All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses

• Published in: Nature nanotechnology Vol. 16; no. 12; pp. 1355 - 1361
• Main Authors: Shi, Jiaojian, Sun, Weiwei, Utzat, Hendrik, Farahvash, Ardavan, Gao, Frank Y., Zhang, Zhuquan, Barotov, Ulugbek, Willard, Adam P., Nelson, Keith A., Bawendi, Moungi G.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.12.2021; Nature Publishing Group
• Subjects: 119/118; 140/125; 639/301/357/1017; 639/624/400/385; 639/638/439/945; 639/766/119; 639/766/400/3925; Blinking; Cadmium selenides; Cadmium sulfide; Chemical engineering; Chemistry and Materials Science; Diamonds; Emissions control; Emitters; Excitons; Flicker; Fluorescence; Luminescence; Materials Science; Nanotechnology; Nanotechnology and Microengineering; Particle tracking; Photoluminescence; Photons; Quantum dots; Quantum tunnelling; Science & Technology - Other Topics; Stability; Trions; Two dimensional materials
• DOI: 10.1038/s41565-021-01016-w
• ISSN: 1748-3387

Photoluminescence intermittency is a ubiquitous phenomenon, reducing the temporal emission intensity stability of single colloidal quantum dots (QDs) and the emission quantum yield of their ensembles. Despite efforts to achieve blinking reduction by chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate a deterministic all-optical suppression of QD blinking using a compound technique of visible and mid-infrared excitation. We show that moderate-field ultrafast mid-infrared pulses (5.5 μm, 150 fs) can switch the emission from a charged, low quantum yield grey trion state to the bright exciton state in CdSe/CdS core–shell QDs, resulting in a significant reduction of the QD intensity flicker. Quantum-tunnelling simulations suggest that the mid-infrared fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced photoluminescence intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials. Photoluminescence blinking is a ubiquitous phenomenon that detrimentally reduces emission stability and quantum yield. Now, an all-optical method, which employs ultrafast mid-infrared pulses, can effectively suppress the blinking of single CdSe/CdS core–shell quantum dots.