Communications Chemistry最新文献_第9页

Ultrafast probing of isotope-induced explicit symmetry breaking in ethylene. 乙烯中同位素诱导显对称破缺的超快探测。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-31 DOI: 10.1038/s42004-025-01621-z

Alessandro Nicola Nardi, Alexie Boyer, Yaowei Hu, Vincent Loriot, Franck Lépine, Morgane Vacher, Saikat Nandi

{"title":"Ultrafast probing of isotope-induced explicit symmetry breaking in ethylene.","authors":"Alessandro Nicola Nardi, Alexie Boyer, Yaowei Hu, Vincent Loriot, Franck Lépine, Morgane Vacher, Saikat Nandi","doi":"10.1038/s42004-025-01621-z","DOIUrl":"10.1038/s42004-025-01621-z","url":null,"abstract":"Symmetry governs nature's laws, yet many of the natural phenomena occur due to the breakdown of symmetry. Here, we show how isotope-induced inversion symmetry breaking influences ultrafast photoisomerization processes in ethylene. Using extreme ultraviolet pump - near infrared probe time-of-flight mass spectrometry, we find that replacing one of the carbon atoms in ethylene with a 13C isotope leads to twice-faster structural relaxation via ethylene-ethylidene isomerization in the photo-excited molecular cation. Advanced trajectory surface hopping calculations incorporating the nuclear symmetry of the molecular systems, reveal that it arises from the mixing of different normal modes in the isotope-substituted species, interactions otherwise forbidden by symmetry. Although the mixing does not alter the symmetry of the electronic Hamiltonian, it modifies that of the nuclear Hamiltonian, causing explicit symmetry breaking. This facilitates efficient intra-molecular vibrational energy redistribution, lowering the isomerization yield. Our findings offer opportunities to use isotope-induced nuclear symmetry breaking to control the outcome of light-molecule interactions across ultrafast timescales.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"222"},"PeriodicalIF":6.2,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12314038/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144759369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Titanocenes functionalization with high chemical diversity via titanium protecting groups. 通过钛保护基团实现高化学多样性的二茂钛基团功能化。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-30 DOI: 10.1038/s42004-025-01624-w

Emanuele Casali, Andrea Gandini, Gabriele Merlo, Lorenzo Carli, Jan J Weigand, Alessio Porta, Giuseppe Zanoni

{"title":"Titanocenes functionalization with high chemical diversity via titanium protecting groups.","authors":"Emanuele Casali, Andrea Gandini, Gabriele Merlo, Lorenzo Carli, Jan J Weigand, Alessio Porta, Giuseppe Zanoni","doi":"10.1038/s42004-025-01624-w","DOIUrl":"10.1038/s42004-025-01624-w","url":null,"abstract":"Titanocenes are well-recognized for their diverse applications in catalysis and biomedical research. Despite their potential, challenges related to stability and functionalization have limited broader utility, especially in medicinal chemistry. In this study, we present a strategy for the functionalization of titanocenes using a class of titanium protecting groups. This approach provides enhanced control over reactivity and significantly broadens the scope of structurally diverse modifications accessible for these complexes. Furthermore, we demonstrate the successful integration of a BODIPY fluorophore into titanocene-based systems, enabling advanced cellular imaging and visualizing the real perinuclear distribution of these organometallic compounds in living cell. The efficient incorporation of biomolecules such as biotin and cholesteryl derivatives through click-chemistry ligation underscores the potential of this method to facilitate the development of titanocene-based agents for pharmaceutical applications. By addressing previous limitations, this work paves the way for more effective utilization of titanocenes in both synthetic and biomedical fields.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"221"},"PeriodicalIF":6.2,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12310976/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144752625","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cardiolipin acyl chain composition tailors the conformation of mammalian ATP synthase dimers. 心磷脂酰基链的组成决定了哺乳动物ATP合酶二聚体的构象。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-30 DOI: 10.1038/s42004-025-01611-1

M Makowski, V G Almendro-Vedia, I López-Montero

引用次数: 0

Synthesis, biological evaluation and clinical trials of Cereblon-based PROTACs. 小脑基PROTACs的合成、生物学评价及临床试验。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-29 DOI: 10.1038/s42004-025-01598-9

André T S Vicente, Sara P S P Moura, Jorge A R Salvador

引用次数: 0

Structural molecular details of the endocytic adaptor protein CALM upon binding with phosphatidylinositol 4,5-bisphosphate-containing model membranes. 与含4,5-二磷酸磷脂酰肌醇模型膜结合的内吞衔接蛋白CALM的结构分子细节。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-29 DOI: 10.1038/s42004-025-01590-3

