Retrieval of the molecular orientation distribution from atom-pair angular distributions
Abstract
Imaging laser-induced rotational dynamics is an important and active field due to its applications in capturing reactions in the molecular frame and in molecular imaging. Experimental measurement of the molecular orientation distribution, as a function of the Euler angles, has only been demonstrated for special cases when the detectable signal is generated along the molecular symmetry axis. Here we developed the general theory that maps the probability density distribution of the molecular orientation to the atom-pair angular distributions for nonlinear molecules. With the theory, the molecular orientation distribution can be retrieved from the measured atom-pair angular distribution, which we demonstrate experimentally using ultrafast electron diffractive imaging of impulsively aligned trifluoro-iodomethane molecules. Here, the retrieved molecular orientation distribution is in good agreement with direct numerical simulations of the time-dependent Schrodinger equation using the experimental conditions. Unlike the existing retrieval methods, the retrieval method does not require solving Schrodinger equation, works for any alignment method, and is in principle applicable to asymmetric top molecules.
- Authors:
-
- Univ. of Nebraska, Lincoln, NE (United States)
- Publication Date:
- Research Org.:
- Univ. of Nebraska, Lincoln, NE (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation, Physics Division, Atomic, Molecular and Optical Sciences
- OSTI Identifier:
- 1887801
- Grant/Contract Number:
- SC0014170; PHY-1606619
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 106; Journal Issue: 3; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; Atomic & molecular processes in external fields; Electron & positron scattering; Electron beams & optics; Light-matter interaction; Ultrafast phenomena
Citation Formats
Xiong, Yanwei, Wilkin, Kyle J., Saha, Sajib Kumar, Muvva, Sri Bhavya, Zhao, Haoran, and Centurion, Martin. Retrieval of the molecular orientation distribution from atom-pair angular distributions. United States: N. p., 2022.
Web. doi:10.1103/physreva.106.033109.
Xiong, Yanwei, Wilkin, Kyle J., Saha, Sajib Kumar, Muvva, Sri Bhavya, Zhao, Haoran, & Centurion, Martin. Retrieval of the molecular orientation distribution from atom-pair angular distributions. United States. https://doi.org/10.1103/physreva.106.033109
Xiong, Yanwei, Wilkin, Kyle J., Saha, Sajib Kumar, Muvva, Sri Bhavya, Zhao, Haoran, and Centurion, Martin. Mon .
"Retrieval of the molecular orientation distribution from atom-pair angular distributions". United States. https://doi.org/10.1103/physreva.106.033109. https://www.osti.gov/servlets/purl/1887801.
@article{osti_1887801,
title = {Retrieval of the molecular orientation distribution from atom-pair angular distributions},
author = {Xiong, Yanwei and Wilkin, Kyle J. and Saha, Sajib Kumar and Muvva, Sri Bhavya and Zhao, Haoran and Centurion, Martin},
abstractNote = {Imaging laser-induced rotational dynamics is an important and active field due to its applications in capturing reactions in the molecular frame and in molecular imaging. Experimental measurement of the molecular orientation distribution, as a function of the Euler angles, has only been demonstrated for special cases when the detectable signal is generated along the molecular symmetry axis. Here we developed the general theory that maps the probability density distribution of the molecular orientation to the atom-pair angular distributions for nonlinear molecules. With the theory, the molecular orientation distribution can be retrieved from the measured atom-pair angular distribution, which we demonstrate experimentally using ultrafast electron diffractive imaging of impulsively aligned trifluoro-iodomethane molecules. Here, the retrieved molecular orientation distribution is in good agreement with direct numerical simulations of the time-dependent Schrodinger equation using the experimental conditions. Unlike the existing retrieval methods, the retrieval method does not require solving Schrodinger equation, works for any alignment method, and is in principle applicable to asymmetric top molecules.},
doi = {10.1103/physreva.106.033109},
journal = {Physical Review A},
number = 3,
volume = 106,
place = {United States},
year = {Mon Sep 19 00:00:00 EDT 2022},
month = {Mon Sep 19 00:00:00 EDT 2022}
}
Works referenced in this record:
Attosecond transient-absorption spectroscopy on aligned molecules
journal, October 2016
- Bækhøj, Jens E.; Madsen, Lars Bojer
- Physical Review A, Vol. 94, Issue 4
Laser-Induced Coulomb Explosion Imaging of Aligned Molecules and Molecular Dimers
journal, April 2022
- Schouder, Constant A.; Chatterley, Adam S.; Pickering, James D.
