Facile fabrication of two-dimensional inorganic nanostructures and their conjugation to nanocrystals

Nanocomposites of two-dimensional (2D) inorganic nanosheets and inorganic nanocrystals are fabricated. Freestanding atomically flat gamma-AlOOH nanosheets (thickness <1 nm) are synthesized from a one-pot hydrothermal reaction. The freestanding and binder-free film composed of the gamma-AlOOH nanosheets is fabricated by sedimentation. Because they have positive zeta potentials in the pH range below ca. 9.3, the gamma-AlOOH nanosheets can function as positively charged 2D inorganic matrices in a broad pH range. By solution phase (pH 7.0) mixing of the gamma-AlOOH nanosheets (zeta potential: 30.7 +/- 0.8 mV) and inorganic nanocrystals with negative surface charge, including Au nanoparticles, Au nanorods, CdSe quantum dots, CdSe/CdS/ZnS quantum dots and CdSe nanorods, the nanocomposites are self-assembled via electrostatic interactions. Negatively charged inorganic nanostructures with a wide range of chemical compositions, shapes, sizes, surface ligands and adsorbates can be used as building blocks for gamma-AlOOH nanocomposites. Adsorption densities of inorganic nanocrystals on the nanocomposites can be controlled by varying concentrations of nanocrystal solutions. Nanocomposite films containing alternating layers of gamma-AlOOH and nanocrystals are obtained by a simple drop casting method.close3

Highly Fluorescent and Stable Quantum Dot-Polymer-Layered Double Hydroxide Composites

We report a designed strategy for a synthesis of highly luminescent and photostable composites by incorporating quantum dots (QDs) into layered double hydroxide (LDH) matrices without deterioration of a photoluminescence (PL) efficiency of the fluorophores during the entire processes of composite formations. The QDs synthesized in an organic solvent are encapsulated by polymers, poly(maleic acid-alt-octadecene) to transfer them into water without altering the initial surface ligands. The polymer-encapsulated QDs with negative zeta potentials (-29.5 +/- 2.2 mV) were electrostatically assembled with positively charged (24.9 +/- 0.6 mV) LDH nanosheets to form QD-polymer-LDH composites (PL quantum yield: 74.1%). QD-polymer-LDH composite films are fabricated by a drop-casting of the solution on substrates. The PL properties of the films preserve those of the organic QD solutions. We also demonstrate that the formation of the QD-polymer-LDH composites affords enhanced photostabilities through multiple protections of QD surface by polymers and LDH nanosheets from the environment

Highly Fluorescent and Stable Quantum Dot-Polymer-Layered Double Hydroxide Composites

We report a designed strategy for a synthesis of highly luminescent and photostable composites by incorporating quantum dots (QDs) into layered double hydroxide (LDH) matrices without deterioration of a photoluminescence (PL) efficiency of the fluorophores during the entire processes of composite formations. The QDs synthesized in an organic solvent are encapsulated by polymers, poly(maleic acid-alt-octadecene) to transfer them into water without altering the initial surface ligands. The polymer-encapsulated QDs with negative zeta potentials (-29.5 +/- 2.2 mV) were electrostatically assembled with positively charged (24.9 +/- 0.6 mV) LDH nanosheets to form QD-polymer-LDH composites (PL quantum yield: 74.1%). QD-polymer-LDH composite films are fabricated by a drop-casting of the solution on substrates. The PL properties of the films preserve those of the organic QD solutions. We also demonstrate that the formation of the QD-polymer-LDH composites affords enhanced photostabilities through multiple protections of QD surface by polymers and LDH nanosheets from the environment.X114441sciescopu

Femto-second laser beam with a low power density achieved a two-photon photodynamic cancer therapy with quantum dots

