Two-photon absorption-induced effects in femtosecond coherent anti-Stokes Raman-scattering microspectroscopy of silicon photonic components

We study the effects related to two-photon absorption (TPA) in the microspectroscopy of the silicon photonic components based on coherent anti-Stokes Raman scattering (CARS) of femtosecond pulses. With 300-fs pulses of 1.24-μm Cr:forsterite laser radiation delivering pump and probe fields and a frequency-shifted soliton output of a large-mode area photonic-crystal fiber employed as a Stokes field, pronounced TPA effects have been observed in the CARS microspectroscopy of silicon components for pump-pulse intensities exceeding 10 GW/cm².     

Two-octave spectral broadening of subnanojoule Cr:forsterite femtosecond laser pulses in tapered fibers

Spectral broadening of femtosecond Cr:forsterite laser pulses is enhanced due to the use of tapered fibers. Supercontinuum generation with unamplified subnanojoule femtosecond Cr:forsterite laser pulses is observed for the first time. With 40-fs 0.6-nJ pulses of 1.25-μm Cr:forsterite laser radiation coupled into a tapered fiber having a taper waist diameter of about 2 μm and a taper waist length of 90 mm, we observed the spectra spanning more than two octaves at the output of the fiber in the regime of anomalous group-velocity dispersion. This result opens the way for the creation of compact femtosecond Cr:forsterite laser plus tapered fiber systems for optical metrology and biomedical applications. Received: 23 October 2001 / Accepted: 16 January 2002 / Published online: 14 March 2002     

Pump-probe nonlinear absorption spectroscopy of molecular aggregates using chirped frequency-shifted light pulses from a photonic-crystal fiber

Photonic-crystal fibers provide efficient nonlinear-optical transformations of femtosecond Cr: forsterite laser pulses, delivering linearly chirped frequency-shifted broadband light pulses optimized for pump-probe nonlinear absorption spectroscopy of molecular aggregates. The blue-shifted output of a photonic-crystal fiber with a spectrum stretching from 530 to 680 nm is used to probe one-and two-exciton bands of thiacarbocyanine J aggregates in a polymer film excited by femtosecond second-harmonic pulses of the Cr: forsterite laser.     

Spectral superbroadening of subnanojoule Cr:Forsterite femtosecond laser pulses in a tapered fiber

Spectral superbroadening of subnanojoule femtosecond Cr:forsterite laser pulses is demonstrated for the first time in experiments with a tapered fiber. Coupling 40-fs 0.6-nJ pulses of 1.25-μm Cr:forsterite laser radiation into a tapered fiber with a taper waist diameter of about 2 μm and a taper waist length of 90 mm, we observed the spectra spanning more than two octaves at the output of the fiber. These experimental results open new horizons for the creation of compact femtosecond systems based on Cr:forsterite lasers and tapered fibers for optical metrology and biomedical applications.     

Femtosecond spectroscopy of coherent anti-Stokes Raman scattering with frequency-tunable chirped pulses generated in a microstructure fiber

A new scheme of chirped-pulse femtosecond coherent anti-Stokes Raman scattering spectroscopy is proposed and experimentally implemented. A theory of this modification of coherent nonlinear spectroscopy is developed. We use this approach to show that a linear time-frequency mapping defined by linearly chirped pulses allows the spectra of nonlinear response of a medium to be measured by varying the delay time between the pump pulses. Microstructure fibers with a special dispersion profile are at the heart of the experimental implementation of this technique. Such fibers are ideally suited for the generation of frequency-tunable pulses with a smooth envelope and a controlled chirp. We present the results of experimental characterization of the envelope, spectrum, and chirp of anti-Stokes pulses generated in microstructure fibers by femtosecond Cr:forsterite-laser pulses. These frequency-tunable anti-Stokes pulses produced and shaped in microstructure fibers are then employed for coherent anti-Stokes Raman scattering spectroscopy of toluene solution.     

Coherent anti-Stokes Raman scattering microspectroscopy of silicon components with a photonic-crystal fiber frequency shifter

Coherent anti-Stokes Raman scattering (CARS) microspectroscopy of silicon components is demonstrated with pump and probe fields delivered by a mode-locked Cr:forsterite laser and the frequency-shifted soliton output of a photonic-crystal fiber as a Stokes field. CARS microspectroscopy is shown to allow a visualization of microscale features and defects on the surface of silicon wafers, offering much promise for online diagnostics of electronic and photonic silicon chip components.     

