Ling Yang

Since the concept of aggregation‐induced emission (AIE) was proposed by Benzhong Tang's research group in 2001, the exploration of the mechanism of AIE and the development of new high‐performance AIE materials have been the focus and goal of this field. On the basis of a large number of experiment results, AIE mechanism has been well explained by lots of works, such as restricted intramolecular motion (RIM), J‐aggregate et al. As tetraphenylethlene (TPE) molecules are stacked, the rotation of the benzene ring rotor is blocked, and the energy attenuation is released in the form of radiation, showing the AIE effect. In order to further explore the AIE effect of TPE, we performed electronic structure, spectrum simulation, and AIE mechanism calculations of the anthryl‐tetraphenylethene (TPE‐an) monomer and dimer in the gas phase, tetrahydrofuran (THF), and aqueous solutions at the B3LYP/6‐31G** level. The calculation results show that TPE‐an molecule is in a propeller‐like configuration, and its fluorescence intensity is weak; compared with the monomer, the fluorescence intensity of the dimer increases by 87% in aqueous solution; the fluorescence intensity in the gas phase, THF solution, and aqueous solution gradually enhances with the increase of the degree of aggregation, which are consistent with the experimental results. The enhancement of fluorescence intensity is caused by the change of molecular structure caused by aggregation. This detailed AIE luminescence mechanism will provide theoretical guidance for AIE material design.

Cells orchestrate the motion and force of hundreds of protein motors to perform various mechanical tasks over multiple length scales. However, engineering active biomimetic materials from protein motors that consume energy to propel continuous motion of micrometer-sized assembling systems remains challenging. Here, we report rotary biomolecular motor-powered supramolecular (RBMS) colloidal motors that are hierarchically assembled from a purified chromatophore membrane containing F _O F ₁ -ATP synthase molecular motors, and an assembled polyelectrolyte microcapsule. The micro-sized RBMS motor with asymmetric distribution of F _O F ₁ -ATPases can autonomously move under light illumination and is collectively powered by hundreds of rotary biomolecular motors. The propulsive mechanism is that a transmembrane proton gradient generated by a photochemical reaction drives F _O F ₁ -ATPases to rotate for ATP biosynthesis, which creates a local chemical field for self-diffusiophoretic force. Such an active supramolecular architecture endowed with motility and biosynthesis offers a promising platform for intelligent colloidal motors resembling the propulsive units in swimming bacteria.

The recently synthesized triangulenes with non-bonding edge states could have broad potential applications in magnetics, spintronics and electro-optics if they have appropriate electronic structure modulation. In the present work, strategies based on molecular orbital theory through heteroatom doping are proposed to redistribute, reduce or eliminate the spin of triangulenes for novel functional materials design, and the role of B, N, NBN, and BNB in such intended electronic structure manipulation is scrutinized. π-Extended triangulenes with tunable electronic properties could be potential nonlinear optical (NLO) materials with appropriate inhibition of their polyradical nature. The elimination of spin is achieved by B, N, NBN, and BNB doping with the intended geometric arrangement for enhanced polarity. Intended doping of BNB results in an optimal structure with large static first hyperpolarizability (〈β₀〉) as well as strong Hyper–Rayleigh scattering (HRS) β_HRS(−2ω; ω, ω) (ω = 1064.0 nm), TG7-BNB-ba with a large 〈β₀〉 (18.85 × 10⁻³⁰ esu per heavy atom) and β_HRS (1.15 × 10⁻²⁸ esu per heavy atom) much larger than that of a synthesized triangular molecule (1.12 × 10⁻³⁰ esu of 〈β₀〉 per heavy atom and 5.04 × 10⁻³⁰ esu of β_HRS per heavy atom). The strong second order NLO responses in the near-infrared and visible regions, particularly the strong sum frequency generation, make these B or (and) N doped triangulenes promising candidates for the fabrication of novel carbon-based optoelectronic devices and micro-NLO devices.

Utilizing bottom-up controllable molecular assembly, the bio-inspired polyelectrolyte multilayer conical nanoswimmers with gold-nanoshell functionalization on different segments are presented to achieve the optimal upstream propulsion performance. The experimental investigation reveals that the presence of the gold nanoshells on the big openings of the nanoswimmers could not only bestow efficient directional propulsion but could also minimize the impact from the external flow. The gold nanoshells at the big openings of nanoswimmers facilitate the acoustically powered propulsion against a flow velocity of up to 2.00 mm s^-1, which is higher than the blood velocity in capillaries and thus provides a proof-of-concept design for upstream nanoswimmers.

The high stability, feasible modification, and good π-conjugation of porphyrin derivatives render these porphyrin-based nanomaterials suitable as potential third order nonlinear optical (NLO) materials. Introducing an azulene in pristine porphyrins can significantly improve the second order NLO properties of the system, and this is studied in the present work using density functional theory based methods and the sum-over-states model. The relative orientation of azulene plays a determinant role in the enhancement of the static first hyperpolarizability (〈β₀〉), e.g., the 〈β₀〉 per heavy atom increases from 0.31 × 10⁻³⁰ esu to 9.78 × 10⁻³⁰ esu. Further addition of metals (Mg and Zn) in these azulene-fused porphyrin systems leads to an even larger 〈β₀〉 per heavy atom of 41.59 × 10⁻³⁰ esu, much larger than that of a recently reported porphyrin derivative (26.47 × 10⁻³⁰ esu). A novel strategy to stabilize the electronic structures as well as maintain good second order NLO responses by introducing appropriate metals into the azulene-fused porphyrins is extendable to other similar systems. Strong sum frequency generation and different frequency generations of those azulene-fused porphyrins in visible and near-infrared regions may inspire experimental exploration and related applications of azulene-based porphyrins particularly in biological nonlinear optics.