Far-Field Super-Resolution Vibrational Spectroscopy

Graefe, Christian T.; Punihaole, David; Harris, Celina M.; Lynch, Michael J.; Leighton, Ryan; Frontiera, Renee R.

doi:10.1021/acs.analchem.9b01731

Cited by 31 publications

(27 citation statements)

References 88 publications

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“…SERS remained analytically non-exploitable for many years because of its erratic nature and this until the detailed mechanisms involved in localised surface plasmon resonance (LSPR) as a function of morphological details were clarified. Currently, a method being used is tip-enhanced Raman spectrometry (TERS), a sensitive molecular detection and imaging tool with a detection limit down to the singlemolecule level [18,19]. Metallic nanoparticles can also be used to increase the sensitivity of fluorescent detection because they generate a phenomenon known as metalenhanced fluorescence, thus increasing fluorescence lifetime and quantum yields.…”

Section: Analytical Chemistry and Physicsmentioning

confidence: 99%

The metamorphosis of analytical chemistry

Adams

Adriaens

2019

Anal Bioanal Chem

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Defining analytical chemistry as the measurement of isolated compositional features in a selected study object ignores the unique perspective that analytical chemists bring to twenty-first century science and society. In this feature article, we will discuss some of the existing preconceptions and misinterpretations of analytical chemistry that occur at present and will tackle them from the more up-to-date perspective of science in the Big Data Era. This will place their influence in context while simultaneously enlarging the scope of the discipline analytical chemistry to its well-deserved prevalent position in present-day science and technology.

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Section: Analytical Chemistry and Physicsmentioning

confidence: 99%

The metamorphosis of analytical chemistry

Adams

Adriaens

2019

Anal Bioanal Chem

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“…[37][38] In our experiment, however, we did not vary the relative focus of the two beams in the z direction, and the collinear CARS signal from the entire focal volume was collected. This is equivalent to integrating the signal in the focal volume, which eliminates the zdependency in equation (2). Also, we note the laser beam is not monochromatic and thus has a finite spectral width.…”

Section: Theorymentioning

confidence: 99%

Spectral Narrowing Accompanies Enhanced Spatial Resolution in Saturated Coherent Anti-Stokes Raman Scattering (CARS): Comparisons of Experiment and Theory

et al. 2020

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We demonstrate theoretically and confirm experimentally the mechanism by which spectral narrowing accompanies enhanced spatial resolution in a saturated coherent anti-Stokes Raman scattering (CARS) signal that is demodulated at the third harmonic (3f) of the pump modulation frequency (f). Under these modulation conditions, theory predicts a narrowing of the full width at half-maximum (FWHM) of the CARS spectrum by a factor of 2.0 with respect to that of the spectrum obtained by demodulation at the fundamental frequency. Theory also predicts an improvement of spatial resolution by a factor of 1.7. Experimentally, narrowing of the FWHM of the CARS spectrum of 1,4-bis((E)-2-methylstyryl) benzene (MSB) crystals by a factor of 2.5 is observed upon saturation. Further experimental confirmation is provided from investigating diamond particles, for which spectral narrowing was enhanced by a factor of 2.8 and spatial resolution was enhanced by a factor of 2. Details of the mechanism and execution of the saturated CARS experiment are elucidated and limits to its applicability are suggested, one of which is the conclusion that the saturation approach is not suitable for extraction of harmonics beyond 3f. In this work, we have developed a more comprehensive understanding of the correlation between the observed experimental results and experimental factors than has been previously reported. Disciplines Disciplines Physical Chemistry Comments Comments

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“…One example in the current research, where pulse energies in the order of hundreds of nano‐joules and pulses with a duration in the femtosecond regime are needed, is the field of spatial resolution enhancement in CRS, [ 18,20‐25 ] to overcome the diffraction limit given by Abbe. [ 26 ] All these methods are based on depleting one of the three scattering resources: the pump photons, the Stokes photons, or the molecules in the ground state.…”

Section: Introductionmentioning

confidence: 99%

Mitigating cross‐phase modulation artifacts in femtosecond stimulated Raman scattering

Würthwein

Lüpken

Irwin

et al. 2020

J Raman Spectroscopy

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In contrast to spontaneous Raman scattering, coherent Raman scattering techniques, such as femtosecond stimulated Raman scattering (FSRS), show advantages for many applications. Besides an enhanced signal strength, FSRS is free of a nonresonant background but is affected by cross‐phase modulation (XPM). The resulting artifacts in FSRS become relevant for high pulse intensities (GW/cm2‐regime) and ultrashort pulses (<2 ps), both necessary for super‐resolution experiments. As the pulse duration is a crucial parameter for XPM as well as for FSRS, we present a setup in which we adjust the pulse duration across the relevant range (0.5–3 ps), in order to investigate the XPM influence on the spectra. Furthermore, we vary the peak intensity, the temporal overlap between the interacting pulses, and the nonlinear refractive index coefficient n2 of the sample, showing that a trade‐off between all these quantities enables the measurement of unaffected FSRS spectra

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Far-Field Super-Resolution Vibrational Spectroscopy

Cited by 31 publications

References 88 publications

The metamorphosis of analytical chemistry

The metamorphosis of analytical chemistry

Spectral Narrowing Accompanies Enhanced Spatial Resolution in Saturated Coherent Anti-Stokes Raman Scattering (CARS): Comparisons of Experiment and Theory

Mitigating cross‐phase modulation artifacts in femtosecond stimulated Raman scattering

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