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Article ; Online: Developing FRET Networks for Sensing.

Algar, W Russ / Krause, Katherine D

Annual review of analytical chemistry (Palo Alto, Calif.)

2022 Volume 15, Issue 1, Page(s) 17–36

Abstract: Förster resonance energy transfer (FRET) is a widely used fluorescence-based sensing mechanism. To date, most implementations of FRET sensors have relied on a discrete donor-acceptor pair for detection of each analytical target. FRET networks are an ... ...

Abstract	Förster resonance energy transfer (FRET) is a widely used fluorescence-based sensing mechanism. To date, most implementations of FRET sensors have relied on a discrete donor-acceptor pair for detection of each analytical target. FRET networks are an emerging concept in which target recognition perturbs a set of interconnected FRET pathways between multiple emitters. Here, we review the energy transfer topologies and scaffold materials for FRET networks, propose a general nomenclature, and qualitatively summarize the dynamics of the competitive, sequential, homoFRET, and heteroFRET pathways that constitute FRET networks. Implementations of FRET networks for sensing are also described, including concentric FRET probes, other single-vector multiplexing, and logic gates and switches. Unresolved questions and future research directions for current systems are discussed, as are potential but currently unexplored applications of FRET networks in sensing.
MeSH term(s)	Fluorescence Resonance Energy Transfer ; Quantum Dots
Language	English
Publishing date	2022-03-17
Publishing country	United States
Document type	Journal Article ; Review ; Research Support, Non-U.S. Gov't
ZDB-ID	2398707-8
ISSN	1936-1335 ; 1936-1327
ISSN (online)	1936-1335
ISSN	1936-1327
DOI	10.1146/annurev-anchem-061020-014925
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: A Dendrimer-Based Time-Gated Concentric FRET Configuration for Multiplexed Sensing.

Tsai, Hsin-Yun / Algar, W Russ

ACS nano

2022 Volume 16, Issue 5, Page(s) 8150–8160

Abstract: Förster resonance energy transfer (FRET) is widely used for the development of biological probes and sensors. In this context, the norm for multiplexed detection is deployment of multiple probes, each a discrete donor-acceptor pair. Concentric FRET ( ... ...

Abstract	Förster resonance energy transfer (FRET) is widely used for the development of biological probes and sensors. In this context, the norm for multiplexed detection is deployment of multiple probes, each a discrete donor-acceptor pair. Concentric FRET (cFRET) probes enable multiplexed sensing with a single vector but, to date, have only been developed around semiconductor quantum dots, which may limit the scope of biological applications for such probes. Here, we demonstrate that dendrimers labeled with a luminescent terbium complex (Tb) are a viable and advantageous alternative platform for cFRET probes. Polyamidoamine dendrimers were functionalized with Tb, biotin, NeutrAvidin, and three types of dye-labeled oligonucleotide probes to establish a network of competitive and sequential Tb-to-dye and dye-to-dye FRET pathways. These probes were characterized physically and photophysically, and a time-gated multiplexed assay for DNA targets was demonstrated. The time-gating offered by the Tb allowed the rejection of background autofluorescence from serum. More broadly, this dendrimer-based architecture shows that cFRET is a general concept and is an important step toward a new generation of probes for biological sensing.
MeSH term(s)	Fluorescence Resonance Energy Transfer ; Dendrimers ; Quantum Dots ; Terbium ; Luminescence
Chemical Substances	Dendrimers ; Terbium (06SSF7P179)
Language	English
Publishing date	2022-05-02
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1936-086X
ISSN (online)	1936-086X
DOI	10.1021/acsnano.2c01473
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Article ; Online: Are We There Yet? Intracellular Sensing with Luminescent Nanoparticles and FRET

Algar, W. Russ / Szwarczewski, Agnes / Massey, Melissa

Analytical Chemistry. 2023 Jan. 03, v. 95, no. 2 p.551-559

2023

Abstract: Combinations of luminescent nanoparticles (LNPs) and Förster resonance energy transfer (FRET) offer properties and features that are advantageous for sensing of biomolecular targets and activity. Despite a multitude of designs for LNP-FRET sensors, ... ...

Abstract	Combinations of luminescent nanoparticles (LNPs) and Förster resonance energy transfer (FRET) offer properties and features that are advantageous for sensing of biomolecular targets and activity. Despite a multitude of designs for LNP-FRET sensors, intracellular sensing applications are underdeveloped. We introduce readers to this field, summarize essential concepts, meta-analyze the literature, and offer a perspective on the bottleneck in LNP-FRET sensor development.
Keywords	analytical chemistry ; energy transfer ; luminescence ; nanoparticles
Language	English
Dates of publication	2023-0103
Size	p. 551-559.
Publishing place	American Chemical Society
Document type	Article ; Online
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.2c03751
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Dextran-Functionalized Super-nanoparticle Assemblies of Quantum Dots for Enhanced Cellular Immunolabeling and Imaging.

Rees, Kelly / Darwish, Ghinwa H / Algar, W Russ

ACS applied materials & interfaces

2023 Volume 15, Issue 15, Page(s) 18672–18684

Abstract: Colloidal semiconductor quantum dots (QDs) are a popular material for applications in bioanalysis and imaging. Although individual QDs are bright, some applications benefit from the use of even brighter materials. One approach to achieve higher ... ...

Abstract	Colloidal semiconductor quantum dots (QDs) are a popular material for applications in bioanalysis and imaging. Although individual QDs are bright, some applications benefit from the use of even brighter materials. One approach to achieve higher brightness is to form super-nanoparticle (super-NP) assemblies of many QDs. Here, we present the preparation, characterization, and utility of dextran-functionalized super-NP assemblies of QDs. Amphiphilic dextran was synthesized and used to encapsulate many hydrophobic QDs via a simple emulsion-based method. The resulting super-NP assemblies or "super-QDs" had hydrodynamic diameters of
MeSH term(s)	Quantum Dots/chemistry ; Dextrans ; Nanoparticles/chemistry ; Semiconductors ; Diagnostic Imaging
Chemical Substances	Dextrans
Language	English
Publishing date	2023-04-05
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.3c00861
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Assessing the Steric Impact of Surface Ligands on the Proteolytic Turnover of Quantum Dot-Peptide Conjugates.

Krause, Katherine D / Rees, Kelly / Algar, W Russ

ACS applied materials & interfaces

2023

Abstract: Proteases are important biomarkers and targets for the diagnosis and treatment of disease. The advantageous properties of semiconductor quantum dots (QDs) have made these nanoparticles useful as probes for protease activity; however, the effects of QD ... ...

Abstract	Proteases are important biomarkers and targets for the diagnosis and treatment of disease. The advantageous properties of semiconductor quantum dots (QDs) have made these nanoparticles useful as probes for protease activity; however, the effects of QD surface chemistry on protease activity are not yet fully understood. Here, we present a systematic study of the impact of sterics on the proteolysis of QD-peptide conjugates. The study utilized eight proteases (chymotrypsin, trypsin, endoproteinase Lys C, papain, endoproteinase Arg C, thrombin, factor Xa, and plasmin) and 41 distinct surface chemistries. The latter included three molecular weights of each of three macromolecular ligands derived from dextran and polyethylene glycol, as well as anionic and zwitterionic small-molecule ligands, and an array of mixed coatings of macromolecular and small-molecule ligands. These surface chemistries spanned a diversity of thicknesses, densities, and packing organization, as characterized by gel electrophoresis, capillary electrophoresis, dynamic light scattering, and infrared spectroscopy. The macromolecular ligands decreased the adsorption of proteases on the QDs and decelerated proteolysis of the QD-peptide conjugates via steric hindrance. The properties of the QD surface chemistry, rather than the protease properties, were the main factor in determining the magnitude of deceleration. The broad scope of this study provides insights into the many ways in which QD surface chemistry affects protease activity, and will inform the development of optimized nanoparticle-peptide conjugates for sensing of protease activity and resistance to unwanted proteolysis.
Language	English
Publishing date	2023-12-04
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.3c12665
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Article ; Online: Quantitative and Multiplexed Chopper-Based Time-Gated Imaging for Bioanalysis on a Smartphone.

