编译|冯维维
Science, 30 July 2026,Volume 393, Issue 6810
《科学》2026年7月30日,第393卷,6810期
物理学Physics
Toward an exact quantum many-body treatment of Kondo correlation in magnetic impurities
迈向磁性杂质中近藤关联的精确量子多体处理
▲ 作者:TIANYU ZHU, LINQING PENG, HUANCHEN ZHAI, ZHI-HAO CUI, RUNZE CHI, AND GARNET KIN-LIC CHAN
▲链接:
https://www.science.org/doi/10.1126/science.adq7402
▲摘要:
近藤效应是一种典型的量子现象,源于磁性杂质中的局域电子与金属基体中的巡游电子之间的相互作用。
尽管这一现象数十年来一直是量子多体方法的试验场,但如何以材料特异性精确描述近藤物理仍具挑战性。
研究者提出了一种系统的从头算方法,以趋近于对近藤关联进行精确的零温电子结构处理。在一系列3d过渡金属中,他们提取出的近藤温度与实验上细微的变化趋势相匹配,其精度超过了标准模型。
研究者进一步从微观层面深入了解了这些趋势的根源。更广泛地说,该研究展示了从完全从头算多体模拟出发,并推向收敛预测领域的可能性。
▲ Abstract:
The Kondo effect is a prototypical quantum phenomenon arising from the interaction between localized electrons in a magnetic impurity and itinerant electrons in a metallic host. Although this phenomenon has served as the testing ground for quantum many-body methods for decades, the precise description of Kondo physics with material specificity remains challenging. Here, we present a systematic ab initio approach to converge toward an exact zero-temperature electronic treatment of Kondo correlations. Across a series of 3d transition metals, we extracted Kondo temperatures matching subtle experimental trends, with accuracy exceeding that of standard models. We further obtained microscopic insight into the origin of these trends. More broadly, we demonstrate the possibility to start from fully ab initio many-body simulations and push toward the realm of converged predictions.
化学Chemistry
Catalytic Appel fluorination of alcohols with potassium fluoride
氟化钾催化Appel反应实现醇的氟化
▲ 作者:ANIRBAN MONDAL, JOB J. C. STRUIJS, CALEB J. N. DOYLE, ZIJUN CHEN, ZIAN WANG, WORAWIT TANGAMORNCHAIPATTANA, CHRISTOPHE ALLAIS, PAUL F. RICHARDSON, JARED PIPER, AND VéRONIQUE GOUVERNEUR
▲链接:
https://www.science.org/doi/10.1126/science.aec6298
▲摘要:
Appel卤化反应广泛用于将醇转化为烷基卤化物,但不适用于制备烷基氟化物,因为氟会被二氟鏻烷螯合而无法参与反应。
研究者引入了可在空气中稳定存放的新戊氧基鏻盐来解决这一长期存在的挑战。利用这些试剂,多种醇可在氢键相转移催化条件下与氟化钾发生氟化反应,该反应模式为实现醇的对映选择性氟化提供了一条途径。
其机理是:首先形成新戊氧基氟鏻烷,该中间体倾向于与醇底物发生可逆交换,而非生成二氟鏻烷。
催化剂有助于氟化钾的溶解以及磷–氟键的解离,从而使烷氧基鏻氟离子对发生构型翻转的氟化反应。催化循环的周转源于催化剂对氟离子的结合强于对氧化膦(反应的副产物)的结合,而氧化膦可作为合成鏻试剂的起始原料进行回收利用。
▲ Abstract:
Appel halogenation reactions are widely used to convert alcohols to alkyl halides but are not suitable to prepare alkyl fluorides because fluoride is sequestered as a difluorophosphorane. In this work, we introduce bench-stable neopentoxyphosphonium salts to solve this enduring challenge. With these reagents, various alcohols undergo fluorination with potassium fluoride under hydrogen bonding phase-transfer catalysis, a manifold offering a pathway to enantioselective fluorination of alcohols. Mechanistically, a neopentoxyfluorophosphorane is formed, which undergoes reversible exchange with the alcohol substrate in preference to difluorophosphorane formation. The catalyst assists with potassium fluoride solubilization and with phosphorus–fluorine bond dissociation, leading to the alkoxyphosphonium fluoride ion pair undergoing stereoinvertive fluorination. Turnover results from stronger binding of the catalyst to fluoride than phosphine oxide, the by-product of the reaction, which is recyclable as starting material for the synthesis of the phosphonium reagents.
