{"title":"Fluorinated Benzothiadiazole-Based Polymers for Organic Solar Cells: Progress and Prospects","authors":"Zhibo Wang, Shenbo Zhu, Tongzi Li, Wenting Liang, Jiang Zhou and Huawei Hu*, ","doi":"10.1021/acsmaterialsau.4c0009910.1021/acsmaterialsau.4c00099","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00099https://doi.org/10.1021/acsmaterialsau.4c00099","url":null,"abstract":"<p >The integration of fluorinated benzothiadiazole (FBT) into donor–acceptor (D–A) copolymers represents a major advancement in the field of organic solar cells (OSCs). The fluorination process effectively fine-tunes the energy levels, reduces the highest occupied molecular orbital levels, and enhances the open-circuit voltages of the polymers. Furthermore, fluorination improves molecular packing and crystallinity, which significantly boosts the charge transport and overall device performance. This review provides a detailed analysis of the progress made with FBT-based polymers in OSCs, classifying these materials according to their copolymerization units. It discusses the design strategies and structure–property relationships that have emerged as well as the current challenges and future directions for optimizing these polymers. By offering a comprehensive overview of the existing research, this review aims to facilitate the development of high-performance FBT-based organic photovoltaic materials, ultimately contributing to the advancement of sustainable energy solutions.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"57–71 57–71"},"PeriodicalIF":5.7,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00099","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091847","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":"Fluorinated Benzothiadiazole-Based Polymers for Organic Solar Cells: Progress and Prospects.","authors":"Zhibo Wang, Shenbo Zhu, Tongzi Li, Wenting Liang, Jiang Zhou, Huawei Hu","doi":"10.1021/acsmaterialsau.4c00099","DOIUrl":"10.1021/acsmaterialsau.4c00099","url":null,"abstract":"<p><p>The integration of fluorinated benzothiadiazole (FBT) into donor-acceptor (D-A) copolymers represents a major advancement in the field of organic solar cells (OSCs). The fluorination process effectively fine-tunes the energy levels, reduces the highest occupied molecular orbital levels, and enhances the open-circuit voltages of the polymers. Furthermore, fluorination improves molecular packing and crystallinity, which significantly boosts the charge transport and overall device performance. This review provides a detailed analysis of the progress made with FBT-based polymers in OSCs, classifying these materials according to their copolymerization units. It discusses the design strategies and structure-property relationships that have emerged as well as the current challenges and future directions for optimizing these polymers. By offering a comprehensive overview of the existing research, this review aims to facilitate the development of high-performance FBT-based organic photovoltaic materials, ultimately contributing to the advancement of sustainable energy solutions.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"57-71"},"PeriodicalIF":5.7,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11718542/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142972387","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}
ACS Materials AuPub Date : 2024-11-05DOI: 10.1021/acsmaterialsau.4c0010210.1021/acsmaterialsau.4c00102
Uchenna V. Chinaegbomkpa, Xudong Huai, Michal J. Winiarski, Hugo Sanabria and Thao T. Tran*,
{"title":"Chemical Origins of Optically Addressable Spin States in Eu2(P2S6) and Eu2(P2Se6)","authors":"Uchenna V. Chinaegbomkpa, Xudong Huai, Michal J. Winiarski, Hugo Sanabria and Thao T. Tran*, ","doi":"10.1021/acsmaterialsau.4c0010210.1021/acsmaterialsau.4c00102","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00102https://doi.org/10.1021/acsmaterialsau.4c00102","url":null,"abstract":"<p >Lanthanide materials with a 4f<sup>7</sup> electron configuration (<sup>8</sup>S<sub>7/2</sub>) offer an exciting system for realizing multiple addressable spin states for qubit design. While the <sup>8</sup>S<sub>7/2</sub> ground state of 4f<sup>7</sup> free ions displays an isotropic character, breaking degeneracy of this ground state and excited states can be achieved through local symmetry of the lanthanide and the choice of ligands. This makes Eu<sup>2+</sup> attractive as it mirrors Gd<sup>3+</sup> in exhibiting the <sup>8</sup>S<sub>7/2</sub> ground state, capable of seven spin-allowed transitions. In this work, we identify Eu<sub>2</sub>(P<sub>2</sub>S<sub>6</sub>) and Eu<sub>2</sub>(P<sub>2</sub>Se<sub>6</sub>) as viable candidates for optically