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This study aims to identify dynamic patterns within the spatiotemporal feature space that are specific to nonpsychotic major depression (NPMD), psychotic major depression (PMD), and schizophrenia (SCZ). The study also evaluates the effectiveness of machine learning algorithms based on these network manifestations in differentiating individuals with NPMD, PMD, and SCZ. A total of 579 participants were recruited, including 152 patients with NPMD, 45 patients with PMD, 185 patients with SCZ, and 197 healthy controls (HCs). A dynamic functional connectivity (DFC) approach was employed to estimate the principal FC states within each diagnostic group. Incremental proportions of data (ranging from 10% to 100%) within each diagnostic group were used for variability testing. DFC metrics, such as proportion, mean duration, and transition number, were examined among the four diagnostic groups to identify disease-related neural activity patterns. These patterns were then used to train a two-layer classifier for the four groups (HC, NPMD, PMD, and SCZ). The four principal brain states (i.e., states 1,2,3, and 4) identified by the DFC approach were highly representative within and across diagnostic groups. Between-group comparisons revealed significant differences in network metrics of state 2 and state 3, within delta, theta, and gamma frequency bands, between healthy individuals and patients in each diagnostic group (p< 0.01, FDR corrected). Moreover, the identified key dynamic network metrics achieved an accuracy of 73.1 ± 2.8% in the four-way classification of HC, NPMD, PMD, and SCZ, outperforming the static functional connectivity (SFC) approach (p< 0.001). These findings suggest that the proposed DFC approach can identify dynamic network biomarkers at the single-subject level. These biomarkers have the potential to accurately differentiate individual subjects among various diagnostic groups of psychiatric disorders or healthy controls. This work may contribute to the development of a valuable EEG-based diagnostic tool with enhanced accuracy and assistive capabilities.

Metal whisker growth poses a significant reliability threat to electronic devices. Previous investigations have predominantly focused on metal platings and alloy solder samples, yet the intricate factors involved have yielded inconsistent comprehension of the phenomenon. To achieve a comprehensive understanding, exploring intermetallic compounds (IMCs) may offer a novel standpoint. Herein, we present the first report on the growth of single crystal cadmium (Cd) whiskers on Ti2Cd IMC, accompanied by the characterization of their composition, crystal structure, and morphological features. Furthermore, the influence of mechanical damage and temperature on the whisker growth is examined. Ball milling induces the decomposition of Ti2Cd, liberating active Cd atoms with elevated chemical potentials that consequently feed the whisker growth. These findings augment the existing knowledge on the topic of the metal whisker growth and provide fresh perspectives and references for further investigations in this field.

Introduction: Unbiased metagenomic next-generation sequencing (mNGS) has been used for infection diagnosis. In this study, we explored the clinical diagnosis value of mNGS for pulmonary complications after allogeneic hematopoietic stem cell transplantation (allo-HSCT). Methods: From August 2019 to June 2021, a prospective study was performed to comparatively analyze the pathogenic results of mNGS and conventional tests for bronchoalveolar lavage fluid (BALF) from 134 cases involving 101 patients with pulmonary complications after allo-HSCT. Results: More pathogens were identified by mNGS than with conventional tests (226 vs 120). For bacteria, the diagnostic sensitivity (P= 0.144) and specificity (P= 0.687) were similar between the two methods. For fungus except Pneumocystis jirovecii(PJ), conventional tests had a significantly higher sensitivity (P= 0.013) with a similarly high specificity (P= 0.109). The sensitivities for bacteria and fungi could be increased with the combination of the two methods. As for PJ, both the sensitivity (100%) and specificity (99.12%) of mNGS were very high. For viruses, the sensitivity of mNGS was significantly higher (P= 0.021) and the negative predictive value (NPV) was 95.74% (84.27–99.26%). Pulmonary infection complications accounted for 90.30% and bacterium was the most common pathogen whether in single infection (63.43%) or mixed infection (81.08%). The 6-month overall survival (OS) of 88.89% in the early group (mNGS ≤ 7 days) was significantly higher than that of 65.52% (HR 0.287, 95% CI 0.101–0.819, P= 0.006) in the late group (mNGS > 7 days). Conclusions: mNGS for BALF could facilitate accurate and fast diagnosis for pulmonary complications. Early mNGS could improve the prognosis of patients with pulmonary complications after allo-HSCT. Trial Registration: ClinicalTrials.gov identifier, NCT 04051372.

•High-performance as-cast OSCs could be achieved by a simple alkyl-modified strategy.•Based on as-cast PM6:Y6-eC6-BO OSCs processed from chloroform, a PCE over 17% is achieved.•As-cast PM6:Y6-eC6-BO OSCs processed from o-XY delivered a PCE of 16.38%, this is the highest efficiency of non-halogenated-solvent processed as-cast OSCs to date.

