Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules
Abstract
High-order harmonic signals generated in molecules are the consequence of coherent summation of complex laser-induced transition dipoles $$\textit{d}(θ, ω)$$ with each fixed-in-space molecule; here $$\theta$$ is the angle of the molecular axis with respect to the laser polarization axis and $$\omega$$ is the harmonic energy. In the so-called rotational coherent spectroscopy, it is proposed to extract the fixed-in-space $$\textit{d}(θ, ω)$$ in the molecular frame by measuring harmonics generated by a probing laser from the rotational molecular wave packets that have been prepared by a prior pump laser. By varying the time delay between the two lasers, methods have been utilized to extract the $$\theta$$ dependence of both the amplitude and phase of each individual harmonic, but the relative phase between harmonics cannot be retrieved. Here we report that this limitation can be removed. It requires the additional measurement of harmonic spectra versus the pump-probe angles at one fixed time delay. The two-dimensional input harmonic data (time-delay and pump-probe angle) are then used to retrieve the full complex transition dipole $$\textit{d}(θ, ω)$$ using a retrieval method based on machine learning algorithms. Finally, we demonstrate this method on N2 and CO2 molecules.
- Authors:
-
- Huazhong Univ. of Science and Technology, Wuhan (China); Wuhan Institute of Technology (China)
- Huazhong Univ. of Science and Technology, Wuhan (China)
- Wuhan Institute of Technology (China)
- Publication Date:
- Research Org.:
- Kansas State Univ., Manhattan, KS (United States)
- Sponsoring Org.:
- National Key R&D Program; National Natural Science Foundation of China (NSFC); China Scholarship Council (CSC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1800612
- Grant/Contract Number:
- FG02-86ER13491
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review A
- Additional Journal Information:
- Journal Volume: 101; Journal Issue: 6; Journal ID: ISSN 2469-9926
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS; Optics; Physics
Citation Formats
Wang, Bincheng, He, Yanqing, Zhao, Xi, He, Lixin, Lan, Pengfei, Lu, Peixiang, and Lin, C. D. Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules. United States: N. p., 2020.
Web. doi:10.1103/physreva.101.063417.
Wang, Bincheng, He, Yanqing, Zhao, Xi, He, Lixin, Lan, Pengfei, Lu, Peixiang, & Lin, C. D. Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules. United States. https://doi.org/10.1103/physreva.101.063417
Wang, Bincheng, He, Yanqing, Zhao, Xi, He, Lixin, Lan, Pengfei, Lu, Peixiang, and Lin, C. D. Tue .
"Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules". United States. https://doi.org/10.1103/physreva.101.063417. https://www.osti.gov/servlets/purl/1800612.
@article{osti_1800612,
title = {Retrieval of full angular- and energy-dependent complex transition dipoles in the molecular frame from laser-induced high-order harmonic signals with aligned molecules},
author = {Wang, Bincheng and He, Yanqing and Zhao, Xi and He, Lixin and Lan, Pengfei and Lu, Peixiang and Lin, C. D.},
abstractNote = {High-order harmonic signals generated in molecules are the consequence of coherent summation of complex laser-induced transition dipoles $\textit{d}(θ, ω)$ with each fixed-in-space molecule; here $\theta$ is the angle of the molecular axis with respect to the laser polarization axis and $\omega$ is the harmonic energy. In the so-called rotational coherent spectroscopy, it is proposed to extract the fixed-in-space $\textit{d}(θ, ω)$ in the molecular frame by measuring harmonics generated by a probing laser from the rotational molecular wave packets that have been prepared by a prior pump laser. By varying the time delay between the two lasers, methods have been utilized to extract the $\theta$ dependence of both the amplitude and phase of each individual harmonic, but the relative phase between harmonics cannot be retrieved. Here we report that this limitation can be removed. It requires the additional measurement of harmonic spectra versus the pump-probe angles at one fixed time delay. The two-dimensional input harmonic data (time-delay and pump-probe angle) are then used to retrieve the full complex transition dipole $\textit{d}(θ, ω)$ using a retrieval method based on machine learning algorithms. Finally, we demonstrate this method on N2 and CO2 molecules.},
doi = {10.1103/physreva.101.063417},
journal = {Physical Review A},
number = 6,
volume = 101,
place = {United States},
year = {Tue Jun 30 00:00:00 EDT 2020},
month = {Tue Jun 30 00:00:00 EDT 2020}
}
Works referenced in this record:
Role of Rotational Wave Packets in Strong Field Experiments
journal, December 2013
- Weber, S. J.; Oppermann, M.; Marangos, J. P.
- Physical Review Letters, Vol. 111, Issue 26
Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry
journal, August 2017
- Marceau, Claude; Makhija, Varun; Platzer, Dominique
- Physical Review Letters, Vol. 119, Issue 8
Probing Molecular Frame Photoionization via Laser Generated High-Order Harmonics from Aligned Molecules
journal, May 2009
- Le, Anh-Thu; Lucchese, R. R.; Lee, M. T.
- Physical Review Letters, Vol. 102, Issue 20
Cooper minimum of high-order harmonic spectra from an MgO crystal in an ultrashort laser pulse
journal, March 2020
- Zhao, Yiting; Xu, Xiaoqin; Jiang, Shicheng
- Physical Review A, Vol. 101, Issue 3
Rotational coherence spectroscopy: studies of the geometries of large gas-phase species by picosecond time-domain methods
journal, October 1992
- Felker, Peter M.
