Analysis of Blinking SERS by a Power Law with an Exponential Function

Kitahama, Yasutaka; Ozaki, Yukihiro

doi:10.1002/9781118703601.ch6

Cited by 4 publications

(13 citation statements)

References 75 publications

(165 reference statements)

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“…Since the Raman spectrum provides detailed information about molecular structure based on the sharp peak positions, through the vibrational modes of functional groups in the molecules, the information of a single molecule on a metal surface can be investigated using SERS 1,2,3 . From a silver nanoaggregate with an adsorbate at the single-molecule level, a blinking signal is observed 1,2,3,4,5,6,7,8,9,10,11,12,13,14,15,16 , and the spectrum fluctuates 1,2,3,4,5,6,7,8,9,10,11,12,13,14 . Blinking can be induced by a single molecule that randomly moves in and out of an enhanced electromagnetic (EM) field at a nanometer-sized silver nanoaggregate junction.…”

Section: Introductionmentioning

confidence: 99%

“…The random behavior of a single molecule within a wide range (for instance, in blinking SERS) can be represented as a power law rather than an average 4,5,6,7,8,9,10,11 , similar to blinking fluorescence from a single semiconductor quantum dot (QD) 18,19 . By using a power law analysis 4,5,6,7,8,9,10,11 , molecular behavior can be estimated in both the bright state (in the enhanced EM field) and dark state…”

Section: Introductionmentioning

confidence: 99%

“…For this technique, silver colloidal nanoaggregates are used 4,5,6,7,8,9,10,11 . These nanoaggregates show various localized surface plasmon resonance (LSPR) bands that strongly affect enhanced electromagnetic fields when they are excited at certain wavelengths.…”

mentioning

confidence: 99%

“…In the case of simple nanostructures, which have specific sizes, shapes, and arrangements, the LSPR dependence of SERS blinking can conceal other dependences 7 ; namely, if the good or bad nanostructure to LSPR is used, the parameters will be constant, and the other dependences will therefore be hidden. Power law analysis has been used to discover various dependences of the blinking SERS from silver colloidal nanoaggregates 4,5,6,7,8,9,10,11 . 1.…”

mentioning

confidence: 99%

“…, because the probability distribution is given by: , whose numerator in the middle term (derived from protocol 3.2.5; see the third line of Table 2) tends to decrease at longer durations of t, because even the number of bright and dark events for longer durations tends to be decreased by the fact that the molecules move randomly and can hardly stay in a non-emissive state or emissive state (the junction of the nanoaggregate) for a long period of time, as expressed in the second line of Table 2. The power law exponent α = -1.5 or -1, can be derived from the fact that the molecule randomly walks on the silver surface one-or two-dimensionally, respectively 4,5,18 . In contrast, the truncation time is shortened by a quicker molecular random walk and/ or higher energy barrier from a non-emissive to emissive state 4,5,19 .…”

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confidence: 99%

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Observation and Analysis of Blinking Surface-enhanced Raman Scattering

Kitahama¹

2018

JoVE

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From a single molecule at a silver nanoaggregate junction, blinking surface-enhanced Raman scattering (SERS) is observed. Here, a protocol is presented on how to prepare the SERS-active silver nanoaggregate, record a video of certain blinking spots in the microscopic image, and analyze the blinking statistics. In this analysis, a power law reproduces the probability distributions for bright events relative to their duration. The probability distributions for dark events are fitted by a power law with an exponential function. The parameters of the power law represent molecular behavior in both bright and dark states. The random walk model and the speed of the molecule across the entire silver surface can be estimated. It is difficult to estimate even when using averages, autocorrelation functions, and super-resolution SERS imaging. In the future, power law analyses should be combined with spectral imaging, because the origins of blinking cannot be confirmed by this analysis method alone.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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confidence: 99%

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confidence: 99%

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Observation and Analysis of Blinking Surface-enhanced Raman Scattering

Kitahama¹

2018

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Analysis of blinking from multicoloured SERS‐active Ag colloidal nanoaggregates with poly‐L‐lysine via truncated power law

Kitahama

Nagahiro

Tanaka

et al. 2017

J Raman Spectroscopy

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Silver colloidal nanoaggregates have been widely used for surface‐enhanced Raman scattering (SERS) measurements. SERS‐active nanoaggregates generally show monotone colors, although multicoloured‐blinking emissions, which occur at the single‐molecule level, have been observed from each Ag colloidal nanoaggregate with poly‐L‐lysine. For the same single nanoaggregates, SERS peaks of poly‐L‐lysine were observed at shorter wavelengths than those of the background emission band; thus, their blinking can be measured separately. The background emission is attributed to fluorescence from an Ag atomic cluster. This may be modulated by the surface plasmon enhancement of each Ag nanoaggregate and is the likely cause of multicoloured background emission. Notably, the probability distributions as a function of time for not only the dark events of SERS but also those of the background emission were reproduced via a truncated power law, indicating the same random‐walk mechanism for their blinking despite the different illuminants. The power law for the dark background emission events was truncated at a shorter tail than that for the dark SERS events. This result suggests that the fluorescent Ag cluster reaches a junction of the Ag nanoaggregate covered with citrate anions more quickly than the cationic polymer chain. Copyright © 2017 John Wiley & Sons, Ltd.

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SERS Blinking on Anisotropic Nanoparticles

2020

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A truncated power law analysis was developed for surface-enhanced Raman scattering (SERS) blinking observed on anisotropic silver nanoparticles (NPs). Using modified equations, a richer and more diverse set of SERS blinking parameters was obtained, enabling the heterogeneity of the SERS blinking behaviors to be extracted. As a result of a profound analysis, three complex hot spots engaging the edges, tops, and junction can be recognized and described. This new approach regarding the analysis of SERS blinking has encouraged a revision of the base theory of this phenomenon, particularly the definition of the energy barrier between nonemissive and emissive states.

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Analysis of Blinking SERS by a Power Law with an Exponential Function

Cited by 4 publications

References 75 publications

Observation and Analysis of Blinking Surface-enhanced Raman Scattering

Observation and Analysis of Blinking Surface-enhanced Raman Scattering

Analysis of blinking from multicoloured SERS‐active Ag colloidal nanoaggregates with poly‐L‐lysine via truncated power law

SERS Blinking on Anisotropic Nanoparticles

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