High-Temperature Surface Thermometry Technique based on Upconversion Nano-Phosphors

NASA Astrophysics Data System (ADS)

Combs, C.; Clemens, N.; Guo, X.; Song, H.; Zhao, H.; Li, K. K.; Zou, Y. K.; Jiang, H.

2011-11-01

Downconversion thermographic phosphors have been extensively used for high-temperature surface thermometry applications (e.g., aerothermodynamics, turbine blades) where temperature-sensitive paint is not viable. In downconversion techniques the phosphorescence is at longer wavelengths than the excitation source. We are developing a new upconversion thermographic phosphor technique that employs rare-earth-doped ceramics whose phosphorescence exhibit a strong temperature dependence. In the upconversion technique the phosphor is excited with near-IR light and emission is at visible wavelengths; thus, it does not require expensive UV windows and does not suffer from interference from background fluorescence. In this work the upconversion phosphors have been characterized in terms of their intensity, lifetimes and spectral content over a temperature range of 300K to 1500K. The technique has been evaluated for applications of 2D surface temperature measurements by using the total integrated intensity and the ratio of emission in different visible color bands. The results indicate that upconversion phosphor thermometry is a promising technique for making non-contact high-surface temperature measurements with good accuracy. Work supported by NASA under contract NNX11CG89P.

Synthesis and up-conversion luminescence of Er{sup 3+} and Y b{sup 3+} codoped nanocrystalline tetra- (KLaP{sub 4}O{sub 12}) and pentaphosphates (LaP{sub 5}O{sub 14})

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marciniak, L., E-mail: l.marciniak@int.pan.wroc.pl; Stefanski, M.; Tomala, R.

2015-09-07

The up-converting nanocrystals of KLa{sub 0.95}Er{sub 0.05}Y b{sub x}P{sub 4}O{sub 12} and La{sub 0.95−x}Er{sub 0.05}Y b{sub x}P{sub 5}O{sub 14} were prepared using co-precipitation method. The spectroscopic properties of these materials were investigated in a function of Y b{sup 3+} concentration. The up-conversion emission, power dependence of emission intensities, and the luminescence decay times were investigated. It was found that the green to red and {sup 2}H{sub 11/2} → {sup 4}I{sub 15/2} to {sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} emission intensity ratio were strongly affected by the Y b{sup 3+} concentration. Moreover, the order of up-conversion emission and threshold powermore » rises up with Y b{sup 3+} concentration for {sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} transition. The luminescence decay time of the {sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} emission increases with Y b{sup 3+} concentration while the {sup 4}F{sub 9/2} → {sup 4}I{sub 15/2} emission is independent of dopant concentration. The influence of the Y b{sup 3+} concentration on the up-conversion emission intensities was discussed in terms of concentration dependent hetero looped photon avalanche process. A comparison of the up-conversion properties of KLa{sub 0.95}Er{sub 0.05}Y b{sub x}P{sub 4}O{sub 12} and La{sub 0.95−x}Er{sub 0.05}Y b{sub x}P{sub 5}O{sub 14} nanocrystals was presented.« less

Upconversion emission study of Er{sup 3+} doped CaMoO{sub 4} phosphor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sinha, Shriya, E-mail: Shriya.sinha6@gmail.com; Mahata, Manoj Kumar; Kumar, Kaushal

2016-05-06

The infrared to visible upconversion emission in Er{sup 3+} doped CaMoO{sub 4} phosphor has been investigated upon 980 nm diode laser excitation. The X-ray diffraction analysis reveals well crystalline nature and tetragonal phase structure of the prepared phosphor annealed at 800 °C. The Er{sup 3+} doped CaMoO{sub 4} phosphor has shown intense green upconversion emission upon 980 nm didode laser excitation. The green emission bands at 530 nm and 552 nm corresponds to the {sup 2}H{sub 11/2}→{sup 4}I{sub 15/2} and {sup 4}S{sub 3/2}→{sup 4}I{sub 15/2} electronic transitions, respectively of Er{sup 3+} ion. The very weak red emission band around 656more » nm is assigned to the {sup 4}F{sub 9/2}→{sup 4}I{sub 15/2} transition of Er{sup 3+} ion. The CIE color coordinate exhibits the emission color in intense green region, indicating the use of present phosphor in display device applications.« less

Structure and intense UV up-conversion emissions in RE3+-doped sol-gel glass-ceramics containing KYF4 nanocrystals

NASA Astrophysics Data System (ADS)

Yanes, A. C.; Santana-Alonso, A.; Méndez-Ramos, J.; del-Castillo, J.

2013-12-01

Transparent nano-glass-ceramics containing KYF4 nanocrystals were successfully obtained by the sol-gel method, doped with Eu3+ and co-doped with Yb3+ and Tm3+ ions. Precipitation of cubic KYF4 nanocrystals was confirmed by X-ray diffraction and high-resolution transmission electron microscope images. Excitation and emission spectra let us to discern between ions into KYF4 nanocrystals and those remaining in a glassy environment, supplemented with time-resolved photoluminescence decays, that also clearly reveal differences between local environments. Unusual high-energy up-conversion emissions in the UV range were obtained in Yb3+-Tm3+ co-doped samples, and involved mechanisms were discussed. The intensity of these high-energy emissions was analyzed as a function of Yb3+ concentration, heat treatment temperature of precursor sol-gel glasses and pump power, determining the optimum values for potential optical applications as highly efficient UV up-conversion materials in UV solid-state lasers.

Energy transfer dynamics of Er3+/Nd3+ embedded SiO2-Al2O3-Na2CO3-SrF2-CaF2 glasses for optical communications

NASA Astrophysics Data System (ADS)

Gelija, Devarajulu; Kadathala, Linganna; Borelli, Deva Prasad Raju

2018-04-01

The fluorescence and upconversion studies of Er3+ doped and Er3+/Nd3+ co-doped silicate based oxyfluoride glasses have been systematically analyzed. The broad band NIR emissions (830-1700 nm), includes optical bands like O, E, S, C and L were observed in the Er3+-Nd3+ co-doped glasses. The NIR emission intensity peaks centered at 876, 1057, 1329 and 1534 nm were observed for the Er3+-Nd3+ co-doped glasses. In the co-doped samples the strongest emission intensity at 1534 nm increased up to 0.5 mol % and then decreased to 3.0 mol % of Nd3+ ions under the excitation of 980 nm. The upconversion studies of the co-doped samples were recorded under the excitation of 980 and 808 nm and found the upconversion emission peaks centered at 524, 530, 547, 590 and 656 nm. The energy transfer processes between the relevant excitation levels of Er3+ and Nd3+ ions and energy transfer efficiency were discussed. The obtained results indicate that Nd3+ can be an efficient sensitizer for Er3+ to enhance upconversion emission at green laser transition for sensors and NIR emission at 1534 nm for optical communication applications.

Yb3+ sensitized Tm3+ upconversion in tellurite lead oxide glass.

PubMed

Mohanty, Deepak Kumar; Rai, Vineet Kumar; Dwivedi, Y

2012-04-01

Triply ionized thulium/thulium--ytterbium doped/codoped TeO2-Pb3O4 (TPO) glasses have been fabricated by classical quenching method. The upconversion emission spectra in the Tm3+/Tm3+-Yb3+ doped/codoped glasses upon excitation with a diode laser lasing at ∼980 nm has been studied. Effect of the addition of the Yb3+ on the upconversion emission intensity in the visible and near infrared regions of the Tm3+ doped in TPO glass has been studied and the processes involved explored. Copyright © 2011 Elsevier B.V. All rights reserved.

Highly efficient upconversion luminescence in hexagonal NaYF4:Yb3+, Er3+ nanocrystals synthesized by a novel reverse microemulsion method

NASA Astrophysics Data System (ADS)

Gunaseelan, M.; Yamini, S.; Kumar, G. A.; Senthilselvan, J.

2018-01-01

A new reverse microemulsion system is proposed for the first time to synthesize NaYF4:Yb,Er nanocrystals, which demonstrated high upconversion emission in 550 and 662 nm at 980 nm diode laser excitation. The reverse microemulsion (μEs) system is comprised of CTAB and oleic acid as surfactant and 1-butanol co-surfactant and isooctane oil phase. The surfactant to water ratio is able to tune the microemulsion droplet size from 14 to 220 nm, which eventually controls the crystallinity and particulate morphology of NaYF4:Yb,Er. Also, the microemulsion precursor and calcination temperature plays certain role in transforming the cubic NaYF4:Yb,Er to highly luminescent hexagonal crystal structured upconversion material. Single phase hexagonal NaYF4:YbEr nanorod prepared by water-in-oil reverse microemulsion (μEs) gives intense red upconversion emission. Both nanosphere and nanorod shaped NaYF4:Yb,Er was obtained, but nanorod morphology resulted an enhanced upconversion luminescence. The structural, morphological, thermal and optical luminescence properties of the NaYF4:Yb,Er nanoparticles are discussed in detail by employing powder X-ray diffraction, dynamic light scattering, high resolution electron microscopy, TGA-DTA, UV-DRS, FTIR and photoluminescence spectroscopy. Intense upconversion emission achieved in the microemulsion synthesized NaYF4:Yb3+,Er3+ nanocrystal can make it as useful optical phosphor for solar cell applications.

Near-Infrared to Visible Organic Upconversion Devices Based on Organic Light-Emitting Field Effect Transistors.

PubMed

Li, Dongwei; Hu, Yongsheng; Zhang, Nan; Lv, Ying; Lin, Jie; Guo, Xiaoyang; Fan, Yi; Luo, Jinsong; Liu, Xingyuan

2017-10-18

The near-infrared (NIR) to visible upconversion devices have attracted great attention because of their potential applications in the fields of night vision, medical imaging, and military security. Herein, a novel all-organic upconversion device architecture has been first proposed and developed by incorporating a NIR absorption layer between the carrier transport layer and the emission layer in heterostructured organic light-emitting field effect transistors (OLEFETs). The as-prepared devices show a typical photon-to-photon upconversion efficiency as high as 7% (maximum of 28.7% under low incident NIR power intensity) and millisecond-scale response time, which are the highest upconversion efficiency and one of the fastest response time among organic upconversion devices as referred to the previous reports up to now. The high upconversion performance mainly originates from the gain mechanism of field-effect transistor structures and the unique advantage of OLEFETs to balance between the photodetection and light emission. Meanwhile, the strategy of OLEFETs also offers the advantage of high integration so that no extra OLED is needed in the organic upconversion devices. The results would pave way for low-cost, flexible and portable organic upconversion devices with high efficiency and simplified processing.

White up-conversion emission in Ho3+/Tm3+/Yb3+ tri-doped glass ceramics embedding BaF2 nanocrystals

NASA Astrophysics Data System (ADS)

Li, Chenxia; Xu, Shiqing; Ye, Rengguang; Deng, Degang; Hua, Youjie; Zhao, Shilong; Zhuang, Songlin

2011-04-01

Ho3+/Tm3+/Yb3+ tri-doped glass ceramics with white light emitting have been developed and demonstrated. Pumped by 980 nm laser diode (LD), intensive red, green and blue up-conversions (UC) were obtained. The green emission is assigned to Ho3+ ion and the blue emission is assigned to Tm3+ ion, whereas the red emission is the combination contribution of the Ho3+ and Tm3+ ions. The RGB intensities could be adjusted by tuning the rare-earth ion concentration and pump power intensity. Thus, multicolor of the luminescence, including perfect white light with CIE-X=0.329 and CIE-Y=0.342 in the 1931 CIE chromaticity diagram can be obtained in 0.15 Ho3+/0.2Tm3+/3Yb3+ tri-doped glass ceramics embedding BaF2 nanocrystals pumped by a single infrared laser diode source of 980 nm at 500 mW. The up-conversion luminescence mechanism of Yb3+ sensitize Ho3+ and Tm3+ ions and the energy transfer from Ho3+ to Tm3+ in oxy-fluoride silicate glass ceramics were analyzed.

Tuning upconversion luminescence of LiYF4:Yb3+,Er3+/Tm3+/Ho3+ microcrystals synthesized through a molten salt process.

PubMed

Niu, Na; He, Fei; Wang, Liuzhen; Wang, Lin; Wang, Yan; Gai, Shili; Yang, Piaoping

2014-05-01

In this paper, well-defined tetragonal-phase LiYF4:Yb3+,Er3+/Tm3+/Ho3+ micro-crystals with octahedral morphology were successfully prepared through a surfactant-free molten salt process for the first time. By gradually increasing the LiF content in the NaNO3-KNO3 reaction medium, the crystal phase transforms from a mixture of YF3 and LiYF4 to pure tetragonal-phase LiYF4. The possible formation process for the phase and morphology evolution is also presented. Moreover, upon 980 nm laser diode (LD) excitation, the lanthanide ions (Yb3+, Er3+/Tm3+/Ho3+) doped LiYF4 crystals exhibit intense upconversion emission lights. By tuning the sensitizer concentrations of Yb3+ ions in LiYF4:Yb3+,Er3+, the relative intensities of green and red emissions can be precisely adjusted under single wavelength excitation. Consequently, multicolor upconversion emissions can be obtained. On the other hand, UC mechanisms were also given based on the emission spectra and the plot of luminescence intensity to pump power.

Ho3+-Yb3+ codoped tellurite based glasses in visible lasers and optical devices: Judd-Ofelt analysis and frequency upconversion

NASA Astrophysics Data System (ADS)

Azam, Mohd; Rai, Vineet Kumar

2017-04-01

The optical absorption and frequency upconversion emission in the Ho3+/Yb3+ codoped TeO2-ZnO (TZ), TeO2-ZnO-WO3 (TZW) and TeO2-ZnO-WO3-TiO2 (TZWTi) glasses prepared by melting and quenching method has been studied. Judd-Ofelt theory has been used to calculate the Judd-Ofelt intensity parameters (Ω2, Ω4 and Ω6), transition probabilities, radiative lifetimes, absorption cross sections and the branching ratios. Upconversion (UC) emission bands centered at ∼ 549 nm, ∼658 nm and ∼754 nm are observed upon 980 nm excitation. On codoping with the Yb3+ ions at 3.0 mol% the upconversion emission intensity enhancement of about ∼57 times, ∼342 times and ∼480 times for the green band whereas for the red band arising from the Ho3+ ions it is about ∼71 times, ∼438 times and ∼707 times respectively have been observed. The enhancement observed in the UC emission intensity is explained on the basis of efficient energy transfer from Yb3+ to Ho3+, larger absorption cross section, larger oscillator strengths and increase in the local field corrections factor. The spectroscopic quality factor Ω4/Ω6 has been calculated to get the information about the developed materials for laser applications. The upconversion emission cross section determined on the basis of Judd-Ofelt analysis is found to be maximum for Ho-Yb-TZWTi glass. The nephelauxetic ratio, bonding and covalency parameters have been calculated to know the nature of bonding between the rare earth ions and neighbouring oxygen atoms. The high color purity 83.8% has been reported in the codoped glasses at ∼81.2 W/cm2 pump power density.

Bright up-conversion white light emission from Er3+ doped lithium fluoro zinc borate glasses for photonic applications

NASA Astrophysics Data System (ADS)

Vijayalakshmi, L.; Naveen Kumar, K.; Rao, K. Srinivasa; Hwang, Pyung

2018-03-01

Various concentrations of Er3+ (0.3, 0.5, 1.0 and 1.5 mol %) doped lithium fluoro zinc borate glasses were synthesized by a traditional melt quenching method. XRD, FTIR and FESEM have been employed to analyze the structural, compositional and morphological analysis respectively. Judd-Ofelt theory has been employed to analyze the intensity parameters (Ωλ, λ = 2, 4 and 6) which can be used to estimate the radiative properties of fluorescent levels of Er3+. We have been observed a strong NIR emission peak at 1.53 μm (4I13/2 → 4I15/2) under the excitation of 980 nm from Er3+: LBZ glasses. Nevertheless, the NIR emission is remarkably enhanced by increasing the Er3+ ions concentration until the optimized concentration of 0.5 mol%. The lifetime of the excited level of 4I13/2 in the NIR emission transition is evaluated and it is found to be1.22 ms from the decay analysis of 0.5 mol% Er3+: LBZ glass. Apart from the NIR emission, a bright up-conversion green emission is observed at 544 nm (4S3/2 → 4I15/2) along with an intense red emission at 659 nm (4F9/2 → 4I15/2) and a weak blue emission (2H9/2 → 4I15/2) under the excitation of 980 nm. Up-conversion emission features were significantly enhanced with increasing the Er3+ concentration up to 1.0 mol%. The combination of the obtained up-conversion emission colors of green, red and blue could generate white light emission. The cool white-light emission from the optimized glass sample has been confirmed from the Commission International de I'Echairage (CIE) 1931 chromaticity diagram analysis and their correlated color temperature (CCT) values. Based on the NIR and up-conversion emission features, Er3+: LBZ glasses could be suggested as promising candidates for optical amplifiers, optical telecommunication windows and white light photonic applications.

Intense green and red upconversion emission of Er3+,Yb3+ co-doped CaZrO3 obtained by a solution combustion reaction

NASA Astrophysics Data System (ADS)

Singh, Vijay; Kumar Rai, Vineet; Haase, Markus

2012-09-01

CaZrO3 phosphors co-doped with Er3+ and Yb3+ ions have been prepared by the urea combustion route. The formation of the orthorhombic phase of CaZrO3 was confirmed by powder x-ray diffraction. The absorption in the 280-1800 nm region and excitation spectrum corresponding to the emission at 545 nm for CaZrO3:Er3+/CaZrO3:Er3+,Yb3+ phosphors have been recorded. Upon excitation at 978 nm, the material displays strong energy transfer upconversion emission in the green and red spectral regions. The upconversion emission of the CaZrO3:Er3+,Yb3+ co-doped material shows an increased red-to-green ratio, indicating cross relaxation between Er3+ ions.

Spectroscopic Imaging of NIR to Visible Upconversion from NaYF4:Yb3+, Er3+ Nanoparticles on Au Nano-cavity Arrays

NASA Astrophysics Data System (ADS)

Fisher, Jon; Zhao, Bo; Lin, Cuikun; Berry, Mary; May, P. Stanley; Smith, Steve

2015-03-01

We use spectroscopic imaging to assess the spatial variations in upconversion luminescence from NaYF4:Er3+,Yb3+ nanoparticles embedded in PMMA on Au nano-cavity arrays. The nano-cavity arrays support a surface plasmon (SP) resonance at 980nm, coincident with the peak absorption of the Yb3+ sensitizer. Spatially-resolved upconversion spectra show a 30X to 3X luminescence intensity enhancement on the nano-cavity array compared to the nearby smooth Au surface, corresponding to excitation intensities from 1 W/cm2 to 300kW/cm2. Our analysis shows the power dependent enhancement in upconversion luminescence can be almost entirely accounted for by a constant shift in the effective excitation intensity, which is maintained over five orders of magnitude variation in excitation intensity. The variations in upconversion luminescence enhancement with power are modeled by a 3-level-system near the saturation limit, and by simultaneous solution of a system of coupled nonlinear differential equations, both analyses agree well with the experiments. Analysis of the statistical distribution of emission intensities in the spectroscopic images on and off the nano-cavity arrays provides an estimate of the average enhancement factor independent of fluctuations in nano-particle density. Funding provided by NSF Award # 0903685 (IGERT).

Optical transitions of Ho(3+) in oxyfluoride glasses and upconversion luminescence of Ho(3+)/Yb(3+)-codoped oxyfluoride glasses.

PubMed

Feng, Li; Wu, Yinsu

2015-05-05

Optical properties of Ho(3+)-doped SiO2-BaF2-ZnF2 glasses have been investigated on the basis of the Judd-Ofelt theory. Judd-Ofelt intensity parameters, radiative transition probabilities, fluorescence branching ratios and radiative lifetimes have been calculated for different glass compositions. Upconversion emissions were observed in Ho(3+)/Yb(3+)-codoped SiO2-BaF2-ZnF2 glasses under 980nm excitation. The effects of composition, concentration of the doping ions, and excitation pump power on the upconversion emissions were also systematically studied. Copyright © 2015 Elsevier B.V. All rights reserved.

Optical transitions of Tm3+ in oxyfluoride glasses and compositional and thermal effect on upconversion luminescence of Tm3+/Yb3+-codoped oxyfluoride glasses.

PubMed

Feng, Li; Wu, Yinsu; Liu, Zhuo; Guo, Tao

2014-01-24

Optical properties of Tm(3+)-doped SiO2-BaF2-ZnF2 glasses have been investigated on the basis of the Judd-Ofelt theory. Judd-Ofelt intensity parameters, radiative transition probabilities, fluorescence branching ratios and radiative lifetimes have been calculated for different glass compositions. Upconversion emissions were observed in Tm(3+)/Yb(3+)-codoped SiO2-BaF2-ZnF2 glasses under 980 nm excitation. The effects of composition, concentration of the doping ions, temperature, and excitation pump power on the upconversion emissions were also systematically studied. Copyright © 2013 Elsevier B.V. All rights reserved.

Upconversion luminescence, intensity saturation effect, and thermal effect in Gd{sub 2}O{sub 3}:Er{sup 3},Yb{sup 3+} nanowires

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lei Yanqiang; Song Hongwei; Yang Linmei

2005-11-01

In this paper, the upconversion luminescent properties of Gd{sub 2}O{sub 3}:Er{sup 3+},Yb{sup 3+} nanowires as a function of Yb concentration and excitation power were studied under 978-nm excitation. The results indicated that the relative intensity of the red emission ({sup 4}F{sub 9/2}-{sup 4}I{sub 15/2}) increased with increasing the Yb{sup 3+} concentration, while that of the green emission ({sup 4}S{sub 3/2}/{sup 2}H{sub 11/2}-{sup 4}I{sub 15/2}) decreased. As a function of excitation power in ln-ln plot, the green emission of {sup 4}S{sub 3/2}-{sup 4}I{sub 15/2} yielded a slope of {approx}2, while the red emission of {sup 4}F{sub 9/2}-{sup 4}I{sub 15/2} yielded amore » slope of {approx}1. Moreover, the slope decreased with increasing the Yb{sup 3+} concentration. This was well explained by the expanded theory of competition between linear decay and upconversion processes for the depletion of the intermediate excited states. As the excitation power density was high enough, the emission intensity of upconversion decreased due to thermal quenching. The thermal effect caused by the exposure of the 978-nm laser was studied according to the intensity ratio of {sup 2}H{sub 11/2}-{sup 4}I{sub 15/2} to {sup 4}S{sub 3/2}-{sup 4}I{sub 15/2}. The practical sample temperature at the exposed spot as a function of excitation power and Yb{sup 3+} concentration was deduced. The result indicated that at the irradiated spot (0.5x0.5 mm{sup 2}) the practical temperature considerably increased.« less

Up-conversion green emission of Yb3+/Er3+ ions doped YVO4 nanocrystals obtained via modified Pechini's method

NASA Astrophysics Data System (ADS)

Szczeszak, Agata; Runowski, Marcin; Wiglusz, Rafal J.; Grzyb, Tomasz; Lis, Stefan

2017-12-01

A series of lanthanide doped yttrium vanadates were prepared by Pechini's method (sol-gel process). The as-prepared precursors, in the presence of citric acid, were calcined in the temperature range of 600-900 °C. The obtained products were composed of small nanoparticles, in the size range of 20-50 nm, depending on the annealing temperature, exhibiting a bright green up-conversion emission, under NIR laser irradiation, and emission lifetimes in the range of 4.7-18.3 μs. Their structural, morphological and spectroscopic properties were investigated in detail by XRD, HR-TEM including FFT analysis, EDX and spectroscopic techniques (emission, power dependence and emission kinetics). The luminescence quenching phenomenon, manifested in a decrease of up-conversion intensity and shortening of emission lifetime, was observed with increasing of the Yb3+ ion concentration and decreasing the particle size. The optimal concentration of the Yb3+ ions was found to be 15 mol% (YVO4: Yb3+ 15 mol%, Er3+ 2 mol%).

Effect of the CTAB concentration on the upconversion emission of ZrO 2:Er 3+ nanocrystals

NASA Astrophysics Data System (ADS)

López-Luke, T.; De la Rosa, E.; Sólis, D.; Salas, P.; Angeles-Chavez, C.; Montoya, A.; Díaz-Torres, L. A.; Bribiesca, S.

2006-10-01

Upconversion emission of ZrO 2:Er 3+ (0.2 mol%) nanophosphor were studied as function of surfactant concentration after excitation at 968 nm. The strong green emission was produced by the transition 2H 11/2 + 4S 3/2 → 4I 15/2 and was explained in terms of cooperative energy transfer between neighboring ions. The upconverted signal was enhanced but the fluorescence decay time was reduced as either the surfactant concentration increases or the annealing time reduces. Experimental results show that surfactant concentration controls the particle size and morphology while annealing time control the phase composition and crystallite size. The highest intensity was obtained for a sample composed of a mixture of tetragonal (33 wt.%) and monoclinic (67 wt.%) phase with crystallite size of 31 and 59 nm, respectively. This result suggests that tetragonal crystalline structure and small crystallite size are more favorable for the upconversion emission.

Strong emission in Yb3+/Er3+ co-doped phosphate glass ceramics

NASA Astrophysics Data System (ADS)

Liu, Yanling; Song, Feng; Jia, Guozhi; Zhang, Yanbang; Tang, Yi

Yb3+/Er3+ co-doped phosphate glass and glass ceramics were prepared by high-temperature melting method. The X-ray diffraction, transmission electron micrographs, up-conversion and infrared emissions, photothermal conversion properties of the samples have been measured. The results showed the annealing time had a great impact on the microstructure and luminous performance of the phosphate glass. At the beginning of annealing, the metaphosphate crystals were firstly dissolved out. The metaphosphate crystals gradually turned into the orthophosphate with the increasing of annealing time. The emission intensity of the sample was obviously improved after the precursor glass was annealed. The up-conversion and infrared emissions of the sample annealed at 600 °C for 24 h, reached the maximum intensity. Compared with the photothermal properties of glass, the lower photothermal conversion efficiency of the glass ceramics testified the strong emission.

Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Mengfei; Congreve, Daniel N.; Wilson, Mark W. B.

2015-11-23

Optical upconversion via sensitized triplet–triplet exciton annihilation converts incoherent low-energy photons to shorter wavelengths under modest excitation intensities1,2,3. Here, we report a solid-state thin film for infrared-to-visible upconversion that employs lead sulphide colloidal nanocrystals as a sensitizer. Upconversion is achieved from pump wavelengths beyond λ = 1 μm to emission at λ = 612 nm. When excited at λ = 808 nm, two excitons in the sensitizer are converted to one higher-energy state in the emitter at a yield of 1.2 ± 0.2%. Peak efficiency is attained at an absorbed intensity equivalent to less than one sun. We demonstrate thatmore » colloidal nanocrystals are an attractive alternative to existing molecular sensitizers, given their small exchange splitting, wide wavelength tunability, broadband infrared absorption, and our transient observations of efficient energy transfer. This solid-state architecture for upconversion may prove useful for enhancing the capabilities of solar cells and photodetectors.« less

Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Mengfei; Congreve, Daniel N.; Wilson, Mark W. B.

2015-11-23

Optical upconversion via sensitized triplet–triplet exciton annihilation converts incoherent low-energy photons to shorter wavelengths under modest excitation intensities1, 2, 3. Here, we report a solid-state thin film for infrared-to-visible upconversion that employs lead sulphide colloidal nanocrystals as a sensitizer. Upconversion is achieved from pump wavelengths beyond λ = 1 μm to emission at λ = 612 nm. When excited at λ = 808 nm, two excitons in the sensitizer are converted to one higher-energy state in the emitter at a yield of 1.2 ± 0.2%. Peak efficiency is attained at an absorbed intensity equivalent to less than one sun. Wemore » demonstrate that colloidal nanocrystals are an attractive alternative to existing molecular sensitizers, given their small exchange splitting, wide wavelength tunability, broadband infrared absorption, and our transient observations of efficient energy transfer. This solid-state architecture for upconversion may prove useful for enhancing the capabilities of solar cells and photodetectors.« less

Solid-state infrared-to-visible upconversion sensitized by colloidal nanocrystals

NASA Astrophysics Data System (ADS)

Wu, Mengfei; Congreve, Daniel N.; Wilson, Mark W. B.; Jean, Joel; Geva, Nadav; Welborn, Matthew; van Voorhis, Troy; Bulović, Vladimir; Bawendi, Moungi G.; Baldo, Marc A.

2016-01-01

Optical upconversion via sensitized triplet-triplet exciton annihilation converts incoherent low-energy photons to shorter wavelengths under modest excitation intensities. Here, we report a solid-state thin film for infrared-to-visible upconversion that employs lead sulphide colloidal nanocrystals as a sensitizer. Upconversion is achieved from pump wavelengths beyond λ = 1 μm to emission at λ = 612 nm. When excited at λ = 808 nm, two excitons in the sensitizer are converted to one higher-energy state in the emitter at a yield of 1.2 ± 0.2%. Peak efficiency is attained at an absorbed intensity equivalent to less than one sun. We demonstrate that colloidal nanocrystals are an attractive alternative to existing molecular sensitizers, given their small exchange splitting, wide wavelength tunability, broadband infrared absorption, and our transient observations of efficient energy transfer. This solid-state architecture for upconversion may prove useful for enhancing the capabilities of solar cells and photodetectors.

Biocompatible Er, Yb co-doped fluoroapatite upconversion nanoparticles for imaging applications

NASA Astrophysics Data System (ADS)

Anjana, R.; K. M., Kurias; M. K., Jayaraj

2017-08-01

Upconversion luminescence, visible emission on infra red (IR) excitation was achieved in a biocompatible material, fluoroapatite. Fluoroapatite crystals are well known biomaterials, which is a component of tooth enamel. Also it can be considered as an excellent host material for lanthanide doping since the ionic radii of lanthanide is similar to that of calcium ion(Ca2+) hence successful incorporation of dopants within the lattice is possible. Erbium (Er), Ytterbium (Yb) co-doped fluorapatite (FAp) nanoparticles were prepared by precipitation method. The particles show intense visible emission when excited with 980 nm laser. Since upconversion luminescence is a multiphoton process the excitation power dependence on emission will give number of photons involved in the emission of single photon. Excitation power dependence studies show that two photons are involved in the emission of single photons. The value of slope was different for different emission peak because of the difference in intermediate energy level involved. The crystal structure and morphology of the particle were determined using X-ray diffractometer (XRD) and field emission scanning electron microscope (FESEM). These particles with surface functionalisation can be used for live cell imaging.

Enhancement of luminescence properties in Er3+ doped TeO2-Na2O-PbX (X=O and F) ternary glasses.

PubMed

Kumar, Kaushal; Rai, S B; Rai, D K

2007-04-01

An enhancement of luminescence properties in Er3+ doped ternary glasses is observed on the addition of PbO/PbF2. The infrared to visible upconversion emission bands are observed at 410, 525, 550 and 658 nm, due to the 2H9/2-->4I15/2, 2H11/2-->4I15/2, 4S3/2-->4I15/2, 4F9/2-->4I15/2 transitions respectively, on excitation with 797 nm laser line. A detailed study reveals that the 2H9/2-->4I15/2 transition arises due to three step upconversion process while other transitions arise due to two step absorption. On excitation with 532 nm radiation, ultraviolet and violet upconversion bands centered at 380, 404, 410 and 475 nm wavelengths are observed along with one photon luminescence bands at 525, 550, 658 and 843 nm wavelengths. These bands are found due to the 4G11/2-->4I15/2, 2P3/2-->4I13/2, 2H9/2-->4I15/2, 2P3/2-->4I11/2, 2H11/2-->4I15/2, 4S3/2-->4I15/2, 4F9/2-->4I15/2 and 4S3/2-->4I13/2 transitions, respectively. Though incorporation of PbO and PbF2 both enhances fluorescence intensities however, PbF2 content has an important influence on upconversion luminescence emission. The incorporation of PbF2 enhances the red emission (658 nm) intensity by 1.5 times and the violet emission (410 nm) intensity by 2.0 times. A concentration dependence study of fluorescence reveals the rapid increase in the red (4F9/2-->4I15/2) emission intensity relative to the green (4S3/2-->4I15/2) emission with increase in the Er3+ ion concentration. This behaviour has been explained in terms of an energy transfer by relaxation between excited ions.

Structural morphology, upconversion luminescence and optical thermometric sensing behavior of Y2O3:Er(3+)/Yb(3+) nano-crystalline phosphor.

PubMed

Joshi, C; Dwivedi, A; Rai, S B

2014-08-14

Infrared-to-visible upconverting rare earths Er(3+)/Yb(3+) co-doped Y2O3 nano-crystalline phosphor samples have been prepared by solution combustion method followed by post-heat treatment at higher temperatures. A slight increase in average crystallite size has been found on calcinations verified by X-ray analysis. Transmission electron microscopy (TEM) confirms the nano-crystalline nature of the as-prepared and calcinated samples. Fourier transform infrared (FTIR) analysis shows the structural changes in as-prepared and calcinated samples. Upconversion and downconversion emission recorded using 976 and 532 nm laser sources clearly demonstrates a better luminescence properties in the calcinated samples as compared to as-prepared sample. Upconversion emission has been quantified in terms of standard chromaticity diagram (CIE) showing a shift in overall upconversion emission of as-prepared and calcinated samples. Temperature sensing behaviour of this material has also been investigated by measurement of fluorescence intensity ratio (FIR) of various signals in green emission in the temperature range of 315 to 555 K under 976 nm laser excitation. Copyright © 2014 Elsevier B.V. All rights reserved.

Synthesis of Er(III)/Yb(III)-doped BiF3 upconversion nanoparticles for use in optical thermometry.

PubMed

Du, Peng; Yu, Jae Su

2018-03-23

The authors describe an ethylene glycol assisted precipitation method for synthesis of Er(III)/Yb(III)-doped BiF 3 nanoparticles (NPs) at room temperature. Under 980-nm light irradiation, the NPs emit upconversion (UC) emission of Er(III) ions as a result of a two-photon absorption process. The temperature-dependent green emissions (peaking at 525 and 545 nm) are used to establish an unambiguous relationship between the ratio of fluorescence intensities and temperature. The NPs have a maximum sensitivity of 6.5 × 10 -3  K -1 at 619 K and can be applied over the 291-691 K temperature range. The results indicate that these NPs are a promising candidate for optical thermometry. Graphical abstract Schematic of the room-temperature preparation of Er(III)/Yb(III)-doped BiF 3 nanoparticles with strongly temperature-dependent upconversion emission.

IR Image upconversion using band-limited ASE illumination fiber sources.

PubMed

Maestre, H; Torregrosa, A J; Capmany, J

2016-04-18

We study the field-of-view (FOV) of an upconversion imaging system that employs an Amplified Spontaneous Emission (ASE) fiber source to illuminate a transmission target. As an intermediate case between narrowband laser and thermal illumination, an ASE fiber source allows for higher spectral intensity than thermal illumination and still keeps a broad wavelength spectrum to take advantage of an increased non-collinear phase-matching angle acceptance that enlarges the FOV of the upconversion system when compared to using narrowband laser illumination. A model is presented to predict the angular acceptance of the upconverter in terms of focusing and ASE spectral width and allocation. The model is experimentally checked in case of 1550-630 nm upconversion.

Upconversion luminescence from Er-N codoped of ZnO nanowires prepared by ion implantation method

NASA Astrophysics Data System (ADS)

Zhong, Kun; Xu, Jie; Su, Jing; Chen, Yu lin

2011-02-01

Nitrogen and erbium co-doped of ZnO nanowires (NWs) are fabricated by ion implantation and subsequent annealing in air. The incorporation of Er3+ and N+ ions is verified by energy dispersive X-ray spectroscopy (EDS) and Raman spectra. The samples exhibit upconversion photoluminescence around ∼550 nm and ∼660 nm under an excitation at 980 nm. It is discovered that the N-doped can drastically increase the upconversion photoluminescence intensity by modifying the local structure around Er3+ in ZnO matrix. The enhancement of the PL intensity by the N-doped is caused by the formation of ErO6-xNx octahedron complexes. With the increase of the annealing temperature (Ta), the Er3+ ions diffuse towards the surface of the NWs, which benefits the red emission and evokes the variation of intensity ratio owing to the existence of some organic groups.

Synthesis of novel branched β-NaLuF4: Yb/Er upconversion luminescence material and investigation of its optical properties

NASA Astrophysics Data System (ADS)

Ding, Yanli; Yang, Tonghui; Yin, Naiqiang; Shu, Fangjie; Zhao, Ying; Zhang, Xiaodan

2018-05-01

Branched β-NaLuF4: Yb/Er was synthesized using a simple hydrothermal method by controlling the NaF/Ln molar ratio. In contrast to the β-NaYF4: Yb/Er hexagonal disks, the branched β-NaLuF4: Yb/Er has stronger emission intensity. The integrated intensities of green and red emission bands were as 6.2 and 3.3 times as that of NaYF4, respectively. The branched β-NaLuF4: Yb/Er has the smaller unit cell volume, the higher absorption intensity around 980 nm and the lower crystal field symmetry than NaYF4, which made a significant contribution to the stronger upconversion (UC) fluorescence emissions. The results indicate that the branched β-NaLuF4: Yb/Er is an excellent UC luminescence material. The current research has a great potential in improving near-infrared conversion efficiency of solar cells.

Strong upconversion from Er3Al5O12 ceramic powders prepared by low temperature direct combustion synthesis

NASA Astrophysics Data System (ADS)

Maciel, Glauco S.; Rakov, Nikifor; Fokine, Michael; Carvalho, Isabel C. S.; Pinheiro, Carlos B.

2006-08-01

Crystalline ceramic powders of Er3Al5O12 were obtained by low temperature direct combustion synthesis. Irradiating the sample with a low-power continuous-wave infrared (1.48μm) diode laser led to ultraviolet, violet, blue, green, and red (380, 410, 456, 495, 525, 550, and 660nm) emissions. The strong upconversion luminescence appeared to the eyes as an intense green color. The presence of efficient four- and three-photon frequency upconversion processes makes this material an excellent candidate for use in photonic devices based on upconverter phosphors.

Lanthanide-doped upconversion nanocrystals: Synthesis and optical properties study

NASA Astrophysics Data System (ADS)

Sun, Qiang

Upconversion phosphor materials have attracted considerable attention in recent years for their potential applications in a wide range of fields, including three-dimensional displays technologies, bio-imaging and photovoltaics. This dissertation aims to develop novel lanthanide-doped upconversion luminescent nanomaterials by using wet chemistry methods. Considerable efforts have been devoted to manipulating the optical properties of the synthesized lanthanide-doped nanoparticles under excitation of different wavelengths, for example, 808, 980 and 1532 nm. In the first research work, a novel core-shell-shell design has been developed for finely tuning of energy migration upconversion of activators without long-lived mediated states, such as Eu3+ and Tb3+ upon excitation at 808 nm by using Nd3+ as sensitizer. Exquisite control the composition of each layer gives rise to maximized upconversion emissions of the activators. For example, with the use of core layer for energy harvesting (NaGdF4:Yb/Nd, active core), the optimal doping concentrations of Eu3+ and Tb3+ is fixed to 15 and 15 mol%, respectively. In contrast, active shell can also provide access to strong upconversion of Eu3+ and Tb3+ by doping Nd (40 mol%) into the outmost layer. Note that the effect of active shell is much stronger than active core in generating upconversion emissions of Eu3+ and Tb3+. Next, upconversion emission tuning of Er/Tm/Yb-doped NaYF4 upconversion nanoparticles has been conducted under excitation at 1532 nm. The output color of the nanoparticles is tunable by changing the doping levels of the lanthanides. With the use of core-shell design, the optical properties of the doped nanoparticles can be further optimized, for example, strongest upconversion emission was observed for NaYF4:Er(10 mol%) NaYF4:Er(0.5 mol%) with a relative emission of green-to-red of 1.2. This work provides a new dimension to control the color output of upconversion nanoparticles. It should be noted that the emission profiles of upconversion nanoparticles will be further enriched by using a combination of different excitation wavelengths. Finally, the orthorhombic-phase K2YF5 nanobelts doped with upconverting lanthanide ions (Er3+ and Tm3+) were synthesized by using a coprecipitation method. The growth kinetics of the nanobelts can be regulated by either control of the volume ratio of oleic acid in the synthetic system or period of reaction time. It was found that desirable lanthanide-doped K2YF5 nanobelts were yielded through the use of long time high-temperature annealing treatment (270 °C, 6 h) in the presence of low content of oleic acid. The assynthesized lanthanide-doped K2YF5 nanobelts show intense upconversion emissions upon excitation at 980 nm. For example, bright yellow emission was observed from K2YF5:Yb/Er(18/2 mol%), resulting from weak optical transitions of 2H11/2 → 4I15/2 (520 nm) and 4S3/2 → 4I15/2 (540 nm) and a dominant transition of 4F9/2 → 4I15/2 (centered at 650 nm) of the doped Er3+. In the case of K2YF5:Yb/Tm(30/0.5 mol%) nanobelts, three main emission bands centered at 479 (blue), 650 (red) and 800 nm (NIR) corresponding to 1D2 → 3H6, 1D2 → 3H4, and 3H4 ¨ 3H6 transition of Tm3+ were observed.

Enhancement of 800 nm upconversion emission in a thulium doped tellurite microstructured fiber pumped by a 1560 nm femtosecond fiber laser

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jia, Zhixu; Zheng, Kezhi; State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, Changchun 130012

We report enhanced upconversion (UC) fluorescence in Tm{sup 3+} doped tellurite microstructured fibers (TDTMFs) fabricated by using a rod-in-tube method. Under the pumping of a 1560 nm femtosecond fiber laser, ultrabroadband supercontinuum light expanding from ∼1050 to ∼2700 nm was generated in a 4 cm long TDTMF. Simultaneously, intense 800 nm UC emission from the {sup 3}H{sub 4} → {sup 3}H{sub 6} transition of Tm{sup 3+} was observed in the same TDTMF. Compared to that pumped by a 1560 nm continuous wave fiber laser, the UC emission intensity was enhanced by ∼4.1 times. The enhancement was due to the spectral broadening in the TDTMF under themore » pumping of the 1560 nm femtosecond fiber laser.« less

Frequency upconversion and fluorescence intensity ratio method in Yb3+-ion-sensitized Gd2O3:Er3+-Eu3+ phosphors for display and temperature sensing

NASA Astrophysics Data System (ADS)

Ranjan, Sushil Kumar; Soni, Abhishek Kumar; Rai, Vineet Kumar

2017-09-01

Near infrared (NIR) to visible frequency upconversion emission studies in Er3+-Eu3+/Er3+-Eu3+-Yb3+ co-doped/tri-doped Gd2O3 phosphors prepared by the co-precipitation technique have been explored under 980 nm laser diode radiation. The developed phosphors were characterized with the help of XRD, FE-SEM and FTIR analysis. No upconversion (UC) emission was found in the Eu3+-doped Gd2O3 phosphor. UC emission from Eu3+ ions along with Er3+ ions was observed in Er3+-Eu3+ and Er3+-Eu3+-Yb3+ co-doped/tri-doped phosphors. The UC emission arising from the Er3+ and Eu3+ ions was enhanced several times due to the incorporation of Yb3+ ions. The processes involved in the UC emission were obtained on the basis of the effect of energy transfer/sensitization through the Yb3+ → Er3+ → Eu3+ process. The red/green intensity ratio was improved from 0.16 to 1.50 and 1.01 to 1.50 for Er3+-Eu3+-Yb3+ tri-doped phosphors as compared to the Er3+-doped and Er3+-Yb3+ co-doped phosphors, respectively, at a fixed pump power density. A UC fluorescence intensity ratio (FIR)-based temperature sensing study was performed in the prepared Er3+-Eu3+-Yb3+ tri-doped Gd2O3 phosphors for green upconversion emission bands in the 300 K-443 K temperature range. A maximum sensor sensitivity of about ˜0.0043 K-1 at 300 K was achieved for the synthesized tri-doped phosphors upon excitation with a 980 nm laser diode. The colour coordinates lying in the green-yellow region are invariant, with variation in pump power density and temperature. The observed results support the utility of the prepared tri-doped phosphors in optical temperature sensing, display devices and NIR to visible upconverters.

Blue upconversion in Yb3+/Tm3+ co-doped silica fiber based on glass phase-separation technology

NASA Astrophysics Data System (ADS)

Yang, Yu; Chu, Yingbo; Chen, Zhangru; Xing, Yingbin; Hu, Xionwei; Li, Haiqing; Peng, Jinggang; Dai, Nengli; Li, Jinyan; Yang, Luyun

2018-02-01

Yb3+/Tm3+ co-doped silica fiber was prepared successfully by glass phase-separation technology. The measured refractive index profile indicated that the active fiber core had an excellent uniformity. The highest emission intensity was obtained in a sample with a Yb3+ concentration of 0.3 mol/L and a Tm3+ concentration of 0.1 mol/L. Under the excitation at 976 nm, intense blue upconversion emission of Tm3+ at 474 nm was observed due to energy transfer from Yb3+ to Tm3+. A three-photon process was responsible for the blue emission. Due to re-absorption resulted from the Tm3+:3H6→1G4 transition, the blue emission peak was red-shifted. It is suggested that the fiber preparation technology based on glass phase-separation technology can be a potential candidate for preparing active fibers with large core or complex fiber structure.

Enhancing multiphoton upconversion through energy clustering at sublattice level

NASA Astrophysics Data System (ADS)

Wang, Juan; Deng, Renren; MacDonald, Mark A.; Chen, Bolei; Yuan, Jikang; Wang, Feng; Chi, Dongzhi; Andy Hor, Tzi Sum; Zhang, Peng; Liu, Guokui; Han, Yu; Liu, Xiaogang

2014-02-01

The applications of lanthanide-doped upconversionnanocrystals in biological imaging, photonics, photovoltaics and therapeutics have fuelled a growing demand for rational control over the emission profiles of the nanocrystals. A common strategy for tuning upconversion luminescence is to control the doping concentration of lanthanide ions. However, the phenomenon of concentration quenching of the excited state at high doping levels poses a significant constraint. Thus, the lanthanide ions have to be stringently kept at relatively low concentrations to minimize luminescence quenching. Here we describe a new class of upconversion nanocrystals adopting an orthorhombic crystallographic structure in which the lanthanide ions are distributed in arrays of tetrad clusters. Importantly, this unique arrangement enables the preservation of excitation energy within the sublattice domain and effectively minimizes the migration of excitation energy to defects, even in stoichiometric compounds with a high Yb3+ content (calculated as 98 mol%). This allows us to generate an unusual four-photon-promoted violet upconversion emission from Er3+ with an intensity that is more than eight times higher than previously reported. Our results highlight that the approach to enhancing upconversion through energy clustering at the sublattice level may provide new opportunities for light-triggered biological reactions and photodynamic therapy.

Multiple Temperature-Sensing Behavior of Green and Red Upconversion Emissions from Stark Sublevels of Er³⁺.

PubMed

Cao, Baosheng; Wu, Jinlei; Wang, Xuehan; He, Yangyang; Feng, Zhiqing; Dong, Bin

2015-12-10

Upconversion luminescence properties from the emissions of Stark sublevels of Er(3+) were investigated in Er(3+)-Yb(3+)-Mo(6+)-codoped TiO₂ phosphors in this study. According to the energy levels split from Er(3+), green and red emissions from the transitions of four coupled energy levels, ²H11/2(I)/²H11/2(II), ⁴S3/2(I)/⁴S3/2(II), ⁴F9/2(I)/⁴F9/2(II), and ²H11/2(I) + ²H11/2(II)/⁴S3/2(I) + ⁴S3/2(II), were observed under 976 nm laser diode excitation. By utilizing the fluorescence intensity ratio (FIR) technique, temperature-dependent upconversion emissions from these four coupled energy levels were analyzed at length. The optical temperature-sensing behaviors of sensing sensitivity, measurement error, and operating temperature for the four coupled energy levels are discussed, all of which are closely related to the energy gap of the coupled energy levels, FIR value, and luminescence intensity. Experimental results suggest that Er(3+)-Yb(3+)-Mo(6+)-codoped TiO₂ phosphor with four pairs of energy levels coupled by Stark sublevels provides a new and effective route to realize multiple optical temperature-sensing through a wide range of temperatures in an independent system.

The Quality of In Vivo Upconversion Fluorescence Signals Inside Different Anatomic Structures.

PubMed

Wang, Lijiang; Draz, Mohamed Shehata; Wang, Wei; Liao, Guodong; Xu, Yuhong

2015-02-01

Fluorescence imaging is a broadly interesting and rapidly growing strategy for non-invasive clinical applications. However, because of interference from light scattering, absorbance, and tissue autofluorescence, the images can exhibit low sensitivity and poor quality. Upconversion fluorescence imaging, which is based on the use of near-infrared (NIR) light for excitation, has recently been introduced as an improved approach to minimize the effects of light scattering and tissue autofluorescence. This strategy is promising for ultrasensitive and deep tissue imaging applications. However, the emitted upconversion fluorescence signals are primarily in the visible range and are likely to be absorbed and scattered by tissues. Therefore, different anatomic structures could impose various effects on the quality of the images. In this study, we used upconversion-core/silica-shell nanoprobes to evaluate the quality of upconversion fluorescence at different anatomic locations in athymic nude mice. The nanoprobe contained an upconversion core, which was green (β-NaYF4:Yb3+/Ho3+) or red (β-NaYF4:Yb3+/Er3+), and a nonporous silica shell to allow for multicolor imaging. High-quality upconversion fluorescence signals were detected with signal-to-noise ratios of up to 170 at tissue depths of up to - 1.0 cm when a 980 nm laser excitation source and a bandpass emission filter were used. The presence of dense tissue structures along the imaging path reduced the signal intensity and imaging quality, and nanoprobes with longer-wavelength emission spectra were therefore preferable. This study offers a detailed analysis of the quality of upconversion signals in vivo inside different anatomic structures. Such information could be essential for the analysis of upconversion fluorescence images in any in vivo biodiagnostic and microbial tracking applications.

Co-operative energy transfer in Yb3+-Er3+ co-doped SrGdxOy upconverting phosphor

NASA Astrophysics Data System (ADS)

Kumar, Ashwini; Pathak, Trilok K.; Dhoble, S. J.; . Terblans, J. J.; Swart, H. C.

2018-04-01

Upconversion nanoparticles (UCNPs) have shown considerable interest in many fields; however, low upconversion efficiency of UCNPs is still the most severe limitation of their applications. Yb3+ and Er3+ co-doped SrGd4O7/Gd2O3(SGO) upconversion (UC) phosphors were synthesized by a modified co-precipitation process. The UC properties were investigated by direct excitation with a 980 nm laser. It was observed that the as prepared materials showed relatively strong green emission, while upon the incorporation of the Er3+ ion, there was an increase in the upconversion luminescence intensity for the red component. The effect of different doping concentration of Er3+on the emission spectra and X-ray diffraction patterns of the UC materials have also been studied. The luminescence lifetimes and Commission Internationale de L'Eclairage coordinates for these as prepared samples were determined to understand the energy transfer (ET) mechanisms occurring between Yb3+ and Er3+ in the SGO host matrix. The UC luminescence intensity as a function of laser pump power was monitored and it was confirmed that the UC process in SGO:Yb3+/Er3+is a two-photon absorption process. The findings reported here are expected to provide a better approach for understanding of the ET mechanisms in the oxide based Yb3+/Er3+ co-doped UC phosphors. This study might be helpful in precisely defined applications where optical transitions are essential criterion and this can be easily achieved by smart tuning of the emission properties of Yb3+/Er3+ co-doped UC phosphors.

Spectroscopy and visible frequency upconversion in Er3+-Yb3+: TeO2-ZnO glass.

PubMed

Mohanty, Deepak Kumar; Rai, Vineet Kumar

2014-01-01

The UV-Vis-NIR absorption studies of the Er(3+)/Er(3+)-Yb(3+) doped/codoped TeO2-ZnO (TZO) glasses fabricated by the melting and quenching method has been performed. The spectroscopic radiative parameters viz. radiative transition probabilities, branching ratios and lifetimes have been determined from the absorption spectrum by using Judd-Ofelt theory. The near infrared (NIR) to visible frequency upconversion (UC) have been monitored by using an excitation of 976 nm wavelength radiation from a CW diode laser. The effect of codoping with Yb(3+) ions on the intensity of the UC emission bands from the Er(3+) ions throughout visible region has been studied. The mechanism responsible for the observed upconversion emissions in the prepared samples have been explained on the basis of excited state absorption and efficient energy transfer processes. Copyright © 2013 Elsevier B.V. All rights reserved.

UV-visible-NIR light generation through frequency upconversion in Tm3+-doped low silica calcium aluminosilicate glasses using multiple excitation around 1.2 μm

NASA Astrophysics Data System (ADS)

Trindade, C. M.; Rego-Filho, F. G.; Astrath, N. G. C.; Jacinto, C.; Gouveia-Neto, A. S.

2018-04-01

Intense ultraviolet upconversion emission was produced in single Tm3+-doped OH--free low silica calcium aluminosilicate glasses. A new excitation route based upon multi-Stokes Raman emissions generated in an optical fiber pumped at 1.064 μm, and exploiting the absorption band around 1.2 μm by means of the 3H5 thulium excited state, was used. Furthermore, the other bands of the stimulated Raman scattering spectrum resonantly enhances all the upconversion processes, resulting in efficient ultraviolet (295 nm, 360 nm), blue (456 nm, 480 nm), red (650 nm, 667 nm), and near-infrared (800 nm) emissions. The population of the 1P0, 1D2, 1G4, 3F2 and 3H4 excited-state emitting levels was accomplished through stepwise multi-photon absorption. Results indicate competing cross-relaxation processes involving Tm3+ ion-pairs producing UV emission population quenching Simplified energy-level diagram of Tm3+- doped sample excited using multi-stokes emissions. The λp indication describes all excitation wavelengths, represented by a single arrow for the sake of simplicity.

Color Tunable and Upconversion Luminescence in Yb-Tm Co-Doped Yttrium Phosphate Inverse Opal Photonic Crystals.

PubMed

Wang, Siqin; Qiu, Jianbei; Wang, Qi; Zhou, Dacheng; Yang, Zhengwen

2016-04-01

For this paper, YPO4: Tm, Yb inverse opals with the photonic band gaps at 475 nm and 655 nm were prepared by polystyrene colloidal crystal templates. We investigated the influence of photonic band gaps on the Tm-Yb upconversion emission which was in the YPO4: Tm Yb inverse opal photonic crystals. Comparing with the reference sample, significant suppression of both the blue and red upconversion luminescence of Tm3+ ions were observed in the inverse opals. The color purity of the blue emission was improved in the inverse opal by the suppression of red upconversion emission. Additionally, mechanism of upconversion emission in the inverse opal was discussed. We believe that the present work will be valuable for not only the foundational study of upconversion emission modification but also the development of new optical devices in upconversion lighting and display.

Enhancement of luminescence emission from GdVO{sub 4}:Er{sup 3+}/Yb{sup 3+} phosphor by Li{sup +} co-doping

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gavrilović, Tamara V.; Jovanović, Dragana J., E-mail: draganaj@vinca.rs; Lojpur, Vesna M.

2014-09-15

This paper demonstrates the effects of Li{sup +} co-doping on the structure, morphology, and luminescence properties of GdVO{sub 4}:Er{sup 3+}/Yb{sup 3+} phosphor prepared using a high-temperature solid-state chemistry method. The GdVO{sub 4}:Er{sup 3+}/Yb{sup 3+} powders synthesized with the Li{sup +} co-dopant (in concentrations of 0, 5, 10, and 15 mol%) are characterized by X-ray powder diffraction, scanning electron microscopy, and photoluminescence spectroscopy. Structural analysis showed that powders co-doped with Li{sup +} have larger crystallite sizes and slightly smaller crystal lattice parameters than powders prepared without Li{sup +} ions. Photoluminescence down-conversion (345-nm excitation) and up-conversion (980-nm excitation) spectra show characteristic Er{supmore » 3+} emissions, with the most intense bands peaking at 525 nm ({sup 2}H{sub 11/2}→{sup 4}I{sub 15/2} transition) and 552 nm ({sup 4}S{sub 3/2}→{sup 4}I{sub 15/2}). The intensity of up-conversion emission from GdVO{sub 4}:Er{sup 3+}/Yb{sup 3+} is enhanced (by a factor of four) by co-doping with 5 mol% of Li{sup +} ions. The mechanisms responsible for this emission enhancement are discussed. - Graphical abstract: UC emission spectra for GdVO{sub 4}:1.5-mol% Er{sup 3+}/20-mol% Yb{sup 3+} powders co-doped with different concentrations of Li{sup +} ions, recorded under 980-nm excitation. - Highlights: • 5-mol% Li{sup +} co-doped powders have 400% enhanced up-conversion emission intensity. • 15-mol% Li{sup +} co-doping produces 40% higher emission in down-conversion. • Li{sup +} co-doped powders have larger crystallite size and smaller lattice parameters.« less

Amplified stimulated emission in upconversion nanoparticles for super-resolution nanoscopy

NASA Astrophysics Data System (ADS)

Liu, Yujia; Lu, Yiqing; Yang, Xusan; Zheng, Xianlin; Wen, Shihui; Wang, Fan; Vidal, Xavier; Zhao, Jiangbo; Liu, Deming; Zhou, Zhiguang; Ma, Chenshuo; Zhou, Jiajia; Piper, James A.; Xi, Peng; Jin, Dayong

2017-02-01

Lanthanide-doped glasses and crystals are attractive for laser applications because the metastable energy levels of the trivalent lanthanide ions facilitate the establishment of population inversion and amplified stimulated emission at relatively low pump power. At the nanometre scale, lanthanide-doped upconversion nanoparticles (UCNPs) can now be made with precisely controlled phase, dimension and doping level. When excited in the near-infrared, these UCNPs emit stable, bright visible luminescence at a variety of selectable wavelengths, with single-nanoparticle sensitivity, which makes them suitable for advanced luminescence microscopy applications. Here we show that UCNPs doped with high concentrations of thulium ions (Tm3+), excited at a wavelength of 980 nanometres, can readily establish a population inversion on their intermediate metastable 3H4 level: the reduced inter-emitter distance at high Tm3+ doping concentration leads to intense cross-relaxation, inducing a photon-avalanche-like effect that rapidly populates the metastable 3H4 level, resulting in population inversion relative to the 3H6 ground level within a single nanoparticle. As a result, illumination by a laser at 808 nanometres, matching the upconversion band of the 3H4 → 3H6 transition, can trigger amplified stimulated emission to discharge the 3H4 intermediate level, so that the upconversion pathway to generate blue luminescence can be optically inhibited. We harness these properties to realize low-power super-resolution stimulated emission depletion (STED) microscopy and achieve nanometre-scale optical resolution (nanoscopy), imaging single UCNPs; the resolution is 28 nanometres, that is, 1/36th of the wavelength. These engineered nanocrystals offer saturation intensity two orders of magnitude lower than those of fluorescent probes currently employed in stimulated emission depletion microscopy, suggesting a new way of alleviating the square-root law that typically limits the resolution that can be practically achieved by such techniques.

Singlet oxygen generation of photosensitizers effectively activated by Nd3+-doped upconversion nanoparticles of luminescence intensity enhancing with shell thickness decreasing

NASA Astrophysics Data System (ADS)

Zou, Haixia; Jin, Fengmin; Song, Xiaoyan; Xing, Jinfeng

2017-04-01

The introduction of a thick shell structure has been widely used to enhance the emission intensity of upconversion nanoparticles (UCNPs). However, a thick shell could increase the distance between UCNPs and photosensitizers, which is not favourable to the generation of singlet oxygen (1O2) in photodynamic therapy (PDT) due to the low fluorescence resonance energy transfer (FRET) efficiency. In this study, we used a facile method to prepare UCNPs that the emission intensity could increase with the shell thickness decreasing, which facilitated the efficient FRET between UCNPs and photosensitizers. In detail, the Nd3+-doped UCNPs with different dopant concentration of Yb3+ were prepared and characterized firstly. The Ir/g (intensity of red luminescence to green luminescence) was tuned to increase largely by precisely controlling Yb3+ concentration in core-shell, which could make UCNPs effectively activate methylene blue (MB). Then, a unique procedure was used to prepare NaYF4:Yb/Er/Nd@NaYF4:Nd (Yb3+:30%) core-shell nanoparticles with different shell thickness by tuning the amount of the core. The upconversion luminescence (UCL) intensity of those UCNPs enhanced dramatically with the shell thickness decreasing. Furthermore, UCNPs and MB were encapsulated into SiO2 nanoparticles. FRET efficiency between UCNPs and MB largely increased with the shell thickness of UCNPs decreasing. Correspondingly, the efficiency of 1O2 generation obviously increased. We provided a new method to optimize the UCL intensity and FRET efficiency at the same time to produce 1O2 efficiently.

Optical thermometry through infrared excited green upconversion in monoclinic phase Gd2(MoO4)3:Yb3+/Er3+ phosphor

NASA Astrophysics Data System (ADS)

Xu, Weijiang; Li, Dongyu; Hao, Haoyue; Song, Yinglin; Wang, Yuxiao; Zhang, Xueru

2018-04-01

Monoclinic phase Gd2(MoO4)3: Yb3+/Er3+ phosphor is synthesized via a simple sol-gel method. The XRD result reveals that the phosphor possesses monoclinic structure with space group C2/c(15). Under the excitation of a 980 nm laser, its emission spectra shows remarkably intense green and negligible red emissions, which are all two-photon process. By investigating effect of temperature on green emission of the sample, the competition between the thermal agitation and non-radiative relaxation of 2H11/2 level can be found, which is verified by the measurement of lifetime. In addition, the sensitivity of optical thermometry is studied based on the fluorescence intensity ratio technique through infrared excited green upconversion. The maximum sensitivity is found to be about 0.02574 K-1 at 510.2 K, suggesting that the phosphor can be used as an excellent material for optical temperature sensing.

Mechanisms and concentrations dependence of up-conversion luminescence in Tm^3^+/Yb^3^+ codoped oxyfluoride glass-ceramics [rapid communication

NASA Astrophysics Data System (ADS)

Zhang, Junjie; He, Dongbing; Duan, Zhongchao; Zhang, Liyan; Dai, Shixun; Hu, Lili

2005-04-01

The up-conversion properties of Tm3+/Yb3+ codoped oxyfluoride glass-ceramics under 980 nm excitation were investigated. Intense blue up-conversion luminescence due to the Tm3+: 1G4 → 3H6 transition was observed in the glass-ceramics. The intensity of the blue up-conversion luminescence in a 1 mol% YbF3-containing glass-ceramic was found to be about 40 times stronger than that in the precursor oxyfluoride glass. The up-conversion mechanism is proposed. The reason for the intense Tm3+ up-conversion luminescence in the oxyfluoride glass-ceramics and the concentrations dependence of upconversion luminescence are also discussed.

Temperature dependence of luminescence behavior in Er3+-doped BaY2F8 single crystal

NASA Astrophysics Data System (ADS)

Wang, Shuai; Ruan, Yongfeng; Tsuboi, Taiju; Tong, Hongshuang; Wang, Youfa; Zhang, Shouchao

2013-12-01

BaY2F8 single crystals doped with Er3+ ions have been grown by the temperature gradient method. The absorption, excitation and emission spectra for Er3+-doped BaY2F8 crystals were measured at room temperature (297 K) and 12 K. The effect of temperature on the luminescence intensity and effective bandwidth was investigated in the range of 12-297 K. The temperature dependence of the fluorescence intensity ratio (FIR) for the 522 nm emission (2H11/2→4I15/2 transition) and the 552 nm emission (4S3/2→4I15/2 transition) was also studied in the range of 12-297 K. Based on the fitting FIR curve, the value of the constant term B (2.25) was obtained. The fitting FIR curve and FIR equation may have a potential application in the temperature measurement. In addition, the up-conversion spectrum at room temperature was recorded under excitation of 980 nm and the up-conversion mechanism was analyzed in detail.

Effect of B2O3 on luminescence of erbium doped tellurite glasses.

PubMed

Shen, Xiang; Nie, Qiuhua; Xu, Tiefeng; Dai, Shixun; Wang, Xunsi

2007-02-01

The B2O3 was introduced into the Er3+ doped TeO2-ZnO-Na2O glass to increase the phonon energy of the host. The effect of B2O3 on the non-radiative rate of the 4I11/2-->4I13/2 transition of Er3+, the lifetime of the 4I11/2 and 4I13/2 levels, the green and red upconversion emissions intensity, and the 4I13/2-->4I15/2 emission intensity was discussed. The results show that the phonon energy of boro-tellurite glass is close to that of germanate glass and is quite smaller than that of borate glass. The lifetime of 4I11/2 level and the upconversion emissions decrease with increasing B2O3 concentration. The higher OH group concentration presented in the boro-tellurite glass may shorten the lifetime of 4I13/2 level and also reduce the quantum efficiency of 4I13/2-->4I15/2 emission. The future dehydrating procedures are suggested to enhance the efficiency of amplification at 1.5 microm band.

Enhancement of red upconversion emission of cubic phase NaLuF{sub 4}: Yb{sup 3+}/Ho{sup 3+}/Ce{sup 3+} nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Wei, E-mail: gaowei@xupt.edu.com; Dong, Jun, E-mail: dongjun@xupt.edu.cn; Liu, Jihong

Highlights: • The upconversion emission of Ho{sup 3+} ions was tuned from green to red. • The upconversion mechanism of Ho{sup 3+} ions was discussed based on emission spectrum. • The conversion efficiency between Ho{sup 3+} and Ce{sup 3+} were studied and calculated. - Abstract: The red upconversion emission of lanthanide-doped fluoride nanocrystals have great potential applications in color display and anticounterfeiting applications, especially for biological imaging and biomedical. In this work, a significant enhancement of red upconversion emission of Ho{sup 3+} ions was successfully obtained in the cubic phase NaLuF{sub 4} nanocrystals through codoping Ce{sup 3+} ions under NIRmore » 980 nm excitation. The ratio of red-to-green emission of Ho{sup 3+} ions was enhanced about 10-fold, which is due to two efficient cross relaxation processes derived from Ho{sup 3+} and Ce{sup 3+} ions promoted the red emission and quenched the green emission. The upconversion emission and luminescent colors of NaLuF{sub 4}: Yb{sup 3+}/Ho{sup 3+} nanocrystals were carefully investigated by a confocal microscopy setup. The possible upconversion emission mechanism and conversion efficiency of cross relaxation between Ho{sup 3+} and Ce{sup 3+} ions were discussed in detail. The current study suggests that strong red emission of NaLuF{sub 4}: Yb{sup 3+}/Ho{sup 3+}/Ce{sup 3+} nanomaterials can be used for color display and anticounterfeiting techniques.« less

Effect of various surfactants on changes in the emission color chromaticity in upconversion YVO4: Yb3+, Er3+ nanoparticles

NASA Astrophysics Data System (ADS)

Woźny, Przemysław; Szczeszak, Agata; Lis, Stefan

2018-02-01

YVO4: Yb3+,Er3+ upconverting nanocrystals were synthesized via a hydrothermal method using different compounds as surfactants. Structure and morphology of the nanocrystals were investigated by X-ray diffraction and transmission electron microscopy. Tetragonal crystal structure of the nanocrystals appeared irrespective of the type of surfactant used. The average crystallite size was estimated by TEM images. The obtained products were composed of small nanoparticles, in the size range of 10-60 nm, depending on the surfactant used. The morphology of the nanoparticles was also regulated by the type of surfactant. Spectroscopic analysis of the materials obtained was carried out by measuring the emission and excitation spectra and the intensity of luminescence as a function of laser energy and luminescence decays. The nanocrystals prepared exhibited a green upconversion emission attributed to the 2H11/2 → 4I15/2 and 4S3/2 → 4I15/2 transitions of Er3+, under NIR (985 nm) pulse laser irradiation, and their emission lifetimes were in the range 3.84-4.90 μs. On the basis of the spectroscopic investigation, the upconversion mechanism was proposed and chromaticity coordinates were calculated. Surfactants were found to influence on chromaticity of luminescence.

Enhancement of a-Si:H solar cell efficiency by Y2O3 : Yb3+, Er3+ near infrared spectral upconverter

NASA Astrophysics Data System (ADS)

Markose, Kurias K.; Anjana, R.; Subha, P. P.; Antony, Aldrin; Jayaraj, M. K.

2016-09-01

The optical properties of Yb3+/Er3+ doped Y2O3 upconversion phosphor and the enhancement of efficiency of a-Si:H solar cell on incorporation of upconverter are investigated. The Y2O3 host material has high corrosion resistance, thermal stability, chemical stability, low toxicity and relatively low phonon energy (≈ 500 cm-1). Y2O3:Yb3+ (x %): Er3+ (y %) upconversion nanophosphors with different dopant concentrations were synthesized via simple hydrothermal method followed by a heat treatment at 1200°C for 12 hrs. Highly crystalline, quasi-spherical, body centered cubic Y2O3 structure was obtained. The structure, phase and morphology of the nanocrystals were determined using x-ray diffraction and SEM. Following pumping at 980 nm two dominant emission bands were observed at about 550 nm(green) and 660 nm(red), corresponding to 2H11/2, 4S3/2 -> 4I15/2 and 4F9/2 -> 4I15/2 transitions respectively. The dependence of emission intensity on pump power shows that the mechanism involved is two photon absorption. The upconversion phosphor along with a binder is coupled behind the a-Si:H solar cell which absorbs transmitted sub-band-gap photons and emits back the upconverted visible light which can be absorbed by the solar cell. Under suitable intensity of illumination the solar cell short circuit current is found to be increased on adding the upconversion layer.

The upconversion luminescence and magnetism in Yb3+/Ho3+ co-doped LaF3 nanocrystals for potential bimodal imaging

NASA Astrophysics Data System (ADS)

Syamchand, Sasidharanpillai S.; George, Sony

2016-12-01

Biocompatible upconversion nanoparticles with multifunctional properties can serve as potential nanoprobes for multimodal imaging. Herein, we report an upconversion nanocrystal based on lanthanum fluoride which is developed to address the imaging modalities, upconversion luminescence imaging and magnetic resonance imaging (MRI). Lanthanide ions (Yb3+ and Ho3+) doped LaF3 nanocrystals (LaF3 Yb3+/Ho3+) are fabricated through a rapid microwave-assisted synthesis. The hexagonal phase LaF3 nanocrystals exhibit nearly spherical morphology with average diameter of 9.8 nm. The inductively coupled plasma mass spectrometry (ICP-MS) analysis estimated the doping concentration of Yb3+ and Ho3+ as 3.99 and 0.41%, respectively. The nanocrystals show upconversion luminescence when irradiated with near-infrared (NIR) photons of wavelength 980 nm. The emission spectrum consists of bands centred at 542, 645 and 658 nm. The stronger green emission at 542 nm and the weak red emissions at 645 and 658 nm are assigned to 5S2 → 5I8 and 5F5 → 5I8 transitions of Ho3+, respectively. The pump power dependence of luminescence intensity confirmed the two-photon upconversion process. The nanocrystals exhibit paramagnetism due to the presence of lanthanide ion dopant Ho3+ and the magnetization is 19.81 emu/g at room temperature. The nanocrystals exhibit a longitudinal relaxivity ( r 1) of 0.12 s-1 mM-1 and transverse relaxivity ( r 2) of 28.18 s-1 mM-1, which makes the system suitable for developing T2 MRI contrast agents based on holmium. The LaF3 Yb3+/Ho3+ nanocrystals are surface modified by PEGylation to improve biocompatibility and enhance further functionalisation. The PEGylated nanocrystals are found to be non-toxic up to 50 μg/mL for 48 h of incubation, which is confirmed by the MTT assay as well as morphological studies in HeLa cells. The upconversion luminescence and magnetism together with biocompatibility enables the adaptability of the present system as a nanoprobe for potential bimodal imaging.

Security writing application of thermal decomposition assisted NaYF4:Er3+/Yb3+ upconversion phosphor

NASA Astrophysics Data System (ADS)

Kumar, A.; Tiwari, S. P.; Esteves da Silva, Joaquim C. G.; Kumar, K.

2018-07-01

The authors have synthesized water-dispersible NaYF4:Er3+/Yb3+ upconversion particles via a thermal decomposition route and optimized the green upconversion emission through a concentration variation of the Yb3+ sensitizer. The prepared particles were found to be ellipsoid in shape having an average particle dimension of 600  ×  150 nm. It is observed that the sample with 18 mmol% Yb3+ ion concentration and 2 mmol% Er3+ ion gives optimum upconversion intensity in the green region under 980 nm excitation. Colloidal dispersibility of the sample in different solvents was checked and hexane was found to be the best medium for the prepared particles. The particle size of the sample was found to be suitable for the preparation of colloidal ink and security writing on a plain sheet of paper. This was demonstrated successfully using ink prepared in polyvinyl chloride gold medium.

Synergistic plasmonic and photonic crystal light-trapping: architectures for optical up-conversion in thin-film solar cells.

PubMed

Le, Khai Q; John, Sajeev

2014-01-13

We demonstrate, numerically, that with a 60 nanometer layer of optical up-conversion material, embedded with plasmonic core-shell nano-rings and placed below a sub-micron silicon conical-pore photonic crystal it is possible to absorb sunlight well above the Lambertian limit in the 300-1100 nm range. With as little as 500 nm, equivalent bulk thickness of silicon, the maximum achievable photo-current density (MAPD) is about 36 mA/cm2, using above-bandgap sunlight. This MAPD increases to about 38 mA/cm2 for one micron of silicon. Our architecture also provides solar intensity enhancement by a factor of at least 1400 at the sub-bandgap wavelength of 1500 nm, due to plasmonic and photonic crystal resonances, enabling a further boost of photo-current density from up-conversion of sub-bandgap sunlight. With an external solar concentrator, providing 100 suns, light intensities sufficient for significant nonlinear up-conversion can be realized. Two-photon absorption of sub-bandgap sunlight is further enhanced by the large electromagnetic density of states in the photonic crystal at the re-emission wavelength near 750 nm. It is suggested that this synergy of plasmonic and photonic crystal resonances can lead to unprecedented power conversion efficiency in ultra-thin-film silicon solar cells.

Time delay and excitation mode induced tunable red/near-infrared to green emission ratio of Er doped BiOCl

NASA Astrophysics Data System (ADS)

Avram, Daniel; Florea, Mihaela; Tiseanu, Ion; Tiseanu, Carmen

2015-09-01

Herein, we report on the emission color tunability of Er doped BiOCl measured under up—conversion as well as x-ray excitation modes. The dependence of red (670 nm) to green emission (543 nm) ratio on Er concentration (1 and 5%), excitation wavelength into different (656.4, 802 and 976 nm) or across single Er absorption levels (965 ÷ 990 nm) and delay after the laser pulse (0.001 ÷ 1 ms) is discussed in terms of ground state absorption/excited state absorption and energy transfer up-conversion mechanisms. A first example of extended Er x-ray emission measured in the range of 500 to 1700 nm shows comparable emission intensities corresponding to 543 nm and 1500 nm based transitions. The present results together with our earlier report on the upconversion emission of Er doped BiOCl excited at 1500 nm, suggest that Er doped BiOCl may be considered an attractive system for optical and x-ray imaging applications.

Core-shell-shell heterostructures of α-NaLuF4:Yb/Er@NaLuF4:Yb@MF2 (M = Ca, Sr, Ba) with remarkably enhanced upconversion luminescence.

PubMed

Su, Yue; Liu, Xiuling; Lei, Pengpeng; Xu, Xia; Dong, Lile; Guo, Xianmin; Yan, Xingxu; Wang, Peng; Song, Shuyan; Feng, Jing; Zhang, Hongjie

2016-07-05

Core-shell-shell heterostructures of α-NaLuF4:Yb/Er@NaLuF4:Yb@MF2 (M = Ca, Sr, Ba) have been successfully fabricated via the thermal decomposition method. Upconversion nanoparticles (UCNPs) were characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), upconversion luminescence (UCL) spectroscopy, etc. Under 980 nm excitation, the emission intensities of the UCNPs are remarkably enhanced after coating the MF2 (M = Ca, Sr, and Ba) shell. Among these samples, CaF2 coated UCNPs show the strongest overall emission, while BaF2 coated UCNPs exhibit the longest lifetime. These results demonstrate that alkaline earth metal fluorides are ideal materials to improve the UCL properties. Meanwhile, although the lattice mismatch between the ternary NaREF4 core and the binary MF2 (M = Sr and Ba) shell is relatively large, the successfully synthesized NaLuF4:Yb/Er@NaLuF4:Yb@MF2 indicates a new outlook on the fabrication of heterostructural core-shell UCNPs.

Gold decorated NaYF4:Yb,Er/NaYF4/silica (core/shell/shell) upconversion nanoparticles for photothermal destruction of BE(2)-C neuroblastoma cells

NASA Astrophysics Data System (ADS)

Qian, Li Peng; Zhou, Li Han; Too, Heng-Phon; Chow, Gan-Moog

2011-02-01

Gold decorated NaYF4:Yb,Er/NaYF4/silica (core/shell/shell) upconversion (UC) nanoparticles ( 70-80 nm) were synthesized using tetraethyl orthosilicate and chloroauric acid in a one-step reverse microemulsion method. Gold nanoparticles ( 6 nm) were deposited on the surface of silica shell of these core/shell/shell nanoparticles. The total upconversion emission intensity (green, red, and blue) of the core/shell/shell nanoparticles decreased by 31% after Au was deposited on the surface of silica shell. The upconverted green light was coupled with the surface plasmon of Au leading to rapid heat conversion. These UC/silica/Au nanoparticles were very efficient to destroy BE(2)-C cancer cells and showed strong potential in photothermal therapy.

1.319 μm excited intense 800 nm frequency upconversion emission in Tm{sup 3+}-doped fluorogermanate glass

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gouveia-Neto, A. S.; Vermelho, M. V. D.; Gouveia, E. A.

2015-11-23

Generation of near-infrared light within the first biological optical window via frequency upconversion in Tm{sup 3+}-doped PbGeO{sub 3}-PbF{sub 2}-CdF{sub 2} glass excited within the second biological window at 1.319 μm is reported. The upconversion emission at 800 nm is the sole light signal observed in the entire ultraviolet-visible-near-infrared spectral region making it possible obtaining high contrast imaging. The dependence of the 800 nm signal upon the sample temperature was investigated and results showed an increase by a factor of ×2.5 in the 30–280 °C range. Generation of detectable 690 nm for temperatures above 100 °C in addition to the intense 800 nm main signal was also observed.more » The proposed excitation mechanism for the 800 nm thulium emitting level is assigned to a multiphonon-assisted excitation from the ground-state {sup 3}H{sub 6} to the {sup 3}H{sub 5} excited-state level, a rapid relaxation to the {sup 3}F{sub 4} level and followed by an excited-state absorption of the pump photons mediated by multiphonons connecting the {sup 3}F{sub 4} level to the {sup 3}H{sub 4} emitting level.« less

Scalable Direct Writing of Lanthanide-Doped KMnF3 Perovskite Nanowires into Aligned Arrays with Polarized Up-Conversion Emission.

PubMed

Shi, Shuo; Sun, Ling-Dong; Xue, Ying-Xian; Dong, Hao; Wu, Ke; Guo, Shi-Chen; Wu, Bo-Tao; Yan, Chun-Hua

2018-05-09

The use of one-dimensional nano- and microstructured semiconductor and lanthanide materials is attractive for polarized-light-emission studies. Up-conversion emission from single-nanorod or anisotropic nanoparticles with a degree of polarization has also been discussed. However, microscale arrays of nanoparticles, especially well-aligned one-dimensional nanostructures as well as their up-conversion polarization characterization, have not been investigated yet. Herein, we present a novel and facile paradigm for preparing highly aligned arrays of lanthanide-doped KMnF 3 (KMnF 3 :Ln) perovskite nanowires, which are good candidates for polarized up-conversion emission studies. These perovskite nanowires, with a width of 10 nm and length of a few micrometers, are formed through the oriented attachment of KMnF 3 :Ln nanocubes along the [001] direction. By the employment of KMnF 3 :Ln nanowire gel as nanoink, a direct-writing method is developed to obtain diverse types of aligned patterns from the nanoscale to the wafer scale. Up-conversion emissions from the highly aligned nanowire arrays are polarized along the array direction with a polarization degree up to 60%. Taking advantage of microscopic nanowire arrays, these polarized up-conversion emissions should offer potential applications in light or information transportation.