物理化学Physical Chemistry
n-Type polymer layers enable efficient, scalable, and thermally stable perovskite solar modules
n型聚合物层助力高效、可扩展且热稳定的钙钛矿太阳能电池组件
▲ 作者:DANPENG GAO, JIE GONG, LEI YANG, NING WANG, BOHONG CHANG, LIANGCHEN QIAN, FRANCESCO VANIN, CHUNLEI ZHANG, ZEXIN YU, AND ZONGLONG ZHU
▲链接:
https://www.science.org/doi/10.1126/science.aed8175
▲摘要:
倒置(p-i-n)结构钙钛矿太阳能电池中使用的富勒烯基电子传输层(ETL)存在成本高、可扩展性差和不稳定等问题,而高稳定性无机氧化物则存在能级匹配不佳和磁滞增强等缺点,从而降低了功率转换效率(PCE)。
研究者报道了一种非富勒烯共轭聚合物——2PB-T,该聚合物在主链中引入了共面且吸电子的苝二酰亚胺(PBI)单元。PBI聚合物主链和侧链工程通过优化电子传输性能、薄膜均匀性和界面结合力,解决了小分子ETL的不稳定性问题。
小面积器件实现了27.8%的冠军PCE,经认证的最大功率点跟踪(MPPT)效率为27.3%。面积为20.6和625平方厘米的钙钛矿组件的PCE分别达到24.4%和22.5%。
小面积器件在空气中85℃下连续MPPT测试1752小时后,仍保持初始PCE的98.6%以上;625平方厘米组件在户外运行5900小时后,仍保持初始PCE的96.9%。
▲ Abstract:
Fullerene-based electron transport layers (ETLs) used in inverted (p-i-n) perovskite solar cells face issues regarding cost, scalability, and instability, whereas highly stable inorganic oxides feature unfavorable energy alignment and enhance hysteresis, which reduce power conversion efficiency (PCE). We report a nonfullerene conjugated polymer, 2PB-T, that incorporates coplanar and electron-withdrawing perylene bisimide (PBI) units into its backbone. The PBI polymeric backbone and side-chain engineering address the instability of small-molecule ETLs by optimizing electron transport properties, film uniformity, and interfacial binding. Small-area devices achieved a champion PCE of 27.8%, with a certified maximum power point tracking (MPPT) efficiency of 27.3%. Perovskite modules with areas of 20.6 and 625 square centimeters reached PCEs of 24.4 and 22.5%, respectively. Small-area devices retained more than 98.6% of their initial PCE after 1752 hours of continuous MPPT at 85°C in air, and the 625-square-centimeter module maintained 96.9% of its initial PCE after 5900 hours of outdoor operation.
Plasma surface engineering for efficient and stable perovskite solar cells and modules
等离子体表面工程用于高效稳定的钙钛矿太阳能电池及组件
▲ 作者:RUNDONG FAN, YUE MA, SHUOYANG XU, LIANG CHENG, ZHONGYANG ZHANG, YAN LI, HUIJUN LIU, ZHAOBOXUN BAO, GUILIN LIU,AND HUANPING ZHOU
▲链接:
https://www.science.org/doi/10.1126/science.aeg1730
▲摘要:
钙钛矿太阳能电池(PSC)的不稳定性主要源于与软质多组分钙钛矿晶格相关的界面缺陷的形成和演化。
研究者报道了一种可规模化、基于等离子体的钝化策略,该策略通过在大面积钙钛矿薄膜上进行原位化学反应,形成共形、均匀且强键合的异质结构。
该方法还能减轻激光划刻互连区域内的缺陷积累,而局部损伤往往是这些区域导致组件级别性能损失的主要原因。
研究者在小面积器件(有效面积8.313平方毫米)中实现了27.2%的功率转换效率(PCE),在100平方厘米组件(孔径面积65.05平方厘米)中实现了24.0%的PCE(认证效率为23.5%)。
小面积器件在85°C、1倍太阳光照下经过2000小时最大功率点跟踪后,仍保持初始PCE的98.1%;100平方厘米组件在65°C、1倍太阳光照下经过1600小时后,仍保持初始PCE的99.3%。
▲ Abstract:
The instability of perovskite solar cells (PSCs) stems largely from the formation and evolution of interfacial defects associated with the soft, multicomponent perovskite lattice. We report a scalable, plasma-based passivation strategy that forms conformal, uniform, and strong-bonded heterostructure through in situ chemical reactions on large-area perovskite films. This approach also mitigates defect accumulation within the laser-scribed interconnection regions, where localized damage often dominates module-level performance losses. We achieved a power conversion efficiency (PCE) of 27.2% in small-area devices (active area 8.313 square millimeters) and 24.0% (certified efficiency of 23.5%) in 100-square-centimeter (cm2) modules (aperture area 65.05 cm2). The small-area device retained 98.1% of its initial PCE after 2000 hours of maximum power point tracking at 85°C under 1-sun illumination, and the 100-cm2 module retained 99.3% of its initial PCE after 1600 hours at 65°C under 1-sun illumination.
