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e., without involving the Pauli exchange repulsion, which is taken into account in the conventional theories of physical adsorption. The results obtained provide a fresh insight into the physics of adsorption in physical electronics, chemical physics, and electrochemistry.Controlling self-organization in precipitation reactions has received growing attention in the efforts of engineering highly ordered spatial structures. Experiments have been successful in regulating the band patterns of the Liesegang phenomenon on various scales. Herein, we show that by adjusting the composition of the hydrogel medium, we can switch the final pattern between the classical band structure and the rare precipitate spots with hexagonal symmetry. The accompanying modeling study reveals that besides the modification of gel property, tuning of the time scale of diffusional spreading of hydroxide ions with respect to that of the phase separation drives the mode selection between one-dimensional band and two-dimensional spot patterns.Multireference computations of large-scale chemical systems are typically limited by the computational cost of quantum chemistry methods. In this work, we develop a zeroth-order active space embedding theory [ASET(0)], a simple and automatic approach for embedding any multireference dynamical correlation method based on a frozen-orbital treatment of the environment. ASET(0) is combined with the second-order multireference driven similarity renormalization group and tested on several benchmark problems, including the excitation energy of 1-octene and bond-breaking in ethane and pentyldiazene. Finally, we apply ASET(0) to study the singlet-triplet gap of p-benzyne and 9,10-anthracyne diradicals adsorbed on a NaCl surface. Our results show that despite its simplicity, ASET(0) is a powerful and sufficiently accurate embedding scheme applicable when the coupling between the fragment and the environment is in the weak to medium regime.We present a simple yet powerful synthesis process to prepare compound-phase perovskite nanoparticles (MAPbX3-nY n ; MA = CH3NH3+ and X/Y = I, Br, or Cl). This is achieved by mixing two pure-phase perovskites (MAPbX3 and MAPbY3) by using ultrasonic vibration as a mechanochemical excitation. Unlike conventional methods, this procedure does not require any effort in designing a reaction or choosing any particular precursor. X-ray diffraction and TEM studies confirm compound-phase formation in all possible stoichiometries. The origin behind ultrasonic mixing lies in the generation of mechanical stress and high temperature arising from acoustic cavitation during reaction. Long-term experimental stability of the compound-phase is comprehended theoretically by simulating the temperature-dependent Gibbs free energy. Negative mixing entropy plays a crucial role during the synthesis which leads to better stabilization of the compound-phase perovskite over the pure-phase. The ease of synthesis and remarkable phase stability make this process effective and less cumbersome for perovskite nanoparticle synthesis.A [3 + 2] cycloaddition reaction of unstable difluoromethylphosphonate-containing diazoalkanes with vinyl sulfones under simple reaction conditions is developed, which provides an efficient route toward functionalized fluorinated pyrazolines derivatives in good chemical yields. The difluoro diazoalkanes are generated in situ using t-BuONO for the diazotization of (β-amino-α,α-difluoroethyl)phosphonates, and their stabilities and reactivities were carefully investigated.The regio- and enantioselective allylic substitution of branched alkyl-substituted allylic acetates employing malonates has been achieved through a process that calls for Krische's π-allyliridium C,O-benzoate catalyst. The protocol reported herein can be applied to a diverse set of branched alkyl substrates that are generally not well tolerated in the other two types of Ir-catalyzed allylation.Most oligonucleotides fail to enter a cell and cannot escape from endosomes after endocytosis because of their negative charge and large molecular weight. More efficient cellular delivery of oligonucleotides should be developed for the widespread implementation of antisense imaging. The purpose of this study was to construct a novel antisense nanoprobe, 99mTc-labeled anti-miRNA oligonucleotides/cell-penetrating peptide PepFect6 (99mTc-AMO/PF6), and to evaluate its efficacy for imaging the miRNA-21 expression in A549 lung adenocarcinoma xenografts. Naked AMO and commercial Lipofectamine 2000-based nanoparticles (AMO/LIP) were used for comparison. The cellular delivery efficiency of AMO/PF6 was first investigated by laser confocal scanning microscopy using Cy5.5-labeled probes and further validated by in vivo fluorescence imaging. Then, the probes were labeled with 99mTc via hydrazinonicotinamide (HYNIC). The cytotoxicity assay, cellular uptake, and retention kinetics of the probes were evaluated in vitro. The he kidneys and the liver. The results of in vivo fluorescence and SPECT imaging were consistent with the results of the biodistribution. The tumor was visualized at 6 h after injection of AMO/PF6 with the highest T/M ratio among these probes (P less then 0.05). PF6 improves cellular delivery of antisense oligonucleotides via noncovalent nanoparticles. 99mTc-AMO/PF6 shows favorable imaging properties and is promising for miRNAs imaging in vivo.An all-inorganic lead-free halides Cs-Cu-I system, represented by Cs3Cu2I5 and CsCu2I3, has attracted attention for their good photophysical characteristics recently. Successive works had reported their application potential in light-emitting devices. learn more However, there is no report for CsCu2I3 in X-ray scintillation detectors so far. We notice that CsCu2I3 may be advantageous in such an application due to the one-dimensional crystal structure, the congruent-melting feature, and the high spectral matching to some photosensors. In this work, we explore the scintillation properties and imaging application of CsCu2I3 in X-ray scintillator detector. The oriented structure is designed to enhance the imaging performance of a CsCu2I3 detector. Close-space sublimation process and nanoscale seed screening strategy are employed to realize this design by producing a large-area (25 cm2) CsCu2I3 thick film layer with the oriented nanorod structure. This CsCu2I3 detector eventually achieves a high spatial resolution of 7.5 lp mm-1 in X-ray imaging.