Measurements on the strong-field ionization of carbonyl sulfide molecules by short, intense, 2 µm wavelength laser pulses are presented from experiments where angle-resolved photoelectron distributions were recorded with a high-energy velocity map imaging spectrometer, designed to reach a maximum kinetic energy of 500 eV. The laser-field-free elastic-scattering cross section of carbonyl sulfide was extracted from the measurements and is found in good agreement with previous experiments, performed using conventional electron diffraction. By comparing our measurements to the results of calculations, based on the quantitative rescattering theory, the bond lengths and molecular geometry were extracted from the experimental differential cross sections to a precision better than ±5 pm and in agreement with the known values.

1.
J.
Küpper
,
S.
Stern
,
L.
Holmegaard
,
F.
Filsinger
,
A.
Rouzée
,
A.
Rudenko
,
P.
Johnsson
,
A. V.
Martin
,
M.
Adolph
,
A.
Aquila
,
S.
Bajt
,
A.
Barty
,
C.
Bostedt
,
J.
Bozek
,
C.
Caleman
,
R.
Coffee
,
N.
Coppola
,
T.
Delmas
,
S.
Epp
,
B.
Erk
,
L.
Foucar
,
T.
Gorkhover
,
L.
Gumprecht
,
A.
Hartmann
,
R.
Hartmann
,
G.
Hauser
,
P.
Holl
,
A.
Hömke
,
N.
Kimmel
,
F.
Krasniqi
,
K.-U.
Kühnel
,
J.
Maurer
,
M.
Messerschmidt
,
R.
Moshammer
,
C.
Reich
,
B.
Rudek
,
R.
Santra
,
I.
Schlichting
,
C.
Schmidt
,
S.
Schorb
,
J.
Schulz
,
H.
Soltau
,
J. C. H.
Spence
,
D.
Starodub
,
L.
Strüder
,
J.
Thøgersen
,
M. J. J.
Vrakking
,
G.
Weidenspointner
,
T. A.
White
,
C.
Wunderer
,
G.
Meijer
,
J.
Ullrich
,
H.
Stapelfeldt
,
D.
Rolles
, and
H. N.
Chapman
, “
X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser
,”
Phys. Rev. Lett.
112
,
083002
(
2014
); e-print arXiv:1307.4577 [physics].
2.
J. M.
Glownia
,
A.
Natan
,
J. P.
Cryan
,
R.
Hartsock
,
M.
Kozina
,
M. P.
Minitti
,
S.
Nelson
,
J.
Robinson
,
T.
Sato
,
T.
van Driel
,
G.
Welch
,
C.
Weninger
,
D.
Zhu
, and
P. H.
Bucksbaum
, “
Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion
,”
Phys. Rev. Lett.
117
,
153003
(
2016
); e-print arXiv:1608.03039 [physics].
3.
S. P.
Weathersby
,
G.
Brown
,
M.
Centurion
,
T. F.
Chase
,
R.
Coffee
,
J.
Corbett
,
J. P.
Eichner
,
J. C.
Frisch
,
A. R.
Fry
,
M.
Gühr
,
N.
Hartmann
,
C.
Hast
,
R.
Hettel
,
R. K.
Jobe
,
E. N.
Jongewaard
,
J. R.
Lewandowski
,
R. K.
Li
,
A. M.
Lindenberg
,
I.
Makasyuk
,
J. E.
May
,
D.
McCormick
,
M. N.
Nguyen
,
A. H.
Reid
,
X.
Shen
,
K.
Sokolowski-Tinten
,
T.
Vecchione
,
S. L.
Vetter
,
J.
Wu
,
J.
Yang
,
H. A.
Dürr
, and
X. J.
Wang
, “
Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory
,”
Rev. Sci. Instrum.
86
,
073702
(
2015
).
4.
J.
Yang
,
M.
Guehr
,
X.
Shen
,
R.
Li
,
T.
Vecchione
,
R.
Coffee
,
J.
Corbett
,
A.
Fry
,
N.
Hartmann
,
C.
Hast
,
K.
Hegazy
,
K.
Jobe
,
I.
Makasyuk
,
J.
Robinson
,
M. S.
Robinson
,
S.
Vetter
,
S.
Weathersby
,
C.
Yoneda
,
X.
Wang
, and
M.
Centurion
, “
Diffractive imaging of coherent nuclear motion in isolated molecules
,”
Phys. Rev. Lett.
