A new scheme for significant enhancement of the second order nonlinear optical response from molecules to ordered aggregates
文献信息
Weiqi Li, Xin Zhou, Wei Quan Tian, Xiudong Sun
How to achieve maximum nonlinear optical (NLO) properties from the molecular to the macro block is very crucial to the development of nonlinear optical materials, which is the impetus of the present work. Buckybowls present large first hyperpolarizability ascribed to noncentrosymmetric charge distribution due to the curved shape of the system. The role of their packing pattern in maximizing the NLO response of buckybowl aggregates is investigated. In (corannulene)10 and (sumanene)10 aggregates, the first order hyperpolarizabilities (β0) per molecule are enhanced 5.59 and 6.21 times with respect to a single entity respectively. For a larger buckybowl, C36H12, the β0 value per molecule of its pentamer reaches 191.4 × 10−30 esu which is much higher than conventional dipolar or octupolar NLO chromophores ones. The cohesive coupling among electric dipoles in packing of buckybowls is responsible for significant enhancement of the nonlinear optical response of the aggregates, which could pave the way for designing large 2nd order NLO materials with a good balance of nonlinearity, transparency, and stability.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.














