Unveiling the nonadiabatic rotational excitation process in a symmetric-top molecule induced by two intense laser pulses

Daeyul, Baek; Hasegawa, H.; Ohshima, Yasuhiro

doi:10.1063/1.3598962

Cited by 20 publications

(14 citation statements)

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“…Daems et al [565] showed that a combination of a half-cycle pulse and a short nonresonant laser pulse produces a strongly enhanced post-pulse orientation. Baek et al [566] studied the field-free dynamics of benzene aligned by two consecutive short laser pulses, while the interaction of rotationally excited molecules with short laser pulses was studied by Owschimikow et al [567][568][569]. Yun et al [570] analyzed the time evolution of the quantum phases of the rotational states contributing to the rotational wave packet which provided new insights into the post-pulse alignment dynamics.…”

Section: Interaction With Short Laser Pulses: Nonadiabatic Alignment ...mentioning

confidence: 99%

Manipulation of molecules with electromagnetic fields

et al. 2013

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I. INTRODUCTIONThe past few decades have witnessed remarkable developments of laser techniques setting the stage for new areas of research in molecular physics. It is now possible to interrogate molecules in the ultrafast and ultracold regimes of molecular dynamics and the measurements of molecular structure and dynamics can be made with unprecedented precision. Molecules are inherently complex quantum-mechanical systems. The complexity of molecular structure, if harnessed, can be exploited for yet another step forward in science, potentially leading to technology for quantum computing, quantum simulation, precise field sensors, and new lasers.The goal of the present article is to review the major developments that have led to the current understanding of molecule -field interactions and experimental methods for manipulating molecules with electromagnetic fields. Molecule -field interactions are at the core of several, seemingly distinct, areas of molecular physics. This is reflected in the organization of this article, which includes sections on Field control of molecular beams, External field traps for cold molecules, Control of molecular orientation and molecular alignment, Manipulation of molecules by nonconservative forces, Ultracold molecules and ultracold chemistry, Controlled many-body phenomena, Entanglement of molecules and dipole arrays, and Stability of molecular systems in high-frequency super-intense laser fields. By combining these topics in the same review, we would like to emphasize that all this work is based on the same basic Hamiltonian.This review is also intended to serve as an introduction to the excellent collection of articles appearing in this same-titled volume of Molecular Physics [1-27]. These original contributions demonstrate the latest developments exploiting control of molecules with electromagnetic fields. The reader will be treated to a colourful selection of articles on topics as diverse as Chemistry in laser fields, Quantum dynamics in helium droplets, Effects of microwave and laser fields on molecular motion, Rydberg molecules, Molecular structure in external fields, Quantum simulation with ultracold molecules, and Controlled molecular interactions, written by many of the leading protagonists of these fields.This article is concerned chiefly with the effects of electromagnetic fields on low-energy rotational, fine-structure and translational degrees of freedom. There are several important research areas that are left outside the scope of this paper, most notably the large body of work on the interaction of molecules with attosecond laser pulses and high harmonic generation [28], coherent control of molecular dynamics [29] and optimal control of molecular processes [30]. We limit the discussion of resonant interaction of light with molecules to laser cooling strategies. We do not survey spectroscopy or transfer of population between molecular states. Even with these restrictions, this is a vast area to review, as is apparent from the number of references. We did our best to in...

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Section: Interaction With Short Laser Pulses: Nonadiabatic Alignment ...mentioning

confidence: 99%

Manipulation of molecules with electromagnetic fields

et al. 2013

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“…Using phase-shaped femtosecond ionizing laser pulses Hertz et al reported excitation of only odd J states of the O molecule, and achieved alignment of 0.86 at 60 K 25 . Experimental investigation of the nonadiabatic rotational excitation for ground state symmetric-top molecules, by two intense nonresonant ultrafast laser fields, leads to excitation of states if while and if 26 . Hirokazu et al calculated the time evolution of the rotational-state distribution for NO molecules at varying pump intensities 27 .…”

