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a) Illustrations of binary encoding capacity with orthogonal or correlated emission lifetime and intensity. b) Luminescence images of PDMS beads encapsulating co-doping (top) or gradient doping (bottom) UCNPs. Scale bar: 1 mm. Excitation power density = 13.1 Wcm À2 . c) Lifetime and intensity binary encoding results of luminescent beads in (b). d) Lifetime profiles with standard deviation extracted from the dotted lines shown in (b).
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The lanthanide sensitizer gradient doping structure in near‐infrared (NIR) excitable upconversion nanoparticles (UCNPs) was studied. With gradient doping, independent emission intensity and lifetime tuning is realized.
Abstract
Luminescent materials with engineered optical properties have been developed for multiplexed labeling detection, where en...
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... lifetime values can be further tuned by changing the Tm 3+ activator doping concentration or increasing the outer shell2 thickness. Lifetime can change from the original 620 ms to a range of 1352-480 ms by tuning Tm 3+ concentration (Supporting Information, Figure S3) or from 1173 ms to 1018-1340 ms by tuning shell2 thickness (Supporting Information, Figure S4). These orthogonal modulations lay the foundation for applications in luminescent multiplexing (Supporting Information, Figure S5). ...
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... independent modulation method can enrich the capacity of practically multiplexing. A theoretical encoding number by combining orthogonally adjustable upconversion luminescence intensity (n) and lifetime (k) is (k + 1) n À1, [3b] (Figure 3 a). However, this two dimensions are actually not independent, as shown in conventional co-doping UCNPs (NaYF 4 :x%Yb,1 %Tm@NaYF 4 , x = 19, 29, 49; Supporting Information, Figure S9), which makes the practical encoding capacity much smaller. ...
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... this two dimensions are actually not independent, as shown in conventional co-doping UCNPs (NaYF 4 :x%Yb,1 %Tm@NaYF 4 , x = 19, 29, 49; Supporting Information, Figure S9), which makes the practical encoding capacity much smaller. To directly show the merits of independent lifetime and emission intensity, polydimethylsiloxane (PDMS) beads encapsulating co-doping or gradient doping UCNPs with three lifetime levels were imaged simultaneously (Figure 3 b). The co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). ...
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... directly show the merits of independent lifetime and emission intensity, polydimethylsiloxane (PDMS) beads encapsulating co-doping or gradient doping UCNPs with three lifetime levels were imaged simultaneously (Figure 3 b). The co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). In comparison, lifetime patterns of the gradient one (NaYF 4 @NaYF 4 : x%Yb,1 %Tm@ NaYF 4 : y%Yb @NaYF 4 (x/y = 20:50, 50:20, 80:5) with the same intensity levels can all be clearly resolved with precise shape (Figure 3 b bottom and Figure 3 c) and lower coefficient of variation (1.32 % vs. 6.44 % in co-doping UCNPs) (Figure 3 d). ...
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... directly show the merits of independent lifetime and emission intensity, polydimethylsiloxane (PDMS) beads encapsulating co-doping or gradient doping UCNPs with three lifetime levels were imaged simultaneously (Figure 3 b). The co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). In comparison, lifetime patterns of the gradient one (NaYF 4 @NaYF 4 : x%Yb,1 %Tm@ NaYF 4 : y%Yb @NaYF 4 (x/y = 20:50, 50:20, 80:5) with the same intensity levels can all be clearly resolved with precise shape (Figure 3 b bottom and Figure 3 c) and lower coefficient of variation (1.32 % vs. 6.44 % in co-doping UCNPs) (Figure 3 d). ...
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... co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). In comparison, lifetime patterns of the gradient one (NaYF 4 @NaYF 4 : x%Yb,1 %Tm@ NaYF 4 : y%Yb @NaYF 4 (x/y = 20:50, 50:20, 80:5) with the same intensity levels can all be clearly resolved with precise shape (Figure 3 b bottom and Figure 3 c) and lower coefficient of variation (1.32 % vs. 6.44 % in co-doping UCNPs) (Figure 3 d). ...
