High‐efficiency electromagnetic (EM) functional materials are the core building block of high‐performance EM absorbers and devices, and they are indispensable in various fields ranging from ...industrial manufacture to daily life, or even from national defense security to space exploration. Searching for high‐efficiency EM functional materials and realizing high‐performance EM devices remain great challenges. Herein, a simple solution‐process is developed to rapidly grow gram‐scale organic–inorganic (MAPbX3, X = Cl, Br, I) perovskite microcrystals. They exhibit excellent EM response in multi bands covering microwaves, visible light, and X‐rays. Among them, outstanding microwave absorption performance with multiple absorption bands can be achieved, and their intrinsic EM properties can be tuned by adjusting polar group. An ultra‐wideband bandpass filter with high suppression level of −71.8 dB in the stopband in the GHz band, self‐powered photodetectors with tunable broadband or narrowband photoresponse in the visible‐light band, and a self‐powered X‐ray detector with high sensitivity of 3560 µC Gyair−1 cm−2 in the X‐ray band are designed and realized by precisely regulating the physical features of perovskite and designing a novel planar device structure. These findings open a door toward developing high‐efficiency EM functional materials for realizing high‐performance EM absorbers and devices.
A facile one‐step solution processing method is developed to rapidly prepare gram‐scale MAPbX3 microcrystals. Utilizing its intrinsic electromagnetic (EM) properties, a series of EM devices is designed and fabricated, which can be applied in the fields of ultra‐wideband bandpass filters and multi‐band photodetection covering X‐rays, UV, visible light, and microwaves.
Abstract
Although chirality is an ever-present characteristic in biology and some artificial molecules, controlling the chirality and demystifying the chirality origin of complex assemblies remain ...challenging. Herein, we report two homochiral Ag
14
nanoclusters with inherent chirality originated from identical rotation of six square faces on a Ag
8
cube driven by intra-cluster π···π stacking interaction between pntp
−
(Hpntp =
p-
nitrothiophenol) ligands. The spontaneous resolution of the racemic (SD/
rac
-Ag14a) to homochiral nanoclusters (SD/
L
-Ag14 and SD/
R
-Ag14) can be realized by re-crystallizing SD/
rac
-Ag14a in acetonitrile, which promotes the homochiral crystallization in solid state by forming C–H···O/N hydrogen bonds with nitro oxygen atoms in pntp
−
or aromatic hydrogen atoms in dpph (dpph = 1,6-bis(diphenylphosphino)hexane) on Ag
14
nanocluster. This work not only provides strategic guidance for the syntheses of chiral silver nanoclusters in an all-achiral environment, but also deciphers the origin of chirality at molecular level by identifying the special effects of intra- and inter-cluster supramolecular interactions.
It remains unclear whether and how cardiomyocytes contribute to the inflammation in chronic heart failure (CHF). We recently reviewed the capacity of cardiomyocytes to initiate inflammation, by means ...of expressing certain immune receptors such as toll‐like receptors (TLRs) that respond to pathogen‐ and damage‐associated molecular patterns (PAMP and DAMP). Previous studies observed TLR4‐mediated inflammation within days of myocardial infarction (MI). This study examined TLR4 expression and function in cardiomyocytes of failing hearts after 4 weeks of MI in rats. The increases of TLR4 mRNA and proteins, as well as inflammatory cytokine production, were observed in both the infarct and remote myocardium. Enhanced immunostaining for TLR4 was observed in cardiomyocytes but not infiltrating leucocytes. The injection of lentivirus shRNA against TLR4 into the infarcted heart decreased inflammatory cytokine production and improved heart function in vivo. Accordingly, in cardiomyocytes isolated from CHF hearts, increases of TLR4 mRNA and proteins were detected. More robust binding of TLR4 with lipopolysaccharide (LPS), a PAMP ligand for TLR4, and heat shock protein 60 (HSP60), a DAMP ligand for TLR4, was observed in CHF cardiomyocytes under a confocal microscope. The maximum binding capacity (Bmax) of TLR4 was increased for LPS and HSP60, whereas the binding affinity (Kd) was not significantly changed. Furthermore, both LPS and HSP60 induced more robust production of inflammatory cytokines in CHF cardiomyocytes, which was reduced by TLR4‐blocking antibodies. We conclude that the expression, ligand‐binding capacity and pro‐inflammatory function of cardiomyocyte TLR4 are up‐regulated after long‐term MI, which promote inflammation and exacerbate heart failure.
Pleiotropic drug resistance (PDR) transporters belonging to the ABCG subfamily of ATP‐binding cassette (ABC) transporters are identified only in fungi and plants. Members of this family are expressed ...in plants in response to various biotic and abiotic stresses and transport a diverse array of molecules across membranes. Although their detailed transport mechanism is largely unknown, they play important roles in detoxification processes, preventing water loss, transport of phytohormones, and secondary metabolites. This review provides insights into transport mechanisms of plant PDR transporters, their expression profiles, and multitude functions in plants.
