Multistate Redox Switching and Near-Infrared Electrochromism Based on a Star-Shaped Triruthenium Complex with a Triarylamine Core

Tang, Jian‐Hong; He, Yan-Qin; Shao, Jiang‐Yang; Gong, Zhong‐Liang; Zhong, Yu‐Wu

doi:10.1038/srep35253

Cited by 32 publications

(9 citation statements)

References 52 publications

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“…The averaged distance between ruthenium ions and the central nitrogen atom is around 6.18 Å. Furthermore, we have calculated the cohesive energy of a system constituting multiple CTTC molecules, demonstrating that van der Waals force between CTTC molecules is too weak to form molecular crystals, which is consistent with experimental reports [23].…”

Section: Molecule Structuresupporting

confidence: 88%

“…A molecular model of the cyclometalated triruthenium complex with a triarylamine core and terpyridine terminals (CTTC) is initially constructed using Monte Carlo (MC) molecular simulation method [22] according to the reported chemical configuration, as shown in Figure 1 [23], which is used as the input structure for geometry optimization of energy minimization. Total energy, electron structure, and optical property of CTTC molecule are calculated using the first-principles method based on spin density functional theory (SDFT) as implemented in DMol3 program of Materials Studio v2017R2 (Accelrys Inc., San Diego, CA, USA) software package [24,25], which are performed utilizing all-electron numerical orbital basis-set scheme with PBEsol gradient-corrected (GGA) exchange-correlation functional [26].…”

Section: Theoretical Calculation Methodologymentioning

confidence: 99%

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First-Principles Study on Redox Magnetism and Electrochromism of Cyclometalated Triarylamine-Core Triruthenium Complex

Li¹,

Wang²,

Chen³

et al. 2021

Crystals

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Spin electronic states and optical properties of a circular ruthenium (Ru) terpyridine complex with a triarylamine core (CTTC) are theoretically investigated by first-principles calculations within an all-electron numerical orbital scheme based on spin density functional theory (SDFT), which demonstrate five well-defined redox states for electrochromic functions. Atomic structure of CTTC molecule is obtained by geometric optimization, and its electronic structure with a decreasing semiconductor band-gap exhibits five consecutive single-electron redox states of Ru-coordinated centers. Except for CTTC in (Ru)3+4 redox state exhibiting a net spin of 2.25 (ћ/2), the other redox states are almost zero in total spin. Density distribution and energy-splitting of spin states indicate that the ferromagnetic coupling of Ru cations coordinating with terpyridine/triarylamine ligands originates dominantly from the spin polarization of Ru 4d-orbitals coordinated by N- and C-2p electrons of triarylamine. CTTC molecule in each redox state represents a well-discriminated absorption in visible region, with the highest characteristic peaks locating at 24.2, 20.2, 21.3, and 19.3/21.7 (103 cm−1) and a manifold of peaks at 13.4~25.3 (103 cm−1) for +2~+6 redox states, respectively. Theoretical electronic structure and optics of CTTC complex are used to evaluate the underlying physical mechanism of realizing a multi-color visible electrochromism by four couples of redox pairs, which is suggested to be applied for monitoring electrical information.

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Section: Molecule Structuresupporting

confidence: 88%

Section: Theoretical Calculation Methodologymentioning

confidence: 99%

First-Principles Study on Redox Magnetism and Electrochromism of Cyclometalated Triarylamine-Core Triruthenium Complex

Li¹,

Wang²,

Chen³

et al. 2021

Crystals

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“…[ 28 ] The triruthenium complex 10 3+ with a triarylamine core has also been prepared (Figure 5). [ 29 ] This complex displays four consecutive redox waves at +0.082, +0.31, +0.74, and +1.07 V vs Ag/AgCl, respectively. The absorption spectra at different redox states are displayed in Figure 5b, wherein strong spectral overlap among 10 4+ , 10 5+ , 10 6+ states is observed.…”

Section: Ruthenium‐amine Conjugated Complexes Showing Multistage Nearmentioning

confidence: 99%

Photofunction‐Directed Coordination Molecular Engineering

Zhong

2021

Chin. J. Chem.