Andreas Santamaria, Daniel Pereira, Nisha Pawar, Bernard T Kelly, Javier Carrascosa-Tejedor, Mariana Sardo, Luís Mafra, Giovanna Fragneto, David J Owen, Ildefonso Marín-Montesinos, Eduardo Guzmán, Nathan R Zaccai, Armando Maestro

{"title":"Structural molecular details of the endocytic adaptor protein CALM upon binding with phosphatidylinositol 4,5-bisphosphate-containing model membranes.","authors":"Andreas Santamaria, Daniel Pereira, Nisha Pawar, Bernard T Kelly, Javier Carrascosa-Tejedor, Mariana Sardo, Luís Mafra, Giovanna Fragneto, David J Owen, Ildefonso Marín-Montesinos, Eduardo Guzmán, Nathan R Zaccai, Armando Maestro","doi":"10.1038/s42004-025-01590-3","DOIUrl":"10.1038/s42004-025-01590-3","url":null,"abstract":"Clathrin assembly lymphoid myeloid leukaemia protein (CALM) is involved in the formation of clathrin-mediated endocytic coats by virtue of binding many proteins involved in the process, including clathrin itself and AP2 cargo adaptor complex. CALM is able to specifically recognize the inner leaflet of the plasma membrane by binding the membrane's phosphatidylinositol 4,5-bisphosphate (PtdIns(4,5)P2). Here, a quantitative biophysical approach -combining neutron/X-ray scattering, solid-state NMR, atomic force microscopy, and quartz crystal microbalance with dissipation monitoring-, was exploited to investigate CALM interaction with PtdIns(4,5)P2-presenting model membranes. The presented experimental data reveal CALM's folded domain partially embeds (12% volume occupancy) within the membrane, directly coordinating a cluster of 4 to 5 PtdIns(4,5)P2 molecules via phosphate interactions. The N-terminal amphipathic helix inserts ~8 Å into the headgroup region, reducing local membrane stiffness by 36% (from 22 to 14 MPa) while increasing viscoelastic dissipation. These results establish a plausible threefold curvature-generation mechanism: PtdIns(4,5)P2 clustering, helix insertion-induced lipid compaction and global mechanical softening-collectively lowering the energy barrier for membrane deformation.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"219"},"PeriodicalIF":6.2,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12307879/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144741418","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Publisher Correction: Locating hydrogen in the Mg₅Bi₃H_x Zintl phase. 更正：定位氢在Mg5Bi3Hx Zintl相。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-28 DOI: 10.1038/s42004-025-01616-w

Teuta Neziraj, Lev Akselrud, Marcus Schmidt, Ulrich Burkhardt, Yuri Grin, Ulrich Schwarz

引用次数: 0

Dynamics of hydrogen-bonded end groups in bulk polymers revealed by solid-state NMR spectroscopy relaxation dispersion experiments. 固体核磁共振波谱弛豫色散实验揭示了大块聚合物中氢键端基的动力学。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-28 DOI: 10.1038/s42004-025-01597-w

Sophia Thiele, Christopher J G Plummer, Laura Piveteau, Holger Frauenrath

{"title":"Dynamics of hydrogen-bonded end groups in bulk polymers revealed by solid-state NMR spectroscopy relaxation dispersion experiments.","authors":"Sophia Thiele, Christopher J G Plummer, Laura Piveteau, Holger Frauenrath","doi":"10.1038/s42004-025-01597-w","DOIUrl":"10.1038/s42004-025-01597-w","url":null,"abstract":"The dynamic nature of supramolecular networks of telechelic polymers offers new avenues for the design of novel materials with enhanced melt strength and extensibility, increased energy at break, or self-healing properties. However, monitoring the kinetics of the underlying molecular-level scission-reaggregation events remains challenging, particularly in high-molar-mass polymers in the bulk state. Here, we employ solid-state 1H NMR spectroscopy relaxation dispersion experiments to investigate the aggregation-scission dynamics in poly(ε-caprolactone) modified with oligopeptide end groups that form one-dimensional hydrogen-bonded aggregates. We have successfully determined the timescale of end-group dissociation directly and independently of any relaxation of the polymer segments at different temperatures in the bulk semi-crystalline and melt state. This site-specific, non-destructive method is applicable to entangled, high-molar-mass polymers without chemical modifications or modeling, provides critical insight into the dynamics of supramolecular networks in the bulk state, and promises to be a valuable tool for the directed development of next-generation functional materials.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"217"},"PeriodicalIF":6.2,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12304251/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144728386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Design of Mn(1,4-DO2A) derivatives as stable and inert contrast agents for magnetic resonance imaging. Mn（1,4- do2a）衍生物作为稳定和惰性磁共振成像造影剂的设计。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-26 DOI: 10.1038/s42004-025-01615-x

