JACS Au最新文献

{"title":"Revealing the Ultrafast Energy Transfer Pathways in Energetic Materials: Time-Dependent and Quantum State-Resolved","authors":"Jia Liu,&nbsp;Jitai Yang,&nbsp;Gangbei Zhu,&nbsp;Jiarui Li,&nbsp;You Li,&nbsp;Yu Zhai,&nbsp;Huajie Song*,&nbsp;Yanqiang Yang* and Hui Li*,&nbsp;","doi":"10.1021/jacsau.4c0077510.1021/jacsau.4c00775","DOIUrl":"https://doi.org/10.1021/jacsau.4c00775https://doi.org/10.1021/jacsau.4c00775","url":null,"abstract":"<p >Intramolecular vibrational energy transfer is gaining tremendous attention as a regulator of condensed-phase behavior and reactions. In polyatomic molecules, this transfer is an ultrafast process involving multiple modes with numerous quantum states. The inherent complexity and rapid evolution of these processes pose significant challenges to experimental observation, and the high computational costs make full quantum mechanical calculations impractical with current technology. In the intramolecular energy transfer process, whether the doorway modes are intermediaries for transferring energy from lattice phonons to high-frequency intramolecular vibrational modes has been a controversial issue. However, the broad range of doorway modes complicates the experimental identification of a specific doorway in the transfer process corresponding to a specific end point. Here, for the first time, we utilize a combination of vibrational projection, statistical analysis, and the local quantum vibrational embedding (LQVE) method to elucidate the ultrafast energy transfer pathways that upconvert energy from lattice phonons to intramolecular modes in the typical energetic material β-HMX. This approach enables us to resolve the coupled vibrational mode groups, identify the most probable energy transfer pathways corresponding to the different final modes, and clearly confirm that the doorway region is a mandatory pathway for energy transfer. The LQVE method’s time-dependent and quantum state-resolved advantages are leveraged to reveal the microscopic mechanism of the energy transfer process. The time scale of these processes is determined at about 1 ps, and the first theoretical two-dimensional infrared spectroscopy evidence is provided, which is confirmed by the experimental results. These findings deliver important insights into the fundamental mechanisms of ultrafast energy transfer in energetic materials, providing theoretical support for controlling explosive behavior and designing new explosives. The methodologies developed in this work can be extended to other condensed phase materials and used to evaluate the coupling between multiple vibrational modes.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4455–4465 4455–4465"},"PeriodicalIF":8.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00775","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mechanistic Insights into Nonadiabatic Interband Transitions on a Semiconductor Surface Induced by Hydrogen Atom Collisions","authors":"Lingjun Zhu,&nbsp;Qijing Zheng,&nbsp;Yingqi Wang,&nbsp;Kerstin Krüger,&nbsp;Alec M. Wodtke,&nbsp;Oliver Bünermann,&nbsp;Jin Zhao*,&nbsp;Hua Guo* and Bin Jiang*,&nbsp;","doi":"10.1021/jacsau.4c0090910.1021/jacsau.4c00909","DOIUrl":"https://doi.org/10.1021/jacsau.4c00909https://doi.org/10.1021/jacsau.4c00909","url":null,"abstract":"<p >To understand the recently observed enigmatic nonadiabatic energy transfer for hyperthermal H atom scattering from a semiconductor surface, Ge(111)<i>c</i>(2 × 8), we present a mixed quantum-classical nonadiabatic molecular dynamics model based on the time-dependent evolution of Kohn–Sham orbitals and a classical path approximation. Our results suggest that facile nonadiabatic electronic transitions from the valence band to the conduction band occur selectively at the rest atom site, where surface states are doubly occupied, but not at the adatom site, where empty surface states are localized. This drastic site specificity can be attributed to the changes of the local band structure upon energetic H collisions at different surface sites, leading to transient near degeneracies and significant couplings between occupied and unoccupied orbitals at the rest atom but not at the adatom. These insights shed valuable light on the collision-induced nonadiabatic dynamics at semiconductor surfaces.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4518–4526 4518–4526"},"PeriodicalIF":8.