117
,
153002
(
2016
).
5.
P. B.
Corkum
, “
Plasma perspective on strong-field multiphoton ionization
,”
Phys. Rev. Lett.
71
,
1994
1997
(
1993
).
6.
M.
Spanner
,
O.
Smirnova
,
P. B.
Corkum
, and
M. Y.
Ivanov
, “
Reading diffraction images in strong field ionization of diatomic molecules
,”
J. Phys. B: At. Mol. Opt. Phys.
37
,
L243
L250
(
2004
).
7.
C. I.
Blaga
,
J.
Xu
,
A. D.
DiChiara
,
E.
Sistrunk
,
K.
Zhang
,
P.
Agostini
,
T. A.
Miller
,
L. F.
DiMauro
, and
C. D.
Lin
, “
Imaging ultrafast molecular dynamics with laser-induced electron diffraction
,”
Nature
483
,
194
197
(
2012
).
8.
M.
Okunishi
,
T.
Morishita
,
G.
Prümper
,
K.
Shimada
,
C. D.
Lin
,
S.
Watanabe
, and
K.
Ueda
, “
Experimental retrieval of target structure information from laser-induced rescattered photoelectron momentum distributions
,”
Phys. Rev. Lett.
100
,
143001
(
2008
).
9.
J.
Xu
,
C. I.
Blaga
,
A. D.
DiChiara
,
E.
Sistrunk
,
K.
Zhang
,
Z.
Chen
,
A.-T.
Le
,
T.
Morishita
,
C. D.
Lin
,
P.
Agostini
, and
L. F.
DiMauro
, “
Laser-induced electron diffraction for probing rare gas atoms
,”
Phys. Rev. Lett.
109
,
233002
(
2012
).
10.
J.
Xu
,
C. I.
Blaga
,
K.
Zhang
,
Y. H.
Lai
,
C. D.
Lin
,
T. A.
Miller
,
P.
Agostini
, and
L. F.
DiMauro
, “
Diffraction using laser-driven broadband electron wave packets
,”
Nat. Commun.
5
,
4635
(
2014
).
11.
M. G.
Pullen
,
B.
Wolter
,
A.-T.
Le
,
M.
Baudisch
,
M.
Hemmer
,
A.
Senftleben
,
C. D.
Schroter
,
J.
Ullrich
,
R.
Moshammer
,
C. D.
Lin
, and
J.
Biegert
, “
Imaging an aligned polyatomic molecule with laser-induced electron diffraction
,”
Nat. Commun.
6
,
7262
(
2015
).
12.
Y.
Ito
,
R.
Carranza
,
M.
Okunishi
,
R. R.
Lucchese
, and
K.
Ueda
, “
Extraction of geometrical structure of ethylene molecules by laser-induced electron diffraction combined with ab initio scattering calculations
,”
Phys. Rev. A
96
,
053414
(
2017
).
13.
Y.
Ito
,
C.
Wang
,
A.-T.
Le
,
M.
Okunishi
,
D.
Ding
,
C. D.
Lin
, and
K.
Ueda
, “
Extracting conformational structure information of benzene molecules via laser-induced electron diffraction
,”
Struct. Dyn.
3
,
034303
(
2016
).
14.
S. G.
Walt
,
B. N.
Ram
,
M.
Atala
,
N. I.
Shvetsov-Shilovski
,
A.
von Conta
,
D.
Baykusheva
,
M.
Lein
, and
H. J.
Wörner
, “
Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering
,”
Nat. Commun.
8
,
15651
(
2017
).
15.
B.
Wolter
,
M. G.
Pullen
,
A. T.
Le
,
M.
Baudisch
,
K.
Doblhoff-Dier
,
A.
Senftleben
,
M.
Hemmer
,
C. D.
Schroter
,
J.
Ullrich
,
T.
Pfeifer
,
R.
Moshammer
,
S.
Gräfe
,
O.
Vendrell
,
C. D.
Lin
, and
J.
Biegert
, “
Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene
,”
Science
354
,
308
312
(
2016
).
16.
M.
Brouard
,
A. V.
Green
,
F.
Quadrini
, and
C.
Vallance
, “
Photodissociation dynamics of OCS at 248 nm: The S(D21) atomic angular momentum polarization
,”
J. Chem. Phys.
127
,
084304
(
2007
).
