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Title: Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications

Abstract

A near-infrared (NIR) dye-sensitized upconversion nanoparticles (UCNPs) can broaden the absorption range and boost upconversion efficiency of UCNPs. We achieved significantly enhanced upconversion luminescence in dye-sensitized core/active shell UCNPs via the doping of ytterbium ions (Yb 3+ ) in the UCNP shell, which bridged the energy transfer from the dye to the UCNP core. As a result, we synergized the two most practical upconversion booster effectors (dye-sensitizing and core/shell enhancement) to amplify upconversion efficiency. We also demonstrated two biomedical applications using these UCNPs. By using dye-sensitized core/active shell UCNP embedded poly(methyl methacrylate) polymer implantable systems, we successfully shifted the optogenetic neuron excitation window to a biocompatible and deep tissue penetrable 800 nm wavelength. Furthermore, UCNPs were water-solubilized with Pluronic F127 with high upconversion efficiency and can be imaged in a mouse model.

Authors:
 [1];  [2];  [3];  [2];  [2];  [2];  [4];  [5];  [6];  [7];  [8];  [3];  [3];  [2]
  1. Univ. of Massachusetts Medical School, Worcester, MA (United States). Dept. of Biochemistry and Molecular Pharmacology; Dalian Univ. of Technology (People's Republic of China)
  2. Univ. of Massachusetts Medical School, Worcester, MA (United States). Dept. of Biochemistry and Molecular Pharmacology
  3. Univ. of Massachusetts Medical School, Worcester, MA (United States). Neurobiology Dept.
  4. Zhejiang Univ., Hangzhou (China).. Dept. of Materials Science and Engineering
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  6. Univ. of Massachusetts, Amherst, MA (United States). Chemical Engineering Dept.
  7. Dalian Univ. of Technology (People's Republic of China). State Key Lab. of Fine Chemicals
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH)
OSTI Identifier:
1379046
Grant/Contract Number:  
AC02-05CH11231; R01MH103133; RGY-0090/2014
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bioimaging; core/active shell structure; dye-sensitizing; near-infrared; optogenetics; upconversion nanoparticles

Citation Formats

Wu, Xiang, Zhang, Yuanwei, Takle, Kendra, Bilsel, Osman, Li, Zhanjun, Lee, Hyungseok, Zhang, Zijiao, Li, Dongsheng, Fan, Wei, Duan, Chunying, Chan, Emory M., Lois, Carlos, Xiang, Yang, and Han, Gang. Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications. United States: N. p., 2016. Web. doi:10.1021/acsnano.5b06383.
Wu, Xiang, Zhang, Yuanwei, Takle, Kendra, Bilsel, Osman, Li, Zhanjun, Lee, Hyungseok, Zhang, Zijiao, Li, Dongsheng, Fan, Wei, Duan, Chunying, Chan, Emory M., Lois, Carlos, Xiang, Yang, & Han, Gang. Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications. United States. doi:10.1021/acsnano.5b06383.
Wu, Xiang, Zhang, Yuanwei, Takle, Kendra, Bilsel, Osman, Li, Zhanjun, Lee, Hyungseok, Zhang, Zijiao, Li, Dongsheng, Fan, Wei, Duan, Chunying, Chan, Emory M., Lois, Carlos, Xiang, Yang, and Han, Gang. Wed . "Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications". United States. doi:10.1021/acsnano.5b06383. https://www.osti.gov/servlets/purl/1379046.
@article{osti_1379046,
title = {Dye-Sensitized Core/Active Shell Upconversion Nanoparticles for Optogenetics and Bioimaging Applications},
author = {Wu, Xiang and Zhang, Yuanwei and Takle, Kendra and Bilsel, Osman and Li, Zhanjun and Lee, Hyungseok and Zhang, Zijiao and Li, Dongsheng and Fan, Wei and Duan, Chunying and Chan, Emory M. and Lois, Carlos and Xiang, Yang and Han, Gang},
abstractNote = {A near-infrared (NIR) dye-sensitized upconversion nanoparticles (UCNPs) can broaden the absorption range and boost upconversion efficiency of UCNPs. We achieved significantly enhanced upconversion luminescence in dye-sensitized core/active shell UCNPs via the doping of ytterbium ions (Yb 3+ ) in the UCNP shell, which bridged the energy transfer from the dye to the UCNP core. As a result, we synergized the two most practical upconversion booster effectors (dye-sensitizing and core/shell enhancement) to amplify upconversion efficiency. We also demonstrated two biomedical applications using these UCNPs. By using dye-sensitized core/active shell UCNP embedded poly(methyl methacrylate) polymer implantable systems, we successfully shifted the optogenetic neuron excitation window to a biocompatible and deep tissue penetrable 800 nm wavelength. Furthermore, UCNPs were water-solubilized with Pluronic F127 with high upconversion efficiency and can be imaged in a mouse model.},
doi = {10.1021/acsnano.5b06383},
journal = {ACS Nano},
number = 1,
volume = 10,
place = {United States},
year = {2016},
month = {1}
}

