Quantum dots: using the known as well as exploring the unknown

Super-resolution microscopy, the imaging of features below the Abbe diffraction limit, has been achieved by a number of methods in recent years. Each of these methods relies on breaking one of the assumptions made in the derivation of the diffraction limit. While uniform spatial illumination, linearity and time independence have been the most common cornerstones of the Abbe limit broken in super-resolution modalities, breaking the ‘classicality of light’ assumption as a pathway to achieve super-resolution has not been shown. Here we demonstrate a method that utilizes the antibunching characteristic of light emitted by Quantum Dots (QDs), a purely quantum feature of light, to obtain imaging beyond the diffraction limit. Measuring such high order correlations in the emission of a single QD necessitates stability at saturation conditions while avoiding damage and enhanced blinking. This ability was facilitated through new understandings that arisen from exploring the QD ‘blinking’ phenomena. We summarize here two studies that contributed to our current understanding of QD stability.

[1]  Christian Eggeling,et al.  Major signal increase in fluorescence microscopy through dark-state relaxation , 2007, Nature Methods.

[2]  J. Lippincott-Schwartz,et al.  Imaging Intracellular Fluorescent Proteins at Nanometer Resolution , 2006, Science.

[3]  S. Lloyd,et al.  Sub-Rayleigh-diffraction-bound quantum imaging , 2008, 0804.2875.

[4]  Dan Oron,et al.  Superresolution microscopy with quantum emitters. , 2013, Nano letters.

[5]  Justin M. Hodgkiss,et al.  Blue semiconductor nanocrystal laser , 2005 .

[6]  Preston T. Snee,et al.  Multiexcitonic two-state lasing in a CdSe nanocrystal laser , 2004 .

[7]  R. Pooser,et al.  Entangled Images from Four-Wave Mixing , 2008, Science.

[8]  E. Solano,et al.  Quantum imaging with incoherent photons , 2007, 2007 Quantum Electronics and Laser Science Conference.

[9]  A. Nozik Quantum dot solar cells , 2002 .

[10]  R. Heintzmann,et al.  Saturated patterned excitation microscopy--a concept for optical resolution improvement. , 2002, Journal of the Optical Society of America. A, Optics, image science, and vision.

[11]  Robert W Boyd,et al.  Quantum spatial superresolution by optical centroid measurements. , 2011, Physical review letters.

[12]  G. Brida,et al.  Experimental realization of sub-shot-noise quantum imaging , 2010 .

[13]  S. Hell,et al.  Two- and multiphoton detection as an imaging mode and means of increasing the resolution in far-field light microscopy: A study based on photon-optics , 1995 .

[14]  Michael J Rust,et al.  Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM) , 2006, Nature Methods.

[15]  Dan Oron,et al.  Improved resolution in fluorescence microscopy using quantum correlations , 2012 .

[16]  Kolobov,et al.  Quantum limits on optical resolution , 2000, Physical review letters.

[17]  S. Hell,et al.  Breaking the diffraction resolution limit by stimulated emission: stimulated-emission-depletion fluorescence microscopy. , 1994, Optics letters.

[18]  Jian-Wei Pan,et al.  De Broglie wavelength of a non-local four-photon state , 2003, Nature.

[19]  M. Teich,et al.  Wolf equations for two-photon light. , 2005, Physical review letters.

[20]  Masaru Kuno,et al.  Universal emission intermittency in quantum dots, nanorods and nanowires , 2008, 0810.2509.

[21]  F. Grosshans,et al.  Enhancing single-molecule photostability by optical feedback from quantum jump detection , 2007, 0707.3200.

[22]  M. Kovalenko,et al.  Prospects of colloidal nanocrystals for electronic and optoelectronic applications. , 2010, Chemical reviews.

[23]  M. Gustafsson Nonlinear structured-illumination microscopy: wide-field fluorescence imaging with theoretically unlimited resolution. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[24]  S. Gambhir,et al.  Quantum Dots for Live Cells, in Vivo Imaging, and Diagnostics , 2005, Science.

[25]  Talon,et al.  Photon antibunching in the fluorescence of a single dye molecule trapped in a solid. , 1992, Physical review letters.

[26]  S. Weiss,et al.  Fast, background-free, 3D super-resolution optical fluctuation imaging (SOFI) , 2009, Proceedings of the National Academy of Sciences.

[27]  M. Bawendi,et al.  Challenge to the charging model of semiconductor-nanocrystal fluorescence intermittency from off-state quantum yields and multiexciton blinking. , 2010, Physical review letters.

[28]  R. Heintzmann,et al.  Superresolution by localization of quantum dots using blinking statistics. , 2005, Optics express.

[29]  E. Abbe Beiträge zur Theorie des Mikroskops und der mikroskopischen Wahrnehmung , 1873 .

[30]  M. Nirmal,et al.  Fluorescence intermittency in single cadmium selenide nanocrystals , 1996, Nature.

[31]  T. Mokari,et al.  Selective growth of metal sulfide tips onto cadmium chalcogenide nanostructures , 2012 .

[32]  B. Dubertret,et al.  Bright and grey states in CdSe-CdS nanocrystals exhibiting strongly reduced blinking. , 2009, Physical review letters.

[33]  O. Schwartz,et al.  Colloidal quantum dots as saturable fluorophores. , 2012, ACS nano.

[34]  W. E. Moerner,et al.  Photon antibunching in single CdSe/ZnS quantum dot fluorescence , 2000 .

[35]  Y. Silberberg,et al.  High-NOON States by Mixing Quantum and Classical Light , 2010, Science.

[36]  D. Oron,et al.  Studying quantum dot blinking through the addition of an engineered inorganic hole trap. , 2013, ACS nano.

[37]  A. Efros,et al.  Random Telegraph Signal in the Photoluminescence Intensity of a Single Quantum Dot , 1997 .

[38]  M. Tsang Quantum imaging beyond the diffraction limit by optical centroid measurements. , 2009, Physical review letters.

[39]  P. Guyot-Sionnest,et al.  Evidence for the role of holes in blinking: negative and oxidized CdSe/CdS dots. , 2012, ACS nano.

[40]  O. Schwartz,et al.  Transient fluorescence of the off state in blinking CdSe/CdS/ZnS semiconductor nanocrystals is not governed by Auger recombination. , 2010, Physical review letters.

[41]  Marcus Dyba,et al.  Concepts for nanoscale resolution in fluorescence microscopy , 2004, Current Opinion in Neurobiology.

[42]  A. Malko,et al.  Optical gain and stimulated emission in nanocrystal quantum dots. , 2000, Science.

[43]  C. Galland,et al.  Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots , 2011, Nature.