Although the polymer/polymer blend systems still lag far behind small-molecule-acceptor-based counterparts in power conversion efficiencies (PCEs), the ternary blending strategy provides a simple and promising avenue to achieve an ideal nanoscale blend morphology for reducing the efficiency-stability gap of all-polymer solar cells (all-PSCs). Herein, we designed a narrow-band-gap chlorinated polymer acceptor PY-2Cl and incorporated into the PM6:PY-1S1Se host blend. The addition of PY-2Cl extends the absorption spectra, improves the molecular packing of host-guest acceptors, solidifies the blend microstructure, and suppresses the non-radiative recombination. Consequently, the PCE of the ternary blend is improved up to 18.2% (certified value 17.8%), which represents the highest PCE reported for all-PSCs so far. Impressively, the ternary blend exhibited smaller Urbach energy and better operation stability than did the corresponding binary systems. This work heralds a brighter future for accelerating the development of high-performance all-polymer systems by molecular design and ternary strategy.

Inflammatory bowel disease (IBD) is a global chronic disease with a long duration and repeated relapse. Currently, there is still a lack of effective approaches to prevent IBD. Food-derived oryzanol (ORY) possesses extensive biological activities, such as ameliorating bowel diseases, antioxidation, and antiobesity. However, the mechanism of ORY in preventing colitis remains unclear. The present research aims to explore the potential mechanism of ORY in dextran sulfate sodium (DSS)-stimulated colitis in a rat model. The results showed that the symptoms of colitis were significantly improved with the administration of ORY. Mechanismly, the expression levels of Zonula occludens-1 (ZO-1), Claudin-1, Occludin, MUC2, and TFF3 were elevated through ORY treatment, suggesting that oral ORY relieved the degree of gut barrier damage of colitis rats. Meanwhile, 16S sequencing results found that ORY supplementation increased the abundances of Alloprevotella, Roseburia, Treponema, Muribaculaceae, and Ruminococcus, which are associated with the synthesis of short-chain fatty acids (SCFAs). Moreover, GC-MS results confirmed that ORY supplementation reversed the DSS-induced reduction of acetic acid, butyric acid, and total acid. Further research indicated that ORY intervention downregulated the TLR4/NF-κB/NLRP3 pathway, which is closely linked to the expression of proinflammatory cytokines and colon injury. Taken together, ORY ameliorates DSS-stimulated gut barrier damage and inflammatory responses via the gut microbiota–TLR4/NF-κB/NLRP3 signaling axis.

The development of the internet-of-thing (IoT) ecosystem has an urgent demand for convenient energy sources, such as indoor organic photovoltaics (IOPVs), to power IoT devices. However, the limited medium band-gap acceptors hinder the development of IOPVs. Herein, we report a ternary system suitable for indoor applications. Introducing BTA1 into the J52-Cl:BTA3 host blend can optimize energy offsets and molecular packing of the host materials and suppress the non-radiative recombination. Consequently, the tetrahydrofuran-processed ternary devices exhibit a power conversion efficiency (PCE) of 11.22% under 1 sun and an outstanding PCE of 28.84% under a 1,000 lux LED light. Furthermore, we have constructed large-scale opaque and semitransparent modules with PCEs of 22.0% and 14.77%, respectively. Impressively, the ternary IOPV also displays a normal organic light-emitting diode performance. This work suggests that the designed ternary system possesses great potential light-emitting functions for indoor multifunctional-integrated applications.

Side-chain engineering has been demonstrated as an effective method for fine-tuning the optical, electrical, and morphological properties of organic semiconductors toward efficient organic solar cells (OSCs). In this work, three isomeric non-fullerene small molecule acceptors (SMAs), named BTP-4F-T2C8, BTP-4F-T2EH and BTP-4F-T3EH, with linear and branched alkyl chains substituted on the αor βpositions of thiophene as the side chains, were synthesized and systematically investigated. The results demonstrate that the size and substitution position of alkyl side chains can greatly affect the electronic properties, molecular packing as well as crystallinity of the SMAs. After blending with donor polymer D18-Cl, the prominent device performance of 18.25% was achieved by the BTP-4F-T3EH-based solar cells, which is higher than those of the BTP-4F-T2EH-based (17.41%) and BTP-4F-T2C8-based (15.92%) ones. The enhanced performance of the BTP-4F-T3EH-based devices is attributed to its stronger crystallinity, higher electron mobility, suppressed biomolecular recombination, and the appropriate intermolecular interaction with the donor polymer. This work reveals that the side chain isomerization strategy can be a practical way in tuning the molecular packing and blend morphology for improving the performance of organic solar cells.

Non-fused medium bandgap acceptors consisting of multi-noncovalent interaction assisted unfused core enable organic photovoltaics with the desirable cost-efficiency balance.

