Electronic transfer integrals between the frontier orbitals of adjacent molecules represent the most important parameter governing charge transport in organic crystals. Different transfer integrals may be significantly modulated by the same modes of molecular vibrations as a result of nonlocal electron-phonon couplings, leading to spatial correlations between the transfer integrals. Here, by employing a multiscale modeling approach, we investigate theoretically the impacts of transfer-integral correlations (TICs) on the two-dimensional electronic and charge-transport properties of a monolayer pentacene crystal. In particular, we focus on the collinear TICs that are present between molecular pairs along the same direction of molecular packings in the crystal. We reveal that the interplay of the collinear TICs along different directions leads to diverse landscapes of nonlocal electron-phonon couplings in reciprocal space, of which the impacts explicitly manifest themselves in the band structures at finite temperatures. We also evaluate the anisotropic hole mobility of the pentacene monolayer and demonstrate that the consequence of the collinear TICs can be reflected in the behaviors of the temperature-dependent band-like mobility observed in experiment. These findings provide an insight into how nonlocal electron-phonon couplings operate through TICs to impact the electronic and electrical properties of organic crystals in two dimension.

相邻分子前沿轨道之间的电子转移积分代表了控制有机晶体中电荷传输的最重要参数。由于非局部电子-声子耦合，不同的传递积分可能会因分子振动的相同模式而受到显着调制，从而导致传递积分之间存在空间相关性。在这里，通过采用多尺度建模方法，我们从理论上研究了转移积分相关性（TIC）对单层并五苯晶体的二维电子和电荷传输性质的影响。特别地，我们集中于沿着晶体中分子堆积的相同方向存在于分子对之间的共线TIC。我们揭示了共线TIC沿不同方向的相互作用导致互易空间中非局域电子-声子耦合的不同态势，其中的影响在有限温度下的能带结构中明确表现出来。我们还评估了并五苯单层的各向异性空穴迁移率，并证明了共线TICs的结果可以反映在实验中观察到的与温度相关的带状迁移率的行为中。这些发现提供了对非局部电子-声子耦合如何通过TIC起作用以二维影响有机晶体的电子和电学性质的见解。其中的影响在有限温度下明显地表现在能带结构中。我们还评估了并五苯单层的各向异性空穴迁移率，并证明了共线TICs的结果可以反映在实验中观察到的与温度相关的带状迁移率的行为中。这些发现提供了对非局部电子-声子耦合如何通过TIC起作用以二维影响有机晶体的电子和电学性质的见解。其中的影响在有限温度下明显地表现在能带结构中。我们还评估了并五苯单层的各向异性空穴迁移率，并证明了共线TICs的结果可以反映在实验中观察到的与温度相关的带状迁移率的行为中。这些发现提供了对非局部电子-声子耦合如何通过TIC起作用以二维影响有机晶体的电子和电学性质的见解。