Photon upconversion employing semiconductor nanocrystals (NCs) makes use of their large and tunable absorption to harvest light in the near-infrared (NIR) wavelengths as well as their small gap between singlet and triplet excited states to reduce energy losses. Here, we report the highest QY (11.8%) thus far for the conversion of NIR to yellow photons by improving the quality of the PbS NC. This high QY was achieved by using highly purified lead and thiourea precursors. This QY is 2.6 times higher than from NCs prepared with commercially available lead and sulfide precursors. Transient absorption spectroscopy reveals two reasons for the enhanced QY: longer intrinsic exciton lifetimes of PbS NCs and the ability to support a longer triplet lifetime for the surface-bound transmitter molecule. Overall, this results in a higher efficiency of triplet exciton transfer from the PbS NC light absorber to the emitter and thus a higher photon upconversion QY.
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http://dx.doi.org/10.1021/jacs.9b03385 | DOI Listing |
Nanophotonics
January 2025
Institute of Physics, Swiss Federal Institute of Technology Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
Sum-frequency generation (SFG) enables the coherent upconversion of electromagnetic signals and plays a significant role in mid-infrared vibrational spectroscopy for molecular analysis. Recent research indicates that plasmonic nanocavities, which confine light to extremely small volumes, can facilitate the detection of vibrational SFG signals from individual molecules by leveraging surface-enhanced Raman scattering combined with mid-infrared laser excitation. In this article, we compute the degree of second order coherence ( (0)) of the upconverted mid-infrared field under realistic parameters and accounting for the anharmonic potential that characterizes vibrational modes of individual molecules.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
School of Materials Science& Engineering, Zhejiang Sci-Tech University, Hangzhou 310018, China.
Lanthanide-doped upconversion luminescent nanoparticles (UCNPs) have garnered extensive attention due to their notable anti-Stokes shifts and superior photostability. Notably, Ho-based UCNPs present a complex energy level configuration, which poses challenges in augmenting their luminescence efficiency. Herein, a rational design strategy was used to enhance the upconversion luminescence intensity of Ho ions by improving the photon absorption ability and energy utilization efficiency.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
January 2025
Huzhou Key Laboratory of Materials for Energy Conversion and Storage, College of Science, Huzhou University, Huzhou 313000, China. Electronic address:
1550 nm-responsive upconversion luminescence (UCL) has attracted increasing attention due to its potential applicability in a new generation of bio-probes and photonic devices. However, regulating multi-color UCL with pump power remains a challenge. In this work, through constructing the coupling between Er and Tm ions and suppressing the energy transfer upconversion process of Er ions, the response of UCL color in Gd(MoO):Er/Tm to pump power is enhanced significantly.
View Article and Find Full Text PDFAdv Sci (Weinh)
January 2025
Key Laboratory for High Efficiency Energy Conversion Science and Technology of Henan Province, International Joint Research Laboratory of New Energy Materials and Devices of Henan Province, School of Physics and Electronics, Henan University, Kaifeng, 475004, P. R. China.
Multimode luminescent materials exhibit tunable photon emissions under different excitation or stimuli channels, endowing them high encoding capacity and confidentiality for anti-counterfeiting and encryption. Achieving multimode luminescence into a stable single material presents a promising but remains a challenge. Here, the downshifting/upconversion emissions, color-tuning persistent luminescence (PersL), temperature-dependent multi-color emissions, and hydrochromism are integrated into Er ions doped CsNaYbCl nanocrystals (NCs) by leveraging shallow defect levels and directed energy migration.
View Article and Find Full Text PDFAnal Chem
January 2025
Department of Life Technologies/Biotechnology, Faculty of Technology, University of Turku, Kiinamyllynkatu 10, 20520 Turku, Finland.
The anti-Stokes emission of photon upconversion nanoparticles (UCNPs) facilitates their use as labels for ultrasensitive detection in biological samples as infrared excitation does not induce autofluorescence at visible wavelengths. The detection of extremely low-abundance analytes, however, remains challenging as it is impossible to completely avoid nonspecific binding of label conjugates. To overcome this limitation, we developed a novel hybridization complex transfer technique using UCNP labels to detect short nucleic acids directly without target amplification.
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