Abstract
In the context of data storage miniaturization, it was recently shown that digital information can be stored in the monomer sequences of non-natural macromolecules. However, the sequencing of such digital polymers is currently limited to short chains. Here, we report that intact multi-byte digital polymers can be sequenced in a moderate resolution mass spectrometer and that full sequence coverage can be attained without requiring pre-analysis digestion or the help of sequence databases. In order to do so, the polymers are designed to undergo controlled fragmentations in collision-induced dissociation conditions. Each byte of the sequence is labeled by an identification tag and a weak alkoxyamine group is placed between 2 bytes. As a consequence of this design, the NO-C bonds break first upon collisional activation, thus leading to a pattern of mass tag-shifted intact bytes. Afterwards, each byte is individually sequenced in pseudo-MS3 conditions and the whole sequence is found.
Highlights
In the context of data storage miniaturization, it was recently shown that digital information can be stored in the monomer sequences of non-natural macromolecules
Two important molecular features are implemented in the analyte design: alkoxyamine groups are placed between the bytes and each byte is labeled by a mass tag
We have recently reported that non-natural digital oligomers constructed with repeating units containing alkoxyamine[9, 17] or carbamate[10] linkages are very easy to sequence by MS/MS due to the low-energy fragmentation of these bonds
Summary
In the context of data storage miniaturization, it was recently shown that digital information can be stored in the monomer sequences of non-natural macromolecules. We report that intact multi-byte digital polymers can be sequenced in a moderate resolution mass spectrometer and that full sequence coverage can be attained without requiring pre-analysis digestion or the help of sequence databases. Afterwards, each byte is individually sequenced in pseudo-MS3 conditions and the whole sequence is found It has been demonstrated in recent years that digital information can be stored in biological[1] and synthetic macromolecules[2]. In such digital polymers, the monomer units that constitute the chains are used as molecular bits and assembled through controlled synthesis into readable digital sequences[3]. In collision-induced dissociation (CID) conditions, the weak NO-C bonds are selectively cleaved, leading to a series of mass tag-shifted intact bytes. Full sequence coverage can be obtained in a single measurement performed in a moderate resolution mass spectrometer
Sign-in/Register to view highlights & summary 
Published Version (
Free)
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a call