Effects of Vacuum-Induced Coherence on One- and Two-Photon Absorption Spectra of Transient Process in a Y-Type System

We investigate the influence of the vacuum-induced coherence on one- and two-photon absorption of the transient process in a four-level Y-type atomic system. We find that the one- and two-photon t, ransient absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra of the transient process can be dramatically affected by modulating the relative phase of the applied fields. By apprdpriately choosing the relative phase, the amplification of the probe field can be achieved.

One- and two-photon absorption-amplification response in a four-level atomic system with vacuum-induced coherence

This paper theoretically studies the effects of the vacuum-induced coherence on one- and two-photon absorption in a four-level atomic medium. It finds that the one- and two-photon absorption and amplification properties are quite sensitive to the vacuum-induced coherence. It is also shown that the one- and two-photon absorption spectra can be dramatically affected by modulating the relative phase of the applied fields, With the proper choice of the relative phase, the amplification without inversion for the probe field can be realized.

Protonation Effect on One- and Two-photon Absorption Property of a Newly Synthesized Octupolar Chromophore

The protonation effects on one- and two-photon absorption properties of an octupolar molecule TA with 1,3,5-triazine core and pyrrole electron-donating end-groups have been studied at hybrid density functional theory level. A computational scheme is developed to simulate a proton attached to an atom. The numerical results show that large changes in both one- and two-photon absorption properties are observed when the compound is transformed from neutral to threefold protonated states. When the compound is protonated, more charge transfer states appear and the absorption band has a red-shift. Furthermore, the two-photon absorption cross-section is largely enhanced. The theoretical calculations demonstrate the protonation effect on promoting the intramolecular charge transfer strength. The results present qualitative agreement with the experimental observations. A two-photon absorption switch with the compound TA based on the protonation effect is proposed.

One- and two-photon absorption properties of two metalloporphyrin complexes

The linear and nonlinear optical properties of two metalloporphyrin complexes formed by the complementary coordination of central zinc or magnesium ions to the ligand 5, 10, 15-tri-（p-tolyl）-20-phenylethynylporphyrin are theo- retically investigated by using the analytic response theory at the density functional theory level. The results indicate that the studied complexes present more symmetric geometry structures than the ligand. The charge-transfer states of the two complexes in the lower energy region are all almost degenerate but those of the ligand are well separated. The ratio of the two-photon absorption cross sections of the ligand, zinc-porphyrin and magnesium-porphyrin com- plexes is 1.0：1.5：1.8, demonstrating that the two-photon absorption capability can be greatly increased when the ligand is coordinated with a metal ion. Moreover, several physical micro-mechanisms including electron transitions and in- tramolecular charge-transfer processes are discussed to explore the differences in optical property between the ligand and two complexes.

Two-photon absorption of FAPbBr_(3) perovskite nanocrystals

Perovskite nanocrystals(NCs) with high two-photon absorption(TPA) cross-section are of great interest due to their potential applications in three-dimensional optical data storage and multiphoton fluorescence microscopy. Among various perovskite materials, FAPbBr_(3) NCs show a better development prospect due to their excellent stability. However, there are few reports on their nonlinear optical properties. In this work, the nonlinear optical behavior of FAPbBr_(3) NCs is studied.The methods of multiphoton absorption photoluminescence saturation and open aperture Z-scan technique were applied to determine the TPA cross-section of FAPbBr_(3)NCs, which was around 2.76 × 10^(-45)cm^(4)·s·photon^(-1) at 800 nm. In addition,temperature-dependent photoluminescence induced by TPA was investigated, and the small longitudinal optical phonon energy and electron–phonon coupling strength was obtained, which confirm the weak Pb–Br interaction. Meanwhile, it is found that the exciton binding energy in FAPbBr_(3) NCs was 69.668 me V, which may be ascribed to the strong hydrogen bond interaction. It is expected that our findings will promote the application of FAPbBr_(3) NCs in optoelectronic devices.

Theoretical Studies on One-photon and Two-photon Absorption Properties of Pyrene-core Derivatives

The analytic response theory at density functional theory level is applied to investigate onephoton and two-photon absorption properties of a series of recently synthesized pyrene-core derivatives. The theoretical results show that there are a few charge-transfer states for each compound in the lower energy region. The one-photon absorption properties of the five investigated compounds are highly consistent with those given by experimental measurements. The two-photon absorption intensities of the compounds are greatly enhanced with the increments of the molecular sizes, in which the two-photon absorption cross section of the four-branched compound is about 5.6 times of that of the mono-branched molecule. Fhrthermore, it is shown that the two-photon absorption properties are sensitive to the geometrical arrangements.

