Servier Research Institute of Medicinal Chemistry, H-1031 Budapest, Hungary.
Hevesy György PhD School of Chemistry, Eötvös Loránd University, H-1053 Budapest, Hungary.
J Am Chem Soc. 2022 Oct 19;144(41):19078-19088. doi: 10.1021/jacs.2c08135. Epub 2022 Oct 7.
Information storage at the molecular level commonly entails encoding in the form of ordered sequences of different monomers and subsequent fragmentation and tandem mass spectrometry analysis to read this information. Recent approaches also include the use of mixtures of distinct molecules noncovalently bonded to one another. Here, we present an alternate isotope ratio encoding approach utilizing deuterium-labeled monomers to produce hundreds of oligomers endowed with unique isotope distribution patterns. Mass spectrometric recognition of these patterns then allowed us to directly readout encoded information with high fidelity. Specifically, we show that all 256 tetramers composed of four different monomers of identical constitution can be distinguished by their mass fingerprint using mono-, di-, tri-, and tetradeuterated building blocks. The method is robust to experimental errors and does not require the most sophisticated mass spectrometry instrumentation. Such isotope ratio-encoded oligomers may serve as tags that carry information, but the method mainly opens up the capability to write information, for example, about molecular identity, directly into a pure compound via its isotopologue distribution obviating the need for additional tagging and avoiding the use of mixtures of different molecules.
信息在分子水平上的存储通常需要以不同单体的有序序列的形式进行编码，然后进行碎片化和串联质谱分析，以读取这些信息。最近的方法还包括使用非共价键彼此连接的不同分子的混合物。在这里，我们提出了一种替代的同位素比编码方法，利用氘标记的单体来产生数百种具有独特同位素分布模式的寡聚物。然后，通过质谱对这些模式的识别，我们可以直接以高保真度读出编码信息。具体来说，我们表明，使用单、二、三、四氘代构建块，可以通过质量指纹图区分由相同组成的四个不同单体组成的所有 256 个四聚体。该方法对实验误差具有鲁棒性，并且不需要最复杂的质谱仪器。这种同位素比编码的寡聚物可以作为携带信息的标签，但该方法主要开辟了通过其同位素分布将信息直接写入纯化合物的能力，从而无需额外的标记，并避免使用不同分子的混合物。
