Ultrafast laser

Lasers, Chemical Lasers, Color Center Lasers, Dye Lasers, Free Electron Lasers, Gas Lasers, Nuclear Pumped Lasers, Optical Fiber Lasers, Semiconductor Lasers, Solid State Lasers, Ultrafast Pulse TLchnology Lasers, X-Ray... 

Cryogenic Process Engineering Lasers Lasers, Dye Lasers, Excimer Lasers, Ultrafast Pulse Technology... 

Acousto-Optics Lasers Lasers, Semiconductor Lasers, Ultrafast Pulse Technology Light Emitting Diodes... 

In the last two decades, thanks to the advance of stable laser, ultrafast electronics, and personal computer, LLS (especially dynamic LLS) has evolved from a very special instrument for physicists and physical chemists to a routine analytical tool in polymer laboratories or even to a daily quality-control device in production lines. Commercially available research-grade LLS instruments (eg, ALV, Germany, and Brookhaven, U.S.A.) are capable of making static and dynamic measurements simultaneously for studies of colloidal particles in suspensions or macromolecules in solutions as well as in gels and viscous media. 

Electron Transfer Reactions Coherent Control OF Chemical Reactions Lasers, Ultrafast Pulse ItecHNOLOGY Luminescence Molecular Beam Epitaxy, Semiconductors Nanostructured Materials, Chemistry of Noni.inf.ar Optical Processes... 

According to Kramers model, for flat barrier tops associated with predominantly small barriers, the transition from the low- to the high-damping regime is expected to occur in low-density fluids. This expectation is home out by an extensively studied model reaction, the photoisomerization of tran.s-stilbene and similar compounds [70, 71] involving a small energy barrier in the first excited singlet state whose decay after photoexcitation is directly related to the rate coefficient of tran.s-c/.s-photoisomerization and can be conveniently measured by ultrafast laser spectroscopic teclmiques. 

Albrecht A C, Smith S P, Tan D, Schaertel S A and DeMott D 1995 Ultrasharp spectra and ultrafast timing from noisy coherence in four wave mixing Laser Rhys. 5 667-75... 

Free-electron lasers have long enabled the generation of extremely intense, sub-picosecond TFlz pulses that have been used to characterize a wide variety of materials and ultrafast processes [43]. Due to their massive size and great expense, however, only a few research groups have been able to operate them. Other approaches to the generation of sub-picosecond TFlz pulses have therefore been sought, and one of the earliest and most successfid involved semiconducting materials. In a photoconductive semiconductor, carriers (for n-type material, electrons)... 

Especially with LTG GaAs, materials became available that were nearly ideal for time-resolved THz spectroscopy. Due to the low growth temperature and the slight As excess incorporated, clusters are fonned which act as recombination sites for the excited carriers, leading to lifetimes of <250 fs [45], With such recombination lifetunes, THz radiators such as dipole anteimae or log-periodic spirals placed onto optoelectronic substrates and pumped with ultrafast lasers can be used to generate sub-picosecond pulses with optical bandwidths of 2-4 THz. Moreover, coherent sub-picosecond detection is possible, which enables both... 

Wokosin D L, Centonze V, White J G, Armstrong D, Robertson G and Ferguson A I 1996 All-solid-state ultrafast lasers facilitate multiphoton excitation fluorescence imaging IEEE J. Sel. Top. Quantum Electron. 21051-65... 

The dynamics of fast processes such as electron and energy transfers and vibrational and electronic deexcitations can be probed by using short-pulsed lasers. The experimental developments that have made possible the direct probing of molecular dissociation steps and other ultrafast processes in real time (in the femtosecond time range) have, in a few cases, been extended to the study of surface phenomena. For instance, two-photon photoemission has been used to study the dynamics of electrons at interfaces [ ]. Vibrational relaxation times have also been measured for a number of modes such as the 0-Fl stretching m silica and the C-0 stretching in carbon monoxide adsorbed on transition metals [ ]. Pump-probe laser experiments such as these are difficult, but the field is still in its infancy, and much is expected in this direction m the near fiitiire. 

The development of ultrafast spectroscopy has paralleled progress in the teclmical aspects of pulse fomiation [Uj. Because mode-locked laser sources are tunable only with diflSculty, until recently the most heavily studied physical and chemical systems were those that had strong electronic absorption spectra in the neighbourhood of conveniently produced wavelengths. 