Focusing the femto-second (fs) laser beam on the target was the usual way to carry out a two-photon excitation (TPE) in previous photodynamic therapy (PDT) studies. However, focusing the laser deep inside the tissues of the tumor is unrealistic due to tissue scattering, so that this focusing manner seems unfit for practical TPE PDT applications. In this work, we prepared a conjugate of quantum dots (QDs) and sulfonated aluminum phthalocyanine (AlPcS) for TPE PDT, because QDs have a very high two-photon absorption cross section (TPACS) and thus QDs can be excited by an unfocused 800 nm fs laser beam with a low power density and then transfer the energy to a conjugated AlPcS via fluorescence resonance energy transfer (FRET). The FRET efficiency of the QD-AlPcS conjugate in water was as high as 90%, and the FRET process of the cellular QD-AlPcS was also observed in both KB and HeLa cells under TPE of a 800 nm fs laser. The singlet oxygen (O-1(2)) products were produced by the QD-AlPcS under the TPE of the unfocused 800 nm fs laser via FRET mediated PDT. Moreover, the QD-AlPcS can effectively destroy these cancer cells under the irradiation of the 800 nm unfocused fs laser beam with a power density of 92 mW mm(-2), and particularly the killing efficiency of the TPE is comparable to that of the commonly used one-photon excitation (OPE) at visible wavelengths. These results highlight the potential of QD-AlPcS for TPE PDT with a near infrared wavelength.open112019sciescopu

Imaging Depths of Near-Infrared Quantum Dots in First and Second Optical Windows

Potential advantages of quantum dot (QD) imaging in the second optical window (SOW) at 1,000 to 1,400 nm over the first optical window (FOW) at 700 to 900 nm have attracted much interest. QDs that emit at 800 nm (800QDs) and QDs that emit at 1,300 nm (1,300QDs) are used to investigate the imaging depths at the FOW and SOW. QD images in biologic tissues are processed binarized via global thresholding method, and the imaging depths are determined using the criteria of contrast to noise ratio and relative apparent size. Owing to the reduced scattering in the SOW, imaging depth in skin can be extended by approximately three times for 1,300QD/SOW over 800QD/FOW. In liver, excitation of 1,300QD/SOW can be shifted to longer wavelengths; thus, the imaging depth can be extended by 1.4 times. Effects of quantum yield (QY), concentration, incidence angle, polarization, and fluence rate F on imaging depth are comprehensively studied. Under F approved by the Food and Drug Administration, 1,300QDs with 50% QY can reach imaging depths of 29.7 mm in liver and 17.5 mm in skin. A time-gated excitation using 1,000 times higher F pulses can obtain the imaging depth of ≈ 5 cm. To validate our estimates, in vivo whole-body imaging experiments are performed using small-animal models

Highly Fluorescent and Stable Quantum Dot-Polymer-Layered Double Hydroxide Composites

We report a designed strategy for a synthesis of highly luminescent and photostable composites by incorporating quantum dots (QDs) into layered double hydroxide (LDH) matrices without deterioration of a photoluminescence (PL) efficiency of the fluorophores during the entire processes of composite formations. The QDs synthesized in an organic solvent are encapsulated by polymers, poly­(maleic acid-alt-octadecene) to transfer them into water without altering the initial surface ligands. The polymer-encapsulated QDs with negative zeta potentials (−29.5 ± 2.2 mV) were electrostatically assembled with positively charged (24.9 ± 0.6 mV) LDH nanosheets to form QD-polymer-LDH composites (PL quantum yield: 74.1%). QD-polymer-LDH composite films are fabricated by a drop-casting of the solution on substrates. The PL properties of the films preserve those of the organic QD solutions. We also demonstrate that the formation of the QD-polymer-LDH composites affords enhanced photostabilities through multiple protections of QD surface by polymers and LDH nanosheets from the environment