Quadratic general rotary unitized design for doping concentrations and up-conversion luminescence properties of Er{sup 3+}/Yb{sup 3+} co-doped NaLa(MoO{sub 4}){sub 2} phosphors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Jiashi, E-mail: sunjs@dlmu.edu.cn; Shi, Linlin; Li, Shuwei

Highlights: • NaLa(MoO4)2: Er3+/Yb3+ phosphor is synthesized by solid state method. • QGRUD is first applied to the codoping concentration option. • Optimized phosphor presents more stable UC emissions than the commercial phosphor. - Abstract: It is still a great challenge that designing proper codoping concentrations of rare earth ions for achieving intensest expected emission from the studied phosphor. In this work, the quadratic general rotary unitized design (QGRUD) was introduced into the codoping concentration option of NaLa(MoO{sub 4}){sub 2}: Er{sup 3+}/Yb{sup 3+} phosphor for upconversion (UC) applications, and the optimum doping concentrations of Er{sup 3+} and Yb{sup 3+} formore » achieving maximum UC luminescence intensity, which is close to commercial NaYF{sub 4}:Er{sup 3+}/Yb{sup 3+} phosphor, were obtained. The two-photon process was assigned to the green UC emissions in the optimized NaLa(MoO{sub 4}){sub 2}: Er{sup 3+}/Yb{sup 3+} phosphor. It was also demonstrated that the optimized phosphor presented more stable upconversion emissions than the commercial NaYF{sub 4}:Er{sup 3+}/Yb{sup 3+} phosphor.« less

Enhanced red emission of 808 nm excited upconversion nanoparticles by optimizing the composition of shell for efficient generation of singlet oxygen

NASA Astrophysics Data System (ADS)

Liu, Jinxue; Zhang, Tingbin; Song, Xiaoyan; Xing, Jinfeng

2018-01-01

With the aim to enhance the upconversion luminescence (UCL) intensity, much attention was paid to reduce the energy-back transfer from Er3+ ions to Nd3+ ions by constructing various kinds of multilayer upconversion nanoparticles (UCNPs). However, the energy-back transfer was difficult to be completely eliminated. Also, the thick shell of multilayer UCNPs is not favourable for effective Förster resonance energy transfer (FRET) in photodynamic therapy (PDT) system. Herein, an effective and facile method was applied to prepare UCNPs by optimizing the composition to largely enhance the red emission (at 660 nm) for efficient generation of singlet oxygen (1O2). In detail, the concentrations of Nd3+ ions and Yb3+ ions doped in the sensitizing shell were systematically researched to balance the energy back-transfer and the light harvest ability. The optimal emission and a relatively high Red/Green (R/G) ratio of NaYF4:Yb,Er,Nd@NaYF4:Yb0.1Nd0.2 UCNPs were obtained simultaneously. Furthermore, the emission under 980 nm excitation demonstrated the energy back-transfer from Er3+ to Yb3+ ions was also notable which was largely ignored previously. Then, UCNPs were encapsulated into mesoporous silica shell, and the photosensitizer Chlorin e6 (Ce6) was covalently conjugated to form a non-leaking nanoplatform. The efficiency of 1O2 generation obviously increased with the enhanced emission of UCNPs.

Monitoring Delamination of Thermal Barrier Coatings by Near-Infrared and Upconversion Luminescence Imaging

NASA Technical Reports Server (NTRS)

Eldridge, J. I.; Martin, R. E.; Singh, Jogender; Wolfe, Doug E.

2008-01-01

Previous work has demonstrated that TBC delamination can be monitored by incorporating a thin luminescent sublayer that produces greatly increased luminescence intensity from delaminated regions of the TBC. Initial efforts utilized visible-wavelength luminescence from either europium or erbium doped sublayers. This approach exhibited good sensitivity to delamination of electron-beam physical-vapor-deposited (EB-PVD) TBCs, but limited sensitivity to delamination of the more highly scattering plasma-sprayed TBCs due to stronger optical scattering and to interference by luminescence from rare-earth impurities. These difficulties have now been overcome by new strategies employing near-infrared (NIR) and upconversion luminescence imaging. NIR luminescence at 1550 nm was produced in an erbium plus ytterbium co-doped yttria-stabilized zirconia (YSZ) luminescent sublayer using 980-nm excitation. Compared to visible-wavelength luminescence, these NIR emission and excitation wavelengths are much more weakly scattered by the TBC and therefore show much improved depth-probing capabilities. In addition, two-photon upconversion luminescence excitation at 980 nm wavelength produces luminescence emission at 562 nm with near-zero fluorescence background and exceptional contrast for delamination indication. The ability to detect TBC delamination produced by Rockwell indentation and by furnace cycling is demonstrated for both EB-PVD and plasma-sprayed TBCs. The relative strengths of the NIR and upconversion luminescence methods for monitoring TBC delamination are discussed.

Optical properties of Mg2+, Yb3+, and Ho3+ tri-doped LiNbO3 crystals

NASA Astrophysics Data System (ADS)

Dai, Li; Liu, Chun-Rui; Tan, Chao; Yan, Zhe-Hua; Xu, Yu-Heng

2017-04-01

A series of LiNbO3 crystals tri-doped with Mg{}2+, Yb{}3+, and Ho{}3+ are grown by the conventional Czochraski technique. The concentrations of Mg{}2+, Yb{}3+, and Ho{}3+ ions in Mg:Yb:Ho:LiNbO3 crystals are measured by using an inductively coupled plasma atomic emission spectrometry. The x-ray diffraction is proposed to determine the lattice constant and analyze the internal structure of the crystal. The light-induced scattering of Mg:Yb:Ho:LiNbO3 crystal is quantitatively described via the threshold effect of incident exposure energy flux. The exposure energy ({E}{{r}}) is calculated to discuss the optical damage resistance ability. The exposure energy of Mg(7 mol):Yb:Ho:LiNbO3 crystal is 709.17 J/cm2, approximately 425 times higher than that of the Mg(1 mol):Yb:Ho:LiNbO3 crystal in magnitude. The blue, red, and very intense green bands of Mg:Yb:Ho:LiNbO3 crystal are observed under the 980-nm laser excitation to evaluate the up-conversion emission properties. The dependence of the emission intensity on pumping power indicates that the up-conversion emission is a two-photon process. The up-conversion emission mechanism is discussed in detail. This study indicates that Mg:Yb:Ho:LiNbO3 crystal can be applied to the fabrication of new multifunctional photoluminescence devices. Project supported by the National Natural Science Foundation of China (Grant No. 51301055), the Youth Science Fund of Heilongjiang Province, China (Grant No. QC2015061), the Special Funds of Harbin Innovation Talents in Science and Technology Research, China (Grant No. 2015RQQXJ045 ), and the Science Funds for the Young Innovative Talents of Harbin University of Science and Technology, China (Grant No. 201501).

A fruitful demonstration in sensors based on upconversion luminescence of Yb3+/Er3+codoped Sb2O3-WO3-Li2O (SWL) glass-ceramic

NASA Astrophysics Data System (ADS)

Prasad Sukul, Prasenjit; Kumar, Kaushal

2016-07-01

In this article, erbium and ytterbium doped lithium tungsten antimonate (Yb3+/Er3+:Sb2O3-WO3-Li2O) glass-ceramics (GC) is synthesized and its novel applications in temperature sensing and detection of latent fingerprints is studied. It is also estimated that this material could be useful as a solar cell concentrator. The upconversion emission studies on Yb3+/Er3+:SWL glass-ceramics have shown intense green emission at 525 nm (2H11/2 → 4I15/2) & 545 nm (4s3/2 → 4I15/2). The variation of UC intensities with external temperature have shown a well-fashioned pattern, which suggests that the 2H11/2 and 4S3/2 levels of Er3+ ion are thermally coupled and can act as a temperature sensor in the 300-500 K temperature range. Dry powder of Yb3+/Er3+:SWL glass-ceramic is used to develop latent fingerprint with high contrast in green color on glass slide.

Near-infrared-emitting colloidal Ag2S quantum dots exhibiting upconversion luminescence

NASA Astrophysics Data System (ADS)

Zhang, Yanyan; Jiang, Danyu; Yang, Wei; Wang, Dandan; Zheng, Huiping; Du, Yuansheng; Li, Xi; Li, Qiang

2017-02-01

Ag2S quantum dots (QDs) coated with thioglycolic acid (Ag2S QDs-TGA) have been synthesized in an organic solvent via a stepwise addition of reagents. When excited by a 980 nm laser, the near-infrared-emitting colloidal Ag2S QDs-TGA exhibit upconversion luminescence (UCL). The observed photoluminescence (PL) was attributed to the presence of ligand-modified Ag2S on the QD surfaces. Hence, upon dilution of the solution, the PL intensity initially increased before subsequently decreasing, accompanied by a blue shift in the PL spectra. The PL phenomena can be attributed to the increase in the amount of ligand-modified Ag2S on the QD surfaces upon dilution, which in turn affected the fluorescence resonance energy transfer (FRET) and re-emission of the surface energy level. The relations between the emission intensity of Ag2S QDs-TGA and the excitation power are investigated, and the results confirm that the UCL in Ag2S QDs-TGA can be ascribed to a two-photon-assisted absorption process via a real energy state.

The Upconversion Luminescence of Er3+/Yb3+/Nd3+ Triply-Doped β-NaYF4 Nanocrystals under 808-nm Excitation

PubMed Central

Tian, Lijiao; Xu, Zheng; Zhao, Suling; Cui, Yue; Liang, Zhiqin; Zhang, Junjie; Xu, Xurong

2014-01-01

In this paper, Nd3+–Yb3+–Er3+-doped β-NaYF4 nanocrystals with different Nd3+ concentrations are synthesized, and the luminescence properties of the upconversion nanoparticles (UCNPs) have been studied under 808-nm excitation for sensitive biological applications. The upconversion luminescence spectra of NaYF4 nanoparticles with different dopants under 808-nm excitation proves that the Nd3+ ion can absorb the photons effectively, and the Yb3+ ion can play the role of an energy-transfer bridging ion between the Nd3+ ion and Er3+ ion. To investigate the effect of the Nd3+ ion, the decay curves of the 4S3/2 → 4I15/2 transition at 540 nm are measured and analyzed. The NaYF4: 20% Yb3+, 2% Er3+, 0.5% Nd3+ nanocrystals have the highest emission intensity among all samples under 808-nm excitation. The UC (upconversion) mechanism under 808-nm excitation is discussed in terms of the experimental results. PMID:28788246

Er3+-Tm3+-Yb3+:CaMoO4 phosphor as an outstanding upconversion-based optical temperature sensor and optical heater.

PubMed

Dey, Riya; Kumar Rai, Vineet

2017-03-22

Optical temperature sensing in Er 3+ -Tm 3+ -Yb 3+ codoped CaMoO 4 phosphor prepared by chemical co-precipitation route based on the near infrared (NIR) to green upconversion emission from Er 3+ ion is reported. The variation with respect to external temperature in emission intensity ratio of the green emissions around 530 nm and 552 nm, corresponding to the 2 H 11/2  →  4 I 15/2 and 4 S 3/2  →  4 I 15/2 transitions respectively, under 980 nm excitation has been studied in detail, to report the sensing property of the prepared material; the maximum sensor sensitivity ∼0.0182 K -1 was attained at 413 K. The laser induced optical heating within the prepared phosphor has been explored and the heat generation caused by the laser effect has been verified by comparison of experimental and calculated data.

Observing quantum control of up-conversion luminescence in Dy3+ ion doped glass from weak to intermediate shaped femtosecond laser fields

NASA Astrophysics Data System (ADS)

Liu, Pei; Cheng, Wenjing; Yao, Yunhua; Xu, Cheng; Zheng, Ye; Deng, Lianzhong; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong; Zhang, Shian

2017-11-01

Controlling the up-conversion luminescence of rare-earth ions in real-time, in a dynamical and reversible manner, is very important for their application in laser sources, fiber-optic communications, light-emitting diodes, color displays and biological systems. In previous studies, the up-conversion luminescence control mainly focused on the weak femtosecond laser field. Here, we further extend this control behavior from weak to intermediate femtosecond laser fields. In this work, we experimentally and theoretically demonstrate that the up-conversion luminescence in Dy3+ ion doped glass can be artificially controlled by a π phase step modulation, but the up-conversion luminescence control behavior will be affected by the femtosecond laser intensity, and the up-conversion luminescence is suppressed by lower laser intensity while enhanced by higher laser intensity. We establish a new theoretical model (i.e. the fourth-order perturbation theory) to explain the physical control mechanism by considering the two- and four-photon absorption processes, and the theoretical results show that the relative weight of four-photon absorption in the whole excitation process will increase with the increase in laser intensity, and the interference between two- and four-photon absorptions results in up-conversion luminescence control modulation under different laser intensities. These theoretical and experimental works can provide a new method to control and understand up-conversion luminescence in rare-earth ions, and also may open a new opportunity to the related application areas of rare-earth ions.

Upconversion improvement in KLaF4:Yb3+/Er3+ nanoparticles by doping Al3+ ions

NASA Astrophysics Data System (ADS)

Zhou, Haifang; Wang, Xiechun; Lai, Yunfeng; Cheng, Shuying; Zheng, Qiao; Yu, Jinlin

2017-10-01

Rare-earth ion-doped upconversion (UC) materials show great potential applications in optical and optoelectronic devices due to their novel optical properties. In this work, hexagonal KLaF4:Yb3+/Er3+ nanoparticles (NPs) were successfully synthesized by a hydrothermal method, and remarkably enhanced upconversion luminescence in green and red emission bands in KLaF4:Yb3+/Er3+ NPs has been achieved by doping Al3+ ions under 980 nm excitation. Compared to the aluminum-free KLaF4:Yb3+/Er3+ NPs sample, the UC fluorescence intensities of the green and red emissions of NPs doped with 10 at.% Al3+ ions were significantly enhanced by 5.9 and 7.3 times, respectively. Longer lifetimes of the doped samples were observed for the 4S3/2 state and 4F9/2 state. The underlying reason for the UC enhancement by doping Al3+ ions was mainly ascribed to distortion of the local symmetry around Er3+ ions and adsorption reduction of organic ligands on the surface of NPs. In addition, the influence of doping Al3+ ions on the structure and morphology of the NPs samples was also discussed.

Sensitivity-enhanced Tm3+/Yb3+ co-doped YAG single crystal optical fiber thermometry based on upconversion emissions

NASA Astrophysics Data System (ADS)

Yu, Lu; Ye, Linhua; Bao, Renjie; Zhang, Xianwei; Wang, Li-Gang

2018-03-01

Optical thermometry based on Y3Al5O12 (YAG) single crystal optical fiber with end Tm3+/Yb3+ co-doped is presented. The YAG crystal fiber with end Tm3+/Yb3+ co-doped was grown by laser heated pedestal growth (LHPG) method. Under a 976 nm laser diode excitation, the upconversion (UC) emissions, originating from 3F2,3 →3H6 and 3H4 →3H6 transitions of Tm3+ ions, were investigated in the temperature range from 333 K to 733 K. Interestingly, the UC emission intensity of 3F2,3 →3H6 transition was significantly enhanced with increase of temperature, as compared with the other Tm3+/Yb3+ co-doped materials. The temperature dependence of fluorescence intensity ratio (FIR) of these two emission bands (3F2,3/3H4 →3H6) suggests that this doped YAG crystal fiber can be used as a highly sensitive optical thermal probe, which demonstrates a high absolute sensitivity with the maximum value of 0.021 K-1 at 733 K. In addition, due to the compact structure, strong mechanical strength and high thermal stability, such thermal probe may be a more promising candidate for temperature sensor with a high spatial resolution.

Local symmetric distortion boosted photon up-conversion and thermometric sensitivity in lanthanum oxide nanospheres.

PubMed

Suo, Hao; Zhao, Xiaoqi; Zhang, Zhiyu; Shi, Rui; Wu, Yanfang; Xiang, Jinmeng; Guo, Chongfeng

2018-05-17

It is essential to simultaneously boost the luminescence intensity and thermometric sensitivity of up-converted optical thermometers towards potential biomedical sensing applications. Herein, the effects of local site symmetry on the up-conversion (UC) emission and thermal sensing ability in trigonal-phased La2O3:Er3+/Yb3+ nanospheres were qualitatively explored using cubic-phased Lu2O3 and Y2O3 with a similar shape and phonon energy as contrasts. Under 980 nm light excitation, much stronger UC emissions were detected in La2O3 samples than that in cubic Lu2O3 and Y2O3 samples, and the possible mechanisms were elaborately proposed using Eu3+ as a luminescent probe. Thermo-responsive emission intensity from 2H11/2/4S3/2 levels was monitored to evaluate the absolute sensitivity of three samples, which strongly depends on the dopant-induced local site symmetric distortions according to the Judd-Ofelt theory. The potentiality of La2O3:Er3+/Yb3+ for sub-tissue thermometry was also validated by ex vivo experiments. Results open a promising avenue for realizing highly sensitive thermometry with a large signal-to-noise ratio in sub-tissues via finely tailoring the local site symmetry.

Formation Mechanism, Structural, and Upconversion Properties of Alkaline Rare-Earth Fluoride Nanocrystals Doped With Yb3+/Er3+ Ions.

PubMed

Grzyb, Tomasz; Przybylska, Dominika

2018-06-04

Ultrasmall (9-30 nm) Yb 3+ /Er 3+ -doped, upconverting alkaline rare-earth fluorides that are promising for future applications were synthesized by the microwave-assisted hydrothermal method. The formation mechanism was proposed, indicating the influence of the stability of metal ions complexes with ethylenediaminetetraacetic acid on the composition of the product and tendency to form M 2 REF 7 (M 0.67 RE 0.33 F 2.33 ) cubic compounds in the M-RE-F systems. Their physicochemical properties (structure, morphology, and spectroscopic properties) are compared and discussed. The obtained nanoparticles exhibited emission of light in the visible spectra under excitation by 976 nm laser radiation. Excitation and emission spectra, luminescence decays, laser energy dependencies, and upconversion quantum yields were measured to determine the spectroscopic properties of prepared materials. The Yb 3+ /Er 3+ pair of ions used as dopants was responsible for an intense yellowish-green emission. The upconversion quantum yields determined for the first time for M 2 REF 7 -based materials were 0.0192 ± 0.001% and 0.0176 ± 0.001% for Sr 2 LuF 7 :Yb 3+ ,Er 3+ and Ba 2 LuF 7 :Yb 3+ ,Er 3+ respectively, the two best emitting samples. These results indicated the prepared materials are good and promising alternatives for the most studied NaYF 4 :Yb 3+ ,Er 3+ nanoparticles.

Study of upconversion fluorescence property of novel Er3+/Yb3+ co-doped tellurite glasses.

PubMed

Xu, Tie-Feng; Li, Guang-Po; Nie, Qiu-Hua; Shen, Xiang

2006-06-01

Er3+/Yb3+ co-doped TeO2-B2O3-Nb2O5-ZnO (TBN) glasses were prepared. The absorption spectra and upconversion luminescence spectra of TBN glasses were measured and analyzed. The upconversion emission bands centered at 530, 546 and 658 nm were observed under the excitation at 975 nm, corresponding to the transitions of 2H11/2-->4I15/2, 4S3/2-->4I15/2 and 4F9/2-->4I15/2 respectively. The ratio of red emission to green emission increases with an increasing of Yb3+ ions concentration. According to the quadratic dependence on excitation power, the possible upconversion mechanisms and processes were discussed.

Sub-10 nm lanthanide doped BaLuF{sub 5} nanocrystals: Shape controllable synthesis, tunable multicolor emission and enhanced near-infrared upconversion luminescence

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rao, Ling; Lu, Wei; Wang, Haibo

2015-04-15

Highlights: • Sub-10 nm cubic phase BaLuF{sub 5} nanocrystals were synthesized by a hydrothermal method for the first time. • Tunable multicolor from yellow to yellow-green was achieved by controlling Gd{sup 3+} content in BaLuF{sub 5}:Yb/Er system. • Intense near-infrared upconversion luminescence in BaLuF{sub 5}:Gd/Yb/Tm nanocrystal. • The enhancement near-infrared luminescence can be realized by adjusting the content of Gd{sup 3+} in BaLuF{sub 5}:Gd/Yb/Tm system. - Abstract: In this study, sub-10 nm BaLuF{sub 5} nanocrystals with cubic phase structure were synthesized by a solvothermal method using oleic acid as the stabilizing agent. The as-prepared BaLuF{sub 5} nanocrystals were characterized bymore » transmission electron microscopy (TEM), X-ray diffraction (XRD), and analyzed by the upconversion (UC) spectra. The TEM results reveal that these samples present high uniformity. Compared with Gd-free samples, the size of BaLuF{sub 5}:Yb/Er doped with 10% Gd{sup 3+} decreased to 5.6 nm. In addition, BaLuF{sub 5}:Yb/Tm/Gd upconversion nanoparticles (UCNPs) presented efficient near-infrared (NIR)-NIR UC luminescence. Therefore, it is expected that these ultra-small BaLuF{sub 5} nanocrystals with well-controlled shape, size, and UC emission have potential applications in biomedical imaging fields.« less

Upconversion luminescence in BaMoO{sub 4}:Pr{sup 3+} phosphor for display devices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Soni, Abhishek Kumar; Rai, Vineet Kumar, E-mail: vineetkrrai@yahoo.co.in

2015-08-28

The frequency upconversion is an important nonlinear optical property by which near infrared light is converted into the visible light. The BaMoO{sub 4}:Pr{sup 3+} powder phosphor has been synthesized by solid state reaction method. The upconversion emission bands are recorded under the excitation of 808 nm diode laser. The phase formation of the prepared phosphor has been identified by powder X-ray diffraction (XRD) technique. The upconversion emission mechanism and colour coordinate have been explained by using energy level and CIE (International Commission on Illumination) chromaticity diagram study, respectively.

Light-Harvesting Organic Nanocrystals Capable of Photon Upconversion.

PubMed

Li, Li; Zeng, Yi; Yu, Tianjun; Chen, Jinping; Yang, Guoqiang; Li, Yi

2017-11-23

Harvesting and converting low energy photons into higher ones through upconversion have great potential in solar energy conversion. A light-harvesting nanocrystal assembled from 9,10-distyrylanthracene and palladium(II) meso-tetraphenyltetrabenzoporphyrin as the acceptor and the sensitizer, respectively effects red-to-green upconversion under incoherent excitation of low power density. An upconversion quantum yield of 0.29±0.02 % is obtained upon excitation with 640 nm laser of 120 mW cm -2 . The well-organized packing of acceptor molecules with aggregation-induced emission in the nanocrystals dramatically reduces the nonradiative decay of the excited acceptor, benefits the triplet-triplet annihilation (TTA) upconversion and guides the consequent upconverted emission. This work provides a straightforward strategy to develop light-harvesting nanocrystals based on TTA upconversion, which is attractive for energy conversion and photonic applications. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cooperative upconversion luminescence in Tb{sup 3+}:Yb{sup 3+} co-doped Y{sub 2}SiO{sub 5} powders prepared by combustion synthesis

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rakov, Nikifor, E-mail: nikifor.gomez@univasf.edu.br; Vieira, Simone A.; Guimarães, Renato B.

2014-03-15

Frequency upconversion (UC) luminescence via cooperative energy transfer (CET) process between pairs of Yb{sup 3+} and Tb{sup 3+} ions was investigated in Tb{sup 3+}:Yb{sup 3+}:Y{sub 2}SiO{sub 5} crystalline ceramic powders prepared by combustion synthesis. Surface morphology and structure of the powders were investigated by scanning electronic microscopy and X-ray powder diffraction. Photoluminescence experiments were performed in Tb{sup 3+}-singly doped samples using ultraviolet light (λ=255 nm) and in Tb{sup 3+}:Yb{sup 3+} co-doped samples using a near-infrared (NIR) diode laser (λ=975 nm). Upon excitation with the NIR diode laser, UC luminescence with an intense emission band centered at ∼549 nm, corresponding tomore » the 4f intraband {sup 5}D{sub 4}→{sup 7}F{sub 5} transition of Tb{sup 3+}, along with less intense emission bands at ∼490, ∼590 and ∼620 nm, corresponding to other {sup 5}D{sub 4}→{sup 7}F{sub J} transitions, was detected. The CET rate was estimated by analyzing the dynamics of UC luminescence with rate equations model of the electronic populations. -- Graphical Abstract: Left: Cooperative upconversion luminescence spectra of three powder samples prepared by combustion synthesis. Right: The SEM image of the powder showing that it consists of agglomerated flake-like shaped particles of various sizes. Full scale bar is 20 μm. Highlights: • Yttrium orthosilicate (Y{sub 2}SiO{sub 5}) powders were prepared by combustion synthesis. • Cooperative upconversion is observed for the first time in Tb{sup 3+}–Yb{sup 3+} doped Y{sub 2}SiO{sub 5}. • Energy transfer and back-transfer rates between Tb{sup 3+} and Yb{sup 3+} pairs were estimated.« less

Preparation of ZnO nanoparticles showing upconversion luminescence through simple chemical method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Anjana, R.; Subha, P. P.; Markose, Kurias K.

2016-05-23

Upconversion luminescence is an interesting area while considering its applications in a vast variety of fields. Rare earth ions like erbium is the most studied and efficient candidate for achieving upconversion. Erbium and ytterbium co-doped ZnO nanoparticles were prepared through co-precipitation method. A strong red emission has been obtained while exciting with 980 nm laser. Dependence of luminescence emission colour on ytterbium concentration has been studied.

Down- and up-conversion emissions in Er-doped transparent fluorotellurite glass-ceramics

NASA Astrophysics Data System (ADS)

Miguel, A.; Morea, R.; Gonzalo, J.; Fernandez, J.; Balda, R.

2015-03-01

In this work, we report the near infrared and upconversion emissions of Er3+-doped transparent fluorotellurite glassceramics obtained by heat treatment of the precursor Er-doped TeO2-ZnO-ZnF2 glass. Structural analysis shows that ErF3 nanocrystals nucleated in the glass-ceramic sample are homogeneously distributed in the glass matrix with a typical size of 45±10 nm. The comparison of the fluorescence properties of Er3+-doped precursor glass and glass-ceramic confirms the successful incorporation of the rare-earth into the nanocrystals. An enhancement of the red upconversion emission due to 4F9/2→4I15/2 transition together with weak emission bands due to transitions from 2H9/2, 4F3/2,5/2, and 4F7/2 levels to the ground state are observed under excitation at 801 nm in the glass-ceramic sample. The temporal evolution of the red emission together with the excitation upconversion spectrum suggest that energy transfer processes are responsible for the enhancement of the red emission.

Structural and optical properties of thermal decomposition assisted Gd2O3:Ho(3+)/Yb(3+) upconversion phosphor annealed at different temperatures.

PubMed

Kumar, A; Tiwari, S P; Kumar, K; Rai, V K

2016-10-05

The infrared to visible upconversion fluorescent nanoparticles of Ho(3+)/Yb(3+) codoped Gd2O3 phosphor is synthesized via thermal decomposition route. The as-synthesized sample was annealed at 800, 1000 and 1200°C for 3h and then structural and optical properties were studied. The Rietveld refinement of X-ray diffraction (XRD) data was analyzed to probe the effect of Ho(3+)/Yb(3+) dopant on the structural parameters of Gd2O3 host. The upconversion emission spectra of as-synthesized and annealed samples are compared using 980nm diode laser excitation and five emission bands noticed at 490, 539, 550, 667 and 757nm corresponding to the (5)F3→(5)I8, (5)F4→(5)I8, (5)S2→(5)I8,(5)F5→(5)I8 and (5)I4→(5)I8 manifolds, respectively. The local temperature induced by laser light is also calculated. The fluorescence intensity ratio (FIR) of two thermally coupled transitions (5)F4→(5)I8 and (5)S2→(5)I8 is plotted against the sample temperature and sensor sensitivity of sample is calculated. Copyright © 2016 Elsevier B.V. All rights reserved.

ZnMoO4:Er3+,Yb3+ phosphor with controlled morphology and enhanced upconversion through alkali ions doping

NASA Astrophysics Data System (ADS)

Luitel, Hom Nath; Chand, Rumi; Watari, Takanori

2018-04-01

A facile hydrothermal method was used to synthesize ZnMoO4:Er3+,Yb3+ nanoparticles. The shapes and sizes of the nanoparticles were well tuned by simply monitoring the pH of the starting solution. Microballs consisting of agglomerated nanograins were observed at strong acidic condition. At mild pH, plates and rectangular particles were realized, while strong basic pH stabilized rods. Further increasing pH to extremely basic conditions (pH > 13), rods changed to fragile hairy structures. The nucleation and growth mechanism of nanograins to form different morphology nanoparticles were studied and illustrated. XRD patterns confirmed well crystalline, triclinic structure despite small amount of aliovalent metal ions doping. Under 980 nm excitation, the ZnMoO4:Er3+,Yb3+ nanophosphor exhibited strong green (centered at 530 and 560 nm) and weak red (centered at 660 nm) upconversion (UC) emissions. Substitution of part of the Zn2+ ions by monovalent alkali ions intensified the UC emission intensities drastically. The order of intensification was K+>Na+>Li+>Rb+>no alkali ion. When Zn2+ ions were substituted with 10 at% K+ ions, the green and red UC emissions intensities increased by more than 50 and 15 folds, respectively. Time dependent measurements confirmed efficient Yb to Er energy transfer in the ZnMoO4:Er3+,Yb3+,K+ nanophosphor. The optimized ZnMoO4:Er3+,Yb3+,K+ phosphor exhibited intense UC emissions with 0.31% quantum yield. The upconverted light is visible to naked eye while pumping by laser of less than 1 mW power and opens door for variety of novel applications.

Multicolor upconversion emission from Tm3++Ho3++Yb3+ codoped tellurite glass on NIR excitations

NASA Astrophysics Data System (ADS)

Giri, N. K.; Rai, D. K.; Rai, S. B.

2008-06-01

Multicolor emission has been produced using 798 nm and 980 nm laser excitation in a Tm3++Ho3++Yb3+ codoped tellurite based glass. This glass generates simultaneously red, green and blue (RGB) emission on 798 nm excitation. Multicolor emission thus obtained was tuned to white luminescence by adjusting the Ho3+ ion concentration. There is a close match between the calculated color coordinate for the white luminescence obtained here and the point of equal energy which represents white in the 1931 CIE chromaticity diagram. The 980 nm excitation of the same sample on the other hand gives intense green and red emission and the glass appears greenish.

White light emission and effect of annealing on the Ho{sup 3+}–Yb{sup 3+} codoped BaCa{sub 2}Al{sub 8}O{sub 15} phosphor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumari, Astha; Rai, Vineet Kumar, E-mail: vineetkrrai@yahoo.co.in

Graphical abstract: The upconversion emission spectra of the Ho{sup 3+}/Yb{sup 3+} doped/codoped BaCa{sub 2}Al{sub 8}O{sub 15} phosphors with different doping concentrations of Ho{sup 3+}/Yb{sup 3+} ions along with UC emission spectrum of the white light emitting phosphor annealed at 800 °C. - Highlights: • BaCa{sub 2}Al{sub 8}O{sub 15} phosphors codoped with Ho{sup 3+}–Yb{sup 3+} have been prepared by combustion method. • Phosphor annealed at 800 °C, illuminate an intense white light upon NIR excitation. • The sample annealed at higher temperatures emits in the pure green region. • The colour emitted persists in the white region even at high pumpmore » power density. • Developed phosphor is suitable for making upconverters and WLEDs. - Abstract: The BaCa{sub 2}Al{sub 8}O{sub 15} (BCAO) phosphors codoped with suitable Ho{sup 3+}–Yb{sup 3+} dopant concentration prepared by combustion method illuminate an intense white light upon near infrared diode laser excitation. The structural analysis of the phosphors and the detection of impurity contents have been performed by using the X-Ray Diffraction, FESEM and FTIR analysis. The purity of white light emitted from the sample has been confirmed by the CIE chromaticity diagram. Also, the white light emitted from the sample persists with the variation of pump power density. The phosphors emit upconversion (UC) emission bands in the blue, green and red region (three primary colours required for white light emission) along with one more band in the near infrared region of the electromagnetic spectrum. On annealing the white light emitting sample at higher temperatures, the sample starts to emit green colour and also the intensity of green and red UC emission bands get enhanced largely.« less

Up-conversion fluorescence: noncoherent excitation by sunlight.

PubMed

Baluschev, S; Miteva, T; Yakutkin, V; Nelles, G; Yasuda, A; Wegner, G

2006-10-06

We demonstrate up-conversion of noncoherent sunlight realized by ultralow excitation intensity. The bimolecular up-conversion process in our systems relies on the presence of a metastable triplet excited state, and thus has dramatically different photophysical characteristics relative to the other known methods for photon up-conversion (two-photon absorption, parametric processes, second harmonic generation, sequential multiphoton absorption, etc.).

Mechanisms of low-power noncoherent photon upconversion in metalloporphyrin-organic blue emitter systems in solution.

PubMed

Sugunan, Sunish K; Tripathy, Umakanta; Brunet, Sophie M K; Paige, Matthew F; Steer, Ronald P

2009-07-30

The mechanisms of noncoherent photon upconversion that involve triplet-triplet annihilation (TTA) in solution have been investigated for two model systems. ZnTPP (meso-tetraphenylporphine zinc) is used as the model visible light-absorbing metalloporphyrin because its S(1) fluorescence intensity can be used to monitor the initial rate of porphyrin triplet state production and because its S(2) fluorescence intensity can be used as a direct measure of the rate of porphyrin TTA. When perylene, which has a triplet energy lower than that of ZnTPP, is added as a signaling blue emitter (BE), the mechanism of photon upconversion involves triplet energy transfer from the porphyrin to the BE followed by TTA in the BE to form the fluorescent perylene S(1) state. The kinetics of this process have been characterized and are unremarkable. When coumarin 343 (C343), which has photophysical properties similar to those of perylene except that it has a much higher triplet energy than ZnTPP, is added as the signaling BE, emission from the ZnTPP S(2) state is quenched and fluorescence from the C343 grows in. Contrary to previous suggestions, the mechanism of photon upconversion in this system does not involve singlet energy transfer from the porphyrin S(2) state to the BE. Instead, ground-state C343 complexes with the ZnTPP triplet to form a triplet exciplex, which then undergoes TTA with a second ZnTPP triplet to give the fluorescent state of the BE in a three-center process.

Thiazole derivative-modified upconversion nanoparticles for Hg2+ detection in living cells

NASA Astrophysics Data System (ADS)

Gu, Bin; Zhou, Yi; Zhang, Xiao; Liu, Xiaowang; Zhang, Yuhai; Marks, Robert; Zhang, Hua; Liu, Xiaogang; Zhang, Qichun

2015-12-01

Mercury ion (Hg2+) is an extremely toxic ion, which will accumulate in human bodies and cause severe nervous system damage. Therefore, the sensitive and efficient monitoring of Hg2+ in human bodies is of great importance. Upconversion nanoparticle (UCNPs) based nano probes exhibit no autofluorescence, deep penetration depth and chemical stability in biological samples, as well as a large anti-stokes shift. In this study, we have developed thiazole-derivative-functionalized UCNPs, and employed an upconversion emission intensity ratio of 540 nm to 803 nm (I540/I803) as a ratiometric signal to detect Hg2+ in living cells showing excellent photo stability and high selectivity. Our nano probe was characterized using transmission electron microscopy (TEM) and powder X-ray diffraction (PXRD). The low cytotoxicity of our probe was confirmed by an MTT assay and the UCL test in HeLa cells was carried out by confocal microscopy. Our results demonstrated that organic-dye-functionalized UCNPs should be a good strategy for detecting toxic metal ions when studying cellular biosystems.Mercury ion (Hg2+) is an extremely toxic ion, which will accumulate in human bodies and cause severe nervous system damage. Therefore, the sensitive and efficient monitoring of Hg2+ in human bodies is of great importance. Upconversion nanoparticle (UCNPs) based nano probes exhibit no autofluorescence, deep penetration depth and chemical stability in biological samples, as well as a large anti-stokes shift. In this study, we have developed thiazole-derivative-functionalized UCNPs, and employed an upconversion emission intensity ratio of 540 nm to 803 nm (I540/I803) as a ratiometric signal to detect Hg2+ in living cells showing excellent photo stability and high selectivity. Our nano probe was characterized using transmission electron microscopy (TEM) and powder X-ray diffraction (PXRD). The low cytotoxicity of our probe was confirmed by an MTT assay and the UCL test in HeLa cells was carried out by confocal microscopy. Our results demonstrated that organic-dye-functionalized UCNPs should be a good strategy for detecting toxic metal ions when studying cellular biosystems. Electronic supplementary information (ESI) available: NMR, MALDI-TOF MS spectra, etc. See DOI: 10.1039/c5nr05286f

High efficiency upconversion nanophosphors for high-contrast bioimaging

NASA Astrophysics Data System (ADS)

Alkahtani, Masfer H.; Alghannam, Fahad S.; Sanchez, Carlos; Gomes, Carmen L.; Liang, Hong; Hemmer, Philip R.

2016-12-01

Upconversion nanoparticles (UCNPs) are of interest because they allow suppression of tissue autofluorescence and are therefore visible deep inside biological tissue. Compared to upconversion dyes, UCNPs have a lower pump intensity threshold, better photostability, and less toxicity. Recently, YVO4: Er+3, Yb+3 nanoparticles were shown to exhibit strong up-conversion luminescence with a relatively low 10 kW cm-2 excitation intensity even in water, which makes them excellent bio-imaging candidates. Herein, we investigate their use as internal probes in insects by injecting YVO4 : Er+3, Yb+3 nanoparticles into fire ants as a biological model, and obtain 2D optical images with 980 nm illumination. High-contrast images with high signal-to-noise ratio are observed by detecting the up-conversion fluorescence as the excitation laser is scanned.

Change in structural morphology on addition of ZnO and its effect on fluorescence of Yb³⁺/Er³⁺ doped Y₂O₃.

PubMed

Yadav, R V; Verma, R K; Kaur, G; Rai, S B

2013-02-15

Yb(3+)/Er(3+) codoped Y(2)O(3) phosphor and its composite with ZnO have been synthesized by combustion method. Morphology of the materials has been investigated using X-ray diffraction pattern (XRD) and scanning electron microscopy (SEM) techniques. XRD confirms the constituents as Y(2)O(3) and ZnO, with average crystallite size of 112 nm. On addition of ZnO, a small shifting in XRD pattern of Y(2)O(3) is observed. SEM pattern suggests that the average particle size lies in micro-range (0.5 μm). A dumble like structure is observed for hybrid material on annealing at 1473 K. A strong green (525, 546 nm) with weak blue (411 nm) and red (657 nm) emissions through upconversion has been observed from the phosphor on excitation with 976 nm diode laser. The observed emissions involve (2)H(9/2)→(4)I(15/2), (2)H(11/2)→(4)I(15/2), (4)S(3/2)→(4)I(15/2) and (4)F(9/2)→(4)I(15/2) electronic transitions, respectively. The upconversion process has been confirmed by power dependence measurements and its slope value was found to be 1.85, 1.72 for green and red emissions, respectively. On addition of ZnO, the intensity of these emissions is enhanced several times. The reason behind the enhancement is discussed with the help of the emitting level lifetime. An interesting dual mode property (upconversion and downconversion) to the same material has been observed on excitation with 532 nm laser source. Copyright © 2012 Elsevier B.V. All rights reserved.

[Multiply upconversion emission in oxyfluoride ceramics].

PubMed

Xiao, Si-guo; Yang, Xiao-liang; Liu, Zhen-wei

2003-02-01

Oxyfluoride ceramics with the host composition of SiO2 and PbF2 have been prepared. X-ray diffraction analysis of the ceramics revealed that fluoride type beta-PbF2 solid solution regions are precipitated in the glass matrix. Rare earth ions in the beta-PbF2 solid solution show highly efficient upconversion performance due to the very small multi-phonon relaxation rates. Eight upconversion emission bands whose central wavelength are 846, 803, 665, 549, 523, 487, 456 and 411 nm have been observed when the sample was excited with 930 nm diode light. Four possible energy transfer processes between Er3+ and Yb3+ cause the electronic population of high energy level of Er3+ and realize the abound upconversion luminescence bands.

Survey and research on up-conversion emission character and energy transition of Yb3+/Er3+/Tm3+ co-doped phosphate glass and glass ceramic

NASA Astrophysics Data System (ADS)

Yu, Yin; Song, Feng; Ming, Chengguo; Liu, Jiadong; Li, Wei; Liu, Yanling; Zhao, Hongyan

2012-11-01

By conventional high-temperature melting method, Yb3+/Er3+/Tm3+ co-doped phosphate glass was synthesized. After annealing the precursor glass, the phosphate glass ceramic (GC) was obtained. By measuring the X-ray diffraction (XRD) spectrum, it is proved that the LiYbP4O12 and Li6P6O18 nano-crystals have existed in the phosphate GC. The up-conversion (UC) emission intensity of the GC is obvious stronger compared to that of the glass. The reason is that the shorter distance between rare earth ions in the glass ceramic increases the energy transitions from the sensitized ions (Yb3+) to the luminous ions (Er3+ and Tm3+). By studying the dependence of UC emissions on the pump power, the 523 and 546 nm green emissions of Er3+ ions in the glass are two-photon processes. But in the glass ceramic, they are two/three-photon processes. The phenomenon implies that a three-photon process has participated in the population of the two green emissions. Using Dexter theory, we discuss the energy transitions of Er3+ and Tm3+. The results indicate the energy transition of Tm3+ to Er3+ is very strong in the GC, which changes the population mechanism of UC emissions of Er3+.

Upconverting fluorescent nanoparticles for biodetection and photoactivation

NASA Astrophysics Data System (ADS)

Huang, Kai; Li, WenKai; Jayakumar, Muthu Kumara Gnanasammandhan; Zhang, Yong

2013-03-01

Fluorophores including fluorescent dyes/proteins and quantum dots (QDs) are used for fluorescence-based imaging and detection. These are based on `downconversion fluorescence' and have several drawbacks: photobleaching, autofluorescence, short tissue penetration depth and tissue photo-damage. Upconversion fluorescent nanoparticles (UCNs) emit detectable photons of higher energy in the short wavelength range upon irradiation with near-infrared (NIR) light based on a process termed `upconversion'. UCNs show absolute photostability, negligible autofluorescence, high penetration depth and minimum photodamage to biological tissues. Lanthanide doped nanocrystals with nearinfrared NIR-to-NIR and/or NIR-to-VIS and/or NIR-to-UV upconversion fluorescence emission have been synthesized. The nanocrystals with small size and tunable multi-color emission have been developed. The emission can be tuned by doping different upconverting lanthanide ions into the nanocrystals. The nanocrystals with core-shell structure have also been prepared to tune the emission color. The surfaces of these nanocrystals have been modified to render them water dispersible and biocompatible. They can be used for ultrasensitive interference-free biodetection because most biomolecules do not have upconversion properties. UCNs are also useful for light based therapy with enhanced efficiency, for example, photoactivation.

Upconversion properties of Er3+/Yb3+ co-doped TeO2-TiO2-K2O glasses.

PubMed

Su, Fangning; Deng, Zaide

2006-01-01

The Er3+/Yb3+ co-doped TeO2-TiO2-K2O glasses were prepared by conventional melting procedures, and their upconversion spectra were performed. The dependence of luminescence intensity on the ratio of Yb3+/Er3+ was studied, and the relationship between green upconversion luminescence intensity and Er3+ concentration is discussed in detail. The 546 nm green upconversion luminescence intensity is optimised in the studied glasses either when the Yb3+/Er3+ ratio is 25/1 and Er3+ concentration is 0.1 mol%, or when the Yb3+/Er3+ ratio is 10/1 and Er3+ concentration is 0.15 mol%. These glasses could be one of the potential candidates for LD pumping microchip solid-state lasers.

Up-conversion luminescence of Er3+ ions in lead-free germanate glasses under 800 nm and 980 nm cw diode laser excitation

NASA Astrophysics Data System (ADS)

Janek, J.; Lisiecki, R.; Ryba-Romanowski, W.; Pisarska, J.; Pisarski, W. A.

2017-12-01

Up-conversion luminescence spectra of Er3+ ions in multicomponent oxyfluoride glasses GeO2 - BaO - BaF2 - Ga2O3 - Er2O3 were examined. It was found that the up-conversion luminescence spectra of Er3+ are dependent on pumping wavelengths. The spectra recorded upon the excitation at 800 nm contained an intense green up-conversion luminescence corresponding to the 2H11/2,4S3/2 → 4I15/2 transitions and a very weak red luminescence related to the 4F9/2 - 4I15/2 transition. In spectra recorded upon 980 nm excitation the contribution of the red luminescence was markedly higher. The interaction mechanisms involved in up-conversion processes are proposed and observed dependence of intensity of up-converted luminescence on excitation power is discussed. The experimental results suggest that Er3+ singly doped lead-free oxyfluoride germanate glass is useful for up-conversion luminescence applications.

Synthesis of Gd2O3:Ho3+/Yb3+ upconversion nanoparticles for latent fingermark detection on difficult surfaces

NASA Astrophysics Data System (ADS)

Kumar, A.; Tiwari, S. P.; Singh, A. K.; Kumar, K.

2016-07-01

Infrared to visible upconversion fluorescent nanoparticles of Gd2O3 codoped with Ho3+/Yb3+ ions are synthesized via thermal decomposition process. The X-ray diffraction analysis of as-synthesized nanoparticles and annealed sample at 1000 °C has shown body-centered cubic phase of Gd2O3. The synthesized phosphor has shown intense green emission upon 980-nm excitation. High-contrast latent fingermarks on some difficult semi-porous and non-porous surfaces under 980-nm diode laser excitation were developed through powder dusting and colloidal solution spraying techniques and the results are compared with the commercial green luminescent fingermark powder. The latent fingermarks were developed on transparent (biological glass slides), single-color (aluminum foil) and multicolor (plywood, plastic bottle and book cover page) background surfaces. The present study depicts that the upconversion-based latent fingermarks detection using Gd2O3:Ho3+/Yb3+ phosphor material is suitable over the other conventional powders and has potential for practical applications in forensic science.

Three-dimensional quick response code based on inkjet printing of upconversion fluorescent nanoparticles for drug anti-counterfeiting

NASA Astrophysics Data System (ADS)

You, Minli; Lin, Min; Wang, Shurui; Wang, Xuemin; Zhang, Ge; Hong, Yuan; Dong, Yuqing; Jin, Guorui; Xu, Feng

2016-05-01

Medicine counterfeiting is a serious issue worldwide, involving potentially devastating health repercussions. Advanced anti-counterfeit technology for drugs has therefore aroused intensive interest. However, existing anti-counterfeit technologies are associated with drawbacks such as the high cost, complex fabrication process, sophisticated operation and incapability in authenticating drug ingredients. In this contribution, we developed a smart phone recognition based upconversion fluorescent three-dimensional (3D) quick response (QR) code for tracking and anti-counterfeiting of drugs. We firstly formulated three colored inks incorporating upconversion nanoparticles with RGB (i.e., red, green and blue) emission colors. Using a modified inkjet printer, we printed a series of colors by precisely regulating the overlap of these three inks. Meanwhile, we developed a multilayer printing and splitting technology, which significantly increases the information storage capacity per unit area. As an example, we directly printed the upconversion fluorescent 3D QR code on the surface of drug capsules. The 3D QR code consisted of three different color layers with each layer encoded by information of different aspects of the drug. A smart phone APP was designed to decode the multicolor 3D QR code, providing the authenticity and related information of drugs. The developed technology possesses merits in terms of low cost, ease of operation, high throughput and high information capacity, thus holds great potential for drug anti-counterfeiting.Medicine counterfeiting is a serious issue worldwide, involving potentially devastating health repercussions. Advanced anti-counterfeit technology for drugs has therefore aroused intensive interest. However, existing anti-counterfeit technologies are associated with drawbacks such as the high cost, complex fabrication process, sophisticated operation and incapability in authenticating drug ingredients. In this contribution, we developed a smart phone recognition based upconversion fluorescent three-dimensional (3D) quick response (QR) code for tracking and anti-counterfeiting of drugs. We firstly formulated three colored inks incorporating upconversion nanoparticles with RGB (i.e., red, green and blue) emission colors. Using a modified inkjet printer, we printed a series of colors by precisely regulating the overlap of these three inks. Meanwhile, we developed a multilayer printing and splitting technology, which significantly increases the information storage capacity per unit area. As an example, we directly printed the upconversion fluorescent 3D QR code on the surface of drug capsules. The 3D QR code consisted of three different color layers with each layer encoded by information of different aspects of the drug. A smart phone APP was designed to decode the multicolor 3D QR code, providing the authenticity and related information of drugs. The developed technology possesses merits in terms of low cost, ease of operation, high throughput and high information capacity, thus holds great potential for drug anti-counterfeiting. Electronic supplementary information (ESI) available: Calculating details of UCNP content per 3D QR code and decoding process of the 3D QR code. See DOI: 10.1039/c6nr01353h

The role of Nb in intensity increase of Er ion upconversion luminescence in zirconia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smits, K., E-mail: smits@cfi.lu.lv; Sarakovskis, A.; Grigorjeva, L.

2014-06-07

It is found that Nb co-doping increases the luminescence and upconversion luminescence intensity in rare earth doped zirconia. Er and Yb-doped nanocrystalline samples with or without Nb co-doping were prepared by sol-gel method and thermally annealed to check for the impact of phase transition on luminescence properties. Phase composition and grain sizes were examined by X-ray diffraction; the morphology was checked by scanning- and high-resolution transmission electron microscopes. Both steady-state and time-resolved luminescence were studied. Comparison of samples with different oxygen vacancy concentrations and different Nb concentrations confirmed the known assumption that oxygen vacancies are the main agents for tetragonalmore » or cubic phase stabilization. The oxygen vacancies quench the upconversion luminescence; however, they also prevent agglomeration of rare-earth ions and/or displacement of rare-earth ions to grain surfaces. It is found that co-doping with Nb ions significantly (>20 times) increases upconversion luminescence intensity. Hence, ZrO{sub 2}:Er:Yb:Nb nanocrystals may show promise for upconversion applications.« less

Upconversion microparticles as time-resolved luminescent probes for multiphoton microscopy: desired signal extraction from the streaking effect

NASA Astrophysics Data System (ADS)

Pominova, Daria V.; Ryabova, Anastasia V.; Grachev, Pavel V.; Romanishkin, Igor D.; Kuznetsov, Sergei V.; Rozhnova, Julia A.; Yasyrkina, Daria S.; Fedorov, Pavel P.; Loschenov, Victor B.

2016-09-01

The great interest in upconversion nanoparticles exists due to their high efficiency under multiphoton excitation. However, when these particles are used in scanning microscopy, the upconversion luminescence causes a streaking effect due to the long lifetime. This article describes a method of upconversion microparticle luminescence lifetime determination with help of modified Lucy-Richardson deconvolution of laser scanning microscope (LSM) image obtained under near-IR excitation using nondescanned detectors. Determination of the upconversion luminescence intensity and the decay time of separate microparticles was done by intensity profile along the image fast scan axis approximation. We studied upconversion submicroparticles based on fluoride hosts doped with Yb3+-Er3+ and Yb3+-Tm3+ rare earth ion pairs, and the characteristic decay times were 0.1 to 1.5 ms. We also compared the results of LSM measurements with the photon counting method results; the spread of values was about 13% and was associated with the approximation error. Data obtained from live cells showed the possibility of distinguishing the position of upconversion submicroparticles inside and outside the cells by the difference of their lifetime. The proposed technique allows using the upconversion microparticles without shells as probes for the presence of OH- ions and CO2 molecules.

Activation of the surface dark-layer to enhance upconversion in a thermal field

NASA Astrophysics Data System (ADS)

Zhou, Jiajia; Wen, Shihui; Liao, Jiayan; Clarke, Christian; Tawfik, Sherif Abdulkader; Ren, Wei; Mi, Chao; Wang, Fan; Jin, Dayong

2018-03-01

Thermal quenching, in which light emission experiences a loss with increasing temperature, broadly limits luminescent efficiency at higher temperature in optical materials, such as lighting phosphors1-3 and fluorescent probes4-6. Thermal quenching is commonly caused by the increased activity of phonons that leverages the non-radiative relaxation pathways. Here, we report a kind of heat-favourable phonons existing at the surface of lanthanide-doped upconversion nanomaterials to combat thermal quenching. It favours energy transfer from sensitizers to activators to pump up the intermediate excited-state upconversion process. We identify that the oxygen moiety chelating Yb3+ ions, [Yb...O], is the key underpinning this enhancement. We demonstrate an approximately 2,000-fold enhancement in blue emission for 9.7 nm Yb3+-Tm3+ co-doped nanoparticles at 453 K. This strategy not only provides a powerful solution to illuminate the dark layer of ultra-small upconversion nanoparticles, but also suggests a new pathway to build high-efficiency upconversion systems.

Intense upconversion luminescence and effect of local environment for Tm3+/Yb3+ co-doped novel TeO2-BiCl3 glass system.

PubMed

Wang, Guonian; Dai, Shixun; Zhang, Junjie; Wen, Lei; Yang, Jianhu; Jiang, Zhonghong

2006-05-15

We present the results of a study that uses theoretical and experimental methods to investigate the characteristics of the upconversion luminescence of Tm3+/Yb3+ codoped TeO2-BiCl3 glass system as a function of the BiCl3 fraction. These glasses are potentially important in the design of upconversion fiber lasers. Effect of local environment around Tm3+ on upconversion fluorescence intensity was analyzed by theoretical calculations. The structure and spectroscopic properties were investigated in the experiments by measuring the Raman spectra, IR transmission spectra, and absorption and fluorescence intensities at room temperature. The results indicate that blue luminescence quantum efficiency increases with increasing BiCl3 content from 10 to 60 mol%, which were interpreted by the increase of asymmetry of glass structure, decrease of phonon energy and removing of OH- groups.

Enhanced frequency upconversion in Er3+-Yb3+ codoped heavy metal oxides based tellurite glasses.

PubMed

Azam, Mohd; Rai, Vineet Kumar

2018-01-24

The spectroscopic investigations on the Er 3+ /Yb 3+ ions doped/codoped TeO 2 -ZnO (TZ), TeO 2 -ZnO-WO 3 (TZW) and TeO 2 -ZnO-WO 3 -TiO 2 (TZWTi) heavy metal oxide (HMO) glasses have been made. The absorption, photoluminescence, decay curve and Judd-Ofelt analysis have been performed to optimise the optical properties of the Er 3+ /Yb 3+ ions. The effect of incorporation of HMOs like WO 3 and TiO 2 in the Er 3+ /Yb 3+ doped/codoped TZ glass on its optical properties have been investigated. The enhancement in upconversion emission intensity has been explained on the basis of efficient energy transfer and inhomogeneous local field generation around the rare earth ions. The spectroscopic quality factor, absorption and stimulated emission cross-sections, optical gain, quantum efficiency (∼17.53%), energy transfer efficiency (∼61.64%), colour purity (∼94.7%) and ionic nature of the bonding have been determined. The Er 3+ -Yb 3+ -TZWTi glass can be used in visible lasers, yellowish green optical devices and home appliances.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhou Bo; Pun, Edwin Yue-Bun; Yang Dianlai

Ho{sup 3+}-doped and Ho{sup 3+}/Yb{sup 3+}-codoped lead bismuth gallate (PBG) oxide glasses were prepared and their spectroscopic properties were investigated. The derived Judd-Ofelt intensity parameters (OMEGA{sub 2}=6.81x10{sup -20} cm{sup 2}, OMEGA{sub 4}=2.31x10{sup -20} cm{sup 2}, and OMEGA{sub 6}=0.67x10{sup -20} cm{sup 2}) indicate a higher asymmetry and stronger covalent environment for Ho{sup 3+} sites in PBG glass compared with those in tellurite, fluoride (ZBLAN), and some other lead-contained glasses. Intense frequency upconversion emissions peaking at 547, 662, and 756 nm as well as infrared emissions at 1.20 and 2.05 mum in Ho{sup 3+}/Yb{sup 3+}-codoped PBG glass were observed, confirming that energymore » transfer between Yb{sup 3+} and Ho{sup 3+} takes place, and a two-phonon-assisted energy transfer from Yb{sup 3+} to Ho{sup 3+} ions was determined by the calculation using phonon sideband theory. The 1.20 mum emission observed was primarily due to the weak multiphonon deexcitation originated from the small phonon energy of PBG glass (approx535 cm{sup -1}). A large product of emission cross-section and measured lifetime (9.93x10{sup -25} cm{sup 2} s) was obtained for the 1.20 mum emission and the gain coefficient dependence on wavelength with population inversion rate (P) was performed. The peak emission cross-section for 2.05 mum emission was calculated to be 4.75x10{sup -21} cm{sup 2}. The relative mechanism of Ho{sup 3+}-doped and Ho{sup 3+}/Yb{sup 3+}-codoped PBG glasses on their spectroscopic properties was also discussed. Our results suggest that Ho{sup 3+}/Yb{sup 3+}-doped PBG glasses are a good potential candidate for the frequency upconversion devices and infrared amplifiers/lasers.« less

Three-dimensional quick response code based on inkjet printing of upconversion fluorescent nanoparticles for drug anti-counterfeiting.

PubMed

You, Minli; Lin, Min; Wang, Shurui; Wang, Xuemin; Zhang, Ge; Hong, Yuan; Dong, Yuqing; Jin, Guorui; Xu, Feng

2016-05-21

Medicine counterfeiting is a serious issue worldwide, involving potentially devastating health repercussions. Advanced anti-counterfeit technology for drugs has therefore aroused intensive interest. However, existing anti-counterfeit technologies are associated with drawbacks such as the high cost, complex fabrication process, sophisticated operation and incapability in authenticating drug ingredients. In this contribution, we developed a smart phone recognition based upconversion fluorescent three-dimensional (3D) quick response (QR) code for tracking and anti-counterfeiting of drugs. We firstly formulated three colored inks incorporating upconversion nanoparticles with RGB (i.e., red, green and blue) emission colors. Using a modified inkjet printer, we printed a series of colors by precisely regulating the overlap of these three inks. Meanwhile, we developed a multilayer printing and splitting technology, which significantly increases the information storage capacity per unit area. As an example, we directly printed the upconversion fluorescent 3D QR code on the surface of drug capsules. The 3D QR code consisted of three different color layers with each layer encoded by information of different aspects of the drug. A smart phone APP was designed to decode the multicolor 3D QR code, providing the authenticity and related information of drugs. The developed technology possesses merits in terms of low cost, ease of operation, high throughput and high information capacity, thus holds great potential for drug anti-counterfeiting.

Structural and optical characterization of NaGdF{sub 4}: Ho{sup 3+}/Yb{sup 3+} UC nano-particles for lateral finger mark detections

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, A., E-mail: ak.phy87@gmail.com; Tiwari, S. P.; Krishna, K. M.

2016-05-23

Ho{sup 3+}/Yb{sup 3+} co-doped NaGdF{sub 4} up-conversion (UC) nano-particles were synthesized by thermal decomposition method. X-ray diffraction and FE-SEM image analysis were done to confirm the structure, morphology and determination of particle size. The UC emission spectra for as prepared as well as 100°C, 200°C, 300°C, 400°C, 800°C, 1000°C and 1200°C heated for 3h samples were recorded and there emission intensities were compared at a constant pump power of excitations 98.1 W/cm{sup 2}. The effect of emission intensity on decay time was also studied through focused and unfocused excitations. The synthesized material was successfully utilized in lateral finger mark detections onmore » the glass substrate through powder dusting method.« less

Interference-enhanced infrared-to-visible upconversion in solid-state thin films sensitized by colloidal nanocrystals

NASA Astrophysics Data System (ADS)

Wu, Mengfei; Jean, Joel; Bulović, Vladimir; Baldo, Marc A.

2017-05-01

Infrared-to-visible photon upconversion has potential applications in photovoltaics, sensing, and bioimaging. We demonstrate a solid-state thin-film device that utilizes sensitized triplet-triplet exciton annihilation, converting infrared photons absorbed by colloidal lead sulfide nanocrystals (NCs) into visible photons emitted from a luminescent dopant in rubrene at low incident light intensities. A typical bilayer device consisting of a monolayer of NCs and a doped film of rubrene is limited by low infrared absorption in the thin NC film. Here, we augment the bilayer with an optical spacer layer and a silver-film back reflector, resulting in interference effects that enhance the optical field and thus the absorption in the NC film. The interference-enhanced device shows an order-of-magnitude increase in the upconverted emission at the wavelength of λ = 610 nm when excited at λ = 980 nm. At incident light intensities above 1.1 W/cm2, the device attains maximum efficiency, converting (1.6 ± 0.2)% of absorbed infrared photons into higher-energy singlet excitons in rubrene.

Auger Up-Conversion of Low-Intensity Infrared Light in Engineered Quantum Dots

DOE PAGES

Makarov, Nikolay S.; Lin, Qianglu; Pietryga, Jeffrey M.; ...

2016-11-29

One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. Thismore » process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.« less

Colour emission tunability in Ho3+-Tm3+-Yb3+ co-doped Y2O3 upconverted phosphor

NASA Astrophysics Data System (ADS)

Pandey, Anurag; Rai, Vineet Kumar

2012-12-01

The frequency upconversion (UC) emission throughout the visible region from the Y2O3:Ho3+-Tm3+-Yb3+ co-doped phosphors synthesized by using low temperature combustion process upon excitation with a diode laser operating at 980 nm have been presented. The colour emission tunability in co-doped phosphor has been observed on increasing the pump power and seen by the naked eyes. The tunability in colour emission has also been visualized by CIE chromaticity diagram. The variation in UC emission intensity of the 1G4 → 3H6 (Tm3+) and 5F3 → 5I8 (Ho3+) transitions lying in the blue region has been monitored with increase in the pump power and marked that their ratio can be used to determine the temperature. The developed phosphor has been used to record fingerprints. The observed most intense visible colour emission from the developed material may be used for photodynamic therapy and as an alternative of traditional fluorescent biolabels.

One-step synthesis of NaLu80-xGdxF4:Yb183+/Er23+(Tm3+) upconversion nanoparticles for in vitro cell imaging.

PubMed

Gerelkhuu, Zayakhuu; Huy, Bui The; Sharipov, Mirkomil; Jung, Dasom; Phan, The-Long; Conte, Eric D; Lee, Yong-Ill

2018-05-01

Upconversion nanoparticles (UCNPs) possess a unique type of photoluminescence (PL) in which lower-energy excitation is converted into higher-energy emission via multi-photon absorption processes. In this work, we have used a facile one-step hydrothermal method promoted water solubility to synthesis NaLuGdF 4 :Yb 3+ /Er 3+ (Tm 3+ ) UCNPs coated with malonic acid (MA). Scanning electron microscopy images and X-ray diffraction patterns reveal sphere-shaped UCNPs with an average size of ~80nm crystallized in the cubic NaLuF 4 structure. The characteristic vibrations of cubic UCNPs have been taken into account by using Fourier-transform infrared spectroscopy. Based on PL studies, we have determined an optimal concentration of Gd 3+ doping. The dependence of upconversion PL intensity on Gd 3+ concentration is discussed via the results of magnetization measurements, which is related to the coupling/uncoupling of Gd 3+ ions. Particularly, our study reveals that carboxyl-functionalized NaLuGdF 4 :Yb 3+ /Er 3+ (Tm 3+ ) UCNPs have a relatively high cell viability with HeLa cells. Copyright © 2017 Elsevier B.V. All rights reserved.

Thermometry properties of Er, Yb-Gd2O2S microparticles: dependence on the excitation mode (cw versus pulsed excitation) and excitation wavelength (980 nm versus 1500 nm)

NASA Astrophysics Data System (ADS)

Avram, Daniel; Tiseanu, Carmen

2018-04-01

Herein, we present a first report on the luminescence thermometry properties of Er, Yb doped Gd2O2S microparticles under near infrared up-conversion excitation at 980 and 1500 nm measured in the 280-800 K interval. The thermometry properties are assessed using both cw and ns pulsed excitation as well as tuning the excitation wavelength across Yb and Er absorption profiles. For low cw (300 mW cm-1) and pulsed ns (400 ÷ 550 mW cm-1) excitation modes, no thermal load is observed. At room-temperature (280 K), the maximum relative sensitivity values are comparable under pulsed excitation at 980 and 1500 nm, around ˜0.01 and ˜0.008% K-1, respectively. In addition, a relative intense up-conversion emission at 980 nm under excitation at 1500 nm is measured. Our findings evidence attractive up-conversion and thermometry properties Er, Yb doped Gd2O2S under near-infrared excitation and highlight the need to explore further these properties in the nanoparticulate regime.

Flexible transparent displays based on core/shell upconversion nanophosphor-incorporated polymer waveguides

PubMed Central

Park, Bong Je; Hong, A-Ra; Park, Suntak; Kyung, Ki-Uk; Lee, Kwangyeol; Seong Jang, Ho

2017-01-01

Core/shell (C/S)-structured upconversion nanophosphor (UCNP)-incorporated polymer waveguide-based flexible transparent displays are demonstrated. Bright green- and blue-emitting Li(Gd,Y)F4:Yb,Er and Li(Gd,Y)F4:Yb,Tm UCNPs are synthesized via solution chemical route. Their upconversion luminescence (UCL) intensities are enhanced by the formation of C/S structure with LiYF4 shell. The Li(Gd,Y)F4:Yb,Er/LiYF4 and Li(Gd,Y)F4:Yb,Tm/LiYF4 C/S UCNPs exhibit 3.3 and 2.0 times higher UCL intensities than core counterparts, respectively. In addition, NaGdF4:Yb,Tm/NaGdF4:Eu C/S UCNPs are synthesized and they show red emission via energy transfer and migration of Yb3+ → Tm3+ → Gd3+ → Eu3+. The C/S UCNPs are incorporated into bisphenol A ethoxylate diacrylate which is used as a core material of polymer waveguides. The fabricated stripe-type polymer waveguides are highly flexible and transparent (transmittance > 90% in spectral range of 443–900 nm). The polymer waveguides exhibit bright blue, green, and red luminescence, depending on the incorporated UCNPs into the polymer core, under coupling with a near infrared (NIR) laser. Moreover, patterned polymer waveguide-based display devices are fabricated by reactive ion etching process and they realize bright blue-, green-, and red-colored characters under coupling with an NIR laser. PMID:28368021

Flexible transparent displays based on core/shell upconversion nanophosphor-incorporated polymer waveguides

NASA Astrophysics Data System (ADS)

Park, Bong Je; Hong, A.-Ra; Park, Suntak; Kyung, Ki-Uk; Lee, Kwangyeol; Seong Jang, Ho

2017-04-01

Core/shell (C/S)-structured upconversion nanophosphor (UCNP)-incorporated polymer waveguide-based flexible transparent displays are demonstrated. Bright green- and blue-emitting Li(Gd,Y)F4:Yb,Er and Li(Gd,Y)F4:Yb,Tm UCNPs are synthesized via solution chemical route. Their upconversion luminescence (UCL) intensities are enhanced by the formation of C/S structure with LiYF4 shell. The Li(Gd,Y)F4:Yb,Er/LiYF4 and Li(Gd,Y)F4:Yb,Tm/LiYF4 C/S UCNPs exhibit 3.3 and 2.0 times higher UCL intensities than core counterparts, respectively. In addition, NaGdF4:Yb,Tm/NaGdF4:Eu C/S UCNPs are synthesized and they show red emission via energy transfer and migration of Yb3+ → Tm3+ → Gd3+ → Eu3+. The C/S UCNPs are incorporated into bisphenol A ethoxylate diacrylate which is used as a core material of polymer waveguides. The fabricated stripe-type polymer waveguides are highly flexible and transparent (transmittance > 90% in spectral range of 443-900 nm). The polymer waveguides exhibit bright blue, green, and red luminescence, depending on the incorporated UCNPs into the polymer core, under coupling with a near infrared (NIR) laser. Moreover, patterned polymer waveguide-based display devices are fabricated by reactive ion etching process and they realize bright blue-, green-, and red-colored characters under coupling with an NIR laser.

Up-conversion routines of Er{sup 3+}–Yb{sup 3+} doped Y{sub 6}O{sub 5}F{sub 8} and YOF phosphors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Sangmoon, E-mail: spark@silla.ac.kr; Yang, Wonseok; Park, Chu-Young

2015-11-15

Highlights: • Single-phase optical materials of Y{sub 6}O{sub 5}F{sub 8}:Er and YOF:Er were prepared. • Effective spectral converting properties were observed in Y{sub 6}O{sub 5}F{sub 8}:Er,Yb. • 980 nm diode laser was irradiated for up-converting analysis. • A multi-photon process in the phosphors was investigated. - Abstract: Optical materials composed of a Y{sub 6(1−p−q)}Er{sub 6p}Yb{sub 6q}O{sub 5}F{sub 8} (p = 0.001–0.1, q = 0.005–0.1) solid solution with Y{sub 0.99}Er{sub 0.01}OF were prepared via a solid-state reaction using excess NH{sub 4}F flux at 950 °C for 30 min. X-ray diffraction patterns of Y{sub 6(1−p−q)}Er{sub 6p}Yb{sub 6q}O{sub 5}F{sub 8} and Y{sub 0.99}Er{submore » 0.01}OF were compared upon altering the synthesis temperature and the molar ratio of the NH{sub 4}F flux to the Y{sup 3+} (Er{sup 3+}, Yb{sup 3+}) ions. The effective spectral-conversion properties of Er{sup 3+} and Er{sup 3+}–Yb{sup 3+} ions in Y{sub 6}O{sub 5}F{sub 8} phosphors were monitored during excitation with a 980 nm wavelength diode-laser. Selection of appropriate Er{sup 3+} and/or Yb{sup 3+} concentrations in the Y{sub 6}O{sub 5}F{sub 8} structure led to achievement of the desired up-conversion emission, from the green to the red regions of the spectra. Furthermore, the mechanism of up-conversion in the phosphors was described by an energy-level schematic. Up-conversion emission spectra and the dependence of the emission intensity on pump power (between 193 and 310 mW) in the Y{sub 6(0.995−q)}Er{sub 0.03}Yb{sub 6q}O{sub 5}F{sub 8} phosphors were also investigated.« less

Color-tunable up-conversion emission in Y2O3:Yb3+, Er3+ nanoparticles prepared by polymer complex solution method

PubMed Central

2013-01-01

Abstract Powders of Y2O3 co-doped with Yb3+ and Er3+ composed of well-crystallized nanoparticles (30 to 50 nm in diameter) with no adsorbed ligand species on their surface are prepared by polymer complex solution method. These powders exhibit up-conversion emission upon 978-nm excitation with a color that can be tuned from green to red by changing the Yb3+/Er3+ concentration ratio. The mechanism underlying up-conversion color changes is presented along with material structural and optical properties. PACS 42.70.-a, 78.55.Hx, 78.60.-b PMID:23522083

Nd3+/Yb3+ cascade-sensitized single-band red upconversion emission in active-core/active-shell nanocrystals.

PubMed

Ding, M Y; Hou, J J; Yuan, Y J; Bai, W F; Lu, C H; Xi, J H; Ji, Z G; Chen, D Q

2018-08-24

Lanthanide-doped upconversion nanomaterials (UCNMs) have promoted extensive interest for its biological research and biomedical applications, benefiting from low autofluorescence background, deep light penetration depth, and minimal photo-damage to biological tissues. However, owing to the 980 nm laser-induced overheating issue and the attenuation effect associated with conventional multi-peak emissions, the usage of UCNMs as fluorescent bioprobes is still limited. To address these issues, an effective strategy has been proposed to tune both the excitation and emission peaks of UCNMs into the first biological window (650 ∼ 900 nm), where the light absorption by water and hemoglobin in biological tissues is minimal. Based on the Nd 3+ /Yb 3+ cascade-sensitized upconversion process and efficient exchange-energy transfer between Mn 2+ and Er 3+ in conjunction with the active-core@active-shell nanostructured design, we have developed a new class of upconversion nanoparticles (UCNPs) that exhibit strong single-band red emission upon excitation of an 808 nm near-infrared laser. Hopefully, the well-designed KMnF 3 :Yb/Er/Nd@ KMnF 3 :Yb/Nd core-shell nanocrystals will be considered a promising alternative to conventionally used UCNPs for biolabeling applications without the concern of the overheating issue and the attenuation constraints.

Er3+ -doped anatase TiO2 nanocrystals: crystal-field levels, excited-state dynamics, upconversion, and defect luminescence.

PubMed

Luo, Wenqin; Fu, Chengyu; Li, Renfu; Liu, Yongsheng; Zhu, Haomiao; Chen, Xueyuan

2011-11-04

A comprehensive survey of electronic structure and optical properties of rare-earth ions embedded in semiconductor nanocrystals (NCs) is of vital importance for their potential applications in areas as diverse as luminescent bioprobes, lighting, and displays. Er3+ -doped anatase TiO2 NCs, synthesized via a facile sol-gel solvothermal method, exhibit intense and well-resolved intra-4f emissions of Er3+ . Crystal-field (CF) spectra of Er3+ in TiO2 NCs are systematically studied by means of high-resolution emission and excitation spectra at 10-300 K. The CF analysis of Er3+ assuming a site symmetry of C(2v) yields a small root-mean-square deviation of 25.1 cm(-1) and reveals the relatively large CF strength (549 cm(-1) ) of Er3+, thus verifying the rationality of the C(2v) symmetry assignment of Er3+ in anatase TiO2 NCs. Based on a simplified thermalization model for the temperature-dependent photoluminescence (PL) dynamics from (4) S(3/2) , the intrinsic radiative luminescence lifetimes of (4) S(3/2) and (2) H(11/2) are experimentally determined to be 3.70 and 1.73 μs, respectively. Green and red upconversion (UC) luminescence of Er3+ can be achieved upon laser excitation at 974.5 nm. The UC intensity of Er3+ in Yb/Er-codoped NCs is found to be about five times higher than that of Er-singly-doped counterparts as a result of efficient Yb3+ sensitization and energy transfer upconversion (ETU) evidenced by its distinct UC luminescence dynamics. Furthermore, the origin of defect luminescence is revealed based on the temperature-dependent PL spectra upon excitation above the TiO2 bandgap at 325 nm. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Paradigms and challenges for bioapplication of rare earth upconversion luminescent nanoparticles: small size and tunable emission/excitation spectra.

PubMed

Sun, Ling-Dong; Wang, Ye-Fu; Yan, Chun-Hua

2014-04-15

Rare earth (RE) materials, which are excited in the ultraviolet and emit in the visible light spectrum, are widely used as phosphors for lamps and displays. In the 1960's, researchers reported an abnormal emission phenomenon where photons emitted from a RE element carried more energy than those absorbed, owing to the sequential energy transfer between two RE ions--Yb(3+)-sensitized Er(3+) or Tm(3+)--in the solid state. After further study, researchers named this abnormal emission phenomenon upconversion (UC) emission. More recent approaches take advantage of solution-based synthesis, which allows creation of homogenous RE nanoparticles (NPs) with controlled size and structure that are capable of UC emission. Such nanoparticles are useful for many applications, especially in biology. For these applications, researchers seek small NPs with high upconversion emission intensity. These UCNPs have the potential to have multicolor and tunable emissions via various activators. A vast potential for future development remains by developing molecular antennas and energy transfer within RE ions. We expect UCNPs with optimized spectra behavior to meet the increasing demand of potential applications in bioimaging, biological detection, and light conversion. This Account focuses on efforts to control the size and modulate the spectra of UCNPs. We first review efforts in size control. One method is careful control of the synthesis conditions to manipulate particle nucleation and growth, but more recently researchers have learned that the doping conditions can affect the size of UCNPs. In addition, constructing homogeneous core/shell structures can control nanoparticle size by adjusting the shell thickness. After reviewing size control, we consider how diverse applications impose different requirements on excitation and/or emission photons and review recent developments on tuning of UC spectral profiles, especially the extension of excitation/emission wavelengths and the adjustment and purification of emission colors. We describe strategies that employ various dopants and others that build rationally designed nanostructures and nanocomposites to meet these goals. As the understanding of the energy transfer in the UC process has improved, core/shell structures have been proved useful for simultaneous tuning of excitation and emission wavelengths. Finally, we present a number of typical examples to highlight the upconverted emission in various applications, including imaging, detection, and sensing. We believe that with deeper understanding of emission phenomena and the ability to tune spectral profiles, UCNPs could play an important role in light conversion studies and applications.

Multicolor tunability and upconversion enhancement of fluoride nanoparticles by oxygen dopant

NASA Astrophysics Data System (ADS)

Niu, Wenbin; Wu, Suli; Zhang, Shufen; Su, Liap Tat; Tok, Alfred Iing Yoong

2013-08-01

The ability to manipulate the upconversion luminescence of lanthanide-ion doped fluoride upconversion nanoparticles (UCNPs) is particularly important and highly desired due to their wide applications in color displays, multiplexing bioassays and multicolor imaging. Here, we developed a strategy for simultaneously tuning color output and enhancing upconversion emission of Yb/Er doped fluoride UCNPs, based on adjusting the oxygen doping level. The synthesis of multicolored multifunctional NaGdF4:Yb,Er UCNPs was used as the model host system to demonstrate this protocol. Ammonium nitrate (NH4NO3) was used as the oxygen source and added into the reaction system at the beginning stage of nucleation and growth process of fluoride UCNPs, which facilitates the formation of enough oxygen atoms and the diffusion of these into the fluoride host matrix. The results revealed that multicolour output and upconversion enhancement mainly resulted from the variation of phonon energy and crystal field symmetry of the host lattice, respectively. This strategy can be further expanded to other fluoride host matrices. As an example of an application, multicolored UCNPs were used as a color converter in light emitting diodes, which can effectively convert near-infrared light into visible light. It is expected that these multicolored UCNPs will be promising for applications in multiplexing biodetection, bioimaging (optical and magnetic resonance imaging) and other optical technologies, and the present method for the control of O2- doping may also be used in other functional nanomaterials.The ability to manipulate the upconversion luminescence of lanthanide-ion doped fluoride upconversion nanoparticles (UCNPs) is particularly important and highly desired due to their wide applications in color displays, multiplexing bioassays and multicolor imaging. Here, we developed a strategy for simultaneously tuning color output and enhancing upconversion emission of Yb/Er doped fluoride UCNPs, based on adjusting the oxygen doping level. The synthesis of multicolored multifunctional NaGdF4:Yb,Er UCNPs was used as the model host system to demonstrate this protocol. Ammonium nitrate (NH4NO3) was used as the oxygen source and added into the reaction system at the beginning stage of nucleation and growth process of fluoride UCNPs, which facilitates the formation of enough oxygen atoms and the diffusion of these into the fluoride host matrix. The results revealed that multicolour output and upconversion enhancement mainly resulted from the variation of phonon energy and crystal field symmetry of the host lattice, respectively. This strategy can be further expanded to other fluoride host matrices. As an example of an application, multicolored UCNPs were used as a color converter in light emitting diodes, which can effectively convert near-infrared light into visible light. It is expected that these multicolored UCNPs will be promising for applications in multiplexing biodetection, bioimaging (optical and magnetic resonance imaging) and other optical technologies, and the present method for the control of O2- doping may also be used in other functional nanomaterials. Electronic supplementary information (ESI) available: Upconversion spectra of NaYF4:Yb,Er UCNPs prepared with various oxygen sources (trimethylamine N-oxide and ammonium carbonate, Fig. S1) and different addition temperatures of NH4NO3 (Fig. S2), enlarged XRD patterns (Fig. S3), the intensity ratios of green to red emissions of NaGdF4:Yb,Er UCNPs prepared with various amounts of NH4NO3 (Fig. S4), power dependence of upconversion spectra of NaGdF4:Yb,Er UCNPs prepared at 300 °C for 1 h (Fig. S5), upconversion spectra of the product after further reaction between as-prepared NaYF4:Yb,Er and 50 mg of NH4NO3 at 300 °C for 1 h (Fig. S6), XRD patterns of NaYF4:Yb,Er and NaLuF4:Yb,Er UCNPs prepared with various amounts of NH4NO3 (Fig. S7 and S8), the corresponding magnetization curves of NaGdF4:Yb,Er UCNPs (Fig. S9). See DOI: 10.1039/c3nr01612a

Using lead chalcogenide nanocrystals as spin mixers: a perspective on near-infrared-to-visible upconversion.

PubMed

Nienhaus, Lea; Wu, Mengfei; Bulović, Vladimir; Baldo, Marc A; Bawendi, Moungi G

2018-03-01

The process of upconversion leads to emission of photons higher in energy than the incident photons. Near-infrared-to-visible upconversion, in particular, shows promise in sub-bandgap sensitization of silicon and other optoelectronic materials, resulting in potential applications ranging from photovoltaics that exceed the Shockley-Queisser limit to infrared imaging. A feasible mechanism for near-infrared-to-visible upconversion is triplet-triplet annihilation (TTA) sensitized by colloidal nanocrystals (NCs). Here, the long lifetime of spin-triplet excitons in the organic materials that undergo TTA makes upconversion possible under incoherent excitation at relatively low photon fluxes. Since this process relies on optically inactive triplet states, semiconductor NCs are utilized as efficient spin mixers, absorbing the incident light and sensitizing the triplet states of the TTA material. The state-of-the-art system uses rubrene with a triplet energy of 1.14 eV as the TTA medium, and thus allows upconversion of light with photon energies above ∼1.1 eV. In this perspective, we review the field of lead sulfide (PbS) NC-sensitized near-infrared-to-visible upconversion, discuss solution-based upconversion, and highlight progress made on solid-state upconversion devices.

