scholarly journals Quantifying through-space charge transfer dynamics in π-coupled molecular systems

2012 ◽  
Vol 3 (1) ◽  
Author(s):  
Arunabh Batra ◽  
Gregor Kladnik ◽  
Héctor Vázquez ◽  
Jeffrey S. Meisner ◽  
Luca Floreano ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Space Charge ◽  
Molecular Systems ◽  
Charge Transfer Dynamics

scholarly journals Stacking Effects on Charge Transfer Dynamics in Fluctuating DNA

2020 ◽  
Author(s):  
Zhongwei Li ◽  
Keli Han
Keyword(s):  
Charge Transfer ◽  
Kinetic Monte Carlo ◽  
General Rule ◽  
Md Simulations ◽  
Squeezing Effect ◽  
Molecular Systems ◽  
Hopping Mechanism ◽  
Electron Transfer Theory ◽  
Charge Transfer Dynamics ◽  
Charge Transfer In Dna

Base-stacked structure is an important feature of DNA molecules. But dynamics study on the influences of the stacking effects on charge transfer in DNA is yet rare.In this article, a general rule about the relationship of onsite energies of same bases in a stack is derived by H ̈uckel theory. It is found that the base in the middle position of the stack has lower onsite energy than the bases at the terminals due to squeezing effect, which is different from previous studied neighboring base effect. The former is along-range effect while the latter acts in a short range. Semiempirical MNDO calculations on (A:T) n (n=1∼10) systems verfied the H ̈uckel analysis. From this perspective,the so-called incoherent hopping mechanism is actually somewhat coherent due to the squeezing effect. To understand these stacking effects on charge transfer in DNA,a cross-scale method which combines classical MD simulations, quantum mechanism calculations, Marcus electron transfer theory and kinetic Monte Carlo simulations is developed and applied on hole dynamics in (A:T) n (G:C) (n=1∼10) systems. Although no superexchange mechanism is explicitly involved in the studied systems, a crossover from strong to weak distance-dependency of hole arrival rates, which is an experimentally observed property of hole dynamics in DNA and is thought an evidence of the conversion from superexchange to hopping mechanism, also appears. We attribute it to the stacking effects. Such a result provides a new idea on explaining the crossover of different distance-dependencies of charge transfer rates in DNA. In addition, the squeezing effect may be a new driving force for long-range charge transfer. At the same time, some technical methods developed in the dynamics, e.g. calculations of onsite energies and electronic couplings in a stack, and simulated hole dynamics, etc.,can be generalized to other complex molecular systems with charge transfer behaviors.<br><br>

scholarly journals Direct Non-adiabatic Simulations of the Photoinduced Charge Transfer Dynamics

2020 ◽  
Author(s):  
Sharma Yamijala ◽  
Pengfei Huo
Keyword(s):  
Charge Transfer ◽  
Density Functional ◽  
Time Dependent ◽  
Photoinduced Charge Transfer ◽  
Molecular Systems ◽  
Classical Path ◽  
Charge Transfer Dynamics ◽  
Dynamics Simulations ◽  
High Level ◽  
Photoinduced Charge

We apply direct non-adiabatic dynamics simulations to investigate photoinduced charge transfer reactions. Our approach is based on the mixed quantum-classical fewest switches surface hopping (FSSH) method that treats the transferring electron through time-dependent density functional theory and the nuclei classically. The photoinduced excited state is modeled as a transferring single-electron that initially occupies the LUMO of the donor molecule/moiety. This single-particle electronic wavefunction is then propagated quantum mechanically by solving the time-dependent Schr\"odinger equation in the basis of the instantaneous molecular orbitals (MOs) of the entire system. The non-adiabatic transitions among electronic states are modeled using the FSSH approach within the classical-path approximation. We apply this approach to simulate the photoinduced charge transfer dynamics in a few well-characterized molecular systems. Our results are in excellent agreement with both the experimental measurements and high-level (yet expensive) theoretical results.

Exploiting a single intramolecular conformational switching Ni-TPP molecule to probe charge transfer dynamics at the nanoscale on bare Si(100)-2 × 1

2017 ◽  
Vol 19 (42) ◽  
pp. 28982-28992 ◽  
Author(s):  
Hatem Labidi ◽  
Henry P. Pinto ◽  
Jerzy Leszczynski ◽  
Damien Riedel
Keyword(s):  
Charge Transfer ◽  
Quantitative Information ◽  
Electronic Excitations ◽  
Conformational Switching ◽  
Molecular Systems ◽  
Charge Transfer Dynamics ◽  
Switching Efficiency

Acquiring quantitative information on charge transfer is performed on a single intramolecular switch. Using local electronic excitations allow to trigger (CT) process and tune its switching efficiency. Our method can be applied to investigate various molecular systems.

scholarly journals Stacking Effects on Charge Transfer Dynamics in Fluctuating DNA

2020 ◽  
Author(s):  
Zhongwei Li ◽  
Keli Han
Keyword(s):  
Charge Transfer ◽  
Kinetic Monte Carlo ◽  
General Rule ◽  
Md Simulations ◽  
Squeezing Effect ◽  
Molecular Systems ◽  
Hopping Mechanism ◽  
Electron Transfer Theory ◽  
Charge Transfer Dynamics ◽  
Charge Transfer In Dna

Base-stacked structure is an important feature of DNA molecules. But dynamics study on the influences of the stacking effects on charge transfer in DNA is yet rare.In this article, a general rule about the relationship of onsite energies of same bases in a stack is derived by H ̈uckel theory. It is found that the base in the middle position of the stack has lower onsite energy than the bases at the terminals due to squeezing effect, which is different from previous studied neighboring base effect. The former is along-range effect while the latter acts in a short range. Semiempirical MNDO calculations on (A:T) n (n=1∼10) systems verfied the H ̈uckel analysis. From this perspective,the so-called incoherent hopping mechanism is actually somewhat coherent due to the squeezing effect. To understand these stacking effects on charge transfer in DNA,a cross-scale method which combines classical MD simulations, quantum mechanism calculations, Marcus electron transfer theory and kinetic Monte Carlo simulations is developed and applied on hole dynamics in (A:T) n (G:C) (n=1∼10) systems. Although no superexchange mechanism is explicitly involved in the studied systems, a crossover from strong to weak distance-dependency of hole arrival rates, which is an experimentally observed property of hole dynamics in DNA and is thought an evidence of the conversion from superexchange to hopping mechanism, also appears. We attribute it to the stacking effects. Such a result provides a new idea on explaining the crossover of different distance-dependencies of charge transfer rates in DNA. In addition, the squeezing effect may be a new driving force for long-range charge transfer. At the same time, some technical methods developed in the dynamics, e.g. calculations of onsite energies and electronic couplings in a stack, and simulated hole dynamics, etc.,can be generalized to other complex molecular systems with charge transfer behaviors.<br><br>

scholarly journals Direct Non-adiabatic Simulations of the Photoinduced Charge Transfer Dynamics

2020 ◽  
Author(s):  
Sharma Yamijala ◽  
Pengfei Huo
Keyword(s):  
Charge Transfer ◽  
Density Functional ◽  
Time Dependent ◽  
Photoinduced Charge Transfer ◽  
Molecular Systems ◽  
Classical Path ◽  
Charge Transfer Dynamics ◽  
Dynamics Simulations ◽  
High Level ◽  
Photoinduced Charge

We apply direct non-adiabatic dynamics simulations to investigate photoinduced charge transfer reactions. Our approach is based on the mixed quantum-classical fewest switches surface hopping (FSSH) method that treats the transferring electron through time-dependent density functional theory and the nuclei classically. The photoinduced excited state is modeled as a transferring single-electron that initially occupies the LUMO of the donor molecule/moiety. This single-particle electronic wavefunction is then propagated quantum mechanically by solving the time-dependent Schr\"odinger equation in the basis of the instantaneous molecular orbitals (MOs) of the entire system. The non-adiabatic transitions among electronic states are modeled using the FSSH approach within the classical-path approximation. We apply this approach to simulate the photoinduced charge transfer dynamics in a few well-characterized molecular systems. Our results are in excellent agreement with both the experimental measurements and high-level (yet expensive) theoretical results.

Charge-Transfer Dynamics at Ag/Ni-MOF/Cu2O heterostructure in Photoelectrochemical NH3 production

2021 ◽  
Author(s):  
Ying Liu ◽  
Jianmin Lu ◽  
Qianxiao Zhang ◽  
Yajie Bai ◽  
Xuliang Pang ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Absorption Spectroscopy ◽  
Transient Absorption ◽  
Transient Absorption Spectroscopy ◽  
Yield Rate ◽  
Ultrafast Transient Absorption ◽  
Charge Transfer Dynamics ◽  
Ultrafast Transient Absorption Spectroscopy

Decoration of Ag-ultrathin Ni-MOF onside Cu2O was firstly fabricated. The charge-transfer dynamics at heterostructure was in-depth revealed by ultrafast transient absorption spectroscopy. NH3 yield rate (4.63 μg h-1 cm-2) with...

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