Self-deprotonation and colorization of 1,3-bis(dicyanomethylidene)indan in polar media: a facile route to a minimal polymethine dye for NIR fluorescence imaging

Colorless 1,3-bis(dicyanomethylidene)indan is an organic acid (pK(a) ≈3.0) that turns blue in polar media owing to self-deprotonation. Moreover, its colored conjugate base shows potential as a minimal anionic polymethine dye for probing biomolecules in cells and in vivo through noncovalent complexation and near-infrared fluorescence signaling.     

Surface-enhanced Raman scattering of 4,4'-dimercaptoazobenzene trapped in Au nanogaps

The surface-enhanced Raman scattering (SERS) of 4,4'-dimercaptoazobenzene (4,4'-DMAB), an alpha, omega-dithiol possessing also an azo moiety, has seen a surge of interest recently, since 4,4'-DMAB might be able to form from 4-aminobenzenethiol (4-ABT) via a surface-induced photoreaction. An understanding of the intrinsic SERS characteristics of 4,4'-DMAB is thus very important to evaluate the possibility of such a photoreaction. We found in this work that 4,4'-DMAB should adsorb on a flame-annealed Au substrate via one of its two thiol groups such that Au nanoparticles could adsorb further on the pendent thiol group, forming a SERS hot site. The most distinctive feature in the SERS of 4,4'-DMAB was the appearance of a(g) bands, which were quite similar to the b(2)-type bands occurring in the SERS of 4-ABT. In an electrochemical environment, the a(g) bands of 4,4'-DMAB at 1431, 1387, and 1138 cm(-1) became weakened at lower potentials, completely disappearing at -1.0 V, but the bands were restored upon increasing the electrode potential, implying that neither electro- nor photo-chemical reaction to break the azo group took place, in agreement with data from a cyclic voltammogram. The appearance and disappearance of these a(g) bands are thus concluded to be associated with the charge transfer phenomenon: 4,4'-DMAB must then be one of a unique group of compounds exhibiting chemical enhancement when subjected to a SERS environment.     

SSA-MOA: a novel CTC isolation platform using selective size amplification (SSA) and a multi-obstacle architecture (MOA) filter

Circulating tumor cells (CTCs) have gained increasing attention as physicians and scientists learn more about the role these extraordinarily rare cells play in metastatic cancer. In developing CTC technology, the critical criteria are high recovery rates and high purity. Current isolation methods suffer from an inherent trade-off between these two goals. Moreover, ensuring minimal cell stress and robust reproducibility is also important for the clinical application of CTCs. In this paper, we introduce a novel CTC isolation technology using selective size amplification (SSA) for target cells and a multi-obstacle architecture (MOA) filter to overcome this trade-off, improving both recovery rate and purity. We also demonstrate SSA-MOA's advantages in minimizing cell deformation during filter transit, resulting in more stable and robust CTC isolation. In this technique, polymer microbeads conjugated with anti-epithelial cell adhesion molecules (anti-EpCAM) were used to selectively size-amplify MCF-7 breast cancer cells, definitively differentiating from the white blood cells (WBCs) by avoiding the size overlap that compromises other size selection methods. 3 μm was determined to be the optimal microbead diameter, not only for size discrimination but also in maximizing CTC surface coverage. A multi-obstacle architecture filter was fabricated using silicon-on-glass (SOG) technology-a first such application of this fabrication technique-to create a precise microfilter structure with a high aspect ratio. The filter was designed to minimize cell deformation as simulation results predicted that cells captured via this MOA filter would experience 22% less moving force than with a single-obstacle architecture. This was verified by experiments, as we observed reliable cell capture and reduced cell deformation, with a 92% average recovery rate and 351 peripheral blood leukocytes (PBL) per millilitre (average). We expect the SSA-MOA platform to optimize CTC recovery rates, purity, and stability, increasing the sensitivity and reliability of such tests, thereby potentially expanding the utilization of CTC technologies in the clinic.     

