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Physical Review A

Control of polarized iodine atom branching ratio in NaI photodissociation

Babak H. Hosseini, H. R. Sadeghpour, N. Balakrishnan

Published Feb 2, 2005• 19 citations
Publisher

Abstract

We report branching ratios between the ground and excited states of iodine atoms in the photodissociation of sodium iodide. We employ wave packet propagation techniques to study the optimal production of polarized iodine atoms and find experimentally realizable laser parameters to control the outcome. Application of a learning algorithm shows that the product branching can be controlled by suitably varying the time delay, the chirp, and the relative phase of the pump and control laser pulses. Periodic modulation of the polarized iodine atom branching ratio as a function of the delay between the firing of the two ultrashort laser pulses provides interesting insights into the photodissociation process.

DOI
10.1103/physreva.71.023402

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We report branching ratios between the ground and excited states of iodine atoms in the photodissociation of sodium iodide. We employ wave packet propagation techniques to study the optimal production of polarized iodine atoms and find experimentally realizable laser parameters to control the outcome. Application of a learning algorithm shows that the product branching can be controlled by suitably varying the time delay, the chirp, and the relative phase of the pump and control laser pulses. Periodic modulation of the polarized iodine atom branching ratio as a function of the delay between the firing of the two ultrashort laser pulses provides interesting insights into the photodissociation process.
Control over the product branching ratio in the photodissociation of Na2{\mathrm{a}}_{2}a2​ into Na(3s)+Na(3p)\mathrm{Na}(3s)+\mathrm{Na}(3p)Na(3s)+Na(3p) and Na(3s)+Na(3d)\mathrm{Na}(3s)+\mathrm{Na}(3d)Na(3s)+Na(3d) is demonstrated using a two-photon incoherent interference control scenario. Ordinary pulsed nanosecond lasers are used and Na2{\mathrm{a}}_{2}a2​ is at thermal equilibrium in a heat pipe. Results show a depletion in the Na(3d)\mathrm{Na}(3d)Na(3d) product of at least 25% and a concomitant increase in the Na(3p)\mathrm{Na}(3p)Na(3p) yield as the relative frequency of the two lasers is scanned.
A method for controlling branching unimolecular reactions, developed in collaboration with M. Shapiro of the Weizmann Institute, which uses the coherence of weak lasers, is presented. It is shown that preselected chemical products may be obtained, in preference to others, by utilizing the interference between naturally occurring processes. Our specific application then entails the dissociation of a bound superposition state with control attained by manipulating the relative intensities and phases of coherent laser beams. Enhanced yields of chemical products of interest are shown to result. Similar control is attainable for the populations of individual product quantum states. Computational results on the I*II branching ratios in the photodissociation of CH3, I and FI are presented as examples. Proposals for experiments which demonstrate coherent control present a challenge to the laser community which is well worth accepting.
This thesis presents original work contributing to the understanding of coherent control of wave packet dynamics in atomic and molecular systems excited by sequences of ultrafast laser pulses. An introduction to coherent control and a review of the literature is presented in chapter 1. Different approaches to coherent control are considered from the perspective of the phase complexity of the light fields used to achieve them, starting with a single transform-limited pulse, advancing through two-colour and multi-pulse schemes to chirped pulses, and finally arbitrarily shaped pulses. The purpose of this literature review is to position the work described in this thesis within the context of contemporary coherent control. In particular, our approach is seen to be in line with the current trend towards understanding the physics underlying coherent control processes. In chapter 2, development of a sodium atom and dimer beam source for use in optical coherent control experiments is described. The concepts of molecular beams are introduced along with a brief review of the literature on sodium atom and dimer beams. The beam source is considered in two parts. Firstly the sodium oven and nozzle are described in detail, along with the vacuum chamber that houses them. This is followed by a description of the experimental chamber, which contains a time-of-flight mass spectrometer. Finally a number of potential improvements to the system are discussed. Experiments to control the angular momentum composition of Rydberg electronic wave packets in atomic sodium are reported in chapter 3. The control scheme uses phase-locked pairs of transform-limited picosecond laser pulses to create pairs of identical radial wave packets in the Rydberg states. Quantum interference between the wave packets, or the excitation pathways to them, is manipulated to control the total angular composition of the resultant wave packet, which is detected either by the optical Ramsey method or by state-selective field ionisation. The results are interpreted both from the perspective of time evolution of the wave packet and the frequency content of the laser fields. The control strategy is then extended theoretically by the inclusion of linear chirp in one of the laser pulses. Chapter 4 describes progress towards a novel experiment for optical coherent control of vibrational wave packet dynamics in the sodium dimer. A coherent superposition of high-lying Rydberg states of the Na2 is excited by the broad bandwidth of a femtosecond laser pulse. The Rydberg states converge to several vibrational ionisation limits of the dimer, so the excitation effectively forms a vibrational wave packet in the X+ 22g+ ionic potential. Excitation of several wave packets by a series of phase-locked transform-limited pulses allows control over the composition and dynamics of the wave packet, and its detection using a combination of the optical Ramsey method and pulsed-field ionisation techniques adapted from ZEKE spectroscopy. A simple genetic algorithm is presented in chapter 5. It has been implemented to investigate the suitably of this type of optimisation procedure in simulations of Rydberg electronic wave packet coherent control in atomic sodium. The operation of the algorithm is described in detail. It is then tested against known solutions for two experimental scenarios: coherent control based on pairs of transform-limited laser pulses and transform-limited first pulse followed by a chirped second pulse. The behaviour of the algorithm is discussed in detail for each of these cases. Finally, the potential for application of the algorithm to unknown problems is briefly discussed.
Extensive control over relative product yields is shown to result from weak laser photodissociation in a two-color coherent control scenario. Photodissociation takes place from a superposition state prepared by stimulated emission pumping. The method allows for control in the presence of laser phase jumps by using four-wave mixing to prepare the required laser frequencies. The near UV photodissociation of Na2, resulting in the Na(3s) + Na(4s) and the Na(3s) + Na(3d) products, is used to illustrate the method.
We have extended our studies of control of the branching ratio for photoionization of atomic barium. This control is based on an interference between two distinct photoexcitation routes, each of which is a resonantly enhanced two-photon process. We report our experimental studies of the dependence of the interference on atomic beam density, laser power, selection of intermediate states, and relative polarization of the two field components. We observe that the potential for product control increases dramatically with increasing atomic beam density and depends strongly on the laser pulse energies as well.
Three-pulse four-wave mixing (FWM) is used here to study and control laser excitation processes. For general laser excitation processes, after a molecule interacts resonantly with a laser pulse, the molecule has a probability of being in the ground or in the excited state. Control over this process depends on the phase and amplitude of the electric fields that interact with the molecular system. Here we show how three-pulse FWM can be used to control the excitation of iodine molecules. Depending on the time delay between the first two pulses, the observed signal reflects the dynamics of the ground or excited state. A theoretical formalism based on the density matrix formulation is presented and solved for a four-level system. Experiments are found to be in excellent agreement with the theory. The influence of linear chirp on three-pulse FWM experiments is explored. Spectrally dispersed three-pulse FWM is found to be extremely useful for studying the effect of chirp on laser excitation of molecular systems. Experimental demonstrations of these effects are included.