arXiv subjects

C. A. Ullrich

Publications and source records attributed to C. A. Ullrich.

33 records · Page 2Linked to original sources

arXiv2006

Time-dependent density-functional theory beyond the adiabatic approximation: insights from a two-electron model system

Most applications of time-dependent density-functional theory (TDDFT) use the adiabatic local-density approximation (ALDA) for the dynamical exchange-correlation potential Vxc(r,t). An exact (i.e., nonadiabatic) extension of the ground-state LDA into the dynamical regime leads to a Vxc(r,t) with a memory, which causes the electron dynamics to become dissipative. To illustrate and explain this nonadiabatic behavior, this paper studies the dynamics of two interacting electrons on a two-dimensional quantum strip of finite size, comparing TDDFT within and beyond the ALDA with numerical solutions of the two-electron time-dependent Schroedinger equation. It is shown explicitly how dissipation arises through multiple particle-hole excitations, and how the nonadiabatic extension of the ALDA fails for finite systems, but becomes correct in the thermodynamic limit.

cond-mat.mes-hall↗

arXiv2006

Degenerate ground states and nonunique potentials: breakdown and restoration of density functionals

The Hohenberg-Kohn (HK) theorem is one of the most fundamental theorems of quantum mechanics, and constitutes the basis for the very successful density-functional approach to inhomogeneous interacting many-particle systems. Here we show that in formulations of density-functional theory (DFT) that employ more than one density variable, applied to systems with a degenerate ground state, there is a subtle loophole in the HK theorem, as all mappings between densities, wave functions and potentials can break down. Two weaker theorems which we prove here, the joint-degeneracy theorem and the internal-energy theorem, restore the internal, total and exchange-correlation energy functionals to the extent needed in applications of DFT to atomic, molecular and solid-state physics and quantum chemistry. The joint-degeneracy theorem constrains the nature of possible degeneracies in general many-body systems.

cond-mat.mtrl-sci↗

arXiv2006

Enhanced carrier scattering rates in dilute magnetic semiconductors with correlated impurities

In III-V dilute magnetic semiconductors (DMSs) such as Ga$_{1-x}$Mn$_x$As, the impurity positions tend to be correlated, which can drastically affect the electronic transport properties of these materials. Within the memory function formalism we have derived a general expression for the current relaxation kernel in spin and charge disordered media and have calculated spin and charge scattering rates in the weak-disorder limit. Using a simple model for magnetic impurity clustering, we find a significant enhancement of the charge scattering. The enhancement is sensitive to cluster parameters and may be controllable through post-growth annealing.

cond-mat.mtrl-sci↗

arXiv2006

Non-adiabatic electron dynamics in time-dependent density-functional theory

Time-dependent density-functional theory (TDDFT) treats dynamical exchange and correlation (xc) via a single-particle potential, Vxc(r,t), defined as a nonlocal functional of the density n(r',t'). The popular adiabatic local-density approximation (ALDA) for Vxc(r,t) uses only densities at the same space-time point (r,t). To go beyond the ALDA, two local approximations have been proposed based on quantum hydrodynamics and elasticity theory: (a) using the current as basic variable (C-TDDFT) [G. Vignale, C. A. Ullrich, and S. Conti, Phys. Rev. Lett. 79, 4878 (1997)], (b) working in a co-moving Lagrangian reference frame (L-TDDFT) [I. V. Tokatly, Phys. Rev. B 71, 165105 (2005)]. This paper illustrates, compares, and analyzes both non-adiabatic theories for simple time-dependent model densities in the linear and nonlinear regime, for a broad range of time and frequency scales. C- and L-TDDFT are identical in certain limits, but in general exhibit qualitative and quantitative differences in their respective treatment of elastic and dissipative electron dynamics. In situations where the electronic density rapidly undergoes large deformations, it is found that non-adiabatic effects can become significant, causing the ALDA to break down.

cond-mat.mes-hall↗

arXiv2005

Dissipation through spin Coulomb drag in electronic spin dynamics

Spin Coulomb drag (SCD) constitutes an intrinsic source of dissipation for spin currents in metals and semiconductors. We discuss the power loss due to SCD in potential spintronics devices and analyze in detail the associated damping of collective spin-density excitations. It is found that SCD contributes substantially to the linewidth of intersubband spin plasmons in parabolic quantum wells, which suggests the possibility of a purely optical quantitative measurement of the SCD effect by means of inelastic light scattering.

