Arunasish Layek

Ultranarrow and widely tunable Mn2+-Induced photoluminescence from single Mn-doped nanocrystals of ZnS-CdS alloys.

Extensively studied Mn-doped semiconductor nanocrystals have invariably exhibited photoluminescence over a narrow energy window of width ≤150  meV in the orange-red region and a surprisingly large spectral width (≥180  meV), contrary to its presumed atomic-like origin. Carrying out emission measurements on individual single nanocrystals and supported by ab initio calculations, we show that Mn PL emission, in fact, can (i) vary over a much wider range (∼370  meV) covering the deep green--deep red region and (ii) exhibit widths substantially lower (∼60-75  meV) than reported so far, opening newer application possibilities and requiring a fundamental shift in our perception of the emission from Mn-doped semiconductor nanocrystals.

Spectrally Resolved Photoluminescence Imaging of ZnO Nanocrystals at Single-Particle Levels

The intrinsic spectral line widths of defect-related transitions in quantum-confined semiconductor nanocrystals are often difficult to estimate using ensemble measurements because the extent of inhomogeneous broadening due to particle size distributions is not known precisely. To address this problem, we performed spectrally resolved photoluminescence (PL) microscopy of individual ZnO NC by directly populating the defects states using low-energy laser excitation. The temporal evolution of PL intensities shows discrete blinking behaviors, suggesting that the NCs are detected near single-particle levels. The transition energies of individual NCs are found to fluctuate around their mean position (2.25 eV) by ∼0.130 eV, which is attributed to particle size distribution and defects densities associated with each NC. The spectral line width associated with defect emission envelope of ZnO NCs is found to be inherently broad (200-400 meV), which further establishes the presence of multiple closely spaced defect energy levels within every ZnO NC.

Quantum-confined stark effect in localized luminescent centers within InGaN/GaN quantum-well based light emitting diodes

The nature of the polarization-field in disorder induced nanoscale potential fluctuations (radiative traps) within (In,Ga)N based quantum-well (QW) heterostructures remains ambiguous. Spectrally resolved photoluminescence microscopy has been utilized to probe the local polarization field by monitoring the extent of quantum-confined Stark effect (QCSE) in radiative trap centers spontaneously formed within an (In,Ga)N QW based light emitting diode. Interestingly, two distinct categories of nanoscale radiative domains, which arise from indium compositional and interface-morphology related fluctuations of the active layers, are found to have very different degree of built-in polarization fields. Screening of QCSE in indium-rich emission centers results in blue-shift of transition energies by up to 400 meV, significantly higher than that reported previously for group III-nitride based semiconductor heterostructures. A lack of correlation between the extent of QCSE and local indium mole-fractions suggests that ...

Optoelectronic behaviors and carrier dynamics of individual localized luminescent centers in InGaN quantum-well light emitting diodes

Spatially, spectrally, and temporally resolved photoluminescence (PL) microscopy was performed on InGaN quantum-well light emitting diodes to probe individual localized luminescent centers arising from disorder induced potential fluctuations. Two energetically distinct localization centers were identified where the photoemission quantum-efficiency (QE) are correlated to the transition energies. PL lifetime measurements on emission centers suggest that activation barrier for non-radiative recombination (NR) processes determines their QE. The disparity in carrier dynamics not only substantiate two diverse mechanisms for localization processes, but also indicate the presence of multiple NR channels even within the trap centers implying their lateral dimensions to span several nanometers.

Synthesis of rare-earth doped ZnO nanorods and their defect–dopant correlated enhanced visible-orange luminescence

We report the synthesis of size controlled ZnO and rare-earth doped ZnO nanorods in the sub-10 nm diameter regime. The preferential anisotropic growth of the nanostructures along the polar c-axis leads to the formation of wurtzite phase ZnO nanorods. Photoluminescence measurements reveal enhancement of visible luminescence intensity with increasing RE3+ concentrations upon excitation of host ZnO into the band gap. The broad visible luminescence originates from multiple intrinsic or extrinsic defects. The luminescence from RE3+ is enabled by energy transfer from defect centers of the host nanocrystal lattice to dopant sites. Host–guest energy transfer facilitates efficient intra-4f orbital transitions (5D4 → 7Fj for Tb3+ and 5D0 → 7Fj for Eu3+) related characteristic green or red emission. Interestingly, different decay rates of host defects and RE3+ emission transition also allow temporal control to achieve either pure green or red color. This study suggests that manipulation of defects through bottom-up techniques is a viable method to modulate the energy transfer dynamics, which may help enable the future applications of ZnO-based phosphor materials in optoelectronic and multicolor emission displays.

ZnO-NANOCRYSTALS IN STRONG CONFINEMENT REGIMES: INSIGHT ON RELAXATION DYNAMICS OF DEFECT STATES RESPONSIBLE FOR THE VISIBLE LUMINESCENCE

The broad visible photoluminescence (PL) observed in ZnO nanocrystals (NCs) is widely attributed to multiple low lying surface-defects. We have performed steady state and time-resolved PL measurements on size-selected ZnO NCs in the strong confinement regimes. Our results show that radiative relaxation rates and coupling between excitons and surface defect states vary dramatically for sizes between 2 nm and 3 nm. Energy dependent PL lifetimes reveal that relaxation dynamics of these defect states in the blue- and red-edge of the emission are very different from each other.