Yinthai Chan

Blue semiconductor nanocrystal laser

We demonstrate tunable room-temperature amplified spontaneous emission and lasing from blue-emitting core-shell CdS∕ZnS nanocrystals (NCs) stabilized in a sol-gel derived silica matrix. Variable stripe length measurements show that these NC-silica composites have a modal gain of ∼100cm−1 at room temperature. Coating microspheres with a NC-silica composite film via a facile process resulted in uniform resonators that exhibit room-temperature lasing over long periods of continuous excitation. This work opens up a spectral window for emission tunable, microscale NC-based lasers.

Ultralow-threshold two-photon pumped amplified spontaneous emission and lasing from seeded CdSe/CdS nanorod heterostructures

Ultralow-threshold two-photon pumped amplified spontaneous emission (2ASE) and lasing in seeded CdSe/CdS nanodot/nanorod heterostructures is demonstrated for the first time. Such heterostructures allow the independent tunability of the two-photon absorption (2PA) cross-section (σ(2)) through varying the CdS rod size, and that of the emission wavelength through varying the CdSe dot size. With an enhanced σ(2), 2ASE in these heterostructures is achieved with an ultralow threshold fluence of ~1.5 mJ/cm(2), which is as much as one order less than that required for spherical semiconductor NCs. Importantly, by exploiting this unique property of the seeded nanorods exhibiting strong quantum confinement even at relatively large rod sizes, a near reciprocal relation between the 2ASE threshold and the 2PA action cross-section (σ(2)η) (where η is the quantum yield) was found and validated over a wide volume range for II-VI semiconductor nanostructures. Ultrafast optical spectroscopy verified that while the Auger processes in these heterostructures are indeed suppressed, ASE in these samples could also be strongly affected by a fast hole-trapping process to the NR surface states. Lastly, to exemplify the potential of these seeded CdSe/CdS nanodot/nanorod heterostructures as a viable gain media for achieving two-photon lasing, a highly photostable microsphere laser with an ultralow pump threshold is showcased.

pH-Responsive quantum dots via an albumin polymer surface coating.

Multifunctional peptide-polymer hybrid materials have been applied as efficient and biocompatible quantum-dot coating materials. Significant pH responsiveness (e.g., an influence of the pH on the quantum yields of the peptide-polymer/QDs) was found and is attributed to conformational rearrangements of the peptide backbone.

Light-Induced Selective Deposition of Metals on Gold-Tipped CdSe-Seeded CdS Nanorods

We introduce a facile approach for the selective deposition of metals on Au-tipped CdSe-seeded CdS nanorods that exploits the transfer of electrons from CdS to the Au tips upon UV excitation. This light-induced deposition method was used for the deposition of Pd under mild conditions, which produced a Pd/Au alloyed tip while preserving the rest of the semiconductor nanoarchitecture. The highly site-selective deposition method was extended to the deposition of Fe, yielding monodispersed, structurally complex Au core/Fe(x)O(y) hollow shell-tipped semiconductor nanorods. These structurally well-defined rods were found to exhibit magnetic functionality. The synthetic strategies described in this work expand on the range of metals that can be deposited on heterostructured semiconductor nanorods, opening up new avenues for the hierarchical buildup of structural complexity and therefore multifunctionality in nanoparticles.

Multiexcitonic two-state lasing in a CdSe nanocrystal laser

We report simultaneous amplified spontaneous emission from two different multiexcitonic transitions −1Se–1S3∕2 and 1Pe–1P3∕2− of colloidal CdSe nanocrystals (NCs) stabilized in high volume fraction in titania matrices. Two-state lasing from both multiexcitonic transitions is achieved in a surface-emitting distributed feedback CdSe NC laser. Variable stripe length measurements show that the gain from the 1Pe–1P3∕2 transition is approximately twice that of the −1Se–1S3∕2 transition for 4.2nm radius CdSe∕ZnS core-shell NCs.