Frequency-shifted megawatt soliton output of a hollow photonic-crystal fiber for time-resolved coherent anti-Stokes Raman scattering microspectroscopy

Hollow-core photonic-crystal fibers (PCFs) provide soliton delivery and frequency shifting of 2.8 MW femtosecond pulses with an input central wavelength of 618 nm. The frequency-shifted megawatt soliton output of the hollow PCF is used as a high-peak-power Stokes field for coherent anti-Stokes Raman scattering (CARS) microspectroscopy, providing a dynamic range of nearly four decades for anti-Stokes signal detection, thus enabling time-resolved CARS studies of ultrafast relaxation processes on time scales from tens of femtoseconds up to tens of picoseconds.     

Highly sensitive single-beam heterodyne coherent anti-Stokes Raman scattering

Single-beam coherent anti-Stokes Raman-scattering (CARS) microspectroscopy achieves a complete CARS scheme with a femtosecond laser. Here, we introduce heterodyne detection in a simple experimental extension: the optical fields driving the CARS process and the local oscillator used for heterodyning are derived from a single beam of ultrashort laser pulses by pulse shaping. The heterodyne signal is amplified by more than 3 orders of magnitude and is linearly dependent on the concentration of Raman scatterers. This dramatically increases the sensitivity of chemically selective detection at microscopic resolution while maintaining the simplicity of the single-beam setup.     

Tunable light source for coherent anti-Stokes Raman scattering microspectroscopy based on the soliton self-frequency shift

We present a photonic crystal fiber (PCF)-based light source for generating tunable excitation pulses (pump and Stokes) that are applicable to coherent anti-Stokes Raman scattering (CARS) microspectroscopy. The laser employed is an unamplified Ti:sapphire femtosecond laser oscillator. The CARS pump pulse is generated by spectral compression of a laser pulse in a PCF. The Stokes pulse is generated by redshifting a laser pulse in a PCF through the soliton self-frequency shift. This setup allows for probing up to 4000 cm(-1) with a spectral resolution of approximately 25 cm(-1). We characterize the stability and robustness of CARS microspectroscopy employing this light source.     

Selective excitation and suppression of coherent anti-Stokes Raman scattering by shaping femtosecond pulses

Femtosecond coherent anti-Stokes Raman scattering (CARS) suffers from poor selectivity between neighbouring Raman levels due to the large bandwidth of the femtosecond pulses. This paper provides a new method to realize the selective excitation and suppression of femtosecond CARS by manipulating both the probe and pump (or Stokes) spectra. These theoretical results indicate that the CARS signals between neighbouring Raman levels are differentiated from their indistinguishable femtosecond CARS spectra by tailoring the probe spectrum, and then their selective excitation and suppression can be realized by supplementally manipulating the pump (or Stokes) spectrum with the $\pi $ spectral phase step.     

飞秒激光在双折射微结构光纤中模式控制的四波混频效应的实验研究

利用飞秒激光脉冲在长度为10cm，包层具有大空气比的双折射微结构光纤中通过高阶模相位 匹配的四波混频获得了波长可调谐的反斯托克斯波.实验中脉冲宽度为35fs，中心波长820nm ，单脉冲能量4nJ的飞秒激光脉冲耦合到长轴直径为5μm，短轴为46μm的双折射微结构光 纤中.在高阶模传输情况下，通过调制耦合光的偏振方向，获得了具有不同中心波长的反斯 托克斯波.通过对比分析，讨论了输入光的偏振态对双折射微结构光纤中高阶模式下四波混 频效应的影响情况.理论计算分析很好的解释了实验结果. 关键词： 微结构光纤 飞秒脉冲激光 四波混频     

Fourier-transform coherent anti-Stokes Raman scattering microscopy

We report a novel Fourier-transform-based implementation of coherent anti-Stokes Raman scattering (CARS) microscopy. The method employs a single femtosecond laser source and a Michelson interferometer to create two pulse replicas that are fed into a scanning multiphoton microscope. By varying the time delay between the pulses, we time-resolve the CARS signal, permitting easy removal of the nonresonant background while providing high resolution, spectrally resolved images of CARS modes over the laser bandwidth (approximately 1500 cm(-1)). We demonstrate the method by imaging polystyrene beads in solvent.     

Phase-matched four-wave mixing of isolated waveguide modes of high-intensity femtosecond pulses in a hollow photonic-crystal fiber

Hollow-core photonic-crystal fibers with a special dispersion profile are shown to allow phase-matched nonlinear optical interactions of isolated air-guided modes of high-intensity femtosecond laser pulses confined in the hollow fiber core. We present theoretical and experimental studies of the four-wave mixing of fundamental and second-harmonic pulses of a Cr:forsterite laser with an initial pulse duration of about 50 fs and an intensity on the order of 10¹⁴ W/cm² in waveguide modes of a hollow photonic-crystal fiber with a core diameter of about 13μm.     

