Use of electron-beam induced crosslinking to pattern films of monolayer-protected gold nanoparticles (MPNs) onto a chemiresistor (CR) sensor array is described. Each of the four CRs comprises a 100 µm(2) set of interdigital electrodes (IDEs) with 100 nm widths and spaces, separated from adjacent devices by 4 µm. Films of four MPNs, each with a different thiolate monolayer, were successively patterned on the IDEs. Vapor exposures yield rapid, reversible changes in CR resistances and differential vapor sensitivities comparable to those reported for larger CRs with unpatterned MPN films. The array response patterns facilitate vapor discrimination. This is the smallest MPN-coated CR array yet reported. The advantages of using such an array as the detector in microfabricated gas chromatographic analyzers are considered.
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http://dx.doi.org/10.1039/c0lc00071j | DOI Listing |
J Phys Chem A
September 2024
Department of Chemistry, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
The electronic relaxation dynamics of gold monolayer protected clusters (MPCs) are influenced by the hydrocarbon structure of thiolate protecting ligands. Here, we present ligand-dependent electronic relaxation for a series of Au(SR) (SR = SCH, SCH, SCH) MPCs using femtosecond time-resolved transient absorption spectroscopy. Relaxation pathways included a ligand-independent femtosecond internal conversion and a competing ligand-dependent picosecond intersystem crossing process.
View Article and Find Full Text PDFACS Nano
July 2024
Department of Materials Science and Engineering, University of California Berkeley, Berkeley, California 94720, United States.
Monolayer protected metal clusters comprise a rich class of molecular systems and are promising candidate materials for a variety of applications. While a growing number of protected nanoclusters have been synthesized and characterized in crystalline forms, their dynamical behavior in solution, including prenucleation cluster formation, is not well understood due to limitations both in characterization and first-principles modeling techniques. Recent advancements in machine-learned interatomic potentials are rapidly enabling the study of complex interactions such as dynamical behavior and reactivity on the nanoscale.
View Article and Find Full Text PDFNanomaterials (Basel)
May 2024
Department of Chemistry, Gottwald Center for the Sciences, University of Richmond, Richmond, VA 23173, USA.
Fentanyl (FTN) and synthetic analogs of FTN continue to ravage populations across the globe, including in the United States where opioids are increasingly being used and abused and are causing a staggering and growing number of overdose deaths each year. This growing pandemic is worsened by the ease with which FTN can be derivatized into numerous derivatives. Understanding the chemical properties/behaviors of the FTN class of compounds is critical for developing effective chemical detection schemes using nanoparticles (NPs) to optimize important chemical interactions.
View Article and Find Full Text PDFTalanta
August 2024
Department of Chemistry, Louisville, KY, 40292, USA. Electronic address:
Whereas the close associations of cesium ion with organochlorine compounds have been previously documented, the present report is the first attempt to exploit these interactions to create a trichloroethylene (TCE)-selective sensor. Gold monolayer-protected clusters peripherally functionalized with Cs ions were used to prepare a chemiresistance film on MEMS-fabricated interdigitated electrodes. Vapor sensing properties of the cesium-rich chemiresistor were determined using a panel of chlorinated hydrocarbons including TCE as well as polar and non-polar VOCs for comparison.
View Article and Find Full Text PDFBiosensors (Basel)
August 2023
Department of Chemistry, Gottwald Center for the Sciences, University of Richmond, Richmond, VA 23173, USA.
The incorporation of nanomaterials (NMs) into biosensing schemes is a well-established strategy for gaining signal enhancement. With electrochemical biosensors, the enhanced performance achieved from using NMs is often attributed to the specific physical properties of the chosen nanocomponents, such as their high electronic conductivity, size-dependent functionality, and/or higher effective surface-to-volume ratios. First generation amperometric biosensing schemes, typically utilizing NMs in conjunction with immobilized enzyme and semi-permeable membranes, can possess complex sensing mechanisms that are difficult to study and challenging to understand beyond the observable signal enhancement.
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