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Journal of Modern Optics

Variations on adiabatic passage in optical control of molecular processes

Jiangbin Gong, Stuart A. Rice

Published Nov 1, 2004• 1 citation
Publisher

Abstract

A number of variations on adiabatic passage for the realization of efficient and selective population transfer in both the gas and liquid phases are presented. The advantageous use of decaying quantum states and/or the influence of continuous measurements during the population transfer are stressed and an intriguing adiabatic passage scheme, which is sensitive to the relative phases of the control laser fields, is introduced.

DOI
10.1080/09500340408231806

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A number of variations on adiabatic passage for the realization of efficient and selective population transfer in both the gas and liquid phases are presented. The advantageous use of decaying quantum states and/or the influence of continuous measurements during the population transfer are stressed and an intriguing adiabatic passage scheme, which is sensitive to the relative phases of the control laser fields, is introduced.
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 Al3O{\mathrm{Al}}_{3}\mathrm{O}Al3​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.
The feasibility of efficient population transfer between an initial state and a decaying target state of the same parity without populating an intermediate state, in the presence of large-amplitude stochastic energy level fluctuations that mimic the dephasing in a solute molecule due to the influence of a solvent, is demonstrated theoretically. In particular, it is shown that a decaying target state, whose decay rate constant is large compared with the band width of picosecond laser pulses but small compared with the associated peak Rabi frequencies, can dramatically suppress the dephasing-induced nonadiabaticity associated with the dynamics of population transfer, resulting in, irrespective of the correlation time of stochastic energy level fluctuations, negligible population in the intermediate state and complete population transfer to the decaying target state. These results should further motivate experimental studies of optical control of molecular dynamics in a liquid. An interesting connection between our results and the quantum Zeno and anti-Zeno effects is also discussed.
In the past two decades many schemes to actively control the dynamical evolution of a quantum system have been proposed and established. We focus attention on the use of assisted adiabatic processes to generate selected target states with high efficiency. Specific control protocols that fall in this category are sometimes called shortcuts to adiabaticity. We review two assisted adiabatic population transfer schemes, the counter-diabatic and fast-forward protocols, with the intent of calling attention to their conceptual basis and applications to real systems, specifically vibrational energy transfer in polyatomic molecules and manipulation of Bose-Einstein (BEC) condensates. The particular applications of the counter-diabatic and fast-forward protocols to improving the efficiency of population transfer between vibrational states of a polyatomic molecule that we have studied are (i) selective vibrational energy transfer in the nonrotating thiophosgene (SCCl2) molecule and (ii) enhancing the yield of HNC in the driven rotation free isomerization reaction HCN→CNH. A major component of our considerations concerns reduction of the degradation of population transfer efficiency within a subset of states that is generated by coupling of the subset of states to a manifold of background states. We have examined the influence of a manifold of background vibrational states on population transfer within a subset of embedded vibrational states, and on how that influence can be suppressed. We emphasize that any control protocol must be designed to minimize interference between the background states and excitations within the selected subset of states that are used to define initial and target states. We have also examined the application of the fast-forward protocol to the transport of population between sites of a BEC in an optical lattice. Through the applications we illustrate how the theoretical framework of an assisted adiabatic process depends on the character of the system studied, on the available control parameters, on the constraints imposed by the experimental setting, on the efficiency of population transfer (fidelity) to be achieved, and on the stability of the control process with respect to the variation of the external control fields.
Optical excitation of material transitions by adiabatic passage with frequency modulated (chirped) laser pulses is a useful spectroscopic tool.1,2 Here we demonstrate that picosecond frequency modulated laser pulses produce more efficient population transfer, and more selective excitation than equivalent (same spectral bandwidth) nearly transform limited laser pulses. We apply frequency modulated pulses to gas-phase and condensed phase systems. We also point out the "robustness", or insensitivity of the properties of the material excitation to the parameters of the laser field, that is inherent to the adiabatic process. The robustness obtainable by adiabatic passage will ultimately prove useful to laboratory applications of theoretical schemes which require frequency modulated ultrashort laser pulses to control chemical reaction dynamics.3
Highly efficient and selective population transfer in NO molecules in the electronic ground state (X2{\mathit{X}}^{2}X2${\mathrm{\ensuremath{\Pi}}}_{1/2}$) from the vibrational level v''=0 to the level v''=6 is demonstrated. It shows, for the first time with pulsed lasers, that a rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counterintuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage.