Completely understanding the working mechanisms of sophisticated supramolecular self-assembly exhibiting competing paths is very important for chemists en route to acquiring the ability of constructing supramolecular systems with controlled structures and designed functions. Here, the self-aggregation behaviors of an N-heterocyclic aromatic dicarboximide molecule 1, boasting two competing paths that give rise to different supramolecular structures and exhibit distinct thermodynamic features, are carefully examined. First, a group of H-aggregates are observed when providing a medium driving force for aromatic stacking, and their formation is manifested as an anticooperative process. When exposed to enhanced strength of aromatic interactions, these H-aggregates are found to transform into J-aggregates via a cooperative assembly mechanism. With the assistance of a mathematic model accommodating two competing polymerization pathways, calculations are conducted to simulate and explain the thermodynamic equilibria of such a unique supramolecular system. The calculation results are highly consistent with the experimental observations, and some important properties are elucidated. Specifically, the anticooperative assembly mechanism generally promotes the formation of low to medium oligomers, whereas the cooperative path is more competent at producing high polymers. If the anticooperative and cooperative routes coexist and compete for the same molecule, the cooperative formations of high polymers are significantly suppressed unless a very high degree of polymerization can be achieved. Such a unique feature of concurring anticooperative and cooperative paths emerges to the H- and J-aggregates of molecule 1 and thus brings about the interesting sequential appearances of the two types of aggregates under conditions of continuously enlarged driving force for self-aggregation. Finally, based on the knowledge acquired from this study and by analyzing the steric features of 1 that influence its supramolecular packing motifs, a slightly modified molecular structure is designed, with which the intermediate H-aggregation state was successfully suppressed, and a single cooperative J-aggregation path is manifested.
Nanoelectronic devices with specifically designed structures for performance promotion or function expansion are of great interest, aiming for diversified advanced nanoelectronic systems. In this work, we report a dual-material gate (DMG) carbon nanotube (CNT) device with multiple functions, which can be configured either as a high-performance p-type field-effect transistor (FET) or a diode by changing the input manners of the device. When operating as a FET, the device exhibits a large current on/off ratio of more than 108 and a drain-induced barrier lowering of 97.3 mV V−1. When configured as a diode, the rectification ratio of the device can be greater than 105. We then demonstrate configurable analog and digital integrated circuits that are enabled by utilizing these devices. The configurability enables the realization of transformable functions in a single device or circuits, which gives future electronic systems the flexibility to adapt to the diverse requirements of their applications and/or ever-changing operating environments.
Worldwide there has been deterioration of lakeshore habitat and increasing eutrophication. These stresses have impacted littoral macroinvertebrate communities. However, bioassessment and rehabilitation have been largely carried out offshore, and the inshore macroinvertebrates have received less attention especially in shallow plateau lakes. In this study, we compared inshore and offshore macroinvertebrate communities in a shallow plateau lake, Lake Dianchi, China. The environmental parameters determining the distribution of macroinvertebrates were analyzed with partial redundancy analysis. Our results showed that macroinvertebrate communities differed significantly between inshore and offshore. Taxonomic richness was much higher inshore than offshore, due to higher habitat heterogeneity. By contrast, both density and biomass inshore were significantly lower than those of offshore. Generally, vegetation and substrate type were the key environmental parameters shaping macroinvertebrate communities. Eutrophication exerted great effect on offshore communities, while its impacts on inshore communities varied spatially. Shoreline degradation and seasonal eutrophication effects resulted in the limited density and biomass of inshore communities. Our results emphasized the significance of inshore habitats for macroinvertebrates in Lake Dianchi, and provided important implications for bioassessment and ecological rehabilitation in shallow lakes.
Background: Change in the prevalence of raised blood pressure could be due to both shifts in the entire distribution of blood pressure (representing the combined effects of public health interventions and secular trends) and changes in its high-blood-pressure tail (representing successful clinical interventions to control blood pressure in the hypertensive population). Our aim was to quantify the contributions of these two phenomena to the worldwide trends in the prevalence of raised blood pressure.
