Abstract

The merging of coherent control (CC) and adiabatic passage (AP) and the type of problems that can be solved using the resulting coherently controlled adiabatic passage (CCAP) method are discussed. The discussion starts with the essence of CC as the guiding of a quantum system to arrive at a given final state via a number of different quantum pathways. The guiding is done by ``tailor-made'' external laser fields. Selectivity in a host of physical and chemical processes is shown to be achieved by controlling the interference between such quantum pathways. The AP process is then discussed, in which a system is navigated adiabatically along a single quantum pathway, resulting in a complete population transfer between two energy eigenstates. The merging of the two techniques (CCAP) is shown to achieve both selectivity and completeness. Application of CCAP to the solution of the nondegenerate quantum control problem is first discussed and shown that it is possible to completely transfer population from an initial wave packet of arbitrary shape, composed of a set of nondegenerate energy eigenstates, to a final arbitrary wave packet, also composed of nondegenerate states. The treatment is then extended to systems with degenerate states and shown how to induce isomerization between the broken-symmetry local minima of a Jahn-Teller ${\mathrm{Al}}_{3}\mathrm{O}$ molecule. These approaches can be further generalized to situations with many initial, intermediate, and final states and applied to quantum coding and decoding problems. CCAP is then applied to cyclic population transfer (CPT), induced by coupling three states of a chiral molecule in a cyclic fashion, $\ensuremath{\mid}1⟩\ensuremath{\leftrightarrow}\ensuremath{\mid}2⟩\ensuremath{\leftrightarrow}\ensuremath{\mid}3⟩\ensuremath{\leftrightarrow}\ensuremath{\mid}1⟩$. Interference between two adiabatic pathways in CPT allows for a complete population transfer, coupled with multichannel selectivity, by virtue of its phase sensitivity. CPT can be used to show the purification of mixtures of right-handed and left-handed chiral molecules. Finally, quantum-field coherent control is introduced, where CCAP is extended to the use of nonclassical light. This emerging field may be used to generate new types of entangled radiation-matter states.

Highlights

  • Moshe Shapiro‡ Departments of Chemistry and Physics, The University of British Columbia, Vancouver, British Columbia, Canada V6T 1Z1 and Department of Chemical Physics, The Weizmann Institute of Science, Rehovot 76100, IsraelPublished 2 January 2007͒

  • The discussion starts with the essence of CC as the guiding of a quantum system to arrive at a given final state via a number of different quantum pathways

  • As particular applications of CCAP we have shown how to prepare arbitrary wave packets made of nondegenerate or degenerate energy states

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Summary

Coherent control

Coherent controlBrumer and Shapiro, 1986; Shapiro and Brumer, 2003͒ is a method of selecting between differentenergetically allowedoutcomes using multiply interfering quantum pathways. Most experiments of those days attempted to achieve selectivity by using frequency control as afforded by narrow-band lasers Since such lasers lead to preferential excitation of atomic and molecular levels that are in resonance with the laser linesKurzel and Steinfeld, 1970; Bergmann and Demtröder, 1971͒, the hope was that such energy selectivity will result in selectivity of subsequent events such as ionization and dissociation. The injection rates into the ± kcmomentum states of conduction electrons leaving the excitation spot depend on the ␾1 − 2␾2 relative phase, which results in symmetry breaking of the population distributionsee Král and Sipe2000͔͒. This asymmetry leads to the generation of dduc cetlieocntrivcacleunrrceentbjacnκdokfcPtkhcedksec mi0conjvducjctori.nIntheFicgo. Its direction can be clearly controlled by the relative phase ␾1 − 2␾2

Adiabatic passage
NONDEGENERATE QUANTUM CONTROL PROBLEM
QUANTUM CONTROL PROBLEM IN THE PRESENCE OF DEGENERATE STATES
COHERENTLY CONTROLLED QUANTUM ADIABATIC ENCODING AND DECODING
PURIFICATION OF MIXTURES OF RIGHT-HANDED AND LEFT-HANDED CHIRAL MOLECULES
SUMMARY
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