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Sample records for femtosecond fluorescence upconversion

  1. Femtosecond broadband fluorescence upconversion spectroscopy: Spectral coverage versus efficiency.

    PubMed

    Gerecke, Mario; Bierhance, Genaro; Gutmann, Michael; Ernsting, Nikolaus P; Rosspeintner, Arnulf

    2016-05-01

    Sum frequency mixing of fluorescence and ∼1300 nm gate pulses, in a thin β-barium borate crystal and non-collinear type II geometry, is quantified as part of a femtosecond fluorimeter [X.-X. Zhang et al., Rev. Sci. Instrum. 82, 063108 (2011)]. For a series of fixed phasematching angles, the upconversion efficiency is measured depending on fluorescence wavelength. Two useful orientations of the crystal are related by rotation around the surface normal. Orientation A has higher efficiency (factor ∼3) compared to B at the cost of some loss of spectral coverage for a given crystal angle. It should be used when subtle changes of an otherwise stationary emission band are to be monitored. With orientation B, the fluorescence range λF > 420-750 nm is covered with a single setting of the crystal and less gate scatter around time zero. The accuracy of determining an instantaneous emission band shape is demonstrated by comparing results from two laboratories. PMID:27250400

  2. 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

  3. Femtosecond fluorescence upconversion studies of excited-state proton-transfer dynamics in 2-(2 '-hydroxyphenyl)benzoxazole (HBO) in liquid solution and DNA

    NASA Astrophysics Data System (ADS)

    Wang, H.; Zhang, H.; Abou-Zied, O. K.; Yu, C.; Romesberg, F. E.; Glasbeek, M.

    2003-01-01

    A femtosecond fluorescence upconversion study is reported for HBO in solution, as well as for HBO incorporated in DNA. The typical time for the excited-state intramolecular proton-transfer reaction of the syn-enol tautomer in solution and in DNA has been determined to be 150 fs. In addition, the lifetimes of the keto, the anti-enol and the 'solvated enol' tautomer forms were determined in protic solvents, aprotic solvents and DNA. Picosecond rise and decay components in the fluorescence transients with characteristic times between 3 and 25 ps are also observed and attributed to the effects of vibrational cooling.

  4. Dielectric controlled excited state relaxation pathways of a representative push-pull stilbene: A mechanistic study using femtosecond fluorescence up-conversion technique

    NASA Astrophysics Data System (ADS)

    Rafiq, Shahnawaz; Sen, Pratik

    2013-02-01

    Femtosecond fluorescence up-conversion technique was employed to reinvestigate the intriguing dependence of fluorescence quantum yield of trans-4-dimethylamino-4'-nitrostilbene (DNS) on dielectric properties of the media. In polar solvents, such as methanol and acetonitrile, the two time components of the fluorescence transients were assigned to intramolecular charge transfer (ICT) dynamics and to the depletion of the ICT state to the ground state via internal conversion along the torsional coordinate of nitro moiety. The viscosity independence of the first time component indicates the absence of any torsional coordinate in the charge transfer process. In slightly polar solvent (carbon tetrachloride) the fluorescence transients show a triple exponential behavior. The first time component was assigned to the formation of the ICT state on a 2 ps time scale. Second time component was assigned to the relaxation of the ICT state via two torsion controlled channels. First channel involves the torsional motion about the central double bond leading to the trans-cis isomerization via a conical intersection or avoided crossing. The other channel contributing to the depopulation of ICT state involves the torsional coordinates of dimethylanilino and/or nitrophenyl moieties and leads to the formation of a conformationally relaxed state, which subsequently relaxes back to the ground state radiatively, and is responsible for the high fluorescence quantum yield of DNS in slightly polar solvents such as carbon tetrachloride, toluene, etc. The excited singlet state which is having a dominant π-π* character may also decay via intersystem crossing to the n-π* triplet manifold and thus accounts for the observed triplet yield of the molecule in slightly polar solvents.

  5. Femtosecond Laser-Induced Upconversion Luminescence in Rare-Earth Ions by Nonresonant Multiphoton Absorption.

    PubMed

    Yao, Yunhua; Xu, Cheng; Zheng, Ye; Yang, Chengshuai; Liu, Pei; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong; Zhang, Shian

    2016-07-21

    The upconversion luminescence of rare-earth ions has attracted considerable interest because of its important applications in photoelectric conversion, color display, laser device, multiplexed biolabeling, and security printing. Previous studies mainly explored the upconversion luminescence generation through excited state absorption, energy transfer upconversion, and photon avalanche under the continuous wave laser excitation. Here, we focus on the upconversion luminescence generation through a nonresonant multiphoton absorption by using the intense femtosecond pulsed laser excitation and study the upconversion luminescence intensity control by varying the femtosecond laser phase and polarization. We show that the upconversion luminescence of rare-earth ions under the intense femtosecond laser field excitation is easy to be obtained due to the nonresonant multiphoton absorption through the nonlinear interaction between light and matter, which is not available by the continuous wave laser excitation in previous works. We also show that the upconversion luminescence intensity can be effectively controlled by varying the femtosecond pulsed laser phase and polarization, which can open a new technological opportunity to generate and control the upconversion luminescence of rare-earth ions and also can be further extended to the relevant application areas. PMID:27367751

  6. 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

  7. Paper-based microfluidic device with upconversion fluorescence assay.

    PubMed

    He, Mengyuan; Liu, Zhihong

    2013-12-17

    A paper-based microfluidic device with upconversion fluorescence assay (named as UC-μPAD) is proposed. The device is fabricated on a normal office printing sheet with a simple plotting method. Upconversion phosphors (UCPs) tagged with specific probes are spotted to the test zones on the μPAD, followed by the introduction of assay targets. Upconversion fluorescence measurements are directly conducted on the test zones after the completion of the probe-to-target reactions, without any post-treatments. The UC-μPAD features very easy fabrication and operation, simple and fast detection, low cost, and high sensitivity. UC-μPAD is a promising prospect for a clinical point-of-care test. PMID:24308347

  8. Unravelling molecular mechanisms in the fluorescence spectra of doxorubicin in aqueous solution by femtosecond fluorescence spectroscopy.

    PubMed

    Changenet-Barret, Pascale; Gustavsson, Thomas; Markovitsi, Dimitra; Manet, Ilse; Monti, Sandra

    2013-02-28

    Doxorubicin (DOX) is a potent anti-tumoral agent widely used for cancer therapy. Despite numerous studies, the fluorescence properties of DOX, usually exploited for the characterization of the interaction with biological media, have until now led to controversial interpretations, mainly due to self-association of the drug in aqueous solution. We present here the first femtosecond study of DOX based on measurements with the fluorescence up-conversion technique in combination with time-correlated single photon counting using the same laser source. We provide evidence that fluorescence signals of DOX stem from monomers and dimers. DOX dimerization induces a dramatic decrease in the fluorescence quantum yield from 3.9 × 10(-2) to 10(-5) associated with the red shift of the fluorescence spectrum by ~25 nm. While the fluorescence lifetime of the monomer is 1 ns, the dimer fluorescence is found to decay with a lifetime of about 2 ps. In contrast to monomers, the fluorescence anisotropy of dimers is found to be negative. These experimental observations are consistent with an ultrafast internal conversion (<200 fs) between two exciton states, possibly followed by a charge separation process. PMID:23340955

  9. Ratiometric fluorescent nanosensors for selective detecting cysteine with upconversion luminescence.

    PubMed

    Guan, Yunlong; Qu, Songnan; Li, Bin; Zhang, Liming; Ma, Heping; Zhang, Ligong

    2016-03-15

    Fluorescent sensors based on upconversion (UC) luminescence have been considered as a promising strategy to detect bio-analyte due to their advantages in deep penetration, minimum autofluorescence, and ratiometric fluorescent output. A prototype of nanosensors combined with mesoporous silica coated upconversion nanoparticles (UCNPs) and a fluorescein-based fluorescent probe loaded in pores was therefore designed to detect cysteine (Cys). The silica shell provided loading space for the probe and enabled the nanosensors to disperse in water. In the presence of Cys, the fluorescent probe was transformed into 5(6)-carboxyfluorescein with an emission band centering at 518 nm which was secondarily excited by the light at around 475 nm from NaYF4:Yb(3+), Tm(3+) UCNPs driven by 980 nm near-infrared (NIR) laser. The intensity ratio between green and blue luminescence (I518/I475) grew exponentially with increasing concentrations of Cys over a range of 20-200 μmolL(-1). The response of the nanosensors towards Cys was recognizable with naked eyes by luminescence color change. Evidences suggest that these nanosensors are capable of sensing Cys in aqueous solution and distinguishing Cys from homocysteine (Hcy) with kinetically-controlled selectivity. The system was further employed to detect Cys in human serum and the result was in agreement with it tested by high performance liquid chromatography with acceptable recovery. PMID:26402589

  10. 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. PMID:27236725

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

    NASA Astrophysics Data System (ADS)

    Jia, Zhixu; Yao, Chuanfei; Wang, Shunbin; Zheng, Kezhi; Xiong, Liangming; Luo, Jie; Lv, Dajuan; Qin, Guanshi; Ohishi, Yasutake; Qin, Weiping

    2016-04-01

    We report enhanced upconversion (UC) fluorescence in Tm3+ 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 3H4 → 3H6 transition of Tm3+ 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 the pumping of the 1560 nm femtosecond fiber laser.

  12. Graphene quantum dots from graphite by liquid exfoliation showing excitation-independent emission, fluorescence upconversion and delayed fluorescence.

    PubMed

    Sarkar, Suprabhat; Gandla, Dayakar; Venkatesh, Yeduru; Bangal, Prakriti Ranjan; Ghosh, Sutapa; Yang, Yang; Misra, Sunil

    2016-08-21

    Facile synthesis of 2-10 nm-sized graphene quantum dots (GQDs) from graphite powder by organic solvent-assisted liquid exfoliation using a sonochemical method is reported in this study. Synthesized GQDs are well dispersed in organic solvents like ethyl acetoacetate (EAA), dimethyl formamide (DMF) and also in water. MALDI-TOF mass spectrometry reveals its selective mass fragmentation. Detailed characterizations by various techniques like X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy and high resolution transmission electron microscopy (HRTEM) confirm the formation of disordered, functional GQDs. Density functional theory (DFT) calculation confirms HOMO-LUMO energy gap variation with changing size and functionalities. Photoluminescence (PL) properties of as-prepared GQDs were studied in detail. The ensemble studies of GQDs showed excellent photoluminescence properties comprising normal and upconverted fluorescence, delayed fluorescence and room-temperature phosphorescence. PL decay dynamics of GQDs has been explored using time-correlated single-photon technique (TCSPC) as well as femtosecond fluorescence upconversion technique. In vitro cytotoxicity study reveals its biocompatibility and high cell viability (>91%) even at high concentration (400 μg mL(-1)) of GQDs in Chinese Hamster Ovary (CHO) cells. PMID:27302411

  13. Ultrafast fluorescence upconversion technique and its applications to proteins.

    PubMed

    Chosrowjan, Haik; Taniguchi, Seiji; Tanaka, Fumio

    2015-08-01

    The basic principles and main characteristics of the ultrafast time-resolved fluorescence upconversion technique (conventional and space-resolved), including requirements for nonlinear crystals, mixing spectral bandwidth, acceptance angle, etc., are presented. Applications to flavoproteins [wild-type (WT) FMN-binding protein and its W32Y, W32A, E13R, E13K, E13Q and E13T mutants] and photoresponsive proteins [WT photoactive yellow protein and its R52Q mutant in solution and as single crystals] are demonstrated. For flavoproteins, investigations elucidating the effects of ionic charges on ultrafast electron transfer (ET) dynamics are summarized. It is shown that replacement of the ionic amino acid Glu13 and the resulting modification of the electrostatic charge distribution in the protein chromphore-binding pocket substantially alters the ultrafast fluorescence quenching dynamics and ET rate in FMN-binding protein. It is concluded that, together with donor-acceptor distances, electrostatic interactions between ionic photoproducts and other ionic groups in the proteins are important factors influencing the ET rates. In WT photoactive yellow protein and the R52Q mutant, ultrafast photoisomerization dynamics of the chromophore (deprotonated trans-p-coumaric acid) in liquid and crystal phases are investigated. It is shown that the primary dynamics in solution and single-crystal phases are quite similar; hence, the photocycle dynamics and structural differences observed at longer time scales arise mostly from the structural restraints imposed by the crystal lattice rigidity versus the flexibility in solution. PMID:25532707

  14. 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. PMID:18596348

  15. Ultrafast Dynamics of Polythiophene with Phenyl Vinylene Branches Studied by Femtosecond Fluorescence Spectroscopy in Solution

    NASA Astrophysics Data System (ADS)

    Chu, Sai-Sai; Gao, Chao; Wang, Shu-Feng; Gong, Qi-Huang

    2011-11-01

    Two polythiophene based polymers, poly[(3-[2-[4-(2-ethyl-hexyloxy)-phenyl]-vinyl]-thiophene)-co-thiophene] (PT1) and poly(3-[2-[4-(2-ethyl-hexyloxy)-phenyl]-vinyl]-thiophene) (PT2), are synthesized and investigated by static, picosecond fluorescence spectroscopies and the femtosecond up-conversion technique in solution. Compared with pristine poly(3-hexylthiophene) (P3HT), PT1 and PT2, in which the main chains are decorated with phenyl vinylene present a ‘camel back’ structure in the absorption spectra. Phenyl vinylene side chains induce a new process of charge transfer, chain twisting motion and defect-induced fluorescence quenching at time scales of 1 ps, 10 ps and 150 ps, respectively.

  16. Laser polarization and phase control of up-conversion fluorescence in rare-earth ions

    PubMed Central

    Yao, Yunhua; Zhang, Shian; Zhang, Hui; Ding, Jingxin; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong

    2014-01-01

    We theoretically and experimentally demonstrate the up-conversion fluorescence control via resonance-mediated two-photon absorption in rare-earth ions by varying both the laser polarization and phase. We show that both the laser polarization and phase can control the up-conversion fluorescence, and the up-conversion fluorescence intensity is decreased when the laser polarization changes from linear through elliptical to circular. We also show that the laser polarization will affect the control efficiency of the up-conversion fluorescence by varying the laser phase, and the circular polarization will reduce the control efficiency. Furthermore, we suggest that the control efficiency by varying the laser polarization and the effect of the laser polarization on the control efficiency by varying the laser phase can be artificially manipulated by controlling the laser spectral bandwidth. This optical control method opens a new opportunity to control the up-conversion fluorescence of rare-earth ions, which may have significant impact on the related applications of rare-earth ions. PMID:25465401

  17. Fluorescence upconversion properties of a class of improved pyridinium dyes induced by two-photon absorption

    NASA Astrophysics Data System (ADS)

    Xu, Guibao; Hu, Dawei; Zhao, Xian; Shao, Zongshu; Liu, Huijun; Tian, Yupeng

    2007-06-01

    We report the fluorescence upconversion properties of a class of improved pyridinium toluene- p-sulfonates having donor- π-acceptor (D- π-A) structure under two-photon excitation at 1064 nm. The experimental results show that both the two-photon excited (TPE) fluorescence lifetime and the two-photon pumped (TPP) energy upconversion efficiency were increased with the enhancement of electron-donating capability of the donor in the molecule. It is also indicated that an overlong alkyl group tends to result in a weakened molecular conjugation, leading to a decreased two-photon absorption (TPA) cross section. By choosing the donor, we can obtain a longest fluorescence lifetime of 837 ps, a highest energy upconversion efficiency of ˜6.1%, and a maximum TPA cross-section of 8.74×10 -48 cm 4 s/photon in these dyes.

  18. Paper-based upconversion fluorescence resonance energy transfer biosensor for sensitive detection of multiple cancer biomarkers

    PubMed Central

    Xu, Sai; Dong, Biao; Zhou, Donglei; Yin, Ze; Cui, Shaobo; Xu, Wen; Chen, Baojiu; Song, Hongwei

    2016-01-01

    A paper-based upconversion fluorescence resonance energy transfer assay device is proposed for sensitive detection of CEA. The device is fabricated on a normal filter paper with simple nano-printing method. Upconversion nanoparticles tagged with specific antibodies are printed to the test zones on the test paper, followed by the introduction of assay antigen. Upconversion fluorescence measurements are directly conducted on the test zones after the antigen-to-antibody reactions. Furthermore, a multi-channel test paper for simultaneous detection of multiple cancer biomarkers was established by the same method and obtained positive results. The device showed high anti-interfere, stability, reproducible and low detection limit (0.89 ng/mL), moreover it is very easy to fabricate and operate, which is a promising prospect for a clinical point-of-care test. PMID:27001460

  19. Paper-based upconversion fluorescence resonance energy transfer biosensor for sensitive detection of multiple cancer biomarkers

    NASA Astrophysics Data System (ADS)

    Xu, Sai; Dong, Biao; Zhou, Donglei; Yin, Ze; Cui, Shaobo; Xu, Wen; Chen, Baojiu; Song, Hongwei

    2016-03-01

    A paper-based upconversion fluorescence resonance energy transfer assay device is proposed for sensitive detection of CEA. The device is fabricated on a normal filter paper with simple nano-printing method. Upconversion nanoparticles tagged with specific antibodies are printed to the test zones on the test paper, followed by the introduction of assay antigen. Upconversion fluorescence measurements are directly conducted on the test zones after the antigen-to-antibody reactions. Furthermore, a multi-channel test paper for simultaneous detection of multiple cancer biomarkers was established by the same method and obtained positive results. The device showed high anti-interfere, stability, reproducible and low detection limit (0.89 ng/mL), moreover it is very easy to fabricate and operate, which is a promising prospect for a clinical point-of-care test.

  20. Microbubble embedded with upconversion nanoparticles as a bimodal contrast agent for fluorescence and ultrasound imaging

    NASA Astrophysics Data System (ADS)

    Jin, Birui; Lin, Min; You, Minli; Zong, Yujin; Wan, Mingxi; Xu, Feng; Duan, Zhenfeng; Lu, Tianjian

    2015-08-01

    Bimodal imaging offers additional imaging signal thus finds wide spread application in clinical diagnostic imaging. Fluorescence/ultrasound bimodal imaging contrast agent using fluorescent dyes or quantum dots for fluorescence signal has emerged as a promising method, which however requires visible light or UV irradiation resulting in photobleaching, photoblinking, auto-fluorescence and limited tissue penetration depth. To surmount these problems, we developed a novel bimodal contrast agent using layer-by-layer assembly of upconversion nanoparticles onto the surface of microbubbles. The resulting microbubbles with average size of 2 μm provide enhanced ultrasound echo for ultrasound imaging and upconversion emission upon near infrared irradiation for fluorescence imaging. The developed bimodal contrast agent holds great potential to be applied in ultrasound target technique for targeted diseases diagnostics and therapy.

  1. Enhanced upconversion luminescence from ZnO/Zn hybrid nanostructures induced on a Zn foil by femtosecond laser ablation.

    PubMed

    Li, Hui; Zhang, Cheng-Yun; Li, Xian-Feng; Xiang, Jin; Tie, Shao-Long; Lan, Sheng

    2015-11-16

    ZnO/Zn hybrid nanostructures including nanowires and nanonets were induced on a Zn foil by using 400-nm femtosecond (fs) laser pulses with a low repetition rate of 1 kHz and duration of 100 fs. The laser fluence was chosen to be slightly above the ablation threshold of Zn. The luminescence of the formed ZnO/Zn hybrid nanostructures was examined by using fs laser pulses with a high repetition rate of 76 MHz and duration of ~130 fs through both single-photon and multiphoton excitation. While the luminescence spectrum under the single-photon excitation exhibited a single peak at ~480 nm, a broadband upconversion luminescence with many ripples was observed under the multiphoton excitation. More interestingly, the upconversion luminescence of the ZnO/Zn hybrid nanostructures was significantly enhanced by the underlying Zn nanostructures which induced strongly localized electric field. The enhancement of the upconversion luminescence was verified by the short lifetime of only ~79 ps observed for the ZnO/Zn hybrid nanostructures, which is nearly one order of magnitude smaller as compared with the luminescence lifetime of the ZnO nanorods synthesized by using the chemical coprecipitation method. The localization of electric field in the ZnO/Zn hybrid nanostructures was confirmed by the numerical simulations based the finite-difference time-domain technique. PMID:26698492

  2. Multifunctional upconversion nanoprobe for tumor fluorescence imaging and near-infrared thermal therapy

    NASA Astrophysics Data System (ADS)

    Wei, Yanchun; Chen, Qun; Wu, Baoyan; Xing, Da

    2014-09-01

    The combination of diagnostics and therapeutics is growing rapidly in cancer treatment. Here, using upconversion nanoparticles coated with chitosan conjugated with a targeting molecule and loaded with indocyanine green (ICG), an excitation-selectable nanoprobe with highly integrated functionalities, including the emission of visible and near-infrared (NIR) light, strong optical absorption in the NIR region and high photostability was developed. After injected in mice, the nanoprobes targeted to the tumor vascular system. NIR lasers (980 and 808 nm) were then selectively applied to the mice. The results show that, the emitted upconversion fluorescence and NIR fluorescence can be used in a complementary manner for high signal/noise ratio and sensitive tumor imaging for more precise tumor localization; Highly effective photothermal therapy can be realized using 808 nm laser irradiation. The upconversion fluorescence at 654 nm is useful for monitoring treatment effect during thermal therapy. In summary, using the nanoprobes, outstanding therapeutic efficacy could be realized and the nanofabrication strategy would highlight the promise of upconversion nanoparticles in cancer theranostics.

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

    SciTech Connect

    Wu, Tony C.; Congreve, Daniel N.; Baldo, Marc A.

    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 is 1.1%. Our results demonstrate upconversion in solid state geometries and with non-heavy metal-based sensitizer materials.

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

    NASA Astrophysics Data System (ADS)

    Wu, Tony C.; Congreve, Daniel N.; Baldo, Marc A.

    2015-07-01

    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 is 1.1%. Our results demonstrate upconversion in solid state geometries and with non-heavy metal-based sensitizer materials.

  5. An upconversion fluorescent resonant energy transfer biosensor for hepatitis B virus (HBV) DNA hybridization detection.

    PubMed

    Zhu, Hao; Lu, Feng; Wu, Xing-Cai; Zhu, Jun-Jie

    2015-11-21

    A novel fluorescent resonant energy transfer (FRET) biosensor was fabricated for the detection of hepatitis B virus (HBV) DNA using poly(ethylenimine) (PEI) modified upconversion nanoparticles (NH2-UCNPs) as energy donor and gold nanoparticles (Au NPs) as acceptor. The PEI modified upconversion nanoparticles were prepared directly with a simple one-pot hydrothermal method, which provides high quality amino-group functionalized UCNPs with uniform morphology and strong upconversion luminescence. Two single-stranded DNA strands, which were partially complementary to each other, were then conjugated with NH2-UCNPs and Au NPs. When DNA conjugated NH2-UCNPs and Au NPs are mixed together, the hybridization between complementary DNA sequences on UCNPs and Au NPs will lead to the quenching of the upconversion luminescence due to the FRET process. Meanwhile, upon the addition of target DNA, Au NPs will leave the surface of the UCNPs and the upconversion luminescence can be restored because of the formation of the more stable double-stranded DNA on the UCNPs. The sensor we fabricated here for target DNA detection shows good sensitivity and high selectivity, which has the potential for clinical applications in the analysis of HBV and other DNA sequences. PMID:26421323

  6. A high performance fluorescence switching system triggered electrochemically by Prussian blue with upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Zhai, Yiwen; Zhang, Hui; Zhang, Lingling; Dong, Shaojun

    2016-05-01

    A high performance fluorescence switching system triggered electrochemically by Prussian blue with upconversion nanoparticles was proposed. We synthesized a kind of hexagonal monodisperse β-NaYF4:Yb3+,Er3+,Tm3+ upconversion nanoparticle and manipulated the intensity ratio of red emission (at 653 nm) and green emission at (523 and 541 nm) around 2 : 1, in order to match well with the absorption spectrum of Prussian blue. Based on the efficient fluorescence resonance energy transfer and inner-filter effect of the as-synthesized upconversion nanoparticles and Prussian blue, the present fluorescence switching system shows obvious behavior with high fluorescence contrast and good stability. To further extend the application of this system in analysis, sulfite, a kind of important anion in environmental and physiological systems, which could also reduce Prussian blue to Prussian white nanoparticles leading to a decrease of the absorption spectrum, was chosen as the target. And we were able to determine the concentration of sulfite in aqueous solution with a low detection limit and a broad linear relationship.A high performance fluorescence switching system triggered electrochemically by Prussian blue with upconversion nanoparticles was proposed. We synthesized a kind of hexagonal monodisperse β-NaYF4:Yb3+,Er3+,Tm3+ upconversion nanoparticle and manipulated the intensity ratio of red emission (at 653 nm) and green emission at (523 and 541 nm) around 2 : 1, in order to match well with the absorption spectrum of Prussian blue. Based on the efficient fluorescence resonance energy transfer and inner-filter effect of the as-synthesized upconversion nanoparticles and Prussian blue, the present fluorescence switching system shows obvious behavior with high fluorescence contrast and good stability. To further extend the application of this system in analysis, sulfite, a kind of important anion in environmental and physiological systems, which could also reduce Prussian blue to

  7. Broadband up-conversion at subsolar irradiance: triplet-triplet annihilation boosted by fluorescent semiconductor nanocrystals.

    PubMed

    Monguzzi, A; Braga, D; Gandini, M; Holmberg, V C; Kim, D K; Sahu, A; Norris, D J; Meinardi, F

    2014-11-12

    Conventional solar cells exhibit limited efficiencies in part due to their inability to absorb the entire solar spectrum. Sub-band-gap photons are typically lost but could be captured if a material that performs up-conversion, which shifts photon energies higher, is coupled to the device. Recently, molecular chromophores that undergo triplet-triplet annihilation (TTA) have shown promise for efficient up-conversion at low irradiance, suitable for some types of solar cells. However, the molecular systems that have shown the highest up-conversion efficiency to date are ill suited to broadband light harvesting, reducing their applicability. Here we overcome this limitation by combining an organic TTA system with highly fluorescent CdSe semiconductor nanocrystals. Because of their broadband absorption and spectrally narrow, size-tunable fluorescence, the nanocrystals absorb the radiation lost by the TTA chromophores, returning this energy to the up-converter. The resulting nanocrystal-boosted system shows a doubled light-harvesting ability, which allows a green-to-blue conversion efficiency of ∼12.5% under 0.5 suns of incoherent excitation. This record efficiency at subsolar irradiance demonstrates that boosting the TTA by light-emitting nanocrystals can potentially provide a general route for up-conversion for different photovoltaic and photocatalytic applications. PMID:25322197

  8. A high performance fluorescence switching system triggered electrochemically by Prussian blue with upconversion nanoparticles.

    PubMed

    Zhai, Yiwen; Zhang, Hui; Zhang, Lingling; Dong, Shaojun

    2016-05-01

    A high performance fluorescence switching system triggered electrochemically by Prussian blue with upconversion nanoparticles was proposed. We synthesized a kind of hexagonal monodisperse β-NaYF4:Yb(3+),Er(3+),Tm(3+) upconversion nanoparticle and manipulated the intensity ratio of red emission (at 653 nm) and green emission at (523 and 541 nm) around 2 : 1, in order to match well with the absorption spectrum of Prussian blue. Based on the efficient fluorescence resonance energy transfer and inner-filter effect of the as-synthesized upconversion nanoparticles and Prussian blue, the present fluorescence switching system shows obvious behavior with high fluorescence contrast and good stability. To further extend the application of this system in analysis, sulfite, a kind of important anion in environmental and physiological systems, which could also reduce Prussian blue to Prussian white nanoparticles leading to a decrease of the absorption spectrum, was chosen as the target. And we were able to determine the concentration of sulfite in aqueous solution with a low detection limit and a broad linear relationship. PMID:27102984

  9. Femtosecond laser fluorescence and propagation in very dense potassium vapor.

    PubMed

    Makdisi, Y; Kokaj, J; Afrousheh, K; Nair, R; Mathew, J; Pichler, G

    2013-12-16

    Femtosecond (fs) laser propagation and fluorescence of dense potassium vapor was studied, and the spectral region around the first and the second doublets of the principal series lines of potassium atoms was investigated. In our search we did not observe the conical emission in the far field, although it was previously observed in the case of rubidium. We discuss the possible reason of this unexpected result. The fluorescence spectrum revealed Rb impurity resonance lines in emission due to the collisional redistribution from the K(4p) levels into the Rb(5p) levels. In the forward propagation of 400 nm femtosecond light we observed the molecular band red shifted from potassium second doublet. However, no molecular spectrum was observed when the mode-locked fs laser light was discretely tuned within the wings of the first resonance lines, at 770 nm. PMID:24514609

  10. Optical properties and upconversion fluorescence in Er 3+-doped ZZA glass

    NASA Astrophysics Data System (ADS)

    Zhang, X.; Pita, K.; Buddhudu, S.; Daran, E.; Lam, Y. L.; Liu, X. R.

    2002-08-01

    We report the optical properties and upconversion emissions from the Er 3+ ions in a ZrF 4-based glass system ZrF 4-ZnF 2-AlF 3. Judd-Ofelt intensity parameters ( Ω (t) with t=2,4,6) were obtained by analyzing the room temperature absorption spectrum. Upon 800 nm laser excitation, upconversion fluorescence was observed in blue, green and red regions at both 25 and 300 K. The main mechanism appears to be energy transfer among Er 3+ ions in excited states. The green and red emissions result from a two-step process while the blue one is owing to a three-step energy transfer process.

  11. Efficient green and red fluorescence upconversion in erbium doped new low phonon antimony glasses

    NASA Astrophysics Data System (ADS)

    Som, Tirtha; Karmakar, Basudeb

    2009-02-01

    New K 2O-B 2O 3-Sb 2O 3 (KBS) glass system having low phonon energy (about 600 cm -1) doped with Er 3+ ions has been developed. Infrared reflection spectroscopic (IRRS) studies have been employed to establish its low phonon energy. Ultraviolet-visible-near infrared (UV-vis-NIR) absorption and photoluminescence upconversion properties with special emphasis on the spectrochemistry of the 15K 2O-15B 2O 3-70Sb 2O 3 (mol%) glass have been studied doping with different concentrations (0.1-1.0 wt%) of Er 2O 3. UV-vis-NIR absorption band positions have been justified with quantitative calculation of nephelauxetic parameter and covalent bonding characteristics of the host. NIR to visible upconversion has been investigated by exciting at 798 nm at room temperature. Three upconverted bands originating from the 2H 11/2 → 4I 15/2, 4S 3/2 → 4I 15/2 and 4F 9/2 → 4I 15/2 transitions are found to be centered at 522 (green, very weak), 536 (green, medium) and 645 (red, strong) nm, respectively. These bands have been explained from the evaluation of the absorption, normal (down conversion) fluorescence and excitation spectra. The upconversion processes have been explained by the excited state absorption (ESA), energy transfer (ET), cooperative energy transfer (CET) and cross relaxation (CR) mechanisms involving population of the metastable (storage) energy levels ( 2H 11/2, 4S 3/2 and 4F 9/2) by effects of multiphonon deexcitation and thermal population. It is evident from the IRRS study that the upconversion phenomena are expedited by the low multiphonon relaxation rate in antimony glasses owing to their high intense low phonon energy (602 cm -1) which is very close to that of fluoride glasses (500-600 cm -1). We are the first to report the upconversion fluorescence of Er 3+ ions in KBS antimony glasses.

  12. Hybrid lanthanide nanoparticles with paramagnetic shell coated on upconversion fluorescent nanocrystals.

    PubMed

    Li, Zhengquan; Zhang, Yong; Shuter, Borys; Muhammad Idris, Niagara

    2009-10-20

    Nanoparticles comprising of fluorescent probes and MRI contrast agents are highly desirable for biomedical applications due to their ability to be detected at different modes, optically and magnetically. However, most fluorescent probes in such nanoparticles synthesized so far are down-conversion phosphors such as organic dyes and quantum dots, which are known to display many intrinsic limitations. Here, we report a core-shell hybrid lanthanide nanoparticle consisting of an upconverting lanthanide nanocrystal core and a paramagnetic lanthanide complex shell. These nanoparticles are uniform in size, stable in water, and show both high MR relaxivities and upconversion fluorescence, which may have the potential to serve as a versatile imaging tool for smart detection or diagnosis in future biomedical engineering. PMID:19764797

  13. Quantifying Aflatoxin B1 in peanut oil using fabricating fluorescence probes based on upconversion nanoparticles.

    PubMed

    Sun, Cuicui; Li, Huanhuan; Koidis, Anastasios; Chen, Quansheng

    2016-08-01

    Rare earth doped upconversion nanoparticles convert near-infrared excitation light into visible emission light. Compared to organic fluorophores and semiconducting nanoparticles, upconversion nanoparticles (UCNPs) offer high photochemical stability, sharp emission bandwidths, and large anti-Stokes shifts. Along with the significant light penetration depth and the absence of autofluorescence in biological samples under infrared excitation, these UCNPs have attracted more and more attention on toxin detection and biological labelling. Herein, the fluorescence probe based on UCNPs was developed for quantifying Aflatoxin B1 (AFB1) in peanut oil. Based on a specific immunity format, the detection limit for AFB1 under optimal conditions was obtained as low as 0.2ng·ml(-1), and in the effective detection range 0.2 to 100ng·ml(-1), good relationship between fluorescence intensity and AFB1 concentration was achieved under the linear ratios up to 0.90. Moreover, to check the feasibility of these probes on AFB1 measurements in peanut oil, recovery tests have been carried out. A good accuracy rating (93.8%) was obtained in this study. Results showed that the nanoparticles can be successfully applied for sensing AFB1 in peanut oil. PMID:27124091

  14. Quantifying Aflatoxin B1 in peanut oil using fabricating fluorescence probes based on upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Sun, Cuicui; Li, Huanhuan; Koidis, Anastasios; Chen, Quansheng

    2016-08-01

    Rare earth doped upconversion nanoparticles convert near-infrared excitation light into visible emission light. Compared to organic fluorophores and semiconducting nanoparticles, upconversion nanoparticles (UCNPs) offer high photochemical stability, sharp emission bandwidths, and large anti-Stokes shifts. Along with the significant light penetration depth and the absence of autofluorescence in biological samples under infrared excitation, these UCNPs have attracted more and more attention on toxin detection and biological labelling. Herein, the fluorescence probe based on UCNPs was developed for quantifying Aflatoxin B1 (AFB1) in peanut oil. Based on a specific immunity format, the detection limit for AFB1 under optimal conditions was obtained as low as 0.2 ng·ml- 1, and in the effective detection range 0.2 to 100 ng·ml- 1, good relationship between fluorescence intensity and AFB1 concentration was achieved under the linear ratios up to 0.90. Moreover, to check the feasibility of these probes on AFB1 measurements in peanut oil, recovery tests have been carried out. A good accuracy rating (93.8%) was obtained in this study. Results showed that the nanoparticles can be successfully applied for sensing AFB1 in peanut oil.

  15. Controllable self-assembly of NaREF4 upconversion nanoparticles and their distinctive fluorescence properties

    NASA Astrophysics Data System (ADS)

    Liu, Xiaoxia; Ni, Yaru; Zhu, Cheng; Fang, Liang; Kou, Jiahui; Lu, Chunhua; Xu, Zhongzi

    2016-07-01

    The paper presents the growth of hexagonal NaYF4:Yb3+, Tm3+ nanocrystals with tunable sizes induced by different contents of doped Yb3+ ions (10%–99.5%) using the thermal decomposition method. These nanoparticles, which have different sizes, are then self-assembled at the interface of cyclohexane and ethylene and transferred onto a normal glass slide. It is found that the size of nanoparticles directs their self-assembly. Due to the appropriate size of 40.5 nm, 15% Yb3+ ions doped nanoparticles are able to be self-assembled into an ordered inorganic monolayer membrane with a large area of about 10 × 10 μm2. More importantly, the obvious short-wave (300–500 nm) fluorescence improvement of the ordered 2D self-assembly structure is observed to be relative to disordered nanoparticles, which is because intrinsic absorption and scattering of upconversion nanoparticles leads to the self-loss of fluorescence, especially the short-wave fluorescence inside the disordered structure, and the relative emission of short-wave fluorescence is reduced. The construction of a 2D self-assembly structure can effectively avoid this and improve the radiated short-wave fluorescence, especially UV photons, and is able to direct the design of new types of solid-state optical materials in many fields.

  16. Controllable self-assembly of NaREF4 upconversion nanoparticles and their distinctive fluorescence properties.

    PubMed

    Liu, Xiaoxia; Ni, Yaru; Zhu, Cheng; Fang, Liang; Kou, Jiahui; Lu, Chunhua; Xu, Zhongzi

    2016-07-22

    The paper presents the growth of hexagonal NaYF4:Yb(3+), Tm(3+) nanocrystals with tunable sizes induced by different contents of doped Yb(3+) ions (10%-99.5%) using the thermal decomposition method. These nanoparticles, which have different sizes, are then self-assembled at the interface of cyclohexane and ethylene and transferred onto a normal glass slide. It is found that the size of nanoparticles directs their self-assembly. Due to the appropriate size of 40.5 nm, 15% Yb(3+) ions doped nanoparticles are able to be self-assembled into an ordered inorganic monolayer membrane with a large area of about 10 × 10 μm(2). More importantly, the obvious short-wave (300-500 nm) fluorescence improvement of the ordered 2D self-assembly structure is observed to be relative to disordered nanoparticles, which is because intrinsic absorption and scattering of upconversion nanoparticles leads to the self-loss of fluorescence, especially the short-wave fluorescence inside the disordered structure, and the relative emission of short-wave fluorescence is reduced. The construction of a 2D self-assembly structure can effectively avoid this and improve the radiated short-wave fluorescence, especially UV photons, and is able to direct the design of new types of solid-state optical materials in many fields. PMID:27292186

  17. Upconversion fluorescence metal-organic frameworks thermo-sensitive imprinted polymer for enrichment and sensing protein.

    PubMed

    Guo, Ting; Deng, Qiliang; Fang, Guozhen; Gu, Dahai; Yang, Yukun; Wang, Shuo

    2016-05-15

    A novel fluorescence material with thermo-sensitive for the enrichment and sensing of protein was successfully prepared by combining molecular imprinting technology with upconversion nanoparticles (UCNPs) and metal-organic frameworks (MOFs). Herein, the UCNPs acted as signal reporter for composite materials because of its excellent fluorescence property and chemical stability. MOFs were introduced to molecularly imprinted polymer (MIP) due to its high specific surface area which increases the rate of mass transfer relative to that of traditional bulk MIP. The thermo-sensitive imprinted material which allows for swelling and shrinking with response to temperature changes was prepared by choosing Bovine hemoglobin (BHB) as the template, N-isopropyl acrylamide (NIPAAM) as the temperature-sensitive functional monomer and N,N-methylenebisacrylamide (MBA) as the cross-linker. The recognition characterizations of imprinted material-coated UCNPs/MOFs (UCNPs/MOFs/MIP) were evaluated, and the results showed that the fluorescence intensity of UCNPs/MOFs/MIP reduced gradually with the increase of BHB concentration. The fluorescence material was response to the temperature. The adsorption capacity was as much as 167.6 mg/g at 28°C and 101.2mg/g at 44°C, which was higher than that of traditional MIP. Therefore, this new fluorescence material for enrichment and sensing protein is very promising for future applications. PMID:26722764

  18. 808 nm driven Nd3+-sensitized upconversion nanostructures for photodynamic therapy and simultaneous fluorescence imaging.

    PubMed

    Wang, Dan; Xue, Bin; Kong, Xianggui; Tu, Langping; Liu, Xiaomin; Zhang, Youlin; Chang, Yulei; Luo, Yongshi; Zhao, Huiying; Zhang, Hong

    2015-01-01

    The in vivo biological applications of upconversion nanoparticles (UCNPs) prefer excitation at 700-850 nm, instead of 980 nm, due to the absorption of water. Recent approaches in constructing robust Nd(3+) doped UCNPs with 808 nm excitation properties rely on a thick Nd(3+) sensitized shell. However, for the very important and popular Förster resonance energy transfer (FRET)-based applications, such as photodynamic therapy (PDT) or switchable biosensors, this type of structure has restrictions resulting in a poor energy transfer. In this work, we have designed a NaYF4:Yb/Ho@NaYF4:Nd@NaYF4 core-shell-shell nanostructure. We have proven that this optimal structure balances the robustness of the upconversion emission and the FRET efficiency for FRET-based bioapplications. A proof of the concept was demonstrated for photodynamic therapy and simultaneous fluorescence imaging of HeLa cells triggered by 808 nm light, where low heating and a high PDT efficacy were achieved. PMID:25406514

  19. [The study of up-conversion fluorescence in Er3+:Yb3+ co-doped oxy-fluoride glasses].

    PubMed

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

    2002-06-01

    Er3+:Yb3+ co-doped oxy-fluoride glasses with composition of (50-x) GeO2.PbF2.WO3.(6 + x) CdF2.1.4Yb2O3.0.6Er2O3 (x = 10,20,30) were prepared. Their up-conversion fluorescence characteristics were investigated under excitation of 930 nm diode laser. Three strong fluorescence bands of Er3+ whose central wavelength lie in 543, 550 and 655 nm have been observed. The maximum phonon energy is obtained by measuring anti-stokes Raman shifts of the samples, and the up-conversion mechanism is briefly discussed. The influences of host materials composition on up-conversion efficiency are also discussed adopting the average electronegative difference and the cationic field strength of the host. It is found that relative small average electronegative difference and large cationic field strength of host benefit to energy up-conversion. PMID:12938302

  20. Synthesis of improved upconversion nanoparticles as ultrasensitive fluorescence probe for mycotoxins.

    PubMed

    Chen, Quansheng; Hu, Weiwei; Sun, Cuicui; Li, Huanhuan; Ouyang, Qin

    2016-09-28

    Rare earth-doped upconversion nanoparticles (UCNPs) have promising potentials in biodetection due to their unique frequency upconverting capability and high detection sensitivity. This paper reports an improved UCNPs-based fluorescence probe for dual-sensing of Aflatoxin B1 (AFB1) and Deoxynivalenol (DON) using a magnetism-induced separation and the specific formation of antibody-targets complex. Herein, the improved UCNPs, which were namely NaYF4:Yb/Ho/Gd and NaYF4:Yb/Tm/Gd, were systematically studied based on the optimization of reaction time, temperature and the concentration of dopant ions with simultaneous phase and size controlled NaYF4 nanoparticles; and the targets were detected using the pattern of competitive combination assay. Under an optimized condition, the advanced fluorescent probes revealed stronger fluorescent properties, broader biological applications and better storage stabilities compared to traditional UCNPs-based ones; and ultrasensitive determinations of AFB1 and DON were achieved under a wide sensing range of 0.001-0.1 ng ml(-1) with the limit of detection (LOD) of 0.001 ng ml(-1). Additionally, the applicability of the improved nanosensor for the detection of mycotoxins was also confirmed in adulterated oil samples. PMID:27619096

  1. Upconversion particles coated with molecularly imprinted polymers as fluorescence probe for detection of clenbuterol.

    PubMed

    Tang, Yiwei; Gao, Ziyuan; Wang, Shuo; Gao, Xue; Gao, Jingwen; Ma, Yong; Liu, Xiuying; Li, Jianrong

    2015-09-15

    A novel fluorescence probe based on upconversion particles, YF3:Yb(3+), Er(3+), coating with molecularly imprinted polymers (MIPs@UCPs) has been synthesized for selective recognition of the analyte clenbuterol (CLB), which was characterized by scan electron microscope and X-ray powder diffraction. The fluorescence of the MIPs@UCPs probe is quenched specifically by CLB, and the effect is much stronger than the NIPs@UCPs (non-imprinting polymers, NIPs). Good linear correlation was obtained for CLB over the concentration range of 5.0-100.0 μg L(-1) with a detection limit of 0.12 μg L(-1) (S/N=3). The developed method was also used in the determination of CLB in water and pork samples, and the recoveries ranged from 81.66% to 102.46% were obtained with relative standard deviation of 2.96-4.98% (n=3). The present study provides a new and general tactics to synthesize MIPs@UCPs fluorescence probe with highly selective recognition ability to the CLB and is desirable for application widely in the near future. PMID:25884733

  2. MMP2-sensing up-conversion nanoparticle for fluorescence biosensing in head and neck cancer cells.

    PubMed

    Chan, Yung-Chieh; Chen, Chieh-Wei; Chan, Ming-Hsien; Chang, Yu-Chan; Chang, Wei-Min; Chi, Li-Hsing; Yu, Hui-Ming; Lin, Yuan-Feng; Tsai, Din Ping; Liu, Ru-Shi; Hsiao, Michael

    2016-06-15

    Upconversion nanoparticles (UCNPs) have extensive biological-applications because of their bio-compatibility, tunable optical properties and their ability to be excited by infrared radiation. Matrix metalloproteinases (MMPs) play important roles in extracellular matrix remodelling; they are usually found to significantly increase during cancer progression, and these increases may lead to poor patient survival. In this study, we produced a biosensor that can be recognized by MMP2 and then be unravelled by the attached quencher to emit visible light. We used 3.5-nm gold nanoparticles as a quencher that absorbed emission from UCNPs at a wavelength of 540 nm. The biosensor consists of an upconversion nanoparticle, MMP2-recognized polypeptides and quenchers. Here, UCNPs consisting of NaYF4:Yb(3+)/Er(3+) were prepared via a high temperature co-precipitation method while protecting the oleic acid ligand. To improve the biocompatibility and modify the UCNPs with a polypeptide, they were coated with a silica shell and further conjugated with MMP-recognizing polypeptides. The polypeptide has two ends of featuring carboxylic and thiol groups that react with UCNPs and AuNPs, and the resulting nanoparticles were referred to as UCNP@p-Au. According to the in vitro cell viability analysis, UCNP@p-Au exhibited little toxicity and biocompatibility in head and neck cancer cells. Cellular uptake studies showed that the MMP-based biosensor was activated by 980-nm irradiation to emit green light. This MMP-based biosensor may serve as sensitive and specific molecular fluorescent probe in biological-applications. PMID:26820361

  3. 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

  4. Upconversion fluorescence resonance energy transfer based biosensor for ultrasensitive detection of matrix metalloproteinase-2 in blood.

    PubMed

    Wang, Yuhui; Shen, Pei; Li, Chunya; Wang, Yanying; Liu, Zhihong

    2012-02-01

    Matrix metalloproteinase-2 (MMP-2) is a very important biomarker in blood. Presently, sensitive and selective determination of MMP-2 directly in blood samples is still a challenging job because of the high complexity of the sample matrix. In this work, we reported a new homogeneous biosensor for MMP-2 based on fluorescence resonance energy transfer (FRET) from upconversion phosphors (UCPs) to carbon nanoparticles (CNPs). A polypeptide chain (NH(2)-GHHYYGPLGVRGC-COOH) comprising both the specific MMP-2 substrate domain (PLGVR) and a π-rich motif (HHYY) was designed and linked to the surface of UCPs at the C terminus. The FRET process was initiated by the π-π interaction between the peptide and CNPs, which thus quenched the fluorescence of the donor. Upon the cleavage of the substrate by the protease at the amide bond between Gly and Val, the donor was separated from the acceptor while the π-rich motif stayed on the acceptor. As a result, the fluorescence of the donor was restored. The fluorescence recovery was found to be proportional to the concentration of MMP-2 within the range from 10-500 pg/mL in an aqueous solution. The quantification limit of this sensor was at least 1 order of magnitude lower than that of other reported assays for MMP-2. The sensor was used to determine the MMP-2 level directly in human plasma and whole blood samples with satisfactory results obtained. Owing to the hypersensitivity of the method, clinical samples of only less than 1 μL were needed for accurate quantification, which can be meaningful in MMP-2-related clinical and bioanalytical applications. PMID:22242647

  5. Spatiotemporal control of degenerate multiphoton fluorescence microscopy with delay-tunable femtosecond pulse pairs

    NASA Astrophysics Data System (ADS)

    Das, Dhiman; Bhattacharyya, Indrajit; Goswami, Debabrata

    2016-07-01

    Selective excitation of a particular fluorophore in an ensemble of different fluorophores with overlapping fluorescence spectra is shown to be dependent on the time delay of femtosecond pulse pairs in multiphoton fluorescence microscopy. In particular, the two-photon fluorescence behavior of the Texas Red and DAPI dye pair inside Bovine Pulmonary Artery Endothelial (BPAE) cells depends strongly on the center wavelength of the laser, as well as the delay between two identical laser pulses in one-color femtosecond pulse-pair excitation scheme. Thus, we present a novel design concept using pairs of femtosecond pulses at different central wavelengths and tunable pulse separations for controlling the image contrast between two spatially and spectrally overlapping fluorophores. This femtosecond pulse-pair technique is unique in utilizing the variation of dye dynamics inside biological cells as a contrast mode in microscopy of different fluorophores.

  6. Ultrafast Time-Resolved Emission and Absorption Spectra of meso-Pyridyl Porphyrins upon Soret Band Excitation Studied by Fluorescence Up-Conversion and Transient Absorption Spectroscopy.

    PubMed

    Venkatesh, Yeduru; Venkatesan, M; Ramakrishna, B; Bangal, Prakriti Ranjan

    2016-09-01

    A comprehensive study of ultrafast molecular relaxation processes of isomeric meso-(pyridyl) porphyrins (TpyPs) has been carried out by using femtosecond time-resolved emission and absorption spectroscopic techniques upon pumping at 400 nm, Soret band (B band or S2), in 4:1 dichloromethane (DCM) and tetrahydrofuran (THF) solvent mixture. By combined studies of fluorescence up-conversion, time-correlated single photon counting, and transient absorption spectroscopic techniques, a complete model with different microscopic rate constants associated with elementary processes involved in electronic manifolds has been reported. Besides, a distinct coherent nuclear wave packet motion in Qy state is observed at low-frequency mode, ca. 26 cm(-1) region. Fluorescence up-conversion studies constitute ultrafast time-resolved emission spectra (TRES) over the whole emission range (430-710 nm) starting from S2 state to Qx state via Qy state. Careful analysis of time profiles of up-converted signals at different emission wavelengths helps to reveal detail molecular dynamics. The observed lifetimes are as indicated: A very fast decay component with 80 ± 20 fs observed at ∼435 nm is assigned to the lifetime of S2 (B) state, whereas being a rise component in the region of between 550 and 710 nm emission wavelength pertaining to Qy and Qx states, it is attributed to very fast internal conversion (IC) occurring from B → Qy and B → Qx as well. Two distinct components of Qy emission decay with ∼200-300 fs and ∼1-1.5 ps time constants are due to intramolecular vibrational redistribution (IVR) induced by solute-solvent inelastic collisions and vibrational redistribution induced by solute-solvent elastic collision, respectively. The weighted average of these two decay components is assigned as the characteristic lifetime of Qy, and it ranges between 0.3 and 0.5 ps. An additional ∼20 ± 2 ps rise component is observed in Qx emission, and it is assigned to the formation time of

  7. 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. PMID:27119377

  8. Singlet-based photon upconversion in multichromophore organic thin films (Presentation Recording)

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

    Solid-state energy upconversion has many potential applications, from nonlinear photonics and biophotonics to expanding the spectrum available for solar energy harvest. In organic molecular systems, upconversion is frequently done in solution to mitigate aggregation-induced photoluminescence quenching or to facilitate the diffusion of triplet donors in Triplet-Triplet Annihilation (TTA) systems. Here we demonstrate an organic thin film upconversion system utilizing two-photon absorption (TPA) properties to improve upconversion efficiency. In blend films of Stilbene-420 and Rhodamine 6G we observe a tenfold increase in up-converted fluorescence compared to the fluorescence yield of TPA in pristine stilbene films. While TPA normally has quadratic dependence on excitation intensity, these blend films exhibit sub-quadratic intensity dependence, indicating a combination of linear and quadratic upconversion processes and dramatically improving upconversion efficiency at lower excitation intensities. This improvement in intensity dependence allows for relatively efficient upconversion upon excitation by a nanosecond laser pulse, in contrast to the more expensive femtosecond lasers generally required for excitation in TPA microscopy and similar systems. Time-resolved photoluminescence decay measurements reveal that all excited states involved in this upconversion process are singlets, which indicates the potential for reduced energy losses when compared to TTA upconversion systems and their inherent intersystem-crossing energy losses. We observe emission from both the Rhodamine 6G donor molecules and Stilbene-420 acceptor molecules, indicating the presence of prompt fluorescence from the donor as well as upconversion to the acceptor, and FRET losses from acceptor back to donor. By fitting to a kinetic model we extract rates for these competing processes.

  9. Upconversion-induced delayed fluorescence in multicomponent organic systems: Role of Dexter energy transfer

    NASA Astrophysics Data System (ADS)

    Monguzzi, A.; Tubino, R.; Meinardi, F.

    2008-04-01

    The efficiency of the upconversion-induced delayed fluorescence in a solution of multicomponent organic systems is limited by two steps of the overall process: (i) a triplet-triplet energy transfer between a phosphorescent donor and an emitting acceptor, and (ii) a bimolecular acceptor triplet-triplet annihilation generating acceptor singlet excited states from which the high-energy emission takes place. In this work, the energy transfer process has been investigated in a model system constituted by solutions of Pt(II)octaethylporphyrin, which acts as a donor, and 9,10 diphenylanthracene, which acts as an acceptor. At low temperature, the experimental data have been interpreted in the frame of a pure Dexter energy transfer by using the Perrin approximation. A Dexter radius as large as 26.5 Å has been found. At room temperature, the fast diffusion of the molecules in the solution is no longer negligible, which gives rise to a strong increase in the energy transfer rates.

  10. Nonlinear frequency up-conversion of femtosecond pulses from an erbium fibre laser to the range of 0.8 - 1 {mu}m in silica fibres

    SciTech Connect

    Anashkina, E A; Andrianov, A V; Kim, A V

    2013-03-31

    We consider different mechanisms of nonlinear frequency up-conversion of femtosecond pulses emitted by an erbium fibre system ({lambda} = 1.5 {mu}m) to the range of 0.8 - 1.2 {mu}m in nonlinear silica fibres. The generation efficiency and the centre frequencies of dispersive waves are found as functions of the parameters of the fibre and the input pulse. Simple analytical estimates are obtained for the spectral distribution of the intensity and the frequency shift of a wave packet in the region of normal dispersion during the emission of a high-order soliton under phase matching conditions. In the geometrical optics approximation the frequency shifts are estimated in the interaction of dispersive waves with solitons in various regimes. (extreme light fields and their applications)

  11. Deoxycholate induced tetramer of αA-crystallin and sites of phosphorylation: Fluorescence correlation spectroscopy and femtosecond solvation dynamics

    NASA Astrophysics Data System (ADS)

    Chowdhury, Aritra; Mojumdar, Supratik Sen; Choudhury, Aparajita; Banerjee, Rajat; Das, Kali Pada; Sasmal, Dibyendu Kumar; Bhattacharyya, Kankan

    2012-04-01

    Structure and dynamics of acrylodan labeled αA-crystallin tetramer formed in the presence of a bile salt (sodium deoxycholate, NaDC) has been studied using fluorescence correlation spectroscopy (FCS) and femtosecond up-conversion techniques. Using FCS it is shown that, the diffusion constant (Dt) of the αA-crystallin oligomer (mass ˜800 kDa) increases from ˜35 μm2 s-1 to ˜68 μm2 s-1. This corresponds to a decrease in hydrodynamic radius (rh) from ˜6.9 nm to ˜3.3 nm. This corresponds to about 10-fold decrease in molecular mass to ˜80 kDa and suggests formation of a tetramer (since mass of αA-crystallin monomer is ˜20 kDa). The steady state emission maximum and average solvation time (<τs>) of acrylodan labeled at cysteine 131 position of αA-crystallin is markedly affected on addition of NaDC, while the tryptophan (trp-9) becomes more exposed. This suggests that NaDC binds near the cys-131 and makes the terminal region of αA-crystallin exposed. This may explain the enhanced auto-phosphorylation activity of αA-crystallin near the terminus of the 173 amino acid protein (e.g., at the threonine 13, serine 45, or serine 169 and 172) and suggests that phosphorylation at ser-122 (close to cys-131) is relatively less important.

  12. Materials Integrating Photochemical Upconversion.

    PubMed

    McCusker, Catherine E; Castellano, Felix N

    2016-04-01

    This review features recent experimental work focused on the preparation and characterization of materials that integrate photochemical upconversion derived from sensitized triplet-triplet annihilation, resulting in the conversion of low energy photons to higher energy light, thereby enabling numerous wavelength-shifting applications. Recent topical developments in upconversion include encapsulating or rigidifying fluid solutions to give them mechanical strength, adapting inert host materials to enable upconversion, and using photoactive materials that incorporate the sensitizer and/or the acceptor. The driving force behind translating photochemical upconversion from solution into hard and soft materials is the incorporation of upconversion into devices and other applications. At present, some of the most promising applications of upconversion materials include imaging and fluorescence microscopy, photoelectrochemical devices, water disinfection, and solar cell enhancement. PMID:27573144

  13. Upconversion fluorescence resonance energy transfer biosensor with aromatic polymer nanospheres as the lable-free energy acceptor.

    PubMed

    Wang, Yuhui; Wu, Zhengjun; Liu, Zhihong

    2013-01-01

    We report a new upconversion fluorescence resonance energy transfer (UC-FRET) biosensor using poly-m-phenylenediamine (PMPD) nanospheres as the energy acceptor in this paper. A single-stranded DNA (ssDNA) tagged with a sulfydryl group at the 5'-terminus was covalently linked to poly(ethylenimine) (PEI) functionalized upconversion phosphors (UCPs, the energy donor). Because of the π-rich electronic structure of PMPD, self-assembly of the donor and the acceptor was achieved through the π-π stacking interaction between ssDNA and PMPD. The fluorescence of the donor was quenched by the acceptor in a PMPD-concentration-dependent manner. A maximum quenching degree of 90% was acquired, which was among the highest levels of all previous reports. Upon the formation of double-stranded DNA (dsDNA) between the target DNA and the probe DNA, the energy acceptor was separated from the donor due to the weakened interaction between dsDNA and PMPD. The fluorescence of UCPs was accordingly restored, and a linear response was obtained with the target concentration ranging from 0.1 to 6.0 nM. The limit of detection was calculated as 0.036 nM, which was a highly competitive sensitivity. The sensor also showed high precision, pronounced specificity, and the applicability to complicated sample matrix (human serum). The UCPs-PMPD FRET sensing platform takes advantages of both the optical merits of the upconversion donors and the superquenching ability and good water-solubility of the aromatic polymer nanoparticles. This study will open the opportunity to develop a new class of UC-FRET biosensors. PMID:23186324

  14. Efficient holmium-doped fluoride fiber laser emitting 2.1 µm and blue upconversion fluorescence upon excitation at 2 µm.

    PubMed

    Guhur, A; Jackson, S D

    2010-09-13

    We demonstrate a highly efficient and high power Ho(3+)-doped fluoride glass fiber laser that is resonantly pumped with a Tm(3+)-doped silicate glass fiber laser operating at 2.051 µm. The laser operates at 2080 nm and generated 6.66 W at a slope efficiency of 72%. We observe strong visible upconversion fluorescence centered at a variety of wavelengths including 491 nm which results from three sequential energy transfer upconversion processes; the fluorescence to pump energy ratio for this emission is one the largest reported to date. PMID:20940907

  15. 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

  16. Design of poly(ethylene glycol)/streptavidin coimmobilized upconversion nanophosphors and their application to fluorescence biolabeling.

    PubMed

    Kamimura, Masao; Miyamoto, Daisuke; Saito, Yu; Soga, Kohei; Nagasaki, Yukio

    2008-08-19

    Infrared-to-visible upconversion phosphors (i.e., rare earth ion-doped Y2O3 nanoparticles (UNPs)) were synthesized by the homogeneous precipitation method. Because the charge on the erbium (Er) ion-doped Y2O3 (Y2O3:Er) NP (UNP1) surface is positive under neutral conditions, the UNP1 surface was electrostatically PEGylated using negatively charged poly(ethylene glycol)- b-poly(acrylic acid) (PEG- b-PAAc). The adsorption of PEG- b-PAAc was confirmed by Fourier transform infrared (FT-IR) measurements and thermal gravimetric analysis (TGA). The surface charge of the PEGylated UNP1s (PEG-UNP1s) was effectively shielded by the PEGylation. The dispersion stability of the UNP1s was also significantly improved by the PEGylation. The PEG-UNP1s were dispersed over 1 week under physiological conditions as a result of the steric repulsion between the PEG chains on the UNP1 surface. The upconversion emission spectrum of PEG-UNP1s was observed under physiological conditions and was confirmed by near-infrared excited fluorescence microscope observation. Streptavidin (SA)-installed ytterbium (Yb) and Er ion-codoped Y2O3 (Y2O3:Yb,Er) NPs (UNP2s) were prepared by the coimmobilization of PEG- b-PAAc and streptavidin. The PEG/SA coimmobilized UNP2s (PEG/SA-UNP2s) specifically recognized biotinylated antibodies and emitted strong upconversion luminescence upon near-infrared excitation. The obtained PEG/streptavidin coimmobilized UNPs are promising as high-performance near-infrared biolabeling materials. PMID:18652424

  17. Enhancement of the Upconversion Emission by Visible-to-Near-Infrared Fluorescent Graphene Quantum Dots for miRNA Detection.

    PubMed

    Laurenti, Marco; Paez-Perez, Miguel; Algarra, Manuel; Alonso-Cristobal, Paulino; Lopez-Cabarcos, Enrique; Mendez-Gonzalez, Diego; Rubio-Retama, Jorge

    2016-05-25

    We developed a sensor for the detection of specific microRNA (miRNA) sequences that was based on graphene quantum dots (GQDs) and ssDNA-UCNP@SiO2. The proposed sensor exploits the interaction between the sp(2) carbon atoms of the GQD, mainly π-π stacking, and the DNA nucleobases anchored on the upconversion nanoparticles (UCNPs). This interaction brings the GQD to the surface of the ssDNA-UCNP@SiO2 system, enhancing the upconversion emission. On the other hand, hybridization of the single-stranded DNA (ssDNA) chains anchored on the nanoparticles with their complementary miRNA sequences blocks the capacity of the UCNPs to interact with the GQD through π-π stacking. That gives as result a reduction of the fluorescent enhancement, which is dependent on the concentration of miRNA sequences. This effect was used to create a sensor for miRNA sequences with a detection limit of 10 fM. PMID:27153453

  18. Multi-color femtosecond source for simultaneous excitation of multiple fluorescent proteins in two-photon fluorescence microscopy

    NASA Astrophysics Data System (ADS)

    Wang, Ke; Liu, Tzu-Ming; Wu, Juwell; Horton, Nicholas G.; Lin, Charles P.; Xu, Chris

    2013-02-01

    Simultaneous imaging of cells expressing multiple fluorescent proteins (FPs) is of particular interest in applications such as mapping neural circuits, tracking multiple immune cell populations, etc. To visualize both in vivo and ex vivo tissue morphology and physiology at a cellular level deep within scattering tissues, two-photon fluorescence microscopy (2PM) is a powerful tool that has found wide applications. However, simultaneous imaging of multiple FPs with 2PM is greatly hampered by the lack of proper ultrafast lasers offering multi-color femtosecond pulses, each targeting the two-photon absorption peak of a different FP. Here we demonstrate simultaneous two-photon fluorescence excitation of RFP, YFP, and CFP in human melanoma cells engineered to express a "rainbow" pallet of colors, using a novel fiber-based source with energetic, three-color femtosecond pulses. The three-color pulses, centered at 775 nm, 864 nm and 950 nm, are obtained through second harmonic generation of the 1550 nm pump laser and SHG of the solitons at 1728 nm and 1900 nm generated through soliton self-frequency shift (SSFS) of the pump laser in a large-mode-area (LMA) fiber. The resulting wavelengths are well matched to the two-photon absorption peaks of the three FPs for efficient excitation. Our results demonstrate that multi-color femtosecond pulse generation using SSFS and a turn-key, fiber-based femtosecond laser can fulfill the requirements for simultaneous imaging of multiple FPs in 2PM, opening new opportunities for a wide range of biological applications where non-invasive, high-resolution imaging of multiple fluorescent indicators is required.

  19. Ultraviolet femtosecond Kerr-gated wide-field fluorescence microscopy.

    PubMed

    Blake, Jolie C; Nieto-Pescador, Jesus; Li, Zhengxin; Gundlach, Lars

    2016-06-01

    A Kerr-gated microscope capable of imaging ultraviolet luminescence with femtosecond time resolution has been developed. The system allows the spatial, spectral, and temporal measurement of UV-emitting samples. The instrumentation was optimized for emission collection in the UV, resulting in sub 90 fs time resolution of gated signals. ZnO nanowires were used to demonstrate the performance of the instrument. The evolution of the emission from a single nanowire was tracked via ultrafast transient spectroscopy and through sequential imaging. Transient dynamics were extracted from a region of intense emission on a single ZnO nanowire. This technique is a powerful tool capable of contactless ultrafast measurements of charge carrier dynamics in single nanoparticles. PMID:27244389

  20. Three-color femtosecond source for simultaneous excitation of three fluorescent proteins in two-photon fluorescence microscopy

    PubMed Central

    Wang, Ke; Liu, Tzu-Ming; Wu, Juwell; Horton, Nicholas G.; Lin, Charles P.; Xu, Chris

    2012-01-01

    We demonstrate a fiber-based, three-color femtosecond source for simultaneous imaging of three fluorescent proteins (FPs) using two-photon fluorescence microscopy (2PM). The three excitation wavelengths at 775 nm, 864 nm and 950 nm, are obtained through second harmonic generation (SHG) of the 1550-nm pump laser and the 1728-nm and 1900-nm solitons generated through soliton self-frequency shift (SSFS) in a large-mode-area (LMA) fiber. These energetic pulses are well matched to the two-photon excitation peaks of red, cyan and yellow fluorescent proteins (TagRFPs, TagCFPs, and TagYFPs) for efficient excitation. We demonstrate simultaneous 2PM of human melanoma cells expressing a “rainbow” combination of these three fluorescent proteins. PMID:23024893

  1. Femtosecond lasing from a fluorescent protein in a one dimensional random cavity

    PubMed Central

    Drane, T.M.; Bach, H.; Shapiro, M.; Milner, V.

    2015-01-01

    We present evidence of random lasing from the fluorescent protein DsRed2 embedded in a random one-dimensional cavity. Lasing is achieved when a purified protein solution, placed inside a layered random medium, is optically excited with a femtosecond pump pulse in the direction perpendicular to the plane of random layers. We demonstrate that pumping with ultrashort pulses resulted in a lasing threshold two orders of magnitude lower than that found for nanosecond excitation. PMID:26137388

  2. Femtosecond lasing from a fluorescent protein in a one dimensional random cavity.

    PubMed

    Drane, T M; Bach, H; Shapiro, M; Milner, V

    2015-05-01

    We present evidence of random lasing from the fluorescent protein DsRed2 embedded in a random one-dimensional cavity. Lasing is achieved when a purified protein solution, placed inside a layered random medium, is optically excited with a femtosecond pump pulse in the direction perpendicular to the plane of random layers. We demonstrate that pumping with ultrashort pulses resulted in a lasing threshold two orders of magnitude lower than that found for nanosecond excitation. PMID:26137388

  3. Upconversion Nanoparticles and Monodispersed Magnetic Polystyrene Microsphere Based Fluorescence Immunoassay for the Detection of Sulfaquinoxaline in Animal-Derived Foods.

