Optical parametric oscillators/amplifiers

In order to achieve a reasonable signal strength from the nonlinear response of approximately one atomic monolayer at an interface, a laser source with high peak power is generally required. Conuuon sources include Q-switched ( 10 ns pulsewidth) and mode-locked ( 100 ps) Nd YAG lasers, and mode-locked ( 10 fs-1 ps) Ti sapphire lasers. Broadly tunable sources have traditionally been based on dye lasers. More recently, optical parametric oscillator/amplifier (OPO/OPA) systems are coming into widespread use for tunable sources of both visible and infrared radiation. 

For 2PA or ESA spectral measurements, it is necessary to use tunable laser sources where optical parametric oscillators/amplifiers (OPOs/OPAs) are extensively used for nonlinear optical measurements. An alternative approach, which overcomes the need of expensive and misalignment prone OPO/OPA sources, is the use of an intense femtosecond white-light continuum (WLC) for Z-scan measurements [71,72]. Balu et al. have developed the WLC Z-scan technique by generating a strong WLC in krypton gas, allowing for a rapid characterization of the nonlinear absorption and refraction spectra in the range of 400-800 nm [72]. 

Still an alternative way for tuning is to mix fix-frequency terawatt radiation (cOf) with tuneable radiation (o from an optical parametric oscillator/amplifier [29], which is pumped by a fraction of the fixed-frequency output. This is done in a pulsed rare-gas jet, where new frequency components ncOf mco are generated. Here, n normally is a large number and m a small number. Promising results have been obtained [30,31]. 

It is well known that by inserting an optical amplifier obtained by population inversion in an optical cavity, one can realize sources of coherent radiations, namely lasers. One can operate in the same way with parametric amphfication as shown on Fig. 1. A nonlinear crystal illuminated by an input pump is inserted in an optical cavity. This cavity is represented for convenience as a ring cavity but consists usually of a linear cavity. An important difference with the laser is that there are three different fields, insfead of one, which are presenf in the amplifying medium, all these fields being able to be recycled by the cavity mirrors. One obtain thus different types of "Optical Parametric Oscillators" or OPOs. 

Optical parametric oscillator (OPO, see 20) is the real equivalent to the radio frequency shifter however OPO can be replaced by a simple addition of a local oscillator (e.g. laser) through a beam splitter. Multiplication takes place at the level of detectors. For sake of S5mimetry, detectors can be placed at both output of the beam splitter, the intermediate frequency is then the output of the differential amplifier. 

This positive development is partly based on new experimental techniques, such as improvements of existing lasers and the invention of new laser types, the realization of optical parametric oscillators and amplifiers in the femtosecond range, the generation of attosecond pulses, the revolution in the measurements of absolute optical frequencies and phases of optical waves using the optical Ifequency comb, or the different methods developed for the generation of Bose-Einstein condensates of atoms and molecules and the demonstration of atom lasers as a particle equivalent to photon lasers. 

The Optical Parametric Oscillator (OPO) process should also be mentioned. Here a nonlinear crystal in a cavity is used to generate two new frequencies (oji and 0J2) out of a single one (a ) that is used to pump the crystal. Energy conservation requires Ui- U 2 = ct . The frequency division between the two new waves (the signal and the idler) is chosen by the phase matching condition. The parametric process can also be used in Optical Parametric Amplifiers (OPA). Parametric laser light generation was reviewed in [8.77,78]. 

Unfortunately, powerful IR lasers tunable over a significant frequency range are difficult to obtain. Currently, the most effective but highly demanding approach to this end is represented by the free-electron laser (FEL). FEL facilities are limited and offer access for researchers to perform their experiments at dedicated ports on a tight schedule (Fig. 9.35). Alternatively, optical parametric oscil-lator/amplifiers (OPO/As) can serve as tunable IR light sources [139,156]. 

Numerical aperture Nematic liquid crystal Optical coherent tomography Optical parametric amplifier Optical parametric oscillator Photo multiplier tube Nonlinear polarization Picosecond... 

Up to now, the most common laser sources used for CARS microscopy are based on Tirsapphire or Nd YVO lasers with pulse durations from tens of femtoseconds up to 10 ps. Different approaches are possible in order to generate pump and Stokes beams use of two femtosecond laser sources electronically synchronized [19], pumping of an optical parametric amplifier (OPA) to produce the Stokes beam and use of the residual pump as pump beam [18], pumping of an optical parametric oscillator (OPO) to obtain the pump beam and use the residual pump light as Stokes [20], using signal and idler beams from a synchronously pumped OPO to provide directly the two excitation beams [11, 21]. 

Figure 3 Schematic representation of a singly-resonant optical parametric oscillator. Pump wave of frequency cop, (reflected) signal wave of frequency os, idler wave of frequency a>. The signal wave (Os becomes amplified. 6p denotes the angle of orientation of the direction of propagation with respect to the crystal optic axis. Adapted with permission from Tang CL and Cheng LK (1995) Fundamentals of Optical Parametric Processes and Oscillators. Amsterdam Harwood Academic Publishers.

These limitations have recently been eliminated using solid-state sources of femtosecond pulses. Most of the femtosecond dye laser teclmology that was in wide use in the late 1980s [11] has been rendered obsolete by tliree teclmical developments the self-mode-locked Ti-sapphire oscillator [23, 24, 25, 26 and 27], the chirped-pulse, solid-state amplifier (CPA) [28, 29, 30 and 31], and the non-collinearly pumped optical parametric amplifier (OPA) [32, 33 and 34]- Moreover, although a number of investigators still construct home-built systems with narrowly chosen capabilities, it is now possible to obtain versatile, nearly state-of-the-art apparatus of the type described below Ifom commercial sources. Just as home-built NMR spectrometers capable of multidimensional or solid-state spectroscopies were still being home built in the late 1970s and now are almost exclusively based on commercially prepared apparatus, it is reasonable to expect that ultrafast spectroscopy in the next decade will be conducted almost exclusively with apparatus ifom conmiercial sources based around entirely solid-state systems. 

The laser system consisted of a home-built Ti sapphire fs laser oscillator and regenerative amplifier (RGA). The pulse duration was 50 fs at 800 nm and 1 kHz repetition rate. The output of the RGA was split into two parts. One part was used as pump pulse. The other part served as a source for the generation of probe pulses with the help of a non-collinear optical parametric amplifier (NOPA, Clark). The sample preparation was explained elsewhere [7]. Briefly, sodium (Alfa Aesar) was used as received and sodium bromide (Alfa Aesar) was dried and re-crystallized under vacuum. The preparation of the samples was carried out in a glovebox under argon atmosphere. Localized electrons were generated by heating the metal-salt mixture to 800 °C, i.e. well above the melting point of the salt. 

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