Kanani, Sahil S / Tsai, Hsin-Yun / Algar, W Russ

Analytical chemistry

2023 Volume 95, Issue 35, Page(s) 13258–13265

Abstract: Smartphones are emerging platforms for point-of-care diagnostics (POCDs), where the on-board camera is, for example, used to image fluorescence. Many laboratory instruments are capable of time-gated (TG) photoluminescence (PL) measurements─an analytical ... ...

Abstract	Smartphones are emerging platforms for point-of-care diagnostics (POCDs), where the on-board camera is, for example, used to image fluorescence. Many laboratory instruments are capable of time-gated (TG) photoluminescence (PL) measurements─an analytical method leveraged by multiple commercial assay kits. When paired with long-lived PL emitters such as luminescent lanthanide complexes (LLCs), time-gating eliminates background from sample autofluorescence and many other sources. This capability is amenable to minimally processed samples and would thus be useful for POCDs on a smartphone-based platform. Here, we report a double-chopper design for TG PL imaging using a portable, 3D-printed, smartphone-based device. The rotation speed, dimensions, and overlap of the chopper blades and gaps set the timing parameters, with delay times on the order of hundreds of microseconds to milliseconds. The device was capable of quantitative TG imaging of PL from terbium(III) and europium(III) LLCs, including rejection of short-lived PL background from serum and tissue phantoms, spectral and temporal multiplexing, a model time-gated Förster resonance energy transfer (TG-FRET) assay, and imaging of cells. As the first smartphone-based demonstrations of these important analytical capabilities, this work is an important foundation for developing POCD methods based on TG PL imaging.
MeSH term(s)	Smartphone ; Diagnostic Imaging ; Phantoms, Imaging ; Biological Assay ; Europium ; Lanthanoid Series Elements
Chemical Substances	Europium (444W947O8O) ; Lanthanoid Series Elements
Language	English
Publishing date	2023-08-23
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.3c02397
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Article ; Online: Are We There Yet? Intracellular Sensing with Luminescent Nanoparticles and FRET.

Algar, W Russ / Szwarczewski, Agnes / Massey, Melissa

Analytical chemistry

2023 Volume 95, Issue 2, Page(s) 551–559

Abstract	Combinations of luminescent nanoparticles (LNPs) and Förster resonance energy transfer (FRET) offer properties and features that are advantageous for sensing of biomolecular targets and activity. Despite a multitude of designs for LNP-FRET sensors, intracellular sensing applications are underdeveloped. We introduce readers to this field, summarize essential concepts, meta-analyze the literature, and offer a perspective on the bottleneck in LNP-FRET sensor development.
MeSH term(s)	Fluorescence Resonance Energy Transfer ; Nanoparticles ; Luminescence ; Luminescent Proteins
Chemical Substances	Luminescent Proteins
Language	English
Publishing date	2023-01-03
Publishing country	United States
Document type	News ; Research Support, Non-U.S. Gov't
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.2c03751
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Article ; Online: Supra-Quantum Dot Assemblies to Maximize Color-Based Multiplexed Fluorescence Detection with a Smartphone Camera.

Darwish, Ghinwa H / Baker, Daina V / Algar, W Russ

ACS sensors

2023 Volume 8, Issue 12, Page(s) 4686–4695

Abstract: Photoluminescence (PL) imaging and bioanalysis with smartphone-based devices are of growing interest for point-of-care/point-of-need diagnostics. Strategies for maximizing sensitivity have been explored in this context, but color multiplexing has been ... ...

