Cold atmospheric plasma therapy for Malassezia folliculitis: Laboratory investigations and a randomized clinical trial.

BACKGROUND: Current treatment options for Malassezia folliculitis (MF) are limited. Recent research has demonstrated the inhibitory effect of cold atmospheric plasma (CAP) on the growth of Malassezia pachydermatis in vitro, suggesting CAP as a potential therapeutic approach for managing MF. OBJECTIVES: The objective of our study is to assess the in vitro antifungal susceptibility of Malassezia yeasts to CAP. Additionally, we aim to evaluate the efficacy and tolerability of CAP in treating patients with MF. METHODS: We initially studied the antifungal effect of CAP on planktonic and biofilm forms of Malassezia yeasts, using well-established techniques such as zone of inhibition, transmission electron microscopy, colony count assay and 2,3-bis(2-methoxy-4-nitro-5-sulfophenyl)-2H-tetrazolium-5-carboxanilide salt assay. Subsequently, a randomized (1:1 ratio), active comparator-controlled, observer-blind study was conducted comparing daily CAP therapy versus itraconazole 200 mg/day for 2 weeks in 50 patients with MF. Efficacy outcomes were measured by success rate, negative microscopy rate and changes in Dermatology Life Quality Index (DLQI) and Global Aesthetic Improvement Scale (GAIS) scores. Safety was assessed by monitoring adverse events (AEs) and local tolerability. RESULTS: In laboratory investigations, CAP time-dependently inhibited the growth of Malassezia yeasts in both planktonic and biofilm forms. Forty-nine patients completed the clinical study. At week 2, success was achieved by 40.0% of subjects in the CAP group versus 58.3% in the itraconazole group (p = 0.199). The negative direct microscopy rates of follicular samples were 56.0% in the CAP group versus 66.7% in the itraconazole group (p = 0.444). No significant differences were found in the proportion of subjects achieving DLQI scores of 0/1 (p = 0.456) or in the GAIS responder rates (p = 0.588) between the two groups. Three patients in the CAP group and one patient in the itraconazole group reported mild AEs. CONCLUSION: CAP demonstrated significant antifungal activity against Malassezia yeasts in vitro and exhibited comparable efficacy to itraconazole in treating MF patients. Without the associated adverse effects of oral antifungal drugs, CAP can be considered a promising and safe treatment modality for MF.

Fractal Branched Microwires of Organic Semiconductor with Controlled Branching and Low-Threshold Amplified Spontaneous Emission.

Fractals are quite normal in nature. However, fractal self-assembly of organic semiconductors remains challenging. Herein, we develop a facile solution assembly route to access organic microwires (MWs) comprising an oligo(p-phenylenevinylene) derivative (OPV-A) with and without branching. Instead of kinetically controlled ß-OPV-A microrods (MRs), thermodynamically favored α-OPV-A gives fractal branching MW patterns. As-prepared 9,10-dicyanoanthracene (DCA) alloyed assemblies function as seeds to allow for the heteroepitaxial growth of branching α-OPV-A MWs via either coassembly or two-step seeded growth. Consequently, fractal MWs with single- and multisite growth were both achieved, accompanied by tailorable branching densities and hierarchies. Thermodynamic control and a well-matched epitaxial relationship should be crucial to the formation of fractal MW patterns. Importantly, the aligned α-OPV-A MW array functions as a multichannel optical gain medium and exhibits low-threshold amplified spontaneous emission (ASE). The present work deepens the research into fractal self-assembly of functional organic semiconductors.

Cocrystallization tailoring radiative decay pathways for thermally activated delayed fluorescence and room-temperature phosphorescence emission.

Modulation of excited-state processes in binary organic cocrystals has been rarely explored so far. Here, we develop two charge-transfer (CT) cocrystal microrods with a 1 : 1 stoichiometric ratio where halogenated dibenzothiophene (DBT) compounds act as π-electron donors and 1,2,4,5-tetracyanobenzene (TCNB) acts as an acceptor. Unexpectedly, the cocrystal containing one bromine (Br) atom at the 3-position of DBT (3-BrTC) presents thermally activated delayed fluorescence (TADF), while the other one comprising one Br atom at the 4-position of DBT (4-BrTC) exhibits both TADF and room-temperature phosphorescence (RTP). Experimental and theoretical calculation results reveal that CT interactions in 3- and 4-BrTC decrease the S1-T2 energy gap, whereas abundant lone-pair electrons from the Br atom in 4-BrTC facilitate the n → π* transition. As a consequence, single TADF and dual-emissive TADF/RTP were realized, respectively. The present work offers wonderful insight into the effect of molecular structures on the excited-state pathways of organic CT cocrystals.

