Building the Chessboard-like Supramolecular Structure on Au (111) Surfaces

链状结构单羟基醇的动力学：氢键寿命、链交换与德拜过程

Dynamics of monohydroxy alcohols with chain-like structures: Hydrogen bonding lifetime, chain swapping, and Debye process

基于可逆氢键缔合与解离，提出活链模型描述单羟基醇的超分子结构与动力学，揭示四种时间尺度及五个动力学区域，其中德拜弛豫源于链端偶极重定向。

Supramolecular self-assembly as a tool to preserve electronic purity of perylene diimide chromophores

Small molecule organic semiconductors hold great promise for efficient, printable, and flexible optoelectronic applications like solar cells and displays. However, strong excited-state quenching due to uncontrolled aggregation currently limits their performance and employability in devices. Here, we report on the self-assembly of a supramolecular pseudo-cube formed from six modified tetradentate perylene diimides (PDIs). The rigid, shape-persistent cage sets the distance and orientation of the PDI chromophores and suppresses intramolecular rotations and vibrations, leading to non-aggregated, m…

Transition-Based Constrained DFT for the Robust and Reliable Treatment of Excitations in Supramolecular Systems

Despite the variety of available computational approaches, state-of-the-art methods for calculating excitation energies such as time-dependent density functional theory (TDDFT), are computationally demanding and thus limited to moderate system sizes. Here, we introduce a new variation of constrained DFT (CDFT), wherein the constraint corresponds to a particular transition (T), or combination of transitions, between occupied and virtual orbitals, rather than a region of the simulation space as in traditional CDFT. We compare T-CDFT with TDDFT and $Δ$SCF results for the low lying excited states …

Revealing the Physico-Chemical Basis of Organic Solid-Solid Wetting Deposition: Casimir-Like Forces, Hydrophobic Collapse, and the Role of the Zeta Potential

Supramolecular self-assembly at the solid-solid interface enables the deposition and monolayer formation of insoluble organic semiconductors under ambient conditions. The underlying process, termed as the Organic Solid-Solid Wetting Deposition (OSWD), generates two-dimensional adsorbates directly from dispersed three-dimensional organic crystals. This straightforward process has important implications in various fields of research and technology, such as in the domains of low-dimensional crystal engineering, the chemical doping and band-gap engineering of graphene, and in the area of field-eff…

Surface-confined 2D polymerization of a brominated copper-tetraphenylporphyrin on Au(111)

A coupling-limited approach for the Ullmann reaction-like on-surface synthesis of a two-dimensional covalent organic network starting from a halogenated metallo-porphyrin is demonstrated. Copper-octabromo-tetraphenylporphyrin molecules can diffuse and self-assemble when adsorbed on the inert Au(111) surface. Splitting-off of bromine atoms bonded at the macrocyclic core of the porphyrin starts at room temperature after the deposition and is monitored by X-ray photoelectron spectroscopy for different annealing steps. Direct coupling between the reactive carbon sites of the molecules is, however,…