17.
T.
Suzuki
,
H.
Katayanagi
,
S.
Nanbu
, and
M.
Aoyagi
, “
Nonadiabatic bending dissociation in 16 valence electron system OCS
,”
J. Chem. Phys.
109
,
5778
5794
(
1998
).
18.
N.
Sivakumar
,
I.
Burak
,
W. Y.
Cheung
,
P. L.
Houston
, and
J. W.
Hepburn
, “
State-resolved photofragmentation of carbonyl sulfide (OCS) monomers and clusters
,”
J. Phys. Chem.
89
,
3609
3611
(
1985
).
19.
J. H.
Sanderson
,
T. R. J.
Goodworth
,
A.
El-Zein
,
W. A.
Bryan
,
W. R.
Newell
,
A. J.
Langley
, and
P. F.
Taday
, “
Coulombic and pre-Coulombic geometry evolution of carbonyl sulfide in an intense femtosecond laser pulse, determined by momentum imaging
,”
Phys. Rev. A
65
,
043403
(
2002
).
20.
A. T. J. B.
Eppink
and
D. H.
Parker
, “
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen
,”
Rev. Sci. Instrum.
68
,
3477
3484
(
1997
).
21.
F.
Salvat
,
A.
Jablonski
, and
C.
Powell
, “
ELSEPA—Dirac partial-wave calculation of elastic scattering of electrons and positrons by atoms, positive ions and molecules
,”
Comput. Phys. Commun.
165
,
157
190
(
2005
).
22.
T. W.
Dakin
,
W. E.
Good
, and
D. K.
Coles
, “
Bond distances in OCS from microwave absorption lines
,”
Phys. Rev.
71
,
640
641
(
1947
).
23.
J. S.
Kienitz
,
K.
Długołęcki
,
S.
Trippel
, and
J.
Küpper
, “
Improved spatial separation of neutral molecules
,”
J. Chem. Phys.
147
,
024304
(
2017
); e-print arXiv:1704.08912 [physics].
24.
Y.-P.
Chang
,
D. A.
Horke
,
S.
Trippel
, and
J.
Küpper
, “
Spatially-controlled complex molecules and their applications
,”
Int. Rev. Phys. Chem.
34
,
557
590
(
2015
); e-print arXiv:1505.05632 [physics].
25.
N.
Teschmit
,
D. A.
Horke
, and
J.
Küpper
, “
Spatially separating the conformers of the dipeptide Ac-Phe-Cys-NH2
,”
Angew. Chem., Int. Ed.
57
,
13775
13779
(
2018
); e-print arXiv:1805.12396 [physics].
26.
S.
Trippel
,
M.
Johny
,
T.
Kierspel
,
J.
Onvlee
,
H.
Bieker
,
H.
Ye
,
T.
Mullins
,
L.
Gumprecht
,
K.
Długołęcki
, and
J.
Küpper
, “
Knife edge skimming for improved separation of molecular species by the deflector
,”
Rev. Sci. Instrum.
89
,
096110
(
2018
); e-print arXiv:1802.04053 [physics].
27.
J. H.
Nielsen
,
P.
Simesen
,
C. Z.
Bisgaard
,
H.
Stapelfeldt
,
F.
Filsinger
,
B.
Friedrich
,
G.
Meijer
, and
J.
Küpper
, “
Stark-selected beam of ground-state OCS molecules characterized by revivals of impulsive alignment
,”
Phys. Chem. Chem. Phys.
13
,
18971
18975
(
2011
); e-print arXiv:1105.2413 [physics].
28.
E. T.
Karamatskos
,
S.
Raabe
,
T.
Mullins
,
A.
Trabattoni
,
P.
Stammer
,
G.
Goldsztejn
,
R. R.
Johansen
,
K.
Długołęcki
,
H.
Stapelfeldt
,
M. J. J.
Vrakking
,
S.
Trippel
,
A.
Rouzée
, and
J.
Küpper
, “
Molecular movie of ultrafast coherent rotational dynamics
,”
Nat. Comm.
, e-print arXiv:1807.01034 (
2018
).
29.
V.
Dribinski
,
A.
Ossadtchi
,
V. A.
Mandelshtam
, and
H.
Reisler
, “
Reconstruction of Abel-transformable images: The Gaussian basis-set expansion Abel transform method
,”
Rev. Sci. Instrum.
