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null (Ed.)Abstract Data encoded in molecules offers opportunities for secret messaging and extreme information density. Here, we explore how the same chemical and physical dimensions used to encode molecular information can expose molecular messages to detection and manipulation. To address these vulnerabilities, we write data using an object’s pre-existing surface chemistry in ways that are indistinguishable from the original substrate. While it is simple to embed chemical information onto common objects (covers) using routine steganographic permutation, chemically embedded covers are found to be resistant to detection by sophisticated analytical tools. Using Turbo codes for efficient digital error correction, we demonstrate recovery of secret keys hidden in the pre-existing chemistry of American one dollar bills. These demonstrations highlight ways to improve security in other molecular domains, and show how the chemical fingerprints of common objects can be harnessed for data storage and communication.more » « less
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Rosenstein, Jacob K.; Rose, Christopher; Reda, Sherief; Weber, Peter M.; Kim, Eunsuk; Sello, Jason; Geiser, Joseph; Kennedy, Eamonn; Arcadia, Christopher; Dombroski, Amanda; et al (, IEEE Transactions on NanoBioscience)
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Arcadia, Christopher E.; Kennedy, Eamonn; Geiser, Joseph; Dombroski, Amanda; Oakley, Kady; Chen, Shui-Ling; Sprague, Leonard; Ozmen, Mustafa; Sello, Jason; Weber, Peter M.; et al (, Nature Communications)Abstract Multicomponent reactions enable the synthesis of large molecular libraries from relatively few inputs. This scalability has led to the broad adoption of these reactions by the pharmaceutical industry. Here, we employ the four-component Ugi reaction to demonstrate that multicomponent reactions can provide a basis for large-scale molecular data storage. Using this combinatorial chemistry we encode more than 1.8 million bits of art historical images, including a Cubist drawing by Picasso. Digital data is written using robotically synthesized libraries of Ugi products, and the files are read back using mass spectrometry. We combine sparse mixture mapping with supervised learning to achieve bit error rates as low as 0.11% for single reads, without library purification. In addition to improved scaling of non-biological molecular data storage, these demonstrations offer an information-centric perspective on the high-throughput synthesis and screening of small-molecule libraries.more » « less
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