Vapor-Phase Living Assembly of π-Conjugated Organic Semiconductors.

In contrast to well-studied amphiphilic block copolymers (BCPs) and π-stacked dyes, living assembly of hydrophobic π-conjugated materials has not yet been explored to date. Using a microspacing physical vapor transport (PVT) technique, the prefabricated microrods of organic semiconductors involving 9,10-dicyanoanthracene (DCA, A) or its binary alloy (B) can act as seeds to initiate living homoepitaxial growth from their ends, giving elongated microrods with controlled length. Red-green-red tricolor fluorescent microrod heterostructures with low dispersity are further realized by living heteroepitaxial growth of B microrod blocks on A seed microrod tips. Upon varying the growth sequence of each block, reverse triblock microrods are also accessible. Such a seed-induced living growth is applicable to triblock microrod heterostructures of more binary combinations as well as even more complex penta- and hepta-block heterostructures comprising A and B. By virtue of a convenient vapor-phase growth method, the present work demonstrates the generality of living assembly of π-conjugated materials.

Hyperbranched Microwire Networks of Organic Cocrystals with Optical Waveguiding and Light-Harvesting Abilities.

We report the synthesis of hyperbranched organic microwire (MW) networks comprising 1,4-bis(pentafluorostyryl)benzene (10Ft) and 9,10-bis(phenylethynyl)anthracene (BA) using a simple solution co-assembly route. Pure 10Ft or BA assemblies cannot produce such complex MW networks; in contrast with a binary cocrystal of 10Ft and BA with a 2:1 molar ratio ((2:1)10Ft:BA), which is formed via intermolecular arene-perfluoroarene (AP) interactions. A new generation of multiple MWs grow epitaxially on the previous generation of MWs to form MW arrays in which BA may also act as an intermediate product to facilitate the regeneration of (2:1)10Ft:BA. Highly aligned and well-connected MW networks enable superior optical waveguiding ability. Moreover, a red-emitting dopant, 5,12-bis(phenylethynyl)naphthacene (BN) was incorporated into (2:1)10Ft:BA host MWs, giving light-harvesting hierarchical MW networks via an energy-transfer (ET) process. The realization of the hyperbranched MWs provides us with deep insight into the rational creation of complex branched arrays from functional organic cocrystals.

Structural evolution from the CdSSe alloy to the CdS/CdSe core/shell in Cd(S and Se) composite quantum dots and its impact on the performance of sensitized solar cells.

CdSSe alloy and CdS/CdSe core/shell quantum dots (QDs) are widely studied in quantum dot solar cells (QDSSCs). However, to date, there have been no detailed comparative investigations into the cell performance between CdSSe alloy and CdS/CdSe core/shell structures prepared with the same preparation process. In this work, the performances of CdSSe alloy and CdS/CdSe core/shell QDSSCs, which are prepared with the same SILAR (successive ionic layer adsorption and reactions) process, are investigated in detail. By simply tuning the layer numbers and arrangement sequence of the CdS and CdSe layers, a series of QDs, including CdSSe alloy structures, CdS/CdSe multilayer structures, and CdS/CdSe core/shell structures, are successfully prepared with a layer-by-layer technique, while maintaining a similar morphology. Based on these QD sensitized TiO2 photoanodes, QDSSCs are assembled. The CdS/CdSe core/shell QDSSCs yield a maximum power conversion efficiency of 5.08% under AM 1.5 illumination of 100 mW cm-2, which is increased by 77% in comparison with that of CdSSe alloy QDSSCs (2.87%). The significantly enhanced photovoltaic performance of QDSSCs with core/shell architectures is mainly attributed to their high short-circuit current density, which arises from the enhanced absorption intensity. In addition, the CdS/CdSe core-shell contributes to the attenuation of the interfacial charge recombination rate and prolongs the electron lifetime, resulting in more efficient charge collection in QDSSCs.