addressable spin states. The materials feature paramagnetic behavior at 2.0 ≤ <i>T</i> ≤ 400 K and μ<sub>0</sub><i>H</i> = 0.01 and 7 T. The field-dependent magnetization <i>M</i>(<i>H</i>) curve reveals a single-ion spin with effective magnetic moments comparable to the expected magnetic moment of Eu<sup>2+</sup>. Seven well-defined narrow peaks in the excitation and emission spectra of Eu<sup>2+</sup> are resolved. Phonon contributions to the Eu<sup>2+</sup> spin environment are evaluated through heat capacity measurements. Insights into how the spin-polarized band structure and density of states of the materials influence the physical properties are described by using density functional theory calculations. These results present a foundational study of Eu<sub>2</sub>(P<sub>2</sub>S<sub>6</sub>) and Eu<sub>2</sub>(P<sub>2</sub>Se<sub>6</sub>) as a feasible platform for harnessing the spin, charge, orbital, and lattice degrees of freedom of Eu<sup>2+</sup> for qubit design.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"182–190 182–190"},"PeriodicalIF":5.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00102","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091875","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}
ACS Materials AuPub Date : 2024-11-05eCollection Date: 2025-01-08DOI: 10.1021/acsmaterialsau.4c00102
Uchenna V Chinaegbomkpa, Xudong Huai, Michal J Winiarski, Hugo Sanabria, Thao T Tran
{"title":"Chemical Origins of Optically Addressable Spin States in Eu<sub>2</sub>(P<sub>2</sub>S<sub>6</sub>) and Eu<sub>2</sub>(P<sub>2</sub>Se<sub>6</sub>).","authors":"Uchenna V Chinaegbomkpa, Xudong Huai, Michal J Winiarski, Hugo Sanabria, Thao T Tran","doi":"10.1021/acsmaterialsau.4c00102","DOIUrl":"10.1021/acsmaterialsau.4c00102","url":null,"abstract":"<p><p>Lanthanide materials with a 4f<sup>7</sup> electron configuration (<sup>8</sup>S<sub>7/2</sub>) offer an exciting system for realizing multiple addressable spin states for qubit design. While the <sup>8</sup>S<sub>7/2</sub> ground state of 4f<sup>7</sup> free ions displays an isotropic character, breaking degeneracy of this ground state and excited states can be achieved through local symmetry of the lanthanide and the choice of ligands. This makes Eu<sup>2+</sup> attractive as it mirrors Gd<sup>3+</sup> in exhibiting the <sup>8</sup>S<sub>7/2</sub> ground state, capable of seven spin-allowed transitions. In this work, we identify Eu<sub>2</sub>(P<sub>2</sub>S<sub>6</sub>) and Eu<sub>2</sub>(P<sub>2</sub>Se<sub>6</sub>) as viable candidates for optically addressable spin states. The materials feature paramagnetic behavior at 2.0 ≤ <i>T</i> ≤ 400 K and μ<sub>0</sub> <i>H</i> = 0.01 and 7 T. The field-dependent magnetization <i>M</i>(<i>H</i>) curve reveals a single-ion spin with effective magnetic moments comparable to the expected magnetic moment of Eu<sup>2+</sup>. Seven well-defined narrow peaks in the excitation and emission spectra of Eu<sup>2+</sup> are resolved. Phonon contributions to the Eu<sup>2+</sup> spin environment are evaluated through heat capacity measurements. Insights into how the spin-polarized band structure and density of states of the materials influence the physical properties are described by using density functional theory calculations. These results present a foundational study of Eu<sub>2</sub>(P<sub>2</sub>S<sub>6</sub>) and Eu<sub>2</sub>(P<sub>2</sub>Se<sub>6</sub>) as a feasible platform for harnessing the spin, charge, orbital, and lattice degrees of freedom of Eu<sup>2+</sup> for qubit design.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"182-190"},"PeriodicalIF":5.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11718534/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142972349","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}
ACS Materials AuPub Date : 2024-10-31eCollection Date: 2024-11-13DOI: 10.1021/acsmaterialsau.4c00103
Priscila Alessio, Milene K C da Silva, Vitoria Barossi, Celina M Miyazaki
{"title":"Nanostructured Thin Films Enhancing the Performance of New Organic Electronic Devices: Does It Make Sense?","authors":"Priscila Alessio, Milene K C da Silva, Vitoria Barossi, Celina M Miyazaki","doi":"10.1021/acsmaterialsau.4c00103","DOIUrl":"10.1021/acsmaterialsau.4c00103","url":null,"abstract":"<p><p>Electronics have evolved significantly with the development of semiconductor materials and devices, with emerging areas such as organic and flexible electronics showing great promise, particularly in applications such as wearable devices and environmental sensors. Since the discovery of conducting polymers in the late 1970s, organic electronics have paved the way for innovations such as organic field-effect transistors (OFETs), organic light-emitting diodes (OLEDs), and organic solar cells (OPVs). Recent advances have focused on nanostructuring techniques to enhance device properties, such as charge mobility and luminescence efficiency. The growing concern for sustainability has also led to the exploration of biodegradable organic electronics as a potential solution to electronic waste. This perspective briefly discusses the impact of nanostructuring on the performance of both conventional and biodegradable organic devices, exploring the challenges and opportunities associated with using alternative substrates like paper. This perspective emphasizes the importance of understanding molecular organization at the nanoscale to optimize device performance and ensure stability under practical conditions.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"4 6","pages":"574-581"},"PeriodicalIF":5.7,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11565282/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142649105","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}
ACS Materials AuPub Date : 2024-10-30DOI: 10.1021/acsmaterialsau.4c0009010.1021/acsmaterialsau.4c00090
Hanna Z. Porter, Emily E. Foley, Wen Jin, Eric Chen, Erick A. Lawrence, Euan N. Bassey and Raphaële J. Clément*,
{"title":"Impact of Mg Substitution on the Structure, Stability, and Properties of the Na2Fe2F7 Weberite Cathode","authors":"Hanna Z. Porter, Emily E. Foley, Wen Jin, Eric Chen, Erick A. Lawrence, Euan N. Bassey and Raphaële J. Clément*, ","doi":"10.1021/acsmaterialsau.4c0009010.1021/acsmaterialsau.4c00090","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00090https://doi.org/10.1021/acsmaterialsau.4c00090","url":null,"abstract":"<p >Of the few weberite-type Na-ion cathodes explored to date, Na<sub>2</sub>Fe<sub>2</sub>F<sub>7</sub> exhibits the best performance, with capacities up to 184 mAh/g and energy densities up to 550 Wh/kg reported for this material. However, the development of robust structure–property relationships for this material is complicated by its tendency to form as a mixture of metastable polymorphs, and transform to a lower-energy Na<i><sub>y</sub></i>FeF<sub>3</sub> perovskite compound during electrochemical cycling. Our first-principles-guided exploration of Fe-based weberite solid solutions with redox-inactive Mg<sup>2+</sup> and Al<sup>3+</sup> predicts an enhanced thermodynamic stability of Na<sub>2</sub>Mg<i><sub>x</sub></i>Fe<sub>2–<i>x</i></sub> F<sub>7</sub> as the Mg content is increased, and the <i>x</i> = 0.125 composition is selected for further exploration. We demonstrate that the monoclinic polymorph (space group <i>C</i>2/c) of Na<sub>2</sub>Fe<sub>2</sub>F<sub>7</sub> (Mg0) and of a new Mg-substituted weberite composition, Na<sub>2</sub>Mg<sub>0.125</sub>Fe<sub>1.875</sub>F<sub>7</sub> (Mg0.125), can be isolated using an optimized synthesis protocol. The impact of Mg substitution on the stability of the weberite phase during electrochemical cycling, and on the extent and rate of Na (de)intercalation, is examined. Irrespective of the Mg content, we find that the weberite phase is retained when cycling over a narrow voltage window (2.8–4.0 V vs Na/Na<sup>+</sup>). Over a wider voltage range (1.9–4.0 V), Mg0 shows steady capacity fade due to its transformation to the Na<i><sub>y</sub></i>FeF<sub>3</sub> perovskite phase, while Mg0.125 displays more reversible cycling and a reduced phase transformation. Yet, Mg incorporation also leads to kinetically limited Na extraction and a reduced overall capacity. These findings highlight the need for the continued compositional optimization of weberite cathodes to improve their structural stability while maximizing their energy density.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"170–181 170–181"},"PeriodicalIF":5.7,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00090","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091634","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}
ACS Materials AuPub Date : 2024-10-30eCollection Date: 2025-01-08DOI: 10.1021/acsmaterialsau.4c00090
Hanna Z Porter, Emily E Foley, Wen Jin, Eric Chen, Erick A Lawrence, Euan N Bassey, Raphaële J Clément
