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Chemical Physics

Coherence transfer processes in vibrational relaxation of polyatomic molecules in condensed media

Karl F. Freed, A. A. Villaeys

Published May 1, 1979• 11 citations
Publisher
DOI
10.1016/0301-0104(79)85076-4

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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.

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Coherent control of molecules for quantum computation

Daniel Weidinger

Molecules under the inuence of light can be used to perform quantum computational operations when their vibrational or rotational quantum states are coherently controlled. An analysis is presented of quantum computation within the vibrational degrees of freedom of a polyatomic molecule. A set of 2n vibrational states covering a range of energies is used to encode n qubits in place of n separate degrees of freedom. Computer simulations are used to demonstrate the capacity of a shaped laser pulse to execute 4-qubit quantum computational algorithms with high delity on gas phase thiophosgene. An alternative light-molecule system using terahertz pulses on gas phase D3O+ is also analyzed and found to have the capability of performing 2-qubit operations. Simulations of closed loop experiments in coherent control are presented, and elements of the experimental procedure are tested to demonstrate how intramolecular vibrational relaxation (IVR) may be slowed in the ground state vibrational energy levels of gas phase thiophosgene.

•Jan 1, 2008•0 citations
We show that the theory of nuclear magnetic relaxation applies with equal validity to intramolecular relaxation in the quasicontinuum of polyatomic molecules. This theory permits an analysis of the laser-pulse requirements for vibrational-mode selectivity and coherent multiphoton excitation. The laser Rabi precession frequency, microepsilon/h, should exceed 1/T(1) or 1/T(2), the intramolecular relaxation rates in the quasicontinuum. In practice this requires either an ultra-fast optical-pulse risetime or a slower pulse that is tuned far to the red side of the transition.
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.
Molecules under the inuence of light can be used to perform quantum computational operations when their vibrational or rotational quantum states are coherently controlled. An analysis is presented of quantum computation within the vibrational degrees of freedom of a polyatomic molecule. A set of 2n vibrational states covering a range of energies is used to encode n qubits in place of n separate degrees of freedom. Computer simulations are used to demonstrate the capacity of a shaped laser pulse to execute 4-qubit quantum computational algorithms with high delity on gas phase thiophosgene. An alternative light-molecule system using terahertz pulses on gas phase D3O+ is also analyzed and found to have the capability of performing 2-qubit operations. Simulations of closed loop experiments in coherent control are presented, and elements of the experimental procedure are tested to demonstrate how intramolecular vibrational relaxation (IVR) may be slowed in the ground state vibrational energy levels of gas phase thiophosgene.