    PubMed

    Hu, Gaoshuang; Sheng, Wei; Zhang, Yan; Wang, Junping; Wu, Xuening; Wang, Shuo

    2016-05-18

    A novel fluorescence immunoassay for detecting sulfaquinoxaline (SQX) in animal-derived foods was developed using NaYF4:Yb/Tm upconversion nanoparticles (UCNPs) conjugated with antibodies as fluorescence signal probes, and monodisperse magnetic polystyrene microspheres (MMPMs) modified with coating antigen as immune-sensing capture probes for trapping and separating the signal probes. Based on a competitive immunoassay format, the detection limit of the proposed method for detecting SQX was 0.1 μg L(-1) in buffer and 0.5 μg kg(-1) in food samples. The recoveries of SQX in spiked samples ranged from 69.80 to 133.00%, with coefficients of variation of 0.24-25.06%. The extraction procedure was fast, simple, and environmentally friendly, requiring no organic solvents. In particular, milk samples can be analyzed directly after simple dilution. This method has appealing properties, such as sensitive fluorescence response, a simple and fast extraction procedure, and environmental friendliness, and could be applied to detecting SQX in animal-derived foods. PMID:27134048

  4. A novel upconversion, fluorescence resonance energy transfer biosensor (FRET) for sensitive detection of lead ions in human serum.

    PubMed

    Xu, Sai; Xu, Shihan; Zhu, Yongsheng; Xu, Wen; Zhou, Pingwei; Zhou, Chunyang; Dong, Biao; Song, Hongwei

    2014-11-01

    There has been great progress in the development of fluorescence biosensors based on quantum dots (QDs) for the detection of lead ions. However, most methods are detecting lead ions in aqueous solution rather than in human serum due to the influence of protein autofluorescence in serum excited by visible light. Thus, we developed a novel fluorescence resonance energy transfer (FRET) biosensor by choosing the upconversion NaYF4:Yb(3+)/Tm(3+) nanoparticles as the energy donor and the CdTe QDs as the energy acceptor for lead ion detection. It is the first near infrared (NIR)-excited fluorescent probe for determination of lead ions in serum that is capable of overcoming self-luminescence from serum excitation with visible light. The sensor also shows high selectivity, a low detection limit (80 nm) and good linear Stern-Volmer characteristics (R = 0.996), both in the buffer and serum. This biosensor has great potential for versatile applications in lead ion detection in biological and analytical fields. PMID:25184968

  5. Theoretical analysis of fluorescence signals in filamentation of femtosecond laser pulses in nitrogen molecular gas

    SciTech Connect

    Arevalo, E.; Becker, A.

    2005-10-15

    We study numerically and analytically the role of the combined effect of self-focusing, geometrical focusing, and the plasma defocusing in the formation of the fluorescence signal during the filamentation of a Ti:sapphire laser pulse in nitrogen molecular gas. Results of numerical simulations are used to estimate the number of excited ions in the focal volume, which is proportional to the fluorescence signal. We find good agreement between the theoretical results and the experimental data, showing that such data can be used to get further insight into the effective focal volume during filamentation of femtosecond laser pulses in transparent media.

  6. Fine tunable red-green upconversion luminescence from glass ceramic containing 5%Er{sup 3+}:NaYF{sub 4} nanocrystals under excitation of two near infrared femtosecond lasers

    SciTech Connect

    Shang, Xiaoying; Cheng, Wenjing; Zhou, Kan; Ma, Jing; Feng, Donghai; Zhang, Shian; Sun, Zhenrong; Jia, Tianqing; Chen, Ping; Qiu, Jianrong

    2014-08-14

    In this paper, we report fine tunable red-green upconversion luminescence of glass ceramic containing 5%Er{sup 3+}: NaYF{sub 4} nanocrystals excited simultaneously by two near infrared femtosecond lasers. When the glass ceramic was irradiated by 800 nm femtosecond laser, weak red emission centered at 670 nm was detected. Bright red light was observed when the fs laser wavelength was tuned to 1490 nm. However, when excited by the two fs lasers simultaneously, the sample emitted bright green light centered at 550 nm, while the red light kept the same intensity. The dependences of the red and the green light intensities on the two pump lasers are much different, which enables us to manipulate the color emission by adjusting the two pump laser intensities, respectively. We present a theoretical model of Er{sup 3+} ions interacting with two fs laser fields, and explain well the experimental results.

  7. Manipulation of cellular light from green fluorescent protein by a femtosecond laser

    NASA Astrophysics Data System (ADS)

    He, Hao; Li, Shiyang; Wang, Shaoyang; Hu, Minglie; Cao, Youjia; Wang, Chingyue

    2012-10-01

    Green fluorescent protein (GFP) is one of the most widely studied and exploited proteins in biochemistry and cell biology. It emits fluorescence following optical excitation, which is usually provided by a laser. Here, we report that fluorescence from enhanced GFP can be `turned off' by exposing cells to laser light. A short flash of femtosecond laser light is shown to deplete calcium in the endoplasmic reticulum of cells. Calcium-release-activated calcium channels are then activated by stromal interaction molecule 1 (STIM1). The rise in intracellular Ca2+ depolarizes mitochondria and increases the leakage of reactive oxygen species, which then permanently bleach the GFP. This controllable optical scheme for reactive oxygen species generation can also be used to modulate the photoconversion of GFP fluorescence from green to red emission and provide a mechanism for influencing cellular molecular dynamics.

  8. Serial Femtosecond Crystallography and Ultrafast Absorption Spectroscopy of the Photoswitchable Fluorescent Protein IrisFP.

    PubMed

    Colletier, Jacques-Philippe; Sliwa, Michel; Gallat, François-Xavier; Sugahara, Michihiro; Guillon, Virginia; Schirò, Giorgio; Coquelle, Nicolas; Woodhouse, Joyce; Roux, Laure; Gotthard, Guillaume; Royant, Antoine; Uriarte, Lucas Martinez; Ruckebusch, Cyril; Joti, Yasumasa; Byrdin, Martin; Mizohata, Eiichi; Nango, Eriko; Tanaka, Tomoyuki; Tono, Kensuke; Yabashi, Makina; Adam, Virgile; Cammarata, Marco; Schlichting, Ilme; Bourgeois, Dominique; Weik, Martin

    2016-03-01

    Reversibly photoswitchable fluorescent proteins find growing applications in cell biology, yet mechanistic details, in particular on the ultrafast photochemical time scale, remain unknown. We employed time-resolved pump-probe absorption spectroscopy on the reversibly photoswitchable fluorescent protein IrisFP in solution to study photoswitching from the nonfluorescent (off) to the fluorescent (on) state. Evidence is provided for the existence of several intermediate states on the pico- and microsecond time scales that are attributed to chromophore isomerization and proton transfer, respectively. Kinetic modeling favors a sequential mechanism with the existence of two excited state intermediates with lifetimes of 2 and 15 ps, the second of which controls the photoswitching quantum yield. In order to support that IrisFP is suited for time-resolved experiments aiming at a structural characterization of these ps intermediates, we used serial femtosecond crystallography at an X-ray free electron laser and solved the structure of IrisFP in its on state. Sample consumption was minimized by embedding crystals in mineral grease, in which they remain photoswitchable. Our spectroscopic and structural results pave the way for time-resolved serial femtosecond crystallography aiming at characterizing the structure of ultrafast intermediates in reversibly photoswitchable fluorescent proteins. PMID:26866390

  9. Investigation on the structure and upconversion fluorescence of Yb3+/Ho3+ co-doped fluorapatite crystals for potential biomedical applications

    PubMed Central

    Li, Xiyu; Zhu, Jingxian; Man, Zhentao; Ao, Yingfang; Chen, Haifeng

    2014-01-01

    Rare-earth Yb3+ and Ho3+ co-doped fluorapatite (FA:Yb3+/Ho3+) crystals were prepared by hydrothermal synthesis, and their structure, upconversion properties, cell proliferation and imaging were investigated. The synthesized crystals, with a size of 16 by 286 nm, have a hexagonal crystal structure of classic FA and a Ca/Yb/Ho molar ratio of 100/16/2.1. Several reasonable Yb3+/Ho3+ -embedding lattice models along the fluorine channel of the FA crystal cell are proposed for the first time, such as models for (Ca7YbHo©)(PO4)6F2 and (Ca6YbHoNa2)(PO4)6F2. The activated FA:Yb3+/Ho3+ crystals were found to exhibit distinct upconversion fluorescence. The 543- and 654-nm signals in the emission spectra could be assigned, respectively, to the 5F4 (5S2) - 5I8 and 5F5 - 5I8 transitions of holmium via 980-nm near-infrared excitation and the energy transfer of ytterbium. After the surfaces were grafted with hydrophilic dextran, the crystals displayed clear fluorescent cell imaging. Thus, the prepared novel FA:Yb3+/Ho3+ upconversion fluorescent crystals have potential applications in the biomedical field. PMID:24658285

  10. Investigation on the structure and upconversion fluorescence of Yb3+/Ho3+ co-doped fluorapatite crystals for potential biomedical applications

    NASA Astrophysics Data System (ADS)

    Li, Xiyu; Zhu, Jingxian; Man, Zhentao; Ao, Yingfang; Chen, Haifeng

    2014-03-01

    Rare-earth Yb3+ and Ho3+ co-doped fluorapatite (FA:Yb3+/Ho3+) crystals were prepared by hydrothermal synthesis, and their structure, upconversion properties, cell proliferation and imaging were investigated. The synthesized crystals, with a size of 16 by 286 nm, have a hexagonal crystal structure of classic FA and a Ca/Yb/Ho molar ratio of 100/16/2.1. Several reasonable Yb3+/Ho3+ -embedding lattice models along the fluorine channel of the FA crystal cell are proposed for the first time, such as models for (Ca7YbHo©)(PO4)6F2 and (Ca6YbHoNa2)(PO4)6F2. The activated FA:Yb3+/Ho3+ crystals were found to exhibit distinct upconversion fluorescence. The 543- and 654-nm signals in the emission spectra could be assigned, respectively, to the 5F4 (5S2) - 5I8 and 5F5 - 5I8 transitions of holmium via 980-nm near-infrared excitation and the energy transfer of ytterbium. After the surfaces were grafted with hydrophilic dextran, the crystals displayed clear fluorescent cell imaging. Thus, the prepared novel FA:Yb3+/Ho3+ upconversion fluorescent crystals have potential applications in the biomedical field.

  11. Investigation on the structure and upconversion fluorescence of Yb³⁺/Ho³⁺ co-doped fluorapatite crystals for potential biomedical applications.

    PubMed

    Li, Xiyu; Zhu, Jingxian; Man, Zhentao; Ao, Yingfang; Chen, Haifeng

    2014-01-01

    Rare-earth Yb(3+) and Ho(3+) co-doped fluorapatite (FA:Yb(3+)/Ho(3+)) crystals were prepared by hydrothermal synthesis, and their structure, upconversion properties, cell proliferation and imaging were investigated. The synthesized crystals, with a size of 16 by 286 nm, have a hexagonal crystal structure of classic FA and a Ca/Yb/Ho molar ratio of 100/16/2.1. Several reasonable Yb(3+)/Ho(3+) -embedding lattice models along the fluorine channel of the FA crystal cell are proposed for the first time, such as models for (Ca7YbHo©)(PO4)6F2 and (Ca6YbHoNa2)(PO4)6F2. The activated FA:Yb(3+)/Ho(3+) crystals were found to exhibit distinct upconversion fluorescence. The 543- and 654-nm signals in the emission spectra could be assigned, respectively, to the (5)F4 ((5)S2) - (5)I8 and (5)F5 - (5)I8 transitions of holmium via 980-nm near-infrared excitation and the energy transfer of ytterbium. After the surfaces were grafted with hydrophilic dextran, the crystals displayed clear fluorescent cell imaging. Thus, the prepared novel FA:Yb(3+)/Ho(3+) upconversion fluorescent crystals have potential applications in the biomedical field. PMID:24658285

  12. Influence of laser polarization on plasma fluorescence emission during the femtosecond filamentation in air

    NASA Astrophysics Data System (ADS)

    Shi, Yan; Chen, Anmin; Jiang, Yuanfei; Li, Suyu; Jin, Mingxing

    2016-05-01

    The laser polarization state has a great influence on the plasma fluorescence emission during femtoseond filamentation in air. For the spectral lines from N2, in the case of focusing lens with longer focal length (f=100 cm), due to the impact excitation, circular polarization leads to stronger fluorescence emission when the laser energy is higher than the 'energy threshold' (2.0 mJ). As a lens with shorter focal length (f=40 cm) is used, a similar phenomenon can be observed, however, the 'energy threshold' is much lower, which is lower than 0.8 mJ. For the lines from N2+, especially for the 391 nm one, their emission is stronger in the linear polarization state. The mechanism of plasma fluorescence emission during femtosecond filamentation is discussed based on the analysis of these phenomena, which will be helpful to the remote sensing and spectrum analysis.

  13. Valence state change and defect centers induced by infrared femtosecond laser in Yb:YAG crystals

    NASA Astrophysics Data System (ADS)

    Wang, Xinshun; Liu, Yang; Zhao, Panjuan; Guo, Zhongyi; Li, Yan; Qu, Shiliang

    2015-04-01

    The broad band upconversion luminescence in Yb3+:YAG crystal has been observed in experiments under the irradiation of focused infrared femtosecond laser. The dependence of the fluorescence intensity on the pump power shows that the upconversion luminescence is due to simultaneous two-photon absorption process, which indicates that the broad emission bands at 365 and 463 nm could be assigned to the 5d → 4f transitions of Yb2+ ions and the one at 692 nm could be attributed to the electron-hole recombination process on (Yb2+-F+) centers. The absorption spectra of the Yb:YAG crystal samples before and after femtosecond laser irradiation, and after further annealing reveal that permanent valence state change of Yb ions from Yb3+ to Yb2+ and (Yb2+-F+) centers have been induced by infrared femtosecond laser irradiation in Yb3+:YAG crystal.

  14. Upconverting rare-earth nanoparticles with a paramagnetic lanthanide complex shell for upconversion fluorescent and magnetic resonance dual-modality imaging

    NASA Astrophysics Data System (ADS)

    Wang, Yan; Ji, Lei; Zhang, Bingbo; Yin, Peihao; Qiu, Yanyan; Song, Daqian; Zhou, Juying; Li, Qi

    2013-05-01

    Multi-modal imaging based on multifunctional nanoparticles is a promising alternative approach to improve the sensitivity of early cancer diagnosis. In this study, highly upconverting fluorescence and strong relaxivity rare-earth nanoparticles coated with paramagnetic lanthanide complex shells and polyethylene glycol (PEGylated UCNPs@DTPA-Gd3+) are synthesized as dual-modality imaging contrast agents (CAs) for upconverting fluorescent and magnetic resonance dual-modality imaging. PEGylated UCNPs@DTPA-Gd3+ with sizes in the range of 32-86 nm are colloidally stable. They exhibit higher longitudinal relaxivity and transverse relaxivity in water (r1 and r2 values are 7.4 and 27.8 s-1 per mM Gd3+, respectively) than does commercial Gd-DTPA (r1 and r2 values of 3.7 and 4.6 s-1 per mM Gd3+, respectively). They are found to be biocompatible. In vitro cancer cell imaging shows good imaging contrast of PEGylated UCNPs@DTPA-Gd3+. In vivo upconversion fluorescent imaging and T1-weighted MRI show excellent enhancement of both fluorescent and MR signals in the livers of mice administered PEGylated UCNPs@DTPA-Gd3+. All the experimental results indicate that the synthesized PEGylated UCNPs@DTPA-Gd3+ present great potential for biomedical upconversion of fluorescent and magnetic resonance dual-modality imaging applications.

  15. [Upconversion and mid-infrared fluorescence properties of Ho3+/Yb3+ co-doped 50SiO2-50PbF2 glass ceramic].

    PubMed

    Zhang, Xiao-guang; Ren, Guo-zhong; Yang, Huai

    2014-08-01

    In the present paper, the upconversion and mid-infrared fluorescence properties of Ho3+/Yb3+ co-doped 50SiO2- 50PbF2 glass ceramic (GC) were studied. The GC has the following composition (in mol%): 50SiO2-50PbF2-1YbF3-0. 5HoF3. The mixtures of about 10 g were placed in a corundum crucible and melted at 1000 degrees C for 15 min in a SiC electric furnace in air and then poured on a brass plate. The GCs were obtained just by heat treatment at 450 degrees C. The X-ray diffraction pattern of the GC indicates that very small size crystals were precipitated in the precursor glass by heat treatment. The GCs have as high transmittance as glasses. The GCs have higher absorption cross section and narrower absorption peaks compared to the corresponding glasses, indicating that fluoride is doped with Ho ions. The Judd-Ofelt intensity parameters were determined from the absorption spectrum and Judd-Ofelt theory. The omega2 value is 0.17 x 10(-20) cm2 lower than that of fluoride glass ZBLA (2.28 x 10(-20) cm2), because of Ho3+ doping in PbF2 microcrystal. The intense green upconversion light was observed in Ho3+/Yb3+ co-doped 50SiO2-50PbF2 GCs excited by 980 nm laser diode. A main emission band centered around 540 nm (green), and three week emission bands centered around 420 nm(violet), 480 nm (blue), and 650 nm (red) which correspond to the Ho3+ : ((5)F4-->(5)I8) ((5)G-->(5)I8), ((8)K3--(5)I8) and ((5)F5-->(5)I8) transitions, respectively, were simultaneously observed in GCs. Compared with the glass sample, GCs have significantly intension in the green and blue upconversion fluorescence, and not significant change in the red upconversion fluorescence. Those changes are because that Ho ion in GCs locates in lower phonon energy environment than in glasses. Lower phonon energy can make the nonradiative relaxation rate reduce, which improves the green light upconversion efficiency, at the same time reduces the population of the intermediate energy level ((5)I7) of the red light

  16. [Upconversion and mid-infrared fluorescence properties of Ho3+/Yb3+ co-doped 50SiO2-50PbF2 glass ceramic].

    PubMed

    Zhang, Xiao-guang; Ren, Guo-zhong; Yang, Huai

    2014-08-01

    In the present paper, the upconversion and mid-infrared fluorescence properties of Ho3+/Yb3+ co-doped 50SiO2- 50PbF2 glass ceramic (GC) were studied. The GC has the following composition (in mol%): 50SiO2-50PbF2-1YbF3-0. 5HoF3. The mixtures of about 10 g were placed in a corundum crucible and melted at 1000 degrees C for 15 min in a SiC electric furnace in air and then poured on a brass plate. The GCs were obtained just by heat treatment at 450 degrees C. The X-ray diffraction pattern of the GC indicates that very small size crystals were precipitated in the precursor glass by heat treatment. The GCs have as high transmittance as glasses. The GCs have higher absorption cross section and narrower absorption peaks compared to the corresponding glasses, indicating that fluoride is doped with Ho ions. The Judd-Ofelt intensity parameters were determined from the absorption spectrum and Judd-Ofelt theory. The omega2 value is 0.17 x 10(-20) cm2 lower than that of fluoride glass ZBLA (2.28 x 10(-20) cm2), because of Ho3+ doping in PbF2 microcrystal. The intense green upconversion light was observed in Ho3+/Yb3+ co-doped 50SiO2-50PbF2 GCs excited by 980 nm laser diode. A main emission band centered around 540 nm (green), and three week emission bands centered around 420 nm(violet), 480 nm (blue), and 650 nm (red) which correspond to the Ho3+ : ((5)F4-->(5)I8) ((5)G-->(5)I8), ((8)K3--(5)I8) and ((5)F5-->(5)I8) transitions, respectively, were simultaneously observed in GCs. Compared with the glass sample, GCs have significantly intension in the green and blue upconversion fluorescence, and not significant change in the red upconversion fluorescence. Those changes are because that Ho ion in GCs locates in lower phonon energy environment than in glasses. Lower phonon energy can make the nonradiative relaxation rate reduce, which improves the green light upconversion efficiency, at the same time reduces the population of the intermediate energy level ((5)I7) of the red light

  17. Femtosecond Fluorescence Spectra of Tryptophan in Human γ-Crystallin Mutants: Site-Dependent Ultrafast Quenching

    PubMed Central

    Xu, Jianhua; Chen, Jiejin; Toptygin, Dmitri; Tcherkasskaya, Olga; Callis, Patrik; King, Jonathan; Brand, Ludwig; Knutson, Jay R.

    2012-01-01

    The eye lens crystallin proteins are subject to UV irradiation throughout life, and the photochemistry of damage proceeds through the excited state; thus, their tryptophan (Trp) fluorescence lifetimes are physiologically important properties. The time resolved fluorescence spectra of single Trps in human γD- and γS-crystallins have been measured with both an upconversion spectrophotofluorometer on the 300fs to 100ps time scale, and a time correlated single photon counting apparatus on the 100ps to 10ns time scale, respectively. Three Trps in each wild type protein were replaced by phenylalanine, leading to single-Trp mutants: W68-only and W156-only of HγD- and W72-only and W162-only of HγS-crystallin. These proteins exhibit similar ultrafast signatures: positive definite decay associated spectra (DAS) for 50 – 65ps decay constants that indicate dominance of fast, heterogeneous quenching. The quenched population (judged by amplitude) of this DAS differs among mutants. Trps 68, 156 in human γD- and Trp72 in human γS-crystallin are buried, but water can reach amide oxygen and ring HE1 atoms through narrow channels. QM-MM simulations of quenching by electron transfer predict heterogeneous decay times from 50–500 ps that agree with our experimental results. Further analysis of apparent radiative lifetimes allow us to deduce that substantial subpopulations of Trp are fully quenched in even faster (sub-300 fs) processes for several of the mutants. The quenching of Trp fluorescence of human γD- and γS-crystallin may protect them from ambient light induced photo damage. PMID:19919143

  18. Two-photon fluorescence excitation spectroscopy by pulse shaping ultrabroad-bandwidth femtosecond laser pulses

    SciTech Connect

    Xu Bingwei; Coello, Yves; Lozovoy, Vadim V.; Dantus, Marcos

    2010-11-10

    A fast and automated approach to measuring two-photon fluorescence excitation (TPE) spectra of fluorophores with high resolution ({approx}2 nm ) by pulse shaping ultrabroad-bandwidth femtosecond laser pulses is demonstrated. Selective excitation in the range of 675-990 nm was achieved by imposing a series of specially designed phase and amplitude masks on the excitation pulses using a pulse shaper. The method eliminates the need for laser tuning and is, thus, suitable for non-laser-expert use. The TPE spectrum of Fluorescein was compared with independent measurements and the spectra of the pH-sensitive dye 8-hydroxypyrene-1,3,6-trisulfonic acid (HPTS) in acidic and basic environments were measured for the first time using this approach.

  19. Theoretical description of femtosecond fluorescence depletion spectrum of molecules in solution.

    PubMed

    Niu, Kai; Dong, Li-Qing; Cong, Shu-Lin

    2007-09-28

    A theoretical model used for calculating the fluorescence depletion spectrum (FDS) of molecules in liquids induced by femtosecond pump-probe laser pulses is proposed based on the reduced density matrix theory. The FDS intensity is obtained by calculating the stimulated emission of the excited electronic state. As an application of the theoretical model, the FDS of oxazine 750 (OX-750) molecule in acetone solution is calculated. The simulated FDS agrees with the experimental result of Liu et al. [J. Y. Liu et al., J. Phys. Chem. A 107, 10857 (2003)]. The calculated vibrational relaxation rate is 2.5 ps(-1) for the OX-750 molecule. Vibrational population dynamics and wave packet evolution in the excited state are described in detail. The effect of the probe pulse parameter on the FDS is also discussed. PMID:17902916

  20. Femtosecond laser pulse optimization for multiphoton cytometry and control of fluorescence

    NASA Astrophysics Data System (ADS)

    Tkaczyk, Eric Robert

    This body of work encompasses optimization of near infrared femtosecond laser pulses both for enhancement of flow cytometry as well as adaptive pulse shaping to control fluorescence. A two-photon system for in vivo flow cytometry is demonstrated, which allows noninvasive quantification of circulating cell populations in a single live mouse. We monitor fluorescently-labeled red blood cells for more than two weeks, and are also able to noninvasively measure circulation times of two distinct populations of breast cancer cells simultaneously in a single mouse. We build a custom laser excitation source in the form of an extended cavity mode-locked oscillator, which enables superior detection in whole blood or saline of cell lines expressing fluorescent proteins including the green fluorescent protein (GFP), tdTomato and mPlum. A mathematical model explains unique features of the signals. The ability to distinguish different fluorescent species is central to simultaneous measurement of multiple molecular targets in high throughput applications including the multiphoton flow cytometer. We demonstrate that two dyes which are not distinguishable to one-photon measurements can be differentiated and in fact quantified in mixture via phase-shaped two-photon excitation pulses found by a genetic algorithm. We also selectively enhance or suppress two-photon fluorescence of numerous common dyes with tailored pulse shapes. Using a multiplicative (rather than ratiometric) fitness parameter, we are able to control the fluorescence while maintaining a strong signal. With this method, we control the two-photon fluorescence of the blue fluorescent protein (BFP), which is of particular interest in investigations of protein-protein interactions, and has frustrated previous attempts of control. Implementing an acousto-optic interferometer, we use the same experimental setup to measure two-photon excitation cross-sections of dyes and prove that photon-photon interferences are the

  1. Sensitive detection of Porphyromonas gingivalis based on magnetic capture and upconversion fluorescent identification with multifunctional nanospheres.

    PubMed

    Qin, Wei; Zheng, Bin; Yuan, Yuan; Li, Meng; Bai, Yang; Chang, Jin; Wang, Hanjie; Wang, Yonglan

    2016-08-01

    A specific and sensitive detection system was designed to detect Porphyromonas gingivalis, a major periodontal pathogen, in mixed bacterial fluids. This new detection system was based on the use of fluorescent and magnetic encoding nanospheres that were conjugated with monoclonal antibodies specific to P. gingivalis, thus enabling rapid detection of the target bacterium. This strategy simplifies the detection process and improves the sensitivity compared with conventional methods, with a detection limit of approximately 10 colony-forming units (CFU) ml(-1) . This new method shows strong anti-interference ability and excellent selectivity and specificity to detect P. gingivalis in mixed solutions. PMID:27334431

  2. A novel and sensitive fluorescence immunoassay for the detection of fluoroquinolones in animal-derived foods using upconversion nanoparticles as labels.

    PubMed

    Hu, Gaoshuang; Sheng, Wei; Zhang, Yan; Wu, Xuening; Wang, Shuo

    2015-11-01

    A novel fluorescence immunoassay to detect fluoroquinolones in animal-derived foods was developed for the first time by use of upconversion nanoparticles as signal-probe labels. The bioassay system was established by the use of coating-antigen-modified polystyrene particles as immune-sensing probes for separation and anti-norfloxacin monoclonal antibody conjugated with carboxyl-functionalized NaYF4:Yb,Er upconversion nanoparticles which were prepared via a pyrolysis method and a subsequent ligand exchange process as fluorescent-signal probes (emission intensity recorded at 542 nm with excitation at 980 nm). Under optimized conditions, detection of fluoroquinolones was performed easily. The detection limit of this fluorescence immunoassay for norfloxacin, for example, was 10 pg mL(-1), within a wide linear range of 10 pg mL(-1) to 10 ng mL(-1) (R (2)  = 0.9959). For specificity analysis, the data obtained indicate this method could be applied in broad-spectrum detection of fluoroquinolones. The recoveries of norfloxacin-spiked animal-derived foods ranged from 82.37 to 132.22 %, with coefficients of variation of 0.24-25.06 %. The extraction procedure was rapid and simple, especially for milk samples, which could be analyzed directly without any pretreatment. In addition, the results obtained with the method were in good agreement with those obtained with commercial ELISA kits. The fluorescence immunoassay was more sensitive, especially with regard to the detection limit in milk samples (0.01 ng mL(-1) for norfloxacin): it was 50-fold more sensitive than commercial ELISA kits (0.5 ng mL(-1) for norfloxacin). The results show the proposed fluorescence immunoassay was facile, sensitive, and interference free, and is an alternative method for the quantitative detection of fluoroquinolone residues in animal-derived foods. PMID:26337749

  3. Fluorescence-quenching-based homogeneous caspase-3 activity assay using photon upconversion.

    PubMed

    Vuojola, Johanna; Riuttamäki, Terhi; Kulta, Essi; Arppe, Riikka; Soukka, Tero

    2012-05-01

    Caspase proteases are key mediators in apoptosis and thus of great interest in pharmaceutical industry. Enzyme-activity assays are commonly employed in the screening of protease inhibitors that are potential drug candidates. Conventional homogeneous fluorescence-based assays are susceptible to autofluorescence originating from biological material. This background autofluorescence can be eliminated by using upconverting phosphors (UCPs) that emit visible light upon excitation at near-infrared. In the assay energy was transferred from a UCP-donor to a conventional fluorophore acceptor that resided at one end of a caspase-3-specific substrate peptide. Attached to the other end was a quencher molecule that was used to attenuate the acceptor emission through intramolecular energy transfer in an intact peptide. In non-inhibitory conditions the enzyme reaction separated the fluorophore from the quencher and the emission of the fluorophore was recovered. The method was applied for the detection and characterization of a known caspase-3 inhibitor Z-DEVD-FMK, and the assay gave IC(50) values of approximately 13 nM for this inhibitor. We have demonstrated the applicability of UCPs on a fluorescence-quenching-based homogeneous enzyme-activity assay for the detection of caspase-3 inhibitors. The use of near-infrared excitable UCPs enables inexpensive instrumentation and total elimination of autofluorescence, while the use of an internally quenched substrate molecule diminishes the background resulting from radiatively excited acceptor molecules. The reduction of autofluorescence and radiative background result in high signal-to-background ratios (ratios of approximately 100 were obtained). By further utilizing assay miniaturization and signal enhancement in a white microtitration plate, a significant reduction in the reagent consumption can be achieved rendering the assay applicable for high-throughput screening. PMID:22502613

  4. ``Molecular spectrometers'' in the condensed phase: local THz-FIR response from femtosecond fluorescence

    NASA Astrophysics Data System (ADS)

    Ernsting, Nikolaus

    2011-03-01

    We examine dye molecules whose color depends on the polarity of the environment. Following fast optical excitation, their fluorescence band typically red-shifts by 0.5 eV on femtosecond to nanosecond time scales. This ``dynamic Stokes shift'' reflects the joint molecular and environmental reorganisation of the system. Solvation dynamics has been studied for decades in the hope that the dynamics of the environment itself can be extracted. We contribute with two research lines: (1) development of rigid polar solvation probes whose vibrational response is removed from that of water, for example, and (2) fluorescence techniques which measure the dynamic Stokes shifts more precisely. Two results will be shown. The frequency-dependent permittivity ɛ (ω) of water surrounding N-Methyl-6-Quinolone is extracted up to about 100 cm-1 from the time-resolved fluorescence shift R(t). The key consists in an analytical connection ɛ (ω) --> R(t) which is needed for data fitting. Measurements with the cryoprotectant disaccharide trehalose in water serve to establish the method. Its unique feature is locality, i . e . the possibility to measure ɛ (ω) around a supramolecular structure with a covalently connected or embedded probe. THz vibrational activity of a biopolymer is thus measured locally, on the effective length scale for polar solvation, with an embedded molecular probe. For this purpose 2-hydroxy-7-nitro-fluorene was linked into a 13mer duplex opposite an abasic site. The NMR solution structure shows that the fluorene moiety occupies a well-defined position in place of a base-pair. The dynamic Stokes shifts for solution in H2 O and D2 O are quantified. Their difference is much larger than expected for free water, suggesting that only bound water is observed. A weak 26 cm-1 spectral oscillation of the emission band is observed which is not present when the probe is free in solution, and is therefore caused by the supramolecular structure (DNA and hydration water).

  5. Excitation energy dependence of excited states dynamics in all- trans-carotenes determined by femtosecond absorption and fluorescence spectroscopy

    NASA Astrophysics Data System (ADS)

    Kosumi, Daisuke; Yanagi, Kazuhiro; Nishio, Tomohiro; Hashimoto, Hideki; Yoshizawa, Masayuki

    2005-06-01

    Ultrafast relaxation kinetics in β-carotene and lycopene has been investigated by femtosecond absorption and fluorescence spectroscopies using tunable excitation pulses. The transient signals induced by the photoexcitation with larger excess energy have broader bands and longer lifetimes both in the 11Bu+and21Ag- excited states. The excess vibrational energy remains longer than several picoseconds and slows the relaxation kinetics in carotenoids.

  6. Initial photochemistry of bilirubin probed by femtosecond spectroscopy.

    PubMed

    Zietz, Burkhard; Gillbro, Tomas

    2007-10-18

    Bilirubin is a breakdown product from heme catabolism, and reduced excretion of bilirubin can lead to jaundice. Phototherapy is the most common treatment for neonatal jaundice, a condition frequently encountered in newborn infants. Knowledge of the photochemistry of bilirubin, which is dominated by (ultra)fast components, is necessary for the profound understanding of the processes in phototherapy. Here, we report results from femtosecond fluorescence upconversion measurements on bilirubin and half-bilirubin model compounds, as well as pump-probe absorption measurements on bilirubin. A fast component of ca. 120 fs in the multiexponential fluorescence decay, being only visible in the bilirubin molecule, is interpreted as exciton localization within the molecular halves. The slower components of several hundreds of femtoseconds and a few picoseconds, occurring in bilirubin and the half-bilirubin model, are interpreted as relaxation to a (twisted) intermediate, which decays further with ca. 15 ps to the ground state. PMID:17927274

  7. Intense red upconversion fluorescence emission in NIR-excited erbium-ytterbium doped laponite-derived phosphor

    NASA Astrophysics Data System (ADS)

    da Silva, Andréa F.; Moura, Diógenes S.; Gouveia-Neto, Artur S.; Silva, Elias A., Jr.; Bueno, Luciano A.; Costa, Ernande B.; Azevedo, Eduardo N.

    2011-02-01

    In this report the optical properties and energy-transfer frequency upconversion luminescence of Er3+/Yb3+-codoped laponite-derived powders under 975 nm infrared excitation is investigated. The 75%(laponite):25%(PbF2) samples doped with erbium and ytterbium ions, generated high intensity red emission around 660 nm and lower intensity green emission around 525, and 545 nm. The observed emission signals were examined as a function of the excitation power and annealing temperature. The results indicate that energy-transfer, and excited-state absorption are the major upconversion excitation mechanism for the erbium excited-state red emitting level. The precursor glass samples were also heat treated at annealing temperatures of 300 °C, 400 °C, 500 °C, and 600 °C, for a 2h period. The dependence of the visible upconversion luminescence emission upon the annealing temperature indicated the existence of an optimum temperature which leads to the generation of the most intense and spectrally pure red emission signal.

  8. Lasing dynamics study by femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy

    NASA Astrophysics Data System (ADS)

    Wei, Dang; Qing, Liao; Peng-Cheng, Mao; Hong-Bing, Fu; Yu-Xiang, Weng

    2016-05-01

    Femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy (FNOPAS) is a versatile technique with advantages of high sensitivity, broad detection bandwidth, and intrinsic spectrum correction function. These advantages should benefit the study of coherent emission, such as measurement of lasing dynamics. In this letter, the FNOPAS was used to trace the lasing process in Rhodamine 6G (R6G) solution and organic semiconductor nano-wires. High-quality transient emission spectra and lasing dynamic traces were acquired, which demonstrates the applicability of FNOPAS in the study of lasing dynamics. Our work extends the application scope of the FNOPAS technique. Project supported by the National Natural Science Foundation of China (Grant Nos. 20925313 and 21503066), the Innovation Program of Chinese Academy of Sciences (Grant No. KJCX2-YW-W25), the Postdoctoral Project of Hebei University, China, and the Project of Science and Technology Bureau of Baoding City, China (Grant No. 15ZG029).

  9. Two-photon excited fluorescence enhancement with broadband versus tunable femtosecond laser pulse excitation

    NASA Astrophysics Data System (ADS)

    Wang, Chao; Yeh, Alvin T.

    2012-02-01

    The inverse relationship between two-photon excited fluorescence (TPEF) and laser pulse duration suggests that two-photon microscopy (TPM) performance may be improved by decreasing pulse duration. However, for ultrashort pulses of sub-10 femtosecond (fs) in duration, its spectrum contains the effective gain bandwidth of Ti:Sapphire and its central wavelength is no longer tunable. An experimental study was performed to explore this apparent tradeoff between untuned sub-10 fs transform-limited pulse (TLP) and tunable 140 fs pulse for TPEF. Enhancement factors of 1.6, 6.7, and 5.2 are measured for Indo-1, FITC, and TRITC excited by sub-10 fs TLP compared with 140 fs pulse tuned to the two-photon excitation (TPE) maxima at 730 nm, 800 nm, and 840 nm, respectively. Both degenerate (v1=v2) and nondegenerate (v1≠v2) mixing of sub-10 fs TLP spectral components result in its broad second-harmonic (SH) power spectrum and high spectral density, which can effectively compensate for the lack of central wavelength tuning and lead to large overlap with dye TPE spectra for TPEF enhancements. These pulse properties were also exploited for demonstrating its potential applications in multicolor imaging with TPM.

  10. Fluorescence Up-Conversion Studies of [2,2'-Bipyridyl]-3,3'-diol in Octyl-β-d-glucoside and Other Micellar Aggregates.

    PubMed

    Satpathi, Sagar; Gavvala, Krishna; Hazra, Partha

    2015-12-24

    In this present work, excited state double proton transfer dynamics (ESIDPT) of 2,2'-bipyridyl-3,3'-diol (BP(OH)2) molecules has been probed in a nontoxic, biocompatible sugar surfactant assembly, namely, octyl-β-d-glucoside (OBG) micelle with the help of steady state and fluorescence up-conversion techniques. Moreover, the ultrafast double proton transfer dynamics in conventional micelles (SDS, CTAB) and bile salts aggregates have been probed and compared. Interestingly, in all these supramolecular aggregates, the ESIDPT dynamics is found to follow sequential pathway; however, the time-scale of proton transfer dynamics varies from 11 to 30 ps. This difference in proton transfer time scale in different supramolecular aggregates has been explained in terms of accessibility of water molecules in the vicinity of probe. PMID:26613290

  11. ``Smart'' theranostic lanthanide nanoprobes with simultaneous up-conversion fluorescence and tunable T1-T2 magnetic resonance imaging contrast and near-infrared activated photodynamic therapy

    NASA Astrophysics Data System (ADS)

    Zhang, Yan; Das, Gautom Kumar; Vijayaragavan, Vimalan; Xu, Qing Chi; Padmanabhan, Parasuraman; Bhakoo, Kishore K.; Tamil Selvan, Subramanian; Tan, Timothy Thatt Yang

    2014-10-01

    The current work reports a type of ``smart'' lanthanide-based theranostic nanoprobe, NaDyF4:Yb3+/NaGdF4:Yb3+,Er3+, which is able to circumvent the up-converting poisoning effect of Dy3+ ions to give efficient near infrared (980 nm) triggered up-conversion fluorescence, and offers not only excellent dark T2-weighted MR contrast but also tunable bright and T1-weighted MR contrast properties. Due to the efficient up-converted energy transfer from the nanocrystals to chlorin e6 (Ce6) photosensitizers loaded onto the nanocrystals, cytotoxic singlet oxygen was generated and photodynamic therapy was demonstrated. Therefore, the current multifunctional nanocrystals could be potentially useful in various image-guided diagnoses where bright or dark MRI contrast could be selectively tuned to optimize image quality, but also as an efficient and more penetrative near-infrared activated photodynamic therapy agent.The current work reports a type of ``smart'' lanthanide-based theranostic nanoprobe, NaDyF4:Yb3+/NaGdF4:Yb3+,Er3+, which is able to circumvent the up-converting poisoning effect of Dy3+ ions to give efficient near infrared (980 nm) triggered up-conversion fluorescence, and offers not only excellent dark T2-weighted MR contrast but also tunable bright and T1-weighted MR contrast properties. Due to the efficient up-converted energy transfer from the nanocrystals to chlorin e6 (Ce6) photosensitizers loaded onto the nanocrystals, cytotoxic singlet oxygen was generated and photodynamic therapy was demonstrated. Therefore, the current multifunctional nanocrystals could be potentially useful in various image-guided diagnoses where bright or dark MRI contrast could be selectively tuned to optimize image quality, but also as an efficient and more penetrative near-infrared activated photodynamic therapy agent. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr01717j

  12. Upconversion fluorescence and its thermometric sensitivity of Er3+:Yb3+ co-doped SrF2 powders prepared by combustion synthesis

    NASA Astrophysics Data System (ADS)

    Rakov, Nikifor; Maciel, Glauco S.; Xiao, Mufei

    2014-09-01

    Upconversion fluorescence of co-doped Er3+:Yb3+:SrF2 powders prepared by combustion synthesis was investigated under near-infrared ( λ = 980 nm) continuous wave laser excitation. Surface morphology of the samples and structures of the Er3+:Yb3+:SrF2 powders were studied with scanning electronic microscopy, energy dispersive x-ray, and x-ray powder diffraction. The spectrum of the fluorescence contains bands centered at ~410, ~522, ~545 and ~660 nm, corresponding respectively to transitions from upper levels 2H9/2, 2H11/2, 4S3/2 and 4F9/2 to the ground state 4I15/2, which can be identified as 4 f-4 f transitions from Er3+ excited states. In addition, the fluorescence is found sensitive to the temperature, which suggests that an optical temperature sensor would be feasible. The maximum sensitivity of the proposed sensor was found 0.00396 K-1.

  13. [An effect enhancement mechanism of up-conversion luminescence--up-conversion sensitization].

    PubMed

    Meng, C; Meng, G; Song, Z

    2001-04-01

    The research of frequency up-conversion has been developed greatly in recent ten years. In order to achieve its applications, it needs to enhance the up-conversion efficiency further greatly, which is the core problem of up-conversion. Because of the specialty of Yb3+ ion energy level, Yb3+ can greatly enhance up-conversion luminescence of co-doped rare earth ion activator through energy transfer. Meanwhile it may not cause the obvious fluorescence quenching. Thus it is very significance to investigate up-conversion sensitization which Yb3+ ion acts as a sensitizer. It is more important that it is quite urgent to combine up-conversion efficiency and material property to develop up-conversion. This paper reviews the proposing and developing process of up-conversion sensitization. The achievement of up-conversion sensitization field especial the originate fruit in indirect up-conversion sensitization obtained by China are introduce emphatically. PMID:12947606

  14. Highly sensitive optical thermometry based on the upconversion fluorescence from Yb3+/Er3+ codoped La2(WO4)3:Yb3+ ,Er3+ phosphor

    NASA Astrophysics Data System (ADS)

    Yang, Yan-min; Mi, Chao

    2013-12-01

    An optical temperature sensor based on Yb3+ and Er3+ codoped La2(WO4)3 phosphor for using in the high temperature region is discussed on the basis of fluorescence intensity ratio (FIR) method. The dependence of temperature on the upconversion green emission was intensive studied when the temperature increased from 300 K to 550 K under the excitation of 971 nm laser diode. The fluorescence intensity ratio of the two green emissions bands centered at 525 nm, 545 nm changed dramatically with the thermal treatment. By analyzing the experimental data according to the FIR method, the result on the thermometric property of La2(WO4)3:Yb3+, Er3+ was obtained and it shows that the sensitivity of La2(WO4)3:Yb3+, Er3+ reached the maximal value of about 0.0097 K-1 at the temperature of 510 K, even when the temperature was as high as 900 K, the sensitivity could still exceed 0.007 K-1. Results indicate that La2(WO4)3:Yb3+, Er3+ has higher sensitivity for thermometry in high temperature area. Owing to its good thermal stability, low synthesis cost and high sensitivity, La2(WO4)3: Yb3+, Er3+ phosphor has potential application in optical temperature sensing.

  15. Ultraviolet upconversion fluorescence of Er3+ in Yb3+/Er3+-codoped Gd2O3 nanotubes.

    PubMed

    Zheng, Kezhi; Zhao, Dan; Zhang, Daisheng; Liu, Zhenyu; Qin, Weiping

    2011-11-01

    Under 980 nm excitation, room-temperature ultraviolet (UV) upconversion (UC) emissions of Er3+ from the 4G(9/2), 2K(13/2), and 2P(3/2) states were observed in Gd2O3:Yb3+/Er3+ nanotubes, which were synthesized via a simple wet-chemical route at low temperature and ambient pressure followed by a subsequent heat treatment at 800 degrees C. The experimental results exhibited that these UV emissions came from four-photon UC processes. In the Gd2O3:Yb3+/Er3+ nanocrystals, the energy transfers (ETs) from Yb3+ to Er3+ played important roles in populating the high-energy states of Er3+ ions. This material provides a possible candidate for building UV compact solid-state lasers or fiber lasers. PMID:22413290

  16. Fluorescent MoS2 Quantum Dots: Ultrasonic Preparation, Up-Conversion and Down-Conversion Bioimaging, and Photodynamic Therapy.

    PubMed

    Dong, Haifeng; Tang, Songsong; Hao, Yansong; Yu, Haizhu; Dai, Wenhao; Zhao, Guifeng; Cao, Yu; Lu, Huiting; Zhang, Xueji; Ju, Huangxian

    2016-02-10

    Small size molybdenum disulfide (MoS2) quantum dots (QDs) with desired optical properties were controllably synthesized by using tetrabutylammonium-assisted ultrasonication of multilayered MoS2 powder via OH-mediated chain-like Mo-S bond cleavage mode. The tunable up-bottom approach of precise fabrication of MoS2 QDs finally enables detailed experimental investigations of their optical properties. The synthesized MoS2 QDs present good down-conversion photoluminescence behaviors and exhibit remarkable up-conversion photoluminescence for bioimaging. The mechanism of the emerging photoluminescence was investigated. Furthermore, superior (1)O2 production ability of MoS2 QDs to commercial photosensitizer PpIX was demonstrated, which has great potential application for photodynamic therapy. These early affording results of tunable synthesis of MoS2 QDs with desired photo properties can lead to application in fields of biomedical and optoelectronics. PMID:26761391

  17. NIR-responsive silica-coated NaYbF4:Er/Tm/Ho upconversion fluorescent nanoparticles with tunable emission colors and their applications in immunolabeling and fluorescent imaging of cancer cells

    PubMed Central

    Wang, Meng; Mi, Congcong; Zhang, Yixin; Liu, Jinling; Li, Feng; Mao, Chuanbin; Xu, Shukun

    2009-01-01

    NaYbF4: RE upconversion (UC) fluorescent nanoparticles (NPs) were synthesized with variable rare-earth dopants (RE= Er3+, Tm3+, or Ho3+, or a combination of these ions), from rare-earth stearate precursors in a water-ethanol-oleic acid system by using a two-phase solvothermal method. The NPs were shown to emit visible light such as orange, yellow, green, cyan, blue or pink light in response to near infrared (NIR) irradiation, and their emission colors could be simply tuned by changing either the co-dopant concentration or dopant species. The UC NPs were well-dispersed and spherical with an average size of 15~35 nm. They emitted strong UC fluorescence under the 980 nm NIR excitation. The effects of solvothermal reaction time and temperature on nanoparticle size and phase structure as well as UC fluorescence intensity were systematically studied. Water dispersibility was achieved by forming a silica coat on the surface of the UC NPs. After animo-functionalization, the silica-coated UC NPs were chemically conjugated with the rabbit anti-CEA8 antibody and then used as fluorescent biolabels for the immunolabeling and imaging of HeLa cells. The NIR-responsive multicolor visible light emission of these UC NPs will enable potential applications in biolabeling and multiplexed analysis because NIR light can penetrate tissue as deep as several inches and is safe to human body. PMID:20160878

  18. Single and two-photon fluorescence control of Er3+ ions by phase-shaped femtosecond laser pulse

    NASA Astrophysics Data System (ADS)

    Zhang, Shian; Xu, Shuwu; Ding, Jingxin; Lu, Chenhui; Jia, Tianqing; Qiu, Jianrong; Sun, Zhenrong

    2014-01-01

    We experimentally demonstrate the control of the single and two-photon fluorescence (SPF and TPF) in Er3+ ions by shaping the femtosecond laser pulse with a π or square phase modulation. With the low laser intensity (8.4 × 1010 W/cm2), SPF keeps a constant while TPF is effectively suppressed by the two control schemes. With the high laser intensity (1.2 × 1013 W/cm2), both SPF and TPF are simultaneously enhanced or suppressed by the π phase modulation, and SPF is enhanced while TPF is effectively suppressed by the square phase modulation. The up/down-conversion fluorescence enhancement, suppression, or tuning by the optical control method can greatly expand its applications in various related fields.

  19. Femtosecond, two-photon laser-induced-fluorescence imaging of atomic oxygen in an atmospheric-pressure plasma jet

    NASA Astrophysics Data System (ADS)

    Schmidt, Jacob B.; Sands, Brian L.; Kulatilaka, Waruna D.; Roy, Sukesh; Scofield, James; Gord, James R.

    2015-06-01

    Femtosecond, two-photon-absorption laser-induced-fluorescence (fs-TALIF) spectroscopy is employed to measure space- and time-resolved atomic-oxygen distributions in a nanosecond, repetitively pulsed, externally grounded, atmospheric-pressure plasma jet flowing helium with a variable oxygen admixture. The high-peak-intensity, low-average-energy femtosecond pulses result in increased TALIF signal with reduced photolytic inferences. This allows 2D imaging of absolute atomic-oxygen number densities ranging from 5.8   ×   1015 to 2.0   ×   1012cm-3 using a cooled CCD with an external intensifier. Xenon is used for signal and imaging-system calibrations to quantify the atomic-oxygen fluorescence signal. Initial results highlight a transition in discharge morphology from annular to filamentary, corresponding with a change in plasma chemistry from ozone to atomic oxygen production, as the concentration of oxygen in the feed gas is changed at a fixed voltage-pulse-repetition rate. In this configuration, significant concentrations of reactive oxygen species may be remotely generated by sustaining an active discharge beyond the confines of the dielectric capillary, which may benefit applications that require large concentrations of reactive oxygen species such as material processing or biomedical devices.

  20. Dual fluorescence resonance energy transfer assay between tunable upconversion nanoparticles and controlled gold nanoparticles for the simultaneous detection of Pb²⁺ and Hg²⁺.

    PubMed

    Wu, Shijia; Duan, Nuo; Shi, Zhao; Fang, Congcong; Wang, Zhouping

    2014-10-01

    In this work, we presented a novel dual fluorescence resonance energy transfer (FRET) system for the simultaneous detection of Pb(2+) and Hg(2+). This system employed two color upconversion nanoparticles (UCNPs) as the donors, and controlled gold nanoparticles (AuNPs) as the acceptors. The two donor-acceptor pairs were fabricated by hybridizing the aptamers and their corresponding complementary DNA. Thus, the green and red upconversion fluorescence could be quenched because of a good overlap between the UCNPs fluorescence emission and the AuNPs absorption spectrum. In the presence of Pb(2+) and Hg(2+), the aptamers preferred to bind to their corresponding analytes and formed a G-quadruplexes structure for Pb(2+) and the hairpin-like structure for Hg(2+). As a result, the dual FRET was disrupted, and the green and red upconversion fluorescence was restored. Under optimized experimental conditions, the relative fluorescence intensity increased as the metal ion concentrations were increased, allowing for the quantification of Pb(2+) and Hg(2+). The relationships between the fluorescence intensity and plotting logarithms of ion concentrations were linear in the range from 0.1 to 100 nM for Pb(2+) and 0.5 to 500 nM for Hg(2+), and the detection limits of Pb(2+) and Hg(2+) were 50 pM and 150 pM, respectively. As a practical application, the aptasensor was used to monitor Pb(2+) and Hg(2+) levels in naturally contaminated samples and human serum samples. Ultimately, this type of dual FRET could be used to detect other metal ions or contaminants in food safety analysis and environment monitoring. PMID:25059168

  1. Coherent photon interference elimination and spectral correction in femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy

    NASA Astrophysics Data System (ADS)

    Dang, Wei; Mao, Pengcheng; Weng, Yuxiang

    2013-07-01

    We report an improved setup of femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy (FNOPAS) with a 210 fs temporal response. The system employs a Cassegrain objective to collect and focus fluorescence photons, which eliminates the interference from the coherent photons in the fluorescence amplification by temporal separation of the coherent photons and the fluorescence photons. The gain factor of the Cassegrain objective-assisted FNOPAS is characterized as 1.24 × 105 for Rhodamine 6G. Spectral corrections have been performed on the transient fluorescence spectra of Rhodamine 6G and Rhodamine 640 in ethanol by using an intrinsic calibration curve derived from the spectrum of superfluorescence, which is generated from the amplification of the vacuum quantum noise. The validity of spectral correction is illustrated by comparisons of spectral shape and peak wavelength between the corrected transient fluorescence spectra of these two dyes acquired by FNOPAS and their corresponding standard reference spectra collected by the commercial streak camera. The transient fluorescence spectra of the Rhodamine 6G were acquired in an optimized phase match condition, which gives a deviation in the peak wavelength between the retrieved spectrum and the reference spectrum of 1.0 nm, while those of Rhodamine 640 were collected in a non-optimized phase match condition, leading to a deviation in a range of 1.0-3.0 nm. Our results indicate that the improved FNOPAS can be a reliable tool in the measurement of transient fluorescence spectrum for its high temporal resolution and faithfully corrected spectrum.

  2. Single-layer MoS2 nanosheet grafted upconversion nanoparticles for near-infrared fluorescence imaging-guided deep tissue cancer phototherapy.

    PubMed

    Han, Jianyu; Xia, Hongping; Wu, Yafeng; Kong, Shik Nie; Deivasigamani, Amudha; Xu, Rong; Hui, Kam M; Kang, Yuejun

    2016-04-21

    A multifunctional nanostructure is prepared by covalently grafting upconversion nanoparticles (UCNPs) with chitosan functionalized MoS2 (MoS2-CS) and folic acid (FA) and then loading phthalocyanine (ZnPc) on the surface of MoS2, which integrates photodynamic therapy (PDT) with photothermal therapy (PTT) and upconversion luminescence imaging into one system for enhanced antitumor efficiency. PMID:27035265

  3. Two-photon excitation spectrum of light-harvesting complex II and fluorescence upconversion after one- and two-photon excitation of the carotenoids

    SciTech Connect

    Walla, P.J.; Yom, J.; Krueger, B.P.; Fleming, G.R.

    2000-05-18

    The two-photon excitation (TPE) spectrum of light-harvesting complex II (LHC II) has been measured in the spectral region of 1,000--1,600 nm, corresponding to one-photon wavelengths of 500--800 nm. The authors observed a band with an origin at {approximately}2 x 660 nm (ca. 15,100 {+-} 300 cm{sup {minus}1}) and a maximum at {approximately}2 x 600 nm. The line shape and origin of this band strongly suggest that the observed signal is due to the two-photon-allowed S{sub 1} state of the energy-transferring carotenoids (Car ) in LHC II. The authors also report the time dependence of the upconverted chlorophyll (Chl) fluorescence after TPE at the maximum of the observed band. Surprisingly, a fast rise of 250 {+-} 50 fs followed by a multiexponential decay on the picosecond time scale was observed. This result provides strong indication that there is a fast energy transfer even from the dipole-forbidden Car S{sub 1} state to the Chl's. The sub picosecond energy transfer from the Car S{sub 1} state is likely a consequence of the large number of energy-accepting Chls in van der Waals contact with the central Car's in LHC II. They also present upconversion data of the Car S{sub 2}, Chl a, and Chl b fluorescence observed after one-photon excitation into the dipole-allowed Car S{sub 2} state. The lifetime of the Car S{sub 2} state is {approximately}120 {+-} 30 fs. With the observed time constants they are able to calculate quantum yields for the different possible pathways contributing to the overall Car to Chl energy transfer in LHC II.

  4. Hexamodal imaging with porphyrin-phospholipid-coated upconversion nanoparticles.

    PubMed

    Rieffel, James; Chen, Feng; Kim, Jeesu; Chen, Guanying; Shao, Wei; Shao, Shuai; Chitgupi, Upendra; Hernandez, Reinier; Graves, Stephen A; Nickles, Robert J; Prasad, Paras N; Kim, Chulhong; Cai, Weibo; Lovell, Jonathan F

    2015-03-11

    Hexamodal imaging using simple nanoparticles is demonstrated. Porphyrin-phospholipids are used to coat upconversion nanoparticles in order to generate a new biocompatible material. The nanoparticles are characterized in vitro and in vivo for imaging via fluorescence, upconversion, positron emission tomography, computed tomography, Cerenkov luminescence, and photoacoustic tomography. PMID:25640213

  5. Processing window for femtosecond laser microsurgery and fluorescence imaging of an arterial tissue hosted in a microfluidic chip

    NASA Astrophysics Data System (ADS)

    Karimelahi, Samira; Li, Jianzhao; Herman, Peter R.

    2016-02-01

    We study the exposure limitations of femtosecond laser microsurgery and multiphoton imaging in a microfluidic chip environment, assessing damage thresholds at various interfaces as well as interference from bubble formation in the hosting solution. Both heat accumulation and incubation effects from multipulse laser exposures at 1-MHz repetition rate were evaluated. For demonstration, three microsurgery approaches of laser scribing, percussion drilling and trepanning were applied to arterial walls loaded in vitro in a lab-on-a-chip device. We report that deleterious effects from interface damage and microbubble formation can be avoided to offer laser processing windows for damage-free fluorescence imaging and precise microsurgery of live tissue hosted inside small microfluidic chambers.

  6. Single-layer MoS2 nanosheet grafted upconversion nanoparticles for near-infrared fluorescence imaging-guided deep tissue cancer phototherapy

    NASA Astrophysics Data System (ADS)

    Han, Jianyu; Xia, Hongping; Wu, Yafeng; Kong, Shik Nie; Deivasigamani, Amudha; Xu, Rong; Hui, Kam M.; Kang, Yuejun

    2016-04-01

    A multifunctional nanostructure is prepared by covalently grafting upconversion nanoparticles (UCNPs) with chitosan functionalized MoS2 (MoS2-CS) and folic acid (FA) and then loading phthalocyanine (ZnPc) on the surface of MoS2, which integrates photodynamic therapy (PDT) with photothermal therapy (PTT) and upconversion luminescence imaging into one system for enhanced antitumor efficiency.A multifunctional nanostructure is prepared by covalently grafting upconversion nanoparticles (UCNPs) with chitosan functionalized MoS2 (MoS2-CS) and folic acid (FA) and then loading phthalocyanine (ZnPc) on the surface of MoS2, which integrates photodynamic therapy (PDT) with photothermal therapy (PTT) and upconversion luminescence imaging into one system for enhanced antitumor efficiency. Electronic supplementary information (ESI) available: Experimental details and figures. See DOI: 10.1039/c6nr00150e

  7. Plasmonic modulation of the upconversion fluorescence in NaYF4 :Yb/Tm hexaplate nanocrystals using gold nanoparticles or nanoshells.

    PubMed

    Zhang, Hua; Li, Yujing; Ivanov, Ivan A; Qu, Yongquan; Huang, Yu; Duan, Xiangfeng

    2010-04-01

    Automatic upgrade: attachment of gold nanoparticles (NPs) onto upconversion nanocrystals (NCs) results in plasmonic interactions that lead to a significant enhancement of upconversion emission of more than 2.5. Conversely, formation of a gold shell greatly suppresses the NC emission because of considerable scattering of excitation irradiation (see picture; a=NC before seed attachment; b, c=NC with attached Au NPs; c=NC with Au shell; scale bar=50 nm). PMID:20235253

  8. Correlation of femtosecond wave packets and fluorescence interference in a conjugated polymer: Towards the measurement of site homogeneous dephasing

    NASA Astrophysics Data System (ADS)

    Milota, F.; Sperling, J.; Szöcs, V.; Tortschanoff, A.; Kauffmann, H. F.

    2004-05-01

    Probing electronic femtosecond (fs) coherence among segmental sites that are congested by static and dynamic site disorder and subject to structural relaxation is a big, experimental challenge in the study of photophysics of poly(p-phenylenevinylene). In this work, fs-wave-packet fluorescence interferometry experiments are presented that measure macroscopic coherent kernels and their phase-relaxation in the low-temperature, bottom-state regime of the density-of-states below the migrational threshold energy where downhill site-to-site transfer is marginal. By using freely propagating and tunable 70 fs excitation/probing pulses and employing narrow-band spectral filtering of wave packets, fluorescence interferograms with strongly damped beatings can be observed. The coherences formally follow the in-phase superpositions of two site-optical free-induction-decays and originate from distinct pairs of coherent doorway-states, different in energy and space, each of them being targeted, by two discrete quantum-arrival-states 1α and 1β, via independent, isoenergetic 0→1 fluorescence transitions. The coherent transients are explained as site-to-site polarization beatings, caused by the interference of two fluorescence correlation signals. The numerical analysis of the damping regime, based upon second-order perturbational solutions, reveals the lower limit value of homogeneous dephasing in the range from T2≃100 fs to T2≃200 fs depending on the site-excitation energy of the bottom-states. The experiments enable to look into the formation of the relaxed state as a special molecular process of electron-phonon coupling and hence open-up a quite new perspective in the puzzle of multichromophore optical dynamics and structural relaxation in conjugated polymers.

  9. Superior optical nonlinearity of an exceptional fluorescent stilbene dye

    SciTech Connect

    He, Tingchao; Sreejith, Sivaramapanicker; Zhao, Yanli; Gao, Yang; Grimsdale, Andrew C.; Lin, Xiaodong E-mail: hdsun@ntu.edu.sg; Sun, Handong E-mail: hdsun@ntu.edu.sg

    2015-03-16

    Strong multiphoton absorption and harmonic generation in organic fluorescent chromophores are, respectively, significant in many fields of research. However, most of fluorescent chromophores fall short of the full potential due to the absence of the combination of such different nonlinear upconversion behaviors. Here, we demonstrate that an exceptional fluorescent stilbene dye could exhibit efficient two- and three-photon absorption under the excitation of femtosecond pulses in solution phase. Benefiting from its biocompatibility and strong excited state absorption behavior, in vitro two-photon bioimaging and superior optical limiting have been exploited, respectively. Simultaneously, the chromophore could generate efficient three-photon excited fluorescence and third-harmonic generation (THG) when dispersed into PMMA film, circumventing the limitations of classical fluorescent chromophores. Such chromophore may find application in the production of coherent light sources of higher photon energy. Moreover, the combination of three-photon excited fluorescence and THG can be used in tandem to provide complementary information in biomedical studies.

  10. Valence state change and defect centers induced by infrared femtosecond laser in Yb:YAG crystals

    SciTech Connect

    Wang, Xinshun Liu, Yang; Zhao, Panjuan; Guo, Zhongyi; Li, Yan; Qu, Shiliang

    2015-04-21

    The broad band upconversion luminescence in Yb{sup 3+}:YAG crystal has been observed in experiments under the irradiation of focused infrared femtosecond laser. The dependence of the fluorescence intensity on the pump power shows that the upconversion luminescence is due to simultaneous two-photon absorption process, which indicates that the broad emission bands at 365 and 463 nm could be assigned to the 5d → 4f transitions of Yb{sup 2+} ions and the one at 692 nm could be attributed to the electron-hole recombination process on (Yb{sup 2+}-F{sup +}) centers. The absorption spectra of the Yb:YAG crystal samples before and after femtosecond laser irradiation, and after further annealing reveal that permanent valence state change of Yb ions from Yb{sup 3+} to Yb{sup 2+} and (Yb{sup 2+}-F{sup +}) centers have been induced by infrared femtosecond laser irradiation in Yb{sup 3+}:YAG crystal.

  11. Photolytic-interference-free, femtosecond, two-photon laser-induced fluorescence imaging of atomic oxygen in flames

    NASA Astrophysics Data System (ADS)

    Kulatilaka, Waruna D.; Roy, Sukesh; Jiang, Naibo; Gord, James R.

    2016-02-01

    Ultrashort-pulse lasers are well suited for nonlinear diagnostic techniques such as two-photon laser-induced fluorescence (TPLIF) because the signals generated scale as the laser intensity squared. Furthermore, the broad spectral bandwidths associated with nearly Fourier-transform-limited ultrashort pulses effectively contribute to efficient nonlinear excitation by coupling through a large number of in-phase photon pairs, thereby producing strong fluorescence signals. Additionally, femtosecond (fs)-duration amplified laser systems typically operate at 1-10 kHz repetition rates, enabling high-repetition-rate imaging in dynamic environments. In previous experiments, we have demonstrated utilization of fs pulses for kilohertz (kHz)-rate, interference-free imaging of atomic hydrogen (H) in flames. In the present study, we investigate the utilization of fs-duration pulses to photolytic-interference-free TPLIF imaging of atomic oxygen (O). In TPLIF of O, photodissociation of vibrationally excited carbon dioxide (CO2) is known to be the prominent interference that produces additional O atoms in the medium. We have found that through the use of fs excitation, such interferences can be virtually eliminated in premixed laminar methane flames, which paves the way for two-dimensional imaging of O at kHz data rates. Such measurements can provide critical data for validating complex, multidimensional turbulent-combustion models as well as for investigating flame dynamics in practical combustion devices.

  12. Blue upconversion thulium laser

    SciTech Connect

    Nguyen, D.C.; Faulkner, G.E.; Weber, M.E.; Dulick, M.

    1990-01-01

    Upconversion has been an active area of research for at least two decades, mainly because of its wide ranging applications from infrared quantum counters, visible-emitting phosphors, to upconversion lasers. The upconversion lasers have recently become attractive with the advent of semiconductor laser diodes as the pump source. In an upconversion laser, the laser active ion is excited by internal upconversion of near-ir or red light via multiphoton excitation or cooperative processes and emits anti-Stokes visible light. Since the laser diode output wavelength can be composition turned to match the upconversion laser ion absorption lines, a substantial fraction of the ions can be driven into higher energy levels, thus enhancing the upconversion process. These upconversion solid-state lasers offer a potentially simple and compact source of visible coherent light with semiconductor laser diode excitation. We recently reported a novel upconversion thulium laser that emits blue light at 77 K. In this paper additional data on this 77 K upconversion laser as well as preliminary results on the room temperature upconversion laser are presented. In these demonstrations, dye lasers were used instead of diode lasers because they were more readily available than high power semiconductor laser diodes and their wavelengths could be adjusted easily. 14 refs., 5 figs., 1 tab.

  13. Imaging electronic trap states in perovskite thin films with combined fluorescence and femtosecond transient absorption microscopy

    DOE PAGESBeta

    Xiao, Kai; Ma, Ying -Zhong; Simpson, Mary Jane; Doughty, Benjamin; Yang, Bin

    2016-04-22

    Charge carrier trapping degrades the performance of organometallic halide perovskite solar cells. To characterize the locations of electronic trap states in a heterogeneous photoactive layer, a spatially resolved approach is essential. Here, we report a comparative study on methylammonium lead tri-iodide perovskite thin films subject to different thermal annealing times using a combined photoluminescence (PL) and femtosecond transient absorption microscopy (TAM) approach to spatially map trap states. This approach coregisters the initially populated electronic excited states with the regions that recombine radiatively. Although the TAM images are relatively homogeneous for both samples, the corresponding PL images are highly structured. Themore » remarkable variation in the PL intensities as compared to transient absorption signal amplitude suggests spatially dependent PL quantum efficiency, indicative of trapping events. Furthermore, detailed analysis enables identification of two trapping regimes: a densely packed trapping region and a sparse trapping area that appear as unique spatial features in scaled PL maps.« less

  14. Imaging Electronic Trap States in Perovskite Thin Films with Combined Fluorescence and Femtosecond Transient Absorption Microscopy.

