Photoluminescence spectroscopy and lifetime measurements from self-assembled semiconductor-metal nanoparticle hybrid arrays

We present results of photoluminescence spectroscopy and lifetime measurements on thin film hybrid arrays of semiconductor quantum dots and metal nanoparticles embedded in a block copolymer template. The intensity of emission as well as the measured lifetime would be controlled by varying the volume fraction and location of gold nanoparticles in the matrix. We demonstrate the ability to both enhance and quench the luminescence in the hybrids as compared to the quantum dot array films while simultaneously engineering large reduction in luminescence lifetime with incorporation of gold nanoparticles. (C) 2010 American Institute of Physics. [doi:10.1063/1.3483162].

Two-channel Kondo physics in odd impurity chains

We study odd-membered chains of spin-1/2 impurities, with each end connected to its own metallic lead. For antiferromagnetic exchange coupling, universal two-channel Kondo (2CK) physics is shown to arise at low energies. Two overscreening mechanisms are found to occur depending on coupling strength, with distinct signatures in physical properties. For strong interimpurity coupling, a residual chain spin-1/2 moment experiences a renormalized effective coupling to the leads, while in the weak-coupling regime, Kondo coupling is mediated via incipient single-channel Kondo singlet formation. We also investigate models in which the leads are tunnel-coupled to the impurity chain, permitting variable dot filling under applied gate voltages. Effective low-energy models for each regime of filling are derived, and for even fillings where the chain ground state is a spin singlet, an orbital 2CK effect is found to be operative. Provided mirror symmetry is preserved, 2CK physics is shown to be wholly robust to variable dot filling; in particular, the single-particle spectrum at the Fermi level, and hence the low-temperature zero-bias conductance, is always pinned to half-unitarity. We derive a Friedel-Luttinger sum rule and from it show that, in contrast to a Fermi liquid, the Luttinger integral is nonzero and determined solely by the ``excess'' dot charge as controlled by gate voltage. The relevance of the work to real quantum dot devices, where interlead charge-transfer processes fatal to 2CK physics are present, is also discussed. Physical arguments and numerical renormalization-group techniques are used to obtain a detailed understanding of these problems.

Ionic Bonding between Artificial Atoms

Conventional solids are prepared from building blocks that are conceptually no larger than a hundred atoms. While van der Waals and dipole-dipole interactions also influence the formation of these materials, stronger interactions, referred to as chemical bonds, play a more decisive role in determining the structures of most solids. Chemical bonds that hold such materials together are said to be ionic, covalent, metallic, dative, or otherwise a combination of these. Solids that utilize semiconductor nanocrystal quantum dots as building units have been demonstrated to exist; however, the interparticle forces in such materials are decidedly not chemical. Here we demonstrate the formation of charge transfer states in a binary quantum dot mixture. Charge is observed to reside in quantum confined states of one of the participating quantum dots. These interactions lead to materials that may be regarded as the nanoscale analog of an ionic solid. The process by which these materials form has interesting parallels to chemical reactions in conventional chemistry.

Interplay of electrostatics and lipid packing determines the binding of charged polymer coated nanoparticles to model membranes

Understanding of nanoparticle-membrane interactions is useful for various applications of nanoparticles like drug delivery and imaging. Here we report on the studies of interaction between hydrophilic charged polymer coated semiconductor quantum dot nanoparticles with model lipid membranes. Atomic force microscopy and X-ray reflectivity measurements suggest that cationic nanoparticles bind and penetrate bilayers of zwitterionic lipids. Penetration and binding depend on the extent of lipid packing and result in the disruption of the lipid bilayer accompanied by enhanced lipid diffusion. On the other hand, anionic nanoparticles show minimal membrane binding although, curiously, their interaction leads to reduction in lipid diffusivity. It is suggested that the enhanced binding of cationic QDs at higher lipid packing can be understood in terms of the effective surface potential of the bilayers which is tunable through membrane lipid packing. Our results bring forth the subtle interplay of membrane lipid packing and electrostatics which determine nanoparticle binding and penetration of model membranes with further implications for real cell membranes.

Hidden role of anion exchange reactions in nucleation of colloidal nanocrystals

We investigate the processes involved in the nucleation of colloidal lead selenide nanoparticles. Our studies show that an unusual pathway - an anion exchange reaction, causes the nucleation of lead selenide nanocrystals. In this process, one quantum dot is transformed into another due to a substitution of its constituent anions. The existence of this pathway was never anticipated perhaps due to its unusually rapid kinetics. The nucleation and growth kinetics of colloidal lead selenide quantum dots are found to fit well to a two-step process. The rate constant associated with the anion exchange process is found to be four orders of magnitude greater than that of the nanocrystal growth. The complete consumption of the initial oxide nanoparticle thus provides a sharp, temporally well-defined nucleation event.

