Department of Chemistry, Princeton University, Princeton, NJ 08544, USA.
Phys Chem Chem Phys. 2011 Apr 28;13(16):7348-62. doi: 10.1039/c0cp02234a. Epub 2011 Mar 22.
A traditional quantum optimal control experiment begins with a specific physical system and seeks an optimal time-dependent field to steer the evolution towards a target observable value. In a more general framework, the Hamiltonian structure may also be manipulated when the material or molecular 'stockroom' is accessible as a part of the controls. The current work takes a step in this direction by considering the converse of the normal perspective to now start with a specific fixed field and employ the system's time-independent Hamiltonian structure as the control to identify an optimal form. The Hamiltonian structure control variables are taken as the system energies and transition dipole matrix elements. An analysis is presented of the Hamiltonian structure control landscape, defined by the observable as a function of the Hamiltonian structure. A proof of system controllability is provided, showing the existence of a Hamiltonian structure that yields an arbitrary unitary transformation when working with virtually any field. The landscape analysis shows that there are no suboptimal traps (i.e., local extrema) for controllable quantum systems when unconstrained structural controls are utilized to optimize a state-to-state transition probability. This analysis is corroborated by numerical simulations on model multilevel systems. The search effort to reach the top of the Hamiltonian structure landscape is found to be nearly invariant to system dimension. A control mechanism analysis is performed, showing a wide variety of behavior for different systems at the top of the Hamiltonian structure landscape. It is also shown that reducing the number of available Hamiltonian structure controls, thus constraining the system, does not always prevent reaching the landscape top. The results from this work lay a foundation for considering the laboratory implementation of optimal Hamiltonian structure manipulation for seeking the best control performance, especially with limited electromagnetic resources.
传统的量子最优控制实验从特定的物理系统开始,并寻求最优的时变场来引导演化达到目标可观测量值。在更一般的框架中,当物质或分子“仓库”作为控制的一部分可访问时,也可以操纵哈密顿结构。当前的工作朝着这个方向迈出了一步,考虑到正常视角的反转,现在从特定的固定场开始,并采用系统的时不变哈密顿结构作为控制来确定最佳形式。哈密顿结构控制变量被视为系统能量和跃迁偶极矩矩阵元。分析了由可观测量作为哈密顿结构函数定义的哈密顿结构控制景观。提供了系统可控性的证明,表明当使用几乎任何场时,存在一个哈密顿结构可以产生任意幺正变换。景观分析表明,当使用无约束结构控制来优化态到态跃迁概率时,对于可控量子系统不存在次优陷阱(即局部极值)。对模型多能级系统的数值模拟验证了这一分析。发现到达哈密顿结构景观顶部的搜索努力几乎与系统维度无关。进行了控制机制分析,表明在哈密顿结构景观顶部,不同系统具有广泛的行为。还表明,减少可用的哈密顿结构控制数量,从而限制系统,并不总是可以防止达到景观顶部。这项工作的结果为考虑在实验室中实施最优哈密顿结构操纵以寻求最佳控制性能奠定了基础,特别是在电磁资源有限的情况下。