Tunable green/red luminescence by infrared upconversion in biocompatible forsterite nanoparticles with high erbium doping uptake

NASA Astrophysics Data System (ADS)

Zampiva, Rúbia Young Sun; Acauan, Luiz Henrique; Venturini, Janio; Garcia, Jose Augusto Martins; da Silva, Diego Silverio; Han, Zhaohong; Kassab, Luciana Reyes Pires; Wetter, Niklaus Ursus; Agarwal, Anuradha; Alves, Annelise Kopp; Bergmann, Carlos Pérez

2018-02-01

Nanoparticles represent a promising platform for diagnostics and therapy of human diseases. For biomedical applications, these nanoparticles are usually coated with photosensitizers regularly activated in a spectral window of 530-700 nm. The emissions at 530 nm (green) and 660 nm (red) are of particular interest for imaging and photodynamic therapy, respectively. This work presents the Mg2SiO4:Er3+ system, produced by reverse strike co-precipitation, with up to 10% dopant and no secondary phase formation. These nanoparticles when excited at 985 nm show upconversion emission with peaks around 530 and 660 nm, although excitation at 808 nm leads to only a single emission peak at around 530 nm. The direct upconversion of this biomaterial without a co-dopant, and its tunability by the excitation source, renders Mg2SiO4:Er3+ nanoparticles a promising system for biomedical applications.

Solar-Pumping Upconversion of Interfacial Coordination Nanoparticles.

PubMed

Ishii, Ayumi; Hasegawa, Miki

2017-01-30

An interfacial coordination nanoparticle successfully exhibited an upconversion blue emission excited by very low-power light irradiation, such as sunlight. The interfacial complex was composed of Yb ions and indigo dye, which formed a nano-ordered thin shell layer on a Tm 2 O 3 nanoparticle. At the surface of the Tm 2 O 3 particle, the indigo dye can be excited by non-laser excitation at 640 nm, following the intramolecular energy transfer from the indigo dye to the Yb ions. Additionally, the excitation energy of the Yb ion was upconverted to the blue emission of the Tm ion at 475 nm. This upconversion blue emission was achieved by excitation with a CW Xe lamp at an excitation power of 0.14 mW/cm 2 , which is significantly lower than the solar irradiation power of 1.4 mW/cm 2 at 640 ± 5 nm.

Tuning sputtered gold thickness to enhance absorption and emission in core-shell type erbium doped upconversion nanoparticles

NASA Astrophysics Data System (ADS)

Manurung, R. V.; Wu, C. T.; Chattopadhyay, S.

2018-03-01

Upconversion nanoparticles (UCNPs) converts near-infrared excitation to visible emission with advantages e.g. photostable, non-blinking, and background-free probes for bioimaging and biosensor. However, low quantum yield and low efficiency (∼1%) as drawback need to be enhanced. A plasmonic gold nano-structured surface was designed and fabricated to couple with the 980 nm radiation and produce plasmonic enhancement of the upconversion luminescence. The synthesis of the UCNPs was done by thermal decomposition and SiO2 coating prepared by the reverse microemulsion process. Here, we report a novel tunable plasmon-enhanced fluorescence by modulating the thickness and surface roughness of gold island film on Si. The localized surface plasmon resonance (LSPR) at 980 nm was obtained, matched with the native excitation of UCNPs resulting in maximum enhancement of 10-fold of green emission band at 540 nm for the Er-doped UCNPs.

Synthetic and spectroscopic studies of vanadate glaserites I: Upconversion studies of doubly co-doped (Er, Tm, or Ho):Yb:K{sub 3}Y(VO{sub 4}){sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kimani, Martin M., E-mail: kimani@g.clemson.edu; Chen, Hongyu, E-mail: hongyuc@g.clemson.edu; McMillen, Colin D., E-mail: cmcmill@g.clemson.edu

2015-03-15

The synthesis and upconversion properties of trigonal glaserite-type K{sub 3}Y(VO{sub 4}){sub 2} co-doped with Er{sup 3+}/Yb{sup 3+}, Ho{sup 3+}/Yb{sup 3+}, or Tm{sup 3+}/Yb{sup 3+} were studied. Powder samples were synthesized by solid state reactions at 1000 °C for 48 h, while well-formed hexagonal single crystals of the same were grown hydrothermally using 10 M K{sub 2}CO{sub 3} at 560–650 °C. Infrared-to-visible upconversion by Er{sup 3+}/Yb{sup 3+}, Ho{sup 3+}/Yb{sup 3+}, or Tm{sup 3+}/Yb{sup 3+} codoped-K{sub 3}Y(VO{sub 4}){sub 2} glaserite powder and single crystals was observed, and the upconversion spectral properties were studied as a function of different Er{sup 3+}, Tm{sup 3+},more » Ho{sup 3+}, and Yb{sup 3+} ion concentrations. The process is observed under 980 nm laser diode excitation and leads to strong green (552 nm) and red (659 nm) emission for Er{sup 3+}/Yb{sup 3+}, green (549 nm) and red (664 nm) emission for Ho{sup 3+}/Yb{sup 3+}, and blue (475 nm) and red (647 nm) emission for Tm{sup 3+}/Yb{sup 3+}. The main mechanism that allows for up-conversion is attributed the energy transfer among Yb{sup 3+} and the various Er{sup 3+}/Ho{sup 3+}/Tm{sup 3+} ions in excited states. These results illustrate the large potential of co-doped alkali double vanadates for photonic applications involving optoelectronics devices. - Graphical abstract: Synthesis and upconversion in vanadate glaserites. - Highlights: • K{sub 3}Y(VO{sub 4}){sub 2} codoped with Er, Tm, or Ho:Yb were synthesized via solid-state and hydrothermal routes. • Upconversion properties are investigated. • The codoped compounds revealed efficient infrared-to-visible upconversion. • The presented compounds are potential host for solid state lighting.« less

Upconversion excitations in Pr3+-doped BaY2F8 crystal

NASA Astrophysics Data System (ADS)

Piramidowicz, R.; Mahiou, R.; Boutinaud, P.; Malinowski, M.

2011-09-01

We report the orange-to-blue and infrared-(IR)-to-blue wavelengths upconversion luminescence in Pr3+:BaY2F8 crystals. Mechanism of the orange light upconversion into blue 3P0 state emission was confirmed to be energy transfer between two Pr3+ ions in the 1D2 state. IR-to-blue upconversion has only been observed under two different color IR pumping. The first resonant step was the 3H4→1G4 ground state absorption transition, and the second resonant transition was the excited state absorption from the 1G4 to 1I6 and 3PJ levels. A comparison of the efficiency of the IR-to-blue upconversion in several praseodymium activated host is presented and discussed. A model of the IR pumped upconversion praseodymium blue laser is presented and the population inversion conditions are calculated.

Enhanced frequency upconversion study in Er3+/Yb3+ doped/codoped TWTi glasses

NASA Astrophysics Data System (ADS)

Azam, Mohd; Rai, Vineet Kumar

2018-04-01

Er3+/Yb3+ doped/codoped TeO2-WO3-TiO2 (TWTi) glasses have been prepared by using the melt-quenching technique. The upconversion (UC) emission spectra of the developed glasses have been recorded upon 980 nm laser excitation. Three intense UC emission bands have been observed within the green and red region centered at ˜532 nm, ˜553 nm and ˜669 nm corresponding to the 2H11/2→4I15/2, 4S3/2→4I15/2 and 4F9/2→4I15/2 transitions respectively in the singly Er3+ doped glass. On introducing Yb3+ ions in the singly Er3+ doped glass, an enhancement of about ˜ 12 times and ˜50 times in the green and red bands respectively have been observed even at low pump power ˜ 364 mW followed by two photon absorption process. Colour tunability from yellowish green to pure green colour region has been observed on varying the pump power. The prepared glass can be used to produce NIR to green upconverter and colour tunable display devices.

Annihilation limit of a visible-to-UV photon upconversion composition ascertained from transient absorption kinetics.

PubMed

Deng, Fan; Blumhoff, Jörg; Castellano, Felix N

2013-05-30

Noncoherent sensitized green-to-near-visible upconversion has been achieved utilizing palladium(II) octaethylporphyrin (PdOEP) as the triplet sensitizer and anthracene as the energy acceptor/annihilator in vacuum degassed toluene. Selective 547 nm excitation of PdOEP with incident irradiance as low as 600 μW/cm(2) results in the observation of anthryl fluorescence at higher energy. Stern-Volmer analysis of the dynamic phosphorescence quenching of PdOEP by anthracene possesses an extremely large K(SV) of 810,000 M(-1), yielding a triplet-triplet energy transfer quenching constant of 3.3 × 10(9) M(-1) s(-1). Clear evidence for the subsequent triplet-triplet annihilation (TTA) of anthracene was afforded by numerous experiments, one of the most compelling was an excitation scan illustrating that the Q-band absorption features of PdOEP are solely responsible for sensitizing the anti-Stokes fluorescence. The upconverted emission intensity with respect to the excitation power was shown to vary between quadratic and linear using either coherent or noncoherent light sources, illustrating the expected kinetic limits for the light producing photochemistry under continuous wave illumination. Time-resolved experiments directly comparing the total integrated anthracene intensity/time fluorescence data produced through upconversion (λ(ex) = 547 nm, delayed signal) and with direct excitation (λ(ex) = 355 nm, prompt signal) under conditions where the laser pulse is completely absorbed by the sample reveal annihilation efficiencies of approximately 40%. Similarly, the delayed fluorescence kinetic analysis reported by Schmidt and co-workers (J. Phys. Chem. Lett. 2010, 1, 1795-1799) was used to reveal the maximum possible efficiency from a model red-to-yellow upconverting composition and this treatment was applied to the anthryl triplet absorption decay transients of anthracene measured for the PdOEP/anthracene composition at 430 nm. From this analysis approximately 50% of the anthryl triplets that decay by TTA produce singlet fluorescence, consistent with the notion that annihilation spin statistics does not impose efficiency limits on upconversion photochemistry.

A temperature sensor based on the enhanced upconversion luminescence of Li+ doped NaLuF4:Yb3+,Tm3+/Er3+ nano/microcrystals.

PubMed

Qiang, Qinping; Du, Shanshan; Ma, Xinlong; Chen, Wenbo; Zhang, Gangyi; Wang, Yuhua

2018-05-09

In this paper, fluorescent and optical temperature sensing bi-functional Li+-doping NaLuF4:Ln (Ln = Yb3+, Tm3+/Er3+) nanocrystals were synthesized via a simple hydrothermal method using oleic acid as a capping ligand. The crystal phase, size, upconversion (UC) properties, and optical temperature sensing characteristics of the crystals can be easily modified by Li+ doping. The results reveal that additional Li+ can promote the transformation from the hexagonal phase to the cubic phase and reduce the size of the nanocrystals. In addition, NaLuF4:Ln (Ln = Yb3+, Tm3+, Li+) nanocrystals present efficient near infrared (NIR) emission, which is beneficial for in vivo biomedical applications due to the increased penetration depth and low radiation damage of NIR light in bio-tissues. More importantly, under 980 nm excitation, the temperature dependent UCL from the 2H11/2 and 4S3/2 levels of Er3+ ions in NaLuF4:Yb3+,Er3+,Li+ microcrystals was investigated systematically. The fluorescence intensity ratios (FIR) of the pairs of thermally coupled levels were studied as a function of temperature in the range of 298-523 K. The maximum sensor sensitivities were found to be about 0.0039 K-1 (523 K) by exploiting the UC emissions from the 2H11/2 and 4S3/2 levels. This suggests that the Li+-doped upconversion luminescence (UCL) materials are promising prototypes for application as multi-mode probes for use in bio-separation and optical thermometers.

Luminescence studies and infrared emission of erbium-doped calcium zirconate phosphor.

PubMed

Tiwari, Neha; Dubey, Vikas

2016-05-01

The near-infrared-to-visible upconversion luminescence behaviour of Er(3+)-doped CaZrO3 phosphor is discussed in this manuscript. The phosphor was prepared by a combustion synthesis technique that is suitable for less-time-taking techniques for nanophosphors. The starting materials used for sample preparation were Ca(NO3)2.4H2O, Zr(NO3)4 and Er(NO3)2, and urea was used as a fuel. The prepared sample was characterized by X-ray diffraction (XRD). The surface morphology of prepared phosphor was determined by field emission gun scanning electron microscopy (FEGSEM). The functional group analysis was determined by Fourier transform infrared (FTIR) spectroscopy. All prepared phosphors with variable Er(3+) concentrations (0.5-2.5 mol%) were studied by photoluminescence analysis. It was found that the excitation spectra of the prepared phosphor showed a sharp excitation peak centred at 980 nm. The emission spectra with variable Er(3+) concentrations showed strong peaks in the 555 nm and 567 nm range, with a dominant peak at 555 nm due to the ((2)H(11/2),(4)S(3/2)) transition and a weaker transition at 567 nm associated with 527 nm. Spectrophotometric determination of the peak was evaluated by the Commission Internationale de I'Eclairage (CIE) method These upconverted emissions were attributed to a two-photon process. The excitation wavelength dependence of the upconverted luminescence, together with its time evolution after infrared pulsed excitation, suggested that energy transfer upconversion processes were responsible for the upconversion luminescence. The upconversion mechanisms were studied in detail through laser power dependence. Excited state absorption and energy transfer processes were discussed as possible upconversion mechanisms. The cross-relaxation process in Er(3+) was also investigated. Copyright © 2015 John Wiley & Sons, Ltd.

Enhanced electrical properties, color-tunable up-conversion luminescence, and temperature sensing behaviour in Er-doped Bi3Ti1.5W0.5O9 multifunctional ferroelectric ceramics

NASA Astrophysics Data System (ADS)

Zhang, Ying; Li, Jun; Chai, Xiaona; Wang, Xusheng; Li, Yongxiang; Yao, Xi

2017-03-01

Er-doped Bi3Ti1.5W0.5O9 (BTW-x) ferroelectric ceramics were prepared by a conventional solid-state reaction synthesis method, and their structure, electrical properties, up-conversion (UC) luminescence, and temperature sensing behaviour were investigated. A high piezoelectric coefficient d33 (9.6 pC/N), a large remnant polarization Pr (12.75 μC/cm2), a high Curie temperature Tc (730.2 °C), and the optimal luminescent intensity are obtained for the samples at x = 0.05. By changing the Er doped concentration, the BTW-x ceramics are capable of generating various UC spectra and the color could be tunable from green to yellow. According to the fluorescence intensity ratio of green emissions at 532.6 nm and 549.2 nm in the temperature range from 83 K to 423 K, optical temperature sensing properties are investigated and the maximum sensing sensitivity is found to be 0.00314 K-1 at 423 K. The results conclude that BTW-x would be a candidate in high temperature sensor, fluorescence thermometry, and opto-electronic integration applications.

Luminescence of Er/Yb and Tm/Yb doped FAp nanoparticles and ceramics

NASA Astrophysics Data System (ADS)

Grigorjeva, L.; Smits, K.; Millers, D.; Jankoviča, Dz

2015-03-01

The nanoparticles of hydroxiapatite and fluorapatite doped with Er/Yb and Tm/Yb were synthesized and characterized by FTIR, XRD, SEM and TEM methods. The results of up-conversion luminescence studies were presented for the samples as prepared, annealed at 500°C and at 900-1000 °C. At annealing above 800°C the ceramic state was formed. It is shown that fluorapatite host is more appropriate than hydroxiapatite host for rare ions luminescence and up-conversion processes. The post preparing annealing of nanarticles significantly enhanced the luminescence intensity. The Tm/Yb doped fluorapatite shows intense up-conversion luminescence in 790-800 nm spectral region and is potentially useful for biomedical applications.

Experimental demonstration of plasmon enhanced energy transfer rate in NaYF4:Yb3+,Er3+ upconversion nanoparticles

PubMed Central

Lu, Dawei; Mao, Chenchen; Cho, Suehyun K.; Ahn, Sungmo; Park, Wounjhang

2016-01-01

Energy transfer upconversion (ETU) is known to be the most efficient frequency upconversion mechanism. Surface plasmon can further enhance the upconversion process, opening doors to many applications. However, ETU is a complex process involving competing transitions between multiple energy levels and it has been difficult to precisely determine the enhancement mechanisms. In this paper, we report a systematic study on the dynamics of the ETU process in NaYF4:Yb3+,Er3+ nanoparticles deposited on plasmonic nanograting structure. From the transient near-infrared photoluminescence under various excitation power densities, we observed faster energy transfer rates under stronger excitation conditions until it reached saturation where the highest internal upconversion efficiency was achieved. The experimental data were analyzed using the complete set of rate equations. The internal upconversion efficiency was found to be 56% and 36%, respectively, with and without the plasmonic nanograting. We also analyzed the transient green emission and found that it is determined by the infrared transition rate. To our knowledge, this is the first report of experimentally measured internal upconversion efficiency in plasmon enhanced upconversion material. Our work decouples the internal upconversion efficiency from the overall upconverted luminescence efficiency, allowing more targeted engineering for efficiency improvement. PMID:26739230

Tunable upconversion luminescence of monodisperse Y2O3: Er3+/Yb3+/Tm3+ nanoparticles

NASA Astrophysics Data System (ADS)

Wu, Qibai; Lin, Shaoteng; Xie, Zhongxiang; Zhang, Liqing; Qian, Yannan; Wang, Yaodong; Zhang, Haiyan

2017-12-01

Monodisperse Y2O3: Er3+/Yb3+/Tm3+ nanoparticles with various dopant concentrations have been synthesized successfully by a homogeneous precipitation method. Their phase structures and surface morphologies have been characterized using X-ray diffraction (XRD) and scanning electron microscopy (SEM). The diversities of upconversion luminescence spectra and CIE coordinates of prepared samples are investigated in detail at room temperature under 980 nm excitation. Through adjusting the concentrations of Yb3+, Tm3+ and Er3+ ions, three upconversion emission bands in red, green and blue region could be tunable to achieve the color of interest and near white light emission can be obtained in the tri-doped Y2O3 nanoparticles for a variety of application.

Strategy for thermometry via Tm³⁺-doped NaYF₄ core-shell nanoparticles.

PubMed

Zhou, Shaoshuai; Jiang, Guicheng; Li, Xinyue; Jiang, Sha; Wei, Xiantao; Chen, Yonghu; Yin, Min; Duan, Changkui

2014-12-01

Optical thermometers usually make use of the fluorescence intensity ratio of two thermally coupled energy levels, with the relative sensitivity constrained by the limited energy gap. Here we develop a strategy by using the upconversion (UC) emissions originating from two multiplets with opposite temperature dependences to achieve higher relative temperature sensitivity. We show that the intensity ratio of the two UC emissions, ³F(2,3) and ¹G₄, of Tm³⁺ in β-NaYF₄:20%Yb³⁺, 0.5%Tm³⁺/NaYF₄:1%Pr³⁺ core-shell nanoparticles under 980 nm laser excitation exhibits high relative temperature sensitivity between 350 and 510 K, with a maximum of 1.53%  K⁻¹ at 417 K. This demonstrates the validity of the strategy, and that the studied material has the potential for high-performance optical thermometry.

The Intersection of CMOS Microsystems and Upconversion Nanoparticles for Luminescence Bioimaging and Bioassays

PubMed Central

Wei, Liping.; Doughan, Samer.; Han, Yi.; DaCosta, Matthew V.; Krull, Ulrich J.; Ho, Derek.

2014-01-01

Organic fluorophores and quantum dots are ubiquitous as contrast agents for bio-imaging and as labels in bioassays to enable the detection of biological targets and processes. Upconversion nanoparticles (UCNPs) offer a different set of opportunities as labels in bioassays and for bioimaging. UCNPs are excited at near-infrared (NIR) wavelengths where biological molecules are optically transparent, and their luminesce in the visible and ultraviolet (UV) wavelength range is suitable for detection using complementary metal-oxide-semiconductor (CMOS) technology. These nanoparticles provide multiple sharp emission bands, long lifetimes, tunable emission, high photostability, and low cytotoxicity, which render them particularly useful for bio-imaging applications and multiplexed bioassays. This paper surveys several key concepts surrounding upconversion nanoparticles and the systems that detect and process the corresponding luminescence signals. The principle of photon upconversion, tuning of emission wavelengths, UCNP bioassays, and UCNP time-resolved techniques are described. Electronic readout systems for signal detection and processing suitable for UCNP luminescence using CMOS technology are discussed. This includes recent progress in miniaturized detectors, integrated spectral sensing, and high-precision time-domain circuits. Emphasis is placed on the physical attributes of UCNPs that map strongly to the technical features that CMOS devices excel in delivering, exploring the interoperability between the two technologies. PMID:25211198

Yb3+/Ho3+ Co-Doped Apatite Upconversion Nanoparticles to Distinguish Implanted Material from Bone Tissue.

PubMed

Li, Xiyu; Chen, Haifeng

2016-10-07

The exploration of bone reconstruction with time requires the combination of a biological method and a chemical technique. Lanthanide Yb 3+ and Ho 3+ co-doped fluorapatite (FA:Yb 3+ /Ho 3+ ) and hydroxyapatite (HA:Yb 3+ /Ho 3+ ) particles with varying dopant concentrations were prepared by hydrothermal synthesis and thermal activation. Controllable green and red upconversion emissions were generated under 980 nm near-infrared excitation; the FA:Yb 3+ /Ho 3+ particles resulted in superior green luminescence, while HA:Yb 3+ /Ho 3+ dominated in red emission. The difference in the green and red emission behavior was dependent on the lattice structure and composition. Two possible lattice models were proposed for Yb 3+ /Ho 3+ co-doped HA and FA along the hydroxyl channel and fluorine channel of the apatite crystal structure. We first reported the use of the upconversion apatite particles to clearly distinguish implanted material from bone tissue on stained histological sections of harvested in vivo samples. The superposition of the tissue image and material image is a creative method to show the material-tissue distribution and interrelation. The upconversion apatite particles and image superposition method provide a novel strategy for long-term discriminable fluorescence tracking of implanted material or scaffold during bone regeneration.

Energy Migration Upconversion in Manganese(II)-Doped Nanoparticles.

PubMed

Li, Xiyan; Liu, Xiaowang; Chevrier, Daniel M; Qin, Xian; Xie, Xiaoji; Song, Shuyan; Zhang, Hongjie; Zhang, Peng; Liu, Xiaogang

2015-11-02

We report the synthesis and characterization of cubic NaGdF4:Yb/Tm@NaGdF4:Mn core-shell structures. By taking advantage of energy transfer through Yb→Tm→Gd→Mn in these core-shell nanoparticles, we have realized upconversion emission of Mn(2+) at room temperature in lanthanide tetrafluoride based host lattices. The upconverted Mn(2+) emission, enabled by trapping the excitation energy through a Gd(3+) lattice, was validated by the observation of a decreased lifetime from 941 to 532 μs in the emission of Gd(3+) at 310 nm ((6)P(7/2)→(8)S(7/2)). This multiphoton upconversion process can be further enhanced under pulsed laser excitation at high power densities. Both experimental and theoretical studies provide evidence for Mn(2+) doping in the lanthanide-based host lattice arising from the formation of F(-) vacancies around Mn(2+) ions to maintain charge neutrality in the shell layer. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Spectroscopy and enhanced frequency upconversion in Nd3+-Yb3+ codoped TPO glasses: energy transfer and NIR to visible upconverter.

PubMed

Azam, Mohd; Rai, Vineet Kumar; Mohanty, Deepak Kumar

2017-09-22

TeO 2 -Pb 3 O 4 (TPO) glasses codoped with Nd 3+ and Yb 3+ ions have been fabricated by conventional melting technique. The absorption, emission and excitation spectra of the samples have been recorded. The optical band gap in both the doped/codoped glasses is found to be ∼3.31 eV. Judd-Ofelt analysis has been carried out by using the absorption spectrum of 0.8 mol% Nd 3+ doped glass to determine the radiative properties viz radiative transition probabilities, branching ratios, radiative lifetimes, quality factor and emission cross sections of some emitting levels for Nd 3+ ions. The radiative transition probability for the 4 G 7/2  →  4 I 9/2 transition (∼1926 Hz) is found to be maximum compared to other 4 G 5/2  →  4 I 9/2 (∼1622 Hz) and 4 F 5/2  →  4 I 9/2 (∼865 Hz) transitions. Upconversion (UC) luminescence of the samples has been examined by the 980 nm CW diode laser excitation. Effect of addition of Yb 3+ ions in the Nd 3+ doped glasses on UC emission intensity has been discussed. The UC emission intensity corresponding to the green, red and NIR bands in the codoped glass has been enhanced by ∼17, ∼12 and ∼42 times as compared to that of the Nd 3+ singly doped glass. The quantum efficiency for the 4 G 7/2 level is found to be ∼32%. The nephelauxetic ratio, bonding parameter and covalency of Nd 3+ ions have been found positive which represents the covalent bonding between Nd 3+ ion and oxygen atom. The colour tunability from yellowish-green to dominant green region has been obtained in the optimized codoped TPO glass.

Spectroscopy and enhanced frequency upconversion in Nd3+-Yb3+ codoped TPO glasses: energy transfer and NIR to visible upconverter

NASA Astrophysics Data System (ADS)

Azam, Mohd; Rai, Vineet Kumar; Mohanty, Deepak Kumar

2017-09-01

TeO2-Pb3O4 (TPO) glasses codoped with Nd3+ and Yb3+ ions have been fabricated by conventional melting technique. The absorption, emission and excitation spectra of the samples have been recorded. The optical band gap in both the doped/codoped glasses is found to be ˜3.31 eV. Judd-Ofelt analysis has been carried out by using the absorption spectrum of 0.8 mol% Nd3+ doped glass to determine the radiative properties viz radiative transition probabilities, branching ratios, radiative lifetimes, quality factor and emission cross sections of some emitting levels for Nd3+ ions. The radiative transition probability for the 4G7/2 → 4I9/2 transition (˜1926 Hz) is found to be maximum compared to other 4G5/2 → 4I9/2 (˜1622 Hz) and 4F5/2 → 4I9/2 (˜865 Hz) transitions. Upconversion (UC) luminescence of the samples has been examined by the 980 nm CW diode laser excitation. Effect of addition of Yb3+ ions in the Nd3+ doped glasses on UC emission intensity has been discussed. The UC emission intensity corresponding to the green, red and NIR bands in the codoped glass has been enhanced by ˜17, ˜12 and ˜42 times as compared to that of the Nd3+ singly doped glass. The quantum efficiency for the 4G7/2 level is found to be ˜32%. The nephelauxetic ratio, bonding parameter and covalency of Nd3+ ions have been found positive which represents the covalent bonding between Nd3+ ion and oxygen atom. The colour tunability from yellowish-green to dominant green region has been obtained in the optimized codoped TPO glass.

Crystal growth and upconversion luminescent properties of KLu2F7:Yb,Er nanocrystals

NASA Astrophysics Data System (ADS)

Xu, Dekang; Yao, Lu; Lin, Hao; Yang, Shenghong; Zhang, Yueli

2018-05-01

Crystal growth of KLu2F7 nanocrystals is investigated by dosage- and time-dependent analysis. XRD patterns reveal the phase transition along with the dosage of fluorine source and reaction times, where the cubic-phase KLu3F10 turns into orthorhombic KLu2F7. TEM images show that the dimensions of as-prepared samples are below a hundred nanometers, with different shapes from hexagonal plate to hexagonal rod. The upconversion properties of the as-prepared samples are investigated. It is found that the upconversion emission is lowered as the shape of the samples varies. Moreover, the orthorhombic KLu2F7:Yb,Er nanocrystals present more enormous upconversion luminescence than the cubic counterparts. In a word, the orthorhombic nanocrystals are found to be good candidate for upconversion luminescence and of great importance for potential applications in solar cells, multicolor display and bioimaging.

Energy-Cascaded Upconversion in an Organic Dye-Sensitized Core/Shell Fluoride Nanocrystal.

PubMed

Chen, Guanying; Damasco, Jossana; Qiu, Hailong; Shao, Wei; Ohulchanskyy, Tymish Y; Valiev, Rashid R; Wu, Xiang; Han, Gang; Wang, Yan; Yang, Chunhui; Ågren, Hans; Prasad, Paras N

2015-11-11

Lanthanide-doped upconversion nanoparticles hold promises for bioimaging, solar cells, and volumetric displays. However, their emission brightness and excitation wavelength range are limited by the weak and narrowband absorption of lanthanide ions. Here, we introduce a concept of multistep cascade energy transfer, from broadly infrared-harvesting organic dyes to sensitizer ions in the shell of an epitaxially designed core/shell inorganic nanostructure, with a sequential nonradiative energy transfer to upconverting ion pairs in the core. We show that this concept, when implemented in a core-shell architecture with suppressed surface-related luminescence quenching, yields multiphoton (three-, four-, and five-photon) upconversion quantum efficiency as high as 19% (upconversion energy conversion efficiency of 9.3%, upconversion quantum yield of 4.8%), which is about ~100 times higher than typically reported efficiency of upconversion at 800 nm in lanthanide-based nanostructures, along with a broad spectral range (over 150 nm) of infrared excitation and a large absorption cross-section of 1.47 × 10(-14) cm(2) per single nanoparticle. These features enable unprecedented three-photon upconversion (visible by naked eye as blue light) of an incoherent infrared light excitation with a power density comparable to that of solar irradiation at the Earth surface, having implications for broad applications of these organic-inorganic core/shell nanostructures with energy-cascaded upconversion.

Upconversion induced enhancement of dye sensitized solar cells based on core-shell structured β-NaYF4:Er3+, Yb3+@SiO2 nanoparticles

NASA Astrophysics Data System (ADS)

Zhou, Ziyao; Wang, Jiahong; Nan, Fan; Bu, Chenghao; Yu, Zhenhua; Liu, Wei; Guo, Shishang; Hu, Hao; Zhao, Xing-Zhong

2014-01-01

Upconversion materials have been employed as energy relay materials in dye sensitized solar cells (DSCs) to broaden the range of light absorption. However, the origin of the enhancements can be induced by both upconversion and size-dependent light scattering effects. To clarify the role of the upconversion material in the photoelectrode of DSCs, an upconversion induced device was realized here, which has the size-dependent light scattering effect eliminated via the application of NaYF4:Er3+, Yb3+@SiO2 upconversion nanoparticles (β-NYEY@SiO2 UCNPs). An enhancement of 6% in efficiency was observed for the device. This demonstration provided an insight into the possible further employment of upconversion in DSCs.Upconversion materials have been employed as energy relay materials in dye sensitized solar cells (DSCs) to broaden the range of light absorption. However, the origin of the enhancements can be induced by both upconversion and size-dependent light scattering effects. To clarify the role of the upconversion material in the photoelectrode of DSCs, an upconversion induced device was realized here, which has the size-dependent light scattering effect eliminated via the application of NaYF4:Er3+, Yb3+@SiO2 upconversion nanoparticles (β-NYEY@SiO2 UCNPs). An enhancement of 6% in efficiency was observed for the device. This demonstration provided an insight into the possible further employment of upconversion in DSCs. Electronic supplementary information (ESI) available: Details of preparations and characterizations; the TEM images, EDX measurements, XRD measurements and upconversion emission spectrum of bared β-NYEY nanocrystals; SEM and AFM images of the photoelectrode with different concentrations of β-NYEY nanocrystals; J-V characteristics, EIS measurements and fitted EIS parameters of the DSCs based on five different photoelectrodes. See DOI: 10.1039/c3nr04315k

Active media for up-conversion diode-pumped lasers

NASA Astrophysics Data System (ADS)

Tkachuk, Alexandra M.

1996-03-01

In this work, we consider the different methods of populating the initial and final working levels of laser transitions in TR-doped crystals under the selective 'up-conversion' and 'avalanche' diode laser pumping. On the basis of estimates of the probabilities of competing non-radiative energy-transfer processes rates obtained from the experimental data and theoretical calculations, we estimated the efficiency of the up-conversion pumping and selfquenching of the upper TR3+ states excited by laser-diode emission. The effect of the host composition, dopant concentration, and temperature on the output characteristics and up-conversion processes in YLF:Er; BaY2F8:Er; BaY2F8:Er,Yb and BaY2F8:Yb,Ho are determined.

A Paper-Based Sandwich Format Hybridization Assay for Unlabeled Nucleic Acid Detection Using Upconversion Nanoparticles as Energy Donors in Luminescence Resonance Energy Transfer.

PubMed

Zhou, Feng; Noor, M Omair; Krull, Ulrich J

2015-09-24

Bioassays based on cellulose paper substrates are gaining increasing popularity for the development of field portable and low-cost diagnostic applications. Herein, we report a paper-based nucleic acid hybridization assay using immobilized upconversion nanoparticles (UCNPs) as donors in luminescence resonance energy transfer (LRET). UCNPs with intense green emission served as donors with Cy3 dye as the acceptor. The avidin functionalized UCNPs were immobilized on cellulose paper and subsequently bioconjugated to biotinylated oligonucleotide probes. Introduction of unlabeled oligonucleotide targets resulted in a formation of probe-target duplexes. A subsequent hybridization of Cy3 labeled reporter with the remaining single stranded portion of target brought the Cy3 dye in close proximity to the UCNPs to trigger a LRET-sensitized emission from the acceptor dye. The hybridization assays provided a limit of detection (LOD) of 146.0 fmol and exhibited selectivity for one base pair mismatch discrimination. The assay was functional even in undiluted serum samples. This work embodies important progress in developing DNA hybridization assays on paper. Detection of unlabeled targets is achieved using UCNPs as LRET donors, with minimization of background signal from paper substrates owing to the implementation of low energy near-infrared (NIR) excitation.

A novel upconversion@polydopamine core@shell nanoparticle based aptameric biosensor for biosensing and imaging of cytochrome c inside living cells.

PubMed

Ma, Lina; Liu, Fuyao; Lei, Zhen; Wang, Zhenxin

2017-01-15

Herein, a novel upconversion@polydopamine core@shell nanoparticle (termed as UCNP@PDA NP) -based aptameric biosensor has been fabricated for the quantitative analysis of cytochrome c (Cyt c) inside living cells, which comprises an UCNP@PDA NP, acting as an internal reference and fluorescence quenching agent, and Cy3 modified aptamer enabling ratiometric quantitative Cyt c measurement. After the hybridization of Cy3 labeled aptamer with amino-terminated single DNA on the UCNP@PDA NP surface (termed as UCNP@PDA@AP), the fluorescence of Cy3 can be efficiently quenched by the PDA shell. With the spontaneous cellular uptake of UCNP@PDA@AP, the Cyt c aptamer dissociates from UCNP@PDA NP surface through formation of aptamer-Cyt c complex, resulting in concomitant activation of the Cy3 fluorescence. High amount of Cyt c leads to high fluorescence emission, enabling direct visualization/measurement of the Cyt c by fluorescence microscopy/spectroscopy. The steady upconversion luminescent (UCL) signals can be employed not only for intracellular imaging, but also as an internal reference for evaluating intracellular Cyt c amount using the ratio of fluorescence intensity of Cy3 with the UCL intensity of UCNP. The UCNP@PDA@AP shows a reasonable detection limit (20nM) and large dynamic range (50nM to 10μM, which covers the literature reported values (1-10μM) for cytosolic Cyt c in apoptotic cells) for detecting Cyt c in buffer with excellent selectivity. In addition, the UCNP@PDA@AP has been successfully used to monitor etoposide induced intracellular releasing of Cyt c, providing the possibility for cell-based screening of apoptosis-inducing drugs. Copyright © 2016 Elsevier B.V. All rights reserved.

Localized surface plasmons modulated nonlinear optical processes in metal film-coupled and upconversion nanocrystals-coated nanoparticles (Conference Presentation)

NASA Astrophysics Data System (ADS)

Lei, Dangyuan

2016-09-01

In the first part of this talk, I will show our experimental investigation on the linear and nonlinear optical properties of metal film-coupled nanosphere monomers and dimers both with nanometric gaps. We have developed a new methodology - polarization resolved spectral decomposition and color decoding to "visualizing" unambiguously the spectral and radiation properties of the complex plasmonic gap modes in these hybrid nanostructures. Single-particle spectroscopic measurements indicate that these hybrid nanostructures can simultaneously enhance several nonlinear optical processes, such as second harmonic generation, two-photon absorption induced luminescence, and hyper-Raman scattering. In the second part, I will show how the polarization state of the emissions from sub-10 nm upconversion nanocrystals (UCNCs) can be modulated when they form a hybrid complex with a gold nanorod (GNR). Our single-particle scattering experiments expose how an interplay between excitation polarization and GNR orientation gives rise to an extraordinary polarized nature of the upconversion emissions from an individual hybrid nanostructure. We support our results by numerical simulations and, using Förster resonance energy transfer theory, we uncover how an overlap between the UCNC emission and GNR extinction bands as well as the mutual orientation between emission and plasmonic dipoles jointly determine the polarization state of the UC emissions.

Third harmonic from air breakdown plasma induced by nanosecond laser pulses

NASA Astrophysics Data System (ADS)

Stafe, M.; Negutu, C.; Puscas, N. N.

2018-06-01

Harmonic generation is a nonlinear optical effect consisting in frequency up-conversion of intense laser radiation when phase-matching conditions are fulfilled. Here, we study the mechanisms involved in the third harmonic (TH) generation process, the conversion efficiency, and the properties of TH radiation generated in air by focusing infrared linearly polarized nanosecond laser pulses at intensities of the order of TW/cm2. By analyzing the emission from the air breakdown plasma, we demonstrate that filamentary breakdown plasma containing molecular nitrogen ions acts as an optical nonlinear medium enabling generation of TH radiation in the axial direction. The data reveal important properties of the TH radiation: maximum conversion efficiency of 0.04%, sinc2 dependence of the TH intensity on the square root of the pump intensity, and three times smaller divergence and pulse duration of TH as compared to the pump radiation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Makarov, Nikolay S.; Lin, Qianglu; Pietryga, Jeffrey M.

One source of efficiency losses in photovoltaic cells is their transparency toward solar photons with energies below the band gap of the absorbing layer. This loss can be reduced using a process of up-conversion whereby two or more sub-band-gap photons generate a single above-gap exciton. Traditional approaches to up-conversion, such as nonlinear two-photon absorption (2PA) or triplet fusion, suffer from low efficiency at solar light intensities, a narrow absorption bandwidth, nonoptimal absorption energies, and difficulties for implementing in practical devices. We show that these deficiencies can be alleviated using the effect of Auger up-conversion in thick-shell PbSe/CdSe quantum dots. Thismore » process relies on Auger recombination whereby two low-energy, core-based excitons are converted into a single higher-energy, shell-based exciton. When compared to their monocomponent counterparts, the tailored PbSe/CdSe heterostructures feature enhanced absorption cross-sections, a higher efficiency of the “productive” Auger pathway involving re-excitation of a hole, and longer lifetimes of both core- and shell-localized excitons. These features lead to effective up-conversion cross-sections that are more than 6 orders of magnitude higher than for standard nonlinear 2PA, which allows for efficient up-conversion of continuous wave infrared light at intensities as low as a few watts per square centimeter.« less

Defect-mediated photoluminescence up-conversion in cadmium sulfide nanobelts (Conference Presentation)

NASA Astrophysics Data System (ADS)

Morozov, Yurii; Kuno, Masaru K.

2017-02-01

The concept of optical cooling of solids has existed for nearly 90 years ever since Pringsheim proposed a way to cool solids through the annihilation of phonons via phonon-assisted photoluminescence (PL) up-conversion. In this process, energy is removed from the solid by the emission of photons with energies larger than those of incident photons. However, actually realizing optical cooling requires exacting parameters from the condensed phase medium such as near unity external quantum efficiencies as well as existence of a low background absorption. Until recently, laser cooling has only been successfully realized in rare earth doped solids. In semiconductors, optical cooling has very recently been demonstrated in cadmium sulfide (CdS) nanobelts as well as in hybrid lead halide perovskites. For the former, large internal quantum efficiencies, sub-wavelength thicknesses, which decrease light trapping, and low background absorption, all make near unity external quantum yields possible. Net cooling by as much as 40 K has therefore been possible with CdS nanobelts. In this study, we describe a detailed investigation of the nature of efficient anti-Stokes photoluminescence (ASPL) in CdS nanobelts. Temperature-dependent PL up-conversion and optical absorption studies on individual NBs together with frequency-dependent up-converted PL intensity spectroscopies suggest that ASPL in CdS nanobelts is defect-mediated through involvement of defect levels below the band gap.

Blue upconversion with excitation into Tm ions at 780 nm in Yb- and Tm-codoped fluoride crystals

NASA Astrophysics Data System (ADS)

Zhang, X. X.; Hong, P.; Bass, M.; Chai, B. H. T.

1995-04-01

Strong blue emissions have been observed in fluoride crystals, such as LiYF4, BaY2F8, and KYF4, codoped with Tm3+ and Yb3+ when excited into the Tm3+ 3F4 state at ~780 nm. Energy transfer from Tm3+ to Yb3+ ions followed by the transfer from Yb3+ to Tm3+ was demonstrated to be responsible for the upconversion process. A pumping scheme is proposed based on this upconversion mechanism for blue-laser applications using these materials.

Advances in highly doped upconversion nanoparticles.

PubMed

Wen, Shihui; Zhou, Jiajia; Zheng, Kezhi; Bednarkiewicz, Artur; Liu, Xiaogang; Jin, Dayong

2018-06-20

Lanthanide-doped upconversion nanoparticles (UCNPs) are capable of converting near-infra-red excitation into visible and ultraviolet emission. Their unique optical properties have advanced a broad range of applications, such as fluorescent microscopy, deep-tissue bioimaging, nanomedicine, optogenetics, security labelling and volumetric display. However, the constraint of concentration quenching on upconversion luminescence has hampered the nanoscience community to develop bright UCNPs with a large number of dopants. This review surveys recent advances in developing highly doped UCNPs, highlights the strategies that bypass the concentration quenching effect, and discusses new optical properties as well as emerging applications enabled by these nanoparticles.

Growth and optical properties of Pr,Yb-codoped KY 3F 10 fluoride single crystals for up-conversion visible luminescence

NASA Astrophysics Data System (ADS)

Kim, Kyoung Jin; Jouini, Anis; Yoshikawa, Akira; Simura, Rayko; Boulon, Georges; Fukuda, Tsuguo

2007-02-01

We investigate different ways to realize laser emission from (Pr 3+) 3P J=0,1,2 levels by pump sources other than the common argon and excimer-dye laser. The use of infrared (IR) laser diodes in combination with intra- and inter-ionic energy transfer processes (up-conversion) could be an efficient solution towards laser oscillation. Pr 3+,Yb 3+-codoped KY 3F 10 (Pr, Yb:KYF) single crystals were successfully grown by the micro-pulling-down (μ-PD) method. The crystals were transparent with a slightly greenish color, 2.0-2.5 mm in diameter, 20-30 mm in length and free from visible inclusions and cracks. Effective segregation coefficients of Pr and Yb in KYF were studied by means of absorption and chemical analysis. Strong visible emission via selective IR pumping with λ=975 nm and up-conversion excitation were obtained in Pr, Yb:KYF at room temperature (RT). Luminescence measurements have been carried out and the decay kinetics of the Pr 3+ visible emissions was investigated by room temperature time-resolved spectra.

Highly efficient saturated visible up-conversion photoluminescent Y 2 O 3 :Er 3+ microspheres pumped with a 1.55 μm laser diode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Jinbo; Wu, Lili; Zhang, Chuanjiang

2017-01-01

Highly efficient saturation up-conversion (UC) luminescent Y2O3:Er3+ microspheres have been successfully prepared via a hydrothermal-homogeneous precipitation method. Bright visible luminescence can be clearly seen with a 1.55 mu m laser diode excitation power as low as similar to 0.03 W cm(-2). The up-conversion (UC) emission spectra indicate that the strongest red emission with a peak situated at similar to 660 nm originated from the I-4(9/2) -> I-4(15/2) transition of Er3+. The peaks situated at similar to 520 and 550 nm can be assigned to the transition from H-2(11/2)/S-4(3/2) state to the ground state of Er3+. The high efficient saturation up-conversionmore » emission is related to the highly crystalline structure. These results indicate a new way to enhance UC radiation in rare-earth ion-doped materials prepared using a hydrothermal-homogeneous precipitation method.« less

Plasmon-Induced Selective Enhancement of Green Emission in Lanthanide-Doped Nanoparticles.

PubMed

Zhang, Weina; Li, Juan; Lei, Hongxiang; Li, Baojun

2017-12-13

By introducing an 18 nm thick Au nanofilm, selective enhancement of green emission from lanthanide-doped (β-NaYF 4 :Yb 3+ /Er 3+ ) upconversion nanoparticles (UCNPs) is demonstrated. The Au nanofilm is deposited on a microfiber surface by the sputtering method and then covered with the UCNPs. The plasma on the surface of the Au nanofilm can be excited by launching a 980 nm wavelength laser beam into the microfiber, resulting in an enhancement of the local electric field and a strong thermal effect. A 36-fold luminescence intensity enhancement of the UCNPs at 523 nm is observed, with no obvious reduction in the photostability of the UCNPs. Further, the intensity ratios of the emissions at 523-545 nm and at 523-655 nm are enhanced with increasing pump power, which is attributed to the increasing plasmon-induced thermal effect. Therefore, the fabricated device is further demonstrated to exhibit an excellent ability in temperature sensing. By controlling the pump power and the UCNP concentration, a wide temperature range (325-811 K) and a high temperature resolution (0.035-0.046 K) are achieved in the fabricated device.

Photodegradation of near-infrared-pumped Tm(3+)-doped ZBLAN fiber upconversion lasers.

PubMed

Booth, I J; Archambault, J L; Ventrudo, B F

1996-03-01

Photodegradation has been observed in Tm(3+)-doped ZBLAN fiber lasers pumped with laser diodes at 1135 nm. After upconversion lasing at 482 nm, the fiber develops color centers that absorb strongly at wavelengths below ~650 nm, affecting further upconversion lasing. The rate of damage formation is strongly dependent on the pump power level and on the thulium concentration. The color centers are bleached by intense blue light but recover with thermal excitation and can be removed by thermal annealing at temperature near 100 degrees C.

Yb3+-Er3+-Tm3+ co-doped nano-glass-ceramics tuneable up-conversion phosphor

NASA Astrophysics Data System (ADS)

Méndez-Ramos, J.; Rodriguez, V. D.; Tikhomirov, V. K.; Del-Castillo, J.; Yanes, A. C.

2008-08-01

Transparent Yb3+-Er3+-Tm3+ co-doped nano-glass-ceramics have been prepared, 32(SiO{2}) 9(AlO{1.5}) 31.5(CdF{2}) 18.5(PbF{2}) 5.5(ZnF{2}): 3.5(Yb-Er-TmF{3}) mol%, where the co-dopants partition mostly to the fluoride PbF{2}-based nano-crystals. A comparative study of the up-conversion luminescence in nano-glass-ceramics and its precursor glass indicates that these materials can be used as blue/green/red tuneable up-conversion phosphor, in particular for white light generation. A ratio between blue, green and red emission bands of the Tm3+ and Er3+ can be widely varied with nano-ceramming of the precursor glass and with changing a pump power of luminescence. The change in the ratio between the blue, green and red emission bands is explained to be due to substantial lowering phonon energy and shortening of inter-dopant distances with nano-ceramming of the precursor glass and due to change in the ratio of 2- and 3-photon up-conversion processes with pump power.

Energy transfer upconversion in Er3+-Tm3+ codoped sodium silicate glass

NASA Astrophysics Data System (ADS)

Kumar, Vinod; Pandey, Anurag; Ntwaeaborwa, O. M.; Swart, H. C.

2018-04-01

Er3+/Tm3+ doped and codoped Na2O-SiO2-ZnO (NSZO) glasses were prepared by the conventional melt-quenching method. The amorphous nature of the prepared glasses was confirmed by the X-ray diffraction analysis. The optical absorption spectrum displayed several peaks, which correspond to Er3+ and Tm3+ dopant ions embedded into the NSZO glass. Both dopants experienced upconversion emission under 980 nm excitation. Efficient energy transfer from Er3+ to Tm3+ was observed in the co-doped samples to enhance the near infrared emission of the Tm3+ ions.

New anthracene derivatives as triplet acceptors for efficient green-to-blue low-power upconversion.

PubMed

Liang, Zuo-Qin; Sun, Bin; Ye, Chang-Qing; Wang, Xiao-Mei; Tao, Xu-Tang; Wang, Qin-Hua; Ding, Ping; Wang, Bao; Wang, Jing-Jing

2013-10-21

Three new anthracene derivatives [2-chloro-9,10-dip-tolylanthracene (DTACl), 9,10-dip-tolylanthracene-2-carbonitrile (DTACN), and 9,10-di(naphthalen-1-yl)anthracene-2-carbonitrile (DNACN)] were synthesized as triplet acceptors for low-power upconversion. Their linear absorption, single-photon-excited fluorescence, and upconversion fluorescence properties were studied. The acceptors exhibit high fluorescence yields in DMF. Selective excitation of the sensitizer Pd(II)octaethylporphyrin (PdOEP) in solution containing DTACl, DTACN, or DNA-CN at 532 nm with an ultralow excitation power density of 0.5 W cm(-2) results in anti-Stokes blue emission. The maximum upconversion quantum yield (Φ(UC) =17.4%) was obtained for the couple PdOEP/DTACl. In addition, the efficiency of the triplet-triplet energy transfer process was quantitatively studied by quenching experiments. Experimental results revealed that a highly effective acceptor for upconversion should combine high fluorescence quantum yields with efficient quenching of the sensitizer triplet. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Polarization-dependent extraordinary optical transmission from upconversion nanoparticles.

PubMed

Wang, Peng Hui; Salcedo, Walter J; Pichaandi, Jothirmayanantham; van Veggel, Frank C J M; Brolo, Alexandre G

2015-11-21

Enhanced upconversion (UC) emission was experimentally demonstrated using gold double antenna nanoparticles coupled to nanoslits in gold films. The transmitted red emission from UC ytterbium and erbium co-doped sodium yttrium fluoride (NaYF4:Yb(3+)/Er(3+)) nanoparticles (UC NPs) at ∼665 nm (excited with a 980 nm diode laser) was enhanced relative to the green emission at ∼550 nm. The relatively enhanced UC NP emission could be tuned by the different polarization-dependent extraordinary optical transmission modes coupled to the gold nanostructures. Finite-difference time-domain calculations suggest that the preferential enhanced UC emission is related to a combination of different surface plasmon mode excitation coupling to cavity Fabry-Perot interactions. A maximum UC enhancement of 6-fold was measured for nanoslit arrays in the absence of the double antennas. In the presence of the double nanoantennas inside the nanoslits, the UC enhancement was between 2- and 4-fold, depending on the experimental conditions.

Explanation of the cw operation of the Er3+ 3-μm crystal laser

NASA Astrophysics Data System (ADS)

Pollnau, M.; Graf, Th.; Balmer, J. E.; Lüthy, W.; Weber, H. P.

1994-05-01

A computer simulation of the Er3+ 3-μm crystal laser considering the full rate-equation scheme up to the 4F7/2 level has been performed. The influence of the important system parameters on lasing and the interaction of these parameters has been clarified with multiple-parameter variations. Stimulated emission is fed mainly by up-conversion from the lower laser level and in many cases is reduced by the quenching of the lifetime of this level. However, also without up-conversion a set of parameters can be found that allows lasing. Up-conversion from the upper laser level is detrimental to stimulated emission but may be compensated by cross relaxation from the 4S3/2 level. For a typical experimental situation we started with the parameters of Er3+:LiYF4. In addition, the host materials Y3Al5O12 (YAG), YAlO3, Y3Sc2Al3O12 (YSGG), and BaY2F8, as well as the possibilities of codoping, are discussed. In view of the consideration of all excited levels up to 4F7/2, all lifetimes and branching ratios, ground-state depletion, excited-state absorption, three up-conversion processes as well as their inverse processes, stimulated emission, and a realistic resonator design, this is, to our knowledge, the most detailed investigation of the Er3+ 3-μm crystal laser performed so far.

Impact of firing temperature on multi-wavelength selective Stokes and anti-Stokes luminescent behavior by Gd2O2S:Er,Yb phosphor and its application in solar energy harvesting

NASA Astrophysics Data System (ADS)

Kataria, V.; Mehta, D. S.

2018-04-01

Erbium (Er3+)-ytterbium (Yb3+) doped gadolinium oxysulphide (Gd2O2S) phosphor has been developed via a facile method of solid-state flux fusion, and offers two-fold spectrum modification with highly intense Stokes and anti-Stokes shift. The effect of the firing cycle on the photoluminescent response and morphology of Gd2O2S:Er,Yb is scrutinized, wherein the firing temperature was varied (1000 °C-1250 °C), keeping firing time and all other parameters constant. Interestingly, the nanostructures fired below 1150 °C showed nanorods of diameter ~200 nm and length ~1-2 µm, whereas firing at 1150 °C and above rendered nanospheres with small diameter, ~350 nm. Highly bright upconversion (UC) emission was achieved even under an extremely low excitation power density of 800 µW cm-2 from a 980 nm laser, and was comfortably visible to the naked eye. The incident power dependent studies disclosed increase in UC-emission intensity with increasing excitation power and a quasi-linear dependence on excitation power density. Intense characteristic UC-emission of Er3+ excited states at 525 nm, 556 nm and 668 nm were observed, and the green emission band was found to be dominant over the red band in intensity. Concurrently, downconversion (DC) emission at 556 nm and 669 nm was also exhibited under ultraviolet excitation (285 nm and 380 nm), with the red band being more powerful than the green, unlike UC-emission. Firing temperature dependent studies divulged the dependence of luminescence intensity on the firing cycle of the luminophore and formation of the respective luminescent phase. The UC-emission intensity was found to be maximum for samples fired at 1150 °C, whereas samples fired at 1000 °C showed the highest DC-emission intensity. The excitation and emission profile of single Gd2O2S:Er,Yb phosphor lying in the desired spectral region and as a dual spectral converter marks its possible application for enhanced harvesting of sunlight.

Intense 2.7 μm mid-infrared emission of Er{sup 3+} in oxyfluoride glass ceramic containing NaYF{sub 4} nanocrystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Yin; Liu, Xueyun; Wang, Weichao

2016-04-15

Highlights: • Transparent oxyfluoride glass-ceramics containing NaYF{sub 4}:Er{sup 3+} nanocrystals have been prepared. • Intense 2.7 μm emission of the glass-ceramics has been demonstrated. • Prolonged decay lifetimes of Er{sup 3+}:{sup 4}I{sub 11/2} and {sup 4}I{sub 13/2} levels have been achieved. - Abstract: Transparent oxyfluoride glass ceramics containing NaYF{sub 4}:Er{sup 3+} nanocrystals have been prepared by melt quenching and subsequent thermal treatment. X-ray diffraction and high-resolution transmission electron microscopy analysis confirmed the precipitation of NaYF{sub 4} nanocrystals in glass. Energy dispersive spectrometer results evidenced the preferential concentration of Er{sup 3+} ions in nanocrystals. Mid-infrared, upconversion, and near-infrared emissions were measuredmore » upon excitation with 980 nm laser diode and the luminescence mechanisms were discussed. Intense 2.7 μm emission originating from the Er{sup 3+}:{sup 4}I{sub 11/2} → {sup 4}I{sub 13/2} transition was achieved due to the incorporation of Er{sup 3+} ions into the precipitated low phonon energy fluoride nanocrystals. The results indicate that oxyfluoride glass ceramic containing NaYF{sub 4}:Er{sup 3+} nanocrystals is a promising candidate material for 2.7 μm laser.« less

Solid state photon upconversion utilizing thermally activated delayed fluorescence molecules as triplet sensitizer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Tony C.; Congreve, Daniel N.; Baldo, Marc A., E-mail: baldo@mit.edu

2015-07-20

The ability to upconvert light is useful for a range of applications, from biological imaging to solar cells. But modern technologies have struggled to upconvert incoherent incident light at low intensities. Here, we report solid state photon upconversion employing triplet-triplet exciton annihilation in an organic semiconductor, sensitized by a thermally activated-delayed fluorescence (TADF) dye. Compared to conventional phosphorescent sensitizers, the TADF dye maximizes the wavelength shift in upconversion due to its small singlet-triplet splitting. The efficiency of energy transfer from the TADF dye is 9.1%, and the conversion yield of sensitizer exciton pairs to singlet excitons in the annihilator ismore » 1.1%. Our results demonstrate upconversion in solid state geometries and with non-heavy metal-based sensitizer materials.« less

Color-coded multilayer photopatterned microstructures using lanthanide (III) ion co-doped NaYF4 nanoparticles with upconversion luminescence for possible applications in security.

PubMed

Kim, Won Jin; Nyk, Marcin; Prasad, Paras N

2009-05-06

We report a method for fabricating predefined photopatterns of upconversion nanophosphors using a chemical amplification reaction for direct writing of films with multilayer color-coded patterning for security applications. To photopattern the nanocrystal film we have synthesized rare-earth ion (Er(3+)/Yb(3+) or Tm(3+)/Yb(3+)) co-doped sodium yttrium fluoride (alpha-NaYF(4)) nanophosphors and functionalized the nanocrystal surfaces by incorporation of a photopatternable ligand such as t-butoxycarbonyl (t-BOC). The surface modification allows photopatterning of the nanophosphor solid state film. Furthermore, upconversion nanophosphors show a nearly quadratic dependence of the upconversion photoluminescence (PL) intensity on the excitation light power, and tailoring of the PL wavelength is possible by changing the lanthanide ions. We have demonstrated the capability of anchoring nanophosphors at desirable locations by a photolithography technique. The photopatterned films exhibit fixed nanophosphor structures clearly identifiable by strong upconversion photoluminescence under IR illumination which is useful for a number of applications in security.

Upconversion luminescence of Er3+/Yb3+ doped Sr5(PO4)3OH phosphor powders

NASA Astrophysics Data System (ADS)

Mokoena, P. P.; Swart, H. C.; Ntwaeaborwa, O. M.

2018-04-01

Sr5(PO4)3OH co-doped with Er3+and Yb3+ powder phosphors were synthesized by urea combustion method. The crystal structure was analyzed using X-ray diffraction (XRD). Particle morphology was analyzed using a Jeol JSM 7800F thermal field emission scanning electron microscope (FE-SEM) and the chemical composition analysis was carried out using an Oxford Instruments AzTEC energy dispersive spectrometer (EDS) attached to the FE-SEM. Upconversion emission was measured by using a FLS980 Spectrometer equipped with a 980 nm NIR laser as the excitation source, and a photomultiplier (PMT) detector. The XRD data of the Sr5(PO4)3OH powder exhibited characteristic diffraction patterns of the hexagonal structure referenced in the standard JCPDS card number 00-033-1348. The sharp peaks revealed the formation of crystalline Sr5(PO4)3OH. The powders were made up of hexagonal nanospheres. The enhanced red emission due to the 4F9/2 → 4I15/2 transitions of Er3+ was observed and was attributed to up conversion (UC) energy transfer from Yb3+. The upconversion energy transfer mechanism from Yb3+ to Er3+ is discussed.

Clean synthesis of YOF:Er3+, Yb3+ upconversion colloidal nanoparticles in water through liquid phase pulsed laser ablation for imaging applications

NASA Astrophysics Data System (ADS)

Anjana, R.; Kurias, K. M.; Jayaraj, M. K.

2017-10-01

Upconversion luminescent nanomaterials have great outlook towards imaging applications. These materials have high chemical and thermal stability, low auto fluorescence, high photo stability and IR excitation does not cause photo damage to living cells and penetrate deeply into tissue. Most of the reported nanoparticles are synthesized through chemical methods in which surface modification is needed for dispersing nanoparticles in water. In this paper we report clean and simple synthesis of upconversion luminescent yttrium oxyfluoride (YOF) nanoparticles through laser ablation in deionized water. YOF:Er3+, Yb3+ pellets were used for ablation. Er3+ is the emission centre Yb3+ is the sensitizer. Obtained colloidal solution is transparent to day light and showing red emission on exciting with 980 nm IR laser. By controlling ablation parameters particles of size less than 10 nm dispersed uniformly in water can be obtained through this surfactant free method. The synthesized nanoparticles can be used for cell imaging.

Up-conversion monodispersed spheres of NaYF4:Yb3+/Er3+: green and red emission tailoring mediated by heating temperature, and greatly enhanced luminescence by Mn2+ doping.

PubMed

Zhu, Qi; Song, Caiyun; Li, Xiaodong; Sun, Xudong; Li, Ji-Guang

2018-04-09

Submicron sized, monodispersed spheres of Mn2+, Yb3+/Er3+ and Mn2+/Yb3+/Er3+ doped α-NaYF4 were easily autoclaved from mixed solutions of the component nitrates and ammonium fluoride (NH4F), in the presence of EDTA-2Na. Detailed characterizations of the resultant phosphors were obtained using XRD, Raman spectroscopy, FE-SEM, HR-TEM, STEM, PLE/PL spectroscopy, and fluorescence decay analysis. Finer structure and better crystal perfection was observed at a higher calcination temperature, and the spherical shape and excellent dispersion of the original particles was retained at temperatures up to 600 °C. Under the 980 nm infrared excitation, the Yb3+/Er3+-doped sample (calcined at 400 °C) exhibits a stronger green emission centered at ∼524 nm (2H11/2 → 4I15/2 transition of Er3+) and a weaker red emission centered at ∼657 nm (4F9/2 → 4I15/2 transition of Er3+). A 200 °C increase in the temperature from 400 °C to 600 °C resulted in the dominant red emission originating from the 4F9/2 → 4I15/2 transition of Er3+, instead of the previously dominant green one. Mn2+ doping induced a remarkable more enhanced intensity at ∼657 nm and ∼667 nm (red emission area) than that at ∼524 nm and ∼546 nm (green emission area), because of the non-radiative energy transfer between Mn2+ and Er3+. However, a poor thermal stability was induced by Mn2+ doping. The observed upconversion luminescence of the samples calcined at 400 °C and 600 °C followed the two photon process and the four photon process, respectively.

Controllable red, green, blue (RGB) and bright white upconversion luminescence of Lu2O3:Yb3+/Er3+/Tm3+ nanocrystals through single laser excitation at 980 nm.

PubMed

Yang, Jun; Zhang, Cuimiao; Peng, Chong; Li, Chunxia; Wang, Lili; Chai, Ruitao; Lin, Jun

2009-01-01

Light fantastic! Lu(2)O(3):Yb(3+)/Er(3+)/Tm(3+) nanocrystals with controllable red, green, blue (RGB) and bright white upconversion luminescence by a single laser excitation of 980 nm have been successfully synthesized (see picture). Due to abundant UC PL colors, it can potentially be used as fluorophores in the field of color displays, back light, UC lasers, photonics, and biomedicine.Lu(2)O(3):Yb(3+)/Er(3+)/Tm(3+) nanocrystals have been successfully synthesized by a solvothermal process followed by a subsequent heat treatment at 800 degrees C. Powder X-ray diffraction, transmission electron microscopy, upconversion photoluminescence spectra, and kinetic decay were used to characterize the samples. Under single-wavelength diode laser excitation of 980 nm, the bright blue emissions of Lu(2)O(3):Yb(3+), Tm(3+) nanocrystals near 477 and 490 nm were observed due to the (1)G(4)-->(3)H(6) transition of Tm(3+). The bright green UC emissions of Lu(2)O(3):Er(3+) nanocrystals appeared near 540 and 565 nm were observed and assigned to the (2)H(11/2)-->(4)I(15/2) and (4)S(3/2)-->(4)I(15/2) transitions, respectively, of Er(3+). The ratio of the intensity of green luminescence to that of red luminescence decreases with an increase of concentration of Yb(3+) in Lu(2)O(3):Er(3+) nanocrystals. In sufficient quantities of Yb(3+) with resprct to Er(3+), the bright red UC emission of Lu(2)O(3):Yb(3+)/Er(3+) centered at 662 nm was predominant, due to the (4)F(9/2)-->(4)I(15/2) transition of Er(3+). Based on the generation of red, green, and blue emissions in the different doped Lu(2)O(3):RE(3+) nanocrystals, it is possible to produce the luminescence with a wide spectrum of colors, including white, by the appropriate doping of Yb(3+), Tm(3+), and Er(3+) in the present Lu(2)O(3) nanocrystals. Namely, Lu(2)O(3):3 %Yb(3+)/0.2 %Tm(3+)/0.4 %Er(3+) nanocrystals show suitable intensities of blue, green, and red (RGB) emission, resulting in the production of perfect and bright white light with CIE-x=0.3456 and CIE-y=0.3179, which is very close to the standard equal energy white light illuminate (x=0.33, y=0.33). Because of abundant luminescent colors from RGB to white in Lu(2)O(3):Yb(3+)/Er(3+)/Tm(3+) nanocrystals under 980 nm laser diode (LD) excitation, they can potentially be used as fluorophores in the field of color displays, back light, UC lasers, photonics, and biomedicine.

NaLa(MoO{sub 4}){sub 2}: RE{sup 3+} (RE{sup 3+} = Eu{sup 3+}, Sm{sup 3+}, Er{sup 3+}/Yb{sup 3+}) microspheres: the synthesis and optical properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Zhiyi; Wang, Zhiying; Fu, Linlin

The strong green upconversion (UC) emission were observed in various Er{sup 3+}, Yb{sup 3+} co-doped NaLa(MoO{sub 4}){sub 2} samples synthesized via a hydrothermal route. The UC intensity depends on the dopant concentration, and the optimal UC emission was obtained in NaLa(MoO{sub 4}){sub 2}: 0.02Er{sup 3+}/0.10 Yb{sup 3+}. - Highlights: • The NaLa(MoO{sub 4}){sub 2} microspheres doped with Eu{sup 3+}, Sm{sup 3+} and Er{sup 3+}/Yb{sup 3+} were synthesized by a hydrothermal method. • The effects of the EDTA in the initial solution crystal phase and morphology were studied. • The down-conversion luminescence properties of NaLa(MoO{sub 4}){sub 2}: RE{sup 3+} (RE{sup 3+}more » = Eu{sup 3+}, Sm{sup 3+}) were investigated. • The UC luminescence properties and mechanism of Er{sup 3+}/Yb{sup 3+} co-doped NaLa(MoO{sub 4}){sub 2} was discussed. - Abstract: NaLa(MoO{sub 4}){sub 2}: RE{sup 3+} (RE{sup 3+} = Eu{sup 3+}, Sm{sup 3+}) microspheres have been synthesized at 180 °C via a facile EDTA-mediated hydrothermal route. X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), photoluminescence (PL) spectra were employed to characterize the samples. It was found that the amount of EDTA in the initial solution was responsible for crystal phase and shape determination. The effect of Eu{sup 3+} and Sm{sup 3+} doping concentrations on the luminescent intensity was also investigated in details. Furthermore, the up-conversion (UC) emissions have been observed in a series of Er{sup 3+}/Yb{sup 3+} co-doped NaLa(MoO{sub 4}){sub 2} samples. Concentration dependent studies revealed that the optimal composition was realized for a 2% Er{sup 3+} and 10% Yb{sup 3+}-doping concentration.« less

Multimodal emissions from Tb{sup 3+}/Yb{sup 3+} co-doped lithium borate glass: Upconversion, downshifting and quantum cutting

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bahadur, A.; Yadav, R.S.; Yadav, R.V.

This paper reports the optical properties of Tb{sup 3+}/Yb{sup 3+} co-doped lithium borate (LB) glass prepared by melt quench method. The absorption spectrum of the Yb{sup 3+} doped LB glass contains intense NIR band centered at 976 nm due to {sup 2}F{sub 7/2}→{sup 2}F{sub 5/2} transition. The emission spectra of the prepared glasses have been monitored on excitation with 266, 355 and 976 nm. The Yb{sup 3+} doped glass emits a broad NIR band centered at 976 nm whereas the Tb{sup 3+} doped glass gives off visible bands on excitations with 266 and 355 nm. When the Tb{sup 3+} andmore » Yb{sup 3+} ions are co-doped together, the emission intensity in the visible region decreases whereas it increases in the NIR region significantly. The increase in the emission intensity in the NIR region is due to efficient cooperative energy transfer (CET) from Tb{sup 3+} to Yb{sup 3+} ions. The quantum cutting efficiency for Tb{sup 3+}/Yb{sup 3+} co-doped glass has been calculated and compared for 266 and 355 nm excitations. The quantum cutting efficiency is larger for 355 nm excitation (137%). The Tb{sup 3+}/Yb{sup 3+} co-doped LB glass also emits upconverted visible bands on excitation with 976 nm. The mechanisms involved in the energy transfer have been discussed using schematic energy level diagram. The Tb{sup 3+}/Yb{sup 3+} co-doped LB glass may be used in the optical devices and in solar cell for solar spectral conversion and behaves as a multi-modal photo-luminescent material. - Graphical abstract: The Tb{sup 3+}/Yb{sup 3+} co-doped lithium borate (LB) glass prepared by melt quench method emits upconverted visible emissions through upconversion CET from Yb{sup 3+} to Tb{sup 3+} ions and quantum cutting emissions through downconversion CET from Tb{sup 3+} to Yb{sup 3+} ions. Therefore, the Tb{sup 3+}/Yb{sup 3+} co-doped LB glass may find applications in optical devices and solar cell and behaves as a multi-modal photo-luminescent material. - Highlights: • The Tb{sup 3+}/Yb{sup 3+} co-doped lithium borate (LB) glass prepared by melt quench method. • The Tb{sup 3+}/Yb{sup 3+} co-doped glass gives QC emissions upon 266 and 355 nm excitations. • The Tb{sup 3+}/Yb{sup 3+} co-doped glass also emits intense green color on excitation with 976 nm. • The quantum cutting efficiency is larger for 355 nm excitation (137%). • The Tb{sup 3+}/Yb{sup 3+} co-doped glass may be used in solar cell and display devices.« less

Er(3+)/Yb(3+) upconverters for InGaP solar cells under concentrated broadband illumination.

PubMed

Feenstra, J; Six, I F; Asselbergs, M A H; van Leest, R H; de Wild, J; Meijerink, A; Schropp, R E I; Rowan, A E; Schermer, J J

2015-05-07

The inability of solar cell materials to convert all incident photon energy into electrical current, provides a fundamental limit to the solar cell efficiency; the so called Shockley-Queisser (SQ) limit. A process termed upconversion provides a pathway to convert otherwise unabsorbed low energy photons passing through the solar cell into higher energy photons, which subsequently can be redirected back to the solar cell. The combination of a semi-transparent InGaP solar cell with lanthanide upconverters, consisting of ytterbium and erbium ions doped in three different host materials (Gd2O2S, Y2O3 and NaYF4) is investigated. Using sub-band gap light of wavelength range 890 nm to 1045 nm with a total accumulated power density of 2.7 kW m(-2), a distinct photocurrent was measured in the solar cell when the upconverters were applied whereas a zero current was measured without upconverter. Furthermore, a time delay between excitation and emission was observed for all upconverter systems which can be explained by energy transfer upconversion. Also, a quadratic dependence on the illumination intensity was observed for the NaYF4 and Y2O3 host material upconverters. The Gd2O2S host material upconverter deviated from the quadratic illumination intensity dependence towards linear behaviour, which can be attributed to saturation effects occurring at higher illumination power densities.

Cysteine optical sensing with an up-conversion host and two chemosensors derived from rhodamine: Construction, characterization and performance

NASA Astrophysics Data System (ADS)

Lin, Chen; Zhigang, Fang

2017-03-01

This paper focused on two rhodamine chemosensors for cysteine optical sensing. To minimize their photobleaching caused by excitation light, up-conversion NaYF4:Yb3 +/Er3 + nanocrystals were prepared and used as excitation host. Photophysical measurement on this host and the two chemosensors suggested that chemosensor absorption matched well with host emission. An efficient energy transfer between them was discussed and confirmed by their spectral analysis and emission lifetime comparison. Job's plot suggested that our chemosensors followed a simple recognition mechanism towards cysteine with binding stoichiometry of 1:1. Both chemosensors showed emission "off-on" effect triggered by cysteine and good photostability. Linear working curves with maximum sensitivity of 2.61 were obtained. S substituent was positive to improve selectivity.

Hydrothermal synthesis infrared to visible upconversion luminescence of SrMoO4: Er3+/Yb3+ phosphor

NASA Astrophysics Data System (ADS)

Sinha, Shriya; Kumar, Kaushal

2018-04-01

The upconversion emission properties in Er3+/Yb3+ doped SrMoO4 phosphor synthesized via hydrothermal method is investigated upon 980 nm laser light excitation. The crystal structure and morphology of the synthesized phosphor are characterized by X-ray diffraction and field emission scanning electron microscopy. The X-ray diffraction pattern suggests that SrMoO4 phosphor has tetragonal phase structure. The phosphor emits strong green (525 and 552 nm) and red (665 nm) UC emissions along with weak blue (410 and 488 nm) and near infrared (798 nm) emission bands. The color emitted from the phosphor is shifted from yellow to green region with increasing the power density from 15 to 65 W/cm2. The result indicates that the present material is suitable for making infrared to visible up-converts and display devices.

All-inorganic colloidal upconversion quantum dots (Conference Presentation)

NASA Astrophysics Data System (ADS)

Oron, Dan; Teitelboim, Ayelet

2017-02-01

Upconversion (UC) is a nonlinear process in which two, or more, long wavelength photons are converted to a shorter wavelength photon. This process is based on sequential absorption of two or more photons, involving metastable, long lived intermediate energy states, thus is not restricted to ultrashort pulsed excitation. Hence, requirements for UC processes are long lived excited states, a ladder like arrangement of energy levels and a mechanism inhibiting cooling of the hot charge carrier. UC holds great promise for bioimaging, enabling to perform multiphoton imaging in scattering specimen at very low powers. Rare-earth-doped nanocrystals, the most commonly used ones for UC, typically require a minimal particle diameter of several tens of nanometers and have a limited action spectrum. Here, we present a novel luminescence upconversion nano-system based on colloidal semiconductor double quantum dots, consisting of a NIR-absorbing component and a visible emitting component separated by a tunneling barrier in a spherical onion-like geometry. These dual near-infrared and visible core/shell/shell PbSe/CdSe/CdS nanocrystals are shown to efficiently upconvert a broad range of NIR wavelengths up to 1.2 microns to visible emission at room temperature, covering a spectral range where there are practically no alternative upconversion systems. The particle diameter is less than ten nanometers, and the synthesis enables versatility and tunability of both the visible emission color and the NIR absorption edge. The physical mechanism for upconversion in this type of structures, as well as potential advances and extensions on this system will be discussed.

Up-conversion of MMW radiation to visual band using glow discharge detector and silicon detector

NASA Astrophysics Data System (ADS)

Aharon Akram, Avihai; Rozban, Daniel; Abramovich, Amir; Yitzhaky, Yitzhak; Kopeika, Natan S.

2016-10-01

In this work we describe and demonstrate a method for up-conversion of millimeter wave (MMW) radiation to the visual band using a very inexpensive miniature Glow Discharge Detector (GDD), and a silicon detector (photodetector). Here we present 100 GHz up-conversion images based on measuring the visual light emitting from the GDD rather than its electrical current. The results showed better response time of 480 ns and better sensitivity compared to the electronic detection that was performed in our previous work. In this work we performed MMW imaging based on this method using a GDD lamp, and a photodetector to measure GDD light emission.

Nd3+, Yb3+ and Ho3+ Codoped Oxyfluoride Glass Ceramics with High Efficient Green Upconversion Luminescence

NASA Astrophysics Data System (ADS)

Zhang, Jun-Jie; Kawamoto, Yoji; Dai, Shi-Xun; Zhang, Li-Yan; Hu, Li-Li

2004-06-01

New oxyfluoride glasses and glass ceramic codoped with Nd3+, Yb3+ and Ho3+ were prepared. The x-ray diffraction analysis revealed that the heat treatments of the oxyfluoride glasses could cause the precipitation of (Nd3+, Yb3+, Ho3+)-doped fluorite-type crystals. Very strong green up-conversion luminescence due to the Ho3+: (5F4, 5S2)rightarrow5I8 transition under 800-nm excitation was observed in these transparent glass ceramics. The intensity of the green up-conversion luminescence in a 1-mol% YbF3-containing glass ceramic was found to be about 120 times stronger than that in the precursor oxyfluoride glass. The reason for the highly efficient Ho3+ up-conversion luminescence in the oxyfluoride glass ceramics is discussed.

Latent fingermark detection for NaYF4:Er3+/Yb3+ upconversion phosphor synthesized by thermal decomposition route

NASA Astrophysics Data System (ADS)

Maurya, S. K.; Tiwari, S. P.; Kumar, A.; Kumar, K.

2018-04-01

The synthesis and spectroscopy of the upconverting nanoparticles, cubic NaYF4:Er3+/Yb3+ phosphor is developed for latent fingermark detection. The cubic phase of NaYF4: Er3+/Yb3+ phosphor is synthesized by thermal decomposition method using trifluoroacetate precursor with coordinating ligand octadecene and oleic acid in a mixture of technical grade. The synthesized samples showed intense green emission using 976 nm diode laser as an excitation source. Because of excellent property of luminescence in green regime the sample is used to detect the latent fingermark on a porous glass surface.

Ultimate waveform reproducibility of extreme-ultraviolet pulses by high-harmonic generation in quartz

NASA Astrophysics Data System (ADS)

Garg, M.; Kim, H. Y.; Goulielmakis, E.

2018-05-01

Optical waveforms of light reproducible with subcycle precision underlie applications of lasers in ultrafast spectroscopies, quantum control of matter and light-based signal processing. Nonlinear upconversion of optical pulses via high-harmonic generation in gas media extends these capabilities to the extreme ultraviolet (EUV). However, the waveform reproducibility of the generated EUV pulses in gases is inherently sensitive to intensity and phase fluctuations of the driving field. We used photoelectron interferometry to study the effects of intensity and carrier-envelope phase of an intense single-cycle optical pulse on the field waveform of EUV pulses generated in quartz nanofilms, and contrasted the results with those obtained in gas argon. The EUV waveforms generated in quartz were found to be virtually immune to the intensity and phase of the driving field, implying a non-recollisional character of the underlying emission mechanism. Waveform-sensitive photonic applications and precision measurements of fundamental processes in optics will benefit from these findings.

Optical properties of Er 3+/Yb 3+-codoped transparent PLZT ceramic

NASA Astrophysics Data System (ADS)

Zheng, Zhiqiang; Li, Xiaoyan; Liu, Jing; Feng, Zhuohong; Li, Baozeng; Yang, Jiwen; Li, Kewen; Jiang, Hua; Chen, Xuesheng; Xie, Jianping; Ming, Hai

2008-01-01

Optical absorption and emission spectra of Er 3+/Yb 3+ ions in PLZT (Pb 1-xLa xZr yTi 1-yO 3) ceramic have been studied. Based on the Judd-Ofelt (J-O) theory, the J-O intensity parameters were calculated to be Ω2=2.021×10 -20 cm 2, Ω4=0.423×10 -20 cm 2, Ω6=0.051×10 -20 cm 2 from the absorption spectrum of Er 3+/Yb 3+-codoped PLZT. The J-O intensity parameters have been used to calculate the radiative lifetimes and the branching ratios for some excited 4I 13/2, 4I 11/2, 4I 9/24F 9/2, and 4S 3/2 levels of Er 3+ ion. The stimulated emission cross-section (8.24×10 -21 cm 2) was evaluated for the 4I 13/2→ 4I 15/2 transition of Er 3+. The upconversion emissions at 538, 564, and 666 nm have been observed in Er 3+/Yb 3+-codoped PLZT by exciting at 980 nm, and their origins were identified and analyzed.