Isomerization of functional groups in photovoltaic materials plays a vital role in molecular packing and their photovoltaic performance. In this work, two narrow-band gap polymer acceptors, PY5-TTz-FT and PY5-TTz-CT, are synthesized by copolymerization of the small-molecule acceptor (SMA) Y5 as the main backbone and thiophene-thiazolothiazole (TTz)-thiophene with isomerized ethylhexyl substitution on the thiophene π-bridges as the linking unit. The polymerized SMA (PSMA) PY5-TTz-CT with the ethylhexyl substituents close to the TTz unit exhibits red-shifted absorption spectra and a relatively higher lying lowest unoccupied molecular orbital (LUMO) energy level, in comparison with PY5-TTz-FT with the ethylhexyl substituents far from the TTz unit. However, PY5-TTz-CT exhibits poorer photovoltaic performance than that of PY5-TTz-FT in the all-polymer solar cells (all-PSCs) with PBDB-T as the polymer donor, due to the poor morphology of the PBDB-T:PY5-TTz-CT active layer, while the optimized all-PSC based on PBDB-T:PY5-TTz-FT shows a higher power conversion efficiency of 12.73%. The results imply that isomerization of polymer acceptors is an effective strategy to tune the molecular packing of the photovoltaic materials and photovoltaic performance of the all-PSCs.

A series of narrow bandgap polymer acceptors (PY5-BTZ, PY5-2TZ, PY5-PZ, and PY5-BT) were synthesized by copolymerizing a Y5-like small molecule acceptor (SMA) and different electron-withdrawing (A) units with thiophene π-bridges. Among the polymerized SMAs (PSMAs), the A-unit is bifluoro-benzotriazole for PY5-BTZ, thiazolo[5,4-d]thiazole for PY5-2TZ, pyrazine for PY5-PZ, and benzothiadiazole for PY5-BT. The four PSMA films possess narrower bandgaps of 1.43–1.45 eV. Interestingly, PY5-BTZ shows a higher-lying LUMO energy level of −3.72 eV (−3.76 eV for PY5-2TZ, −3.75 eV for PY5-PZ, and −3.78 eV for PY5-BT) and a stronger absorbance of 1.5 × 105cm–1(1.4 × 105cm–1for the other three PSMAs). The all-polymer solar cells (all-PSCs) with PY5-BTZ as the polymer acceptor and PBDB-T as the polymer donor exhibit a peak power conversion efficiency of 14.82% with a high open circuit voltage of 0.92 V, which benefits from the higher-lying LUMO level and stronger absorbance of the PY5-BTZ polymer acceptor. The results indicate that introducing weak electron-withdrawing A-units and thiophene π-bridges could be an effective approach in designing and synthesizing high-performance PSMA polymer acceptors for high-efficiency all-PSCs in the future.

Developing donor:acceptor (D:A) blends that work efficiently with small charge separation driving forces (or energetic offset) is highly desired for reducing the voltage loss and unveiling the working mechanism of organic photovoltaics (OPVs). Herein, by incorporating the weak electron-withdrawing acceptor unit of benzobis(thiazole), we design and synthesize two wide-bandgap (∼2 eV) polymer donors, PBTz-TF and PBTz-TCl, with deep highest occupied molecular orbital (HOMO) levels approaching that of the typical electron acceptor Y6, forming negligible HOMO offsets of 0.04 and 0 eV for PBTz-TF:Y6 and PBTz-TCl:Y6 blends, respectively. Interestingly, efficient charge separation is observed in both blends, while the PBTz-TCl:Y6 blend possesses multiple superiorities, including higher mobilities, longer exciton lifetimes, purer domains, and more dominant face-on orientation. These lead to a better efficiency of 15.06% at 0 eV HOMO offset in the PBTz-TCl:Y6-based OPV, which is superior compared to the PBTz-TF:Y6-based OPVs (14.73%) with a HOMO offset of 0.04 eV. This work explores the properties of low driving force D:A blends and should have implications in the fundamental understanding of the carrier dynamics in OPVs with a flat energetic offset.

Optimizing the molecular structures of organic solar cell (OSC) materials and boosting the power conversion efficiencies are the eternal theme in the solar energy region. A series of fused benzotriazole (BTA)-based A–DA′D–A structures of nonfullerene acceptors (such as Y18) were developed for application in efficient OSCs, in which high quantum efficiencies and low voltage losses could be achieved because of the optimized electron-deficient core and specific molecular geometry. Here, based on the BTA core, the bulky alkyl chain on the BTA unit was further tailored to minimize the lateral alkyl chains and enhance the crystallinity while maintaining an adequate solubility. The resulting NFAs of BTA-C1, BTA-C5, and BTA-C6 are synthesized. Compared with the well-designed molecular Y18 (BTA-C8), we found that simply replacing the 2-ethylhexyl chain with a single methyl (BTA-C1) can easily improve the fill factor up to 77%, but its poor light absorption capacity and large domain size impeded further efficiency improvement. In particular, the BTA-C5, with a shortened branch alkyl chain of 2-methylbutyl, achieves suitable solubility and enhanced crystallinity. Significantly, owing to the balanced charge carrier mobility and suitable phase separation, the BTA-C5-based binary single-junction OSCs achieve a high efficiency of 17.11%, which is one of the top values in BTA-based OSCs.

