Field trial of differential-phase-shift quantum key distribution using polarization independent frequency up-conversion detectors.

PubMed

Honjo, T; Yamamoto, S; Yamamoto, T; Kamada, H; Nishida, Y; Tadanaga, O; Asobe, M; Inoue, K

2007-11-26

We report a field trial of differential phase shift quantum key distribution (QKD) using polarization independent frequency up-conversion detectors. A frequency up-conversion detector is a promising device for achieving a high key generation rate when combined with a high clock rate QKD system. However, its polarization dependence prevents it from being applied to practical QKD systems. In this paper, we employ a modified polarization diversity configuration to eliminate the polarization dependence. Applying this method, we performed a long-term stability test using a 17.6-km installed fiber. We successfully demonstrated stable operation for 6 hours and achieved a sifted key generation rate of 120 kbps and an average quantum bit error rate of 3.14 %. The sifted key generation rate was not the estimated value but the effective value, which means that the sifted key was continuously generated at a rate of 120 kbps for 6 hours.

Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications

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

Wu, Xiang; Zhang, Yuanwei; Takle, Kendra

2016-01-26

Near Infrared (NIR) dye-sensitized upconversion nanoparticles (UCNPs) have recently been proposed in order to broaden the absorption range and to boost upconversion efficiency. However, implementing this strategy has been limited only to bare core UCNP structures that are faintly luminescent. Herein, we report on an approach to achieve significantly enhanced upconversion luminescence in dye-sensitized core-active shell UCNPs with a broadened absorption range via the doping of ytterbium ions in the UCNP shell in order to bridge the energy transfer from the dye to the UCNP core. As a result, we have been able to synergize the two most practical upconversionmore » booster effectors (dye-sensitizing and core/shell enhancement). The absolute quantum yield of our dye-sensitized core/active shell UCNPs at 800 nm was determined to be ~6% at 2 W/cm2, about 33 times larger than the highest value reported to date for existing 800 nm excitable UCNPs. Moreover, for the first time, by using dye-sensitized core/active shell UCNP embedded poly(methyl methacrylate) polymer implantable systems, we successfully shifted the optogenetic neuron excitation window to a wavelength that is compatible with deep tissue penetrable near the infrared wavelength at 800 nm. Finally, amphiphilic triblock copolymer, Pluronic F127 coatings permit the transfer of hydrophobic UCNPs into water, resulting in water-soluble nanoparticles with well-preserved optical property in aqueous solution. We believe that this research offers a new solution to enhance upconversion efficiency for photonic and biophotonic purposes and opens up new opportunities to use UCNPs as a NIR relay for optogenetic applications.« less

Distance-dependent plasmon-enhanced fluorescence of upconversion nanoparticles using polyelectrolyte multilayers as tunable spacers.

PubMed

Feng, Ai Ling; You, Min Li; Tian, Limei; Singamaneni, Srikanth; Liu, Ming; Duan, Zhenfeng; Lu, Tian Jian; Xu, Feng; Lin, Min

2015-01-14

Lanthanide-doped upconversion nanoparticles (UCNPs) have attracted widespread interests in bioapplications due to their unique optical properties by converting near infrared excitation to visible emission. However, relatively low quantum yield prompts a need for developing methods for fluorescence enhancement. Plasmon nanostructures are known to efficiently enhance fluorescence of the surrounding fluorophores by acting as nanoantennae to focus electric field into nano-volume. Here, we reported a novel plasmon-enhanced fluorescence system in which the distance between UCNPs and nanoantennae (gold nanorods, AuNRs) was precisely tuned by using layer-by-layer assembled polyelectrolyte multilayers as spacers. By modulating the aspect ratio of AuNRs, localized surface plasmon resonance (LSPR) wavelength at 980 nm was obtained, matching the native excitation of UCNPs resulting in maximum enhancement of 22.6-fold with 8 nm spacer thickness. These findings provide a unique platform for exploring hybrid nanostructures composed of UCNPs and plasmonic nanostructures in bioimaging applications.

Photon up-conversion increases biomass yield in Chlorella vulgaris.

PubMed

Menon, Kavya R; Jose, Steffi; Suraishkumar, Gadi K

2014-12-01

Photon up-conversion, a process whereby lower energy radiations are converted to higher energy levels via the use of appropriate phosphor systems, was employed as a novel strategy for improving microalgal growth and lipid productivity. Photon up-conversion enables the utilization of regions of the solar spectrum, beyond the typical photosynthetically active radiation, that are usually wasted or are damaging to the algae. The effects of up-conversion of red light by two distinct sets of up-conversion phosphors were studied in the model microalgae Chlorella vulgaris. Up-conversion by set 1 phosphors led to a 2.85 fold increase in biomass concentration and a 3.2 fold increase in specific growth rate of the microalgae. While up-conversion by set 2 phosphors resulted in a 30% increase in biomass and 12% increase in specific intracellular neutral lipid, while the specific growth rates were comparable to that of the control. Furthermore, up-conversion resulted in higher levels of specific intracellular reactive oxygen species in C. vulgaris. Up-conversion of red light (654 nm) was shown to improve biomass yields in C. vulgaris. In principle, up-conversion can be used to increase the utilization range of the electromagnetic spectrum for improved cultivation of photosynthetic systems such as plants, algae, and microalgae. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

NASA Astrophysics Data System (ADS)

Singh, Amit T.

2018-05-01

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

Development of Phase-Stable Photon Upconverters for Efficient Solar Energy Utilization

NASA Astrophysics Data System (ADS)

Murakami, Yoichi

Photon upconversion based on triplet-triplet annihilation (TTA) of excited triplet molecules is drawing attention due to its applicability for weak incident light, possessing a potential for improving efficiencies of solar energy conversion devices. Since energy transfer between triplet levels of different molecules and TTA are based on the Dexter mechanism, inter-molecular collision is necessary and hence the majority of previous studies have been done with organic solvents, which are volatile and flammable. This paper presents the development and characterization of phase-stable photon upconverters fabricated with ionic liquids, which are room temperature molten salts with negligible vapor pressure and high thermal stability. The employed aromatic molecules, which are carrier of photo-created energies and are non-polar (or weakly polar) molecules, are found to be stable in the polar environment of ionic liquids, contrary to expectation. The mechanism of the stable solvation is proposed. The upconversion quantum yields are found to rapidly saturate as the excitation light power increases. An analytical model was developed and compared with the experimental data. It is shown that ionic liquids are not viscous media for the purpose of TTA-based upconversion.

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

DOE PAGES

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

2016-11-29

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

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

PubMed

Rafiq, Shahnawaz; Sen, Pratik

2013-02-28

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.

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.

100 km differential phase shift quantum key distribution experiment with low jitter up-conversion detectors

NASA Astrophysics Data System (ADS)

Diamanti, Eleni; Takesue, Hiroki; Langrock, Carsten; Fejer, M. M.; Yamamoto, Yoshihisa

2006-12-01

We present a quantum key distribution experiment in which keys that were secure against all individual eavesdropping attacks allowed by quantum mechanics were distributed over 100 km of optical fiber. We implemented the differential phase shift quantum key distribution protocol and used low timing jitter 1.55 µm single-photon detectors based on frequency up-conversion in periodically poled lithium niobate waveguides and silicon avalanche photodiodes. Based on the security analysis of the protocol against general individual attacks, we generated secure keys at a practical rate of 166 bit/s over 100 km of fiber. The use of the low jitter detectors also increased the sifted key generation rate to 2 Mbit/s over 10 km of fiber.

Photon upconversion using InAs-based quantum structures and the control of intermediate states (Conference Presentation)

NASA Astrophysics Data System (ADS)

Kamiya, Itaru; Tex, David M.; Zhang, Yuwei; Kanemitsu, Yoshihiko

2017-04-01

We have reported that a novel quantum structure which we term quantum well island (QWI), a few monolayer thick and sub-micron wide structure, is effective in confining the carriers and enhancing multi-exciton interactions. By embedding InAs-based QWIs in AlGaAs barrier layers, we demonstrated that upconverted photoluminescence (PL) in the visible regime can be obtained by impinging near infrared (IR) photons, which may potentially be applied for intermediate band (IB) solar cells [1]. Further investigation has revealed that the dominant upconversion mechanism is most likely Auger, while two-step excitation may also take place under selected conditions [2]. The upconverted carriers generated by IR irradiation may also be detected as photocurrents. Through a series of studies using this structure, we note the importance of the carrier trapping involved during the upconversion processes. For instance, multiple laser-beam excitation measurements have shown that trapping and re-trapping processes reduce the photocurrents [3]. However, recently, using a structure that consists of InAs quantum dots embedded in InAs/GaAs multi-quantum wells (MQWs), we find that efficient carrier trapping can enhance upconverted PL [4]. We show the preparation and the control of this structure by molecular beam epitaxy (MBE), and the possible mechanisms of the upconversion. We also discuss how the conversion efficiency may be improved using device structures based on this concept. [1] D. M. Tex and I. Kamiya, Phys. Rev. B 83 (2011) 081309. [2] D. M. Tex, I. Kamiya, and Y. Kanemitsu, Sci. Rep. 4 (2014) 4125. [3] D. M. Tex, T. Ihara, I. Kamiya, and Y. Kanemitsu, to be published. [4] Y. Zhang and I. Kamiya, JSAP Spring Meeting, 2016.

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

NASA Astrophysics Data System (ADS)

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

2011-10-01

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

Cooperative and non-cooperative sensitization upconversion in lanthanide-doped LiYbF4 nanoparticles.

PubMed

Zou, Qilin; Huang, Ping; Zheng, Wei; You, Wenwu; Li, Renfu; Tu, Datao; Xu, Jin; Chen, Xueyuan

2017-05-18

Lanthanide (Ln 3+ )-doped upconversion nanoparticles (UCNPs) have attracted tremendous interest owing to their potential bioapplications. However, the intrinsic photophysics responsible for upconversion (UC) especially the cooperative sensitization UC (CSU) in colloidal Ln 3+ -doped UCNPs has remained untouched so far. Herein, we report a unique strategy for the synthesis of high-quality LiYbF 4 :Ln 3+ core-only and core/shell UCNPs with tunable particle sizes and shell thicknesses. Energy transfer UC from Er 3+ , Ho 3+ and Tm 3+ and CSU from Tb 3+ were comprehensively surveyed under 980 nm excitation. Through surface passivation, we achieved efficient non-cooperative sensitization UC with absolute UC quantum yields (QYs) of 3.36%, 0.69% and 0.81% for Er 3+ , Ho 3+ and Tm 3+ , respectively. Particularly, we for the first time quantitatively determined the CSU efficiency for Tb 3+ with an absolute QY of 0.0085% under excitation at a power density of 70 W cm -2 . By means of temperature-dependent steady-state and transient UC spectroscopy, we unraveled the dominant mechanisms of phonon-assisted cooperative energy transfer (T > 100 K) and sequential dimer ground-state absorption/excited-state absorption (T < 100 K) for the CSU process in LiYbF 4 :Tb 3+ UCNPs.

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

Triplet-sensitized photon upconversion in deep eutectic solvents.

PubMed

Murakami, Yoichi; Das, Sudhir Kumar; Himuro, Yuki; Maeda, Satoshi

2017-11-22

Photon upconversion (UC) is a technology that can increase solar utilization efficiencies in broad photoenergy conversion systems by converting lower-energy photons into usable higher-energy photons. Recently, UC using triplet-triplet annihilation (TTA) of organic molecules has drawn attention because it is presently the only method applicable to weak and noncoherent light. To date, many attempts have been made to realize this UC technology in forms suitable for applications, but they typically suffer from either high cost or insufficient stability and/or safety of materials. Recently, a new class of liquid called deep eutectic solvents (DESs) has emerged as low-cost green fluids that possess low toxicity and vapor pressure, biodegradability, and high thermal stability. DESs have been proposed as an alternative to ionic liquids. This article develops triplet-sensitized UC samples using DESs that are found to be suitable solvents for this purpose, attaining a new materials platform for UC with the aforementioned advantages. The high thermal stability of the samples is qualitatively confirmed and their UC quantum yields are determined to be 0.11-0.21 (based on the definition that the maximum quantum yield is 0.5) depending on the DES composition. The triplet lifetime of the emitter 9,10-diphenylanthracene increases with DES viscosity, resulting in unique kinetics. Analysis of photophysical experimental results allows the relevant physics governing the performance of this sample system to be determined and discussed. Overall, a novel UC platform that simultaneously achieves high thermal stability, low cost, and environmental friendliness is developed using DESs as the solvent.

Distance-Dependent Plasmon-Enhanced Fluorescence of Upconversion Nanoparticles using Polyelectrolyte Multilayers as Tunable Spacers

PubMed Central

Feng, Ai Ling; You, Min Li; Tian, Limei; Singamaneni, Srikanth; Liu, Ming; Duan, Zhenfeng; Lu, Tian Jian; Xu, Feng; Lin, Min

2015-01-01

Lanthanide-doped upconversion nanoparticles (UCNPs) have attracted widespread interests in bioapplications due to their unique optical properties by converting near infrared excitation to visible emission. However, relatively low quantum yield prompts a need for developing methods for fluorescence enhancement. Plasmon nanostructures are known to efficiently enhance fluorescence of the surrounding fluorophores by acting as nanoantennae to focus electric field into nano-volume. Here, we reported a novel plasmon-enhanced fluorescence system in which the distance between UCNPs and nanoantennae (gold nanorods, AuNRs) was precisely tuned by using layer-by-layer assembled polyelectrolyte multilayers as spacers. By modulating the aspect ratio of AuNRs, localized surface plasmon resonance (LSPR) wavelength at 980 nm was obtained, matching the native excitation of UCNPs resulting in maximum enhancement of 22.6-fold with 8 nm spacer thickness. These findings provide a unique platform for exploring hybrid nanostructures composed of UCNPs and plasmonic nanostructures in bioimaging applications. PMID:25586238

Ping-Pong Energy Transfer in a Boron Dipyrromethane Containing Pt(II)-Schiff Base Complex: Synthesis, Photophysical Studies, and Anti-Stokes Shift Increase in Triplet-Triplet Annihilation Upconversion.

PubMed

Razi, Syed S; Koo, Yun Hee; Kim, Woojae; Yang, Wenbo; Wang, Zhijia; Gobeze, Habtom; D'Souza, Francis; Zhao, Jianzhang; Kim, Dongho

2018-05-07

A boron dipyrromethane (BDP)-containing Pt(II)-Schiff base complex (Pt-BDP), showing ping-pong singlet-triplet energy transfer, was synthesized, and the detailed photophysical properties were investigated using various steady-state and time-resolved transient spectroscopies. Femtosecond/nanosecond transient absorption spectroscopies demonstrated that, upon selective excitation of the BDP unit in Pt-BDP at 490 nm, Förster resonance energy transfer from the BDP unit to the Pt(II) coordination center occurred (6.7 ps), accompanied by an ultrafast intersystem crossing at the Pt(II) coordination center (<1 ps) and triplet-triplet energy transfer back to the BDP moiety (148 ps). These processes generated a triplet state localized at BDP, and the lifetime was 103.2 μs, much longer than the triplet-state lifetime of Pt-Ph (3.5 μs), a complex without the BDP moiety. Finally, Pt-BDP was used as a triplet photosensitizer for triplet-triplet annihilation (TTA) upconversion through selective excitation of the BDP unit or the Pt(II) coordination center at lower excitation energy. An upconversion quantum yield of up to 10% was observed with selective excitation of the BDP moiety, and a large anti-Stokes shift of 0.65 eV was observed upon excitation of the lower-energy band of the Pt(II) coordination center. We propose that using triplet photosensitizers with the ping-pong energy-transfer process may become a useful method for increasing the anti-Stokes shift of TTA upconversion.

Red-light-controllable liquid-crystal soft actuators via low-power excited upconversion based on triplet-triplet annihilation.

PubMed

Jiang, Zhen; Xu, Ming; Li, Fuyou; Yu, Yanlei

2013-11-06

A red-light-controllable soft actuator has been achieved, driven by low-power excited triplet-triplet annihilation-based upconversion luminescence (TTA-UCL). First, a red-to-blue TTA-based upconversion system with a high absolute quantum yield of 9.3 ± 0.5% was prepared by utilizing platinum(II) tetraphenyltetrabenzoporphyrin (PtTPBP) as the sensitizer and 9,10-bis(diphenylphosphoryl)anthracene (BDPPA) as the annihilator. In order to be employed as a highly effective phototrigger of photodeformable cross-linked liquid-crystal polymers (CLCPs), the PtTPBP&BDPPA system was incorporated into a rubbery polyurethane film and then assembled with an azotolane-containing CLCP film. The generating assembly film bent toward the light source when irradiated with a 635 nm laser at low power density of 200 mW cm(-2) because the TTA-UCL was effectively utilized by the azotolane moieties in the CLCP film, inducing their trans-cis photoisomerization and an alignment change of the mesogens via an emission-reabsorption process. It is the first example of a soft actuator in which the TTA-UCL is trapped and utilized to create photomechanical effect. Such advantages of using this novel red-light-controllable soft actuator in potential biological applications have also been demonstrated as negligible thermal effect and its excellent penetration ability into tissues. This work not only provides a novel photomanipulated soft actuation material system based on the TTA-UCL technology but also introduces a new technological application of the TTA-based upconversion system in photonic devices.

A highly sensitive biosensing platform based on upconversion nanoparticles and graphene quantum dots for the detection of Ag+

NASA Astrophysics Data System (ADS)

He, Lu; Yang, Lin; Zhu, Hao; Dong, Wenkui; Ding, Yujie; Zhu, Jun-Jie

2017-06-01

A novel luminescence ‘Turn-On’ nanoplatform for the sensitive sensing of Ag+ was fabricated based on luminescence resonance energy transfer technique between sodium citrate functionalized upconversion nanoparticles (Cit-UCNPs, energy donor) and graphene quantum dots (GQDs, energy acceptor). Amino-labeled single-stranded DNA (NH2-ssDNA) containing a number of cytosine (C) was conjugated on the surface of the Cit-UCNPs to capture Ag+ ions. Due to the π-π stacking interaction between NH2-ssDNA and GQDs, the upconversion luminescence can be quenched. However, upon the addition of Ag+, the π-π stacking interaction weakens due to the formation of the hairpin structure of C-Ag+-C on the UCNPs. As a result, GQDs will leave the surface of the UCNPs and the upconversion luminescence can be enhanced (Turn-On). Based on this fact, the sensor was developed for the detection of Ag+ with a linear concentration range from 2 × 10-4 to 1 μM and a detection limit as low as 60 pM. The assay method is fairly simple with high selectivity and sensitivity, which can be used for the determination of Ag+ in environmental water samples.

Enhancing Solar Cell Efficiency Using Photon Upconversion Materials

PubMed Central

Shang, Yunfei; Hao, Shuwei; Yang, Chunhui; Chen, Guanying

2015-01-01

Photovoltaic cells are able to convert sunlight into electricity, providing enough of the most abundant and cleanest energy to cover our energy needs. However, the efficiency of current photovoltaics is significantly impeded by the transmission loss of sub-band-gap photons. Photon upconversion is a promising route to circumvent this problem by converting these transmitted sub-band-gap photons into above-band-gap light, where solar cells typically have high quantum efficiency. Here, we summarize recent progress on varying types of efficient upconversion materials as well as their outstanding uses in a series of solar cells, including silicon solar cells (crystalline and amorphous), gallium arsenide (GaAs) solar cells, dye-sensitized solar cells, and other types of solar cells. The challenge and prospect of upconversion materials for photovoltaic applications are also discussed. PMID:28347095

Direct Generation and Detection of Quantum Correlated Photons with 3.2 um Wavelength Spacing.

PubMed

Sua, Yong Meng; Fan, Heng; Shahverdi, Amin; Chen, Jia-Yang; Huang, Yu-Ping

2017-12-13

Quantum correlated, highly non-degenerate photons can be used to synthesize disparate quantum nodes and link quantum processing over incompatible wavelengths, thereby constructing heterogeneous quantum systems for otherwise unattainable superior performance. Existing techniques for correlated photons have been concentrated in the visible and near-IR domains, with the photon pairs residing within one micron. Here, we demonstrate direct generation and detection of high-purity photon pairs at room temperature with 3.2 um wavelength spacing, one at 780 nm to match the rubidium D2 line, and the other at 3950 nm that falls in a transparent, low-scattering optical window for free space applications. The pairs are created via spontaneous parametric downconversion in a lithium niobate waveguide with specially designed geometry and periodic poling. The 780 nm photons are measured with a silicon avalanche photodiode, and the 3950 nm photons are measured with an upconversion photon detector using a similar waveguide, which attains 34% internal conversion efficiency. Quantum correlation measurement yields a high coincidence-to-accidental ratio of 54, which indicates the strong correlation with the extremely non-degenerate photon pairs. Our system bridges existing quantum technology to the challenging mid-IR regime, where unprecedented applications are expected in quantum metrology and sensing, quantum communications, medical diagnostics, and so on.

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

PubMed

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

2016-11-09

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

Photon correlation in single-photon frequency upconversion.

PubMed

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

2012-01-30

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

Long wavelength identification of microcalcifications in breast cancer tissue using a quantum cascade laser and upconversion detection

NASA Astrophysics Data System (ADS)

Tseng, Y. P.; Bouzy, P.; Stone, N.; Pedersen, C.; Tidemand-Lichtenberg, P.

2018-02-01

Spectral imaging in the long-wave infrared regime has great potential for medical diagnostics. Breast cancer is the most common cancer amongst females in the US. The pathological features and the occurrence of the microcalcifications are still poorly understood. However, two types of microcalcifications have been identified as unique biomarkers: type I consisting of calcium oxalate (benign lesions) and type II composed of hydroxyapatite (benign or invasive lesions). In this study, we propose a new approach based on vibrational spectroscopy that is non-destructive, label-free and chemically specific for breast cancer detection. Long-wave infrared spectroscopy combining quantum cascade lasers (QCL) and upconversion detection, offer to improve signal-to-noise ratios compared to standard long-wave infrared spectroscopy. We demonstrated long-wave identification of synthetic samples of carbonated hydroxyapatite and of microcalcification in breast cancer tissue using upconversion detection. Absorbance spectra and upconverted images of in situ breast cancer biopsy are compared with that of Fourier-transform infrared (FTIR) spectroscopy.

Ln(3+)-doped nanoparticles for upconversion and magnetic resonance imaging: some critical notes on recent progress and some aspects to be considered.

PubMed

van Veggel, Frank C J M; Dong, Cunhai; Johnson, Noah J J; Pichaandi, Jothirmayanantham

2012-12-07

In this feature article we will critically discuss the synthesis and characterisation aspects of Ln(3+)-doped nanoparticles (NPs) that show upconversion, upon 980 nm excitation. Upconversion is a non-linear process that converts two or more low-energy photons, often near-infrared photons, into one of higher energy, e.g. blue and 800 nm from Tm(3+) and green and red from Er(3+) or Ho(3+). Nearly all researchers use the absorption of 980 nm light by Yb(3+) as the sensitiser for the co-doped emissive Ln(3+) ions. The focus will be on LnF(3) and MLnF(4) (M = alkali metal) as the host matrix, because most progress has been made with these. In particular we will argue that a detailed understanding of how the dopant ions and the host Ln(3+) ions are distributed (in the core) and how (doped) shell growth occurs is not well understood. Moreover, their use as optical and magnetic resonance imaging contrast agents will be discussed. We will argue that deep-tissue imaging beyond 600 μm with retention of optical resolution, i.e. to see fine structure such as blood capillaries in brain tissues, has not yet been achieved. Three key parameters have been identified as impediments: (i) the low absorption efficiency of the Yb(3+) sensitiser, (ii) the low quantum yield of upconversion, and (iii) the long-lived excited states. On the other hand, there are very encouraging results that suggest that these nanoparticles could be developed into very potent magnetic resonance imaging (MRI) contrast agents.

Efficient upconversion polymer-inorganic nanocomposite thin film emitters prepared by the double beam matrix assisted pulsed laser evaporation (DB-MAPLE)

NASA Astrophysics Data System (ADS)

Darwish, Abdalla M.; Burkett, Allan; Blackwell, Ashley; Taylor, Keylantra; Walker, Vernell; Sarkisov, Sergey; Koplitz, Brent

2014-09-01

We report on fabrication and investigation of optical and morphological properties of highly efficient (a quantum yield of 1%) upconversion polymer-inorganic nanocomposite thin film emitters prepared by the new technique of double beam matrix assisted pulsed laser evaporation (DB-MAPLE). Polymer poly(methyl methacrylate) (PMMA) host was evaporated on a silicon substrate using a 1064-nm pulsed laser beam using a target made of frozen (to the temperature of liquid nitrogen) solution of PMMA in chlorobenzene. Concurrently, the second 532-nm pulsed beam from the same laser was used to impregnate the polymer host with the inorganic nanoparticulate made of the rare earth upconversion compounds NaYF4: Yb3+, Er3+, NaYF4: Yb3+, Ho3+, and NaYF4: Yb3+, Tm3+. The compounds were initially synthesized using the wet process, baked, and compressed in solid pellet targets. The proposed DB-MAPLE method has the advantage of making highly homogeneous nanocomposite films with precise control of the doping rate due to the optimized overlapping of the plumes produced by the ablation of the organic and inorganic target with the infrared and visible laser beams respectively. X-ray diffraction, electron and atomic force microscopy, and optical fluorescence spectroscopy indicated that the inorganic nanoparticulate preserved its crystalline structure and upconversion properties (strong emission in green, red, and blue bands upon illumination with 980-nm laser diode) after being transferred from the target in the polymer nanocomposite film. The produced films can be used in applications varying from the efficiency enhancement of the photovoltaic cells, optical sensors and biomarkers to anti-counterfeit labels.

Ln3+-doped nanoparticles for upconversion and magnetic resonance imaging: some critical notes on recent progress and some aspects to be considered

NASA Astrophysics Data System (ADS)

van Veggel, Frank C. J. M.; Dong, Cunhai; Johnson, Noah J. J.; Pichaandi, Jothirmayanantham

2012-11-01

In this feature article we will critically discuss the synthesis and characterisation aspects of Ln3+-doped nanoparticles (NPs) that show upconversion, upon 980 nm excitation. Upconversion is a non-linear process that converts two or more low-energy photons, often near-infrared photons, into one of higher energy, e.g. blue and 800 nm from Tm3+ and green and red from Er3+ or Ho3+. Nearly all researchers use the absorption of 980 nm light by Yb3+ as the sensitiser for the co-doped emissive Ln3+ ions. The focus will be on LnF3 and MLnF4 (M = alkali metal) as the host matrix, because most progress has been made with these. In particular we will argue that a detailed understanding of how the dopant ions and the host Ln3+ ions are distributed (in the core) and how (doped) shell growth occurs is not well understood. Moreover, their use as optical and magnetic resonance imaging contrast agents will be discussed. We will argue that deep-tissue imaging beyond 600 μm with retention of optical resolution, i.e. to see fine structure such as blood capillaries in brain tissues, has not yet been achieved. Three key parameters have been identified as impediments: (i) the low absorption efficiency of the Yb3+ sensitiser, (ii) the low quantum yield of upconversion, and (iii) the long-lived excited states. On the other hand, there are very encouraging results that suggest that these nanoparticles could be developed into very potent magnetic resonance imaging (MRI) contrast agents.

1.5- μm single photon counting using polarization-independent up-conversion detector

NASA Astrophysics Data System (ADS)

Takesue, Hiroki; Diamanti, Eleni; Langrock, Carsten; Fejer, M. M.; Yamamoto, Yoshihisa

2006-12-01

We report a 1.5- μm band polarization independent single photon detector based on frequency up-conversion in periodically poled lithium niobate (PPLN) waveguides. To overcome the polarization dependence of the PPLN waveguides, we employed a polarization diversity configuration composed of two up-conversion detectors connected with a polarization beam splitter. We experimentally confirmed polarization independent single photon counting using our detector. We undertook a proof-of-principle differential phase shift quantum key distribution experiment using the detector, and confirmed that the sifted key rate and error rate remained stable when the polarization state was changed during single photon transmission.

Fast and long-range triplet exciton diffusion in metal-organic frameworks for photon upconversion at ultralow excitation power.

PubMed

Mahato, Prasenjit; Monguzzi, Angelo; Yanai, Nobuhiro; Yamada, Teppei; Kimizuka, Nobuo

2015-09-01

The conversion of low-energy light into photons of higher energy based on sensitized triplet-triplet annihilation upconversion (TTA-UC) has emerged as a promising wavelength-shifting methodology because it permits UC at excitation powers as low as the solar irradiance. However, its application has been significantly hampered by the slow diffusion of excited molecules in solid matrices. Here, we introduce metal-organic frameworks (MOFs) that promote TTA-UC by taking advantage of triplet exciton migration among fluorophores that are regularly aligned with spatially controlled chromophore orientations. We synthesized anthracene-containing MOFs with different molecular orientations, and the analysis of TTA-UC emission kinetics unveiled a high triplet diffusion rate with a micrometre-scale diffusion length. Surface modification of MOF nanocrystals with donor molecules and their encapsulation in glassy poly(methyl methacrylate) (PMMA) allowed the construction of molecular-diffusion-free solid-state upconverters, which lead to an unprecedented maximization of overall UC quantum yield at excitation powers comparable to or well below the solar irradiance.

Energy Pooling Upconversion in Free Space and Optical Cavities

NASA Astrophysics Data System (ADS)

LaCount, Michael D.

The ability to efficiently convert the wavelength of light has value in a wide range of disciplines that include the fields of photovoltaics, plant growth, optics and medicine. The processes by which such transformations are carried out are known as upconversions and downconversions. There are several ways to up/down convert light, each with its own attributes, issues, and competing mechanisms. Most are associated with one-body or two-body processes. Three-body dynamics are also possible though, going by the names of quantum cutting (downconversion) and energy pooling (upconversion). These use virtual excited electronic states to mediate conversions as has been experimentally realized using lanthanide ions embedded in wide bandgap materials. The use of lanthanides to convert light is not ideal due to their relative scarcity, toxicity, and the limited range of light frequencies that can be absorbed and emitted. Organic molecules, on the other hand, are typically non-toxic, are made up of abundant elements, and can be designed with tailored spectral properties. At issue is whether or not they can be used to carry out efficient energy pooling, the central question to be answered in this thesis. The research presented here draws on a perturbative quantum electrodynamics framework previously established for generic energy pooling. It was used to develop a computational methodology for determining the rate of energy pooling and its competing processes. This, in turn, draws on a combination of time-dependent density functional theory, quantum electrodynamics, and perturbation theory to generate the requisite material property data. This computational model was applied to two test systems consisting of stilbene-fluorescein and hexabenzocoronene-oligothiophene. The stilbene-fluorescein system was found to have a maximum energy pooling rate efficiency (as compared to competing processes) of 17% and the hexabenzocoronene-oligothiophene system was found to have a maximum energy pooling rate efficiency of 99%. This demonstrates that the energy pooling rate can be made faster than its competing processes. Based on the results of this study, a set of design rules was developed to optimize the rate efficiency of energy pooling. Prior to this research, no attempt had been made to determine if energy pooling could be made to out-pace competing processes--i.e. whether or not a molecular system could be designed to utilize energy pooling as an efficient means of upconversion. This initial investigation was part of a larger effort involving a team of researchers at the University of Colorado, Boulder and at the National Renewable Energy Laboratory. After establishing our computational proof-of-concept, we collectively used the new design rules to select an improved system for energy pooling. This consisted of rhodamine 6G and stilbene-420. These molecules were fabricated into a thin film, and the maximum internal quantum yield was measured to be 36% under sufficiently high intensity light. To further increase the efficiency of energy pooling, encapsulation within optical cavities was considered as a way of changing the rate of processes characterized by electric dipole-dipole coupling. This was carried out using a combination of classical electromagnetism, quantum electrodynamics, and perturbation theory. It was found that, in the near field, if the distance of the energy transfer is smaller than the distance from the energy transfer site and the cavity wall, then the electric dipole-dipole coupling tensor is not influenced by the cavity environment and the rates of energy transfer processes are the same as those in free space. Any increase in energy transfer efficiencies that are experimentally measured must therefore be caused by changing the rate of light absorption and emission. This is an important finding because earlier, less rigorous studies had concluded otherwise. It has been previously demonstrated that an optical cavity can be used to inhibit the spontaneous emission of atoms or molecules placed within it. This too was examined as a possible means of increasing energy pooling efficiency. Using first-principles methods, quantum electrodynamics, perturbation theory, and a kinetic model, the efficiency of energy pooling upconversion within a tuned rectangular cavity was found to be significantly larger than in free space. A model system with a free-space energy pooling upconversion efficiency of 23% was found to increase to 47% when placed in a tuned rectangular cavity.

Organic photochemical storage of solar energy. Progress report, February 1, 1979-January 31, 1980

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

Jones, G. II

1980-02-01

Study of valence isomerization of organic compounds has focused on two mechanisms of photosensitization involving either electron donor-acceptor interaction or energy transfer. The quenching of fluorescent sensitizers by isomerizable substrates results in the formation of excited complexes. These sensitizer-substrate pairs are highly polarized, leading to changes in bond order for the substrates. For several substrates such as quadricyclene, hexamethyldewarbenzene, and a nonbornadiene derivative, this perturbation results in efficient valence isomerization. Isomerization observed on irradiation of charge transfer complexes of isomerizable substrates is consistent with a similar exciplex - template mechanism. The energy transfer mechanism of photosensitization has been studied bymore » measuring the temperature dependence of quantum yield for isomerization of dimethyl norbornadiene-2,3-dicarboxylate sensitized by benzanthrone. From temperature and quencher concentration profiles quenching constants have been obtained which are consistent with an endoergic triplet energy transfer mechanism. The thermal upconversion of the low energy triplet of benzanthrone results in a threefold increase in isomerization quantum yield over a 90/sup 0/ temperature range.« less

All-inorganic colloidal upconversion quantum dots (Conference Presentation)

NASA Astrophysics Data System (ADS)

Oron, Dan; Teitelboim, Ayelet

2017-02-01

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

Quantum frequency up-conversion of continuous variable entangled states

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

Liu, Wenyuan; Wang, Ning; Li, Zongyang

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 pumpmore » field, making it a practical building block for quantum information processing and communication networks.« less

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.

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

Delivery and reveal of localization of upconversion luminescent microparticles and quantum dots in the skin in vivo by fractional laser microablation, multimodal imaging, and optical clearing

NASA Astrophysics Data System (ADS)

Volkova, Elena K.; Yanina, Irina Yu; Genina, Elina A.; Bashkatov, Alexey N.; Konyukhova, Julia G.; Popov, Alexey P.; Speranskaya, Elena S.; Bucharskaya, Alla B.; Navolokin, Nikita A.; Goryacheva, Irina Yu.; Kochubey, Vyacheslav I.; Sukhorukov, Gleb B.; Meglinski, Igor V.; Tuchin, Valery V.

2018-02-01

Delivery and spatial localization of upconversion luminescent microparticles [Y2O3:Yb, Er] (mean size ˜1.6 μm) and quantum dots (QDs) (CuInS2/ZnS nanoparticles coated with polyethylene glycol-based amphiphilic polymer, mean size ˜20 nm) inside rat skin was studied in vivo using a multimodal optical imaging approach. The particles were embedded into the skin dermis to the depth from 300 to 500 μm through microchannels performed by fractional laser microablation. Low-frequency ultrasound was applied to enhance penetration of the particles into the skin. Visualization of the particles was revealed using a combination of luminescent spectroscopy, optical coherence tomography, confocal microscopy, and histochemical analysis. Optical clearing was used to enhance the image contrast of the luminescent signal from the particles. It was demonstrated that the penetration depth of particles depends on their size, resulting in a different detection time interval (days) of the luminescent signal from microparticles and QDs inside the rat skin in vivo. We show that luminescent signal from the upconversion microparticles and QDs was detected after the particle delivery into the rat skin in vivo during eighth and fourth days, respectively. We hypothesize that the upconversion microparticles have created a long-time depot localized in the laser-created channels, as the QDs spread over the surrounding tissues.

Two-step photon up-conversion solar cells

PubMed Central

Asahi, Shigeo; Teranishi, Haruyuki; Kusaki, Kazuki; Kaizu, Toshiyuki; Kita, Takashi

2017-01-01

Reducing the transmission loss for below-gap photons is a straightforward way to break the limit of the energy-conversion efficiency of solar cells (SCs). The up-conversion of below-gap photons is very promising for generating additional photocurrent. Here we propose a two-step photon up-conversion SC with a hetero-interface comprising different bandgaps of Al0.3Ga0.7As and GaAs. The below-gap photons for Al0.3Ga0.7As excite GaAs and generate electrons at the hetero-interface. The accumulated electrons at the hetero-interface are pumped upwards into the Al0.3Ga0.7As barrier by below-gap photons for GaAs. Efficient two-step photon up-conversion is achieved by introducing InAs quantum dots at the hetero-interface. We observe not only a dramatic increase in the additional photocurrent, which exceeds the reported values by approximately two orders of magnitude, but also an increase in the photovoltage. These results suggest that the two-step photon up-conversion SC has a high potential for implementation in the next-generation high-efficiency SCs. PMID:28382945

Spectral evidence for multi-pathway contribution to the upconversion pathway in NaYF4:Yb3+,Er3+ phosphors.

PubMed

Cho, Youngho; Song, Si Won; Lim, Soo Yeong; Kim, Jae Hun; Park, Chan Ryang; Kim, Hyung Min

2017-03-08

Although upconversion phosphors have been widely used in nanomedicine, laser engineering, bioimaging, and solar cell technology, the upconversion luminescence mechanism of the phosphors has been fiercely debated. A comprehensive understanding of upconversion photophysics has been significantly impeded because the number of photons incorporated in the process in different competitive pathways could not be resolved. Few convincing results to estimate the contribution of each of the two-, three-, and four-photon channels of near-infrared (NIR) energy have been reported in yielding upconverted visible luminescence. In this study, we present the energy upconversion process occurring in NaYF 4 :Yb 3+ ,Er 3+ phosphors as a function of excitation frequency and power density. We investigated the upconversion mechanism of lanthanide phosphors by comparing UV/VIS one-photon excitation spectra and NIR multi-photon spectra. A detailed analysis of minor transitions in one-photon spectra and luminescence decay enables us to assign electronic origins of individual bands in multi-photon upconversion luminescence and provides characteristic transitions representing the corresponding upconversion channel. Furthermore, we estimated the quantitative contribution of multiple channels with respect to irradiation power and excitation energy.

Integrated four-channel all-fiber up-conversion single-photon-detector with adjustable efficiency and dark count.

PubMed

Zheng, Ming-Yang; Shentu, Guo-Liang; Ma, Fei; Zhou, Fei; Zhang, Hai-Ting; Dai, Yun-Qi; Xie, Xiuping; Zhang, Qiang; Pan, Jian-Wei

2016-09-01

Up-conversion single photon detector (UCSPD) has been widely used in many research fields including quantum key distribution, lidar, optical time domain reflectrometry, and deep space communication. For the first time in laboratory, we have developed an integrated four-channel all-fiber UCSPD which can work in both free-running and gate modes. This compact module can satisfy different experimental demands with adjustable detection efficiency and dark count. We have characterized the key parameters of the UCSPD system.

Donor-Acceptor-Collector Ternary Crystalline Films for Efficient Solid-State Photon Upconversion.

PubMed

Ogawa, Taku; Hosoyamada, Masanori; Yurash, Brett; Nguyen, Thuc-Quyen; Yanai, Nobuhiro; Kimizuka, Nobuo

2018-06-25

It is pivotal to achieve efficient triplet-triplet annihilation based photon upconversion (TTA-UC) in the solid-state for enhancing potentials of renewable energy production devices. However, the UC efficiency of solid materials is largely limited by low fluorescence quantum yields that originate from the aggregation of TTA-UC chromophores, and also by severe back energy transfer from the acceptor singlet state to the singlet state of the triplet donor in the condensed state. In this work, to overcome these issues, we introduce a highly fluorescent singlet energy collector as the third component of donor-doped acceptor crystalline films, in which dual energy migration, i.e., triplet energy migration for TTA-UC and succeeding singlet energy migration for transferring energy to a collector, takes place. To demonstrate this scheme, a highly fluorescent singlet energy collector was added as the third component of donor-doped acceptor crystalline films. An anthracene-based acceptor containing alkyl chains and a carboxylic moiety is mixed with the triplet donor Pt(II) octaethylporphyrin (PtOEP) and the energy collector 2,5,8,11-tetra- tert-butylperylene (TTBP) in solution, and spin-coating of the mixed solution gives acceptor films of nanofibrous crystals homogeneously doped with PtOEP and TTBP. Interestingly, delocalized singlet excitons in acceptor crystals are found to diffuse effectively over the distance of ~37 nm. Thanks to this high diffusivity, only 0.5 mol% of doped TTBP can harvest most of the singlet excitons, which successfully doubles the solid-state fluorescent quantum yield of acceptor/TTBP blend films to 76%. Furthermore, since the donor PtOEP and the collector TTBP are separately isolated in the nanofibrous acceptor crystals, the singlet back energy transfer from the collector to the donor is effectively avoided. Such efficient singlet energy collection and inhibited back energy transfer processes result in a large increase of UC efficiency up to 9.0%, offering rational design principles towards ultimately efficient solid-state upconverters.

Delivery and reveal of localization of upconversion luminescent microparticles and quantum dots in the skin in vivo by fractional laser microablation, multimodal imaging, and optical clearing.

PubMed

Volkova, Elena K; Yanina, Irina Yu; Genina, Elina A; Bashkatov, Alexey N; Konyukhova, Julia G; Popov, Alexey P; Speranskaya, Elena S; Bucharskaya, Alla B; Navolokin, Nikita A; Goryacheva, Irina Yu; Kochubey, Vyacheslav I; Sukhorukov, Gleb B; Meglinski, Igor V; Tuchin, Valery V

2018-02-01

Delivery and spatial localization of upconversion luminescent microparticles [Y2O3:Yb, Er] (mean size ∼1.6  μm) and quantum dots (QDs) (CuInS2/ZnS nanoparticles coated with polyethylene glycol-based amphiphilic polymer, mean size ∼20  nm) inside rat skin was studied in vivo using a multimodal optical imaging approach. The particles were embedded into the skin dermis to the depth from 300 to 500  μm through microchannels performed by fractional laser microablation. Low-frequency ultrasound was applied to enhance penetration of the particles into the skin. Visualization of the particles was revealed using a combination of luminescent spectroscopy, optical coherence tomography, confocal microscopy, and histochemical analysis. Optical clearing was used to enhance the image contrast of the luminescent signal from the particles. It was demonstrated that the penetration depth of particles depends on their size, resulting in a different detection time interval (days) of the luminescent signal from microparticles and QDs inside the rat skin in vivo. We show that luminescent signal from the upconversion microparticles and QDs was detected after the particle delivery into the rat skin in vivo during eighth and fourth days, respectively. We hypothesize that the upconversion microparticles have created a long-time depot localized in the laser-created channels, as the QDs spread over the surrounding tissues. (2018) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE).

Enhanced upconversion emission in colloidal (NaYF4:Er(3+))/NaYF4 core/shell nanoparticles excited at 1523 nm.

PubMed

Shao, Wei; Chen, Guanying; Damasco, Jossana; Wang, Xianliang; Kachynski, Aliaksandr; Ohulchanskyy, Tymish Y; Yang, Chunhui; Ågren, Hans; Prasad, Paras N

2014-03-15

In this work, we report on efficient visible and near-IR upconversion emissions in colloidal hexagonal-phase core/shell NaYF4:Er(3+)/NaYF4 nanoparticles (∼38  nm) under IR laser excitation at 1523 nm. Varying amounts of Er(3+) dopants were introduced into the core NaYF4:Er(3+) nanoparticles, revealing an optimized Er(3+) concentration of 10% for the highest luminescent efficiency. An inert epitaxial shell layer of NaYF4 grown onto the core of the NaYF4:Er(3+) 10% nanoparticle increased its upconversion emission intensity fivefold due to suppression of surface-related quenching mechanisms, yielding the absolute upconversion efficiency to be as high as ∼3.9±0.3% under an excitation density of 18  W/cm(2). The dependence of the intensity of upconversion emission peaks on laser excitation density in the core/shell nanoparticle displayed "saturation effects" at low excitation density in the range of 1.5-18  W/cm(2), which again demonstrates high upconversion efficiency.

CdSe/AsS core-shell quantum dots: preparation and two-photon fluorescence.

PubMed

Wang, Junzhong; Lin, Ming; Yan, Yongli; Wang, Zhe; Ho, Paul C; Loh, Kian Ping

2009-08-19

Arsenic(II) sulfide (AsS)-coated CdSe core-shell nanocrystals can be prepared by a cluster-complex deposition approach under mild conditions. At 60 degrees C, growth of an AsS shell onto a CdSe nanocrystal can be realized through the crystallization of a cluster complex of AsS/butylamine in a mixed solvent of isopropanol/chloroform. The new, type I core-shell nanocrystal exhibits markedly enhanced one-photon fluorescence as well two-photon upconversion fluorescence. The nanocrystals can be used for infrared-excited upconversion cellular labeling.

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

PubMed

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

2011-10-15

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

Joint temporal density measurements for two-photon state characterization.

PubMed

Kuzucu, Onur; Wong, Franco N C; Kurimura, Sunao; Tovstonog, Sergey

2008-10-10

We demonstrate a technique for characterizing two-photon quantum states based on joint temporal correlation measurements using time-resolved single-photon detection by femtosecond up-conversion. We measure for the first time the joint temporal density of a two-photon entangled state, showing clearly the time anticorrelation of the coincident-frequency entangled photon pair generated by ultrafast spontaneous parametric down-conversion under extended phase-matching conditions. The new technique enables us to manipulate the frequency entanglement by varying the down-conversion pump bandwidth to produce a nearly unentangled two-photon state that is expected to yield a heralded single-photon state with a purity of 0.88. The time-domain correlation technique complements existing frequency-domain measurement methods for a more complete characterization of photonic entanglement.

Fabrication and characterization of biological tissue phantoms with embedded nanoparticles

NASA Astrophysics Data System (ADS)

Skaptsov, A. A.; Ustalkov, S. O.; Mohammed, A. H. M.; Savenko, O. A.; Novikova, A. S.; Kozlova, E. A.; Kochubey, V. I.

2017-11-01

Phantoms are imitations of biological tissue, which are used for modelling of the light propagation in biological tissues. Carrying out any biophysical experiments requires an indispensable constancy of the initial experiment conditions. The use of solid undegradable phantoms is the basis to obtain reliable reproducible experimental results. The fabrication of biological tissues phantoms containing high absorbance or fluorescence nanoparticles and corresponding to specific mechanical, optical properties is an actual task. This work describes development, fabrication and characterization of such solid tissue phantoms with embedded CdSe/ZnS quantum dots, gold and upconversion nanoparticles. Luminescence of samples with CdSe/ZnS quantum dots and upconversion nanoparticles were recorded. A sample of gold nanorods was analyzed using thermal gravimetric analysis. It can be concluded that the samples are well suited for experiments on laser thermolysis.

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

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

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

2015-07-20

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

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

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

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

2015-11-23

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

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

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

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

2015-11-23

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

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

NASA Astrophysics Data System (ADS)

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

2016-01-01

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

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

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

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

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.

Lanthanide‐Doped Upconversion Nanoparticles: Emerging Intelligent Light‐Activated Drug Delivery Systems

PubMed Central

Bagheri, Ali; Arandiyan, Hamidreza

2016-01-01

The development of drug delivery systems (DDSs) using near infrared (NIR) light and upconversion nanoparticles (UCNPs) has generated intensive interest over the past five years. These NIR‐initiated DDSs not only offer a high degree of spatial and temporal determination of therapeutic release but also provide precise control over the released dosage. Furthermore, these nanoplatforms confer several advantages over conventional light‐based DDSs—NIR offers better tissue penetration depth and a reduced risk of cellular photo‐damage caused by exposure to light at high‐energy wavelengths (e.g., ultraviolet light, <400 nm). The development of DDSs that can be activated by low intensity NIR illumination is highly desirable to avoid exposing living tissues to excessive heat that can limit the in vivo application of these DDSs. This encompasses research in three directions: (i) enhancing the quantum yield of the UCNPs; (ii) incorporation of photo‐responsive materials with red‐shifted absorptions into the UCNPs; and (iii) tuning the UCNPs excitation wavelength. This review focuses on recent advances in the development of NIR‐initiated DDS, with emphasis on the use of photo‐responsive compounds and polymeric materials conjugated onto UCNPs. The challenges that limit UCNPs clinical applications, alongside with the aforementioned techniques that have emerged to overcome these limitations, are highlighted. PMID:27818904

Two-photon absorption and upconversion luminescence of colloidal CsPbX3 quantum dots

NASA Astrophysics Data System (ADS)

Han, Qiuju; Wu, Wenzhi; Liu, Weilong; Yang, Qingxin; Yang, Yanqiang

2018-01-01

The nonlinear optical and the upconversion luminescence (UCL) properties of CsPbX3 (X = Br or its binary mixtures with Cl, I) quantum dots (QDs) are investigated by femtosecond open-aperture (OA) Z-scan and time-resolved luminescence techniques in nonresonant spectral region. The OA Z-scan results show that CsPbX3 QDs have strong reverse saturable absorption (RSA), which is ascribed to two-photon absorption. Partially changing halide composition from Cl to Br, to I, two-photon absorption cross sections become larger at the same laser excitation intensity. The composition-tunable nonlinear absorption should be attributed to the gradual decrease of the lowest direct band gaps with the halide substitute. Moreover, the strong UCL can be observed under near infrared femtosecond laser excitation. Halide composition-tunable UCL dynamics of CsPbX3 QDs is analyzed by use of two-exponential fitting with deconvolution. When CsPbX3 QDs have similar sizes (10-13 nm), with partially changing halide composition from Cl to Br, to I, the average UCL lifetime becomes longer due to the variation of Kane energy. Our findings suggest all-inorganic perovskite QDs can be used as excellent gain medium for high-performance frequency-upconversion lasers and provide reference to engineer such QDs toward practical optoelectronic applications.