Additives and solvents-induced phase and morphology modification of NaYF{sub 4} for improving up-conversion emission

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhuang, Jianle, E-mail: zhuangjianle@126.com; MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry and Chemical Engineering, Sun Yat-Sen University, Guangzhou 510275; Yang, Xianfeng

Both cubic and hexagonal NaYF{sub 4} were synthesized in different reaction systems via hydro/solvo-thermal route. The effects of reaction temperature, solvents, and additives on the synthesis of NaYF{sub 4} have been studied in detail. It has been shown that phase transformation from cubic NaYF{sub 4} to hexagonal NaYF{sub 4} always occurred. The sequence of the ability for inducing the phase transformation was ethanol>H{sub 2}O>acetic acid. It is found that ethanol can not only facilitate the formation of hexagonal NaYF{sub 4} but also control the growth of the crystal. This is quite unusual for the growth of H-NaYF{sub 4}. The up-conversionmore » emission properties of Yb/Er co-doped NaYF{sub 4} have also been investigated and the results demonstrated some general principles for improving up-conversion emission. - Graphical abstract: Additives and solvents can induce the phase transformation of NaYF{sub 4}, typically the use of organic sodium salt and ethanol. - Highlights: • The effect of additives and solvents on the synthesis of NaYF{sub 4} was studied in detail. • Ethanol can facilitate the formation of H-NaYF{sub 4} while acetic acid restrain it. • Three general principles for improving up-conversion emission were summarized.« less

Optical ridge waveguides in Er3+/Yb3+ co-doped phosphate glass produced by ion irradiation combined with femtosecond laser ablation for guided-wave green and red upconversion emissions

NASA Astrophysics Data System (ADS)

Chen, Chen; He, Ruiyun; Tan, Yang; Wang, Biao; Akhmadaliev, Shavkat; Zhou, Shengqiang; de Aldana, Javier R. Vázquez; Hu, Lili; Chen, Feng

2016-01-01

This work reports on the fabrication of ridge waveguides in Er3+/Yb3+ co-doped phosphate glass by the combination of femtosecond laser ablation and following swift carbon ion irradiation. The guiding properties of waveguides have been investigated at 633 and 1064 nm through end face coupling arrangement. The refractive index profile on the cross section of the waveguide has been constructed. The propagation losses can be reduced considerably after annealing treatment. Under the optical pump laser at 980 nm, the upconversion emission of both green and red fluorescence has been realized through the ridge waveguide structures.

High-Order Model and Dynamic Filtering for Frame Rate Up-Conversion.

PubMed

Bao, Wenbo; Zhang, Xiaoyun; Chen, Li; Ding, Lianghui; Gao, Zhiyong

2018-08-01

This paper proposes a novel frame rate up-conversion method through high-order model and dynamic filtering (HOMDF) for video pixels. Unlike the constant brightness and linear motion assumptions in traditional methods, the intensity and position of the video pixels are both modeled with high-order polynomials in terms of time. Then, the key problem of our method is to estimate the polynomial coefficients that represent the pixel's intensity variation, velocity, and acceleration. We propose to solve it with two energy objectives: one minimizes the auto-regressive prediction error of intensity variation by its past samples, and the other minimizes video frame's reconstruction error along the motion trajectory. To efficiently address the optimization problem for these coefficients, we propose the dynamic filtering solution inspired by video's temporal coherence. The optimal estimation of these coefficients is reformulated into a dynamic fusion of the prior estimate from pixel's temporal predecessor and the maximum likelihood estimate from current new observation. Finally, frame rate up-conversion is implemented using motion-compensated interpolation by pixel-wise intensity variation and motion trajectory. Benefited from the advanced model and dynamic filtering, the interpolated frame has much better visual quality. Extensive experiments on the natural and synthesized videos demonstrate the superiority of HOMDF over the state-of-the-art methods in both subjective and objective comparisons.

Color tunable emission through energy transfer from Yb3+ co-doped SrSnO3: Ho3+ perovskite nano-phosphor

NASA Astrophysics Data System (ADS)

Jain, Neha; Singh, Rajan Kr.; Sinha, Shriya; Singh, R. A.; Singh, Jai

2018-04-01

First time color tunable lighting observed from Ho3+ and Yb3+ co-doped SrSnO3 perovskite. Down-conversion and up-conversion (UC) photoluminescence emission spectra were recorded to understand the whole mechanism of energy migration between Ho3+ and Yb3+ ions. The intensity of green and red emission varies with Yb3+ doping which causes multicolour emissions from nano-phosphor. The intensity of UC red emission (654 nm) obtained from 1 at.% Ho3+ and 3 at.% Yb3+ co-doped nano-phosphor is nine times higher than from 1 at.% Ho3+ doped SrSnO3 nano-phosphor. Enhanced brightness of 654 nm in UC process belongs in biological transparency window so that it might be a promising phosphor in the bio-medical field. Moreover, for the other Yb3+ co-doped nano-phosphor, Commission Internationale de l'Éclairage chromaticity co-ordinates were found near the white region and their CCT values lie in the range 4900-5100 K indicating cool white. Decay time was measured for 545 nm emission of Ho3+ ion found in 7.652 and 8.734 µs at 355 nm excitation. The variation in lifetime was observed in ascending order with increasing Yb3+ concentration which supports PL emission spectra observation that with increasing Yb3+ concentration, rate of transition has changed. These studies reveal that Ho3+ and Yb3+ co-doped phosphor is useful for fabrication of white LEDs.

Experimental demonstration of photon upconversion via cooperative energy pooling

DOE PAGES

Weingarten, Daniel H.; LaCount, Michael D.; van de Lagemaat, Jao; ...

2017-03-15

Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly andmore » simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. As a result, design guidelines are presented to facilitate further research and development of more optimized CEP systems.« less

Experimental demonstration of photon upconversion via cooperative energy pooling

PubMed Central

Weingarten, Daniel H.; LaCount, Michael D.; van de Lagemaat, Jao; Rumbles, Garry; Lusk, Mark T.; Shaheen, Sean E.

2017-01-01

Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly and simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. Design guidelines are presented to facilitate further research and development of more optimized CEP systems. PMID:28294129

Experimental demonstration of photon upconversion via cooperative energy pooling

NASA Astrophysics Data System (ADS)

Weingarten, Daniel H.; Lacount, Michael D.; van de Lagemaat, Jao; Rumbles, Garry; Lusk, Mark T.; Shaheen, Sean E.

2017-03-01

Photon upconversion is a fundamental interaction of light and matter that has applications in fields ranging from bioimaging to microfabrication. However, all photon upconversion methods demonstrated thus far involve challenging aspects, including requirements of high excitation intensities, degradation in ambient air, requirements of exotic materials or phases, or involvement of inherent energy loss processes. Here we experimentally demonstrate a mechanism of photon upconversion in a thin film, binary mixture of organic chromophores that provides a pathway to overcoming the aforementioned disadvantages. This singlet-based process, called Cooperative Energy Pooling (CEP), utilizes a sensitizer-acceptor design in which multiple photoexcited sensitizers resonantly and simultaneously transfer their energies to a higher-energy state on a single acceptor. Data from this proof-of-concept implementation is fit by a proposed model of the CEP process. Design guidelines are presented to facilitate further research and development of more optimized CEP systems.

Deep Photoacoustic/Luminescence/Magnetic Resonance Multimodal Imaging in Living Subjects Using High-Efficiency Upconversion Nanocomposites.

PubMed

Liu, Yu; Kang, Ning; Lv, Jing; Zhou, Zijian; Zhao, Qingliang; Ma, Lingceng; Chen, Zhong; Ren, Lei; Nie, Liming

2016-08-01

A gadolinium-doped multi-shell upconversion nanoparticle under 800 nm excitation is synthesized with a 10-fold fluorescence-intensity enhancement over that under 980 nm. The nanoformulations exhibit excellent photoacoustic/luminescence/magnetic resonance tri-modal imaging capabilities, enabling visualization of tumor morphology and microvessel distribution at a new imaging depth. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Upconversion luminescence nanosensor for TNT selective and label-free quantification in the mixture of nitroaromatic explosives.

PubMed

Ma, Yingxin; Wang, Leyu

2014-03-01

This paper reports a rapid, sensitive, and selective nanosensor for the detection of 2,4,6-trinitrotoluene (TNT) in the mixture aqueous solution of nitroaromatics independent of immunoassay or molecularly imprinted technology and complicated instruments. Despite many strategies including immunoassay and molecularly imprinted technologies been successfully developed for the detection of TNT, it is not easy to differentiate TNT from 2,4,6-trinitrophenol (TNP) due to their very similar chemical structures and properties. In this work, the amine functionalized NaYF4:Yb(3+)/Er(3+) upconversion luminescence nanoparticles (UCNPs) whose excitation (980 nm) and emission (543 nm) wavelength were far from the absorbance bands of other usual interference nitroaromatics including 2,4-dinitrotoluene (DNT), nitrobenzene (NB), and especially TNP, were utilized as the luminescent nanosensors for TNT luminescence detection. To make these UCNPs highly water stable and render the charge transfer from UCNPs to TNT easier, amino groups were introduced onto the surface of the UCNPs by coating a polymer layer of ethylene glycol dimethacrylate (EGDMA) hybridized with 3-aminopropyltriethoxysilane (APTS). After binding with TNT through amino groups on the UCNPs, the naked eye visible green upconversion luminescence of the UCNPs was dramatically quenched and thus a sensitive UC luminescence nanosensor was developed for TNT detection. However, other nitroaromatics including TNP, DNT, and NB have no influence on the green UC luminescence and thus no influence on the TNT detection. The luminescence intensity is negatively proportional to the concentration of TNT in the range of 0.01-9.0 µg/mL with the 3σ limit of detection (LOD) of 9.7 ng/mL. The present studies provide a novel and facile strategy to fabricate the upconversion luminescence sensors with highly selective recognition ability in aqueous media and are desirable for label free analysis of TNT in mixed solution independent of immunoassay and molecularly imprinted technology and complicated instruments. © 2013 Published by Elsevier B.V.

Mechanisms of optical losses in the 5D4 and 5D3 levels in Tb3+ doped low silica calcium aluminosilicate glasses

NASA Astrophysics Data System (ADS)

dos Santos, J. F. M.; Terra, I. A. A.; Astrath, N. G. C.; Guimarães, F. B.; Baesso, M. L.; Nunes, L. A. O.; Catunda, T.

2015-02-01

Trivalent Tb-doped materials exhibit strong emission in the green and weak emission in the UV-blue levels. Usually, this behavior is attributed to the cross relaxation (CR) process. In this paper, the luminescence properties of Tb3+-doped low silica calcium aluminosilicate glasses are analyzed for UV (λexc = 325 nm) and visible (488 nm) excitations. Under 325 nm excitation, the intensity of green luminescence increases proportionally to Tb3+ concentration. However, the blue luminescence intensity is strongly reduced with the increase of concentration from 0.5-15.0 wt. %. In the case of 488 nm excitation, a saturation behavior of the green emission is observed at intensities two orders of magnitude smaller than expected for bleaching of the ground state population. Using a rate equation model, we showed that this behavior can be explained by an excited state absorption cross section two orders of magnitude larger than the ground state absorption. The blue emission is much weaker than expected from our rate equations (325 nm and 488 nm excitation). We concluded that only the CR process cannot explain the overall feature of measured luminescence quenching in the wide range of Tb3+ concentrations. Cooperative upconversion from a pair of excited ions (5D3:5D3 or 5D3:5D4) and other mechanisms involving upper lying states (4f5d, charge transfer, host matrix, defects, etc.) may play a significant role.

Thermal, optical and vibrational studies of tyrosine doped LaF3:Ce nanoparticles for bioimaging and biotagging

NASA Astrophysics Data System (ADS)

Singh, Amit T.

2018-05-01

Upconversion quantum dots of tyrosine doped LaF3:Ce nanoparticles have been synthesized by wet chemical route. The thermal studies (TGA/DTA) confirm the crystallinity and stability of different phases of synthesized nanoparticles. The UV-Visible spectra show multiple absorption edges at 215.60 nm and 243.10 nm indicating quantum dot nature of the synthesized nanoparticles. The PL spectra showed upconversion with sharp emission peak at 615 nm (red colour). The FT-RAMAN spectra of the synthesized nanoparticles show the modification of the surface of the nanoparticles in the form of functional groups and skeletal groups. Upconversion nature of the synthesized nanoparticles indicates their potential application in bioimaging and biotagging.

Photon correlation in single-photon frequency upconversion.

PubMed

Gu, Xiaorong; Huang, Kun; Pan, Haifeng; Wu, E; Zeng, Heping

2012-01-30

We experimentally investigated the intensity cross-correlation between the upconverted photons and the unconverted photons in the single-photon frequency upconversion process with multi-longitudinal mode pump and signal sources. In theoretical analysis, with this multi-longitudinal mode of both signal and pump sources system, the properties of the signal photons could also be maintained as in the single-mode frequency upconversion system. Experimentally, based on the conversion efficiency of 80.5%, the joint probability of simultaneously detecting at upconverted and unconverted photons showed an anti-correlation as a function of conversion efficiency which indicated the upconverted photons were one-to-one from the signal photons. While due to the coherent state of the signal photons, the intensity cross-correlation function g(2)(0) was shown to be equal to unity at any conversion efficiency, agreeing with the theoretical prediction. This study will benefit the high-speed wavelength-tunable quantum state translation or photonic quantum interface together with the mature frequency tuning or longitudinal mode selection techniques.

Measuring upconversion nanoparticles photoluminescence lifetime with FastFLIM and phasor plots

NASA Astrophysics Data System (ADS)

Sun, Yuansheng; Lee, Hsien-Ming; Qiu, Hailin; Liao, Shih-Chu Jeff; Coskun, Ulas; Barbieri, Beniamino

2018-02-01

Photon upconversion is a nonlinear process in which the sequential of absorption of two or more photons leads to the anti-stoke emission. Different than the conventional multiphoton excitation process, upconversion can be efficiently performed at low excitation densities. Recent developments in lanthanide-doped upconversion nanoparticles (UCNPs) have led to a diversity of applications, including detecting and sensing of biomolecules, imaging of live cells, tissues and animals, cancer diagnostic and therapy, etc. Measuring the upconversion lifetime provides a new dimension of its imaging and opens a new window for its applications. Due to the long metastable intermediate excited state, UCNP typically has a long excited state lifetime ranging from sub-microseconds to milliseconds. Here, we present a novel development using the FastFLIM technique to measure UCNP lifetime by laser scanning confocal microscopy. FastFLIM is capable of measuring lifetime from 100 ps to 100 ms and features the high data collection efficiency (up to 140-million counts per second). Other than the traditional nonlinear least-square fitting analysis, the raw data acquired by FastFLIM can be directly processed by the model-free phasor plots approach for instant and unbiased lifetime results, providing the ideal routine for the UCNP photoluminescence lifetime microscopy imaging.

Enhanced Power Conversion Efficiency of Perovskite Solar Cells with an Up-Conversion Material of Er3+-Yb3+-Li+ Tri-doped TiO2

NASA Astrophysics Data System (ADS)

Zhang, Zhenlong; Qin, Jianqiang; Shi, Wenjia; Liu, Yanyan; Zhang, Yan; Liu, Yuefeng; Gao, Huiping; Mao, Yanli

2018-05-01

In this paper, Er3+-Yb3+-Li+ tri-doped TiO2 (UC-TiO2) was prepared by an addition of Li+ to Er3+-Yb3+ co-doped TiO2. The UC-TiO2 presented an enhanced up-conversion emission compared with Er3+-Yb3+ co-doped TiO2. The UC-TiO2 was applied to the perovskite solar cells. The power conversion efficiency (PCE) of the solar cells without UC-TiO2 was 14.0%, while the PCE of the solar cells with UC-TiO2 was increased to 16.5%, which presented an increase of 19%. The results suggested that UC-TiO2 is an effective up-conversion material. And this study provided a route to expand the spectral absorption of perovskite solar cells from visible light to near-infrared using up-conversion materials.

Tailoring Plasmonic Enhanced Upconversion in Single NaYF4:Yb3+/Er3+ Nanocrystals

NASA Astrophysics Data System (ADS)

Wang, Ya-Lan; Mohammadi Estakhri, Nasim; Johnson, Amber; Li, Hai-Yang; Xu, Li-Xiang; Zhang, Zhenyu; Alù, Andrea; Wang, Qu-Quan; Shih, Chih-Kang (Ken)

2015-05-01

By using silver nanoplatelets with a widely tunable localized surface plasmon resonance (LSPR), and their corresponding local field enhancement, here we show large manipulation of plasmonic enhanced upconversion in NaYF4:Yb3+/Er3+ nanocrystals at the single particle level. In particular, we show that when the plasmonic resonance of silver nanolplatelets is tuned to 656 nm, matching the emission wavelength, an upconversion enhancement factor ~5 is obtained. However, when the plasmonic resonance is tuned to 980 nm, matching the nanocrystal absorption wavelength, we achieve an enhancement factor of ~22 folds. The precise geometric arrangement between fluorescent nanoparticles and silver nanoplatelets allows us to make, for the first time, a comparative analysis between experimental results and numerical simulations, yielding a quantitative agreement at the single particle level. Such a comparison lays the foundations for a rational design of hybrid metal-fluorescent nanocrystals to harness the upconversion enhancement for biosensing and light harvesting applications.

Enhanced Power Conversion Efficiency of Perovskite Solar Cells with an Up-Conversion Material of Er3+-Yb3+-Li+ Tri-doped TiO2.

PubMed

Zhang, Zhenlong; Qin, Jianqiang; Shi, Wenjia; Liu, Yanyan; Zhang, Yan; Liu, Yuefeng; Gao, Huiping; Mao, Yanli

2018-05-11

In this paper, Er 3+ -Yb 3+ -Li + tri-doped TiO 2 (UC-TiO 2 ) was prepared by an addition of Li + to Er 3+ -Yb 3+ co-doped TiO 2 . The UC-TiO 2 presented an enhanced up-conversion emission compared with Er 3+ -Yb 3+ co-doped TiO 2 . The UC-TiO 2 was applied to the perovskite solar cells. The power conversion efficiency (PCE) of the solar cells without UC-TiO 2 was 14.0%, while the PCE of the solar cells with UC-TiO 2 was increased to 16.5%, which presented an increase of 19%. The results suggested that UC-TiO 2 is an effective up-conversion material. And this study provided a route to expand the spectral absorption of perovskite solar cells from visible light to near-infrared using up-conversion materials.

Tuning the morphology, luminescence and magnetic properties of hexagonal-phase NaGdF4: Yb, Er nanocrystals via altering the addition sequence of the precursors

NASA Astrophysics Data System (ADS)

Zhao, Shuwen; Xia, Donglin; Zhao, Ruimin; Zhu, Hao; Zhu, Yiru; Xiong, Yuda; Wang, Youfa

2017-01-01

Hexagonal-phase NaGdF4: Yb, Er upconversion nanocrystals (UCNCs) with tunable morphology and properties were successfully prepared via a thermal decomposition method. The influences of the adding sequence of the precursors on the morphology, chemical composition, luminescence and magnetic properties were investigated by transmission electron microscopy (TEM), inductively coupled plasma-atomic emission spectrometry (ICP-AES), upconversion (UC) spectroscopy, and a vibrating sample magnetometer (VSM). It was found that the resulting nanocrystals, with different sizes ranging from 24 to 224 nm, are in the shape of spheres, hexagonal plates and flakes; moreover, the composition percentage of Yb3+-Er3+ and Gd3+ ions was found to vary in a regular pattern with the adding sequence. Furthermore, the intensity ratios of emission colors (f g/r, f g/p), and the magnetic mass susceptibility of hexagonal-phase NaGdF4: Yb, Er nanocrystals change along with the composition of the nanocrystals. A positive correlation between the susceptibility and f g/r of NaGdF4: Yb, Er was proposed. The decomposition processes of the precursors were investigated by a thermogravimetric (TG) analyzer. The result indicated that the decomposition of the resolved lanthanide trifluoroacetate is greatly different from lanthanide trifluoroacetate powder. It is of tremendous help to recognize the decomposition process of the precursors and to understand the related reaction mechanism.

Temperature-dependent luminescence and temperature-stimulated NIR-to-VIS up-conversion in Nd3+-doped La2O3-Na2O-ZnO-TeO2 glasses

NASA Astrophysics Data System (ADS)

Sobczyk, Marcin

2013-04-01

Telluride glasses of the composition xNd2O3-(7-x)La2O3-3Na2O-25ZnO-65TeO2, where (0≤x≤7) were prepared by the melt quench technique. Some physical and optical properties of the glasses were evaluated. The thermal behavior i.e. glass transition and crystallization temperatures were studied by using TGA-DTA technique. Optical properties of Nd3+-doped telluride glasses were investigated between 298 and 700 K. Basing on the obtained values of J-O parameter values (×10-20 cm2: Ω2=4.49±0.84, Ω4=5.03±0.61, Ω6=4.31±0.73), the radiative transition probabilities (AT), radiative lifetimes (τR), fluorescence branching ratios (β) and emission cross-sections (σem) were calculated for the 4F3/2→4IJ/2 (where J=9, 11 and 13) transitions of Nd3+ ions. The τR value of the 4F3/2 level amount to 164 μs and is slightly higher than the measured decay time of 162 μs. With the increasing of Nd2O3 concentration from 0.5 to 7.0 mol% the experimental lifetime of the fluorescent level decreases from 162 to 5.6 μs. The estimated quantum efficiency amount to 100%, based on a comparison of τR and the experimental decay time of a slightly doped Nd3+ telluride glass. An analysis of the non-radiative decay was based on the cross-relaxation mechanisms. The 4F3/2→4I9/2 and 4F5/2→4I9/2 transitions were analyzed with respect to the fluorescence intensity ratio (FIR) and were found to be temperature dependent. Infrared-to-visible up-conversion emissions with a maximum at 603.0 and 635.3 nm were observed at high temperatures using the 804 nm excitation and are due to the 4G5/2→4I9/2 and 4G5/2→4I11/2 transitions of Nd3+ ions, respectively. The near quadratic dependence of fluorescence on excitation laser power confirms that two photons contribute to up-conversion of the orange emissions. The temperature-stimulated up-conversion excitation processes have been analyzed in detail. The optical results indicate that the investigated glasses are potentially applicable as a 1063 nm laser host as well as an optical sensor for temperature measurements.

Dual functional NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Nd3+ core-shell nanoparticles for cell temperature sensing and imaging

NASA Astrophysics Data System (ADS)

Shi, Zengliang; Duan, Yue; Zhu, Xingjun; Wang, Qiwei; Li, DongDong; Hu, Ke; Feng, Wei; Li, Fuyou; Xu, Chunxiang

2018-03-01

Lanthanide-doped up-conversion nanoparticles (UCNPs) provide a remote temperature sensing approach to monitoring biological microenvironments. In this research, the UCNPs of NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Nd3+ with hexagonal (β)-phase were synthesized and applied in cell temperature sensing as well as imaging after surface modification with meso-2, 3-dimercaptosuccinic acid. In the core-shell UCNPs, Yb3+ ions were introduced as energy transfer media between sensitizers of Nd3+ and activators of Er3+ to improve Er3+emission and prevent their quenching behavior due to multiple energy levels of Nd3+. Under the excitations of 808 nm and 980 nm lasers, the NaYF4:Yb3+, Er3+@NaYF4:Yb3+, Nd3+ nanoparticles exhibited an efficient green band with two emission peaks at 525 nm and 545 nm, respectively, which originated from the transitions of 2H11/2 → 4I15/2 and 4S3/2 → 4I15/2 for Er3+ ions. We demonstrate that an occurrence of good logarithmic linearity exists between the intensity ratio of these two emission peaks and the reciprocal of the inside or outside temperature of NIH-3T3 cells. A better thermal stability is proved through temperature-dependent spectra with a heating-cooling cycle. The obtained viability of NIH-3T3 cells is greater than 90% after incubations of about 12 and 24 (h), and they possess a lower cytotoxicity of UCNPs. This work provides a method for monitoring the cell temperature and its living state from multiple dimensions including temperature response, cell images and visual up-conversion fluorescent color.

Structural and optical investigation in Er3+ doped Y2MoO6 phosphors

NASA Astrophysics Data System (ADS)

Mondal, Manisha; Rai, Vineet Kumar

2018-05-01

The Er3+ doped Y2MoO6 phosphors have been structurally and optically characterized by X-ray Diffraction (XRD), Field emission scanning electron microscopy (FESEM), UV-Vis absorption spectroscopy and frequency upconversion (UC) emission studies. The crystal and the particles size are found to be ˜ 85 nm and ˜ 200 nm from XRD and FESEM analysis. The intense peak at ˜ 206 nm in the UV-Vis absorption spectroscopy is attributed due to the charge transfer transition between the Mo6+ and the O2- ions in the MoO4 group in the host molybdate. The frequency UC emission studies of the prepared phosphors under 980 nm diode laser excitation shows the intense UC emission in the 0.3 mol% concentrations for the Er3+ ions. In the UC emission spectra, the emission peaks at green (˜ 525 nm and ˜ 546 nm) and red (˜ 656 nm) bands are corresponding to the 2H11/2, 4S3/2 → 4I15/2 and 4F9/2 → 4I15/2 transitions of Er3+ ions. The mechanisms involved in the UC process have been explored with the help of energy level diagram. Moreover, the CIE point (0.31, 0.60) lie in the green colour region which indicates that the developed phosphor have suitable applications in NIR to visible upconverter and in making green light display devices.

Blue-green upconversion laser

DOEpatents

Nguyen, D.C.; Faulkner, G.E.

1990-08-14

A blue-green laser (450--550 nm) uses a host crystal doped with Tm[sup 3+]. The Tm[sup 3+] is excited through upconversion by a red pumping laser and an IR pumping laser to a state which transitions to a relatively lower energy level through emissions in the blue-green band, e.g., 450.20 nm at 75 K. The exciting laser may be tunable dye lasers or may be solid-state semiconductor laser, e.g., GaAlAs and InGaAlP. 3 figs.

Blue-green upconversion laser

DOEpatents

Nguyen, Dinh C.; Faulkner, George E.

1990-01-01

A blue-green laser (450-550 nm) uses a host crystal doped with Tm.sup.3+. The Tm.sup.+ is excited through upconversion by a red pumping laser and an IR pumping laser to a state which transitions to a relatively lower energy level through emissions in the blue-green band, e.g., 450.20 nm at 75 K. The exciting laser may be tunable dye lasers or may be solid-state semiconductor laser, e.g., GaAlAs and InGaAlP.

Dental optical tomography with upconversion nanoparticles—a feasibility study

PubMed Central

Long, Feixiao; Intes, Xavier

2017-01-01

Abstract. Upconversion nanoparticles (UCNPs) have the unique ability to emit multiple colors upon excitation by near-infrared (NIR) light. Herein, we investigate the potential use of UCNPs as contrast agents for dental optical tomography, with a focus on monitoring the status of fillings after dental restoration. The potential of performing tomographic imaging using UCNP emission of visible or NIR light is established. This in silico and ex vivo study paves the way toward employing UCNPs as theranostic agents for dental applications. PMID:28586852

Dental optical tomography with upconversion nanoparticles—a feasibility study

NASA Astrophysics Data System (ADS)

Long, Feixiao; Intes, Xavier

2017-06-01

Upconversion nanoparticles (UCNPs) have the unique ability to emit multiple colors upon excitation by near-infrared (NIR) light. Herein, we investigate the potential use of UCNPs as contrast agents for dental optical tomography, with a focus on monitoring the status of fillings after dental restoration. The potential of performing tomographic imaging using UCNP emission of visible or NIR light is established. This in silico and ex vivo study paves the way toward employing UCNPs as theranostic agents for dental applications.

Dental optical tomography with upconversion nanoparticles-a feasibility study.

PubMed

Long, Feixiao; Intes, Xavier

2017-06-01

Upconversion nanoparticles (UCNPs) have the unique ability to emit multiple colors upon excitation by near-infrared (NIR) light. Herein, we investigate the potential use of UCNPs as contrast agents for dental optical tomography, with a focus on monitoring the status of fillings after dental restoration. The potential of performing tomographic imaging using UCNP emission of visible or NIR light is established. This in silico and ex vivo study paves the way toward employing UCNPs as theranostic agents for dental applications.

Highly efficient up-conversion and bright white light in RE co-doped KYF4 nanocrystals in sol-gel silica matrix

NASA Astrophysics Data System (ADS)

Méndez-Ramos, J.; Yanes, A. C.; Santana-Alonso, A.; del-Castillo, J.

2013-01-01

Transparent nano-glass-ceramics comprising Yb3+, Er3+ and Tm3+ co-doped KYF4 nanocrystals have been developed from sol-gel method. A structural analysis by means of X-ray diffraction confirmed the precipitation of cubic KYF4 nanocrystals into a silica matrix. Visible luminescence has been analyzed as function of treatment temperature of precursor sol-gel glasses. Highly efficient up-conversion emissions have been obtained under 980 nm excitation and studied by varying the doping level, processing temperature and pump power. Color tuneability has been quantified in terms of CIE diagram and in particular, a white-balanced overall emission has been achieved for a certain doping level and thermal treatment.

Characterization and cysteine sensing performance of nanocomposites based on up-conversion excitation host and rhodamine-derived probes

NASA Astrophysics Data System (ADS)

Yuqing, Zhao; Yi, Xing; Lihua, Li; Juanjuan, Ma

2018-02-01

Optical sensing for cysteine (Cys) recognition is an interesting topic due to Cys biological participation. In this paper, two rhodamine-based chemosensors were designed for Cys optical sensing. For chemosensor photostability improvement, up-conversion nanocrystals were synthesized and used as excitation host. These nanocrystals were modified with a phase transfer reagent α-cyclodextrin (α-CD) to improve their compatibility with chemosensors. An efficient energy transfer from these nanocrystals to chemosensors under 980 nm radiation was observed and confirmed by spectral match analysis, energy transfer radius calculation and emission decay lifetime comparison. A direct bonding mechanism between Cys and chemosensors with bonding stoichiometry of 1:1 was established by Job's plot experiment. Given the presence of Cys, chemosensor emission was increased, showing emission turn on effect. These two chemosensors showed good selectivity, improved photostability and linear sensing response towards Cys.

Optical transitions of Er3+/Yb3+ codoped TeO2-WO3-Bi2O3 glass.

PubMed

Shen, Xiang; Nie, Qiuhua; Xu, Tiefeng; Gao, Yuan

2005-10-01

Optical absorption and emission properties of the Er3+/Yb3+ codoped TeO2-WO3-Bi2O3 (TWB) glass has been investigated. The transition probabilities, excited state lifetimes, and the branching ratios have been predicted for Er3+ based on the Judd-Ofelt theory. The broad 1.5 microm fluorescence was observed under 970 nm excitation, and its full width at half maximum (FWHM) is 77 nm. The emission cross-section is calculated using the McCumber theory, and the peak emission cross-section is 1.03 x 10(-21) cm2 at 1.531 microm. This value is much larger than those of the silicate and phosphate glasses. Efficient green and weak red upconversion luminescence from Er3+ centers in the glass sample was observed at room temperature, and the upconversion excitation processes have been analyzed.

Magnetic Field Effects on Triplet-Triplet Annihilation in Solutions: Modulation of Visible/NIR Luminescence.

PubMed

Mani, Tomoyasu; Vinogradov, Sergei A

2013-08-06

Photon upconversion based on sensitized triplet-triplet annihilation (TTA) presents interest for such areas as photovoltaics and imaging. Usually energy upconversion is observed as p -type delayed fluorescence from molecules whose triplet states are populated via energy transfer from a suitable triplet donor, followed by TTA. Magnetic field effects (MFE) on delayed fluorescence in molecular crystals are well known; however, there exist only a few examples of MFE on TTA in solutions, and all of them are limited to UV-emitting materials. Here we present MFE on TTA-mediated visible and near infrared (NIR) emission, sensitized by far-red absorbing metalloporphyrins in solutions at room temperature. In addition to visible delayed fluorescence from annihilator, we also observed NIR emission from the sensitizer, occurring as a result of triplet-triplet energy transfer back from annihilator, termed "delayed phosphorescence". This emission also exhibits MFE, but opposite in sign to the annihilator fluorescence.

Improvement of Er 3+ emissions in oxyfluoride glass ceramic nano-composite by thermal treatment

NASA Astrophysics Data System (ADS)

Chen, Daqin; Wang, Yuansheng; Yu, Yunlong; Ma, En

2006-05-01

In order to improve the 1.53 μm emission of Er 3+-doped oxyfluoride glass ceramic containing CaF 2 nano-crystals, series of samples with same Er 3+ doping lever thermal treated under different conditions were prepared. The UV-VIR-NIR absorption spectra, near-infrared and up-conversion emission spectra, and 4I13/2 decay curves were measured. Based on Judd-Ofelt theory, the radiative transition probability, fluorescence branching ratio and radiative decay time of various metastable transitions of precursor glass and glass ceramics were evaluated. With the increasing of heating temperature, the Judd-Ofelt intensity parameter Ω2 monotonously decreased from 4.39×10 -20 to 2.72×10 -20 cm 2; the emission lifetime and quantum efficiency significantly increased from 5.9 to 8.0 ms and 70% to 98%, respectively. The wavelength dependence of gain cross-sections of oxyfluoride glass and glass ceramics were computed to be relatively flat in the range of 1530-1565 nm for population inversion from 0.7 to 1.0.

Stark sublevels investigation in Y2WO6:Tm3+-Yb3+ phosphor for thermometry and internal temperature measurement

NASA Astrophysics Data System (ADS)

Soni, Abhishek Kumar

2018-05-01

Intensity ratio investigation in the Y2WO6:Tm3+-Yb3+ phosphors synthesized by solid state reaction method has been discussed first time under 980 nm laser diode excitation with the help of multiple peak fitting. The temperature dependent upconversion emission study has been performed for optical temperature sensing by using stark sublevels of 1G4 level of Tm3+ ion. The intensity of the two stark sublevels is varied due to the thermalization under the application of external temperature. The energy gap has been calculated about ∼427 cm‑1 of the two stark sublevels via Boltzmann’s population distribution law. The calculated sensitivity (maximum about ∼34 × 10‑4 K‑1 at 303 K) and optical heating properties prove the utility of the prepared phosphor in making optical temperature sensing probe and optical heater.

[Preparation, characterization and upconversion fluorescence of NaYF4 : Yb, Er /graphene oxide nanocomposites].

PubMed

Ji, Tian-Hao; Qie, Nan; Wang, Ji-Mei; Hua, Yong-Yong; Ji, Zhi-Jiang

2013-03-01

NaYF4 : Yb, Er/rGO and SiO2-coated NaYF4 : Yb, Er/rGO nanocomposites can be prepared through "one-pot" and directly mixing preparation routes. Various measurement results show that the NaYF4 : Yb, Er in the nanocomposites exhibits a cubic a-type structure and nanoparticle-like morphology with a diameter range of 30-70 nm; the rGO layers are well-dispersed in the nanocomposites, and whereas the rGO obtained from "one-pot" preparation renders relatively better dispersion. Raman spectra demonstrate that there exists a surface coupling action between the two kinds of nanomaterials, and with the increase in the relative rGO content, such action becomes stronger. UC fluorescence measurement results reveal that the rGO has significantly quenching effect and optical-limiting performance on the UC fluorescence, particularly on the red-emission of the NaYFa : Yb, Er or SiO2-coated NaYF4 : Yb, Er nanoparticles. The red-emission intensity gradually decreases with an increase in the rGO content, but the green-emission shows less change. It should be stressed that, in comparison with NaYF4 : Yb, Er/rGO, with a similar rGO content, the red-emission intensity of SiO2-coated NaYF4 : Yb, Er/rGO decreases much obviously due to a stronger light-absorption caused by part rGO aggregation.

Photon upconversion towards applications in energy conversion and bioimaging

NASA Astrophysics Data System (ADS)

Sun, Qi-C.; Ding, Yuchen C.; Sagar, Dodderi M.; Nagpal, Prashant

2017-12-01

The field of plasmonics can play an important role in developing novel devices for application in energy and healthcare. In this review article, we consider the progress made in design and fabrication of upconverting nanoparticles and metal nanostructures for precisely manipulating light photons, with a wavelength of several hundred nanometers, at nanometer length scales, and describe how to tailor their interactions with molecules and surfaces so that two or more lower energy photons can be used to generate a single higher energy photon in a process called photon upconversion. This review begins by introducing the current state-of-the-art in upconverting nanoparticle synthesis and achievements in color tuning and upconversion enhancement. Through understanding and tailoring physical processes, color tuning and strong upconversion enhancement have been demonstrated by coupling with surface plasmon polariton waves, especially for low intensity or diffuse infrared radiation. Since more than 30% of incident sunlight is not utilized in most photovoltaic cells, this photon upconversion is one of the promising approaches to break the so-called Shockley-Queisser thermodynamic limit for a single junction solar cell. Furthermore, since the low energy photons typically cover the biological window of optical transparency, this approach can also be particularly beneficial for novel biosensing and bioimaging techniques. Taken together, the recent research boosts the applications of photon upconversion using designed metal nanostructures and nanoparticles for green energy, bioimaging, and therapy.

Enhancing light harvesting and charge transport in organic solar cells via integrating lanthanide-doped upconversation materials

NASA Astrophysics Data System (ADS)

Wang, Fei; Yang, Xiao-Yu; Niu, Meng-si; Feng, Lin; Lv, Cheng-kun; Zhang, Kang-ning; Bi, Peng-qing; Yang, Junliang; Hao, Xiao-Tao

2018-07-01

Irradiation of lanthanide-doped upconversion nanoparticles with infrared light can lead to the emission of visible light, which is subsequently absorbed by the organic photoactive layer resulting in the performance enhancement of organic solar cells (OSCs). In this work, OSCs based on poly (3-hexylthiophene) (P3HT) and Phenyl C61 butyric acid methyl ester (PC61BM) blending ytterbium(III), erbium(III) co-doped sodium yttrium fluoride (NaYF4: Yb3+, Er3+) nanoparticles were fabricated with inverted structures. The results indicated that the short current density (J sc) and fill factor were apparently enhanced from 8.60 mA cm‑2 to 9.31 mA cm‑2 and from 57.96% to 64.84%, respectively, leading to an increment of power conversion efficiency (PCE). The photocurrent improvement may have attributed to the additional absorption light generated from upconversion with 980 nm excitation. The active layers with upconversion nanoparticles were investigated to prove enhanced light harvesting, charge transport and energy transfer from upconversion nanoparticles to P3HT. A synergistic effect of broadening light harvesting, efficient energy transfer process, increased carrier mobility and enhanced exciton dissociation in the polymer bulk heterojunction may contribute to the performance enhancement.

Investigation of Upconversion, downshifting and quantum –cutting behavior of Eu3+, Yb3+, Bi3+ co-doped LaNbO4 phosphor as a spectral conversion material

NASA Astrophysics Data System (ADS)

Dwivedi, A.; Mishra, K.; Rai, S. B.

2018-06-01

This work presents the spectral conversion characteristics [upconversion (UC), downshifting (DS) and quantum–cutting (QC) optical processes] of Eu3+, Yb3+ and Bi3+ co-doped LaNbO4 (LBO) phosphor samples synthesized by solid state reaction technique. The crystal structure and the pure phase formation have been confirmed by x-ray diffraction (XRD) measurements. The surface morphology and particle size are studied by scanning electron microscopy (SEM). The rarely observed intense red UC emission from Eu3+ ion has been successfully obtained in Eu3+/Yb3+ co-doped LaNbO4 phosphor (on excitation with 980 nm) by optimizing the concentrations of Eu3+ and Yb3+ ions. The downshifting (DS) behavior has been studied by photoluminescence (PL) measurements on excitation with 265 nm wavelength from a Xe lamp source. A broad blue emission in the region 300–550 nm with its maximum ∼415 nm due to charge transfer band (CTB) of the host and large number of sharp peaks due to f-f transitions of Eu3+ ion have been observed. The energy transfer has been observed from (NbO4)3‑ to Eu3+ ion and the fluorescence emission has been optimized by varying the concentration of Eu3+ ion. An intense red emission has also been observed corresponding to 5D0 → 7F2 transition of Eu3+ ion at 611 nm in LBO: 0.09Eu3+ phosphor on excitation with 394 nm. The luminescence properties of Eu3+ ion are enhanced further through the sensitization effect of Bi3+ ion. The near infra-red (NIR) quantum cutting (QC) behavior due to Yb3+ ion has been monitored on excitation with 265 as well as 394 nm. The NIR QC is observed due to 2F5/2 → 2F7/2 transition of Yb3+ ion via co-operative energy transfer (CET) process from (NbO4)3‑ as well as Eu3+ ions to Yb3+ ion. This multimodal behavior (UC, DS and QC) makes this a promising phosphor material for multi-purpose spectral converter.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Santos, J. F. M. dos; Terra, I. A. A.; Nunes, L. A. O.

Trivalent Tb-doped materials exhibit strong emission in the green and weak emission in the UV-blue levels. Usually, this behavior is attributed to the cross relaxation (CR) process. In this paper, the luminescence properties of Tb{sup 3+}-doped low silica calcium aluminosilicate glasses are analyzed for UV (λ{sub exc} = 325 nm) and visible (488 nm) excitations. Under 325 nm excitation, the intensity of green luminescence increases proportionally to Tb{sup 3+} concentration. However, the blue luminescence intensity is strongly reduced with the increase of concentration from 0.5–15.0 wt. %. In the case of 488 nm excitation, a saturation behavior of the green emission is observed at intensities two ordersmore » of magnitude smaller than expected for bleaching of the ground state population. Using a rate equation model, we showed that this behavior can be explained by an excited state absorption cross section two orders of magnitude larger than the ground state absorption. The blue emission is much weaker than expected from our rate equations (325 nm and 488 nm excitation). We concluded that only the CR process cannot explain the overall feature of measured luminescence quenching in the wide range of Tb{sup 3+} concentrations. Cooperative upconversion from a pair of excited ions ({sup 5}D{sub 3}:{sup 5}D{sub 3} or {sup 5}D{sub 3}:{sup 5}D{sub 4}) and other mechanisms involving upper lying states (4f5d, charge transfer, host matrix, defects, etc.) may play a significant role.« less

Upconversion luminescence and blackbody radiation in tetragonal YSZ co-doped with Tm(3+) and Yb(3+).

PubMed

Soares, M R N; Ferro, M; Costa, F M; Monteiro, T

2015-12-21

Lanthanide doped inorganic nanoparticles with upconversion luminescence are of utmost importance for biomedical applications, solid state lighting and photovoltaics. In this work we studied the downshifted luminescence, upconversion luminescence (UCL) and blackbody radiation of tetragonal yttrium stabilized zirconia co-doped with Tm(3+) and Yb(3+) single crystals and nanoparticles produced by laser floating zone and laser ablation in liquids, respectively. The photoluminescence (PL) and PL excitation (PLE) were investigated at room temperature (RT). PL spectra exhibit the characteristic lines in UV, blue/green, red and NIR regions of the Tm(3+) (4f(12)) under resonant excitation into the high energy (2S+1)LJ multiplets. Under NIR excitation (980 nm), the samples placed in air display an intense NIR at ∼800 nm due to the (1)G4→(3)H5/(3)H4→(3)H6 transitions. Additionally, red, blue/green and ultraviolet UCL is observed arising from higher excited (1)G4 and (1)D2 multiplets. The power excitation dependence of the UCL intensity indicated that 2-3 low energy absorbed photons are involved in the UCL for low power levels, while for high powers, the identified saturation is dependent on the material size with a enhanced effect on the NPs. The temperature dependence of the UCL was investigated for single crystals and targets used in the ablation. An overall increase of the integrated intensity was found to occur between 12 K and the RT. The thermally activated process is described by activation energies of 10 meV and 30 meV for single crystals and targets, respectively. For the NPs, the UCL was found to be strongly sensitive to pressure conditions. Under vacuum conditions, instead of the narrow lines of the Tm(3+), a wide blackbody radiation was detected, responsible for the change in the emission colour from blue to orange. This phenomenon is totally reversible when the NPs are placed at ambient pressure. The UCL/blackbody radiation in the nanosized material exhibits non-contact pressure colour-based sensor characteristics. Moreover, tuning the color of the blackbody radiation in the nanoparticles by harvesting the low energy photons into the visible spectral region was found to be possible by adjusting the excitation power, paving the way for further developments of these nanoparticles for lighting and photovoltaic applications.

2D Layered Materials of Rare-Earth Er-Doped MoS2 with NIR-to-NIR Down- and Up-Conversion Photoluminescence.

PubMed

Bai, Gongxun; Yuan, Shuoguo; Zhao, Yuda; Yang, Zhibin; Choi, Sin Yuk; Chai, Yang; Yu, Siu Fung; Lau, Shu Ping; Hao, Jianhua

2016-09-01

A 2D system of Er-doped MoS2 layered nanosheets is developed. Structural studies indicate that the Er atoms can be substitutionally introduced into MoS2 to form stable doping. Density functional theory calculation implies that the system remains stable. Both NIR-to-NIR up-conversion and down-conversion light-emissions are observed in 2D transition metal dichalcogenides, ascribed to the energy transition from Er(3+) dopants. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Slow-light-enhanced upconversion for photovoltaic applications in one-dimensional photonic crystals.

PubMed

Johnson, Craig M; Reece, Peter J; Conibeer, Gavin J

2011-10-15

We present an approach to realizing enhanced upconversion efficiency in erbium (Er)-doped photonic crystals. Slow-light-mode pumping of the first Er excited state transition can result in enhanced emission from higher-energy levels that may lead to finite subbandgap external quantum efficiency in crystalline silicon solar cells. Using a straightforward electromagnetic model, we calculate potential field enhancements of more than 18× within he slow-light mode of a one-dimensional photonic crystal and discuss design trade-offs and considerations for photovoltaics.

Energy transfer and up-conversion in rare-earth doped dielectric crystals

NASA Astrophysics Data System (ADS)

Tkachuk, Alexandra M.

1996-01-01

In this work, we consider the prospects of development of the visible, and IR laser-diode pumped lasers based on TR3+-doped double-fluoride crystals. On the basis of estimates of the probabilities of competing non-radiative energy-transfer processes obtained from the experiments and theoretical calculations, the conclusions are drawn on the efficiency of up-conversion pumping and selfquenching of the upper TR3+ states excited by laser-diode emission. The effect of the host composition, dopant concentration, and temperature on the efficiency of up-conversion processes is demonstrated on the example of the YLF:Nd, YLF:Er, BaY2F8:Er, and BaY2F8:Er,Yb crystals. The transfer microparameters for most important cross-relaxation transitions are determined and the conclusions about interaction mechanisms are drawn.

NaGd(MoO4)2 nanocrystals with diverse morphologies: controlled synthesis, growth mechanism, photoluminescence and thermometric properties.

PubMed

Li, Anming; Xu, Dekang; Lin, Hao; Yang, Shenghong; Shao, Yuanzhi; Zhang, Yueli

2016-08-10

Pure tetragonal phase, uniform and well-crystallized sodium gadolinium molybdate (NaGd(MoO4)2) nanocrystals with diverse morphologies, e.g. nanocylinders, nanocubes and square nanoplates have been selectively synthesized via oleic acid-mediated hydrothermal method. The phase, structure, morphology and composition of the as-synthesized products are studied. Contents of both sodium molybdate and oleic acid of the precursor solutions are found to affect the morphologies of the products significantly, and oleic acid plays a key role in the morphology-controlled synthesis of NaGd(MoO4)2 nanocrystals with diverse morphologies. Growth mechanism of NaGd(MoO4)2 nanocrystals is proposed based on time-dependent morphology evolution and X-ray diffraction analysis. Morphology-dependent down-shifting photoluminescence properties of NaGd(MoO4)2: Eu(3+) nanocrystals, and upconversion photoluminescence properties of NaGd(MoO4)2: Yb(3+)/Er(3+) and Yb(3+)/Tm(3+) nanoplates are investigated in detail. Charge transfer band in the down-shifting excitation spectra shows a slight blue-shift, and the luminescence intensities and lifetimes of Eu(3+) are decreased gradually with the morphology of the nanocrystals varying from nanocubes to thin square nanoplates. Upconversion energy transfer mechanisms of NaGd(MoO4)2: Yb(3+)/Er(3+), Yb(3+)/Tm(3+) nanoplates are proposed based on the energy level scheme and power dependence of upconversion emissions. Thermometric properties of NaGd(MoO4)2: Yb(3+)/Er(3+) nanoplates are investigated, and the maximum sensitivity is determined to be 0.01333 K(-1) at 285 K.

NaGd(MoO4)2 nanocrystals with diverse morphologies: controlled synthesis, growth mechanism, photoluminescence and thermometric properties

PubMed Central

Li, Anming; Xu, Dekang; Lin, Hao; Yang, Shenghong; Shao, Yuanzhi; Zhang, Yueli

2016-01-01

Pure tetragonal phase, uniform and well-crystallized sodium gadolinium molybdate (NaGd(MoO4)2) nanocrystals with diverse morphologies, e.g. nanocylinders, nanocubes and square nanoplates have been selectively synthesized via oleic acid-mediated hydrothermal method. The phase, structure, morphology and composition of the as-synthesized products are studied. Contents of both sodium molybdate and oleic acid of the precursor solutions are found to affect the morphologies of the products significantly, and oleic acid plays a key role in the morphology-controlled synthesis of NaGd(MoO4)2 nanocrystals with diverse morphologies. Growth mechanism of NaGd(MoO4)2 nanocrystals is proposed based on time-dependent morphology evolution and X-ray diffraction analysis. Morphology-dependent down-shifting photoluminescence properties of NaGd(MoO4)2: Eu3+ nanocrystals, and upconversion photoluminescence properties of NaGd(MoO4)2: Yb3+/Er3+ and Yb3+/Tm3+ nanoplates are investigated in detail. Charge transfer band in the down-shifting excitation spectra shows a slight blue-shift, and the luminescence intensities and lifetimes of Eu3+ are decreased gradually with the morphology of the nanocrystals varying from nanocubes to thin square nanoplates. Upconversion energy transfer mechanisms of NaGd(MoO4)2: Yb3+/Er3+, Yb3+/Tm3+ nanoplates are proposed based on the energy level scheme and power dependence of upconversion emissions. Thermometric properties of NaGd(MoO4)2: Yb3+/Er3+ nanoplates are investigated, and the maximum sensitivity is determined to be 0.01333 K−1 at 285 K. PMID:27506629

Fluorine-18-labeled Gd3+/Yb3+/Er3+ co-doped NaYF4 nanophosphors for multimodality PET/MR/UCL imaging.

PubMed

Zhou, Jing; Yu, Mengxiao; Sun, Yun; Zhang, Xianzhong; Zhu, Xingjun; Wu, Zhanhong; Wu, Dongmei; Li, Fuyou

2011-02-01

Molecular imaging modalities provide a wealth of information that is highly complementary and rarely redundant. To combine the advantages of molecular imaging techniques, (18)F-labeled Gd(3+)/Yb(3+)/Er(3+) co-doped NaYF(4) nanophosphors (NPs) simultaneously possessing with radioactivity, magnetic, and upconversion luminescent properties have been fabricated for multimodality positron emission tomography (PET), magnetic resonance imaging (MRI), and laser scanning upconversion luminescence (UCL) imaging. Hydrophilic citrate-capped NaY(0.2)Gd(0.6)Yb(0.18)Er(0.02)F(4) nanophosphors (cit-NPs) were obtained from hydrophobic oleic acid (OA)-coated nanoparticles (OA-NPs) through a process of ligand exchange of OA with citrate, and were found to be monodisperse with an average size of 22 × 19 nm. The obtained hexagonal cit-NPs show intense UCL emission in the visible region and paramagnetic longitudinal relaxivity (r(1) = 0.405 s(-1)·(mM)(-1)). Through a facile inorganic reaction based on the strong binding between Y(3+) and F(-), (18)F-labeled NPs have been fabricated in high yield. The use of cit-NPs as a multimodal probe has been further explored for T(1)-weighted MR and PET imaging in vivo and UCL imaging of living cells and tissue slides. The results indicate that (18)F-labeled NaY(0.2)Gd(0.6)Yb(0.18)Er(0.02) is a potential candidate as a multimodal nanoprobe for ultra-sensitive molecular imaging from the cellular scale to whole-body evaluation. Copyright © 2010 Elsevier Ltd. All rights reserved.

Controlled synthesis and luminescence properties of β-NaGdF4: Yb3+, Er3+ upconversion nanoparticles

NASA Astrophysics Data System (ADS)

Zhang, Yueli; Yao, Lu; Xu, Dekang; Lin, Hao; Yang, Shenghong

2018-06-01

β-NaGdF4:Yb3+,Er3+ upconversion (UC) nanoparticles (UCNPs) were prepared by a facile hydrothermal process with the assistance of sodium ethylene diaminetetraacetate salt (EDTA-2Na). The morphologies of the β-NaGdF4 UCNPs were controlled by changing the doses of EDTA-2Na and NaOH in precursor. With increasing concentration of EDTA-2Na in precursor, the size of crystals decreased, resulting in the decreasing of luminescence intensity. With increasing concentration of NaOH in precursor, the morphology became more homogeneous. However, due to the reduction of grain size and crystal quality, the luminescence intensity decreased. Nevertheless, the above results demonstrated a simple route to fabricate homogeneous UCNPs.

Coupling of Ag Nanoparticle with Inverse Opal Photonic Crystals as a Novel Strategy for Upconversion Emission Enhancement of NaYF4: Yb(3+), Er(3+) Nanoparticles.

PubMed

Shao, Bo; Yang, Zhengwen; Wang, Yida; Li, Jun; Yang, Jianzhi; Qiu, Jianbei; Song, Zhiguo

2015-11-18

Rare-earth-ion-doped upconversion (UC) nanoparticles have generated considerable interest because of their potential application in solar cells, biological labeling, therapeutics, and imaging. However, the applications of UC nanoparticles were still limited because of their low emission efficiency. Photonic crystals and noble metal nanoparticles are applied extensively to enhance the UC emission of rare earth ions. In the present work, a novel substrate consisting of inverse opal photonic crystals and Ag nanoparticles was prepared by the template-assisted method, which was used to enhance the UC emission of NaYF4: Yb(3+), Er(3+) nanoparticles. The red or green UC emissions of NaYF4: Yb(3+), Er(3+) nanoparticles were selectively enhanced on the inverse opal substrates because of the Bragg reflection of the photonic band gap. Additionally, the UC emission enhancement of NaYF4: Yb(3+), Er(3+) nanoparticles induced by the coupling of metal nanoparticle plasmons and photonic crystal effects was realized on the Ag nanoparticles included in the inverse opal substrate. The present results demonstrated that coupling of Ag nanoparticle with inverse opal photonic crystals provides a useful strategy to enhance UC emission of rare-earth-ion-doped nanoparticles.

Effect of Gallium and Indium Co-Substituting on Upconversion Properties of Er/Yb:Yttrium Aluminum Garnet Powders Prepared by the Co-Precipitation Method.

PubMed

Zhang, Wei; Liang, Yun-Ling; Hu, Zheng-Fa; Feng, Zu-Yong; Lun, Ma; Zhang, Xiu-ping; Sheng, Xia; Liu, Qian; Luo, Jie

2016-04-01

Gallium and Indium co-substituted Yb, Er:YAG was fabricated through the chemical co-precipitation method. The formation process and structure of the Ga3+ and In3+ substituted phosphor powders were characterized by the X-ray diffraction, thermo-gravimetry analyzer, infrared spectra, and X-ray photoelectron spectroscopy, and the effects of Ga3+ and In3+ concentration on the luminescence properties were investigated by spectrum. The results showed that the blue shift occurred after the substitution of Ga3+ and In3+ for Al3+ in matrix, and the intensity of emission spectrum was affected by the concentration of Ga3+ and In3+.

Tuning into single-band red upconversion luminescence in Yb(3+)/Ho(3+) activated nano-glass-ceramics through Ce(3+) doping.

PubMed

Chen, Daqin; Zhou, Yang; Wan, Zhongyi; Ji, Zhenguo; Huang, Ping

2015-03-28

Yb(3+)/Ho(3+) activated glass ceramics containing β-YF3 nanocrystals were successfully fabricated. The green ((5)S2/(5)F4→(5)I8) upconversion emission is dominant in the glass ceramics and is about 160 times stronger than that of the precursor glass, resulting from the partition of lanthanide activators into a low-phonon-energy crystalline lattice and the subsequent low probability of multi-phonon nonradiative relaxation from the (5)S2/(5)F4 and (5)I6 states to the lower ones. Upon the introduction of Ce(3+) ions into nano-glass-ceramics, two efficient cross-relaxation processes between Ho(3+) and Ce(3+), i.e., Ho(3+):(5)S2/(5)F4 + Ce(3+):(2)F5/2→Ho(3+):(5)F5 + Ce(3+):(2)F7/2 and Ho(3+):(5)I6 + Ce(3+):(2)F5/2→Ho(3+):(5)I7 + Ce(3+):(2)F7/2, are demonstrated to greatly suppress the population of the green-emitting (5)S2/(5)F4 state and to enhance the population of the red-emitting (5)F5 one, leading to the intense single-band red UC radiation of Ho(3+).

Synthesis and photoluminescence studies of Tm3+/Yb3+ codoped Y2O3 phosphors

NASA Astrophysics Data System (ADS)

Maurya, S. K.; Tiwari, S. P.; Kumar, A.; Kumar, K.

2018-05-01

Tm3+/Yb3+ codoped Y2O3 phosphor nanoparticles are synthesized by the solution combustion method using urea as a fuel regent. The nitrate of all rare earths RE(NO)3.6H2O (RE = Y, Tm and Yb) are used in a stoichiometric ratios to get the optimized emission intensities. The sample is further annealed at 900 °C for characterizations. The phase confirmation of synthesized samples is carried out by using XRD analysis. FESEM images are analyzed to confirm the shape and size of particles. The EDX image shows all elements are present in the sample. The agglomerated particles are monitored for annealed samples. The comparative studies in upconversion and downconversion behavior of annealed powder samples are monitored, consequently, the emission intensity is dominantly assigned at 464, 477 and 655 nm corresponding to 1D2→3F4, 1G4→3H6 and 1G4→3F4, respectively. The CIE coordinates of the recorded samples are calculated with different excitation wavelength and found to be invariant which exhibits the applicability of sample for display devices.

A cobalt oxyhydroxide-modified upconversion nanosystem for sensitive fluorescence sensing of ascorbic acid in human plasma

NASA Astrophysics Data System (ADS)

Cen, Yao; Tang, Jun; Kong, Xiang-Juan; Wu, Shuang; Yuan, Jing; Yu, Ru-Qin; Chu, Xia

2015-08-01

Ascorbic acid (AA), a potent antioxidant readily scavenging reactive species, is a crucial micronutrient involved in many biochemical processes. Here, we have developed a cobalt oxyhydroxide (CoOOH)-modified upconversion nanosystem for fluorescence sensing of AA activity in human plasma. The nanosystem consists of upconversion nanoparticles (UCNPs) NaYF4:30% Yb,0.5% Tm@NaYF4, which serve as energy donors, and CoOOH nanoflakes formed on the surface of UCNPs, which act as efficient energy acceptors. The fluorescence resonance energy transfer (FRET) process from the UCNPs to the absorbance of the CoOOH nanoflakes occurs in the nanosystem. The AA-mediated specific redox reaction reduces CoOOH into Co2+, leading to the inhibition of FRET, and resulting in the recovery of upconversion emission spectra. On the basis of these features, the nanosystem can be used for sensing AA activity with sensitivity and selectivity. Moreover, due to the minimizing background interference provided by UCNPs, the nanosystem has been applied to monitoring AA levels in human plasma sample with satisfactory results. The proposed approach may potentially provide an analytical platform for research and clinical diagnosis of AA related diseases.Ascorbic acid (AA), a potent antioxidant readily scavenging reactive species, is a crucial micronutrient involved in many biochemical processes. Here, we have developed a cobalt oxyhydroxide (CoOOH)-modified upconversion nanosystem for fluorescence sensing of AA activity in human plasma. The nanosystem consists of upconversion nanoparticles (UCNPs) NaYF4:30% Yb,0.5% Tm@NaYF4, which serve as energy donors, and CoOOH nanoflakes formed on the surface of UCNPs, which act as efficient energy acceptors. The fluorescence resonance energy transfer (FRET) process from the UCNPs to the absorbance of the CoOOH nanoflakes occurs in the nanosystem. The AA-mediated specific redox reaction reduces CoOOH into Co2+, leading to the inhibition of FRET, and resulting in the recovery of upconversion emission spectra. On the basis of these features, the nanosystem can be used for sensing AA activity with sensitivity and selectivity. Moreover, due to the minimizing background interference provided by UCNPs, the nanosystem has been applied to monitoring AA levels in human plasma sample with satisfactory results. The proposed approach may potentially provide an analytical platform for research and clinical diagnosis of AA related diseases. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr03588k

Investigation of mid-infrared emission characteristics and energy transfer dynamics in Er3+ doped oxyfluoride tellurite glass

PubMed Central

Chen, Fangze; Wei, Tao; Jing, Xufeng; Tian, Ying; Zhang, Junjie; Xu, Shiqing

2015-01-01

Er3+ doped oxyfluoride tellurite glasses have been prepared. Three Judd-Ofelt parameters Ωt (t = 2, 4, 6) and radiative properties are calculated for prepared glasses. Emission characteristics are analyzed and it is found that prepared glasses possess larger calculated predicted spontaneous transition probability (39.97 s−1), emission cross section σem (10.18 × 10−21 cm2) and σem × Δλeff (945.32 × 10−28 cm3), corresponding to the 2.7 μm emission of Er3+: 4I11/2→ 4I13/2 transition. The results suggest that the prepared glasses might be appropriate optical material for mid-infrared laser application. Moreover, rate equation analysis which is rarely used in bulk glass has been carried out to explain the relationship between emission intensity and Er3+ concentration. The calculation results show that with the increment of Er3+ concentration, the energy transfer up-conversion rate of 4I13/2 state increases while the rate of 4I11/2 state reduces, resulting in the change of 2.7 μm emission. PMID:26032900

Exploiting the benefit of S0 → T1 excitation in triplet-triplet annihilation upconversion to attain large anti-stokes shifts: tuning the triplet state lifetime of a tris(2,2'-bipyridine) osmium(ii) complex.

PubMed

Liu, Dongyi; Zhao, Yingjie; Wang, Zhijia; Xu, Kejing; Zhao, Jianzhang

2018-03-07

Os(ii) complexes are particularly interesting for triplet-triplet annihilation (TTA) upconversion, due to the strong direct S 0 → T 1 photoexcitation, as in this way, energy loss is minimized and large anti-Stokes shift can be achieved for TTA upconversion. However, Os(bpy) 3 has an intrinsic short T 1 state lifetime (56 ns), which is detrimental for the intermolecular triplet-triplet energy transfer (TTET), one of the crucial steps in TTA upconversion. In order to prolong the triplet state lifetime, we prepared an Os(ii) tris(bpy) complex with a Bodipy moiety attached, so that an extended T 1 state lifetime is achieved by excited state electronic configuration mixing or triplet state equilibrium between the coordination center-localized state ( 3 MLCT state) and Bodipy ligand-localized state ( 3 IL state). With steady-state and time-resolved transient absorption/emission spectroscopy, we proved that the 3 MLCT is slightly above the 3 IL state (by 0.05 eV), and the triplet state lifetime was prolonged by 31-fold (from 56 ns to 1.73 μs). The TTA upconversion quantum yield was increased by 4-fold as compared to that of the unsubstituted Os(ii) complex.

Luminescence of Er 3+-doped nanostructured SiO 2-LaF 3 glass-ceramics prepared by the sol-gel method

NASA Astrophysics Data System (ADS)

Rodríguez, V. D.; Del Castillo, J.; Yanes, A. C.; Méndez-Ramos, J.; Torres, M.; Peraza, J.

2007-07-01

Transparent glass ceramics with composition of 95SiO2-5LaF3 doped with 0.1 mol% of Er3+ were synthesized by thermal treatment of precursor sol-gel glasses. Segregated LaF3 nanocrystals in the glass were confirmed from a structural analysis performed by X-ray diffraction. Blue, green and red efficient up-conversion emissions were observed under 980 nm excitation at room temperature. Under this excitation near infrared down-conversion at 1.55 μm is also observed. These results could be attributed to the precipitation of LaF3 nanocrystals and the incorporation of most Er3+ ions in these nanocrystals. The mechanisms involved in the up-conversion emissions could be ascribed to two and three photon processes.

Optical parametric amplification and oscillation assisted by low-frequency stimulated emission.

PubMed

Longhi, Stefano

2016-04-15

Optical parametric amplification and oscillation provide powerful tools for coherent light generation in spectral regions inaccessible to lasers. Parametric gain is based on a frequency down-conversion process and, thus, it cannot be realized for signal waves at a frequency ω3 higher than the frequency of the pump wave ω1. In this Letter, we suggest a route toward the realization of upconversion optical parametric amplification and oscillation, i.e., amplification of the signal wave by a coherent pump wave of lower frequency, assisted by stimulated emission of the auxiliary idler wave. When the signal field is resonated in an optical cavity, parametric oscillation is obtained. Design parameters for the observation of upconversion optical parametric oscillation at λ3=465 nm are given for a periodically poled lithium-niobate (PPLN) crystal doped with Nd(3+) ions.

Amplified Photon Upconversion by Photonic Shell of Cholesteric Liquid Crystals.

PubMed

Kang, Ji-Hwan; Kim, Shin-Hyun; Fernandez-Nieves, Alberto; Reichmanis, Elsa

2017-04-26

As an effective platform to exploit triplet-triplet-annihilation-based photon upconversion (TTA-UC), microcapsules composed of a fluidic UC core and photonic shell are microfluidically prepared using a triple emulsion as the template. The photonic shell consists of cholesteric liquid crystals (CLCs) with a periodic helical structure, exhibiting a photonic band gap. Combined with planar anchoring at the boundaries, the shell serves as a resonance cavity for TTA-UC emission and enables spectral tuning of the UC under low-power-density excitation. The CLC shell can be stabilized by introducing a polymerizable mesogen in the LC host. Because of the microcapsule spherical symmetry, spontaneous emission of the delayed fluorescence is omnidirectionally amplified at the edge of the stop band. These results demonstrate the range of opportunities provided by TTA-UC systems for the future design of low-threshold photonic devices.

Synthesis, Structural Characterization and Up-Conversion Luminescence Properties of NaYF4:Er3+,Yb3+@MOFs Nanocomposites

NASA Astrophysics Data System (ADS)

Giang, Lam Thi Kieu; Marciniak, Lukasz; Huy, Tran Quang; Vu, Nguyen; Le, Ngo Thi Hong; Binh, Nguyen Thanh; Lam, Tran Dai; Minh, Le Quoc

2017-10-01

This paper describes a facile synthesis of NaYF4:Er3+,Yb3+ nanoparticles embraced in metal-organic frameworks (MOFs), known as NaYF4:Er3+, Yb3+@MOFs core/shell nanostructures, by using iron(III) carboxylate (MIL-100) and zeolitic imidazolate frameworks (ZIF-8). Morphological, structural and optical characterization of these nanostructures were investigated by field emission-scanning electron microscopy, Fourier transform infrared spectroscopy, x-ray diffraction, and up-conversion luminescence measurements. Results showed that spherical-shaped NaYF4:Er3+,Yb3+@MIL-100 nanocomposites with diameters of 150-250 nm, and rod-shaped NaYF4:Er3+,Yb3+@ZIF-8 nanocomposites with lengths of 300-550 nm, were successfully synthesized. Under a 980-nm laser excitation at room temperature, the NaYF4:Er3+,Yb3+@MOFs nanocomposites exhibited strong up-conversion luminescence with two emission bands in the green part of spectrum at 520 nm and 540 nm corresponding to the 2H11/2 → 4I15/2 and 4S3/2 → 4I15/2 transitions of Er3+ ions, respectively, and a red emission band at 655 nm corresponding to the 4F9/2 → 4I15/2 transition of Er3+ ions. The above properties of NaYF4:Er3+,Yb3+@MOFs make them promising candidates for applications in biotechnology.

Evaluation of the upconversion mechanisms in Ho3+-doped crystals: Experiment and theoretical modeling

NASA Astrophysics Data System (ADS)

Osiac, E.; Sokólska, I.; Kück, S.

2002-06-01

The paper compares the mechanisms that enable the upconverted green emission (5S2-->5I8) of the Ho3+ ion under infrared excitation (700-920 nm) in several crystalline hosts (YAlO3, YLiF4, Y3Sc2Ga3O12, and BaY2F8). Parameters involved in the upconversion such as excited-state absorption and cross-relaxation rates were determined from spectroscopic measurements. A system of differential equation (rate equations) was used to describe the upconversion mechanism and was numerically solved. The results were compared with experimental data. A reduction of this system to a three-level ``simplified system'' is presented, which includes only the ground level, the emitting level, and the intermediate level. The differences between the photon-avalanche mechanism and the looping mechanism are discussed and analyzed according to this simplified system.

Temperature dependence of the ratio of intensities of up-conversion fluorescence bands of YVO4 and YGdVO4 crystals and lead fluoride nano glass ceramics activated with erbium ions

NASA Astrophysics Data System (ADS)

Varaksa, Yu. A.; Sinitsyn, G. V.; Khodasevich, M. A.; Aseev, V. A.; Kolobkova, E. V.; Yasyukevich, A. S.

2015-01-01

Up-conversion fluorescence spectra of YVO4 and YGdVO4 crystals and lead fluoride nano glass ceramics coactivated with erbium and ytterbium ions have been studied in the wavelength range of 520-560 nm under 967-nm pumping. The ratio of intensities of fluorescence bands in the ranges of 520-530 and 540-550 nm has been measured in the temperature range of from room temperature to 150°C. It is shown that the considered materials can be used for preparing a sensing element of optical fluorescent temperature sensors; the sensitivity of measuring the temperature of nano glass-ceramics can be close to that of crystal samples.

A broadening temperature sensitivity range with a core-shell YbEr@YbNd double ratiometric optical nanothermometer

NASA Astrophysics Data System (ADS)

Marciniak, L.; Prorok, K.; Francés-Soriano, L.; Pérez-Prieto, J.; Bednarkiewicz, A.

2016-02-01

The chemical architecture of lanthanide doped core-shell up-converting nanoparticles can be engineered to purposely design the properties of luminescent nanomaterials, which are typically inaccessible to their homogeneous counterparts. Such an approach allowed to shift the up-conversion excitation wavelength from ~980 to the more relevant ~808 nm or enable Tb or Eu up-conversion emission, which was previously impossible to obtain or inefficient. Here, we address the issue of limited temperature sensitivity range of optical lanthanide based nano-thermometers. By covering Yb-Er co-doped core nanoparticles with the Yb-Nd co-doped shell, we have intentionally combined temperature dependent Er up-conversion together with temperature dependent Nd --> Yb energy transfer, and thus have expanded the temperature response range ΔT of a single nanoparticle based optical nano-thermometer under single ~808 nm wavelength photo-excitation from around ΔT = 150 K to over ΔT = 300 K (150-450 K). Such engineered nanocrystals are suitable for remote optical temperature measurements in technology and biotechnology at the sub-micron scale.The chemical architecture of lanthanide doped core-shell up-converting nanoparticles can be engineered to purposely design the properties of luminescent nanomaterials, which are typically inaccessible to their homogeneous counterparts. Such an approach allowed to shift the up-conversion excitation wavelength from ~980 to the more relevant ~808 nm or enable Tb or Eu up-conversion emission, which was previously impossible to obtain or inefficient. Here, we address the issue of limited temperature sensitivity range of optical lanthanide based nano-thermometers. By covering Yb-Er co-doped core nanoparticles with the Yb-Nd co-doped shell, we have intentionally combined temperature dependent Er up-conversion together with temperature dependent Nd --> Yb energy transfer, and thus have expanded the temperature response range ΔT of a single nanoparticle based optical nano-thermometer under single ~808 nm wavelength photo-excitation from around ΔT = 150 K to over ΔT = 300 K (150-450 K). Such engineered nanocrystals are suitable for remote optical temperature measurements in technology and biotechnology at the sub-micron scale. Electronic supplementary information (ESI) available: Characterization, structural and morphological characterization of nanocrystals, the measurement setup. See DOI: 10.1039/c5nr08223d

Synthesis of Multicolor Core/Shell NaLuF4:Yb3+/Ln3+@CaF2 Upconversion Nanocrystals

PubMed Central

Li, Hui; Hao, Shuwei; Yang, Chunhui; Chen, Guanying

2017-01-01

The ability to synthesize high-quality hierarchical core/shell nanocrystals from an efficient host lattice is important to realize efficacious photon upconversion for applications ranging from bioimaging to solar cells. Here, we describe a strategy to fabricate multicolor core @ shell α-NaLuF4:Yb3+/Ln3+@CaF2 (Ln = Er, Ho, Tm) upconversion nanocrystals (UCNCs) based on the newly established host lattice of sodium lutetium fluoride (NaLuF4). We exploited the liquid-solid-solution method to synthesize the NaLuF4 core of pure cubic phase and the thermal decomposition approach to expitaxially grow the calcium fluoride (CaF2) shell onto the core UCNCs, yielding cubic core/shell nanocrystals with a size of 15.6 ± 1.2 nm (the core ~9 ± 0.9 nm, the shell ~3.3 ± 0.3 nm). We showed that those core/shell UCNCs could emit activator-defined multicolor emissions up to about 772 times more efficient than the core nanocrystals due to effective suppression of surface-related quenching effects. Our results provide a new paradigm on heterogeneous core/shell structure for enhanced multicolor upconversion photoluminescence from colloidal nanocrystals. PMID:28336867

Fabrication and evaluation of chitosan/NaYF4:Yb3+/Tm3+ upconversion nanoparticles composite beads based on the gelling of Pickering emulsion droplets.

PubMed

Yan, Huiqiong; Chen, Xiuqiong; Shi, Jia; Shi, Zaifeng; Sun, Wei; Lin, Qiang; Wang, Xianghui; Dai, Zihao

2017-02-01

The rare earth ion doped upconversion nanoparticles (UCNPs) synthesized by hydrophobic organic ligands possess poor solubility and low fluorescence quantum yield in aqueous media. To conquer this issue, NaYF 4 :Yb 3+ /Tm 3+ UCNPs, synthesized by a hydrothermal method, were coated with F127 and then assembled with chitosan to fabricate the chitosan/NaYF 4 :Yb 3+ /Tm 3+ composite beads (CS/NaYF 4 :Yb 3+ /Tm 3+ CBs) by Pickering emulsion system. The characterization results revealed that the as-synthesized NaYF 4 :Yb 3+ /Tm 3+ UCNPs with an average size of 20nm exhibited spherical morphology, high crystallinity and characteristic emission upconversion fluorescence with an overall blue color output. The NaYF 4 :Yb 3+ /Tm 3+ UCNPs were successfully conjugated on the surface of chitosan beads by the gelling of emulsion droplets. The resultant CS/NaYF 4 :Yb 3+ /Tm 3+ CBs showed good upconversion luminescent property, drug-loading capacity, release performance and excellent biocompatibility, exhibiting great potentials in targeted drug delivery and tissue engineering with potential tracking capability and lasting release performance. Copyright © 2016 Elsevier B.V. All rights reserved.

NIR Ratiometric Luminescence Detection of pH Fluctuation in Living Cells with Hemicyanine Derivative-Assembled Upconversion Nanophosphors.

PubMed

Li, Haixia; Dong, Hao; Yu, Mingming; Liu, Chunxia; Li, Zhanxian; Wei, Liuhe; Sun, Ling-Dong; Zhang, Hongyan

2017-09-05

It is crucial for cell physiology to keep the homeostasis of pH, and it is highly demanded yet challenging to develop luminescence resonance energy transfer (LRET)-based near-infrared (NIR) ratiometric luminescent sensor for the detection of pH fluctuation with NIR excitation. As promising energy donors for LRET, upconversion nanoparticles (UCNPs) have been widely used to fabricate nanosensors, but the relatively low LRET efficiency limits their application in bioassay. To improve the LRET efficiency, core/shell/shell structured β-NaGdF 4 @NaYF 4 :Yb,Tm@NaYF 4 UCNPs were prepared and decorated with hemicyanine dyes as an LRET-based NIR ratiometric luminescent pH fluctuation-nanosensor for the first time. The as-developed nanosensor not only exhibits good antidisturbance ability, but it also can reversibly sense pH and linearly sense pH in a range of 6.0-9.0 and 6.8-9.0 from absorption and upconversion emission spectra, respectively. In addition, the nanosensor displays low dark toxicity under physiological temperature, indicating good biocompatibility. Furthermore, live cell imaging results revealed that the sensor can selectively monitor pH fluctuation via ratiometric upconversion luminescence behavior.

Excitonic luminescence upconversion in a two-dimensional semiconductor

DOE PAGES

Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; ...

2015-12-21

Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). We demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors(4). Since the charged exciton binding energy(5) closelymore » matches the 31 meV A(1)' optical phonon(6-9), we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. Additionally, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.« less

Capacitively Coupled Plasma Discharge of Ionic Liquid Solutions to Synthesize Carbon Dots as Fluorescent Sensors.

PubMed

Ke, Ching-Bin; Lu, Te-Ling; Chen, Jian-Lian

2018-05-26

Oxygen and nitrogen capacitively coupled plasma (CCP) was used to irradiate mixtures of aliphatic acids in high boiling point solvents to synthesize fluorescent carbon dots (C-dots). With a high fluorescence intensity, the C-dots obtained from the O₂/CCP radiation of a 1-ethyl-3-methylimidazolium dicyanamide ionic liquid solution of citric acid were characterized with an average diameter of 8.6 nm (σ = 1.1 nm), nitrogen and oxygen bonding functionalities, excitation-independent emissions, and upconversion fluorescence. Through dialysis of the CCP-treated C-dots, two emissive surface states corresponding to their respective functionalities and emissions were identified. The fluorescence spectrum of the CCP-treated C-dots was different from that of the microwave irradiation and possessed higher intensity than that of hydrothermal pyrolysis. By evaluation of the fluorescence quenching effect on flavonoids and metal ions, the CCP-treated C-dots showed a high selectivity for quercetin and sensitivity to Hg 2+ . Based on the Perrin model, a calibration curve ( R ² = 0.9992) was established for quercetin ranging from 2.4 μM to 119 μM with an LOD (limit of detection) = 0.5 μM. The quercetin in the ethanol extract of the sun-dried peel of Citrus reticulata cv. Chachiensis was determined by a standard addition method to be 4.20 ± 0.15 mg/g with a matrix effect of 8.16%.

Size-tunable and monodisperse Tm³⁺/Gd³⁺-doped hexagonal NaYbF₄ nanoparticles with engineered efficient near infrared-to-near infrared upconversion for in vivo imaging.

PubMed

Damasco, Jossana A; Chen, Guanying; Shao, Wei; Ågren, Hans; Huang, Haoyuan; Song, Wentao; Lovell, Jonathan F; Prasad, Paras N

2014-08-27

Hexagonal NaYbF4:Tm(3+) upconversion nanoparticles hold promise for use in high contrast near-infrared-to-near-infrared (NIR-to-NIR) in vitro and in vivo bioimaging. However, significant hurdles remain in their preparation and control of their morphology and size, as well as in enhancement of their upconversion efficiency. Here, we describe a systematic approach to produce highly controlled hexagonal NaYbF4:Tm(3+) nanoparticles with superior upconversion. We found that doping appropriate concentrations of trivalent gadolinium (Gd(3+)) can convert NaYbF4:Tm(3+) 0.5% nanoparticles with cubic phase and irregular shape into highly monodisperse NaYbF4:Tm(3+) 0.5% nanoplates or nanospheres in a pure hexagonal-phase and of tunable size. The intensity and the lifetime of the upconverted NIR luminescence at 800 nm exhibit a direct dependence on the size distribution of the resulting nanoparticles, being ascribed to the varied surface-to-volume ratios determined by the different nanoparticle size. Epitaxial growth of a thin NaYF4 shell layer of ∼2 nm on the ∼22 nm core of hexagonal NaYbF4:Gd(3+) 30%/Tm(3+) 0.5% nanoparticles resulted in a dramatic 350 fold NIR upconversion efficiency enhancement, because of effective suppression of surface-related quenching mechanisms. In vivo NIR-to-NIR upconversion imaging was demonstrated using a dispersion of phospholipid-polyethylene glycol (DSPE-PEG)-coated core/shell nanoparticles in phosphate buffered saline.