Theoretical Study on One- and Two-Photon Absorption Properties of PPV Derivative with Electron-Donor Phenylanthracene as Pendent Group

Based on the equilibrium structures from quantum mechanics AM1 method, employing INDO/CI method and the sum-over-state （SOS） formula, the one-photon absorption （OPA） and two-photon absorption （TPA） properties as well as the second hyperpolarizabilities were discussed in detail for a kind of PPV derivative poly 2-（9-phenylanthracen-10-yl）-1,4-phenylenevinylene （P1）. The results indicate that the two-photon cross section （3） increases with the increasing of the number of repeating segment （n）, however only a slight increase corresponds to the increasing of molecular weight when the repeating unit number arrives at a certain number. From this point of view, the TPA cross section values of P1 were extrapolated through the linear fit of 3 value vs. 1/n. The δ value of P1 is as high as 181 GM （1 GM=10^-50 cm^4·s·photon^-1）. Concerning the influence of pendent group and extension of π-conjugation on 3 values, another four oligomers P2, PPV, P1-1, and P2-1 were investigated for comparison. The calculation results reveal that the position and property of pendent group have great influence on the OPA and TPA properties. A most crucial role for relatively larger 3 value was played by the extension of π-conjugation.

Theoretical studies on the one-and two-photon absorption properties of azulenylporphyrins and azulene-fused porphyrins

The electronic structures, one-photon absorption （OPA） and two-photon absorption （TPA） properties of the azulenylporphyrins and azulene-fused porphyrins have been comparatively studied by using DFT/B3LYP/6-31G（d） and the ZINDO/SDCI method. With the number of azulenyl groups increasing, the OPA wavelengths of all molecules are red-shifted in 400-600 nm and the two-photon absorption cross section is gradually enlarged. The azulene-fused structures facilitate an expanding conjugated area and increasing TPA cross section. The origin of TPA properties of studied compounds is studied with a two-level model. In summary, the azulene-fused porphyrins exhibit strong two-photon absorption.

Multi-branched carbazole derivatives for two-photon absorption and two-photon excited fluorescence

Carbazole-core multi-branched chromophores 9-ethyl- 3, 6-bis （ 2- { 4- [ 5- （4-tert-butyl-phenyl） - [ 1, 3, 4 ] oxadiazol-2-yl ] - phenyl }-vinyl） -carbazole（3） and 9-ethyl-3-（ 2- {4-[ 5-（4-tert-butyl- phenyl） -[ 1, 3, 4 ] oxadiazol-2-yl ] -phenyl }-vinyl ） -carbazole （ 2 ） are synthesized through Wittig reaction and characterized by nuclear magnetic resonance（NMR）and infrared（IR）. The two- photon absorption properties of chromophores are investigated. These chromophores exhibit large two-photon absorption crosssections and strong blue two-photon excited fluorescence. The cooperative enhancement of two-photon absorption（TPA） in the multi-branched structures is observed. This enhancement is partly attributed to the electronic coupling between the branches. The electronic push-pull structures in the arm and their cooperative effects help the extended charge transfer for TPA.

Synthesis, Structure of a Symmetrically Substituted Stilbene with Strong Two-photon Absorption and Up-converted Blue Fluorescence

Efficient Ti-catalyzed reductive coupling methodology was first employed to synthesize the symmetrical bis-donor stilbene, trans-4, 4'-bis[diphenyl amino] stilbene (BDPAS). X-ray diffraction analyses reveal that this new crystal belongs to the triclinic crystal system of centro-symmetric P-1 space group. The DBPAS solution, with the linear transmission at wavelength of greater than or equal to 450 nm, possesses large two-photon absorption cross section as high as 39.4x10(-48) cm(4).s/photon resulting in strong two-photon induced blue fluorescence of 460 nm, pumped by 740 nm laser irradiation.

Two-photon Absorption and Optical Power Limiting Properties of Two Novel Dibenzothiophene-based Chromophores

Two novel V-shaped symmetric chromophores： E-2,8-bis（4-vinyl-4-carbazol-9-yl）diben- zothiophene （abbreviated as SK-G1） and E-2,8-bis（4-vinyl-4-triphenylamino） dibenzothiophene （abbreviated as ST-G1） have been synthesized and characterized. Their two photon absorption properties were measured by the open-aperture femtosecond Z-scan technique and the nanosecond nonlinear optical transmission （NLT）, respectively, when pumped by Ti： sapphire laser at 750 nm and 800 nm.

Novel triphenylamine-based two-photon absorption dyes including benzophenone parts

New two-photon absorption dyes including benzophenone parts, p-N,N-diphenylamino-p＇-phenacylstilbene （C1）, 4,4-di-（4- benzoylstyrene）yltriphenylamine （C2） and 4,4＇,4＇-tri（4-benzoylstyrene）yltriphenylamine （C3）, were synthesized and characterized by ^1H NMR and elemental analysis. The ratio of the molar extinction coefficients of compounds was approximately equal to the ratio of the branch amount of the compounds, namely, C1：C2：C3 was 1：2：3. Extremely high fluorescence quantum yields were detected for these compounds. These molecules exhibited obvious two-photon upconcerted fluorescence as excited by 800 nm Ti：sapphire femtosecond laser.

Synthesis and Two-photon Absorption Properties of s-Triazine Derivatives

Two new s-triazine derivatives, which belong to linear dipolar type and triangle octupolar type respectively, have been synthesized. The structure of the dipolar compound has been determined by X-ray diffraction. The two-photon absorption cross-section σ, and the two-photon excited fluorescence (TPEF) intensities are increased significantly from dipolar compound to octupolar compound.