Synthesis of upconversion nanoparticles conjugated with graphene oxide quantum dots and their use against cancer cell imaging and photodynamic therapy.

PubMed

Choi, Seung Yoo; Baek, Seung Hoon; Chang, Sung-Jin; Song, Yohan; Rafique, Rafia; Lee, Kang Taek; Park, Tae Jung

2017-07-15

Multifunctional nanocomposite has a huge potential for cell imaging, drug delivery, and improving therapeutic effect with less side effects. To date, diverse approaches have been demonstrated to endow a single nanostructure with multifunctionality. Herein, we report the synthesis and application of core-shell nanoparticles composed with upconversion nanoparticle (UCNP) as a core and a graphene oxide quantum dot (GOQD) as a shell. The UCNP was prepared and applied for imaging-guided analyses of upconversion luminescence. GOQD was prepared and employed as promising drug delivery vehicles to improve anti-tumor therapy effect in this study. Unique properties of UCNPs and GOQDs were incorporated into a single nanostructure to provide desirable functions for cell imaging and drug delivery. In addition, hypocrellin A (HA) was loaded on GOQDs for photo-dynamic therapy (PDT). HA, a commonly used chemotherapy drug and a photo-sensitizer, was conjugated with GOQD by π-π interaction and loaded on PEGylated UCNP without complicated synthetic process, which can break structure of HA. Applying these core-shell nanoparticles to MTT assay, we demonstrated that the UCNPs with GOQD shell loaded with HA could be excellent candidates as multifunctional agents for cell imaging, drug delivery and cell therapy. Copyright © 2016 Elsevier B.V. All rights reserved.

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

2016-05-05

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.

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

Upconversion fluorescence tyrosine doped LaF3:Dy quantum dots useful in biolabeling and biotagging

NASA Astrophysics Data System (ADS)

Singh, Amit T.; Khandpekar, M. M.

2018-04-01

Water soluble hexahedral colloidal quantum dots (QDOTs) of Tyrosine doped LaF3:Dy have been synthesized by wet chemical route. The nanoparticles have been irradiated by microwave during synthesis for drying and also to reduce agglomeration. The coating of the LaF3:Dy nanoparticles by the amino acid tyrosine results in colloidal quantum dots. XRD studies indicates hexagonal lattice and confirms JCPDS data. The average particle size obtained by XRD and SEM are 22.89nm and 25.5nm respectively. The average sizes of nanorods obtained from TEM are 55 nm. The presence of elements has been verified with EDAX and ICP-AES technique. The SAED pattern of the samples shows sharp concentric rings indicating the crystalline nature of the synthesized nanoparticles. The FTIR spectra have been used to study the surface modification of the nanoparticles. The optical studies have been done using UV-visible and PL spectra. The PL spectra showed upconversion nature of the synthesized nanoparticles with sharp emission at 618 nm. The nanoparticles synthesized have potential application as biomaterials in bio imaging and biotagging.

Electron-Deficient Near-Infrared Pt(II) and Pd(II) Benzoporphyrins with Dual Phosphorescence and Unusually Efficient Thermally Activated Delayed Fluorescence: First Demonstration of Simultaneous Oxygen and Temperature Sensing with a Single Emitter.

PubMed

Zach, Peter W; Freunberger, Stefan A; Klimant, Ingo; Borisov, Sergey M

2017-11-01

We report a family of Pt and Pd benzoporphyrin dyes with versatile photophysical properties and easy access from cheap and abundant chemicals. Attaching 4 or 8 alkylsulfone groups onto a meso-tetraphenyltetrabenzoporphyrin (TPTBP) macrocylcle renders the dyes highly soluble in organic solvents, photostable, and electron-deficient with the redox potential raised up to 0.65 V versus the parent porphyrin. The new dyes intensively absorb in the blue (Soret band, 440-480 nm) and in the red (Q-band, 620-650 nm) parts of the electromagnetic spectrum and show bright phosphorescence at room-temperature in the NIR with quantum yields up to 30% in solution. The small singlet-triplet energy gap yields unusually efficient thermally activated delayed fluorescence (TADF) at elevated temperatures in solution and in polymeric matrices with quantum yields as high as 27% at 120 °C, which is remarkable for benzoporphyrins. Apart from oxygen sensing, these properties enable unprecedented simultaneous, self-referenced oxygen and temperature sensing with a single indicator dye: whereas oxygen can be determined either via the decay time of phosphorescence or TADF, the temperature is accessed via the ratio of the two emissions. Moreover, the dyes are efficient sensitizers for triplet-triplet annihilation (TTA)-based upconversion making possible longer sensitization wavelength than the conventional benzoporphyrin complexes. The Pt-octa-sulfone dye also features interesting semireversible transformation in basic media, which generates new NIR absorbing species.

Solar upconversion with plasmon-enhanced bimolecular complexes

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

Dionne, Jennifer

2017-04-14

Upconversion of sub-bandgap photons is a promising approach to exceed the Shockley-Queisser limit in solar technologies. However, due to the low quantum efficiencies and narrow absorption bandwidths of upconverters, existing systems have only led to fractional percent improvements in photovoltaic devices (~0.01%). In this project, we aimed to develop an efficient upconverting material that could improve cell efficiencies by at least one absolute percent. To achieve this goal, we first used thermodynamic calculations to determine cell efficiencies with realistic upconverting materials. Then, we designed, synthesized, and characterized nanoantennas that promise >100x enhancement in both the upconverter absorption cross-section and emissivemore » radiative rate. Concurrently, we optimized the upconverer by designing new ionic and molecular complexes that promise efficient solid-state upconversion. Lastly, with Bosch, we simulated record-efficiency semi-transparent cells that will allow for ready incorporation of our upconverting materials. While we were not successful in designing record efficiency upconverters during our three years of funding, we gained significant insight into the existing limitations of upconverters and how to best address these challenges. Ongoing work is aimed at addressing these limitations, to make upconversion a cost-competitive solar technology in future years.« less

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

NASA Astrophysics Data System (ADS)

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

1997-07-01

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

Photophysics of Zinc Porphyrin Aggregates in Dilute Water-Ethanol Solutions.

PubMed

Stevens, Amy L; Joshi, Neeraj K; Paige, Matthew F; Steer, Ronald P

2017-12-14

Dimeric and multimeric aggregates of a model metalloporphyrin, zinc tetraphenylporphyrin (ZnTPP), have been produced in a controlled manner by incrementally increasing the water content of dilute aqueous ethanol solutions. Steady state absorption, fluorescence emission, and fluorescence excitation spectra have been measured to identify the aggregates present as a function of solvent composition. The dynamics of the excited states of the aggregates produced initially by excitation in the Soret region have been measured by ultrafast fluorescence upconversion techniques. Only the monomer produces measurable emission from S 2 with a picosecond lifetime; all Soret-excited aggregates, including the dimer, decay radiationlessly on a femtosecond time scale. The S 1 state is the only significant product of the radiationless decay of the S 2 state of the excited monomer, and the aggregates also produce substantial quantum yields of S 1 fluorescence when initially excited in the Soret region. The resulting fluorescent aggregates all decay on a subnanosecond time scale, likely by a mechanism that involves dissociation of the excited monomer from the excitonic multimer. The ZnTPP dimers excited at their ground state geometries in the Soret region exhibit a dynamic behavior that is quite different from those produced following noncoherent triplet-triplet annihilation under the same conditions. The important implications of these observations in determining the aggregation conditions promoting efficient photon upconversion by excitonic annihilation in a variety of media are thoroughly discussed.

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

NASA Astrophysics Data System (ADS)

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

2015-05-01

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

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

PubMed Central

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

2014-01-01

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

Simultaneous parametric generation and up-conversion of entangled optical images

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

Saygin, M. Yu., E-mail: mihasyu@gmail.com; Chirkin, A. S., E-mail: aschirkin@rambler.r

A quantum theory of parametric amplification and frequency conversion of an optical image in coupled nonlinear optical processes that include one parametric amplification process at high-frequency pumping and two up-conversion processes in the same pump field is developed. The field momentum operator that takes into account the diffraction and group velocities of the waves is used to derive the quantum equations related to the spatial dynamics of the images during the interaction. An optical scheme for the amplification and conversion of a close image is considered. The mean photon number density and signal-to-noise ratio are calculated in the fixed-pump-field approximationmore » for images at various frequencies. It has been established that the signal-to-noise ratio decreases with increasing interaction length in the amplified image and increases in the images at the generated frequencies, tending to asymptotic values for all interacting waves. The variance of the difference of the numbers of photons is calculated for various pairs of frequencies. The quantum entanglement of the optical images formed in a high-frequency pump field is shown to be converted to higher frequencies during the generation of sum frequencies. Thus, two pairs of entangled optical images are produced in the process considered.« less

Amplifying the Red-Emission of Upconverting Nanoparticles for Biocompatible Clinically Used Prodrug-Induced Photodynamic Therapy

DOE PAGES

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira; ...

2014-09-25

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP–PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major stepmore » forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors.Lastly, it also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.« less

Amplifying the red-emission of upconverting nanoparticles for biocompatible clinically used prodrug-induced photodynamic therapy.

PubMed

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira; El-Rifai, Mahmoud; Lee, Hyungseok; Zhang, Yuanwei; Wang, Chao; Liu, Zhuang; Chan, Emory M; Duan, Chunying; Han, Gang

2014-10-28

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP-PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major step forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors. It also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.

Amplifying the Red-Emission of Upconverting Nanoparticles for Biocompatible Clinically Used Prodrug-Induced Photodynamic Therapy

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

Punjabi, Amol; Wu, Xiang; Tokatli-Apollon, Amira

A class of biocompatible upconverting nanoparticles (UCNPs) with largely amplified red-emissions was developed. The optimal UCNP shows a high absolute upconversion quantum yield of 3.2% in red-emission, which is 15-fold stronger than the known optimal β-phase core/shell UCNPs. When conjugated to aminolevulinic acid, a clinically used photodynamic therapy (PDT) prodrug, significant PDT effect in tumor was demonstrated in a deep-tissue (>1.2 cm) setting in vivo at a biocompatible laser power density. Furthermore, we show that our UCNP–PDT system with NIR irradiation outperforms clinically used red light irradiation in a deep tumor setting in vivo. This study marks a major stepmore » forward in photodynamic therapy utilizing UCNPs to effectively access deep-set tumors.Lastly, it also provides an opportunity for the wide application of upconverting red radiation in photonics and biophotonics.« less

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

PubMed

Sun, Jifu; Wu, Wanhua; Zhao, Jianzhang

2012-06-25

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

Computational modelling of Er(3+): Garnet laser materials

NASA Technical Reports Server (NTRS)

Spangler, Lee H.

1994-01-01

The Er(3+) ion has attracted a lot of interest for four reasons: (1) Its (4)I(sub 13/2) yields (4)I(sub 15/2) transition lases in the eyesafe region near 1.5 micron; (2) the (4)I(sub 13/2) transition lases near 2.8 micron, an important wavelength for surgical purposes; (3) it displays surprisingly efficient upconversion with lasing observed at 1.7, 1.2, 0.85, 0.56, 0.55, and 0.47 micron following 1.5 micron pumping; and (4) it has absorption bands at 0.96 and 0.81 micron and thus can be diode pumped. However, properties desirable for upconversion reduce the efficiency of 1.5 and 3 micron laser operation and vice versa. Since all of the processes are influenced by the host via the crystal field induced stark splittings in the Er levels, this project undertook modelling of the host influence on the Er lasinng behavior. While growth and measurement of all ten Er(3+) doped garnets is the surest way of identifying hosts which maximize upconversion (or conversly, 1.5 and 3 micron performance), it is also expensive - costing approximately $10,000/material or approximately $100,000 for the materials computationally investigated here. The calculations were performed using a quantum mechanical point charge model developed by Clyde Morrison at Harry Diamond Laboratories. The programs were used to fit the Er:YAG experimental energy levels so that the crystal field parameters, B(sub nm) could be extracted. From these radial factors, rho (sub n) were determined for Er(3+) in garnets. These, in combination with crystal field components, Anm, available from X-ray data, were used to predict energy levels for Er in the other nine garnet hosts. The levels in Er:YAG were fit with an rms error of 12.2/cm over a 22,000/cm range. Predicted levels for two other garnets for which literature values were available had rms errors of less than 17/cm , showing the calculations to be reliable. Based on resonances between pairs of calculated stark levels, the model predicts GSGG as the best host for 1.5 micron laser operation, GSGG or YSAG as the best host for a 2.8 micron operation, and LuGG as the best host for an upconversion material.

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

NASA Astrophysics Data System (ADS)

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

2017-02-01

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

Photocatalytic Water-Splitting Enhancement by Sub-Bandgap Photon Harvesting.

PubMed

Monguzzi, Angelo; Oertel, Amadeus; Braga, Daniele; Riedinger, Andreas; Kim, David K; Knüsel, Philippe N; Bianchi, Alberto; Mauri, Michele; Simonutti, Roberto; Norris, David J; Meinardi, Francesco

2017-11-22

Upconversion is a photon-management process especially suited to water-splitting cells that exploit wide-bandgap photocatalysts. Currently, such catalysts cannot utilize 95% of the available solar photons. We demonstrate here that the energy-conversion yield for a standard photocatalytic water-splitting device can be enhanced under solar irradiance by using a low-power upconversion system that recovers part of the unutilized incident sub-bandgap photons. The upconverter is based on a sensitized triplet-triplet annihilation mechanism (sTTA-UC) obtained in a dye-doped elastomer and boosted by a fluorescent nanocrystal/polymer composite that allows for broadband light harvesting. The complementary and tailored optical properties of these materials enable efficient upconversion at subsolar irradiance, allowing the realization of the first prototype water-splitting cell assisted by solid-state upconversion. In our proof-of concept device the increase of the performance is 3.5%, which grows to 6.3% if concentrated sunlight (10 sun) is used. Our experiments show how the sTTA-UC materials can be successfully implemented in technologically relevant devices while matching the strict requirements of clean-energy production.

A dual-targeting upconversion nanoplatform for two-color fluorescence imaging-guided photodynamic therapy.

PubMed

Wang, Xu; Yang, Cheng-Xiong; Chen, Jia-Tong; Yan, Xiu-Ping

2014-04-01

The targetability of a theranostic probe is one of the keys to assuring its theranostic efficiency. Here we show the design and fabrication of a dual-targeting upconversion nanoplatform for two-color fluorescence imaging-guided photodynamic therapy (PDT). The nanoplatform was prepared from 3-aminophenylboronic acid functionalized upconversion nanocrystals (APBA-UCNPs) and hyaluronated fullerene (HAC60) via a specific diol-borate condensation. The two specific ligands of aminophenylboronic acid and hyaluronic acid provide synergistic targeting effects, high targetability, and hence a dramatically elevated uptake of the nanoplatform by cancer cells. The high generation yield of (1)O2 due to multiplexed Förster resonance energy transfer between APBA-UCNPs (donor) and HAC60 (acceptor) allows effective therapy. The present nanoplatform shows great potential for highly selective tumor-targeted imaging-guided PDT.

Near-Infrared-to-Visible Photon Upconversion Enabled by Conjugated Porphyrinic Sensitizers under Low-Power Noncoherent Illumination.

PubMed

Olivier, Jean-Hubert; Bai, Yusong; Uh, Hyounsoo; Yoo, Hyejin; Therien, Michael J; Castellano, Felix N

2015-06-04

We report four supermolecular chromophores based on (porphinato)zinc(II) (PZn) and (polypyridyl)metal units bridged via ethyne connectivity (Pyr1RuPZn2, Pyr1RuPZnRuPyr1, Pyr1RuPZn2RuPyr1, and OsPZn2Os) that fulfill critical sensitizer requirements for NIR-to-vis triplet-triplet annihilation upconversion (TTA-UC) photochemistry. These NIR sensitizers feature: (i) broad, high oscillator strength NIR absorptivity (700 nm < λ(max(NIR)) < 770 nm; 6 × 10(4) M(-1) cm(-1) < extinction coefficient (λ(max(NIR))) < 1.6 × 10(5) M(-1) cm(-1); 820 cm(-1) < fwhm < 1700 cm(-1)); (ii) substantial intersystem crossing quantum yields; (iii) long, microsecond time scale T1 state lifetimes; and (iv) triplet states that are energetically poised for exergonic energy transfer to the molecular annihilator (rubrene). Using low-power noncoherent illumination at power densities (1-10 mW cm(-2)) similar to that of terrestrial solar photon illumination conditions, we demonstrate that Pyr1RuPZn2, Pyr1RuPZn2RuPyr1, and Pyr1RuPZnRuPyr1 sensitizers can be used in combination with the rubrene acceptor/annihilator to achieve TTA-UC: these studies represent the first examples whereby a low-power noncoherent NIR light source drives NIR-to-visible upconverted fluorescence centered in a spectral window within the bandgap of amorphous silicon.

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

PubMed

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

2016-04-13

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

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

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

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

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

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

PubMed Central

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

2017-01-01

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

Architecture, development and implementation of a SWIR to visible integrated up-conversion imaging device

NASA Astrophysics Data System (ADS)

Sarusi, Gabby; Templeman, Tzvi; Hechster, Elad; Nissim, Nimrod; Vitenberg, Vladimir; Maman, Nitzan; Tal, Amir; Solodar, Assi; Makov, Guy; Abdulhalim, Ibrahim; Visoly-Fisher, Iris; Golan, Yuval

2016-04-01

A new concept of short wavelength infrared (SWIR) to visible upconversion integrated imaging device is proposed, modeled and some initial measured results are presented. The device is a hybrid inorganic-organic device that comprises six nano-metric scale sub-layers grown on n-type GaAs substrates. The first layer is a ~300nm thick PbSe nano-columnar absorber layer grown in (111) orientation to the substrate plan (100), with a diameter of 8- 10nm and therefore exhibit quantum confinement effects parallel to the substrate and bulk properties perpendicular to it. The advantage of this structure is the high oscillator strength and hence absorption to incoming SWIR photons while maintaining the high bulk mobility of photo-excited charges along the columns. The top of the PbSe absorber layer is coated with 20nm thick metal layer that serves as a dual sided mirror, as well as a potentially surface plasmon enhanced absorption in the PbSe nano-columns layer. The photo-excited charges (holes and electrons in opposite directions) are drifted under an external applied field to the OLED section (that is composed of a hole transport layer, an emission layer and an electron transport layer) where they recombine with injected electron from the transparent cathode and emit visible light through this cathode. Due to the high absorption and enhanced transport properties this architecture has the potential of high quantum efficiency, low cost and easy implementation in any optical system. As a bench-mark, alternative concept where InGaAs/InP heterojunction couple to liquid crystal optical spatial light modulator (OSLM) structure was built that shows a full upconversion to visible of 1550nm laser light.

Quantum Phenomena in High Energy Density Plasmas

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

Murnane, Margaret; Kapteyn, Henry

The possibility of implementing efficient (phase matched) HHG upconversion of deep- UV lasers in multiply-ionized plasmas, with potentially unprecedented conversion efficiency is a fascinating prospect. HHG results from the extreme nonlinear response of matter to intense laser light:high harmonics are radiated as a result of a quantum coherent electron recollision process that occurs during laser field ionization of an atom. Under current support from this grant in work published in Science in 2015, we discovered a new regime of bright HHG in highly-ionized plasmas driven by intense UV lasers, that generates bright harmonics to photon energies >280eV

Widely tunable quantum cascade laser-based terahertz source.

PubMed

Danylov, Andriy A; Light, Alexander R; Waldman, Jerry; Erickson, Neal; Qian, Xifeng

2014-07-10

A compact, tunable, ultranarrowband terahertz source, Δν∼1  MHz, is demonstrated by upconversion of a 2.324 THz, free-running quantum cascade laser with a THz Schottky-diode-balanced mixer using a swept, synthesized microwave source to drive the nonlinearity. Continuously tunable radiation of 1 μW power is demonstrated in two frequency regions: ν(Laser) ± 0 to 50 GHz and ν(Laser) ± 70 to 115 GHz. The sideband spectra were characterized with a Fourier-transform spectrometer, and the radiation was tuned through CO, HDO, and D2O rotational transitions.

Experimental Measurement-Device-Independent Quantum Key Distribution

NASA Astrophysics Data System (ADS)

Liu, Yang; Chen, Teng-Yun; Wang, Liu-Jun; Liang, Hao; Shentu, Guo-Liang; Wang, Jian; Cui, Ke; Yin, Hua-Lei; Liu, Nai-Le; Li, Li; Ma, Xiongfeng; Pelc, Jason S.; Fejer, M. M.; Peng, Cheng-Zhi; Zhang, Qiang; Pan, Jian-Wei

2013-09-01

Quantum key distribution is proven to offer unconditional security in communication between two remote users with ideal source and detection. Unfortunately, ideal devices never exist in practice and device imperfections have become the targets of various attacks. By developing up-conversion single-photon detectors with high efficiency and low noise, we faithfully demonstrate the measurement-device-independent quantum-key-distribution protocol, which is immune to all hacking strategies on detection. Meanwhile, we employ the decoy-state method to defend attacks on a nonideal source. By assuming a trusted source scenario, our practical system, which generates more than a 25 kbit secure key over a 50 km fiber link, serves as a stepping stone in the quest for unconditionally secure communications with realistic devices.

Experimental measurement-device-independent quantum key distribution.

PubMed

Liu, Yang; Chen, Teng-Yun; Wang, Liu-Jun; Liang, Hao; Shentu, Guo-Liang; Wang, Jian; Cui, Ke; Yin, Hua-Lei; Liu, Nai-Le; Li, Li; Ma, Xiongfeng; Pelc, Jason S; Fejer, M M; Peng, Cheng-Zhi; Zhang, Qiang; Pan, Jian-Wei

2013-09-27

Quantum key distribution is proven to offer unconditional security in communication between two remote users with ideal source and detection. Unfortunately, ideal devices never exist in practice and device imperfections have become the targets of various attacks. By developing up-conversion single-photon detectors with high efficiency and low noise, we faithfully demonstrate the measurement-device-independent quantum-key-distribution protocol, which is immune to all hacking strategies on detection. Meanwhile, we employ the decoy-state method to defend attacks on a nonideal source. By assuming a trusted source scenario, our practical system, which generates more than a 25 kbit secure key over a 50 km fiber link, serves as a stepping stone in the quest for unconditionally secure communications with realistic devices.

Lanthanide-doped upconversion nanocrystals: Synthesis and optical properties study

NASA Astrophysics Data System (ADS)

Sun, Qiang

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

Synthesis and application of nanohybrids based on upconverting nanoparticles and polymers.

PubMed

Cheng, Ziyong; Lin, Jun

2015-05-01

Lanthanide-doped upconversion nanoparticles (UCNPs) have been an emerging and exciting research field in recent years due to their unique luminescent properties of converting near-infrared light to shorter wavelength radiation. UCNPs offer excellent prospects in luminescent labeling, displays, bioimaging, bioassays, drug delivery, sensors, and anticounterfeiting applications. Along with the abundant studies and rapid progress in this area, UCNPs are promising to be a new class of luminescent probe owing to their special advantages over the conventional organic dyes and quantum dots. Among them, polymers play an important role to improve properties or endow new function of UCNPs such as for matrix materials, water solubility, linking active targeting molecules, biocompatibility, and stimuli-responsive behavior. This article briefly reviews the compositions, optical mechanisms, architectures of upconversion nanocrystals and highlights the works on various functional UCNPs/polymer nanohybrids as well as many new interesting fruits in applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Femtowatt incoherent image conversion from mid-infrared light to near-infrared light

NASA Astrophysics Data System (ADS)

Huang, Nan; Liu, Hongjun; Wang, Zhaolu; Han, Jing; Zhang, Shuan

2017-03-01

We report on the experimental conversion imaging of an incoherent continuous-wave dim source from mid-infrared light to near-infrared light with a lowest input power of 31 femtowatt (fW). Incoherent mid-infrared images of light emission from a heat lamp bulb with an adjustable power supply at window wavelengths ranging from 2.9 µm to 3.5 µm are used for upconversion. The sum-frequency generation is realized in a laser cavity with the resonant wavelength of 1064 nm pumped by an LD at 806 nm built around a periodically poled lithium niobate (PPLN) crystal. The converted infrared image in the wavelength range ~785 nm with a resolution of about 120  ×  70 is low-noise detected using a silicon-based camera. By optimizing the system parameters, the upconversion quantum efficiency is predicted to be 28% for correctly polarized, on-axis and phase-matching light.

Anti-Stokes Luminescence in High Quality Quantum Wells

NASA Astrophysics Data System (ADS)

Vinattieri, A.; Bogani, F.; Miotto, A.; Ceccherini, S.

1997-11-01

We present a detailed investigation of the anti-Stokes (AS) luminescence which originates from exciton recombination when below gap excitation is used, in a set of high quality quantum well structures. We observe strong excitonic resonances in the AS signal as measured from photoluminescence and photoluminescence excitation spectra. We demonstrate that neither the electromagnetic coupling between the wells nor the morphological disorder can explain this up-conversion effect. Time-resolved luminescence data after ps excitation and fs correlation spectroscopy results provide clear evidence of the occurrence of a two-step absorption which is assisted by the exciton population resonantly excited by the first photon.

Broadband continuous-variable entanglement source using a chirped poling nonlinear crystal

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

Zhao, J. S.; Sun, L.; Yu, X. Q.

2010-01-15

Aperiodically poled nonlinear crystal can be used as a broadband continuous-variable entanglement source and has strong stability under perturbations. We study the conversion dynamics of the sum-frequency generation and the quantum correlation of the two pump fields in a chirped-structure nonlinear crystal using the quantum stochastic method. The results show that there exists a frequency window for the pumps where two optical fields can perform efficient upconversion. The two pump fields are demonstrated to be entangled in the window and the chirped-structure crystal can be used as a continuous-variable entanglement source with a broad response bandwidth.

Opto-electronic conversion logic behaviour through dynamic modulation of electron/energy transfer states at the TiO2-carbon quantum dot interface.

PubMed

Wang, Fang; Zhang, Yonglai; Liu, Yang; Wang, Xuefeng; Shen, Mingrong; Lee, Shuit-Tong; Kang, Zhenhui

2013-03-07

Here we show a bias-mediated electron/energy transfer process at the CQDs-TiO(2) interface for the dynamic modulation of opto-electronic properties. Different energy and electron transfer states have been observed in the CQDs-TNTs system due to the up-conversion photoluminescence and the electron donation/acceptance properties of the CQDs decorated on TNTs.

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

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

Walla, P.J.; Yom, J.; Krueger, B.P.

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 aftermore » 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.« less

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

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

NASA Astrophysics Data System (ADS)

Boriskina, Svetlana V.; Chen, Gang

2014-03-01

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

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

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

Lei Yanqiang; Song Hongwei; Yang Linmei

2005-11-01

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

Efficiency enhancement of hybridized solar cells through co-sensitization and fast charge extraction by up-converted polyethylene glycol modified carbon quantum dots

NASA Astrophysics Data System (ADS)

Zhu, Wanlu; Duan, Jialong; Duan, Yanyan; Zhao, Yuanyuan; Tang, Qunwei

2017-11-01

Photovoltaics are promising solutions to energy crisis and environmental pollution problems. The dye-sensitized solar cells with mesoscopic structures have attracted growing interests because of zero emissions, easy fabrication, scalable materials and techniques, etc. However, the state-of-the-art dye-sensitized solar cells have narrow spectral absorption for photoelectric conversion and high electron-hole recombination rate under sunlight illumination. Therefore, it is a persistent object to make wide-spectral absorption and fast charge extraction solar cells for energy harvest in both solar and dark-light conditions. To address this issue, we present here experimental realization of a category of solar cells converting visible and near-infrared light into electricity by co-sensitizing photoanode with N719 dye and polyethylene glycol (PEG) modified carbon quantum dots (PEG-m-CQDs), arising from up-conversion and hole-transporting behaviors of PEG-m-CQDs as well as photofluorescence of green-emitting long persistence phosphors. The optimized solar cell yields maximized photoelectric conversion efficiencies of 9.89% and 25.81% under simulated sunlight (air mass 1.5, 100 mW cm-2) illumination and dark conditions, respectively. This work is far from optimization, but the physical proof-of-concept hybridized solar cell may markedly increase electricity generation time and total power output of photovoltaic platforms.

Quantum dot-decorated semiconductor micro- and nanoparticles: A review of their synthesis, characterization and application in photocatalysis.

PubMed

Bajorowicz, Beata; Kobylański, Marek P; Gołąbiewska, Anna; Nadolna, Joanna; Zaleska-Medynska, Adriana; Malankowska, Anna

2018-06-01

Quantum dot (QD)-decorated semiconductor micro- and nanoparticles are a new class of functional nanomaterials that have attracted considerable interest for their unique structural, optical and electronic properties that result from the large surface-to-volume ratio and the quantum confinement effect. In addition, because of QDs' excellent light-harvesting capacity, unique photoinduced electron transfer, and up-conversion behaviour, semiconductor nanoparticles decorated with quantum dots have been used widely in photocatalytic applications for the degradation of organic pollutants in both the gas and aqueous phases. This review is a comprehensive overview of the recent progress in synthesis methods for quantum dots and quantum dot-decorated semiconductor composites with an emphasis on their composition, morphology and optical behaviour. Furthermore, various approaches used for the preparation of QD-based composites are discussed in detail with respect to visible and UV light-induced photoactivity. Finally, an outlook on future development is proposed with the goal of overcoming challenges and stimulating further research into this promising field. Copyright © 2018 Elsevier B.V. All rights reserved.

BaY2F8 doped with Er3+: An upconverter material for photovoltaic application

NASA Astrophysics Data System (ADS)

Boccolini, A.; Faoro, R.; Favilla, E.; Veronesi, S.; Tonelli, M.

2013-08-01

Fluoride crystals (BaY2F8) doped with Er3+ ions with different doping level have been grown with a home-made Czochralski furnace. A spectroscopic characterization consisting in both absorption and fluorescence measurements were performed in order to investigate the upconversion mechanism occurring when the material is excited with a radiation at 1557 nm. The measured emission spectrum shows a photoluminescence mainly distributed in the Near Infrared (NIR) region at ≃1 μm. The spectral conversion due to the upconversion makes this material suitable for photovoltaic applications, especially if we combine it with a crystalline silicon solar cell. A device made of single face solar cell+upconverter material (PV-UC) was designed and his external quantum efficiency (EQE) at 1557 nm was measured. EQE values of 6.5% and 4.1% were reached under 8.5 W cm-2 power density illumination for the 30%Er3+ and 20%Er3+ samples, respectively.

Topology optimized gold nanostrips for enhanced near-infrared photon upconversion

NASA Astrophysics Data System (ADS)

Vester-Petersen, Joakim; Christiansen, Rasmus E.; Julsgaard, Brian; Balling, Peter; Sigmund, Ole; Madsen, Søren P.

2017-09-01

This letter presents a topology optimization study of metal nanostructures optimized for electric-field enhancement in the infrared spectrum. Coupling of such nanostructures with suitable ions allows for an increased photon-upconversion yield, with one application being an increased solar-cell efficiency by exploiting the long-wavelength part of the solar spectrum. In this work, topology optimization is used to design a periodic array of two-dimensional gold nanostrips for electric-field enhancements in a thin film doped with upconverting erbium ions. The infrared absorption band of erbium is utilized by simultaneously optimizing for two polarizations, up to three wavelengths, and three incident angles. Geometric robustness towards manufacturing variations is implemented considering three different design realizations simultaneously in the optimization. The polarization-averaged field enhancement for each design is evaluated over an 80 nm wavelength range and a ±15-degree incident angle span. The highest polarization-averaged field enhancement is 42.2 varying by maximally 2% under ±5 nm near-uniform design perturbations at three different wavelengths (1480 nm, 1520 nm, and 1560 nm). The proposed method is generally applicable to many optical systems and is therefore not limited to enhancing photon upconversion.

A sensitive infrared imaging up converter and spatial coherence of atmospheric propagation

NASA Technical Reports Server (NTRS)

Boyd, R. W.; Townes, C. H.

1977-01-01

An infrared imaging technique based on the nonlinear interaction known as upconversion was used to obtain images of several astronomical objects in the 10 micrometer spectral region, and to demonstrate quantitatively the sharper images allowed for wavelengths beyond the visible region. The deleterious effects of atmospheric inhomogeneities on telescope resolution were studied in the infrared region using the technique developed. The low quantum efficiency of the device employed severely limited its usefulness as an astronomical detector.

A photonic quantum information interface.

PubMed

Tanzilli, S; Tittel, W; Halder, M; Alibart, O; Baldi, P; Gisin, N; Zbinden, H

2005-09-01

Quantum communication requires the transfer of quantum states, or quantum bits of information (qubits), from one place to another. From a fundamental perspective, this allows the distribution of entanglement and the demonstration of quantum non-locality over significant distances. Within the context of applications, quantum cryptography offers a provably secure way to establish a confidential key between distant partners. Photons represent the natural flying qubit carriers for quantum communication, and the presence of telecommunications optical fibres makes the wavelengths of 1,310 nm and 1,550 nm particularly suitable for distribution over long distances. However, qubits encoded into alkaline atoms that absorb and emit at wavelengths around 800 nm have been considered for the storage and processing of quantum information. Hence, future quantum information networks made of telecommunications channels and alkaline memories will require interfaces that enable qubit transfers between these useful wavelengths, while preserving quantum coherence and entanglement. Here we report a demonstration of qubit transfer between photons of wavelength 1,310 nm and 710 nm. The mechanism is a nonlinear up-conversion process, with a success probability of greater than 5 per cent. In the event of a successful qubit transfer, we observe strong two-photon interference between the 710 nm photon and a third photon at 1,550 nm, initially entangled with the 1,310 nm photon, although they never directly interacted. The corresponding fidelity is higher than 98 per cent.

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

NASA Astrophysics Data System (ADS)

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

2005-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2014-01-01

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

An instrument to measure mechanical up-conversion phenomena in metals in the elastic regime

NASA Astrophysics Data System (ADS)

Vajente, G.; Quintero, E. A.; Ni, X.; Arai, K.; Gustafson, E. K.; Robertson, N. A.; Sanchez, E. J.; Greer, J. R.; Adhikari, R. X.

2016-06-01

Crystalline materials, such as metals, are known to exhibit deviation from a simple linear relation between strain and stress when the latter exceeds the yield stress. In addition, it has been shown that metals respond to varying external stress in a discontinuous way in this regime, exhibiting discrete releases of energy. This crackling noise has been extensively studied both experimentally and theoretically when the metals are operating in the plastic regime. In our study, we focus on the behavior of metals in the elastic regime, where the stresses are well below the yield stress. We describe an instrument that aims to characterize non-linear mechanical noise in metals when stressed in the elastic regime. In macroscopic systems, this phenomenon is expected to manifest as a non-stationary noise modulated by external disturbances applied to the material, a form of mechanical up-conversion of noise. The main motivation for this work is for the case of maraging steel components (cantilevers and wires) in the suspension systems of terrestrial gravitational wave detectors. Such instruments are planned to reach very ambitious displacement sensitivities, and therefore mechanical noise in the cantilevers could prove to be a limiting factor for the detectors' final sensitivities, mainly due to non-linear up-conversion of low frequency residual seismic motion to the frequencies of interest for the gravitational wave observations. We describe here the experimental setup, with a target sensitivity of 10-15 m/ √{ Hz } in the frequency range of 10-1000 Hz, a simple phenomenological model of the non-linear mechanical noise, and the analysis method that is inspired by this model.

Quantum cascade laser-based mid-IR frequency metrology system with ultra-narrow linewidth and 1  ×  10⁻¹³-level frequency instability.

PubMed

Hansen, Michael G; Magoulakis, Evangelos; Chen, Qun-Feng; Ernsting, Ingo; Schiller, Stephan

2015-05-15

We demonstrate a powerful tool for high-resolution mid-IR spectroscopy and frequency metrology with quantum cascade lasers (QCLs). We have implemented frequency stabilization of a QCL to an ultra-low expansion (ULE) reference cavity, via upconversion to the near-IR spectral range, at a level of 1×10(-13). The absolute frequency of the QCL is measured relative to a hydrogen maser, with instability <1×10(-13) and inaccuracy 5×10(-13), using a frequency comb phase stabilized to an independent ultra-stable laser. The QCL linewidth is determined to be 60 Hz, dominated by fiber noise. Active suppression of fiber noise could result in sub-10 Hz linewidth.

A chip-scale, telecommunications-band frequency conversion interface for quantum emitters.

PubMed

Agha, Imad; Ates, Serkan; Davanço, Marcelo; Srinivasan, Kartik

2013-09-09

We describe a chip-scale, telecommunications-band frequency conversion interface designed for low-noise operation at wavelengths desirable for common single photon emitters. Four-wave-mixing Bragg scattering in silicon nitride waveguides is used to demonstrate frequency upconversion and downconversion between the 980 nm and 1550 nm wavelength regions, with signal-to-background levels > 10 and conversion efficiency of ≈ -60 dB at low continuous wave input pump powers (< 50 mW). Finite element simulations and the split-step Fourier method indicate that increased input powers of ≈ 10 W (produced by amplified nanosecond pulses, for example) will result in a conversion efficiency > 25 % in existing geometries. Finally, we present waveguide designs that can be used to connect shorter wavelength (637 nm to 852 nm) quantum emitters with 1550 nm.

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

PubMed

Azam, Mohd; Rai, Vineet Kumar

2018-01-24

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

Direct Evidence of Significant Cation Intermixing in Upconverting Core@Shell Nanocrystals: Toward a New Crystallochemical Model

DOE PAGES

Hudry, Damien; Busko, Dmitry; Popescu, Radian; ...

2017-11-02

Core@shell design represents an important class of architectures because of its capability to dramatically increase the absolute upconversion quantum yield (UCQY) of upconverting nanocrystals (UCNCs) but also to tune energy migration pathways. A relatively new trend towards the use of very thick optically inert shells affording significantly higher absolute UCQYs raises the question of the crystallographic and chemical characteristics of such nanocrystals (NCs). In this article, local chemical analyses performed by scanning transmission electron microscopy (STEM) combined with energy dispersive x-ray spectroscopy (EDXS) and x-ray total scattering experiments together with pair distribution function (PDF) analyses were used to probe themore » local chemical and structural characteristics of hexagonal β-NaGd0.78Yb0.2Er0.02F4@NaYF4 core@shell UCNCs. The investigations lead to a new crystallochemical model to describe core@shell UCNCs that considerably digresses from the commonly accepted epitaxial growth concept with sharp interfaces. The results obtained on ultra-small (4.8 ± 0.5 nm) optically active cores (β-NaGd0.78Yb0.2Er0.02F4) surrounded by an optically inert shell (NaYF4) of tunable thickness (roughly 0, 1, 2, and 3.5 nm) clearly indicate the massive dissolution of the starting seeds and the inter-diffusion of the shell element (such as Y) into the Gd/Yb/Er-containing core giving rise to the formation of a non-homogeneous solid solution characterized by concentration gradients and the lack of sharp interfaces. Independently of the inert shell thickness, core/interface/shell architectures were observed for all synthesized UCNCs. The presented results constitute a significant step towards the comprehensive understanding of the “structure - property” relationship of upconverting core@shell architectures, which is of prime interest not only in the development of more efficient structures but also to provide new physical insights at the nanoscale to better explain upconversion (UC) properties alterations.« less

Direct Evidence of Significant Cation Intermixing in Upconverting Core@Shell Nanocrystals: Toward a New Crystallochemical Model

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

Hudry, Damien; Busko, Dmitry; Popescu, Radian

Core@shell design represents an important class of architectures because of its capability to dramatically increase the absolute upconversion quantum yield (UCQY) of upconverting nanocrystals (UCNCs) but also to tune energy migration pathways. A relatively new trend towards the use of very thick optically inert shells affording significantly higher absolute UCQYs raises the question of the crystallographic and chemical characteristics of such nanocrystals (NCs). In this article, local chemical analyses performed by scanning transmission electron microscopy (STEM) combined with energy dispersive x-ray spectroscopy (EDXS) and x-ray total scattering experiments together with pair distribution function (PDF) analyses were used to probe themore » local chemical and structural characteristics of hexagonal β-NaGd0.78Yb0.2Er0.02F4@NaYF4 core@shell UCNCs. The investigations lead to a new crystallochemical model to describe core@shell UCNCs that considerably digresses from the commonly accepted epitaxial growth concept with sharp interfaces. The results obtained on ultra-small (4.8 ± 0.5 nm) optically active cores (β-NaGd0.78Yb0.2Er0.02F4) surrounded by an optically inert shell (NaYF4) of tunable thickness (roughly 0, 1, 2, and 3.5 nm) clearly indicate the massive dissolution of the starting seeds and the inter-diffusion of the shell element (such as Y) into the Gd/Yb/Er-containing core giving rise to the formation of a non-homogeneous solid solution characterized by concentration gradients and the lack of sharp interfaces. Independently of the inert shell thickness, core/interface/shell architectures were observed for all synthesized UCNCs. The presented results constitute a significant step towards the comprehensive understanding of the “structure - property” relationship of upconverting core@shell architectures, which is of prime interest not only in the development of more efficient structures but also to provide new physical insights at the nanoscale to better explain upconversion (UC) properties alterations.« less

Infrared upconversion for astronomy

NASA Technical Reports Server (NTRS)

Boyd, R. W.

1977-01-01

The basic theory of upconversion is presented, along with a brief historical summary of upconversion techniques. Upconverters were used in astronomical studies, but have met with only modest success. Upconversion will become a useful detection method for astronomy only if substantial but perhaps forseeable, improvements can be realized.

Luminescence upconversion under hydrostatic pressure in the 3d-metal systems Ti2+:NaCl and Ni2+:CsCdCl3

NASA Astrophysics Data System (ADS)

Wenger, Oliver S.; Salley, G. Mackay; Valiente, Rafael; Güdel, Hans U.

2002-06-01

We present a study of upconversion materials and processes under external hydrostatic pressure. The near-infrared to visible photon upconversion properties of Ti2+-doped NaCl and Ni2+-doped CsCdCl3 at 15 K are studied as a function of external hydrostatic pressure. It is found that in Ti2+:NaCl pressure can be used to switch on an efficient upconversion mechanism, which is inactive at ambient pressure, leading to an order-of-magnitude enhancement of the overall upconversion efficiency of this material. For Ni2+:CsCdCl3 it is demonstrated that upconversion luminescence excitation spectroscopy can be used to study the pressure dependence of excited state absorption transitions. The results demonstrate the ability to tune upconversion properties by altering the local crystal field of active ions, in addition to probing the pressure dependence of excited state absorption transitions via upconversion spectroscopy.

Current Advances in Lanthanide‐Doped Upconversion Nanostructures for Detection and Bioapplication

PubMed Central

Chen, Cailing

2016-01-01

Along with the development of science and technology, lanthanide‐doped upconversion nanostructures as a new type of materials have taken their place in the field of nanomaterials. Upconversion luminescence is a nonlinear optical phenomenon, which absorbs two or more photons and emits one photon. Compared with traditional luminescence materials, upconversion nanostructures have many advantages, such as weak background interference, long lifetime, low excitation energy, and strong tissue penetration. These interesting nanostructures can be applied in anticounterfeit, solar cell, detection, bioimaging, therapy, and so on. This review is focused on the current advances in lanthanide‐doped upconversion nanostructures, covering not only basic luminescence mechanism, synthesis, and modification methods but also the design and fabrication of upconversion nanostructures, like core–shell nanoparticles or nanocomposites. At last, this review emphasizes the application of upconversion nanostructure in detection and bioimaging and therapy. Learning more about the advances of upconversion nanostructures can help us better exploit their excellent performance and use them in practice. PMID:27840794

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

PubMed

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

2018-03-01

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

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

PubMed

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

2017-10-18

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

Facile synthesis of S, N co-doped carbon dots and investigation of their photoluminescence properties.

PubMed

Zhang, Yue; He, Junhui

2015-08-21

A facile one-pot approach to prepare photoluminescent carbon dots (CDs) was developed through hydrothermal treatment of cysteine and citric acid. The obtained CDs show stable and bright blue emission with a quantum yield of 54% and an average lifetime of 11.61 ns. Moreover, the two-photon induced upconversion fluorescence of the CDs was observed and demonstrated. Interestingly, both down and up conversion fluorescence of the CDs show excitation-independent emission, which is quite different from most of the previously reported CDs. Ultrafast spectroscopy was also employed here to study the photoluminescence (PL) properties of the CDs. After characterization using various spectroscopic techniques, a unique PL mechanism for the as-prepared CDs' fluorescence was proposed accordingly. In addition, the influence of various metal ions on the CD fluorescence was examined and no quenching phenomena were observed. Meanwhile, gold nanoparticles (Au NPs) were found to be good quenchers of CD fluorescence and their quenching behavior was fitted to the Stern-Volmer equation. This provides new opportunities for fluorescence sensor designs and light energy conversion applications. Finally, the as-prepared CDs were inkjet-printed to form a desirable pattern, which is useful for fluorescent patterns, and anti-counterfeiting labeling.

The Role of Triplet Exciton Diffusion in Light-Upconverting Polymer Glasses.

PubMed

Raišys, Steponas; Kazlauskas, Karolis; Juršėnas, Saulius; Simon, Yoan C

2016-06-22

Light upconversion (UC) via triplet-triplet annihilation (TTA) by using noncoherent photoexcitation at subsolar irradiance power densities is extremely attractive, particularly for enhanced solar energy harvesting. Unfortunately, practical TTA-UC application is hampered by low UC efficiency of upconverting polymer glasses, which is commonly attributed to poor exciton diffusion of the triplet excitons across emitter molecules. The present study addresses this issue by systematically evaluating triplet exciton diffusion coefficients and diffusion lengths (LD) in a UC model system based on platinum-octaethylporphyrin-sensitized poly(methyl methacrylate)/diphenylanthracene (emitter) films as a function of emitter concentration (15-40 wt %). For this evaluation time-resolved photoluminescence bulk-quenching technique followed by Stern-Volmer-type quenching analysis of experimental data was employed. The key finding is that although increasing emitter concentration in the disordered PMMA/DPA/PtOEP films improves triplet exciton diffusion, and thus LD, this does not result in enhanced UC quantum yield. Conversely, improved LD accompanied by the accelerated decay of UC intensity on millisecond time scale degrades TTA-UC performance at high emitter loadings (>25 wt %) and suggests that diffusion-enhanced nonradiative decay of triplet excitons is the major limiting factor.

In vivo 808 nm image-guided photodynamic therapy based on an upconversion theranostic nanoplatform

NASA Astrophysics Data System (ADS)

Liu, Xiaomin; Que, Ivo; Kong, Xianggui; Zhang, Youlin; Tu, Langping; Chang, Yulei; Wang, Tong Tong; Chan, Alan; Löwik, Clemens W. G. M.; Zhang, Hong

2015-09-01

A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the 1O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, 1O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm-2) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy.A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the 1O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, 1O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm-2) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr03690a

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.

Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications

DOE PAGES

Wu, Xiang; Zhang, Yuanwei; Takle, Kendra; ...

2016-01-06

A near-infrared (NIR) dye-sensitized upconversion nanoparticles (UCNPs) can broaden the absorption range and boost upconversion efficiency of UCNPs. We achieved significantly enhanced upconversion luminescence in dye-sensitized core/active shell UCNPs via the doping of ytterbium ions (Yb 3+ ) in the UCNP shell, which bridged the energy transfer from the dye to the UCNP core. As a result, we synergized the two most practical upconversion booster effectors (dye-sensitizing and core/shell enhancement) to amplify upconversion efficiency. We also demonstrated two biomedical applications using these UCNPs. By using dye-sensitized core/active shell UCNP embedded poly(methyl methacrylate) polymer implantable systems, we successfully shifted the optogeneticmore » neuron excitation window to a biocompatible and deep tissue penetrable 800 nm wavelength. Furthermore, UCNPs were water-solubilized with Pluronic F127 with high upconversion efficiency and can be imaged in a mouse model.« less

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

Up-conversion fluorescence: noncoherent excitation by sunlight.

PubMed

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

2006-10-06

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

Intermolecular interaction approach for TADF (Conference Presentation)

NASA Astrophysics Data System (ADS)

Wong, Ken-Tsung

2016-09-01

Materials with thermally activated delayed fluorescence (TADF) have recently emerged as new fluorescent emitters for highly efficient organic light-emitting diodes (OLEDs). Molecule with TADF behavior needs to have a small singlet-triplet energy difference (ΔES-T) that allows the up-conversion from nonradiative triplet state (T1) to radiative singlet state (S1) via reverse intersystem crossing (RISC) process. Generally, molecules with small ΔES-T can be obtained via carefully manipulate the degree of "intramolecular" charge transfer (ICT) between electron-donating and -accepting components, such that the electron exchange energy that contributes to ΔES-T, can be minimized. Alternatively, excited state with small ΔES-T can be feasibly realized via "intermolecular" charge transfer occurring at the interface between spatially separating donor (D) and acceptor (A) molecules. Because the exchange energy decreases as the HOMO-LUMO separation distance increases, theoretically, the intermolecular D/A charge transfer state (or exciplex) should have rather small ΔES-T, leading to efficient TADF. However, it is still a challenge to access highly efficient exciplex systems. This is mainly because exciplex formation is commonly accompanied with a large red shift of emission spectra and long radiative lifetime, which tend to diminish photoluminescence quantum yield (PLQY) as well as electroluminescence (EL) performance. Until now, exciplex-based OLEDs with external quantum efficiency (EQE) above 10% are still limited. By judicious selection of donor and acceptor, the formation of efficient exciplex can be feasibly achieved. In this conference, our recent efforts on highly efficient exciplexes using C3-symmetry triazine acceptors and various donors, and their device characteristics will be presented.

