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Field-free molecular orientation of nonadiabatically aligned OCS

Published on Feb 1, 2018in Chemical Physics Letters1.901
· DOI :10.1016/j.cplett.2018.01.009
Kotaro Sonoda2
Estimated H-index: 2
(UTokyo: University of Tokyo),
Atsushi Iwasaki11
Estimated H-index: 11
(UTokyo: University of Tokyo)
+ 1 AuthorsHiroshi Hasegawa18
Estimated H-index: 18
(UTokyo: University of Tokyo)
Abstract
Abstract We investigate an enhancement of the orientation of OCS molecules by irradiating them with a near IR (ω) ultrashort laser pulse for alignment followed by another ultrashort laser pulse for orientation, which is synthesized by a phase-locked coherent superposition of the near IR laser pulse and its second harmonic (2ω). On the basis of the asymmetry in the ejection direction of S3+ fragment ions generated by the Coulomb explosion of multiply charged OCS, we show that the extent of the orientation of OCS is significantly enhanced when the delay between the alignment pulse and the orientation pulse is a quarter or three quarters of the rotational period. The recorded enhanced orientation was interpreted well by a numerical simulation of the temporal evolution of a rotational wave packet prepared by the alignment and orientation pulses.
  • References (23)
  • Citations (2)
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References23
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#1Irina Znakovskaya (MPG: Max Planck Society)H-Index: 16
#2Michael Spanner (National Research Council)H-Index: 29
Last. Matthias F. Kling (MPG: Max Planck Society)H-Index: 36
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The transition between two distinct mechanisms for the laser-induced field-free orientation of CO molecules is observed via measurements of orientation revival times and subsequent comparison to theoretical calculations. In the first mechanism, which we find responsible for the orientation of CO up to peak intensities of 8 x 10^13 W/cm^2, the molecules are impulsively oriented through the hyperpolarizability interaction. At higher intensities, asymmetric depletion through orientation-selective i...
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#1Hideki OhmuraH-Index: 8
#2Naoaki SaitoH-Index: 11
Last. Toru MorishitaH-Index: 19
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#1Peter M. KrausH-Index: 14
#2Alisa RupenyanH-Index: 11
Last. Hans Jakob WörnerH-Index: 27
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Nonresonant optimal control simulation is applied to a CO molecule to design two-color phase-locked laser pulses (800 nm + 400 nm) with the aim of orienting the molecule under the field-free condition. The optimal pulse consists of two subpulses: the first subpulse aligns the molecule and the second one orients it. The molecular alignment induced by the first subpulse considerably enhances the degree of orientation, the value of which is close to an ideal value at temperature T = 0 K. To confirm...
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#1E. Frumker (MPG: Max Planck Society)H-Index: 14
Last. Paul B. CorkumH-Index: 69
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We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wavepacket is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution ...
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#1Michael SpannerH-Index: 29
Last. Paul B. CorkumH-Index: 69
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Two mechanisms of two-color (\omega + 2\omega) laser-induced field-free molecular orientation, based on the hyperpolarizability and ionization depletion, are explored and compared. The CO molecule is used as a computational example. While the hyperpolarizability mechanism generates small amounts of orientation at intensities below the ionization threshold, ionization depletion quickly becomes the dominant mechanism as soon as ionizing intensities are reached. Only the ionization mechanism leads ...
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#1Zhang Shi-AnH-Index: 4
#2Lu ChenhuiH-Index: 2
Last. Sun Zhen-Rong (ECNU: East China Normal University)H-Index: 5
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We propose a scheme to achieve the field-free molecular orientation around the half rotational periods with the combination of single- and dual-color laser pulses. We show that the molecular orientation can be obtained and controlled by precisely controlling the time delay between the two laser pulses. Furthermore, we discuss the effect of the laser intensity and pulse duration of the single-color laser pulse on the molecular orientation created by the dual-color laser pulse, and show that the m...
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#1Yasuhiro Ohshima (Graduate University for Advanced Studies)H-Index: 24
#2Hiroshi Hasegawa (Graduate University for Advanced Studies)H-Index: 18
The rotation of molecules in the gas phase can be coherently excited by irradiation with strong nonresonant short laser pulses, interacting with the molecular anisotropic polarisability. Such coherent rotational excitation has been attracting much attention because of the intriguing nature of the rotational wave packet thus created, and its wide applicability to dynamical studies and advanced optics. In this review article, we first survey various experimental schemes adopted so far for external...
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#1George Maroulis (University of Patras)H-Index: 37
#2Manolis Menadakis (University of Patras)H-Index: 1
Abstract We have used very large, purpose-oriented Gaussian-type basis sets to calculate static electric (hyper)polarizabilities for COS and NNO. For COS, we have obtained near-Hartree–Fock values with a [9s6p5d2f1g/9s6p5d2f1g/9s8p5d2f1g] basis set. Our best SCF values for the mean first and second hyperpolarizability of COS are β ¯ / e 3 a 0 3 E h - 2 = - 75.7 and γ ¯ / e 4 a 0 4 E h - 3 = 4966 . For NNO a [9s6p5d3f1g/9s6p5d3f1g/9s6p5d3f1g] basis yields SCF values β ¯ / e 3 a 0 3 E h - 2 = 38.0...
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#1Tamar Seideman (NU: Northwestern University)H-Index: 41
#2Edward Hamilton (NU: Northwestern University)H-Index: 12
We review the theory of intense laser alignment of molecules and present a survey of the many recent developments in this rapidly evolving field. Starting with a qualitative discussion that emphasizes the physical mechanism responsible for laser alignment, we proceed with a detailed exposition of the underlying theory, focusing on aspects that have not been presented in the past. Application of the theory in several pedagogical illustrations is then followed by a review of the recent experimenta...
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#1Qi-Yuan ChengH-Index: 1
#2Jingsong LiuH-Index: 1
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The molecular alignment induced by external fields is of significance in manipulating a chemical reaction. In this paper, the field-free alignment of a FCN molecule steered by a terahertz (THz) half-cycle laser pulse (HCP) is investigated by solving the density matrix equation. It is shown that a high degree of molecular alignment can be achieved by adjusting the carrier envelope phase (CEP) of the THz HCP. The appearance of a saturation threshold for the molecular alignment by a THz HCP when th...
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