Organic multicomponent microparticle libraries.

Multimetallic nanostructures can be synthesized by integrating up to seven or eight metallic elements into a single nanoparticle, which represent a great advance in developing complex multicomponent nanoparticle libraries. Contrary, organic micro- and nanoparticles beyond three π-conjugated components have not been explored because of the diversity and structural complexity of molecular assemblies. Here, we report a library of microparticles composed of an arbitrary combination of four luminescent organic semiconductors. We demonstrate that the composition and emission color of each domain as well as its spatial distribution can be rationally modulated. Unary, binary, ternary, and quaternary microparticles are thus realized in a predictable manner based on the miscibility of the components, resulting in mixed-composition phases or alloyed or phase separated heterostructures. This work reports a simple yet available synthetic methodology for rational modulation of organic multicomponent microparticles with complex architectures, which can be used to direct the design of functional microparticles.

Color- and Dimension-Tunable Light-Harvesting Organic Charge-Transfer Alloys for Controllable Photon-Transport Photonics.

An electron donor/acceptor pair comprising perylene (Pe) and 9,10-dicyanoanthracene (DCA) was specifically designed to construct organic charge-transfer (CT) alloys via weak CT interaction through a solution co-assembly route. By adjusting the molar ratio between Pe and DCA, we achieve color- and dimension-tunable CT alloy assemblies involving one-dimensional (1D) (DCA)1-x (Pe)x (0 ≤ x ≤10 %) microribbons and two-dimensional (2D) (Pe)1-y (DCA)y (0 ≤ y ≤5 %) nanosheets as a consequence of energy transfer from DCA or α-Pe to Pe-DCA CT complex. Importantly, dimension-related optical waveguiding performances are also revealed: continuously adjustable optical loss in 1D (DCA)1-x (Pe)x microribbons and successive conversion from isotropic waveguide to anisotropic waveguide in 2D (Pe)1-y (DCA)y nanosheets. The present work provides a desired platform for in-depth investigation of light-harvesting organic CT alloy assemblies, which show promising applications in miniaturized optoelectronic devices.

Heat-treatment-induced development of the crystalline structure and chemical stoichiometry of a CuxS counter electrode, and the influence on performance of quantum-dot-sensitized solar cells.

Recently, various phases of CuxS (1 ≤ x ≤ 2) were extensively explored as superb counter electrode (CE) materials for quantum dot-sensitized solar cells (QDSSCs). Herein, hexagonal covellite CuS (HC-CuS) with hierarchical nanostructure was grown on porous Ti substrates by chemical bath deposition, and then heat treated in the temperature range of 150-450 °C under N2 atmosphere. The reaction process and the evolution of morphology, composition and crystalline structure of CuxS with the variation of heat treatment temperature were studied by XRD, SEM, EDX, TEM and XPS. The photovoltaic properties of TiO2/CdS/CdSe QDSSCs based on CuxS CEs showed an obvious dependence on the element stoichiometry and crystalline structure of the CuxS. With HC-Cu1.28S heat-treated at 230 °C as CEs, QDSSCs achieved a power conversion efficiency of 3.88% under one sun illumination (100 mW cm-2, AM 1.5 G), which was higher than the counterparts with other compositions. Electrochemical impedance spectroscopy, Tafel polarization and cyclic voltammetry measurement showed that the electrocatalytic activity of HC-Cu1.28S CE was much higher than that of other CuxS CEs, which supported the results of the enhanced short-circuit current density, open circuit voltage and filling factor.

Epitaxial Growth of Nanorod Meshes from Luminescent Organic Cocrystals via Crystal Transformation.

Two-dimensional (2D) nanorod meshes made of benzoperylene-1,3-dicyanotetrafluorobenzene (BP-1,3-DTFB) were formed via crystal transformation of the pre-existing BP microsheets. The transformation was driven by a cooperative effect of intermolecular charge-transfer and arene-perfluoroarene interactions. Epitaxial growth of cyan-emitting BP-1,3-DTFB nanorod meshes was directed by small lattice mismatch between BP and BP-1,3-DTFB, followed by the consumption of BP and the formation of BP-1,3-DTFB. Such a crystal transformation strategy can also be used to guide the formation of BP-1,4-dicyanotetrafluorobenzene (BP-1,4-DTFB) nanorod meshes. The present work reports a simple yet effective approach for the realization of aligned organic nanorod superstructures.

