A5089648168- Origins and Evolution of Life
- thermodynamics and calorimetric analyses
- Advanced Thermodynamics and Statistical Mechanics
- RNA and protein synthesis mechanisms
- Nanopore and Nanochannel Transport Studies
- Bacteriophages and microbial interactions
- Field-Flow Fractionation Techniques
- Protein Structure and Dynamics
- DNA and Nucleic Acid Chemistry
- Enzyme Structure and Function
- Microfluidic and Capillary Electrophoresis Applications
- Photoreceptor and optogenetics research
- RNA Interference and Gene Delivery
- Methane Hydrates and Related Phenomena
- Protist diversity and phylogeny
- ATP Synthase and ATPases Research
- Genomics and Phylogenetic Studies
- Biofield Effects and Biophysics
- Advanced biosensing and bioanalysis techniques
- Chemical Synthesis and Analysis
- Supramolecular Self-Assembly in Materials
- DNA and Biological Computing
- Bacterial Genetics and Biotechnology
- Renin-Angiotensin System Studies
- Chemical Reactions and Isotopes
Ludwig-Maximilians-Universität München
2016-2025
Center for NanoScience
2011-2024
Nanosystems Initiative Munich
2016-2023
Abstract The emergence of biopolymer building blocks is a crucial step during the origins life 1–6 . However, all known formation pathways rely on rare pure feedstocks and demand successive purification mixing steps to suppress unwanted side reactions enable high product yields. Here we show that heat flows through thin, crack-like geo-compartments could have provided widely available yet selective mechanism separates more than 50 prebiotically relevant from complex mixtures amino acids,...
For the emergence of early life, formation biopolymers such as RNA is essential. However, addition nucleotide monomers to existing oligonucleotides requires millimolar concentrations. Even in optimistic settings, no polymerization longer than about 20 bases could be demonstrated. How then self-replicating ribozymes appear, for which recent experiments suggest a minimal length 200 nt? Here, we demonstrate mechanism bridge this gap: escalated nucleotides by spatially confined thermal gradient....
The hallmark of living matter is the replication genetic molecules and their active storage against diffusion. We implement both in simple nonequilibrium environment a temperature gradient. Convective flow drives DNA replicating polymerase chain reaction while concurrent thermophoresis accumulates replicated 143 base pair bulk solution. time constant for accumulation 92 s doubled every 50 s. experiments explore conditions pores hydrothermal rock which can serve as model origin life.
Abstract Key requirements for the first cells on Earth include ability to compartmentalize and evolve. Compartmentalization spatially localizes biomolecules from a dilute pool an evolving cell, which, as it grows divides, permits mixing propagation of information daughter cells. Complex coacervate microdroplets are excellent candidates primordial with partition concentrate molecules into their core support primitive complex biochemical reactions. However, evolution protocells by fusion,...
How life developed in its earliest stages is a central but notoriously difficult question science. The lifeforms likely used reduced set of codon sequences that were progressively completed over time, driven by chemical, physical, and combinatorial constraints. However, despite importance for prebiotic chemistry, UV radiation has not been considered selection pressure the evolution early sequences. In this proof-of-principle study, we quantified susceptibility large pools DNA protogenomes...
Abstract Recent progress in the synthesis of nucleotides from prebiotically plausible precursors has opened up new ways to explain origin genetic matter. Mechanisms for polymerization without help catalysts are, however, rare. Complementary experiments done by Costanzo et al., we found that drying 3′,5′‐cyclic GMP leads poly‐G RNA strands with lengths 40 nucleotides. We also show long is considerably more efficient under dry conditions than cGMP water. The length depends on incubation time...
Abstract For the emergence of life, abiotic synthesis RNA from its monomers is a central step. We found that in alkaline, drying conditions bulk and at heated air‐water interfaces, 2′,3′‐cyclic nucleotides oligomerised without additional catalyst, forming up to 10‐mers within day. The oligomerisation proceeded pH range 7–12, temperatures between 40–80 °C was marginally enhanced by K + ions. Among canonical ribonucleotides, cGMP most efficiently. Quantification performed using HPLC coupled...
Abstract Dew is a common form of water that deposits from saturated air on colder surfaces. Although presumably primordial Earth, its potential involvement in the origin life early replication has not been investigated detail. Here we report it can drive first stages Darwinian evolution for DNA and RNA, by periodically denaturing their structures at low temperatures second promoting long strands over short, faster replicating ones. Our experiments mimicked partially water-filled rock pore...
Abstract Proton gradients are essential for biological systems. They not only drive the synthesis of ATP, but initiate molecule degradation and recycling inside lysosomes. However, high mobility permeability protons through membranes make pH very hard to sustain in vitro. Here we report that heat flow across a water-filled chamber forms sustains stable gradients. Charged molecules accumulate by convection thermophoresis better than uncharged species. In dissociation reaction, this imbalances...