Isomerism and coordination mode effects on two-photon absorption of tris(picolyl)amine-based fluorescent probes for zinc ions

One-photon absorption and two-photon absorption（TPA） properties of three tris（picolyl）amine-based zinc ion sensors are investigated by employing the density functional response theory in combination with the polarizable continuum model.The different isomer and coordination geometry of each probe are taken into account. Special emphasis is placed on the effects of isomerism and the coordination mode on the optical properties. The intra-molecular charge transfer（ICT）properties are specified by natural bond orbital charge analysis. It is shown that the isomerism has non-negligible effects on TPA properties of free ligands. It is found that both the TPA wavelength and the cross section are highly dependent on the coordination mode. When the zinc ion connects with the picolyl unit in the middle of a ligand, the zinc complex has a large TPA intensity in a long wavelength range due to the increased ICT mechanism.

Two-photon absorption properties of aggregation systems on the basis of (E)-4-(2-nitrovinyl) benzenamine molecules

Aggregation effect caused by the intermolecular hydrogen-bonding interactions on two-photon absorption prop- erties of （E）-4-（2-nitrovinyl） benzenamine molecules is studied at a hybrid density functional level. The geometry optimization studies indicate that there exist two probable conformations for the dimers and three for the trimers. A strong red-shift of the charge-transfer states is shown. The two-photon absorption cross sections of the molecule for certain conformations are greatly enhanced by the aggregation effect, from which a ratio of 1.0：2.6：3.6 is found for the molecule and its dimer and trimer with nearly planar structures. Namely, a 30 or 20 percent increase of the two-photon absorption cross section is observed.

Two-photon absorption coefficient dichroism in Ⅱ-Ⅵ semiconductor crystals

Considering two beams propagate in semiconductor crystal, this paper discusses the polarization dependence of pump beam-induced intensity attenuation of probe beam due to two-photon absorption （TPA）. Numerical calculation and experimental measurement demonstrate that TPA coefficient is polarization dependent. For homogeneous materials, probe beam attenuation arises from the imaginary part of diagonal and off-diagonal components of third-order nonlinear susceptibilities.

Observation of Two-Photon Absorption and Nonlinear Refraction in AlN

Two-photon absorption （TPA） and nonlinear refraction in AlN single crystals are revealed with the single beam Z-scan technique. A large TPA coefficient of 134-3 cm/CW at 355 nm and third-order nonlinear refractive indices of-1.91±0.38×10-13 cm2/W at 355nm, 1.79±0.36 × 10-13 cm2/W at 532nm and 1.61±0.32 ×10-12 cm2/W at 1064nm are derived. It is inferred that the TPA-generated free carriers are responsible for the large negative nonlinear refractive index at 355 nm, while the oxygen impurity induced bandgap narrowing may account for the large third-order nonlinear refractive indices at 532nm and 1064nm. The large nonlinear optical responses of AIN promise wide applications in the deep ultraviolet nonlinear optical devices.

Soliton evolution and control in a two-mode fiber with two-photon absorption

Soliton dynamics are numerically investigated in a two-mode fiber with the two-photon absorption,and the effects of the two-photon absorption on the soliton propagation and interaction are demonstrated in different dispersion regimes.Soliton dynamics depend strictly on the sign and magnitude of the group velocity dispersion(GVD)coefficient of each mode and the strength(coefficient)of the two-photon absorption.The two-photon absorption leads to the soliton collapse,enhances the neighboring soliton interaction in both modes,and increases the energy exchange between the two modes.Finally,an available control is proposed to suppress the effects by the use of the nonlinear gain with filter.

The theoretical studies on the two-photon absorption properties of symmetric l,4-bis{2-[4-(2-aryl)phenyl]vinyl}-2,5-bisdialkoxybenzenes

On the level of the time-dependent hybrid density functional theory, the one- and two-photon absorption properties of a series of symmetric 4-bis{2-[4-（2-aryl） phenyl]vinyl）-2,5-bisdialkoxybenzenes are studied respectively utilizing the analytic response theory and the few-state model methods. The calculated results show that the planarity of the geometrical structure plays a great role in enhancing the linear and nonlinear optical abilities of the molecule. However the effect of the length of the chain linked to the π-centre on the optical property is very little. For the investigated compounds, the A-π-A type charge-transfer molecules display more superior one- and two-photon absorption characteristics than the D-π-D type ones. Furthermore, the two-photon absorption results by use of few-state model are generally consistent with those by analytic response theory, demonstrating the reliability of the few-state model for evaluating the two-photon absorption cross section. The numerical simulations are in good agreement in tendency with the available experimental measurements.

Inhibition of Two-Photon Absorption in a Four-Level Atomic System with Closed-Loop Configuration

We theoretically investigate the features of two-photon absorption in a coherently driven four-level atomic system with closed-loop configuration. It is found that two-photon absorption can be completely suppressed just by properly adjusting the relative phase of four coherent low-intensity driving fields and the atomic system becomes trans- parent against two-photon absorption. From a physical point of view, we explicitly explain these results in terms of quantum interference induced by two different two-photon excitation channels.