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... co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). In comparison, lifetime patterns of the gradient one (NaYF 4 @NaYF 4 : x%Yb,1 %Tm@ NaYF 4 : y%Yb @NaYF 4 (x/y = 20:50, 50:20, 80:5) with the same intensity levels can all be clearly resolved with precise shape (Figure 3 b bottom and Figure 3 c) and lower coefficient of variation (1.32 % vs. 6.44 % in co-doping UCNPs) (Figure 3 d). ...
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... co-doping one shows correlated lifetime levels with intensity levels ( Figure 3 c; Supporting Information, Figure S10) which hampered the extraction of lifetime value from the dim UCNPs [17] (Figure 3 b top). In comparison, lifetime patterns of the gradient one (NaYF 4 @NaYF 4 : x%Yb,1 %Tm@ NaYF 4 : y%Yb @NaYF 4 (x/y = 20:50, 50:20, 80:5) with the same intensity levels can all be clearly resolved with precise shape (Figure 3 b bottom and Figure 3 c) and lower coefficient of variation (1.32 % vs. 6.44 % in co-doping UCNPs) (Figure 3 d). ...
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Luminescent materials with engineered optical properties have been developed for multiplexed labeling detection, where encoding capacity plays a pivotal role in the efficiency. However, multi‐dimensional optical identities are usually not independent which essentially hinder the practical encoding numbers to access theoretical capacity. In this wor...
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... 稀土元素因其丰富的能级而能够发出绚丽多彩的 光芒，这些不同颜色的发光可以在不同的条件下被触 发，用于信息存储或防伪 [102][103][104][105][106][107][108][109][110] [111] Figure 14 Simulated encryption and decryption process. Non-switching pixels are covered with NaYF 4 ∶40%Yb 3+ , 2%Ho 3+ , while switching pixels are covered with Y 2 Mo 4 O 15 ∶40%Yb 3+ , 2%Ho 3+ (a)~(b); Overlaying (a) and (b) to obtain (c) [111] 对标准偏差 5% 或更低的优异性能，且无需任何校准 [113] Figure 16 Three overlapping patterns are printed with different Tm τ-dots∶(C Yb ∶C Tm ) 20∶4 for the "Macquarie University" logo, 20∶1 for the "Sydney Opera House" image, and 20∶ 0.5 for the "Sydney Harbour Bridge" image. ...
... Commercial ODS, e.g., Blu-ray Disc (BD) [6][7][8], employs the confocal scanning method to achieve the recording track pitch of 320 nm and minimum recording mark length of about 150 nm with a capacity of 400 GB per disk, which is far from satisfying the exploding demand of next-generation information storage. To further improve the disk capacity, information multiplexing is exploited to extend the dimensions of ODS, i.e., wavelength [9,10], polarization [11][12][13], lifetime [14], and spatial dimensions [15][16][17][18][19]. The five-dimensional optical recording technique [20], integrated with the multiplexing of wavelength, polarization, and spatial dimensions, extends the disk capacity to 1.6 TB for a DVD-sized disk. ...
... The authors declare no conflicts of interest. Nanomaterials 2024, 14, 364 ...
The big data era demands an efficient and permanent data storage technology with the capacity of PB to EB scale. Optical data storage (ODS) offers a good candidate for long-lifetime storage, as the developing far-field super-resolution nanoscale writing technology improves its capacity to the PB scale. However, methods to efficiently read out this intensive ODS data are still lacking. In this paper, we demonstrate a sub-diffraction readout method based on polarization modulation, which experimentally achieves the sub-diffraction readout on Disperse Red 13 thin film with a resolution of 500 nm, exceeding the diffraction limit by 1.2 times (NA = 0.5). Differing from conventional binary encoding, we propose a specific polarization encoding method that enhances the capacity of ODS by 1.5 times. In the simulation, our method provides an optical data storage readout resolution of 150 nm, potentially to 70 nm, equivalent to 1.1 PB in a DVD-sized disk. This sub-diffraction readout method has great potential as a powerful readout tool for next-generation optical data storage.
