Bing Gu

Ultrafast optical nonlinearities and figures of merit in acceptor-substituted 3,4,5-trimethoxy chalcone derivatives: Structure-property relationships

By performing both Z-scan and transient transmission measurements with 130 fs laser pulses in the near infrared region, we investigated structure-property relationships for χ(3) in acceptor-substituted 3,4,5-trimethoxy chalcone derivatives. We determined all nonlinear parameters, including two-photon absorption (2PA) cross section, 2PA-induced excited-state absorption (ESA) cross section, microscopic second-order hyperpolarizability, and lifetime of the excited state in these molecules. We found that the microscopic second-order hyperpolarizability γR and 2PA cross section σ2PA in chalcone derivatives increase as the acceptor strength of the molecules increases, which demonstrates an enhancement in optical nonlinearities by simple structural variations. We evaluated the one-photon, two-photon, and effective three-photon figures of merit for acetone solutions of chalcone derivatives at irradiance of 100 GW/cm2. Furthermore, we observed optical limiting behavior in these compounds, which result from both 2P...

Two-photon-induced excited-state absorption: Theory and experiment

We develop an open-aperture (OA) Z scan and nonlinear transmission theory of two-photon-induced excited-state absorption, under the excitation of spatial Gaussian laser pulses with temporal Gaussian and hyperbolic secant profiles. The found analytic expressions allow us to straightforwardly fit the OA Z-scan trace and the nonlinear transmission curve, for convenient extraction of the nonlinear absorption coefficients. As a test, the two-photon-induced excited-state absorption in a chalcone derivative of 3,4-dimethoxy-4′-fluorochalcone is explored by performing femtosecond Z-scan measurement and is analyzed by our theory.

Giant optical nonlinearity of a Bi2Nd2Ti3O12 ferroelectric thin film

We investigate the optical nonlinearity of a Bi2Nd2Ti3O4 ferroelectric thin film using the top-hat Z scan technique at a wavelength of 532nm with 35ps duration pulses. The film exhibits the fast and giant optical nonlinearities having the two-photon absorption coefficient of 3.1×104cm∕GW and the nonlinear refraction coefficient of 0.7cm2∕GW, respectively. The mechanism of the optical nonlinearity is discussed in detail. In particular, we also give two important formulas for the top-hat Z scan, which are very valuable and helpful for estimating the nonlinear optical coefficients when the material possesses the simultaneous nonlinear absorption and nonlinear refraction.

Nonlinear optical properties of 2,4,5-Trimethoxy-4-nitrochalcone: observation of two-photon-induced excited-state nonlinearities.

We report experimental investigations of optical nonlinearities and nonlinear dynamics in acetone solution of 2,4,5-Trimethoxy-4- nitrochalcone. By performing Z-scans with femtosecond laser pulses at low excitation intensity, two-photon absorption (2PA) and third-order nonlinear refraction are measured. As laser excitation intensity exceeds a critical value, however, the interplay between third- and fifth-order nonlinearities is observed. It is also confirmed that fifth-order processes mainly originate from 2PA-induced excited-state nonlinearities by conducting femtosecond time-resolved degenerate pump-probe measurements. All the nonlinear parameters are determined unambiguously in the near infrared region of the 2PA cross-section, second-order hyperpolarizability, excited-state absorption cross-section, excited-state refraction cross-section, lifetime of excited states induced by 2PA, and critical population of the excited states in 2,4,5-Trimethoxy-4-nitrochalcone molecule.

Z-scan theory for material with two- and three-photon absorption

We present a theoretical study on the Z-scan characteristics of thin nonlinear optical media with simultaneous two- and three-photon absorption, a situation that exists, for example, in polydiacetylenes. With the introduction of a coupling function between two- and three-photon absorption, we find a quasi-analytic expression for open aperture Z-scan traces. We make a comparison of the analytic solutions with numerical solutions in detail, showing that they are in good agreement. This theoretical result allows us to easily identify and determine simultaneously the two- and three-photon absorption coefficients from the open aperture Z-scan traces.

