High quantum-yield phosphors via quantum splitting and upconversion

NASA Astrophysics Data System (ADS)

Jeong, Joayoung

The Gd3+ ion has been used to induce quantum splitting in luminescent materials by using cross-relaxation energy transfer (CRET). In Nd:LiGdF4, quantum splitting results from a two-step CRET between Gd3+ and Nd3+, first involving a transition 6G→6I on Gd3+ and an excitation within the 4f3 configuration of Nd3+ followed by a second CRET that brings Gd3+ to 6P7/2. The excited Nd3+ ion rapidly relaxes nonradiatively to the emitting 4F3/2. The excited Gd3+ ion then transfers its energy back to Nd3+, which gives rise to the second photon. The result is a quantum yield of 1.05 +/- 0.35 with emission in the NIR following excitation at 175 nm. GdF3:Pr3+, Eu 3+ also exhibits quantum splitting, but only at very low concentration of Pr3+ (0.3%) and Eu3+ (0.2%), resulting in a quantum yield of approximately 20% under 160-nm excitation. Host intrinsic emission via a self-trapped exciton (STE) was also examined as a means to sensitize Gd3+ emission. The material ScPO4:Gd 3+ exhibits a high absolute quantum yield of 0.9 +/- 0.2 under 170-nm excitation, demonstrating a potentially new and efficient pathway for exciting quantum splitting phosphors. Single crystals of the material GdZrF7 were grown, and its structure was established via single-crystal X-ray diffraction methods. Doped samples of GdZrF7:Yb3+, Er3+ exhibit bright up-conversion luminescence with light output that is up to twice that of a commercial material based on the host Gd2O2S. When doped with Eu3+, the fluoride also emits a nearly white color under vacuum ultraviolet excitation with an absolute quantum yield near 0.9. The new compound Gd4.67(SiO4)3S was synthesized and studied. The structure was established via single-crystal X-ray methods, and the luminescence of Tb3+ samples was investigated.

The Chameleonic Nature of Platinum(II) Imidazopyridine Complexes.

PubMed

Pinter, Piermaria; Pittkowski, Rebecca; Soellner, Johannes; Strassner, Thomas

2017-10-12

The synthesis and characterization of cyclometalated C^C* platinum(II) complexes with unique photophysical properties, aggregation induced enhancement of the quantum yields with a simultaneous decrease of phosphorescence lifetimes, is reported. Additionally, a change of emission color is induced by variation of the excitation wavelength. The aggregation behavior of these complexes is controlled by the steric demand of the substituents. The photophysical properties of these complexes are investigated through emission-excitation matrix analysis (EEM). The monomeric complexes are excellent room temperature phosphorescent blue emitters with emission maxima below 470 nm and quantum yields of up to 93 %. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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.

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.

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.

High-Performance Blue-Excitable Yellow Phosphor Obtained from an Activated Solvochromic Bismuth-Fluorophore Metal–Organic Framework

DOE PAGES

Deibert, Benjamin J.; Velasco, Ever; Liu, Wei; ...

2016-06-23

Here, we report the synthesis, structure, and photoluminescence properties of a new bismuth based luminescent metal-organic framework (LMOF). The framework is comprised of a 9-coordinated Bi 3+ building unit and 4', 4''', 4''''', 4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis([1,1'-biphenyl]-4-carboxylic acid) (H 4tcbpe) organic linker, which has strong yellow aggregation induced emission (AIE). The structure can be viewed as two interpenetrated 4,4-anionic nets that are stabilized by K + ions forming one-dimensional helical inorganic chains by connecting bismuth nodes through shared oxygen bonds. The as-made LMOF has a bluish emission centered at 459 nm with an internal quantum yield of 57% when excited at 360 nm.more » The emission properties of the LMOF were found to be highly solvochromic with respect to DMF. Upon partial solvent removal, the framework undergoes significant red-shifting to a greenish emission centered at 500 nm. Complete removal of DMF results in additional red-shifting fluorescence coupled with structural changes. The resulting material has strong blue-excitable (455 nm) yellow emission centered at 553 nm, with a quantum yield of 74%, which is maintained after heating in air for 5 days at 90°C. This is the second highest quantum yield value for blue-excited yellow emission among all reported LMOFs.« less

High-Performance Blue-Excitable Yellow Phosphor Obtained from an Activated Solvochromic Bismuth-Fluorophore Metal–Organic Framework

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

Deibert, Benjamin J.; Velasco, Ever; Liu, Wei

Here, we report the synthesis, structure, and photoluminescence properties of a new bismuth based luminescent metal-organic framework (LMOF). The framework is comprised of a 9-coordinated Bi 3+ building unit and 4', 4''', 4''''', 4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis([1,1'-biphenyl]-4-carboxylic acid) (H 4tcbpe) organic linker, which has strong yellow aggregation induced emission (AIE). The structure can be viewed as two interpenetrated 4,4-anionic nets that are stabilized by K + ions forming one-dimensional helical inorganic chains by connecting bismuth nodes through shared oxygen bonds. The as-made LMOF has a bluish emission centered at 459 nm with an internal quantum yield of 57% when excited at 360 nm.more » The emission properties of the LMOF were found to be highly solvochromic with respect to DMF. Upon partial solvent removal, the framework undergoes significant red-shifting to a greenish emission centered at 500 nm. Complete removal of DMF results in additional red-shifting fluorescence coupled with structural changes. The resulting material has strong blue-excitable (455 nm) yellow emission centered at 553 nm, with a quantum yield of 74%, which is maintained after heating in air for 5 days at 90°C. This is the second highest quantum yield value for blue-excited yellow emission among all reported LMOFs.« less

Free volume dependence of an ionic molecular rotor in Fluoroalkylphosphate (FAP) based ionic liquids

NASA Astrophysics Data System (ADS)

Singh, Prabhat K.; Mora, Aruna K.; Nath, Sukhendu

2016-01-01

The emission properties of Thioflavin-T (ThT), a cationic molecular rotor, have been investigated in two fluoroalkylphosphate ([FAP]) anion based ionic liquids, namely, 1-ethyl-3-methylimidazolium tris(pentafluoroethyl)trifluorophosphate and 1-(2-hydroxyethyl)-3-methylimidazolium tris(pentafluoroethyl)trifluorophosphate, over a wide temperature range. The micro-viscosities of ionic liquids around ThT, measured from the emission quantum yield, are found to be quite different from their bulk viscosities. The temperature dependence of the viscosity and the emission quantum yield reveals that, despite the very low shear viscosity of these ILs, the non-radiative torsional relaxation has a strong dependence on the free volume of these [FAP] anion based ILs.

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 .

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.

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.

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

Luminescence and luminescence quenching of highly efficient Y2Mo4O15:Eu3+ phosphors and ceramics

PubMed Central

Janulevicius, Matas; Marmokas, Paulius; Misevicius, Martynas; Grigorjevaite, Julija; Mikoliunaite, Lina; Sakirzanovas, Simas; Katelnikovas, Arturas

2016-01-01

A good LED phosphor must possess strong enough absorption, high quantum yields, colour purity, and quenching temperatures. Our synthesized Y2Mo4O15:Eu3+ phosphors possess all of these properties. Excitation of these materials with near-UV or blue radiation yields bright red emission and the colour coordinates are relatively stable upon temperature increase. Furthermore, samples doped with 50% Eu3+ showed quantum yields up to 85%, what is suitable for commercial application. Temperature dependent emission spectra revealed that heavily Eu3+ doped phosphors possess stable emission up to 400 K and lose half of the efficiency only at 515 K. In addition, ceramic disks of Y2Mo4O15:75%Eu3+ phosphor with thickness of 0.71 and 0.98 mm were prepared and it turned out that they efficiently convert radiation of 375 and 400 nm LEDs to the red light, whereas combination with 455 nm LED yields purple colour. PMID:27180941

Luminescence and luminescence quenching of highly efficient Y2Mo4O15:Eu(3+) phosphors and ceramics.

PubMed

Janulevicius, Matas; Marmokas, Paulius; Misevicius, Martynas; Grigorjevaite, Julija; Mikoliunaite, Lina; Sakirzanovas, Simas; Katelnikovas, Arturas

2016-05-16

A good LED phosphor must possess strong enough absorption, high quantum yields, colour purity, and quenching temperatures. Our synthesized Y2Mo4O15:Eu(3+) phosphors possess all of these properties. Excitation of these materials with near-UV or blue radiation yields bright red emission and the colour coordinates are relatively stable upon temperature increase. Furthermore, samples doped with 50% Eu(3+) showed quantum yields up to 85%, what is suitable for commercial application. Temperature dependent emission spectra revealed that heavily Eu(3+) doped phosphors possess stable emission up to 400 K and lose half of the efficiency only at 515 K. In addition, ceramic disks of Y2Mo4O15:75%Eu(3+) phosphor with thickness of 0.71 and 0.98 mm were prepared and it turned out that they efficiently convert radiation of 375 and 400 nm LEDs to the red light, whereas combination with 455 nm LED yields purple colour.

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

Viscosity and medium effects on the fluorescence and photochemical behaviour of some aryl chalcones

NASA Astrophysics Data System (ADS)

Ebeid, El-Zeiny M.; Abdel-Kader, Mahmood H.; Issa, Raafat M.; El-Daly, Samy A.

1988-05-01

The emission, excitation and absorption spectra toghether with the fluorescence and photochemical quantum yields of some chalcone derivatives have been studied in organic solvents and micellar and microemulsion media. Both 4-[2-(2-pyridyl)ethenyl] ( I) and 4-[2-(4-pyridyl)ethenyl ( II) chalcones show large positive solvatochromic effects. The fluorescence quantum yields increase substantially as the medium viscosity increases with a subsequent decrease in the photochemical quatum yield. Compounds I and II undergo excited-state molecular aggregation in concentrated solutions giving excimer-like emission that coincides with emission from crystalline samples. The enthalpies of photoassociation have been estimated. The chalcone derivative I acts as an efficient quencher of the fluorescence of the laser dye 1,4-bis (β-pyridyl-2-vinyl)benzene via a long-range mechanism. The excited-state lifetimes of both I and II are short and at 20°C their τ values are less than 800 ps.

Luminescent carbon quantum dots with high quantum yield as a single white converter for white light emitting diodes

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

Feng, X. T.; Zhang, Y.; Liu, X. G., E-mail: liuxuguang@tyut.edu.cn

Carbon quantum dots (CQDs) with high quantum yield (51.4%) were synthesized by a one-step hydrothermal method using thiosalicylic acid and ethylenediamine as precursor. The CQDs have the average diameter of 2.3 nm and possess excitation-independent emission wavelength in the range from 320 to 440 nm excitation. Under an ultraviolet (UV) excitation, the CQDs aqueous solutions emit bright blue fluorescence directly and exhibit broad emission with a high spectral component ratio of 67.4% (blue to red intensity to total intensity). We applied the CQDs as a single white-light converter for white light emitting diodes (WLEDs) using a UV-LED chip as the excitation lightmore » source. The resulted WLED shows superior performance with corresponding color temperature of 5227 K and the color coordinates of (0.34, 0.38) belonging to the white gamut.« less

Probing structure and dynamics of DNA with 2-aminopurine: effects of local environment on fluorescence.

PubMed

Rachofsky, E L; Osman, R; Ross, J B

2001-01-30

2-Aminopurine (2AP) is an analogue of adenine that has been utilized widely as a fluorescence probe of protein-induced local conformational changes in DNA. Within a DNA strand, this fluorophore demonstrates characteristic decreases in quantum yield and emission decay lifetime that vary sensitively with base sequence, temperature, and helix conformation but that are accompanied by only small changes in emission wavelength. However, the molecular interactions that give rise to these spectroscopic changes have not been established. To develop a molecular model for interpreting the fluorescence measurements, we have investigated the effects of environmental polarity, hydrogen bonding, and the purine and pyrimidine bases of DNA on the emission energy, quantum yield, and intensity decay kinetics of 2AP in simple model systems. The effects of environmental polarity were examined in a series of solvents of varying dielectric constant, and hydrogen bonding was investigated in binary mixtures of water with 1,4-dioxane or N,N-dimethylformamide (DMF). The effects of the purine and pyrimidine bases were studied by titrating 2AP deoxyriboside (d2AP) with the nucleosides adenosine (rA), cytidine (rC), guanosine (rG), and deoxythymidine (dT), and the nucleoside triphosphates ATP and GTP in neutral aqueous solution. The nucleosides and NTPs each quench the fluorescence of d2AP by a combination of static (affecting only the quantum yield) and dynamic (affecting both the quantum yield and the lifetime, proportionately) mechanisms. The peak wavelength and shape of the emission spectrum are not altered by either of these effects. The static quenching is saturable and has half-maximal effect at approximately 20 mM nucleoside or NTP, consistent with an aromatic stacking interaction. The rate constant for dynamic quenching is near the diffusion limit for collisional interaction (k(q) approximately 2 x 10(9) M(-1) s(-1)). Neither of these effects varies significantly between the various nucleosides and NTPs studied. In contrast, hydrogen bonding with water was observed to have a negligible effect on the emission wavelength, fluorescence quantum yield, or lifetime of 2AP in either dioxane or DMF. In nonpolar solvents, the fluorescence lifetime and quantum yield decrease dramatically, accompanied by significant shifts in the emission spectrum to shorter wavelengths. However, these effects of polarity do not coincide with the observed emission wavelength-independent quenching of 2AP fluorescence in DNA. Therefore, we conclude that the fluorescence quenching of 2AP in DNA arises from base stacking and collisions with neighboring bases only but is insensitive to base-pairing or other hydrogen bonding interactions. These results implicate both structural and dynamic properties of DNA in quenching of 2AP and constitute a simple model within which the fluorescence changes induced by protein-DNA binding or other perturbations may be interpreted.

Phosphorescent binuclear iridium complexes based on terpyridine-carboxylate: an experimental and theoretical study.

PubMed

Andreiadis, Eugen S; Imbert, Daniel; Pécaut, Jacques; Calborean, Adrian; Ciofini, Ilaria; Adamo, Carlo; Demadrille, Renaud; Mazzanti, Marinella

2011-09-05

The phosphorescent binuclear iridium(III) complexes tetrakis(2-phenylpyridine)μ-(2,2':6',2''-terpyridine-6,6''-dicarboxylic acid)diiridium (Ir1) and tetrakis(2-(2,4-difluorophenyl) pyridine))μ-(2,2':6',2''-terpyridine-6,6''-dicarboxylic acid)diiridium (Ir2) were synthesized in a straightforward manner and characterized using X-ray diffraction, NMR, UV-vis absorption, and emission spectroscopy. The complexes have similar solution structures in which the two iridium centers are equivalent. This is further confirmed by the solid state structure of Ir2. The newly reported complexes display intense luminescence in dichloromethane solutions with maxima at 538 (Ir1) and 477 nm (Ir2) at 298 K (496 and 468 nm at 77 K, respectively) and emission quantum yields reaching ~18% for Ir1. The emission quantum yield for Ir1 is among the highest values reported for dinuclear iridium complexes. It shows only a 11% decrease with respect to the emission quantum yield reported for its mononuclear analogue, while the molar extinction coefficient is roughly doubled. This suggests that such architectures are of potential interest for the development of polymetallic assemblies showing improved optical properties. DFT and time-dependent-DFT calculations were performed on the ground and excited states of the complexes to provide insights into their structural, electronic, and photophysical properties.

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.

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.

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.

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.

Detection and evaluation of normal and malignant cells using laser-induced fluorescence spectroscopy.

PubMed

Khosroshahi, Mohamad E; Rahmani, Mahya

2012-01-01

The aim of this research is to study the normalized fluorescence spectra (intensity variations and area under the fluorescence signal), relative quantum yield, extinction coefficient and intracellular properties of normal and malignant human bone cells. Using Laser-Induced Fluorescence Spectroscopy (LIFS) upon excitation of 405 nm, the comparison of emission spectra of bone cells revealed that fluorescence intensity and the area under the spectra of malignant bone cells was less than that of normal. In addition, the area ratio and shape factor were changed. We obtained two emission bands in spectra of normal cells centered at about 486 and 575 nm and for malignant cells about 482 and 586 nm respectively, which are most likely attributed to NADH and riboflavins. Using fluorescein sodium emission spectrum, the relative quantum yield of bone cells is numerically determined.

Spectroscopic studies, fluorescence quenching by molecular oxygen and amplified spontaneous emission of 1,4-bis [2-(2-pyridyl) vinyl] benzene (P2VB) diolefinic laser dye

NASA Astrophysics Data System (ADS)

El-Daly, Samy A.; Ebeid, E. M.

2014-04-01

The UV-visible electronic absorption spectra, molar absorptivity, fluorescence spectra, fluorescence quantum yield and excited state lifetime of 1,4-bis [2-(2-pyridyl) vinyl] benzene P2VB were measured in different solvents. The fluorescence quenching of P2VB by molecular oxygen was also studied using lifetime measurements. A 2 × 10-4 mol dm-3 solution of P2VB in dimethyl formamide (DMF) gave amplified spontaneous emission (ASE) in blue spectral region with emission maximum at 420 nm upon pumping by 337.1 nitrogen laser pulse. The photochemical quantum yields (ϕc) of trans-cis photoisomerization of P2VB were calculated in different organic solvents. The photoreactivity of P2VB are also studied PMMA matrix.

An insight into non-emissive excited states in conjugated polymers

NASA Astrophysics Data System (ADS)

Hu, Zhongjian; Willard, Adam P.; Ono, Robert J.; Bielawski, Christopher W.; Rossky, Peter J.; vanden Bout, David A.

2015-09-01

Conjugated polymers in the solid state usually exhibit low fluorescence quantum yields, which limit their applications in many areas such as light-emitting diodes. Despite considerable research efforts, the underlying mechanism still remains controversial and elusive. Here, the nature and properties of excited states in the archetypal polythiophene are investigated via aggregates suspended in solvents with different dielectric constants (ε). In relatively polar solvents (ε>~ 3), the aggregates exhibit a low fluorescence quantum yield (QY) of 2-5%, similar to bulk films, however, in relatively nonpolar solvents (ε<~ 3) they demonstrate much higher fluorescence QY up to 20-30%. A series of mixed quantum-classical atomistic simulations illustrate that dielectric induced stabilization of nonradiative charge-transfer (CT) type states can lead to similar drastic reduction in fluorescence QY as seen experimentally. Fluorescence lifetime measurement reveals that the CT-type states exist as a competitive channel of the formation of emissive exciton-type states.

Use of the fluorescence quantum yield for the determination of the number-average molecular weight of polymers of epicatechin with 4β→8 interflavin bonds

Treesearch

D. Cho; W.L. Mattice; L.J. Porter; Richard W. Hemingway

1989-01-01

Excitation at 280 nm produces a structureless emission band with a maximum at 321-324 nm for dilute solutions of catechin, epicatechin, and their oligomers in l,4-dioxane or water. The fluorescence quantum yield, Q, has been measured in these two solvents for five dimers, a trimer, a tetramer, a pentamer, a hexamer, and a polymer in which the monomer...

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.

Synthesis, linear and nonlinear optical properties of phosphonato-substituted bithiophenes derived from 2,2'-biphenol.

PubMed

Freeman, Jason L; Zhao, Qun; Zhang, Yuanli; Wang, Jianwei; Lawson, Christopher M; Gray, Gary M

2013-10-21

Two new series of phosphonato-substituted bithiophenes, BpP(X)(C4H2S)2H and BpP(X)(C4H2S)2P(X)Bp (Bp = 2,2'-C12H8O2, X = O, S, Se), have been synthesized and characterized using linear absorption and emission spectra, and third-order nonlinear absorption measurements at 430 nm with 27 ps laser pulses. The compounds were synthesized in three steps: (1) reacting lithiated bithiophene with (Et2N)2PCl; (2) reacting the product from the first step with biphenol; and (3) reacting the product from the second step with the appropriate chalcogen. The X-ray crystal structures of two of the compounds, BpP(O)(C4H2S)2P(O)Bp and BpP(Se)(C4H2S)2P(Se)Bp, are reported and show a number of intermolecular π-π interactions. The linear absorption spectra, emission spectra, and emission quantum yields show distinct trends with respect to the chalcogen and the number of phosphorus substituents attached to the 2,2'-bithiophene ring. The compounds show emission maxima at wavelengths ranging from 380-400 nm and, BpP(S)(C4H2S)2H shows a 23-fold increase in fluorescence quantum yield relative to that of 2,2'-bithiophene. Fluorescence lifetimes and radiative and non-radiative decay rate constants for the first singlet excited state have been extracted from the quantum yields using time-dependent DFT calculations. Nonlinear transmission measurements indicate that all of the compounds show nonlinear absorption at 430 nm with 27 ps laser pulses in spite of their low solubilities. Notably, the nonlinear absorption threshold of a 0.16 mol L(-1) CH2Cl2 solution of BpP(Se)(C4H2S)2H is 0.9 J cm(-2). The excellent emission quantum yields and good nonlinear absorptions make these compounds promising candidates for optical power limiting applications and as host materials for violet-blue organic light emitting diodes.

In vitro energy transfer in Renilla bioluminescence

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

Ward, W.W.; Cormier, M.J.

1976-09-23

A quantitative study of in vitro energy transfer in a natural biological system is reported. The in vitro bioluminescent oxidation of Renilla (sea pansy) luciferin by luciferase produces a broad, structureless emission, peaking in the blue at 490 nm. In contrast, the live animal produces a structured emission peaking in the green at 509 nm. This difference in emission characteristics is due to the presence, in Renilla, of a green fluorescent protein (GFP). Addition of GFP in vitro sensitizes the oxyluciferin product excited state, resulting in the narrow, structured green emission characteristic of GFP fluorescence (lambda/sub max/ 509 nm). Undermore » conditions of efficient in vitro energy transfer (2.7 x 10/sup -6/ M GFP) the radiative quantum yield (with respect to luciferin) increases 5.7-fold from 5.3% (blue pathway) to 30% (green pathway). The fluorescence quantum yield of the Renilla GFP has been measured as 30%; thus, within the precision of our measurements (15% coefficient of variation) the in vitro energy transfer efficiency is a surprising 100%.« less

Responses of growth, photosynthesis and VOC emissions of Pinus tabulaeformis Carr. Exposure to elevated CO2 and/or elevated O3 in an urban area.

PubMed

Xu, Sheng; Chen, Wei; Huang, Yanqing; He, Xingyuan

2012-03-01

Responses of growth, photosynthesis and emission of volatile organic compounds of Pinus tabulaeformis exposed to elevated CO(2) (700 ppm) and O(3) (80 ppb) were studied in open top chambers. Elevated CO(2) increased growth, but it did not significantly (p > 0.05) affect net photosynthetic rate, stomatal conductance, chlorophyll content, the maximum quantum yield of photosystem II, or the effective quantum yield of photosystem II electron transport after 90 d of gas exposure. Elevated O(3) decreased growth (by 42.2% in needle weight and 25.8% in plant height), net photosynthetic rate and stomatal conductance after 90 d of exposure, but its negative effects were alleviated by elevated CO(2). Elevated O(3) significantly (p < 0.05) increased the emission rate of volatile organic compounds, which may be a helpful response to protect photosynthetic apparatus against O(3) damage.

Experimental assessment of fluorescence microscopy signal enhancement by stimulated emission

NASA Astrophysics Data System (ADS)

Dake, Fumihiro; Yazawa, Hiroki

2017-10-01

The quantity of photons generated during fluorescence microscopy is principally determined by the quantum yield of the fluorescence dyes and the optical power of the excitation beam. However, even though low quantum yields can produce poor images, it is challenging to tune this parameter, while increasing the power of the excitation beam often results in photodamage. Here, we propose the use of stimulated emission (SE) as a means of enhancing both the signal intensity and signal-to-noise ratio during confocal fluorescence microscopy. This work experimentally confirmed that both these factors can be enhanced by SE radiation, through generating a greater number of photons than are associated with the standard fluorescence signal. We also propose the concept of stimulated emission enhancing fluorescence (SEEF) microscopy, which employs both the SE and fluorescence signals, and demonstrate that the intensity of an SEEF signal is greater than those of the individual SE and fluorescence signals.

Convenient determination of luminescence quantum yield using a combined electronic absorption and emission spectrometer

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

Prakash, John; Mishra, Ashok Kumar

2016-01-15

It is possible to measure luminescence quantum yield in a facile way, by designing an optical spectrometer capable of obtaining electronic absorption as well as luminescence spectra, with a setup that uses the same light source and detector for both the spectral measurements. Employment of a single light source and single detector enables use of the same correction factor profile for spectral corrections. A suitable instrumental scaling factor is used for adjusting spectral losses.

Spectroscopic investigation of alloyed quantum dot-based FRET to cresyl violet dye.

PubMed

Kotresh, M G; Adarsh, K S; Shivkumar, M A; Mulimani, B G; Savadatti, M I; Inamdar, S R

2016-05-01

Quantum dots (QDs), bright luminescent semiconductor nanoparticles, have found numerous applications ranging from optoelectronics to bioimaging. Here, we present a systematic investigation of fluorescence resonance energy transfer (FRET) from hydrophilic ternary alloyed quantum dots (CdSeS/ZnS) to cresyl violet dye with a view to explore the effect of composition of QD donors on FRET efficiency. Fluorescence emission of QD is controlled by varying the composition of QD without altering the particle size. The results show that quantum yield of the QDs increases with increase in the emission wavelength. The FRET parameters such as spectral overlap J(λ), Förster distance R0, intermolecular distance (r), rate of energy transfer k(T)(r), and transfer efficiency (E) are determined by employing both steady-state and time-resolved fluorescence spectroscopy. Additionally, dynamic quenching is noticed to occur in the present FRET system. Stern-Volmer (K(D)) and bimolecular quenching constants (k(q)) are determined from the Stern-Volmer plot. It is observed that the transfer efficiency follows a linear dependence on the spectral overlap and the quantum yield of the donor as predicted by the Förster theory upon changing the composition of the QD. Copyright © 2015 John Wiley & Sons, Ltd.

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.

Photophysical properties of blue – emitting silicon nanoparticles

PubMed Central

Portolés, Manuel J. Llansola; Nieto, Felipe Rodriguez; Soria, Delia B.; Amalvy, Javier I.; Peruzzo, Pablo J.; Mártire, Daniel O.; Kotler, Mónica; Holub, Oliver; Gonzalez, Mónica C.

2012-01-01

Silicon nanoparticles with strong blue photoluminescence were synthesized by electrochemical etching of silicon wafers and ultrasonically removed under N2 atmosphere in organic solvents to produce colloids. Thermal treatment leads to the formation of colloidal Si particles of 3 ± 1 nm diameter, which upon excitation with 340 – 380 nm light exhibited room temperature luminescence in the range from 400 to 500 nm. The emission and the one- and two-photon excitation spectra of the particles are not sensitive to surface functionalization with methyl 2-methylprop-2-enoate. However, the derivatized particles show higher emission quantum yields in air-saturated suspensions (44%) than the underivatized particles (27%), as well as higher stability of its dispersions. FTIR and XPS spectra indicate a significant surface oxidation of the particles. The Si:O:C ratio at the surface of the derivatized particles estimated from XPS is Si3O6(C5O2Hy)1, with y = 7 - 8. Vibronic spacing is observed in both the emission and excitation spectra. The information obtained from one-photon excitation experiments (emission and excitation spectra, photoluminescence quantum yields, luminescence decay lifetimes and anisotropy correlation lifetimes), as well as from two-photon excitation fluorescence correlation spectroscopy (brightness and diffusion coefficients) and TEM indicate that the blue-emitting particles are monodisperse and ball-shaped. Particle size clearly determines the emission and excitation spectral region, as expected from quantum confinement, but the presence and extent of Si-O species on the silicon networks seem crucial for determining the spectrum features and intensity of emission. The nanoparticles could hold great potential as quantum dots for applications as luminescence sensors in biology and environmental science. PMID:22866180

Single photon emission from plasma treated 2D hexagonal boron nitride.

PubMed

Xu, Zai-Quan; Elbadawi, Christopher; Tran, Toan Trong; Kianinia, Mehran; Li, Xiuling; Liu, Daobin; Hoffman, Timothy B; Nguyen, Minh; Kim, Sejeong; Edgar, James H; Wu, Xiaojun; Song, Li; Ali, Sajid; Ford, Mike; Toth, Milos; Aharonovich, Igor

2018-05-03

Artificial atomic systems in solids are becoming increasingly important building blocks in quantum information processing and scalable quantum nanophotonic networks. Amongst numerous candidates, 2D hexagonal boron nitride has recently emerged as a promising platform hosting single photon emitters. Here, we report a number of robust plasma and thermal annealing methods for fabrication of emitters in tape-exfoliated hexagonal boron nitride (hBN) crystals. A two-step process comprising Ar plasma etching and subsequent annealing in Ar is highly robust, and yields an eight-fold increase in the concentration of emitters in hBN. The initial plasma-etching step generates emitters that suffer from blinking and bleaching, whereas the two-step process yields emitters that are photostable at room temperature with emission wavelengths greater than ∼700 nm. Density functional theory modeling suggests that the emitters might be associated with defect complexes that contain oxygen. This is further confirmed by generating the emitters via annealing hBN in air. Our findings advance the present understanding of the structure of quantum emitters in hBN and enhance the nanofabrication toolkit needed to realize integrated quantum nanophotonic circuits.

Aqueous synthesis of highly luminescent AgInS2-ZnS quantum dots and their biological applications

NASA Astrophysics Data System (ADS)

Regulacio, Michelle D.; Win, Khin Yin; Lo, Seong Loong; Zhang, Shuang-Yuan; Zhang, Xinhai; Wang, Shu; Han, Ming-Yong; Zheng, Yuangang

2013-02-01

Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated.Highly emissive and air-stable AgInS2-ZnS quantum dots (ZAIS QDs) with quantum yields of up to 20% have been successfully synthesized directly in aqueous media in the presence of polyacrylic acid (PAA) and mercaptoacetic acid (MAA) as stabilizing and reactivity-controlling agents. The as-prepared water-dispersible ZAIS QDs are around 3 nm in size, possess the tetragonal chalcopyrite crystal structure, and exhibit long fluorescence lifetimes (>100 ns). In addition, these ZAIS QDs are found to exhibit excellent optical and colloidal stability in physiologically relevant pH values as well as very low cytotoxicity, which render them particularly suitable for biological applications. Their potential use in biological labelling of baculoviral vectors is demonstrated. Electronic supplementary information (ESI) available: Quantum yields, EDX spectrum and photoluminescence decay curves. See DOI: 10.1039/c3nr34159c

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

Hawking radiation as tunneling in Schwarzschild anti-de Sitter black hole

NASA Astrophysics Data System (ADS)

Sefiedgar, A. S.; Ashrafinejad, A.

2017-08-01

The Hawking radiation from a (d+1) -dimensional Schwarzschild Anti-de Sitter (SAdS) black hole is investigated within rainbow gravity. Based on the method proposed by Kraus, Parikh and Wilczek, the Hawking radiation is considered as a tunneling process across the horizon. The emission rate of massless particles which are tunneling across the quantum-corrected horizon is calculated. Enforcing the energy conservation law leads to a dynamical geometry. Both the dynamical geometry and the quantum effects of space-time yield some corrections to the emission rate. The corrected radiation spectrum is not purely thermal. The emission rate is related to the changes of modified entropy in rainbow gravity and the corrected thermal spectrum may be consistent with an underlying unitary quantum theory. The correlations between emitted particles are also investigated in order to address the recovery of information.

Lanthanide complexes with 2-(tosylamino)benzylidene-N-benzoylhydrazone, which exhibit high NIR emission.

PubMed

Utochnikova, V V; Kovalenko, A D; Burlov, A S; Marciniak, L; Ananyev, I V; Kalyakina, A S; Kurchavov, N A; Kuzmina, N P

2015-07-28

New NIR emitting materials were found among the lanthanide complexes with 2-(tosylamino)benzylidene-N-benzoylhydrazone. Complexes of Nd(3+), Er(3+) and Yb(3+), as well as Eu(3+), Gd(3+) and Lu(3+), were synthesized for the first time. Owing to the absence of vibration quenching the ytterbium complex was found to exhibit a photoluminescence quantum yield of 1.4%. Since the sensitization efficiency was calculated to be 55%, the losses in the quantum yield are probably due to Yb-Yb resonant energy transfer.

Near-Unity Quantum Yields of Biexciton Emission from CdSe=CdS Nanocrystals Measured Using Single-Particle Spectroscopy

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

Park, Young-Shin; Malko, Anton V.; Vela, Javier

2011-05-03

Biexciton photoluminescence (PL) quantum yields (Q 2X) of individual CdSe/CdS core-shell nanocrystal quantum dots with various shell thicknesses are derived from independent PL saturation and two-photon correlation measurements. We observe a near-unity Q{sub 2X} for some nanocrystals with an ultrathick 19-monolayer shell. High Q 2X’s are, however, not universal and vary widely among nominally identical nanocrystals indicating a significant dependence of Q 2X upon subtle structural differences. Interestingly, our measurements indicate that high Q 2X’s are not required to achieve complete suppression of PL intensity fluctuations in individual nanocrystals.

Stable CdS QDs with intense broadband photoluminescence and high quantum yields

NASA Astrophysics Data System (ADS)

Mandal, Abhijit; Saha, Jony; De, Goutam

2011-11-01

Aqueous synthesis of CdS quantum dots (QDs) using thiolactic acid (TLA) as a capping agent was reported. These QDs exhibited excellent colloidal and photostability over a span of 2 years and showed intense broadband and almost white photoluminescence suitable for solid state lighting devices. The photoluminescence (PL) property of the aqueous CdS QDs is optimized by adjusting various processing parameters. The highest quantum yield (QY) achieved for TLA capped CdS QDs of average size 3.5 nm was ˜50%. Luminescence lifetime measurements of CdS-TLA QDs indicated longer lifetimes and a larger contribution of the surface-related emission, indicating removal of quenching defects.

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 .

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.

Efficient and Stable CsPb(Br/I)3@Anthracene Composites for White Light-Emitting Devices.

PubMed

Shen, Xinyu; Sun, Chun; Bai, Xue; Zhang, Xiaoyu; Wang, Yu; Wang, Yiding; Song, Hongwei; Yu, William W

2018-05-16

Inorganic perovskite quantum dots bear many unique properties that make them potential candidates for optoelectronic applications, including color display and lighting. However, the white emission with inorganic perovskite quantum dots has rarely been realized due to the anion-exchange reaction. Here, we proposed a one-pot preparation to fabricate inorganic perovskite quantum dot-based white light-emitting composites by introducing anthracene as a blue emission component. The as-prepared white light-emitting composite exhibited a photoluminescence quantum yield of 41.9%. By combining CsPb(Br/I) 3 @anthracene composites with UV light-emitting device (LED) chips, white light-emitting devices with a color rendering index of 90 were realized with tunable color temperature from warm white to cool white. These results can promote the application of inorganic perovskite quantum dots in the field of white LEDs.

Aggregation-induced emission in lamellar solids of colloidal perovskite quantum wells

PubMed Central

Jagielski, Jakub; Kumar, Sudhir; Wang, Mingchao; Scullion, Declan; Lawrence, Robert; Li, Yen-Ting; Yakunin, Sergii; Tian, Tian; Kovalenko, Maksym V.; Chiu, Yu-Cheng; Santos, Elton J. G.; Lin, Shangchao; Shih, Chih-Jen

2017-01-01

The outstanding excitonic properties, including photoluminescence quantum yield (ηPL), of individual, quantum-confined semiconductor nanoparticles are often significantly quenched upon aggregation, representing the main obstacle toward scalable photonic devices. We report aggregation-induced emission phenomena in lamellar solids containing layer-controlled colloidal quantum wells (QWs) of hybrid organic-inorganic lead bromide perovskites, resulting in anomalously high solid-state ηPL of up to 94%. Upon forming the QW solids, we observe an inverse correlation between exciton lifetime and ηPL, distinct from that in typical quantum dot solid systems. Our multiscale theoretical analysis reveals that, in a lamellar solid, the collective motion of the surface organic cations is more restricted to orient along the [100] direction, thereby inducing a more direct bandgap that facilitates radiative recombination. Using the QW solids, we demonstrate ultrapure green emission by completely downconverting a blue gallium nitride light-emitting diode at room temperature, with a luminous efficacy higher than 90 lumen W−1 at 5000 cd m−2, which has never been reached in any nanomaterial assemblies by far. PMID:29282451

Emitting color tunable carbon dots by adjusting solvent towards light-emitting devices

NASA Astrophysics Data System (ADS)

Zhu, Jinyang; Bai, Xue; Bai, Jialin; Pan, Gencai; Zhu, Yongsheng; Zhai, Yue; Shao, He; Chen, Xu; Dong, Biao; Zhang, Hanzhuang; Song, Hongwei

2018-02-01

Carbon dots (CDs), one of the most significant classes of carbon-based nanophosphors, have attracted extensive attention in recent years. However, few attempts have been reported for realizing CDs with tunable emissions, especially for obtaining the red-light emissions with high photoluminescence quantum yields. Herein, we synthesized CDs with different chromatic blue, green and red emissions by facilely changing the reaction solvent during hydrothermal conditions. The photoluminescence quantum yields of 34%, 19% and 47% for the blue, green and red emissions, respectively, were achieved. Furthermore, the solid-state CD/PVA composite films were constructed through mixing the CDs with PVA polymer, in which the self-quenching of photoluminescence of CDs had been successfully avoided benefiting from the formation of hydrogen bonds between the CDs and PVA molecules. Finally, the warm white light emitting diode (WLED) was fabricated by integrating CD/PVA film on a UV-LED chip. The WLED exhibited the Commission International de l’Eclairage coordinates (CIE) of (0.38, 0.34), correlated color temperature of 3913 K and color rendering index of 91, respectively, which were comparable with the commercial WLEDs.

Primary photophysical properties of moxifloxacin--a fluoroquinolone antibiotic.

PubMed

Lorenzo, Fernando; Navaratnam, Suppiah; Edge, Ruth; Allen, Norman S

2008-01-01

The photophysical properties of the fluoroquinolone antibiotic moxifloxacin (MOX) were investigated in aqueous media. MOX in water, at pH 7.4, shows two intense absorption bands at 287 and 338 nm (epsilon = 44,000 and 17,000 dm(3) mol(-1) cm(-1), respectively). The absorption and emission properties of MOX are pH-dependent, pK(a) values for the protonation equilibria of both the ground (6.1 and 9.6) and excited singlet states (6.8 and 9.1) of MOX were determined spectroscopically. MOX fluoresces weakly, the quantum yield for fluorescence emission being maximum (0.07) at pH 8. Phosphorescence from the excited triplet state in frozen ethanol solution has a quantum yield of 0.046. Laser flash photolysis and pulse radiolysis studies have been carried out to characterize the transient species of MOX in aqueous solution. On laser excitation, MOX undergoes monophotonic photoionization with a quantum yield of 0.14. This leads to the formation of a long-lived cation radical whose absorption is maximum at 470 nm (epsilon(470) = 3400 dm(3) mol(-1) cm(-1)). The photoionization process releases hydrated electron which rapidly reacts (k = 2.8 x 10(10) dm(3) mol(-1) s(-1)) with ground state MOX, yielding a long-lived anion radical with maximum absorption at 390 nm (epsilon(390) = 2400 dm(3) mol(-1) cm(-1)). The cation radical of MOX is able to oxidize protein components tryptophan and tyrosine. The bimolecular rate constants for these reactions are 2.3 x 10(8) dm(3) mol(-1) s(-1) and 1.3 x 10(8) dm(3) mol(-1) s(-1), respectively. Singlet oxygen sensitized by the MOX triplet state was also detected only in oxygen-saturated D(2)O solutions, with a quantum yield of 0.075.

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

Arene-Inserted Extended Germa[n]pericyclynes: Synthesis, Structure, and Phosphorescence Properties.

PubMed

Tanimoto, Hiroki; Mori, Junta; Ito, Shunichiro; Nishiyama, Yasuhiro; Morimoto, Tsumoru; Tanaka, Kazuo; Chujo, Yoshiki; Kakiuchi, Kiyomi

2017-07-26

This report describes the synthesis and characterization of arene-inserted extended (ArEx) germa[n]pericyclynes composed of germanium and 1,4-diethynylbenzene units. These novel cyclic germanium-π unit materials were synthesized with diethynylbenzene and germanium dichloride. X-ray crystallographic analysis revealed their structures, and the planar conformation of ArEx germa[4]pericyclyne along with the regular aromatic rings. UV/Vis absorption spectra and fluorescence emission spectra showed considerably unique and highly improved character compared to previously reported germa[n]pericyclynes. Even in the absence of transition metal components, phosphorescence emissions were observed, and the emission lifetimes were dramatically improved. ArEx germa[n]pericyclynes showed high photoluminescence quantum yields, whereas low photoluminescence quantum yields were observed for acyclic compounds. Density functional theory calculations show delocalized orbitals between skipped alkyne units through a germanium tether, and an increase in the HOMO energy level, leading to a small HOMO-LUMO energy gap. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Near-Unity Internal Quantum Efficiency of Luminescent Silicon Nanocrystals with Ligand Passivation.

PubMed

Sangghaleh, Fatemeh; Sychugov, Ilya; Yang, Zhenyu; Veinot, Jonathan G C; Linnros, Jan

2015-07-28

Spectrally resolved photoluminescence (PL) decays were measured for samples of colloidal, ligand-passivated silicon nanocrystals. These samples have PL emission energies with peak positions in the range ∼1.4-1.8 eV and quantum yields of ∼30-70%. Their ensemble PL decays are characterized by a stretched-exponential decay with a dispersion factor of ∼0.8, which changes to an almost monoexponential character at fixed detection energies. The dispersion factors and decay rates for various detection energies were extracted from spectrally resolved curves using a mathematical approach that excluded the effect of homogeneous line width broadening. Since nonradiative recombination would introduce a random lifetime variation, leading to a stretched-exponential decay for an ensemble, we conclude that the observed monoexponential decay in size-selected ensembles signifies negligible nonradiative transitions of a similar strength to the radiative one. This conjecture is further supported as extracted decay rates agree with radiative rates reported in the literature, suggesting 100% internal quantum efficiency over a broad range of emission wavelengths. The apparent differences in the quantum yields can then be explained by a varying fraction of "dark" or blinking nanocrystals.

Solvent-Controlled Synthesis of Highly Luminescent Carbon Dots with a Wide Color Gamut and Narrowed Emission Peak Widths.

PubMed

Ding, Hui; Wei, Ji-Shi; Zhang, Peng; Zhou, Zi-Yuan; Gao, Qing-Yu; Xiong, Huan-Ming

2018-05-01

Carbon dots (CDs) have tremendous potential applications in bioimaging, biomedicine, and optoelectronics. By far, it is still difficult to produce photoluminescence (PL) tunable CDs with high quantum yield (QY) across the entire visible spectrum and narrow the emission peak widths of CDs close to those of typical quantum dots. In this work, a series of CDs with tunable emission from 443 to 745 nm, quantum yield within 13-54%, and narrowed full width at half maximum (FWHM) from 108 to 55 nm, are obtained by only adjusting the reaction solvents in a one-pot solvothermal route. The distinct optical features of these CDs are based on their differences in the particle size, and the content of graphitic nitrogen and oxygen-containing functional groups, which can be modulated by controlling the dehydration and carbonization processes during solvothermal reactions. Blue, green, yellow, red, and even pure white light emitting films (Commission Internationale de L'Eclairage (CIE)= 0.33, 0.33, QY = 39%) are prepared by dispersing one or three kinds of CDs into polyvinyl alcohol with appropriate ratios. The near-infrared emissive CDs are excellent fluorescent probes for both in vitro and in vivo bioimaging because of their high QY in water, long-term stability, and low cytotoxicity. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Controls of the quantum yield and saturation light of isoprene emission in different-aged aspen leaves

PubMed Central

Niinemets, Ülo; Sun, Zhihong; Talts, Eero

2018-01-01

Leaf age alters the balance between the use of end-product of plastidic isoprenoid synthesis pathway, dimethylallyl diphosphate (DMADP), in prenyltransferase reactions leading to synthesis of pigments of photosynthetic machinery and in isoprene synthesis, but the implications of such changes on environmental responses of isoprene emission have not been studied. Because under light-limited conditions, isoprene emission rate is controlled by DMADP pool size (SDMADP), shifts in the share of different processes are expected to particularly strongly alter the light dependency of isoprene emission. We examined light responses of isoprene emission in young fully-expanded, mature and old non-senescent leaves of hybrid aspen (Populus tremula x P. tremuloides) and estimated in vivo SDMADP and isoprene synthase activity from postillumination isoprene release. Isoprene emission capacity was 1.5-fold larger in mature than in young and old leaves. The initial quantum yield of isoprene emission (αI) increased by 2.5-fold with increasing leaf age primarily as the result of increasing SDMADP. The saturating light intensity (QI90) decreased by 2.3-fold with increasing leaf age, and this mainly reflected limited light-dependent increase of SDMADP possibly due to feedback inhibition by DMADP. These major age-dependent changes in the shape of the light response need consideration in modeling canopy isoprene emission. PMID:26037962

Controls of the quantum yield and saturation light of isoprene emission in different-aged aspen leaves.

PubMed

Niinemets, Ülo; Sun, Zhihong; Talts, Eero

2015-12-01

Leaf age alters the balance between the use of end-product of plastidic isoprenoid synthesis pathway, dimethylallyl diphosphate (DMADP), in prenyltransferase reactions leading to synthesis of pigments of photosynthetic machinery and in isoprene synthesis, but the implications of such changes on environmental responses of isoprene emission have not been studied. Because under light-limited conditions, isoprene emission rate is controlled by DMADP pool size (SDMADP ), shifts in the share of different processes are expected to particularly strongly alter the light dependency of isoprene emission. We examined light responses of isoprene emission in young fully expanded, mature and old non-senescent leaves of hybrid aspen (Populus tremula x P. tremuloides) and estimated in vivo SDMADP and isoprene synthase activity from post-illumination isoprene release. Isoprene emission capacity was 1.5-fold larger in mature than in young and old leaves. The initial quantum yield of isoprene emission (αI ) increased by 2.5-fold with increasing leaf age primarily as the result of increasing SDMADP . The saturating light intensity (QI90 ) decreased by 2.3-fold with increasing leaf age, and this mainly reflected limited light-dependent increase of SDMADP possibly due to feedback inhibition by DMADP. These major age-dependent changes in the shape of the light response need consideration in modelling canopy isoprene emission. © 2015 John Wiley & Sons Ltd.

Quantum dots in imaging, drug delivery and sensor applications

PubMed Central

Matea, Cristian T; Mocan, Teodora; Tabaran, Flaviu; Pop, Teodora; Mosteanu, Ofelia; Puia, Cosmin; Iancu, Cornel; Mocan, Lucian

2017-01-01

Quantum dots (QDs), also known as nanoscale semiconductor crystals, are nanoparticles with unique optical and electronic properties such as bright and intensive fluorescence. Since most conventional organic label dyes do not offer the near-infrared (>650 nm) emission possibility, QDs, with their tunable optical properties, have gained a lot of interest. They possess characteristics such as good chemical and photo-stability, high quantum yield and size-tunable light emission. Different types of QDs can be excited with the same light wavelength, and their narrow emission bands can be detected simultaneously for multiple assays. There is an increasing interest in the development of nano-theranostics platforms for simultaneous sensing, imaging and therapy. QDs have great potential for such applications, with notable results already published in the fields of sensors, drug delivery and biomedical imaging. This review summarizes the latest developments available in literature regarding the use of QDs for medical applications. PMID:28814860

Quantum dots in imaging, drug delivery and sensor applications.

PubMed

Matea, Cristian T; Mocan, Teodora; Tabaran, Flaviu; Pop, Teodora; Mosteanu, Ofelia; Puia, Cosmin; Iancu, Cornel; Mocan, Lucian

2017-01-01

Quantum dots (QDs), also known as nanoscale semiconductor crystals, are nanoparticles with unique optical and electronic properties such as bright and intensive fluorescence. Since most conventional organic label dyes do not offer the near-infrared (>650 nm) emission possibility, QDs, with their tunable optical properties, have gained a lot of interest. They possess characteristics such as good chemical and photo-stability, high quantum yield and size-tunable light emission. Different types of QDs can be excited with the same light wavelength, and their narrow emission bands can be detected simultaneously for multiple assays. There is an increasing interest in the development of nano-theranostics platforms for simultaneous sensing, imaging and therapy. QDs have great potential for such applications, with notable results already published in the fields of sensors, drug delivery and biomedical imaging. This review summarizes the latest developments available in literature regarding the use of QDs for medical applications.

Homeotropic alignment and Förster resonance energy transfer: The way to a brighter luminescent solar concentrator

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

Tummeltshammer, Clemens; Taylor, Alaric; Kenyon, Anthony J.

2014-11-07

We investigate homeotropically aligned fluorophores and Förster resonance energy transfer (FRET) for luminescent solar concentrators using Monte-Carlo ray tracing. The homeotropic alignment strongly improves the trapping efficiency, while FRET circumvents the low absorption at homeotropic alignment by separating the absorption and emission processes. We predict that this design doped with two organic dye molecules can yield a 82.9% optical efficiency improvement compared to a single, arbitrarily oriented dye molecule. We also show that quantum dots are prime candidates for absorption/donor fluorophores due to their wide absorption band. The potentially strong re-absorption and low quantum yield of quantum dots is notmore » a hindrance for this design.« less

Combined atomic force microscopy and photoluminescence imaging to select single InAs/GaAs quantum dots for quantum photonic devices.

PubMed

Sapienza, Luca; Liu, Jin; Song, Jin Dong; Fält, Stefan; Wegscheider, Werner; Badolato, Antonio; Srinivasan, Kartik

2017-07-24

We report on a combined photoluminescence imaging and atomic force microscopy study of single, isolated self-assembled InAs quantum dots. The motivation of this work is to determine an approach that allows to assess single quantum dots as candidates for quantum nanophotonic devices. By combining optical and scanning probe characterization techniques, we find that single quantum dots often appear in the vicinity of comparatively large topographic features. Despite this, the quantum dots generally do not exhibit significant differences in their non-resonantly pumped emission spectra in comparison to quantum dots appearing in defect-free regions, and this behavior is observed across multiple wafers produced in different growth chambers. Such large surface features are nevertheless a detriment to applications in which single quantum dots are embedded within nanofabricated photonic devices: they are likely to cause large spectral shifts in the wavelength of cavity modes designed to resonantly enhance the quantum dot emission, thereby resulting in a nominally perfectly-fabricated single quantum dot device failing to behave in accordance with design. We anticipate that the approach of screening quantum dots not only based on their optical properties, but also their surrounding surface topographies, will be necessary to improve the yield of single quantum dot nanophotonic devices.

Surface defect assisted broad spectra emission from CdSe quantum dots for white LED application

NASA Astrophysics Data System (ADS)

Samuel, Boni; Mathew, S.; Anand, V. R.; Correya, Adrine Antony; Nampoori, V. P. N.; Mujeeb, A.

2018-02-01

This paper reports, broadband photoluminescence from CdSe quantum dots (QDs) under the excitation of 403 nm using fluorimeter and 403 nm CW laser excitation. The broad spectrum obtained from the colloidal quantum dots was ranges from 450 nm to 800 nm. The broadness of the spectra was attributed to the merging of band edge and defect driven emissions from the QDs. Six different sizes of particles were prepared via kinetic growth method by using CdO and elemental Se as sources of Cd and Se respectively. The particle sizes were measured from TEM images. The size dependent effect on broad emission was also studied and the defect state emission was found to be predominant in very small QDs. The defect driven emission was also observed to be redshifted, similar to the band edge emission, due to quantum confinement effect. The emission corresponding to different laser power was also studied and a linear relation was obtained. In order to study the colour characteristics of the emission, CIE chromaticity coordinate, CRI and CCT of the prepared samples were measured. It is observed that, these values were tunable by the addition of suitable intensity of blue light from the excitation source to yield white light of various colour temperatures. The broad photoluminescence spectrum of the QDs, were compared with that of a commercially available white LED. It was found that the prepared QDs are good alternatives for the phosphor in phosphor converted white LEDs, to provide good spectral tunability.

Quantum molecular dynamics and multistep-direct analyses of multiple preequilibrium emission

NASA Astrophysics Data System (ADS)

Chadwick, M. B.; Chiba, S.; Niita, K.; Maruyama, T.; Iwamoto, A.

1995-11-01

We study multiple preequilibrium emission in nucleon induced reactions at intermediate energies, and compare quantum molecular dynamics (QMD) calculations with multistep-direct Feshbach-Kerman-Koonin results [M. B. Chadwick, P. G. Young, D. C. George, and Y. Watanabe, Phys. Rev. C 50, 996 (1994)]. When the theoretical expressions of this reference are reformulated so that the definitions of primary and multiple emission correspond to those used in QMD, the two theories yield similar results for primary and multiple preequilibrium emission. We use QMD as a tool to determine the multiplicities of fast preequilibrium nucleons as a function of incident energy. For fast particle cross sections to exceed 5% of the inclusive preequilibrium emission cross sections we find that two particles should be included in reactions above 50 MeV, three above about 180 MeV, and four are only needed when the incident energy exceeds about 400 MeV.

Deterministic implementation of a bright, on-demand single photon source with near-unity indistinguishability via quantum dot imaging.

PubMed

He, Yu-Ming; Liu, Jin; Maier, Sebastian; Emmerling, Monika; Gerhardt, Stefan; Davanço, Marcelo; Srinivasan, Kartik; Schneider, Christian; Höfling, Sven

2017-07-20

Deterministic techniques enabling the implementation and engineering of bright and coherent solid-state quantum light sources are key for the reliable realization of a next generation of quantum devices. Such a technology, at best, should allow one to significantly scale up the number of implemented devices within a given processing time. In this work, we discuss a possible technology platform for such a scaling procedure, relying on the application of nanoscale quantum dot imaging to the pillar microcavity architecture, which promises to combine very high photon extraction efficiency and indistinguishability. We discuss the alignment technology in detail, and present the optical characterization of a selected device which features a strongly Purcell-enhanced emission output. This device, which yields an extraction efficiency of η = (49 ± 4) %, facilitates the emission of photons with (94 ± 2.7) % indistinguishability.

Low light CMOS contact imager with an integrated poly-acrylic emission filter for fluorescence detection.

PubMed

Dattner, Yonathan; Yadid-Pecht, Orly

2010-01-01

This study presents the fabrication of a low cost poly-acrylic acid (PAA) based emission filter integrated with a low light CMOS contact imager for fluorescence detection. The process involves the use of PAA as an adhesive for the emission filter. The poly-acrylic solution was chosen due its optical transparent properties, adhesive properties, miscibility with polar protic solvents and most importantly its bio-compatibility with a biological environment. The emission filter, also known as an absorption filter, involves dissolving an absorbing specimen in a polar protic solvent and mixing it with the PAA to uniformly bond the absorbing specimen and harden the filter. The PAA is optically transparent in solid form and therefore does not contribute to the absorbance of light in the visible spectrum. Many combinations of absorbing specimen and polar protic solvents can be derived, yielding different filter characteristics in different parts of the spectrum. We report a specific combination as a first example of implementation of our technology. The filter reported has excitation in the green spectrum and emission in the red spectrum, utilizing the increased quantum efficiency of the photo sensitive sensor array. The thickness of the filter (20 μm) was chosen by calculating the desired SNR using Beer-Lambert's law for liquids, Quantum Yield of the fluorophore and the Quantum Efficiency of the sensor array. The filters promising characteristics make it suitable for low light fluorescence detection. The filter was integrated with a fully functional low noise, low light CMOS contact imager and experimental results using fluorescence polystyrene micro-spheres are presented.

Femtosecond laser-induced size reduction and emission quantum yield enhancement of colloidal silicon nanocrystals: Effect of laser ablation time.

PubMed

Zhang, Yingxiong; Wu, Wenshun; Hao, Huilian; Shen, Wenzhong

2018-06-19

Colloidal silicon (Si) nanocrystals (NCs) with different sizes were successfully prepared by femtosecond laser ablation under different laser ablation time (LAT). The mean size decreases from 4.23 to 1.42 nm with increasing LAT from 30 to 120 min. In combination with structural characterization, temperature-dependent photoluminescence (PL), time-resolved PL, and PL excitation spectra, we attribute room temperature blue emissions peaked at 405 and 430 nm to the radiative recombination of electron-hole pairs via the oxygen deficient centers related to Si-C-H2 and Si-O-Si bonds of colloidal Si NCs prepared in 1-octene, respectively. In particular, the measured PL quantum yield of colloidal Si NCs has been enhanced significantly from 23.6% to 55.8% with prolonging LAT from 30 to 120 min. © 2018 IOP Publishing Ltd.

Rigid biimidazole ancillary ligands as an avenue to bright deep blue cationic iridium(iii) complexes.

PubMed

Henwood, Adam F; Evariste, Sloane; Slawin, Alexandra M Z; Zysman-Colman, Eli

2014-01-01

Herein we report the synthesis and optoelectronic characterisation of three deep blue-emitting cationic iridium complexes, of the form [Ir(dFppy)(2)(N^N)]PF(6), bearing biimidazole-type N^N ancillary ligands (dFppyH = 2-(2,4-difluorophenyl)pyridine). Complex 1 contains the parent biimidazole, biim, while 2 contains a dimethylated analog, dMebiim, and 3 contains an ortho-xylyl-tethered biimidzole, o-xylbiim. We explore a strategy of tethering the biimidazole in order to rigidify the complex and increase the photoluminescent quantum yield, culminating in deep blue (λ(max): 457 nm in MeOH at 298 K) ligand-centered emission with a very high photoluminescent quantum yield of 68% and microsecond emission lifetime. Density functional theory calculations elucidate the origin of such disparate excited state kinetics across this series, especially in light of virtually identical optoelectronic properties observed for these compounds.

Surface structures for enhancement of quantum yield in broad spectrum emission nanocrystals

DOEpatents

Schreuder, Michael A.; McBride, James R.; Rosenthal, Sandra J.

2014-07-22

Disclosed are inorganic nanoparticles comprising a body comprising cadmium and/or zinc crystallized with selenium, sulfur, and/or tellurium; a multiplicity of phosphonic acid ligands comprising at least about 20% of the total surface ligand coverage; wherein the nanocrystal is capable of absorbing energy from a first electromagnetic region and capable of emitting light in a second electromagnetic region, wherein the maximum absorbance wavelength of the first electromagnetic region is different from the maximum emission wavelength of the second electromagnetic region, thereby providing a Stokes shift of at least about 20 nm, wherein the second electromagnetic region comprises an at least about 100 nm wide band of wavelengths, and wherein the nanoparticle exhibits has a quantum yield of at least about 10%. This abstract is intended as a scanning tool for purposes of searching in the particular art and is not intended to be limiting of the present invention.

Photophysical parameters and fluorescence quenching of 7-diethylaminocoumarin (DEAC) laser dye

NASA Astrophysics Data System (ADS)

El-Mossalamy, E. H.; Obaid, A. Y.; El-Daly, S. A.

2011-10-01

The optical properties including electronic absorption spectrum, emission spectrum, fluorescence quantum yield, and dipole moment of electronic transition of 7-diethylaminocoumarin (DEAC) laser dye have been measured in different solvents. Both electronic absorption and fluorescence spectra are red shifted as the polarity of the medium increases, indicating that the dipole moment of molecule increases on excitation. The fluorescence quantum yield of DEAC decreases as the polarity of solvent increases, a result of the role of solvent polarity in stabilization of the twisting of the intramolecular charge transfer (TICT) in excited state, which is a non-emissive state, as well as hydrogen bonding with the hetero-atom of dye. The emission spectrum of DEAC has also been measured in cationic (CTAC) and anionic (SDS) micelles, the intensity increases as the concentration of surfactant increases, and an abrupt change in emission intensity is observed at critical micelle concentration (CMC) of surfactant. 2×10 -3 mol dm -3 of DEAC gives laser emission in the blue region on pumping with nitrogen laser ( λex=337.1 nm). The laser parameters such as tuning range, gain coefficient ( α), emission cross section ( σe), and half-life energy have been calculated in different solvents, namely acetone, dioxane , ethanol, and dimethyforamide (DMF). The photoreactivity of DEAC has been studied in CCl 4 at a wavelength of 366 nm. The values of photochemical yield ( ϕc) and rate constant ( k) are determined. The interaction of organic acceptors such as picric acid (PA), tetracyanoethylene (TCNE), and 7,7,8,8-tetracynoquinonedimethane (TCNQ) with DEAC is also studied using fluorescence measurements in acetonitrile (CH 3CN); from fluorescence quenching study we assume the possible electron transfer from excited donor DEAC to organic acceptor forming non-emissive exciplex.

Photochemical properties of squarylium cyanine dyes.

PubMed

Ferreira, D P; Conceição, D S; Ferreira, V R A; Graça, V C; Santos, P F; Vieira Ferreira, L F

2013-11-01

This study presents several new squarylium dyes derived from benzothiazole and benzoselenazole with several structural variations, namely the nature of the heteroaromatic ring and the length of the N,N'-dialkyl groups. Before being investigated in connection with their effect on living cells and/or tissues, these novel compounds were characterized, namely with respect to the determination of their main photophysical parameters. Therefore, a study of the ground state absorption, fluorescence emission (quantum yields and lifetimes) and singlet oxygen generation quantum yields was performed for all the compounds synthesized in order to evaluate their efficiency as photosensitizers. An increase of the alkyl chain length from ethyl to hexyl did not produce a clear change in the fluorescence quantum yields, showing no influence on the photoisomerization process. Heavy atom inclusion (Se instead of S) enhanced the singlet oxygen generation efficiency and decreased the intensity of the fluorescence emission. The external heavy atom effect (I(-) as a counterion instead of CF3SO3(-)) produced a significant increase in the singlet oxygen formation quantum yield (about 20%). Transient absorption studies in aerated and oxygen free samples revealed that the photoisomerization process, which could compete with the triplet state formation for all dyes in solution, is a negligible pathway for the excited state deactivation, in accordance with the rigidity introduced by the squaric ring into the polymethine chain of the dye, both in chloroform and ethanol. However, in the case of the chloroform solution a new transient was detected in air equilibrated solutions, resulting from a reaction of the excited squarylium dye in the singlet state with CHCl3˙, and assigned to the radical cation (SQ(+)˙) of the dye.

Blue and green electroluminescence from CdSe nanocrystal quantum-dot-quantum-wells

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

Lu, Y. F.; Cao, X. A., E-mail: xacao@mail.wvu.edu

2014-11-17

CdS/CdSe/ZnS quantum dot quantum well (QDQW) nanocrystals were synthesized using the successive ion layer adsorption and reaction technique, and their optical properties were tuned by bandgap and strain engineering. 3-monolayer (ML) CdSe QWs emitted blue photoluminescence at 467 nm with a spectral full-width-at-half-maximum of ∼30 nm. With a 3 ML ZnS cladding layer, which also acts as a passivating and strain-compensating layer, the QDQWs acquired a ∼35% quantum yield of the QW emission. Blue and green electroluminescence (EL) was obtained from QDQW light-emitting devices with 3–4.5 ML CdSe QWs. It was found that as the peak blueshifted, the overall EL was increasinglymore » dominated by defect state emission due to poor hole injection into the QDQWs. The weak EL was also attributed to strong field-induced charge separation resulting from the unique QDQW geometry, weakening the oscillator strength of optical transitions.« less

Photophysical parameters and laser performance of 3-(4‧-dimethylaminophenyl)-1-(2-furanyl)prop-2-en-1-one (DMAFP): A new laser dye

NASA Astrophysics Data System (ADS)

El-Daly, S. A.; Gaber, M.; El-Sayed, Y. S.

2009-09-01

The spectral properties such as singlet absorption, molar absorptivity, emission spectra, fluorescence quantum yield and excited state lifetime of 3-(4'-dimethylaminophenyl)-1-(2-furanyl)prop-2-en-1-one (DMAFP) have been determined in different solvents. DMAFP dye exhibits a large red shift in both electronic absorption and emission spectra as the solvent polarity increases, indicating a large change in the dipole moment of molecules upon excitation. A crystalline solid of DMAFP gives an excimer like emission at 566 nm due to the excitation of molecular aggregates. This is expected from the idealized crystal structure of the dye that belongs to the B-type class of Steven's classification. The ground and excited state protonation constants of DMAFP are calculated and amounted to 1.71 and 8.3, respectively. DMAFP acts as a good laser dye upon pumping with nitrogen laser ( λex=337.1 nm) in chloroform, methylene chloride and dioxane and gives laser emission in the range 460-590 nm. The laser parameters such as the tuning range, gain coefficient ( α), emission cross section ( σ e) and half-life energy ( E1/2) are calculated. The photoreactivity and net photochemical quantum yield of DMAFP in chloromethane solvents are also studied.

