{"title":"Attomolar Nucleic Acid Detection Using CRISPR Enhanced Phase-Sensitive Surface Plasmon Resonance Imaging.","authors":"Xiaoqi Dai,Changle Meng,Songfeng Huang,Yuye Wang,Jianan He,Zhi Chen,Yinyue Ji,Jiali Tai,Jinming Zhang,Hailong Ni,Zhuolun Zhuang,Jiajie Chen,Han Zhang,Junle Qu,Yonghong Shao","doi":"10.1021/acs.analchem.5c01772","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01772","url":null,"abstract":"Driven by the growing need for real-time, amplification-free, and label-free nucleic acid detection in clinical diagnostics and pathogen surveillance, traditional methods often fall short due to limited sensitivity, a narrow dynamic range, and difficulties in detecting low-concentration nucleic acids and single-nucleotide mutations. To address these challenges, we developed a clustered regularly interspaced short palindromic repeats (CRISPR) enhanced Phase-interrogation Surface Plasmon Resonance imaging (CRISPR-PSPRi) sensor that employs phase delay modulation for highly sensitive extraction of SPR phase signals and a wavelength scanning strategy to extend its dynamic range. By harnessing CRISPR-Cas12a for target DNA recognition and activating trans-cleavage to cleave ssDNA-linked gold nanoparticle probes, our platform converts extremely weak signals from low-concentration DNA into readily detectable cleavage signals. Achieving a sensitivity of 1.436 × 10-6 RIU and a dynamic range of 0.0111 RIU, this system successfully detects specific DNA from the SARS-CoV-2 Omicron BA.2 variant and monkeypox virus, and it can detect single-nucleotide mutations down to 1 aM. This breakthrough offers a real-time, high-throughput, and ultrasensitive nucleic acid detection approach, promising significant advancements in clinical diagnostics and pathogen monitoring.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"115 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684402","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Markus Salbreiter,Annette Wagenhaus,Petra Rösch,Jürgen Popp
{"title":"p-Cresol and C. difficile: A Love-Hate Story Revealed by Raman Spectroscopy.","authors":"Markus Salbreiter,Annette Wagenhaus,Petra Rösch,Jürgen Popp","doi":"10.1021/acs.analchem.5c02927","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02927","url":null,"abstract":"Clostridioides difficile is known to produce p-cresol, a phenolic compound with selective antimicrobial properties, which may contribute to its competitive advantage within the gut microbiome. In this study, we investigated the interaction between Clostrioides difficile and Escherichia coli in coculture to assess the role of p-cresol in modulating interspecies dynamics. Raman spectroscopy was employed as a label-free, nondestructive analytical technique to profile the molecular signatures of both species in mono- and coculture. Excitation wavelengths at 244 and 532 nm were used to enhance complementary vibrational features, including those associated with aromatic compounds like p-cresol. Our results demonstrate distinct spectral changes in coculture conditions suggesting the involvement of p-cresol and its impact on the biochemical composition of E. coli. This dual-wavelength Raman approach offers a powerful means of characterizing microbial interactions and identifying metabolic markers that may drive microbial competition and survival.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"14 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144684403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catia Costa,Johanna von Gerichten,Vladimir Palitsin,Geoffrey W Grime,Steve J Hinder,Naoko Sano,Roger Webb,Melanie J Bailey
{"title":"Multimodal Ion Beam Imaging to Correlate Elements and Metabolites at the Micron Scale Using Water Cluster Secondary Ion Mass Spectrometry and MeV Ion Beam Analysis.","authors":"Catia Costa,Johanna von Gerichten,Vladimir Palitsin,Geoffrey W Grime,Steve J Hinder,Naoko Sano,Roger Webb,Melanie J Bailey","doi":"10.1021/acs.analchem.5c02890","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02890","url":null,"abstract":"Multiomics imaging at or below the single cell level is highly sought after for correlating the location of metal containing drugs, nanoparticles, or bioaccumulated metals with host metabolites and lipids. Secondary ion mass spectrometry (SIMS) is a technique that can image lipids and metabolites at high spatial resolution (∼1 μm), especially water cluster SIMS. Similarly, X-ray mapping techniques such as particle induced X-ray emission (PIXE) can image elements at submicron spatial resolution in tissues. Here we developed a workflow for SIMS followed by X-ray elemental mapping, performed on the same section of tissue. To enable compatibility with X-ray spectrometry, samples were mounted on a thin polymer film, which proved challenging for SIMS due to charge accumulation on the sample surface. Various sample preparation strategies, including carbon coating and metallic grids, were tested to overcome this issue. Multimodal imaging using SIMS and ion beam analysis (IBA) was then successfully performed on a porcine skin section. By way of example, we show how SIMS-IBA can be applied to image the different regions of a hair follicle to colocate elements, metals, and lipids using sequential elemental and molecular mapping, without any delocalization or loss by the preceding measurement.