Photoluminescence upconversion at GaAs /InGa P2 interfaces driven by a sequential two-photon absorption mechanism

NASA Astrophysics Data System (ADS)

Hylton, N. P.; Hinrichsen, T. F.; Vaquero-Stainer, A. R.; Yoshida, M.; Pusch, A.; Hopkinson, M.; Hess, O.; Phillips, C. C.; Ekins-Daukes, N. J.

2016-06-01

This paper reports on the results of an investigation into the nature of photoluminescence upconversion at GaAs /InGa P2 interfaces. Using a dual-beam excitation experiment, we demonstrate that the upconversion in our sample proceeds via a sequential two-photon optical absorption mechanism. Measurements of photoluminescence and upconversion photoluminescence revealed evidence of the spatial localization of carriers in the InGa P2 material, arising from partial ordering of the InGa P2 . We also observed the excitation of a two-dimensional electron gas at the GaAs /InGa P2 heterojunction that manifests as a high-energy shoulder in the GaAs photoluminescence spectrum. Furthermore, the results of upconversion photoluminescence excitation spectroscopy demonstrate that the photon energy onset of upconversion luminescence coincides with the energy of the two-dimensional electron gas at the GaAs /InGa P2 interface, suggesting that charge accumulation at the interface can play a crucial role in the upconversion process.

Intense blue up-conversion luminescence in Tm 3+/Yb 3+ codoped oxyfluoride glass-ceramics containing β-PbF 2 nanocrystals

NASA Astrophysics Data System (ADS)

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

2005-12-01

Up-conversion luminescence properties of a Tm 3+/Yb 3+ codoped oxyfluoride glass-ceramics under 980 nm excitation are investigated. Intense blue emission centered at 476 nm, corresponding to 1G 4 → 3H 6 transitions of Tm 3+ was simultaneously observed in the transparent oxyfluoride glass ceramics at room temperature. The intensity of the blue up-conversion luminescence in a 1 mol% YbF 3-containing glass-ceramic was found to be about 40 times stronger than that in the precursor oxyfluoride glass. The reason for the intense Tm 3+ up-conversion luminescence in the oxyfluoride glass-ceramics is discussed. The dependence of up-conversion intensities on excitation power and possible up-conversion mechanism are also evaluated.

Intense blue up-conversion luminescence in Tm3+/Yb3+ codoped oxyfluoride glass-ceramics containing beta-PbF2 nanocrystals.

PubMed

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

2005-12-01

Up-conversion luminescence properties of a Tm3+/Yb3+ codoped oxyfluoride glass-ceramics under 980 nm excitation are investigated. Intense blue emission centered at 476 nm, corresponding to 1G4-->3H6 transitions of Tm3+ was simultaneously observed in the transparent oxyfluoride glass ceramics at room temperature. The intensity of the blue up-conversion luminescence in a 1 mol% YbF3-containing glass-ceramic was found to be about 40 times stronger than that in the precursor oxyfluoride glass. The reason for the intense Tm3+ up-conversion luminescence in the oxyfluoride glass-ceramics is discussed. The dependence of up-conversion intensities on excitation power and possible up-conversion mechanism are also evaluated.

In vivo 808 nm image-guided photodynamic therapy based on an upconversion theranostic nanoplatform.

PubMed

Liu, Xiaomin; Que, Ivo; Kong, Xianggui; Zhang, Youlin; Tu, Langping; Chang, Yulei; Wang, Tong Tong; Chan, Alan; Löwik, Clemens W G M; Zhang, Hong

2015-09-28

A new strategy for efficient in vivo image-guided photodynamic therapy (PDT) has been demonstrated utilizing a ligand-exchange constructed upconversion-C60 nanophotosensitizer. This theranostic platform is superior to the currently reported nanophotosensitizers in (i) directly bonding photosensitizer C60 to the surface of upconversion nanoparticles (UCNPs) by a smart ligand-exchange strategy, which greatly shortened the energy transfer distance and enhanced the (1)O2 production, resulting in the improvement of the therapeutic effect; (ii) realizing in vivo NIR 808 nm image-guided PDT with both excitation (980 nm) and emission (808 nm) light falling in the biological window of tissues, which minimized auto-fluorescence, reduced light scatting and improved the imaging contrast and depth, and thus guaranteed noninvasive diagnostic accuracy. In vivo and ex vivo tests demonstrated its favorable bio-distribution, tumor-selectivity and high therapeutic efficacy. Owing to the effective ligand exchange strategy and the excellent intrinsic photophysical properties of C60, (1)O2 production yield was improved, suggesting that a low 980 nm irradiation dosage (351 J cm(-2)) and a short treatment time (15 min) were sufficient to perform NIR (980 nm) to NIR (808 nm) image-guided PDT. Our work enriches the understanding of UCNP-based PDT nanophotosensitizers and highlights their potential use in future NIR image-guided noninvasive deep cancer therapy.

Ultrasensitive Detection of Ebola Virus Oligonucleotide Based on Upconversion Nanoprobe/Nanoporous Membrane System.

PubMed

Tsang, Ming-Kiu; Ye, WeiWei; Wang, Guojing; Li, Jingming; Yang, Mo; Hao, Jianhua

2016-01-26

Ebola outbreaks are currently of great concern, and therefore, development of effective diagnosis methods is urgently needed. The key for lethal virus detection is high sensitivity, since early-stage detection of virus may increase the probability of survival. Here, we propose a luminescence scheme of assay consisting of BaGdF5:Yb/Er upconversion nanoparticles (UCNPs) conjugated with oligonucleotide probe and gold nanoparticles (AuNPs) linked with target Ebola virus oligonucleotide. As a proof of concept, a homogeneous assay was fabricated and tested, yielding a detection limit at picomolar level. The luminescence resonance energy transfer is ascribed to the spectral overlapping of upconversion luminescence and the absorption characteristics of AuNPs. Moreover, we anchored the UCNPs and AuNPs on a nanoporous alumina (NAAO) membrane to form a heterogeneous assay. Importantly, the detection limit was greatly improved, exhibiting a remarkable value at the femtomolar level. The enhancement is attributed to the increased light-matter interaction throughout the nanopore walls of the NAAO membrane. The specificity test suggested that the nanoprobes were specific to Ebola virus oligonucleotides. The strategy combining UCNPs, AuNPs, and NAAO membrane provides new insight into low-cost, rapid, and ultrasensitive detection of different diseases. Furthermore, we explored the feasibility of clinical application by using inactivated Ebola virus samples. The detection results showed great potential of our heterogeneous design for practical application.

Er{sup 3+}/Yb{sup 3+}co-doped bismuth molybdate nanosheets upconversion photocatalyst with enhanced photocatalytic activity

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

Adhikari, Rajesh; Gyawali, Gobinda; Cho, Sung Hun

2014-01-15

In this paper, we report the microwave hydrothermal synthesis of Er{sup 3+}/Yb{sup 3+} co-doped Bi{sub 2}MoO{sub 6} upconversion photocatalyst. Crystal structure, morphology, elemental composition, optical properties and BET surface area were analyzed in detail. Infrared to visible upconversion luminescence at 532 nm and 546 nm of the co-doped samples was investigated under excitation at 980 nm. The results revealed that the co-doping of Er{sup 3+}/Yb{sup 3+} into Bi{sub 2}MoO{sub 6} exhibited enhanced photocatalytic activity for the decomposition of rhodamine B under simulated solar light irradiation. Enhanced photocatalytic activity can be attributed to the energy transfer between Er{sup 3+}/Yb{sup 3+} andmore » Bi{sub 2}MoO{sub 6} via infrared to visible upconversion from Er{sup 3+}/Yb{sup 3+} ion and higher surface area of the Bi{sub 2}MoO{sub 6} nanosheets. Therefore, this synthetic approach may exhibit a better alternative to fabricate upconversion photocatalyst for integral solar light absorption. - Graphical abstract: Schematic illustration of the upconversion photocatalysis. Display Omitted - Highlights: • Er{sup 3+}/Yb{sup 3+} co-doped Bi{sub 2}MoO{sub 6} upconversion photocatalyst is successfully synthesized. • We obtained the nanosheets having high surface area. • Upconversion of IR to visible light was confirmed. • Upconversion phenomena can be utilized for effective photocatalysis.« less

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

Nonplasmonic Hot-Electron Photocurrents from Mn-Doped Quantum Dots in Photoelectrochemical Cells.

PubMed

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

2016-03-03

We report the measurement of the hot-electron current in a photoelectrochemical cell constructed from a glass/ITO/Al2 O3 (ITO=indium tin oxide) electrode coated with Mn-doped quantum dots, where hot electrons with a large excess kinetic energy were produced through upconversion of the excitons into hot electron hole pairs under photoexcitation at 3 eV. In our recent study (J. Am. Chem. Soc. 2015, 137, 5549), we demonstrated the generation of hot electrons in Mn-doped II-VI semiconductor quantum dots and their usefulness in photocatalytic H2 production reaction, taking advantage of the more efficient charge transfer of hot electrons compared with band-edge electrons. Here, we show that hot electrons produced in Mn-doped CdS/ZnS quantum dots possess sufficient kinetic energy to overcome the energy barrier from a 5.4-7.5 nm thick Al2 O3 layer producing a hot-electron current in photoelectrochemical cell. This work demonstrates the possibility of harvesting hot electrons not only at the interface of the doped quantum dot surface, but also far away from it, thus taking advantage of the capability of hot electrons for long-range electron transfer across a thick energy barrier. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Effect of B2O3 on luminescence of erbium doped tellurite glasses.

PubMed

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

2007-02-01

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

Upconversion excitations in Pr3+-doped BaY2F8 crystal

NASA Astrophysics Data System (ADS)

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

2011-09-01

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

Decorating fiber nanotip with single perovskite quantum dot and other luminescent nanocrystals synthesized in oil-phase

NASA Astrophysics Data System (ADS)

Qian, Yu; Xing, Xing; Xu, Ya; Lu, Zhenda; Zhang, Weihua

2017-11-01

We report a simple yet robust method for fabricating single perovskite quantum dot (QD) decorated fiber nanotips. In this method, a single QD is directly picked up and subsequently glued on the apex of a specially fabricated cantilever fiber tip with a high success rate (approx. 70%) without using expensive close-loop feedback systems. Thanks to the flexibility and robustness of the fiber tips, no damage of the tips was observed in the process. Moreover, nanocrystal (NC) dispersing technique was developed to avoid undesired aggregations of QDs, and it guarantees that only one QD is glued each time. Finally, we demonstrate that this technique can also be applied to other oil-phase synthesized NCs, including CdSe QDs and upconversion luminescent NCs. It leads to many important applications on probing the local environment using high performance luminescent nanoprobes.

An Nd3+-sensitized upconversion nanophosphor modified with a cyanine dye for the ratiometric upconversion luminescence bioimaging of hypochlorite

NASA Astrophysics Data System (ADS)

Zou, Xianmei; Liu, Yi; Zhu, Xingjun; Chen, Min; Yao, Liming; Feng, Wei; Li, Fuyou

2015-02-01

Excessive or misplaced production of ClO- in living systems is usually associated with many human diseases. Therefore, it is of great importance to develop an effective and sensitive method to detect ClO- in living systems. Herein, we designed an 808 nm excited upconversion luminescence nanosystem, composed of the Nd3+-sensitized core-shell upconversion nanophosphor NaYF4:30%Yb,1%Nd,0.5%Er@NaYF4:20%Nd, which serves as an energy donor, and the ClO--responsive cyanine dye hCy3, which acts as an energy acceptor, for ratiometric upconversion luminescence (UCL) monitoring of ClO-. The detection limit of ClO- for this nanoprobe in aqueous solution is 27 ppb and the nanoprobe was successfully used to detect the ClO- in the living cells by ratiometric upconversion luminescence. Importantly, the nanoprobe realized the detection of ClO- in a mouse model of arthritis, which produced an excess of ROS, under 808 nm irradiation in vivo. The excitation laser efficiently reduced the heating effect, compared to the commonly used 980 nm laser for upconversion systems.Excessive or misplaced production of ClO- in living systems is usually associated with many human diseases. Therefore, it is of great importance to develop an effective and sensitive method to detect ClO- in living systems. Herein, we designed an 808 nm excited upconversion luminescence nanosystem, composed of the Nd3+-sensitized core-shell upconversion nanophosphor NaYF4:30%Yb,1%Nd,0.5%Er@NaYF4:20%Nd, which serves as an energy donor, and the ClO--responsive cyanine dye hCy3, which acts as an energy acceptor, for ratiometric upconversion luminescence (UCL) monitoring of ClO-. The detection limit of ClO- for this nanoprobe in aqueous solution is 27 ppb and the nanoprobe was successfully used to detect the ClO- in the living cells by ratiometric upconversion luminescence. Importantly, the nanoprobe realized the detection of ClO- in a mouse model of arthritis, which produced an excess of ROS, under 808 nm irradiation in vivo. The excitation laser efficiently reduced the heating effect, compared to the commonly used 980 nm laser for upconversion systems. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr06407k

Near-infrared photocatalysts of BiVO4/CaF2:Er3+, Tm3+, Yb3+ with enhanced upconversion properties

NASA Astrophysics Data System (ADS)

Huang, Shouqiang; Zhu, Nanwen; Lou, Ziyang; Gu, Lin; Miao, Chen; Yuan, Haiping; Shan, Aidang

2014-01-01

Upconversion photocatalysts have the potential to absorb the near-infrared (NIR) light in solar energy and improve the photocatalytic performance. A hierarchical upconversion photocatalyst of BiVO4 (BVO)/CaF2:Er3+, Tm3+, Yb3+ (CF) combined with the narrow-band semiconductor of BVO and the luminescence agent of CF to enhance upconversion properties was synthesized via the hydrothermal method. The CF particles were deposited homogeneously on the surface of the BVO/CF composite with regular dendritic structure, which led to efficient upconversion emissions. The upconversion emission intensity of the BVO/CF composite was 8 times higher than that of pure CF, through tailoring the crystal symmetry of lanthanide ions by Bi3+ ions. The upconverted ultraviolet (361 and 379 nm), violet (408 nm), and blue (485 nm) light was able to excite BVO for photocatalysis in BVO/CF under NIR irradiation, which improved the degradation rate of methyl orange (MO).Upconversion photocatalysts have the potential to absorb the near-infrared (NIR) light in solar energy and improve the photocatalytic performance. A hierarchical upconversion photocatalyst of BiVO4 (BVO)/CaF2:Er3+, Tm3+, Yb3+ (CF) combined with the narrow-band semiconductor of BVO and the luminescence agent of CF to enhance upconversion properties was synthesized via the hydrothermal method. The CF particles were deposited homogeneously on the surface of the BVO/CF composite with regular dendritic structure, which led to efficient upconversion emissions. The upconversion emission intensity of the BVO/CF composite was 8 times higher than that of pure CF, through tailoring the crystal symmetry of lanthanide ions by Bi3+ ions. The upconverted ultraviolet (361 and 379 nm), violet (408 nm), and blue (485 nm) light was able to excite BVO for photocatalysis in BVO/CF under NIR irradiation, which improved the degradation rate of methyl orange (MO). Electronic supplementary information (ESI) available: Additional tables and figures. See DOI: 10.1039/c3nr05266d

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.

Understanding the infrared to visible upconversion luminescence properties of Er{sup 3+}/Yb{sup 3+} co-doped BaMoO{sub 4} nanocrystals

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

Adhikari, Rajesh; Choi, Jinhyuk; Narro-García, R.

2014-08-15

In this paper we report the infrared to visible upconversion luminescence properties of Er{sup 3+}/Yb{sup 3+} co-doped BaMoO{sub 4} nanocrystals synthesized via microwave assisted sol–gel processing route. Structural, morphological and upconversion luminescence properties were investigated by X-ray diffraction (XRD), Transmission Electron Microscopy (TEM), UV–vis diffuse reflectance spectroscopy (UV–vis DRS) and Upconversion Photoluminescence spectra analysis. Results revealed that the oval shaped BaMoO{sub 4} nanocrystals ranging in size from 40 to 60 nm having tetragonal scheelite crystal structure were obtained by sol–gel route. The infrared to visible upconversion luminescence has been investigated in Er{sup 3+}/Yb{sup 3+} co-doped in BaMoO{sub 4}with different Yb{supmore » 3+} concentrations. Intense green upconversion emissions around 528, 550 nm, and red emission at 657 nm corresponding to the {sup 2}H{sub 11/2}, {sup 4}S{sub 3/2}, and {sup 4}F{sub 9/2} transitions, respectively to the {sup 4}I{sub 15/2} ground state were observed when excited by CW laser radiation at 980 nm. The green emissions were greatly enhanced after the addition of sensitizer (Yb{sup 3+} ions). The effect of Yb{sup 3+} on the upconversion luminescence intensity was analyzed and explained in terms of the energy transfer process based. The reported work establishes the understanding of molybdates as an alternative host material for upconversion luminescence. - Graphical abstract: Infrared to visible upconversion luminescence of Er{sup 3+}/Yb{sup 3+} co-doped BaMoO{sub 4} nanocrystals. - Highlights: • Nanocrystals were synthesized by microwave assisted sol–gel processing route. • Strong green emissions were observed in Er{sup 3+}/Yb{sup 3+} co-doped BaMoO{sub 4} nanocrystals. • Provides an insight on Upconversion luminescence properties of oxides host materials.« less

Ultrasmall lanthanide-doped nanoparticles as multimodal platforms

NASA Astrophysics Data System (ADS)

Yust, Brian G.; Pedraza, Francisco J.; Sardar, Dhiraj K.

2014-03-01

Recently, there has been a great amount of interest in nanoparticles which are able to provide a platform with high contrast for multiple imaging modalities in order to advance the tools available to biomedical researchers and physicians. However, many nanoparticles do not have ideal properties to provide high contrast in different imaging modes. In order to address this, ultrasmall lanthanide doped oxide and fluoride nanoparticles with strong NIR to NIR upconversion fluorescence and a strong magnetic response for magnetic resonance imaging (MRI) have been developed. Specifically, these nanoparticles incorporate gadolinium, dysprosium, or a combination of both into the nano-crystalline host to achieve the magnetic properties. Thulium, erbium, and neodymium codopants provide the strong NIR absorption and emission lines that allow for deeper tissue imaging since near infrared light is not strongly absorbed or scattered by most tissues within this region. This also leads to better image quality and lower necessary excitation intensities. As a part of the one pot synthesis, these nanoparticles are coated with peg, pmao, or d-glucuronic acid to make them water soluble, biocompatible, and bioconjugable due to the available carboxyl or amine groups. Here, the synthesis, morphological characterization, magnetic response, NIR emission, and the quantum yield will be discussed. Cytotoxicity tested through cell viability at varying concentrations of nanoparticles in growth media will also be discussed.

Spatial height directed microfluidic synthesis of transparent inorganic upconversion nano film

NASA Astrophysics Data System (ADS)

Liu, Xiaoxia; Zhu, Cheng; Liao, Wei; Jin, Junyang; Ni, Yaru; Lu, Chunhua; Xu, Zhongzi

2017-11-01

A microfluidic-based synthesis of an inorganic upconversion nano film has been developed with a large area of dense-distributed NaYF4 crystal grains in a silica glass micro-reactor and the film exhibits high transparence, strong upconversion luminescence and robust adhesion with the substrate. The spatial heights of micro-reactors are tuned between 31 and 227 mm, which can regulate flow regimes. The synergistic effect of spatial height and fluid regime is put forward, which influences diffusion paths and assembly ways of different precursor molecules and consequently directs final distributions and morphologies of crystal grains, as well as optical properties due to diversity of surface and thickness of films. The spatial height of 110 mm is advantageous for high transmittance of upconversion film due to the flat surface and appropriate film thickness of 67 nm. The height of 150 mm is in favor of uniform distribution of upconversion fluorescence and achieving the strongest fluorescence due to minimized optical loss. Such a transparent upconversion film with a large area of uniform distribution is promising to promote the application of upconversion materials and spatial height directed microfluidic regime have a certain significance on many microfluidic synthesis.

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

PubMed

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

2013-05-30

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

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

PubMed

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

2015-02-01

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Photon energy upconversion through thermal radiation with the power efficiency reaching 16%.

PubMed

Wang, Junxin; Ming, Tian; Jin, Zhao; Wang, Jianfang; Sun, Ling-Dong; Yan, Chun-Hua

2014-11-28

The efficiency of many solar energy conversion technologies is limited by their poor response to low-energy solar photons. One way for overcoming this limitation is to develop materials and methods that can efficiently convert low-energy photons into high-energy ones. Here we show that thermal radiation is an attractive route for photon energy upconversion, with efficiencies higher than those of state-of-the-art energy transfer upconversion under continuous wave laser excitation. A maximal power upconversion efficiency of 16% is achieved on Yb(3+)-doped ZrO2. By examining various oxide samples doped with lanthanide or transition metal ions, we draw guidelines that materials with high melting points, low thermal conductivities and strong absorption to infrared light deliver high upconversion efficiencies. The feasibility of our upconversion approach is further demonstrated under concentrated sunlight excitation and continuous wave 976-nm laser excitation, where the upconverted white light is absorbed by Si solar cells to generate electricity and drive optical and electrical devices.

Interactions of DNA coated upconversion nanoparticles with 2D materials

NASA Astrophysics Data System (ADS)

Giust, Davide; Lucío, María. Isabel; Muskens, Otto L.; Kanaras, Antonios G.

2018-02-01

In this work we investigated the nature of quenching between different types of 2D materials (WS2, MoS2 and graphene oxide) and oligonucleotide coated-upconversion nanoparticles. This study contributes towards the efficient design of biosensors based on 2D materials and DNA-coated upconversion nanoparticles.

Upconversion fiber-optic confocal microscopy under near-infrared pumping.

PubMed

Kim, Do-Hyun; Kang, Jin U; Ilev, Ilko K

2008-03-01

We present a simple upconversion fiber-optic confocal microscope design using a near-infrared laser for pumping of a rare-earth-doped glass powder. The nonlinear optical frequency conversion process is highly efficient with more than 2% upconversion fluorescence efficiency at a near-infrared pumping wavelength of 1.55 microm. The upconversion confocal design allows the use of conventional Si detectors and 1.55 microm near-infrared pump light. The lateral and axial resolutions of the system were equal to or better than 1.10 and 13.11 microm, respectively.

Controlling upconversion nanocrystals for emerging applications

NASA Astrophysics Data System (ADS)

Zhou, Bo; Shi, Bingyang; Jin, Dayong; Liu, Xiaogang

2015-11-01

Lanthanide-doped upconversion nanocrystals enable anti-Stokes emission with pump intensities several orders of magnitude lower than required by conventional nonlinear optical techniques. Their exceptional properties, namely large anti-Stokes shifts, sharp emission spectra and long excited-state lifetimes, have led to a diversity of applications. Here, we review upconversion nanocrystals from the perspective of fundamental concepts and examine the technical challenges in relation to emission colour tuning and luminescence enhancement. In particular, we highlight the advances in functionalization strategies that enable the broad utility of upconversion nanocrystals for multimodal imaging, cancer therapy, volumetric displays and photonics.

High efficiency upconversion nanophosphors for high-contrast bioimaging

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Laser-diode-excited blue upconversion in Tm3+/Yb3+ -codoped TeO2-Ga2O3-R2O (R=Li, Na, K) glasses.

PubMed

Zhao, Chun; Zhang, Qinyuan; Yang, Gangfeng; Jiang, Zhonghong

2008-01-01

This paper reports on intense blue upconversion in Tm(3+)/Yb(3+) codoped TeO(2)-Ga(2)O(3)-R(2)O(R=Li, Na, K) glasses upon excitation with commercial available laser diode (LD). Effects of alkali ions on the Raman spectra, thermal stability and spectroscopic properties of the tellurite-gallium glasses have also been investigated. Energy transfer and the involved upconversion mechanisms have been discussed. Intense blue upconversion emission centered at 476 nm along with a weak red emission at 650 nm has been observed upon excitation of 977 nm LD, assigned to the transitions of 1G4-->3H6, and 1G4-->3H4 and/or 3F(2,3)-->3H6 of Tm(3+), respectively. The blue upconversion intensity has a cubelike dependence on incident pump laser power, indicating a three-photon process. However, a quadratic dependence of the 476 nm upconversion intensity on the incident pump laser power has been observed when samples under excitation of 808 nm LD due to a two-photon absorption process. Enhanced upconversion luminescence have been observed with replacing K(+) for Na(+) and Li(+).

Plasmon enhanced upconversion luminescence of NaYF4:Yb,Er@SiO2@Ag core-shell nanocomposites for cell imaging.

PubMed

Yuan, Peiyan; Lee, Yih Hong; Gnanasammandhan, Muthu Kumara; Guan, Zhenping; Zhang, Yong; Xu, Qing-Hua

2012-08-21

NaYF(4):Yb,Er@SiO(2)@Ag core-shell nanocomposites were prepared to investigate metal-enhanced upconversion luminescence. Two sizes (15 and 30 nm) of Ag nanoparticles were used. The emission intensity of the upconversion nanocrystals was found to be strongly modulated by the presence of Ag nanoparticles (NPs) on the outer shell layer of the nanocomposites. The extent of modulation depended on the separation distance between Ag NPs and upconversion nanocrystals. The optimum upconversion luminescence enhancement was observed at a separation distance of 10 nm for Ag NPs with two different sizes (15 and 30 nm). A maximum upconversion luminescence enhancement of 14.4-fold was observed when 15 nm Ag nanoparticles were used and 10.8-fold was observed when 30 nm Ag NPs were used. The separation distance dependent emission intensity is ascribed to the competition between energy transfer and enhanced radiative decay rates. The biocompatibility of the nanocomposites was significantly improved by surface modification with DNA. The biological imaging capabilities of these nanocomposites were demonstrated using B16F0 cells.

Efficient upconversion emission in Ho3+/Nd3+ co-doped oxyfluorosilicate glasses

NASA Astrophysics Data System (ADS)

Devarajulu, G.; Raju, B. Deva Prasad

2018-04-01

We report on an efficient Ho3+ and Ho3+/Nd3+ co-doped oxyfluorosilicate glasses upon excitation with an 808 nm laser diode. The detailed fluorescence have been studied under this excitation source and energy transfer mechanisms in Ho3+/Nd3+ co-doped oxyfluorosilicate glasses. The upconversion peaks at 486, 547 and 596 nm were observed in Nd3+/Ho3+ co-doped sample. The intensity of upconversion emission transitions in Ho3+ depends on the neodymium codopent concentration. These results indicate that Nd3+ ions can be potentially used as sensitizer for Ho3+ ions to stimulate the intense upconversion emission. The energy transfer mechanism between Nd3+ and Ho3+ was analyzed pursuant to the absorption spectra, upconversion spectra and the energy level structures of Nd3+ and Ho3+ ions have been briefly discussed.

Low-noise mid-IR upconversion detector for improved IR-degenerate four-wave mixing gas sensing.

PubMed

Høgstedt, Lasse; Dam, Jeppe Seidelin; Sahlberg, Anna-Lena; Li, Zhongshan; Aldén, Marcus; Pedersen, Christian; Tidemand-Lichtenberg, Peter

2014-09-15

We compare a nonlinear upconversion detector with a conventional cryogenic InSb detector for the detection of coherent infrared light showing near-shot-noise-limited performance in the upconversion system. The InSb detector is limited by dark noise, which results in a 500 times lower signal-to-noise ratio. The two detectors are compared for the detection of a coherent degenerate four-wave mixing (DFWM) signal in the mid-infrared, and applied to measure trace-level acetylene in a gas flow at atmospheric pressure, probing its fundamental rovibrational transitions. In addition to lower noise, the upconversion system provides image information of the signal, thus adding new functionality compared to standard point detection methods. We further show that the upconversion detector system can be implemented as a simple replacement of the cryogenic detector.

The dissociative recombination of O2(+) - The quantum yield of O(1S) and O(1D)

NASA Technical Reports Server (NTRS)

Abreu, V. J.; Solomon, S. C.; Sharp, W. E.; Hays, P. B.

1983-01-01

Data from the visible airglow experiment on the Atmosphere Explorer-E satellite have been used to determine the quantum yield of O(1S) and O(1D) from the dissociative recombination of O2(+). A range of values between 0.09 and 0.23 has been obtained for the quantum yield of O(1S). It is shown that the quantum yield of O(1S) depends on the ratio of electron density to atomic oxygen density. This suggests that the quantum yield of O(1S) may depend on the degree of vibrational excitation of the recombining O2(+). The quantum yield of O(1D) has been measured to be 1.23 + or - 0.42, with no dependence on the electron-oxygen ratio.

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

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

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

2015-08-28

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

Plasmon enhanced upconversion luminescence of NaYF4:Yb,Er@SiO2@Ag core-shell nanocomposites for cell imaging

NASA Astrophysics Data System (ADS)

Yuan, Peiyan; Lee, Yih Hong; Gnanasammandhan, Muthu Kumara; Guan, Zhenping; Zhang, Yong; Xu, Qing-Hua

2012-07-01

NaYF4:Yb,Er@SiO2@Ag core-shell nanocomposites were prepared to investigate metal-enhanced upconversion luminescence. Two sizes (15 and 30 nm) of Ag nanoparticles were used. The emission intensity of the upconversion nanocrystals was found to be strongly modulated by the presence of Ag nanoparticles (NPs) on the outer shell layer of the nanocomposites. The extent of modulation depended on the separation distance between Ag NPs and upconversion nanocrystals. The optimum upconversion luminescence enhancement was observed at a separation distance of 10 nm for Ag NPs with two different sizes (15 and 30 nm). A maximum upconversion luminescence enhancement of 14.4-fold was observed when 15 nm Ag nanoparticles were used and 10.8-fold was observed when 30 nm Ag NPs were used. The separation distance dependent emission intensity is ascribed to the competition between energy transfer and enhanced radiative decay rates. The biocompatibility of the nanocomposites was significantly improved by surface modification with DNA. The biological imaging capabilities of these nanocomposites were demonstrated using B16F0 cells.NaYF4:Yb,Er@SiO2@Ag core-shell nanocomposites were prepared to investigate metal-enhanced upconversion luminescence. Two sizes (15 and 30 nm) of Ag nanoparticles were used. The emission intensity of the upconversion nanocrystals was found to be strongly modulated by the presence of Ag nanoparticles (NPs) on the outer shell layer of the nanocomposites. The extent of modulation depended on the separation distance between Ag NPs and upconversion nanocrystals. The optimum upconversion luminescence enhancement was observed at a separation distance of 10 nm for Ag NPs with two different sizes (15 and 30 nm). A maximum upconversion luminescence enhancement of 14.4-fold was observed when 15 nm Ag nanoparticles were used and 10.8-fold was observed when 30 nm Ag NPs were used. The separation distance dependent emission intensity is ascribed to the competition between energy transfer and enhanced radiative decay rates. The biocompatibility of the nanocomposites was significantly improved by surface modification with DNA. The biological imaging capabilities of these nanocomposites were demonstrated using B16F0 cells. Electronic supplementary information (ESI) available: More TEM images, distribution histograms, UV-Vis extinction spectra, and XRD analysis of the core-shell nanocomposites; the emission enhancement mechanisms, bright field images, the effect of DNA modification on the emission; luminescence stability and size changes of the DNA modified nanocomposites in the cell culture. See DOI: 10.1039/c2nr31241g

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Sub-Band Gap Turn-On Near-Infrared-to-Visible Up-Conversion Device Enabled by an Organic-Inorganic Hybrid Perovskite Photovoltaic Absorber.

PubMed

Yu, By Hyeonggeun; Cheng, Yuanhang; Li, Menglin; Tsang, Sai-Wing; So, Franky

2018-05-09

Direct integration of an infrared (IR) photodetector with an organic light-emitting diode (OLED) enables low-cost, pixel-free IR imaging. However, the operation voltage of the resulting IR-to-visible up-conversion is large because of the series device architecture. Here, we report a low-voltage near-IR (NIR)-to-visible up-conversion device using formamidinium lead iodide as a NIR absorber integrated with a phosphorescent OLED. Because of the efficient photocarrier injection from the hybrid perovskite layer to the OLED, we observed a sub-band gap turn-on of the OLED under NIR illumination. The device showed a NIR-to-visible up-conversion efficiency of 3% and a luminance on/off ratio of 10 3 at only 5 V. Finally, we demonstrate pixel-free NIR imaging using the up-conversion device.

Quantum Yield of Single Surface Plasmons Generated by a Quantum Dot Coupled with a Silver Nanowire.

PubMed

Li, Qiang; Wei, Hong; Xu, Hongxing

2015-12-09

The interactions between surface plasmons (SPs) in metal nanostructures and excitons in quantum emitters (QEs) lead to many interesting phenomena and potential applications that are strongly dependent on the quantum yield of SPs. The difficulty in distinguishing all the possible exciton recombination channels hinders the experimental determination of SP quantum yield. Here, we experimentally measured for the first time the quantum yield of single SPs generated by the exciton-plasmon coupling in a system composed of a single quantum dot and a silver nanowire (NW). By utilizing the SP guiding property of the NW, the decay rates of all the exciton recombination channels, i.e., direct free space radiation channel, SP generation channel, and nonradiative damping channel, are quantitatively obtained. It is determined that the optimum emitter-NW coupling distance for the largest SP quantum yield is about 10 nm, resulting from the different distance-dependent decay rates of the three channels. These results are important for manipulating the coupling between plasmonic nanostructures and QEs and developing on-chip quantum plasmonic devices for potential nanophotonic and quantum information applications.

Absolute quantum yield measurement of powder samples.

PubMed

Moreno, Luis A

2012-05-12

Measurement of fluorescence quantum yield has become an important tool in the search for new solutions in the development, evaluation, quality control and research of illumination, AV equipment, organic EL material, films, filters and fluorescent probes for bio-industry. Quantum yield is calculated as the ratio of the number of photons absorbed, to the number of photons emitted by a material. The higher the quantum yield, the better the efficiency of the fluorescent material. For the measurements featured in this video, we will use the Hitachi F-7000 fluorescence spectrophotometer equipped with the Quantum Yield measuring accessory and Report Generator program. All the information provided applies to this system. Measurement of quantum yield in powder samples is performed following these steps: 1. Generation of instrument correction factors for the excitation and emission monochromators. This is an important requirement for the correct measurement of quantum yield. It has been performed in advance for the full measurement range of the instrument and will not be shown in this video due to time limitations. 2. Measurement of integrating sphere correction factors. The purpose of this step is to take into consideration reflectivity characteristics of the integrating sphere used for the measurements. 3. Reference and Sample measurement using direct excitation and indirect excitation. 4. Quantum Yield calculation using Direct and Indirect excitation. Direct excitation is when the sample is facing directly the excitation beam, which would be the normal measurement setup. However, because we use an integrating sphere, a portion of the emitted photons resulting from the sample fluorescence are reflected by the integrating sphere and will re-excite the sample, so we need to take into consideration indirect excitation. This is accomplished by measuring the sample placed in the port facing the emission monochromator, calculating indirect quantum yield and correcting the direct quantum yield calculation. 5. Corrected quantum yield calculation. 6. Chromaticity coordinates calculation using Report Generator program. The Hitachi F-7000 Quantum Yield Measurement System offer advantages for this application, as follows: High sensitivity (S/N ratio 800 or better RMS). Signal is the Raman band of water measured under the following conditions: Ex wavelength 350 nm, band pass Ex and Em 5 nm, response 2 sec), noise is measured at the maximum of the Raman peak. High sensitivity allows measurement of samples even with low quantum yield. Using this system we have measured quantum yields as low as 0.1 for a sample of salicylic acid and as high as 0.8 for a sample of magnesium tungstate. Highly accurate measurement with a dynamic range of 6 orders of magnitude allows for measurements of both sharp scattering peaks with high intensity, as well as broad fluorescence peaks of low intensity under the same conditions. High measuring throughput and reduced light exposure to the sample, due to a high scanning speed of up to 60,000 nm/minute and automatic shutter function. Measurement of quantum yield over a wide wavelength range from 240 to 800 nm. Accurate quantum yield measurements are the result of collecting instrument spectral response and integrating sphere correction factors before measuring the sample. Large selection of calculated parameters provided by dedicated and easy to use software. During this video we will measure sodium salicylate in powder form which is known to have a quantum yield value of 0.4 to 0.5.

Sensitive Infrared Signal Detection by Upconversion Technique

NASA Technical Reports Server (NTRS)

Wong, Teh-Hwa; Yu, Jirong; Bai, Yingxin; Johnson, William; Chen, Songsheng; Petros, Mulugeta; Singh, Upendra N.

2014-01-01

We demonstrated upconversion assisted detection of a 2.05-micron signal by sum frequency generation to generate a 700-nm light using a bulk periodically poled lithium niobate crystal. The achieved 94% intrinsic upconversion efficiency and 22.58% overall detection efficiency at a pW level of 2.05 micron pave the path to detect extremely weak infrared (IR) signals for remote sensing applications.

Facile synthesis of hydrophilic multi-colour and upconversion photoluminescent mesoporous carbon nanoparticles for bioapplications.

PubMed

Kong, Qinglu; Zhang, Lingxia; Liu, Jianan; Wu, Meiying; Chen, Yu; Feng, Jingwei; Shi, Jianlin

2014-12-25

Hydrophilic mesoporous carbon nanoparticles (MCNs) have been synthesized via an extremely facile precursor carbonization-in-hot solvent route. The synthesized MCNs show well-defined particle and pore size distribution at around 100 nm and 2.7 nm, respectively, and multicolor and upconversion photoluminescence, which endow the MCNs with multicolor/upconversion bioimaging and drug delivery properties.

Infrared upconversion for astronomical applications. [laser applications to astronomical spectroscopy of infrared spectra

NASA Technical Reports Server (NTRS)

Abbas, M. M.; Kostiuk, T.; Ogilvie, K. W.

1975-01-01

The performance of an upconversion system is examined for observation of astronomical sources in the low to middle infrared spectral range. Theoretical values for the performance parameters of an upconversion system for astronomical observations are evaluated in view of the conversion efficiencies, spectral resolution, field of view, minimum detectable source brightness and source flux. Experimental results of blackbody measurements and molecular absorption spectrum measurements using a lithium niobate upconverter with an argon-ion laser as the pump are presented. Estimates of the expected optimum sensitivity of an upconversion device which may be built with the presently available components are given.

Bifunctional NaYF4:Er3+/Yb3+ submicron rods, implemented in quantum dot sensitized solar cell(Conference Presentation)

NASA Astrophysics Data System (ADS)

Guerrero, J. Pablo; Cerdán Pasarán, Andrea; López-Luke, Tzarara; Ramachari, D.; Esparza, Diego; De la Rosa Cruz, Elder; Romero Arellano, Victor Hugo

2016-09-01

In this work are presented the results obtained with solar cells sensitized with quantum dots of cadmium sulphide (CdS) incorporating luminescent materials (NaYF4:Yb/Er). The study revealed that through using a bifunctional layer of NaYF4:Yb/Er submicron rods, the infrared radiation is absorbed in 980nm to generate luminescence in the visible region to 530nm, under the UP-conversion process, in the same way simultaneously, NaYF4:Yb/Er layer causes scattering toward the quantum dots, the emission and scattering generated by this material is reabsorbed by the QD-CdS, and these in turn are absorbing in its range of solar radiation absorption, Thus generates an increase in the electron injection into the semiconductor of TiO2. The results of a cell incorporating NaYF4: Yb/Er at 0.07M shown photoconversion efficiencies of 3.39% improving efficiency with respect to the reference solar cell without using NaYF4: Yb/Er of 1.99%. The obtained values of current and voltage showed a strong dependence of the percentage of NaYF4 Yb/Er, and the mechanism of incorporation of this material.

Ladder Climbing and Autoresonant Acceleration of Plasma Waves

NASA Astrophysics Data System (ADS)

Barth, Ido; Dodin, Ilya; Fisch, Nathaniel

2015-11-01

When the background density in a bounded plasma is modulated in time, discrete modes become coupled. Interestingly, for appropriately chosen modulations, the average plasmon energy might be made to grow in a ladder-like manner, achieving up-conversion or down-conversion of the plasmon energy. This reversible process is identified as a classical analog of the effect known as quantum ladder climbing, so that the efficiency and the rate of this process can be written immediately by analogy to a quantum particle in a box. In the limit of densely spaced spectrum, ladder climbing transforms into continuous autoresonance; plasmons may then be manipulated by chirped background modulations much like electrons are autoresonantly manipulated by chirped fields. By formulating the wave dynamics within a universal Lagrangian framework, similar ladder climbing and autoresonance effects are predicted to be achievable with general linear waves in both plasma and other media. Supported by NNSA grant DE274-FG52-08NA28553, DOE contract DE-AC02-09CH11466, and DTRA grant HDTRA1-11-1-0037.

Development of ytterbium-doped oxyfluoride glasses for laser cooling applications.

PubMed

Krishnaiah, Kummara Venkata; de Lima Filho, Elton Soares; Ledemi, Yannick; Nemova, Galina; Messaddeq, Younes; Kashyap, Raman

2016-02-26

Oxyfluoride glasses doped with 2, 5, 8, 12, 16 and 20 mol% of ytterbium (Yb(3+)) ions have been prepared by the conventional melt-quenching technique. Their optical, thermal and thermo-mechanical properties were characterized. Luminescence intensity at 1020 nm under laser excitation at 920 nm decreases with increasing Yb(3+) concentration, suggesting a decrease in the photoluminescence quantum yield (PLQY). The PLQY of the samples was measured with an integrating sphere using an absolute method. The highest PLQY was found to be 0.99(11) for the 2 mol% Yb(3+): glass and decreases with increasing Yb(3+) concentration. The mean fluorescence wavelength and background absorption of the samples were also evaluated. Upconversion luminescence under 975 nm laser excitation was observed and attributed to the presence of Tm(3+) and Er(3+) ions which exist as impurity traces with YbF3 starting powder. Decay curves for the Yb(3+): (2)F5/2 → (2)F7/2 transition exhibit single exponential behavior for all the samples, although lifetime decrease was observed for the excited level of Yb(3+) with increasing Yb(3+) concentration. Also observed are an increase in the PLQY and a slight decrease in lifetime with increasing the pump power. Finally, the potential of these oxyfluoride glasses with high PLQY and low background absorption for laser cooling applications is discussed.

Development of ytterbium-doped oxyfluoride glasses for laser cooling applications

PubMed Central

Krishnaiah, Kummara Venkata; Soares de Lima Filho, Elton; Ledemi, Yannick; Nemova, Galina; Messaddeq, Younes; Kashyap, Raman

2016-01-01

Oxyfluoride glasses doped with 2, 5, 8, 12, 16 and 20 mol% of ytterbium (Yb3+) ions have been prepared by the conventional melt-quenching technique. Their optical, thermal and thermo-mechanical properties were characterized. Luminescence intensity at 1020 nm under laser excitation at 920 nm decreases with increasing Yb3+ concentration, suggesting a decrease in the photoluminescence quantum yield (PLQY). The PLQY of the samples was measured with an integrating sphere using an absolute method. The highest PLQY was found to be 0.99(11) for the 2 mol% Yb3+: glass and decreases with increasing Yb3+ concentration. The mean fluorescence wavelength and background absorption of the samples were also evaluated. Upconversion luminescence under 975 nm laser excitation was observed and attributed to the presence of Tm3+ and Er3+ ions which exist as impurity traces with YbF3 starting powder. Decay curves for the Yb3+: 2F5/2 → 2F7/2 transition exhibit single exponential behavior for all the samples, although lifetime decrease was observed for the excited level of Yb3+ with increasing Yb3+ concentration. Also observed are an increase in the PLQY and a slight decrease in lifetime with increasing the pump power. Finally, the potential of these oxyfluoride glasses with high PLQY and low background absorption for laser cooling applications is discussed. PMID:26915817

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.

Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

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

Ma, Xuedan; Diroll, Benjamin T.; Cho, Wooje

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g( 2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicatingmore » the importance of surface passivation on NPL emission quality. Second-order photon correlation (g( 2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. In conclusion, these findings reveal that by careful growth control and core–shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.« less

Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets

DOE PAGES

Ma, Xuedan; Diroll, Benjamin T.; Cho, Wooje; ...

2017-08-08

Quasi-two-dimensional nanoplatelets (NPLs) possess fundamentally different excitonic properties from zero-dimensional quantum dots. We study lateral size-dependent photon emission statistics and carrier dynamics of individual NPLs using second-order photon correlation (g( 2)(τ)) spectroscopy and photoluminescence (PL) intensity-dependent lifetime analysis. Room-temperature radiative lifetimes of NPLs can be derived from maximum PL intensity periods in PL time traces. It first decreases with NPL lateral size and then stays constant, deviating from the electric dipole approximation. Analysis of the PL time traces further reveals that the single exciton quantum yield in NPLs decreases with NPL lateral size and increases with protecting shell thickness, indicatingmore » the importance of surface passivation on NPL emission quality. Second-order photon correlation (g( 2)(τ)) studies of single NPLs show that the biexciton quantum yield is strongly dependent on the lateral size and single exciton quantum yield of the NPLs. In large NPLs with unity single exciton quantum yield, the corresponding biexciton quantum yield can reach unity. In conclusion, these findings reveal that by careful growth control and core–shell material engineering, NPLs can be of great potential for light amplification and integrated quantum photonic applications.« less

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

PubMed

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

2009-05-06

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

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

One-step hydrothermal synthesis of carboxyl-functionalized upconversion phosphors for bioapplications.

PubMed

Yang, Jianping; Shen, Dengke; Li, Xiaomin; Li, Wei; Fang, Yin; Wei, Yong; Yao, Chi; Tu, Bo; Zhang, Fan; Zhao, Dongyuan

2012-10-22

In this paper, we report a facile one-step hydrothermal method to synthesize phase-, size-, and shape-controlled carboxyl-functionalized rare-earth fluorescence upconversion phosphors by using a small-molecule binary acid, such as malonic acid, oxalic acid, succinic acid, or tartaric acid as capping agent. The crystals, from nano- to microstructures with diverse shapes that include nanospheres, microrods, hexagonal prisms, microtubes, microdisks, polygonal columns, and hexagonal tablets, can be obtained with different reaction times, reaction temperatures, molar ratios of capping agent to sodium hydroxide, and by varying the binary acids. Fourier transform infrared, thermogravimetric analysis, and upconversion luminescence spectra measurements indicate that the synthesized NaYF(4):Yb/Er products with hydrophilic carboxyl-functionalized surface offer efficient upconversion luminescent performance. Furthermore, the antibody/secondary antibody conjugation can be realized by the carboxyl-functionalized surfaces of the upconversion phosphors, thus indicating the potential bioapplications of these kinds of materials. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Upconversion-Triggered Charge Separation in Polymer Semiconductors.

PubMed

Jang, Yu Jin; Kim, Eunah; Ahn, Seonghyeon; Chung, Kyungwha; Kim, Jihyeon; Kim, Heejun; Wang, Huan; Lee, Jiseok; Kim, Dong-Wook; Kim, Dong Ha

2017-01-19

Upconversion is a unique optical property that is driven by a sequential photon pumping and generation of higher energy photons in a consecutive manner. The efficiency improvement in photovoltaic devices can be achieved when upconverters are integrated since upconverters contribute to the generation of extra photons. Despite numerous experimental studies confirming the relationship, fundamental explanations for a real contribution of upconversion to photovoltaic efficiency are still in demand. In this respect, we suggest a new approach to visualize the upconversion event in terms of surface photovoltage (SPV) by virtue of Kelvin probe force microscopy (KPFM). One of the most conventional polymer semiconductors, poly(3-hexyl thiophene) (P3HT), is employed as a sensitizer to generate charge carriers by upconverted light. KPFM measurements reveal that the light upconversion enabled the formation of charge carriers in P3HT, resulting in large SPV of -54.9 mV. It confirms that the energy transfer from upconverters to P3HT can positively impact the device performance in organic solar cells (OSCs).

Enhanced Upconversion Luminescence in Yb3+/Tm3+-Codoped Fluoride Active Core/Active Shell/Inert Shell Nanoparticles through Directed Energy Migration.

PubMed

Qiu, Hailong; Yang, Chunhui; Shao, Wei; Damasco, Jossana; Wang, Xianliang; Ågren, Hans; Prasad, Paras N; Chen, Guanying

2014-01-03

The luminescence efficiency of lanthanide-doped upconversion nanoparticles is of particular importance for their embodiment in biophotonic and photonic applications. Here, we show that the upconversion luminescence of typically used NaYF₄:Yb 3+ 30%/Tm 3+ 0.5% nanoparticles can be enhanced by ~240 times through a hierarchical active core/active shell/inert shell (NaYF₄:Yb 3+ 30%/Tm 3+ 0.5%)/NaYbF₄/NaYF₄ design, which involves the use of directed energy migration in the second active shell layer. The resulting active core/active shell/inert shell nanoparticles are determined to be about 11 times brighter than that of well-investigated (NaYF₄:Yb 3+ 30%/Tm 3+ 0.5%)/NaYF₄ active core/inert shell nanoparticles when excited at ~980 nm. The strategy for enhanced upconversion in Yb 3+ /Tm 3+ -codoped NaYF₄ nanoparticles through directed energy migration might have implications for other types of lanthanide-doped upconversion nanoparticles.