- Annual Review of Physical Chemistry, Vol. 73, Issue 1
Experimental Observation of Revival Structures in Picosecond Laser-Induced Alignment of I2
journal, September 2001
- Rosca-Pruna, F.; Vrakking, M.
- Physical Review Letters, Vol. 87, Issue 15
Molecular Alignment Induced by Ultrashort Laser Pulses and Its Impact on Molecular Motion
journal, April 2012
- Fleischer , Sharly; Khodorkovsky, Yuri; Gershnabel, Erez
- Israel Journal of Chemistry, Vol. 52, Issue 5
Strong-field induced fragmentation and isomerization of toluene probed by ultrafast femtosecond electron diffraction and mass spectrometry
journal, January 2021
- Xiong, Yanwei; Borne, Kurtis; Carrascosa, Andrés Moreno
- Faraday Discussions, Vol. 228
Femtosecond gas phase electron diffraction with MeV electrons
journal, January 2016
- Yang, Jie; Guehr, Markus; Vecchione, Theodore
- Faraday Discussions, Vol. 194
Generalized molecular orbital tomography
journal, June 2011
- Vozzi, C.; Negro, M.; Calegari, F.
- Nature Physics, Vol. 7, Issue 10
Towards molecular frame photoelectron angular distributions in polyatomic molecules from lab frame coherent rotational wavepacket evolution
journal, July 2021
- Gregory, Margaret; Hockett, Paul; Stolow, Albert
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 54, Issue 14
Role of rotational temperature in adiabatic molecular alignment
journal, November 2006
- Kumarappan, Vinod; Bisgaard, Christer Z.; Viftrup, Simon S.
- The Journal of Chemical Physics, Vol. 125, Issue 19
Tilted femtosecond pulses for velocity matching in gas-phase ultrafast electron diffraction
journal, August 2014
- Zhang, Ping; Yang, Jie; Centurion, Martin
- New Journal of Physics, Vol. 16, Issue 8
Alignment of symmetric top molecules by short laser pulses
journal, October 2005
- Hamilton, Edward; Seideman, Tamar; Ejdrup, Tine
- Physical Review A, Vol. 72, Issue 4
Nonadiabatic laser-induced alignment of iodobenzene molecules
journal, December 2004
- Péronne, Emmanuel; Poulsen, Mikael D.; Stapelfeldt, Henrik
- Physical Review A, Vol. 70, Issue 6
Photodissociation of laser aligned iodobenzene: Towards selective photoexcitation
journal, August 2002
- Poulsen, Mikael D.; Skovsen, Esben; Stapelfeldt, Henrik
- The Journal of Chemical Physics, Vol. 117, Issue 5
Colloquium : Aligning molecules with strong laser pulses
journal, April 2003
- Stapelfeldt, Henrik; Seideman, Tamar
- Reviews of Modern Physics, Vol. 75, Issue 2
Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules
journal, March 2009
- Bisgaard, C. Z.; Clarkin, O. J.; Wu, G.
- Science, Vol. 323, Issue 5920
The quantitative determination of laser-induced molecular axis alignment
journal, July 2013
- Mikosch, Jochen; Bisgaard, Christer Z.; Boguslavskiy, Andrey E.
- The Journal of Chemical Physics, Vol. 139, Issue 2
Role of orbital symmetry in high-order harmonic generation from aligned molecules
journal, March 2004
- Nalda, R. de; Heesel, E.; Lein, M.
- Physical Review A, Vol. 69, Issue 3
Molecular movie of ultrafast coherent rotational dynamics of OCS
journal, July 2019
- Karamatskos, Evangelos T.; Raabe, Sebastian; Mullins, Terry
- Nature Communications, Vol. 10, Issue 1
Manipulating the Torsion of Molecules by Strong Laser Pulses
journal, February 2009
- Madsen, C. B.; Madsen, L. B.; Viftrup, S. S.