Size-Tunable and Monodisperse Tm3+/Gd3+-Doped Hexagonal NaYbF4 Nanoparticles with Engineered Efficient Near Infrared-to-Near Infrared Upconversion for In Vivo Imaging

PubMed Central

2015-01-01

Hexagonal NaYbF4:Tm3+ upconversion nanoparticles hold promise for use in high contrast near-infrared-to-near-infrared (NIR-to-NIR) in vitro and in vivo bioimaging. However, significant hurdles remain in their preparation and control of their morphology and size, as well as in enhancement of their upconversion efficiency. Here, we describe a systematic approach to produce highly controlled hexagonal NaYbF4:Tm3+ nanoparticles with superior upconversion. We found that doping appropriate concentrations of trivalent gadolinium (Gd3+) can convert NaYbF4:Tm3+ 0.5% nanoparticles with cubic phase and irregular shape into highly monodisperse NaYbF4:Tm3+ 0.5% nanoplates or nanospheres in a pure hexagonal-phase and of tunable size. The intensity and the lifetime of the upconverted NIR luminescence at 800 nm exhibit a direct dependence on the size distribution of the resulting nanoparticles, being ascribed to the varied surface-to-volume ratios determined by the different nanoparticle size. Epitaxial growth of a thin NaYF4 shell layer of ∼2 nm on the ∼22 nm core of hexagonal NaYbF4:Gd3+ 30%/Tm3+ 0.5% nanoparticles resulted in a dramatic 350 fold NIR upconversion efficiency enhancement, because of effective suppression of surface-related quenching mechanisms. In vivo NIR-to-NIR upconversion imaging was demonstrated using a dispersion of phospholipid-polyethylene glycol (DSPE-PEG)-coated core/shell nanoparticles in phosphate buffered saline. PMID:25027118

Excited-state absorption and fluorescence dynamics of Er3+:KY3F10

NASA Astrophysics Data System (ADS)

Labbé, C.; Doualan, J. L.; Moncorgé, R.; Braud, A.; Camy, P.

2018-05-01

We report here on a complete investigation of the excited-state absorption and fluorescence dynamics of Er3+ doped KY3F10 single crystals versus dopant concentrations and optical excitation conditions. Radiative and effective (including non-radiative relaxations) emission lifetimes and branching ratios are determined from a Judd-Ofelt analysis of the absorption spectra and via specific fluorescence experiments using wavelength selective laser excitations. Excited-state absorption and emission spectra are registered within seven spectral domains, i.e. 560 nm, 650 nm, 710 nm, 810 nm, 970 nm, 1550 nm and 2750 nm. A maximum gain cross-section of 0.93 × 10-21 cm2 is determined at the potential laser wavelength of 2.801 μm for a population ratio of 0.48. Saturation of fluorescence intensities and variations of population ratios versus pumping rates are registered and confronted with a rate equation model to derive the rates of the most important up-conversion and cross-relaxation energy transfers occurring at high dopant concentrations.

Multispectral Emissions of Lanthanide-Doped Gadolinium Oxide Nanophosphors for Cathodoluminescence and Near-Infrared Upconversion/Downconversion Imaging

PubMed Central

Thi Kim Dung, Doan; Fukushima, Shoichiro; Furukawa, Taichi; Niioka, Hirohiko; Sannomiya, Takumi; Kobayashi, Kaori; Yukawa, Hiroshi; Baba, Yoshinobu; Hashimoto, Mamoru; Miyake, Jun

2016-01-01

Comprehensive imaging of a biological individual can be achieved by utilizing the variation in spatial resolution, the scale of cathodoluminescence (CL), and near-infrared (NIR), as favored by imaging probe Gd2O3 co-doped lanthanide nanophosphors (NPPs). A series of Gd2O3:Ln3+/Yb3+ (Ln3+: Tm3+, Ho3+, Er3+) NPPs with multispectral emission are prepared by the sol-gel method. The NPPs show a wide range of emissions spanning from the visible to the NIR region under 980 nm excitation. The dependence of the upconverting (UC)/downconverting (DC) emission intensity on the dopant ratio is investigated. The optimum ratios of dopants obtained for emissions in the NIR regions at 810 nm, 1200 nm, and 1530 nm are applied to produce nanoparticles by the homogeneous precipitation (HP) method. The nanoparticles produced from the HP method are used to investigate the dual NIR and CL imaging modalities. The results indicate the possibility of using Gd2O3 co-doped Ln3+/Yb3+ (Ln3+: Tm3+, Ho3+, Er3+) in correlation with NIR and CL imaging. The use of Gd2O3 promises an extension of the object dimension to the whole-body level by employing magnetic resonance imaging (MRI). PMID:28335291

Multispectral Emissions of Lanthanide-Doped Gadolinium Oxide Nanophosphors for Cathodoluminescence and Near-Infrared Upconversion/Downconversion Imaging.

PubMed

Thi Kim Dung, Doan; Fukushima, Shoichiro; Furukawa, Taichi; Niioka, Hirohiko; Sannomiya, Takumi; Kobayashi, Kaori; Yukawa, Hiroshi; Baba, Yoshinobu; Hashimoto, Mamoru; Miyake, Jun

2016-09-06

Comprehensive imaging of a biological individual can be achieved by utilizing the variation in spatial resolution, the scale of cathodoluminescence (CL), and near-infrared (NIR), as favored by imaging probe Gd₂O₃ co-doped lanthanide nanophosphors (NPPs). A series of Gd₂O₃:Ln 3+ /Yb 3+ (Ln 3+ : Tm 3+ , Ho 3+ , Er 3+ ) NPPs with multispectral emission are prepared by the sol-gel method. The NPPs show a wide range of emissions spanning from the visible to the NIR region under 980 nm excitation. The dependence of the upconverting (UC)/downconverting (DC) emission intensity on the dopant ratio is investigated. The optimum ratios of dopants obtained for emissions in the NIR regions at 810 nm, 1200 nm, and 1530 nm are applied to produce nanoparticles by the homogeneous precipitation (HP) method. The nanoparticles produced from the HP method are used to investigate the dual NIR and CL imaging modalities. The results indicate the possibility of using Gd₂O₃ co-doped Ln 3+ /Yb 3+ (Ln 3+ : Tm 3+ , Ho 3+ , Er 3+ ) in correlation with NIR and CL imaging. The use of Gd₂O₃ promises an extension of the object dimension to the whole-body level by employing magnetic resonance imaging (MRI).

Highly efficient green up-conversion luminescence of Nd3+-Yb3+-Ho3+ codoped fluorite-type nanocrystals in transparent glass ceramics

NASA Astrophysics Data System (ADS)

Qiu, Jianbei; Kawamoto, Yoji; Zhang, Junjie

2002-11-01

Oxyfluoride glasses were developed with composition 30SiO2[middle dot]15AlO1.5[middle dot]28PbF2[middle dot]22CdF2[middle dot](4.8-x)GdF3[middle dot]0.1NdF3[middle dot]0.1HoF3[middle dot]xYbF3 (x=0, 0.1, 0.2, 0.5, 1, 2, 3, 4, and 4.8) in mole percent. Powder x-ray diffraction analysis revealed that the heat treatments of the oxyfluoride glasses at 450 degC for 0.5 h cause the precipitation of Nd3+-Yb3+-Ho3+ codoped fluorite-type nanocrystals of about 16.3 nm in diameter in the glass matrix. These transparent glass ceramics exhibited very strong green up-conversion luminescence due to the Ho3+: (5F4, 5S2)[right arrow]5I8 transition under 800 nm excitation. The intensity of the green up-conversion luminescence in a 1 mol % YbF3-containing glass ceramic was found to be about 120 times stronger than that in the precursor oxyfluoride glass. The reason for the highly efficient Ho3+ up-conversion luminescence in the oxyfluoride glass ceramics is discussed. An up-conversion mechanism is also proposed.

Upconversion-pumped luminescence efficiency of rare-earth-doped hosts sensitized with trivalent ytterbium

DOE Office of Scientific and Technical Information (OSTI.GOV)

Page, R.H.; Schaffers, K.I.; Waide, P.A.

We discuss the upconversion luminescence efficiencies of phosphors that generate red, green, and blue light. The phosphors studied are single crystals and powders co-doped with Er{sup 3+} and Yb{sup 3+}, and with Tm{sup 3+} and Yb{sup 3+}. The Yb ions are pumped near 980 nm; transfers of two or three quanta to the co-doped rare earth ion generate visible luminescence. The main contribution embodied in this work is the quantitative measurement of this upconversion efficiency, based on the use of a calibrated integrating sphere, determination of the fraction of pump light absorbed, and careful control of the pump laser beammore » profile. The green phosphors are the most efficient, yielding efficiency values as high as 4 %, with the red and blue materials giving 1 - 2 %. Saturation was observed in all cases, suggesting that populations of upconversion steps of the ions are maximized at higher power. Quasi-CW modeling of the intensity- dependent upconversion efficiency was attempted; input data included level lifetimes, transition cross sections, and cross-relaxation rate coefficients. The saturation of the Yb,Er:fluoride media is explained as the pumping of Er{sup 3+} ions into a bottleneck (long-lived state)- the {sup 4}I{sub 13/2} metastable level, making them unavailable for further excitation transfer. 32 refs., 5 figs., 3 tabs.« less

Monitoring Delamination of Thermal Barrier Coatings During Interrupted High-Heat-Flux Laser Testing using Luminescence Imaging

NASA Technical Reports Server (NTRS)

Eldridge, Jeffrey I.; Zhu, Dongming; Wolfe, Douglas E.

2011-01-01

This presentation showed progress made in extending luminescence-base delamination monitoring to TBCs exposed to high heat fluxes, which is an environment that much better simulates actual turbine engine conditions. This was done by performing upconversion luminescence imaging during interruptions in laser testing, where a high-power CO2 laser was employed to create the desired heat flux. Upconverison luminescence refers to luminescence where the emission is at a higher energy (shorter wavelength) than the excitation. Since there will be negligible background emission at higher energies than the excitation, this methods produces superb contrast. Delamination contrast is produced because both the excitation and emission wavelengths are reflected at delamination cracks so that substantially higher luminescence intensity is observed in regions containing delamination cracks. Erbium was selected as the dopant for luminescence specifically because it exhibits upconversion luminescence. The high power CO2 10.6 micron wavelength laser facility at NASA GRC was used to produce the heat flux in combination with forced air backside cooling. Testing was performed at a lower (95 W/sq cm) and higher (125 W/sq cm) heat flux as well as furnace cycling at 1163C for comparison. The lower heat flux showed the same general behavior as furnace cycling, a gradual, "spotty" increase in luminescence associated with debond progression; however, a significant difference was a pronounced incubation period followed by acceleration delamination progression. These results indicate that extrapolating behavior from furnace cycling measurements will grossly overestimate remaining life under high heat flux conditions. The higher heat flux results were not only accelerated, but much different in character. Extreme bond coat rumpling occurred, and delamination propagation extended over much larger areas before precipitating macroscopic TBC failure. This indicates that under the higher heat flux (and surface & interface temperatures), the TBC was more tolerant of damage. The main conclusions were that high heat flux conditions can not only accelerate TBC debond progression but can also grossly alter the pathway of delamination.

Luminescence properties of Tm3+ ions single-doped YF3 materials in an unconventional excitation region.

PubMed

Chen, Yuan; Liu, Qing; Lin, Han; Yan, Xiaohong

2018-05-01

According to the spectral distribution of solar radiation at the earth's surface, under the excitation region of 1150 to 1350 nm, the up-conversion luminescence of Tm 3+ ions was investigated. The emission bands were matched well with the spectral response region of silicon solar cells, achieved by Tm 3+ ions single-doped yttrium fluoride (YF 3 ) phosphor, which was different from the conventional Tm 3+ /Yb 3+ ion couple co-doped materials. Additionally, the similar emission bands of Tm 3+ ions were achieved under excitation in the ultraviolet region. It is expected that via up-conversion and down-conversion routes, Tm 3+ -sensitized materials could convert photons to the desired wavelengths in order to reduce the energy loss of silicon solar cells, thereby enhancing the photovoltaic efficiency. Copyright © 2018 John Wiley & Sons, Ltd.

Laser characteristics at 1535 nm and thermal effects of an Er:Yb phosphate glass microchip pumped by Ti:sapphire laser

NASA Astrophysics Data System (ADS)

Cai, Zhiping; Chardon, Alain; Xu, Huiying; Féron, Patrice; Michel Stéphan, Guy

2002-03-01

An Er:Yb codoped phosphate glass microchip laser has been studied under pumping with a Ti:sapphire laser ranging from 945 to 990 nm. The characteristics (threshold, slope efficiency) are first described for an optimized laser. The gain spectrum is calculated for the transition 4I13/2→ 4I15/2 around 1535 nm from fundamental spectroscopic data and from experimental results. Red-shift effect on the frequency of a single mode is experimentally observed when the pump power is increased, originating from thermal effects. Temperature inside the microchip cavity and thermal expansion coefficient were determined by employing the intensity ratio of two green upconversion emission line centered at 530 and 554 nm, respectively, which quantitatively explain this red shift.

[Preparation and photoluminescence study of Er3+ : Y2O3 transparent ceramics].

PubMed

Luo, Jun-ming; Li, Yong-xiu; Deng, Li-ping

2008-10-01

Y2O3 acted as the matrix material, which was doped with different concentrations of Er3+, Er3+ : Y2O3 nanocrystalline powder was prepared by co-precipitation method, and Er3+ : Y2O3 transparent ceramics was fabricated by vacuum sintering at 1700 degrees C, 1 x 10(-3) Pa for 8 h. By using the X-ray diffraction (D/MAX-RB), transmission electron microscopy(Philips EM420), automatic logging spectrophotometer(DMR-22), fluorescence analyzer (F-4500) and 980 nm diode laser, the structural, morphological and luminescence properties of the sample were investigated. The results show that Er3+ dissolved completely in the Y2O3 cubic phase, the precursor was amorphous, weak diffraction peaks appeared after calcination at 400 degrees C, and if calcined at 700 degrees C, the precursor turned to pure cubic phase. With increasing the calcining temperature, the diffraction peaks became sharp quickly, and when the calcining temperature reached 1100 degrees C, the diffraction peaks became very sharp, indicating that the grains were very large. The particles of Er+ : Y2O3 is homogeneous and nearly spherical, the average diameter of the particles is in the range of 40-60 nm after being calcined at 1000 degrees C for 2 h. The relative density of Er3+ : Y2O3 transparent ceramics is 99.8%, the transmittance of the Er2+ : Y2O3 transparent ceramics is markedly lower than the single crystal at the short wavelength, but the transmittance is improved noticeably with increasing the wavelength, and the transmittance exceeds 60% at the wavelength of 1200 nm. Excited under the 980 nm diode laser, there are two main up-conversion emission bands, green emission centers at 562 nm and red emission centers at 660 nm, which correspond to (4)S(3/2) / (2)H(11/2) - (4)I(15/2) and (4)F(9/2) - (4)I(15/2) radiative transitions respectively. By changing the doping concentrations of Er3+, the color of up-conversion luminescence can be tuned from green to red gradually. The luminescence intensity is not reinforce with the increase in the concentration, so the doping concentration of Er3+ should not exceed 2%. If the doping concentration of Er3+ exceeds the range, the concentration has very small effect on the improvement of luminescence intensity.

Strain-sensitive upconversion for imaging biological forces (Conference Presentation)

NASA Astrophysics Data System (ADS)

Lay, Alice; Wisser, Michael; Lin, Yu; Narayan, Tarun; Krieg, Michael; Atre, Ashwin; Goodman, Miriam; Dionne, Jennifer A.

2016-09-01

Nearly all diseases can be traced back to abnormal mechanotransduction, but few sensors can reliably measure biologically-relevant forces in vivo. Here, we investigate sub-25nm lanthanide-doped upconverting nanoparticles as novel optical force probes, which provide several biocompatible features: sharp emission peaks with near infrared illumination, a high signal-to-noise ratio, and photostability. To increase force sensitivity, we include d-metal doping in the nanoparticles; the d-metal siphons energy from the lanthanide ions with an efficiency that varies with pressure. We synthesize cubic-phase NaYF4: Er3+,Yb3+ nanoparticles doped with 0-5% Mn2+ and compress them in a hydrostatic environment using a diamond anvil cell. When illuminated at 980nm, the nanoparticles show sharp emission peaks centered at wavelengths of 522nm, 545nm, and 660nm. In 20nN increments, up to 700nN, the ratio of the red-to-green peaks in 0% Mn-doped nanoparticles increases by nearly 30%, resulting in a perceived color change from orange to red. In contrast, the 1% Mn-doped samples exhibit little color change but a large 40% decrease in upconversion intensity. In both cases, the red-to-green ratio varies linearly with strain and the optical properties are recoverable upon release. We further use atomic force microscopy to characterize optical responses at lower, pico-Newton to nano-Newton forces. To demonstrate in vivo imaging capabilities, we incubate C. elegans with nanoparticles dispersed in buffer solution (5mg/mL concentration) and image forces involved in digestion using confocal microscopy. Our nanoparticles provide a platform for the first, non-genetically-encoded in vivo force sensors, and we describe routes to increase their sensitivity to the single-pN range.

Fabrication and Luminescence Characterization of a Silica Nanomatrix Embedded with NaYF4:Yb:Er:Tm@NaGdF4/Fe3O4 Nanoparticles

NASA Astrophysics Data System (ADS)

Thangaraju, Dheivasigamani; Santhana, Vedi; Matsuda, Satoshi; Hayakawa, Yasuhiro

2018-05-01

Hexagonal NaYF4:Yb:Er:Tm@NaGdF4 core-shell nanocrystals were synthesized using a seed mediated hot injection method, and monodispersed Fe3O4 (4 nm) nanoparticles were prepared from iron(II) actylacetonate by a precursor thermal decomposition method. Structural and morphology verified NaYF4:Yb:Er:Tm@NaGdF4 and Fe3O4 nanoparticles were utilized for the preparation of NaYF4:Yb:Er:Tm@NaGdF4/Fe3O4@SiO2 nanocomposite using a micro-emulsion method. Existence of Fe3O4 in NaYF4:Yb:Er:Tm@NaGdF4 in SiO2 nano-spheres were confirmed with transmission electron microscopy. Luminescence measurement revealed that NaYF4:Yb:Er:Tm@NaGdF4 exhibited strong emissions at green and red regions, in addition to a weak blue emission also observed under 980 nm excitation. Up-conversion emission of the nanoparticle-embedded silica nanocomposite showed that the up-conversion emission was not affected by Fe3O4 nanoparticles.

Spectroscopic investigation of zinc tellurite glasses doped with Yb(3+) and Er(3+) ions.

PubMed

Bilir, Gökhan; Kaya, Ayfer; Cinkaya, Hatun; Eryürek, Gönül

2016-08-05

This paper presents a detailed spectroscopic investigation of zinc tellurite glasses with the compositions (0.80-x-y) TeO2+(0.20) ZnO+xEr2O3+yYb2O3 (x=0, y=0; x=0.004, y=0; x=0, y=0.05 and x=0.004, y=0.05 per moles). The samples were synthesized by the conventional melt quenching method. The optical absorption and emission measurements were conducted at room temperature to determine the spectral properties of lanthanides doped zinc tellurite glasses and, to study the energy transfer processes between dopant lanthanide ions. The band gap energies for both direct and indirect possible transitions and the Urbach energies were measured from the absorption spectra. The absorption spectra of the samples were analyzed by using the Judd-Ofelt approach. The effect of the ytterbium ions on the emission properties of erbium ions was investigated and the energy transfer processes between dopant ions were studied by measuring the up-conversion emission properties of the materials. The color quality parameters of obtained visible up-conversion emission were also determined as well as possibility of using the Er(3+) glasses as erbium doped fiber amplifiers at 1.55μm in infrared emission region. Copyright © 2016 Elsevier B.V. All rights reserved.

Spectroscopic investigation of zinc tellurite glasses doped with Yb3 + and Er3 + ions

NASA Astrophysics Data System (ADS)

Bilir, Gökhan; Kaya, Ayfer; Cinkaya, Hatun; Eryürek, Gönül

2016-08-01

This paper presents a detailed spectroscopic investigation of zinc tellurite glasses with the compositions (0.80 - x - y) TeO2 + (0.20) ZnO + xEr2O3 + yYb2O3 (x = 0, y = 0; x = 0.004, y = 0; x = 0, y = 0.05 and x = 0.004, y = 0.05 per moles). The samples were synthesized by the conventional melt quenching method. The optical absorption and emission measurements were conducted at room temperature to determine the spectral properties of lanthanides doped zinc tellurite glasses and, to study the energy transfer processes between dopant lanthanide ions. The band gap energies for both direct and indirect possible transitions and the Urbach energies were measured from the absorption spectra. The absorption spectra of the samples were analyzed by using the Judd-Ofelt approach. The effect of the ytterbium ions on the emission properties of erbium ions was investigated and the energy transfer processes between dopant ions were studied by measuring the up-conversion emission properties of the materials. The color quality parameters of obtained visible up-conversion emission were also determined as well as possibility of using the Er3 + glasses as erbium doped fiber amplifiers at 1.55 μm in infrared emission region.

Enhanced infrared-to-visible up-conversion emission and temperature sensitivity in (Er3+,Yb3+, and W6+) tri-doped Bi4Ti3O12 ferroelectric oxide

NASA Astrophysics Data System (ADS)

Bokolia, Renuka; Mondal, Manisha; Rai, V. K.; Sreenivas, K.

2017-02-01

Strong up conversion (UC) luminescence at 527, 550, and 662 nm is compared under an excitation of 980 nm in single doped (Er3+), co-doped (Er3+/Yb3+), and (Er3+/Yb3+/W6+) tri-doped bismuth titanate (Bi4Ti3O12). For the co-doped system, the frequency (UC) emission intensity due to Er3+ ions is enhanced significantly in the green bands due to the efficient energy transfer from Yb3+ to Er3+ ions. Further increase in the emission intensity is seen with non-luminescent W6+ ions in the tri-doped system due to the modification in the local crystal field around the Er3+ ions, and is evidenced through a gradual change in the crystal structure of the host lattice with increasing W6+ content. The observed changes in the fluorescence lifetime and the associated energy transfer mechanisms are discussed. A progressive reduction of the lifetime of the 4S3/2 levels of Er3+ ions from 72 to 58.7 μs with the introduction of Yb3+ and W6+ dopant increases the transition probability and enhances the UC emission intensity. The efficiency of the energy transfer process ( η ) in the co-doped and tri-doped systems is found to be 9.4% and 18.6%, respectively, in comparison to the single doped system. Temperature sensing based on the fluorescence intensity ratio (FR) technique shows high sensitivity (0.0123 K-1) in the high temperature range (293 to 523 K) for an optimum content of Er3+, Yb3+, and W6+ with x = 0.03, y = 0.18, and z = 0.06 at. % in the tri-doped Bi4-x-yErxYbyTi3-zWzO12 ferroelectric composition, and is found useful for potential applications in optical thermometry.

A theory of Jovian decameter radiation

NASA Technical Reports Server (NTRS)

Goldstein, M. L.; Sharma, R. R.; Papadopoulos, K.; Ben-Ari, M.; Eviatar, A.

1983-01-01

A theory of the Jovian decameter radiation is presented based on the assumed existence of beams of energetic electrons in the inner Jovian magnetosphere. Beam-like electron distributions are shown to be unstable to the growth of both upper hybrid and lower hybrid electrostatic waves. The upconversion of these waves to fast extraordinary mode electromagnetic radiation is calculated by using a fluid model. Two possibilities are considered. First, a random phase approximation is made which leads to a very conservative estimate of intensity that can be expected in decameter radiation. The alternative possibility is also considered, viz, that the upconversion process is coherent. A comparison of both processes suggests that an incoherent interaction may be adequate to account for the observed intensity of decametric radiation, except perhaps near the peak of the spectrum (8 MHz). The coherent process is intrinsically more efficient and can easily produce the observed intensity near 8 MHz if only 0.01% of the energy in the beam is converted to electrostatic energy.

Long-lived room-temperature deep-red-emissive intraligand triplet excited state of naphthalimide in cyclometalated Ir(III) complexes and its application in triplet-triplet annihilation-based upconversion.

PubMed

Sun, Jifu; Wu, Wanhua; Zhao, Jianzhang

2012-06-25

Cyclometalated Ir(III) complexes with acetylide ppy and bpy ligands were prepared (ppy = 2-phenylpyridine, bpy = 2,2'-bipyridine) in which naphthal (Ir-2) and naphthalimide (NI) were attached onto the ppy (Ir-3) and bpy ligands (Ir-4) through acetylide bonds. [Ir(ppy)(3)] (Ir-1) was also prepared as a model complex. Room-temperature phosphorescence was observed for the complexes; both neutral and cationic complexes Ir-3 and Ir-4 showed strong absorption in the visible range (ε=39,600  M(-1)  cm(-1) at 402 nm and ε=25,100  M(-1)  cm(-1) at 404 nm, respectively), long-lived triplet excited states (τ(T)=9.30 μs and 16.45 μs) and room-temperature red emission (λ(em)=640 nm, Φ(p)=1.4 % and λ(em)=627 nm, Φ(p)=0.3 %; cf. Ir-1: ε=16,600  M(-1)  cm(-1) at 382 nm, τ(em)=1.16 μs, Φ(p)=72.6 %). Ir-3 was strongly phosphorescent in non-polar solvent (i.e., toluene), but the emission was completely quenched in polar solvents (MeCN). Ir-4 gave an opposite response to the solvent polarity, that is, stronger phosphorescence in polar solvents than in non-polar solvents. Emission of Ir-1 and Ir-2 was not solvent-polarity-dependent. The T(1) excited states of Ir-2, Ir-3, and Ir-4 were identified as mainly intraligand triplet excited states ((3)IL) by their small thermally induced Stokes shifts (ΔE(s)), nanosecond time-resolved transient difference absorption spectroscopy, and spin-density analysis. The complexes were used as triplet photosensitizers for triplet-triplet annihilation (TTA) upconversion and quantum yields of 7.1 % and 14.4 % were observed for Ir-2 and Ir-3, respectively, whereas the upconversion was negligible for Ir-1 and Ir-4. These results will be useful for designing visible-light-harvesting transition-metal complexes and for their applications as triplet photosensitizers for photocatalysis, photovoltaics, TTA upconversion, etc. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cubic sub-20 nm NaLuF(4)-based upconversion nanophosphors for high-contrast bioimaging in different animal species.

PubMed

Yang, Tianshe; Sun, Yun; Liu, Qian; Feng, Wei; Yang, Pengyuan; Li, Fuyou

2012-05-01

A new upconversion luminescence (UCL) nanophosphors based on host matrix of cubic NaLuF(4) with bright luminescence have been synthesized by a solvothermal method, facilitate the nanocrystals potential candidates for imaging in vivo, especially large-animals. The sub-20 nm NaLuF(4) co-doped Yb(3+) and Er(3+) (Tm(3+)) showed about 10-fold stronger UCL emission than that of corresponding hexagonal NaYF(4)-based nanocrystals with a 20 nm diameter. Near-infrared to near-infrared (NIR-to-NIR) UCL emission of PAA-coated NaLuF(4):20%Yb,1%Tm (PAA-Lu(Tm)) can penetrate >1.5 cm tissue of pork with high contrast. Based on super-strong UCL emission and deep penetration, PAA-Lu(Tm) as optical bioprobe has been demonstrated by in vivo UCL imaging of a normal black mouse, even rabbit with excellent signal-to-noise ratio. Furthermore, such cubic NaLuF(4)-based nanophosphor was applied in lymph node imaging of live Kunming mouse with rich white fur. Copyright © 2012 Elsevier Ltd. All rights reserved.

Controllable optical modulation of blue/green up-conversion fluorescence from Tm3+ (Er3+) single-doped glass ceramics upon two-step excitation of two-wavelengths

PubMed Central

Chen, Zhi; Kang, Shiliang; Zhang, Hang; Wang, Ting; Lv, Shichao; Chen, Qiuqun; Dong, Guoping; Qiu, Jianrong

2017-01-01

Optical modulation is a crucial operation in photonics for network data processing with the aim to overcome information bottleneck in terms of speed, energy consumption, dispersion and cross-talking from conventional electronic interconnection approach. However, due to the weak interactions between photons, a facile physical approach is required to efficiently manipulate photon-photon interactions. Herein, we demonstrate that transparent glass ceramics containing LaF3: Tm3+ (Er3+) nanocrystals can enable fast-slow optical modulation of blue/green up-conversion fluorescence upon two-step excitation of two-wavelengths at telecom windows (0.8–1.8 μm). We show an optical modulation of more than 1500% (800%) of the green (blue) up-conversion fluorescence intensity, and fast response of 280 μs (367 μs) as well as slow response of 5.82 ms (618 μs) in the green (blue) up-conversion fluorescence signal, respectively. The success of manipulating laser at telecom windows for fast-slow optical modulation from rear-earth single-doped glass ceramics may find application in all-optical fiber telecommunication areas. PMID:28368041

Long-lived room temperature deep-red/near-IR emissive intraligand triplet excited state (3IL) of naphthalimide in cyclometalated platinum(II) complexes and its application in upconversion.

PubMed

Wu, Wenting; Guo, Huimin; Wu, Wanhua; Ji, Shaomin; Zhao, Jianzhang

2011-11-21

[C(^)NPt(acac)] (C(^)N = cyclometalating ligand; acac = acetylacetonato) complexes in which the naphthalimide (NI) moiety is directly cyclometalated (NI as the C donor of the C-Pt bond) were synthesized. With 4-pyrazolylnaphthalimide, isomers with five-membered (Pt-2) and six-membered (Pt-3) chelate rings were obtained. With 4-pyridinylnaphthalimide, only the complex with a five-membered chelate ring (Pt-4) was isolated. A model complex with 1-phenylpyrazole as the C(^)N ligand was prepared (Pt-1). Strong absorption of visible light (ε = 21,900 M(-1) cm(-1) at 443 nm for Pt-3) and room temperature (RT) phosphorescence at 630 nm (Pt-2 and Pt-3) or 674 nm (Pt-4) were observed. Long-lived phosphorescences were observed for Pt-2 (τ(P) = 12.8 μs) and Pt-3 (τ(P) = 61.9 μs). Pt-1 is nonphosphorescent at RT in solution because of the acac-localized T(1) excited state [based on density functional theory (DFT) calculations and spin density analysis], but a structured emission band centered at 415 nm was observed at 77 K. Time-resolved transient absorption spectra and spin density analysis indicated a NI-localized intraligand triplet excited state ((3)IL) for complexes Pt-2, Pt-3, and Pt-4. DFT calculations on the transient absorption spectra (T(1) → T(n) transitions, n > 1) also support the (3)IL assignment of the T(1) excited states of Pt-2, Pt-3, and Pt-4. The complexes were used as triplet sensitizers for triplet-triplet-annihilation (TTA) based upconversion, and the results show that Pt-3 is an efficient sensitizer with an upconversion quantum yield of up to 14.1%, despite its low phosphorescence quantum yield of 5.2%. Thus, we propose that the sensitizer molecules at the triplet excited state that are otherwise nonphosphorescent were involved in the TTA upconversion process, indicating that weakly phosphorescent or nonphosphorescent transition-metal complexes can be used as triplet sensitizers for TTA upconversion.

Structure, upconversion photoluminescence, and dielectric properties of Ho{sup 3+}- and Yb{sup 3+}-codoped tetragonal tungsten bronze Sr{sub 4}La{sub 2}Ti{sub 4}Nb{sub 6}O{sub 30}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wei, T., E-mail: weitong.nju@gmail.com; Li, C.P.; Zhou, Q.J.

2015-04-15

Highlights: • TTB-type SLTN: Ho-Ybx with space group P4/mbm was determined. • UC photoluminescence of SLTN: Ho-Ybx ceramics was first reported. • Bright UC green emission was observed at room temperature. • Two-photon energy transfer process was confirmed for the UC processes. • Temperature stability of dielectric permittivity was improved for SLTN: Ho-Ybx. - Abstract: Ho{sup 3+}- and Yb{sup 3+}-codoped Sr{sub 4}La{sub 2}Ti{sub 4}Nb{sub 6}O{sub 30} (Sr{sub 4}La{sub 1.94–x}Ho{sub 0.06}Yb{sub x}Ti{sub 4}Nb{sub 6}O{sub 30}, abbreviated as SLTN: Ho-Ybx) ceramics have been synthesized, and their structural, up-conversion (UC) photoluminescence, and dielectric properties have been carefully investigated. Through Rietveld structural refinement, SLTN:more » Ho-Ybx samples are determined as single tetragonal tungsten bronze (TTB) phase with space group P4/mbm in which larger Sr{sup 2+} ions fill the A{sub 2}-sites, relative smaller La{sup 3+}, Ho{sup 3+}, and Yb{sup 3+} ions occupy the A{sub 1}-sites, while Ti{sup 4+} and Nb{sup 4+} ions fill the B-sites. Under 980 nm near infrared (NIR) excitation, bright UC green emission, relatively weak red and near-infrared (NIR) emissions, originating from {sup 5}F{sub 4}/{sup 5}S{sub 2} → {sup 5}I{sub 8}, {sup 5}F{sub 5} → {sup 5}I{sub 8}, and {sup 5}F{sub 4}/{sup 5}S{sub 2} → {sup 5}I{sub 7} transitions of Ho{sup 3+} ions, are confirmed for SLTN: Ho-Ybx. Two-photon energy transfer process is proved through pumping laser power dependence of emission intensity measurement. Furthermore, the influence of Ho{sup 3+}- and Yb{sup 3+}- ions on the dielectric properties of SLTN: Ho-Ybx is also investigated and the temperature stability of dielectric permittivity is improved.« less

Z-scan Measurement of Upconversion in Er:YAG

DTIC Science & Technology

2010-12-01

of each manifold, e.g.   22414313212121 NCWNWNWNNfNfh I td Nd upae    . (1) Here, N1 (N2) is the population of the 4I15/2 (4I13/2...manifold, I is the laser intensity,  is the absolute cross section, fa ( fe ) is the probability that an ion in the 4I15/2 (4I13/2) manifold is in a...sublevel that can absorb (emit) a laser photon, Wij is the relaxation rate from level i to level j, and Cup is the upconversion coefficient. Also

Enabling valley selective exciton scattering in monolayer WSe2 through upconversion

PubMed Central

Manca, M.; Glazov, M. M.; Robert, C.; Cadiz, F.; Taniguchi, T.; Watanabe, K.; Courtade, E.; Amand, T.; Renucci, P.; Marie, X.; Wang, G.; Urbaszek, B.

2017-01-01

Excitons, Coulomb bound electron–hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe2 monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy; we also observe the excited A-excitons state 2s. Detuning of the continuous wave, low-power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal. PMID:28367962

Efficient upconversion-pumped continuous wave Er3+:LiLuF4 lasers

NASA Astrophysics Data System (ADS)

Moglia, Francesca; Müller, Sebastian; Reichert, Fabian; Metz, Philip W.; Calmano, Thomas; Kränkel, Christian; Heumann, Ernst; Huber, Günter

2015-04-01

We report on detailed spectroscopic investigations and efficient visible upconversion laser operation of Er3+:LiLuF4. This material allows for efficient resonant excited-state-absorption (ESA) pumping at 974 nm. Under spectroscopic conditions without external feedback, ESA at the laser wavelength of 552 nm prevails stimulated emission. Under lasing conditions in a resonant cavity, the high intracavity photon density bleaches the ESA at 552 nm, allowing for efficient cw laser operation. We obtained the highest output power of any room-temperature crystalline upconversion laser. The laser achieves a cw output power of 774 mW at a slope efficiency of 19% with respect to the incident pump power delivered by an optically-pumped semiconductor laser. The absorption efficiency of the pump radiation is estimated to be below 50%. To exploit the high confinement in waveguides for this laser, we employed femtosecond-laser pulses to inscribe a cladding of parallel tracks of modified material into Er3+:LiLuF4 crystals. The core material allows for low-loss waveguiding at pump and laser wavelengths. Under Ti:sapphire pumping at 974 nm, the first crystalline upconversion waveguide laser has been realized. We obtained waveguide-laser operation with up to 10 mW of output power at 553 nm.

Simultaneous realization of Hg2+ sensing, magnetic resonance imaging and upconversion luminescence in vitro and in vivo bioimaging based on hollow mesoporous silica coated UCNPs and ruthenium complex

NASA Astrophysics Data System (ADS)

Ge, Xiaoqian; Sun, Lining; Ma, Binbin; Jin, Di; Dong, Liang; Shi, Liyi; Li, Nan; Chen, Haige; Huang, Wei

2015-08-01

We have constructed a multifunctional nanoprobe with sensing and imaging properties by using hollow mesoporous silica coated upconversion nanoparticles (UCNPs) and Hg2+ responsive ruthenium (Ru) complex. The Ru complex was loaded into the hollow mesoporous silica and the UCNPs acted as an energy donor, transferring luminescence energy to the Ru complex. Furthermore, polyethylenimine (PEI) was assembled on the surface of mesoporous silica to achieve better hydrophilic and bio-compatibility. Upon addition of Hg2+, a blue shift of the absorption peak of the Ru complex is observed and the energy transfer process between the UCNPs and the Ru complex was blocked, resulting in an increase of the green emission intensity of the UCNPs. The un-changed 801 nm emission of the nanoprobe was used as an internal standard reference and the detection limit of Hg2+ was determined to be 0.16 μM for this nanoprobe in aqueous solution. In addition, based on the low cytotoxicity as studied by CCK-8 assay, the nanoprobe was successfully applied for cell imaging and small animal imaging. Furthermore, when doped with Gd3+ ions, the nanoprobe was successfully applied to in vivo magnetic resonance imaging (MRI) of Kunming mice, which demonstrates its potential as a MRI positive-contrast agent. Therefore, the method and results may provide more exciting opportunities to afford nanoprobes with multimodal bioimaging and multifunctional applications.We have constructed a multifunctional nanoprobe with sensing and imaging properties by using hollow mesoporous silica coated upconversion nanoparticles (UCNPs) and Hg2+ responsive ruthenium (Ru) complex. The Ru complex was loaded into the hollow mesoporous silica and the UCNPs acted as an energy donor, transferring luminescence energy to the Ru complex. Furthermore, polyethylenimine (PEI) was assembled on the surface of mesoporous silica to achieve better hydrophilic and bio-compatibility. Upon addition of Hg2+, a blue shift of the absorption peak of the Ru complex is observed and the energy transfer process between the UCNPs and the Ru complex was blocked, resulting in an increase of the green emission intensity of the UCNPs. The un-changed 801 nm emission of the nanoprobe was used as an internal standard reference and the detection limit of Hg2+ was determined to be 0.16 μM for this nanoprobe in aqueous solution. In addition, based on the low cytotoxicity as studied by CCK-8 assay, the nanoprobe was successfully applied for cell imaging and small animal imaging. Furthermore, when doped with Gd3+ ions, the nanoprobe was successfully applied to in vivo magnetic resonance imaging (MRI) of Kunming mice, which demonstrates its potential as a MRI positive-contrast agent. Therefore, the method and results may provide more exciting opportunities to afford nanoprobes with multimodal bioimaging and multifunctional applications. Electronic supplementary information (ESI) available: DLS of Ru-UCNPs@HmSiO2-PEI in water. The zeta potential. The XRD patterns. EDX spectrum of Ru-UCNPs@HmSiO2-PEI. FT-IR spectra. N2 adsorption-desorption isotherm and pore size distribution. The investigation of the stability of Ru-UCNPs@HmSiO2-PEI. TG curves. UV/Vis absorption spectra of Ru complex at different concentrations. The sensitivity test of Ru-UCNPs@HmSiO2-PEI towards Hg2+. Cell viabilities of HeLa cells incubated with Ru-UCNPs@HmSiO2-PEI. See DOI: 10.1039/c5nr04006j

Laser and gain parameters at 2.7 μm of Er 3+-doped oxyfluoride transparent glass-ceramics

NASA Astrophysics Data System (ADS)

Tikhomirov, V. K.; Méndez-Ramos, J.; Rodríguez, V. D.; Furniss, D.; Seddon, A. B.

2006-07-01

The room temperature emission spectrum at about 2.7 μm corresponding to the laser transition 4I 11/2 → 4I 13/2 in Er 3+-doped nano-scaled transparent oxyfluoride glass-ceramic has been measured and stimulated emission cross-section for the transition has been calculated. The intensity of the transition has been found to be 40 times stronger and lifetime 50 times longer in the glass-ceramics compared to the precursor glass, which we show to be due to a change of frequency of the phonon involved in non-radiative de-excitation of the 4I 11/2 level from 900 cm -1 in the precursor glass to 240 cm -1 in the ensuing glass-ceramics. The absorption cross-section for the excited state absorption 4I 13/2 → 4I 11/2 has been calculated based on the experimental reciprocal emission spectrum and wavelength dependence of the gain cross-section for the lasing transition 4I 11/2 → 4I 13/2 vs population inversion has been derived. The lasing/optical amplification gain parameters, such as population inversion, pump saturation intensity and product of emission cross-section and fluorescence lifetime have been obtained at the 2.7 μm wavelength. A noteworthy result is that laser action at 2.7 μm is possible in these Er 3+-doped glass-ceramics, already not taking into account energy transfer or up-conversion processes, related to the 4I 13/2 level, which favour the population inversion.

Up-conversion luminescence properties and energy transfer of Tm{sup 3+}/Yb{sup 3+} co-doped BaLa{sub 2}ZnO{sub 5}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xie, Jing; Mei, Lefu, E-mail: mlf@cugb.edu.cn; Deng, Junru

2015-11-15

Tm{sup 3+}/Yb{sup 3+} co-doped BaLa{sub 2}ZnO{sub 5} up-conversion (UC) phosphors were successfully synthesized by high temperature solid-state reaction method. The X-ray diffraction (XRD) results show that synthesized phosphor co-doped with 0.75% Tm/10% Yb has the optimum pure phase of BaLa{sub 2}ZnO{sub 5} among different co-doping concentrations. The structure of BaLa{sub 2}ZnO{sub 5}:0.75% Tm/10% Yb phosphor was refined by the Rietveld method and results show the decreased unit cell parameters and cell volume after doping Tm{sup 3+}/Yb{sup 3+}, indicating that Tm{sup 3+}/Yb{sup 3+} have successfully replaced La{sup 3+}. Under excitation at 980 nm, Tm{sup 3+}/Yb{sup 3+} co-doped BaLa{sub 2}ZnO{sub 5} phosphorsmore » present bright blue emission near 478 nm generated by the {sup 1}G{sub 4}→{sup 3}H{sub 6} transition and weak red emissions around 653 nm and 692 nm generated by the {sup 1}G{sub 4}→{sup 3}F{sub 4} and {sup 3}F{sub 3}→{sup 3}H{sub 6} transitions of Tm{sup 3+}, respectively. The UC luminescence properties of BaLa{sub 2}ZnO{sub 5} phosphors co-doped with different Tm{sup 3+}/Yb{sup 3+} concentrations were investigated, and the related UC mechanisms of Tm{sup 3+}/Yb{sup 3+} co-doped BaLa{sub 2}ZnO{sub 5} depending on pump power were studied in detail. - Graphical abstract: Up-conversion luminescence of BaLa{sub 2}ZnO{sub 5}:Tm{sup 3+}/Yb{sup 3+} and its crystal structure and up-conversion mechanisms. - Highlights: • Up-conversion phosphors BaLa{sub 2}ZnO{sub 5} co-doped with Tm{sup 3+}/Yb{sup 3+} were synthesized by high temperature solid-state reaction method. • The crystal structure of BaLa{sub 2}ZnO{sub 5} and the changes of cell parameters and volume of BaLa{sub 2}ZnO{sub 5} after doping Tm{sup 3+} and Yb{sup 3+} have been discussed. • Up-conversion luminescence properties and energy transfer between Tm{sup 3+} and Yb{sup 3+} in BaLa{sub 2}ZnO{sub 5} have been discussed in detail.« less

Optical thermometry using fluorescence intensities multi-ratios in NaGdTiO4:Yb3+/Tm3+ phosphors

NASA Astrophysics Data System (ADS)

Zhou, Aihua; Song, Feng; Song, Feifei; Feng, Ming; Adnan, Khan; Ju, Dandan; Wang, Xueqing

2018-04-01

The NaGdTiO4:Yb3+/Tm3+ phosphor has been effectively synthesized by the traditional solid-state reaction method and its down-conversion and up-conversion luminescence properties were systematically studied. The results indicate that the electric dipole-dipole interaction is the main mechanism for the luminescence quenching. The fact that the ratios of the up-conversion intensities, i.e., I795nm/I798nm, I807nm/I798nm, and I812nm/I798nm, increase linearly with temperature (100 K-300 K) provides us a simple and accurate temperature measurement method. Multi-ratios can be more accurate than using only one ratio, allowing for self-referenced temperature determination. It's promising for NaGdTiO4: Yb3+/Tm3+ to be used for optical temperature sensors.

Stochastic three-wave interaction in flaring solar loops

NASA Technical Reports Server (NTRS)

Vlahos, L.; Sharma, R. R.; Papadopoulos, K.

1983-01-01

A model is proposed for the dynamic structure of high-frequency microwave bursts. The dynamic component is attributed to beams of precipitating electrons which generate electrostatic waves in the upper hybrid branch. Coherent upconversion of the electrostatic waves to electromagnetic waves produces an intrinsically stochastic emission component which is superposed on the gyrosynchrotron continuum generated by stably trapped electron fluxes. The role of the density and temperature of the ambient plasma in the wave growth and the transition of the three wave upconversion to stochastic, despite the stationarity of the energy source, are discussed in detail. The model appears to reproduce the observational features for reasonable parameters of the solar flare plasma.

Cooperative infrared to visible upconversion and visible to near-infrared quantum cutting in Tb and Yb co-doped glass containing Ag nanoparticles

NASA Astrophysics Data System (ADS)

Pan, Z.; Sekar, G.; Akrobetu, R.; Mu, R.; Morgan, S. H.

2011-10-01

Tb, Yb, and Ag co-doped glass nano-composites were synthesized in a lithium-lanthanum-aluminosilicate glass matrix (LLAS) by a melt-quench technique. Ag nanoparticles (NPs) were formed in the glass matrix and confirmed by optical absorption and transmission electron microscopy (TEM). Plasmon enhanced luminescence was observed. Cooperative infrared to visible upconversion and visible to near-infrared quantum cutting were studied for samples with different thermal annealing times. Because the Yb3+ emission at 940 - 1020 nm is matched well with the band gap of crystalline Si, the quantum cutting effect may have its potential application in silicon-based solar cells.

Auger heating of carriers in {GaAs}/{AlAs} heterostructures

NASA Astrophysics Data System (ADS)

Borri, P.; Ceccherini, S.; Gurioli, M.; Bogani, F.

1997-07-01

The photoluminescence of {GaAs}/{AlAs} multiple quantum wells structures under optical ps excitation is investigated for carrier densities in the range 10 18-4 × 10 19 cm -3 with frequency and time-resolved spectroscopic techniques. The measurements give a direct evidence of the occurrence in the sample of carrier heating. This energy up-conversion gives rise to photoluminescence from the states near the Fermi level whose intensity and time evolution depend on the carrier density in a strongly non-linear way. The observed behaviour can be explained introducing in the carrier dynamics an up-conversion mechanism due to Auger-like processes.

Up-conversion white light of Tm 3+/Er 3+/Yb 3+ tri-doped CaF 2 phosphors

NASA Astrophysics Data System (ADS)

Cao, Chunyan; Qin, Weiping; Zhang, Jisen; Wang, Yan; Wang, Guofeng; Wei, Guodong; Zhu, Peifen; Wang, Lili; Jin, Longzhen

2008-03-01

Tm3+/Er3+/Yb3+ tri-doped CaF2 phosphors were synthesized using a hydrothermal method. The phosphors were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), and up-conversion (UC) emission spectra. After annealing, the phosphors emitted white light under a 980 nm continuous wave diode laser (CW LD 2 W) excitation. As the excitation power density changed in the range of 20-260 W/cm2, the chromaticity coordinates of the UC light of the phosphor Ca0.885Tm0.005Er0.01Yb0.1F2 fell well in the white region of the 1931 CIE diagram. For the proportion of red, green and blue (RGB) in white light is strict, key factors for achieving UC white light, such as host materials, rare earth ions doping concentrations, annealing temperatures, as well as the excitation power densities, were investigated and discussed.

Near-infrared-to-near-infrared down-shifting and upconversion luminescence of KY{sub 3}F{sub 10} with single dopant of Nd{sup 3+} ion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Huihong; State Key Laboratory of Luminescence Materials and Devices and Institute of Optical Communication Materials, South China University of Technology, Guangzhou 510641; Yu, Ting

2016-01-25

We have studied the structural and near-infrared (NIR) luminescent properties of KY{sub 3}F{sub 10} phosphors, singly doped with Nd{sup 3+} serving as both sensitizer and activator. With a single laser diode at the wavelength of 808 nm as a pump source, simultaneous NIR-to-NIR upconversion (UC) and down-shifting (DS) emissions are effectively achieved, due to the specific energy levels of Nd{sup 3+} dopant and the low phonon energy of the host. The luminescence mechanism related to energy transfer is discussed. The luminescence can be modulated through controlling the population of Nd{sup 3+}:{sup 4}F{sub 3/2} state in our experiment. Interestingly, both UC andmore » DS emissions of the material fall within the dual biological window, suggesting that the prepared phosphors have potential applications in the bioimaging field.« less

Photoemission of Energetic Hot Electrons Produced via Up-Conversion in Doped Quantum Dots.

PubMed

Dong, Yitong; Parobek, David; Rossi, Daniel; Son, Dong Hee

2016-11-09

The benefits of the hot electrons from semiconductor nanostructures in photocatalysis or photovoltaics result from their higher energy compared to that of the band-edge electrons facilitating the electron-transfer process. The production of high-energy hot electrons usually requires short-wavelength UV or intense multiphoton visible excitation. Here, we show that highly energetic hot electrons capable of above-threshold ionization are produced via exciton-to-hot-carrier up-conversion in Mn-doped quantum dots under weak band gap excitation (∼10 W/cm 2 ) achievable with the concentrated solar radiation. The energy of hot electrons is as high as ∼0.4 eV above the vacuum level, much greater than those observed in other semiconductor or plasmonic metal nanostructures, which are capable of performing energetically and kinetically more-challenging electron transfer. Furthermore, the prospect of generating solvated electron is unique for the energetic hot electrons from up-conversion, which can open a new door for long-range electron transfer beyond short-range interfacial electron transfer.

White phosphor using Yb3+-sensitized Er3+-and Tm3+-doped sol-gel derived lead-fluorosilicate transparent glass ceramic excited at 980 nm

NASA Astrophysics Data System (ADS)

Tavares, M. C. P.; da Costa, E. B.; Bueno, L. A.; Gouveia-Neto, A. S.

2018-01-01

Generation of primary colors and white light through frequency upconversion using sol-gel derived 80SiO2:20PbF2 vitroceramic phosphors doped with Er3+, Er3+/Yb3+, Tm3+/Yb3+, and Er3+/Tm3+/Yb3+ excited at 980 nm is demonstrated. For Er3+ and Er3+/Yb3+ doped samples emissions were obtained in the blue (410 nm), green (530, and 550 nm) and red (670 nm) regions, corresponding to the 2H9/2 → 4I15/2,2H11/2 → 4I15/2, 4S3/2 → 4I152 and 4F9/2 → 4I15/2 transitions of Er3+, respectively. The codoping with Yb3+ ions altered the spectral profile of most of the emissions compared to the single doped samples, resulting in changes in the emitted color, in addition to a significant increase in the emission intensity. In Tm3+/Yb3+ co-doped samples visible emissions in the blue (480 nm), and red (650 nm), corresponding to transitions 1G4 → 3H6 and 1G4 → 3F4 of Tm3+, respectively, were obtained. The emission intensity around 480 nm overcome the red emission, and luminescence showed a predominantly blue tone. White light with CIE-1931 coordinates (0.36; 0.34) was produced by homogeneously mixing up powders of heat treated at 400 °C co-doped samples 5.0Er3+/5.0Yb3+ and 0.5Tm3+/2.5Yb3+ in the mass ratio of 13%, and 87%, respectively. The measured emission spectrum for a sample resulting from the mixture showed a profile with very good agreement with the spectrum found from the superimposition of the spectra of the co-doped samples.

Synthesis of Core-shell Lanthanide-doped Upconversion Nanocrystals for Cellular Applications.

PubMed

Ai, Xiangzhao; Lyu, Linna; Mu, Jing; Hu, Ming; Wang, Zhimin; Xing, Bengang

2017-11-10

Lanthanide-doped upconversion nanocrystals (UCNs) have attracted much attention in recent years based on their promising and controllable optical properties, which allow for the absorption of near-infrared (NIR) light and can subsequently convert it into multiplexed emissions that span over a broad range of regions from the UV to the visible to the NIR. This article presents detailed experimental procedures for high-temperature co-precipitation synthesis of core-shell UCNs that incorporate different lanthanide ions into nanocrystals for efficiently converting deep-tissue penetrable NIR excitation (808 nm) into a strong blue emission at 480 nm. By controlling the surface modification with biocompatible polymer (polyacrylic acid, PAA), the as-prepared UCNs acquires great solubility in buffer solutions. The hydrophilic nanocrystals are further functionalized with specific ligands (dibenzyl cyclooctyne, DBCO) for localization on the cell membrane. Upon NIR light (808 nm) irradiation, the upconverted blue emission can effectively activate the light-gated channel protein on the cell membrane and specifically regulate the cation (e.g., Ca 2+ ) influx in the cytoplasm. This protocol provides a feasible methodology for the synthesis of core-shell lanthanide-doped UCNs and subsequent biocompatible surface modification for further cellular applications.

Excited-state absorption in Er: BaY2F8 and Cs3Er2Br9 and comparison with Er: LiYF4

NASA Astrophysics Data System (ADS)

Pollnau, M.; Lüthy, W.; Weber, H. P.; Krämer, K.; Güdel, H. U.; McFarlane, R. A.

1996-04-01

The influence of Excited-State Absorption (ESA) on the green laser transition and the overlap of Ground-State Absorption (GSA) and ESA for 970 nm upconversion pumping in erbium is investigated in Er3+ : BaY2F8 and Cs3Er2Br9. Results are compared to Er3+ : LiYF4. In Er3+: BaY2F8, a good overlap between GSA and ESA is found at 969 nm in one polarization direction. The emission cross section at 550 nm is a factor of two smaller than in LiYF4. In Cs3Er2Br9, the smaller Stark splitting of the levels shifts the wavelengths of the green emission and ESA from4 I 1 3/2 off resonance. It enhances, however, ground-state reabsorption. The emission cross section at 550 nm is comparable to LiYF4. Upconversion leads to significant green fluorescence from2 H 9/2. A significant population of the4 I 11/2 level and ESA at 970 nm are not present under 800 nm pumping.

Enhanced near-infrared to visible upconversion nanoparticles of Ho³⁺-Yb³⁺-F⁻ tri-doped TiO₂ and its application in dye-sensitized solar cells with 37% improvement in power conversion efficiency.

PubMed

Yu, Jia; Yang, Yulin; Fan, Ruiqing; Liu, Danqing; Wei, Liguo; Chen, Shuo; Li, Liang; Yang, Bin; Cao, Wenwu

2014-08-04

New near-infrared (NIR)-to-green upconversion nanoparticles of Ho(3+)-Yb(3+)-F(-) tridoped TiO2 (UC-F-TiO2) were designed and fabricated via the hydrosol-hydrothermal method. Under 980 nm NIR excitation, UC-F-TiO2 emit strong green upconversion fluorescence with three emission bands at 543, 644, and 751 nm and convert the NIR light in situ to the dye-sensitive visible light that could effectively reduce the distance between upconversion materials and sensitizers; thus, they minimize the loss of the converted light. Our results show that this UC-F-TiO2 offers excellent opportunities for the other types of solar cells applications, such as organic solar cells, c-Si solar cells, multijunction solar cells, and so on. When integrating the UC-F-TiO2 into dye-sensitized solar cells (DSSCs), superior total energy conversion efficiency was achieved. Under AM1.5G light, open-circuit voltage reached 0.77 ± 0.01 V, short-circuit current density reached 21.00 ± 0.69 mA cm(-2), which resulted in an impressive overall energy conversion efficiency of 9.91 ± 0.30%, a 37% enhancement compared to DSSCs with pristine TiO2 photoanode.

Highly Efficient LiYF4:Yb(3+), Er(3+) Upconversion Single Crystal under Solar Cell Spectrum Excitation and Photovoltaic Application.

PubMed

Chen, Xu; Xu, Wen; Song, Hongwei; Chen, Cong; Xia, Haiping; Zhu, Yongsheng; Zhou, Donglei; Cui, Shaobo; Dai, Qilin; Zhang, Jiazhong

2016-04-13

Luminescent upconversion is a promising way to harvest near-infrared (NIR) sunlight and transforms it into visible light that can be directly absorbed by active materials of solar cells and improve their power conversion efficiency (PCE). However, it is still a great challenge to effectively improve the PCE of solar cells with the assistance of upconversion. In this work, we demonstrate the application of the transparent LiYF4:Yb(3+), Er(3+) single crystal as an independent luminescent upconverter to improve the PCE of perovskite solar cells. The LiYF4:Yb(3+), Er(3+) single crystal is prepared by an improved Bridgman method, and its internal quantum efficiency approached to 5.72% under 6.2 W cm(-2) 980 nm excitation. The power-dependent upconversion luminescence indicated that under the excitation of simulated sunlight the (4)F(9/2)-(4)I(15/2) red emission originally results from the cooperation of a 1540 nm photon and a 980 nm photon. Furthermore, when the single crystal is placed in front of the perovskite solar cells, the PCE is enhanced by 7.9% under the irradiation of simulated sunlight by 7-8 solar constants. This work implies the upconverter not only can serve as proof of principle for improving PCE of solar cells but also is helpful to practical application.

Exceeding the solar cell Shockley-Queisser limit via thermal up-conversion of low-energy photons

NASA Astrophysics Data System (ADS)

Boriskina, Svetlana V.; Chen, Gang

2014-03-01

Maximum efficiency of ideal single-junction photovoltaic (PV) cells is limited to 33% (for 1 sun illumination) by intrinsic losses such as band edge thermalization, radiative recombination, and inability to absorb below-bandgap photons. This intrinsic thermodynamic limit, named after Shockley and Queisser (S-Q), can be exceeded by utilizing low-energy photons either via their electronic up-conversion or via the thermophotovoltaic (TPV) conversion process. However, electronic up-conversion systems have extremely low efficiencies, and practical temperature considerations limit the operation of TPV converters to the narrow-gap PV cells. Here we develop a conceptual design of a hybrid TPV platform, which exploits thermal up-conversion of low-energy photons and is compatible with conventional silicon PV cells by using spectral and directional selectivity of the up-converter. The hybrid platform offers sunlight-to-electricity conversion efficiency exceeding that imposed by the S-Q limit on the corresponding PV cells across a broad range of bandgap energies, under low optical concentration (1-300 suns), operating temperatures in the range 900-1700 K, and in simple flat panel designs. We demonstrate maximum conversion efficiency of 73% under illumination by non-concentrated sunlight. A detailed analysis of non-ideal hybrid platforms that allows for up to 15% of absorption/re-emission losses yields limiting efficiency value of 45% for Si PV cells.

Investigating the evolution of local structure around Er and Yb in ZnO:Er and ZnO:Er, Yb on annealing using X-ray absorption spectroscopy

NASA Astrophysics Data System (ADS)

Anjana, R.; Jayaraj, M. K.; Yadav, A. K.; Jha, S. N.; Bhattacharyya, D.

2018-04-01

The local structure around Er and Yb centre in ZnO favouring upconversion luminescence was studied using EXAFS (Extended X-ray absorption fine structure spectroscopy). Due to the ionic radii difference between Zn and Er, Yb ions, the dopants cannot replace Zn in the ZnO lattice properly. Er2O3 and Yb2O3 impurity phases are formed at the grain boundaries of ZnO. It is found that the local structure around the Er centre in ZnO is modified on annealing in air. The symmetry around both erbium and ytterbium reduces with increase in annealing temperature. Symmetry reduction will favour the intra-4f transition and the energy transitions causing upconversion luminescence. By fitting the EXAFS data with theoretically simulated data, it is found that the Er centre forms a local structure similar to C4ν symmetry which is a distorted octahedron. On annealing the sample to 1200 °C, all the erbium centres are transformed to C4ν symmetry causing enhanced upconversion emission. Yb centre has also been modified on annealing. The decrease in co-ordination number with annealing temperature will decrease the symmetry and increase the near infrared absorption cross section. The decrease in symmetry around both the erbium and ytterbium centre and formation of C4ν symmetry around Er centre is the reason behind the activation of upconversion luminescence with high temperature annealing in both Er doped and Er, Yb co-doped ZnO samples. The study will be useful for the synthesis of high efficiency upconversion materials.

Compositional dependence of broadband near-infrared downconversion and upconversion of Yb3+-doped multi-component glasses

NASA Astrophysics Data System (ADS)

Zhang, Liaolin; Xia, Yu; Shen, Xiao; Wei, Wei

2017-07-01

Yb3+ single-doped glasses show a strong excitation band in the 300-400 nm region, and efficiently emit photons with wavelengths of 920-1150 nm, and have potential applications in solar cells operating in an extraterrestrial situation. In this work, we systematically study the broadband near-infrared downconversion and upconversion of Yb3+-doped silicate, germanate, phosphate, tellurite and tungsten tellurite glasses. All samples show a broad excitation band in the 300-400 nm range, which is attributed to the charge transfer of the Yb3+-O2- couple. The position of the charge transfer band (CTB) shifts from 300 nm to longer wavelengths around 350 nm when the length of the R-O(Si, P, Ge, Te) increases. The longer R-O gives rise to a smaller central void for Yb3+, thus resulting in a small proportion of Yb3+ ions, thus leading to the blue-shift of the CTB. A smaller proportion of Yb3+ in silicate glasses causes in the strongest upconversion emission at 500 nm.

Low-power upconversion in dye-doped polymer nanoparticles.

PubMed

Simon, Yoan C; Bai, Shuo; Sing, Michelle K; Dietsch, Hervé; Achermann, Marc; Weder, Christoph

2012-04-13

Examples of nanoscale low-power upconverting systems are rapidly increasing because of their potential application in numerous areas such as bioimaging or drug delivery. The fabrication of dye-doped cross-linked rubbery nanoparticles that exhibit upconversion even at relatively low power densities is reported here. The nanoparticles were prepared by surfactant-free emulsion polymerization of n-butylacrylate with divinylbenzene as a cross-linker, followed by dyeing of the resulting particles with a two-chromophore system composed of a palladium porphyrin sensitizer, and diphenylanthracene. Blue emission (≈440 nm) of these systems was observed upon excitation at 532 nm. In addition to their optical properties, the particles were characterized by electron microscopy and dynamic light scattering. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Efficient near-infrared up-conversion photoluminescence in carbon nanotubes

PubMed Central

Akizuki, Naoto; Aota, Shun; Mouri, Shinichiro; Matsuda, Kazunari; Miyauchi, Yuhei

2015-01-01

Photoluminescence phenomena normally obey Stokes' law of luminescence according to which the emitted photon energy is typically lower than its excitation counterparts. Here we show that carbon nanotubes break this rule under one-photon excitation conditions. We found that the carbon nanotubes exhibit efficient near-infrared photoluminescence upon photoexcitation even at an energy lying >100–200 meV below that of the emission at room temperature. This apparently anomalous phenomenon is attributed to efficient one-phonon-assisted up-conversion processes resulting from unique excited-state dynamics emerging in an individual carbon nanotube with accidentally or intentionally embedded localized states. These findings may open new doors for energy harvesting, optoelectronics and deep-tissue photoluminescence imaging in the near-infrared optical range. PMID:26568250

Transition Metal-Involved Photon Upconversion.

PubMed

Ye, Shi; Song, En-Hai; Zhang, Qin-Yuan

2016-12-01

Upconversion (UC) luminescence of lanthanide ions (Ln 3+ ) has been extensively investigated for several decades and is a constant research hotspot owing to its fundamental significance and widespread applications. In contrast to the multiple and fixed UC emissions of Ln 3+ , transition metal (TM) ions, e.g., Mn 2+ , usually possess a single broadband emission due to its 3 d 5 electronic configuration. Wavelength-tuneable single UC emission can be achieved in some TM ion-activated systems ascribed to the susceptibility of d electrons to the chemical environment, which is appealing in molecular sensing and lighting. Moreover, the UC emissions of Ln 3+ can be modulated by TM ions (specifically d -block element ions with unfilled d orbitals), which benefits from the specific metastable energy levels of Ln 3+ owing to the well-shielded 4 f electrons and tuneable energy levels of the TM ions. The electric versatility of d 0 ion-containing hosts ( d 0 normally viewed as charged anion groups, such as MoO 6 6- and TiO 4 4- ) may also have a strong influence on the electric dipole transition of Ln 3+ , resulting in multifunctional properties of modulated UC emission and electrical behaviour, such as ferroelectricity and oxide-ion conductivity. This review focuses on recent advances in the room temperature (RT) UC of TM ions, the UC of Ln 3+ tuned by TM or d 0 ions, and the UC of d 0 ion-centred groups, as well as their potential applications in bioimaging, solar cells and multifunctional devices.

Transition Metal‐Involved Photon Upconversion

PubMed Central

Song, En‐Hai

2016-01-01

Upconversion (UC) luminescence of lanthanide ions (Ln3+) has been extensively investigated for several decades and is a constant research hotspot owing to its fundamental significance and widespread applications. In contrast to the multiple and fixed UC emissions of Ln3+, transition metal (TM) ions, e.g., Mn2+, usually possess a single broadband emission due to its 3d 5 electronic configuration. Wavelength‐tuneable single UC emission can be achieved in some TM ion‐activated systems ascribed to the susceptibility of d electrons to the chemical environment, which is appealing in molecular sensing and lighting. Moreover, the UC emissions of Ln3+ can be modulated by TM ions (specifically d‐block element ions with unfilled d orbitals), which benefits from the specific metastable energy levels of Ln3+ owing to the well‐shielded 4f electrons and tuneable energy levels of the TM ions. The electric versatility of d 0 ion‐containing hosts (d 0 normally viewed as charged anion groups, such as MoO6 6‐ and TiO4 4‐) may also have a strong influence on the electric dipole transition of Ln3+, resulting in multifunctional properties of modulated UC emission and electrical behaviour, such as ferroelectricity and oxide‐ion conductivity. This review focuses on recent advances in the room temperature (RT) UC of TM ions, the UC of Ln3+ tuned by TM or d 0 ions, and the UC of d 0 ion‐centred groups, as well as their potential applications in bioimaging, solar cells and multifunctional devices. PMID:27981015

The effect of MgO on the optical properties of lithium sodium borate doped with Cu+ ions

NASA Astrophysics Data System (ADS)

Alajerami, Yasser Saleh Mustafa; Hashim, Suhairul; Hassan, Wan Muhamad Saridan Wan; Ramli, Ahmad Termizi; Saleh, Muneer Aziz

2013-04-01

The current work presented the photoluminescence (PL) properties of a new glass system, which are reported for the first time. Based on the attractive properties of borate glass, a mixture of boric acid (70-x mol %) modified with lithium (20 mol %) and sodium carbonate (10 mol %) was prepared. The current study illustrated the effect of dopant and co-dopant techniques on the lithium sodium borate (LNB). Firstly, 0.1 mol % of copper ions doped with LNB was excited at 610 nm. The emission spectrum showed two prominent peaks in the violet region (403 and 440 nm). Then, we remarked the effect of adding different concentration of MgO on the optical properties of LNB. The results showed the great effect of magnesium oxide on the PL intensities (enhanced more than two times). Moreover, an obvious shifting has been defined toward the blue region (440 → 475 nm). The up-conversion optical properties were observed in all emission spectra. This enhancement is contributed to the energy transfer from MgO ions to monovalent Cu+ ion. It is well known that magnesium oxide alone generates weak emission intensity, but during this increment the MgO act as an activator (co-doped) for Cu+ ions. Finally, energy band gap, density, ion concentration, molar volume, Polaron radius and inter-nuclear distance all were measured for the current samples. The current samples were subjected to XRD for amorphous confirmation and IR for glass characterization before and after dopants addition. Finally, some of significant physical and optical parameters were also calculated.

Upconversion luminescence of CsScF4 crystals doped with erbium and ytterbium

NASA Astrophysics Data System (ADS)

Ikonnikov, D. A.; Voronov, V. N.; Molokeev, M. S.; Aleksandrovsky, A. S.

2016-10-01

Tetragonal CsScF4 crystals doped with (5 at.%) Er and Er/Yb (0.5 at.%/5 at.%) are grown and their crystal structure is determined to belong to Pmmn space group. Er and Yb ions are shown to occupy distorted octahedral Sc sites with the center of inversion. Bright visible upconversion luminescence was observed under 970-980 nm pumping with red (4F9/2), yellow (4S3/2) and green (2H11/2) bands of comparable intensity. UCL tuning curves maximize at 972 nm (CSF:Er) and at 969.7 nm (CSF:Er,Yb) pumping wavelengths. Different ratios between yellow-green and red luminescence intensities in CSF:Er and CSF:Er, Yb are explained by contribution of cross-relaxation in CSF:Er UCL. UC in CSF:Er is a three stage process while UC in CSF:Er, Yb is a two stage process. The peculiarities of power dependences are explained by the power-dependent repopulation between starting levels of UC.

Magnetic and upconverted luminescent properties of multifunctional lanthanide doped cubic KGdF4 nanocrystals.

PubMed

Yang, L W; Zhang, Y Y; Li, J J; Li, Y; Zhong, J X; Chu, Paul K

2010-12-01

Lanthanide (Ln3+) doped KGdF4 (Ln=Yb3+, Er3+, Ho3+, Tm3+) nanocrystals with a mean diameter of approximately 12 nm were synthesized by a hydrothermal method using oleic acid as a stabilizing agent at 180 °C. The nanocrystals crystallize in the cubic phase as α-NaGdF4. When excited by a 980 nm laser, these Ln3+ doped nanocrystals exhibit multicolor up-conversion (UC) emissions in red, yellow, blue and white. The calculated color coordinates demonstrate that white UC emission (CIE-X=0.352, CIE-Y=0.347) can be obtained by varying the dopant concentrations in the Yb3+/Ho3+/Tm3+ triply-doped nanocrystals to yield different RGB emission intensities. The measured field dependence of magnetization (M-H curves) of the KGdF4 nanocrystals shows their paramagnetic characteristics that can be ascribed to the non-interacting localized nature of the magnetic moment of Gd3+ ions. Moreover, low temperature thermal treatment can enhance UC properties, magnetization and magnetic mass susceptibility of Ln3+ doped KGdF4 nanocrystals. The multifunctional Ln3+ doped KGdF4 nanocrystals have potential applications in color displays, bioseparation, and optical-magnetic dual modal nanoprobes in biomedical imaging.

Magnetic and upconverted luminescent properties of multifunctional lanthanide doped cubic KGdF4nanocrystals

NASA Astrophysics Data System (ADS)

Yang, L. W.; Zhang, Y. Y.; Li, J. J.; Li, Y.; Zhong, J. X.; Chu, Paul K.

2010-12-01

Lanthanide (Ln3+) doped KGdF4 (Ln = Yb3+, Er3+, Ho3+, Tm3+) nanocrystals with a mean diameter of approximately 12 nm were synthesized by a hydrothermal method using oleic acid as a stabilizing agent at 180 °C. The nanocrystals crystallize in the cubic phase as α-NaGdF4. When excited by a 980 nm laser, these Ln3+ doped nanocrystals exhibit multicolor up-conversion (UC) emissions in red, yellow, blue and white. The calculated color coordinates demonstrate that white UC emission (CIE-X = 0.352, CIE-Y = 0.347) can be obtained by varying the dopant concentrations in the Yb3+/Ho3+/Tm3+ triply-doped nanocrystals to yield different RGB emission intensities. The measured field dependence of magnetization (M-H curves) of the KGdF4nanocrystals shows their paramagnetic characteristics that can be ascribed to the non-interacting localized nature of the magnetic moment of Gd3+ ions. Moreover, low temperature thermal treatment can enhance UC properties, magnetization and magnetic mass susceptibility of Ln3+ doped KGdF4nanocrystals. The multifunctional Ln3+ doped KGdF4nanocrystals have potential applications in color displays, bioseparation, and optical-magnetic dual modal nanoprobes in biomedical imaging.

Surface modification of upconverting nanoparticles by layer-by-layer assembled polyelectrolytes and metal ions.

PubMed

Palo, Emilia; Salomäki, Mikko; Lastusaari, Mika

2017-12-15

Modificating and protecting the upconversion luminescence nanoparticles is important for their potential in various applications. In this work we demonstrate successful coating of the nanoparticles by a simple layer-by-layer method using negatively charged polyelectrolytes and neodymium ions. The layer fabrication conditions such as number of the bilayers, solution concentrations and selected polyelectrolytes were studied to find the most suitable conditions for the process. The bilayers were characterized and the presence of the desired components was studied and confirmed by various methods. In addition, the upconversion luminescence of the bilayered nanoparticles was studied to see the effect of the surface modification on the overall intensity. It was observed that with selected deposition concentrations the bilayer successfully shielded the particle resulting in stronger upconversion luminescence. The layer-by-layer method offers multiple possibilities to control the bilayer growth even further and thus gives promises that the use of upconverting nanoparticles in applications could become even easier with less modification steps in the future. Copyright © 2017 Elsevier Inc. All rights reserved.

Triplet-Triplet Annihilation Photon Upconversion in Polymer Thin Film: Sensitizer Design.

PubMed

Jiang, Xinpeng; Guo, Xinyan; Peng, Jiang; Zhao, Dahui; Ma, Yuguo

2016-05-11

Efficient visible-to-UV photon upconversion via triplet-triplet annihilation (TTA) is accomplished in polyurethane (PU) films by developing new, powerful photosensitizers fully functional in the solid-state matrix. These rationally designed triplet sensitizers feature a bichromophoric scaffold comprising a tris-cyclometalated iridium(III) complex covalently tethered to a suitable organic small molecule. The very rapid intramolecular triplet energy transfer from the former to the latter is pivotal for achieving the potent sensitizing ability, because this process out-competes the radiative and nonradiative decays inherent to the metal complex and produces long-lived triplet excitons localized with the acceptor moiety readily available for intermolecular transfer and TTA. Nonetheless, compared to the solution state, the molecular diffusion is greatly limited in solid matrices, which even creates difficulty for the Dexter-type intramolecular energy transfer. This is proven by the experimental results showing that the sensitizing performance of the bichromophoric molecules strongly depends on the spatial distance separating the donor (D) and acceptor (A) units and that incorporating a longer linker between the D and A evidently curbs the TTA upconversion efficiency in PU films. Using a rationally optimized sensitizer structure in combination with 2,7-di-tert-butylpyrene as the annihilator/emitter, the doped polyurethane (PU) films demonstrate effective visible-to-UV upconverted emission signal under noncoherent-light irradiation, attaining an upconversion quantum yield of 2.6%. Such quantum efficiency is the highest value so far reported for the visible-to-UV TTA systems in solid matrices.

Modifying the size and uniformity of upconversion Yb/Er:NaGdF4 nanocrystals through alkaline-earth doping.

PubMed

Lei, Lei; Chen, Daqin; Huang, Ping; Xu, Ju; Zhang, Rui; Wang, Yuansheng

2013-11-21

NaGdF4 is regarded as an ideal upconversion (UC) host material for lanthanide (Ln(3+)) activators because of its unique crystal structure, high Ln(3+) solubility, low phonon energy and high photochemical stability, and Ln(3+)-doped NaGdF4 UC nanocrystals (NCs) have been widely investigated as bio-imaging and magnetic resonance imaging agents recently. To realize their practical applications, controlling the size and uniformity of the monodisperse Ln(3+)-doped NaGdF4 UC NCs is highly desired. Unlike the routine routes by finely adjusting the multiple experimental parameters, herein we provide a facile and straightforward strategy to modify the size and uniformity of NaGdF4 NCs via alkaline-earth doping for the first time. With the increase of alkaline-earth doping content, the size of NaGdF4 NCs increases gradually, while the size-uniformity is still retained. We attribute this "focusing" of size distribution to the diffusion controlled growth of NaGdF4 NCs induced by alkaline-earth doping. Importantly, adopting the Ca(2+)-doped Yb/Er:NaGdF4 NCs as cores, the complete Ca/Yb/Er:NaGdF4@NaYF4 core-shell particles with excellent size-uniformity can be easily achieved. However, when taking the Yb/Er:NaGdF4 NCs without Ca(2+) doping as cores, they could not be perfectly covered by NaYF4 shells, and the obtained products are non-uniform in size. As a result, the UC emission intensity of the complete core-shell NCs increases by about 30 times in comparison with that of the cores, owing to the effective surface passivation of the Ca(2+)-doped cores and therefore protection of Er(3+) in the cores from the non-radiative decay caused by surface defects, whereas the UC intensity of the incomplete core-shell NCs is enhanced by only 3 times.

Luminescence resonance energy transfer (LRET) aptasensor for ochratoxin A detection using upconversion nanoparticles

NASA Astrophysics Data System (ADS)

Jo, Eun-Jung; Byun, Ju-Young; Mun, Hyoyoung; Kim, Min-Gon

2017-07-01

We report an aptasensor for homogeneous ochratoxin A (OTA) detection based on luminescence resonance energy transfer (LRET). This system uses upconversion nanoparticles (UCNPs), such as NaYF4:Yb3+, Er 3+, as the donor. The aptamer includes the optimum-length linker (5-mer-length DNA) and OTA-specific aptamer sequences. Black hole quencher 1 (BHQ1), as the acceptor, was modified at the 3' end of the aptamer sequence. BHQ1 plays as a quencher in LRET aptasensor and shows absorption at 543 nm, which overlaps with well the emission of the UCNPs. When OTA is added, the BHQ1-labeled OTA aptamer was folded due to the formation of the G-quadruplex-OTA complex, which induced the BHQ1 close to the UCNPs. Consequently, resonance energy transfer between UCNPs (donor) and BHQ1 (acceptor) enables quenching of upconversion luminescence signals under laser irradiation of 980 nm. Our results showed that the LRET-based aptasensor allows specific OTA analysis with a limit of detection of 0.03 ng/mL. These results demonstrated that the OTA in diverse foods can be detected specifically and sensitively in a homogeneous manner.

Rare Earth Ion-Doped Upconversion Nanocrystals: Synthesis and Surface Modification

PubMed Central

Chang, Hongjin; Xie, Juan; Zhao, Baozhou; Liu, Botong; Xu, Shuilin; Ren, Na; Xie, Xiaoji; Huang, Ling; Huang, Wei

2014-01-01

The unique luminescent properties exhibited by rare earth ion-doped upconversion nanocrystals (UCNPs), such as long lifetime, narrow emission line, high color purity, and high resistance to photobleaching, have made them widely used in many areas, including but not limited to high-resolution displays, new-generation information technology, optical communication, bioimaging, and therapy. However, the inherent upconversion luminescent properties of UCNPs are influenced by various parameters, including the size, shape, crystal structure, and chemical composition of the UCNPs, and even the chosen synthesis process and the surfactant molecules used. This review will provide a complete summary on the synthesis methods and the surface modification strategies of UCNPs reported so far. Firstly, we summarize the synthesis methodologies developed in the past decades, such as thermal decomposition, thermal coprecipitation, hydro/solvothermal, sol-gel, combustion, and microwave synthesis. In the second part, five main streams of surface modification strategies for converting hydrophobic UCNPs into hydrophilic ones are elaborated. Finally, we consider the likely directions of the future development and challenges of the synthesis and surface modification, such as the large-scale production and actual applications, stability, and so on, of the UCNPs. PMID:28346995

Broadband dye-sensitized upconverting nanocrystals enabled near-infrared planar perovskite solar cells

NASA Astrophysics Data System (ADS)

Lai, Xuesen; Li, Xitao; Lv, Xinding; Zheng, Yan-Zhen; Meng, Fanli; Tao, Xia

2017-12-01

Extending the spectral absorption of perovskite solar cells (PSCs) from visible into near-infrared (NIR) range is a promising strategy to minimize non-absorption loss of solar photons and enhance the cell photovoltaic performance. Herein, we report on for the first time a viable strategy of incorporating IR806 dye-sensitized upconversion nanocrystals (IR806-UCNCs) into planar PSC for broadband upconversion of NIR light (800-1000 nm) into perovskite absorber-responsive visible emissions. A smart trick is firstly adopted to prepare hydrophilic IR806-UCNCs via a NOBF4 assisted two-step ligand-exchange that allows incorporating with perovskite precursor for in-situ growth of upconverting planar perovskite film. Unlike typically reported upconverting nanoparticles with narrow NIR absorption, the as-prepared IR806-UCNCs are able to harvest NIR light broadly and then transfer the captured energy to the UCNCs for an efficient visible upconversion. The IR806-UCNCs-incorporated cell exhibits a power conversion efficiency of 17.49%, corresponding to 29% increment from that of the pristine cell (13.52%). This strategy provides a feasible way to enable the most efficient harvesting of NIR sunlight for solar cells and other optoelectric devices.

Bioinspired near-infrared-excited sensing platform for in vitro antioxidant capacity assay based on upconversion nanoparticles and a dopamine-melanin hybrid system.