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

PubMed

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

2018-05-09

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

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

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

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

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

Absolute I(asterisk) quantum yields for the ICN A state by diode laser gain-vs-absorption spectroscopy

NASA Technical Reports Server (NTRS)

Hess, Wayne P.; Leone, Stephen R.

1987-01-01

Absolute I(asterisk) quantum yields have been measured as a function of wavelength for room temperature photodissociation of the ICN A state continuum. The yields are obtained by the technique of time-resolved diode laser gain-vs-absorption spectroscopy. Quantum yields are evaluated at seven wavelengths from 248 to 284 nm. The yield at 266 nm is 66.0 + or - 2 percent and it falls off to 53.4 + or - 2 percent and 44.0 + or - 4 percent at 284 and 248 nm, respectively. The latter values are significantly higher than those obtained by previous workers using infrared fluorescence. Estimates of I(asterisk) quantum yields obtained from analysis of CN photofragment rotational distributions, as discussed by other workers, are in good agreement with the I(asterisk) yields reported here. The results are considered in conjunction with recent theoretical and experimental work on the CN rotational distributions and with previous I(asterisk) quantum yield results.

Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids.

PubMed

Talgorn, Elise; Gao, Yunan; Aerts, Michiel; Kunneman, Lucas T; Schins, Juleon M; Savenije, T J; van Huis, Marijn A; van der Zant, Herre S J; Houtepen, Arjan J; Siebbeles, Laurens D A

2011-09-25

Solid films of colloidal quantum dots show promise in the manufacture of photodetectors and solar cells. These devices require high yields of photogenerated charges and high carrier mobilities, which are difficult to achieve in quantum-dot films owing to a strong electron-hole interaction and quantum confinement. Here, we show that the quantum yield of photogenerated charges in strongly coupled PbSe quantum-dot films is unity over a large temperature range. At high photoexcitation density, a transition takes place from hopping between localized states to band-like transport. These strongly coupled quantum-dot films have electrical properties that approach those of crystalline bulk semiconductors, while retaining the size tunability and cheap processing properties of colloidal quantum dots.

Control of Emission Color of High Quantum Yield CH3NH3PbBr3 Perovskite Quantum Dots by Precipitation Temperature.

PubMed

Huang, He; Susha, Andrei S; Kershaw, Stephen V; Hung, Tak Fu; Rogach, Andrey L

2015-09-01

Emission color controlled, high quantum yield CH 3 NH 3 PbBr 3 perovskite quantum dots are obtained by changing the temperature of a bad solvent during synthesis. The products for temperatures between 0 and 60 °C have good spectral purity with narrow emission line widths of 28-36 nm, high absolute emission quantum yields of 74% to 93%, and short radiative lifetimes of 13-27 ns.

Preparation of ZnO nanoparticles showing upconversion luminescence through simple chemical method

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

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

2016-05-23

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

[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.

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

PubMed

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

2006-06-01

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

Active media for up-conversion diode-pumped lasers

NASA Astrophysics Data System (ADS)

Tkachuk, Alexandra M.

1996-03-01

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

Creating high yield water soluble luminescent graphene quantum dots via exfoliating and disintegrating carbon nanotubes and graphite flakes.

PubMed

Lin, Liangxu; Zhang, Shaowei

2012-10-21

We have developed an effective method to exfoliate and disintegrate multi-walled carbon nanotubes and graphite flakes. With this technique, high yield production of luminescent graphene quantum dots with high quantum yield and low oxidization can be achieved.

Note: Measuring instrument of singlet oxygen quantum yield in photodynamic effects

NASA Astrophysics Data System (ADS)

Li, Zhongwei; Zhang, Pengwei; Zang, Lixin; Qin, Feng; Zhang, Zhiguo; Zhang, Hongli

2017-06-01

Using diphenylisobenzofuran (C20H14O) as a singlet oxygen (1O2) reporter, a comparison method, which can be used to measure the singlet oxygen quantum yield (ΦΔ) of the photosensitizer quantitatively, is presented in this paper. Based on this method, an automatic measuring instrument of singlet oxygen quantum yield is developed. The singlet oxygen quantum yield of the photosensitizer hermimether and aloe-emodin is measured. It is found that the measuring results are identical to the existing ones, which verifies the validity of the measuring instrument.

Ultrafast fluorescence spectroscopy via upconversion applications to biophysics.

PubMed

Xu, Jianhua; Knutson, Jay R

2008-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed.

Current advances in lanthanide ion (Ln(3+))-based upconversion nanomaterials for drug delivery.

PubMed

Yang, Dongmei; Ma, Ping'an; Hou, Zhiyou; Cheng, Ziyong; Li, Chunxia; Lin, Jun

2015-03-21

Lanthanide ion (Ln(3+))-based upconversion nano/micromaterials that emit higher-energy visible light when excited by low-energy NIR light have aroused considerable attention in the forefront of materials science and biomedical fields, which stems from their unique optical and chemical properties including minimum photodamage to living organisms, low autofluorescence, high signal-to-noise ratio and detection sensitivity, and high penetration depth in biological or environmental samples. Thus, Ln(3+)-based upconversion materials are rising new stars and are quickly emerging as potential candidates to revolutionize novel biomedical applications. In this review article, we mainly focus on the recent progress in various chemical syntheses of Ln(3+)-based upconversion nanomaterials, with special emphasis on their application in stimuli-response controlled drug release and subsequent therapy. Functional groups that are introduced into the stimuli-responsive system can respond to external triggers, such as pH, temperature, light, and even magnetic fields, which can regulate the movement of the pharmaceutical cargo and release the drug at a desired time and in a desired area. This is crucial to boost drug efficacy in cancer treatment while minimizing the side effects of cytotoxic drugs. Many multifunctional (magnetic/upconversion luminescence and porous) composite materials based on Ln(3+) have been designed for controlled drug delivery and multimodal bioimaging. Finally, the challenges and future opportunities for Ln(3+)-based upconversion materials are discussed.

Photon upconversion towards applications in energy conversion and bioimaging

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Enhanced Upconversion Luminescence in Yb3+/Tm3+-Codoped Fluoride Active Core/Active Shell/Inert Shell Nanoparticles through Directed Energy Migration

PubMed Central

Qiu, Hailong; Yang, Chunhui; Shao, Wei; Damasco, Jossana; Wang, Xianliang; Ågren, Hans; Prasad, Paras N.; Chen, Guanying

2014-01-01

The luminescence efficiency of lanthanide-doped upconversion nanoparticles is of particular importance for their embodiment in biophotonic and photonic applications. Here, we show that the upconversion luminescence of typically used NaYF4:Yb3+30%/Tm3+0.5% nanoparticles can be enhanced by ~240 times through a hierarchical active core/active shell/inert shell (NaYF4:Yb3+30%/Tm3+0.5%)/NaYbF4/NaYF4 design, which involves the use of directed energy migration in the second active shell layer. The resulting active core/active shell/inert shell nanoparticles are determined to be about 11 times brighter than that of well-investigated (NaYF4:Yb3+30%/Tm3+0.5%)/NaYF4 active core/inert shell nanoparticles when excited at ~980 nm. The strategy for enhanced upconversion in Yb3+/Tm3+-codoped NaYF4 nanoparticles through directed energy migration might have implications for other types of lanthanide-doped upconversion nanoparticles. PMID:28348285

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

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

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

2014-06-07

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

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

NASA Astrophysics Data System (ADS)

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

2011-11-01

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

Quantum Yields in Mixed-Conifer Forests and Ponderosa Pine Plantations

NASA Astrophysics Data System (ADS)

Wei, L.; Marshall, J. D.; Zhang, J.

2008-12-01

Most process-based physiological models require canopy quantum yield of photosynthesis as a starting point to simulate carbon sequestration and subsequently gross primary production (GPP). The quantum yield is a measure of photosynthetic efficiency expressed in moles of CO2 assimilated per mole of photons absorbed; the process is influenced by environmental factors. In the summer 2008, we measured quantum yields on both sun and shade leaves for four conifer species at five sites within Mica Creek Experimental Watershed (MCEW) in northern Idaho and one conifer species at three sites in northern California. The MCEW forest is typical of mixed conifer stands dominated by grand fir (Abies grandis (Douglas ex D. Don) Lindl.). In northern California, the three sites with contrasting site qualities are ponderosa pine (Pinus ponderosa C. Lawson var. ponderosa) plantations that were experimentally treated with vegetation control, fertilization, and a combination of both. We found that quantum yields in MCEW ranged from ~0.045 to ~0.075 mol CO2 per mol incident photon. However, there were no significant differences between canopy positions, or among sites or tree species. In northern California, the mean value of quantum yield of three sites was 0.051 mol CO2/mol incident photon. No significant difference in quantum yield was found between canopy positions, or among treatments or sites. The results suggest that these conifer species maintain relatively consistent quantum yield in both MCEW and northern California. This consistency simplifies the use of a process-based model to accurately predict forest productivity in these areas.

Absolute 1* quantum yields for the ICN A state by diode laser gain versus absorption spectroscopy

NASA Technical Reports Server (NTRS)

Hess, Wayne P.; Leone, Stephen R.

1987-01-01

Absolute I* quantum yields were measured as a function of wavelength for room temperature photodissociation of the ICN A state continuum. The temperature yields are obtained by the technique of time-resolved diode laser gain-versus-absorption spectroscopy. Quantum yields are evaluated at seven wavelengths from 248 to 284 nm. The yield at 266 nm is 66.0 +/- 2% and it falls off to 53.4 +/- 2% and 44.0 +/- 4% at 284 and 248 respectively. The latter values are significantly higher than those obtained by previous workers using infrared fluorescence. Estimates of I* quantum yields obtained from analysis of CN photofragment rotational distributions, as discussed by other workers, are in good agreement with the I* yields. The results are considered in conjunction with recent theoretical and experimental work on the CN rotational distributions and with previous I* yield results.

New nanoplatforms based on UCNPs linking with polyhedral oligomeric silsesquioxane (POSS) for multimodal bioimaging

NASA Astrophysics Data System (ADS)

Ge, Xiaoqian; Dong, Liang; Sun, Lining; Song, Zhengmei; Wei, Ruoyan; Shi, Liyi; Chen, Haige

2015-04-01

A new and facile method was used to transfer upconversion luminescent nanoparticles from hydrophobic to hydrophilic using polyhedral oligomeric silsesquioxane (POSS) linking on the surface of upconversion nanoparticles. In comparison with the unmodified upconversion nanoparticles, the POSS modified upconversion nanoplatforms [POSS-UCNPs(Er), POSS-UCNPs(Tm)] displayed good monodispersion in water and exhibited good water-solubility, while their particle size did not change substantially. Due to the low cytotoxicity and good biocompatibility as determined by methyl thiazolyl tetrazolium (MTT) assay and histology and hematology analysis, the POSS modified upconversion nanoplatforms were successfully applied to upconversion luminescence imaging of living cells in vitro and nude mouse in vivo (upon excitation at 980 nm). In addition, the doped Gd3+ ion endows the POSS-UCNPs with effective T1 signal enhancement and the POSS-UCNPs were successfully applied to in vivo magnetic resonance imaging (MRI) for a Kunming mouse, which makes them potential MRI positive-contrast agents. More importantly, the corner organic groups of POSS can be easily modified, resulting in kinds of POSS-UCNPs with many potential applications. Therefore, the method and results may provide more exciting opportunities for multimodal bioimaging and multifunctional applications.A new and facile method was used to transfer upconversion luminescent nanoparticles from hydrophobic to hydrophilic using polyhedral oligomeric silsesquioxane (POSS) linking on the surface of upconversion nanoparticles. In comparison with the unmodified upconversion nanoparticles, the POSS modified upconversion nanoplatforms [POSS-UCNPs(Er), POSS-UCNPs(Tm)] displayed good monodispersion in water and exhibited good water-solubility, while their particle size did not change substantially. Due to the low cytotoxicity and good biocompatibility as determined by methyl thiazolyl tetrazolium (MTT) assay and histology and hematology analysis, the POSS modified upconversion nanoplatforms were successfully applied to upconversion luminescence imaging of living cells in vitro and nude mouse in vivo (upon excitation at 980 nm). In addition, the doped Gd3+ ion endows the POSS-UCNPs with effective T1 signal enhancement and the POSS-UCNPs were successfully applied to in vivo magnetic resonance imaging (MRI) for a Kunming mouse, which makes them potential MRI positive-contrast agents. More importantly, the corner organic groups of POSS can be easily modified, resulting in kinds of POSS-UCNPs with many potential applications. Therefore, the method and results may provide more exciting opportunities for multimodal bioimaging and multifunctional applications. Electronic supplementary information (ESI) available: Schematic illustration of the formation of POSS-UCNPs. TEM images of NaYF4:Yb,Tm and NaYF4:Yb,Tm@NaGdF4 nanoparticles in cyclohexane; the TEM image of POSS-UCNPs(Tm) in water. DLS of POSS-UCNPs(Tm) in water. The energy dispersive X-ray (EDX) spectrum of POSS-UCNPs(Er). XPS of POSS-UCNPs(Er); XPS of Si element. UCL spectra of POSS-UCNPs(Er) in physiology saline as a function of time. UCL spectra of NaYF4:Yb,Tm@NaGdF4 [UCNPs(Tm)] and POSS-UCNPs(Tm), excited with a 980 nm laser (100 mW cm-2). In vivo UCL imaging of Kunming mice after intravenous injection with POSS-UCNPs(Tm) at different time points. See DOI: 10.1039/c5nr00950b

High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method.

PubMed

Yang, Weimin; Yang, Huafang; Ding, Wenhao; Zhang, Bing; Zhang, Le; Wang, Lixi; Yu, Mingxun; Zhang, Qitu

2016-11-01

Green emission ZnO quantum dots were synthesized by an ultrasonic microreactor. Ultrasonic radiation brought bubbles through ultrasonic cavitation. These bubbles built microreactor inside the microreactor. The photoluminescence properties of ZnO quantum dots synthesized with different flow rate, ultrasonic power and temperature were discussed. Flow rate, ultrasonic power and temperature would influence the type and quantity of defects in ZnO quantum dots. The sizes of ZnO quantum dots would be controlled by those conditions as well. Flow rate affected the reaction time. With the increasing of flow rate, the sizes of ZnO quantum dots decreased and the quantum yields first increased then decreased. Ultrasonic power changed the ultrasonic cavitation intensity, which affected the reaction energy and the separation of the solution. With the increasing of ultrasonic power, sizes of ZnO quantum dots first decreased then increased, while the quantum yields kept increasing. The effect of ultrasonic temperature on the photoluminescence properties of ZnO quantum dots was influenced by the flow rate. Different flow rate related to opposite changing trend. Moreover, the quantum yields of ZnO QDs synthesized by ultrasonic microreactor could reach 64.7%, which is higher than those synthesized only under ultrasonic radiation or only by microreactor. Copyright © 2016 Elsevier B.V. All rights reserved.

Ultrafast Fluorescence Spectroscopy via Upconversion: Applications to Biophysics

PubMed Central

Xu, Jianhua; Knutson, Jay R.

2012-01-01

This chapter reviews basic concepts of nonlinear fluorescence upconversion, a technique whose temporal resolution is essentially limited only by the pulse width of the ultrafast laser. Design aspects for upconversion spectrophotofluorometers are discussed, and a recently developed system is described. We discuss applications in biophysics, particularly the measurement of time-resolved fluorescence spectra of proteins (with subpicosecond time resolution). Application of this technique to biophysical problems such as dynamics of tryptophan, peptides, proteins, and nucleic acids is reviewed. PMID:19152860

Upconversion of Tm3+ ions in BaY2F8

NASA Astrophysics Data System (ADS)

Ruan, Yongfeng; Tsuboi, Taiju

1999-06-01

Up-conversion of red light with wavelength of 660 nm in Tm3+-doped BaY2F8 powder results in the two violet luminescence bands with peaks at 417 and 430 nm and two blue luminescence bands with peaks at 455 and 470 nm. The two violet bands are observed to be stronger than the blue bands. The blue luminescence is also observed by pumping with 993 nm light. The up-conversion is explained by a multiple excited state absorption process.

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

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

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

2015-03-15

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

Degradation Mechanisms in Blue Phosphorescent Organic Light-Emitting Devices by Exciton-Polaron Interactions: Loss in Quantum Yield versus Loss in Charge Balance.

PubMed

Zhang, Yingjie; Aziz, Hany

2017-01-11

We study the relative importance of deterioration of material quantum yield and charge balance to the electroluminescence stability of PHOLEDs, with a special emphasis on blue devices. Investigations show that the quantum yields of both host and emitter in the emission layer degrade due to exciton-polaron interactions and that the deterioration in material quantum yield plays the primary role in device degradation under operation. On the other hand, the results show that the charge balance factor is also affected by exciton-polaron interactions but only plays a secondary role in determining device stability. Finally, we show that the degradation mechanisms in blue PHOLEDs are fundamentally the same as those in green PHOLEDs. The limited stability of the blue devices is a result of faster deterioration in the quantum yield of the emitter.

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

NASA Astrophysics Data System (ADS)

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

2004-06-01

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

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

PubMed

Su, Fangning; Deng, Zaide

2006-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-01-01

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

Quantum Dots' Photo-luminescence Line Shape Modeling

NASA Astrophysics Data System (ADS)

Hua, Muchuan; Decca, Ricardo

Two usual phenomena observed in quantum dots (QDs) photo-luminescence (PL) spectra are line broadening and energy shift between absorption and emission peaks. They have been attributed to electron-phonon coupling and surface trapping during the PL process. Although many qualitative work describing these phenomena has been carried out, quantitative results are far less common. In this work, a semi-empirical model is introduced to simulate steady state QDs' PL processes at room temperature. It was assumed that the vast majority of radiative recombination happens from surface trapped states. Consequently, the PL line shape should be highly modulated by transition rates between states in the conduction band and between them and surface trapping states. CdSe/ZnS (core/shell) colloidal QD samples with different sizes were used to examine the model. The model was able to successfully reproduce the PL spectra of these samples even when the excitation happens within the emission spectra, giving raise to up-conversion events. This model might help understand and make more precise predictions of QDs' PL spectra and could also aid on the design of QDs' optical devices.

Ultrafast hydrogen bond dynamics and partial electron transfer after photoexcitation of diethyl ester of 7-(diethylamino)-coumarin-3-phosphonic acid and its benzoxaphosphorin analog.

PubMed

Wagner, M S; Ilieva, E D; Petkov, P St; Nikolova, R D; Kienberger, R; Iglev, H

2015-04-21

The solvation dynamics after optical excitation of two phosphono-substituted coumarin derivatives dissolved in various solutions are studied by fluorescence up-conversion spectroscopy and quantum chemical simulations. The Kamlet-Taft analysis of the conventional absorption and emission spectra suggests weakening of the solvent-solute H-bonds upon optical excitation, which is in contrast to the results gained by the quantum simulations and earlier studies reported for coumarin derivatives without phosphono groups. The simulations give evidence that the solvent reorganisation around the excited fluorophore leads to partial electron transfer to the first solvation shell. The process occurs on a timescale between 1 and 10 ps depending on the solvent polarity and leads to a fast decay of the time-resolved emission signal. Using the ultrafast spectral shift of the time-dependent fluorescence we estimated the relaxation time of the H-bonds in the electronically excited state to be about 0.6 ps in water, 1.5 ps in ethanol and 2.8 ps in formamide.

Fluorescence Quantum Yield Measurements of Fluorescent Proteins: A Laboratory Experiment for a Biochemistry or Molecular Biophysics Laboratory Course

ERIC Educational Resources Information Center

Wall, Kathryn P.; Dillon, Rebecca; Knowles, Michelle K.

2015-01-01

Fluorescent proteins are commonly used in cell biology to assess where proteins are within a cell as a function of time and provide insight into intracellular protein function. However, the usefulness of a fluorescent protein depends directly on the quantum yield. The quantum yield relates the efficiency at which a fluorescent molecule converts…

Measuring upconversion nanoparticles photoluminescence lifetime with FastFLIM and phasor plots

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Enhancing multiphoton upconversion through energy clustering at sublattice level

NASA Astrophysics Data System (ADS)

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

2014-02-01

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

Frequency upconversion in Er3+ doped tungsten tellurite glass containing Ag nanoparticles

NASA Astrophysics Data System (ADS)

Mahajan, S. K.; Parashar, J.

2018-05-01

The frequency upconversion emission in Er3+ doped TeO2-WO3-Li2O containing Ag nanoparticle (TWLEOAG) glasses at 980nm excitation is reported. The absorption spectra reveal not only the peaks due to Er3+ ions, but also the surface plasmon resonance band of silver NPs located around 525nm and 650 nm. The spherical AgNPs with average size ˜38 nm in the glassy matrix is evidenced from the TEM measurement. Under 980nm laser excitation upconversion emission spectra show two major emission at 550nm and 638nm originating from 4S3/2 and 4F9/2 energy levels of the Er3+ ions, respectively was observed. Upconversion emission enhancement factor 7 fold has been measured for sample heat treated during 40h. However for 18h heat treated TWLEOAG sample under 980 nm flash lamp excitation produced Intense green compare to red emission. Since the 980nm frequency is far from the AgNPs surface plasmon resonance frequency, visible emission ehancement is attributed to local field increase in proximity of the Ag NPs and not energy tranfer from NPs to emitters. Possible energy transfer upconversion mechanism has been also discussed.

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

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

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

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

Spectroscopy characterization and quantum yield determination of quantum dots

NASA Astrophysics Data System (ADS)

Contreras Ortiz, S. N.; Mejía Ospino, E.; Cabanzo, R.

2016-02-01

In this paper we show the characterization of two kinds of quantum dots: hydrophilic and hydrophobic, with core and core/shell respectively, using spectroscopy techniques such as UV-Vis, fluorescence and Raman. We determined the quantum yield in the quantum dots using the quinine sulphate as standard. This salt is commonly used because of its quantum yield (56%) and stability. For the CdTe excitation, we used a wavelength of 549nm and for the CdSe/ZnS excitation a wavelength of 527nm. The results show that CdSe/ZnS (49%) has better fluorescence, better quantum dots, and confirm the fluorescence result. The quantum dots have shown a good fluorescence performance, so this property will be used to replace dyes, with the advantage that quantum dots are less toxic than some dyes like the rhodamine. In addition, in this work we show different techniques to find the quantum dots emission: fluorescence spectrum, synchronous spectrum and Raman spectrum.

Limitations on the upconversion of ion sound to Langmuir turbulence

NASA Technical Reports Server (NTRS)

Vlahos, L.; Papadopoulos, K.

1982-01-01

The weak turbulence theory of Tsytovich, Stenflo and Wilhelmsson (1981) for evaluation of the nonlinear transfer of ion acoustic waves to Langmuir waves is shown to be limited in its region of validity to the level of ion acoustic waves. It is also demonstrated that, in applying the upconversion of ion sound to Langmuir waves for electron acceleration, nonlinear scattering should be self-consistently included, with a suppression of the upconversion process resulting. The impossibility of accelerating electrons by such a process for any reasonable physical system is thereby reaffirmed.

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

PubMed

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

1996-03-01

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

Increasing conversion efficiency of two-step photon up-conversion solar cell with a voltage booster hetero-interface.

PubMed

Asahi, Shigeo; Kusaki, Kazuki; Harada, Yukihiro; Kita, Takashi

2018-01-17

Development of high-efficiency solar cells is one of the attractive challenges in renewable energy technologies. Photon up-conversion can reduce the transmission loss and is one of the promising concepts which improve conversion efficiency. Here we present an analysis of the conversion efficiency, which can be increased by up-conversion in a single-junction solar cell with a hetero-interface that boosts the output voltage. We confirm that an increase in the quasi-Fermi gap and substantial photocurrent generation result in a high conversion efficiency.

Ultralow noise up-conversion detector and spectrometer for the telecom band.

PubMed

Shentu, Guo-Liang; Pelc, Jason S; Wang, Xiao-Dong; Sun, Qi-Chao; Zheng, Ming-Yang; Fejer, M M; Zhang, Qiang; Pan, Jian-Wei

2013-06-17

We demonstrate up-conversion single-photon detection for the 1550-nm telecommunications band using a PPLN waveguide, long-wavelength pump, and narrowband filtering using a volume Bragg grating. We achieve total-system detection efficiency of around 30% with noise at the dark-count level of a Silicon APD. Based on the new detector, a single-pixel up-conversion infrared spectrometer with a noise equivalent power of -142 dBm Hz(-1/2) was demonstrated, which was as good as a liquid nitrogen cooled CCD camera.

Research progress of infrared detecting and display integrated device based on infrared-visible up-conversion technology

NASA Astrophysics Data System (ADS)

Xu, Junfeng; Li, Weile; He, Bo; Wang, Haowei; Song, Yong; Yang, Shengyi; Ni, Guoqiang

2018-01-01

Infrared detecting and display device (IR-DDD) is a newly developed optical up-conversion device that integrates the light-emitting diode (LED) onto the infrared (IR) photo-detector, in order to convert IR light into the carriers photo-generated in detection materials and inject them into LED to emit visible light. This IR-DDD can achieve the direct up-conversion from IR ray to visible light, showing the considerable potential in night-vision application. This paper attempts a review of its working principle and current research progresses.

Presence of photoluminescent carbon dots in Nescafe® original instant coffee: applications to bioimaging.

PubMed

Jiang, Chengkun; Wu, Hao; Song, Xiaojie; Ma, Xiaojun; Wang, Jihui; Tan, Mingqian

2014-09-01

The presence of the carbon dots (C-dots) in food is a hotly debated topic and our knowledge about the presence and the use of carbon dots (C-dots) in food is still in its infancy. We report the finding of the presence of photoluminescent (PL) C-dots in commercial Nescafe instant coffee. TEM analysis reveals that the extracted C-dots have an average size of 4.4 nm. They were well-dispersed in water and strongly photoluminescent under the excitation of ultra-violet light with a quantum yield (QY) about 5.5%, which were also found to possess clear upconversion PL properties. X-ray photoelectron spectroscopy characterization demonstrates that the C-dots contain C, O and N three elements with the relative contents ca. 30.1, 62.2 and 7.8%. The X-ray diffraction (XRD) analysis indicates that the C-dots are amorphous. Fourier-transform infrared (FTIR) spectra were employed to characterize the surface groups of the C-dots. The C-dots show a pH independent behavior by varying the pH value from 2 to 11. The cytotoxicity study revealed that the C-dots did not cause any toxicity to cells at a concentration as high as 20 mg/mL. The C-dots have been directly applied in cells and fish imaging, which suggested that the C-dots present in commercial coffee may have more potential biological applications. Copyright © 2014. Published by Elsevier B.V.

Structure and up-conversion luminescence in sol-gel derived Er 3+-Yb 3+ co-doped SiO 2:PbF 2 nano-glass-ceramics

NASA Astrophysics Data System (ADS)

del-Castillo, J.; Yanes, A. C.; Méndez-Ramos, J.; Tikhomirov, V. K.; Rodríguez, V. D.

2009-11-01

Transparent oxyfluoride nano-glass-ceramics 90(SiO 2)10(PbF 2) co-doped with 0.3 Yb 3+ and 0.1 Er 3+ (mol%) have been prepared by thermal treatment of precursor sol-gel glasses. X-ray diffraction and high resolution transmission electron microscopy analysis pointed out a precipitation of cubic β-PbF 2 nanocrystals of certain diameter in nano-glass-ceramics varying from 10 to 20 nm depending on heat treatment conditions. The incorporation of Yb 3+ and Er 3+ dopants in these nanocrystals has been confirmed by signatures of luminescence spectroscopy. Up-conversion luminescence pumped at 980 nm has been detected. Colour tuneability of up-conversion luminescence varying pump power has been analyzed in terms of standard chromaticity diagram. This tuneability opens applications for up-conversion phosphors and three-dimensional optical recording.

Experimental demonstration of photon upconversion via cooperative energy pooling

DOE PAGES

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

2017-03-15

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

Achieving high-efficiency emission depletion nanoscopy by employing cross relaxation in upconversion nanoparticles.

PubMed

Zhan, Qiuqiang; Liu, Haichun; Wang, Baoju; Wu, Qiusheng; Pu, Rui; Zhou, Chao; Huang, Bingru; Peng, Xingyun; Ågren, Hans; He, Sailing

2017-10-20

Stimulated emission depletion microscopy provides a powerful sub-diffraction imaging modality for life science studies. Conventionally, stimulated emission depletion requires a relatively high light intensity to obtain an adequate depletion efficiency through only light-matter interaction. Here we show efficient emission depletion for a class of lanthanide-doped upconversion nanoparticles with the assistance of interionic cross relaxation, which significantly lowers the laser intensity requirements of optical depletion. We demonstrate two-color super-resolution imaging using upconversion nanoparticles (resolution ~ 66 nm) with a single pair of excitation/depletion beams. In addition, we show super-resolution imaging of immunostained cytoskeleton structures of fixed cells (resolution ~ 82 nm) using upconversion nanoparticles. These achievements provide a new perspective for the development of photoswitchable luminescent probes and will broaden the applications of lanthanide-doped nanoparticles for sub-diffraction microscopic imaging.

Experimental demonstration of photon upconversion via cooperative energy pooling

PubMed Central

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

2017-01-01

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

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

Microwave hydrothermal synthesis and upconversion properties of Yb3+/Er3+ doped YVO4 nanoparticles

NASA Astrophysics Data System (ADS)

Kshetri, Yuwaraj K.; Regmi, Chhabilal; Kim, Hak-Soo; Wohn Lee, Soo; Kim, Tae-Ho

2018-05-01

Yb3+ and Er3+ doped YVO4 (Yb3+/Er3+:YVO4) nanoparticles with highly efficient near-infrared to visible upconversion properties have been synthesized by microwave hydrothermal process. Uniform-sized Yb3+/Er3+:YVO4 nanoparticles were synthesized within 1 h at 140 °C which is relatively faster than the conventional hydrothermal process. Under 980 nm laser excitation, strong green and less strong red emissions are observed which are attributed to 2H11/2, 4S3/2 to 4I15/2 and 4F9/2 to 4I15/2 transitions of Er3+ respectively. The emission intensity is found to depend strongly on the concentration of Yb3+. The quadratic dependence of upconversion intensity on the excitation power indicates that the upconversion process is governed by two-photon absorption process.

[Up-conversion luminescent materials of Y2O3: RE(RE=Er or Er/Yb) prepared by sol-gel combustion synthesis].

PubMed

Han, Peng-de; Zhang, Le; Huang, Xiao-gu; Wang, Li-xi; Zhang, Qi-tu

2010-11-01

Y2O3 powders doped with rare-earth ions were synthesized by sol-gel combustion synthesis. Effects of different calcinating temperatures, Er+ doping concentration and Yb3+ doping concentration were investigated. It was shown that the single well crystallized Y2O3 powders could be obtained at 800 degrees C; as the calcinating temperature increased, the crystallinity and upconversion luminescence intensity were higher; the particle size was uniform around 1 microm at 900 degrees C; when Er3+ doping concentration was 1 mol%, the green upconversion luminescence intensity reached the maximum, but for red upconversion luminescence, when Er3+ doping concentration was 4 mol%, its luminescence intensity reached the maximum; as the ratio of Yb3+ to Er3+ was 4:1, the green emission intensity reached the maximum, while the red emission intensity was always increasing as Yb3+ doping concentration increased.

Microwave hydrothermal synthesis and upconversion properties of Yb3+/Er3+ doped YVO4 nanoparticles.

PubMed

Kshetri, Yuwaraj K; Regmi, Chhabilal; Kim, Hak-Soo; Lee, Soo Wohn; Kim, Tae-Ho

2018-05-18

Yb 3+ and Er 3+ doped YVO 4 (Yb 3+ /Er 3+ :YVO 4 ) nanoparticles with highly efficient near-infrared to visible upconversion properties have been synthesized by microwave hydrothermal process. Uniform-sized Yb 3+ /Er 3+ :YVO 4 nanoparticles were synthesized within 1 h at 140 °C which is relatively faster than the conventional hydrothermal process. Under 980 nm laser excitation, strong green and less strong red emissions are observed which are attributed to 2 H 11/2 , 4 S 3/2 to 4 I 15/2 and 4 F 9/2 to 4 I 15/2 transitions of Er 3+ respectively. The emission intensity is found to depend strongly on the concentration of Yb 3+ . The quadratic dependence of upconversion intensity on the excitation power indicates that the upconversion process is governed by two-photon absorption process.

Single-band upconversion nanoprobes for multiplexed simultaneous in situ molecular mapping of cancer biomarkers.

PubMed

Zhou, Lei; Wang, Rui; Yao, Chi; Li, Xiaomin; Wang, Chengli; Zhang, Xiaoyan; Xu, Congjian; Zeng, Aijun; Zhao, Dongyuan; Zhang, Fan

2015-04-24

The identification of potential diagnostic markers and target molecules among the plethora of tumour oncoproteins for cancer diagnosis requires facile technology that is capable of quantitatively analysing multiple biomarkers in tumour cells and tissues. Diagnostic and prognostic classifications of human tumours are currently based on the western blotting and single-colour immunohistochemical methods that are not suitable for multiplexed detection. Herein, we report a general and novel method to prepare single-band upconversion nanoparticles with different colours. The expression levels of three biomarkers in breast cancer cells were determined using single-band upconversion nanoparticles, western blotting and immunohistochemical technologies with excellent correlation. Significantly, the application of antibody-conjugated single-band upconversion nanoparticle molecular profiling technology can achieve the multiplexed simultaneous in situ biodetection of biomarkers in breast cancer cells and tissue specimens and produce more accurate results for the simultaneous quantification of proteins present at low levels compared with classical immunohistochemical technology.

Optical Temperature Sensor Based on Infrared Excited Green Upconversion Emission in Hexagonal Phase NaLuF4:Yb3+/Er3+ Nanorods.

PubMed

Li, Dongyu; Tian, Linlin; Huang, Zhen; Shao, Lexi; Quan, Jun; Wang, Yuxiao

2016-04-01

Hexagonal phase NaLuF4:Yb3+/Er3+ nanorods were synthesized hydrothermally. An analysis of the intense green upconversion emissions at 525 nm and 550 nm in hexagonal phase NaLuF4:Yb3/+Er3+ nanorods under excitation power density of 4.2 W/cm2 available from a diode laser emitting at 976 nm, have been undertaken. Fluorescence intensity ratio (FIR) variation of temperature-sensitive green upconversion emissions at 525 nm and 550 nm in this material was recorded in the physiological range from 295 to 343 K. The maximum sensitivity derived from the FIR technique of the green upconversion emissions is approximately 0.0044 K-1. Experimental results implied that hexagonal phase NaLuF4:Yb3/+Er3+ nanorods was a potential candidate for optical temperature sensor.

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.

Experimental demonstration of photon upconversion via cooperative energy pooling

NASA Astrophysics Data System (ADS)

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

2017-03-01

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

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

PubMed

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

2014-08-27

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

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

PubMed Central

2015-01-01

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

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

Surface-functionalized nanoparticles for biosensing and imaging-guided therapeutics

NASA Astrophysics Data System (ADS)

Jiang, Shan; Win, Khin Yin; Liu, Shuhua; Teng, Choon Peng; Zheng, Yuangang; Han, Ming-Yong

2013-03-01

In this article, the very recent progress of various functional inorganic nanomaterials is reviewed including their unique properties, surface functionalization strategies, and applications in biosensing and imaging-guided therapeutics. The proper surface functionalization renders them with stability, biocompatibility and functionality in physiological environments, and further enables their targeted use in bioapplications after bioconjugation via selective and specific recognition. The surface-functionalized nanoprobes using the most actively studied nanoparticles (i.e., gold nanoparticles, quantum dots, upconversion nanoparticles, and magnetic nanoparticles) make them an excellent platform for a wide range of bioapplications. With more efforts in recent years, they have been widely developed as labeling probes to detect various biological species such as proteins, nucleic acids and ions, and extensively employed as imaging probes to guide therapeutics such as drug/gene delivery and photothermal/photodynamic therapy.

Quantum Yields of Soluble and Particulate Material in the Ocean

DTIC Science & Technology

1999-09-30

and prospects. IEEE Transactions, 46(5): 825-829 In Press Moisan, T.A. & B.G. Mitchell UV Absorption by Mycosporine - like Amino Acids in Phaeocystis...were grown to evaluate the spectral quantum yield of in vivo chlorophyll a fluorescence. We determined that mycosporine amino acids with UV absorption...evaluate the role of photoprotective pigments, including mycosporine amino acids and the xanthophyll pigments in Phaeocystis, on the spectral quantum yield

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

NASA Astrophysics Data System (ADS)

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

2006-08-01

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

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

PubMed

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

2012-04-01

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

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

NASA Astrophysics Data System (ADS)

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

1995-04-01

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

Advances in highly doped upconversion nanoparticles.

PubMed

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

2018-06-20

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

The effect of micro-structure on upconversion luminescence of Nd3+/Yb3+ co-doped La2O3-TiO2-ZrO2 glass-ceramics

NASA Astrophysics Data System (ADS)

Zhang, Minghui; Wen, Haiqin; Pan, Xiuhong; Yu, Jianding; Jiang, Meng; Yu, Huimei; Tang, Meibo; Gai, Lijun; Ai, Fei

2018-03-01

Nd3+/Yb3+ co-doped La2O3-TiO2-ZrO2 glasses have been prepared by aerodynamic levitation method. The glasses show high refractive index of 2.28 and Abbe number of 18.3. Glass-ceramics heated at 880 °C for 50 min perform the strongest upconversion luminescence. X-ray diffraction patterns of glass-ceramics with different depths indicate that rare earth ions restrain crystallization. Body crystallization mechanism mixed with surface crystallization is confirmed in the heat treatment. Surface crystals achieve priority to grow, resulting in important effects on upconversion luminescence. The results of atomic force microscope and scanning electron microscope indicate that crystal particles with uniform size distribute densely and homogenously on the surface and large amount of glass matrix exists in the glass ceramics heated at 880 °C for 50 min. Crystals in the glass-ceramics present dense structure and strong boundaries, which can reduce the mutual nonradiative relaxation rate among rare earth ions and then improve upconversion luminescence effectively. Based on micro-structural study, the mechanism that upconversion luminescence can be improved by heat treatment has been revealed. The results of micro-structural analysis agree well with the spectra.

Perspectives and challenges of photon-upconversion nanoparticles - Part I: routes to brighter particles and quantitative spectroscopic studies.

PubMed

Resch-Genger, Ute; Gorris, Hans H

2017-10-01

Lanthanide-doped photon-upconversion nanoparticles (UCNPs) have been the focus of many research activities in materials and life sciences in the last 15 years because of their potential to convert light between different spectral regions and their unique photophysical properties. To fully exploit the application potential of these fascinating nanomaterials, a number of challenges have to be overcome, such as the low brightness, particularly of small UCNPs, and the reliable quantification of the excitation-power-density-dependent upconversion luminescence. In this series of critical reviews, recent developments in the design, synthesis, optical-spectroscopic characterization, and application of UCNPs are presented with special focus on bioanalysis and the life sciences. Here we guide the reader from the synthesis of UCNPs to different concepts to enhance their luminescence, including the required optical-spectroscopic assessment to quantify material performance; surface modification strategies and bioanalytical applications as well as selected examples of the use of UCNPs as reporters in different assay formats are addressed in part II. Future trends and challenges in the field of upconversion are discussed with special emphasis on UCNP synthesis and material characterization, particularly quantitative luminescence studies. Graphical Abstract Both synthesis and spectroscopy as well bioanalytical applications of UCNPs are driven and supported by COST Action CM1403 "The European Upconversion Network".

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

NASA Astrophysics Data System (ADS)

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

2015-03-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-07-01

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

Triplet photosensitizers: from molecular design to applications.

PubMed

Zhao, Jianzhang; Wu, Wanhua; Sun, Jifu; Guo, Song

2013-06-21

Triplet photosensitizers (PSs) are compounds that can be efficiently excited to the triplet excited state which subsequently act as catalysts in photochemical reactions. The name is originally derived from compounds that were used to transfer the triplet energy to other compounds that have only a small intrinsic triplet state yield. Triplet PSs are not only used for triplet energy transfer, but also for photocatalytic organic reactions, photodynamic therapy (PDT), photoinduced hydrogen production from water and triplet-triplet annihilation (TTA) upconversion. A good PS should exhibit strong absorption of the excitation light, a high yield of intersystem crossing (ISC) for efficient production of the triplet state, and a long triplet lifetime to allow for the reaction with a reactant molecule. Most transition metal complexes show efficient ISC, but small molar absorption coefficients in the visible spectral region and short-lived triplet excited states, which make them unsuitable as triplet PSs. One obstacle to the development of new triplet PSs is the difficulty in predicting the ISC of chromophores, especially of organic compounds without any heavy atoms. This review article summarizes some molecular design rationales for triplet PSs, based on the molecular structural factors that facilitate ISC. The design of transition metal complexes with large molar absorption coefficients in the visible spectral region and long-lived triplet excited states is presented. A new method of using a spin converter to construct heavy atom-free organic triplet PSs is discussed, with which ISC becomes predictable, C60 being an example. To enhance the performance of triplet PSs, energy funneling based triplet PSs are proposed, which show broadband absorption in the visible region. Applications of triplet PSs in photocatalytic organic reactions, hydrogen production, triplet-triplet annihilation upconversion and luminescent oxygen sensing are briefly introduced.

[Fluorescence spectra and quantum yield of TiO2 nanocrystals synthesized by alcohothermal method].

PubMed

Song, Cui-Hong; Li, Yan-Ting; Li, Jing; Wei, Yong-Ju; Hu, Yu-Zhu; Wei, Yu

2008-01-01

Fluorescence spectra and fluorescence quantum yield of TiO2 nanocrystals were studied. Using tetra n-butyl titanate as a starting material, a facile alcohothermal technique was used to synthesize TiO2 nanocrystals. As can be seen from the transmittance electron microscopy (TEM) image, TiO2 nanocrystals with a relatively uniform particle size distribution of < 10 nm are present in the transparent sol. The transparent sol presents a strong stable fluorescence emission with a maximum at 450 nm, which is greatly dependent on the size quantization effects, defect energy level and the surface state of TiO2 nanocrystals. The quantum yield (gamma) of TiO2 was determined by the relative comparison procedure, using freshly prepared analytical purity quinine sulfate in 0.05 mol x L(-1) H2SO4 as a relative quantum yield standard. The emission quantum yield of TiO2 nanocrystals prepared in alcoholic media was calculated to be about 0.20 at wavelengths ranging from 330 to 370 nm, which was much higher than the values reported in previous works. So, it is supposed that nano-TiO2 will be applied as a potential quantum dots fluorescence probe in biological analysis.

Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals

DOE PAGES

Miller, Joseph B.; Van Sickle, Austin R.; Anthony, Rebecca J.; ...

2012-07-18

Here, we report on the quantum yield, photoluminescence (PL) lifetime and ensemble photoluminescent stability of highly monodisperse plasma-synthesized silicon nanocrystals (SiNCs) prepared though density-gradient ultracentrifugation in mixed organic solvents. Improved size uniformity leads to a reduction in PL line width and the emergence of entropic order in dry nanocrystal films. We find excellent agreement with the anticipated trends of quantum confinement in nanocrystalline silicon, with a solution quantum yield that is independent of nanocrystal size for the larger fractions but decreases dramatically with size for the smaller fractions. We also find a significant PL enhancement in films assembled from themore » fractions, and we use a combination of measurement, simulation and modeling to link this ‘brightening’ to a temporally enhanced quantum yield arising from SiNC interactions in ordered ensembles of monodisperse nanocrystals. Using an appropriate excitation scheme, we exploit this enhancement to achieve photostable emission.« less

Aeronomical determinations of the quantum yields of O (1S) and O (1D) from dissociative recombination of O2(+)

NASA Technical Reports Server (NTRS)

Yee, Jeng-Hwa; Abreu, Vincent J.; Colwell, William B.

1989-01-01

Data from the visible-airglow experiment on the Atmosphere Explorer-E satellite have been used to determine the quantum yields of O (1S) and O (1D) from the dissociative recombination of O2(+) based on a constant total recombination rate from each vibrational level. A range of values between 0.05 and 0.18 has been obtained for the quantum yield of O (1S) and shows a positive correlation with the extent of the vibrational excitation of O2(+). The quantum yield of O (1D) has been measured to be 0.9 + or - 0.2, with no apparent dependence on the vibrational distribution of O2(+).

Tuning Single Quantum Dot Emission with a Micromirror.

PubMed

Yuan, Gangcheng; Gómez, Daniel; Kirkwood, Nicholas; Mulvaney, Paul

2018-02-14

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

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

NASA Astrophysics Data System (ADS)

Sobczyk, Marcin

2013-04-01

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

NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} core/shell nanocomposite: A highly efficient visible-light-driven photocatalyst utilizing upconversion

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

Sun, Yuanyuan; Wang, Wenzhong, E-mail: wzwang@mail.sic.ac.cn; Sun, Songmei

2014-04-01

Highlights: • Design and synthesis of NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} based on upconversion. • NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} nanocomposite was prepared for the first time. • Core–shell structure benefits the properties. • Upconversion contributed to the enhanced photocatalytic activity. • Helps to understand the functionality of new type photocatalysts. - Abstract: NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} core/shell nanocomposite was designed and prepared for the first time based on upconversion. The products were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution TEM (HRTEM), energy dispersive X-ray spectroscopy (EDS) and diffuse reflectance spectra (DRS). The results revealed that the as-synthesizedmore » NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} consisted of spheres with a core diameter of about 26 nm and a shell diameter of around 6 nm. The core was upconversion illuminant NaYF{sub 4}:Er,Yb and the shell was Bi{sub 2}MoO{sub 6} around the core, which was confirmed by EDS. The NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} exhibited higher photocatalytic activity for the photodecomposition of Rhodamine B (RhB) under the irradiation of Xe lamp and green light emitting diode (g-LED). The mechanism of the high photocatalytic activity was discussed by photoluminescence spectra (PL), which is mainly attributed to upconversion of NaYF{sub 4}:Er,Yb in the NaYF{sub 4}:Er,Yb/Bi{sub 2}MoO{sub 6} nanocomposite and the core–shell structure.« less

Orbital angular momentum light frequency conversion and interference with quasi-phase matching crystals.

PubMed

Zhou, Zhi-Yuan; Ding, Dong-Sheng; Jiang, Yun-Kun; Li, Yan; Shi, Shuai; Wang, Xi-Shi; Shi, Bao-Sen

2014-08-25

Light with helical phase structures, carrying quantized orbital angular momentum (OAM), has many applications in both classical and quantum optics, such as high-capacity optical communications and quantum information processing. Frequency conversion is a basic technique to expand the frequency range of the fundamental light. The frequency conversion of OAM-carrying light gives rise to new physics and applications such as up-conversion detection of images and generation of high dimensional OAM entanglements. Quasi-phase matching (QPM) nonlinear crystals are good candidates for frequency conversion, particularly due to their high-valued effective nonlinear coefficients and no walk-off effect. Here we report the first experimental second-harmonic generation (SHG) of an OAM-carried light with a QPM crystal, where a UV light with OAM of 100 ℏ is generated. OAM conservation is verified using a specially designed interferometer. With a pump beam carrying an OAM superposition of opposite sign, we observe interesting interference phenomena in the SHG light; specifically, a photonics gear-like structure is obtained that gives direct evidence of OAM conservation, which will be very useful for ultra-sensitive angular measurements. Besides, we also develop a theory to reveal the underlying physics of the phenomena. The methods and theoretical analysis shown here are also applicable to other frequency conversion processes, such as sum frequency generation and difference-frequency generation, and may also be generalized to the quantum regime for single photons.

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

NIR-to-visible upconversion nanoparticles for fluorescent labeling and targeted delivery of siRNA

NASA Astrophysics Data System (ADS)

Jiang, Shan; Zhang, Yong; Lim, Kian Meng; Sim, Eugene K. W.; Ye, Lei

2009-04-01

Near-infrared (NIR)-to-visible upconversion fluorescent nanoparticles were synthesized and used for imaging and targeted delivery of small interfering RNA (siRNA) to cancer cells. Silica-coated NaYF4 upconversion nanoparticles (UCNs) co-doped with lanthanide ions (Yb/Er) were synthesized. Folic acid and anti-Her2 antibody conjugated UCNs were used to fluorescently label the folate receptors of HT-29 cells and Her2 receptors of SK-BR-3 cells, respectively. The intracellular uptake of the folic acid and antibody conjugated UCNs was visualized using a confocal fluorescence microscope equipped with an NIR laser. siRNA was attached to anti-Her2 antibody conjugated UCNs and the delivery of these nanoparticles to SK-BR-3 cells was studied. Meanwhile, a luciferase assay was established to confirm the gene silencing effect of siRNA. Upconversion nanoparticles can serve as a fluorescent probe and delivery system for simultaneous imaging and delivery of biological molecules.

Self-assembly of an upconverting nanocomplex and its application to turn-on detection of metalloproteinase-9 in living cells

NASA Astrophysics Data System (ADS)

Nguyen, Phuong-Diem; Thanh Cong, Vu; Baek, Changyoon; Min, Junhong

2016-10-01

Upcoversion nanoparticles are an emerging luminescent nanomaterial with excellent photophysical properties that have great benefits in biological sensing. In this study, a luminescent turn-on biosensor for cell-secreted protease activity assay is established based on resonance energy transfer in an upconversion nanoparticle-graphene oxide nano-assembly. The proposed biosensor consists of a blue-emitting upconversion nanoparticle covered with a quenching complex, comprising gelatin as the proteinase substrate and graphene oxide nanosheets as luminescence acceptors. After enzymatic digestion, the upconversion nanoparticles lose the gelatin cover due to the disassembly of the quenching complex, thus the upconverting luminescence in the blue region is restored (a turn-on response). The recovered upconverting luminescence is proportional to the protease concentration; the limit of detection was 12 ng ml-1. Finally, the upconversion-graphene oxide nanocomplex was successfully applied in the detection of cell-secreted protease-metalloproteinase in MCF-7 cancer cells with high sensitivity and specificity.

