ACS Central SciencePub Date : 2025-03-27eCollection Date: 2025-04-23DOI: 10.1021/acscentsci.4c02184
Lukas Lüthy, Leon Gabor Sacha Thies, Konstantin Nikolaus Beitl, Moritz Hansen, Joshua McManus, Muhammad Afzal, Lukas Schrangl, Susanne Bloch, Guruprakash Subbiahdoss, Erik Reimhult, Christina Schäffer, Erick M Carreira
{"title":"Synthesis, Microbiology, and Biophysical Characterization of Mutanofactins from the Human Oral Microbiome.","authors":"Lukas Lüthy, Leon Gabor Sacha Thies, Konstantin Nikolaus Beitl, Moritz Hansen, Joshua McManus, Muhammad Afzal, Lukas Schrangl, Susanne Bloch, Guruprakash Subbiahdoss, Erik Reimhult, Christina Schäffer, Erick M Carreira","doi":"10.1021/acscentsci.4c02184","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02184","url":null,"abstract":"<p><p>Mutanofactins are a family of natural products produced by <i>Streptococcus mutans</i> from the human oral microbiome. We report a unified approach to all mutanofactins by developing a total synthesis amenable to diversification. The key to success for the most complex members, mutanofactins 607 and 697, was an acyl ketene based strategy. Access to the family enabled comprehensive biological profiling, where we demonstrate that all mutanofactins are biofilm promoting in <i>Streptococcus mutans</i>. Experiments were extended to other inhabitants of the oral microbiome for the first time: <i>Streptococcus gordonii</i> and <i>Streptococcus oralis</i>, two early colonizers, were similarly affected with mutanofactins being biofilm promoting. Conversely, <i>Veillonella dispar</i> and <i>Fusobacterium nucleatum</i> showed little to no reaction to mutanofactins. Biophysical investigations based on quartz crystal microbalance with dissipation monitoring and atomic force microscopy reveal a previously unknown mucin-mutanofactin 697 interaction. Incubation of a mucin layer with mutanofactin 697 induces a morphology change within the mucin layer, which promotes bacterial adhesion and biofilm formation. This unique property of mutanofactin 697 might be key to early stages of biofilm formation in the human oral microbiome. Combined, an interdisciplinary approach consisting of total synthesis, microbiology and biophysical characterization provides insight into the roles of mutanofactins in the oral microbiome.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"601-611"},"PeriodicalIF":12.7,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12022917/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-26DOI: 10.1021/acscentsci.4c0218410.1021/acscentsci.4c02184
Lukas Lüthy, Leon Gabor Sacha Thies, Konstantin Nikolaus Beitl, Moritz Hansen, Joshua McManus, Muhammad Afzal, Lukas Schrangl, Susanne Bloch, Guruprakash Subbiahdoss, Erik Reimhult*, Christina Schäffer* and Erick M. Carreira*,
{"title":"Synthesis, Microbiology, and Biophysical Characterization of Mutanofactins from the Human Oral Microbiome","authors":"Lukas Lüthy, Leon Gabor Sacha Thies, Konstantin Nikolaus Beitl, Moritz Hansen, Joshua McManus, Muhammad Afzal, Lukas Schrangl, Susanne Bloch, Guruprakash Subbiahdoss, Erik Reimhult*, Christina Schäffer* and Erick M. Carreira*, ","doi":"10.1021/acscentsci.4c0218410.1021/acscentsci.4c02184","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02184https://doi.org/10.1021/acscentsci.4c02184","url":null,"abstract":"<p >Mutanofactins are a family of natural products produced by <i>Streptococcus mutans</i> from the human oral microbiome. We report a unified approach to all mutanofactins by developing a total synthesis amenable to diversification. The key to success for the most complex members, mutanofactins 607 and 697, was an acyl ketene based strategy. Access to the family enabled comprehensive biological profiling, where we demonstrate that all mutanofactins are biofilm promoting in <i>Streptococcus mutans</i>. Experiments were extended to other inhabitants of the oral microbiome for the first time: <i>Streptococcus gordonii</i> and <i>Streptococcus oralis</i>, two early colonizers, were similarly affected with mutanofactins being biofilm promoting. Conversely, <i>Veillonella dispar</i> and <i>Fusobacterium nucleatum</i> showed little to no reaction to mutanofactins. Biophysical investigations based on quartz crystal microbalance with dissipation monitoring and atomic force microscopy reveal a previously unknown mucin–mutanofactin 697 interaction. Incubation of a mucin layer with mutanofactin 697 induces a morphology change within the mucin layer, which promotes bacterial adhesion and biofilm formation. This unique property of mutanofactin 697 might be key to early stages of biofilm formation in the human oral microbiome. Combined, an interdisciplinary approach consisting of total synthesis, microbiology and biophysical characterization provides insight into the roles of mutanofactins in the oral microbiome.</p><p >Mutanofactins are metabolites from the human oral microbiome. Our study includes synthesis, microbiology and biophysics. Key results are effects on mucin and biofilms of commensal bacteria.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"601–611 601–611"},"PeriodicalIF":12.7,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02184","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858425","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-24DOI: 10.1021/acscentsci.4c0191910.1021/acscentsci.4c01919
Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado*, Matthew S. Sigman* and Corey R. J. Stephenson*,
{"title":"Data-Driven Workflow for the Development and Discovery of N-Oxyl Hydrogen Atom Transfer Catalysts","authors":"Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado*, Matthew S. Sigman* and Corey R. J. Stephenson*, ","doi":"10.1021/acscentsci.4c0191910.1021/acscentsci.4c01919","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01919https://doi.org/10.1021/acscentsci.4c01919","url":null,"abstract":"<p ><i>N</i>-oxyl species are promising hydrogen atom transfer (HAT) catalysts to advance C–H bond activation reactions. However, because of the complex structure–activity relationship within the <i>N</i>-oxyl structure, catalyst optimization is a key challenge, particularly for simultaneous improvement across multiple parameters. This paper describes a data-driven approach to optimize <i>N</i>-oxyl hydrogen atom transfer catalysts. A focused library of 50 <i>N</i>-hydroxy compounds was synthesized and characterized by three parameters─oxidation peak potential, HAT reactivity, and stability─to generate a database. Statistical modeling of these activities described by their intrinsic physical organic parameters was used to build predictive models for catalyst discovery and to understand their structure–activity relationships. Virtual screening of 102 synthesizable candidates allowed for rapid identification of several ideal catalyst candidates. These statistical models clearly suggest that <i>N</i>-oxyl substructures bearing an adjacent heteroatom are more optimal HAT catalysts compared to the historical focus, phthalimide-<i>N</i>-oxyl, by striking the best balance among all three target experimental properties.</p><p >Machine learning models revealed that <i>N</i>-oxyl compounds bearing adjacent heteroatoms to carbonyls are more promising hydrogen atom transfer catalysts by striking a balance between multiple parameters.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"592–600 592–600"},"PeriodicalIF":12.7,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01919","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-24eCollection Date: 2025-04-23DOI: 10.1021/acscentsci.4c01919
Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado, Matthew S Sigman, Corey R J Stephenson
{"title":"Data-Driven Workflow for the Development and Discovery of <i>N</i>-Oxyl Hydrogen Atom Transfer Catalysts.","authors":"Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado, Matthew S Sigman, Corey R J Stephenson","doi":"10.1021/acscentsci.4c01919","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01919","url":null,"abstract":"<p><p><i>N</i>-oxyl species are promising hydrogen atom transfer (HAT) catalysts to advance C-H bond activation reactions. However, because of the complex structure-activity relationship within the <i>N</i>-oxyl structure, catalyst optimization is a key challenge, particularly for simultaneous improvement across multiple parameters. This paper describes a data-driven approach to optimize <i>N</i>-oxyl hydrogen atom transfer catalysts. A focused library of 50 <i>N</i>-hydroxy compounds was synthesized and characterized by three parameters-oxidation peak potential, HAT reactivity, and stability-to generate a database. Statistical modeling of these activities described by their intrinsic physical organic parameters was used to build predictive models for catalyst discovery and to understand their structure-activity relationships. Virtual screening of 102 synthesizable candidates allowed for rapid identification of several ideal catalyst candidates. These statistical models clearly suggest that <i>N</i>-oxyl substructures bearing an adjacent heteroatom are more optimal HAT catalysts compared to the historical focus, phthalimide-<i>N</i>-oxyl, by striking the best balance among all three target experimental properties.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"592-600"},"PeriodicalIF":12.7,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12022910/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143950963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-18DOI: 10.1021/acscentsci.5c0002210.1021/acscentsci.5c00022
Ruibing Lv, Lei Sun, Zhenghang Luo, Yujie Song, Shuo Li and Qi Zhang,
{"title":"Host–Guest Synergy of Metal–Organic Frameworks for Enhanced Near-Infrared Ultrafast Laser Responsiveness","authors":"Ruibing Lv, Lei Sun, Zhenghang Luo, Yujie Song, Shuo Li and Qi Zhang, ","doi":"10.1021/acscentsci.5c0002210.1021/acscentsci.5c00022","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00022https://doi.org/10.1021/acscentsci.5c00022","url":null,"abstract":"<p >Host–guest metal–organic frameworks (MOFs) offer significant potential and value in regulating and optimizing novel material properties and functionalities, owing to the synergistic effects between the host framework and the guest units. This study reported two silver-based host–guest MOFs, [Ag(ATRZ)(BrO<sub>3</sub>)]<sub>n</sub> (CMOF-1) and [Ag(ATRZ)<sub>1.5</sub>(ClO<sub>4</sub>)]<sub>n</sub> (CMOF-2), as promising candidates for laser-responsive materials. These materials feature 1D and 3D structures, respectively, comprising Ag-ATRZ cationic MOF frameworks integrated with two distinct oxidizing anionic guests, BrO<sub>3</sub><sup>–</sup> and ClO<sub>4</sub><sup>–</sup>. CMOF-1 and CMOF-2 are synthesized through straightforward, environmentally benign methods, enabling rapid fabrication. The exceptional near-infrared (NIR) laser responsiveness of CMOF-1 and CMOF-2 was achieved through the modulation of the cationic MOFs (CMOFs) architectures and synergistic interactions between the host and guest components. Moreover, both exhibit ultrafast deflagration-to-detonation transition (DDT) capabilities, alongside excellent thermal stability. This work expands the application scope of host–guest MOFs, and provides an effective strategy for developing high-performance laser-responsive materials.