    PubMed

    Simpson, Mary Jane; Doughty, Benjamin; Yang, Bin; Xiao, Kai; Ma, Ying-Zhong

    2016-05-01

    Charge carrier trapping degrades the performance of organometallic halide perovskite solar cells. To characterize the locations of electronic trap states in a heterogeneous photoactive layer, a spatially resolved approach is essential. Here, we report a comparative study on methylammonium lead tri-iodide perovskite thin films subject to different thermal annealing times using a combined photoluminescence (PL) and femtosecond transient absorption microscopy (TAM) approach to spatially map trap states. This approach coregisters the initially populated electronic excited states with the regions that recombine radiatively. Although the TAM images are relatively homogeneous for both samples, the corresponding PL images are highly structured. The remarkable variation in the PL intensities as compared to transient absorption signal amplitude suggests spatially dependent PL quantum efficiency, indicative of trapping events. Detailed analysis enables identification of two trapping regimes: a densely packed trapping region and a sparse trapping area that appear as unique spatial features in scaled PL maps. PMID:27103096

  15. Femtosecond single optical fiber tweezers enabled two-photon fluorescence excitation of trapped microscopic objects

    NASA Astrophysics Data System (ADS)

    Mishra, Yogeshwar N.; Pinto, Mervyn; Ingle, Ninad; Mohanty, Samarendra K.

    2011-03-01

    Analysis of trapped microscopic objects using fluorescence and Raman spectroscopy is gaining considerable interest. We report on the development of single fiber femto second optical tweezers and its use in two-photon fluorescence (TPF) excitation of trapped fluorescent particles. Trapping of the floating objects led to stable fluorescence emission intensity over a long period of time, suitable for spectroscopic measurements. Trapping depth of few cm was achieved inside colloidal sample with TPF from the trapped particle being visible to the naked eye. Furthermore, the fiber optic trapping was so stable that the trapped particle could be moved in 3D even by holding the fiber in hand and slow maneuvering of the same. Owing to the propagation distance of the Bessel-like beam emerging from the axicon-fiber tip, a relatively longer streak of fluorescence was observed along the microsphere length. The cone angle of axicon was engineered so as to provide better trapping stability and high axial confinement of TPF. The theoretical simulation of fiber optical microbeam profiles emerging from the axicon tip and trapping force estimations was found to be in good agreement with the experimentally observed stiffness and TPF patterns. Apart from miniaturization capability into lab-on- a-chip micro-fluidic devices, the proposed non-invasive micro axicon tipped optical fiber can be used in multifunctional mode for in-depth trapping, rotation, sorting and ablation as well as for two-photon fluorescence excitation of motile sample which will revolutionize biophysics and research in material science.

  16. Remarkable enhancement of upconversion fluorescence and confocal imaging of PMMA Opal/NaYF(4):Yb(3+), Tm(3+)/Er(3+) nanocrystals.

    PubMed

    Yin, Ze; Zhu, Yongsheng; Xu, Wen; Wang, Jing; Xu, Sai; Dong, Biao; Xu, Lin; Zhang, Shuang; Song, Hongwei

    2013-05-01

    Novel PMMA opal photonic crystal/NaYF(4):Yb(3+), Tm(3+)/Er(3+) nanocrystal composites were fabricated and tremendous improvement in upconversion luminescence (UCL) was observed under infrared 980 nm excitation. They were also explored to improve brightness of cell images. PMID:23539518

  17. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures

    NASA Astrophysics Data System (ADS)

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y.

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism.

  18. Integrated femtosecond stimulated Raman scattering and two-photon fluorescence imaging of subcellular lipid and vesicular structures.

    PubMed

    Li, Xuesong; Lam, Wen Jiun; Cao, Zhe; Hao, Yan; Sun, Qiqi; He, Sicong; Mak, Ho Yi; Qu, Jianan Y

    2015-11-01

    The primary goal of this study is to demonstrate that stimulated Raman scattering (SRS) as a new imaging modality can be integrated into a femtosecond (fs) nonlinear optical (NLO) microscope system. The fs sources of high pulse peak power are routinely used in multimodal nonlinear microscopy to enable efficient excitation of multiple NLO signals. However, with fs excitations, the SRS imaging of subcellular lipid and vesicular structures encounters significant interference from proteins due to poor spectral resolution and a lack of chemical specificity, respectively. We developed a unique NLO microscope of fs excitation that enables rapid acquisition of SRS and multiple two-photon excited fluorescence (TPEF) signals. In the in vivo imaging of transgenic C. elegans animals, we discovered that by cross-filtering false positive lipid signals based on the TPEF signals from tryptophan-bearing endogenous proteins and lysosome-related organelles, the imaging system produced highly accurate assignment of SRS signals to lipid. Furthermore, we demonstrated that the multimodal NLO microscope system could sequentially image lipid structure/content and organelles, such as mitochondria, lysosomes, and the endoplasmic reticulum, which are intricately linked to lipid metabolism. PMID:26580697

  19. Multi-channel lock-in amplifier assisted femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy with efficient rejection of superfluorescence background

    SciTech Connect

    Mao, Pengcheng; Wang, Zhuan; Dang, Wei; Weng, Yuxiang

    2015-12-15

    Superfluorescence appears as an intense background in femtosecond time-resolved fluorescence noncollinear optical parametric amplification spectroscopy, which severely interferes the reliable acquisition of the time-resolved fluorescence spectra especially for an optically dilute sample. Superfluorescence originates from the optical amplification of the vacuum quantum noise, which would be inevitably concomitant with the amplified fluorescence photons during the optical parametric amplification process. Here, we report the development of a femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectrometer assisted with a 32-channel lock-in amplifier for efficient rejection of the superfluorescence background. With this spectrometer, the superfluorescence background signal can be significantly reduced to 1/300–1/100 when the seeding fluorescence is modulated. An integrated 32-bundle optical fiber is used as a linear array light receiver connected to 32 photodiodes in one-to-one mode, and the photodiodes are further coupled to a home-built 32-channel synchronous digital lock-in amplifier. As an implementation, time-resolved fluorescence spectra for rhodamine 6G dye in ethanol solution at an optically dilute concentration of 10{sup −5}M excited at 510 nm with an excitation intensity of 70 nJ/pulse have been successfully recorded, and the detection limit at a pump intensity of 60 μJ/pulse was determined as about 13 photons/pulse. Concentration dependent redshift starting at 30 ps after the excitation in time-resolved fluorescence spectra of this dye has also been observed, which can be attributed to the formation of the excimer at a higher concentration, while the blueshift in the earlier time within 10 ps is attributed to the solvation process.

  20. Multi-channel lock-in amplifier assisted femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy with efficient rejection of superfluorescence background

    NASA Astrophysics Data System (ADS)

    Mao, Pengcheng; Wang, Zhuan; Dang, Wei; Weng, Yuxiang

    2015-12-01

    Superfluorescence appears as an intense background in femtosecond time-resolved fluorescence noncollinear optical parametric amplification spectroscopy, which severely interferes the reliable acquisition of the time-resolved fluorescence spectra especially for an optically dilute sample. Superfluorescence originates from the optical amplification of the vacuum quantum noise, which would be inevitably concomitant with the amplified fluorescence photons during the optical parametric amplification process. Here, we report the development of a femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectrometer assisted with a 32-channel lock-in amplifier for efficient rejection of the superfluorescence background. With this spectrometer, the superfluorescence background signal can be significantly reduced to 1/300-1/100 when the seeding fluorescence is modulated. An integrated 32-bundle optical fiber is used as a linear array light receiver connected to 32 photodiodes in one-to-one mode, and the photodiodes are further coupled to a home-built 32-channel synchronous digital lock-in amplifier. As an implementation, time-resolved fluorescence spectra for rhodamine 6G dye in ethanol solution at an optically dilute concentration of 10-5M excited at 510 nm with an excitation intensity of 70 nJ/pulse have been successfully recorded, and the detection limit at a pump intensity of 60 μJ/pulse was determined as about 13 photons/pulse. Concentration dependent redshift starting at 30 ps after the excitation in time-resolved fluorescence spectra of this dye has also been observed, which can be attributed to the formation of the excimer at a higher concentration, while the blueshift in the earlier time within 10 ps is attributed to the solvation process.

  1. Multi-channel lock-in amplifier assisted femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectroscopy with efficient rejection of superfluorescence background.

    PubMed

    Mao, Pengcheng; Wang, Zhuan; Dang, Wei; Weng, Yuxiang

    2015-12-01

    Superfluorescence appears as an intense background in femtosecond time-resolved fluorescence noncollinear optical parametric amplification spectroscopy, which severely interferes the reliable acquisition of the time-resolved fluorescence spectra especially for an optically dilute sample. Superfluorescence originates from the optical amplification of the vacuum quantum noise, which would be inevitably concomitant with the amplified fluorescence photons during the optical parametric amplification process. Here, we report the development of a femtosecond time-resolved fluorescence non-collinear optical parametric amplification spectrometer assisted with a 32-channel lock-in amplifier for efficient rejection of the superfluorescence background. With this spectrometer, the superfluorescence background signal can be significantly reduced to 1/300-1/100 when the seeding fluorescence is modulated. An integrated 32-bundle optical fiber is used as a linear array light receiver connected to 32 photodiodes in one-to-one mode, and the photodiodes are further coupled to a home-built 32-channel synchronous digital lock-in amplifier. As an implementation, time-resolved fluorescence spectra for rhodamine 6G dye in ethanol solution at an optically dilute concentration of 10(-5)M excited at 510 nm with an excitation intensity of 70 nJ/pulse have been successfully recorded, and the detection limit at a pump intensity of 60 μJ/pulse was determined as about 13 photons/pulse. Concentration dependent redshift starting at 30 ps after the excitation in time-resolved fluorescence spectra of this dye has also been observed, which can be attributed to the formation of the excimer at a higher concentration, while the blueshift in the earlier time within 10 ps is attributed to the solvation process. PMID:26724012

  2. Upconversion Spectrophotofluorometry

    PubMed Central

    Biesso, Arianna; Xu, Jianhua; Knutson, Jay R.

    2014-01-01

    As the other chapters attest, sensitivity of fluorescent molecules to their local environment has created powerful tools in the study of molecular biology, particularly in the study of protein, DNA, and lipid dynamics. Surprisingly, even events faster than the nanosecond lifetimes of fluorophores are important in protein function, and in particular, events lasting just a few ps reflect on water motion and the coupled dynamics of proteins. These ultrafast phenomena can best be studied by using the same laser that excites fluorescence to also “strobe” the emission, providing sub-picosecond time slices of the action. We explain the strobing “upconversion” technique and some limits on its execution. PMID:24108631

  3. Plasmon-Enhanced Upconversion.

    PubMed

    Wu, Di M; García-Etxarri, Aitzol; Salleo, Alberto; Dionne, Jennifer A

    2014-11-20

    Upconversion, the conversion of photons from lower to higher energies, is a process that promises applications ranging from high-efficiency photovoltaic and photocatalytic cells to background-free bioimaging and therapeutic probes. Existing upconverting materials, however, remain too inefficient for viable implementation. In this Perspective, we describe the significant improvements in upconversion efficiency that can be achieved using plasmon resonances. As collective oscillations of free electrons, plasmon resonances can be used to enhance both the incident electromagnetic field intensity and the radiative emission rates. To date, this approach has shown upconversion enhancements up to 450×. We discuss both theoretical underpinnings and experimental demonstrations of plasmon-enhanced upconversion, examining the roles of upconverter quantum yield, plasmonic geometry, and plasmon spectral overlap. We also discuss nonoptical consequences of including metal nanostructures near upconverting emitters. The rapidly expanding field of plasmon-enhanced upconversion provides novel fundamental insight into nanoscale light-matter interactions while improving prospects for technological relevance. PMID:26276488

  4. Synthesis of NIR-Responsive NaYF₄:Yb,Er Upconversion Fluorescent Nanoparticles Using an Optimized Solvothermal Method and Their Applications in Enhanced Development of Latent Fingerprints on Various Smooth Substrates.

    PubMed

    Wang, Meng; Zhu, Ye; Mao, Chuanbin

    2015-06-30

    Fingerprints at crime scenes are usually latent. The powder-dusting method is the most commonly used procedure for developing latent fingerprints in forensic science. However, the traditional powder-dusting method has characteristics of low sensitivity, low contrast, high background noise, and high autofluorescence interference. To overcome the drawbacks faced by the traditional method, we first optimized an oleic acid-based solvothermal approach for the synthesis of NaYF4:Yb,Er fluorescent upconversion nanoparticles (UCNPs) with the highest possible fluorescence intensity under near-infrared (NIR) irradiation. To optimize the synthesis, we studied the effects of the reaction time, reaction temperature, and volume of oleic acid on the size, phase composition, and UC fluorescence intensity of the UCNPs. We then used the resultant UCNPs to fluorescently label the fingerprints on various smooth substrates to improve the development of latent fingerprints because the UCNPs could undergo excitation under 980 nm NIR light to emit visible light. Latent fingerprints on three major types of smooth substrates were studied, including those with a single background color (transparent glass, white ceramic tiles, and black marbles), with multiple background colors (marbles with different complex surface patterns) and with strong background autofluorescence (note papers, Chinese paper money, and plastic plates). Compared with fingerprint development using traditional powders such as bronze powder, magnetic powder, and green fluorescent powder, our development procedure using UCNPs is facile and exhibits very high sensitivity, high contrast, low background interference, and low autofluorescence interference. This work shows that UCNPs synthesized under optimized conditions are a versatile fluorescent label for the facile development of fingerprints and can find their practical applications in forensic sciences. PMID:26089129

  5. [Direct upconversion sensitization luminescence of Tm(0.1)Yb(10.9): oxyfluoride glass].

    PubMed

    Chen, X B; Sawanobori, N; Song, Z F

    2001-12-01

    This paper studied the direct upconversion sensitization luminescence of Tm(0.1)Yb(10.9): oxyfluoride glass pumped by 966 nm diode laser. We found that there are strong 474 nm three-photon upconversion fluorescence of 1G4-->3H6 transition. As well as there are weak 362, 452 and 650 nm three-photon upconversion fluorescence of 1D2-->3H6, 1D2-->3F4, 1G4-->3F4 and 681 nm two-photon upconversion fluorescence of 3F3-->3H6 transitions respectively. Their upconversion mechanism has been analyzed and discussed simply. PMID:12958885

  6. Imaging of the expansion of femtosecond-laser-produced silicon plasma atoms by off-resonant planar laser-induced fluorescence.

    PubMed

    Samek, Ota; Leis, Franz; Margetic, Vanja; Malina, Radomir; Niemax, Kay; Hergenröder, Roland

    2003-10-20

    Planar laser-induced fluorescence measurements were used to investigate the expansion dynamics of a femtosecond laser-induced plasma. Temporally and spatially resolved measurements were performed to monitor the atoms that were ablated from a silicon target. A dye laser (lambda = 288.16 nm) was used to excite fluorescence signals. The radiation of an off-resonant transition (Si 390.55 nm) was observed at different distances from the target surface. This allowed easy detection of the ablated Si atoms without problems caused by scattered laser light. Abel inversion was applied to obtain the radial distribution of the Si atoms. The atom distribution in the plasma shows some peculiarities, depending on the crater depth. PMID:14594057

  7. Ultrafast unequilibrated charge transfer: A new channel in the quenching of fluorescent biological probes

    NASA Astrophysics Data System (ADS)

    Wan, Chaozhi; Xia, Tianbing; Becker, Hans-Christian; Zewail, Ahmed H.

    2005-08-01

    The dynamics of two biological fluorescent probes, 2-aminopurine (Ap) and daunomycin, were studied using both femtosecond transient absorption and fluorescence upconversion techniques. Various Ap-containing structures were investigated in solution: free Ap, non-covalently bonded (with guanine, adenine, and tryptophan) and covalently bonded in DNA constructs (with guanine, 7-deazaguanine, and adenine). The distinct difference of transient absorption and fluorescence dynamics on the ultrafast time scale, and their dependence on free energy change (Δ G), and the abrupt decrease of the initial fluorescence intensity suggest the efficient depopulation by charge transfer from the unequilibrated hot molecules. We provide a model for this possibly general mechanism and obtain the rate constants for charge separation, vibrational relaxation, and charge recombination.

  8. 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

  9. Multiple temperature effects on up-conversion fluorescences of Er{sup 3+}-Y b{sup 3+}-Mo{sup 6+} codoped TiO{sub 2} and high thermal sensitivity

    SciTech Connect

    Cao, B. S.; Wu, J. L.; Wang, X. H.; He, Y. Y.; Feng, Z. Q.; Dong, B. E-mail: bscao@dlnu.edu.cn; Rino, L.

    2015-08-15

    We report multiple temperature effects on green and red up-conversion emissions in Er{sup 3+}-Y b{sup 3+}-Mo{sup 6+} codoped TiO{sub 2} phosphors. With increasing temperature, the decrease of the red emission from {sup 4}F{sub 9/2}→{sup 4}I{sub 15/2}, the increase of green emission from {sup 2}H{sub 11/2}→{sup 4}I{sub 15/2} and another unchanged green emission from {sup 4}S{sub 3/2}→{sup 4}I{sub 15/2} were simultaneously observed, which are explained by steady-state rate equations analysis. Due to different evolution with temperature of the two green emissions, higher thermal sensitivity of optical thermal sensor was obtained based on the transitions with the largest fluorescence intensity ratio. Two parameters, maximum theoretical sensitivity (S{sub max}) and optimum operating temperature (T{sub max}) are given to describe thermal sensing properties of the produced sensors. The intensity ratio and energy difference ΔE of a pair of energy levels are two main factors for the sensitivity and accuracy of sensors, which should be referred to design sensors with optimized sensing properties.

  10. Investigation of upconversion and downconversion fluorescence emissions from β-NaLn1F{sub 4}:Yb{sup 3+}, Ln2{sup 3+} (Ln1 = Y, Lu; Ln2 = Er, Ho, Tm, Eu) hexagonal disk system

    SciTech Connect

    He, Enjie; Zheng, Hairong; Gao, Wei; Tu, Yinxun; Lu, Ying; Li, Guian

    2013-09-01

    Graphical abstract: Well-defined β-NaLn1F4:Yb{sup 3+}, Ln2{sup 3+} (Ln1 = Y, Lu; Ln2 = Er, Ho, Tm, Eu) hexagonal thin disks with a simple and user-friendly hydrothermal approach by using sodium citrate as a shape modifier. Much stronger UC and DC fluorescence emissions were observed in NaLuF{sub 4}-based hexagonal disks than that for NaYF{sub 4} counterparts. The strength of hypersensitive transitions is mainly attributed to the decrease of local symmetry Ln-F bond lengths in β-NaLuF{sub 4}. It will show a great potential in improving near-infrared conversion efficiency of silicon solar cells and removable sub-micro luminescent platforms. - Highlights: • Regular hexagonal disks (NaLnF{sub 4}) were synthesized by a simple hydrothermal method. • Much stronger UC and DC emissions were observed in NaLuF{sub 4}-based disks. • Stronger fluorescence emissions in NaLuF{sub 4}-based disks were explained reasonably. • NaLuF{sub 4}-based disks can act as a removable luminescent platform for nano-assembly. • NaLuF{sub 4}-based disks can be applied in improving efficiency of solar cells. - Abstract: Uniform hexagonal β-NaLn1F{sub 4}:Yb{sup 3+}, Ln2{sup 3+} (Ln1 = Y, Lu; Ln2 = Er, Ho, Tm, Eu) disks were synthesized with hydrothermal method in which the sodium citrate was used as a shape modifier. The experimental observation indicated that both upconversion and downconversion fluorescence emissions were significantly stronger in β-NaLuF{sub 4} than that for β-NaYF{sub 4}. It was found that the stronger hypersensitive transitions were mainly due to the increase of J–O parameter (Ω{sub 2}) in β-NaLuF{sub 4} host, while the stronger insensitive transitions were mainly caused by the stronger overlap of electron cloud that was induced by the decrease of Ln-F bond lengths. Additionally, the larger absorption strength in the near-infrared region is another important factor for the stronger fluorescence emissions. The current research has a great potential in

  11. Effect of OH - on upconversion luminescence of Er 3+-doped oxyhalide tellurite glasses

    NASA Astrophysics Data System (ADS)

    Xu, Shiqing; Fang, Dawei; Zhang, Zaixuan; Jiang, Zhonghong

    2005-06-01

    The Raman spectra, infrared spectra and upconversion luminescence spectra were studied, and the effect mechanism of OH - groups on the upconversion luminescence of Er 3+-doped oxyhalide tellurite glasses was analyzed. The results show that the phonon energy of lead chloride tellurite (PCT) glass was lower than that of lead fluoride tellurite (PFT) glass, but upconversion luminescence intensity of Er 3+-doped PFT glass was higher than that of Er 3+-doped PCT glass. The analysis considers that it was attributed mainly to the effect of OH - groups. The lower the absorption coefficient of the OH - groups, the higher the fluorescence lifetime of Er 3+, and as a result the higher upconversion luminescence intensity of Er 3+. In this work, the effect of OH - groups on the upconversion luminescence of Er 3+ was bigger than that of the phonon energy.

  12. Upconversion in Nd{sup 3+}-doped glasses: Microscopic theory and spectroscopic measurements

    SciTech Connect

    Oliveira, S. L.; Sousa, D. F. de; Andrade, A. A.; Nunes, L. A. O.; Catunda, T.

    2008-01-15

    In this work, we report a systematic investigation of upconversion losses and their effects on fluorescence quantum efficiency and fractional thermal loading in Nd{sup 3+}-doped fluoride glasses. The energy transfer upconversion ({gamma}{sub up}) parameter, which describes upconversion losses, was experimentally determined using different methods: thermal lens (TL) technique and steady state luminescence (SSL) measurements. Additionally, the upconversion parameter was also obtained from energy transfer models and excited state absorption measurements. The results reveal that the microscopic treatment provided by the energy transfer models is similar to the macroscopic ones achieved from the TL and SSL measurements because similar {gamma}{sub up} parameters were obtained. Besides, the achieved results also point out the migration-assisted energy transfer according to diffusion-limited regime rather than hopping regime as responsible for the upconversion losses in Nd-doped glasses.

  13. Plasmon enhancement of luminescence upconversion.

    PubMed

    Park, Wounjhang; Lu, Dawei; Ahn, Sungmo

    2015-05-21

    Frequency conversion has always been an important topic in optics. Nonlinear optics has traditionally focused on frequency conversion based on nonlinear susceptibility but with the recent development of upconversion nanomaterials, luminescence upconversion has begun to receive renewed attention. While upconversion nanomaterials open doors to a wide range of new opportunities, they remain too inefficient for most applications. Incorporating plasmonic nanostructures provides a promising pathway to highly efficient upconversion. Naturally, a plethora of theoretical and experimental studies have been published in recent years, reporting enhancements up to several hundred. It is however difficult to make meaningful comparisons since the plasmonic fields are highly sensitive to the local geometry and excitation condition. Also, many luminescence upconversion processes involve multiple steps via different physical mechanisms and the overall output is often determined by a delicate interplay among them. This review is aimed at offering a comprehensive framework for plasmon enhanced luminescence upconversion. We first present quantum electrodynamics descriptions for all the processes involved in luminescence upconversion, which include absorption, emission, energy transfer and nonradiative transitions. We then present a bird's eye view of published works on plasmon enhanced upconversion, followed by more detailed discussion on comparable classes of nanostructures, the effects of spacer layers and local heating, and the dynamics of the plasmon enhanced upconversion process. Plasmon enhanced upconversion is a challenging and exciting field from the fundamental scientific perspective and also from technological standpoints. It offers an excellent system to study how optical processes are affected by the local photonic environment. This type of research is particularly timely as the plasmonics is placing heavier emphasis on nonlinearity. At the same time, efficient upconversion

  14. Dual-modal fluorescent/magnetic bioprobes based on small sized upconversion nanoparticles of amine-functionalized BaGdF5:Yb/Er

    NASA Astrophysics Data System (ADS)

    Zeng, Songjun; Tsang, Ming-Kiu; Chan, Chi-Fai; Wong, Ka-Leung; Fei, Bin; Hao, Jianhua

    2012-07-01

    A new type of BaGdF5:Yb/Er nanoprobe for dual-modal fluorescent and magnetic resonance imaging (MRI) is demonstrated. Water soluble and amine-functionalized BaGdF5:Yb/Er nanoparticles (NPs) with average size of about 10 nm were synthesized by a facile one-pot hydrothermal method. The in vitro up-converted emission of BaGdF5:Yb/Er NPs is observed in HeLa cells with near-infrared excitation at 980 nm and served as a fluorescent label. In addition, the cytotoxicity assay in HeLa cells shows low cell toxicity of the amine-functionalized BaGdF5:Yb/Er NPs. Moreover, these BaGdF5 NPs exhibit excellent intrinsic paramagnetic properties and enhanced T1-weighted MRI images with increased concentrations of BaGdF5 NPs. Therefore, these results suggest that the amine-functionalized BaGdF5 NPs with an optimized size and low cell toxicity are promising dual-modal bioprobes for optical bioimaging and MRI.A new type of BaGdF5:Yb/Er nanoprobe for dual-modal fluorescent and magnetic resonance imaging (MRI) is demonstrated. Water soluble and amine-functionalized BaGdF5:Yb/Er nanoparticles (NPs) with average size of about 10 nm were synthesized by a facile one-pot hydrothermal method. The in vitro up-converted emission of BaGdF5:Yb/Er NPs is observed in HeLa cells with near-infrared excitation at 980 nm and served as a fluorescent label. In addition, the cytotoxicity assay in HeLa cells shows low cell toxicity of the amine-functionalized BaGdF5:Yb/Er NPs. Moreover, these BaGdF5 NPs exhibit excellent intrinsic paramagnetic properties and enhanced T1-weighted MRI images with increased concentrations of BaGdF5 NPs. Therefore, these results suggest that the amine-functionalized BaGdF5 NPs with an optimized size and low cell toxicity are promising dual-modal bioprobes for optical bioimaging and MRI. Electronic supplementary information (ESI) available: FTIR spectra, EDS, and the simplified energy-level diagrams of Yb3+/Er3+. See DOI: 10.1039/c2nr31294h

  15. Thermally activated delayed fluorescence from {sup 3}nπ* to {sup 1}nπ* up-conversion and its application to organic light-emitting diodes

    SciTech Connect

    Li, Jie; Zhang, Qisheng; Nomura, Hiroko; Miyazaki, Hiroshi; Adachi, Chihaya

    2014-07-07

    Intense nπ* fluorescence from a nitrogen-rich heterocyclic compound, 2,5,8-tris(4-fluoro-3-methylphenyl)-1,3,4,6,7,9,9b-heptaazaphenalene (HAP-3MF), is demonstrated. The overlap-forbidden nature of the nπ* transition and the higher energy of the {sup 3}ππ* state than the {sup 3}nπ* one lead to a small energy difference between the lowest singlet (S{sub 1}) and triplet (T{sub 1}) excited states of HAP-3MF. Green-emitting HAP-3MF has a moderate photoluminescence quantum yield of 0.26 in both toluene and doped film. However, an organic light-emitting diode containing HAP-3MF achieved a high external quantum efficiency of 6.0%, indicating that HAP-3MF harvests singlet excitons through a thermally activated T{sub 1} → S{sub 1} pathway in the electroluminescent process.

  16. Thermally activated delayed fluorescence from 3nπ* to 1nπ* up-conversion and its application to organic light-emitting diodes

    NASA Astrophysics Data System (ADS)

    Li, Jie; Zhang, Qisheng; Nomura, Hiroko; Miyazaki, Hiroshi; Adachi, Chihaya

    2014-07-01

    Intense nπ* fluorescence from a nitrogen-rich heterocyclic compound, 2,5,8-tris(4-fluoro-3-methylphenyl)-1,3,4,6,7,9,9b-heptaazaphenalene (HAP-3MF), is demonstrated. The overlap-forbidden nature of the nπ* transition and the higher energy of the 3ππ* state than the 3nπ* one lead to a small energy difference between the lowest singlet (S1) and triplet (T1) excited states of HAP-3MF. Green-emitting HAP-3MF has a moderate photoluminescence quantum yield of 0.26 in both toluene and doped film. However, an organic light-emitting diode containing HAP-3MF achieved a high external quantum efficiency of 6.0%, indicating that HAP-3MF harvests singlet excitons through a thermally activated T1 → S1 pathway in the electroluminescent process.

  17. LDS-750 as a probe of solvation dynamics: a femtosecond time-resolved fluorescence study in liquid aniline

    NASA Astrophysics Data System (ADS)

    Smith, Neil A.; Meech, Stephen R.; Rubtsov, Igor V.; Yoshihara, Keitaro

    1999-04-01

    The dynamics of the fluorescence Stokes shift of the styryl dye LDS-750 have been measured in liquid aniline with sub-100 fs time resolution. The shape of the time-resolved spectra are time dependent, which is not consistent with the predictions of a solvation dynamics mechanism. However, the measured spectral shift correlation function is reasonably well described by the dynamical mean spherical approximation model of solvation dynamics. It is suggested that these observations are consistent if solvent dynamics is the rate controlling process in both solvation of the increased dipole moment of the excited state of LDS-750 and the stabilisation of a distribution of solute conformers in the excited state.

  18. Fluorescence kinetics of Trp-Trp dipeptide and its derivatives in water via ultrafast fluorescence spectroscopy.

    PubMed

    Jia, Menghui; Yi, Hua; Chang, Mengfang; Cao, Xiaodan; Li, Lei; Zhou, Zhongneng; Pan, Haifeng; Chen, Yan; Zhang, Sanjun; Xu, Jianhua

    2015-08-01

    Ultrafast fluorescence dynamics of Tryptophan-Tryptophan (Trp-Trp/Trp2) dipeptide and its derivatives in water have been investigated using a picosecond resolved time correlated single photon counting (TCSPC) apparatus together with a femtosecond resolved upconversion spectrophotofluorometer. The fluorescence decay profiles at multiple wavelengths were fitted by a global analysis technique. Nanosecond fluorescence kinetics of Trp2, N-tert-butyl carbonyl oxygen-N'-aldehyde group-l-tryptophan-l-tryptophan (NBTrp2), l-tryptophan-l-tryptophan methyl ester (Trp2Me), and N-acetyl-l-tryptophan-l-tryptophan methyl ester (NATrp2Me) exhibit multi-exponential decays with the average lifetimes of 1.99, 3.04, 0.72 and 1.22ns, respectively. Due to the intramolecular interaction between two Trp residues, the "water relaxation" lifetime was observed around 4ps, and it is noticed that Trp2 and its derivatives also exhibit a new decay with a lifetime of ∼100ps, while single-Trp fluorescence decay in dipeptides/proteins shows 20-30ps. The intramolecular interaction lifetime constants of Trp2, NBTrp2, Trp2Me and NATrp2Me were then calculated to be 3.64, 0.93, 11.52 and 2.40ns, respectively. Candidate mechanisms (including heterogeneity, solvent relaxation, quasi static self-quenching or ET/PT quenching) have been discussed. PMID:26111991

  19. Up-conversion luminescence and optical temperature sensing behaviour of Yb3+/Er3+ codoped CaWO4 material

    NASA Astrophysics Data System (ADS)

    Cheng, Xuerui; Yang, Kun; Wang, Jiankun; Yang, Linfu; Cheng, Xiaoshuai

    2016-08-01

    Present article report on structural and optical properties of Er3+/Yb3+ codoped CaWO4 phosphors. Structural properties are explored using XRD and Raman technologies. The upconversion emission has been investigated with 980 nm excitation. The upconversion emission intensity is dependent on the concentrations of Yb3+ ions and reaches a maximum at 7%. Logarithmic plots of power dependencies reveal that the green and red emissions originate from a two-photon upconversion process. Based on the photon energy and the emission spectra, the possible upconversion processes and emission mechanisms are discussed. Finally, the optical temperature sensing properties has been performed using the fluorescence intensity ratio technique based on green upconversion emissions. Its temperature sensitivity is found to be above 0.0025 K-1 in the whole temperature range of 300-540 K, revealing this phosphor to be a promising optical temperature sensing material.

  20. Effect of OH{sup -} on upconversion luminescence of Er{sup 3+}-doped oxyhalide tellurite glasses

    SciTech Connect

    Xu Shiqing . E-mail: shiquingxu75@hotmail.com; Fang Dawei; Zhang Zaixuan; Jiang Zhonghong

    2005-06-15

    The Raman spectra, infrared spectra and upconversion luminescence spectra were studied, and the effect mechanism of OH{sup -} groups on the upconversion luminescence of Er{sup 3+}-doped oxyhalide tellurite glasses was analyzed. The results show that the phonon energy of lead chloride tellurite (PCT) glass was lower than that of lead fluoride tellurite (PFT) glass, but upconversion luminescence intensity of Er{sup 3+}-doped PFT glass was higher than that of Er{sup 3+}-doped PCT glass. The analysis considers that it was attributed mainly to the effect of OH{sup -} groups. The lower the absorption coefficient of the OH{sup -} groups, the higher the fluorescence lifetime of Er{sup 3+}, and as a result the higher upconversion luminescence intensity of Er{sup 3+}. In this work, the effect of OH{sup -} groups on the upconversion luminescence of Er{sup 3+} was bigger than that of the phonon energy.

  1. 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. PMID:22996059

  2. Detection of telomerase on upconversion nanoparticle modified cellulose paper.

    PubMed

    Wang, Faming; Li, Wen; Wang, Jiasi; Ren, Jinsong; Qu, Xiaogang

    2015-07-25

    Herein we report a convenient and sensitive method for the detection of telomerase activity based on upconversion nanoparticle (UCNP) modified cellulose paper. Compared with many solution-phase systems, this paper chip is more stable and easily stores the test results. What's more, the low background fluorescence of the UCNPs increases the sensitivity of this method, and the low telomerase levels in different cell lines can clearly be discriminated by the naked eye. PMID:26095724

  3. Multifunctional Upconversion-Magnetic Hybrid Nanostructured Materials: Synthesis and Bioapplications

    PubMed Central

    Li, Xiaomin; Zhao, Dongyuan; Zhang, Fan

    2013-01-01

    The combination of nanotechnology and biology has developed into an emerging research area: nano-biotechnology. Upconversion nanoparticles (UCNPs) have attracted a great deal of attention in bioapplications due to their high chemical stability, low toxicity, and high signal-to-noise ratio. Magnetic nanoparticles (MNPs) are also well-established nanomaterials that offer controlled size, ability to be manipulated externally, and enhancement of contrast in magnetic resonance imaging (MRI). As a result, these nanoparticles could have many applications in biology and medicine, including protein purification, drug delivery, and medical imaging. Because of the potential benefits of multimodal functionality in biomedical applications, researchers would like to design and fabricate multifunctional upconversion-magnetic hybrid nanostructured materials. The hybrid nanostructures, which combine UCNPs with MNPs, exhibit upconversion fluorescence alongside superparamagnetism property. Such structures could provide a platform for enhanced bioimaging and controlled drug delivery. We expect that the combination of unique structural characteristics and integrated functions of multifunctional upconversion-magnetic nanoparticles will attract increasing research interest and could lead to new opportunities in nano-bioapplications. PMID:23650477

  4. Intramolecular charge transfer with the planarized 4-cyanofluorazene and its flexible counterpart 4-cyano-N-phenylpyrrole. Picosecond fluorescence decays and femtosecond excited-state absorption.

    PubMed

    Druzhinin, Sergey I; Kovalenko, Sergey A; Senyushkina, Tamara A; Demeter, Attila; Machinek, Reinhard; Noltemeyer, Mathias; Zachariasse, Klaas A

    2008-09-11

    The fluorescence spectrum of the rigidified 4-cyanofluorazene (FPP4C) in n-hexane consists of a dual emission from a locally excited (LE) and an intramolecular charge-transfer (ICT) state, with an ICT/LE fluorescence quantum yield ratio of Phi'(ICT)/Phi(LE) = 3.3 at 25 degrees C. With the flexible 4-cyano- N-phenylpyrrole (PP4C) in n-hexane, such an ICT reaction also takes place, with Phi'(ICT)/Phi(LE) = 1.5, indicating that for this reaction, a perpendicular twist of the pyrrole and benzonitrile moieties is not required. The ICT emission band of FPP4C and PP4C in n-hexane has vibrational structure, but a structureless band is observed in all other solvents more polar than the alkanes. The enthalpy difference Delta H of the LE --> ICT reaction in n-hexane, -11 kJ/mol for FPP4C and -7 kJ/mol for PP4C, is determined by analyzing the temperature dependence of Phi'(ICT)/Phi(LE). Using these data, the energy E(FC,ICT) of the Franck-Condon ground state populated by the ICT emission is calculated, 41 (FPP4C) and 40 kJ/mol (PP4C). These large values for E(FC,ICT) lead to the conclusion that with FPP4C and PP4C, direct ICT excitation, bypassing LE, does not take place. FPP4C has an ICT dipole moment of 15 D, similar to that of PP4C (16 D). Picosecond fluorescence decays allow the determination of the ICT lifetime, from which the radiative rate constant k'(f)(ICT) is derived, with comparable values for FPP4C and PP4C. This shows that an argument for a twisted ICT state of PP4C cannot come from k'(f)(ICT). After correction for the solvent refractive index and the energy of the emission maximum nu(max)(ICT), it appears that k'(f)(ICT) is solvent-polarity-independent. Femtosecond transient absorption with FPP4C and PP4C in n-hexane reveals that the ICT state is already nearly fully present at 100 fs after excitation, in rapid equilibrium with LE. In MeCN, the ICT state of FPP4C and PP4C is likewise largely developed at this delay time, and the reaction is limited by dielectric

  5. TPGS-stabilized NaYbF4:Er upconversion nanoparticles for dual-modal fluorescent/CT imaging and anticancer drug delivery to overcome multi-drug resistance.

    PubMed

    Tian, Gan; Zheng, Xiaopeng; Zhang, Xiao; Yin, Wenyan; Yu, Jie; Wang, Dongliang; Zhang, Zhiping; Yang, Xiangliang; Gu, Zhanjun; Zhao, Yuliang

    2015-02-01

    Multi-drug resistance (MDR) is a major cause of failure in cancer chemotherapy. Tocopheryl polyethylene glycol 1000 succinate (TPGS) has been extensively investigated for overcoming MDR in cancer therapy because of its ability to inhibit P-glycoprotein (P-gp). In this work, TPGS was for the first time used as a new surface modifier to functionalize NaYbF4:Er upconversion nanoparticles (UNCPs) and endowed the as-prepared products (TPGS-UCNPs) with excellent water-solubility, P-gp inhibition capability and imaging-guided drug delivery property. After the chemotherapeutic drug (doxorubicin, DOX) loading, the as-formed composites (TPGS-UCNPs-DOX) exhibited potent killing ability for DOX-resistant MCF-7 cells. Flow-cytometric assessment and Western blot assay showed that the TPGS-UCNPs could potently decrease the P-gp expression and facilitate the intracellular drug accumulation, thus achieving MDR reversal. Moreover, considering that UCNPs process efficient upconversion emission and Yb element contained in UCNPs has strong X-ray attenuation ability, the as-obtained composite could also serve as a dual-modal probe for upconversion luminescence (UCL) imaging and X-ray computed tomography (CT) imaging, making them promising for imaging-guided cancer therapy. PMID:25433607

  6. Preservation of fluorescence and Raman gain in the buried channel waveguides in neodymium-doped KGd(WO{sub 4}){sub 2}(Nd:KGW) by femtosecond laser writing

    SciTech Connect

    Liu Xiaoyu; Qu Shiliang; Tan Yang; Chen Feng

    2011-02-20

    We report on the preservation of fluorescence and Raman gain in low-repetition-rate femtosecond laser written buried channel waveguides in neodymium-doped KGd(WO{sub 4}){sub 2}. The propagation loss index, profile reconstruction, and calculation of the modal intensity distribution by the beam propagation method of the waveguide are presented. Microluminescence spectra of the waveguides show that the fluorescence properties of Nd{sup 3+} ions are not significantly affected by the waveguide formation processing, which indicates a fairly good potential for further laser actions in a compact device. Micro-Raman spectra are also performed to reveal the preservation of the characteristic 768 and 901 cm{sup -1} Raman mode intensities in the guiding regions.

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

    PubMed Central

    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)

    2015-01-01

    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. PMID:25976870

  8. Tailoring Plasmonic Enhanced Upconversion in Single NaYF4:Yb(3+)/Er(3+) Nanocrystals.

    PubMed

    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

    2015-01-01

    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:Yb(3+)/Er(3+) 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. PMID:25976870

  9. Upconversion nanoparticles and their composite nanostructures for biomedical imaging and cancer therapy

    NASA Astrophysics Data System (ADS)

    Cheng, Liang; Wang, Chao; Liu, Zhuang

    2012-12-01

    Upconversion nanoparticles (UCNPs), particularly lanthanide-doped nanocrystals, which emit high energy photons under excitation by the near-infrared (NIR) light, have found potential applications in many different fields, including biomedicine. Compared with traditional down-conversion fluorescence imaging, the NIR light excited upconversion luminescence (UCL) imaging relying on UCNPs exhibits improved tissue penetration depth, higher photochemical stability, and is free of auto-fluorescence background, which promises biomedical imaging with high sensitivity. On the other hand, the unique upconversion process of UCNPs may be utilized to activate photosensitive therapeutic agents for applications in cancer treatment. Moreover, the integration of UCNPs with other functional nanostructures could result in the obtained nanocomposites having highly enriched functionalities, useful in imaging-guided cancer therapies. This review article will focus on the biomedical imaging and cancer therapy applications of UCNPs and their nanocomposites, and discuss recent advances and future prospects in this emerging field.

  10. Mid-infrared nonlinear upconversion imaging and sensing

    NASA Astrophysics Data System (ADS)

    Pedersen, Christian; Tidemand-Lichtenberg, Peter

    2016-03-01

    The mid-IR wavelength range is highly relevant for a number of applications related to gas spectroscopy and spectral analysis of complex molecules such as those including CH bounds. The main obstacles for exploitation of mid-IR applications include suitable and affordable mid-IR light sources for excitation of the sample and sensitive mid-IR detectors. With the advent of mid-IR Quantum cascaded lasers and super continuum light sources new possibilities has emerged. However, low-noise, mid-IR (2-15 μm) detection is still challenging requiring cryogenic cooling to gain sensitivities needed for measurements of fluorescence or absorptions signals. Mid-IR upconversion imaging and detection using nonlinear crystals offers good promise as an alternative, sensitive mid-IR imaging and detection technology. In this paper the fundamental properties of upconversion is discussed.

  11. Sodium yttrium fluoride based upconversion nano phosphors for biosensing

    NASA Astrophysics Data System (ADS)

    Parameswaran Nampi, Padmaja; Varma, Harikrishna; Biju, P. R.; Kakkar, Tarun; Jose, Gin; Saha, Sikha; Millner, Paul

    2015-06-01

    In the present study, NaYF4-Yb3+/Er3+ having the composition NaYF4-18%Yb3+/2%Er3+ and NaYF4-20%Yb3+/2%Er3+ with and without the addition of PVP (polyvinyl pyrolidone) have been synthesised by a solution method using NaF, yttrium nitrate, ytterbium nitrate and erbium nitrate as precursors. Upconversion spectra of prepared nanomaterial under 980 nm laser excitation have been studied. The variation in upconversion spectra with new born calf serum and myoglobin has been studied. Myoglobin (Mb) may be helpful when used in conjunction with other cardiac markers for rapid determination of acute myocardial ischemia, especially in patients with a typical chest pain or nonspecific ECG changes. The variation of UC fluorescence with addition of Mb indicates the suitability of using NaYF4 based UC nanoparticles in cardiac marker detection. The detailed study is currently under progress.

  12. A general strategy for biocompatible, high-effective upconversion nanocapsules based on triplet-triplet annihilation.

    PubMed

    Liu, Qian; Yin, Baoru; Yang, Tianshe; Yang, Yongchao; Shen, Zhen; Yao, Ping; Li, Fuyou

    2013-04-01

    A general strategy for constructing high-effective upconversion nanocapsules based on triplet-triplet annihilation (TTA) was developed by loading both sensitizer and annihilator into BSA-dextran stabilized oil droplets. This strategy can maintain high translational mobility of the chromophores, avoid luminescence quenching of chromophore by aggregation, and decrease the O2-induced quenching of TTA-based upconversion emission. Pt(II)-tetraphenyl-tetrabenzoporphyrin (PtTPBP) and BODIPY dyes (BDP-G and BDP-Y with the maximal fluorescence emission at 528 and 546 nm, respectively) were chosen as sensitizer/annihilator couples to fabricate green and yellow upconversion luminescent emissive nanocapsules, named UCNC-G and UCNC-Y, respectively. In water under the atmospheric environment, interestingly, UCNC-G and UCNC-Y exhibit intense upconversion luminescence (UCL) emission (λex = 635 nm) with the quantum efficiencies (ΦUCL) of 1.7% and 4.8%, respectively, whereas very weak UCL emission (ΦUCL < 0.1%) was observed for the corresponding previous reported SiO2-coating nanosystems because of aggregation-induced fluorescence quenching of annihilators. Furthermore, application of theses upconversion nanocapsules for high-contrast UCL bioimaging in vivo of living mice without removing the skin was demonstrated under 635-nm excitation with low power density of 12.5 mW cm(-2). PMID:23464990

  13. Photon-avalanche upconversion in thulium-doped lutetium aluminum garnet.

    PubMed

    Patel, D N; Reddy, B R; Nash-Stevenson, S K

    1999-05-20

    Strong blue fluorescence at 487 nm corresponding to the (1)G(4) --> (3)H(6) transition was generated from Tm(3+)-doped lutetium aluminum garnet on excitation with a 618-nm dye laser as a result of a photon-avalanche upconversion mechanism. PMID:18319920

  14. 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…

  15. Upconversion processes in Yb-sensitized Tm:ZBLAN

    SciTech Connect

    Carrig, T.J.; Cockroft, N.J.

    1996-10-01

    A spectroscopic study of 22 rare-earth-ion doped ZBLAN (fluorozirconate) glass was done to study feasibility of sensitizing Tm:ZBLAN with Yb to facilitate development of an efficient, conveniently pumped blue upconversion fiber laser. it was found that, under single-color pumping, 480 nm emission from Tm{sup 3+} was strongest when Yb,Tm:ZBLAN is excited at 975 nm; the strongest blue blue emission was obtained from a glass sample with 2.0 wt% Yb + 0.3 wt% Tm. Also, for weak 975 nm pump intensities, strength of blue upconversion emission can be greatly enhanced by simultaneously pumping at 785 nm. This increased upconversion efficiency is due to reduced number of energy transfer steps needed to populate the Tm{sup 3+} {sup 1}G{sub 4} energy level. Measurements of fluorescence lifetimes vs dopant concentration were also made for Yb{sup 3+}, Tm{sup 3+}, and Pr{sup 3+} transitions in ZBLAN in order to better characterize concentration quenching effects. Energy transfer between Tm{sup 3+} and Pr{sup 3+} in ZBLAN is also described.

  16. Simultaneous excitation and emission enhancements in upconversion luminescence using plasmonic double-resonant gold nanorods

    NASA Astrophysics Data System (ADS)

    Liu, Xin; Yuan Lei, Dang

    2015-10-01

    The geometry and dimension of a gold nanorod (GNR) are optimally designed to enhance the fluorescence intensity of a lanthanide-doped upconversion nanocrystal placed in close proximity to the GNR. A systematic study of the electromagnetic interaction between the upconversion emitter of three energy levels and the GNR shows that the enhancement effect arising from localized electric field-induced absorption can be balanced by the negative effect of electronic transition from an intermediate state to the ground state of the emitter. The dependence of fluorescence enhancement on the emitter-GNR separation is investigated, and the results demonstrate a maximum enhancement factor of 120 folds and 160 folds at emission wavelengths 650 and 540 nm, respectively. This is achieved at the emitter-GNR separation ranging from 5 to 15 nm, depending on the initial quantum efficiency of the emitter. The modified upconversion luminescence behavior by adjusting the aspect ratio of the GNR and the relative position of the emitter indicates the dominate role of excitation process in the total fluorescence enhancement. These findings are of great importance for rationally designing composite nanostructures of metal nanoparticles and upconversion nanocrystals with maximized plasmonic enhancement for bioimaging and sensing applications.

  17. Simultaneous excitation and emission enhancements in upconversion luminescence using plasmonic double-resonant gold nanorods

    PubMed Central

    Liu, Xin; Yuan Lei, Dang

    2015-01-01

    The geometry and dimension of a gold nanorod (GNR) are optimally designed to enhance the fluorescence intensity of a lanthanide-doped upconversion nanocrystal placed in close proximity to the GNR. A systematic study of the electromagnetic interaction between the upconversion emitter of three energy levels and the GNR shows that the enhancement effect arising from localized electric field-induced absorption can be balanced by the negative effect of electronic transition from an intermediate state to the ground state of the emitter. The dependence of fluorescence enhancement on the emitter-GNR separation is investigated, and the results demonstrate a maximum enhancement factor of 120 folds and 160 folds at emission wavelengths 650 and 540 nm, respectively. This is achieved at the emitter-GNR separation ranging from 5 to 15 nm, depending on the initial quantum efficiency of the emitter. The modified upconversion luminescence behavior by adjusting the aspect ratio of the GNR and the relative position of the emitter indicates the dominate role of excitation process in the total fluorescence enhancement. These findings are of great importance for rationally designing composite nanostructures of metal nanoparticles and upconversion nanocrystals with maximized plasmonic enhancement for bioimaging and sensing applications. PMID:26468686

  18. Simultaneous excitation and emission enhancements in upconversion luminescence using plasmonic double-resonant gold nanorods.

    PubMed

    Liu, Xin; Yuan Lei, Dang

    2015-01-01

    The geometry and dimension of a gold nanorod (GNR) are optimally designed to enhance the fluorescence intensity of a lanthanide-doped upconversion nanocrystal placed in close proximity to the GNR. A systematic study of the electromagnetic interaction between the upconversion emitter of three energy levels and the GNR shows that the enhancement effect arising from localized electric field-induced absorption can be balanced by the negative effect of electronic transition from an intermediate state to the ground state of the emitter. The dependence of fluorescence enhancement on the emitter-GNR separation is investigated, and the results demonstrate a maximum enhancement factor of 120 folds and 160 folds at emission wavelengths 650 and 540 nm, respectively. This is achieved at the emitter-GNR separation ranging from 5 to 15 nm, depending on the initial quantum efficiency of the emitter. The modified upconversion luminescence behavior by adjusting the aspect ratio of the GNR and the relative position of the emitter indicates the dominate role of excitation process in the total fluorescence enhancement. These findings are of great importance for rationally designing composite nanostructures of metal nanoparticles and upconversion nanocrystals with maximized plasmonic enhancement for bioimaging and sensing applications. PMID:26468686

  19. Optical transitions and visible upconversion in Er3+ doped niobic tellurite glass

    NASA Astrophysics Data System (ADS)

    Lin, Hai; Meredith, Gerald; Jiang, Shibin; Peng, Xiang; Luo, Tao; Peyghambarian, Nasser; Pun, Edwin Yue-Bun

    2003-01-01

    Er3+ doped Nb2O5-TeO2 (NT) glass suitable for developing optical fiber laser and amplifier has been fabricated and characterized. Intense and broad 1.53 μm infrared fluorescence and visible upconversion luminescence were observed under 975 nm diode laser and 798 nm laser excitation. For 1.53 μm emission band, the full width at half-maximum is 51 nm, the fluorescence lifetime is 2.6 ms, and the quantum efficiency is ˜100%. The maximum emission cross section is 8.52×10-21 cm2 at 1.532 μm, and is higher than the values in silicon and phosphate glasses. Under 798 nm excitation, efficient 531, 553, and 670 nm upconversion emissions are due to two-photon absorption processes. The "standardized" efficiency for the green upconversion light is 9.5×10-4, and this value is comparable to that reported for Er3+/Yb3+ codoped fluoride glasses. Intense visible upconversion fluorescence in Er3+ doped NT glass can be used in color display, undersea communication, and infrared sensor.

  20. A new medium for triplet-triplet annihilated upconversion and photocatalytic application.

    PubMed

    Ye, Changqing; Wang, Jingjing; Wang, Xiaomei; Ding, Ping; Liang, Zuoqin; Tao, Xutang

    2016-02-01

    Since the triplet-triplet annihilated upconversion (TTA-UC) materials work efficiently only in degassing organic solvents, it is of significance to find a new medium without toxicity and volatility and that promotes TTA-UC. Here, we firstly reported the effect of an OH-containing medium on low power upconversion and found that in alcohol solvent containing β-cyclodextrin (β-CD), the phosphorescence lifetime (τp) of the sensitizer (PdTPP) and the fluorescence quantum yield (Φf) of the acceptor (DPA) were enhanced with the increase in the number of OH-groups of the medium. A large triplet-triplet quenching constant (kq, 1.91 × 10(9) M(-1) s(-1)) and high upconversion efficiency (ΦUC, ∼ 36%) of PdTPP/DPA were obtained under the excitation of a diode laser (532 nm, 60 mW cm(-2)). Under our green-to-blue upconversion irradiation, in a demonstration experiment the photocurrent was recorded at 0.09 μA cm(-2), resulting from photocatalytic water splitting by a Cd0.7Zn0.3S photoanode and a Pt counter-electrode in a photoelectrochemical cell. The importance of this study suggests that upconversion-powered photoelectrochemistry possesses potential application for hydrogen generation from water under excitation of sun energy. PMID:26580451

  1. An upconversion luminescence nanoprobe for the ultrasensitive detection of hyaluronidase.

    PubMed

    Wang, Zhe; Li, Xiaohua; Song, Yanchao; Li, Lihong; Shi, Wen; Ma, Huimin

    2015-06-01

    A new upconversion luminescence nanoprobe for the detection of hyaluronidase has been developed by coupling the hyaluronic acid-bearing upconversion fluorescence nanoparticles (HA-UCNPs) with poly(m-phenylenediamine) (PMPD) nanospheres via covalent linkage. The nanoprobe alone exhibits an extremely low background signal owing to the effective fluorescence quenching by electron-rich PMPD and the near-infrared excitation characteristic (λex = 980 nm) of HA-UCNPs; upon reaction with hyaluronidase, however, a more than 31-fold fluorescence enhancement is produced. Compared with the corresponding nanosystem assembled via physical adsorption, the prepared nanoprobe shows a largely increased stability and a much higher signal-to-background ratio, which offers an ultrasensitive assay for hyaluronidase, with a detection limit of 0.6 ng/mL. The nanoprobe has been successfully used to determine hyaluronidase in human serum samples from both colorectal cancer patients and healthy people, disclosing that the serum hyaluronidase level in colorectal cancer patients is roughly 3 times higher than that in healthy people. Furthermore, the nanoprobe has also been employed to study the activity change of hyaluronidase affected by different concentrations of arsenate (a potential carcinogen), and the results show that even a low dosage of arsenate (50 μg/L) can raise the activity of hyaluronidase by about one-third, revealing the relationship between arsenate and the enzyme. The proposed method is not only simple but also highly sensitive, making it useful to assay hyaluronidase in relevant clinical samples. PMID:25947627

  2. Photon upconversion with directed emission.

    PubMed

    Börjesson, K; Rudquist, P; Gray, V; Moth-Poulsen, K

    2016-01-01

    Photon upconversion has the potential to increase the efficiency of single bandgap solar cells beyond the Shockley Queisser limit. Efficient light management is an important point in this context. Here we demonstrate that the direction of upconverted emission can be controlled in a reversible way, by embedding anthracene derivatives together with palladium porphyrin in a liquid crystalline matrix. The system is employed in a triplet-triplet annihilation photon upconversion scheme demonstrating controlled switching of directional anti Stokes emission. Using this approach an emission ratio of 0.37 between the axial and longitudinal emission directions and a directivity of 1.52 is achieved, reasonably close to the theoretical maximal value of 2 obtained from a perfectly oriented sample. The system can be switched for multiple cycles without any visible degradation and the speed of switching is only limited by the intrinsic rate of alignment of the liquid crystalline matrix. PMID:27573539

  3. Femtosecond upconverted photocurrent spectroscopy of InAs quantum nanostructures

    SciTech Connect

    Yamada, Yasuhiro; Tex, David M.; Kanemitsu, Yoshihiko; Kamiya, Itaru

    2015-07-06

    The carrier upconversion dynamics in InAs quantum nanostructures are studied for intermediate-band solar-cell applications via ultrafast photoluminescence and photocurrent (PC) spectroscopy based on femtosecond excitation correlation (FEC) techniques. Strong upconverted PC-FEC signals are observed under resonant excitation of quantum well islands (QWIs), which are a few monolayer-thick InAs quantum nanostructures. The PC-FEC signal typically decays within a few hundred picoseconds at room temperature, which corresponds to the carrier lifetime in QWIs. The photoexcited electron and hole lifetimes in InAs QWIs are evaluated as functions of temperature and laser fluence. Our results provide solid evidence for electron–hole–hole Auger process, dominating the carrier upconversion in InAs QWIs at room temperature.

  4. Photon upconversion in core-shell nanoparticles.

    PubMed

    Chen, Xian; Peng, Denfeng; Ju, Qiang; Wang, Feng

    2015-03-21

    Photon upconversion generally results from a series of successive electronic transitions within complex energy levels of lanthanide ions that are embedded in the lattice of a crystalline solid. In conventional lanthanide-doped upconversion nanoparticles, the dopant ions homogeneously distributed in the host lattice are readily accessible to surface quenchers and lose their excitation energy, giving rise to weak and susceptible emissions. Therefore, present studies on upconversion are mainly focused on core-shell nanoparticles comprising spatially confined dopant ions. By doping upconverting lanthanide ions in the interior of a core-shell nanoparticle, the upconversion emission can be substantially enhanced, and the optical integrity of the nanoparticles can be largely preserved. Optically active shells are also frequently employed to impart multiple functionalities to upconversion nanoparticles. Intriguingly, the core-shell design introduces the possibility of constructing novel upconversion nanoparticles by exploiting the energy exchange interactions across the core-shell interface. In this tutorial review, we highlight recent advances in the development of upconversion core-shell nanoparticles, with particular emphasis on the emerging strategies for regulating the interplay of dopant interactions through core-shell nanostructural engineering that leads to unprecedented upconversion properties. The improved control over photon energy conversion will open up new opportunities for biological and energy applications. PMID:25058157

  5. 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.

  6. The dependence of the ultrafast relaxation kinetics of the S2 and S1 states in β-carotene homologs and lycopene on conjugation length studied by femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies

    NASA Astrophysics Data System (ADS)

    Kosumi, Daisuke; Fujiwara, Masazumi; Fujii, Ritsuko; Cogdell, Richard J.; Hashimoto, Hideki; Yoshizawa, Masayuki

    2009-06-01

    The ultrafast relaxation kinetics of all-trans-β-carotene homologs with varying numbers of conjugated double bonds n(n =7-15) and lycopene (n =11) has been investigated using femtosecond time-resolved absorption and Kerr-gate fluorescence spectroscopies, both carried out under identical excitation conditions. The nonradiative relaxation rates of the optically allowed S2(1Bu+1) state were precisely determined by the time-resolved fluorescence. The kinetics of the optically forbidden S1(2Ag-1) state were observed by the time-resolved absorption measurements. The dependence of the S1 relaxation rates upon the conjugation length is adequately described by application of the energy gap law. In contrast to this, the nonradiative relaxation rates of S2 have a minimum at n =9 and show a reverse energy gap law dependence for values of n above 11. This anomalous behavior of the S2 relaxation rates can be explained by the presence of an intermediate state (here called the Sx state) located between the S2 and S1 states at large values of n (such as n =11). The presence of such an intermediate state would then result in the following sequential relaxation pathway S2→Sx→S1→S0. A model based on conical intersections between the potential energy curves of these excited singlet states can readily explain the measured relationships between the decay rates and the energy gaps.

  7. Energy transfer and upconversion in Yb:YAG and Yb:Er:YAG

    SciTech Connect

    Lacovara, P.

    1992-01-01

    Energy transfer and upconversion have been studied in ytterbium, and ytterbium-erbium doped YAG (yttrium-aluminum garnet Y[sub 2]Al[sub 5]O[sub 12]). The energy-transfer probabilities were calculated for Yb-Yb, Yb-Er, and Er-Yb interactions, as well as for Er-Er and Yb-Er upconversion. The transfer of excitation from ytterbium to erbium was found experimentally to be efficient at Er concentrations above about 1%, with an Yb concentration of 6.5%. The Burshtein hopping model for donor migration-assisted transfer was applied to the Yb-Er system for different Er concentrations. Fitting the decay predicted by the Burshtein model to the Yb fluorescence gave a value for the Yb-Er dipole-dipole interaction strength which was in very close agreement with the calculated value, but discrepancies were noted for the donor-donor interaction. Upconversion was observed during pulsed measurements, and studies in detail with intense CW pumping. The Yb-Er upconversion was observed to dominate the Er-Er upconversion in the Yb-Er samples. Values for the Yb-Er and Er-Er ([sup 4]I[sub 1 1/2]) upconversion coefficients were determined from quantitative measurements of the [sup 4]S[sub 3/2] fluorescence which these processes generate, and measurements of the change in [sup 4]I[sub 1 1/2] population with increasing pump density. The quenching of nominally pure Yb:YAG by trace rare-earth impurities was also studied. The time dependence of the Yb fluorescence decay in some high-concentration samples suggested a fast quenching process active at high excited-ion densities, and a slower one at lower excited-ion densities. Study of the cooperative luminescence emitted by excited Yb pairs suggested a quenching mechanism acting preferentially on pairs. Sensitive Ar[sup +]-ion laser-pumped fluorescence measurements showed the presence of high ppm levels of several impurities, including Er, Tm and Cr. Pumping the ytterbium at 940 nm using pulsed and CW lasers revealed Er and Tm upconversion.

  8. Tuning Crystal Phase and Emission Properties of Upconversion Nanocrystals Through Lanthanide Doping.

    PubMed

    Luo, L; Liu, H B; Yao, L L; Dong, G S; Zhang, W; Wang, Y H; Qiu, Z R; Chen, J

    2016-01-01

    Infrared-to-visible upconversion fluorescent nanocrystals of Yb³⁺/Er³⁺-codoped NaYF₄ and Yb³⁺/Er³⁺/Gd³⁺-tridoped NaYF₄ were synthesized using a modified coprecipitation process. X-ray diffraction and transmission electron diffraction scans of the nanocrystals confirmed that Gd³⁺ doping caused a phase transition to occur in the nanocrystals, changing them from a cubic to a hexagonal phase. Hexagonal phase Yb³⁺/Er³⁺/Gd³⁺-tridoped NaYF₄ nanocrystals displayed much stronger and sharper upconversion luminescence, and larger intensity ratios of red over green emissions relative to their cubic phase counterparts. The influence of the crystal phase on the upconversion emission properties was explored by use of excitation power dependence curves, dynamic fluorescence and Raman spectra. The results suggest that the cubic-to-hexagonal phase transition decreases the crystal field symmetry, and then enhances upconversion luminescence intensity by relaxing forbidden selection rules. The conversion into the hexagonal phase also increases the number of phonon modes, and consequently improves the phonon-assisted energy transfer efficiency from Yb³⁺ to Er³⁺, thus facilitating the output of red emissions. PMID:27398498

  9. Photosynthetic light-harvesting complexes: fluorescent and absorption spectroscopy under two-photon (1200-1500 nm) and one-photon (600-750 nm) excitation by laser femtosecond pulses

    NASA Astrophysics Data System (ADS)

    Stepanenko, Il'ya A.; Kompanets, Viktor O.; Chekalin, Sergey V.; Makhneva, Zoya K.; Moskalenko, Andrey A.; Razjivin, Andrei P.

    2010-09-01

    The pathways of excitation energy transfer (EET) via pigments of the light-harvesting antenna are still in discussion. The bacteriochlorophyll fluorescence of peripheral light-harvesting complexes (LH2) from purple bacteria can be observed upon two-photon excitation (TPE) within 1200-1500 nm spectral range (a broad band near 1300 nm). Earlier the occurrence of this band was taken as an evidence for the participation of "dark" carotenoid S1 state in EET processes (see [Walla et al., Proc. Nat. Acad. Sci. U.S.A. 97, 10808-10813 (2000)] and references in it). However we showed that TPE spectrum of LH2 fluorescence within 1200-1500 nm is not associated with carotenoids [Stepanenko et al., J. Phys. Chem. B. 113(34), 11720-11723 (2009)]. Here we present TPE spectra of fluorescence for chromatophores and lightharvesting complexes LH2 and LH1 from wild-type cells and from carotenoid-depleted or carotenoidless mutant cells of several purple bacteria. The broad band within 1300-1400 nm was found for all preparations. Absorption pump-probe femtosecond spectroscopy applied to LH2 complex from Rb. sphaeroides revealed the similar spectral and kinetic patterns for TPE at 1350 nm and one-photon excitation at 675 nm. Analysis of pigment composition of this complex by high-pressure liquid chromatography showed that even under mild isolation conditions some bacteriochlorophyll molecules were oxidized to 3-acetyl-chlorophyll molecules having the long-wavelength absorption peak in the 650-700 nm range. It is proposed that these 3-acetyl-chlorophyll molecules are responsible for the broad band in TPE spectra within the 1200-1500 nm region.

  10. Photosynthetic light-harvesting complexes: fluorescent and absorption spectroscopy under two-photon (1200-1500 nm) and one-photon (600-750 nm) excitation by laser femtosecond pulses

    NASA Astrophysics Data System (ADS)

    Stepanenko, Il'ya A.; Kompanets, Viktor O.; Chekalin, Sergey V.; Makhneva, Zoya K.; Moskalenko, Andrey A.; Razjivin, Andrei P.

    2011-02-01

    The pathways of excitation energy transfer (EET) via pigments of the light-harvesting antenna are still in discussion. The bacteriochlorophyll fluorescence of peripheral light-harvesting complexes (LH2) from purple bacteria can be observed upon two-photon excitation (TPE) within 1200-1500 nm spectral range (a broad band near 1300 nm). Earlier the occurrence of this band was taken as an evidence for the participation of "dark" carotenoid S1 state in EET processes (see [Walla et al., Proc. Nat. Acad. Sci. U.S.A. 97, 10808-10813 (2000)] and references in it). However we showed that TPE spectrum of LH2 fluorescence within 1200-1500 nm is not associated with carotenoids [Stepanenko et al., J. Phys. Chem. B. 113(34), 11720-11723 (2009)]. Here we present TPE spectra of fluorescence for chromatophores and lightharvesting complexes LH2 and LH1 from wild-type cells and from carotenoid-depleted or carotenoidless mutant cells of several purple bacteria. The broad band within 1300-1400 nm was found for all preparations. Absorption pump-probe femtosecond spectroscopy applied to LH2 complex from Rb. sphaeroides revealed the similar spectral and kinetic patterns for TPE at 1350 nm and one-photon excitation at 675 nm. Analysis of pigment composition of this complex by high-pressure liquid chromatography showed that even under mild isolation conditions some bacteriochlorophyll molecules were oxidized to 3-acetyl-chlorophyll molecules having the long-wavelength absorption peak in the 650-700 nm range. It is proposed that these 3-acetyl-chlorophyll molecules are responsible for the broad band in TPE spectra within the 1200-1500 nm region.

