Electronic states in a magnetic quantum-dot molecule: phase transitions and spontaneous symmetry breaking

We show that a double quantum-dot system made of diluted magnetic semiconductor behaves unlike usual molecules. In a semiconductor double quantum dot or in a diatomic molecule, the ground state of a single carrier is described by a symmetric orbital. In a magnetic material molecule, new ground states with broken symmetry can appear due the competition between the tunnelling and magnetic polaron energy. With decreasing temperature, the ground state changes from the normal symmetric state to a state with spontaneously broken symmetry. Interestingly, the symmetry of a magnetic molecule is recovered at very low temperatures. A magnetic double quantum dot with broken-symmetry phases can be used a voltage-controlled nanoscale memory cell.Comment: 4 pages, 5 figure

Spin-Forster transfer in optically excited quantum dots

The mechanisms of energy and spin transfer in quantum dot pairs coupled via the Coulomb interaction are studied. Exciton transfer can be resonant or phonon-assisted. In both cases, the transfer rates strongly depend on the resonance conditions. The spin selection rules in the transfer process come from the exchange and spin-orbit interactions. The character of energy dissipation in spin transfer is different than that in the traditional spin currents. The spin-dependent photon cross-correlation functions reflect the exciton transfer process. In addition, a mathematical method to calculate F\"orster transfer in crystalline nanostructures beyond the dipole-dipole approximation is described.Comment: 22 pages, 10 figures, Phys. Rev. B, in pres

Semiconductor-metal nanoparticle molecules: hybrid excitons and non-linear Fano effect

Modern nanotechnology opens the possibility of combining nanocrystals of various materials with very different characteristics in one superstructure. The resultant superstructure may provide new physical properties not encountered in homogeneous systems. Here we study theoretically the optical properties of hybrid molecules composed of semiconductor and metal nanoparticles. Excitons and plasmons in such a hybrid molecule become strongly coupled and demonstrate novel properties. At low incident light intensity, the exciton peak in the absorption spectrum is broadened and shifted due to incoherent and coherent interactions between metal and semiconductor nanoparticles. At high light intensity, the absorption spectrum demonstrates a surprising, strongly asymmetric shape. This shape originates from the coherent inter-nanoparticle Coulomb interaction and can be viewed as a non-linear Fano effect which is quite different from the usual linear Fano resonance.Comment: 5 pages, 5 figures, submitted to Phys. Rev. Let

Understanding Hot-Electron Generation and Plasmon Relaxation in Metal Nanocrystals: Quantum and Classical Mechanisms

Generation of energetic (hot) electrons is an intrinsic property of any plasmonic nanostructure under illumination. Simultaneously, a striking advantage of metal nanocrystals over semiconductors lies in their very large absorption cross sections. Therefore, metal nanostructures with strong and tailored plasmonic resonances are very attractive for photocatalytic applications. However, the central questions regarding plasmonic hot electrons are how to quantify and extract the optically-excited energetic electrons in a nanocrystal. We develop a theory describing the generation rates and the energy-distributions of hot electrons in nanocrystals with various geometries. In our theory, hot electrons are generated owing to surfaces and hot spots. The formalism predicts that large optically-excited nanocrystals show the excitation of mostly low-energy Drude electrons, whereas plasmons in small nanocrystals involve mostly hot electrons. The energy distributions of electrons in an optically-excited nanocrystal show how the quantum many-body state in small particles evolves towards the classical state described by the Drude model when increasing nanocrystal size. We show that the rate of surface decay of plasmons in nanocrystals is directly related to the rate of generation of hot electrons. Based on a detailed many-body theory involving kinetic coefficients, we formulate a simple scheme describing the plasmon's dephasing. In most nanocrystals, the main decay mechanism of a plasmon is the Drude friction-like process and the secondary path comes from generation of hot electrons due to surfaces and electromagnetic hot spots. This latter path strongly depends on the size, shape and material of the nanocrystal, correspondingly affecting its efficiency of hot-electron production. The results in the paper can be used to guide the design of plasmonic nanomaterials for photochemistry and photodetectors.Comment: 90 pages, 21 figures, including Supplementary Informatio