169 GHz repetition rate passively harmonically mode-locked VECSEL emitting 265 fs pulses

High repetition rate passively mode-locked sources are of significant interest due to their potential for applications including optical clocking, optical sampling, communications and others. Due to their short excited state lifetimes mode-locked VECSELs are ideally suited to high repetition rate operation, however fundamentally mode-locked quantum well-based VECSELs have not achieved repetition rates above 10 GHz due to the limitations placed on the cavity geometry by the requirement that the saturable absorber saturates more quickly than the gain. This issue has been overcome by the use of quantum dot-based saturable absorbers with lower saturation fluences leading to repetition rates up to 50 GHz, but sub-picosecond pulses have not been achieved at these repetition rates. We present a passively harmonically mode-locked VECSEL emitting pulses of 265 fs duration at a repetition rate of 169 GHz with an output power of 20 mW. The laser is based around an antiresonant 6 quantum well gain sample and is mode-locked using a semiconductor saturable absorber mirror. Harmonic modelocking is achieved by using an intracavity sapphire etalon. The sapphire then acts as a coupled cavity, setting the repetition rate of the laser while still allowing a tight focus on the saturable absorber. RF spectra of the laser output show no peaks at harmonics of the fundamental repetition rate up to 26 GHz, indicating stable harmonic modelocking. Autocorrelations reveal groups of pulses circulating in the cavity as a result of an increased tendency towards Q-switched modelocking due to the low pulse energies.

Three-dimensional supercell simulation of novel semiconductor nanostructures

In this thesis we investigate atomic scale imperfections and fluctuations in the quantum transport properties of novel semiconductor nanostructures. For this purpose, we have developed a numerically efficient supercell model of quantum transport capable of representing potential variations in three dimensions. This flexibility allows us to examine new quantum device structures made possible through state-of-the-art semiconductor fabrication techniques such as molecular beam epitaxy and nanolithography. These structures, with characteristic dimensions on the order of a few nanometers, hold promise for much smaller, faster and more efficient devices than those in present operation, yet they are highly sensitive to structural and compositional variations such as defect impurities, interface roughness and alloy disorder. If these quantum structures are to serve as components of reliable, mass-produced devices, these issues must be addressed.

In Chapter 1 we discuss some of the important issues in resonant tunneling devices and mention some of thier applications. In Chapters 2 and 3, we describe our supercell model of quantum transport and an efficient numerical implementation. In the remaining chapters, we present applications.

In Chapter 4, we examine transport in single and double barrier tunneling structures with neutral impurities. We find that an isolated attractive impurity in a single barrier can produce a transmission resonance whose position and strength are sensitive to the location of the impurity within the barrier. Multiple impurities can lead to a complex resonance structure that fluctuates widely with impurity configuration. In addition, impurity resonances can give rise to negative differential resistance. In Chapter 5, we study interface roughness and alloy disorder in double barrier structures. We find that interface roughness and alloy disorder can shift and broaden the n = 1 transmission resonance and give rise to new resonance peaks, especially in the presence of clusters comparable in size to the electron deBroglie wavelength. In Chapter 6 we examine the effects of interface roughness and impurities on transmission in a quantum dot electron waveguide. We find that variation in the configuration and stoichiometry of the interface roughness leads to substantial fluctuations in the transmission properties. These fluctuations are reduced by an attractive impurity placed near the center of the dot.

Single-particle probing of edge-state formation in a graphene nanoribbon

We investigate the effect of a perpendicular magnetic field on the single-particle charging spectrum of a graphene quantum dot embedded inline with a nanoribbon. We observe uniform shifts in the single-particle spectrum which coincide with peaks in the magnetoconductance, implicating Landau level condensation and edge state formation as the mechanism underlying magnetic field-enhanced transmission through graphene nanostructures. The experimentally determined ratio of bulk to edge states is supported by single-particle band-structure simulations, while a fourfold beating of the Coulomb blockade transmission amplitude points to many-body interaction effects during Landau level condensation of the ν=0 state. © 2012 American Physical Society.

Superradiant emission in semiconductor diode laser structures

This paper reviews recent advances in superradiant (SR) emission in semiconductors at room temperature, a process which has been shown to enable the generation on demand of high power picosecond or subpicosecond pulses across a range of different wavelengths. The different characteristic features of SR emission from semiconductor devices with bulk, quantum-well, and quantum-dot active regions are outlined, and particular emphasis is placed on comparing the characteristic features of SR with those of lasing. Finally, potential applications of SR pulses are discussed. © 1995-2012 IEEE.

