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1.
J Phys Chem Lett ; 15(19): 5177-5182, 2024 May 16.
Article in English | MEDLINE | ID: mdl-38717311

ABSTRACT

Exciton dynamics of perovskite nanoclusters has been investigated for the first time using femtosecond transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopy. The TA results show two photoinduced absorption signals at 420 and 461 nm and a photoinduced bleach (PB) signal at 448 nm. The analysis of the PB recovery kinetic decay and kinetic model uncovered multiple processes contributing to electron-hole recombination. The fast component (∼8 ps) is attributed to vibrational relaxation within the initial excited state, and the medium component (∼60 ps) is attributed to shallow carrier trapping. The slow component is attributed to deep carrier trapping from the initial conduction band edge (∼666 ps) and the shallow trap state (∼40 ps). The TRPL reveals longer time dynamics, with modeled lifetimes of 6.6 and 93 ns attributed to recombination through the deep trap state and direct band edge recombination, respectively. The significant role of exciton trapping processes in the dynamics indicates that these highly confined nanoclusters have defect-rich surfaces.

2.
J Phys Chem Lett ; 13(45): 10543-10549, 2022 Nov 17.
Article in English | MEDLINE | ID: mdl-36342415

ABSTRACT

Nanosized molecular clusters (MCs) composed of PbBr2 and neutral ligand butylamine (BTYA) with unique optical properties in solution and solid states have been synthesized using ligand-assisted reprecipitation and spin-coating, separately. The studies of their optical properties using ultraviolet-visible (UV-vis) absorption and photoluminescence (PL) show the first electronic absorption and PL band of the MCs at 401 and 411 nm, respectively, for the solution and solid state samples that exhibit good stability under ambient conditions. Low-temperature PL spectra below 30 K show vibronic peaks indicative of a single size or a very narrow size distribution of the MCs. On the basis of Raman, X-ray diffraction, and transmission electron microscopy measurements, a layered structural model is proposed for the MCs with a BTYA ligand capping on the surface of the corner-shared tilted [PbBr6]4- octahedral framework. The stable and retained structure of MCs in the solid state is promising for photonics applications.


Subject(s)
Ligands , X-Ray Diffraction , Microscopy, Electron, Transmission
3.
J Phys Chem B ; 125(44): 12344-12352, 2021 11 11.
Article in English | MEDLINE | ID: mdl-34726922

ABSTRACT

Hollow gold nanospheres (HGNs) have been used as the template for seed-mediated growth of multibranched hollow gold nanostars (HNS). The HGNs were synthesized via anerobic reduction of cobalt chloride to cobalt nanoparticles and then formation of a gold shell via galvanic replacement followed by the oxidation of the cobalt core. We obtained control of the inner core size of the HGNs by increasing the size of the sacrificial cobalt core and by varying the ratio of B(OH)3/BH4 using boric acid rather than 48 h aged borohydride. We synthesized the HNS by reducing Au3+ ions in the presence of Ag+ ions using ascorbic acid, creating a spiky morphology that varied with the Au3+/Ag+ ratio. A broadly tunable localized surface plasmon resonance was achieved through control of both the inner core and the spike length. Amyloid beta (Aß) was conjugated to the HNS by using a heterobifunctional PEG linker and identified by the vibrational modes associated with the conjugated ring phenylalanine side chain. A bicinchoninic acid assay was used to determine the concentration of Aß conjugated to HNS as 20 nM, which is below the level of Aß that negatively affects long-term potentiation. Both the core size and spike length were shown to affect the optical properties of the resulting nanostructures. This HGN templated method introduced a new parameter for enhancing the plasmonic properties of gold nanostars, namely, the addition of a hollow core. Hollow gold nanostars are highly desirable for a wide range of applications, including high sensitivity disease detection and monitoring.


Subject(s)
Gold , Nanospheres , Amyloid beta-Peptides , Polyethylene Glycols , Silver
4.
Article in English | MEDLINE | ID: mdl-33501780

ABSTRACT

Hollow gold nanospheres (HGNs) are core/shell structures with a dielectric material core, usually composed of solvent, and a gold metal shell. Such structures have two metal/dielectric interfaces to allow interaction between the gold metal with the interior and external dielectric environment. Upon illumination by light, HGNs exhibit unique surface plasmon resonance (SPR) properties compared to solid gold nanoparticles. Their SPR absorption/scattering can be tuned by changing their diameter, shell thicknesses, and surface morphologies. In addition to the low toxicity, easy functionalization, resistance to photobleaching, and sensitivity to changes in surrounding medium of gold, the enhanced surface-to-volume ratio and tunable SPR of HGNs make them highly attractive for different applications in the fields of sensing, therapy, and theranostics. In this article, we review recent progress on the synthesis and structural control of HGNs and applications of their SPR properties in biomedical sensing and theranostics. This article is categorized under: Diagnostic Tools > Biosensing Diagnostic Tools > in vitro Nanoparticle-Based Sensing Diagnostic Tools > in vivo Nanodiagnostics and Imaging.


Subject(s)
Gold , Metal Nanoparticles , Nanospheres , Diagnostic Imaging , Surface Plasmon Resonance
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