Nonfullerene acceptor (NFA) organic solar cells (OSCs) with power conversion efficiency (PCE) reaching up to 18% has shown tremendous potential toward practical applications. However, the non-radiative recombination loss in high-efficiency NFA OSCs is evidently large, and the origin remains unclear. Herein, by combining transient absorption spectroscopy, photovoltaic characterization, and detailed energy loss analysis, we unambiguously show the formation of NFA triplet exciton from free carrier recombination as a main non-radiative recombination and energy loss channel. More importantly, in contrast to the previous energetics point of view, we show side-chain fluorination in high-efficiency NFA OSCs has little effect on charge transfer energy landscapes but efficiently inhibits charge recombination to NFA triplet excitons, leading to higher VOCand PCE. Our findings provide a new view about energy loss in NFA OSCs and pave the way toward OSCs with lower VOCloss and efficiency exceeding 20%.

The field of all-polymer solar cells (all-PSCs) has experienced rapid development during the past few years, mainly driven by the design of efficient polymer acceptors (PAs). However, the polymer/polymer blend systems still lag far behind polymer/small molecule acceptor counterparts in power conversion efficiencies (PCEs). Here, we designed a near-infrared PAPY2F-T and paired it with polymer donor PM6 to fabricate all-PSCs with 15.0% PCE. Afterwards, PYT as the third component was introduced into the PM6:PY2F-T host system. Because of the complementary absorption bands and finely tuned microstructures of the ternary blend, the PCE is improved up to 17.2%, with the external quantum efficiency over 80% in visible and near-infrared spectral regions. Impressively, the ternary blend exhibited less energy loss, better light-soaking and photo-thermal stabilities than did the corresponding binary systems. This work promotes the development of high-performance ternary all-polymer systems and heralds a brighter future for accelerating the possible applications of all-PSCs.

Liquid crystal small molecules (LCSMs) are manifested as the effective additives to regulate the morphology of active layers and elevate the performance of ternary organic solar cells (TOSCs) in fullerene systems. However, the current studies for TOSCs based on efficient LCSMs are most out of the LC phase transition temperature, which is not conducive to accurately disclosure the effect of LCSMs on the morphology evolution. Besides, the inner working mechanism of LCSMs has not been investigated systematically and in-depth. Herein, a structurally simple donor–acceptor–donor type LCSM DFBT-TT6 with a low liquid crystal phase transition temperature is utilized as the third component to construct TOSCs based on a highly efficient nonfullerene system PM6:Y6. To unveil the work mechanism of LCSMs on the TOSCs performance and eliminate other interferences simultaneously, a structurally similar non-LCSM DFBT-DT6 with a low glass-transition temperature is further synthesized for a more clear comparison. Interestingly, the addition of DFBT-TT6 can delicately control the crystallinity and phase separation of PM6:Y6, rendering the optimized morphology with only 3 wt % DFBT-TT6. In contrast, the non-LCSM DFBT-DT6 shows a negligible effect on morphology regulation, indicating the unique ability of LC molecules in morphology control. The underlying working mechanism is revealed by the combined study of miscibility and the wetting coefficient of the blends, elucidating that the LCSM DFBT-TT6 has good compatibility with PM6 and Y6. Therefore, DFBT-TT6 is more prone to being located at the interface of PM6 and Y6, and it is energetically favorable for charge transfer. The aforementioned favorable morphology evolution is associated with improved crystallinity, phase separation, charge transfer, exciton dissociation, and collection efficiency, ultimately boosting the power conversion efficiency of TOSCs from 15.76% to 17.05% with a remarkable short-circuit current density of 26.56 mA/cm2. This work not only offers deep insight into the LCSM induced morphology evolution but also puts forward an affordable strategy to achieve high-performance TOSCs.

Rheumatoid arthritis (RA) is an autoimmune disease characterized by long duration and repeated relapse. This study explored the preventive effect of tangeretin (TAN) and 5-hydroxy-6,7,8,3′,4′-pentamethoxyflavone (5-HPMF) on RA, and the underlying molecular mechanism based on a rat model stimulated by bovine type II collagen (BIIC). After the intervention of TAN or 5-HPMF (TAN/5-HPMF) for 5 weeks, the RA lesions and autophagy levels of the synovial tissue were significantly reduced, and the ROS content and HO-1 expression level were down-regulated simultaneously. The relative expression levels of p-AKT and p-mTOR were down-regulated after TAN/5-HPMF feeding. Meanwhile, the relative expression level of p62 increased by more than two-fold for TAN/5-HPMF treated rats at 200 mg/kg BW comparing with those in BIIC group. Results of immunofluorescence staining and Western blotting further confirmed that TAN/5-HPMF treatment reduced BIIC-induced conversion from LC3I to LC3II. Observations under transmission electron microscope also demonstrated that the autophagy level was reduced upon TAN/5-HPMF intervention. Collectively, these results revealed that TAN and 5-HPMF prevented the pathological process of BIIC-stimulated arthritis through inhibiting the autophagy of synovial cells, achieved via the ROS-AKT/mTOR signal axis. Thus, our findings confirmed the protective potential of TAN and 5-HPMF for RA disease.