生命科学Life Science
Atlas of lysosomal aging reveals a metabolite signature shared with lysosomal storage disorders
溶酶体衰老图谱揭示一种与溶酶体贮积症共享的代谢特征
▲ 作者:ANNA M. PUSZYNSKA, THAO P. NGUYEN, ANDREW L. CANGELOSI, ANDREA ARMANI, JUSTIN M. ROBERTS, KRISTIN A. SINGH, JAMES C. CAMERON, TENZIN TSEYANG, GRACE Y. LIU, AND JONATHAN S. WEISSMAN
▲链接:
https://www.science.org/doi/10.1126/science.ady0832
▲摘要:
溶酶体长期以来被认为会在衰老过程中退化,但这种退化的分子基础一直不清楚。研究者将快速溶酶体分离技术与细胞器分辨代谢组学相结合,绘制了跨组织和跨物种的溶酶体衰老图谱。
在小鼠、大鼠和恒河猴中,脑、心脏、肌肉和脂肪组织中的衰老溶酶体累积了甘油磷酸二酯和胱氨酸——这些代谢物与幼年型溶酶体贮积症(巴顿病和胱氨酸病)相关。
在小鼠中,这些变化随年龄增长而逐渐加重,早于机体整体的衰退,并且在心脏和肌肉中受到热量限制的减缓。这揭示了一种保守的溶酶体衰老代谢特征,与某些溶酶体贮积症的分子特征相呼应。
▲ Abstract:
Lysosomes have long been suspected to deteriorate during aging, but the molecular basis of this decline has remained unclear. Puszynska et al. combined rapid lysosome isolation with organelle-resolved metabolomics to profile lysosomal aging across tissues and species (see the Perspective by Na and Brunet). In mice, rats, and rhesus macaques, aged lysosomes in brain, heart, muscle, and adipose tissue accumulated glycerophosphodiesters and cystine, metabolites associated with the juvenile lysosomal storage disorders Batten disease and cystinosis. In mice, these changes increased progressively with age, preceded organismal decline, and were attenuated by caloric restriction in heart and muscle, revealing a conserved metabolic signature of lysosomal aging that mirrors the molecular features of select lysosomal storage disorders.
DNA polymerization activates RNA cleavage of a reverse transcriptase–like antiviral enzyme
DNA聚合作用激活一种逆转录酶样抗病毒酶的RNA切割活性
▲ 作者:XUEJUN RONG (荣雪君), JUN XIAO (肖军) , XINYUAN ZHAO (赵新元) , YAN YAN (闫艳), JING LI (李静), YIFAN CHEN (陈逸凡), YIHUA FAN (范益华), ZHICHAO LIU (刘志超), YUE CAO (曹越) , AND BIN ZHU (朱斌)
▲链接:
https://www.science.org/doi/10.1126/science.aef3178
▲摘要:
防御相关逆转录酶(DRTs)通过多种策略介导细菌的抗病毒免疫,其中许多策略依赖于非编码RNA(ncRNAs)。
Rong等人揭示了一种不依赖非编码RNA的机制,在该机制中,DRT4感知噬菌体诱导的核苷酸升高,并合成蛋白质引物引导的单链DNA。这种DNA通过折叠成稳定结构或在病毒蛋白的协助下,从聚合酶口袋中被置换出来。
DNA置换随后触发DRT4的构象变化,激活其RNA水解酶活性,导致病毒和细菌RNA的降解。这种精妙的策略可终止感染并诱导宿主进入休眠状态,揭示了一种将DNA合成与RNA切割联系起来的抗病毒免疫新范式。
▲ Abstract:
Defense-associated reverse transcriptases (DRTs) mediate bacterial antiviral immunity through diverse strategies, many of which rely on noncoding RNAs (ncRNAs). Rong et al. uncovered an ncRNA-independent mechanism in which DRT4 senses phage-induced nucleotide elevation and synthesizes protein-primed single-stranded DNA. This DNA is displaced from the polymerase pocket either by folding into stable structures or with the assistance of viral proteins. DNA displacement then triggers a conformational change in DRT4 that activates its RNA hydrolase activity, leading to the degradation of both viral and bacterial RNA. This elegant strategy halts infection and induces host dormancy, revealing a paradigm of antiviral immunity that links DNA synthesis to RNA cleavage.
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