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Science

Comment on "Coherent Control of Retinal Isomerization in Bacteriorhodopsin"

M. Joffre

Published Jul 26, 2007• 25 citations
Publisher

Abstract

Prokhorenko et al. (Research Articles, 1 September 2006, p. 1257) reported that, in the weak-field regime, the efficiency of retinal isomerization in bacteriorhodopsin can be controlled by modulating the spectral phase of the photoexcitation pulse. However, in the linear excitation regime, the signal measured in an experiment involving a time-invariant, stationary process can be shown to be independent of the pulse spectral phase.

DOI
10.1126/science.1137011

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arXiv:0711.1425•Physical Review A•Oct 30, 2007•24 citations
Prokhorenko et al. (Research Articles, 1 September 2006, p. 1257) reported that, in the weak-field regime, the efficiency of retinal isomerization in bacteriorhodopsin can be controlled by modulating the spectral phase of the photoexcitation pulse. However, in the linear excitation regime, the signal measured in an experiment involving a time-invariant, stationary process can be shown to be independent of the pulse spectral phase.
Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.
We numerically study the implementation of a NOT gate by laser pulses in a model molecular system presenting two electronic surfaces coupled by nonadiabatic interactions. The two states of the bit are the fundamental states of the cis-trans isomers of the molecule. The gate is classical in the sense that it involves a one-qubit flip so that the encoding of the outputs is based on population analysis which does not take the phases into account. This gate can also be viewed as a double photoswitch process with the property that the same electric field controls the two isomerizations. As an example, we consider one-dimensional cuts in a model of the retinal in rhodopsin already proposed in the literature. The laser pulses are computed by the multitarget optimal control theory with chirped pulses as trial fields. Very high fidelities are obtained. We also examine the stability of the control when the system is coupled to a bath of oscillators modeled by an ohmic spectral density. The bath correlation time scale being smaller than the pulse duration, the dynamics is carried out in the Markovian approximation