Photoelectrochemical DNA biosensor based on g-C3N4/MoS2 2D/2D heterojunction electrode matrix and co-sensitization amplification with CdSe QDs for the sensitive detection of ssDNA.

A novel enhanced photoelectrochemical (PEC) DNA biosensor, based on a compact heterojunction g-C3N4/MoS2 and co-sensitization effect with CdSe quantum dots (QDs), was first proposed for simple and accurate analysis of a short ssDNA. In this work, the g-C3N4/MoS2 was successfully synthesized and used as the electrode matrix material to construct PEC biosensor. 2D/2D heterojunction was formed between g-C3N4 and MoS2, which could promote the separation of photogenerated electron-hole pairs resulting in an enhanced photocurrent. In the presence of target DNA, CdSe QDs labeled reporter DNA was complementary pairing with target DNA which was specific recognized by capture DNA loading on self-assembled CdS QDs film, leading to close contact between CdSe QDs and g-C3N4/MoS2 modified electrode surface, thereby resulting in the enhanced photocurrent intensity due to the co-sensitization effect. Under the optimal operating conditions, the photoelectrochemical biosensor demonstrated favorable accuracy and could respond to 0.32 pM (S/N = 3) with a linear concentration range from 1.0 pM to 2.0 µM. Moreover, the proposed PEC DNA biosensor exhibits high sensitivity, excellent specificity, acceptable reproducibility and accuracy, showing a promising potential in DNA bioanalysis and other relative fields.

Construction of photoelectrochemical thrombin aptasensor via assembling multilayer of graphene-CdS nanocomposites.

A photoelectrochemical (PEC) aptasensor for highly sensitive and specific detection of thrombin was developed by using graphene­CdS nanocomposites multilayer as photoactive species and electroactive mediator hexaammineruthenium(III) chloride (Ru(NH(3))(6)(3+)) as signal enhancer. Graphene­CdS nanocomposites (G­CdS) were synthesized by one-pot reduction of oxide graphene and CdCl2 with thioacetamide. The photoactive multilayer was prepared by alternative assembly of the negatively charged 3-mercaptopropionic acid modified graphene­CdS nanocomposites (MPA-G­CdS) and the positively charged polyethylenimine (PEI) on ITO electrode. This layer-by-layer assembly method enhanced the stability and homogeneity of the photocurrent readout of G­CdS. Thrombin aptamer was covalently bound to the multilayer by using glutaraldehyde as cross-linking. Electroactive mediator (Ru(NH(3))(6)(3+)) could interact with the DNA phosphate backbone and thus facilitated the electron transfer between G­CdS multilayer and electrode and enhanced the photocurrent. Hybridizing of a long complementary DNA with thrombin aptamer could increase the adsorption amount of (Ru(NH(3))(6)(3+)), which in turn boosted the signal readout. In the presence of target thrombin, the affinity interaction between thrombin and its aptamer resulted in the long complementary DNA releasing from the G­CdS multilayer and decreasing of photocurrent signal. On the basis of G­CdS multilayer as the photoactive species, (Ru (NH(3))(6)(3+)) as an electroactive mediator, and aptamer as a recognition module, a high sensitive PEC aptasensor for thrombin detection was proposed. The thrombin aptasensor displayed a linear range from 2.0 pM to 600.0 pM and a detection limit of 1.0 pM. The present strategy provided a promising ideology for the future development of PEC biosensor.

Photocurrent polarization anisotropy of randomly oriented nanowire networks.

While the polarization sensitivity of single or aligned NW ensembles is well-known, this article reports on the existence of residual photocurrent polarization sensitivities in random NW networks. In these studies, CdSe and CdTe NWs were deposited onto glass substrates and contacted with Au electrodes separated by 30-110 microm gaps. SEM and AFM images of resulting devices show isotropically distributed NWs between the electrodes. Complementary high resolution TEM micrographs reveal component NWs to be highly crystalline with diameters between 10 and 20 nm and with lengths ranging from 1 to 10 microm. When illuminated with visible (linearly polarized) light, such random NW networks exhibit significant photocurrent anisotropies rho = 0.25 (sigma = 0.04) [rho = 0.22 (sigma = 0.04)] for CdSe (CdTe) NWs. Corresponding bandwidth measurements yield device polarization sensitivities up to 100 Hz. Additional studies have investigated the effects of varying the electrode potential, gap width, and spatial excitation profile. These experiments suggest electrode orientation as the determining factor behind the polarization sensitivity of NW devices. A simple geometric model has been developed to qualitatively explain the phenomenon. The main conclusion from these studies, however, is that polarization sensitive devices can be made from random NW networks without the need to align component wires.

Polarization-sensitive nanowire photodetectors based on solution-synthesized CdSe quantum-wire solids.

Polarization-sensitive photodetectors are demonstrated using solution-synthesized CdSe nanowire (NW) solids. Photocurrent action spectra taken with a tunable white light source match the solution linear absorption spectra of the NWs, showing that the NW network is responsible for the device photoconductivity. Temperature-dependent transport measurements reveal that carriers responsible for the dark current through the nanowire solids are thermally excited across CdSe band gap. The NWs are aligned using dielectrophoresis between prepatterned electrodes using conventional optical photolithography. The photocurrent through the NW solid is found to be polarization-sensitive, consistent with complementary absorption (emission) measurements of both single wires and their ensembles. The range of solution-processed semiconducting NW materials, their facile synthesis, ease of device fabrication, and compatibility with a variety of substrates make them attractive for potential nanoscale polarization-sensitive photodetectors.

Role of free cadmium and selenium ions in the potential mechanism for the enhancement of photoluminescence of CdSe quantum dots under ultraviolet irradiation.

The present study describes an enhancement of the photoluminescence of CdSe quantum dots under long-term ultraviolet irradiation in organic solvents. The photoenhancement effect followed multiexponential kinetics and was found to depend on several factors: intensity of ultraviolet light, polarity of the solvent, presence of capping agents on the nanocrystal surface, and presence of free Cd and Se ions in the solution. High intensity ultraviolet irradiation provoked a rapid enhancement of the photoluminescence of CdSe nanocrystals, reaching the maximum with subsequent photoluminescence decay. Low-intensity ultraviolet irradiation provoked a comparatively slow enhancement of the photoluminescence of CdSe nanocrystals, reaching saturation after 5-6 hours of irradiation in organic solvents (butanol and chloroform). The photoenhancement effect was reversible or irreversible depending on the additional ingredients. The role of free Cd and Se in these processes was clarified. The results are discussed in the context of ultraviolet induced liberation of free Cd and Se ions from the nanocrystal surface and their hypothetical reversible deposition with trapping of the surface holes and influencing the efficiency of radiative versus nonradiative exciton decay during the enhancement of photoluminescence.

Monodispersed spherical colloids of Se@CdSe: synthesis and use as building blocks in fabricating photonic crystals.

Monodispersed spherical core-shell colloids of Se@Ag(2)Se have been exploited as a chemical template to synthesize Se@CdSe core-shell particles using a cation-exchange reaction. A small amount of tributylphosphine could facilitate the replacement of Ag(+) by Cd(2+) in methanol at 50 degrees C to complete the conversion within 150 min. The orthorhombic structure of beta-Ag(2)Se changed to a well-defined wurtzite lattice for CdSe. The CdSe shells could be converted back to beta-Ag(2)Se by reacting with AgNO(3) in methanol at room temperature. Because of the uniformity in size and high refractive index associated with the Se@CdSe core-shell colloids, they could serve as a new class of building blocks to fabricate photonic crystals with wide and strong stop bands.