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Optimizing energy and charge transport is key in design and implementation ofefficient two-dimensional (2D) conductive metal-organic frameworks (MOFs) forpractical applications. In this work, for the first time, we investigate therole of both long-range excitonic and short-range charge transfer (CT) couplingas well as their dependency on reorganization energy on through-space transportproperties in 2D MOFs. A pi-stacked model system is built based on thearchetypal Ni3(HITP)2 2D MOF and a Frenkel/CT Holstein Hamiltonian is developedthat takes into account both electronic coupling and intramolecular vibrations.The dependency of the long and short-range couplings of both secondary buildingunits (SBUs) and organic linkers to different dynamical motions in 2D MOFs areevaluated which predicts that photophysical properties of 2D MOFs criticallydepend on the degree of ordering between layers. Using the model system, weshow that the impact of the two coupling sources in these materials can bediscerned or enhanced by sliding of the SBU in a cofacial configuration alongthe long- or short molecular axis. The effects of vibronic spectral signaturesare examined for integrated Frenkel/CT systems in both perturbative andresonance regimes. Although to the best of our knowledge sliding engineering in2D MOFs currently remains beyond reach, the findings reported here offer newdetails on the photophysical structure-property relationships on 2D MOFs andprovide suggestions into how to combine elements of molecular design andengineering to achieve desirable properties and functions for nano- andmesoscale optoelectronic applications.

Frenkel/charge transfer Holstein Hamiltonian applied to energy transfer in 2D layered metal-organic frameworks