Annika Bande

Electron dynamics of interatomic Coulombic decay in quantum dots induced by a laser field

In this paper we investigated the dynamics of an electron in the presence of a time-dependent laser field in a model potential for a two-level single-electron semiconductor quantum dot (QD) that is capable of undergoing interatomic Coulombic decay (ICD) together with an electron bound to a neighboring QD. We demonstrate that ICD can be initiated by coupling the two-level QD to either a continuous or a pulsed moderate to strong laser and we obtain the total and partial decay widths of the resonance excited state in agreement with that from the solely decay of the resonance [A. Bande, K. Gokhberg, and L. S. Cederbaum, J. Chem. Phys. 135, 144112 (2011)]. A detailed discussion of the effects of direct ionization by the laser in single- or multi-photon process as well as Rabi oscillations is furthermore presented.

Dynamics of interatomic Coulombic decay in quantum dots.

In this work we demonstrate that the interatomic Coulombic decay (ICD), an ultrafast electron relaxation process known for atoms and molecules, is possible in general binding potentials. We used the multiconfiguration time-dependent Hartree method for fermions to study ICD in real time in a two-electron model system of two potential wells. Two decay channels were identified and analyzed by using the box stabilization analysis as well as by evaluating the autocorrelation function and measuring the outgoing electron flux during time-propagations. The total and partial ICD widths of an excited state localized in one potential well as a function of the distance between the two potentials was obtained. Finally, we discuss the results with a view to a possible application of ICD in quantum dot technology.

Controlled energy-selected electron capture and release in double quantum dots

Highly accurate quantum electron dynamics calculations demonstrate that energy can be efficiently transferred between quantum dots. Specifically, in a double quantum dot an incoming electron is captured by one dot and the excess energy is transferred to the neighboring dot and used to remove an electron from this dot. This process is due to long-range electron correlation and shown to be operative at rather large distances between the dots. The efficiency of the process is greatly enhanced by preparing the double quantum dot such that the incoming electron is initially captured by a two-electron resonance state of the system. In contrast to atoms and molecules in nature, double quantum dots can be manipulated to achieve this enhancement. This mechanism leads to a surprisingly narrow distribution of the energy of the electron removed in the process which is explained by resonance theory. We argue that the process could be exploited in practice.

Rydberg states with quantum Monte Carlo

Calculations on Rydberg states are performed using quantum Monte Carlo methods. Excitation energies and singlet-triplet splittings are calculated for two model systems, the carbon atom (3P and 1P) and carbon monoxide ((1Sigma and 3Sigma). Kohn-Sham wave functions constructed from open-shell localized Hartree-Fock orbitals are used as trial and guide functions. The fixed-node diffusion quantum Monte Carlo (FN-DMC) method depends strongly on the wave functions nodal hypersurface. Nodal artefacts are investigated for the ground state of the carbon atom. Their effect on the FN-DMC results can be analyzed quantitatively. FN-DMC leads to accurate excitation energies but to less accurate singlet-triplet splittings. Variational Monte Carlo calculations are able to reproduce the experimental results for both the excitation energies and the singlet-triplet splittings.

Electron-correlation driven capture and release in double quantum dots.

We recently predicted that the interatomic Coulombic electron capture (ICEC) process, a long-range electron correlation driven capture process, is achievable in gated double quantum dots (DQDs). In ICEC an incoming electron is captured by one quantum dot (QD) and the excess energy is used to remove an electron from the neighboring QD. In this work we present systematic full three-dimensional electron dynamics calculations in quasi-one dimensional model potentials that allow for a detailed understanding of the connection between the DQD geometry and the reaction probability for the ICEC process. We derive an effective one-dimensional approach and show that its results compare very well with those obtained using the full three-dimensional calculations. This approach substantially reduces the computation times. The investigation of the electronic structure for various DQD geometries for which the ICEC process can take place clarify the origin of its remarkably high probability in the presence of two-electron resonances.

Geometrical control of the interatomic coulombic decay process in quantum dots for infrared photodetectors

In electron dynamics calculations the interatomic Coulombic decay (ICD) process has recently been shown to take place in two vertically‐aligned quantum dots (QDs). Energy emitted during the relaxation of one electron in one QD is converted into kinetic energy of another electron ejected from a neighboring QD. As the electronic structure of QDs can be controlled by their geometries, we prove here in thorough scans of the transversal and vertical QD confinement potentials’ widths that geometries are likewise control parameters for ICD. Such a comprehensive investigation has been enabled by a significant development of the calculations in terms of speed achieved among others by optimization of the grid and Coulomb interaction operator representations. As key result of this study we propose two cigar‐shaped singly‐charged GaAs QDs vertically aligned in the direction of their long side for a most efficient QD ICD realization useful for an infrared photodetector.

Favoritism of quantum dot inter-Coulombic decay over direct and multi-photon ionization by laser strength and focus

We study the dynamics of a two-electron system undergoing resonant excitation and inter-Coulombic decay (ICD) in a pair of quantum dots. The influence of the focus of the exciting laser on the ICD process is investigated for a π-pulse with a close look on competing processes, i.e., direct ionization and multi-photon excitations. We scan through the field strength up to six Rabi cycles to show that ICD is still verifiable after several population inversions. With novel analyses, we determine for the first time populations of the different continuum states and thus conclude on the importance of several multi-photon excitation channels. Finally, we look into the influence of complex absorbing potentials on the dynamics.

Interdependence of ICD rates in paired quantum dots on geometry

Using state‐of‐the‐art antisymmetrized multiconfiguration time‐dependent Hartree (MCTDH) electron dynamics calculations we study the interdependence of the intermolecular Coulombic decay (ICD) process on the geometric parameters of a doubly‐charged paired quantum dot (PQD) model system in the framework of the effective mass approximation (EMA). We find that ICD displays a maximum rate for a certain geometry of the electron‐emitting quantum dot, which is simultaneously dependent on both the distance between the quantum dots as well as the photon‐absorbing quantum dots geometry. The rate maximum is shown to be caused by the competing effects of polarization of electron density and Coulomb repulsion. The ICD rate‐maximized PQD geometry in GaAs QDs yields a decay time of 102.39 ps. It is given by two vertically‐aligned cylindrical QDs with radii of 14.42 nm separated by 86.62 nm. The photon absorbing QD then has a height of 46.59 nm and the electron emitting QD a height of 16.33 nm.

Analysis of the Electronic Structure of Aqueous Urea and Its Derivatives: A Systematic Soft X-Ray-TD-DFT Approach.

Soft X-ray emission (XE), absorption (XA), and resonant inelastic scattering (RIXS) experiments have been conducted at the nitrogen K-edge of urea and its derivatives in aqueous solution and were compared with density functional theory and time-dependent density functional theory calculations. This comprehensive study provides detailed information on the occupied and unoccupied molecular orbitals of urea, thiourea, acetamide, dimethylurea, and biuret at valence levels. By identifying the electronic transitions that contribute to the experimental spectral features, the energy gap between the highest occupied and the lowest unoccupied molecular orbital of each molecule is determined. Moreover, a theoretical approach is introduced to simulate resonant inelastic X-ray scattering spectra by adding an extra electron to the lowest unoccupied molecular orbital, thereby mimicking the real initial state of the core-electron absorption before the subsequent relaxation process.

Electron dynamics of interatomic Coulombic decay in quantum dots

The existence of interatomic Coulombic decay in general binding potentials is demonstrated by numerical study of real-time electron dynamics.