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"25 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693336","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Hydrogen-Bond Duality Underlying the Enthalpy Anomaly in D2O-Ethanol Mixtures.","authors":"Ying Wang,Lu Xing,Chenglin Sun,Fabing Li","doi":"10.1021/acs.analchem.5c03200","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03200","url":null,"abstract":"Thermodynamic anomalies in aqueous ethanol mixtures, such as the well-known enthalpy minimum at intermediate concentrations, have long eluded a clear molecular-level explanation. Here, we employ excess Raman spectroscopy (ERS) and two-dimensional correlation Raman spectroscopy (2DCRS) to track hydrogen-bond transformations in D2O-ethanol mixtures. The spectra reveal two distinct types of hydrogen-bonding interactions formed between ethanol and water molecules near the ethanol volume fraction of 0.4, where the enthalpy minimum occurs. Density functional theory (DFT) calculations indicate that these two types of hydrogen-bond structures correspond to water-like (shorter, linear) and ethanol-like (longer, bent) interactions, respectively, and exhibit distinct electronic characters: one governed by charge-transfer (CT) interactions and the other by local excitation (LE) interactions. The stable coexistence of CT and LE type hydrogen bonds forms a highly coordinated and energetically favorable hydrogen-bonding network, providing direct microscopic insight into the enthalpic anomaly. This study establishes a combined spectroscopic-theoretical framework for resolving thermodynamic features in complex hydrogen-bonded liquids.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"115 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Open Type Solid Photoacoustic Trace Gas Sensor with Multi-Pass Absorption Enhancement.","authors":"Junlin Zhang,Lixian Liu,Jialiang Sun,Xueshi Zhang,Baisong Chen,Yize Liang,Binxing Zhao,Huiting Huan,Xuesen Xu,Huailiang Xu,Andreas Mandelis","doi":"10.1021/acs.analchem.5c03412","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c03412","url":null,"abstract":"A wavelength modulation solid photoacoustic spectroscopic (WM-SPAS) sensor enhanced with an open-type multi-pass cell (OMPC) is reported for highly sensitive detection of trace gases, especially suitable for highly corrosive and long optical-to-thermal (non-radiative) relaxation gaseous species. Such open configuration is quite different from traditional trace gas detection methods in that the separation design of the acoustic signal detector and gas absorption cavity avoids the adversely corrosive effect and reduces signal fluctuations caused by high flow rates. The modulated beam after the optical absorption by the target gas in the designed open-type multi-pass path is directed into a self-designed solid chamber, filled with carbon powder while the photoacoustic (PA) pressure signal is analyzed to yield the target gas concentration. By optimizing the incident beam angle, the OMPC achieves 96 reflections, yielding a 9.6 m optical path length enhancement. Using acetylene (C2H2) as a test sample and a DFB laser as the excitation source, this WM-SPAS sensor achieves sensitivity of 80 ppb and corresponding normalized noise equivalent absorption coefficient equal to 2.42 × 10-9 cm-1 W/Hz-1/2 with 1 s time constant and modulation frequency as low as 39 Hz, which enables the sensor to detect gases with slow non-radiative relaxation. An Allan deviation analysis indicated the minimum detection limit could be further improved to 7 ppb at 100 s integration time. The response deviation of the PA signal under different flow rates was characterized by a coefficient of variation of 0.71‰. With its separate structure design, this newly developed PAS trace gas sensor offers unique advantages for open trace gas detection in high-flow and corrosive environments.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yipei Zhang*, Mark G. Qian, Xuemei Yang and Linlin Dong*,
{"title":"","authors":"Yipei Zhang*, Mark G. Qian, Xuemei Yang and Linlin Dong*, ","doi":"","DOIUrl":"","url":null,"abstract":"","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"97 28","pages":"XXX-XXX XXX-XXX"},"PeriodicalIF":6.7,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.analchem.5c00927","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144671444","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}