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Principles Of Fluorescence Spectroscopy

We show nanoscale phase stabilization of CsPbI 3 quantum dots (QDs) to low temperatures that can be used as the active component of efficient optoelectronic devices. CsPbI 3 is an all-inorganic analog to the hybrid organic cation halide perovskites, but the cubic phase of bulk CsPbI 3 (α-CsPbI 3 )—the variant with desirable band gap—is only stable at high temperatures. We describe the formation of α-CsPbI 3 QD films that are phase-stable for months in ambient air. The films exhibit long-range electronic transport and were used to fabricate colloidal perovskite QD photovoltaic cells with an open-circuit voltage of 1.23 volts and efficiency of 10.77%. These devices also function as light-emitting diodes with low turn-on voltage and tunable emission.

http://science.sciencemag.org/content/sci/354/6308/92.full.pdf

Quantum dot-induced phase stabilization of α-CsPbI3 perovskite for high-efficiency photovoltaics.

Recently, Kovalenko and co-workers and Li and co-workers developed CsPbX3 (X = Cl, Br, I) inorganic perovskite quantum dots (IPQDs), which exhibited ultrahigh photoluminescence (PL) quantum yields (QYs), low-threshold lasing, and multicolor electroluminescence. However, the usual synthesis needs high temperature, inert gas protection, and localized injection operation, which are severely against applications. Moreover, the so unexpectedly high QYs are very confusing. Here, for the first time, the IPQDs' room-temperature (RT) synthesis, superior PL, underlying origins and potentials in lighting and displays are reported. The synthesis is designed according to supersaturated recrystallization (SR), which is operated at RT, within few seconds, free from inert gas and injection operation. Although formed at RT, IPQDs' PLs have QYs of 80%, 95%, 70%, and FWHMs of 35, 20, and 18 nm for red, green, and blue emissions. As to the origins, the observed 40 meV exciton binding energy, halogen self-passivation effect, and CsPbX3@X quantum-well band alignment are proposed to guarantee the excitons generation and high-rate radiative recombination at RT. Moreover, such superior optical merits endow them with promising potentials in lighting and displays, which are primarily demonstrated by the white light-emitting diodes with tunable color temperature and wide color gamut.

CsPbX3 Quantum Dots for Lighting and Displays: Room-Temperature Synthesis, Photoluminescence Superiorities, Underlying Origins and White Light-Emitting Diodes

Lead halide perovskites (LHPs) in the form of nanometre-sized colloidal crystals, or nanocrystals (NCs), have attracted the attention of diverse materials scientists due to their unique optical versatility, high photoluminescence quantum yields and facile synthesis. LHP NCs have a 'soft' and predominantly ionic lattice, and their optical and electronic properties are highly tolerant to structural defects and surface states. Therefore, they cannot be approached with the same experimental mindset and theoretical framework as conventional semiconductor NCs. In this Review, we discuss LHP NCs historical and current research pursuits, challenges in applications, and the related present and future mitigation strategies explored.

/pdf/genesis-challenges-and-opportunities-for-colloidal-lead-3uh77e26ys.pdf

Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals

Lead halide perovskite materials have attracted significant attention in the context of photovoltaics and other optoelectronic applications, and recently, research efforts have been directed to nanostructured lead halide perovskites. Collodial nanocrystals (NCs) of cesium lead halides (CsPbX3, X = Cl, Br, I) exhibit bright photoluminescence, with emission tunable over the entire visible spectral region. However, previous studies on CsPbX3 NCs did not address key aspects of their chemistry and photophysics such as surface chemistry and quantitative light absorption. Here, we elaborate on the synthesis of CsPbBr3 NCs and their surface chemistry. In addition, the intrinsic absorption coefficient was determined experimentally by combining elemental analysis with accurate optical absorption measurements. 1H solution nuclear magnetic resonance spectroscopy was used to characterize sample purity, elucidate the surface chemistry, and evaluate the influence of purification methods on the surface composition. We fi...

/pdf/highly-dynamic-ligand-binding-and-light-absorption-1hkm97tv0e.pdf

Highly Dynamic Ligand Binding and Light Absorption Coefficient of Cesium Lead Bromide Perovskite Nanocrystals

Focused ion beam (FIB) has recently been used to tune the optical properties of lead halide perovskites (LHPs), opening an interesting avenue for applications in optoelectronic devices. However, it has remained an open question to date whether FIB can be used to locally enhance the photoluminescence (PL) of LHPs. In this work we irradiate MAPbBr3 (MA = methylammonium) single crystals with a high energy micron-sized ion probe of different ionic masses (3 MeV He+, 12.5 MeV Br5+, and 20 MeV I7+) and study the PL as a function of the damage induced by the ion beam. We find that at low damage levels the PL is enhanced about six times with respect to the pristine material, while increasing the damage level produces a progressive PL decrease, and, above a threshold, the PL is finally quenched below the value of the pristine crystal. We attribute this behavior to the interaction of free carriers with irradiation induced surface defects: at low damage levels the migration of carriers toward the bulk is inhibited via trapping–detrapping events at surface defects, allowing their radiative recombination near the surface; at higher damage, though, the probability for non-radiative recombination increases and gradually becomes dominant. We thus present a method to locally increase the PL of bulk LHP, which could be applied in a wide range of fields, such as highly sensitive ion beam detection or future optoelectronic device design.