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Regulating the color output and simultaneously enhancing the intensity of upconversion nanoparticles via a dye sensitization strategy
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  • Xue, Bin; Wang, Dan; Zhang, Youlin
  • Journal of Materials Chemistry C, Vol. 7, Issue 28
  • DOI: 10.1039/c9tc02293g

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Brain Photobiomodulation Therapy: a Narrative Review
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Optical nanoprobes for biomedical applications: shining a light on upconverting and near-infrared emitting nanoparticles for imaging, thermal sensing, and photodynamic therapy
journal, January 2017

  • Hemmer, E.; Acosta-Mora, P.; Méndez-Ramos, J.
  • Journal of Materials Chemistry B, Vol. 5, Issue 23
  • DOI: 10.1039/c7tb00403f

Regulating the color output and simultaneously enhancing the intensity of upconversion nanoparticles via a dye sensitization strategy
journal, January 2019

  • Xue, Bin; Wang, Dan; Zhang, Youlin
  • Journal of Materials Chemistry C, Vol. 7, Issue 28
  • DOI: 10.1039/c9tc02293g

Near‐Infrared Manipulation of Membrane Ion Channels via Upconversion Optogenetics
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Luminescent Ions in Advanced Composite Materials for Multifunctional Applications
journal, July 2016

  • Bai, Gongxun; Tsang, Ming-Kiu; Hao, Jianhua
  • Advanced Functional Materials, Vol. 26, Issue 35
  • DOI: 10.1002/adfm.201602142

Er 3+ Sensitized Photon Upconversion Nanocrystals
journal, April 2018

  • Cheng, Xingwen; Pan, Yue; Yuan, Ze
  • Advanced Functional Materials, Vol. 28, Issue 22
  • DOI: 10.1002/adfm.201800208

Band Gap Engineering Improves the Efficiency of Double Quantum Dot Upconversion Nanocrystals
journal, April 2019

  • Yang, Gaoling; Meir, Noga; Raanan, Dekel
  • Advanced Functional Materials, Vol. 29, Issue 23
  • DOI: 10.1002/adfm.201900755

Near‐Infrared‐Light Activatable Nanoparticles for Deep‐Tissue‐Penetrating Wireless Optogenetics
journal, January 2019

  • Yu, Nuo; Huang, Ling; Zhou, Yubin
  • Advanced Healthcare Materials, Vol. 8, Issue 6
  • DOI: 10.1002/adhm.201801132

Ultra-Wideband Multi-Dye-Sensitized Upconverting Nanoparticles for Information Security Application
journal, October 2016


808-nm-Light-Excited Lanthanide-Doped Nanoparticles: Rational Design, Luminescence Control and Theranostic Applications
journal, March 2017


Gold and Hairpin DNA Functionalization of Upconversion Nanocrystals for Imaging and In Vivo Drug Delivery
journal, March 2017

  • Han, Sanyang; Samanta, Animesh; Xie, Xiaoji
  • Advanced Materials, Vol. 29, Issue 18
  • DOI: 10.1002/adma.201700244

Photothermal-Responsive Conjugated Polymer Nanoparticles for Remote Control of Gene Expression in Living Cells
journal, January 2018

  • Wang, Yunxia; Li, Shengliang; Zhang, Pengbo
  • Advanced Materials, Vol. 30, Issue 8
  • DOI: 10.1002/adma.201705418

Expanding the Toolbox of Upconversion Nanoparticles for In Vivo Optogenetics and Neuromodulation
journal, August 2019

  • All, Angelo Homayoun; Zeng, Xiao; Teh, Daniel Boon Loong
  • Advanced Materials, Vol. 31, Issue 41
  • DOI: 10.1002/adma.201803474

Nanotransducers for Near‐Infrared Photoregulation in Biomedicine
journal, June 2019


