Introducing mesoscopic charge transfer rates into molecular electronics

2020 ◽  
Vol 22 (19) ◽  
pp. 10828-10832 ◽  
Author(s):  
Adriano Santos ◽  
Ushula M. Tefashe ◽  
Richard L. McCreery ◽  
Paulo R. Bueno
Keyword(s):  
Charge Transfer ◽  
Molecular Electronics ◽  
Molecular Electronic ◽  
Transfer Rates

It has been demonstrated that the concept of mesoscopic rate is able to establish a bridge between electrochemical and molecular electronic concepts.

scholarly journals Charge transfer through single molecule contacts: How reliable are rate descriptions?

2011 ◽  
Vol 2 ◽  
pp. 416-426 ◽  
Author(s):  
Denis Kast ◽  
L Kecke ◽  
J Ankerhold
Keyword(s):  
Charge Transfer ◽  
Exact Solutions ◽  
Ab Initio ◽  
Molecular Electronics ◽  
Single Molecule ◽  
Building Blocks ◽  
Transport Processes ◽  
Intramolecular Electron Transfer ◽  
Transfer Rates ◽  
The Impact

Background: The trend for the fabrication of electrical circuits with nanoscale dimensions has led to impressive progress in the field of molecular electronics in the last decade. However, a theoretical description of molecular contacts as the building blocks of future devices is challenging, as it has to combine the properties of Fermi liquids in the leads with charge and phonon degrees of freedom on the molecule. Outside of ab initio schemes for specific set-ups, generic models reveal the characteristics of transport processes. Particularly appealing are descriptions based on transfer rates successfully used in other contexts such as mesoscopic physics and intramolecular electron transfer. However, a detailed analysis of this scheme in comparison with numerically exact solutions is still elusive. Results: We show that a formulation in terms of transfer rates provides a quantitatively accurate description even in domains of parameter space where strictly it is expected to fail, e.g., at lower temperatures. Typically, intramolecular phonons are distributed according to a voltage driven steady state that can only roughly be captured by a thermal distribution with an effective elevated temperature (heating). An extension of a master equation for the charge–phonon complex, to effectively include the impact of off-diagonal elements of the reduced density matrix, provides very accurate solutions even for stronger electron–phonon coupling. Conclusion: Rate descriptions and master equations offer a versatile model to describe and understand charge transfer processes through molecular junctions. Such methods are computationally orders of magnitude less expensive than elaborate numerical simulations that, however, provide exact solutions as benchmarks. Adjustable parameters obtained, e.g., from ab initio calculations allow for the treatment of various realizations. Even though not as rigorously formulated as, e.g., nonequilibrium Green’s function methods, they are conceptually simpler, more flexible for extensions, and from a practical point of view provide accurate results as long as strong quantum correlations do not modify the properties of the relevant subunits substantially.

Charge Transport through Molecular Junctions

MRS Bulletin ◽  
2004 ◽  
Vol 29 (6) ◽  
pp. 385-390 ◽  
Author(s):  
M.C. Hersam ◽  
R.G. Reifenberger
Keyword(s):  
Charge Transfer ◽  
Solid State ◽  
Charge Transport ◽  
Molecular Electronics ◽  
Resonant Tunneling ◽  
Dominant Role ◽  
Electronic Devices ◽  
Molecular Electronic ◽  
Electron Stimulated Desorption ◽  
Interface Effects

AbstractIn conventional solid-state electronic devices, junctions and interfaces play a significant if not dominant role in controlling charge transport. Although the emerging field of molecular electronics often focuses on the properties of the molecule in the design and understanding of device behavior, the effects of interfaces and junctions are often of comparable importance. This article explores recent work in the study of metal–molecule–metal and semiconductor–molecule–metal junctions. Specific issues include the mixing of discrete molecular levels with the metal continuum, charge transfer between molecules and semiconductors, electron-stimulated desorption, and resonant tunneling. By acknowledging the consequences of junction/interface effects, realistic prospects and limitations can be identified for molecular electronic devices.

Photoinduced Charge Transfer Dynamics in Carotenoid-Porphyrin-C60 Triad via the Linearized Semiclassical Nonequilibrium Fermi's Golden Rule

2020 ◽  
Author(s):  
Zhengqing Tong ◽  
Margaret S. Cheung ◽  
Barry D. Dunietz ◽  
Eitan Geva ◽  
Xiang Sun
Keyword(s):  
Charge Transfer ◽  
Golden Rule ◽  
Time Dependent ◽  
Rate Coefficients ◽  
Initial State ◽  
Photoinduced Charge Transfer ◽  
Transfer Rates ◽  
Fermi's Golden Rule ◽  
Photoinduced Charge ◽  
Fermi’S Golden Rule

