# Holistic energy landscape management in 2D/3D heterojunction via molecular engineering for efficient perovskite solar cells

## TL;DR

This paper introduces a molecular engineering strategy to improve the efficiency and stability of perovskite solar cells by managing energy landscapes in 2D/3D heterojunctions.

## Contribution

A novel approach using π-conjugated organic cations to tune energy levels and reduce charge barriers in 2D/3D perovskite heterojunctions.

## Key findings

- Designing π-conjugated cations reduces hole transfer energy barriers at 2D/3D heterojunctions.
- Solar cells achieved a power conversion efficiency of 24.6%, the highest for PTAA-based n-i-p devices.
- The method enhances stability and reproducibility while being compatible with multiple hole transporting materials.

## Abstract

Constructing two-dimensional (2D) perovskite atop of 3D with energy landscape management is still a challenge in perovskite photovoltaics. Here, we report a strategy through designing a series of π-conjugated organic cations to construct stable 2D perovskites and to realize delicate energy level tunability at 2D/3D heterojunctions. As a result, the hole transfer energy barriers can be reduced both at heterojunctions and within 2D structures, and the preferable work function shift reduces charge accumulation at interface. Leveraging these insights and also benefitted from the superior interface contact between conjugated cations and poly(triarylamine) (PTAA) hole transporting layer, a solar cell with power conversion efficiency of 24.6% has been achieved, which is the highest among PTAA-based n-i-p devices to the best of our knowledge. The devices exhibit greatly enhanced stability and reproducibility. This approach is generic to several hole transporting materials, offering opportunities to realize high efficiency without using the unstable Spiro-OMeTAD.

Conjugated ligand design for 2D/3D heterojunctions improves band alignment and charge transport in perovskite solar cells.