Coherent control pulses

This section begins with a brief description of the basic light-molecule interaction. As already indicated, coherent light pulses excite coherent superpositions of molecular eigenstates, known as wavepackets , and we will give a description of their motion, their coherence properties, and their interplay with the light. Then we will turn to linear and nonlinear spectroscopy, and, finally, to a brief account of coherent control of molecular motion. 

The pioneering use of wavepackets for describing absorption, photodissociation and resonance Raman spectra is due to Heller [12, 13,14,15 and 16]- The application to pulsed excitation, coherent control and nonlinear spectroscopy was initiated by Taimor and Rice ([17] and references therein). 

In Section II, the basic equations of OCT are developed using the methods of variational calculus. Methods for solving the resulting equations are discussed in Section III. Section IV is devoted to a discussion of the Electric Nuclear Bom-Oppenhermer (ENBO) approximation [41, 42]. This approximation provides a practical way of including polarization effects in coherent control calculations of molecular dynamics. In general, such effects are important as high electric fields often occur in the laser pulses used experimentally or predicted theoretically for such processes. The limits of validity of the ENBO approximation are also discussed in this section. 

Coherent Control with Femtosecond Laser Pulses, Eur. Phys. J. Sci. D, 14(2), (2001). 

Double pump experiments on an organic charge transfer complex TTF-CA by Iwai and coworkers demonstrated a new class of coherent control on a strongly correlated electron-lattice system [44]. While the amplitude of the coherent oscillation increased linearly with pump fluence for single pump experiments, the amplitude in the double pump experiments with a fixed pulse interval At = T exhibited a strongly super-linear fluence dependence (Fig. 3.16). The striking difference between the single- and double-pulse results indicated a cooperative nature of the photo-induced neutral-ionic transition. 

Dudovich, N., Oron, D., and Silberberg, Y. 2002. Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy. Nature 418 512-14. 

Lim, S. H., Gaster, A. G., and Leone, S. R. 2005. Single-pulse coherently controlled nonlinear Raman scattering spectroscopy. Phys. Rev. A 72 0418031. 

Figure 6.2 Steering of photochemical reactions by coherent control of ultrafast electron dynamics in molecules by shaped femtosecond laser pulses. Ultrafast excitation of electronic target states in molecules launches distinct nuclear dynamics, which eventually lead to specific outcomes of the photochemical reaction. The ability to switch efficiently between different electronic target channels, optimally achieved by turning only a single control knob on the control field, provides an enhanced flexibility in the triggering of photochemical events, such as fragmentation, excited state vibration, and isomerization.

In the following, we describe two prominent types of spectral phase modulation, each of which plays an important role in coherent control. Both types, namely sinusoidal (Section 6.2.1) and quadratic (Section 6.2.2) spectral phase modulation, are relevant for the experiments and simulations presented in this contribution. We provide analytic expressions for the modulated laser fields in the time domain and briefly discuss the main characteristics of both classes of pulse shapes. 

A negative chirped pulse is shown in Figure 6.4c. Experiments and 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. 

Looking ahead, coherent laser pulses covering the complete spectral range of valence bond excitation from the UV to the IR spectral region are becoming available (see, e.g., [119]), and we expect SPODS to increase in importance in coherently controlled photochemistry with applications ranging from reaction control within molecules up to discrimination between different molecules in a mixture and laser-based quantum information technologies. 

D. B. Strasfeld, S.-H. Shim, and M. T. Zanni. New Advances in Mid-IR Pulse Shaping and its Application to 2D IR Spectroscopy and Ground-State Coherent Control, pages 1-28. John Wiley Sons, Inc., Hoboken, NJ (2009). 

SLI is not specific to molecular eigenstates, but universal to the superposition of any eigenstates in a variety of quantum systems. It is thus expected as a new tool for quantum logic gates not only in MEIP but also for other systems such as atoms, ions, and quantum dots. SLI also provides a new method to manipulate WPs with fs laser pulses in general applications of coherent control. 

We demonstrate coherent control in strong fields beyond (i) population control and (ii) spectral interference, since (i) control is achieved without altering the population during the second intense laser pulse, i.e., the population during the second laser pulse is frozen, and (ii) the quantum mechanical phase is controlled without changing the spectrum of the pulse sequence. The control mechanism relies on the interplay of the quantum mechanical phase set by the intensity of the first pulse and the phase of the second pulse determined by the time delay. 

B. Coherence Control by Phase-Coherent Multiple Pulses... 

COHERENT CONTROL WITH FEMTOSECOND LASER PULSES... 

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