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Abstract Titanium nitride nanoparticles have become a research interest due to their distinguished optical and photothermal properties. Furthermore, the search for nanoparticle solutions with tunable nonlinear optical properties for laser‐based applications is critical. More specifically, third order optical nonlinearities such as reverse saturable absorption, optical liming, and self‐focusing are important in the biomedical and electronics fields. The optical nonlinearities of titanium nitride plasmonic nanoparticles are investigated as a function of material concentration in water solutions. Furthermore, the effect of nanoparticle clustering on optical nonlinearities is investigated by fabricating micrometer‐sized clusters of ≈50 nm titanium nitride particles. These studies demonstrate that the nonlinear absorption coefficient increases linearly with concentration. However, clusters require higher concentrations compared to the freestanding nanoparticles to exhibit similar nonlinear absorption coefficient and optical density. Similarly, the optical limiting threshold for titanium nitride nanoparticles appears to be lower compared to the cluster solutions, which is impacted by the collective scattering of nanoparticles and high reverse saturable absorption. In addition, self‐focusing is observed in the continuous resonant regime. This study provides an in‐depth analysis of the nonlinear optical properties of titanium nitride, with relevant consequences for applications such as sensor protection and photothermal therapy.
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Nonlinear effects in single-particle photothermal imaging
Although photothermal imaging was originally designed to detect individual molecules that do not emit or small nanoparticles that do not scatter, the technique is now being applied to image and spectroscopically characterize larger and more sophisticated nanoparticle structures that scatter light strongly. Extending photothermal measurements into this regime, however, requires revisiting fundamental assumptions made in the interpretation of the signal. Herein, we present a theoretical analysis of the wavelength-resolved photothermal image and its extension to the large particle scattering regime, where we find the photothermal signal to inherit a nonlinear dependence upon pump intensity, together with a contraction of the full-width-at-half-maximum of its point spread function. We further analyze theoretically the extent to which photothermal spectra can be interpreted as an absorption spectrum measure, with deviations between the two becoming more prominent with increasing pump intensities. Companion experiments on individual 10, 20, and 100 nm radius gold nanoparticles evidence the predicted nonlinear pump power dependence and image contraction, verifying the theory and demonstrating new aspects of photothermal imaging relevant to a broader class of targets.
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- PAR ID:
- 10433771
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 158
- Issue:
- 2
- ISSN:
- 0021-9606
- Page Range / eLocation ID:
- 024202
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0132167