Rosidae, a clade of approximately 90 000 species of angiosperms, exhibits remarkable morphological diversity and extraordinary heterogeneity in habitats and life forms. Resolving phylogenetic ...relationships within Rosidae has been difficult, in large part due to nested radiations and the enormous size of the clade. Current estimates of phylogeny contain areas of poor resolution and/or support, and there have been few attempts to synthesize the available data into a comprehensive view of Rosidae phylogeny. We aim to improve understanding of the phylogeny of Rosidae with a dense sampling scheme using both newly generated sequences and data from GenBank of the chloroplast rbcL, atpB, and mark genes and the mitochondrial matR gene. We combined sequences from 9300 species, representing 2775 genera, 138 families, and 17 orders into a supermatrix. Although 59.26% of the cells in the supermatrix have no data, our results generally agree with previous estimates of Rosidae phylogeny and provide greater resolution and support in several areas of the topology. Several noteworthy phylogenetic relationships are recovered, including some novel relationships. Two families （Euphorbiaceae and Salvadoraceae） and 467 genera are recovered as non-monophyletic in our sampling, suggesting the need for future systematic studies of these groups. Our study shows the value of a botanically informed bioinformatics approach and dense taxonomic sampling for resolving rosid relationships. The resulting tree provides a starting point for large-scale analyses of the evolutionary patterns within Rosidae.
Structural modulation of core‐shell silver nanoclusters from the inside is a huge challenge but of great importance in their syntheses. Herein, two silver nanoclusters Ag3S9@Ag42 (SD/Ag45b) and ...Ag9S9@Ag42 (SD/Ag51a) are isolated in the presence of different kinds of sulfonic acids. Uniquely, SD/Ag45b and SD/Ag51a show typical core‐shell structures with the similar Ag42 shell but different cores. The outer shell of 42 silver atoms comprises two Ag3 trigons at two poles encircled by three equatorial distorted square cupolas (J4, Ag12). The core in SD/Ag45b is a silver trigon ligated by nine S2− ions (Ag3S9), while a tricapped triangular prismatic Ag9 also ligated by the same amount of S2− ions (Ag9S9) is observed in the inner core of SD/Ag51a. The electrospray ionization mass spectrometry (ESI‐MS) indicates that the introduction of p‐toluenesulfonic acid can realize the transformation from SD/Ag45b to Ag51. SD/Ag45b and SD/Ag51a show inverse luminescence thermochromic behaviors in the near‐infrared (NIR) region, mainly dictated by the inner silver cores. This work not only realizes the synthesis of new silver nanoclusters by core modulation but also provides a prototype to get molecular‐level insight into the correlation between structure and luminescence thermochromism.
SD/Ag45b and SD/Ag51a show typical core‐shell structures with similar Ag42 shell but different cores; the formation of different cores is dictated by the type of sulfonic acid. Two clusters exhibit inverse luminescence thermochromic behaviors in the near‐infrared (NIR) region upon cooling. The close correlation of structure and luminescence thermochromic behaviors in the silver nanocluster field is revealed.
Previous studies have shown that the addition of carboplatin to neoadjuvant chemotherapy improved the pathologic complete response (pCR) rate in patients suffering from triple‐negative breast cancer ...(TNBC) and patients who obtained a pCR could achieve prolonged event‐free survival (EFS) and overall survival (OS). However, no studies have assessed the effects of the combination of docetaxel and carboplatin without anthracycline with taxane‐based and anthracycline‐based regimens. The NeoCART study was designed as a multicenter, randomized controlled, open‐label, phase II trial to assess the efficacy and safety of docetaxel combined with carboplatin in untreated stage II‐III TNBC. All eligible patients were randomly assigned, at a 1:1 ratio, to an experimental docetaxel plus carboplatin (DCb) for six cycles group (DCb group) or an epirubicin plus cyclophosphamide for four cycles followed by docetaxel for four cycles group (EC‐D group). PCR (ypT0/is ypN0) was evaluated as the primary outcome. Between 1 September 2016 and 31 December 2019, 93 patients were randomly assigned and 88 patients were evaluated for the primary endpoint (44 patients in each group). In the primary endpoint analysis, 27 patients in the DCb group (61.4%, 95% CI 47.0‐75.8) and 17 patients in the EC‐D group achieved a pCR (38.6%, 95% CI 24.3‐53.0; odds ratio 2.52, 95% CI 2.4‐43.1; Pnoninferiority = .004). Noninferiority was met, and the DCb regimen was confirmed to be superior to the EC‐D regimen (P = .044, superiority margin of 5%). At the end of the 37‐month median follow‐up period, OS and EFS rates were equivalent in both groups.