- The Journal of Physical Chemistry, Vol. 96, Issue 20
Direct imaging of molecular rotation with high-order-harmonic generation
journal, May 2019
- He, Yanqing; He, Lixin; Lan, Pengfei
- Physical Review A, Vol. 99, Issue 5
Direct Measurement of the Angular Dependence of the Single-Photon Ionization of Aligned N 2 and CO 2 †
journal, October 2008
- Thomann, Isabell; Lock, Robynne; Sharma, Vandana
- The Journal of Physical Chemistry A, Vol. 112, Issue 39
Generalized molecular orbital tomography
journal, June 2011
- Vozzi, C.; Negro, M.; Calegari, F.
- Nature Physics, Vol. 7, Issue 10
Applications of B -splines in atomic and molecular physics
journal, November 2001
- Bachau, H.; Cormier, E.; Decleva, P.
- Reports on Progress in Physics, Vol. 64, Issue 12
Elements of the quantitative rescattering theory
journal, April 2018
- Lin, C. D.; Le, Anh-Thu; Jin, Cheng
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 51, Issue 10
High-harmonic spectroscopy of isoelectronic molecules: Wavelength scaling of electronic-structure and multielectron effects
journal, March 2013
- Rupenyan, A.; Kraus, P. M.; Schneider, J.
- Physical Review A, Vol. 87, Issue 3
Investigation of isolated attosecond pulse reconstruction from angular integrated photoelectron streaking spectra
journal, June 2020
- Zhao, Xi; Wei, Changli; Wang, Su-Ju
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 53, Issue 15
A new method for accurate retrieval of atomic dipole phase or photoionization group delay in attosecond photoelectron streaking experiments
journal, October 2017
- Zhao, Xi; Wei, Hui; Wei, Changli
- Journal of Optics, Vol. 19, Issue 11
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
Photoelectron Angular Distributions from O Shell of Oriented CO Molecules: A Critical Comparison between Theory and Experiment
journal, July 2000
- Ito, K.; Adachi, J.; Hikosaka, Y.
- Physical Review Letters, Vol. 85, Issue 1
Low Photon Count Phase Retrieval Using Deep Learning
journal, December 2018
- Goy, Alexandre; Arthur, Kwabena; Li, Shuai
- Physical Review Letters, Vol. 121, Issue 24
Role of the Intramolecular Phase in High-Harmonic Generation
journal, April 2002
- Lein, M.; Hay, N.; Velotta, R.
- Physical Review Letters, Vol. 88, Issue 18
Quantum interference during high-order harmonic generation from aligned molecules
journal, May 2005
- Kanai, Tsuneto; Minemoto, Shinichirou; Sakai, Hirofumi
- Nature, Vol. 435, Issue 7041
Channel- and Angle-Resolved Above Threshold Ionization in the Molecular Frame
journal, January 2013
- Mikosch, Jochen; Boguslavskiy, Andrey E.; Wilkinson, Iain
- Physical Review Letters, Vol. 110, Issue 2
Method for spectral phase retrieval of single attosecond pulses utilizing the autocorrelation of photoelectron streaking spectra
journal, March 2019
- Yu, Wei-Wei; Zhao, Xi; Wei, Hui
- Physical Review A, Vol. 99, Issue 3
Simulated Annealing: Theory and Applications
book, January 1987
- van Laarhoven, Peter J. M.; Aarts, Emile H. L.
- Springer Dordrecht
Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules
journal, April 2010
- Pabst, Stefan; Ho, Phay J.; Santra, Robin
- Physical Review A, Vol. 81, Issue 4
Field-Free Three Dimensional Molecular Axis Alignment
journal, April 2005
- Underwood, Jonathan G.; Sussman, Benjamin J.; Stolow, Albert
- Physical Review Letters, Vol. 94, Issue 14
Angle-dependent strong-field ionization of halomethanes
journal, November 2019
- Sándor, Péter; Sissay, Adonay; Mauger, François
- The Journal of Chemical Physics, Vol. 151, Issue 19
Measurement of molecular rotational temperature in a supersonic gas jet with high-order harmonic generation
journal, January 2009
- Yoshii, Kazumichi; Miyaji, Godai; Miyazaki, Kenzo
- Optics Letters, Vol. 34, Issue 11
Machine learning applications in genetics and genomics
journal, May 2015
- Libbrecht, Maxwell W.; Noble, William Stafford
- Nature Reviews Genetics, Vol. 16, Issue 6
Metrology of Time-Domain Soft X-Ray Attosecond Pulses and Reevaluation of Pulse Durations of Three Recent Experiments
journal, March 2020
- Zhao, Xi; Wang, Su-Ju; Yu, Wei-Wei
- Physical Review Applied, Vol. 13, Issue 3
Reconstruction of the complex angle-dependent photoionization transition dipole from a laser-dressed streaking experiment
journal, November 2018
- Zhao, Xi; Wei, Hui; Yu, Wei-Wei
- Physical Review A, Vol. 98, Issue 5
Tomographic imaging of molecular orbitals
journal, December 2004
- Itatani, J.; Levesque, J.; Zeidler, D.
- Nature, Vol. 432, Issue 7019
Quantitative rescattering theory for high-order harmonic generation from molecules
journal, July 2009
- Le, Anh-Thu; Lucchese, R. R.; Tonzani, S.
- Physical Review A, Vol. 80, Issue 1
Phase-retrieval algorithm for the characterization of broadband single attosecond pulses
journal, April 2017
- Zhao, Xi; Wei, Hui; Wu, Yan
- Physical Review A, Vol. 95, Issue 4
Field-free one-dimensional alignment of ethylene molecule
journal, March 2006
- Rouzée, A.; Guérin, S.; Boudon, V.
- Physical Review A, Vol. 73, Issue 3