Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

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

Journal Article · · Journal of Physical Chemistry. C
Synthetic advances in the formation of ultrasmall (<10 nm) fluorescent poly(ethylene glycol)-coated (PEGylated) core–shell silica nanoparticles (SNPs), enabling improved particle size and surface chemical property control, have led to successful clinical translation of SNPs as diagnostic probes in oncology. Despite the success of such probes, details of the dye incorporation and resulting silica architecture are still poorly understood. Here, we employ afterpulse-corrected fluorescence correlation spectroscopy (FCS) to monitor fast fluorescence fluctuations (lag times <10–5 s) of the negatively charged cyanine dye Cy5 as a probe to study such details for dye encapsulation in 5 nm silica cores of PEGylated core–shell SNPs (C dots). Upon deposition of additional silica shells over the silica core, we find that the amplitude of photoinduced cis–trans isomerization decreases, suggesting that the Cy5 dyes are located near or on the surface of the original SNP cores. In combination with time-correlated fluorescence decay measurements, we deduce radiative and nonradiative rates of the Cy5 dye in these particles. Finally, results demonstrate that FCS is a well-suited tool to investigate aspects of the photophysics of fluorescent nanoparticles, and that conformational changes of cyanine dyes like Cy5 are excellent indicators for the local dye environment within ultrasmall SNPs.
Research Organization:
Cornell Univ., Ithaca, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); National Institutes of Health (NIH)
Grant/Contract Number:
SC0010560
OSTI ID:
1593725
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 15 Vol. 123; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (50)

Amorphous Quantum Nanomaterials journal December 2018
Fluorescence correlation spectroscopy. I. Conceptual basis and theory journal January 1974
Fluorescence correlation spectroscopy. II. An experimental realization journal January 1974
Fluorescence correlation spectroscopy and Brownian rotational diffusion journal January 1975
Large Stokes-Shift Fluorescent Silica Nanoparticles with Enhanced Emission Over Free Dye for Single Excitation Multiplexing: Large Stokes-Shift Fluorescent Silica Nanoparticles with … journal September 2009
Contrast variation in light scattering: Silica spheres dispersed in apolar solvent mixtures journal August 1980
Correction for refractive index in the comparison of radiative lifetimes in vapour and solution phases journal January 1980
Rotational brownian motion and fluorescence intensify fluctuations journal June 1974
Analysis of Coupled Bimolecular Reaction Kinetics and Diffusion byTwo-Color Fluorescence Correlation Spectroscopy: Enhanced Resolution of Kinetics by Resonance Energy Transfer journal July 2002
Separation of the rotational contribution in fluorescence correlation experiments journal February 1989
Photodynamic properties of green fluorescent proteins investigated by fluorescence correlation spectroscopy journal December 1999
Ultrasmall dual-modality silica nanoparticle drug conjugates: Design, synthesis, and characterization journal November 2015
Cyanine dyes in biophysical research: the photophysics of polymethine fluorescent dyes in biomolecular environments journal November 2010
Comparison of Photophysical and Colloidal Properties of Biocompatible Semiconductor Nanocrystals Using Fluorescence Correlation Spectroscopy journal April 2005
Sensitive Single Particle Method for Characterizing Rapid Rotational and Translational Diffusion and Aspect Ratio of Anisotropic Nanoparticles and Its Application in Immunoassays journal September 2013
Trans–Cis Isomerization of Lipophilic Dyes Probing Membrane Microviscosity in Biological Membranes and in Live Cells journal May 2015
Control of Ultrasmall Sub-10 nm Ligand-Functionalized Fluorescent Core–Shell Silica Nanoparticle Growth in Water journal May 2015
Elucidating the Mechanism of Silica Nanoparticle PEGylation Processes Using Fluorescence Correlation Spectroscopies journal February 2016
Quantitative Measure of the Size Dispersity in Ultrasmall Fluorescent Organic–Inorganic Hybrid Core–Shell Silica Nanoparticles by Small-Angle X-ray Scattering journal January 2019
Dynamics of Nanoparticles in Entangled Polymer Solutions journal December 2017
Melanocortin-1 Receptor-Targeting Ultrasmall Silica Nanoparticles for Dual-Modality Human Melanoma Imaging journal January 2018
Nanotechnology Strategies To Advance Outcomes in Clinical Cancer Care journal December 2017
High-Performance Chromatographic Characterization of Surface Chemical Heterogeneities of Fluorescent Organic–Inorganic Hybrid Core–Shell Silica Nanoparticles journal January 2019
Cyanine dye labeling reagents: Sulfoindocyanine succinimidyl esters journal March 1993
Single Dye Molecule Behavior in Fluorescent Core–Shell Silica Nanoparticles journal December 2011
Silica Nanoparticle Architecture Determines Radiative Properties of Encapsulated Fluorophores journal April 2008
Single-Molecule Fluorescence Studies of Protein Folding and Conformational Dynamics journal May 2006
Fluorescence correlation spectroscopy of triplet states in solution: a theoretical and experimental study journal September 1995
Rotational and Translational Diffusion of Peptide-Coated CdSe/CdS/ZnS Nanorods Studied by Fluorescence Correlation Spectroscopy journal February 2006
Characterization of Photoinduced Isomerization and Back-Isomerization of the Cyanine Dye Cy5 by Fluorescence Correlation Spectroscopy journal July 2000
Accurate Sizing of Nanoparticles Using Confocal Correlation Spectroscopy journal December 2006
Two-Photon Fluorescence Correlation Spectroscopy of Gold Nanoparticles under Stationary and Flow Conditions journal October 2014
Amplitude of Relaxations in Fluorescence Correlation Spectroscopy for Fluorophores That Diffuse Together journal January 2013
Bright and Stable Core−Shell Fluorescent Silica Nanoparticles journal January 2005
Photophysics of Cy3-Encapsulated Calcium Phosphate Nanoparticles journal April 2009
A quantitative fluorescence study of protein monolayer formation on colloidal nanoparticles journal August 2009
Ultrasmall targeted nanoparticles with engineered antibody fragments for imaging detection of HER2-overexpressing breast cancer journal October 2018
Self-assembly of highly symmetrical, ultrasmall inorganic cages directed by surfactant micelles journal June 2018
Fluorescence correlation spectroscopy in polymer science journal January 2014
Relative fluorescence quantum yields using a computer-controlled luminescence spectrometer journal January 1983
Dye structure–optical property correlations in near-infrared fluorescent core-shell silica nanoparticles journal January 2009
Relationship between Absorption Intensity and Fluorescence Lifetime of Molecules journal August 1962
Thermodynamic Fluctuations in a Reacting System—Measurement by Fluorescence Correlation Spectroscopy journal September 1972
Core-shell silica nanoparticles as fluorescent labels for nanomedicine journal January 2007
Clinical translation of an ultrasmall inorganic optical-PET imaging nanoparticle probe journal October 2014
An Algorithm for Least-Squares Estimation of Nonlinear Parameters journal June 1963
Introduction to Polymers book June 2011
Afterpulsing and its correction in fluorescence correlation spectroscopy experiments journal January 2003
Fluorescence Correlation Spectroscopy and Its Potential for Intracellular Applications journal January 2001
Tunable Blinking Kinetics of Cy5 for Precise DNA Quantification and Single-Nucleotide Difference Detection journal July 2008

Cited By (1)