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Chemistry is considered as one of the more promising applications to science of near-term quantum computing. Recent work in transitioning classical algorithms to a quantum computer has led to great strides in improving quantum algorithms and illustrating their quantum advantage. Because of the limitations of near-term quantum computers, the most effective strategies split the work over classical and quantum computers. There is a proven set of methods in computational chemistry and materials physics that has used this same idea of splitting a complex physical system into parts that are treated at different levels of theory to obtain solutions for the complete physical system for which a brute force solution with a single method is not feasible. These methods are variously known as embedding, multi-scale, and fragment techniques and methods. We review these methods and then propose the embedding approach as a method for describing complex biochemical systems, with the parts not only treated with different levels of theory, but computed with hybrid classical and quantum algorithms. Such strategies are critical if one wants to expand the focus to biochemical molecules that contain active regions that cannot be properly explained with traditional algorithms on classical computers. While we do not solve this problem here, we provide an overview of where the field is going to enable such problems to be tackled in the future. 

We herein describe a new design principle to achieve B/N‐doped cyclophane where an electron‐donor block of three triarylamines (Ar₃N) and an acceptor block of three triarylboranes (Ar₃B) are spatially separated on opposite sides of the π‐extended ring system. DFT computations revealed the distinct electronic structure of theblock‐type macrocycleMC‐b‐B3N3with a greatly enhanced dipole moment and reduced HOMO–LUMO energy gap in comparison to its analogue with alternating B and N sites,MC‐alt‐B3N3. The unique arrangement of borane acceptor Ar₃B and amine donor Ar₃N components inMC‐b‐B3N3induces exceptionally strong intramolecular charge transfer in the excited state, which is reflected in a largely red‐shifted luminescence at 612 nm in solution. The respective linear open‐chain oligomerL‐b‐B3N3was also synthesized for comparison. Our new approach to donor–acceptor macrocycles offers important fundamental insights and opens up a new avenue to unique optoelectronic materials.

 

We herein describe a new design principle to achieve B/N‐doped cyclophane where an electron‐donor block of three triarylamines (Ar₃N) and an acceptor block of three triarylboranes (Ar₃B) are spatially separated on opposite sides of the π‐extended ring system. DFT computations revealed the distinct electronic structure of theblock‐type macrocycleMC‐b‐B3N3with a greatly enhanced dipole moment and reduced HOMO–LUMO energy gap in comparison to its analogue with alternating B and N sites,MC‐alt‐B3N3. The unique arrangement of borane acceptor Ar₃B and amine donor Ar₃N components inMC‐b‐B3N3induces exceptionally strong intramolecular charge transfer in the excited state, which is reflected in a largely red‐shifted luminescence at 612 nm in solution. The respective linear open‐chain oligomerL‐b‐B3N3was also synthesized for comparison. Our new approach to donor–acceptor macrocycles offers important fundamental insights and opens up a new avenue to unique optoelectronic materials.