Studies of polaron motion

Holstein, T.

doi:10.1016/0003-4916(59)90002-8

Cited by 3,078 publications

(1,247 citation statements)

References 0 publications

Supporting

Mentioning

1,165

Contrasting

Unclassified

Order By: Relevance

“…which describes a Holstein-like phonon 46 coupled to the charge density of the LUMO level. An external light field is used to promote an electron from the HOMO to the LUMO level.…”

Section: Donor-c60 Hamiltonianmentioning

confidence: 99%

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

et al. 2018

View full text Add to dashboard Cite

We use the Nonequilibrium Green's Function (NEGF) method to perform real-time simulations of the ultrafast electron dynamics of photoexcited donor-C60 complexes modeled by a Pariser-ParrPople Hamiltonian. The NEGF results are compared to mean-field Hartree-Fock (HF) calculations to disentangle the role of correlations. Initial benchmarking against numerically highly accurate time-dependent Density Matrix Renormalization Group calculations verifies the accuracy of NEGF. We then find that charge-transfer (CT) excitons partially decay into charge separated (CS) states if dynamical non-local correlation corrections are included. This CS process occurs in ∼ 10 fs after photoexcitation. In contrast, the probability of exciton recombination is almost 100% in HF simulations. These results are largely unaffected by nuclear vibrations; the latter become however essential whenever level misalignment hinders the CT process. The robust nature of our findings indicate that ultrafast CS driven by correlation-induced decoherence may occur in many organic nanoscale systems, but it will only be correctly predicted by theoretical treatments that include time-nonlocal correlations.

show abstract

“…which describes a Holstein-like phonon 46 coupled to the charge density of the LUMO level. An external light field is used to promote an electron from the HOMO to the LUMO level.…”

Section: Donor-c60 Hamiltonianmentioning

confidence: 99%

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

et al. 2018

View full text Add to dashboard Cite

show abstract

“…More recently, microscopic models from generalized master equation approach 15 , and dynamical mean-field theory 16 have been developed. Polaron transport theory developed by Holstein in his seminal work 7,8 was based upon perturbation expansions with its validity sometimes limited to cases of small transfer integrals 8 . Despite its limitation, the theory has been widely used for qualitative interpretations of experimental data, including the temperature dependence of bandnarrowing effect as well as the crossover from band-like behavior to hopping transport with increasing temperature.…”

Section: Introductionmentioning

confidence: 99%

On the Munn−Silbey Approach to Polaron Transport with Off-Diagonal Coupling and Temperature-Dependent Canonical Transformations

Chen

Zhang

et al. 2011

J. Phys. Chem. B

View full text Add to dashboard Cite

Improved results using a method similar to the Munn-Silbey approach have been obtained on the temperature dependence of transport properties of an extended Holstein model incorporating simultaneous diagonal and off-diagonal exciton-phonon coupling. The Hamiltonian is partially diagonalized by a canonical transformation, and optimal transformation coefficients are determined in a self-consistent manner. Calculated transport properties exhibit substantial corrections on those obtained previously by Munn and Silbey for a wide range of temperatures thanks to a numerically exact evaluation and an added momentum-dependence of the transformation matrix. Results on the diffusion coefficient in the moderate and weak coupling regime show distinct band-like and hopping-like transport features as a function of temperature.

show abstract

“…28 Its energy is determined by electron-phonon coupling through Coulomb interactions. 29,30 Depending on whether long-range or short-range electron-lattice interactions dominate, qualitatively different types of self-trapping occur. A carrier with a long-range interaction self-traps to form a "large" polaron wherein the charge carriers are delocalized over more than a single site.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Dynamics of Polarons in Conductive Polyaniline: Comparison of Primary and Secondary Doped Forms

2008

View full text Add to dashboard Cite

Time-and wavelength-resolved pump-probe measurements are performed on the conductive, primary and secondary doped, forms of polyaniline in solution to investigate the relaxation dynamics of photoexcited polarons. Contrasting dynamics observed in the two forms allow investigation of electronic (and structural) relaxation of this material. Pump pulse at 800 nm photoexcites an electron from the valence to polaron band, and subsequent relaxation dynamics are probed by a white light continuum pulse. Three distinct features are observed in the primary doped sample: (1) absorption near time zero in the 900-1025 nm probe wavelength region; (2) delayed absorption from 850 to 1025 nm; (3) pronounced oscillations with frequencies of 165 and 210 cm -1 . The first two features are associated with intraband absorptions to higher-lying states in the polaron band from the initial excited and conformationally changed intermediate states. The oscillations reflect torsional motions associated with photoexcitation and relaxation. In the secondary doped material, only bleaching and stimulated emission are observed throughout the whole spectral region; neither transient absorption signals nor oscillatory dynamics are observed. Kinetic modeling is performed to establish the mechanism of relaxation. We propose that the excited polaron relaxes nonradiatively to the ground state through an intermediate state(s) with a twisted geometry. Our measurements and analysis allow us to describe the structure of the polaron bands for primary and secondary doped polyaniline; they are in the small and large polaron limits, respectively, and are consistent with a bandgap for the primary doped form and without a bandgap (i.e., metallic) for the secondary doped material.

show abstract

Studies of polaron motion

Cited by 3,078 publications

References 0 publications

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

On the Munn−Silbey Approach to Polaron Transport with Off-Diagonal Coupling and Temperature-Dependent Canonical Transformations

Ultrafast Dynamics of Polarons in Conductive Polyaniline: Comparison of Primary and Secondary Doped Forms

Contact Info

Product

Resources

About

Studies of polaron motion

Cited by 3,078 publications

References 0 publications

Charge Separation in Donor–C60 Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

Charge Separation in Donor–C60 Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

On the Munn−Silbey Approach to Polaron Transport with Off-Diagonal Coupling and Temperature-Dependent Canonical Transformations

Ultrafast Dynamics of Polarons in Conductive Polyaniline: Comparison of Primary and Secondary Doped Forms

Contact Info

Product

Resources

About

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations

Charge Separation in Donor–C₆₀ Complexes with Real-Time Green Functions: The Importance of Nonlocal Correlations