Imaging depths of near-infrared quantum dots in first and second optical windows

Potential advantages of quantum dot (QD) imaging in the second optical window (SOW) at 1,000 to 1,400 nm over the first optical window (FOW) at 700 to 900 nm have attracted much interest. QDs that emit at 800 nm (800QDs) and QDs that emit at 1,300 nm (1,300QDs) are used to investigate the imaging depths at the FOW and SOW. QD images in biologic tissues are processed binarized via global thresholding method, and the imaging depths are determined using the criteria of contrast to noise ratio and relative apparent size. Owing to the reduced scattering in the SOW, imaging depth in skin can be extended by approximately three times for 1,300QD/SOW over 800QD/FOW. In liver, excitation of 1,300QD/SOW can be shifted to longer wavelengths; thus, the imaging depth can be extended by 1.4 times. Effects of quantum yield (QY), concentration, incidence angle, polarization, and fluence rate F on imaging depth are comprehensively studied. Under F approved by the Food and Drug Administration, 1,300QDs with 50% QY can reach imaging depths of 29.7 mm in liver and 17.5 mm in skin. A time-gated excitation using 1,000 times higher F pulses can obtain the imaging depth of approximate to 5 cm. To validate our estimates, in vivo whole-body imaging experiments are performed using small-animal models.archiving status unknown114941sciescopu

Metal ion-induced dual fluorescent change for aza-crown ether acridinedione-functionalized gold nanorods and quantum dots

Aza-crown ether acridinedione-functionalized quantum dots (ACEADD-QDs) and aza-crown ether acridinedione-functionalized gold nanorods (ACEADD-GNRs) have been developed as a pair for a fluorescent chemosensor detecting metal ions. The ACEADD-QDs have dual emissions at a visible wavelength of similar to 430 nm from the acridinedione dye moiety and at a near-infrared (NIR) wavelength of similar to 775 nm from the CdTeSe QDs. In the presence of Ca2+ or Mg2+ ions, the ACEADD-QD and ACEADD-GNR pair can form a sandwich complex mediated by the metal ion. The ACEADD-QD and ACEADD-GNR complex pair shows visible fluorescence enhancement from the acridinedione dye and concurrent fluorescence quenching from the NIR QD. The aza-crown ether complex results in the suppression of photoinduced electron transfer from the aza-crown ether to the acridinedione dye moiety. At the same time, the QD fluorescence can be effectively quenched by the nanometal surface energy transfer from the QD to the GNR. This ACEADD-QD and ACEADD-GNR pair can effectively transduce the selective binding event of crown ethers with metal ions into the simultaneous modulation of the enhancement in dye fluorescence and the quenching of QD emission, which can open a new strategy for ratiometric sensors that are selective and robust against the environment conditions.open111315sciescopu

Quantum dot-engineered M13 virus layer-by-layer composite films for highly selective and sensitive turn-on TNT sensors

We developed quantum dot-engineered M13 virus layer-by-layer hybrid composite films with incorporated fluorescence quenchers. TNT is designed to displace the quenchers and turn on the quantum dot fluorescence. TNT was detected at the sub ppb level with a high selectivity.open111516sciescopu

Imaging Depths of Near-Infrared Quantum Dots in First and Second Optical Windows

Potential advantages of quantum dot (QD) imaging in the second optical window (SOW) at 1,000 to 1,400 nm over the first optical window (FOW) at 700 to 900 nm have attracted much interest. QDs that emit at 800 nm (800QDs) and QDs that emit at 1,300 nm (1,300QDs) are used to investigate the imaging depths at the FOW and SOW. QD images in biologic tissues are processed binarized via global thresholding method, and the imaging depths are determined using the criteria of contrast to noise ratio and relative apparent size. Owing to the reduced scattering in the SOW, imaging depth in skin can be extended by approximately three times for 1,300QD/SOW over 800QD/FOW. In liver, excitation of 1,300QD/SOW can be shifted to longer wavelengths; thus, the imaging depth can be extended by 1.4 times. Effects of quantum yield (QY), concentration, incidence angle, polarization, and fluence rate F on imaging depth are comprehensively studied. Under F approved by the Food and Drug Administration, 1,300QDs with 50% QY can reach imaging depths of 29.7 mm in liver and 17.5 mm in skin. A time-gated excitation using 1,000 times higher F pulses can obtain the imaging depth of ≈ 5 cm. To validate our estimates, in vivo whole-body imaging experiments are performed using small-animal models