Picosecond carrier dynamics induced by coupling of wavefunctions in a Si-nanodisk array fabricated by neutral beam etching using bio-nano-templates

The picosecond carrier dynamics in a closely packed Si-nanodisk (Si-ND) array with ultrathin potential barrier fabricated by neutral beam etching using bio-nano-templates was investigated by time-resolved photoluminescence (PL). The PL decay curves were analyzed as a function of photon energy by the global fitting method. We show three spectral components with different decay times, where the systematic energy differences of the spectral peaks are clarified: 2.03 eV for the fastest decaying component with a decay time τ = 40 ps, 2.02 eV for τ = 300 ps, and 2.00 eV for τ = 1.6 ns. These energy separations ranging from 10 to 30 meV among the emissive states can be attributed to the coupling of wavefunctions of carriers between neighboring NDs

Layer-selective spin amplification in size-modulated quantum nanocolumn

The optical spin properties of size-modulated quantum nanocolumns (QNCs), which are composed of 9 layers of vertically coupled InGaAs quantum dots (QDs), have been studied by circularly polarized time-resolved photoluminescence spectroscopy of QD excited states with barrier excitation. High spin polarization at the emissive state is one of the essential elements in the development of spin-functional optical devices. Coupling of QD excited states can enhance the spin polarization if only minority spins are effectively removed from the emissive excited states. In this study, size-modulated QNCs with the increasing size toward the upper layer were grown, and we revealed that the combination of QD size modulation and electron wavefunction coupling in the stacking direction can greatly enhance spin polarization during light emission from the smaller-sized QD layers. We observed a temporal spin amplification of more than 80% at coupled excited states. This enhancement is derived from the size-modulation-induced selective transfer of minority spins to the larger-sized QD layers, which have abundant excited states where electron spins are transferred. In addition, we found that QNCs can retain high spin polarization even at high excitation spin density. Our findings of spin amplification during light emission will provide QNC systems suitable for spin-functional optical devices. Published under license by AIP Publishing

Spectral Narrowing of UV-Visible Absorption and Emission Spectra of Anthracene-Derivatives in β-Cyclodextrin Nanocavity: Effects of Host/Guest Stoichiometry

Cyclodextrins (CD) are cyclic oligosaccharides consisting of six or more D-glucopyranose units, the interior of which forms a hydrophobic cavity. In the present study, we employed the CD confinement effects as a tool to suppress an electronic decoherence of guest wavefunction by reducing intermolecular interactions between a guest molecule and the surrounding environment. Effects of host/guest stoichiometry on the decoherence suppresion were investigated by comparing native β-CD with trimethyl-β-CD that should form only a 1:1 complex. Both fluorecence and fluorecence-excitation spectra of inclusion complexes exhibited spectral narrowings only for the β-CD host, suggesting that the formation of barrel-type β-CD dimer plays a key role for the pronounced spectral narrowings

Solvent-assisted intramolecular vibrational energy redistribution of S1 perylene in ketone solvents

We investigated vibrational energy relaxations of S1 perylene at an excess energy of ca. 2800 cm-1 in several ketone solvents by femtosecond time-resolved fluorescence measurements. Temporal evolution of fluorescence emissions occurs on the following distinct timescales: 70 - 330 fs, 0.6 - 1.1 ps and 1.8 - 4.9 ps. The latter two was assigned to the intramolecular vibrational redistribution (IVR), and to the solvent-assisted IVR (SA-IVR), respectively. In SA-IVR, intramolecular vibrational couplings are affected by elastic or quasi-elastic interactions between solute and solvents. Solvent dependence of the SA-IVR rates can be explained qualitatively by the tier V-V coupling mechanism

Picosecond transient photoluminescence in high-density Si-nanodisk arrays fabricated using bio-nano-templates