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 shortest optical pulses actually used so far (1998) in ultrafast spectroscopic experunents were obtained by Shank and co-workers from an amplified CPM laser [ ]. In these extraordinary experiments, a sequence of a pair of prisms... 

Time-resolved fluorescence is perhaps the most direct experunent in the ultrafast spectroscopist s palette. Because only one laser pulse interacts with the sample, the mediod is essentially free of the problems with field-matter time orderings that arise in all of the subsequently discussed multipulse methods. The signal... 

Katzenellenbogen N and Grischkowsky D 1991 Efficient generation of 380 fs pulses of THz radiation by ultrafast laser pulse excitation of a biased metal-semiconductor interface Appl. Phys. Lett. 58 222-4... 

Ippen E 1997 Characterizing optical components for ultrafast laser applications Optics 1997/98 Catalog (Irvine, CA Newport Corp.) pp 8-2-8-3... 

Zewail A H 2000 Femtochemistry atomic-scale dynamics of the chemical bond using ultrafast lasers (Nobel lecture) Angew. Chem. 39 2586-631... 

Ultrafast TRCD has also been measured in chemical systems by incoriDorating a PEM into the probe beam optics of a picosecond laser pump-probe absorjDtion apparatus [35]. The PEM resonant frequency is very low (1 kHz) in these experiments, compared with the characteristic frequencies of ultrafast processes and so does not interfere with the detection of ultrafast CD changes. 

Major breakthroughs in early ultrafast VER measurements were made in 1972 by Laubereau et al [22], who used picosecond lasers in an SRS pump-incoherent anti-Stokes Raman probe configuration, to study VER of C-H... 

The most powerful teclmique for studying VER in polyatomic molecules is the IR-Raman method. Initial IR-Raman studies of a few systems appeared more than 20 years ago [16], but recently the teclmique has taken on new life with newer ultrafast lasers such as Ti sapphire [39]. With more sensitive IR-Raman systems based on these lasers, it has become possible to monitor VER by probing virtually every vibration of a polyatomic molecule, as illustrated by recent studies of chlorofonn [40], acetonitrile [41, 42] (see example C3.5.6.6 below) and nitromethane [39, 43]. 

Schematic diagrams of modem experimental apparatus used for IR pump-probe by Payer and co-workers [50] and for IR-Raman experiments by Dlott and co-workers [39] are shown in figure C3.5.3. Ultrafast mid-IR pulse generation by optical parametric amplification (OPA) [71] will not discussed here. Single-colour IR pump-probe or vibrational echo experiments have been perfonned with OP As or free-electron lasers. Free-electron lasers use...

Fig. 4. Temporal pulse characteristics of lasers (a) millisecond laser pulse (b) relaxation oscillations (c) Q-switched pulse (d) mode-locked train of pulses, where Fis the distance between mirrors and i is the velocity of light for L = 37.5 cm, 2L j c = 2.5 ns (e) ultrafast (femtosecond or picosecond) pulse.

Another variation is the mode-locked dye laser, often referred to as an ultrafast laser. Such lasers offer pulses having durations as short as a few hundred femtoseconds (10 s). These have been used to study the dynamics of chemical reactions with very high temporal resolution (see Kinetic LffiASURELffiNTS). 

Several laser systems have been used in our time-resolved PM measurements. For the ultrafast measurements, a colliding pulse mode-locked (CPM) dye laser was employed [11]. Its characteristic pulsewidth is about 70 fs, however, its wavelength is fixed at 625 nin (or 2.0 cV). For ps measurements at various wavelengths two synchronously pumped dye lasers were used (12], Although their time resolution was not belter than 5 ps, they allowed us to probe in the probe photon energy range from 1.25 cV to 2.2 cV. In addition, a color center laser... 

The chapter is organized as follows in Section 8.2 a brief overview of ultrafast optical dynamics in polymers is given in Section 8.3 we present m-LPPP and give a summary of optical properties in Section 8.4 the laser source and the measuring techniques are described in Section 8.5 we discuss the fundamental photoexcitations of m-LPPP Section 8.6 is dedicated to radiative recombination under several excitation conditions and describes in some detail amplified spontaneous emission (ASE) Section 8.7 discusses the charge generation process and the photoexcitation dynamics in the presence of an external electric field conclusions are reported in the last section. 

---