Up-Conversion Fluorescent Labels for Plastic Recycling: A Review
journal, May 2017

  • Gao, Guojun; Turshatov, Andrey; Howard, Ian A.
  • Advanced Sustainable Systems, Vol. 1, Issue 5
  • DOI: 10.1002/adsu.201600033

Advanced Near-Infrared Light-Responsive Nanomaterials as Therapeutic Platforms for Cancer Therapy
journal, November 2018

  • Chien, Yi-Hsin; Chan, Kok Ken; Anderson, Tommy
  • Advanced Therapeutics, Vol. 2, Issue 3
  • DOI: 10.1002/adtp.201800090

A Strategy of NIR Dual‐Excitation Upconversion for Ratiometric Intracellular Detection
journal, September 2019


Intrinsic Time‐Tunable Emissions in Core–Shell Upconverting Nanoparticle Systems
journal, June 2019

  • Tessitore, Gabriella; Maurizio, Steven L.; Sabri, Tarek
  • Angewandte Chemie, Vol. 131, Issue 29
  • DOI: 10.1002/ange.201904445

Intrinsic Time‐Tunable Emissions in Core–Shell Upconverting Nanoparticle Systems
journal, July 2019

  • Tessitore, Gabriella; Maurizio, Steven L.; Sabri, Tarek
  • Angewandte Chemie International Edition, Vol. 58, Issue 29
  • DOI: 10.1002/anie.201904445

Boosting Luminance Energy Transfer Efficiency in Upconversion Nanoparticles with an Energy‐Concentrating Zone
journal, August 2019

  • Zhang, Xiaobo; Chen, Weiwei; Xie, Xiaoyu
  • Angewandte Chemie International Edition, Vol. 58, Issue 35
  • DOI: 10.1002/anie.201906380

Upconversion in Nanostructured Materials: From Optical Tuning to Biomedical Applications
journal, January 2018

  • Sun, Tianying; Ai, Fujin; Zhu, Guangyu
  • Chemistry - An Asian Journal, Vol. 13, Issue 4
  • DOI: 10.1002/asia.201701660

Energy Transfer in Dye-Coupled Lanthanide-Doped Nanoparticles: From Design to Application
journal, February 2018


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journal, October 2019

  • Avellanal‐Zaballa, Edurne; Ventura, Juan; Gartzia‐Rivero, Leire
  • Chemistry – A European Journal, Vol. 25, Issue 65
  • DOI: 10.1002/chem.201903804

Core or Shell? Er 3+ FRET Donors in Upconversion Nanoparticles: Core or Shell? Er 3+ FRET Donors in Upconversion Nanoparticles
journal, October 2017

  • Bhuckory, Shashi; Hemmer, Eva; Wu, Yu-Tang
  • European Journal of Inorganic Chemistry, Vol. 2017, Issue 44
  • DOI: 10.1002/ejic.201700904

Photon Upconversion Kinetic Nanosystems and Their Optical Response: Photon Upconversion Kinetic Nanosystems and Their Optical Response
journal, November 2017

  • Liu, Haichun; Huang, Kai; Valiev, Rashid R.
  • Laser & Photonics Reviews, Vol. 12, Issue 1
  • DOI: 10.1002/lpor.201700144

Organic Soluble LaPO 4 :Eu 3+ Nanorods: Sensitization of Surface Eu 3+ Ions and Phase Transfer in Water
journal, May 2018

  • Vats, Bal Govind; Shafeeq, Muhammed; Singhal, Pallavi
  • ChemistrySelect, Vol. 3, Issue 17
  • DOI: 10.1002/slct.201800276

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journal, July 2017


Miniaturized, Battery-Free Optofluidic Systems with Potential for Wireless Pharmacology and Optogenetics
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Lanthanide Doped Near Infrared Active Upconversion Nanophosphors: Fundamental Concepts, Synthesis Strategies, and Technological Applications
journal, July 2018

  • Lingeshwar Reddy, Kumbam; Balaji, Ramachandran; Kumar, Ashish
  • Small, Vol. 14, Issue 37
  • DOI: 10.1002/smll.201801304

Neodymium‐Sensitized Nanoconstructs for Near‐Infrared Enabled Photomedicine
journal, November 2019


Upconversion Nanoparticles–Based Multiplex Protein Activation to Neuron Ablation for Locomotion Regulation
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Perspectives and challenges of photon-upconversion nanoparticles - Part I: routes to brighter particles and quantitative spectroscopic studies
journal, July 2017

