Ultrafast femtosecond all-optical modulation through nondegenerate two-photon absorption in silicon-on-insulator waveguides

We present numerical investigations of ultrafast femtosecond (with time duration of 100 fs at 1/e intensity point) all-optical modulation of a pump-probe wave arrangement by using nondegenerate two-photon absorption (TPA), namely cross absorption, inside silicon-on-insulator (SOI) optical waveguides. Our results show that when a pump pulse with femtosecond duration and a continuous probe wave are co-propagating along the SOI, the probe wave can be modulated inversely by the ultrafast pump pulse, whose modulation depth depends strongly on the system parameters such as the waveguide length, the peak power and initial chirp of the pump wave, the group velocity dispersion (GVD), etc.; this means that the modulation depth can be improved by an appropriate increase of the waveguide length, the pump peak, and the initial chirp, in addition, which has a larger value for the probe wavelength in the normal dispersion regime compared with the case of abnormal dispersion when the center wavelength of the pump wave is located at the zero-dispersion wavelength.     

Ultrafast all-optical shutter based on two-photon absorption

An ultrafast all-optical shutter is presented, based on a simple two-color, two-photon absorption technique. For time-resolved luminescence measurements, this shutter is an interesting alternative to the optical Kerr gate. The rejection efficiency is 99%; the switching-off and switching-on speeds are limited by the pulse length only; the rejection time is determined by the crystal slab thickness; and the bandwidth spans the entire visible spectrum. We show that our shutter can also be used for accurate measurement of group velocity inside a transparent material.     

Ultrafast dynamics of three novel oligomers with strong two-photon absorption properties

A comparative study of the nonlinear optical properties and ultrafast dynamics of three oligomers were carried out using femtosecond laser spectroscopic techniques. All oligomers showed intense fluorescence emission induced by a two-photon absorption process. Relaxation features with parallel and perpendicular polarization configurations were investigated in a one-color pump–probe experiment at 400 nm. Two relaxation components were assigned to the exciton migration and exciton recombination processes, respectively. Time-resolved fluorescence results showed that the electron–phonon interaction happens on the picosecond-scale, while the recombination lifetimes of the excited state are relatively long. PACS 33.80.Rv; 34.30.+h; 82.53.-k; 82.35.Ej     

Ultrafast pulse compression by semiconductor two-photon gain

We demonstrate experimentally the compression of femtosecond-scale pulses by two-photon gain in a compact electrically driven AlGaAs waveguide. Dynamic control of the pulse width from 240 to 140 fs is achieved by varying the current injection levels--in good agreement with the calculations. The pulse width is measured by a high-sensitivity intensity autocorrelator based on two-photon absorption in a GaAs photomultiplier tube.     

Infrared free-electron laser measurement of power limiting by two-photon absorption in InSb

We have performed the first experiment on the free-electron laser (CLIO) at the Laboratoire pour l'Utilisation du Rayonnement Électromagnétique (LURE). In a transmission experiment we observed strong power limiting at wavelengths longer than the absorption edge associated with induced free carrier absorption produced by direct interband two-photon transitions in InSb. We have estimated the two-photon absorption (TPA) coefficient () of InSb at 8.9 m to be 2 cm MW^-1, by fitting the power-limiting effect with a simple theoretical model. An important feature of this result is that we are utilizing the broad tunability of the FEL to explore the TPA theory to shorter wavelengths than hitherto available with CO₂ lasers. The result is in broad agreement with the longer-wavelength measurements of Sheik-Bahae et al.     

Impact of two-photon absorption on self-phase modulation in silicon waveguides

We study the effects of two-photon absorption on the self-phase modulation (SPM) process in silicon waveguides while including both free-carrier absorption and free-carrier dispersion. An analytical solution is provided in the case in which the density of generated carriers is relatively low; it is useful for estimating spectral bandwidth of pulses at low repetition rates. The free-carrier effects are studied numerically with emphasis on their role on the nonlinear phase shift and spectral broadening. We also consider how the repetition rate of a pulse train affects the SPM process.     

Simulating resonance-mediated two-photon absorption enhancement in rare-earth ions by a rectangle phase modulation

Improving the up-conversion luminescence efficiency of rare-earth ions via the multi-photon absorption process is crucial in several related application areas. In this work, we theoretically propose a feasible scheme to enhance the resonance-mediated two-photon absorption in Er~(3+) ions by shaping the femtosecond laser field with a rectangle phase modulation. Our theoretical results show that the resonance-mediated two-photon absorption can be decomposed into the on-resonant and near-resonant parts, and the on-resonant part mainly comes from the contribution of laser central frequency components, while the near-resonant part mainly results from the excitation of low and high laser frequency components.So, the rectangle phase modulation can induce a constructive interference between the two parts by properly designing the modulation depth and width, and finally realizes the resonance-mediated two-photon absorption enhancement. Moreover, our results also show that the enhancement efficiency of resonance-mediated two-photon absorption depends on the laser pulse width(or laser spectral bandwidth), final state transition frequency, and intermediate and final state absorption bandwidths. The enhancement efficiency modulation can be attributed to the relative weight manipulation of on-resonant and near-resonant two-photon absorption in the whole excitation process. This study presents a clear physical insight for the quantum control of resonance-mediated two-photon absorption in the rare-earth ions, and there will be an important significance for improving the up-conversion luminescence efficiency of rare-earthions.     

Sensitive measurement of nonlinear refraction and two-photon absorption by spectrally resolved two-beam coupling

A simple and very sensitive method for determining refractive and absorptive nonlinearities based on spectral resolution of two-beam coupling is demonstrated. Nonlinear phase shifts as small as ~10(-6) rad and two-photon absorption coefficients as small as 10(-4) cm/GW are readily observed by use of this technique with nanojoule pulses from a mode-locked laser.     