  11. Superresolved femtosecond laser nanosurgery of cells

    PubMed Central

    Pospiech, Matthias; Emons, Moritz; Kuetemeyer, Kai; Heisterkamp, Alexander; Morgner, Uwe

    2011-01-01

    We report on femtosecond nanosurgery of fluorescently labeled structures in cells with a spatially superresolved laser beam. The focal spot width is reduced using phase filtering applied with a programmable phase modulator. A comprehensive statistical analysis of the resulting cuts demonstrates an achievable average resolution enhancement of 30 %. PMID:21339872

  12. Ultrafast Excited-State Dynamics in the Green Fluorescent Protein Variant S65T/H148D. 2. Unusual Photophysical Properties†

    PubMed Central

    Shi, Xinghua; Abbyad, Paul; Shu, Xiaokun; Kallio, Karen; Kanchanawong, Pakorn; Childs, William; Remington, S. James; Boxer, Steven G.

    2008-01-01

    In the preceding accompanying paper (1), the 1.5 Å resolution crystal structure of GFP variant S65T/H148D is presented and the possible consequences of an unusual short hydrogen bond (≤2.4 Å) between the carboxyl oxygen of Asp148 and phenol oxygen of the chromophore are discussed. In this work, we report the femtosecond time-resolved emission of this variant at pH 5.6 by ultrafast fluorescence upconversion spectroscopy. Following excitation at 400 nm, green fluorescence is observed at 510 nm with a rise on a timescale that is faster than the 170 femtosecond instrument response. Time-resolved emission spectra at 140 K also exhibit the immediate appearance of green fluorescence, and this extremely fast process is hardly affected by deuteration of exchangeable protons. These results appear to be dramatically different from those of wild-type GFP, in which the green fluorescence at 508 nm is produced on the picosecond timescale as a result of excited-state proton transfer from the state that is excited at 400 nm. The unique features observed in S65T/H148D and apparent ultrafast excited-state proton transfer are discussed in light of evidence for multiple states underlying the band at around 415 nm, as suggested by steady-state fluorescence spectra. The behavior of these different states may explain the novel photophysical properties observed for this GFP variant, including the ultrafast green fluorescence and the absence of completely matched decay in blue fluorescence. We speculate that two different orientations of the Asp introduced at position 148, not distinguishable by chromatography, mass spectrometry or x-ray crystallography, give rise to the two functionally distinct populations. PMID:17918960

  13. 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.

  14. 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.

  15. 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.

  16. Upconversion Nanoparticles: Synthesis, Surface Modification, and Biological Applications

    PubMed Central

    Wang, Meng; Abbineni, Gopal; Clevenger, April; Mao, Chuanbin; Xu, Shukun

    2011-01-01

    New generation fluorophores, also termed upconversion nanoparticles (UCNPs), have the ability to convert near infrared radiations with lower energy into visible radiations with higher energy via a non-linear optical process. Recently, these UCNPs have evolved as alternative fluorescent labels to traditional fluorophores, showing great potential for imaging and biodetection assays in both in vitro and in vivo applications. UCNPs exhibit unique luminescent properties, including high penetration depth into tissues, low background signals, large Stokes shifts, sharp emission bands, and high resistance to photo-bleaching, making UCNPs an attractive alternative source for overcoming current limitations in traditional fluorescent probes. In this review, we discuss the recent progress in the synthesis and surface modification of rare earth doped UCNPs with a specific focus on their biological applications. PMID:21419877

  17. Engineered Upconversion Nanoparticles for Resolving Protein Interactions inside Living Cells.

    PubMed

    Drees, Christoph; Raj, Athira Naduviledathu; Kurre, Rainer; Busch, Karin B; Haase, Markus; Piehler, Jacob

    2016-09-12

    Upconversion nanoparticles (UCNPs) convert near-infrared into visible light at much lower excitation densities than those used in classic two-photon absorption microscopy. Here, we engineered <50 nm UCNPs for application as efficient lanthanide resonance energy transfer (LRET) donors inside living cells. By optimizing the dopant concentrations and the core-shell structure for higher excitation densities, we observed enhanced UCNP emission as well as strongly increased sensitized acceptor fluorescence. For the application of these UCNPs in complex biological environments, we developed a biocompatible surface coating functionalized with a nanobody recognizing green fluorescent protein (GFP). Thus, rapid and specific targeting to GFP-tagged fusion proteins in the mitochondrial outer membrane and detection of protein interactions by LRET in living cells was achieved. PMID:27510808

  18. Upconversion, size analysis, and fiber filling of NaYF4: Ho3+, Yb3+ crystals and nanocolloids

    NASA Astrophysics Data System (ADS)

    Patel, Darayas; Lewis, Ashley; Wright, Donald; Velentine, Maucus; Lewis, Danielle; Valentine, Ruben; Sarkisov, Sergey

    2014-03-01

    Nano-colloids and nano-crystals doped with ions of rare-earth elements have recently attracted a lot of attention in the scientific community. This attention is due to unique physical, chemical and optical properties attributed to nanometer size of the particles. They have great potential of being used in applications spanning from new types of lasers, especially blue and UV ones, phosphorous display monitors, optical communications, and fluorescence imaging. In this paper we investigate the near-infrared upconversion luminescence in bulk crystals and nanocolloid filled photonic crystal fiber with ytterbium and holmium co-doped NaYF4 phosphor. The phosphor is prepared by using simple co-precipitation synthetic method. The initially prepared phosphor has very week upconversion fluorescence. The fluorescence significantly increased after the phosphor was annealed at a temperature of 600 °C. Nanocolloids of this phosphor were obtained using 1-propanol as solvent and they were utilized as laser filling medium in photonic crystal fibers. Under 980 nm diode laser excitation very strong upconversion signals were obtained for ytterbium and holmium co-doped phosphor at 541 nm, 646 nm and 751 nm. Pump power emissions, laser ablation and size analysis of the particles was conducted to understand the upconversion mechanisms. The particle sizes of the nanocolloids were analyzed using Atomic Force Microscope and Malvern Zetasizer instrument. The reported nanocolloids are good candidates for fluorescent biosensing applications and also as a new laser filling medium in fiber laser.

  19. Up-conversion luminescence polarization control in Er3+-doped NaYF4 nanocrystals

    NASA Astrophysics Data System (ADS)

    Hui, Zhang; Yun-Hua, Yao; Shi-An, Zhang; Chen-Hui, Lu; Zhen-Rong, Sun

    2016-02-01

    We propose a femtosecond laser polarization modulation scheme to control the up-conversion (UC) luminescence in Er3+-doped NaYF4 nanocrystals dispersed in the silicate glass. We show that the UC luminescence can be suppressed when the laser polarization is changed from linear through elliptical to circular, and the higher repetition rate will yield the lower control efficiency. We theoretically analyze the physical control mechanism of the UC luminescence polarization modulation by considering on- and near-resonant two-photon absorption, energy transfer up-conversion, and excited state absorption, and show that the polarization control mainly comes from the contribution of near-resonant two-photon absorption. Furthermore, we propose a method to improve the polarization control efficiency of UC luminescence in rare-earth ions by applying a two-color femtosecond laser field. Project supported by the Young Scientists Fund of the National Natural Science Foundation of China (Grant No. 11304396), the National Natural Science Foundation of China (Grant Nos. 11474096 and 51132004), and the Shanghai Municipal Science and Technology Commission, China (Grant No. 14JC1401500).

  20. Fluorescence Behaviour of an Aluminium Octacarboxy Phthalocyanine--NaYGdF4:Yb/Er Nanoparticle Conjugate.

    PubMed

    Taylor, Jessica; Litwinski, Christian; Nyokong, Tebello; Antunes, Edith

    2015-05-01

    Using a methanol assisted thermal decomposition approach, sphere shaped NaYGdF4:Yb/Er upconversion nanoparticles (UCNPs) were successfully synthesized. The chemical, spectroscopic and fluorescence properties of the UCNPs were fully characterized. Characteristic upconversion fluorescence emissions were produced by the NPs in the green, red and NIR regions and the NPs were also shown to possess paramagnetic properties. The influence of the UCNPs on the spectroscopic and fluorescence properties of an aluminium octacarboxy phthalocyanine AlOCPc was investigated. Covalent conjugation to an AlOCPc resulted in a large blue shift of the phthalocyanine's Q band, which was accompanied by a decrease in the Pc's fluorescence lifetime in DMSO. By combining the phthalocyanine and upconversion nanoparticle, we present a system capable of multimodal imaging, using both the upconversion nanoparticle's and phthalocyanine's emission, and magnetic resonance imaging (as a result of doping the upconversion nanoparticles with Gd(3+) ions). PMID:25744527

  1. Controlled synthesis of uniform and monodisperse upconversion core/mesoporous silica shell nanocomposites for bimodal imaging.

    PubMed

    Liu, Jianan; Bu, Wenbo; Zhang, Shengjian; Chen, Feng; Xing, Huaiyong; Pan, Limin; Zhou, Liangping; Peng, Weijun; Shi, Jianlin

    2012-02-20

    Here we report the design and controlled synthesis of monodisperse and precisely size-controllable UCNP@mSiO(2) nanocomposites smaller than 50 nm by directly coating a mesoporous silica shell (mSiO(2)) on upconversion nanocrystals NaYF(4):Tm/Yb/Gd (UCNPs), which can be used as near-infrared fluorescence and magnetic resonance imaging (MRI) agents and a platform for drug delivery as well. Some key steps such as transferring hydrophobic UCNPs to the water phase by using cetyltrimethylammonium bromide (CTAB), removal of the excess amount of CTAB, and temperature-controlled ultrasonication treatment should be adopted and carefully monitored to obtain uniform upconversion core/mesoporous silica shell nanocomposites. The excellent performance of the core-shell-structured nanocomposite in near-infrared fluorescence and magnetic resonance imaging was also demonstrated. PMID:22252972

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

    PubMed

    Feng, Li; Wu, Yinsu

    2015-05-01

    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. PMID:25703369

  3. 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.

  4. DNA-mediated excitonic upconversion FRET switching

    NASA Astrophysics Data System (ADS)

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

    2015-11-01

    Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy upconversion via upconversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based upconversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an upconversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy upconversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy upconversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.

  5. Stimuli responsive upconversion luminescence nanomaterials and films for various applications.

    PubMed

    Tsang, Ming-Kiu; Bai, Gongxun; Hao, Jianhua

    2015-03-21

    Upconversion luminescence (UCL) refers to nonlinear optical processes, which can convert near-infrared photons to short-wavelength emission. Recent advances in nanotechnology have contributed to the development of photon upconversion materials as promising new generation candidates of fluorescent bioprobes and spectral converters for biomedical and optoelectronic applications. Apart from the remarkable photoluminescence of the materials under photon excitation, some UCL materials may exhibit intrinsic magnetic, ferroelectric, X-ray absorption properties, and so on. These interesting characteristics provide an opportunity for us to couple a single stimulus or multiple stimuli (electric field, magnetic field, X-ray, electron beam, temperature and pH, etc.) to various types of UCL materials. In this review, we will primarily focus on the stimuli responsive properties of UCL materials beyond light-matter interaction, which can aid both fundamental research and widespread applications of the materials. The mechanisms of the response to various stimuli in the UCL materials are discussed. This article will also highlight recent advances in the development of these materials in response to various stimuli and their applications in multimodal bioimaging, drug delivery and release, electro-optical devices, magnetic, temperature and pH sensors and multiple anti-counterfeiting inks. Lastly, we will present potential directions of future research and challenging issues which arise in expanding the applications of stimuli responsive UCL materials. PMID:25200182

  6. [Study on red up-conversion luminescence of fluoride glasses doped with Er3+, Yb3+ and Tm3+].

    PubMed

    Yan, Lei; Liu, Zheng-wei; Yang, Xiao-liang

    2005-06-01

    When the quality of Er2O3 is 10 times the former, the authors found that its character of up-conversion luminescence is distinct. Then the authors studied the luminescence system of Es3+ /Tm3+, Er3+ /Er3+ and Er3+ /Yb3+ /Tm3+ and their character of upconversion and fluorescence spectrum at 980 nm. In addition, the authors studied the relation between the three systems and the consistency of Er2O3. The authors found that the intensity of green and red light changed with the consistence of Er3+ in the experiment. It's the consistence of Er3+ that is the most causative. The chance is equal for each lanthanonion that makes up the luminescence system in the uniformity matter. With the distance between each pair of lanthanonions in the luminescence system is changed, the luminescence system and the color of the up-conversion luminescence also changed. PMID:16201349

  7. Femtosecond Laser Filamentation for Atmospheric Sensing

    PubMed Central

    Xu, Huai Liang; Chin, See Leang

    2011-01-01

    Powerful femtosecond laser pulses propagating in transparent materials result in the formation of self-guided structures called filaments. Such filamentation in air can be controlled to occur at a distance as far as a few kilometers, making it ideally suited for remote sensing of pollutants in the atmosphere. On the one hand, the high intensity inside the filaments can induce the fragmentation of all matters in the path of filaments, resulting in the emission of characteristic fluorescence spectra (fingerprints) from the excited fragments, which can be used for the identification of various substances including chemical and biological species. On the other hand, along with the femtosecond laser filamentation, white-light supercontinuum emission in the infrared to UV range is generated, which can be used as an ideal light source for absorption Lidar. In this paper, we present an overview of recent progress concerning remote sensing of the atmosphere using femtosecond laser filamentation. PMID:22346566

  8. Upconversion Luminescence Properties of Y2Mo4O15: Yb3+, Er3+ by Solid State Combustion Method.

    PubMed

    Jiang, Tao; Xing, Mingming; Fu, Yao; Tian, Ying; Luo, Xixian

    2016-04-01

    The Yb3+ and Er3+ co-doped yttrium molybdenum oxide upconversion phosphors were prepared by the solid state combustion method using urea as fuel at ignition temperature of 550 °C. The upconversion phosphors were characterized by X-ray diffraction (XRD), scanning electronic microscope (SEM), and photoluminescence spectra XRD results revealed the samples were pure monoclinic Y2Mo4O15 phases when the sintering temperature was 700 °C. SEM micrographs illustrated particle size distribution was almost uniform with an average particle diameter of about 0.5-1.0 µm. The obtained Y2MO4O15: Yb3+, Er3+ presents bright and pure green upconversion luminescence during daylight pumping under 980 nm LD. According to the analysis of upconversion luminescent mechanism, the cross relaxation processes of Er3+ ions restrained the electron population of red emission energy level, which not only increased the green light upconversion emissions fluorescent branching ratio (IGIR = 153:1) but also enhanced the efficiency and purity of green light emissions. PMID:27451756

  9. Two-photon spectral fluorescence lifetime and second-harmonic generation imaging of the porcine cornea with a 12-femtosecond laser microscope

    NASA Astrophysics Data System (ADS)

    Batista, Ana; Breunig, Hans Georg; Uchugonova, Aisada; Morgado, António Miguel; König, Karsten

    2016-03-01

    Five dimensional microscopy with a 12-fs laser scanning microscope based on spectrally resolved two-photon autofluorescence lifetime and second-harmonic generation (SHG) imaging was used to characterize all layers of the porcine cornea. This setup allowed the simultaneous excitation of both metabolic cofactors, NAD(P)H and flavins, and their discrimination based on their spectral emission properties and fluorescence decay characteristics. Furthermore, the architecture of the stromal collagen fibrils was assessed by SHG imaging in both forward and backward directions. Information on the metabolic state and the tissue architecture of the porcine cornea were obtained with subcellular resolution, and high temporal and spectral resolutions.

  10. Blue emission from Eu2+-doped high silica glass by near-infrared femtosecond laser irradiation

    NASA Astrophysics Data System (ADS)

    Qiao, Yanbo; Chen, Danping; Ren, Jinjun; Wu, Botao; Qiu, Jianrong; Akai, Tomoko

    2008-01-01

    Eu2+-doped high silica glass (HSG) is fabricated by sintering porous glass which is impregnated with europium ions. Eu2+-doped HSG is revealed to yield intense blue emission excited by ultraviolet (UV) light and near-infrared femtosecond laser. The emission profile obtained by UV excitation can be well traced by near-infrared femtosecond laser. The upconversion emission excited by 800 nm femtosecond laser is considered to be related to a two-photon absorption process from the relationship between the integrated intensity and the pump power. A tentative scheme of upconverted blue emission from Eu2+-doped HSG was also proposed. The HSG materials presented herein are expected to find applications in high density optical storage and three-dimensional color displays.

  11. Autofluorescence-free in vivo multicolor imaging using upconversion fluoride nanocrystals.

    PubMed

    Tian, Zhen; Chen, Guanying; Li, Xiang; Liang, Huijuan; Li, Yuanshi; Zhang, Zhiguo; Tian, Ye

    2010-07-01

    Non-invasive fluorescence imaging is an important technique in biology. However, detection of traditional biomarker emissions is accompanied by a high background signal. In this study we examined whether upconversion sodium yttrium fluoride (NaYF(4)) nanocrystals were suitable for autofluorescence-free multicolor fluorescence imaging in a living animal. Tissue autofluorescence was induced with a 405 nm light source, then rats were subjected to injection of fluorescein isothiocyanate (FITC), cadmium selenide/zinc sulfide (CdSe/ZnS) quantum dots (QDs), or NaYF(4):ytterbium/thulium (Yb(3+)/Tm(3+)), NaYF(4):Yb(3+)/holmium (Ho(3+)), and NaYF(4):Yb(3+)/Ho(3+)/cerium (Ce(3+)) nanocrystals. Imaging with NaYF(4) nanocrystals (974 nm laser) completely removed the high tissue autofluorescence, in marked contrast to imaging with FITC and QDs (405 nm light). Optical imaging experiments demonstrated that multiple biological targets and organs could be imaged at the same time using multicolor NaYF(4) upconversion nanocrystals under a single excitation wavelength (974 nm). These data demonstrated the proof-of-principle that autofluorescence-free multicolor imaging using near-infrared to visible upconversion of NaYF(4) nanocrystals excited by laser can be performed in a living animal. PMID:19322625

  12. Neurotoxin-conjugated upconversion nanoprobes for direct visualization of tumors under near-infrared irradiation.

    PubMed

    Yu, Xue-Feng; Sun, Zhengbo; Li, Min; Xiang, Yang; Wang, Qu-Quan; Tang, Fenfen; Wu, Yingliang; Cao, Zhijian; Li, Wenxin

    2010-11-01

    We report the development of neurotoxin-mediated upconversion nanoprobes for tumor targeting and visualization in living animals. The nanoprobes were synthesized by preparing polyethylenimine-coated hexagonal-phase NaYF(4):Yb,Er/Ce nanoparticles and conjugating them with recombinant chlorotoxin, a typical peptide neurotoxin that could bind with high specificity to many types of cancer cells. Nanoprobes that specifically targeted glioma cells were visualized by laser scanning upconversion fluorescence microscopy. Good probe biocompatibility was displayed with cellular and animal toxicity determinations. Animal studies were performed using Balb-c nude mice injected intravenously with the nanoprobes. The obtained high-contrast images demonstrated highly specific tumor binding and direct tumor visualization with bright red fluorescence under 980-nm near-infrared irradiation. The high sensitivity and high specificity of the neurotoxin-mediated upconversion nanoprobes and the simplification of the required optical device for tumor visualization suggest an approach that may help improve the effectiveness of the diagnostic and therapeutic modalities available for tumor patients. PMID:20728213

  13. 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.

  14. 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. PMID:16378753

  15. Twisting in the excited state of an N-methylpyridinium fluorescent dye modulated by nano-heterogeneous micellar systems.

    PubMed

    Cesaretti, A; Carlotti, B; Gentili, P L; Germani, R; Spalletti, A; Elisei, F

    2016-04-13

    A push-pull N-methylpyridinium fluorescent dye with a pyrenyl group as the electron-donor portion was investigated within the nano-heterogeneous media provided by some micellar systems. The molecule was studied by stationary and time-resolved spectroscopic techniques in spherical micellar solutions and viscoelastic hydrogels, in order to throw light on the role played by twisting in its excited state deactivation. As proven by femtosecond fluorescence up-conversion and transient absorption experiments, the excited state dynamics of the molecule is ruled by charge transfer and twisting processes, which, from the locally excited (LE) state initially populated upon excitation, progressively lead to twisted (TICT) and planar (PICT) intramolecular charge transfer states. The inclusion within micellar aggregates was found to slow down and/or limit the rotation of the molecule with respect to what had previously been observed in water, while its confinement within the hydrophobic domains of the gel matrixes prevents any molecular torsion. The increasing viscosity of the medium, when passing from water to micellar systems, implies that the detected steady-state fluorescence comes from an excited state which is not fully relaxed, as is the case with the TICT state in micelles or the LE state in hydrogels, where the detected emission changes its usual orange colour to yellow. PMID:26982966

  16. [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. PMID:12939954

  17. Dual-band pixelless upconversion imaging devices.

    PubMed

    Wu, Le Ke; Hao, Hui Lian; Shen, Wen Zhong; Ariyawansa, Gamini; Perera, A G Unil; Matsik, Steven G

    2007-08-15

    We have proposed a type of mid-infrared (MIR) and far-infrared (FIR) dual-band imaging device, which employs the photon frequency upconversion concept in a GaN/AlGaN MIR and FIR dual-band detector integrated with a GaN/AlGaN violet light emitting diode. On the basis of the photoresponse of single-period GaN/AlGaN dual-band detectors, we present the detailed optimization of multiperiod GaN emitter/AlGaN barrier detectors and their applications to dual-band pixelless upconversion imaging. Satisfying images have been received through the analysis of the modulation transfer function and the upconversion efficiency in the GaN/AlGaN dual-band pixelless upconverters, which exhibit good image resolution, high quantum efficiency, and negligible cross talk. PMID:17700787

  18. Enhanced UV upconversion emission using plasmonic nanocavities.

    PubMed

    El Halawany, Ahmed; He, Sha; Hodaei, Hossein; Bakry, Ahmed; Razvi, Mir A N; Alshahrie, Ahmed; Johnson, Noah J J; Christodoulides, Demetrios N; Almutairi, Adah; Khajavikhan, Mercedeh

    2016-06-27

    Upconversion of near infrared (NIR) into ultraviolet (UV) radiation could lead to a number of applications in bio-imaging, diagnostics and drug delivery. However, for bare nanoparticles, the conversion efficiency is extremely low. In this work, we experimentally demonstrate strongly enhanced upconversion emission from an ensemble of β-NaYF4:Gd3+/Yb3+/Tm3+ @NaLuF4 core-shell nanoparticles trapped in judiciously designed plasmonic nanocavities. In doing so, different metal platforms and nanostructures are systematically investigated. Our results indicate that using a cross-shape silver nanocavity, a record high enhancement of 170-fold can be obtained in the UV band centered at a wavelength of 345 nm. The observed upconversion efficiency improvement may be attributed to the increased absorption at NIR, the tailored photonic local density of states, and the light out-coupling characteristics of the cavity. PMID:27410563

  19. Luminescence upconversion in colloidal double quantum dots.

    PubMed

    Deutsch, Zvicka; Neeman, Lior; Oron, Dan

    2013-09-01

    Luminescence upconversion nanocrystals capable of converting two low-energy photons into a single photon at a higher energy are sought-after for a variety of applications, including bioimaging and photovoltaic light harvesting. Currently available systems, based on rare-earth-doped dielectrics, are limited in both tunability and absorption cross-section. Here we present colloidal double quantum dots as an alternative nanocrystalline upconversion system, combining the stability of an inorganic crystalline structure with the spectral tunability afforded by quantum confinement. By tailoring its composition and morphology, we form a semiconducting nanostructure in which excited electrons are delocalized over the entire structure, but a double potential well is formed for holes. Upconversion occurs by excitation of an electron in the lower energy transition, followed by intraband absorption of the hole, allowing it to cross the barrier to a higher energy state. An overall conversion efficiency of 0.1% per double excitation event is achieved. PMID:23912060

  20. Tuning the Upconversion Luminescence Lifetimes of KYb2 F7 :Ho(3+) Nanocrystals for Optical Multiplexing.

    PubMed

    Ding, Mingye; Chen, Daqin; Ma, Danyang; Liu, Peng; Song, Kaixin; Lu, Hongwei; Ji, Zhenguo

    2015-12-21

    Conventional luminescent color coding is limited by spectral overlap and the interference of background fluorescence, thus restricting the number of distinguishable identities that can be used in practice. Here, we demonstrate the possibility of generating diverse time-domain codes, specially designed for a single emission band, using lanthanide-doped upconversion nanocrystals. Based on the knowledge of concentration quenching, the upconversion luminescence kinetics of KYb2 F7 : Ho(3+) nanocrystals can be precisely controlled by modifying the dopant concentration of Ho(3+) ions, resulting in a tunable emission lifetime from 75.8 to 1944.5 μs, which suggests the practicality of these time-domain codes for optical multiplexing. PMID:26436998

  1. Characterization and modeling of thulium:ZBLAN blue upconversion fiber lasers

    SciTech Connect

    Paschotta, R.; Barber, P.R.; Tropper, A.C.; Hanna, D.C.

    1997-05-01

    We have investigated the performance of blue upconversion fiber lasers based on thulium-doped ZBLAN fiber, operating at 480 nm with a 1140-nm pump. Extensive fluorescence measurements have provided the necessary spectroscopic data to present a computer model that describes the performance of such lasers with good accuracy despite the complicated three-step upconversion mechanism and the influence of ion{endash}ion energy transfer processes. We have identified the mechanisms that populate the levels above the {sup 1}G{sub 4} level and are able to specify the corresponding spectroscopic parameters. We discuss the relevance of these processes to the 480-nm laser performance. Furthermore, we have calculated optimized parameters for such lasers. {copyright} 1997 Optical Society of America

  2. Femtosecond beam science

    NASA Astrophysics Data System (ADS)

    Uesaka, Mitsuru

    1. Introduction -- 2. Femtosecond beam generation. 2.1. Theory and operation of femtosecond terawatt lasers. 2.2. Linear accelerator. 2.3. Synchrotron. 2.4. Laser plasma acceleration. 2.5. Inverse compton scattering x-ray generation. 2.6. Beam slicing by femtosecond laser. 2.7. Free electron lasers. 2.8. Energy recovery linac -- 3. Diagnosis and synchronization. 3.1. Pulse shape diagnostics. 3.2. Synchronization -- 4. Applications. 4.1. Radiation chemistry. 4.2. Time-resolved x-ray diffraction. 4.3. Protein dynamics. 4.4. Molecular dynamics simulation.

  3. Enhancement of the short wavelength upconversion emission in inverse opal photonic crystals.

    PubMed

    Wu, Hangjun; Zhu, Jialun; Yang, Zhengwen; Yan, Dong; Wang, Rongfei; Qiu, Jianbei; Song, Zhiguo; Yu, Xue; Yang, Yong; Zhou, Dacheng; Yin, Zhaoyi

    2014-05-01

    Upconversion luminescence properties of Yb-Tb codoped Bi4Ti3O12 inverse opals have been investigated. The results show that the upconversion emission can be modulated by the photonic band gap. More significantly, in the upconversion inverse opals, the excited-state absorption of Tb3+ is greatly enhanced by the suppression of upconversion spontaneous emissions of the intermediate excited state, and thus the short wavelength upconversion emission from Tb3+ is considerably improved. We believe that the present work will be valuable for not only the foundational study of upconversion emission modifications but also new optical devices in upconversion displays and short wavelength upconversion lasers. PMID:24734648

  4. Up-conversion luminescence from Er3+, Yb3+ co-doped GeO II-PbF II-Nb IIO 5 glass ceramic

    NASA Astrophysics Data System (ADS)

    Lv, Jinwen; Sang, Lanfen; Zhang, Jing; Fu, Xingguo

    2006-01-01

    The paper reports a new up-conversion luminescence material based on Yb 3+, Er 3+ co-doped germanate glass ceramic, the matrix system is GeO II-PbF II-Nb IIO 5. The luminescence characteristics of the Yb3+ , Er3+ co-doped glass ceramic have been studied. The structural properties of the germinate glass ceramic have been analysed by X-ray diffraction. Under the condition of 980nm semiconductor laser pumping, the green fluorescence intensity shows that the existence of niobate components plays an important role for up-conversion luminescence.

  5. 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. PMID:24051289

  6. Multihydroxy dendritic upconversion nanoparticles with enhanced water dispersibility and surface functionality for bioimaging.

    PubMed

    Zhou, Li; He, Benzhao; Huang, Jiachang; Cheng, Zehong; Xu, Xu; Wei, Chun

    2014-05-28

    Upconversion nanoparticle (UCNP) as a new class of imaging agent is gaining prominence because of its unique optical properties. An ideal UCNP for bioimaging should simultaneously possess fine water dispersibility and favorable functional groups. In this paper, we present a simple but effective method to the synthesis of a UCNP-based nanohybrid bearing a multihydroxy hyperbranched polyglycerol (HPG) shell by the combination of a "grafting from" strategy with a ring-opening polymerization technique. The structure and morphology of the resulting UCNP-g-HPG nanohybrid were characterized in detail by Fourier transform infrared, (1)H NMR, thermogravimetric analysis, and transmission electron microscopy measurements. The results reveal that the amount of grafted HPG associated with the thickness of the HPG shell can be well tuned. UCNP-g-HPG shows high water dispersibility and strong and stable upconversion luminescence. On the basis of its numerous surface hydroxyl groups, UCNP-g-HPG can be tailored by a representative fluorescent dye rhodamine B to afford a UCNP-g-HPG-RB nanohybrid that simultaneously presents upconversion and downconversion luminescence. Preliminary biological studies demonstrate that UCNP-g-HPG shows low cytotoxicity, high luminescent contrast, and deep light penetration depth, posing promising potential for bioimaging applications. PMID:24749852

  7. 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.

  8. Converting visible light into UVC: microbial inactivation by Pr(3+)-activated upconversion materials.

    PubMed

    Cates, Ezra L; Cho, Min; Kim, Jae-Hong

    2011-04-15

    Herein we report the synthesis and properties of light-activated antimicrobial surfaces composed of lanthanide-doped upconversion luminescent nano- and microcrystalline Y(2)SiO(5). Unlike photocatalytic surfaces, which convert light energy into reactive chemical species, this work describes surfaces that inactivate microorganisms through purely optical mechanisms, wherein incident visible light is partially converted into germicidal UVC radiation. Upconversion phosphors utilizing a Pr(3+) activator ion were synthesized and their visible-to-ultraviolet conversion capabilities were confirmed via photoluminescence spectroscopy. Polycrystalline films were prepared on glass substrates, and the extent of surface microbial inactivation and biofilm inhibition under visible light excitation were investigated. Results show that, under normal visible fluorescent lamp exposure, a sufficient amount of UVC radiation was emitted to inhibit Pseudomonas aeruginosa biofilm formation and to inactivate Bacillus subtilis spores on the dry surfaces. This new application of upconversion luminescence shows for the first time its ability to deter microbial contamination and could potentially lead to new material strategies for disinfection of surfaces and water. PMID:21428395

  9. Photon upconversion with hot carriers in plasmonic systems

    SciTech Connect

    Naik, Gururaj V.; Dionne, Jennifer A.

    2015-09-28

    We propose a scheme of photon upconversion based on harnessing the energy of plasmonic hot carriers. Low-energy photons excite hot electrons and hot holes in a plasmonic nanoparticle, which are then injected into an adjacent semiconductor quantum well where they radiatively recombine to emit a photon of higher energy. We theoretically study the proposed upconversion scheme using Fermi-liquid theory and determine the internal quantum efficiency of upconversion to be as high as 25% in 5 nm silver nanocubes. This upconversion scheme is linear in its operation, does not require coherent illumination, offers spectral tunability, and is more efficient than conventional upconverters.

  10. 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. PMID:25155721

  11. Homogeneous assay for whole blood folate using photon upconversion.

    PubMed

    Arppe, Riikka; Mattsson, Leena; Korpi, Krista; Blom, Sami; Wang, Qi; Riuttamäki, Terhi; Soukka, Tero

    2015-02-01

    Red blood cell folate is measured for folate deficiency diagnosis, because it reflects the long-term folate level in tissues, whereas serum folate only represents the dietary intake. Direct homogeneous assay from whole blood would be ideal but conventional fluorescence techniques in blood suffer from high background and strong absorption of light at ultraviolet and visible wavelengths. In this study, a new photon upconversion-based homogeneous assay for whole blood folate is introduced based on resonance energy transfer from upconverting nanophosphor donor coated with folate binding protein to a near-infrared fluorescent acceptor dye conjugated to folate analogue. The sensitized acceptor emission is measured at 740 nm upon 980 nm excitation. Thus, optically transparent wavelengths are utilized for both donor excitation and sensitized acceptor emission to minimize the sample absorption, and anti-Stokes detection completely eliminates the Stokes-shifted autofluorescence. The IC50 value of the assay was 6.0 nM and the limit of detection (LOD) was 1 nM. The measurable concentration range was 2 orders of magnitude between 1.0-100 nM, corresponding to 40-4000 nM folate in the whole blood sample. Recoveries of added folic acid were 112%-114%. A good correlation was found when compared to a competitive heterogeneous assay based on the DELFIA-technology. The introduced assay provides a simple and fast method for whole blood folate measurement. PMID:25548870

  12. IRRS, UV-Vis-NIR absorption and photoluminescence upconversion in Ho 3+-doped oxyfluorophosphate glasses

    NASA Astrophysics Data System (ADS)

    Karmakar, Basudeb

    2005-09-01

    Infrared reflection spectroscopic (IRRS), ultraviolet-visible-near infrared (UV-Vis-NIR) absorption and photoluminescence upconversion properties with special emphasis on the spectrochemistry of the oxyfluorophosphate (oxide incorporated fluorophosphates) glasses of the Ba(PO 3) 2-AlF 3-CaF 2-SrF 2-MgF 2-Ho 2O 3 system have been studied with different concentrations (0.1, 0.3 and 1.0 mol%) of Ho 2O 3. IRRS spectral band position and intensity of Ho 3+ ion doped oxyfluorophosphate glasses have been discussed in terms of reduced mass and force constant. UV-Vis-NIR absorption band position has been justified with quantitative calculation of nephelauxetic parameter and covalent bonding characteristics of the host. NIR to visible upconversion has been investigated by exciting at 892 nm at room temperature. Three upconverted bands originated from the 5F 3→ 5I 8, ( 5S 2, 5F 4)→ 5I 8 and 5F 5→ 5I 8 transitions have found to be centered at 491 nm (blue, medium), 543 nm (green, very strong) and 658 nm (red, weak), respectively. These bands have been justified from the evaluation of the absorption, normal (down conversion) fluorescence and excitation spectra. The upconversion processes have been explained by the excited state absorption (ESA), energy transfer (ET) and cross relaxation (CR) mechanisms involving population of the metastable (storage) energy levels by multiphonon deexcitation effect. It is evident from the IRRS study that the upconversion phenomena are expedited by the low multiphonon relaxation rate in oxyfluorophosphate glasses owing to their high intense low phonon energy (˜600 cm -1) which is very close to that of fluoride glasses (500-600 cm -1).

  13. LOW POWER UPCONVERSION FOR SOLAR FUELS PHOTOCHEMISTRY

    SciTech Connect

    Castellano, Felix N.

    2013-08-05

    Earth abundant copper(I) diimine complexes represent a renewable and economically feasible alternative to commonly used heavy metal containing chromophores. In the metal-to-ligand charge transfer (MLCT) excited state, copper(I) diimine complexes typically undergo a significant structural rearrangement, leading to molecules with large Stokes shifts and very short excited state lifetimes, thereby limiting their usefulness as sensitizers in bimolecular electron and triplet energy transfer reactions. Strategically placed bulky substituents on the coordinating phenanthroline ligands have proven useful in restricting the transiently produced excited state Jahn-Teller distortion, leading to longer-lived excited states. By combining bulky sec-butyl groups in the 2- and 9- positions with methyl groups in the 3-,4-, 7-, and 8- positions, a remarkably long-lived (2.8 μs in DCM) copper(I) bis-phenanthroline complex, [Cu(dsbtmp)2]+, has been synthesized and characterized. Unlike other copper(I) diimine complexes, [Cu(dsbtmp)2]+ also retains a μs lifetime in coordinating solvents such as acetonitrile and water as a result of the cooperative sterics inherent in the molecular design. Preliminary results on the use of this complex in hydrogen-forming homogeneous photocatalysis is presented. Photon upconversion based on sensitized triplet-triplet annihilation (TTA) represents a photochemical means to generate high-energy photons (or high-energy chemical products) from low-energy excitation, having potential applications in solar energy conversion and solar fuels producing devices. For the first time, synthetically facile and earth abundant Cu(I) MLCT sensitizers have been successfully incorporated into two distinct photochemical upconversion schemes, affording both red-to-green and orange-to-blue wavelength conversions. Preliminary results on aqueous-based photochemical upconversion as well as intramolecular Sn(IV) porphyrins containing axially coordinated aromatic hydrocarbon

  14. Photon Upconversion Through Tb(3+) -Mediated Interfacial Energy Transfer.

    PubMed

    Zhou, Bo; Yang, Weifeng; Han, Sanyang; Sun, Qiang; Liu, Xiaogang

    2015-10-28

    A strategy of interfacial energy transfer upconversion is demonstrated through the use of a terbium (Tb(3+) ) dopant as energy donor or energy migrator in core-shell-structured nanocrystals. This mechanistic investigation presents a new pathway for photon upconversion, and, more importantly, contributes to the better control of energy transfer at the nanometer length scale. PMID:26378771

  15. Fluorescence excitation by enhanced plasmon upconversion under continuous wave illumination

    NASA Astrophysics Data System (ADS)

    Tasgin, Mehmet Emre; Salakhutdinov, Ildar; Kendziora, Dania; Abak, Musa Kurtulus; Turkpence, Deniz; Piantanida, Luca; Fruk, Ljiljana; Lazzarino, Marco; Bek, Alpan

    2016-09-01

    We demonstrate effective background-free continuous wave nonlinear optical excitation of molecules that are sandwiched between asymmetrically constructed plasmonic gold nanoparticle clusters. We observe that near infrared photons are converted to visible photons through efficient plasmonic second harmonic generation. Our theoretical model and simulations demonstrate that Fano resonances may be responsible for being able to observe nonlinear conversion using a continuous wave light source. We show that nonlinearity enhancement of plasmonic nanostructures via coupled quantum mechanical oscillators such as molecules can be several orders larger as compared to their classical counterparts.

  16. Photon upconversion sensitized nanoprobes for sensing and imaging of pH

    NASA Astrophysics Data System (ADS)

    Arppe, Riikka; Näreoja, Tuomas; Nylund, Sami; Mattsson, Leena; Koho, Sami; Rosenholm, Jessica M.; Soukka, Tero; Schäferling, Michael

    2014-05-01

    Acidic pH inside cells indicates cellular dysfunctions such as cancer. Therefore, the development of optical pH sensors for measuring and imaging intracellular pH is a demanding challenge. The available pH-sensitive probes are vulnerable to e.g. photobleaching or autofluorescence background in biological materials. Our approach circumvents these problems due to near infrared excitation and upconversion photoluminescence. We introduce a nanosensor based on upconversion resonance energy transfer (UC-RET) between an upconverting nanoparticle (UCNP) and a fluorogenic pH-dependent dye pHrodo™ Red that was covalently bound to the aminosilane surface of the nanoparticles. The sensitized fluorescence of the pHrodo™ Red dye increases strongly with decreasing pH. By referencing the pH-dependent emission of pHrodo™ Red with the pH-insensitive upconversion photoluminescence of the UCNP, we developed a pH-sensor which exhibits a dynamic range from pH 7.2 to 2.5. The applicability of the introduced pH nanosensor for pH imaging was demonstrated by imaging the two emission wavelengths of the nanoprobe in living HeLa cells with a confocal fluorescence microscope upon 980 nm excitation. This demonstrates that the presented pH-nanoprobe can be used as an intracellular pH-sensor due to the unique features of UCNPs: excitation with deeply penetrating near-infrared light, high photostability, lack of autofluorescence and biocompatibility due to an aminosilane coating.Acidic pH inside cells indicates cellular dysfunctions such as cancer. Therefore, the development of optical pH sensors for measuring and imaging intracellular pH is a demanding challenge. The available pH-sensitive probes are vulnerable to e.g. photobleaching or autofluorescence background in biological materials. Our approach circumvents these problems due to near infrared excitation and upconversion photoluminescence. We introduce a nanosensor based on upconversion resonance energy transfer (UC-RET) between an

  17. Optical Temperature Sensor Through Upconversion Emission from the Er3+ Doped SrBi8Ti7O27 Ferroelectrics

    NASA Astrophysics Data System (ADS)

    Zou, Hua; Wang, Xusheng; Hu, Yifeng; Zhu, Xiaoqing; Sui, Yongxing; Song, Zhitang

    2016-06-01

    Er doped SrBi8Ti7O27 (SBT) ferroelectric ceramics were prepared by a solid-state reaction technique. By Er doping, the intensive green upconversion emissions were recorded under 980 nm diode laser excitation with 20 mW. The fluorescence spectrum was investigated in the temperature range of 150-580 K. By the fluorescence intensity ratio technique, the green emission band was studied as a function of temperature with a maximum sensing sensitivity of 0.0028 at 510 K. These results indicate that the Er doped SBT ferroelectric ceramics are promising multifunctional sensing materials.

  18. Efficient up-conversion of triplet excitons into a singlet state and its application for organic light emitting diodes

    NASA Astrophysics Data System (ADS)

    Endo, Ayataka; Sato, Keigo; Yoshimura, Kazuaki; Kai, Takahiro; Kawada, Atsushi; Miyazaki, Hiroshi; Adachi, Chihaya

    2011-02-01

    A material possessing a very small energy gap between its singlet and triplet excited states, ΔE1-3, which allows efficient up-conversion of triplet excitons into a singlet state and leads to efficient thermally activated delayed fluorescence (TADF), is reported. The compound, 2-biphenyl-4,6-bis(12-phenylindolo[2,3-a] carbazole-11-yl)-1,3,5-triazine, breaks the restriction of a large energy gap, with a ΔE1-3 of just 0.11 eV, while maintaining a high fluorescent radiative decay rate (kr˜107). The intense TADF provides a pathway for highly efficient electroluminescence.

  19. Upconversion Nanomaterials: Synthesis, Mechanism, and Applications in Sensing

    PubMed Central

    Chen, Jiao; Zhao, Julia Xiaojun

    2012-01-01

    Upconversion is an optical process that involves the conversion of lower-energy photons into higher-energy photons. It has been extensively studied since mid-1960s and widely applied in optical devices. Over the past decade, high-quality rare earth-doped upconversion nanoparticles have been successfully synthesized with the rapid development of nanotechnology and are becoming more prominent in biological sciences. The synthesis methods are usually phase-based processes, such as thermal decomposition, hydrothermal reaction, and ionic liquids-based synthesis. The main difference between upconversion nanoparticles and other nanomaterials is that they can emit visible light under near infrared irradiation. The near infrared irradiation leads to low autofluorescence, less scattering and absorption, and deep penetration in biological samples. In this review, the synthesis of upconversion nanoparticles and the mechanisms of upconversion process will be discussed, followed by their applications in different areas, especially in the biological field for biosensing. PMID:22736958

  20. Application of upconversion detection to pulsed CO2 lidar

    NASA Technical Reports Server (NTRS)

    Itabe, T.; Bufton, J. L.

    1982-01-01

    In this paper the application of an upconversion detector to pulsed CO2 lidar is investigated. In this device a nonlinear IR crystal would be used to convert 10-micron lidar radiation into the visible region for conventional detection with a photomultiplier tube. A pulsed CO2 lidar can be substantially improved with an upconversion detector configured for rejection of thermal background radiation using a narrowband filter for the upconverted signal or a cold filter front end. The sensitivity of the upconversion detector with the narrowband visible wavelength filter is estimated to be 2 orders of magnitude better than that of the usual direct detection diode. The cold filter can improve upconversion detection to nearly the signal-shot limit. These upconversion detectors are not limited by speckle noise as is a pulsed heterodyne detector.

  1. [High efficiency and low threshold upconversion from IR to red for Er3+ and Tm3+ co-doped fluoride-oxide glass-ceramic].

    PubMed

    Qin, Guan-shi; Qin, Wei-ping; Chen, Bao-jiu; E, Shu-lin; Ge, Zhong-jiu; Ren, Xin-guang; Huang, Shi-hua

    2002-10-01

    In this paper, high efficiency and low threshold upconversion from IR to red is reported, for Er3+ and Tm3+ co-doped fluoride-oxide glass-ceramic under 978 nm LD excitation. The component of sample in experiment is 65GeO2-25NaF-8.5BaF2-1Er2O3-0.5 Tm2O3, and the prepared method is obtained. The upconversion emission spectra under 978 nm LD excitation is measured at room temperature. Analyzing it, we find that introduction of Tm3+ into Er3+ doped system preferentially quenches the green upconversion fluorescence from 4S3/2 level of Er3+ duo to the efficient cross-relaxation of 4I13/2-->4I15/2 (Er): 3H6-->3H4 (Tm) which can significantly reduce the upconversion efficiency from 4I13/2 level to the emitting 4S3/2 level, and the Tm3+ behaves as a good sensitizer of the red upconversion from the 4F9/2 level of Er3+ which is mainly populated by the cross-relaxation of 3H4-->3H6 (Tm): 4I11/2-->4F9/2 (Er). However, at low Er3+ concentration (2 mol%), it is impossible for strong red upconversion. X-ray analysis is done, there are lots of nanocrystallites in MFG glass-ceramic. So we think, this red upconversion is attributed to Er3+ enriched fluoride microcrystallites, which makes the cross-relaxation of 3H4-->3H6 (Tm): 4I11/2-->4F9/2 (Er) more effective, therefore their active optical properties may be optimised. In the end, the relationship between LD working current and intensity of upconversion luminescence is discussed, the results confirm that both red and green upconversion processes are consisted by two photons. PMID:12938407

  2. Reduced erbium-doped ceria nanoparticles: one nano-host applicable for simultaneous optical down- and up-conversions

    PubMed Central

    2014-01-01

    This paper introduces a new synthesis procedure to form erbium-doped ceria nanoparticles (EDC NPs) that can act as an optical medium for both up-conversion and down-conversion in the same time. This synthesis process results qualitatively in a high concentration of Ce3+ ions required to obtain high fluorescence efficiency in the down-conversion process. Simultaneously, the synthesized nanoparticles contain the molecular energy levels of erbium that are required for up-conversion. Therefore, the synthesized EDC NPs can emit visible light when excited with either UV or IR photons. This opens new opportunities for applications where emission of light via both up- and down-conversions from a single nanomaterial is desired such as solar cells and bio-imaging. PMID:24940173

  3. 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

  4. Hemifusion of cells using femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Katchinskiy, Nir; Godbout, Roseline; Goez, Helly R.; Elezzabi, Abdulhakem Y.

    2015-03-01

    Attachment of single cells via hemifusion of cellular membranes using femtosecond laser pulses is reported in this manuscript. This is a method to attach single cells using sub-10 femtosecond laser pulses, with 800 nm central wavelength delivered from a Ti:Sapphire laser is described. A fluorescent dye, Calcein AM, was used to verify that the cell's cytoplasm did not migrate from a dyed cell to a non-dyed cell, in order to ascertain that the cells did not go through cell-fusion process. An optical tweezer was used in order to assess the mechanical integrity of the attached joint membranes. Hemifusion of cellular membranes was successful without initiating full cell fusion. Attachment efficiency of 95% was achieved, while the cells' viability was preserved. The attachment was performed via the delivery of one to two trains of sub-10 femtosecond laser pulses lasting 15 milliseconds each. An ultrafast reversible destabilization of the phospholipid molecules in the cellular membranes was induced due to a laser-induced ionization process. The inner phospholipid cell membrane remained intact during the attachment procedure, and cells' cytoplasm remained isolated from the surrounding medium. The unbounded inner phospholipid molecules bonded to the nearest free phospholipid molecule, forming a joint cellular membrane at the connection point. The cellular membrane hemifusion technique can potentially provide a platform for the creation of engineered tissue and cell cultures.

  5. Bioapplications and biotechnologies of upconversion nanoparticle-based nanosensors.

    PubMed

    Wang, Chengli; Li, Xiaomin; Zhang, Fan

    2016-06-21

    Upconversion nanoparticles (UCNPs), which can emit ultraviolet/visible (UV/Vis) light under near-infrared (NIR) excitation, are regarded as a new generation of nanoprobes because of their unique optical properties, including a virtually zero auto-fluorescence background for the improved signal-to-noise ratio, narrow emission bandwidths and high resistance to photo-bleaching. These properties make UCNPs promising candidates as luminescent bioprobes in biomedicine and biotechnology. In this review, we focus on the recent progress in the development of UCNP-based nanoprobes for biosensing. Firstly, as the FRET process is a widely used method for biosensing to improve the sensitivity, we summarize recent research studies about UCNP-based nanocomposites utilizing the FRET process for biosensing. Different energy acceptors (organic dyes, noble metal nanoparticles, carbon nanomaterials and semiconductor nanomaterials) with their own advantages and limitations are well summarized in this review. Secondly, since UCNPs have been utilized for the detection of different kinds of analytes, we introduce recent research studies about UCNPs for ions, gas molecules, biomolecules and thermal sensing. Finally, we highlight the typical detection techniques and UCNP based devices for bioapplications. PMID:26978012

  6. Photoluminescence and upconversion on Ag/CdTe quantum dots

    NASA Astrophysics Data System (ADS)

    Ragab, A. E.; Gadallah, A.-S.; Mohamed, M. B.; Azzouz, I. M.

    2014-11-01

    Different sizes of aqueous CdTe QDs have been prepared by microwave via controlling the temperature and time of irradiation. To study the plasmonic effect on CdTe QDs, Silver NPs were prepared by using a chemical reduction method. Structure characterization of the nanocrystals (Ag NPs and CdTe QDs) was determined by transmission electron microscopy “TEM”. For optical characterization, the absorption and photolumincence (PL) spectra were measured. It has been found that there are two opposite behaviors (quenching and enhancement) in the fluorescence spectra based on the spectral coupling strength between Ag NPs and CdTe QDs. When there is strong overlapping, PL enhancement of CdTe QDs has been observed. On the other hand, when the overlapping is weak, the PL quenching was predominant at all Ag NPS concentrations. Input-output PL intensity dependence was also studied. Upconversion photoluminescence with low excitation intensity was observed in our CdTe QDs with a standard spectrofluorometer at excitation wavelength of 800 nm. Thermally assisted surface state mechanism has been proposed to be responsible for the upconverion process.

  7. Quantitative Imaging of Single Upconversion Nanoparticles in Biological Tissue

    PubMed Central

    Nadort, Annemarie; Sreenivasan, Varun K. A.; Song, Zhen; Grebenik, Ekaterina A.; Nechaev, Andrei V.; Semchishen, Vladimir A.; Panchenko, Vladislav Y.; Zvyagin, Andrei V.

    2013-01-01

    The unique luminescent properties of new-generation synthetic nanomaterials, upconversion nanoparticles (UCNPs), enabled high-contrast optical biomedical imaging by suppressing the crowded background of biological tissue autofluorescence and evading high tissue absorption. This raised high expectations on the UCNP utilities for intracellular and deep tissue imaging, such as whole animal imaging. At the same time, the critical nonlinear dependence of the UCNP luminescence on the excitation intensity results in dramatic signal reduction at (∼1 cm) depth in biological tissue. Here, we report on the experimental and theoretical investigation of this trade-off aiming at the identification of optimal application niches of UCNPs e.g. biological liquids and subsurface tissue layers. As an example of such applications, we report on single UCNP imaging through a layer of hemolyzed blood. To extend this result towards in vivo applications, we quantified the optical properties of single UCNPs and theoretically analyzed the prospects of single-particle detectability in live scattering and absorbing bio-tissue using a human skin model. The model predicts that a single 70-nm UCNP would be detectable at skin depths up to 400 µm, unlike a hardly detectable single fluorescent (fluorescein) dye molecule. UCNP-assisted imaging in the ballistic regime thus allows for excellent applications niches, where high sensitivity is the key requirement. PMID:23691012

  8. G-Quadruplex Supramolecular Assemblies in Photochemical Upconversion.

    PubMed

    Mutsamwira, Saymore; Ainscough, Eric W; Partridge, Ashton C; Derrick, Peter J; Filichev, Vyacheslav V

    2016-07-18

    Parallel, tetramolecular G-quadruplex (G4) DNA possessing TINA monomer, (R)-1-O-[4-(1-pyrenylethynyl)phenylmethyl]glycerol, were synthesised and evaluated in complexes with tris(2,2'-bipyridine)ruthenium(II), [Ru(bpy)3 ](2+) , and the Zn(2+) derivative of 5,10,15,20-tetrakis-(1-methyl-4-pyridyl)-21 H,23H-porphine, ZnTMpyP4. UV/Vis, fluorescence, and circular dichroism (CD) spectroscopy showed that the use of G4-DNA as a template resulted in the effective communication between the ligands and the TINA molecule that was covalently attached to the 5'-end and between T and dG at the 5'-end of the dTG4 T sequence. Only one G4-DNA possessing the TINA molecule at the 5'-end of the dTG4 T sequence was able to yield a green-to-blue photochemical upconversion (PUC, λem =420 nm) in the presence of [Ru(bpy)3 ](2+) upon excitation at 500 nm. Different DNA secondary structures can thus be used in DNA-based assemblies for PUC and the way of attachment of chromophores to DNA plays a pivotal role for the creation of a photosynthetic centre. PMID:27172273

  9. Femtosecond laser materials processing

    SciTech Connect

    Stuart, B.C.

    1997-02-01

    The use femtosecond pulses for materials processing results in very precise cutting and drilling with high efficiency. Energy deposited in the electrons is not coupled into the bulk during the pulse, resulting in negligible shock or thermal loading to adjacent areas.

  10. Molecularly imprinted upconversion nanoparticles for highly selective and sensitive sensing of Cytochrome c.

    PubMed

    Guo, Ting; Deng, Qiliang; Fang, Guozhen; Liu, Cuicui; Huang, Xuan; Wang, Shuo

    2015-12-15

    A novel method combined the high selectivity of molecular imprinting technology with the strong fluorescence property of upconversion nanoparticles (UCNPs) for sensing of Cytochrome c (Cyt c) was proposed. The molecularly imprinted material-coated upconversion nanoparticles (UCNPs@MIP) were obtained by in situ coating Cyt c imprinted materials to the surface of the carboxyl modified UCNPs through sol-gel technique. The structure and component of the prepared UCNPs@MIP was investigated by transmission electron microscopy (TEM), power X-ray diffraction (XRD), energy-dispersive X-ray analysis (EDXA) and X-ray photoelectron spectroscopic (XPS). The TEM showed the diameter of UCNPs was 40 nm, and thickness of MIP was 5-10nm. The fluorescence intensity of UCNPs@MIP reduced gradually with the increase of Cyt c concentration. Under optimum conditions, the imprinting factor is 3.19, and the UCNPs@MIP showed selective recognition for Cyt c among other proteins such as bovine serum albumin (BSA) and Lysozyme (Lyz). Therefore, this new method for sensing protein is very promising for future applications. PMID:26176210

  11. Polymer encapsulated upconversion nanoparticle/iron oxide nanocomposites for multimodal imaging and magnetic targeted drug delivery.

    PubMed

    Xu, Huan; Cheng, Liang; Wang, Chao; Ma, Xinxing; Li, Yonggang; Liu, Zhuang

    2011-12-01

    Multimodal imaging and imaging-guided therapies have become a new trend in the current development of cancer theranostics. In this work, we encapsulate hydrophobic upconversion nanoparticles (UCNPs) together with iron oxide nanoparticles (IONPs) by using an amphiphilic block copolymer, poly (styrene-block-allyl alcohol) (PS(16)-b-PAA(10)), via a microemulsion method, obtaining an UC-IO@Polymer multi-functional nanocomposite system. Fluorescent dye and anti-cancer drug molecules can be further loaded inside the UC-IO@Polymer nanocomposite for additional functionalities. Utilizing the Squaraine (SQ) dye loaded nanocomposite (UC-IO@Polymer-SQ), triple-modal upconversion luminescence (UCL)/down-conversion fluorescence (FL)/magnetic resonance (MR) imaging is demonstrated in vitro and in vivo, and also applied for in vivo cancer cell tracking in mice. On the other hand, a chemotherapy drug, doxorubicin, is also loaded into the nanocomposite, forming an UC-IO@Polymer-DOX complex, which enables novel imaging-guided and magnetic targeted drug delivery. Our work provides a method to fabricate a nanocomposite system with highly integrated functionalities for multimodal biomedical imaging and cancer therapy. PMID:21880364

  12. Adaptive Femtosecond Quantum Control

    NASA Astrophysics Data System (ADS)

    Gerber, Gustav

    2003-03-01

    Obtaining active control over the dynamics of quantum-mechanical systems is a fascinating perspective in modern physics. A promising tool for this purpose is available with femtosecond laser technologies. The intrinsically broad spectral distribution and the phase function of femtosecond laser pulses can be specifically manipulated by pulse shapers to drive molecular systems coherently into the desired reaction pathways [1]. The approach of adaptive femtosecond quantum control follows the suggestion of Judson and Rabitz [2], in which a computer-controlled pulse shaper is used in combination with a learning algorithm [3] and direct feedback from the experiment to achieve coherent control over quantum-mechanical processes in an automated fashion, without requiring any model for the system's response. This technique can be applied to the control of gas-phase photodissociation processes [4]. Different bond-cleaving reactions can be preferentially selected, resulting in chemically different products. Prior knowledge about molecular Hamiltonians or reaction mechanisms is not required in this automated control loop, and this scheme works for complex systems. Adaptive pulse-shaping techniques can be transferred to the control of photoprocesses in the liquid phase as well, motivated by the wish to achieve control at particle densities high enough for (bimolecular) synthetic-chemical applications. Chemically selective molecular excitation is achieved by many-parameter adaptive quantum control [5], despite the failure of typical single-parameter approaches (such as wavelength control, intensity control, or linear chirp control). This experiment demonstrates that photoprocesses in two different molecular species can be controlled simultaneously. Applications are envisioned in bimolecular reaction control where specific educt molecules could selectively be "activated" for purposes of chemical synthesis. A new technological development further increases the possibilities and

  13. Solar upconversion with plasmonic hot carriers

    NASA Astrophysics Data System (ADS)

    Dionne, Jennifer A.

    Upconversion of sub-bandgap photons is a promising approach to exceed the Shockley-Queisser limit in solar technologies. Placed behind a solar cell, upconverting materials convert lower-energy photons transmitted through the cell to higher-energy above-bandgap photons that can then be absorbed by the cell and contribute to photocurrent. Because the upconverter is electrically isolated from the active cell, it need not be current-matched to the cell, nor will it add mid-gap recombination pathways. Calculations have indicated that single-junction cell efficiencies can exceed 44% upon addition of an upconverter - a significant improvement over the maximum cell efficiency of 30% without an upconverter. However, due to the low quantum efficiencies and narrow absorption bandwidths of existing upconverters, such significant cell improvements have yet to be observed experimentally. In this presentation, we will describe an entirely new solar upconverting scheme based on hot-carrier injection from a plasmonic absorber to an adjacent semiconductor. The plasmonic system both induces upconversion based on injection of hot-electrons and hot-holes and also enhances light-matter interactions. Low-energy photons incident on a plasmonic particle generate hot electrons and hot holes, which are injected into a semiconducting quantum well and subsequently radiatively recombine. Importantly, the bandgap of the quantum well can be higher than the energy of the incident photon, enabling emission of a higher-energy photon than that absorbed. First, we present analytic calculations showing that efficiencies as high as 25% are possible, significantly higher than existing solid-state upconverters, which are only 2-5% efficient. We also describe how further improvements in the efficiency are possible by employing materials and geometries that allow for more efficient carrier injection. Then, we describe experiments on InGaN/GaN quantum wells decorated with Au disks. On their own, the In

  14. Hybrid upconversion nanomaterials for optogenetic neuronal control

    NASA Astrophysics Data System (ADS)

    Shah, Shreyas; Liu, Jing-Jing; Pasquale, Nicholas; Lai, Jinping; McGowan, Heather; Pang, Zhiping P.; Lee, Ki-Bum

    2015-10-01

    Nanotechnology-based approaches offer the chemical control required to develop precision tools suitable for applications in neuroscience. We report a novel approach employing hybrid upconversion nanomaterials, combined with the photoresponsive ion channel channelrhodopsin-2 (ChR2), to achieve near-infrared light (NIR)-mediated optogenetic control of neuronal activity. Current optogenetic methodologies rely on using visible light (e.g. 470 nm blue light), which tends to exhibit high scattering and low tissue penetration, to activate ChR2. In contrast, our approach enables the use of 980 nm NIR light, which addresses the short-comings of visible light as an excitation source. This was facilitated by embedding upconversion nanomaterials, which can convert NIR light to blue luminescence, into polymeric scaffolds. These hybrid nanomaterial scaffolds allowed for NIR-mediated neuronal stimulation, with comparable efficiency as that of 470 nm blue light. Our platform was optimized for NIR-mediated optogenetic control by balancing multiple physicochemical properties of the nanomaterial (e.g. size, morphology, structure, emission spectra, concentration), thus providing an early demonstration of rationally-designing nanomaterial-based strategies for advanced neural applications.Nanotechnology-based approaches offer the chemical control required to develop precision tools suitable for applications in neuroscience. We report a novel approach employing hybrid upconversion nanomaterials, combined with the photoresponsive ion channel channelrhodopsin-2 (ChR2), to achieve near-infrared light (NIR)-mediated optogenetic control of neuronal activity. Current optogenetic methodologies rely on using visible light (e.g. 470 nm blue light), which tends to exhibit high scattering and low tissue penetration, to activate ChR2. In contrast, our approach enables the use of 980 nm NIR light, which addresses the short-comings of visible light as an excitation source. This was facilitated by

  15. Y2O3:Tm,Yb nanophosphors for correlative upconversion luminescence and cathodoluminescence imaging.

    PubMed

    Fukushima, Shoichiro; Furukawa, Taichi; Niioka, Hirohiko; Ichimiya, Masayoshi; Miyake, Jun; Ashida, Masaaki; Araki, Tsutomu; Hashimoto, Mamoru

    2014-12-01

    We present a phosphor nanoparticle that shows both upconversion luminescence (UCL) and cathodoluminescence (CL). With this particle, low-autofluorescence, deep-tissue and wide-field fluorescence imaging can be achieved with nanometer-order high-spatial-resolution imaging. We synthesized Y2O3:Tm,Yb nanophosphors that emit visible and near-infrared UCL under 980 nm irradiation and blue CL via electron beam excitation. The phosphors were applied to fluorescent imaging of HeLa cells. The photostability of the phosphors was superior to that of a conventional organic dye. We show that after uptake by HeLa cells, the particles can be imaged with SEM and CL contrast in a cellular section. This indicates that correlative UCL and CL imaging of biological samples could be realized. PMID:25146422

  16. Photo-induced electron transfer in a diamino-substituted Ru(bpy)3[PF6]2 complex and its application as a triplet photosensitizer for nitric oxide (NO)-activated triplet-triplet annihilation upconversion.

    PubMed

    Xu, Kejing; Zhao, Jianzhang; Moore, Evan G

    2016-08-01

    A system demonstrating Nitric Oxide (NO) activated Triplet-Triplet Annihilation (TTA) upconversion has been devised, based on a substituted [Ru(II)(bpy)3](PF6)2 complex (bpy = 2,2'-dipyridine) bearing a single 1,2-diaminophenyl moiety as an NO activatable triplet photosensitizer (Ru-1), and 9,10-diphenylanthracene (DPA) as a triplet acceptor/emitter. The excited triplet state of Ru-1 is significantly quenched (ΦT∼ 22%) by a Photoinduced Electron Transfer (PET) reaction, as confirmed by steady state phosphorescence and transient absorption spectroscopy, and hence Ru-1 does not function as a TTA upconversion sensitizer. However, in the presence of NO/O2, the 1,2-diaminophenyl group of Ru-1 is transformed into a benzotriazole. This inhibits PET, and the triplet state quantum yield is increased to ca. 85%, switching on the TTA upconversion process which increases by 10-fold. These processes were studied using a combination of steady state and time-resolved luminescence together with transient absorption spectroscopy on the nanosecond and femtosecond timescales. The energy level of the charge transfer state (CTS) for Ru-1 was also obtained electrochemically, supporting the PET mechanism of triplet state quenching and hence the lack of TTA upconversion with Ru-1. PMID:27387268

  17. Lanthanide upconversion luminescence at the nanoscale: fundamentals and optical properties.

    PubMed

    Nadort, Annemarie; Zhao, Jiangbo; Goldys, Ewa M

    2016-07-01

    Upconversion photoluminescence is a nonlinear effect where multiple lower energy excitation photons produce higher energy emission photons. This fundamentally interesting process has many applications in biomedical imaging, light source and display technology, and solar energy harvesting. In this review we discuss the underlying physical principles and their modelling using rate equations. We discuss how the understanding of photophysical processes enabled a strategic influence over the optical properties of upconversion especially in rationally designed materials. We subsequently present an overview of recent experimental strategies to control and optimize the optical properties of upconversion nanoparticles, focussing on their emission spectral properties and brightness. PMID:26986473

  18. Lanthanide upconversion luminescence at the nanoscale: fundamentals and optical properties

    NASA Astrophysics Data System (ADS)

    Nadort, Annemarie; Zhao, Jiangbo; Goldys, Ewa M.

    2016-07-01

    Upconversion photoluminescence is a nonlinear effect where multiple lower energy excitation photons produce higher energy emission photons. This fundamentally interesting process has many applications in biomedical imaging, light source and display technology, and solar energy harvesting. In this review we discuss the underlying physical principles and their modelling using rate equations. We discuss how the understanding of photophysical processes enabled a strategic influence over the optical properties of upconversion especially in rationally designed materials. We subsequently present an overview of recent experimental strategies to control and optimize the optical properties of upconversion nanoparticles, focussing on their emission spectral properties and brightness.

  19. Silver nanoclusters emitting weak NIR fluorescence biomineralized by BSA

    NASA Astrophysics Data System (ADS)

    Li, Baoshun; Li, Jianjun; Zhao, Junwu

    2015-01-01

    Noble metal (e.g., gold and silver) nanomaterials possess unique physical and chemical properties. In present work, silver nanoclusters (also known as silver quantum clusters or silver quantum dots) were synthesized by bovine serum albumin (BSA) biomineralization. The synthesized silver nanoclusters were characterized by UV-VIS absorption spectroscopy, fluorescence spectroscopy, upconversion emission spectroscopy, TEM, HRTEM and FTIR spectroscopy. TEM results showed that the average size of the silver nanoclusters was 2.23 nm. Fluorescence results showed that these silver nanoclusters could emit weak near-infrared (NIR) fluorescence (the central emission wavelength being about 765 nm). And the central excitation wavelength was about 395 nm, in the UV spectral region. These silver nanoclusters showed an extraordinarily large gap (about 370 nm) between the central excitation wavelength and central emission wavelength. In addition, it was found that these silver nanoclusters possess upconversion emission property. Upconversion emission results showed that the upconversion emission spectrum of the silver nanoclusters agreed well with their normal fluorescence emission spectrum. The synthesized silver nanoclusters showed high stability in aqueous solution and it was considered that they might be confined in BSA molecules. It was found that silver nanoclusters might enhance and broaden the absorption of proteins, and the protein absorption peak showed an obvious red shift (being 7 nm) after the formation of silver nanoclusters.

