Control of molecular orientation with combined near-single-cycle THz and optimally designed non-resonant laser pulses: Carrier-envelope phase effects

Yoshida, Masahiro; Ohtsuki, Yukiyoshi

doi:10.1016/j.cplett.2015.05.041

Cited by 12 publications

(4 citation statements)

References 43 publications

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“…The control time was optimized in [188]. Different extensions of the standard algorithms were proposed to account for some specific experimental constraints such as the requirement of a zero-area field [189,190], spectral constraints [191], fields with specific shape constraints [183,192,193,194], and different polarizations [54,195]. Polarizability and hyperpolarizability terms lead to a non-linear interaction between the molecular system and the control field.…”

Section: Optimal Control For Alignment and Orientationmentioning

confidence: 99%

Quantum control of molecular rotation

2019

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The angular momentum of molecules, or, equivalently, their rotation in three-dimensional space, is ideally suited for quantum control. Molecular angular momentum is naturally quantized, time evolution is governed by a well-known Hamiltonian with only a few accurately known parameters, and transitions between rotational levels can be driven by external fields from various parts of the electromagnetic spectrum. Control over the rotational motion can be exerted in one-, two-and many-body scenarios, thereby allowing to probe Anderson localization, target stereoselectivity of bimolecular reactions, or encode quantum information, to name just a few examples. The corresponding approaches to quantum control are pursued within separate, and typically disjoint, subfields of physics, including ultrafast science, cold collisions, ultracold gases, quantum information science, and condensed matter physics. It is the purpose of this review to present the various control phenomena, which all rely on the same underlying physics, within a unified framework. To this end, we recall the Hamiltonian for free rotations, assuming the rigid rotor approximation to be valid, and summarize the different ways for a rotor to interact with external electromagnetic fields. These interactions can be exploited for control -from achieving alignment, orientation, or laser cooling in a one-body framework, steering bimolecular collisions, or realizing a quantum computer or quantum simulator in the many-body setting. IntroductionMolecules, unlike atoms, are extended objects that possess a number of different types of internal motion. In particular, the geometric arrangement of their constituent atoms endows molecules with the basic capability to rotate in three-dimensional space. Rotations can couple to vibrations of the atomic nuclei as well as to the orbital and spin angular momentum of the electrons. The resulting complexity of the energy level structure [1,2,3,4] may be daunting. It offers, on the other hand, a variety of knobs for control and thus is at the core of numerous applications, from the classic example of the ammonia maser [5] all the way to recent measurements of the electron's electric dipole moment in a cryogenic molecular beam of thorium monoxide [6].A key advantage of internal degrees of freedom such as rotation is that they occupy the low-energy part of the energy spectrum. Quantization of the rotational motion has been an early hallmark of quantum mechanics due to its connection to selection rules that govern all light-matter interactions [7]. Nowadays, rotational states and rotational molecular dynamics feature prominently in all active areas of AMO physics research as well as in neighbouring fields such as physical chemistry and quantum information science. Control over the rotational motion is crucial in one-body, two-body and many-body scenarios. For example, rotational state-selective excitation could pave the way towards separating left-and right handed enantiomers of chiral molecules [8,9]. Still within the one-body scenar...

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Section: Optimal Control For Alignment and Orientationmentioning

confidence: 99%

Quantum control of molecular rotation

2019

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“…A straightforward and effective way is to optimize laser fields using quantum optimal control theory. 73,[78][79][80][81][82][83][84][85][86] Due to the complexity of optimal pulses, it is often tricky to experimentally generate the optimal laser pulses and to obtain an understanding of the underlying physics. Theoretically, defining the target state that can generate the maximum orientation of hcos yi = 1 is challenging because the operator cos y has a continuous spectrum.…”

Section: Niels E Henriksenmentioning

confidence: 99%

Quantum control of field-free molecular orientation

Hong,

Lian,

Shu

et al. 2023

Phys. Chem. Chem. Phys.

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“…Recent advances in both the theoretical tools for designing spatiotemporal profiles of such tailored laser pulses based on optimal control theory and ultrashort pulsed laser technology have enabled sophisticated manipulation of finite quantum systems. This has been demonstrated in photochemical reactions, with high efficiency [7][8][9][10][11][12][13][14][15], molecular alignment, or orientation in a gas phase [16][17][18][19][20][21][22][23][24], high-order harmonic generation [25], qubit operation by light-driven unitary transformations in quantum computation [26][27][28][29][30][31] and so on.…”

Section: Introductionmentioning

confidence: 99%

A simple formula to predict the influence of the near-field in the optical control of confined electron systems

Takeuchi

Ohnuki

Sako

2017

J. Phys. B: At. Mol. Opt. Phys.

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A simple formula for predicting the ratio between the field strengths of the incident laser pulse and of the near-field created in the vicinity of the target electron system has been proposed, in the context of optically controlling confined electron systems. The formula is easy to use and does not involve elaborate computation, thus enabling one to judge whether to use the timeconsuming Maxwell-Schrödinger hybrid simulation or to stay with the conventional timedependent Schrödinger equation approach that takes no near-field effect into account. As a demonstration we have examined in detail the system of an electron confined in a quasi-onedimensional nanoscale potential well. The highly accurate Maxwell-Schrödinger hybrid simulation has been employed to demonstrate the usefulness of the proposed formula in predicting the significance of the near-field effect. The near-field effect has shown to depend sensitively on the characteristics of the laser pulse and of the geometry of the confined electron system, which can be predicted well by the proposed formula.

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Control of molecular orientation with combined near-single-cycle THz and optimally designed non-resonant laser pulses: Carrier-envelope phase effects

Cited by 12 publications

References 43 publications

Quantum control of molecular rotation

Quantum control of molecular rotation

Quantum control of field-free molecular orientation

A simple formula to predict the influence of the near-field in the optical control of confined electron systems

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