</p><p >This study reports Ag-based host−guest MOFs with ultrafast NIR laser responsiveness: CMOF-1 and CMOF-2, which exhibit excellent ultrafast deflagration-to-detonation transition and thermal stability.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"583–591 583–591"},"PeriodicalIF":12.7,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Host-Guest Synergy of Metal-Organic Frameworks for Enhanced Near-Infrared Ultrafast Laser Responsiveness.","authors":"Ruibing Lv, Lei Sun, Zhenghang Luo, Yujie Song, Shuo Li, Qi Zhang","doi":"10.1021/acscentsci.5c00022","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00022","url":null,"abstract":"<p><p>Host-guest metal-organic frameworks (MOFs) offer significant potential and value in regulating and optimizing novel material properties and functionalities, owing to the synergistic effects between the host framework and the guest units. This study reported two silver-based host-guest MOFs, [Ag(ATRZ)(BrO<sub>3</sub>)]<sub>n</sub> (CMOF-1) and [Ag(ATRZ)<sub>1.5</sub>(ClO<sub>4</sub>)]<sub>n</sub> (CMOF-2), as promising candidates for laser-responsive materials. These materials feature 1D and 3D structures, respectively, comprising Ag-ATRZ cationic MOF frameworks integrated with two distinct oxidizing anionic guests, BrO<sub>3</sub> <sup>-</sup> and ClO<sub>4</sub> <sup>-</sup>. CMOF-1 and CMOF-2 are synthesized through straightforward, environmentally benign methods, enabling rapid fabrication. The exceptional near-infrared (NIR) laser responsiveness of CMOF-1 and CMOF-2 was achieved through the modulation of the cationic MOFs (CMOFs) architectures and synergistic interactions between the host and guest components. Moreover, both exhibit ultrafast deflagration-to-detonation transition (DDT) capabilities, alongside excellent thermal stability. This work expands the application scope of host-guest MOFs, and provides an effective strategy for developing high-performance laser-responsive materials.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"583-591"},"PeriodicalIF":12.7,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12022905/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-18eCollection Date: 2025-04-23DOI: 10.1021/acscentsci.5c00012
Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek, Alanna Schepartz
{"title":"Hastened Fusion-Dependent Endosomal Escape Improves Activity of Delivered Enzyme Cargo.","authors":"Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek, Alanna Schepartz","doi":"10.1021/acscentsci.5c00012","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00012","url":null,"abstract":"<p><p>There is enormous interest in strategies to traffic biologics into the mammalian cell cytosol. Not only must these materials reach the appropriate cellular locale intact and in therapeutically relevant concentrations, they must also retain activity upon arrival. The question of residual activity is especially critical when delivery involves the late endocytic pathway, whose acidic environment can denature and/or degrade internalized material. ZF5.3 is a compact mini-protein that escapes efficiently from late endocytic vesicles, with or without covalently linked protein cargo. Here, we redesign the sequence of ZF5.3 to hasten the timing of endosomal escape. The new mini-protein we describe, AV5.3, escapes earlier than ZF5.3 along the endocytic pathway with no loss in efficiency, with or without enzyme cargo. More importantly, earlier endosomal escape translates into higher enzymatic activity of a pH-sensitive enzyme upon arrival in the cytosol. Delivery of the pH-sensitive enzyme DHFR with AV5.3 results in substantial catalytic activity in the cytosol, whereas delivery with ZF5.3 does not. The activity of delivered AV5.3-DHFR successfully rescues a DHFR deletion in CHO cells. AV5.3 represents an improved strategy for the efficient and direct delivery of active therapeutic proteins and enzymes.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"574-582"},"PeriodicalIF":12.7,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12022911/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143950959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-17DOI: 10.1021/acscentsci.5c0001210.1021/acscentsci.5c00012
Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek and Alanna Schepartz*,