- Physical Review Letters, Vol. 102, Issue 7
Quantum interference during high-order harmonic generation from aligned molecules
journal, May 2005
- Kanai, Tsuneto; Minemoto, Shinichirou; Sakai, Hirofumi
- Nature, Vol. 435, Issue 7041
Isotope detection in molecules with ultrafast electron diffraction and rotational spectrometry
journal, May 2022
- Xiong, Yanwei; Zhao, Haoran; Saha, Sajib Kumar
- Journal of Physics Communications, Vol. 6, Issue 5
Field-free molecular alignment for studies using x-ray pulses from a synchrotron radiation source
journal, April 2009
- Ho, Phay J.; Miller, Michelle R.; Santra, Robin
- The Journal of Chemical Physics, Vol. 130, Issue 15
Harmonic generation by molecules in intense laser and magnetic fields: Orientation effects
journal, June 2004
- Bandrauk, André D.; Lu, Huizhong
- International Journal of Quantum Chemistry, Vol. 99, Issue 4
Time-Resolved Photoelectron Angular Distributions from Strong-Field Ionization of Rotating Naphthalene Molecules
journal, February 2011
- Hansen, Jonas L.; Stapelfeldt, Henrik; Dimitrovski, Darko
- Physical Review Letters, Vol. 106, Issue 7
High current table-top setup for femtosecond gas electron diffraction
journal, July 2017
- Zandi, Omid; Wilkin, Kyle J.; Xiong, Yanwei
- Structural Dynamics, Vol. 4, Issue 4
Alignment-Dependent Strong Field Ionization of Molecules
journal, June 2003
- Litvinyuk, I. V.; Lee, Kevin F.; Dooley, P. W.
- Physical Review Letters, Vol. 90, Issue 23
Angle-dependent strong-field ionization and fragmentation of carbon dioxide measured using rotational wave packets
journal, October 2020
- Lam, Huynh Van Sa; Yarlagadda, Suresh; Venkatachalam, Anbu
- Physical Review A, Vol. 102, Issue 4
Tomographic imaging of molecular orbitals
journal, December 2004
- Itatani, J.; Levesque, J.; Zeidler, D.
- Nature, Vol. 432, Issue 7019
Spatiotemporal rotational dynamics of laser-driven molecules
journal, April 2020
- Lin, Kang; Tutunnikov, Ilia; Ma, Junyang
- Advanced Photonics, Vol. 2, Issue 02
Direct imaging of rotational wave-packet dynamics of diatomic molecules
journal, August 2003
- Dooley, P. W.; Litvinyuk, I. V.; Lee, Kevin F.
- Physical Review A, Vol. 68, Issue 2
3. Inconsistent systems of linear equations
journal, October 1979
- Planitz, M.
- The Mathematical Gazette, Vol. 63, Issue 425
Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene
journal, October 2016
- Wolter, B.; Pullen, M. G.; Le, A. -T.
- Science, Vol. 354, Issue 6310
Ultrafast isolated molecule imaging without crystallization
journal, April 2022
- Ma, Zhuoran; Zou, Xiao; Zhao, Lingrong
- Proceedings of the National Academy of Sciences, Vol. 119, Issue 15
An x-ray probe of laser-aligned molecules
journal, March 2008
- Peterson, E. R.; Buth, C.; Arms, D. A.
- Applied Physics Letters, Vol. 92, Issue 9
Controlling the Branching Ratio of Photodissociation Using Aligned Molecules
journal, August 1999
- Larsen, Jakob Juul; Wendt-Larsen, Ida; Stapelfeldt, Henrik
- Physical Review Letters, Vol. 83, Issue 6
Quantum control of molecular rotation
journal, September 2019
- Koch, Christiane P.; Lemeshko, Mikhail; Sugny, Dominique
- Reviews of Modern Physics, Vol. 91, Issue 3
Rotational excitation and molecular alignment in intense laser fields
journal, November 1995
- Seideman, Tamar
- The Journal of Chemical Physics, Vol. 103, Issue 18
Imaging of Isolated Molecules with Ultrafast Electron Pulses
journal, September 2012
- Hensley, Christopher J.; Yang, Jie; Centurion, Martin
- Physical Review Letters, Vol. 109, Issue 13
Dynamic Stark Control of Torsional Motion by a Pair of Laser Pulses
journal, August 2014
- Christensen, Lauge; Nielsen, Jens H.; Brandt, Christian B.
- Physical Review Letters, Vol. 113, Issue 7
Time-resolved photoelectron angular distributions as a means of studying polyatomic nonadiabatic dynamics
journal, August 2000
- Seideman, Tamar
- The Journal of Chemical Physics, Vol. 113, Issue 5
Theory of retrieving orientation-resolved molecular information using time-domain rotational coherence spectroscopy
journal, August 2017
- Wang, Xu; Le, Anh-Thu; Zhou, Zhaoyan
- Physical Review A, Vol. 96, Issue 2
X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
journal, February 2014
- Küpper, Jochen; Stern, Stephan; Holmegaard, Lotte
- Physical Review Letters, Vol. 112, Issue 8
Imaging of alignment and structural changes of carbon disulfide molecules using ultrafast electron diffraction
journal, September 2015
- Yang, Jie; Beck, Joshua; Uiterwaal, Cornelis J.