Vibrant research has demonstrated that the layer-by-layer (LBL) approach can achieve a preferable vertical microstructure; however, the lack of precise control over vertical composition and molecular organization remains. Herein, we demonstrated a guest polymer-tailored LBL (GPT-LBL) strategy to achieve the p-i-n microstructure constructed by in situmonitoring pre-aggregation behaviors of non-fullerene acceptors. This superior structure with built-in interpenetrating networks alleviates the trap density states and the energy loss, improves hole transfer dynamics, and balances the charge transport, thus maximizing open-circuit voltage (VOC), short-circuit current density (JSC), and fill factor (FF) simultaneously. Consequently, a highly efficient GPT-LBL organic solar cell (OSC) with a power conversion efficiency (PCE) of 19.41% (certified 19.0%) was achieved. Noticeably, the large-area (1.03 cm2) device for GPT-LBL OSCs yields a satisfactory PCE of 17.52% in open-air blade coating, which is one of the best values in green-solvent-processed OSCs. The insights for p-i-n structure will give implications for the device engineering and photo physics understanding, offering an effective way to enable efficient, stable, and scalable OSCs.

Zirconium disilicide (ZrSi2) has been investigated experimentally and theoretically for its structural and physical properties at high pressures. In situ compression experiments demonstrate that at low pressure, ZrSi2adopts the C49 structure (space group Cmcm), which persists up to 54.5 GPa at room temperature, and the unit cell of ZrSi2along b-axis is at least twice as compressible as along a- and c-axis. A bulk modulus of 170.0 ± 0.7 GPa (K′0= 4) is derived from the compression experiment employing methanol–ethanol mixture as the pressure-transmitting medium. Diffraction line-width analysis suggests a yield strength of about 3.0 GPa for ZrSi2under high pressures at room temperature. The first-principles calculations mostly agree with the experimental results, such as mechanical and dynamic stability and elastic anisotropy (Kc> Ka≫ Kb). However, predicted axial modulus Kbby modeling is significantly smaller than the experimentally determined value, resulting in a sizable discrepancy between experimental (170.0 GPa) and theoretical (121.0 GPa) bulk moduli.

A solid additive-assisted layer-by-layer (SAA-LBL) processing was developed to facilitate the inter-diffusion between polymer donor and acceptor and optimize the morphology of quasi-planar heterojunction for high-performance organic solar cells (OSCs).The pre-phase separation between fatty acid and polymer donor, easily tuned via controlling the cohesive energy, is critical to form the desired vertical phase-separation morphology.The SAA-LBL is generally applicable to various OSC systems, and enables the record efficiency of 19.02% among the binary OSCs.

The introduction of gas is the principal difference between external gas-assisted injection molding (EGAIM) and conventional injection molding. In this study, the effects of gas thickness and gas delay time on polymer temperature were discussed. A modified one-dimensional transient heat conduction model of polymer was established to reveal the relationships between polymer temperature and gas thickness and gas delay time in EGAIM. The temperature histories of polymer were obtained by the simulation methods, including Moldflow and ANSYS, and were verified by comparing the experimental data to numerical simulation results. The effects of gas thickness and gas delay time on the temperature histories of polymer will be discussed in detail. The results showed that the polymer temperature is strongly affected by the heat preservation of gas, which in turn, increases with the increase of gas thickness and delay time. This paper provides quantitative methods and theoretical guidance for the study of the effects of gas on the polymer temperature in EGAIM.

There has been considerable research interest paid to rare-earth transition-metal-doped Y3Al5O12, which has great potential for application as a laser crystal of new-type laser devices because of its unique optoelectronic and photophysical properties. Here, we present new research conducted on the structural evolution and crystal-field characteristics of a rare-earth Nd-doped Y3Al5O12laser crystal by using the CALYPSO structure search method and our newly developed WEPMD method. A novel cage-like structure with a Nd3+concentration of 4.16% is uncovered, which belongs to the standardized C222space group. Our results indicate that the impurity Nd3+ions are likely to substitute the Y3+at the central site of the host Y3Al5O12crystal lattice. The laser emission 4F3/2→ 4I11/2occurring at 1077 nm is in accord with that of the experimental data. By introducing the proper correlation crystal field, three transitions, 4G5/2→ 4I9/2, 4F7/2→ 4I9/2, and 4S3/2→ 4I9/2, are predicted to be good candidates for laser action. These findings can provide powerful guidelines for further experiments of rare-earth-metal-doped laser crystals.

