Search for: All records

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. 

Chemical mixtures can be leveraged to store large amounts of data in a highly compact form and have the potential for massive scalability owing to the use of large-scale molecular libraries. With the parallelism that comes from having many species available, chemical-based memory can also provide the physical substrate for computation with increased throughput. Here, we represent non-binary matrices in chemical solutions and perform multiple matrix multiplications and additions, in parallel, using chemical reactions. As a case study, we demonstrate image processing, in which small greyscale images are encoded in chemical mixtures and kernel-based convolutions are performed using phenol acetylation reactions. In these experiments, we use the measured concentrations of reaction products (phenyl acetates) to reconstruct the output image. In addition, we establish the chemical criteria required to realize chemical image processing and validate reaction-based multiplication. Most importantly, this work shows that fundamental arithmetic operations can be reliably carried out with chemical reactions. Our approach could serve as a basis for developing more advanced chemical computing architectures. 

Autocatalysis is fundamental to many biological processes, and kinetic models of autocatalytic reactions have mathematical forms similar to activation functions used in artificial neural networks. Inspired by these similarities, we use an autocatalytic reaction, the copper-catalyzed azide–alkyne cycloaddition, to perform digital image recognition tasks. Images are encoded in the concentration of a catalyst across an array of liquid samples, and the classification is performed with a sequence of automated fluid transfers. The outputs of the operations are monitored using UV-vis spectroscopy. The growing interest in molecular information storage suggests that methods for computing in chemistry will become increasingly important for querying and manipulating molecular memory. 

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.