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

NASA Astrophysics Data System (ADS)

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

2018-07-01

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

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

PubMed

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

2018-05-11

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

Solvent Dependency in the Quantum Efficiency of 4-[(4-Aminophenyl)-(4-imino-1-cyclohexa-2, 5- dienylidene) methyl] Aniline Hydrochloride.

PubMed

Pathrose, Bini; Nampoori, V P N; Radhakrishnan, P; Sahira, H; Mujeeb, A

2015-05-01

In the present work dual beam thermal lens technique is used for studying the solvent dependency on the quantum efficiency of a novel dye used for biomedical applications. The role of solvent in the absolute fluorescence quantum yield of 4-[(4-Aminophenyl)-(4-imino-1-cyclohexa-2, 5- dienylidene) methyl] aniline hydrochloride is studied using thermal lens technique. It is observed that the variation in solvents and its concentration results considerable variations in the fluorescence quantum yield. These variations are due to the non-radiative relaxation of the absorbed energy and because of the different solvent properties. The highest quantum yield of the dye is observed in the polar protic solvent-water.

In Search of the Perfect Photocage: Structure-Reactivity Relationships in meso-Methyl BODIPY Photoremovable Protecting Groups.

PubMed

Slanina, Tomáš; Shrestha, Pradeep; Palao, Eduardo; Kand, Dnyaneshwar; Peterson, Julie A; Dutton, Andrew S; Rubinstein, Naama; Weinstain, Roy; Winter, Arthur H; Klán, Petr

2017-10-25

A detailed investigation of the photophysical parameters and photochemical reactivity of meso-methyl BODIPY photoremovable protecting groups was accomplished through systematic variation of the leaving group (LG) and core substituents as well as substitutions at boron. Efficiencies of the LG release were evaluated using both steady-state and transient absorption spectroscopies as well as computational analyses to identify the optimal structural features. We find that the quantum yields for photorelease with this photocage are highly sensitive to substituent effects. In particular, we find that the quantum yields of photorelease are improved with derivatives with higher intersystem crossing quantum yields, which can be promoted by core heavy atoms. Moreover, release quantum yields are dramatically improved by boron alkylation, whereas alkylation in the meso-methyl position has no effect. Better LGs are released considerably more efficiently than poorer LGs. We find that these substituent effects are additive, for example, a 2,6-diiodo-B-dimethyl BODIPY photocage features quantum yields of 28% for the mediocre LG acetate and a 95% quantum yield of release for chloride. The high chemical and quantum yields combined with the outstanding absorption properties of BODIPY dyes lead to photocages with uncaging cross sections over 10 000 M -1 cm -1 , values that surpass cross sections of related photocages absorbing visible light. These new photocages, which absorb strongly near the second harmonic of an Nd:YAG laser (532 nm), hold promise for manipulating and interrogating biological and material systems with the high spatiotemporal control provided by pulsed laser irradiation, while avoiding the phototoxicity problems encountered with many UV-absorbing photocages. More generally, the insights gained from this structure-reactivity relationship may aid in the development of new highly efficient photoreactions.

Quantum yield measurements of light-induced H₂ generation in a photosystem I-[FeFe]-H₂ase nanoconstruct.

PubMed

Applegate, Amanda M; Lubner, Carolyn E; Knörzer, Philipp; Happe, Thomas; Golbeck, John H

2016-01-01

The quantum yield for light-induced H2 generation was measured for a previously optimized bio-hybrid cytochrome c 6-crosslinked PSI(C13G)-1,8-octanedithiol-[FeFe]-H2ase(C97G) (PSI-H2ase) nanoconstruct. The theoretical quantum yield for the PSI-H2ase nanoconstruct is 0.50 molecules of H2 per photon absorbed, which equates to a requirement of two photons per H2 generated. Illumination of the PSI-H2ase nanoconstruct with visible light between 400 and 700 nm resulted in an average quantum yield of 0.10-0.15 molecules of H2 per photon absorbed, which equates to a requirement of 6.7-10 photons per H2 generated. A possible reason for the difference between the theoretical and experimental quantum yield is the occurrence of non-productive PSI(C13G)-1,8-octanedithiol-PSIC13G (PSI-PSI) conjugates, which would absorb light without generating H2. Assuming the thiol-Fe coupling is equally efficient at producing PSI-PSI conjugates as well as in producing PSI-H2ase nanoconstructs, the theoretical quantum yield would decrease to 0.167 molecules of H2 per photon absorbed, which equates to 6 photons per H2 generated. This value is close to the range of measured values in the current study. A strategy that purifies the PSI-H2ase nanoconstructs from the unproductive PSI-PSI conjugates or that incorporates different chemistries on the PSI and [FeFe]-H2ase enzyme sites could potentially allow the PSI-H2ase nanoconstruct to approach the expected theoretical quantum yield for light-induced H2 generation.

Photogeneration of reactive transient species upon irradiation of natural water samples: Formation quantum yields in different spectral intervals, and implications for the photochemistry of surface waters.

PubMed

Marchisio, Andrea; Minella, Marco; Maurino, Valter; Minero, Claudio; Vione, Davide

2015-04-15

Chromophoric dissolved organic matter (CDOM) in surface waters is a photochemical source of several transient species such as CDOM triplet states ((3)CDOM*), singlet oxygen ((1)O2) and the hydroxyl radical (OH). By irradiation of lake water samples, it is shown here that the quantum yields for the formation of these transients by CDOM vary depending on the irradiation wavelength range, in the order UVB > UVA > blue. A possible explanation is that radiation at longer wavelengths is preferentially absorbed by the larger CDOM fractions, which show lesser photoactivity compared to smaller CDOM moieties. The quantum yield variations in different spectral ranges were definitely more marked for (3)CDOM* and OH compared to (1)O2. The decrease of the quantum yields with increasing wavelength has important implications for the photochemistry of surface waters, because long-wavelength radiation penetrates deeper in water columns compared to short-wavelength radiation. The average steady-state concentrations of the transients ((3)CDOM*, (1)O2 and OH) were modelled in water columns of different depths, based on the experimentally determined wavelength trends of the formation quantum yields. Important differences were found between such modelling results and those obtained in a wavelength-independent quantum yield scenario. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

Syamchand, Sasidharanpillai S.; George, Sony

2016-12-01

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

Quantum Yield Heterogeneity among Single Nonblinking Quantum Dots Revealed by Atomic Structure-Quantum Optics Correlation

DOE PAGES

Orfield, Noah J.; McBride, James R.; Wang, Feng; ...

2016-02-05

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging,more » rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.« less

Ultrafast exciton dynamics in cadmium selenide nanocrystals determined by femtosecond fluorescence upconversion spectroscopy

NASA Astrophysics Data System (ADS)

Underwood, David Frederick

Femtosecond fluorescence upconversion spectroscopy is a technique that allows the unambiguous determination of the excited state dynamics of an analyte. Combining this method with the use of tunable laser excitation, the exciton dynamics in semiconducting nanocrystals (NC's) of cadmium selenide (CdSe) have been determined, devoid of the complications arising from more common spectroscopic methods such as pump-probe. The results of this investigation were used to construct a model to fully describe the three-level system comprising of the valence and conduction bands and surface states, which have been calculated by others to lie mid-gap in energy. Smaller NC's showed faster decay components due to increased interaction between the exciton and surface states. The deep trap emission, which has never before been measured by ultrafast fluorescence techniques, shows a rapid rise time (˜2 ps), which is attributed to surface selenium dangling bonds relaxing to the valence band and radiatively combining with the photo-generated hole. The band edge fluorescence decays as the deep trap emission grows in, inherently coupling the two processes. An experiment which measured the dependence of the excitation energy showed that increased energy imparted to the NC's resulted in increased rise times, yielding the timescales for exciton relaxation through the valence and conduction band states to the lowest emitting state. Surface-oxidized and normally-passivated NC's display the same decay dynamics in time but differ in relative amplitude; the latter point agrees with steady-state measurements. The rotational anisotrophy of the NC's was measured and agrees with previous pump-probe data. Upconversion on the red and blue sides of the static fluorescence spectrum showed no discernable differences, which is either and inherent limitation of the experimental apparatus, or the possibility that lower-lying triplet states are populated on a timescale below the instrument resolution.

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

PubMed

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

2011-11-04

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

Integrated optical modulator for signal up-conversion over radio-on-fiber link.

PubMed

Kim, Woo-Kyung; Kwon, Soon-Woo; Jeong, Woo-Jin; Son, Geun-Sik; Lee, Kwang-Hyun; Choi, Woo-Young; Yang, Woo-Seok; Lee, Hyung-Man; Lee, Han-Young

2009-02-16

An integrated optical modulator, which consists of a dual-sideband suppressed carrier (DSB-SC) modulator cascaded with a single-sideband (SSB) modulator, is proposed for signal up-conversion over Radio-on-Fiber. Utilizing a single-drive domain inverted structure in both modulators, balanced modulations were obtained without complicated radio frequency (RF) driving circuits and delicate RF phase adjustments. Intermediate frequency (IF) band signal was up-conversed to 60GHz band by using the fabricated device and was transmitted over optical fiber. Experiment results show that the proposed device enables millimeter wave generation and signal transmission without any power penalty caused by chromatic dispersion.

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

NASA Astrophysics Data System (ADS)

Qiu, Jianbei; Kawamoto, Yoji; Zhang, Junjie

2002-11-01

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

[Two-photon up-conversion fluorescence of a neodymium organic framework Nd(BTC)].

PubMed

Xu, Hui; Jin, Run-zhi; Wu, Chun-yang; Yang, Yu; Qian, Guo-dong

2008-08-01

In the present work, a neodymium organic framework Nd(BTC) was synthesized by the solvothermal reaction of Nd(NO3)3 x 5H2O and H3BTC (BTC = 1,3,5-benzenetricarboxylate) in mixed solvents of DMF, ethanol and water, and was identified by elemental analysis. This MOF complex was characterized using X-ray diffraction (XRD), thermogravimetry-differential scanning calorimetry (TGA-DSC) analysis, UV-visible absorption spectra and fluorescence spectra. This polycrystalline powder lost DMF and H2O when heated to 120 degrees C, then remained stable till the temperature reached 500 degrees C. Near infrared fluorescence at 1064 nm due to the 4 F3/2--> 4 I11/2 transition of Nd3+ ions was exhibited when excited by 808 nm laser beam. It was also been found that up-conversion fluorescence of Nd(BTC) peaked at about 450 nm due to 2 D5/2 -->4 I11/2 transition of Nd3+ ions can be observed under the excitation of a 580 nm laser line. The mechanism of the up-conversion fluorescence of Nd(BTC) at around 450 nm under the excitation of 580 nm laser can be ascribed to both excited-state absorption and energy transfer up-conversion. This result indicated that such MOF can be employed as an up-conversion luminescence material in many potential application areas such as bio-labeling and fluorescence image.

The Broken Ring: Reduced Aromaticity in Lys-Trp Cations and High pH Tautomer Correlates with Lower Quantum Yield and Shorter Lifetimes

PubMed Central

2015-01-01

Several nonradiative processes compete with tryptophan fluorescence emission. The difficulty in spectral interpretation lies in associating specific molecular environmental features with these processes and thereby utilizing the fluorescence spectral data to identify the local environment of tryptophan. Here, spectroscopic and molecular modeling study of Lys-Trp dipeptide charged species shows that backbone-ring interactions are undistinguished. Instead, quantum mechanical ground state isosurfaces reveal variations in indole π electron distribution and density that parallel charge (as a function of pK1, pK2, and pKR) on the backbone and residues. A pattern of aromaticity-associated quantum yield and fluorescence lifetime changes emerges. Where quantum yield is high, isosurfaces have a charge distribution similar to the highest occupied molecular orbital (HOMO) of indole, which is the dominant fluorescent ground state of the 1La transition dipole moment. Where quantum yield is low, isosurface charge distribution over the ring is uneven, diminished, and even found off ring. At pH 13, the indole amine is deprotonated, and Lys-Trp quantum yield is extremely low due to tautomer structure that concentrates charge on the indole amine; the isosurface charge distribution bears scant resemblance to the indole HOMO. Such greatly diminished fluorescence has been observed for proteins where the indole nitrogen is hydrogen bonded, lending credence to the association of aromaticity changes with diminished quantum yield in proteins as well. Thus tryptophan ground state isosurfaces are an indicator of indole aromaticity, signaling the partition of excitation energy between radiative and nonradiative processes. PMID:24882092

Primary quantum yields of NO2 photodissociation

NASA Technical Reports Server (NTRS)

Gardner, Edward P.; Sperry, Paul D.; Calvert, Jack G.

1987-01-01

The quantum yields of formation of NO, O2, and NO2 loss are measured for NO2 vapor at low pressures (0.13-0.30 torr) irradiated at 334-405 nm wavelengths and temperature in the range 273-370 K in order to study the primary quantum efficiencies of NO2 photodecomposition. The temperature and wavelength dependences of the primary quantum efficiencies are examined. It is observed that the primary quantum efficiencies increase rapidly from near zero at 424 nm to near unity for excitation at wavelengths less than 394 nm. The theory of Pitts et al. (1964) that the energy deficiency for photodissociation of NO2 excited at wavelengths greater than 397.9 nm is due to the rotational and vibrational energy of the NO2 molecules is confirmed by the data. Values for the primary quantum yields of NO2 photodecomposition as a function of wavelength are presented.

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…

Photosensitized electron transfer processes in SiO2 colloids and sodium lauryl sulfate micellar systems: Correlation of quantum yields with interfacial surface potentials

PubMed Central

Laane, Colja; Willner, Itamar; Otvos, John W.; Calvin, Melvin

1981-01-01

The effectiveness of negatively charged colloidal SiO2 particles in controlling photosensitized electron transfer reactions has been studied and compared with that of the negatively charged sodium lauryl sulfate (NaLauSO4) micellar system. In particular, the photosensitized reduction of the zwitterionic electron acceptor propylviologen sulfonate (PVS0) with tris(2,2′-bipyridinium)ruthenium(II) [Ru(bipy)32+] as the sensitizer and triethanolamine as the electron donor is found to have a quantum yield of 0.033 for formation of the radical anion (PVS[unk]) in the SiO2 colloid compared with 0.005 in the homogeneous system and 0.0086 in a NaLauSO4 micellar solution. The higher quantum yields obtained with the SiO2 colloidal system are attributed to substantial stabilization against back reaction of the intermediate photoproducts—i.e., Ru(bipy)33+ and PVS[unk]—by electrostatic repulsion of the reduced electron acceptor from the negatively charged particle surface. The binding properties of the SiO2 particles and NaLauSO4 micelles were investigated by flow dialysis. The results show that the sensitizer binds to both interfaces and that the SiO2 interface is characterized by a much higher surface potential than the micellar interface (≈-170 mV vs. -85 mV). The effect of ionic strength on the surface potential was estimated from the Gouy-Chapman theory, and the measured quantum yields of photosensitized electron transfer were correlated with surface potential at different ionic strengths. This correlation shows that the quantum yield is not affected by surface potentials smaller than ≈-40 mV. At larger potentials, the quantum yield increases rapidly. The quantum yield obtained in the micellar system at different strengths fits nicely on the correlation curve for the colloid SiO2 system. These results indicate that the surface potential is the dominant factor in the quantum yield improvement for PVS0 reduction. PMID:16593095

A paper-based resonance energy transfer nucleic acid hybridization assay using upconversion nanoparticles as donors and quantum dots as acceptors.

PubMed

Doughan, Samer; Uddayasankar, Uvaraj; Krull, Ulrich J

2015-06-09

Monodisperse aqueous upconverting nanoparticles (UCNPs) were covalently immobilized on aldehyde modified cellulose paper via reduction amination to develop a luminescence resonance energy transfer (LRET)-based nucleic acid hybridization assay. This first account of covalent immobilization of UCNPs on paper for a bioassay reports an optically responsive method that is sensitive, reproducible and robust. The immobilized UCNPs were decorated with oligonucleotide probes to capture HPRT1 housekeeping gene fragments, which in turn brought reporter conjugated quantum dots (QDs) in close proximity to the UCNPs for LRET. This sandwich assay could detect unlabeled oligonucleotide target, and had a limit of detection of 13 fmol and a dynamic range spanning nearly 3 orders of magnitude. The use of QDs, which are excellent LRET acceptors, demonstrated improved sensitivity, limit of detection, dynamic range and selectivity compared to similar assays that have used molecular fluorophores as acceptors. The selectivity of the assay was attributed to the decoration of the QDs with polyethylene glycol to eliminate non-specific adsorption. The kinetics of hybridization were determined to be diffusion limited and full signal development occurred within 3 min. Copyright © 2015 Elsevier B.V. All rights reserved.

Fluorescent Nanomaterials for the Development of Latent Fingerprints in Forensic Sciences

PubMed Central

Li, Ming; Yu, Aoyang; Zhu, Ye

2018-01-01

This review presents an overview on the application of latent fingerprint development techniques in forensic sciences. At present, traditional developing methods such as powder dusting, cyanoacrylate fuming, chemical method, and small particle reagent method, have all been gradually compromised given their emerging drawbacks such as low contrast, sensitivity, and selectivity, as well as high toxicity. Recently, much attention has been paid to the use of fluorescent nanomaterials including quantum dots (QDs) and rare earth upconversion fluorescent nanomaterials (UCNMs) due to their unique optical and chemical properties. Thus, this review lays emphasis on latent fingerprint development based on QDs and UCNMs. Compared to latent fingerprint development by traditional methods, the new methods using fluorescent nanomaterials can achieve high contrast, sensitivity, and selectivity while showing reduced toxicity. Overall, this review provides a systematic overview on such methods. PMID:29657570

Electro Optical Properties of Copolymer Blends: Lasing, Electroluminescence and Photophysics

DTIC Science & Technology

2006-04-15

conjugated main chain structures with high photoluminescent and electroluminescent quantum yields. The structures incorporated fluorene containing moieties...The systems studied focused on novel conjugated main chain structures with high photoluminescent and electroluminescent quantum yields. The structures...the quantum efficient fluorine group. The properties of segmented copolymers that incorporate fluorenes were compared to the homo-PPV type systems

Multicolor tunability and upconversion enhancement of fluoride nanoparticles by oxygen dopant

NASA Astrophysics Data System (ADS)

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

2013-08-01

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

A versatile method for the determination of photochemical quantum yields via online UV-Vis spectroscopy.

PubMed

Stadler, Eduard; Eibel, Anna; Fast, David; Freißmuth, Hilde; Holly, Christian; Wiech, Mathias; Moszner, Norbert; Gescheidt, Georg

2018-05-16

We have developed a simple method for determining the quantum yields of photo-induced reactions. Our setup features a fibre coupled UV-Vis spectrometer, LED irradiation sources, and a calibrated spectrophotometer for precise measurements of the LED photon flux. The initial slope in time-resolved absorbance profiles provides the quantum yield. We show the feasibility of our methodology for the kinetic analysis of photochemical reactions and quantum yield determination. The typical chemical actinometers, ferrioxalate and ortho-nitrobenzaldehyde, as well as riboflavin, a spiro-compound, phosphorus- and germanium-based photoinitiators for radical polymerizations and the frequently utilized photo-switch azobenzene serve as paradigms. The excellent agreement of our results with published data demonstrates the high potential of the proposed method as a convenient alternative to the time-consuming chemical actinometry.

Fluorescence quantum yield measurements of fluorescent proteins: a laboratory experiment for a biochemistry or molecular biophysics laboratory course.

PubMed

Wall, Kathryn P; Dillon, Rebecca; Knowles, Michelle K

2015-01-01

Fluorescent proteins are commonly used in cell biology to assess where proteins are within a cell as a function of time and provide insight into intracellular protein function. However, the usefulness of a fluorescent protein depends directly on the quantum yield. The quantum yield relates the efficiency at which a fluorescent molecule converts absorbed photons into emitted photons and it is necessary to know for assessing what fluorescent protein is the most appropriate for a particular application. In this work, we have designed an upper-level, biochemistry laboratory experiment where students measure the fluorescence quantum yields of fluorescent proteins relative to a standard organic dye. Four fluorescent protein variants, enhanced cyan fluorescent protein (ECFP), enhanced green fluorescent protein (EGFP), mCitrine, and mCherry, were used, however the methods described are useful for the characterization of any fluorescent protein or could be expanded to fluorescent quantum yield measurements of organic dye molecules. The laboratory is designed as a guided inquiry project and takes two, 4 hr laboratory periods. During the first day students design the experiment by selecting the excitation wavelength, choosing the standard, and determining the concentration needed for the quantum yield experiment that takes place in the second laboratory period. Overall, this laboratory provides students with a guided inquiry learning experience and introduces concepts of fluorescence biophysics into a biochemistry laboratory curriculum. © 2014 The International Union of Biochemistry and Molecular Biology.

Photochemical redox reactions of copper(II)-alanine complexes in aqueous solutions.

PubMed

Lin, Chen-Jui; Hsu, Chao-Sheng; Wang, Po-Yen; Lin, Yi-Liang; Lo, Yu-Shiu; Wu, Chien-Hou

2014-05-19

The photochemical redox reactions of Cu(II)/alanine complexes have been studied in deaerated solutions over an extensive range of pH, Cu(II) concentration, and alanine concentration. Under irradiation, the ligand-to-metal charge transfer results in the reduction of Cu(II) to Cu(I) and the concomitant oxidation of alanine, which produces ammonia and acetaldehyde. Molar absorptivities and quantum yields of photoproducts for Cu(II)/alanine complexes at 313 nm are characterized mainly with the equilibrium Cu(II) speciation where the presence of simultaneously existing Cu(II) species is taken into account. By applying regression analysis, individual Cu(I) quantum yields are determined to be 0.094 ± 0.014 for the 1:1 complex (CuL) and 0.064 ± 0.012 for the 1:2 complex (CuL2). Individual quantum yields of ammonia are 0.055 ± 0.007 for CuL and 0.036 ± 0.005 for CuL2. Individual quantum yields of acetaldehyde are 0.030 ± 0.007 for CuL and 0.024 ± 0.007 for CuL2. CuL always has larger quantum yields than CuL2, which can be attributed to the Cu(II) stabilizing effect of the second ligand. For both CuL and CuL2, the individual quantum yields of Cu(I), ammonia, and acetaldehyde are in the ratio of 1.8:1:0.7. A reaction mechanism for the formation of the observed photoproducts is proposed.

Enhanced Photocatalytic Activity toward Organic Pollutants Degradation and Mechanism Insight of Novel CQDs/Bi₂O₂CO₃ Composite.

PubMed

Zhang, Zisheng; Lin, Shuanglong; Li, Xingang; Li, Hong; Zhang, Tong; Cui, Wenquan

2018-05-15

Novel carbon quantum dots (CQDs) modified with Bi₂O₂CO₃ (CQDs/Bi₂O₂CO₃) were prepared using a simple dynamic-adsorption precipitation method. X-ray diffractometry (XRD), transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), and scanning electron microscopy (SEM) were used to test the material composition, structure, and band structures of the as-prepared samples. Methylene blue (MB) and colorless phenol, as target organic pollutants, were used to evaluate the photocatalytic performance of the CQDs/Bi₂O₂CO₃ hybrid materials under visible light irradiation. Experimental investigation shows that 2⁻5 nm CQDs were uniformly decorated on the surface of Bi₂O₂CO₃; CQDs/Bi₂O₂CO₃ possess an efficient photocatalytic performance, and the organic matter removal rate of methylene blue and phenol can reach up to 94.45% and 61.46% respectively, within 2 h. In addition, the degradation analysis of phenol by high performance liquid chromatography (HPLC) proved that there are no other impurities in the degradation process. Photoelectrochemical testing proved that the introduction of CQDs (electron acceptor) effectively suppresses the recombination of e - -h⁺, and promotes charge transfer. Quenching experiments and electron spin resonance (ESR) suggested that ·OH, h⁺, and ·O₂ - were involved in the photocatalytic degradation process. These results suggested that the up-conversion function of CQDs could improve the electron transfer and light absorption ability of photocatalysts and ·O₂ - formation. Furthermore, the up-conversion function of CQDs would help maintain photocatalytic stability. Finally, the photocatalytic degradation mechanism was proposed according to the above experimental result.

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

PubMed Central

2013-01-01

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

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

PubMed

Feng, Li; Wu, Yinsu

2015-05-05

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

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

PubMed

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

2014-01-24

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

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

NASA Astrophysics Data System (ADS)

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

2015-03-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

Polariton-Assisted Singlet Fission in Acene Aggregates.

PubMed

Martínez-Martínez, Luis A; Du, Matthew; F Ribeiro, Raphael; Kéna-Cohen, Stéphane; Yuen-Zhou, Joel

2018-04-19

Singlet fission is an important candidate to increase energy conversion efficiency in organic photovoltaics by providing a pathway to increase the quantum yield of excitons per photon absorbed in select materials. We investigate the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities. Starting from an open-quantum-systems approach, we build a kinetic model for time-evolution of species of interest in the presence of singlet quenchers and show that polaritons can decrease or increase exciton quantum yields compared to the cavity-free case. In particular, we find that hexacene, under the conditions of our model, can feature a higher yield than cavity-free pentacene when assisted by polaritonic effects. Similarly, we show that pentacene yield can be increased when assisted by polariton states. Finally, we address how various relaxation processes between bright and dark states in lossy microcavities affect polariton photochemistry. Our results also provide insights on how to choose microcavities to enhance similarly related chemical processes.

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

PubMed Central

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

2014-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2015-03-01

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

Light propagation and fluorescence quantum yields in liquid scintillators

NASA Astrophysics Data System (ADS)

Buck, C.; Gramlich, B.; Wagner, S.

2015-09-01

For the simulation of the scintillation and Cherenkov light propagation in large liquid scintillator detectors a detailed knowledge about the absorption and emission spectra of the scintillator molecules is mandatory. Furthermore reemission probabilities and quantum yields of the scintillator components influence the light propagation inside the liquid. Absorption and emission properties are presented for liquid scintillators using 2,5-Diphenyloxazole (PPO) and 4-bis-(2-Methylstyryl)benzene (bis-MSB) as primary and secondary wavelength shifter. New measurements of the quantum yields for various aromatic molecules are shown.

808 nm-excited upconversion nanoprobes with low heating effect for targeted magnetic resonance imaging and high-efficacy photodynamic therapy in HER2-overexpressed breast cancer.

PubMed

Zeng, Leyong; Pan, Yuanwei; Zou, Ruifen; Zhang, Jinchao; Tian, Ying; Teng, Zhaogang; Wang, Shouju; Ren, Wenzhi; Xiao, Xueshan; Zhang, Jichao; Zhang, Lili; Li, Aiguo; Lu, Guangming; Wu, Aiguo

2016-10-01

To avoid the overheating effect of excitation light and improve the efficacy of photodynamic therapy (PDT) of upconversion nanoplatform, a novel nanoprobe based on 808 nm-excited upconversion nanocomposites (T-UCNPs@Ce6@mSiO2) with low heating effect and deep penetration has been successfully constructed for targeted upconversion luminescence, magnetic resonance imaging (MRI) and high-efficacy PDT in HER2-overexpressed breast cancer. In this nanocomposite, photosensitizers (Ce6) were covalently conjugated inside of mesoporous silica to enhance the PDT efficacy by shortening the distance of fluorescence resonance energy transfer and to decrease the cytotoxicity by preventing the undesired leakage of Ce6. Compared with UCNPs@mSiO2@Ce6, UCNPs@Ce6@mSiO2 greatly promoted the singlet oxygen generation and amplified the PDT efficacy under the excitation of 808 nm laser. Importantly, the designed nanoprobe can greatly improve the uptake of HER2-positive cells and tumors by modifying the site-specific peptide, and the in vivo experiments showed excellent MRI and PDT via intravenous injection by modeling MDA-MB-435 tumor-bearing nude mice. Our strategy may provide an effective solution for overcoming the heating effect and improving the PDT efficacy of upconversion nanoprobes, and has potential application in visualized theranostics of HER2-overexpressed breast cancer. Copyright © 2016 Elsevier Ltd. All rights reserved.

One-step nucleotide-programmed growth of porous upconversion nanoparticles: application to cell labeling and drug delivery

NASA Astrophysics Data System (ADS)

Zhou, Li; Li, Zhenhua; Liu, Zhen; Yin, Meili; Ren, Jinsong; Qu, Xiaogang

2014-01-01

A simple and ``green'' strategy has been reported for the first time to fabricate upconversion nanoparticles (UCNPs) by utilizing nucleotides as bio-templates. The influence of the functionalities present on the nucleotide on the production of nanoparticles was investigated in detail. Through the effects of nucleotides, the obtained nanoparticles possessed a porous structure. The use of the as-prepared UCNPs for cell imaging, drug delivery and versatile therapy applications were demonstrated. In view of the bright up-conversion luminescence as well as the excellent biocompatibility, and the good colloidal stability of the as-prepared UCNPs, we envision that our synthesis protocol might advance both the fields of UCNPs and biomolecule-based nanotechnology for future studies.A simple and ``green'' strategy has been reported for the first time to fabricate upconversion nanoparticles (UCNPs) by utilizing nucleotides as bio-templates. The influence of the functionalities present on the nucleotide on the production of nanoparticles was investigated in detail. Through the effects of nucleotides, the obtained nanoparticles possessed a porous structure. The use of the as-prepared UCNPs for cell imaging, drug delivery and versatile therapy applications were demonstrated. In view of the bright up-conversion luminescence as well as the excellent biocompatibility, and the good colloidal stability of the as-prepared UCNPs, we envision that our synthesis protocol might advance both the fields of UCNPs and biomolecule-based nanotechnology for future studies. Electronic supplementary information (ESI) available: Supporting figures. See DOI: 10.1039/c3nr04255c

Folic acid-functionalized up-conversion nanoparticles: toxicity studies in vivo and in vitro and targeted imaging applications

NASA Astrophysics Data System (ADS)

Sun, Lining; Wei, Zuwu; Chen, Haige; Liu, Jinliang; Guo, Jianjian; Cao, Ming; Wen, Tieqiao; Shi, Liyi

2014-07-01

Folate receptors (FRs) are overexpressed on a variety of human cancer cells and tissues, including cancers of the breast, ovaries, endometrium, and brain. This over-expression of FRs can be used to target folate-linked imaging specifically to FR-expressing tumors. Fluorescence is emerging as a powerful new modality for molecular imaging in both the diagnosis and treatment of disease. Combining innovative molecular biology and chemistry, we prepared three kinds of folate-targeted up-conversion nanoparticles as imaging agents (UCNC-FA: UCNC-Er-FA, UCNC-Tm-FA, and UCNC-Er,Tm-FA). In vivo and in vitro toxicity studies showed that these nanoparticles have both good biocompatibility and low toxicity. Moreover, the up-conversion luminescence imaging indicated that they have good targeting to HeLa cells and can therefore serve as potential fluorescent contrast agents.Folate receptors (FRs) are overexpressed on a variety of human cancer cells and tissues, including cancers of the breast, ovaries, endometrium, and brain. This over-expression of FRs can be used to target folate-linked imaging specifically to FR-expressing tumors. Fluorescence is emerging as a powerful new modality for molecular imaging in both the diagnosis and treatment of disease. Combining innovative molecular biology and chemistry, we prepared three kinds of folate-targeted up-conversion nanoparticles as imaging agents (UCNC-FA: UCNC-Er-FA, UCNC-Tm-FA, and UCNC-Er,Tm-FA). In vivo and in vitro toxicity studies showed that these nanoparticles have both good biocompatibility and low toxicity. Moreover, the up-conversion luminescence imaging indicated that they have good targeting to HeLa cells and can therefore serve as potential fluorescent contrast agents. Electronic supplementary information (ESI) available: Up-conversion luminescence spectra of UCNC-Er and UCNC-Er-FA, UCNC-Tm and UCNC-Tm-FA. Confocal luminescence imaging data collected as a series along the Z optical axis. See DOI: 10.1039/c4nr02312a

Infrared spectroscopy and upconversion luminescence behaviour of erbium doped yttrium (III) oxide phosphor

NASA Astrophysics Data System (ADS)

Dubey, Vikas; Tiwari, Ratnesh; Tamrakar, Raunak Kumar; Rathore, Gajendra Singh; Sharma, Chitrakant; Tiwari, Neha

2014-11-01

The paper reports upconversion luminescence behaviour and infra-red spectroscopic pattern of erbium doped yttrium (III) oxide phosphor. Sample was synthesized by solid state reaction method with variable concentration or erbium (0.5-2.5 mol%). The conventional solid state method is suitable for large scale production and eco-friendly method. The prepared sample was characterized by X-ray diffraction (XRD) technique. From structural analysis by XRD technique shows cubic structure of prepared sample with variable concentration of erbium and no impurity phase were found when increase the concentration of Er3+. Particle size was calculated by Scherer's formula and it varies from 67 nm to 120 nm. The surface morphology of prepared phosphor was determined by field emission gun scanning electron microscopy (FEGSEM) technique. The surface morphology of the sample shows good connectivity with grains as well as some agglomerates formation occurs in sample. The functional group analysis was done by Fourier transform infra-red technique (FTIR) analysis which confirm the formation of Y2O3:Er3+ phosphor was prepared. The results indicated that the Y2O3:Er3+ phosphors might have high upconversion efficiency because of their low vibrational energy. Under 980 nm laser excitation sample shows intense green emission at 555 nm and orange emission at 590 nm wavelength. For green emission transition occurs 2H11/2 → 4I15/2, 4S3/2 → 4I15/2 for upconversion emissions. Excited state absorption and energy transfer process were discussed as possible upconversion mechanisms. The near infrared luminescence spectra was recorded. The upconversion luminescence intensity increase with increasing the concentration or erbium up to 2 mol% after that luminescence intensity decreases due to concentration quenching occurs. Spectrophotometric determinations of peaks are evaluated by Commission Internationale de I'Eclairage (CIE) technique. From CIE technique the dominant peak of from PL spectra shows intense green emission so the prepared phosphor is may be useful for green light emitting diode (GLED) application.

Quantum mechanics: The Bayesian theory generalized to the space of Hermitian matrices

NASA Astrophysics Data System (ADS)

Benavoli, Alessio; Facchini, Alessandro; Zaffalon, Marco

2016-10-01

We consider the problem of gambling on a quantum experiment and enforce rational behavior by a few rules. These rules yield, in the classical case, the Bayesian theory of probability via duality theorems. In our quantum setting, they yield the Bayesian theory generalized to the space of Hermitian matrices. This very theory is quantum mechanics: in fact, we derive all its four postulates from the generalized Bayesian theory. This implies that quantum mechanics is self-consistent. It also leads us to reinterpret the main operations in quantum mechanics as probability rules: Bayes' rule (measurement), marginalization (partial tracing), independence (tensor product). To say it with a slogan, we obtain that quantum mechanics is the Bayesian theory in the complex numbers.

Intermediate quantum maps for quantum computation

NASA Astrophysics Data System (ADS)

Giraud, O.; Georgeot, B.

2005-10-01

We study quantum maps displaying spectral statistics intermediate between Poisson and Wigner-Dyson. It is shown that they can be simulated on a quantum computer with a small number of gates, and efficiently yield information about fidelity decay or spectral statistics. We study their matrix elements and entanglement production and show that they converge with time to distributions which differ from random matrix predictions. A randomized version of these maps can be implemented even more economically and yields pseudorandom operators with original properties, enabling, for example, one to produce fractal random vectors. These algorithms are within reach of present-day quantum computers.

Quantum Yields of CAM Plants Measured by Photosynthetic O2 Exchange 1

PubMed Central

Adams, William W.; Nishida, Kojiro; Osmond, C. Barry

1986-01-01

The quantum yield of photosynthetic O2 exchange was measured in eight species of leaf succulents representative of both malic enzyme type and phosphoenolpyruvate carboxykinase type CAM plants. Measurements were made at 25°C and CO2 saturation using a leaf disc O2 electrode system, either during or after deacidification. The mean quantum yield was 0.095 ± 0.012 (sd) moles O2 per mole quanta, which compared with 0.094 ± 0.006 (sd) moles O2 per mole quanta for spinach leaf discs measured under the same conditions. There were no consistent differences in quantum yield between decarboxylation types or during different phases of CAM metabolism. On the basis of current notions of compartmentation of CAM biochemistry, our observations are interpreted to indicate that CO2 refixation is energetically independent of gluconeogenesis during deacidification. PMID:16664793

Poly(vinylpyrrolidone) supported copper nanoclusters: glutathione enhanced blue photoluminescence for application in phosphor converted light emitting devices

NASA Astrophysics Data System (ADS)

Wang, Zhenguang; Susha, Andrei S.; Chen, Bingkun; Reckmeier, Claas; Tomanec, Ondrej; Zboril, Radek; Zhong, Haizheng; Rogach, Andrey L.

2016-03-01

Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92.Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92. Electronic supplementary information (ESI) available: The optical spectra of control experiments for Cu NC synthesis, optimization of the reaction conditions, and spectra for LEDs chips and blue LEDs. See DOI: 10.1039/c6nr00806b

Single-particle tracking of quantum dot-conjugated prion proteins inside yeast cells

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

Tsuji, Toshikazu; Kawai-Noma, Shigeko; Pack, Chan-Gi

2011-02-25

Research highlights: {yields} We develop a method to track a quantum dot-conjugated protein in yeast cells. {yields} We incorporate the conjugated quantum dot proteins into yeast spheroplasts. {yields} We track the motions by conventional or 3D tracking microscopy. -- Abstract: Yeast is a model eukaryote with a variety of biological resources. Here we developed a method to track a quantum dot (QD)-conjugated protein in the budding yeast Saccharomyces cerevisiae. We chemically conjugated QDs with the yeast prion Sup35, incorporated them into yeast spheroplasts, and tracked the motions by conventional two-dimensional or three-dimensional tracking microscopy. The method paves the way towardmore » the individual tracking of proteins of interest inside living yeast cells.« less

The Sensitive Infrared Signal Detection by Sum Frequency Generation

NASA Technical Reports Server (NTRS)

Wong, Teh-Hwa; Yu, Jirong; Bai, Yingxin

2013-01-01

An up-conversion device that converts 2.05-micron light to 700 nm signal by sum frequency generation using a periodically poled lithium niobate crystal is demonstrated. The achieved 92% up-conversion efficiency paves the path to detect extremely weak 2.05-micron signal with well established silicon avalanche photodiode detector for sensitive lidar applications.

Snap-through twinkling energy generation through frequency up-conversion

NASA Astrophysics Data System (ADS)

Panigrahi, Smruti R.; Bernard, Brian P.; Feeny, Brian F.; Mann, Brian P.; Diaz, Alejandro R.

2017-07-01

A novel experimental energy harvester is investigated for its energy harvesting capability by frequency up-conversion using snap-through structures. In particular, a single-degree-of-freedom (SDOF) experimental energy harvester model is built using a snap-through nonlinear element. The snap-through dynamics is facilitated by the experimental setup of a twinkling energy generator (TEG) consisting of linear springs and attracting cylindrical bar magnets. A cylindrical coil of enamel-coated magnet wire is used as the energy generator. The governing equations are formulated mathematically and solved numerically for a direct comparison with the experimental results. The experimental TEG and the numerical simulation results show 25-fold frequency up-conversion and the power harvesting capacity of the SDOF TEG.

Zirconia nanocrystals as submicron level biological label

NASA Astrophysics Data System (ADS)

Smits, K.; Liepins, J.; Gavare, M.; Patmalnieks, A.; Gruduls, A.; Jankovica, D.

2012-08-01

Inorganic nanocrystals are of increasing interest for their usage in biology and pharmacology research. Our interest was to justify ZrO2 nanocrystal usage as submicron level biological label in baker's yeast Saccharomyces cerevisia culture. For the first time (to our knowledge) images with sub micro up-conversion luminescent particles in biologic media were made. A set of undoped as well as Er and Yb doped ZrO2 samples at different concentrations were prepared by sol-gel method. The up-conversion luminescence for free standing and for nanocrystals with baker's yeast cells was studied and the differences in up-conversion luminescence spectra were analyzed. In vivo toxic effects of ZrO2 nanocrystals were tested by co-cultivation with baker's yeast.

Bi-stable frequency up-conversion piezoelectric energy harvester driven by non-contact magnetic repulsion

NASA Astrophysics Data System (ADS)

Tang, Q. C.; Yang, Y. L.; Li, Xinxin

2011-12-01

This paper presents miniaturized energy harvesters, where the frequency up-conversion technique is used to improve the bandwidth of vibration energy harvesters. The proposed and developed miniature piezoelectric energy harvester utilizes magnetic repulsion forces to achieve non-contact frequency up-conversion, thereby avoiding mechanical collision and wear for long-term working durability. A pair of piezoelectric resonant cantilevers is micro-fabricated to generate electric power. A simplified model involving linear oscillators and magnetic interaction is deployed to demonstrate the feasibility of the device design. A bench-top harvester has been fabricated and characterized, resulting in average power generation of over 10 µW within a broad frequency range of 10-22 Hz under 1g acceleration.

Photoelectric Effect: Back to Basics.

ERIC Educational Resources Information Center

Powell, R. A.

1978-01-01

Presents a simplified theoretical analysis of the variation of quantum yield with photon energy in the photoelectric experiment. Describes a way to amplify the experiment and make it more instructive to advanced students through the measurement of quantum yield of a photo cell. (GA)

DETERMINATION OF APPARENT QUANTUM YIELD SPECTRA FOR THE FORMATION OF BIOLOGICALLY LABILE PHOTOPRODUCTS

EPA Science Inventory

Quantum yield spectra for the photochemical formation of biologically labile photoproducts from dissolved organic matter (DOM) have not been available previously, although they would greatly facilitate attempts to model photoproduct formation rates across latitudinal, seasonal, a...

Terahertz cascades from nanoparticles

NASA Astrophysics Data System (ADS)

Arnardottir, K. B.; Liew, T. C. H.

2018-05-01

In this article we propose a system capable of terahertz (THz) radiation with quantum yield above unity. The system consists of nanoparticles where the material composition varies along the radial direction of each nanoparticle in such a way that a ladder of equidistant energy levels emerges. By then exciting the highest level of this ladder we produce multiple photons of the same frequency in the THz range. We demonstrate how we can calculate a continuous material composition profile that achieves a high quantum yield and then show that a more experimentally friendly design of a multishell nanoparticle can still result in a high quantum yield.

Photo-kinetics of photoinduced transformation reaction of methylene green with titanium trichloride in different solvents

NASA Astrophysics Data System (ADS)

Nadeem, Syed Muhammad Saqib; Saeed, Rehana

2017-08-01

The photo-kinetics of photoinduced transformation reaction of methylene green and titanium trichloride was investigated in water and different aqueous-alcoholic solvents. The reaction is pseudo-first order, dependent only on the concentration of titanium trichloride at fixed concentration of methylene green. The effect of water and aqueous-alcoholic solvents was studied in the acidic range from 4 to 7. It was observed that the quantum yield (φ) of reaction increased with increase in polarity of the solvent. The quantum yield (φ) was high in acidic condition and decreased with further increase in acidity. The quantum yield (φ) increased sharply with increase in concentration of titanium trichloride while it almost remained unaffected by change in concentration of methylene green. The addition of ions increased the quantum yield (φ) of reaction. The increase in temperature decreased the rate and quantum yield (φ) of reaction. An electron transfer mechanism for the reaction has been proposed in accordance with the kinetics of reaction. The absence of any reaction intermediate was confirmed by spectroscopic investigations. Activation energy ( E a) was calculated by Arrhenius relation. Thermodynamic parameters such as activation energy ( E a), enthalpy change (Δ H), free energy change (Δ G) and entropy change (Δ S) were also evaluated.

Fluorescence quantum yield of carbon dioxide for quantitative UV laser-induced fluorescence in high-pressure flames

NASA Astrophysics Data System (ADS)

Lee, T.; Bessler, W. G.; Yoo, J.; Schulz, C.; Jeffries, J. B.; Hanson, R. K.

2008-11-01

The fluorescence quantum yield for ultraviolet laser-induced fluorescence of CO2 is determined for selected excitation wavelengths in the range 215-250 nm. Wavelength-resolved laser-induced fluorescence (LIF) spectra of CO2, NO, and O2 are measured in the burned gases of a laminar CH4/air flame ( φ=0.9 and 1.1) at 20 bar with additional NO seeded into the flow. The fluorescence spectra are fit to determine the relative contribution of the three species to infer an estimate of fluorescence quantum yield for CO2 that ranges from 2-8×10-6 depending on temperature and excitation wavelength with an estimated uncertainty of ±0.5×10-6. The CO2 fluorescence signal increases linearly with gas pressure for flames with constant CO2 mole fraction for the 10 to 60 bar range, indicating that collisional quenching is not an important contributor to the CO2 fluorescence quantum yield. Spectral simulation calculations are used to choose two wavelengths for excitation of CO2, 239.34 and 242.14 nm, which minimize interference from LIF of NO and O2. Quantitative LIF images of CO2 are demonstrated using these two excitation wavelengths and the measured fluorescence quantum yield.

Control of the external photoluminescent quantum yield of emitters coupled to nanoantenna phased arrays

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

Guo, Ke; Verschuuren, Marc A.; Lozano, Gabriel

2015-08-21

Optical losses in metals represent the largest limitation to the external quantum yield of emitters coupled to plasmonic antennas. These losses can be at the emission wavelength, but they can be more important at shorter wavelengths, i.e., at the excitation wavelength of the emitters, where the conductivity of metals is usually lower. We present accurate measurements of the absolute external photoluminescent quantum yield of a thin layer of emitting material deposited over a periodic nanoantenna phased array. Emission and absorptance measurements of the sample are performed using a custom-made setup including an integrating sphere and variable angle excitation. The measurementsmore » reveal a strong dependence of the external quantum yield on the angle at which the optical field excites the sample. Such behavior is attributed to the coupling between far-field illumination and near-field excitation mediated by the collective resonances supported by the array. Numerical simulations confirm that the inherent losses associated with the metal can be greatly reduced by selecting an optimum angle of illumination, which boosts the light conversion efficiency in the emitting layer. This combined experimental and numerical characterization of the emission from plasmonic arrays reveals the need to carefully design the illumination to achieve the maximum external quantum yield.« less

Efficient Carrier Multiplication in Colloidal Silicon Nanorods

DOE PAGES

Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan; ...

2017-08-01

In this study, auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimesmore » increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E g. Beyond a critical length, the CM quantum yield decreases. Finally, nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E g, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.« less

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

Stolle, Carl Jackson; Lu, Xiaotang; Yu, Yixuan

In this study, auger recombination lifetimes, absorption cross sections, and the quantum yields of carrier multiplication (CM), or multiexciton generation (MEG), were determined for solvent-dispersed silicon (Si) nanorods using transient absorption spectroscopy (TAS). Nanorods with an average diameter of 7.5 nm and aspect ratios of 6.1, 19.3, and 33.2 were examined. Colloidal Si nanocrystals of similar diameters were also studied for comparison. The nanocrystals and nanorods were passivated with organic ligands by hydrosilylation to prevent surface oxidation and limit the effects of surface trapping of photoexcited carriers. All samples used in the study exhibited relatively efficient photoluminescence. The Auger lifetimesmore » increased with nanorod length, and the nanorods exhibited higher CM quantum yield and efficiency than the nanocrystals with a similar band gap energy E g. Beyond a critical length, the CM quantum yield decreases. Finally, nanorods with the aspect ratio of 19.3 had the highest CM quantum yield of 1.6 ± 0.2 at 2.9E g, which corresponded to a multiexciton yield that was twice as high as observed for the spherical nanocrystals.« less

Tetherless near-infrared control of brain activity in behaving animals using fully implantable upconversion microdevices.

PubMed

Wang, Ying; Lin, Xudong; Chen, Xi; Chen, Xian; Xu, Zhen; Zhang, Wenchong; Liao, Qinghai; Duan, Xin; Wang, Xin; Liu, Ming; Wang, Feng; He, Jufang; Shi, Peng

2017-10-01

Many nanomaterials can be used as sensors or transducers in biomedical research and they form the essential components of transformative novel biotechnologies. In this study, we present an all-optical method for tetherless remote control of neural activity using fully implantable micro-devices based on upconversion technology. Upconversion nanoparticles (UCNPs) were used as transducers to convert near-infrared (NIR) energy to visible light in order to stimulate neurons expressing different opsin proteins. In our setup, UCNPs were packaged in a glass micro-optrode to form an implantable device with superb long-term biocompatibility. We showed that remotely applied NIR illumination is able to reliably trigger spiking activity in rat brains. In combination with a robotic laser projection system, the upconversion-based tetherless neural stimulation technique was implemented to modulate brain activity in various regions, including the striatum, ventral tegmental area, and visual cortex. Using this system, we were able to achieve behavioral conditioning in freely moving animals. Notably, our microscale device was at least one order of magnitude smaller in size (∼100 μm in diameter) and two orders of magnitude lighter in weight (less than 1 mg) than existing wireless optogenetic devices based on light-emitting diodes. This feature allows simultaneous implantation of multiple UCNP-optrodes to achieve modulation of brain function to control complex animal behavior. We believe that this technology not only represents a novel practical application of upconversion nanomaterials, but also opens up new possibilities for remote control of neural activity in the brains of behaving animals. Copyright © 2017 Elsevier Ltd. All rights reserved.

Light-Emitting Photon-Upconversion Nanoparticles in the Generation of Transdermal Reactive-Oxygen Species.