What's new?
In triple‐negative breast cancer (TNBC), neoadjuvant chemotherapy based on anthracycline and taxane can improve survival, if pathologic complete response (pCR) is achieved. The addition of carboplatin to this neoadjuvant regimen for TNBC potentially improves pCR rate. The randomized trial reported here shows that, compared to a standard taxane‐ and anthracycline‐based regimen without carboplatin, pCR rate is significantly improved by combining docetaxel and carboplatin and leaving out anthracycline. Survival rates were similar between the different regimens. The findings suggest that docetaxel plus carboplatin is a promising alternative approach, particularly in TNBC patients who have a contraindication to treatment with an anthracycline.
The electronic properties, in particular, the occupation number of 5f electrons and the valence state of U ions in uranium sesquinitride (U
N
) are studied by using density functional theory (DFT) ...calculations merged with dynamical mean-field theory (DMFT). The results demonstrate that j=5/2 and j=7/2 manifolds are in the weakly correlated metallic and weakly correlated insulating regimes, respectively. The quasi-particle weights indicate that LS coupling scheme is more feasible for 5f electrons, which are not in the orbital-selective localized state. The weighted summation of the occupation probabilities of 5f
(n=0,1,2,3,4) atomic configurations suggests that 5f electrons have the inter-configuration fluctuation, or the mixed-valence state for U ions, together with an average occupation number of 5f electrons n
∼2.234, which is in good agreement with the electron localization function (ELF) and occupation analysis based on other DFT-based calculations. The 5f
-mixing-driven inter-configuration fluctuation might originate from the dual nature of 5f electrons, and the flexible electronic configuration of U ions. Finally, the so-called quasiparticle band structure is also discussed.
Adult Langerhans cell histiocytosis (LCH) remains poorly defined. We retrospectively studied 266 newly diagnosed LCH patients to understand the clinical presentation, treatment, and prognosis of ...adult LCH. The median age at diagnosis was 32 years (range, 18–79 years). At the time of diagnosis, 40 patients had single lesions within a single system, 18 patients had single pulmonary LCH, 26 patients had multiple lesions within a single system (SS‐m), and 182 patients had multisystem disease (MS). The most common organ involved in MS patients was the bone (69.8%), followed by the pituitary (61.5%) and lung (61.0%). BRAFV600E, BRAF deletion, and MAP2K1 mutation were detected in 38.8%, 25.4%, and 19.4% patients, respectively. BRAF deletion was found more common in patients with MS LCH compared to single‐system LCH (38.5% vs 7.1%, p = .004), also in patients with liver involvement (69.2% vs 14.3%, p < .001). The estimated 3‐year overall survival (OS) and event‐free survival (EFS) rates were 94.4% and 54.7%, respectively, in SS‐m and MS LCH. Multivariate Cox regression showed that involvement of the liver or spleen at baseline predicted poor EFS and receiving cytarabine‐based therapy as a first‐line treatment and age older than 30 years at diagnosis predicted favorable EFS. The involvement of risk organs and age older than 50 years predicted poor OS, and receiving cytarabine‐based therapy predicted favorable OS. Therefore, BRAF deletion was correlated with MS LCH, particularly those with liver involvement. Liver or spleen involvement at baseline indicates a poor prognosis, and a cytarabine‐based regimen could be considered as first‐line treatment for adult LCH patients.
Summary
Erdheim–Chester disease (ECD) is a rare form of non‐Langerhans cell histiocytosis that typically affects many organs, including the lung and pleura. However, there are few studies concerning ...pulmonary involvement in ECD patients, as well as the difference of pulmonary involvement between ECD and Langerhans cell histiocytosis (LCH). We performed a retrospective study of 54 ECD patients, and compared the pulmonary manifestations with those of adult LCH patients in our centre. The median age of diagnosis of the 54 ECD patients was 48 years (range 9–66 years). Chest computed tomography (CT) scans revealed lung involvement in 49 (91%) patients and pleural involvement in 34 (63%). Thirty‐three (61%) patients had interstitial lung disease (ILD) with varying degrees of interlobular septal thickening, micronodules, and ground‐glass opacities. ECD and LCH patients with pulmonary involvement showed significant differences in smoking status (P < 0·001), respiratory symptoms (P = 0·001) such as cough and pneumothorax (P < 0·001), and radiological findings, including cysts (P < 0·001), opacities (P < 0·001), and pleural thickening (P < 0·001). With a median follow‐up duration of 24 months (range, 1–84 months), the estimated three‐year overall survival (OS) of this entire ECD cohort was 90·2%. Patients with ILD tended to have worse progression‐free survival (PFS) than those with no ILD (P = 0·29).
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