Re-evaluating how charge transfer modifies the conformation of adsorbed molecules.
Re-evaluating how charge transfer modifies the conformation of adsorbed molecules.
复制标题
DOI：
10.1039/c8nr02237b
复制
发表时间：
2018-08-09
期刊：
影响因子：
6.7
通讯作者：
Woodruff DP
中科院分区：
文献类型：
--
作者：
Blowey PJ ;Velari S ;Rochford LA ;Duncan DA ;Warr DA ;Lee TL ;De Vita A ;Costantini G ;Woodruff DP
结合定量实验和理论结构测定表明，TCNQ并不像传统观点所期望的那样倾向于Ag（111）。典型的电子受体分子，TCNQ，通常被认为在吸附在铸币金属表面时弯曲成倒碗状，并带负电荷。新的定量实验结构测量表明，Ag（111）上的TCNQ并非如此。DFT计算表明，包含色散力修正不仅降低了分子-衬底层间距，而且降低了预测的分子键合程度。然而，实验确定的结构参数和理论预测的结构参数之间的完全一致只能通过在分子层中包含银原子来实现，这也是能量上有利的构型。研究结果强调需要实验和理论定量结构方法来可靠地理解类似的金属-有机界面，并强调需要重新评估一些先前研究的系统。
A combined quantitative experimental and theoretical structure determination shows TCNQ is not bent on Ag(111) as expected from conventional wisdom. The archetypal electron acceptor molecule, TCNQ, is generally believed to become bent into an inverted bowl shape upon adsorption on the coinage metal surfaces on which it becomes negatively charged. New quantitative experimental structural measurements show that this is not the case for TCNQ on Ag(111). DFT calculations show that the inclusion of dispersion force corrections reduces not only the molecule-substrate layer spacing but also the degree of predicted molecular bonding. However, complete agreement between experimentally-determined and theoretically-predicted structural parameters is only achieved with the inclusion of Ag adatoms into the molecular layer, which is also the energetically favoured configuration. The results highlight the need for both experimental and theoretical quantitative structural methods to reliably understand similar metal–organic interfaces and highlight the need to re-evaluate some previously-investigated systems.
登录
查看更多内容
影响因子：
3
作者：
Grimme, Stefan
通讯作者：
Grimme, Stefan
影响因子：
3
作者：
Barone, Vincenzo;Casarin, Maurizio;Vittadini, Andrea
通讯作者：
Vittadini, Andrea
影响因子：
8.6
作者：
Dion, M;Rydberg, H;Lundqvist, BI
通讯作者：
Lundqvist, BI
影响因子：
16.6
作者：
Classen, T;Fratesi, G;Kern, K
通讯作者：
Kern, K
影响因子：
3.7
作者：
Katayama, Tetsuo;Mukai, Kozo;Yoshinobu, Jun
通讯作者：
Yoshinobu, Jun