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Title: 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:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. 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


Laser-Induced Coulomb Explosion Imaging of Aligned Molecules and Molecular Dimers
journal, April 2022


Experimental Observation of Revival Structures in Picosecond Laser-Induced Alignment of I2
journal, September 2001


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
  • DOI: 10.1002/ijch.201100161

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
  • DOI: 10.1039/D0FD00125B

Femtosecond gas phase electron diffraction with MeV electrons
journal, January 2016

  • Yang, Jie; Guehr, Markus; Vecchione, Theodore
  • Faraday Discussions, Vol. 194
  • DOI: 10.1039/C6FD00071A

Generalized molecular orbital tomography
journal, June 2011

  • Vozzi, C.; Negro, M.; Calegari, F.
  • Nature Physics, Vol. 7, Issue 10
  • DOI: 10.1038/nphys2029

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
  • DOI: 10.1088/1361-6455/ac135f

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
  • DOI: 10.1063/1.2388273

Tilted femtosecond pulses for velocity matching in gas-phase ultrafast electron diffraction
journal, August 2014


Alignment of symmetric top molecules by short laser pulses
journal, October 2005


Nonadiabatic laser-induced alignment of iodobenzene molecules
journal, December 2004


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
  • DOI: 10.1063/1.1489901

Colloquium : Aligning molecules with strong laser pulses
journal, April 2003


Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules
journal, March 2009


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
  • DOI: 10.1063/1.4812787

Role of orbital symmetry in high-order harmonic generation from aligned molecules
journal, March 2004


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
  • DOI: 10.1038/s41467-019-11122-y

Manipulating the Torsion of Molecules by Strong Laser Pulses
journal, February 2009


Quantum interference during high-order harmonic generation from aligned molecules
journal, May 2005

  • Kanai, Tsuneto; Minemoto, Shinichirou; Sakai, Hirofumi
  • Nature, Vol. 435, Issue 7041
  • DOI: 10.1038/nature03577

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
  • DOI: 10.1088/2399-6528/ac6aaf

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
  • DOI: 10.1063/1.3120608

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
  • DOI: 10.1002/qua.20039

Time-Resolved Photoelectron Angular Distributions from Strong-Field Ionization of Rotating Naphthalene Molecules
journal, February 2011


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
  • DOI: 10.1063/1.4983225

Alignment-Dependent Strong Field Ionization of Molecules
journal, June 2003


Angle-dependent strong-field ionization and fragmentation of carbon dioxide measured using rotational wave packets
journal, October 2020


Tomographic imaging of molecular orbitals
journal, December 2004


Spatiotemporal rotational dynamics of laser-driven molecules
journal, April 2020


Direct imaging of rotational wave-packet dynamics of diatomic molecules
journal, August 2003


3. Inconsistent systems of linear equations
journal, October 1979

  • Planitz, M.
  • The Mathematical Gazette, Vol. 63, Issue 425
  • DOI: 10.2307/3617890

Ultrafast electron diffraction imaging of bond breaking in di-ionized acetylene
journal, October 2016


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
  • DOI: 10.1073/pnas.2122793119

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
  • DOI: 10.1063/1.2890846

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
  • DOI: 10.1103/PhysRevLett.83.1123

Quantum control of molecular rotation
journal, September 2019


Rotational excitation and molecular alignment in intense laser fields
journal, November 1995

  • Seideman, Tamar
  • The Journal of Chemical Physics, Vol. 103, Issue 18
  • DOI: 10.1063/1.470206

Imaging of Isolated Molecules with Ultrafast Electron Pulses
journal, September 2012


Dynamic Stark Control of Torsional Motion by a Pair of Laser Pulses
journal, August 2014


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
  • DOI: 10.1063/1.481968

Theory of retrieving orientation-resolved molecular information using time-domain rotational coherence spectroscopy
journal, August 2017


X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
journal, February 2014


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
  • DOI: 10.1038/ncomms9172

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
  • DOI: 10.1063/1.2069866

High-Order Harmonic Generation in Aligned Molecules
journal, October 2001


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
  • DOI: 10.1063/1.480112

Alignment and Trapping of Molecules in Intense Laser Fields
journal, June 1995


Laser Control of Chemical Reactions
journal, March 1998


Evaluation of the rotation matrices in the basis of real spherical harmonics
journal, December 1997


Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera
journal, May 2015


Manipulation of molecules with electromagnetic fields
journal, June 2013


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
  • DOI: 10.1088/0953-4075/37/24/L03

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
  • DOI: 10.1038/ncomms11232

Ultrafast optical imaging by molecular wakes
journal, October 2010

  • Wu, Jian; Lu, Peifen; Liu, Jia
  • Applied Physics Letters, Vol. 97, Issue 16
  • DOI: 10.1063/1.3505138

Time-resolved photoelectron angular distributions as a probe of coupled polyatomic dynamics
journal, September 2001


High-resolution movies of molecular rotational dynamics captured with ultrafast electron diffraction
journal, October 2020


Phase Modulation of Ultrashort Light Pulses using Molecular Rotational Wave Packets
journal, December 2001


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
  • DOI: 10.1063/1.2180449

Phase Control of Rotational Wave Packets and Quantum Information
journal, November 2004


Quantum state tomography of molecules by ultrafast diffraction
journal, September 2021


Coherent rotational excitation by intense nonresonant laser fields
journal, September 2010


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
  • DOI: 10.1038/nphys1980

High-order harmonic generation in laser-aligned molecules
journal, April 2002