PubMed

Wang, Dong; Chen, Chuan; Ke, Xuebin; Kang, Ning; Shen, Yuqing; Liu, Yongliang; Zhou, Xi; Wang, Hongjun; Chen, Changqing; Ren, Lei

2015-02-11

A novel core-shell structure based on upconversion fluorescent nanoparticles (UCNPs) and dopamine-melanin has been developed for evaluation of the antioxidant capacity of biological fluids. In this approach, dopamine-melanin nanoshells facilely formed on the surface of UCNPs act as ultraefficient quenchers for upconversion fluorescence, contributing to a photoinduced electron-transfer mechanism. This spontaneous oxidative polymerization of the dopamine-induced quenching effect could be effectively prevented by the presence of various antioxidants (typically biothiols, ascorbic acid (Vitamin C), and Trolox). The chemical response of the UCNPs@dopamine-melanin hybrid system exhibited great selectivity and sensitivity toward antioxidants relative to other compounds at 100-fold higher concentration. A satisfactory correlation was established between the ratio of the "anti-quenching" fluorescence intensity and the concentration of antioxidants. Besides the response of the upconversion fluorescence signal, a specific evaluation process for antioxidants could be visualized by the color change from colorless to dark gray accompanied by the spontaneous oxidation of dopamine. The near-infrared (NIR)-excited UCNP-based antioxidant capacity assay platform was further used to evaluate the antioxidant capacity of cell extracts and human plasma, and satisfactory sensitivity, repeatability, and recovery rate were obtained. This approach features easy preparation, fluorescence/visual dual mode detection, high specificity to antioxidants, and enhanced sensitivity with NIR excitation, showing great potential for screening and quantitative evaluation of antioxidants in biological systems.

Photon upconversion in homogeneous fluorescence-based bioanalytical assays.

PubMed

Soukka, Tero; Rantanen, Terhi; Kuningas, Katri

2008-01-01

Upconverting phosphors (UCPs) are very attractive reporters for fluorescence resonance energy transfer (FRET)-based bioanalytical assays. The large anti-Stokes shift and capability to convert near-infrared to visible light via sequential absorption of multiple photons enable complete elimination of autofluorescence, which commonly impairs the performance of fluorescence-based assays. UCPs are ideal donors for FRET, because their very narrow-banded emission allows measurement of the sensitized acceptor emission, in principle, without any crosstalk from the donor emission at a wavelength just tens of nanometers from the emission peak of the donor. In addition, acceptor dyes emitting at visible wavelengths are essentially not excited by near-infrared, which further emphasizes the unique potential of upconversion FRET (UC-FRET). These characteristics result in favorable assay performance using detection instrumentation based on epifluorometer configuration and laser diode excitation. Although UC-FRET is a recently emerged technology, it has already been applied in both immunoassays and nucleic acid hybridization assays. The technology is also compatible with optically difficult biological samples, such as whole blood. Significant advances in assay performance are expected using upconverting lanthanide-doped nanocrystals, which are currently under extensive research. UC-FRET, similarly to other fluorescence techniques based on resonance energy transfer, is strongly distance dependent and may have limited applicability, for example in sandwich-type assays for large biomolecules, such as viruses. In this article, we summarize the essentials of UC-FRET, describe its current applications, and outline the expectations for its future potential.

Multicolor tuning towards single red-emission band of upconversion nanoparticles for tunable optical component and optical/x-ray imaging agents via Ce(3+) doping.

PubMed

Yi, Zhigao; Zeng, Tianmei; Xu, Yaru; Lu, Wei; Qian, Chao; Liu, Hongrong; Zeng, Songjun; Hao, Jianhua

2015-09-25

A simple strategy of Ce(3+) doping is proposed to realize multicolor tuning and predominant red emission in BaLnF5:Yb(3+)/Ho(3+) (Ln(3+) = Gd(3+), Y(3+), Yb(3+)) systems. A tunable upconversion (UC) multicolor output from green/yellow to red can be readily achieved in a fixed Yb(3+)/Ho(3+) composition by doping Ce(3+), providing an effective route for multicolor tuning widely used for various optical components. Moreover, compared with Ce(3+)-free UC nanoparticles (UCNPs), a remarkable enhancement of the red-to-green (R/G) ratio is observed by doping 30% Ce(3+), arising from the two largely promoted cross-relaxation (CR) processes between Ce(3+) and Ho(3+). UCNPs with pure red emission are selected as in vivo UC bioimaging agents, demonstrating the merits of deep penetration depth, the absence of autofluorescence and high contrast in small animal bioimaging. Moreover, such fluorescence imaging nanoprobes can also be used as contrast agents for three-dimensional (3D) x-ray bioimaging by taking advantage of the high K-edge values and x-ray absorption coefficients of Ba(2+), Gd(3+), and Ce(3+) in our designed nanoprobes. Thus, the simultaneous realization of multicolor output, highly enhanced R/G ratio, and predominant red emission makes the Ce(3+)-doped UCNPs very useful for widespread applications in optical components and bioimaging.

Red-light-controllable liquid-crystal soft actuators via low-power excited upconversion based on triplet-triplet annihilation.

PubMed

Jiang, Zhen; Xu, Ming; Li, Fuyou; Yu, Yanlei

2013-11-06

A red-light-controllable soft actuator has been achieved, driven by low-power excited triplet-triplet annihilation-based upconversion luminescence (TTA-UCL). First, a red-to-blue TTA-based upconversion system with a high absolute quantum yield of 9.3 ± 0.5% was prepared by utilizing platinum(II) tetraphenyltetrabenzoporphyrin (PtTPBP) as the sensitizer and 9,10-bis(diphenylphosphoryl)anthracene (BDPPA) as the annihilator. In order to be employed as a highly effective phototrigger of photodeformable cross-linked liquid-crystal polymers (CLCPs), the PtTPBP&BDPPA system was incorporated into a rubbery polyurethane film and then assembled with an azotolane-containing CLCP film. The generating assembly film bent toward the light source when irradiated with a 635 nm laser at low power density of 200 mW cm(-2) because the TTA-UCL was effectively utilized by the azotolane moieties in the CLCP film, inducing their trans-cis photoisomerization and an alignment change of the mesogens via an emission-reabsorption process. It is the first example of a soft actuator in which the TTA-UCL is trapped and utilized to create photomechanical effect. Such advantages of using this novel red-light-controllable soft actuator in potential biological applications have also been demonstrated as negligible thermal effect and its excellent penetration ability into tissues. This work not only provides a novel photomanipulated soft actuation material system based on the TTA-UCL technology but also introduces a new technological application of the TTA-based upconversion system in photonic devices.

Comparative analysis of luminescent properties of germanate glass and double-clad optical fibers co-doped with Yb3+/Ho3+ ions

NASA Astrophysics Data System (ADS)

Pietrzycki, Marcin; Kochanowicz, Marcin; Romańczuk, Patryk; Żmojda, Jacek; Miluski, Piotr; Ragiń, Tomasz; Jeleń, Piotr; Sitarz, Maciej; Dorosz, Dominik

2016-09-01

The 2 μm and visible emission of low phonon (805 cm-1) germanate glasses and double - clad optical fiber co-doped with 0.7Yb2O3/(0.07-0.7)Ho2O3 ions have been investigated. Luminescence at 2 μm corresponding to Ho3+: 5I7 → 5I8 as well as upconversion luminescence in the visible spectral range corresponding to the Ho3+: 5S2(5F4)→5I8 (545 nm), and Ho3+: 5F5→5I8 (655 nm) transition, respectively were obtained. The optimization of the acceptor content and donor-acceptor ratio were conducted with the purpose of maximizing the luminescence intensity. The highest luminescence intensity in both spectral range was obtained in glass co-doped with 0.7Yb2O3/0.15 Ho2O3. Despite relatively small effective absorption coefficient of the optical fiber comparative analysis of luminescent properties of fabricated glasses (further core) and double - clad optical fiber showed significant contribution of reabsorption process of emitted ASE signal.

Enantiopure distorted ribbon-shaped nanographene combining two-photon absorption-based upconversion and circularly polarized luminescence.

PubMed

Cruz, Carlos M; Márquez, Irene R; Mariz, Inês F A; Blanco, Victor; Sánchez-Sánchez, Carlos; Sobrado, Jesús M; Martín-Gago, José A; Cuerva, Juan M; Maçôas, Ermelinda; Campaña, Araceli G

2018-04-28

Herein we describe a distorted ribbon-shaped nanographene exhibiting unprecedented combination of optical properties in graphene-related materials, namely upconversion based on two-photon absorption (TPA-UC) together with circularly polarized luminescence (CPL). The compound is a graphene molecule of ca. 2 nm length and 1 nm width with edge defects that promote the distortion of the otherwise planar lattice. The edge defects are an aromatic saddle-shaped ketone unit and a [5]carbohelicene moiety. This system is shown to combine two-photon absorption and circularly polarized luminescence and a remarkably long emission lifetime of 21.5 ns. The [5]helicene is responsible for the chiroptical activity while the push-pull geometry and the extended network of sp 2 carbons are factors favoring the nonlinear absorption. Electronic structure theoretical calculations support the interpretation of the results.

Aptamer-Mediated Up-conversion Core/MOF Shell Nanocomposites for Targeted Drug Delivery and Cell Imaging

PubMed Central

Deng, Kerong; Hou, Zhiyao; Li, Xuejiao; Li, Chunxia; Zhang, Yuanxin; Deng, Xiaoran; Cheng, Ziyong; Lin, Jun

2015-01-01

Multifunctional nanocarriers for targeted bioimaging and drug delivery have attracted much attention in early diagnosis and therapy of cancer. In this work, we develop a novel aptamer-guided nanocarrier based on the mesoporous metal-organic framework (MOF) shell and up-conversion luminescent NaYF4:Yb3+/Er3+ nanoparticles (UCNPs) core for the first time to achieve these goals. These UCNPs, chosen as optical labels in biological assays and medical imaging, could emit strong green emission under 980 nm laser. The MOF structure based on iron (III) carboxylate materials [MIL-100 (Fe)] possesses high porosity and non-toxicity, which is of great value as nanocarriers for drug storage/delivery. As a unique nanoplatform, the hybrid inorganic-organic drug delivery vehicles show great promising for simultaneous targeted labeling and therapy of cancer cells. PMID:25597762

Excited-state lifetime measurement of silicon vacancy centers in diamond by single-photon frequency upconversion

NASA Astrophysics Data System (ADS)

Rong, Youying; Ma, Jianhui; Chen, Lingxiao; Liu, Yan; Siyushev, Petr; Wu, Botao; Pan, Haifeng; Jelezko, Fedor; Wu, E.; Zeng, Heping

2018-05-01

We report a method with high time resolution to measure the excited-state lifetime of silicon vacancy centers in bulk diamond avoiding timing jitter from the single-photon detectors. Frequency upconversion of the fluorescence emitted from silicon vacancy centers was achieved from 738 nm to 436 nm via sum frequency generation with a short pump pulse. The excited-state lifetime can be obtained by measuring the intensity of upconverted light while the pump delay changes. As a probe, a pump laser with pulse duration of 11 ps provided a high temporal resolution of the measurement. The lifetime extracted from the pump–probe curve was 0.755 ns, which was comparable to the timing jitter of the single-photon detectors.

Energy Pooling Upconversion in Free Space and Optical Cavities

NASA Astrophysics Data System (ADS)

LaCount, Michael D.

The ability to efficiently convert the wavelength of light has value in a wide range of disciplines that include the fields of photovoltaics, plant growth, optics and medicine. The processes by which such transformations are carried out are known as upconversions and downconversions. There are several ways to up/down convert light, each with its own attributes, issues, and competing mechanisms. Most are associated with one-body or two-body processes. Three-body dynamics are also possible though, going by the names of quantum cutting (downconversion) and energy pooling (upconversion). These use virtual excited electronic states to mediate conversions as has been experimentally realized using lanthanide ions embedded in wide bandgap materials. The use of lanthanides to convert light is not ideal due to their relative scarcity, toxicity, and the limited range of light frequencies that can be absorbed and emitted. Organic molecules, on the other hand, are typically non-toxic, are made up of abundant elements, and can be designed with tailored spectral properties. At issue is whether or not they can be used to carry out efficient energy pooling, the central question to be answered in this thesis. The research presented here draws on a perturbative quantum electrodynamics framework previously established for generic energy pooling. It was used to develop a computational methodology for determining the rate of energy pooling and its competing processes. This, in turn, draws on a combination of time-dependent density functional theory, quantum electrodynamics, and perturbation theory to generate the requisite material property data. This computational model was applied to two test systems consisting of stilbene-fluorescein and hexabenzocoronene-oligothiophene. The stilbene-fluorescein system was found to have a maximum energy pooling rate efficiency (as compared to competing processes) of 17% and the hexabenzocoronene-oligothiophene system was found to have a maximum energy pooling rate efficiency of 99%. This demonstrates that the energy pooling rate can be made faster than its competing processes. Based on the results of this study, a set of design rules was developed to optimize the rate efficiency of energy pooling. Prior to this research, no attempt had been made to determine if energy pooling could be made to out-pace competing processes--i.e. whether or not a molecular system could be designed to utilize energy pooling as an efficient means of upconversion. This initial investigation was part of a larger effort involving a team of researchers at the University of Colorado, Boulder and at the National Renewable Energy Laboratory. After establishing our computational proof-of-concept, we collectively used the new design rules to select an improved system for energy pooling. This consisted of rhodamine 6G and stilbene-420. These molecules were fabricated into a thin film, and the maximum internal quantum yield was measured to be 36% under sufficiently high intensity light. To further increase the efficiency of energy pooling, encapsulation within optical cavities was considered as a way of changing the rate of processes characterized by electric dipole-dipole coupling. This was carried out using a combination of classical electromagnetism, quantum electrodynamics, and perturbation theory. It was found that, in the near field, if the distance of the energy transfer is smaller than the distance from the energy transfer site and the cavity wall, then the electric dipole-dipole coupling tensor is not influenced by the cavity environment and the rates of energy transfer processes are the same as those in free space. Any increase in energy transfer efficiencies that are experimentally measured must therefore be caused by changing the rate of light absorption and emission. This is an important finding because earlier, less rigorous studies had concluded otherwise. It has been previously demonstrated that an optical cavity can be used to inhibit the spontaneous emission of atoms or molecules placed within it. This too was examined as a possible means of increasing energy pooling efficiency. Using first-principles methods, quantum electrodynamics, perturbation theory, and a kinetic model, the efficiency of energy pooling upconversion within a tuned rectangular cavity was found to be significantly larger than in free space. A model system with a free-space energy pooling upconversion efficiency of 23% was found to increase to 47% when placed in a tuned rectangular cavity.

Near-field thermal upconversion and energy transfer through a Kerr medium.

PubMed

Khandekar, Chinmay; Rodriguez, Alejandro W

2017-09-18

We present an approach for achieving large Kerr χ (3) -mediated thermal energy transfer at the nanoscale that exploits a general coupled-mode description of triply resonant, four-wave mixing processes. We analyze the efficiency of thermal upconversion and energy transfer from mid- to near-infrared wavelengths in planar geometries involving two slabs supporting far-apart surface plasmon polaritons and separated by a nonlinear χ (3) medium that is irradiated by externally incident light. We study multiple geometric and material configurations and different classes of intervening mediums-either bulk or nanostructured lattices of nanoparticles embedded in nonlinear materials-designed to resonantly enhance the interaction of the incident light with thermal slab resonances. We find that even when the entire system is in thermodynamic equilibrium (at room temperature) and under typical drive intensities ~ W/μm 2 , the resulting upconversion rates can approach and even exceed thermal flux rates achieved in typical symmetric and non-equilibrium configurations of vacuum-separated slabs. The proposed nonlinear scheme could potentially be exploited to achieve thermal cooling and refrigeration at the nanoscale, and to actively control heat transfer between materials with dramatically different resonant responses.

A double responsive smart upconversion fluorescence sensing material for glycoprotein.

PubMed

Guo, Ting; Deng, Qiliang; Fang, Guozhen; Yun, Yaguang; Hu, Yongjin; Wang, Shuo

2016-11-15

A novel strategy was developed to prepare double responsive smart upconversion fluorescence material for highly specific enrichment and sensing of glycoprotein. The novel double responsive smart sensing material was synthesized by choosing Horse radish peroxidase (HRP) as modal protein, the grapheme oxide (GO) as support material, upconversion nanoparticles (UCNPs) as fluorescence signal reporter, N-isopropyl acrylamide (NIPAAM) and 4-vinylphenylboronic acid (VPBA) as functional monomers. The structure and component of smart sensing material was investigated by transmission electron microscopy (TEM), Scanning electron microscopy (SEM), X-ray photoelectron spectroscopic (XPS) and Fourier transform infrared (FTIR), respectively. These results illustrated the smart sensing material was prepared successfully. The recognition characterizations of smart sensing material were evaluated, and results showed that the fluorescence intensity of smart sensing material was reduced gradually, as the concentration of protein increased, and the smart sensing material showed selective recognition for HRP among other proteins. Furthermore, the recognition ability of the smart sensing material for glycoprotein was regulated by controlling the pH value and temperature. Therefore, this strategy opens up new way to construct smart material for detection of glycoprotein. Copyright © 2016 Elsevier B.V. All rights reserved.

Nano-optomechanical transducer

DOEpatents

Rakich, Peter T; El-Kady, Ihab F; Olsson, Roy H; Su, Mehmet Fatih; Reinke, Charles; Camacho, Ryan; Wang, Zheng; Davids, Paul

2013-12-03

A nano-optomechanical transducer provides ultrabroadband coherent optomechanical transduction based on Mach-wave emission that uses enhanced photon-phonon coupling efficiencies by low impedance effective phononic medium, both electrostriction and radiation pressure to boost and tailor optomechanical forces, and highly dispersive electromagnetic modes that amplify both electrostriction and radiation pressure. The optomechanical transducer provides a large operating bandwidth and high efficiency while simultaneously having a small size and minimal power consumption, enabling a host of transformative phonon and signal processing capabilities. These capabilities include optomechanical transduction via pulsed phonon emission and up-conversion, broadband stimulated phonon emission and amplification, picosecond pulsed phonon lasers, broadband phononic modulators, and ultrahigh bandwidth true time delay and signal processing technologies.

Tuning donut profile for spatial resolution in stimulated emission depletion microscopy.

PubMed

Neupane, Bhanu; Chen, Fang; Sun, Wei; Chiu, Daniel T; Wang, Gufeng

2013-04-01

In stimulated emission depletion (STED)-based or up-conversion depletion-based super-resolution optical microscopy, the donut-shaped depletion beam profile is of critical importance to its resolution. In this study, we investigate the transformation of the donut-shaped depletion beam focused by a high numerical aperture (NA) microscope objective, and model STED point spread function (PSF) as a function of donut beam profile. We show experimentally that the intensity profile of the dark kernel of the donut can be approximated as a parabolic function, whose slope is determined by the donut beam size before the objective back aperture, or the effective NA. Based on this, we derive the mathematical expression for continuous wave (CW) STED PSF as a function of focal plane donut and excitation beam profiles, as well as dye properties. We find that the effective NA and the residual intensity at the center are critical factors for STED imaging quality and the resolution. The effective NA is critical for STED resolution in that it not only determines the donut shape but also the area the depletion laser power is dispersed. An improperly expanded depletion beam will have negligible improvement in resolution. The polarization of the depletion beam also plays an important role as it affects the residual intensity in the center of the donut. Finally, we construct a CW STED microscope operating at 488 nm excitation and 592 nm depletion with a resolution of 70 nm. Our study provides detailed insight to the property of donut beam, and parameters that are important for the optimal performance of STED microscopes. This paper will provide a useful guide for the construction and future development of STED microscopes.

Yttrium orthoaluminate nanoperovskite doped with Tm3+ ions as upconversion optical temperature sensor in the near-infrared region.

PubMed

Hernández-Rodriguez, M A; Lozano-Gorrín, A D; Lavín, V; Rodríguez-Mendoza, U R; Martín, I R

2017-10-30

The thermal sensing capability of the Tm 3+ -doped yttrium orthoaluminate nanoperovskite in the infrared range, synthetized by a sol-gel method, was studied. The temperature dependence of the infrared upconverted emission bands located at around 705 nm ( 3 F 2,3 → 3 H 6 ) and 800 nm ( 3 H 4 → 3 H 6 ) of YAP: Tm 3+ nanoperovskite under excitation at 1210 nm was analyzed from RT up to 425 K. Calibration of the optical sensor has been made using the fluorescence intensity ratio technique, showing a high sensitivity in the near-infrared compared to other trivalent rare-earth based optical sensors working in the same range. In addition, a second calibration procedure of the YAP: Tm 3+ optical sensor was performed by using the FIR technique on the emission band associated to the 3 H 4 → 3 H 6 transition in the physiological temperature range (293-333 K), showing a very high relative sensitivity compared with other rare-earth based optical temperature sensors working in the physiological range. Moreover, the main advantage compared with other optical sensors is that the excitation source and the upconverted emissions do not overlap, since they lie in different biological windows, thus allowing its potential use as an optical temperature probe in the near-infrared range for biological applications.

Tunable multicolor and enhanced red emission of monodisperse CaF2:Yb3+/Ho3+ microspheres via Mn2+ doping

NASA Astrophysics Data System (ADS)

Wang, Rui; Yuan, Maohui; Zhang, Chaofan; Wang, Hongyan; Xu, Xiaojun

2018-05-01

Transition metal ions (e.g. Mn2+) and lanthanide co-doped upconversion (UC) materials have attracted wide attention in recent years due to their promising application in multicolor display. Here, we report the hydrothermal synthesis and characterization of Mn2+ doped monodisperse CaF2:Yb3+/Ho3+ microspheres. The results of X-ray diffraction (XRD) revealed that Mn2+ doping does not change the cubic phase of CaF2 material but will lead to diffraction peaks shifting slightly towards higher angle due to the substitution of larger Ca2+ by the relatively smaller Mn2+. Under the excitation of 980 nm continuous wave (CW) laser, these microspheres exhibit green-yellow-red tuning colors and remarkable enhancement of both red to green ratio (R/G) and red to blue ratio (R/B) when increasing Mn2+ concentration from 0 to 30 mol%. The energy migration process between Ho3+ and Mn2+ was proposed and supported by time-decay and power dependence measurements of Ho3+ UC emission. These upconversion materials may have potential applications in optical devices, color display, nanoscale lasers and biomedical imaging.

Role of Gd{sup 3+} ion on downshifting and upconversion emission properties of Pr{sup 3+}, Yb{sup 3+} co-doped YNbO{sub 4} phosphor and sensitization effect of Bi{sup 3+} ion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dwivedi, A.; Rai, S. B., E-mail: sbrai49@yahoo.co.in; Mishra, Kavita

Dual-mode luminescence (downshifting-DS and upconversion-UC) properties of Pr{sup 3+}/Yb{sup 3+} co-doped Y{sub 1−x}Gd{sub x}NbO{sub 4} (x = 0.0, 0.5, and 1.0) phosphors synthesized by solid state reaction technique have been explored with and without Gd{sup 3+} ion. The structural characterizations (XRD, SEM, and FTIR) confirm the pure phase of YNbO{sub 4} phosphor. Further, with the Gd{sup 3+} ion co-doping, the YNbO{sub 4} phosphors having a random shape and the large particle size are found to be transformed into nearly spherical shape particles with the reduced particle size. The optical band gaps (E{sub g}) of Y{sub 1−x}Gd{sub x}NbO{sub 4} (x = 0.00, 0.25, 0.50, andmore » 1.00) calculated from UV-Vis-NIR measurements are ∼3.69, 4.00, 4.38, and 4.44 eV, respectively. Moreover, YNbO{sub 4} phosphor is a promising blue emitting material, whereas Y{sub 1−x−y−z}Pr{sub y}Yb{sub z}Gd{sub x}NbO{sub 4} phosphor gives intense green, blue, and red emissions via dual-mode optical processes. The broad blue emission arises due to (NbO{sub 4}){sup 3−} group of the host with λ{sub ex} = 264 nm, whereas Pr{sup 3+} doped YNbO{sub 4} phosphor gives dominant red and blue emissions along with comparatively weak green emission on excitation with λ{sub ex} = 300 nm and 491 nm. The concentration dependent variation in emission intensity at 491 nm ({sup 3}P{sub 0}→{sup 3}H{sub 4} transition) and 612 nm ({sup 1}D{sub 2}→{sup 3}H{sub 4} transition); at 612 nm ({sup 1}D{sub 2}→{sup 3}H{sub 4} transition) and 658 nm ({sup 3}P{sub 0}→{sup 3}F{sub 2} transition) of Pr{sup 3+} ion in YNbO{sub 4} phosphor with λ{sub ex} = 300 nm and 491 nm excitations, respectively, has been thoroughly explored and explained by the cross-relaxation process through different channels. The sensitization effect of Bi{sup 3+} ion co-doping on DS properties of the phosphor has also been studied. The observed DS results have been optimized by varying the concentration of Pr{sup 3+} and Bi{sup 3+} ions, and the results are explained by the well-known simple band structure model. The study of Gd{sup 3+} co-doping reveals noticeable differences in DS characteristics of Y{sub 1−x}Pr{sub x}NbO{sub 4} phosphors: the overall decrement and increment (except for 612 nm emission) in intensity of DS emission on excitation with λ{sub ex} = 264 nm and 491 nm, respectively. These observations have been thoroughly explained, and the {sup 1}D{sub 2}→{sup 3}H{sub 4} transition (612 nm) of Pr{sup 3+} ion is found to be strongly dependent on surrounding environment of the host matrix. The UC properties of Y{sub 0.95−x}Pr{sub x}Yb{sub 0.05}NbO{sub 4} phosphors have been explored using Near Infra-Red (NIR) excitation. The material gives intense green and relatively weak blue and red UC emissions with λ{sub ex} = 980 nm. Interestingly, the UC emission intensity is further enhanced in the case of Y{sub 0.949−x}Pr{sub 0.001}Yb{sub 0.05}Gd{sub x}NbO{sub 4} phosphors. In addition, the less explored laser induced heating effect with the pump power as well as the irradiation time on the UC emission has been explored in Y{sub 0.949−x}Pr{sub 0.001}Yb{sub 0.05}Gd{sub x}NbO{sub 4} (x = 0, 0.5, and 0.949) phosphor samples, and subsequently, this feature has been found to be superior for Gd{sub 0.949}Pr{sub 0.001}Yb{sub 0.05}NbO{sub 4} phosphor. The comparative study between the two hosts, viz., YNbO{sub 4} and GdNbO{sub 4} shows that GdNbO{sub 4} is better than YNbO{sub 4} for UC emission behavior; however, a reverse is observed as for as DS behavior is concerned only for the particular excitation wavelength (λ{sub ex} = 264 nm).« less

Luminescence in Conjugated Molecular Materials under Sub-bandgap Excitation

DOE Office of Scientific and Technical Information (OSTI.GOV)

So, Franky

2014-05-08

Light emission in semiconductors occurs when they are under optical and electrical excitation with energy larger than the bandgap energy. In some low-dimensional semiconductor heterostructure systems, this thermodynamic limit can be violated due to radiative Auger recombination (AR), a process in which the sub-bandgap energy released from a recombined electron-hole pair is transferred to a third particle leading to radiative band-to-band recombination.1 Thus far, photoluminescence up-conversion phenomenon has been observed in some low dimensional semiconductor systems, and the effect is very weak and it can only be observed at low temperatures. Recently, we discovered that efficient electroluminescence in poly[2-methoxy-5-(2’-ethylhexyloxy)-1, phenylenevinylene]more » (MEH-PPV) polymer light-emitting devices (PLEDs) at drive voltages below its bandgap voltage could be observed when a ZnO nanoparticles (NPs) electron injection layer was inserted between the polymer and the aluminum electrode. Specifically, emitted photons with energy of 2.13 eV can be detected at operating voltages as low as 1.2 V at room temperature. Based on these data, we propose that the sub-bandgap turn-on in the MEH-PPV device is due to an Auger-assisted energy up-conversion process. The significance of this discovery is three-fold. First, radiative recombination occurs at operating voltages below the thermodynamic bandgap voltage. This process can significantly reduce the device operating voltage. For example, the current density of the device with the ZnO NC layer is almost two orders of magnitude higher than that of the device without the NC layer. Second, a reactive metal is no longer needed for the cathode. Third, this electroluminescence up-conversion process can be applied to inorganic semiconductors systems as well and their operation voltages of inorganic LEDs can be reduced to about half of the bandgap energy. Based on our initial data, we propose that the sub-bandgap turn-on in MEH-PPV devices is due to Auger-assisted energy up-conversion process. Specifically, we propose that the up-conversion process is due to charge accumulation at the polymer/NPs interface. This model requires that holes should be the dominant carriers in the polymer and the polymer/ZnO NCs heterojunction should be a type II alignment. In order to determine the mechanism of the up-conversion process, we will characterize devices fabricated using polymers with different carrier transporting properties to determine whether hole accumulation at the polymer/nanocrystals is required. Likewise, we will also use NPs with different electronic structures to fabricate devices to determine how electron accumulation affects the up-conversion process. Finally, we will measure quantitatively the interface charge accumulation by electroabsorption and correlate the results with the up-conversion photoluminescence efficiency measurements under an applied electric field.« less

Photon up-conversion increases biomass yield in Chlorella vulgaris.

PubMed

Menon, Kavya R; Jose, Steffi; Suraishkumar, Gadi K

2014-12-01

Photon up-conversion, a process whereby lower energy radiations are converted to higher energy levels via the use of appropriate phosphor systems, was employed as a novel strategy for improving microalgal growth and lipid productivity. Photon up-conversion enables the utilization of regions of the solar spectrum, beyond the typical photosynthetically active radiation, that are usually wasted or are damaging to the algae. The effects of up-conversion of red light by two distinct sets of up-conversion phosphors were studied in the model microalgae Chlorella vulgaris. Up-conversion by set 1 phosphors led to a 2.85 fold increase in biomass concentration and a 3.2 fold increase in specific growth rate of the microalgae. While up-conversion by set 2 phosphors resulted in a 30% increase in biomass and 12% increase in specific intracellular neutral lipid, while the specific growth rates were comparable to that of the control. Furthermore, up-conversion resulted in higher levels of specific intracellular reactive oxygen species in C. vulgaris. Up-conversion of red light (654 nm) was shown to improve biomass yields in C. vulgaris. In principle, up-conversion can be used to increase the utilization range of the electromagnetic spectrum for improved cultivation of photosynthetic systems such as plants, algae, and microalgae. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

PEGylated NaLuF4: Yb/Er upconversion nanophosphors for in vivo synergistic fluorescence/X-ray bioimaging and long-lasting, real-time tracking.

PubMed

Yi, Zhigao; Lu, Wei; Xu, Yaru; Yang, Jing; Deng, Li; Qian, Chao; Zeng, Tianmei; Wang, Haibo; Rao, Ling; Liu, Hongrong; Zeng, Songjun

2014-12-01

Simultaneous in vivo luminescence and X-ray bioimaging in a tissue or animal integrates the advantages of each single-modal imaging technology, and will find widespread application in biological and clinical fields. However, synergistic dual-modal bioimaging that utilizes a new generation of upconversion nanoprobes is still limited. In addition, investigations concentrated on in vivo biodistribution of these nanoprobes may contribute to diagnosis and treatment, but long-term in vivo tracking based on these nanoprobes is rarely reported. In this work, water-soluble NaLuF4: Yb/Er nanophosphors were prepared through modified one-pot simultaneous synthesis and surface modification method. Owing to the outstanding upconverting emissions and large X-ray absorption coefficient/K-edge value of Lu and doped Yb ions, the obtained nanoprobes were successfully used as luminescent nanoprobes and X-ray contrast agents for in vivo synergistic upconversion luminescence and X-ray bioimaging. The in vivo biodistribution of these nanoprobes were observed, and the results based on long-term tracking reveal that the as-prepared nanoprobes first aggregated in the lung of the mouse, transferred to the liver, and finally moved to the spleen. Copyright © 2014 Elsevier Ltd. All rights reserved.

Water-stable NaLuF4-based upconversion nanophosphors with long-term validity for multimodal lymphatic imaging.

PubMed

Zhou, Jing; Zhu, Xingjun; Chen, Min; Sun, Yun; Li, Fuyou

2012-09-01

Multimodal imaging is rapidly becoming an important tool for biomedical applications because it can compensate for the deficiencies of individual imaging modalities. Herein, multifunctional NaLuF(4)-based upconversion nanoparticles (Lu-UCNPs) were synthesized though a facile one-step microemulsion method under ambient condition. The doping of lanthanide ions (Gd(3+), Yb(3+) and Er(3+)/Tm(3+)) endows the Lu-UCNPs with high T(1)-enhancement, bright upconversion luminescence (UCL) emissions, and excellent X-ray absorption coefficient. Moreover, the as-prepared Lu-UCNPs are stable in water for more than six months, due to the protection of sodium glutamate and diethylene triamine pentacetate acid (DTPA) coordinating ligands on the surface. Lu-UCNPs have been successfully applied to the trimodal CT/MR/UCL lymphatic imaging on the modal of small animals. It is worth noting that Lu-UCNPs could be used for imaging even after preserving for over six months. In vitro transmission electron microscope (TEM), methyl thiazolyl tetrazolium (MTT) assay and histological analysis demonstrated that Lu-UCNPs exhibited low toxicity on living systems. Therefore, Lu-UCNPs could be multimodal agents for CT/MR/UCL imaging, and the concept can be served as a platform technology for the next-generation of probes for multimodal imaging. Copyright © 2012 Elsevier Ltd. All rights reserved.

Structural, optical and photo thermal properties of Er3+:Y2O3 doped PMMA nanocomposite

NASA Astrophysics Data System (ADS)

Tabanli, Sevcan; Eryurek, Gonul

2018-02-01

Thermal decomposition technique was employed to synthesize of phosphors of yttria (Y2O3) doped with erbium (Er3+) ions. After the synthesized procedure, the nano-sized crystalline powders were annealed at 800oC for 24 h. Annealed powders were embedded in poly(methyl methacrylate) (PMMA) by free radical polymerization to fabricate nanocomposite polymer materials. The crystalline structure of the powder and doped PMMA nanocomposite samples were determined using X-ray diffraction technique. Scherrer's equation and the FW1/5/4/5M method were used to determine average crystalline size and grain size distributions, respectively. The spectroscopic properties of the powders and doped PMMA nanocomposites were studied by measuring the upconversion emission spectra under near-infrared laser excitation at room temperature. The laser-induced photo thermal behaviors of Er3+:Y2O3 nano-powders and doped PMMA nanocomposite were investigated using the fluorescence intensity ratio (FIR) technique.

Bifunction in Er{sup 3+}/Yb{sup 3+} co-doped BaTi{sub 2}O{sub 5}–Gd{sub 2}O{sub 3} glasses prepared by aerodynamic levitation method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Minghui; University of Chinese Academy of Sciences, Beijing 100039; Yu, Jianding

2013-11-15

Graphical abstract: - Highlights: • Novel BaTi{sub 2}O{sub 5}–Gd{sub 2}O{sub 3} based glasses have been prepared by aerodynamic levitation. • The obtained glasses show high thermal stability with T{sub g} = 763.3 °C. • Er{sup 3+}/Yb{sup 3+} co-doped glasses show strong upconversion based on a two-photon process. • Red emission is stronger than green emissions for EBT by high Yb{sup 3+} concentration. • Magnetic ions are paramagnetic and the distribution is homogeneous in the glasses. - Abstract: Novel Er{sup 3+}/Yb{sup 3+} co-doped BaTi{sub 2}O{sub 5}–Gd{sub 2}O{sub 3} spherical glasses have been fabricated by aerodynamic levitation method. The thermal stability, upconversionmore » luminescence, and magnetic properties of the present glass have been studied. The glasses show high thermal stability with 763.3 °C of the onset temperature of the glass transition. Red and green emissions centered at 671 nm, 548 nm and 535 nm are obtained at 980 nm excitation. The upconversion is based on a two-photon process by energy transfer, excited-state absorption, and energy back transfer. Yb{sup 3+} ions are more than Er{sup 3+} ions in the glass, resulting in efficient energy back transfer from Er{sup 3+} to Yb{sup 3+}. So the red emission is stronger than the green emissions. Magnetization curves indicate that magnetic rare earth ions are paramagnetic and the distribution is homogeneous and random in the glass matrix. Aerodynamic levitation method is an efficient way to prepare glasses with homogeneous rare earth ions.« less

Study of broadband near-infrared emission in Tm3+-Er3+ codoped TeO2-WO3-PbO glasses.

PubMed

Balda, R; Fernández, J; Fernández-Navarro, J M

2009-05-25

In this work, we report the near-infrared emission properties of Tm(3+)-Er(3+) codoped tellurite TeO(2)-WO(3)-PbO glasses under 794 nm excitation. A broad emission from 1350 to 1750 nm corresponding to the Tm(3+) and Er(3+) emissions is observed. The full width at half-maximum of this broadband increases with increasing [Tm]/[Er] concentration ratio up to a value of ~ 160 nm. The energy transfer between Tm(3+) and Er(3+) ions is evidenced by both the temporal behavior of the near-infrared luminescence and the effect of Tm3+ codoping on the visible upconversion of Er(3+) ions.

Infrared upconversion for astronomy

NASA Technical Reports Server (NTRS)

Boyd, R. W.

1977-01-01

The basic theory of upconversion is presented, along with a brief historical summary of upconversion techniques. Upconverters were used in astronomical studies, but have met with only modest success. Upconversion will become a useful detection method for astronomy only if substantial but perhaps forseeable, improvements can be realized.

Luminescence upconversion under hydrostatic pressure in the 3d-metal systems Ti2+:NaCl and Ni2+:CsCdCl3

NASA Astrophysics Data System (ADS)

Wenger, Oliver S.; Salley, G. Mackay; Valiente, Rafael; Güdel, Hans U.

2002-06-01

We present a study of upconversion materials and processes under external hydrostatic pressure. The near-infrared to visible photon upconversion properties of Ti2+-doped NaCl and Ni2+-doped CsCdCl3 at 15 K are studied as a function of external hydrostatic pressure. It is found that in Ti2+:NaCl pressure can be used to switch on an efficient upconversion mechanism, which is inactive at ambient pressure, leading to an order-of-magnitude enhancement of the overall upconversion efficiency of this material. For Ni2+:CsCdCl3 it is demonstrated that upconversion luminescence excitation spectroscopy can be used to study the pressure dependence of excited state absorption transitions. The results demonstrate the ability to tune upconversion properties by altering the local crystal field of active ions, in addition to probing the pressure dependence of excited state absorption transitions via upconversion spectroscopy.

Current Advances in Lanthanide‐Doped Upconversion Nanostructures for Detection and Bioapplication

PubMed Central

Chen, Cailing

2016-01-01

Along with the development of science and technology, lanthanide‐doped upconversion nanostructures as a new type of materials have taken their place in the field of nanomaterials. Upconversion luminescence is a nonlinear optical phenomenon, which absorbs two or more photons and emits one photon. Compared with traditional luminescence materials, upconversion nanostructures have many advantages, such as weak background interference, long lifetime, low excitation energy, and strong tissue penetration. These interesting nanostructures can be applied in anticounterfeit, solar cell, detection, bioimaging, therapy, and so on. This review is focused on the current advances in lanthanide‐doped upconversion nanostructures, covering not only basic luminescence mechanism, synthesis, and modification methods but also the design and fabrication of upconversion nanostructures, like core–shell nanoparticles or nanocomposites. At last, this review emphasizes the application of upconversion nanostructure in detection and bioimaging and therapy. Learning more about the advances of upconversion nanostructures can help us better exploit their excellent performance and use them in practice. PMID:27840794

Femtowatt incoherent image conversion from mid-infrared light to near-infrared light

NASA Astrophysics Data System (ADS)

Huang, Nan; Liu, Hongjun; Wang, Zhaolu; Han, Jing; Zhang, Shuan

2017-03-01

We report on the experimental conversion imaging of an incoherent continuous-wave dim source from mid-infrared light to near-infrared light with a lowest input power of 31 femtowatt (fW). Incoherent mid-infrared images of light emission from a heat lamp bulb with an adjustable power supply at window wavelengths ranging from 2.9 µm to 3.5 µm are used for upconversion. The sum-frequency generation is realized in a laser cavity with the resonant wavelength of 1064 nm pumped by an LD at 806 nm built around a periodically poled lithium niobate (PPLN) crystal. The converted infrared image in the wavelength range ~785 nm with a resolution of about 120  ×  70 is low-noise detected using a silicon-based camera. By optimizing the system parameters, the upconversion quantum efficiency is predicted to be 28% for correctly polarized, on-axis and phase-matching light.

Distance-dependent plasmon-enhanced fluorescence of upconversion nanoparticles using polyelectrolyte multilayers as tunable spacers.

PubMed

Feng, Ai Ling; You, Min Li; Tian, Limei; Singamaneni, Srikanth; Liu, Ming; Duan, Zhenfeng; Lu, Tian Jian; Xu, Feng; Lin, Min

2015-01-14

Lanthanide-doped upconversion nanoparticles (UCNPs) have attracted widespread interests in bioapplications due to their unique optical properties by converting near infrared excitation to visible emission. However, relatively low quantum yield prompts a need for developing methods for fluorescence enhancement. Plasmon nanostructures are known to efficiently enhance fluorescence of the surrounding fluorophores by acting as nanoantennae to focus electric field into nano-volume. Here, we reported a novel plasmon-enhanced fluorescence system in which the distance between UCNPs and nanoantennae (gold nanorods, AuNRs) was precisely tuned by using layer-by-layer assembled polyelectrolyte multilayers as spacers. By modulating the aspect ratio of AuNRs, localized surface plasmon resonance (LSPR) wavelength at 980 nm was obtained, matching the native excitation of UCNPs resulting in maximum enhancement of 22.6-fold with 8 nm spacer thickness. These findings provide a unique platform for exploring hybrid nanostructures composed of UCNPs and plasmonic nanostructures in bioimaging applications.

Ln(3+)-doped nanoparticles for upconversion and magnetic resonance imaging: some critical notes on recent progress and some aspects to be considered.

PubMed

van Veggel, Frank C J M; Dong, Cunhai; Johnson, Noah J J; Pichaandi, Jothirmayanantham

2012-12-07

In this feature article we will critically discuss the synthesis and characterisation aspects of Ln(3+)-doped nanoparticles (NPs) that show upconversion, upon 980 nm excitation. Upconversion is a non-linear process that converts two or more low-energy photons, often near-infrared photons, into one of higher energy, e.g. blue and 800 nm from Tm(3+) and green and red from Er(3+) or Ho(3+). Nearly all researchers use the absorption of 980 nm light by Yb(3+) as the sensitiser for the co-doped emissive Ln(3+) ions. The focus will be on LnF(3) and MLnF(4) (M = alkali metal) as the host matrix, because most progress has been made with these. In particular we will argue that a detailed understanding of how the dopant ions and the host Ln(3+) ions are distributed (in the core) and how (doped) shell growth occurs is not well understood. Moreover, their use as optical and magnetic resonance imaging contrast agents will be discussed. We will argue that deep-tissue imaging beyond 600 μm with retention of optical resolution, i.e. to see fine structure such as blood capillaries in brain tissues, has not yet been achieved. Three key parameters have been identified as impediments: (i) the low absorption efficiency of the Yb(3+) sensitiser, (ii) the low quantum yield of upconversion, and (iii) the long-lived excited states. On the other hand, there are very encouraging results that suggest that these nanoparticles could be developed into very potent magnetic resonance imaging (MRI) contrast agents.

Efficient upconversion polymer-inorganic nanocomposite thin film emitters prepared by the double beam matrix assisted pulsed laser evaporation (DB-MAPLE)

NASA Astrophysics Data System (ADS)

Darwish, Abdalla M.; Burkett, Allan; Blackwell, Ashley; Taylor, Keylantra; Walker, Vernell; Sarkisov, Sergey; Koplitz, Brent

2014-09-01

We report on fabrication and investigation of optical and morphological properties of highly efficient (a quantum yield of 1%) upconversion polymer-inorganic nanocomposite thin film emitters prepared by the new technique of double beam matrix assisted pulsed laser evaporation (DB-MAPLE). Polymer poly(methyl methacrylate) (PMMA) host was evaporated on a silicon substrate using a 1064-nm pulsed laser beam using a target made of frozen (to the temperature of liquid nitrogen) solution of PMMA in chlorobenzene. Concurrently, the second 532-nm pulsed beam from the same laser was used to impregnate the polymer host with the inorganic nanoparticulate made of the rare earth upconversion compounds NaYF4: Yb3+, Er3+, NaYF4: Yb3+, Ho3+, and NaYF4: Yb3+, Tm3+. The compounds were initially synthesized using the wet process, baked, and compressed in solid pellet targets. The proposed DB-MAPLE method has the advantage of making highly homogeneous nanocomposite films with precise control of the doping rate due to the optimized overlapping of the plumes produced by the ablation of the organic and inorganic target with the infrared and visible laser beams respectively. X-ray diffraction, electron and atomic force microscopy, and optical fluorescence spectroscopy indicated that the inorganic nanoparticulate preserved its crystalline structure and upconversion properties (strong emission in green, red, and blue bands upon illumination with 980-nm laser diode) after being transferred from the target in the polymer nanocomposite film. The produced films can be used in applications varying from the efficiency enhancement of the photovoltaic cells, optical sensors and biomarkers to anti-counterfeit labels.

Ln3+-doped nanoparticles for upconversion and magnetic resonance imaging: some critical notes on recent progress and some aspects to be considered

NASA Astrophysics Data System (ADS)

van Veggel, Frank C. J. M.; Dong, Cunhai; Johnson, Noah J. J.; Pichaandi, Jothirmayanantham

2012-11-01

In this feature article we will critically discuss the synthesis and characterisation aspects of Ln3+-doped nanoparticles (NPs) that show upconversion, upon 980 nm excitation. Upconversion is a non-linear process that converts two or more low-energy photons, often near-infrared photons, into one of higher energy, e.g. blue and 800 nm from Tm3+ and green and red from Er3+ or Ho3+. Nearly all researchers use the absorption of 980 nm light by Yb3+ as the sensitiser for the co-doped emissive Ln3+ ions. The focus will be on LnF3 and MLnF4 (M = alkali metal) as the host matrix, because most progress has been made with these. In particular we will argue that a detailed understanding of how the dopant ions and the host Ln3+ ions are distributed (in the core) and how (doped) shell growth occurs is not well understood. Moreover, their use as optical and magnetic resonance imaging contrast agents will be discussed. We will argue that deep-tissue imaging beyond 600 μm with retention of optical resolution, i.e. to see fine structure such as blood capillaries in brain tissues, has not yet been achieved. Three key parameters have been identified as impediments: (i) the low absorption efficiency of the Yb3+ sensitiser, (ii) the low quantum yield of upconversion, and (iii) the long-lived excited states. On the other hand, there are very encouraging results that suggest that these nanoparticles could be developed into very potent magnetic resonance imaging (MRI) contrast agents.

Low-frequency wideband vibration energy harvesting by using frequency up-conversion and quin-stable nonlinearity

NASA Astrophysics Data System (ADS)

Wang, Chen; Zhang, Qichang; Wang, Wei

2017-07-01

This work presents models and experiments of an impact-driven and frequency up-converted wideband piezoelectric-based vibration energy harvester with a quintuple-well potential induced by the combination effect of magnetic nonlinearity and mechanical piecewise-linearity. Analysis shows that the interwell motions during coupled vibration period enable to increase electrical power output in comparison to conventional frequency up-conversion technology. Besides, the quintuple-well potential with shallower potential wells could extend the harvester's operating bandwidth to lower frequencies. Experiments demonstrate our proposed approach can dramatically boost the measured power of the energy harvester as much as 35 times while its lower cut-off frequency is two times lower than that of a conventional counterpart. These results reveal our proposed approach shows promise for powering portable wireless smart devices from low-intensity, low-frequency vibration sources.

In vivo 808 nm image-guided photodynamic therapy based on an upconversion theranostic nanoplatform

NASA Astrophysics Data System (ADS)

Liu, Xiaomin; Que, Ivo; Kong, Xianggui; Zhang, Youlin; Tu, Langping; Chang, Yulei; Wang, Tong Tong; Chan, Alan; Löwik, Clemens W. G. M.; Zhang, Hong

2015-09-01

A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the 1O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, 1O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm-2) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy.A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the 1O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, 1O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm-2) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr03690a

A new near infrared photosensitizing nanoplatform containing blue-emitting up-conversion nanoparticles and hypocrellin A for photodynamic therapy of cancer cells

NASA Astrophysics Data System (ADS)

Jin, Shan; Zhou, Liangjun; Gu, Zhanjun; Tian, Gan; Yan, Liang; Ren, Wenlu; Yin, Wenyan; Liu, Xiaodong; Zhang, Xiao; Hu, Zhongbo; Zhao, Yuliang

2013-11-01

The utilization of up-conversion nanoparticles (UCNPs) for photodynamic therapy (PDT) has gained significant interest due to their unique ability to convert near infrared light to UV/visible light. Previous work mainly focused on the fabrication of green and red emitting UCNPs to load photosensitizers (PSs) for PDT. In this work, we firstly developed a new multifunctional nanoplatform combining blue-emitting UCNPs with blue-light excited PS (hypocrellin A, HA) as a NIR photosensitizing nanoplatform for PDT of cancer cells. Tween 20 coated NaYbF4:Tm, Gd@NaGdF4 UCNPs (Tween 20-UCNPs) with strong blue up-conversion luminescence and good water dispersibility were prepared for use as PS carriers. The blue emission band matched well with the efficient absorption band of HA, thereby facilitating the resonance energy transfer from UCNPs to HA and then activating HA to produce singlet oxygen (1O2). The in vitro study showed that these Tween 20-UCNPs@HA complexes could efficiently produce 1O2 to kill cancer cells under 980 nm NIR excitation. Moreover, these Gd3+ and Yb3+ containing nanoparticles also exhibited positive contrast effects in both T1 weighted magnetic resonance imaging (MRI) and computed tomography (CT) imaging, making them become a multifunctional platform for simultaneous PDT and bio-imaging.The utilization of up-conversion nanoparticles (UCNPs) for photodynamic therapy (PDT) has gained significant interest due to their unique ability to convert near infrared light to UV/visible light. Previous work mainly focused on the fabrication of green and red emitting UCNPs to load photosensitizers (PSs) for PDT. In this work, we firstly developed a new multifunctional nanoplatform combining blue-emitting UCNPs with blue-light excited PS (hypocrellin A, HA) as a NIR photosensitizing nanoplatform for PDT of cancer cells. Tween 20 coated NaYbF4:Tm, Gd@NaGdF4 UCNPs (Tween 20-UCNPs) with strong blue up-conversion luminescence and good water dispersibility were prepared for use as PS carriers. The blue emission band matched well with the efficient absorption band of HA, thereby facilitating the resonance energy transfer from UCNPs to HA and then activating HA to produce singlet oxygen (1O2). The in vitro study showed that these Tween 20-UCNPs@HA complexes could efficiently produce 1O2 to kill cancer cells under 980 nm NIR excitation. Moreover, these Gd3+ and Yb3+ containing nanoparticles also exhibited positive contrast effects in both T1 weighted magnetic resonance imaging (MRI) and computed tomography (CT) imaging, making them become a multifunctional platform for simultaneous PDT and bio-imaging. Electronic supplementary information (ESI) available. See DOI: 10.1039/c3nr03515h

Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications

DOE PAGES

Wu, Xiang; Zhang, Yuanwei; Takle, Kendra; ...

2016-01-06

A near-infrared (NIR) dye-sensitized upconversion nanoparticles (UCNPs) can broaden the absorption range and boost upconversion efficiency of UCNPs. We achieved significantly enhanced upconversion luminescence in dye-sensitized core/active shell UCNPs via the doping of ytterbium ions (Yb 3+ ) in the UCNP shell, which bridged the energy transfer from the dye to the UCNP core. As a result, we synergized the two most practical upconversion booster effectors (dye-sensitizing and core/shell enhancement) to amplify upconversion efficiency. We also demonstrated two biomedical applications using these UCNPs. By using dye-sensitized core/active shell UCNP embedded poly(methyl methacrylate) polymer implantable systems, we successfully shifted the optogeneticmore » neuron excitation window to a biocompatible and deep tissue penetrable 800 nm wavelength. Furthermore, UCNPs were water-solubilized with Pluronic F127 with high upconversion efficiency and can be imaged in a mouse model.« less

Two-photon absorption and upconversion luminescence of colloidal CsPbX3 quantum dots

NASA Astrophysics Data System (ADS)

Han, Qiuju; Wu, Wenzhi; Liu, Weilong; Yang, Qingxin; Yang, Yanqiang

2018-01-01

The nonlinear optical and the upconversion luminescence (UCL) properties of CsPbX3 (X = Br or its binary mixtures with Cl, I) quantum dots (QDs) are investigated by femtosecond open-aperture (OA) Z-scan and time-resolved luminescence techniques in nonresonant spectral region. The OA Z-scan results show that CsPbX3 QDs have strong reverse saturable absorption (RSA), which is ascribed to two-photon absorption. Partially changing halide composition from Cl to Br, to I, two-photon absorption cross sections become larger at the same laser excitation intensity. The composition-tunable nonlinear absorption should be attributed to the gradual decrease of the lowest direct band gaps with the halide substitute. Moreover, the strong UCL can be observed under near infrared femtosecond laser excitation. Halide composition-tunable UCL dynamics of CsPbX3 QDs is analyzed by use of two-exponential fitting with deconvolution. When CsPbX3 QDs have similar sizes (10-13 nm), with partially changing halide composition from Cl to Br, to I, the average UCL lifetime becomes longer due to the variation of Kane energy. Our findings suggest all-inorganic perovskite QDs can be used as excellent gain medium for high-performance frequency-upconversion lasers and provide reference to engineer such QDs toward practical optoelectronic applications.

Magnetic nanosensor particles in luminescence upconversion capability.

PubMed

Wilhelm, Stefan; Hirsch, Thomas; Scheucher, Elisabeth; Mayr, Torsten; Wolfbeis, Otto S

2011-09-05

Nanoparticles (NPs) exhibit interesting size-dependent electrical, optical, magnetic, and chemical properties that cannot be observed in their bulk counterparts. The synthesis of NPs (i.e., crystalline particles ranging in size from 1 to 100 nm) has been intensely studied in the past decades. Magnetic nanoparticles (MNPs) form a particularly attractive class of NPs and have found numerous applications such as in magnetic resonance imaging to visualize cancer, cardiovascular, neurological and other diseases. Other uses include drug targeting, tissue imaging, magnetic immobilization, hyperthermia, and magnetic resonance imaging. MNPs, due to their magnetic properties, can be easily separated from (often complex) matrices and manipulated by applying external magnetic field. Near-infrared to visible upconversion luminescent nanoparticles (UCLNPs) form another type of unusual nanoparticles. They are capable of emitting visible light upon NIR light excitation. Lanthanide-doped (Yb, Er) hexagonal NaYF₄ UCLNPs are the most efficient upconversion phosphors known up to now. The use of UCLNPs for in vitro imaging of cancer cells and in vivo imaging in tissues has been demonstrated. UCLNPs show great potential as a new class of luminophores for biological, biomedical, and sensor applications. We are reporting here on our first results on the combination of MNP and UCLNP technology within an ongoing project supported by the DFG and the FWF (Austria).

Ultrasmall lanthanide-doped nanoparticles as multimodal platforms

NASA Astrophysics Data System (ADS)

Yust, Brian G.; Pedraza, Francisco J.; Sardar, Dhiraj K.

2014-03-01

Recently, there has been a great amount of interest in nanoparticles which are able to provide a platform with high contrast for multiple imaging modalities in order to advance the tools available to biomedical researchers and physicians. However, many nanoparticles do not have ideal properties to provide high contrast in different imaging modes. In order to address this, ultrasmall lanthanide doped oxide and fluoride nanoparticles with strong NIR to NIR upconversion fluorescence and a strong magnetic response for magnetic resonance imaging (MRI) have been developed. Specifically, these nanoparticles incorporate gadolinium, dysprosium, or a combination of both into the nano-crystalline host to achieve the magnetic properties. Thulium, erbium, and neodymium codopants provide the strong NIR absorption and emission lines that allow for deeper tissue imaging since near infrared light is not strongly absorbed or scattered by most tissues within this region. This also leads to better image quality and lower necessary excitation intensities. As a part of the one pot synthesis, these nanoparticles are coated with peg, pmao, or d-glucuronic acid to make them water soluble, biocompatible, and bioconjugable due to the available carboxyl or amine groups. Here, the synthesis, morphological characterization, magnetic response, NIR emission, and the quantum yield will be discussed. Cytotoxicity tested through cell viability at varying concentrations of nanoparticles in growth media will also be discussed.

Bioimaging and toxicity assessments of near-infrared upconversion luminescent NaYF4:Yb,Tm nanocrystals.

PubMed

Zhou, Jia-Cai; Yang, Zheng-Lin; Dong, Wei; Tang, Ruo-Jin; Sun, Ling-Dong; Yan, Chun-Hua

2011-12-01

In vitro or in vivo bioimaging utilizing the upconversion (UC) luminescence of rare earth fluoride nanocrystals (NCs) has attracted much attention, especially for Yb(3+)/Tm(3+) doped NCs with a near-infrared (NIR) UC emission at 800 nm. Herein, water-soluble NaYF(4):Yb,Tm NCs with strong NIR UC emission were synthesized with a solvothermal method. In vitro and in vivo bioimaging and toxicity assessments were carried out with HeLa cell and Caenorhabditis elegans (C. elegans) cases, respectively. NaYF(4):Yb,Tm NCs afforded an efficient NIR image of the HeLa cells with an incubation concentration of 10 μg mL(-1), and CCK-8 assay revealed a low cytotoxicity. Fed with Escherichia coli (E. coli) and NCs together, the C. elegans showed a NIR image in the gut from the pharynx to the anus. Further, these NCs could be excreted out when those worms were then fed with only E. coli. Toxicity studies were further addressed with protein expression, life span, egg production, egg viability, and growth rate of the worms in comparison with those of the intact ones. The feeding of rare earth fluoride NCs with a dose of 100 μg does not arise obvious toxicity effect from the growth to procreation. The in vitro and in vivo studies confirm that NaYF(4):Yb,Tm NCs could be served as an excellent NIR emission bioprobe with low toxicity. Copyright © 2011 Elsevier Ltd. All rights reserved.

White light generation via up-conversion and blue tone in Er3+/Tm3+/Yb3+-doped zinc-tellurite glasses

NASA Astrophysics Data System (ADS)

Rivera, V. A. G.; Ferri, F. A.; Nunes, L. A. O.; Marega, E.

2017-05-01

Yb3+, Er3+ and Tm3+ triply doped zinc-tellurite glass have been prepared containing up to 3.23 wt% of rare-earth ion oxides, were characterized by absorption spectroscopy, excitation, emission and up-conversion spectra. Transparent and homogeneous glasses have been produced, managing the red, green and blue emission bands, in order to generate white light considering the human eye perception. The energy transfer (resonant or non-resonant) between those rare-earth ions provides a color balancing mechanism that maintains the operating point in the white region, generating warm white light, cool white light and artificial daylight through the increase of the 976/980 nm diode laser excitation power from 4 to 470 mW. A light source at 4000 K is obtained under the excitation at 980 nm with 15 mW, providing a white light environment that is comfortable to the human eye vision. The spectroscopic study presented in this work describes the white light generation by the triply-doped zinc-tellurite glass, ranging from blue, green and red, by controlling the laser excitation power and wavelength at 976/980 nm. Such white tuning provokes healthy effects on human health throughout the day, especially the circadian system.

Spectral evidence for multi-pathway contribution to the upconversion pathway in NaYF4:Yb3+,Er3+ phosphors.

PubMed

Cho, Youngho; Song, Si Won; Lim, Soo Yeong; Kim, Jae Hun; Park, Chan Ryang; Kim, Hyung Min

2017-03-08

Although upconversion phosphors have been widely used in nanomedicine, laser engineering, bioimaging, and solar cell technology, the upconversion luminescence mechanism of the phosphors has been fiercely debated. A comprehensive understanding of upconversion photophysics has been significantly impeded because the number of photons incorporated in the process in different competitive pathways could not be resolved. Few convincing results to estimate the contribution of each of the two-, three-, and four-photon channels of near-infrared (NIR) energy have been reported in yielding upconverted visible luminescence. In this study, we present the energy upconversion process occurring in NaYF 4 :Yb 3+ ,Er 3+ phosphors as a function of excitation frequency and power density. We investigated the upconversion mechanism of lanthanide phosphors by comparing UV/VIS one-photon excitation spectra and NIR multi-photon spectra. A detailed analysis of minor transitions in one-photon spectra and luminescence decay enables us to assign electronic origins of individual bands in multi-photon upconversion luminescence and provides characteristic transitions representing the corresponding upconversion channel. Furthermore, we estimated the quantitative contribution of multiple channels with respect to irradiation power and excitation energy.

NIR-triggered high-efficient photodynamic and chemo-cascade therapy using caspase-3 responsive functionalized upconversion nanoparticles.

PubMed

Zhao, Na; Wu, Baoyan; Hu, Xianglong; Xing, Da

2017-10-01

Stimuli-responsive nanoparticles with multiple therapeutic/diagnostic functions are highly desirable for effective tumor treatment. Herein novel caspase-3 responsive functionalized upconversion nanoparticles (CFUNs) were fabricated with three-in-one functional integration: near-infrared (NIR) triggered photodynamic damage along with caspase-3 activation, subsequent caspase-3 responsive drug release, and cascade chemotherapeutic activation. CFUNs were formulated from the self-assembly of caspase-3 responsive doxorubicin (DOX) prodrug tethered with DEVD peptide (DEVD-DOX), upconversion nanoparticles (UCNP), a photosensitizer (pyropheophorbide-a methyl ester, MPPa), and tumor-targeting cRGD-PEG-DSPE to afford multifunctional CFUNs, MPPa/UCNP-DEVD-DOX/cRGD. Upon cellular uptake and NIR irradiation, the visible light emission of UCNP could excite MPPa to produce reactive oxygen species for photodynamic therapy (PDT) along with the activation of caspase-3, which further cleaved DEVD peptide to release DOX within tumor cells, thus accomplishing NIR-triggered PDT and cascade chemotherapy. CFUNs presented silent therapeutic potency and negligible cytotoxicity in the dark, whereas in vitro and in vivo experiments demonstrated the NIR-triggered cascade therapeutic activation and tumor inhibition due to consecutive PDT and chemotherapy. Current NIR-activated cascade tumor therapy with two distinct mechanisms is significantly favorable to overcome multidrug resistance and tumor heterogeneity for persistent tumor treatment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Multifunctional Optical Sensors for Nanomanometry and Nanothermometry: High-Pressure and High-Temperature Upconversion Luminescence of Lanthanide-Doped Phosphates-LaPO4/YPO4:Yb3+-Tm3.

PubMed

Runowski, Marcin; Shyichuk, Andrii; Tymiński, Artur; Grzyb, Tomasz; Lavín, Víctor; Lis, Stefan

2018-05-23

Upconversion luminescence of nano-sized Yb 3+ and Tm 3+ codoped rare earth phosphates, that is, LaPO 4 and YPO 4 , has been investigated under high-pressure (HP, up to ∼25 GPa) and high-temperature (293-773 K) conditions. The pressure-dependent luminescence properties of the nanocrystals, that is, energy red shift of the band centroids, changes of the band ratios, shortening of upconversion lifetimes, and so forth, make the studied nanomaterials suitable for optical pressure sensing in nanomanometry. Furthermore, thanks to the large energy difference (∼1800 cm -1 ), the thermalized states of Tm 3+ ions are spectrally well-separated, providing high-temperature resolution, required in optical nanothermometry. The temperature of the system containing such active nanomaterials can be determined on the basis of the thermally induced changes of the Tm 3+ band ratio ( 3 F 2,3 → 3 H 6 / 3 H 4 → 3 H 6 ), observed in the emission spectra. The advantage of such upconverting optical sensors is the use of near-infrared light, which is highly penetrable for many materials. The investigated nanomanometers/nanothermometers have been successfully applied, as a proof-of-concept of a novel bimodal optical gauge, for the determination of the temperature of the heated system (473 K), which was simultaneously compressed under HP (1.5 and 5 GPa).

In vivo 808 nm image-guided photodynamic therapy based on an upconversion theranostic nanoplatform.

PubMed

Liu, Xiaomin; Que, Ivo; Kong, Xianggui; Zhang, Youlin; Tu, Langping; Chang, Yulei; Wang, Tong Tong; Chan, Alan; Löwik, Clemens W G M; Zhang, Hong

2015-09-28

A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the (1)O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, (1)O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm(-2)) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy.

Photoluminescence upconversion at GaAs /InGa P2 interfaces driven by a sequential two-photon absorption mechanism

NASA Astrophysics Data System (ADS)

Hylton, N. P.; Hinrichsen, T. F.; Vaquero-Stainer, A. R.; Yoshida, M.; Pusch, A.; Hopkinson, M.; Hess, O.; Phillips, C. C.; Ekins-Daukes, N. J.

2016-06-01

This paper reports on the results of an investigation into the nature of photoluminescence upconversion at GaAs /InGa P2 interfaces. Using a dual-beam excitation experiment, we demonstrate that the upconversion in our sample proceeds via a sequential two-photon optical absorption mechanism. Measurements of photoluminescence and upconversion photoluminescence revealed evidence of the spatial localization of carriers in the InGa P2 material, arising from partial ordering of the InGa P2 . We also observed the excitation of a two-dimensional electron gas at the GaAs /InGa P2 heterojunction that manifests as a high-energy shoulder in the GaAs photoluminescence spectrum. Furthermore, the results of upconversion photoluminescence excitation spectroscopy demonstrate that the photon energy onset of upconversion luminescence coincides with the energy of the two-dimensional electron gas at the GaAs /InGa P2 interface, suggesting that charge accumulation at the interface can play a crucial role in the upconversion process.

Ultrafast exciton dynamics in cadmium selenide nanocrystals determined by femtosecond fluorescence upconversion spectroscopy

NASA Astrophysics Data System (ADS)

Underwood, David Frederick

Femtosecond fluorescence upconversion spectroscopy is a technique that allows the unambiguous determination of the excited state dynamics of an analyte. Combining this method with the use of tunable laser excitation, the exciton dynamics in semiconducting nanocrystals (NC's) of cadmium selenide (CdSe) have been determined, devoid of the complications arising from more common spectroscopic methods such as pump-probe. The results of this investigation were used to construct a model to fully describe the three-level system comprising of the valence and conduction bands and surface states, which have been calculated by others to lie mid-gap in energy. Smaller NC's showed faster decay components due to increased interaction between the exciton and surface states. The deep trap emission, which has never before been measured by ultrafast fluorescence techniques, shows a rapid rise time (˜2 ps), which is attributed to surface selenium dangling bonds relaxing to the valence band and radiatively combining with the photo-generated hole. The band edge fluorescence decays as the deep trap emission grows in, inherently coupling the two processes. An experiment which measured the dependence of the excitation energy showed that increased energy imparted to the NC's resulted in increased rise times, yielding the timescales for exciton relaxation through the valence and conduction band states to the lowest emitting state. Surface-oxidized and normally-passivated NC's display the same decay dynamics in time but differ in relative amplitude; the latter point agrees with steady-state measurements. The rotational anisotrophy of the NC's was measured and agrees with previous pump-probe data. Upconversion on the red and blue sides of the static fluorescence spectrum showed no discernable differences, which is either and inherent limitation of the experimental apparatus, or the possibility that lower-lying triplet states are populated on a timescale below the instrument resolution.

Er{sup 3+}/Yb{sup 3+}co-doped bismuth molybdate nanosheets upconversion photocatalyst with enhanced photocatalytic activity

DOE Office of Scientific and Technical Information (OSTI.GOV)

Adhikari, Rajesh; Gyawali, Gobinda; Cho, Sung Hun

2014-01-15

In this paper, we report the microwave hydrothermal synthesis of Er{sup 3+}/Yb{sup 3+} co-doped Bi{sub 2}MoO{sub 6} upconversion photocatalyst. Crystal structure, morphology, elemental composition, optical properties and BET surface area were analyzed in detail. Infrared to visible upconversion luminescence at 532 nm and 546 nm of the co-doped samples was investigated under excitation at 980 nm. The results revealed that the co-doping of Er{sup 3+}/Yb{sup 3+} into Bi{sub 2}MoO{sub 6} exhibited enhanced photocatalytic activity for the decomposition of rhodamine B under simulated solar light irradiation. Enhanced photocatalytic activity can be attributed to the energy transfer between Er{sup 3+}/Yb{sup 3+} andmore » Bi{sub 2}MoO{sub 6} via infrared to visible upconversion from Er{sup 3+}/Yb{sup 3+} ion and higher surface area of the Bi{sub 2}MoO{sub 6} nanosheets. Therefore, this synthetic approach may exhibit a better alternative to fabricate upconversion photocatalyst for integral solar light absorption. - Graphical abstract: Schematic illustration of the upconversion photocatalysis. Display Omitted - Highlights: • Er{sup 3+}/Yb{sup 3+} co-doped Bi{sub 2}MoO{sub 6} upconversion photocatalyst is successfully synthesized. • We obtained the nanosheets having high surface area. • Upconversion of IR to visible light was confirmed. • Upconversion phenomena can be utilized for effective photocatalysis.« less

Purely organic electroluminescent material realizing 100% conversion from electricity to light

PubMed Central

Kaji, Hironori; Suzuki, Hajime; Fukushima, Tatsuya; Shizu, Katsuyuki; Suzuki, Katsuaki; Kubo, Shosei; Komino, Takeshi; Oiwa, Hajime; Suzuki, Furitsu; Wakamiya, Atsushi; Murata, Yasujiro; Adachi, Chihaya

2015-01-01

Efficient organic light-emitting diodes have been developed using emitters containing rare metals, such as platinum and iridium complexes. However, there is an urgent need to develop emitters composed of more abundant materials. Here we show a thermally activated delayed fluorescence material for organic light-emitting diodes, which realizes both approximately 100% photoluminescence quantum yield and approximately 100% up-conversion of the triplet to singlet excited state. The material contains electron-donating diphenylaminocarbazole and electron-accepting triphenyltriazine moieties. The typical trade-off between effective emission and triplet-to-singlet up-conversion is overcome by fine-tuning the highest occupied molecular orbital and lowest unoccupied molecular orbital distributions. The nearly zero singlet–triplet energy gap, smaller than the thermal energy at room temperature, results in an organic light-emitting diode with external quantum efficiency of 29.6%. An external quantum efficiency of 41.5% is obtained when using an out-coupling sheet. The external quantum efficiency is 30.7% even at a high luminance of 3,000 cd m−2. PMID:26477390

Intra-cavity upconversion to 631 nm of images illuminated by an eye-safe ASE source at 1550 nm.

PubMed

Torregrosa, A J; Maestre, H; Capmany, J

2015-11-15

We report an image wavelength upconversion system. The system mixes an incoming image at around 1550 nm (eye-safe region) illuminated by an amplified spontaneous emission (ASE) fiber source with a Gaussian beam at 1064 nm generated in a continuous-wave diode-pumped Nd(3+):GdVO(4) laser. Mixing takes place in a periodically poled lithium niobate (PPLN) crystal placed intra-cavity. The upconverted image obtained by sum-frequency mixing falls around the 631 nm red spectral region, well within the spectral response of standard silicon focal plane array bi-dimensional sensors, commonly used in charge-coupled device (CCD) or complementary metal-oxide-semiconductor (CMOS) video cameras, and of most image intensifiers. The use of ASE illumination benefits from a noticeable increase in the field of view (FOV) that can be upconverted with regard to using coherent laser illumination. The upconverted power allows us to capture real-time video in a standard nonintensified CCD camera.

In vivo covalent cross-linking of photon-converted rare-earth nanostructures for tumour localization and theranostics

NASA Astrophysics Data System (ADS)

Ai, Xiangzhao; Ho, Chris Jun Hui; Aw, Junxin; Attia, Amalina Binte Ebrahim; Mu, Jing; Wang, Yu; Wang, Xiaoyong; Wang, Yong; Liu, Xiaogang; Chen, Huabing; Gao, Mingyuan; Chen, Xiaoyuan; Yeow, Edwin K. L.; Liu, Gang; Olivo, Malini; Xing, Bengang

2016-01-01

The development of precision nanomedicines to direct nanostructure-based reagents into tumour-targeted areas remains a critical challenge in clinics. Chemical reaction-mediated localization in response to tumour environmental perturbations offers promising opportunities for rational design of effective nano-theranostics. Here, we present a unique microenvironment-sensitive strategy for localization of peptide-premodified upconversion nanocrystals (UCNs) within tumour areas. Upon tumour-specific cathepsin protease reactions, the cleavage of peptides induces covalent cross-linking between the exposed cysteine and 2-cyanobenzothiazole on neighbouring particles, thus triggering the accumulation of UCNs into tumour site. Such enzyme-triggered cross-linking of UCNs leads to enhanced upconversion emission upon 808 nm laser irradiation, and in turn amplifies the singlet oxygen generation from the photosensitizers attached on UCNs. Importantly, this design enables remarkable tumour inhibition through either intratumoral UCNs injection or intravenous injection of nanoparticles modified with the targeting ligand. Our strategy may provide a multimodality solution for effective molecular sensing and site-specific tumour treatment.

BaY2F8 doped with Er3+: An upconverter material for photovoltaic application

NASA Astrophysics Data System (ADS)

Boccolini, A.; Faoro, R.; Favilla, E.; Veronesi, S.; Tonelli, M.

2013-08-01

Fluoride crystals (BaY2F8) doped with Er3+ ions with different doping level have been grown with a home-made Czochralski furnace. A spectroscopic characterization consisting in both absorption and fluorescence measurements were performed in order to investigate the upconversion mechanism occurring when the material is excited with a radiation at 1557 nm. The measured emission spectrum shows a photoluminescence mainly distributed in the Near Infrared (NIR) region at ≃1 μm. The spectral conversion due to the upconversion makes this material suitable for photovoltaic applications, especially if we combine it with a crystalline silicon solar cell. A device made of single face solar cell+upconverter material (PV-UC) was designed and his external quantum efficiency (EQE) at 1557 nm was measured. EQE values of 6.5% and 4.1% were reached under 8.5 W cm-2 power density illumination for the 30%Er3+ and 20%Er3+ samples, respectively.

Distance-Dependent Plasmon-Enhanced Fluorescence of Upconversion Nanoparticles using Polyelectrolyte Multilayers as Tunable Spacers

PubMed Central

Feng, Ai Ling; You, Min Li; Tian, Limei; Singamaneni, Srikanth; Liu, Ming; Duan, Zhenfeng; Lu, Tian Jian; Xu, Feng; Lin, Min

2015-01-01

Lanthanide-doped upconversion nanoparticles (UCNPs) have attracted widespread interests in bioapplications due to their unique optical properties by converting near infrared excitation to visible emission. However, relatively low quantum yield prompts a need for developing methods for fluorescence enhancement. Plasmon nanostructures are known to efficiently enhance fluorescence of the surrounding fluorophores by acting as nanoantennae to focus electric field into nano-volume. Here, we reported a novel plasmon-enhanced fluorescence system in which the distance between UCNPs and nanoantennae (gold nanorods, AuNRs) was precisely tuned by using layer-by-layer assembled polyelectrolyte multilayers as spacers. By modulating the aspect ratio of AuNRs, localized surface plasmon resonance (LSPR) wavelength at 980 nm was obtained, matching the native excitation of UCNPs resulting in maximum enhancement of 22.6-fold with 8 nm spacer thickness. These findings provide a unique platform for exploring hybrid nanostructures composed of UCNPs and plasmonic nanostructures in bioimaging applications. PMID:25586238

Designed Er(3+)-singly doped NaYF4 with double excitation bands for simultaneous deep macroscopic and microscopic upconverting bioimaging.

PubMed

Wen, Xuanyuan; Wang, Baoju; Wu, Ruitao; Li, Nana; He, Sailing; Zhan, Qiuqiang

2016-06-01

Simultaneous deep macroscopic imaging and microscopic imaging is in urgent demand, but is challenging to achieve experimentally due to the lack of proper fluorescent probes. Herein, we have designed and successfully synthesized simplex Er(3+)-doped upconversion nanoparticles (UCNPs) with double excitation bands for simultaneous deep macroscopic and microscopic imaging. The material structure and the excitation wavelength of Er(3+)-singly doped UCNPs were further optimized to enhance the upconversion emission efficiency. After optimization, we found that NaYF4:30%Er(3+)@NaYF4:2%Er(3+) could simultaneously achieve efficient two-photon excitation (2PE) macroscopic tissue imaging and three-photon excitation (3PE) deep microscopic when excited by 808 nm continuous wave (CW) and 1480 nm CW lasers, respectively. In vitro cell imaging and in vivo imaging have also been implemented to demonstrate the feasibility and potential of the proposed simplex Er(3+)-doped UCNPs as bioprobe.

Multifunctional NaYF4:Yb, Er@mSiO2@Fe3O4-PEG nanoparticles for UCL/MR bioimaging and magnetically targeted drug delivery.

PubMed

Liu, Bei; Li, Chunxia; Ma, Ping'an; Chen, Yinyin; Zhang, Yuanxin; Hou, Zhiyao; Huang, Shanshan; Lin, Jun

2015-02-07

A low toxic multifunctional nanoplatform, integrating both mutimodal diagnosis methods and antitumor therapy, is highly desirable to assure its antitumor efficiency. In this work, we show a convenient and adjustable synthesis of multifunctional nanoparticles NaYF4:Yb, Er@mSiO2@Fe3O4-PEG (MFNPs) based on different sizes of up-conversion nanoparticles (UCNPs). With strong up-conversion fluorescence offered by UCNPs, superparamagnetism properties attributed to Fe3O4 nanoparticles and porous structure coming from the mesoporous SiO2 shell, the as-obtained MFNPs can be utilized not only as a contrast agent for dual modal up-conversion luminescence (UCL)/magnetic resonance (MR) bio-imaging, but can also achieve an effective magnetically targeted antitumor chemotherapy both in vitro and in vivo. Furthermore, the UCL intensity of UCNPs and the magnetic properties of Fe3O4 in the MFNPs were carefully balanced. Silica coating and further PEG modifying can improve the hydrophilicity and biocompatibility of the as-synthesized MFNPs, which was confirmed by the in vitro/in vivo biocompatibility and in vivo long-time bio-distributions tests. Those results revealed that the UCNPs based magnetically targeted drug carrier system we synthesized has great promise in the future for multimodal bio-imaging and targeted cancer therapy.