Binary boron-based compounds are expected to possess unique molecular architecture and chemical bonding. Here, we explore how incorporation of a valence isoelectronic Al atom into boron clusters containing from 10 to 20 atoms modifies the structures and properties of the initial clusters. The global minima structures of neutral and anionic Al-doped boron cluster in the size range from 10 to 20 have been identified using the Crystal structure AnaLYsis by Particle Swarm Optimization method. The states with the promising geometrical structures are reoptimized using density functional theory and triple-ζ basis sets. It is found that the geometries of the ground states of the AlBnand AlBn–clusters possess planar, quasi-planar, and exohedral topologies. A nearly circular planar AlB18–cluster with C2vsymmetry and a large energy gap 2.98 eV has been discovered. The calculated photoelectron spectra of the anions are well in accord with the experimental spectra. The chemical-bonding analysis suggests that both large HLG and double π-aromaticity have much contribution to the electronic stability of AlB18–cluster. Our results elucidate the structural growth behavior of Al-doped boron clusters and enrich the growth pattern and chemical bonding nature of boron-based clusters.

Aluminum and aluminum-doped clusters have gained much attention in cluster science due to their potential applications in nanotechnology. Here, we report a combined photoelectron spectroscopy and density functional theory study of V-doped aluminum clusters. The lowest-energy geometric structures of neutral and anionic AlnV0/–(n= 5–14) clusters are identified by comparing the theoretical photoelectron spectra with the experimental results. Our results reveal that ground-state structural evolution of neutral and anionic clusters follows different patterns. The V atom in neutral AlnV clusters moves from convex capped to surface-substituted, to encapsulated site at n= 12, and then returns to surface-substituted sites again. However, as for the anionic AlnV–, the metal V atom always occupies the convex capped sites with the cluster size increasing to n= 14. The most stable structure of Al14V–cluster possesses a C3vsymmetric cagelike structure with the highest occupied molecular orbital–lowest unoccupied molecular orbital gap of 1.52 eV. Molecular orbital and adaptive natural density partitioning analysis of Al14V–suggests that the peripheral Al–Al interactions and delocalized Al–V interactions play important roles in its structural stability.

Objective :this study investigated the efficacy and safety of azacitidine and interferon α preemptive treatment in the post-transplant in patients with AML/MDS. Methods:between Octorber 1, 2019 and July 31, 2022, a total of 49 patients aged 17 to 62 years were enrolled into this prospective clinical study of post-transplant azacitidine combined with interferon α preemptive treatment. Patients with minimal residual disease (MRD) positive and / or mixed chimerism were scheduled to receive azacitidine, given as 32 mg/m 2per day subcutaneously for 5 days, and interferon α 3 million units/m 2per day from 8th day and continued for 28th day for 1 cycle. Results:patients who acquired treatment response were 34 (69.4%), of which turned MRD-negative and obtained complete chimerism were 22 (44.9%) and 5 (10.2%) at 1 cycle, respectively. Median follow-up time after preemptive intervention was 440(range, 45 to 927) days. Cumulative incidences of relapse (CIR) and no relapse mortality (NRM) were 36.7% and 4.1%, respectively. Probabilities of event-free survival (EFS) and overall survival (OS) were 55.1% and 71.4%, respectively. The most common adverse events were graft-versus-host disease (GVHD) (38.8%), liver toxicity (46.9%) and neutropenia (28.6%). Conclusion:these data support the notion that azacitidine combined with interferon α is better used as the preemptive therapy against relapse tendency for patients after allo-HSCT performed for AML/MDS. Side effects were mainly GVHD, reversible cytopenia and hepatic toxicity. This prospective trial in the post-transplant setting was feasible and safe but challenging. This trial was registered at www.clinicaltrials.gov as#NCT04078399.

Non-fused ring electron acceptors (NFREAs) have a broad application prospect in the commercialization of organic solar cells (OSCs) due to the advantages of simple synthesis and low cost. The selection of intermediate block cores of non-fused frameworks and the establishment of the relationship between molecular structure and device performance are crucial for the realization of high-performance OSCs. Herein, two A-D-A’-D-A type NFREAs namely CBTBO-4F and CBTBO-4Cl, constructed with a novel electron-deficient block unit N-(2-butyloctyl)-carbazole[3,4-c:5,6-c]bis[1,2,5]thiadiazole (CBT) and bridging unit 4,4-bis(2-ethylhexyl)-4H-cyclopenta[2,1-b:3,4-b']dithiophene (DTC) coupling with different terminals (IC-2F/2Cl), were designed and synthesized. The two NFREAs feature broad and strong photoresponse from 500 nm to 900 nm due to the strong intramolecular charge transfer characteristics. Compared with CBTBO-4F, CBTBO-4Cl shows better molecular planarity, stronger crystallinity, more ordered molecular stacking, larger van der Waals surface, lower energy level and better active layer morphology, contributing to much better charge separation and transport behaviors in its based devices. As a result, the CBTBO-4Cl based device obtains a higher power conversion efficiency of 10.18% with an open-circuit voltage of 0.80 V and a short-circuit current density of 21.20 mA/cm2. These results not only demonstrate the great potential of CBT, a new building block of the benzothiazole family, in the construction of high-performance organic conjugated semiconductors, but also suggest that the terminal chlorination is an effective strategy to improve device performance.