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

PubMed Central

Schröder, Tim; Trusheim, Matthew E.; Walsh, Michael; Li, Luozhou; Zheng, Jiabao; Schukraft, Marco; Sipahigil, Alp; Evans, Ruffin E.; Sukachev, Denis D.; Nguyen, Christian T.; Pacheco, Jose L.; Camacho, Ryan M.; Bielejec, Edward S.; Lukin, Mikhail D.; Englund, Dirk

2017-01-01

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ∼32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ∼2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ∼51 GHz and close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ∼1.4 times the natural linewidth. This method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors. PMID:28548097

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

DOE PAGES

Schroder, Tim; Trusheim, Matthew E.; Walsh, Michael; ...

2017-05-26

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ~32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ~2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ~51 GHz andmore » close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ~1.4 times the natural linewidth. Furthermore, this method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors.« less

Scalable focused ion beam creation of nearly lifetime-limited single quantum emitters in diamond nanostructures

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

Schroder, Tim; Trusheim, Matthew E.; Walsh, Michael

The controlled creation of defect centre—nanocavity systems is one of the outstanding challenges for efficiently interfacing spin quantum memories with photons for photon-based entanglement operations in a quantum network. Here we demonstrate direct, maskless creation of atom-like single silicon vacancy (SiV) centres in diamond nanostructures via focused ion beam implantation with ~32 nm lateral precision and <50 nm positioning accuracy relative to a nanocavity. We determine the Si+ ion to SiV centre conversion yield to be ~2.5% and observe a 10-fold conversion yield increase by additional electron irradiation. Low-temperature spectroscopy reveals inhomogeneously broadened ensemble emission linewidths of ~51 GHz andmore » close to lifetime-limited single-emitter transition linewidths down to 126±13 MHz corresponding to ~1.4 times the natural linewidth. Furthermore, this method for the targeted generation of nearly transform-limited quantum emitters should facilitate the development of scalable solid-state quantum information processors.« less

Photodissociation of pernitric acid (HO2NO2) at 248 nm

NASA Technical Reports Server (NTRS)

Macleod, Helene; Smith, Gregory P.; Golden, David M.

1989-01-01

The photodissociation of pernitric acid (PNA) was studied at 248 nm. The quantum yield for production of OH radicals is 34 + or - 16 percent. The yield of OH from PNA was measured relative to that of H2O2. The translational and rotational energy content of the OH photofragment from PNA was characterized. A fluorescent emission was also observed and characterized. It is attributed to electronically excited NO2 produced in the PNA photodissociation. A maximum yield of 30 percent for NO2 production was determined. The intensity of this emission, and a mass spectrometric peak at m/e = 33, were found to be useful means of characterizing the purity of the PNA sample.

Fluorinated Alq3 derivatives with tunable optical properties.

PubMed

Shi, Yue-Wen; Shi, Min-Min; Huang, Jia-Chi; Chen, Hong-Zheng; Wang, Mang; Liu, Xiao-Dong; Ma, Yu-Guang; Xu, Hai; Yang, Bing

2006-05-14

This communication reports that not only the emission colour but also the photoluminescence quantum yield of Alq3 can be tuned by introducing fluorine atoms at different positions; with fluorination at C-5 the emission is red-shifted with a tremendously decreased intensity, fluorination at C-6 causes a blue-shift with a significantly increased intensity, and fluorination at C-7 has a minor effect on both the colour and intensity of Alq3's emission.

Extremely low amplified spontaneous emission threshold and blue electroluminescence from a spin-coated octafluorene neat film

NASA Astrophysics Data System (ADS)

Kim, D.-H.; Sandanayaka, A. S. D.; Zhao, L.; Pitrat, D.; Mulatier, J. C.; Matsushima, T.; Andraud, C.; Ribierre, J. C.; Adachi, C.

2017-01-01

We report on the photophysical, amplified spontaneous emission (ASE), and electroluminescence properties of a blue-emitting octafluorene derivative in spin-coated films. The neat film shows an extremely low ASE threshold of 90 nJ/cm2, which is related to its high photoluminescence quantum yield of 87% and its large radiative decay rate of 1.7 × 109 s-1. Low-threshold organic distributed feedback semiconductor lasers and fluorescent organic light-emitting diodes with a maximum external quantum efficiency as high as 4.4% are then demonstrated, providing evidence that this octafluorene derivative is a promising candidate for organic laser applications.

Long-lived and Well-resolved Mn2+ Ion Emissions in CuInS-ZnS Quantum Dots

PubMed Central

Cao, Sheng; Li, Chengming; Wang, Lin; Shang, Minghui; Wei, Guodong; Zheng, Jinju; Yang, Weiyou

2014-01-01

CuInS2 (CIS) quantum dots (QDs) have tunable photoluminescence (PL) behaviors in the visible and near infrared spectral range with markedly lower toxicity than the cadmium-based counterparts, making them very promising applications in light emitting and solar harvesting. However, there still remain material- and fabrication- related obstacles in realizing the high-performance CIS-based QDs with well-resolved Mn2+ d-d emission, long emission lifetimes as well as high efficiencies. Here, we demonstrate the growth of high-quality Mn2+-doped CuInS-ZnS (CIS-ZnS) QDs based on a multi-step hot-injection strategy. The resultant QDs exhibit a well-resolved Mn2+ d-d emission with a high PL quantum yield (QY) up to 66% and an extremely long excited state lifetime up to ~3.78 ms, which is nearly two times longer than the longest one of “green” QDs ever reported. It is promising that the synthesized Mn2+-doped CIS-ZnS QDs might open new doors for their practical applications in bioimaging and opto/electronic devices. PMID:25515207

Laboratory study of nitrate photolysis in Antarctic snow. I. Observed quantum yield, domain of photolysis, and secondary chemistry

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

Meusinger, Carl; Johnson, Matthew S.; Berhanu, Tesfaye A.

2014-06-28

Post-depositional processes alter nitrate concentration and nitrate isotopic composition in the top layers of snow at sites with low snow accumulation rates, such as Dome C, Antarctica. Available nitrate ice core records can provide input for studying past atmospheres and climate if such processes are understood. It has been shown that photolysis of nitrate in the snowpack plays a major role in nitrate loss and that the photolysis products have a significant influence on the local troposphere as well as on other species in the snow. Reported quantum yields for the main reaction spans orders of magnitude – apparently amore » result of whether nitrate is located at the air-ice interface or in the ice matrix – constituting the largest uncertainty in models of snowpack NO{sub x} emissions. Here, a laboratory study is presented that uses snow from Dome C and minimizes effects of desorption and recombination by flushing the snow during irradiation with UV light. A selection of UV filters allowed examination of the effects of the 200 and 305 nm absorption bands of nitrate. Nitrate concentration and photon flux were measured in the snow. The quantum yield for loss of nitrate was observed to decrease from 0.44 to 0.003 within what corresponds to days of UV exposure in Antarctica. The superposition of photolysis in two photochemical domains of nitrate in snow is proposed: one of photolabile nitrate, and one of buried nitrate. The difference lies in the ability of reaction products to escape the snow crystal, versus undergoing secondary (recombination) chemistry. Modeled NO{sub x} emissions may increase significantly above measured values due to the observed quantum yield in this study. The apparent quantum yield in the 200 nm band was found to be ∼1%, much lower than reported for aqueous chemistry. A companion paper presents an analysis of the change in isotopic composition of snowpack nitrate based on the same samples as in this study.« less

Next-generation in vivo optical imaging with short-wave infrared quantum dots.

PubMed

Bruns, Oliver T; Bischof, Thomas S; Harris, Daniel K; Franke, Daniel; Shi, Yanxiang; Riedemann, Lars; Bartelt, Alexander; Jaworski, Frank B; Carr, Jessica A; Rowlands, Christopher J; Wilson, Mark W B; Chen, Ou; Wei, He; Hwang, Gyu Weon; Montana, Daniel M; Coropceanu, Igor; Achorn, Odin B; Kloepper, Jonas; Heeren, Joerg; So, Peter T C; Fukumura, Dai; Jensen, Klavs F; Jain, Rakesh K; Bawendi, Moungi G

2017-01-01

For in vivo imaging, the short-wavelength infrared region (SWIR; 1000-2000 nm) provides several advantages over the visible and near-infrared regions: general lack of autofluorescence, low light absorption by blood and tissue, and reduced scattering. However, the lack of versatile and functional SWIR emitters has prevented the general adoption of SWIR imaging by the biomedical research community. Here, we introduce a class of high-quality SWIR-emissive indium-arsenide-based quantum dots (QDs) that are readily modifiable for various functional imaging applications, and that exhibit narrow and size-tunable emission and a dramatically higher emission quantum yield than previously described SWIR probes. To demonstrate the unprecedented combination of deep penetration, high spatial resolution, multicolor imaging and fast-acquisition-speed afforded by the SWIR QDs, we quantified, in mice, the metabolic turnover rates of lipoproteins in several organs simultaneously and in real time as well as heartbeat and breathing rates in awake and unrestrained animals, and generated detailed three-dimensional quantitative flow maps of the mouse brain vasculature.

Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs.

PubMed

Yuan, Fanglong; Yuan, Ting; Sui, Laizhi; Wang, Zhibin; Xi, Zifan; Li, Yunchao; Li, Xiaohong; Fan, Louzhen; Tan, Zhan'ao; Chen, Anmin; Jin, Mingxing; Yang, Shihe

2018-06-08

Carbon quantum dots (CQDs) have emerged as promising materials for optoelectronic applications on account of carbon's intrinsic merits of high stability, low cost, and environment-friendliness. However, the CQDs usually give broad emission with full width at half maximum exceeding 80 nm, which fundamentally limit their display applications. Here we demonstrate multicolored narrow bandwidth emission (full width at half maximum of 30 nm) from triangular CQDs with a quantum yield up to 54-72%. Detailed structural and optical characterizations together with theoretical calculations reveal that the molecular purity and crystalline perfection of the triangular CQDs are key to the high color-purity. Moreover, multicolored light-emitting diodes based on these CQDs display good stability, high color-purity, and high-performance with maximum luminance of 1882-4762 cd m -2 and current efficiency of 1.22-5.11 cd A -1 . This work will set the stage for developing next-generation high-performance CQDs-based light-emitting diodes.

Effect of antimony incorporation on the density, shape, and luminescence of InAs quantum dots

NASA Astrophysics Data System (ADS)

Chen, J. F.; Chiang, C. H.; Wu, Y. H.; Chang, L.; Chi, J. Y.

2008-07-01

This work investigates the surfactant effect on exposed and buried InAs quantum dots (QDs) by incorporating Sb into the QD layers with various Sb beam equivalent pressures (BEPs). Secondary ion mass spectroscopy shows the presence of Sb in the exposed and buried QD layers with the Sb intensity in the exposed layer substantially exceeding that in the buried layer. Incorporating Sb can reduce the density of the exposed QDs by more than two orders of magnitude. However, a high Sb BEP yields a surface morphology with a regular periodic structure of ellipsoid terraces. A good room-temperature photoluminescence (PL) at ˜1600 nm from the exposed QDs is observed, suggesting that the Sb incorporation probably improves the emission efficiency by reducing the surface recombination velocity at the surface of the exposed QDs. Increasing Sb BEP causes a blueshift of the emission from the exposed QDs due to a reduction in the dot height as suggested by atomic force microscopy. Increasing Sb BEP can also blueshift the ˜1300 nm emission from the buried QDs by decreasing the dot height. However, a high Sb BEP yields a quantum well-like PL feature formed by the clustering of the buried QDs into an undulated planar layer. These results indicate a marked Sb surfactant effect that can be used to control the density, shape, and luminescence of the exposed and buried QDs.

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

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

Dimitrov, D. A.; Bell, G. I.; Smedley, J.

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Modeling quantum yield, emittance, and surface roughness effects from metallic photocathodes

DOE PAGES

Dimitrov, D. A.; Bell, G. I.; Smedley, J.; ...

2017-10-26

Here, detailed measurements of momentum distributions of emitted electrons have allowed the investigation of the thermal limit of the transverse emittance from metal photocathodes. Furthermore, recent developments in material design and growth have resulted in photocathodes that can deliver high quantum efficiency and are sufficiently robust to use in high electric field gradient photoinjectors and free electron lasers. The growth process usually produces photoemissive material layers with rough surface profiles that lead to transverse accelerating fields and possible work function variations, resulting in emittance growth. To better understand the effects of temperature, density of states, and surface roughness on themore » properties of emitted electrons, we have developed realistic three-dimensional models for photocathode materials with grated surface structures. They include general modeling of electron excitation due to photon absorption, charge transport, and emission from flat and rough metallic surfaces. The models also include image charge and field enhancement effects. We report results from simulations with flat and rough surfaces to investigate how electron scattering, controlled roughness, work function variation, and field enhancement affect emission properties. Comparison of simulation results with measurements of the quantum yield and transverse emittance from flat Sb emission surfaces shows the importance of including efficient modeling of photon absorption, temperature effects, and the material density of states to achieve agreement with the experimental data.« less

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications.

PubMed

Ellis, Matthew A; Grandinetti, Giovanna; Fichter, Katye M; Fichter, Kathryn M

2016-02-06

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd(2+) ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications.

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications

PubMed Central

Ellis, Matthew A.; Grandinetti, Giovanna; Fichter, Katye M.

2016-01-01

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd2+ ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications. PMID:26891282

Defect induced photoluminescence in MoS2 quantum dots and effect of Eu3+/Tb3+ co-doping towards efficient white light emission

NASA Astrophysics Data System (ADS)

Haldar, Dhrubaa; Ghosh, Arnab; Bose, Saptasree; Mondal, Supriya; Ghorai, Uttam Kumar; Saha, Shyamal K.

2018-05-01

Intensive research has been carried out on optical properties of MoS2 quantum dots for versatile applications in photo catalytic, sensing and optoelectronic devices. However, white light generation from MoS2 quantum dots particularly using doping effect is relatively unexplored. Herein we report successful synthesis of Europium (Eu)/Terbium (Tb) co-doped MoS2 quantum dots to achieve white light for potential applications in optoelectronic devices. The dopant ions are introduced into the host lattice to retain the emission colors to cover the entire range of visible light of solar spectrum. Perfect white light (CIE = 0.31, 0.33) with high intensity (quantum yield = 28.29%) is achieved in these rare earth elements co-doped quantum dot system. A new peak is observed in the NIR region which is attributed to the defects present in MoS2 quantum dots. Temperature dependent study has been carried out to understand the origin of this new peak in the NIR region. It is seen that the 'S' defects in the QDs cause the appearance of this peak which shows a blue shift at higher temperature.

Bifunctional Diaminoterephthalate Fluorescent Dye as Probe for Cross-Linking Proteins.

PubMed

Wallisch, Melanie; Sulmann, Stefan; Koch, Karl-Wilhelm; Christoffers, Jens

2017-05-11

Diaminoterephthalates are fluorescent dyes and define scaffolds, which can be orthogonally functionalized at their two carboxylate residues with functional residues bearing task specific reactive groups. The synthesis of monofunctionalized dyes with thiol groups for surface binding, an azide for click chemistry, and a biotinoylated congener for streptavidin binding is reported. Two bifunctionalized dyes were prepared: One with an azide for click chemistry and a biotin for streptavidin binding, the other with a maleimide for reaction with thiol and a cyclooctyne moiety for ligation with copper-free click chemistry. In general, the compounds are red to orange, fluorescent materials with an absorption at about 450 nm and an emission at 560 nm with quantum yields between 2-41 %. Of particular interest is the maleimide-functionalized compound, which shows low fluorescence quantum yield (2 %) by itself. After addition of a thiol, the fluorescence is "turned on"; quantum yield 41 %. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

PubMed Central

Antaris, Alexander L.; Chen, Hao; Diao, Shuo; Ma, Zhuoran; Zhang, Zhe; Zhu, Shoujun; Wang, Joy; Lozano, Alexander X.; Fan, Quli; Chew, Leila; Zhu, Mark; Cheng, Kai; Hong, Xuechuan; Dai, Hongjie; Cheng, Zhen

2017-01-01

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with >1,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. Here, we report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for the fastest video-rate imaging in the second NIR window with ∼50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. In addition, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body. PMID:28524850

Synthesis and spectroscopic properties of some new difluoroboron bis-β-diketonate derivatives.

PubMed

Pi, Yan; Wang, Dun-Jia; Liu, Hua; Hu, Yan-Jun; Wei, Xian-Hong; Zheng, Jing

2014-10-15

Six new bis-β-diketones (RCOCH2CO-C7H7N-COCH2COR) were synthesized from 3,5-diacetyl-2,6-dimethylpyridine via Claisen condensation with the corresponding esters, and then reacted with boron trifluoride etherate to afford difluoroboron bis-β-diketonate derivatives. Their spectroscopic properties were investigated by UV-vis, FTIR, (1)H NMR and fluorescence spectroscopic techniques. It was found that these boron complexes exhibited violet or blue fluorescence emission at 422-445nm and possessed high extinction coefficients. The results indicate that the extending π-conjugation can increase the fluorescence intensity and quantum yield for these boron complexes. Especially, the compound 2b displayed the stronger fluorescence intensity and the highest fluorescence quantum yield (Φu=0.94) in these boron compounds. However, compounds 2c and 2d had the lower fluorescence intensity and quantum yield as a result of the heavy atom effect of the chlorine atom in the molecules. Copyright © 2014 Elsevier B.V. All rights reserved.

Synthesis and spectroscopic properties of some new difluoroboron bis-β-diketonate derivatives

NASA Astrophysics Data System (ADS)

Pi, Yan; Wang, Dun-Jia; Liu, Hua; Hu, Yan-Jun; Wei, Xian-Hong; Zheng, Jing

2014-10-01

Six new bis-β-diketones (RCOCH2CO-C7H7N-COCH2COR) were synthesized from 3,5-diacetyl-2,6-dimethylpyridine via Claisen condensation with the corresponding esters, and then reacted with boron trifluoride etherate to afford difluoroboron bis-β-diketonate derivatives. Their spectroscopic properties were investigated by UV-vis, FTIR, 1H NMR and fluorescence spectroscopic techniques. It was found that these boron complexes exhibited violet or blue fluorescence emission at 422-445 nm and possessed high extinction coefficients. The results indicate that the extending π-conjugation can increase the fluorescence intensity and quantum yield for these boron complexes. Especially, the compound 2b displayed the stronger fluorescence intensity and the highest fluorescence quantum yield (Φu = 0.94) in these boron compounds. However, compounds 2c and 2d had the lower fluorescence intensity and quantum yield as a result of the heavy atom effect of the chlorine atom in the molecules.

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

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

Antaris, Alexander L.; Chen, Hao; Diao, Shuo

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with 41,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. We report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for themore » fastest video-rate imaging in the second NIR window with B50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. Additionally, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body.« less

A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging

DOE PAGES

Antaris, Alexander L.; Chen, Hao; Diao, Shuo; ...

2017-05-19

Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with 41,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. We report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for themore » fastest video-rate imaging in the second NIR window with B50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. Additionally, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body.« less

[Optical and spectral parameters in Ce3+ -doped gadolinium gallium aluminum garnet glass-ceramics].

PubMed

Gong, Hua; Zhao, Xin; Yu, Xiao-bo; Setsuhisa, Tanabe; Lin, Hai

2010-01-01

The crystalline phases of Ce3+ -doped gadolinium gallium aluminum garnet (GGAG) glass-ceramics were investigated by X-ray diffraction, and the fluorescence spectra were recorded under the pumping of blue light-emitting diode (LED) using an integrating sphere of 10-inch in diameter, which connected to a CCD detector. The spectral power distribution of the glass-ceramics was obtained from the measured spectra first, and then the quantum yield was derived based on the photon distribution. The quantum yield of Ce3+ emission in GGAG glass-ceramics is 29.2%, meanwhile, the color coordinates and the correlated color temperature (CCT) of combined white light were proved to be x = 0.319, y = 0.349 and 6086 K, respectively. Although the quantum yield is a little smaller than the value in Ce3+ -doped YAG glass-ceramics, the CCT of the combined white light is much smaller than that in the latter. The optical behavior of GGAG glass-ceramics provides new vision for developing comfortable LED lighting devices.

Analogues of uracil nucleosides with intrinsic fluorescence (NIF-analogues): synthesis and photophysical properties.

PubMed

Segal, Meirav; Fischer, Bilha

2012-02-28

Uridine cannot be utilized as fluorescent probe due to its extremely low quantum yield. For improving the uracil fluorescence characteristics we extended the natural chromophore at the C5 position by coupling substituted aromatic rings directly or via an alkenyl or alkynyl linker to create fluorophores. Extension of the uracil base was achieved by treating 5-I-uridine with the appropriate boronic acid under the Suzuki coupling conditions. Analogues containing an alkynyl linker were obtained from 5-I-uridine and the suitable boronic acid in a Sonogashira coupling reaction. The uracil fluorescent analogues proposed here were designed to satisfy the following requirements: a minimal chemical modification at a position not involved in base-pairing, resulting in relatively long absorption and emission wavelengths and high quantum yield. 5-((4-Methoxy-phenyl)-trans-vinyl)-2'-deoxy-uridine, 6b, was found to be a promising fluorescent probe. Probe 6b exhibits a quantum yield that is 3000-fold larger than that of the natural chromophore (Φ 0.12), maximum emission (478 nm) which is 170 nm red shifted as compared to uridine, and a Stokes shift of 143 nm. In addition, since probe 6b adopts the anti conformation and S sugar puckering favored by B-DNA, it makes a promising nucleoside analogue to be incorporated in an oligonucleotide probe for detection of genetic material.

Facile synthesis of fluorescent polymer nanoparticles by covalent modification-nanoprecipitation of amine-reactive ester polymers.

PubMed

Lee, Yeonju; Hanif, Sadaf; Theato, Patrick; Zentel, Rudolf; Lim, Jeewoo; Char, Kookheon

2015-06-01

Emission wavelength control in fluorescent nanoparticles (NPs) is crucial for their applications. In the case of inorganic quantum dots or dye-impregnated silica NPs, such a control is readily achieved by changing the size of the particles or choosing appropriate fluorescent dyes, respectively. A similar modular approach for controlling the emission wavelength of fluo-rescent polymer NPs, however, is difficult. This article reports on fluorescent polymer NPs, the synthesis of which provides a platform for a modular approach towards the preparation of fluorescent NPs of desired emission wavelength. Atom-transfer radical polymerization (ATRP) is employed to synthesize reactive ester polymers, which are then easily modified with a commercially available dye and subsequently subjected to nanoprecipitation. The resulting NPs, with low size polydispersity, show an enhanced emission quantum yield when compared with the same dye molecules in solution. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photon-enhanced thermionic emission for solar concentrator systems.

PubMed

Schwede, Jared W; Bargatin, Igor; Riley, Daniel C; Hardin, Brian E; Rosenthal, Samuel J; Sun, Yun; Schmitt, Felix; Pianetta, Piero; Howe, Roger T; Shen, Zhi-Xun; Melosh, Nicholas A

2010-09-01

Solar-energy conversion usually takes one of two forms: the 'quantum' approach, which uses the large per-photon energy of solar radiation to excite electrons, as in photovoltaic cells, or the 'thermal' approach, which uses concentrated sunlight as a thermal-energy source to indirectly produce electricity using a heat engine. Here we present a new concept for solar electricity generation, photon-enhanced thermionic emission, which combines quantum and thermal mechanisms into a single physical process. The device is based on thermionic emission of photoexcited electrons from a semiconductor cathode at high temperature. Temperature-dependent photoemission-yield measurements from GaN show strong evidence for photon-enhanced thermionic emission, and calculated efficiencies for idealized devices can exceed the theoretical limits of single-junction photovoltaic cells. The proposed solar converter would operate at temperatures exceeding 200 degrees C, enabling its waste heat to be used to power a secondary thermal engine, boosting theoretical combined conversion efficiencies above 50%.

Emission efficiency limit of Si nanocrystals

PubMed Central

Limpens, Rens; Luxembourg, Stefan L.; Weeber, Arthur W.; Gregorkiewicz, Tom

2016-01-01

One of the important obstacles on the way to application of Si nanocrystals for development of practical devices is their typically low emissivity. In this study we explore the limits of external quantum yield of photoluminescence of solid-state dispersions of Si nanocrystals in SiO2. By making use of a low-temperature hydrogen passivation treatment we demonstrate a maximum emission quantum efficiency of approximately 35%. This is the highest value ever reported for this type of material. By cross-correlating PL lifetime with EQE values, we obtain a comprehensive understanding of the efficiency limiting processes induced by Pb-defects. We establish that the observed record efficiency corresponds to an interface density of Pb-centers of 1.3 × 1012 cm12, which is 2 orders of magnitude higher than for the best Si/SiO2 interface. This result implies that Si nanocrystals with up to 100% emission efficiency are feasible. PMID:26786062

Gamma emission of the atmosphere in the vicinity of the Earth. [28 keV to 4. 1 MeV

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

Golenetskii, S.V.; Gur'yan, Yu.A.; Il'inskii, V.N.

1975-01-01

The X-ray and ..gamma..-emissions of the earth's atmosphere were measured on Kosmos 461 in the range of 28 keV to 4.1 MeV. The energy spectrum of the emission was measured and the geomagnetic dependence of intensity in the continuous spectrum and in the 0.511-MeV line was determined. Measurements on Kosmos 135 yielded data on the height dependence of the atmospheric ..gamma..-quantum flux. 10 references.

Semiconductor Seeded Nanorods with Graded Composition Exhibiting High Quantum-Yield, High Polarization, and Minimal Blinking.

PubMed

Hadar, Ido; Philbin, John P; Panfil, Yossef E; Neyshtadt, Shany; Lieberman, Itai; Eshet, Hagai; Lazar, Sorin; Rabani, Eran; Banin, Uri

2017-04-12

Seeded semiconductor nanorods represent a unique family of quantum confined materials that manifest characteristics of mixed dimensionality. They show polarized emission with high quantum yield and fluorescence switching under an electric field, features that are desirable for use in display technologies and other optical applications. So far, their robust synthesis has been limited mainly to CdSe/CdS heterostructures, thereby constraining the spectral tunability to the red region of the visible spectrum. Herein we present a novel synthesis of CdSe/Cd 1-x Zn x S seeded nanorods with a radially graded composition that show bright and highly polarized green emission with minimal intermittency, as confirmed by ensemble and single nanorods optical measurements. Atomistic pseudopotential simulations elucidate the importance of the Zn atoms within the nanorod structure, in particular the effect of the graded composition. Thus, the controlled addition of Zn influences and improves the nanorods' optoelectronic performance by providing an additional handle to manipulate the degree confinement beyond the common size control approach. These nanorods may be utilized in applications that require the generation of a full, rich spectrum such as energy-efficient displays and lighting.

Why is gas phase 2-nitrophenol photolysis a potentially important source of OH radicals in the polluted atmosphere?

NASA Astrophysics Data System (ADS)

Zhu, L.

2017-12-01

2-Nitrophenol is an important component of "brown carbon" in the atmosphere. The concentration of 2-nitrophenol is higher in polluted urban areas where there are increased emissions of aromatic hydrocarbons. To assess the air quality impacts of pollutant emissions, it is important to understand the oxidant formation potential of the emitted species. Photolysis is the dominant atmospheric removal process for 2-nitrophenol. Although photodissociation dynamics studies of 2-nitrophenol have reported OH formation at photolysis wavelengths of 266 nm, 355 nm, and over the 361-390 nm range, and HONO has been observed as a product from 2-nitrophenol photolysis in an environmental chamber, the lack of quantitative absorption cross section and product quantum yield information has prevented quantitative assessment of the extent of oxidant formation from the photolysis of 2-nitrophenol in the atmosphere. My group determined the gas phase absorption cross sections of 2-nitrophenol in the 295-400 nm region by using cavity ring-down spectroscopy. The OH, HONO, and NO2 formation channels following the gas phase photolysis of 2-nitrophenol at 308 and 351 nm were investigated. Direct NO2 formation was not observed. OH and HONO were direct products from the 2-nitrophenol photolysis, and their quantum yields were obtained. The sum of the OH and the HONO quantum yields was about unity at both photolysis wavelengths. The estimated photolysis rate constant of 2-nitrophenol was about twice that of NO2. I will discuss the importance of 2-nitrophenol gas phase photolysis as a potential source of OH and HONO in regions of high anthropogenic emissions.

Imaging of Biological Cells Using Luminescent Silver Nanoparticles

NASA Astrophysics Data System (ADS)

Kravets, Vira; Almemar, Zamavang; Jiang, Ke; Culhane, Kyle; Machado, Rosa; Hagen, Guy; Kotko, Andriy; Dmytruk, Igor; Spendier, Kathrin; Pinchuk, Anatoliy

2016-01-01

The application of luminescent silver nanoparticles as imaging agents for neural stem and rat basophilic leukemia cells was demonstrated. The experimental size dependence of the extinction and emission spectra for silver nanoparticles were also studied. The nanoparticles were functionalized with fluorescent glycine dimers. Spectral position of the resonance extinction and photoluminescence emission for particles with average diameters ranging from 9 to 32 nm were examined. As the particle size increased, the spectral peaks for both extinction and the intrinsic emission of silver nanoparticles shifted to the red end of the spectrum. The intrinsic photoluminescence of the particles was orders of magnitude weaker and was spectrally separated from the photoluminescence of the glycine dimer ligands. The spectral position of the ligand emission was independent of the particle size; however, the quantum yield of the nanoparticle-ligand system was size-dependent. This was attributed to the enhancement of the ligand's emission caused by the local electric field strength's dependence on the particle size. The maximum quantum yield determined for the nanoparticle-ligand complex was (5.2 ± 0.1) %. The nanoparticles were able to penetrate cell membranes of rat basophilic leukemia and neural stem cells fixed with paraformaldehyde. Additionally, toxicity studies were performed. It was found that towards rat basophilic leukemia cells, luminescent silver nanoparticles had a toxic effect in the silver atom concentration range of 10-100 μM.

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

Wang, Peng; State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012; Bai, Xue, E-mail: baix@jlu.edu.cn, E-mail: yuzhang@jlu.edu.cn

High quantum yield, narrow full width at half-maximum and tunable emission color of perovskite quantum dots (QDs) make this kind of material good prospects for light-emitting diodes (LEDs). However, the relatively poor stability under high temperature and air condition limits the device performance. To overcome this issue, the liquid-type packaging structure in combination with blue LED chip was employed to fabricate the fluorescent perovskite quantum dot-based LEDs. A variety of monochromatic LEDs with green, yellow, reddish-orange, and red emission were fabricated by utilizing the inorganic cesium lead halide perovskite quantum dots as the color-conversion layer, which exhibited the narrow fullmore » width at half-maximum (<35 nm), the relatively high luminous efficiency (reaching 75.5 lm/W), and the relatively high external quantum efficiency (14.6%), making it the best-performing perovskite LEDs so far. Compared to the solid state LED device, the liquid-type LED devices exhibited excellent color stability against the various working currents. Furthermore, we demonstrated the potential prospects of all-inorganic perovskite QDs for the liquid-type warm white LEDs.« less

Quantum radiation reaction in laser-electron-beam collisions.

PubMed

Blackburn, T G; Ridgers, C P; Kirk, J G; Bell, A R

2014-01-10

It is possible using current high-intensity laser facilities to reach the quantum radiation reaction regime for energetic electrons. An experiment using a wakefield accelerator to drive GeV electrons into a counterpropagating laser pulse would demonstrate the increase in the yield of high-energy photons caused by the stochastic nature of quantum synchrotron emission: we show that a beam of 10(9) 1 GeV electrons colliding with a 30 fs laser pulse of intensity 10(22)  W cm(-2) will emit 6300 photons with energy greater than 700 MeV, 60× the number predicted by classical theory.

Photophysics and catalysis of porphyrinoids

NASA Astrophysics Data System (ADS)

Aggarwal, Amit

Organic nanoparticles (ONP) of metalloporphyrins can be versatile catalysts for the selective oxidation of alkenes and other hydrocarbons. Herein, we report the catalytic activity of ONP of 5,10,15,20-tetrakis-[4-(1'H,1'H,2'H,2'H-heptadecafluorodecane-1-thiol)-2,3,5,6-tetrafluorophenyl] porphyrinato iron(III), Fe(III)TPPF84, and 5,10,15,20-tetakis-(2,3,4,5,6-pentafluorophenyl) porphyrinato manganese(III), Mn(III)TPPF20, for cyclohexene oxidation using molecular oxygen as an oxidant in water under ambient conditions. Sequential dipping of indium-tin-oxide electrodes into solutions of tetra cationic porphyrins and tetra anionic polyoxometalates results in the controlled formation of nm thick films. The potential applications of these robust films on electrodes range from catalysts to sensors. This chapter focuses on the electrochemistry of the multilayered films where it is found that the oxidation and reduction potentials of each species remain largely the same as found in solution. Photophysical properties of Porphyrinoids bearing four rigid hydrogen bonding motifs on the meso positions, self-assembled into a cofacial cage with four complementary bis(decyl)melamine units in dry solvents are presented here. Self-assembly was investigated by NMR spectroscopy, dynamic light scattering, and atomic force microscopy. The phototphysical properties of the cage formation involve the measurement of their absorption and emission spectra and the fluorescence life time in dry THF. The hydrocarbon chains on the bis(decyl)melamine mediate the formation of nanofilms on surfaces as the solvent slowly evaporates. A systematic study of the photophysical properties of a series of porphyrinoids is presented. The role of the location of a heavy atom in shunting the excited state from the singlet to the triplet manifolds is compared for three cases. It is well known that Pt(II) metalloporphyrins do not fluoresce. For meso pyridyl porphyrins, the fluorescence quantum yield decreases as the number of coordinatively attached Pt(II) complexes increase from 0-4, but the tetracoordinated species retains about 30% of the fluorescence. Covalently attaching a heavy metal complex e.g. Pt(II) complex to the macrocycle by an organometalic bond at the peripheral meso position causes greater than a 20-fold decrease in fluorescence quantum yield and may enhance some internal conversion to the ground state. For comparison, the fluorescence quantum yield decreases somewhat as the number of pyridyl groups on the meso positions increase 0-4. We also evaluate the photophysical properties of a series of porphyrins with nitro groups on the beta pyrrole position and on the meso phenyl group, which also quenches the fluorescence. These studies bear on the use of metal ions to enhance the photophysical properties of these dyes as photodynamic therapeutics and for supramolecular systems, while the nitrated macrocycles have potential application in non linear optics. The photophysical properties of non-hydrolysable tetra- thioglycosylated conjugates of chlorin (CGlc4), isobacteriochlorin (IGlc4) and bacteriochlorin (BGlc4) and core F20 platforms are reported here. These studies involve the measurement of absorption and emission spectra, fluorescence quantum yield, singlet oxygen quantum yield, and singlet state life time in three different solvents: phosphate buffer saline (PBS), ethanol, and ethylacetate. Compared to the porphyrin in PBS, CGlc4 has a markedly greater absorbance of red light near 650 nm and a 6-fold increase in fluorescence quantum yield; whereas IGlc4 has broad Q bands and a 12-fold increase in fluorescence quantum yield. Since IGlc4 CGlc4 very slowly bleach, these properties may enable their use as fluorescent tags to track biological processes. BGlc4 has a similar fluorescence quantum yield to PGlc4, (<10%), but the lowest energy absorption/emission peaks of BGlc4 are considerably red shifted to near 730 nm with a nearly 50-fold greater absorbance, which may allow this conjugate to be an effective PDT agent. (Abstract shortened by UMI.)

Colloidal Spherical Quantum Wells with Near-Unity Photoluminescence Quantum Yield and Suppressed Blinking.

PubMed

Jeong, Byeong Guk; Park, Young-Shin; Chang, Jun Hyuk; Cho, Ikjun; Kim, Jai Kyeong; Kim, Heesuk; Char, Kookheon; Cho, Jinhan; Klimov, Victor I; Park, Philip; Lee, Doh C; Bae, Wan Ki

2016-10-02

Thick inorganic shell endows colloidal nanocrystals (NCs) with enhanced photochemical stability and suppression of photoluminescence intermittency (also known as blinking). However, the progress of using thick-shell heterostructure NCs in applications has been limited, due to low photoluminescence quantum yield (PL QY  60%) at room temperature. Here, we demonstrate thick-shell NCs with CdS/CdSe/CdS seed/spherical quantum well/shell (SQW) geometry that exhibit near-unity PL QY at room temperature and suppression of blinking. In SQW NCs, the lattice mismatch is diminished between the emissive CdSe layer and the surrounding CdS layers as a result of coherent strain, which suppresses the formation of misfit defects and consequently permits ~ 100% PL QY for SQW NCs with thick CdS shell (≥ 5 nm). High PL QY of thick-shell SQW NCs are preserved even in concentrated dispersion and in film under thermal stress, which makes them promising candidates for applications in solid-state lightings and luminescent solar concentrators.

Mechanism for the Green Glow of the Upper Ionosphere

NASA Technical Reports Server (NTRS)

Guberman, Steven L.

1997-01-01

The generation of the green line of atomic oxygen by dissociative recombination of 02 plus occurs by the capture of an electron into a repulsive state of 02 followed by dissociation along another state of a different electronic symmetry. The two states are coupled together by mixed symmetry Rydberg states. Quantum chemical calculations give a rate coefficient at room temperature of (0.39 (+ 0.31 or -0.19)) x 10 exp -8 cubic centimeters per second. The quantum yield of excited oxygen is within the range deduced from ground, rocket, and satellite observations. The rate coefficients and yields are needed in models of the optical emission, chemistry, and energy balance of planetary ionospheres.

An Environmentally Sensitive Fluorescent Dye as a Multidimensional Probe of Amyloid Formation

PubMed Central

2016-01-01

We have explored amyloid formation using poly(amino acid) model systems in which differences in peptide secondary structure and hydrophobicity can be introduced in a controlled manner. We show that an environmentally sensitive fluorescent dye, dapoxyl, is able to identify β-sheet structure and hydrophobic surfaces, structural features likely to be related to toxicity, as a result of changes in its excitation and emission profiles and its relative quantum yield. These results show that dapoxyl is a multidimensional probe of the time dependence of amyloid aggregation, which provides information about the presence and nature of metastable aggregation intermediates that is inaccessible to the conventional probes that rely on changes in quantum yield alone. PMID:26865546

Coexistence of strongly and weakly confined energy levels in (Cd,Zn)Se quantum dots: Tailoring the near-band-edge and defect-levels for white light emission

NASA Astrophysics Data System (ADS)

Das, Tapan Kumar; Ilaiyaraja, P.; Sudakar, C.

2017-05-01

We demonstrate white light emission (WLE) from (Cd,Zn)Se system, which is a composite of Zn alloyed CdSe quantum dot and ZnSe-amorphous (ZnSe-a) phase. Detailed structural and photoluminescence emission studies on pure CdSe and (Cd,Zn)Se show cubic zinc blende structure in the size range of 2.5 to 5 nm. (Cd,Zn)Se quantum dots (QDs) also have a significant fraction of ZnSe-a phase. The near-band-edge green-emission in crystalline CdSe and (Cd,Zn)Se is tunable between 500 to 600 nm. The (Cd,Zn)Se system also exhibits a broad, deep defect level (DL) red-emission in the range 600 to 750 nm and a sharp ZnSe near-band-edge blue-emission (ZS-NBE) between 445 to 465 nm. While DL and CdSe near-band-edge (CS-NBE) emissions significantly shift with the size of QD due to strong confinement effect, the ZS-NBE show minimal change in peak position indicating a weak confinement effect. The intensities of ZS-NBE and DL emissions also exhibit a strong dependence on the QD size. A gamut of emission colors is obtained by combining the CS-NBE with the ZS-NBE emission and broad DL emission in (Cd,Zn)Se system. Interestingly, we find the convergence of Commission Internationale de l'Eclairage (CIE) coordinates towards the white light with increasing Zn concentration in CdSe. We demonstrate by combining these three emissions in a proper weight ratio WLE can be achieved. Cd1-yZnySe (y = 0. 5; QD size ˜4.9 nm) alloy with a maximum quantum yield of 57% exhibits CIE coordinates of (0.39, 0.4), color rendering index (CRI) of 82, correlated color temperature (CCT) of 3922 K, and Duv of 0.0078 which is very promising for white light applications.

Growth of Nanosized Single Crystals for Efficient Perovskite Light-Emitting Diodes.

PubMed

Lee, Seungjin; Park, Jong Hyun; Nam, Yun Seok; Lee, Bo Ram; Zhao, Baodan; Di Nuzzo, Daniele; Jung, Eui Dae; Jeon, Hansol; Kim, Ju-Young; Jeong, Hu Young; Friend, Richard H; Song, Myoung Hoon

2018-04-24

Organic-inorganic hybrid perovskites are emerging as promising emitting materials due to their narrow full-width at half-maximum emissions, color tunability, and high photoluminescence quantum yields (PLQYs). However, the thermal generation of free charges at room temperature results in a low radiative recombination rate and an excitation-intensity-dependent PLQY, which is associated with the trap density. Here, we report perovskite films composed of uniform nanosized single crystals (average diameter = 31.7 nm) produced by introducing bulky amine ligands and performing the growth at a lower temperature. By effectively controlling the crystal growth, we maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges. Finally, highly bright and efficient green emissive perovskite light-emitting diodes that do not suffer from electroluminescence blinking were achieved with a luminance of up to 55 400 cd m -2 , current efficiency of 55.2 cd A -1 , and external quantum efficiency of 12.1%.

Double labelling of intracellular mitochondria and nucleolus using thiophene pyridium salt with high quantum yield as biosensor and its application in stimulated emission depletion nanoscopy.

PubMed

Tian, Xiaohe; Wang, Hui; Zhang, Qiong; Zhang, Mingzhu; Zhu, Yingzhong; Chen, Yan; Wu, Jieying; Tian, Yupeng

2018-05-30

Probe for dual-site target distinct subcellular compartments from cytosol and nucleus is an attractive approach, however, which was scarcely reported. Herein, a series of small-molecular thiophene pyridium salt derivatives (MitoNuc1-4) possessing water-soluble, high quantum yield and two-photon activity were rationally designed, and their structures were crystallographic confirmed. Systematic photophysical and biological imaging property investigations were carried out for them. It was found that MitoNuc1-4 exhibit two-photon absorption properties in the near infrared region, and MitoNuc1 has membrane permeability and cationic nature, rendering it to be double labelling of mitochondria and nucleolus in living cells with superb photo-stability and non-invasiveness. It also demonstrated that MitoNuc1 in living cells can monitor mitochondrial division in real time and revealed nucleolar ultrastructure under stimulated emission depletion nanoscopy. Copyright © 2017 Elsevier B.V. All rights reserved.

Solvatochromic fluorescence characteristics of cinnamoyl pyrone derivatives

NASA Astrophysics Data System (ADS)

Benosmane, Nadjib; Boutemeur, Baya; Hamdi, Safouane M.; Hamdi, Maamar; Silva, Artur S. M.

2017-12-01

The solvatochromic fluorescence behavior of cinnamoyl pyrone derivatives has been studied in several polar and non-polar solvents. The fluorescence spectra of these compounds exhibit red shift from its absorption spectra and present an excellent correlation with solvent polarity. Cinnamoyl pyrones show a significant spectral shift in fluorescence emission as a function of water composition in binary aqueous solutions mixture. This change is due to the specific intermolecular hydrogen bonding of cinnamoyl pyrones with a molecules of water, due to the deactivation of the lowest excited singlet state of these compounds. The relative quantum yields are calculated. It is found that the quantum yields of the cinnamoyl pyrones vary with the change in the solvent polarity indicating the dependency of fluorescence properties on the solvent nature. It has been observed that the addition of water and pH medium can affect the fluorescence properties of cinnamoyl pyrones in ethanol. This study exhibited that due to the solvent sensitive emission, cinnamoyl pyrone derivatives are a good compound to be used as fluorescence probes.

pH-Induced transformation of ligated Au25 to brighter Au23 nanoclusters.

PubMed

Waszkielewicz, Magdalena; Olesiak-Banska, Joanna; Comby-Zerbino, Clothilde; Bertorelle, Franck; Dagany, Xavier; Bansal, Ashu K; Sajjad, Muhammad T; Samuel, Ifor D W; Sanader, Zeljka; Rozycka, Miroslawa; Wojtas, Magdalena; Matczyszyn, Katarzyna; Bonacic-Koutecky, Vlasta; Antoine, Rodolphe; Ozyhar, Andrzej; Samoc, Marek

2018-05-01

Thiolate-protected gold nanoclusters have recently attracted considerable attention due to their size-dependent luminescence characterized by a long lifetime and large Stokes shift. However, the optimization of nanocluster properties such as the luminescence quantum yield is still a challenge. We report here the transformation of Au25Capt18 (Capt labels captopril) nanoclusters occurring at low pH and yielding a product with a much increased luminescence quantum yield which we have identified as Au23Capt17. We applied a simple method of treatment with HCl to accomplish this transformation and we characterized the absorption and emission of the newly created ligated nanoclusters as well as their morphology. Based on DFT calculations we show which Au nanocluster size transformations can lead to highly luminescent species such as Au23Capt17.

Highly Efficient Carbon Dots with Reversibly Switchable Green-Red Emissions for Trichromatic White Light-Emitting Diodes.

PubMed

Yuan, Biao; Guan, Shanyue; Sun, Xingming; Li, Xiaoming; Zeng, Haibo; Xie, Zheng; Chen, Ping; Zhou, Shuyun

2018-05-09

Carbon dots (CDs) have potentials to be utilized in optoelectronic devices, bioimaging, and photocatalysis. The majority of the current CDs with high quantum yield to date were limited in the blue light emission region. Herein, on the basis of surface electron-state engineering, we report a kind of CDs with reversible switching ability between green and red photoluminescence with a quantum yield (QY) of both up to 80%. Highly efficient green and red solid-state luminescence is realized by doping CDs into a highly transparent matrix of methyltriethoxysilane and 3-triethoxysilylpropylamine to form CDs/gel glasses composites with QYs of 80 and 78%. The CDs/gel glasses show better transmittance in visible light bands and excellent thermal stability. A blue-pumped CDs/gel glasses phosphor-based trichromatic white light-emitting diode (WLED) is realized, whose color rendering index is 92.9. The WLED gets the highest luminous efficiency of 71.75 lm W -1 in CDs-based trichromatic WLEDs. This work opens a door for developing highly efficient green- and red-emissive switching CDs which were used as phosphors for WLEDs and have the tendency for applications in other fields, such as sensing, bioimaging, and photocatalysis.

Novel highly luminescent amine-functionalized bridged silsesquioxanes

NASA Astrophysics Data System (ADS)

Pereira, Rui F. P.; Nunes, Sílvia C.; Toquer, Guillaume; Cardoso, Marita A.; Valente, Artur J. M.; Ferro, Marta C.; Silva, Maria M.; Carlos, Luís D.; Ferreira, Rute A. S.; de Zea Bermudez, Verónica

2017-12-01

Amine-functionalized bridged silsesquioxanes were synthesized from bis[(3-trimethoxysilyl)propyl] amine via a solvent-mediated route. BS-1 and BS-2 were obtained with neutral pH with sub- and stoichiometric amounts of water, respectively, and high tetrahydrofuran content. BS-3 was prepared with hyperstoichiometric water concentration, high tetrahydrofuran content and hydrochloric acid. BS-4 was synthesized with hyperstoichiometric water concentration, high ethanol content and sodium hydroxide. BS-1 and BS-2 were produced as transparent films, whereas BS-3 and BS-4 formed white powders. Face-to-face stacking of flat or folded lamellae yielded quasi-hydrophobic platelets with emission quantum yields of 0.05±0.01 (BS-1 and BS-2) or superhydrophilic onion-like nanoparticles with exciting emission quantum yields of 0.38±0.03 (BS-3) and 0.33±0.04 (BS-4), respectively. The latter two values are the largest ever reported for amine-functionalized siloxane-based hybrids lacking aromatic groups. Fast Grotthus proton hopping between =NH2+/=NH groups (BS-3) and =N-/=NH groups (BS-4), promoted by H+ and OH- ions, respectively, and aided by short amine-amine contacts provided by the onion-like morphology, account for this unique optical behavior.

Quantum-capacity-approaching codes for the detected-jump channel

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

Grassl, Markus; Wei Zhaohui; Ji Zhengfeng

2010-12-15

The quantum-channel capacity gives the ultimate limit for the rate at which quantum data can be reliably transmitted through a noisy quantum channel. Degradable quantum channels are among the few channels whose quantum capacities are known. Given the quantum capacity of a degradable channel, it remains challenging to find a practical coding scheme which approaches capacity. Here we discuss code designs for the detected-jump channel, a degradable channel with practical relevance describing the physics of spontaneous decay of atoms with detected photon emission. We show that this channel can be used to simulate a binary classical channel with both erasuresmore » and bit flips. The capacity of the simulated classical channel gives a lower bound on the quantum capacity of the detected-jump channel. When the jump probability is small, it almost equals the quantum capacity. Hence using a classical capacity-approaching code for the simulated classical channel yields a quantum code which approaches the quantum capacity of the detected-jump channel.« less

Mesoscopic entanglement induced by spontaneous emission in solid-state quantum optics.

PubMed

González-Tudela, Alejandro; Porras, Diego

2013-02-22

Implementations of solid-state quantum optics provide us with devices where qubits are placed at fixed positions in photonic or plasmonic one-dimensional waveguides. We show that solely by controlling the position of the qubits and with the help of a coherent driving, collective spontaneous decay may be engineered to yield an entangled mesoscopic steady state. Our scheme relies on the realization of pure superradiant Dicke models by a destructive interference that cancels dipole-dipole interactions in one dimension.

Enhanced Fluorescence Properties of Carbon Dots in Polymer Films

PubMed Central

Liu, Yamin; Wang, Ping; Shiral Fernando, K. A.; LeCroy, Gregory E.; Maimaiti, Halidan; Harruff-Miller, Barbara A.; Lewis, William K.; Bunker, Christopher E.; Hou, Zhi-Ling; Sun, Ya-Ping

2016-01-01

Carbon dots of small carbon nanoparticles surface-functionalized with 2,2′-(ethylenedioxy)bis(ethylamine) (EDA) were synthesized, and the as-synthesized sample was separated on an aqueous gel column to obtain fractions of the EDA-carbon dots with different fluorescence quantum yields. As already discussed in the literature, the variations in fluorescence performance among the fractions were attributed to the different levels and/or effectiveness of the surface functionalization-passivation in the carbon dots. These fractions, as well as carbon nanoparticles without any deliberate surface functionalization, were dispersed into poly(vinyl alcohol) (PVA) for composite films. In the PVA film matrix, the carbon dots and nanoparticles exhibited much enhanced fluorescence emissions in comparison with their corresponding aqueous solutions. The increased fluorescence quantum yields in the films were determined quantitatively by using a specifically designed and constructed film sample holder in the emission spectrometer. The observed fluorescence decays of the EDA-carbon dots in film and in solution were essentially the same, suggesting that the significant enhancement in fluorescence quantum yields from solution to film is static in nature. Mechanistic implications of the results, including a rationalization in terms of the compression effect on the surface passivation layer (similar to a soft corona) in carbon dots when embedded in the more restrictive film environment resulting in more favorable radiative recombinations of the carbon particle surface-trapped electrons and holes, and also potential technological applications of the brightly fluorescent composite films are highlighted and discussed. PMID:28133537

Highly luminescent and color-tunable salicylate ionic liquids

DOE PAGES

Campbell, Paul S.; Yang, Mei; Pitz, Demian; ...

2014-03-11

High quantum yields of up to 40.5 % can be achieved in salicylate-bearing ionic liquids. A range of these ionic liquids have been synthesized and their photoluminescent properties studied in detail. The differences noted can be related back to the structure of the ionic liquid cation and possible interionic interactions. It is found that shifts of emission, particularly in the pyridinium-based ionic liquids, can be related to cation–anion pairing interactions. Furthermore, facile and controlled emission color mixing is demonstrated through combining different ILs, with emission colors ranging from blue to yellow.

Next-generation in vivo optical imaging with short-wave infrared quantum dots

PubMed Central

Bruns, Oliver T.; Bischof, Thomas S.; Harris, Daniel K.; Franke, Daniel; Shi, Yanxiang; Riedemann, Lars; Bartelt, Alexander; Jaworski, Frank B.; Carr, Jessica A.; Rowlands, Christopher J.; Wilson, Mark W.B.; Chen, Ou; Wei, He; Hwang, Gyu Weon; Montana, Daniel M.; Coropceanu, Igor; Achorn, Odin B.; Kloepper, Jonas; Heeren, Joerg; So, Peter T.C.; Fukumura, Dai; Jensen, Klavs F.; Jain, Rakesh K.; Bawendi, Moungi G.

2017-01-01

For in vivo imaging, the short-wavelength infrared region (SWIR; 1000–2000 nm) provides several advantages over the visible and near-infrared regions: general lack of autofluorescence, low light absorption by blood and tissue, and reduced scattering. However, the lack of versatile and functional SWIR emitters has prevented the general adoption of SWIR imaging by the biomedical research community. Here, we introduce a class of high-quality SWIR-emissive indium-arsenide-based quantum dots (QDs) that are readily modifiable for various functional imaging applications, and that exhibit narrow and size-tunable emission and a dramatically higher emission quantum yield than previously described SWIR probes. To demonstrate the unprecedented combination of deep penetration, high spatial resolution, multicolor imaging and fast-acquisition-speed afforded by the SWIR QDs, we quantified, in mice, the metabolic turnover rates of lipoproteins in several organs simultaneously and in real time as well as heartbeat and breathing rates in awake and unrestrained animals, and generated detailed three-dimensional quantitative flow maps of the mouse brain vasculature. PMID:29119058

Realization of a Cascaded Quantum System: Heralded Absorption of a Single Photon Qubit by a Single-Electron Charged Quantum Dot.

PubMed

Delteil, Aymeric; Sun, Zhe; Fält, Stefan; Imamoğlu, Atac

2017-04-28

Photonic losses pose a major limitation for the implementation of a quantum state transfer between nodes of a quantum network. A measurement that heralds a successful transfer without revealing any information about the qubit may alleviate this limitation. Here, we demonstrate the heralded absorption of a single photonic qubit, generated by a single neutral quantum dot, by a single-electron charged quantum dot that is located 5 m away. The transfer of quantum information to the spin degree of freedom takes place upon the emission of a photon; for a properly chosen or prepared quantum dot, the detection of this photon yields no information about the qubit. We show that this process can be combined with local operations optically performed on the destination node by measuring classical correlations between the absorbed photon color and the final state of the electron spin. Our work suggests alternative avenues for the realization of quantum information protocols based on cascaded quantum systems.

Optical and Photophysical Investigation of (2E)-1-(2,5-Dimethylfuran-3-Yl)-3-(9-Ethyl-9H-Carbazol-3-Yl)Prop-2-en-1-One (DEPO) by Spectrofluorometer in Organized Medium.

PubMed

Asiri, Abdullah M; Al-Dies, Al-Anood M; Khan, Salman A

2017-07-01

(2E)-1-(2,5-dimethylfuran-3-yl)-3-(9-ethyl-9H-carbazol-3-yl)prop-2-en-1-one (DEPO) was prepared by the reaction of 9-ethyl-9H-carbazole-3-carbaldehyde with 1-(2,5-dimethylfuran-3-yl)ethanone under microwave irradiation. The structure of DEPO was established experimentally by EI-MS, FT-IR, 1 H and 13 C NMR spectral studies. Electronic absorption and emission spectra of DEPO were studied in different solvents on the basis of polarities, and the obtain data were used to determine the solvatochromic properties such as extinction coefficient, oscillator strength, transition dipole moment, stokes shift, fluorescence quantum yield and photochemical quantum yield. Photochemical quantum yield (Φ c ) of DEPO dye was determined in different solvent. The dye comparatively photostable in DMSO but undergoes photodecomposition in chloro methane solvents. The DEPO dye may be use as probe or quencher to determine critical micelle concentration (CMC) of cetyltri methyl ammonium bromide (CTAB) and sodium dodecyl sulfate (SDS).

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

Mieno, H.; Kabe, R.; Allendorf, M. D.

Here, the first metal–organic framework exhibiting thermally activated delayed fluorescence (TADF) was developed. The zirconium-based framework (UiO-68-dpa) uses a newly designed linker composed of a terphenyl backbone, an electron-accepting carboxyl group, and an electron-donating diphenylamine and exhibits green TADF emission with a photoluminescence quantum yield of 30% and high thermal stability.

Optimal control of photoelectron emission by realistic waveforms

NASA Astrophysics Data System (ADS)

Solanpää, J.; Ciappina, M. F.; Räsänen, E.

2017-09-01

Recent experimental techniques in multicolor waveform synthesis allow the temporal shaping of strong femtosecond laser pulses with applications in the control of quantum mechanical processes in atoms, molecules, and nanostructures. Prediction of the shapes of the optimal waveforms can be done computationally using quantum optimal control theory. In this work we demonstrate the control of above-threshold photoemission of one-dimensional hydrogen model with pulses feasible for experimental waveform synthesis. By mixing different spectral channels and thus lowering the intensity requirements for individual channels, the resulting optimal pulses can extend the cutoff energies by at least up to 50% and bring up the electron yield by several orders of magnitude. Insights into the electron dynamics for optimized photoelectron emission are obtained with a semiclassical two-step model.

Quantum Chemical Design Guidelines for Absorption and Emission Color Tuning of fac-Ir(ppy)₃ Complexes.

PubMed

Natori, Yoshiki; Kitagawa, Yasutaka; Aoki, Shogo; Teramoto, Rena; Tada, Hayato; Era, Iori; Nakano, Masayoshi

2018-03-05

The fac -Ir(ppy)₃ complex, where ppy denotes 2-phenylpyridine, is one of the well-known luminescent metal complexes having a high quantum yield. However, there have been no specific molecular design guidelines for color tuning. For example, it is still unclear how its optical properties are changed when changing substitution groups of ligands. Therefore, in this study, differences in the electronic structures and optical properties among several substituted fac -Ir(ppy)₃ derivatives are examined in detail by density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations. On the basis of those results, we present rational design guidelines for absorption and emission color tuning by modifying the species of substituents and their substitution positions.

Effects of surface and interface traps on exciton and multi-exciton dynamics in core/shell quantum dots

NASA Astrophysics Data System (ADS)

Bozio, Renato; Righetto, Marcello; Minotto, Alessandro

2017-08-01

Exciton interactions and dynamics are the most important factors determining the exceptional photophysical properties of semiconductor quantum dots (QDs). In particular, best performances have been obtained for ingeniously engineered core/shell QDs. We have studied two factors entering in the exciton decay dynamics with adverse effects for the luminescence efficiency: exciton trapping at surface and interface traps, and non-radiative Auger recombination in QDs carrying either net charges or multiple excitons. In this work, we present a detailed study into the optical absorption, fluorescence dynamics and quantum yield, as well as ultrafast transient absorption properties of CdSe/CdS, CdSe/Cd0.5Zn0.5S, and CdSe/ZnS QDs as a function of shell thickness. It turns out that de-trapping processes play a pivotal role in determining steady state emission properties. By studying the excitation dependent photoluminescence quantum yields (PLQY) in different CdSe/CdxZn1-xS (x = 0, 0.5, 1) QDs, we demonstrate the different role played by hot and cold carrier trapping rates in determining fluorescence quantum yields. Finally, the use of global analysis allows us untangling the complex ultrafast transient absorption signals. Smoothing of interface potential, together with effective surface passivation, appear to be crucial factors in slowing down both Auger-based and exciton trapping recombination processes.

Water-soluble multidentate polymers compactly coating Ag2S quantum dots with minimized hydrodynamic size and bright emission tunable from red to second near-infrared region.

PubMed

Gui, Rijun; Wan, Ajun; Liu, Xifeng; Yuan, Wen; Jin, Hui

2014-05-21

Hydrodynamic size-minimized quantum dots (QDs) have outstanding physicochemical properties for applications in multicolor molecular and cellular imaging at the level of single molecules and nanoparticles. In this study, we have reported the aqueous synthesis of Ag2S QDs by using thiol-based multidentate polymers as capping reagents. By regulating the composition of the precursors (AgNO3 and sulfur-N2H4·H2O complex) and multidentate polymers (poly(acrylic acid)-graft-cysteamine-graft-ethylenediamine), as well as the reaction time, Ag2S QDs (2.6-3.7 nm) are prepared, displaying tunable photoluminescence (PL) emission from red to the second near-infrared region (687-1096 nm). The small hydrodynamic thickness (1.6-1.9 nm) of the multidentate polymers yields a highly compact coating for the QDs, which results in the bright fluorescent QDs with high PL quantum yields (QYs: 14.2-16.4%). Experimental results confirm that the QDs have high PL stability and ultralow cytotoxicity, as well as high PLQYs and small hydrodynamic sizes (4.5-5.6 nm) similar to fluorescent proteins (27-30 kDa), indicating the feasibility of highly effective PL imaging in cells and living animals.

Optical Properties of CdSe/ZnS Nanocrystals

PubMed Central

Gaigalas, Adolfas K; DeRose, Paul; Wang, Lili; Zhang, Yu-Zhong

2014-01-01

Measurements are presented of the absorbance, fluorescence emission, fluorescence quantum yield, and fluorescence lifetime of CdSe/ZnS nanocrystals, also known as quantum dots (QDs). The study included three groups of nanocrystals whose surfaces were either passivated with organic molecules, modified further with carboxyl groups, or conjugated with CD14 mouse anti-human antibodies. The surface modifications had observable effects on the optical properties of the nanocrystals. The oscillator strength (OS) of the band edge transition was about 1.0 for the nanocrystals emitting at 565 nm, 605 nm, and 655 nm. The OS could not be determined for QDs with emission at 700 nm and 800 nm. The fluorescence lifetimes varied from 26 ns for nanocrystals emitting near 600 nm to 150 ns for nanocrystals emitting near 800 nm. The quantum yield ranged between 0.4 and 0.9 for the nanocrystals in this study. A brightness index (BI) was used to evaluate the suitability of the nanocrystal labels for flow cytometer measurements. Most QD labels are at least as bright as fluorescein for applications in flow cytometer assays with 488 nm excitation. For optimal brightness the QDs should be excited with 405 nm light. We observed a strong dependence of the QD absorbance at 250 nm on the surface modification of the QD. PMID:26601047

Near-infrared emission from mesoporous crystalline germanium

NASA Astrophysics Data System (ADS)

Boucherif, Abderraouf; Korinek, Andreas; Aimez, Vincent; Arès, Richard

2014-10-01

Mesoporous crystalline germanium was fabricated by bipolar electrochemical etching of Ge wafer in HF-based electrolyte. It yields uniform mesoporous germanium layers composed of high density of crystallites with an average size 5-7 nm. Subsequent extended chemical etching allows tuning of crystallites size while preserving the same chemical composition. This highly controllable nanostructure exhibits photoluminescence emission above the bulk Ge bandgap, in the near-infrared range (1095-1360nm) with strong evidence of quantum confinement within the crystallites.

Single-mode light source fabrication based on colloidal quantum dots

NASA Astrophysics Data System (ADS)

Xu, Jianfeng; Chen, Bing; Baig, Sarfaraz; Wang, Michael R.

2009-02-01

There are huge market demands for innovative, cheap and efficient light sources, including light emitting devices, such as LEDs and lasers. However, the light source development in the visible spectral range encounters significant difficulties these years. The available visible wavelength LEDs or lasers are few, large and expensive. The main challenge lies at the lack of efficient light media. Semiconductor nanocrystal quantum dots (QDs) have recently commanded considerable attention. As a result of quantum confinement effect, the emission color of these QDs covers the whole visible spectral range and can be modified dramatically by simply changing their size. Such spectral tunability, together with large photoluminescence quantum yield and photostability, make QDs attractive for potential applications in a variety of light emitting technologies. However, there are still several technical problems that hinder their application as light sources. One main issue is how to fabricate these QDs into a solid state device while still retaining their original optical emission properties. A vacuum assisted micro-fluidic fabrication of guided wave devices has demonstrated low waveguide propagation loss, lower crosstalk, and improved waveguide structures. We report herein the combination of the excellent emission properties of QDs and novel vacuum assisted micro-fluidic photonic structure fabrication technique to realize single-mode efficient light sources.

Excited-state decay processes of binuclear rhodium(I) isocyanide complexes

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

Miskowski, V.M.; Rice, S.F.; Gray, H.B.

1993-04-29

Emission lifetimes, quantum yields, and polarized excitation spectra of Rh[sub 2]b[sub 4][sup 2+] and Rh[sub 2](TMB)[sub 4][sup 2+] (b = 1,3-diisocyanopropane; TMB = 2,5-diisocyano-2,5-dimethylhexane) have been determined. The singlet and triplet d[sigma]* [yields] p[sigma]([sup 1,3]A[sub 2u]) excited states are luminescent with radiative rates of ca. 10[sup 8] and 10[sup 4] s[sup [minus

Red electroluminescence and photoluminescence properties of new porphyrin compounds

NASA Astrophysics Data System (ADS)

Zhang, X. H.; Xie, Z. Y.; Wu, F. P.; Zhou, L. L.; Wong, O. Y.; Lee, C. S.; Kwong, H. L.; Lee, S. T.; Wu, S. K.