73
,
2634
(
2002
).
30.
Z.
Chen
,
A.-T.
Le
,
T.
Morishita
, and
C. D.
Lin
, “
Quantitative rescattering theory for laser-induced high-energy plateau photoelectron spectra
,”
Phys. Rev. A
79
,
033409
(
2009
).
31.
J.
Xu
,
Z.
Chen
,
A.-T.
Le
, and
C. D.
Lin
, “
Self-imaging of molecules from diffraction spectra by laser-induced rescattering electrons
,”
Phys. Rev. A
82
,
033403
(
2010
).
32.
W. C.
Fon
,
K. A.
Berrington
,
P. G.
Burke
, and
A.
Hibbert
, “
The elastic scattering of electrons from inert gases. III. Argon
,”
J. Phys. B: At. Mol. Phys.
16
,
307
(
1983
).
33.
W. C.
Fon
,
K. A.
Berrington
, and
A.
Hibbert
, “
The elastic scattering of electrons from inert gases. IV. Krypton
,”
J. Phys. B: At. Mol. Phys.
17
,
3279
3294
(
1984
).
34.
H.
Murai
,
Y.
Ishijima
,
T.
Mitsumura
,
Y.
Sakamoto
,
H.
Kato
,
M.
Hoshino
,
F.
Blanco
,
G.
Garcia
,
P.
Limao-Vieira
,
M. J.
Brunger
,
S. J.
Buckman
, and
H.
Tanaka
, “
A comprehensive and comparative study of elastic electron scattering from OCS and CS2 in the energy region from 1.2 to 200 eV
,”
J. Chem. Phys.
138
,
054302
(
2013
).
35.
S. E.
Michelin
,
T.
Kroin
,
I.
Iga
,
M. G. P.
Homem
,
H. S.
Miglio
, and
M. T.
Lee
, “
Elastic and total cross sections for electron-carbonyl sulfide collisions
,”
J. Phys. B
33
,
3293
(
2000
).
36.
F.
Schell
,
T.
Bredtmann
,
C.-P.
Schulz
,
S.
Patchkovskii
,
M. J. J.
Vrakking
, and
J.
Mikosch
, “
Molecular orbital imprint in laser-driven electron recollision
,”
Sci. Adv.
4
,
eaap8148
(
2018
).
37.
F.
Krečinić
,
P.
Wopperer
,
B.
Frusteri
,
F.
Brauße
,
J.-G.
Brisset
,
U.
De Giovannini
,
A.
Rubio
,
A.
Rouzée
, and
M. J. J.
Vrakking
, “
Multiple-orbital effects in laser-induced electron diffraction of aligned molecules
,”
Phys. Rev. A
98
,
041401
(
2018
).
38.
A.
Trabattoni
,
S.
Trippel
,
U. D.
Giovannini
,
J. F.
Olivieri
,
J.
Wiese
,
T.
Mullins
,
J.
Onvlee
,
S.-K.
Son
,
A. R.
Biagio Frusteri
, and
J.
Küpper
, “
Setting the clock of photoelectron emission through molecular alignment
,” e-print arXiv:1802.06622 [physics] (
2018
).
39.
L.
Holmegaard
,
J. L.
Hansen
,
L.
Kalhoj
,
S. L.
Kragh
,
H.
Stapelfeldt
,
F.
Filsinger
,
J.
Küpper
,
G.
Meijer
,
D.
Dimitrovski
,
M.
Abu-samha
,
C. P. J.
Martiny
, and
L. B.
Madsen
, “
Photoelectron angular distributions from strong-field ionization of oriented molecules
,”
Nat. Phys.
6
,
428
(
2010
).
40.
G.
Bilalbegovic
, “
Carbonyl sulphide under strong laser field: Time-dependent density functional theory
,”
Eur. Phys. J. D
49
,
43
49
(
2008
).
41.
I.
Hargittai
and
M.
Hargittai
,
Stereochemical Applications of Gas-Phase Electron Diffraction
(
VCH Verlagsgesellschaft
,
Weinheim, Germany
,
1988
).
42.
C. D.
Lin
,
A.-T.
Le
,
Z.
Chen
,
T.
Morishita
, and
R.
Lucchese
, “
Strong-field rescattering physics—Self-imaging of a molecule by its own electrons
,”
J. Phys. B: At., Mol. Opt. Phys.
43
,
122001
(
2010
).
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