Molecular components are vital to introduce and manipulate quantum interference (QI) in charge transport through molecular electronic devices. Up to now, the functional molecular units that show QI are mostly found in conventional π‐ and σ‐bond‐based systems; it is thus intriguing to study QI in multicenter bonding systems without both π‐ and σ‐conjugations. Now the presence of QI in multicenter‐bond‐based systems is demonstrated for the first time, through the single‐molecule conductance investigation of carborane junctions. We find that all the three connectivities in carborane frameworks show different levels of destructive QI, which leads to highly suppressed single‐molecule conductance in para‐ and meta‐connected carboranes. The investigation of QI into carboranes provides a promising platform to fabricate molecular electronic devices based on multicenter bonds.
The single-molecule break junction technique provides a high-throughput method to explore the charge transport phenomena through a molecular junction at the ultimate scale of a single molecule. The most probable conductance of a molecular junction is normally extracted from histogram generated from repeated and massive break junction data. However, this conventional data analysis method only exhibits general charge transport properties of molecular junctions, and insightful information hidden in those recorded data remains unexplored. Among them, some of the conductance variations corresponding to different molecular junction conformations that occur during the break junction process might easily be overlooked. To accurately extract those hidden events, here we demonstrated a customized spectral clustering method with the evaluation of the Calinski–Harabasz index, which could be employed to analyze a large amount of data and to automatically extract different molecular junction conformations without subjective bias. Our approach was first validated through simulated data sets and was confirmed to be suitable for the product analysis during a chemical reaction. Moreover, using this method, an easily overlooked but unignorable junction conformation was found during the carborane molecular junction measurement, suggesting that spectral clustering with the Calinski–Harabasz index as a criterion offers a promising algorithm for junction conformation analysis in massive break junction data.
In this transcultural study of schizophrenic delusions among Koreans, Korean-Chinese and Chinese, many delusions were shown to be different among the three groups in their frequency and content and the differences could be explained by sociocultural and political factors. Delusional themes sensitive to influence by sociocultural or political situations and changes seem to be 'family', 'love affairs', 'religious matters', 'economic matters', 'specific physical damage' and 'political themes.' Delusions about 'family', 'love affair', 'being raped', 'religious matters' and 'economic and business matters' were most frequent in Koreans. Delusions of 'blood-relatedness', 'longevity' and 'political themes' were most frequent in Korean-Chinese. Delusions of 'bloodsucking and brain or viscera extracted' and 'poison or being pricked by poisoned needle' were most prominent in Chinese.
The sensing platform based on single-molecule measurements provides a new perspective for constructing ultrasensitive systems. However, most of these sensing platforms are unavailable for the accurate determination of target analytes. Herein, we demonstrate a conductance ratiometric strategy combing with the single-molecule conductance techniques for ultrasensitive and precise determination. A single-molecule sensing platform was constructed with the 3,3′,5,5′-tetramethylbenzidine (TMB) and oxidized TMB (oxTMB) as the conductance ratiometric probes, which was applied in the detection of Ag[I] and nicotinamide adenine dinucleotide (NADH). It was found that the charge transport properties of TMB and oxTMB were distinct with more than an order of magnitude change of the conductance, thus enabling conductance ratiometric analysis of the Ag[I] and NADH in the real samples. The proposed method is ultrasensitive and has an anti-interference ability in the complicated matrix. The limit of detection can be as low as attomolar concentrations (∼34 aM). We believe that the proposed conductance ratiometric approach is generally enough to have a promising potential for broad and complicated analysis.
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