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00909","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694469","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"CF3-Cyclobutanes: Synthesis, Properties, and Evaluation as a Unique tert-Butyl Group Analogue","authors":"Volodymyr Ahunovych,&nbsp;Anton A. Klipkov,&nbsp;Maksym Bugera,&nbsp;Karen Tarasenko,&nbsp;Serhii Trofymchuk,&nbsp;Bohdan Razhyk,&nbsp;Andrii Boretskyi,&nbsp;Oleh Stanko,&nbsp;Yaroslav Panasiuk,&nbsp;Oleh Shablykin,&nbsp;Galeb Al-Maali,&nbsp;Dmytro Lesyk,&nbsp;Oleksii Klymenko-Ulianov,&nbsp;Kateryna Horbatok,&nbsp;Iryna Bodenchuk,&nbsp;Viktoriia Kosach,&nbsp;Petro Borysko,&nbsp;Vladimir Kubyshkin and Pavel K. Mykhailiuk*,&nbsp;","doi":"10.1021/jacsau.4c0086410.1021/jacsau.4c00864","DOIUrl":"https://doi.org/10.1021/jacsau.4c00864https://doi.org/10.1021/jacsau.4c00864","url":null,"abstract":"<p >Isosteric replacement of functional groups is an emerging strategy for optimizing bioactive molecules in drug discovery. <i>tert</i>-Butyl group is a particularly important moiety, yet its isosteric replacement with 1-trifluoromethyl-cyclobutyl group has been rather neglected. To enable the advance of this molecular fragment in drug discovery programs, we report the synthesis of over 30 small-molecule building blocks featuring the trifluoromethyl-cyclobutyl fragment, achieved by reacting sulfur tetrafluoride with cyclobutylcarboxylic acids on a gram-to-multigram scale. Furthermore, we characterized the structural properties of this group through X-ray analysis, studied its effect on acid–base transitions, and evaluated its Hammett parameters. Finally, we evaluated the replacement of <i>tert</i>-butyl with 1-trifluoromethyl-cyclobutyl in several bioactive compounds that represent commercial drugs and agrochemicals. Our findings indicate that while the trifluoromethyl-cyclobutyl group exhibited slightly larger steric size and moderately increased lipophilicity, it preserved the original mode of bioactivity in the examined cases and, in some cases, enhanced resistance to metabolic clearance.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4507–4517 4507–4517"},"PeriodicalIF":8.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00864","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694570","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Design and Evaluation of Pyridinyl Sulfonyl Piperazine LpxH Inhibitors with Potent Antibiotic Activity Against Enterobacterales","authors":"Amanda F. Ennis,&nbsp;C. Skyler Cochrane,&nbsp;Patrick A. Dome,&nbsp;Pyeonghwa Jeong,&nbsp;Jincheng Yu,&nbsp;Hyejin Lee,&nbsp;Carly S. Williams,&nbsp;Yang Ha,&nbsp;Weitao Yang,&nbsp;Pei Zhou* and Jiyong Hong*,&nbsp;","doi":"10.1021/jacsau.4c0073110.1021/jacsau.4c00731","DOIUrl":"https://doi.org/10.1021/jacsau.4c00731https://doi.org/10.1021/jacsau.4c00731","url":null,"abstract":"<p >Enterobacterales, a large order of Gram-negative bacteria, including <i>Escherichia coli</i> and <i>Klebsiella pneumoniae</i>, are major causes of urinary tract and gastrointestinal infections, pneumonia, and other diseases in healthcare settings and communities. ESBL-producing Enterobacterales and carbapenem-resistant Enterobacterales can break down commonly used antibiotics, with some strains being resistant to all available antibiotics. This public health threat necessitates the development of novel antibiotics, ideally targeting new pathways in these bacteria. Gram-negative bacteria possess an outer membrane enriched with lipid A, a saccharolipid that serves as the membrane anchor of lipopolysaccharides and the active component of the bacterial endotoxin, causing septic shock. The biosynthesis of lipid A is crucial for the viability of Gram-negative bacteria, and as an essential enzyme in this process, LpxH has emerged as a promising target for developing novel antibiotics against multidrug-resistant Gram-negative pathogens. Here, we report the development of pyridinyl sulfonyl piperazine LpxH inhibitors. Among them, <i>ortho</i>-substituted pyridinyl compounds significantly boost LpxH inhibition and antibiotic activity over the original phenyl series. Structural and QM/MM analyses reveal that these improved activities are primarily due to the enhanced interaction between F141 of the LpxH insertion lid and the pyridinyl group. Incorporation of the <i>N</i>-methyl-<i>N</i>-phenyl-methanesulfonamide moiety into the pyridinyl sulfonyl piperazine backbone results in JH-LPH-106 and JH-LPH-107, both of which exhibit potent antibiotic activity against wild-type Enterobacterales such as <i>K. pneumoniae</i> and <i>E. coli</i>. JH-LPH-107 exhibits a low rate of spontaneous resistance and a high safety window <i>in vitro</i>, rendering it an excellent lead for further clinical development.