Amorphous Quantum Nanomaterials

Kohle, Ferdinand F.  E.; Hinckley, Joshua A.; Li, Songying; Dhawan, Nikhil; Katt, William P.; Erstling, Jacob A.; Werner-Zwanziger, Ulrike; Zwanziger, Josef; Cerione, Richard A.; Wiesner, Ulrich B.

doi:10.1002/adma.201806993

Title: Amorphous Quantum Nanomaterials

Journal Article · 05 December 2018 · Advanced Materials

DOI: https://doi.org/10.1002/adma.201806993 · OSTI ID:1593724

Kohle, Ferdinand F. E. ^[1];

^[2]; Li, Songying ^[2]; Dhawan, Nikhil ^[2]; Katt, William P. ^[2]; Erstling, Jacob A. ^[2]; Werner-Zwanziger, Ulrike ^[3]; Zwanziger, Josef ^[3]; Cerione, Richard A. ^[2];

^[2]

Cornell Univ., Ithaca, NY (United States); Cornell University
Cornell Univ., Ithaca, NY (United States)
Dalhousie Univ., Halifax, Nova Scotia (Canada)

In quantum materials macroscopic behavior is governed in non-trivial ways by quantum phenomena. This is usually achieved by exquisite control over atomic positions in crystalline solids. Here we demonstrate that the use of disordered glassy materials provides unique opportunities to tailor quantum material properties. By borrowing ideas from single molecule spectroscopy, we isolate single delocalized π-electron dye systems in relatively rigid ultrasmall (<10nm diameter) amorphous silica nanoparticles. We demonstrate that chemically tuning the local amorphous silica environment around the dye over a range of compositions enables exquisite control over dye quantum behavior, leading to efficient probes for photodynamic therapy (PDT) and stochastic optical reconstruction microscopy (STORM). Results suggest that efficient fine-tuning of light-induced quantum behavior mediated via effects like spin-orbit coupling can be effectively achieved by systematically varying averaged local environments in glassy amorphous materials as opposed to tailoring well-defined neighboring atomic lattice positions in crystalline solids. Finally, resulting nanoprobes have required features proven to enable clinical translation.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Cornell Univ., Ithaca, NY (United States)

Sponsoring Organization:: National Institutes of Health (NIH); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0010560

OSTI ID:: 1593724

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 5 Vol. 31; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (41)

Super-Resolution Imaging with Small Organic Fluorophores Heilemann, Mike; van de Linde, Sebastian; Mukherjee, Anindita Angewandte Chemie International Edition, Vol. 48, Issue 37 https://doi.org/10.1002/anie.200902073	journal	September 2009
Toxicological Studies of 2-Mercaptoethanol White, Kenneth; Bruckner, J. V.; Guess, W. L. Journal of Pharmaceutical Sciences, Vol. 62, Issue 2 https://doi.org/10.1002/jps.2600620211	journal	February 1973
Photoswitching Mechanism of Cyanine Dyes Dempsey, Graham T.; Bates, Mark; Kowtoniuk, Walter E. Biophysical Journal, Vol. 98, Issue 3 https://doi.org/10.1016/j.bpj.2009.12.2126	journal	January 2010
Multimodal Biophotonics of Semiconducting Polymer Nanoparticles Jiang, Yuyan; Pu, Kanyi Accounts of Chemical Research, Vol. 51, Issue 8 https://doi.org/10.1021/acs.accounts.8b00242	journal	July 2018
Control of Ultrasmall Sub-10 nm Ligand-Functionalized Fluorescent Core–Shell Silica Nanoparticle Growth in Water Ma, Kai; Mendoza, Carlie; Hanson, Margaret Chemistry of Materials, Vol. 27, Issue 11 https://doi.org/10.1021/acs.chemmater.5b01222	journal	May 2015
Elucidating the Mechanism of Silica Nanoparticle PEGylation Processes Using Fluorescence Correlation Spectroscopies Ma, Kai; Zhang, Duhan; Cong, Ying Chemistry of Materials, Vol. 28, Issue 5 https://doi.org/10.1021/acs.chemmater.6b00030	journal	February 2016
Modular and Orthogonal Post-PEGylation Surface Modifications by Insertion Enabling Penta-Functional Ultrasmall Organic-Silica Hybrid Nanoparticles Ma, Kai; Wiesner, Ulrich Chemistry of Materials, Vol. 29, Issue 16 https://doi.org/10.1021/acs.chemmater.7b02009	journal	August 2017
Photochemical heavy-atom effects Koziar, Joseph C.; Cowan, Dwaine O. Accounts of Chemical Research, Vol. 11, Issue 9 https://doi.org/10.1021/ar50129a003	journal	September 1978
Silica Nanoparticle Architecture Determines Radiative Properties of Encapsulated Fluorophores Larson, Daniel R.; Ow, Hooisweng; Vishwasrao, Harshad D. Chemistry of Materials, Vol. 20, Issue 8 https://doi.org/10.1021/cm7026866	journal	April 2008
Nanoparticles in Photodynamic Therapy Lucky, Sasidharan Swarnalatha; Soo, Khee Chee; Zhang, Yong Chemical Reviews, Vol. 115, Issue 4 https://doi.org/10.1021/cr5004198	journal	January 2015
Fluorescence correlation spectroscopy of triplet states in solution: a theoretical and experimental study Widengren, Jerker; Mets, Uelo; Rigler, Rudolf The Journal of Physical Chemistry, Vol. 99, Issue 36 https://doi.org/10.1021/j100036a009	journal	September 1995
Carbocyanine Dyes as Efficient Reversible Single-Molecule Optical Switch Heilemann, Mike; Margeat, Emmanuel; Kasper, Robert Journal of the American Chemical Society, Vol. 127, Issue 11 https://doi.org/10.1021/ja044686x	journal	March 2005
Photoswitching Mechanism of Cyanine Dyes Dempsey, Graham T.; Bates, Mark; Kowtoniuk, Walter E. Journal of the American Chemical Society, Vol. 131, Issue 51 https://doi.org/10.1021/ja904588g	journal	December 2009
Characterization of Photoinduced Isomerization and Back-Isomerization of the Cyanine Dye Cy5 by Fluorescence Correlation Spectroscopy Widengren, Jerker; Schwille, Petra The Journal of Physical Chemistry A, Vol. 104, Issue 27 https://doi.org/10.1021/jp000059s	journal	July 2000
Iodide as a Fluorescence Quencher and Promoter—Mechanisms and Possible Implications Chmyrov, Andriy; Sandén, Tor; Widengren, Jerker The Journal of Physical Chemistry B, Vol. 114, Issue 34 https://doi.org/10.1021/jp103837f	journal	September 2010
External Heavy-Atomic Construction of Photosensitizer Nanoparticles for Enhanced in Vitro Photodynamic Therapy of Cancer Zhou, Lin; Wei, Shaohua; Ge, Xuefeng The Journal of Physical Chemistry B, Vol. 116, Issue 42 https://doi.org/10.1021/jp305137j	journal	October 2012
Organically Modified Silica Nanoparticles with Intraparticle Heavy-Atom Effect on the Encapsulated Photosensitizer for Enhanced Efficacy of Photodynamic Therapy Kim, Sehoon; Ohulchanskyy, Tymish Y.; Bharali, Dhruba The Journal of Physical Chemistry C, Vol. 113, Issue 29 https://doi.org/10.1021/jp900573s	journal	June 2009
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems Engel, Gregory S.; Calhoun, Tessa R.; Read, Elizabeth L. Nature, Vol. 446, Issue 7137 https://doi.org/10.1038/nature05678	journal	April 2007
Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic Mundy, Julia A.; Brooks, Charles M.; Holtz, Megan E. Nature, Vol. 537, Issue 7621 https://doi.org/10.1038/nature19343	journal	September 2016
Negative-pressure-induced enhancement in a freestanding ferroelectric Wang, Jin; Wylie-van Eerd, Ben; Sluka, Tomas Nature Materials, Vol. 14, Issue 10 https://doi.org/10.1038/nmat4365	journal	August 2015
Evaluation of fluorophores for optimal performance in localization-based super-resolution imaging Dempsey, Graham T.; Vaughan, Joshua C.; Chen, Kok Hao Nature Methods, Vol. 8, Issue 12 https://doi.org/10.1038/nmeth.1768	journal	November 2011
Sub-diffraction-limit imaging by stochastic optical reconstruction microscopy (STORM) Rust, Michael J.; Bates, Mark; Zhuang, Xiaowei Nature Methods, Vol. 3, Issue 10 https://doi.org/10.1038/nmeth929	journal	August 2006
Charge transport in strongly coupled quantum dot solids Kagan, Cherie R.; Murray, Christopher B. Nature Nanotechnology, Vol. 10, Issue 12 https://doi.org/10.1038/nnano.2015.247	journal	November 2015
Emergent functions of quantum materials Tokura, Yoshinori; Kawasaki, Masashi; Nagaosa, Naoto Nature Physics, Vol. 13, Issue 11 https://doi.org/10.1038/nphys4274	journal	September 2017
Direct stochastic optical reconstruction microscopy with standard fluorescent probes van de Linde, Sebastian; Löschberger, Anna; Klein, Teresa Nature Protocols, Vol. 6, Issue 7 https://doi.org/10.1038/nprot.2011.336	journal	June 2011
Fluorescent probes for super-resolution imaging in living cells Fernández-Suárez, Marta; Ting, Alice Y. Nature Reviews Molecular Cell Biology, Vol. 9, Issue 12 https://doi.org/10.1038/nrm2531	journal	November 2008
Ultrasmall targeted nanoparticles with engineered antibody fragments for imaging detection of HER2-overexpressing breast cancer Chen, Feng; Ma, Kai; Madajewski, Brian Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-06271-5	journal	October 2018
Three-dimensional total-internal reflection fluorescence nanoscopy with nanometric axial resolution by photometric localization of single molecules Szalai, Alan M.; Siarry, Bruno; Lukin, Jerónimo Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-020-20863-0	journal	January 2021
Identification and characterization of diverse coherences in the Fenna–Matthews–Olson complex Thyrhaug, Erling; Tempelaar, Roel; Alcocer, Marcelo J. P. Nature Chemistry, Vol. 10, Issue 7 https://doi.org/10.1038/s41557-018-0060-5	journal	May 2018
Single-molecule spectroscopy and imaging over the decades Moerner, W. E.; Shechtman, Yoav; Wang, Quan Faraday Discussions, Vol. 184 https://doi.org/10.1039/C5FD00149H	journal	January 2015
Oxidative transformation of thiol groups to disulfide bonds in mesoporous silicas: a diagnostic reaction for probing distribution of organic functional groups Kao, Hsien-Ming; Chiu, Po-Jui; Jheng, Guang-Liang New Journal of Chemistry, Vol. 33, Issue 11 https://doi.org/10.1039/b9nj00389d	journal	January 2009
Collisional Perturbation of Spin‐Orbital Coupling and the Mechanism of Fluorescence Quenching. A Visual Demonstration of the Perturbation Kasha, Michael The Journal of Chemical Physics, Vol. 20, Issue 1 https://doi.org/10.1063/1.1700199	journal	January 1952
Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state Brus, L. E. The Journal of Chemical Physics, Vol. 80, Issue 9 https://doi.org/10.1063/1.447218	journal	May 1984
ThunderSTORM: a comprehensive ImageJ plug-in for PALM and STORM data analysis and super-resolution imaging Ovesný, Martin; Křížek, Pavel; Borkovec, Josef Bioinformatics, Vol. 30, Issue 16 https://doi.org/10.1093/bioinformatics/btu202	journal	May 2014
Breaking the Diffraction Barrier in Fluorescence Microscopy by Optical Shelving Bretschneider, Stefan; Eggeling, Christian; Hell, Stefan W. Physical Review Letters, Vol. 98, Issue 21 https://doi.org/10.1103/PhysRevLett.98.218103	journal	May 2007
Communication in the Presence of Noise Shannon, C. E. Proceedings of the IRE, Vol. 37, Issue 1 https://doi.org/10.1109/JRPROC.1949.232969	journal	January 1949
Communication In The Presence Of Noise Shannon, C. E. Proceedings of the IEEE, Vol. 86, Issue 2 https://doi.org/10.1109/jproc.1998.659497	journal	February 1998
Communication in the presence of noise Shannon, C. E. Proceedings of the IEEE, Vol. 72, Issue 9 https://doi.org/10.1109/proc.1984.12998	journal	January 1984
Clinical translation of an ultrasmall inorganic optical-PET imaging nanoparticle probe Phillips, E.; Penate-Medina, O.; Zanzonico, P. B. Science Translational Medicine, Vol. 6, Issue 260 https://doi.org/10.1126/scitranslmed.3009524	journal	October 2014
Basic Research Needs Workshop on Quantum Materials for Energy Relevant Technology Broholm, Collin; Fisher, Ian; Moore, Joel https://doi.org/10.2172/1616509	report	February 2016
Dye Sensitizers for Photodynamic Therapy Ormond, Alexandra; Freeman, Harold Materials, Vol. 6, Issue 3 https://doi.org/10.3390/ma6030817	journal	March 2013

Similar Records

Dye Encapsulation in Fluorescent Core–Shell Silica Nanoparticles as Probed by Fluorescence Correlation Spectroscopy

Journal Article · 2019 · Journal of Physical Chemistry. C · OSTI ID:1593725

Kohle, Ferdinand F. E.; Hinckley, Joshua A.; Wiesner, Ulrich B.

Porous cage-derived nanomaterial inks for direct and internal three-dimensional printing

Journal Article · 2020 · Nature Communications · OSTI ID:1802126

Aubert, Tangi; Huang, Jen-Yu; Ma, Kai; +2 more

Artificial zeolites

Patent · 2023 · OSTI ID:1998371

Elam, Jeffrey W.; Canlas, Christian P.

Related Subjects

36 MATERIALS SCIENCE
amorphous silica nanoparticles
optical super-resolution microscopy
organic dyes
photodynamic theraphy (PDT)

Title: Amorphous Quantum Nanomaterials

Citation Formats

References (41)

Similar Records

Related Subjects