The contribution of lymphocyte subset composition of the graft on the outcomes following haploidentical peripheral blood stem cell transplantation (haploPBSCT) is not fully elucidated. We retrospectively analyzed 314 patients with hematological malignancies who underwent haploPBSCT from 2016 to 2020 in our center. We obtained a cutoff value of CD3+ T cell dose (2.96 × 108/kg) that separated the risk of II–IV acute graft-versus-host disease (aGvHD) and divided patients into the low CD3+ T cell dose group (CD3+ low) and the high CD3+ T cell dose (CD3+ high) group. Significantly higher incidences of I-IV aGvHD, II–IV aGvHD, and III–IV aGvHD were identified in the CD3+ high group (50.8%, 19.8%, and 8.1% in the high group, 23.1%, 6.0%, and 0.9% in the low group, P< 0.0001, P= 0.002, and P= 0.02, respectively). We found that CD4+ T cell and its naïve and memory subpopulations of grafts had a significant impact on aGvHD (P= 0.005, P= 0.018, and P= 0.044). Besides, we found an inferior reconstitution of natural killer (NK) cells in the CD3+ high group than in the low group within the first-year posttransplant (239 cells/μL vs 338 cells/μL, P= 0.0003). No differences in engraftment, chronic GvHD (cGvHD), relapse rate, transplant-related mortality (TRM), and overall survival (OS) were identified between the two groups. In conclusion, our study found that a high CD3+ T cell dose led to a high risk of aGvHD and inferior reconstitution of NK cells in the haploPBSCT setting. In the future, carefully manipulating the composition of lymphocyte subsets of grafts might reduce the risk of aGvHD and improve the transplant outcome.

Organic photovoltaics (OPVs) have achieved great progress in recent years due to delicately designed non-fullerene acceptors (NFAs). Compared with tailoring of the aromatic heterocycles on the NFA backbone, the incorporation of conjugated side-groups is a cost-effective way to improve the photoelectrical properties of NFAs. However, the modifications of side-groups also need to consider their effects on device stability since the molecular planarity changes induced by side-groups are related to the NFA aggregation and the evolution of the blend morphology under stresses. Herein, a new class of NFAs with local-isomerized conjugated side-groups are developed and the impact of local isomerization on their geometries and device performance/stability are systematically investigated. The device based on one of the isomers with balanced side- and terminal-group torsion angles can deliver an impressive power conversion efficiency (PCE) of 18.5%, with a low energy loss (0.528 V) and an excellent photo- and thermal stability. A similar approach can also be applied to another polymer donor to achieve an even higher PCE of 18.8%, which is among the highest efficiencies obtained for binary OPVs. This work demonstrates the effectiveness of applying local isomerization to fine-tune the side-group steric effect and non-covalent interactions between side-group and backbone, therefore improving both photovoltaic performance and stability of fused ring NFA-based OPVs.

Standard anti-thymocyte globulin (ATG) weight-based dosing often resulted in highly variable ATG exposure, which had profound effects on relapse and survival, especially in recipients with relatively low absolute lymphocyte count (ALC) before conditioning. Data regarding rabbit ATG pharmacokinetics and pharmacodynamics in the setting of HLA-haploidentical peripheral blood stem cell transplantation (haplo-PBSCT) is lacking. We conducted a retrospective study on 90 consecutive patients who underwent haplo-PBSCT with low dose rabbit ATG (5 mg/kg) plus low dose post-transplant cyclophosphamide (50 mg/kg) based regimen for graft-versus-host disease (GvHD) prophylaxis. We compared serum concentration of ATG and post-transplant results between patients with ALC<500/μl and ALC≥500/μl before conditioning. Patients with ALC<500/μl had higher ATG concentrations, delayed immune reconstitution, lower incidence of grade II-IV acute GvHD (0 vs. 19.42%, P= 0.043), higher risk of Epstein-Barr virus infection within 100 days post-transplant (47.78% vs. 22.22%, P= 0.020) and 1-year relapse rate (33.33% vs.11.59%, P= 0.041), and lower 1-year overall survival (OS) (52.38% vs.79.71%, P= 0.004), 1-year relapse free survival (RFS) (47.62% vs.75.36% for RFS, P= 0.014), and 1-year GvHD free relapse-free survival (GRFS) (42.89% vs.65.22%, P= 0.043). ALC<500/μl before conditioning was a significant poor risk factor for relapse, OS, RFS, and GRFS.