... Lanthanide-doped luminescent nanoparticles can convert low-energy infrared photons into higherenergy visible photons which are called upconversion nanoparticles (UCNPs) [1][2][3][4][5][6][7][8] . They have received extensive attention due to their unique fluorescence characteristics including sharp emission peaks 7 , abundant color output 5,9 , long lifetime 3,4,10,11 , and excellent stability, so that they are potentially suitable for the applications in the fields of microlaser 12,13 , bioimaging 14,15 , biodetection [16][17][18] , photovoltaics 19,20 , catalysis 21 , 3D printing 22,23 , and anti-counterfeiting 24,25 . Under the excitation of infrared light, upconversion nanoparticles can emit visible light with multicolors from long wavelength red to short wavelength violet. ...
Lanthanide-doped upconversion nanoparticles have unique optical properties that can absorb low-energy infrared photons and then emit higher-energy visible ones, which have been widely used for advanced optical sensors and fluorescent probes. Efficiently tailoring the upconversion emission is desirable for meeting the wavelength requirement in various application fields. However, up to now, optimizing the composition combining with core/shell structure is still the predominant way to reach this goal. Here, we show that the relative intensities of the emission peaks of upconverting nanoparticles can be tuned by coupling to single microcavity mode with specific symmetry. Theoretical calculation based on the finite-difference method in time-domain (FDTD) indicates that the symmetries of the microcavity modes dominate their resonant absorption properties in the visible region. As a result, the upconversion emission peaks vary in these microcavities with different symmetries. This route can be developed for tailoring the emission spectra of other luminescent materials, such as quantum dots and fluorescent dyes.
... Owing to their unique advantages of long fluorescence lifetime, narrow emission bandwidth, high optical/chemical stability, and low biotoxicity, rare-earth upconversion nanomaterials have recently drawn enduring attention of researchers and have been shown to be promising for application in a wide range of fields including biological imaging [1][2][3], photodynamic therapy [4][5][6][7], information storage [8][9][10][11], and multilevel anticounterfeiting [12][13][14][15][16][17][18][19][20]. Because of their characteristic 4f configuration, trivalent lanthanides are rich in ladder-like energy levels, from which upconversion luminescence (UCL) spanning ultraviolet (UV), visible (vis), and near-infrared (NIR) spectral regions can be accessible in lanthanide-doped upconversion nanoparticles (UCNPs). ...
Lanthanide-doped upconversion nanoparticles (UCNPs) have been extensively investigated owing to their unique advantages. So far, the most favored modality of UCNPs is still the classical Yb–A (where A refers to Er3+, Tm3+, and Ho3+)-coupled nanosystems under 980-nm excitation. However, the frequently used Yb3+ ion with the single-excited 2F5/2 state can barely transfer energy to other acceptors owing to its lack of matched excited levels. Herein, a novel strategy is proposed for energy transfer via Ho3+ as a bridge ion coupling donor-acceptor pairs (e.g., Yb3+–Nd3+), where little direct energy transfer occurs, and the involved energy transport mechanisms are investigated. The findings reveal that long-distance energy transportation can occur in the Ho3+ sublattice owing to the energy migration capability of Ho3+ and that Ho3+ as a bridge ion can realize interparticle energy transfer for upconversion luminescence. Moreover, well-designed NaYbF4:40%Ho@NaYF4:10%Nd core-shell nanoparticles with multimode responsiveness can emit different colored lights under varying excitation wavelengths, which are demonstrated in high-level anticounterfeiting and information identification. Therefore, this work paves a new way to understand the functionality of the Ho3+ bridge in energy transfer upconversion and offers strategies for broadening energy transfer pathways and finely manipulating photon upconversion.