The nonequilibrium Fermi’s golden rule (NE-FGR) describes the time-dependent rate coefficient for electronic transitions, when the nuclear degrees of freedom start out in a <i>nonequilibrium</i> state. In this letter, the linearized semiclassical (LSC) approximation of the NE-FGR is used to calculate the photoinduced charge transfer rates in the carotenoid-porphyrin-C<sub>60</sub> molecular triad dissolved in explicit tetrahydrofuran. The initial nonequilibrium state corresponds to impulsive photoexcitation from the equilibrated ground-state to the ππ* state, and the porphyrin-to-C<sub>60</sub> and the carotenoid-to-C<sub>60</sub> charge transfer rates are calculated. Our results show that accounting for the nonequilibrium nature of the initial state significantly enhances the transition rate of the porphyrin-to-C<sub>60</sub> CT process. We also derive the instantaneous Marcus theory (IMT) from LSC NE-FGR, which casts the CT rate coefficients in terms of a Marcus-like expression, with explicitly time-dependent reorganization energy and reaction free energy. IMT is found to reproduce the CT rates in the system under consideration remarkably well.

Correction to Effect of Backbone Flexibility on Charge Transfer Rates in Peptide Nucleic Acid Duplexes

2012 ◽  
Vol 134 (31) ◽  
pp. 13141-13141 ◽  
Author(s):  
Emil Wierzbinski ◽  
Arnie de Leon ◽  
Xing Yin ◽  
Alexander Balaeff ◽  
Kathryn L. Davis ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Nucleic Acid ◽  
Peptide Nucleic Acid ◽  
Backbone Flexibility ◽  
Transfer Rates

Effect of Backbone Flexibility on Charge Transfer Rates in Peptide Nucleic Acid Duplexes

2012 ◽  
Vol 134 (22) ◽  
pp. 9335-9342 ◽  
Author(s):  
Emil Wierzbinski ◽  
Arnie de Leon ◽  
Xing Yin ◽  
Alexander Balaeff ◽  
Kathryn L. Davis ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Nucleic Acid ◽  
Peptide Nucleic Acid ◽  
Backbone Flexibility ◽  
Transfer Rates

On the Interplay between Electronic Structure and Polarizable Force Fields When Calculating Solution-Phase Charge-Transfer Rates

2020 ◽  
Vol 16 (10) ◽  
pp. 6481-6490
Author(s):  
Jaebeom Han ◽  
Pengzhi Zhang ◽  
Huseyin Aksu ◽  
Buddhadev Maiti ◽  
Xiang Sun ◽  
...  
Keyword(s):  
Electronic Structure ◽  
Charge Transfer ◽  
Force Fields ◽  
Solution Phase ◽  
Transfer Rates ◽  
Polarizable Force Fields

scholarly journals Effects of the Distributions of Energy or Charge Transfer Rates on Spectral Hole Burning in Pigment–Protein Complexes at Low Temperatures

2011 ◽  
Vol 115 (50) ◽  
pp. 15098-15109 ◽  
Author(s):  
Nicoleta Herascu ◽  
Somaya Ahmouda ◽  
Rafael Picorel ◽  
Michael Seibert ◽  
Ryszard Jankowiak ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Low Temperatures ◽  
Protein Complexes ◽  
Hole Burning ◽  
Spectral Hole Burning ◽  
Transfer Rates ◽  
Spectral Hole ◽  
Pigment Protein Complexes

scholarly journals Nanofabrication Techniques in Large-Area Molecular Electronic Devices

2020 ◽  
Vol 10 (17) ◽  
pp. 6064
Author(s):  
Lucía Herrer ◽  
Santiago Martín ◽  
Pilar Cea
Keyword(s):  
Molecular Electronics ◽  
Global Economy ◽  
Electronic Devices ◽  
Functional Materials ◽  
Large Area ◽  
Molecular Electronic ◽  
Hybrid Technology ◽  
Top Contact ◽  
Silicon Based ◽  
Molecular Electronic Devices

The societal impact of the electronics industry is enormous—not to mention how this industry impinges on the global economy. The foreseen limits of the current technology—technical, economic, and sustainability issues—open the door to the search for successor technologies. In this context, molecular electronics has emerged as a promising candidate that, at least in the short-term, will not likely replace our silicon-based electronics, but improve its performance through a nascent hybrid technology. Such technology will take advantage of both the small dimensions of the molecules and new functionalities resulting from the quantum effects that govern the properties at the molecular scale. An optimization of interface engineering and integration of molecules to form densely integrated individually addressable arrays of molecules are two crucial aspects in the molecular electronics field. These challenges should be met to establish the bridge between organic functional materials and hard electronics required for the incorporation of such hybrid technology in the market. In this review, the most advanced methods for fabricating large-area molecular electronic devices are presented, highlighting their advantages and limitations. Special emphasis is focused on bottom-up methodologies for the fabrication of well-ordered and tightly-packed monolayers onto the bottom electrode, followed by a description of the top-contact deposition methods so far used.

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