Anomalous DNA hybridisation kinetics on gold nanorods revealed <i>via</i> a dual single-molecule imaging and optoplasmonic sensing platform

Eerqing, Narima; Wu, Hsin‐Yu; Subramanian, Sivaraman; Vincent, S.; Vollmer, Frank

doi:10.1039/d3nh00080j

Cited by 3 publications

(3 citation statements)

References 51 publications

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“…This indicates that the sizes, numbers, and optical properties of the objects being studied lead to proportional red (or blue) WGM resonance wavelength shifts based on their polarizability. Specifically, molecules such as DNA and protein with an excess polarizability in water induce a red shift in the resonance wavelength, known as the reactive sensing mechanism. , Herein, we reveal that increased intensity of WGM leads to disproportional and sign-changed resonance wavelength shifts in optoplasmonic single molecule detection, which subsequently can be used to estimate the absorption cross-section of single molecules. For this, we built an optoplasmonic sensor with WGMs excited at near-infrared wavelength and gold nanoparticles with near-infrared plasmon resonances to study single-protein attachment events.…”

Section: Introductionmentioning

confidence: 94%

Thermo-Optoplasmonic Single-Molecule Sensing on Optical Microcavities

Toropov,

Houghton,

et al. 2024

ACS Nano

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Section: Introductionmentioning

confidence: 94%

Thermo-Optoplasmonic Single-Molecule Sensing on Optical Microcavities

Toropov,

Houghton,

et al. 2024

ACS Nano

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“…This real-time measurement allows the sensing of the conformational states of enzymes and measurements of thermodynamic parameters such as activation heat capacity . Beyond the measurement of enzymatic processes and detection of regular and anomalous DNA hybridization events, − optoplasmonic WGM sensing has been demonstrated to be capable of detecting single ions in solution, as well as single-molecule chemical reactions . With ongoing advancements, there is potential to enhance sensitivity, readout modalities, and capabilities of optoplasmonic single-molecule sensors, thereby paving the way for diverse new research avenues in single-molecule studies.…”

Section: Introductionmentioning

confidence: 99%

Whispering-Gallery Mode Optoplasmonic Microcavities: From Advanced Single-Molecule Sensors and Microlasers to Applications in Synthetic Biology

Houghton,

Kashanian,

Derrien

et al. 2024

ACS Photonics

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Optical microcavities, specifically, whispering-gallery mode (WGM) microcavities, with their remarkable sensitivity to environmental changes, have been extensively employed as biosensors, enabling the detection of a wide range of biomolecules and nanoparticles. To push the limits of detection down to the most sensitive single-molecule level, plasmonic nanorods are strategically introduced to enhance the evanescent fields of WGM microcavities. This advancement of optoplasmonic WGM sensors allows for the detection of single molecules of a protein, conformational changes, and even atomic ions, marking significant contributions in single-molecule sensing. This Perspective discusses the exciting research prospects in optoplasmonic WGM sensing of single molecules, including the study of enzyme thermodynamics and kinetics, the emergence of thermooptoplasmonic sensing, the ultrasensitive single-molecule sensing on WGM microlasers, and applications in synthetic biology.

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“…This indicates that the sizes, numbers, and optical properties of the objects being studied lead to proportional red (or blue) WGM resonance wavelength shifts based on their polarizability. Specifically, molecules such as DNA and protein with an excess polarizability in water induce a red shift in the resonance wavelength, known as reactive sensing mechanism (28, 29). Herein, we reveal that increased intensity of WGM leads to disproportional and sign-changed resonance wavelength shifts in optoplasmonic single molecule detection which subsequently can be used to estimate the absorption cross-section of single molecules.…”

Section: Introductionmentioning

confidence: 99%

Thermo-optoplasmonic single-molecule sensing on optical microcavities

Toropov,

Houghton,

et al. 2023

Preprint

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Whispering-gallery-mode (WGM) resonators are powerful instruments for single-molecule sensing in biological and biochemical investigations. WGM sensors leveraged by plasmonic nanostructures, known as optoplasmonic sensors, provide unprecedented sensitivity down to single atomic ions. In this article, we describe that the response of optoplasmonic sensors upon the attachment of single protein molecules strongly depends on the intensity of WGM. At low intensity, protein binding causes red shifts of WGM resonance wavelengths, known as the reactive sensing mechanism. By contrast, blue shifts are obtained at high intensities, which we explain as thermo-optoplasmonic (TOP) sensing, where molecules transform absorbed WGM radiation into heat. To support our conclusions, we experimentally investigated seven molecules and complexes; we observed blue shifts for dye molecules, amino acids and anomalous absorption of enzymes in the near-infrared spectral region. As an example of application, we propose a physical model of TOP sensing that can be used for the development of single-molecule absorption spectrometers.Significance StatementA notable contribution to the optical detection of single molecules has been brought about by using optical microcavities, specifically whispering-gallery-mode resonators that combine optical and plasmon resonances for the most sensitive single-molecule and ion detection. Adding absorption measurements to a single-molecule technique that operates in an aqueous solution would provide powerful new detection capabilities for sensing the properties of single molecules. We demonstrate here, for the first time, the detection of absorption cross-sections of protein molecules on optoplasmonic microcavities and validate the technique with seven different molecules and complexes. A proof-of-concept for single-molecule optoplasmonic absorption spectrometers is presented, based on a thermo-optoplasmonic sensing mechanism.

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Anomalous DNA hybridisation kinetics on gold nanorods revealed via a dual single-molecule imaging and optoplasmonic sensing platform

Abstract: Observing the hybridisation kinetics of DNA probes immobilised on plasmonic nanoparticles is key in plasmon-enhanced fluorescence detection of weak emitting species, and refractive index based single-molecule detection on optoplasmonic sensors....

Cited by 3 publications

References 51 publications

Thermo-Optoplasmonic Single-Molecule Sensing on Optical Microcavities

Thermo-Optoplasmonic Single-Molecule Sensing on Optical Microcavities

Whispering-Gallery Mode Optoplasmonic Microcavities: From Advanced Single-Molecule Sensors and Microlasers to Applications in Synthetic Biology

Thermo-optoplasmonic single-molecule sensing on optical microcavities

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