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4383–4393 4383–4393"},"PeriodicalIF":8.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00731","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694458","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhanced Carbon Dioxide Capture from Diluted Streams with Functionalized Metal–Organic Frameworks","authors":"Andrzej Gładysiak*,&nbsp;Ah-Young Song,&nbsp;Rebecca Vismara,&nbsp;Madison Waite,&nbsp;Nawal M. Alghoraibi,&nbsp;Ammar H. Alahmed,&nbsp;Mourad Younes,&nbsp;Hongliang Huang,&nbsp;Jeffrey A. Reimer and Kyriakos C. Stylianou*,&nbsp;","doi":"10.1021/jacsau.4c0092310.1021/jacsau.4c00923","DOIUrl":"https://doi.org/10.1021/jacsau.4c00923https://doi.org/10.1021/jacsau.4c00923","url":null,"abstract":"<p >Capturing carbon dioxide from diluted streams, such as flue gas originating from natural gas combustion, can be achieved using recyclable, humidity-resistant porous materials. Three such materials were synthesized by chemically modifying the pores of metal–organic frameworks (MOFs) with Lewis basic functional groups. These materials included aluminum 1,2,4,5-tetrakis(4-carboxylatophenyl) benzene (Al-TCPB) and two novel MOFs: Al-TCPB(OH), and Al-TCPB(NH₂), both isostructural to Al-TCPB, and chemically and thermally stable. Single-component adsorption isotherms revealed significantly increased CO₂ uptakes upon pore functionalization. Breakthrough experiments using a 4/96 CO₂/N₂ gas mixture humidified up to 75% RH at 25 °C showed that Al-TCPB(OH) displayed the highest CO₂ dynamic breakthrough capacity (0.52 mmol/g) followed by that of Al-TCPB(NH₂) (0.47 mmol/g) and Al-TCPB (0.26 mmol/g). All three materials demonstrated excellent recyclability over eight humid breakthrough-regeneration cycles. Solid-state nuclear magnetic resonance spectra revealed that upon CO₂/H₂O loading, H₂O molecules do not interfere with CO₂ physisorption and are localized near the Al-O(H) chain and the –NH₂ functional group, whereas CO₂ molecules are spatially confined in Al-TCPB(OH) and relatively mobile in Al-TCPB(NH₂). Density functional theory calculations confirmed the impact of the adsorbaphore site between of two parallel ligand-forming benzene rings for CO₂ capture. Our study elucidates how pore functionalization influences the fundamental adsorption properties of MOFs, underscoring their practical potential as porous sorbent materials.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4527–4536 4527–4536"},"PeriodicalIF":8.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00923","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694500","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Concise Asymmetric Total Syntheses of (+)-Dihydropleurotinic Acid and (−)-Pleurotin, Enabling Rapid Late-Stage Diversification","authors":"Bin Huang*,&nbsp;Jing Pang,&nbsp;Nan Cao,&nbsp;Ya-Shuang Dai and Ya-Qiu Long*,&nbsp;","doi":"10.1021/jacsau.4c0094210.1021/jacsau.4c00942","DOIUrl":"https://doi.org/10.1021/jacsau.4c00942https://doi.org/10.1021/jacsau.4c00942","url":null,"abstract":"<p >(−)-Pleurotin (<b>1</b>) and (+)-dihydropleurotinic acid (<b>2</b>) are benzoquinone meroterpenoids isolated from fungal sources with powerful antitumor and antibiotic activities. Concise asymmetric total syntheses of the stereochemically pure (+)-dihydropleurotinic acid (<b>2</b>) and (−)-pleurotin (<b>1</b>) from the chiral pool (<i>R</i>)-Roche ester-derived vinyl bromide <b>7</b> have been achieved in 12 and 13 longest linear steps, respectively. The key transformations feature a Michael addition/alkylation cascade reaction to forge three contiguous stereocenters matched with the natural products, a PtO₂-catalyzed stereoselective reduction of olefin to generate the correct stereocenter at C3, a palladium-catalyzed Negishi cross-coupling between triflate and zinc reagent to introduce the redox-sensitive para-quinone moiety, and a hydroboration/copper-catalyzed carboxylation sequence to incorporate the vital carboxyl group. Thus, the highly efficient and scalable preparation of pleurotin’s pentacyclic skeleton enables the late-stage diversification, affording otherwise unavailable pleurotin analogs with significantly improved antiproliferative activities against the thioredoxin reductase (TrxR) overexpressed human breast cancer cell lines relative to the natural product pleurotin (<b>1</b>).