All-optical field-free three-dimensional orientation of asymmetric-top molecules

Lin, Kang; Tutunnikov, Ilia; Qiang, Junjie; Ma, Jing; Song, Qiying; Ji, Qinying; Zhang, Wenbing; Li, Hanxiao; Sun, Fenghao; Gong, Xiaochun; Li, Hui; Lu, Peifen; Zeng, Heping; Prior, Yehiam; Averbukh, Ilya Sh.; Wu, Jian

doi:10.1038/s41467-018-07567-2

Cited by 74 publications

(48 citation statements)

References 57 publications

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“…Laser-induced molecular orientation is a more challenging task; however, several techniques have been suggested and demonstrated for impulsive orientation of linear and even asymmetric top molecules under field-free condition (see, e.g. (7 ), and references therein).…”

mentioning

confidence: 99%

Observation of persistent orientation of chiral molecules by a laser field with twisted polarization

Tutunnikov¹,

Floß²,

Gershnabel³

et al. 2020

Phys. Rev. A

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Molecular chirality is an omnipresent phenomenon of fundamental significance in physics, chemistry and biology. For this reason, search for novel techniques for enantioselective control, detection and separation of chiral molecules is of particular importance. It has been recently predicted that laser fields with twisted polarization may induce persistent enantioselective field-free orientation of chiral molecules. Here we report the first experimental observation of this phenomenon using propylene oxide molecules (CH 3 CHCH 2 O, or PPO) spun by an optical centrifuge -a laser pulse, whose linear polarization undergoes an accelerated rotation around its propagation direction. We show that PPO molecules remain oriented on a time scale exceeding the duration of the centrifuge pulse by several orders of magnitude. The demonstrated long-time field-free enantioselective orientation opens new avenues for optical manipulation, discrimination, and, potentially, separation of molecular enantiomers.

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mentioning

confidence: 99%

Observation of persistent orientation of chiral molecules by a laser field with twisted polarization

Tutunnikov¹,

Floß²,

Gershnabel³

et al. 2020

Phys. Rev. A

Self Cite

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“…A fundamentally new aspect of field free orientation initiated by fields with twisted polarization was discovered 66,122,145 -the orientation does not return to zero shortly after the end of the excitation but persists over time exceeding the time scale of the excitation pulses by several orders of magnitude. In all the previously known approaches to impulsive orientation of nonchiral molecules, including techniques using single-cycle THz pulses, 39,45,[111][112][113][114]119 alone or in combination with optical pulses, [116][117][118] or two-color laser fields, [44][45][46][47][48][49][50][51]146 the orientation is short-lived and disappears rapidly after the end of the excitation pulses. Transient revival spikes may appear at longer times, however, they ride on a zero baseline and their time average is exactly zero.…”

Section: Persistent Orientationmentioning

confidence: 99%

“…Here we review the first experimental demonstration of alloptical field-free orientation of asymmetric-top SO 2 molecules using phase-locked orthogonal two-color (OTC) laser fields, 146 consisting of FW and its temporally overlapped SH. The FW aligns the MPA of the molecule along the polarization direction, whereas the two fields together orient the molecules via the offdiagonal components of the molecular hyperpolarizability tensor.…”

Section: Three-dimensional Orientation Of Asymmetric-top Moleculesmentioning

confidence: 99%

Spatiotemporal rotational dynamics of laser-driven molecules

Lin

Tutunnikov

et al. 2020

Adv. Photon.

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Molecular alignment and orientation by laser fields has attracted significant attention in recent years, mostly due to new capabilities to manipulate the molecular spatial arrangement. Molecules can now be efficiently prepared for ionization, structural imaging, orbital tomography, and more, enabling, for example, shooting of dynamic molecular movies. Furthermore, molecular alignment and orientation processes give rise to fundamental quantum and classical phenomena like quantum revivals, Anderson localization, and rotational echoes, just to mention a few. We review recent progress on the visualization, coherent control, and applications of the rich dynamics of molecular rotational wave packets driven by laser pulses of various intensities, durations, and polarizations. In particular, we focus on the molecular unidirectional rotation and its visualization, the orientation of chiral molecules, and the three-dimensional orientation of asymmetric-top molecules. Rotational echoes are discussed as an example of nontrivial dynamics and detection of prepared molecular states.

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“…In the present work, we demonstrate the application of machine learning in HHS to probe molecular rotational dynamics with high resolution and fidelity. Molecular rotational control by coherently manipulating the rota- tional wave packet (RWP) has been proved an efficient way to connect the molecular and laboratory frames [40][41][42][43][44], which is significant for molecular structure imaging [25][26][27] and chemical reaction steering [22,45]. In experiment, the molecular frame dynamics is usually convolved with the rotational distribution of molecules in laboratory.…”

Section: Introductionmentioning

confidence: 99%

Direct imaging of molecular rotation with high-order-harmonic generation

Lan

et al. 2019

Phys. Rev. A

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Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet is fully reconstructed from the angular distributions of HHG measured at various time delays of the probe pulse. The experimental retrievals are in good agreement with the numerical simulations. These findings provide a comprehensive picture of molecular rotation in space and time which will facilitate the development of related researches on molecular dynamics imaging.

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All-optical field-free three-dimensional orientation of asymmetric-top molecules

Cited by 74 publications

References 57 publications

Observation of persistent orientation of chiral molecules by a laser field with twisted polarization

Observation of persistent orientation of chiral molecules by a laser field with twisted polarization

Spatiotemporal rotational dynamics of laser-driven molecules

Direct imaging of molecular rotation with high-order-harmonic generation

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