Hendzel Maciej, Fidrysiak Maciej, Spałek Józef
Institute of Theoretical Physics, Jagiellonian University, ulica Łojasiewicza 11, PL-30-348 Kraków, Poland.
J Phys Chem Lett. 2022 Nov 10;13(44):10261-10266. doi: 10.1021/acs.jpclett.2c02544. Epub 2022 Oct 27.
A precise discussion of a single bond requires consideration of two-particle wave function for the particles involved. Here we define and determine rigorously the intrinsic covalency and connected characteristics of the canonical example of the H molecule. This is achieved by starting from an analytic form for the two-particle wave function for electrons forming the bond, in which we single out the atomic contribution () in an unequivocal manner. The presence of the and ionicity factors complements the existing attributes of the bond. In this way, a gradual evolution of the molecular state to its two-atom correspondent is traced systematically with increasing interatomic distance. In effect, a direct relation to the onset of incipient Mott-Hubbard atomicity () to the intrinsic covalency and ionicity is established. This goal is achieved formally by combining the single-particle wave function readjustment in the entangled state with a simultaneous determination of two-particle states in the particle (second quantization) representation.
对单键进行精确讨论需要考虑所涉及粒子的双粒子波函数。在这里，我们严格定义并确定了H分子典型例子的本征共价性和连接特性。这是通过从形成键的电子的双粒子波函数的解析形式出发来实现的，在这种形式中，我们以明确的方式分离出原子贡献（）。和离子性因子的存在补充了键的现有属性。通过这种方式，随着原子间距离的增加，系统地追踪分子态向其双原子对应物的逐渐演化。实际上，建立了初始莫特 - 哈伯德原子性（）的起始与本征共价性和离子性之间的直接关系。通过将纠缠态中的单粒子波函数调整与粒子（二次量子化）表示中双粒子态的同时确定相结合，正式实现了这一目标。
