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Applications of Raman Spectroscopy in Sensors

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A special issue of Sensors (ISSN 1424-8220). This special issue belongs to the section "Chemical Sensors".

Deadline for manuscript submissions: closed (31 October 2018) | Viewed by 68682

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Prof. Dr. Aris Docoslis

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Department of Chemical Engineering, Queen's University, Kingston, ON, Canada
Interests: raman spectroscopy; surface-based sensors; biosensors; electrokinetics; interfacial phenomena; colloidal assembly
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

As a non-invasive/non-destructive technique that can provide qualitative and quantitative information on the chemical content of samples, Raman spectroscopy lends itself to the development of (bio)chemical sensors that can serve, among others, in point-of-care diagnosis, in situ identification of food contaminants and detection of narcotics and terrorism agents (viruses, explosives). Raman spectroscopy, offers key advantages in the field of sensor development, such as sensitive and label-free identification of (bio)chemical compounds through their unique vibrational “fingerprints”, minimal sample preparation, user friendliness and miniaturization potential. Moreover, powerful Raman techniques, such as Surface-enhanced Raman Scattering (SERS), Surface-enhanced Resonance Raman Scattering (SERRS), Tip-enhanced Raman Scattering (TERS) can produce theoretically up to a 10¹⁴-fold signal enhancement, thus reaching single-molecule detection capabilities.

For this Special Issue, we invite both reviews and original research articles discussing novel Raman-based (bio)chemical sensing techniques that can be applied to analyte detection, quantification, or mapping. Research articles may focus on the use of Raman-based sensors in biological analysis, medical diagnostics, illicit drug detection, science, public safety, or food and water quality inspection. Chemical, colloidal, nanofabrication or other methods that can lead to ultrasensitive analyte detection through Raman signal enhancement (e.g., ultrasensitive SERS substrates) are welcome. Of special interest are applications of Raman spectroscopy with the potential to lead to miniaturized sensors, such as microfluidic (Lab-on-a-chip) devices, portable/handheld Raman sensors for point-of-need applications, etc. Reviews must offer a critical and up-to-date overview of the state of the art in a particular application, or discuss present and future challenges of Raman-based sensors (limit of detection, multiplexing, detection in complex matrices, etc.).

Should you require clarifications, or wish to discuss your submission in advance, we encourage you to contact us. We are looking forward to receiving your contribution to this Special Issue.

Prof. Aris Docoslis
Guest Editor

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Keywords

Raman-based sensors
SERS
SERRS
SRS
Raman mapping
Multiphoton Raman spectroscopy imaging
Portable sensors
Microfluidic sensors
In situ diagnostics
Point-of-need sensors
Standoff detection
Illicit drug and cannabis detection
Food and water quality monitoring
Homeland security
Multivariate analysis in sensing

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Published Papers (11 papers)

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Research

19 pages, 11965 KiB

Open AccessArticle

Monitoring Candida parapsilosis and Staphylococcus epidermidis Biofilms by a Combination of Scanning Electron Microscopy and Raman Spectroscopy

by Kamila Hrubanova, Vladislav Krzyzanek, Jana Nebesarova, Filip Ruzicka, Zdenek Pilat and Ota Samek

Sensors 2018, 18(12), 4089; https://doi.org/10.3390/s18124089 - 22 Nov 2018

Cited by 25 | Viewed by 7214

Abstract

The biofilm-forming microbial species Candida parapsilosis and Staphylococcus epidermidis have been recently linked to serious infections associated with implanted medical devices. We studied microbial biofilms by high resolution scanning electron microscopy (SEM), which allowed us to visualize the biofilm structure, including the distribution of cells inside the extracellular matrix and the areas of surface adhesion. We compared classical SEM (chemically fixed samples) with cryogenic SEM, which employs physical sample preparation based on plunging the sample into various liquid cryogens, as well as high-pressure freezing (HPF). For imaging the biofilm interior, we applied the freeze-fracture technique. In this study, we show that the different means of sample preparation have a fundamental influence on the observed biofilm structure. We complemented the SEM observations with Raman spectroscopic analysis, which allowed us to assess the time-dependent chemical composition changes of the biofilm in vivo. We identified the individual spectral peaks of the biomolecules present in the biofilm and we employed principal component analysis (PCA) to follow the temporal development of the chemical composition. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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15 pages, 4540 KiB