2003-12-01

Three new porphyrin compounds with saturated red emission were synthesized and their photoluminescence and electroluminescence were studied. The emission of the new dopants peaked at about 635-655 nm and the half-width of the emission peaks was very narrow (below 30 nm). Of the three porphyrin compounds, the one (TBDPP) with the smallest conjugation system had the highest fluorescent quantum yield of 21% in solution. Organic light-emitting diodes using TBDPP as a dopant showed saturated red emission (CIE coordinates of x=0.69, y=0.29) with a luminance of 150 cd/m 2 at a driving voltage of 22 V.

Controlled synthesis of AlN/GaN multiple quantum well nanowire structures and their optical properties.

PubMed

Qian, Fang; Brewster, Megan; Lim, Sung K; Ling, Yichuan; Greene, Christopher; Laboutin, Oleg; Johnson, Jerry W; Gradečak, Silvija; Cao, Yu; Li, Yat

2012-06-13

We report the controlled synthesis of AlN/GaN multi-quantum well (MQW) radial nanowire heterostructures by metal-organic chemical vapor deposition. The structure consists of a single-crystal GaN nanowire core and an epitaxially grown (AlN/GaN)(m) (m = 3, 13) MQW shell. Optical excitation of individual MQW nanowires yielded strong, blue-shifted photoluminescence in the range 340-360 nm, with respect to the GaN near band-edge emission at 368.8 nm. Cathodoluminescence analysis on the cross-sectional MQW nanowire samples showed that the blue-shifted ultraviolet luminescence originated from the GaN quantum wells, while the defect-associated yellow luminescence was emitted from the GaN core. Computational simulation provided a quantitative analysis of the mini-band energies in the AlN/GaN superlattices and suggested the observed blue-shifted emission corresponds to the interband transitions between the second subbands of GaN, as a result of quantum confinement and strain effect in these AlN/GaN MQW nanowire structures.

Color tunable hybrid light-emitting diodes based on perovskite quantum dot/conjugated polymer

NASA Astrophysics Data System (ADS)

Germino, José C.; Yassitepe, Emre; Freitas, Jilian N.; Santiago, Glauco M.; Bonato, Luiz Gustavo; de Morais, Andréia; Atvars, Teresa D. Z.; Nogueira, Ana F.

2017-08-01

Inorganic organic metal halide perovskite materials have been investigated for several technological applications, such as photovoltaic cells, lasers, photodetectors and light emitting diodes (LEDs), either in the bulk form or as colloidal nanoparticles. Recently, all inorganic Cesium Lead Halide (CsPbX3, X=Cl,Br, I) perovskite quantum dots (PQDs) were reported with high photoluminescence quantum yield with narrow emission lines in the visible wavelengths. Here, green-emitting perovskite quantum dots (PQDs) prepared by a synthetic method based on a mixture of oleylamine and oleic acid as surfactants were applied in the electroluminescent layer of hybrid LEDs in combination with two different conjugated polymers: polyvinylcarbazole (PVK) or poly(9,9-di-n-octylfluorenyl-2,7-diyl) (PFO). The performance of the diodes and the emission color tuning upon dispersion of different concentrations of the PQDs in the polymer matrix is discussed. The presented approach aims at the combination of the optical properties of the PQDs and their interaction with wide bandgap conjugated polymers, associated with the solution processing ability of these materials.

Room temperature synthesis of pH-switchable polyaniline quantum dots as a turn-on fluorescent probe for acidic biotarget labeling.

PubMed

Liu, Yanfeng; Ding, Yin; Gou, Huilin; Huang, Xin; Zhang, Guiyang; Zhang, Qi; Liu, Yunzhong; Meng, Zhen; Xi, Kai; Jia, Xudong

2018-04-05

The synthesis of well-defined light-element-derived quantum dots (LEQDs) with advanced optical properties under mild conditions is highly desirable yet challenging. Here, a polyaniline (PANI) structure is introduced into carbon-rich LEQDs to yield well-defined, fluorescent polyaniline quantum dots (PAQDs), PAQD24, through a one-pot room temperature reaction. The mild synthetic conditions effectively minimize the defects introduced during the conventional synthesis and endow PAQD24 with desirable optical properties, including a narrow emission band (full width at half maximum = 55 nm), an optimal quantum yield of 32.5% and two-photon fluorescence. Furthermore, the bandgap of PAQD24 is highly sensitive toward pH variations in the near-neutral region, due to the proton doping and dedoping of the PANI structure. Such unique properties together with its fine bio-compatibility enable the application of this material as a turn-on fluorescent probe for the labeling of acidic biotargets from sub-cellular to organ levels, providing potential applications in diagnosis and surgery guidance for certain diseases.

Phase transfer of 1- and 2-dimensional Cd-based nanocrystals

NASA Astrophysics Data System (ADS)

Kodanek, Torben; Banbela, Hadeel M.; Naskar, Suraj; Adel, Patrick; Bigall, Nadja C.; Dorfs, Dirk

2015-11-01

In this work, luminescent CdSe@CdS dot-in-rod nanocrystals, CdSe@CdS/ZnS nanorods as well as CdSe-CdS core-crown nanoplatelets were transferred into aqueous phase via ligand exchange reactions. For this purpose, bifunctional thiol-based ligands were employed, namely mercaptoacetic acid (MAA), 3-mercaptopropionic acid (MPA), 11-mercaptoundecanoic acid (MUA) as well as 2-(dimethylamino)ethanthiol (DMAET). Systematic investigations by means of photoluminescence quantum yield measurements as well as photoluminescence decay measurements have shown that the luminescence properties of the transferred nanostructures are affected by hole traps (induced by the thiol ligands themselves) as well as by spatial insulation and passivation against the environment. The influence of the tips of the nanorods on the luminescence is, however, insignificant. Accordingly, different ligands yield optimum results for different nanoparticle samples, mainly depending on the inorganic passivation of the respective samples. In case of CdSe@CdS nanorods, the highest emission intensities have been obtained by using short-chain ligands for the transfer preserving more than 50% of the pristine quantum yield of the hydrophobic nanorods. As opposed to this, the best possible quantum efficiency for the CdSe@CdS/ZnS nanorods has been achieved via MUA. The gained knowledge could be applied to transfer for the first time 2-dimensional CdSe-CdS core-crown nanoplatelets into water while preserving significant photoluminescence (up to 12% quantum efficiency).In this work, luminescent CdSe@CdS dot-in-rod nanocrystals, CdSe@CdS/ZnS nanorods as well as CdSe-CdS core-crown nanoplatelets were transferred into aqueous phase via ligand exchange reactions. For this purpose, bifunctional thiol-based ligands were employed, namely mercaptoacetic acid (MAA), 3-mercaptopropionic acid (MPA), 11-mercaptoundecanoic acid (MUA) as well as 2-(dimethylamino)ethanthiol (DMAET). Systematic investigations by means of photoluminescence quantum yield measurements as well as photoluminescence decay measurements have shown that the luminescence properties of the transferred nanostructures are affected by hole traps (induced by the thiol ligands themselves) as well as by spatial insulation and passivation against the environment. The influence of the tips of the nanorods on the luminescence is, however, insignificant. Accordingly, different ligands yield optimum results for different nanoparticle samples, mainly depending on the inorganic passivation of the respective samples. In case of CdSe@CdS nanorods, the highest emission intensities have been obtained by using short-chain ligands for the transfer preserving more than 50% of the pristine quantum yield of the hydrophobic nanorods. As opposed to this, the best possible quantum efficiency for the CdSe@CdS/ZnS nanorods has been achieved via MUA. The gained knowledge could be applied to transfer for the first time 2-dimensional CdSe-CdS core-crown nanoplatelets into water while preserving significant photoluminescence (up to 12% quantum efficiency). Electronic supplementary information (ESI) available: Further TEM images, further extinction spectra, particle size distribution and discussion about optical properties of the hydrophobic nanostructures. See DOI: 10.1039/c5nr06221g

Synthesis and fluorescence properties of some difluoroboron β-diketonate complexes and composite containing PMMA

NASA Astrophysics Data System (ADS)

Xing, Dongye; Hou, Yanjun; Niu, Haijun

2018-03-01

A series of difluoroboron β-diketonate complexes, containing the indon-β-diketonate ligand carrying methyl or methoxyl substituents was synthesized. The crystal structures of the complexes were confirmed by single crystal X-ray diffraction studies. The fluorescence properties of compounds were studied in solution state, solid state and on PMMA polymer matrix. The photophysical data of compounds 2a-2d exhibited strong fluorescence and photostability under the ultraviolet light (Hg lamp). The complex 2b showed higher fluorescence intensity in solution state as compared to other complexes of the series. The complexes 2c and 2d showed higher fluorescence intensity in the solid state, which are ascribed to the stronger π-π interactions between ligands in the solid state. The introduction of methoxyl or methyl groups on the benzene rings enhanced the absorption intensity, emission intensity, quantum yields and fluorescence lifetimes due to their electron-donating nature. Furthermore, the complex 2b was doped into the PMMA to produce hybrid materials, where the PMMA matrix acted as sensitizer for the central boron ion to enhance the fluorescence emission intensity and quantum yields.

Synthesis and spectroscopic behavior of highly luminescent Eu 3+-dibenzoylmethanate (DBM) complexes with sulfoxide ligands

NASA Astrophysics Data System (ADS)

Niyama, E.; Brito, H. F.; Cremona, M.; Teotonio, E. E. S.; Reyes, R.; Brito, G. E. S.; Felinto, M. C. F. C.

2005-09-01

In this paper the synthesis, characterization and photoluminescent behavior of the [RE(DBM) 3L 2] complexes (RE = Gd and Eu) with a variety of sulfoxide ligands; L = benzyl sulfoxide (DBSO), methyl sulfoxide (DMSO), phenyl sulfoxide (DPSO) and p-tolyl sulfoxide (PTSO) have been investigated in solid state. The emission spectra of the Eu 3+-β-diketonate complexes show characteristics narrow bands arising from the 5D 0 → 7F J ( J = 0-4) transitions, which are split according to the selection rule for C n, C nv or C s site symmetries. The experimental Judd-Ofelt intensity parameters ( Ω2 and Ω4), radiative ( Arad) and non-radiative ( Anrad) decay rates, and R02 for the europium complexes have been determined and compared. The highest value of Ω2 (61.9 × 10 -20 cm 2) was obtained to the complex with PTSO ligand, indicating that Eu 3+ ion is in the highly polarizable chemical environment. The higher values of the experimental quantum yield ( q) and emission quantum efficiency of the emitter 5D 0 level ( η) for the Eu-complexes with DMSO, DBSO and PTSO sulfoxides suggest that these complexes are promising Light Conversion Molecular Devices (LCMDs). The lower value of quantum yield ( q = 1%), for the hydrated complex [Eu(DBM) 3(H 2O)], indicates that the luminescence quenching occurs via multiphonon relaxation by coupling with the OH-oscillators from water molecule coordinated to rare earth ion. The pure red emission of the Eu-complexes has been confirmed by ( x, y) color coordinates.

Poly(naphthalene diimide) vinylene: solid state red emission and semiconducting properties for transistors

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

Liang, Xianfeng; Tan, Luxi; Liu, Zitong

Here in this work, a conjugated polymer PNV is developed, linking naphthalene diimide with a vinyl linkage. Owing to the C-H ∙∙∙O hydrogen bond between the carbonyl and the vinyl, PNV exhibits a high red emission with a quantum yield of 33.4% in the solid state while it shows n-type properties with an electron mobility up to 1.5 x 10 -3 cm 2 V -1 s -1 in organic field effect transistors, simultaneously.

Poly(naphthalene diimide) vinylene: solid state red emission and semiconducting properties for transistors

DOE PAGES

Liang, Xianfeng; Tan, Luxi; Liu, Zitong; ...

2017-04-06

Here in this work, a conjugated polymer PNV is developed, linking naphthalene diimide with a vinyl linkage. Owing to the C-H ∙∙∙O hydrogen bond between the carbonyl and the vinyl, PNV exhibits a high red emission with a quantum yield of 33.4% in the solid state while it shows n-type properties with an electron mobility up to 1.5 x 10 -3 cm 2 V -1 s -1 in organic field effect transistors, simultaneously.

Optical characterization of Nd (3+):AgBr.

PubMed

Bunimovich, D; Nagli, L; Katzir, A

1997-10-20

The luminescence of silver bromide crystals, doped with neodymium, was investigated over the visible and near-infrared spectral ranges. The emission, excitation, and absorption spectra were measured over a broad temperature range. The absolute luminescence quantum yield was estimated by comparing the luminescence with that of a neodymium-doped phosphate glass, for which the manufacturer gives a value of 0.4. The Judd-Ofelt analysis was applied to both materials, and transition rates, branching ratios, and quantum efficiencies were calculated for all the observed bands. Good agreement was obtained between theory and experiment.

Synthesis and formation mechanistic investigation of nitrogen-doped carbon dots with high quantum yields and yellowish-green fluorescence

NASA Astrophysics Data System (ADS)

Hou, Juan; Wang, Wei; Zhou, Tianyu; Wang, Bo; Li, Huiyu; Ding, Lan

2016-05-01

Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively.Heteroatom doped carbon dots (CDs) have received increasing attention due to their unique properties and related applications. However, previously reported CDs generally show strong emission only in the blue-light region, thus restricting their further applications. And the fundamental investigation on the preparation process is always neglected. Herein, we have developed a simple and solvent-free synthetic strategy to fabricate nitrogen-doped CDs (N-CDs) from citric acid and dicyandiamide. The as-prepared N-CDs exhibited a uniform size distribution, strong yellowish-green fluorescence emission and a high quantum yield of 73.2%. The products obtained at different formation stages were detailedly characterized by transmission electron microscopy, X-ray diffraction spectrometer, X-ray photoelectron spectroscopy and UV absorbance spectroscopy. A possible formation mechanism has thus been proposed including dehydration, polymerization and carbonization. Furthermore, the N-CDs could serve as a facile and label-free probe for the detection of iron and fluorine ions with detection limits of 50 nmol L-1 and 75 nmol L-1, respectively. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr02701f

Excited-State Proton-Transfer-Induced Trapping Enhances the Fluorescence Emission of a Locked GFP Chromophore

PubMed Central

2016-01-01

The chemical locking of the central single bond in core chromophores of green fluorescent proteins (GFPs) influences their excited-state behavior in a distinct manner. Experimentally, it significantly enhances the fluorescence quantum yield of GFP chromophores with an ortho-hydroxyl group, while it has almost no effect on the photophysics of GFP chromophores with a para-hydroxyl group. To unravel the underlying physical reasons for this different behavior, we report static electronic structure calculations and nonadiabatic dynamics simulations on excited-state intramolecular proton transfer, cis–trans isomerization, and excited-state deactivation in a locked ortho-substituted GFP model chromophore (o-LHBI). On the basis of our previous and present results, we find that the S1 keto species is responsible for the fluorescence emission of the unlocked o-HBI and the locked o-LHBI species. Chemical locking does not change the parts of the S1 and S0 potential energy surfaces relevant to enol–keto tautomerization; hence, in both chromophores, there is an ultrafast excited-state intramolecular proton transfer that takes only 35 fs on average. However, the locking effectively hinders the S1 keto species from approaching the keto S1/S0 conical intersections so that most of trajectories are trapped in the S1 keto region for the entire 2 ps simulation time. Therefore, the fluorescence quantum yield of o-LHBI is enhanced compared with that of unlocked o-HBI, in which the S1 excited-state decay is efficient and ultrafast. In the case of the para-substituted GFP model chromophores p-HBI and p-LHBI, chemical locking hardly affects their efficient excited-state deactivation via cis–trans isomerization; thus, the fluorescence quantum yields in these chromophores remain very low. The insights gained from the present work may help to guide the design of new GFP chromophores with improved fluorescence emission and brightness. PMID:26744782

Why Do Simple Molecules with "Isolated" Phenyl Rings Emit Visible Light?

PubMed

Zhang, Haoke; Zheng, Xiaoyan; Xie, Ni; He, Zikai; Liu, Junkai; Leung, Nelson L C; Niu, Yingli; Huang, Xuhui; Wong, Kam Sing; Kwok, Ryan T K; Sung, Herman H Y; Williams, Ian D; Qin, Anjun; Lam, Jacky W Y; Tang, Ben Zhong

2017-11-15

π-Bonds connected with aromatic rings were generally believed as the standard structures for constructing highly efficient fluorophores. Materials without these typical structures, however, exhibited only low fluorescence quantum yields and emitted in the ultraviolet spectral region. In this work, three molecules, namely bis(2,4,5-trimethylphenyl)methane, 1,1,2,2-tetrakis(2,4,5-trimethylphenyl)ethane, and 1,1,2,2-tetraphenylethane, with nonconjugated structures and isolated phenyl rings were synthesized and their photophysical properties were systematically investigated. Interestingly, the emission spectra of these three molecules could be well extended to 600 nm with high solid-state quantum yields of up to 70%. Experimental and theoretical analyses proved that intramolecular through-space conjugation between the "isolated" phenyl rings played an important role for this abnormal phenomenon.

A hybrid plasmonic waveguide terahertz quantum cascade laser

NASA Astrophysics Data System (ADS)

Degl'Innocenti, Riccardo; Shah, Yash D.; Wallis, Robert; Klimont, Adam; Ren, Yuan; Jessop, David S.; Beere, Harvey E.; Ritchie, David A.

2015-02-01

We present the realization of a quantum cascade laser emitting at around 2.85 THz, based on a hybrid plasmonic waveguide with a low refractive index dielectric cladding. This hybrid waveguide design allows the performance of a double-metal waveguide to be retained, while improving the emission far-field. A set of lasers based on the same active region material were fabricated with different metal layer thicknesses. A detailed characterization of the performance of these lasers revealed that there is an optimal trade-off that yields the best far-field emission and the maximum temperature of operation. By exploiting the pure plasmonic mode of these waveguides, the standard operation conditions of a double-metal quantum cascade laser were retrieved, such that the maximum operating temperature of these devices is not affected by the process. These results pave the way to realizing a class of integrated devices working in the terahertz range which could be further exploited to fabricate terahertz on-chip circuitry.

A hybrid plasmonic waveguide terahertz quantum cascade laser

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

Degl'Innocenti, Riccardo, E-mail: rd448@cam.ac.uk; Shah, Yash D.; Wallis, Robert

2015-02-23

We present the realization of a quantum cascade laser emitting at around 2.85 THz, based on a hybrid plasmonic waveguide with a low refractive index dielectric cladding. This hybrid waveguide design allows the performance of a double-metal waveguide to be retained, while improving the emission far-field. A set of lasers based on the same active region material were fabricated with different metal layer thicknesses. A detailed characterization of the performance of these lasers revealed that there is an optimal trade-off that yields the best far-field emission and the maximum temperature of operation. By exploiting the pure plasmonic mode of thesemore » waveguides, the standard operation conditions of a double-metal quantum cascade laser were retrieved, such that the maximum operating temperature of these devices is not affected by the process. These results pave the way to realizing a class of integrated devices working in the terahertz range which could be further exploited to fabricate terahertz on-chip circuitry.« less

Enhanced carrier multiplication in engineered quasi-type-II quantum dots

PubMed Central

Cirloganu, Claudiu M.; Padilha, Lazaro A.; Lin, Qianglu; Makarov, Nikolay S.; Velizhanin, Kirill A.; Luo, Hongmei; Robel, Istvan; Pietryga, Jeffrey M.; Klimov, Victor I.

2014-01-01

One process limiting the performance of solar cells is rapid cooling (thermalization) of hot carriers generated by higher-energy solar photons. In principle, the thermalization losses can be reduced by converting the kinetic energy of energetic carriers into additional electron-hole pairs via carrier multiplication (CM). While being inefficient in bulk semiconductors this process is enhanced in quantum dots, although not sufficiently high to considerably boost the power output of practical devices. Here we demonstrate that thick-shell PbSe/CdSe nanostructures can show almost a fourfold increase in the CM yield over conventional PbSe quantum dots, accompanied by a considerable reduction of the CM threshold. These structures enhance a valence-band CM channel due to effective capture of energetic holes into long-lived shell-localized states. The attainment of the regime of slowed cooling responsible for CM enhancement is indicated by the development of shell-related emission in the visible observed simultaneously with infrared emission from the core. PMID:24938462

Luminescence properties of In(Zn)P alloy core/ZnS shell quantum dots

NASA Astrophysics Data System (ADS)

Thuy, Ung Thi Dieu; Reiss, Peter; Liem, Nguyen Quang

2010-11-01

Chemically synthesized InP/ZnS core/shell quantum dots (QDs) are studied using time-resolved photoluminescence spectroscopy and x-ray diffraction. Zinc stearate, which is added during the synthesis of the InP core, significantly improves the optical characteristics of the QDs. The luminescence quantum yield (QY) reaches 60%-70% and the emission is tunable from 485 to 586 nm by varying the Zn2+:In3+ molar ratio and growth temperature. The observed increased Stokes shift, luminescence decay time, and QY in the presence of Zn are rationalized by the formation of an In(Zn)P alloy structure that causes band-edge fluctuation to enhance the confinement of the excited carriers.

Plasmonic enhancement of electroluminescence

NASA Astrophysics Data System (ADS)

Guzatov, D. V.; Gaponenko, S. V.; Demir, H. V.

2018-01-01

Here plasmonic effect specifically on electroluminescence (EL) is studied in terms of radiative and nonradiative decay rates for a dipole near a metal spherical nanoparticle (NP). Contribution from scattering is taken into account and is shown to play a decisive role in EL enhancement owing to pronounced size-dependent radiative decay enhancement and weak size effect on non-radiative counterpart. Unlike photoluminescence where local incident field factor mainly determines the enhancement possibility and level, EL enhancement is only possible by means of quantum yield rise, EL enhancement being feasible only for an intrinsic quantum yield Q0 < 1. The resulting plasmonic effect is independent of intrinsic emitter lifetime but is exclusively defined by the value of Q0, emission spectrum, NP diameter and emitter-metal spacing. For 0.1< Q0 < 0.25, Ag nanoparticles are shown to enhance LED/OLED intensity by several times over the whole visible whereas Au particles feature lower effect within the red-orange range only. Independently of positive effect on quantum yield, metal nanoparticles embedded in an electroluminescent device will improve its efficiency at high currents owing to enhanced overall recombination rate which will diminish manifestation of Auger processes. The latter are believed to be responsible for the known undesirable efficiency droop in semiconductor commercial quantum well based LEDs at higher current. For the same reason plasmonics can diminish quantum dot photodegradation from Auger process induced non-radiative recombination and photoionization thus opening a way to avoid negative Auger effects in emerging colloidal semiconductor LEDs.

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

Luo, Yue; Ahmadi, Ehsaneh D.; Shayan, Kamran

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

Temperature dependence of tris(2,2'-bipyridine) ruthenium (II) device characteristics

NASA Astrophysics Data System (ADS)

Slinker, Jason D.; Malliaras, George G.; Flores-Torres, Samuel; Abruña, Héctor D.; Chunwachirasiri, Withoon; Winokur, Michael J.

2004-04-01

We have investigated the temperature dependence of the current, radiance, and efficiency from electroluminescent devices based on [Ru(bpy)3]2+(PF6-)2, where bpy is 2,2'-bipyridine. We find that the current increases monotonically with temperature from 200 to 380 K, while the radiance reaches a maximum near room temperature. For temperatures greater than room temperature, an irreversible, current-induced degradation occurs with thermal cycling that diminishes both the radiance and the photoluminescence (PL) quantum yield, but does not affect the current. The temperature dependence of the external quantum efficiency is fully accounted for by the dependence of the PL quantum yield as measured from the emissive area of the device. This implies that the contacts remain ohmic throughout the temperature range investigated. The quenching of the PL with temperature was attributed to thermal activation to a nonradiative d-d transition. The temperature dependence of the current shows a complex behavior in which transport appears to be thermally activated, with distinct low-temperature and high-temperature regimes.

Interaction of light with dye-doped calcium phosphate nanoparticles

NASA Astrophysics Data System (ADS)

Russin, Timothy John

In this work we present work on a novel amorphous calcium phosphate nanoparticle system for use in bioimaging and drug delivery applications. The system, by virtue of its synthesis, can be made to encapsulate and protect any number of molecules that are not suitable for biological applications on their own; for example, medication that is poorly soluble in aqueous solution can be encapsulated for delivery, or fragile optical molecules can be encapsulated to protect them from the local environment. We have encapsulated the near-infrared dye indocyanine green, which has beneficial properties for optical imaging (low biotoxicity, absorption and emission at a minimum of tissue absorption). There are two original works presented in this thesis. The first describes the measurement of the quantum yield of the indocyanine green-doped nanoparticles, as well as the development of a theoretical method to extract the molecular quantum yield of a fluorophore encapsulated in a dielectric sphere from effective quantum yield measurements of nanoparticle dispersions in solution. The second work is an application of diffuse scattering theory to the problem of light propagation in biological tissue; specifically, the limits on penetration depth for photodynamic therapy and bioimaging.

Measuring FeO variation using astronomical spectroscopic observations

NASA Astrophysics Data System (ADS)

Unterguggenberger, Stefanie; Noll, Stefan; Feng, Wuhu; Plane, John M. C.; Kausch, Wolfgang; Kimeswenger, Stefan; Jones, Amy; Moehler, Sabine

2017-03-01

Airglow emission lines of OH, O2, O and Na are commonly used to probe the MLT (mesosphere-lower thermosphere) region of the atmosphere. Furthermore, molecules like electronically excited NO, NiO and FeO emit a (pseudo-) continuum. These continua are harder to investigate than atomic emission lines. So far, limb-sounding from space and a small number of ground-based low-to-medium resolution spectra have been used to measure FeO emission in the MLT. In this study the medium-to-high resolution echelle spectrograph X-shooter at the Very Large Telescope (VLT) in the Chilean Atacama Desert (24°37' S, 70°24' W; 2635 m) is used to study the FeO pseudo-continuum in the range from 0.5 to 0.72 µm based on 3662 spectra. Variations of the FeO spectrum itself, as well as the diurnal and seasonal behaviour of the FeO and Na emission intensities, are reported. These airglow emissions are linked by their common origin, meteoric ablation, and they share O3 as a common reactant. Major differences are found in the main emission peak of the FeO airglow spectrum between 0.58 and 0.61 µm, compared with a theoretical spectrum. The FeO and Na airglow intensities exhibit a similar nocturnal variation and a semi-annual seasonal variation with equinoctial maxima. This is satisfactorily reproduced by a whole atmosphere chemistry climate model, if the quantum yields for the reactions of Fe and Na with O3 are 13 ± 3 and 11 ± 2 % respectively. However, a comparison between the modelled O3 in the upper mesosphere and measurements of O3 made with the SABER satellite instrument suggests that these quantum yields may be a factor of ˜ 2 smaller.

Efficient nanosecond photoluminescence from infrared PbS quantum dots coupled to plasmonic nanoantennas

DOE PAGES

Akselrod, Gleb M.; Weidman, Mark C.; Li, Ying; ...

2016-09-13

Infrared (IR) light sources with high modulation rates are critical components for on-chip optical communications. Lead-based colloidal quantum dots are promising nonepitaxial materials for use in IR light-emitting diodes, but their slow photoluminescence lifetime is a serious limitation. Here we demonstrate coupling of PbS quantum dots to colloidal plasmonic nanoantennas based on film-coupled metal nanocubes, resulting in a dramatic 1300-fold reduction in the emission lifetime from the microsecond to the nanosecond regime. This lifetime reduction is primarily due to a 1100-fold increase in the radiative decay rate owing to the high quantum yield (65%) of the antenna. The short emissionmore » lifetime is accompanied by high antenna quantum efficiency and directionality. Lastly, this nonepitaxial platform points toward GHz frequency, electrically modulated, telecommunication wavelength light-emitting diodes and single-photon sources.« less

Nanocrystals of Cesium Lead Halide Perovskites (CsPbX₃, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut.

PubMed

Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I; Krieg, Franziska; Caputo, Riccarda; Hendon, Christopher H; Yang, Ruo Xi; Walsh, Aron; Kovalenko, Maksym V

2015-06-10

Metal halides perovskites, such as hybrid organic-inorganic CH3NH3PbI3, are newcomer optoelectronic materials that have attracted enormous attention as solution-deposited absorbing layers in solar cells with power conversion efficiencies reaching 20%. Herein we demonstrate a new avenue for halide perovskites by designing highly luminescent perovskite-based colloidal quantum dot materials. We have synthesized monodisperse colloidal nanocubes (4-15 nm edge lengths) of fully inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, and I or mixed halide systems Cl/Br and Br/I) using inexpensive commercial precursors. Through compositional modulations and quantum size-effects, the bandgap energies and emission spectra are readily tunable over the entire visible spectral region of 410-700 nm. The photoluminescence of CsPbX3 nanocrystals is characterized by narrow emission line-widths of 12-42 nm, wide color gamut covering up to 140% of the NTSC color standard, high quantum yields of up to 90%, and radiative lifetimes in the range of 1-29 ns. The compelling combination of enhanced optical properties and chemical robustness makes CsPbX3 nanocrystals appealing for optoelectronic applications, particularly for blue and green spectral regions (410-530 nm), where typical metal chalcogenide-based quantum dots suffer from photodegradation.

Emission and Propagation Properties of Midinfrared Quantum Cascade Lasers

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

Krishnaswami, Kannan; Bernacki, Bruce E.; Cannon, Bret D.

2008-02-15

We report divergence, astigmatism and M 2 measurements of quantum cascade lasers (QCL) with an emission wavelength of 8.77 mum. Emission profiles from the QCL facet showed divergence angles of 62° and 32° FWHM ± 2° for the fast and slow axes, respectively. The observation of far field structure superimposed on the fast axes profiles was attributed to the position of the QCL die with respect to the edge of the laser submount, emphasizing the need for careful placement. Two diffraction-limited Germanium aspheric microlenses were designed and fabricated to efficiently collect, collimate, and focus QCL emission. A confocal system comprisedmore » of these lenses was used to measure the beam propagation figure of merit (M2) yielding 1.8 and 1.2 for the fast and slow axes, respectively. Astigmatism at the exit facet was calculated to be about 3.4 mum, or less than half a wave. To the best of our knowledge, this is the first experimental measurement of astigmatism and M 2 reported for mid-IR QCLs.« less

Carbon "Quantum" Dots for Fluorescence Labeling of Cells.

PubMed

Liu, Jia-Hui; Cao, Li; LeCroy, Gregory E; Wang, Ping; Meziani, Mohammed J; Dong, Yiyang; Liu, Yuanfang; Luo, Pengju G; Sun, Ya-Ping

2015-09-02

The specifically synthesized and selected carbon dots of relatively high fluorescence quantum yields were evaluated in their fluorescence labeling of cells. For the cancer cell lines, the cellular uptake of the carbon dots was generally efficient, resulting in the labeling of the cells with bright fluorescence emissions for both one- and two-photon excitations from predominantly the cell membrane and cytoplasm. In the exploration on labeling the live stem cells, the cellular uptake of the carbon dots was relatively less efficient, though fluorescence emissions could still be adequately detected in the labeled cells, with the emissions again predominantly from the cell membrane and cytoplasm. This combined with the observed more efficient internalization of the same carbon dots by the fixed stem cells might suggest some significant selectivity of the stem cells toward surface functionalities of the carbon dots. The needs and possible strategies for more systematic and comparative studies on the fluorescence labeling of different cells, including especially live stem cells, by carbon dots as a new class of brightly fluorescent probes are discussed.

Impact of Site-Directed Mutant Luciferase on Quantitative Green and Orange/Red Emission Intensities in Firefly Bioluminescence

NASA Astrophysics Data System (ADS)

Wang, Yu; Akiyama, Hidefumi; Terakado, Kanako; Nakatsu, Toru

2013-08-01

Firefly bioluminescence has attracted great interest because of its high quantum yield and intriguing modifiable colours. Modifications to the structure of the enzyme luciferase can change the emission colour of firefly bioluminescence, and the mechanism of the colour change has been intensively studied by biochemists, structural biologists, optical physicists, and quantum-chemistry theorists. Here, we report on the quantitative spectra of firefly bioluminescence catalysed by wild-type and four site-directed mutant luciferases. While the mutation caused different emission spectra, the spectra differed only in the intensity of the green component (λmax ~ 560 nm). In contrast, the orange (λmax ~ 610 nm) and red (λmax ~ 650 nm) components present in all the spectra were almost unaffected by the modifications to the luciferases and changes in pH. Our results reveal that the intensity of the green component is the unique factor that is influenced by the luciferase structure and other reaction conditions.

The effects of side-chain-induced disorder on the emission spectra and quantum yields of oligothiophene nano-aggregates. A combined experimental and MD-TDDFT study

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

Hong, Jiyun; Jeon, SuKyung; Kim, Janice J.

2014-07-24

Oligomeric thiophenes are commonly-used components in organic electronics and solar cells. These molecules stack and/or aggregate readily under the processing conditions used to form thin films for these applications, significantly altering their optical and charge-transport properties. To determine how these effects depend on the substitution pattern of the thiophene main chains, nano-aggregates of three sexi-thiophene (6T) oligomers having different alkyl substitution patterns were formed using solvent poisoning techniques and studied using steady-state and time-resolved emission spectroscopy. The results indicate the substantial role played by the side-chain substituents in determining the emissive properties of these species. Both the measured spectral changesmore » and their dependence on substitution are well modeled by combined quantum chemistry and molecular dynamics simulations. The simulations connect the side-chain-induced disorder, which determines the favorable chain packing configurations within the aggregates, with their measured electronic spectra.« less

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

PubMed

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

2013-10-21

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

A simple and facile synthesis of MPA capped CdSe and CdSe/CdS core/shell nanoparticles

NASA Astrophysics Data System (ADS)

Sukanya, D.; Sagayaraj, P.

2015-06-01

II-VI semiconductor nanostructures, in particular, CdSe quantum dots have drawn a lot of attention because of their promising potential applications in biological tagging, photovoltaic, display devices etc. due to their excellent optical properties, high emission quantum yield, size dependent emission wavelength and high photostability. In this paper, we describe the synthesis and properties of mercaptopropionic acid capped CdSe and CdSe/CdS nanoparticles through a simple and efficient co-precipitation method followed by hydrothermal treatment. The growth process, characterization and the optical absorption as a function of wavelength for the synthesized MPA capped CdSe and CdSe/CdS nanoparticles have been determined using X-ray diffraction study (XRD), Ultraviolet-Visible spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR) and High Resolution Transmission Electron Microscopy (HRTEM).

Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects

DOE PAGES

He, Xiaowei; Gifford, Brendan J.; Hartmann, Nicolai F.; ...

2017-09-28

Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. Here, we observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral linemore » width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 ueV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. Our findings point to the tremendous potential of sp3 defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.« less

Low-Temperature Single Carbon Nanotube Spectroscopy of sp 3 Quantum Defects

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

He, Xiaowei; Gifford, Brendan J.; Hartmann, Nicolai F.

Aiming to unravel the relationship between chemical configuration and electronic structure of sp3 defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. Here, we observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000-1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral linemore » width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 ueV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. Our findings point to the tremendous potential of sp3 defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range via use of larger diameter SWCNTs.« less

Solvothermal synthesis of InP quantum dots and their enhanced luminescent efficiency by post-synthetic treatments.

PubMed

Byun, Ho-June; Lee, Ju Chul; Yang, Heesun

2011-03-01

InP quantum dots (QDs) were solvothermally synthesized by using a greener phosphorus source of P(N(CH(3))(2))(3) instead of highly toxic P(TMS)(3) widely used, and subsequently subjected to a size-sorting processing. While as-grown QDs showed an undetectably low emission intensity, post-synthetic treatments such as photo-etching, photo-radiation, and photo-assisted ZnS shell coating gave rise to a substantial increase in emission efficiency due to the effective removal and passivation of surface states. The emission efficiency of the photo-etched QDs was further enhanced by a consecutive UV photo-radiation, attributable to the photo-oxidation at QD surface. Furthermore, a relatively thick ZnS shell on the surface of InP QDs that were surface-modified with hydrophilic ligands beforehand was photochemically generated in an aqueous solution at room temperature. The resulting InP/ZnS core/shell QDs, emitting from blue to red wavelengths, were more efficient than the above photo-treated InP QDs, and their luminescent properties (emission bandwidth and quantum yield) were comparable to those of InP QDs synthesized with P(TMS)(3). Structural, size, and compositional analyses on InP/ZnS QDs were also conducted to elucidate their core/shell structure. Copyright © 2010 Elsevier Inc. All rights reserved.

Fluorescence kinetics of emission from a small finite volume of a biological system

NASA Astrophysics Data System (ADS)

Dagen, A. J.; Alfano, R. R.; Zilinskas, B. A.; Swenberg, C. E.

1985-07-01

The fluorescence decay, apparent quantum yield and transmission from chromophores constrained to a microscopic volume using a single picosecond laser excitation were measured as a function of incident intensity. The β subunit of phycoeryhthrin aggregate isolated from the photosynthetic antenna system of Nostoc sp. was selected since it contains only four chromophores in a volume of less than 5.6×10 4 Å 3. The non-exponential fluorescence decay profiles were intensity independent for the intensity range studied (5 × 10 13 - 2 × 10 15 photon cm -2 per pulse). The apparent decrease in the relative fluorescence quantum yield and increase of the relative transmission with increasing excitation intensity is attributed to the combined effects of ground state depletion and upper excited state absorption. Evidence suggests that exciton annihilation is absent within isolated β subunits.

Optical Control of Fluorescence through plasmonic eigenmode extinction

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

Xu, Xiaoying; Lin, Shih-Che; Li, Quanshui

We introduce the concept of optical control of the fluorescence yield of CdSe quantum dots through plasmon-induced structural changes in random semicontinuous nanostructured gold films. We demonstrate that the wavelength- and polarization dependent coupling between quantum dots and the semicontinuous films, and thus the fluorescent emission spectrum, can be controlled and significantly increased through the optical extinction of a selective band of eigenmodes in the films. This optical method of effecting controlled changes in the metal nanostructure allows for versatile functionality in a single sample and opens a pathway to in situ control over the fluorescence spectrum.

X-ray-induced fluorescent centers formation in zinc- phosphate glasses doped with Ag and Cu ions

NASA Astrophysics Data System (ADS)

Klyukin, D. A.; Pshenova, A. S.; Sidorov, A. I.; Stolyarchuk, M. V.

2016-08-01

Fluorescent properties of silver and copper doped zinc-phosphate glasses were studied. By X-ray irradiation of silver and copper co-doped glasses we could create and identify new emission centers which do not exist in single-doped samples. Doping of the glass with both silver and copper ions leads to the increase of quantum yield by 2.7 times. The study was complemented by quantum chemical calculations using the time-dependent density functional theory. It was shown that fluorescence may be attributed to the formation of mixed Ag-Cu molecular clusters.

Optical Control of Fluorescence through plasmonic eigenmode extinction

DOE PAGES

Xu, Xiaoying; Lin, Shih-Che; Li, Quanshui; ...

2015-04-30

We introduce the concept of optical control of the fluorescence yield of CdSe quantum dots through plasmon-induced structural changes in random semicontinuous nanostructured gold films. We demonstrate that the wavelength- and polarization dependent coupling between quantum dots and the semicontinuous films, and thus the fluorescent emission spectrum, can be controlled and significantly increased through the optical extinction of a selective band of eigenmodes in the films. This optical method of effecting controlled changes in the metal nanostructure allows for versatile functionality in a single sample and opens a pathway to in situ control over the fluorescence spectrum.

Synthesis and Crystal Structure of Highly Strained [4]Cyclofluorene: Green-Emitting Fluorophore.

PubMed

Liu, Yu-Yu; Lin, Jin-Yi; Bo, Yi-Fan; Xie, Ling-Hai; Yi, Ming-Dong; Zhang, Xin-Wen; Zhang, Hong-Mei; Loh, Teck-Peng; Huang, Wei

2016-01-15

[4]Cyclo-9,9-dipropyl-2,7-fluorene ([4]CF) with the strain energy of 79.8 kcal/mol is synthesized in high quantum yield. Impressively, hoop-shaped [4]CF exhibits a green fluorescence emission around 512 nm offering a new explanation for the green band (g-band) in polyfluorenes. The solution-processed [4]CF-based organic light emitting diode (OLED) has also been fabricated with the a stronger green band emission. Strained semiconductors offer a promising approach to fabricating multifunctional optoelectronic materials in organic electronics and biomedicine.

Emission color tuning in AlQ3 complexes with extended conjugated chromophores.

PubMed

Pohl, Radek; Anzenbacher, Pavel

2003-08-07

[reaction: see text] A new method for the synthesis of 5-arylethynyl-8-hydroxyquinoline ligands using Sonogashira-Hagihara coupling was developed. The electronic nature of arylethynyl substituents affects the emission color and quantum yield of the resulting Al(III) complex. Photophysical properties of the metallocomplexes correspond to the electron-withdrawing/-donating character of the arylethynyl substituents. Optical properties of such Al(III) complexes correlate with the Hammett constant values of the respective substituents. This strategy offers a powerful tool for the preparation of electroluminophores with predictable photophysical properties.

Growth patterns of self-assembled InAs quantum dots near the two-dimensional to three-dimensional transition

NASA Astrophysics Data System (ADS)

Colocci, M.; Bogani, F.; Carraresi, L.; Mattolini, R.; Bosacchi, A.; Franchi, S.; Frigeri, P.; Rosa-Clot, M.; Taddei, S.

1997-06-01

Self-assembled InAs quantum dots have been grown by molecular beam epitaxy in such a way as to obtain a continuous variation of InAs coverages across the wafer. Structured photoluminescence spectra are observed after excitation of a large number of dots; deconvolution into Gaussian components yields narrow emission bands (full width at half-maximum 20-30 meV) separated in energy by an average spacing of 30-40 meV. We ascribe the individual bands of the photoluminescence spectra after low excitation to families of dots with similar shapes and with heights differing by one monolayer, as strongly supported by numerical calculations of the fundamental electronic transitions in quantum dot structures.

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

PubMed

Grzyb, Tomasz; Przybylska, Dominika

2018-06-04

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

High Color Rendering Index White-Light Emission from UV-Driven LEDs Based on Single Luminescent Materials: Two-Dimensional Perovskites (C6H5C2H4NH3)2PbBr xCl4- x.

PubMed

Yang, Shuming; Lin, Zhenghuan; Wang, Jingwei; Chen, Yunxiang; Liu, Zhengde; Yang, E; Zhang, Jian; Ling, Qidan

2018-05-09

Two-dimensional (2D) white-light-emitting hybrid perovskites (WHPs) are promising active materials for single-component white-light-emitting diodes (WLEDs) driven by UV. However, the reported WHPs exhibit low quantum yields (≤9%) and low color rendering index (CRI) values less than 85, which does not satisfy the demand of solid-state lighting applications. In this work, we report a series of mixed-halide 2D layered WHPs (C 6 H 5 C 2 H 4 NH 3 ) 2 PbBr x Cl 4- x (0 < x < 4) obtained from the phenethylammonium cation. Unlike the reported WHPs including (C 6 H 5 C 2 H 4 NH 3 ) 2 PbCl 4 , the mixed-halide perovskites display morphology-dependent white emission for the different extents of self-absorption. Additionally, the amount of Br has a huge influence on the photophysical properties of mixed-halide WHPs. With the increasing content of Br, the quantum yields of WHPs increase gradually from 0.2 to 16.9%, accompanied by tunable color temperatures ranging from 4000 K ("warm" white light) to 7000 K ("cold" white light). When applied to the WLEDs, the mixed-halide perovskite powders exhibit tunable white electroluminescent emission with very high CRI of 87-91.

Tailored Emission Properties of ZnTe/ZnTe:O/ZnO Core-Shell Nanowires Coupled with an Al Plasmonic Bowtie Antenna Array.

PubMed

Nie, Kui-Ying; Tu, Xuecou; Li, Jing; Chen, Xuanhu; Ren, Fang-Fang; Zhang, Guo-Gang; Kang, Lin; Gu, Shulin; Zhang, Rong; Wu, Peiheng; Zheng, Youdou; Tan, Hark Hoe; Jagadish, Chennupati; Ye, Jiandong

2018-06-14

The ability to manipulate light-matter interaction in semiconducting nanostructures is fascinating for implementing functionalities in advanced optoelectronic devices. Here, we report the tailoring of radiative emissions in a ZnTe/ZnTe:O/ZnO core-shell single nanowire coupled with a one-dimensional aluminum bowtie antenna array. The plasmonic antenna enables changes in the excitation and emission processes, leading to an obvious enhancement of near band edge emission (2.2 eV) and subgap excitonic emission (1.7 eV) bound to intermediate band states in a ZnTe/ZnTe:O/ZnO core-shell nanowire as well as surface-enhanced Raman scattering at room temperature. The increase of emission decay rate in the nanowire/antenna system, probed by time-resolved photoluminescence spectroscopy, yields an observable enhancement of quantum efficiency induced by local surface plasmon resonance. Electromagnetic simulations agree well with the experimental observations, revealing a combined effect of enhanced electric near-field intensity and the improvement of quantum efficiency in the ZnTe/ZnTe:O/ZnO nanowire/antenna system. The capability of tailoring light-matter interaction in low-efficient emitters may provide an alternative platform for designing advanced optoelectronic and sensing devices with precisely controlled response.

A displaced and low-frequency vibration of phosphorescent state of trans-[Rh(ethylenediamine)2Cl2]PF6 in a range of 5-497 K

NASA Astrophysics Data System (ADS)

Islam, Ashraful; Ikeda, Noriaki; Nozaki, Koichi; Ohno, Takeshi

1998-09-01

The lowest 3(dπ-dσ*) excited states of both cis- and trans-isomers of [Rh(en)2Cl2]X (en=ethylenediamine; X=PF6-, NO3-) and the deuteriated crystal of trans-[Rh(en-d4)2Cl2]PF6 have been investigated in the solid state and in a wide temperature range of 5-497 K by means of emission spectra, lifetime and quantum yield measurements. Emission spectral simulation of trans-[Rh(en)2Cl2]PF6 shows that the emission from the lowest 3(dπ-dσ*) excited state exhibits a progression of a low-frequency metal-chloride stretching vibration (250 cm-1) with a large Huang-Rhys factor (S) of 21 and a progression of a high-frequency N-H stretching vibration (3000 cm-1). The increasing full-width at half maximum (2200 cm-1→4400 cm-1) with increasing temperature (77 K→468 K) is ascribed to hot bands from the excited levels of low-frequency vibration. The luminescence quantum yields of the crystal samples are determined to 0.0008 at 298 K and 0.003 at 80 K for trans-[Rh(en)2Cl2]PF6 and 0.18 at 298 K and 0.40 at 80 K for trans-[Rh(en-d4)2Cl2]PF6. From a combination of lifetime and emission quantum yield measurements, values for kr and knr have been obtained. The observed temperature dependence of nonradiative decay rates of trans-[Rh(en-d4)2Cl2]PF6 in a low-temperature region (<300 K) is possible to reconstitute by using the emission spectral fitting parameters and assuming nuclear tunneling mechanism. The temperature effect and deuteriation effect on the nonradiative rate definitively establishes that the dominant "accepting" modes in the nonradiative transition are a highly displaced (S=21) vibrational mode of low-frequency Cl-Rh-Cl stretching and a weakly displaced (S=0.1) vibrational mode of high-frequency N-D stretching. The nonradiative transition in a high-temperature region occurs via barrier passing along a displaced coordinate of Cl-Rh-Cl vibration with a pre-exponential factor of 1011s-1 and is relatively insensitive to the high-frequency vibrational mode. The crystal of cis-[Rh(en)2Cl2]NO3 shows a red shift of the emission peak energy and an increase in the full-width at half maximum with increasing temperature. The results of temperature-dependent decay and spectra of emission can be interpreted in terms of two 3(dπ-dσ*) emitting states model.

Photoinhibition of Photosystems I and II Using Chlorophyll Fluorescence Measurements

ERIC Educational Resources Information Center

Quiles, Maria Jose

2005-01-01

In this study the photoinhibition of photosystems (PS) I and II caused by exposure to high intensity light in oat ("Avena sativa," var Prevision) is measured by the emission of chlorophyll fluorescence in intact leaves adapted to darkness. The maximal quantum yield of PS II was lower in plants grown under high light intensity than in plants grown…

Thermally activated delayed fluorescence of a Zr-based metal–organic framework

DOE PAGES

Mieno, H.; Kabe, R.; Allendorf, M. D.; ...

2017-12-22

Here, the first metal–organic framework exhibiting thermally activated delayed fluorescence (TADF) was developed. The zirconium-based framework (UiO-68-dpa) uses a newly designed linker composed of a terphenyl backbone, an electron-accepting carboxyl group, and an electron-donating diphenylamine and exhibits green TADF emission with a photoluminescence quantum yield of 30% and high thermal stability.

One-pot synthesis of highly luminescent InP/ZnS nanocrystals without precursor injection.

PubMed

Li, Liang; Reiss, Peter

2008-09-03

InP/ZnS core/shell nanocrystals are prepared using a single-step heating-up method relying on the difference in reactivity of the applied InP and ZnS precursors. The obtained particles exhibit size-dependent emission in the range of 480-590 nm, a fluorescence quantum yield of 50-70%, and high photostability.

Photochemical synthesis and photophysical properties of coumarins bearing extended polyaromatic rings studied by emission and transient absorption measurements.

PubMed

Yamaji, Minoru; Hakoda, Yuma; Okamoto, Hideki; Tani, Fumito

2017-04-12

We prepared a variety of coumarin derivatives having expanded π-electron systems along the direction crossing the C 3 -C 4 bond of the coumarin skeleton via a photochemical cyclization process and investigated their photophysical features as a function of the number (n) of the added benzene rings based on emission and transient absorption measurements. Upon increasing n, the fluorescence quantum yields of the π-extended coumarins increased. Expanding the π-electron system on the C 3 -C 4 bond of the coumarin skeleton was found to be efficient for increasing the fluorescence ability more than that on the C 7 -C 8 bond. Introducing the methoxy group at the 7-position was also efficient for enhancing the fluorescence quantum yield and rate of the expanded coumarins. The non-radiative process from the fluorescence state was not substantially influenced by the expanded π-electron system. The competitive process with the fluorescence was found to be intersystem crossing to the triplet state based on the observations of the triplet-triplet absorption. The effects of the expanded π-electron systems on the fluorescence ability were investigated with the aid of TD-DFT calculations.

Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

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

Zhou, Chenkun; Worku, Michael; Neu, Jennifer

Here, we report the synthesis and characterization of (Ph 4P) 2SbCl 5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph 4P +) and antimony (Sb 3+) chloride salts, (Ph 4P) 2SbCl 5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl 5 2– with strong excited-state structuralmore » distortion. Interestingly, (Ph 4P) 2SbCl 5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.« less

Lead-free/rare earth-free Green-light-emitting crystal based on organic-inorganic hybrid [(C10H16N)2][MnBr4] with high emissive quantum yields and large crystal size

NASA Astrophysics Data System (ADS)

Cai, Xing-Wei; Zhao, Yu-Yuan; Li, Hong; Huang, Cui-Ping; Zhou, Zhen

2018-06-01

With the flourishing development of emitting materials, tremendous technological progress has been accomplished. However, they still face great challenges in convenient economical environmental-friendly large-scale commercial production. Herein we designed this organic-inorganic hybrid lead-free compound, an emerging class of high-efficiency emitting materials, [(C10H16N)2][MnBr4] (1), which emits intense greenish photoluminescence with a high emissive quantum yields of 72.26%, was prepared through the convenient economical solution method. What's more, compared with rare earth fluorescent materials (especially green-emitting Tb), Mn material is rich in natural resources and low commercial cost, which would possess an increasingly predominant advantage in the preparation of luminescent materials. Additionally, the exceptional thermal stability as well as the low-cost/convenient preparation process makes crystal 1 with the large size of more than 1 cm to be an ideal technologically important green-emitting material and it would open up a new route towards the commercialization process of lead-free/rare earth-free hybrid emitting materials in display and sensing.

Facile Preparation of Light Emitting Organic Metal Halide Crystals with Near-Unity Quantum Efficiency

DOE PAGES

Zhou, Chenkun; Worku, Michael; Neu, Jennifer; ...

2018-03-12

Here, we report the synthesis and characterization of (Ph 4P) 2SbCl 5, a novel ionically bonded organic metal halide hybrid with a zero-dimensional (0D) structure at the molecular level. By cocrystallization of tetraphenylphosphonium (Ph 4P +) and antimony (Sb 3+) chloride salts, (Ph 4P) 2SbCl 5 bulk single crystals can be prepared in high yield, which exhibit a highly efficient broadband red emission peaked at 648 nm with a photoluminescence quantum efficiency (PLQE) of around 87%. Density functional theory (DFT) calculations reveal the origin of emission as phosphorescence from the excitons localized at SbCl 5 2– with strong excited-state structuralmore » distortion. Interestingly, (Ph 4P) 2SbCl 5 bulk crystals with a PLQE of around 100% can be prepared via a rapid crystal growth process within minutes, followed by a spontaneous structural transformation. It was found that the rapid growth process yielded a yellow emitting kinetically favored metastable product containing solvent molecules, which turned into the red emitting thermodynamically stable product slowly at room temperature or quickly upon thermal treatment.« less

Color stable white phosphorescent organic light emitting diodes with red emissive electron transport layer

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

Wook Kim, Jin; Yoo, Seung Il; Sung Kang, Jin

2015-06-28

We analyzed the performance of multi-emissive white phosphorescent organic light-emitting diodes (PHOLEDs) in relation to various red emitting sites of hole and electron transport layers (HTL and ETL). The shift of the recombination zone producing stable white emission in PHOLEDs was utilized as luminance was increased with red emission in its electron transport layer. Multi-emissive white PHOLEDs including the red light emitting electron transport layer yielded maximum external quantum efficiency of 17.4% with CIE color coordinates (−0.030, +0.001) shifting only from 1000 to 10 000 cd/m{sup 2}. Additionally, we observed a reduction of energy loss in the white PHOLED via Ir(piq){submore » 3} as phosphorescent red dopant in electron transport layer.« less

Effect of organic materials used in the synthesis on the emission from CdSe quantum dots

NASA Astrophysics Data System (ADS)

Lee, Jae-Won; Yang, Ho-Soon; Hong, K. S.; Kim, S. M.

2013-12-01

Quantum-dot nanocrystals have particular optical properties due to the quantum confinement effect and the surface effect. This study focuses on the effect of surface conditions on the emission from quantum dots. The quantum dots prepared with 1-hexadecylamine (HDA) in the synthesis show strong emission while the quantum dots prepared without HDA show weak emission, as well as emission from surface energy traps. The comparison of the X-ray patterns of these two sets of quantum dots reveals that HDA forms a layer on the surface of quantum dot during the synthesis. This surface passivation with a layer of HDA reduces surface energy traps, therefore the emission from surface trap levels is suppressed in the quantum dots synthesized with HDA.

Metal plasmon-coupled fluorescence imaging and label free coenzyme detection in cells

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

Zhang, Jian, E-mail: jian@cfs.bioment.umaryland.edu; Fu, Yi; Li, Ge

2012-08-31

Highlights: Black-Right-Pointing-Pointer Metal nanoparticle for fluorescence cell imaging. Black-Right-Pointing-Pointer Non-invasive emission detection of coenzyme in cell on time-resolved confocal microscope. Black-Right-Pointing-Pointer Near-field interaction of flavin adenine dinucleotide with silver substrate. Black-Right-Pointing-Pointer Isolation of emissions by coenzymes from cellular autofluorescence on fluorescence cell imaging. -- Abstract: Flavin adenine dinucleotide (FAD) is a key metabolite in cellular energy conversion. Flavin can also bind with some enzymes in the metabolic pathway and the binding sites may be changed due to the disease progression. Thus, there is interest on studying its expression level, distribution, and redox state within the cells. FAD is naturally fluorescent,more » but it has a modest extinction coefficient and quantum yield. Hence the intrinsic emission from FAD is generally too weak to be isolated distinctly from the cellular backgrounds in fluorescence cell imaging. In this article, the metal nanostructures on the glass coverslips were used as substrates to measure FAD in cells. Particulate silver films were fabricated with an optical resonance near the absorption and the emission wavelengths of FAD which can lead to efficient coupling interactions. As a result, the emission intensity and quantum yield by FAD were greatly increased and the lifetime was dramatically shortened resulting in less interference from the longer lived cellular background. This feature may overcome the technical limits that hinder the direct observation of intrinsically fluorescent coenzymes in the cells by fluorescence microscopy. Fluorescence cell imaging on the metallic particle substrates may provide a non-invasive strategy for collecting the information of coenzymes in cells.« less

Red carbon dots-based phosphors for white light-emitting diodes with color rendering index of 92.

PubMed

Zhai, Yuechen; Wang, Yi; Li, Di; Zhou, Ding; Jing, Pengtao; Shen, Dezhen; Qu, Songnan

2018-05-29

Exploration of solid-state efficient red emissive carbon dots (CDs) phosphors is strongly desired for the development of high performance CDs-based white light-emitting diodes (WLEDs). In this work, enhanced red emissive CDs-based phosphors with photoluminescence quantum yields (PLQYs) of 25% were prepared by embedding red emissive CDs (PLQYs of 23%) into polyvinyl pyrrolidone (PVP). Because of the protection of PVP, the phosphors could preserve strong luminescence under long-term UV excitation or being mixed with conventional packaging materials. By applying the red emissive phosphors as the color conversion layer, WLEDs with high color rendering index of 92 and color coordinate of (0.33, 0.33) are fabricated. Copyright © 2018 Elsevier Inc. All rights reserved.

Utilization of solvothermally grown InP/ZnS quantum dots as wavelength converters for fabrication of white light-emitting diodes.

PubMed

Jang, Eun-Pyo; Yang, Heesun

2013-09-01

This work reports on a simple solvothermal synthesis of InP/ZnS core/shell quantum dots (QDs) using a much safer and cheaper phosphorus precursor of tris(dimethylamino)phosphine than the most popularly chosen tris(trimethylsilyl)phosphine. The band gap of InP QDs is facilely controlled by varying the solvothermal core growth time (4 vs. 6 h) with a fixed temperature of 150 degrees C, and the successive solvothermal ZnS shelling at 220 degrees C for 6 h results in green- and yellow-emtting InP/ZnS QD with emission quantum yield of 41-42%. The broad size distribution of as-synthesized InP/ZnS QDs, which appears to be inherent in the current solvothermal approach, is improved by a size-selective sorting procedure, and the emission properties of the resulting size-sorted QD fractions are investigated. To produce white emission for general lighting source, a blue light-emitting diode (LED) is combined with non-size-soroted green or yellow QDs as wavelength converters. Furthermore, the QD-LED that includes a blend of green and yellow QDs is fabricated to generate a white lighting source with an enhanced color rendering performance, and its electroluminescent properties are characterized in detail.

Synthesis, luminescence, and energy-transfer properties of β-Na2Ca4(PO4)2(SiO4):A (A = Eu(2+), Dy(3+), Ce(3+)/Tb(3+)) phosphors.

PubMed

Li, Kai; Shang, Mengmeng; Geng, Dongling; Lian, Hongzhou; Zhang, Yang; Fan, Jian; Lin, Jun

2014-07-07

A series of β-Na2Ca4(PO4)2(SiO4) (β-NCPS):A (A = Eu(2+), Dy(3+), Ce(3+)/Tb(3+)) phosphors were prepared via a high-temperature solid-state reaction route. The X-ray diffraction, Fourier transform infrared, photoluminescence (PL), cathodoluminescence (CL) properties, fluorescent lifetimes, and absolute quantum yield were exploited to characterize the samples. Under UV radiation, the β-NCPS:Eu(2+) phosphors present bright green emissions, and the β-NCPS:Ce(3+) phosphors show strong blue emissions, which are attributed to their 4f(6)5d(1) → 4f(7) and 5d-4f allowed transitions, respectively. The β-NCPS:Ce(3+), Tb(3+) phosphors display intense tunable color from blue to green and high absolute quantum yields (81% for β-NCPS:0.12Ce(3+) and 83% for β-NCPS:0.12Ce(3+), 0.08Tb(3+)) when excited at 365 nm. Simultaneously, the energy transfer from Ce(3+) to Tb(3+) ions is deduced from the spectral overlap between Ce(3+) emission and Tb(3+) excitation spectra and demonstrated by the change of emission spectra and decay lifetimes. Moreover, the energy-transfer mechanism from Ce(3+) to Tb(3+) ions is confirmed to be exchange interaction according to the discussion of expression from Dexter and Reisfeld. Under a low-voltage electron-beam excitation, the β-NCPS:A (A = Eu(2+), Dy(3+), Ce(3+)/Tb(3+)) phosphors exhibit their characteristic emissions, and the emission profiles of β-NCPS:Ce(3+),Tb(3+) phosphors are obviously different from those of the PL spectra; this difference might be ascribed to their different luminescence mechanisms. These results in PL and CL properties suggest that β-NCPS:A (A = Eu(2+), Dy(3+), Ce(3+)/Tb(3+)) phosphors are potential candidates for solid-state lighting and field-emission displays.

Photoluminescence spectroscopy and the effective mass theory of strained (In,Ga)As/GaAs heterostructures grown on (112)B GaAs substrates

NASA Technical Reports Server (NTRS)

Henderson, R. H.; Sun, D.; Towe, E.

1995-01-01

The photoluminescence characteristics of pseudomorphic In(0.19)Ga(0.81)As/GaAs quantum well structures grown on both the conventional (001) and the unconventional (112)B GaAs substrate are investigated. It is found that the emission spectra of the structures grown on the (112)B surface exhibit some spectral characteristics not observed on similar structures grown on the (001) surface. A spectral blue shift of the e yields hh1 transition with increasing optical pump intensity is observed for the quantum wells on the (112) surface. This shift is interpreted to be evidence of a strain-induced piezoelectric field. A second spectral feature located within the band gap of the In(0.19)Ga(0.81)As layer is also observed for the (112) structure; this feature is thought to be an impurity-related emission. The expected transition energies of the quantum well structures are calculated using the effective mass theory based on the 4 x 4 Luttinger valence band Hamiltonian, and related strain Hamiltonian.

Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect

NASA Astrophysics Data System (ADS)

Park, Kyoung-Duck; Jiang, Tao; Clark, Genevieve; Xu, Xiaodong; Raschke, Markus B.

2018-01-01

Excitons, Coulomb-bound electron-hole pairs, are elementary photo-excitations in semiconductors that can couple to light through radiative relaxation. In contrast, dark excitons (XD) show anti-parallel spin configuration with generally forbidden radiative emission. Because of their long lifetimes, these dark excitons are appealing candidates for quantum computing and optoelectronics. However, optical read-out and control of XD states has remained challenging due to their decoupling from light. Here, we present a tip-enhanced nano-optical approach to induce, switch and programmably modulate the XD emission at room temperature. Using a monolayer transition metal dichalcogenide (TMD) WSe2 on a gold substrate, we demonstrate 6 × 105-fold enhancement in dark exciton photoluminescence quantum yield achieved through coupling of the antenna-tip to the dark exciton out-of-plane optical dipole moment, with a large Purcell factor of ≥2 × 103 of the tip-sample nano-cavity. Our approach provides a facile way to harness excitonic properties in low-dimensional semiconductors offering new strategies for quantum optoelectronics.

Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect.

PubMed

Park, Kyoung-Duck; Jiang, Tao; Clark, Genevieve; Xu, Xiaodong; Raschke, Markus B

2018-01-01

Excitons, Coulomb-bound electron-hole pairs, are elementary photo-excitations in semiconductors that can couple to light through radiative relaxation. In contrast, dark excitons (X D ) show anti-parallel spin configuration with generally forbidden radiative emission. Because of their long lifetimes, these dark excitons are appealing candidates for quantum computing and optoelectronics. However, optical read-out and control of X D states has remained challenging due to their decoupling from light. Here, we present a tip-enhanced nano-optical approach to induce, switch and programmably modulate the X D emission at room temperature. Using a monolayer transition metal dichalcogenide (TMD) WSe 2 on a gold substrate, we demonstrate ~6 × 10 5 -fold enhancement in dark exciton photoluminescence quantum yield achieved through coupling of the antenna-tip to the dark exciton out-of-plane optical dipole moment, with a large Purcell factor of ≥2 × 10 3 of the tip-sample nano-cavity. Our approach provides a facile way to harness excitonic properties in low-dimensional semiconductors offering new strategies for quantum optoelectronics.