Weiyuan Xu, Zheng Cai, Fabio Carniato, Yi Lu, Xinjian Ye, Xinhui Xiao, Jiao Xu, Gengshen Mo, Yinghui Ding, Yong Jian, Xinzhong Ruan, Zhihan Yan, Fangfu Ye, Carlos Platas-Iglesias, Mauro Botta, Lixiong Dai

{"title":"Design of Mn(1,4-DO2A) derivatives as stable and inert contrast agents for magnetic resonance imaging.","authors":"Weiyuan Xu, Zheng Cai, Fabio Carniato, Yi Lu, Xinjian Ye, Xinhui Xiao, Jiao Xu, Gengshen Mo, Yinghui Ding, Yong Jian, Xinzhong Ruan, Zhihan Yan, Fangfu Ye, Carlos Platas-Iglesias, Mauro Botta, Lixiong Dai","doi":"10.1038/s42004-025-01615-x","DOIUrl":"10.1038/s42004-025-01615-x","url":null,"abstract":"Manganese(II) is considered a valuable alternative to gadolinium(III) in developing contrast agents (CAs) for magnetic resonance imaging (MRI). However, due to the labile nature of common Mn(II) complexes, designing ligands that enable stable and inert complexation is essential before clinical application. Mn(1,4-Et4DO2A) bearing four ethyl groups, is found to have a log KMnL as high as 17.86, together with a pMn of 7.52 at pH 7.4. Kinetically, Mn(1,4-Et4DO2A) is approximately 20 times more inert than Mn(1,4-DO2A) in the presence of a 25-fold excess of Zn(II) at pH 6.0 and 37 °C, with the incorporation of a benzoic group to one pendant arm extending the half-life time (t1/2) to around 22 hours. Its r1 is measured as 2.34 and 2.20 mM-1 s-1 at 310 K and 1.5 and 3.0 T, respectively, representing an approximate 50% increase compared to Mn(1,4-DO2A). Mn(1,4-Et4DO2A) shows hepatic preference in mice, and its efficacy in diagnosing orthotopic hepatocellular carcinoma (HCC) is also confirmed.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"215"},"PeriodicalIF":6.2,"publicationDate":"2025-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12297526/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144717658","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Emergence of conformational diversity and complexity of supramolecular structure by the interaction of a simple molecule with a uniform surface. 由具有均匀表面的简单分子相互作用而产生的构象多样性和复杂的超分子结构。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-24 DOI: 10.1038/s42004-025-01607-x

S Fatemeh Mousavi, Aisha Ahsan, Aaron Oechsle, Narmadha Devi, Yoshitaka Matsushita, Luiza Buimaga-Iarinca, Cristian Morari, Waka Nakanishi, Katsuhiko Ariga, Yutaka Wakayama, Yusuke Yamauchi, Thomas A Jung, Jonathan P Hill

{"title":"Emergence of conformational diversity and complexity of supramolecular structure by the interaction of a simple molecule with a uniform surface.","authors":"S Fatemeh Mousavi, Aisha Ahsan, Aaron Oechsle, Narmadha Devi, Yoshitaka Matsushita, Luiza Buimaga-Iarinca, Cristian Morari, Waka Nakanishi, Katsuhiko Ariga, Yutaka Wakayama, Yusuke Yamauchi, Thomas A Jung, Jonathan P Hill","doi":"10.1038/s42004-025-01607-x","DOIUrl":"10.1038/s42004-025-01607-x","url":null,"abstract":"The emergence of complexity during self-assembly of simple molecular building blocks is an important aspect in the synthesis of nanoarchitectures from supramolecular functional units. In particular, two-dimensional nanostructures are important from the point-of-view of technological applications. Here, a remarkably complex on surface network is observed to form spontaneously from a single molecular module (porphyrin) having multiple site-specific conformations. The interplay of different physicochemical interactions at the surface contributes to the site-specific symmetry breaking of the porphyrin conformation, and was investigated at different substrates. Molecular conformational flexure, relocation in the corrugated surface potential, interactions with surface state electrons, and last but not least mutual intermolecular binding by hydrogen bonding at different elevations above the substrate are critical elements. We discuss the possibility of surfaces and interfaces causing quasidegeneracy of molecular configurations in supramolecular self-assembly, and the adsorbate-adsorbent interface as the driver for this system to behave counterintuitively to equilibrium thermodynamics.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":"8 1","pages":"214"},"PeriodicalIF":6.2,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12290036/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144706598","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Towards net zero by data-driven discovery of sustainable cement alternatives. 通过数据驱动的可持续水泥替代品的发现，实现净零。

IF 6.2 2区化学

Communications Chemistry Pub Date : 2025-07-24 DOI: 10.1038/s42004-025-01608-w

Jack D Evans

引用次数: 0