Measurements of two-photon fluorescence excitation (TPE) spectra are presented for 11 common molecular fluorophores in the excitation wavelength range 690 nm < λ < 1050 nm. Results of excitation by ∼100-fs pulses of a mode-locked Ti:sapphire laser are corroborated by single-mode cw Ti:sapphire excitation data in the range 710 nm < λ < 840 nm. Absolute values of the TPE cross section for Rhodamine B and Fluorescein are obtained by comparison with one-photon-excited fluorescence, assuming equal emission quantum efficiencies. TPE action cross sections for the other nine fluorophores are also determined. No differences between one-photon- and two-photon-excited fluorescence emission spectra are found. TPE emission spectra are independent of excitation wavelength. With both pulsed and cw excitation the fluorescence emission intensities are strictly proportional to the square of the excitation intensity to within ±4% for excitation intensities sufficiently below excited-state saturation.

Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690 to 1050 nm

4. Survey of Novel Multiphoton Active Materials 1257 4.1. Multiphoton Absorbing Systems 1257 4.2. Organic Molecules 1257 4.3. Organic Liquids and Liquid Crystals 1259 4.4. Conjugated Polymers 1259 4.4.1. Polydiacetylenes 1261 4.4.2. Polyphenylenevinylenes (PPVs) 1261 4.4.3. Polythiophenes 1263 4.4.4. Other Conjugated Polymers 1265 4.4.5. Dendrimers 1265 4.4.6. Hyperbranched Polymers 1267 4.5. Fullerenes 1267 4.6. Coordination and Organometallic Compounds 1271 4.6.1. Metal Dithiolenes 1271 4.6.2. Pyridine-Based Multidentate Ligands 1272 4.6.3. Other Transition-Metal Complexes 1273 4.6.4. Lanthanide Complexes 1275 4.6.5. Ferrocene Derivatives 1275 4.6.6. Alkynylruthenium Complexes 1279 4.6.7. Platinum Acetylides 1279 4.7. Porphyrins and Metallophophyrins 1279 4.8. Nanoparticles 1281 4.9. Biomolecules and Derivatives 1282 5. Nonlinear Optical Characterizations of Multiphoton Active Materials 1282

Multiphoton Absorbing Materials : Molecular Designs, Characterizations, and Applications

Graphene has been hailed as a wonderful material in electronics, and recently, it is the rising star in photonics, as well. The wonderful optical properties of graphene afford multiple functions of signal emitting, transmitting, modulating, and detection to be realized in one material. In this paper, the latest progress in graphene photonics, plasmonics, and broadband optoelectronic devices is reviewed. Particular emphasis is placed on the ability to integrate graphene photonics onto the silicon platform to afford broadband operation in light routing and amplification, which involves components like polarizer, modulator, and photodetector. Other functions like saturable absorber and optical limiter are also reviewed.

Graphene photonics, plasmonics, and broadband optoelectronic devices.

Two-photon absorption has important advantages over conventional one-photon absorption, which has led to applications in microscopy, microfabrication, three-dimensional data storage, optical power limiting, up-converted lasing, photodynamic therapy, and for the localized release of bio-active species. These applications have generated a demand for new dyes with high two-photon absorption cross-sections. This Review introduces the theory of two-photon absorption, surveys the wide range of potential applications, and highlights emerging structure-property correlations that can serve as guidelines for the development of efficient two-photon dyes.

Two-photon absorption and the design of two-photon dyes.

CRYSTALLINE MATERIALS Introduction Physical Properties Optical Properties Mechanical Properties Thermal Properties Magnetooptic Properties Electrooptic Properties Elastooptic Properties Nonlinear Optical Properties GLASSES Introduction Commercial Optical Glasses Specialty Optical Glasses Fused Silica Fluoride Glasses Chalcogenide Glasses Magnetooptic Properties Electrooptic Properties Elastooptic Properties Nonlinear Optical Properties Special Glasses POLYMERIC MATERIALS Optical Plastics Index of Refraction Nonlinear Optical Properties Thermal Properties Engineering Data METALS Physical Properties of Selected Metals Optical Properties Mechanical Properties Thermal Properties Mirror Substrate Materials LIQUIDS Introduction Water Physical Properties of Selected Liquids Index of Refraction Nonlinear Optical Properties Magnetooptic Properties Commercial Optical Liquids GASES Introduction Physical Properties of Selected Gases Index of Refraction Nonlinear Optical Properties Magnetooptic Properties Atomic Resonance Filters APPENDICES Safe Handling of Optical Materials Abbreviations, Acronyms, and Mineralogical or Common Names for Optical Materials Abbreviations for Methods of Preparing Optical Materials and Thin Films Fundamental Physical Constants Units and Conversion Factors