Two-dimensional C60 nano-meshes via crystal transformation.

Developing a rational and general approach towards complex two-dimensional (2D) nanostructures represents potential promising applications in a wide variety of fields, such as electronics, catalysis, and energy conversion. However, the synthesis of 2D nanoscale superstructures remains a great challenge because of the great difficulty in arranging the growth units in a rational manner. Here, we develop a simple yet effective solution-phase strategy to achieve hexagonal mesh networks made of aligned nanorods which are obtained via crystal transformation of 2D C60 microplates. The transformation is triggered by the removal and inclusion of solvent molecules and hence, driven by a small free energy difference. The change in the local solvent environment leads to the formation of pores in the C60 plates and the subsequent growth of nanorods. The epitaxial growth of ordered nanorod arrays is due to the matching lattice between the (111) facet of the fcc plate and the (101[combining macron]0) facet of the hcp rod. This route of co-solvent induced crystal transformation provides a unique mechanistic perspective and a new direction for designing complex crystals. Furthermore, more complicated 2D C60 mesh networks, such as multi-layer hexagonal meshes, have also been rationally achieved via such a facile crystal transformation strategy.

Complex assembly from planar and twisted π-conjugated molecules towards alloy helices and core-shell structures.

Integrating together two dissimilar π-conjugated molecules into controlled complex topological configurations remains a largely unsolved problem owing to the diversity of organic species and their respective different assembly features. Here, we find that two structurally similar organic semiconductors, 9,10-bis(phenylethynyl)anthracene (BA) and 5,12-bis(phenylethynyl)naphthacene (BN), co-assemble into two-component helices by control of the growth kinetics as well as the molar ratio of BA/BN. The helical superstructures made of planar and twisted bis(phenylethynyl) derivatives can be regarded as (BA)x(BN)1-x alloys, which are formed due to compatible structural relationship between BA and BN. Moreover, epitaxial growth of (BA)x(BN)1-x alloy layer on the surface of BA tube to form BA@(BA)x(BN)1-x core-shell structure is also achieved via a solute exchange process. The precise control over composition and morphology towards organic alloy helices and core-shell microstructures opens a door for understanding the complex co-assembly features of two or more different material partners with similar structures.

Solvatomechanical Bending of Organic Charge Transfer Cocrystal.

We report here a new ternary solvated (perylene-TCNB)·2THF cocrystal, which can transform into binary perylene-TCNB cocrystal reversibly by successive desorption or absorption of THF solvent. As a consequence, macroscopic mechanical bending would be realized when repeated stimulation with THF solvent. The present results clearly demonstrated that solvent induced mechanical bending is driven by structural change at the molecular scale. Such solvatomechanical bending behavior is clearly revealed for the first time.

Competition between Arene-Perfluoroarene and Charge-Transfer Interactions in Organic Light-Harvesting Systems.

Two typical types of luminescent organic cocrystals comprising pyrene-octafluoronaphthalene (pyrene-OFN) and pyrene-1,2,4,5-tetracyanobezene (pyrene-TCNB) were developed by a simple supramolecular assembly strategy. The cocrystals exhibit distinct optical properties because of their different intermolecular interaction modes; that is, arene-perfluoroarene (AP) and charge-transfer (CT) interactions. Unexpectedly, a pyrene-TCNB system with strong CT interactions was incorporated into a pyrene-OFN host as a robust guest to generate white-light emission (WLE). In the supramolecular cocrystal system, an efficient energy-transfer process from pyrene-OFN to pyrene-TCNB occurred because of the well-matched spectra of the constituents and a desirable energy donor/acceptor (D/A) distance. The present competitive intermolecular interaction strategy could be applied to the fabrication of more complicated organic light-harvesting systems.

Facet-Selective Growth of Organic Heterostructured Architectures via Sequential Crystallization of Structurally Complementary π-Conjugated Molecules.

