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Cavity-Vibration Mixed States: Chemistry in Etalons

空腔振动混合态：标准具中的化学

基本信息

批准号：
1800414
负责人：
Jim Coe
金额：
$ 30万
依托单位：
Ohio State University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-08-15 至 2021-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800414&HistoricalAwards=false
关键词：
Cavity Vibration Mixed States Chemistry

项目摘要

Molecules typically vibrate at frequencies that correspond to infrared light (the wavelength range important in night vision technologies). Etalons are optical devices that consist of two parallel reflective metal plates whose spacing corresponds to infrared wavelengths (roughly 1 micrometer to 1 millimeter). If molecules are placed inside an etalon with just the right spacing, their vibrational properties can change. The molecule+cavity system is called a "mixed state", an interesting combination of light and matter. Since molecular vibrations have very important roles in how molecules undergo chemical reactions, there is the possibility that by simply changing cavity spacings, we can change vibrational properties of the molecules as well as their reactivity. In this project supported by the Chemical Structure, Dynamics and Mechanisms-A Program of the Division of Chemistry, Professor James Coe and his graduate students at The Ohio State University seek to demonstrate the feasibility of making mixed states of infrared etalon cavity modes and condensed phase vibrations to change reaction rates. "Chemistry in Etalons" would represent an entirely new field of chemistry, and may offer significant opportunities for producing chemicals more efficiently. The students involved in this project are gaining experience in both advanced optical spectroscopy and theoretical chemistry calculations. Professor Coe also plans to collaborate with professors at Cal State Dominguez Hills, which has an ethnically and economically diverse student body. The project begins with the construction of alignable and adjustable etalons in order to produce etalon fringes of variable width. The etalon is filled with a condensed phase material which has vibrations of interest. Etalon fringes are angle-tuned into resonance with the vibrations and an infrared transmission spectrum is recorded which enables the measurement of Rabi splittings--the energy difference between the mixed states of cavity and vibration. In order for the measured Rabi splittings to be related to fundamental quantum mechanical properties such as dipole derivatives, our models show that the etalon fringe width and vibrational transition width should be the same. Since vibrational features show a wide range of widths, there is a need to be able to carefully design etalons that match molecular vibrations. This project is focusing on: 1) the effect of etalon fringe width on measured Rabi splittings, 2) the conjugated double bond system of CO2 in water, and 3) broadened gas phase systems, all in order to establish the relation of these measurements to fundamental quantum mechanical properties. Finally, selected reactions are being studied within the wavelength-scale etalon cavity as informed by the previous results and as followed by infrared transmission spectra that allow assessment of whether the rates of reactions can be affected by mixed states of cavities and vibrations. While this project seeks fundamental insights into etalon-molecule mixed states, there is a potential for implications in a wide range of technological applications, including chemical and nanoparticle sensors, and even in heterogeneous catalysis (e.g., the etalon mirrors could serve as catalysts or catalyst supports).This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

分子的振动频率通常与红外线(夜视技术中重要的波长范围)相对应。标准具是由两个平行的反射金属板组成的光学设备，它们的间距对应于红外波长(大约1微米到1毫米)。如果分子以合适的间距放置在标准具内部，它们的振动特性就会改变。分子+空腔系统被称为“混合态”，是光和物质的有趣结合。由于分子振动在分子如何发生化学反应中起着非常重要的作用，因此有可能通过简单地改变空穴间距，我们就可以改变分子的振动性质以及它们的反应性。在这项由化学结构、动力学和机制-化学系计划支持的项目中，俄亥俄州立大学的James Coe教授和他的研究生试图证明利用红外标准具腔模和凝聚相振动的混合态来改变反应速率的可行性。“标准具中的化学”将代表一个全新的化学领域，并可能为更有效地生产化学品提供重要的机会。参与这个项目的学生在高级光学光谱学和理论化学计算方面都获得了经验。科教授还计划与加州州立多明格斯山庄的教授们合作，该校的学生群体在种族和经济上都不同。该项目首先建造可对准和可调节的标准具，以便产生宽度可变的标准具条纹。标准具填充了一种具有感兴趣的振动的凝聚相材料。标准具条纹被角度调谐成与振动的共振，并记录了红外透射谱，这使得能够测量拉比分裂--腔和振动的混合态之间的能量差。为了使测量的Rabi分裂与偶极导数等基本量子力学性质相关联，我们的模型表明标准具条纹宽度和振动跃迁宽度应该是相同的。由于振动特征显示的宽度范围很大，因此需要能够仔细设计与分子振动相匹配的标准具。这个项目的重点是：1)标准具条纹宽度对测量的Rabi分裂的影响，2)二氧化碳在水中的共轭双键系统，以及3)展宽的气相系统，所有这些测量都是为了建立这些测量与基本量子力学性质的关系。最后，根据先前的结果以及随后的红外透射谱，正在研究波长尺度标准具腔内选定的反应，以评估反应速率是否会受到腔和振动的混合态的影响。虽然这个项目寻求对标准具-分子混合状态的基本见解，但在包括化学和纳米粒子传感器在内的广泛技术应用中，甚至在非均相催化领域(例如，标准具反射镜可以用作催化剂或催化剂载体)，都有潜在的影响。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。