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Development of Highly Sensitive Raman Spectroscopy for Subnano and Single-Atom Detection.

ABSTRACT: Direct detection and characterisation of small materials are fundamental challenges in analytical chemistry. A particle composed of dozens of metallic atoms, a so-called subnano-particle (SNP), and a single-atom catalyst (SAC) are ultimate analysis targets in terms of size, and the topic is now attracting increasing attention as innovative frontier materials in catalysis science. However, characterisation techniques for the SNP and SAC adsorbed on substrates requires sophisticated and large-scale analytical facilities. Here we demonstrate the development of an ultrasensitive, laboratory-scale, vibrational spectroscopic technique to characterise SNPs and SACs. The fine design of nano-spatial local enhancement fields generated by the introduction of anisotropic stellate-shaped signal amplifiers expands the accessibility of small targets on substrates into evanescent electromagnetic fields, achieving not only the detection of isolated small targets but also revealing the effects of intermolecular/interatomic interactions within the subnano configuration under actual experimental conditions. Such a development of "in situ subnano spectroscopy" will facilitate a comprehensive understanding of subnano and SAC science.

SUBMITTER: Tang Y

PROVIDER: S-EPMC8400086 | biostudies-literature | 2021 Aug

REPOSITORIES: biostudies-literature

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Development of Highly Sensitive Raman Spectroscopy for Subnano and Single-Atom Detection.

Tang Yuansen Y Haruta Naoki N Kuzume Akiyoshi A Yamamoto Kimihisa K

Molecules (Basel, Switzerland) 20210823 16

Direct detection and characterisation of small materials are fundamental challenges in analytical chemistry. A particle composed of dozens of metallic atoms, a so-called subnano-particle (SNP), and a single-atom catalyst (SAC) are ultimate analysis targets in terms of size, and the topic is now attracting increasing attention as innovative frontier materials in catalysis science. However, characterisation techniques for the SNP and SAC adsorbed on substrates requires sophisticated and large-scal ...[more]

PMID: 34443684

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Project description:We report the demonstration of an optofluidic surface enhanced Raman spectroscopy (SERS) device that leverages a nanoporous microfluidic matrix to improve the SERS detection performance by more than two orders of magnitude as compared to a typical open microfluidic channel. Although it is a growing trend to integrate optical biosensors into microfluidic channels, this basic combination has been detrimental to the sensing performance when applied to SERS. Recently, however, synergistic combinations between microfluidic functions and photonics (i.e., optofluidics) have been implemented that improve the detection performance of SERS. Conceptually, the simplest optofluidic SERS techniques reported to date utilize a single nanofluidic channel to trap nanoparticle-analyte conjugates as a method of preconcentration before detection. In this work, we leverage this paradigm while improving upon the simplicity by forming a 3D nanofluidic network with packed nanoporous silica microspheres in a microfluidic channel; this creates a concentration matrix that traps silver nanoclusters and adsorbed analytes into the SERS detection volume. With this approach, we are able to achieve a detection limit of 400 attomoles of Rhodamine 6G after only 2 min of sample loading with high chip-to-chip repeatability. Due to the high number of fluidic paths in the nanoporous channel, this approach is less prone to clogging than single nanofluidic inlets, and the loading time is decreased compared to previous reports. In addition, fabrication of this microsystem is quite simple, as nanoscale fabrication is not necessary. Finally, integrated multimode fiber optic cables eliminate the need for optical alignment, and thus the device is relevant for portable and automated applications in the field, including point-of-sample and point-of-care detection. To illustrate a relevant field-based application, we demonstrate the detection of 12 ppb of the organophosphate malathion in water using the nanofluidic SERS microsystem.

Dataset Information

Development of Highly Sensitive Raman Spectroscopy for Subnano and Single-Atom Detection.

Publications

Development of Highly Sensitive Raman Spectroscopy for Subnano and Single-Atom Detection.

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