In contrast to those for their polymeric counterparts, the controlled construction of organic heterostructured architectures derived from π-conjugated organic molecules has been rare and remains a great challenge. Herein, we develop a simple single-step solution strategy for the realization of organic heterostructures comprising coronene and perylene. Under a sequential crystallization process, an efficient doping step for coronene and perylene domains enables their perfect lattice matching, which facilitates facet-selective epitaxial growth of perylene domains on both the tips and the side surfaces of the preformed seed microwires by manipulating the growth pathways of the two pairs of materials. The present synthetic route provides a promising platform to investigate the detailed formation mechanism of complex organic heterostructures with specific topological configurations, further directing the construction of more functional heterostructured materials.

Constructing luminescent particle/MOF composites by employing polyvinylpyrrolidone-modified organic crystals as seeds.

We develop a novel and facile chemical reaction route to modulate the crystallization process of luminescent zinc 8-hydroxyquinoline (Znq2) particles. Polyvinylpyrrolidone (PVP)-modified octahedral Znq2 micro- and nano-crystals were used as seeds to construct two distinct hybrid structures, i.e., Znq2@ZIF-8 core-shell and multiple Znq2 particles on each ZIF-8.

Hierarchically porous Pd nanospheres: facile synthesis and their application in HCOOH electrooxidation.

With the help of rhodamine B base (RBB), novel Pd nanospheres were synthesized by a facile one-step approach. Owing to their hierarchically porous characteristics, these nanospheres exhibited highly catalytic activity for HCOOH electrooxidation (∼1.84 times and 1.67 times higher than those of a commercial Pd/C catalyst for mass and specific activity, respectively).

Two-dimensional optical waveguiding and luminescence vapochromic properties of 8-hydroxyquinoline zinc (Znq2) hexagonal microsheets.

Two-dimensional (2D) hexagonal microsheets of 8-hydroxyquinoline zinc (Znq2) were synthesized readily via a mixed solvent induced self-assembly method. The 2D optical waveguiding properties of the microsheets have been clearly revealed by both fluorescence microscopy and confocal microscopy. In addition, the reversible vapochromic properties of the microsheets have also been demonstrated when the Znq2 is exposed to HCl and NH3 vapors.

White-light emitting microtubes of mixed organic charge-transfer complexes.

Self-assembled microtubes of mixed charge-transfer (CT) complexes comprising TCNB and naphthalene can be constructed with pyrene as dopant by an etching-assisted CT-induced interaction. Highly efficient Förster resonance energy transfer (FRET) from the excited naphthalene-TCNB to pyrene-TCNB molecules is obtained in mixed CT complex microtubes. White-light emissive CT complex microtubes can be formed by adjusting the dopant concentration and serve as an active optical waveguide.

Fullerene hollow microspheres prepared by bubble-templates as sensitive and selective electrocatalytic sensor for biomolecules.

We developed an electrocatalytic sensor based on C(60) hollow microspheres for highly sensitive and selective detection of dopamine (DA) in the presence of ascorbic acid (AA), and uric acid (UA) in the presence of l-cysteine (RSH). The hollow microspheres of C(60) with a diameter controllable in the range of 0.5 to 1.5 µm and a thickness of 200 nm are synthesized by a high-temperature reprecipitation method with the assistance of alcohol bubbles. The superhydrophobicity of C(60) hollow microspheres makes them capable of forming a compact thin film at air/water interface, which can be readily transferred on the surface of gold or glassy carbon electrodes. This porous C(60) film made from C(60) hollow microspheres shows a specific surface area as high as 107 m(2) g(-1). In order to obtain a conducting film, the C(60)-modified electrode is pretreated by scanning the potential range from 0.0 to -1.5 V in 1 M KOH followed by potential cycling between 550 to -50 mV in a pH 7.2 phosphate buffer solution. On the basis of XPS and IR measurements, we found that surface oxides, such as -OH and C═O groups, are introduced on the surfaces of the conducting C(60) film. This, combined with the porosity that enhances the adsorption activity of C(60)-modified electrodes, enable the electrocatalytic analysis of target biomolecules with detection limit as low as 0.1 nM for DA in the presence of AA, and 1 µM for UA in the presence of RSH.