An Nd3+-sensitized upconversion nanophosphor modified with a cyanine dye for the ratiometric upconversion luminescence bioimaging of hypochlorite

NASA Astrophysics Data System (ADS)

Zou, Xianmei; Liu, Yi; Zhu, Xingjun; Chen, Min; Yao, Liming; Feng, Wei; Li, Fuyou

2015-02-01

Excessive or misplaced production of ClO- in living systems is usually associated with many human diseases. Therefore, it is of great importance to develop an effective and sensitive method to detect ClO- in living systems. Herein, we designed an 808 nm excited upconversion luminescence nanosystem, composed of the Nd3+-sensitized core-shell upconversion nanophosphor NaYF4:30%Yb,1%Nd,0.5%Er@NaYF4:20%Nd, which serves as an energy donor, and the ClO--responsive cyanine dye hCy3, which acts as an energy acceptor, for ratiometric upconversion luminescence (UCL) monitoring of ClO-. The detection limit of ClO- for this nanoprobe in aqueous solution is 27 ppb and the nanoprobe was successfully used to detect the ClO- in the living cells by ratiometric upconversion luminescence. Importantly, the nanoprobe realized the detection of ClO- in a mouse model of arthritis, which produced an excess of ROS, under 808 nm irradiation in vivo. The excitation laser efficiently reduced the heating effect, compared to the commonly used 980 nm laser for upconversion systems.Excessive or misplaced production of ClO- in living systems is usually associated with many human diseases. Therefore, it is of great importance to develop an effective and sensitive method to detect ClO- in living systems. Herein, we designed an 808 nm excited upconversion luminescence nanosystem, composed of the Nd3+-sensitized core-shell upconversion nanophosphor NaYF4:30%Yb,1%Nd,0.5%Er@NaYF4:20%Nd, which serves as an energy donor, and the ClO--responsive cyanine dye hCy3, which acts as an energy acceptor, for ratiometric upconversion luminescence (UCL) monitoring of ClO-. The detection limit of ClO- for this nanoprobe in aqueous solution is 27 ppb and the nanoprobe was successfully used to detect the ClO- in the living cells by ratiometric upconversion luminescence. Importantly, the nanoprobe realized the detection of ClO- in a mouse model of arthritis, which produced an excess of ROS, under 808 nm irradiation in vivo. The excitation laser efficiently reduced the heating effect, compared to the commonly used 980 nm laser for upconversion systems. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr06407k

Quantum Phenomena in High Energy Density Plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murnane, Margaret; Kapteyn, Henry

The possibility of implementing efficient (phase matched) HHG upconversion of deep- UV lasers in multiply-ionized plasmas, with potentially unprecedented conversion efficiency is a fascinating prospect. HHG results from the extreme nonlinear response of matter to intense laser light:high harmonics are radiated as a result of a quantum coherent electron recollision process that occurs during laser field ionization of an atom. Under current support from this grant in work published in Science in 2015, we discovered a new regime of bright HHG in highly-ionized plasmas driven by intense UV lasers, that generates bright harmonics to photon energies >280eV

Comparison of the up-conversion photoluminescence for GAP, GAG and GAM phosphors

NASA Astrophysics Data System (ADS)

Deng, Taoli; Jiang, Xianbang

2018-04-01

GdAlO3:Er3+/Yb3+, Gd3Al5O12:Er3+/Yb3+ and Gd4Al2O9:Er3+/Yb3+ phosphors were prepared by co-precipitation. The effects for Gd2O3-Al2O3 composite oxides as the host materials with different crystal structures such as GdAlO3, Gd3Al5O12 and Gd4Al2O9 were investigated. It was found that the perovskite structured GdAlO3:Er3+/Yb3+ (GAP phosphor) could be obtained from the precursor when the calcination temperature was 1000 °C, while the garnet structured Gd3Al5O12:Er3+/Yb3+ (GAG phosphor) could be formed when the calcination temperature was 1300 °C, but the monoclinic-structured Gd4Al2O9:Er3+/Yb3+ (GAM phosphor) could be formed only when the calcination temperature was raised up to 1500 °C. The difference of the up-conversion photoluminescence (UCPL) spectra under 980 nm between the GAP, GAG and GAM phosphors was studied. The result showed that the UCPL intensity of the GAP phosphor was close to that of the GAM phosphor with much higher red-to-green intensity ratio than that of GAP phosphor. The UCPL intensity of GAG phosphor was the weakest among them. Finally, the factors which influenced on the UCPL of the GAP, GAG and GAM phosphors were discussed.

Infrared Signal Detection by Upconversion Technique

NASA Technical Reports Server (NTRS)

Wong, Teh-Hwa; Yu, Jirong; Bai, Yingxin; Johnson, William E.

2014-01-01

We demonstrated up-conversion assisted detection of a 2.05-micron signal by using a bulk periodically poled Lithium niobate crystal. The 94% intrinsic up-conversion efficiency and 22.58% overall detection efficiency at pW level of 2.05-micron was achieved.

Lanthanide‐Doped Upconversion Nanoparticles: Emerging Intelligent Light‐Activated Drug Delivery Systems

PubMed Central

Bagheri, Ali; Arandiyan, Hamidreza

2016-01-01

The development of drug delivery systems (DDSs) using near infrared (NIR) light and upconversion nanoparticles (UCNPs) has generated intensive interest over the past five years. These NIR‐initiated DDSs not only offer a high degree of spatial and temporal determination of therapeutic release but also provide precise control over the released dosage. Furthermore, these nanoplatforms confer several advantages over conventional light‐based DDSs—NIR offers better tissue penetration depth and a reduced risk of cellular photo‐damage caused by exposure to light at high‐energy wavelengths (e.g., ultraviolet light, <400 nm). The development of DDSs that can be activated by low intensity NIR illumination is highly desirable to avoid exposing living tissues to excessive heat that can limit the in vivo application of these DDSs. This encompasses research in three directions: (i) enhancing the quantum yield of the UCNPs; (ii) incorporation of photo‐responsive materials with red‐shifted absorptions into the UCNPs; and (iii) tuning the UCNPs excitation wavelength. This review focuses on recent advances in the development of NIR‐initiated DDS, with emphasis on the use of photo‐responsive compounds and polymeric materials conjugated onto UCNPs. The challenges that limit UCNPs clinical applications, alongside with the aforementioned techniques that have emerged to overcome these limitations, are highlighted. PMID:27818904

Spatial height directed microfluidic synthesis of transparent inorganic upconversion nano film

NASA Astrophysics Data System (ADS)

Liu, Xiaoxia; Zhu, Cheng; Liao, Wei; Jin, Junyang; Ni, Yaru; Lu, Chunhua; Xu, Zhongzi

2017-11-01

A microfluidic-based synthesis of an inorganic upconversion nano film has been developed with a large area of dense-distributed NaYF4 crystal grains in a silica glass micro-reactor and the film exhibits high transparence, strong upconversion luminescence and robust adhesion with the substrate. The spatial heights of micro-reactors are tuned between 31 and 227 mm, which can regulate flow regimes. The synergistic effect of spatial height and fluid regime is put forward, which influences diffusion paths and assembly ways of different precursor molecules and consequently directs final distributions and morphologies of crystal grains, as well as optical properties due to diversity of surface and thickness of films. The spatial height of 110 mm is advantageous for high transmittance of upconversion film due to the flat surface and appropriate film thickness of 67 nm. The height of 150 mm is in favor of uniform distribution of upconversion fluorescence and achieving the strongest fluorescence due to minimized optical loss. Such a transparent upconversion film with a large area of uniform distribution is promising to promote the application of upconversion materials and spatial height directed microfluidic regime have a certain significance on many microfluidic synthesis.

Chemiluminescence of nitrogen-rich quantum dots in diperiodatoargentate(III) solution and its application in ferulic acid analysis.

PubMed

Fu, Zhaofu; Li, Gongke; Hu, Yufei

2016-12-01

A novel chemiluminescence (CL) system based on the reaction of fluorescent water-soluble nitrogen-rich quantum dots (N-dots) and diperiodatoargentate(III) (DPA) was developed. The prepared N-dots have a small size (≤10 nm) and high percentage of nitrogen (39.9 %), which exceeds the content of carbon in the same N-dots. The N-dots exhibit characteristic blue fluorescence under UV light and up-conversion luminescence. The relatively intense CL emission is based on the direct oxidation of N-dots by DPA. The CL emission may be attributed to the high nitrogen content and the special structure of the N-dots. The CL mechanism of N-dots and DPA was investigated by using CL, UV-Vis absorption, IR, fluorescence, and radical scavenging experiments. This investigation provides a way to study the optical properties of N-dots. The analytical applicability of the N-dots and DPA CL system in the determination of ferulic acid (FA) was explored. The CL intensity was linearly proportional to the concentration of ferulic acid from 3.0 × 10 -7 to 1.0 × 10 -5 g mL -1 with a detection limit of 8.0 × 10 -8 g mL -1 (3σ); the relative standard deviation was 2.4 % for 4.0 × 10 -7 g mL -1 FA (n = 9). The proposed method was successfully applied to the determination of ferulic acid in Angelica sinensis. The study provides valuable insight into the role of nitrogen-rich quantum dots in CL.

NIR to NIR upconversion in KYb2F7: RE3+ (RE = Tm, Er) nanoparticles for biological imaging

NASA Astrophysics Data System (ADS)

Pedraza, F.; Yust, B.; Tsin, A.; Sardar, D.

2014-03-01

Until recently, many contrast agents widely used in biological imaging have absorbed and emitted in the visible region, limiting their usefulness for deeper tissue imaging. In order to push the boundaries of deep tissue imaging with non-ionizing radiation, contrast agents in the near infrared (NIR) regime, which is not strongly absorbed or scattered by most tissues, are being sought after. Upconverting nanoparticles (UCNPs) are attractive candidates since their upconversion emission is tunable with a very narrow bandwidth and they do not photobleach or blink. The upconversion produced by the nanoparticles can be tailored for NIR to NIR by carefully choosing the lanthanide dopants and dopant ratios such as KYb2F7: RE3+ (RE = Tm, Er). Spectroscopic characterization was done by analyzing absorption, fluorescence, and quantum yield data. In order to study the toxicity of the nanoparticles Monkey Retinal Endothelial Cells (MREC) were cultivated in 24 well plates and then treated with nanoparticles at different concentrations in triplicate to obtain the optimal concentration for in vivo experiments. It will be shown that these UCNPs do not elicit a strong toxic response such as quantum dots and some noble metal nanoparticles. 3-D optical slices of nanoparticle treated fibroblast cells were imaged using a confocal microscope where the nucleus and cytoplasm were stained with DAPI and Alexa Fluor respectively. These results presented support the initial assumption, which suggests that KYb2F7: RE3+ would be excellent candidates for NIR contrast agents.

Accurate Quantitative Sensing of Intracellular pH based on Self-ratiometric Upconversion Luminescent Nanoprobe.

PubMed

Li, Cuixia; Zuo, Jing; Zhang, Li; Chang, Yulei; Zhang, Youlin; Tu, Langping; Liu, Xiaomin; Xue, Bin; Li, Qiqing; Zhao, Huiying; Zhang, Hong; Kong, Xianggui

2016-12-09

Accurate quantitation of intracellular pH (pH i ) is of great importance in revealing the cellular activities and early warning of diseases. A series of fluorescence-based nano-bioprobes composed of different nanoparticles or/and dye pairs have already been developed for pH i sensing. Till now, biological auto-fluorescence background upon UV-Vis excitation and severe photo-bleaching of dyes are the two main factors impeding the accurate quantitative detection of pH i . Herein, we have developed a self-ratiometric luminescence nanoprobe based on förster resonant energy transfer (FRET) for probing pH i , in which pH-sensitive fluorescein isothiocyanate (FITC) and upconversion nanoparticles (UCNPs) were served as energy acceptor and donor, respectively. Under 980 nm excitation, upconversion emission bands at 475 nm and 645 nm of NaYF 4 :Yb 3+ , Tm 3+ UCNPs were used as pH i response and self-ratiometric reference signal, respectively. This direct quantitative sensing approach has circumvented the traditional software-based subsequent processing of images which may lead to relatively large uncertainty of the results. Due to efficient FRET and fluorescence background free, a highly-sensitive and accurate sensing has been achieved, featured by 3.56 per unit change in pH i value 3.0-7.0 with deviation less than 0.43. This approach shall facilitate the researches in pH i related areas and development of the intracellular drug delivery systems.

Accurate Quantitative Sensing of Intracellular pH based on Self-ratiometric Upconversion Luminescent Nanoprobe

NASA Astrophysics Data System (ADS)

Li, Cuixia; Zuo, Jing; Zhang, Li; Chang, Yulei; Zhang, Youlin; Tu, Langping; Liu, Xiaomin; Xue, Bin; Li, Qiqing; Zhao, Huiying; Zhang, Hong; Kong, Xianggui

2016-12-01

Accurate quantitation of intracellular pH (pHi) is of great importance in revealing the cellular activities and early warning of diseases. A series of fluorescence-based nano-bioprobes composed of different nanoparticles or/and dye pairs have already been developed for pHi sensing. Till now, biological auto-fluorescence background upon UV-Vis excitation and severe photo-bleaching of dyes are the two main factors impeding the accurate quantitative detection of pHi. Herein, we have developed a self-ratiometric luminescence nanoprobe based on förster resonant energy transfer (FRET) for probing pHi, in which pH-sensitive fluorescein isothiocyanate (FITC) and upconversion nanoparticles (UCNPs) were served as energy acceptor and donor, respectively. Under 980 nm excitation, upconversion emission bands at 475 nm and 645 nm of NaYF4:Yb3+, Tm3+ UCNPs were used as pHi response and self-ratiometric reference signal, respectively. This direct quantitative sensing approach has circumvented the traditional software-based subsequent processing of images which may lead to relatively large uncertainty of the results. Due to efficient FRET and fluorescence background free, a highly-sensitive and accurate sensing has been achieved, featured by 3.56 per unit change in pHi value 3.0-7.0 with deviation less than 0.43. This approach shall facilitate the researches in pHi related areas and development of the intracellular drug delivery systems.

Design, Synthesis, and Structure-Property Relationships of Er3+-Doped TiO2 Luminescent Particles Synthesized by Sol-Gel

PubMed Central

Lopez-Iscoa, Pablo; Baldi, Giovanni

2018-01-01

Titania particles doped with various concentrations of Erbium were synthesized by the sol-gel method followed by different heat treatments. The shape and the grain growth of the particles were noticeably affected by the concentration of Erbium and the heat treatment conditions. An infrared emission at 1530 nm, as well as green and red up-conversion emissions at 550 and 670 nm, were observed under excitation at 976 nm from all of the synthesized particles. The emission spectra and lifetime values appeared to be strongly influenced by the presence of the different crystalline phases. This work presents important guidelines for the synthesis of functional Er3+-doped titania particles with controlled and tailored spectroscopic properties for photonic applications. PMID:29301282

Visible upconversion emission and non-radiative direct Yb 3+ to Er 3+ energy transfer processes in nanocrystalline ZrO 2:Yb 3+,Er 3+

NASA Astrophysics Data System (ADS)

Diaz-Torres, L. A.; Meza, O.; Solis, D.; Salas, P.; De la Rosa, E.

2011-06-01

Wide band gap Yb 3+ and Er 3+ codoped ZrO 2 nanocrystals have been synthesized by a modified sol-gel method. Under 967 nm excitation strong green and red upconversion emission is observed for several Er 3+ to Yb 3+ ions concentration ratios. A simple microscopic rate equation model is used to study the effects of non-radiative direct Yb 3+ to Er 3+ energy transfer processes on the visible and near infrared fluorescence decay trends of both Er 3+ and Yb 3+ ions. The microscopic rate equation model takes into account the crystalline phase as well as the size of nanocrystals. Nanocrystals phase and size were estimated from XRD patterns. The rate equation model succeeds to fit simultaneously all visible and near infrared fluorescence decay profiles. The dipole-dipole interaction parameters that drive the non-radiative energy transfer processes depend on doping concentration due to crystallite phase changes. In addition the non-radiative relaxation rate ( 4I11/2→ 4I13/2) is found to be greater than that estimated by the Judd-Ofelt parameters due to the action of surface impurities. Results suggest that non-radiative direct Yb 3+ to Er 3+ energy transfer processes in ZrO 2:Yb,Er are extremely efficient.

Photophysics of Zinc Porphyrin Aggregates in Dilute Water-Ethanol Solutions.

PubMed

Stevens, Amy L; Joshi, Neeraj K; Paige, Matthew F; Steer, Ronald P

2017-12-14

Dimeric and multimeric aggregates of a model metalloporphyrin, zinc tetraphenylporphyrin (ZnTPP), have been produced in a controlled manner by incrementally increasing the water content of dilute aqueous ethanol solutions. Steady state absorption, fluorescence emission, and fluorescence excitation spectra have been measured to identify the aggregates present as a function of solvent composition. The dynamics of the excited states of the aggregates produced initially by excitation in the Soret region have been measured by ultrafast fluorescence upconversion techniques. Only the monomer produces measurable emission from S 2 with a picosecond lifetime; all Soret-excited aggregates, including the dimer, decay radiationlessly on a femtosecond time scale. The S 1 state is the only significant product of the radiationless decay of the S 2 state of the excited monomer, and the aggregates also produce substantial quantum yields of S 1 fluorescence when initially excited in the Soret region. The resulting fluorescent aggregates all decay on a subnanosecond time scale, likely by a mechanism that involves dissociation of the excited monomer from the excitonic multimer. The ZnTPP dimers excited at their ground state geometries in the Soret region exhibit a dynamic behavior that is quite different from those produced following noncoherent triplet-triplet annihilation under the same conditions. The important implications of these observations in determining the aggregation conditions promoting efficient photon upconversion by excitonic annihilation in a variety of media are thoroughly discussed.

Development and Application of Multifunctional Lanthanide-Doped Nanoparticles in Medical Imaging

NASA Astrophysics Data System (ADS)

Pedraza, Francisco J., III

Medical imaging has become one of the most important tools of modern medicine soon after it was developed. Presently, several imaging modalities are available to clinicians for the detection of skeletal fractures and functional abnormalities of organs and tissues; and also an excellent tool during surgical procedures. Unfortunately, each imaging technique possesses its own strengths and inherent limitations which can be mitigated via the use of multiple imaging modalities and imaging probes. Through the use of multiple imaging modalities, it is possible to gather complementary information for a more reliable diagnosis. Each imaging technique requires its own imaging probes, providing selectivity and improved contrast. However, conventional contrast agents are incapable of providing what the new generation of multifunctional nanomaterials offer. In addition to improved selectivity and contrast, multifunctional materials possess therapeutic capabilities such as photo-thermal therapy and controlled drug delivery. Lanthanide-based nanomaterials are viable candidates for multimodal imaging agents due to possessing multifunctional capabilities, optical and chemical stability, and an intense tunable emission. This doctoral dissertation will delve into the development of lanthanide-based nanoparticles by proposing a novel multifunctional contrast agent for Near Infrared Fluorescence Imaging and Magnetic Resonance Imaging. Furthermore, the study of surface modification effects on upconversion emission and nanoparticle-cell interactions was performed. Results presented will confirm the potential application of multifunctional lanthanide-based nanomaterials as multimodal imaging probes.

Photon energy upconversion through thermal radiation with the power efficiency reaching 16%.

PubMed

Wang, Junxin; Ming, Tian; Jin, Zhao; Wang, Jianfang; Sun, Ling-Dong; Yan, Chun-Hua

2014-11-28

The efficiency of many solar energy conversion technologies is limited by their poor response to low-energy solar photons. One way for overcoming this limitation is to develop materials and methods that can efficiently convert low-energy photons into high-energy ones. Here we show that thermal radiation is an attractive route for photon energy upconversion, with efficiencies higher than those of state-of-the-art energy transfer upconversion under continuous wave laser excitation. A maximal power upconversion efficiency of 16% is achieved on Yb(3+)-doped ZrO2. By examining various oxide samples doped with lanthanide or transition metal ions, we draw guidelines that materials with high melting points, low thermal conductivities and strong absorption to infrared light deliver high upconversion efficiencies. The feasibility of our upconversion approach is further demonstrated under concentrated sunlight excitation and continuous wave 976-nm laser excitation, where the upconverted white light is absorbed by Si solar cells to generate electricity and drive optical and electrical devices.

Plasmon-Enhanced Sub-Bandgap Photocatalysis via Triplet-Triplet Annihilation Upconversion for Volatile Organic Compound Degradation.

PubMed

Kim, Hyoung-Il; Weon, Seunghyun; Kang, Homan; Hagstrom, Anna L; Kwon, Oh Seok; Lee, Yoon-Sik; Choi, Wonyong; Kim, Jae-Hong

2016-10-18

This study demonstrates the first reported photocatalytic decomposition of an indoor air pollutant, acetaldehyde, using low-energy, sub-bandgap photons harnessed through sensitized triplet-triplet annihilation (TTA) upconversion (UC). To utilize low-intensity noncoherent indoor light and maximize photocatalytic activity, we designed a plasmon-enhanced sub-bandgap photocatalyst device consisting of two main components: (1) TTA-UC rubbery polymer films containing broad-band plasmonic particles (Ag-SiO 2 ) to upconvert sub-bandgap photons, and (2) nanodiamond (ND)-loaded WO 3 as a visible-light photocatalyst composite. Effective decomposition of acetaldehyde was achieved using ND/WO 3 (E g = 2.8 eV) coupled with TTA-UC polymer films that emit blue photons (λ Em = 425 nm, 2.92 eV) upconverted from green photons (λ Ex = 532 nm, 2.33 eV), which are wasted in most environmental photocatalysis. The overall photocatalytic efficiency was amplified by the broad-band surface plasmon resonance of AgNP-SiO 2 particles incorporated into the TTA-UC films.

Intense blue upconversion emission and intrinsic optical bistability in Tm3+/Yb3+/Zn2+ tridoped YVO4 phosphors

NASA Astrophysics Data System (ADS)

Yadav, Manglesh; Mondal, Manisha; Mukhopadhyay, Lakshmi; Rai, Vineet Kumar

2018-04-01

Tm3+/Yb3+/Zn2+:yttrium metavanadate (YVO4) phosphors prepared through chemical coprecipitation and the solid state reaction method have been structurally characterized by an x-ray diffraction (XRD) study. Photoluminescence study of the developed phosphors under ultraviolet (UV) and near infrared (NIR) excitation has been performed. The excitation spectrum of the tetragonal zircon type YVO4 phosphors corresponding to the emission at ˜476 nm exhibits a broad excitation peak in the 250-350 nm region, which is due to charge distribution in the {{{{VO}}}4}3- group. Under 980 nm CW diode laser excitation, enhancements of about ˜3000 times and ˜40 times have been observed for the blue band in the tridoped Tm3+Yb3+Zn2+:YVO4 phosphors compared to those of the Tm3+:YVO4 singly and Tm3+/Yb3+:YVO4 codoped phosphors, respectively. A downconversion (DC) emission study shows an enhancement of about ˜50 times for the blue band in the tridoped phosphors compared to that of the singly doped phosphors. Optical bistability (OB) behavior of the developed phosphors has been also investigated upon 980 nm excitation. The calculated Commission Internationale de l’Éclairage (CIE) color coordinates lie in the blue region with 96.5% color purity under 980 nm excitation, having a color temperature of ˜3400 K. Our observations show that the developed phosphors may be suitably used in dual mode luminescence spectroscopy, display devices, and UV LED chips.

Intense blue upconversion emission and intrinsic optical bistability in Tm3+/Yb3+/Zn2+ tridoped YVO4 phosphors.

PubMed

Yadav, Manglesh; Mondal, Manisha; Mukhopadhyay, Lakshmi; Rai, Vineet Kumar

2018-01-22

Tm 3+ /Yb 3+ /Zn 2+ :yttrium metavanadate (YVO 4 ) phosphors prepared through chemical coprecipitation and the solid state reaction method have been structurally characterized by an x-ray diffraction (XRD) study. Photoluminescence study of the developed phosphors under ultraviolet (UV) and near infrared (NIR) excitation has been performed. The excitation spectrum of the tetragonal zircon type YVO 4 phosphors corresponding to the emission at ∼476 nm exhibits a broad excitation peak in the 250-350 nm region, which is due to charge distribution in the [Formula: see text] group. Under 980 nm CW diode laser excitation, enhancements of about ∼3000 times and ∼40 times have been observed for the blue band in the tridoped Tm 3+ Yb 3+ Zn 2+ :YVO 4 phosphors compared to those of the Tm 3+ :YVO 4 singly and Tm 3+ /Yb 3+ :YVO 4 codoped phosphors, respectively. A downconversion (DC) emission study shows an enhancement of about ∼50 times for the blue band in the tridoped phosphors compared to that of the singly doped phosphors. Optical bistability (OB) behavior of the developed phosphors has been also investigated upon 980 nm excitation. The calculated Commission Internationale de l'Éclairage (CIE) color coordinates lie in the blue region with 96.5% color purity under 980 nm excitation, having a color temperature of ∼3400 K. Our observations show that the developed phosphors may be suitably used in dual mode luminescence spectroscopy, display devices, and UV LED chips.

Thermal, structural and optical properties of new TeO2sbnd Sb2O3sbnd GeO2 ternary glasses

NASA Astrophysics Data System (ADS)

Pereira, C.; Barbosa, J.; Cassanjes, F. C.; Gonçalves, R. R.; Ribeiro, S. J. L.; Poirier, G.

2016-12-01

In this work the novel glass system TeO2sbnd Sb2O3sbnd GeO2 was investigated and promising glass compositions were selected for further specific studies. Glass samples in the (80-0.8x)TeO2-(20-0.2x)Sb2O3-xGeO2 molar composition were prepared by the melt-quenching method with a glass-forming domain from x = 10 to x = 90. Samples were investigated by XRD, DSC, FTIR, Raman spectroscopy and UV-visible absorption. The XRD and DSC results bring informations about the non-crystalline state and thermal properties of these materials. It has been observed that higher GeO2 contents lead to higher glass transition temperatures and thermal stabilities against crystallization. FTIR and Raman spectroscopies suggest a progressive incorporation of GeO2 in the covalent network of TeO2 with conversion of structural units TeO4 to TeO3. Absorption spectra revealed the high visible transparency of these samples and an increase of the optical band gap with GeO2 addition, in agreement with a decreasing polarizability of the glass network. Er3+ doped and Er3+/Yb3+ codoped samples were also studied with respect to their infrared emission properties and higher GeO2 contents lead to an increase in IR emission intensity at 1,5 μm as well as longer radiative lifetimes. Finally, upconversion emission in the visible were also recorded and were shown to be strongly dependent of the composition.

Interactions of DNA coated upconversion nanoparticles with 2D materials

NASA Astrophysics Data System (ADS)

Giust, Davide; Lucío, María. Isabel; Muskens, Otto L.; Kanaras, Antonios G.

2018-02-01

In this work we investigated the nature of quenching between different types of 2D materials (WS2, MoS2 and graphene oxide) and oligonucleotide coated-upconversion nanoparticles. This study contributes towards the efficient design of biosensors based on 2D materials and DNA-coated upconversion nanoparticles.

Upconversion fiber-optic confocal microscopy under near-infrared pumping.

PubMed

Kim, Do-Hyun; Kang, Jin U; Ilev, Ilko K

2008-03-01

We present a simple upconversion fiber-optic confocal microscope design using a near-infrared laser for pumping of a rare-earth-doped glass powder. The nonlinear optical frequency conversion process is highly efficient with more than 2% upconversion fluorescence efficiency at a near-infrared pumping wavelength of 1.55 microm. The upconversion confocal design allows the use of conventional Si detectors and 1.55 microm near-infrared pump light. The lateral and axial resolutions of the system were equal to or better than 1.10 and 13.11 microm, respectively.

Multiple visible emissions by means of up-conversion process in a microstructured tellurite glass optical fiber.

PubMed

Boetti, Nadia G; Lousteau, Joris; Negro, Davide; Mura, Emanuele; Scarpignato, Gerardo; Abrate, Silvio; Milanese, Daniel

2012-02-27

We present a microstructured fiber whose 9 µm diameter core consists in three concentric rings made of three active glasses having different rare earth oxide dopants, Yb3+/Er3+, Yb3+/Tm3+ and Yb3+/Pr3+, respectively. Morphological and optical characterization of the optical fiber are presented. The photoluminescence spectrum is investigated for different pumping conditions using a commercial 980 nm laser diode. Tuning of the RGB (or white light) emission is demonstrated not only by adjusting the pump power but also by using an optical iris as spatial filter which, thanks to the microstructured core, also acts as a spectral filter.

Multifunctional upconversion nanoparticles based on NaYGdF4 for laser induced heating, non-contact temperature sensing and controlled hyperthermia with use of pulsed periodic laser excitation

NASA Astrophysics Data System (ADS)

Pominova, Daria V.; Ryabova, Anastasia V.; Romanishkin, Igor D.; Grachev, Pavel V.; Burmistrov, Ivan A.; Kuznetsov, Sergei V.

2018-04-01

For clinical application in photothermal therapy the nanoparticles should be efficient light-to-heat converters and luminescent markers. In this work, we investigate upconversion nanoparticles with NaYxGd1-xF4 (x=0-1) host lattice as self-monitored thermo-agents for bioimaging and local laser hyperthermia with real-time temperature control. The ability of non-contact temperature sensing using NaYxGd1-xF4 on one hand and laser induced heating on the other hand was shown. It was found, that the heat conversion luminescence efficiency is strongly affected by the concentration ratio of Gd3+ to Y3+ ions in host lattice. The optimal composition among the studied is NaY0.4Gd0.4Yb0.17Er0.03 with luminescence efficiency of 3.5% under 1 W/cm2 pumping power. Higher Gd3+ concentrations lead to higher heating temperature, but also to the decrease of the luminescence intensity and the accuracy of the ratiometric temperature determination. It was also shown that the optimization of Yb3+ doping concentration is one of the possible ways for optimization of the conditions of laser induced photothermal effects. Experimental in vitro study of hyperthermia with use of upconversion nanoparticles on HeLa and C6 cell lines was performed. The investigated nanoparticles are capable of in vitro photothermal heating, luminescent localization and thermal sensing.

Synthesis of NaYF4:Yb/Er/Gd up-conversion luminescent nanoparticles and luminescence resonance energy transfer-based protein detection

PubMed Central

Zhang, Jingpu; Mi, Congcong; Wu, Hongyan; Huang, Huaiqing; Mao, Chuanbin; Xu, Shukun

2012-01-01

High-quality NaYF4:Yb/Er/Gd up-conversion nanoparticles (UCNPs) were first synthesized by a solvothermal method using rare earth stearate, sodium fluoride, ethanol, water, and oleic acid as precursors. Doped Gd3+ ions can promote the transition of NaYF4 from cubic to hexagonal phase, shorten the reaction time, and reduce the reaction temperature without reducing the luminescence intensity of NaYF4:Yb/Er UCNPs. X-ray diffraction, infrared spectroscopy, transmission electron microscopy, and luminescence spectroscopy were applied to characterize the UCNPs. The nanoparticles exhibited small size and excellent green up-conversion photoluminescence, making them suitable for biological applications. After the surfaces of NaYF4:Yb/Er/Gd UCNPs were modified with amino groups through the Stöber method, they could be brought close enough to the analytically important protein called R-phycoerythrin (R-PE) bearing multiple carboxyl groups so that energy transfer could occur. A luminescence resonance energy transfer (LRET) system was developed using NaYF4:Yb/Er/Gd UCNPs as an energy donor and R-PE as an energy acceptor. As a result, a detection limit of R-PE of 0.5 μg/ml was achieved by the LRET system with a relative standard deviation of 2.0%. Although this approach was first used successfully to detect R-PE, it can also be extended to the detection of other biological molecules. PMID:22155069

Low-noise mid-IR upconversion detector for improved IR-degenerate four-wave mixing gas sensing.

PubMed

Høgstedt, Lasse; Dam, Jeppe Seidelin; Sahlberg, Anna-Lena; Li, Zhongshan; Aldén, Marcus; Pedersen, Christian; Tidemand-Lichtenberg, Peter

2014-09-15

We compare a nonlinear upconversion detector with a conventional cryogenic InSb detector for the detection of coherent infrared light showing near-shot-noise-limited performance in the upconversion system. The InSb detector is limited by dark noise, which results in a 500 times lower signal-to-noise ratio. The two detectors are compared for the detection of a coherent degenerate four-wave mixing (DFWM) signal in the mid-infrared, and applied to measure trace-level acetylene in a gas flow at atmospheric pressure, probing its fundamental rovibrational transitions. In addition to lower noise, the upconversion system provides image information of the signal, thus adding new functionality compared to standard point detection methods. We further show that the upconversion detector system can be implemented as a simple replacement of the cryogenic detector.

Chemical sensing and imaging based on photon upconverting nano- and microcrystals: a review

NASA Astrophysics Data System (ADS)

Christ, Simon; Schäferling, Michael

2015-09-01

The demand for photostable luminescent reporters that absorb and emit light in the red to near-infrared (NIR) spectral region continues in biomedical research and bioanalysis. In recent years, classical organic fluorophores have increasingly been displaced by luminescent nanoparticles. These consist of either polymer or silica based beads that are loaded with luminescent dyes, conjugated polymers, or inorganic nanomaterials such as semiconductor nanocrystals (quantum dots), colloidal clusters of silver and gold, or carbon dots. Among the inorganic materials, photon upconversion nanocrystals exhibit a high potential for application to bioimaging or biomolecular assays. They offer an exceptionally high photostability, can be excited in the NIR, and their anti-Stokes emission enables luminescence detection free of background and perturbing scatter effects even in complex biological samples. These lanthanide doped inorganic crystals have multiple emission lines that can be tuned by the selection of the dopants. This review article is focused on the applications of functionalized photon upconversion nanoparticles (UCNPs) to chemical sensing. This is a comparatively new field of research activity and mainly directed at the sensing and imaging of ubiquitous chemical analytes in biological samples, particularly in living cells. For this purpose, the particles have to be functionalized with suitable indicator dyes or recognition elements, as they do not show an intrinsic or specific luminescence response to most of these analytes (e.g. pH, oxygen, metal ions). We describe the strategies for the design of such responsive nanocomposites utilizing either luminescence resonance energy transfer or emission-reabsorption (inner filter effect) mechanisms and also highlight examples for their use either immobilized in sensor layers or directly as nanoprobes for intracellular sensing and imaging.

Accurate thermometry based on the red and green fluorescence intensity ratio in NaYF₄: Yb, Er nanocrystals for bioapplication.

PubMed

Liu, Lixin; Qin, Feng; Lv, Tianquan; Zhang, Zhiguo; Cao, Wenwu

2016-10-15

A biological temperature measurement method based on the fluorescence intensity ratio (FIR) was developed to reduce uncertainty. The upconversion luminescence of NaYF₄:Yb, Er nanocrystals was studied as a function of temperature around the physiologically relevant range of 300-330 K. We found that the green-green FIR Fe and red-green FIR (I₆₆₀/I₅₄₀) varied linearly as temperature increased. The thermometric uncertainties using the two FIRs were discussed and were determined to be almost constant at 0.6 and 0.09 K for green-green and red-green, respectively. The lower thermometric uncertainty comes from the intense signal-to-noise ratio of the measured FIRs owing to their comparable fluorescence intensities.

Upconversion fluorescence tyrosine doped LaF3:Dy quantum dots useful in biolabeling and biotagging

NASA Astrophysics Data System (ADS)

Singh, Amit T.; Khandpekar, M. M.

2018-04-01

Water soluble hexahedral colloidal quantum dots (QDOTs) of Tyrosine doped LaF3:Dy have been synthesized by wet chemical route. The nanoparticles have been irradiated by microwave during synthesis for drying and also to reduce agglomeration. The coating of the LaF3:Dy nanoparticles by the amino acid tyrosine results in colloidal quantum dots. XRD studies indicates hexagonal lattice and confirms JCPDS data. The average particle size obtained by XRD and SEM are 22.89nm and 25.5nm respectively. The average sizes of nanorods obtained from TEM are 55 nm. The presence of elements has been verified with EDAX and ICP-AES technique. The SAED pattern of the samples shows sharp concentric rings indicating the crystalline nature of the synthesized nanoparticles. The FTIR spectra have been used to study the surface modification of the nanoparticles. The optical studies have been done using UV-visible and PL spectra. The PL spectra showed upconversion nature of the synthesized nanoparticles with sharp emission at 618 nm. The nanoparticles synthesized have potential application as biomaterials in bio imaging and biotagging.

Specific Visualization of Tumor Cells Using Upconversion Nanophosphors

PubMed Central

Grebenik, E. A.; Generalova, A. N.; Nechaev, A. V.; Khaydukov, E.V.; Mironova, K. E.; Stremovskiy, O. A.; Lebedenko, E.N.; Zvyagin, A. V.; Deyev, S. M.

2014-01-01

The development of targeted constructs on the basis of photoluminescent nanoparticles with a high photo- and chemical stability and absorption/emission spectra in the “transparency window” of biological tissues is an important focus area of present-day medical diagnostics. In this work, a targeted two-component construct on the basis of upconversion nanophosphors (UCNPs) and anti-tumor 4D5 scFv was developed for selective labeling of tumor cells overexpressing the HER2 tumor marker characteristic of a number of human malignant tumors. A high affinity barnase : barstar (Bn : Bs) protein pair, which exhibits high stability in a wide range of pH and temperatures, was exploited as a molecular adapter providing self-assembly of the two-component construct. High selectivity for the binding of the two-component 4D5 scFv-Bn : UCNP-Bs construct to human breast adenocarcinoma SK-BR-3 cells overexpressing HER2 was demonstrated. This approach provides an opportunity to produce similar constructs for the visualization of different specific markers in pathogenic tissues, including malignant tumors. PMID:25558394

Titanium Dioxide/Upconversion Nanoparticles/Cadmium Sulfide Nanofibers Enable Enhanced Full-Spectrum Absorption for Superior Solar Light Driven Photocatalysis.

PubMed

Zhang, Fu; Zhang, Chuan-Ling; Wang, Wan-Ni; Cong, Huai-Ping; Qian, Hai-Sheng

2016-06-22

In this work, we demonstrate an electrospinning technique to fabricate TiO2 /upconversion nanoparticles (UCNPs)/CdS nanofibers on large scale. In addition, the as-prepared TiO2 nanofibers are incorporated with a high population of UCNPs and CdS nanospheres; this results in Förster resonance energy-transfer configurations of the UCNPs, TiO2 , and CdS nanospheres that are in close proximity. Hence, strong fluorescent emissions for the Tm(3+) ions including the (1) G4 →(3) H6 transition are efficiently transferred to TiO2 and the CdS nanoparticles through an energy-transfer process. The as-prepared TiO2 /UCNPs/CdS nanofibers exhibit full-spectrum solar-energy absorption and enable the efficient degradation of organic dyes by fluorescence resonance energy transfer between the UCNPs and TiO2 (or CdS). The UCNPs/TiO2 /CdS nanofibers may also have enhanced energy-transfer efficiency for wide applications in solar cells, bioimaging, photodynamics, and chemotherapy. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fast and long-range triplet exciton diffusion in metal-organic frameworks for photon upconversion at ultralow excitation power.

PubMed

Mahato, Prasenjit; Monguzzi, Angelo; Yanai, Nobuhiro; Yamada, Teppei; Kimizuka, Nobuo

2015-09-01

The conversion of low-energy light into photons of higher energy based on sensitized triplet-triplet annihilation upconversion (TTA-UC) has emerged as a promising wavelength-shifting methodology because it permits UC at excitation powers as low as the solar irradiance. However, its application has been significantly hampered by the slow diffusion of excited molecules in solid matrices. Here, we introduce metal-organic frameworks (MOFs) that promote TTA-UC by taking advantage of triplet exciton migration among fluorophores that are regularly aligned with spatially controlled chromophore orientations. We synthesized anthracene-containing MOFs with different molecular orientations, and the analysis of TTA-UC emission kinetics unveiled a high triplet diffusion rate with a micrometre-scale diffusion length. Surface modification of MOF nanocrystals with donor molecules and their encapsulation in glassy poly(methyl methacrylate) (PMMA) allowed the construction of molecular-diffusion-free solid-state upconverters, which lead to an unprecedented maximization of overall UC quantum yield at excitation powers comparable to or well below the solar irradiance.

Upconversion luminescent logic gates and turn-on sensing of glutathione based on two-photon excited quantum dots conjugated with dopamine.

PubMed

Gui, Rijun; Jin, Hui; Liu, Xifeng; Wang, Zonghua; Zhang, Feifei; Xia, Jianfei; Yang, Min; Bi, Sai

2014-12-07

Under the two-photon excitation, upconversion luminescent "INHIBIT" and "OR" logic gates of water-dispersed CdTe quantum dots (QDs) were constituted by conjugating the QDs with dopamine. This facilitated the development of a novel QDs-based upconversion luminescent probe for efficient turn-on sensing of glutathione.

Thermal noise in mid-infrared broadband upconversion detectors.

PubMed

Barh, Ajanta; Tidemand-Lichtenberg, Peter; Pedersen, Christian

2018-02-05

Low noise detection with state-of-the-art mid-infrared (MIR) detectors (e.g., PbS, PbSe, InSb, HgCdTe) is a primary challenge owing to the intrinsic thermal background radiation of the low bandgap detector material itself. However, researchers have employed frequency upconversion based detectors (UCD), operable at room temperature, as a promising alternative to traditional direct detection schemes. UCD allows for the use of a low noise silicon-CCD/camera to improve the SNR. Using UCD, the noise contributions from the nonlinear material itself should be evaluated in order to estimate the limits of the noise-equivalent power of an UCD system. In this article, we rigorously analyze the optical power generated by frequency upconversion of the intrinsic black-body radiation in the nonlinear material itself due to the crystals residual emissivity, i.e. absorption. The thermal radiation is particularly prominent at the optical absorption edge of the nonlinear material even at room temperature. We consider a conventional periodically poled lithium niobate (PPLN) based MIR-UCD for the investigation. The UCD is designed to cover a broad spectral range, overlapping with the entire absorption edge of the PPLN (3.5 - 5 µm). Finally, an upconverted thermal radiation power of ~30 pW at room temperature (~30°C) and a maximum of ~70 pW at 120°C of the PPLN crystal are measured for a CW mixing beam of power ~60 W, supporting a good quantitative agreement with the theory. The analysis can easily be extended to other popular nonlinear conversion processes including OPO, DFG, and SHG.

Sub-Band Gap Turn-On Near-Infrared-to-Visible Up-Conversion Device Enabled by an Organic-Inorganic Hybrid Perovskite Photovoltaic Absorber.

PubMed

Yu, By Hyeonggeun; Cheng, Yuanhang; Li, Menglin; Tsang, Sai-Wing; So, Franky

2018-05-09

Direct integration of an infrared (IR) photodetector with an organic light-emitting diode (OLED) enables low-cost, pixel-free IR imaging. However, the operation voltage of the resulting IR-to-visible up-conversion is large because of the series device architecture. Here, we report a low-voltage near-IR (NIR)-to-visible up-conversion device using formamidinium lead iodide as a NIR absorber integrated with a phosphorescent OLED. Because of the efficient photocarrier injection from the hybrid perovskite layer to the OLED, we observed a sub-band gap turn-on of the OLED under NIR illumination. The device showed a NIR-to-visible up-conversion efficiency of 3% and a luminance on/off ratio of 10 3 at only 5 V. Finally, we demonstrate pixel-free NIR imaging using the up-conversion device.

Bench-scale evaluation of water disinfection by visible-to-UVC upconversion under high-intensity irradiation.

PubMed

Cates, Ezra L; Kim, Jae-Hong

2015-12-01

The feasibility of applying visible-to-UVC upconversion (UC) luminescence to enhance the kinetics of solar water disinfection was evaluated using Lu7O5F9:Pr(3+) ceramics incorporated into a solar reactor containing E. coli suspensions. Inactivation was assessed in batch conditions using both laser and lens-concentrated sunlight excitation conditions. Under 840-mW argon laser excitation, the UC efficiency was estimated to be 1 order of magnitude greater than previously reported under lamp excitation and UVC emitted by the reactors resulted in 3.6-log inactivation in 20 min. However, experiments using ~1500 mW of concentrated natural sunlight showed no additional inactivation that could be attributed to UC within the timescale studied. Due to the fundamental and practical limitations of solar focusing, the optical concentration ratio employed herein prevented the excitation beam from achieving the power densities required to attain UC efficiencies comparable to the laser experiments. We also observed that the high intensity of both the laser and sunlight induced rapid photoreactivation by the bacteria, which detracted from net disinfection performance. The results suggest that current UC materials perform inadequately for environmental application; nonetheless, valuable qualitative and quantitative insight was gained that more explicitly defines materials development goals and considerations for application of UC to environmental technology. Copyright © 2015 Elsevier B.V. All rights reserved.

Recent advances in enhanced luminescence upconversion of lanthanide-doped NaYF4 phosphors

NASA Astrophysics Data System (ADS)

Kumar, Deepak; Verma, Kartikey; Verma, Shefali; Chaudhary, Babulal; Som, Sudipta; Sharma, Vishal; Kumar, Vijay; Swart, Hendrik C.

2018-04-01

NaYF4 is regarded as the best upconversion (UC) matrix owing to its low phonon energy, more chemical stability, and a superior refractive index. This review reports on the various synthesis techniques of lanthanide-doped NaYF4 phosphors for UC application. The UC intensity depends on different properties of the matrix and those are discussed in detail. Plasmon-enhanced luminescence UC of the lanthanide-doped NaYF4 core-shells structure is discussed based on a literature survey. The present review provides the information about how the UC intensity can be enhanced. The idea about the UC is then deliberately used for versatile applications such as luminescent materials, display devices, biomedical imaging and different security appliances. In addition, the present review demonstrates the recent trends of NaYF4 UC materials in solar cell devices. The role of NaYF4 phosphor to eradicate the spectral variance among the incident solar spectrum, semiconductor as well as the sub-band gap nature of the semiconductor materials is also discussed in detail. Considering the fact that the research status on NaYF4 phosphor for photovoltaic application is now growing, the present review is therefore very important to the researchers. More importantly, this may promote more interesting research platforms to investigate the realistic use of UC nanophosphors as spectral converters for solar cells.

Sensitive Infrared Signal Detection by Upconversion Technique

NASA Technical Reports Server (NTRS)

Wong, Teh-Hwa; Yu, Jirong; Bai, Yingxin; Johnson, William; Chen, Songsheng; Petros, Mulugeta; Singh, Upendra N.

2014-01-01

We demonstrated upconversion assisted detection of a 2.05-micron signal by sum frequency generation to generate a 700-nm light using a bulk periodically poled lithium niobate crystal. The achieved 94% intrinsic upconversion efficiency and 22.58% overall detection efficiency at a pW level of 2.05 micron pave the path to detect extremely weak infrared (IR) signals for remote sensing applications.

Facile synthesis of hydrophilic multi-colour and upconversion photoluminescent mesoporous carbon nanoparticles for bioapplications.

PubMed

Kong, Qinglu; Zhang, Lingxia; Liu, Jianan; Wu, Meiying; Chen, Yu; Feng, Jingwei; Shi, Jianlin

2014-12-25

Hydrophilic mesoporous carbon nanoparticles (MCNs) have been synthesized via an extremely facile precursor carbonization-in-hot solvent route. The synthesized MCNs show well-defined particle and pore size distribution at around 100 nm and 2.7 nm, respectively, and multicolor and upconversion photoluminescence, which endow the MCNs with multicolor/upconversion bioimaging and drug delivery properties.

Infrared upconversion for astronomical applications. [laser applications to astronomical spectroscopy of infrared spectra

NASA Technical Reports Server (NTRS)

Abbas, M. M.; Kostiuk, T.; Ogilvie, K. W.

1975-01-01

The performance of an upconversion system is examined for observation of astronomical sources in the low to middle infrared spectral range. Theoretical values for the performance parameters of an upconversion system for astronomical observations are evaluated in view of the conversion efficiencies, spectral resolution, field of view, minimum detectable source brightness and source flux. Experimental results of blackbody measurements and molecular absorption spectrum measurements using a lithium niobate upconverter with an argon-ion laser as the pump are presented. Estimates of the expected optimum sensitivity of an upconversion device which may be built with the presently available components are given.

Up-conversion in rare-earth doped micro-particles applied to new emissive two-dimensional displays

NASA Astrophysics Data System (ADS)

Milliez, Anne Janet

Up-conversion (UC) in rare-earth co-doped fluorides to convert diode laser light in the near infrared to red, green and blue visible light is applied to make possible high performance emissive displays. The infrared-to-visible UC in the materials we study is a sequential form of non-linear two photon absorption in which a strong absorbing constituent absorbs two low energy photons and transfers this energy to another constituent which emits visible light. Some of the UC emitters' most appealing characteristics for displays are: a wide color gamut with very saturated colors, very high brightness operation without damage to the emitters, long lifetimes and efficiencies comparable to those of existing technologies. Other advantages include simplicity of fabrication, versatility of operating modes, and the potential for greatly reduced display weight and depth. Thanks to recent advances in material science and diode laser technology at the excitation wavelength, UC selected materials can be very efficient visible emitters. However, optimal UC efficiencies strongly depend on chosing proper operating conditions. In this thesis, we studied the conditions required for optimization. We demonstrated that high efficiency UC depends on high pump irradiance, low temperature and low scattering. With this understanding we can predict how to optimally use UC emitters in a wide range of applications. In particular, we showed how our very efficient UC emitters can be applied to make full color displays and very efficient white light sources.

CdS/ZnS core-shell nanocrystal photosensitizers for visible to UV upconversion.

PubMed

Gray, Victor; Xia, Pan; Huang, Zhiyuan; Moses, Emily; Fast, Alexander; Fishman, Dmitry A; Vullev, Valentine I; Abrahamsson, Maria; Moth-Poulsen, Kasper; Lee Tang, Ming

2017-08-01

Herein we report the first example of nanocrystal (NC) sensitized triplet-triplet annihilation based photon upconversion from the visible to ultraviolet (vis-to-UV). Many photocatalyzed reactions, such as water splitting, require UV photons in order to function efficiently. Upconversion is one possible means of extending the usable range of photons into the visible. Vis-to-UV upconversion is achieved with CdS/ZnS core-shell NCs as the sensitizer and 2,5-diphenyloxazole (PPO) as annihilator and emitter. The ZnS shell was crucial in order to achieve any appreciable upconversion. From time resolved photoluminescence and transient absorption measurements we conclude that the ZnS shell affects the NC and triplet energy transfer (TET) from NC to PPO in two distinct ways. Upon ZnS growth the surface traps are passivated thus increasing the TET. The shell, however, also acts as a tunneling barrier for TET, reducing the efficiency. This leads to an optimal shell thickness where the upconversion quantum yield ( Φ ' UC ) is maximized. Here the maximum Φ ' UC was determined to be 5.2 ± 0.5% for 4 monolayers of ZnS shell on CdS NCs.

Color-tunable up-conversion emission from Yb{sup 3+}/Er{sup 3+}/Tm{sup 3+} tri-doped T-AgGd(W,Mo){sub 2}O{sub 8} phosphors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Jijian; Liu, Ni; Xu, Ling, E-mail: xuling@snnu.edu.cn

Graphical abstract: The doping ions tune the UC luminescence of the T- AgGd(W,Mo){sub 2}O{sub 8}:Yb{sup 3+}/Er{sup 3+}/Tm{sup 3+} material. - Highlights: • AgGd(W,Mo){sub 2}O{sub 8}:Yb{sup 3+}/Er{sup 3+}/Tm{sup 3+} phosphors show color-tunable blue, green, and red UC emissions. • The samples’ UC emission color can be switched with the concentrations of doped ions. • The blue, green and red UC mechanisms are interpreted reasonably as three- and two- photon process. - Abstract: Tetragonal Yb{sup 3+}/Er{sup 3+}/Tm{sup 3+} tri-doped AgGd(W,Mo){sub 2}O{sub 8} phosphors were prepared by the high-temperature solid-state method. When the phosphors were excited at 980 nm, the UC emission ofmore » blue at 475 nm, green at 525 and 550 nm, and red at 656 nm were corresponding to the {sup 1}G{sub 4} → {sup 3}H{sub 6} transition of Tm{sup 3+} ions, the {sup 2}H{sub 11/2},{sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} transitions of Er{sup 3+} ions, and the {sup 4}F{sub 9/2} → {sup 4}I{sub 15/2} transition of Er{sup 3+} ions, respectively. The blue UC emissions originate from a three-photon mechanism, while the green and red ones of Er{sup 3+} from two-photon process. The UC emission color of the Yb{sup 3+}/Er{sup 3+}/Tm{sup 3+} tri-doped AgGdW{sub 2}O{sub 8} samples switched from green to white, and then to red depending on the concentrations of Er{sup 3+} and Tm{sup 3+}. After doping with Mo(VI), tetragonal AgGdW{sub 2}O{sub 8} was transformed into tetragonal AgGdMo{sub 2}O{sub 8}, resulting in a slightly enhanced UC luminescence intensity with the favor of the red emission of Er{sup 3+} ion.« less

Taking the temperature of the interiors of magnetically heated nanoparticles.

PubMed

Dong, Juyao; Zink, Jeffrey I

2014-05-27

The temperature increase inside mesoporous silica nanoparticles induced by encapsulated smaller superparamagnetic nanocrystals in an oscillating magnetic field is measured using a crystalline optical nanothermometer. The detection mechanism is based on the temperature-dependent intensity ratio of two luminescence bands in the upconversion emission spectrum of NaYF4:Yb(3+), Er(3+). A facile stepwise phase transfer method is developed to construct a dual-core mesoporous silica nanoparticle that contains both a nanoheater and a nanothermometer in its interior. The magnetically induced heating inside the nanoparticles varies with different experimental conditions, including the magnetic field induction power, the exposure time to the magnetic field, and the magnetic nanocrystal size. The temperature increase of the immediate nanoenvironment around the magnetic nanocrystals is monitored continuously during the magnetic oscillating field exposure. The interior of the nanoparticles becomes much hotter than the macroscopic solution and cools to the temperature of the ambient fluid on a time scale of seconds after the magnetic field is turned off. This continuous absolute temperature detection method offers quantitative insight into the nanoenvironment around magnetic materials and opens a path for optimizing local temperature controls for physical and biomedical applications.

Upconversion in solar cells

PubMed Central

2013-01-01

The possibility to tune chemical and physical properties in nanosized materials has a strong impact on a variety of technologies, including photovoltaics. One of the prominent research areas of nanomaterials for photovoltaics involves spectral conversion. Modification of the spectrum requires down- and/or upconversion or downshifting of the spectrum, meaning that the energy of photons is modified to either lower (down) or higher (up) energy. Nanostructures such as quantum dots, luminescent dye molecules, and lanthanide-doped glasses are capable of absorbing photons at a certain wavelength and emitting photons at a different (shorter or longer) wavelength. We will discuss upconversion by lanthanide compounds in various host materials and will further demonstrate upconversion to work for thin-film silicon solar cells. PMID:23413889

Red, green, and blue luminescence by carbon dots: full-color emission tuning and multicolor cellular imaging.

PubMed

Jiang, Kai; Sun, Shan; Zhang, Ling; Lu, Yue; Wu, Aiguo; Cai, Congzhong; Lin, Hengwei

2015-04-27

A facile approach for preparation of photoluminescent (PL) carbon dots (CDs) is reported. The three resulting CDs emit bright and stable red, green and blue (RGB) colors of luminescence, under a single ultraviolet-light excitation. Alterations of PL emission of these CDs are tentatively proposed to result from the difference in their particle size and nitrogen content. Interestingly, up-conversion (UC)PL of these CDs is also observed. Moreover, flexible full-color emissive PVA films can be achieved through mixing two or three CDs in the appropriate ratios. These CDs also show low cytotoxicity and excellent cellular imaging capability. The facile preparation and unique optical features make these CDs potentially useful in numerous applications such as light-emitting diodes, full-color displays, and multiplexed (UC)PL bioimaging. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Amplifying the Red-Emission of Upconverting Nanoparticles for Biocompatible Clinically Used Prodrug-Induced Photodynamic Therapy

DOE PAGES

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira; ...

2014-09-25

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP–PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major stepmore » forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors.Lastly, it also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.« less

Amplifying the red-emission of upconverting nanoparticles for biocompatible clinically used prodrug-induced photodynamic therapy.

PubMed

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira; El-Rifai, Mahmoud; Lee, Hyungseok; Zhang, Yuanwei; Wang, Chao; Liu, Zhuang; Chan, Emory M; Duan, Chunying; Han, Gang

2014-10-28

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP-PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major step forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors. It also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.

Photoluminescence of Er-doped silicon-rich oxide thin films with high Al concentrations

NASA Astrophysics Data System (ADS)

Rozo, Carlos; Fonseca, Luis F.; Jaque, Daniel; García Solé, José

Er-doped silicon-rich oxide (SRO) thin films co-doped with Al in high concentrations were prepared by sputtering. Some films were deposited using a substrate heater (150 °C

Amplifying the Red-Emission of Upconverting Nanoparticles for Biocompatible Clinically Used Prodrug-Induced Photodynamic Therapy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP–PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major stepmore » forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors.Lastly, it also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.« less

Effect of silica surface coating on the luminescence lifetime and upconversion temperature sensing properties of semiconductor zinc oxide doped with gallium(III) and sensitized with rare earth ions Yb(III) and Tm(III).

PubMed

Li, Yuemei; Li, Yongmei; Wang, Rui; Zheng, Wei

2018-02-26

Optical sensing of temperature by measurement of the ratio of the intensities of the 700 nm emission and the 800 nm emission of Ga(III)-doped ZnO (GZO) nanoparticles (NPs) and of GZO NPs coated with a silica shell are demonstrated at 980 nm excitation. It is found that the relative sensitivity of SiO 2 @Yb/Tm/GZO is 6.2% K -1 at a temperature of 693 K. This is ~3.4 times higher than that of Yb/Tm/GZO NPs. Obviously, the SiO 2 shell structure decreases the rate of the nonradiative decay. The decay time of the 800 nm emission of the Yb/Tm/GZO NPs (15 mol% Ga; 7 mol% Yb; 0.5 mol% Tm) displays a biexponential decay with a dominant decay time of 148 μs and a second decay time of ~412 μs. The lifetime of the Yb/Tm/GZO NPs at 293 K, and of the SiO 2 @Yb/Tm/GZO NPs are ~412 μs. Both the Yb/Tm/GZO and SiO 2 @Yb/Tm/GZO can be used up to 693 K. These results indicate that the SiO 2 shell on the Yb/Tm/GZO is beneficial in terms of sensitivity and resolution. Graphical abstract The enhancement the decay time and thermal sensitivity in the SiO 2 @Yb/Tm/GZO shell@core structure have been studied compared to the Ga(III)-doped Yb/Tm-doped ZnO (Yb/Tm/GZO). The SiO 2 @Yb/Tm/GZO have good thermal accuracy up to 693 °C.

Photon energy upconverting nanopaper: a bioinspired oxygen protection strategy.

PubMed

Svagan, Anna J; Busko, Dmitry; Avlasevich, Yuri; Glasser, Gunnar; Baluschev, Stanislav; Landfester, Katharina

2014-08-26

The development of solid materials which are able to upconvert optical radiation into photons of higher energy is attractive for many applications such as photocatalytic cells and photovoltaic devices. However, to fully exploit triplet-triplet annihilation photon energy upconversion (TTA-UC), oxygen protection is imperative because molecular oxygen is an ultimate quencher of the photon upconversion process. So far, reported solid TTA-UC materials have focused mainly on elastomeric matrices with low barrier properties because the TTA-UC efficiency generally drops significantly in glassy and semicrystalline matrices. To overcome this limit, for example, combine effective and sustainable annihilation upconversion with exhaustive oxygen protection of dyes, we prepare a sustainable solid-state-like material based on nanocellulose. Inspired by the structural buildup of leaves in Nature, we compartmentalize the dyes in the liquid core of nanocellulose-based capsules which are then further embedded in a cellulose nanofibers (NFC) matrix. Using pristine cellulose nanofibers, a sustainable and environmentally friendly functional nanomaterial with ultrahigh barrier properties is achieved. Also, an ensemble of sensitizers and emitter compounds are encapsulated, which allow harvesting of the energy of the whole deep-red sunlight region. The films demonstrate excellent lifetime in synthetic air (20.5/79.5, O2/N2)-even after 1 h operation, the intensity of the TTA-UC signal decreased only 7.8% for the film with 8.8 μm thick NFC coating. The lifetime can be further modulated by the thickness of the protective NFC coating. For comparison, the lifetime of TTA-UC in liquids exposed to air is on the level of seconds to minutes due to fast oxygen quenching.

Fluorescence investigation of Ho3+ in Yb3+ sensitized mixed-alkali bismuth gallate glasses.

PubMed

Lin, H; Zhang, Y Y; Pun, E Y B

2008-12-15

Efficient 2.0 microm infrared and visible upconversion emissions have been observed in Ho3+/Yb3+ co-doped mixed-alkali bismuth gallate (LKBBG) glasses having a maximum-phonon energy of 673 cm(-1). The Judd-Ofelt parameters Omega2, Omega4 and Omega6 of Ho3+ indicate that there is a high asymmetry and strong covalent environment in LKBBG glasses. The large absorption and emission cross-sections of Yb3+ confirm that it is a suitable sensitizer for capturing and transferring pump energy to Ho3+. The emission cross-section profile for the 5I7-->5I8 transition is derived using the reciprocity method and the peak value is 5.54 x 10(-21)cm2, which is much larger than the value in fluorozircoaluminate glasses. LKBBG glasses exhibit low maximum-phonon energy and large refractive index, and it is possible to achieve an effective 1.66 microm U-band emission of Ho3+ under 900 nm laser radiation.

One-step hydrothermal synthesis of carboxyl-functionalized upconversion phosphors for bioapplications.

PubMed

Yang, Jianping; Shen, Dengke; Li, Xiaomin; Li, Wei; Fang, Yin; Wei, Yong; Yao, Chi; Tu, Bo; Zhang, Fan; Zhao, Dongyuan

2012-10-22

In this paper, we report a facile one-step hydrothermal method to synthesize phase-, size-, and shape-controlled carboxyl-functionalized rare-earth fluorescence upconversion phosphors by using a small-molecule binary acid, such as malonic acid, oxalic acid, succinic acid, or tartaric acid as capping agent. The crystals, from nano- to microstructures with diverse shapes that include nanospheres, microrods, hexagonal prisms, microtubes, microdisks, polygonal columns, and hexagonal tablets, can be obtained with different reaction times, reaction temperatures, molar ratios of capping agent to sodium hydroxide, and by varying the binary acids. Fourier transform infrared, thermogravimetric analysis, and upconversion luminescence spectra measurements indicate that the synthesized NaYF(4):Yb/Er products with hydrophilic carboxyl-functionalized surface offer efficient upconversion luminescent performance. Furthermore, the antibody/secondary antibody conjugation can be realized by the carboxyl-functionalized surfaces of the upconversion phosphors, thus indicating the potential bioapplications of these kinds of materials. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Upconversion-Triggered Charge Separation in Polymer Semiconductors.

PubMed

Jang, Yu Jin; Kim, Eunah; Ahn, Seonghyeon; Chung, Kyungwha; Kim, Jihyeon; Kim, Heejun; Wang, Huan; Lee, Jiseok; Kim, Dong-Wook; Kim, Dong Ha

2017-01-19

Upconversion is a unique optical property that is driven by a sequential photon pumping and generation of higher energy photons in a consecutive manner. The efficiency improvement in photovoltaic devices can be achieved when upconverters are integrated since upconverters contribute to the generation of extra photons. Despite numerous experimental studies confirming the relationship, fundamental explanations for a real contribution of upconversion to photovoltaic efficiency are still in demand. In this respect, we suggest a new approach to visualize the upconversion event in terms of surface photovoltage (SPV) by virtue of Kelvin probe force microscopy (KPFM). One of the most conventional polymer semiconductors, poly(3-hexyl thiophene) (P3HT), is employed as a sensitizer to generate charge carriers by upconverted light. KPFM measurements reveal that the light upconversion enabled the formation of charge carriers in P3HT, resulting in large SPV of -54.9 mV. It confirms that the energy transfer from upconverters to P3HT can positively impact the device performance in organic solar cells (OSCs).

Enhanced Upconversion Luminescence in Yb3+/Tm3+-Codoped Fluoride Active Core/Active Shell/Inert Shell Nanoparticles through Directed Energy Migration.

PubMed

Qiu, Hailong; Yang, Chunhui; Shao, Wei; Damasco, Jossana; Wang, Xianliang; Ågren, Hans; Prasad, Paras N; Chen, Guanying

2014-01-03

The luminescence efficiency of lanthanide-doped upconversion nanoparticles is of particular importance for their embodiment in biophotonic and photonic applications. Here, we show that the upconversion luminescence of typically used NaYF₄:Yb 3+ 30%/Tm 3+ 0.5% nanoparticles can be enhanced by ~240 times through a hierarchical active core/active shell/inert shell (NaYF₄:Yb 3+ 30%/Tm 3+ 0.5%)/NaYbF₄/NaYF₄ design, which involves the use of directed energy migration in the second active shell layer. The resulting active core/active shell/inert shell nanoparticles are determined to be about 11 times brighter than that of well-investigated (NaYF₄:Yb 3+ 30%/Tm 3+ 0.5%)/NaYF₄ active core/inert shell nanoparticles when excited at ~980 nm. The strategy for enhanced upconversion in Yb 3+ /Tm 3+ -codoped NaYF₄ nanoparticles through directed energy migration might have implications for other types of lanthanide-doped upconversion nanoparticles.

Structural and luminescent properties of a NaYF4-aerogel composite

NASA Astrophysics Data System (ADS)

Alattar, Ashraf M.; Drexler, Matthew; Twej, Wesam A. A.; Alamgir, Faisal M.

2018-07-01

Upconversion materials, capable of energy-shifting light, have direct application in devices where the tunability of the optical spectrum can result in higher performance. Due to the low transparency of upconversion nanomaterials, it is beneficial to disperse them in a medium with a low optical attenuation coefficient in order to allow light to reach and increase the contributions from each individual particle. Silica aerogels, with their high transparency and open porosity, are ideal media for the dispersion of the nanomaterials throughout a volume. NaYF4-based nanocrystals with differing dopants were incorporated into silica xerogels and aerogels to observe the effect of the composites on the properties of each. It was observed that, while the average surface area of the aerogel decreased in the composite, the shape and phase of the nanocrystals were preserved during xerogel processing. The luminescence of the nanoparticles increased upon incorporation into the xerogel composites. By accounting for effects emerging from collection geometry and the composite morphology, it is argued that the increase in the composite luminescent intensity is due to the nanoparticles being shielded from quenching effects by the silica matrix.

Seeing the invisible plasma with transient phonons in cuprous oxide

DOE PAGES

Frazer, Laszlo; Schaller, Richard D.; Chang, Kelvin B.; ...

2016-12-12

Here, the emission of phonons from electron–hole plasma is the primary limit on the efficiency of photovoltaic devices operating above the bandgap. In cuprous oxide (Cu 2O) there is no luminescence from electron–hole plasma. Therefore, we searched for optical phonons emitted by energetic charge carriers using phonon-to-exciton upconversion transitions. We found 14 meV phonons with a lifetime of 0.916 ± 0.008 ps and 79 meV phonons that are longer lived and overrepresented. It is surprising that the higher energy phonon has a longer lifetime.

Single-step synthesis of Er3+ and Yb3+ ions doped molybdate/Gd2O3 core-shell nanoparticles for biomedical imaging

NASA Astrophysics Data System (ADS)

Kamińska, Izabela; Elbaum, Danek; Sikora, Bożena; Kowalik, Przemysław; Mikulski, Jakub; Felcyn, Zofia; Samol, Piotr; Wojciechowski, Tomasz; Minikayev, Roman; Paszkowicz, Wojciech; Zaleszczyk, Wojciech; Szewczyk, Maciej; Konopka, Anna; Gruzeł, Grzegorz; Pawlyta, Mirosława; Donten, Mikołaj; Ciszak, Kamil; Zajdel, Karolina; Frontczak-Baniewicz, Małgorzata; Stępień, Piotr; Łapiński, Mariusz; Wilczyński, Grzegorz; Fronc, Krzysztof

2018-01-01

Nanostructures as color-tunable luminescent markers have become major, promising tools for bioimaging and biosensing. In this paper separated molybdate/Gd2O3 doped rare earth ions (erbium, Er3+ and ytterbium, Yb3+) core-shell nanoparticles (NPs), were fabricated by a one-step homogeneous precipitation process. Emission properties were studied by cathodo- and photoluminescence. Scanning electron and transmission electron microscopes were used to visualize and determine the size and shape of the NPs. Spherical NPs were obtained. Their core-shell structures were confirmed by x-ray diffraction and energy-dispersive x-ray spectroscopy measurements. We postulated that the molybdate rich core is formed due to high segregation coefficient of the Mo ion during the precipitation. The calcination process resulted in crystallization of δ/ξ (core/shell) NP doped Er and Yb ions, where δ—gadolinium molybdates and ξ—molybdates or gadolinium oxide. We confirmed two different upconversion mechanisms. In the presence of molybdenum ions, in the core of the NPs, Yb3+-{{{{MoO}}}4}2- (∣2F7/2, 3T2〉) dimers were formed. As a result of a two 980 nm photon absorption by the dimer, we observed enhanced green luminescence in the upconversion process. However, for the shell formed by the Gd2O3:Er, Yb NPs (without the Mo ions), the typical energy transfer upconversion takes place, which results in red luminescence. We demonstrated that the NPs were transported into cytosol of the HeLa and astrocytes cells by endocytosis. The core-shell NPs are sensitive sensors for the environment prevailing inside (shorter luminescence decay) and outside (longer luminescence decay) of the tested cells. The toxicity of the NPs was examined using MTT assay.

Architecture, development and implementation of a SWIR to visible integrated up-conversion imaging device

NASA Astrophysics Data System (ADS)

Sarusi, Gabby; Templeman, Tzvi; Hechster, Elad; Nissim, Nimrod; Vitenberg, Vladimir; Maman, Nitzan; Tal, Amir; Solodar, Assi; Makov, Guy; Abdulhalim, Ibrahim; Visoly-Fisher, Iris; Golan, Yuval

2016-04-01

A new concept of short wavelength infrared (SWIR) to visible upconversion integrated imaging device is proposed, modeled and some initial measured results are presented. The device is a hybrid inorganic-organic device that comprises six nano-metric scale sub-layers grown on n-type GaAs substrates. The first layer is a ~300nm thick PbSe nano-columnar absorber layer grown in (111) orientation to the substrate plan (100), with a diameter of 8- 10nm and therefore exhibit quantum confinement effects parallel to the substrate and bulk properties perpendicular to it. The advantage of this structure is the high oscillator strength and hence absorption to incoming SWIR photons while maintaining the high bulk mobility of photo-excited charges along the columns. The top of the PbSe absorber layer is coated with 20nm thick metal layer that serves as a dual sided mirror, as well as a potentially surface plasmon enhanced absorption in the PbSe nano-columns layer. The photo-excited charges (holes and electrons in opposite directions) are drifted under an external applied field to the OLED section (that is composed of a hole transport layer, an emission layer and an electron transport layer) where they recombine with injected electron from the transparent cathode and emit visible light through this cathode. Due to the high absorption and enhanced transport properties this architecture has the potential of high quantum efficiency, low cost and easy implementation in any optical system. As a bench-mark, alternative concept where InGaAs/InP heterojunction couple to liquid crystal optical spatial light modulator (OSLM) structure was built that shows a full upconversion to visible of 1550nm laser light.

Designing lanthanide-doped nanocrystals with both up- and down-conversion luminescence for anti-counterfeiting

NASA Astrophysics Data System (ADS)

Liu, Yanlan; Ai, Kelong; Lu, Lehui

2011-11-01

The widespread forgery in all kinds of paper documents and certificates has become a real threat to society. Traditional fluorescent anti-counterfeiting materials generally exhibit unicolor display and suffer greatly from substitution, thus leading to a poor anti-counterfeiting effect. In this work, unseen but significant enhanced blue down-conversion emission from oleic acid-stabilized lanthanide-doped fluoride nanocrystals is first present and the mechanism is proposed and validated. This not only endows these nanocrystals with dual-mode fluorescence, but also offers a simplified synthesis approach for dual-mode fluorescent nanocrystals involving no further complicated assembly or coating procedures, unlike the traditional methods. Furthermore, by changing the host/dopant combination or the content of dopant, these nanocrystals can exhibit simultaneously multicolor up-conversion emission under excitation at near-infrared light and unalterable blue down-conversion emission under ultraviolet light. A preliminary investigation of their anti-counterfeiting performance has been made, and the results indicate that this color tuning capability and high concealment makes these nanocrystals behave in a similar way to chameleons and can provide a strengthened and more reliable anti-counterfeiting effect.The widespread forgery in all kinds of paper documents and certificates has become a real threat to society. Traditional fluorescent anti-counterfeiting materials generally exhibit unicolor display and suffer greatly from substitution, thus leading to a poor anti-counterfeiting effect. In this work, unseen but significant enhanced blue down-conversion emission from oleic acid-stabilized lanthanide-doped fluoride nanocrystals is first present and the mechanism is proposed and validated. This not only endows these nanocrystals with dual-mode fluorescence, but also offers a simplified synthesis approach for dual-mode fluorescent nanocrystals involving no further complicated assembly or coating procedures, unlike the traditional methods. Furthermore, by changing the host/dopant combination or the content of dopant, these nanocrystals can exhibit simultaneously multicolor up-conversion emission under excitation at near-infrared light and unalterable blue down-conversion emission under ultraviolet light. A preliminary investigation of their anti-counterfeiting performance has been made, and the results indicate that this color tuning capability and high concealment makes these nanocrystals behave in a similar way to chameleons and can provide a strengthened and more reliable anti-counterfeiting effect. Electronic supplementary information (ESI) available: Fig. S1-S6, Table S. See DOI: 10.1039/c1nr10752f

Multiscale optical imaging of rare-earth-doped nanocomposites in a small animal model

NASA Astrophysics Data System (ADS)

Higgins, Laura M.; Ganapathy, Vidya; Kantamneni, Harini; Zhao, Xinyu; Sheng, Yang; Tan, Mei-Chee; Roth, Charles M.; Riman, Richard E.; Moghe, Prabhas V.; Pierce, Mark C.

2018-03-01

Rare-earth-doped nanocomposites have appealing optical properties for use as biomedical contrast agents, but few systems exist for imaging these materials. We describe the design and characterization of (i) a preclinical system for whole animal in vivo imaging and (ii) an integrated optical coherence tomography/confocal microscopy system for high-resolution imaging of ex vivo tissues. We demonstrate these systems by administering erbium-doped nanocomposites to a murine model of metastatic breast cancer. Short-wave infrared emissions were detected in vivo and in whole organ imaging ex vivo. Visible upconversion emissions and tissue autofluorescence were imaged in biopsy specimens, alongside optical coherence tomography imaging of tissue microstructure. We anticipate that this work will provide guidance for researchers seeking to image these nanomaterials across a wide range of biological models.

Light up-conversion from near-infrared to blue using a photoresponsive organic light-emitting device

NASA Astrophysics Data System (ADS)

Chikamatsu, Masayuki; Ichino, Yoshiro; Takada, Noriyuki; Yoshida, Manabu; Kamata, Toshihide; Yase, Kiyoshi

2002-07-01

A photoresponsive organic light-emitting device combining blue-emitting organic electroluminescent (EL) diode with titanyl phthalocyanine as a near-infrared (IR) sensitive layer was fabricated. By irradiating near-IR light to the device, blue emission occurred in the lower drive voltage (between 5 and 12 V). The result indicates that the device acts as a light switch and/or an up-converter from near-IR light (1.6 eV) to blue (2.6 eV). The EL response times of rise and decay using a near-IR light trigger were 260 and 330 mus, respectively. At a higher voltage (above 12 V), enhancement of blue emission was observed with near-IR light irradiation. The ON/OFF ratio reached a maximum of 103.

Preparation of silica coated and 90Y-radiolabeled β-NaYF4 upconverting nanophosphors for multimodal tracing

NASA Astrophysics Data System (ADS)

Najmr, Stan; Lu, Tianfeng; Keller, Austin W.; Zhang, Mingyue; Lee, Jennifer D.; Makvandi, Mehran; Pryma, Daniel A.; Kagan, Cherie R.; Murray, Christopher B.

2018-06-01

Rare-earth (RE) compounds have been actively pursued for therapeutic and diagnostic applications due to their ability to upconvert near infrared light into the UV–vis range. Through nanoengineering and bottom-up synthesis, additional functionality can be added to these upconverting systems. Herein, we report the synthesis of 90Y-doped β-NaYF4:Er, Yb upconverting nanophosphors (UCNPs) to enable β-particle emission and upconversion by the same UCNP. To homogenously incorporate the radionuclides, we employ a hydroxide metathesis method to produce the RE precursor required for the solvothermal synthesis of monodisperse UCNPs. Once incorporated, we find that the β-emitting 90Y dopants do not influence the energy pathways required for upconversion, enabling simultaneous radio- and optical-tracing. The resulting large (>100 nm in height and width), anisotropic, 90Y-radiolabeled β-NaYF4 UCNPs are then coated with silica using a modified, micelle-driven Stöber process to enable their dispersion in polar solvents. Doing so highlights the importance of surfactant (Igepal CO-520) and silica source (tetraethyl orthosilicate) interactions to the continuity of the silica shell and makes the vast library of silica surface chemistry and functionality accessible to upconverting radiotracers.

Ultrafast fluorescence spectroscopy via upconversion applications to biophysics.

PubMed

Xu, Jianhua; Knutson, Jay R

2008-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed.

Current advances in lanthanide ion (Ln(3+))-based upconversion nanomaterials for drug delivery.

PubMed

Yang, Dongmei; Ma, Ping'an; Hou, Zhiyou; Cheng, Ziyong; Li, Chunxia; Lin, Jun

2015-03-21

Lanthanide ion (Ln(3+))-based upconversion nano/micromaterials that emit higher-energy visible light when excited by low-energy NIR light have aroused considerable attention in the forefront of materials science and biomedical fields, which stems from their unique optical and chemical properties including minimum photodamage to living organisms, low autofluorescence, high signal-to-noise ratio and detection sensitivity, and high penetration depth in biological or environmental samples. Thus, Ln(3+)-based upconversion materials are rising new stars and are quickly emerging as potential candidates to revolutionize novel biomedical applications. In this review article, we mainly focus on the recent progress in various chemical syntheses of Ln(3+)-based upconversion nanomaterials, with special emphasis on their application in stimuli-response controlled drug release and subsequent therapy. Functional groups that are introduced into the stimuli-responsive system can respond to external triggers, such as pH, temperature, light, and even magnetic fields, which can regulate the movement of the pharmaceutical cargo and release the drug at a desired time and in a desired area. This is crucial to boost drug efficacy in cancer treatment while minimizing the side effects of cytotoxic drugs. Many multifunctional (magnetic/upconversion luminescence and porous) composite materials based on Ln(3+) have been designed for controlled drug delivery and multimodal bioimaging. Finally, the challenges and future opportunities for Ln(3+)-based upconversion materials are discussed.