Contrast ratio variation caused by radiation attenuation in pulse width measurement by two-photon absorption fluorescence

In the technique for measuring pulse width by two-photon absorption fluorescence, theoretical calculations indicate that one can hope to obtain a maximum contrast ratio of three between the point at which the two peaks overlap and the point at which there is no superposition. Nevertheless, this calculation has been carried out assuming that the pulse is not attenuated as it traverses the fluorescent medium. In this paper it will be shown that this attenuation gives rise to a decrease in the contrast ratio. As the fluorescence intensity is proportional to the absorption, an increase in the former will be to the detriment of the contrast ratio. We will attempt to give a criterion for the selection of experimental conditions which lead to maximum intensity without an appreciable decrease in the contrast ratio.     

Photochromism induced by infrared two-photon absorption

An IR laser of 940 nm wavelength induced photochromic reaction in acrylate that contained both spirobenzopyran and rare-earth doped oxide (Gd(2)O(2)S:YbEr). The rare-earth elements were excited by two 940 nm photons and emitted a 550 nm photon, which caused photochromic isomerization of spirobenzopyran. This acrylate turned to its original orange color by either thermal relaxation or ultraviolet irradiation, and was bleached again by IR laser irradiation.     

Photorefractive polymers sensitized by two-photon absorption

We demonstrate the recording of holograms and their nondestructive readout in a photorefractive polymer, using two-photon absorption. Sensitivity is provided by the excitation of the electroactive chromophore with femtosecond pulses, followed by charge injection into the photoconducting poly(N -vinylcarbazole) matrix. The holograms can be fully erased with a pulsed laser source but are insensitive to cw laser beams with the same wavelength. Studies of the field and intensity dependence of the diffraction efficiency indicate that the holograms are formed through the photorefractive effect.     

Exciton-polaritons by two-photon absorption in semiconductors

The creation of excitonic polariton states by two-photon absorption is theoretically investigated. A semi-classical approach is adopted to compute the two-photon transition probability to polariton states through an intermediate exciton state. The numerical results in CuCl show two peaks corresponding to the longitudinal exciton and transverse polariton states, respectively. These results are in good agreement with the experiment.     

Calorimetric measurement of two-photon absorption and color-center formation in ultraviolet-window materials

Intensity-dependent absorption of 25 ns excimer laser pulses in common UV-window materials was investigated. By employing a calorimetric technique which provides greatly enhanced sensitivity compared to transmissive measurements, two-photon absorption coefficients were determined at intensities of 2–80 MW/cm² and found to be in good agreement with previous measurements at 10–100 GW/cm². Also, color-center formation in fused silica was observed. It was possible to quantify transient and cumulative effects as a function of intensity.     

Excitonic molecule in semiconductors by two-photon absorption

Direct creation of bi-exciton states by two-photon absorption in direct gap semiconductors is investigated theoretically. A numerical application to the case of CuCl shows that the two-photon absorption coefficient for bi-excitonic transitions is larger than that for two-photon interband transitions by three orders of magnitude. It becomes comparable to that for one-photon excitonic transitions for available laser intensities. The main contribution to this enhancement of the absorption coefficient for the transitions to the bi-exciton states is found to be from the resonance effect.     

Squeezing in two-photon absorption

The conditions for homodyne detection of squeezing are related to the density matrix of the squeezed light. It is shown that coherent light subjected to two-photon absorption for an appropriate length of time develops a small amount of squeezing.     

Adaptive pulse compression by two-photon absorption in semiconductors

We investigate the adaptive optimization of broadband laser pulses, using a closed-loop learning algorithm in which the merit function is derived from two-photon absorption in semiconductors. Photoluminescence experiments with CdS thin films and photocurrent measurements of a GaAsP photodiode have been performed. The experimental data demonstrate that reliable and accurate pulse compression to the bandwidth limit can be achieved, unperturbed by nontrivial phase effects. Therefore two-photon absorption proves to be an easy-to-implement alternative to second-harmonic generation for the compression of broadband laser pulses.     

Exciton molecule in semiconductors by phonon-assisted two-photon absorption

Direct creation of bi-excitonic states by photon-assisted two-photon absorption in indirect-gap semiconductors is investigated theoretically. The symmetry of the indirect bi-exciton states and of the phonon used are given for the case of Ge. A numerical application to the case of Si shows that the indirect two-photon absorption coefficient for bi-excitonic α²_I (bi-ex) transitions is several orders of magnitude larger than both indirect two-photon interband, α²_I (band), and excitonic, α²_I (exc), transitions. It becomes smaller than both indirect one-photon interband, α¹_I (band), and excitonic, α¹_I (exc), transitions for available laser intensities. The essential contribution to this enhancement of α²_I (bi-ex) is found to be from the resonance effect in the first process and from both the resonance effect and matrix elements included in the second process.     

Ultrafast Raman loss spectroscopy

This paper deals with a new form of nonlinear Raman spectroscopy called ‘ultrafast Raman loss spectroscopy (URLS)’. URLS is analogous to stimulated Raman spectroscopy (SRS) but is much more sensitive than SRS. The signals are background (noise) free unlike in coherent anti‐Stokes Raman spectroscopy (CARS) and it provides natural fluorescence rejection, which is a major problem in Raman spectroscopy. In addition, being a self‐phase matching process, the URLS experiment is much easier than CARS, which requires specific phase matching of the laser pulses. URLS is expected to be alternative if not competitive to CARS microscopy, which has become a popular technique in applications to materials, biology and medicine. Copyright © 2009 John Wiley & Sons, Ltd.