{"title":"Impact of Mg Substitution on the Structure, Stability, and Properties of the Na<sub>2</sub>Fe<sub>2</sub>F<sub>7</sub> Weberite Cathode.","authors":"Hanna Z Porter, Emily E Foley, Wen Jin, Eric Chen, Erick A Lawrence, Euan N Bassey, Raphaële J Clément","doi":"10.1021/acsmaterialsau.4c00090","DOIUrl":"10.1021/acsmaterialsau.4c00090","url":null,"abstract":"<p><p>Of the few weberite-type Na-ion cathodes explored to date, Na<sub>2</sub>Fe<sub>2</sub>F<sub>7</sub> exhibits the best performance, with capacities up to 184 mAh/g and energy densities up to 550 Wh/kg reported for this material. However, the development of robust structure-property relationships for this material is complicated by its tendency to form as a mixture of metastable polymorphs, and transform to a lower-energy Na <i><sub>y</sub></i> FeF<sub>3</sub> perovskite compound during electrochemical cycling. Our first-principles-guided exploration of Fe-based weberite solid solutions with redox-inactive Mg<sup>2+</sup> and Al<sup>3+</sup> predicts an enhanced thermodynamic stability of Na<sub>2</sub>Mg <i><sub>x</sub></i> Fe<sub>2-<i>x</i></sub> F<sub>7</sub> as the Mg content is increased, and the <i>x</i> = 0.125 composition is selected for further exploration. We demonstrate that the monoclinic polymorph (space group <i>C</i>2/c) of Na<sub>2</sub>Fe<sub>2</sub>F<sub>7</sub> (Mg0) and of a new Mg-substituted weberite composition, Na<sub>2</sub>Mg<sub>0.125</sub>Fe<sub>1.875</sub>F<sub>7</sub> (Mg0.125), can be isolated using an optimized synthesis protocol. The impact of Mg substitution on the stability of the weberite phase during electrochemical cycling, and on the extent and rate of Na (de)intercalation, is examined. Irrespective of the Mg content, we find that the weberite phase is retained when cycling over a narrow voltage window (2.8-4.0 V vs Na/Na<sup>+</sup>). Over a wider voltage range (1.9-4.0 V), Mg0 shows steady capacity fade due to its transformation to the Na <i><sub>y</sub></i> FeF<sub>3</sub> perovskite phase, while Mg0.125 displays more reversible cycling and a reduced phase transformation. Yet, Mg incorporation also leads to kinetically limited Na extraction and a reduced overall capacity. These findings highlight the need for the continued compositional optimization of weberite cathodes to improve their structural stability while maximizing their energy density.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"170-181"},"PeriodicalIF":5.7,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11718529/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142972292","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}
ACS Materials AuPub Date : 2024-10-29DOI: 10.1021/acsmaterialsau.4c0006410.1021/acsmaterialsau.4c00064
Hila Shinar, and , Tali Ilovitsh*,
{"title":"Volumetric Passive Acoustic Mapping and Cavitation Detection of Nanobubbles under Low-Frequency Insonation","authors":"Hila Shinar, and , Tali Ilovitsh*, ","doi":"10.1021/acsmaterialsau.4c0006410.1021/acsmaterialsau.4c00064","DOIUrl":"https://doi.org/10.1021/acsmaterialsau.4c00064https://doi.org/10.1021/acsmaterialsau.4c00064","url":null,"abstract":"<p >Gas bubbles, commonly used in medical ultrasound (US), witness advancements with nanobubbles (NB), providing improved capabilities over microbubbles (MB). NBs offer enhanced penetration into capillaries and the ability to extravasate into tumors following systemic injection, alongside prolonged circulation and persistent acoustic contrast. Low-frequency insonation (<1 MHz) with NBs holds great potential in inducing significant bioeffects, making the monitoring of their acoustic response critical to achieving therapeutic goals. We introduce a US-guided focused US system comprising a one-dimensional (1D) motorized rotating imaging transducer positioned within a low-frequency therapeutic transducer (center frequencies of 105 and 200 kHz), facilitating precise monitoring of NB cavitation activity in three-dimensional (3D) and comparison with MBs. Passive cavitation detection (PCD) revealed frequency-dependent responses, with NBs exhibiting significantly higher stable and inertial cavitation doses compared to MBs of the same gas volume when excited at a center frequency of 105 kHz and peak negative pressures ranging from 100 to 350 kPa. At 200 kHz, MBs showed higher cavitation doses than NBs. PCD showed that 105 kHz enhanced both NBs’ and MBs’ oscillations compared to 200 kHz. The system was further used for 3D passive acoustic mapping (PAM) to provide spatial resolution alongside PCD monitoring. Two-dimensional PAM was captured for each rotation angle and used to generate a complete 3D PAM reconstruction. Experimental results obtained from a tube phantom demonstrated consistent contrast PAM full-width half-maximum (FWHM) as a function of rotation angle, with similar FWHM between MBs and NBs. Frequency-selective PAM maps distinguished between stable and inertial cavitation via the harmonic, ultraharmonic and broadband content, offering insights into cavitation dynamics. These findings highlight NBs’ superior performance at lower frequencies. The developed 3D-PAM technique with a 1D transducer presents a promising technology for real-time, noninvasive monitoring of cavitation-based US therapies.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"159–169 159–169"},"PeriodicalIF":5.7,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsmaterialsau.4c00064","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143091620","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}
