Universal Synthesis of Large-Area Hybrid Perovskite Monolayers Enabling Lithography-Free, Low-Static-Power Optoelectronics
Abstract
Solution-phase synthesis of monolayer hybrid organic-inorganic perovskites is constrained by rapid out-of-plane crystal growth, uncontrolled nucleation, and strong interlayer aggregation, yielding flakes of only a few μm. We introduce a steric-engineering ternary-solvent growth strategy to synthesize monolayer and few-layer A2MX4 hybrid perovskites with exceptionally large surface areas. By combining alcohol cosolvents with an amine additive, out-of-plane stacking is suppressed. Using (PEA)2CuCl4 as a model system, monolayers with lateral areas exceeding 1000 μm2 are achieved, representing a massive dimensional increase over conventional methods. Molecular dynamics and quantum-chemical calculations show that longer-chain alcohols reorganize precursor solvation, while solvent volatility prolongs edge-mediated precursor transport during annealing. This strategy demonstrates universal applicability across diverse organic spacer cations (PEA+, F-PEA+, PentA+), metal centers (Cu2+, Mn2+, Pb2+), and halides (Cl-, Br-, I-). The large lateral dimensions enable direct, solvent-free electrical contact fabrication via physical shadow masking, bypassing chemical degradation from solvents used in conventional lithography. Planar devices fabricated from isolated ultrathin (PEA)2PbI4 channels exhibit ultra-low dark currents down to the 10^-15 - 10^-13 A range, enabling femtowatt-to-picowatt static power consumption, ~ 0.2 pW at 5 V, a 250-fold reduction relative to drop-cast films, while maintaining a high light-to-dark current ratio of 4.3 x 102. This work establishes precise steric and solvation control as a paradigm for scalable, compositionally diverse, low-static-power monolayer 2D perovskite optoelectronics.
Related
- Quasi-2D Perovskite Photonic Crystals for Single-Mode Lasing via Synergistic Material and Structural Optimization by Nanoimprint Lithography
- Perovskite Nanocrystal-Based Scintillators: Synthesis Routes, Matrix Engineering, and Performance Optimization for Radiation Detection
- Universal empirical coupled channel calculations for capture cross sections in synthesis of superheavy nuclei
- Spatiotemporal programming via asymmetric dielectric engineering for nonvolatile 2D optoelectronics
- Passive axial confinement in two-photon lithography with a 3D-printed pupil filter
BibTeX
@misc{kalyanasundaram2026universal,
title = {{Universal Synthesis of Large-Area Hybrid Perovskite Monolayers Enabling Lithography-Free, Low-Static-Power Optoelectronics}},
author = {Shankeerthan Kalyanasundaram and Swarit Dwivedi and Sanje Mahasivam and Christopher R. McNeill and Sudha Mokkapati},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.30764},
eprint = {2610.30764},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.30764},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Universal Synthesis of Large-Area Hybrid Perovskite Monolayers Enabling Lithography-Free, Low-Static-Power Optoelectronics
AU - Shankeerthan Kalyanasundaram
AU - Swarit Dwivedi
AU - Sanje Mahasivam
AU - Christopher R. McNeill
AU - Sudha Mokkapati
PY - 2026
DA - 2026/10/22
PB - arXiv
DO - 10.48550/arxiv.2610.30764
UR - https://arxiv.org/abs/2610.30764
AB - Solution-phase synthesis of monolayer hybrid organic-inorganic perovskites is constrained by rapid out-of-plane crystal growth, uncontrolled nucleation, and strong interlayer aggregation, yielding flakes of only a few μm. We introduce a steric-engineering ternary-solvent growth strategy to synthesize monolayer and few-layer A2MX4 hybrid perovskites with exceptionally large surface areas. By combining alcohol cosolvents with an amine additive, out-of-plane stacking is suppressed. Using (PEA)2CuCl4 as a model system, monolayers with lateral areas exceeding 1000 μm2 are achieved, representing a massive dimensional increase over conventional methods. Molecular dynamics and quantum-chemical calculations show that longer-chain alcohols reorganize precursor solvation, while solvent volatility prolongs edge-mediated precursor transport during annealing. This strategy demonstrates universal applicability across diverse organic spacer cations (PEA+, F-PEA+, PentA+), metal centers (Cu2+, Mn2+, Pb2+), and halides (Cl-, Br-, I-). The large lateral dimensions enable direct, solvent-free electrical contact fabrication via physical shadow masking, bypassing chemical degradation from solvents used in conventional lithography. Planar devices fabricated from isolated ultrathin (PEA)2PbI4 channels exhibit ultra-low dark currents down to the 10^-15 - 10^-13 A range, enabling femtowatt-to-picowatt static power consumption, ~ 0.2 pW at 5 V, a 250-fold reduction relative to drop-cast films, while maintaining a high light-to-dark current ratio of 4.3 x 102. This work establishes precise steric and solvation control as a paradigm for scalable, compositionally diverse, low-static-power monolayer 2D perovskite optoelectronics.
ER -