cond-mat.mes-hall↗

arXiv2005

Nonuniqueness in spin-density-functional theory on lattices

In electronic many-particle systems, the mapping between densities and spin magnetizations, {n(r), m(r)}, and potentials and magnetic fields, {v(r), B(r)}, is known to be nonunique, which has fundamental and practical implications for spin-density-functional theory (SDFT). This paper studies the nonuniqueness (NU) in SDFT on arbitrary lattices. Two new, non-trivial cases are discovered, here called local saturation and global noncollinear NU, and their properties are discussed and illustrated. In the continuum limit, only some well-known special cases of NU survive.

cond-mat.mes-hall↗

arXiv2004

Time-dependent Kohn-Sham theory with memory

In time-dependent density-functional theory, exchange and correlation (xc) beyond the adiabatic local density approximation can be described in terms of viscoelastic stresses in the electron liquid. In the time domain, this leads to a velocity-dependent xc vector potential with a memory containing short- and long-range components. The resulting time-dependent Kohn-Sham formalism describes the dynamics of electronic systems including decoherence and relaxation. For the example of collective charge-density oscillations in a quantum well, we illustrate the xc memory effects, clarify the dissipation mechanism, and extract intersubband relaxation rates for weak and strong excitations.

cond-mat.mes-hall↗

arXiv2003

Coherent control of intersubband optical bistability in quantum wells

We present a study of the nonlinear intersubband (ISB) response of conduction electrons in a GaAs/AlGaAs quantum well to strong THz radiation, using a density-matrix approach combined with time-dependent density-functional theory. We demonstrate coherent control of ISB optical bistability, using THz control pulses to induce picosecond switching between the bistable states. The switching speed is determined by the ISB relaxation and decoherence times, T1 and T2.

cond-mat.mes-hall↗

arXiv2003

Anisotropic splitting of intersubband spin plasmons in quantum wells with bulk and structural inversion asymmetry

In semiconductor heterostructures, bulk and structural inversion asymmetry and spin-orbit coupling induce a k-dependent spin splitting of valence and conduction subbands, which can be viewed as being caused by momentum-dependent crystal magnetic fields. This paper studies the influence of these effective magnetic fields on the intersubband spin dynamics in an asymmetric n-type GaAs/AlGaAs quantum well. We calculate the dispersions of intersubband spin plasmons using linear response theory. The so-called D'yakonov-Perel' decoherence mechanism is inactive for collective intersubband excitations, i.e., crystal magnetic fields do not lead to decoherence of spin plasmons. Instead, we predict that the main signature of bulk and structural inversion asymmetry in intersubband spin dynamics is a three-fold, anisotropic splitting of the spin plasmon dispersion. The importance of many-body effects is pointed out, and conditions for experimental observation with inelastic light scattering are discussed.

cond-mat.mes-hall↗

arXiv2002

Intersubband spin-density excitations in quantum wells with Rashba spin splitting

In inversion-asymmetric semiconductors, spin-orbit coupling induces a k-dependent spin splitting of valence and conduction bands, which is a well-known cause for spin decoherence in bulk and heterostructures. Manipulating nonequilibrium spin coherence in device applications thus requires understanding how valence and conduction band spin splitting affects carrier spin dynamics. This paper studies the relevance of this decoherence mechanism for collective intersubband spin-density excitations (SDEs) in quantum wells. A density-functional formalism for the linear spin-density matrix response is presented that describes SDEs in the conduction band of quantum wells with subbands that may be non-parabolic and spin-split due to bulk or structural inversion asymmetry (Rashba effect). As an example, we consider a 40 nm GaAs/AlGaAs quantum well, including Rashba spin splitting of the conduction subbands. We find a coupling and wavevector-dependent splitting of the longitudinal and transverse SDEs. However, decoherence of the SDEs is not determined by subband spin splitting, due to collective effects arising from dynamical exchange and correlation.