ACS Materials AuPub Date : 2024-10-29eCollection Date: 2025-01-08DOI: 10.1021/acsmaterialsau.4c00064
Hila Shinar, Tali Ilovitsh
{"title":"Volumetric Passive Acoustic Mapping and Cavitation Detection of Nanobubbles under Low-Frequency Insonation.","authors":"Hila Shinar, Tali Ilovitsh","doi":"10.1021/acsmaterialsau.4c00064","DOIUrl":"10.1021/acsmaterialsau.4c00064","url":null,"abstract":"<p><p>Gas bubbles, commonly used in medical ultrasound (US), witness advancements with nanobubbles (NB), providing improved capabilities over microbubbles (MB). NBs offer enhanced penetration into capillaries and the ability to extravasate into tumors following systemic injection, alongside prolonged circulation and persistent acoustic contrast. Low-frequency insonation (<1 MHz) with NBs holds great potential in inducing significant bioeffects, making the monitoring of their acoustic response critical to achieving therapeutic goals. We introduce a US-guided focused US system comprising a one-dimensional (1D) motorized rotating imaging transducer positioned within a low-frequency therapeutic transducer (center frequencies of 105 and 200 kHz), facilitating precise monitoring of NB cavitation activity in three-dimensional (3D) and comparison with MBs. Passive cavitation detection (PCD) revealed frequency-dependent responses, with NBs exhibiting significantly higher stable and inertial cavitation doses compared to MBs of the same gas volume when excited at a center frequency of 105 kHz and peak negative pressures ranging from 100 to 350 kPa. At 200 kHz, MBs showed higher cavitation doses than NBs. PCD showed that 105 kHz enhanced both NBs' and MBs' oscillations compared to 200 kHz. The system was further used for 3D passive acoustic mapping (PAM) to provide spatial resolution alongside PCD monitoring. Two-dimensional PAM was captured for each rotation angle and used to generate a complete 3D PAM reconstruction. Experimental results obtained from a tube phantom demonstrated consistent contrast PAM full-width half-maximum (FWHM) as a function of rotation angle, with similar FWHM between MBs and NBs. Frequency-selective PAM maps distinguished between stable and inertial cavitation via the harmonic, ultraharmonic and broadband content, offering insights into cavitation dynamics. These findings highlight NBs' superior performance at lower frequencies. The developed 3D-PAM technique with a 1D transducer presents a promising technology for real-time, noninvasive monitoring of cavitation-based US therapies.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"159-169"},"PeriodicalIF":5.7,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11718533/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142972395","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}
ACS Materials AuPub Date : 2024-10-29eCollection Date: 2025-01-08DOI: 10.1021/acsmaterialsau.4c00118
Kamil Marcisz, Mosayeb Gharakhloo, Damian Jagleniec, Jan Pawlowski, Jan Romanski, Marcin Karbarz
{"title":"Electrochemical Controlling of Double Microgel Layer Formation on an Electrode Surface via an Electrosensitive Inclusion Complex.","authors":"Kamil Marcisz, Mosayeb Gharakhloo, Damian Jagleniec, Jan Pawlowski, Jan Romanski, Marcin Karbarz","doi":"10.1021/acsmaterialsau.4c00118","DOIUrl":"10.1021/acsmaterialsau.4c00118","url":null,"abstract":"<p><p>In this study, we demonstrate the formation of a self-assembled microgel double layer on an electrode surface, utilizing the ability to form electro-responsive, reversible inclusion complexes between microgels modified with ferrocene and β-cyclodextrin in these systems. The bottom layer was based on microgels containing ferrocene moieties and derivatives of cysteine. The presence of the amino acid derivative enabled the formation of the well-packed monolayer on the gold surface through chemisorption, while ferrocene was responsible for electroactivity. The addition of βCD-modified microgel led to the formation of the second monolayer, ultimately creating the double layer. Our investigation focuses on the electrochemically controlled formation and deformation processes of the double microgel layer.</p>","PeriodicalId":29798,"journal":{"name":"ACS Materials Au","volume":"5 1","pages":"191-199"},"PeriodicalIF":5.7,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11718541/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142972386","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}