- Nature Communications, Vol. 6, Issue 1
Rotational Raman spectroscopy of ethylene using a femtosecond time-resolved pump-probe technique
journal, October 2005
- Rouzée, A.; Boudon, V.; Lavorel, B.
- The Journal of Chemical Physics, Vol. 123, Issue 15
High-Order Harmonic Generation in Aligned Molecules
journal, October 2001
- Velotta, R.; Hay, N.; Mason, M. B.
- Physical Review Letters, Vol. 87, Issue 18
Aligning molecules with intense nonresonant laser fields
journal, November 1999
- Larsen, Jakob Juul; Sakai, Hirofumi; Safvan, C. P.
- The Journal of Chemical Physics, Vol. 111, Issue 17
Alignment and Trapping of Molecules in Intense Laser Fields
journal, June 1995
- Friedrich, Bretislav; Herschbach, Dudley
- Physical Review Letters, Vol. 74, Issue 23
Laser Control of Chemical Reactions
journal, March 1998
- Zare, Richard N.
- Science, Vol. 279, Issue 5358, p. 1875-1879
Evaluation of the rotation matrices in the basis of real spherical harmonics
journal, December 1997
- Blanco, Miguel A.; Flórez, M.; Bermejo, M.
- Journal of Molecular Structure: THEOCHEM, Vol. 419, Issue 1-3
Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera
journal, May 2015
- Slater, Craig S.; Blake, Sophie; Brouard, Mark
- Physical Review A, Vol. 91, Issue 5
Manipulation of molecules with electromagnetic fields
journal, June 2013
- Lemeshko, Mikhail; Krems, Roman V.; Doyle, John M.
- Molecular Physics, Vol. 111, Issue 12-13
Resonant structures in the low-energy electron continuum for single ionization of atoms in the tunnelling regime
journal, December 2004
- Rudenko, A.; Zrost, K.; Schröter, C. D.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 37, Issue 24
Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses
journal, April 2016
- Yang, Jie; Guehr, Markus; Vecchione, Theodore
- Nature Communications, Vol. 7, Issue 1
Ultrafast optical imaging by molecular wakes
journal, October 2010
- Wu, Jian; Lu, Peifen; Liu, Jia
- Applied Physics Letters, Vol. 97, Issue 16
Time-resolved photoelectron angular distributions as a probe of coupled polyatomic dynamics
journal, September 2001
- Seideman, Tamar
- Physical Review A, Vol. 64, Issue 4
High-resolution movies of molecular rotational dynamics captured with ultrafast electron diffraction
journal, October 2020
- Xiong, Yanwei; Wilkin, Kyle J.; Centurion, Martin
- Physical Review Research, Vol. 2, Issue 4
Phase Modulation of Ultrashort Light Pulses using Molecular Rotational Wave Packets
journal, December 2001
- Bartels, R. A.; Weinacht, T. C.; Wagner, N.
- Physical Review Letters, Vol. 88, Issue 1
A portable thermoelectric-power-generating module composed of oxide devices
journal, March 2006
- Funahashi, R.; Mikami, M.; Mihara, T.
- Journal of Applied Physics, Vol. 99, Issue 6
Phase Control of Rotational Wave Packets and Quantum Information
journal, November 2004
- Lee, Kevin F.; Villeneuve, D. M.; Corkum, P. B.
- Physical Review Letters, Vol. 93, Issue 23
Quantum state tomography of molecules by ultrafast diffraction
journal, September 2021
- Zhang, Ming; Zhang, Shuqiao; Xiong, Yanwei
- Nature Communications, Vol. 12, Issue 1
Coherent rotational excitation by intense nonresonant laser fields
journal, September 2010
- Ohshima, Yasuhiro; Hasegawa, Hirokazu
- International Reviews in Physical Chemistry, Vol. 29, Issue 4
Time-resolved imaging of purely valence-electron dynamics during a chemical reaction
journal, April 2011
- Hockett, Paul; Bisgaard, Christer Z.; Clarkin, Owen J.
- Nature Physics, Vol. 7, Issue 8
High-order harmonic generation in laser-aligned molecules
journal, April 2002
- Hay, N.; Velotta, R.; Lein, M.
- Physical Review A, Vol. 65, Issue 5