</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4206–4211 4206–4211"},"PeriodicalIF":8.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00942","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694503","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Sequence-Encoded Spatiotemporal Dependence of Viscoelasticity of Protein Condensates Using Computational Microrheology","authors":"Dinesh Sundaravadivelu Devarajan*,&nbsp; and ,&nbsp;Jeetain Mittal*,&nbsp;","doi":"10.1021/jacsau.4c0074010.1021/jacsau.4c00740","DOIUrl":"https://doi.org/10.1021/jacsau.4c00740https://doi.org/10.1021/jacsau.4c00740","url":null,"abstract":"<p >Many biomolecular condensates act as viscoelastic complex fluids with distinct cellular functions. Deciphering the viscoelastic behavior of biomolecular condensates can provide insights into their spatiotemporal organization and physiological roles within cells. Although there is significant interest in defining the role of condensate dynamics and rheology in physiological functions, the quantification of their time-dependent viscoelastic properties is limited and is mostly done through experimental rheological methods. Here, we demonstrate that a computational passive probe microrheology technique, coupled with continuum mechanics, can accurately characterize the linear viscoelasticity of condensates formed by intrinsically disordered proteins (IDPs). Using a transferable coarse-grained protein model, we first provide a physical basis for choosing optimal values that define the attributes of the probe particle, namely, its size and interaction strength with the residues in an IDP chain. We show that the technique captures the sequence-dependent viscoelasticity of heteropolymeric IDPs that differ in either sequence charge patterning or sequence hydrophobicity. We also illustrate the technique’s potential in quantifying the spatial dependence of viscoelasticity in heterogeneous IDP condensates. The computational microrheology technique has important implications for investigating the time-dependent rheology of complex biomolecular architectures, resulting in the sequence–rheology–function relationship for condensates.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4394–4405 4394–4405"},"PeriodicalIF":8.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00740","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Development of Oral, Potent, and Selective CK1α Degraders for AML Therapy","authors":"Lu Huang,&nbsp;Lu Chen,&nbsp;Lu Chen,&nbsp;Bo Peng,&nbsp;Lixin Zhou,&nbsp;Yanli Sun,&nbsp;Taiting Shi,&nbsp;Jiayi Lu,&nbsp;Weiye Lin,&nbsp;Yuhang Liu,&nbsp;Linhui Cao,&nbsp;Lanlan Li,&nbsp;Qiangqiang Han,&nbsp;Xi Chen,&nbsp;Ping Yang,&nbsp;Shuo Zhang,&nbsp;Zhe Wang,&nbsp;Jing Yang,&nbsp;Zhixiang Guo*,&nbsp;Baishan Jiang* and Wenchao Lu*,&nbsp;","doi":"10.1021/jacsau.4c0076210.1021/jacsau.4c00762","DOIUrl":"https://doi.org/10.1021/jacsau.4c00762https://doi.org/10.1021/jacsau.4c00762","url":null,"abstract":"<p >Molecular glue degraders (MGDs) are proximity-inducing agents that mediate the cooperative interaction between a target protein and an E3 ligase, introducing an additional layer of specificity beyond that afforded by traditional small molecules. Historically, molecular glues that stabilize protein–protein interactions were often discovered serendipitously. In this study, we leveraged the reprogramming potential of cereblon (CRBN)-based ligands and conducted a CRBN-dependent proliferation screen to identify CRBN-based MGDs capable of inducing the degradation of proteins essential for cell viability. Through our screening and subsequent medicinal chemistry optimization, we identified dCK1α-1 as a potent and selective CK1α-targeting molecular glue degrader. Furthermore, we synthesized an orally active derivative, dCK1α-2, with enhanced pharmacokinetic properties, which exhibited pronounced degradation activity and demonstrated efficacy in mouse models following oral gavage. These findings indicate that phenotypic drug discovery campaigns, in combination with chemically distinct CRBN ligand libraries, can accelerate the development of therapeutically relevant MGDs. Furthermore, the development of dCK1α-1 and dCK1α-2 provides new therapeutic options for cancers with functional p53 signaling and offers valuable chemical tools for future investigations into the role of CK1α.