Stochastic multi-configuration time-dependent Hartree for dissipative quantum dynamics with strong intramolecular coupling

Mandal, Souvik; Gatti, Fabien; Bindech, Oussama; Marquardt, Roberto; Tremblay, Jean Christophe

doi:10.1063/5.0105308

Cited by 5 publications

(1 citation statement)

References 53 publications

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“…However, it is not clear whether the thermalization is treated on an equal foot in wave packet with initial time average and in the open quantum system. Noise could also be introduced in a stochastic time-dependent Schrödinger equation with an improved treatment of the thermalization [104].…”

Section: Discussionmentioning

confidence: 99%

Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control

et al. 2022

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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 that 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 sequence of pulses on the optimal field. The overall result is efficient and robust disymmetry control over reasonable time scales 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 (TT) representation with propagation using the time dependent variational method.

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Section: Discussionmentioning

confidence: 99%

Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control

et al. 2022

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Open quantum dynamics of strongly coupled oscillators with multi-configuration time-dependent Hartree propagation and Markovian quantum jumps

Triana

Herrera

2022

The Journal of Chemical Physics

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Modeling the non-equilibrium dissipative dynamics of strongly interacting quantized degrees of freedom is a fundamental problem in several branches of physics and chemistry. We implement a quantum state trajectory scheme for solving Lindblad quantum master equations that describe coherent and dissipative processes for a set of strongly-coupled quantized oscillators. The scheme involves a sequence of stochastic quantum jumps with transition probabilities determined the system state and the system-reservoir dynamics. Between consecutive jumps, the wavefunction is propagated in coordinate space using the multi-configuration time-dependent Hartree (MCTDH) method. We compare this hybrid propagation methodology with exact Liouville space solutions for physical systems of interest in cavity quantum electrodynamics, demonstrating accurate results for experimentally relevant observables using a tractable number of quantum trajectories. We show the potential for solving the dissipative dynamics of finite size arrays of strongly interacting quantized oscillators with high excitation densities, a scenario that is challenging for conventional density matrix propagators due to the large dimensionality of the underlying Hilbert space.

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Coupling polyatomic molecules to lossy nanocavities: Lindblad vs Schrödinger description

Fábri,

Császár,

Halász

et al. 2024

The Journal of Chemical Physics

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The use of cavities to impact molecular structure and dynamics has become popular. As cavities, in particular plasmonic nanocavities, are lossy and the lifetime of their modes can be very short, their lossy nature must be incorporated into the calculations. The Lindblad master equation is commonly considered an appropriate tool to describe this lossy nature. This approach requires the dynamics of the density operator and is thus substantially more costly than approaches employing the Schrödinger equation for the quantum wave function when several or many nuclear degrees of freedom are involved. In this work, we compare numerically the Lindblad and Schrödinger descriptions discussed in the literature for a molecular example where the cavity is pumped by a laser. The laser and cavity properties are varied over a range of parameters. It is found that the Schrödinger description adequately describes the dynamics of the polaritons and emission signal as long as the laser intensity is moderate and the pump time is not much longer than the lifetime of the cavity mode. Otherwise, it is demonstrated that the Schrödinger description gradually fails. We also show that the failure of the Schrödinger description can often be remedied by renormalizing the wave function at every step of time propagation. The results are discussed and analyzed.

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Stochastic multi-configuration time-dependent Hartree for dissipative quantum dynamics with strong intramolecular coupling

Cited by 5 publications

References 53 publications

Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control

Laser-controlled electronic symmetry breaking in a phenylene ethynylene dimer: Simulation by the hierarchical equations of motion and optimal control

Open quantum dynamics of strongly coupled oscillators with multi-configuration time-dependent Hartree propagation and Markovian quantum jumps

Coupling polyatomic molecules to lossy nanocavities: Lindblad vs Schrödinger description

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