Abstract
Two-photon excitation is gaining rapidly in interest and significance in spectroscopy and microscopy. Here we introduce a new approach that suggests versatile optical labels suitable for both one- and two-photon excitation and also two-photon-excited ultrasensitive, nondestructive chemical probing. The underlying spectroscopic effect is the incoherent inelastic scattering of two photons on the vibrational quantum states called hyper-Raman scattering (HRS). The rather weak effect can be strengthened greatly if HRS takes place in the local optical fields of gold and silver nanostructures. This so-called surface-enhanced HRS (SEHRS) is the two-photon analogue to surface-enhanced Raman scattering (SERS). SEHRS provides structurally sensitive vibrational information complementary to those obtained by SERS. SEHRS combines the advantages of two-photon spectroscopy with the structural information of vibrational spectroscopy and the high-sensitivity and nanometer-scale local confinement of plasmonics-based spectroscopy. We infer effective two-photon cross-sections for SEHRS on the order of 10 −46 to 10 −45 cm 4 ·s, similar to or higher than the best “action” cross-sections (product of the two-photon absorption cross-section and fluorescence quantum yield) for two-photon fluorescence, and we demonstrate HRS on biological structures such as single cells after incubation with gold nanoparticles.
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Dates
Type | When |
---|---|
Created | 18 years, 9 months ago (Nov. 6, 2006, 8:54 p.m.) |
Deposited | 3 years, 4 months ago (April 12, 2022, 3:40 p.m.) |
Indexed | 4 days, 4 hours ago (Aug. 29, 2025, 6:05 a.m.) |
Issued | 18 years, 9 months ago (Nov. 14, 2006) |
Published | 18 years, 9 months ago (Nov. 14, 2006) |
Published Online | 18 years, 9 months ago (Nov. 14, 2006) |
Published Print | 18 years, 9 months ago (Nov. 14, 2006) |
@article{Kneipp_2006, title={Two-photon vibrational spectroscopy for biosciences based on surface-enhanced hyper-Raman scattering}, volume={103}, ISSN={1091-6490}, url={http://dx.doi.org/10.1073/pnas.0608262103}, DOI={10.1073/pnas.0608262103}, number={46}, journal={Proceedings of the National Academy of Sciences}, publisher={Proceedings of the National Academy of Sciences}, author={Kneipp, Janina and Kneipp, Harald and Kneipp, Katrin}, year={2006}, month=nov, pages={17149–17153} }