Good solvent, poor solvent: A simple precipitation method enabled the spontaneous formation of homogeneous C70 cube crystals by self‐crystallization in cavities of a good solvent (mesitylene) surrounded by a poor solvent (isopropyl alcohol, IPA; see picture). The enormously increased photoluminescence (PL) intensity of the C70 cube crystals relative to that of C70 powder was mainly attributed to the high crystallinity of the cubes.
We have explored the link between morphologies and conductivities for ionic liquids (ILs) incorporated block copolymer electrolytes by combining small-angle X-ray scattering, transmission electron microscopy, and impedance spectroscopy. The block copolymer electrolytes investigated in present study are a series of partially sulfonated poly(styrenesulfonate-b-methylbutylene) (S
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) copolymers with different molecular weights and sulfonation levels (SLs). Imidazolium-based ILs are selectively doped into hydrophilic domains of S
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copolymers, and various morphologies have been observed as a function of the amount of absorbed ILs and SLs in S
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copolymers. We have demonstrated that the morphologies of ILs impregnated S
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copolymers are sensitive function of kinds of counteranions in IL, yielding remarkable discrepancy in conductivities. When the morphology of sample is appeared to be a lamellar structure, significant reduction in through-plane conductivity value was detected due to the nonrandom orientation of microdomains. In contrast, hexagonally perforated lamellar forming samples exhibit the highest conductivities in both through-plane and in-plane directions on account of the better connectivity of ionic domains along the perforated hydrophilic phases. Once the morphology effects were vanished by employing highly sulfonated S
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copolymers, it has been revealed that the conductivities of ILs incorporated copolymers are closely related to the polarity of ILs as confirmed by solvation dynamics study.
Fluorescent proteins with large Stokes shifted emission beyond 600 nm are actively sought for live-cell imaging applications. The mechanism of excited-state relaxation leading to the Stokes shift in the mPlum fluorescent protein, which emits at a peak wavelength of 650 nm, has been previously investigated by both ultrafast spectroscopy and theoretical methods. Here, we report that femtosecond time-resolved area-normalized emission spectra of mPlum show a clear isoemissive point. This feature can only result from a system with two emitting states, rather than a system that undergoes a continuous spectral red shift, for example, as expected from typical solvation. Global analysis of the femtosecond time-resolved fluorescence spectra reveals time constants associated with chromophore relaxation, excited-state population transfer, and an excited-state lifetime of the final state. The observations confirm the findings of recent quantum chemical calculations on mPlum.
Gutes Solvens, schlechtes Solvens: Durch einfaches Fällen gelingt die spontane Bildung homogener würfelförmiger C70‐Kristalle durch Selbstkristallisation in den Hohlräumen eines guten Solvens (Mesitylen), die von einem schlechten Solvens (Isopropylalkohol, IPA; siehe Bild) umgeben sind. Die enorm erhöhte Photolumineszenz(PL)‐Intensität der C70‐ Kristalle gegenüber C70‐Pulver wurde in erster Linie auf die hohe Kristallinität der Würfel zurückgeführt.
Using a macroscopic ensemble of highly-enriched (6,5) single-wall carbon nanotubes, combined with high signal-to-noise ratio, time-dependent differential transmission spectroscopy, we have generated vibrational modes in an ultrawide spectral range (10-3000 cm −1 ). A total of fourteen modes were clearly resolved and identified, including fundamental modes of A, E1, and E2 symmetries and their combinational modes involving two and three phonons. Through comparison with CW Raman spectra as well as calculations based on an extended tight-binding model, we were able to identify all the observed peaks and determine the frequencies of the individual and combined modes. We provide a full summary of phonon frequencies for (6,5) nanotubes that can serve as a basic reference with which to refine our understanding of nanotube phonon spectra as well as a testbed for new theoretical models.
EDGE ARTICLEAndrew J. deMello, Joshua B. Edel et al. Rapid cell extraction in aqueous twophase microdroplet systems PERSPECTIVE Barry M. Trost et al. Catalytic asymmetric allylic alkylation employing heteroatom nucleophiles: a powerful method for C-X bond formation
Far-red fluorescent proteins are critical for in vivo imaging applications, but the relative importance of structure versus dynamics in generating large Stokes-shifted emission is unclear. The unusually red-shifted emission of TagRFP675, a derivative of mKate, has been attributed to the multiple hydrogen bonds with the chromophore N-acylimine carbonyl. We characterized TagRFP675 and point mutants designed to perturb these hydrogen bonds with spectrally-resolved transient grating and time-resolved fluorescence (TRF) spectroscopies supported by molecular dynamics simulations. TRF results for TagRFP675 and the mKate/M41Q variant show ps timescale red-shifts followed by ns time blue-shifts. Global analysis of the TRF spectra reveals spectrally-distinct emitting states that do not interconvert during the S1 lifetime. These dynamics originate from photoexcitation of a mixed ground state population of acylimine hydrogen bond conformers. Strategically tuning the chromophore environment in TagRFP675 might stabilize the most red-shifted conformation and result in a variant with a larger Stokes shift.
Background: Decreased cerebral glucose metabolism has been reported in patients with sleep apnea syndrome (SAS), but it has yet to be decided whether cerebral glucose metabolism in SAS can be altered by continuous positive airway pressure (CPAP) treatment. Objective: The aim of this study was to evaluate cerebral glucose metabolism changes in patients with SAS after CPAP treatment. Methods: Thirteen middle-aged male patients with severe SAS [mean age 49.3 ± 7.2 years, mean apnea-hypopnea index (AHI) 60.4 ± 21.2] and 13 male controls (mean age 46.0 ± 9.4 years, mean AHI 4.1 ± 3.7) participated in the study. All 26 study subjects underwent fluorodeoxyglucose-positron emission tomography (FDG-PET), but SAS patients underwent FDG-PET twice, namely before and 3 months after acceptable CPAP usage. Results: Significant hypometabolism was observed in the bilateral prefrontal areas, left cuneus and left cingulate cortex of SAS patients before CPAP, and after CPAP, significant increases in cortical glucose metabolism were observed in the bilateral precentral gyri and left anterior cingulate cortex. However, these improvements in hypometabolism in both areas were insufficient to reach control levels, and hypometabolism in other regions persisted after CPAP treatment. Conclusions: Reduced cerebral glucose metabolism in the precentral gyrus and the cingulate cortex in patients with SAS was modestly improved by acceptable CPAP treatment. The findings of this study suggest that acceptable CPAP usage cannot completely reverse reduced cerebral glucose metabolism in SAS patients. Further studies are required to evaluate the long-term effects of CPAP treatment with total compliance.
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