Two-dimensional microstructures induced by femtosecond vector light fields on silicon

We have fabricated the complicated two-dimensional subwave-length microstructures induced by the femtosecond vector light fields on silicon. The fabricated microstructures have the interval between two ripples in microstructures to be around 670-690 nm and the depth of the grooves to be about 300 nm when the pulse fluence of 0.26 J/cm2 is slightly higher than the ablated threshold of 0.2 J/cm2 for silicon under the irradiation of 100 pulses. The ripples are always perpendicular to the direction of the locally linear polarization. The designable spatial structure of polarization of the femtosecond vector light field can be used to manipulate the fabricated microstructure.

Z-scan theory of two-photon absorption saturation and experimental evidence

In our article [B. Gu, Y. X. Fan, J. Wang, J. Chen, J. P. Ding, H. T. Wang, and B. Guo, Phys. Rev. A 73, 065803 (2006)] we have presented the theory of open-aperture Gaussian-beam Z-scan, based on the Adomian decomposition method, which is available only for the saturable absorption caused by single-photon absorption transition. In the present article, using the same technique (Adomian decomposition method, as a common technique), we develop an open-aperture Z-scan theory for evaluating the property of the saturable absorption originating from two-photon absorption (2PA) transition, when a spatial Gaussian beam is used as the excitation source. We find analytic polynomial expressions of the Z-scan traces for a continuous wave laser or a temporal Gaussian pulsed laser. As the experimental evidence, we investigate the saturable 2PA behaviors caused by the interband two-photon transition in the direct-gap II–VI semiconductors CdS, CdSe, ZnSe, and ZnTe, under the excitation condition of a femtosecond laser wi...

Two-photon-induced excited-state nonlinearities.

We report a theoretical investigation of laser-pulse-duration dependence of excited-state nonlinearities induced by two-photon absorption (2PA). We investigate the spatiotemporal characteristics of the transmitted pulses caused by 2PA-induced excited-state absorption, which strongly depends on laser pulse duration. By taking into account 2PA cross-section, excited-state photophysical properties, as well as laser pulse duration, we quantitatively determine the effective fifth-order nonlinearities caused by excited-state absorption and refraction. The results are capable of predicting the magnitude of 2PA-induced excited-state nonlinearities on the time scales where laser pulse duration is less than or comparable to the lifetime of 2PA-induced excited states. We also develop Z-scan theories for quickly yet unambiguously estimation of 2PA coefficient, third-order nonlinear refraction index, and excited-state absorption and refraction cross-sections.

Three-photon absorption saturation in ZnO and ZnS crystals

We reported the observation of the saturation of interband three-photon absorption (3PA) in wide-gap semiconductors under intense femtosecond laser excitation. Theoretically, we developed a 3PA saturation model that is in agreement with the Z-scan experimental results. The characteristic saturation intensities were determined to be 44 and 210GW∕cm2 for ZnO and ZnS crystals, respectively. The 3PA saturation model is also consistent with the ultrafast dynamics of 3PA-generated charge carriers in ZnO and ZnS crystals, obtained from the femtosecond transient absorption measurements.

Theory of Gaussian beam Z scan with simultaneous third- and fifth-order nonlinear refraction based on a Gaussian decomposition method

We present a detailed theoretical investigation on the Gaussian beam Z scan for arbitrary aperture and arbitrary nonlinear refraction phase shifts, based on the Gaussian decomposition method, including cases when the medium exhibits the single (2n+1)th-order nonlinear refraction effect and the simultaneous third- and fifth-order nonlinear refraction effects. We find the optimum sum upper limit, which is of great importance to fit the Z-scan traces and extract the nonlinear refraction coefficients related to the third- and fifth-order effects. This method has not only a high accuracy but is also time saving. We also discuss the influence of two-photon absorption on the Z-scan traces when materials possess the simultaneous third- and fifth-order nonlinear refraction effects associated with the two-photon absorption using the fast Fourier transform.