Enhanced Upconversion Luminescence in Yb3+/Tm3+-Codoped Fluoride Active Core/Active Shell/Inert Shell Nanoparticles through Directed Energy Migration

PubMed Central

Qiu, Hailong; Yang, Chunhui; Shao, Wei; Damasco, Jossana; Wang, Xianliang; Ågren, Hans; Prasad, Paras N.; Chen, Guanying

2014-01-01

The luminescence efficiency of lanthanide-doped upconversion nanoparticles is of particular importance for their embodiment in biophotonic and photonic applications. Here, we show that the upconversion luminescence of typically used NaYF4:Yb3+30%/Tm3+0.5% nanoparticles can be enhanced by ~240 times through a hierarchical active core/active shell/inert shell (NaYF4:Yb3+30%/Tm3+0.5%)/NaYbF4/NaYF4 design, which involves the use of directed energy migration in the second active shell layer. The resulting active core/active shell/inert shell nanoparticles are determined to be about 11 times brighter than that of well-investigated (NaYF4:Yb3+30%/Tm3+0.5%)/NaYF4 active core/inert shell nanoparticles when excited at ~980 nm. The strategy for enhanced upconversion in Yb3+/Tm3+-codoped NaYF4 nanoparticles through directed energy migration might have implications for other types of lanthanide-doped upconversion nanoparticles. PMID:28348285

Two-step photon up-conversion solar cells

PubMed Central

Asahi, Shigeo; Teranishi, Haruyuki; Kusaki, Kazuki; Kaizu, Toshiyuki; Kita, Takashi

2017-01-01

Reducing the transmission loss for below-gap photons is a straightforward way to break the limit of the energy-conversion efficiency of solar cells (SCs). The up-conversion of below-gap photons is very promising for generating additional photocurrent. Here we propose a two-step photon up-conversion SC with a hetero-interface comprising different bandgaps of Al0.3Ga0.7As and GaAs. The below-gap photons for Al0.3Ga0.7As excite GaAs and generate electrons at the hetero-interface. The accumulated electrons at the hetero-interface are pumped upwards into the Al0.3Ga0.7As barrier by below-gap photons for GaAs. Efficient two-step photon up-conversion is achieved by introducing InAs quantum dots at the hetero-interface. We observe not only a dramatic increase in the additional photocurrent, which exceeds the reported values by approximately two orders of magnitude, but also an increase in the photovoltage. These results suggest that the two-step photon up-conversion SC has a high potential for implementation in the next-generation high-efficiency SCs. PMID:28382945

Enhancing Solar Cell Efficiency Using Photon Upconversion Materials

PubMed Central

Shang, Yunfei; Hao, Shuwei; Yang, Chunhui; Chen, Guanying

2015-01-01

Photovoltaic cells are able to convert sunlight into electricity, providing enough of the most abundant and cleanest energy to cover our energy needs. However, the efficiency of current photovoltaics is significantly impeded by the transmission loss of sub-band-gap photons. Photon upconversion is a promising route to circumvent this problem by converting these transmitted sub-band-gap photons into above-band-gap light, where solar cells typically have high quantum efficiency. Here, we summarize recent progress on varying types of efficient upconversion materials as well as their outstanding uses in a series of solar cells, including silicon solar cells (crystalline and amorphous), gallium arsenide (GaAs) solar cells, dye-sensitized solar cells, and other types of solar cells. The challenge and prospect of upconversion materials for photovoltaic applications are also discussed. PMID:28347095

New nanoplatforms based on UCNPs linking with polyhedral oligomeric silsesquioxane (POSS) for multimodal bioimaging

NASA Astrophysics Data System (ADS)

Ge, Xiaoqian; Dong, Liang; Sun, Lining; Song, Zhengmei; Wei, Ruoyan; Shi, Liyi; Chen, Haige

2015-04-01

A new and facile method was used to transfer upconversion luminescent nanoparticles from hydrophobic to hydrophilic using polyhedral oligomeric silsesquioxane (POSS) linking on the surface of upconversion nanoparticles. In comparison with the unmodified upconversion nanoparticles, the POSS modified upconversion nanoplatforms [POSS-UCNPs(Er), POSS-UCNPs(Tm)] displayed good monodispersion in water and exhibited good water-solubility, while their particle size did not change substantially. Due to the low cytotoxicity and good biocompatibility as determined by methyl thiazolyl tetrazolium (MTT) assay and histology and hematology analysis, the POSS modified upconversion nanoplatforms were successfully applied to upconversion luminescence imaging of living cells in vitro and nude mouse in vivo (upon excitation at 980 nm). In addition, the doped Gd3+ ion endows the POSS-UCNPs with effective T1 signal enhancement and the POSS-UCNPs were successfully applied to in vivo magnetic resonance imaging (MRI) for a Kunming mouse, which makes them potential MRI positive-contrast agents. More importantly, the corner organic groups of POSS can be easily modified, resulting in kinds of POSS-UCNPs with many potential applications. Therefore, the method and results may provide more exciting opportunities for multimodal bioimaging and multifunctional applications.A new and facile method was used to transfer upconversion luminescent nanoparticles from hydrophobic to hydrophilic using polyhedral oligomeric silsesquioxane (POSS) linking on the surface of upconversion nanoparticles. In comparison with the unmodified upconversion nanoparticles, the POSS modified upconversion nanoplatforms [POSS-UCNPs(Er), POSS-UCNPs(Tm)] displayed good monodispersion in water and exhibited good water-solubility, while their particle size did not change substantially. Due to the low cytotoxicity and good biocompatibility as determined by methyl thiazolyl tetrazolium (MTT) assay and histology and hematology analysis, the POSS modified upconversion nanoplatforms were successfully applied to upconversion luminescence imaging of living cells in vitro and nude mouse in vivo (upon excitation at 980 nm). In addition, the doped Gd3+ ion endows the POSS-UCNPs with effective T1 signal enhancement and the POSS-UCNPs were successfully applied to in vivo magnetic resonance imaging (MRI) for a Kunming mouse, which makes them potential MRI positive-contrast agents. More importantly, the corner organic groups of POSS can be easily modified, resulting in kinds of POSS-UCNPs with many potential applications. Therefore, the method and results may provide more exciting opportunities for multimodal bioimaging and multifunctional applications. Electronic supplementary information (ESI) available: Schematic illustration of the formation of POSS-UCNPs. TEM images of NaYF4:Yb,Tm and NaYF4:Yb,Tm@NaGdF4 nanoparticles in cyclohexane; the TEM image of POSS-UCNPs(Tm) in water. DLS of POSS-UCNPs(Tm) in water. The energy dispersive X-ray (EDX) spectrum of POSS-UCNPs(Er). XPS of POSS-UCNPs(Er); XPS of Si element. UCL spectra of POSS-UCNPs(Er) in physiology saline as a function of time. UCL spectra of NaYF4:Yb,Tm@NaGdF4 [UCNPs(Tm)] and POSS-UCNPs(Tm), excited with a 980 nm laser (100 mW cm-2). In vivo UCL imaging of Kunming mice after intravenous injection with POSS-UCNPs(Tm) at different time points. See DOI: 10.1039/c5nr00950b

Near-infrared light-activated red-emitting upconverting nanoplatform for T1-weighted magnetic resonance imaging and photodynamic therapy.

PubMed

Tang, Xiang-Long; Wu, Jun; Lin, Ben-Lan; Cui, Sheng; Liu, Hong-Mei; Yu, Ru-Tong; Shen, Xiao-Dong; Wang, Ting-Wei; Xia, Wei

2018-05-12

Photodynamic therapy (PDT) has increasingly become an efficient and attractive cancer treatment modality based on reactive oxygen species (ROS) that can induce tumor death after irradiation with ultraviolet or visible light. Herein, to overcome the limited tissue penetration in traditional PDT, a novel near-infrared (NIR) light-activated NaScF 4 : 40% Yb, 2% Er@CaF 2 upconversion nanoparticle (rUCNP) is successfully designed and synthesized. Chlorin e6, a photosensitizer and a chelating agent for Mn 2+ , is loaded into human serum albumin (HSA) that further conjugates onto rUCNPs. To increase the ability to target glioma tumor, an acyclic Arg-Gly-Asp peptide (cRGDyK) is linked to rUCNPs@HSA(Ce6-Mn). This nanoplatform enables efficient adsorption and conversion of NIR light (980 nm) into bright red emission (660 nm), which can trigger the photosensitizer Ce6-Mn complex for PDT and T 1 -weighted magnetic resonance imaging (T 1 -weighted MRI) for glioma diagnosis. Our in vitro and in vivo experiments demonstrate that NIR light-activated and glioma tumor-targeted PDT can generate large amounts of intracellular ROS that induce U87 cell apoptosis and suppress glioma tumor growth owing to the deep tissue penetration of irradiated light and excellent tumor-targeting ability. Thus, this nanoplatform holds potential for applications in T 1 -weighted MRI diagnosis and PDT of glioma for antitumor therapy. A near-infrared (NIR) light-activated nanoplatform for photodynamic therapy (PDT) was designed and synthesized. The Red-to-Green (R/G) ratio of NaScF 4 : 40% Yb, 2% Er almost reached 9, a value that was much higher than that of a traditional Yb/Er-codoped upconversion nanoparticle (rUCNP). By depositing a CaF 2 shell, the red-emission intensities of the rUCNPs were seven times strong as that of NaScF 4 : 40% Yb, 2% Er. The enhanced red-emitting rUCNPs could be applied in many fields such as bioimaging, controlled release, and real-time diagnosis. The nanoplatform had a strong active glioma-targeting ability, and all results achieved on subcutaneous glioma demonstrated that our NIR light-activated red-emitting upconverting nanoplatform was efficient for PDT. By loading Ce6-Mn complex into rUCNPs@HSA-RGD, the nanoplatform could be used as a T 1 -weighted magnetic resonance imaging agent for tumor diagnosis. Copyright © 2018 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Ultrafast Fluorescence Spectroscopy via Upconversion: Applications to Biophysics

PubMed Central

Xu, Jianhua; Knutson, Jay R.

2012-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed. PMID:19152860

Upconversion of Tm3+ ions in BaY2F8

NASA Astrophysics Data System (ADS)

Ruan, Yongfeng; Tsuboi, Taiju

1999-06-01

Up-conversion of red light with wavelength of 660 nm in Tm3+-doped BaY2F8 powder results in the two violet luminescence bands with peaks at 417 and 430 nm and two blue luminescence bands with peaks at 455 and 470 nm. The two violet bands are observed to be stronger than the blue bands. The blue luminescence is also observed by pumping with 993 nm light. The up-conversion is explained by a multiple excited state absorption process.

Microwave sol–gel synthesis and upconversion photoluminescence properties of CaGd{sub 2}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} phosphors with incommensurately modulated structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lim, Chang Sung; Aleksandrovsky, Aleksandr; Department of Photonics and Laser Technologies, Siberian Federal University, Krasnoyarsk 660079

2015-08-15

CaGd{sub 2−x}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} phosphors with the doping concentrations of Er{sup 3+} and Yb{sup 3+} (x=Er{sup 3+}+Yb{sup 3+}, Er{sup 3+}=0.05, 0.1, 0.2 and Yb{sup 3+}=0.2, 0.45) have been successfully synthesized by the microwave sol–gel method. The crystal structure of CaGd{sub 2−x}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} tungstates have been refined, and upconversion photoluminescence properties have been investigated. The synthesized particles, being formed after the heat-treatment at 900 °C for 16 h, showed a well crystallized morphology. Under the excitation at 980 nm, CaGd{sub 2}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} particles exhibited a strong 525-nm and a weak 550-nm emission bandsmore » in the green region and a very weak 655-nm emission band in the red region. The Raman spectrum of undoped CaGd{sub 2}(WO{sub 4}){sub 4} revealed about 12 narrow lines. The strongest band observed at 903 cm{sup −1} was assigned to the ν{sub 1} symmetric stretching vibration of WO{sub 4} tetrahedrons. The spectra of the samples doped with Er and Yb obtained under the 514.5 nm excitation were dominated by Er{sup 3+} luminescence preventing the recording of these samples Raman spectra. Concentration quenching of the erbium luminescence at {sup 2}H{sub 11/2}→{sup 4}I{sub 15/2} transition is weak in the range of erbium doping level x{sub Er}=0.05–0.2, while, for transition {sup 4}S{sub 3/2}→{sup 4}I{sub 15/2}, the signs of concentration quenching become pronounced at x{sub Er}=0.2. - Graphical abstract: CaGd{sub 2−x}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} phosphors with the doping concentrations of Er{sup 3+} and Yb{sup 3+} (x=Er{sup 3+}+Yb{sup 3+}, Er{sup 3+}=0.05, 0.1, 0.2 and Yb{sup 3+}=0.2, 0.45) have been successfully synthesized by the microwave sol–gel method and the crystal structure refinement, and upconversion photoluminescence properties have been investigated. - Highlights: • CaGd{sub 2−x}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} phosphors have been synthesized by the microwave sol–gel method. • The crystal structure of CaGd{sub 2−x}(WO{sub 4}){sub 4}:Er{sup 3+}/Yb{sup 3+} tungstates have been refined. • The upconversion photoluminescence properties have been investigated.« less

Spectral management and morphology evolution of β-NaGdF4:Yb3+,Er3+ by tuning the concentration of citric acid

NASA Astrophysics Data System (ADS)

Yao, Lu; Xu, Dekang; Lin, Hao; Yang, Shenghong; Zhang, Yueli

2018-05-01

β-NaGdF4:Yb3+,Er3+ upconversion (UC) particles were prepared by a facile hydrothermal process with assistance of citric acid (CA). The morphologies of β-NaGdF4 UC particles were controlled by changing the doses of CA in precursor. With an increase CA concentration in precursor, increase sizes of crystals were observed, resulting in the increasing of luminescence intensity. The energy transfer ET mechanism was analyzed in detail.

Near-field refrigeration and tunable heat exchange through four-wave mixing

NASA Astrophysics Data System (ADS)

Khandekar, Chinmay; Messina, Riccardo; Rodriguez, Alejandro W.

2018-05-01

We modify and extend a recently proposed four-wave mixing scheme [C. Khandekar and A. Rodriguez, Opt. Express 25(19), 23164 (2017)] for achieving near-field thermal upconversion and energy transfer, to demonstrate efficient thermal refrigeration at low intensities ˜ 109W/m2 over a wide range of gap sizes (from tens to hundreds of nanometers) and operational temperatures (from tens to hundreds of Kelvins). We further exploit the scheme to achieve magnitude and directional tunability of near-field heat exchange between bodies held at different temperatures.

Limitations on the upconversion of ion sound to Langmuir turbulence

NASA Technical Reports Server (NTRS)

Vlahos, L.; Papadopoulos, K.

1982-01-01

The weak turbulence theory of Tsytovich, Stenflo and Wilhelmsson (1981) for evaluation of the nonlinear transfer of ion acoustic waves to Langmuir waves is shown to be limited in its region of validity to the level of ion acoustic waves. It is also demonstrated that, in applying the upconversion of ion sound to Langmuir waves for electron acceleration, nonlinear scattering should be self-consistently included, with a suppression of the upconversion process resulting. The impossibility of accelerating electrons by such a process for any reasonable physical system is thereby reaffirmed.

Increasing conversion efficiency of two-step photon up-conversion solar cell with a voltage booster hetero-interface.

PubMed

Asahi, Shigeo; Kusaki, Kazuki; Harada, Yukihiro; Kita, Takashi

2018-01-17

Development of high-efficiency solar cells is one of the attractive challenges in renewable energy technologies. Photon up-conversion can reduce the transmission loss and is one of the promising concepts which improve conversion efficiency. Here we present an analysis of the conversion efficiency, which can be increased by up-conversion in a single-junction solar cell with a hetero-interface that boosts the output voltage. We confirm that an increase in the quasi-Fermi gap and substantial photocurrent generation result in a high conversion efficiency.

Ultralow noise up-conversion detector and spectrometer for the telecom band.

PubMed

Shentu, Guo-Liang; Pelc, Jason S; Wang, Xiao-Dong; Sun, Qi-Chao; Zheng, Ming-Yang; Fejer, M M; Zhang, Qiang; Pan, Jian-Wei

2013-06-17

We demonstrate up-conversion single-photon detection for the 1550-nm telecommunications band using a PPLN waveguide, long-wavelength pump, and narrowband filtering using a volume Bragg grating. We achieve total-system detection efficiency of around 30% with noise at the dark-count level of a Silicon APD. Based on the new detector, a single-pixel up-conversion infrared spectrometer with a noise equivalent power of -142 dBm Hz(-1/2) was demonstrated, which was as good as a liquid nitrogen cooled CCD camera.

Research progress of infrared detecting and display integrated device based on infrared-visible up-conversion technology

NASA Astrophysics Data System (ADS)

Xu, Junfeng; Li, Weile; He, Bo; Wang, Haowei; Song, Yong; Yang, Shengyi; Ni, Guoqiang

2018-01-01

Infrared detecting and display device (IR-DDD) is a newly developed optical up-conversion device that integrates the light-emitting diode (LED) onto the infrared (IR) photo-detector, in order to convert IR light into the carriers photo-generated in detection materials and inject them into LED to emit visible light. This IR-DDD can achieve the direct up-conversion from IR ray to visible light, showing the considerable potential in night-vision application. This paper attempts a review of its working principle and current research progresses.

Er-doped lead borate glasses and transparent glass ceramics for near-infrared luminescence and up-conversion applications.

PubMed

Pisarski, Wojciech A; Goryczka, Tomasz; Pisarska, Joanna; Ryba-Romanowski, Witold

2007-03-15

Lead borate based glasses have been analyzed using Raman and infrared spectroscopy. The formation of different borate groups and the direction of BO3 <--> BO4 conversion strongly depends on the PbO- and/or PbF2-to-B2O3 ratio in chemical composition. PbF2-PbO-B2O3 based glasses containing Er3+ ions have been studied after annealing. The orthorhombic PbF2 crystallites are formed during thermal treatment, which was evidenced by X-ray diffraction analysis. Near-infrared luminescence at 1530 nm and green up-conversion at 545 nm have been registered for samples before and after annealing. The luminescence bands correspond to 4I13/2-4I15/2 and 4S3/2-4I15/2 transitions of Er3+ ions, respectively. In comparison to the precursor glasses, the luminescence intensities are higher in the studied transparent oxyfluoride glass ceramics. Simultaneously, the half-width of the luminescence lines slightly decreases. It can be the evidence that a small amount of the Er3+ ions is incorporated into the orthorhombic PbF2 phase.

Sensing Using Rare-Earth-Doped Upconversion Nanoparticles

PubMed Central

Hao, Shuwei; Chen, Guanying; Yang, Chunhui

2013-01-01

Optical sensing plays an important role in theranostics due to its capability to detect hint biochemical entities or molecular targets as well as to precisely monitor specific fundamental psychological processes. Rare-earth (RE) doped upconversion nanoparticles (UCNPs) are promising for these endeavors due to their unique frequency converting capability; they emit efficient and sharp visible or ultraviolet (UV) luminescence via use of ladder-like energy levels of RE ions when excited at near infrared (NIR) light that are silent to tissues. These features allow not only a high penetration depth in biological tissues but also a high detection sensitivity. Indeed, the energy transfer between UCNPs and biomolecular or chemical indicators provide opportunities for high-sensitive bio- and chemical-sensing. A temperature-sensitive change of the intensity ratio between two close UC bands promises them for use in temperature mapping of a single living cell. In this work, we review recent investigations on using UCNPs for the detection of biomolecules (avidin, ATP, etc.), ions (cyanide, mecury, etc.), small gas molecules (oxygen, carbon dioxide, ammonia, etc.), as well as for in vitro temperature sensing. We also briefly summarize chemical methods in synthesizing UCNPs of high efficiency that are important for the detection limit. PMID:23650480

Spiny Nanorod and Upconversion Nanoparticle Satellite Assemblies for Ultrasensitive Detection of Messenger RNA in Living Cells.

PubMed

Gao, Rui; Hao, Changlong; Xu, Liguang; Xu, Chuanlai; Kuang, Hua

2018-04-17

Quantitation and in situ monitoring of target mRNA (mRNA) in living cells remains a significant challenge for the chemical and biomedical communities. To quantitatively detect mRNA expression levels in living cells, we have developed DNA-driven gold nanorod coated platinum-upconversion nanoparticle satellite assemblies (termed Au NR@Pt-UCNP satellites) for intracellular thymidine kinase 1 (TK1) mRNA analysis. The nanostructures were capable of recognizing target mRNA in a sequence-specific manner as luminescence of UCNPs was effectively quenched by Au NR@Pt within the assemblies. Following recognition, UCNPs detached from Au NR@Pt, resulting in luminescence restoration to achieve effective in situ imaging and quantifiable detection of target mRNA. The upconversional luminescence intensity of confocal images showed a good linear relationship with intracellular TK1 mRNA ranging from 1.17 to 65.21 fmol/10 μg RNA and a limit of detection (LOD) of 0.67 fmol/10 μg RNA. We believe that our present assay can be broadly applied for detection of endogenous biomolecules at the cellular and tissue levels and restoration of tissue homeostasis in vivo.

Temperature sensing of adipose tissue heating with the luminescent upconversion nanoparticles as nanothermometer: in vitro study

NASA Astrophysics Data System (ADS)

Yanina, I. Yu.; Volkova, E. K.; Zaharevich, A. M.; Konyukhova, J. G.; Kochubey, V. I.; Tuchin, V. V.

2017-03-01

The luminescence spectra of upconversion nanoparticles (UCNPs) imbedded in fat tissue were measured in a wide temperature range, from room to human body and further to hyperthermic temperatures. The two types of synthesized UCNP [NaYF4:Yb3+, Er3+] specimens, namely, powdered as-is and embedded into polymer film, were used. The results show that the luminescence of UCNPs placed under the adipose tissue layer is reasonably good sensitive to temperature change and reflects phase transitions of lipids in tissue cells. The most likely, multiple phase transitions are associated with the different components of fat cells such as phospholipids of cell membrane and lipids of fat droplets. In the course of fat cell heating, lipids of fat droplet first transit from a crystalline form to a liquid crystal form and then to a liquid form, which is characterized by much less scattering. The phase transitions of lipids were observed as the changes of the slope of the temperature dependence of UCNP luminescence intensity. The obtained results confirm a high sensitivity of the luminescent UCNPs to the temperature variations within tissues and show a strong potential for providing a controllable tissue thermolysis.

Quantum sized Ag nanocluster assisted fluorescence enhancement in Tm{sup 3+}-Yb{sup 3+} doped optical fiber beyond plasmonics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chattopadhyay, Rik; Haldar, Arindam; Paul, Mukul C.

2015-12-07

We report a process for enhancing fluorescence emission from conventional rare earth ions in optical fiber by metal nanocluster (MNC) in nonresonant indirect pumping. The process is completely different from formal metal enhanced fluorescence phenomenon as the MNCs are too small in size to support localized surface plasmon and the excitation wavelength is far from plasmon resonance frequency. We used an established theory of two coupled oscillators to explain the simultaneous enhancement of Ytterbium (Yb{sup 3+}) and Thulium (Tm{sup 3+}) emission by silver (Ag) NCs under nonresonant pumping in optical fiber. The fiber is pumped with a 980 nm fiber pigtailedmore » laser diode with input power of 20–100 mW to excite the Yb{sup 3+}. Four times enhancement of Yb{sup 3+} emission of 900–1100 nm and Tm{sup 3+} upconversion emission around 474 nm, 650 nm, and 790 nm is observed in the fiber with Ag NCs.« less

2.7 μm emission properties of Er3+ doped tungsten-tellurite glass sensitized by Yb3+ ions.

PubMed

Guo, Yanyan; Ma, Yaoyao; Huang, Feifei; Peng, Yapei; Zhang, Liyan; Zhang, Junjie

2013-07-01

With a 980 nm laser diode (LD) pumped, the sensitized effect of Yb(3+) ions on 2.7 μm emission properties and energy transfer mechanism in Yb(3+)/Er(3+) co-doped tungsten-tellurite glass were investigated in present paper. Based on absorption spectra, Judd-Ofelt parameters and radiative transition probabilities were calculated and analyzed. The emission spectra were tested and the optimized concentration ratio of Yb(3+) to Er(3+) ions was found to be 3:0.5 with a largest calculated emission cross-section (6.05×10(-21) cm(2)) corresponding to Er(3+):(4)I11/2→(4)I13/2 transition. When the concentration ratio of Yb(3+) to Er(3+) ions was 4:0.5, 1.5 μm and 2.7 μm emission decreased while up-conversion increased. The decreased 1.5 μm and 2.7 μm emission were induced by the saturation of Er(3+):(4)I13/2 level. In brief, the advantageous spectroscopic characteristics indicated that Yb(3+)/Er(3+) co-doped tungsten-tellurite glass may be a promising candidate for application of 2.7 μm emission. Copyright © 2013 Elsevier B.V. All rights reserved.

High-efficiency electroluminescence and amplified spontaneous emission from a thermally activated delayed fluorescent near-infrared emitter

NASA Astrophysics Data System (ADS)

Kim, Dae-Hyeon; D'Aléo, Anthony; Chen, Xian-Kai; Sandanayaka, Atula D. S.; Yao, Dandan; Zhao, Li; Komino, Takeshi; Zaborova, Elena; Canard, Gabriel; Tsuchiya, Youichi; Choi, Eunyoung; Wu, Jeong Weon; Fages, Frédéric; Brédas, Jean-Luc; Ribierre, Jean-Charles; Adachi, Chihaya

2018-02-01

Near-infrared organic light-emitting diodes and semiconductor lasers could benefit a variety of applications including night-vision displays, sensors and information-secured displays. Organic dyes can generate electroluminescence efficiently at visible wavelengths, but organic light-emitting diodes are still underperforming in the near-infrared region. Here, we report thermally activated delayed fluorescent organic light-emitting diodes that operate at near-infrared wavelengths with a maximum external quantum efficiency of nearly 10% using a boron difluoride curcuminoid derivative. As well as an effective upconversion from triplet to singlet excited states due to the non-adiabatic coupling effect, this donor-acceptor-donor compound also exhibits efficient amplified spontaneous emission. By controlling the polarity of the active medium, the maximum emission wavelength of the electroluminescence spectrum can be tuned from 700 to 780 nm. This study represents an important advance in near-infrared organic light-emitting diodes and the design of alternative molecular architectures for photonic applications based on thermally activated delayed fluorescence.

Determining the average path length of amplified spontaneous emission in a four-level laser near the 1/3 mode-degeneracy cavity configurations

NASA Astrophysics Data System (ADS)

Chen, Ching-Hsu; Lu, Ming-Lun; Tai, Po-Tse

2015-08-01

We determine the average path length ls of amplified spontaneous emission (ASE) by comparing the numerical slope of a straight line with the experimental slope in the graph of the square of relaxation oscillation frequency versus normalized pump ratio. The simple method is applied in an end-pumped Nd:YVO4 laser with the 1/3 mode-degeneracy cavity having the transverse mode spacing equal to 1/3 of the longitudinal mode spacing. We find that ls is larger at the degeneracy than that far from the degeneracy. This result indicates the existence of stronger ASE at the degeneracy, which is confirmed below the threshold. This is because many spontaneous emission photons can undergo amplification not only before escaping from the gain medium but also after leaving the gain medium, owing to cavity reflection. Our method can be applied in the situations where the Auger upconversion effect is absent, weak, or well-known.

Structure and up-conversion luminescence in sol-gel derived Er 3+-Yb 3+ co-doped SiO 2:PbF 2 nano-glass-ceramics

NASA Astrophysics Data System (ADS)

del-Castillo, J.; Yanes, A. C.; Méndez-Ramos, J.; Tikhomirov, V. K.; Rodríguez, V. D.

2009-11-01

Transparent oxyfluoride nano-glass-ceramics 90(SiO 2)10(PbF 2) co-doped with 0.3 Yb 3+ and 0.1 Er 3+ (mol%) have been prepared by thermal treatment of precursor sol-gel glasses. X-ray diffraction and high resolution transmission electron microscopy analysis pointed out a precipitation of cubic β-PbF 2 nanocrystals of certain diameter in nano-glass-ceramics varying from 10 to 20 nm depending on heat treatment conditions. The incorporation of Yb 3+ and Er 3+ dopants in these nanocrystals has been confirmed by signatures of luminescence spectroscopy. Up-conversion luminescence pumped at 980 nm has been detected. Colour tuneability of up-conversion luminescence varying pump power has been analyzed in terms of standard chromaticity diagram. This tuneability opens applications for up-conversion phosphors and three-dimensional optical recording.

Realizing up-conversion fluorescence tuning in lanthanide-doped nanocrystals by femtosecond pulse shaping method

PubMed Central

Zhang, Shian; Yao, Yunhua; Shuwu, Xu; Liu, Pei; Ding, Jingxin; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong

2015-01-01

The ability to tune color output of nanomaterials is very important for their applications in laser, optoelectronic device, color display and multiplexed biolabeling. Here we first propose a femtosecond pulse shaping technique to realize the up-conversion fluorescence tuning in lanthanide-doped nanocrystals dispersed in the glass. The multiple subpulse formation by a square phase modulation can create different excitation pathways for various up-conversion fluorescence generations. By properly controlling these excitation pathways, the multicolor up-conversion fluorescence can be finely tuned. This color tuning by the femtosecond pulse shaping technique is realized in single material by single-color laser field, which is highly desirable for further applications of the lanthanide-doped nanocrystals. This femtosecond pulse shaping technique opens an opportunity to tune the color output in the lanthanide-doped nanocrystals, which may bring a new revolution in the control of luminescence properties of nanomaterials. PMID:26290391

Single-band upconversion nanoprobes for multiplexed simultaneous in situ molecular mapping of cancer biomarkers.

PubMed

Zhou, Lei; Wang, Rui; Yao, Chi; Li, Xiaomin; Wang, Chengli; Zhang, Xiaoyan; Xu, Congjian; Zeng, Aijun; Zhao, Dongyuan; Zhang, Fan

2015-04-24

The identification of potential diagnostic markers and target molecules among the plethora of tumour oncoproteins for cancer diagnosis requires facile technology that is capable of quantitatively analysing multiple biomarkers in tumour cells and tissues. Diagnostic and prognostic classifications of human tumours are currently based on the western blotting and single-colour immunohistochemical methods that are not suitable for multiplexed detection. Herein, we report a general and novel method to prepare single-band upconversion nanoparticles with different colours. The expression levels of three biomarkers in breast cancer cells were determined using single-band upconversion nanoparticles, western blotting and immunohistochemical technologies with excellent correlation. Significantly, the application of antibody-conjugated single-band upconversion nanoparticle molecular profiling technology can achieve the multiplexed simultaneous in situ biodetection of biomarkers in breast cancer cells and tissue specimens and produce more accurate results for the simultaneous quantification of proteins present at low levels compared with classical immunohistochemical technology.

Triplet-triplet annihilation photon-upconversion: towards solar energy applications.

PubMed

Gray, Victor; Dzebo, Damir; Abrahamsson, Maria; Albinsson, Bo; Moth-Poulsen, Kasper

2014-06-14

Solar power production and solar energy storage are important research areas for development of technologies that can facilitate a transition to a future society independent of fossil fuel based energy sources. Devices for direct conversion of solar photons suffer from poor efficiencies due to spectrum losses, which are caused by energy mismatch between the optical absorption of the devices and the broadband irradiation provided by the sun. In this context, photon-upconversion technologies are becoming increasingly interesting since they might offer an efficient way of converting low energy solar energy photons into higher energy photons, ideal for solar power production and solar energy storage. This perspective discusses recent progress in triplet-triplet annihilation (TTA) photon-upconversion systems and devices for solar energy applications. Furthermore, challenges with evaluation of the efficiency of TTA-photon-upconversion systems are discussed and a general approach for evaluation and comparison of existing systems is suggested.

Analysis on energy transfer process of Ho3+ doped fluoroaluminate glass sensitized by Yb3+ for mid-infrared 2.85 μm emission

NASA Astrophysics Data System (ADS)

Zhou, Beier; Wei, Tao; Cai, Muzhi; Tian, Ying; Zhou, Jiajia; Deng, Degang; Xu, Shiqing; Zhang, Junjie

2014-12-01

This work reports the mid-infrared emission properties around 2.85 μm in a Yb3+/Ho3+ codoped fluoroaluminate glass. This fluoroaluminate glass shows a good thermal stability and high transmittance around 3 μm. The mid-infrared emission characteristics and energy transfer mechanism upon the excitation of the conventional 980 nm laser diode have been investigated. The prepared glass possesses higher spontaneous transition probability (31.77 s-1) along with the larger calculated emission cross section (1.91×10-20 cm2) corresponding to the laser transition of Ho3+:5I6→5I7. Besides, the upconversion, 1.2 μm and 2 μm fluorescence spectra were measured to understand mid-infrared emission behavior together with decay curves of Ho3+:5I6 level. Moreover, energy transfer microparameters between Yb3+ and Ho3+ were calculated and discussed based on Dexter's model. Hence, the advantageous spectroscopic characteristics of Yb3+/Ho3+ codoped fluoroaluminate glass as well as the good thermal property indicate that this kind of glass is an attractive host for developing mid-infrared solid state laser.

Broadband sensitized photon up-conversion at subsolar irradiance (Conference Presentation)

NASA Astrophysics Data System (ADS)

Pedrini, Jacopo; Monguzzi, Angelo; Meinardi, Francesco

2016-09-01

A crucial limit of solar devices is their inability to harvest the full solar spectrum. Currently, sensitized up-conversion based on triplet-tripled annihilation (STTA-UC) in bi-component organic systems is the most promising technique to recover sub-bandgap photons, showing good efficiencies also at excitation intensities comparable to the solar irradiance. In STTA-UC, high-energy light is generated through annihilation of metastable triplet states of molecules acting as emitters, which are populated via resonant energy transfer from a light-harvesting sensitizer. However, suitable sensitizers show narrow absorption bands, limiting the fraction of recoverable photons, therefore preventing the application of STTA-UC to real-world devices. Here we demonstrate how to overcome the described limit by using multiple sensitizers that work cooperatively to broaden the overall system absorption band. This is obtained using an additional sensitizer that transfers the extra harvested energy to the main one (sensitization of the sensitizer), or a set of properly designed complementary absorbing sensitizers all able to excite simultaneously the same emitter (multi-sensitizers). In both cases STTA-UC performances result strongly enhanced compared to the corresponding mono-sensitizer system, increasing the up-converted light intensity generated at AM 1.5 up to two times. Remarkably, by coupling our light converters to a DSSC we prove its operation by exploiting exclusively sub-bandgap photons. A detailed modeling of the photophysical processes involved in these complex systems allows us to draw the guidelines for the design of the next generation STTA-UC materials, encouraging their application to photovoltaic technologies.

High quality polyacrylic acid modified multifunction luminescent nanorods for tri-modality bioimaging, in vivo long-lasting tracking and biodistribution

NASA Astrophysics Data System (ADS)

Yi, Zhigao; Lu, Wei; Liu, Hongrong; Zeng, Songjun

2014-12-01

Polyacrylic acid (PAA) modified NaYF4:Gd/Yb/Er upconversion nanorods (denoted as PAA-UCNRs) are demonstrated for tri-modal upconversion (UC) optical, computed X-ray tomography (CT), and magnetic resonance imaging (MRI). The hydrophilic PAA-UCNRs were obtained from hydrophobic oleic acid (OA) capped UCNRs (denoted as OA-UCNRs) using a ligand exchange method. The as-prepared UCNRs with a hexagonal phase structure present high monodispersity. These PAA-UCNRs are successfully used as ideal probes for in vivo UC luminescence bioimaging and synergistic X-ray and UC bioimaging. Moreover, X-ray CT imaging reveals that PAA-UCNRs can act as contrast agents for improved detection of the liver and spleen. In addition, a significant signal enhancement in the liver is observed in in vivo MRI, indicating that PAA-UCNRs are ideal T1-weighted MRI agents. More importantly, in vivo long-term tracking based on these PAA-UCNRs in the live mice and the corresponding ex vivo bioimaging of isolated organs also verify the translocation of PAA-UCNRs from the liver to the spleen, and the observed intense UC signals from the feces reveal the biliary excretion mechanism of these UCNRs. These findings contribute to understanding of the translocation and potential route for excretion of PAA-UCNRs, which can provide an important guide for the diagnosis and detection of diseases based on these UCNRs.Polyacrylic acid (PAA) modified NaYF4:Gd/Yb/Er upconversion nanorods (denoted as PAA-UCNRs) are demonstrated for tri-modal upconversion (UC) optical, computed X-ray tomography (CT), and magnetic resonance imaging (MRI). The hydrophilic PAA-UCNRs were obtained from hydrophobic oleic acid (OA) capped UCNRs (denoted as OA-UCNRs) using a ligand exchange method. The as-prepared UCNRs with a hexagonal phase structure present high monodispersity. These PAA-UCNRs are successfully used as ideal probes for in vivo UC luminescence bioimaging and synergistic X-ray and UC bioimaging. Moreover, X-ray CT imaging reveals that PAA-UCNRs can act as contrast agents for improved detection of the liver and spleen. In addition, a significant signal enhancement in the liver is observed in in vivo MRI, indicating that PAA-UCNRs are ideal T1-weighted MRI agents. More importantly, in vivo long-term tracking based on these PAA-UCNRs in the live mice and the corresponding ex vivo bioimaging of isolated organs also verify the translocation of PAA-UCNRs from the liver to the spleen, and the observed intense UC signals from the feces reveal the biliary excretion mechanism of these UCNRs. These findings contribute to understanding of the translocation and potential route for excretion of PAA-UCNRs, which can provide an important guide for the diagnosis and detection of diseases based on these UCNRs. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr05161k

Upconversion-based receivers for quantum hacking-resistant quantum key distribution

NASA Astrophysics Data System (ADS)

Jain, Nitin; Kanter, Gregory S.

2016-07-01

We propose a novel upconversion (sum frequency generation)-based quantum-optical system design that can be employed as a receiver (Bob) in practical quantum key distribution systems. The pump governing the upconversion process is produced and utilized inside the physical receiver, making its access or control unrealistic for an external adversary (Eve). This pump facilitates several properties which permit Bob to define and control the modes that can participate in the quantum measurement. Furthermore, by manipulating and monitoring the characteristics of the pump pulses, Bob can detect a wide range of quantum hacking attacks launched by Eve.

The effect of micro-structure on upconversion luminescence of Nd3+/Yb3+ co-doped La2O3-TiO2-ZrO2 glass-ceramics

NASA Astrophysics Data System (ADS)

Zhang, Minghui; Wen, Haiqin; Pan, Xiuhong; Yu, Jianding; Jiang, Meng; Yu, Huimei; Tang, Meibo; Gai, Lijun; Ai, Fei

2018-03-01

Nd3+/Yb3+ co-doped La2O3-TiO2-ZrO2 glasses have been prepared by aerodynamic levitation method. The glasses show high refractive index of 2.28 and Abbe number of 18.3. Glass-ceramics heated at 880 °C for 50 min perform the strongest upconversion luminescence. X-ray diffraction patterns of glass-ceramics with different depths indicate that rare earth ions restrain crystallization. Body crystallization mechanism mixed with surface crystallization is confirmed in the heat treatment. Surface crystals achieve priority to grow, resulting in important effects on upconversion luminescence. The results of atomic force microscope and scanning electron microscope indicate that crystal particles with uniform size distribute densely and homogenously on the surface and large amount of glass matrix exists in the glass ceramics heated at 880 °C for 50 min. Crystals in the glass-ceramics present dense structure and strong boundaries, which can reduce the mutual nonradiative relaxation rate among rare earth ions and then improve upconversion luminescence effectively. Based on micro-structural study, the mechanism that upconversion luminescence can be improved by heat treatment has been revealed. The results of micro-structural analysis agree well with the spectra.

Perspectives and challenges of photon-upconversion nanoparticles - Part I: routes to brighter particles and quantitative spectroscopic studies.

PubMed

Resch-Genger, Ute; Gorris, Hans H

2017-10-01

Lanthanide-doped photon-upconversion nanoparticles (UCNPs) have been the focus of many research activities in materials and life sciences in the last 15 years because of their potential to convert light between different spectral regions and their unique photophysical properties. To fully exploit the application potential of these fascinating nanomaterials, a number of challenges have to be overcome, such as the low brightness, particularly of small UCNPs, and the reliable quantification of the excitation-power-density-dependent upconversion luminescence. In this series of critical reviews, recent developments in the design, synthesis, optical-spectroscopic characterization, and application of UCNPs are presented with special focus on bioanalysis and the life sciences. Here we guide the reader from the synthesis of UCNPs to different concepts to enhance their luminescence, including the required optical-spectroscopic assessment to quantify material performance; surface modification strategies and bioanalytical applications as well as selected examples of the use of UCNPs as reporters in different assay formats are addressed in part II. Future trends and challenges in the field of upconversion are discussed with special emphasis on UCNP synthesis and material characterization, particularly quantitative luminescence studies. Graphical Abstract Both synthesis and spectroscopy as well bioanalytical applications of UCNPs are driven and supported by COST Action CM1403 "The European Upconversion Network".

Structural and light up-conversion luminescence properties of Er3+-Yb3+-W6+ substituted Bi4Ti3O12

NASA Astrophysics Data System (ADS)

Bokolia, Renuka; Rai, Vineet K.; Chauhan, Lalita; Sreenivas, K.

2016-05-01

The structural and light up-conversion (UC) luminescence properties of W6+ substituted Bi3.79Er0.03Yb0.18Ti3-xWxO12 (0 ≤ x ≤ 0.10) ceramics prepared by solid state reaction method have been investigated. X-ray diffraction (XRD) confirms the formation of single phase material with orthorhombic structure. A decrease in the lattice parameters and unit cell volume is observed with increasing W content. Strong UC luminescence at 527, 548 and 662 nm is seen under an excitation of 980 nm for an optimum W content (x = 0.06) and is attributed to the transitions 2H11/2 →4I15/2, 4S3/2 →4I15/2 and 4F9/2 →4I15/2 respectively. The improved UC luminescence is ascribed to the reduced defects such as oxygen vacancies and change in the crystal field around Er3+ ions due to B-site (Ti4+) substitution with W6+ ions. Enhanced UC emission is observed for an optimum content of w6+ in the prepared composition Bi3.79Er0.03Yb0.18Ti3-xWxO12 for x = 0.06.

Synthesis and characterization of α-NaYF{sub 4}: Yb, Er nanoparticles by reverse microemulsion method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gunaseelan, M.; Senthilselvan, J., E-mail: jsselvan@hotmail.com

2016-05-06

A simple and cost effective reverse microemulsion system was newly designed to synthesis NaYF{sub 4}:20%Yb,2%Er upconverting luminescent nanoparticles. XRD results confirms the cubic structure of NaYF{sub 4} nanophosphor in the as prepared condition without any other impurity phases. The as-prepared sample itself having highly crystalline nanoparticle with well dispersed uniform morphology is the advantage of this reverse microemulsion process. HRTEM images of as prepared and calcined samples revealed spherical nanoclusters morphology with size of ~210 nm and ~245 nm respectively. The characteristic absorption wavelength that occurs at 980 nm due to transition of energy levels {sup 2}F{sub 5/2} to {sup 2}F{sub 7/2} formore » Yb{sup 3+} rare earth ion in as prepared and calcined upconversion nanoparticle confirms the presence of Yb{sup 3+} by UV-Visible spectroscopy which can act as a sensitizer for photonic upconversion. Therefore the absorption at NIR region and emission spectrum at visible region suggests that NaYF{sub 4}:20%Yb,2%Er is suitable for upcoversion process, due to its optical property and chemical stability this material also be useful for bio imaging applications.« less

Instantaneous ballistic velocity of suspended Brownian nanocrystals measured by upconversion nanothermometry

NASA Astrophysics Data System (ADS)

Brites, Carlos D. S.; Xie, Xiaoji; Debasu, Mengistie L.; Qin, Xian; Chen, Runfeng; Huang, Wei; Rocha, João; Liu, Xiaogang; Carlos, Luís D.

2016-10-01

Brownian motion is one of the most fascinating phenomena in nature. Its conceptual implications have a profound impact in almost every field of science and even economics, from dissipative processes in thermodynamic systems, gene therapy in biomedical research, artificial motors and galaxy formation to the behaviour of stock prices. However, despite extensive experimental investigations, the basic microscopic knowledge of prototypical systems such as colloidal particles in a fluid is still far from being complete. This is particularly the case for the measurement of the particles' instantaneous velocities, elusive due to the rapid random movements on extremely short timescales. Here, we report the measurement of the instantaneous ballistic velocity of Brownian nanocrystals suspended in both aqueous and organic solvents. To achieve this, we develop a technique based on upconversion nanothermometry. We find that the population of excited electronic states in NaYF4:Yb/Er nanocrystals at thermal equilibrium can be used for temperature mapping of the nanofluid with great thermal sensitivity (1.15% K-1 at 296 K) and a high spatial resolution (<1 μm). A distinct correlation between the heat flux in the nanofluid and the temporal evolution of Er3+ emission allows us to measure the instantaneous velocity of nanocrystals with different sizes and shapes.

Recent Advances in Upconversion Nanoparticles-Based Multifunctional Nanocomposites for Combined Cancer Therapy.

PubMed

Tian, Gan; Zhang, Xiao; Gu, Zhanjun; Zhao, Yuliang

2015-12-16

Lanthanide-doped upconversion nanoparticles (UCNPs) have the ability to generate ultraviolet or visible emissions under continuous-wave near-infrared (NIR) excitation. Utilizing this special luminescence property, UCNPs are approved as a new generation of contrast agents in optical imaging with deep tissue-penetration ability and high signal-to-noise ratio. The integration of UCNPs with other functional moieties can endow them with highly enriched functionalities for imaging-guided cancer therapy, which makes composites based on UCNPs emerge as a new class of theranostic agents in biomedicine. Here, recent progress in combined cancer therapy using functional nanocomposites based on UCNPs is reviewed. Combined therapy referring to the co-delivery of two or more therapeutic agents or a combination of different treatments is becoming more popular in clinical treatment of cancer because it generates synergistic anti-cancer effects, reduces individual drug-related toxicity and suppresses multi-drug resistance through different mechanisms of action. Here, the recent advances of combined therapy contributed by UCNPs-based nanocomposites on two main branches are reviewed: i) photodynamic therapy and ii) chemotherapy, which are the two most widely adopted therapies of UCNPs-based composites. The future prospects and challenges in this emerging field will be also discussed. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} core/shell nanocomposite: A highly efficient visible-light-driven photocatalyst utilizing upconversion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sun, Yuanyuan; Wang, Wenzhong, E-mail: wzwang@mail.sic.ac.cn; Sun, Songmei

2014-04-01

Highlights: • Design and synthesis of NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} based on upconversion. • NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} nanocomposite was prepared for the first time. • Core–shell structure benefits the properties. • Upconversion contributed to the enhanced photocatalytic activity. • Helps to understand the functionality of new type photocatalysts. - Abstract: NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} core/shell nanocomposite was designed and prepared for the first time based on upconversion. The products were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution TEM (HRTEM), energy dispersive X-ray spectroscopy (EDS) and diffuse reflectance spectra (DRS). The results revealed that the as-synthesizedmore » NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} consisted of spheres with a core diameter of about 26 nm and a shell diameter of around 6 nm. The core was upconversion illuminant NaYF{sub 4}:Er,Yb and the shell was Bi{sub 2}MoO{sub 6} around the core, which was confirmed by EDS. The NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} exhibited higher photocatalytic activity for the photodecomposition of Rhodamine B (RhB) under the irradiation of Xe lamp and green light emitting diode (g-LED). The mechanism of the high photocatalytic activity was discussed by photoluminescence spectra (PL), which is mainly attributed to upconversion of NaYF{sub 4}:Er,Yb in the NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} nanocomposite and the core–shell structure.« less

The Er3+-Yb3+ codoped La2O3 phosphor in finger print detection and optical heating.

PubMed

Dey, Riya; Pandey, Anurag; Rai, Vineet Kumar

2014-07-15

The presence of impurities and morphological information about the Er(3+)-Yb(3+) codoped La2O3 phosphors prepared by two different synthesis techniques have been obtained with the help of Fourier transform infrared (FTIR) spectroscopy and Scanning electron microscopy (SEM) respectively. The effect of synthesis process on the frequency upconversion (UC) emission with an excitation at 980 nm from laser diode radiation has been performed. The use of codoped phosphor in latent finger print detection and laser induced heat generation has also been explored. Copyright © 2014 Elsevier B.V. All rights reserved.

NIR-to-visible upconversion nanoparticles for fluorescent labeling and targeted delivery of siRNA

NASA Astrophysics Data System (ADS)

Jiang, Shan; Zhang, Yong; Lim, Kian Meng; Sim, Eugene K. W.; Ye, Lei

2009-04-01

Near-infrared (NIR)-to-visible upconversion fluorescent nanoparticles were synthesized and used for imaging and targeted delivery of small interfering RNA (siRNA) to cancer cells. Silica-coated NaYF4 upconversion nanoparticles (UCNs) co-doped with lanthanide ions (Yb/Er) were synthesized. Folic acid and anti-Her2 antibody conjugated UCNs were used to fluorescently label the folate receptors of HT-29 cells and Her2 receptors of SK-BR-3 cells, respectively. The intracellular uptake of the folic acid and antibody conjugated UCNs was visualized using a confocal fluorescence microscope equipped with an NIR laser. siRNA was attached to anti-Her2 antibody conjugated UCNs and the delivery of these nanoparticles to SK-BR-3 cells was studied. Meanwhile, a luciferase assay was established to confirm the gene silencing effect of siRNA. Upconversion nanoparticles can serve as a fluorescent probe and delivery system for simultaneous imaging and delivery of biological molecules.

Self-assembly of an upconverting nanocomplex and its application to turn-on detection of metalloproteinase-9 in living cells

NASA Astrophysics Data System (ADS)

Nguyen, Phuong-Diem; Thanh Cong, Vu; Baek, Changyoon; Min, Junhong

2016-10-01

Upcoversion nanoparticles are an emerging luminescent nanomaterial with excellent photophysical properties that have great benefits in biological sensing. In this study, a luminescent turn-on biosensor for cell-secreted protease activity assay is established based on resonance energy transfer in an upconversion nanoparticle-graphene oxide nano-assembly. The proposed biosensor consists of a blue-emitting upconversion nanoparticle covered with a quenching complex, comprising gelatin as the proteinase substrate and graphene oxide nanosheets as luminescence acceptors. After enzymatic digestion, the upconversion nanoparticles lose the gelatin cover due to the disassembly of the quenching complex, thus the upconverting luminescence in the blue region is restored (a turn-on response). The recovered upconverting luminescence is proportional to the protease concentration; the limit of detection was 12 ng ml-1. Finally, the upconversion-graphene oxide nanocomplex was successfully applied in the detection of cell-secreted protease-metalloproteinase in MCF-7 cancer cells with high sensitivity and specificity.

Labeling of HeLa cells using ZrO2:Yb3+-Er3+ nanoparticles with upconversion emission

NASA Astrophysics Data System (ADS)

Ceja-Fdez, Andrea; López-Luke, Tzarara; Oliva, Jorge; Vivero-Escoto, Juan; Gonzalez-Yebra, Ana Lilia; Rojas, Ruben A. Rodriguez; Martínez-Pérez, Andrea; de la Rosa, Elder

2015-04-01

This work reports the synthesis, structural characterization, and optical properties of ZrO2:Yb3+-Er3+ (2-1 mol%) nanocrystals. The nanoparticles were coated with 3-aminopropyl triethoxysilane (APTES) and further modified with biomolecules, such as Biotin-Anti-rabbit (mouse IgG) and rabbit antibody-AntiKi-67, through a conjugation method. The conjugation was successfully confirmed by Fourier transform infrared, zeta potential, and dynamic light scattering. The internalization of the conjugated nanoparticles in human cervical cancer (HeLa) cells was followed by two-photon confocal microscopy. The ZrO2:Yb3+-Er3+ nanocrystals exhibited strong red emission under 970-nm excitation. Moreover, the luminescence change due to the addition of APTES molecules and biomolecules on the nanocrystals was also studied. These results demonstrate that ZrO2:Yb3+-Er3+ nanocrystals can be successfully functionalized with biomolecules to develop platforms for biolabeling and bioimaging.

Multiscale optical imaging of rare-earth-doped nanocomposites in a small animal model.

PubMed

Higgins, Laura M; Ganapathy, Vidya; Kantamneni, Harini; Zhao, Xinyu; Sheng, Yang; Tan, Mei-Chee; Roth, Charles M; Riman, Richard E; Moghe, Prabhas V; Pierce, Mark C

2018-03-01

Rare-earth-doped nanocomposites have appealing optical properties for use as biomedical contrast agents, but few systems exist for imaging these materials. We describe the design and characterization of (i) a preclinical system for whole animal in vivo imaging and (ii) an integrated optical coherence tomography/confocal microscopy system for high-resolution imaging of ex vivo tissues. We demonstrate these systems by administering erbium-doped nanocomposites to a murine model of metastatic breast cancer. Short-wave infrared emissions were detected in vivo and in whole organ imaging ex vivo. Visible upconversion emissions and tissue autofluorescence were imaged in biopsy specimens, alongside optical coherence tomography imaging of tissue microstructure. We anticipate that this work will provide guidance for researchers seeking to image these nanomaterials across a wide range of biological models. (2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

Integrated optical modulator for signal up-conversion over radio-on-fiber link.

PubMed

Kim, Woo-Kyung; Kwon, Soon-Woo; Jeong, Woo-Jin; Son, Geun-Sik; Lee, Kwang-Hyun; Choi, Woo-Young; Yang, Woo-Seok; Lee, Hyung-Man; Lee, Han-Young

2009-02-16

An integrated optical modulator, which consists of a dual-sideband suppressed carrier (DSB-SC) modulator cascaded with a single-sideband (SSB) modulator, is proposed for signal up-conversion over Radio-on-Fiber. Utilizing a single-drive domain inverted structure in both modulators, balanced modulations were obtained without complicated radio frequency (RF) driving circuits and delicate RF phase adjustments. Intermediate frequency (IF) band signal was up-conversed to 60GHz band by using the fabricated device and was transmitted over optical fiber. Experiment results show that the proposed device enables millimeter wave generation and signal transmission without any power penalty caused by chromatic dispersion.

1.5- μm single photon counting using polarization-independent up-conversion detector

NASA Astrophysics Data System (ADS)

Takesue, Hiroki; Diamanti, Eleni; Langrock, Carsten; Fejer, M. M.; Yamamoto, Yoshihisa

2006-12-01

We report a 1.5- μm band polarization independent single photon detector based on frequency up-conversion in periodically poled lithium niobate (PPLN) waveguides. To overcome the polarization dependence of the PPLN waveguides, we employed a polarization diversity configuration composed of two up-conversion detectors connected with a polarization beam splitter. We experimentally confirmed polarization independent single photon counting using our detector. We undertook a proof-of-principle differential phase shift quantum key distribution experiment using the detector, and confirmed that the sifted key rate and error rate remained stable when the polarization state was changed during single photon transmission.

[Two-photon up-conversion fluorescence of a neodymium organic framework Nd(BTC)].

PubMed

Xu, Hui; Jin, Run-zhi; Wu, Chun-yang; Yang, Yu; Qian, Guo-dong

2008-08-01

In the present work, a neodymium organic framework Nd(BTC) was synthesized by the solvothermal reaction of Nd(NO3)3 x 5H2O and H3BTC (BTC = 1,3,5-benzenetricarboxylate) in mixed solvents of DMF, ethanol and water, and was identified by elemental analysis. This MOF complex was characterized using X-ray diffraction (XRD), thermogravimetry-differential scanning calorimetry (TGA-DSC) analysis, UV-visible absorption spectra and fluorescence spectra. This polycrystalline powder lost DMF and H2O when heated to 120 degrees C, then remained stable till the temperature reached 500 degrees C. Near infrared fluorescence at 1064 nm due to the 4 F3/2--> 4 I11/2 transition of Nd3+ ions was exhibited when excited by 808 nm laser beam. It was also been found that up-conversion fluorescence of Nd(BTC) peaked at about 450 nm due to 2 D5/2 -->4 I11/2 transition of Nd3+ ions can be observed under the excitation of a 580 nm laser line. The mechanism of the up-conversion fluorescence of Nd(BTC) at around 450 nm under the excitation of 580 nm laser can be ascribed to both excited-state absorption and energy transfer up-conversion. This result indicated that such MOF can be employed as an up-conversion luminescence material in many potential application areas such as bio-labeling and fluorescence image.

Development of infrared sensors using energy transfer/energy upconversion processes: Study of laser excited fluorescence in rare Earth ion doped crystals

NASA Technical Reports Server (NTRS)

Nash-Stevenson, S. K.; Reddy, B. R.; Venkateswarlu, P.

1994-01-01

A summary is presented of the spectroscopic study of three systems: LaF3:Ho(3+), LaF3:Er(3+) and CaF2:Nd(3+). When the D levels of Ho(3+) in LaF3 were resonantly excited with a laser beam of 640 nm, upconverted emissions were detected from J (416 nm), F (485 nm), and E (546 nm) levels. Energy upconverted emissions were also observed from F and E levels of Ho(3+) when the material was excited with an 800 nm near infrared laser. When the D levels of Er(3+) in LaF3 were resonantly excited with a laser beam of 637 nm, upconverted emissions were detected from the E (540 nm) and P (320, 400, and 468 nm) levels. Energy upconverted emissions were also observed from F, E, and D levels of Er(3+) when the material was resonantly excited with an 804 nm near infrared laser. When the D levels of Nd(3+) in CaF2 were resonantly excited with a laser beam of 577 nm, upconverted emissions were detected from the L (360 and 382 nm), K (418 nm), and I (432 nm) levels. Very weak upconverted emissions were detected when this system was irradiated with a near infrared laser. The numbers in parentheses are the wavelengths of the emissions.

Photochemical Upconversion: A Physical or Inorganic Chemistry Experiment for Undergraduates Using a Conventional Fluorimeter

ERIC Educational Resources Information Center

Wilke, Bryn M.; Castellano, Felix N.

2013-01-01

Photochemical upconversion is a regenerative process that transforms lower-energy photons into higher-energy light through two sequential bimolecular reactions, triplet sensitization of an appropriate acceptor followed by singlet fluorescence producing triplet-triplet annihilation derived from two energized acceptors. This laboratory directly…

IR-stimulated visible fluorescence in pink and brown diamond.

PubMed

Byrne, K S; Chapman, J G; Luiten, A N

2014-03-19

Irradiation of natural pink and brown diamond by middle-ultraviolet light (photon energy ϵ ≥ 4.1 eV ) is seen to induce anomalous fluorescence phenomena at N3 defect centres (structure N3-V). When diamonds primed in this fashion are subsequently exposed to infrared light (even with a delay of many hours), a transient burst of blue N3 fluorescence is observed. The dependence of this IR-triggered fluorescence on pump wavelength and intensity suggest that this fluorescence phenomena is intrinsically related to pink diamond photochromism. An energy transfer process between N3 defects and other defect species can account for both the UV-induced fluorescence intensity changes, and the apparent optical upconversion of IR light. From this standpoint, we consider the implications of this N3 fluorescence behaviour for the current understanding of pink diamond photochromism kinetics.

Measurement of laser power for photo-triggered drug delivery in vivo

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, R.; Zhang, X. L.; Liu, F.

Thus far, despite many investigations have been carried out for photo-triggered drug delivery systems, most of them suffer from an intrinsic drawback of without real-time monitoring mechanism. Incident intensity of light is a feasible parameter to monitor the drug release profiles. However, it is difficult to measure the incident laser power irradiated onto the photo-triggered carriers in drug delivery systems during in vivo therapy. We design an online measurement method based on the fluorescence intensity ratio (FIR) technique through upconversion nanoparticles. FIR value varies with temperature of sample due to the thermal effect induced by the incident laser, which validatesmore » the laser power measurement. Effects of rare earth doping concentration, as well as experimental conditions including laser spots and wavelengths on the measurement behavior were also investigated.« less

Comparison of temperature sensing of the luminescent upconversion and ZnCdS nanoparticles

NASA Astrophysics Data System (ADS)

Yanina, I. Yu.; Volkova, E. K.; Sagaidachnaya, E. A.; Konyukhova, J. G.; Kochubey, V. I.; Tuchin, V. V.

2018-02-01

The luminescence spectra of upconversion nanoparticles (UCNPs) and ZnCdS nanoparticles (ZnCdSNPs) were measured and analyzed in a wide temperature range: from room to human body and further to a hyperthermic temperature resulting in tissue morphology change. The results show that the luminescence signal of UCNPs and ZnCdSNPs placed within the tissue is reasonably good sensitive to temperature change and accompanied by phase transitions of lipid structures of adipose tissue. The most likely that the multiple phase transitions are associated with the different components of fat cells, such as phospholipids of cell membrane and lipids of fat droplets. In the course of fat cell heating, lipids of fat droplet first transit from a crystalline form to a liquid crystal form and then to a liquid form, which is characterized by much less scattering. The results of phase transitions of lipids were observed as the changes in the slope of the temperature dependence of the intensity of luminescence of the film with nanoparticles embedded into tissue. The obtained results confirm a high sensitivity of the luminescent UCNPs and ZnCdSNPs to the temperature variations within thin tissue samples and show a strong potential for the controllable tissue thermolysis.

Smartphone based visual and quantitative assays on upconversional paper sensor.

PubMed

Mei, Qingsong; Jing, Huarong; Li, You; Yisibashaer, Wuerzha; Chen, Jian; Nan Li, Bing; Zhang, Yong

2016-01-15

The integration of smartphone with paper sensors recently has been gain increasing attentions because of the achievement of quantitative and rapid analysis. However, smartphone based upconversional paper sensors have been restricted by the lack of effective methods to acquire luminescence signals on test paper. Herein, by the virtue of 3D printing technology, we exploited an auxiliary reusable device, which orderly assembled a 980nm mini-laser, optical filter and mini-cavity together, for digitally imaging the luminescence variations on test paper and quantitative analyzing pesticide thiram by smartphone. In detail, copper ions decorated NaYF4:Yb/Tm upconversion nanoparticles were fixed onto filter paper to form test paper, and the blue luminescence on it would be quenched after additions of thiram through luminescence resonance energy transfer mechanism. These variations could be monitored by the smartphone camera, and then the blue channel intensities of obtained colored images were calculated to quantify amounts of thiram through a self-written Android program installed on the smartphone, offering a reliable and accurate detection limit of 0.1μM for the system. This work provides an initial demonstration of integrating upconversion nanosensors with smartphone digital imaging for point-of-care analysis on a paper-based platform. Copyright © 2015 Elsevier B.V. All rights reserved.

Femtosecond Fluorescence Upconversion Study of a Naphthalimide-Bithiophene-Triphenylamine Push-Pull Dye in Solution.

PubMed

Maffeis, Valentin; Brisse, Romain; Labet, Vanessa; Jousselme, Bruno; Gustavsson, Thomas

2018-06-13

There is a high interest in the development of new push-pull dyes for the use in dye sensitized solar cells. The pronounced charge transfer character of the directly photoexcited state is in principle favorable for a charge injection. Here, we report a time-resolved fluorescence study of a triphenylamine-bithiophene-naphthalimide dye in four solvents of varying polarity using fluorescence upconversion. The recording of femtosecond time-resolved fluorescence spectra corrected for the group velocity dispersion allows for a detailed analysis discriminating between spectral shifts and total intensity decays. After photoexcitation, the directly populated state (S 1 /FC) evolves toward a relaxed charge transfer state (S 1 /CT). This S 1 /CT state is characterized by a lower radiative transition moment and a higher nonradiative quenching. The fast dynamic shift of the fluorescence band is well described by solvation dynamics in polar solvents, but less so in nonpolar solvents, hinting that the excited-state relaxation process occurs on a free energy surface whose topology is strongly governed by the solvent polarity. This study underlines the influence of the environment on the intramolecular charge transfer (ICT) process, and the necessity to analyze time-resolved data in detail when solvation and ICT occur simultaneously.

Optical frequency upconversion technique for transmission of wireless MIMO-type signals over optical fiber.

PubMed

Shaddad, R Q; Mohammad, A B; Al-Gailani, S A; Al-Hetar, A M

2014-01-01

The optical fiber is well adapted to pass multiple wireless signals having different carrier frequencies by using radio-over-fiber (ROF) technique. However, multiple wireless signals which have the same carrier frequency cannot propagate over a single optical fiber, such as wireless multi-input multi-output (MIMO) signals feeding multiple antennas in the fiber wireless (FiWi) system. A novel optical frequency upconversion (OFU) technique is proposed to solve this problem. In this paper, the novel OFU approach is used to transmit three wireless MIMO signals over a 20 km standard single mode fiber (SMF). The OFU technique exploits one optical source to produce multiple wavelengths by delivering it to a LiNbO3 external optical modulator. The wireless MIMO signals are then modulated by LiNbO3 optical intensity modulators separately using the generated optical carriers from the OFU process. These modulators use the optical single-sideband with carrier (OSSB+C) modulation scheme to optimize the system performance against the fiber dispersion effect. Each wireless MIMO signal is with a 2.4 GHz or 5 GHz carrier frequency, 1 Gb/s data rate, and 16-quadrature amplitude modulation (QAM). The crosstalk between the wireless MIMO signals is highly suppressed, since each wireless MIMO signal is carried on a specific optical wavelength.

Enhanced light emission near 2.7 μm from Er-Nd co-doped germanate glass

NASA Astrophysics Data System (ADS)

Bai, Gongxun; Tao, Lili; Li, Kefeng; Hu, Lili; Tsang, Yuen Hong

2013-04-01

Laser glass gain medium that can convert low cost 808 nm diode laser into 2.7 μm has attracted considerable interest due to its potential application for medical surgery fiber laser system. In this study, enhanced 2.7 μm emission has been achieved in Er3+:germanate glass by co-doping with Nd3+ ions under the excitation of an 808 nm diode laser. In the co-doped sample, the experimental results show that the harmful visible emissions via up-conversion were effectively restricted. The reduction of 1.5 μm emission was also detected in the co-doped sample, which indicates significant de-excitation of 4I13/2 Er3+ ion through energy transfer and non-radiative decay in Nd3+ ions. In conclusion, the 2.7 μm emission enhancement achieved was due to the increased optical absorption of 808 nm, efficient energy transfer (ET) with efficiency of 81.73% between Er3+ and Nd3+ ions, and shortening the lifetime of the lower lasing level 4I13/2 Er3+ in the co-doped sample. Therefore, Er3+/Nd3+ co-doped germanate glass could be used to fabricate fiber optical gain media for 2.7 μm laser generation.

High quantum-yield phosphors via quantum splitting and upconversion

NASA Astrophysics Data System (ADS)

Jeong, Joayoung

The Gd3+ ion has been used to induce quantum splitting in luminescent materials by using cross-relaxation energy transfer (CRET). In Nd:LiGdF4, quantum splitting results from a two-step CRET between Gd3+ and Nd3+, first involving a transition 6G→6I on Gd3+ and an excitation within the 4f3 configuration of Nd3+ followed by a second CRET that brings Gd3+ to 6P7/2. The excited Nd3+ ion rapidly relaxes nonradiatively to the emitting 4F3/2. The excited Gd3+ ion then transfers its energy back to Nd3+, which gives rise to the second photon. The result is a quantum yield of 1.05 +/- 0.35 with emission in the NIR following excitation at 175 nm. GdF3:Pr3+, Eu 3+ also exhibits quantum splitting, but only at very low concentration of Pr3+ (0.3%) and Eu3+ (0.2%), resulting in a quantum yield of approximately 20% under 160-nm excitation. Host intrinsic emission via a self-trapped exciton (STE) was also examined as a means to sensitize Gd3+ emission. The material ScPO4:Gd 3+ exhibits a high absolute quantum yield of 0.9 +/- 0.2 under 170-nm excitation, demonstrating a potentially new and efficient pathway for exciting quantum splitting phosphors. Single crystals of the material GdZrF7 were grown, and its structure was established via single-crystal X-ray diffraction methods. Doped samples of GdZrF7:Yb3+, Er3+ exhibit bright up-conversion luminescence with light output that is up to twice that of a commercial material based on the host Gd2O2S. When doped with Eu3+, the fluoride also emits a nearly white color under vacuum ultraviolet excitation with an absolute quantum yield near 0.9. The new compound Gd4.67(SiO4)3S was synthesized and studied. The structure was established via single-crystal X-ray methods, and the luminescence of Tb3+ samples was investigated.

Y{sub 2}O{sub 3}:Yb/Er nanotubes: Layer-by-layer assembly on carbon-nanotube templates and their upconversion luminescence properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Huang, Weishi; Shen, Jianfeng; Wan, Lei

2012-11-15

Graphical abstract: Well-shaped Y{sub 2}O{sub 3}:Yb/Er nanotubes have been successfully synthesized on a large scale via layer-by-layer assembly on carbon nanotubes templates followed by a subsequent heat treatment process. The as-prepared Y{sub 2}O{sub 3}:Yb/Er nanotubes show a strong red emission corresponding to the {sup 4}F{sub 9/2}–{sup 4}I{sub 15/2} transition of the Er{sup 3+} ions under excitation at 980 nm. Display Omitted Highlights: ► Well-shaped Y{sub 2}O{sub 3}:Yb/Er nanotubes have been successfully synthesized. ► CNTs were used as templates for Y{sub 2}O{sub 3}:Yb/Er nanotubes. ► LBL assembly and calcination were used for preparation of Y{sub 2}O{sub 3}:Yb/Er nanotubes. ► The as-preparedmore » Y{sub 2}O{sub 3}:Yb/Er nanotubes show a strong red emission. -- Abstract: Well-shaped Y{sub 2}O{sub 3}:Yb/Er nanotubes have been successfully synthesized on a large scale via layer-by-layer (LBL) assembly on carbon nanotubes (CNTs) templates followed by a subsequent heat treatment process. The crystal structure, element analysis, morphology and upconversion luminescence properties were characterized. XRD results demonstrate that the diffraction peaks of the samples calcinated at 800 °C or above can be indexed to the pure cubic phase of Y{sub 2}O{sub 3}. SEM images indicate that a large quantity of uniform and rough nanotubes with diameters of about 30–60 nm can be observed. The as-prepared Y{sub 2}O{sub 3}:Yb/Er nanotubes show a strong red emission corresponding to the {sup 4}F{sub 9/2}–{sup 4}I{sub 15/2} transition of the Er{sup 3+} ions under excitation at 980 nm, which have potential applications in such fields as nanoscale devices, molecular catalysts, nanobiotechnology, photonics and optoelectronics.« less

Role of Er3+ concentration in spectroscopic and laser performance of CaYAlO4 crystal

NASA Astrophysics Data System (ADS)

Lv, Shaozhen; Wang, Yan; Zhu, Zhaojie; You, Zhenyu; Li, Jianfu; Wang, Hongyan; Tu, Chaoyang

2015-04-01

Three heavily Er3+-doped CaYAlO4 single crystals were successfully grown by Czochralski method. The emission spectra and the fluorescence decay curves have been recorded at room temperature. A combination of experimental data, rate equation and Dexter theory are used to investigate the influence of Er3+ doping concentration on the spectra character and the inner cross relaxation of Er3+:CaYAlO4 crystal. Results show that the self terminate effect of the transition 4I11/2 → 4I13/2 can be suppressed by heavy Er3+doping. But if the doping concentration goes too high, the much larger cross relaxation coefficient of 4I11/2 level than that of 4I13/2 level would results in the increase of up-conversion emission and the quench of near and mid infrared emission. The laser performance was also studied. The maximum output power of 225 mW at 2733 nm was acquired with an optical conversion efficiency of 14.9%.

Photocatalytic Water-Splitting Enhancement by Sub-Bandgap Photon Harvesting.

PubMed

Monguzzi, Angelo; Oertel, Amadeus; Braga, Daniele; Riedinger, Andreas; Kim, David K; Knüsel, Philippe N; Bianchi, Alberto; Mauri, Michele; Simonutti, Roberto; Norris, David J; Meinardi, Francesco

2017-11-22

Upconversion is a photon-management process especially suited to water-splitting cells that exploit wide-bandgap photocatalysts. Currently, such catalysts cannot utilize 95% of the available solar photons. We demonstrate here that the energy-conversion yield for a standard photocatalytic water-splitting device can be enhanced under solar irradiance by using a low-power upconversion system that recovers part of the unutilized incident sub-bandgap photons. The upconverter is based on a sensitized triplet-triplet annihilation mechanism (sTTA-UC) obtained in a dye-doped elastomer and boosted by a fluorescent nanocrystal/polymer composite that allows for broadband light harvesting. The complementary and tailored optical properties of these materials enable efficient upconversion at subsolar irradiance, allowing the realization of the first prototype water-splitting cell assisted by solid-state upconversion. In our proof-of concept device the increase of the performance is 3.5%, which grows to 6.3% if concentrated sunlight (10 sun) is used. Our experiments show how the sTTA-UC materials can be successfully implemented in technologically relevant devices while matching the strict requirements of clean-energy production.

808 nm-excited upconversion nanoprobes with low heating effect for targeted magnetic resonance imaging and high-efficacy photodynamic therapy in HER2-overexpressed breast cancer.

PubMed

Zeng, Leyong; Pan, Yuanwei; Zou, Ruifen; Zhang, Jinchao; Tian, Ying; Teng, Zhaogang; Wang, Shouju; Ren, Wenzhi; Xiao, Xueshan; Zhang, Jichao; Zhang, Lili; Li, Aiguo; Lu, Guangming; Wu, Aiguo

2016-10-01

To avoid the overheating effect of excitation light and improve the efficacy of photodynamic therapy (PDT) of upconversion nanoplatform, a novel nanoprobe based on 808 nm-excited upconversion nanocomposites (T-UCNPs@Ce6@mSiO2) with low heating effect and deep penetration has been successfully constructed for targeted upconversion luminescence, magnetic resonance imaging (MRI) and high-efficacy PDT in HER2-overexpressed breast cancer. In this nanocomposite, photosensitizers (Ce6) were covalently conjugated inside of mesoporous silica to enhance the PDT efficacy by shortening the distance of fluorescence resonance energy transfer and to decrease the cytotoxicity by preventing the undesired leakage of Ce6. Compared with UCNPs@mSiO2@Ce6, UCNPs@Ce6@mSiO2 greatly promoted the singlet oxygen generation and amplified the PDT efficacy under the excitation of 808 nm laser. Importantly, the designed nanoprobe can greatly improve the uptake of HER2-positive cells and tumors by modifying the site-specific peptide, and the in vivo experiments showed excellent MRI and PDT via intravenous injection by modeling MDA-MB-435 tumor-bearing nude mice. Our strategy may provide an effective solution for overcoming the heating effect and improving the PDT efficacy of upconversion nanoprobes, and has potential application in visualized theranostics of HER2-overexpressed breast cancer. Copyright © 2016 Elsevier Ltd. All rights reserved.

One-step nucleotide-programmed growth of porous upconversion nanoparticles: application to cell labeling and drug delivery

NASA Astrophysics Data System (ADS)

Zhou, Li; Li, Zhenhua; Liu, Zhen; Yin, Meili; Ren, Jinsong; Qu, Xiaogang

2014-01-01

A simple and ``green'' strategy has been reported for the first time to fabricate upconversion nanoparticles (UCNPs) by utilizing nucleotides as bio-templates. The influence of the functionalities present on the nucleotide on the production of nanoparticles was investigated in detail. Through the effects of nucleotides, the obtained nanoparticles possessed a porous structure. The use of the as-prepared UCNPs for cell imaging, drug delivery and versatile therapy applications were demonstrated. In view of the bright up-conversion luminescence as well as the excellent biocompatibility, and the good colloidal stability of the as-prepared UCNPs, we envision that our synthesis protocol might advance both the fields of UCNPs and biomolecule-based nanotechnology for future studies.A simple and ``green'' strategy has been reported for the first time to fabricate upconversion nanoparticles (UCNPs) by utilizing nucleotides as bio-templates. The influence of the functionalities present on the nucleotide on the production of nanoparticles was investigated in detail. Through the effects of nucleotides, the obtained nanoparticles possessed a porous structure. The use of the as-prepared UCNPs for cell imaging, drug delivery and versatile therapy applications were demonstrated. In view of the bright up-conversion luminescence as well as the excellent biocompatibility, and the good colloidal stability of the as-prepared UCNPs, we envision that our synthesis protocol might advance both the fields of UCNPs and biomolecule-based nanotechnology for future studies. Electronic supplementary information (ESI) available: Supporting figures. See DOI: 10.1039/c3nr04255c

Folic acid-functionalized up-conversion nanoparticles: toxicity studies in vivo and in vitro and targeted imaging applications

NASA Astrophysics Data System (ADS)

Sun, Lining; Wei, Zuwu; Chen, Haige; Liu, Jinliang; Guo, Jianjian; Cao, Ming; Wen, Tieqiao; Shi, Liyi

2014-07-01

Folate receptors (FRs) are overexpressed on a variety of human cancer cells and tissues, including cancers of the breast, ovaries, endometrium, and brain. This over-expression of FRs can be used to target folate-linked imaging specifically to FR-expressing tumors. Fluorescence is emerging as a powerful new modality for molecular imaging in both the diagnosis and treatment of disease. Combining innovative molecular biology and chemistry, we prepared three kinds of folate-targeted up-conversion nanoparticles as imaging agents (UCNC-FA: UCNC-Er-FA, UCNC-Tm-FA, and UCNC-Er,Tm-FA). In vivo and in vitro toxicity studies showed that these nanoparticles have both good biocompatibility and low toxicity. Moreover, the up-conversion luminescence imaging indicated that they have good targeting to HeLa cells and can therefore serve as potential fluorescent contrast agents.Folate receptors (FRs) are overexpressed on a variety of human cancer cells and tissues, including cancers of the breast, ovaries, endometrium, and brain. This over-expression of FRs can be used to target folate-linked imaging specifically to FR-expressing tumors. Fluorescence is emerging as a powerful new modality for molecular imaging in both the diagnosis and treatment of disease. Combining innovative molecular biology and chemistry, we prepared three kinds of folate-targeted up-conversion nanoparticles as imaging agents (UCNC-FA: UCNC-Er-FA, UCNC-Tm-FA, and UCNC-Er,Tm-FA). In vivo and in vitro toxicity studies showed that these nanoparticles have both good biocompatibility and low toxicity. Moreover, the up-conversion luminescence imaging indicated that they have good targeting to HeLa cells and can therefore serve as potential fluorescent contrast agents. Electronic supplementary information (ESI) available: Up-conversion luminescence spectra of UCNC-Er and UCNC-Er-FA, UCNC-Tm and UCNC-Tm-FA. Confocal luminescence imaging data collected as a series along the Z optical axis. See DOI: 10.1039/c4nr02312a

Enantiopure distorted ribbon-shaped nanographene combining two-photon absorption-based upconversion and circularly polarized luminescence† †Electronic supplementary information (ESI) available: General details, synthesis and spectroscopy data of new compounds. Experimental details on optical, chiroptical, electrochemical and on-surface measurements. Crystal data and structure refinement of compounds 1, and 6. Further details on theoretical calculations and Cartesian coordinates of computed structures. VT-H1NMR, 2D-NMR and HRMS spectra of 1. CCDC 1561552 and 1561553. For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c8sc00427g

PubMed Central

Cruz, Carlos M.; Márquez, Irene R.; Mariz, Inês F. A.; Blanco, Victor; Sánchez-Sánchez, Carlos; Sobrado, Jesús M.; Martín-Gago, José A.; Cuerva, Juan M.

2018-01-01

Herein we describe a distorted ribbon-shaped nanographene exhibiting unprecedented combination of optical properties in graphene-related materials, namely upconversion based on two-photon absorption (TPA-UC) together with circularly polarized luminescence (CPL). The compound is a graphene molecule of ca. 2 nm length and 1 nm width with edge defects that promote the distortion of the otherwise planar lattice. The edge defects are an aromatic saddle-shaped ketone unit and a [5]carbohelicene moiety. This system is shown to combine two-photon absorption and circularly polarized luminescence and a remarkably long emission lifetime of 21.5 ns. The [5]helicene is responsible for the chiroptical activity while the push–pull geometry and the extended network of sp2 carbons are factors favoring the nonlinear absorption. Electronic structure theoretical calculations support the interpretation of the results. PMID:29780523

Neuroendocrine Tumor-Targeted Upconversion Nanoparticle-Based Micelles for Simultaneous NIR-Controlled Combination Chemotherapy and Photodynamic Therapy, and Fluorescence Imaging.

PubMed

Chen, Guojun; Jaskula-Sztul, Renata; Esquibel, Corinne R; Lou, Irene; Zheng, Qifeng; Dammalapati, Ajitha; Harrison, April; Eliceiri, Kevin W; Tang, Weiping; Chen, Herbert; Gong, Shaoqin

2017-02-23

Although neuroendocrine tumors (NETs) are slow growing, they are frequently metastatic at the time of discovery and no longer amenable to curative surgery, emphasizing the need for the development of other treatments. In this study, multifunctional upconversion nanoparticle (UCNP)-based theranostic micelles are developed for NET-targeted and near-infrared (NIR)-controlled combination chemotherapy and photodynamic therapy (PDT), and bioimaging. The theranostic micelle is formed by individual UCNP functionalized with light-sensitive amphiphilic block copolymers poly(4,5-dimethoxy-2-nitrobenzyl methacrylate)-polyethylene glycol (PNBMA-PEG) and Rose Bengal (RB) photosensitizers. A hydrophobic anticancer drug, AB3, is loaded into the micelles. The NIR-activated UCNPs emit multiple luminescence bands, including UV, 540 nm, and 650 nm. The UV peaks overlap with the absorption peak of photocleavable hydrophobic PNBMA segments, triggering a rapid drug release due to the NIR-induced hydrophobic-to-hydrophilic transition of the micelle core and thus enabling NIR-controlled chemotherapy. RB molecules are activated via luminescence resonance energy transfer to generate 1 O 2 for NIR-induced PDT. Meanwhile, the 650 nm emission allows for efficient fluorescence imaging. KE108, a true pansomatostatin nonapeptide, as an NET-targeting ligand, drastically increases the tumoral uptake of the micelles. Intravenously injected AB3-loaded UCNP-based micelles conjugated with RB and KE108-enabling NET-targeted combination chemotherapy and PDT-induce the best antitumor efficacy.

Efficient charge transfer and utilization of near-infrared solar spectrum by ytterbium and thulium codoped gadolinium molybdate (Gd2(MoO4)3:Yb/Tm) nanophosphor in hybrid solar cells.

PubMed

Sun, Weifu; Chen, Zihan; Zhang, Qin; Zhou, Junli; Li, Feng; Jin, Xiao; Li, Dongyu; Li, Qinghua

2016-11-09

In this work, thulium and ytterbium codoped gadolinium molybdate (Gd 2 (MoO 4 ) 3 :Yb/Tm) nanophosphors (NPs) have been synthesized, followed by being incorporated into a photo-catalytic titania (TiO 2 ) nanoparticle layer. In detail, morphology and phase identification of the prepared NPs are first characterized and then the up-conversion of the Gd 2 (MoO 4 ) 3 :Yb/Tm NPs is studied. Electron transfer dynamics after interfacing with bare or NP-doped electron donor TiO 2 and the corresponding photovoltaic performance of solar cells are explored. The results show that Gd 2 (MoO 4 ) 3 :Yb/Tm NPs excited at 976 nm exhibit intense blue (460-498 nm) and weak red (627-669 nm) emissions. The lifetime of electron transfer is shortened from 817 to 316 ps after incorporating NPs and correspondingly the electron transfer rate outstrips by 3 times that of the bare TiO 2 . Consequently, a notable power conversion efficiency of 4.15% is achieved as compared to 3.17% of pure TiO 2 /PTB7. This work demonstrates that the co-doping of robust rare earth ions with different unique functions can widen the harvesting range of the solar spectrum, boost electron transfer rate and eventually strengthen device performance, without complicated interfacial and structural engineering.