▪ Abstract Solution phase syntheses and size-selective separation methods to prepare semiconductor and metal nanocrystals, tunable in size from ∼1 to 20 nm and monodisperse to ≤5%, are presented. Preparation of monodisperse samples enables systematic characterization of the structural, electronic, and optical properties of materials as they evolve from molecular to bulk in the nanometer size range. Sample uniformity makes it possible to manipulate nanocrystals into close-packed, glassy, and ordered nanocrystal assemblies (superlattices, colloidal crystals, supercrystals). Rigorous structural characterization is critical to understanding the electronic and optical properties of both nanocrystals and their assemblies. At inter-particle separations 5–100 A, dipole-dipole interactions lead to energy transfer between neighboring nanocrystals, and electronic tunneling between proximal nanocrystals gives rise to dark and photoconductivity. At separations <5 A, exchange interactions cause otherwise insulating ass...

Synthesis and Characterization of Monodisperse Nanocrystals and Close-Packed Nanocrystal Assemblies

Electronic excitations lie at the origin of most of the commonly measured spectra. However, the first-principles computation of excited states requires a larger effort than ground-state calculations, which can be very efficiently carried out within density-functional theory. On the other hand, two theoretical and computational tools have come to prominence for the description of electronic excitations. One of them, many-body perturbation theory, is based on a set of Green’s-function equations, starting with a one-electron propagator and considering the electron-hole Green’s function for the response. Key ingredients are the electron’s self-energy S and the electron-hole interaction. A good approximation for S is obtained with Hedin’s GW approach, using density-functional theory as a zero-order solution. First-principles GW calculations for real systems have been successfully carried out since the 1980s. Similarly, the electron-hole interaction is well described by the Bethe-Salpeter equation, via a functional derivative of S. An alternative approach to calculating electronic excitations is the time-dependent density-functional theory (TDDFT), which offers the important practical advantage of a dependence on density rather than on multivariable Green’s functions. This approach leads to a screening equation similar to the Bethe-Salpeter one, but with a two-point, rather than a four-point, interaction kernel. At present, the simple adiabatic local-density approximation has given promising results for finite systems, but has significant deficiencies in the description of absorption spectra in solids, leading to wrong excitation energies, the absence of bound excitonic states, and appreciable distortions of the spectral line shapes. The search for improved TDDFT potentials and kernels is hence a subject of increasing interest. It can be addressed within the framework of many-body perturbation theory: in fact, both the Green’s functions and the TDDFT approaches profit from mutual insight. This review compares the theoretical and practical aspects of the two approaches and their specific numerical implementations, and presents an overview of accomplishments and work in progress.

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Electronic excitations: density-functional versus many-body Green's-function approaches

The authors formulate a new paradigm for computing with cellular automata (CAS) composed of arrays of quantum devices-quantum cellular automata. Computing in such a paradigm is edge driven. Input, output, and power are delivered at the edge of the CA array only; no direct flow of information or energy to internal cells is required. Computing in this paradigm is also computing with the ground state. The architecture is so designed that the ground-state configuration of the array, subject to boundary conditions determined by the input, yields the computational result. The authors propose a specific realization of these ideas using two-electron cells composed of quantum dots. The charge density in the cell is very highly polarized (aligned) along one of the two cell axes, suggestive of a two-state CA. The polarization of one cell induces a polarization in a neighboring cell through the Coulomb interaction in a very non-linear fashion. Quantum cellular automata can perform useful computing. The authors show that AND gates, OR gates, and inverters can be constructed and interconnected.

https://iopscience.iop.org/article/10.1088/0957-4484/4/1/004/pdf

Quantum Cellular Automata

The goal of this paper is to review in brief the basic physics of single-election devices, as well as their-current and prospective applications. These devices based on the controllable transfer of single electrons between small conducting "islands", have already enabled several important scientific experiments. Several other applications of analog single-election devices in unique scientific instrumentation and metrology seem quite feasible. On the other hand, the prospect of silicon transistors being replaced by single-electron devices in integrated digital circuits faces tough challenges and remains uncertain. Nevertheless, even if this replacement does not happen, single electronics will continue to play an important role by shedding light on the fundamental size limitations of new electronic devices. Moreover, recent research in this field has generated some by-product ideas which may revolutionize random-access-memory and digital-data-storage technologies.

Single-electron devices and their applications

Six years after their birth, terahertz quantum-cascade lasers can now deliver milliwatts or more of continuous-wave coherent radiation throughout the terahertz range — the spectral regime between millimetre and infrared wavelengths, which has long resisted development. This paper reviews the state-of-the-art and future prospects for these lasers, including efforts to increase their operating temperatures, deliver higher output powers and emit longer wavelengths.

Terahertz quantum-cascade lasers

The existence of multipole surface-plasmon modes at simple-metal surfaces is demonstrated both experimentally and theoretically. Inelastic reflection electron-scattering experiments on smooth films of K and Na show loss peaks originating from the ordinary surface plasmon as well as from a higher-energy multipole mode. Microscopic density-functional calculations of the electron-loss function reproduce the energy and momentum dispersion of both of these surface modes. For Al, the multipole mode is shown to be too weak to be observable in electron-loss spectroscopy.

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Multipole plasmon modes at a metal surface.

The normal modes at the surface of simple metals

Les interactions a plusieurs corps ne produisent aucun deplacement significatif dans la frequence d'absorption de l'infra-rouge lointain pour un systeme de points quantiques bien separes avec des potentiels de confinement paraboliques. Ceci est contraire au resultat base sur l'approximation de la phase aleatoire, mais en bon accord avec de recents resultats experimentaux

Electromagnetic response of quantum dots.

We investigate the possibility of generating a spontaneous anti‐ferroelectric polarization in an array of elongated quantum dots, which we call ‘‘quantum dashes.’’ We suggest ways in which this phenomenon might be observed and point out possible technological applications resulting from this phenomenon.

Spontaneous polarization of electrons in quantum dashes

We develop a first-principles, self-consistent theory of the far-infrared (FIR) electromagnetic response for electrons confined in a quantum dot. We find that for small electron number ${\mathit{n}}_{\mathit{e}}$, the FIR absorption spectrum corresponds to that associated with parabolic confinement, i.e., absorption dominated by a single peak, which occurs at the frqeuency corresponding to the interlevel separation of the parabolic potential, and is roughly independent of ${\mathit{n}}_{\mathit{e}}$. For large electron number, an upward shift in the resonance frequency occurs as the electron density probes the increasingly nonparabolic curvature of the dot potential. Effects of an applied magnetic field are also investigated.

Pradip Bakshi

Papers

Multipole plasmon modes at a metal surface.

The normal modes at the surface of simple metals

Electromagnetic response of quantum dots.

Spontaneous polarization of electrons in quantum dashes

Self-Consistent Far-Infrared Response of Quantum-Dot Structures