PubMed

Prieto, Martin; Rwei, Alina Y; Alejo, Teresa; Wei, Tuo; Lopez-Franco, Maria Teresa; Mendoza, Gracia; Sebastian, Victor; Kohane, Daniel S; Arruebo, Manuel

2017-12-06

Common photosensitizers used in photodynamic therapy do not penetrate the skin effectively. In addition, the visible blue and red lights used to excite such photosensitizers have shallow penetration depths through tissue. To overcome these limitations, we have synthesized ultraviolet- and visible-light-emitting, energy-transfer-based upconversion nanoparticles and coencapsulated them inside PLGA-PEG (methoxy poly(ethylene glycol)-b-poly(lactic-co-glycolic acid)) nanoparticles with the photosensitizer protoporphyrin IX. Nd 3+ has been introduced as a sensitizer in the upconversion nanostructure to allow its excitation at 808 nm. The subcytotoxic doses of the hybrid nanoparticles have been evaluated on different cell lines (i.e., fibroblasts, HaCaT, THP-1 monocytic cell line, U251MG (glioblastoma cell line), and mMSCs (murine mesenchymal stem cells). Upon NIR (near infrared)-light excitation, the upconversion nanoparticles emitted UV and VIS light, which consequently activated the generation of reactive-oxygen species (ROS). In addition, after irradiating at 808 nm, the resulting hybrid nanoparticles containing both upconversion nanoparticles and protoporphyrin IX generated 3.4 times more ROS than PLGA-PEG nanoparticles containing just the same dose of protoporphyrin IX. Their photodynamic effect was also assayed on different cell cultures, demonstrating their efficacy in selectively killing treated and irradiated cells. Compared to the topical application of the free photosensitizer, enhanced skin permeation and penetration were observed for the nanoparticulate formulation, using an ex vivo human-skin-permeation experiment. Whereas free protoporphyrin IX remained located at the outer layer of the skin, nanoparticle-encapsulated protoporphyrin IX was able to penetrate through the epidermal layer slightly into the dermis.

Broadband sum-frequency generation using d₃₃ in periodically poled LiNbO₃ thin film in the telecommunications band.

PubMed

Li, Guangzhen; Chen, Yuping; Jiang, Haowei; Chen, Xianfeng

2017-03-01

We demonstrate the first, to the best of our knowledge, type-0 broadband sum-frequency generation (SFG) based on single-crystal periodically poled LiNbO₃ (PPLN) thin film. The broad bandwidth property was largely tuned from mid-infrared region to the telecommunications band by engineering the thickness of PPLN from bulk crystal to nanoscale. It provides SFG a solution with both broadband and high efficiency by using the highest nonlinear coefficient d₃₃ instead of d₃₁ in type-I broadband SFG or second-harmonic generation. The measured 3 dB upconversion bandwidth is about 15.5 nm for a 4 cm long single crystal at 1530 nm wavelength. It can find applications in chip-scale spectroscopy, quantum information processing, LiNbO₃-thin-film-based microresonator and optical nonreciprocity devices, etc.

Recent advances in nanomaterial-based biosensors for antibiotics detection.

PubMed

Lan, Lingyi; Yao, Yao; Ping, Jianfeng; Ying, Yibin

2017-05-15

Antibiotics are able to be accumulated in human body by food chain and may induce severe influence to human health and safety. Hence, the development of sensitive and simple methods for rapid evaluation of antibiotic levels is highly desirable. Nanomaterials with excellent electronic, optical, mechanical, and thermal properties have been recognized as one of the most promising materials for opening new gates in the development of next-generation biosensors. This review highlights the current advances in the nanomaterial-based biosensors for antibiotics detection. Different kinds of nanomaterials including carbon nanomaterials, metal nanomaterials, magnetic nanoparticles, up-conversion nanoparticles, and quantum dots have been applied to the construction of biosensors with two main signal-transducing mechanisms, i.e. optical and electrochemical. Furthermore, the current challenges and future prospects in this field are also included to provide an overview for future research directions. Copyright © 2017 Elsevier B.V. All rights reserved.

Donor-σ-Acceptor Motifs: Thermally Activated Delayed Fluorescence Emitters with Dual Upconversion.

PubMed

Geng, Yan; D'Aleo, Anthony; Inada, Ko; Cui, Lin-Song; Kim, Jong Uk; Nakanotani, Hajime; Adachi, Chihaya

2017-12-22

A family of organic emitters with a donor-σ-acceptor (D-σ-A) motif is presented. Owing to the weakly coupled D-σ-A intramolecular charge-transfer state, a transition from the localized excited triplet state ( 3 LE) and charge-transfer triplet state ( 3 CT) to the charge-transfer singlet state ( 1 CT) occurred with a small activation energy and high photoluminescence quantum efficiency. Two thermally activated delayed fluorescence (TADF) components were identified, one of which has a very short lifetime of 200-400 ns and the other a longer TADF lifetime of the order of microseconds. In particular, the two D-σ-A materials presented strong blue emission with TADF properties in toluene. These results will shed light on the molecular design of new TADF emitters with short delayed lifetimes. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effects of Bleaching by Nitrogen Deficiency on the Quantum Yield of Photosystem II in Synechocystis sp. PCC 6803 Revealed by Chl Fluorescence Measurements.

PubMed

Ogawa, Takako; Sonoike, Kintake

2016-03-01

Estimation of photosynthesis by Chl fluorescence measurement of cyanobacteria is always problematic due to the interference from respiratory electron transfer and from phycocyanin fluorescence. The interference from respiratory electron transfer could be avoided by the use of DCMU or background illumination by blue light, which oxidizes the plastoquinone pool that tends to be reduced by respiration. On the other hand, the precise estimation of photosynthesis in cells with a different phycobilisome content by Chl fluorescence measurement is difficult. By subtracting the basal fluorescence due to the phycobilisome and PSI, it becomes possible to estimate the precise maximum quantum yield of PSII in cyanobacteria. Estimated basal fluorescence accounted for 60% of the minimum fluorescence, resulting in a large difference between the 'apparent' yield and 'true' yield under high phycocyanin conditions. The calculated value of the 'true' maximum quantum yield of PSII was around 0.8, which was similar to the value observed in land plants. The results suggest that the cause of the apparent low yield reported in cyanobacteria is mainly ascribed to the interference from phycocyanin fluorescence. We also found that the 'true' maximum quantum yield of PSII decreased under nitrogen-deficient conditions, suggesting the impairment of the PSII reaction center, while the 'apparent' maximum quantum yield showed a marginal change under the same conditions. Due to the high contribution of phycocyanin fluorescence in cyanobacteria, it is essential to eliminate the influence of the change in phycocyanin content on Chl fluorescence measurement and to evaluate the 'true' photosynthetic condition. © The Author 2016. Published by Oxford University Press on behalf of Japanese Society of Plant Physiologists. All rights reserved. For permissions, please email: journals.permissions@oup.com.

Smart pH-responsive upconversion nanoparticles for enhanced tumor cellular internalization and near-infrared light-triggered photodynamic therapy.

PubMed

Wang, Sheng; Zhang, Lei; Dong, Chunhong; Su, Lin; Wang, Hanjie; Chang, Jin

2015-01-01

A smart pH-responsive photodynamic therapy system based on upconversion nanoparticle loaded PEG coated polymeric lipid vesicles (RB-UPPLVs) was designed and prepared. These RB-UPPLVs which are promising agents for deep cancer photodynamic therapy applications can achieve enhanced tumor cellular internalization and near-infrared light-triggered photodynamic therapy.

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

PubMed Central

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

2017-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2008-08-01

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

White light upconversion emission in Yb3+/ Er3+/ Tm3+ codoped oxy-fluoride lithium tungsten tellurite glass ceramics

NASA Astrophysics Data System (ADS)

Ansari, Ghizal F.; Mahajan, S. K.

2012-02-01

The bright white upconversion emission ( tri-colour UC) is generated in Er/Tm/Yb tri -doped oxy-fluoride lithium tungsten tellurite (TWLOF)glass ceramics containing crystalline phase LiYbF4 under the excitation of 980nm laser diode. The most appropriate combination of rare-earth ions (2mol% YbF3 1mol% ErF3 and 1mol%TmF3 )of glass ceramic sample has been determined to tune the primary colour (RGB and generate white light emission. By varying the pump power, intense and weak blue (487nm, 437nm), green (525nm and 545nm) and red (662nm) emission are simultaneously observed at room temperature. The dependence of upconversion emission intensity suggest that a theephoton process is responsible for the blue emission of Tm3+ ions and red emission due to both Tm3+ and Er3+ ions , while green emission originated from two photon processes in Er3+ ions. Also tri colour upconvesion and energy transfer in this glass ceramics sample were studied under 808nm laser diode excitation. The Upconversion mechanisms and Tm3+ ions plays role of both emitter and activator (transfer energy to Er) were discussed.

Up-Conversion Y2O3:Yb(3+),Er(3+) Hollow Spherical Drug Carrier with Improved Degradability for Cancer Treatment.

PubMed

Ge, Kun; Zhang, Cuimiao; Sun, Wentong; Liu, Huifang; Jin, Yi; Li, Zhenhua; Liang, Xing-Jie; Jia, Guang; Zhang, Jinchao

2016-09-28

The rare earth hollow spheres with up-conversion luminescence properties have shown potential applications in drug delivery and bioimaging fields. However, there have been few reports for the degradation properties of rare earth oxide drug carriers. Herein, uniform and well-dispersed Y2O3:Yb(3+),Er(3+) hollow spheres (YOHSs) have been fabricated by a general Pechini sol-gel process with melamine formaldehyde colloidal spheres as template. The novel YOHSs with up-conversion luminescence has good drug loading amount and drug-release efficiency; moreover, it exhibits pH-responsive release patterns. In particular, the YOHSs sample exhibits low cytotoxicity and excellent degradable properties in acid buffer. After the sample was loaded with anticancer drug doxorubicin (DOX), the antitumor result in vitro indicates that YOHS-DOX might be effective in cancer treatment. The animal imaging test also reveals that the YOHSs drug carrier can be used as an outstanding luminescent probe for bioimaging in vivo application prospects. The results suggest that the degradable drug carrier with up-conversion luminescence may enhance the delivery efficiency of drugs and improve the cancer therapy in clinical applications.

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

PubMed

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

2014-08-14

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

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

PubMed

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

2017-09-05

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

DNA-assisted upconversion nanoplatform for imaging-guided synergistic therapy and laser-switchable drug detoxification.

PubMed

Li, Luoyuan; Hao, Panlong; Wei, Peng; Fu, Limin; Ai, Xicheng; Zhang, Jianping; Zhou, Jing

2017-08-01

The side effects of chemotherapy bring significant physical and psychological suffering to patients. To solve this urgent medical problem, Yb 3+ and Er 3+ co-doped NaLuF 4 upconversion nanoparticles (UCNPs) were constructed for upconversion luminescence (UCL)-labeled diagnosis under 980 nm laser irradiation. The UCNPs were then modified layer by layer with polypyrrole and a special programming DNA segment as photothermal conversion agents and controllable drug carriers, respectively. The nanoplatform was successfully used for imaging-guided synergistic therapy (photothermal therapy and chemotherapy) at a safe power density (300 mW cm -2 ), and DNA-assisted detoxification at lower temperature in cancer cells when the laser off. The synergistic therapy of the nanoplatform achieved a higher therapeutic index (∼85%) than chemotherapy only (∼44%) and photothermal therapy only (∼25%) in vitro. In vivo experiments also suggested that the nanoplatform had a higher therapeutic effect and lower side effects. The toxicity study was also evaluated, indicating the nanoplatform is low toxic to living system. This multifunctional upconversion nanoplatform provided an innovative method for imaging-guided photothermal-chemotherapy and laser-switchable drug detoxification. Copyright © 2017 Elsevier Ltd. All rights reserved.

Excitonic luminescence upconversion in a two-dimensional semiconductor

DOE PAGES

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

2015-12-21

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

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Luminescence in Conjugated Molecular Materials under Sub-bandgap Excitation

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

So, Franky

2014-05-08

Light emission in semiconductors occurs when they are under optical and electrical excitation with energy larger than the bandgap energy. In some low-dimensional semiconductor heterostructure systems, this thermodynamic limit can be violated due to radiative Auger recombination (AR), a process in which the sub-bandgap energy released from a recombined electron-hole pair is transferred to a third particle leading to radiative band-to-band recombination.1 Thus far, photoluminescence up-conversion phenomenon has been observed in some low dimensional semiconductor systems, and the effect is very weak and it can only be observed at low temperatures. Recently, we discovered that efficient electroluminescence in poly[2-methoxy-5-(2’-ethylhexyloxy)-1, phenylenevinylene]more » (MEH-PPV) polymer light-emitting devices (PLEDs) at drive voltages below its bandgap voltage could be observed when a ZnO nanoparticles (NPs) electron injection layer was inserted between the polymer and the aluminum electrode. Specifically, emitted photons with energy of 2.13 eV can be detected at operating voltages as low as 1.2 V at room temperature. Based on these data, we propose that the sub-bandgap turn-on in the MEH-PPV device is due to an Auger-assisted energy up-conversion process. The significance of this discovery is three-fold. First, radiative recombination occurs at operating voltages below the thermodynamic bandgap voltage. This process can significantly reduce the device operating voltage. For example, the current density of the device with the ZnO NC layer is almost two orders of magnitude higher than that of the device without the NC layer. Second, a reactive metal is no longer needed for the cathode. Third, this electroluminescence up-conversion process can be applied to inorganic semiconductors systems as well and their operation voltages of inorganic LEDs can be reduced to about half of the bandgap energy. Based on our initial data, we propose that the sub-bandgap turn-on in MEH-PPV devices is due to Auger-assisted energy up-conversion process. Specifically, we propose that the up-conversion process is due to charge accumulation at the polymer/NPs interface. This model requires that holes should be the dominant carriers in the polymer and the polymer/ZnO NCs heterojunction should be a type II alignment. In order to determine the mechanism of the up-conversion process, we will characterize devices fabricated using polymers with different carrier transporting properties to determine whether hole accumulation at the polymer/nanocrystals is required. Likewise, we will also use NPs with different electronic structures to fabricate devices to determine how electron accumulation affects the up-conversion process. Finally, we will measure quantitatively the interface charge accumulation by electroabsorption and correlate the results with the up-conversion photoluminescence efficiency measurements under an applied electric field.« less

Photoactive High Explosives: Substituents Effects on Tetrazine Photochemistry and Photophysics

DOE PAGES

McGrane, Shawn David; Bolme, Cynthia Anne; Greenfield, Margo Torello; ...

2016-01-21

High explosives that are photoactive, i.e., can be initiated with light, offer significant advantages in reduced potential for accidental electrical initiation. In this study, we examined a series of structurally related tetrazine based photoactive high explosive materials to detail their photochemical and photophysical properties. Using photobleaching infrared absorption, we determined quantum yields of photochemistry for nanosecond pulsed excitation at 355 and 532 nm. Changes in mass spectrometry during laser irradiation in vacuum measured the evolution of gaseous products. Fluorescence spectra, quantum yields, and lifetimes were measured to observe radiative channels of energy decay that compete with photochemistry. For the 6more » materials studied, quantum yields of photochemistry ranged from <10 –5 to 0.03 and quantum yield of fluorescence ranged from <10 –3 to 0.33. In all cases, the photoexcitation nonradiatively relaxed primarily to heat, appropriate for supporting photothermal initiation processes. Lastly, the photochemistry observed was dominated by ring scission of the tetrazine, but there was evidence of more extensive multistep reactions as well.« less

Optomechanical Control of Quantum Yield in Trans-Cis Ultrafast Photoisomerization of a Retinal Chromophore Model.

PubMed

Valentini, Alessio; Rivero, Daniel; Zapata, Felipe; García-Iriepa, Cristina; Marazzi, Marco; Palmeiro, Raúl; Fdez Galván, Ignacio; Sampedro, Diego; Olivucci, Massimo; Frutos, Luis Manuel

2017-03-27

The quantum yield of a photochemical reaction is one of the most fundamental quantities in photochemistry, as it measures the efficiency of the transduction of light energy into chemical energy. Nature has evolved photoreceptors in which the reactivity of a chromophore is enhanced by its molecular environment to achieve high quantum yields. The retinal chromophore sterically constrained inside rhodopsin proteins represents an outstanding example of such a control. In a more general framework, mechanical forces acting on a molecular system can strongly modify its reactivity. Herein, we show that the exertion of tensile forces on a simplified retinal chromophore model provokes a substantial and regular increase in the trans-to-cis photoisomerization quantum yield in a counterintuitive way, as these extension forces facilitate the formation of the more compressed cis photoisomer. A rationale for the mechanochemical effect on this photoisomerization mechanism is also proposed. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cationic carbon quantum dots derived from alginate for gene delivery: One-step synthesis and cellular uptake.

PubMed

Zhou, Jie; Deng, Wenwen; Wang, Yan; Cao, Xia; Chen, Jingjing; Wang, Qiang; Xu, Wenqian; Du, Pan; Yu, Qingtong; Chen, Jiaxin; Spector, Myron; Yu, Jiangnan; Xu, Ximing

2016-09-15

Carbon quantum dots (CQDs), unlike semiconductor quantum dots, possess fine biocompatibility, excellent upconversion properties, high photostability and low toxicity. Here, we report multifunctional CQDs which were developed using alginate, 3% hydrogen peroxide and double distilled water through a facile, eco-friendly and inexpensive one-step hydrothermal carbonization route. In this reaction, the alginate served as both the carbon source and the cationization agent. The resulting CQDs exhibited strong and stable fluorescence with water-dispersible and positively-charged properties which could serve as an excellent DNA condensation. As non-viral gene vector being used for the first time, the CQDs showed considerably high transfection efficiency (comparable to Lipofectamine2000 and significantly higher than PEI, p<0.05) and negligible toxicity. The photoluminescence properties of CQDs also permitted easy tracking of the cellular-uptake. The findings showed that both caveolae- and clathrin-mediated endocytosis pathways were involved in the internalization process of CQDs/pDNA complexes. Taken together, the alginate-derived photoluminescent CQDs hold great potential in biomedical applications due to their dual role as efficient non-viral gene vectors and bioimaging probes. This manuscript describes a facile and simple one-step hydrothermal carbonization route for preparing optically tunable photoluminescent carbon quantum dots (CQDs) from a novel raw material, alginate. These CQDs enjoy low cytotoxicity, positive zeta potential, excellent ability to condense macromolecular DNA, and most importantly, notably high transfection efficiency. The interesting finding is that the negatively-charged alginate can convert into positively charged CQDs without adding any cationic reagents. The significance of this study is that the cationic carbon quantum dots play dual roles as both non-viral gene vectors and bioimaging probes at the same time, which are most desirable in many fields of applications such as gene therapy, drug delivery, and bioimaging. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2015-08-01

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

Chemical sensing and imaging based on photon upconverting nano- and microcrystals: a review

NASA Astrophysics Data System (ADS)

Christ, Simon; Schäferling, Michael

2015-09-01

The demand for photostable luminescent reporters that absorb and emit light in the red to near-infrared (NIR) spectral region continues in biomedical research and bioanalysis. In recent years, classical organic fluorophores have increasingly been displaced by luminescent nanoparticles. These consist of either polymer or silica based beads that are loaded with luminescent dyes, conjugated polymers, or inorganic nanomaterials such as semiconductor nanocrystals (quantum dots), colloidal clusters of silver and gold, or carbon dots. Among the inorganic materials, photon upconversion nanocrystals exhibit a high potential for application to bioimaging or biomolecular assays. They offer an exceptionally high photostability, can be excited in the NIR, and their anti-Stokes emission enables luminescence detection free of background and perturbing scatter effects even in complex biological samples. These lanthanide doped inorganic crystals have multiple emission lines that can be tuned by the selection of the dopants. This review article is focused on the applications of functionalized photon upconversion nanoparticles (UCNPs) to chemical sensing. This is a comparatively new field of research activity and mainly directed at the sensing and imaging of ubiquitous chemical analytes in biological samples, particularly in living cells. For this purpose, the particles have to be functionalized with suitable indicator dyes or recognition elements, as they do not show an intrinsic or specific luminescence response to most of these analytes (e.g. pH, oxygen, metal ions). We describe the strategies for the design of such responsive nanocomposites utilizing either luminescence resonance energy transfer or emission-reabsorption (inner filter effect) mechanisms and also highlight examples for their use either immobilized in sensor layers or directly as nanoprobes for intracellular sensing and imaging.

Multiphoton microscopy and image guided light activated therapy using nanomaterials (Conference Presentation)

NASA Astrophysics Data System (ADS)

Prasad, Paras N.

2017-02-01

This talk will focus on design and applications of nanomaterials exhibiting strong multiphoton upconversion for multiphoton microscopy as well as for image-guided and light activated therapy .1-3 Such processes can occur by truly nonlinear optical interactions proceeding through virtual intermediate states or by stepwise coupled linear excitations through real intermediate states. Multiphoton processes in biocompatible multifunctional nanoparticles allow for 3D deep tissue imaging. In addition, they can produce in-situ photon conversion of deep tissue penetrating near IR light into a needed shorter wavelength light for photo-activated therapy at a targeted site, thus overcoming the limited penetration of UV or visible light into biological media. We are using near IR emitters such as silicon quantum dots which also exhibit strong multiphoton excitation for multiphoton microscopy. Another approach involves nonlinear nanocrystals such as ZnO which can produce four wave mixing, sum frequency generation as well as second harmonic generation to convert a deep tissue penetrating Near IR light at the targeted biological site to a desired shorter wavelength light suitable for bio imaging or activation of a therapy. We have utilized this approach to activate a photosensitizer for photodynamic therapy. Yet another type of upconversion materials is rare-earth ion doped optical nanotransformers which transform a Near IR (NIR) light from an external source by sequential single photon absorption, in situ and on demand, to a needed wavelength. Applications of these nanotransformers in multiphoton photoacoustic imaging will also be presented. An exciting direction pursued by us using these multiphoton nanoparticles, is functional imaging of brain. Simultaneously, they can effect optogenetics for regioselective stimulation of neurons for providing an effective intervention/augmentation strategy to enhance the cognitive state and lead to a foundation for futuristic vision of super human capabilities. Challenges and opportunities will be discussed.

Efficient 525 nm laser generation in single or double resonant cavity

NASA Astrophysics Data System (ADS)

Liu, Shilong; Han, Zhenhai; Liu, Shikai; Li, Yinhai; Zhou, Zhiyuan; Shi, Baosen

2018-03-01

This paper reports the results of a study into highly efficient sum frequency generation from 792 and 1556 nm wavelength light to 525 nm wavelength light using either a single or double resonant ring cavity based on a periodically poled potassium titanyl phosphate crystal (PPKTP). By optimizing the cavity's parameters, the maximum power achieved for the resultant 525 nm laser was 263 and 373 mW for the single and double resonant cavity, respectively. The corresponding quantum conversion efficiencies were 8 and 77% for converting 1556 nm photons to 525 nm photons with the single and double resonant cavity, respectively. The measured intra-cavity single pass conversion efficiency for both configurations was about 5%. The performances of the sum frequency generation in these two configurations was studied and compared in detail. This work will provide guidelines for optimizing the generation of sum frequency generated laser light for a variety of configurations. The high conversion efficiency achieved in this work will help pave the way for frequency up-conversion of non-classical quantum states, such as the squeezed vacuum and single photon states. The proposed green laser source will be used in our future experiments, which includes a plan to generate two-color entangled photon pairs and achieve the frequency down-conversion of single photons carrying orbital angular momentum.

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

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

Photosynthetic Physiological Response of Radix Isatidis (Isatis indigotica Fort.) Seedlings to Nicosulfuron

PubMed Central

Ning, Na; Wen, Yinyuan; Dong, Shuqi; Yin, Meiqiang; Guo, Meijun; Wang, Binqiang; Feng, Lei; Guo, Pingyi

2014-01-01

Radix Isatidis (Isatis indigotica Fort.) is one of the most important traditional Chinese medicine plants. However, there is no suitable herbicide used for weed control in Radix Isatidis field during postemergence stage. To explore the safety of sulfonylurea herbicide nicosulfuron on Radix Isatidis (Isatis indigotica Fort.) seedlings and the photosynthetic physiological response of the plant to the herbicide, biological mass, leaf area, photosynthetic pigment content, photosynthetic rate, chlorophyll fluorescence characteristics, and P700 parameters of Radix Isatidis seedlings were analyzed 10 d after nicosulfuron treatment at 5th leaf stage in this greenhouse research. The results showed that biological mass, total chlorophyll, chlorophyll a, and carotenoids content, photosynthetic rate, stomatal conductance, PS II maximum quantum yield, PS II effective quantum yield, PS II electron transport rate, photochemical quenching, maximal P700 change, photochemical quantum yield of PS I, and PS I electron transport rate decreased with increasing herbicide concentrations, whereas initial fluorescence, quantum yield of non-regulated energy dissipation in PS II and quantum yield of non-photochemical energy dissipation due to acceptor side limitation in PS I increased. It suggests that nicosulfuron ≥1 mg L−1 causes the damage of chloroplast, PS II and PS I structure. Electron transport limitations in PS I receptor side, and blocked dark reaction process may be the main cause of the significantly inhibited growth and decreased photosynthetic rate of Radix Isatidis seedlings. PMID:25165819

Synthesis, characterization and photophysical-theoretical analysis of compounds A-π-D. 1. Effect of alkyl-phenyl substituted amines in photophysical properties

NASA Astrophysics Data System (ADS)

Ortega, E.; Montecinos, R.; Cattin, L.; Díaz, F. R.; del Valle, M. A.; Bernède, J. C.

2017-08-01

The study of new dipolar A-π-D molecules, which have an acceptor (A) and donor (D) charge joined by a conjugate bridge, have been an attention focus in the recent years due their different properties. In the current work, a molecular system has been modified in order to compare the effect on properties, such as quantum yield. Thus, two series were generated (alkyl- and alkoxy-substituted) to determine if molecules with tertiary asymmetric amines change their optical properties and whether quantum yield is affected. The different products have been characterized by several techniques such as UV-Vis spectrophotometry, elemental analysis, NMR, FT-IR, mass spectroscopy and fluorescence spectroscopy. Furthermore, their behavior in eight organic solvents, dichloromethane, tetrahydrofuran, ethyl acetate, 1,4-dioxane, acetone, acetonitrile, dimethylformamide and dimethylsulfoxide were experimentally and theoretically studied. The quantum yields were higher for the alkyl-substituted series. Theoretically, the dihedral angles formed between the tertiary amine and carbonyl group moieties have a correlation with quantum yield values, helping to explain why they are higher in non-polar solvents. Consequently, the maximum quantum yield was obtained with (E)-2-cyano-3-(5-((E)-2-(9,9-diethyl-7-(methyl(phenyl)amino)-9H-fluoren-2-yl) vinyl)thiophen-2-yl)acrylic acid (M8-1) in 1,4-dioxane, reaching 98.8%.

Silicon Nanoparticles with Surface Nitrogen: 90% Quantum Yield with Narrow Luminescence Bandwidth and the Ligand Structure Based Energy Law.

PubMed

Li, Qi; Luo, Tian-Yi; Zhou, Meng; Abroshan, Hadi; Huang, Jingchun; Kim, Hyung J; Rosi, Nathaniel L; Shao, Zhengzhong; Jin, Rongchao

2016-09-27

Silicon nanoparticles (NPs) have been widely accepted as an alternative material for typical quantum dots and commercial organic dyes in light-emitting and bioimaging applications owing to silicon's intrinsic merits of least toxicity, low cost, and high abundance. However, to date, how to improve Si nanoparticle photoluminescence (PL) performance (such as ultrahigh quantum yield, sharp emission peak, high stability) is still a major issue. Herein, we report surface nitrogen-capped Si NPs with PL quantum yield up to 90% and narrow PL bandwidth (full width at half-maximum (fwhm) ≈ 40 nm), which can compete with commercial dyes and typical quantum dots. Comprehensive studies have been conducted to unveil the influence of particle size, structure, and amount of surface ligand on the PL of Si NPs. Especially, a general ligand-structure-based PL energy law for surface nitrogen-capped Si NPs is identified in both experimental and theoretical analyses, and the underlying PL mechanisms are further discussed.

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

PubMed

Tiwari, Neha; Dubey, Vikas

2016-05-01

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

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

Do the cations in clay and the polymer matrix affect quantum dot fluorescent properties?

PubMed

Wei, Wenjun; Liu, Cui; Liu, Jiyan; Liu, Xueqing; Zou, Linling; Cai, Shaojun; Shi, Hong; Cao, Yuan-Cheng

2016-06-01

This paper studied the effects of cations and polymer matrix on the fluorescent properties of quantum dots (QDs). The results indicated that temperature has a greater impact on fluorescence intensity than clay cations (mainly K(+) and Na(+) ). Combined fluorescence lifetime and steady-state spectrometer tests showed that QD lifetimes all decreased when the cation concentration was increased, but the quantum yields were steady at various cation concentrations of 0, 0.05, 0.5 and 1 M. Poly(ethylene oxide) (PEO), poly(vinyl alcohol) (PVA) and diepoxy resin were used to study the effects of polymers on QD lifetime and quantum yield. The results showed that the lifetime for QDs 550 nm in PEO and PVA was 17.33 and 17.12 ns, respectively; for the epoxy resin, the lifetime was 0.74 ns, a sharp decrease from 24.47 ns. The quantum yield for QDs 550 nm changed from 34.22% to 7.45% and 7.81% in PEO and PVA, respectively; for the epoxy resin the quantum yield was 2.25%. QDs 580 nm and 620 nm showed the same results as QDs 550 nm. This study provides useful information on the design, synthesis and application of QDs-polymer luminescent materials. Copyright © 2015 John Wiley & Sons, Ltd. Copyright © 2015 John Wiley & Sons, Ltd.

Action spectra of photosystems II and I and quantum yield of photosynthesis in leaves in State 1.

PubMed

Laisk, Agu; Oja, Vello; Eichelmann, Hillar; Dall'Osto, Luca

2014-02-01

The spectral global quantum yield (YII, electrons/photons absorbed) of photosystem II (PSII) was measured in sunflower leaves in State 1 using monochromatic light. The global quantum yield of PSI (YI) was measured using low-intensity monochromatic light flashes and the associated transmittance change at 810nm. The 810-nm signal change was calibrated based on the number of electrons generated by PSII during the flash (4·O2 evolution) which arrived at the PSI donor side after a delay of 2ms. The intrinsic quantum yield of PSI (yI, electrons per photon absorbed by PSI) was measured at 712nm, where photon absorption by PSII was small. The results were used to resolve the individual spectra of the excitation partitioning coefficients between PSI (aI) and PSII (aII) in leaves. For comparison, pigment-protein complexes for PSII and PSI were isolated, separated by sucrose density ultracentrifugation, and their optical density was measured. A good correlation was obtained for the spectral excitation partitioning coefficients measured by these different methods. The intrinsic yield of PSI was high (yI=0.88), but it absorbed only about 1/3 of quanta; consequently, about 2/3 of quanta were absorbed by PSII, but processed with the low intrinsic yield yII=0.63. In PSII, the quantum yield of charge separation was 0.89 as detected by variable fluorescence Fv/Fm, but 29% of separated charges recombined (Laisk A, Eichelmann H and Oja V, Photosynth. Res. 113, 145-155). At wavelengths less than 580nm about 30% of excitation is absorbed by pigments poorly connected to either photosystem, most likely carotenoids bound in pigment-protein complexes. Copyright © 2013 Elsevier B.V. All rights reserved.

ABSORBANCE, ABSORPTION COEFFICIENT, AND APPARENT QUANTUM YIELD: A COMMENT ON AMBIGUITY IN THE USE OF THESE OPTICAL CONCEPTS

EPA Science Inventory

Several important optical terms such as "absorbance" and "absorption coefficient" are frequently used ambiguously in the current peer-reviewed literature. Since they are important terms that are required to derive other quantities such as the "apparent quantum yield" of photoprod...

A novel contrast agent with rare earth-doped up-conversion luminescence and Gd-DTPA magnetic resonance properties

NASA Astrophysics Data System (ADS)

Lu, Qing; Wei, Daixu; Cheng, Jiejun; Xu, Jianrong; Zhu, Jun

2012-08-01

The magnetic-luminescent multifunctional nanoparticles based on Gd-DTPA and NaYF4:Yb, Er were successfully synthesized by the conjugation of activated DTPA and silica-coated/surface-aminolated NaYF4:Yb, Er nanoparticles through EDC/NHS coupling chemistry. The as-prepared products were characterized by powder X-ray diffraction, transmission electron microscopy, dynamic light scattering, energy dispersive X-ray analysis, and fourier transform infrared spectrometry. The room-temperature upconversion luminescent spectra and T1-weighted maps of the obtained nanoparticles were carried out by 980 nm NIR light excitation and a 3T MR imaging scanner, respectively. The results indicated that the as-synthesized multifunctional nanoparticles with small size, highly solubility in water, and both high MR relaxivities and upconversion luminescence may have potential usage for MR imaging in future.

Ultrafast mid-infrared spectroscopy by chirped pulse upconversion in 1800-1000cm(-1) region.

PubMed

Zhu, Jingyi; Mathes, Tilo; Stahl, Andreas D; Kennis, John T M; Groot, Marie Louise

2012-05-07

Broadband femtosecond mid-infrared pulses can be converted into the visible spectral region by chirped pulse upconversion. We report here the upconversion of pump probe transient signals in the frequency region below 1800cm(-1), using the nonlinear optical crystal AgGaGeS4, realizing an important expansion of the application range of this method. Experiments were demonstrated with a slab of GaAs, in which the upconverted signals cover a window of 120cm(-1), with 1.5cm(-1) resolution. In experiments on the BLUF photoreceptor Slr1694, signals below 1 milliOD were well resolved after baseline correction. Possibilities for further optimization of the method are discussed. We conclude that this method is an attractive alternative for the traditional MCT arrays used in most mid-infrared pump probe experiments.

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

NASA Astrophysics Data System (ADS)

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

2011-02-01

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

Near infrared harvesting dye-sensitized solar cells enabled by rare-earth upconversion materials.

PubMed

Li, Deyang; Ågren, Hans; Chen, Guanying

2018-02-01

Dye-sensitized solar cells (DSSCs) have been deemed as promising alternatives to silicon solar cells for the conversion of clean sunlight energy into electricity. A major limitation to their conversion efficiency is their inability to utilize light in the infrared (IR) spectral range, which constitutes almost half the energy of the sun's radiation. This fact has elicited motivations and endeavors to extend the response wavelength of DSSCs to the IR range. Photon upconversion through rare-earth ions constitutes one of the most promising approaches toward the goal of converting near-IR (NIR) or IR light into visible or ultraviolet light, where DSSCs typically have high sensitivity. In the present review, we summarize recent progress based on the utilization of various upconversion materials and device structures to improve the performance of dye-sensitized solar cells.

[A study on the concentration quenching of Tm3+ upconversion luminescence].

PubMed

Chen, B; Wang, H; Huang, S

2001-06-01

In this work, we have a designation and preparation of MFT glasses for upconversion, the glasses consisted of TeO2 and fluoride: PbF2, AlF3, BaF2, NaF and the impurity Tm2O3. In this glass system the oxide improve forming ability, the fluorides improve the microscopic environment around RE ions in glasses. In this glass host the content of Tm2O3 achieves to 4% mol and crystallization no occurred. A detail study on the concentration quenching of upconversion luminescence for 1G4-->3H6 and 1D2-->3H4 transitions was completed. The experimental results directed that the quenching concentration was 0.6 mol.% and higher 3 times than in other glasses materials. The cross relaxation and mechanism of concentration quenching were discussed.

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

NASA Astrophysics Data System (ADS)

Tkachuk, Alexandra M.

1996-01-01

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

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

NASA Astrophysics Data System (ADS)

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

2012-09-01

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

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

PubMed

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

2016-08-01

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

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

PubMed

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

2018-08-24

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

Pyropheophorbide A and c(RGDyK) comodified chitosan-wrapped upconversion nanoparticle for targeted near-infrared photodynamic therapy.

PubMed

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

2012-06-04

Near-infrared (NIR)-to-visible upconversion nanoparticle (UCNP) has shown promising prospects in photodynamic therapy (PDT) as a drug carrier or energy donor. In this work, a photosensitizer pyropheophorbide a (Ppa) and RGD peptide c(RGDyK) comodified chitosan-wrapped NaYF(4):Yb/Er upconversion nanoparticle UCNP-Ppa-RGD was developed for targeted near-infrared photodynamic therapy. The properties of UCNP-Ppa-RGD, such as morphology, stability, optical spectroscopy and singlet oxygen generation efficiency, were investigated. The results show that covalently linked pyropheophorbide a molecule not only is stable but also retains its spectroscopic and functional properties. In vitro studies confirm a stronger targeting specificity of UCNP-Ppa-RGD to integrin α(v)β(3)-positive U87-MG cells compared with that in the corresponding negative group. The photosensitizer-attached nanostructure exhibited low dark toxicity and high phototoxicity against cancer cells upon 980 nm laser irradiation at an appropriate dosage. These results represent the first demonstration of a highly stable and efficient photosensitizer modified upconversion nanostructure for targeted near-infrared photodynamic therapy of cancer cells. The novel UCNP-Ppa-RGD nanoparticle may provide a powerful alternative for near-infrared photodynamic therapy with an improved tumor targeting specificity.

Improvement Photocatalytic Activity of P25 by Modification with a Rare Earth-Free Upconversion Nanocrystal.

PubMed

Yin, Dongguang; Liu, Yumin; Zhao, Feifei; Zhang, Xinyu; Zhang, Tingting; Wu, Chenglong; Chang, Na; Chen, Zhiwen

2018-05-01

It has been reported that coupling TiO2 with rare earth upconversion nanocrystals (UCNCs) is an efficient strategy to significantly improve photocatalytic activity of TiO2. However, the rare earth materials are scarcity and cost, and the synthesis process of UCNCs using the rare earth materials is complicated. In the present study, we have designed a new approach using a rare earth-free upconversion nanocrystal (REF-UCNCs) as upconversion luminescent material to replace the rare earth UCNCs. A novel nanocomposite photocatalyst of REF-UCNCs@P25: Mo/GN was developed for the first time. Based on the designed structure, the REF-UCNCs, Mo-doping, and GN (graphene) have a synergistic effect that can improve catalytic activity of P25 significantly. The results of photocatalytic experiments using RhB as a model pollutant under simulated solar light irradiation show that the photocatalytic efficiency of the as-prepared catalyst is 3-folds higher than that of benchmark substance P25. This work provides a new strategy for efficiently improving catalytic activity of semiconductor photocatalysts by coupling with REF-UCNCs. This approach is facile and low-cost which can be widely applied for modification of semiconductor photocatalysts and facilitates their applications in environmental protection issues using solar light.

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.

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

PubMed

Li, Xiyu; Chen, Haifeng

2016-10-07

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

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

PubMed

Le, Khai Q; John, Sajeev

2014-01-13

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

Quantum Criticality and Black Holes

ScienceCinema

Sachdev, Subir [Harvard University, Cambridge, Massachusetts, United States

2017-12-09

I will describe the behavior of a variety of condensed matter systems in the vicinity of zero temperature quantum phase transitions. There is a remarkable analogy between the hydrodynamics of such systems and the quantum theory of black holes. I will show how insights from this analogy have shed light on recent experiments on the cuprate high temperature superconductors. Studies of new materials and trapped ultracold atoms are yielding new quantum phases, with novel forms of quantum entanglement. Some materials are of technological importance: e.g. high temperature superconductors. Exact solutions via black hole mapping have yielded first exact results for transport coefficients in interacting many-body systems, and were valuable in determining general structure of hydrodynamics. Theory of VBS order and Nernst effect in cuprates. Tabletop 'laboratories for the entire universe': quantum mechanics of black holes, quark-gluon plasma, neutrons stars, and big-bang physics.

Brightly Luminescent and Color-Tunable Colloidal CH3NH3PbX3 (X = Br, I, Cl) Quantum Dots: Potential Alternatives for Display Technology.

PubMed

Zhang, Feng; Zhong, Haizheng; Chen, Cheng; Wu, Xian-gang; Hu, Xiangmin; Huang, Hailong; Han, Junbo; Zou, Bingsuo; Dong, Yuping

2015-04-28

Organometal halide perovskites are inexpensive materials with desirable characteristics of color-tunable and narrow-band emissions for lighting and display technology, but they suffer from low photoluminescence quantum yields at low excitation fluencies. Here we developed a ligand-assisted reprecipitation strategy to fabricate brightly luminescent and color-tunable colloidal CH3NH3PbX3 (X = Br, I, Cl) quantum dots with absolute quantum yield up to 70% at room temperature and low excitation fluencies. To illustrate the photoluminescence enhancements in these quantum dots, we conducted comprehensive composition and surface characterizations and determined the time- and temperature-dependent photoluminescence spectra. Comparisons between small-sized CH3NH3PbBr3 quantum dots (average diameter 3.3 nm) and corresponding micrometer-sized bulk particles (2-8 μm) suggest that the intense increased photoluminescence quantum yield originates from the increase of exciton binding energy due to size reduction as well as proper chemical passivations of the Br-rich surface. We further demonstrated wide-color gamut white-light-emitting diodes using green emissive CH3NH3PbBr3 quantum dots and red emissive K2SiF6:Mn(4+) as color converters, providing enhanced color quality for display technology. Moreover, colloidal CH3NH3PbX3 quantum dots are expected to exhibit interesting nanoscale excitonic properties and also have other potential applications in lasers, electroluminescence devices, and optical sensors.

Structural Basis for Near Unity Quantum Yield Core/Shell Nanostructures

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

McBride, James; Treadway, Joe; Pennycook, Stephen J

2006-01-01

Aberration-corrected Z-contrast scanning transmission electron microscopy of core/shell nanocrystals shows clear correlations between structure and quantum efficiency. Uniform shell coverage is obtained only for a graded CdS/ZnS shell material and is found to be critical to achieving near 100% quantum yield. The sublattice sensitivity of the images confirms that preferential growth takes place on the anion-terminated surfaces. This explains the three-dimensional "nanobullet" shape observed in the case of core/shell nanorods.

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

Chen Lin; Chen Yixin

We show that no universal quantum cloning machine exists that can broadcast an arbitrary mixed qubit with a constant fidelity. Based on this result, we investigate the dependent quantum cloner in the sense that some parameter of the input qubit {rho}{sub s}({theta},{omega},{lambda}) is regarded as constant in the fidelity. For the case of constant {omega}, we establish the 1{yields}2 optimal symmetric dependent cloner with a fidelity 1/2. It is also shown that the 1{yields}M optimal quantum cloning machine for pure qubits is also optimal for mixed qubits, when {lambda} is the unique parameter in the fidelity. For general N{yields}M broadcastingmore » of mixed qubits, the situation is very different.« less

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

Bisio, Alessandro; D'Ariano, Giacomo Mauro; Perinotti, Paolo

We analyze quantum algorithms for cloning of a quantum measurement. Our aim is to mimic two uses of a device performing an unknown von Neumann measurement with a single use of the device. When the unknown device has to be used before the bipartite state to be measured is available we talk about 1{yields}2 learning of the measurement, otherwise the task is called 1{yields}2 cloning of a measurement. We perform the optimization for both learning and cloning for arbitrary dimension d of the Hilbert space. For 1{yields}2 cloning we also propose a simple quantum network that achieves the optimal fidelity.more » The optimal fidelity for 1{yields}2 learning just slightly outperforms the estimate and prepare strategy in which one first estimates the unknown measurement and depending on the result suitably prepares the duplicate.« less

Influence of quantum dot's quantum yield to chemiluminescent resonance energy transfer.

PubMed

Wang, Hai-Qiao; Li, Yong-Qiang; Wang, Jian-Hao; Xu, Qiao; Li, Xiu-Qing; Zhao, Yuan-Di

2008-03-03

The resonance energy transfer between chemiluminescence donor (luminol-H2O2 system) and quantum dots (QDs, emission at 593 nm) acceptors (CRET) was investigated. The resonance energy transfer efficiencies were compared while the oil soluble QDs, water soluble QDs (modified with thioglycolate) and QD-HRP conjugates were used as acceptor. The fluorescence of QD can be observed in the three cases, indicating that the CRET occurs while QD acceptor in different status was used. The highest CRET efficiency (10.7%) was obtained in the case of oil soluble QDs, and the lowest CRET efficiency (2.7%) was observed in the QD-HRP conjugates case. This result is coincident with the quantum yields of the acceptors (18.3% and 0.4%). The same result was observed in another similar set of experiment, in which the amphiphilic polymer modified QDs (emission at 675 nm) were used. It suggests that the quantum yield of the QD in different status is the crucial factor to the CRET efficiency. Furthermore, the multiplexed CRET between luminol donor and three different sizes QD acceptors was observed simultaneously. This work will offer useful support for improving the CRET studies based on quantum dots.

Triazatruxene: A Rigid Central Donor Unit for a D-A3 Thermally Activated Delayed Fluorescence Material Exhibiting Sub-Microsecond Reverse Intersystem Crossing and Unity Quantum Yield via Multiple Singlet-Triplet State Pairs.

PubMed

Dos Santos, Paloma L; Ward, Jonathan S; Congrave, Daniel G; Batsanov, Andrei S; Eng, Julien; Stacey, Jessica E; Penfold, Thomas J; Monkman, Andrew P; Bryce, Martin R

2018-06-01

By inverting the common structural motif of thermally activated delayed fluorescence materials to a rigid donor core and multiple peripheral acceptors, reverse intersystem crossing (rISC) rates are demonstrated in an organic material that enables utilization of triplet excited states at faster rates than Ir-based phosphorescent materials. A combination of the inverted structure and multiple donor-acceptor interactions yields up to 30 vibronically coupled singlet and triplet states within 0.2 eV that are involved in rISC. This gives a significant enhancement to the rISC rate, leading to delayed fluorescence decay times as low as 103.9 ns. This new material also has an emission quantum yield ≈1 and a very small singlet-triplet gap. This work shows that it is possible to achieve both high photoluminescence quantum yield and fast rISC in the same molecule. Green organic light-emitting diode devices with external quantum efficiency >30% are demonstrated at 76 cd m -2 .

The Effect of Correlated Energetic Disorder on Charge Transport in Organic Semiconductors

NASA Astrophysics Data System (ADS)

Allen, Jonathan; Röding, Sebastian; Cherqui, Charles; Dunlap, David

2012-10-01

In their 1995 paper describing a Monte Carlo simulation for dissociation of an electron-hole pair in the presence of Gaussian energetic disorder, Albrect and Bäassler reported a surprising result. They found that increasing the width σ of the energetic disorder increases the quantum yield φ. They attributed this behavior to the tendency for energy fluctuations to compete against the Coulombic pair attraction, driving the electron-hole pair apart at short distances where, without disorder, recombination would be almost certain. We have expanded upon this notion, and introduced spatial correlation into the energetic disorder. By correlating the energetic disorder, we have demonstrated even larger quantum yields in simulation, attributable to the tendency of correlation to drive the charges further apart spatially than merely random disorder. Our results generally support the findings of Greenham et al. in that a larger correlation radius gives a larger quantum yield. In addition to larger quantum yield, we believe that correlated disorder could be used to create pathways for charge transport within a material, allowing the charge carrier behavior to be tuned.

Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission.

PubMed

Quan, Li Na; Zhao, Yongbiao; García de Arquer, F Pelayo; Sabatini, Randy; Walters, Grant; Voznyy, Oleksandr; Comin, Riccardo; Li, Yiying; Fan, James Z; Tan, Hairen; Pan, Jun; Yuan, Mingjian; Bakr, Osman M; Lu, Zhenghong; Kim, Dong Ha; Sargent, Edward H

2017-06-14

Organo-metal halide perovskites are a promising platform for optoelectronic applications in view of their excellent charge-transport and bandgap tunability. However, their low photoluminescence quantum efficiencies, especially in low-excitation regimes, limit their efficiency for light emission. Consequently, perovskite light-emitting devices are operated under high injection, a regime under which the materials have so far been unstable. Here we show that, by concentrating photoexcited states into a small subpopulation of radiative domains, one can achieve a high quantum yield, even at low excitation intensities. We tailor the composition of quasi-2D perovskites to direct the energy transfer into the lowest-bandgap minority phase and to do so faster than it is lost to nonradiative centers. The new material exhibits 60% photoluminescence quantum yield at excitation intensities as low as 1.8 mW/cm 2 , yielding a ratio of quantum yield to excitation intensity of 0.3 cm 2 /mW; this represents a decrease of 2 orders of magnitude in the excitation power required to reach high efficiency compared with the best prior reports. Using this strategy, we report light-emitting diodes with external quantum efficiencies of 7.4% and a high luminescence of 8400 cd/m 2 .

Synchronous and noncollinear infrared upconversion in AgGaS/sub 2/. [JERRY 0999; JERRY 0998; JERRY 1111

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

Bhar, G.C.; Das, S.; Chatterjee, U.

1989-04-17

Synchronous noncollinear upconversion detection is reported for the first time with a Nd:YAG laser in AgGaS/sub 2/. Q-switched pump laser pulses with a repetition rate up to 50 Hz were synchronized with intracavity chopped continuous wave CO/sub 2/ laser pulses. Results were obtained both by tuning the CO/sub 2/ laser and by varying the angle between the laser beams.

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.