Highly fluorescent chameleon nanoparticles and polymer films: multicomponent organic systems that combine FRET and photochromic switching

We describe the preparation of highly efficient stimulus-responsive fluorescence color-tuning in self-assembled supramolecular scaffold systems. The systems consisted of a photochromic compound (BP-BTE) in combination with unique luminescent organic materials (CN-MBE, TPS-CNMBE, TPA-2CNMBE) that exhibited intense fluorescence in the solid state. The emission spectrum was tuned by introducing fluorescence resonance energy transfer and photochromic switching capabilities into the system. The materials were used to successfully demonstrate novel fluorescence patterns that were responsive to multiple stimuli, displayed reversible fluorescence switching, and provided a nondestructive readout of the fluorescence signal.     

Optimal Wloc2,2-regularity,Pohozhaevʼs identity,and nonexistence of weak solutions to some quasilinear elliptic equations

We begin by establishing a sharp (optimal) $W_{\mathrm{loc}}^{2,2}$-regularity result for bounded weak solutions to a nonlinear elliptic equation with the p-Laplacian, ${\mathrm{\Delta }}_{p}u\stackrel{\mathrm{def}}{=}\mathrm{div}({|\mathrm{?}u|}^{p?2}\mathrm{?}u)$, $1<p<\infty$. We develop very precise, optimal regularity estimates on the ellipticity of this degenerate (for $2<p<\infty$) or singular (for $1<p<2$) problem. We apply this regularity result to prove Pohozhaev?s identity for a weak solution $u\in W^{1,p}(\Omega )$ of the elliptic Neumann problem(P)$?{\mathrm{\Delta }}_{p}u+W^{\prime }(u)=f(x)\text{in}\Omega ;?u/?\nu =0\text{on}?\Omega .$ Here, Ω is a bounded domain in ${\mathbb{R}}^N$ whose boundary ?Ω is a $C^2$-manifold, $\nu \equiv \nu (x_0)$ denotes the outer unit normal to ?Ω at $x_0\in ?\Omega$, $x=(x_1,\dots ,x_N)$ is a generic point in Ω, and $f\in L^{\infty }(\Omega )\cap W^{1,1}(\Omega )$. The potential $W:\mathbb{R}\to \mathbb{R}$ is assumed to be of class $C^1$ and of the typical double-well shape of type $W(s)={|1?{|s|}^{\beta }|}^{\alpha }$ for $s\in \mathbb{R}$, where $\alpha ,\beta >1$ are some constants. Finally, we take an advantage of the Pohozhaev identity to show that problem (P) with $f\equiv 0$ in Ω has no phase transition solution $u\in W^{1,p}(\Omega )$ ($1<p?N$), such that $?1?u?1$ in Ω with $u\equiv ?1$ in ${\Omega }_{?1}$ and $u\equiv 1$ in ${\Omega }_1$, where both ${\Omega }_{?1}$ and ${\Omega }_1$ are some nonempty subdomains of Ω. Such a scenario for u is possible only if $N=1$ and ${\Omega }_{?1}$, ${\Omega }_1$ are finite unions of suitable subintervals of the open interval $\Omega ?{\mathbb{R}}^1$.     

Surface characteristics of Ag‐doped Au nanoparticles probed by Raman scattering spectroscopy