Dual Wavelength Electroluminescence from CdSe/CdS Tetrapods

We fabricated a single active layer quantum dot light-emitting diode device based on colloidal CdSe (core)/CdS (arm) tetrapod nanostructures capable of simultaneously producing room temperature electroluminesence (EL) peaks at two spectrally distinct wavelengths, namely, at ∼500 and ∼660 nm. This remarkable dual EL was found to originate from the CdS arms and CdSe core of the tetrapod architecture, which implies that the radiative recombination of injected charge carriers can independently take place at spatially distinct regions of the tetrapod. In contrast, control experiments employing CdSe-core-seeded CdS nanorods showed near-exclusive EL from the CdSe core. Time-resolved spectroscopy measurements on tetrapods revealed the presence of hole traps, which facilitated the localization and subsequent radiative recombination of excitons in the CdS arm regions, whereas excitonic recombination in nanorods took place predominantly within the vicinity of the CdSe core. These observations collectively highlight the role of morphology in the achievement of light emission from the different material components in heterostructured semiconductor nanoparticles, thus showing a way in developing a class of materials which are capable of exhibiting multiwavelength electroluminescence.

Ultralow-threshold multiphoton-pumped lasing from colloidal nanoplatelets in solution

Although multiphoton-pumped lasing from a solution of chromophores is important in the emerging fields of nonlinear optofluidics and bio-photonics, conventionally used organic dyes are often rendered unsuitable because of relatively small multiphoton absorption cross-sections and low photostability. Here, we demonstrate highly photostable, ultralow-threshold multiphoton-pumped biexcitonic lasing from a solution of colloidal CdSe/CdS nanoplatelets within a cuvette-based Fabry–Pérot optical resonator. We find that colloidal nanoplatelets surprisingly exhibit an optimal lateral size that minimizes lasing threshold. These nanoplatelets possess very large gain cross-sections of 7.3 × 10−14 cm2 and ultralow lasing thresholds of 1.2 and 4.3 mJ cm−2 under two-photon (λexc=800 nm) and three-photon (λexc=1.3 μm) excitation, respectively. The highly polarized emission from the nanoplatelet laser shows no significant photodegradation over 107 laser shots. These findings constitute a more comprehensive understanding of the utility of colloidal semiconductor nanoparticles as the gain medium in high-performance frequency-upconversion liquid lasers.

Aqueous-Phase Reactions on Hollow Silica-Encapsulated Semiconductor Nanoheterostructures

We introduce a facile and robust methodology for the aggregation-free aqueous-phase synthesis of hierarchically complex metal-semiconductor heterostructures. By encapsulating semiconductor nanostructures within a porous SiO(2) shell with a hollow interior, we can isolate each individual particle while allowing it access to metal precursors for subsequent metal growth. We illustrate this by Pt deposition on CdSe-seeded CdS tetrapods, which we found to be facilitated via the surprising formation of a thin interfacial layer of PtS coated onto the original CdS surface. We took advantage of this unique architecture to perform cation exchange reactions with Ag(+) and Pd(2+), thus demonstrating the feasibility of achieving such transformations in complex metal-semiconductor nanoparticle systems.

Enhanced tunability of the multiphoton absorption cross-section in seeded CdSe/CdS nanorod heterostructures

We present a method to separately tune the multiphoton absorption (MPA) and multiphoton excited photoluminescence using semiconductor core/enlarged-shell quantum dots (QDs), where the enlarged shell greatly enhances the MPA cross-sections while varying the core size facilitates emission wavelength selectivity. Following two-photon absorption (2PA) primarily in the shell and ultrafast charge-carrier localization to the core, luminescence occurs. We exemplify the validity of this method with CdSe/CdS nanorod heterostructures and find that the 2PA cross-section is enlarged to ∼1.4×106 GM for 180 nm nanorods (with 800 nm, 150 fs laser pulse excitation) which is two to four orders larger than that of CdSe QDs.

Low Threshold, Amplified Spontaneous Emission from Core‐Seeded Semiconductor Nanotetrapods Incorporated into a Sol–Gel Matrix

Wet-chemically synthesized colloidal semiconductor nanocrystals (NCs) are desirable as optical gain media due to their sizedependent emission wavelengths, ease of fabrication and fl exible surface chemistry which facilitates incorporation into an optical feedback device of various confi gurations. [ 1–3 ] Early attempts to achieve stimulated emission via close-packed fi lms of NCs required low temperature and high pump fl uences since such fi lms generally suffer from low optical quality, poor heat dissipation, and consequently short operational device lifetimes. [ 4 , 5 ]