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Recoil-induced ultrafast molecular rotation probed by dynamical rotational Doppler effect
Synchrotron SOLEIL, F-91191 Gif Sur Yvette, France..
North China Elect Power Univ, Dept Math & Phys, Beijing 102206, Peoples R China..ORCID iD: 0000-0002-4341-4823
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology. Uppsala Univ, Dept Phys & Astron, S-75120 Uppsala, Sweden..ORCID iD: 0000-0002-1763-9383
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2019 (English)In: Proceedings of the National Academy of Sciences of the United States of America, ISSN 0027-8424, E-ISSN 1091-6490, Vol. 116, no 11, p. 4877-4882Article in journal (Refereed) Published
Abstract [en]

Observing and controlling molecular motion and in particular rotation are fundamental topics in physics and chemistry. To initiate ultrafast rotation, one needs a way to transfer a large angular momentum to the molecule. As a showcase, this was performed by hard X-ray C1s ionization of carbon monoxide accompanied by spinning up the molecule via the recoil "kick" of the emitted fast photoelectron. To visualize this molecular motion, we use the dynamical rotational Doppler effect and an X-ray "pump-probe" device offered by nature itself: the recoil-induced ultrafast rotation is probed by subsequent Auger electron emission. The time information in our experiment originates from the natural delay between the C1s photoionization initiating the rotation and the ejection of the Auger electron. From a more general point of view, time-resolved measurements can be performed in two ways: either to vary the "delay" time as in conventional time-resolved pump-probe spectroscopy and use the dynamics given by the system, or to keep constant delay time and manipulate the dynamics. Since in our experiment we cannot change the delay time given by the core-hole lifetime tau, we use the second option and control the rotational speed by changing the kinetic energy of the photoelectron. The recoil-induced rotational dynamics controlled in such a way is observed as a photon energy-dependent asymmetry of the Auger line shape, in full agreement with theory. This asymmetry is explained by a significant change of the molecular orientation during the core-hole lifetime, which is comparable with the rotational period.

Place, publisher, year, edition, pages
NATL ACAD SCIENCES , 2019. Vol. 116, no 11, p. 4877-4882
Keywords [en]
rotational Doppler effect, recoil effect, ultrafast rotation, hard X-ray, Auger peak asymmetry
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-247807DOI: 10.1073/pnas.1807812116ISI: 000460911500027PubMedID: 30733297Scopus ID: 2-s2.0-85062818673OAI: oai:DiVA.org:kth-247807DiVA, id: diva2:1300909
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QC 20190401

Available from: 2019-04-01 Created: 2019-04-01 Last updated: 2019-04-01Bibliographically approved

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Liu, Ji-Caida Cruz, Vinicius VazÅgren, HansGel'mukhanov, Faris
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