Open AccessArticle

Sensitive and Reproducible Gold SERS Sensor Based on Interference Lithography and Electrophoretic Deposition

by June Sik Hwang and Minyang Yang

Sensors 2018, 18(11), 4076; https://doi.org/10.3390/s18114076 - 21 Nov 2018

Cited by 24 | Viewed by 6914

Abstract

Surface-enhanced Raman spectroscopy (SERS) is a promising analytical tool due to its label-free detection ability and superior sensitivity, which enable the detection of single molecules. Since its sensitivity is highly dependent on localized surface plasmon resonance, various methods have been applied for electric field-enhanced metal nanostructures. Despite the intensive research on practical applications of SERS, fabricating a sensitive and reproducible SERS sensor using a simple and low-cost process remains a challenge. Here, we report a simple strategy to produce a large-scale gold nanoparticle array based on laser interference lithography and the electrophoretic deposition of gold nanoparticles, generated through a pulsed laser ablation in liquid process. The fabricated gold nanoparticle array produced a sensitive, reproducible SERS signal, which allowed Rhodamine 6G to be detected at a concentration as low as 10⁻⁸ M, with an enhancement factor of 1.25 × 10⁵. This advantageous fabrication strategy is expected to enable practical SERS applications. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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8 pages, 2471 KiB

Open AccessArticle

Tip-Enhanced Raman Spectroscopy with High-Order Fiber Vector Beam Excitation

by Fanfan Lu, Tengxiang Huang, Lei Han, Haisheng Su, Heng Wang, Min Liu, Wending Zhang, Xiang Wang and Ting Mei

Sensors 2018, 18(11), 3841; https://doi.org/10.3390/s18113841 - 9 Nov 2018

Cited by 21 | Viewed by 5655

Abstract

We investigated tip-enhanced Raman spectra excited by high-order fiber vector beams. Theoretical analysis shows that the high-order fiber vector beams have stronger longitudinal electric field components than linearly polarized light under tight focusing conditions. By introducing the high-order fiber vector beams and the linearly polarized beam from a fiber vector beam generator based on an electrically-controlled acoustically-induced fiber grating into a top-illumination tip-enhanced Raman spectroscopy (TERS) setup, the tip-enhanced Raman signal produced by the high-order fiber vector beams was 1.6 times as strong as that produced by the linearly polarized light. This result suggests a new type of efficient excitation light beams for TERS. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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16 pages, 2794 KiB

Open AccessArticle

Improving the Surface-Enhanced Raman Scattering Performance of Silver Nanodendritic Substrates with Sprayed-On Graphene-Based Coatings

by Aida Mohammadi, Danielle Lilly Nicholls and Aristides Docoslis

Sensors 2018, 18(10), 3404; https://doi.org/10.3390/s18103404 - 11 Oct 2018

Cited by 20 | Viewed by 5165

Abstract

This study examines the improvements in surface-enhanced Raman scattering (SERS) performance achieved when silver nanodendritic structures are coated with various graphene-based materials, namely graphene oxide (GO), reduced graphene oxide (rGO), and graphene nanoplatelets (GNPs). The tests are performed on our unique SERS-active substrates, prepared on the surface of planar microelectrode chips using an electric field-guided Ag nanoparticle assembly process. The graphene-based materials are introduced into the substrate by means of an in-house spray-coating technique. The SERS enhancement effect of each coating is examined as a function of spray nozzle passes (N) and optimal values are identified for each coating type. The enhancements found for GO, rGO, and GNP (6–9 graphene layers thick) coatings are 2.3 (N = 25), 2.5 (N = 5), and 1.6 (N = 1), respectively. Additionally, in comparison with their uncoated counterparts, substrates coated with rGO (N = 5) are shown to enhance the intensity of the methamphetamine (5 ppb) spectrum in artificial saliva by approximately 3-fold. Overall, it can be concluded that the introduction of GO or rGO to the SERS substrate using spray-coating, a simple and also scalable method, can produce substantial SERS performance enhancement. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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13 pages, 3050 KiB

