Nonspecificity induces chiral specificity in the folding transition of giant DNA

The all-or-none type DNA folding transition from a coil to globule can be differentiated by the chirality of the triamines. The fluorescent microscope observation on single DNA molecules makes it clear that the tripeptides obtained from naturally occurring basic amino acids (l-lysine or l-arginine) can compact DNA molecules at concentrations lower than those from d-isomers. Nanometer-sized beads are found in the AFM images on the folded DNA molecule.     

Widely useful DMAP-catalyzed esterification under auxiliary base- and solvent-free conditions

With regard to atom economy and E-factor, catalytic condensation of carboxylic acids with equimolar amounts of alcohols is the most desirable. Although several highly active dehydration catalysts have been reported, more efficient alternatives are still strongly needed because the dehydrative esterification of tertiary alcohols, phenols, acid-sensitive alcohols, amino acids, and hardly soluble alcohols has never proceeded satisfactorily. Here we report new insights into the classical DMAP-catalyzed acylation of alcohols: surprisingly, only a 0.05-2 mol % of DMAP can efficiently promote acylation of alcohols with acid anhydrides under auxiliary base- and solvent-free conditions to give the corresponding esters in high yields. Furthermore, we achieved the recovery and reuse of commercially available polystyrene-supported DMAP without using any solvents. These serendipitous findings provide widely useful and environmentally benign esterification methods, which might be more practical and reliable than catalytic dehydrative condensation methods, in particular, for the less reactive alcohols which hardly condense with carboxylic acid directly.     

Molecular shape of palytoxin in aqueous solution

Palytoxin, one of the most toxic non-peptide substances, formed an associated dimer of 5 nm length in aqueous solution.     

Probability Distribution on Full Rooted Trees

The recursive and hierarchical structure of full rooted trees is applicable to statistical models in various fields, such as data compression, image processing, and machine learning. In most of these cases, the full rooted tree is not a random variable; as such, model selection to avoid overfitting is problematic. One method to solve this problem is to assume a prior distribution on the full rooted trees. This enables the optimal model selection based on Bayes decision theory. For example, by assigning a low prior probability to a complex model, the maximum a posteriori estimator prevents the selection of the complex one. Furthermore, we can average all the models weighted by their posteriors. In this paper, we propose a probability distribution on a set of full rooted trees. Its parametric representation is suitable for calculating the properties of our distribution using recursive functions, such as the mode, expectation, and posterior distribution. Although such distributions have been proposed in previous studies, they are only applicable to specific applications. Therefore, we extract their mathematically essential components and derive new generalized methods to calculate the expectation, posterior distribution, etc.     

Stochastic Model of Block Segmentation Based on Improper Quadtree and Optimal Code under the Bayes Criterion

Most previous studies on lossless image compression have focused on improving preprocessing functions to reduce the redundancy of pixel values in real images. However, we assumed stochastic generative models directly on pixel values and focused on achieving the theoretical limit of the assumed models. In this study, we proposed a stochastic model based on improper quadtrees. We theoretically derive the optimal code for the proposed model under the Bayes criterion. In general, Bayes-optimal codes require an exponential order of calculation with respect to the data lengths. However, we propose an algorithm that takes a polynomial order of calculation without losing optimality by assuming a novel prior distribution.     

Exact bounds on epsilon processes

In this paper we show that the lengths of the approximating processes in epsilon substitution method are calculable by ordinal recursions in an optimal way.     

Space-selective phase separation inside a glass by controlling compositional distribution with femtosecond-laser irradiation

Space-selective phase separation was induced inside Na₂O–SiO₂ glasses by changing the glass composition locally from a miscible composition to an immiscible one via femtosecond-laser irradiation at a high repetition rate. The formation of a nanoscale co-continuous structure due to phase separation was confirmed by scanning electron microscopy after heat treatment, polishing until the laser-modified area was exposed, and subsequent etching. The configuration of the structure could be controlled by changing the heat-treatment time.     

Sequence-specific alkylation of double-strand human telomere repeat sequence by pyrrole-imidazole polyamides with indole linkers

We designed and synthesized pyrrole (Py)-imidazole (Im) hairpin polyamide 1-(chloromethyl)-5-hydroxy-1,2-dihydro-3H-benz[e]indole (seco-CBI) conjugates 1 and 2, which target both strands of the double-stranded region of the human telomere repeat sequences, 5'-d(TTAGGG)(n)-3'/5'-d(CCCTAA)(n)-3'. High-resolution denaturing polyacrylamide gel electrophoresis demonstrated that conjugates 1 and 2 alkylated DNA at the 3' A of 5'-ACCCTA-3' and 5'-AGGGTTA-3', respectively. Cytotoxicities of conjugates 1 and 2 were evaluated using 39 human cancer cell lines; averages of log IC(50) values for conjugates 1 and 2 were -6.96 (110 nM) and -7.24 (57.5 nM), respectively. Conjugates 1 and 2 have potential as antitumor drugs capable of targeting telomere repeat sequence.     

Simultaneous tailoring of phase evolution and dopant distribution in the glassy phase for controllable luminescence

Construction of an active composite with multicolor visible and broadband near-infrared luminescence is of great technological importance for various applications, including three-dimensional (3D) display, broadband telecommunication, and tunable lasers. The major challenge is the effective management of energy transfer between different dopants in composite. Here we present an in situ strategy for controlling energy transfer between multiple active centers via simultaneous tailoring of the evolution of phases and the distribution of dopants in the glassy phase. We show that the orderly precipitation of Ga(2)O(3) and LaF(3) nanocrystals and the selective incorporation of Ni(2+) and Er(3+) into them can be achieved. The obtained composite shows unique multicolor visible and broadband near-infrared emission. Possible mechanisms for the selective doping phenomenon are proposed, based on thorough structural and optical characterizations and crystal-field calculation results. Moreover, the strategy can be successfully extended to accomplish space-selective control of multicolor luminescence by employing the modulated stimulation field. The results suggest that the strategy could be applied to fabricate a multifunctional light source with a broad range of important host/activator combinations and to construct various types of three-dimensional active microstructures.