  • Resch-Genger, Ute; Gorris, Hans H.
  • Analytical and Bioanalytical Chemistry, Vol. 409, Issue 25
  • DOI: 10.1007/s00216-017-0499-z

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journal, March 2017


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journal, July 2016

  • Escudero, Alberto; Carrillo-Carrión, Carolina; Zyuzin, Mikhail V.
  • Topics in Current Chemistry, Vol. 374, Issue 4
  • DOI: 10.1007/s41061-016-0049-8

Utilizing the power of Cerenkov light with nanotechnology
journal, February 2017

  • Shaffer, Travis M.; Pratt, Edwin C.; Grimm, Jan
  • Nature Nanotechnology, Vol. 12, Issue 2
  • DOI: 10.1038/nnano.2016.301

Near-infrared light-mediated rare-earth nanocrystals: recent advances in improving photon conversion and alleviating the thermal effect
journal, August 2018


Achieving high-efficiency emission depletion nanoscopy by employing cross relaxation in upconversion nanoparticles
journal, October 2017


Intracellular localization of nanoparticle dimers by chirality reversal
journal, November 2017


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journal, March 2019


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journal, October 2019

  • Zhang, Zhen; Jayakumar, Muthu Kumara Gnanasammandhan; Zheng, Xiang
  • Nature Communications, Vol. 10, Issue 1
  • DOI: 10.1038/s41467-019-12506-w

Continuous-wave upconverting nanoparticle microlasers
journal, June 2018

  • Fernandez-Bravo, Angel; Yao, Kaiyuan; Barnard, Edward S.
  • Nature Nanotechnology, Vol. 13, Issue 7
  • DOI: 10.1038/s41565-018-0161-8

Activation of the surface dark-layer to enhance upconversion in a thermal field
journal, February 2018


Enrichment of molecular antenna triplets amplifies upconverting nanoparticle emission
journal, April 2018


Future and challenges for hybrid upconversion nanosystems
journal, October 2019


A water-dispersible dye-sensitized upconversion nanocomposite modified with phosphatidylcholine for lymphatic imaging
journal, January 2016

  • Zou, Xianmei; Xu, Ming; Yuan, Wei
  • Chemical Communications, Vol. 52, Issue 91
  • DOI: 10.1039/c6cc07180e

Anti-Stokes shift luminescent materials for bio-applications
journal, January 2017

  • Zhu, Xingjun; Su, Qianqian; Feng, Wei
  • Chemical Society Reviews, Vol. 46, Issue 4
  • DOI: 10.1039/c6cs00415f

Dye-sensitized lanthanide-doped upconversion nanoparticles
journal, January 2017

  • Wang, Xindong; Valiev, Rashid R.; Ohulchanskyy, Tymish Y.
  • Chemical Society Reviews, Vol. 46, Issue 14
  • DOI: 10.1039/c7cs00053g

NIR/blue light emission optimization of NaY 1−(x+y) Yb x F 4 :Tm y upconversion nanoparticles via Yb 3+ /Tm 3+ dopant balancing
journal, January 2018

  • Bagheri, Ali; Li, Zheye; Boyer, Cyrille
  • Dalton Transactions, Vol. 47, Issue 26
  • DOI: 10.1039/c7dt04768a

Soft X-ray activated NaYF 4 :Gd/Tb scintillating nanorods for in vivo dual-modal X-ray/X-ray-induced optical bioimaging
journal, January 2018

  • Li, Xiaolong; Xue, Zhenluan; Jiang, Mingyang
  • Nanoscale, Vol. 10, Issue 1
  • DOI: 10.1039/c7nr02926h

Targeted and efficient activation of channelrhodopsins expressed in living cells via specifically-bound upconversion nanoparticles
journal, January 2017

  • Yadav, Kanchan; Chou, Ai-Chuan; Ulaganathan, Rajesh Kumar
  • Nanoscale, Vol. 9, Issue 27
  • DOI: 10.1039/c7nr03246c

Recent progress in upconversion luminescence nanomaterials for biomedical applications
journal, January 2018

  • Duan, Chengchen; Liang, Liuen; Li, Li
  • Journal of Materials Chemistry B, Vol. 6, Issue 2
  • DOI: 10.1039/c7tb02527k

