Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films

Hao Zhang; Altaf Pasha; Isaac Metcalf; Jianlin Zhou; Mathias Staunstrup; Yunxuan Zhu; Shusen Liao; Ken Ssennyimba; Jia-Shiang Chen; Surya Prakash Reddy; Simon Thébaud; Jin Hou; Xinting Shuai; Faiz Mandani; Siraj Sidhik; Matthew R. Jones; Xuedan Ma; R Geetha Balakrishna; Sandhya Susarla; David S. Ginger; Claudine Katan; Mercouri G. Kanatzidis; Moungi G. Bawendi; Douglas Natelson; Philippe Tamarat; Brahim Lounis; Jacky Even; Aditya D. Mohite

arXiv · 2501.06061

Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films

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Abstract

Colloidal perovskite quantum dots (PQDs) are an exciting platform for on-demand quantum, and classical optoelectronic and photonic devices. However, their potential success is limited by the extreme sensitivity and low stability arising from their weak intrinsic lattice bond energy and complex surface chemistry. Here we report a novel platform of buried perovskite quantum dots (b-PQDs) in a three-dimensional perovskite thin-film, fabricated using one-step, flash annealing, which overcomes surface related instabilities in colloidal perovskite dots. The b-PQDs demonstrate ultrabright and stable single-dot emission, with resolution-limited linewidths below 130 μeV, photon-antibunching (g^2(0)=0.1), no blinking, suppressed spectral diffusion, and high photon count rates of 10^4/s, consistent with unity quantum yield. The ultrasharp linewidth resolves exciton fine-structures (dark and triplet excitons) and their dynamics under a magnetic field. Additionally, b-PQDs can be electrically driven to emit single photons with 1 meV linewidth and photon-antibunching (g^2(0)=0.4). These results pave the way for on-chip, low-cost single-photon sources for next generation quantum optical communication and sensing.

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Hao Zhang, Altaf Pasha, Isaac Metcalf, Jianlin Zhou, Mathias Staunstrup, Yunxuan Zhu, Shusen Liao, Ken Ssennyimba, Jia-Shiang Chen, Surya Prakash Reddy, Simon Thébaud, Jin Hou, Xinting Shuai, Faiz Mandani, Siraj Sidhik, Matthew R. Jones, Xuedan Ma, R Geetha Balakrishna, Sandhya Susarla, David S. Ginger, Claudine Katan, Mercouri G. Kanatzidis, Moungi G. Bawendi, Douglas Natelson, Philippe Tamarat, Brahim Lounis, Jacky Even, Aditya D. Mohite. 2025-01-10. Overcoming the surface paradox: Buried perovskite quantum dots in wide-bandgap perovskite thin films. https://arxiv.org/abs/2501.06061

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