  20. Optical gene transfer by femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Konig, Karsten; Riemann, Iris; Tirlapur, Uday K.

    2003-07-01

    Targeted transfection of cells is an important technique for gene therapy and related biomedical applications. We delineate how high-intensity (1012 W/cm2) near-infrared (NIR) 80 MHz nanojoule femtosecond laser pulses can create highly localised membrane perforations within a minute focal volume, enabling non-invasive direct transfection of mammalian cells with DNA. We suspended Chinese hamster ovarian (CHO), rat kangaroo kidney epithelial (PtK2) and rat fibroblast cells in 0.5 ml culture medium in a sterile miniaturized cell chamber (JenLab GmbH, Jena, Germany) containing 0.2 μg plasmid DNA vector pEGFP-N1 (4.7 kb), which codes for green fluorescent protein (GFP). The NIR laser beam was introduced into a femtosecond laser scanning microscope (JenLab GmbH, Jena, Germany; focussed on the edge of the cell membrane of a target cell for 16 ms. The integration and expression efficiency of EGFP were assessed in situ by two-photon fluorescence-lifetime imaging using time-correlated single photon counting. The unique capability to transfer foreign DNA safely and efficiently into specific cell types (including stem cells), circumventing mechanical, electrical or chemical means, will have many applications, such as targeted gene therapy and DNA vaccination.

  1. Upconversion studies in Gd2O3:Tm3+/Yb3+ phosphor

    NASA Astrophysics Data System (ADS)

    Singh, A. K.; Kumar, K.; Rai, S. B.; Rai, D. K.

    2013-06-01

    The Tm3+/Yb3+ doped Gd2O3 phosphor is prepared through combustion technique and its visible upconversion emission studies are made on 980 nm near infrared excitation. The upconversion studied showed good upconversion emission in blue region (477nm) but the highest emission intensity was observed at 802 nm wavelength. The Tm3+ ion concentration dependence of upconversion emission intensity studies are also done and optimum concentration of Tm3+ ion is found 0.2mol% for blue upconversion. The power dependence studies are also made to know the process of upconversion emission.

  2. Upconversion Nanoparticles for Bioimaging and Regenerative Medicine.

    PubMed

    González-Béjar, María; Francés-Soriano, Laura; Pérez-Prieto, Julia

    2016-01-01

    Nanomaterials are proving useful for regenerative medicine in combination with stem cell therapy. Nanoparticles (NPs) can be administrated and targeted to desired tissues or organs and subsequently be used in non-invasive real-time visualization and tracking of cells by means of different imaging techniques, can act as therapeutic agent nanocarriers, and can also serve as scaffolds to guide the growth of new tissue. NPs can be of different chemical nature, such as gold, iron oxide, cadmium selenide, and carbon, and have the potential to be used in regenerative medicine. However, there are still many issues to be solved, such as toxicity, stability, and resident time. Upconversion NPs have relevant properties such as (i) low toxicity, (ii) capability to absorb light in an optical region where absorption in tissues is minimal and penetration is optimal (note they can also be designed to emit in the near-infrared region), and (iii) they can be used in multiplexing and multimodal imaging. An overview on the potentiality of upconversion materials in regenerative medicine is given. PMID:27379231

  3. Upconversion Nanoparticles for Bioimaging and Regenerative Medicine

    PubMed Central

    González-Béjar, María; Francés-Soriano, Laura; Pérez-Prieto, Julia

    2016-01-01

    Nanomaterials are proving useful for regenerative medicine in combination with stem cell therapy. Nanoparticles (NPs) can be administrated and targeted to desired tissues or organs and subsequently be used in non-invasive real-time visualization and tracking of cells by means of different imaging techniques, can act as therapeutic agent nanocarriers, and can also serve as scaffolds to guide the growth of new tissue. NPs can be of different chemical nature, such as gold, iron oxide, cadmium selenide, and carbon, and have the potential to be used in regenerative medicine. However, there are still many issues to be solved, such as toxicity, stability, and resident time. Upconversion NPs have relevant properties such as (i) low toxicity, (ii) capability to absorb light in an optical region where absorption in tissues is minimal and penetration is optimal (note they can also be designed to emit in the near-infrared region), and (iii) they can be used in multiplexing and multimodal imaging. An overview on the potentiality of upconversion materials in regenerative medicine is given. PMID:27379231

  4. Magnetic nanosensor particles in luminescence upconversion capability.

    PubMed

    Wilhelm, Stefan; Hirsch, Thomas; Scheucher, Elisabeth; Mayr, Torsten; Wolfbeis, Otto S

    2011-09-01

    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). PMID:22022719

  5. [Femtosecond lenticule extraction (FLEx)].

    PubMed

    Blum, M; Sekundo, W

    2010-10-01

    Starting in 2006 a new "all femto" method of refractive correction for myopia and myopic astigmatism was introduced. This new method was originally introduced as femtosecond lenticule extraction (FLEx) and further developed with a small incision into SMILE (small incision lenticule extraction). To simplify the terminology the manufacturer brought this onto the market in April 2010 as ReLEx (refractive lenticule extraction). In this procedure a lenticule of intrastromal corneal tissue and a flap-like access cut are subsequently cut utilizing the VisuMax® femtosecond system (Carl Zeiss Meditec, Jena, Germany). The lenticule is then manually removed and the flap repositioned (only by FLEx). In approximately 1,000 successful surgical operations only few side effects were found. The number of eyes treated is currently being expanded in order to further standardize this new clinical procedure. PMID:20694728

  6. Femtosecond Laser Materials Processing

    SciTech Connect

    Banks, P.S.; Stuart, B.C.; Komashko, A.M.; Feit, M.D.; Rubenchik, A.M.; Perry, M.D.

    2000-03-06

    The use of femtosecond lasers allows materials processing of practically any material with extremely high precision and minimal collateral damage. Advantages over conventional laser machining (using pulses longer than a few tens of picoseconds) are realized by depositing the laser energy into the electrons of the material on a time scale short compared to the transfer time of this energy to the bulk of the material, resulting in increased ablation efficiency and negligible shock or thermal stress. The improvement in the morphology by using femtosecond pulses rather than nanosecond pulses has been studied in numerous materials from biologic materials to dielectrics to metals. During the drilling process, we have observed the onset of small channels which drill faster than the surrounding material.

  7. Ligand-centred fluorescence and electronic relaxation cascade at vibrational time scales in transition-metal complexes.

    PubMed

    Messina, Fabrizio; Pomarico, Enrico; Silatani, Mahsa; Baranoff, Etienne; Chergui, Majed

    2015-11-19

    Using femtosecond-resolved photoluminescence up-conversion, we report the observation of the fluorescence of the high-lying ligand-centered (LC) electronic state upon 266 nm excitation of an iridium complex, Ir(ppy)3, with a lifetime of 70 ± 10 fs. It is accompanied by a simultaneous emission of all lower-lying electronic states, except the lowest triplet metal-to-ligand charge-transfer ((3)MLCT) state that shows a rise on the same time scale. Thus, we observe the departure, the intermediate steps, and the arrival of the relaxation cascade spanning ∼1.6 eV from the (1)LC state to the lowest (3)MLCT state, which then yields the long-lived luminescence of the molecule. This represents the first measurement of the total relaxation time over an entire cascade of electronic states in a polyatomic molecule. We find that the relaxation cascade proceeds in ≤10 fs, which is faster than some of the highest-frequency modes of the system. We invoke the participation of the latter modes in conical intersections and their overdamping to low-frequency intramolecular modes. On the basis of literature, we also conclude that this behavior is not specific to transition-metal complexes but also applies to organic molecules. PMID:26509329

  8. Femtosecond laser materials processing

    SciTech Connect

    Stuart, B. C., LLNL

    1998-06-02

    Femtosecond lasers enable materials processing of most any material with extremely high precision and negligible shock or thermal loading to the surrounding area Applications ranging from drilling teeth to cutting explosives to making high-aspect ratio cuts in metals with no heat-affected zone are made possible by this technology For material removal at reasonable rates, we developed a fully computer-controlled 15-Watt average power, 100-fs laser machining system.

  9. Growth, characterization and upconversion properties of erbium-doped potassium lithium tantalate niobate single crystals under 975 nm laser excitation

    NASA Astrophysics Data System (ADS)

    Zhou, Zhongxiang; Li, Lei; Duan, Qianqian; Feng, Lei; Tian, Hao

    2012-04-01

    Potassium lithium tantalate niobate single crystals doped with erbium ions are grown by top-seeded solution growth method. The crystals are characterized by X-ray diffraction and differential thermal analysis. The refractive indices of the crystal are measured using ellipsometry method and fitted by Sellmeier equation. The as-grown crystals are tetragonal phase tungsten bronze-type structure with Curie temperature of 271.3 °C. Characteristic Er3 + absorption bands are observed from 350 to 1100 nm in ultraviolet-visible-near infrared absorption spectra. These crystals emit brightly green and red upconversion fluorescence under 975 nm LD laser excitation, and the steady state upconversion spectra are obtained at room temperature. The red emission intensity increases as the erbium ions concentration increases in crystals. Processes of excited state absorption and energy transfer are responsible for upconversion luminescence. The emission intensities are quadratic dependences on pump power from pump power dependence analyses and deduction of transition rate equation model.

  10. Enhanced upconversion luminescence through core/shell structures and its application for detecting organic dyes in opaque fishes.

    PubMed

    Hu, Pan; Wu, Xiaofeng; Hu, Shigang; Chen, Zenghui; Yan, Huanyuan; Xi, Zaifang; Yu, Yi; Dai, Gangtao; Liu, Yunxin

    2016-02-10

    Here, we report the enhanced upconversion luminescence of NaLuF4:18%Yb(3+),2%Er(3+) through core/shell structures. Among NaYF4, NaGdF4, and NaLuF4 shells, the first one presents the highest efficiency. These upconversion fluorescent nanoprobes with an oleic acid/PEG hybrid ligand can efficiently capture Rhodamine B (RB) and sodium fluorescein (SF) in opaque fishes to present their residues in vivo through luminescence resonant energy transfer (LRET) processes. It can be confirmed based on LRET technology that no RB is absorbed by opaque fishes after incubating in the aqueous solution of 1 μg ml(-1) RB for one day, while SF residue can be obviously detected after incubating in the aqueous solution of 1 μg ml(-1) SF for one day. The merit of this LRET technology with the upconversion nanoparticle (UCNP) donor is ascribed to the deep penetration depth of the infrared pumping laser and high signal to noise ratio. PMID:26806612

  11. 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. PMID:27376560

  12. Fabrication and upconversion luminescence properties of YF3:Er3+ hollow nanofibers via monoaxial electrospinning combined with fluorination method.

    PubMed

    Li, Dan; Dong, Xiangting; Yu, Wensheng; Wang, Jinxian; Liu, Guixia

    2014-06-01

    YF3:Er3+ hollow nanofibers were successfully fabricated via fluorination of the relevant Y2O3:Er3+ hollow nanofibers which were obtained by calcining the electrospun PVP/[Y(NO3)3 + Er(NO3)3] composite nanofibers. The morphology and properties of the products were investigated in detail by X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscope (TEM), and fluorescence spectrometer. YF3:Er3+ hollow nanofibers were pure orthorhombic phase with space group Pnma and were hollow-centered structure with the mean diameter of 172 +/- 23 nm, and YF3:Er3+ hollow nanofibers were composed of nanoparticles with the diameter ranging from 30 nm to 50 nm. Upconversion emission spectrum analysis manifested that YF3:Er3+ hollow nanofibers emitted strong green and weak red upconversion emission centering at 524 nm, 543 nm and 653 nm, respectively. The green emissions and the red emission were respectively originated from 2H11/2/4S3/2 --> 4I15/2 and 4F9/2 --> 4I15/2 energy levels transitions of the Er3+ ions. Moreover, the emitting colors of YF3:Er3+ hollow nanofibers were located in the green region in CIE chromaticity coordinates diagram. The luminescent intensity of YF3:Er3+ hollow nanofibers was increased remarkably with the increasing doping concentration of Er3+ ions. The possible formation mechanism of YF3:Er3+ upconversion luminescence hollow nanofibers was also discussed. This preparation technique could be applied to prepare other rare earth fluoride upconversion luminescence hollow nanofibers. PMID:24738372

  13. Nile Red Derivative-Modified Nanostructure for Upconversion Luminescence Sensing and Intracellular Detection of Fe(3+) and MR Imaging.

    PubMed

    Wei, Ruoyan; Wei, Zuwu; Sun, Lining; Zhang, Jin Z; Liu, Jinliang; Ge, Xiaoqian; Shi, Liyi

    2016-01-13

    Iron ion (Fe(3+)) which is the physiologically most abundant and versatile transition metal in biological systems, has been closely related to many certain cancers, metabolism, and dysfunction of organs, such as the liver, heart, and pancreas. In this Research Article, a novel Nile red derivative (NRD) fluorescent probe was synthesized and, in conjunction with polymer-modified core-shell upconversion nanoparticles (UCNPs), demonstrated in the detection of Fe(3+) ion with high sensitivity and selectivity. The core-shell UCNPs were surface modified using a synthesized PEGylated amphiphilic polymer (C18PMH-mPEG), and the resulting mPEG modified core-shell UCNPs (mPEG-UCNPs) show good water solubility. The overall Fe(3+)-responsive upconversion luminescence nanostructure was fabricated by linking the NRD to the mPEG-UCNPs, denoted as mPEG-UCNPs-NRD. In the nanostructure, the core-shell UCNPs, NaYF4:Yb,Er,Tm@NaGdF4, serve as the energy donor while the Fe(3+)-responsive NRD as the energy acceptor, which leads to efficient luminescence resonance energy transfer (LRET). The mPEG-UCNPs-NRD nanostructure shows high selectivity and sensitivity for detecting Fe(3+) in water. In addition, benefited from the good biocompatibility, the nanostructure was successfully applied for detecting Fe(3+) in living cells based on upconversion luminescence (UCL) from the UCNPs. Furthermore, the doped Gd(3+) ion in the UCNPs endows the mPEG-UCNPs-NRD nanostructure with effective T1 signal enhancement, making it a potential magnetic resonance imaging (MRI) contrast agent. This work demonstrates a simple yet powerful strategy to combine metal ion sensing with multimodal bioimaging based on upconversion luminescence for biomedical applications. PMID:26702512

  14. Advances in femtosecond laser technology

    PubMed Central

    Callou, Thais Pinheiro; Garcia, Renato; Mukai, Adriana; Giacomin, Natalia T; de Souza, Rodrigo Guimarães; Bechara, Samir J

    2016-01-01

    Femtosecond laser technology has become widely adopted by ophthalmic surgeons. The purpose of this study is to discuss applications and advantages of femtosecond lasers over traditional manual techniques, and related unique complications in cataract surgery and corneal refractive surgical procedures, including: LASIK flap creation, intracorneal ring segment implantation, presbyopic treatments, keratoplasty, astigmatic keratotomy, and intrastromal lenticule procedures. PMID:27143847

  15. Advances in femtosecond laser technology.

    PubMed

    Callou, Thais Pinheiro; Garcia, Renato; Mukai, Adriana; Giacomin, Natalia T; de Souza, Rodrigo Guimarães; Bechara, Samir J

    2016-01-01

    Femtosecond laser technology has become widely adopted by ophthalmic surgeons. The purpose of this study is to discuss applications and advantages of femtosecond lasers over traditional manual techniques, and related unique complications in cataract surgery and corneal refractive surgical procedures, including: LASIK flap creation, intracorneal ring segment implantation, presbyopic treatments, keratoplasty, astigmatic keratotomy, and intrastromal lenticule procedures. PMID:27143847

  16. Polyacrylic acid modified upconversion nanoparticles for simultaneous pH-triggered drug delivery and release imaging.

    PubMed

    Jia, Xuekun; Yin, Jinjin; He, Dinggeng; He, Xiaoxiao; Wang, Kemin; Chen, Mian; Li, Yuhong

    2013-12-01

    A poly(acrylicacid)-modified NaYF4:Yb, Er upconversion nanoparticles (PAA-UCNPs) with dual functions of drug delivery and release imaging have been successfully developed. The PAA polymer coated on the surface of UCNPs serve as a pH-sensitive nanovalve for loading drug molecules via electrostatic interaction. The drug-loading efficiency of the PAA-UCNPs was investigated by using doxorubicin hydrochloride (DOX) as a model anticancer drug to evaluate their potential as a delivery system. Results showed loading and releasing of DOX from PAA-UCNPs were controlled by varying pH, with high encapsulation rate at weak alkaline conditions and an increased drug dissociation rate in acidic environment, which is favorable for construct a pH-responsive controlled drug delivery system. The in vitro cytotoxicity test using HeLa cell line indicated that the DOX loaded PAA-UCNPs (DOX@PAA-UCNPs) were distinctly cytotoxic to HeLa cells, while the PAA-UCNPs were highly biocompatible and suitable to use as drug carriers. Furthermore, the upconversion fluorescence resonance energy transfer (UFRET) imaging through the two-photon laser scanning microscopy (TLSM) revealed the time course of intracellular delivery of DOX from DOX@PAA-UCNPs. Thus, PAA-UCNPs are effective for constructing pH-responsive controlled drug delivery systems for multi-functional cancer therapy and imaging. PMID:24266261

  17. Enhancing the Imaging and Biosafety of Upconversion Nanoparticles through Phosphonate Coating

    PubMed Central

    Li, Ruibin; Ji, Zhaoxia; Dong, Juyao; Chang, Chong Hyun; Wang, Xiang; Sun, Bingbing; Wang, Meiying; Liao, Yu-Pei; Zink, Jeffrey I.; Nel, Andre E.; Xia, Tian

    2015-01-01

    Upconversion nanoparticles (UCNPs), which are generated by doping with rare earth (RE) metals, are increasingly used for bio-imaging because of the advantages they hold over conventional fluorophores. However, because pristine RE nanoparticles (NPs) are unstable in acidic physiological fluids (e.g., lysosomes), leading to intracellular phosphate complexation with the possibility of the lysosomal injury, it is important to ensure that UCNPs are safe designed. In this study, we used commercially available NaYF4: Er/Yb UCNPs to study their stability in lysosomes and simulated lysosomal fluid. We demonstrate that phosphate complexation leads to REPO4 deposition on the particle surfaces and morphological transformation. This leads to a decline in upconversion fluorescence efficiency as well as inducing pro-inflammatory effects at cellular level and in the intact lung. In order to preserve the imaging properties of the UCNPs as well as improve their safety, we experimented with a series of phosphonate chemical moieties to passivate particle surfaces through the strong coordination of the organophosphates with RE atoms. Particle screening and physicochemical characterization revealed that ethylenediaminetetra methylenephosphonic acid (EDTMP) surface coating provides the most stable UCNPs, which maintain their imaging intensity and do not induce pro-inflammatory effects in vitro and in vivo. In summary, phosphonate coating presents a safer design method that preserves and improves the bio-imaging properties of UCNPs, thereby enhancing their biological use. PMID:25727446

  18. Visible upconversion fiber lasers in ring configuration

    NASA Astrophysics Data System (ADS)

    Caspary, Reinhard; Baraniecki, Tomasz P.; Kozak, Marcin M.; Kowalsky, Wolfgang

    2005-09-01

    Up-conversion fiber lasers based on Pr3+/Yb3+ doped fluoride fibers and pumped at 835 nm can operate on emission lines in the red, orange, green, and blue spectral region. Up to now only Fabry-Perot configurations with two mirrors butt-coupled to the fiber ends were investigated. In this paper we present the first visible Pr3+/Yb3+ fiber lasers in a ring configuration. In contrast to the usual Fabry-Perot configuration, the basic ring resonator setup contains no free-space optics and no parts which need to be adjusted. The main challenge for such a setup is the connection between the fluoride laser fiber and the remaining part of the ring resonator, which is made from silica fibers. Due to the very different melting temperatures of both glasses usual fusion splices are impossible. We use a special technique to couple the fibers with glue.

  19. Energy pooling upconversion in organic molecular systems.

    PubMed

    LaCount, Michael D; Weingarten, Daniel; Hu, Nan; Shaheen, Sean E; van de Lagemaat, Jao; Rumbles, Garry; Walba, David M; Lusk, Mark T

    2015-04-30

    A combination of molecular quantum electrodynamics, perturbation theory, and ab initio calculations was used to create a computational methodology capable of estimating the rate of three-body singlet upconversion in organic molecular assemblies. The approach was applied to quantify the conditions under which such relaxation rates, known as energy pooling, become meaningful for two test systems, stilbene-fluorescein and hexabenzocoronene-oligothiophene. Both exhibit low intramolecular conversion, but intermolecular configurations exist in which pooling efficiency is at least 90% when placed in competition with more conventional relaxation pathways. For stilbene-fluorescein, the results are consistent with data generated in an earlier experimental investigation. Exercising these model systems facilitated the development of a set of design rules for the optimization of energy pooling. PMID:25793313

  20. Upconversion luminescence behavior of single nanoparticles

    NASA Astrophysics Data System (ADS)

    Zhou, Jiajia; Xu, Shiqing; Zhang, Junjie; Qiu, Jianrong

    2015-09-01

    Upconversion nanoparticles (UCNPs) have made a significant and valuable contribution to materials science, photophysics, and biomedicine due to their specific spectroscopic characteristics. However, the ensemble spectroscopy of UCNPs is limited because of the electronic behavior in average effect, which ignores the fact that these nanoparticles are heterogeneous. With regards to the research focus on heterogeneous intrinsic structures, unique photophysical phenomena, and advanced applications, the optical characterization of single UCNPs have been promoted to the frontier development of the UCNPs community. In this review, we give an overview of the importance of single UCNPs characterization, typical principles of UC, and single particle detection methods. Considerable emphasis is placed on the specific spectroscopic study of single UCNPs, which shows fantastic photophysical phenomena beyond ensemble measurement. Parallel efforts are devoted to the current applications of single UCNPs.

  1. Femtosecond laser cataract surgery.

    PubMed

    Nagy, Zoltan Z; McAlinden, Colm

    2015-01-01

    Femtosecond laser (FSL) cataract surgery is in its infancy but is rapidly gaining popularity due to the improved consistency and predictability for corneal incisions and anterior capsulorhexis. It enables subsequently less phacoemulsification energy and time to be employed, which has gains in terms of reduced corneal oedema. In addition, the FSL allows better circularity of the anterior capsulotomy, capsule overlap, intraocular lens (IOL) placement and centration of the IOL. These advantages have resulted in improved visual and refractive outcomes in the short term. Complication rates are low which reduce with surgeon experience. This review article focuses on the Alcon LenSx system. PMID:26605364

  2. Femtosecond polarization pulse shaping.

    PubMed

    Brixner, T; Gerber, G

    2001-04-15

    We report computer-controlled femtosecond polarization pulse shaping where intensity, momentary frequency, and light polarization are varied as functions of time. For the first time to our knowledge, a pulse shaper is used to modulate the degree of ellipticity as well as the orientation of the elliptical principal axes within a single laser pulse by use of a 256-pixel two-layer liquid-crystal display inside a zero-dispersion compressor. Interferometric stability of the setup is not required. Complete pulse characterization is achieved by dual-channel spectral interferometry. This technology has a large range of applications, especially in the field of quantum control. PMID:18040384

  3. Phase and Size Controllable Synthesis of NaYbF4 Nanocrystals in Oleic Acid/ Ionic Liquid Two-Phase System for Targeted Fluorescent Imaging of Gastric Cancer

    PubMed Central

    Pan, Liyuan; He, Meng; Ma, Jiebing; Tang, Wei; Gao, Guo; He, Rong; Su, Haichuan; Cui, Daxiang

    2013-01-01

    Upconversion nanocrystals with small size and strong fluorescent signals own great potential in applications such as biomolecule-labeling, in vivo tracking and molecular imaging. Herein we reported that NaYbF4: 25%Gd, 2%Tm upconversion nanocrystals with small size and strong fluorescent signals were controllably synthesized by oleic acid (OA)/ ionic liquid (IL) two-phase system for targeted fluorescent imaging of gastric cancer in vivo. The optimal synthesis condition of NaYbF4: 25%Gd, 2%Tm upconversion nanocrystals by OA/IL two-phase system was established, adding more metal ion such as Na+ ion could facilitate the size control and crystal-phase transition, more importantly, markedly enhancing fluorescent intensity of beta-phase nanocrystals compared with traditional methods. Alpha-phase NaYbF4, 2%Tm upconversion nanocrystals with less than 10nm in diameter and beta-phase NaYbF4: 25%Gd, 2%Tm upconversion nanocrystals with 30 nm or so in diameter and strong fluorescent signals were obtained, these synthesized nanocrystals exhibited very low cytotoxicity. Folic acid-conjugated silica-modified beta-phase NaYbF4: 25%Gd, 2%Tm upconversion nanocrystals were prepared, could actively target gastric cancer tissues implanted into nude mice in vivo, and realized targeted fluorescent imaging. Folic acid-conjugated silica-modified NaYbF4: 25%Gd, 2%Tm upconversion nanocrystals show great potential in applications such as targeted near infared radiation fluorescent imaging, magnetic resonance imaging and targeted therapy of gastric cancer in the near future. PMID:23471455

  4. 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

  5. Fabrication of a novel nanocomposite Ag/graphene@SiO2-NaLuF4:Yb,Gd,Er for large enhancement upconversion luminescence.

    PubMed

    Yin, Dongguang; Cao, Xianzhang; Zhang, Lu; Tang, Jingxiu; Huang, Wenfeng; Han, Yanlin; Wu, Minghong

    2015-06-28

    Upconversion nanocrystals have a lot of advantages over other fluorescent materials. However, their applications are still limited due to their comparatively low upconversion luminescence (UCL). In the present study, a novel nanocomposite of Ag/graphene@SiO2-NaLuF4:Yb,Gd,Er for enhancing UCL was fabricated successfully, and its morphology, crystalline phase, composition, and fluorescent property were investigated. It is interesting to find that the Ag/graphene@SiO2-NaLuF4:Yb,Gd,Er and Ag@SiO2-NaLuF4:Yb,Gd,Er nanocomposites showed high UCL enhancements of 52- and 10-fold compared to the control of Ag-free nanocomposite SiO2-NaLuF4:Yb,Gd,Er, respectively. The enhancement of 52-fold is greater than those reported in our previous studies and some papers. Moreover, the measured life times of the Ag-presented nanocrystals were longer than that of Ag-absent counterparts. These enhancements of UCL can be ascribed to the effect of metal-enhanced fluorescence, which is caused by the enhancement of the local electric field. The UCL intensity of Ag/graphene@SiO2-NaLuF4:Yb,Gd,Er was 5.2-fold higher than that of Ag@SiO2-NaLuF4:Yb,Gd,Er, indicating that graphene presented in the fabricated nanocomposite structure favors metal-enhanced UCL. The small-sized Ag nanoparticles anchored on the graphene sheet mutually enhanced each other's polarizability and surface plasmon resonance, resulting in a big metal-enhanced UCL. This study provides a new strategy for effectively enhancing the UCL of upconversion nanocrystals. The enhancement potentially increases the overall upconversion nanocrystal detectability for highly sensitive biological, medical, and optical detections. PMID:25999289

  6. Time-domain upconversion measurements of group-velocity dispersion in quantum cascade lasers.

    PubMed

    Choi, Hyunyong; Diehl, Laurent; Capasso, Federico; Bour, David; Corzine, Scott; Zhu, Jintian; Hofler, Gloria; Norris, Theodore B

    2007-11-26

    A time-resolved mid-infrared upconversion technique based on sum-frequency generation was applied to measure pulse propagation in lambda approximately 5.0 mum quantum cascade lasers operated in continuous wave at 30 K. The wavelength-dependent propagation delay of femtosecond mid-infrared pulses was measured to determine the total group-velocity dispersion. The material and waveguide dispersion were calculated and their contributions to the total group-velocity dispersion were found to be relatively small and constant. The small-signal gain dispersion was estimated from a measurement of the electroluminescence spectrum without a laser cavity, and was found to be the largest component of the total GVD. A negative group-velocity dispersion of beta2 ( =d2beta/d omega2) approximately - 4.6x10-6 ps2/mum was observed at the peak emission wavelength, and good agreement was found for the measured and calculated pulse-broadening. PMID:19550877

  7. Theory of femtosecond stimulated Raman spectroscopy.

    PubMed

    Lee, Soo-Y; Zhang, Donghui; McCamant, David W; Kukura, Philipp; Mathies, Richard A

    2004-08-22

    Femtosecond broadband stimulated Raman spectroscopy (FSRS) is a new technique that produces high-resolution (time-resolved) vibrational spectra from either the ground or excited electronic states of molecules, free from background fluorescence. FSRS uses simultaneously a narrow bandwidth approximately 1-3 ps Raman pump pulse with a continuum approximately 30-50 fs Stokes probe pulse to produce sharp Raman gains, at positions corresponding to vibrational transitions in the sample, riding on top of the continuum Stokes probe spectrum. When FSRS is preceded by a femtosecond actinic pump pulse that initiates the photochemistry of interest, time-resolved Raman spectroscopy can be carried out. We present two theoretical approaches to FSRS: one is based on a coupling of Raman pump and probe light waves with the vibrations in the medium, and another is a quantum-mechanical description. The latter approach is used to discuss the conditions of applicability and limitations of the coupled-wave description. Extension of the quantum-mechanical description to the case where the Raman pump beam is on resonance with an excited electronic state, as well as when FSRS is used to probe a nonstationary vibrational wave packet prepared by an actinic pump pulse, is also discussed. PMID:15303930

  8. Three-dimensional micro-printing of temperature sensors based on up-conversion luminescence

    SciTech Connect

    Wickberg, Andreas; Mueller, Jonathan B.; Mange, Yatin J.; Nann, Thomas; Fischer, Joachim; Wegener, Martin

    2015-03-30

    The pronounced temperature dependence of up-conversion luminescence from nanoparticles doped with rare-earth elements enables local temperature measurements. By mixing these nanoparticles into a commercially available photoresist containing the low-fluorescence photo-initiator Irgacure 369, and by using three-dimensional direct laser writing, we show that micrometer sized local temperature sensors can be positioned lithographically as desired. Positioning is possible in pre-structured environments, e.g., within buried microfluidic channels or on optical or electronic chips. We use the latter as an example and demonstrate the measurement for both free space and waveguide-coupled excitation and detection. For the free space setting, we achieve a temperature standard deviation of 0.5 K at a time resolution of 1 s.

  9. Regiospecific Hetero-Assembly of DNA-Functionalized Plasmonic Upconversion Superstructures

    PubMed Central

    2015-01-01

    We report a novel strategy for regiospecific hetero-assembly of DNA-modified gold nanoparticles (DNA-AuNPs) onto upconversion nanoparticles (UCNPs) into hybrid lab-on-a-particle systems. The DNA-AuNPs have been assembled onto the hexagonal plate-like UCNPs with well-regulated stoichiometry and controlled organization onto the different facets of UCNP, forming various addressable superstructures. The fine-tuning of stoichiometry and organization is realized by biorecognition specificity of DNA toward specific crystal facets of UCNPs. Such a hetero-assembled DNA-AuNP/UCNP system maintains both plasmonic resonance of AuNPs and fluorescent properties of UCNPs, allowing targeted dual-modality imaging of cancer cells using an aptamer. PMID:25853565

  10. Regiospecific Hetero-Assembly of DNA-Functionalized Plasmonic Upconversion Superstructures.

    PubMed

    Li, Le-Le; Lu, Yi

    2015-04-29

    We report a novel strategy for regiospecific hetero-assembly of DNA-modified gold nanoparticles (DNA-AuNPs) onto upconversion nanoparticles (UCNPs) into hybrid lab-on-a-particle systems. The DNA-AuNPs have been assembled onto the hexagonal plate-like UCNPs with well-regulated stoichiometry and controlled organization onto the different facets of UCNP, forming various addressable superstructures. The fine-tuning of stoichiometry and organization is realized by biorecognition specificity of DNA toward specific crystal facets of UCNPs. Such a hetero-assembled DNA-AuNP/UCNP system maintains both plasmonic resonance of AuNPs and fluorescent properties of UCNPs, allowing targeted dual-modality imaging of cancer cells using an aptamer. PMID:25853565

  11. Monitoring femtosecond laser microscopic photothermolysis with multimodal microscopy (Conference Presentation)

    NASA Astrophysics Data System (ADS)

    Huang, Yimei; Lui, Harvey; Zhao, Jianhua; McLean, David I.; Zeng, Haishan

    2016-02-01

    Photothermolysis induced by femtosecond (fs) lasers may be a promising modality in dermatology because of its advantages of high precision due to multiphoton absorption and deeper penetration due to the use of near infrared wavelengths. Although multiphoton absorption nonlinear effects are capable of precision targeting, the femtosecond laser photothermolysis could still have effects beyond the targeted area if a sufficiently high dose of laser light is used. Such unintended effects could be minimized by real time monitoring photothermolysis during the treatment. Targeted photothermolytic treatment of ex vivo mouse skin dermis was performed with tightly focused fs laser beams. Images of reflectance confocal microscopy (RCM), second harmonic generation (SHG), and two-photon fluorescence (TPF) of the mouse skins were obtained with integrated multimodal microscopy before, during, and after the laser treatment. The RCM, SHG, and TPF signal intensities of the treatment areas changed after high power femtosecond laser irradiation. The intensities of the RCM and SHG signals decreased when the tissue was damaged, while the intensity of the TPF signal increased when the photothermolysis was achieved. Moreover, the TPF signal was more susceptible to the degree of the photothermolysis than the RCM and SHG signals. The results suggested that multimodal microscopy is a potentially useful tool to monitor and assess the femtosecond laser treatment of the skin to achieve microscopic photothermolysis with high precision.

  12. Blue Upconversion Luminescence in Tm3+/Yb3+-Codoped Lead Chloride Tellurite Glass

    NASA Astrophysics Data System (ADS)

    Xu, Shi-Qing; Zhang, Jun-Jie; Wang, Guo-Nian; Dai, Shi-Xun; Hu, Li-Li; Jiang, Zhong-Hong

    2004-05-01

    The upconversion properties of Tm3+/Yb3+-codoped lead chloride tellurite glass under 980 nm excitation were investigated. The intense blue (476 nm) emission and weak red (649 nm) emission corresponding to the 1G4rightarrow3H6 and 1G4rightarrow3H4 transitions of Tm3+ ions, respectively, were simultaneously observed at room temperature. The dependence of upconversion intensities on excitation power and the possible upconversion mechanisms are evaluated. The intense blue upconversion luminescence of Tm3+/Yb3+-codoped lead chloride tellurite glass can be used as potential host material for the development of blue upconversion optical devices.

  13. Upconversion luminescence properties of nanocrystallite MgAl2O4 spinel doped with Ho3+ and Yb3+ ions

    NASA Astrophysics Data System (ADS)

    Watras, A.; Dereń, P. J.; Pązik, R.; Maleszka-Bagińska, K.

    2012-10-01

    The upconversion luminescence spectra of nanocrystallite MgAl2O4 doped with 1% of Ho3+ and 5% of Yb3+ ions after excitation at 980 nm were measured. Influence of excitation regime either continuous or pulse on upconversion mechanisms was shown. For continuous wave (CW) laser excitation upconversion process is due to phonon assisted Excited State Absorption (ESA). For pulse laser excitation upconversion emission is due to Energy Transfer Upconversion (ETU).

  14. Laser induced thermal effect on upconversion luminescence and temperature-dependent upconversion mechanism in Ho3+/Yb3+-codoped Gd2(WO4)3 phosphor

    NASA Astrophysics Data System (ADS)

    Liu, Wei; Sun, Jiashi; Li, Xiangping; Zhang, Jinsu; Tian, Yue; Fu, Shaobo; Zhong, Hua; Liu, Tianhong; Cheng, Lihong; Zhong, Haiyang; Xia, Haiping; Dong, Bin; Hua, Ruinian; Zhang, Xiangqing; Chen, Baojiu

    2013-05-01

    Sub-micro sized Gd2(WO4)3:Yb3+/Ho3+ phosphor was synthesized via a co-precipitation reaction. The crystal structure and morphology of the phosphor were characterized by XRD and SEM. The time scanning of green and red upconversion emissions displayed that the upconversion luminescent intensities were dependent on the irradiation time and the excitation powder, which was resulted from the thermal effect induced by LD (laser diode) irradiation. The upconversion luminescence of Gd2(WO4)3:Yb3+/Ho3+ phosphor at different sample temperatures was studied. It was found that at room temperature the red and green upconversion emissions were 1.5- and 2-photon processes, respectively. With increasing sample temperature the 2-photon process for the red upconversion emission and 3-photon process for green upconversion emission occurred.

  15. Fluorescence from rubrene single crystals: Interplay of singlet fission and energy trapping

    NASA Astrophysics Data System (ADS)

    Ma, Lin; Zhang, Keke; Kloc, Christian; Sun, Handong; Soci, Cesare; Michel-Beyerle, Maria E.; Gurzadyan, Gagik G.

    2013-05-01

    We have studied fluorescence in rubrene single crystals by use of fluorescence up-conversion, fluorescence anisotropy, and temperature-dependent time-resolved fluorescence techniques. Thermally activated singlet fission was demonstrated to play an important role in the quenching of two intrinsic fluorescence bands, 565 and 610 nm. At low temperatures, singlet fission is suppressed while another process, namely energy trapping, becomes pronounced. The 650 nm fluorescence originates from the hole trap states located 0.27 eV above the valence band.

  16. Enhanced upconversion luminescence in NaGdF4:Yb,Er nanocrystals by Fe3+ doping and their application in bioimaging

    NASA Astrophysics Data System (ADS)

    Ramasamy, Parthiban; Chandra, Prakash; Rhee, Seog Woo; Kim, Jinkwon

    2013-08-01

    The visible green and red upconversion emissions in Er3+/Yb3+ doped β-NaGdF4 nanoparticles were enhanced by tridoping with Fe3+ ions (0-40 mol%). XRD, XPS, ICP-AES and EDS data demonstrated successful incorporation of Fe3+ ions in NaGdF4:Yb3+/Er3+ nanoparticles. The effect of Fe3+ tridoping on the upconversion luminescence in NaGdF4:Yb3+/Er3+ NPs was investigated in detail. The green and red emission intensities were enhanced by 34 and 30 times, respectively. The maximum emission was observed in a sample containing 30 mol% Fe3+ ions. A possible mechanism for the enhanced upconversion emission is proposed. In addition, a layer of silica was coated onto the surface of UCNPs to improve the biocompatibility. Folic acid was covalently linked to the silica coated UCNPs to form UCNP@SiO2-FA nanoprobes, which have been successfully applied to the fluorescent imaging HeLa cells.The visible green and red upconversion emissions in Er3+/Yb3+ doped β-NaGdF4 nanoparticles were enhanced by tridoping with Fe3+ ions (0-40 mol%). XRD, XPS, ICP-AES and EDS data demonstrated successful incorporation of Fe3+ ions in NaGdF4:Yb3+/Er3+ nanoparticles. The effect of Fe3+ tridoping on the upconversion luminescence in NaGdF4:Yb3+/Er3+ NPs was investigated in detail. The green and red emission intensities were enhanced by 34 and 30 times, respectively. The maximum emission was observed in a sample containing 30 mol% Fe3+ ions. A possible mechanism for the enhanced upconversion emission is proposed. In addition, a layer of silica was coated onto the surface of UCNPs to improve the biocompatibility. Folic acid was covalently linked to the silica coated UCNPs to form UCNP@SiO2-FA nanoprobes, which have been successfully applied to the fluorescent imaging HeLa cells. Electronic supplementary information (ESI) available: EDS spectrum, mechanism of enhanced UC emission, XPS data, and TEM images and PL spectra of UCNPs@SiO2 NPs. See DOI: 10.1039/c3nr01608k

  17. Femtosecond Stimulated Raman Spectroscopy.

    PubMed

    Dietze, Daniel R; Mathies, Richard A

    2016-05-01

    Femtosecond stimulated Raman spectroscopy (FSRS) is an ultrafast nonlinear optical technique that provides vibrational structural information with high temporal (sub-50 fs) precision and high spectral (10 cm(-1) ) resolution. Since the first full demonstration of its capabilities ≈15 years ago, FSRS has evolved into a mature technique, giving deep insights into chemical and biochemical reaction dynamics that would be inaccessible with any other technique. It is now being routinely applied to virtually all possible photochemical reactions and systems spanning from single molecules in solution to thin films, bulk crystals and macromolecular proteins. This review starts with an historic overview and discusses the theoretical and experimental concepts behind this technology. Emphasis is put on the current state-of-the-art experimental realization and several variations of FSRS that have been developed. The unique capabilities of FSRS are illustrated through a comprehensive presentation of experiments to date followed by prospects. PMID:26919612

  18. Confining energy migration in upconversion nanoparticles towards deep ultraviolet lasing

    NASA Astrophysics Data System (ADS)

    Chen, Xian; Jin, Limin; Kong, Wei; Sun, Tianying; Zhang, Wenfei; Liu, Xinhong; Fan, Jun; Yu, Siu Fung; Wang, Feng

    2016-01-01

    Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors. Here we report an insulator system composed of NaYbF4:Tm in which size effect can be harnessed to enhance multiphoton upconversion. Our mechanistic investigations suggest that the phenomenon stems from spatial confinement of energy migration in nanosized structures. We show that confining energy migration constitutes a general and versatile strategy to manipulating multiphoton upconversion, demonstrating an efficient five-photon upconversion emission of Tm3+ in a stoichiometric Yb lattice without suffering from concentration quenching. The high emission intensity is unambiguously substantiated by realizing room-temperature lasing emission at around 311 nm after 980-nm pumping, recording an optical gain two orders of magnitude larger than that of a conventional Yb/Tm-based system operating at 650 nm. Our findings thus highlight the viability of realizing diode-pumped lasing in deep ultraviolet regime for various practical applications.

  19. Energy upconversion in holmium doped lead-germano-tellurite glass

    SciTech Connect

    Kamma, Indumathi; Reddy, B. Rami

    2010-06-15

    Holmium doped lead-germano-tellurite glass was prepared by the melt quenching technique. The Judd-Ofelt intensity parameters were estimated as {Omega}{sub 2}=7.6x10{sup -20}, {Omega}{sub 4}=12.9x10{sup -20}, and {Omega}{sub 6}=2.5x10{sup -20} cm{sup 2}. Radiative transition probabilities and lifetimes were also determined for some of the levels. Room temperature upconversion emissions have been observed from Ho{sup 3+} at 497 nm under 532 nm laser excitation, and at 557 and 668 nm under 762 nm laser excitation. The upconversion emission mechanisms were found to be due to a step wise excitation process. Upconversion emission intensity enhanced in a heat treated glass.

  20. Low Power Upconversion Mixer for Medical Remote Sensing

    PubMed Central

    Lioe, De Xing; Shafie, Suhaidi; Tan, Gim Heng

    2014-01-01

    This work presents the design of a low power upconversion mixer adapted in medical remote sensing such as wireless endoscopy application. The proposed upconversion mixer operates in ISM band of 433 MHz. With the carrier power of −5 dBm, the proposed mixer has an output inferred 1 dB compression point of −0.5 dBm with a corresponding output third-order intercept point (OIP3) of 7.1 dBm. The design of the upconversion mixer is realized on CMOS 0.13 μm platform, with a current consumption of 594 μA at supply voltage headroom of 1.2 V. PMID:25133266

  1. A paradigm shift in the excitation wavelength of upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Jayakumar, Muthu Kumara Gnanasammandhan; Idris, Niagara Muhammad; Huang, Kai; Zhang, Yong

    2014-07-01

    The past two decades witnessed the emergence of upconversion nanoparticles as promising luminophores finding multifarious uses from biological studies to solar cells. Progress in their practical use, however, has been hampered by requirements to be excited within a narrow absorption band at around 980 nm. Since the main constituent of biological tissue - water - absorbs strongly in this region, significant reduction in the penetration depth is anticipated as the 980 nm light gets attenuated travelling through tissues, besides also risking tissue damage from the overheating effect. Just recently, remarkable efforts to engineer the excitation of upconversion nanoparticles to a more suitable wavelength for biological applications were reported. This article gives an insightful view on the different ingenious designs that have been reported and their progression towards the development of upconversion nanoparticles with biologically friendlier excitation wavelength.

  2. An experimental design approach for hydrothermal synthesis of NaYF4: Yb3+, Tm3+ upconversion microcrystal: UV emission optimization

    NASA Astrophysics Data System (ADS)

    Kaviani Darani, Masoume; Bastani, Saeed; Ghahari, Mehdi; Kardar, Pooneh

    2015-11-01

    Ultraviolet (UV) emissions of hydrothermally synthesized NaYF4: Yb3+, Tm3+ upconversion crystals were optimized using the response surface methodology experimental design. In these experimental designs, 9 runs, two factors namely (1) Tm3+ ion concentration, and (2) pH value were investigated using 3 different ligands. Introducing UV upconversion emissions as responses, their intensity were separately maximized. Analytical methods such as XRD, SEM, and FTIR could be used to study crystal structure, morphology, and fluorescent spectroscopy in order to obtain luminescence properties. From the photo-luminescence spectra, emissions centered at 347, 364, 452, 478, 648 and 803 nm were observed. Some results show that increasing each DOE factor up to an optimum value resulted in an increase in emission intensity, followed by reduction. To optimize UV emission, as a final result to the UV emission optimization, each design had a suggestion.

  3. Visible and near infra-red up-conversion in Tm3+/Yb3+ co-doped silica fibers under 980 nm excitation.

    PubMed

    Simpson, D A; Gibbs, W E; Collins, S F; Blanc, W; Dussardier, B; Monnom, G; Peterka, P; Baxter, G W

    2008-09-01

    The spectroscopic properties of Tm(3+)/Yb(3+) co-doped silica fibers under excitation at 980 nm are reported. Three distinct up-conversion fluorescence bands were observed in the visible to near infra-red regions. The blue and red fluorescence bands at 475 and 650 nm, respectively, were found to originate from the (1)G(4) level of Tm(3+). A three step up-conversion process was established as the populating mechanism for these fluorescence bands. The fluorescence band at 800 nm was found to originate from two possible transitions in Tm(3+); one being the transition from the (3)H(4) to (3)H(6) manifold which was found to dominate at low pump powers; the other being the transition from the (1)G(4) to (3)H(6) level which dominates at higher pump powers. The fluorescence lifetime of the (3)H(4) and (3)F(4) levels of Tm(3+) and (2)F(5/2) level of Yb(3+) were studied as a function of Yb(3+) concentration, with no significant energy back transfer from Tm(3+) to Yb(3+) observed. PMID:18772989

  4. Femtosecond broadband stimulated Raman spectroscopy: Apparatus and methods

    PubMed Central

    McCamant, David W.; Kukura, Philipp; Yoon, Sangwoon; Mathies, Richard A.

    2005-01-01

    The laser, detection system, and methods that enable femtosecond broadband stimulated Raman spectroscopy (FSRS) are presented in detail. FSRS is a unique tool for obtaining high time resolution (<100 fs) vibrational spectra with an instrument response limited frequency resolution of <10 cm–1. A titanium:Sapphire-based laser system produces the three different pulses needed for FSRS: (1) A femtosecond visible actinic pump that initiates the photochemistry, (2) a narrow bandwidth picosecond Raman pump that provides the energy reservoir for amplification of the probe, and (3) a femtosecond continuum probe that is amplified at Raman resonances shifted from the Raman pump. The dependence of the stimulated Raman signal on experimental parameters is explored, demonstrating the expected exponential increase in Raman intensity with concentration, pathlength, and Raman pump power. Raman spectra collected under different electronic resonance conditions using highly fluorescent samples highlight the fluorescence rejection capabilities of FSRS. Data are also presented illustrating our ability: (i) To obtain spectra when there is a large transient absorption change by using a shifted excitation difference technique and (ii) to obtain high time resolution vibrational spectra of transient electronic states. PMID:17183413

  5. Infrared hyperspectral upconversion imaging using spatial object translation.

    PubMed

    Kehlet, Louis Martinus; Sanders, Nicolai; Tidemand-Lichtenberg, Peter; Dam, Jeppe Seidelin; Pedersen, Christian

    2015-12-28

    In this paper hyperspectral imaging in the mid-infrared wavelength region is realised using nonlinear frequency upconversion. The infrared light is converted to the near-infrared region for detection with a Si-based CCD camera. The object is translated in a predefined grid by motorized actuators and an image is recorded for each position. A sequence of such images is post-processed into a series of monochromatic images in a wavelength range defined by the phasematch condition and numerical aperture of the upconversion system. A standard USAF resolution target and a polystyrene film are used to impart spatial and spectral information unto the source. PMID:26832059

  6. Green upconversion in Y2O3:Yb nanopowder

    NASA Astrophysics Data System (ADS)

    Horvat, Darja; Lazar, Dušan; Možina, Janez; Križan, Janez; Diaci, Janez; Terzić, Mira

    2015-01-01

    Green emission lines, in addition to the blue and the red, were observed upon 980 nm excitation in yttrium oxide (Y2O3) nanopowder codoped with Yb and Tm, synthesized by the chemical combustion method. Upconversion emission studies suggest that the number and characteristics of the green lines are influenced by the annealing temperature as well as by the Yb/Tm concentration ratio, opening possibilities for new customized applications. The chromaticity properties of the upconversion spectra were quantified by the Commission Internationale de l'éclairage coordinate analysis.

  7. Investigation on up-conversion luminescence properties of novel transparent Ho3+-Tm3+-Yb3+ co-doped oxyfluoride glass ceramics

    NASA Astrophysics Data System (ADS)

    Liu, Xiao-bo; Han, Wan-lei; Xu, Fang; Song, Ying-lin

    2011-06-01

    In the present letter, the transparent oxyfluoride glass ceramics containing Ho3+-Tm3+-Yb3+:NaYF4 were successfully prepared by melt-quenching at 1400°C and subsequent heating at 650-680°C for 1~2 hours . X-ray diffraction (XRD) with Cu Kα radiation (λ=0.154nm) investigation revealed that NaYF4 nano-crystals in the glass ceramics was fabricated. Their sizes were determined by Sherrer's equation. The emission spectra red green and blue up-conversion (UC) under 980nm laser diode (LD) pumping and absorption spectra were measured. Luminescence measurements confirmed the partition of RE ions in nano-crystals NaYF4. The blue red and green UC radiations correspond to the transitions 1G4-3H6, 1G4-3H4 of Tm3+, 5F4, 5S2-5I8, 5F5-5I8, of Ho3+ ions, respectively. This is similar to that in Tm3+-Yb3+ and/or Ho3+-Yb3+ co-doped glass ceramics. To obtain upconversion fluorescence mechanisms, upconversion fluorescence intensity versus LD pump power were analyzed in view of energy levels of rare earth. Up-conversion mechanisms were discussed and the ratio between red, green and blue UC emission bands was found to be varied as a function of temperature of heat treatment and pump power. This result could be mainly attributed to the cross-relaxation between Ho3+ ions. The excellent optical properties and its convenient, low-cost synthesis of the present glass ceramic imply that it is an excellent substitution material for the unobtainable bulk NaYF4 crystal and may have potentially applications in tunable visible laser or many other fields.

  8. Dual enhancement of electroluminescence efficiency and operational stability by rapid upconversion of triplet excitons in OLEDs

    PubMed Central

    Furukawa, Taro; Nakanotani, Hajime; Inoue, Munetomo; Adachi, Chihaya

    2015-01-01

    Recently, triplet harvesting via a thermally activated delayed fluorescence (TADF) process has been established as a realistic route for obtaining ultimate internal electroluminescence (EL) quantum efficiency in organic light-emitting diodes (OLEDs). However, the possibility that the rather long transient lifetime of the triplet excited states would reduce operational stability due to an increased chance for unwarranted chemical reactions has been a concern. Herein, we demonstrate dual enhancement of EL efficiency and operational stability in OLEDs by employing a TADF molecule as an assistant dopant and a fluorescent molecule as an end emitter. The proper combination of assistant dopant and emitter molecules realized a “one-way” rapid Förster energy transfer of singlet excitons from TADF molecules to fluorescent emitters, reducing the number of cycles of intersystem crossing (ISC) and reverse ISC in the TADF molecules and resulting in a significant enhancement of operational stability compared to OLEDs with a TADF molecule as the end emitter. In addition, we found that the presence of this rapid energy transfer significantly suppresses singlet-triplet annihilation. Using this finely-tuned rapid triplet-exciton upconversion scheme, OLED performance and lifetime was greatly improved. PMID:25673259

  9. Dual enhancement of electroluminescence efficiency and operational stability by rapid upconversion of triplet excitons in OLEDs.

    PubMed

    Furukawa, Taro; Nakanotani, Hajime; Inoue, Munetomo; Adachi, Chihaya

    2015-01-01

    Recently, triplet harvesting via a thermally activated delayed fluorescence (TADF) process has been established as a realistic route for obtaining ultimate internal electroluminescence (EL) quantum efficiency in organic light-emitting diodes (OLEDs). However, the possibility that the rather long transient lifetime of the triplet excited states would reduce operational stability due to an increased chance for unwarranted chemical reactions has been a concern. Herein, we demonstrate dual enhancement of EL efficiency and operational stability in OLEDs by employing a TADF molecule as an assistant dopant and a fluorescent molecule as an end emitter. The proper combination of assistant dopant and emitter molecules realized a "one-way" rapid Förster energy transfer of singlet excitons from TADF molecules to fluorescent emitters, reducing the number of cycles of intersystem crossing (ISC) and reverse ISC in the TADF molecules and resulting in a significant enhancement of operational stability compared to OLEDs with a TADF molecule as the end emitter. In addition, we found that the presence of this rapid energy transfer significantly suppresses singlet-triplet annihilation. Using this finely-tuned rapid triplet-exciton upconversion scheme, OLED performance and lifetime was greatly improved. PMID:25673259

  10. Dual enhancement of electroluminescence efficiency and operational stability by rapid upconversion of triplet excitons in OLEDs

    NASA Astrophysics Data System (ADS)

    Furukawa, Taro; Nakanotani, Hajime; Inoue, Munetomo; Adachi, Chihaya

    2015-02-01

    Recently, triplet harvesting via a thermally activated delayed fluorescence (TADF) process has been established as a realistic route for obtaining ultimate internal electroluminescence (EL) quantum efficiency in organic light-emitting diodes (OLEDs). However, the possibility that the rather long transient lifetime of the triplet excited states would reduce operational stability due to an increased chance for unwarranted chemical reactions has been a concern. Herein, we demonstrate dual enhancement of EL efficiency and operational stability in OLEDs by employing a TADF molecule as an assistant dopant and a fluorescent molecule as an end emitter. The proper combination of assistant dopant and emitter molecules realized a ``one-way'' rapid Förster energy transfer of singlet excitons from TADF molecules to fluorescent emitters, reducing the number of cycles of intersystem crossing (ISC) and reverse ISC in the TADF molecules and resulting in a significant enhancement of operational stability compared to OLEDs with a TADF molecule as the end emitter. In addition, we found that the presence of this rapid energy transfer significantly suppresses singlet-triplet annihilation. Using this finely-tuned rapid triplet-exciton upconversion scheme, OLED performance and lifetime was greatly improved.

  11. Pr3+/Yb3+ co-doped beta-phase NaYF4 microprisms: controlled synthesis and upconversion luminescence.

    PubMed

    Gao, Wei; Zheng, Hairong; Gao, Dangli; He, Enjie; Li, Jiao; Tu, Yinxun

    2014-06-01

    Pr3+/Yb3+ co-doped hexagonal NaYF4(beta-NaYF4) microprisms were synthesized by the hydrothermal method, and ethylenediaminetetraacetic acid (EDTA) was introduced to control the size of the microcrystal samples. Bright upconverted fluorescence emission was observed when the samples were excited with an infrared (IR) laser at 976.4 nm. The emission was found to originate from the transitions of 3P0-3F2, 3P0-3H6 or 1G4-3H4, 3P1-3H6, 3P0-3H5, 3P1-3H5, and 3P0-3H4 of Pr3+ ions. Possible mechanisms for upconversion fluorescence and concentration dependence as well as the crystal structure and its formation of NaYF4:Yb3+/Pr3+ microprisms were explored and discussed based on the experimental observations. PMID:24738388

  12. White upconversion luminescence in CaF2:Yb(3+)/Eu(3+) powders via the incorporation of Y(3+) ions.

    PubMed

    Li, Yangyang; Guo, Junjie; Liu, Xiaohui; Aidilibike, Tuerxun; Qin, Weiping

    2016-06-28

    White upconversion luminescence (UCL) was achieved under 980 nm excitation in the CaF2:Yb(3+)/Eu(3+) material using Y(3+) to adjust the luminescence performance. In this luminescent system, Yb(3+) not only plays the role of a sensitizer of Eu(3+), but also generates green fluorescence from Yb(3+) dimers (2-Yb(3+)) by cooperative transitions in the CaF2 matrix. One of the primary colors of green corresponds to the 2-Yb(3+) cooperative emission exactly. Eu(3+) acts as an activator for emitting red and blue fluorescence simultaneously. Interestingly, the color of the UCL can be controlled by adjusting the doping concentration of Y(3+) ions, and white UCL was realized when the concentration of Y(3+) was 1%. PMID:27265683

  13. Noncontact microsurgery of cell membranes using femtosecond laser pulses for optoinjection of specified substances into cells

    SciTech Connect

    Il'ina, I V; Ovchinnikov, A V; Chefonov, O V; Sitnikov, D S; Agranat, Mikhail B; Mikaelyan, A S

    2013-04-30

    IR femtosecond laser pulses were used for microsurgery of a cell membrane aimed at local and short-duration change in its permeability and injection of specified extracellular substances into the cells. The possibility of noncontact laser delivery of the propidium iodide fluorescent dye and the pEGFP plasmid, encoding the green fluorescent protein, into the cells with preservation of the cell viability was demonstrated. (extreme light fields and their applications)

  14. Fluorescence in rare earth-doped fluorozirconate fibers.

    PubMed

    Saissy, A; Ostrowsky, D B; Maze, G

    1991-05-20

    Spontaneous fluorescence bands of erbium-, holmium-, and thulium-doped fluorozirconate fibers are studied experimentally and theoretically. From experimental data and for each trivalent ion we identify the set of optical transitions that gives rise to the observed linear fluorescence and upconversion process. Fiber perturbation theory and density matrix formalism are used to model fluorescence spectra with particular attention to modal structure, loss, and mode coupling in the fiber. The relationship between the experimental emission spectrum of thulium-doped fiber and the theoretical model is discussed. PMID:20700160

  15. Development of Pressure sensing Particles through SERS and Upconversion

    NASA Astrophysics Data System (ADS)

    Widejko, Ryan; Wang, Fenglin; Anker, Jeff

    2012-03-01

    With the increasing distance of space travel, there is a critical need for non-invasive point-of-care diagnostic techniques. According to the NASA Human Research Roadmap, the ``lack of non-invasive diagnostic imaging capability and techniques to diagnose identified Exploration Medical Conditions involving internal body parts,'' is a critical capability gap for long distance space travel. To address this gap, we developed a novel technique for non-invasive monitoring of strain on implanted devices. We constructed a prototype tension-indicating washer with an upconversion spectrum that depended upon strain. The washer was made of a polydimethylsiloxane (PDMS) mixture with upconversion particles embedded in it. This mixture was cured onto a lenticular lens. Methylene blue dye solution was sealed between the lenticular lens and PDMS so that pressure on the washer displaced the dye and uncovered the upconversion particles. We also began work on a tension-indicating screw based upon surface enhanced Raman spectroscopy (SERS). Future work for this project is to quantitatively correlate the spectral intensity with pressure, further develop SERS washers, and construct SERS and/or upconversion screws or bolts. Non-invasive tension-indicating devices and techniques such as these can be applied to orthopedics, used as a general technique for measuring micro-strain, verifying proper assembly of equipment, and observing/studying bolt loosening.

  16. 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

  17. Single-cell optoporation and transfection using femtosecond laser and optical tweezers.

    PubMed

    Waleed, Muhammad; Hwang, Sun-Uk; Kim, Jung-Dae; Shabbir, Irfan; Shin, Sang-Mo; Lee, Yong-Gu

    2013-01-01

    In this paper, we demonstrate a new single-cell optoporation and transfection technique using a femtosecond Gaussian laser beam and optical tweezers. Tightly focused near-infrared (NIR) femtosecond laser pulse was employed to transiently perforate the cellular membrane at a single point in MCF-7 cancer cells. A distinct technique was developed by trapping the microparticle using optical tweezers to focus the femtosecond laser precisely on the cell membrane to puncture it. Subsequently, an external gene was introduced in the cell by trapping and inserting the same plasmid-coated microparticle into the optoporated cell using optical tweezers. Various experimental parameters such as femtosecond laser exposure power, exposure time, puncture hole size, exact focusing of the femtosecond laser on the cell membrane, and cell healing time were closely analyzed to create the optimal conditions for cell viability. Following the insertion of plasmid-coated microparticles in the cell, the targeted cells exhibited green fluorescent protein (GFP) under the fluorescent microscope, hence confirming successful transfection into the cell. This new optoporation and transfection technique maximizes the level of selectivity and control over the targeted cell, and this may be a breakthrough method through which to induce controllable genetic changes in the cell. PMID:24049675

  18. Near diffraction limited mid-IR spectromicroscopy using frequency upconversion

    NASA Astrophysics Data System (ADS)

    Sanders, Nicolai; Dam, Jeppe Seidelin; Tidemand-Lichtenberg, Peter; Pedersen, Christian

    2014-02-01

    Mid-infrared microscopy and spectroscopy is interesting due to its medical, biological and chemical applications. Spectromicroscopy can be used for histopathology, sample analysis and diagnosis. The ability to do spectromicroscopy in the 2.5 to 4.5 μm wavelength range where many organic molecules have their fundamental vibrations, with the addition of sufficient spectroscopic resolution to resolve these bands, can e.g. potentially allow for diagnostics without the need for staining of the sample. On a longer timeframe, mid-IR spectromicroscopy has the potential for in-vivo diagnostics, combining morphological and spectral imaging. Recent developments in nonlinear frequency upconversion, have demonstrated the potential to perform both imaging and spectroscopy in the mid-IR range at unparalleled low levels of illumination, the low upconversion detector noise being orders of magnitude below competing technologies. With these applications in mind, we have incorporated microscopy optics into an image upconversion system, achieving near diffraction limited spatial resolution in the 3 μm range. Spectroscopic information is further acquired by appropriate control of the phase match condition of the upconversion process. Multispectral images for a region of interest can be obtained by XY-scanning this region of interest within the field of view of the mid-IR upconversion system. Thus, the whole region of interest can be imaged with all available converter wavelengths, and the spectral representation becomes equal for all points in the image. In addition, the range of converted/imaged wavelengths can be tuned continuously by changing the temperature of the crystal, or discretely by using a different poling channel in the PPLN crystal.

  19. Comprehensive studies on an overall proton transfer cycle of the ortho-green fluorescent protein chromophore.

    PubMed

    Hsieh, Cheng-Chih; Chou, Pi-Tai; Shih, Chun-Wei; Chuang, Wei-Ti; Chung, Min-Wen; Lee, Junghwa; Joo, Taiha

    2011-03-01

    Initiated by excited-state intramolecular proton transfer (ESIPT) reaction, an overall reaction cycle of 4-(2-hydroxybenzylidene)-1,2-dimethyl-1H-imidazol-5(4H)-one (o-HBDI), an analogue of the core chromophore of the green fluorescent protein (GFP), has been investigated. In contrast to the native GFP core, 4-(4-hydroxybenzylidene)-1,2-dimethyl-1H-imidazol-5(4H)-one (p-HBDI), which requires hydrogen-bonding relay to accomplish proton transfer in vivo, o-HBDI possesses a seven-membered-ring intramolecular hydrogen bond and thus provides an ideal system for mimicking an intrinsic proton-transfer reaction. Upon excitation, ESIPT takes place in o-HBDI, resulting in a ∼600 nm proton-transfer tautomer emission. The o-HBDI tautomer emission, resolved by fluorescence upconversion, is comprised of an instantaneous rise to a few hundred femtosecond oscillation in the early relaxation stage. Frequency analysis derived from ultrashort pulse gives two low-frequency vibrations at 115 and 236 cm(-1), corresponding to skeletal deformation motions associated with the hydrogen bond. The results further conclude that ESIPT in o-HBDI is essentially triggered by low-frequency motions and may be barrierless along the reaction coordinate. Femtosecond UV/vis transient absorption spectra also provide supplementary evidence for the structural evolution during the reaction. In CH(3)CN, an instant rise of a 530 nm transient is resolved, which then undergoes 7.8 ps decay, accompanied by the growth of a rather long-lived 580 nm transient species. It is thus concluded that following ESIPT the cis-proton transfer isomer undergoes cis-trans-isomerization. The results of viscosity-dependent dynamics are in favor of the one-bond-flip mechanism, which is in contrast to the volume-conserving isomerization behavior for cis-stilbene and p-HBDI. Further confirmation is given by the picosecond-femtosecond transient IR absorption spectra, where several new and long-lived IR bands in the range of 1400

  20. Advances in the theoretical understanding of photon upconversion in rare-earth activated nanophosphors.

    PubMed

    Liu, Guokui

    2015-03-21

    Photon upconversion in rare earth activated phosphors involves multiple mechanisms of electronic transitions. Stepwise optical excitation, energy transfer, and various nonlinear and collective light-matter interaction processes act together to convert low-energy photons into short-wavelength light emission. Upconversion luminescence from nanomaterials exhibits additional size and surface dependencies. A fundamental understanding of the overall performance of an upconversion system requires basic theories on the spectroscopic properties of solids containing rare earth ions. This review article surveys the recent progress in the theoretical interpretations of the spectroscopic characteristics and luminescence dynamics of photon upconversion in rare earth activated phosphors. The primary aspects of upconversion processes, including energy level splitting, transition probability, line broadening, non-radiative relaxation and energy transfer, are covered with an emphasis on interpreting experimental observations. Theoretical models and methods for analyzing nano-phenomena in upconversion are introduced with detailed discussions on recently reported experimental results. PMID:25286989

  1. Photophysical properties of new bis-perylene dyads for potential upconversion use

    NASA Astrophysics Data System (ADS)

    Ribas, Marcos R.; Steer, Ronald P.; Rüther, Ricardo

    2014-06-01

    Two new bis-perylenes, BPC with a meta-disubstituted benzene linker, and BPD with a p,p‧-disubstituted biphenyl linker, have been synthesized and their photophysical parameters measured. Their singlet and triplet energies decrease incrementally in the order perylene, BPC, BPD, making them ideally matched with C60 for triplet-triplet energy transfer in sensitized photon upconversion schemes. Following photosensitization by triplet C60, BPC exhibits strong fluorescence upconversion by triplet-triplet annihilation, indicating that these bis-perylene dyads (and the multimers that can be constructed from them) will be interesting candidates for use in organic devices such as bulk-heterojunction and dye-sensitized solar cells employing non-coherent photon upconversion. Excitation of C60 at 532 nm will produce its long-lived lowest triplet state with near unit quantum efficiency under the conditions of this experiment [33]. The thermal energy loss usually associated with triplet-triplet energy transfer, Eq. (2), is minimal in this system as the triplet energies of the donor and acceptor are nearly identical at ca. 1.5 eV. In the absence of self-quenching of the fluorescing singlet state, increasing the relative concentrations of acceptor to donor can raise the overall efficiency of the sensitization process to nearly 100%, even if their triplet energies are the same, due to entropic assistance [34]. This was confirmed by measuring the upconversion intensity as a function of dyad concentration at constant absorbed power (Supplementary Information), and by transient absorption measurements of C60 (T1) at 740 nm (Supplementary Information). The latter show that C60(T1) decays with a lifetime on the order of 400 ns for equimolar C60 + BPC concentrations, i.e. at a rate at least 100 times faster (due to quenching by energy transfer) than it would decay in the absence of the BPC triplet energy acceptor. Note also that the dimers with their slightly lower triplet energies are

  2. Dual-Mode Luminescent Nanopaper Based on Ultrathin g-C3N4 Nanosheets Grafted with Rare-Earth Upconversion Nanoparticles.

