Femtomolar Detection of Prostate-Specific Antigen:  An Immunoassay Based on Surface-Enhanced Raman Scattering and Immunogold Labels

Grubisha, Desirée S.; Lipert, Robert J.; Park, Hye Young; Driskell, Jeremy D.; Porter, Marc D.

doi:10.1021/ac034356f

Cited by 764 publications

(745 citation statements)

References 66 publications

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“…Most studies applying nanomaterials for protein detection have been limited to single target-based assays. [91][92][93] This is not surprising considering that the issues described earlier such as chemical stability, cross-reactivity between different probes and targets as well as non-specific adsorption are also equally applicable to nanomaterial enhanced biosensing. …”

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confidence: 85%

Microarray methods for protein biomarker detection

Lee

Wark

Corn

2008

Analyst

137

108

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The application of protein biomarkers as an aid for the detection and treatment of diseases has been subject to intensified interest in recent years. The quantitative assaying of protein biomarkers in easily obtainable biological fluids such as serum and urine offers the opportunity to improve patient care via earlier and more accurate diagnoses in a convenient, non-invasive manner as well as providing a potential route towards more individually targeted treatment. Essential to achieving progress in biomarker technology is the ability to screen large numbers of proteins simultaneously in a single experiment with high sensitivity and selectivity. In this article, we highlight recent progress in the use of microarrays for high-throughput biomarker profiling and discuss some of the challenges associated with these efforts. I IntroductionThe discovery of protein biomarkers whose change in expression level or state correlates with the progression of a disease is becoming increasingly important. Once validated, proposed biomarkers can be involved in achieving an earlier diagnosis, differentiating between disease types with greater accuracy, and assessing response to treatment. Prominent examples of biomarkers include proteins that are associated with a variety of cancers, 1-4 as well as heart, 5,6 renal, 7,8 andAlzheimer's 9,10 diseases.Most biomarker studies reported to date have focused on serum-, plasmaand urine-based samples. A number of other possibilities include saliva, tears, breath condensates, cerebrospinal fluid and tissue lysates extracted from biopsy samples. There are several excellent reviews detailing biomarker discovery and validation. [11][12][13][14][15] The potential benefits of biomarkers have greatly motivated both academic and industry researchers to apply new proteomic technologies for biomarker discovery and to develop quantitative analytical methodologies for rapid and sensitive biomarker detection. Many clinically relevant biomarkers reside in blood at picomolar concentrations and lower, which is five to seven orders of magnitude lower than the most abundant plasma proteins. Therefore, protein detection with high specificity and sensitivity is required; unfortunately, no universal ultrasensitive enzymatic amplification method (such as PCR for the case of nucleic acid detection) exists for proteins. Additionally, it is desirable to screen multiple proteins simultaneously in a single sample. Multiplexed measurements are attractive not only for economic reasons but also for identifying characteristic signal patterns associated with the relative changes in entire sets of proteins as this will provide much more insight and diagnostic accuracy than individual biomarker measurements.hyejinlee@knu.ac.kr. 14,19,[24][25][26][27][28][29][30] Although microarray methods are wellestablished for high-throughput nucleic acid studies, their application for protein detection has been limited by issues such as the surface immobilization of protein capture probes without loss in bioactivity as well a...

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confidence: 85%

Microarray methods for protein biomarker detection

Lee

Wark

Corn

2008

Analyst

137

108

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“…Traditional SERS substrates, chosen because they provide the desired optical properties, include electrodes roughened by the oxidation-reduction cycle (ORC), island films, colloidal nanoparticles, and surface-confined nanostructures (Figure 2). ORC-roughened electrodes provide reproducible, in situ SERS substrates with moderate (~10 6 ) enhancement factors. These substrates were exploited in the initial SERS studies of pyridine (3) and are used to study catalytic reactions on transition-metalcoated gold electrodes as well as other electrochemically active systems (27 ).…”

Section: Sers Substratesmentioning

confidence: 99%

“…Recently, SERS has been used extensively as a signal transduction mechanism in biological and chemical sensing. Examples are trace analysis of pesticides (4 ), anthrax (5), prostate-specific antigen (6 ), glucose (7,8), and nuclear waste (9). SERS has also been implemented for identification of bacteria (10), genetic diagnostics (11), and immunoassay labeling (12)(13)(14).…”

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confidence: 99%

Surface-Enhanced Raman Spectroscopy

Haynes¹,

McFarland²,

Duyne³

2005

Anal. Chem.

1,077

855

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mekal theoretically predicted inelastic light scattering in 1923 (1). Raman and Krishnan first experimentally observed the phenomenon and reported in their 1928 Nature paper that the inelastic scattering effect was characterized by "its feebleness in comparison with the ordinary scattering" (2). This "feeble" phenomenon is now known as Raman scattering. The change in wavelength that is observed when a photon undergoes Raman scattering is attributed to the excitation (or relaxation) of vibrational modes of a molecule. Because different functional groups have different characteristic vibrational energies, every molecule has a unique Raman spectrum. In accordance with the Raman selection rule, the molecular polarizability changes as the molecular vibrations displace the constituent atoms from their equilibrium positions. The intensity of Raman scattering is proportional to the magnitude of the change in molecular polarizability. Thus, aromatic molecules exhibit more intense Raman scattering than aliphatic molecules.Even so, Raman scattering cross sections are typically 14 orders of magnitude smaller than those of fluorescence; therefore, the Raman signal is still several orders of magnitude weaker than the fluorescence emission in most cases. Because of the inherently small intensity of the Raman signal, the sensitivity limits of available detectors, and the intensity of the excitation sources, the applicability of Raman scattering was restricted for many years. However, its utility as an analytical technique improved with the advent of the laser and the evolution of photon detection technology.In 1977, Jeanmaire and Van Duyne demonstrated that the magnitude of the Raman scattering signal can be greatly enhanced when the scatterer is placed on or near a roughened noble-metal substrate (3). Strong electromagnetic fields are generated when the localized surface plasmon resonance (LSPR) of nanoscale roughness features on a silver, gold, or copper substrate is excited by visible light. When the Raman scatterer is subjected to these intensified electromagnetic fields, the magnitude of the induced dipole increases, and accordingly, the intensity of the inelastic scattering increases. This enhanced scattering process is known as surface-enhanced Raman (SER) scattering-a term that emphasizes the key role of the noblemetal substrate in this phenomenon.

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“…Raman spectra enable fingerprinting of molecules which is of particular interest for bio-applications. Surface enhanced Raman scattering (SERS) provides greater detection sensitivity than conventional Raman spectroscopy [1][2][3], and it is quickly gaining traction in the study of biological molecules adsorbed on a metal surface [4][5][6][7][8][9][10][11][12]. SERS spectroscopy allows for the detection and analysis of minute quantities of analytes because it is possible to obtain high-quality SERS spectra at submonolayer molecular coverage as a result of the large scattering enhancements.…”

Section: Introductionmentioning

confidence: 99%

Adaptive silver films for surface‐enhanced Raman spectroscopy of biomolecules

Drachev

Thoreson

Nashine

et al. 2005

J Raman Spectroscopy

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The interaction of biological molecules with a typical substrate for surface-enhanced Raman scattering (SERS) often leads to their structural and functional changes. In this work we describe SERS substrates, called adaptive silver films (ASFs), in which the biomaterial and the substrate act in concert to produce excellent Raman enhancement through local restructuring of the metal surface while at the same time preserving the properties (such as conformational state and binding activity) of the analyte. These adaptive substrates show great promise for SERS spectroscopy of many different types of biomolecules, and we provide several current examples of their use. IntroductionOne of main advantages of Raman scattering as a detection method for molecule sensing is well known. Raman spectra enable fingerprinting of molecules which is of particular interest for bio-applications. Surface enhanced Raman scattering (SERS) provides greater detection sensitivity than conventional Raman spectroscopy [1][2][3], and it is quickly gaining traction in the study of biological molecules adsorbed on a metal surface [4][5][6][7][8][9][10][11][12]. SERS spectroscopy allows for the detection and analysis of minute quantities of analytes because it is possible to obtain high-quality SERS spectra at submonolayer molecular coverage as a result of the large scattering enhancements. SERS has also been shown to be sensitive to molecular orientation and to the distance from the metal surface [13]. Thus, SERS is well-suited for biomolecule studies in which specificity and sensitivity to the conformational state and orientation of the molecule are very important.The SERS enhancement mechanism originates in part from the large local electromagnetic fields caused by resonant surface plasmons that can be optically excited at certain wavelengths for metal particles of different shapes or closely spaced groups of particles [14][15][16][17][18][19][20][21]. For aggregates of interacting particles, which are often structured as fractals, plasmon resonances can be excited in a very broad spectral range [22]. In addition to electromagnetic field enhancement, metal nanostructures and molecules can form charge-transfer complexes that provide further enhancement for SERS [23][24][25][26][27][28][29]. The resulting overall enhancement depends critically on the particle or aggregate nanostructure morphology [22,[30][31][32][33][34][35][36], and it can be as high as 10 5 to 10 8 for

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Femtomolar Detection of Prostate-Specific Antigen: An Immunoassay Based on Surface-Enhanced Raman Scattering and Immunogold Labels

Cited by 764 publications

References 66 publications

Microarray methods for protein biomarker detection

Microarray methods for protein biomarker detection

Surface-Enhanced Raman Spectroscopy

Adaptive silver films for surface‐enhanced Raman spectroscopy of biomolecules

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