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Communication: Time-dependent optimized coupled-cluster method for multielectron dynamics.

Takeshi Sato1, Himadri Pathak2, Yuki Orimo2

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|February 10, 2018
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Summary
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A new time-dependent optimized coupled-cluster (TD-OCC) method models multielectron dynamics under intense laser fields. This accurate and efficient approach is applied to argon atoms, advancing computational chemistry for laser-matter interactions.

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Area of Science:

  • Computational Quantum Chemistry
  • Theoretical Chemistry
  • Laser-Matter Interactions

Background:

  • Accurate modeling of multielectron dynamics in intense laser fields is crucial for understanding atomic and molecular responses.
  • Existing methods like time-dependent multiconfiguration self-consistent-field (TD-MCSCF) can be computationally expensive.
  • Need for efficient and accurate theoretical frameworks to simulate quantum dynamics under extreme conditions.

Purpose of the Study:

  • To formulate and implement a novel time-dependent optimized coupled-cluster (TD-OCC) method.
  • To enable accurate simulations of multielectron dynamics driven by intense laser fields.
  • To provide a computationally feasible alternative to existing methods for studying laser-driven electron dynamics.

Main Methods:

  • Derivation of equations of motion for cluster amplitudes and optimized orbital functions using a real action functional.
  • Implementation of the TD-OCC method, including variants with double (TD-OCCD) and double-triple (TD-OCCDT) excitations.
  • Utilized optimized active orbitals for computational efficiency and accuracy.

Main Results:

  • Successful formulation and implementation of the TD-OCC method for time-dependent quantum dynamics.
  • Demonstrated that the TD-OCC method is size-extensive and gauge-invariant.
  • Reported the first application of TD-OCC to simulate intense-laser driven correlated electron dynamics in an Argon atom.

Conclusions:

  • The developed TD-OCC method offers a size-extensive and gauge-invariant approach for simulating electron dynamics in intense laser fields.
  • TD-OCC presents a polynomial cost-scaling alternative to TD-MCSCF, making complex quantum dynamics simulations more accessible.
  • The successful application to Argon demonstrates the potential of TD-OCC for advancing research in laser-driven atomic and molecular physics.