Abstract	Photoluminescence (PL) imaging and bioanalysis with smartphone-based devices are of growing interest for point-of-care/point-of-need diagnostics. Strategies for maximizing sensitivity have been explored in this context, but color multiplexing has been very limited, with its maximum level unexplored. Here, we evaluated color multiplexing with smartphone-based PL imaging by using supra-nanoparticle assemblies of quantum dots (supra-QDs). These materials were prepared as composite colors that were tailored to the red-green-blue (RGB) color space of smartphone cameras by coassembling different ratios of R-, G-, and B-emitting QDs on a silica nanoparticle scaffold. The supra-QDs were characterized and used to label cell-sized objects that were measured under flow with a smartphone-based device. Each color followed an approximately linear trajectory in the RGB space, and training of support vector machine models enabled color classification with overall accuracies ≥87% for 10-color multiplexing and better accuracies for fewer colors. Most misclassification occurred at low signal levels, such that establishing a nonclassifiable zone near the origin of RGB color space improved the overall 10-color classification accuracy to ≥94%. Similar improvements in accuracy with greater retention of data were possible with a probabilistic rather than a radial threshold. Simulations that were parameterized by experimental data suggested that ≥14-color multiplexing with accuracies ≥90% should be possible with an optimized supra-QD color set. This study is an important foundation for advancing RGB color-based multiplexing for imaging and analyses with smartphone cameras and related charge-coupled device and CMOS color image sensor technologies.
MeSH term(s)	Quantum Dots ; Smartphone ; Nanoparticles ; Fluorescence Resonance Energy Transfer
Language	English
Publishing date	2023-11-20
Publishing country	United States
Document type	Journal Article
ISSN	2379-3694
ISSN (online)	2379-3694
DOI	10.1021/acssensors.3c01741
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Quantitative and Multiplexed Chopper-Based Time-Gated Imaging for Bioanalysis on a Smartphone

Kanani, Sahil S. / Tsai, Hsin-Yun / Algar, W. Russ

Analytical Chemistry. 2023 Aug. 23, v. 95, no. 35 p.13258-13265

2023

Abstract	Smartphones are emerging platforms for point-of-care diagnostics (POCDs), where the on-board camera is, for example, used to image fluorescence. Many laboratory instruments are capable of time-gated (TG) photoluminescence (PL) measurements—an analytical method leveraged by multiple commercial assay kits. When paired with long-lived PL emitters such as luminescent lanthanide complexes (LLCs), time-gating eliminates background from sample autofluorescence and many other sources. This capability is amenable to minimally processed samples and would thus be useful for POCDs on a smartphone-based platform. Here, we report a double-chopper design for TG PL imaging using a portable, 3D-printed, smartphone-based device. The rotation speed, dimensions, and overlap of the chopper blades and gaps set the timing parameters, with delay times on the order of hundreds of microseconds to milliseconds. The device was capable of quantitative TG imaging of PL from terbium(III) and europium(III) LLCs, including rejection of short-lived PL background from serum and tissue phantoms, spectral and temporal multiplexing, a model time-gated Förster resonance energy transfer (TG-FRET) assay, and imaging of cells. As the first smartphone-based demonstrations of these important analytical capabilities, this work is an important foundation for developing POCD methods based on TG PL imaging.
Keywords	analytical chemistry ; analytical methods ; blood serum ; cameras ; diagnostic techniques ; energy transfer ; fluorescence ; lanthanides ; mobile telephones ; photoluminescence ; point-of-care systems
Language	English
Dates of publication	2023-0823
Size	p. 13258-13265.
Publishing place	American Chemical Society
Document type	Article ; Online
ZDB-ID	1508-8
ISSN	1520-6882 ; 0003-2700
ISSN (online)	1520-6882
ISSN	0003-2700
DOI	10.1021/acs.analchem.3c02397
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Analytical nanoscience.

Algar, W Russ / Albrecht, Tim / Faulds, Karen / Zhu, Jun-Jie

The Analyst

2022 Volume 147, Issue 5, Page(s) 765–766

Language	English
Publishing date	2022-02-28
Publishing country	England
Document type	Editorial
ZDB-ID	210747-8
ISSN	1364-5528 ; 0003-2654
ISSN (online)	1364-5528
ISSN	0003-2654
DOI	10.1039/d1an90110a
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