title: Visualization of the spontaneous emergence of a complex, dynamic, and autocatalytic system.
abstract: Autocatalytic chemical reactions are widely studied as models of biological processes and to better understand the origins of life on Earth. Minimal self-reproducing amphiphiles have been developed in this context and as an approach to de novo "bottom-up" synthetic protocells. How chemicals come together to produce living systems, however, remains poorly understood, despite much experimentation and speculation. Here, we use ultrasensitive label-free optical microscopy to visualize the spontaneous emergence of an autocatalytic system from an aqueous mixture of two chemicals. Quantitative, in situ nanoscale imaging reveals heterogeneous self-reproducing aggregates and enables the real-time visualization of the synthesis of new aggregates at the reactive interface. The aggregates and reactivity patterns observed vary together with differences in the respective environment. This work demonstrates how imaging of chemistry at the nanoscale can provide direct insight into the dynamic evolution of nonequilibrium systems across molecular to microscopic length scales.
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford, Oxford OX1 3QZ, United Kingdom.
authors.forename: Jaime
authors.initials: J
authors.lastname: Ortega-Arroyo
authors.affiliation: Chemistry Research Laboratory, University of Oxford, Oxford OX1 3TA, United Kingdom.
authors.forename: Andrew J
authors.identifier: 0000-0002-4062-4761
authors.initials: AJ
authors.lastname: Bissette
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford, Oxford OX1 3QZ, United Kingdom; stephen.fletcher@chem.ox.ac.uk philipp.kukura@chem.ox.ac.uk.
authors.forename: Philipp
authors.initials: P
authors.lastname: Kukura
authors.affiliation: Chemistry Research Laboratory, University of Oxford, Oxford OX1 3TA, United Kingdom stephen.fletcher@chem.ox.ac.uk philipp.kukura@chem.ox.ac.uk.
authors.forename: Stephen P
authors.initials: SP
authors.lastname: Fletcher
keywords: autocatalysis; emergence; interferometric scattering; label-free microscopy; protocells