Escalation of polymerization in a thermal gradient
Open accessAbstract
For the emergence of early life, the formation of biopolymers such as RNA is essential. However, the addition of nucleotide monomers to existing oligonucleotides requires millimolar concentrations. Even in such optimistic settings, no polymerization of RNA longer than about 20 bases could be demonstrated. How then could self-replicating ribozymes appear, for which recent experiments suggest a minimal length of 200 nt? Here, we demonstrate a mechanism to bridge this gap: the escalated polymerization of nucleotides by a spatially confined thermal gradient. The gradient accumulates monomers by thermophoresis and convection while retaining longer polymers exponentially better. Polymerization and accumulation become mutually self-enhancing and result in a hyperexponential escalation of polymer length. We describe this escalation theoretically under the conservative assumption of reversible polymerization. Taking into account the separately measured thermophoretic properties of RNA, we extrapolate the results for primordial RNA polymerization inside a temperature gradient in pores or fissures of rocks. With a dilute, nanomolar concentration of monomers the model predicts that a pore length of 5 cm and a temperature difference of 10 K suffice to polymerize 200-mers of RNA in micromolar concentrations. The probability to generate these long RNAs is raised by a factor of >10 600 compared with polymerization in a physical equilibrium. We experimentally validate the theory with the reversible polymerization of DNA blocks in a laser-driven thermal trap. The results confirm that a thermal gradient can significantly enlarge the available sequence space for the emergence of catalytically active polymers.
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Temperature gradients across narrow channels can concentrate oligonucleotides, facilitating the assembly of longer DNA strands.
“Subsequent experiments have shown that temperature gradients across narrow channels can concentrate oligonucleotides, facilitating the assembly of longer DNA strands (Mast et al. 2013).”
From Protocells and RNA Self-Replication (2018) · cites this paper as Mast et al. 2013
Cites
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Self-citationRobust self-replication of combinatorial information via crystal growth and scission
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The Origin of Life in Alkaline Hydrothermal Vents
Sojo, V., Herschy, B., Whicher, A., Camprubí, E., & Lane, N. (2016) · Astrobiology · doi:10.1089/ast.2015.1406 · Cited by 341 · see citing works
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“However, research by the Braun group illustrates how nucleic acids might be concentrated in such a complex system (Mast et al., 2013).”
An origin-of-life reactor to simulate alkaline hydrothermal vents
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Heated gas bubbles enrich, crystallize, dry, phosphorylate and encapsulate prebiotic molecules
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Whicher, A., Camprubi, E., Pinna, S., Herschy, B., & Lane, N. (2018) · Origins of Life and Evolution of Biospheres · doi:10.1007/s11084-018-9555-8 · Cited by 81 · see citing works
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Self-citationThermal Habitat for RNA Amplification and Accumulation
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Self-citationPriye, A., Yu, Y., Hassan, Y. A., & Ugaz, V. M. (2017) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1612924114 · Cited by 18 · see citing works
- Authors
- Mast, C. B., Schink, S., Gerland, U., & Braun, D.
- Affiliations
- Center for NanoScience (DE)
- Venue
- Proceedings of the National Academy of Sciences
- Publisher
- National Academy of Sciences
- Published
- 2013-04-29
- Volume
- 110
- Issue
- 20
- Pages
- 8030-8035
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC3657786
- OpenAlex
- W2161899115
- Cited by
- 165
- References
- 5
- Citations by year
- 2026: 8 · 2025: 12 · 2024: 12 · 2023: 9 · 2022: 18 · 2021: 20 · 2020: 10 · 2019: 11 · 2018: 11 · 2017: 11 · 2016: 17 · 2015: 11 · 2014: 13 · 2013: 1
- FWCI
- 7.56
- Type
- journal article
- Language
- en
- Open access
- green
- www.ncbi.nlm.nih.gov
- Locations
- Proceedings of the National Academy of Sciences (publishedVersion)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- Topics
- Physical Sciences › Physics and Astronomy › Astronomy and Astrophysics › Origins and Evolution of Life
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › RNA and protein synthesis mechanisms
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Genetics › Evolution and Genetic Dynamics
- Keywords
- RNA polymerization, temperature gradient, thermophoresis, convection, nucleotide accumulation, origin of life, reversible polymerization, sequence spaces
- MeSH terms
- Biopolymers, Calibration, Catalysis, DNA, Geology, Kinetics, Nucleotides, RNA, Temperature, Water, Models, Statistical, RNA, Catalytic, Fluorescence Resonance Energy Transfer, Polymerization
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