Details
| Original language | English |
|---|---|
| Article number | 3364 |
| Journal | Nature Communications |
| Volume | 10 |
| Issue number | 1 |
| Early online date | 29 Jul 2019 |
| Publication status | Published - 1 Dec 2019 |
| Externally published | Yes |
Abstract
Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.
ASJC Scopus subject areas
- Chemistry(all)
- General Chemistry
- Biochemistry, Genetics and Molecular Biology(all)
- General Biochemistry,Genetics and Molecular Biology
- Physics and Astronomy(all)
- General Physics and Astronomy
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In: Nature Communications, Vol. 10, No. 1, 3364, 01.12.2019.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Molecular movie of ultrafast coherent rotational dynamics of OCS
AU - Karamatskos, Evangelos T.
AU - Raabe, Sebastian
AU - Mullins, Terry
AU - Trabattoni, Andrea
AU - Stammer, Philipp
AU - Goldsztejn, Gildas
AU - Johansen, Rasmus R.
AU - Długołecki, Karol
AU - Stapelfeldt, Henrik
AU - Vrakking, Marc J.J.
AU - Trippel, Sebastian
AU - Rouzée, Arnaud
AU - Küpper, Jochen
PY - 2019/12/1
Y1 - 2019/12/1
N2 - Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.
AB - Recording molecular movies on ultrafast timescales has been a longstanding goal for unravelling detailed information about molecular dynamics. Here we present the direct experimental recording of very-high-resolution and -fidelity molecular movies over more than one-and-a-half periods of the laser-induced rotational dynamics of carbonylsulfide (OCS) molecules. Utilising the combination of single quantum-state selection and an optimised two-pulse sequence to create a tailored rotational wavepacket, an unprecedented degree of field-free alignment, 〈cos2θ2D〉 = 0.96 (〈cos2θ〉 = 0.94) is achieved, exceeding the theoretical limit for single-pulse alignment. The very rich experimentally observed quantum dynamics is fully recovered by the angular probability distribution obtained from solutions of the time-dependent Schrödinger equation with parameters refined against the experiment. The populations and phases of rotational states in the retrieved time-dependent three-dimensional wavepacket rationalises the observed very high degree of alignment.
UR - http://www.scopus.com/inward/record.url?scp=85069897091&partnerID=8YFLogxK
U2 - 10.1038/s41467-019-11122-y
DO - 10.1038/s41467-019-11122-y
M3 - Article
C2 - 31358749
AN - SCOPUS:85069897091
VL - 10
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 3364
ER -