    PubMed

    Zhao, Yafei; Wei, Ruoyan; Feng, Xin; Sun, Lining; Liu, Panpan; Su, Yongxiang; Shi, Liyi

    2016-08-24

    Ultrathin graphite-like carbon nitride (g-C3N4) nanosheets have attracted considerable attention due to the enhanced intrinsic photoabsorption and photoresponse with respect to bulk g-C3N4. For the first time, a dual-mode of down- and upconversion luminescent g-C3N4 nanopaper with high optical transparency and mechanical robustness was successfully fabricated through a simple thermal evaporation process using chitosan as a green cross-linking agent. The dual-mode of down- and upconversion fluorescence emission originated from the amino terminated ultrathin g-C3N4 nanosheets functionalized with carboxylic acid modified multicolored rare-earth upconversion nanoparticles (cit-UCNPs) via EDC/NHS coupling chemistry. The homogeneously distributed cit-UCNPs@g-C3N4 nanoconjugates with excellent hydrophilicity displayed good film-forming ability and structural integrity; thus, the photoluminescence of each ingredient was substantially maintained. Results indicated that the freestanding chitosan cross-linked cit-UCNPs@g-C3N4 luminescent nanopaper possessed high transmittance, excellent mechanical properties, and remarkable dual-mode emission. The smart design of high performance luminescent nanopaper based on ultrathin g-C3N4 nanosheets grafted with multicolored UCNPs offers a potential strategy to immobilize other multifunctional luminescent materials for easily recognizable and hardly replicable anticounterfeiting fields. PMID:27494116

  3. Structural morphology, upconversion luminescence and optical thermometric sensing behavior of Y2O3:Er3+/Yb3+ nano-crystalline phosphor

    NASA Astrophysics Data System (ADS)

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

    2014-08-01

    Infrared-to-visible upconverting rare earths Er3+/Yb3+ 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.

  4. Femtosecond tunable light source

    NASA Astrophysics Data System (ADS)

    Miesak, Edward Jozef

    1999-09-01

    A practical source of continuously tunable coherent visible and infrared light would have an enormous impact on science, medicine and technology. While microwave and radio transmitters offer wide tunability at the ``turn of a knob,'' the best known source of coherent optical radiation, the laser, does not possess the same versatility. Dye lasers provide some degree of tunability, but many dyes are needed to cover even the visible region. Ti:sapphire lasers are tunable only over the red to near infra-red portion of the spectrum (about 65 0 nm to about 1.1μm). This presentation documents the development of a unique pulsed light source tunable across the visible and near infrared portion of the spectrum, a femtosecond optical parametric amplifier (OPA). Much work was expended in developing the system itself. But a great deal of work was also done in developing the support equipment (hardware and software) necessary to build as well as maintain and operate an OPA. Once completed, the system characteristics were measured and documented. Initially it possessed ``personality'' which had to be understood and removed as much as possible. In addition, the pump source for this OPA, a regenerative amplifier, is unique in that it uses Cr3+:LiSGaF as the gain medium. This regen was also characterized and compared to other more standard regenerative amplifiers. System verification was done by performing a standard experiment (Z-scan) on well known samples, several of which are well characterized at specific wavelengths (1.06 μm, 0.523 μm) in the nanosecond and picosecond regimes. The results were compared against previously published results. The OPA was also compared against another very similar system which became commercially available during the time of this research. The results were helpful in analyzing the light source(s) and data acquisition systems for areas that could be improved.

  5. Holographic vector-wave femtosecond laser processing

    NASA Astrophysics Data System (ADS)

    Hayasaki, Yoshio; Hasegawa, Satoshi

    2016-03-01

    Arbitrary and variable beam shaping of femtosecond pulses by a computer-generated hologram (CGH) displayed on a spatial light modulator (SLM) have been applied to femtosecond laser processing. The holographic femtosecond laser processing has been widely used in many applications such as two-photon polymerization, optical waveguide fabrication, fabrication of volume phase gratings in polymers, and surface nanostructuring. A vector wave that has a spatial distribution of polarization states control of femtosecond pulses gives good performances for the femtosecond laser processing. In this paper, an in- system optimization of a CGH for massively-parallel femtosecond laser processing, a dynamic control of spatial spectral dispersion to improve the focal spot shape, and the holographic vector-wave femtosecond laser processing are demonstrated.

  6. Two-photon excitation of dyes in a polymer matrix by femtosecond pulses from a Ti:sapphire laser

    SciTech Connect

    Meshalkin, Yu P; Myachin, A Yu; Bakhareva, S S; Svetlichnyi, Valerii A; Kopylova, T N; Reznichenko, A V; Dolotov, S M; Ponomarenko, E P

    2003-09-30

    Two-photon fluorescence was observed for 18 organic dyes in a polymethyl methacrylate (PMMA) matrix excited by a femtosecond Ti:sapphire laser. The product of the cross section for two-photon absorption by the quantum yield of fluorescence (two-photon fluorescence cross section) is estimated by comparing it with fluorescence of Rhodamine 6G in ethanol. Using this parameter, dyes are selected that exhibit the most intense fluorescence in PMMA and their concentrations in PMMA are optimised. Coumarin and rhodamine dyes in polymer matrices are proposed for using as visualisers of femtosecond radiation of a Ti:sapphire laser and as detectors in self-triggering systems. (active media. lasers)

  7. Anomalous fluorescence line intensity in megavoltage bremsstrahlung

    NASA Astrophysics Data System (ADS)

    Pereira, Nino; Litz, Marc; Merkel, George; Schumer, Joseph; Seely, John; Carroll, Jeff

    2009-11-01

    A Cauchois transmission crystal spectrometer intended for laser plasma diagnostics has measured an anomalous ratio between the fluorescence lines in megavoltage bremsstrahlung. When observed in reflection, Kα1 fluorescence is twice as strong as the Kβ line, as is usual. However, in forward-directed bremsstrahlung from a 2 MV end point linear accelerator with a tungsten converter, the Kα1 and Kβ fluorescence are approximately equal. The anomalous fluorescence line ratio, unity, reflects the large amount of fluorescence generated on the side of the converter where the electrons enter, and the differential attenuation of the fluorescence photons as they pass through the converter to opposite side. Understanding of fluorescence in megavoltage bremsstrahlung is relevant to the explanation of anomalous line ratios in spectra produced by high-energy electrons generated by intense femtosecond laser irradiation.

  8. 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. PMID:24589842

  9. 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.

  10. 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.

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

    PubMed Central

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

    2015-01-01

    Upconversion luminescence properties from the emissions of Stark sublevels of Er3+ were investigated in Er3+-Yb3+-Mo6+-codoped TiO2 phosphors in this study. According to the energy levels split from Er3+, 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 Er3+-Yb3+-Mo6+-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. PMID:26690431

  12. NIR to NIR upconversion in KYb2F7: RE3+ (RE = Tm, Er) nanoparticles for biological imaging

    PubMed Central

    Pedraza, F.; Yust, B.; Tsin, A.; Sardar, D.

    2015-01-01

    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. PMID:26120238

  13. 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

    2015-01-01

    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. PMID:26690431

  14. IRRS, UV-Vis-NIR absorption and photoluminescence upconversion in Ho{sup 3+}-doped oxyfluorophosphate glasses

    SciTech Connect

    Karmakar, Basudeb . E-mail: basudebk@cgcri.res.in

    2005-09-15

    Infrared reflection spectroscopic (IRRS), ultraviolet-visible-near infrared (UV-Vis-NIR) absorption and photoluminescence upconversion properties with special emphasis on the spectrochemistry of the oxyfluorophosphate (oxide incorporated fluorophosphates) glasses of the Ba(PO{sub 3}){sub 2}-AlF{sub 3}-CaF{sub 2}-SrF{sub 2}-MgF{sub 2}-Ho{sub 2}O{sub 3} system have been studied with different concentrations (0.1, 0.3 and 1.0 mol%) of Ho{sub 2}O{sub 3}. IRRS spectral band position and intensity of Ho{sup 3+} ion doped oxyfluorophosphate glasses have been discussed in terms of reduced mass and force constant. UV-Vis-NIR absorption band position has been justified with quantitative calculation of nephelauxetic parameter and covalent bonding characteristics of the host. NIR to visible upconversion has been investigated by exciting at 892 nm at room temperature. Three upconverted bands originated from the {sup 5}F{sub 3}{yields}{sup 5}I{sub 8} ({sup 5}S{sub 2}, {sup 5}F{sub 4}){yields}{sup 5}I{sub 8} and {sup 5}F{sub 5}{yields}{sup 5}I{sub 8} transitions have found to be centered at 491 nm (blue, medium), 543 nm (green, very strong) and 658 nm (red, weak), respectively. These bands have been justified from the evaluation of the absorption, normal (down conversion) fluorescence and excitation spectra. The upconversion processes have been explained by the excited state absorption (ESA), energy transfer (ET) and cross relaxation (CR) mechanisms involving population of the metastable (storage) energy levels by multiphonon deexcitation effect. It is evident from the IRRS study that the upconversion phenomena are expedited by the low multiphonon relaxation rate in oxyfluorophosphate glasses owing to their high intense low phonon energy ({approx}600 cm{sup -1}) which is very close to that of fluoride glasses (500-600 cm{sup -1})

  15. Application of femtosecond-laser induced nanostructures in optical memory.

    PubMed

    Shimotsuma, Yasuhiko; Sakakura, Masaaki; Miura, Kiyotaka; Qiu, Jiarong; Kazansky, Peter G; Fujita, Koji; Hirao, Kazuyuki

    2007-01-01

    The femtosecond laser induced micro- and nanostructures for the application to the three-dimensional optical data storage are investigated. We have observed the increase of refractive index due to local densification and atomic defect generation, and demonstrated the real time observation of photothermal effect after the femtosecond laser irradiation inside a glass by the transient lens (TrL) method. The TrL signal showed a damped oscillation with about an 800 ps period. The essential feature of the oscillation can be reproduced by the pressure wave creation and propagation to the outward direction from the irradiated region. The simulation based on elastodynamics has shown that a large thermoelastic stress is relaxed by the generation of the pressure wave. In the case of soda-lime glass, the velocity of the pressure wave is almost same as the longitudinal sound velocity at room temperature (5.8 microm/ns). We have also observed the localized photo-reduction of Sm3+ to Sm2+ inside a transparent and colorless Sm(3+)-doped borate glass. Photoluminescence spectra showed that some the Sm3+ ions in the focal spot within the glass sample were reduced to Sm2+ ions after femtosecond laser irradiation. A photo-reduction bit of 200 nm in three-dimensions can be recorded with a femtosecond laser and readout clearly by detecting the fluorescence excited by Ar+ laser (lambda = 488 nm). A photo-reduction bit can be also erased by photo-oxidation with a cw Ar+ laser (lambda = 514.5 nm). Since photo-reduction bits can be spaced 150 nm apart in a layer within glass, a memory capacity of as high as 1 Tbit can be achieved in a glass piece with dimensions of 10 mm x 10 mm x 1 mm. We have also demonstrated the first observation of the polarization-dependent periodic nanostructure formation by the interference between femtosecond laser light and electron acoustic waves. The observed nanostructures are the smallest embedded structures ever created by light. The period of self

  16. Enhanced 1.0 μm emission and simultaneously suppressed upconversion emission in Yb:PbF2 laser crystal codoped with NaF

    NASA Astrophysics Data System (ADS)

    Zhang, P. X.; Yin, J. G.; Hang, Y.; Yin, J. P.

    2013-04-01

    Na-codoped and only Yb-doped Yb:PbF2 crystals were successfully grown using the vertical Bridgman method. The influence of the ions codoped with Na+ on the distribution coefficients has been studied. Enhanced ˜1.0 μm emission and simultaneously suppressed upconversion emission was observed for Yb:PbF2 crystals codoped with 2 mol% NaF. A time-resolved spectroscopy study showed that the ions codoped with Na+ lengthen the fluorescence lifetime by 6%. Absorption spectra were also studied and showed that the ions codoped with Na+ can effectively suppress the formation of Yb2+ ions.

  17. Structural characterizations and intense green upconversion emission in Yb3+, Pr3+ co-doped Y2O3 nano-phosphor.

    PubMed

    Yadav, R S; Verma, R K; Bahadur, A; Rai, S B

    2015-02-25

    We report the structural and optical properties of Yb(3+), Pr(3+) co-doped Y2O3 nano-phosphor synthesized through solution combustion method. The structural studies reveal the nano-crystalline structure of the sample. The energy dispersive spectroscopy (EDS) measurements confirm the presence of Y, O, Pr and Yb elements in the sample. Fourier transform infrared studies show the vibrational features of the samples. The fluorescence spectra of the samples have been monitored on excitation with 976 nm and the intense green upconversion emission observed at 552 nm is due to (3)P0→(3)H5 electronic transition. The concentration of Pr(3+) ion in the sample is optimized and the fluorescence intensity is maximum at 0.08 mol% of Pr(3+). The power dependence studies reveal the involvement of two photons in the emission process. The possible mechanism of upconversion has been discussed on the basis of schematic energy level diagram. The sample annealed at higher temperature enhances the fluorescence intensity up to 8 times and this enhancement is discussed in terms of the removal of optical quenching centers. The nano-phosphor can be applicable in the field of display devices and green laser. PMID:25233026

  18. Structural characterizations and intense green upconversion emission in Yb3+, Pr3+ co-doped Y2O3 nano-phosphor

    NASA Astrophysics Data System (ADS)

    Yadav, R. S.; Verma, R. K.; Bahadur, A.; Rai, S. B.

    2015-02-01

    We report the structural and optical properties of Yb3+, Pr3+ co-doped Y2O3 nano-phosphor synthesized through solution combustion method. The structural studies reveal the nano-crystalline structure of the sample. The energy dispersive spectroscopy (EDS) measurements confirm the presence of Y, O, Pr and Yb elements in the sample. Fourier transform infrared studies show the vibrational features of the samples. The fluorescence spectra of the samples have been monitored on excitation with 976 nm and the intense green upconversion emission observed at 552 nm is due to 3P0 → 3H5 electronic transition. The concentration of Pr3+ ion in the sample is optimized and the fluorescence intensity is maximum at 0.08 mol% of Pr3+. The power dependence studies reveal the involvement of two photons in the emission process. The possible mechanism of upconversion has been discussed on the basis of schematic energy level diagram. The sample annealed at higher temperature enhances the fluorescence intensity up to 8 times and this enhancement is discussed in terms of the removal of optical quenching centers. The nano-phosphor can be applicable in the field of display devices and green laser.

  19. Subwavelength imaging through ion-beam-induced upconversion

    PubMed Central

    Mi, Zhaohong; Zhang, Yuhai; Vanga, Sudheer Kumar; Chen, Ce-Belle; Tan, Hong Qi; Watt, Frank; Liu, Xiaogang; Bettiol, Andrew A.

    2015-01-01

    The combination of an optical microscope and a luminescent probe plays a pivotal role in biological imaging because it allows for probing subcellular structures. However, the optical resolutions are largely constrained by Abbe's diffraction limit, and the common dye probes often suffer from photobleaching. Here we present a new method for subwavelength imaging by combining lanthanide-doped upconversion nanocrystals with the ionoluminescence imaging technique. We experimentally observed that the ion beam can be used as a new form of excitation source to induce photon upconversion in lanthanide-doped nanocrystals. This approach enables luminescence imaging and simultaneous mapping of cellular structures with a spatial resolution of sub-30 nm. PMID:26560858

  20. Functionalized Upconversion Nanoparticles: Versatile Nanoplatforms for Translational Research

    PubMed Central

    Chen, Feng; Bu, Wenbo; Cai, Weibo; Shi, Jianlin

    2013-01-01

    The design, application, and translation of targeted multimodality molecular imaging probes based on nanotechnology has attracted increasing attentions during the last decade and will continue to play vital roles in cancer diagnosis and personalized medicine. With the growing awareness of drawbacks of traditional organic dyes and quantum dots, biocompatible lanthanide ion doped upconversion nanoparticles have emerged as promising candidates for clinically translatable imaging probes, owing to their unique features that are suitable for future targeted multimodal imaging in living subjects. In this review, we summarized the recent advances in the field of functionalized upconversion nanoparticles (f-UCNP) for biological imaging and therapy in vivo, and discussed the future research directions, obstacles ahead, and the potential use of f-UCNP in translational research. PMID:24206131

  1. Oxyfluoroborate host glass for upconversion application: phonon energy calculation

    NASA Astrophysics Data System (ADS)

    Abdel-Baki, Manal; El-Diasty, Fouad

    2016-04-01

    Reducing the glass phonon energy is an essential procedure to achieve high efficient radiative upconversion process. The degree of covalence of chemical bonds is responsible for the high oscillator strength of intracenter transitions in rare-earth ions. So, conversion covalent to ionic glass character is proposed as a structure-sensitive criterion that controls the phonon energy of the glasses. A series of oxyfluoro aluminum-borate host glasses used for upconversion application is prepared by the conventional melt-quenching technique. Through lithium oxide substitution by lithium fluoride, the ionic-covalent property of Li+ ion successes to regulate the band gap energies of the studied glasses. Furthermore, a new method to determine the glass phonon energy is offered.

  2. Upconversion imaging using an all-fiber supercontinuum source.

    PubMed

    Huot, Laurent; Moselund, Peter Morten; Tidemand-Lichtenberg, Peter; Leick, Lasse; Pedersen, Christian

    2016-06-01

    In this Letter, the first demonstration, to the best of our knowledge, of pulsed upconversion imaging using supercontinuum light is presented. A mid-infrared (IR) imaging system was built by combining a mid-IR supercontinuum source emitting between 1.8 and 2.6 μm with upconversion detection. The infrared signal is used to probe a sample and mixed with a synchronized 1550 nm laser pulse inside a lithium niobate (LiNbO3) crystal. The signal is thus upconverted to the 860-970 nm range and acquired on a standard silicon CCD array at a rate of 22 frames per second. In our implementation, spatial features in the sample plane as small as 55 μm could be resolved. PMID:27244390

  3. Inkjet printing of upconversion nanoparticles for anti-counterfeit applications

    NASA Astrophysics Data System (ADS)

    You, Minli; Zhong, Junjie; Hong, Yuan; Duan, Zhenfeng; Lin, Min; Xu, Feng

    2015-02-01

    Patterning of upconversion luminescent materials has been widely used for anti-counterfeit and security applications, where the preferred method should be easy, fast, multicolor, high-throughput and designable. However, conventional patterning methods are complex and inflexible. Here, we report a digital and flexible inkjet printing based approach for producing high-resolution and high-luminescence anti-counterfeit patterns. We successfully printed different multicolor luminescent patterns by inkjet printing of upconversion nanoparticles with controlled and uniform luminescence intensity through optimizing the inks and substrates. Combined with another downconversion luminescent material, we achieved two different patterns in the same area, which show up separately under excitation by different wavelength laser sources. The developed technology is promising to use one single substrate for carrying abundant information by printing multilayer patterns composed of luminescent materials with different excitation light sources.Patterning of upconversion luminescent materials has been widely used for anti-counterfeit and security applications, where the preferred method should be easy, fast, multicolor, high-throughput and designable. However, conventional patterning methods are complex and inflexible. Here, we report a digital and flexible inkjet printing based approach for producing high-resolution and high-luminescence anti-counterfeit patterns. We successfully printed different multicolor luminescent patterns by inkjet printing of upconversion nanoparticles with controlled and uniform luminescence intensity through optimizing the inks and substrates. Combined with another downconversion luminescent material, we achieved two different patterns in the same area, which show up separately under excitation by different wavelength laser sources. The developed technology is promising to use one single substrate for carrying abundant information by printing multilayer

  4. Multispectral mid-infrared imaging using frequency upconversion

    NASA Astrophysics Data System (ADS)

    Sanders, Nicolai; Dam, Jeppe Seidelin; Jensen, Ole Bjarlin; Tidemand-Lichtenberg, Peter; Pedersen, Christian

    2013-03-01

    It has recently been shown that it is possible to upconvert infrared images to the near infrared region with high quantum efficiency and low noise by three-wave mixing with a laser field [1]. If the mixing laser is single-frequency, the upconverted image is simply a band-pass filtered version of the infrared object field, with a bandwidth corresponding given by the acceptance parameter of the conversion process, and a center frequency given by the phase-match condition. Tuning of the phase-matched wavelengths has previously been demonstrated by changing the temperature [2] or angle [3 Keywords: Infrared imaging, nonlinear frequency conversion, diode lasers, upconversion ] of the nonlinear material. Unfortunately, temperature tuning is slow, and angle tuning typically results in alignment issues. Here we present a novel approach where the wavelength of the mixing field is used as a tuning parameter, allowing for fast tuning and hence potentially fast image acquisition, paving the way for upconversion based real time multispectral imaging. In the present realization the upconversion module consists of an external cavity tapered diode laser in a Littrow configuration with a computer controlled feedback grating. The output from a tunable laser is used as seed for a fiber amplifier system, boosting the power to approx. 3 W over the tuning range from 1025 to 1085 nm. Using a periodically poled lithium niobate crystal, the infrared wavelength that can be phase-matched is tunable over more than 200 nm. Using a crystal with multiple poling periods allows for upconversion within the entire transparency range of the nonlinear material.

  5. Synthesis of fluorescent carbon nanoparticles directly from active carbon via a one-step ultrasonic treatment

    SciTech Connect

    Li, Haitao; He, Xiaodie; Liu, Yang; Yu, Hang; Kang, Zhenhui; Lee, Shuit-Tong

    2011-01-15

    Water-soluble fluorescent carbon nanoparticles were synthesized directly from active carbon by a one-step hydrogen peroxide-assisted ultrasonic treatment. The carbon nanoparticles were characterized by transmission electron microscopy, optical fluorescent microscopy, fluorescent spectroscopy, Fourier transform infrared spectroscopy and ultraviolet-visible spectrophotometer. The results showed that the surface of carbon nanoparticles was rich of hydroxyl groups resulting in high hydrophilicity. The carbon nanoparticles could emit bright and colorful photoluminescence covering the entire visible-to-near infrared spectral range. Furthermore, these carbon nanoparticles also had excellent up-conversion fluorescent properties.

  6. Excitonic luminescence upconversion in a two-dimensional semiconductor

    NASA Astrophysics Data System (ADS)

    Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Taniguchi, Takashi; Watanabe, Kenji; Dery, Hanan; Yao, Wang; Xu, Xiaodong

    2016-04-01

    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. This phenomenon lies at the heart of optical refrigeration in solids, where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities or exciton-phonon coupling. Here, 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. Since the charged exciton binding energy closely matches the 31 meV A1' optical phonon, 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. In addition, 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.

  7. Confining energy migration in upconversion nanoparticles towards deep ultraviolet lasing

    PubMed Central

    Chen, Xian; Jin, Limin; Kong, Wei; Sun, Tianying; Zhang, Wenfei; Liu, Xinhong; Fan, Jun; Yu, Siu Fung; Wang, Feng

    2016-01-01

    Manipulating particle size is a powerful means of creating unprecedented optical properties in metals and semiconductors. Here we report an insulator system composed of NaYbF4:Tm in which size effect can be harnessed to enhance multiphoton upconversion. Our mechanistic investigations suggest that the phenomenon stems from spatial confinement of energy migration in nanosized structures. We show that confining energy migration constitutes a general and versatile strategy to manipulating multiphoton upconversion, demonstrating an efficient five-photon upconversion emission of Tm3+ in a stoichiometric Yb lattice without suffering from concentration quenching. The high emission intensity is unambiguously substantiated by realizing room-temperature lasing emission at around 311 nm after 980-nm pumping, recording an optical gain two orders of magnitude larger than that of a conventional Yb/Tm-based system operating at 650 nm. Our findings thus highlight the viability of realizing diode-pumped lasing in deep ultraviolet regime for various practical applications. PMID:26739352

  8. Enhanced up-conversion for photovoltaics via concentrating integrated optics.

    PubMed

    Arnaoutakis, Georgios E; Marques-Hueso, Jose; Ivaturi, Aruna; Krämer, Karl W; Fischer, Stefan; Goldschmidt, Jan Christoph; Richards, Bryce S

    2014-03-10

    Concentrating optics are integrated into up-conversion photovoltaic (UC-PV) devices to independently concentrate sub-band-gap photons on the up-conversion layer, without affecting the full solar concentration on the overlying solar cell. The UC-PV devices consist of silicon solar cells optimized for up-conversion, coupled with tapered and parabolic dielectric concentrators, and hexagonal sodium yttrium fluoride (β-NaYF₄) up-converter doped with 25% trivalent erbium (Er³⁺). A normalized external quantum efficiency of 1.75x10⁻² cm²/W and 3.38x10⁻² cm²/W was obtained for the UC-PV device utilizing tapered and parabolic concentrators respectively. Although low to moderate concentration was shown to maximize UC, higher concentration lead to saturation and reduced external quantum efficiency. The presented work highlights some of the implications associated with the development of UC-PV devices and designates a substantial step for integration in concentrating PV. PMID:24922255

  9. Femtosecond pulse shaping using plasmonic snowflake nanoantennas

    SciTech Connect

    Tok, Ruestue Umut; Sendur, Kuersat

    2011-09-15

    We have theoretically demonstrated femtosecond pulse manipulation at the nanoscale using the plasmonic snowflake antenna's ability to localize light over a broad spectrum. To analyze the interaction of the incident femtosecond pulse with the plasmonic nanoantenna, we first decompose the diffraction limited incident femtosecond pulse into its spectral components. The interaction of each spectral component with the nanoantenna is analyzed using finite element technique. The time domain response of the plasmonic antenna is obtained using inverse Fourier transformation. It is shown that the rich spectral characteristics of the plasmonic snowflake nanoantenna allow manipulation of the femtosecond pulses over a wide spectrum. Light localization around the gap region of the nanoantenna is shown for femtosecond pulses. As the alignment of incident light polarization is varied, different antenna elements oscillate, which in turn creates a different spectrum and a distinct femtosecond response.

  10. Femtosecond lasers for machining of transparent, brittle materials: ablative vs. non-ablative femtosecond laser processing

    NASA Astrophysics Data System (ADS)

    Hendricks, F.; Matylitsky, V. V.

    2016-03-01

    This paper focuses on precision machining of transparent materials by means of ablative and non-ablative femtosecond laser processing. Ablation technology will be compared with a newly developed patent pending non-ablative femtosecond process, ClearShapeTM, using the Spectra-Physics Spirit industrial femtosecond laser.

  11. High contrast in vivo bioimaging using multiphoton upconversion in novel rare-earth-doped fluoride upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Chen, Guanying; Yang, Chunhui; Prasad, Paras N.

    2013-02-01

    Upconversion in rare-earth ions is a sequential multiphoton process that efficiently converts two or more low-energy photons, which are generally near infrared (NIR) light, to produce anti-Stokes emission of a higher energy photon (e.g., NIR, visible, ultraviolet) using continuous-wave (cw) diode laser excitation. Here, we show the engineering of novel, efficient, and biocompatible NIRin-to-NIRout upconversion nanoparticles for biomedical imaging with both excitation and emission being within the "optical transparency window" of tissues. The small animal whole-body imaging with exceptional contrast (signal-to-noise ratio of 310) was shown using BALB/c mice intravenously injected with aqueously dispersed nanoparticles. An imaging depth as deep as 3.2-cm was successfully demonstrated using thick animal tissue (pork) under cw laser excitation at 980 nm.

  12. Photodegradation and photocuring in the operation of a blue upconversion fiber laser

    SciTech Connect

    Qin Guanshi; Huang Shenghong; Feng Yan; Shirakawa, A.; Musha, M.; Ueda, Ken-ichi

    2005-06-15

    Photodegradation and photocuring effects were investigated in the operation of a Tm{sup 3+}-doped blue upconversion fiber laser. Our experimental results indicate that a competition between photodegradation and photocuring greatly affects the maximum output power of a blue upconversion fiber laser.

  13. Sensitive Water Probing through Nonlinear Photon Upconversion of Lanthanide-Doped Nanoparticles.

    PubMed

    Guo, Shaohong; Xie, Xiaoji; Huang, Ling; Huang, Wei

    2016-01-13

    Lanthanide-doped upconversion nanoparticles have received growing attention in the development of low-background, highly sensitive and selective sensors. Here, we report a water probe based on ligand-free NaYF4:Yb/Er nanoparticles, utilizing their intrinsically nonlinear upconversion process. The water molecule sensing was realized by monitoring the upconversion emission quenching, which is mainly attributed to efficient energy transfer between upconversion nanoparticles and water molecules as well as water-absorption-induced excitation energy attenuation. The nonlinear upconversion process, together with power function relationship between upconversion emission intensity and excitation power density, offers a sensitive detection of water content down to 0.008 vol % (80 ppm) in an organic solvent. As an added benefit, we show that noncontact detection of water can be achieved just by using water attenuation effect. Moreover, these upconversion nanoparticle based recyclable probes should be particularly suitable for real-time and long-term water monitoring, due to their superior chemical and physical stability. These results could provide insights into the design of upconversion nanoparticle based sensors. PMID:26651357

  14. Facile and high spatial resolution ratio-metric luminescence thermal mapping in microfluidics by near infrared excited upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Wang, Yu; Cao, Wenbin; Li, Shunbo; Wen, Weijia

    2016-02-01

    A local area temperature monitor is important for precise control of chemical and biological processes in microfluidics. In this work, we developed a facile method to realize micron spatial resolution of temperature mapping in a microfluidic channel quickly and cost effectively. Based on the temperature dependent fluorescence emission of NaYF4:Yb3+, Er3+ upconversion nanoparticles (UCNPs) under near-infrared irradiation, ratio-metric imaging of UCNPs doped polydimethylsiloxane can map detailed temperature distribution in the channel. Unlike some reported strategies that utilize temperature sensitive organic dye (such as Rhodamine) to achieve thermal sensing, our method is highly chemically inert and physically stable without any performance degradation in long term operation. Moreover, this method can be easily scaled up or down, since the spatial and temperature resolution is determined by an optical imaging system. Our method supplied a simple and efficient solution for temperature mapping on a heterogeneous surface where usage of an infrared thermal camera was limited.

  15. [Preparation and characterization of upconversion phosphor based on AlF3-YbF3 : Er3+].

    PubMed

    Zhou, He-Feng; Zhang, Shu-Quan; Wang, Hua; Li, Jie; Wang, Li; Wang, Shu-Hao; Lin, Wen-Jing; Lin, Hong-Li

    2013-01-01

    In the present paper, AlF3-YbF3 : Er3+ was prepared by high temperature solid phase reaction, and the concentration effect of Er3+ on luminous intensity of phosphors was studied. The crystal structures of the phosphors were characterized by means of X-ray diffraction (XRD), and the upconversion luminescence properties of phosphor were studied by fluorescence emission spectra. Upon 980 nm excitation, when the Er3+ concentration was fixed to be 0.7 mol%, the maximum red emission intensities can be obtained in the sample. Furthermore, the research results showed that the fitted slope for red transition emission was 2.24, indicating that red emission is due to a two-photon excitation process. PMID:23586216

  16. Bi-Plasma Interactions on Femtosecond Time-Scales

    SciTech Connect

    Not Available

    2011-06-22

    Ultrafast THz radiation has important applications in materials science studies, such as characterizing transport properties, studying the vibrational response of materials, and in recent years, controlling materials and elucidating their response in intense electromagnetic fields. THz fields can be generated in a lab setting using various plasma-based techniques. This study seeks to examine the interaction of two plasmas in order to better understand the fundamental physics associated with femtosecond filamentation processes and to achieve more efficient THz generation in a lab setting. The intensity of fluorescence in the region of overlap was measured as a function of polarization, power, and relative time delay of the two plasma-generating laser beams. Results of time dependent intensity studies indicate strikingly similar behaviors across polarizations and power levels; a sudden intensity spike was observed at time-zero, followed by a secondary maxima and subsequent decay to the initial plasma intensity. Dependence of the intensity on the power through either beam arm was also observed. Spectral studies of the enhanced emission were also carried out. Although this physical phenomenon is still not fully understood, future studies, including further spectral analysis of the fluorescence overlap, could yield new insight into the ultrafast processes occurring at the intersection of femtosecond filaments, and would provide a better understanding of the mechanisms for enhanced THz production.

  17. Cornea surgery with nanojoule femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Koenig, Karsten; Wang, Bagui; Riemann, Iris; Kobow, Jens

    2005-04-01

    We report on a novel optical method for (i) flap-generation in LASIK procedures as well as (ii) for flap-free intrastromal refractive surgery based on nanojoule femtosecond laser pulses. The near infrared 200 fs pulses for multiphoton ablation have been provided by ultracompact turn-key MHz laser resonators. LASIK flaps and intracorneal cavities have been realized with high precision within living New Zealand rabbits using the system FemtoCutO (JenLab GmbH, Jena, Germany) at 800 nm laser wavelength. Using low-energy sub-2 nJ laser pulses, collateral damage due to photodisruptive and self-focusing effects was avoided. The laser ablation system consists of fast galvoscanners, focusing optics of high numerical aperture as well as a sensitive imaging system and provides also the possibility of 3D multiphoton imaging of fluorescent cellular organelles and SHG signals from collagen. Multiphoton tomography of the cornea was used to determine the exact intratissue beam position and to visualize intraocular post-laser effects. The wound healing process has been investigated up to 90 days after instrastromal laser ablation by histological analysis. Regeneration of damaged collagen structures and the migration of inflammation cells have been detected.

  18. Femtosecond single-electron diffraction

    PubMed Central

    Lahme, S.; Kealhofer, C.; Krausz, F.; Baum, P.

    2014-01-01

    Ultrafast electron diffraction allows the tracking of atomic motion in real time, but space charge effects within dense electron packets are a problem for temporal resolution. Here, we report on time-resolved pump-probe diffraction using femtosecond single-electron pulses that are free from intra-pulse Coulomb interactions over the entire trajectory from the source to the detector. Sufficient average electron current is achieved at repetition rates of hundreds of kHz. Thermal load on the sample is avoided by minimizing the pump-probe area and by maximizing heat diffusion. Time-resolved diffraction from fibrous graphite polycrystals reveals coherent acoustic phonons in a nanometer-thick grain ensemble with a signal-to-noise level comparable to conventional multi-electron experiments. These results demonstrate the feasibility of pump-probe diffraction in the single-electron regime, where simulations indicate compressibility of the pulses down to few-femtosecond and attosecond duration. PMID:26798778

  19. Nanoflow electrospinning serial femtosecond crystallography

    SciTech Connect

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-11-01

    A low flow rate liquid microjet method for delivery of hydrated protein crystals to X-ray lasers is presented. Linac Coherent Light Source data demonstrates serial femtosecond protein crystallography with micrograms, a reduction of sample consumption by orders of magnitude. An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min{sup −1} to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min{sup −1} and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption.

  20. Femtosecond Photon-Counting Receiver

    NASA Technical Reports Server (NTRS)

    Krainak, Michael A.; Rambo, Timothy M.; Yang, Guangning; Lu, Wei; Numata, Kenji

    2016-01-01

    An optical correlation receiver is described that provides ultra-precise distance and/or time-pulse-width measurements even for weak (single photons) and short (femtosecond) optical signals. A new type of optical correlation receiver uses a fourth-order (intensity) interferometer to provide micron distance measurements even for weak (single photons) and short (femtosecond) optical signals. The optical correlator uses a low-noise-integrating detector that can resolve photon number. The correlation (range as a function of path delay) is calculated from the variance of the photon number of the difference of the optical signals on the two detectors. Our preliminary proof-of principle data (using a short-pulse diode laser transmitter) demonstrates tens of microns precision.

  1. Femtosecond Photon-Counting Receiver

    NASA Technical Reports Server (NTRS)

    Krainak, Michael A.; Rambo, Timothy M.; Yang, Guangning; Lu, Wei; Numata, Kenji

    2016-01-01

    An optical correlation receiver is described that provides ultra-precise distance and/or time/pulse-width measurements even for weak (single photons) and short (femtosecond) optical signals. A new type of optical correlation receiver uses a fourth-order (intensity) interferometer to provide micron distance measurements even for weak (single photons) and short (femtosecond) optical signals. The optical correlator uses a low-noise-integrating detector that can resolve photon number. The correlation (range as a function of path delay) is calculated from the variance of the photon number of the difference of the optical signals on the two detectors. Our preliminary proof-of principle data (using a short-pulse diode laser transmitter) demonstrates tens of microns precision.

  2. Infrared upconversion as a means of seeing in the dark. [based on nonlinear crystal optics

    NASA Technical Reports Server (NTRS)

    Gurski, T. R.

    1975-01-01

    A new approach to seeing in the dark is described which is based on the principles of nonlinear optics employing a crystal such as lithium iodate. A nonlinear optical device capable of producing photons at higher frequencies from lower-frequency incident light is shown to upconvert infrared light directly into visible light. The major advantages of the infrared upconversion process is that it permits the infrared signal to be detected by photon-counting devices presently available for the visible spectral region, and that it can provide sensitivity to infrared radiation without the need for cryogenic cooling of the detector used. Early works on infrared upconversion are reviewed. The development of applications is discussed as to astronomical spectroscopy and infrared image upconversion involving either angular or positional resolution elements. The demonstration of infrared upconversion in rectangular waveguides of single-crystal GaAs by Anderson et al. (1971) indicates future possibilities in upconversion by the use of integrated optics devices.

  3. Photon upconversion: from two-photon absorption (TPA) to triplet-triplet annihilation (TTA).

    PubMed

    Ye, Changqing; Zhou, Liwei; Wang, Xiaomei; Liang, Zuoqin

    2016-04-20

    Organic upconversion is a unique process in which low-energy light (usually NIR light) is converted to high-energy light through either the two-photon absorption (TPA) mechanism or the triplet-triplet annihilation (TTA) mechanism. Both TPA upconversion (TPA-UC) and TTA upconversion (TTA-UC) have been actively investigated in recent years due to their intriguing applications in optics, biophotonics, and solar energy utilization. Although they show some similarity (i.e., belonging to the nonlinear two-quantum process and needing focused excitation light), TPA-UC and TTA-UC are very different, such as in mechanism, characteristics involved, molecular design and potential applications. Here, we collectively reviewed these two kinds of upconversion processes and compared their respective characteristics and merits. We also present recent advances made in the areas of TPA- and TTA-UC, the remaining challenges and opportunities, with particular emphasis on molecular engineering of these two active upconversion materials. PMID:26843136

  4. Compositional and thermal effect on upconversion luminescence of Ho3+/Yb3+-codoped oxyfluoride glasses.

    PubMed

    Feng, Li; Su, Qiang; Li, Yan; Zheng, Chunrui; Wang, Cheng; Du, Hongli

    2009-07-01

    The upconversion luminescence properties of Ho3+/Yb3+-codoped SiO2-BaF2-ZnF2 glasses were investigated upon excitation with 980 nm diode laser. The visible emission bands centered at 546 and 661 nm correspond to 5F4, 5S2-->5I8 and 5F5-->5I8 transitions were observed. The effect of composition and temperature on the upconversion emission intensity was examined. It was found that the upconversion emission signals decrease with increasing ZnF2 content and temperature. The dependence of the upconversion emission intensity upon the excitation power was also examined, and the upconversion mechanisms were discussed. PMID:19237311

  5. Effects of chloride introduction on up-conversion luminescence in Tm3+ -doped tellurite glasses.

    PubMed

    Xu, Shiqing; Yang, Zhongmin; Wang, Guonian; Zhang, Junjie; Dai, Shixun; Hu, Lili; Jiang, Zhonghong

    2004-11-01

    Blue up-conversion luminescence properties in Tm3+ -doped lead chloride tellurite glasses have been studied under 980 nm excitation. The intense blue and relatively weak red emissions centered at 476 and 649 nm corresponding to the transitions 1G4 --> 3H6 and 1G4 --> 3H4 of Tm3+, respectively, are simultaneously observed at room temperature. The effect of PbCl2 on up-conversion intensity is observed and discussed, and possible up-conversion mechanisms are evaluated. The intense blue up-conversion luminescence of Tm3+ -doped lead chloride tellurite glasses may be a potentially useful material for developing up-conversion optical devices. PMID:15477139

  6. Effects of chloride introduction on up-conversion luminescence in Tm 3+-doped tellurite glasses

    NASA Astrophysics Data System (ADS)

    Xu, Shiqing; Yang, Zhongmin; Wang, Guonian; Zhang, Junjie; Dai, Shixun; Hu, Lili; Jiang, Zhonghong

    2004-11-01

    Blue up-conversion luminescence properties in Tm 3+-doped lead chloride tellurite glasses have been studied under 980 nm excitation. The intense blue and relatively weak red emissions centered at 476 and 649 nm corresponding to the transitions 1G4→ 3H6 and 1G4→ 3H4 of Tm 3+, respectively, are simultaneously observed at room temperature. The effect of PbCl 2 on up-conversion intensity is observed and discussed, and possible up-conversion mechanisms are evaluated. The intense blue up-conversion luminescence of Tm 3+-doped lead chloride tellurite glasses may be a potentially useful material for developing up-conversion optical devices.

  7. Modulation of a double-line frequency up-conversion process in cesium vapor

    NASA Astrophysics Data System (ADS)

    Gai, Baodong; Cao, Rui; Xia, Xusheng; Hu, Shu; Liu, Jinbo; Guo, Jingwei; Tan, Yannan; Liu, Wanfa; Jin, Yuqi; Sang, Fengting

    2016-06-01

    We have observed frequency up-conversion in Cs vapor. The pulsed pumping laser beam of 767.2 nm was converted to simultaneous collinear ultraviolet and blue radiation of wavelengths 387.7 and 455.6 nm, respectively (double-line frequency up-conversion). We examined properties of this up-conversion such as energy efficiency and pulse widths. An infrared laser of ~2.4 μm was successful in modulating the laser beam of the frequency up-conversion. The modulation shifts the wavelength of the blue radiation and the intensities of both the blue and ultraviolet radiation. At nanosecond grade, such modulations are expected to have applications in near-infrared up-conversion and optical communications.

  8. Nanoflow electrospinning serial femtosecond crystallography.

    PubMed

    Sierra, Raymond G; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W; Echols, Nathaniel; Gildea, Richard J; Grosse-Kunstleve, Ralf W; Sellberg, Jonas; McQueen, Trevor A; Fry, Alan R; Messerschmidt, Marc M; Miahnahri, Alan; Seibert, M Marvin; Hampton, Christina Y; Starodub, Dmitri; Loh, N Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H; Glatzel, Pieter; Milathianaki, Despina; White, William E; Adams, Paul D; Williams, Garth J; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K; Bogan, Michael J

    2012-11-01

    An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14-3.1 µl min(-1) to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min(-1) and diffracted to beyond 4 Å resolution, producing 14,000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption. PMID:23090408

  9. Time-Resolved Down-Conversion of 2-Aminopurine in a DNA Hairpin: Fluorescence Anisotropy and Solvent Effects

    NASA Astrophysics Data System (ADS)

    Tourón Touceda, Patricia; Gelot, Thomas; Crégut, Olivier; Léonard, Jérémie; Haacke, Stefan

    2013-03-01

    Femtosecond fluorescence anisotropy decay measured by type II difference frequency generation provides new insight into the local structural dynamics of ΔP(-)PBS fragments of the HIV- 1 DNA primary binding sequence, labeled with 2-aminopurine.

  10. In situ observation of photo-bleaching in human single living cell excited by a NIR femtosecond laser

    NASA Astrophysics Data System (ADS)

    Cho, Sung-Hak; Chang, Won-Seok; Kim, Jae-Goo; Whang, Kyoung-Hyun; Choi, Kyeong-Sook; Sohn, Seong-Hyang

    2008-03-01

    The photo-bleaching of single living cells excited by femtosecond laser irradiation was observed in situ to study the nonlinear interaction between ultrafast laser pulses and living human breast MDA-MB-231 cells. We conducted a systematic study of the energy dependence of plasma-mediated photo-disruption of fluorescently labeled subcellular structures in the nucleus of living cells using near-infrared (NIR) femtosecond laser pulses through a numerical aperture objective lens (0.75 NA). The behavior of photo-bleached living cells with fluorescently labeled nuclei was observed for 18 h after femtosecond laser irradiation under a fluorescence microscope. The photo-bleaching of single living cells without cell disruption occurred at between 470 and 630 nJ. To study the photo-disruption of subcellular organelles in single living cells using the nonlinear absorption excited by a NIR femtosecond laser pulse, the process of photo-bleaching without photo-disruption provides key information for clarifying the nonlinear interaction between NIR ultrashort, high-intensity laser light and transparent fluorescently labeled living cells.

  11. Upconversion Nanoparticles for Security Printing and CdSe QDs for Drug Delivery Applications

    NASA Astrophysics Data System (ADS)

    Baride, Aravind

    Upconversion is an anti-Stokes luminescence process, in which NIR excitation results in visible emission. Lanthanide ions, such as Yb3+ , Er3+ and Tm3+ ions, doped in beta-NaYF 4 crystals exhibit upconversion. Doped NaYF4 nanocrystals retain the bulk-like upconversion property in colloidal dispersions. The doping composition influences both the spectral output and efficiency of the upconversion emission. Red, green and blue primary color upconversion ink formulations were prepared using upconversion nanoparticles. We optimized the Er/Tm doping composition to produce spectrally pure red emitting nanoparticles. RGB upconversion inks were printed on various substrates and chromaticity of the printed features was investigated. Upconversion inks printed on substrates are not visible to the naked eye under ambient conditions, but the printed features appear upon 980 nm excitation. The upconversion inks, because of covertness, have numerous security printing and anti-counterfeiting applications. Colors produced by combinations of primary colors involving blue are excitation power density dependent. We evaluated the relation between the print density, excitation power density and chromaticity of the prints. In addition to NIR-to-visible inks, we also developed NIR-to-NIR inks for security printing systems. Spectrally pure NIR-to-NIR (980nm-to-800nm) emission was achieved by optimization of Yb/Tm doping composition. We demonstrated excitation and capture of NIR-to-NIR images from upconversion prints coated with NIR transparent materials. The upconversion inks described so far were prepared in non-polar ink bases. We also prepared upconversion inks in polar solvent bases. As synthesized nanoparticles are capped with oleic acid ligands. Polar solvent dispersibility of the nanoparticles was achieved by post-synthetic ligand exchange techniques. Polar-solvent-based upconversion inks were printed with a piezo inkjet and a thermal inkjet printer. In a second project, we

  12. Temperature-Sensing Behavior Based on Upconversion Luminescence at the Rhombohedral-Tetragonal Phase Boundary

    NASA Astrophysics Data System (ADS)

    Zou, Hua; Hu, Yifeng; Zhu, Xiaoqin; Zhang, Jianhao; Wang, Xusheng; Song, Zhitang

    2016-06-01

    In this work, (1-x)(K0.48Na0.52)(Nb0.95Sb0.05)O3-x -xEr0.5(Na0.82K0.18)0.5ZrO3 (x = 0-0.05) ceramics were fabricated by solid-state reaction techniques. The rhombohedral-tetragonal (R-T) phase boundary of the ceramics was identified at 0.04 ≤ x, thus providing an opportunity to investigate the upconversion emission derived from the Er3+ ions at the R-T phase boundary. Under 980 nm laser excitation, the R-T phase ceramics exhibited a strong green emission. In addition, the fluorescence intensity ratios of green emissions at 530 nm and 550 nm were investigated in a temperature range of 180-510 K, and maximum sensing sensitivity was found to be 0.0037 K-1. The results indicate that Er3+-doped ceramics with R-T phase boundaries can be applied to new multifunctional electro-optical temperature sensors. Laser excitation heating effects were also observed in detail.

  13. Upconversion luminescence resonance energy transfer-based aptasensor for the sensitive detection of oxytetracycline.

    PubMed

    Zhang, Hui; Fang, Congcong; Wu, Shijia; Duan, Nuo; Wang, Zhouping

    2015-11-15

    In this work, a biosensor based on luminescence resonance energy transfer (LRET) from NaYF4:Yb,Tm upconversion nanoparticles (UCNPs) to SYBR Green I has been developed. The aptamers are covalently linked to UCNPs and hybridized with their complementary strands. The subsequent addition of SYBR Green allows SYBR Green I to insert into the formed double-stranded DNA (dsDNA) duplex and brings the energy donor and acceptor into close proximity, leading to the fluorescence of UCNPs transferred to SYBR Green I. When excited at 980 nm, the UCNPs emit luminescence at 477 nm, and this energy is transferred to SYBR Green I, which emits luminescence at 530 nm. In the presence of oxytetracycline (OTC), the aptamers prefer to bind to its corresponding analyte and dehybridize with the complementary DNA. This dehybridization leads to the liberation of SYBR Green I, which distances SYBR Green I from the UCNPs and recovers the UCNPs' luminescence. Under optimal conditions, a linear calibration is obtained between the ratio of I530 to I477 nm (I530/I477) and the OTC concentration, which ranges from 0.1 to 10 ng/ml with a limit of detection (LOD) of 0.054 ng/ml. PMID:26302361

  14. Photophysical Properties and Efficient, Stable, Electrogenerated Chemiluminescence of Donor-Acceptor Molecules Exhibiting Thermal Spin Upconversion.

    PubMed

    Ishimatsu, Ryoichi; Edura, Tomohiko; Adachi, Chihaya; Nakano, Koji; Imato, Toshihiko

    2016-03-24

    The photophysical properties and electrogenerated chemiluminescence (ECL) of three donor-acceptor molecules composed of dicyanobenzene and methyl-, tert-butyl-, and phenyl-substituted carbazolyl groups, 1,2,3,5-tetrakis(3,6-disubstituted-carbazol-9-yl)-4,6-dicyanobenzene (4CzIPN-Me, 4CzIPN-tBu, and 4CzIPN-Ph, respectively) are described. These molecules show delayed fluorescence as a result of thermal spin upconversion from the lowest triplet state to the lowest singlet state at room temperature. The three molecules showed yellow to yellowish-red ECL. Remarkably, the ECL efficiencies of 4CzIPN-tBu in dichloromethane reached almost 40 %. Moreover, stable ECL was emitted from 4CzIPN-tBu and 4CzIPN-Ph. In case of 4CzIPN-Me, the ECL intensity decreased during voltage cycles because of polymerization. Quantum chemical calculations revealed that polymerization was inhibited by the steric hindrance of the bulky tert-butyl and phenyl groups on the carbazolyl moieties and lowered the spin density on the carbazolyl groups through electron conjugation for 4CzIPN-Ph. PMID:26916843

  15. Paramagnetism and improved upconversion luminescence properties of NaYF4:Yb,Er/NaGdF4 nanocomposites synthesized by a boiling water seed-mediated route

    NASA Astrophysics Data System (ADS)

    Yang, Chao-Qing; Li, Ao-Ju; Guo, Wei; Tian, Peng-Hua; Yu, Xiao-Long; Liu, Zhong-Xin; Cao, Yang; Sun, Zhong-Liang

    2016-03-01

    In a route boiling water served as reaction medium, a stoichiometric amount of rare-earth compound and fluoride are put into this system to form α-NaYF4:Yb, Er nuclei. Then prepared sample is heated at elevated temperature to improve the fluorescence intensity, and next a NaGdF4 shell grows on the surface of NaYF4 nuclei. NaYF4:Yb,Er/NaGdF4 core-shell structured upconversion nanoparticles (CSUCNPs) have been successfully synthesized by above route. The use of boiling water decreases the cubic-to-hexagonal phase transition temperature of NaYF4:Yb,Er to 350°C and increases its upconversion (UC) luminescence intensity. A heterogeneous NaGdF4 epitaxially growing on the surface of Ln3+-doped NaYF4 not only improves UC luminescence, but also creates a paramagnetic shell, which can be used as contrast agents in magnetic resonance imaging (MRI). The solution of CSUCNPs shows bright green UC fluorescence under the excitation at 980 nm in a power density only about 50 mW·cm-2. A broad spectrum with a dominant resonance at g of about 2 is observed by the electron paramagnetic resonance (EPR) spectrum of CSUCNPs. Above properties suggest that the obtained CSUCNPs could be potential candidates for dual-mode optical/magnetic bioapplications.

  16. 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

    2016-10-01

    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. PMID:27284763

  17. Molecular fragmentation induced by a femtosecond laser

    NASA Astrophysics Data System (ADS)

    Kosmidis, Constantine E.; Ledingham, Kenneth W. D.; Kilic, H. S.; McCanny, T.; Singhal, Raghunandan P.; Smith, D.; Langley, Andrew J.

    1998-07-01

    The 90 femtosecond laser induced fragmentation at 375 nm for a number of different nitro-molecules is compared to that induced by a nanosecond laser at the same wavelength by means of time-of-flight mass spectrometry. The potential of femtosecond laser mass spectrometry for analytical purposes is discussed.

  18. 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. PMID:26487489

  19. Attenuated total reflectance spectroscopy with chirped-pulse upconversion.

    PubMed

    Shirai, Hideto; Duchesne, Constance; Furutani, Yuji; Fuji, Takao

    2014-12-01

    Chirped-pulse upconversion technique has been applied to attenuated total reflectance (ATR) infrared spectroscopy. An extremely broadband infrared pulse was sent to an ATR diamond prism and the reflected pulse was converted to the visible by using four-wave mixing in krypton gas. Absorption spectra of liquids in the range from 200 to 5500 cm(-1) were measured with a visible spectrometer on a single-shot basis. The system was applied to observe the dynamics of exchanging process of two solvents, water and acetone, which give clear vibrational spectral contrast. We observed that the exchange was finished within ∼ 10 ms. PMID:25606893

  20. Transparent organic upconversion devices for near-infrared sensing.

    PubMed

    Liu, Shun-Wei; Lee, Chih-Chien; Yuan, Chih-Hsien; Su, Wei-Cheng; Lin, Shao-Yu; Chang, Wen-Chang; Huang, Bo-Yao; Lin, Chun-Feng; Lee, Ya-Ze; Su, Tsung-Hao; Chen, Kuan-Ting

    2015-02-18

    Transparent organic upconversion devices are shown in a night-vision demonstration of a real object under near-infrared (NIR) illumination in the dark. An extraordinarily high current gain - reflecting the on-off switching effect - greater than 15 000 at a driving voltage of 3 V is demonstrated, indicating the high sensitivity to NIR light and potential of using the proposed upconverter in practical applications. A maximum luminance exceeding 1500 cd m(-2) at 7 V is achieved. Unlike previous studies, where 2D aperture projection is reported, the current study shows 3D images of real objects under NIR illumination in the dark. PMID:25504521

  1. Photon upconversion in degenerately sulfur doped InP nanowires.

    PubMed

    Mergenthaler, K; Lehmann, S; Wallentin, J; Zhang, W; Borgström, M T; Yartsev, A; Pistol, M-E

    2015-12-28

    Radiative recombination in degenerately n-doped InP nanowires is studied for excitation above and below the Fermi energy of the electron gas, using photoluminescence. Laser-induced electron heating is observed, which allows absorption below the Fermi energy. We observe photon upconversion where photo-excited holes recombine with high |k| electrons. This can be attributed to hole scattering to high |k|-values, and the temperature dependence of this process is measured. We show that hole relaxation via phonon scattering can be observed in continuous wave excitation luminescence measurements. PMID:26585229

  2. Core-shell hybrid upconversion nanoparticles carrying stable nitroxide radicals as potential multifunctional nanoprobes for upconversion luminescence and magnetic resonance dual-modality imaging

    NASA Astrophysics Data System (ADS)

    Chen, Chuan; Kang, Ning; Xu, Ting; Wang, Dong; Ren, Lei; Guo, Xiangqun

    2015-03-01

    Nitroxide radicals, such as 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) and its derivatives, have recently been used as contrast agents for magnetic resonance imaging (MRI) and electron paramagnetic resonance imaging (EPRI). However, their rapid one-electron bioreduction to diamagnetic N-hydroxy species when administered intravenously has limited their use in in vivo applications. In this article, a new approach of silica coating for carrying stable radicals was proposed. A 4-carboxyl-TEMPO nitroxide radical was covalently linked with 3-aminopropyl-trimethoxysilane to produce a silanizing TEMPO radical. Utilizing a facile reaction based on the copolymerization of silanizing TEMPO radicals with tetraethyl orthosilicate in reverse microemulsion, a TEMPO radicals doped SiO2 nanostructure was synthesized and coated on the surface of NaYF4:Yb,Er/NaYF4 upconversion nanoparticles (UCNPs) to generate a novel multifunctional nanoprobe, PEGylated UCNP@TEMPO@SiO2 for upconversion luminescence (UCL) and magnetic resonance dual-modality imaging. The electron spin resonance (ESR) signals generated by the TEMPO@SiO2 show an enhanced reduction resistance property for a period of time of up to 1 h, even in the presence of 5 mM ascorbic acid. The longitudinal relaxivity of PEGylated UCNPs@TEMPO@SiO2 nanocomposites is about 10 times stronger than that for free TEMPO radicals. The core-shell NaYF4:Yb,Er/NaYF4 UCNPs synthesized by this modified user-friendly one-pot solvothermal strategy show a significant enhancement of UCL emission of up to 60 times more than the core NaYF4:Yb,Er. Furthermore, the PEGylated UCNP@TEMPO@SiO2 nanocomposites were further used as multifunctional nanoprobes to explore their performance in the UCL imaging of living cells and T1-weighted MRI in vitro and in vivo.Nitroxide radicals, such as 2,2,6,6-tetramethylpiperidine 1-oxyl (TEMPO) and its derivatives, have recently been used as contrast agents for magnetic resonance imaging (MRI) and electron

  3. Highly efficient Yb3+/Tm3+ co-doped NaYF4 nanotubes: Synthesis and intense ultraviolet to infrared up-conversion luminescence

    NASA Astrophysics Data System (ADS)

    Zhang, Y. Y.; Wang, Y.; Deng, J. Q.; Wang, J.; Ni, S. C.

    2014-02-01

    Nanocrystals of up-conversion (UC) phosphor Yb3+/Tm3+ co-doped NaYF4 are prepared by a facile hydrothermal method using oleic acid as a stabilizing agent. The as-prepared nanocrystals are of hexagonal phase, and have tube-like morphology and strong ultraviolet (UV) and blue UC fluorescence intensity, which have been characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and luminescence spectroscopy. The effect of Yb3+ concentration on the UC emission properties is also analyzed. Our results reveal that the intensity of emission peaks can be controlled by varying the Yb3+ concentration and these NaYF4 nanotubes are highly efficient host material. The as-prepared NaYF4 nanotubes show potential applications in UV compact solid state lasers and multi-channel fluorescent label.

  4. Mercaptopropionic acid-capped Mn(2+):ZnSe/ZnO quantum dots with both downconversion and upconversion emissions for bioimaging applications.

    PubMed

    Zhao, Bingxia; Yao, Yulian; Yang, Kai; Rong, Pengfei; Huang, Peng; Sun, Kang; An, Xiao; Li, Zhiming; Chen, Xiaoyuan; Li, Wanwan

    2014-11-01

    Doped quantum dots (d-dots) can serve as fluorescent biosensors and biolabels for biological applications. Our study describes a synthesis of mercaptopropionic acid (MPA)-capped Mn(2+):ZnSe/ZnO d-dots through a facile, cost-efficient hydrothermal route. The as-prepared water-soluble d-dots exhibit strong emission at ca. 580 nm, with a photoluminescence quantum yield (PLQY) as high as 31%, which is the highest value reported to date for such particles prepared via an aqueous route. They also exhibit upconversion emission when excited at 800 nm. With an overall diameter of around 6.7 nm, the d-dots could gain access to the cell nucleus without any surface decoration, demonstrating their promising broad applications as fluorescent labels. PMID:25189675

  5. Nanoflow electrospinning serial femtosecond crystallography

    PubMed Central

    Sierra, Raymond G.; Laksmono, Hartawan; Kern, Jan; Tran, Rosalie; Hattne, Johan; Alonso-Mori, Roberto; Lassalle-Kaiser, Benedikt; Glöckner, Carina; Hellmich, Julia; Schafer, Donald W.; Echols, Nathaniel; Gildea, Richard J.; Grosse-Kunstleve, Ralf W.; Sellberg, Jonas; McQueen, Trevor A.; Fry, Alan R.; Messerschmidt, Marc M.; Miahnahri, Alan; Seibert, M. Marvin; Hampton, Christina Y.; Starodub, Dmitri; Loh, N. Duane; Sokaras, Dimosthenis; Weng, Tsu-Chien; Zwart, Petrus H.; Glatzel, Pieter; Milathianaki, Despina; White, William E.; Adams, Paul D.; Williams, Garth J.; Boutet, Sébastien; Zouni, Athina; Messinger, Johannes; Sauter, Nicholas K.; Bergmann, Uwe; Yano, Junko; Yachandra, Vittal K.; Bogan, Michael J.

    2012-01-01

    An electrospun liquid microjet has been developed that delivers protein microcrystal suspensions at flow rates of 0.14–3.1 µl min−1 to perform serial femtosecond crystallography (SFX) studies with X-ray lasers. Thermolysin microcrystals flowed at 0.17 µl min−1 and diffracted to beyond 4 Å resolution, producing 14 000 indexable diffraction patterns, or four per second, from 140 µg of protein. Nanoflow electrospinning extends SFX to biological samples that necessitate minimal sample consumption. PMID:23090408

  6. Dynamics of the up-conversion emission in holmium doped ZBLAN fiber

    NASA Astrophysics Data System (ADS)

    Wnuk, A.; Kaczkan, M.; Piramidowicz, R.; Mahiou, R.; Bertrand, G.; Joubert, M. F.; Malinowski, M.

    2003-01-01

    The dynamics of up-conversion, green emission under excitation at different infra-red wavelength in Ho3+ doped ZBLAN fiber is reported. Under infrared, 890 nm quasi cw pumping the complicated temporal behavior of the up-conversion signal is strongly influenced by the intermediate I-5(5) state cross relaxation. The mechanisms of the observed up-conversion processes are proposed and the time evolution of the S-5(2) population is described by the rate equation model. Parameters of the model are determined and numerical simulations of the excited state dynamics are performed.

  7. Metallophthalocyanines as triplet sensitizers for highly efficient photon upconversion based on sensitized triplet-triplet annihilation.

    PubMed

    Han, J L; You, J; Yonemura, H; Yamada, S; Wang, S R; Li, X G

    2016-08-01

    Soluble palladium and platinum phthalocyanines with coumarin moieties were synthesized with Q bands in the red and near-IR regions, in which the molar extinction coefficients were up to 1.01 × 10(5) cm(-1) mol(-1). These metallophthalocyanines were coupled with rubrene and applied in photon upconversion systems based on triplet-triplet annihilation. The highest upconversion efficiency of the palladium phthalocyanine was 5.6%, which is higher than that of the platinum phthalocyanine-rubrene system. The larger molar extinction coefficient resulted in high upconversion capability (>10(5) cm(-1) mol(-1)) and low saturation incident power (<20 mW cm(-2)). PMID:27431880

  8. Upconversion luminescence in BaMoO4:Pr3+ phosphor for display devices

    NASA Astrophysics Data System (ADS)

    Soni, Abhishek Kumar; Rai, Vineet Kumar

    2015-08-01

    The frequency upconversion is an important nonlinear optical property by which near infrared light is converted into the visible light. The BaMoO4:Pr3+ 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.

  9. High-power femtosecond pulse generation in a passively mode-locked Nd:SrLaAlO4 laser

    NASA Astrophysics Data System (ADS)

    Liu, Shan-De; Dong, Lu-Lu; Zheng, Li-He; Berkowski, Marek; Su, Liang-Bi; Ren, Ting-Qi; Peng, Yan-Dong; Hou, Jia; Zhang, Bai-Tao; He, Jing-Liang

    2016-07-01

    A high optical quality Nd:SrLaAlO4 (Nd:SLA) crystal was grown using the Czochralski method and showed broad fluorescence spectrum with a full width at half maximum value of 34 nm, which is beneficial for generating femtosecond laser pulses. A stable diode-pumped passively mode-locked femtosecond Nd:SLA laser with 458 fs pulse duration was achieved for the first time at a central wavelength of 1077.9 nm. The average output power of the continuous-wave mode-locked laser was 520 mW and the repetition rate was 78.5 MHz.

  10. Ti:Sapphire micro-structures by femtosecond laser inscription: Guiding and luminescence properties

    NASA Astrophysics Data System (ADS)

    Ren, Yingying; Jiao, Yang; Vázquez de Aldana, Javier R.; Chen, Feng

    2016-08-01

    We report on the fabrication of buried cladding waveguides with different diameters in a Ti:Sapphire crystal by femtosecond laser inscription. The propagation properties are studied, showing that the cladding waveguides could support near- to mid-infrared waveguiding at both TE and TM polarizations. Confocal micro-photoluminescence experiments reveal that the original fluorescence properties in the waveguide region are very well preserved, while it suffers from a strong quenching at the centers of laser induced filaments. Broadband waveguide fluorescence emissions with high efficiency are realized, indicating the application of the cladding waveguides in Ti:Sapphire as compact broadband luminescence sources in biomedical fields.

  11. Visible light-absorbing rhenium(I) tricarbonyl complexes as triplet photosensitizers in photooxidation and triplet-triplet annihilation upconversion.

