Rotational Echoes as a Tool for Investigating Ultrafast Collisional Dynamics of Molecules

Zhang, Haisu; Lavorel, B.; Billard, F.; Hartmann, Jean‐Michel; Hertz, E.; Faucher, O.; Ma, Jing; Wu, Jian; Gershnabel, E.; Prior, Yehiam; Averbukh, Ilya Sh.

doi:10.1103/physrevlett.122.193401

Cited by 37 publications

(40 citation statements)

References 39 publications

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“…It is only very recently that the collisional dissipation of echoes has been studied 12,13 , by analyzing the evolution of their amplitudes for various delays at fixed gas density. The interest of this approach to probe the dissipation of the alignment under high-pressure conditions where standard alignment revivals cannot be used was demonstrated in ref.…”

Section: Resultsmentioning

confidence: 99%

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Observing collisions beyond the secular approximation limit

Zhang

Lavorel

et al. 2019

Nat Commun

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Quantum coherence plays an essential role in diverse natural phenomena and technological applications. The unavoidable coupling of the quantum system to an uncontrolled environment incurs dissipation that is often described using the secular approximation. Here we probe the limit of this approximation in the rotational relaxation of molecules due to thermal collisions by using the laser-kicked molecular rotor as a model system. Specifically, rotational coherences in N2O gas (diluted in He) are created by two successive nonresonant short and intense laser pulses and probed by studying the change of amplitude of the rotational alignment echo with the gas density. By interrogating the system at the early stage of its collisional relaxation, we observe a significant variation of the dissipative influence of collisions with the time of appearance of the echo, featuring a decoherence process that is well reproduced by the nonsecular quantum master equation for modeling molecular collisions.

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Section: Resultsmentioning

confidence: 99%

“…The interest of this approach to probe the dissipation of the alignment under high-pressure conditions where standard alignment revivals cannot be used was demonstrated in ref. 12 . Indeed, revivals restrict the probing of the system to specific times that are tied to the moment of inertia of the molecule.…”

Section: Resultsmentioning

confidence: 99%

Observing collisions beyond the secular approximation limit

Zhang

Lavorel

et al. 2019

Nat Commun

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“…3(a), one can see that higher-order fractional molecular echoes experience a much rapid transition from alignment to anti-alignment. Such a rapid transition will be beneficial for the ultrashort-time measurement in molecules [19,21].…”

Section: Resultsmentioning

confidence: 99%

All-optical measurement of high-order fractional molecular echoes by high-order harmonic generation

Wang

et al. 2019

Opt. Express

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An all-optical measurement of high-order fractional molecular echoes is demonstrated by using high-order harmonic generation (HHG). Excited by a pair of time-delayed short laser pulses, the signatures of full and high order fractional (1/2 and 1/3) alignment echoes are observed in the HHG signals measured from CO2 molecules at various time delays of the probe pulse. By increasing the time delay of the pump pulses, much higher order fractional (1/4) alignment echo is also observed in N2O molecules. With an analytic model based on the impulsive approximation, the spatiotemporal dynamics of the echo process are retrieved from the experiment. Compared to the typical molecular alignment revivals, high-order fractional molecular echoes are demonstrated to dephase more rapidly, which will open a new route towards the ultrashort-time measurement. The proposed HHG method paves an efficient way for accessing the high-order fractional echoes in molecules.

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“…16(a), the collisional decay is extracted from maximal echo responses at each time delay. Recently, Zhang et al 174 implemented a different strategy to measure the ps-scale irreversible dissipation in CO 2 − He mixture and pure CO 2 gas at pressure up to 50 bar. They found a range of time delays where the echo response is not very sensitive, as shown in Fig.…”

Section: Application Of Rotational Alignment Echoesmentioning

confidence: 99%

“…They use a different methodology as the one described in Ref. 174 by measuring the amplitude of the echo signal versus the gas density for different time delays τ between P 1 and P 2 . Using this approach, the authors could define a decay time constant of collisional dissipation estimated at different intervals.…”

Section: Application Of Rotational Alignment Echoesmentioning

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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Rotational Echoes as a Tool for Investigating Ultrafast Collisional Dynamics of Molecules

Cited by 37 publications

References 39 publications

Observing collisions beyond the secular approximation limit

Observing collisions beyond the secular approximation limit

All-optical measurement of high-order fractional molecular echoes by high-order harmonic generation

Spatiotemporal rotational dynamics of laser-driven molecules

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