Storing and Reading Information in Mixtures of Fluorescent Molecules

Nagarkar, Amit A.; Root, Samuel E.; Fink, Michael; Ten, Alexei S.; Cafferty, Brian J.; Richardson, Douglas S.; Mrksich, Milan; Whitesides, George M.

doi:10.1021/acscentsci.1c00728

Cited by 39 publications

(39 citation statements)

References 44 publications

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“…Recently, Whitesides et al used inkjet printing to create fluorescent patterns for long-term data storage. [40] While the authors required seven different dyes to store 8-bit information in one pixel, in our approach, we can create >256 distinguishable ratios in one spot by using only two fluorophores. To achieve this, we screened many nested lasing parameter gradients (Figure S48, Supporting Information) to obtain optimum parameters for a precise red-green color mixing.…”

Section: Laser-based Synthesis Of Fluorophore Microarraysmentioning

confidence: 99%

Automated Laser‐Transfer Synthesis of High‐Density Microarrays for Infectious Disease Screening

et al. 2022

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Laser‐induced forward transfer (LIFT) is a rapid laser‐patterning technique for high‐throughput combinatorial synthesis directly on glass slides. A lack of automation and precision limits LIFT applications to simple proof‐of‐concept syntheses of fewer than 100 compounds. Here, an automated synthesis instrument is reported that combines laser transfer and robotics for parallel synthesis in a microarray format with up to 10 000 individual reactions cm−2. An optimized pipeline for amide bond formation is the basis for preparing complex peptide microarrays with thousands of different sequences in high yield with high reproducibility. The resulting peptide arrays are of higher quality than commercial peptide arrays. More than 4800 15‐residue peptides resembling the entire Ebola virus proteome on a microarray are synthesized to study the antibody response of an Ebola virus infection survivor. Known and unknown epitopes that serve now as a basis for Ebola diagnostic development are identified. The versatility and precision of the synthesizer is demonstrated by in situ synthesis of fluorescent molecules via Schiff base reaction and multi‐step patterning of precisely definable amounts of fluorophores. This automated laser transfer synthesis approach opens new avenues for high‐throughput chemical synthesis and biological screening.

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Section: Laser-based Synthesis Of Fluorophore Microarraysmentioning

confidence: 99%

Automated Laser‐Transfer Synthesis of High‐Density Microarrays for Infectious Disease Screening

et al. 2022

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“…Writing (encoding) information at the molecular level can be achieved with either (i) sequences of monomers concatenated within one molecular string 7 – 12 or with (ii) mixtures of individual, unique compounds 19 – 23 . For both, there is a trade-off between synthetic difficulty, material demands, and information capacity.…”

Section: Introductionmentioning

confidence: 99%

“…Long sequences can be made from a few monomers, but synthetic writing is difficult, slow, and prone to errors 7 – 9 . On the other hand, mixtures are easy to make but require a high number of uniquely distinguishable components, which eventually become a limiting factor 19 – 23 . Theoretically, an alternative approach, better balancing the need to generate many codes with a small number of components and synthetic steps, is (iii) to first synthesize short sequences and then use them as unique components in mixtures.…”

Section: Introductionmentioning

confidence: 99%

“…Another challenge for spectroscopic methods are signal overlaps that limit the number of distinguishable codes. For example, fluorescent labels, as one of the most important tools for interrogation of biological systems, provide relatively broad signals within a narrow spectral window 23 – 26 . Up to ten different fluorescent tags can be distinguished from mixtures with advanced computational methods, but this still amounts only to 2 10 – 1 = 1023 codes 26 .…”

Section: Introductionmentioning

confidence: 99%

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Paramagnetic encoding of molecules

et al. 2022

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Contactless digital tags are increasingly penetrating into many areas of human activities. Digitalization of our environment requires an ever growing number of objects to be identified and tracked with machine-readable labels. Molecules offer immense potential to serve for this purpose, but our ability to write, read, and communicate molecular code with current technology remains limited. Here we show that magnetic patterns can be synthetically encoded into stable molecular scaffolds with paramagnetic lanthanide ions to write digital code into molecules and their mixtures. Owing to the directional character of magnetic susceptibility tensors, each sequence of lanthanides built into one molecule produces a unique magnetic outcome. Multiplexing of the encoded molecules provides a high number of codes that grows double-exponentially with the number of available paramagnetic ions. The codes are readable by nuclear magnetic resonance in the radiofrequency (RF) spectrum, analogously to the macroscopic technology of RF identification. A prototype molecular system capable of 16-bit (65,535 codes) encoding is presented. Future optimized systems can conceivably provide 64-bit (~10^19 codes) or higher encoding to cover the labelling needs in drug discovery, anti-counterfeiting and other areas.

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“…Color-tunable light-emitting materials, especially in their aggregate state 1,2 , are of increasing interest due to their potential in various applications including fluorescent sensing 3,4 and imaging 5,6 , multicolor displays 7 , information encryption [8][9][10][11] and data storage 12 . Within the family of multicolor emissive materials, polymers offer highly flexible structural design and outstanding processability [13][14][15] .…”

Section: Introductionmentioning

confidence: 99%

Machine Learning-assisted Exploration of a Universal Polymer Platform with Charge Transfer-dependent Full-color Emission

Meftahi

Lyskov

et al. 2022

Preprint

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Understanding the color tuning of solid-state emissive materials is essential from a fundamental mechanistic viewpoint, as well as for practical applications. The development of color-tunable fluorescent materials with simple chemical compositions and easy to synthesize is highly desirable, but practically challenging. Despite copious research into molecular design and engineering, a general and facile polymer platform that offers high flexibility and broad extensibility in emission color tuning is still lacking. Here, we report a universal yet simple platform based on through-space charge transfer (TSCT) polymers, that has full-color tunable emission and was developed with the aid of predictive machine learning models. Using a single acceptor (A) fluorophore as the initiator for atom transfer radical polymerization (ATRP), a series of electron donor (D) groups containing simple polycyclic aromatic moieties (e.g., pyrene) are introduced either by one-step copolymerization or by end-group functionalization of a pre-synthesized polymer. By manipulating donor-acceptor (D-A) interactions via controlled polymer synthesis, continuous blue-to-red emission color tuning was easily achieved in solid polymers. Theoretical investigations confirm the structurally dependent TSCT-induced emission redshifts. We also exemplify how these TSCT polymers can be used as a general design platform for solid-state stimuli-responsive materials with high-contrast photochromic emission, by applying them to proof-of-concept information encryption.

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Storing and Reading Information in Mixtures of Fluorescent Molecules

Cited by 39 publications

References 44 publications

Automated Laser‐Transfer Synthesis of High‐Density Microarrays for Infectious Disease Screening

Automated Laser‐Transfer Synthesis of High‐Density Microarrays for Infectious Disease Screening

Paramagnetic encoding of molecules

Machine Learning-assisted Exploration of a Universal Polymer Platform with Charge Transfer-dependent Full-color Emission

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