    PubMed

    Yi, Xiuyu; Zhao, Jianzhang; Sun, Jifu; Guo, Song; Zhang, Hongli

    2013-02-14

    We prepared N^N Re(I) tricarbonyl chloride complexes (Re-1 and Re-2) that give very strong absorption of visible light. To this end, it is for the first time that boron dipyrimethane (Bodipy) was used to prepare Re(I) tricarbonyl chloride complexes. The π-conjugation linker between the π-conjugation framework of the antenna Bodipy and the Re(I) coordination centre ensures efficient intersystem crossing (ISC). Re-0 without visible light-harvesting ligand was prepared as a model complex in the photophysical studies. Re-1 (with Bodipy) and Re-2 (with carbazole-ethynyl Bodipy) show unprecedented strong absorption of visible light at 536 nm (ε = 91700 M(−1) cm(−1)) and 574 nm (ε = 64,600 M(−1) cm(−1)), respectively. Interestingly, different from Re-0, Re-1 and Re-2 show fluorescence of the ligand, not the phosphorescence of the Re(I) coordination centre. However, long-lived triplet excited states were observed upon visible light excitation (τ(T) = 104.0 μs for Re-1; τ(T) = 127.2 μs for Re-2) vs. the short lifetime of Re-0 (τ(T) = 26 ns). With nanosecond time-resolved transient absorption spectroscopy and DFT calculations, we proved that the triplet excited states of Re-1 and Re-2 are localized on the Bodipy ligands. The complexes were used as triplet photosensitizers for two triplet–triplet-energy-transfer (TTET) processes, i.e.(1)O(2) mediated photooxidation and triplet–triplet annihilation (TTA) upconversion. With the strong visible light-harvesting ability, Re-1 proved to be a better (1)O(2) photosensitizer than the conventional triplet photosensitizer tetraphenylporphyrin (TPP). Significant upconversion was observed with Re-1 as the triplet photosensitizer. Our result is useful for preparation of Re(I) tricarbonyl chloride complexes that show strong absorption of visible light and long-lived triplet excited states and for the application of these complexes as triplet photosensitizers in photocatalysis, photodynamic therapy and TTA upconversion

  12. Frequency Up-Conversion Photon-Type Terahertz Imager.

    PubMed

    Fu, Z L; Gu, L L; Guo, X G; Tan, Z Y; Wan, W J; Zhou, T; Shao, D X; Zhang, R; Cao, J C

    2016-01-01

    Terahertz imaging has many important potential applications. Due to the failure of Si readout integrated circuits (ROICs) and the thermal mismatch between the photo-detector arrays and the ROICs at temperatures below 40 K, there are big technical challenges to construct terahertz photo-type focal plane arrays. In this work, we report pixel-less photo-type terahertz imagers based on the frequency up-conversion technique. The devices are composed of terahertz quantum-well photo-detectors (QWPs) and near-infrared (NIR) light emitting diodes (LEDs) which are grown in sequence on the same substrates using molecular beam epitaxy. In such an integrated QWP-LED device, photocurrent in the QWP drives the LED to emit NIR light. By optimizing the structural parameters of the QWP-LED, the QWP part and the LED part both work well. The maximum values of the internal and external energy up-conversion efficiencies are around 20% and 0.5%. A laser spot of a homemade terahertz quantum cascade laser is imaged by the QWP-LED together with a commercial Si camera. The pixel-less imaging results show that the image blurring induced by the transverse spreading of photocurrent is negligible. The demonstrated pixel-less imaging opens a new way to realize high performance terahertz imaging devices. PMID:27147281

  13. Photon upconversion in degenerately sulfur doped InP nanowires

    NASA Astrophysics Data System (ADS)

    Mergenthaler, K.; Lehmann, S.; Wallentin, J.; Zhang, W.; Borgström, M. T.; Yartsev, A.; Pistol, M.-E.

    2015-12-01

    Radiative recombination in degenerately n-doped InP nanowires is studied for excitation above and below the Fermi energy of the electron gas, using photoluminescence. Laser-induced electron heating is observed, which allows absorption below the Fermi energy. We observe photon upconversion where photo-excited holes recombine with high |k| electrons. This can be attributed to hole scattering to high |k|-values, and the temperature dependence of this process is measured. We show that hole relaxation via phonon scattering can be observed in continuous wave excitation luminescence measurements.Radiative recombination in degenerately n-doped InP nanowires is studied for excitation above and below the Fermi energy of the electron gas, using photoluminescence. Laser-induced electron heating is observed, which allows absorption below the Fermi energy. We observe photon upconversion where photo-excited holes recombine with high |k| electrons. This can be attributed to hole scattering to high |k|-values, and the temperature dependence of this process is measured. We show that hole relaxation via phonon scattering can be observed in continuous wave excitation luminescence measurements. Electronic supplementary information (ESI) available. See DOI: 10.1039/C5NR05472A

  14. Frequency Up-Conversion Photon-Type Terahertz Imager

    PubMed Central

    Fu, Z. L.; Gu, L. L.; Guo, X. G.; Tan, Z. Y.; Wan, W. J.; Zhou, T.; Shao, D. X.; Zhang, R.; Cao, J. C.

    2016-01-01

    Terahertz imaging has many important potential applications. Due to the failure of Si readout integrated circuits (ROICs) and the thermal mismatch between the photo-detector arrays and the ROICs at temperatures below 40 K, there are big technical challenges to construct terahertz photo-type focal plane arrays. In this work, we report pixel-less photo-type terahertz imagers based on the frequency up-conversion technique. The devices are composed of terahertz quantum-well photo-detectors (QWPs) and near-infrared (NIR) light emitting diodes (LEDs) which are grown in sequence on the same substrates using molecular beam epitaxy. In such an integrated QWP-LED device, photocurrent in the QWP drives the LED to emit NIR light. By optimizing the structural parameters of the QWP-LED, the QWP part and the LED part both work well. The maximum values of the internal and external energy up-conversion efficiencies are around 20% and 0.5%. A laser spot of a homemade terahertz quantum cascade laser is imaged by the QWP-LED together with a commercial Si camera. The pixel-less imaging results show that the image blurring induced by the transverse spreading of photocurrent is negligible. The demonstrated pixel-less imaging opens a new way to realize high performance terahertz imaging devices. PMID:27147281

  15. WDM up-conversion employing frequency quadrupling in optical modulator.

    PubMed

    Shih, Po-Tsung; Lin, Chun-Ting; Jiang, Wen-Jr; Chen, Jason Jyehong; Huang, Han-Sheng; Chen, Yu-Hung; Peng, Peng-Chun; Chi, Sien

    2009-02-01

    This work presents an optical up-conversion system with frequency quadrupling for wavelength-division-multiplexing (WDM) communication systems using a dual-parallel Mach-Zehnder modulator without optical filtering. Four-channel 1.25-Gb/s wired fiber-to-the-x (FTTx) and wireless radio-over-fiber (RoF) signals are generated and transmitted simultaneously. Moreover, the decline in receiver sensitivities due to Mach-Zehnder modulator bias drifts is also investigated. Receiver power penalties of the 20-GHz up-converted WDM signals and baseband (BB) FTTx signals are less than 1 dB when bias deviation voltage is less the 20% of the half-wave voltage. After transmission over a 50-km SSMF, the receiver power penalties of both the BB and 20-GHz RF OOK signals are less than 1 dB. Notably, 60-GHz optical up-conversion can be achieved using 15-GHz radio frequency (RF) components and equipment. PMID:19189002

  16. 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

    2015-11-01

    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. PMID:26358961

  17. Frequency Up-Conversion Photon-Type Terahertz Imager

    NASA Astrophysics Data System (ADS)

    Fu, Z. L.; Gu, L. L.; Guo, X. G.; Tan, Z. Y.; Wan, W. J.; Zhou, T.; Shao, D. X.; Zhang, R.; Cao, J. C.

    2016-05-01

    Terahertz imaging has many important potential applications. Due to the failure of Si readout integrated circuits (ROICs) and the thermal mismatch between the photo-detector arrays and the ROICs at temperatures below 40 K, there are big technical challenges to construct terahertz photo-type focal plane arrays. In this work, we report pixel-less photo-type terahertz imagers based on the frequency up-conversion technique. The devices are composed of terahertz quantum-well photo-detectors (QWPs) and near-infrared (NIR) light emitting diodes (LEDs) which are grown in sequence on the same substrates using molecular beam epitaxy. In such an integrated QWP-LED device, photocurrent in the QWP drives the LED to emit NIR light. By optimizing the structural parameters of the QWP-LED, the QWP part and the LED part both work well. The maximum values of the internal and external energy up-conversion efficiencies are around 20% and 0.5%. A laser spot of a homemade terahertz quantum cascade laser is imaged by the QWP-LED together with a commercial Si camera. The pixel-less imaging results show that the image blurring induced by the transverse spreading of photocurrent is negligible. The demonstrated pixel-less imaging opens a new way to realize high performance terahertz imaging devices.

  18. Probing the nature of upconversion nanocrystals: instrumentation matters.

    PubMed

    Liu, Xiaowang; Deng, Renren; Zhang, Yuhai; Wang, Yu; Chang, Hongjin; Huang, Ling; Liu, Xiaogang

    2015-03-21

    Probing the nature of nanocrystalline materials such as the surface state, crystal structure, morphology, composition, optical and magnetic characteristics is a crucial step in understanding their chemical and physical performance and in exploring their potential applications. Upconversion nanocrystals have recently attracted remarkable interest due to their unique nonlinear optical properties capable of converting incident near-infrared photons to visible and even ultraviolet emissions. These optical nanomaterials also hold great promise for a broad range of applications spanning from biolabeling to optoelectronic devices. In this review, we overview the instrumentation techniques commonly utilized for the characterization of upconversion nanocrystals. A considerable emphasis is placed on the analytical tools for probing the optical properties of the luminescent nanocrystals. The advantages and limitations of each analytical technique are compared in an effort to provide a general guideline, allowing optimal conditions to be employed for the characterization of such nanocrystals. Parallel efforts are devoted to new strategies that utilize a combination of advanced emerging tools to characterize such nanosized phosphors. PMID:25693872

  19. Low phase noise microwave extraction from femtosecond laser by frequency conversion pair and IF-domain processing.

    PubMed

    Dai, Yitang; Cen, Qizhuang; Wang, Lei; Zhou, Yue; Yin, Feifei; Dai, Jian; Li, Jianqiang; Xu, Kun

    2015-12-14

    Extraction of a microwave component from a low-time-jitter femtosecond pulse train has been attractive for current generation of spectrally pure microwave. In order to avoid the transfer from the optical amplitude noise to microwave phase noise (AM-PM), we propose to down-convert the target component to intermediate frequency (IF) before the opto-electronic conversion. Due to the much lower carrier frequency, the AM-PM is greatly suppressed. The target is then recovered by up-conversion with the same microwave local oscillation (LO). As long as the time delay of the second LO matches that of the IF carrier, the phase noise of the LO shows no impact on the extraction process. The residual noise of the proposed extraction is analyzed in theory, which is also experimentally demonstrated as averagely around -155 dBc/Hz under offset frequency larger than 1 kHz when 10-GHz tone is extracted from a home-made femtosecond fiber laser. Large tunable extraction from 1 GHz to 10 GHz is also reported. PMID:26698985

  20. 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.

  1. Surface plasmon resonance enhanced upconversion luminescence in aqueous media for TNT selective detection.

    PubMed

    Tu, Nina; Wang, Leyu

    2013-07-18

    We present a novel report on a surface plasmon resonance enhanced upconversion luminescence strategy in aqueous media for highly sensitive and selective detection of 2,4,6-trinitrotoluene (TNT). PMID:23739225

  2. Metal-Organic Frameworks Modulated by Doping Er(3+) for Up-Conversion Luminescence.

    PubMed

    Zhang, Xindan; Li, Bin; Ma, Heping; Zhang, Liming; Zhao, Haifeng

    2016-07-13

    Here we present metal-organic frameworks prepared by a one-step synthesis method, possessing both architectural properties of MOF building and up-conversion luminescence of rare earth Er(3+) (hereafter denoted as Up-MOFs). Up-MOFs have characteristic up-conversion emissions at 520, 540, and 651 nm under the excitation of 980 nm owing to the multiple photon absorption. The up-conversion mechanism of these Up-MOFs has been discussed, and it can be attributed to the excited state absorption process. The design and synthesis of Up-MOF materials possessing near-infrared region excitation and up-conversion luminescence are fully expected to be candidates for the advancement of applications in bioimaging, sensors, optoelectronics, and energy conversion/storage devices. PMID:27315339

  3. Up-conversion and Photoluminescence in Er3+ Single Crystal MgAl-spinel

    NASA Astrophysics Data System (ADS)

    Mironova-Ulmane, N.; Sarakovskis, A.; Skvortsova, V.

    Traditional and up-conversion luminescence of MgAl2O4 single crystal doped with erbium ions obtained by the Verneuil method has been investigated. The time resolved spectral measurements of the green and red up-conversion luminescence bands show that a build-up part is present in the up-conversion luminescence kinetics. This means that energy transfer process is involved in the creation of the luminescence. Considering rather small concentration of Er3+ in the material (0.12 mass %), the expected up-conversion mechanism should be excited state absorption since the average distance between erbium ions is high. The above-mentioned considerations suggest that clustering of the activator ions is present in the material, which is supported by SEM analysis.

  4. Plasmon-Enhanced Upconversion Luminescence on Vertically Aligned Gold Nanorod Monolayer Supercrystals.

    PubMed

    Yin, Ze; Zhou, Donglei; Xu, Wen; Cui, Shaobo; Chen, Xu; Wang, He; Xu, Shihan; Song, Hongwei

    2016-05-11

    Upconversion nanophosphor is attracting worldwide interests owing to its unique optical properties and great application potentials. However, it is still a great challenge to effectively improve the efficiency/strength of upconversion nanophosphor. Plasmonic modulation is a promising way to solve this bottleneck. In this work, we present a simple yet versatile concept on magnifying upconversion luminescence of NaYF4:Yb(3+), Er(3+) nanocrystals through local field manipulation of surface plasmon. Gold nanorods were directionally assembled into a vertically aligned monolayer supercrystals over large areas. The FDTD simulation indicates that the electromagnetic field strength |E|(2) can be improved about 113 folds at the hot spots of monolayer supercrystals. After optimization, on the surface of the vertically aligned monolayer supercrystals, the overall upconversion luminescence intensity of NaYF4:Yb(3+), Er(3+) under 980 nm excitation was improved more than 35 fold. PMID:27111717

  5. Recent emergence of photon upconversion based on triplet energy migration in molecular assemblies.

    PubMed

    Yanai, Nobuhiro; Kimizuka, Nobuo

    2016-04-01

    An emerging field of triplet energy migration-based photon upconversion (TEM-UC) is reviewed. Highly efficient photon upconversion has been realized in a wide range of chromophore assemblies, such as non-solvent liquids, ionic liquids, amorphous solids, gels, supramolecular assemblies, molecular crystals, and metal-organic frameworks (MOFs). The control over their assembly structures allows for unexpected air-stability and maximum upconversion quantum yield at weak solar irradiance that has never been achieved by the conventional molecular diffusion-based mechanism. The introduction of the "self-assembly" concept offers a new perspective in photon upconversion research and triplet exciton science, which show promise for numerous applications ranging from solar energy conversion to chemical biology. PMID:26947379

  6. Up-conversion single-photon detector using multi-wavelength sampling techniques.

    PubMed

    Ma, Lijun; Bienfang, Joshua C; Slattery, Oliver; Tang, Xiao

    2011-03-14

    The maximum achievable data-rate of a quantum communication system can be critically limited by the efficiency and temporal resolution of the system's single-photon detectors. Frequency up-conversion technology can be used to increase detection efficiency for IR photons. In this paper we describe a scheme to improve the temporal resolution of an up-conversion single-photon detector using multi-wavelength optical-sampling techniques, allowing for increased transmission rates in single-photon communications systems. We experimentally demonstrate our approach with an up-conversion detector using two spectrally and temporally distinct pump pulses, and show that it allows for high-fidelity single-photon detection at twice the rate supported by a conventional single-pump up-conversion detector. We also discuss the limiting factors of this approach and identify important performance-limiting trade offs. PMID:21445185

  7. 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. PMID:27451700

  8. Internal upconversion and doubling of an optical parametric oscillator to extend the tuning range.

    NASA Technical Reports Server (NTRS)

    Campillo, A. J.

    1972-01-01

    Efficient extension of the tuning range of a 1.09-1.95-micron parametric oscillator to 0.435-0.975 microns by upconversion and doubling internally to the oscillator cavity is reported. Unlike previously studied external mixing, internal upconversion and doubling yielded uniform powers of 30 and 60 kW, respectively, over the entire extended tuning range with an unfocused 2-mm ruby laser pump beam of 750 kW.-

  9. Preparation of ZnO nanoparticles showing upconversion luminescence through simple chemical method

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

    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.

  10. Characterization and control of peak intensity distribution at the focus of a spatiotemporally focused femtosecond laser beam.

    PubMed

    He, Fei; Zeng, Bin; Chu, Wei; Ni, Jielei; Sugioka, Koji; Cheng, Ya; Durfee, Charles G

    2014-04-21

    We report on experimental examination of two-photon fluorescence excitation (TPFE) at the focus of a spatially chirped femtosecond laser beam, which reveals an unexpected tilted peak intensity distribution in the focal spot. Our theoretical calculation shows that the tilting of the peak intensity distribution originates from the fact that along the optical axis of objective lens, the spatiotemporally focused pulse reaches its shortest duration exactly at the focal plane. However, when moving away from the optical axis along the direction of spatial chirp of the incident pulse, the pulse reaches its shortest duration either before or after the focal plane, depending on whether the pulse duration is measured above or below the optical axis as well as the sign of the spatial chirp. The tilting of the peak intensity distribution in the focal spot of the spatiotemporally focused femtosecond laser beam can play important roles in applications such as femtosecond laser micromachining and bio-imaging. PMID:24787858

  11. Spectroscopic analysis of femtosecond laser plasma filament in air

    NASA Astrophysics Data System (ADS)

    Bernhardt, J.; Liu, W.; Théberge, F.; Xu, H. L.; Daigle, J. F.; Châteauneuf, M.; Dubois, J.; Chin, S. L.

    2008-03-01

    We report a spectroscopic analysis of a filament generated by a femtosecond laser pulse in air. In the filament spectra, the characteristic Stark broadened atomic oxygen triplet centered at 777.4 nm has been observed. The measured electron impact Stark broadening parameter of the triplet is larger than the theoretical value by Griem [H.R. Griem, Plasma Spectroscopy, McGraw Hill, New York, 1964] by a factor 6.7 . Using the experimental value 0.0166nm , the plasma densities derived from Stark broadening agree well with those most recently obtained from Théberge et al.'s measurement of the nitrogen fluorescence calibrated by longitudinal diffraction [F. Théberge, W. Liu, P.T. Simard, A. Becker, S. L. Chin, Phys. Rev. E 74 (2006) 036406]. However, the Stark broadening approach is much simpler and can be used to non-invasively measure the filament plasma density distribution in air under different propagation conditions.

  12. Multiphoton excitation fluorescence correlation spectroscopy of fluorescent DNA base analogs

    NASA Astrophysics Data System (ADS)

    Katilius, Evaldas; Woodbury, Neal W.

    2004-06-01

    Two- and three-photon excitation was used to investigate the properties of two fluorescent DNA base analogs: 2-aminopurine and 6-methylisoxanthopterin. 2-aminopurine is a widely used fluorescent analog of the DNA base adenine. Three-photon excitation of 2-aminopurine is achievable by using intense femtosecond laser pulses in 850-950 nm spectral region. Interestingly, the three-photon excitation spectrum is blue-shifted relative to the three-times-wavelength single-photon excitation spectrum. The maximum of the absorbance band in the UV is at 305 nm, while the three-photon excitation spectrum has a maximum at around 880 nm. Fluorescence correlation measurements were attempted to evaluate the feasibility of using three-photon excitation of 2-aminopurine for DNA-protein interaction studies. However, due to relatively small three-photon absorption cross-section, a good signal-to-noise fluorescence correlation curves take very long time to obtain. Fluorescence properties of 6-methylisoxanthopterin, the fluorescent analog of guanine, were investigated using two-photon excitation. This molecule has the lowest energy absorption band centered around 350 nm, thus, two-photon excitation is attainable using 700 to 760 nm output of Ti-sapphire laser. The excitation spectrum of this molecule in the infrared well matches the doubled-wavelength single-photon excitation spectrum in the UV. The high fluorescence quantum yield of 6-methylisoxanthopterin allows efficient fluorescence correlation measurements and makes this molecule a very good candidate for using in in vitro DNA-protein interaction studies.

  13. Programmable femtosecond laser pulses in the ultraviolet

    SciTech Connect

    Hacker, M.; Feurer, T.; Sauerbrey, R.; Lucza, T.; Szabo, G.

    2001-06-01

    Using a combination of a zero-dispersion compressor and spectrally compensated sum-frequency generation, we have produced amplitude-modulated femtosecond pulses in the UV at 200 nm. {copyright} 2001 Optical Society of America

  14. Live cell opto-injection by femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Baumgart, J.; Bintig, W.; Ngezahayo, A.; Ertmer, W.; Lubatschowski, H.; Heisterkamp, A.

    2007-02-01

    Fluorescence imaging of cells and cell organelles requires labeling by fluorophores. The labeling of living cells is often done by transfection of fluorescent proteins. Viral vectors are transferring the DNA into the cell. To avoid the use of viruses, it is possible to perforate the cell membrane for example by electro-shocks, the so called electroporation, so that the fluorescent proteins can diffuse into the cell. This method causes cell death in up to 50% of the treated cells because the damage of the outer membrane is too large. A less lethal perforation of the cell membrane with high efficiency can be realized by femtosecond (fs) laser pulses. Transient pores are created by focusing the laser beam for some milliseconds on the membrane. Through this pore, the proteins can enter into the cell. This was demonstrated in a proof of principle experiment for a few cells, but it is essential to develop an opto-perforation system for large numbers of cells in order to obtain statistically significant samples for biological experiments. The relationship between pulse energy, irradiation time, repetition rate and efficacy of the transfer of a chromophor into the cells as well as the viability of the cells was analysed. The cell viability was observed up to 90 minutes after manipulation.

  15. Pulse energy dependence of subcellular dissection by femtosecond laser pulses

    NASA Technical Reports Server (NTRS)

    Heisterkamp, A.; Maxwell, I. Z.; Mazur, E.; Underwood, J. M.; Nickerson, J. A.; Kumar, S.; Ingber, D. E.

    2005-01-01

    Precise dissection of cells with ultrashort laser pulses requires a clear understanding of how the onset and extent of ablation (i.e., the removal of material) depends on pulse energy. We carried out a systematic study of the energy dependence of the plasma-mediated ablation of fluorescently-labeled subcellular structures in the cytoskeleton and nuclei of fixed endothelial cells using femtosecond, near-infrared laser pulses focused through a high-numerical aperture objective lens (1.4 NA). We find that the energy threshold for photobleaching lies between 0.9 and 1.7 nJ. By comparing the changes in fluorescence with the actual material loss determined by electron microscopy, we find that the threshold for true material ablation is about 20% higher than the photobleaching threshold. This information makes it possible to use the fluorescence to determine the onset of true material ablation without resorting to electron microscopy. We confirm the precision of this technique by severing a single microtubule without disrupting the neighboring microtubules, less than 1 micrometer away. c2005 Optical Society of America.

  16. Effect of Metal Coating on NaYF4:Yb3+,Tm 3+ Upconversion Nanoparticles

    NASA Astrophysics Data System (ADS)

    Alazemi, Abdulrahman

    Upconversion is the process in which two or more low-energy photons are absorbed and emitted as one high-energy photon. This research reports on the effect of layer-by-layer polyelectrolytes and silver coating on hexagonal NaYF4:Yb3+,Tm3+ in an attempt to enhance the upconversion intensity. The synthesized upconversion nanoparticles were separated into two, ˜140 nm and a mixture of two populations, ˜250 nm and ˜25 nm. The former case observed enhancement, when silver coated on the upconversion nanoparticles using hydroquinone as the reducing agent, with no layers and with several layers (three, four and five) of polyelectrolytes. The size (140 nm) and morphology of the hexagonal NaYF4:Yb 3+,Tm3+ were similar. The enhancement was confirmed when sodium cyanide was added to remove the silver coating from the sample resulting in a decrease in the upconversion intensity. Quenching was observed in the latter case, when silver coating was unsuccessful and that there are two populations of upconversion nanoparticles (large ˜250 nm and small ˜25 nm).

  17. One-Step Hydrothermal Synthesis of Butanetetracarboxylic Acid-Coated NaYF₄:Yb³⁺, Er³⁺ Upconversion Phosphors with Enhancement Upconversion Luminescence.

    PubMed

    Zhang, Liming; Mao, Lanlan; Lu, Zhuoxuan; Deng, Yan; He, Nongyue

    2016-01-01

    Butanetetracarboxylic acid (BTCA)/NaYF₄:Yb³⁺, Er³⁺ upconversion phosphors have been successfully synthesized by a one-step hydrothermal method. The SEM and XRD results show the as-prepared phosphors exhibit main hexagonal lattice structures and uniform morphologies. FT-IR spectra confirm that the surface of as-prepared phosphors is inherently modified with the carboxyl groups. Under the excitation of 980 nm, it has been observed that BTCA/NaYF₄:Yb³⁺, Er³⁺ upconversion phosphors have a higher upconversion luminescence efficiency than that coated with citrate, ethylenediamine tetraacetic acid (EDTA), or polyacrylic acid (PAA). These results indicate that the BTCA/NaYF₄:Yb³⁺, Er³⁺ phosphors may have superior optical properties, and thus have great potential for biological applications. PMID:27398591

  18. Upconversion white-light emission in Ho3+/Yb3+/Tm3+ tridoped LiNbO3 single crystal.

    PubMed

    Xing, Lili; Wu, Xiaohong; Wang, Rui; Xu, Wei; Qian, Yannan

    2012-09-01

    Ho3+/Yb3+/Tm3+ tridoped LiNbO3 single crystal exhibiting intense upconversion white light under 980 nm excitation has been successfully fabricated by the Czochralski method. The tridoped LiNbO3 single crystal offers power dependent color tuning properties by simply changing excitation power. Efficient three-photon blue upconversion emission and two-photon green and red upconversion emissions have been observed. In addition, the red emission of Ho3+ originates dominantly from the nonradiative decay of green emission. The LiNbO3 with upconversion white light will be a potential laser candidate material. PMID:22940941

  19. Excitation-Selectable Nanoprobe for Tumor Fluorescence Imaging and Near-Infrared Thermal Therapy.

    PubMed

    Wei, Yanchun; Chen, Qun; Wu, Baoyan; Xing, Da

    2016-01-01

    The combination of diagnostics and therapeutics is growing rapidly in cancer treatment. Here, using upconversion nanoparticles coated with chitosan conjugated with a targeting molecule and loaded with indocyanine green (ICG), we develop an excitation-selectable nanoprobe with highly integrated functionalities, including the emission of visible and near-infrared (NIR) light, strong optical absorption in the NIR region and high photostability. After intravenous injection in tumor bearing mice, the nanoprobes target to the tumor vascular system. NIR lasers (980 and 808 nm) are then selectively applied to the mice. The results show that the emitted upconversion fluorescence and NIR fluorescence can be used in a complementary manner for high signal/noise ratio and sensitive tumor imaging for more precise tumor localization. Highly effective photothermal therapy is realized using 808 nm laser irradiation, and the upconversion fluorescence at 654 nm can be used for monitoring treatment effect during the thermal therapy. In summary, using the nanoprobes, outstanding therapeutic efficacy could be realized through flexible excitation control, precise tumor localization, highly effective photothermal conversion and real-time treatment monitoring. The nanofabrication strategy highlights the promise of nanoparticles in cancer theranostics. PMID:27301175

  20. Rhodamine-modified upconversion nanophosphors for ratiometric detection of hypochlorous acid in aqueous solution and living cells.

    PubMed

    Zhou, Yi; Pei, Wenbo; Wang, Chenyuan; Zhu, Jixin; Wu, Jiansheng; Yan, Qinyu; Huang, Ling; Huang, Wei; Yao, Cheng; Loo, Joachim Say Chye; Zhang, Qichun

    2014-09-10

    Hypochlorous acid (HOCl), a reactive oxygen species (ROS) produced by myeloperoxidase (MPO) enzyme-mediated peroxidation of chloride ions, acts as a key microbicidal agent in immune systems. However, misregulated production of HOCl could damage host tissues and cause many inflammation-related diseases. Due to its biological importance, many efforts have been focused on developing fluorescent probes to image HOCl in living system. Compared with those conventional fluorescent probes, up-conversion luminescence (UCL) detection system has been proven to exhibit a lot of advantages including no photo-bleaching, higher light penetration depth, no autofluorescence and less damage to biosamples. Herein, we report a novel water-soluble organic-nano detection system based on rhodamine-modified UCNPs for UCL-sensing HOCl. Upon the interaction with HOCl, the green UCL emission intensity in the detection system were gradually decreased, but the emissions in the NIR region almost have no change, which is very important for the ratiometric UCL detection of HOCl in aqueous solution. More importantly, RBH1-UCNPs could be used for the ratiometric UCL visualization of HOCl released by MPO-mediated peroxidation of chloride ions in living cells. This organic-nano system could be further developed into a novel next-generation imaging technique for bio-imaging HOCl in living system without background noise. PMID:24497481

  1. 2 micron femtosecond fiber laser

    DOEpatents

    Liu, Jian; Wan, Peng; Yang, Lihmei

    2014-07-29

    Methods and systems for generating femtosecond fiber laser pulses are disclose, including generating a signal laser pulse from a seed laser oscillator; using a first amplifier stage comprising an input and an output, wherein the signal laser pulse is coupled into the input of the first stage amplifier and the output of the first amplifier stage emits an amplified and stretched signal laser pulse; using an amplifier chain comprising an input and an output, wherein the amplified and stretched signal laser pulse from the output of the first amplifier stage is coupled into the input of the amplifier chain and the output of the amplifier chain emits a further amplified, stretched signal laser pulse. Other embodiments are described and claimed.

  2. High energy femtosecond pulse compression

    NASA Astrophysics Data System (ADS)

    Lassonde, Philippe; Mironov, Sergey; Fourmaux, Sylvain; Payeur, Stéphane; Khazanov, Efim; Sergeev, Alexander; Kieffer, Jean-Claude; Mourou, Gerard

    2016-07-01

    An original method for retrieving the Kerr nonlinear index was proposed and implemented for TF12 heavy flint glass. Then, a defocusing lens made of this highly nonlinear glass was used to generate an almost constant spectral broadening across a Gaussian beam profile. The lens was designed with spherical curvatures chosen in order to match the laser beam profile, such that the product of the thickness with intensity is constant. This solid-state optics in combination with chirped mirrors was used to decrease the pulse duration at the output of a terawatt-class femtosecond laser. We demonstrated compression of a 33 fs pulse to 16 fs with 170 mJ energy.

  3. Photoemission using femtosecond laser pulses

    SciTech Connect

    Srinivasan-Rao, T.; Tsang, T.; Fischer, J.

    1991-10-01

    Successful operation of short wavelength FEL requires an electron bunch of current >100 A and normalized emittance < 1 mm-mrad. Recent experiments show that RF guns with photocathodes as the electron source may be the ideal candidate for achieving these parameters. To reduce the emittance growth due to space charge and RF dynamics effects, the gun may have to operate at high field gradient (hence at high RF frequency) and a spot size small compared to the aperture. This may necessitate the laser pulse duration to be in the subpicosecond regime to reduce the energy spread. We will present the behavior of metal photocathodes upon irradiation with femtosecond laser beams, comparison of linear and nonlinear photoemission, and scalability to high currents. Theoretical estimate of the intrinsic emittance at the photocathode in the presence of the anomalous heating of the electrons, and the tolerance on the surface roughness of the cathode material will be discussed.

  4. Plasmon-Enhanced Light Harvesting of Chlorophylls on Near-Percolating Silver Films via One-Photon Anti-Stokes Upconversion

    PubMed Central

    Wang, Ya-Lan; Nan, Fan; Liu, Xiao-Li; Zhou, Li; Peng, Xiao-Niu; Zhou, Zhang-Kai; Yu, Ying; Hao, Zhong-Hua; Wu, Yan; Zhang, Wei; Wang, Qu-Quan; Zhang, Zhenyu

    2013-01-01

    There exists a wealth of means of efficient utilization of solar energy in nature, with photosynthesis of chlorophylls as a prime example. Separately, artificially structured plasmonic materials are versatile in light harvesting and energy conversion. Using a simple and scalable design of near-percolating silver nanostructures, we demonstrate that the light-harvesting efficiency of chlorophylls can be drastically enhanced by tuning the plasmon frequency of the constituent silver nanoparticles to coincide with the maximal photon flux of sunlight. In particular, we show that the photon upconversion efficiency can be readily enhanced by over 20 folds, with the room-temperature fluorescence quantum yield increased by a factor of 2.63. The underlying mechanism for the upconversion enhancement is attributed to a one-electron-per-photon anti-Stokes process, involving absorption of a characteristic phonon mode of the chlorophylls. These findings suggest that chlorophylls can serve as molecular building blocks for high-efficiency light harvesting and solar energy conversion. PMID:23689426

  5. Incorporation of Zn(2+) ions into BaTiO3:Er(3+)/Yb(3+) nanophosphor: an effective way to enhance upconversion, defect luminescence and temperature sensing.

    PubMed

    Mahata, Manoj Kumar; Koppe, Tristan; Mondal, Tanusree; Brüsewitz, Christoph; Kumar, Kaushal; Kumar Rai, Vineet; Hofsäss, Hans; Vetter, Ulrich

    2015-08-28

    Ferroelectric BaTiO3 became a multifunctional material via doping of lanthanide ions (0.3 mol% Er(3+)/3.0 mol% Yb(3+)) and subsequently upconversion luminescence was enhanced by incorporation of Zn(2+) ions. Upconversion luminescence of BaTiO3:Er(3+)/Yb(3+) perovskite nanophosphor has been studied using 800 and 980 nm laser excitations. The emission dynamics is studied with respect to its dependence on input power and external temperature including lifetime. Based on time-resolved spectroscopy, it is inferred that two types of Er(3+) sites are present in the barium titanate lattice. The first one is a short lived component (minor species) present at 6-coordinated Ti-sites of low symmetry while the second one is a long lived component (major species), present at 12-coordinated Ba-sites with high symmetry. The influence of the introduction of Zn(2+) ions on the lifetime of (4)S3/2 and (4)F9/2 levels of Er(3+) ions is also investigated. Enhanced temperature sensing performance (120 K to 505 K) of the material is observed using the fluorescence intensity ratio technique, employing the emission from the thermally coupled, (2)H11/2 and (4)S3/2 energy levels of Er(3+) ions. The defect luminescence of the material is also found to increase upon Zn-doping. PMID:26206553

  6. Quantum frequency up-conversion of continuous variable entangled states

    SciTech Connect

    Liu, Wenyuan; Wang, Ning; Li, Zongyang; Li, Yongmin

    2015-12-07

    We demonstrate experimentally quantum frequency up-conversion of a continuous variable entangled optical field via sum-frequency-generation process. The two-color entangled state initially entangled at 806 and 1518 nm with an amplitude quadrature difference squeezing of 3.2 dB and phase quadrature sum squeezing of 3.1 dB is converted to a new entangled state at 530 and 1518 nm with the amplitude quadrature difference squeezing of 1.7 dB and phase quadrature sum squeezing of 1.8 dB. Our implementation enables the observation of entanglement between two light fields spanning approximately 1.5 octaves in optical frequency. The presented scheme is robust to the excess amplitude and phase noises of the pump field, making it a practical building block for quantum information processing and communication networks.

  7. Photon avalanche up-conversion in holmium doped fluoride glasses

    SciTech Connect

    Chen, Y.H.; Liu, G.K.; Beitz, J.V.; Jie Wang

    1996-08-01

    Photon avalanche green up-conversion emission centered at 545 nm has been observed in Ho{sup 3+} doped and Ho{sup 3+}, Tm{sup 3+} co-doped ZrF{sub 4}-based fluoride glasses when excited near 585 nm which is off resonance with any ground state absorption bands of either Ho{sup 3+} or Tm{sup 3+} ions. Detailed spectral measurements and analysis suggest that the 545 nm emission occurs from the {sup 5}S{sub 2},{sup 5}F{sub 4} states of Ho{sup 3+} that are populated by excited state absorption from the {sup 5}I{sub 7} state of Ho{sup 3+}. Strong cross-relaxation that efficiently populates the {sup 5}I{sub 7} state makes the photon avalanche process possible in this system.

  8. Multimodal cancer imaging using lanthanide-based upconversion nanoparticles.

    PubMed

    Yang, Dongmei; Li, Chunxia; Lin, Jun

    2015-01-01

    Multimodal nanoprobes that integrate different imaging modalities in one nano-system could offer synergistic effect over any modality alone to satisfy the higher requirements on the efficiency and accuracy for clinical diagnosis and medical research. Upconversion nanoparticles (UCNPs), particularly lanthanide (Ln)-based NPs have been regarded as an ideal building block for constructing multimodal bioprobes due to their fascinating properties. In this review, we first summarize recent advances in the optimizations of existing UCNPs. In particular, we highlight the applications of Ln-based UCNPs for multimodal cancer imaging in vitro and in vivo. The explorations of UCNPs-based multimodal nanoprobes for targeting diagnosis and imaging-guided therapeutics are also presented. Finally, the challenges and perspectives of Ln-based UCNPs in this rapid growing field are discussed. PMID:26293416

  9. Synchronous detection in monolithically integrated AM upconversion receivers

    NASA Astrophysics Data System (ADS)

    Vanderplas, Jacob

    1990-01-01

    The design of a synchronous detector for an integrated AM (Amplitude Modulated) upconversion receiver with a tuning range from 150 kHz to 30 MHz is addressed. The following are described: synchronous detector architecture; design of the synchronous detector HF circuits; design of the on-chip continuous time audio low pass filter; and design of the synchronous detector LF circuits. The results of the calculations combined with the results of the prototypes confirm the technical feasibility of a synchronous detector that guarantees at least 50 dB additional channel selectivity. However, the relatively large amount of overhead circuitry for the regeneration of the carrier makes the economic feasibility for the consumer market doubtful.

  10. Quantum frequency up-conversion of continuous variable entangled states

    NASA Astrophysics Data System (ADS)

    Liu, Wenyuan; Wang, Ning; Li, Zongyang; Li, Yongmin

    2015-12-01

    We demonstrate experimentally quantum frequency up-conversion of a continuous variable entangled optical field via sum-frequency-generation process. The two-color entangled state initially entangled at 806 and 1518 nm with an amplitude quadrature difference squeezing of 3.2 dB and phase quadrature sum squeezing of 3.1 dB is converted to a new entangled state at 530 and 1518 nm with the amplitude quadrature difference squeezing of 1.7 dB and phase quadrature sum squeezing of 1.8 dB. Our implementation enables the observation of entanglement between two light fields spanning approximately 1.5 octaves in optical frequency. The presented scheme is robust to the excess amplitude and phase noises of the pump field, making it a practical building block for quantum information processing and communication networks.

  11. Enhancement of upconversion deep-tissue imaging using optical clearing

    NASA Astrophysics Data System (ADS)

    Popov, A. P.; Khaydukov, E. V.; Bykov, A. V.; Semchishen, V. A.; Tuchin, V. V.

    2015-07-01

    We report on the deep-tissue imaging using novel upconversion nanoparticles (UCNPs) β-NaYF4:Yb3+ ,Tm3+ (excitation wavelength: 975 nm, detection wavelength: 800 nm) and glycerol as an optical clearing agent to enhance imaging from under 6-mm-thick porcine muscle tissue samples. We show that improvement of luminescent label visualization is caused by transforming of the diffuse label-emitted light into the direct component. This results in the increase in visibility (ratio of the sum and difference of the maximal and minimal intensity) of the label and increase in maximal signal intensity thus making the combination of the phosphors and optical clearing promising for precise detection of tissue-embedded labelled inhomogeneities.

  12. Elimination of photon quenching by a transition layer to fabricate a quenching-shield sandwich structure for 800 nm excited upconversion luminescence of Nd3+-sensitized nanoparticles.

    PubMed

    Zhong, Yeteng; Tian, Gan; Gu, Zhanjun; Yang, Yijun; Gu, Lin; Zhao, Yuliang; Ma, Ying; Yao, Jiannian

    2014-05-01

    Nd3+-sensitized quenching-shield sandwich-structured upconversion nanoparticles are reported, which exhibit highly efficient upconversion photoluminescence under excitation by an 800 nm continuous-wave laser. The transition-layer structure is essential to bridge energy transfer from the sensitizer to the activator and simultaneously block energy back-transfer from the activator to the sensitizer. These 800 nm-excited upconversion nanoparticles are a key step toward the development of upconversion nanophosphors for biological applications. PMID:24338994

  13. Cyclometallated ruthenium complex-modified upconversion nanophosphors for selective detection of Hg2+ ions in water

    NASA Astrophysics Data System (ADS)

    Li, Xianghong; Wu, Yongquan; Liu, Yi; Zou, Xianmei; Yao, Liming; Li, Fuyou; Feng, Wei

    2013-12-01

    Upconversion detection nanocomposites were assembled for the selective luminescent detection of mercury ions in water. A hydrophobic cyclometallated ruthenium complex [RuII(bpy)2(thpy)]PF6 (abbreviated as Ru1; bpy = 2,2'-bipyridine and thpy = 2-(2-thienyl)pyridine) is employed as a chemodosimeter to assemble on amphiphilic polymer-coating upconversion nanophosphors (UCNPs) based on the hydrophobic-hydrophobic interaction. Upon addition of Hg2+, the nanocomposite not only exhibits a remarkable color change from deep-red to yellow, but also an enhanced upconversion luminescence (UCL) emission by hindering the luminescent resonance energy transfer (LRET) process from the upconversion emission of UCNPs to Ru1. Using the ratiometric UCL emission as a detection signal, the detection limit of Hg2+ for this nanoprobe in aqueous solution is 8.2 ppb, which is much lower than that (329 ppb) determined by UV/Vis technology. Such an Hg2+-tunable LRET process provides a general strategy for fabricating a water-soluble upconversion-based nanoprobe for some special analyte.Upconversion detection nanocomposites were assembled for the selective luminescent detection of mercury ions in water. A hydrophobic cyclometallated ruthenium complex [RuII(bpy)2(thpy)]PF6 (abbreviated as Ru1; bpy = 2,2'-bipyridine and thpy = 2-(2-thienyl)pyridine) is employed as a chemodosimeter to assemble on amphiphilic polymer-coating upconversion nanophosphors (UCNPs) based on the hydrophobic-hydrophobic interaction. Upon addition of Hg2+, the nanocomposite not only exhibits a remarkable color change from deep-red to yellow, but also an enhanced upconversion luminescence (UCL) emission by hindering the luminescent resonance energy transfer (LRET) process from the upconversion emission of UCNPs to Ru1. Using the ratiometric UCL emission as a detection signal, the detection limit of Hg2+ for this nanoprobe in aqueous solution is 8.2 ppb, which is much lower than that (329 ppb) determined by UV/Vis technology

  14. Wavelength dependence of femtosecond laser-induced breakdown in water and implications for laser surgery

    NASA Astrophysics Data System (ADS)

    Linz, Norbert; Freidank, Sebastian; Liang, Xiao-Xuan; Vogel, Alfred

    2016-07-01

    The wavelength dependence of the threshold for femtosecond optical breakdown in water provides information on the interplay of multiphoton, tunneling, and avalanche ionization and is of interest for parameter selection in laser surgery. We measured the bubble threshold from ultraviolet to near-infrared wavelengths and found a continuous decrease of the irradiance threshold with increasing wavelength λ . Results are compared to the predictions of a numerical model that assumes a band gap of 9.5 eV and considers the existence of a separate initiation channel via excitation of valence band electrons into a solvated state followed by rapid upconversion into the conduction band. Fits to experimental data yield an electron collision time of ≈1 fs and an estimate for the capacity of the initiation channel. Using that collision time, the breakdown dynamics were explored up to λ = 2 μ m . The irradiance threshold first continues to decrease but levels out for wavelengths longer than 1.3 μ m . This opens promising perspectives for laser surgery at wavelengths around 1.3 and 1.7 μ m , which are attractive because of their large penetration depth into scattering tissues.

  15. Femtosecond solvation dynamics in a neat ionic liquid and ionic liquid microemulsion: excitation wavelength dependence.

    PubMed

    Adhikari, Aniruddha; Sahu, Kalyanasis; Dey, Shantanu; Ghosh, Subhadip; Mandal, Ujjwal; Bhattacharyya, Kankan

    2007-11-01

    Solvation dynamics in a neat ionic liquid, 1-pentyl-3-methyl-imidazolium tetra-flouroborate ([pmim][BF4]) and its microemulsion in Triton X-100 (TX-100)/benzene is studied using femtosecond up-conversion. In both the neat ionic liquid and the microemulsion, the solvation dynamics is found to depend on excitation wavelength (lambda(ex)). The lambda(ex) dependence is attributed to structural heterogeneity in neat ionic liquid (IL) and in IL microemulsion. In neat IL, the heterogeneity arises from clustering of the pentyl groups which are surrounded by a network of cation and anions. Such a nanostructural organization is predicted in many recent simulations and observed recently in an X-ray diffraction study. In an IL microemulsion, the surfactant (TX-100) molecules aggregate in form of a nonpolar peripheral shell around the polar pool of IL. The micro-environment in such an assembly varies drastically over a short distance. The dynamic solvent shift (and average solvation time) in neat IL as well as in IL microemulsions decreases markedly as lambda(ex) increases from 375 to 435 nm. In a [pmim][BF4]/water/TX-100/benzene quaternary microemulsion, the solvation dynamics is slower than that in a microemulsion without water. This is ascribed to the smaller size of the water containing microemulsion. The anisotropy decay in an IL microemulsion is found to be faster than that in neat IL. PMID:17944511

  16. Upconversion nanoparticles with a strong acid-resistant capping

    NASA Astrophysics Data System (ADS)

    Recalde, Ileana; Estebanez, Nestor; Francés-Soriano, Laura; Liras, Marta; González-Béjar, María; Pérez-Prieto, Julia

    2016-03-01

    Water-dispersible upconversion nanoparticles (β-NaYF4:Yb3+,Er3+, UCNP) coated with a thin shell of a biocompatible copolymer comprising 2-hydroxyethylmethacrylate (HEMA) and 2-acrylamido-2-methyl-1-propanesulphonsulphonic acid (AMPS), which we will term COP, have been prepared by multidentate grafting. This capping is remarkably resistant to strong acidic conditions as low as pH 2. The additional functionality of the smart UCNP@COP nanosystem has been proved by its association to a well-known photosensitizer (namely, methylene blue, MB). The green-to-red emission ratio of the UC@COP@MB nanohybrid exhibits excellent linear dependence in the 7 to 2 pH range as a consequence of the release of the dye as the pH decreases.Water-dispersible upconversion nanoparticles (β-NaYF4:Yb3+,Er3+, UCNP) coated with a thin shell of a biocompatible copolymer comprising 2-hydroxyethylmethacrylate (HEMA) and 2-acrylamido-2-methyl-1-propanesulphonsulphonic acid (AMPS), which we will term COP, have been prepared by multidentate grafting. This capping is remarkably resistant to strong acidic conditions as low as pH 2. The additional functionality of the smart UCNP@COP nanosystem has been proved by its association to a well-known photosensitizer (namely, methylene blue, MB). The green-to-red emission ratio of the UC@COP@MB nanohybrid exhibits excellent linear dependence in the 7 to 2 pH range as a consequence of the release of the dye as the pH decreases. Electronic supplementary information (ESI) available: Additional spectra and data of HEMA, AMPS, COP, UCNP@oleate, UCNP@COP, and UCNP@COP@MB. See DOI: 10.1039/c5nr06653k

  17. Effects of Upconversion Nanoparticles on Polymerase Chain Reaction

    PubMed Central

    Hwang, Sang-Hyun; Im, Su-Gyeong; Hah, Sang Soo; Cong, Vu Thanh; Lee, Eun Jeong; Lee, Yeon-Su; Lee, Geon Kook

    2013-01-01

    Nanoparticles (NPs) are attractive materials owing to their physical and electrochemical properties, which make them extremely useful in diagnostic applications. Photon upconversion is the phenomenon where high-energy photons are emitted upon excitation of low-energy photons. Nucleic acids detection based on upconversion nanoparticles (UCNPs), which display a high signal-to-noise ratio and no photobleaching, has been widely applied. We evaluated whether UCNPs can improve polymerase chain reaction (PCR) specificity and affect PCR amplification. The effects of UCNPs with a diameter size of 40, 70, and 250 nm were evaluated using 3 PCR kits (AccuPower PCR PreMix, AmpliTaq Gold 360 Master Mix, and HotStarTaq Plus Master Mix) and 3 real-time PCR kits (AccuPower GreenStar qPCR PreMix, SYBR Green PCR Master Mix, and QuantiTect SYBR Green PCR Kit). Quantum dots were used for comparison with the UCNPs. In the presence of an appropriate concentration of UCNPs, PCR specificity was optimized. UCNPs of 40-nm size improved PCR specificity more effectively than did UCNPs sized 70 or 250 nm. As the size and concentrations of the UCNPs were increased, PCR amplification was more severely inhibited. At lower annealing temperatures (25°C–45°C), addition of the 40 nm UCNP (1 µg/µL) to the PCR reagent produced specific PCR products without nonspecific sequence amplification. Therefore, UCNPs of different sizes, with different DNA polymerases used in the commercial kits, showed different inhibitory effects on PCR amplification. These results demonstrate that optimization of UCNPs, added to reaction mixtures at appropriate concentrations, can improve PCR specificity. However, the mechanism underlining UCNPs effect on PCR remains unclear and will require further investigation. PMID:24039935

  18. Femtosecond Broadband Stimulated Raman: A New Approach for High-Performance Vibrational Spectroscopy

    PubMed Central

    McCAMANT, DAVID W.; KUKURA, PHILIPP; MATHIES, RICHARD A.

    2005-01-01

    Femtosecond stimulated Raman spectroscopy (FSRS) is a new technique that produces high-quality vibrational spectra free from background fluorescence. FSRS combines a narrow-bandwidth picosecond Raman pump pulse with an ∼80 fs continuum probe pulse to produce stimulated Raman spectra from the pump-induced gain in the probe spectrum. The high intensity of the Raman pump combined with the broad bandwidth of the probe produces high signal-to-noise vibrational spectra with very short data acquisition times. FSRS spectra of standard solutions and solvents such as aqueous Na2SO4, aqueous KNO3, methanol, isopropanol, and cyclohexane are collected in seconds. Furthermore, stimulated Raman spectra can be obtained using just a single pump–probe pulse pair that illuminates the sample for only ∼1 ps. Fluorescence rejection is demonstrated by collecting FSRS spectra of dyes (rhodamine 6G, chlorophyll a, and DTTCI) with varying degrees of fluorescence background and resonance enhancement. The high signal-to-noise, short data acquisition time, fluorescence rejection, and high spectral and temporal resolution of femtosecond stimulated Raman spectroscopy make it a valuable new vibrational spectroscopic technique. PMID:14658143

  19. Optical imaging-guided cancer therapy with fluorescent nanoparticles

    PubMed Central

    Jiang, Shan; Gnanasammandhan, Muthu Kumara; Zhang, Yong

    2010-01-01

    The diagnosis and treatment of cancer have been greatly improved with the recent developments in nanotechnology. One of the promising nanoscale tools for cancer diagnosis is fluorescent nanoparticles (NPs), such as organic dye-doped NPs, quantum dots and upconversion NPs that enable highly sensitive optical imaging of cancer at cellular and animal level. Furthermore, the emerging development of novel multi-functional NPs, which can be conjugated with several functional molecules simultaneously including targeting moieties, therapeutic agents and imaging probes, provides new potentials for clinical therapies and diagnostics and undoubtedly will play a critical role in cancer therapy. In this article, we review the types and characteristics of fluorescent NPs, in vitro and in vivo imaging of cancer using fluorescent NPs and multi-functional NPs for imaging-guided cancer therapy. PMID:19759055

  20. Multi-functionality of fluorescent nanocrystals in glass ceramics

    PubMed Central

    Schweizer, S.; Henke, B.; Miclea, P.T.; Ahrens, B.; Johnson, J.A.

    2012-01-01

    Thermal processing of as-made fluorozirconate glasses, which were additionally doped with rare-earth and chlorine ions, results in the formation of fluorescent nanocrystals therein. For medical applications, the glasses were doped with divalent europium ions as the fluorescent rare-earth ion, while trivalent neodymium was used to develop up-conversion systems. The samples were annealed up to 290 °C to initiate the growth of hexagonal or orthorhombic phase BaCl2 nanocrystals therein. Upon annealing some of the rare-earth ions were incorporated into the BaCl2 nanocrystals leading to enhanced fluorescence properties. The particle diameters were in the range of a few nanometers to several tens of nanometers. PMID:23637567

  1. Optimizing single-nanoparticle two-photon microscopy by in situ adaptive control of femtosecond pulses

    NASA Astrophysics Data System (ADS)

    Li, Donghai; Deng, Yongkai; Chu, Saisai; Jiang, Hongbing; Wang, Shufeng; Gong, Qihuang

    2016-07-01

    Single-nanoparticle two-photon microscopy shows great application potential in super-resolution cell imaging. Here, we report in situ adaptive optimization of single-nanoparticle two-photon luminescence signals by phase and polarization modulations of broadband laser pulses. For polarization-independent quantum dots, phase-only optimization was carried out to compensate the phase dispersion at the focus of the objective. Enhancement of the two-photon excitation fluorescence intensity under dispersion-compensated femtosecond pulses was achieved. For polarization-dependent single gold nanorod, in situ polarization optimization resulted in further enhancement of two-photon photoluminescence intensity than phase-only optimization. The application of in situ adaptive control of femtosecond pulse provides a way for object-oriented optimization of single-nanoparticle two-photon microscopy for its future applications.

  2. Femtosecond optical transfection as a tool for genetic manipulation of human embryonic stem cells

    NASA Astrophysics Data System (ADS)

    Torres-Mapa, M. L.; Gardner, J.; Bradburn, H.; King, J.; Dholakia, K.; Gunn-Moore, F.

    2013-03-01

    We demonstrate the use of femtosecond optical transfection for the genetic manipulation of human embryonic stem cells. Using a system with an SLM combined with a scanning mirror allows poration of both single-cell and colony-formed human embryonic stem cells in a rapid and targeted manner. In this work, we show successful transfection of plasmid DNA tagged with fluorescent reporters into human embryonic stem cells using three doses of focused femtosecond laser. A significant number of transfected cells retained their undifferentiated morphological feature of large nucleus with high nucleus to cytoplasmic ratio, 48h after photoporation. Furthermore, DNA constructs driven by different types of promoters were also successfully transfected into human embryonic stem cells using this technique.

  3. Optical investigation of femtosecond laser induced microstress in neodymium doped lithium niobate crystals

    NASA Astrophysics Data System (ADS)

    Ródenas, A.; Sanz García, J. A.; Jaque, D.; Torchia, G. A.; Mendez, C.; Arias, I.; Roso, L.; Agulló-Rueda, F.

    2006-08-01

    The depth-resolved micromodification of single-crystalline femtosecond laser irradiated Nd3+ doped MgO:LiNbO3 crystals is investigated by means of micro-Raman and microluminescence experiments. We have found that a permanent tensile stress of the order of 2GPa is induced in the vicinity of ablated volume as a consequence of the pressure-wave propagation due to the thermoelastic relaxation of the laser irradiated material. Microluminescence experiments have revealed that, as a consequence of the permanent laser induced microstress, a localized redshift of the F3/24→I9/24 luminescence band of Nd3+ ions also takes place due to a crystal field modification. The analysis of Raman and fluorescence bandwidths indicates that a slight lattice disorder and densification is induced by femtosecond laser irradiation.

  4. Optical investigation of femtosecond laser induced microstress in neodymium doped lithium niobate crystals

    SciTech Connect

    Rodenas, A.; Sanz Garcia, J. A.; Jaque, D.; Torchia, G. A.; Mendez, C.; Arias, I.; Roso, L.; Agullo-Rueda, F.

    2006-08-01

    The depth-resolved micromodification of single-crystalline femtosecond laser irradiated Nd{sup 3+} doped MgO:LiNbO{sub 3} crystals is investigated by means of micro-Raman and microluminescence experiments. We have found that a permanent tensile stress of the order of 2 GPa is induced in the vicinity of ablated volume as a consequence of the pressure-wave propagation due to the thermoelastic relaxation of the laser irradiated material. Microluminescence experiments have revealed that, as a consequence of the permanent laser induced microstress, a localized redshift of the {sup 4}F{sub 3/2}{yields}{sup 4}I{sub 9/2} luminescence band of Nd{sup 3+} ions also takes place due to a crystal field modification. The analysis of Raman and fluorescence bandwidths indicates that a slight lattice disorder and densification is induced by femtosecond laser irradiation.

  5. Femtosecond Laser Microfabrication of an Integrated Device for Optical Release and Sensing of Bioactive Compounds

    PubMed Central

    Ghezzi, Diego; Vazquez, Rebeca Martinez; Osellame, Roberto; Valtorta, Flavia; Pedrocchi, Alessandra; Valle, Giuseppe Della; Ramponi, Roberta; Ferrigno, Giancarlo; Cerullo, Giulio

    2008-01-01

    Flash photolysis of caged compounds is one of the most powerful approaches to investigate the dynamic response of living cells. Monolithically integrated devices suitable for optical uncaging are in great demand since they greatly simplify the experiments and allow their automation. Here we demonstrate the fabrication of an integrated bio-photonic device for the optical release of caged compounds. Such a device is fabricated using femtosecond laser micromachining of a glass substrate. More in detail, femtosecond lasers are used both to cut the substrate in order to create a pit for cell growth and to inscribe optical waveguides for spatially selective uncaging of the compounds present in the culture medium. The operation of this monolithic bio-photonic device is tested using both free and caged fluorescent compounds to probe its capability of multipoint release and optical sensing. Application of this device to the study of neuronal network activity can be envisaged.

  6. Targeted transfection of stem cells with sub-20 femtosecond laser pulses.

    PubMed

    Uchugonova, Aisada; König, Karsten; Bueckle, Rainer; Isemann, Andreas; Tempea, Gabriel

    2008-06-23

    Multiphoton microscopes have become important tools for non-contact sub-wavelength three-dimensional nanoprocessing of living biological specimens based on multiphoton ionization and plasma formation. Ultrashort laser pulses are required, however, dispersive effects limit the shortest pulse duration achievable at the focal plane. We report on a compact nonlinear laser scanning microscope with sub-20 femtosecond 75 MHz near infrared laser pulses for nanosurgery of human stem cells and two-photon high-resolution imaging. Single point illumination of the cell membrane was performed to induce a transient nanopore for the delivery of extracellular green fluorescent protein plasmids. Mean powers of less than 7 mW (<93 pJ) and low millisecond exposure times were found to be sufficient to transfect human pancreatic and salivary gland stem cells in these preliminary studies. Ultracompact sub-20 femtosecond laser microscopes may become optical tools for nanobiotechnology and nanomedicine including optical stem cell manipulation. PMID:18575499

  7. Femtosecond laser structuring in dielectrics

    NASA Astrophysics Data System (ADS)

    Juodkazis, Saulius

    2008-03-01

    Three-dimensional (3D) structuring of glasses, crystals, and polymers by tightly focused femtosecond laser pulses is a promising technique for microfluidic, micro-optical, photonic crystal and micro-mechanical applications [1-4]. The 3D laser micro-structuring of resists is demonstrated by direct laser writing [1] and holographic recording using phase control of interfering pulses [2]. Tightly focused laser pulses can reach dielectric breakdown irradiance without self-focusing when sub-1 ps pulses are used for laser-structuring inside dielectrics. The limiting case of microstructuring, a void recording, can be achieved [3]. The mechanism of void formation has been explained as a result of dielectric breakdown and micro-explosion. The absorption is localized within a skin depth of tens-of-nanometers in the plasma at the focus. This defines an ultimate localization of the energy delivery by a laser pulse. The absorbance reaches 0.6 in a fully ionized solid state density breakdown plasma. The high temperature and pressure buildup is large enough to generate a shock wave (strong micro-explosion). For example, a single 100 nJ laser pulse forms a void under tight focusing conditions even in the high strength sapphire (Young modulus of 400 GPa). It is considered that material fails upon compression rather than tension for which the mechanical failure threshold is by an order of magnitude smaller. This scenario of breakdown by compression is corroborated by numerical modeling of the strong explosion at our experimental conditions. Modification of materials by tightly focused femtosecond pulses opens new material processing routes for inert dielectrics [4] and can possibly be used for creation of new high-temperature and pressure phases inside the volume of irradiated samples. These regions with altered nano-structure have different chemical properties as was found in silica glass, quartz, and sapphire by wet etching of the ``shocked'' regions in aqueous solution of

  8. Two-photon excited quantum dots with compact surface coatings of polymer ligands used as an upconversion luminescent probe for dopamine detection in biological fluids.

    PubMed

    Jin, Hui; Gui, Rijun; Wang, Zonghua; Zhang, Feifei; Xia, Jianfei; Yang, Min; Bi, Sai; Xia, Yanzhi

    2015-03-21

    Water-soluble multidentate polymer coated CdTe quantum dots (QDs) were prepared via a stepwise addition of raw materials in a one-pot aqueous solution under ambient conditions. Just by adjusting the compositions of raw materials, different sized CdTe QDs were achieved within a short time. The as-prepared QDs showed compact surface coating (1.6-1.8 nm) of polymer ligands and photoluminescence (PL) emitted at 533-567 nm, as well as high colloidal/photo-stability and quantum yields (58-67%). Moreover, these QDs exhibited significant upconversion luminescence (UCL) upon excitation using an 800 nm femtosecond laser. Experimental results confirm that the UCL was ascribed to the two-photon assisted process via a virtual energy state. Then, the two-photon excited QDs were further developed as a novel UCL probe of dopamine (DA) due to self-assembled binding of DA molecules with QDs via non-covalent bonding. As a receptor, the DA attached onto the QD surface induced an electron transfer from QDs to DA, triggering UCL quenching of QDs. This UCL probe of DA presented a low limit of detection (ca. 5.4 nM), and high selectivity and sensitivity in the presence of potential interferences. In particular, it was favorably applied to the detection of DA in biological fluids, with quantitative recoveries (96.0-102.6%). PMID:25684191

  9. Er{sup 3+}/Yb{sup 3+}co-doped bismuth molybdate nanosheets upconversion photocatalyst with enhanced photocatalytic activity

    SciTech Connect

    Adhikari, Rajesh; Gyawali, Gobinda; Cho, Sung Hun; Narro-García, R.; Sekino, Tohru; Lee, Soo Wohn

    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+} and 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.

  10. 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

  11. Femtosecond lasers for microsurgery of cornea

    NASA Astrophysics Data System (ADS)

    Vartapetov, Sergei K.; Khudyakov, D. V.; Lapshin, Konstantin E.; Obidin, Aleksei Z.; Shcherbakov, Ivan A.

    2012-03-01

    The review of femtosecond laser installations for medical applications is given and a new femtosecond ophthalmologic system for creation of a flap of corneal tissue during the LASIK operation is described. An all-fibre femtosecond laser emitting ~400-fs pulses at 1067 nm is used. The pulse repetition rate can vary from 200 kHz up to 1 MHz. The output energy of the femtosecond system does not exceed 1 μJ. A specially developed objective with small spherical and chromatic aberrations is applied to focus laser radiation to an area of an eye cornea. The size of the focusing spot does not exceed 3 μm. To process the required area, scanning by a laser beam is applied with a speed no less than 5 m s-1. At a stage of preliminary tests of the system, the Κ8 glass, organic PMMA glass and specially prepared agarose gels are used as a phantom of an eye. The femtosecond system is successfully clinically tested on a plenty of eyes of a pig and on several human eyes. The duration of the procedure of creation of a corneal flap does not exceed 20 s.

  12. Femtosecond lasers for microsurgery of cornea

    SciTech Connect

    Vartapetov, Sergei K; Khudyakov, D V; Lapshin, Konstantin E; Obidin, Aleksei Z; Shcherbakov, Ivan A

    2012-03-31

    The review of femtosecond laser installations for medical applications is given and a new femtosecond ophthalmologic system for creation of a flap of corneal tissue during the LASIK operation is described. An all-fibre femtosecond laser emitting {approx}400-fs pulses at 1067 nm is used. The pulse repetition rate can vary from 200 kHz up to 1 MHz. The output energy of the femtosecond system does not exceed 1 {mu}J. A specially developed objective with small spherical and chromatic aberrations is applied to focus laser radiation to an area of an eye cornea. The size of the focusing spot does not exceed 3 {mu}m. To process the required area, scanning by a laser beam is applied with a speed no less than 5 m s{sup -1}. At a stage of preliminary tests of the system, the {Kappa}8 glass, organic PMMA glass and specially prepared agarose gels are used as a phantom of an eye. The femtosecond system is successfully clinically tested on a plenty of eyes of a pig and on several human eyes. The duration of the procedure of creation of a corneal flap does not exceed 20 s.

  13. Recent Progress on Plasmon-Enhanced Fluorescence

    NASA Astrophysics Data System (ADS)

    Dong, Jun; Zhang, Zhenglong; Zheng, Hairong; Sun, Mentao

    2015-12-01

    The optically generated collective electron density waves on metal-dielectric boundaries known as surface plasmons have been of great scientific interest since their discovery. Being electromagnetic waves on gold or silver nanoparticle's surface, localised surface plasmons (LSP) can strongly enhance the electromagnetic field. These strong electromagnetic fields near the metal surfaces have been used in various applications like surface enhanced spectroscopy (SES), plasmonic lithography, plasmonic trapping of particles, and plasmonic catalysis. Resonant coupling of LSPs to fluorophore can strongly enhance the emission intensity, the angular distribution, and the polarisation of the emitted radiation and even the speed of radiative decay, which is so-called plasmon enhanced fluorescence (PEF). As a result, more and more reports on surface-enhanced fluorescence have appeared, such as SPASER-s, plasmon assisted lasing, single molecule fluorescence measurements, surface plasmoncoupled emission (SPCE) in biological sensing, optical orbit designs etc. In this review, we focus on recent advanced reports on plasmon-enhanced fluorescence (PEF). First, the mechanism of PEF and early results of enhanced fluorescence observed by metal nanostructure will be introduced. Then, the enhanced substrates, including periodical and nonperiodical nanostructure, will be discussed and the most important factor of the spacer between molecule and surface and wavelength dependence on PEF is demonstrated. Finally, the recent progress of tipenhanced fluorescence and PEF from the rare-earth doped up-conversion (UC) and down-conversion (DC) nanoparticles (NPs) are also commented upon. This review provides an introduction to fundamentals of PEF, illustrates the current progress in the design of metallic nanostructures for efficient fluorescence signal amplification that utilises propagating and localised surface plasmons.

  14. Drug delivery function of carboxymethyl-β-cyclodextrin modified upconversion nanoparticles for adamantine phthalocyanine and their NIR-triggered cancer treatment.

    PubMed

    Wang, Ao; Jin, Weiwei; Chen, Enyi; Zhou, Jiahong; Zhou, Lin; Wei, Shaohua

    2016-03-01

    Near-infrared (NIR) light triggered photodynamic therapy (PDT), based on upconversion nanoparticles (UCNPs), has attracted great attention because of its high tissue penetration and low photodamage to living organisms. However, most UCNPs cannot be stably dispersed in aqueous solution and cannot carry photosensitive drugs directly. Besides, UCNP mediated PDT is a fluorescence resonance energy transfer (FRET) process from the UCNPs to the attached photosensitive drugs. So the drug and UCNPs must be stably connected and close enough. In this manuscript, carboxymethyl-β-cyclodextrin (COOH-β-CD) was used to connect UCNPs and adamantine modified phthalocyanine (Ad-ZnPc) through a self-assembly process followed by a host-guest interaction. COOH-β-CD can provide good water solubility of the system and short-distance linking between the UCNPs and Ad-ZnPc. Most importantly, the system has a strong NIR light triggered PDT activity toward cancer cells. PMID:26824705

  15. Upconversion of SrWO4:Er3+/Yb3+: Improvement by Yb3+ codoping and temperature sensitivity for optical temperature sensors

    NASA Astrophysics Data System (ADS)

    Wei, Zhen; Zheng, Wei; Zhu, Zhiyong; Guo, Xiongfei

    2016-05-01

    SrWO4:Er3+/Yb3+ phosphors are synthesized by a solid state reaction. The XRD patterns indicate that the doping ions will not change the phase of SrWO4. Under the excitation at 980 nm, SrWO4:Er3+/Yb3+ phosphors show emission bands in green and red regions. The temperature-dependence of upconversion efficiency and temperature-sensing properties of SrWO4:Er3+/Yb3+ phosphors have been discussed according to the fluorescence intensity ratio of green emissions from 2H11/2/4S3/2 → 4I15/2 transitions of Er3+ in the range of 95-775 K under the excitation at 980 nm. The maximum sensitivity of SrWO4:1%Er3+/6%Yb3+ phosphor is found to be 0.01282 K-1 at 489 K.

