# The Role of Pressure in Inverse Design for Assembly

## TL;DR

This paper demonstrates how inverse design using relative entropy optimization can create pair potentials that self-assemble into specific structures at a prescribed pressure, enabling thermodynamic control in self-assembly.

## Contribution

It introduces a method to incorporate pressure control into inverse design for self-assembly, expanding the design space for targeted structures.

## Key findings

- Generated potentials that self-assemble at different pressures
- Demonstrated control over assembled structures via pressure tuning
- Showed the versatility of the method for thermodynamic property control

## Abstract

Isotropic pairwise interactions that promote the self assembly of complex particle morphologies have been discovered by inverse design strategies derived from the molecular coarse-graining literature. While such approaches provide an avenue to reproduce structural correlations, thermodynamic quantities such as the pressure have typically not been considered in self-assembly applications. In this work, we demonstrate that relative entropy optimization can be used to discover potentials that self-assemble into targeted cluster morphologies with a prescribed pressure when the iterative simulations are performed in the isothermal-isobaric ensemble. By tuning the pressure in the optimization, we generate a family of simple pair potentials that all self-assemble the same structure. Selecting an appropriate simulation ensemble to control the thermodynamic properties of interest is a general design strategy that could also be used to discover interaction potentials that self-assemble structures having, for example, a specified chemical potential.