New Wine in Old Bottle: Crown Ether-Functionalized Digital Polymer toward Efficient MALDI-TOF MS/MS Decoding via a...

Area of Science:

• Polymer Chemistry
• Supramolecular Chemistry
• Analytical Chemistry

Background:

• Digital polymers (DPs) are promising for molecular data storage.
• Efficient synthesis and sequencing are crucial for DP applications.
• Current sequencing methods using weak bonds limit DP length and storage capacity.

Purpose of the Study:

• To improve the readability and fidelity of tandem mass spectrometry (MS/MS) for digital polymers.
• To enhance the information storage capacity of DPs by enabling longer polymer chains.
• To develop a novel strategy for decoding digital polymer sequences.

Main Methods:

• Introducing crown ether (CE) moieties at the terminus of digital oligo(γ-butyrolactone)s (DOBLs).
• Utilizing the supramolecular interaction between CE and alkali cations for selective fragmentation.
• Analyzing long-chain DPs (up to 32-mer) using matrix-assisted laser desorption/ionization time-of-flight tandem mass spectrometry (MALDI-TOF MS/MS).

Main Results:

• Crown ether incorporation significantly enhanced the predictability and fidelity of MALDI-TOF MS/MS spectra.
• The CE-mediated selective fragmentation improved the decoding process for DPs.
• The method successfully analyzed long-chain DPs up to 32-mer with customizable fragmentation patterns.

Conclusions:

• Crown ether functionalization is a novel and effective strategy for improving MS/MS readability of DPs.
• This approach overcomes limitations of previous methods, enabling longer DP chains and higher information storage density.
• The study presents a significant advancement in polymer-based data storage technology.