Open AccessArticle

Development of a Gas-Tight Microfluidic System for Raman Sensing of Single Pulmonary Arterial Smooth Muscle Cells Under Normoxic/Hypoxic Conditions

by Fenja Knoepp, Joel Wahl, Anders Andersson, Johan Borg, Norbert Weissmann and Kerstin Ramser

Sensors 2018, 18(10), 3238; https://doi.org/10.3390/s18103238 - 26 Sep 2018

Cited by 3 | Viewed by 3630

Abstract

Acute hypoxia changes the redox-state of pulmonary arterial smooth muscle cells (PASMCs). This might influence the activity of redox-sensitive voltage-gated K⁺-channels (Kv-channels) whose inhibition initiates hypoxic pulmonary vasoconstriction (HPV). However, the molecular mechanism of how hypoxia—or the subsequent change in the cellular redox-state—inhibits Kv-channels remains elusive. For this purpose, a new multifunctional gas-tight microfluidic system was developed enabling simultaneous single-cell Raman spectroscopic studies (to sense the redox-state under normoxic/hypoxic conditions) and patch-clamp experiments (to study the Kv-channel activity). The performance of the system was tested by optically recording the O₂-content and taking Raman spectra on murine PASMCs under normoxic/hypoxic conditions or in the presence of H₂O₂. Oxygen sensing showed that hypoxic levels in the gas-tight microfluidic system were achieved faster, more stable and significantly lower compared to a conventional open system (1.6 ± 0.2%, respectively 6.7 ± 0.7%, n = 6, p < 0.001). Raman spectra revealed that the redistribution of biomarkers (cytochromes, FeS, myoglobin and NADH) under hypoxic/normoxic conditions were improved in the gas-tight microfluidic system (p-values from 0.00% to 16.30%) compared to the open system (p-value from 0.01% to 98.42%). In conclusion, the new redox sensor holds promise for future experiments that may elucidate the role of Kv-channels during HPV. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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18 pages, 5368 KiB

Open AccessArticle

Detection of Chloroalkanes by Surface-Enhanced Raman Spectroscopy in Microfluidic Chips

by Zdeněk Pilát, Martin Kizovský, Jan Ježek, Stanislav Krátký, Jaroslav Sobota, Martin Šiler, Ota Samek, Tomáš Buryška, Pavel Vaňáček, Jiří Damborský, Zbyněk Prokop and Pavel Zemánek

Sensors 2018, 18(10), 3212; https://doi.org/10.3390/s18103212 - 23 Sep 2018

Cited by 9 | Viewed by 6170

Abstract

Optofluidics, a research discipline combining optics with microfluidics, currently aspires to revolutionize the analysis of biological and chemical samples, e.g., for medicine, pharmacology, or molecular biology. In order to detect low concentrations of analytes in water, we have developed an optofluidic device containing a nanostructured substrate for surface enhanced Raman spectroscopy (SERS). The geometry of the gold surface allows localized plasmon oscillations to give rise to the SERS effect, in which the Raman spectral lines are intensified by the interaction of the plasmonic field with the electrons in the molecular bonds. The SERS substrate was enclosed in a microfluidic system, which allowed transport and precise mixing of the analyzed fluids, while preventing contamination or abrasion of the highly sensitive substrate. To illustrate its practical use, we employed the device for quantitative detection of persistent environmental pollutant 1,2,3-trichloropropane in water in submillimolar concentrations. The developed sensor allows fast and simple quantification of halogenated compounds and it will contribute towards the environmental monitoring and enzymology experiments with engineered haloalkane dehalogenase enzymes. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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11 pages, 3950 KiB