Non-blinking (Zn)CuInS/ZnS Quantum Dots Prepared by In Situ Interfacial Alloying Approach

PubMed Central

Zhang, Aidi; Dong, Chaoqing; Li, Liang; Yin, Jinjin; Liu, Heng; Huang, Xiangyi; Ren, Jicun

2015-01-01

Semiconductor quantum dots (QDs) are very important optical nanomaterials with a wide range of potential applications. However, blinking behavior of single QD is an intrinsic drawback for some biological and photoelectric applications based on single-particle emission. Herein we present a rational strategy for fabrication of non-blinking (Zn)CuInS/ZnS QDs in organic phase through in situ interfacial alloying approach. This new strategy includes three steps: synthesis of CuInS QDs, eliminating the interior traps of QDs by forming graded (Zn)CuInS alloyed QDs, modifying the surface traps of QDs by introducing ZnS shells onto (Zn)CuInS QDs using alkylthiols as sulfur source and surface ligands. The suppressed blinking mechanism was mainly attributed to modifying QDs traps from interior to exterior via a step-by-step modification. Non-blinking QDs show high quantum yield, symmetric emission spectra and excellent crystallinity, and will enable applications from biology to optoelectronics that were previously hindered by blinking behavior of traditional QDs. PMID:26458511

Highly Sensitive Detection of Glucose by a "Turn-Off-On" Fluorescent Probe Using Gadolinium-Doped Carbon Dots and Carbon Microparticles.

PubMed

Hu, Meixin; Qi, Jianrong; Ruan, Jing; Shen, Guangxia

2018-06-01

Carbon dots, as a potential substitute for semiconductor quantum dots, have drawn great interest in recent years. The preparation of fluorescent carbon dots has been made easy with many significant advances, but the complicated purifying processes, low quantum yield, and blue emission wavelength still limit its wider application in biosensors, biomedicine, and photonic devices. Here we report a strategy to synthesis Gd-doped carbon dots (Gd-Cdots) of super-high quantum yield with a microwave assisted hydrothermal method. The Gd-Cdots, with a diameter of 47∼8 nm, can be purified easily with conventional centrifugal techniques. Carbon microparticles (CMPs) have also been synthesized with a similar procedure. Meanwhile, we demonstrated a novel "turn-off-on" fluorescent biosensor, which has been developed for highly sensitive detection of glucose using Gd-doped carbon dots as probes. The proposed biosensor has exhibited low-cost and non-toxic properties, with high sensitivity and good specificity. In addition, the results in real blood samples further confirmed it as a promising application in diabetes diagnosis.

Bright conjugated polymer nanoparticles containing a biodegradable shell produced at high yields and with tuneable optical properties by a scalable microfluidic device.

PubMed

Abelha, T F; Phillips, T W; Bannock, J H; Nightingale, A M; Dreiss, C A; Kemal, E; Urbano, L; deMello, J C; Green, M; Dailey, L A

2017-02-02

This study compares the performance of a microfluidic technique and a conventional bulk method to manufacture conjugated polymer nanoparticles (CPNs) embedded within a biodegradable poly(ethylene glycol) methyl ether-block-poly(lactide-co-glycolide) (PEG 5K -PLGA 55K ) matrix. The influence of PEG 5K -PLGA 55K and conjugated polymers cyano-substituted poly(p-phenylene vinylene) (CN-PPV) and poly(9,9-dioctylfluorene-2,1,3-benzothiadiazole) (F8BT) on the physicochemical properties of the CPNs was also evaluated. Both techniques enabled CPN production with high end product yields (∼70-95%). However, while the bulk technique (solvent displacement) under optimal conditions generated small nanoparticles (∼70-100 nm) with similar optical properties (quantum yields ∼35%), the microfluidic approach produced larger CPNs (140-260 nm) with significantly superior quantum yields (49-55%) and tailored emission spectra. CPNs containing CN-PPV showed smaller size distributions and tuneable emission spectra compared to F8BT systems prepared under the same conditions. The presence of PEG 5K -PLGA 55K did not affect the size or optical properties of the CPNs and provided a neutral net electric charge as is often required for biomedical applications. The microfluidics flow-based device was successfully used for the continuous preparation of CPNs over a 24 hour period. On the basis of the results presented here, it can be concluded that the microfluidic device used in this study can be used to optimize the production of bright CPNs with tailored properties with good reproducibility.

Decoherence by spontaneous emission: A single-atom analog of superradiance

NASA Astrophysics Data System (ADS)

Souza, Reinaldo de Melo e.; Impens, François; Neto, Paulo A. Maia

2016-12-01

We show that the decoherence of the atomic center-of-mass induced by spontaneous emission involves interferences corresponding to a single-atom analog of superradiance. We use a decomposition of the stationary decoherence rate as a sum of local and nonlocal contributions obtained to second order in the interaction by the influence functional method. These terms are respectively related to the strength of the coupling between system and environment, and to the quality of the information about the system leaking into the environment. While the local contribution always yields a positive decoherence rate, the nonlocal one may lead to recoherence when only partial information about the system is obtained from the disturbed environment. The nonlocal contribution contains interferences between different quantum amplitudes leading to oscillations of the decoherence rate reminiscent of superradiance. These concepts, illustrated here in the framework of atom interferometry within a trap, may be applied to a variety of quantum systems.

Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

DOE PAGES

Yan, Yong; Crisp, Ryan W.; Gu, Jing; ...

2017-04-03

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QDmore » photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.« less

Photochemical and Photophysical Properties of Phthalocyanines Modified with Optically Active Alcohols.

PubMed

Ramos, Aline A; Nascimento, Francisco B; de Souza, Thaiza F M; Omori, Alvaro T; Manieri, Tânia M; Cerchiaro, Giselle; Ribeiro, Anderson O

2015-07-24

Three phthalocyanine derivatives were synthesized and characterized: one modified with a racemic mixture of 1-(4-bromophenyl)ethanol and two other macrocycles modified with each one of the enantioenriched isomers (R)-1-(4-bromophenyl)ethanol and (S)-1-(4-bromophenyl)ethanol. The compounds were characterized by 1H-NMR spectroscopy, mass spectrometry, UV-Vis absorption, and excitation and emission spectra. Additionally, partition coefficient values and the quantum yield of the generation of oxygen reactive species were determined. Interestingly, the phthalocyanine containing a (R)-1-(4-bromophenyl)ethoxy moiety showed higher quantum yield of reactive oxygen species generation than other compounds under the same conditions. In addition, the obtained fluorescence microscopy and cell viability results have shown that these phthalocyanines have different interactions with mammary MCF-7 cells. Therefore, our results indicate that the photochemical and biological properties of phthalocyanines with chiral ligands should be evaluated separately for each enantiomeric species.

Kinetics of bacterial fluorescence staining with 3,3'-diethylthiacyanine.

PubMed

Thomas, Marlon S; Nuñez, Vicente; Upadhyayula, Srigokul; Zielins, Elizabeth R; Bao, Duoduo; Vasquez, Jacob M; Bahmani, Baharak; Vullev, Valentine I

2010-06-15

For more than a century, colorimetric and fluorescence staining have been the foundation of a broad range of key bioanalytical techniques. The dynamics of such staining processes, however, still remains largely unexplored. We investigated the kinetics of fluorescence staining of two gram-negative and two gram-positive species with 3,3'-diethylthiacyanine (THIA) iodide. An increase in the THIA fluorescence quantum yield, induced by the bacterial dye uptake, was the principal reason for the observed emission enhancement. The fluorescence quantum yield of THIA depended on the media viscosity and not on the media polarity, which suggested that the microenvironment of the dye molecules taken up by the cells was restrictive. The kinetics of fluorescence staining did not manifest a statistically significant dependence neither on the dye concentration, nor on the cell count. In the presence of surfactant additives, however, the fluorescence-enhancement kinetic patterns manifested species specificity with statistically significant discernibility.

Ultrafast Room-Temperature Single Photon Emission from Quantum Dots Coupled to Plasmonic Nanocavities.

PubMed

Hoang, Thang B; Akselrod, Gleb M; Mikkelsen, Maiken H

2016-01-13

Efficient and bright single photon sources at room temperature are critical components for quantum information systems such as quantum key distribution, quantum state teleportation, and quantum computation. However, the intrinsic radiative lifetime of quantum emitters is typically ∼10 ns, which severely limits the maximum single photon emission rate and thus entanglement rates. Here, we demonstrate the regime of ultrafast spontaneous emission (∼10 ps) from a single quantum emitter coupled to a plasmonic nanocavity at room temperature. The nanocavity integrated with a single colloidal semiconductor quantum dot produces a 540-fold decrease in the emission lifetime and a simultaneous 1900-fold increase in the total emission intensity. At the same time, the nanocavity acts as a highly efficient optical antenna directing the emission into a single lobe normal to the surface. This plasmonic platform is a versatile geometry into which a variety of other quantum emitters, such as crystal color centers, can be integrated for directional, room-temperature single photon emission rates exceeding 80 GHz.

Achieving deep-red-to-near-infrared emissions in Sn-doped Cu-In-S/ZnS quantum dots for red-enhanced white LEDs and near-infrared LEDs.

PubMed

Chen, Jixin; Li, Ye; Wang, Le; Zhou, Tianliang; Xie, Rong-Jun

2018-05-16

Semiconductor quantum dots (QDs) are promising luminescent materials for use in lighting, display and bio-imaging, and the color tuning is a necessity for such applications. In this work, we report tunable colors and deep-red or near infrared (NIR) emissions in Cu-In-S and Cu-In-S/ZnS QDs by incorporating Sn. These QDs (with a size of 5 nm) with varying Sn concentrations and/or Cu/In ratios were synthesized by a non-injection method, and characterized by a variety of analytical techniques (i.e., XRD, TEM, XPS, absorption, photoluminescence, decay time, etc.). The Cu-Sn-In-S and Cu-Sn-In-S/ZnS QDs with Cu/In = 1/2 show the emission maximum in the ranges of 701-894 nm and 628-785 nm, respectively. The red-shift in emission is ascribed to the decrease of the band gap with the Sn doping. The highest quantum yield of 75% is achieved in Cu-Sn-In-S/ZnS with 0.1 mmol Sn and Cu/In = 1/2. Both the white and NIR LEDs were fabricated by using Cu-Sn-In-S/ZnS QDs and a 365 nm LED chip. The white LED exhibits superhigh color rendering indices of Ra = 97.2 and R9 = 91 and a warm color temperature of 2700 K. And the NIR LED shows an interesting broadband near-infrared emission centered at 741 nm, allowing for applications in optical communication, sensing and medical devices.

Red-luminescence band: A tool for the quality assessment of germanium and silicon nanocrystals

NASA Astrophysics Data System (ADS)

Fraj, I.; Favre, L.; David, T.; Abbarchi, M.; Liu, K.; Claude, J. B.; Ronda, A.; Naffouti, M.; Saidi, F.; Hassen, F.; Maaref, H.; Aqua, J. N.; Berbezier, I.

2017-10-01

We present the photoluminescence (PL) emission of Silicon and Germanium nanocrystals (NCs) of different sizes embedded in two different matrices. Formation of the NCs is achieved via solid-state dewetting during annealing in a molecular beam epitaxy ultra-high vacuum system of ultrathin amorphous Si and Ge layers deposited at room temperature on SiO2. During the dewetting process, the bi-dimensional amorphous layers transform into small pseudo-spherical islands whose mean size can be tuned directly with the deposited thickness. The nanocrystals are capped either ex situ by silicon dioxide or in situ by amorphous Silicon. The surface-state dependent emission (typically in the range 1.74 eV-1.79 eV) exhibited higher relative PL quantum yields compared to the emission originating from the band gap transition. This red-PL emission comes from the radiative transitions between a Si band and an interface level. It is mainly ascribed to the NCs and environment features deduced from morphological and structural analyses. Power dependent analysis of the photoluminescence intensity under continuous excitation reveals a conventional power law with an exponent close to 1, in agreement with the type II nature of the emission. We show that Ge-NCs exhibit much lower quantum efficiency than Si-NCs due to non-radiative interface states. Low quantum efficiency is also obtained when NCs have been exposed to air before capping, even if the exposure time is very short. Our results indicate that a reduction of the non-radiative surface states is a key strategy step in producing small NCs with increased PL emission for a variety of applications. The red-PL band is then an effective tool for the quality assessment of NCs based structures.

Study of absorption and re-emission processes in a ternary liquid scintillation system

NASA Astrophysics Data System (ADS)

Xiao, Hua-Lin; Li, Xiao-Bo; Zheng, Dong; Cao, Jun; Wen, Liang-Jian; Wang, Nai-Yan

2010-11-01

Liquid scintillators are widely used as the neutrino target in neutrino experiments. The absorption and emission of different components of a ternary liquid scintillator (Linear Alkyl Benzene (LAB) as the solvent, 2,5-diphenyloxazole (PPO) as the fluor and p-bis-(o-methylstyryl)-benzene (bis-MSB) as wavelength shifter) are studied. It is shown that the absorption of this liquid scintillator is dominant by LAB and PPO at wavelengths less than 349 nm, and the absorption by bis-MSB becomes prevalent at the wavelength larger than 349 nm. The fluorescence quantum yields, which are the key parameters to model the absorption and re-emission processes in large liquid scintillation detectors, are measured.

InP/ZnSe/ZnS core-multishell quantum dots for improved luminescence efficiency

NASA Astrophysics Data System (ADS)

Greco, Tonino; Ippen, Christian; Wedel, Armin

2012-04-01

Semiconductor quantum dots (QDs) exhibit unique optical properties like size-tunable emission color, narrow emission peak, and high luminescence efficiency. QDs are therefore investigated towards their application in light-emitting devices (QLEDs), solar cells, and for bio-imaging purposes. In most cases QDs made from cadmium compounds like CdS, CdSe or CdTe are studied because of their facile and reliable synthesis. However, due to the toxicity of Cd compounds and the corresponding regulation (e.g. RoHS directive in Europe) these materials are not feasible for customer applications. Indium phosphide is considered to be the most promising alternative because of the similar band gap (InP 1.35 eV, CdSe 1.73 eV). InP QDs do not yet reach the quality of CdSe QDs, especially in terms of photoluminescence quantum yield and peak width. Typically, QDs are coated with another semiconductor material of wider band gap, often ZnS, to passivate surface defects and thus improve luminescence efficiency. Concerning CdSe QDs, multishell coatings like CdSe/CdS/ZnS or CdSe/ZnSe/ZnS have been shown to be advantageous due to the improved compatibility of lattice constants. Here we present a method to improve the luminescence efficiency of InP QDs by coating a ZnSe/ZnS multishell instead of a ZnS single shell. ZnSe exhibits an intermediate lattice constant of 5.67 Å between those of InP (5.87 Å) and ZnS (5.41 Å) and thus acts as a wetting layer. As a result, InP/ZnSe/ZnS is introduced as a new core-shell quantum dot material which shows improved photoluminescence quantum yield (up to 75 %) compared to the conventional InP/ZnS system.

Size-controlled synthesis of ZnO quantum dots in microreactors

NASA Astrophysics Data System (ADS)

Schejn, Aleksandra; Frégnaux, Mathieu; Commenge, Jean-Marc; Balan, Lavinia; Falk, Laurent; Schneider, Raphaël

2014-04-01

In this paper, we report on a continuous-flow microreactor process to prepare ZnO quantum dots (QDs) with widely tunable particle size and photoluminescence emission wavelengths. X-ray diffraction, electron diffraction, UV-vis, photoluminescence and transmission electron microscopy measurements were used to characterize the synthesized ZnO QDs. By varying operating conditions (temperature, flow rate) or the capping ligand, ZnO QDs with diameters ranging from 3.6 to 5.2 nm and fluorescence maxima from 500 to 560 nm were prepared. Results obtained show that low reaction temperatures (20 or 35 °C), high flow rates and the use of propionic acid as a stabilizing agent are favorable for the production of ZnO QDs with high photoluminescence quantum yields (up to 30%).

One-pot synthesis of polythiol ligand for highly bright and stable hydrophilic quantum dots toward bioconjugate formation

NASA Astrophysics Data System (ADS)

Dezhurov, Sergey V.; Krylsky, Dmitry V.; Rybakova, Anastasia V.; Ibragimova, Sagila A.; Gladyshev, Pavel P.; Vasiliev, Alexey A.; Morenkov, Oleg S.

2018-03-01

A fast and efficient one-pot synthesis of thiol-terminated poly(vinylpirrolidone-co-maleic anhydride-co-ethylene glycol dimethacrylate) based heterobifunctional polymer (PTVP) has been developed. The polymer was used for the modification of quantum dots (QDs) to prepare water soluble and stable QDs with emission quantum yield as high as 80%. Using carbodiimide method, PTVP-capped red light-emitting QDs were conjugated to model monoclonal antibodies specific to glycoprotein B (gB) of Aujeszky’s disease virus (ADV) and successfully used in the lateral flow assay (LFA) for the detection of ADV gB in biological fluids. A comparative analysis of the sensitivity of the method was carried out using three types of QDs emitting in the red and far-red region.

Room-temperature processing of CdSe quantum dots with tunable sizes

NASA Astrophysics Data System (ADS)

Joo, So-Yeong; Jeong, Da-Woon; Lee, Chan-Gi; Kim, Bum-Sung; Park, Hyun-Su; Kim, Woo-Byoung

2017-06-01

In this work, CdSe quantum dots (QDs) with tunable sizes have been fabricated via photo-induced chemical etching at room temperature, and the related reaction mechanism was investigated. The surface of QDs was oxidized by the holes generated through photon irradiation of oxygen species, and the obtained oxide layer was dissolved in an aqueous solution of 3-amino-1-propanol (APOL) with an APOL:H2O volume ratio of 5:1. The generated electrons promoted QD surface interactions with amino groups, which ultimately passivated surface defects. The absorption and photoluminescence emission peaks of the produced QDs were clearly blue-shifted about 26 nm with increasing time, and the resulting quantum yield for an 8 h etched sample was increased from 20% to 26%, as compared to the initial sample.

Cadmium-containing quantum dots: properties, applications, and toxicity.

PubMed

Mo, Dan; Hu, Liang; Zeng, Guangming; Chen, Guiqiu; Wan, Jia; Yu, Zhigang; Huang, Zhenzhen; He, Kai; Zhang, Chen; Cheng, Min

2017-04-01

The marriage of biology with nanomaterials has significantly accelerated advancement of biological techniques, profoundly facilitating practical applications in biomedical fields. With unique optical properties (e.g., tunable broad excitation, narrow emission spectra, robust photostability, and high quantum yield), fluorescent quantum dots (QDs) have been reasonably functionalized with controllable interfaces and extensively used as a new class of optical probe in biological researches. In this review, we summarize the recent progress in synthesis and properties of QDs. Moreover, we provide an overview of the outstanding potential of QDs for biomedical research and innovative methods of drug delivery. Specifically, the applications of QDs as novel fluorescent nanomaterials for biomedical sensing and imaging have been detailedly highlighted and discussed. In addition, recent concerns on potential toxicity of QDs are also introduced, ranging from cell researches to animal models.

Tuning of the emission color of organic light emitting diodes via smartly designed aluminum plasmonics

NASA Astrophysics Data System (ADS)

Auer-Berger, Manuel; Tretnak, Veronika; Wenzl, Franz-Peter; Krenn, Joachim; List-Kratochvil, Emil J. W.

2017-02-01

With the invention of phosphorescent emitter material, organic light emitting diodes with internal quantum yields of up to 100% can be realized. Still, the extraction of the light from the OLED stack is a bottleneck, which hampers the availability of OLEDs with large external quantum efficiencies. In this contribution, we highlight the advantages of integrating aluminum nanodisc arrays into the OLED stack. By this, not only the out-coupling of light can be enhanced, but also the emission color can be tailored and controlled. By means of extinction- and fluorescence spectroscopy measurements we are able to show how the sharp features observed in the extinction measurements correlate with a very selective fluorescence enhancement of the organic emitter materials used in these studies. At the same time, localized surface plasmon resonances of the individual nanodiscs further modify the emission spectrum, e.g., by filtering the green emission tail. A combination of these factors leads to a modification of the emission color in between CIE1931 (x,y) chromaticity coordinates of (0.149, 0.225) and (0.152, 0.352). After accounting for the sensitivity of the human eye, we are able to demonstrate that this adjustment of the chromaticity coordinates goes is accompanied by an increase in device efficiency.

Dual emissive manganese and copper Co-doped Zn-In-S quantum dots as a single color-converter for high color rendering white-light-emitting diodes.

PubMed

Yuan, Xi; Ma, Ruixin; Zhang, Wenjin; Hua, Jie; Meng, Xiangdong; Zhong, Xinhua; Zhang, Jiahua; Zhao, Jialong; Li, Haibo

2015-04-29

Novel white light emitting diodes (LEDs) with environmentally friendly dual emissive quantum dots (QDs) as single color-converters are one of the most promising high-quality solid-state lighting sources for meeting the growing global demand for resource sustainability. A facile method was developed for the synthesis of the bright green-red-emitting Mn and Cu codoped Zn-In-S QDs with an absorption bangdgap of 2.56 eV (485 nm), a large Stokes shift of 150 nm, and high emission quantum yield up to 75%, which were suitable for warm white LEDs based on blue GaN chips. The wide photoluminescence (PL) spectra composed of Cu-related green and Mn-related red emissions in the codoped QDs could be controlled by varying the doping concentrations of Mn and Cu ions. The energy transfer processes in Mn and Cu codoped QDs were proposed on the basis of the changes in PL intensity and lifetime measured by means of steady-state and time-resolved PL spectra. By integrating these bicolor QDs with commercial GaN-based blue LEDs, the as-fabricated tricolor white LEDs showed bright natural white light with a color rendering index of 95, luminous efficacy of 73.2 lm/W, and color temperature of 5092 K. These results indicated that (Mn,Cu):Zn-In-S/ZnS QDs could be used as a single color-converting material for the next generation of solid-state lighting.

Two-step narrow ridge cascade diode lasers emitting near $$2~\\mu$$ m

DOE PAGES

Feng, Tao; Hosoda, Takashi; Shterengas, Leon; ...

2017-01-02

Nearly diffraction limited GaSb-based type-I quantum well cascade diode lasers emitting in the spectral region 1.95-2 μm were designed and fabricated. Two-step 5.5-μm-wide shallow and 14-μm-wide deep etched ridge waveguide design yielded devices generating stable single lobe beams with 250 mW of continuous wave output power at 20 °C. Quantum well radiative recombination current contributes about 13% to laser threshold as estimated from true spontaneous emission and modal gain analysis. Here, recombination at etched sidewalls of the 14-μmwide deep ridges controls about 30% of the threshold.

Dual-excitation upconverting nanoparticle and quantum dot aptasensor for multiplexed food pathogen detection.

PubMed

Kurt, Hasan; Yüce, Meral; Hussain, Babar; Budak, Hikmet

2016-07-15

In this report, a dual-excitation sensing method was developed using aptamer-functionalized quantum dots and upconverting nanoparticles, exhibiting Stokes and anti-Stokes type excitation profiles, respectively. Conjugation of the aptamer-functionalized luminescent nanoparticles with the magnetic beads, comprising short DNA sequences that were partially complementary to the aptamer sequences, enabled facile separation of the analyte-free conjugates for fluorescent measurement. UV-Visible spectroscopy, Circular Dichroism spectroscopy, Dynamic Light Scattering and Polyacrylamide Gel Electrophoresis techniques were used to characterize the aptamer probes developed. The target-specific luminescent conjugates were applied for multiplex detection of model food pathogens, Salmonella typhimurium, and Staphylococcus aureus, in which the fluorescent emission spectra were obtained under UV excitation at 325nm for quantum dots and NIR excitation at 980nm for upconverting nanoparticles, respectively. The dual-excitation strategy was aimed to minimize cross-talk between the luminescent signals for multiplexed detection, and yielded limit of detection values of 16 and 28cfumL(-1) for Staphylococcus aureus, and Salmonella typhimurium, respectively. By employing a greater number of quantum dots and upconverting nanoparticles with non-overlapping fluorescent emissions, the proposed methodology might be exploited further to detect several analytes, simultaneously. Copyright © 2016 Elsevier B.V. All rights reserved.

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications

PubMed Central

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-01-01

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided. PMID:28788080

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications.

PubMed

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-07-28

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided.

Temporal switching of homo-FRET pathways in single-chromophore dimer models of π-conjugated polymers.

PubMed

Stangl, Thomas; Bange, Sebastian; Schmitz, Daniela; Würsch, Dominik; Höger, Sigurd; Vogelsang, Jan; Lupton, John M

2013-01-09

A set of π-conjugated oligomer dimers templated in molecular scaffolds is presented as a model system for studying the interactions between chromophores in conjugated polymers (CPs). Single-molecule spectroscopy was used to reveal energy transfer dynamics between two oligomers in either a parallel or oblique-angle geometry. In particular, the conformation of single molecules embedded in a host matrix was investigated via polarized excitation and emission fluorescence microscopy in combination with fluorescence correlation spectroscopy. While the intramolecular interchromophore conformation was found to have no impact on the fluorescence quantum yield, lifetime, or photon statistics (antibunching), the long-term nonequilibrium dynamics of energy transfer within these bichromophoric systems was accessible by studying the linear dichroism in emission at the single-molecule level, which revealed reversible switching of the emission between the two oligomers. In bulk polymer films, interchromophore coupling promotes the migration of excitation energy to quenching sites. Realizing the presence and dynamics of such interactions is crucial for understanding limitations on the quantum efficiency of larger CP materials.

Broadband Enhancement of Spontaneous Emission in Two-Dimensional Semiconductors Using Photonic Hypercrystals.

PubMed

Galfsky, Tal; Sun, Zheng; Considine, Christopher R; Chou, Cheng-Tse; Ko, Wei-Chun; Lee, Yi-Hsien; Narimanov, Evgenii E; Menon, Vinod M

2016-08-10

The low quantum yield observed in two-dimensional semiconductors of transition metal dichalcogenides (TMDs) has motivated the quest for approaches that can enhance the light emission from these systems. Here, we demonstrate broadband enhancement of spontaneous emission and increase in Raman signature from archetype two-dimensional semiconductors: molybdenum disulfide (MoS2) and tungsten disulfide (WS2) by placing the monolayers in the near field of a photonic hypercrystal having hyperbolic dispersion. Hypercrystals are characterized by a large broadband photonic density of states due to hyperbolic dispersion while having enhanced light in/out coupling by a subwavelength photonic crystal lattice. This dual advantage is exploited here to enhance the light emission from the 2D TMDs and can be utilized for developing light emitters and solar cells using two-dimensional semiconductors.

Comparison of physical and photophysical properties of monometallic and bimetallic ruthenium(II) complexes containing structurally altered diimine ligands

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

Macatangay, A.; Jackman, D.C.; Merkert, J.W.

1996-11-06

The physical and photophysical properties of a series of monometallic, [Ru(bpy){sub 2}(dmb)]{sup 2+}, [Ru(bpy){sub 2}(BPY)]{sup 2+}, [Ru(bpy)(Obpy)]{sup 2+} and [Ru(bpy){sub 2}(Obpy)] {sup 2+}, and bimetallic, [(Ru(bpy){sub 2}){sub 2}(BPY)]{sup 4+} and [(Ru(bpy){sub 2}){sub 2}(Obpy)]{sup 4+}, complexes are examined, where bpy is 2,2{prime}-bipyridine, dmb is 4,4{prime}-dimethyl-2,2{prime}-bipyridine, BPY is 1,2-bis(4-methyl-2,2{prime}-bipyridin-4{prime}-yl)ethane, and Obpy is 1,2-bis(2,2{prime}-bipyridin-6-yl)ethane. The complexes display metal-to-ligand charge transfer transitions in the 450 nmn region, intraligand {pi}{yields}{pi}* transitions at energies greater than 300 nm, a reversible oxidation of the ruthenium(II) center in the 1.25-1.40 V vs SSCE region, a series of three reductions associated with each coordinated ligand commencing at {minus}1.3 Vmore » and ending at {approximately}{minus}1.9 V, and emission from a {sup 3}MLCT state having energy maxima between 598 and 610 nm. The Ru{sup III}/Ru{sup II} oxidation of the two bimetallic complexes is a single, two one-electron process. Relative to [Ru(bpy){sub 2}(BPY)]{sup 2+}, the Ru{sup III}/Ru{sup II} potential for [Ru-(bpy){sub 2}(Obpy)]{sup 2+} increases from 1.24 to 1.35 V, the room temperature emission lifetime decreases from 740 to 3ns, and the emission quantum yield decreases from 0.078 to 0.000 23. Similarly, relative to [(Ru(bpy){sub 2}){sub 2}(BPY)]{sup 4+}, the Ru{sup III}/Ru{sup II} potential for [(Ru(bpy){sub 2}){sub 2}(Obpy)]{sup 4+} increases from 1.28 to 1.32 V, the room temperature emission lifetime decreases from 770 to 3 ns, and the room temperature emission quantum yield decreases from 0.079 to 0.000 26.« less

Absorption and emission spectroscopic characterisation of combined wildtype LOV1-LOV2 domain of phot from Chlamydomonas reinhardtii.

PubMed

Song, S-H; Dick, B; Zirak, P; Penzkofer, A; Schiereis, T; Hegemann, P

2005-10-03

An absorption and emission spectroscopic characterisation of the combined wild-type LOV1-LOV2 domain string (abbreviated LOV1/2) of phot from the green alga Chlamydomonas reinhardtii is carried out at pH 8. A LOV1/2-MBP fusion protein (MBP=maltose binding protein) and LOV1/2 with a His-tag at the C-terminus (LOV1/2-His) expressed in an Escherichia coli strain are investigated. Blue-light photo-excitation generates a non-fluorescent intermediate photoproduct (flavin-C(4a)-cysteinyl adduct with absorption peak at 390 nm). The photo-cycle dynamics is studied by dark-state absorption and fluorescence measurement, by following the temporal absorption and emission changes under blue and violet light exposure, and by measuring the temporal absorption and fluorescence recovery after light exposure. The fluorescence quantum yield, phi(F), of the dark adapted samples is phi(F)(LOV1/2-His) approximately 0.15 and phi(F)(LOV1/2-MBP) approximately 0.17. A bi-exponential absorption recovery after light exposure with a fast (in the several 10-s range) and a slow component (in the near 10-min range) are resolved. The quantum yield of photo-adduct formation, phi(Ad), is extracted from excitation intensity dependent absorption measurements. It decreases somewhat with rising excitation intensity. The behaviour of the combined wildtype LOV1-LOV2 double domains is compared with the behaviour of the separate LOV1 and LOV2 domains.

Luminescence in Primordial Helium Lines at the Pre-recombination Epoch

NASA Astrophysics Data System (ADS)

Dubrovich, V. K.; Grachev, S. I.

2018-04-01

The formation of luminescent subordinate He I lines by the absorption of radiation from a source in lines of the main He I series in an expanding Universe is considered. A burst of radiation in continuum is assumed to occur at some instant of time corresponding to redshift z 0. This radiation is partially absorbed at different z < z 0 in lines of the main He I series (different pumping channels) and then is partially converted into radiation in subordinate lines. If ν ik is the laboratory transition frequency of some subordinate line emerging at some z, then at the present epoch its frequency will be ν = ν ik /(1 + z). The quantum yield, i.e., the number of photons emitted in the subordinate line per initial excited atom, has been calculated for different z (and, consequently, for different ν). Several pumping channels have been considered. We show that the luminescent lines can be both emission and absorption ones; the same line can be an emission one for one of the pumping channels and an absorption one for another. For example, the 1s2s-1s2p (1S-1P*) line is an emission one for the 1s2-1s2p pumping and an absorption one for the 1s2-1s3p pumping. We show that in the frequency range 30-80 GHz the total quantum yield for the first and second of the above channels can reach +50 and -50%, respectively.

Spectroscopic properties and amplified spontaneous emission of fluorescein laser dye in ionic liquids as green media

NASA Astrophysics Data System (ADS)

AL-Aqmar, Dalal M.; Abdelkader, H. I.; Abou Kana, Maram T. H.

2015-09-01

The use of ionic liquids (ILs) as milieu materials for laser dyes is a promising field and quite competitive with volatile organic solvents and solid state-dye laser systems. This paper investigates some photo-physical parameters of fluorescein dye incorporated into ionic liquids; 1-Butyl-3-methylimidazolium chloride (BMIM Cl), 1-Butyl-3-methylimidazolium tetrachloroaluminate (BMIM AlCl4) and 1-Butyl-3-methylimidazolium tetrafluoroborate (BMIM BF4) as promising host matrix in addition to ethanol as reference. These parameters are: absorption and emission cross-sections, fluorescence lifetime and quantum yield, in addition to the transition dipole moment, the attenuation length and oscillator strength were also investigated. Lasing characteristics such as amplified spontaneous emission (ASE), the gain, and the photostability of fluorescein laser dye dissolved in different host materials were assessed. The composition and properties of the matrix of ILs were found that it has great interest in optimizing the laser performance and photostability of the investigated laser dye. Under transverse pumping of fluorescein dye by blue laser diode (450 nm) of (400 mW), the initial ASE for dye dissolved in BMIM AlCl4 and ethanol were decreased to 39% and 36% respectively as time progressed 132 min. Relatively high efficiency and high fluorescence quantum yield (11.8% and 0.82% respectively) were obtained with good photostability in case of fluorescein in BMIM BF4 that was decreased to ∼56% of the initial ASE after continuously pumping with 400 mW for 132 min.

Coumarin Derivative Directly Coordinated to Lanthanides Acts as an Excellent Antenna for UV-Vis and Near-IR Emission.

PubMed

Guzmán-Méndez, Óscar; González, Federico; Bernès, Sylvain; Flores-Álamo, Marcos; Ordóñez-Hernández, Javier; García-Ortega, Héctor; Guerrero, Joselin; Qian, Wenjie; Aliaga-Alcalde, Nuria; Gasque, Laura

2018-02-05

A chelating coumarin-derived ligand sensitizes all emitting lanthanide ions in the solid state and gives high absolute quantum yields for ethanol solutions of complexes of Sm, Eu, Tb, and Dy, above 20% for the last two. Crystal structures of these four complexes are [Ln(Cum) 3 (H 2 O)(X)]·X where X = MeOH or EtOH.

Synthesis and systematic evaluation of dark resonance energy transfer (DRET)-based library and its application in cell imaging.

PubMed

Su, Dongdong; Teoh, Chai Lean; Kang, Nam-Young; Yu, Xiaotong; Sahu, Srikanta; Chang, Young-Tae

2015-03-01

In this paper, we report a new strategy for constructing a dye library with large Stokes shifts. By coupling a dark donor with BODIPY acceptors of tunable high quantum yield, a novel dark resonance energy transfer (DRET)-based library, named BNM, has been synthesized. Upon excitation of the dark donor (BDN) at 490 nm, the absorbed energy is transferred to the acceptor (BDM) with high efficiency, which was tunable in a broad range from 557 nm to 716 nm, with a high quantum yield of up to 0.8. It is noteworthy to mention that the majority of the non-radiative energy loss of the donor was converted into the acceptor's fluorescence output with a minimum leak of donor emission. Fluorescence imaging tested in live cells showed that the BNM compounds are cell-permeable and can also be employed for live-cell imaging. This is a new library which can be excited through a dark donor allowing for strong fluorescence emission in a wide range of wavelengths. Thus, the BNM library is well suited for high-throughput screening or multiplex experiments in biological applications by using a single laser excitation source. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Efficient Carrier-to-Exciton Conversion in Field Emission Tunnel Diodes Based on MIS-Type van der Waals Heterostack.

PubMed

Wang, Shunfeng; Wang, Junyong; Zhao, Weijie; Giustiniano, Francesco; Chu, Leiqiang; Verzhbitskiy, Ivan; Zhou Yong, Justin; Eda, Goki

2017-08-09

We report on efficient carrier-to-exciton conversion and planar electroluminescence from tunnel diodes based on a metal-insulator-semiconductor (MIS) van der Waals heterostack consisting of few-layer graphene (FLG), hexagonal boron nitride (hBN), and monolayer tungsten disulfide (WS 2 ). These devices exhibit excitonic electroluminescence with extremely low threshold current density of a few pA·μm -2 , which is several orders of magnitude lower compared to the previously reported values for the best planar EL devices. Using a reference dye, we estimate the EL quantum efficiency to be ∼1% at low current density limit, which is of the same order of magnitude as photoluminescence quantum yield at the equivalent excitation rate. Our observations reveal that the efficiency of our devices is not limited by carrier-to-exciton conversion efficiency but by the inherent exciton-to-photon yield of the material. The device characteristics indicate that the light emission is triggered by injection of hot minority carriers (holes) to n-doped WS 2 by Fowler-Nordheim tunneling and that hBN serves as an efficient hole-transport and electron-blocking layer. Our findings offer insight into the intelligent design of van der Waals heterostructures and avenues for realizing efficient excitonic devices.

Solvent induced fluorescence enhancement of graphene oxide studied by ultrafast spectroscopy

NASA Astrophysics Data System (ADS)

Zhao, Litao; Chen, Jinquan; He, Xiaoxiao; Yu, Xiantong; Yan, Shujun; Zhang, Sanjun; Pan, Haifeng; Xu, Jianhua

2018-05-01

Femtosecond transient absorption (TA) spectroscopy combined with picosecond time resolved fluorescence (TRF) were used to reveal the fluorescence kinetics of graphene oxide (GO) in water, ethanol and water-ethanol mixtures. Size-independent fluorescence of GO were observed in water, and pH-dependent fluorescence spectra could be fitted well by a triple emission relaxation with peaks around 440 nm, 500 nm, and 590 nm respectively. The results indicate that polycyclic aromatic hydrocarbons (PAHs) linked by oxygen-containing functional groups dominate GO's fluorescence emission. GO's fluorescence quantum yield was measured to be 2.8% in ethanol but 1.2% in water. The three decay components fluorescence decay, as well as the transient absorption dynamics with an offset, confirmed this solvent induced fluorescence enhancement. GO's Raman spectral signals showed that GO in ethanol has a smaller average size of PAHs than that of GO in water. Therefore, besides other enhancement effects reported in literatures, we proposed that solvents could also change the size of PAHs, resulting in a photoluminescence enhancement. Our experimental data demonstrates that GO's quantum yield could be up to 2.8% in water and 8.4% in ethanol and this observation may help ones to improve GO's photoluminescence efficiency as well as its applications in solution.

Single component Mn-doped perovskite-related CsPb2ClxBr5-x nanoplatelets with a record white light quantum yield of 49%: a new single layer color conversion material for light-emitting diodes.

PubMed

Wu, Hao; Xu, Shuhong; Shao, Haibao; Li, Lang; Cui, Yiping; Wang, Chunlei

2017-11-09

Single component nanocrystals (NCs) with white fluorescence are promising single layer color conversion media for white light-emitting diodes (LED) because the undesirable changes of chromaticity coordinates for the mixture of blue, green and red emitting NCs can be avoided. However, their practical applications have been hindered by the relative low photoluminescence (PL) quantum yield (QY) for traditional semiconductor NCs. Though Mn-doped perovskite nanocube is a potential candidate, it has been unable to realize a white-light emission to date. In this work, the synthesis of Mn-doped 2D perovskite-related CsPb 2 Cl x Br 5-x nanoplatelets with a pure white emission from a single component is reported. Unlike Mn-doped perovskite nanocubes with insufficient energy transfer efficiency, the current reported Mn-doped 2D perovskite-related CsPb 2 Cl x Br 5-x nanoplatelets show a 10 times higher energy transfer efficiency from perovskite to Mn impurities at the required emission wavelengths (about 450 nm for perovskite emission and 580 nm for Mn emission). As a result, the Mn/perovskite dual emission intensity ratio surprisingly elevates from less than 0.25 in case of Mn-doped nanocubes to 0.99 in the current Mn-doped CsPb 2 Cl x Br 5-x nanoplatelets, giving rise to a pure white light emission with Commission Internationale de l'Eclairage (CIE) color coordinates of (0.35, 0.32). More importantly, the highest PL QY for Mn-doped perovskite-related CsPb 2 Cl x Br 5-x nanoplatelets is up to 49%, which is a new record for white-emitting nanocrystals with single component. These highly luminescent nanoplatelets can be blended with polystyrene (PS) without changing the white light emission but dramatically improving perovskite stability. The perovskite-PS composites are available not only as a good solution processable coating material for assembling LED, but also as a superior conversion material for achieving white light LED with a single conversion layer.

Single-exciton optical gain in semiconductor nanocrystals.

PubMed

Klimov, Victor I; Ivanov, Sergei A; Nanda, Jagjit; Achermann, Marc; Bezel, Ilya; McGuire, John A; Piryatinski, Andrei

2007-05-24

Nanocrystal quantum dots have favourable light-emitting properties. They show photoluminescence with high quantum yields, and their emission colours depend on the nanocrystal size--owing to the quantum-confinement effect--and are therefore tunable. However, nanocrystals are difficult to use in optical amplification and lasing. Because of an almost exact balance between absorption and stimulated emission in nanoparticles excited with single electron-hole pairs (excitons), optical gain can only occur in nanocrystals that contain at least two excitons. A complication associated with this multiexcitonic nature of light amplification is fast optical-gain decay induced by non-radiative Auger recombination, a process in which one exciton recombines by transferring its energy to another. Here we demonstrate a practical approach for obtaining optical gain in the single-exciton regime that eliminates the problem of Auger decay. Specifically, we develop core/shell hetero-nanocrystals engineered in such a way as to spatially separate electrons and holes between the core and the shell (type-II heterostructures). The resulting imbalance between negative and positive charges produces a strong local electric field, which induces a giant ( approximately 100 meV or greater) transient Stark shift of the absorption spectrum with respect to the luminescence line of singly excited nanocrystals. This effect breaks the exact balance between absorption and stimulated emission, and allows us to demonstrate optical amplification due to single excitons.

Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules.

PubMed

Han, M; Gao, X; Su, J Z; Nie, S

2001-07-01

Multicolor optical coding for biological assays has been achieved by embedding different-sized quantum dots (zinc sulfide-capped cadmium selenide nanocrystals) into polymeric microbeads at precisely controlled ratios. Their novel optical properties (e.g., size-tunable emission and simultaneous excitation) render these highly luminescent quantum dots (QDs) ideal fluorophores for wavelength-and-intensity multiplexing. The use of 10 intensity levels and 6 colors could theoretically code one million nucleic acid or protein sequences. Imaging and spectroscopic measurements indicate that the QD-tagged beads are highly uniform and reproducible, yielding bead identification accuracies as high as 99.99% under favorable conditions. DNA hybridization studies demonstrate that the coding and target signals can be simultaneously read at the single-bead level. This spectral coding technology is expected to open new opportunities in gene expression studies, high-throughput screening, and medical diagnostics.

Quantum efficiencies exceeding unity in amorphous silicon solar cells

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

Vanmaekelbergh, D.; Lagemaat, J. van de; Schropp, R.E.I.

1994-12-31

The experimental observation of internal quantum efficiencies above unity in crystalline silicon solar cells has brought up the question whether the generation of multiple electron/hole pairs has to be taken into consideration also in solar cells based on direct gap amorphous semiconductors. To study photogenerated carrier dynamics, the authors have applied Intensity Modulated Photocurrent Spectroscopy (IMPS) to hydrogenated amorphous silicon p-i-n solar cells. In the reverse voltage bias region at low illumination intensities it has been observed that the low frequency limit of the AC quantum yield Y increases significantly above unit with decreasing light intensity, indicating that more thanmore » one electron per photon is detected in the external circuit. This phenomenon can be explained by considering trapping and thermal emission of photogenerated carriers at intragap atmospheric dangling bond defect centers.« less

Spectroscopic Analysis of Red Fluorescent Proteins and Development of a Microfluidic Cell Sorter for the Generation of Improved Variants

NASA Astrophysics Data System (ADS)

Lubbeck, Jennifer L.

The discovery of the green fluorescent protein (GFP) launched the development of a wide variety of fluorescent protein (FP) mutants whose spectral and photophysical diversity revolutionized in vivo imaging. The excitation and emission spectra of red fluorescent proteins (RFPs), in particular, have been ideally tuned to a window optically favorable for in vivo work. However, their quantum yields, photostabilities and fluorescence intermittency properties require improvement if they are to be broadly employed for low-copy or single-molecule measurements. Attempts to engineer improved RFPs often result in optimization of one photophysical property at the expense of others. We developed a microfluidic-based cytometer for screening HeLa cell-based genetic RFP-libraries simultaneously on the basis of fluorescence lifetime (a proxy for quantum yield), photostability, and brightness. Ten 532 nm excitation beams interrogate each cell in flow. The first is electro-optically modulated (30 MHz) to enable lifetime measurement with phase fluorimetry. The remaining beams act as a pulse sequence for isolating the irreversible photobleaching time constant. Optical-force switching is employed to sort cells based on any combination of the photophysical parameters. Screening with this instrument enables identification of regions of the structure that synergistically affect quantum yield and photostability and the sorting capability provides a new tool for accelerating the development of next generation RFPs.

Electric field-induced emission enhancement and modulation in individual CdSe nanowires.

PubMed

Vietmeyer, Felix; Tchelidze, Tamar; Tsou, Veronica; Janko, Boldizsar; Kuno, Masaru

2012-10-23

CdSe nanowires show reversible emission intensity enhancements when subjected to electric field strengths ranging from 5 to 22 MV/m. Under alternating positive and negative biases, emission intensity modulation depths of 14 ± 7% are observed. Individual wires are studied by placing them in parallel plate capacitor-like structures and monitoring their emission intensities via single nanostructure microscopy. Observed emission sensitivities are rationalized by the field-induced modulation of carrier detrapping rates from NW defect sites responsible for nonradiative relaxation processes. The exclusion of these states from subsequent photophysics leads to observed photoluminescence quantum yield enhancements. We quantitatively explain the phenomenon by developing a kinetic model to account for field-induced variations of carrier detrapping rates. The observed phenomenon allows direct visualization of trap state behavior in individual CdSe nanowires and represents a first step toward developing new optical techniques that can probe defects in low-dimensional materials.

Dy3+ doped tellurite glasses containing silver nanoparticles for lighting devices

NASA Astrophysics Data System (ADS)

Hua, Chenxiao; Shen, Lifan; Pun, Edwin Yue Bun; Li, Desheng; Lin, Hai

2018-04-01

Efficient warm yellowish-white fluorescence emissions of Dy3+ were observed in heavy metal germanium tellurite (HGT) glasses under the excitation of 454 nm. Further, the luminescence intensity of Dy3+ is increased by ∼29% accompanying the introduction of Ag NPs with diameter ∼7 nm when compared with that of the silver-free case, which is caused by the existence of localized surface plasmon resonance (LSPR). The larger net emission power, the more net emission photon number and the higher quantum yield in Dy2O3 doped HGT glasses containing Ag NPs (HGT-Ag) confirm the availability of utilizing laser. Presupposed fluorescence color trace reveals that white luminescence can be achieved when the intensity ratio between residual laser and Dy3+ emission reaches the appropriate range. The productive transition emissions and the tunable white fluorescence illustrate tellurite glasses embodying noble-metal NPs are a potential candidate for high-quality lighting devices.

Spectroscopic Characterization of Streptavidin Functionalized Quantum dots1

PubMed Central

Wu, Yang; Lopez, Gabriel P.; Sklar, Larry A.; Buranda, Tione

2007-01-01

The spectroscopic properties of quantum dots can be strongly influenced by the conditions of their synthesis. In this work we have characterized several spectroscopic properties of commercial, streptavidin functionalized quantum dots (QD525, lot#1005-0045 and QD585, Lot#0905-0031 from Invitrogen). This is the first step in the development of calibration beads, to be used in a generalizable quantification scheme of multiple fluorescent tags in flow cytometry or microscopy applications. We used light absorption, photoexcitation, and emission spectra, together with excited-state lifetime measurements to characterize their spectroscopic behavior, concentrating on the 400-500nm wavelength ranges that are important in biological applications. Our data show an anomalous dependence of emission spectrum, lifetimes, and quantum yield (QY) on excitation wavelength that is particularly pronounced in the QD525. For QD525, QY values ranged from 0.2 at 480nm excitation up to 0.4 at 450nm and down again to 0.15 at 350nm. For QD585, QY values were constant at 0.2 between 500nm and 400nm, but dropped to 0.1 at 350nm. We attribute the wavelength dependences to heterogeneity in size and surface defects in the QD525, consistent with characteristics previously described in the chemistry literature. The results are discussed in the context of bridging the gap between what is currently known in the physical chemistry literature of quantum dots, and the quantitative needs of assay development in biological applications. PMID:17368555

Tapping the potential of trioctylphosphine (TOP) in the realization of highly luminescent blue-emitting colloidal indium phosphide (InP) quantum dots

NASA Astrophysics Data System (ADS)

Singh, Akanksha; Chawla, Parul; Jain, Shefali; Sharma, Shailesh Narain

2017-06-01

In this work, extremely small blue emitting colloidal InP-based quantum dots (size 2-5 nm) have been synthesized using trioctylphosphine (TOP) as a source of phosphorus. The method reported here is unconventional, quite rapid ( 90 min), more viable, less expensive and relatively greener as compared to other conventional methods that employ tristrimethylsilyylphosphine(P(SiMe3)3) which is scarce, expensive, flammable, highly toxic and even banned in a few countries. Highly luminescent InP QDs having bluish-green emission (λ 490 nm) can be synthesized using this method without resorting to any post-synthesis etching to tune the emission to the blue region. Besides being the source of phosphorus and the particle size regulating agent, the efficacy of TOP is further realized during synthesis via its reduction of indium salt, which aids in the formation of indium metal and then subsequently in the development of InP QDs. The PL intensity of as-synthesized InP QDs is further enhanced by growing a shell of wide band gap material, i.e. ZnS resulting in a concurrent increment in quantum yield from 25% to 38% respectively.

Compact Biocompatible Quantum Dots Functionalized for Cellular Imaging

PubMed Central

Liu, Wenhao; Howarth, Mark; Greytak, Andrew B.; Zheng, Yi; Nocera, Daniel G.; Ting, Alice Y.; Bawendi, Moungi G.

2009-01-01

We present a family of water-soluble quantum dots (QDs) that exhibit low nonspecific binding to cells, small hydrodynamic diameter, tunable surface charge, high quantum yield, and good solution stability across a wide pH range. These QDs are amenable to covalent modification via simple carbodiimide coupling chemistry, which is achieved by functionalizing the surface of QDs with a new class of heterobifunctional ligands incorporating dihydrolipoic acid, a short poly(ethylene glycol) (PEG) spacer, and an amine or carboxylate terminus. The covalent attachment of molecules is demonstrated by appending a rhodamine dye to form a QD-dye conjugate exhibiting fluorescence resonance energy transfer (FRET). High-affinity labeling is demonstrated by covalent attachment of streptavidin, thus enabling the tracking of biotinylated epidermal growth factor (EGF) bound to EGF receptor on live cells. In addition, QDs solubilized with the heterobifunctional ligands retain their metal-affinity driven conjugation chemistry with polyhistidine-tagged proteins. This dual functionality is demonstrated by simultaneous covalent attachment of a rhodamine FRET acceptor and binding of polyhistidine-tagged streptavidin on the same nanocrystal to create a targeted QD, which exhibits dual-wavelength emission. Such emission properties could serve as the basis for ratiometric sensing of the cellular receptor’s local chemical environment. PMID:18177042

Parallel Synthesis of photoluminescent π-conjugated polymers by polymer reactions of an organotitanium polymer with a titanacyclopentadiene unit.

PubMed

Matsumura, Yoshimasa; Fukuda, Katsura; Inagi, Shinsuke; Tomita, Ikuyoshi

2015-04-01

A regioregular organometallic polymer with titanacyclopentadiene unit, obtained by the reaction of a 2,7-diethynylfluorene derivative and a low-valent titanium complex, is subjected to the reaction with three kinds of electrophiles (i.e., sulfur monochloride, hydrochloric acid, and dichlorophenylphosphine) to give π-conjugated polymers possessing both fluorene and building blocks originated from the transformation of the titanacycles in the main chain. For example, a phosphole-containing polymer whose number-average molecular weight is estimated as 5000 is obtained in 50% yield. The obtained thiophene, butadiene, and phosphole-containing polymers exhibit efficient photoluminescence (PL) with emission colors of blue, green, and yellow, respectively. For example, the phosphole-containing polymer exhibits yellow PL with an emission maximum (Emax ) of 533 nm and a quantum yield (Φ) of 0.37. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and Spectral Evaluation of Some Unsymmetrical Mesoporphyrinic Complexes

PubMed Central

Boscencu, Rica; Oliveira, Anabela Sousa; Ferreira, Diana P.; Ferreira, Luís Filipe Vieira

2012-01-01

Synthesis and spectral evaluation of new zinc and copper unsymmetrical mesoporphyrinic complexes are reported. Zn(II)-5-(4-acetoxy-3-methoxyphenyl)-10,15,20- tris-(4-carboxymethylphenyl)porphyrin, Zn(II)-5-[(3,4-methylenedioxy)phenyl]-10,15,20- tris-(4-carboxymethylphenyl)porphyrin, Cu(II)-5-(4-acetoxy-3-methoxyphenyl)-10,15,20- tris-(4-carboxymethylphenyl)porphyrin and Cu(II)-5-[(3,4-methylenedioxy)phenyl]-10,15,20- tris-(4-carboxymethylphenyl)porphyrin were synthesized using microwave-assisted synthesis. The complexes were characterized by elemental analysis, FT-IR, UV-Vis, EPR and NMR spectroscopy, which fully confirmed their structure. The spectral absorption properties of the porphyrinic complexes were studied in solvents with different polarities. Fluorescence emission and singlet oxygen formation quantum yields were evaluated for the compounds under study, revealing high yields for the zinc derivatives. The copper complexes are not emissive and only display residual capacity for singlet oxygen formation. PMID:22942693

Optical parameters of diode lasers based on an InAsSb/InAsSbP heterostructure

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

Astakhova, A. P.; Bez'yazychnaya, T. V.; Burov, L. I.

2008-02-15

The rates of radiative recombination (including transitions induced by enhanced luminescence) and nonradiative recombination, internal quantum yield of luminescence, and the matrix element for band-to-band optical transitions were determined for the first time for InAsSb/InAsSbP diode lasers oscillating at wavelengths of 3.1-3.2 {mu}m. It is established that the contribution of nonradiative recombination to the lasing threshold can be as large as 97%. The internal quantum yield of luminescence for the InAs{sub 0.97}Sb{sub 0.03} compound is no higher than 3%. Most likely, the nonradiative channel is formed with involvement of Auger recombination with the constant C = 4.2 Multiplication-Sign 10{sup -38}more » m{sup 6}s{sup -1} (T = 77 K). The studied samples of lasers feature relatively low optical losses {rho} = 900 m{sup -1} and internal quantum efficiency of emission at the level of 0.6. The spontaneous lifetime of nonequilibrium charge carriers as determined from the radiative-recombination rate is equal to 6 Multiplication-Sign 10{sup -8} s, which is consistent with known published data.« less

Optical parameters of diode lasers based on an InAsSb/InAsSbP heterostructure

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

Astakhova, A. P.; Bez'yazychnaya, T. V.; Burov, L. I.

2008-02-15

The rates of radiative recombination (including transitions induced by enhanced luminescence) and nonradiative recombination, internal quantum yield of luminescence, and the matrix element for band-to-band optical transitions were determined for the first time for InAsSb/InAsSbP diode lasers oscillating at wavelengths of 3.1-3.2 {mu}m. It is established that the contribution of nonradiative recombination to the lasing threshold can be as large as 97%. The internal quantum yield of luminescence for the InAs{sub 0.97}Sb{sub 0.03} compound is no higher than 3%. Most likely, the nonradiative channel is formed with involvement of Auger recombination with the constant C = 4.2 x 10{sup -38}more » m{sup 6}s{sup -1} (T = 77 K). The studied samples of lasers feature relatively low optical losses {rho} = 900 m{sup -1} and internal quantum efficiency of emission at the level of 0.6. The spontaneous lifetime of nonequilibrium charge carriers as determined from the radiative-recombination rate is equal to 6 x 10{sup -8} s, which is consistent with known published data.« less

Phosphorescent Iridium(III) Complexes Bearing Fluorinated Aromatic Sulfonyl Group with Nearly Unity Phosphorescent Quantum Yields and Outstanding Electroluminescent Properties.

PubMed

Zhao, Jiang; Yu, Yue; Yang, Xiaolong; Yan, Xiaogang; Zhang, Huiming; Xu, Xianbin; Zhou, Guijiang; Wu, Zhaoxin; Ren, Yixia; Wong, Wai-Yeung

2015-11-11

A series of heteroleptic functional Ir(III) complexes bearing different fluorinated aromatic sulfonyl groups has been synthesized. Their photophysical features, electrochemical behaviors, and electroluminescent (EL) properties have been characterized in detail. These complexes emit intense yellow phosphorescence with exceptionally high quantum yields (ΦP > 0.9) at room temperature, and the emission maxima of these complexes can be finely tuned depending upon the number of the fluorine substituents on the pendant phenyl ring of the sulfonyl group. Furthermore, the electrochemical properties and electron injection/transporting (EI/ET) abilities of these Ir(III) phosphors can also be effectively tuned by the fluorinated aromatic sulfonyl group to furnish some desired characters for enhancing the EL performance. Hence, the maximum luminance efficiency (ηL) of 81.2 cd A(-1), corresponding to power efficiency (ηP) of 64.5 lm W(-1) and external quantum efficiency (ηext) of 19.3%, has been achieved, indicating the great potential of these novel phosphors in the field of organic light-emitting diodes (OLEDs). Furthermore, a clear picture has been drawn for the relationship between their optoelectronic properties and chemical structures. These results should provide important information for developing highly efficient phosphors.

High-Z Nanoparticle/Polymer Nanocomposites for Gamma-Ray Scintillation Detectors

NASA Astrophysics Data System (ADS)

Liu, Chao

An affordable and reliable solution for spectroscopic gamma-ray detection has long been sought after due to the needs from research, defense, and medical applications. Scintillators resolve gamma energy by proportionally converting a single high-energy photon into a number of photomultiplier-tube-detectable low-energy photons, which is considered a more affordable solution for general purposes compared to the delicate semiconductor detectors. An ideal scintillator should simultaneously exhibit the following characteristics: 1) high atomic number (Z) for high gamma stopping power and photoelectron production; 2) high light yield since the energy resolution is inversely proportional to the square root of light yield; 3) short emission decay lifetime; and 4) low cost and scalable production. However, commercial scintillators made from either inorganic single crystals or plastics fail to satisfy all requirements due to their intrinsic material properties and fabrication limitations. The concept of adding high-Z constituents into plastic scintillators to harness high Z, low cost, and fast emission in the resulting nanocomposite scintillators is not new in and of itself. Attempts have been made by adding organometallics, quantum dots, and scintillation nanocrystals into the plastic matrix. High-Z organometallics have long been used to improve the Z of plastic scintillators; however, their strong spin-orbit coupling effect entails careful triplet energy matching using expensive triplet emitters to avoid severe quenching of the light yield. On the other hand, reported quantum dot- and nanocrystal-polymer nanocomposites suffer from moderate Z and high optical loss due to aggregation and self-absorption at loadings higher than 10 wt%, limiting their potential for practical application. This dissertation strives to improve the performance of nanoparticle-based nanocomposite scintillators. One focus is to synthesize transparent nanocomposites with higher loadings of high-Z inorganic nanoparticles. A facile single-precursor method is first developed to synthesize HfO2 nanoparticles, the highest-Z simple oxide with band gap larger than polyvinyltoluene, with uniform size distribution around 5 nm. A nanoparticle-surface-modification protocol is then developed for the fabrication of transparent nanocomposite monoliths with high nanoparticle loadings (up to 40 wt%). Using this method, transparent HfO2-loaded blue-emitting nanocomposite scintillators (2 mm thick, transmittance at 550 nm >75%) have been fabricated capable of producing a full energy photopeak for 662 keV gamma rays, with the best deconvoluted photopeak energy resolution < 8%, representing a significant improvement over previous nanoparticle-based nanocomposite scintillators. Although the HfO2 work represents a great improvement over previous reports, it is also found in this system that the light yield deteriorates at higher nanoparticle loadings. This is attributed to the trapping of fast electron energy deposited in the non-emitting nanoparticles. To overcome this deterioration issue, a revisit to the previously proposed quantum-dot-loaded nanocomposite scintillator is made with significant improvements. Transparent, ultra-high-loading (up to 60 wt%) CdxZn1-xS/ZnS core/shell quantum dot/polymer nanocomposite monoliths are first synthesized by in situ copolymerization of the partially mathacrylate-functionalized quantum dots in a monomer solution. With efficient Forster resonance energy transfer from the high-atomic-number quantum dots to lower-band-gap organic dyes, quantum-dot-borne excitons are extracted for photon production. The resulting nanocomposites thus exhibit unprecedented simultaneous enhancements in both light yield (visible photons produced per MeV of gamma photon energy) and gamma attenuation power. In a best demonstration, a 60 wt% quantum-dot nanocomposite scintillator exhibits a light yield of 9255 photons/MeV and a photopeak resolution of 9.8% under 662 keV Cs-137 gamma irradiation, demonstrating the potential of this model system for future high-performance low-cost spectroscopic gamma detectors.

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

Lisitsyn, V. M.; Stepanov, S. A., E-mail: stepanovsa@tpu.ru; Yangyang, Ju

In most promising widespread gallium nitride based LEDs emission is generated in the blue spectral region with a maximum at about 450 nm which is converted to visible light with the desired spectrum by means of phosphor. The thermal energy in the conversion is determined by the difference in the energies of excitation and emission quanta and the phosphor quantum yield. Heat losses manifest themselves as decrease in the luminous efficacy. LED heating significantly reduces its efficiency and life. In addition, while heating, the emission generation output and the efficiency of the emission conversion decrease. Therefore, the reduction of the energymore » losses caused by heating is crucial for LED development. In this paper, heat losses in phosphor-converted LEDs (hereinafter chips) during spectrum conversion are estimated. The limit values of the luminous efficacy for white LEDs are evaluated.« less

Aggregation-induced emission: phenomenon, mechanism and applications.

PubMed

Hong, Yuning; Lam, Jacky W Y; Tang, Ben Zhong

2009-08-07

It is textbook knowledge that chromophore aggregation generally quenches light emission. In this feature article, we give an account on how we observed an opposite phenomenon termed aggregation-induced emission (AIE) and identified the restriction of intramolecular rotation as a main cause for the AIE effect. Based on the mechanistic understanding, we developed a series of new fluorescent and phosphorescent AIE systems with emission colours covering the entire visible spectral region and luminescence quantum yields up to unity. We explored high-tech applications of the AIE luminogens as, for example, fluorescence sensors (for explosive, ion, pH, temperature, viscosity, pressure, etc.), biological probes (for protein, DNA, RNA, sugar, phospholipid, etc.), immunoassay markers, PAGE visualization agents, polarized light emitters, monitors for layer-by-layer assembly, reporters for micelle formation, multistimuli-responsive nanomaterials, and active layers in the fabrication of organic light-emitting diodes.

High mobility emissive organic semiconductor

PubMed Central

Liu, Jie; Zhang, Hantang; Dong, Huanli; Meng, Lingqiang; Jiang, Longfeng; Jiang, Lang; Wang, Ying; Yu, Junsheng; Sun, Yanming; Hu, Wenping; Heeger, Alan J.

2015-01-01

The integration of high charge carrier mobility and high luminescence in an organic semiconductor is challenging. However, there is need of such materials for organic light-emitting transistors and organic electrically pumped lasers. Here we show a novel organic semiconductor, 2,6-diphenylanthracene (DPA), which exhibits not only high emission with single crystal absolute florescence quantum yield of 41.2% but also high charge carrier mobility with single crystal mobility of 34 cm2 V−1 s−1. Organic light-emitting diodes (OLEDs) based on DPA give pure blue emission with brightness up to 6,627 cd m−2 and turn-on voltage of 2.8 V. 2,6-Diphenylanthracene OLED arrays are successfully driven by DPA field-effect transistor arrays, demonstrating that DPA is a high mobility emissive organic semiconductor with potential in organic optoelectronics. PMID:26620323

Realizing Highly Efficient Solution-Processed Homojunction-Like Sky-Blue OLEDs by Using Thermally Activated Delayed Fluorescent Emitters Featuring an Aggregation-Induced Emission Property.

PubMed

Wu, Kailong; Wang, Zian; Zhan, Lisi; Zhong, Cheng; Gong, Shaolong; Xie, Guohua; Yang, Chuluo

2018-04-05

Two new blue emitters, i.e., bis-[2-(9,9-dimethyl-9,10-dihydroacridine)-phenyl]-sulfone ( o-ACSO2) and bis-[3-(9,9-dimethyl-9,10-dihydroacridine)-phenyl]-sulfone ( m-ACSO2), with reserved fine thermally activated delayed fluorescent (TADF) nature and simply tuned thermal and optoelectronic properties, were synthesized by isomer engineering. The meta-linking compound, i.e., m-ACSO2, obtains the highest photoluminescence quantum yield with a small singlet-triplet energy gap, a moderate delayed fluorescent lifetime, excellent solubility, and neat film homogeneity. Due to its unique aggregation-induced emission (AIE) character, neat film-based heterojunction-like organic light-emitting diodes (OLEDs) are achievable. By inserting an excitonic inert exciton-blocking layer, the PN heterojunction-like emission accompanied by intefacial exciplex was shifted to a homojunction-like channel mainly from the AIE emitter itself, providing a new tactic to generate efficient blue color from neat films. The solution-processed nondoped sky-blue OLED employing m-ACSO2 as emitter with homojunction-like emission achieved a maximum external quantum efficiency of 17.2%. The design strategies presented herein provide practical methods to construct efficient blue TADF dyes and realize high-performance blue TADF devices.

