Nonlinear Optical Properties of Organosilicons: Intramolecular Charge Transfer in Pyridyldisilanes with a Donor‐Acceptor Linker

Abstract

As a novel kind of organosilicon complex, dipyridyldisilane and 1‐phenyl‐2‐pyridyl‐disilane with a donor‐ acceptor link by the σ‐π interaction and intramolecular charge transfer, has been investigated by the density functional theory. It is found that the phenyl replaced by the pyridy in diphenyldisilane can significantly narrow the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) gap, and enhance the electronic polarization, thus make the electronic distribution more diffuse. As a result, the static first hyperpolarizability (β0) of dipyridyldisilane is enhanced to the range of 10.365×10−30 esu ∼ 26.385×10−30esu. And in order to know the effect of the number of pyridyl ring and the position of pyridyl ring on NLO responses, we calculated the β0 values for 1‐phenyl‐2‐pyridyl‐disilane, they are in the range of 6.475×10−30 esu ∼ 1482.613×10−30esu. The smaller HOMO‐LUMO gap and the smaller transition energy make the larger value of β0. This kind of organosilicon complex is one of the potentially versatile and fascinating nonlinear optical materials.

External electric field driven electronic structures: tunable nonlinear optical properties of helical bilayer nanographenes

“…[1][2][3][4][5][6][7][8] The realm of NLO materials encompasses inorganic materials, 9,10 organic materials 11,12 and metal-organic materials, 13,14 garnering significant interest from both theoretical and experimental researchers. Currently, various strategies aim to enhance NLO properties, including the introduction of donor (D) and acceptor (A) moieties, [15][16][17] strengthening p-conjugated chain structures, 18,19 and applying external electric fields to organic compounds. [20][21][22] In recent years, the significant enhancement of NLO performance has been achieved through the application of external electric fields, given their profound effects on molecular structures and electronic properties.…”

“…1–8 The realm of NLO materials encompasses inorganic materials, 9,10 organic materials 11,12 and metal–organic materials, 13,14 garnering significant interest from both theoretical and experimental researchers. Currently, various strategies aim to enhance NLO properties, including the introduction of donor (D) and acceptor (A) moieties, 15–17 strengthening π-conjugated chain structures, 18,19 and applying external electric fields to organic compounds. 20–22…”