Defining the Basis of Cyanine Phototruncation Enables a New Approach to Single-Molecule Localization Microscopy,ACS Central Science

当前位置： X-MOL 学术 › ACS Cent. Sci. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Defining the Basis of Cyanine Phototruncation Enables a New Approach to Single-Molecule Localization Microscopy
ACS Central Science ( IF 12.7 ) Pub Date : 2021-06-03 , DOI: 10.1021/acscentsci.1c00483
Siddharth S Matikonda ₁ , Dominic A Helmerich ₂ , Mara Meub ₂ , Gerti Beliu ₂ , Philip Kollmannsberger ₃ , Alexander Greer _{4,

5} , Markus Sauer ₂ , Martin J Schnermann ₁

Affiliation

The light-promoted conversion of extensively used cyanine dyes to blue-shifted emissive products has been observed in various contexts. However, both the underlying mechanism and the species involved in this photoconversion reaction have remained elusive. Here we report that irradiation of heptamethine cyanines provides pentamethine cyanines, which, in turn, are photoconverted to trimethine cyanines. We detail an examination of the mechanism and substrate scope of this remarkable two-carbon phototruncation reaction. Supported by computational analysis, we propose that this reaction involves a singlet oxygen-initiated multistep sequence involving a key hydroperoxycyclobutanol intermediate. Building on this mechanistic framework, we identify conditions to improve the yield of photoconversion by over an order of magnitude. We then demonstrate that cyanine phototruncation can be applied to super-resolution single-molecule localization microscopy, leading to improved spatial resolution with shorter imaging times. We anticipate these insights will help transform a common, but previously mechanistically ill-defined, chemical transformation into a valuable optical tool.

中文翻译：

定义花青光截断的基础使单分子定位显微镜的新方法成为可能

已在各种情况下观察到广泛使用的花青染料在光促进下转化为蓝移发光产品。然而，涉及这种光转化反应的潜在机制和物种仍然难以捉摸。在这里我们报告七次甲基花青的辐照提供五次甲基花青，反过来，它被光转化为三甲基花青。我们详细研究了这种显着的双碳光截断反应的机制和底物范围。在计算分析的支持下，我们提出该反应涉及单线态氧引发的多步序列，涉及关键的氢过氧环丁醇中间体。在此机制框架的基础上，我们确定了将光转换产量提高一个数量级的条件。然后，我们证明花青光截断可以应用于超分辨率单分子定位显微镜，从而以更短的成像时间提高空间分辨率。我们预计这些见解将有助于将一种常见但以前在机械上定义不明确的化学转化转变为一种有价值的光学工具。

更新日期：2021-07-28

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南