{"title":"Hastened Fusion-Dependent Endosomal Escape Improves Activity of Delivered Enzyme Cargo","authors":"Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek and Alanna Schepartz*, ","doi":"10.1021/acscentsci.5c0001210.1021/acscentsci.5c00012","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00012https://doi.org/10.1021/acscentsci.5c00012","url":null,"abstract":"<p >There is enormous interest in strategies to traffic biologics into the mammalian cell cytosol. Not only must these materials reach the appropriate cellular locale intact and in therapeutically relevant concentrations, they must also retain activity upon arrival. The question of residual activity is especially critical when delivery involves the late endocytic pathway, whose acidic environment can denature and/or degrade internalized material. ZF5.3 is a compact mini-protein that escapes efficiently from late endocytic vesicles, with or without covalently linked protein cargo. Here, we redesign the sequence of ZF5.3 to hasten the timing of endosomal escape. The new mini-protein we describe, AV5.3, escapes earlier than ZF5.3 along the endocytic pathway with no loss in efficiency, with or without enzyme cargo. More importantly, earlier endosomal escape translates into higher enzymatic activity of a pH-sensitive enzyme upon arrival in the cytosol. Delivery of the pH-sensitive enzyme DHFR with AV5.3 results in substantial catalytic activity in the cytosol, whereas delivery with ZF5.3 does not. The activity of delivered AV5.3-DHFR successfully rescues a DHFR deletion in CHO cells. AV5.3 represents an improved strategy for the efficient and direct delivery of active therapeutic proteins and enzymes.</p><p >Rational redesign of a zinc finger mini-protein delivery agent hastens the timing of endosomal escape and avoids irreversible denaturation of enzyme cargo in late endocytic vesicles.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"574–582 574–582"},"PeriodicalIF":12.7,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00012","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-14DOI: 10.1021/acscentsci.4c0215710.1021/acscentsci.4c02157
Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte and Frank Würthner*,
{"title":"Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates","authors":"Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte and Frank Würthner*, ","doi":"10.1021/acscentsci.4c0215710.1021/acscentsci.4c02157","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02157https://doi.org/10.1021/acscentsci.4c02157","url":null,"abstract":"<p >Tunability of functional properties in a continuous manner is desired but challenging to accomplish for organic solid-state materials. Herein, we describe a method for tuning optoelectronic properties of solid-state aggregates with narrow absorption bands. First, we systematically shift the absorption maxima of highly dipolar merocyanine dyes in solution by chemical alterations of their chromophore cores. This leaves their solid-state packing arrangements unchanged, affording similar J- and H-coupled aggregate absorption bands at different wavelengths. Next, mixing these isostructural dyes leads to a spectral fine-tuning of the mixed layers, which could be characterized as crystalline organic solid solutions and utilized in narrowband color-selective organic photodiodes. Finally, we devise a semiempirical model, which explains the observed spectral tuning in terms of the molecular exciton theory. Thus, we demonstrate narrowband absorbing solid-state aggregates spanning the wavelength range of 437–760 nm, whose absorption can be fine-tuned over 40% of the visible light range.</p><p >Spectral tuning of absorption properties for color sensing is achieved by design of isostructural compounds and binary mixtures thereof, which self-assemble into identical supramolecular aggregates.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"452–464 452–464"},"PeriodicalIF":12.7,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02157","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
ACS Central SciencePub Date : 2025-03-14eCollection Date: 2025-03-26DOI: 10.1021/acscentsci.4c02157
Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte, Frank Würthner
{"title":"Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates.","authors":"Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte, Frank Würthner","doi":"10.1021/acscentsci.4c02157","DOIUrl":"10.1021/acscentsci.4c02157","url":null,"abstract":"<p><p>Tunability of functional properties in a continuous manner is desired but challenging to accomplish for organic solid-state materials. Herein, we describe a method for tuning optoelectronic properties of solid-state aggregates with narrow absorption bands. First, we systematically shift the absorption maxima of highly dipolar merocyanine dyes in solution by chemical alterations of their chromophore cores. This leaves their solid-state packing arrangements unchanged, affording similar J- and H-coupled aggregate absorption bands at different wavelengths. Next, mixing these isostructural dyes leads to a spectral fine-tuning of the mixed layers, which could be characterized as crystalline organic solid solutions and utilized in narrowband color-selective organic photodiodes. Finally, we devise a semiempirical model, which explains the observed spectral tuning in terms of the molecular exciton theory. Thus, we demonstrate narrowband absorbing solid-state aggregates spanning the wavelength range of 437-760 nm, whose absorption can be fine-tuned over 40% of the visible light range.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"452-464"},"PeriodicalIF":12.7,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950854/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}