We have examined the surface characteristics of Ag‐doped Au nanoparticles (below 5 mol% of Ag) by means of the surface‐enhanced Raman scattering (SERS) of 2,6‐dimethylphenylisocyanide (2,6‐DMPI) and 4‐nitrobenzenethiol (4‐NBT). When Ag was added to Au to form ∼35‐nm‐sized alloy nanoparticles, the surface plasmon resonance band was blue‐shifted linearly from 523 to 517 nm in proportion to the content of Ag up to 5%. In the SERS spectra of 2,6‐DMPI, the N‐C stretching peak also shifted almost linearly from 2184 to 2174 cm⁻¹ when the Ag content was 5 mol% or less; the peak then remained the same as that of the pure Ag film. The potential variation of the SERS spectrum of 2,6‐DMPI in an electrochemical environment, as well as the effect of organic vapor, also showed a similar tendency. From the SERS of 4‐NBT, we confirmed the occurrence of a surface‐induced photoreaction converting 4‐NBT to 4‐aminobenzenethiol, when Ag was added to Au to form alloy nanoparticles. The photoreaction induction ability also increased linearly with the Ag content, reaching a plateau level at 5 mol% of Ag. All these observations suggest that the surface content of Ag should increase almost linearly as a function of the overall mole fraction of Ag and, once the Au/Ag nanoparticles reach 5 mol% of Ag, their surfaces are fully covered with Ag, showing the same surface characteristics of pure Ag nanoparticles. Copyright © 2011 John Wiley & Sons, Ltd.     

Surface potential variation of gold nanoparticles by organic vapors revealed by Raman scattering of 1,4‐phenylenediisocyanide

The NC stretching frequency in the potential‐dependent surface‐enhanced Raman scattering spectrum of 1,4‐phenylenediisocyanide (1,4‐PDI) is very sensitive to the electrode potential, and much the same peak shift is observed when an Au nanoparticle with mean diameter from 16 to 90 nm attached to 1,4‐PDI‐adsorbed gold nanogap system is exposed solely to organic vapors. This leads us to conclude that the surface potential of Au nanoparticles should change by as much as +0.57 and −0.34 V, respectively, in the presence of CCl₄ and NH₃ because of their respective electron‐withdrawing and electron‐donating properties, regardless of the size of Au nanoparticles in the gold nanogap system. Copyright © 2012 John Wiley & Sons, Ltd.     

Primordial curvature perturbation during and at the end of multi-field inflation

We study the generation of the primordial curvature perturbation in multi-field inflation. Considering both the evolution of the perturbation during inflation and the effects generated at the end of inflation, we present a general formula for the curvature perturbation. We provide the analytic expressions of the power spectrum, spectral tilt and non-Gaussianity for the separable potentials of two inflaton scalars, and apply them to some specific models.     

Multichannel transceiver dual-tuned RF coil for proton/sodium MR imaging of knee cartilage at 3 T

Sodium magnetic resonance (MR) imaging is a promising technique for detecting changes of proteoglycan (PG) content in cartilage associated with knee osteoarthritis. Despite its potential clinical benefit, sodium MR imaging in vivo is challenging because of intrinsically low sodium concentration and low MR signal sensitivity. Some of the challenges in sodium MR imaging may be eliminated by the use of a high-sensitivity radiofrequency (RF) coil, specifically, a dual-tuned (DT) proton/sodium RF coil which facilitates the co-registration of sodium and proton MR images and the evaluation of both physiochemical and structural properties of knee cartilage. Nevertheless, implementation of a DT proton/sodium RF coil is technically difficult because of the coupling effect between the coil elements (particularly at high field) and the required compact design with improved coil sensitivity. In this study, we applied a multitransceiver RF coil design to develop a DT proton/sodium coil for knee cartilage imaging at 3 T. With the new design, the size of the coil was minimized, and a high signal-to-noise ratio (SNR) was achieved. DT coil exhibited high levels of reflection S11 (～-21 dB) and transmission coefficient S12 (～-19 dB) for both the proton and sodium coils. High SNR (range 27-38) and contrast-to-noise ratio (CNR) (range 15-21) were achieved in sodium MR imaging of knee cartilage in vivo at 3-mm(3) isotropic resolution. This DT coil performance was comparable to that measured using a sodium-only birdcage coil (SNR of 28 and CNR of 20). Clinical evaluation of the DT coil on four normal subjects demonstrated a consistent acquisition of high-resolution proton images and measurement of relative sodium concentrations of knee cartilages without repositioning of the subjects during the same MR scanning session.