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Guyot-Sionnest, Philippe

Publications and source records attributed to Guyot-Sionnest, Philippe.

Bright Fluorophores in the Second Near-Infrared Window: HgSe/CdSe Quantum Dots

Fluorophores emitting in the NIR-IIb wavelength range (1.5-1.7 μm) show great potential for bioimaging due to their large tissue penetration. However, current fluorophores suffer from poor emission with quantum yields similar to 2% in aqueous solvents. In this work, we report the synthesis of HgSe/CdSe core/shell quantum dots (QDs) emitting at 1.7 μm through the interband transition. Growth of a thick shell led to a drastic increase in the photoluminescence quantum yield, with a value of 63% in nonpolar solvents. The quantum yields of our QDs and other reported QDs are explained well by a model of Forster resonance energy transfer to ligands and solvent molecules. The model predicts a quantum yield >12% when these HgSe/CdSe QDs are solubilized in water. In conclusion, our work demonstrates the importance of a thick type-I shell to obtain bright emission in the NIR-IIb region.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Polarized near-infrared intersubband absorptions in CdSe colloidal quantum wells

Colloidal quantum wells are two-dimensional materials grown with atomically-precise thickness that dictates their electronic structure. Although intersubband absorption in epitaxial quantum wells is well-known, analogous observations in non-epitaxial two-dimensional materials are sparse. Here in this paper, we show that CdSe nanoplatelet quantum wells have narrow (30–200 meV), polarized intersubband absorption features when photoexcited or under applied bias, which can be tuned by thickness across the near-infrared (NIR) spectral window (900–1600 nm) inclusive of important telecommunications wavelengths. By examination of the optical absorption and polarization-resolved measurements, the NIR absorptions are assigned to electron intersubband transitions. Under photoexcitation, the intersubband features display hot carrier and Auger recombination effects similar to excitonic absorptions. Sequenced two-color photoexcitation permits the sub-picosecond modulation of the carrier temperature in such colloidal quantum wells. This work suggests that colloidal quantum wells may be promising building blocks for NIR technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mid-infrared photodetectors

Nanoparticles, methods of manufacture, devices comprising the nanoparticles, methods of their manufacture, and methods of their use are provided herein. The nanoparticles and devices having photoabsorptions in the range of 1.7 μm to 12 μm and can be used as photoconductors, photodiodes, phototransistors, charge-coupled devices (CCD), luminescent probes, lasers, thermal imagers, night-vision systems, and/or photodetectors.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Conduction Band Fine Structure in Colloidal HgTe Quantum Dots

HgTe colloidal quantum dots (QDs) are of interest because quantum confinement of semimetallic bulk HgTe allows one to synthetically control the bandgap throughout the infrared. Here, we synthesize highly monodisperse HgTe QDs and tune their doping both chemically and electrochemically. The monodispersity of the QDs was evaluated using small-angle X-ray scattering (SAXS) and suggests a diameter distribution of similar to 10% across multiple batches of different sizes. Electron-doped HgTe QDs display an intraband absorbance and bleaching of the first two excitonic features. We see splitting of the intraband peaks corresponding to electronic transitions from the occupied 1S e state to a series of nondegenerate 1P e states. Spectroelectrochemical studies reveal that the degree of splitting and relative intensity of the intraband features remain constant across doping levels up to two electrons per QD. Theoretical modeling suggests that the splitting of the 1P e level arises from spin-orbit coupling and reduced QD symmetry. As a result, the fine structure of the intraband transitions is observed in the ensemble studies due to the size uniformity of the as-synthesized QDs and strong spin-orbit coupling inherent to HgTe.

36 MATERIALS SCIENCE↗

Final report

Conductivity and Magnetism in Strongly Coupled Quantum Dot Solids. One outcome of the project is the discovery of a rather universal 1/f noise magnitude in electrical transport across nanocrystals. The noise is extensive in the number of dots in the device, and inversely proportional to the interdot resistance. The other outcome is a study of the magneto-resistance of light and heavy doped chalcogenides semiconductor quantum dots with Manganese. Strong MR was observed at low temperature in n-doped Mn doped quantum dot films, and this was attributed to the formation of magnetic polarons.

1/f noise↗

Mid-infrared photodetectors

Nanoparticles, methods of manufacture, devices comprising the nanoparticles, methods of their manufacture, and methods of their use are provided herein. The nanoparticles and devices having photoabsorptions in the range of 1.7 .mu.m to 12 .mu.m and can be used as photoconductors, photodiodes, phototransistors, charge-coupled devices (CCD), luminescent probes, lasers, thermal imagers, night-vision systems, and/or photodetectors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Background limited mid-infrared photodetection with photovoltaic HgTe colloidal quantum dots

The photovoltaic response of thin films of HgTe colloidal quantum dots in the 3–5 μm range is observed. With no applied bias, internal quantum efficiency exceeding 40%, specific detectivity above 10{sup 10} Jones and microseconds response times are obtained at 140 K. The cooled devices detect the ambient thermal radiation. A detector with 5.25 μm cut-off achieves Background Limited Infrared Photodetection at 90 K.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

1/f noise in semiconductor and metal nanocrystal solids

Electrical 1/f noise is measured in thin films of CdSe, CdSe/CdS, ZnO, HgTe quantum dots and Au nanocrystals. The 1/f noise, normalized per nanoparticle, shows no systematic dependence on the nanoparticle material and the coupling material. However, over 10 orders of magnitude, it correlates well with the nearest neighbor conductance suggesting some universal magnitude of the 1/f noise in these granular conductors. In the hopping regime, the main mechanism of 1/f noise is determined to be mobility fluctuated. In the metallic regime obtained with gold nanoparticle films, the noise drops to a similar level as bulk gold films and with a similar temperature dependence.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