Millimeter-Deep Detection of Single Shortwave-Infrared-Emitting Polymer Dots through Turbid Media
Abstract
Fluorescence imaging at longer wavelengths, especially in the shortwave-infrared (SWIR: 1000–1700 nm) region, leads to a substantial decrease in light attenuation, scattering, and background autofluorescence, thereby enabling enhanced penetration into biological tissues. The limited selection of fluorescent probes is a major bottleneck in SWIR fluorescence imaging. Here, we develop SWIR-emitting nanoparticles composed of donor–acceptor-type conjugated polymers. The bright SWIR fluorescence of the polymer dots (primarily attributable to their large absorption cross-section and high fluorescence saturation intensity (as high as 113 kW·cm –2 )) enables the unprecedented detection of single particles as small as 14 nm through millimeter-thick turbid media. Unlike most SWIR-emitting nanomaterials, which have an excited-state lifetime in the range of microseconds to milliseconds, our polymer dots exhibit a subnanosecond excited-state lifetime. These characteristics enable us to demonstrate new time-gated single-particle imaging with a high signal-to-background ratio. These findings expand the range of potential applications of single-particle deep-tissue imaging.
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Photophysical characterization demonstrated that Φfl was independent of the particle size, whereas the fluorescence brightness under microscopy conditions increased gradually with the size of Pdots.
“Photophysical characterization demonstrated that Φfl was independent of the particle size, whereas the fluorescence brightness under microscopy conditions increased gradually with the size of Pdots.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
Single-particle SWIR fluorescence imaging with one-photon excitation has recently been demonstrated using SWIR emitting Pdots consisting of PSN conjugated polymer.
“Single-particle SWIR fluorescence imaging with one-photon excitation has recently been demonstrated using SWIR emitting Pdots consisting of PSN CP (Figure 14).215”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
Using a sub-nanosecond time-gated imaging mode with a high repetition rate pulsed laser, a significant improvement in signal-to-background ratio (29× improvement of SBR) has been observed for PSN Pdots.
“Using this mode of time-gated imaging, a significant improvement in signal-to-background-ratio (29× improvement of SBR) has been observed for the PSN Pdots (Figure 16).215”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
The improvement of SBR was achieved without substantially affecting the detection efficiency of the emitted fluorescence photon.
“The improvement of SBR was achieved without substantially affecting the detection efficiency of the emitted fluorescence photon, which is the major disadvantage in afterglow fluorescence imaging, where the improved SBR is achieved at the expense of fluorescence brightness.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
The very bright SWIR fluorescence of the PSN Pdots enabled single-particle imaging through tissue phantoms that mimic optical properties of biological tissues.
“The very bright SWIR fluorescence of the PSN Pdots enabled single-particle imaging through tissue phantoms that mimic optical properties of biological tissues.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
The increase in fluorescence brightness with Pdot size was primarily attributed to their large absorption cross section and high fluorescence saturation intensity.
“This was primarily attributed to their large absorption cross section and high fluorescence saturation intensity.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
SWIR emitting Pdots (PSN and BBT) with short excited-state lifetimes (in the order of sub-nanosecond) showed higher saturation intensities.
“On the other hand, SWIR emitting Pdots (PSN and BBT) with short excited-state lifetimes (in the order of sub-nanosecond) showed higher saturation intensities (Figure 15).215”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
Detection of the Pdots through a millimeter-thick phantom was demonstrated using Pdots as small as 14 nm.
“A detection of the Pdots through a millimeter-thick phantom was demonstrated using Pdots as small as 14 nm.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
SWIR emitting inorganic nanoparticles (PbS QDs) exhibit relatively low saturation intensities due to the long excited-state lifetime (in the order of microseconds).
“On the one hand, SWIR emitting inorganic nanoparticles (PbS QDs) exhibit relatively low saturation intensities due to the long excited-state lifetime (in the order of microseconds).”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
PSN Pdots with diameters of 3.5, 14.3, and 31.9 nm were obtained by controlling the size of nanoparticles formulated in the nanoprecipitation process with an adjusted ratio of the organic to water phases.
“PSN Pdots with diameters of 3.5, 14.3, and 31.9 nm were obtained by this protocol.”
From The Pursuit of Shortwave Infrared-Emitting Nanoparticles with Bright Fluorescence through Molecular Design and Excited-State Engineering of Molecular Aggregates (2022) · cites this paper as [215]
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- Authors
- Piwoński, H., Wang, Y., Li, W., Michinobu, T., & Habuchi, S.
- Affiliations
- King Abdullah University of Science and Technology (SA)
- Tokyo Institute of Technology (JP)
- Corresponding author
- Piwoński, Hubert
- Habuchi, Satoshi
- Venue
- Nano Letters
- Publisher
- American Chemical Society (ACS)
- Published
- 2020-11-18
- Volume
- 20
- Issue
- 12
- Pages
- 8803-8810
- ISSN
- 1530-6984 (ISSN-L)
- 1530-6992
- OpenAlex
- W3102344778
- Cited by
- 19
- References
- 40
- Citations by year
- 2026: 1 · 2025: 1 · 2024: 3 · 2023: 5 · 2022: 5 · 2021: 4
- FWCI
- 1.36
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Locations
- Nano Letters (publishedVersion)
- PubMed (publishedVersion)
- Institutional Repositories DataBase (IRDB) (submittedVersion)
- King Abdullah University of Science and Technology Repository (King Abdullah University of Science and Technology) (submittedVersion)
- Tokyo Tech Research Repository (Tokyo Institute of Technology) (submittedVersion)
- Funders
- King Abdullah University of Science and Technology (OSR-2016-2967-CRG5)
- Topics
- Physical Sciences › Materials Science › Materials Chemistry › Luminescence and Fluorescent Materials
- Physical Sciences › Materials Science › Materials Chemistry › Quantum Dots Synthesis And Properties
- Physical Sciences › Materials Science › Materials Chemistry › Luminescence Properties of Advanced Materials
- Keywords
- polymer dots, donor-acceptor polymers, single-particle detection, turbid media, deep tissue imaging, time-gated imaging, fluorescence saturation, autofluorescence suppression, light scattering
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