... [1][2][3][4][5][6][7][8][9][10][11][12] Obviously, a deep understanding of the working principles behind those individual applications is the key to successful modulation of UCL emission with expected parameters in terms of lifetime, relative intensity, and wavelength, toward different purposes. [13][14][15][16][17][18][19][20] Unfortunately, UCL process was empirically assumed to have the same time-resolved output profile as that of organic dye/quantum dot, [21][22][23][24] which works as one luminescing unit and is composed of a sharp rise and a steep decay edge originated from population and depopulation process, [25] respectively. In detail, electrons are pumped to excited state under proper excitation, and (after a quick relaxation) return immediately to the ground state accompanied with luminescence emission (Figure 1a). ...
Different from organic dye/quantum dot possessing one luminescent center, upconversion luminescence (UCL) is actually a statistic of temporal behaviors of countless individual activators. Our experimental results have shown that the rise and decay dynamics of UCL is directly associated with the relative contribution of sensitizer‐to‐activator energy transfer and energy migration among sensitizers, which can be physically modulated by simply tuning the excitation laser. Therefore, dynamic UCL with record‐wide 20‐fold lifetime, ≈70‐fold red‐to‐green intensity ratio, and reversibly definable emission color is easily realized by just modulating the excitation laser. Moreover, this generally applicable strategy only requires a simplest‐possible UCL system whereas prevalent material engineering such as complicated composition design, sophisticated core–shell construction, or tedious chemical synthesis, is no longer needed.
Optical encryption technologies based on persistent luminescence material have currently drawn increasing attention due to the distinctive and long‐lived optical properties, which enable multi‐dimensional and dynamic optical information encryption to improve the security level. However, the controlled synthesis of persistent phosphors remains largely unexplored and it is still a great challenge to regulate the structure for optical properties optimization, which inevitably sets significant limitations on the practical application of persistent luminescent materials. Herein, a controlled synthesis method is proposed based on defect structure regulation and a series of porous persistent phosphors is obtained with different luminous intensities, lifetime, and wavelengths. By simply using diverse templates during the sol–gel process, the oxygen vacancy defects structures are successfully regulated to improve the optical properties. Additionally, the obtained series of porous Al 2 O 3 are utilized for multi‐color and dynamic optical information encryption to increase the security level. Overall, the proposed defect regulation strategy in this work is expected to provide a general and facile method for optimizing the optical properties of persistent luminescent materials, paving new ways for broadening their applications in multi‐dimensional and dynamic information encryption.
The optical nanoprobes with emissions in the second near‐infrared window (NIR‐II, 1000–1700 nm) show low tissue autofluorescence and photon scattering; therefore, they provide high spatial resolution and acceptable tissue penetration depth. These advantages make them appropriate for in vivo applications, including bioimaging, NIR‐II triggered disease therapy, and even on‐site efficacy monitoring. Among the various developed NIR‐II fluorescence probes, lanthanide‐doped nanoparticles (LDNPs) exhibit high photo stability and narrow emission bandwidths with long photoluminescence lifetimes and low cytotoxicity; therefore, they have been widely studied in the biomedical field. This review summarizes the typical compositions and optical properties of recently developed NIR‐II emitting LDNPs. Their applications in in vivo NIR‐II bioimaging and cancer therapy are reviewed. The perspectives and challenges of NIR‐II LDNPs are also discussed.
NaErF4 is the most extensively studied host for self-sensitized upconversion (UC), and Yb3+ is the most commonly used energy absorber. It’s reported that the red luminescence of Er3+ can be...
Different from organic dye/quantum dot possessing one luminescent center, upconversion luminescence (UCL) is actually a temporal statistic of countless individual activators. Our experimental results have shown that the rise and decay dynamics of UCL is directly associated with the relative contribution of sensitizer‐to‐activator energy transfer and energy migration among sensitizers, which can be physically modulated by tuning the excitation laser. Therefore, dynamic UCL with record‐wide 20‐fold lifetime, ~70‐fold red‐to‐green intensity ratio, and reversibly definable emission color is easily realized by just modulating the excitation laser. Moreover, this generally applicable strategy only requires a simplest‐possible UCL system whereas prevalent material engineering such as complicated composition design, sophisticated core‐shell construction, or tedious chemical synthesis, is no longer needed.