Methods: We pooled 1018 population-based studies with blood pressure measurements on 88.6 million participants from 1985 to 2016. We first calculated mean systolic blood pressure (SBP), mean diastolic blood pressure (DBP) and prevalence of raised blood pressure by sex and 10-year age group from 20-29 years to 70-79 years in each study, taking into account complex survey design and survey sample weights, where relevant. We used a linear mixed effect model to quantify the association between (probit-transformed) prevalence of raised blood pressure and age-group- and sex-specific mean blood pressure. We calculated the contributions of change in mean SBP and DBP, and of change in the prevalence-mean association, to the change in prevalence of raised blood pressure.
Results: In 2005-16, at the same level of population mean SBP and DBP, men and women in South Asia and in Central Asia, the Middle East and North Africa would have the highest prevalence of raised blood pressure, and men and women in the high-income Asia Pacific and high-income Western regions would have the lowest. In most region-sex-age groups where the prevalence of raised blood pressure declined, one half or more of the decline was due to the decline in mean blood pressure. Where prevalence of raised blood pressure has increased, the change was entirely driven by increasing mean blood pressure, offset partly by the change in the prevalence-mean association.
Conclusions: Change in mean blood pressure is the main driver of the worldwide change in the prevalence of raised blood pressure, but change in the high-blood-pressure tail of the distribution has also contributed to the change in prevalence, especially in older age groups.
Background: Change in the prevalence of raised blood pressure could be due to both shifts in the entire distribution of blood pressure (representing the combined effects of public health interventions and secular trends) and changes in its high-blood-pressure tail (representing successful clinical interventions to control blood pressure in the hypertensive population). Our aim was to quantify the contributions of these two phenomena to the worldwide trends in the prevalence of raised blood pressure. Methods: We pooled 1018 population-based studies with blood pressure measurements on 88.6 million participants from 1985 to 2016. We first calculated mean systolic blood pressure (SBP), mean diastolic blood pressure (DBP) and prevalence of raised blood pressure by sex and 10-year age group from 20-29 years to 70-79 years in each study, taking into account complex survey design and survey sample weights, where relevant. We used a linear mixed effect model to quantify the association between (probit-transformed) prevalence of raised blood pressure and age-group-and sex-specific mean blood pressure. We calculated the contributions of change in mean SBP and DBP, and of change in the prevalence-mean association, to the change in prevalence of raised blood pressure. Results: In 2005-16, at the same level of population mean SBP and DBP, men and women in South Asia and in Central Asia, the Middle East and North Africa would have the highest prevalence of raised blood pressure, and men and women in the high-income Asia Pacific and high-income Western regions would have the lowest. In most region-sex-age groups where the prevalence of raised blood pressure declined, one half or more of the decline was due to the decline in mean blood pressure. Where prevalence of raised blood pressure has increased, the change was entirely driven by increasing mean blood pressure, offset partly by the change in the prevalence-mean association. Conclusions: Change in mean blood pressure is the main driver of the worldwide change in the prevalence of raised blood pressure, but change in the high-blood-pressure tail of the distribution has also contributed to the change in prevalence, especially in older age groups.
Gyrotron performance is sensitive to cavity structure parameters, and the cavity shape is temperature dependent due to thermal deformation induced by temperature rise from ohmic loss power on finite-conductivity cavity wall. Accordingly, this paper studies a frequency-tuning scheme for terahertz gyrotron by properly controlling the cavity thermal deformation. By combining gyrotron nonlinear theory and finite-element method software, controllable thermal-frequency-tuning capability of a continuous-wave 263-GHz gyrotron is systematically investigated, toward maintaining gyrotron operating under gyromonotron condition in frequency-tuning band, and achieving high efficiency in broadband frequency-tuning range. After studying cavity thermal distribution, structure deformation, and electron beam-wave interaction, an optimized cavity structure with transition sections on both ends is proposed. Simulation predicts that with the two-transition-section cavity, via additional thermal tuning, the continuous-frequency-tuning band is capable of reaching 1.75 GHz, which is 5 times of the initial bandwidth. Furthermore, using the thermal-frequency-tuning technology, impressive high efficiency above 17% is obtainable in the whole frequency-tuning range.
