Defect Engineered Layer Dependent Nonlinear Optical Response in Two Dimensional Muscovite for Efficient Optical Limiting

Dipanwita Mitra; Guilherme S. L. Fabris; Raphael Benjamim; Mateus M. Ferrer; Marcelo Lopes Pereira Junior; Riya Sadhukhan; Dipak Kumar Goswami; Gelu Costin; Douglas S. Galvão; Chandra Sekhar Tiwary; Prasanta Kumar Dattaa

arXiv · 2507.14786

Defect Engineered Layer Dependent Nonlinear Optical Response in Two Dimensional Muscovite for Efficient Optical Limiting

Dipanwita Mitra·Guilherme S. L. Fabris·Raphael Benjamim·Mateus M. Ferrer·Marcelo Lopes Pereira Junior·Riya Sadhukhan·Dipak Kumar Goswami·Gelu Costin·Douglas S. Galvão·Chandra Sekhar Tiwary·Prasanta Kumar Dattaa

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Abstract

Light-matter interactions in two-dimensional (2D) materials have gained significant interest due to their distinctive optical and electronic properties. Recently, silicates have emerged as a promising new class of 2D materials, but their nonlinear optical properties remain largely unexplored. In this study, we demonstrate layer-dependent nonlinear absorption and optical limiting capabilities of 2D muscovite using femtosecond laser excitation at 450 nm. The two-photon absorption (TPA) coefficient is highly sensitive to both the number of layers and excitation intensity, increasing markedly from (3.91+/-0.06)x10^3 cm GW^-1 in multilayer structures to (6.94+/-0.17)x10^5 cm GW^-1 in the monolayer limit at a peak intensity of 68 GW cm^-2, highlighting a strong layer-dependent enhancement in nonlinear absorption. Additionally, monolayer muscovite exhibits an optical limiting threshold of 1.46 mJ cm^-2, outperforming graphene and other 2D dichalcogenides. This enhanced TPA arises from quantum confinement and intrinsic lattice defects that facilitate nonlinear optical transitions. Density functional theory reveals that liquid-phase exfoliation disrupts potassium interlayers and induces oxygen vacancies, generating mid-gap electronic states that significantly enhance TPA. These insights open new avenues for designing low-fluence, high-efficiency optical limiters using 2D silicates.

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Dipanwita Mitra, Guilherme S. L. Fabris, Raphael Benjamim, Mateus M. Ferrer, Marcelo Lopes Pereira Junior, Riya Sadhukhan, Dipak Kumar Goswami, Gelu Costin, Douglas S. Galvão, Chandra Sekhar Tiwary, Prasanta Kumar Dattaa. 2025-07-20. Defect Engineered Layer Dependent Nonlinear Optical Response in Two Dimensional Muscovite for Efficient Optical Limiting. https://arxiv.org/abs/2507.14786

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