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Molecular engineering has emerged as a highly interdisciplinary field of study on function‐directed molecular design, material synthesis, and property optimization, accompanied by a deep understanding of the structure‐property relationship. In this review, our recent progress on the design and preparations of photofunctional metal complexes and related materials is summarized from the perspective of coordination molecular engineering. In particular, a series of cyclometalated diruthenium complexes with near‐infrared (NIR) electrochromic property have been synthesized by engineering the bridging ligand structures. A group of ruthenium‐amine conjugated complexes with multistage NIR electrochromism are obtained on the basis of a multicenter strategy. By engineering the ligand structures, a series of new ruthenium and platinum complexes are synthesized to show switchable luminescence in response to various stimuli. In addition, photoluminescent ruthenium, iridium, and platinum complexes are assembled to afford micro/nanocrystals with well‐defined morphology and luminescent properties. What is the most favorite and original chemistry developed in your research group? Ruthenium‐triarylamine conjugated system is one of my favorite topics. How do you get into this specific field? Molecular materials with multistage redox processes and multiple near‐ infrared absorptions are a challenging task in the field of electrochromism and molecular switching. The combination of cyclometalated ruthenium complexes and triarylamines allows us to solve this issue by using a multicenter strategy with a great structural and functional diversity. What is the most important personality for scientific research? Personally, I consider honesty, curiosity, and persistence are the most important and fundamental personalities in carrying out scientific research. What's your hobbies? I enjoy playing basketball and watching basketball matches in leisure time. How do you keep balance between research and family? I like managing time by prioritizing daily tasks. If time permits, I'm glad to join family activities in cooking, walking, exercising, etc. I always appreciate and support my wife's career and my daughter's studies, from which I receive their returns in support of my career. Could you please give us some advices on improving Chinese Journal of Chemistry? Chin. J. Chem. is a classical and influential journal of chemistry. The impact of the journal keeps increasing especially in recent years. In my point of view, it would be helpful for the journal by keeping a balance among different subjects of chemistry while welcoming manuscripts on material and energy‐related interdisciplinary researches. In addition, in order to further boost its global reputation, I would like to suggest inviting more international scientists to contribute to the journal.

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“…Consequently, scientists anticipate finding some EC materials with electrofluorochromic (EFC) merit controlled by an electric field, which could be used in either daytime or dusk. , Liou, Sun, Xu, and Niu’s group and others paved the way to integrate EC and EFC. They combined emitters, such as fluorine or quantum dots, which possess EFC properties with EC materials to obtain EFC devices. − Nevertheless, the desired light color, such as white light, is difficult to simultaneously obtain. Inspired by Zhang et al, we selected polyimides (PIs) as the mother chain and integrate different fluorophores onto the chain.…”

Section: Introductionmentioning

confidence: 99%

Multifunctional Flexible Polyimides for Electroactive Devices with Electrochromic, Electrofluorochromic, and Photodetection Properties

Zheng

Huang

Niu

et al. 2021

ACS Appl. Polym. Mater.

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In this study, we report three electroactive carbazolyl polyimides (PIs) containing spiropyran, pyrene, and fluorescein fluorescent groups. The PIs exhibit red, blue, and green fluorescence emissions, respectively. The PIs exhibit aggregation-induced emission and electrochromic (EC) and electrofluorochromic properties. Moreover, white light emission can be achieved by adjusting the mixing ratio of the three PIs. The PIs show high photoluminescence intensity in a solution and solid state. Interestingly, as the volume of ethyl acetate in the PI dimethyl sulfoxide solutions increases, the fluorescence intensity increases continuously. This is due to the decrease in solvent polarity and is distorted by the twisted intramolecular charge-transfer effect, enhancing the emission intensity. The PI films have excellent electrochemical stability between the neutral and first oxidation states of 2000 cycles, and their electrical activities are maintained at 99% CzpP-SPP, 99% CzpP-PREP, and 99% CzpP-FRNP. Under the action of an external electric field, the PIs exhibit excellent EC performance, and the highest EC efficiency was 187 cm 2 C −1 . Furthermore, the fluorescence and color switching between the oxidation state (nonfluorescent state) and reduced state (fluorescent state) of the PI films are reversible. This work provides a simple strategy for the direct functionalization of Cz-based materials and opens the way for exploring more applications of Cz-based materials.

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Multistate Redox Switching and Near-Infrared Electrochromism Based on a Star-Shaped Triruthenium Complex with a Triarylamine Core

Cited by 32 publications

References 52 publications

First-Principles Study on Redox Magnetism and Electrochromism of Cyclometalated Triarylamine-Core Triruthenium Complex

First-Principles Study on Redox Magnetism and Electrochromism of Cyclometalated Triarylamine-Core Triruthenium Complex

Photofunction‐Directed Coordination Molecular Engineering

Multifunctional Flexible Polyimides for Electroactive Devices with Electrochromic, Electrofluorochromic, and Photodetection Properties

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