<p><b>Harnessing and then controlling </b><b>combinatorial explosions</b><b> in </b><b>uncontrolled condensation reactions of simple building
blocks is a key problem to many hypotheses on the origin</b><b> of </b><b>life. Much has been achieved in understanding how the
building blocks of biopolymers may be formed, and in understanding how
macromolecules may produce functional and increasingly life-like systems. How</b><b> these </b><b>steps can be joined, and how defined populations</b><b> of </b><b>macromolecules can form from mixtures</b><b> of </b><b>simple building blocks, instead of an undifferentiated
</b><b>mess</b><b>, remain open questions.</b><b> Herein, we show </b><b>how</b><b> unconstrained </b><b>condensation</b><b> reactions of both amino acids, and prebiotic soup mixtures
produced by spark discharge, can be steered</b><b> by changes in the reaction environment, such as order
of reactant addition (mixing history), and addition of salts or minerals. Using
</b><b>techniques akin to
untargeted metabolomics</b><b>
to survey product distributions we</b><b> demonstrate that while these reactions do produce a large range of
species, there are distinct, significant, and reproducible differences between the
product ensembles</b><b>.
Furthermore, we observe that differences in composition </b><b>are </b><b>demonstrated through</b><b> clearly different structural and functional properties. </b><b>Using this approach, we
demonstrate for the first time that simple variations in environmental
parameters can mediate the differentiation of distinct ensembles from both
amino acid mixtures and a classic primordial soup model (products of a ‘Miller
Urey’ type spark discharge reaction). </b><b>This shows that </b><b>the
synthetic complexity produced by such unconstrained reactions is not as
intractable as often suggested, when viewed through a chemically agnostic lens.
An open</b><b> approach
to complexity can generate compositional, structural, and functional diversity
from fixed sets of simple starting materials, suggesting that differentiation
of product mixtures can occur in the wider environment without the need for
biological machinery.</b><b></b></p>