Synthesis and Characterization of Manganese Doped Silicon Nanoparticles

PubMed Central

Zhang, Xiaoming; Brynda, Marcin; Britt, R. David; Carroll, Elizabeth; Larsen, Delmar S.; Louie, Angelique Y.; Kauzlarich, Susan M.

2008-01-01

Mn doped Si nanoparticles have been synthesized via a low temperature solution route and characterize by X-ray powder diffraction, TEM, optical and emission spectroscopy and by EPR. The particle diameter was 4 nm and the surface was capped by octyl groups. 5% Mn doping resulted in a green emission with slightly lower quantum yield than undoped Si nanoparticles prepared by the same method. Mn2+ doped into the nanoparticle is confirmed by epr hyperfine and the charge carrier dynamics were probed by ultrafast transient absorption spectroscopy. Both techniques are consistent with Mn2+ on or close to the surface of the nanoparticle. PMID:17691792

Highly solid-state emissive pyridinium-substituted tetraphenylethylene salts: emission color-tuning with counter anions and application for optical waveguides.

PubMed

Hu, Fang; Zhang, Guanxin; Zhan, Chi; Zhang, Wei; Yan, Yongli; Zhao, Yongsheng; Fu, Hongbing; Zhang, Deqing

2015-03-18

In this paper seven salts of pyridinium-substituted tetraphenylethylene with different anions are reported. They show typical aggregation-induced emission. Crystal structures of three of the salts with (CF(3)SO(2))(2) N(-), CF(3) SO(3)(-), and SbF(6)(-) as the respective counter anions, are determined. The emission behavior of their amorphous and crystalline solids is investigated. Both amorphous and crystalline solids, except for the one with I(-), are highly emissive. Certain amorphous solids are red-emissive with almost the same quantum yields and fluorescence life-times. However, some crystalline solids are found to show different emission colors varying from green to yellow. Thus, their emission colors can be tuned by the counter anions. Furthermore, certain crystalline solids are highly emissive compared to the respective amorphous solids. Such solid-state emission behavior of these pyridinium-substituted tetraphenylethylene salts is interpreted on the basis of their crystal structures. In addition, optical waveguiding behavior of fabricated microrods is presented. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Purely organic electroluminescent material realizing 100% conversion from electricity to light

PubMed Central

Kaji, Hironori; Suzuki, Hajime; Fukushima, Tatsuya; Shizu, Katsuyuki; Suzuki, Katsuaki; Kubo, Shosei; Komino, Takeshi; Oiwa, Hajime; Suzuki, Furitsu; Wakamiya, Atsushi; Murata, Yasujiro; Adachi, Chihaya

2015-01-01

Efficient organic light-emitting diodes have been developed using emitters containing rare metals, such as platinum and iridium complexes. However, there is an urgent need to develop emitters composed of more abundant materials. Here we show a thermally activated delayed fluorescence material for organic light-emitting diodes, which realizes both approximately 100% photoluminescence quantum yield and approximately 100% up-conversion of the triplet to singlet excited state. The material contains electron-donating diphenylaminocarbazole and electron-accepting triphenyltriazine moieties. The typical trade-off between effective emission and triplet-to-singlet up-conversion is overcome by fine-tuning the highest occupied molecular orbital and lowest unoccupied molecular orbital distributions. The nearly zero singlet–triplet energy gap, smaller than the thermal energy at room temperature, results in an organic light-emitting diode with external quantum efficiency of 29.6%. An external quantum efficiency of 41.5% is obtained when using an out-coupling sheet. The external quantum efficiency is 30.7% even at a high luminance of 3,000 cd m−2. PMID:26477390

Nanophotonic photon echo memory based on rare-earth-doped crystals

NASA Astrophysics Data System (ADS)

Zhong, Tian; Kindem, Jonathan; Miyazono, Evan; Faraon, Andrei; Caltech nano quantum optics Team

2015-03-01

Rare earth ions (REIs) are promising candidates for implementing solid-state quantum memories and quantum repeater devices. Their high spectral stability and long coherence times make REIs a good choice for integration in an on-chip quantum nano-photonic platform. We report the coupling of the 883 nm transition of Neodymium (Nd) to a Yttrium orthosilicate (YSO) photonic crystal nano-beam resonator, achieving Purcell enhanced spontaneous emission by 21 times and increased optical absorption. Photon echoes were observed in nano-beams of different doping concentrations, yielding optical coherence times T2 up to 80 μs that are comparable to unprocessed bulk samples. This indicates the remarkable coherence properties of Nd are preserved during nanofabrication, therefore opening the possibility of efficient on-chip optical quantum memories. The nano-resonator with mode volume of 1 . 6(λ / n) 3 was fabricated using focused ion beam, and a quality factor of 3200 was measured. Purcell enhanced absorption of 80% by an ensemble of ~ 1 × 106 ions in the resonator was measured, which fulfills the cavity impedance matching condition that is necessary to achieve quantum storage of photons with unity efficiency.

The Application of Fluorescent Quantum Dots to Confocal, Multiphoton, and Electron Microscopic Imaging

PubMed Central

Deerinck, Thomas J.

2009-01-01

Fluorescent quantum dots are emerging as an important tool for imaging cells and tissues, and their unique optical and physical properties have captured the attention of the research community. The most common types of commercially available quantum dots consist of a nanocrystalline semiconductor core composed of cadmium selenide with a zinc sulfide capping layer and an outer polymer layer to facilitate conjugation to targeting biomolecules such as immunoglobulins. They exhibit high fluorescent quantum yields and have large absorption cross-sections, possess excellent photostability, and can be synthesized so that their narrow-band fluorescence emission can occur in a wide spectrum of colors. These properties make them excellent candidates for serving as multiplexing molecular beacons using a variety of imaging modalities including highly correlated microscopies. Whereas much attention has been focused on quantum-dot applications for live-cell imaging, we have sought to characterize and exploit their utility for enabling simultaneous multiprotein immunolabeling in fixed cells and tissues. Considerations for their application to immunolabeling for correlated light and electron microscopic analysis are discussed. PMID:18337229

Integrated photonics using colloidal quantum dots

NASA Astrophysics Data System (ADS)

Menon, Vinod M.; Husaini, Saima; Okoye, Nicky; Valappil, Nikesh V.

2009-11-01

Integrated photonic devices were realized using colloidal quantum dot composites such as flexible microcavity laser, microdisk emitters and integrated active-passive waveguides. The microcavity laser structure was realized using spin coating and consisted of an all-polymer distributed Bragg reflector with a poly-vinyl carbazole cavity layer embedded with InGaP/ZnS colloidal quantum dots. These microcavities can be peeled off the substrate yielding a flexible structure that can conform to any shape and whose emission spectra can be mechanically tuned. Planar photonic devices consisting of vertically coupled microring resonators, microdisk emitters, active-passive integrated waveguide structures and coupled active microdisk resonators were realized using soft lithography, photo-lithography, and electron beam lithography, respectively. The gain medium in all these devices was a composite consisting of quantum dots embedded in SU8 matrix. Finally, the effect of the host matrix on the optical properties of the quantum dots using results of steady-state and time-resolved luminescence measurements was determined. In addition to their specific functionalities, these novel device demonstrations and their development present a low-cost alternative to the traditional photonic device fabrication techniques.

Photonic emitters and circuits based on colloidal quantum dot composites

NASA Astrophysics Data System (ADS)

Menon, Vinod M.; Husaini, Saima; Valappil, Nikesh; Luberto, Matthew

2009-02-01

We discuss our work on light emitters and photonic circuits realized using colloidal quantum dot composites. Specifically we will report our recent work on flexible microcavity laser, microdisk emitters and integrated active - passive waveguides. The entire microcavity laser structure was realized using spin coating and consisted of an all-polymer distributed Bragg reflector with a poly-vinyl carbazole cavity layer embedded with InGaP/ZnS colloidal quantum dots. These microcavities can be peeled off the substrate yielding a flexible structure that can conform to any shape and whose emission spectra can be mechanically tuned. The microdisk emitters and the integrated waveguide structures were realized using soft lithography and photo-lithography, respectively and were fabricated using a composite consisting of quantum dots embedded in SU8 matrix. Finally, we will discuss the effect of the host matrix on the optical properties of the quantum dots using results of steady-state and time-resolved luminescence measurements. In addition to their specific functionalities, these novel device demonstrations and their development present a low cost alternative to the traditional photonic device fabrication techniques.

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.

Multiple exciton generation in cluster-free alloy Cd(x)Hg(1-x)Te colloidal quantum dots synthesized in water.

PubMed

Kershaw, Stephen V; Kalytchuk, Sergii; Zhovtiuk, Olga; Shen, Qing; Oshima, Takuya; Yindeesuk, Witoon; Toyoda, Taro; Rogach, Andrey L

2014-12-21

A number of different composition CdxHg1-xTe alloy quantum dots have been synthesized using a modified aqueous synthesis and ion exchange method. The benefits of good stoichiometric control and high emission quantum yield were retained whilst also ensuring that the tendency to form gel-like clusters and adsorb excess cations in the stabilizing ligand shells was mitigated using a sequestering method to remove excess ionic material during and after the synthesis. This was highly desirable for ultrafast carrier dynamics measurements, avoiding strong photocharging effects which may mask fundamental carrier signals. Transient grating measurements revealed a composition dependent carrier multiplication process which competes with phonon mediated carrier cooling to deplete the initial hot carrier population. The interplay between these two mechanisms is strongly dependent on the electron effective mass which in these alloys has a marked composition dependence and may be considerably lower than the hole effective mass. For a composition x = 0.52 we measured a maximum carrier multiplication quantum yield of 199 ± 19% with pump photon energy 3 times the bandgap energy, Eg, whilst the threshold energy is calculated to be just 2.15Eg. There is some evidence to suggest an impact ionization process analogous to the inverse Auger S mechanism seen in bulk CdxHg1-xTe.

Blue light emission from cyclometallated iridium (III) cyano complexes: Syntheses, crystal structures, and photophysical properties

DOE PAGES

Sanner, Robert D.; Cherepy, Nerine J.; Young, Jr., Victor G.

2015-11-02

In this study, we describe the synthesis and crystal structures of four iridium compounds containing the 2-(4,6-difluorophenyl)pyridyl ligand. Cleavage of dichloro-bridged iridium(III) dimers with phosphorus ligands leads to (46dfppy)2Ir(L)(Cl) where L = PPh 3 or P(OPh) 3. Treatment of the chloro compounds with cyanide forms the cyano complexes (46dfppy) 2Ir(L)(CN). All complexes exhibit a trans effect in their molecular structures due to the phosphorus ligands, with the phosphite having a greater effect than the phosphine. With L = PPh 3, blue photoluminescence with CIE coordinates (x = 0.16, y = 0.24), quantum yield of 0.66 ± 0.15 and 4.5 ±more » 0.5 μs decay time is measured. For L = P(OPh) 3, blue photoluminescence with CIE coordinates (x = 0.16, y = 0.21), quantum yield of 0.65 ± 0.15 and 2.9 ± 0.3 μs decay time is measured.« less

Substituent effect on photophysical properties of bi-1,3,4-oxadiazole derivatives in solution

NASA Astrophysics Data System (ADS)

Chen, Fangyi; Tian, Taiji; Zhao, Chengxiao; Bai, Binglian; Li, Min; Wang, Haitao

2016-04-01

A series of phenyl substituted bi-1,3,4-oxadiazole derivatives were designed and synthesized; the effect of substituent on the photophysical properties and molecular electronic structures was fully studied by the combination of experimental techniques and theoretical calculations. Compared to parent compound without any substituent (BOXD), fluoro-substituent shows little effect on the absorption and emission spectra, whilst a little larger spectral red-shift could be observed for methoxy-, nitro-substituted derivatives and thienyl-substituted bi-1,3,4-oxadiazole (TBOXD). These spectral changes can be well explained by theoretically calculated HOMO and LUMO energy level changes. All these molecules show high fluorescence quantum yield except for nitro-substituted derivative in dilute solutions. The quantum yield of BOXD changes with the concentration and exhibits a high value at the concentrated solution. This work revealed the influence of substituent on the photophysical properties of bi-1,3,4-oxadizaole derivatives in dilute solutions and provided guidance for designing molecules with potential application.

Some fluorescence properties of dimethylaminochalcone and its novel cyclic analogues

NASA Astrophysics Data System (ADS)

Tomečková, Vladimíra; Poškrobová, Martina; Štefanišinová, Miroslava; Perjési, Pál

2009-12-01

This paper demonstrates the basic character (polarity, solubility, colour, absorption and fluorescence quantum yield) of synthetic dimethylaminochalcone ( 1) and its cyclic analogues measured in toluene, chloroform, dimethylsulfoxide and ethanol, which have been studied by absorption and fluorescence spectroscopy. The biologically active dye 4'-dimethylaminochalcone ( 1b) and its less flexible analogues 4-dimethylaminoindanone ( 2b), -tetralone ( 3b), and -benzosuberone ( 4b) are lipophilic molecules that displayed the best solubility in toluene and chloroform. The highest fluorescence and quantum yields of compounds 1 and 2 have been obtained in DMSO and chloroform. Quenching effect of fluorescence compounds ( 1- 4) has been studied in the mixture of the most polar organic solvents DMSO and water. In the presence of water, fluorescence of compound 1 has been quenched the best from all studied chalcones and emission maxima of molecules 1- 4 have been shifted to the longer wavelengths. Quenching effect of fluorescence by water was in order 1 > 2 > 3 > 4.

Blue phosphorescent nitrile containing C^C* cyclometalated NHC platinum(II) complexes.

PubMed

Tronnier, Alexander; Metz, Stefan; Wagenblast, Gerhard; Muenster, Ingo; Strassner, Thomas

2014-02-28

Since C^C* cyclometalated Pt(II) complexes with N-heterocyclic carbene (NHC) ligands have been identified as potential emitter materials in organic light-emitting devices (OLEDs), very promising results regarding quantum yields, colour and stability have been presented. Herein, we report on four nitrile substituted complexes with a chelating NHC ligand (1-(4-cyanophenyl)-3-isopropyl-1H-benzo[d]imidazole or 4-(tert-butyl)-1-(4-cyanophenyl)-3-methyl-1H-imidazole) and a bidentate monoanionic auxiliary ligand (acetylacetone or dimesitoylmethane). The complexes have been fully characterized including extensive 2D NMR studies (COSY, HSQC, HMBC, NOESY, (195)Pt NMR), three of them also by solid-state structures. Photophysical measurements in amorphous PMMA films and pure emitter films at room temperature reveal the impact of the mesityl groups in the auxiliary ligand, which led to a significant increase of the quantum yield, while the decay lifetimes decreased. The electron withdrawing nitrile groups shift the emission towards blue colour coordinates.

Chemiluminescence reactions with cationic, neutral, and anionic ruthenium(II) complexes containing 2,2'-bipyridine and bathophenanthroline disulfonate ligands.

PubMed

Francis, Paul S; Papettas, Dimitra; Zammit, Elizabeth M; Barnett, Neil W

2010-07-15

Ruthenium complexes containing 4,7-diphenyl-1,10-phenanthroline disulfonate (bathophenanthroline disulfonate; BPS) ligands, Ru(BPS)(3)(4-), Ru(BPS)(2)(bipy)(2-) and Ru(BPS)(bipy)(2), were compared to tris(2,2'-bipyridine)ruthenium(II) (Ru(bipy)(3)(2+)), including examination of the wavelengths of maximum absorption and corrected emission intensity, photoluminescence quantum yield, stability of their oxidised ruthenium(III) form, and relative chemiluminescence intensities and signal-to-blank ratios with cerium(IV) sulfate and six analytes (codeine, morphine cocaine, potassium oxalate, furosemide and hydrochlorothiazide) in acidic aqueous solution. The presence of BPS ligands in the complex increased the photoluminescence quantum yield, but decreased the stability of the oxidised form of the reagent. In contrast to previous evidence showing much greater electrochemiluminescence intensities using Ru(BPS)(2)(bipy)(2-) and Ru(BPS)(bipy)(2), these complexes did not provide superior chemiluminescence signals than their homoleptic analogues. Copyright 2010 Elsevier B.V. All rights reserved.

Formation of hemoglobin photoproduct is responsible for two-photon and single photon-excited fluorescence of red blood cells

NASA Astrophysics Data System (ADS)

Shirshin, Evgeny A.; Yakimov, Boris P.; Rodionov, Sergey A.; Omelyanenko, Nikolai P.; Priezzhev, Alexander V.; Fadeev, Victor V.; Lademann, Juergen; Darvin, Maxim E.

2018-07-01

Two-photon excited fluorescence of red blood cells (RBC) has been reported to be applicable for their assessment in vitro and in vivo. The corresponding fluorescence emission was ascribed to hemoglobin (Hb), however, as Hb is essentially non-fluorescent at single-photon excitation, the mechanism of two-photon excited fluorescence of RBC remains debatable. Here we show that a fluorescent photoproduct, characterized by an ultrafast decay of excitation, is formed after irradiation of Hb with femtosecond laser pulses with ca. 8 · 10‑5 quantum yield, and that it is also fluorescent at single-photon excitation. The formation of a similar photoproduct was also shown for Hb continuous wave irradiation with blue light with ca. 10‑5 formation quantum yield. The kinetics of the Hb photoproduct formation and its spectral properties were investigated. The obtained results clarify the processes responsible for RBC fluorescence observed in two-photon microscopy experiments.

Synthesis and spectral characterization of environmentally responsive fluorescent deoxycytidine analogs

PubMed Central

Elmehriki, Adam AH; Suchý, Mojmír; Chicas, Kirby J; Wojciechowski, Filip; Hudson, Robert HE

2014-01-01

Herein, we describe the synthesis and spectroscopic properties of five novel pyrrolodeoxycytidine analogs, and the related 5-(1-pyrenylethynyl)-2’-deoxycytidine analog; as well as fluorescence characterization of 5-(p-methoxyphenylethynyl)-2’-deoxyuridine. Within this series of compounds, rigidification of the structure from 6-phenylpyrrolodeoxycytidine to 5,6-benzopyrroldeoxycytidine made remarkable improvement of the fluorescence quantum yield (Φ ~1, EtOH) and substantially increased the Stokes shift. Exchange of the phenyl group of 6-phenylpyrrolodeoxycytidine for other heterocycles (benzofuryl or indolyl) produced an increase in the extinction coefficient at the excitation wavelength while preserving high quantum yields. The steady-state fluorescence response to the environment was determined by sensitivity of Stokes shift to solvent polarity. The effect of solvent polarity on fluorescence emission intensity was concurrently examined and showed that 5,6-benzopyrrolodeoxycytidine is highly sensitive to the presence of water. On the other hand, the previously synthesized 5-(p-methoxyphenylethynyl)-2’-deoxyuridine was found to be sensitive to solvent viscosity indicating molecular rotor behavior. PMID:25483932

Tunable Optical Properties and Increased Thermal Quenching in the Blue-Emitting Phosphor Series: Ba 2 (Y 1–x Lu x ) 5 B 5 O 17 :Ce 3+ ( x = 0–1)

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

Hermus, Martin; Phan, Phu-Cuong; Duke, Anna C.

The preparation of cerium-substituted barium lutetium borate, Ba2Lu5B5O17:Ce3+, is achieved using high temperature solid state synthesis. This compound crystallizes in the Ba2Y5B5O17-type structure and shows an efficient blue emission (λmax = 447 nm) when excited by UV-light (λex = 340 nm) with a photoluminescent quantum yield near 90%, a fast luminescence decay time (<40 ns), and a thermal quenching temperature of 452 K. Further, preparing a solid solution following Ba2(Y1–xLux)5B5O17:Ce3+ (x = 0, 0.25, 0.50, 0.75, 1) confirms that all compounds are isostructural and follow Vegard’s law. Substituting Y3+ for Lu3+ yields a nearly constant emission spectrum that blue-shifts bymore » only 9 nm and has a consistent luminescence lifetime across the range prepared. The photoluminescent quantum yield (PLQY) and thermal quenching (T50) of the solid solution, however, are dramatically impacted by the composition, with the PLQY decreasing to ≈70% and the T50 dropping 49 K going from x = 1 to x = 0. These significant changes in the optical properties likely stem from enhanced structural rigidity as the larger, more polarizable Y3+ is substituted for the smaller, harder Lu3+ cation. These results highlight the importance of optimizing chemical bonding to improve a phosphor’s optical properties.« less

Polarization control of spontaneous emission for rapid quantum-state initialization

NASA Astrophysics Data System (ADS)

DiLoreto, C. S.; Rangan, C.

2017-04-01

We propose an efficient method to selectively enhance the spontaneous emission rate of a quantum system by changing the polarization of an incident control field, and exploiting the polarization dependence of the system's spontaneous emission rate. This differs from the usual Purcell enhancement of spontaneous emission rates as it can be selectively turned on and off. Using a three-level Λ system in a quantum dot placed in between two silver nanoparticles and a linearly polarized, monochromatic driving field, we present a protocol for rapid quantum state initialization, while maintaining long coherence times for control operations. This process increases the overall amount of time that a quantum system can be effectively utilized for quantum operations, and presents a key advance in quantum computing.

The effect of precursor on the optical properties of carbon quantum dots synthesized by hydrothermal/solvothermal method

NASA Astrophysics Data System (ADS)

Mozdbar, Afsaneh; Nouralishahi, Amideddin; Fatemi, Shohreh; Mirakhori, Ghazaleh

2018-01-01

In the recent decade, Carbon Quantum Dots (CQDs) have attracted lots of attention due to their excellent properties such as tunable photoluminescence, high chemical stability, low toxicity, and biocompatibility. Among all synthesis methods, the hydrothermal/solvothermal rout has been considered as one of the most common and simplest method. The type of precursors can affect the size of CQDs and determine their surface functional groups, the essential properties that deeply influence the optical specifications. In this work, the effect of different precursors on the final properties of carbon quantum dots is investigated. The carbon quantum dots were synthesized by hydrothermal/solvothermal rout using citric acid, thiourea, ethylamine and monoethanolamine as precursors in almost the same conditions of time and temperature. Resultant CQDs were characterized by using FTIR, UV-Visible Spectroscopy and Photoluminescence (PL) analysis. The results of UV-Vis spectroscopy showed that quantum dots synthesized from monoethanolamine have wider absorption band rather than the CQDs from other precursors and the absorption edge shifted from about 270 nm for ethylamine to about 470 nm in monoethanolamine. Furthermore, the results demonstrate that using citric acid and monoethanolamine as precursor improved production efficiency and emission quantum yield of the carbon dots.

Complete Quantum Control of a Single Silicon-Vacancy Center in a Diamond Nanopillar

NASA Astrophysics Data System (ADS)

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan-Kai; Dory, Constantin; Radulaski, Marina; Kelaita, Yousif; Shen, Zhi-Xun; Melosh, Nicholas A.; Chu, Steven; Vuckovic, Jelena

Coherent quantum control of a quantum bit (qubit) is an important step towards its use in a quantum network. SiV- center in diamond offers excellent physical qualities such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the fast spin manipulation and techniques to extend the spin coherence time are under active investigation. Here, we demonstrate full coherent control over the state of a single SiV- center in a diamond nanopillar using ultrafast optical pulses. The high quality of the chemical vapor deposition grown SiV- centers allows us to coherently manipulate and quasi-resonantly read out the state of the single SiV- center. Moreover, the SiV- centers being coherently controlled are integrated into diamond nanopillar arrays in a site-controlled, individually addressable manner with high yield, low strain, and high spectral stability, which paves the way for scalable on chip optically accessible quantum system in a quantum photonic network. Financial support is provided by the DOE Office of Basic Energy Sciences, Division of Materials Sciences through Stanford Institute for Materials and Energy Sciences (SIMES) under contract DE-AC02-76SF00515.

High-efficiency tris(8-hydroxyquinoline)aluminum (Alq3) complexes for organic white-light-emitting diodes and solid-state lighting.

PubMed

Pérez-Bolívar, César; Takizawa, Shin-ya; Nishimura, Go; Montes, Victor A; Anzenbacher, Pavel

2011-08-08

Combinations of electron-withdrawing and -donating substituents on the 8-hydroxyquinoline ligand of the tris(8-hydroxyquinoline)aluminum (Alq(3)) complexes allow for control of the HOMO and LUMO energies and the HOMO-LUMO gap responsible for emission from the complexes. Here, we present a systematic study on tuning the emission and electroluminescence (EL) from Alq(3) complexes from the green to blue region. In this study, we explored the combination of electron-donating substituents on C4 and C6. Compounds 1-6 displayed the emission tuning between 478 and 526 nm, and fluorescence quantum yield between 0.15 and 0.57. The compounds 2-6 were used as emitters and hosts in organic light-emitting diodes (OLEDs). The highest OLED external quantum efficiency (EQE) observed was 4.6%, which is among the highest observed for Alq(3) complexes. Also, the compounds 3-5 were used as hosts for red phosphorescent dopants to obtain white light-emitting diodes (WOLED). The WOLEDs displayed high efficiency (EQE up to 19%) and high white color purity (color rendering index (CRI≈85). Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Structural control of InP/ZnS core/shell quantum dots enables high-quality white LEDs.

PubMed

Kumar, Baskaran Ganesh; Sadeghi, Sadra; Melikov, Rustamzhon; Aria, Mohammad Mohammadi; Jalali, Houman Bahmani; Ow-Yang, Cleva W; Nizamoglu, Sedat

2018-08-24

Herein, we demonstrate that the structural and optical control of InP-based quantum dots (QDs) can lead to high-performance light-emitting diodes (LEDs). Zinc sulphide (ZnS) shells passivate the InP QD core and increase the quantum yield in green-emitting QDs by 13-fold and red-emitting QDs by 8-fold. The optimised QDs are integrated in the liquid state to eliminate aggregation-induced emission quenching and we fabricated white LEDs with a warm, neutral and cool-white appearance by the down-conversion mechanism. The QD-functionalized white LEDs achieve luminous efficiency (LE) up to 14.7 lm W -1 and colour-rendering index up to 80. The structural and optical control of InP/ZnS core/shell QDs enable 23-fold enhancement in LE of white LEDs compared to ones containing only QDs of InP core.

High power cascade diode lasers emitting near 2 μm

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

Hosoda, Takashi; Feng, Tao; Shterengas, Leon, E-mail: leon.shterengas@stonybrook.edu

2016-03-28

High-power two-stage cascade GaSb-based type-I quantum well diode lasers emitting near 2 μm were designed and fabricated. Coated devices with cavity length of 3 mm generated about 2 W of continuous wave power from 100-μm-wide aperture at the current of 6 A. The power conversion efficiency peaked at 20%. Carrier recycling between quantum well gain stages was realized using band-to-band tunneling in GaSb/AlSb/InAs heterostructure complemented with optimized electron and hole injector regions. Design optimization eliminated parasitic optical absorption and thermionic emission, and included modification of the InAs quantum wells of electron and composition and doping profile of hole injectors. Utilization of the cascade pumpingmore » scheme yielded 2 μm lasers with improved output power and efficiency compared to existing state-of-the-art diodes.« less

Strategy for synthesizing quantum dot-layered double hydroxide nanocomposites and their enhanced photoluminescence and photostability.

PubMed

Cho, Seungho; Jung, Sungwook; Jeong, Sanghwa; Bang, Jiwon; Park, Joonhyuck; Park, Youngrong; Kim, Sungjee

2013-01-08

Layered double hydroxide-quantum dot (LDH-QD) composites are synthesized via a room temperature LDH formation reaction in the presence of QDs. InP/ZnS (core/shell) QD, a heavy metal free QD, is used as a model constituent. Interactions between QDs (with negative zeta potentials), decorated with dihydrolipoic acids, and inherently positively charged metal hydroxide layers of LDH during the LDH formations are induced to form the LDH-QD composites. The formation of the LDH-QD composites affords significantly enhanced photoluminescence quantum yields and thermal- and photostabilities compared to their QD counterparts. In addition, the fluorescence from the solid LDH-QD composite preserved the initial optical properties of the QD colloid solution without noticeable deteriorations such as red-shift or deep trap emission. Based on their advantageous optical properties, we also demonstrate the pseudo white light emitting diode, down-converted by the LDH-QD composites.

Emission switching of 4,6-diphenylpyrimidones: solvent and solid state effects.

PubMed

Adjaye-Mensah, Edward; Gonzalez, Walter G; Bussé, David R; Captain, Burjor; Miksovska, Jaroslava; Wilson, James N

2012-08-30

The photophysics of 1-ethyl-4,6-bis(4-methoxyphenyl)-2(1H)-pyrimidone (1) and 1-ethyl-4,6-bis(4-(dimethylamino)phenyl)-2(1H)-pyrimidone (2) were investigated to determine the mechanisms of emission switching in response to protonation. UV-vis and steady state emission spectroscopy of the protonated and unprotonated forms across a range of solvents reveal the polarity dependence of the vertical excitation energies. Emission lifetimes and quantum yields show the solvent dependency of the excited states. Emission enhancements were observed in polyethylene glycol solutions and in the solid state (both thin film and single crystal), demonstrating the role of intramolecular rotation in thermal relaxation of the excited states. TD-DFT calculations provide insights into the excited state geometries and the role of intramolecular charge transfer. The collected data show that emission of diphenylpyrimidones can be modulated by four factors, including the identity of the electron-donating auxochrome, protonation state, solvent polarity, and viscosity.

Model study of greenline dayglow emission under geomagnetic storm conditions.

NASA Astrophysics Data System (ADS)

Singh, V.; Bag, T.; Sunil Krishna, M. V.

2016-12-01

A comprehensive model is developed to study the influences of geomagnetic storms on greenline (557.7 nm) dayglow emission during the solar active and solar quiet conditions in thermosphere. This study is based on a photochemical model which is developed using the latest reaction rate coefficients, quantum yields and collisional cross-sections obtained from the experimental observations and empirical models. This study is for a low latitude station Tirunelveli (8.7N,77.8E), India. The volume emission rate (VER) has been calculated using the densities and temperature from NRLMSISE-00 and IRI-2012 models. The modeled VER shows a positive correlation with the Dst index, and a negative correlation with the number densities of O, O2, and N2. The VER calculated at the peak emission altitude shows depletion during the main phase of the storm. The peak emission altitude doesn't show any appreciable variation during storm period. On the other hand, the peak emission altitude shows an upward movement with the increase in F10.7 solar index.

Physicochemical Investigation of 2,4,5-Trimethoxybenzylidene Propanedinitrile (TMPN) Dye as Fluorescence off-on Probe for Critical Micelle Concentration (CMC) of SDS and CTAB.

PubMed

Khan, Salman A; Asiri, Abdullah M

2015-11-01

2,4,5-trimethoxybenzylidene propanedinitrile (TMPN) was synthesized by Knoevenagel condensation. Structure of the TMPN was conformed by the elemental analysis and EI-MS, FT-IR, (1)H-NMR, (13)C-NMR spectroscopy. Absorbance and emission spectrum of the TMPN was studied in different solvent provide that TMPN is good absorbent and emission red shift in absorbance and emission spectra as polarity of the solvents increase. Photophysical properties including, oscillator strength, extinction coefficient, transition dipole moment, stokes shift and fluorescence quantum yield were investigated in order to investigate the physicochemical behaviors of TMPN. Dye undergoes solubilization in different micelles and may be used as a probe to determine the critical micelle concentration (CMC) of SDS and CTAB.

Color-tunable, aggregation-induced emission of a butterfly-shaped molecule comprising a pyran skeleton and two cholesteryl wings.

PubMed

Tong, Hui; Hong, Yuning; Dong, Yongqiang; Ren, Yan; Häussler, Matthias; Lam, Jacky W Y; Wong, Kam Sing; Tang, Ben Zhong

2007-03-01

A chiral pyran derivative containing two cholesteryl groups (1) is synthesized, and its optical properties are investigated. Whereas the isolated molecule of 1 is virtually nonluminescent in dilute solutions, it becomes highly emissive with a 2 orders of magnitude increase in fluorescence quantum yield upon aggregation in poor solvents or in solid state, showing a novel phenomenon of aggregation-induced emission (AIE). The color and efficiency of the AIE of 1 can be tuned by varying the morphology of its aggregates: photoluminescence of its aggregates formed in a tetrahydrofuran/water mixture progressively red-shifts (green --> yellow --> red) with increasing water content of the mixture, with the crystalline aggregates emitting bluer lights in higher efficiencies than their amorphous counterparts.

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.

Beneficial effects of water in the colloidal synthesis of InP/ZnS core-shell quantum dots for optoelectronic applications.

PubMed

Ramasamy, Parthiban; Kim, Bumjin; Lee, Min-Sang; Lee, Jong-Soo

2016-10-21

We demonstrate that the presence of a small amount of water as an impurity during the hot-injection synthesis can significantly decrease the emission lines full width at half-maximum (FWHM) and improve the quantum yield (QY) of InP/ZnS quantum dots (QDs). By utilizing the water present in the indium precursor and solvent, we obtained InP/ZnS QDs emitting around 530 nm with a FWHM as narrow as 46 nm and a QY up to 45%. Without water, the synthesized QDs have emission around 625 nm with a FWHM of 66 nm and a QY of about 33%. Absorption spectra, XRD and XPS analyses revealed that when water is present, an amorphous phosphate layer is formed over the InP QDs and inhibits the QD growth. This amorphous layer favors the formation of a very thick ZnS shell by decreasing the lattice mismatch between the InP core and the ZnS shell. We further show the possibility to tune the emission wavelengths of InP/ZnS QDs by simply adjusting the amount of water present in the system while keeping all the other reaction parameters (i.e., precursor concentration, reaction temperature and time) constant. As an example of their application in light-emitting diodes (LEDs), the green and red InP/ZnS QDs are combined with a blue LED chip to produce white light.

Absorption and emission behaviour of trans- p-coumaric acid in aqueous solutions and some organic solvents

NASA Astrophysics Data System (ADS)

Putschögl, M.; Zirak, P.; Penzkofer, A.

2008-01-01

The absorption and fluorescence behaviour of trans- p-coumaric acid ( trans-4-hydroxycinnamic acid) is investigated in buffered aqueous solution over a wide range from pH 1 to pH 12, in un-buffered water, and in some organic solvents. Absorption cross-section spectra, fluorescence quantum distributions, fluorescence quantum yields, and degrees of fluorescence polarisation are measured. p-Coumaric acid exists in different ionic forms in aqueous solution depending on the pH. There is an equilibrium between the neutral form ( p-CAH 2) and the single anionic form ( p-CAH -) at low pH (p Kna ≈ 4.9), and between the single anionic and the double anionic form ( p-CA 2-) at high pH (p Kaa ≈ 9.35). In the organic solvents studied trans- p-coumaric acid is dissolved in its neutral form. The fluorescence quantum yield of trans- p-coumaric acid in aqueous solution is ϕF ≈ 1.4 × 10 -4 for the neutral and the single anionic form, while it is ϕF ≈ 1.3 × 10 -3 for the double anionic form. For trans- p-coumaric acid in organic solvents fluorescence quantum yields in the range from 4.8 × 10 -5 (acetonitrile) to 1.5 × 10 -4 (glycerol) were measured. The fluorescence spectra are 7700-10,000 cm -1 Stokes shifted in aqueous solution, and 5400-8200 cm -1 Stokes shifted in the studied organic solvents. Decay paths responsible for the low fluorescence quantum yields are discussed (photo-isomerisation and internal conversion for p-CA 2-, solvent-assisted intra-molecular charge-transfer or ππ ∗ to nπ ∗ transfer and internal conversion for p-CAH 2 and p-CAH -). The solvent dependence of the first ππ ∗ electronic transition frequency and of the fluorescence Stokes shift of p-CAH 2 is discussed in terms of polar solute-solvent interaction effects. Thereby the ground-state and excite-state molecular dipole moments are extracted.

Functionalization of quantum rods with oligonucleotides for programmable assembly with DNA origami

NASA Astrophysics Data System (ADS)

Doane, Tennyson L.; Alam, Rabeka; Maye, Mathew M.

2015-02-01

The DNA-mediated self-assembly of CdSe/CdS quantum rods (QRs) onto DNA origami is described. Two QR types with unique optical emission and high polarization were synthesized, and then functionalized with oligonucleotides (ssDNA) using a novel protection-deprotection approach, which harnessed ssDNA's tailorable rigidity and denaturation temperature to increase DNA coverage by reducing non-specific coordination and wrapping. The QR assembly was programmable, and occurred at two different assembly zones that had capture strands in parallel alignment. QRs with different optical properties were assembled, opening up future studies on orientation dependent QR FRET. The QR-origami conjugates could be purified via gel electrophoresis and sucrose gradient ultracentrifugation. Assembly yields, QR stoichiometry and orientation, as well as energy transfer implications were studied in light of QR distances, origami flexibility, and conditions.The DNA-mediated self-assembly of CdSe/CdS quantum rods (QRs) onto DNA origami is described. Two QR types with unique optical emission and high polarization were synthesized, and then functionalized with oligonucleotides (ssDNA) using a novel protection-deprotection approach, which harnessed ssDNA's tailorable rigidity and denaturation temperature to increase DNA coverage by reducing non-specific coordination and wrapping. The QR assembly was programmable, and occurred at two different assembly zones that had capture strands in parallel alignment. QRs with different optical properties were assembled, opening up future studies on orientation dependent QR FRET. The QR-origami conjugates could be purified via gel electrophoresis and sucrose gradient ultracentrifugation. Assembly yields, QR stoichiometry and orientation, as well as energy transfer implications were studied in light of QR distances, origami flexibility, and conditions. Electronic supplementary information (ESI) available: Experimental conditions, DNA origami blueprint and sequences, FRET calculations. Additional Fig. S1-S13. See DOI: 10.1039/c4nr07662a

Long Wavelength Excitation of Europium Luminescence in Extended, Carboline-Based Cryptates.

PubMed

Dee, Carolin; Esteban-Gómez, David; Platas-Iglesias, Carlos; Seitz, Michael

2018-06-05

Two new β-carboline-based tris(biaryl) europium cryptates are introduced. The extended antenna moiety incorporated into the cryptand frameworks enables the sensitization of europium emission with excitation wavelengths well above 450 nm. In aqueous solution, the cryptates show great complex stability, luminescence lifetimes around 0.5 ms, and absolute quantum yields of ca. 3%. In addition, the europium luminescence shows a well-defined pH-dependence in the physiologically interesting pH range 7-9.

Fluorescence Properties of Dansyl Groups Covalently Bonded to the Surface of Oxidatively Functionalized Low-Density Polyethylene Film.

DTIC Science & Technology

1985-12-01

Weissberger, A.; Rossiter, B. W., Eds.; Wiley-Interscience: New York, 1972; p 575. *16) This value is based on studies of self-assembled Langmuir - Blodgett ... liquids . The Dansyl group was chosen because its fluorescence emission maximum and quantum yield are sensitive to the polarity and acidity of the local...environment. The wavelength of maximum fluorescence depended only weakly on the character of the contacting liquid phase; the difference between

Bichromophoric dyes for wavelength shifting of dye-protein fluoromodules.

PubMed

Pham, Ha H; Szent-Gyorgyi, Christopher; Brotherton, Wendy L; Schmidt, Brigitte F; Zanotti, Kimberly J; Waggoner, Alan S; Armitage, Bruce A

2015-03-28

Dye-protein fluoromodules consist of fluorogenic dyes and single chain antibody fragments that form brightly fluorescent noncovalent complexes. This report describes two new bichromophoric dyes that extend the range of wavelengths of excitation or emission of existing fluoromodules. In one case, a fluorogenic thiazole orange (TO) was attached to an energy acceptor dye, Cy5. Upon binding to a protein that recognizes TO, red emission due to efficient energy transfer from TO to Cy5 replaces the green emission observed for monochromophoric TO bound to the same protein. Separately, TO was attached to a coumarin that serves as an energy donor. The same green emission is observed for coumarin-TO and TO bound to a protein, but efficient energy transfer allows violet excitation of coumarin-TO, versus longer wavelength, blue excitation of monochromophoric TO. Both bichromophores exhibit low nanomolar KD values for their respective proteins, >95% energy transfer efficiency and high fluorescence quantum yields.

Bichromophoric Dyes for Wavelength Shifting of Dye-Protein Fluoromodules

PubMed Central

Pham, Ha H.; Szent-Gyorgyi, Christopher; Brotherton, Wendy L.; Schmidt, Brigitte F.; Zanotti, Kimberly J.; Waggoner, Alan S.

2015-01-01

Dye-protein fluoromodules consist of fluorogenic dyes and single chain antibody fragments that form brightly fluorescent noncovalent complexes. This report describes two new bichromophoric dyes that extend the range of wavelengths of excitation or emission of existing fluoromodules. In one case, a fluorogenic thiazole orange (TO) was attached to an energy acceptor dye, Cy5. Upon binding to a protein that recognizes TO, red emission due to efficient energy transfer from TO to Cy5 replaces the green emission observed for monochromophoric TO bound to the same protein. Separately, TO was attached to a coumarin that serves as an energy donor. The same green emission is observed for coumarin-TO and TO bound to a protein, but efficient energy transfer allows violet excitation of coumarin-TO, versus longer wavelength, blue excitation of monochromophoric TO. Both bichromophores exhibit low nanomolar KD values for their respective proteins, >95% energy transfer efficiency and high fluorescence quantum yields. PMID:25679477

Atomic Oxygen Tailored Graphene Oxide Nanosheets Emissions for Multicolor Cellular Imaging.

PubMed

Mei, Qingsong; Chen, Jian; Zhao, Jun; Yang, Liang; Liu, Bianhua; Liu, Renyong; Zhang, Zhongping

2016-03-23

Graphene oxide (GO) has been widely used as a fluorescence quencher, but its luminescent properties, especially tailor-made controlling emission colors, have been seldom reported due to its heterogeneous structures. Herein, we demonstrated a novel chemical oxidative strategy to tune GO emissions from brown to cyan without changing excitation wavelength. The precise tuning is simply achieved by varying reaction times of GO nanosheets in piranha solution, but there is no need for complex chromatography separation procedures. With increasing reaction times, oxygen content on the lattice of GO nanosheets increased, accompanied by the diminution of their sizes and sp(2) conjugation system, resulting in an increase of emissive carbon cluster-like states. Thereby, the luminescent colors of GO were tuned from brown to yellow, green, and cyan, and its fluorescent quantum yields were enhanced. The obtained multicolored fluorescent GO nanosheets would open plenty of novel applications in cellular imaging and multiplex encoding analysis.

Optimization via specific fluorescence brightness of a receptor-targeted probe for optical imaging and positron emission tomography of sentinel lymph nodes

PubMed Central

Qin, Zhengtao; Hall, David J.; Liss, Michael A.; Hoh, Carl K.; Kane, Christopher J.; Wallace, Anne M.

2013-01-01

Abstract. The optical properties of a receptor-targeted probe designed for dual-modality mapping of the sentinel lymph node (SLN) was optimized. Specific fluorescence brightness was used as the design criterion, which was defined as the fluorescence brightness per mole of the contrast agent. Adjusting the molar ratio of the coupling reactants, IRDye 800CW-NHS-ester and tilmanocept, enabled us to control the number of fluorescent molecules attached to each tilmanocept, which was quantified by H1 nuclear magnetic resonance spectroscopy. Quantum yields and molar absorptivities were measured for unconjugated IRDye 800CW and IRDye 800CW-tilmanocept (800CW-tilmanocept) preparations at 0.7, 1.5, 2.3, 2.9, and 3.8 dyes per tilmanocept. Specific fluorescence brightness was calculated by multiplication of the quantum yield by the molar absorptivity and the number of dyes per tilmanocept. It predicted that the preparation with 2.3 dyes per tilmanocept would exhibit the brightest signal, which was confirmed by fluorescence intensity measurements using three optical imaging systems. When radiolabeled with Ga68 and injected into the footpads of mice, the probe identified SLNs by both fluorescence and positron emission tomography (PET) while maintaining high percent extraction by the SLN. These studies demonstrated the feasibility of 800CW-tilmanocept for multimodal SLN mapping via fluorescence and PET–computed tomography imaging. PMID:23958947

Blue photoluminescent carbon nanodots from limeade.

PubMed

Suvarnaphaet, Phitsini; Tiwary, Chandra Sekhar; Wetcharungsri, Jutaphet; Porntheeraphat, Supanit; Hoonsawat, Rassmidara; Ajayan, Pulickel Madhavapanicker; Tang, I-Ming; Asanithi, Piyapong

2016-12-01

Carbon-based photoluminescent nanodot has currently been one of the promising materials for various applications. The remaining challenges are the carbon sources and the simple synthetic processes that enhance the quantum yield, photostability and biocompatibility of the nanodots. In this work, the synthesis of blue photoluminescent carbon nanodots from limeade via a single-step hydrothermal carbonization process is presented. Lime carbon nanodot (L-CnD), whose the quantum yield exceeding 50% for the 490nm emission in gram-scale amounts, has the structure of graphene core functionalized with the oxygen functional groups. The micron-sized flake of the as-prepared L-CnD powder exhibits multicolor emission depending on an excitation wavelength. The L-CnDs are demonstrated for rapidly ferric-ion (Fe(3+)) detection in water compared to Fe(2+), Cu(2+), Co(2+), Zn(2+), Mn(2+) and Ni(2+) ions. The photoluminescence quenching of L-CnD solution under UV light is used to distinguish the Fe(3+) ions from others by naked eyes as low concentration as 100μM. Additionally, L-CnDs provide exceptional photostability and biocompatibility for imaging yeast cell morphology. Changes in morphology of living yeast cells, i.e. cell shape variation, and budding, can be observed in a minute-period until more than an hour without the photoluminescent intensity loss. Copyright © 2016 Elsevier B.V. All rights reserved.

A near-infrared fluorescent probe based on BODIPY derivative with high quantum yield for selective detection of exogenous and endogenous cysteine in biological samples.

PubMed

Li, Song-Jiao; Fu, Ya-Jun; Li, Chun-Yan; Li, Yong-Fei; Yi, Lan-Hua; Ou-Yang, Juan

2017-11-22

Cysteine (Cys) is involved in cellular growth and Cys deficiency is related with many diseases. So far, a number of fluorescent probes have been constructed for the detection of Cys successfully. However, the probes are difficult to discriminate Cys from Hcy and the emission wavelength of the probes is in ultraviolet or visible range. Herein, a NIR fluorescent probe named NIR-BODIPY-Ac is synthesized and used to detect Cys. The emission wavelength of the probe is at 708 nm that belongs to near-infrared (NIR) region by attaching indolium to BODIPY core, which is suitable for bioimaging in vivo. Moreover, the probe exhibits high fluorescence quantum yield (Φ = 0.51) after the addition of Cys and high sensitivity toward Cys with 81-fold fluorescence enhancement. The linear range of the probe for Cys covers from 0.2 to 30 μM with a detection limit of 0.05 μM. Furthermore, the probe shows high selectivity towards Cys owing to the fact that there is more fast reaction rate between the probe and Cys than that of Hcy. In particular, the NIR fluorescent probe is applied for the detection of exogenous and endogenous Cys in biological samples such as cell, tissue and mouse with satisfactory results. Copyright © 2017 Elsevier B.V. All rights reserved.

Impact of D2O/H2O Solvent Exchange on the Emission of HgTe and CdTe Quantum Dots: Polaron and Energy Transfer Effects.

PubMed

Wen, Qiannan; Kershaw, Stephen V; Kalytchuk, Sergii; Zhovtiuk, Olga; Reckmeier, Claas; Vasilevskiy, Mikhail I; Rogach, Andrey L

2016-04-26

We have studied light emission kinetics and analyzed carrier recombination channels in HgTe quantum dots that were initially grown in H2O. When the solvent is replaced by D2O, the nonradiative recombination rate changes highlight the role of the vibrational degrees of freedom in the medium surrounding the dots, including both solvent and ligands. The contributing energy loss mechanisms have been evaluated by developing quantitative models for the nonradiative recombination via (i) polaron states formed by strong coupling of ligand vibration modes to a surface trap state (nonresonant channel) and (ii) resonant energy transfer to vibration modes in the solvent. We conclude that channel (i) is more important than (ii) for HgTe dots in either solution. When some of these modes are removed from the relevant spectral range by the H2O to D2O replacement, the polaron effect becomes weaker and the nonradiative lifetime increases. Comparisons with CdTe quantum dots (QDs) served as a reference where the resonant energy loss (ii) a priori was not a factor, also confirmed by our experiments. The solvent exchange (H2O to D2O), however, is found to slightly increase the overall quantum yield of CdTe samples, probably by increasing the fraction of bright dots in the ensemble. The fundamental study reported here can serve as the foundation for the design and optimization principles of narrow bandgap quantum dots aimed at applications in long wavelength colloidal materials for infrared light emitting diodes and photodetectors.

Adapting BODIPYs to singlet oxygen production on silica nanoparticles.

PubMed

Epelde-Elezcano, Nerea; Prieto-Montero, Ruth; Martínez-Martínez, Virginia; Ortiz, María J; Prieto-Castañeda, Alejandro; Peña-Cabrera, Eduardo; Belmonte-Vázquez, José L; López-Arbeloa, Iñigo; Brown, Ross; Lacombe, Sylvie

2017-05-31

A modified Stöber method is used to synthesize spherical core-shell silica nanoparticles (NPs) with an external surface functionalized by amino groups and with an average size around 50 nm. Fluorescent dyes and photosensitizers of singlet oxygen were fixed, either separately or conjointly, respectively in the core or in the shell. Rhodamines were encapsulated in the core with relatively high fluorescence quantum yields (Φ fl ≥ 0.3), allowing fluorescence tracking of the particles. Various photosensitizers of singlet oxygen (PS) were covalenty coupled to the shell, allowing singlet oxygen production. The stability of NP suspensions strongly deteriorated upon grafting the PS, affecting their apparent singlet oxygen quantum yields. Agglomeration of NPs depends both on the type and on the amount of grafted photosensitizer. New, lab-made, halogenated 4,4-difluoro-4-bora-3a,4a-diaza-s-indacenes (BODIPY) grafted to the NPs achieved higher singlet oxygen quantum yields (Φ Δ ∼ 0.35-0.40) than Rose Bengal (RB) grafted NPs (Φ Δ ∼ 0.10-0.27). Finally, we combined both fluorescence and PS functions in the same NP, namely a rhodamine in the silica core and a BODIPY or RB grafted in the shell, achieving the performance Φ fl ∼ 0.10-0.20, Φ Δ ∼ 0.16-0.25 with a single excitation wavelength. Thus, proper choice of the dyes, of their concentrations inside and on the NPs and the grafting method enables fine-tuning of singlet oxygen production and fluorescence emission.

Super-Poissonian statistics of photon emission from single CdSe-CdS core-shell nanocrystals coupled to metal nanostructures.

PubMed

Park, Young-Shin; Ghosh, Yagnaseni; Chen, Yongfen; Piryatinski, Andrei; Xu, Ping; Mack, Nathan H; Wang, Hsing-Lin; Klimov, Victor I; Hollingsworth, Jennifer A; Htoon, Han

2013-03-15

We demonstrate that photon antibunching observed for individual nanocrystal quantum dots (NQDs) can be transformed into photon bunching characterized by super-Poissonian statistics when they are coupled to metal nanostructures (MNs). This observation indicates that, while the quantum yield of a biexciton (Q(2X)) is lower than that of a single exciton (Q(1X)) in freestanding NQDs, Q(2X) becomes greater than Q(1X) in NQDs coupled to MNs. This unique phenomenon is attributed to metal-induced quenching with a rate that scales more slowly with exciton multiplicity than the radiative decay rate and dominates over other nonradiative decay channels for both single excitons and biexcitons.

Field-emission from quantum-dot-in-perovskite solids

PubMed Central

García de Arquer, F. Pelayo; Gong, Xiwen; Sabatini, Randy P.; Liu, Min; Kim, Gi-Hwan; Sutherland, Brandon R.; Voznyy, Oleksandr; Xu, Jixian; Pang, Yuangjie; Hoogland, Sjoerd; Sinton, David; Sargent, Edward

2017-01-01

Quantum dot and well architectures are attractive for infrared optoelectronics, and have led to the realization of compelling light sensors. However, they require well-defined passivated interfaces and rapid charge transport, and this has restricted their efficient implementation to costly vacuum-epitaxially grown semiconductors. Here we report solution-processed, sensitive infrared field-emission photodetectors. Using quantum-dots-in-perovskite, we demonstrate the extraction of photocarriers via field emission, followed by the recirculation of photogenerated carriers. We use in operando ultrafast transient spectroscopy to sense bias-dependent photoemission and recapture in field-emission devices. The resultant photodiodes exploit the superior electronic transport properties of organometal halide perovskites, the quantum-size-tuned absorption of the colloidal quantum dots and their matched interface. These field-emission quantum-dot-in-perovskite photodiodes extend the perovskite response into the short-wavelength infrared and achieve measured specific detectivities that exceed 1012 Jones. The results pave the way towards novel functional photonic devices with applications in photovoltaics and light emission. PMID:28337981

Fluorescence spectroscopy and confocal microscopy of the mycotoxin citrinin in condensed phase and hydrogel films.

PubMed

Lauer, Milena H; Gehlen, Marcelo H; de Jesus, Karen; Berlinck, Roberto G S

2014-05-01

The emission spectra, quantum yields and fluorescence lifetimes of citrinin in organic solvents and hydrogel films have been determined. Citrinin shows complex fluorescence decays due to the presence of two tautomers in solution and interconversion from excited-state double proton transfer (ESDPT) process. The fluorescence decay times associated with the two tautomers have values near 1 and 5 ns depending on the medium. In hydrogel films of agarose and alginate, fluorescence imaging showed that citrinin is not homogeneously dispersed and highly emissive micrometer spots may be formed. Fluorescence spectrum and decay analysis are used to recognize the presence of citrinin in hydrogel films using confocal fluorescence microscopy and spectroscopy.

One-dimensional carrier confinement in “Giant” CdS/CdSe excitonic nanoshells

DOE PAGES

Razgoniaeva, Natalia; Moroz, Pavel; Yang, Mingrui; ...

2017-05-23

Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifestedmore » in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.« less

Highly crystalline carbon dots from fresh tomato: UV emission and quantum confinement.

PubMed

Liu, Weijian; Li, Chun; Sun, Xiaobo; Pan, Wei; Yu, Guifeng; Wang, Jinping

2017-12-01

In this article, fresh tomatoes are explored as a low-cost source to prepare high-performance carbon dots by using microwave-assisted pyrolysis. Given that amino groups might act as nucleophiles for cleaving covalent bridging ester or ether in the crosslinked macromolecules in the biomass bulk, ethylenediamine (EDA) and urea with amino groups were applied as nucleophiles to modulate the chemical composites of the carbon nanoparticles in order to tune their fluorescence emission and enhance their quantum yields. Very interestingly, the carbon dots synthesized in the presence of urea had a highly crystalline nature, a low-degree amorphous surface and were smaller than 5 nm. Moreover, the doped N contributed to the formation of a cyclic form of core that resulted in a strong electron-withdrawing ability within the conjugated C plane. Therefore, this type of carbon dot exhibited marked quantum confinement, with the maximum fluorescence peak located in the UV region. Carbon nanoparticles greater than 20 nm in size, prepared using pristine fresh tomato and in the presence of EDA, emitted surface state controlled fluorescence. Additionally, carbon nanoparticles synthesized using fresh tomato pulp in the presence of EDA and urea were explored for bioimaging of plant pathogenic fungi and the detection of vanillin.

Probing Bioluminescence Resonance Energy Transfer in Quantum Rod-Luciferase Nanoconjugates.

PubMed

Alam, Rabeka; Karam, Liliana M; Doane, Tennyson L; Coopersmith, Kaitlin; Fontaine, Danielle M; Branchini, Bruce R; Maye, Mathew M

2016-02-23

We describe the necessary design criteria to create highly efficient energy transfer conjugates containing luciferase enzymes derived from Photinus pyralis (Ppy) and semiconductor quantum rods (QRs) with rod-in-rod (r/r) microstructure. By fine-tuning the synthetic conditions, CdSe/CdS r/r-QRs were prepared with two different emission colors and three different aspect ratios (l/w) each. These were hybridized with blue, green, and red emitting Ppy, leading to a number of new BRET nanoconjugates. Measurements of the emission BRET ratio (BR) indicate that the resulting energy transfer is highly dependent on QR energy accepting properties, which include absorption, quantum yield, and optical anisotropy, as well as its morphological and topological properties, such as aspect ratio and defect concentration. The highest BR was found using r/r-QRs with lower l/w that were conjugated with red Ppy, which may be activating one of the anisotropic CdSe core energy levels. The role QR surface defects play on Ppy binding, and energy transfer was studied by growth of gold nanoparticles at the defects, which indicated that each QR set has different sites. The Ppy binding at those sites is suggested by the observed BRET red-shift as a function of Ppy-to-QR loading (L), where the lowest L results in highest efficiency and furthest shift.

Highly crystalline carbon dots from fresh tomato: UV emission and quantum confinement

NASA Astrophysics Data System (ADS)

Liu, Weijian; Li, Chun; Sun, Xiaobo; Pan, Wei; Yu, Guifeng; Wang, Jinping

2017-12-01

In this article, fresh tomatoes are explored as a low-cost source to prepare high-performance carbon dots by using microwave-assisted pyrolysis. Given that amino groups might act as nucleophiles for cleaving covalent bridging ester or ether in the crosslinked macromolecules in the biomass bulk, ethylenediamine (EDA) and urea with amino groups were applied as nucleophiles to modulate the chemical composites of the carbon nanoparticles in order to tune their fluorescence emission and enhance their quantum yields. Very interestingly, the carbon dots synthesized in the presence of urea had a highly crystalline nature, a low-degree amorphous surface and were smaller than 5 nm. Moreover, the doped N contributed to the formation of a cyclic form of core that resulted in a strong electron-withdrawing ability within the conjugated C plane. Therefore, this type of carbon dot exhibited marked quantum confinement, with the maximum fluorescence peak located in the UV region. Carbon nanoparticles greater than 20 nm in size, prepared using pristine fresh tomato and in the presence of EDA, emitted surface state controlled fluorescence. Additionally, carbon nanoparticles synthesized using fresh tomato pulp in the presence of EDA and urea were explored for bioimaging of plant pathogenic fungi and the detection of vanillin.

Quantification and imaging of HER2 protein using nanocrystals conjugated with single-domain antibodies

NASA Astrophysics Data System (ADS)

Glukhov, S.; Berestovoy, M.; Chames, P.; Baty, D.; Nabiev, I.; Sukhanova, A.

2017-01-01

This study dealt with quantification and imaging of human epidermal growth factor receptor 2 (HER2), an important prognostic marker for cancer diagnosis and treatment, using specific quantum-dot-based conjugates. Fluorescent inorganic nanocrystals or quantum dots (QDs) are extremely highly resistant to photobleaching and have a high emission quantum yield and a continuous range of emission spectra, from the ultraviolet to the infrared regions. Ultrasmall nanoprobes consisting of highly affine anti-HER2 single-domain antibodies (sdAbs or "nanobodies") conjugated with QDs in a strictly oriented manner have been designed. QDs with a fluorescence peak maxima at wavelengths of 562 nm, 569 nm, 570 nm or in the near-infrared region were used. Here, we present our results of ISA quantification of HER2 protein, in situ imaging of HER2 protein on the surface of HER2-positive SK-BR-3 cells in immunohistochemical experiments, and counting of stained with anti-HER2 conjugates HER2-positive SK-BR-3 cells in their mixture with unstained cells of the same culture in flow cytometry experiments. The data demonstrate that the anti-HER2 QD-sdAb conjugates obtained are highly specific and sensitive and could be used in numerous applications for advanced integrated diagnosis.

Formation mechanism and optimization of highly luminescent N-doped graphene quantum dots

PubMed Central

Qu, Dan; Zheng, Min; Zhang, Ligong; Zhao, Haifeng; Xie, Zhigang; Jing, Xiabin; Haddad, Raid E.; Fan, Hongyou; Sun, Zaicheng

2014-01-01

Photoluminescent graphene quantum dots (GQDs) have received enormous attention because of their unique chemical, electronic and optical properties. Here a series of GQDs were synthesized under hydrothermal processes in order to investigate the formation process and optical properties of N-doped GQDs. Citric acid (CA) was used as a carbon precursor and self-assembled into sheet structure in a basic condition and formed N-free GQD graphite framework through intermolecular dehydrolysis reaction. N-doped GQDs were prepared using a series of N-containing bases such as urea. Detailed structural and property studies demonstrated the formation mechanism of N-doped GQDs for tunable optical emissions. Hydrothermal conditions promote formation of amide between –NH2 and –COOH with the presence of amine in the reaction. The intramoleculur dehydrolysis between neighbour amide and COOH groups led to formation of pyrrolic N in the graphene framework. Further, the pyrrolic N transformed to graphite N under hydrothermal conditions. N-doping results in a great improvement of PL quantum yield (QY) of GQDs. By optimized reaction conditions, the highest PL QY (94%) of N-doped GQDs was obtained using CA as a carbon source and ethylene diamine as a N source. The obtained N-doped GQDs exhibit an excitation-independent blue emission with single exponential lifetime decay. PMID:24938871

One-dimensional carrier confinement in “Giant” CdS/CdSe excitonic nanoshells

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

Razgoniaeva, Natalia; Moroz, Pavel; Yang, Mingrui

Here, the emerging generation of quantum dot optoelectronic devices offers an appealing prospect of a size-tunable band gap. The confinement-enabled control over electronic properties, however, requires nanoparticles to be sufficiently small, which leads to a large area of interparticle boundaries in a film. Such interfaces lead to a high density of surface traps which ultimately increase the electrical resistance of a solid. To address this issue, we have developed an inverse energy-gradient core/shell architecture supporting the quantum confinement in nanoparticles larger than the exciton Bohr radius. The assembly of such nanostructures exhibits a relatively low surface-to-volume ratio, which was manifestedmore » in this work through the enhanced conductance of solution-processed films. The reported core/shell geometry was realized by growing a narrow gap semiconductor layer (CdSe) on the surface of a wide-gap core material (CdS) promoting the localization of excitons in the shell domain, as was confirmed by ultrafast transient absorption and emission lifetime measurements. The band gap emission of fabricated nanoshells, ranging from 15 to 30 nm in diameter, has revealed a characteristic size-dependent behavior tunable via the shell thickness with associated quantum yields in the 4.4–16.0% range.« less

Specific interactions of alcohols and non-alcohols with a biologically active boronic acid derivative: a spectroscopic study.

PubMed

Geethanjali, H S; Melavanki, R M; Nagaraja, D; Patil, N R; Thipperudrappa, J; Kusanur, R A

2016-08-01

The photophysical properties of 4-fluoro-2-methoxyphenyl boronic acid (4FMPBA) are characterized using absorption and fluorescence techniques in series of non-alcohols and alcohols. The results are analyzed using different solvent polarity functions and Kamlet and Catalan's multiple regression approaches. The excited state dipole moment and change in dipole moment are calculated using both the solvatochromic shift method and Reichardt's microscopic solvent polarity parameter ETN. The ground state dipole moment is evaluated using quantum chemical calculations. It is found that general solute-solvent and hydrogen bond interactions are operative in this system. A red shift of ~ 9 nm in the emission spectra is observed with an increase in the solvent polarity, which depicts π→π(*) transitions, as well as the possibility of an intramolecular charge transfer (ICT) character in the emitting singlet state of 4FMPBA. The relative quantum yield, radiative and non-radiative decay constants are calculated in alkanes and alcohols using the single point method. It is found that the quantum yield of the molecule varies from 16.81% to 50.79% with the change in solvent polarity, indicating the dependence of fluorescence on the solvent environment. Copyright © 2015 John Wiley & Sons, Ltd. Copyright © 2015 John Wiley & Sons, Ltd.

Changes in luminescence emission induced by proton irradiation: InGaAs/GaAs quantum wells and quantum dots

NASA Technical Reports Server (NTRS)

Leon, R.; Swift, G. M.; Magness, B.; Taylor, W. A.; Tang, Y. S.; Wang, K. L.; Dowd, P.; Zhang, Y. H.

2000-01-01

The photoluminescence emission from InGaAs/GaAs quantum-well and quantum-dot (QD) structures are compared after controlled irradiation with 1.5 MeV proton fluxes. Results presented here show a significant enhancement in radiation tolerance with three-dimensional quantum confinement.