Maternal and collateral donors were associated with a higher incidence of graft-versus-host disease (GvHD) after haploidentical hematopoietic stem cell transplantation (haplo-HSCT). A more effective regimen for GvHD prophylaxis after haplo-HSCT with maternal/collateral donors needed to be explored. A retrospective study was performed on 62 patients after haploidentical peripheral blood stem cell transplantation (haplo-PBSCT) with maternal/collateral donors, which included 35 patients with low-dose antithymocyte globulin (ATG) plus low-dose posttransplant cyclophosphamide-based (low-dose ATG/PTCy-based) and 27 with ATG-based regimens for GvHD prophylaxis. The 180-day cumulative incidences (CIs) of grades II-IV and III-IV acute GvHD (aGvHD) were 17.7% and 6.8% in low-dose ATG/PTCy-based group, which were significantly lower than that in ATG-based group (55.4% and 31.9%) (P= 0.003 for grade II-IV and P= 0.007 for III-IV aGvHD). In low-dose ATG/PTCy-based group, the 1-year overall survival (OS) and relapse-free survival (RFS) were 80.0%and 80.4%, which were higher than that in ATG-based group with OS of 59.4% and RFS of 62.0%. In multivariate analysis, the low-dose ATG/PTCy-based regimen significantly reduced the risk of grade II-IV (HR = 0.357; P= 0.049) and grade III-IV aGvHD (HR = 0.190; P= 0.046) as an independent risk factor. The results suggested that the low-dose ATG/PTCy-based regimen could effectively prevent the occurrence of aGvHD after haplo-PBSCT with maternal/collateral donors compared with the ATG-based regimen.

Allogeneic hematopoietic stem cell transplantation (allo-HSCT) is one of the consolidation modalities for adult patients with T-cell lymphoblastic lymphoma (T-LBL). However, the optimal conditioning regimen needs to be explored. In the present study, 40 patients with T-LBL undergoing allo-HSCT were retrospectively analyzed, including 23/40 (57.5%) with total body irradiation (TBI)–based conditioning regimen and 17/40 (42.5%) with busulfan (BU)-based regimen. TBI–based regimen significantly increased the cumulative incidence (CI) of grade II to IV acute graft-versus-host disease (aGvHD) as compared with BU-based regimen (13.0% vs 0%, P= 0.000). The relapse risk was significantly lowered in TBI-based group with a 2-year CI of relapse (CIR) of 9.1% as compared with that of 49.6% in BU-based group (P= 0.008). The 1-year and 2-year non-relapse mortalities (NRMs) for all patients were 5.0% and 10.3%, respectively. The 1-year and 2-year NRMs were 8.9% and 16.0% in TBI-based group, and 0.00% and 0.00% in BU-based group (P= 0.140). The 2-year probabilities of overall survival (OS) and relapse-free survival (RFS) were 83.0% [95% confidence interval, 63.4%–100%] and 74.0% (95% confidence interval, 54.4%–93.6%) in TBI-based group, which were higher than that of 35.0% (95% confidence interval, 0.0%–72.2%) and 50.0% (95% confidence interval, 24.5%–75.4%) in BU-based group, respectively (P= 0.020 for OS and P= 0.081 for RFS). In multivariate analysis, TBI-based regimen significantly reduced the risk of relapse [subdistribution hazard ratio (SHR) = 0.030, 95% CI, 0.002–0.040, P= 0.000] and improved the OS [hazard ratio (HR) 0.121, 95% CI, 0.021–0.683, P= 0.017] as an independent prognostic factor. These results suggested that TBI-based regimen might be an optimal choice for adult patients with T-LBL undergoing allo-HSCT.

Unraveling the relationship between nanoscale morphology of active layers and chemical structures of organic semiconductor photovoltaic materials is crucially important for further advancing the development of all-small-molecule organic solar cells (SM-OSCs). Here, in order to delve into the effect of flexible side chains of small molecule donors on the photovoltaic properties of SM-OSCs, we synthesized two new small molecule donors substituted by different flexible alkyl chains (iso-octyl chains for SM1-EH and n-octyl chains for SM1-Oct). As a result, the two small molecules present different absorption properties, energy levels, and stacking characteristics. When blending with Y6 as an acceptor, the SM1-Oct-based SM-OSC demonstrated a higher PCE value of 11.73%, while the SM1-EH-based device presents a relatively poorer PCE value of 8.42%. In addition, the morphology analysis demonstrated that, compared with the SM1-EH:Y6 blend, the SM1-Oct:Y6 blend film displayed better molecular stacking properties with stronger multilevel diffraction and preferable phase separation, resulting in the higher hole mobility, more efficient charge separation efficiency, and better device performance. These results underline that reasonably adjusting the flexible alkyl chains of small molecule donors can be an effective approach to further advance the development of the SM-OSCs field.

The Y11-M and Y11-EB-based devices deliver the PCEs of 16.64% and 17.15% by tailoring side chains on different nitrogen aromatic rings for organic photovoltaics.