Shaped pulse capability

Quality two-dimensional spectra demand high accuracy from the pulse programmer. Accurately timed, well-shaped pulses with minimal phase errors must be generated for both the observe transmitter and for the spin decoupler. The programming and hardware control capabilities of the pulse... 

To answer the question as to whether the fluorescence decay consists of a few distinct exponentials or should be interpreted in terms of a continuous distribution, it is advantageous to use an approach without a priori assumption of the shape of the distribution. In particular, the maximum entropy method (MEM) is capable of handling both continuous and discrete lifetime distributions in a single analysis of data obtained from pulse fluorometry or phase-modulation fluorometry (Brochon, 1994) (see Box 6.1). 

The added benefit of intrinsic interferometric detection is only a further example of the great flexibility of using the pulse shaper in single-beam nonlinear microspectroscopy. The setup used here for CARS in its variants is, of course, also capable of immediately performing all the other nonlinear microspectroscopies simply by changing the shape of the excitation pulses with computer control. This is shown in the next section, where we discuss a broadband TPF application. 

Experiments were performed using a titanium sapphire laser oscillator capable of producing pulses with bandwidths up to 80 nm FWHM. The output of the oscillator was evaluated to make sure there were no changes in the spectrum across the beam and was compressed with a double prism pair arrangement. The pulse shaper uses prisms as the dispersive elements, two cylindrical concave mirrors, and a spatial light modulator (CRI Inc. SLM-256), composed of two 128-pixel liquid crystal masks in series. The SLM was placed at the Fourier plane [5]. After compression and pulse shaping, 200 pJ pulses were used to interrogate the samples. 

Since the fast centrifuge system SISAK is equipped with liquid scintillation counting LSC [12,58], it is in principle capable of investigating short-lived a-decaying nuclides of the transactinides, p/y pulses and a pulses are distinguished by pulse-shape discrimination PSD and pile-up pulses are rejected by a pile-up rejection system PUR. This analog electronics proved to result in insufficient background suppression. Thus, two new approaches... 

Many workers have in fact used density matrix methods for the calculation of line shapes and intensities in multiple resonance experiments, and two excellent reviews of the background theory are available. (49, 50) In addition there is also a simple guide (51) to the actual use of the method which is capable of predicting the results of quite elaborate experiments. Major applications have included the calculation of the complete double resonance spectrum from an AX spin system which gives 12 transitions in all (52) an extremely detailed study of the relaxation behaviour of the AX2 systems provided by 1,1,2-trichloroethane and 2,2-dichloroethanol (53) the effects of gating and of selective and non-selective pulses on AB and AX spin systems and the importance of the time evolution of the off-diagonal elements of the density matrix in repetitively pulsed FT NMR and spin-echo work (54) the use of double resonance to sort out relaxation mechanisms and transient responses (55) the calculation of general multiple resonance spectra (56) and triple resonance studies of relaxation in AB and AX spin systems. (57)... 

Other prominent examples are theoretical proposals for different optical control schemes using laser field parameters for the manipulation of ultrafast process pioneered by Rice and Tannor, Shapiro and Brumer, and Peirce, Dahleh, and Rabitz [2, 56-61]. They stimulated control experiments that were carried out first on simple systems such as metallic dimers and trimers [62-84], and later on more complex systems [23-25, 43, 85-89], confirming theoretically proposed concepts. Since tailored laser pulses have the ability to select pathways that optimally lead to the chosen target, their analysis should allow one to determine the mechanism of the processes and to provide the information about the selected pathways (inversion problem). Therefore, theoretical approaches are needed, which are capable of designing interpretable optimal laser pulses for complex systems (e.g., clusters or biomolecules) by establishing the connection between the underlying dynamical processes and their shapes. In this case, the optimal control can be used as a tool for the analysis. 

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