TY - JOUR
T1 - Integrated Metallo-Dielectric 3D Hotspots From High Refractive Index Nanodiamond-Plasmonic Gold Cryosoret Nano-Assemblies for Photonic Crystal Enhanced Fluorescence
AU - Bhaskar, Seemesh
AU - Liu, Weinan
AU - Shepherd, Skye
AU - Wijewardena, Devinda
AU - Tibbs, Joseph
AU - Cunningham, Brian T.
N1 - S.B. and W.L. contributed equally to this work. S.B. is supported by a postdoctoral fellowship from the Woese Institute for Genomic Biology. S.S. thanks the Cancer Center at Illinois for funding. Research was supported by grants from the National Science Foundation (CBET 22–32681) and the National Institutes of Health (R33 CA27227). J.T. is supported by the Illinois Distinguished Fellowship and the National Science Foundation graduate research fellowship. S.B. thanks the research scientists Elbashir Araud, Kathy Walsh, Roddel Remy, Ying He, Duncan Nall, Umnia Doha, and Glenn Fried for their support and research inputs in the characterization of materials. The support from the IGB Core Facilities, instruments including Cypher AFM Asylum, Research WITec Alpha 300 RA Raman-AFM-SNOM and Confocal-Zeiss LSM 710-Multiphoton Microscope, as well as the clean room facility and BioNanotechnology Laboratory (BNL) at HMNTL and the associated research scientists are gratefully acknowledged. The support from the instruments Asylum Research MFP-3D AFM; Hitachi S-4800 High Resolution SEM; Au-Pd Sputter Coater – Emscope SC 500; and JEOL 2100 CRYO TEM, Malvern Zetasizer, and the associated staff and research scientists at Materials Research Laboratory, The Grainger College of Engineering, UIUC, is gratefully acknowledged. The authors thank the feedback provided by all the members of the Nanosensors group, HMNTL, during scientific discussions.
S.B. and W.L. contributed equally to this work. S.B. is supported by a postdoctoral fellowship from the Woese Institute for Genomic Biology. S.S. thanks the Cancer Center at Illinois for funding. Research was supported by grants from the National Science Foundation (CBET 22–32681) and the National Institutes of Health (R33 CA27227). J.T. is supported by the Illinois Distinguished Fellowship and the National Science Foundation graduate research fellowship. S.B. thanks the research scientists Elbashir Araud, Kathy Walsh, Roddel Remy, Ying He, Duncan Nall, Umnia Doha, and Glenn Fried for their support and research inputs in the characterization of materials. The support from the IGB Core Facilities, instruments including Cypher AFM Asylum, Research WITec Alpha 300 RA Raman‐AFM‐SNOM and Confocal‐Zeiss LSM 710‐Multiphoton Microscope, as well as the clean room facility and BioNanotechnology Laboratory (BNL) at HMNTL and the associated research scientists are gratefully acknowledged. The support from the instruments Asylum Research MFP‐3D AFM; Hitachi S‐4800 High Resolution SEM; Au‐Pd Sputter Coater – Emscope SC 500; and JEOL 2100 CRYO TEM, Malvern Zetasizer, and the associated staff and research scientists at Materials Research Laboratory, The Grainger College of Engineering, UIUC, is gratefully acknowledged. The authors thank the feedback provided by all the members of the Nanosensors group, HMNTL, during scientific discussions.
PY - 2025/10
Y1 - 2025/10
N2 - Hybridizing fluorescent reporters with gold nanoparticles (AuNPs) presents challenges associated with surface-induced quenching in the “zone of inactivity,” compromising the functionality of related point-of-care diagnostic tools. Nano-assembly of high refractive index (HRI) dielectric and plasmonic NPs yields augmented electric and magnetic resonances that are not achievable with the individual counterparts. Here, several long-standing challenges associated with conventional photon-emitting reporters are addressed by integrating HRI dielectric fluorescent nanodiamonds (NDs) with metallo-dielectric nano-assemblies. An adiabatic cooling (−196 °C) driven nano-assembly method is used to synthesize AuND cryosoret (AuNDCS) nano-assemblies. More than 600-fold enhancement of the emission from the nitrogen vacancy of AuNDCS is demonstrated when interfaced with a photonic crystal through interaction with the radiating guided mode resonance. Experimental results are corroborated with extensive simulations of a variety of nano-constructs, including monomers (0D), dimers (1D), trimers (2D), and tetramers (3D) to visualize the electric and magnetic field hotspots. The fluorescence enhancement is utilized to detect a cancer-specific target biomarker, micro-RNA 375, with femtomolar-level detection limits, using the AuNDCS as a molecular tag. The PC-enhanced fluorescence detection instrument does not require prisms, objectives, or cooled photodetectors, resulting in a compact and inexpensive system that would be suitable for environments outside of conventional diagnostic laboratories.
AB - Hybridizing fluorescent reporters with gold nanoparticles (AuNPs) presents challenges associated with surface-induced quenching in the “zone of inactivity,” compromising the functionality of related point-of-care diagnostic tools. Nano-assembly of high refractive index (HRI) dielectric and plasmonic NPs yields augmented electric and magnetic resonances that are not achievable with the individual counterparts. Here, several long-standing challenges associated with conventional photon-emitting reporters are addressed by integrating HRI dielectric fluorescent nanodiamonds (NDs) with metallo-dielectric nano-assemblies. An adiabatic cooling (−196 °C) driven nano-assembly method is used to synthesize AuND cryosoret (AuNDCS) nano-assemblies. More than 600-fold enhancement of the emission from the nitrogen vacancy of AuNDCS is demonstrated when interfaced with a photonic crystal through interaction with the radiating guided mode resonance. Experimental results are corroborated with extensive simulations of a variety of nano-constructs, including monomers (0D), dimers (1D), trimers (2D), and tetramers (3D) to visualize the electric and magnetic field hotspots. The fluorescence enhancement is utilized to detect a cancer-specific target biomarker, micro-RNA 375, with femtomolar-level detection limits, using the AuNDCS as a molecular tag. The PC-enhanced fluorescence detection instrument does not require prisms, objectives, or cooled photodetectors, resulting in a compact and inexpensive system that would be suitable for environments outside of conventional diagnostic laboratories.
KW - cryosorets
KW - electric and magnetic hotspot
KW - gold nanoparticles
KW - guided mode resonance
KW - micro-RNA detection
KW - nanodiamonds
KW - photonic crystal
UR - https://www.scopus.com/pages/publications/105018199060
UR - https://www.scopus.com/pages/publications/105018199060#tab=citedBy
U2 - 10.1002/adfm.202512295
DO - 10.1002/adfm.202512295
M3 - Article
AN - SCOPUS:105018199060
SN - 1616-301X
VL - 36
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 5
M1 - e12295
ER -