ConspectusWhen molecular vibrational modes strongly couple to virtual states of photonic modes, new molecular vibrational polariton states are formed, along with a large population of dark reservoir modes. The polaritons are much like the bonding and antibonding molecular orbitals when atomic orbitals form molecular bonds, while the dark modes are like nonbonding orbitals. Because the polariton states are half-matter and half-light, whose energy is shifted from the parental states, polaritons are predicted to modify chemistry under thermally activated conditions, leading to an exciting and emerging field known as polariton chemistry that could potentially shift paradigms in chemistry. Despite several published results supporting this concept, the chemical physics and mechanism of polariton chemistry remain elusive. One reason for this challenge is that previous works cannot differentiate polaritons from dark modes. This limitation makes delineating the contributions to chemistry from polaritons and dark states difficult. However, this level of insight is critical for developing a solid mechanism for polariton chemistry to design and predict the outcome of strong coupling with any given reaction. My group addressed the challenge of differentiating the dynamics of polaritons and dark modes by ultrafast two-dimensional infrared (2D IR) spectroscopy. Specifically, (1) we found that polaritons can facilitate intra- and intermolecular vibrational energy transfer, opening a pathway to control vibrational energy flow in liquid-phase molecular systems, and (2) by studying a single-step isomerization event, we verified that indeed polaritons can modify chemical dynamics under strong coupling conditions, but in contrast, the dark modes behave like uncoupled molecules and do not change the dynamics. This finding confirmed the central concept of polariton chemistry: polaritons modify the potential energy landscape of reactions. The result also clarified the role of dark modes, which lays a critical foundation for designing cavities for future polariton chemistry. Aside from using 2D IR spectroscopy to study polariton chemistry, we also used the same technique to develop molecular polaritons into a potential quantum simulation platform. We demonstrated that polaritons have Rabi oscillations, and using a checkerboard cavity design, we showed that polaritons could have large nonlinearity across space. We further used the checkerboard polaritons to simulate coherence transfer and visualize it. A unidirectional coherence transfer was observed, indicating non-Hermitian dynamics. The highlighted efforts in this Account provide a solid understanding of the capability of polaritons for chemistry and quantum information science. I conclude this Account by discussing a few challenges for moving polariton chemistry toward being predictable and making the polariton quantum platform a complement to existing systems.

Wei Xiong

Accounts of Chemical Research

ACCOUNTS OF CHEMICAL RESEARCH 提供简短、简洁和批判性的文章，提供化学和生物化学所有领域的基础研究和应用的易于阅读的概述。此外，ACCOUNTS OF CHEMICAL RESEARCH 还出版了专门针对具有不寻常活动和意义的单一问题的特刊。访问 ACCOUNTS SPECIAL ISSUES 页面，查看所有特殊问题的列表、描述和 TOC。从 2008 年开始，ACCOUNTS OF CHEMICAL RESEARCH 将其传统的文章摘要替换为文章“CONSPECTUS”。这些新条目概述了研究，使读者可以更仔细地了解文章的内容和意义。通过对文章内容的更详细描述，CONSPECTUS 提高了文章在搜索引擎中的可发现性和研究的曝光率。

Accounts of Chemical Research publishes concise, clear, and critical articles that provide accessible overviews of fundamental research and applications across all areas of chemistry and biochemistry. Additionally, Accounts of Chemical Research publishes special issues focused on single topics of unusual activity and significance. You can visit the Accounts of Chemical Research Special Issues page to view a list of all special issues, their descriptions, and tables of contents. Since 2008, Accounts of Chemical Research has replaced traditional article abstracts with 'CONSPECTUS.' These new entries summarize the research, allowing readers to gain a deeper understanding of the content and significance of the articles. By providing a more detailed description of the article content, CONSPECTUS enhances the discoverability of articles in search engines and increases the visibility of the research.

《Accounts of Chemical Research》提供简短、清晰且具有批判性的文章，涵盖化学和生物化学各个领域的基础研究和应用，旨在为读者提供易于理解的概述。此外，《Accounts of Chemical Research》还出版专门针对具有特殊活动和重要性的单一主题的特刊。您可以访问《Accounts of Chemical Research》特刊页面，查看所有特刊的列表、描述和目录。从2008年开始，《Accounts of Chemical Research》将传统的文章摘要替换为“CONSPECTUS”，这些新条目概述了研究内容，使读者能够更深入地理解文章的内容和意义。通过对文章内容的详细描述，CONSPECTUS提高了文章在搜索引擎中的可发现性和研究的曝光率。

Category	Quartile
化学	1
化学, 化学综合	1

Molecular Vibrational Polariton Dynamics: What Can Polaritons Do?

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Category	Quartile
CHEMISTRY, MULTIDISCIPLINARY	1