# Incommensurate chirality density wave transition in a hybrid molecular framework

## TL;DR

This study uncovers a novel incommensurate chirality density wave phase in a hybrid molecular framework, revealing a new form of chiral symmetry breaking driven by coupling of lattice and molecular modes.

## Contribution

It demonstrates the existence of an incommensurate chirality density wave phase in a hybrid framework, a previously unknown type of chiral order in solids.

## Key findings

- Identification of the incommensurate phase transition at 235 K.
- Observation of spontaneous chiral resolution in molecular conformations.
- Proposal of coupling mechanisms between acoustic and molecular modes.

## Abstract

Using single-crystal X-ray diffraction we characterise the 235\,K incommensurate phase transition in the hybrid molecular framework tetraethylammonium silver(I) dicyanoargentate, [NEt$_4$]Ag$_3$(CN)$_4$. We demonstrate the transition to involve spontaneous resolution of chiral [NEt$_4$]$^+$ conformations, giving rise to a state in which molecular chirality is incommensurately modulated throughout the crystal lattice. We refer to this state as an incommensurate chirality density wave (XDW) phase, which represents a fundamentally new type of chiral symmetry breaking in the solid state. Drawing on parallels to the incommensurate ferroelectric transition of NaNO$_2$ we suggest the XDW state arises through coupling between acoustic (shear) and molecular rotoinversion modes. Such coupling is symmetry-forbidden at the Brillouin zone centre but symmetry-allowed for small but finite modulation vectors $\mathbf q=[0,0,q_z]^\ast$. The importance of long-wavelength chirality modulations in the physics of this hybrid framework may have implications for the generation of mesoscale chiral textures, as required for advanced photonic materials.