  16. Massively parallel femtosecond laser processing.

    PubMed

    Hasegawa, Satoshi; Ito, Haruyasu; Toyoda, Haruyoshi; Hayasaki, Yoshio

    2016-08-01

    Massively parallel femtosecond laser processing with more than 1000 beams was demonstrated. Parallel beams were generated by a computer-generated hologram (CGH) displayed on a spatial light modulator (SLM). The key to this technique is to optimize the CGH in the laser processing system using a scheme called in-system optimization. It was analytically demonstrated that the number of beams is determined by the horizontal number of pixels in the SLM NSLM that is imaged at the pupil plane of an objective lens and a distance parameter pd obtained by dividing the distance between adjacent beams by the diffraction-limited beam diameter. A performance limitation of parallel laser processing in our system was estimated at NSLM of 250 and pd of 7.0. Based on these parameters, the maximum number of beams in a hexagonal close-packed structure was calculated to be 1189 by using an analytical equation. PMID:27505815

  17. Femtosecond dynamics of cluster expansion

    NASA Astrophysics Data System (ADS)

    Gao, Xiaohui; Wang, Xiaoming; Shim, Bonggu; Arefiev, Alexey; Tushentsov, Mikhail; Breizman, Boris; Downer, Mike

    2010-03-01

    Noble gas clusters irradiated by intense ultrafast laser expand quickly and become typical plasma in picosecond time scale. During the expansion, the clustered plasma demonstrates unique optical properties such as strong absorption and positive contribution to the refractive index. Here we studied cluster expansion dynamics by fs-time-resolved refractive index and absorption measurements in cluster gas jets after ionization and heating by an intense pump pulse. The refractive index measured by frequency domain interferometry (FDI) shows the transient positive peak of refractive index due to clustered plasma. By separating it from the negative contribution of the monomer plasma, we are able to determine the cluster fraction. The absorption measured by a delayed probe shows the contribution from clusters of various sizes. The plasma resonances in the cluster explain the enhancement of the absorption in our isothermal expanding cluster model. The cluster size distribution can be determined. A complete understanding of the femtosecond dynamics of cluster expansion is essential in the accurate interpretation and control of laser-cluster experiments such as phase-matched harmonic generation in cluster medium.

  18. Femtosecond laser ablation of enamel

    NASA Astrophysics Data System (ADS)

    Le, Quang-Tri; Bertrand, Caroline; Vilar, Rui

    2016-06-01

    The surface topographical, compositional, and structural modifications induced in human enamel by femtosecond laser ablation is studied. The laser treatments were performed using a Yb:KYW chirped-pulse-regenerative amplification laser system (560 fs and 1030 nm) and fluences up to 14 J/cm2. The ablation surfaces were studied by scanning electron microscopy, grazing incidence x-ray diffraction, and micro-Raman spectroscopy. Regardless of the fluence, the ablation surfaces were covered by a layer of resolidified material, indicating that ablation is accompanied by melting of hydroxyapatite. This layer presented pores and exploded gas bubbles, created by the release of gaseous decomposition products of hydroxyapatite (CO2 and H2O) within the liquid phase. In the specimen treated with 1-kHz repetition frequency and 14 J/cm2, thickness of the resolidified material is in the range of 300 to 900 nm. The micro-Raman analysis revealed that the resolidified material contains amorphous calcium phosphate, while grazing incidence x-ray diffraction analysis allowed detecting traces of a calcium phosphate other than hydroxyapatite, probably β-tricalcium phosphate Ca3), at the surface of this specimen. The present results show that the ablation of enamel involves melting of enamel's hydroxyapatite, but the thickness of the altered layer is very small and thermal damage of the remaining material is negligible.

  19. Fabrication of freestanding silk fibroin films containing Ag nanowires/NaYF4:Yb,Er nanocomposites with metal-enhanced fluorescence behavior.

    PubMed

    Zhao, Bing; Qi, Ning; Zhang, Ke-Qin; Gong, Xiao

    2016-06-01

    Solar cells containing upconversion nanoparticles (UCNPs) used as a power source in biomedical nanosystems have attracted great interest. However, such solar cells further need to be developed because their substrate materials should be biocompatible, flexible and highly luminescent. Here, we report that freestanding silk fibroin (SF) films containing a mesh of silver nanowires (AgNWs) and β-NaYF4:Yb,Er nanocrystals with metal-enhanced fluorescence behavior can be fabricated. The freestanding composite films exhibit properties such as good optical transparency, conductivity and flexibility. Furthermore, they show significantly enhanced upconversion fluorescence due to surface plasmon polaritons (SPPs) of AgNWs compared to the SF-UCNP films without AgNWs. The freestanding composite films with metal-enhanced fluorescence behavior show great promise for future applications in self-powered nanodevices such as cardiac pacemakers, biosensors and nanorobots. PMID:27210511

  20. Photon-phonon anti-stokes upconversion of a photonically, electronically, and thermally isolated opal

    NASA Astrophysics Data System (ADS)

    Stem, Michelle R.

    2016-05-01

    The purpose of the present research was to investigate an intense violet shift displayed by a non-toxic, natural silicate material with a highly ordered nanostructure. The material displayed an unexpected, nonlinear 2:3 photon-phonon anti-Stokes upconversion while photonically, electronically, and thermally isolated. Conducted aphotonically and at ambient temperatures, the specimen upconverted a low-power, 650 nm constant wave red laser to an internally highly dispersed 433 nm violet wavelength. The strong dispersion was largely due to nearly total internal reflection of the laser. The upconversion had an efficiency of about 78 %, based on specimen volume, with no detectable thermal variance. The 2:3 anti-Stokes upconversion displayed by this material is likely the result of a previously unknown photon-phonon evanescence response that amplified the energy of a portion of the incident laser photons. Thus, a portion of the incident laser photons were upconverted, and the material converted another portion into an amplified energy that caused the upconversion. Internal micro-lasing appeared to be a means of photon-phonon evanescent energy redistribution, enabling dispersed photonic upconversion. Additional analyses also found an unexpectedly rhythmic photonic structure in spectrophotometric scans, polariscopic color changing, and previously undocumented ultraviolet responses.

  1. Infrared to visible and ultraviolet upconversion processes in Nd 3+-doped potassium lead chloride crystal

    NASA Astrophysics Data System (ADS)

    Mendioroz, A.; Balda, R.; Voda, M.; Al-Saleh, M.; Fernández, J.

    2004-09-01

    Infrared to visible and ultraviolet upconversion in Nd 3+ doped KPb 2Cl 5 crystal is reported. Three intense bands have been observed at 535, 595, and 668 nm coming mainly from levels 4G 7/2- 4G 9/2, together with emissions at 362, 388, 420 and 456 nm coming from level 4D 3/2, and a peak at 435 nm, corresponding to the 2P 1/2 → 4I 9/2 transition. A study of the upconversion mechanisms has been carried out that includes the upconversion emission dependence on the wavelength and intensity of the pumping light together with a comparison of the luminescence decays after infrared excitation and after direct one photon excitation of the emitting levels. The results indicate that two- and three-body energy transfer upconversion processes are responsible for emissions from levels 4G 7/2- 4G 9/2 and 4D 3/2 respectively, while level 2P 1/2 is populated by either energy transfer upconversion or excited state absorption depending on the pumping wavelength.

  2. Huge enhancement of upconversion luminescence by broadband dye sensitization of core/shell nanocrystals.

    PubMed

    Yin, Dongguang; Liu, Yumin; Tang, Jingxiu; Zhao, Feifei; Chen, Zhiwen; Zhang, Tingting; Zhang, Xinyu; Chang, Na; Wu, Chenglong; Chen, Dongwei; Wu, Minghong

    2016-09-14

    Upconversion nanocrystals (UCNCs) hold promise for bioimaging, solar cells, photocatalysis and volumetric displays. However, their upconversion luminescence intensities are usually low due to the weak and narrowband near-infrared absorption of lanthanide ions. Herein, we introduce and validate a strategy to hugely enhance upconversion luminescence intensity by using an organic near-infrared dye as an antenna to sensitize core/shell UCNCs. The dye can increase absorptivity and broaden the absorption spectrum of the UCNCs. Such dye sensitization, in combination with a core/shell structure, can tremendously enhance the upconversion luminescence (UCL) intensity of the UCNCs. The UCL intensity of dye-sensitized UCNCs excited at 820 nm is 800-folds higher than that of pure UCNCs excited at 980 nm. Further enhancement can be obtained by optimization of the dye emission and UCNC absorption spectral overlap. Moreover, the proposed approach can be extended to cover any part of the solar spectrum by using a set of dyes. This work provides new insights into the efficient enhancement of upconversion luminescence of the UCNCs and facilitates their applications. PMID:27484165

  3. 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

    2014-01-01

    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. PMID:25430519

  4. Two-photon upconversion affected by intermolecule correlations near metallic nanostructures

    NASA Astrophysics Data System (ADS)

    Osaka, Yoshiki; Yokoshi, Nobuhiko; Ishihara, Hajime

    2016-04-01

    We investigate an efficient two-photon upconversion process in more than one molecule coupled to an optical antenna. In the previous paper [Y. Osaka et al., Phys. Rev. Lett. 112, 133601 (2014), 10.1103/PhysRevLett.112.133601], we considered the two-photon upconversion process in a single molecule within one-dimensional input-output theory and revealed that controlling the antenna-molecule coupling enables the efficient upconversion with radiative loss in the antenna suppressed. In this paper, aiming to propose a way to enhance the total probability of antenna-photon scattering, we extend the model to the case of multiple molecules. In general, the presence of more than one molecule decreases the upconversion probability because they equally share the energy of the two photons. However, it is shown that we can overcome the difficulty by controlling the intermolecule coupling. Our result implies that, without increasing the incident photon number (light power), we can enlarge the net probability of the two-photon upconversion.

  5. Fluorescence advantages with microscopic spatiotemporal control

    NASA Astrophysics Data System (ADS)

    Goswami, Debabrata; Roy, Debjit; De, Arijit K.

    2013-03-01

    We present a clever design concept of using femtosecond laser pulses in microscopy by selective excitation or de-excitation of one fluorophore over the other overlapping one. Using either a simple pair of femtosecond pulses with variable delay or using a train of laser pulses at 20-50 Giga-Hertz excitation, we show controlled fluorescence excitation or suppression of one of the fluorophores with respect to the other through wave-packet interference, an effect that prevails even after the fluorophore coherence timescale. Such an approach can be used both under the single-photon excitation as well as in the multi-photon excitation conditions resulting in effective higher spatial resolution. Such high spatial resolution advantage with broadband-pulsed excitation is of immense benefit to multi-photon microscopy and can also be an effective detection scheme for trapped nanoparticles with near-infrared light. Such sub-diffraction limit trapping of nanoparticles is challenging and a two-photon fluorescence diagnostics allows a direct observation of a single nanoparticle in a femtosecond high-repetition rate laser trap, which promises new directions to spectroscopy at the single molecule level in solution. The gigantic peak power of femtosecond laser pulses at high repetition rate, even at low average powers, provide huge instantaneous gradient force that most effectively result in a stable optical trap for spatial control at sub-diffraction limit. Such studies have also enabled us to explore simultaneous control of internal and external degrees of freedom that require coupling of various control parameters to result in spatiotemporal control, which promises to be a versatile tool for the microscopic world.

  6. Enhancement of upconversion luminescence in Er 3+ doped tellurite glasses due to the introduction of PbCl 2

    NASA Astrophysics Data System (ADS)

    Yang, Jianhu; Dai, Nengli; Dai, Shixun; Wen, Lei; Hu, Lili; Jiang, Zhonghong

    2003-07-01

    The upconversion properties of Er 3+ doped lead chloride tellurite glasses under 980 nm excitation are investigated. Three intense emission bands centered at 525, 547, and 657 nm corresponding to the transitions 2H 11/2 → 4I 15/2, 4S 3/2 → 4I 15/2, and 4F 9/2 → 4I 15/2, respectively, simultaneously occurs. The important role of PbCl 2 in upconversion intensity is observed and its influence on the green (547 nm) and red (657 nm) emissions is compared and discussed. The dependence of upconversion intensities on excitation power and the possible upconversion mechanisms are evaluated. The high-populated 4I 11/2 level is supposed to serve as the intermediate state responsible for the upconversion processes.

  7. [Er3+:Yb3+ co-doped nanocrystals BaGd2ZnO5 of up-conversion optical temperature sensing].

    PubMed

    Liu, Yan-zhou; Yang, Yan-min; Guo, Yan-ming; Zhang, Lian-shui; Mi, Chao; Liu, Lin-lin

    2015-02-01

    By far, the most efficient upconversion nanocrystals luminescence materials BaGd2ZnO5: 4%Yb3+ , 1%Er3+, with stable chemical performance, were prepared by using Sol-gel method. XRD pattern shows that the sample is pure phase, belongs to the orthogonal crystals, and space group is Pbnm; SEM micrograph shows that the prepared sample of the morphology sized around 150 nm is evenly distributed. Samples with 971 nm semiconductor laser excitation produce a strong green emission, visible to the naked eye, and uponversion strength and pump energy relation n = 1.22 is two-photon for the realization of the upconversion emission. They originated from Er3+ ions 2H(11/2)--2H(11/2)-->4I(15/2) and 4S(3/2)-->4I(15/2) transition emission, Er3+ ions main excited state absorption (ESA) process is: 4I(15/2)-->4I(11/2)-->2F(7/2)-->2H(11/2), 4S(3/2), Yb3+ was added because of its large absorption cross section (10(4) cm(-1)) so that it is easy to transfer excitation energy to the E3+ ions which enhance the layout particles number and the energy state of the 1F7/2, thereby enhancing the intensity of the peaks of the spectrum. Fluorescence intensity ratio (FIR) technique based on the green upconversion emission of the sample has been studied because the Er3+ ions 2H(11/2) and 4S(3/2) energy level spacing is small. The electrons at the two levels conform to the Boltzmann distribution which is a function of temperature, and thus the fluorescence intensity ratio of two levels can be used to measure the temperature of the substrate material. This method does not interfere with temperature field of the measured object, and can eliminate the uncertainty of the accuracy; the test has a wide temperature range and reasonable temperature resolution, the pump source used is simple, convenient and inexpensive, and has more commercial values. The temperature range of the samples is from 350 to 800 K, and the highest temperature measuring sensitivity can reach 0.0031 K(1). At the same time, under low

  8. Progress in Cherenkov femtosecond fiber lasers

    NASA Astrophysics Data System (ADS)

    Liu, Xiaomin; Svane, Ask S.; Lægsgaard, Jesper; Tu, Haohua; Boppart, Stephen A.; Turchinovich, Dmitry

    2016-01-01

    We review the recent developments in the field of ultrafast Cherenkov fiber lasers. Two essential properties of such laser systems—broad wavelength tunability and high efficiency of Cherenkov radiation wavelength conversion are discussed. The exceptional performance of the Cherenkov fiber laser systems are highlighted—dependent on the realization scheme, the Cherenkov lasers can generate the femtosecond output tunable across the entire visible and even the UV range, and for certain designs more than 40% conversion efficiency from the pump to Cherenkov signal can be achieved. The femtosecond Cherenkov laser with all-fiber architecture is presented and discussed. Operating in the visible range, it delivers 100-200 fs wavelength-tunable pulses with multimilliwatt output power and exceptionally low noise figure an order of magnitude lower than the traditional wavelength tunable supercontinuum-based femtosecond sources. The applications for Cherenkov laser systems in practical biophotonics and biomedical applications, such as bio-imaging and microscopy, are discussed.

  9. Measurements of Intense Femtosecond Laser Pulse Propagation in Air

    NASA Astrophysics Data System (ADS)

    Ting, Antonio

    2004-11-01

    Intense femtosecond pulses generated from chirped pulse amplification (CPA) lasers can deliver laser powers many times above the critical power for self-focusing in air. Catastrophic collapse of the laser pulse is usually prevented by the defocusing of the plasma column formed when the laser intensity gets above the threshold for multiphoton ionization. The resultant laser/plasma filament can extend many meters as the laser pulse propagates in the atmosphere. We have carried out a series of experiments both for understanding the formation mechanisms of the filaments and the nonlinear effects such as white light and harmonics generation associated with them. Many applications of these filaments such as remote atmospheric breakdown, laser induced electrical discharge and femtosecond laser material interactions require direct measurements of their characteristics. Direct measurements of these filaments had been difficult because the high laser intensity ( ˜10^13 W/cm^2) can damage practically any optical diagnostics. A novel technique was invented to obtain the first absolute measurements of laser energy, transverse profile, fluence and spectral content of the filaments. We are investigating a ``remote atmospheric breakdown'' concept of remotely sensing chemical and biological compounds. A short intense laser pulse can be generated at a remote position by using the group velocity dispersion (GVD) of the air to compress an initially long, frequency negatively chirped laser pulse to generate the air breakdown and filaments. We have observed that nonlinear contributions to the laser spectrum through self-phase modulation can lead to modification of the linear GVD compression. We have also observed the generation of ultraviolet (UV) radiations from these filaments in air and the induced fluorescence by the UV radiation of a surrogate biological agent. These and other results such as laser induced electrical discharges will be presented.

  10. Femtosecond stimulated Raman spectroscopy of ultrafast biophysical reaction dynamics

    NASA Astrophysics Data System (ADS)

    McCamant, David William

    2004-12-01

    I have developed the technique of femtosecond stimulated Raman spectroscopy (FSRS), which enables the rapid acquisition of vibrational spectra with <100-fs time-resolution and <15-cm-1 frequency-resolution. FSRS uses three laser pulses: (1) a femtosecond visible actinic pump that initiates the photochemistry, (2) a narrow bandwidth picosecond Raman pump that provides the energy for amplification of the probe, and (3) a femtosecond continuum probe that is amplified at Raman resonances shifted from the Raman pump. FSRS has the ability to collect Raman spectra and depolarization ratios with only seconds of data averaging and negligible fluorescence interference. The capabilities of FSRS are explored through studies of the polyene beta-carotene. My initial experiments used picosecond time-resolved Stokes and anti-Stokes spontaneous resonance Raman spectroscopy to determine that vibrational relaxation in the S1 (2Ag-) electronic state is nearly complete within 2 ps and to quantify the intramolecular vibrational energy redistribution (IVR) processes in S0. FSRS studies on beta-carotene revealed that following optical excitation to S2 (1Bu +) the molecule relaxes to S1 in 160 fs where it undergoes rapid two-step IVR with 200- and 450-fs time constants. In later work, the FSRS spectrum of S2 beta-carotene was observed, which consists of three intense and broad bands at ˜1100, 1300 and 1650 cm-1 that exhibit kinetics matching the decay of the S2 near-infrared absorption. These data show that there is no additional intermediate 1B u- electronic state involved in the relaxation pathway of beta-carotene. FSRS was also used to study the photoisomerization dynamics in bacteriorhodopsin (bR). Spectra obtained during bR's excited state lifetime exhibit dispersive lineshapes at the ground-state frequencies that decay in 250 fs and are attributed to a nonlinear emission process. This relaxation is significantly faster than the decay of the stimulated emission (˜500 fs), indicating

  11. Femtosecond laser sintering of copper nanoparticles

    NASA Astrophysics Data System (ADS)

    Cheng, C. W.; Chen, J. K.

    2016-04-01

    The ultrafast melting of copper nanoparticles (NPs) induced by a femtosecond laser pulse with duration of 100 fs and wavelength of 800 nm is investigated theoretically and experimentally. The Cu pattern fabricated from sintering of a Cu NP-dispersed film by the femtosecond laser at a repetition rate of 80 MHz is experimentally studied. A one-dimensional two-temperature model with temperature-dependent material properties, including the extended Drude model for dynamic optical properties and the thermophysical properties, is employed to simulate the particles ultrafast melting and re-solidification process.

  12. Ultraviolet femtosecond laser ionization mass spectrometry.

    PubMed

    Imasaka, Totaro

    2008-01-01

    For this study, multiphoton ionization/mass spectrometry using an ultraviolet (UV) femtosecond laser was employed for the trace analysis of organic compounds. Some of the molecules, such as dioxins, contain several chlorine atoms and have short excited-state lifetimes due to a "heavy atom" effect. A UV femtosecond laser is, then, useful for efficient resonance excitation and subsequent ionization. A technique of multiphoton ionization using an extremely short laser pulse (e.g., <10 fs), referred to as "impulsive ionization," may have a potential for use in fragmentation-free ionization, thus providing information on molecular weight in mass spectrometry. PMID:18302290

  13. All-fiber femtosecond Cherenkov radiation source.

    PubMed

    Liu, Xiaomin; Lægsgaard, Jesper; Møller, Uffe; Tu, Haohua; Boppart, Stephen A; Turchinovich, Dmitry

    2012-07-01

    An all-fiber femtosecond source of spectrally isolated Cherenkov radiation is reported, to the best of our knowledge, for the first time. Using a monolithic, self-starting femtosecond Yb-doped fiber laser as the pump source and the combination of photonic crystal fibers as the wave-conversion medium, we demonstrate milliwatt-level, stable, and tunable Cherenkov radiation at visible wavelengths 580-630 nm, with pulse duration of sub-160-fs, and the 3 dB spectral bandwidth not exceeding 36 nm. Such an all-fiber Cherenkov radiation source is promising for practical applications in biophotonics such as bioimaging and microscopy. PMID:22743523

  14. Femtosecond laser fabricated microfluorescence-activated cell sorter for single cell recovery

    NASA Astrophysics Data System (ADS)

    Bragheri, F.; Paiè, P.; Nava, G.; Yang, T.; Minzioni, P.; Martinez Vazquez, R.; Bellini, N.; Ramponi, R.; Cristiani, I.; Osellame, R.

    2014-03-01

    Manipulation, sorting and recovering of specific live cells from samples containing less than a few thousand cells is becoming a major hurdle in rare cell exploration such as stem cell research or cell based diagnostics. Moreover the possibility of recovering single specific cells for culturing and further analysis would be of great impact in many biological fields ranging from regenerative medicine to cancer therapy. In recent years considerable effort has been devoted to the development of integrated and low-cost optofluidic devices able to handle single cells, which usually rely on microfluidic circuits that guarantee a controlled flow of the cells. Among the different microfabrication technologies, femtosecond laser micromachining (FLM) is ideally suited for this purpose as it provides the integration of both microfluidic and optical functions on the same glass chip leading to monolithic, robust and portable devices. Here a new optofluidic device is presented, which is capable of sorting and recovering of single cells, through optical forces, on the basis of their fluorescence and. Both fluorescence detection and single cell sorting functions are integrated in the microfluidic chip by FLM. The device, which is specifically designed to operate with a limited amount of cells but with a very high selectivity, is fabricated by a two-step process that includes femtosecond laser irradiation followed by chemical etching. The capability of the device to act as a micro fluorescence-activated cell sorter has been tested on polystyrene beads and on tumor cells and the results on the single live cell recovery are reported.

  15. 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. PMID:24733519

  16. Up-conversion in rare earth-doped silica hollow spheres

    NASA Astrophysics Data System (ADS)

    Fortes, Luís M.; Li, Yigang; Réfega, Ricardo; Clara Gonçalves, M.

    2012-06-01

    In the present work, Er/Yb co-doped silica hollow spheres are prepared in a two-step process. In a first step, polystyrene-core is silica coated in situ by a modified Stöber sol-gel method and in the second one, the sacrificial polystyrene core is thermally removed. The core-shell and the hollow spheres are characterized by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FTIR) and photoluminescence spectroscopy (PL). PL measurements show up-conversion phenomena upon excitation at 975 nm, through the emission of blue (˜490 nm), green (˜523 nm and ˜536 nm) and red (˜655 nm) light. The up-conversion phenomena are discussed and modelled. The developed model explains the up-conversion phenomena of Er/Yb co-doped silica hollow spheres, with special agreement for high Yb/Er ratio.

  17. Phase closure retrieval in an infrared-to-visible upconversion interferometer for high resolution astronomical imaging.

    PubMed

    Ceus, Damien; Tonello, Alessandro; Grossard, Ludovic; Delage, Laurent; Reynaud, François; Herrmann, Harald; Sohler, Wolfgang

    2011-04-25

    This paper demonstrates the use of a nonlinear upconversion process to observe an infrared source through a telescope array detecting the interferometric signal in the visible domain. We experimentally demonstrate the possibility to retrieve information on the phase of the object spectrum of an infrared source by using a three-arm upconversion interferometer. We focus our study on the acquisition of phase information of the complex visibility by means of the phase closure technique. In our experimental demonstration, a laboratory binary star with an adjustable photometric ratio is used as a test source. A real time comparison between a standard three-arm interferometer and our new concept using upconversion by sum-frequency generation demonstrates the preservation of phase information which is essential for image reconstruction. PMID:21643113

  18. Enhanced 2D-image upconversion using solid-state lasers.

    PubMed

    Pedersen, Christian; Karamehmedović, Emir; Dam, Jeppe Seidelin; Tidemand-Lichtenberg, Peter

    2009-11-01

    Based on enhanced upconversion, we demonstrate a highly efficient method for converting a full image from one part of the electromagnetic spectrum into a new desired wavelength region. By illuminating a metal transmission mask with a 765 nm Gaussian beam to create an image and subsequently focusing the image inside a nonlinear PPKTP crystal located in the high intra-cavity field of a 1342 nm solid-state Nd:YVO(4) laser, an upconverted image at 488 nm is generated. We have experimentally achieved an upconversion efficiency of 40% under CW conditions. The proposed technique can be further adapted for high efficiency mid-infrared image upconversion where direct and fast detection is difficult or impossible to perform with existing detector technologies. PMID:19997325

  19. Nonlinear spectral and lifetime management in upconversion nanoparticles by controlling energy distribution.

    PubMed

    Wang, Yu; Deng, Renren; Xie, Xiaoji; Huang, Ling; Liu, Xiaogang

    2016-03-17

    Optical tuning of lanthanide-doped upconversion nanoparticles has attracted considerable attention over the past decade because this development allows the advance of new frontiers in energy conversion, materials science, and biological imaging. Here we present a rational approach to manipulating the spectral profile and lifetime of lanthanide emission in upconversion nanoparticles by tailoring their nonlinear optical properties. We demonstrate that the incorporation of energy distributors, such as surface defects or an extra amount of dopants, into a rare-earth-based host lattice alters the decay behavior of excited sensitizers, thus markedly improving the emitters' sensitivity to excitation power. This work provides insight into mechanistic understanding of upconversion phenomena in nanoparticles and also enables exciting new opportunities of using these nanomaterials for photonic applications. PMID:26948717

  20. General synthesis route to fabricate uniform upconversion luminescent gadolinium oxide hollow spheres.

    PubMed

    Jia, Guang; Zhang, Cuimiao; Ding, Shiwen; Wang, Liyong

    2011-08-01

    Uniform upconversion luminescent gadolinium oxide hollow spheres were successfully synthesized via a homogeneous precipitation method with carbon spheres as template followed by a calcination process. During the annealing process, the carbon spheres template can be effectively removed and the amorphous precursor has converted to crystalline Gd2O3, which can be confirmed by the XRD and TG-DSC analysis. SEM and TEM images indicate that the Gd2O3 hollow spheres with diameters of 300-400 nm are uniform in size and distribution. The rare earth activator ions Ln3+-doped Gd2O3 hollow spheres exhibit intense upconversion luminescence with different colors under 980 nm light excitation, which may find potential applications in the fields such as drug delivery or biological labeling. Moreover, the upconversion luminescent mechanisms of the hollow spherical phosphors were investigated in detail. PMID:22103093

  1. Video rate passive millimeter-wave imager utilizing optical upconversion with improved size, weight, and power

    NASA Astrophysics Data System (ADS)

    Martin, Richard D.; Shi, Shouyuan; Zhang, Yifei; Wright, Andrew; Yao, Peng; Shreve, Kevin P.; Schuetz, Christopher A.; Dillon, Thomas E.; Mackrides, Daniel G.; Harrity, Charles E.; Prather, Dennis W.

    2015-05-01

    In this presentation we will discuss the performance and limitations of our 220 channel video rate passive millimeter wave imaging system based on a distributed aperture with optical upconversion architecture. We will cover our efforts to reduce the cost, size, weight, and power (CSWaP) requirements of our next generation imager. To this end, we have developed custom integrated circuit silicon-germanium (SiGe) low noise amplifiers that have been designed to efficiently couple with our high performance lithium niobate upconversion modules. We have also developed millimeter wave packaging and components in multilayer liquid crystal polymer (LCP) substrates which greatly improve the manufacturability of the upconversion modules. These structures include antennas, substrate integrated waveguides, filters, and substrates for InP and SiGe mmW amplifiers.

  2. Composition dependent frequency upconversion of Er 3+/Yb 3+-codoped lead chloride tellurite glasses

    NASA Astrophysics Data System (ADS)

    Xu, Shiqing; Wang, Guonian; Dai, Shixun; Zhang, Junjie; Hu, Lili; Jiang, Zhonghong

    2004-09-01

    The green and red upconversion luminescence of Er 3+ in lead chloride tellurite glasses excited at 980 nm is investigated. Three intense emission bands centered at 530, 545, and 658 nm corresponding to the transitions 4S3/2→ 4I 15/2, 2H11/2→ 4I15/2 and 4F9/2→ 4I15/2, respectively, were simultaneously observed at room temperature. With increasing PbCl 2 content, the intensity of green (530 nm) emissions increase slightly, while the green (545 nm) and red (658 nm) emissions increase significantly. The results indicate that PbCl 2 has more influence on the green (545 nm) and red (658 nm) emissions than the green (530 nm) emission. The dependence of upconversion intensities on excitation power and possible upconversion mechanisms are discussed and evaluated.

  3. Single-band upconversion nanoprobes for multiplexed simultaneous in situ molecular mapping of cancer biomarkers

    NASA Astrophysics Data System (ADS)

    Zhou, Lei; Wang, Rui; Yao, Chi; Li, Xiaomin; Wang, Chengli; Zhang, Xiaoyan; Xu, Congjian; Zeng, Aijun; Zhao, Dongyuan; Zhang, Fan

    2015-04-01

    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.

  4. 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

    2015-01-01

    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. PMID:25907226

  5. 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. PMID:27137295

  6. Ultra-sensitive and selective Hg{sup 2+} detection based on fluorescent carbon dots

    SciTech Connect

    Liu, Ruihua; Li, Haitao; Kong, Weiqian; Liu, Juan; Liu, Yang; Tong, Cuiyan; Zhang, Xing; Kang, Zhenhui

    2013-07-15

    Graphical abstract: Fluorescent carbon dots were efficiently synthesized by one-step sodium hydroxide-assisted reflux method from PEG and demonstrated to show high selectivity toward Hg2+ ions detection. - Highlights: • FCDs were synthesized by one-step sodium hydroxide-assisted reflux method from PEG. • The FCDs emit blue photoluminescence and have upconversion fluorescent property. • The FCDs show ultra-sensitive detective ability for Hg{sup 2+} ions. - Abstract: Fluorescent carbon dots (FCDs) were efficiently synthesized by one-step sodium hydroxide-assisted reflux method from poly(ethylene glycol) (PEG). The obtained FCDs exhibit excellent water-solubility and high stability. Under the UV irradiation, the FCDs could emit bright blue photoluminescence, and also they were found to show excellent up-conversion fluorescence. It was further demonstrated that such FCDs can serve as effective fluorescent sensing platform for Hg{sup 2+} ions detection with ultra-sensitivity and selectivity. The sensing system achieved a limit of detection as low as 1 fM, which is much lower than all the previous reported sensing systems for Hg{sup 2+} ions detection. This FCDs sensing system has been successfully applied for the analysis of Hg{sup 2+} ions in water samples from river, lake, and tap water, showing good practical feasibility.

  7. Nonlinear spectral and lifetime management in upconversion nanoparticles by controlling energy distribution

    NASA Astrophysics Data System (ADS)

    Wang, Yu; Deng, Renren; Xie, Xiaoji; Huang, Ling; Liu, Xiaogang

    2016-03-01

    Optical tuning of lanthanide-doped upconversion nanoparticles has attracted considerable attention over the past decade because this development allows the advance of new frontiers in energy conversion, materials science, and biological imaging. Here we present a rational approach to manipulating the spectral profile and lifetime of lanthanide emission in upconversion nanoparticles by tailoring their nonlinear optical properties. We demonstrate that the incorporation of energy distributors, such as surface defects or an extra amount of dopants, into a rare-earth-based host lattice alters the decay behavior of excited sensitizers, thus markedly improving the emitters' sensitivity to excitation power. This work provides insight into mechanistic understanding of upconversion phenomena in nanoparticles and also enables exciting new opportunities of using these nanomaterials for photonic applications.Optical tuning of lanthanide-doped upconversion nanoparticles has attracted considerable attention over the past decade because this development allows the advance of new frontiers in energy conversion, materials science, and biological imaging. Here we present a rational approach to manipulating the spectral profile and lifetime of lanthanide emission in upconversion nanoparticles by tailoring their nonlinear optical properties. We demonstrate that the incorporation of energy distributors, such as surface defects or an extra amount of dopants, into a rare-earth-based host lattice alters the decay behavior of excited sensitizers, thus markedly improving the emitters' sensitivity to excitation power. This work provides insight into mechanistic understanding of upconversion phenomena in nanoparticles and also enables exciting new opportunities of using these nanomaterials for photonic applications. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr00812g

  8. NIR photoregulated chemo- and photodynamic cancer therapy based on conjugated polyelectrolyte-drug conjugate encapsulated upconversion nanoparticles

    NASA Astrophysics Data System (ADS)

    Yuan, Youyong; Min, Yuanzeng; Hu, Qinglian; Xing, Bengang; Liu, Bin

    2014-09-01

    The design of nanoplatforms with target recognition and near-infrared (NIR) laser photoregulated chemo- and photodynamic therapy is highly desirable but remains challenging. In this work, we have developed such a system by taking advantage of a conjugated polyelectrolyte (CPE)-drug conjugate and upconversion nanoparticles (UCNPs). The poly(ethylene glycol) (PEG) grafted CPE not only serves as a polymer matrix for UCNP encapsulation, but also as a fluorescent imaging agent, a photosensitizer as well as a carrier for chemotherapeutic drug doxorubicin (DOX) through a UV-cleavable ortho-nitrobenzyl (NB) linker. Upon 980 nm laser irradiation, the UCNPs emit UV and visible light. The up-converted UV light is utilized for controlled drug release through the photocleavage of the ortho-nitrobenzyl linker, while the up-converted visible light is used to initiate the polymer photosensitizer to produce reactive oxygen species (ROS) for photodynamic therapy. The NIR photo-regulated UCNP@CPE-DOX showed high efficiency of ROS generation and controlled drug release in cancer cells upon single laser irradiation. In addition, the combination therapy showed enhanced inhibition of U87-MG cell growth as compared to sole treatments. As two light sources with different wavelengths are always needed for traditional photodynamic therapy and photoregulated drug release, the adoption of UCNPs as an NIR light switch is highly beneficial to combined chemo- and photodynamic therapy with enhanced therapeutic effects.

  9. Controllable synthesis and upconversion emission of ultrasmall lanthanide-doped Sr2GdF7 nanocrystals

    NASA Astrophysics Data System (ADS)

    Xiang, Lijun; Ren, Guozhong; Mao, Yifu; He, Jin; Su, Rui

    2015-11-01

    The effect of rare-earth ions content on the phase structure, crystal size and morphology of SrF2-GdF3 system were studied under solvothermal conditions. By tuning the molar ratio of reactants, tetragonal phase Sr2GdF7 nanocrystals (NCs) were synthesized via solvothermal method using oleic acid as capping ligands. The effects of reaction conditions on the phase structure, crystal size, morphology, and upconversion (UC) emission properties of the products were investigated. The results reveal that apropos Gd3+ ions content (0.30-0.45 mmol) is favorable to the formation of pure phase Sr2GdF7 NCs with more uniform size distribution. The average crystalline size of the products can be controlled less than 10 nm. The energy transfer UC mechanisms for the fluorescent intensity were also investigated. Following Yb3+, Er3+, Tm3+ and Ho3+ ions doping, the Sr2GdF7 NCs show intense green, yellow, and white-color UC emission under the excitation of a 980 nm laser, and the doping concentration of lanthanide ions was optimized, which makes the NCs show maximum intensities under the excitation of a 980 nm laser.

  10. Self-assembly NaGdF4 nanoparticles: phase controlled synthesis, morphology evolution, and upconversion luminescence properties

    NASA Astrophysics Data System (ADS)

    Zi, Lu; Zhang, Dan; De, Gejihu

    2016-02-01

    Cubic NaGdF4:Yb0.2Er0.02 (α-NaGdF4), self-assembly cubic NaGdF4:Yb0.2Er0.02, and high-resolution structure of hexagonal NaGdF4:Yb0.2Er0.02 (β-NaGdF4) nanoparticles are prepared via the co-thermolysis of Gd(CF3COO)3 and CF3COONa in the presence of 1-octadecene as stabilizer and oleic acid as ligand. Transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), x-ray power diffraction (XRD), and Hitachi F-4600 fluorescence spectrophotometer are used for the characterization of the samples. The results show that by tuning the ratio of CF3COONa/Gd(CF3COO)3 and the reaction temperature, we can control the crystal phase, the relative intensity of upconversion luminescence of nanoparticles, and the morphology evolution of self-assembled α-NaGdF4 nanoparticles.

  11. Rational design of a thermalresponsive-polymer-switchable FRET system for enhancing the temperature sensitivity of upconversion nanophosphors.

    PubMed

    Xiao, Qingbo; Li, Yanfang; Li, Fujin; Zhang, Mengxin; Zhang, Zhijun; Lin, Hongzhen

    2014-09-01

    Here we propose a thermoresponsive polymer PNIPAM modulated fluorescence resonance energy transfer (FRET) system to enhance the temperature sensitivity of upconversion nanophosphors (UCNPs). By utilizing red/near-infrared dual emitting NaLuF4:Mn(2+),Ln(3+) (Ln(3+) = Yb(3+), Er(3+), Tm(3+)) UCNPs as the energy donor and Au nanoparticles as the acceptor, the temperature resolution of the UCNPs is significantly increased from 3.1 °C to 0.9 °C in the physiological temperature range. Conjugating the UCNPs and acceptors into discrete nanocomposites in our samples facilitates reversible regulation of the emission intensity of UCNPs, which thus would extend their application range in biosensing, especially for probing the dynamic changes of local micro-environments in biological tissues. As there are a broad variety of stimuli to which smart polymers can reversibly respond, our experiments are also extendable to various external conditions in local micro-environments, such as pH values, metal ions, glucose, and tissue-specific enzymes. PMID:25046250

  12. Facile microemulsion route to coat carbonized glucose on upconversion nanocrystals as high luminescence and biocompatible cell-imaging probes.

    PubMed

    Li, Zhengquan; Guo, Huichen; Qian, Haisheng; Hu, Yong

    2010-08-01

    Surface modification of lanthanide-doped upconversion nanocrystals is crucial to make them useful for various biological applications. Unfortunately, the current methods available to achieve a desirable surface exhibiting both high luminescence and good biocompatibility are limited. In this work, we present a facile microemulsion route to coat carbonized glucose on hydrophobic NaYF(4) nanocrystals. Owing to the particular structure of the carbonized shell, glucose coating on these UCNs is not only able to preserve strong fluorescence from the core nanocrystals, but it also confers good water solubility and bears various functional groups for conjugating to biomolecules. Compared to 10 nm silica-coated UCNs, these glucose-coated nanocrystals possess better cell biocompatibility, and can be rapidly internalized into cells. Such unique features of glucose-coated UCNs may find promising applications in imaging, diagnosis and therapeutic purposes. Besides, this facile surface-modification route has the potential to be extended to a broad range of other hydrophobic nanocrystals. PMID:20634574

  13. NaYF4:Yb,Tm nanocrystals and TiO2 inverse opal composite films: a novel device for upconversion enhancement and solid-based sensing of avidin

    NASA Astrophysics Data System (ADS)

    Xu, Sai; Xu, Wen; Wang, Yunfeng; Zhang, Shuang; Zhu, Yongsheng; Tao, Li; Xia, Lei; Zhou, Pingwei; Song, Hongwei

    2014-05-01

    Upconversion luminescence (UCL) detection based on rare-earth doped upconversion nanocrystals (UCNCs) as probes has been proved to exhibit a large anti-Stokes shift, no autofluorescence from biological samples, and no photobleaching. However, it is still a challenge to achieve a stable, reproducible solid-based UCL biosensor because of ineffective UCL of the UCNCs. In this work, we fabricated TiO2 inverse opal photonic crystals (IOPCs)/NaYF4:Yb3+,Tm3+ (Er3+) UCNC composite films, which can tremendously improve the overall UCL of Tm3+ as high as 43-fold. Based on the fluorescence resonance energy transfer (FRET) and the specific interaction between biotin and avidin, a novel solid-based UC biosensor is presented for sensing avidin. This solid-based detection system is convenient for detection, and also can offer two parameters for detecting trace amounts of avidin, namely, the emission intensity and the fluorescence decay time. The sensor has a high sensitivity of 34 pmol-1, a good linear relationship of 0.996 and a low detection limit of 48 pmol. It also exhibits excellent long-time photostability, and the absence of autofluorescence, and thus may have great potential for versatile applications in biodetection.

  14. NaYF4:Yb,Tm nanocrystals and TiO2 inverse opal composite films: a novel device for upconversion enhancement and solid-based sensing of avidin.

    PubMed

    Xu, Sai; Xu, Wen; Wang, Yunfeng; Zhang, Shuang; Zhu, Yongsheng; Tao, Li; Xia, Lei; Zhou, Pingwei; Song, Hongwei

    2014-06-01

    Upconversion luminescence (UCL) detection based on rare-earth doped upconversion nanocrystals (UCNCs) as probes has been proved to exhibit a large anti-Stokes shift, no autofluorescence from biological samples, and no photobleaching. However, it is still a challenge to achieve a stable, reproducible solid-based UCL biosensor because of ineffective UCL of the UCNCs. In this work, we fabricated TiO2 inverse opal photonic crystals (IOPCs)/NaYF4:Yb(3+),Tm(3+) (Er(3+)) UCNC composite films, which can tremendously improve the overall UCL of Tm(3+) as high as 43-fold. Based on the fluorescence resonance energy transfer (FRET) and the specific interaction between biotin and avidin, a novel solid-based UC biosensor is presented for sensing avidin. This solid-based detection system is convenient for detection, and also can offer two parameters for detecting trace amounts of avidin, namely, the emission intensity and the fluorescence decay time. The sensor has a high sensitivity of 34 pmol(-1), a good linear relationship of 0.996 and a low detection limit of 48 pmol. It also exhibits excellent long-time photostability, and the absence of autofluorescence, and thus may have great potential for versatile applications in biodetection. PMID:24752220

  15. 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

  16. 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

  17. Upconversion Nanoparticles for Photodynamic Therapy and Other Cancer Therapeutics

    PubMed Central

    Wang, Chao; Cheng, Liang; Liu, Zhuang

    2013-01-01

    Photodynamic therapy (PDT) is a non-invasive treatment modality for a variety of diseases including cancer. PDT based on upconversion nanoparticles (UCNPs) has received much attention in recent years. Under near-infrared (NIR) light excitation, UCNPs are able to emit high-energy visible light, which can activate surrounding photosensitizer (PS) molecules to produce singlet oxygen and kill cancer cells. Owing to the high tissue penetration ability of NIR light, NIR-excited UCNPs can be used to activate PS molecules in much deeper tissues compared to traditional PDT induced by visible or ultraviolet (UV) light. In addition to the application of UCNPs as an energy donor in PDT, via similar mechanisms, they could also be used for the NIR light-triggered drug release or activation of 'caged' imaging or therapeutic molecules. In this review, we will summarize the latest progresses regarding the applications of UCNPs for photodynamic therapy, NIR triggered drug and gene delivery, as well as several other UCNP-based cancer therapeutic approaches. The future prospects and challenges in this emerging field will be also discussed. PMID:23650479

  18. Near-infrared (NIR) up-conversion optogenetics.

    PubMed

    Hososhima, Shoko; Yuasa, Hideya; Ishizuka, Toru; Hoque, Mohammad Razuanul; Yamashita, Takayuki; Yamanaka, Akihiro; Sugano, Eriko; Tomita, Hiroshi; Yawo, Hiromu

    2015-01-01

    Non-invasive remote control technologies designed to manipulate neural functions have been long-awaited for the comprehensive and quantitative understanding of neuronal network in the brain as well as for the therapy of neurological disorders. Recently, it has become possible for the neuronal activity to be optically manipulated using biological photo-reactive molecules such as channelrhodopsin (ChR)-2. However, ChR2 and its relatives are mostly reactive to visible light, which does not effectively penetrate through biological tissues. In contrast, near-infrared (NIR) light (650-1450 nm) penetrates deep into the tissues because biological systems are almost transparent to light within this so-called 'imaging window'. Here we used lanthanide nanoparticles (LNPs), composed of rare-earth elements, as luminous bodies to activate ChRs since they absorb low-energy NIR light to emit high-energy visible light (up-conversion). Here, we created a new type of optogenetic system which consists of the donor LNPs and the acceptor ChRs. The NIR laser irradiation emitted visible light from LNPs, then induced the photo-reactive responses in the near-by cells that expressed ChRs. However, there remains room for large improvements in the energy efficiency of the LNP-ChR system. PMID:26552717

  19. Core-shell upconversion nanoparticle - semiconductor heterostructures for photodynamic therapy.

    PubMed

    Dou, Qing Qing; Rengaramchandran, Adith; Selvan, Subramanian Tamil; Paulmurugan, Ramasamy; Zhang, Yong

    2015-01-01

    Core-shell nanoparticles (CSNPs) with diverse chemical compositions have been attracting greater attention in recent years. However, it has been a challenge to develop CSNPs with different crystal structures due to the lattice mismatch of the nanocrystals. Here we report a rational design of core-shell heterostructure consisting of NaYF4:Yb,Tm upconversion nanoparticle (UCN) as the core and ZnO semiconductor as the shell for potential application in photodynamic therapy (PDT). The core-shell architecture (confirmed by TEM and STEM) enables for improving the loading efficiency of photosensitizer (ZnO) as the semiconductor is directly coated on the UCN core. Importantly, UCN acts as a transducer to sensitize ZnO and trigger the generation of cytotoxic reactive oxygen species (ROS) to induce cancer cell death. We also present a firefly luciferase (FLuc) reporter gene based molecular biosensor (ARE-FLuc) to measure the antioxidant signaling response activated in cells during the release of ROS in response to the exposure of CSNPs under 980 nm NIR light. The breast cancer cells (MDA-MB-231 and 4T1) exposed to CSNPs showed significant release of ROS as measured by aminophenyl fluorescein (APF) and ARE-FLuc luciferase assays, and ~45% cancer cell death as measured by MTT assay, when illuminated with 980 nm NIR light. PMID:25652742

  20. Near-infrared (NIR) up-conversion optogenetics

    NASA Astrophysics Data System (ADS)

    Hososhima, Shoko; Yuasa, Hideya; Ishizuka, Toru; Hoque, Mohammad Razuanul; Yamashita, Takayuki; Yamanaka, Akihiro; Sugano, Eriko; Tomita, Hiroshi; Yawo, Hiromu

    2015-11-01

    Non-invasive remote control technologies designed to manipulate neural functions have been long-awaited for the comprehensive and quantitative understanding of neuronal network in the brain as well as for the therapy of neurological disorders. Recently, it has become possible for the neuronal activity to be optically manipulated using biological photo-reactive molecules such as channelrhodopsin (ChR)-2. However, ChR2 and its relatives are mostly reactive to visible light, which does not effectively penetrate through biological tissues. In contrast, near-infrared (NIR) light (650-1450 nm) penetrates deep into the tissues because biological systems are almost transparent to light within this so-called ‘imaging window’. Here we used lanthanide nanoparticles (LNPs), composed of rare-earth elements, as luminous bodies to activate ChRs since they absorb low-energy NIR light to emit high-energy visible light (up-conversion). Here, we created a new type of optogenetic system which consists of the donor LNPs and the acceptor ChRs. The NIR laser irradiation emitted visible light from LNPs, then induced the photo-reactive responses in the near-by cells that expressed ChRs. However, there remains room for large improvements in the energy efficiency of the LNP-ChR system.

  1. Core - shell upconversion nanoparticle - semiconductor heterostructures for photodynamic therapy

    NASA Astrophysics Data System (ADS)

    Dou, Qing Qing; Rengaramchandran, Adith; Selvan, Subramanian Tamil; Paulmurugan, Ramasamy; Zhang, Yong

    2015-02-01

    Core-shell nanoparticles (CSNPs) with diverse chemical compositions have been attracting greater attention in recent years. However, it has been a challenge to develop CSNPs with different crystal structures due to the lattice mismatch of the nanocrystals. Here we report a rational design of core-shell heterostructure consisting of NaYF4:Yb,Tm upconversion nanoparticle (UCN) as the core and ZnO semiconductor as the shell for potential application in photodynamic therapy (PDT). The core-shell architecture (confirmed by TEM and STEM) enables for improving the loading efficiency of photosensitizer (ZnO) as the semiconductor is directly coated on the UCN core. Importantly, UCN acts as a transducer to sensitize ZnO and trigger the generation of cytotoxic reactive oxygen species (ROS) to induce cancer cell death. We also present a firefly luciferase (FLuc) reporter gene based molecular biosensor (ARE-FLuc) to measure the antioxidant signaling response activated in cells during the release of ROS in response to the exposure of CSNPs under 980 nm NIR light. The breast cancer cells (MDA-MB-231 and 4T1) exposed to CSNPs showed significant release of ROS as measured by aminophenyl fluorescein (APF) and ARE-FLuc luciferase assays, and ~45% cancer cell death as measured by MTT assay, when illuminated with 980 nm NIR light.

  2. Background free imaging of upconversion nanoparticle distribution in human skin

    NASA Astrophysics Data System (ADS)

    Song, Zhen; Anissimov, Yuri G.; Zhao, Jiangbo; Nechaev, Andrei V.; Nadort, Annemarie; Jin, Dayong; Prow, Tarl W.; Roberts, Michael S.; Zvyagin, Andrei V.

    2013-06-01

    Widespread applications of nanotechnology materials have raised safety concerns due to their possible penetration through skin and concomitant uptake in the organism. This calls for systematic study of nanoparticle transport kinetics in skin, where high-resolution optical imaging approaches are often preferred. We report on application of emerging luminescence nanomaterial, called upconversion nanoparticles (UCNPs), to optical imaging in skin that results in complete suppression of background due to the excitation light back-scattering and biological tissue autofluorescence. Freshly excised intact and microneedle-treated human skin samples were topically coated with oil formulation of UCNPs and optically imaged. In the first case, 8- and 32-nm UCNPs stayed at the topmost layer of the intact skin, stratum corneum. In the second case, 8-nm nanoparticles were found localized at indentations made by the microneedle spreading in dermis very slowly (estimated diffusion coefficient, Dnp=3-7×10-12 cm2.s-1). The maximum possible UCNP-imaging contrast was attained by suppressing the background level to that of the electronic noise, which was estimated to be superior in comparison with the existing optical labels.

  3. Basic understanding of the lanthanide related upconversion emissions.

    PubMed

    Dong, Hao; Sun, Ling-Dong; Yan, Chun-Hua

    2013-07-01

    With abundant energy levels of 4f electron configurations, trivalent lanthanide ions (Ln(3+)) are endowed with unique and fascinating luminescent properties. Inheriting the native transition behaviour of the lanthanide ions, Ln(3+) based nanomaterials have aroused great interest for a wide range of applications, including lighting and displays, optical fibers and amplifiers, responsive luminescent stains for biomedical analysis, in vivo and in vitro imaging, and enhancement for silicon solar cell devices. It should be noted that the application depends completely on the corresponding luminescent behaviour. To deepen the understanding of the luminescent mechanism is important for the developing of the field and the design of new Ln(3+) based luminescent materials toward applications. In this review, we focused mainly on the recent developments on upconversion (UC) emission studies. Firstly, the emphasis was put on the introduction of basic luminescent properties of Ln(3+) with f-f transitions, and then the corresponding mechanisms and properties of UC emission were discussed in detail, the potential researches with respect to UC mechanisms and properties were finally outlined. PMID:23423120

  4. Sensing using rare-earth-doped upconversion nanoparticles.

    PubMed

    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

  5. Near-infrared (NIR) up-conversion optogenetics

    PubMed Central

    Hososhima, Shoko; Yuasa, Hideya; Ishizuka, Toru; Hoque, Mohammad Razuanul; Yamashita, Takayuki; Yamanaka, Akihiro; Sugano, Eriko; Tomita, Hiroshi; Yawo, Hiromu

    2015-01-01

    Non-invasive remote control technologies designed to manipulate neural functions have been long-awaited for the comprehensive and quantitative understanding of neuronal network in the brain as well as for the therapy of neurological disorders. Recently, it has become possible for the neuronal activity to be optically manipulated using biological photo-reactive molecules such as channelrhodopsin (ChR)-2. However, ChR2 and its relatives are mostly reactive to visible light, which does not effectively penetrate through biological tissues. In contrast, near-infrared (NIR) light (650–1450 nm) penetrates deep into the tissues because biological systems are almost transparent to light within this so-called ‘imaging window’. Here we used lanthanide nanoparticles (LNPs), composed of rare-earth elements, as luminous bodies to activate ChRs since they absorb low-energy NIR light to emit high-energy visible light (up-conversion). Here, we created a new type of optogenetic system which consists of the donor LNPs and the acceptor ChRs. The NIR laser irradiation emitted visible light from LNPs, then induced the photo-reactive responses in the near-by cells that expressed ChRs. However, there remains room for large improvements in the energy efficiency of the LNP-ChR system. PMID:26552717

  6. 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. PMID:26487270

  7. Upconversion-based receivers for quantum hacking-resistant quantum key distribution

    NASA Astrophysics Data System (ADS)

    Jain, Nitin; Kanter, Gregory S.

    2016-04-01

    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.

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

    NASA Astrophysics Data System (ADS)

    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.

  9. 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. PMID:22265952

  10. 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.

  11. Wideband signal upconversion and phase shifting based on a frequency tunable optoelectronic oscillator

    NASA Astrophysics Data System (ADS)

    Liu, Shifeng; Zhu, Dan; Pan, Shilong

    2014-03-01

    A wideband signal upconversion and phase shifting scheme based on a frequency tunable optoelectronic oscillator (OEO) are proposed and demonstrated. The OEO performs simultaneously tunable high-quality local oscillator (LO) signal generation, wideband frequency upconversion, and phase shifting within the whole 2π range. With the generated LO tuning from 9.549 to 11.655 GHz, wideband square signals are successfully upconverted to the X band. The phase of the upconverted signal is tuned from 0 to 360 deg. The phase noise of the oscillation signal is about -104 dBc/Hz at 10 kHz offset with or without the injected baseband signal.

  12. Label-free multi-photon imaging using a compact femtosecond fiber laser mode-locked by carbon nanotube saturable absorber

    PubMed Central

    Kieu, K.; Mehravar, S.; Gowda, R.; Norwood, R. A.; Peyghambarian, N.

    2013-01-01

    We demonstrate label-free multi-photon imaging of biological samples using a compact Er3+-doped femtosecond fiber laser mode-locked by a single-walled carbon nanotube (CNT). These compact and low cost lasers have been developed by various groups but they have not been exploited for multiphoton microscopy. Here, it is shown that various multiphoton imaging modalities (e.g. second harmonic generation (SHG), third harmonic generation (THG), two-photon excitation fluorescence (TPEF), and three-photon excitation fluorescence (3PEF)) can be effectively performed on various biological samples using a compact handheld CNT mode-locked femtosecond fiber laser operating in the telecommunication window near 1560nm. We also show for the first time that chlorophyll fluorescence in plant leaves and diatoms can be observed using 1560nm laser excitation via three-photon absorption. PMID:24156074

  13. Reversible permeabilization using high-intensity femtosecond laser pulses: applications to biopreservation.

    PubMed

    Kohli, Vikram; Acker, Jason P; Elezzabi, Abdulhakem Y

    2005-12-30

    Non-invasive manipulation of live cells is important for cell-based therapeutics. Herein we report on the uniqueness of using high-intensity femtosecond laser pulses for reversibly permeabilizing mammalian cells for biopreservation applications. When mammalian cells were suspended in a impermeable hyperosmotic cryoprotectant sucrose solution, femtosecond laser pulses were used to transiently permeabilize cells for cytoplasmic solute uptake. The kinetics of cells exposed to 0.2, 0.3, 0.4, and 0.5 M sucrose, following permeabilization, were measured using video microscopy, and post-permeabilization survival was determined by a dual fluorescence membrane integrity assay. Using appropriate laser parameters, we observed the highest cell survival for 0.2 M sucrose solution (>90%), with a progressive decline in cell survival towards higher concentrations. Using diffusion equations describing the transport of solutes, the intracellular osmolarity at the inner surface of the membrane (x = 10 nm) and to a diffusive length of x = 10 microm was estimated, and a high loading efficiency (>98% for x = 10 nm and >70% for x = 10 microm) was calculated for cells suspended in 0.2 M sucrose. This is the first report of using femtosecond laser pulses for permeabilizing cells in the presence of cryoprotectants for biopreservation applications. PMID:16189821

  14. Atmospheric pressure femtosecond laser imaging mass spectrometry

    NASA Astrophysics Data System (ADS)

    Coello, Yves; Gunaratne, Tissa C.; Dantus, Marcos

    2009-02-01

    We present a novel imaging mass spectrometry technique that uses femtosecond laser pulses to directly ionize the sample. The method offers significant advantages over current techniques by eliminating the need of a laser-absorbing sample matrix, being suitable for atmospheric pressure sampling, and by providing 10μm resolution, as demonstrated here with a chemical image of vegetable cell walls.

  15. Two-photon-excited luminescence from a Eu3+-doped lithium niobate crystal pumped by a near-infrared femtosecond laser

    NASA Astrophysics Data System (ADS)

    Li, Ai-Hua; Zheng, Zhi-Ren; Lü, Qiang; Xu, Zhao-Peng; Sun, Liang; Liu, Wei-Long; Wu, Wen-Zhi; Lü, Tian-Quan

    2010-09-01

    Red upconversion luminescence (UCL) is observed using an 800 nm femtosecond laser to irradiate a Eu3+-doped LiNbO3 single crystal. Power-dependent and polarization-dependent experiments demonstrate that the red UCL originates from Eu3+ two-photon simultaneous absorption rather than second harmonic generation of nonlinear optical crystal followed by reabsorption of Eu3+. Two different kinds of Eu3+-centers, called Eu3+-pairs, are revealed via emission spectra. Besides using femtosecond laser excitation to simulate diode laser excitation with broad line, the efficient two-photon simultaneous absorption can populate more Eu3+ to upper levels, these are beneficial to the study of cross relaxation with submicrosecond resolution between Eu3+-pairs occurred in practical application. Transient UCL spectra and decay curves suggest that the luminescent state D50 is fed by way of both multiphonon relaxation through state D51 and cross relaxation of D52+F70→D50+F75.

  16. Controllable synthesis of NaYF4 : Yb,Er upconversion nanophosphors and their application to in vivo imaging of Caenorhabditis elegans†

    PubMed Central

    Chen, Jing; Guo, Changrun; Wang, Meng; Huang, Lei; Mi, Congcong; Li, Jing; Fang, Xuexun

    2011-01-01

    β-NaYF4 : Yb,Er upconversion nanoparticles (UCNPs) can emit bright green fluorescence under near-infrared (NIR) light excitation which is safe to the body and can penetrate deeply into tissues. The application of UCNPs in biolabeling and imaging has received great attention recently. In this work, β-NaYF4 : Yb,Er UCNPs with an average size of 35 nm, uniformly spherical shape, and surface modified with amino groups were synthesized by a one-step green solvothermal approach through the use of room-temperature ionic liquids as the reactant, co-solvent and template. The as-prepared UCNPs were introduced into Caenorhabditis elegans (C. elegans) to achieve successful in vivo imaging. We found that longer incubation time, higher UCNP concentration and smaller UCNP size can make the in vivo fluorescence of C. elegans much brighter and more continuous along their body. The worms have no apparent selectivity on ingestion of the UCNPs capped with different capping ligands while having similar size and shape. The next generation of worms did not show fluorescence under excitation. In addition, low toxicity of the nanoparticles was demonstrated by investigating the survival rates of the worms in the presence of the UCNPs. Our work demonstrates the potential application of the UCNPs in studying the biological behavior of organisms, and lays the foundation for further development of the UCNPs in the detection and diagnosis of diseases. PMID:21666862

  17. Size/morphology induced tunable luminescence in upconversion crystals: ultra-strong single-band emission and underlying mechanisms

    NASA Astrophysics Data System (ADS)

    Wang, Zhaofeng; Zeng, Songshan; Yu, Jingfang; Ji, Xiaoming; Zeng, Huidan; Xin, Shuangyu; Wang, Yuhua; Sun, Luyi

    2015-05-01

    In this work, we present a two-step method to controllably synthesize novel and highly efficient upconversion materials, Lu5O4F7:Er3+,Yb3+ nano/micro-crystals, and investigate their size/morphology induced tunable upconversion properties. In addition to the common phenomenon aroused by a surface quenching effect, direct experimental evidence for the regulation of phonon modes is obtained in nanoparticles. The findings in this work advance the existing mechanisms for the general explanation of size/morphology induced upconversion features. Because of the adjustment of phonon energy and density as well as the surface quenching effect, the biocompatible Lu5O4F7:Er3+,Yb3+ nanoparticles exhibit an ultra-strong single-band red upconversion, rendering them promising for biomedical applications.In this work, we present a two-step method to controllably synthesize novel and highly efficient upconversion materials, Lu5O4F7:Er3+,Yb3+ nano/micro-crystals, and investigate their size/morphology induced tunable upconversion properties. In addition to the common phenomenon aroused by a surface quenching effect, direct experimental evidence for the regulation of phonon modes is obtained in nanoparticles. The findings in this work advance the existing mechanisms for the general explanation of size/morphology induced upconversion features. Because of the adjustment of phonon energy and density as well as the surface quenching effect, the biocompatible Lu5O4F7:Er3+,Yb3+ nanoparticles exhibit an ultra-strong single-band red upconversion, rendering them promising for biomedical applications. Electronic supplementary information (ESI) available: Crystal structure analysis, UV-Vis absorption spectra, SEM micrographs, surface micro-structure investigation, biocompatibility of Lu5O4F7: Er3+, Yb3+, as well as morphology and upconversion properties of the control sample NaYF4: Er3+, Yb3+. See DOI: 10.1039/c5nr01008j

  18. Highly efficient blue electroluminescence based on thermally activated delayed fluorescence.

    PubMed

    Hirata, Shuzo; Sakai, Yumi; Masui, Kensuke; Tanaka, Hiroyuki; Lee, Sae Youn; Nomura, Hiroko; Nakamura, Nozomi; Yasumatsu, Mao; Nakanotani, Hajime; Zhang, Qisheng; Shizu, Katsuyuki; Miyazaki, Hiroshi; Adachi, Chihaya

    2015-03-01

    Organic compounds that exhibit highly efficient, stable blue emission are required to realize inexpensive organic light-emitting diodes for future displays and lighting applications. Here, we define the design rules for increasing the electroluminescence efficiency of blue-emitting organic molecules that exhibit thermally activated delayed fluorescence. We show that a large delocalization of the highest occupied molecular orbital and lowest unoccupied molecular orbital in these charge-transfer compounds enhances the rate of radiative decay considerably by inducing a large oscillator strength even when there is a small overlap between the two wavefunctions. A compound based on our design principles exhibited a high rate of fluorescence decay and efficient up-conversion of triplet excitons into singlet excited states, leading to both photoluminescence and internal electroluminescence quantum yields of nearly 100%. PMID:25485987

  19. Highly efficient blue electroluminescence based on thermally activated delayed fluorescence

    NASA Astrophysics Data System (ADS)

    Hirata, Shuzo; Sakai, Yumi; Masui, Kensuke; Tanaka, Hiroyuki; Lee, Sae Youn; Nomura, Hiroko; Nakamura, Nozomi; Yasumatsu, Mao; Nakanotani, Hajime; Zhang, Qisheng; Shizu, Katsuyuki; Miyazaki, Hiroshi; Adachi, Chihaya

    2015-03-01

    Organic compounds that exhibit highly efficient, stable blue emission are required to realize inexpensive organic light-emitting diodes for future displays and lighting applications. Here, we define the design rules for increasing the electroluminescence efficiency of blue-emitting organic molecules that exhibit thermally activated delayed fluorescence. We show that a large delocalization of the highest occupied molecular orbital and lowest unoccupied molecular orbital in these charge-transfer compounds enhances the rate of radiative decay considerably by inducing a large oscillator strength even when there is a small overlap between the two wavefunctions. A compound based on our design principles exhibited a high rate of fluorescence decay and efficient up-conversion of triplet excitons into singlet excited states, leading to both photoluminescence and internal electroluminescence quantum yields of nearly 100%.

  20. Stand-off detection and classification of CBRNe using a Lidar system based on a high power femtosecond laser

    NASA Astrophysics Data System (ADS)

    Izawa, Jun; Yokozawa, Takeshi; Kurata, Takao; Yoshida, Akihiro; Mastunaga, Yasushi; Somekawa, Toshihiro; Eto, Shuzo; Manago, Naohiro; Horisawa, Hideyuki; Yamaguchi, Shigeru; Fujii, Takashi; Kuze, Hiroaki

    2014-10-01

    We propose a stand-off system that enables detection and classification of CBRNe (Chemical, Biological, Radioactive, Nuclear aerosol and explosive solids). The system is an integrated lidar using a high-power (terawatt) femtosecond laser. The detection and classification of various hazardous targets with stand-off distances from several hundred meters to a few kilometers are achieved by means of laser-induced breakdown spectroscopy (LIBS) and two-photon fluorescence (TPF) techniques. In this work, we report on the technical considerations on the system design of the present hybrid lidar system consisting of a nanosecond laser and a femtosecond laser. Also, we describe the current progress in our laboratory experiments that have demonstrated the stand-off detection and classification of various simulants. For the R and N detection scheme, cesium chloride aerosols have successfully been detected by LIBS using a high-power femtosecond laser. For the B detection scheme, TPF signals of organic aerosols such as riboflavin have clearly been recorded. In addition, a compact femtosecond laser has been employed for the LIBS classification of organic plastics employed as e-simulants.