Photostable and efficient upconverting nanocrystal-based chemical sensors

Tajon, Cheryl A.; Yang, Hao; Tian, Bining; Tian, Yue; Ercius, Peter; Schuck, P. James; Chan, Emory M.; Cohen, Bruce E.

doi:10.1016/j.optmat.2018.07.031

Photostable and efficient upconverting nanocrystal-based chemical sensors

Journal Article · Tue Jul 17 00:00:00 EDT 2018 · Optical Materials

DOI:https://doi.org/10.1016/j.optmat.2018.07.031· OSTI ID:1510755

Tajon, Cheryl A. ^[1]; Yang, Hao ^[1]; Tian, Bining ^[1]; Tian, Yue ^[1]; Ercius, Peter ^[1]; Schuck, P. James ^[1]; Chan, Emory M. ^[1]; Cohen, Bruce E. ^[2]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Columbia Univ., New York, NY (United States)

Chemical sensing in living systems demands optical sensors that are bright, stable, and sensitive to the rapid dynamics of chemical signaling. Lanthanide-doped upconverting nanoparticles (UCNPs) efficiently convert near infrared (NIR) light to higher energy emission and allow biological systems to be imaged with no measurable background or photobleaching, and with reduced scatter for subsurface experiments. Despite their advantages as imaging probes, UCNPs have little innate chemical sensing ability and require pairing with organic fluorophores to act as biosensors, although the design of stable UCNP-fluorophore hybrids with efficient upconverted energy transfer (UET) has remained a challenge. Here, we report Yb³⁺- and Er³⁺-doped UCNP-fluorophore conjugates with UET efficiencies up to 88%, and photostabilities 100-fold greater by UET excitation than those of the free fluorophores under direct excitation. Despite adding distance between Er³⁺ donors and organic acceptors, thin inert shells significantly enhance overall emission without compromising UET efficiency. This can be explained by the large increase in quantum yield of Er³⁺ donors at the core/shell interface and the large number of fluorophore acceptors at the surface. Sensors excited by UET show increases in photostability well beyond those reported for other methods for increasing the longevity of organic fluorophores, and those covalently attached to UCNP surface polymers show greater chemical stability than those directly coordinated to the nanocrystal surface. Furthermore by conjugating other fluorescent chemosensors to UCNPs, these hybrids may be extended to a series of NIR-responsive biosensors for quantifying the dynamic chemical populations critical for cell signaling.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1510755

Alternate ID(s):: OSTI ID: 1544891

Journal Information:: Optical Materials, Journal Name: Optical Materials Journal Issue: C Vol. 84; ISSN 0925-3467

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Ultralow-threshold, continuous-wave upconverting lasing from subwavelength plasmons Fernandez-Bravo, Angel; Wang, Danqing; Barnard, Edward S. Nature Materials, Vol. 18, Issue 11 https://doi.org/10.1038/s41563-019-0482-5	journal	September 2019
In vivo deep-tissue microscopy with UCNP/Janus-dendrimers as imaging probes: resolution at depth and feasibility of ratiometric sensing Plunkett, Shane; El Khatib, Mirna; Şencan, İkbal Nanoscale, Vol. 12, Issue 4 https://doi.org/10.1039/c9nr07778b	journal	January 2020

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Photostable and efficient upconverting nanocrystal-based chemical sensors

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