Open AccessArticle

Distance-Resolving Raman Radar Based on a Time-Correlated CMOS Single-Photon Avalanche Diode Line Sensor

by Jere Kekkonen, Jan Nissinen, Juha Kostamovaara and Ilkka Nissinen

Sensors 2018, 18(10), 3200; https://doi.org/10.3390/s18103200 - 21 Sep 2018

Cited by 11 | Viewed by 5483

Abstract

Remote Raman spectroscopy is widely used to detect minerals, explosives and air pollution, for example. One of its main problems, however, is background radiation that is caused by ambient light and sample fluorescence. We present here, to the best of our knowledge, the first time a distance-resolving Raman radar device that is based on an adjustable, time-correlated complementary metal-oxide-semiconductor (CMOS) single-photon avalanche diode line sensor which can measure the location of the target sample simultaneously with the normal stand-off spectrometer operation and suppress the background radiation dramatically by means of sub-nanosecond time gating. A distance resolution of 3.75 cm could be verified simultaneously during normal spectrometer operation and Raman spectra of titanium dioxide were distinguished by this system at distances of 250 cm and 100 cm with illumination intensities of the background of 250 lux and 7600 lux, respectively. In addition, the major Raman peaks of olive oil, which has a fluorescence-to-Raman signal ratio of 33 and a fluorescence lifetime of 2.5 ns, were distinguished at a distance of 30 cm with a 250 lux background illumination intensity. We believe that this kind of time-correlated CMOS single-photon avalanche diode sensor could pave the way for new compact distance-resolving Raman radars for application where distance information within a range of several metres is needed at the same time as a Raman spectrum. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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11 pages, 4224 KiB

Open AccessArticle

Preparation of Quasi-Three-Dimensional Porous Ag and Ag-NiO Nanofibrous Mats for SERS Application

by Huixiang Wu, Xiangcheng Sun, Changjun Hou, Jingzhou Hou and Yu Lei

Sensors 2018, 18(9), 2862; https://doi.org/10.3390/s18092862 - 30 Aug 2018

Cited by 18 | Viewed by 3831

Abstract

In this study, two new quasi-three-dimensional Surface Enhanced Raman Scattering (SERS) substrates, namely porous Ag and Ag-NiO nanofibrous mats, were prepared using a simple, electrospinning-calcination, two-step synthetic process. AgNO₃/polyvinyl pyrrolidone (PVP) and AgNO₃/Ni(NO₃)₂/PVP composites serving as precursors were electrospun to form corresponding precursory nanofibers. Porous Ag and Ag-NiO nanofibers were successfully obtained after a 3-h calcination at 500 °C under air atmosphere, and analyzed using various material characterization techniques. Synthesized, quasi-three-dimensional porous Ag and Ag-NiO nanofibrous mats were applied as SERS substrates, to measure the model compound Rhodamine 6G (R6G), and investigate the corresponding signal enhancement. Furthermore, porous Ag and Ag-NiO nanofibrous mats were employed as SERS substrates for melamine and methyl parathion respectively. Sensitive detection of melamine and methyl parathion was achieved, indicating their feasibility as an active SERS sensing platform, and potential for food safety and environmental monitoring. All the results suggest that the electrospinning-calcination, two-step method offers a new, low cost, high performance solution in the preparation of SERS substrates. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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11 pages, 2360 KiB

Open AccessArticle

Direct Detection of Toxic Contaminants in Minimally Processed Food Products Using Dendritic Surface-Enhanced Raman Scattering Substrates

by Hannah Dies, Maria Siampani, Carlos Escobedo and Aristides Docoslis

Sensors 2018, 18(8), 2726; https://doi.org/10.3390/s18082726 - 19 Aug 2018

Cited by 39 | Viewed by 7079

Abstract

We present a method for the surface-enhanced Raman scattering (SERS)-based detection of toxic contaminants in minimally processed liquid food products, through the use of a dendritic silver nanostructure, produced through electrokinetic assembly of nanoparticles from solution. The dendritic nanostructure is produced on the surface of a microelectrode chip, connected to an AC field with an imposed DC bias. We apply this chip for the detection of thiram, a toxic fruit pesticide, in apple juice, to a limit of detection of 115 ppb, with no sample preprocessing. We also apply the chip for the detection of melamine, a toxic contaminant/food additive, to a limit of detection of 1.5 ppm in milk and 105 ppb in infant formula. All the reported limits of detection are below the recommended safe limits in food products, rendering this technique useful as a screening method to identify liquid food with hazardous amounts of toxic contaminants. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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14 pages, 4026 KiB

