizer, A: activator).(b)The core-shell structure(S1: type 1 sensitizer, S2:type 2 sensitizer, A: activator). The red solid line, red dashed line, blue solid line, blue dashed line and green arrows represent the excitation, energy transfer, upconversion pathway and fluorescence process[93]

Fig. 11 (a) A schematic illustrations of IR-806 sensitized β-NaYF4: Yb3+/Er3+nanoparticles.(b) Luminescence spectra of β-NaYF4: Yb3+/Er3+nanoparticles(cyan line),IR-806(green line), IR-780/β-NaYF4: Yb3+/Er3+ nanoparticles(red line), IR-806/β-NaYF4: Yb3+/Er3+nanoparticles(blue line)[94]

Fig. 12 Schematic illustration of dye-sensitized nanoparticles with tunable excitation wavelength(a) β-NaYF4: Yb3+/Er3+[96].(b) β-NaYF4:Yb3+/Tm3+[97].(c)Energy diagram of three sensiticers.(d)Excitation power dependence of upconverted emission from NaY0.48Gd0.3Yb0.2Er0.02F4 IR806-UCNP under excitation of the dye(808 nm excitation) or UCNP(980 nm excitation). Error bars represent one standard deviation from the mean. Inset, emission spectra for dye or direct excitation[98]

Fig. 13 Schematic illustration of the surface-photon-enhanced upconversion process[102]

Fig. 14 (a)Schematic illustration of DNA-based NR dimer and UCNP core-satellite assembly for multimodal imaging guided combination phototherapy.(b) Photothermal effect of assemblies of PBS、NR-UCNP-Ce6 and NR-dimer-UCNP-Ce6.(c)Thermal images of HeLa tumor-bearing mice with PBS、UCNP-Ce6、NR、NR dimer、NR-UCNP-Ce6 and NR-dimer-UCNP-Ce6[109]

Fig. 15 (a) Schematic illustration of the sandwich structured UCNPs and the principle of FRET based UC probe for Cu2+ detection[111].(b) FRET detection of avidin by employing biotinylated NCs as the donor and FITC as an acceptor[83].(c)Broadband near-infrared sunlight harvesting and then spectral conversion into visible range to activate N719 dye for the improvement of DSSC device.(d) The current density-voltage(J-V) characteristics of DSSC, DSSC-UCNPs and DSSC-DSUCNPs under AM 1.5 G simulated sunlight irradiation(100 mW·cm-2)[115]

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Enhancement Luminescence and Applications of Rare Earth Fluoride

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Enhancement Luminescence and Applications of Rare Earth Fluoride