Three-photon-excited upconversion luminescence of YVO4 single crystal by infrared femtosecond laser irradiation

We report on the upconversion luminescence of a pure YVO4 single crystal excited by an infrared femtosecond laser. The luminescent spectra show that the upconversion luminescence comes from the transitions from the lowest excited states T-3(1), T-3(2) to the ground state (1)A(1) of the VO43-. The dependence of the fluorescence intensity on the pump power density of laser indicates that the conversion of infrared irradiation to visible emission is dominated by three-photon excitation process. We suggest that the simultaneous absorption of three infrared photons promotes the VO43- to excited states, which quickly cascade down to lowest excited states, and radiatively relax to ground states, resulting in the broad characteristic fluorescence of VO43-. (c) 2005 Optical Society of America.

Theoretical investigation on the one- and two-photon absorption properties for a series of symmetrical charge transfer fluorene-phenylene and fluorene-thiophene derivatives

One- and two-photon absorption properties of a series of fluorene derivatives with symmetrical charge transfer D-IT-D and A-IT-A structural motifs have been theoretically investigated with ZINDO/S method. The optimized structures and the characterization of frontier molecular orbitals were obtained by using AMI calculations. Two-photon absorption properties of molecules have been studied using three-state model. The calculation results have shown that fluorene-thiophene derivatives exhibit larger two-photon absorption cross-section as compared with other studied molecules. To illustrate the results, the crucial effects of thiophene ring on fluorenethiophene derivatives and the net charge changes on the pi-conjugated bridges are analyzed theoretically. (c) 2006 Elsevier B.V. All rights reserved.

Three-photon-excited upconversion luminescence of Ce3+: YAP crystal by femtosecond laser irradiation

Infrared to ultraviolet and visible upconversion luminescence was demonstrated in trivalent cerium doped YAlO3 crystal (Ce3+: YAP) under focused infrared femtosecond laser irradiation. The fluorescence spectra show that the upconverted luminescence comes from the 5d-4f transitions of trivalent cerium ions. The dependence of luminescence intensity of trivalent cerium on infrared pumping power reveals that the conversion of infrared radiation is dominated by three-photon excitation process. It is suggested that the simultaneous absorption of three infrared photons pumps the Ce3+ ion into upper 5d level, which quickly nonradiatively relax to lowest 5d level. Thereafter, the ions radiatively return to the ground states, leading to the characteristic emission of Ce3+. (c) 2005 Optical Society of America.

Two-photon absorption spectrum of the photoinitiator Lucirin TPO-L

Two-photon absorption induced polymerization provides a powerful method for the fabrication of intricate three-dimensional microstructures. Recently, Lucirin TPO-L was shown to be a photoinitiator with several advantageous properties for two-photon induced polymerization. Here we measure the two-photon absorption cross-section spectrum of Lucirin TPO-L, which presents a maximum of 1.2 GM at 610 nm. Despite its small two-photon absorption cross-section, it is possible to fabricate excellent microstructures by two-photon polymerization due to the high polymerization quantum yield of Lucirin TPO-L. These results indicate that optimization of the two-photon absorption cross-section is not the only material parameter to be considered when searching for new photoinitiators for microfabrication via two-photon absorption.

Temperature Effect on the Two-Photon Absorption Spectrum of All-trans-beta-carotene

In this report, we investigate the influence of temperature on the two-photon absorption (2PA) spectrum of all-trans-beta-carotene using the femtosecond white-light-continuum Z-scan technique. We observed that the 2PA cross-section decreases quadratically with the temperature. Such effect was modeled using a three-energy-level diagram within the sum-over-essential states approach, assuming temperature dependencies to the transition dipole moment and refractive index of the solvent. The results show that the transition dipole moments from ground to excited state and between the excited states, which governed the two-photon matrix element, have distinct behaviors with the temperature. The first one presents a quadratic dependence, while the second exhibits a linear dependence. Such effects were attributed mainly to the trans -> cis thermal interconversion process, which decreases the effective conjugation length, contributing to diminishing the transition dipole moments and, consequently, the 2PA cross-section.

Influence of non-stoichiometric defects on nonlinear absorption and refraction in Nd:Zn co-doped lithium niobate

Nonlinear absorption and refraction phenomena in stoichiometric lithium niobate (SLN) pure and co-doped with Zn and Nd, and congruent lithium niobate (CLN) were investigated using Z-scan technique. Femtosecond laser pulses from Ti:Sapphire laser (800 nm, 110 fs pulse width and 1 kHz repetition rate) were utilized for the experiment. The process responsible for nonlinear behavior of the samples was identified to be three photon absorption (3PA). This is in agreement with the band gap energies of the samples obtained from the linear absorption cut off and the slope of the plot of Ln(1 − TOA) vs. Ln(I0) using Sutherland’s theory (s = 2.1, for 3PA). The nonlinear refractive index (n2) of Zn doped samples was found to be lower than that of pure samples. Our experiments show that there exists a correlation between the nonlinear properties and the stoichiometry of the samples. The values of n2 fall into the same range as those obtained for the materials of similar band gap.