Direct detection of the relative strength of Rashba and Dresselhaus spin-orbit interaction: Utilizing the SU(2) symmetry

We propose a simple method to detect the relative strength of Rashba and Dresselhaus spin-orbit interactions in quantum wells (QWs) without relying on the directional-dependent physical quantities. This method utilizes the two different critical gate voltages that leading to the remarkable signals of SU(2) symmetry, which happens to reflect the intrinsic-structure-inversion asymmetry of the QW. We support our proposal by the numerical calculation of in-plane relaxation times based on the self-consistent eight-band Kane model. We find that the two different critical gate voltages leading to the maximum spin-relaxation times [one effect of the SU(2) symmetry] can simply determine the ratio of the coefficients of Rashba and Dresselhaus terms. Our proposal can also be generalized to extract the relative strengths of the spin-orbit interactions in quantum-wire and quantum-dot structures.

Single-photon-emitting diode at liquid nitrogen temperature

We report on the study of a single-photon-emitting diode at 77 K. The device is composed of InAs/GaAs quantum dots embedded in the i-region of a p-i-n diode structure. The high signal to noise ratio of the electroluminescence, as well as the small second order correlation function at zero-delay g((2))(0), implies that the device has a low multiphoton emission probability. By comparing the device performances under different excitation conditions, we have, in detail, discussed the basic parameters, such as signal to noise ratio and g((2))(0), and provided some useful information for the future application. (c) 2008 American Institute of Physics.

Electronic structure of a hydrogenic acceptor impurity in semiconductor nano-structures

The electronic structure and binding energy of a hydrogenic acceptor impurity in 2, 1, and 0-dimensional semiconductor nano-structures (i.e. quantum well (QW), quantum well wire (QWW), and quantum dot (QD)) are studied in the framework of effective-mass envelope-function theory. The results show that (1) the energy levels monotonically decrease as the quantum confinement sizes increase; (2) the impurity energy levels decrease more slowly for QWWs and QDs as their sizes increase than for QWs; (3) the changes of the acceptor binding energies are very complex as the quantum confinement size increases; (4) the binding energies monotonically decrease as the acceptor moves away from the nano-structures' center; (5) as the symmetry decreases, the degeneracy is lifted, and the first binding energy level in the QD splits into two branches. Our calculated results are useful for the application of semiconductor nano-structures in electronic and photoelectric devices.

Reduced dynamics with renormalization in solid-state charge qubit measurement

Quantum measurement will inevitably cause backaction on the measured system, resulting in the well-known dephasing and relaxation. In this paper, in the context of solid-state qubit measurement by a mesoscopic detector, we show that an alternative backaction known as renormalization is important under some circumstances. This effect is largely overlooked in the theory of quantum measurement.

Indium-Induced Effect on Polarized Electroluminescence from InGaN/GaN MQWs Light Emitting Diodes

Polarization-resolved edge-emitting electroluminescence (EL) studies of InGaN/GaN MQWs of wavelengths from near-UV (390 nm) to blue (468 nm) light-emitting diodes (LEDs) are performed. Although the TE mode is dominant in all the samples of InGaN/GaN MQW LEDs, an obvious difference of light polarization properties is found in the InGaN/GaN MQW LEDs with different wavelengths. The polarization degree decreases from 52.4% to 26.9% when light wavelength increases. Analyses of band structures of InGaN/GaN quantum wells and luminescence properties of quantum dots imply that quantum-dot-like behavior is the dominant reason for the low luminescence polarization degree of blue LEDs, and the high luminescence polarization degree of UV LEDs mainly comes from QW confinement and the strain effect. Therefore, indium induced carrier confinement (quantum-dot-like behavior) might play a major role in the polarization degree change of InGaN/GaN MQW LEDs from near violet to blue.

Single-photon source in strong photon-atom interaction regime in quasiperiodic photonic crystals

The antibunching properties of the fluorescence from a two-level ideal system in a 12-fold quasiperiodic photonic crystal are investigated based on the calculated local density of states. We found that the antibunching phenomenon of the fluorescence from two-level ideal systems could be significantly changed by varying their positions, i.e., perfect antibunching and antibunching with damped Rabi oscillation phenomenon occurred in different positions and at different frequencies in photonic crystals as a result of the large differences in the local density of states. This study revealed that the multi-level coherence of fluorescence from a two-level ideal system could be manipulated by controlling the position of the two-level ideal system in photonic crystals and the emission frequency in the photonic band structure. Copyright (C) EPLA, 2008