Open AccessArticle

Microfluidic Cultivation and Laser Tweezers Raman Spectroscopy of E. coli under Antibiotic Stress

by Zdeněk Pilát, Silvie Bernatová, Jan Ježek, Johanna Kirchhoff, Astrid Tannert, Ute Neugebauer, Ota Samek and Pavel Zemánek

Sensors 2018, 18(5), 1623; https://doi.org/10.3390/s18051623 - 18 May 2018

Cited by 40 | Viewed by 7917

Abstract

Analyzing the cells in various body fluids can greatly deepen the understanding of the mechanisms governing the cellular physiology. Due to the variability of physiological and metabolic states, it is important to be able to perform such studies on individual cells. Therefore, we developed an optofluidic system in which we precisely manipulated and monitored individual cells of Escherichia coli. We tested optical micromanipulation in a microfluidic chamber chip by transferring individual bacteria into the chambers. We then subjected the cells in the chambers to antibiotic cefotaxime and we observed the changes by using time-lapse microscopy. Separately, we used laser tweezers Raman spectroscopy (LTRS) in a different micro-chamber chip to manipulate and analyze individual cefotaxime-treated E. coli cells. Additionally, we performed conventional Raman micro-spectroscopic measurements of E. coli cells in a micro-chamber. We found observable changes in the cellular morphology (cell elongation) and in Raman spectra, which were consistent with other recently published observations. The principal component analysis (PCA) of Raman data distinguished between the cefotaxime treated cells and control. We tested the capabilities of the optofluidic system and found it to be a reliable and versatile solution for this class of microbiological experiments. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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14 pages, 13266 KiB

Open AccessArticle

Rapid Determination of Thiabendazole Pesticides in Rape by Surface Enhanced Raman Spectroscopy

by Lei Lin, Tao Dong, Pengcheng Nie, Fangfang Qu, Yong He, Bingquan Chu and Shupei Xiao

Sensors 2018, 18(4), 1082; https://doi.org/10.3390/s18041082 - 4 Apr 2018

Cited by 46 | Viewed by 6799

Abstract

Thiabendazole is widely used in sclerotium blight, downy mildew and black rot prevention and treatment in rape. Accurate monitoring of thiabendazole pesticides in plants will prevent potential adverse effects to the Environment and human health. Surface Enhanced Raman Spectroscopy (SERS) is a highly sensitive fingerprint with the advantages of simple operation, convenient portability and high detection efficiency. In this paper, a rapid determination method of thiabendazole pesticides in rape was conducted combining SERS with chemometric methods. The original SERS were pretreated and the partial least squares (PLS) was applied to establish the prediction model between SERS and thiabendazole pesticides in rape. As a result, the SERS enhancing effect based on silver Nano-substrate was better than that of gold Nano-substrate, where the detection limit of thiabendazole pesticides in rape could reach 0.1 mg/L. Moreover, 782, 1007 and 1576 cm⁻¹ could be determined as thiabendazole pesticides Raman characteristic peaks in rape. The prediction effect of thiabendazole pesticides in rape was the best (

R_{p}^{2}

= 0.94, RMSEP = 3.17 mg/L) after the original spectra preprocessed with 1st-Derivative, and the linear relevance between thiabendazole pesticides concentration and Raman peak intensity at 782 cm⁻¹ was the highest (R² = 0.91). Furthermore, five rape samples with unknown thiabendazole pesticides concentration were used to verify the accuracy and reliability of this method. It was showed that prediction relative standard deviation was 0.70–9.85%, recovery rate was 94.71–118.92% and t value was −1.489. In conclusion, the thiabendazole pesticides in rape could be rapidly and accurately detected by SERS, which was beneficial to provide a rapid, accurate and reliable scheme for the detection of pesticides residues in agriculture products. Full article

(This article belongs to the Special Issue Applications of Raman Spectroscopy in Sensors)

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