Interior Photon Absorption Based Adaptive Regularization Improves Diffuse Optical Tomography

An adaptive regularization algorithm that combines elementwise photon absorption and data misfit is proposed to stabilize the non-linear ill-posed inverse problem. The diffuse photon distribution is low near the target compared to the normal region. A Hessian is proposed based on light and tissue interaction, and is estimated using adjoint method by distributing the sources inside the discretized domain. As iteration progresses, the photon absorption near the inhomogeneity becomes high and carries more weightage to the regularization matrix. The domain's interior photon absorption and misfit based adaptive regularization method improves quality of the reconstructed Diffuse Optical Tomographic images.

Near-resonant two-photon absorption in luminescent CdTe quantum dots

We report the nonlinear optical absorption studies in two differently sized water-soluble cadmium telluride quantum dot (QD) samples, exhibiting first excitonic absorption peaks at 493 nm and 551 nm, respectively. An optical limiting behavior is observed for near-resonant excitation at 532 nm using nanosecond laser pulses, originating from the effective two-photon absorption (TPA) mechanism. The effective TPA coefficient (beta(eff)) is measured to be in the range of 10(-12) m/W. This is one order of magnitude higher than the TPA coefficient (beta) reported for off-resonant excitation. At this excitation wavelength, the smaller QD shows a relatively weaker photoluminescence and stronger nonlinear absorption. (C) 2012 American Institute of Physics. [doi:10.1063/1.3687695]

Nonlinear Refraction and Two-Photon Absorption in Dense 2Bi(2)O(3)-B2O3 Glasses

High density transparent glasses (7.86 g/cc) were fabricated in the 2Bi(2)O(3)-B2O3 (BBO) system. Optical band gap of the obtained glasses was found to be 2.6eV. The refractive index measured for these glasses was 2.25 +/- 0.05 at lambda=543 nm. Nonlinear refraction and absorption studies were carried out on the BBO glasses using z-scan technique a lambda=532 nm of 10 ns pulse width. The nonlinear refractive index obtained was n(2)=12.1x10(-14) cm(2)/W and nonlinear absorption coefficient was beta=15.2 cm/GW. The n(2) and beta values of the BBO glasses were large compared to the other reported high index bismuth based oxide glass systems in the literature. These were attributed to the high density, high linear refractive index, low band gap and two photon absorption associated with these glasses. The electronic origin of large nonlinearities was discussed based on bond-orbital theory.

Large nonlinear refraction and two photon absorption in ferroelectric Bi2VO5.5 thin films

Ferroelectric c-oriented Bi2VO5.5 (BVO) thin films (thickness approximate to 300 nm) were fabricated by pulsed laser deposition on corning glass substrates. Nonlinear refractive index (n(2)) and two photon absorption coefficient (beta) were measured by Z-scan technique at 532 nm wavelength delivering pulses with 10 ns duration. Relatively large values of n(2) = 2.05 +/- 0.2 x 10(-10) cm(2)/W and beta = 9.36 +/- 0.3 cm/MW were obtained for BVO thin films. Origin of the large optical nonlinearities in BVO thin films was discussed based on bond-orbital theory of transition metal oxides. (c) 2012 Elsevier B.V. All rights reserved.

A new strategy of enhancing two-photon absorption in benzothiazole-containing fluorene molecules: Introduction of auxiliary donor-acceptor effects

A series of benzothiazole-containing fluorene molecules have been designed and their one- and two-photon absorption properties have been investigated theoretically by using the ZINDO method. The effects of electron-excessive/deficient heterocyclic bridges as auxiliary donors (auxD)/acceptors (auxA) on TPA cross-sections were studied. The results show that the molecules with D-pi-auxA-A, D-aux D-pi-A, or D-auxD-pi-auxA-A structure types have large TPA cross-section, which can be a valuable strategy in the design of two-photon absorption materials. Also, a linear relationship between the first hyperpolarizability and the TPA cross-section is observed. (c) 2006 Elsevier B.V. All rights reserved.

Three-photon-excited upconversion luminescence of niobium ions doped silicate glass by a femtosecond laser irradiation

We report on the bluish green upconversion luminescence of niobium ions doped silicate glass by a femtosecond laser irradiation. The dependence of the fluorescence intensity on the pump power density of laser indicates that the conversion of infrared irradiation to visible emission is dominated by three-photon excitation process. We suggest that the charge transfer from O-2-to Nb5+ can efficiently contribute to the bluish green emission. The results indicate that transition metal ions without d electrons play an important role in fields of optics when embedded into silicate glass matrix. (C) 2008 Optical Society of America.