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• W4307888977 abstract "The ability to prepare a specific superposition of electronic excited states leading to a transitory symmetry breaking of the electronic density in complex systems remains a challenging concern. We investigate how an initial coherence can be controlled by laser fields. The selected molecular system is a symmetric dimer of phenylene ethynylene presenting different interesting properties: Two bright nearly degenerate excited states coupled through a conical intersection are addressable by orthogonal transition dipole moments and are well separated from neighboring states. Creating a superposed state with equal weights corresponds to a right or left electronic localization as in the double-well system followed by a transitory oscillation between the two wells. To ensure a spectral bandwidth typically smaller than 0.25 eV, the pulse duration is in the tens of femtoseconds range, so nuclear motion cannot be neglected. Optimal control theory (OCT) is applied with guess fields that effectively create the target coherence in the absence of dephasing due to the vibrational baths. We analyze the field reshaping proposed by the control and we further fit a sequence of pulses on the optimal field. The overall result is efficient and robust disymmetry control over reasonable timescales of few tens of femtoseconds, exceeding the pulse duration. The monotonically convergent algorithm is combined with the hierarchical equations of motion (HEOM) able to treat strongly coupled non-Markovian dynamics. We also check the implementation of the combined OCT-HEOM approach in the tensor-train representation with propagation using the time-dependent variational method." @default.
• W4307888977 created "2022-11-06" @default.
• W4307888977 creator A5026931035 @default.
• W4307888977 creator A5030294205 @default.
• W4307888977 creator A5039443212 @default.
• W4307888977 creator A5048686698 @default.
• W4307888977 creator A5079315778 @default.
• W4307888977 creator A5088311318 @default.
• W4307888977 date "2022-10-31" @default.
• W4307888977 modified "2023-09-23" @default.
• W4307888977 title "Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control" @default.
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