Detection of CdSe quantum dot photoluminescence for security label on paper

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

Isnaeni,, E-mail: isnaeni@lipi.go.id; Sugiarto, Iyon Titok; Bilqis, Ratu

CdSe quantum dot has great potential in various applications especially for emitting devices. One example potential application of CdSe quantum dot is security label for anti-counterfeiting. In this work, we present a practical approach of security label on paper using one and two colors of colloidal CdSe quantum dot, which is used as stamping ink on various types of paper. Under ambient condition, quantum dot is almost invisible. The quantum dot security label can be revealed by detecting emission of quantum dot using photoluminescence and cnc machine. The recorded quantum dot emission intensity is then analyzed using home-made program tomore » reveal quantum dot pattern stamp having the word ’RAHASIA’. We found that security label using quantum dot works well on several types of paper. The quantum dot patterns can survive several days and further treatment is required to protect the quantum dot. Oxidation of quantum dot that occurred during this experiment reduced the emission intensity of quantum dot patterns.« less

Synthesis and Characterization of Mercaptoacetic Acid Capped Cadmium Sulphide Quantum Dots.

PubMed

Wageh, S; Maize, Mai; Donia, A M; Al-Ghamdi, Ahmed A; Umar, Ahmad

2015-12-01

This paper reports the facile synthesis and detailed characterization of mercaptoacetic acid capped cadmium sulphide (CdS) quantum dots using various cadmium precursors. The mercaptoacetic acid capped CdS quantum dots were prepared by facile and simple wet chemical method and characterized by several techniques such as energy dispersive spectroscopy (EDS), X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, UV-vis. spectroscopy, photoluminescence spectroscopy, high-resolution transmission microscopy (HRTEM) and thremogravimetric analysis. The EDS studies revealed that the prepared quantum dots possess higher atomic percentage of sulfur compared to cadmium due to the coordination of thiolate to the quantum dots surfaces. The X-ray and absorption analyses exhibited that the size of quantum dots prepared by cadmium acetate is larger than the quantum dots prepared by cadmium chloride and cadmium nitrate. The increase in size can be attributed to the low stability constant of cadmium acetate in comparison with cadmium chloride and cadmium nitrate. The FTIR and thermogravimetric analysis showed that the nature of capping molecule on the surface of quantum dots are different depending on the cadmium precursors which affect the emission from CdS quantum dots. Photoemission spectroscopy revealed that the emission of quantum dots prepared by cadmium acetate has high intensity band edge emission along with low intensity trapping state emission. However the CdS quantum dots prepared by cadmium chloride and cadmium nitrate produced only trapping state emissions.

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.

White light emitting diode based on InGaN chip with core/shell quantum dots

NASA Astrophysics Data System (ADS)

Shen, Changyu; Hong, Yan; Ma, Jiandong; Ming, Jiangzhou

2009-08-01

Quantum dots have many applications in optoelectronic device such as LEDs for its many superior properties resulting from the three-dimensional confinement effect of its carrier. In this paper, single chip white light-emitting diodes (WLEDs) were fabricated by combining blue InGaN chip with luminescent colloidal quantum dots (QDs). Two kinds of QDs of core/shell CdSe /ZnS and core/shell/shell CdSe /ZnS /CdS nanocrystals were synthesized by thermal deposition using cadmium oxide and selenium as precursors in a hot lauric acid and hexadecylamine trioctylphosphine oxide hybrid. This two kinds of QDs exhibited high photoluminescence efficiency with a quantum yield more than 41%, and size-tunable emission wavelengths from 500 to 620 nm. The QDs LED mainly consists of flip luminescent InGaN chip, glass ceramic protective coating, glisten cup, QDs using as the photoluminescence material, pyroceram, gold line, electric layer, dielectric layer, silicon gel and bottom layer for welding. The WLEDs had the CIE coordinates of (0.319, 0.32). The InGaN chip white-light-emitting diodes with quantum dots as the emitting layer are potentially useful in illumination and display applications.

Synthesis and optical properties of metal (M) atom-doped polycarbosilane (PCS) with extended conjugation (M = Al, Dy, Er and Eu)

NASA Astrophysics Data System (ADS)

Yao, Rongqian; Zhao, Haoran; Feng, Zude; Chen, Lifu; Zhang, Ying

2013-10-01

Optical properties of metal atom-doped polycarbosilane (PCS) which originated from σ-conjugation effect were studied. Al, Dy, Er and Eu were introduced into PCS by one-pot method to yield polyaluminocarbosilane (PACS), polydysprosiumcarbosilane (PDCS), polyerbiumcarbosilane (PErCS) and polyeuropiumcarbosilane (PECS), respectively. Effects of oxidation curing and ultraviolet (UV) radiation on the photoluminescence (PL) properties of the samples were investigated. PL spectra show strong blue light-emissions and the intensity of PCS is enhanced by adding metal atoms. PACS with extended σ-conjugation exhibits an obvious PL red-shift, high intensity, high quantum yield and excellent oxidation resistance as compared with those of others. As treated under UV lamp for 3 h in air, PACS retains good UV resistance performance, owing to the AlOx (x = 4, 5, or 6) groups which effectively extend the σ-conjugation. The obtained results are expected to have important applications in active sources for electroluminescence (EL) devices, especially suitable for blue emission.

Impurity-assisted terahertz photoluminescence in quantum wells under conditions of interband stimulated emission

NASA Astrophysics Data System (ADS)

Makhov, I. S.; Panevin, V. Yu; Firsov, D. A.; Vorobjev, L. E.; Sofronov, A. N.; Vinnichenko, M. Ya; Maleev, N. A.; Vasil'ev, A. P.

2018-03-01

Terahertz and near-infrared photoluminescence under conditions of interband stimulated emission are studied in n-GaAs/AlGaAs quantum well laser structure. The observed terahertz emission is related to the optical transitions of nonequilibrium electrons from the first electron subband and excited donor states to donor ground states in quantum wells. The opportunity to increase the intensity of impurity-assisted terahertz emission due to interband stimulated emission with the participation of impurity centres is demonstrated.

Fluorescence Imaging Assisted Photodynamic Therapy Using Photosensitizer-Linked Gold Quantum Clusters.

PubMed

Nair, Lakshmi V; Nazeer, Shaiju S; Jayasree, Ramapurath S; Ajayaghosh, Ayyappanpillai

2015-06-23

Fluorescence imaging assisted photodynamic therapy (PDT) is a viable two-in-one clinical tool for cancer treatment and follow-up. While the surface plasmon effect of gold nanorods and nanoparticles has been effective for cancer therapy, their emission properties when compared to gold nanoclusters are weak for fluorescence imaging guided PDT. In order to address the above issues, we have synthesized a near-infrared-emitting gold quantum cluster capped with lipoic acid (L-AuC with (Au)18(L)14) based nanoplatform with excellent tumor reduction property by incorporating a tumor-targeting agent (folic acid) and a photosensitizer (protoporphyrin IX), for selective PDT. The synthesized quantum cluster based photosensitizer PFL-AuC showed 80% triplet quantum yield when compared to that of the photosensitizer alone (63%). PFL-AuC having 60 μg (0.136 mM) of protoporphyrin IX was sufficient to kill 50% of the tumor cell population. Effective destruction of tumor cells was evident from the histopathology and fluorescence imaging, which confirm the in vivo PDT efficacy of PFL-AuC.

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

Marseglia, L.; Saha, K.; Ajoy, A.

The practical implementation of quantum technologies such as quantum commu- nication and quantum cryptography relies on the development of indistinguishable, robust, and bright single photon sources that works at room temperature. The silicon- vacancy (SiV -) center in diamond has emerged as a possible candidate for a single photon source with all these characteristics. Unfortunately, due to the high refraction index mismatch between diamond and air, color centers in diamond show low photon out-coupling. This drawback can be overcome by fabrication of photonic structures that improve the in-coupling of excitation laser to the diamond defect as well as the out-couplingmore » emission from the color centers. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion effciency to single SiV -, targeted to fabricated nanowires. The co-localization of single SiV - defects with the nanostructures yields a ten times higher light coupling effciency as compared to single SiV - in the bulk. This result, with its intrinsic scalability, enables a new class of devices for integrated photonics and quantum information processing.« less

GaAs/GaP quantum dots: Ensemble of direct and indirect heterostructures with room temperature optical emission

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

Dadgostar, S.; Mogilatenko, A.; Masselink, W. T.

2016-03-07

We describe the optical emission and the carrier dynamics of an ensemble of self-assembled GaAs quantum dots embedded in GaP(001). The QD formation is driven by the 3.6% lattice mismatch between GaAs and GaP in the Stranski-Krastanow mode after deposition of more than 1.2 monolayers of GaAs. The quantum dots have an areal density between 6 and 7.6 × 10{sup 10} per cm{sup −2} and multimodal size distribution. The luminescence spectra show two peaks in the range of 1.7 and 2.1 eV. The samples with larger quantum dots have red emission and show less thermal quenching compared with the samples with smaller QDs.more » The large QDs luminescence up to room temperature. We attribute the high energy emission to indirect carrier recombination in the thin quantum wells or small strained quantum dots, whereas the low energy red emission is due to the direct electron-hole recombination in the relaxed quantum dots.« less

Activation energy of light induced isomerization of resveratrol.

PubMed

Figueiras, Teresa Sofia; Neves-Petersen, Maria Teresa; Petersen, Steffen B

2011-09-01

Isomerization of trans-stilbenes is known to be induced by light. The two isomers have distinct absorption, fluorescence excitation and emission spectra. Resveratrol, 3,4',5-trihydroxystilbene, is a member of the stilbene family. The interest of the scientific community in resveratrol has increased over the last years due to its biomedical properties. Whereas there is a growing confidence that trans-resveratrol is non-toxic, very little is known about the pharmacology of cis-resveratrol. Of this very reason there is considerable interest in knowing the energetics of the trans-cis conversion. Cis-resveratrol is characterized by a large fluorescence quantum yield when compared to trans-resveratrol. In the present paper we report a detailed analysis of the spectral changes induced in trans-resveratrol upon 260 nm excitation for different time periods. Spectral changes have been monitored with UV-visible absorption and steady-state fluorescence spectroscopy at pH 4 at 20, 25, 30, 35, 40, 45 and 50 °C. Continuous 260 nm excitation induces a blue shift in the absorption and fluorescence excitation spectra of resveratrol and a 14 nm blue shift in its fluorescence emission. The photoisomerization yield is reported as a function of 260 nm excitation time. 330 min continuous excitation led to ~60% isomerization yield. The kinetics of trans-cis isomerization has been monitored following the increase in fluorescence quantum yield upon continuous 260 nm excitation of trans-resveratrol. The study was carried out at the above mentioned temperatures in order to obtain the Arrhenius activation energy of photoisomerization. Activation energy and pre-exponential factor were 3.7 ± 0.3 kcal.mol(-1) and 10.6 ± 1.6 s(-1), respectively. The activation energy is comparable with previously reported values for the photoisomerization of other stilbenes.

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.

Postsynthesis Phase Transformation for CsPbBr3/Rb4PbBr6 Core/shell Nanocrystals with Exceptional Photostability.

PubMed

Wang, Bo; Zhang, Congyang; Huang, Shouqiang; Li, Zhichun; Kong, Long; Jin, Ling; Wang, Junhui; Wu, Kaifeng; Li, Liang

2018-06-15

Lead halide perovskite nanocrystals (NCs) as promising optoelectronic materials are intensively researched. However, the instability is one of the biggest challenges needed to overcome before fulfill their practical applications. To improve their stability, we present a postsynthetic controlled phase transformation of CsPbBr3 toward CsPbBr3/Rb4PbBr6 core/shell structure triggered by rubidium oleate treatment. The resulted core/shell NCs show exceptional photostability both in solution and on-chip. The solution of CsPbBr3/Rb4PbBr6 NCs can remain over 90% of the initial emission photoluminescence quantum yields (PLQY) after 42 h of intense light-emitting diodes illumination (450 nm, 175 mW/cm2), which is even better than the conventional CdSe/CdS quantum dots whose emission drop to 50% after 18 h under the same condition. We believe that the exceptional photostability should be resulted from the protection of the robust Rb4PbBr6 shell on CsPbBr3 NCs.

PTFE-based microreactor system for the continuous synthesis of full-visible-spectrum emitting cesium lead halide perovskite nanocrystals.

PubMed

Zhang, Chengxi; Luan, Weiling; Yin, Yuhang; Yang, Fuqian

2017-01-01

Colloidal perovskite nanocrystals comprised of all inorganic cesium lead halide (CsPbX 3 , X = Cl, Br, I or a mixture thereof) have potential as optical gain materials due to their high luminescence efficiency. In this work, cesium lead halide nanocrystals are continuously synthesized via a microreactor system consisting of poly(tetrafluoroethylene) (PTFE) capillaries. The synthesized nanocrystals possess excellent optical properties, including a full width at half maximum of 19-35 nm, high fluorescence quantum yield of 47.8-90.55%, and photoluminescence emission in the range of 450-700 nm. For the same precursor concentrations, the photoluminescence emission peak generally increases with increasing reaction temperature, revealing a controllable temperature effect on the photoluminescence characteristics of the synthesized nanocrystals. For quantum dots synthesized with a Br/I ratio of 1:3, a slight blue shift was observed for reaction temperatures greater than 100 °C. This PTFE-based microreactor system provides the unique capability of continuously synthesizing high-quality perovskite nanocrystals that emit over the full visible spectrum with applications ranging from displays and optoelectronic devices.

PTFE-based microreactor system for the continuous synthesis of full-visible-spectrum emitting cesium lead halide perovskite nanocrystals

PubMed Central

Zhang, Chengxi; Yin, Yuhang

2017-01-01

Colloidal perovskite nanocrystals comprised of all inorganic cesium lead halide (CsPbX3, X = Cl, Br, I or a mixture thereof) have potential as optical gain materials due to their high luminescence efficiency. In this work, cesium lead halide nanocrystals are continuously synthesized via a microreactor system consisting of poly(tetrafluoroethylene) (PTFE) capillaries. The synthesized nanocrystals possess excellent optical properties, including a full width at half maximum of 19–35 nm, high fluorescence quantum yield of 47.8–90.55%, and photoluminescence emission in the range of 450–700 nm. For the same precursor concentrations, the photoluminescence emission peak generally increases with increasing reaction temperature, revealing a controllable temperature effect on the photoluminescence characteristics of the synthesized nanocrystals. For quantum dots synthesized with a Br/I ratio of 1:3, a slight blue shift was observed for reaction temperatures greater than 100 °C. This PTFE-based microreactor system provides the unique capability of continuously synthesizing high-quality perovskite nanocrystals that emit over the full visible spectrum with applications ranging from displays and optoelectronic devices. PMID:29259867

Highly pure yellow light emission of perovskite CsPb(BrxI1-x)3 quantum dots and their application for yellow light-emitting diodes

NASA Astrophysics Data System (ADS)

He, Yuandan; Gong, Jinhui; Zhu, Yiyuan; Feng, Xingcan; Peng, Hong; Wang, Wei; He, Haiyang; Liu, Hu; Wang, Li

2018-06-01

High-quality all-inorganic perovskite CsPb(BrxI1-x)3 quantum dots (QDs) with quantum yield of 50% were systematically studied as yellow light convertor for light emitting diodes (LEDs). A novel heat insulation structure was designed for the QD-converted yellow LEDs. In this structure, a silicone layer was set on top of the GaN LED chip to prevent directly heating of the QDs by the LED chip. Then the CsPb(BrxI1-x)3 QDs were filled in the bowl-shaped silicone layer after ultrasonic dispersion treatment. Finally, an Al2O3 passivation layer was grown on the QDs layer by Atomic Layer Disposition at 40 °C. When x = 0.55, highly pure yellow LEDs with an emission peak at ∼570 nm and a full width at half maximum of 25 nm were achieved. The chromaticity coordinates of the QD-converted yellow LEDs (0.4920 ± 0.0017, 0.4988 ± 0.0053) showed almost no variation under driving current from 5 mA to 150 mA. During an operation period of 60 min, the emission wavelength of the yellow LEDs showed no distinct shift. Moreover, the luminous efficiency of the QD-converted yellow LEDs achieved 13.51 l m/W at 6 mA. These results demonstrated that CsPb(BrxI1-x)3 QDs and the heat insulation structure are promising candidate for high purity yellow LEDs.

Synthesis and characterization of (3-Aminopropyl)trimethoxy-silane (APTMS) functionalized Gd2O3:Eu(3+) red phosphor with enhanced quantum yield.

PubMed

Jain, Akhil; Hirata, G A; Farías, M H; Castillón, F F

2016-02-12

We report the surface modification of nanocrystalline Gd2O3:Eu(3+) phosphor by (3-Aminopropyl)trimethoxysilane (APTMS). The nanoparticles were first coated with silica using the Stöber process, and then annealed at 650 °C for 2 h. Afterwards, APTMS was functionalized onto the silica layer to obtain Gd2O3:Eu(3+) nanoparticles bearing amine groups on the surface. The effect of silica coating, and the subsequent annealing process on the crystallization of the nanophosphor were analyzed by x-ray diffraction (XRD). High-resolution transmission electron microscopy (HR-TEM) confirmed the presence of a silica layer of ∼45 nm thickness. X-ray photoelectron (XPS) and Fourier transform infrared (FTIR) spectroscopy confirmed the presence of silica and the amine groups. Photoluminescence (PL) analysis demonstrated an increased emission after functionalization of nanoparticles. Absolute quantum yield (QY) measurements revealed an 18% enhancement in QY in functionalized nanoparticles compared with unmodified nanoparticles, which is of great importance for their biomedical applications.

Synthesis and characterization of (3-Aminopropyl)trimethoxy-silane (APTMS) functionalized Gd2O3:Eu3+ red phosphor with enhanced quantum yield

NASA Astrophysics Data System (ADS)

Jain, Akhil; Hirata, G. A.; Farías, M. H.; Castillón, F. F.

2016-02-01

We report the surface modification of nanocrystalline Gd2O3:Eu3+ phosphor by (3-Aminopropyl)trimethoxysilane (APTMS). The nanoparticles were first coated with silica using the Stöber process, and then annealed at 650 °C for 2 h. Afterwards, APTMS was functionalized onto the silica layer to obtain Gd2O3:Eu3+ nanoparticles bearing amine groups on the surface. The effect of silica coating, and the subsequent annealing process on the crystallization of the nanophosphor were analyzed by x-ray diffraction (XRD). High-resolution transmission electron microscopy (HR-TEM) confirmed the presence of a silica layer of ∼45 nm thickness. X-ray photoelectron (XPS) and Fourier transform infrared (FTIR) spectroscopy confirmed the presence of silica and the amine groups. Photoluminescence (PL) analysis demonstrated an increased emission after functionalization of nanoparticles. Absolute quantum yield (QY) measurements revealed an 18% enhancement in QY in functionalized nanoparticles compared with unmodified nanoparticles, which is of great importance for their biomedical applications.

End Functionalized Nonionic Water-Dispersible Conjugated Polymers.

PubMed

Zhan, Ruoyu; Liu, Bin

2017-09-01

2,7-Dibromofluorene monomers carrying two or four oligo(ethylene glycol) (OEG) side chains are synthesized. Heck coupling between the monomers and 1,4-divinylbenzene followed by end capping with [4-(4-bromophenoxy)butyl]carbamic acid tert-butyl ester leads to two nonionic water-dispersible poly(fluorene-alt-1,4-divinylenephenylene)s end-functionalized with amine groups after hydrolysis. In water, the polymer with a lower OEG density (P1) has poor water dispersibility with a quantum yield of 0.24, while the polymer with a higher OEG density (P2) possesses excellent water-dispersibility with a high quantum yield of 0.45. Both polymers show fluorescence enhancement and blue-shifted absorption and emission maxima in the presence of surfactant sodium dodecyl sulfate and dodecyltrimethylammonium bromide. The polymers are also resistant to ionic strength with minimal nonspecific interactions to bovine serum albumin. When biotin is incorporated into the end of the polymer backbones through N-hydroxysuccinimide/amine coupling reaction, the biotinylated polymers interact specifically with streptavidin on solid surface. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Radiometric calibration of optical microscopy and microspectroscopy apparata over a broad spectral range using a special thin-film luminescence standard

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

Valenta, J., E-mail: jan.valenta@mff.cuni.cz; Greben, M.

2015-04-15

Application capabilities of optical microscopes and microspectroscopes can be considerably enhanced by a proper calibration of their spectral sensitivity. We propose and demonstrate a method of relative and absolute calibration of a microspectroscope over an extraordinary broad spectral range covered by two (parallel) detection branches in visible and near-infrared spectral regions. The key point of the absolute calibration of a relative spectral sensitivity is application of the standard sample formed by a thin layer of Si nanocrystals with stable and efficient photoluminescence. The spectral PL quantum yield and the PL spatial distribution of the standard sample must be characterized bymore » separate experiments. The absolutely calibrated microspectroscope enables to characterize spectral photon emittance of a studied object or even its luminescence quantum yield (QY) if additional knowledge about spatial distribution of emission and about excitance is available. Capabilities of the calibrated microspectroscope are demonstrated by measuring external QY of electroluminescence from a standard poly-Si solar-cell and of photoluminescence of Er-doped Si nanocrystals.« less

Systematic investigations on fused π-system compounds of seven benzene rings prepared by photocyclization of diphenanthrylethenes.

PubMed

Fujino, Shota; Yamaji, Minoru; Okamoto, Hideki; Mutai, Toshiki; Yoshikawa, Isao; Houjou, Hirohiko; Tani, Fumito

2017-06-14

We studied the photoproducts of 1-(n-phenanthryl)-2-(m-phenanthryl)ethenes (nEm; n, m = 1, 3 and 9) for understanding photocyclization patterns based on NMR spectroscopy. The crystal structures of the photoproducts were analyzed by X-ray crystallography, and the photophysical features of the photocyclized molecules were investigated based on emission and transient absorption measurements. Phenanthrene derivatives substituted at the 1- and 3-positions were prepared for synthesizing nEm by photocyclization of stilbene derivatives. We obtained four types of primary photoproducts (n@m) from the corresponding nEm. Two of them were found to have racemic molecular structures in the single crystal determined by X-ray crystallography. Besides the primary photoproducts, two types of secondary photoproducts (n@mPP) were isolated. Fluorescence quantum yields and lifetimes of the obtained photoproducts were determined in solution whereas the definite fluorescence quantum yields were obtained in the powder. Observation of the triplet-triplet absorption spectra in solution by laser photolysis techniques showed that intersystem crossing to the triplet state competes with the fluorescence process.

Strain-compensated (Ga,In)N/(Al,Ga)N/GaN multiple quantum wells for improved yellow/amber light emission

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

Lekhal, K.; Damilano, B., E-mail: bd@crhea.cnrs.fr; De Mierry, P.

2015-04-06

Yellow/amber (570–600 nm) emitting In{sub x}Ga{sub 1−x}N/Al{sub y}Ga{sub 1−y}N/GaN multiple quantum wells (QWs) have been grown by metal organic chemical vapor deposition on GaN-on- sapphire templates. When the (Al,Ga)N thickness of the barrier increases, the room temperature photoluminescence is red-shifted while its yield increases. This is attributed to an increase of the QW internal electric field and an improvement of the material quality due to the compensation of the compressive strain of the In{sub x}Ga{sub 1−x}N QWs by the Al{sub y}Ga{sub 1−y}N layers, respectively.

Highly luminescent colloidal nanoplates of perovskite cesium lead halide and their oriented assemblies

DOE PAGES

Bekenstein, Yehonadav; Koscher, Brent A.; Eaton, Samuel W.; ...

2015-12-15

Anisotropic colloidal quasi-two-dimensional nanoplates (NPLs) hold great promise as functional materials due to their combination of low dimensional optoelectronic properties and versatility through colloidal synthesis. Recently, lead-halide perovskites have emerged as important optoelectronic materials with excellent efficiencies in photovoltaic and light-emitting applications. Here we report the synthesis of quantum confined all inorganic cesium lead halide nanoplates in the perovskite crystal structure that are also highly luminescent (PLQY 84%). The controllable self-assembly of nanoplates either into stacked columnar phases or crystallographic-oriented thin-sheet structures is demonstrated. Furthermore, the broad accessible emission range, high native quantum yields, and ease of self-assembly make perovskitemore » NPLs an ideal platform for fundamental optoelectronic studies and the investigation of future devices.« less

Stimulated emission in quantum well laser diodes

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

Blood, P.

1989-07-03

We observe that stimulated emission from inhomogeneously pumped quantum well laser diodes is shifted down in energy compared with the subband transition energy. Measured spontaneous emission spectra show that this stimulated emission is due to band-to-band transitions shifted by renormalization at high injected carrier densities, and we suggest that this same mechanism explains reported observations of stimulated emission from inhomogeneously photopumped structures which previously have been interpreted as evidence for longitudinal optic (LO) phonon participation. We show that LO phonon participation cannot account for the photon energy of stimulated emission from conventional homogeneously pumped quantum well laser diodes.

Bright Single InAsP Quantum Dots at Telecom Wavelengths in Position-Controlled InP Nanowires: The Role of the Photonic Waveguide.

PubMed

Haffouz, Sofiane; Zeuner, Katharina D; Dalacu, Dan; Poole, Philip J; Lapointe, Jean; Poitras, Daniel; Mnaymneh, Khaled; Wu, Xiaohua; Couillard, Martin; Korkusinski, Marek; Schöll, Eva; Jöns, Klaus D; Zwiller, Valery; Williams, Robin L

2018-05-09

We report on the site-selected growth of bright single InAsP quantum dots embedded within InP photonic nanowire waveguides emitting at telecom wavelengths. We demonstrate a dramatic dependence of the emission rate on both the emission wavelength and the nanowire diameter. With an appropriately designed waveguide, tailored to the emission wavelength of the dot, an increase in the count rate by nearly 2 orders of magnitude (0.4 to 35 kcps) is obtained for quantum dots emitting in the telecom O-band, showing high single-photon purity with multiphoton emission probabilities down to 2%. Using emission-wavelength-optimized waveguides, we demonstrate bright, narrow-line-width emission from single InAsP quantum dots with an unprecedented tuning range of 880 to 1550 nm. These results pave the way toward efficient single-photon sources at telecom wavelengths using deterministically grown InAsP/InP nanowire quantum dots.

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.

Bright Single InAsP Quantum Dots at Telecom Wavelengths in Position-Controlled InP Nanowires: The Role of the Photonic Waveguide

NASA Astrophysics Data System (ADS)

Haffouz, Sofiane; Zeuner, Katharina D.; Dalacu, Dan; Poole, Philip J.; Lapointe, Jean; Poitras, Daniel; Mnaymneh, Khaled; Wu, Xiaohua; Couillard, Martin; Korkusinski, Marek; Schöll, Eva; Jöns, Klaus D.; Zwiller, Valery; Williams, Robin L.

2018-05-01

We report on the site-selected growth of bright single InAsP quantum dots embedded within InP photonic nanowire waveguides emitting at telecom wavelengths. We demonstrate a dramatic dependence of the emission rate on both the emission wavelength and the nanowire diameter. With an appropriately designed waveguide, tailored to the emission wavelength of the dot, an increase in count rate by nearly two orders of magnitude (0.4kcps to 35kcps) is obtained for quantum dots emitting in the telecom O-band. Using emission-wavelength-optimised waveguides, we demonstrate bright, narrow linewidth emission from single InAsP quantum dots with an unprecedented tuning range from 880nm to 1550nm. These results pave the way towards efficient single photon sources at telecom wavelengths using deterministically grown InAsP/InP nanowire quantum dots.

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.

Rational Design of Emissive NIR-Absorbing Chromophores: Rh(III) Porphyrin-Aza-BODIPY Conjugates with Orthogonal Metal-Carbon Bonds.

PubMed

Zhou, Jinfeng; Gai, Lizhi; Zhou, Zhikuan; Yang, Wu; Mack, John; Xu, Kejing; Zhao, Jianzhang; Zhao, Yue; Qiu, Hailin; Chan, Kin Shing; Shen, Zhen

2016-09-05

The facile synthesis of Group 9 Rh(III) porphyrin-aza-BODIPY conjugates that are linked through an orthogonal Rh-C(aryl) bond is reported. The conjugates combine the advantages of the near-IR (NIR) absorption and intense fluorescence of aza-BODIPY dyes with the long-lived triplet states of transition metal rhodium porphyrins. Only one emission peak centered at about 720 nm is observed, irrespective of the excitation wavelength, demonstrating that the conjugates act as unique molecules rather than as dyads. The generation of a locally excited (LE) state with intramolecular charge-transfer (ICT) character has been demonstrated by solvatochromic effects in the photophysical properties, singlet oxygen quantum yields in polar solvents, and by the results of density functional theory (DFT) calculations. In nonpolar solvents, the Rh(III) conjugates exhibit strong aza-BODIPY-centered fluorescence at around 720 nm (ΦF =17-34 %), and negligible singlet oxygen generation. In polar solvents, enhancements of the singlet-oxygen quantum yield (ΦΔ =19-27 %, λex =690 nm) have been observed. Nanosecond pulsed time-resolved absorption spectroscopy confirms that relatively long-lived triplet excited states are formed. The synthetic methodology outlined herein provides a useful strategy for the assembly of functional materials that are highly desirable for a wide range of applications in material science and biomedical fields. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The coordination- and photochemistry of copper(i) complexes: variation of N^N ligands from imidazole to tetrazole.

PubMed

Bergmann, Larissa; Braun, Carolin; Nieger, Martin; Bräse, Stefan

2018-01-02

The prediction of coordination modes is of high importance when structure-property relationships are discussed. Herein, the coordination chemistry of copper(i) with pyridine-amines with a varying number of coordinating N-atoms, namely pyridine-benzimidazole, -triazole and -tetrazole, or their deprotonated analogues, and different phosphines was systematically studied and the photoluminescence properties of all synthesized complexes examined and related to DFT data. Each complex was characterized by single-crystal X-ray analysis and elemental analysis, and a set of prediction rules derived for the coordination chemistry of copper(i) with these ligands. A mononuclear cationic coordination motif was found for PPh 3 or DPEPhos with all N^N ligands, which exhibits blue to green luminescence of MLCT character d(Cu) → π*(pyridine-amine ligand) with quantum yields up to 46%. With the deprotonated N^N ligands, mononuclear neutral complexes were only expected with DPEPhos. The emission's nature of this complex type is strongly dependent on the electronic effects of the N^N ligand and was characterized as (ML + IL)CT transition. In contrast to the high quantum yields up to 78% for the tetrazolate complexes (as reported before), the triazolate and imidazolate based complexes show much lower emission efficiencies below 10%. Besides the mononuclear copper(i) complexes, cluster-type complexes were obtained, which show moderate luminescence in the blue to green region of the visible spectrum (469-505 nm).

Metal Photocathodes for Free Electron Laser Applications

NASA Astrophysics Data System (ADS)

Greaves, Corin Michael Ricardo

Synchrotron x-ray radiation sources have revolutionized many areas of science from elucidating the atomic structure of proteins to understanding the electronic structure of complex materials such as the cuprate superconductors. In a Free Electron Laser (FEL), the main difference to the synchrotron radiation mechanism is that the light field acts on the electron beam, over a long distance in an undulator, and causes electron bunching at the optical wavelength. Electrons in different parts of the electron bunch are therefore correlated, and so emit coherently, with a brightness that scales as the square of the number of electrons. In order to lase, the electron beam in a FEL must have a transverse geometric emittance less than the wavelength of the light to be produced. For the generation of x-ray wavelengths, this is one of the most difficult challenges in the design and construction of a FEL. The geometric emittance can be "compressed" by acceleration to very high energy, but with the penalty of very large physical size and very large cost. The motivation for this work was provided by the desire to investigate the fundamental origin of the emittance of an electron beam as it is born at a photocathode. If this initial, or "thermal" emittance can be reduced, the energy, scale and cost of accelerators potentially would be reduced. As the LCLS used copper as its photocathode, this material was the one studied in this work. Copper was used in the LCLS as it represented a "robust" material that could stand the very high accelerating gradients used in the photoinjector of the FEL. Metals are also prompt photoemitters, and so can be used to produce very short electron bunches. This can be a useful property for creation of extremely short FEL pulses, and also for creation of beams that are allowed to expand under space charge forces, but in a way that results in linear fields, allowing subsequent recompression. An ideal photocathode for FEL photoinjector should have high quantum efficiency (QE), small emittance, fast temporal response, long lifetime, and minimal complexity. High QE of cathodes require less power for driving laser and also reduce the risk of damaging the cathode materials. Small emittance reduce the scale of the accelerator, therefore, the cost. Metal photocathodes such as copper exhibit long lifetime and fast response, but have quite low quantum efficiency ( < 10-4). The aim in this work was to understand the quantum yield of the metal, and the transverse momentum spectrum, as the product of the latter and the cathode beam spot size gives the transverse emittance. Initial x-ray diffraction work provided evidence that the LCLS photocathode consisted of large low index single crystal grains, and so work focused on the study of single crystals that could be produced with atomically ordered surfaces, rather than a polycrystalline material. Present theories of quantum yield and transverse emittance assume the basic premise that the metal is entirely disordered, and work here shows that this is fundamentally incorrect, and that the order of the surface plays a critical role in determining the characteristics of emission. In order to investigate these surfaces, I constructed a laser-based ultra-low energy angle resolved photoemission system, capable of measuring the momentum spectrum of the emission and wavelength and angle dependent electron yield. This system has been commissioned, and data taken on low index surfaces of copper. Results from this work on single crystal copper demonstrates that emitted electrons from the band structure of a material can exhibit small emittance and high quantum efficiency. We show that the emission from the Cu(111) surface state is highly correlated between angle of incidence and excitation energy. This manifests itself in the form of a truncated emission cone, rather than the isotropic emission predicted from the normal model. This clearly then reduces the emittance from the normal values. It also results in extremely strong polarization dependence, with p-s asymmetry of up to 16 at low photon energy. It also directly suggests ways through changing materials, or by material design to significantly reduce emittance, at the same time increasing electron yield. These results show the benefits that could be gained from electronic engineering of cathodes and should have direct impact in the design of future FEL photoinjectors. (Abstract shortened by UMI.)

Photophysical and Photochemical Properties of Some Fluorescent Derivatives of Vitamin B1

NASA Astrophysics Data System (ADS)

Marciniak, B.

1987-05-01

Absorption and emission spectra, depopulation kinetics of the lowest excited singlet and triplet states and acid-base equilibria of two fluorescent vitamin B, derivatives, the products I and II of the reaction of N-methylated vitamine B, with cytidine and adenosine, respectively, were investigated. Analysis of the lifetime and quantum yield data indicate that at 77 K emissions are the main processes of deactivation of the S1 and T1 states for the free ion and protonated forms. The pKa values indicate a much higher acidity in the excited singlet and triplet states than in the ground state. I and II undergo very slow photochemical reactions in solution in the presence of oxygen (Φ ~ 10-4).

Photonics of a conjugated organometallic Pt-Ir polymer and its model compounds exhibiting hybrid CT excited states.

PubMed

Soliman, Ahmed M; Fortin, Daniel; Zysman-Colman, Eli; Harvey, Pierre D

2012-04-13

Trans- dichlorobis(tri-n-butylphosphine)platinum(II) reacts with bis(2- phenylpyridinato)-(5,5'-diethynyl-2,2'-bipyridine)iridium(III) hexafluorophosphate to form the luminescent conjugated polymer poly[trans-[(5,5'-ethynyl-2,2'-bipyridine)bis(2- phenylpyridinato)-iridium(III)]bis(tri-n-butylphosphine)platinum(II)] hexafluorophosphate ([Pt]-[Ir])n. Gel permeation chromatography indicates a degree of polymerization of 9 inferring the presence of an oligomer. Comparison of the absorption and emission band positions and their temperature dependence, emission quantum yields, and lifetimes with those for models containing only the [Pt] or the [Ir] units indicates hybrid excited states including features from both chromophores. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Preparation of carbon quantum dots from cigarette filters and its application for fluorescence detection of Sudan I.

PubMed

Anmei, Su; Qingmei, Zhong; Yuye, Chen; Yilin, Wang

2018-09-06

Carbon quantum dots (CQDs) with quantum yield of 14% were successfully synthesized via a simple, low-cost, and green hydrothermal treatment using cigarette filters as carbon source for the first time. The obtained CQDs showed a strong emission at the wavelength of 465 nm, with an optimum excitation of 365 nm.Sudan I with maximum absorption wavelength at 477 nm could selectively quench the fluorescence of CQDs. Based on this principle, a fluorescence probe was developed for Sudan I determination. Furthermore, the quenching mechanism of the CQDs was elucidated. A linear relationship was found in the range of 2.40-104.0 μmol/L Sudan I with the detection limit (3σ/k) of 0.95 μmol/L. Satisfactory results were achieved when the method was submitted to the determination of Sudan I in food samples. Copyright © 2018 Elsevier B.V. All rights reserved.

Lead selenide quantum dot polymer nanocomposites

NASA Astrophysics Data System (ADS)

Waldron, Dennis L.; Preske, Amanda; Zawodny, Joseph M.; Krauss, Todd D.; Gupta, Mool C.

2015-02-01

Optical absorption and fluorescence properties of PbSe quantum dots (QDs) in an Angstrom Bond AB9093 epoxy polymer matrix to form a nanocomposite were investigated. To the authors’ knowledge, this is the first reported use of AB9093 as a QD matrix material and it was shown to out-perform the more common poly(methyl methacrylate) matrix in terms of preserving the optical properties of the QD, resulting in the first reported quantum yield (QY) for PbSe QDs in a polymer matrix, 26%. The 1-s first excitonic absorption peak of the QDs in a polymer matrix red shifted 65 nm in wavelength compared to QDs in a hexane solution, while the emission peak in the polymer matrix red shifted by 38 nm. The fluorescence QY dropped from 55% in hexane to 26% in the polymer matrix. A time resolved fluorescence study of the QDs showed single exponential lifetimes of 2.34 and 1.34 μs in toluene solution and the polymer matrix respectively.

Highly luminescent core-shell InP/ZnX (X = S, Se) quantum dots prepared via a phosphine synthetic route.

PubMed

Mordvinova, Natalia; Vinokurov, Alexander; Kuznetsova, Tatiana; Lebedev, Oleg I; Dorofeev, Sergey

2017-01-24

Here we report a simple method for the creation of highly luminescent core-shell InP/ZnX (X = S, Se) quantum dots (QDs) on the basis of a phosphine synthetic route. In this method a Zn precursor was added to the reaction mixture at the beginning of the synthesis to form an In(Zn)P alloy structure, which promoted the formation of a ZnX shell. Core-shell InP/ZnX QDs exhibit highly intensive emission with a quantum yield over 50%. The proposed method is primarily important for practical applications. Advantages of this method compared to the widely used SILAR technique are discussed. We further demonstrate that the SILAR approach consisting of consequent addition of Zn and chalcogen precursors to pre-prepared non-doped InP colloidal nanoparticles is not quite suitable for shell growth without the addition of special activator agents or the use of very reactive precursors.

Experimental evidence of quantum radiation reaction in aligned crystals.

PubMed

Wistisen, Tobias N; Di Piazza, Antonino; Knudsen, Helge V; Uggerhøj, Ulrik I

2018-02-23

Quantum radiation reaction is the influence of multiple photon emissions from a charged particle on the particle's dynamics, characterized by a significant energy-momentum loss per emission. Here we report experimental radiation emission spectra from ultrarelativistic positrons in silicon in a regime where quantum radiation reaction effects dominate the positron's dynamics. Our analysis shows that while the widely used quantum approach is overall the best model, it does not completely describe all the data in this regime. Thus, these experimental findings may prompt seeking more generally valid methods to describe quantum radiation reaction. This experiment is a fundamental test of quantum electrodynamics in a regime where the dynamics of charged particles is strongly influenced not only by the external electromagnetic fields but also by the radiation field generated by the charges themselves and where each photon emission may significantly reduce the energy of the charge.

A theoretical investigation of the influence of gold nanosphere size on the decay and energy transfer rates and efficiencies of quantum emitters.

PubMed

Marocico, Cristian A; Zhang, Xia; Bradley, A Louise

2016-01-14

We present in this contribution a comprehensive investigation of the effect of the size of gold nanospheres on the decay and energy transfer rates of quantum systems placed close to these nanospheres. These phenomena have been investigated before, theoretically and experimentally, but no comprehensive study of the influence of the nanoparticle size on important dependences of the decay and energy transfer rates, such as the dependence on the donor-acceptor spectral overlap and the relative positions of the donor, acceptor, and nanoparticle, exists. As such, different accounts of the energy transfer mechanism have been presented in the literature. We perform an investigation of the energy transfer mechanisms between emitters and gold nanospheres and between donor-acceptor pairs in the presence of the gold nanospheres using a Green's tensor formalism, experimentally verified in our lab. We find that the energy transfer rate to small nanospheres is greatly enhanced, leading to a strong quenching of the emission of the emitter. When the nanosphere size is increased, it acts as an antenna, increasing the emission of the emitter. We also investigate the emission wavelength and intrinsic quantum yield dependence of the energy transfer to the nanosphere. As evidenced from the literature, the energy transfer process between the quantum system and the nanosphere can have a complicated distance dependence, with a r(-6) regime, characteristic of the Förster energy transfer mechanism, but also exhibiting other distance dependences. In the case of a donor-acceptor pair of quantum systems in the presence of a gold nanosphere, when the donor couples strongly to the nanosphere, acting as an enhanced dipole; the donor-acceptor energy transfer rate then follows a Förster trend, with an increased Förster radius. The coupling of the acceptor to the nanosphere has a different distance dependence. The angular dependence of the energy transfer efficiency between donor and acceptor exhibits a strong focusing effect and the same enhanced donor-dipole character in different angular arrangements. The spectral overlap of the donor emission and acceptor absorption spectra shows that the energy transfer follows the near-field scattering efficiency, with a red-shift from the localized surface plasmon peak for small sphere sizes.

Deep-UV emission at 219 nm from ultrathin MBE GaN/AlN quantum heterostructures

NASA Astrophysics Data System (ADS)

Islam, S. M.; Protasenko, Vladimir; Lee, Kevin; Rouvimov, Sergei; Verma, Jai; Xing, Huili Grace; Jena, Debdeep

2017-08-01

Deep ultraviolet (UV) optical emission below 250 nm (˜5 eV) in semiconductors is traditionally obtained from high aluminum containing AlGaN alloy quantum wells. It is shown here that high-quality epitaxial ultrathin binary GaN quantum disks embedded in an AlN matrix can produce efficient optical emission in the 219-235 nm (˜5.7-5.3 eV) spectral range, far above the bulk bandgap (3.4 eV) of GaN. The quantum confinement energy in these heterostructures is larger than the bandgaps of traditional semiconductors, made possible by the large band offsets. These molecular beam epitaxy-grown extreme quantum-confinement GaN/AlN heterostructures exhibit an internal quantum efficiency of 40% at wavelengths as short as 219 nm. These observations together with the ability to engineer the interband optical matrix elements to control the direction of photon emission in such binary quantum disk active regions offer unique advantages over alloy AlGaN quantum well counterparts for the realization of deep-UV light-emitting diodes and lasers.

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

Calva-Tellez, E.

The angular distributions of the process e/sup +/e/sup -/ yields e/sup +/e/sup / measured by the Bologna-CERN-Frascati group at the electron-positron colliding-beam facility Adonc are analyzed in terms of standard quantum 3/ including soft-and hard-photon emission. An analytical expression is given for the cross section of the process e/sup +/e/sup -/ yields e/sup +/e gamma for hard photons. Detailed numerical r esults for that specific experimental setup are obtained by a Monte Carlo progrm. It is found that this bremsstrahlung process is responsible for the noncollinear and noncoplanar events observed at Frasscati. Therefore, these data, together with the present calculation,more » provide a test of QED for this particular physical situation involving high energies and large momentum transfers. (auth)« less

The low-energy, charge-transfer excited states of 4-amino-4-prime-nitrodiphenyl sulfide

NASA Technical Reports Server (NTRS)

O'Connor, Donald B.; Scott, Gary W.; Tran, Kim; Coulter, Daniel R.; Miskowski, Vincent M.; Stiegman, Albert E.; Wnek, Gary E.

1992-01-01

Absorption and emission spectra of 4-amino-4-prime-nitrodiphenyl sulfide in polar and nonpolar solvents were used to characterize and assign the low-energy excited states of the molecule. Fluorescence-excitation anisotropy spectra and fluorescence quantum yields were also used to characterize the photophysics of these states. The lowest-energy fluorescent singlet state was determined to be an intramolecular charge transfer (ICT) state involving transfer of a full electron charge from the amino to the nitro group yielding a dipole moment of about 50 D. A low-energy, intense absorption band is assigned as a transition to a different ICT state involving a partial electron charge transfer from sulfur to the nitro group.

Strongly Cavity-Enhanced Spontaneous Emission from Silicon-Vacancy Centers in Diamond

DOE PAGES

Zhang, Jingyuan Linda; Sun, Shuo; Burek, Michael J.; ...

2018-01-29

Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into themore » cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. Here, we also demonstrate the largest coupling strength ( g/2π = 4.9 ± 0.3 GHz) and cooperativity ( C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.« less

Strongly Cavity-Enhanced Spontaneous Emission from Silicon-Vacancy Centers in Diamond

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

Zhang, Jingyuan Linda; Sun, Shuo; Burek, Michael J.

Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into themore » cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. Here, we also demonstrate the largest coupling strength ( g/2π = 4.9 ± 0.3 GHz) and cooperativity ( C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.« less

Single colloidal quantum dots as sources of single photons for quantum cryptography

NASA Astrophysics Data System (ADS)

Pisanello, Ferruccio; Qualtieri, Antonio; Leménager, Godefroy; Martiradonna, Luigi; Stomeo, Tiziana; Cingolani, Roberto; Bramati, Alberto; De Vittorio, Massimo

2011-02-01

Colloidal nanocrystals, i.e. quantum dots synthesized trough wet-chemistry approaches, are promising nanoparticles for photonic applications and, remarkably, their quantum nature makes them very promising for single photon emission at room temperature. In this work we describe two approaches to engineer the emission properties of these nanoemitters in terms of radiative lifetime and photon polarization, drawing a viable strategy for their exploitation as room-temperature single photon sources for quantum information and quantum telecommunications.

Room temperature synthesis of ultra-small, near-unity single-sized lead halide perovskite quantum dots with wide color emission tunability, high color purity and high brightness.

PubMed

Peng, Lucheng; Geng, Jing; Ai, Lisha; Zhang, Ying; Xie, Renguo; Yang, Wensheng

2016-08-19

Phosphor with extremely narrow emission line widths, high brightness, and wide color emission tunability in visible regions is required for display and lighting applications, yet none has been reported in the literature so far. In the present study, single-sized lead halide perovskite (APbX 3; A = CH3NH3 and Cs; X = Cl, Br, and I) nanocrystalline (NC) phosphors were achieved for the first time in a one-pot reaction at room temperature (25 °C). The size-dependent samples, which included four families of CsPbBr3 NCs and exhibited sharp excitonic absorption peaks and pure band gap emission, were directly obtained by simply varying the concentration of ligands. The continuity of the optical spectrum can be successively tuned over the entire UV-visible spectral region (360-610 nm) by preparing CsPbCl3, CsPbI3, and CsPb(Y/Br)3 (Y = Cl and I) NCs with the use of CsPbBr3 NCs as templates by anion exchange while maintaining the size of NCs and high quantum yields of up to 80%. Notably, an emission line width of 10-24 nm, which is completely consistent with that of their single particles, indicates the formation of single-sized NCs. The versatility of the synthetic strategy was validated by extending it to the synthesis of single-sized CH3NH3PbX 3 NCs by simply replacing the cesium precursor by the CH3NH3 X precursor.

2,5-difluorenyl-substituted siloles for the fabrication of high-performance yellow organic light-emitting diodes.

PubMed

Chen, Bin; Jiang, Yibin; Chen, Long; Nie, Han; He, Bairong; Lu, Ping; Sung, Herman H Y; Williams, Ian D; Kwok, Hoi Sing; Qin, Anjun; Zhao, Zujin; Tang, Ben Zhong

2014-02-10

2,3,4,5-Tetraarylsiloles are a class of important luminogenic materials with efficient solid-state emission and excellent electron-transport capacity. However, those exhibiting outstanding electroluminescence properties are still rare. In this work, bulky 9,9-dimethylfluorenyl, 9,9-diphenylfluorenyl, and 9,9'-spirobifluorenyl substituents were introduced into the 2,5-positions of silole rings. The resulting 2,5-difluorenyl-substituted siloles are thermally stable and have low-lying LUMO energy levels. Crystallographic analysis revealed that intramolecular π-π interactions are prone to form between 9,9'-spirobifluorene units and phenyl rings at the 3,4-positions of the silole ring. In the solution state, these new siloles show weak blue and green emission bands, arising from the fluorenyl groups and silole rings with a certain extension of π conjugation, respectively. With increasing substituent volume, intramolecular rotation is decreased, and thus the emissions of the present siloles gradually improved and they showed higher fluorescence quantum yields (Φ(F) =2.5-5.4%) than 2,3,4,5-tetraphenylsiloles. They are highly emissive in solid films, with dominant green to yellow emissions and good solid-state Φ(F) values (75-88%). Efficient organic light-emitting diodes were fabricated by adopting them as host emitters and gave high luminance, current efficiency, and power efficiency of up to 44,100 cd m(-2), 18.3 cd A(-1), and 15.7 lm W(-1), respectively. Notably, a maximum external quantum efficiency of 5.5% was achieved in an optimized device. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Marocico, Cristian A.; Zhang, Xia; Bradley, A. Louise, E-mail: bradlel@tcd.ie

We present in this contribution a comprehensive investigation of the effect of the size of gold nanospheres on the decay and energy transfer rates of quantum systems placed close to these nanospheres. These phenomena have been investigated before, theoretically and experimentally, but no comprehensive study of the influence of the nanoparticle size on important dependences of the decay and energy transfer rates, such as the dependence on the donor-acceptor spectral overlap and the relative positions of the donor, acceptor, and nanoparticle, exists. As such, different accounts of the energy transfer mechanism have been presented in the literature. We perform anmore » investigation of the energy transfer mechanisms between emitters and gold nanospheres and between donor-acceptor pairs in the presence of the gold nanospheres using a Green’s tensor formalism, experimentally verified in our lab. We find that the energy transfer rate to small nanospheres is greatly enhanced, leading to a strong quenching of the emission of the emitter. When the nanosphere size is increased, it acts as an antenna, increasing the emission of the emitter. We also investigate the emission wavelength and intrinsic quantum yield dependence of the energy transfer to the nanosphere. As evidenced from the literature, the energy transfer process between the quantum system and the nanosphere can have a complicated distance dependence, with a r{sup −6} regime, characteristic of the Förster energy transfer mechanism, but also exhibiting other distance dependences. In the case of a donor-acceptor pair of quantum systems in the presence of a gold nanosphere, when the donor couples strongly to the nanosphere, acting as an enhanced dipole; the donor-acceptor energy transfer rate then follows a Förster trend, with an increased Förster radius. The coupling of the acceptor to the nanosphere has a different distance dependence. The angular dependence of the energy transfer efficiency between donor and acceptor exhibits a strong focusing effect and the same enhanced donor-dipole character in different angular arrangements. The spectral overlap of the donor emission and acceptor absorption spectra shows that the energy transfer follows the near-field scattering efficiency, with a red-shift from the localized surface plasmon peak for small sphere sizes.« less

Emissive sensors and devices incorporating these sensors

DOEpatents

Swager, Timothy M; Zhang, Shi-Wei

2013-02-05

The present invention generally relates to luminescent and/or optically absorbing compositions and/or precursors to those compositions, including solid films incorporating these compositions/precursors, exhibiting increased luminescent lifetimes, quantum yields, enhanced stabilities and/or amplified emissions. The present invention also relates to sensors and methods for sensing analytes through luminescent and/or optically absorbing properties of these compositions and/or precursors. Examples of analytes detectable by the invention include electrophiles, alkylating agents, thionyl halides, and phosphate ester groups including phosphoryl halides, cyanides and thioates such as those found in certain chemical warfare agents. The present invention additionally relates to devices and methods for amplifying emissions, such as those produced using the above-described compositions and/or precursors, by incorporating the composition and/or precursor within a polymer having an energy migration pathway. In some cases, the compositions and/or precursors thereof include a compound capable of undergoing a cyclization reaction.

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

Synthesis and Photoluminescent Properties of Arylethynyl substituted 9,10-Anthraquinones

NASA Technical Reports Server (NTRS)

Yang, Jin-Hua; Dass, Amala; Sotiriou-Leventis, Chariklia; Leventis, Nicholas

2003-01-01

A series of arylethynyl substituted anthraquinones were synthesized via Sonogashira coupling reactions of 2,7- dibromo-, 2,6-dibromo- and 2-bromoanthraquinone with para-substituted phenylacetylenes. While the redox properties of those compounds are almost insensitive to substitution, their absorption maxima are linearly related to the Hammett constants for electron donating and electron withdrawing groups separately. All compounds are photoluminescent both in solution (quantum yield of emission approximately 2%) and as solids. X-ray crystallographic characterization of 2,7-bisphenylethynyl anthraquinone indicates a monoclinic p2(l/n) space group and no indication for pi-overlap that would promote self-quenching. The emission maxima are red- shifted by both electron donating and electron withdrawing groups alike. The Stokes shifts of all compounds are significant and are correlated to the electronic properties of the substituents. The reduced forms of these compounds are also photoluminescent and the emission originates from the dihydroanthraquinone core.

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

NASA Astrophysics Data System (ADS)

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

2018-03-01

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

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

Ultralow-power near-infrared excited neodymium-doped nanoparticles for long-term in vivo bioimaging.

PubMed

Qin, Qing-Song; Zhang, Pei-Zhi; Sun, Ling-Dong; Shi, Shuo; Chen, Nai-Xiu; Dong, Hao; Zheng, Xiao-Yu; Li, Le-Min; Yan, Chun-Hua

2017-04-06

Lanthanide-doped luminescent nanoparticles with both emission and excitation in the near-infrared (NIR-to-NIR) region hold great promise for bioimaging. Herein, core@shell structured LiLuF 4 :Nd@LiLuF 4 (named as Nd@Lu) nanoparticles (NPs) with highly efficient NIR emission were developed for high-performance in vivo bioimaging. Strikingly, the absolute quantum yield of Nd@Lu NPs reached as high as 32%. After coating with polyethylene glycol (PEG), the water-dispersible Nd@Lu NPs showed good bio-compatibility and low toxicity. With efficient NIR emission, the Nd@Lu NPs were clearly detectable in tissues at depths of up to 20 mm. In addition, long-term in vivo biodistribution with a high signal-to-noise ratio of 25.1 was distinctly tracked upon an ultralow-power-density excitation (10 mW cm -2 ) of 732 nm for the first time.

A dual-colored bio-marker made of doped ZnO nanocrystals

NASA Astrophysics Data System (ADS)

Wu, Y. L.; Fu, S.; Tok, A. I. Y.; Zeng, X. T.; Lim, C. S.; Kwek, L. C.; Boey, F. C. Y.

2008-08-01

Bio-compatible ZnO nanocrystals doped with Co, Cu and Ni cations, surface capped with two types of aminosilanes and titania are synthesized by a soft chemical process. Due to the small particle size (2-5 nm), surface functional groups and the high photoluminescence emissions at the UV and blue-violet wavelength ranges, bio-imaging on human osteosarcoma (Mg-63) cells and histiocytic lymphoma U-937 monocyte cells showed blue emission at the nucleus and bright turquoise emission at the cytoplasm simultaneously. This is the first report on dual-color bio-images labeled by one semiconductor nanocrystal colloidal solution. Bright green emission was detected on mung bean seedlings labeled by all the synthesized ZnO nanocrystals. Cytotoxicity tests showed that the aminosilanes capped nanoparticles are non-toxic. Quantum yields of the nanocrystals varied from 79% to 95%. The results showed the potential of the pure ZnO and Co-doped ZnO nanocrystals for live imaging of both human cells and plant systems.

Cascaded emission of single photons from the biexciton in monolayered WSe2

PubMed Central

He, Yu-Ming; Iff, Oliver; Lundt, Nils; Baumann, Vasilij; Davanco, Marcelo; Srinivasan, Kartik; Höfling, Sven; Schneider, Christian

2016-01-01

Monolayers of transition metal dichalcogenide materials emerged as a new material class to study excitonic effects in solid state, as they benefit from enormous Coulomb correlations between electrons and holes. Especially in WSe2, sharp emission features have been observed at cryogenic temperatures, which act as single photon sources. Tight exciton localization has been assumed to induce an anharmonic excitation spectrum; however, the evidence of the hypothesis, namely the demonstration of a localized biexciton, is elusive. Here we unambiguously demonstrate the existence of a localized biexciton in a monolayer of WSe2, which triggers an emission cascade of single photons. The biexciton is identified by its time-resolved photoluminescence, superlinearity and distinct polarization in micro-photoluminescence experiments. We evidence the cascaded nature of the emission process in a cross-correlation experiment, which yields a strong bunching behaviour. Our work paves the way to a new generation of quantum optics experiments with two-dimensional semiconductors. PMID:27830703

Suppression of exciton dephasing in sidewall-functionalized carbon nanotubes embedded into metallo-dielectric antennas.

PubMed

Shayan, Kamran; He, Xiaowei; Luo, Yue; Rabut, Claire; Li, Xiangzhi; Hartmann, Nicolai F; Blackburn, Jeffrey L; Doorn, Stephen K; Htoon, Han; Strauf, Stefan

2018-06-26

Covalent functionalization of single-walled carbon nanotubes (SWCNTs) is a promising route to enhance the quantum yield of exciton emission and can lead to single-photon emission at room temperature. However, the spectral linewidth of the defect-related E11* emission remains rather broad. Here, we systematically investigate the low-temperature exciton emission of individual SWCNTs that have been dispersed with sodium-deoxycholate (DOC) and polyfluorene (PFO-BPy), are grown by laser vaporization (LV) or by CoMoCat techniques and are functionalized with oxygen as well as 3,5-dichlorobenzene groups. The E11 excitons in oxygen-functionalized SWCNTs remain rather broad with up to 10 meV linewidth while exciton emission from 3,5-dichlorobenzene functionalized SWCNTs is found to be about one order of magnitude narrower. In all cases, wrapping with PFO-BPy provides significantly better protection against pump induced dephasing compared to DOC. To further study the influence of exciton localization on pump-induced dephasing, we have embedded the functionalized SWCNTs into metallo-dielectric antenna cavities to maximize light collection. We show that 0D excitons attributed to the E11* emission of 3,5-dichlorobenzene quantum defects of LV-grown SWCNTs can display near resolution-limited linewidths down to 35 μeV. Interestingly, these 0D excitons give rise to a 3-fold suppressed pump-induced exciton dephasing compared to the E11 excitons in the same SWCNT. These findings provide a foundation to build a unified description of the emergence of novel optical behavior from the interplay of covalently introduced defects, dispersants, and exciton confinement in SWCNTs and might further lead to the realization of indistinguishable photons from carbon nanotubes.

Quantum Dot/Siloxane Composite Film Exceptionally Stable against Oxidation under Heat and Moisture.

PubMed

Kim, Hwea Yoon; Yoon, Da-Eun; Jang, Junho; Lee, Daewon; Choi, Gwang-Mun; Chang, Joon Ha; Lee, Jeong Yong; Lee, Doh C; Bae, Byeong-Soo

2016-12-21

We report on the fabrication of a siloxane-encapsulated quantum dot (QD) film (QD-silox film), which exhibits stable emission intensity for over 1 month even at elevated temperature and humidity. QD-silox films are solidified via free radical addition reaction between oligosiloxane resin and ligand molecules on QDs. We prepare the QD-oligosiloxane resin by sol-gel condensation reaction of silane precursors with QDs blended in the precursor solution, forgoing ligand-exchange of QDs. The resulting QD-oligosiloxane resin remains optically clear after 40 days of storage, in contrast to other QD-containing resins which turn turbid and ultimately form sediments. QDs also disperse uniformly in the QD-silox film, whose photoluminescence (PL) quantum yield (QY) remains nearly unaltered under harsh conditions; for example, 85 °C/5% relative humidity (RH), 85 °C/85% RH, strongly acidic, and strongly basic environments for 40 days. The QD-silox film appears to remain equally emissive even after being immersed into boiling water (100 °C). Interestingly, the PL QY of the QD-silox film noticeably increases when the film is exposed to a moist environment, which opens a new, facile avenue to curing dimmed QD-containing films. Given its excellent stability, we envision that the QD-silox film is best suited in display applications, particularly as a PL-type down-conversion layer.

MOVPE growth of (GaIn)As/Ga(AsSb)/(GaIn)As type-II heterostructures on GaAs substrate for near infrared laser applications

NASA Astrophysics Data System (ADS)

Fuchs, C.; Beyer, A.; Volz, K.; Stolz, W.

2017-04-01

The growth of high quality (GaIn)As/Ga(AsSb)/(GaIn)As "W"-quantum well heterostructures is discussed with respect to their application in 1300 nm laser devices. The structures are grown using metal organic vapor phase epitaxy and characterized using high-resolution X-ray diffraction, scanning transmission electron microscopy and photoluminescence measurements. The agreement between experimental high-resolution X-ray diffraction patterns and full dynamical simulations is verified for these structurally challenging heterostructures. Scanning transmission electron microscopy is used to demonstrate that the structure consists of well-defined quantum wells and forms the basis for future improvements of the optoelectronic quality of this materials system. By altering the group-V gas phase ratio, it is possible to cover a large spectral range between 1200 nm and 1470 nm using a growth temperature of 550 °C and a V/III ratio of 7.5. A comparison of a sample with a photoluminescence emission wavelength at 1360 nm with single quantum well material reference samples proves the type-II character of the emission. A further optimization of these structures for application in 1300 nm lasers by applying different V/III ratios yields a stable behavior of the photoluminescence intensity using a growth temperature of 550 °C.

Amine-derived synthetic approach to color-tunable InP/ZnS quantum dots with high fluorescent qualities

NASA Astrophysics Data System (ADS)

Song, Woo-Seuk; Lee, Hye-Seung; Lee, Ju Chul; Jang, Dong Seon; Choi, Yoonyoung; Choi, Moongoo; Yang, Heesun

2013-06-01

High-quality, Cd-free InP quantum dots (QDs) have been conventionally synthesized by exclusively selecting tris(trimethylsilyl)phosphine (P(TMS)3) as a phosphorus (P) precursor, which is problematic from the standpoint of green and economic chemistry. Thus, other synthetic chemistries adopting alternative P sources to P(TMS)3 have been introduced, however, they could not guarantee the production of satisfactorily fluorescence-efficient, color-pure InP QDs. In this study, the unprecedented controlled synthesis of a series of band-gap-tuned InP QDs is demonstrated through a hot-injection of a far safer and cheaper tris(dimethylamino)phosphine in the presence of a key coordinating solvent of oleylamine that enables successful QD nucleation/growth. Effects of the co-existence of Zn additive, the core growth temperature, and the amount of P source injected on the growth behaviors of InP QD are investigated. After ZnS overcoating by a successive injection of 1-dodecanethiol only, high-fluorescence-quality, green-to-red color emission-tunable core/shell QDs of InP/ZnS are obtained. The fluorescent characteristics of different color-emitting QDs desirably exhibit little fluctuations in quantum yield and emission bandwidth, specifically ranging 51-53 % and 60-64 nm, respectively. Lastly, the utility of the introduction of a secondary shelling process in rendering the QDs are more bright, photostable is also proved.

Capture and Emission of Charge Carriers by Quantum Well

NASA Astrophysics Data System (ADS)

Davydov, V. N.; Karankevich, O. A.

2018-06-01

The interaction of electrons from the conduction band of the barrier layer of a LED heterostructure with the quantum well size-quantization level described by the capture time and emission time of charge carriers is considered. Relaxation of an excess energy upon capture and emission of charge carriers occurs as a result of their collisions with phonons of the quantum well substance and the "barrier layer-quantum well" interface. Analytical expressions are obtained for the interaction times, taking into account the depth of the sizequantization level, involved in the interaction with electrons, and the width of the well. Numerical estimates show that in real conditions, the capture time is shorter than the emission time, and this difference increases with increasing depth of the level. At shallow depths, the capture and emission times are comparable.

A review on economic emission dispatch problems using quantum computational intelligence

NASA Astrophysics Data System (ADS)

Mahdi, Fahad Parvez; Vasant, Pandian; Kallimani, Vish; Abdullah-Al-Wadud, M.

2016-11-01

Economic emission dispatch (EED) problems are one of the most crucial problems in power systems. Growing energy demand, limitation of natural resources and global warming make this topic into the center of discussion and research. This paper reviews the use of Quantum Computational Intelligence (QCI) in solving Economic Emission Dispatch problems. QCI techniques like Quantum Genetic Algorithm (QGA) and Quantum Particle Swarm Optimization (QPSO) algorithm are discussed here. This paper will encourage the researcher to use more QCI based algorithm to get better optimal result for solving EED problems.

