Vibrational-Rotational Excitations in Nonlinear Molecular Systems

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Mode-selective vibrational modulation of charge transport in organic electronic devices

Erikhman , Hardcover. Be the first to write a review About this product. In a similar way we can exclaim: "If there would be no nonlinearity than what physics would that be''.

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For example, the general theory of relativity by A. Einstein comes to mind first - one of the most beautiful physical theories, which is in fact essentially nonlinear. Next, the phase transitions crystal liquid and liquid gas are due to the anhar monicity of inter-particle interactions, to dissociation and infinite motion. Similarly, transitions into the superconducting state or the superftuid would be impossible with purely harmonic interaction potentials. Another bril liant achievement in nonlinear physics was the construction of a laser and the subsequent development of nonlinear optics.

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The latter describes the in teraction of the matter with light of super-high intensity, when multi-quanta intra-molecular transitions become essential. Last, we should note here the very beautiful mathematical theory the theory of catastrophes. Its subject is the study of invariant general properties of multi-dimensional surfaces in the vicinity of bifurcation points with respect to continuous transformations. Additional Product Features Number of Volumes.

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During the optimization, the unit-cell parameters were kept fixed at the experimental values. Since there are two independent molecules in the unit cell of the pentacene crystal, all molecular vibration modes are quasi degenerate. Transfer integrals electronic couplings for holes were calculated using a fragment orbital approach based on the unperturbed highest occupied molecular orbitals of the individual neutral molecules extracted from the optimized crystal geometry The non-local hole—phonon coupling constants v come from the modulation of the transfer integrals by lattice vibrations.

The coupling constants can be computed by expanding the electronic couplings into Taylor series of the phonon eigenvectors:.

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  • Here, t 0 is the electronic coupling at the crystal equilibrium geometry; Q j is the normal-mode coordinate of mode j ; v j is the linear non-local electron—phonon coupling constant. In practice, the coupling constants are calculated by distorting the crystal along all normal-mode coordinates with positive and negative steps and then computing numerically the related derivatives of the transfer integrals for each vibrational mode.


    The normal modes of the neutral Q n and cation Q c states are related to each other via a multidimensional rotation Duschinsky matrix Supplementary Table 2 The calculated frequencies for both isolated molecule and crystal were scaled by 0. How to cite this article: Bakulin, A.

    Mode-selective vibrational modulation of charge transport in organic electronic devices. Author contributions A. National Center for Biotechnology Information , U. Nat Commun. Published online Aug 6.

    Vibrational-Rotational Excitations in Nonlinear Molecular Systems

    Artem A. Bakker , 1 Yves L.

    Rezus , 1 Pabitra K. Huib J. Yves L. Pabitra K. Author information Article notes Copyright and License information Disclaimer. Received May 12; Accepted Jun All Rights Reserved. This work is licensed under a Creative Commons Attribution 4. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. This article has been cited by other articles in PMC.

    Abstract The soft character of organic materials leads to strong coupling between molecular, nuclear and electronic dynamics. Results Optoelectronic characterization of model device Figure 1a—c describes the organic bilayer photoresistor model system. Open in a separate window. Figure 1. The molecular electronic device characterization. Pump—push photocurrent measurements In a PPP experiment, an optoelectronic device is illuminated by a sequence of laser pulses interacting with the active material in the device.

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    Figure 2. The results of pump—push photocurrent measurements. Figure 3. Experimental evaluation of vibrational modulation effect. Discussion We observe that the amplitude of the PPP response does not follow the intensity of the infrared absorption. Figure 4. Calculated electron—phonon couplings and comparison with experiments. Methods Materials and devices The gold electrodes for the phototransistor were fabricated on a SiO 2 substrate by a standard microfabrication technique with sequential processes of photolithography, metal evaporation and lift-off.

    Ultrafast experiments Ultrafast experiments were performed inside a N 2 flow compartment. Additional information How to cite this article: Bakulin, A. Footnotes Author contributions A. References Bredas J. Polarons, bipolarons, and solitons in conducting polymers. Accounts Chem. Nuclear coupling and polarization in molecular transport junctions: beyond tunneling to function. Science , — Conical intersection dynamics of the primary photoisomerization event in vision. Nature , — Femtosecond torsional relaxation.

    Molecular vibration-sensing component in human olfaction. Coherent ultrafast charge transfer in an organic photovoltaic blend. Experimental evidence for quantum interference and vibrationally induced decoherence in single-molecule junctions. The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment-protein complexes. Selectivity in vibrationally mediated single-molecule chemistry. Polaron hopping mediated by nuclear tunnelling in semiconducting polymers at high carrier density. Measurement of molecular motion in organic semiconductors by thermal diffuse electron scattering.

    Vibrational and electronic heating in nanoscale junctions.