Development of organic semiconducting materials for deep-tissue optical imaging, phototherapy and photoactivation
journal, January 2019

  • Li, Jingchao; Pu, Kanyi
  • Chemical Society Reviews, Vol. 48, Issue 1
  • DOI: 10.1039/c8cs00001h

Upconversion in photodynamic therapy: plumbing the depths
journal, January 2018


Core–shell rare-earth-doped nanostructures in biomedicine
journal, January 2018

  • Labrador-Páez, Lucía; Ximendes, Erving C.; Rodríguez-Sevilla, Paloma
  • Nanoscale, Vol. 10, Issue 27
  • DOI: 10.1039/c8nr02307g

Self-sensitization induced upconversion of Er 3+ in core–shell nanoparticles
journal, January 2018


Dye-sensitized upconversion nanocomposites for ratiometric semi-quantitative detection of hypochlorite in vivo
journal, January 2019

  • Zou, Xianmei; Zhou, Xiaobo; Cao, Cong
  • Nanoscale, Vol. 11, Issue 6
  • DOI: 10.1039/c8nr09531k

Host sensitized intense infrared emissions from Ln 3+ doped GdVO 4 nanocrystals: ranging from 950 nm to 2000 nm
journal, January 2018

  • Samanta, Tuhin; Praveen, Athma E.; Mahalingam, Venkataramanan
  • Journal of Materials Chemistry C, Vol. 6, Issue 18
  • DOI: 10.1039/c8tc00841h

In vivo clearable inorganic nanophotonic materials: designs, materials and applications
journal, January 2019


Yb,Nd,Er-doped upconversion nanoparticles: 980 nm versus 808 nm excitation
journal, January 2019

  • Wiesholler, Lisa M.; Frenzel, Florian; Grauel, Bettina
  • Nanoscale, Vol. 11, Issue 28
  • DOI: 10.1039/c9nr03127h

Upconversion-mediated ZnFe 2 O 4 nanoplatform for NIR-enhanced chemodynamic and photodynamic therapy
journal, January 2019

  • Dong, Shuming; Xu, Jiating; Jia, Tao
  • Chemical Science, Vol. 10, Issue 15
  • DOI: 10.1039/c9sc00387h

Pick your precursor! Tailoring the size and crystal phase of microwave-synthesized sub-10 nm upconverting nanoparticles
journal, January 2019

  • Halimi, Ilias; Rodrigues, Emille M.; Maurizio, Steven L.
  • Journal of Materials Chemistry C, Vol. 7, Issue 48
  • DOI: 10.1039/c9tc04817k

Expanding the toolbox for lanthanide-doped upconversion nanocrystals
journal, July 2019

  • Wu, Yiming; Ang, Melgious Jin Yan; Sun, Mingzi
  • Journal of Physics D: Applied Physics, Vol. 52, Issue 38
  • DOI: 10.1088/1361-6463/ab29c7

Enhanced upconversion luminescence intensity of core–shell NaYF 4 nanocrystals guided by morphological control
journal, January 2019


Sensitization of upconverting nanoparticles with a NIR-emissive cyanine dye using a micellar encapsulation approach
journal, January 2019

  • Saleh, Maysoon I.; Panas, Ihor D.; Frenzel, Florian
  • Methods and Applications in Fluorescence, Vol. 7, Issue 1
  • DOI: 10.1088/2050-6120/aafe1f

Near-infrared deep brain stimulation via upconversion nanoparticle–mediated optogenetics
journal, February 2018


Plasmon-enhanced upconversion: engineering enhancement and quenching at nano and macro scales
journal, January 2018

  • Rasskazov, Ilia L.; Wang, Lang; Murphy, Catherine J.
  • Optical Materials Express, Vol. 8, Issue 12
  • DOI: 10.1364/ome.8.003787

Factors relating to the biodistribution & clearance of nanoparticles & their effects on in vivo application
journal, June 2018


The Impact of Optogenetics on Regenerative Medicine
journal, December 2019

  • Spagnuolo, Gianrico; Genovese, Fabio; Fortunato, Leonzio
  • Applied Sciences, Vol. 10, Issue 1
  • DOI: 10.3390/app10010173

Recent Progress in Upconversion Photodynamic Therapy
journal, May 2018

  • Qiu, Hailong; Tan, Meiling; Ohulchanskyy, Tymish
  • Nanomaterials, Vol. 8, Issue 5
  • DOI: 10.3390/nano8050344