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Handbook of Optical Materials

A sensitive single-beam technique for measuring both the nonlinear refractive index and nonlinear absorption coefficient for a wide variety of materials is reported. The authors describe the experimental details and present a comprehensive theoretical analysis including cases where nonlinear refraction is accompanied by nonlinear absorption. In these experiments, the transmittance of a sample is measured through a finite aperture in the far field as the sample is moved along the propagation path (z) of a focused Gaussian beam. The sign and magnitude of the nonlinear refraction are easily deduced from such a transmittance curve (Z-scan). Employing this technique, a sensitivity of better than lambda /300 wavefront distortion is achieved in n/sub 2/ measurements of BaF/sub 2/ using picosecond frequency-doubled Nd:YAG laser pulses. >

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Sensitive measurement of optical nonlinearities using a single beam

We extend the application of the Z-scan experimental technique to determine free-carrier nonlinearities in the presence of bound electronic refraction and two-photon absorption. We employ this method, using picosecond pulses in CdTe, GaAs, and ZnTe at 1.06 μm and in ZnSe at 1.06 and 0.53 μm, to measure the refractive-index change induced by two-photon-excited free carriers (coefficient σr,), the two-photon absorption coefficient β, and the bound electronic nonlinear refractive index n2. The real and imaginary parts of the third-order susceptibility (i.e., n2 and β, respectively) are determined by Z scans with low inputs, and the refraction from carriers generated by two-photon absorption (an effecitve fifth-order nonlinearity) is determined from Z scans with higher input energies. We compare our experimental results with theoretical models and deduce that the three measured parameters are well predicted by simple two-band models. n2 changes from positive to negative as the photon energy approaches the band edge, in accordance with a recent theory of the dispersion of n2 in solids based on Kramers–Kronig transformations [ Phys. Rev. Lett.65, 96 ( 1990); IEEE J. Quantum Electron.27, 1296 ( 1991)]. We find that the values of σr are in agreement with simple band-filling models.

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Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe

Direct measurements are reported of the excited singlet-state absorption cross section and the associated nonlinear refractive cross section using picosecond pulses at 532 nm in solutions of phthalocyanine and naphthalocyanine dyes. By monitoring the transmittance and far-field spatial beam distortion for different pulsewidths in the picosecond regime, it is shown that both the nonlinear absorption and refraction are fluence (energy-per-unit-area) rather than irradiance dependent. Thus, excited-state absorption is the dominant nonlinear absorption process, and the observed nonlinear refraction is also due to real population excitation.

Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines

Optical limiting measurements have been made on solutions of several metal containing phthalocyanines and naphthalocyanines. Measurements at 532nm using nanosecond pulses from a Q-switched Nd:YAG laser show limiting throughputs of 1-10 millijoules with mild focussing in alcohol solutions with nominal transmissions of 30-70 percent. Measurements on chloro-aluminum-phthalocyanine solutions utilizing individual 30 psec pulses or trains (spanning about 100nsec) of modelocked pulses have shown even lower limiting throughputs. Thus, the dynamic range of the limiting behavior has been shown to cover at least three orders of magnitude. Prompt limiting is attributed to strong singlet-singlet (S1-Sn) absorption, whereas the longer time limiting behavior is postulated to result from strong triplet-triplet (T1-Tn) absorption. In addition to these studies, efforts have been underway to identify materials with reduced limiting throughput and improved optical transmission characteristics.

Tai-Huei Wei

Papers

Sensitive measurement of optical nonlinearities using a single beam

Determination of bound-electronic and free-carrier nonlinearities in ZnSe, GaAs, CdTe, and ZnTe

Sensitive measurement of optical nonlinearities using a single beam

Direct measurements of nonlinear absorption and refraction in solutions of phthalocyanines

Optical Limiting In Solutions Of Metallo-Phthalocyanines And Naphthalocyanines