The search for the chemical origins of life represents a long-standing and continuously debated enigma. Despite its exceptional complexity, in the last decades the field has experienced a revival, also owing to the exponential growth of the computing power allowing for efficiently simulating the behavior of matter-including its quantum nature-under disparate conditions found, e.g., on the primordial Earth and on Earth-like planetary systems (i.e., exoplanets). In this minireview, we focus on some advanced computational methods capable of efficiently solving the Schro¨dinger equation at different levels of approximation (i.e., density functional theory)-such as ab initio molecular dynamics-and which are capable to realistically simulate the behavior of matter under the action of energy sources available in prebiotic contexts. In addition, recently developed metadynamics methods coupled with first-principles simulations are here reviewed and exploited to answer to old enigmas and to propose novel scenarios in the exponentially growing research field embedding the study of the chemical origins of life.

Department of Mathematical and Computer Science Physical Sciences and Earth Sciences Università degli Studi di Messina 5 le F Stagno d'Alcontres 31 98166 Messina Italy

Institute for Physical Chemical Processes National Research Council of Italy 5 le F Stagno d'Alcontres 37 98158 Messina Italy

Institute of Biophysics of the Czech Academy of Sciences Kràlovopolskà 135 61265 Brno Czech Republic

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