Optical Centrifuge for Molecules

Karczmarek, Joanna L.; Wright, James S.; Corkum, P. B.; Ivanov, Misha

doi:10.1103/physrevlett.82.3420

Cited by 266 publications

(315 citation statements)

References 19 publications

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“…The × points refer to the direct numerical calculations based on the distribution function given by Eq. (28). Although the asymptotic results (40) are formally valid for J T ≥ 1, and P ≫ J T , they provide a good agreement with the exact numerical simulations already for P/J T = 2.…”

Section: Classical Treatment: Weak Deflecting Fieldsupporting

confidence: 66%

“…Narrowing the distribution of the scattering angles may substantially increase the efficiency of separation of multi-component beams, especially when the prealignment is applied selectively to certain molecular species, such as isotopes [25], or nuclear spin isomers [26,27]. More complicated techniques for pre-shaping the molecular angular distribution may be considered, such as confining molecular rotation to a certain plane by using the "optical molecular centrifuge" approach [28], double-pulse ignited "molecular propeller" [29][30][31][32][33], or planar alignment by perpendicularly polarized laser pulses [34]. In this case, a narrow angular peak is expected in molecular scattering, whose position is controllable by inclination of the plane of rotation with respect to the deflecting field [35].…”

Section: Discussionmentioning

confidence: 99%

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Controlling molecular scattering by laser-induced field-free alignment

Gershnabel

Averbukh

2010

Phys. Rev. A

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We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbow-like features in the distribution of the scattering angle. Moreover, by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. We provide quantum and classical treatment of the deflection process. The effects of strong deflecting field on the scattering of rotating molecules are considered by the means of the adiabatic invariants formalism. This new control scheme opens new ways for many applications involving molecular focusing, guiding and trapping by optical and static fields.

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Section: Classical Treatment: Weak Deflecting Fieldsupporting

confidence: 66%

Section: Discussionmentioning

confidence: 99%

Controlling molecular scattering by laser-induced field-free alignment

Gershnabel

Averbukh

2010

Phys. Rev. A

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“…Although sequences of pulses have been successfully used for selective [18][19][20][21] and directional [22][23][24] rotational excitation, the range of accessible rotational states has been limited to relatively low rotational quantum numbers (of order 10 above the initial state) due to the molecular breakdown in intense laser fields. To extend the range of accessible angular momenta, a number of theoretical proposals aimed at guiding the molecules up the "ladder" of rotational levels "step-by-step" instead of exerting a single ultrashort rotational kick [25][26][27][28]. An efficient method of accelerating molecular rotation with an "optical centrifuge" has been proposed [25] and successfully implemented [29][30][31].…”

mentioning

confidence: 99%

“…The final speed of rotation is determined by the spectral bandwidth of the laser pulse and may exceed 10 13 Hz. To make O 2 molecules rotate primarily with this speed in thermal equilibrium, the gas temperature would have to have risen to above 50 000 Kelvin.Since the original proposal [25], an optical centrifuge has been implemented by two experimental groups. In the pioneering work by Villeneuve et al, dissociation of chlorine molecules exposed to the centrifuge field has been attributed to the breaking of the Cl-Cl bond which could not withstand the extremely high spinning rates [29].…”

mentioning

confidence: 99%

“…To extend the range of accessible angular momenta, a number of theoretical proposals aimed at guiding the molecules up the "ladder" of rotational levels "step-by-step" instead of exerting a single ultrashort rotational kick [25][26][27][28]. An efficient method of accelerating molecular rotation with an "optical centrifuge" has been proposed [25] and successfully implemented [29][30][31]. Molecular spinning with an optical centrifuge, also realized in this work, is achieved by forcing the molecules to follow the rotating polarization of a laser field.…”

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confidence: 99%

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Quantum Superrotor

Ohmori¹

2014

Physics

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Extremely fast rotating molecules whose rotational energy is comparable with the molecular bond strength are known as "superrotors." It has been speculated that superrotors may exhibit a number of unique properties, yet only indirect evidence of these molecular objects has been reported to date. Here we demonstrate the first direct observation of molecular superrotors by detecting coherent unidirectional molecular rotation with extreme frequencies exceeding 10 THz. The technique of an "optical centrifuge" is used to control the degree of rotational excitation in an ultrabroad range of rotational quantum numbers, reaching as high as N ¼ 95 in oxygen and N ¼ 60 in nitrogen. State-resolved detection enables us to determine the shape of the excited rotational wave packet and quantify the effect of centrifugal distortion on the rotational spectrum. Femtosecond time resolution reveals coherent rotational dynamics with increasing coherence times at higher angular momentum. We demonstrate that molecular superrotors can be created and observed in dense samples under normal conditions where the effects of ultrafast rotation on manybody interactions, intermolecular collisions, and chemical reactions can be readily explored. DOI: 10.1103/PhysRevLett.112.113004 PACS numbers: 33.15.-e, 33.20.Sn, 33.20.Xx Control of molecular rotation has been long recognized and successfully used as a powerful tool for steering chemical reactions in gases [1], and, at gas-surface interfaces [2,3], for imaging individual molecular orbitals [4] and generating extreme ultraviolet radiation [5,6], for deflecting molecular beams [7], and separating molecular isotopes [8]. The control is achieved by means of the spatial alignment of molecular axes and generally does not require a high degree of rotational excitation. On the other hand, extending the reach of rotational control to high rotational states is motivated by theoretical studies which show that ultrafast molecular rotation may change the character of molecular scattering from solid surfaces [9], alter molecular trajectories in external fields [10], increase stability against collisions [11], and lead to the formation of gas vortices [12]. New ways of molecular cooling [13] and selective chemical bond breaking [14] by ultrafast spinning have been suggested.The appeal of rotational control has stimulated the development of multiple techniques in which molecules are exposed to strong nonresonant laser pulses [15,16]. However, bringing a large number of molecules to fast rotation is rather challenging. Conventional single-pulse excitation schemes lack selectivity with respect to the final speed of molecular rotation and produce broad rotational distributions [17]. Although sequences of pulses have been successfully used for selective [18][19][20][21] and directional [22][23][24] rotational excitation, the range of accessible rotational states has been limited to relatively low rotational quantum numbers (of order 10 above the initial state) due to the molecular breakdown in intense laser f...

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Laser Control of Ultrafast Molecular Rotation

Milner

Hepburn

2016

Advances in Chemical Physics Volume 159

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Optical Centrifuge for Molecules

Cited by 266 publications

References 19 publications

Controlling molecular scattering by laser-induced field-free alignment

Controlling molecular scattering by laser-induced field-free alignment

Quantum Superrotor

Laser Control of Ultrafast Molecular Rotation

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