Show simple item record

dc.contributor.author
Baykusheva, Denitsa
dc.contributor.author
Wörner, Hans Jakob
dc.date.accessioned
2018-10-02T15:29:47Z
dc.date.available
2018-09-22T08:21:43Z
dc.date.available
2018-10-01T12:08:46Z
dc.date.available
2018-10-02T15:29:47Z
dc.date.issued
2018-09-10
dc.identifier.issn
2160-3308
dc.identifier.other
10.1103/PhysRevX.8.031060
en_US
dc.identifier.uri
http://hdl.handle.net/20.500.11850/291145
dc.identifier.doi
10.3929/ethz-b-000291145
dc.description.abstract
Molecular chirality plays an essential role in most biochemical processes. The observation and quantification of chirality-sensitive signals, however, remains extremely challenging, especially on ultrafast timescales and in dilute media. Here, we describe the experimental realization of an all-optical and ultrafast scheme for detecting chiral dynamics in molecules. This technique is based on high-harmonic generation by a combination of two-color counterrotating femtosecond laser pulses with polarization states tunable from linear to circular. We demonstrate two different implementations of chiral-sensitive high-harmonic spectroscopy on an ensemble of randomly oriented methyloxirane molecules in the gas phase. Using two elliptically polarized fields, we observe that the ellipticities maximizing the harmonic signal reach up to 4.4±0.2% (at 17.6 eV). Using two circularly polarized fields, we observe circular dichroisms ranging up to 13±6% (28.3–33.1 eV). Our theoretical analysis confirms that the observed chiral response originates from subfemtosecond electron dynamics driven by the magnetic component of the driving laser field. This assignment is supported by the experimental observation of a strong intensity dependence of the chiral effects and its agreement with theory. We moreover report and explain a pronounced variation of the signal strength and dichroism with the driving-field ellipticities and harmonic orders. Finally, we demonstrate the sensitivity of the experimental observables to the shape of the electron hole. This technique for chiral discrimination will yield femtosecond temporal resolution when integrated in a pump-probe scheme and subfemtosecond resolution on chiral charge migration in a self-probing scheme.
en_US
dc.format
application/pdf
en_US
dc.language.iso
en
en_US
dc.publisher
American Physical Society
en_US
dc.rights.uri
http://creativecommons.org/licenses/by/4.0/
dc.title
Chiral Discrimination through Bielliptical High-Harmonic Spectroscopy
en_US
dc.type
Journal Article
dc.rights.license
Creative Commons Attribution 4.0 International
ethz.journal.title
Physical Review X
ethz.journal.volume
8
en_US
ethz.journal.issue
3
en_US
ethz.journal.abbreviated
Phys. rev., X
ethz.pages.start
031060
en_US
ethz.size
12 p.
en_US
ethz.version.deposit
publishedVersion
en_US
ethz.grant
Measuring attosecond electron dynamics in molecules
en_US
ethz.identifier.wos
ethz.identifier.scopus
ethz.publication.place
Woodbury, NY
en_US
ethz.publication.status
published
en_US
ethz.leitzahl
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02515 - Laboratorium für Physikalische Chemie / Laboratory of Physical Chemistry::03888 - Wörner, Hans Jakob / Wörner, Hans Jakob
ethz.leitzahl.certified
ETH Zürich::00002 - ETH Zürich::00012 - Lehre und Forschung::00007 - Departemente::02020 - Dep. Chemie und Angewandte Biowiss. / Dep. of Chemistry and Applied Biosc.::02515 - Laboratorium für Physikalische Chemie / Laboratory of Physical Chemistry::03888 - Wörner, Hans Jakob / Wörner, Hans Jakob
ethz.grant.agreementno
307270
ethz.grant.agreementno
307270
ethz.grant.fundername
EC
ethz.grant.fundername
EC
ethz.grant.funderDoi
10.13039/501100000780
ethz.grant.funderDoi
10.13039/501100000780
ethz.grant.program
FP7
ethz.grant.program
FP7
ethz.date.deposited
2018-09-22T08:22:04Z
ethz.source
WOS
ethz.eth
yes
en_US
ethz.availability
Open access
en_US
ethz.rosetta.installDate
2018-10-02T15:29:51Z
ethz.rosetta.lastUpdated
2018-12-03T00:39:22Z
ethz.rosetta.exportRequired
true
ethz.rosetta.versionExported
true
ethz.COinS
ctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.atitle=Chiral%20Discrimination%20through%20Bielliptical%20High-Harmonic%20Spectroscopy&rft.jtitle=Physical%20Review%20X&rft.date=2018-09-10&rft.volume=8&rft.issue=3&rft.spage=031060&rft.issn=2160-3308&rft.au=Baykusheva,%20Denitsa&W%C3%B6rner,%20Hans%20Jakob&rft.genre=article&
 Search via SFX

Files in this item

Thumbnail

Publication type

Show simple item record