Photophysical dynamics of the efficient emission and photosensitization of [Ir(pqi)2(NN)]+ complexes.

PubMed

Zanoni, Kassio P S; Ito, Akitaka; Grüner, Malte; Murakami Iha, Neyde Y; de Camargo, Andrea S S

2018-01-23

The photophysical dynamics of three complexes in the highly-emissive [Ir(pqi) 2 (NN)] + series were investigated aiming at unique photophysical features and applications in light-emitting and singlet oxygen sensitizing research fields. Rational elucidation and Franck-Condon analyses of the observed emission spectra in nitrile solutions at 298 and 77 K reveal the true emissive nature of the lowest-lying triplet excited state (T 1 ), consisting of a hybrid 3 MLCT/LC Ir(pqi)→pqi state. Emissive deactivations from T 1 occur mainly by very intense, yellow-orange phosphorescence with high quantum yields and radiative rates. The emission nature experimentally verified is corroborated by theoretical calculations (TD-DFT), with T 1 arising from a mixing of several transitions induced by the spin-orbit coupling, majorly ascribed to 3 MLCT/LC Ir(pqi)→pqi and increasing contributions of 3 MLCT/LLCT Ir(pqi)→NN . The microsecond-lived emission of T 1 is rapidly quenched by molecular oxygen, with an efficient generation of singlet oxygen. Our findings show that the photophysics of [Ir(pqi) 2 (NN)][PF 6 ] complexes is suitable for many applications, from the active layer of electroluminescent devices to photosensitizers for photodynamic therapy and theranostics.

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…

Photoluminescence imaging of solitary dopant sites in covalently doped single-wall carbon nanotubes

DOE PAGES

Hartmann, Nicolai F.; Yalcin, Sibel Ebru; Adamska, Lyudmyla; ...

2015-11-11

Covalent dopants in semiconducting single wall carbon nanotubes (SWCNTs) are becoming important as routes for introducing new photoluminescent emitting states with potential for enhanced quantum yields, new functionality, and as species capable of near-IR room-temperature single photon emission. The origin and behavior of the dopant-induced emission is thus important to understand as a key requirement for successful room-T photonics and optoelectronics applications. Here, we use direct correlated two-color photoluminescence imaging to probe how the interplay between the SWCNT bright E 11 exciton and solitary dopant sites yields the dopant-induced emission for three different dopant species: oxygen, 4-methoxybenzene, and 4-bromobenzene. Wemore » introduce a route to control dopant functionalization to a low level as a means for introducing spatially well-separated solitary dopant sites. Resolution of emission from solitary dopant sites and correlation to their impact on E 11 emission allows confirmation of dopants as trapping sites for localization of E 11 excitons following their diffusive transport to the dopant site. Imaging of the dopant emission also reveals photoluminescence intermittency (blinking), with blinking dynamics being dependent on the specific dopant. Density functional theory calculations were performed to evaluate the stability of dopants and delineate the possible mechanisms of blinking. Furthermore, theoretical modeling suggests that the trapping of free charges in the potential well created by permanent dipoles introduced by dopant atoms/groups is likely responsible for the blinking, with the strongest effects being predicted and observed for oxygen-doped SWCNTs.« less

Phosphor-free nanopyramid white light-emitting diodes grown on (101{sup ¯}1) planes using nanospherical-lens photolithography

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

Wu, Kui; Department of Electronic Engineering, Tsinghua National Laboratory for Information Science and Technology/State Key Lab on Integrated Optoelectronics, Tsinghua University, Beijing 100084; Wei, Tongbo, E-mail: tbwei@semi.ac.cn

2013-12-09

We reported a high-efficiency and low-cost nano-pattern method, the nanospherical-lens photolithography technique, to fabricate a SiO{sub 2} mask for selective area growth. By controlling the selective growth, we got a highly ordered hexagonal nanopyramid light emitting diodes with InGaN/GaN quantum wells grown on nanofacets, demonstrating an electrically driven phosphor-free white light emission. We found that both the quantum well width and indium incorporation increased linearly along the (101{sup ¯}1) planes towards the substrate and the perpendicular direction to the (101{sup ¯}1) planes as well. Such spatial distribution was responsible for the broadband emission. Moreover, using cathodoluminescence techniques, it was foundmore » that the blue emission originated from nanopyramid top, resembling the quantum dots, green emission from the InGaN quantum wells layer at the middle of sidewalls, and yellow emission mainly from the bottom of nanopyramid ridges, similar to the quantum wires.« less

Semiconductor quantum dot super-emitters: spontaneous emission enhancement combined with suppression of defect environment using metal-oxide plasmonic metafilms

NASA Astrophysics Data System (ADS)

Sadeghi, Seyed M.; Wing, Waylin J.; Gutha, Rithvik R.; Sharp, Christina

2018-01-01

We demonstrate that a metal-oxide plasmonic metafilm consisting of a Si/Al oxide junction in the vicinity of a thin gold layer can quarantine excitons in colloidal semiconductor quantum dots against their defect environments. This process happens while the plasmon fields of the gold layer enhance spontaneous emission decay rates of the quantum dots. We study the emission dynamics of such quantum dots when the distance between the Si/Al oxide junction and the gold thin layer is varied. The results show that for distances less than a critical value the lifetime of the quantum dots can be elongated while they experience intense plasmon fields. This suggests that the metal-oxide metafilm can keep photo-excited electrons in the cores of the quantum dots, suppressing their migration to the surface defect sites. This leads to suppression of Auger recombination, offering quantum dot super-emitters with emission that is enhanced not only by the plasmon fields (Purcell effect), but also by strong suppression of the non-radiative decay caused by the defect sites.

Biological sensing and control of emission dynamics of quantum dot bioconjugates using arrays of long metallic nanorods.

PubMed

Sadeghi, Seyed M; Gutha, Rithvik R; Wing, Waylin J; Sharp, Christina; Capps, Lucas; Mao, Chuanbin

2017-01-01

We study biological sensing using plasmonic and photonic-plasmonic resonances of arrays of ultralong metallic nanorods and analyze the impact of these resonances on emission dynamics of quantum dot bioconjugates. We demonstrate that the LSPRs and plasmonic lattice modes of such array can be used to detect a single self-assembled monolayer of alkanethiol at the visible (550 nm) and near infrared (770 nm) range with well resolved shifts. We study adsorption of streptavidin-quantum dot conjugates to this monolayer, demonstrating that formation of nearly two dimensional arrays of quantum dots with limited emission blinking can lead to extra well-defined wavelength shifts in these modes. Using spectrally-resolved lifetime measurements we study the emission dynamics of such quantum dot bioconjugates within their monodispersed size distribution. We show that, despite their close vicinity to the nanorods, the rate of energy transfer from these quantum dots to nanorods is rather weak, while the plasmon field enhancement can be strong. Our results reveal that the nanorods present a strongly wavelength or size-dependent non-radiative decay channel to the quantum dot bioconjugates.

Acoustically regulated optical emission dynamics from quantum dot-like emission centers in GaN/InGaN nanowire heterostructures

NASA Astrophysics Data System (ADS)

Lazić, S.; Chernysheva, E.; Hernández-Mínguez, A.; Santos, P. V.; van der Meulen, H. P.

2018-03-01

We report on experimental studies of the effects induced by surface acoustic waves on the optical emission dynamics of GaN/InGaN nanowire quantum dots. We employ stroboscopic optical excitation with either time-integrated or time-resolved photoluminescence detection. In the absence of the acoustic wave, the emission spectra reveal signatures originated from the recombination of neutral exciton and biexciton confined in the probed nanowire quantum dot. When the nanowire is perturbed by the propagating acoustic wave, the embedded quantum dot is periodically strained and its excitonic transitions are modulated by the acousto-mechanical coupling. Depending on the recombination lifetime of the involved optical transitions, we can resolve acoustically driven radiative processes over time scales defined by the acoustic cycle. At high acoustic amplitudes, we also observe distortions in the transmitted acoustic waveform, which are reflected in the time-dependent spectral response of our sensor quantum dot. In addition, the correlated intensity oscillations observed during temporal decay of the exciton and biexciton emission suggest an effect of the acoustic piezoelectric fields on the quantum dot charge population. The present results are relevant for the dynamic spectral and temporal control of photon emission in III-nitride semiconductor heterostructures.

Photo-degradation behaviour of roseoflavin in some aqueous solutions

NASA Astrophysics Data System (ADS)

Tyagi, A.; Penzkofer, A.; Mathes, T.; Hegemann, P.

2010-03-01

An absorption and emission spectroscopic characterization of roseoflavin (8-dimethylamino-8-demethyl-riboflavin, RoF) in aqueous solutions was carried out. The studies were concentrated on roseoflavin in pH 8 phosphate buffer. Absorption cross-section spectra, fluorescence excitation spectra, fluorescence quantum distributions, fluorescence quantum yields and fluorescence lifetimes were determined. The fluorescence of RoF is quenched by photo-induced intra-molecular charge-transfer at room temperature. The photo-degradation of RoF in un-buffered water, in Tris-HCl buffer, and in phosphate buffer was studied. Phosphate buffer and to a smaller extent Tris buffer catalyse the RoF photo-degradation. Photo-excitation of the primary photoproduct, 8-methylamino-riboflavin (8-MNH-RF), enhanced the RoF degradation by triplet 8-MNH-RF - singlet RoF excitation transfer with subsequent triplet-state RoF degradation.

Polarized quantum dot emission in electrohydrodynamic jet printed photonic crystals

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

See, Gloria G.; Xu, Lu; Nuzzo, Ralph G.

2015-08-03

Tailored optical output, such as color purity and efficient optical intensity, are critical considerations for displays, particularly in mobile applications. To this end, we demonstrate a replica molded photonic crystal structure with embedded quantum dots. Electrohydrodynamic jet printing is used to control the position of the quantum dots within the device structure. This results in significantly less waste of the quantum dot material than application through drop-casting or spin coating. In addition, the targeted placement of the quantum dots minimizes any emission outside of the resonant enhancement field, which enables an 8× output enhancement and highly polarized emission from themore » photonic crystal structure.« less

CdSe white quantum dots-based white light-emitting diodes with high color rendering index

NASA Astrophysics Data System (ADS)

Su, Yu-Sheng; Hsiao, Chih-Chun; Chung, Shu-Ru

2016-09-01

A white light emission CdSe quantum dots (QDs) can be prepared by chemical route under 180°C. An organic oleic acid (OA) is used to react with CdO to form Cd-OA complex. Hexadecylamine (HDA) and 1-Octadecene (ODE) were used as co-surfactants. By controlling the reaction time, a white light emission CdSe QDs can be obtained after reacts for 3 to 10 min. The luminescence spectra compose two obvious emission peaks and entire visible light ranges from 400 to 650 nm. Based on TEM measurement result, spherical morphologies with particle size 2.39+/-0.27 nm can be obtained. The quantum yields (QYs) of white CdSe QD are between 20 and 60 %, which depends on reaction time. A white CdSe QDs were mixed with UV cured gel (OPAS-226) with weight ratios 50.0 wt. %, and putted the mixture into reflective cup (3020, 13 mil) as convert type. The white LEDs have controllable CIE coordinates and correlated color temperature (CCT). The luminous efficacy of the device is less than 3 lm/W, but the color rendering index (CRI) for all devices are higher than 80. Since the luminous efficacy of hybrid devices has a direct dependence on the external QY of the UV-LED as well, the luminous efficacy can be improved by well dispersion of CdSe QDs in UV gel matrix and using optimized LED chips. Therefore, in this study, we provide a new and simple method to prepare high QY of white CdSe QDs and its have a potential to applicate in solid-state lighting.

Bright nanowire single photon source based on SiV centers in diamond

DOE PAGES

Marseglia, L.; Saha, K.; Ajoy, A.; ...

2018-01-01

The practical implementation of quantum technologies such as quantum commu- nication and quantum cryptography relies on the development of indistinguishable, robust, and bright single photon sources that works at room temperature. The silicon- vacancy (SiV -) center in diamond has emerged as a possible candidate for a single photon source with all these characteristics. Unfortunately, due to the high refraction index mismatch between diamond and air, color centers in diamond show low photon out-coupling. This drawback can be overcome by fabrication of photonic structures that improve the in-coupling of excitation laser to the diamond defect as well as the out-couplingmore » emission from the color centers. An additional shortcoming is due to the random localization of native defects in the diamond sample. Here we demonstrate deterministic implantation of Si ions with high conversion effciency to single SiV -, targeted to fabricated nanowires. The co-localization of single SiV - defects with the nanostructures yields a ten times higher light coupling effciency as compared to single SiV - in the bulk. This result, with its intrinsic scalability, enables a new class of devices for integrated photonics and quantum information processing.« less

Green Synthesis of InP/ZnS Core/Shell Quantum Dots for Application in Heavy-Metal-Free Light-Emitting Diodes

NASA Astrophysics Data System (ADS)

Kuo, Tsung-Rong; Hung, Shih-Ting; Lin, Yen-Ting; Chou, Tzu-Lin; Kuo, Ming-Cheng; Kuo, Ya-Pei; Chen, Chia-Chun

2017-09-01

Quantum dot light-emitting diodes (QD-LEDs) have been considered as potential display technologies with the characterizations of high color purity, flexibility, transparency, and cost efficiency. For the practical applications, the development of heavy-metal-free QD-LEDs from environment-friendly materials is the most important issue to reduce the impacts on human health and environmental pollution. In this work, heavy-metal-free InP/ZnS core/shell QDs with different fluorescence were prepared by green synthesis method with low cost, safe, and environment-friendly precursors. The InP/ZnS core/shell QDs with maximum fluorescence peak at 530 nm, superior fluorescence quantum yield of 60.1%, and full width at half maximum of 55 nm were applied as an emission layer to fabricate multilayered QD-LEDs. The multilayered InP/ZnS core/shell QD-LEDs showed the turn-on voltage at 5 V, the highest luminance (160 cd/m2) at 12 V, and the external quantum efficiency of 0.223% at 6.7 V. Overall, the multilayered InP/ZnS core/shell QD-LEDs reveal potential to be the heavy-metal-free QD-LEDs for future display applications.

Fluorescein isothiocyanate and rhodamine B dye encapsulated mesoporous SiO2 for applications of blue LED excited white LED

NASA Astrophysics Data System (ADS)

Das, Sourav; Manam, J.

2018-05-01

In this work, the fluorescein isothiocyanate (FITC) and rhodamine B (RhB) dyes were encapsulated in mesoporous silica nanoparticles (MSNp). The MSNp-FITC-RhB nanohybrids phosphor showed a dichromatic PL emission at green region and orange region when excited at 460 nm. A Forster Resonance Energy Transfer (FRET) was observed from FITC to RhB. The materials were further characterized by XRD, FTIR, TEM, and temperature dependent photoluminescence. The CIE coordinates were tuned from greenish yellow to the orange region and quantum yield was reached 52.04% based on FRET. So by combining the MSNp-FITC-RhB nanohybrids phosphor with the blue LED chip, the white light emission with flexible Color Correlated Temperature and improved Color Rendering Index can be obtained.

Photophysical properties of a laser dye (LD-473) in different solvents

NASA Astrophysics Data System (ADS)

Ibnaouf, K. H.; Alhathlool, R.; Ali, M. K. M.

2018-06-01

In this paper, we investigated the spectroscopic properties the 1, 2, 3, 8-tetrahydrofuran, 2, 3, 8-(LD-473) dissolved in seven types of solvents with different concentrations. The absorption, emission, fluorescence and its quantum yield and Stokes shift of LD-473 were measured. The amplified spontaneous emission (ASE) spectra of LD-473 have been obtained using a transverse laser cavity configuration, where the LD-473 was pumped by laser pulses from the third harmonic of an Nd: YAG laser (355 nm). LD-473 in non-polar solvents exhibits dual ASEs around 445 and 470 nm, whereas the corresponding fluorescence spectrum shows only one peak around 437 nm. The peak at 470 nm is due to the combination of two excited molecules and the solvent between them.

Emission turn-on and solubility turn-off in conjugated polymers: one- and two-photon-induced removal of fluorescence-quenching solubilizing groups.

PubMed

Schelkle, Korwin M; Becht, Steffy; Faraji, Shirin; Petzoldt, Martin; Müllen, Klaus; Buckup, Tiago; Dreuw, Andreas; Motzkus, Marcus; Hamburger, Manuel

2015-01-01

The synthesis of highly efficient two-photon uncaging groups and their potential use in functional conjugated polymers for post-polymerization modification are reported. Careful structural design of the employed nitrophenethyl caging groups allows to efficiently induce bond scission by a two-photon process through a combination of exceptionally high two-photon absorption cross-sections and high reaction quantum yields. Furthermore, π-conjugated polyfluorenes are functionalized with these photocleavable side groups and it is possible to alter their emission properties and solubility behavior by simple light irradiation. Cleavage of side groups leads to a turn-on of the fluorescence while solubility of the π-conjugated materials is drastically reduced. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis and optical properties of new 5'-aryl-substituted 2,5-bis(3-decyl-2,2'-bithiophen-5-yl)-1,3,4-oxadiazoles.

PubMed

Kostyuchenko, Anastasia Sergeevna; Zheleznova, Tatyana Yu; Stasyuk, Anton Jaroslavovich; Kurowska, Aleksandra; Domagala, Wojciech; Pron, Adam; Fisyuk, Alexander S

2017-01-01

New photoluminescent donor-acceptor-donor (DAD) molecules, namely 5'-aryl-substituted 2,5-bis(3-decyl-2,2'-bithiophen-5-yl)-1,3,4-oxadiazoles were prepared by palladium-catalyzed coupling from readily available compounds such as ethyl 3-decyl-2,2'-bithiophene-5-carboxylate and aryl halides. The obtained compounds feature increasing bathochromic shifts in their emission spectra with increasing aryl-substituent size yielding blue to bluish-green emissions. At the same time, their absorption spectra are almost independent from the identity of the terminal substituent with λ max values ranging from 395 to 405 nm. The observed trends are perfectly predicted by quantum chemical DFT/TDDFT calculations carried out for these new molecules.

Synthesis and optical properties of new 5'-aryl-substituted 2,5-bis(3-decyl-2,2'-bithiophen-5-yl)-1,3,4-oxadiazoles

PubMed Central

Kostyuchenko, Anastasia Sergeevna; Zheleznova, Tatyana Yu; Stasyuk, Anton Jaroslavovich; Kurowska, Aleksandra; Domagala, Wojciech

2017-01-01

New photoluminescent donor–acceptor–donor (DAD) molecules, namely 5'-aryl-substituted 2,5-bis(3-decyl-2,2'-bithiophen-5-yl)-1,3,4-oxadiazoles were prepared by palladium-catalyzed coupling from readily available compounds such as ethyl 3-decyl-2,2'-bithiophene-5-carboxylate and aryl halides. The obtained compounds feature increasing bathochromic shifts in their emission spectra with increasing aryl-substituent size yielding blue to bluish-green emissions. At the same time, their absorption spectra are almost independent from the identity of the terminal substituent with λmax values ranging from 395 to 405 nm. The observed trends are perfectly predicted by quantum chemical DFT/TDDFT calculations carried out for these new molecules. PMID:28326140

Emission polarization control in semiconductor quantum dots coupled to a photonic crystal microcavity.

PubMed

Gallardo, E; Martínez, L J; Nowak, A K; van der Meulen, H P; Calleja, J M; Tejedor, C; Prieto, I; Granados, D; Taboada, A G; García, J M; Postigo, P A

2010-06-07

We study the optical emission of single semiconductor quantum dots weakly coupled to a photonic-crystal micro-cavity. The linearly polarized emission of a selected quantum dot changes continuously its polarization angle, from nearly perpendicular to the cavity mode polarization at large detuning, to parallel at zero detuning, and reversing sign for negative detuning. The linear polarization rotation is qualitatively interpreted in terms of the detuning dependent mixing of the quantum dot and cavity states. The present result is relevant to achieve continuous control of the linear polarization in single photon emitters.

Luminescent zinc(ii) and copper(i) complexes for high-performance solution-processed monochromic and white organic light-emitting devices.

PubMed

Cheng, Gang; So, Gary Kwok-Ming; To, Wai-Pong; Chen, Yong; Kwok, Chi-Chung; Ma, Chensheng; Guan, Xiangguo; Chang, Xiaoyong; Kwok, Wai-Ming; Che, Chi-Ming

2015-08-01

The synthesis and spectroscopic properties of luminescent tetranuclear zinc(ii) complexes of substituted 7-azaindoles and a series of luminescent copper(i) complexes containing 7,8-bis(diphenylphosphino)-7,8-dicarba- nido -undecaborate ligand are described. These complexes are stable towards air and moisture. Thin film samples of the luminescent copper(i) complexes in 2,6-dicarbazolo-1,5-pyridine and zinc(ii) complexes in poly(methyl methacrylate) showed emission quantum yields of up to 0.60 (for Cu-3 ) and 0.96 (for Zn-1 ), respectively. Their photophysical properties were examined by ultrafast time-resolved emission spectroscopy, temperature dependent emission lifetime measurements and density functional theory calculations. Monochromic blue and orange solution-processed OLEDs with these Zn(ii) and Cu(i) complexes as light-emitting dopants have been fabricated, respectively. Maximum external quantum efficiency (EQE) of 5.55% and Commission Internationale de l'Eclairage (CIE) coordinates of (0.16, 0.19) were accomplished with the optimized Zn-1 -OLED while these values were, respectively 15.64% and (0.48, 0.51) for the optimized Cu-3 -OLED. Solution-processed white OLEDs having maximum EQE of 6.88%, CIE coordinates of (0.42, 0.44), and colour rendering index of 81 were fabricated by using these luminescent Zn(ii) and Cu(i) complexes as blue and orange light-emitting dopant materials, respectively.

Fragment emission from the mass-symmetric reactions 58Fe,58Ni +58Fe,58Ni at Ebeam=30 MeV/nucleon

NASA Astrophysics Data System (ADS)

Ramakrishnan, E.; Johnston, H.; Gimeno-Nogues, F.; Rowland, D. J.; Laforest, R.; Lui, Y.-W.; Ferro, S.; Vasal, S.; Yennello, S. J.

1998-04-01

The mass-symmetric reactions 58Fe,58Ni +58Fe,58Ni were studied at a beam energy of Ebeam=30 MeV/nucleon in order to investigate the isospin dependence of fragment emission. Ratios of inclusive yields of isotopic fragments from hydrogen through nitrogen were extracted as a function of laboratory angle. A moving source analysis of the data indicates that at laboratory angles around 40° the yield of intermediate mass fragments (IMF's) beyond Z=3 is predominantly from a midrapidity source. The angular dependence of the relative yields of isotopes beyond Z=3 indicates that the IMF's at more central angles originate from a source which is more neutron deficient than the source responsible for fragments emitted at forward angles. The charge distributions and kinetic energy spectra of the IMF's at various laboratory angles were well reproduced by calculations employing a quantum molecular-dynamics code followed by a statistical multifragmentation model for generating fragments. The calculations indicate that the measured IMF's originate mainly from a single source. The isotopic composition of the emitted fragments is, however, not reproduced by the same calculation. The measured isotopic and isobaric ratios indicate an emitting source that is more neutron rich in comparison to the source predicted by model calculations.

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

Tailoring the chirality of light emission with spherical Si-based antennas.

PubMed

Zambrana-Puyalto, Xavier; Bonod, Nicolas

2016-05-21

Chirality of light is of fundamental importance in several enabling technologies with growing applications in life sciences, chemistry and photodetection. Recently, some attention has been focused on chiral quantum emitters. Consequently, optical antennas which are able to tailor the chirality of light emission are needed. Spherical nanoresonators such as colloids are of particular interest to design optical antennas since they can be synthesized at a large scale and they exhibit good optical properties. Here, we show that these colloids can be used to tailor the chirality of a chiral emitter. To this purpose, we derive an analytic formalism to model the interaction between a chiral emitter and a spherical resonator. We then compare the performances of metallic and dielectric spherical antennas to tailor the chirality of light emission. It is seen that, due to their strong electric dipolar response, metallic spherical nanoparticles spoil the chirality of light emission by yielding achiral fields. In contrast, thanks to the combined excitation of electric and magnetic modes, dielectric Si-based particles feature the ability to inhibit or to boost the chirality of light emission. Finally, it is shown that dual modes in dielectric antennas preserve the chirality of light emission.

Versatile Indolocarbazole-Isomer Derivatives as Highly Emissive Emitters and Ideal Hosts for Thermally Activated Delayed Fluorescent OLEDs with Alleviated Efficiency Roll-Off.

PubMed

Zhang, Dongdong; Song, Xiaozeng; Cai, Minghan; Kaji, Hironori; Duan, Lian

2018-02-01

Maintaining high efficiency at high brightness levels is an exigent challenge for real-world applications of thermally activated delayed fluorescent organic light-emitting diodes (TADF-OLEDs). Here, versatile indolocarbazole-isomer derivatives are developed as highly emissive emitters and ideal hosts for TADF-OLEDs to alleviate efficiency roll-off. It is observed that photophysical and electronic properties of these compounds can be well modulated by varying the indolocarbazole isomers. A photoluminescence quantum yield (η PL ) approaching unity and a maximum external quantum efficiency (EQE max ) of 25.1% are obtained for the emitter with indolo[3,2-a]carbazolyl subunit. Remarkably, record-high EQE/power efficiency of 26.2%/69.7 lm W -1 at the brightness level of 5000 cd m -2 with a voltage of only 3.74 V are also obtained using the same isomer as the host in a green TADF-OLED. It is evident that TADF hosts with high η PL values, fast reverse intersystem crossing processes, and balanced charge transport properties may open the path toward roll-off-free TADF-OLEDs. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The emission wavelength dependent photoluminescence lifetime of the N-doped graphene quantum dots

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

Deng, Xingxia; School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210; University of Chinese Academy of Sciences, Beijing 100049

2015-12-14

Aromatic nitrogen doped graphene quantum dots were investigated by steady-state and time-resolved photoluminescence (PL) techniques. The PL lifetime was found to be dependent on the emission wavelength and coincident with the PL spectrum, which is different from most semiconductor quantum dots and fluorescent dyes. This result shows the synergy and competition between the quantum confinement effect and edge functional groups, which may have the potential to guide the synthesis and expand the applications of graphene quantum dots.

Oligofluorenes as polymeric model compounds for providing insight into the triplets of ketone and ketylimine derivatives.

PubMed

Robert, Patricia; Bolduc, Andréanne; Skene, W G

2012-09-20

A series of oligofluorenes ranging between one and three repeating units were prepared as structurally well-defined representative models of polyfluorenes. The photophysics of the oligofluorene models were investigated both by laser flash photolysis and steady-state fluorescence. The effects of the ketone and ketylimine functional groups in the 9-position on the photophysical properties, notably the triplet quantum yield (Φ(TT)) by intersystem crossing and the absolute fluorescence quantum yields (Φ(fl)), were investigated. The singlet depletion method was used to determine both the Φ(TT) and molar absorption coefficients of the observed triplets (ε(TT)). Meanwhile, the absolute Φ(fl) were determined using an integrating sphere. It was found that both the ketone and ketylimine substituents and the degree of oligomerization contributed to quenching the oligofluorene fluorescence. For example, the Φ(fl) was quenched 5-fold with the ketylimine and ketone substituents for the bifluorenyl derivatives compared to their corresponding 9,9-dihexyl bifluorenyl counterparts. Meanwhile, the Φ(fl) quenching increased 14 times with the trifluorenyl ketone and ketylimine derivatives. Measured Φ(TT) values ranged between 22 and 43% for the difluorenyl derivatives with ε(TT) on the order of 13 000 cm(-1) M(-1). The Φ(TT) decreased to <10% concomitant with doubling of the ε(TT) when the degree of oligomerization was increased to 3. A new fluorescence emission at 545 nm formed at low temperatures for the ketone and ketylimine oligofluorene derivatives. The emission intensity was dependent on the temperature, and it disappeared at room temperature.

Direct evidence of single quantum dot emission from GaN islands formed at threading dislocations using nanoscale cathodoluminescence: A source of single photons in the ultraviolet

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

Schmidt, Gordon, E-mail: Gordon.Schmidt@ovgu.de; Berger, Christoph; Veit, Peter

2015-06-22

Intense emission from GaN islands embedded in AlN resulting from GaN/AlN quantum well growth is directly resolved by performing cathodoluminescence spectroscopy in a scanning transmission electron microscope. Line widths down to 440 μeV are measured in a wavelength region between 220 and 310 nm confirming quantum dot like electronic properties in the islands. These quantum dot states can be structurally correlated to islands of slightly enlarged thicknesses of the GaN/AlN quantum well layer preferentially formed in vicinity to dislocations. The quantum dot states exhibit single photon emission in Hanbury Brown-Twiss experiments with a clear antibunching in the second order correlation function atmore » zero time delay.« less

Field electron emission based on resonant tunneling in diamond/CoSi2/Si quantum well nanostructures

PubMed Central

Gu, Changzhi; Jiang, Xin; Lu, Wengang; Li, Junjie; Mantl, Siegfried

2012-01-01

Excellent field electron emission properties of a diamond/CoSi2/Si quantum well nanostructure are observed. The novel quantum well structure consists of high quality diamond emitters grown on bulk Si substrate with a nanosized epitaxial CoSi2 conducting interlayer. The results show that the main emission properties were modified by varying the CoSi2 thickness and that stable, low-field, high emission current and controlled electron emission can be obtained by using a high quality diamond film and a thicker CoSi2 interlayer. An electron resonant tunneling mechanism in this quantum well structure is suggested, and the tunneling is due to the long electron mean free path in the nanosized CoSi2 layer. This structure meets most of the requirements for development of vacuum micro/nanoelectronic devices and large-area cold cathodes for flat-panel displays. PMID:23082241

Field electron emission based on resonant tunneling in diamond/CoSi2/Si quantum well nanostructures.

PubMed

Gu, Changzhi; Jiang, Xin; Lu, Wengang; Li, Junjie; Mantl, Siegfried

2012-01-01

Excellent field electron emission properties of a diamond/CoSi(2)/Si quantum well nanostructure are observed. The novel quantum well structure consists of high quality diamond emitters grown on bulk Si substrate with a nanosized epitaxial CoSi(2) conducting interlayer. The results show that the main emission properties were modified by varying the CoSi(2) thickness and that stable, low-field, high emission current and controlled electron emission can be obtained by using a high quality diamond film and a thicker CoSi(2) interlayer. An electron resonant tunneling mechanism in this quantum well structure is suggested, and the tunneling is due to the long electron mean free path in the nanosized CoSi(2) layer. This structure meets most of the requirements for development of vacuum micro/nanoelectronic devices and large-area cold cathodes for flat-panel displays.

Synthesis of Carbon Dots with Multiple Color Emission by Controlled Graphitization and Surface Functionalization.

PubMed

Miao, Xiang; Qu, Dan; Yang, Dongxue; Nie, Bing; Zhao, Yikang; Fan, Hongyou; Sun, Zaicheng

2018-01-01

Multiple-color-emissive carbon dots (CDots) have potential applications in various fields such as bioimaging, light-emitting devices, and photocatalysis. The majority of the current CDots to date exhibit excitation-wavelength-dependent emissions with their maximum emission limited at the blue-light region. Here, a synthesis of multiple-color-emission CDots by controlled graphitization and surface function is reported. The CDots are synthesized through controlled thermal pyrolysis of citric acid and urea. By regulating the thermal-pyrolysis temperature and ratio of reactants, the maximum emission of the resulting CDots gradually shifts from blue to red light, covering the entire light spectrum. Specifically, the emission position of the CDots can be tuned from 430 to 630 nm through controlling the extent of graphitization and the amount of surface functional groups, COOH. The relative photoluminescence quantum yields of the CDots with blue, green, and red emission reach up to 52.6%, 35.1%, and 12.9%, respectively. Furthermore, it is demonstrated that the CDots can be uniformly dispersed into epoxy resins and be fabricated as transparent CDots/epoxy composites for multiple-color- and white-light-emitting devices. This research opens a door for developing low-cost CDots as alternative phosphors for light-emitting devices. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum Emitters in Two-Dimensional Structured Reservoirs in the Nonperturbative Regime

NASA Astrophysics Data System (ADS)

González-Tudela, A.; Cirac, J. I.

2017-10-01

We show that the coupling of quantum emitters to a two-dimensional reservoir with a simple band structure gives rise to exotic quantum dynamics with no analogue in other scenarios and which cannot be captured by standard perturbative treatments. In particular, for a single quantum emitter with its transition frequency in the middle of the band, we predict an exponential relaxation at a rate different from that predicted by Fermi's golden rule, followed by overdamped oscillations and slow relaxation decay dynamics. This is accompanied by directional emission into the reservoir. This directionality leads to a modification of the emission rate for few emitters and even perfect subradiance, i.e., suppression of spontaneous emission, for four quantum emitters.

Synthesis, spectral behaviour and photophysics of donor-acceptor kind of chalcones: Excited state intramolecular charge transfer and fluorescence quenching studies

NASA Astrophysics Data System (ADS)

Pannipara, Mehboobali; Asiri, Abdullah M.; Alamry, Khalid A.; Arshad, Muhammad N.; El-Daly, Samy A.

2015-02-01

The spectral and photophysical properties of two chalcones containing electron donating and accepting groups with intramolecular charge transfer characteristics were synthesized and characterized by 1H NMR, 13C NMR and X-ray crystallography. Both compounds show very strong solvent polarity dependent changes in their photophysical characteristics, namely, remarkable red shift in the emission spectra with increasing solvent polarity, large change in Stokes shift, significant reduction in the fluorescence quantum yield; indicating that the fluorescence states of these compounds are of intramolecular charge transfer (ICT) character. The solvent effect on the photophysical parameters such as singlet absorption, molar absorptivity, oscillator strength, dipole moment, fluorescence spectra, and fluorescence quantum yield of both compounds have been investigated comprehensively. For both dyes, Lippert-Mataga and Reichardt's correlations were used to estimate the difference between the excited and ground state dipole moments (Δμ). The interactions of dyes with colloidal silver nanoparticles (Ag NPs) were also studied in ethanol using steady state fluorescence quenching measurements. The fluorescence quenching data reveal that dynamic quenching and energy transfer play a major role in the fluorescence quenching of dyes by Ag NPs.

Diboron compound-based organic light-emitting diodes with high efficiency and reduced efficiency roll-off

NASA Astrophysics Data System (ADS)

Wu, Tien-Lin; Huang, Min-Jie; Lin, Chih-Chun; Huang, Pei-Yun; Chou, Tsu-Yu; Chen-Cheng, Ren-Wu; Lin, Hao-Wu; Liu, Rai-Shung; Cheng, Chien-Hong

2018-04-01

Organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) materials are promising for the realization of highly efficient light emitters. However, such devices have so far suffered from efficiency roll-off at high luminance. Here, we report the design and synthesis of two diboron-based molecules, CzDBA and tBuCzDBA, which show excellent TADF properties and yield efficient OLEDs with very low efficiency roll-off. These donor-acceptor-donor (D-A-D) type and rod-like compounds concurrently generate TADF with a photoluminescence quantum yield of 100% and an 84% horizontal dipole ratio in the thin film. A green OLED based on CzDBA exhibits a high external quantum efficiency of 37.8 ± 0.6%, a current efficiency of 139.6 ± 2.8 cd A-1 and a power efficiency of 121.6 ± 3.1 lm W-1 with an efficiency roll-off of only 0.3% at 1,000 cd m-2. The device has a peak emission wavelength of 528 nm and colour coordinates of the Commission International de ĺEclairage (CIE) of (0.31, 0.61), making it attractive for colour-display applications.

Discrimination and quantification of autofluorescence spectra of human lung cells

NASA Astrophysics Data System (ADS)

Rahmani, Mahya; Khani, Mohammad Mehdi; Khazaei Koohpar, Zeinab; Molik, Paria

2016-10-01

To study laser-induced autofluorescence spectroscopy of the human lung cell line, we evaluated the native fluorescence properties of cancer QU-DB and normal MRC-5 human lung cells during continuous exposure to 405 nm laser light. Two emission bands centered at ~470 nm and ~560 nm were observed. These peaks are most likely attributable to mitochondrial fluorescent reduced nicotinamide adenine dinucleotide and riboflavin fluorophores, respectively. This article highlights lung cell autofluorescence characterization and signal discrimination by collective investigation of different spectral features. The absolute intensity, the spectral shape factor or redox ratio, the full width of half-maximum and the full width of quarter maximum was evaluated. Moreover, the intensity ratio, the area under the peak and the area ratio as a contrast factor for normal and cancerous cells were also calculated. Among all these features it seems that the contrast factor precisely and significantly discriminates the spectral differences of normal and cancerous lung cells. On the other hand, the relative quantum yield for both cell types were found by comparing the quantum yield of an unknown compound with known fluorescein sodium as a reference solution.

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

Yang, Lu; Zhang, Sheng; Qu, Xiaoni

Lanthanide MOFs, [Eu(TCA)(NDC)·H{sub 2}O]{sub n} (1) and [Tb(TCA)(NDC)·H{sub 2}O]{sub n} (2), have been prepared with the mixed aromatic carboxylate ligands, namely, 4,4′,4″-tricarboxytriphenylamine (H{sub 3}TCA) and 1,4-naphthalenedicarboxylate (H{sub 2}NDC). Single-crystal X-ray diffraction analysis reveals that isomorphic 1 and 2 present pillar-layered 3D framework that Eu/Tb(III) bond with carboxylate in various coordination fashions. Optical investigation indicates that the as-prepared compounds feature characteristic luminescence emission bands of Eu/Tb ions in the visible regions at room temperature. Moreover, compound 2 shows a relatively longer luminescence lifetime (τ=0.342 ms) and significantly enhanced quantum yield (Φ{sub overall}=11%) comparing with those of 1 (τ=0.335 ms, Φ{sub overall}=0.06%).more » - Graphical abstract: Synoptic: Two Ln-MOFs (Ln=Eu{sup III}, Tb{sup III}) with mixed polycarboxylate ligands present different luminescent properties. - Highlights: • Two Eu/Tb-MOFs with H{sub 3}TCA and H{sub 2}NDC ligands have been obtained. • The ancillary ligand is employed to decrease water molecule coordinate numbers. • 2displays superior quantum yield and lifetime than those of 1.« less

Control of spontaneous emission of quantum dots using correlated effects of metal oxides and dielectric materials

NASA Astrophysics Data System (ADS)

Sadeghi, S. M.; Wing, W. J.; Gutha, R. R.; Capps, L.

2017-03-01

We study the emission dynamics of semiconductor quantum dots in the presence of the correlated impact of metal oxides and dielectric materials. For this we used layered material structures consisting of a base substrate, a dielectric layer, and an ultrathin layer of a metal oxide. After depositing colloidal CdSe/ZnS quantum dots on the top of the metal oxide, we used spectral and time-resolved techniques to show that, depending on the type and thickness of the dielectric material, the metal oxide can characteristically change the interplay between intrinsic excitons, defect states, and the environment, offering new material properties. Our results show that aluminum oxide, in particular, can strongly change the impact of amorphous silicon on the emission dynamics of quantum dots by balancing the intrinsic near band emission and fast trapping of carriers. In such a system the silicon/aluminum oxide charge barrier can lead to large variation of the radiative lifetime of quantum dots and control of the photo-ejection rate of electrons in quantum dots. The results provide unique techniques to investigate and modify physical properties of dielectrics and manage optical and electrical properties of quantum dots.

Control of spontaneous emission of quantum dots using correlated effects of metal oxides and dielectric materials.

PubMed

Sadeghi, S M; Wing, W J; Gutha, R R; Capps, L

2017-03-03

We study the emission dynamics of semiconductor quantum dots in the presence of the correlated impact of metal oxides and dielectric materials. For this we used layered material structures consisting of a base substrate, a dielectric layer, and an ultrathin layer of a metal oxide. After depositing colloidal CdSe/ZnS quantum dots on the top of the metal oxide, we used spectral and time-resolved techniques to show that, depending on the type and thickness of the dielectric material, the metal oxide can characteristically change the interplay between intrinsic excitons, defect states, and the environment, offering new material properties. Our results show that aluminum oxide, in particular, can strongly change the impact of amorphous silicon on the emission dynamics of quantum dots by balancing the intrinsic near band emission and fast trapping of carriers. In such a system the silicon/aluminum oxide charge barrier can lead to large variation of the radiative lifetime of quantum dots and control of the photo-ejection rate of electrons in quantum dots. The results provide unique techniques to investigate and modify physical properties of dielectrics and manage optical and electrical properties of quantum dots.

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(+).

Photon antibunching from a single quantum-dot-microcavity system in the strong coupling regime.

PubMed

Press, David; Götzinger, Stephan; Reitzenstein, Stephan; Hofmann, Carolin; Löffler, Andreas; Kamp, Martin; Forchel, Alfred; Yamamoto, Yoshihisa

2007-03-16

We observe antibunching in the photons emitted from a strongly coupled single quantum dot and pillar microcavity in resonance. When the quantum dot was spectrally detuned from the cavity mode, the cavity emission remained antibunched, and also anticorrelated from the quantum dot emission. Resonant pumping of the selected quantum dot via an excited state enabled these observations by eliminating the background emitters that are usually coupled to the cavity. This device demonstrates an on-demand single-photon source operating in the strong coupling regime, with a Purcell factor of 61+/-7 and quantum efficiency of 97%.

Solvatochromism in highly luminescent environmental friendly carbon quantum dots for sensing applications: Conversion of bio-waste into bio-asset

NASA Astrophysics Data System (ADS)

Pramanik, A.; Biswas, S.; Kumbhakar, P.

2018-02-01

Recently studies on synthesis and fluorescence based sensing in biocompatible carbon quantum dots (CQDs) have become a widely spoken topic of research due to the several advantageous properties of CQDs in compared to semiconductor quantum dots. In this work, we have reported the rarely reported solvatochromism along-with a high photoluminescence (PL) quantum yield (PLQY) of 22%. Samples have been synthesized by using a simple process of hydrothermal carbonization of a naturally occurring bio-waste i.e. Aegle marmelos leaves powder. The linear absorption and PL emission characteristics of CQDs have been studied in different solvent environments to explore the origin of the observed excitation dependent PL emissions characteristics of the sample. The interesting solvatochromic PL (SPL) behavior of CQDs are observed at an excitation wavelength of 325 nm by dispersing them in different polar protic and aprotic solvents, which suggest their possible applications as a replacement of solvatochromic dye molecules for sensing applications. Different polarity functions and molecular-microscopic solvent polarity parameter (ETN) are used to calculate the change in dipole moment (Δδ) of the solute-solvent system and the origin of SPL in CQDs has been explained. The SPL behavior of CQDs has been utilized for fluorescence sensing of organic liquids (Ethanol and Tetrahydrofuran) in water. Whereas, the photo-induced electron transfer mediated quenching in PL of aqueous dispersion of CQDs has led to development of ;turn off; fluorescence Fe3 + ion sensor with a detection limit of 0.12 μM. Therefore, this work may open a new avenue of conversion of a bio-waste into a fluorescent bio-asset.

Halocarbon emissions by selected tropical seaweeds: species-specific and compound-specific responses under changing pH.

PubMed

Mithoo-Singh, Paramjeet Kaur; Keng, Fiona S-L; Phang, Siew-Moi; Leedham Elvidge, Emma C; Sturges, William T; Malin, Gill; Abd Rahman, Noorsaadah

2017-01-01

Five tropical seaweeds, Kappaphycus alvarezii (Doty) Doty ex P.C. Silva, Padina australis Hauck, Sargassum binderi Sonder ex J. Agardh (syn. S. aquifolium (Turner) C. Agardh), Sargassum siliquosum J. Agardh and Turbinaria conoides (J. Agardh) Kützing, were incubated in seawater of pH 8.0, 7.8 (ambient), 7.6, 7.4 and 7.2, to study the effects of changing seawater pH on halocarbon emissions. Eight halocarbon species known to be emitted by seaweeds were investigated: bromoform (CHBr 3 ), dibro-momethane (CH 2 Br 2 ), iodomethane (CH 3 I), diiodomethane (CH 2 I 2 ), bromoiodomethane (CH 2 BrI), bromochlorometh-ane (CH 2 BrCl), bromodichloromethane (CHBrCl 2 ), and dibro-mochloromethane (CHBr 2 Cl). These very short-lived halocarbon gases are believed to contribute to stratospheric halogen concentrations if released in the tropics. It was observed that the seaweeds emit all eight halocarbons assayed, with the exception of K. alvarezii and S. binderi for CH 2 I 2 and CH 3 I respectively, which were not measurable at the achievable limit of detection. The effect of pH on halocarbon emission by the seaweeds was shown to be species-specific and compound specific. The highest percentage changes in emissions for the halocarbons of interest were observed at the lower pH levels of 7.2 and 7.4 especially in Padina australis and Sargassum spp., showing that lower seawater pH causes elevated emissions of some halocarbon compounds. In general the seaweed least affected by pH change in terms of types of halocarbon emission, was P. australis . The commercially farmed seaweed K. alvarezii was very sensitive to pH change as shown by the high increases in most of the compounds in all pH levels relative to ambient. In terms of percentage decrease in maximum quantum yield of photosynthesis ( F v ∕ F m ) prior to and after incubation, there were no significant correlations with the various pH levels tested for all seaweeds. The correlation between percentage decrease in the maximum quantum yield of photosynthesis ( F v ∕ F m ) and halocarbon emission rates, was significant only for CH 2 BrCl emission by P. australis ( r  = 0.47; p  ≤ 0.04), implying that photosynthesis may not be closely linked to halocarbon emissions by the seaweeds studied. Bromine was the largest contributor to the total mass of halogen emitted for all the seaweeds at all pH. The highest total amount of bromine emitted by K. alvarezii (an average of 98% of total mass of halogens) and the increase in the total amount of chlorine with decreasing seawater pH fuels concern for the expanding seaweed farming activities in the ASEAN region.

Halocarbon emissions by selected tropical seaweeds: species-specific and compound-specific responses under changing pH

PubMed Central

Leedham Elvidge, Emma C.; Sturges, William T.; Malin, Gill; Abd Rahman, Noorsaadah

2017-01-01

Five tropical seaweeds, Kappaphycus alvarezii (Doty) Doty ex P.C. Silva, Padina australis Hauck, Sargassum binderi Sonder ex J. Agardh (syn. S. aquifolium (Turner) C. Agardh), Sargassum siliquosum J. Agardh and Turbinaria conoides (J. Agardh) Kützing, were incubated in seawater of pH 8.0, 7.8 (ambient), 7.6, 7.4 and 7.2, to study the effects of changing seawater pH on halocarbon emissions. Eight halocarbon species known to be emitted by seaweeds were investigated: bromoform (CHBr3), dibro­momethane (CH2Br2), iodomethane (CH3I), diiodomethane (CH2I2), bromoiodomethane (CH2BrI), bromochlorometh­ane (CH2BrCl), bromodichloromethane (CHBrCl2), and dibro­mochloromethane (CHBr2Cl). These very short-lived halocarbon gases are believed to contribute to stratospheric halogen concentrations if released in the tropics. It was observed that the seaweeds emit all eight halocarbons assayed, with the exception of K. alvarezii and S. binderi for CH2I2 and CH3I respectively, which were not measurable at the achievable limit of detection. The effect of pH on halocarbon emission by the seaweeds was shown to be species-specific and compound specific. The highest percentage changes in emissions for the halocarbons of interest were observed at the lower pH levels of 7.2 and 7.4 especially in Padina australis and Sargassum spp., showing that lower seawater pH causes elevated emissions of some halocarbon compounds. In general the seaweed least affected by pH change in terms of types of halocarbon emission, was P. australis. The commercially farmed seaweed K. alvarezii was very sensitive to pH change as shown by the high increases in most of the compounds in all pH levels relative to ambient. In terms of percentage decrease in maximum quantum yield of photosynthesis (Fv∕Fm) prior to and after incubation, there were no significant correlations with the various pH levels tested for all seaweeds. The correlation between percentage decrease in the maximum quantum yield of photosynthesis (Fv∕Fm) and halocarbon emission rates, was significant only for CH2BrCl emission by P. australis (r = 0.47; p ≤ 0.04), implying that photosynthesis may not be closely linked to halocarbon emissions by the seaweeds studied. Bromine was the largest contributor to the total mass of halogen emitted for all the seaweeds at all pH. The highest total amount of bromine emitted by K. alvarezii (an average of 98% of total mass of halogens) and the increase in the total amount of chlorine with decreasing seawater pH fuels concern for the expanding seaweed farming activities in the ASEAN region. PMID:28149690

QED (quantum-electrodynamical) theory of excess spontaneous emission noise

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

Milonni, P.W.

1990-01-01

The results of a quantum-electrodynamical theory of excess spontaneous emission noise in lossy resonators will be presented. The Petermann K factor'' does not enter into the spontaneous emission rate of a single atom in the cavity. The QED theory allows different interpretations of the K factor, and we use this fact to justify semiclassical analyses and to provide in one example a simple derivation of K in terms of the amplification of the quantum vacuum field entering the resonator through its mirrors. 17 refs.

Local surface plasmon enhanced polarization and internal quantum efficiency of deep ultraviolet emissions from AlGaN-based quantum wells.

PubMed

Zhang, Cai; Tang, Ning; Shang, Liangliang; Fu, Lei; Wang, Weiying; Xu, Fujun; Wang, Xinqiang; Ge, Weikun; Shen, Bo

2017-05-24

We report the enhancement of the polarization and internal quantum efficiency (IQE) of deep-UV LEDs by evaporating Al nanoparticles on the device surface to induce localized surface plasmons (LSPs). The deep-UV LEDs polarization is improved due to part of TM emission turns into TE emission through LSPs coupling. The significantly enhanced IQE is attributed to LSPs coupling, which suppress the participation of delocalized and dissociated excitons to non-radiative recombination process.

(11-22) semipolar InGaN emitters from green to amber on overgrown GaN on micro-rod templates

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

Bai, J., E-mail: j.bai@sheffield.ac.uk; Xu, B.; Guzman, F. G.

2015-12-28

We demonstrate semipolar InGaN single-quantum-well light emitting diodes (LEDs) in the green, yellow-green, yellow and amber spectral region. The LEDs are grown on our overgrown semipolar (11-22) GaN on micro-rod array templates, which are fabricated on (11-22) GaN grown on m-plane sapphire. Electroluminescence measurements on the (11-22) green LED show a reduced blue-shift in the emission wavelength with increasing driving current, compared to a reference commercial c-plane LED. The blue-shifts for the yellow-green and yellow LEDs are also significantly reduced. All these suggest an effective suppression in quantum confined Stark effect in our (11-22) LEDs. On-wafer measurements yield a linearmore » increase in the light output with the current, and external quantum efficiency demonstrates a significant improvement in the efficiency-droop compared to a commercial c-plane LED. Electro-luminescence polarization measurements show a polarization ratio of about 25% in our semipolar LEDs.« less

Effect of Ligand Exchange on the Photoluminescence Properties of Cu-Doped Zn-In-Se Quantum Dots

NASA Astrophysics Data System (ADS)

Dong, Xiaofei; Xu, Jianping; Yang, Hui; Zhang, Xiaosong; Mo, Zhaojun; Shi, Shaobo; Li, Lan; Yin, Shougen

2018-04-01

The surface-bound ligands of a semiconductor nanocrystal can affect its electron transition behavior. We investigate the photoluminescence (PL) properties of Cu-doped Zn-In-Se quantum dots (QDs) through the exchange of oleylamine with 6-mercaptohexanol (MCH). Fourier transform infrared and 1H nuclear magnetic resonance spectroscopies, and mass spectrometry reveal that the short-chain MCH molecules are bound to the QD surface. The emission peaks remain unchanged after ligand exchange, and the PL quantum yield is reduced from 49% to 38%. The effects of particle size and defect type on the change in PL behavior upon ligand substitution are excluded through high-resolution transmission electron microscopy, UV-Vis absorption, and PL spectroscopies. The origin of the decreased PL intensity is associated with increased ligand density and the stronger ligand electron-donating abilities of MCH-capped QDs that induce an increase in the nonradiative transition probability. A lower PL quenching transition temperature is observed for MCH-capped QDs and is associated with increasing electron-acoustic phonon coupling due to the lower melting temperature of MCH.

Study on the structural, optical, and electrical properties of the yellow light-emitting diode grown on free-standing (0001) GaN substrate

NASA Astrophysics Data System (ADS)

Deng, Gaoqiang; Zhang, Yuantao; Yu, Ye; Yan, Long; Li, Pengchong; Han, Xu; Chen, Liang; Zhao, Degang; Du, Guotong

2018-04-01

In this paper, GaN-based yellow light-emitting diodes (LEDs) were homoepitaxially grown on free-standing (0001) GaN substrates by metal-organic chemical vapor deposition. X-ray diffraction (XRD), photoluminescence (PL), and electroluminescence (EL) measurements were conducted to investigate the structural, optical, and electrical properties of the yellow LED. The XRD measurement results showed that the InGaN/GaN multiple quantum wells (MQWs) in the LED structure have good periodicity because the distinct MQWs related higher order satellite peaks can be clearly observed from the profile of 2θ-ω XRD scan. The low temperature (10 K) and room temperature PL measurement results yield an internal quantum efficiency of 16% for the yellow LED. The EL spectra of the yellow LED present well Gaussian distribution with relatively low linewidth (47-55 nm), indicating the homogeneous In-content in the InGaN quantum well layers in the yellow LED structure. It is believed that this work will aid in the future development of GaN on GaN LEDs with long emission wavelength.

Shedding light into the detailed excited-state relaxation pathways and reaction mechanisms of thionaphthol isomers.

PubMed

Riyad, Yasser M; Naumov, Sergej; Hermann, Ralf; Abel, Bernd

2011-02-10

Nanosecond laser flash photolysis employing transient detection of emission and absorption in combination with pulse radiolysis and quantum theory has been employed to shed light into the kinetics, quantum yields, and mechanisms of the deactivation of the first excited singlet state of 1- and 2-thionaphthols (NpSH(S(1))). In contrast to thiophenols (ArSH(S(1))), the results revealed that the decay of the first excited singlet state of 1- and 2-thionaphthols (NpSH(S(1))) is governed by radiationless internal conversion (Φ(IC) = 0.29-0.46; 0.016-0.190) and intersystem crossing (Φ(ISC) = 0.14-0.15; 0.4-0.6), respectively, with pronounced S-H photodissociation (Φ(D) = 0.40-0.55; 0.35-0.40). Fluorescence as a deactivation channel plays a minor role (Φ(F) = 0.001-0.010; 0.010-0.034). Quantum chemical calculations helped in understanding the formation of naphthylthiyl radicals and rationalizing the differences in the efficiency of intersystem crossing of the 1- and 2-thionaphthol systems.

New Molecular Design Concurrently Providing Superior Pure Blue, Thermally Activated Delayed Fluorescence and Optical Out-Coupling Efficiencies.

PubMed

Rajamalli, P; Senthilkumar, N; Huang, P-Y; Ren-Wu, C-C; Lin, H-W; Cheng, C-H

2017-08-16

Simultaneous enhancement of out-coupling efficiency, internal quantum efficiency, and color purity in thermally activated delayed fluorescence (TADF) emitters is highly desired for the practical application of these materials. We designed and synthesized two isomeric TADF emitters, 2DPyM-mDTC and 3DPyM-pDTC, based on di(pyridinyl)methanone (DPyM) cores as the new electron-accepting units and di(tert-butyl)carbazole (DTC) as the electron-donating units. 3DPyM-pDTC, which is structurally nearly planar with a very small ΔE ST , shows higher color purity, horizontal ratio, and quantum yield than 2DPyM-mDTC, which has a more flexible structure. An electroluminescence device based on 3DPyM-pDTC as the dopant emitter can reach an extremely high external quantum efficiency of 31.9% with a pure blue emission. This work also demonstrates a way to design materials with a high portion of horizontal molecular orientation to realize a highly efficient pure-blue device based on TADF emitters.

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

DOE PAGES

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai; ...

2017-10-23

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Complete coherent control of silicon vacancies in diamond nanopillars containing single defect centers

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

Zhang, Jingyuan Linda; Lagoudakis, Konstantinos G.; Tzeng, Yan -Kai

Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon-vacancy (SiV) centers in diamond offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye–Waller factor. The possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times makes them promising candidates for qubits. Here, we have developed arrays of nanopillars containing single (SiV) centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the excited state population of a single SiV center at the opticalmore » transition frequency. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the excited state population of individual SiV centers on picosecond timescales using ultrafast optical pulses. Furthermore, this work opens new opportunities to create a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.« less

Deep Blue Phosphorescent Organic Light-Emitting Diodes with CIEy Value of 0.11 and External Quantum Efficiency up to 22.5.

PubMed

Li, Xiaoyue; Zhang, Juanye; Zhao, Zifeng; Wang, Liding; Yang, Hannan; Chang, Qiaowen; Jiang, Nan; Liu, Zhiwei; Bian, Zuqiang; Liu, Weiping; Lu, Zhenghong; Huang, Chunhui

2018-03-01

Organic light-emitting diodes (OLEDs) based on red and green phosphorescent iridium complexes are successfully commercialized in displays and solid-state lighting. However, blue ones still remain a challenge on account of their relatively dissatisfactory Commission International de L'Eclairage (CIE) coordinates and low efficiency. After analyzing the reported blue iridium complexes in the literature, a new deep-blue-emitting iridium complex with improved photoluminescence quantum yield is designed and synthesized. By rational screening host materials showing high triplet energy level in neat film as well as the OLED architecture to balance electron and hole recombination, highly efficient deep-blue-emission OLEDs with a CIE at (0.15, 0.11) and maximum external quantum efficiency (EQE) up to 22.5% are demonstrated. Based on the transition dipole moment vector measurement with a variable-angle spectroscopic ellipsometry method, the ultrahigh EQE is assigned to a preferred horizontal dipole orientation of the iridium complex in doped film, which is beneficial for light extraction from the OLEDs. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optical properties of thin films of zinc oxide quantum dots and polydimethylsiloxane: UV-blocking and the effect of cross-linking.

PubMed

Eita, Mohamed; El Sayed, Ramy; Muhammed, Mamoun

2012-12-01

Thin films of polydimethylsiloxane (PDMS) and ZnO quantum dots (QDs) were built up as multilayers by spin-coating. The films are characterized by a UV-blocking ability that increases with increasing number of bilayers. Photoluminescence (PL) emission spectra of the thin films occur at 522 nm, which is the PL wavelength of the ZnO QDs dispersion, but with a lower intensity and a quantum yield (QY) less than 1% that of the dispersion. Cross-linking has introduced new features to the absorption spectra in that the absorption peak was absent. These changes were attributed to the morphological and structural changes revealed by transmission electron microscopy (TEM) and Fourier transform infrared spectroscopy (FTIR), respectively. TEM showed that the ZnO particle size in the film increased from 7 (±2.7) nm to 16 (±7.8) upon cross-linking. The FTIR spectra suggest that ZnO QDs are involved in the cross-linking of PDMS and that the surface of the ZnO QDs has been chemically modified. Copyright © 2012 Elsevier Inc. All rights reserved.

Highly Efficient Red and White Organic Light-Emitting Diodes with External Quantum Efficiency beyond 20% by Employing Pyridylimidazole-Based Metallophosphors.

PubMed

Miao, Yanqin; Tao, Peng; Wang, Kexiang; Li, Hongxin; Zhao, Bo; Gao, Long; Wang, Hua; Xu, Bingshe; Zhao, Qiang

2017-11-01

Two highly efficient red neutral iridium(III) complexes, Ir1 and Ir2, were rationally designed and synthesized by selecting two pyridylimidazole derivatives as the ancillary ligands. Both Ir1 and Ir2 show nearly the same photoluminescence emission with the maximum peak at 595 nm (shoulder band at about 638 nm) and achieve high solution quantum yields of up to 0.47 for Ir1 and 0.57 for Ir2. Employing Ir1 and Ir2 as emitters, the fabricated red organic light-emitting diodes (OLEDs) show outstanding performance with the maximum external quantum efficiency (EQE), current efficiency (CE), and power efficiency (PE) of 20.98%, 33.04 cd/A, and 33.08 lm/W for the Ir1-based device and 22.15%, 36.89 cd/A, and 35.85 lm/W for the Ir2-based device, respectively. Furthermore, using Ir2 as red emitter, a trichromatic hybrid white OLED, showing good warm white emission with low correlated color temperature of <2200 K under the voltage of 4-6 V, was fabricated successfully. The white device also realizes excellent device efficiencies with the maximum EQE, CE, and PE reaching 22.74%, 44.77 cd/A, and 46.89 lm/W, respectively. Such high electroluminescence performance for red and white OLEDs indicates that Ir1 and Ir2 as efficient red phosphors have great potential for future OLED displays and lightings applications.

Synthesis and characterization of high quantum yield and oscillator strength 6-chloro-2-(4-cynophenyl)-4-phenyl quinoline (cl-CN-DPQ) organic phosphor for solid-state lighting.

PubMed

Ghate, Minakshi; Dahule, H K; Thejo Kalyani, N; Dhoble, S J

2018-03-01

A novel blue luminescent 6-chloro-2-(4-cynophenyl) substituted diphenyl quinoline (Cl-CN DPQ) organic phosphor has been synthesized by the acid-catalyzed Friedlander reaction and then characterized to confirm structural, optical and thermal properties. Structural properties of Cl-CN-DPQ were analyzed by Fourier transform infrared (FTIR), nuclear magnetic resonance (NMR) spectroscopy, X-ray diffraction technique (XRD) and scanning electron microscopy (SEM) and energy dispersive analysis of X-ray (EDAX) spectroscopy. FTIR spectra confirmed the presence of different functional groups and bond stretching. 1 H-NMR and 13 C-NMR confirmed the formation of an organic Cl-CN-DPQ compound. X-ray diffraction study provided its crystalline nature. The surface morphology of Cl-CN-DPQ was analyzed by SEM, while EDAX spectroscopy revealed the elemental analysis. Differential thermal analysis (TGA/DTA) disclosed its thermal stability up to 250°C. The optical properties of Cl-CN-DPQ were investigated by UV-vis absorption and photoluminescence (PL) measurements. Cl-CN-DPQ exhibits intense blue emission at 434 nm in a solid-state crystalline powder with CIE co-ordinates (0.157, 0.027), when excited at 373 nm. Cl-CN-DPQ shows remarkable Stokes shift in the range 14800-5100 cm -1 , which is the characteristic feature of intense light emission. A narrow full width at half-maximum (FWHM) value of PL spectra in the range 42-48 nm was observed. Oscillator strength, energy band gap, quantum yield, and fluorescence energy yield were also examined using UV-vis absorption and photoluminescence spectra. These results prove its applications towards developing organic luminescence devices and displays, organic phosphor-based solar cells and displays, organic lasers, chemical sensors and many more. Copyright © 2017 John Wiley & Sons, Ltd.

GaN@ZIF-8: selective formation of gallium nitride quantum dots inside a zinc methylimidazolate framework.

PubMed

Esken, Daniel; Turner, Stuart; Wiktor, Christian; Kalidindi, Suresh Babu; Van Tendeloo, Gustaaf; Fischer, Roland A

2011-10-19

The microporous zeolitic imidazolate framework [Zn(MeIM)(2); ZIF-8; MeIM = imidazolate-2-methyl] was quantitatively loaded with trimethylamine gallane [(CH(3))(3)NGaH(3)]. The obtained inclusion compound [(CH(3))(3)NGaH(3)]@ZIF-8 reveals three precursor molecules per host cavity. Treatment with ammonia selectively yields the caged cyclotrigallazane intermediate (H(2)GaNH(2))(3)@ZIF-8, and further annealing gives GaN@ZIF-8. This new composite material was characterized with FT-IR spectroscopy, solid-state NMR spectroscopy, powder X-ray diffraction, elemental analysis, (scanning) transmission electron microscopy combined with electron energy-loss spectroscopy, photoluminescence (PL) spectroscopy, and N(2) sorption measurements. The data give evidence for the presence of GaN nanoparticles (1-3 nm) embedded in the cavities of ZIF-8, including a blue-shift of the PL emission band caused by the quantum size effect.

Highly Efficient Thermally Activated Delayed Fluorescence from an Excited-State Intramolecular Proton Transfer System

PubMed Central

2017-01-01

Thermally activated delayed fluorescence (TADF) materials have shown great potential for highly efficient organic light-emitting diodes (OLEDs). While the current molecular design of TADF materials primarily focuses on combining donor and acceptor units, we present a novel system based on the use of excited-state intramolecular proton transfer (ESIPT) to achieve efficient TADF without relying on the well-established donor–acceptor scheme. In an appropriately designed acridone-based compound with intramolecular hydrogen bonding, ESIPT leads to separation of the highest occupied and lowest unoccupied molecular orbitals, resulting in TADF emission with a photoluminescence quantum yield of nearly 60%. High external electroluminescence quantum efficiencies of up to 14% in OLEDs using this emitter prove that efficient triplet harvesting is possible with ESIPT-based TADF materials. This work will expand and accelerate the development of a wide variety of TADF materials for high performance OLEDs. PMID:28776019

Understanding photoluminescence of metal nanostructures based on an oscillator model.

