Chirped pulse

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. 

Pessot M, Squier J, Mourou G and Harter D 1989 Chirped-pulse amplification of 100 fsec pulses Opt. Lett. 14 797-9... 

Le Blanc C, Grillon G, Chambaret J P, Migus A and Antonetti A 1993 Compact and efficient multipass Ti sapphire system for femtosecond chirped-pulse amplification at the terawatt level Opt. Lett. 18 140-... 

Bardeen C J, Wang Q and Shank C V 1998 Femtosecond chirped pulse excitation of vibrational wave packets in bacteriorhodopsin J. Phys. Chem. A 102 2759-66... 

The layout of the experimental set-up is shown in Figure 8-3. The laser source was a Ti sapphire laser system with chirped pulse amplification, which provided 140 fs pulses at 780 nm and 700 pJ energy at a repetition rate of 1 kHz. The excitation pulses at 390 nm were generated by the second harmonic of the fundamental beam in a 1-nun-thick LiB305 crystal. The pump beam was focused to a spot size of 80 pm and the excitation energy density was between 0.3 and 12 ntJ/crn2 per pulse. Pump-... 

Figure 34. Contour map of the nonadiabatic transition probability Pn induced by quadratically chirped pulse as a function of the two basic parameters a and p. Taken from Ref. [37]-...

Figure 36. Time variation of the wave packet population on the ground X and excited B states of LiH. The system is excited by a single quadratically chirped pulse with parameters 0(a, = 5.84 X 10 eV fs , = 2.319 eV, and / = 1.00 TWcm . The pulse is centered at t = 0...

The second example is the quadratically chirped pump-dump scheme. Since the pioneering work by Tannor and Rice [119], the pump-dump method has been widely used to control various processes. However, since it is not possible to transfer a wave packet from one potential energy surface to another nearly completely by using the ordinary transform limited or linear chirped pulses, the... 

Figure 37. Electronic excitation of the NaK wavepacket from the inner turning point of the ground X state. The X A transition is considered. The initial wave packet is prepared by two quadratically chirped pulses within the pump-dump mechanism. Taken from Ref. [37].

Figure 39. Pump-dump control of NaK molecule by using two quadratically chirped pulses. The initial state taken as the ground vibrational eigenstate of the ground state X is excited by a quadratically chirped pulse to the excited state A. This excited wavepacket is dumped at the outer turning point at t 230 fs by the second quadratically chirped pulse. The laser parameters used are = 2.75(1.972) X 10-2 eVfs- 1.441(1.031) eV, and / = 0.15(0.10)TWcm-2 for the first (second) pulse. The two pulses are centered at t = 14.5 fs and t2 = 235.8 fs, respectively. Both of them have a temporal width i = 20 fs. (See color insert.) Taken from Ref. [37].

Figure 40. Pump-dump control of NaK by using two quadraticaUy chirped pulses. The initial state and the first step of pump are the same as in Fig. 39. The excited wave packet is now dumped at R 6.5cio on the way to the outer turning point. The parameters of the second pulse are a ) = 1.929 X 10 eVfs , = 1.224eV, and I = 0.lOTWcm . The second pulse is centered at...

Figure 41. Selective bond breaking of H2O by means of the quadratically chirped pulses with the initial wave packets described in the text. The dynamics of the wavepacket moving on the excited potential energy surface is illustrated by the density, (a) The initail wave packet is the ground vibrational eigen state at the equilibrium position, (b) The initial wave packet has the same shape as that of (a), but shifted to the right, (c) The initail wave packet is at the equilibrium position but with a directed momentum toward x direction. Taken from Ref. [37]. (See color insert.)...

Figure 58. Changes of the wavepacket populations on the respective states (upper panels) under the 3.5TWcm quadratically chirped pulses (lower panels) during the sequential pump-dump scheme via the (a) I A —> I B pumping at CHD and [(b) and (c)] 2 A I B —> I A pump...

Fig. 3.14. Left transient reflectivity change of Te obtained with transform limited, negatively chirped, and positively chirped pulses. Right coherent phonon amplitude as a function of the pulse chirp. Adapted from [42]...

K.A. Tillman, D.T. Reid, D. Artigas, J. Hellstrom, V. Pasiskevicius, and F. Laurell, Low-threshold, high-repetition-frequency femtosecond optical parametric oscillator based on chirped-pulse frequency conversion, Journal of the Optical Society of America B 20 1309 (2003). 

B. Torosov, S. Guerin, and N. V. Vitanov. High-fidehty adiabatic passage by composite sequences of chirped pulses. Phys. Rev. Lett., 106 233001 (2011). 

A negative theoretical studies on coherent control of ultrafast electron dynamics by intense chirped laser pulses will be discussed in Sections 6.3.2.3 and 633.2. 

In the following, we will discuss two basic - and in a sense complementary [44] - physical mechanisms to exert efficient control on the strong-field-induced coherent electron dynamics. In the first scenario, SPODS is implemented by a sequence of ultrashort laser pulses (discrete temporal phase jumps), whereas the second scenario utilizes a single chirped pulse (continuous phase variations) to exert control on the dressed state populations. Both mechanisms have distinct properties with respect to multistate excitations such as those discussed in Section 6.3.3. 

Next we employ chirped pulses and investigate the aspects of adiabatic time evolution in the strong-field excitation of the five-state system of Figure 6.9. Similar scenarios to invert multistate systems using chirped pulses have been reported by... 

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