Time-Dependent Complete-Active-Space Self-Consistent-Field Method for Ultrafast Intense Laser Science

  • Takeshi Sato
  • Yuki Orimo
  • Takuma Teramura
  • Oyunbileg Tugs
  • Kenichi L. IshikawaEmail author
Part of the Springer Series in Chemical Physics book series (CHEMICAL, volume 118)


We present the time-dependent complete-active-space self-consistent-field (TD-CASSCF) method to simulate multielectron dynamics in ultrafast intense laser fields from the first principles. While based on multiconfiguration expansion, it divides the orbital space into frozen-core (tightly bound electrons with no response to the field), dynamical-core (electrons tightly bound but responding to the field), and active (fully correlated to describe highly excited and ejected electrons) orbital subspaces. The subspace decomposition can be done flexibly, conforming to phenomena under investigation and desired accuracy. The method is gauge invariant and size extensive. Infinite-range exterior complex scaling in addition to mask-function boundary is adopted as an efficient absorbing boundary. We show numerical examples and illustrate how to extract relevant physical quantities such as ionization yield, high-harmonic spectrum, and photoelectron spectrum from our full-dimensional implementation for atoms. The TD-CASSCF method will open a way to the ab initio simulation study of ultrafast intense laser science in realistic atoms and molecules.



This research was supported in part by a Grant-in-Aid for Scientific Research (Grants No. 23750007, No. 23656043, No. 23104708, No. 25286064, No. 26390076, No. 26600111, No. 16H03881, and 17K05070) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan and also by the Photon Frontier Network Program of MEXT. This research was also partially supported by the Center of Innovation Program from the Japan Science and Technology Agency, JST, and by CREST (Grant No. JPMJCR15N1), JST. Y. O. gratefully acknowledges support from the Graduate School of Engineering, The University of Tokyo, Doctoral Student Special Incentives Program (SEUT Fellowship). O. T. gratefully acknowledges support from the Japanese Government (MEXT) Scholarship. We thank I. Březinová, F. Lackner, S. Nagele, J. Burgdörfer, and A. Scrinzi for fruitful collaborations that have greatly contributed to this work.


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Copyright information

© Springer Nature Switzerland AG 2018

Authors and Affiliations

  • Takeshi Sato
    • 1
  • Yuki Orimo
    • 1
  • Takuma Teramura
    • 1
  • Oyunbileg Tugs
    • 1
  • Kenichi L. Ishikawa
    • 1
    Email author
  1. 1.Department of Nuclear Engineering and Management, Graduate School of EngineeringThe University of TokyoBunkyo-kuJapan

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