PubMed

Cheng, Yuqing; Zhang, Weidong; Zhao, Jingyi; Wen, Te; Hu, Aiqin; Gong, Qihuang; Lu, Guowei

2018-08-03

Scattering and absorption properties of metal nanostructures have been well understood based on the classic oscillator theory. Here, we demonstrate that photoluminescence of metal nanostructures can also be explained based on a classic model. The model shows that inelastic radiation of an oscillator resembles its resonance band after external excitation, and is related to the photoluminescence from metallic nanostructures. The understanding based on the classic oscillator model is in agreement with that predicted by a quantum electromagnetic cavity model. Moreover, by correlating a two-temperature model and the electron distributions, we demonstrate that both one-photon and two-photon luminescence of the metal nanostructures undergo the same mechanism. Furthermore, the model explains most of the emission characteristics of the metallic nanostructures, such as quantum yield, spectral shape, excitation polarization and power dependence. The model based on an oscillator provides an intuitive description of the photoluminescence process and may enable rapid optimization and exploration of the plasmonic properties.

Improved scintillation detector performance via a method of enhanced layered coatings

DOE PAGES

Wakeford, Daniel Tyler; Tornga, Shawn Robert; Adams, Jillian Cathleen; ...

2016-11-16

Increasing demand for better detection performance with a simultaneous reduction in size, weight and power consumption has motivated the use of compact semiconductors as photo-converters for many gamma-ray and neutron scintillators. The spectral response of devices such as silicon avalanche photodiodes (APDs) is poorly matched to many common high-performance scintillators. We have developed a generalized analytical method that utilizes an optical reference database to match scintillator luminescence to the excitation spectrum of high quantum efficiency semiconductor detectors. This is accomplished by the fabrication and application of a series of high quantum yield, short fluorescence lifetime, wavelengthshifting coatings. Furthermore, we showmore » here a 22% increase in photoelectron collection and a 10% improvement in energy resolution when applying a layered coating to an APD-coupled, cerium-doped, yttrium oxyorthosilicate (YSO:Ce) scintillator. Wavelength-shifted radioluminescence emission and rise time analysis are also discussed.« less

Scalable fabrication of coupled NV center - photonic crystal cavity systems by self-aligned N ion implantation

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

Schröder, T.; Walsh, M.; Zheng, J.

2017-04-06

Towards building large-scale integrated photonic systems for quantum information processing, spatial and spectral alignment of single quantum systems to photonic nanocavities is required. In this paper, we demonstrate spatially targeted implantation of nitrogen vacancy (NV) centers into the mode maximum of 2-d diamond photonic crystal cavities with quality factors up to 8000, achieving an average of 1.1 ± 0.2 NVs per cavity. Nearly all NV-cavity systems have significant emission intensity enhancement, reaching a cavity-fed spectrally selective intensity enhancement, F int, of up to 93. Although spatial NV-cavity overlap is nearly guaranteed within about 40 nm, spectral tuning of the NV’smore » zero-phonon-line (ZPL) is still necessary after fabrication. To demonstrate spectral control, we temperature tune a cavity into an NV ZPL, yielding F ZPL int~5 at cryogenic temperatures.« less

Signatures of single-photon interaction between two quantum dots located in different cavities of a weakly coupled double microdisk structure

NASA Astrophysics Data System (ADS)

Seyfferle, S.; Hargart, F.; Jetter, M.; Hu, E.; Michler, P.

2018-01-01

We report on the radiative interaction of two single quantum dots (QDs) each in a separate InP/GaInP-based microdisk cavity via resonant whispering gallery modes. The investigations are based on as-fabricated coupled disk modes. We apply optical spectroscopy involving a 4 f setup, as well as mode-selective real-space imaging and photoluminescence mapping to discern single QDs coupled to a resonant microdisk mode. Excitation of one disk of the double cavity structure and detecting photoluminescence from the other yields proof of single-photon emission of a QD excited by incoherent energy transfer from one disk to the other via a mode in the weak-coupling regime. Finally, we present evidence of photons emitted by a QD in one disk that are transferred to the other disk by a resonant mode and are subsequently resonantly scattered by another QD.

Photosynthesis in chlorolichens: the influence of the habitat light regime.

PubMed

Piccotto, Massimo; Tretiach, Mauro

2010-11-01

The hypothesis that CO(2) gas exchange and chlorophyll a fluorescence (ChlaF) of lichens vary according to the light regimes of their original habitat, as observed in vascular plants, was tested by analysing the photosynthetic performance of 12 populations of seven dorsoventral, foliose lichens collected from open, south-exposed rocks to densely shaded forests. Light response curves were induced at optimum thallus water content and ChlaF emission curves at the species-specific photon flux at which the quantum yield of CO(2) assimilation is the highest and is saturating the photosynthetic process. Photosynthetic pigments were quantified in crude extracts. The results confirm that the maximum rate of gross photosynthesis is correlated with the chlorophyll content of lichens, which is influenced by light as well as by nitrogen availability. Like leaves, shade tolerant lichens emit more ChlaF than sun-loving ones, whereas the photosynthetic quantum conversion is higher in the latter.

Enhancement of emission efficiency of colloidal CdSe quantum dots on silicon substrate via an ultra-thin layer of aluminum oxide.

PubMed

Patty, K; Sadeghi, S M; Nejat, A; Mao, C-B

2014-04-18

We demonstrate that an ultra-thin layer of aluminum oxide can significantly enhance the emission efficiency of colloidal quantum dots on a Si substrate. For an ensemble of single quantum dots, our results show that this super brightening process can increase the fluorescence of CdSe quantum dots, forming well-resolved spectra, while in the absence of this layer the emission remains mostly at the noise level. We demonstrate that this process can be further enhanced with irradiation of the quantum dots, suggesting a significant photo-induced fluorescence enhancement via considerable suppression of non-radiative decay channels of the quantum dots. We study the impact of the Al oxide thickness on Si and interdot interactions, and discuss the results in terms of photo-induced catalytic properties of the Al oxide and the effects of such an oxide on the Coulomb blockade responsible for suppression of photo-ionization of the quantum dots.

Effects of multiple organic ligands on size uniformity and optical properties of ZnSe quantum dots

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

Archana, J., E-mail: archana.jayaram@yahoo.com; Navaneethan, M.; Hayakawa, Y.

2012-08-15

Highlights: ► Highly monodispersed ZnSe quantum dots have been synthesized by wet chemical route. ► Strong quantum confinement effect have been observed in ∼ 4 nm ZnSe quantum dots. ► Enhanced ultraviolet near band emission have been obtained using long chain polymer. -- Abstract: The effects of multi-ligands on the formation and optical transitions of ZnSe quantum dots have been investigated. The dots are synthesized using 3-mercapto-1,2-propanediol and polyvinylpyrrolidone ligands, and have been characterized by X-ray diffraction, transmission electron microscopy (TEM), UV–visible absorption spectroscopy, photoluminescence spectroscopy, and Fourier transform infrared spectroscopy. TEM reveals high monodispersion with an average size ofmore » 4 nm. Polymer-stabilized, organic ligand-passivated ZnSe quantum dots exhibit strong UV emission at 326 nm and strong quantum confinement in the UV–visible absorption spectrum. Uniform size and suppressed surface trap emission are observed when the polymer ligand is used. The possible growth mechanism is discussed.« less

Quantum optical effective-medium theory and transformation quantum optics for metamaterials

NASA Astrophysics Data System (ADS)

Wubs, Martijn; Amooghorban, Ehsan; Zhang, Jingjing; Mortensen, N. Asger

2016-09-01

While typically designed to manipulate classical light, metamaterials have many potential applications for quantum optics as well. We argue why a quantum optical effective-medium theory is needed. We present such a theory for layered metamaterials that is valid for light propagation in all spatial directions, thereby generalizing earlier work for one-dimensional propagation. In contrast to classical effective-medium theory there is an additional effective parameter that describes quantum noise. Our results for metamaterials are based on a rather general Lagrangian theory for the quantum electrodynamics of media with both loss and gain. In the second part of this paper, we present a new application of transformation optics whereby local spontaneous-emission rates of quantum emitters can be designed. This follows from an analysis how electromagnetic Green functions trans- form under coordinate transformations. Spontaneous-emission rates can be either enhanced or suppressed using invisibility cloaks or gradient index lenses. Furthermore, the anisotropic material profile of the cloak enables the directional control of spontaneous emission.

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.

Time-resolved photoluminescence measurements of InP/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Thi Thuy, Pham; Thi Dieu Thuy, Ung; Chi, Tran Thi Kim; Phuong, Le Quang; Liem, Nguyen Quang; Li, Liang; Reiss, Peter

2009-09-01

This paper reports the results on the time-resolved photoluminescence study of InP/ZnS core/shell quantum dots. The ZnS shell played a decisive role to passivate imperfections on the surface of InP quantum dots, consequently giving rise to a strong enhancement of the photoluminescence from the InP core. Under appropriate excitation conditions, not only the emission from the InP core but also that from the ZnS shell was observed. The emission peak in InP core quantum dots varied as a function of quantum dots size, ranging in the 600 - 700 nm region; while the ZnS shell showed emission in the blue region around 470 nm, which is interpreted as resulting from defects in ZnS.

Single photon emission from charged excitons in CdTe/ZnTe quantum dots

NASA Astrophysics Data System (ADS)

Belyaev, K. G.; Rakhlin, M. V.; Sorokin, S. V.; Klimko, G. V.; Gronin, S. V.; Sedova, I. V.; Mukhin, I. S.; Ivanov, S. V.; Toropov, A. A.

2017-11-01

We report on micro-photoluminescence studies of individual self-organized CdTe/ZnTe quantum dots intended for single-photon-source applications in a visible spectral range. The quantum dots surface density below 1010 per cm2 was achieved by using a thermally activated regime of molecular beam epitaxy that allowed fabrication of etched mesa-structures containing only a few emitting quantum dots. The single photon emission with the autocorrelation function g(2)(0)<0.2 was detected and identified as recombination of charged excitons in the individual quantum dot.

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.

Aqueous synthesis of Ag and Mn co-doped In2S3/ZnS quantum dots with tunable emission for dual-modal targeted imaging.

PubMed

Lai, Pei-Yu; Huang, Chih-Ching; Chou, Tzung-Han; Ou, Keng-Liang; Chang, Jia-Yaw

2017-03-01

Here, we present the microwave-assisted synthesis of In 2 S 3 /ZnS core/shell quantum dots (QDs) co-doped with Ag + and Mn 2+ (referred to as AgMn:In 2 S 3 /ZnS). Ag + altered the optical properties of the host QDs, whereas the spin magnetic moment (S=5/2) of Mn 2+ efficiently induced the longitudinal relaxation of water protons. To the best of our knowledge, this is the first report of the aqueous synthesis of color-tunable AgMn:In 2 S 3 /ZnS core/shell QDs with magnetic properties. The synthetic procedure is rapid, facile, reproducible, and scalable. The obtained QDs offered a satisfactory quantum yield (45%), high longitudinal relaxivity (6.84s -1 mM -1 ), and robust photostability. In addition, they exhibited excellent stability over a wide pH range (5-12) and high ionic strength (0.15-2.0M NaCl). As seen by confocal microscopy and magnetic resonance imaging, AgMn:In 2 S 3 /ZnS conjugated to hyaluronic acid (referred to as AgMn:In 2 S 3 /ZnS@HA) efficiently and specifically targeted cluster determinant 44, a receptor overexpressed on cancer cells. Moreover, AgMn:In 2 S 3 /ZnS@HA showed negligible cytotoxicity in vitro and in vivo, rendering it a promising diagnostic probe for dual-modal imaging in clinical applications. In this manuscript, we reported a facial and rapid method to prepare In 2 S 3 /ZnS core/shell quantum dots (QDs) co-doped with Ag + and Mn 2+ (referred to as AgMn:In 2 S 3 /ZnS). Ag + dopants were used to alter the optical properties of the In 2 S 3 host, whereas Mn 2+ co-dopants with their unpaired electrons provided paramagnetic properties. The emission wavelength of the core/shell QDs could be tuned from 550 to 743nm with a maximum PL quantum yield of 45%. The resulting core/shell QDs also maintained a stable emission in aqueous solution at broad ranges of pH (5-12) and ionic strength (0.15-2.0M NaCl), as well as a high photostability under continuous irradiation. In vivo cytotoxicity experiments showed that up to 500μg/mL AgMn:In 2 S 3 /ZnS@HA did not cause obvious toxicity to zebrafish embryos. In vitro targeted cell luminescence and magnetic resonance imaging showed that AgMn:In 2 S 3 /ZnS conjugated to hyaluronic acid was selectively and efficiently internalized in CD44-expressing tumor cells, confirming that the resultant QDs could function as dual-modal imaging probes for accurate diagnosis. Copyright © 2016 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

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

Excited-state proton transfer dynamics of firefly's chromophore D-luciferin in DMSO-water binary mixture.

PubMed

Kuchlyan, Jagannath; Banik, Debasis; Roy, Arpita; Kundu, Niloy; Sarkar, Nilmoni

2014-12-04

In this article we have investigated intermolecular excited-state proton transfer (ESPT) of firefly's chromophore D-luciferin in DMSO-water binary mixtures using steady-state and time-resolved fluorescence spectroscopy. The unusual behavior of DMSO-water binary mixture as reported by Bagchi et al. (J. Phys. Chem. B 2010, 114, 12875-12882) was also found using D-luciferin as intermolecular ESPT probe. The binary mixture has given evidence of its anomalous nature at low mole fractions of DMSO (below XD = 0.4) in our systematic investigation. Upon excitation of neutral D-luciferin molecule, dual fluorescence emissions (protonated and deprotonated form) are observed in DMSO-water binary mixture. A clear isoemissive point in the time-resolved area normalized emission spectra further indicates two emissive species in the excited state of D-luciferin in DMSO-water binary mixture. DMSO-water binary mixtures of different compositions are fascinating hydrogen bonding systems. Therefore, we have observed unusual changes in the fluorescence emission intensity, fluorescence quantum yield, and fluorescence lifetime of more hydrogen bonding sensitive anionic form of D-luciferin in low DMSO content of DMSO-water binary mixture.

Fluorescent and cathodoluminescent phophors structurally related to sodalite

DOEpatents

Phillips, Mark L. F.; Shea, Lauren E.

1998-01-01

Blue, quantum-confined phosphors for field-emission displays made by reducing metal (M) sulfoaluminates at high temperature. This yields phases of the type M.sub.4 (AlO.sub.2).sub.6 S. Bulk sulfide contaminant mixed with the reduced sulfoaluminate phase is removed by treating it with a chelating agent in nonaqueous solution. A photometric cathodoluminescence efficiency of 9 lumen/watt at 1000 V for Sr.sub.3 PbS(AlO.sub.2).sub.6 is observed. Undoped Sr.sub.4 S(AlO).sub.6 displays 5 lumen/watt at 1000 V, with excellent blue chromatic saturation.

Green Synthesis of Bifunctional Fluorescent Carbon Dots from Garlic for Cellular Imaging and Free Radical Scavenging.

PubMed

Zhao, Shaojing; Lan, Minhuan; Zhu, Xiaoyue; Xue, Hongtao; Ng, Tsz-Wai; Meng, Xiangmin; Lee, Chun-Sing; Wang, Pengfei; Zhang, Wenjun

2015-08-12

Nitrogen and sulfur codoped carbon dots (CDs) were prepared from garlic by a hydrothermal method. The as-prepared CDs possess good water dispersibility, strong blue fluorescence emission with a fluorescent quantum yield of 17.5%, and excellent photo and pH stabilities. It is also demonstrated that the fluorescence of CDs are resistant to the interference of metal ions, biomolecules, and high ionic strength environments. Combining with low cytotoxicity properties, CDs could be used as an excellent fluorescent probe for cellular multicolor imaging. Moreover, the CDs were also demonstrated to exhibit favorable radical scavenging activity.

The First Organic-Inorganic Hybrid Luminescent Multiferroic: (Pyrrolidinium)MnBr3.

PubMed

Zhang, Yi; Liao, Wei-Qiang; Fu, Da-Wei; Ye, Heng-Yun; Liu, Cai-Ming; Chen, Zhong-Ning; Xiong, Ren-Gen

2015-07-08

A hybrid organic-inorganic compound, (pyrrolidinium)MnBr3 , distinguished from rare earth (RE)-doped inorganic perovskites, is discovered as a new member of the ferroelectrics family, having excellent luminescent properties and relatively large spontaneous polarization of 6 μC cm(-2) , as well as a weak ferromagnetism at about 2.4 K. With a quantum yield of >28% and emission lifetime >0.1 ms, such multiferroic photoluminescence is a suitable candidate for future applications in luminescence materials, photovoltaics, and magneto-optoelectronic devices. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The alkyl amines effect on the optical properties of inorganic perovskite quantum dot

NASA Astrophysics Data System (ADS)

Yang, Ya-Zhu; Chung, Shu-Ru

2017-08-01

Perovskite quantum dots (P-QDs) is a new kind of optoelectronic materials in recent years. Compared with organic perovskite QDs (MAPbX3), inorganic perovskite QDs (CsPbX3) have a better stability. Inorganic P-QDs can be prepared at low temperature. Those novel QDs can be applied in solar cells, light-emitting diodes (LEDs), display, and biolables. Typical synthesis process to prepare CsPbX3 QDs is used oleic acid (OA) and cesium carbonate (Cs2CO3) to form Cs-oleate complex first. Moreover, the oleylamine (OLA) and octadecene (ODE) are used as capping agents. Cs-oleate complex then reacts with PbX2 to form CsPbX3 QDs (reacts for 5 s). As we know that the CsPbBr3 QDs emits green light, and its emission wavelength can be tuned by adding Cland Iions to replace Brion. However, the reaction rate of CsPbX3 QDs is fast, and it is not easy to control the emission wavelength by particle size. In this study, we use the saturated alkyl amines with difference of carbon chain length such as dodecylamine (DDA), hexadecylamine (HDA), and octadecylamine (ODA) to prepare CsPbBr3 QDs. The result shows that the emission spectra for all samples range from 489 (ODA) to 514 nm (DDA), the full width at half-maximum (FWHM) is between 23 to 28 nm, the surface morphologies of all samples are nearly spherical, and the quantum yields (QYs) are higher up to 130 % (compared with R6G and the excitation wavelength is 450 nm). Based on emission spectra we can find that the emission peaks are fixed even under different excitation wavelength, imply that the particle size distribution of QDs is uniform. Moreover, the emission wavelength blue shifts with increasing carbon chain length of amines. The stability of alkyl amine-capped CsPbBr3 QDs is good, especially for DDA-capped sample. We also find that a small emission peak around 462 nm can be only observed for DDA-capped sample. Furthermore, this small peak also can be observed even prolong the reaction time to 10 min. The emission wavelengths of CsPbBr3 QDs can be controlled by carbon chain length of alkyl amines. The small FWHM and high QYs of CsPbBr3 QDs meaning that it is benefit to enhance the color gamut of display.

Observation of ground-state quantum beats in atomic spontaneous emission.

PubMed

Norris, D G; Orozco, L A; Barberis-Blostein, P; Carmichael, H J

2010-09-17

We report ground-state quantum beats in spontaneous emission from a continuously driven atomic ensemble. Beats are visible only in an intensity autocorrelation and evidence spontaneously generated coherence in radiative decay. Our measurement realizes a quantum eraser where a first photon detection prepares a superposition and a second erases the "which path" information in the intermediate state.

Metal-organic vapor-phase epitaxy-grown ultra-low density InGaAs/GaAs quantum dots exhibiting cascaded single-photon emission at 1.3 μm

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

Paul, Matthias, E-mail: m.paul@ihfg.uni-stuttgart.de; Kettler, Jan; Zeuner, Katharina

By metal-organic vapor-phase epitaxy, we have fabricated InGaAs quantum dots on GaAs substrate with an ultra-low lateral density (<10{sup 7} cm{sup −2}). The photoluminescence emission from the quantum dots is shifted to the telecom O-band at 1.31 μm by an InGaAs strain reducing layer. In time-resolved measurements, we find fast decay times for exciton (∼600 ps) and biexciton (∼300 ps). We demonstrate triggered single-photon emission (g{sup (2)}(0)=0.08) as well as cascaded emission from the biexciton decay. Our results suggest that these quantum dots can compete with their counterparts grown by state-of-the-art molecular beam epitaxy.

Single Benzene Green Fluorophore: Solid-State Emissive, Water-Soluble, and Solvent- and pH-Independent Fluorescence with Large Stokes Shifts.

PubMed

Beppu, Teruo; Tomiguchi, Kosuke; Masuhara, Akito; Pu, Yong-Jin; Katagiri, Hiroshi

2015-06-15

Benzene is the simplest aromatic hydrocarbon with a six-membered ring. It is one of the most basic structural units for the construction of π conjugated systems, which are widely used as fluorescent dyes and other luminescent materials for imaging applications and displays because of their enhanced spectroscopic signal. Presented herein is 2,5-bis(methylsulfonyl)-1,4-diaminobenzene as a novel architecture for green fluorophores, established based on an effective push-pull system supported by intramolecular hydrogen bonding. This compound demonstrates high fluorescence emission and photostability and is solid-state emissive, water-soluble, and solvent- and pH-independent with quantum yields of Φ=0.67 and Stokes shift of 140 nm (in water). This architecture is a significant departure from conventional extended π-conjugated systems based on a flat and rigid molecular design and provides a minimum requirement for green fluorophores comprising a single benzene ring. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nanoscale Imaging of Light-Matter Coupling Inside Metal-Coated Cavities with a Pulsed Electron Beam.

PubMed

Moerland, Robert J; Weppelman, I Gerward C; Scotuzzi, Marijke; Hoogenboom, Jacob P

2018-05-02

Many applications in (quantum) nanophotonics rely on controlling light-matter interaction through strong, nanoscale modification of the local density of states (LDOS). All-optical techniques probing emission dynamics in active media are commonly used to measure the LDOS and benchmark experimental performance against theoretical predictions. However, metal coatings needed to obtain strong LDOS modifications in, for instance, nanocavities, are incompatible with all-optical characterization. So far, no reliable method exists to validate theoretical predictions. Here, we use subnanosecond pulses of focused electrons to penetrate the metal and excite a buried active medium at precisely defined locations inside subwavelength resonant nanocavities. We reveal the spatial layout of the spontaneous-emission decay dynamics inside the cavities with deep-subwavelength detail, directly mapping the LDOS. We show that emission enhancement converts to inhibition despite an increased number of modes, emphasizing the critical role of optimal emitter location. Our approach yields fundamental insight in dynamics at deep-subwavelength scales for a wide range of nano-optical systems.

Prominence of fusion temperature and engineering heteroatoms on multifarious emissive shifts in carbon dots.

PubMed

Velusamy, Jayaramakrishnan; Ramos-Ortiz, Gabriel; Rodríguez, Mario; Hernández-Cruz, Olivia; Ponce, Arturo

2018-05-16

We present a simple but robust strategy to engineering heteroatoms (N, S) on carbon dots (CDs) surface that results in a collection of enhanced photoluminescence (PL) emissions. The use of citric acid (CA) and 2-Imidazolidinethione (2-IZT) as precursors was envisioned to study the impact of thermolysis process on the PL properties. The proposed strategy, implemented at two different temperatures (180 °C and 200 °C), is suitable to produce CDs with tunable PL and quantum yield (QY) up to ∼32%. Similar to earlier reports of CA-based CDs, the self-assembling of fluorophores integrated into the CDs edge is hypothesized, however, in our CDs a double intriguing effect of blue- and red-shifting can be observed for PL as the wavelength of excitation is increased in the range 280-480 nm. Through a comprehensive characterization and evaluation of these CDs in water suspensions, the mechanisms that lead to PL multifarious emissions are proposed. Copyright © 2018 Elsevier Inc. All rights reserved.

Photo-dynamics of roseoflavin and riboflavin in aqueous and organic solvents

NASA Astrophysics Data System (ADS)

Zirak, P.; Penzkofer, A.; Mathes, T.; Hegemann, P.

2009-03-01

Roseoflavin (8-dimethylamino-8-demethyl- D-riboflavin) and riboflavin in aqueous and organic solvents are studied by optical absorption spectroscopy, fluorescence spectroscopy, and fluorescence decay kinetics. Solvent polarity dependent absorption shifts are observed. The fluorescence quantum yields are solvent dependent. For roseoflavin the fluorescence decay shows a bi-exponential dependence (ps to sub-ps time constant, and 100 ps to a few ns time constant). The roseoflavin photo-dynamics is explained in terms of fast intra-molecular charge transfer (diabatic electron transfer) from the dimethylamino electron donor group to the pteridin carbonyl electron acceptor followed by intra-molecular charge recombination. The fast fluorescence component is due to direct locally-excited-state emission, and the slow fluorescence component is due to delayed locally-excited-state emission and charge transfer state emission. The fluorescence decay of riboflavin is mono-exponential. The S 1-state potential energy surface is determined by vibronic relaxation and solvation dynamics due to excited-state dipole moment changes (adiabatic optical electron transfer).

Water-Soluble Polymers with Strong Photoluminescence through an Eco-Friendly and Low-Cost Route.

PubMed

Guo, Zhaoyan; Ru, Yue; Song, Wenbo; Liu, Zhenjie; Zhang, Xiaohong; Qiao, Jinliang

2017-07-01

Photoluminescence (PL) of nonconjugated polymers brings a favorable opportunity for low-cost and nontoxic luminescent materials, while most of them still exhibit relatively weak emission. Strong PL from poly[(maleic anhydride)-alt-(vinyl acetate)] (PMV) from low-cost monomer has been found in organic solvents, yet the necessity of noxious solvents would hinder its practical applications. Herein, through a novel, eco-friendly, and one-step route, PMV-derived PL polymers can be fabricated with the highest quantum yield of 87% among water-soluble nonconjugated PL polymers ever reported. These PMV-derived polymers emit strong blue emission in both solutions and solids, and can be transformed into red-emission agents easily. These PL polymers exhibit application potentials in light-conversion agricultural films. It is assumed that this work not only puts forward a convenient preparation routine for nonconjugated polymers with high PL, but also provides an industrial application possibility for them. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Phosphor-Free Apple-White LEDs with Embedded Indium-Rich Nanostructures Grown on Strain Relaxed Nano-epitaxy GaN.

PubMed

Soh, C B; Liu, W; Yong, A M; Chua, S J; Chow, S Y; Tripathy, S; Tan, R J N

2010-08-01

Phosphor-free apple-white light emitting diodes have been fabricated using a dual stacked InGaN/GaN multiple quantum wells comprising of a lower set of long wavelength emitting indium-rich nanostructures incorporated in multiple quantum wells with an upper set of cyan-green emitting multiple quantum wells. The light-emitting diodes were grown on nano-epitaxially lateral overgrown GaN template formed by regrowth of GaN over SiO(2) film patterned with an anodic aluminum oxide mask with holes of 125 nm diameter and a period of 250 nm. The growth of InGaN/GaN multiple quantum wells on these stress relaxed low defect density templates improves the internal quantum efficiency by 15% for the cyan-green multiple quantum wells. Higher emission intensity with redshift in the PL peak emission wavelength is obtained for the indium-rich nanostructures incorporated in multiple quantum wells. The quantum wells grown on the nano-epitaxially lateral overgrown GaN has a weaker piezoelectric field and hence shows a minimal peak shift with application of higher injection current. An enhancement of external quantum efficiency is achieved for the apple-white light emitting diodes grown on the nano-epitaxially lateral overgrown GaN template based on the light -output power measurement. The improvement in light extraction efficiency, η(extraction,) was found to be 34% for the cyan-green emission peak and 15% from the broad long wavelength emission with optimized lattice period.

Phosphor-Free Apple-White LEDs with Embedded Indium-Rich Nanostructures Grown on Strain Relaxed Nano-epitaxy GaN

NASA Astrophysics Data System (ADS)

Soh, C. B.; Liu, W.; Yong, A. M.; Chua, S. J.; Chow, S. Y.; Tripathy, S.; Tan, R. J. N.

2010-11-01

Phosphor-free apple-white light emitting diodes have been fabricated using a dual stacked InGaN/GaN multiple quantum wells comprising of a lower set of long wavelength emitting indium-rich nanostructures incorporated in multiple quantum wells with an upper set of cyan-green emitting multiple quantum wells. The light-emitting diodes were grown on nano-epitaxially lateral overgrown GaN template formed by regrowth of GaN over SiO2 film patterned with an anodic aluminum oxide mask with holes of 125 nm diameter and a period of 250 nm. The growth of InGaN/GaN multiple quantum wells on these stress relaxed low defect density templates improves the internal quantum efficiency by 15% for the cyan-green multiple quantum wells. Higher emission intensity with redshift in the PL peak emission wavelength is obtained for the indium-rich nanostructures incorporated in multiple quantum wells. The quantum wells grown on the nano-epitaxially lateral overgrown GaN has a weaker piezoelectric field and hence shows a minimal peak shift with application of higher injection current. An enhancement of external quantum efficiency is achieved for the apple-white light emitting diodes grown on the nano-epitaxially lateral overgrown GaN template based on the light -output power measurement. The improvement in light extraction efficiency, ηextraction, was found to be 34% for the cyan-green emission peak and 15% from the broad long wavelength emission with optimized lattice period.

Perylenetetracarboxylic anhydride as a precursor of fluorescent carbon nanoonion rings.

PubMed

Baldoví, Herme G; Herance, José Raul; Manuel Víctor, Víctor; Alvaro, Mercedes; Garcia, Hermenegildo

2015-08-07

Thermal annealing at 400 °C of perylenetetracarboxylic anhydride in low molecular mass PEG gives rise to the formation of well defined nanoobjects of 2.5 nm height and size distribution from 10 to 65 nm (average 40 nm) after purification of the raw mixture with silicagel chromatography. TEM reveals that the flat nanoobjects are constituted of concentric graphenic rings (0.34 nm interlayer distance). The morphology of the nanoparticles resembles onion rings of nanometric dimensions (nanoonion rings C-NOR). C-NOR particles have an excitation dependent emission with λem from 430 to 570 nm and a maximum emission quantum yield of 0.49. C-NOR particles can be internalized into Hep3B human hepatoma cells as determined by confocal fluorescence microscopy and are remarkably biocompatible affecting slightly cell viability according to the MTT test.

Fluorescence emission of disperse Red 1 in solution at room temperature.

PubMed

Toro, Carlos; Thibert, Arthur; De Boni, Leonardo; Masunov, Artëm E; Hernández, Florencio E

2008-01-24

In this article, we report the fluorescence emission of Disperse Red 1 in solution at room temperature and pumping at 532 nm with a 25 mW diode laser. We have measured its fluorescence quantum yield in methanol, ethylene glycol, glycerol, and phenol obtaining values as high as 10(-3) in the aliphatic alcohols. The excitation spectra of Disperse Red 1 in all four solvents as well as its excitation anisotropy in glycerol are presented. Applying a Gaussian decomposition method to the absorption spectra along with the support from the excitation spectra, the positions of the different transitions in this pseudo-stilbene azobenzene dye were determined. Solvatochromic and isomerization constraint effects are discussed. Calculations using density functional theory at TD-B3LYP/6-31G*//HF/6-31G* level were performed to interpret the experimental observations.

Aggregation-Induced Emission (AIE) Fluorophore Exhibits a Highly Ratiometric Fluorescent Response to Zn2+ in vitro and in Human Liver Cancer Cells.

PubMed

Mehdi, Hassan; Gong, Weitao; Guo, Huimin; Watkinson, Michael; Ma, Hua; Wajahat, Ali; Ning, Guiling

2017-09-21

Two novel organic fluorophores, containing bis-naphthylamide and quinoline motifs, have been designed and synthesized. One of the fluorophores contains an isobutylene unit and exhibits a significant aggregation-induced emission (AIE) and a remarkable highly selective ratiometric fluorescence response towards Zn 2+ in solution as well as in human liver cancer cells. The AIE behavior of this fluorophore was fully verified by fluorescence and UV/Vis spectroscopy, quantum yield calculations, and single-crystal X-ray diffraction, which revealed an intricate crystal packing system. Conversely, a fluorophore that lacks the isobutylene moiety did not exhibit any significant fluorescent properties as a result of its more flexible molecular structure that presumably allows free intramolecular rotational processes to occur. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Radiative-emission analysis in charge-exchange collisions of O6 + with argon, water, and methane

NASA Astrophysics Data System (ADS)

Leung, Anthony C. K.; Kirchner, Tom

2017-04-01

Processes of electron capture followed by Auger and radiative decay were investigated in slow ion-atom and -molecule collisions. A quantum-mechanical analysis which utilizes the basis generator method within an independent electron model was carried out for collisions of O 6 + with Ar, H2O , and CH4 at impact energies of 1.17 and 2.33 keV/amu. At these impact energies, a closure approximation in the spectral representation of the Hamiltonian for molecules was found to be necessary to yield reliable results. Total single-, double-, and triple-electron-capture cross sections obtained show good agreement with previous measurements and calculations using the classical trajectory Monte Carlo method. The corresponding emission spectra from single capture for each collision system are in satisfactory agreement with previous calculations.

Al x Ga1‑ x N-based semipolar deep ultraviolet light-emitting diodes

NASA Astrophysics Data System (ADS)

Akaike, Ryota; Ichikawa, Shuhei; Funato, Mitsuru; Kawakami, Yoichi

2018-06-01

Deep ultraviolet (UV) emission from Al x Ga1‑ x N-based light-emitting diodes (LEDs) fabricated on semipolar (1\\bar{1}02) (r-plane) AlN substrates is presented. The growth conditions are optimized. A high NH3 flow rate during metalorganic vapor phase epitaxy yields atomically flat Al y Ga1‑ y N (y > x) on which Al x Ga1‑ x N/Al y Ga1‑ y N multiple quantum wells with abrupt interfaces and good periodicity are fabricated. The fabricated r-Al x Ga1‑ x N-based LED emits at 270 nm, which is in the germicidal wavelength range. Additionally, the emission line width is narrow, and the peak wavelength is stable against the injection current, so the semipolar LED shows promise as a UV emitter.

Protonation-induced ultrafast torsional dynamics in 9-anthrylbenzimidazole: a pH activated molecular rotor.

PubMed

Nandi, Amitabha; Kushwaha, Archana; Das, Dipanwita; Ghosh, Rajib

2018-03-07

We report the photophysical properties and excited state dynamics of 9-anthrylbenzimidazole (ANBI) which exhibits protonation-induced molecular rotor properties. In contrast to the highly emissive behavior of neutral ANBI, protonation of the benzimidazole group of ANBI induces efficient nonradiative deactivation by ultrafast torsional motion around the bond connecting the anthracene and benzimidazole units, as revealed by ultrafast transient absorption and fluorescence spectroscopy. Contrary to viscosity-independent fluorescence of neutral dyes, protonated ANBI is shown to display linear variation of emission yield and lifetime with solvent viscosity. The protonation-induced molecular rotor properties in the studied system are shown to be driven by enhanced charge transfer and are corroborated by quantum chemical calculations. Potential application as a microviscosity sensor of acidic regions in a heterogeneous environment by these proton-activated molecular rotor properties of ANBI is discussed.

The Preparation Conditions of Chromium Doped ZnSe and Their Effect on the Infrared Luminescence Properties

NASA Technical Reports Server (NTRS)

Burger, A.; Chattopadhyay, K.; Ndap, J.-O.; Ma, X.; Morgan, S. H.; Rablau, C. I.; Su, C. H.; Feth, S.

2000-01-01

We report the investigation by photoluminescence lifetime measurements of the near-IR emissions from a series of chromium-doped ZnSe samples, correlated to their preparation conditions. The samples were polycrystalline or single crystals prepared by post growth diffusion doping or single crystals doped during growth by the physical vapor transport method. Room temperature lifetime values between 6 and 8 micro seconds were measured for samples with Cr2+ from low 10(exp 17) to high 10(exp 18) / cubic cm range. Lifetime data taken down to 78 K was found to be rather temperature independent, reconfirming previous reports indicating a quantum yield of the corresponding emission of close to 100% at room temperature. A strong decrease in the room temperature lifetime was found for chromium concentrations higher than 10(exp 19) / cubic CM.

Carbene based photochemical molecular assemblies for solar driven hydrogen generation.

PubMed

Peuntinger, Katrin; Pilz, T David; Staehle, Robert; Schaub, Markus; Kaufhold, Simon; Petermann, Lydia; Wunderlin, Markus; Görls, Helmar; Heinemann, Frank W; Li, Jing; Drewello, Thomas; Vos, Johannes G; Guldi, Dirk M; Rau, Sven

2014-09-28

Novel photocatalysts based on ruthenium complexes with NHC (N-heterocyclic carbene)-type bridging ligands have been prepared and structurally and photophysically characterised. The identity of the NHC-unit of the bridging ligand was established unambiguously by means of X-ray structural analysis of a heterodinuclear ruthenium-silver complex. The photophysical data indicate ultrafast intersystem crossing into an emissive and a non-emissive triplet excited state after excitation of the ruthenium centre. Exceptionally high luminescence quantum yields of up to 39% and long lifetimes of up to 2 μs are some of the triplet excited state characteristics. Preliminary studies into the visible light driven photocatalytic hydrogen formation show no induction phase and constant turnover frequencies that are independent on the concentration of the photocatalyst. In conclusion this supports the notion of a stable assembly under photocatalytic conditions.

Emission behaviors of unsymmetrical 1,3-diaryl-β-diketones: A model perfectly disclosing the effect of molecular conformation on luminescence of organic solids

NASA Astrophysics Data System (ADS)

Cheng, Xiao; Li, Feng; Han, Shenghua; Zhang, Yufei; Jiao, Chuanjun; Wei, Jinbei; Ye, Kaiqi; Wang, Yue; Zhang, Hongyu

2015-03-01

A series of unsymmetrical 1,3-diaryl-β-diketones 1-6 displaying molecular conformation-dependent fluorescence quantum yields have been synthesized. Crystals with planar molecular conformation such as 1, 2, 3 and 4 are highly fluorescent (φf: 39-53%), and the one holding slightly twisted conformation (5) is moderately luminescent (φf = 17%), while crystal 6 possessing heavily bent structure is completely nonluminous (φf ~ 0). The distinct fluorescence efficiencies are ascribed to their different molecular conformations, since all the crystals hold the same crystal system, space group and crystal packing structures. Additionally, the fluorescent crystals 1-5 display low threshold amplified spontaneous emission (ASE) with small full widths at half-maximum (FWHM: 3-7 nm), indicating their potential as candidates for organic crystal lasing devices.

Spectroscopy of Single AlInAs Quantum Dots

NASA Astrophysics Data System (ADS)

Derebezov, I. A.; Gaisler, A. V.; Gaisler, V. A.; Dmitriev, D. V.; Toropov, A. I.; Kozhukhov, A. S.; Shcheglov, D. V.; Latyshev, A. V.; Aseev, A. L.

2018-03-01

A system of quantum dots based on Al x In1- x As/Al y Ga1- y As solid solutions is investigated. The use of Al x In1- x As wide-gap solid solutions as the basis of quantum dots substantially extends the spectral emission range to the short-wavelength region, including the wavelength region near 770 nm, which is of interest for the development of aerospace systems of quantum cryptography. The optical characteristics of Al x In1- x As single quantum dots grown by the Stranski-Krastanov mechanism were studied by cryogenic microphotoluminescence. The statistics of the emission of single quantum dot excitons was studied using a Hanbury Brown-Twiss interferometer. The pair photon correlation function indicates the sub-Poissonian nature of the emission statistics, which directly confirms the possibility of developing single-photon emitters based on Al x In1- x As quantum dots. The fine structure of quantum dot exciton states was investigated at wavelengths near 770 nm. The splitting of the exciton states is found to be similar to the natural width of exciton lines, which is of great interest for the development of entangled photon pair emitters based on Al x In1- x As quantum dots.

A stable wavelength-tunable triggered source of single photons and cascaded photon pairs at the telecom C-band

NASA Astrophysics Data System (ADS)

Zeuner, Katharina D.; Paul, Matthias; Lettner, Thomas; Reuterskiöld Hedlund, Carl; Schweickert, Lucas; Steinhauer, Stephan; Yang, Lily; Zichi, Julien; Hammar, Mattias; Jöns, Klaus D.; Zwiller, Val

2018-04-01

The implementation of fiber-based long-range quantum communication requires tunable sources of single photons at the telecom C-band. Stable and easy-to-implement wavelength-tunability of individual sources is crucial to (i) bring remote sources into resonance, (ii) define a wavelength standard, and (iii) ensure scalability to operate a quantum repeater. So far, the most promising sources for true, telecom single photons are semiconductor quantum dots, due to their ability to deterministically and reliably emit single and entangled photons. However, the required wavelength-tunability is hard to attain. Here, we show a stable wavelength-tunable quantum light source by integrating strain-released InAs quantum dots on piezoelectric substrates. We present triggered single-photon emission at 1.55 μm with a multi-photon emission probability as low as 0.097, as well as photon pair emission from the radiative biexciton-exciton cascade. We achieve a tuning range of 0.25 nm which will allow us to spectrally overlap remote quantum dots or tuning distant quantum dots into resonance with quantum memories. This opens up realistic avenues for the implementation of photonic quantum information processing applications at telecom wavelengths.

Crystal Phase Quantum Well Emission with Digital Control.

PubMed

Assali, S; Lähnemann, J; Vu, T T T; Jöns, K D; Gagliano, L; Verheijen, M A; Akopian, N; Bakkers, E P A M; Haverkort, J E M

2017-10-11

One of the major challenges in the growth of quantum well and quantum dot heterostructures is the realization of atomically sharp interfaces. Nanowires provide a new opportunity to engineer the band structure as they facilitate the controlled switching of the crystal structure between the zinc-blende (ZB) and wurtzite (WZ) phases. Such a crystal phase switching results in the formation of crystal phase quantum wells (CPQWs) and quantum dots (CPQDs). For GaP CPQWs, the inherent electric fields due to the discontinuity of the spontaneous polarization at the WZ/ZB junctions lead to the confinement of both types of charge carriers at the opposite interfaces of the WZ/ZB/WZ structure. This confinement leads to a novel type of transition across a ZB flat plate barrier. Here, we show digital tuning of the visible emission of WZ/ZB/WZ CPQWs in a GaP nanowire by changing the thickness of the ZB barrier. The energy spacing between the sharp emission lines is uniform and is defined by the addition of single ZB monolayers. The controlled growth of identical quantum wells with atomically flat interfaces at predefined positions featuring digitally tunable discrete emission energies may provide a new route to further advance entangled photons in solid state quantum systems.

Pulsed Rabi oscillations in quantum two-level systems: beyond the area theorem

NASA Astrophysics Data System (ADS)

Fischer, Kevin A.; Hanschke, Lukas; Kremser, Malte; Finley, Jonathan J.; Müller, Kai; Vučković, Jelena

2018-01-01

The area theorem states that when a short optical pulse drives a quantum two-level system, it undergoes Rabi oscillations in the probability of scattering a single photon. In this work, we investigate the breakdown of the area theorem as both the pulse length becomes non-negligible and for certain pulse areas. Using simple quantum trajectories, we provide an analytic approximation to the photon emission dynamics of a two-level system. Our model provides an intuitive way to understand re-excitation, which elucidates the mechanism behind the two-photon emission events that can spoil single-photon emission. We experimentally measure the emission statistics from a semiconductor quantum dot, acting as a two-level system, and show good agreement with our simple model for short pulses. Additionally, the model clearly explains our recent results (Fischer and Hanschke 2017 et al Nat. Phys.) showing dominant two-photon emission from a two-level system for pulses with interaction areas equal to an even multiple of π.

Pincer-CNC mononuclear, dinuclear and heterodinuclear Au(III) and Pt(II) complexes supported by mono- and poly-N-heterocyclic carbenes: synthesis and photophysical properties.

PubMed

Gonell, S; Poyatos, M; Peris, E

2016-04-07

A family of cyclometallated Au(iii) and Pt(ii) complexes containing a CNC-pincer ligand (CNC = 2,6-diphenylpyridine) supported by pyrene-based mono- or bis-NHC ligands have been synthesized and characterized, together with the preparation of a Pt-Au hetero-dimetallic complex based on a Y-shaped tris-NHC ligand. The photophysical properties of all the new species and of two related Ru(ii)-arene complexes were studied and compared. Whereas the pyrene-based complexes only exhibit emission in solution, those containing the Y-shaped tris-NHC ligand are only luminescent when dispersed in poly(methyl methacrylate) (PMMA). In particular, the pyrene-based complexes were found to be emissive in the range of 373-440 nm, with quantum yields ranging from 3.1 to 6.3%, and their emission spectra were found to be almost superimposable, pointing to the fluorescent pyrene-centered nature of the emission. This observation suggests that the emission properties of the pyrene fragment may be combined with some of the numerous applications of NHCs as supporting ligands allowing, for instance, the design of biological luminescent agents.

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.

Boron carbon nitride nanostructures from salt melts: tunable water-soluble phosphors.

PubMed

Lei, Weiwei; Portehault, David; Dimova, Rumiana; Antonietti, Markus

2011-05-11

A simple, high yield, chemical process is developed to fabricate layered h-BN nanosheets and BCNO nanoparticles with a diameter of ca. 5 nm at 700 °C. The use of the eutectic LiCl/KCl salt melt medium enhances the kinetics of the reaction between sodium borohydride and urea or guanidine as well as the dispersion of the nanoparticles in water. The carbon content can be tuned from 0 to 50 mol % by adjusting the reactant ratio, thus providing precise control of the light emission of the particles in the range 440-528 nm while reaching a quantum yield of 26%. Because of their green synthesis, low toxicity, small size, and stability against aggregation in water, the as-obtained photoluminescent BCNO nanoparticles show promise for diagnostics and optoelectronics. © 2011 American Chemical Society

Ti-Catalyzed Hydroamination for the Synthesis of Amine-Containing π-Conjugated Materials.

PubMed

Hao, Han; Thompson, Kyle A; Hudson, Zachary M; Schafer, Laurel L

2018-04-11

A series of conjugated enamines were prepared by Ti catalyzed anti-Markovnikov hydroamination. The synthetic route is efficient with yields of up to 94 % and the 100 % atom efficiency of the reaction means that these products are easily isolated and purified. Due to the extended conjugated system, the enamine tautomers were observed exclusively in both solid and solution phases, as determined by X-ray crystallography and NMR spectroscopy. These new conjugated molecules, with N incorporated into the backbone, show interesting photophysical properties including photo-luminescent quantum yields of up to 0.26. Notably, through the incorporation of B to give a donor-acceptor π-conjugated system, a redshift of approximately 100 nm is observed for the emission maximum along with the anticipated solvatochromic shifts. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Masked red-emitting carbopyronine dyes with photosensitive 2-diazo-1-indanone caging group.

PubMed

Kolmakov, Kirill; Wurm, Christian; Sednev, Maksim V; Bossi, Mariano L; Belov, Vladimir N; Hell, Stefan W

2012-03-01

Caged near-IR emitting fluorescent dyes are in high demand in optical microscopy but up to now were unavailable. We discovered that the combination of a carbopyronine dye core and a photosensitive 2-diazo-1-indanone residue leads to masked near-IR emitting fluorescent dyes. Illumination of these caged dyes with either UV or visible light (λ < 420 nm) efficiently generates fluorescent compounds with absorption and emission at 635 nm and 660 nm, respectively. A high-yielding synthetic route with attractive possibilities for further dye design is described in detail. Good photostability, high contrast, and a large fluorescence quantum yield after uncaging are the most important features of the new compounds for non-invasive imaging in high-resolution optical microscopy. For use in immunolabelling the caged dyes were decorated with a (hydrophilic) linker and an (activated) carboxyl group.

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

Photonic engineering of highly linearly polarized quantum dot emission at telecommunication wavelengths

NASA Astrophysics Data System (ADS)

Mrowiński, P.; Emmerling, M.; Schneider, C.; Reithmaier, J. P.; Misiewicz, J.; Höfling, S.; Sek, G.

2018-04-01

In this work, we discuss a method to control the polarization anisotropy of spontaneous emission from neutral excitons confined in quantum-dot-like nanostructures, namely single epitaxial InAs quantum dashes emitting at telecom wavelengths. The nanostructures are embedded inside lithographically defined, in-plane asymmetric photonic mesa structures, which generate polarization-dependent photonic confinement. First, we study the influence of the photonic confinement on the polarization anisotropy of the emission by photoluminescence spectroscopy, and we find evidence of different contributions to a degree of linear polarization (DOLP), i.e., from the quantum dash and the photonic mesa, in total giving rise to DOLP =0.85 . Then, we perform finite-difference time-domain simulations of photonic confinement, and we calculate the DOLP in a dipole approximation showing well-matched results for the established model. Furthermore, by using numerical calculations, we demonstrate several types of photonic confinements where highly linearly polarized emission with DOLP of about 0.9 is possible by controlling the position of a quantum emitter inside the photonic structure. Then, we elaborate on anisotropic quantum emitters allowing for exceeding DOLP =0.95 in an optimized case, and we discuss the ways towards efficient linearly polarized single photon source at telecom bands.

Metal Complexes for Organic Optoelectronic Applications

NASA Astrophysics Data System (ADS)

Huang, Liang

Organic optoelectronic devices have drawn extensive attention by over the past two decades. Two major applications for Organic optoelectronic devices are efficient organic photovoltaic devices(OPV) and organic light emitting diodes (OLED). Organic Solar cell has been proven to be compatible with the low cost, large area bulk processing technology and processed high absorption efficiencies compared to inorganic solar cells. Organic light emitting diodes are a promising approach for display and solid state lighting applications. To improve the efficiency, stability, and materials variety for organic optoelectronic devices, several emissive materials, absorber-type materials, and charge transporting materials were developed and employed in various device settings. Optical, electrical, and photophysical studies of the organic materials and their corresponding devices were thoroughly carried out. In this thesis, Chapter 1 provides an introduction to the background knowledge of OPV and OLED research fields presented. Chapter 2 discusses new porphyrin derivatives- azatetrabenzylporphyrins for OPV and near infrared OLED applications. A modified synthetic method is utilized to increase the reaction yield of the azatetrabenzylporphyrin materials and their photophysical properties, electrochemical properties are studied. OPV devices are also fabricated using Zinc azatetrabenzylporphyrin as donor materials. Pt(II) azatetrabenzylporphyrin were also synthesized and used in near infra-red OLED to achieve an emission over 800 nm with reasonable external quantum efficiencies. Chapter 3, discusses the synthesis, characterization, and device evaluation of a series of tetradentate platinum and palladium complexesfor single doped white OLED applications and RGB white OLED applications. Devices employing some of the developed emitters demonstrated impressively high external quantum efficiencies within the range of 22%-27% for various emitter concentrations. And the palladium complex, i.e. Pd3O3, enables the fabrication of stable devices achieving nearly 1000h. at 1000cd/m2 without any outcoupling enhancement while simultaneously achieving peak external quantum efficiencies of 19.9%. Chapter 4 discusses tetradentate platinum and palladium complexes as deep blue emissive materials for display and lighting applications. The platinum complex PtNON, achieved a peak external quantum efficiency of 24.4 % and CIE coordinates of (0.18, 0.31) in a device structure designed for charge confinement and the palladium complexes Pd2O2 exhibited peak external quantum efficiency of up to 19.2%.

Quantum Dots and Their Multimodal Applications: A Review

PubMed Central

Bera, Debasis; Qian, Lei; Tseng, Teng-Kuan; Holloway, Paul H.

2010-01-01

Semiconducting quantum dots, whose particle sizes are in the nanometer range, have very unusual properties. The quantum dots have band gaps that depend in a complicated fashion upon a number of factors, described in the article. Processing-structure-properties-performance relationships are reviewed for compound semiconducting quantum dots. Various methods for synthesizing these quantum dots are discussed, as well as their resulting properties. Quantum states and confinement of their excitons may shift their optical absorption and emission energies. Such effects are important for tuning their luminescence stimulated by photons (photoluminescence) or electric field (electroluminescence). In this article, decoupling of quantum effects on excitation and emission are described, along with the use of quantum dots as sensitizers in phosphors. In addition, we reviewed the multimodal applications of quantum dots, including in electroluminescence device, solar cell and biological imaging.

On the origin of blue emission from ZnO quantum dots synthesized by a sol-gel route

NASA Astrophysics Data System (ADS)

Han, Li-Li; Cui, Lan; Wang, Wei-Hua; Wang, Jiang-Long; Du, Xi-Wen

2012-06-01

ZnO quantum dots (QDs) with blue emission were synthesized by a sol-gel method. A series of control experiments were conducted to explore the origin of the blue emission. It is found that the blue emission arises from neither the quantum confinement nor intermediate products, and it can be achieved only in the presence of Li+ cations and excessive OH- anions. Moreover, the long decay time of the blue emission suggests a defect-related de-excitation process. On the basis of the experimental and calculation results, possible de-excitation paths for light emission were discussed, and the origin of the blue emission was determined as the electron transition from the conduction band to interstitial oxygen defects. Excessive OH- anions are responsible for the formation of interstitial oxygen defects, and Li+ ions can stabilize the defects by substituting for Zn atoms. Besides, Li+ ions can block the growth of ZnO QDs, broaden their band gap and cause a blue shift of the blue emission.

Targeting N-doped graphene quantum dot with high photothermal conversion efficiency for dual-mode imaging and therapy in vitro.

PubMed

Xuan, Yang; Zhang, Ruo-Yun; Zhang, Xiao-Shuai; An, Jie; Cheng, Kai; Li, Cheng; Hou, Xiao-Lin; Zhao, Yuan-Di

2018-08-31

A graphene quantum dot (GQD) is a novel carbon nanomaterial with the advantages of low cost and no pollution. It has attracted serious attention in the biomedical fields because of its stabilities and tunable fluorescence wavelength. In this manuscript, an N-doped graphene quantum dot (N-GQD) was synthesized by a hydrothermal method using citric acid as the carbon source and urea as the nitrogen source. X-ray diffraction, Raman spectroscopy, transmission electron microscopy, UV-vis absorption spectrum, and fluorescence spectrum were used to characterize the N-GQD. The results showed that the N-GQD had a uniform size of about 5 nm. The two fluorescence emission peaks, one in the visible light region showed a 49.75% quantum yield, while another in the near infrared region was 2.49%. The photothermal conversion efficiency was 62.53%, higher than any kind of carbon nanomaterial in existence today. MTT and a long-term cytotoxicity experiment confirmed that the N-GQD had low cytotoxicity. The probe also had the ability of photoacoustic response at the same time. After coupling with folic acid, it presented imaging and photothermal therapy on the cells, which has great application prospects in the early diagnosis and treatment of tumors.

Highly efficient near-infrared light-emitting diodes by using type-II CdTe/CdSe core/shell quantum dots as a phosphor

NASA Astrophysics Data System (ADS)

Shen, Huaibin; Zheng, Ying; Wang, Hongzhe; Xu, Weiwei; Qian, Lei; Yang, Yixing; Titov, Alexandre; Hyvonen, Jake; Li, Lin Song

2013-11-01

In this paper, we present an innovative method for the synthesis of CdTe/CdSe type-II core/shell structure quantum dots (QDs) using ‘greener’ chemicals. The PL of CdTe/CdSe type-II core/shell structure QDs ranges from 600 to 820 nm, and the as-synthesized core/shell structures show narrow size distributions and stable and high quantum yields (50-75%). Highly efficient near-infrared light-emitting diodes (LEDs) have been demonstrated by employing the CdTe/CdSe type-II core/shell QDs as emitters. The devices fabricated based on these type-II core/shell QDs show color-saturated near-infrared emission from the QD layers, a low turn-on voltage of 1.55 V, an external quantum efficiency (EQE) of 1.59%, and a current density and maximum radiant emittance of 2.1 × 103 mA cm-2 and 17.7 mW cm-2 at 8 V it is the first report to use type-II core/shell QDs as near-infrared emitters and these results may offer a practicable platform for the realization of near-infrared QD-based light-emitting diodes, night-vision-readable displays, and friend/foe identification system.

Full spectral optical modeling of quantum-dot-converted elements for light-emitting diodes considering reabsorption and reemission effect.

PubMed

Li, Jia-Sheng; Tang, Yong; Li, Zong-Tao; Cao, Kai; Yan, Cai-Man; Ding, Xin-Rui

2018-07-20

Quantum dots (QDs) have attracted significant attention in light-emitting diode (LED) illumination and display applications, owing to their high quantum yield and unique spectral properties. However, an effective optical model of quantum-dot-converted elements (QDCEs) for (LEDs) that entirely considers the reabsorption and reemission effect is lacking. This suppresses the design of QDCE structures and further investigation of light-extraction/conversion mechanisms in QDCEs. In this paper, we proposed a full spectral optical modeling method for QDCEs packaged in LEDs, entirely considering the reabsorption and reemission effect, and its results are compared with traditional models without reabsorption or reemission. The comparisons indicate that the QDCE absorption loss of QD emission light is a major factor decreasing the radiant efficacy of LEDs, which should be considered when designing QDCE structures. According to the measurements of fabricated LEDs, only calculation results that entirely consider reabsorption and reemission show good agreement with experimental radiant efficacy, spectra, and peak wavelength at the same down-conversion efficiency. Consequently, it is highly expected that QDCE will be modeled considering the reabsorption and reemission events. This study provides a simple and effective modeling method for QDCEs, which shows great potential for their structure designs and fundamental investigations.

Full spectral optical modeling of quantum-dot-converted elements for light-emitting diodes considering reabsorption and reemission effect

NASA Astrophysics Data System (ADS)

Li, Jia-Sheng; Tang, Yong; Li, Zong-Tao; Cao, Kai; Yan, Cai-Man; Ding, Xin-Rui

2018-07-01

Quantum dots (QDs) have attracted significant attention in light-emitting diode (LED) illumination and display applications, owing to their high quantum yield and unique spectral properties. However, an effective optical model of quantum-dot-converted elements (QDCEs) for (LEDs) that entirely considers the reabsorption and reemission effect is lacking. This suppresses the design of QDCE structures and further investigation of light-extraction/conversion mechanisms in QDCEs. In this paper, we proposed a full spectral optical modeling method for QDCEs packaged in LEDs, entirely considering the reabsorption and reemission effect, and its results are compared with traditional models without reabsorption or reemission. The comparisons indicate that the QDCE absorption loss of QD emission light is a major factor decreasing the radiant efficacy of LEDs, which should be considered when designing QDCE structures. According to the measurements of fabricated LEDs, only calculation results that entirely consider reabsorption and reemission show good agreement with experimental radiant efficacy, spectra, and peak wavelength at the same down-conversion efficiency. Consequently, it is highly expected that QDCE will be modeled considering the reabsorption and reemission events. This study provides a simple and effective modeling method for QDCEs, which shows great potential for their structure designs and fundamental investigations.

Green Synthesis of InP/ZnS Core/Shell Quantum Dots for Application in Heavy-Metal-Free Light-Emitting Diodes.

PubMed

Kuo, Tsung-Rong; Hung, Shih-Ting; Lin, Yen-Ting; Chou, Tzu-Lin; Kuo, Ming-Cheng; Kuo, Ya-Pei; Chen, Chia-Chun

2017-09-19

Quantum dot light-emitting diodes (QD-LEDs) have been considered as potential display technologies with the characterizations of high color purity, flexibility, transparency, and cost efficiency. For the practical applications, the development of heavy-metal-free QD-LEDs from environment-friendly materials is the most important issue to reduce the impacts on human health and environmental pollution. In this work, heavy-metal-free InP/ZnS core/shell QDs with different fluorescence were prepared by green synthesis method with low cost, safe, and environment-friendly precursors. The InP/ZnS core/shell QDs with maximum fluorescence peak at ~ 530 nm, superior fluorescence quantum yield of 60.1%, and full width at half maximum of 55 nm were applied as an emission layer to fabricate multilayered QD-LEDs. The multilayered InP/ZnS core/shell QD-LEDs showed the turn-on voltage at ~ 5 V, the highest luminance (160 cd/m 2 ) at 12 V, and the external quantum efficiency of 0.223% at 6.7 V. Overall, the multilayered InP/ZnS core/shell QD-LEDs reveal potential to be the heavy-metal-free QD-LEDs for future display applications.

Coupled field induced conversion between destructive and constructive quantum interference

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

Jiang, Xiangqian, E-mail: xqjiang@hit.edu.cn; Sun, Xiudong

2016-12-15

We study the control of quantum interference in a four-level atom driven by three coherent fields forming a closed loop. The spontaneous emission spectrum shows two sets of peaks which are dramatically influenced by the fields. Due to destructive quantum interference, a dark line can be observed in the emission spectrum, and the condition of the dark line is given. We found that the conversion between destructive and constructive quantum interference can be achieved through controlling the Rabi frequency of the external fields.

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

Theory of excess noise in unstable resonator lasers

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

Lamprecht, C.; Ritsch, H.

2002-11-01

We theoretically investigate the quantum dynamics of an unstable resonator laser. Compared to a stable cavity laser of equal gain and loss it exhibits a K-fold enhanced linewidth. This excess noise factor K is a measure of the nonorthogonality of the resonator eigenmodes and amounts to an enlargement of the quantum vacuum fluctuations. Using a quantum treatment starting from first principles based on the nonorthogonal eigenmodes, we put previous theoretical predictions onto a more firm ground. While we find a position-dependent enhancement of the spontaneous emission rate into an empty mode of only {radical}(K), the constructive quantum interference of themore » spontaneous emission with a single oscillating mode lets the Petermann excess noise factor K reappear in the phase diffusion (laser linewidth). Hence locally enhanced spontaneous emission as well as noise enhanced by interference (amplified spontaneous emission) play an equal role in the origin of excess noise.« less

Highly efficient and stable blue-emitting CsPbBr3@SiO2 nanospheres through low temperature synthesis for nanoprinting and WLED.

PubMed

Shao, He; Bai, Xue; Pan, Gencai; Cui, Haining; Zhu, Jinyang; Zhai, Yue; Liu, Jingshi; Dong, Biao; Xu, Lin; Song, Hongwei

2018-07-13

Inorganic perovskite quantum dots (QDs) have attracted wide attention in display and solid-state lighting because of their easily tunable band-gaps and high photoluminescence quantum yields (PLQY) of green light emission. However, some drawbacks limit their practical applications, including the low PLQY of blue light emission and the instability in the moisture environment. In this work, efficient blue-light emitting CsPbBr 3 perovskite QDs with PLQY of 72% were developed through a bandgap engineering approach. The achieved blue-light emitting PLQY is much higher than the values acquired in the inorganic perovskite QDs in the literature. And the emission color of the as-prepared QDs can be facially tuned by only adjusting the reaction temperature. Further, the mono-dispersed perovskite QDs@SiO 2 composites were constructed benefiting from the low temperature synthesis. The optical performance of the QDs could be well persisted even in the moisture environment. Finally, the as-prepared QDs@SiO 2 composite was fabricated as the QD ink on the anti-counterfeit printing technology, from which the obtained pattern would emit varied color under UV lamp. And the as-prepared composites was also applied for fabricating WLED, with Commission Internationale de l'Eclairage (CIE) color coordinates of (0.33, 0.38) and power efficiency of 32.5 lm W -1 , demonstrating their promising potentials in solid-state lighting.

Highly efficient and stable blue-emitting CsPbBr3@SiO2 nanospheres through low temperature synthesis for nanoprinting and WLED

NASA Astrophysics Data System (ADS)

Shao, He; Bai, Xue; Pan, Gencai; Cui, Haining; Zhu, Jinyang; Zhai, Yue; Liu, Jingshi; Dong, Biao; Xu, Lin; Song, Hongwei

2018-07-01

Inorganic perovskite quantum dots (QDs) have attracted wide attention in display and solid-state lighting because of their easily tunable band-gaps and high photoluminescence quantum yields (PLQY) of green light emission. However, some drawbacks limit their practical applications, including the low PLQY of blue light emission and the instability in the moisture environment. In this work, efficient blue-light emitting CsPbBr3 perovskite QDs with PLQY of 72% were developed through a bandgap engineering approach. The achieved blue-light emitting PLQY is much higher than the values acquired in the inorganic perovskite QDs in the literature. And the emission color of the as-prepared QDs can be facially tuned by only adjusting the reaction temperature. Further, the mono-dispersed perovskite QDs@SiO2 composites were constructed benefiting from the low temperature synthesis. The optical performance of the QDs could be well persisted even in the moisture environment. Finally, the as-prepared QDs@SiO2 composite was fabricated as the QD ink on the anti-counterfeit printing technology, from which the obtained pattern would emit varied color under UV lamp. And the as-prepared composites was also applied for fabricating WLED, with Commission Internationale de l’Eclairage (CIE) color coordinates of (0.33, 0.38) and power efficiency of 32.5 lm W‑1, demonstrating their promising potentials in solid-state lighting.

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.