Non-Markovian stochastic Schrödinger equation at finite temperatures for charge carrier dynamics in organic crystals

Zhong, Xinxin; Zhao, Yi

doi:10.1063/1.4773319

Cited by 65 publications

(84 citation statements)

References 63 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Numerical simulations have demonstrated that the approach indeed correctly predicts the carrier dynamics for symmetric systems, but it gives out incorrect long time dynamics for asymmetric systems. [27] To investigate the carrier transport in asymmetric systems, we consider molecular vibrational motions quantum mechanically, and propose a mTDWPD method satisfying the detailed balance principle. To do it, we write the phonon Hamiltonian Eq.…”

Section: The Mtdpwd Methodsmentioning

confidence: 99%

See 1 more Smart Citation

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

Han

Zhong

et al. 2014

Int J of Quantum Chemistry

Self Cite

View full text Add to dashboard Cite

Although the carriers in organic semiconductors commonly follow the hopping-type motions caused by strong carrierphonon interactions, they can also present a band-like behavior in well-performed organic crystals. In this article, we review a unified model to describe the carrier dynamics covering from the hopping-type to band-like motions, the timedependent wavepacket diffusion method proposed in our group recently. In the method, the effects of vibrational motions of organic molecules and inter or intramolecular electronic couplings are considered as the fluctuations to the carrier dynamics. Numerical simulations demonstrate that the computational cost of present method is similar to that of mixed quantum-classical methods, but it overcomes the deficiency in those methods that the detailed balance principle is not satisfied. We further present how to combine electronic structure calculations and molecular dynamics simulations with the present model to reveal the carrier dynamics in realistic organic semiconductors.

show abstract

Section: The Mtdpwd Methodsmentioning

confidence: 99%

“…Recently, we have proposed a time-dependent wavepacket diffusion (TDWPD) method to describe the carrier dynamics [26][27][28][29] in organic semiconductors, which essentially incorporates the coherence and tunneling effects, and can be applied to large systems. In this article, we overview the TDWPD method and its applications.…”

Section: Introductionmentioning

confidence: 99%

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

Han

Zhong

et al. 2014

Int J of Quantum Chemistry

Self Cite

View full text Add to dashboard Cite

show abstract

“…This may be ascribed to vibrational progressions [48]. However, it lies outside the scope of this letter to incorporate the vibrational degrees of freedom into the absorption spectra.To investigate the quantum dynamics of the Frenkel-CT excitons in the DNTT, we apply the stochastic Schrödinger equation formulated by Zhao and coworkers [62][63][64][65]. In this formalism, time evolution of an excitonic wave function coupled to a phonon bath is obtained as follows:…”

mentioning

confidence: 99%

“…To investigate the quantum dynamics of the Frenkel-CT excitons in the DNTT, we apply the stochastic Schrödinger equation formulated by Zhao and coworkers [62][63][64][65]. In this formalism, time evolution of an excitonic wave function coupled to a phonon bath is obtained as follows:…”

mentioning

confidence: 99%

“…Here effects of the phonon bath are incorporated through a stochastic force u n (t) and a zerotemperature bath correlation function C (0) n (t). Both of them are calculated from a spectral density j n (ω) for the nth diabatic state [62,65]. The spectral densities [66,67] have been obtained by combing molecular dynamics simulations for the DNTT crystal with excited-state calculations using time-dependent density functional theory at B3LYP/6-31G* level.…”

mentioning

confidence: 99%

See 1 more Smart Citation

Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3-b:2′3′-f]thieno[3,2-b]-thiophene Thin Films: The Importance of Hole Delocalization

Fujita

Atahan-Evrenk

Sawaya

et al. 2016

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

Charge transfer states in organic semiconductors play crucial roles in processes such as singlet fission and exciton dissociation at donor/acceptor interfaces. Recently, a time-resolved spectroscopy study of dinaphtho [2,3-b:2 ′ 3 ′ -f]thieno[3,2-b]-thiophene (DNTT) thin films provided evidence for the formation of mixed Frenkel and charge-transfer excitons after the photoexcitation. Here we investigate optical properties and excitation dynamics of the DNTT thin films by combining ab initio calculations and a stochastic Schrödinger equation. Our theory predicts that the low-energy Frenkel exciton band consists of 8 to 47% CT character. The quantum dynamics simulations show coherent dynamics of Frenkel and CT states in 50 fs after the optical excitation. We demonstrate the role of charge delocalization and localization in the mixing of CT states with Frenkel excitons as well as the role of their decoherence.Organic semiconductors (OSCs) are widely investigated as candidates for inexpensive and flexible materials for photovoltaics and other optoelectronic applications. [1][2][3]. In recent years, new OSCs have been designed and improved through computational modeling [4][5][6] and virtual high-throughput screening [7][8][9]. Modeling energy and charge transport properties is also essential for understanding structure-property relationships and thus for rationally designing novel OSCs [10][11][12][13][14][15][16].The low-energy optical excitations in OSCs lead to the formation of a bound electron-hole (e-h) pair, a Frenkel exciton. Excitonic properties of organic crystals are substantially different from those of isolated molecules, owing to excitonic couplings, near-field interactions between electronic transitions [17][18][19][20]. Interactions with a charge-transfer (CT) statea state in which the electron and hole are located on spatially separated regions-can also affect the optical properties of an exciton, as has been demonstrated by several theoretical studies [21][22][23][24][25][26]. Experimentally, the degree of CT character has been studied by momentum-dependent electron-loss spectroscopy [27][28][29] or electroabsorption spectroscopy [30][31][32]. CT states can act as precursors for interfacial CT states [33][34][35]; mixing of CT states with Frenkel excitons would facilitate charge separation in photovoltaic materials. They have also gained recent attention due to their relevance to singlet fission [36][37][38], in which singlet to triplet conversion can proceed via sequential CT steps [39][40][41].Here we focus on dinaphtho[2,3-b:, a p-type OSC originally introduced by Takimiya and co-workers [42]. DNTT and its derivatives [5,[43][44][45][46][47][48][49] have gained attention due to their high hole mobility values and air stability. A recent time-resolved spectroscopy study by Ishino et al. [48] concludes that mixed Frenkel and CT excitons are formed after the optical excitation. Although the degree of CT character in excited states has been reported as described in the earlier paragraph, its role in...

show abstract

Modeling the Photophysical Processes of Organic Molecular Aggregates with Inclusion of Intermolecular Interactions and Vibronic Couplings

Liang,

Wang,

Feng

et al. 2024

Exploring Chemical Concepts Through Theory and Computation

View full text Add to dashboard Cite

Non-Markovian stochastic Schrödinger equation at finite temperatures for charge carrier dynamics in organic crystals

Cited by 65 publications

References 63 publications

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

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

Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3-b:2′3′-f]thieno[3,2-b]-thiophene Thin Films: The Importance of Hole Delocalization

Modeling the Photophysical Processes of Organic Molecular Aggregates with Inclusion of Intermolecular Interactions and Vibronic Couplings

Contact Info

Product

Resources

About