量子官能团的振动工程。

IF 16.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Haowen Zhou, Taras Khvorost, Anastassia N Alexandrova, Justin R Caram
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引用次数: 0

摘要

化学家对官能团的概念有一个坚定的理解:一个小的分子片段,赋予属性(反应性、溶解度和化学识别)到一个更大的支架上。类似地,量子官能团(QFG)将作为一个孤立的“量子手柄”,可以附着在扩展的分子上,并实现量子态的制备和测量(SPAM)。然而,与分子化学相关的复杂性往往与非热态制备的要求不一致。分子的其余部分充当局部浴,在激发和弛豫时导致失相和量子信息的丢失。然而,存在巨大的潜在化学键基序的化学空间来设计孤立的qfg。本帐户的目标是探索优化QFG性能的潜在化学设计原则。对于典型的状态制备,使用一个应用场将量子比特置于特定的已知状态(通过光循环和激光冷却),在那里它可以被操纵或与其他物种纠缠。相同的字段(或其他字段)可用于读取或报告操作结束时的量子位状态。例如,在被捕获的离子/中性原子中,状态制备是通过使用窄带激光泵送特定的跃迁来完成的。从那里,可以通过选择性射频或激光激发对量子比特进行进一步的操作,并且可以通过荧光读出状态。然而,将这种模式扩展到分子系统是非常具有挑战性的:分子有更多的自由度,可以耦合到吸收或发射场。要克服这一问题,需要通过合理选择QFG和分子底物的振动工程,极大地限制这些“非对角线”衰变途径的数量。我们的工作表明,碱土(I)烷氧化物(MOR)可以满足高效SPAM的必要要求。特别是,我们利用了-OM (M = Ca, Sr)基序,它作为一个量子手柄,已经连接到各种脂肪族和芳香烃上。光学循环特性的精确分解依赖于熟悉的化学概念,包括共轭、构象、吸电子能力和对称性。在这篇文章中,我们回顾了该领域最近在构建qfg和共同设计分子支架方面的努力,这些分子支架可以在不破坏其所需量子特性的情况下承载它们。qfg被探索作为光开关支架的附件,并成对地安装在更大的主机上。从费米共振到超辐射,已经探索了与这些qfg作为量子比特的能力相关的各种物理现象。因此,我们开始推导针对QFG功能的振动工程的第一套规则。展望了通过分子和材料设计来增加量子光纤的数量和密度。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Vibronic Engineering for Quantum Functional Groups.

ConspectusChemists have a firm understanding of the concept of a functional group: a small molecular moiety that confers properties (reactivity, solubility, and chemical recognition) onto a larger scaffold. Analogously, a quantum functional group (QFG) would act as an isolated "quantum handle" that could attach onto an extended molecule and enable quantum state preparation and measurement (SPAM). However, the complexity associated with molecular chemistry is often at odds with the requirements of nonthermal state preparation. The rest of the molecule acts as a local bath that leads to dephasing and loss of quantum information upon excitation and relaxation. Yet, there exists an enormous chemical space of potential chemical bonding motifs to design isolated QFGs. The goal of this Account is to explore the underlying chemical design principles for the optimization of QFG performance.For typical state preparation, an applied field is used to put the qubit into a specific known state (via optical cycling and laser cooling), where it can be manipulated or entangled with other species. That same field (or another) can be used to read out or report on the qubit state at the end of the operation. For example, in trapped ions/neutral atoms, state preparation is accomplished by pumping a specific transition using a narrowband laser. From there, further operations can be performed on the qubit via selective RF or laser excitation, and the state can be read out via fluorescence. However, extending this paradigm to molecular systems is highly challenging: molecules have many more degrees of freedom that can couple to the absorbed or emitted field. Overcoming this requires greatly limiting the number of these "off-diagonal" decay pathways through the judicious selection of the QFG and vibronic engineering of the molecular substrate.Our work has demonstrated that alkaline-earth (I) alkoxides (MOR) may meet the necessary requirements for efficient SPAM. In particular, we capitalize on the -OM (M = Ca, Sr) motif, which acts as a quantum handle that has been attached to a variety of aliphatic and aromatic hydrocarbons. The precise breakdown of the optical cycling property depends on familiar chemical concepts, including conjugation, conformer formation, electron-withdrawing abilities, and symmetry. In this Account, we review the recent efforts in the field to construct QFGs and codesign molecular scaffolds that can host them without destruction of their desired quantum properties. QFGs are explored as attachments to photoswitching scaffolds and mounted in pairs to larger hosts. A variety of physical phenomena relevant to the ability of these QFGs to function as qubits, from Fermi resonances to super radiance, have been explored. We thus began deriving the first set of rules for vibronic engineering toward the QFG functionality. Prospects toward increasing the number densities of these QFGs through molecular and material design are also presented.

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来源期刊
Accounts of Chemical Research
Accounts of Chemical Research 化学-化学综合
CiteScore
31.40
自引率
1.10%
发文量
312
审稿时长
2 months
期刊介绍: Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.
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