Large Molecular Third-Order Optical Nonlinearities in Polarized Carotenoids

Marder, Seth R.; Torruellas, William E.; Blanchard‐Desce, M.; Ricci, Vincent; Stegeman, George I.; Gilmour, Sharon; Brédas, Jean‐Luc; Li, Jun; Bublitz, Greg U.; Boxer, Steve G.

doi:10.1126/science.276.5316.1233

Cited by 357 publications

(216 citation statements)

References 15 publications

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“…Among other properties, large two-photon absorption (TPA) cross-sections are promising for different applications, ranging from optical storage to biological optical imaging 1 . As a consequence, both experimental and theoretical work [2][3][4][5][6][7] have received strong impetus and several interesting strategies have been proposed to improve NLO responses in general 8,9 and TPA cross-section in particular 1,10 . A presently highly debated topic concerns the importance of vibrational contributions to NLO responses of organic materials [11][12][13][14] .…”

Section: Introductionmentioning

confidence: 99%

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Painelli

Freo

Terenziani

2001

Chemical Physics Letters

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Section: Introductionmentioning

confidence: 99%

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Painelli

Freo

Terenziani

2001

Chemical Physics Letters

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“…bridges which lead to states with extended charge separation, 17,18 are critical in enhancing the efficiency of intramolecular charge transfer. Usually double bonds, due to their simple synthetic accessibility, are used in the backbone of the PIs to extend the conjugation length although the so obtained r TPA is normally lower than that of the triple-bondcontaining counterparts.…”

mentioning

confidence: 99%

Synthesis and structure‐activity relationship of several aromatic ketone‐based two‐photon initiators

Siklos

Pucher

et al. 2011

J. Polym. Sci. A Polym. Chem.

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Several novel aromatic ketone-based two-photon initiators containing triple bonds and dialkylamino groups were synthesized and the structure-activity relationships were evaluated. Branched alkyl chains were used at the terminal donor groups to improve the solubility in the multifunctional monomers. Because of the long conjugation length and good coplanarity, the evaluated initiators showed large two-photon cross section values, while their fluorescence lifetimes and quantum yields strongly depend on the solvent polarity. All novel initiators exhibited high activity in terms of two-photon-induced microfabrication. This is especially true for fluorenone-based derivatives, which displayed much broader processing windows than well-known highly active initiators from the literature and commercially available initiators. While the new photoinitiators gave high reactivity in two-photoninduced photopolymerization at concentration as low as 0.1% wt, these compounds are surprisingly stable under one photon condition and nearly no photo initiation activity was found in classical photo DSC experiment.

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“…The greater voltage sensitivity of JR1 compared with the styryl dyes can be seen as a manifestation of the scaling behaviors of nonlinear optical susceptibilities; there is no simple scaling law, but the ratio g/b generally increases with the size of the p system. [41][42][43][44] Equation (3) indicates that, in general, the sensitivity of a dye to electric field (DS/S) will increase as the p systems becomes larger and more polarizable.…”

Section: Methodsmentioning

confidence: 99%

Porphyrins for Probing Electrical Potential Across Lipid Bilayer Membranes by Second Harmonic Generation

et al. 2013

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Neurons communicate by using electrical signals, mediated by transient changes in the voltage across the plasma membrane. Optical techniques for visualizing these transmembrane potentials could revolutionize the field of neurobiology by allowing the spatial profile of electrical activity to be imaged in real time with high resolution, along individual neurons or groups of neurons within their native networks. [1,2] Second harmonic generation (SHG) is one of the most promising methods for imaging membrane potential, although so far this technique has only been demonstrated with a narrow range of dyes. [3] Here we show that SHG from a porphyrin-based membrane probe gives a fast electro-optic response to an electric field which is about 5-10 times greater than that of conventional styryl dyes. Our results indicate that porphyrin dyes are promising probes for imaging membrane potential.Studies of excitable cells, such as neurons and cardiac myocytes, require new methods for mapping changes in membrane potential, ideally with a voltage resolution of about 1 mV, a time resolution of 1 ms, and a spatial resolution of 1 mm. [1,2] Microelectrodes can be used to measure transmembrane potentials with excellent sensitivity and temporal resolution, but they do not provide subcellular spatial resolution. Fluorescent calcium indicators are widely used to probe membrane potential indirectly, through the intracellular Ca 2+ concentration. However, changes in calcium concentration do not accurately reflect voltage transients. [4] Fluorescent voltage-sensitive dyes were first developed 30 years ago, [5] and recent advances in the molecular design of these dyes [6][7][8][9][10] have made it possible to track the spatial evolution of action potentials. [11][12][13][14] Compared with fluorescence, SHG imaging has several advantages as a technique for probing membrane potential: [3,[15][16][17][18][19][20][21] SHG has a greater intrinsic sensitivity to electric fields than fluorescence, [19][20][21] and it is only produced by noncentrosymmetric molecules in noncentrosymmetric environments, thus making it ideal for probing interfaces such as lipid bilayers. Similar to twophoton-excited fluorescence, SHG is a two-photon nonlinear optical effect, and it brings the advantages of depth penetration associated with multiphoton microscopy. [22] The main disadvantage of SHG is that it often gives lower intensity than fluorescence; there is a need for the design of brighter, more voltage-sensitive SHG dyes. [3,23] Styryl dyes and retinal chromophores have been shown to exhibit voltage-sensitive SHG when localized in plasma membranes, [15,24] and the voltage sensitivity of their SHG is greater than that of their fluorescence. [19][20][21] Recently we reported that amphiphilic porphyrins such as JR1 exhibit strong SHG when localized in lipid membranes. [25] Here we compare the voltage sensitivity of the SHG from JR1 with that from three widely studied styryl dyes (FM4-64, di-4-ANEPPS, and RH237) in hemispherical lipid bilayers (HLBs). [15,26,27] ...

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Large Molecular Third-Order Optical Nonlinearities in Polarized Carotenoids

Cited by 357 publications

References 15 publications

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Synthesis and structure‐activity relationship of several aromatic ketone‐based two‐photon initiators

Porphyrins for Probing Electrical Potential Across Lipid Bilayer Membranes by Second Harmonic Generation

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