Fluorescence Blinking Beyond Nanoconfinement: Spatially Synchronous Intermittency of Entire Perovskite Microcrystals

Nithin Pathoor; Ansuman Halder; Amitrajit Mukherjee; Jaladhar Mahato; Shaibal K. Sarkar; Arindam Chowdhury

doi:10.1002/anie.201804852

Fluorescence Blinking Beyond Nanoconfinement: Spatially Synchronous Intermittency of Entire Perovskite Microcrystals

Nithin Pathoor
, Ansuman Halder
, Amitrajit Mukherjee
, Jaladhar Mahato
, Shaibal K. Sarkar
, Arindam Chowdhury

Indian Institute of Technology Bombay

Research output: Contribution to journal › Article › peer-review

39 Scopus citations

Abstract

Abrupt fluorescence intermittency or blinking is long recognized to be characteristic of single nano-emitters. Extended quantum-confined nanostructures also undergo spatially heterogeneous blinking; however, there is no such precedent in dimensionally unconfined (bulk) materials. Herein, we report multi-level blinking of entire individual organo–lead bromide perovskite microcrystals (volume=0.1–3 μm³) under ambient conditions. Extremely high spatiotemporal correlation (>0.9) in intracrystal emission intensity fluctuations signifies effective communication amongst photogenerated carriers at distal locations (up to ca. 4 μm) within each crystal. Fused polycrystalline grains also exhibit this intriguing phenomenon, which is rationalized by correlated and efficient migration of carriers to a few transient nonradiative traps, the nature and population of which determine blinking propensity. Observation of spatiotemporally correlated emission intermittency in bulk semiconductor crystals opens the possibility of designing novel devices involving long-range (mesoscopic) electronic communication.

Original language	English
Pages (from-to)	11603-11607
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	36
DOIs	https://doi.org/10.1002/anie.201804852
State	Published - 3 Sep 2018
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Funding

Financial support provided by Solar Energy Research Institutes of India and US (SERIIUS) and Ministry of New and Renewable Energy (MNRE), Govt. of India. A.C. thanks the National Center for Photovoltaic Research and Education (NCPRE), aided by MNRE for partial financial support. Authors acknowledge IRCC and CRNTS, IIT Bombay for usage of central facility equipment. N.P. and A.M. acknowledge fellowships from CSIR (India). A.C. thanks Subhabrata Dhar, Siuli Mukhopadhyay, Amitabha Tripathi, and the Kaleidoscope-2017 meeting for valuable discussions.

Funders
Ministry of New and Renewable Energy India
Council of Scientific and Industrial Research, India
National Centre for Photovoltaic Research and Education

Keywords

concerted blinking
correlated carrier migration
hybrid perovskites
long-range communication
transient traps

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10.1002/anie.201804852

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title = "Fluorescence Blinking Beyond Nanoconfinement: Spatially Synchronous Intermittency of Entire Perovskite Microcrystals",

abstract = "Abrupt fluorescence intermittency or blinking is long recognized to be characteristic of single nano-emitters. Extended quantum-confined nanostructures also undergo spatially heterogeneous blinking; however, there is no such precedent in dimensionally unconfined (bulk) materials. Herein, we report multi-level blinking of entire individual organo–lead bromide perovskite microcrystals (volume=0.1–3 μm3) under ambient conditions. Extremely high spatiotemporal correlation (>0.9) in intracrystal emission intensity fluctuations signifies effective communication amongst photogenerated carriers at distal locations (up to ca. 4 μm) within each crystal. Fused polycrystalline grains also exhibit this intriguing phenomenon, which is rationalized by correlated and efficient migration of carriers to a few transient nonradiative traps, the nature and population of which determine blinking propensity. Observation of spatiotemporally correlated emission intermittency in bulk semiconductor crystals opens the possibility of designing novel devices involving long-range (mesoscopic) electronic communication.",

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AU - Sarkar, Shaibal K.

AU - Chowdhury, Arindam

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AB - Abrupt fluorescence intermittency or blinking is long recognized to be characteristic of single nano-emitters. Extended quantum-confined nanostructures also undergo spatially heterogeneous blinking; however, there is no such precedent in dimensionally unconfined (bulk) materials. Herein, we report multi-level blinking of entire individual organo–lead bromide perovskite microcrystals (volume=0.1–3 μm3) under ambient conditions. Extremely high spatiotemporal correlation (>0.9) in intracrystal emission intensity fluctuations signifies effective communication amongst photogenerated carriers at distal locations (up to ca. 4 μm) within each crystal. Fused polycrystalline grains also exhibit this intriguing phenomenon, which is rationalized by correlated and efficient migration of carriers to a few transient nonradiative traps, the nature and population of which determine blinking propensity. Observation of spatiotemporally correlated emission intermittency in bulk semiconductor crystals opens the possibility of designing novel devices involving long-range (mesoscopic) electronic communication.

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Fluorescence Blinking Beyond Nanoconfinement: Spatially Synchronous Intermittency of Entire Perovskite Microcrystals

Abstract

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Keywords

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