Application of upconversion luminescent-magnetic microbeads with weak background noise and facile separation in ochratoxin A detection

NASA Astrophysics Data System (ADS)

Liao, Zhenyu; Zhang, Ying; Su, Lin; Chang, Jin; Wang, Hanjie

2017-02-01

Ochratoxin A (OTA), the most harmful and abundant ochratoxin, is chemically stable and commonly existed in foodstuffs. In this work, upconversion luminescent-magnetic microbeads (UCLMMs) -based cytometric bead array for OTA detection with a less reagent consumption and high sensitivity has been established and optimized. In UCLMMs, upconversion nanocrystals (UCNs) for optical code present a weak background noise and no spectral cross talk between the encoding signals and target labels under two excitation conditions to improve detection sensitivity. While the superparamagnetic Fe3O4 nanoparticles (Fe3O4 NPs) aim for rapid analysis. The results show that the developed method has a sensitivity of 9.553 ppt below HPLC with a 50-μL sample and can be completed in <2 h with good accuracy and high reproducibility. Therefore, different colors of UCLMMs will become a promising assay platform for multiple mycotoxins after further improvement.

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

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

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

NASA Astrophysics Data System (ADS)

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

2006-10-01

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

Molecular approaches to third generation photovoltaics: photochemical up-conversion

NASA Astrophysics Data System (ADS)

Cheng, Yuen Yap; Fückel, Burkhard; Roberts, Derrick A.; Khoury, Tony; Clady, Rapha"l. G. C. R.; Tayebjee, Murad J. Y.; Piper, Roland; Ekins-Daukes, N. J.; Crossley, Maxwell J.; Schmidt, Timothy W.

2010-08-01

We have investigated a photochemical up-conversion system comprising a molecular mixture of a palladium porphyrin to harvest light, and a polycyclic aromatic hydrocarbon to emit light. The energy of harvested photons is stored as molecular triplet states which then annihilate to bring about up-converted fluorescence. The limiting efficiency of such triplet-triplet annihilation up-conversion has been believed to be 11% for some time. However, by rigorously investigating the kinetics of delayed fluorescence following pulsed excitation, we demonstrate instantaneous annihilation efficiencies exceeding 40%, and limiting efficiencies for the current system of ~60%. We attribute the high efficiencies obtained to the electronic structure of the emitting molecule, which exhibits an exceptionally high T2 molecular state. We utilize the kinetic data obtained to model an up-converting layer irradiated with broadband sunlight, finding that ~3% efficiencies can be obtained with the current system, with this improving dramatically upon optimization of various parameters.

Rich stochastic dynamics of co-doped Er:Yb fluorescence upconversion nanoparticles in the presence of thermal, non-conservative, harmonic and optical forces

NASA Astrophysics Data System (ADS)

Nome, Rene A.; Sorbello, Cecilia; Jobbágy, Matías; Barja, Beatriz C.; Sanches, Vitor; Cruz, Joyce S.; Aguiar, Vinicius F.

2017-03-01

The stochastic dynamics of individual co-doped Er:Yb upconversion nanoparticles (UCNP) were investigated from experiments and simulations. The UCNP were characterized by high-resolution scanning electron microscopy, dynamic light scattering, and zeta potential measurements. Single UCNP measurements were performed by fluorescence upconversion micro-spectroscopy and optical trapping. The mean-square displacement (MSD) from single UCNP exhibited a time-dependent diffusion coefficient which was compared with Brownian dynamics simulations of a viscoelastic model of harmonically bound spheres. Experimental time-dependent two-dimensional trajectories of individual UCNP revealed correlated two-dimensional nanoparticle motion. The measurements were compared with stochastic trajectories calculated in the presence of a non-conservative rotational force field. Overall, the complex interplay of UCNP adhesion, thermal fluctuations and optical forces led to a rich stochastic behavior of these nanoparticles.

Solar-Pumping Upconversion of Interfacial Coordination Nanoparticles.

PubMed

Ishii, Ayumi; Hasegawa, Miki

2017-01-30

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

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

PubMed

Du, Peng; Yu, Jae Su

2018-03-23

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

Simultaneous quasi-one-dimensional propagation and tuning of upconversion luminescence through waveguide effect

PubMed Central

Gao, Dangli; Tian, Dongping; Zhang, Xiangyu; Gao, Wei

2016-01-01

Luminescence-based waveguide is widely investigated as a promising alternative to conquer the difficulties of efficiently coupling light into a waveguide. But applications have been still limited due to employing blue or ultraviolet light as excitation source with the lower penetration depth leading to a weak guided light. Here, we show a quasi-one-dimensional propagation of luminescence and then resulting in a strong luminescence output from the top end of a single NaYF4:Yb3+/Er3+ microtube under near infrared light excitation. The mechanism of upconversion propagation, based on the optical waveguide effect accompanied with energy migration, is proposed. The efficiency of luminescence output is highly dependent on the concentration of dopant ions, excitation power, morphology, and crystallinity of tube as an indirect evidence of the existence of the optical actived waveguide effect. These findings provide the possibility for the construction of upconversion fiber laser. PMID:26926491

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

PubMed

Mohanty, Deepak Kumar; Rai, Vineet Kumar

2014-01-01

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

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

NASA Astrophysics Data System (ADS)

Osiac, E.; Sokólska, I.; Kück, S.

2002-06-01

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

Simultaneous multiple wavelength upconversion in a core-shell nanoparticle for enhanced near infrared light harvesting in a dye-sensitized solar cell.

PubMed

Yuan, Chunze; Chen, Guanying; Li, Lin; Damasco, Jossana A; Ning, Zhijun; Xing, Hui; Zhang, Tianmu; Sun, Licheng; Zeng, Hao; Cartwright, Alexander N; Prasad, Paras N; Ågren, Hans

2014-10-22

The efficiency of most photovoltaic devices is severely limited by near-infrared (NIR) transmission losses. To alleviate this limitation, a new type of colloidal upconversion nanoparticles (UCNPs), hexagonal core-shell-structured β-NaYbF4:Er(3+)(2%)/NaYF4:Nd(3+)(30%), is developed and explored in this work as an NIR energy relay material for dye-sensitized solar cells (DSSCs). These UCNPs are able to harvest light energy in multiple NIR regions, and subsequently convert the absorbed energy into visible light where the DSSCs strongly absorb. The NIR-insensitive DSSCs show compelling photocurrent increases through binary upconversion under NIR light illumination either at 785 or 980 nm, substantiating efficient energy relay by these UCNPs. The overall conversion efficiency of the DSSCs was improved with the introduction of UCNPs under simulated AM 1.5 solar irradiation.

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

NASA Astrophysics Data System (ADS)

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

2011-02-01

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

Measurement of fluorophore concentrations and fluorescence quantum yield in tissue-simulating phantoms using three diffusion models of steady-state spatially resolved fluorescence.

PubMed

Diamond, Kevin R; Farrell, Thomas J; Patterson, Michael S

2003-12-21

Steady-state diffusion theory models of fluorescence in tissue have been investigated for recovering fluorophore concentrations and fluorescence quantum yield. Spatially resolved fluorescence, excitation and emission reflectance Carlo simulations, and measured using a multi-fibre probe on tissue-simulating phantoms containing either aluminium phthalocyanine tetrasulfonate (AlPcS4), Photofrin meso-tetra-(4-sulfonatophenyl)-porphine dihydrochloride The accuracy of the fluorophore concentration and fluorescence quantum yield recovered by three different models of spatially resolved fluorescence were compared. The models were based on: (a) weighted difference of the excitation and emission reflectance, (b) fluorescence due to a point excitation source or (c) fluorescence due to a pencil beam excitation source. When literature values for the fluorescence quantum yield were used for each of the fluorophores, the fluorophore absorption coefficient (and hence concentration) at the excitation wavelength (mu(a,x,f)) was recovered with a root-mean-square accuracy of 11.4% using the point source model of fluorescence and 8.0% using the more complicated pencil beam excitation model. The accuracy was calculated over a broad range of optical properties and fluorophore concentrations. The weighted difference of reflectance model performed poorly, with a root-mean-square error in concentration of about 50%. Monte Carlo simulations suggest that there are some situations where the weighted difference of reflectance is as accurate as the other two models, although this was not confirmed experimentally. Estimates of the fluorescence quantum yield in multiple scattering media were also made by determining mu(a,x,f) independently from the fitted absorption spectrum and applying the various diffusion theory models. The fluorescence quantum yields for AlPcS4 and TPPS4 were calculated to be 0.59 +/- 0.03 and 0.121 +/- 0.001 respectively using the point source model, and 0.63 +/- 0.03 and 0.129 +/- 0.002 using the pencil beam excitation model. These results are consistent with published values.

Cryogenic on-chip multiplexer for the study of quantum transport in 256 split-gate devices

NASA Astrophysics Data System (ADS)

Al-Taie, H.; Smith, L. W.; Xu, B.; See, P.; Griffiths, J. P.; Beere, H. E.; Jones, G. A. C.; Ritchie, D. A.; Kelly, M. J.; Smith, C. G.

2013-06-01

We present a multiplexing scheme for the measurement of large numbers of mesoscopic devices in cryogenic systems. The multiplexer is used to contact an array of 256 split gates on a GaAs/AlGaAs heterostructure, in which each split gate can be measured individually. The low-temperature conductance of split-gate devices is governed by quantum mechanics, leading to the appearance of conductance plateaux at intervals of 2e2/h. A fabrication-limited yield of 94% is achieved for the array, and a "quantum yield" is also defined, to account for disorder affecting the quantum behaviour of the devices. The quantum yield rose from 55% to 86% after illuminating the sample, explained by the corresponding increase in carrier density and mobility of the two-dimensional electron gas. The multiplexer is a scalable architecture, and can be extended to other forms of mesoscopic devices. It overcomes previous limits on the number of devices that can be fabricated on a single chip due to the number of electrical contacts available, without the need to alter existing experimental set ups.

Adaptation to high CO2 concentration in an optimal environment: radiation capture, canopy quantum yield and carbon use efficiency

NASA Technical Reports Server (NTRS)

Monje, O.; Bugbee, B.

1998-01-01

The effect of elevated [CO2] on wheat (Triticum aestivum L. Veery 10) productivity was examined by analysing radiation capture, canopy quantum yield, canopy carbon use efficiency, harvest index and daily C gain. Canopies were grown at either 330 or 1200 micromoles mol-1 [CO2] in controlled environments, where root and shoot C fluxes were monitored continuously from emergence to harvest. A rapidly circulating hydroponic solution supplied nutrients, water and root zone oxygen. At harvest, dry mass predicted from gas exchange data was 102.8 +/- 4.7% of the observed dry mass in six trials. Neither radiation capture efficiency nor carbon use efficiency were affected by elevated [CO2], but yield increased by 13% due to a sustained increase in canopy quantum yield. CO2 enrichment increased root mass, tiller number and seed mass. Harvest index and chlorophyll concentration were unchanged, but CO2 enrichment increased average life cycle net photosynthesis (13%, P < 0.05) and root respiration (24%, P < 0.05). These data indicate that plant communities adapt to CO2 enrichment through changes in C allocation. Elevated [CO2] increases sink strength in optimal environments, resulting in sustained increases in photosynthetic capacity, canopy quantum yield and daily C gain throughout the life cycle.

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

NASA Astrophysics Data System (ADS)

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

2016-02-01

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

Rigidifying fluorescent linkers by metal-organic framework formation for fluorescence blue shift and quantum yield enhancement.

PubMed

Wei, Zhangwen; Gu, Zhi-Yuan; Arvapally, Ravi K; Chen, Ying-Pin; McDougald, Roy N; Ivy, Joshua F; Yakovenko, Andrey A; Feng, Dawei; Omary, Mohammad A; Zhou, Hong-Cai

2014-06-11

We demonstrate that rigidifying the structure of fluorescent linkers by structurally constraining them in metal-organic frameworks (MOFs) to control their conformation effectively tunes the fluorescence energy and enhances the quantum yield. Thus, a new tetraphenylethylene-based zirconium MOF exhibits a deep-blue fluorescent emission at 470 nm with a unity quantum yield (99.9 ± 0.5%) under Ar, representing ca. 3600 cm(-1) blue shift and doubled radiative decay efficiency vs the linker precursor. An anomalous increase in the fluorescence lifetime and relative intensity takes place upon heating the solid MOF from cryogenic to ambient temperatures. The origin of these unusual photoluminescence properties is attributed to twisted linker conformation, intramolecular hindrance, and framework rigidity.

The reaction of NH2 with NO2

NASA Technical Reports Server (NTRS)

Jayanty, R. K. M.; Simonaitis, R.; Heicklen, J.

1976-01-01

Ammonia (NH3) was photolyzed at 213.9 nm in the presence of NO2 at 25 C in order to study the reactions of NH2 with NO2. The products included NO, with a quantum yield of 1.0. The other measured products of the reaction were N2 and N2O with respective quantum yields of 0.94 plus or minus 0.10 and 0.3 in the presence of small amounts of He and 0.65 plus or minus 0.15 and 0.13 in the presence of a large excess of He. The quantum yield for NO2 consumption was 6.0 plus or minus 2.0 in the absence of He. These results are explained in terms of various reactions.

AgCl-doped CdSe quantum dots with near-IR photoluminescence.

PubMed

Kotin, Pavel Aleksandrovich; Bubenov, Sergey Sergeevich; Mordvinova, Natalia Evgenievna; Dorofeev, Sergey Gennadievich

2017-01-01

We report the synthesis of colloidal CdSe quantum dots doped with a novel Ag precursor: AgCl. The addition of AgCl causes dramatic changes in the morphology of synthesized nanocrystals from spherical nanoparticles to tetrapods and finally to large ellipsoidal nanoparticles. Ellipsoidal nanoparticles possess an intensive near-IR photoluminescence ranging up to 0.9 eV (ca. 1400 nm). In this article, we explain the reasons for the formation of the ellipsoidal nanoparticles as well as the peculiarities of the process. The structure, Ag content, and optical properties of quantum dots are also investigated. The optimal conditions for maximizing both the reaction yield and IR photoluminescence quantum yield are found.

"A bridge over troubled gaps": up-conversion driven photocatalysis for hydrogen generation and pollutant degradation by near-infrared excitation.

PubMed

Acosta-Mora, P; Domen, K; Hisatomi, T; Lyu, H; Méndez-Ramos, J; Ruiz-Morales, J C; Khaidukov, N M

2018-02-15

Spectral up-conversion (UC) has been attracting growing interest for the effective harvesting of the near-infrared (NIR) part of sunlight for photocatalytic hydrogen production and environmental purification. We present evidence of NIR-to-UV-VIS photon conversion for degradation of organic dyes and hydrogen and oxygen evolution via water-splitting by TiO 2 and Rh-Cr oxide-loaded SrTiO 3 :Al photocatalysts, respectively.

White light upconversion emissions in Er3+/Tm3+/Yb3+ tridoped oxyfluoride glass

NASA Astrophysics Data System (ADS)

Guan, Xiaoping; Xu, Wei; Zhu, Shuang; Song, Qiutong; Wu, Xijun; Liu, Hailong

2015-10-01

Rare earth ions doped glasses producing visible upconversion emissions are of great interest due to their potential applications in the photonics filed. In fact, practical application of upconversion emissions has been used to obtain color image displays and white light sources. However, there are few reports on the thermal effect on tuning the emission color of the RE doped materials. In this work, the Er3+/Tm3+/Yb3+ tridoped oxyfluoride glasses were prepared through high temperature solid-state method. Under a 980 nm diode laser excitation, the upconversion emissions from the samples were studied. At room-temperature, bright white luminescence, whose CIE chromaticity coordinate was about (0.28, 0.31), can be obtained when the excitation power was 120 mW. The emission color was changed by varying the intensity ratios between RGB bands, which are strongly dependent on the rare earth ions concentration. The temperature dependent color emissions were also investigated. As temperature increased, the intensities for the emission bands presented different decay rates, finally resulting in the changing of the CIE coordinate. When the temperature was 573 K, white light with color coordinate of (0.31, 0.33) was achieved, which matches well with the white reference (0.33, 0.33). The color tunability, high quality of white light and intense emission intensity make the transparent oxyfluoride glasses excellent candidates for applications in solid-state lighting.

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

A pre-protective strategy for precise tumor targeting and efficient photodynamic therapy with a switchable DNA/upconversion nanocomposite.

PubMed

Yu, Zhengze; Ge, Yegang; Sun, Qiaoqiao; Pan, Wei; Wan, Xiuyan; Li, Na; Tang, Bo

2018-04-14

Tumor-specific targeting based on folic acid (FA) is one of the most common and significant approaches in cancer therapy. However, the expression of folate receptors (FRs) in normal tissues will lead to unexpected targeting and unsatisfactory therapeutic effect. To address this issue, we develop a pre-protective strategy for precise tumor targeting and efficient photodynamic therapy (PDT) using a switchable DNA/upconversion nanocomposite, which can be triggered in the acidic tumor microenvironment. The DNA/upconversion nanocomposite is composed of polyacrylic acid (PAA) coated upconversion nanoparticles (UCNPs), the surface of which is modified using FA and chlorin e6 (Ce6) functionalized DNA sequences with different lengths. Initially, FA on the shorter DNA was protected by a longer DNA to prevent the bonding to FRs on normal cells. Once reaching the acidic tumor microenvironment, C base-rich longer DNA forms a C-quadruplex, resulting in the exposure of the FA groups and the bonding of FA and FRs on cancer cell membranes to achieve precise targeting. Simultaneously, the photosensitizer chlorin e6 (Ce6) gets close to the surface of UCNPs, enabling the excitation of Ce6 to generate singlet oxygen ( 1 O 2 ) under near infrared light via Förster resonance energy transfer (FRET). In vivo experiments indicated that higher tumor targeting efficiency was achieved and the tumor growth was greatly inhibited through the pre-protective strategy.

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.

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.

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

PubMed

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

2014-08-04

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

Smart Self-Assembled Nanosystem Based on Water-Soluble Pillararene and Rare-Earth-Doped Upconversion Nanoparticles for pH-Responsive Drug Delivery.

PubMed

Li, Haihong; Wei, Ruoyan; Yan, Gui-Hua; Sun, Ji; Li, Chunju; Wang, Haifang; Shi, Liyi; Capobianco, John A; Sun, Lining

2018-02-07

Exploring novel drug delivery systems with good stability and new structure to integrate pillararene and upconversion nanoparticles (UCNPs) into one system continues to be an important challenge. Herein, we report a novel preparation of a supramolecular upconversion nanosystem via the host-guest complexation based on carboxylate-based pillar[5]arene (WP5) and 15-carboxy-N,N,N-trialkylpentadecan-1-ammonium bromide (1)-functionalized UCNPs to produce WP5⊃1-UCNPs that can be loaded with the chemotherapeutic drug doxorubicin (DOX). Importantly, the WP5 on the surface of the drug-loaded nanosystem can be efficiently protonated under acidic conditions, resulting in the collapse of the nanosystem and drug release. Moreover, cellular uptake confirms that the nanosystem can enter human cervical cancer (HeLa) cells, resulting in drug accumulation in the cells. More importantly, cytotoxicity experiments demonstrated the excellent biocompatibility of WP5⊃1-UCNPs without loading DOX and that the nanosystem DOX-WP5⊃1-UCNPs exhibited an ability of killing HeLa cells effectively. We also investigated magnetic resonance imaging and upconversion luminescence imaging, which may be employed as visual imaging agents in cancer diagnosis and treatment. Thus, in the present work, we show a simple yet powerful strategy to combine UCNPs and pillar[5]arene to produce a unified nanosystem for dual-mode bioimaging-guided therapeutic applications.

Seasonal and spatial variabilities in the water chemistry of prairie pothole wetlands influence the photoproduction of reactive intermediates.

PubMed

McCabe, Andrew J; Arnold, William A

2016-07-01

The hydrology and water chemistry of prairie pothole wetlands vary spatially and temporally, on annual and decadal timescales. Pesticide contamination of wetlands arising from agricultural activities is a foremost concern. Photochemical reactions are important in the natural attenuation of pesticides and may be important in limiting ecological and human exposure. Little is known, however, about the variable influence of wetland water chemistry on indirect photochemistry. In this study, seasonal water samples were collected from seven sites throughout the prairie pothole region over three years to understand the spatiotemporal dynamics of reactive intermediate photoproduction. Samples were classified by the season in which they were collected (spring, summer, or fall) and the typical hydroperiod of the wetland surface water (temporary or semi-permanent). Under photostable conditions, steady-state concentrations and apparent quantum yields or quantum yield coefficients were measured for triplet excited states of dissolved organic matter, singlet oxygen, hydroxyl radical, and carbonate radical under simulated sunlight. Steady-state concentrations and quantum yields increased on average by 15% and 40% from spring to fall, respectively. Temporary wetlands had 40% higher steady-state concentrations of reactive intermediates than semi-permanent wetlands, but 50% lower quantum yields. Computed quantum yields for reactive intermediate formation were used to predict the indirect photochemical half-lives of seven pesticides in average temporary and semi-permanent prairie pothole wetlands. As a first approximation, the predictions agree to within two orders of magnitude of previously reported half-lives. Copyright © 2016 Elsevier Ltd. All rights reserved.

Enhanced performance of dye-sensitized solar cells based on TiO{sub 2} with NIR-absorption and visible upconversion luminescence

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

Liang, Li; Yulin, Yang, E-mail: ylyang@hit.edu.cn; Mi, Zhou

2013-02-15

TiO{sub 2} with NIR-absorption and visible upconversion luminescence (UC-TiO{sub 2}) is prepared by a sol-gel method and calcined at 700 Degree-Sign C for 6 h. The material broadens the response region of dye sensitized solar cells (DSSCs) from an ultraviolet-visible region to the whole region of the solar spectrum. It shifts NIR sunlight to visible light which matches the strong absorbing region of the dye (N719). DSSCs based on UC-TiO{sub 2} achieved higher conversion efficiency than that on raw TiO{sub 2}. UC-TiO{sub 2} was mixed with commercial raw TiO{sub 2} as additive, and the short-circuit current density, open-circuit voltage andmore » conversion efficiency of the DSSC reached to the optimum values 13.38 mA/cm{sup 2}, 0.78 V and 6.63% (AM1.5 global), comparing with the blank values: 7.99 mA/cm{sup 2}, 0.75 V and 4.07%, respectively. Also the mechanisms of upconversion by multiphoton absorption and energy transfer processes are interpreted in this paper. - Graphical abstract: By introducing TiO{sub 2} with NIR-absorption and visible up-conversion luminescence into DSSC, a signal reflection was explored from ultra-violet region to visible region, and to near-IR region. Highlights: Black-Right-Pointing-Pointer TiO{sub 2} with NIR-absorption and visible up-conversion luminescence (UC-TiO{sub 2}) was prepared by a sol-gel method. Black-Right-Pointing-Pointer A systematic characterization and analysis was carried out to discuss the mechanism. Black-Right-Pointing-Pointer A significantly enhanced performance of DSSC was explored by using UC-TiO{sub 2} as an additive.« less

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

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

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

2015-09-07

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

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

NASA Astrophysics Data System (ADS)

Azam, Mohd; Rai, Vineet Kumar

2017-04-01

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

Generalized Weyl-Wigner map and Vey quantum mechanics

NASA Astrophysics Data System (ADS)

Dias, Nuno Costa; Prata, João Nuno

2001-12-01

The Weyl-Wigner map yields the entire structure of Moyal quantum mechanics directly from the standard operator formulation. The covariant generalization of Moyal theory, also known as Vey quantum mechanics, was presented in the literature many years ago. However, a derivation of the formalism directly from standard operator quantum mechanics, clarifying the relation between the two formulations, is still missing. In this article we present a covariant generalization of the Weyl order prescription and of the Weyl-Wigner map and use them to derive Vey quantum mechanics directly from the standard operator formulation. The procedure displays some interesting features: it yields all the key ingredients and provides a more straightforward interpretation of the Vey theory including a direct implementation of unitary operator transformations as phase space coordinate transformations in the Vey idiom. These features are illustrated through a simple example.

Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities

DOE PAGES

Luo, Yue; Ahmadi, Ehsaneh D.; Shayan, Kamran; ...

2017-11-10

Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (F P) up to F P = 180 (average F P = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore,more » the measured ultra-narrow exciton linewidth (18 ueV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. Furthermore, to demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.« less

Blue-green upconversion laser

DOEpatents

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

1990-08-14

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

Blue-green upconversion laser

DOEpatents

Nguyen, Dinh C.; Faulkner, George E.

1990-01-01

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

Dental optical tomography with upconversion nanoparticles—a feasibility study

PubMed Central

Long, Feixiao; Intes, Xavier

2017-01-01

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

Dental optical tomography with upconversion nanoparticles—a feasibility study

NASA Astrophysics Data System (ADS)

Long, Feixiao; Intes, Xavier

2017-06-01

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

Dental optical tomography with upconversion nanoparticles-a feasibility study.

PubMed

Long, Feixiao; Intes, Xavier

2017-06-01

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

Synthesis and characterization of attosecond light vortices in the extreme ultraviolet

PubMed Central

Géneaux, R.; Camper, A.; Auguste, T.; Gobert, O.; Caillat, J.; Taïeb, R.; Ruchon, T.

2016-01-01

Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units absorbed in the process up to very high orders (57). This allows us to synthesize and characterize helically shaped XUV trains of attosecond pulses. To demonstrate a typical use of these new XUV light beams, we show our ability to generate and control, through photoionization, attosecond electron beams carrying OAM. These breakthroughs pave the route for the study of a series of fundamental phenomena and the development of new ultrafast diagnosis tools using either photonic or electronic vortices. PMID:27573787

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

NASA Astrophysics Data System (ADS)

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

2018-05-01

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

Recent Advances in Inorganic Nanoparticle-Based NIR Luminescence Imaging: Semiconductor Nanoparticles and Lanthanide Nanoparticles.

PubMed

Kim, Dokyoon; Lee, Nohyun; Park, Yong Il; Hyeon, Taeghwan

2017-01-18

Several types of nanoparticle-based imaging probes have been developed to replace conventional luminescent probes. For luminescence imaging, near-infrared (NIR) probes are useful in that they allow deep tissue penetration and high spatial resolution as a result of reduced light absorption/scattering and negligible autofluorescence in biological media. They rely on either an anti-Stokes or a Stokes shift process to generate luminescence. For example, transition metal-doped semiconductor nanoparticles and lanthanide-doped inorganic nanoparticles have been demonstrated as anti-Stokes shift-based agents that absorb NIR light through two- or three-photon absorption process and upconversion process, respectively. On the other hand, quantum dots (QDs) and lanthanide-doped nanoparticles that emit in NIR-II range (∼1000 to ∼1350 nm) were suggested as promising Stokes shift-based imaging agents. In this topical review, we summarize and discuss the recent progress in the development of inorganic nanoparticle-based luminescence imaging probes working in NIR range.

Synthesis and characterization of attosecond light vortices in the extreme ultraviolet

DOE PAGES

Géneaux, R.; Camper, A.; Auguste, T.; ...

2016-08-30

Infrared and visible light beams carrying orbital angular momentum (OAM) are currently thoroughly studied for their extremely broad applicative prospects, among which are quantum information, micromachining and diagnostic tools. Here we extend these prospects, presenting a comprehensive study for the synthesis and full characterization of optical vortices carrying OAM in the extreme ultraviolet (XUV) domain. We confirm the upconversion rules of a femtosecond infrared helically phased beam into its high-order harmonics, showing that each harmonic order carries the total number of OAM units absorbed in the process up to very high orders (57). This allows us to synthesize and characterizemore » helically shaped XUV trains of attosecond pulses. To demonstrate a typical use of these new XUV light beams, we show our ability to generate and control, through photoionization, attosecond electron beams carrying OAM. Furthermore, these breakthroughs pave the route for the study of a series of fundamental phenomena and the development of new ultrafast diagnosis tools using either photonic or electronic vortices.« less

High-efficiency electroluminescence and amplified spontaneous emission from a thermally activated delayed fluorescent near-infrared emitter

NASA Astrophysics Data System (ADS)

Kim, Dae-Hyeon; D'Aléo, Anthony; Chen, Xian-Kai; Sandanayaka, Atula D. S.; Yao, Dandan; Zhao, Li; Komino, Takeshi; Zaborova, Elena; Canard, Gabriel; Tsuchiya, Youichi; Choi, Eunyoung; Wu, Jeong Weon; Fages, Frédéric; Brédas, Jean-Luc; Ribierre, Jean-Charles; Adachi, Chihaya

2018-02-01

Near-infrared organic light-emitting diodes and semiconductor lasers could benefit a variety of applications including night-vision displays, sensors and information-secured displays. Organic dyes can generate electroluminescence efficiently at visible wavelengths, but organic light-emitting diodes are still underperforming in the near-infrared region. Here, we report thermally activated delayed fluorescent organic light-emitting diodes that operate at near-infrared wavelengths with a maximum external quantum efficiency of nearly 10% using a boron difluoride curcuminoid derivative. As well as an effective upconversion from triplet to singlet excited states due to the non-adiabatic coupling effect, this donor-acceptor-donor compound also exhibits efficient amplified spontaneous emission. By controlling the polarity of the active medium, the maximum emission wavelength of the electroluminescence spectrum can be tuned from 700 to 780 nm. This study represents an important advance in near-infrared organic light-emitting diodes and the design of alternative molecular architectures for photonic applications based on thermally activated delayed fluorescence.

Can nanotechnology potentiate photodynamic therapy?

PubMed Central

Huang, Ying-Ying; Sharma, Sulbha K.; Dai, Tianhong; Chung, Hoon; Yaroslavsky, Anastasia; Garcia-Diaz, Maria; Chang, Julie; Chiang, Long Y.

2015-01-01

Photodynamic therapy (PDT) uses the combination of non-toxic dyes and harmless visible light to produce reactive oxygen species that can kill cancer cells and infectious microorganisms. Due to the tendency of most photosensitizers (PS) to be poorly soluble and to form nonphotoactive aggregates, drug-delivery vehicles have become of high importance. The nanotechnology revolution has provided many examples of nanoscale drug-delivery platforms that have been applied to PDT. These include liposomes, lipoplexes, nanoemulsions, micelles, polymer nanoparticles (degradable and nondegradable), and silica nanoparticles. In some cases (fullerenes and quantum dots), the actual nanoparticle itself is the PS. Targeting ligands such as antibodies and peptides can be used to increase specificity. Gold and silver nanoparticles can provide plasmonic enhancement of PDT. Two-photon excitation or optical upconversion can be used instead of one-photon excitation to increase tissue penetration at longer wavelengths. Finally, after sections on in vivo studies and nanotoxicology, we attempt to answer the title question, “can nano-technology potentiate PDT?” PMID:26361572

Ionoluminescence properties of polystyrene-hosted fluorophore films induced by helium ions of energy 50-350 keV

NASA Astrophysics Data System (ADS)

Chakraborty, Subha; Huang, Mengbing

2017-10-01

We report on measurements and analysis of ionoluminescence properties of pure polystyrene films and polystyrene films doped with four types of fluorophores in low kinetic energies (50-350 keV) of ion irradiation. We have developed a theoretical model to understand the experimentally observed ionoluminescence behaviors in terms of scintillation yield from individual ion tracks, photophysical energy transfer mechanisms, and irradiation-induced defects. A comparison of the model and experimental results suggests that singlet up-conversion resulting from triplet-triplet annihilation processes may be responsible for enhanced singlet emission of the fluorophores at high ion beam flux densities. Energy transfer from the polystyrene matrix to the fluorophore molecules has been identified as an effective pathway to increasing the fluorescence efficiency in the doped scintillator films.

Quantum yield and rate constant of the singlet 1Δ g oxygen luminescence in an aqueous medium in the presence of nanoscale inhomogeneities

NASA Astrophysics Data System (ADS)

Jarnikova, E. S.; Parkhats, M. V.; Stasheuski, A. S.; Lepeshkevich, S. V.; Dzhagarov, B. M.

2017-04-01

The quantum yields and lifetimes of photosensitized luminescence of the 1Δ g state of singlet oxygen in an aquatic media with a controlled concentration of dielectric anisotropy centers (polyethylene glycol) have been measured using the methods of laser fluorometry. It is established that the quantum yield and the rate constant ( k r ) of the a 1Δ g → X 3Σ g - luminescence of 1O2 increase as the polymer concentration increases. The effect is analyzed within a general approach involving a relationship between kr and dielectric properties of the medium and is explained by the increased density of photon states and the local field factor in the space around O2( a 1Δ g ).

Accurate quantum yields by laser gain vs absorption spectroscopy - Investigation of Br/Br(asterisk) channels in photofragmentation of Br2 and IBr

NASA Technical Reports Server (NTRS)

Haugen, H. K.; Weitz, E.; Leone, S. R.

1985-01-01

Various techniques have been used to study photodissociation dynamics of the halogens and interhalogens. The quantum yields obtained by these techniques differ widely. The present investigation is concerned with a qualitatively new approach for obtaining highly accurate quantum yields for electronically excited states. This approach makes it possible to obtain an accuracy of 1 percent to 3 percent. It is shown that measurement of the initial transient gain/absorption vs the final absorption in a single time-resolved signal is a very accurate technique in the study of absolute branching fractions in photodissociation. The new technique is found to be insensitive to pulse and probe laser characteristics, molecular absorption cross sections, and absolute precursor density.

Cross sections and quantum yields of the 3 micron emission for Er(3+) and Ho(3+) dopants in crystalsls

NASA Astrophysics Data System (ADS)

Payne, Stephen A.; Smith, Larry K.; Krupke, William F.

1995-05-01

The lifetime, quantum yields, and branching ratios for the 2.8 micron emissions of several Er-and Ho-doped fluorides and oxides were measured. Among the fluoride crystals examined, which included LiYF4, BaY2F8, LaF3, and KY3F10, only the Ho:LiFY4 systems showed any proof of nonradiative decay. Conversely, all the oxide crystals were affected by nonradiative processes, resulting in measured quantum yields ranging from 3.6% for Er:Y3Al5O12 to 62% for Er in Gd3Sc2Ga3O12. In addition, plots of the 2.8 micron emission cross sections for seven Er- and Ho-doped crystals were presented.

Sample-averaged biexciton quantum yield measured by solution-phase photon correlation.

PubMed

Beyler, Andrew P; Bischof, Thomas S; Cui, Jian; Coropceanu, Igor; Harris, Daniel K; Bawendi, Moungi G

2014-12-10

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.

A paper-based multiplexed resonance energy transfer nucleic acid hybridization assay using a single form of upconversion nanoparticle as donor and three quantum dots as acceptors.

PubMed

Doughan, Samer; Uddayasankar, Uvaraj; Peri, Aparna; Krull, Ulrich J

2017-04-15

Monodisperse aqueous upconverting nanoparticles (UCNPs) were covalently immobilized on aldehyde modified cellulose paper via reductive amination to evaluate the multiplexing capacity of luminescence resonance energy transfer (LRET) between UCNPs and quantum dots (QDs). This is the first account of a multiplexed bioassay strategy that demonstrates the principle of use of a single form of UCNP as donor and three different color emitting QDs as acceptors to concurrently determine three analytes. Broad absorbance profiles of green, orange and red QDs that spanned from the first exciton absorption peak to the UV region were in overlap with a blue emission band from UCNPs composed of NaYF 4 that was doped with 30% Yb 3+ , 0.5% Tm 3+ , allowing for LRET that was stimulated using 980 nm near-infrared radiation. The characteristic narrow and well-defined emission peaks of UCNPs and QDs allowed for the collection of luminescence from each nanoparticle using a band-pass optical filter and an epi-fluorescence microscope. The LRET system was used for the concurrent detection of uidA, Stx1A and tetA gene fragments with selectivity even in serum samples, and reached limits of detection of 26 fmol, 56 fmol and 76 fmol, respectively. Copyright © 2017 Elsevier B.V. All rights reserved.

Visible-Light Upconversion Carbon Quantum Dots Decorated TiO2 for the Photodegradation of Flowing Gaseous Acetaldehyde

NASA Astrophysics Data System (ADS)

Hu, Yidan; Xie, Xiaofeng; Wang, Xiao; Wang, Yan; Zeng, Yi; Pui, David Y. H.; Sun, Jing

2018-05-01

Carbon-modified photocatalyst has attracted extensive attentions in the field of gaseous pollutant removal, mainly due to the improved adsorption properties and electronic transport of carbon matrix, such as carbon nanotubes, graphene, and fullerene, etc. In this work, carbon quantum dots (CQDs) were employed to enhance the photocatalytic performance of TiO2-based composites for flowing gaseous acetaldehyde removal. Besides the aforementioned advantages of carbon materials, the unique up-converted photoluminescence property of CQDs is capable of extending the optical absorption to visible-light range. Moreover, the electron spin resonance (ESR) results firstly verified a stable existence of Ti3+ defect in the CQDs/TiO2 composite, which is possibly induced by the electron migration from CQDs to TiO2. And the formed Ti3+ donor energy level in the band gap could further help with the visible-light harvesting. During the photodegradation experiments, with two-hour continuous flowing gaseous acetaldehyde injection (500 ppm, 20 sccm), the CQDs/TiO2 composite remained 99% removal efficiency under fluorescent lamp irradiation (λ > 380 nm). The optimized CQDs content was obtained as 3 wt%, and the underlying mechanism was further analyzed by temperature programmed desorption (TPD) methods. This work will push forward the air purification researches by providing new insights of CQDs sensitized photocatalyst.

Detection of early primary colorectal cancer with upconversion luminescent NP-based molecular probes

NASA Astrophysics Data System (ADS)

Liu, Chunyan; Qi, Yifei; Qiao, Ruirui; Hou, Yi; Chan, Kaying; Li, Ziqian; Huang, Jiayi; Jing, Lihong; Du, Jun; Gao, Mingyuan

2016-06-01

Early detection and diagnosis of cancers is extremely beneficial for improving the survival rate of cancer patients and molecular imaging techniques are believed to be relevant for offering clinical solutions. Towards early cancer detection, we developed a primary animal colorectal cancer model and constructed a tumor-specific imaging probe by using biocompatible NaGdF4:Yb,Er@NaGdF4 upconversion luminescent NPs for establishing a sensitive early tumor imaging method. The primary animal tumor model, which can better mimic the human colorectal cancer, was built upon continual administration of 1,2-dimethylhydrazine in Kunming mice and the tumor development was carefully monitored through histopathological and immunohistochemical analyses to reveal the pathophysiological processes and molecular features of the cancer microenvironment. The upconversion imaging probe was constructed through covalent coupling of PEGylated core-shell NPs with folic acid whose receptor is highly expressed in the primary tumors. Upon 980 nm laser excitation, the primary colorectal tumors in the complex abdominal environment were sensitively imaged owing to the ultralow background of the upconversion luminescence and the high tumor-targeting specificity of the nanoprobe. We believe that the current studies provide a highly effective and potential approach for early colorectal cancer diagnosis and tumor surgical navigation.Early detection and diagnosis of cancers is extremely beneficial for improving the survival rate of cancer patients and molecular imaging techniques are believed to be relevant for offering clinical solutions. Towards early cancer detection, we developed a primary animal colorectal cancer model and constructed a tumor-specific imaging probe by using biocompatible NaGdF4:Yb,Er@NaGdF4 upconversion luminescent NPs for establishing a sensitive early tumor imaging method. The primary animal tumor model, which can better mimic the human colorectal cancer, was built upon continual administration of 1,2-dimethylhydrazine in Kunming mice and the tumor development was carefully monitored through histopathological and immunohistochemical analyses to reveal the pathophysiological processes and molecular features of the cancer microenvironment. The upconversion imaging probe was constructed through covalent coupling of PEGylated core-shell NPs with folic acid whose receptor is highly expressed in the primary tumors. Upon 980 nm laser excitation, the primary colorectal tumors in the complex abdominal environment were sensitively imaged owing to the ultralow background of the upconversion luminescence and the high tumor-targeting specificity of the nanoprobe. We believe that the current studies provide a highly effective and potential approach for early colorectal cancer diagnosis and tumor surgical navigation. Electronic supplementary information (ESI) available: (1) Molecular structure of Jeffamine-modified FA; (2) immunohistochemical analysis of FR expression in the colorectal tissue derived from mice treated with NaCl at different weeks; (3) biodistributions of probes of NP-FA and NP-IgG in the main organs of mice. See DOI: 10.1039/c5nr07858j

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

NASA Astrophysics Data System (ADS)

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

2016-05-01

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

Water relation, leaf gas exchange and chlorophyll a fluorescence imaging of soybean leaves infected with Colletotrichum truncatum.

PubMed

Dias, Carla Silva; Araujo, Leonardo; Alves Chaves, Joicy Aparecida; DaMatta, Fábio M; Rodrigues, Fabrício A

2018-06-01

Considering the potential of anthracnose to decrease soybean yield and the need to gain more information regarding its effect on soybean physiology, the present study performed an in-depth analysis of the photosynthetic performance of soybean leaflets challenged with Colletotrichum truncatum by combining chlorophyll a fluorescence images with gas-exchange measurements and photosynthetic pigment pools. There were no significant differences between non-inoculated and inoculated plants in leaf water potential, apparent hydraulic conductance, net CO 2 assimilation rate, stomatal conductance to water vapor and transpiration rate. For internal CO 2 concentration, significant difference between non-inoculated and inoculated plants occurred only at 36 h after inoculation. Reductions in the values of the chlorophyll a fluorescence parameters [initial fluorescence (F 0 ), maximal fluorescence (F m ), maximal photosystem II quantum yield (F v /F m ), quantum yield of regulated energy dissipation (Y(NPQ))] and increases in effective PS II quantum yield (Y(II)), quantum yield of non-regulated energy dissipation Y(NO) and photochemical quenching coefficient (q P ) were noticed on the necrotic vein tissue in contrast to the surrounding leaf tissue. It appears that the impact of the infection by C. truncatum on the photosynthetic performance of the leaflets was minimal considering the preference of the fungus to colonize the veins. Copyright © 2018 Elsevier Masson SAS. All rights reserved.

Violet-to-Blue Gain and Lasing from Colloidal CdS Nanoplatelets: Low-Threshold Stimulated Emission Despite Low Photoluminescence Quantum Yield

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

Diroll, Benjamin T.; Talapin, Dmitri V.; Schaller, Richard D.

Amplified spontaneous emission (ASE) and lasing from solution-processed materials are demonstrated in the challenging violet-to-blue (430–490 nm) spectral region for colloidal nanoplatelets of CdS and newly synthesized core/shell CdS/ZnS nanoplatelets. Despite modest band-edge photoluminescence quantum yields of 2% or less for single excitons, which we show results from hole trapping, the samples exhibit low ASE thresholds. Furthermore, four-monolayer CdS samples show ASE at shorter wavelengths than any reported film of colloidal quantum-confined material. This work underlines that low quantum yields for single excitons do not necessarily lead to a poor gain medium. The low ASE thresholds originate from negligible dispersionmore » in thickness, large absorption cross sections of 2.8 × 10–14 cm–2, and rather slow (150 to 300 ps) biexciton recombination. We show that under higher-fluence excitation, ASE can kinetically outcompete hole trapping. Using nanoplatelets as the gain medium, lasing is observed in a linear optical cavity. This work confirms the fundamental advantages of colloidal quantum well structures as gain media, even in the absence of high photoluminescence efficiency.« less

Inkjet printed fluorescent nanorod layers exhibit superior optical performance over quantum dots

NASA Astrophysics Data System (ADS)

Halivni, Shira; Shemesh, Shay; Waiskopf, Nir; Vinetsky, Yelena; Magdassi, Shlomo; Banin, Uri

2015-11-01

Semiconductor nanocrystals exhibit unique fluorescence properties which are tunable in size, shape and composition. The high quantum yield and enhanced stability have led to their use in biomedical imaging and flat panel displays. Here, semiconductor nanorod based inkjet inks are presented, overcoming limitations of the commonly reported quantum dots in printing applications. Fluorescent seeded nanorods were found to be outstanding candidates for fluorescent inks, due to their low particle-particle interactions and negligible self-absorption. This is manifested by insignificant emission shifts upon printing, even in highly concentrated printed layers and by maintenance of a high fluorescence quantum yield, unlike quantum dots which exhibit fluorescence wavelength shifts and quenching effects. This behavior results from the reduced absorption/emission overlap, accompanied by low energy transfer efficiencies between the nanorods as supported by steady state and time resolved fluorescence measurements. The new seeded nanorod inks enable patterning of thin fluorescent layers, for demanding light emission applications such as signage and displays.Semiconductor nanocrystals exhibit unique fluorescence properties which are tunable in size, shape and composition. The high quantum yield and enhanced stability have led to their use in biomedical imaging and flat panel displays. Here, semiconductor nanorod based inkjet inks are presented, overcoming limitations of the commonly reported quantum dots in printing applications. Fluorescent seeded nanorods were found to be outstanding candidates for fluorescent inks, due to their low particle-particle interactions and negligible self-absorption. This is manifested by insignificant emission shifts upon printing, even in highly concentrated printed layers and by maintenance of a high fluorescence quantum yield, unlike quantum dots which exhibit fluorescence wavelength shifts and quenching effects. This behavior results from the reduced absorption/emission overlap, accompanied by low energy transfer efficiencies between the nanorods as supported by steady state and time resolved fluorescence measurements. The new seeded nanorod inks enable patterning of thin fluorescent layers, for demanding light emission applications such as signage and displays. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr06248a

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: Kinetics and quantum yield of photoluminescence of EuFOD3 doped into a nanoporous glass with the help of supercritical CO2

NASA Astrophysics Data System (ADS)

Bagratashvili, V. N.; Gerasimova, V. I.; Gordienko, V. M.; Tsypina, S. I.; Chutko, E. A.

2008-08-01

The kinetics of photoluminescence of a EuFOD3 metalloorganic compound doped into a nanoporous Vycor glass by the method of supercritical fluid impregnation is studied. The lifetime of luminescence of EuFOD3 molecules in pores excited by an excimer XeCl laser was 40 μs, which is considerably smaller than this lifetime (150—890 μs) in solutions. The quantum yield of luminescence of EuFOD3 was estimate as ≈4×10-4.

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

PubMed

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

2015-11-02

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

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

NASA Astrophysics Data System (ADS)

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

2013-12-01

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

Rare-earth doped transparent nano-glass-ceramics: a new generation of photonic integrated devices

NASA Astrophysics Data System (ADS)

Rodríguez-Armas, Vicente Daniel; Tikhomirov, Victor K.; Méndez-Ramos, Jorge; Yanes, Angel C.; Del-Castillo, Javier; Furniss, David; Seddon, Angela B.

2007-05-01

We report on optical properties and prospect applications on rare-earth doped oxyfluoride precursor glass and ensuing nano-glass-ceramics. We find out the spectral optical gain of the nano-glass-ceramics and show that its flatness and breadth are advantageous as compared to contemporary used erbium doped optical amplifiers. We present the possibility of flat gain cross-section erbium doped waveguide amplifiers as short 'chip', all-optical, devices capable of dense wavelength division multiplexing, including the potential for direct writing of these devices inside bulk glasses for three-dimensional photonic integration. We carried out a comparative study of the up-conversion luminescence in Er 3+-doped and Yb 3+-Er 3+-Tm 3+ co-doped samples, which indicates that these materials can be used as green/red tuneable up-conversion phosphors and white light simulation respectively. Observed changes in the spectra of the up-conversion luminescence provide a tool for tuning the colour opening the way for producing 3-dimensional optical recording.

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

NASA Astrophysics Data System (ADS)

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

2017-10-01

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

Optical thermometry based on green upconversion emission in Er3+/Yb3+ codoped BaGdF5 glass ceramics

NASA Astrophysics Data System (ADS)

Wu, Ting; Zhao, Shilong; Lei, Ruoshan; Huang, Lihui; Xu, Shiqing

2018-02-01

Er3+/Yb3+ codoped BaGdF5 glass ceramics have been prepared and used to develop a portable all-fiber temperature sensor based on fluorescence intensity ratio technique. XRD and TEM results affirm the generation of BaGdF5 nanocrystals in the borosilicate glass. Eu3+ ions are used as spectral probe to investigate external environment around rare earth (RE) ions. Intense green upconversion emissions from Er3+ ions are detected in the BaGdF5 glass ceramics and their intensity are enhanced about three orders of magnitude after heat treatment, which is attributed to the enrichment of RE ions in the BaGdF5 phase. Based on green upconversion emission from Er3+ ions, the temperature sensing property of the portable all-fiber temperature sensor is studied. The maximum absolute sensitivity is 15.5 × 10-4 K-1 at 567 K and the relative sensitivity is 1.28% K-1 at 298 K, respectively.

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Enabling valley selective exciton scattering in monolayer WSe2 through upconversion

PubMed Central

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

2017-01-01

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

Plasmon-enhanced energy transfer for improved upconversion of infrared radiation in doped-lanthanide nanocrystals

NASA Astrophysics Data System (ADS)

Sun, Qi; Mundoor, Haridas; Ribot, Josep; Singh, Vivek; Smalyukh, Ivan; Nagpal, Prashant

2014-03-01

Upconversion of infrared radiation into visible light has been investigated for applications in biological imaging and photovoltaics. However, low conversion efficiency due to small absorption cross-section for infrared light (Yb3+) , and slow rate of energy transfer (to Er3+ states) has prevented application of upconversion photoluminescence (UPL) for diffuse sunlight or imaging tissue samples. Here, we utilize resonant surface plasmon polaritons (SPP) waves to enhance UPL in doped-lanthanide nanocrystals. Our analysis indicates that SPP waves not only enhance the electromagnetic field, and hence weak Purcell effect, but also increases the rate of resonant energy transfer from Yb3+ to Er3+ ions by 6 fold. While we do observe strong metal mediated quenching (14 fold) of green fluorescence on flat metal surfaces, the nanostructured metal is resonant in the infrared, and hence enhances the nanocrystal UPL. This strong columbic effect on energy transfer can have important implications for other fluorescent and excitonic systems too.