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4423–4434 4423–4434"},"PeriodicalIF":8.5,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00762","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"C2-Linked Arabinose-Functionalized Polystyrene Microbeads Selectively Target Staphylococcus aureus","authors":"Gulab Walke,&nbsp;Cristina Santi,&nbsp;Calum Haydon,&nbsp;Pooja Joshi,&nbsp;Yuiko Takebayashi,&nbsp;Sylvain Rama,&nbsp;Josephine Dorh,&nbsp;Srinivas Hotha*,&nbsp;James Spencer* and M. Carmen Galan*,&nbsp;","doi":"10.1021/jacsau.4c0093110.1021/jacsau.4c00931","DOIUrl":"https://doi.org/10.1021/jacsau.4c00931https://doi.org/10.1021/jacsau.4c00931","url":null,"abstract":"<p >Carbohydrates play pivotal roles in the first stages of microbial infections and can be exploited as decoys to hijack the interactions between bacteria and the host cell. Multivalent glycan probes mimicking the natural presentation of glycans in living cells have been successfully employed to study fundamental carbohydrate/protein interactions in microbial systems; however, most pathogenic glycan receptors exhibit a shared specificity for commonly found sugars present in both healthy and pathogenic cells, posing a challenge for target selectivity. In this study, we report the synthesis of a small library of <span>d</span>-arabinose multivalent probes, a sugar absent in human physiology, and their evaluation in a bacteria agglutination assay using cluster analysis. Our findings reveal preferential binding to <i>Staphylococcus aureus</i> of C2-linked arabinose moieties over C1- or C5-linked probes, underscoring the importance of glycan presentation in targeting specificity. Furthermore, we demonstrate the selectivity of the C2-linked probe toward <i>S. aureus</i> across a panel of common bacterial pathogens. Additionally, these probes are able to disrupt biofilm formation in <i>S. aureus</i> SH1000, thereby further proving the cell surface interactions with <i>S. aureus</i></p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4537–4543 4537–4543"},"PeriodicalIF":8.5,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00931","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Data-Driven Discovery of a New Fluorescent BASHY Dye for Bioimaging","authors":"João M.J.M. Ravasco,&nbsp;João Felicidade,&nbsp;Maria V. Pinto,&nbsp;Fábio M.F. Santos,&nbsp;René Campos-González,&nbsp;Jesús F. Arteaga,&nbsp;Manon Mehraz,&nbsp;Christelle Langevin,&nbsp;Adelaide Fernandes,&nbsp;Ha-Chi Nguyen,&nbsp;David Y.W. Ng,&nbsp;Jaime A.S. Coelho*,&nbsp;Uwe Pischel* and Pedro M.P. Gois*,&nbsp;","doi":"10.1021/jacsau.4c0047310.1021/jacsau.4c00473","DOIUrl":"https://doi.org/10.1021/jacsau.4c00473https://doi.org/10.1021/jacsau.4c00473","url":null,"abstract":"<p >Fluorescent molecules play a crucial role in biomedicine by facilitating the visualization and tracking of biological processes with sensitivity and specificity. However, tailoring their structure to meet the demands of live cell and <i>in vivo</i> imaging presents a significant challenge due to the intricate interplay of factors governing their structural and photophysical properties. In this study, we explored the potential of using multivariate linear free-energy relationships (mLFER) to optimize a multicomponent fluorescent platform. We prepared a small library of 20 fluorescent boronic-acid-derived salicylidenehydrazone (BASHY) complexes using a versatile reaction protocol and characterized their chemical stability in water-containing media. The obtained data served as input for the development of an mLFER model, enabling the prediction of a new BASHY dye and unraveling previously unknown mechanisms governing the stability of this unique platform of fluorescent dyes. The optimized dye was successfully employed in live cell experiments and in zebrafish larvae.</p>","PeriodicalId":94060,"journal":{"name":"JACS Au","volume":"4 11","pages":"4212–4222 4212–4222"},"PeriodicalIF":8.5,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacsau.4c00473","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694425","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}