Time‐dependent wavepacket diffusion method and its applications in organic semiconductors

Han, Lu; Ke, Yaling; Zhong, Xinxin; Zhao, Yi

doi:10.1002/qua.24833

Cited by 16 publications

(20 citation statements)

References 69 publications

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“…(14) can correctly predict exact carrier dynamics for most of realistic organic aggregates. [53][54][55][56][57][58] F α,β (t) is the so-called stochastic force in numerical simulations as we take α and β as random variables, it is generated by the following expression…”

Section: Acs Paragon Plus Environmentmentioning

confidence: 99%

Effects of Charge Transfer State and Exciton Migration on Singlet Fission Dynamics in Organic Aggregates

Zang

Zhao

et al. 2016

J. Phys. Chem. C

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A time-dependent wavepacket diffusion method is used to investigate the effects of charge transfer (CT) states, singlet exciton and multiexciton migrations on singlet fission (SF) dynamics in organic aggregates. The results reveal that the incorporation of CT states can result in a different SF dynamics from the direct interaction between singlet exciton and multiexciton, and an obvious SF interference is also observed between the direct channel and the indirect channel mediated by CT states. In the case of direct interaction, although the fast population transfer of singlet exciton in monomers, by the increase of exciton-exciton interaction, can accelerate the SF process, the spatial coherence alternatively has a counter-productive effect, and their competition leads to an optimal exciton-exciton interaction at which SF has a maximal rate. This trade-off relationship in SF dynamics is further analysed from different perspectives, specifically in spatial and energy representations, is also confirmed through the indication that static energy disorders can speed up SF process by destructing the coherence.Meanwhile, it is found that the couplings among multiexciton states decrease SF rates by the multiexciton coherence and backward conversion from multiexciton to singlet exciton states.

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Section: Acs Paragon Plus Environmentmentioning

confidence: 99%

Effects of Charge Transfer State and Exciton Migration on Singlet Fission Dynamics in Organic Aggregates

Zang

Zhao

et al. 2016

J. Phys. Chem. C

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“…In this work, we will demonstrate that SF rates can be also dramatically affected by H- and J-aggregates via quantum interference and subsequently show how to manipulate SF dynamics through tuning the packing of aggregates. The effect of electron–phonon interaction on the interference is further investigated by using the time-dependent wavepacket diffusion (TDWPD) method. − Finally, we choose a pentacene dimer as a concrete example to control the quantum interferences in SF dynamics by using different packing arrangements.…”

mentioning

confidence: 99%

Quantum Interference in Singlet Fission: J- and H-Aggregate Behavior

Zang

Zhao

Liang

2017

J. Phys. Chem. Lett.

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The quantum interference in singlet fission (SF) among the multiple pathways from singlet excited states to correlated triplet pair states is comprehensively investigated. The analytical analysis reveals that this interference is strongly affected by the exciton-exciton coupling and is closely related to the property of J- and H-type of aggregates. Different from the interference in the spectra of aggregates, which depends only on the sign of exciton-exciton coupling, the interference in SF is additionally related to the signs of couplings between singlet excited states and triplet pair states. The interference dynamics is further demonstrated numerically by a time-dependent wavepacket diffusion method with electron-phonon interactions incorporated. Finally, we take a pentacene dimer as a concrete example to show how to adjust the constructive and destructive interferences in SF dynamics in terms of J-/H-aggregate behaviors. The results presented here may provide guiding principles for designing efficient SF materials through directly tuning quantum interference via morphology engineering.

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“…Previously, due to the lack of knowledge of the full coupling Hamiltonian, the first problem has been addressed by investigating the effect of successive elimination of vibrational degrees of freedom in order to identify the relevant modes 11,12 . To accomplish a faithful simulation of the quantum dynamics following the light excitation, a variety of methods has been applied, including multi-configurational time-dependent Hartree (MCTDH) [23][24][25] , Redfield theory 26,27 and time-dependent wave packet diffusion (TDWPD) 28 . However, despite numerous investigations, there has been few numerically unbiased simulations of a full microscopic Hamiltonian that is generated from first principles for both, electronic molecular and vibronic degrees of freedom 12,29 .…”

Section: Introductionmentioning

confidence: 99%

Quantum dynamics simulation of intramolecular singlet fission in covalently linked tetracene dimer

Mardazad,

Xu,

Yang

et al. 2021

Preprint

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In this work we study singlet fission in tetracene para-dimers, covalently linked by a phenyl group. In contrast to most previous works, we account for the full quantum dynamics of the combined excitonic and vibrational system. For our simulations we choose a numerically unbiased representation of the molecule's wave function enabling us to compare with experiments, exhibiting good agreement. Having access to the full wave function allows us to study in detail the post-quench dynamics of the excitons. Here, one of our main findings is the identification of a time scale t 0 ≈ 35 fs dominated by coherent dynamics.It is within this time scale that the larger fraction of the singlet fission yield is generated.We also report on a reduced number of phononic modes that play a crucial role for the energy transfer between excitonic and vibrational system. Notably, the oscillation frequency of these modes coincides with the observed electronic coherence time t 0 . We extend our investigations by also studying the dependency of the dynamics on the excitonic energy levels that, for instance, can be experimentally tuned by means of the solvent polarity.Here, our findings indicate that the singlet fission yield can be doubled while the electronic coherence time t 0 is mainly unaffected.

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Time‐dependent wavepacket diffusion method and its applications in organic semiconductors

Cited by 16 publications

References 69 publications

Effects of Charge Transfer State and Exciton Migration on Singlet Fission Dynamics in Organic Aggregates

Effects of Charge Transfer State and Exciton Migration on Singlet Fission Dynamics in Organic Aggregates

Quantum Interference in Singlet Fission: J- and H-Aggregate Behavior

Quantum dynamics simulation of intramolecular singlet fission in covalently linked tetracene dimer

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