(Bio)hybrid materials based on optically active particles

NASA Astrophysics Data System (ADS)

Reitzig, Manuela; Härtling, Thomas; Opitz, Jörg

2014-03-01

In this contribution we provide an overview of current investigations on optically active particles (nanodiamonds, upconversion phospors) for biohybrid and sensing applications. Due to their outstanding properties nanodiamonds gain attention in various application elds such as microelectronics, optical monitoring, medicine, and biotechnology. Beyond the typical diamond properties such as high thermal conductivity and extreme hardness, the carbon surface and its various functional groups enable diverse chemical and biological surface functionalization. At Fraunhofer IKTS-MD we develop a customization of material surfaces via integration of chemically modi ed nanodiamonds at variable surfaces, e.g bone implants and pipelines. For the rst purpose, nanodiamonds are covalently modi ed at their surface with amino or phosphate functionalities that are known to increase adhesion to bone or titanium alloys. The second type of surface is approached via mechanical implementation into coatings. Besides nanodiamonds, we also investigate the properties of upconversion phosphors. In our contribution we show how upconversion phosphors are used to verify sterilization processes via a change of optical properties due to sterilizing electron beam exposure.

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

PubMed

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

2011-02-01

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

Giant enhancement of upconversion in ultra-small Er³⁺/Yb³⁺:NaYF₄ nanoparticles via laser annealing.

PubMed

Bednarkiewicz, A; Wawrzynczyk, D; Gagor, A; Kepinski, L; Kurnatowska, M; Krajczyk, L; Nyk, M; Samoc, M; Strek, W

2012-04-13

Most of the synthesis routes of lanthanide-doped phosphors involve thermal processing which results in nanocrystallite growth, stabilization of the crystal structure and augmentation of luminescence intensity. It is of great interest to be able to transform the sample in a spatially localized manner, which may lead to many applications like 2D and 3D data storage, anti-counterfeiting protection, novel design bio-sensors and, potentially, to fabrication of metamaterials, 3D photonic crystals or plasmonic devices. Here we demonstrate irreversible spatially confined infrared-laser-induced annealing (LIA) achieved in a thin layer of dried colloidal solution of ultra-small ∼8 nm NaYF₄ nanocrystals (NCs) co-doped with 2% Er³⁺ and 20% Yb³⁺ ions under a localized tightly focused beam from a continuous wave 976 nm medium power laser diode excitation. The LIA results from self-heating due to non-radiative relaxation accompanying the NIR laser energy upconversion in lanthanide ions. We notice that localized LIA appears at optical power densities as low as 15.5 kW cm⁻² (∼354 ± 29 mW) threshold in spots of 54 ± 3 µm diameter obtained with a 10 × microscope objective. In the course of detailed studies, a complete recrystallization to different phases and giant 2-3 order enhancement in luminescence yield is found. Our results are highly encouraging and let us conclude that the upconverting ultra-small lanthanide-doped nanophosphors are particularly promising for direct laser writing applications.

Giant enhancement of upconversion in ultra-small Er3+/Yb3+:NaYF4 nanoparticles via laser annealing

NASA Astrophysics Data System (ADS)

Bednarkiewicz, A.; Wawrzynczyk, D.; Gagor, A.; Kepinski, L.; Kurnatowska, M.; Krajczyk, L.; Nyk, M.; Samoc, M.; Strek, W.

2012-04-01

Most of the synthesis routes of lanthanide-doped phosphors involve thermal processing which results in nanocrystallite growth, stabilization of the crystal structure and augmentation of luminescence intensity. It is of great interest to be able to transform the sample in a spatially localized manner, which may lead to many applications like 2D and 3D data storage, anti-counterfeiting protection, novel design bio-sensors and, potentially, to fabrication of metamaterials, 3D photonic crystals or plasmonic devices. Here we demonstrate irreversible spatially confined infrared-laser-induced annealing (LIA) achieved in a thin layer of dried colloidal solution of ultra-small ˜8 nm NaYF4 nanocrystals (NCs) co-doped with 2% Er3+ and 20% Yb3+ ions under a localized tightly focused beam from a continuous wave 976 nm medium power laser diode excitation. The LIA results from self-heating due to non-radiative relaxation accompanying the NIR laser energy upconversion in lanthanide ions. We notice that localized LIA appears at optical power densities as low as 15.5 kW cm-2 (˜354 ± 29 mW) threshold in spots of 54 ± 3 µm diameter obtained with a 10 × microscope objective. In the course of detailed studies, a complete recrystallization to different phases and giant 2-3 order enhancement in luminescence yield is found. Our results are highly encouraging and let us conclude that the upconverting ultra-small lanthanide-doped nanophosphors are particularly promising for direct laser writing applications.

MMW/THz imaging using upconversion to visible, based on glow discharge detector array and CCD camera

NASA Astrophysics Data System (ADS)

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

2017-10-01

An inexpensive upconverting MMW/THz imaging method is suggested here. The method is based on glow discharge detector (GDD) and silicon photodiode or simple CCD/CMOS camera. The GDD was previously found to be an excellent room-temperature MMW radiation detector by measuring its electrical current. The GDD is very inexpensive and it is advantageous due to its wide dynamic range, broad spectral range, room temperature operation, immunity to high power radiation, and more. An upconversion method is demonstrated here, which is based on measuring the visual light emitting from the GDD rather than its electrical current. The experimental setup simulates a setup that composed of a GDD array, MMW source, and a basic CCD/CMOS camera. The visual light emitting from the GDD array is directed to the CCD/CMOS camera and the change in the GDD light is measured using image processing algorithms. The combination of CMOS camera and GDD focal plane arrays can yield a faster, more sensitive, and very inexpensive MMW/THz camera, eliminating the complexity of the electronic circuits and the internal electronic noise of the GDD. Furthermore, three dimensional imaging systems based on scanning prohibited real time operation of such imaging systems. This is easily solved and is economically feasible using a GDD array. This array will enable us to acquire information on distance and magnitude from all the GDD pixels in the array simultaneously. The 3D image can be obtained using methods like frequency modulation continuous wave (FMCW) direct chirp modulation, and measuring the time of flight (TOF).

Separation of photoactive conformers based on hindered diarylethenes: efficient modulation in photocyclization quantum yields.

PubMed

Li, Wenlong; Jiao, Changhong; Li, Xin; Xie, Yongshu; Nakatani, Keitaro; Tian, He; Zhu, Weihong

2014-04-25

Endowing both solvent independency and excellent thermal bistability, the benzobis(thiadiazole)-bridged diarylethene system provides an efficient approach to realize extremely high photocyclization quantum yields (Φo-c , up to 90.6 %) by both separating completely pure anti-parallel conformer and suppressing intramolecular charge transfer (ICT). © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Chemiluminescence of nitrogen-rich quantum dots in diperiodatoargentate(III) solution and its application in ferulic acid analysis.

PubMed

Fu, Zhaofu; Li, Gongke; Hu, Yufei

2016-12-01

A novel chemiluminescence (CL) system based on the reaction of fluorescent water-soluble nitrogen-rich quantum dots (N-dots) and diperiodatoargentate(III) (DPA) was developed. The prepared N-dots have a small size (≤10 nm) and high percentage of nitrogen (39.9 %), which exceeds the content of carbon in the same N-dots. The N-dots exhibit characteristic blue fluorescence under UV light and up-conversion luminescence. The relatively intense CL emission is based on the direct oxidation of N-dots by DPA. The CL emission may be attributed to the high nitrogen content and the special structure of the N-dots. The CL mechanism of N-dots and DPA was investigated by using CL, UV-Vis absorption, IR, fluorescence, and radical scavenging experiments. This investigation provides a way to study the optical properties of N-dots. The analytical applicability of the N-dots and DPA CL system in the determination of ferulic acid (FA) was explored. The CL intensity was linearly proportional to the concentration of ferulic acid from 3.0 × 10 -7 to 1.0 × 10 -5 g mL -1 with a detection limit of 8.0 × 10 -8 g mL -1 (3σ); the relative standard deviation was 2.4 % for 4.0 × 10 -7 g mL -1 FA (n = 9). The proposed method was successfully applied to the determination of ferulic acid in Angelica sinensis. The study provides valuable insight into the role of nitrogen-rich quantum dots in CL.

An ultrafast spectroscopic and quantum mechanical investigation of multiple emissions in push-pull pyridinium derivatives bearing different electron donors.

PubMed

Carlotti, B; Benassi, E; Cesaretti, A; Fortuna, C G; Spalletti, A; Barone, V; Elisei, F

2015-08-28

A joint experimental and theoretical approach, involving state-of-the-art femtosecond fluorescence up-conversion measurements and quantum mechanical computations including vibronic effects, was employed to get a deep insight into the excited state dynamics of two cationic dipolar chromophores (Donor-π-Acceptor(+)) where the electron deficient portion is a N-methyl pyridinium and the electron donor a trimethoxyphenyl or a pyrene, respectively. The ultrafast spectroscopic investigation, and the time resolved area normalised emission spectra in particular, revealed a peculiar multiple emissive behaviour and allowed the distinct emitting states to be remarkably distinguished from solvation dynamics, occurring in water in a similar timescale. The two and three emissions experimentally detected for the trimethoxyphenyl and pyrene derivatives, respectively, were associated with specific local emissive minima in the potential energy surface of S1 on the ground of quantum-mechanical calculations. A low polar and planar Locally Excited (LE) state together with a highly polar and Twisted Intramolecular Charge Transfer (TICT) state is identified to be responsible for the dual emission of the trimethoxyphenyl compound. Interestingly, the more complex photobehaviour of the pyrenyl derivative was explained considering the contribution to the fluorescence coming not only from the LE and TICT states but also from a nearly Planar Intramolecular Charge Transfer (PICT) state, with both the TICT and the PICT generated from LE by progressive torsion around the quasi-single bond between the methylpyridinium and the ethene bridge. These findings point to an interconversion between rotamers for the pyrene compound taking place in its excited state against the Non-equilibrated Excited Rotamers (NEER) principle.

Photodissociation of quantum state-selected diatomic molecules yields new insight into ultracold chemistry

NASA Astrophysics Data System (ADS)

McDonald, Mickey; McGuyer, Bart H.; Lee, Chih-Hsi; Apfelbeck, Florian; Zelevinsky, Tanya

2016-05-01

When a molecule is subjected to a sufficiently energetic photon it can break apart into fragments through a process called ``photodissociation''. For over 70 years this simple chemical reaction has served as a vital experimental tool for acquiring information about molecular structure, since the character of the photodissociative transition can be inferred by measuring the 3D photofragment angular distribution (PAD). While theoretical understanding of this process has gradually evolved from classical considerations to a fully quantum approach, experiments to date have not yet revealed the full quantum nature of this process. In my talk I will describe recent experiments involving the photodissociation of ultracold, optical lattice-trapped, and fully quantum state-resolved 88Sr2 molecules. Optical absorption images of the PADs produced in these experiments reveal features which are inherently quantum mechanical in nature, such as matter-wave interference between output channels, and are sensitive to the quantum statistics of the molecular wavefunctions. The results of these experiments cannot be predicted using quasiclassical methods. Instead, we describe our results with a fully quantum mechanical model yielding new intuition about ultracold chemistry.

Aqueous synthesis of high bright and tunable near-infrared AgInSe2-ZnSe quantum dots for bioimaging.

PubMed

Che, Dongchen; Zhu, Xiaoxu; Wang, Hongzhi; Duan, Yourong; Zhang, Qinghong; Li, Yaogang

2016-02-01

Efficient synthetic methods for near-infrared quantum dots with good biophysical properties as bioimaging agents are urgently required. In this work, a simple and fast synthesis of highly luminescent, near-infrared AgInSe2-ZnSe quantum dots (QDs) with tunable emissions in aqueous media is reported. This method avoids high temperature and pressure and organic solvents to directly generate water-dispersible AgInSe2-ZnSe QDs. The photoluminescence emission peak of the AgInSe2-ZnSe QDs ranged from 625 to 940nm, with quantum yields up to 31%. The AgInSe2-ZnSe QDs with high quantum yield, near-infrared and low cytotoxic could be used as good cell labels, showing great potential applications in bio-imaging. Copyright © 2015 Elsevier Inc. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

1994-05-01

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

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

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

Rao, Ling; Lu, Wei; Wang, Haibo

2015-04-15

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

Bioinspired near-infrared-excited sensing platform for in vitro antioxidant capacity assay based on upconversion nanoparticles and a dopamine-melanin hybrid system.

PubMed

Wang, Dong; Chen, Chuan; Ke, Xuebin; Kang, Ning; Shen, Yuqing; Liu, Yongliang; Zhou, Xi; Wang, Hongjun; Chen, Changqing; Ren, Lei

2015-02-11

A novel core-shell structure based on upconversion fluorescent nanoparticles (UCNPs) and dopamine-melanin has been developed for evaluation of the antioxidant capacity of biological fluids. In this approach, dopamine-melanin nanoshells facilely formed on the surface of UCNPs act as ultraefficient quenchers for upconversion fluorescence, contributing to a photoinduced electron-transfer mechanism. This spontaneous oxidative polymerization of the dopamine-induced quenching effect could be effectively prevented by the presence of various antioxidants (typically biothiols, ascorbic acid (Vitamin C), and Trolox). The chemical response of the UCNPs@dopamine-melanin hybrid system exhibited great selectivity and sensitivity toward antioxidants relative to other compounds at 100-fold higher concentration. A satisfactory correlation was established between the ratio of the "anti-quenching" fluorescence intensity and the concentration of antioxidants. Besides the response of the upconversion fluorescence signal, a specific evaluation process for antioxidants could be visualized by the color change from colorless to dark gray accompanied by the spontaneous oxidation of dopamine. The near-infrared (NIR)-excited UCNP-based antioxidant capacity assay platform was further used to evaluate the antioxidant capacity of cell extracts and human plasma, and satisfactory sensitivity, repeatability, and recovery rate were obtained. This approach features easy preparation, fluorescence/visual dual mode detection, high specificity to antioxidants, and enhanced sensitivity with NIR excitation, showing great potential for screening and quantitative evaluation of antioxidants in biological systems.

Quantum yield for carbon monoxide production in the 248 nm photodissociation of carbonyl sulfide (OCS)

NASA Technical Reports Server (NTRS)

Zhao, Z.; Stickel, R. E.; Wine, P. H.

1995-01-01

Tunable diode laser absorption spectroscopy has been coupled with excimer laser flash photolysis to measure the quantum yield for CO production from 248 nm photodissociation of carbonyl sulfide (OCS) relative to the well-known quantum yield for CO production from 248 nm photolysis of phosgene (Cl2CO2). The temporal resolution of the experiments was sufficient to distinguish CO formed directly by photodissociation from that formed by subsequent S((sup 3)P(sub J)) reaction with OCS. Under the experimental conditions employed, CO formation via the fast S((sup 1)D(sub 2)) + OCS reaction was minimal. Measurements at 297K and total pressures from 4 to 100 Torr N2 + N2O show the CO yield to be greater than 0.95 and most likely unity. This result suggests that the contribution of OCS as a precursor to the lower stratospheric sulfate aerosol layer is somewhat larger than previously thought.

Culture expansion of adipose derived stromal cells. A closed automated Quantum Cell Expansion System compared with manual flask-based culture.

PubMed

Haack-Sørensen, Mandana; Follin, Bjarke; Juhl, Morten; Brorsen, Sonja K; Søndergaard, Rebekka H; Kastrup, Jens; Ekblond, Annette

2016-11-16

Adipose derived stromal cells (ASCs) are a rich and convenient source of cells for clinical regenerative therapeutic approaches. However, applications of ASCs often require cell expansion to reach the needed dose. In this study, cultivation of ASCs from stromal vascular fraction (SVF) over two passages in the automated and functionally closed Quantum Cell Expansion System (Quantum system) is compared with traditional manual cultivation. Stromal vascular fraction was isolated from abdominal fat, suspended in α-MEM supplemented with 10% Fetal Bovine Serum and seeded into either T75 flasks or a Quantum system that had been coated with cryoprecipitate. The cultivation of ASCs from SVF was performed in 3 ways: flask to flask; flask to Quantum system; and Quantum system to Quantum system. In all cases, quality controls were conducted for sterility, mycoplasmas, and endotoxins, in addition to the assessment of cell counts, viability, immunophenotype, and differentiation potential. The viability of ASCs passage 0 (P0) and P1 was above 96%, regardless of cultivation in flasks or Quantum system. Expression of surface markers and differentiation potential was consistent with ISCT/IFATS standards for the ASC phenotype. Sterility, mycoplasma, and endotoxin tests were consistently negative. An average of 8.0 × 10 7 SVF cells loaded into a Quantum system yielded 8.96 × 10 7 ASCs P0, while 4.5 × 10 6 SVF cells seeded per T75 flask yielded an average of 2.37 × 10 6 ASCs-less than the number of SVF cells seeded. ASCs P1 expanded in the Quantum system demonstrated a population doubling (PD) around 2.2 regardless of whether P0 was previously cultured in flasks or Quantum, while ASCs P1 in flasks only reached a PD of 1.0. Manufacturing of ASCs in a Quantum system enhances ASC expansion rate and yield significantly relative to manual processing in T-flasks, while maintaining the purity and quality essential to safe and robust cell production. Notably, the use of the Quantum system entails significantly reduced working hours and thereby costs.

Analysis of wavelength-dependent photoisomerization quantum yields in bilirubins by fitting two exciton absorption bands

NASA Astrophysics Data System (ADS)

Mazzoni, M.; Agati, G.; Troup, G. J.; Pratesi, R.

2003-09-01

The absorption spectra of bilirubins were deconvoluted by two Gaussian curves of equal width representing the exciton bands of the non-degenerate molecular system. The two bands were used to study the wavelength dependence of the (4Z, 15Z) rightarrow (4Z, 15E) configurational photoisomerization quantum yield of the bichromophoric bilirubin-IXalpha (BR-IX), the intrinsically asymmetric bile pigment associated with jaundice and the symmetrically substituted bilirubins (bilirubin-IIIalpha and mesobilirubin-XIIIalpha), when they are irradiated in aqueous solution bound to human serum albumin (HSA). The same study was performed for BR-IX in ammoniacal methanol solution (NH4OH/MeOH). The quantum yields of the configurational photoprocesses were fitted with a combination function of the two Gaussian bands normalized to the total absorption, using the proportionality coefficients and a scaling factor as parameters. The decrease of the (4Z, 15Z) rightarrow (4Z, 15E) quantum yield with increasing wavelength, which occurs for wavelengths longer than the most probable Franck-Condon transition of the molecule, did not result in a unique function of the exciton absorptions. In particular we found two ranges corresponding to different exciton interactions with different proportionality coefficients and scaling factors. The wavelength-dependent photoisomerization of bilirubins was described as an abrupt change in quantum yield as soon as the resulting excitation was strongly localized in each chromophore. The change was correlated to a variation of the interaction between the two chromophores when the short-wavelength exciton absorption became vanishingly small. With the help of the circular dichroism (CD) spectrum of BR-IX in HSA, a small band was resolved in the bilirubin absorption spectrum, delivering part of the energy required for the (4Z, 15Z) rightarrow (4Z, 15E) photoisomerization of the molecule.

Comparisons of Photosynthetic Responses of Xanthium strumarium and Helianthus annuus to Chronic and Acute Water Stress in Sun and Shade 1

PubMed Central

Ben, Gui-Ying; Osmond, C. Barry; Sharkey, Thomas D.

1987-01-01

We have examined the effects of mild, chronic water stress and acute water stress on two water stress sensitive plants, Xanthium strumarium and Helianthus annuus. Using a combination of the leaf disc O2 electrode to measure the light responses of photosynthesis and 77 K fluorescence to monitor damage to the primary photochemistry, we have found the following: (a) The CO2 saturated rate of photosynthesis at high light is the most water stress sensitive parameter measured. (b) The apparent quantum yield (moles O2 per mole photons) was slightly, if at all, affected by mild water stress (>−1.5 megapascals). (c) Severe water stress (<−1.5 megapascals) reduced the quantum yield of photosynthesis regardless of whether the stress was applied in sun or shade. The light independent reduction of quantum yield was not associated with a reduction in 77 K fluorescence (Fv/Fm) indicating that the quantum yield reduction was not the result of damage to primary photochemistry. (d) The diel fluctuation in 77 K fluorescence seen in sun-exposed control leaves was greatly exaggerated in water stressed leaves because of enhanced decline in 77 K fluorescence in the morning. The rate of recovery was similar in both control and water stressed leaves. Shaded leaves showed no change in 77 K fluorescence regardless of whether water stress was imposed or not. (e) The water stress sensitive plants used in these experiments did not recover from acute water stress severe enough to reduce the quantum yield or chronic water stress which lasted long enough that light dependent damage to primary photochemistry occurred. PMID:16665465

Comparisons of Photosynthetic Responses of Xanthium strumarium and Helianthus annuus to Chronic and Acute Water Stress in Sun and Shade.

PubMed

Ben, G Y; Osmond, C B; Sharkey, T D

1987-06-01

We have examined the effects of mild, chronic water stress and acute water stress on two water stress sensitive plants, Xanthium strumarium and Helianthus annuus. Using a combination of the leaf disc O(2) electrode to measure the light responses of photosynthesis and 77 K fluorescence to monitor damage to the primary photochemistry, we have found the following: (a) The CO(2) saturated rate of photosynthesis at high light is the most water stress sensitive parameter measured. (b) The apparent quantum yield (moles O(2) per mole photons) was slightly, if at all, affected by mild water stress (>-1.5 megapascals). (c) Severe water stress (<-1.5 megapascals) reduced the quantum yield of photosynthesis regardless of whether the stress was applied in sun or shade. The light independent reduction of quantum yield was not associated with a reduction in 77 K fluorescence (F(v)/F(m)) indicating that the quantum yield reduction was not the result of damage to primary photochemistry. (d) The diel fluctuation in 77 K fluorescence seen in sun-exposed control leaves was greatly exaggerated in water stressed leaves because of enhanced decline in 77 K fluorescence in the morning. The rate of recovery was similar in both control and water stressed leaves. Shaded leaves showed no change in 77 K fluorescence regardless of whether water stress was imposed or not. (e) The water stress sensitive plants used in these experiments did not recover from acute water stress severe enough to reduce the quantum yield or chronic water stress which lasted long enough that light dependent damage to primary photochemistry occurred.

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

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

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

2015-11-15

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

Laser flash photolysis of ozone - O/1D/ quantum yields in the fall-off region 297-325 nm

NASA Technical Reports Server (NTRS)

Brock, J. C.; Watson, R. T.

1980-01-01

The wavelength dependence of the quantum yield for O(1D) production from ozone photolysis has been determined between 297.5 nm and 325 nm in order to resolve serious discrepancies among previous studies. The results of this investigation are compared to earlier work by calculating atmospheric production rate constants for O(1D). It is found that for the purpose of calculating this rate constant, there is now good agreement among three studies at 298 K. Furthermore, it appears that previous data on the temperature dependence of the O(1D) quantum yield fall-off is adequate for determining the vertical profile of the O(1D) production rate constant. Several experimental difficulties associated with using NO2(asterisk) chemiluminescence to monitor O(1D) have been identified.

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

DOE PAGES

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; ...

2014-11-19

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here in this study, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS andmore » InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals.« less

Quantitative photoabsorption and fluorescence spectroscopy of benzene, naphthalene, and some derivatives at 106-295 nm

NASA Technical Reports Server (NTRS)

Suto, Masako; Wang, Xiuyan; Shan, Jun; Lee, L. C.

1992-01-01

Photoabsorption and fluorescence cross sections of benzene, (o-, m-, p-) xylenes, naphthalene, 1-methylnaphthalene, and 2-ethylnaphthalene in the gas phase are measured at 106-295 nm using synchrotron radiation as a light source. Fluorescences are observed from the photoexcitation of benzene and xylenes at 230-280 nm and from naphthalene and its derivatives at 190-295 nm. The absolute fluorescence cross section is determined by calibration with respect to the emission intensity of the NO(A-X) system, for which the fluorescence quantum yield is equal to 1. To cross-check the current calibration method, the quantum yield of the SO2(C-X) system at 220-230 nm was measured since it is about equal to 1. The current quantum-yield data are compared with previously published values measured by different methods.

Sample-Averaged Biexciton Quantum Yield Measured by Solution-Phase Photon Correlation

PubMed Central

Beyler, Andrew P.; Bischof, Thomas S.; Cui, Jian; Coropceanu, Igor; Harris, Daniel K.; Bawendi, Moungi G.

2015-01-01

The brightness of nanoscale optical materials such as semiconductor nanocrystals is currently limited in high excitation flux applications by inefficient multiexciton fluorescence. We have devised a solution-phase photon correlation measurement that can conveniently and reliably measure the average biexciton-to-exciton quantum yield ratio of an entire sample without user selection bias. This technique can be used to investigate the multiexciton recombination dynamics of a broad scope of synthetically underdeveloped materials, including those with low exciton quantum yields and poor fluorescence stability. Here, we have applied this method to measure weak biexciton fluorescence in samples of visible-emitting InP/ZnS and InAs/ZnS core/shell nanocrystals, and to demonstrate that a rapid CdS shell growth procedure can markedly increase the biexciton fluorescence of CdSe nanocrystals. PMID:25409496

A Phosphine-Free Route to Size-Adjustable CdSe and CdSe/CdS Core-Shell Quantum Dots for White-Light-Emitting Diodes.

PubMed

Zhang, Yugang; Li, Guopeng; Zhang, Ting; Song, Zihang; Wang, Hui; Zhang, Zhongping; Jiang, Yang

2018-03-01

The selenium dioxide was used as the precursor to synthesize wide-size-ranged CdSe quantum dots (2.4-5.7 nm) via hot-injection route. The CdSe quantum dots are featured with high crystalline, monodisperse, zinc blende structure and wide emission region (530-635 nm). In order to improve the stability and quantum yield, a phosphine-free single-molecular precursor approach is used to obtain CdSe/CdS core/shell quantum dots. The CdSe/CdS quantum dots are highly fluorescent with quantum yield up to 65%, and persist the good monodispersity and high crystallinity. Moreover, the quantum dots white light-emitting-diodes are fabricated by using the resultant red emission core/shell quantum dots and Y3Al5O12:Ce3+ yellow phosphors as color-conversion layers on a blue InGaN chip. The prepared light-emitting-diodes show good performance with CIE-1931 coordinated of (0.3583, 0.3349), an Ra of 92.9, and a Tc of 4410 K at 20 mA, which indicate that the combination of red-emission QDs and yellow phophors as a promising approach to obtain warm WLEDs with good color rendering.

Excited-state properties of nucleic acid components

NASA Astrophysics Data System (ADS)

Salet, C.; Bensasson, R. V.; Becker, R. S.

1981-12-01

Measurements were made of the fluorescence and phosphorescence spectra and lifetimes, and also of the absorption spectra, lifetimes, extinction coefficients, and quantum yields of the T1 lower triplet states of thymine, uracil, their N, N'-dimethyl derivatives, thymidine, thymidine monophosphate, uridine, and uridine monophosphate in various solvents at 300 °K. The influence of the solvent on the quantum yield of the T1 state of nucleic acid components is discussed.

Laboratory Measurements of Photolytic Parameters for Formaldehyde.

DTIC Science & Technology

1980-11-01

dynamic dilution methods. Compressed air stored in steel cylinders, carefully selected to contain carbon monoxide and hydrogen at mixing ratios of...in air has been investi- gated in the laboratory at two temperatures: 300 and 220 K. Quantum yields for the formation of CO and H2 were determined at...procedures in the case of pure formaldehyde gave consistent results. (b) Quantum Yields Mixtures of formaldehyde in air were photolyzed in a

Synthesis and characterization of near-infrared absorbing water soluble squaraines and study of their photodynamic effects in DLA live cells.

PubMed

Shafeekh, Kulathinte M; Soumya, Mohanannair S; Rahim, Moochikkadavath A; Abraham, Annie; Das, Suresh

2014-01-01

Here, we report the synthesis, photophysical properties and photodynamic effects in DLA live cells of three water soluble squaraine dyes, viz. bisbenzothiazolium squaraine dyes SQMI and SQDI with iodine in one and both benzothiazolium units, respectively, and an unsymmetrical squaraine dye ASQI containing iodinated benzothiazolium and aniline substituents. The diiodinated SQDI showed an anomalous trend in both fluorescence and triplet quantum yields over the monoiodinated SQMI, with SQDI showing higher fluorescence and lower triplet quantum yields compared to SQMI. Nanosecond laser flash photolysis of SQDI and SQMI indicated the formation of triplet excited states with quantum yield of 0.19 and 0.26, respectively. On photoirradiation, both the SQDI and SQMI generate singlet oxygen and it was observed that both dyes undergoing oxidation reactions with the singlet oxygen generated. ASQI which exhibited a lower triplet quantum yield of 0.06 was, however, stable and did not react with the singlet oxygen generated. In vitro cytotoxicity studies of these dyes in DLA live cells were performed using Trypan blue dye exclusion method and it reflect an order of cytotoxicity of SQDI>SQMI>ASQI. Intracellular generation of the ROS was confirmed by dichlorofluorescein assay after the in vitro PDT. © 2014 The American Society of Photobiology.

Efficiencies of induction of DNA double strand breaks in solution by photoabsorption at phosphorus and platinum.

PubMed

Maeda, Munetoshi; Kobayashi, Katsumi; Hieda, Kotaro

2004-01-01

This paper aims at determining and comparing the cross sections and quantum yields for DNA strand break induction by the Auger effect at the K-shell of phosphorus and at the LIII-shell of platinum. Using synchrotron radiation, free and Pt-bound pBR322 plasmid DNA were irradiated in solution with monochromatic X-rays, the energies of which were 2.153 and 2.147 keV, corresponding to "on" and "below" the phosphorus K-shell photoabsorption, and 11.566 and 11.542 keV for "above" and "below" the L(III)-shell photoabsorption of platinum, respectively. To suppress indirect effects by hydroxyl radicals, DMSO (1M) was used as a scavenger. The inner-shell photoabsorption of phosphorus and of platinum significantly increased the induction of DNA double strand breaks (DSB), whereas it had little effect on single strand break (SSB) induction. The quantum yields for the induction of DSB were calculated to be 0.017 and 1.13, in the case of phosphorus and platinum, respectively. CONCLSIONS: The value of the quantum yield for the DSB induction of platinum was about 66-fold larger than that for the phosphorus. These results clearly demonstrate that the quantum yield of DSB depends upon the magnitude of the Auger cascade.

Towards efficient solar hydrogen production by intercalated carbon nitride photocatalyst.

PubMed

Gao, Honglin; Yan, Shicheng; Wang, Jiajia; Huang, Yu An; Wang, Peng; Li, Zhaosheng; Zou, Zhigang

2013-11-07

The development of efficient photocatalytic material for converting solar energy to hydrogen energy as viable alternatives to fossil-fuel technologies is expected to revolutionize energy shortage and environment issues. However, to date, the low quantum yield for solar hydrogen production over photocatalysts has hindered advances in the practical applications of photocatalysis. Here, we show that a carbon nitride intercalation compound (CNIC) synthesized by a simple molten salt route is an efficient polymer photocatalyst with a high quantum yield. We found that coordinating the alkali metals into the C-N plane of carbon nitride will induce the un-uniform spatial charge distribution. The electrons are confined in the intercalated region while the holes are in the far intercalated region, which promoted efficient separation of photogenerated carriers. The donor-type alkali metal ions coordinating into the nitrogen pots of carbon nitrides increase the free carrier concentration and lead to the formation of novel nonradiative paths. This should favor improved transport of the photogenerated electron and hole and decrease the electron-hole recombination rate. As a result, the CNIC exhibits a quantum yield as high as 21.2% under 420 nm light irradiation for solar hydrogen production. Such high quantum yield opens up new opportunities for using cheap semiconducting polymers as energy transducers.

Intense visible emission from ZnO/PAAX (X = H or Na) nanocomposite synthesized via a simple and scalable sol-gel method

NASA Astrophysics Data System (ADS)

Zhu, Y.; Apostoluk, A.; Gautier, P.; Valette, A.; Omar, L.; Cornier, T.; Bluet, J. M.; Masenelli-Varlot, K.; Daniele, S.; Masenelli, B.

2016-03-01

Intense visible nano-emitters are key objects for many technologies such as single photon source, bio-labels or energy convertors. Chalcogenide nanocrystals have ruled this domain for several decades. However, there is a demand for cheaper and less toxic materials. In this scheme, ZnO nanoparticles have appeared as potential candidates. At the nanoscale, they exhibit crystalline defects which can generate intense visible emission. However, even though photoluminescence quantum yields as high as 60% have been reported, it still remains to get quantum yield of that order of magnitude which remains stable over a long period. In this purpose, we present hybrid ZnO/polyacrylic acid (PAAH) nanocomposites, obtained from the hydrolysis of diethylzinc in presence of PAAH, exhibiting quantum yield systematically larger than 20%. By optimizing the nature and properties of the polymeric acid, the quantum yield is increased up to 70% and remains stable over months. This enhancement is explained by a model based on the hybrid type II heterostructure formed by ZnO/PAAH. The addition of PAAX (X = H or Na) during the hydrolysis of ZnEt2 represents a cost effective method to synthesize scalable amounts of highly luminescent ZnO/PAAX nanocomposites.

Faster search by lackadaisical quantum walk

NASA Astrophysics Data System (ADS)

Wong, Thomas G.

2018-03-01

In the typical model, a discrete-time coined quantum walk searching the 2D grid for a marked vertex achieves a success probability of O(1/log N) in O(√{N log N}) steps, which with amplitude amplification yields an overall runtime of O(√{N} log N). We show that making the quantum walk lackadaisical or lazy by adding a self-loop of weight 4 / N to each vertex speeds up the search, causing the success probability to reach a constant near 1 in O(√{N log N}) steps, thus yielding an O(√{log N}) improvement over the typical, loopless algorithm. This improved runtime matches the best known quantum algorithms for this search problem. Our results are based on numerical simulations since the algorithm is not an instance of the abstract search algorithm.

Highly intensified upconversion luminescence of Ca(2+) -doped Yb/Er:NaGdF(4) nanocrystals prepared by a solvothermal route.

PubMed

Lei, Lei; Chen, Daqin; Xu, Ju; Zhang, Rui; Wang, Yuansheng

2014-03-01

Upon introducing Ca(2+) dopants into the grain lattices by substituting Gd(3+) ions, irregular Yb/Er:NaGdF4 nanocrystals prepared through a simple solvothermal route convert into highly uniform nanorods. Meanwhile, their upconversion luminescence intensifies by about 200 times, probably due to a modification of the crystal structure of NaGdF4 and an improvement in the crystallinity of the nanophase. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Tailoring dye-sensitized upconversion nanoparticle excitation bands towards excitation wavelength selective imaging

DOE PAGES

Wu, Xiang; Lee, Hyungseok; Bilsel, Osman; ...

2015-01-01

One of the key roadblocks in UCNP development is its extremely limited choices of excitation wavelengths. We report a generic design to program UCNPs to possess highly tunable dye characteristic excitation bands. Using such distinctive properties, we were able to develop a new excitation wavelength selective security imaging. Finally, this work unleashed the greater freedom of the excitation wavelengths of the upconversion nanoparticles and we believe it is a game-changer in the field and this method will enable numerous applications that are currently limited by existing UCNPs.

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

PubMed

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

2016-09-01

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

NIR-Mediated Nanohybrids of Upconversion Nanophosphors and Fluorescent Conjugated Polymers for High-Efficiency Antibacterial Performance Based on Fluorescence Resonance Energy Transfer.

PubMed

Li, Junting; Zhao, Qi; Shi, Feng; Liu, Chenghui; Tang, Yanli

2016-12-01

A novel nanohybrid comprised of upconversion nanophosphors (UCNPs) and fluorescent conjugated polymers (PFVCN) is rationally fabricated. The new UCNP/PFVCN nanohybrids combine the excellent antibacterial ability of PFVCN and the near IR (NIR) absorbing property of UCNPs, which allows for NIR-mediated antibacterial through the effective fluorescence resonance energy transfer from UCNPs to PFVCN accompanied with generation of reactive oxygen species to kill bacteria. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Up-conversion media on basis single crystals BaY2F8 for UV and VUV solid state lasers

NASA Astrophysics Data System (ADS)

Pushkar, A. A.; Ouvarova, T. V.; Molchanov, V. N.

2007-04-01

Crystal BaY IIF 8 represents the big interest as the perspective active media for lasers ultra-violet (UV) and vacuumultra- violet (VUV) regions. For the decision of problems with solarization this media and a choice of sources pump it is offered to use up-conversion mechanisms pump with activators from rare-earth elements (RE). We have developed technology of grown of oriented monocrystals BaY IIF 8, have defined influence of orientation on growth rate and quality ofthe received monocrystals.

ACTIVE MEDIA: BaY2F8 single crystals doped with rare-earth ions as promising up-conversion media for UV and VUV lasers

NASA Astrophysics Data System (ADS)

Pushkar', A. A.; Uvarova, T. V.; Molchanov, V. N.

2008-04-01

BaY2F8 crystals are studied as promising active media for UV and VUV lasers. The up-conversion pumping of rare-earth activators is proposed to solve problems related to the solarisation of the medium and the selection of pump sources. The technology of growing oriented BaY2F8 single crystals is developed and the influence of the crystal orientation on the growth rate and quality of single crystals is determined.

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

PubMed

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

2017-09-22

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

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

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

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

Orfield, Noah J.; McBride, James R.; Wang, Feng

Physical variations in colloidal nanostructures give rise to heterogeneity in expressed optical behavior. This correlation between nanoscale structure and function demands interrogation of both atomic structure and photophysics at the level of single nanostructures to be fully understood. In this paper, by conducting detailed analyses of fine atomic structure, chemical composition, and time-resolved single-photon photoluminescence data for the same individual nanocrystals, we reveal inhomogeneity in the quantum yields of single nonblinking “giant” CdSe/CdS core/shell quantum dots (g-QDs). We find that each g-QD possesses distinctive single exciton and biexciton quantum yields that result mainly from variations in the degree of charging,more » rather than from volume or structure inhomogeneity. We further establish that there is a very limited nonemissive “dark” fraction (<2%) among the studied g-QDs and present direct evidence that the g-QD core must lack inorganic passivation for the g-QD to be “dark”. Finally and therefore, in contrast to conventional QDs, ensemble photoluminescence quantum yield is principally defined by charging processes rather than the existence of dark g-QDs.« less

Strongly Coupled Tin-Halide Perovskites to Modulate Light Emission: Tunable 550-640 nm Light Emission (FWHM 36-80 nm) with a Quantum Yield of up to 6.4.

PubMed

Chen, Min-Yi; Lin, Jin-Tai; Hsu, Chia-Shuo; Chang, Chung-Kai; Chiu, Ching-Wen; Chen, Hao Ming; Chou, Pi-Tai

2018-05-01

Colloidal perovskite quantum dots represent one of the most promising materials for applications in solar cells and photoluminescences. These devices require a low density of crystal defects and a high yield of photogenerated carriers, which are difficult to realize in tin-halide perovskite because of the intrinsic instability of tin during nucleation. Here, an enhancement in the luminescent property of tin-halide perovskite nanoplates (TPNPs) that are composed of strongly coupled layered structures with the chemical formula of PEA 2 SnX 4 (PEA = C 6 H 5 (CH 2 ) 2 NH 3 , X = Br, I) is reported. TPNPs (X = I) show an emission at a wavelength of 640 nm, with high quantum yield of 6.40 ± 0.14% and full width at half maximum (FWHM) as small as 36 nm. The presence of aliphatic carboxylic acid is found to play a key role in reducing the tin perovskite defect density, which significantly improves the emission intensity and stability of TPNPs. Upon mixing iodo- and bromo- precursors, the emission wavelength is successfully tuned from 640 nm (PEA 2 SnI 4 ) to 550 nm (PEA 2 SnBr 4 ), with a corresponding emission quantum yield and FWHM of 0.16-6.40% and 36-80 nm, respectively. The results demonstrate a major advance for the emission yield and tunability of tin-halide perovskites. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photoswitchable Fluorescent Diarylethene Derivatives with Thiophene 1,1-Dioxide Groups: Effect of Alkyl Substituents at the Reactive Carbons

PubMed Central

Sumi, Takaki; Irie, Masahiro

2017-01-01

Photoswitching and fluorescent properties of sulfone derivatives of 1,2-bis(2-alkyl-4-methyl-5-phenyl-3-thienyl)perfluorocyclopentene, 1–5, having methyl, ethyl, n-propyl, i-propyl, and i-butyl substituents at the reactive carbons (2- and 2′-positions) of the thiophene 1,1-dioxide rings were studied. Diarylethenes 1–5 underwent isomerization reactions between open-ring and closed-ring forms upon alternate irradiation with ultraviolet (UV) and visible light and showed fluorescence in the closed-ring forms. The alkyl substitution at the reactive carbons affects the fluorescent property of the closed-ring isomers. The closed-ring isomers 2b–5b with ethyl, n-propyl, i-propyl, and i-butyl substituents show higher fluorescence quantum yields than 1b with methyl substituents. In polar solvents, the fluorescence quantum yield of 1b markedly decreases, while 2b–5b maintain the relatively high fluorescence quantum yields. Although the cycloreversion quantum yields of the derivatives with methyl, ethyl, n-propyl, and i-propyl substituents are quite low and in the order of 10−5, introduction of i-butyl substituents was found to increase the yield up to the order of 10−3. These results indicate that appropriate alkyl substitution at the reactive carbons is indispensable for properly controlling the photoswitching and fluorescent properties of the photoswitchable fluorescent diarylethenes, which are potentially applicable to super-resolution fluorescence microscopies. PMID:28869489

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

Mthethwa, T.P.; Moloto, M.J., E-mail: mmoloto@uj.ac.za; De Vries, A.

Graphical abstract: SEM images of CdS/PMMA showing coiling as loading of CdS nanoparticles is increased. Thermal stability is increased with increase in %loading of both CdS and CdSe nanoparticles. Research highlights: {yields} TOPO-capped CdS and HDA-capped CdSe nanoparticles were synthesized and fully characterized. {yields} The nanoparticles were mixed with the polymer, PMMA using electrospinning technique using 2, 5 and 10% weight loadings. {yields} The mixture was spun to produce fibres with optical and thermal properties showing significant change and also the increase in loading causing bending or spiraling. {yields} Both TEM images for nanoparticles and SEM for fibres shows themore » morphology and sizes of the particles. -- Abstract: Electrospinning technique was used to fabricate poly(methyl methacrylate) (PMMA) fibres incorporating CdS and CdSe quantum dots (nanoparticles). Different nanoparticle loadings (2, 5 and 10 wt% with respect to PMMA) were used and the effect of the quantum dots on the properties of the fibres was studied. The optical properties of the hybrid composite fibres were investigated by photoluminescence and UV-vis spectrophotometry. Scanning electron microscopy (SEM), X-ray diffraction and FTIR spectrophotometry were also used to investigate the morphology and structure of the fibres. The optical studies showed that the size-tunable optical properties can be achieved in the polymer fibres by addition of quantum dots. SEM images showed that the morphologies of the fibres were dependent on the added amounts of quantum dots. A spiral type of morphology was observed with an increase in the concentration of CdS and CdSe nanoparticles. Less beaded structures and bigger diameter fibres were obtained at higher quantum dot concentrations. X-ray diffractometry detected the amorphous peaks of the polymer and even after the quantum dots were added and the FTIR analysis shows that there was no considerable interaction between the quantum dots and the polymer fibres at low concentration of quantum dots however at higher concentrations some interactions were observed which shows that QDs were present on the surfaces of the fibres.« less

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

A synchronous game for binary constraint systems

NASA Astrophysics Data System (ADS)

Kim, Se-Jin; Paulsen, Vern; Schafhauser, Christopher

2018-03-01

Recently, Slofstra proved that the set of quantum correlations is not closed. We prove that the set of synchronous quantum correlations is not closed, which implies his result, by giving an example of a synchronous game that has a perfect quantum approximate strategy but no perfect quantum strategy. We also exhibit a graph for which the quantum independence number and the quantum approximate independence number are different. We prove new characterisations of synchronous quantum approximate correlations and synchronous quantum spatial correlations. We solve the synchronous approximation problem of Dykema and the second author, which yields a new equivalence of Connes' embedding problem in terms of synchronous correlations.

Raising yield potential in wheat: increasing photosynthesis capacity and efficiency

USDA-ARS?s Scientific Manuscript database

Increasing wheat yields to help to ensure food security is a major challenge. Meeting this challenge requires a quantum improvement in the yield potential of wheat. Past increases in yield potential have largely resulted from improvements in harvest index not through increased biomass. Further large...

Correlation complementarity yields bell monogamy relations.

PubMed

Kurzyński, P; Paterek, T; Ramanathan, R; Laskowski, W; Kaszlikowski, D

2011-05-06

We present a method to derive Bell monogamy relations by connecting the complementarity principle with quantum nonlocality. The resulting monogamy relations are stronger than those obtained from the no-signaling principle alone. In many cases, they yield tight quantum bounds on the amount of violation of single and multiple qubit correlation Bell inequalities. In contrast with the two-qubit case, a rich structure of possible violation patterns is shown to exist in the multipartite scenario.

The effect of axial ligands on the quantum yield of singlet oxygen of new silicon phthalocyanine

NASA Astrophysics Data System (ADS)

Lv, Huafei; Zhang, Xuemei; Yu, Xinxin; Pan, Sujuan; Xie, Shusen; Yang, Hongqin; Peng, Yiru

2016-10-01

The singlet oxygen (1O2) production abilitity is an important factor to assess their potential as effective of photosensitizers. In this paper, the 1O2 production rate, production rate constant and quantum yield of silicon(IV) phthalocyanine axially bearing 1-3 generation dendritic substituents were evaluated by a high performance liquid chromatographic method. The results show that the 1O2 production rate and production rate constant of these compounds increase gradually with dendritic generations increase. And the 1O2 quantum yield of silicon(IV) phthalocyanine with first generation dendritic ligand was the highest. This may be due to the isolation effect of the dendritic ligands on the phthalocyanine core. The parameters of the observed 1O2 production properties will provide valuable data for these dendrimer phthalocyanines as promising photosensitizer in PDT application.

Photochemical studies of a fluorescent chlorophyll catabolite--source of bright blue fluorescence in plant tissue and efficient sensitizer of singlet oxygen.

PubMed

Jockusch, Steffen; Turro, Nicholas J; Banala, Srinivas; Kräutler, Bernhard

2014-02-01

Fluorescent chlorophyll catabolites (FCCs) are fleeting intermediates of chlorophyll breakdown, which is seen as an enzyme controlled detoxification process of the chlorophylls in plants. However, some plants accumulate large amounts of persistent FCCs, such as in senescent leaves and in peels of yellow bananas. The photophysical properties of such a persistent FCC (Me-sFCC) were investigated in detail. FCCs absorb in the near UV spectral region and show blue fluorescence (max at 437 nm). The Me-sFCC fluorescence had a quantum yield of 0.21 (lifetime 1.6 ns). Photoexcited Me-sFCC intersystem crosses into the triplet state (quantum yield 0.6) and generates efficiently singlet oxygen (quantum yield 0.59). The efficient generation of singlet oxygen makes fluorescent chlorophyll catabolites phototoxic, but might also be useful as a (stress) signal and for defense of the plant tissue against infection by pathogens.

Short-Term Flooding Effects on Gas Exchange and Quantum Yield of Rabbiteye Blueberry (Vaccinium ashei Reade) 1

PubMed Central

Davies, Frederick S.; Flore, James A.

1986-01-01

Roots of 1.5-year-old `Woodard' rabbiteye blueberry plants (Vaccinium ashei Reade) were flooded in containers or maintained at container capacity over a 5-day period. Carbon assimilation, and stomatal and residual conductances were monitored on one fully expanded shoot/plant using an open flow gas analysis system. Quantum yield was calculated from light response curves. Carbon assimilation and quantum yield of flooded plants decreased to 64 and 41% of control values, respectively, after 1 day of flooding and continued decreasing to 38 and 27% after 4 days. Stomatal and residual conductances to CO2 also decreased after 1 day of flooding compared with those of unflooded plants with residual conductance severely limiting carbon assimilation after 4 days of flooding. Stomatal opening occurred in 75 to 90 minutes and rate of opening was unaffected by flooding. PMID:16664791

Oligonucleotide Sensor Based on Selective Capture of Upconversion Nanoparticles Triggered by Target-Induced DNA Interstrand Ligand Reaction

PubMed Central

2017-01-01

We present a sensor that exploits the phenomenon of upconversion luminescence to detect the presence of specific sequences of small oligonucleotides such as miRNAs among others. The sensor is based on NaYF4:Yb,Er@SiO2 nanoparticles functionalized with ssDNA that contain azide groups on the 3′ ends. In the presence of a target sequence, interstrand ligation is possible via the click-reaction between one azide of the upconversion probe and a DBCO-ssDNA-biotin probe present in the solution. As a result of this specific and selective process, biotin is covalently attached to the surface of the upconversion nanoparticles. The presence of biotin on the surface of the nanoparticles allows their selective capture on a streptavidin-coated support, giving a luminescent signal proportional to the amount of target strands present in the test samples. With the aim of studying the analytical properties of the sensor, total RNA samples were extracted from healthy mosquitoes and were spiked-in with a specific target sequence at different concentrations. The result of these experiments revealed that the sensor was able to detect 10–17 moles per well (100 fM) of the target sequence in mixtures containing 100 ng of total RNA per well. A similar limit of detection was found for spiked human serum samples, demonstrating the suitability of the sensor for detecting specific sequences of small oligonucleotides under real conditions. In contrast, in the presence of noncomplementary sequences or sequences having mismatches, the luminescent signal was negligible or conspicuously reduced. PMID:28332400

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

NASA Astrophysics Data System (ADS)

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

2018-04-01

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

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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