The RNA world scenario posits replication by polymerases. On early Earth, a geophysical setting is required to separate hybridized strands after their and localize them against diffusion. We present pointed heat source that drives exponential, RNA-catalyzed amplification of short with high efficiency in confined chamber. While shorter were periodically melted laminar convection, the temperature gradient caused aggregated polymerase molecules accumulate, protecting from degradation hot...
Life is based on informational polymers such as DNA or RNA. For their polymerization, high concentrations of complex monomer building blocks are required. Therefore, the dilution by diffusion poses a major problem before early life could establish non-equilibrium compartmentalization. Here, we explored natural habitat to polymerize RNA and DNA. A heat flux across thin rock cracks shown accumulate maintain nucleotides. This boosts polymerization inside crack. Moreover, remain localized,...
Templated ligation offers an efficient approach to replicate long strands in RNA world. The 2′,3′-cyclic phosphate (>P) is a prebiotically available activation that also forms during hydrolysis. Using gel electrophoresis and high-performance liquid chromatography, we found the templated of with >P proceeds simple low-salt aqueous solutions 1 mM MgCl2 under alkaline pH ranging from 9 11 temperatures −20 25 °C. No additional catalysts were required. In contrast previous reports, increase...
Abstract Phosphorus is an essential building block of life, likely since its beginning. Despite this importance for prebiotic chemistry, phosphorus was scarce in Earth’s rock record and mainly bound poorly soluble minerals, with the calcium-phosphate mineral apatite as key example. While specific chemical boundary conditions have been considered to address so-called phosphate problem, a fundamental process that solubilizes enriches from geological sources remains elusive. Here, we show...
Phosphorus is an essential element of life, as observable in modern life forms that have perfected phosphorus accumulation and recycling. Prebiotic chemistry, on the other hand, was likely challenged by low abundance poor solubility minerals early Earth.Current experimental approaches to solve this so-called phosphate problem mainly focus solubilization like apatite or reduced species extraterrestrial schreibersite. However, possibilities for prebiotic chemistry through magmatic evolution...
We measure the thermophoresis of polysterene beads over a wide range temperature gradients and find pronounced nonlinear phoretic characteristic. The transition to behavior is marked by drastic slowing down thermophoretic motion characterized Péclet number order unity as corroborated for different particle sizes salt concentrations. data follow single master curve covering entire regime all system parameters upon proper rescaling with number. For low thermal gradients, drift velocity follows...
Abstract Understanding the sequence-dependent DNA damage formation requires probing a complete pool of sequences over wide dose range damage-causing exposure. We used high throughput sequencing to simultaneously obtain dependence and quantum yields for oligonucleotide damages all possible 4096 with hexamer length. exposed ultraviolet radiation at 266 nm doses up 500 absorbed photons per base. At dimer level, our results confirm existing literature values photodamage, whereas we now...
Abstract Spatial proton gradients create energy in biological systems and are likely a driving force for prebiotic systems. Due to the fast diffusion of protons, they however difficult as steady state, unless driven by other non-equilibria such thermal gradients. Here, we quantitatively predict heat-flux formation pH case simple acid-base reaction system. To this end, (i) establish theoretical framework that describes spatial interplay chemical reactions with convection, thermophoresis,...
Abstract To understand the emergence of life, a better understanding physical chemistry primordial non‐equilibrium conditions is essential. Significant salt concentrations are required for catalytic function RNA. The separation oligonucleotides into single strands difficult problem as hydrolysis RNA becomes limiting factor at high temperatures. Salt modulate melting DNA or RNA, and its periodic modulation would enable annealing cycles low In our experiments, moderate temperature difference...
A long standing goal is the direct optical control of biomolecules and water for applications ranging from microfluidics over biomolecule detection to non-equilibrium biophysics. Thermal forces originating optically applied, dynamic microscale temperature gradients have shown possess great potential reach this goal. It was demonstrated that laser heating by a few Kelvin can generate guide flow on micrometre scale in bulk fluid, gel matrices or ice without requiring any lithographic...
How life emerged is one of the major questions that remains to be answered. Apart from being interest for completeness biology, it also a very interesting study case vantage point physics. Living organisms are inherently non-equilibrium systems. Since thermodynamics still developing field, emergence highly case. Here we present progress have made during last few years, employing experimental biophysics capture mechanisms could eventually lead life. We show how simple system, thermal...
Abstract DNA phase transitions are often induced by the addition of condensation agents or dry concentration. Herein, we show that non‐equilibrium setting a moderate heat flow across water‐filled chamber separates and gelates strands with single‐base resolution. A dilute mix two slightly different gel‐forming sequences into sequence‐pure hydrogels under constant physiological solvent conditions. single base change in 36 mer inhibits gelation. Only ability to form longer concentrated, further...