Controlled light localization and nonlinear-optical interactions of ultrashort laser pulses in micro-and nanostructured fibers with a tunable photonic band gap

Physical principles behind the control of light localization and nonlinear-optical interactions in micro-and nanostructured fibers are demonstrated. Transmission measurements on the cladding of nanostructured fibers having a form of a two-dimensional periodic structure with a pitch less than 500 nm have revealed the existence of a photonic band gap tunable within the range from 930 to 1030 nm. The influence of the structure of the holey-fiber cladding on the effective area of the waveguide mode and the spectral broadening of Ti:sapphire and Cr:forsterite femtosecond laser pulses is experimentally studied. It is shown that the increase in the air-filling fraction of a holey-fiber cladding results in a considerable enhancement of spectral broadening of short laser pulses due to the increase in the light localization degree in the fiber core.     

Tuning the frequency of ultrashort laser pulses by a cross-phase-modulation-induced shift in a photonic crystal fiber

Femtosecond pulses of fundamental Cr:forsterite laser radiation are used as a pump field to tune the frequency of copropagating second-harmonic pulses of the same laser through cross-phase modulation in a photonic crystal fiber. Sub-100-kW femtosecond pump pulses coupled into a photonic crystal fiber with an appropriate dispersion profile can shift the central frequency of the probe field by more than 100 nm, suggesting a convenient way to control propagation and spectral transformations of ultrashort laser pulses.     

Frequency conversion of subnanojoule femtosecond pulses in microstructure fibers

We experimentally demonstrate highly efficient multiplex frequency conversion of unamplified subnanojoule femtosecond pulses of Ti:sapphire laser radiation in fused silica microstructure fibers. Nonlinear optical spectral transformation of femtosecond pulses in an array of fused silica threadlike channels in these microstructure fibers results in the generation of isolated anti-Stokes spectral components within the wavelength range of 400–500 nm. An efficiency of frequency conversion of about 20% is achieved for 800-nm pump pulses with an energy of 0.7 nJ and a pulse duration of 70 fs.     

Multiplying the repetition rate of passive mode-locked femtosecond lasers by an intracavity flat surface with low reflectivity

By inserting a low-reflectivity flat surface inside the oscillator cavity, we demonstrate a flexible and phase-insensitive method for multiplying the repetition rate of a femtosecond passive mode-locked solid-state laser. Without mode matching and feedback control, we successfully multiplied the repetition rate of a passively mode-locked Cr:forsterite laser from 124 MHz to 1.24 GHz. High-repetition-rate femtosecond optical pulses with average power of >100 mW can be obtained with the demonstrated method.     

Broadband coherent anti-Stokes Raman scattering light generation in BBO crystal by using two crossing femtosecond laser pulses

As broad as 12000 cm(-1) coherent anti-Stokes Raman scattering (CARS) light from ultraviolet to infrared was generated in a BBO crystal by using two crossing femtosecond laser pulses with 30% conversion efficiency. More than fifteenth-order anti-Stokes and second-order Stokes Raman sidebands were observed with nice Gaussian spatial mode. The effect of the crossing angle between two input beams on the spectrum and emitting angle of the Raman sidebands was studied in detail. Calculation shows that the phase-matching condition determines the frequencies and angles of the sidebands.     

Quantum-dot-based saturable absorber for femtosecond mode-locked operation of a solid-state laser

A quantum-dot-based saturable absorber has been demonstrated to initiate the generation of femtosecond pulses from a passively mode-locked solid-state laser. Control and tuning of the pulse duration from 58 ps to 158 fs was achieved. The 158 fs transform-limited pulses at 1280 nm are the shortest pulses that were produced from the Cr:forsterite laser passively mode locked by an InAs/InGaAs quantum-dot semiconductor saturable absorber mirror.     

Efficient anti-Stokes generation through phase-matched four-wave mixing in higher-order modes of a microstructure fiber

Phase-matched four-wave mixing in higher-order modes of microstructure fibers allows unprecedentedly high efficiencies of anti-Stokes frequency conversion to be achieved for subnanojoule femtosecond laser pulses. 70-fs pulses of 790-nm radiation were used to generate an anti-Stokes component at 520-530 nm in a higher-order mode of a microstructure fiber with a 4.8-microm core. The maximum ratio of the anti-Stokes signal energy to the energy of the pump component in the output spectrum is estimated as 1.7.