We study picosecond transient photoluminescence (PL) in Si-nanodisk (Si-ND) arrays fabricated using bio-nano-templates. The PL time profiles show multi-exponential decaying kinetics depending on the disk density. We attribute the fastest decaying component with a decay time of 40 ps observed only in the high-density Si-ND array to the electron transfer among the Si-NDs

Impact of artificial lateral quantum confinement on exciton-spin relaxation in a two-dimensional GaAs electronic system

We demonstrate the effect of artificial lateral quantum confinement on exciton-spin relaxation in a GaAs electronic system. GaAs nanodisks (NDs) were fabricated from a quantum well (QW) by top-down nanotechnology using neutral-beam etching aided by protein-engineered bio-nano-templates. The exciton-spin relaxation time was 1.4 ns due to ND formation, significantly extended compared to 0.44 ns for the original QW, which is attributed to weakening of the hole-state mixing in addition to freezing of the carrier momentum. The temperature dependence of the spin-relaxation time depends on the ND thickness, reflecting the degree of quantum confinement. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License

Ultrafast spin tunneling and injection in coupled nanostructures of InGaAs quantum dots and quantum well

We investigate the electron-spin injection dynamics via tunneling from an In0.1Ga0.9As quantum well (QW) to In0.5Ga0.5As quantum dots (QDs) in coupled QW-QDs nanostructures. These coupled nanostructures demonstrate ultrafast (5 to 20 ps) spin injection into the QDs. The degree of spin polarization up to 45% is obtained in the QDs after the injection, essentially depending on the injection time. The spin injection and conservation are enhanced with thinner barriers due to the stronger electronic coupling between the QW and QDs. (C) 2014 AIP Publishing LLC

Interdot carrier and spin dynamics in a two-dimensional high-density quantum-dot array of InGaAs with quantum dots embedded as local potential minima

Interdot carrier and spin dynamics were studied in a two-dimensional array of high-density small quantum dots (SQDs) of InGaAs with an average diameter of 16 nm and a sheet density of 1.2 x 10(11) cm(-2), in which 24 nm diametric large QDs (LQDs) were embedded as local potential minima. We observed a delayed photoluminescence (PL) rise from the lower-lying LQD states and a considerably faster PL decay from the higher-lying SQD states, indicating carrier transfer from the two-dimensionally coupled SQDs into the LQDs. In addition, inverse carrier tunneling from the LQDs into the SQDs was thermally induced, which is characterized by the thermal activation energy between the LQDs and SQDs. Moreover, circularly polarized transient PL behavior from the SQD states exhibits a suppression of the spin polarization decay in the initial time region, depending on the excited spin density. This tentatively suppressed spin relaxation can be quantitatively explained by selective interdot transfer of minority-spin electrons from the SQDs into LQDs, when the majority spin states in both QDs are sufficiently populated by excited spins. These findings indicate that the high-density SQDs behave as the main emitters with suppressed spin relaxation, while the scattered LQDs with lower potential behave as the receivers of minority-spin electrons

Persistent High Polarization of Excited Spin Ensembles During Light Emission in Semiconductor Quantum-Dot-Well Hybrid Nanosystems

We demonstrate persistent high degrees of spin polarization (SPD) up to 70% during light emission in (In1-xGax) As quantum-dot-well (QD-QW) hybrid nanosystems, where QD excited states are laterally tunnel coupled through the adjacent two-dimensional QW potential depending on the QW thickness. Spinpolarized electrons are photo-excited by using circularly polarized light pulses. The decay time of spin relaxation, obtained by that of the SPD, is 70 times larger than the photoluminescence decay time. The temporally constant SPD is sustained by a selective transfer of minority spins among QDs after flipping from the majority spins, which is promoted by a moderate state filling of lower-energy spin sublevels in surrounding QDs. The spin transfer times are deduced as functions of the QW thickness and excited-spin density. These results can provide a precise control of lateral interdot spin-transfer dynamics and resultant suppression of spin relaxation in QD ensembles