cond-mat.mes-hall↗

arXiv2002

Degeneracy in Density Functional Theory: Topology in v- and n-Space

This paper clarifies the topology of the mapping between v- and n-space in fermionic systems. Density manifolds corresponding to degeneracies g=1 and g>1 are shown to have the same mathematical measure: every density near a g-ensemble-v-representable (g-VR) n(r) is also g-VR (except ``boundary densities'' of lower measure). The role of symmetry and the connection between T=0 and T=0+ are discussed. A lattice model and the Be-series are used as illustrations.

cond-mat.mtrl-sci↗

arXiv2002

Time-dependent current density functional theory for the linear response of weakly disordered systems

This paper develops a quantitatively accurate first-principles description for the frequency and the linewidth of collective electronic excitations in inhomogeneous weakly disordered systems. A finite linewidth in general has intrinsic and extrinsic sources. At low temperatures and outside the region where electron-phonon interaction occurs, the only intrinsic damping mechanism is provided by electron-electron interaction. This kind of intrinsic damping can be described within time-dependent density-functional theory (TDFT), but one needs to go beyond the adiabatic approximation and include retardation effects. It was shown previously that a density-functional response theory that is local in space but nonlocal in time has to be constructed in terms of the currents, rather than the density. This theory will be reviewed in the first part of this paper. For quantitatively accurate linewidths, extrinsic dissipation mechanisms, such as impurities or disorder, have to be included. In the second part of this paper, we discuss how extrinsic dissipation can be described within the memory function formalism. We first review this formalism for homogeneous systems, and then present a synthesis of TDFT with the memory function formalism for inhomogeneous systems, to account simultaneously for intrinsic and extrinsic damping of collective excitations. As example, we calculate frequencies and linewidths of intersubband plasmons in a 40 nm wide GaAs/AlGaAs quantum well.

cond-mat.mes-hall↗

arXiv1999

Collective charge-density excitations of non-circular quantum dots in a magnetic field

Recent photoabsorption measurements have revealed a rich fine structure in the collective charge-density excitation spectrum of few-electron quantum dots in the presence of magnetic fields. We have performed systematic computational studies of the far-infrared density response of quantum dots, using time-dependent density-functional theory in the linear regime and treating the dots as two-dimensional disks. It turns out that the main characteristics observed in the experiment can be understood in terms of the electronic shell structure of the quantum dots. However, new features arise if a breaking of the circular symmetry of the dots is allowed, leading to an improved description of the experimental results.

cond-mat.mes-hall↗

arXiv1998

Collective intersubband transitions in quantum wells: a comparative density-functional study

We use time-dependent (current) density functional theory to study collective transitions between the two lowest subbands in GaAs/AlGaAs quantum wells. We focus on two systems where experimental results are available: a wide single and a narrow asymmetric double well. The aim is to calculate frequency and linewidth of collective electronic modes damped via electron-electron interaction only. Since Landau damping is not effective here, the dominant damping mechanism involves dynamical exchange-correlation effects such as multipair production. To capture these effects, one has to go beyond the widely used adiabatic local density approximation (ALDA) and include retardation. We perform a comparative study of two approaches which fall in this category: the dynamical extension of the ALDA by Gross and Kohn, and a more recent method which treats exchange and correlation beyond the ALDA as viscoelastic stresses in the electron liquid. We find that the former method is more robust: it performs similarly for strongly different degrees of collectivity of the electronic motion. Results for quantum wells compare reasonably to experiment, with a tendency towards overdamping. By contrast, the viscoelastic approach is superior for systems where the electron dynamics is predominantly collective, but breaks down if the local velocity field is too rapidly varying, as in the case of a single-electron-like behavior such as tunneling through a potential barrier.

cond-mat.mes-hall↗

arXiv1997

Time-dependent density functional theory beyond the adiabatic local density approximation

In the current density functional theory of linear and nonlinear time-dependent phenomena, the treatment of exchange and correlation beyond the level of the adiabatic local density approximation is shown to lead to the appearance of viscoelastic stresses in the electron fluid. Complex and frequency-dependent viscosity/elasticity coefficients are microscopically derived and expressed in terms of properties of the homogeneous electron gas. As a first consequence of this formalism, we provide an explicit formula for the linewidths of collective excitations in electronic systems.

cond-mat↗