Polyamine detergents tailored for native mass spectrometry studies of membrane proteins.

Native mass spectrometry (MS) is a powerful technique for interrogating membrane protein complexes and their interactions with other molecules. A key aspect of the technique is the ability to preserve native-like structures and noncovalent interactions, which can be challenging depending on the choice of detergent. Different strategies have been employed to reduce charge on protein complexes to minimize activation and preserve non-covalent interactions. Here, we report the synthesis of a class of polyamine detergents tailored for native MS studies of membrane proteins. These detergents, a series of spermine covalently attached to various alkyl tails, are exceptional charge-reducing molecules, exhibiting a ten-fold enhanced potency over spermine. Addition of polyamine detergents to proteins solubilized in maltoside detergents results in improved, charge-reduced native mass spectra and reduced dissociation of subunits. Polyamine detergents open new opportunities to investigate membrane proteins in different detergent environments that have thwarted previous native MS studies.

Photopolymerized superhydrophobic hybrid coating enabled by dual-purpose tetrapodal ZnO for liquid/liquid separation.

Low-cost and scalable superhydrophobic coating methods provide viable approaches for energy-efficient separation of immiscible liquid/liquid mixtures. A scalable photopolymerization method is developed to functionalize porous substrates with a hybrid coating of tetrapodal ZnO (T-ZnO) and polymethacrylate, which exhibits simultaneous superhydrophobicity and superoleophilicity. Here, T-ZnO serves dual purposes by (i) initiating radical photopolymerization during the fabrication process through a hole-mediated pathway and (ii) providing a hierarchical surface roughness to amplify wettability characteristics and suspend liquid droplets in the metastable Cassie-Baxter regime. Photopolymerization provides a means to finely control the conversion and spatial distribution of the formed polymer, whilst allowing for facile large-area fabrication and potential coating on heat-sensitive substrates. Coated stainless-steel meshes and filter papers with desired superhydrophobic/superoleophilic properties exhibit excellent performance in separating stratified oil/water, oil/ionic-liquid, and water/ionic-liquid mixtures as well as water-in-oil emulsions. The hybrid coating demonstrates desired mechanical robustness and chemical resistance for their long-term application in large-scale energy-efficient separation of immiscible liquid/liquid mixtures.

High-Efficiency Red and Near-Infrared Organic Light-Emitting Diodes Enabled by Pure Organic Fluorescent Emitters and an Exciplex-Forming Cohost.

Three D-A-D-configured molecules DTPBT, DTPNT, and DTPNBT with high quantum yield of orange red (628 nm), red (659 nm), and deep-red/NIR (710 nm) fluorescence, respectively, were developed as emitting dopants in an exciplex-forming cohost (TCTA:3P-T2T) for high-efficiency fluorescence-based organic light-emitting diodes (OLEDs). The obtained physical properties together with theoretical calculations analyzed from these new molecules establish a clear structure-property relationship, in which the feature of central acceptor 2,1,3-benzothiadiazole (BT), naphtho[1,2-c:5,6-c']bis[1,2,5]thiadiazole (NT), and 2,1,3-naphthothiadiazole (NBT) plays the crucial role for governing the physical characteristics. The optimized device configured as ITO/HAT-CN/TAPC/TCTA/TCTA:3P-T2T:5% emitter/3P-T2T/LiF/Al gave a record-high efficiency of orange red (591 nm, 15%), red (647 nm, 10%), and deep-red/NIR (689 nm, 9%) electroluminescent devices. The effective harvest of triplet excitons with an exciplex-forming system in conjunction with efficient energy transfer between the exciplex and the dopant is beneficial for such high device efficiencies. More importantly, the stable exciplex-forming cohost and fast radiative decay rate of DTPNT render this particular device exhibiting high device stability as indicated by the low efficiency roll-off under high current densities (EQE (external quantum efficiency) values of 8.1% at 1000 cd m-2 and 6.8% at 10,000 cd m-2). These results reveal the potential of employing an exciplex-forming system as cohost for fluorescent dopants to furnish high-efficiency OLEDs with an emission wavelength extending to the red or even the NIR range.

Frequency-Selective Photobleaching as a Route to Chromatic Control in Supramolecular OLED Devices.

We report a series of molecules that spontaneously self-organize into small electroluminescent domains of sub-micrometer dimensions when dissolved in tetrahydrofuran. The self-assembled spherical aggregates have an average diameter of 300 nm and exhibit efficient energy transfer from the blue to the green or red component. The aggregates can be chromatically addressed or patterned by selective bleaching of the energy-acceptor component using a laser source. This allows the fabrication of electroluminescence devices by directly photopatterning the active layer without the need of additional steps. Submicron features (700 nm) can be achieved using a collimated light source.

Remote Steric Effect as a Facile Strategy for Improving the Efficiency of Exciplex-Based OLEDs.

This work reports a new strategy of introducing remote steric effect onto the electron donor for giving the better performance of the exciplex-based organic light-emitting device (OLED). The bulky triphenylsilyl group (SiPh3) was introduced onto the fluorene bridge of 4,4'-(9H-fluorene-9,9-diyl)bis(N,N-di-p-tolylaniline) (DTAF) to create remote steric interactions for increasing the possibility of effective contacts between electron-donating chromophores and acceptor molecules, rendering the resulting exciplex to have a higher photoluminescence quantum yield (PLQY). The green exciplex device based on DSDTAF:3N-T2T (1:1) as an emitting layer exhibits a low turn-on voltage of 2.0 V, high maximum efficiencies (13.2%, 42.9 cd A-1, 45.5 lm W-1), which are higher than the device employed DTAF (without SiPh3 groups) (11.6%, 35.3 cd A-1, 41.3 lm W-1) as donor under the same device structure. This strategy was further examined for blue exciplex, where the EQE was enhanced from 9.5% to 12.5% as the electron acceptor PO-T2T mixed with a tert-butyl group substituted carbazole-based donor (CPTBF) as the emitting exciplex in device. This strategy is simple and useful for developing high performance exciplex OLEDs.