Photoluminescence enhancement and high accuracy patterning of lead halide perovskite single crystals by MeV ion beam irradiation

In this study the potential of branched polyethyleneimine (PEI) was explored for the in situ generation of ZnO nanoparticles and the electrospinning of zein-based fibers. Zinc acetyl acetonate dihydrate (ZnAcAc·2H2O) was chosen as the precursor for the related sol–gel reactions, leading to the nucleation and growth of wurtzite crystals within the PEI matrix. Control experiments showed that PEI played a vital role in the reaction steps leading to the conversion. Wide angle X-ray diffraction analysis confirmed the crystallographic structure of the ZnO particles formed, while scanning electron microscopy examinations revealed the formation of agglomerates less than 400 nm, made up of much smaller primary nanoparticles. The obtained ZnO/PEI microsuspensions in ethanol were mixed in an ethanol/water solution of zein and used for electrospinning of different types of zein-modified fibers. Differential scanning calorimetry analysis showed that PEI acted as a plasticizer for zein, causing also a broadening of the...

/pdf/in-situ-generation-of-zno-nanoparticles-within-a-22k1s7panu.pdf

In Situ Generation of ZnO Nanoparticles within a Polyethyleneimine Matrix for Antibacterial Zein Fibers

The localization of light known as Anderson localization is a common phenomenon characterizing aggregates of metallic nanostructures. The electromagnetic energy of visible light can be localized inside nanostructures below the diffraction limit by converting the optical modes into nonradiative surface plasmon resonances. The energy of the confined photons is correlated to the size and shape of the nanostructured system. In this work, we studied the photoluminescence dependence of aggregates of 14 nm diameter gold nanoparticles (AuNPs) synthesized by drop-casting a liquid suspension on two different substrates of glass and quartz. The AuNP aggregates were characterized by electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. The dielectric constant of the surrounding medium plays a crucial role in determining the aggregate geometry, which affects the Anderson localization of light in the aggregates and hence causes a red-shift in the plasmonic resonance and in the photoluminescence emission. The geometry of the gold nanoparticle aggregates determine the strength of the Anderson localization, and hence, the light emission from the aggregates. The photoluminescence lifetime was found to be dependent on the AuNP aggregate geometry and the dielectric constant of the medium.

/pdf/effect-of-anderson-localization-on-light-emission-from-gold-1ac2iv080w.pdf

Effect of Anderson localization on light emission from gold nanoparticle aggregates.

Antibacterial activity of nanocrystalline TiO2(B) on multiresistant klebsiella pneumoniae strains

We present the in situ localized formation of silver nanoparticles in chitosan films by pulsed UV laser irradiation, as a result of the photoreduction of the silver nitrate precursor loaded throughout the volume of the polymer. The UV pulsed irradiation is also found to be responsible for the photofragmentation of the previously formed nanoparticles, leading to their average size reduction as the number of pulses increases. In fact, their diameter changes from ~150 to ~30 nm for irradiation with 5 to 200 pulses, respectively. After irradiation the formation of nanoparticles continues for several days, since the already formed nanoparticles act as seeds for the reduction of the unreacted precursor. Indeed, few weeks after irradiation, the chitosan films present a metallic mirror-like appearance on the previously irradiated areas, as they are fully covered by silver. Taking advantage of all these simultaneous mechanisms, and controlling the number of pulses and elapsed time after irradiation, Ag nanoparticles of specific size can be formed in situ on desired areas of the film. Through this process is envisioned the fabrication of nanocomposites with functional properties.

https://iopscience.iop.org/article/10.1088/2053-1591/2/10/105014/pdf

Alice Scarpellini

Papers

Photoluminescence enhancement and high accuracy patterning of lead halide perovskite single crystals by MeV ion beam irradiation

In Situ Generation of ZnO Nanoparticles within a Polyethyleneimine Matrix for Antibacterial Zein Fibers

Effect of Anderson localization on light emission from gold nanoparticle aggregates.

Antibacterial activity of nanocrystalline TiO2(B) on multiresistant klebsiella pneumoniae strains

Laser-induced localized formation of silver nanoparticles on chitosan films: study on particles size and density variation