Section: Introductionmentioning

confidence: 99%

Achieving high molecular alignment and orientation for CH$$_3$$F through manipulation of rotational states with varying optical and THz laser pulse parameters

Chordiya

Simkó

Szidarovszky

et al. 2022

Sci Rep

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Increasing interest in the fields of high-harmonics generation, laser-induced chemical reactions, and molecular imaging of gaseous targets demands high molecular “alignment” and “orientation” (A&O). In this work, we examine the critical role of different pulse parameters on the field-free A&O dynamics of the CH$$_3$$ 3 F molecule, and identify experimentally feasible optical and THz range laser parameters that ensure maximal A&O for such molecules. Herein, apart from rotational temperature, we investigate effects of varying pulse parameters such as, pulse duration, intensity, frequency, and carrier envelop phase (CEP). By analyzing the interplay between laser pulse parameters and the resulting rotational population distribution, the origin of specific A&O dynamics was addressed. We could identify two qualitatively different A&O behaviors and revealed their connection with the pulse parameters and the population of excited rotational states. We report here the highest alignment of $$\langle {\mathrm{cos}^2\theta }\rangle = 0.843$$ ⟨ cos 2 θ ⟩ = 0.843 and orientation of $$\langle {\mathrm{cos}(\theta )}\rangle = 0.886$$ ⟨ cos ( θ ) ⟩ = 0.886 for CH$$_3$$ 3 F molecule at 2 K using a single pulse. Our study should be useful to understand different aspects of laser-induced unidirectional rotation in heteronuclear molecules, and in understanding routes to tune/enhance A&O in laboratory conditions for advanced applications.

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“…Using phase-shaped femtosecond ionizing laser pulses Hertz et al reported excitation of only odd J states of the O 2 molecule, and achieved alignment of 0.86 at 60K 24 . Experimental investigation of the nonadiabatic rotational excitation for ground state symmetric-top molecules, by two intense nonresonant ultrafast laser fields, leads to excitation of ∆J = 2 states if K = 0 while ∆J = 1 and ∆J = 2 if K > 0 25 . Hirokazu et al calculated the time evolution of the rotational-state distribution for NO molecules at varying pump intensities 26 .…”

Section: Introductionmentioning

confidence: 99%

Manipulation of Rotational States With Varying Pulse Parameter: Achieving High Molecular Alignment and Orientation for CH3F

Chordiya

Simkó

Szidarovszky

et al. 2022

Preprint

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Increasing interest in the fields of high-harmonics generation, laser-induced chemical reactions, and molecular imaging of gaseous targets demands high molecular alignment and orientation (AnO). In this work, we examine the critical role of different pulse parameters on the field-free AnO dynamics of the CH3F molecule, and identify experimentally feasible optical and THz range laser parameters that ensure maximal AnO for such molecules. Herein, apart from rotational temperature, we investigate effects of varying pulse parameters such as, pulse duration, intensity, frequency, and carrier envelop phase (CEP). By analyzing the interplay between laser pulse parameters and the resulting rotational population distributions, the origin of specific AnO dynamics was addressed. We could identify two qualitatively different AnO behaviors and revealed their connection with the pulse parameters and the population of excited rotational states. We report here the highest alignment of ⟨cos2θ⟩=0.843 andorientation of⟨cos(θ)⟩=0.886 for CH3F molecule at 2K using single pulse. Our study should be useful to understand different aspects of laser-induced unidirectional rotation in heteronuclear molecules, and in understanding routes to tune/enhance AnO in laboratory conditions for advanced applications.

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Unveiling the nonadiabatic rotational excitation process in a symmetric-top molecule induced by two intense laser pulses

Cited by 20 publications

References 50 publications

Manipulation of molecules with electromagnetic fields

Manipulation of molecules with electromagnetic fields

Achieving high molecular alignment and orientation for CH$$_3$$F through manipulation of rotational states with varying optical and THz laser pulse parameters

Manipulation of Rotational States With Varying Pulse Parameter: Achieving High Molecular Alignment and Orientation for CH3F

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