Walter, D. ; Neuhauser, D. ; Baer, R. Quantum interference in polycyclic hydrocarbon molecular wires. Chem. Phys. 2004, 299, 139–145.Abstract

The construction of devices based on molecular components depends upon the development of molecular wires with adaptable current-voltage characteristics. Here, we report that quantum interference effects could lead to substantial differences in conductance in molecular wires which include some simple polycyclic aromatic hydrocarbons (PAHs). For molecular wires containing a single benzene. anthracene or tetracene molecule a large peak appears in the electron transmission probability spectrum at an energy just above the lowest unoccupied orbital (LUMO). For a molecular wire containing a single naphthalene molecule, however, this same peak essentially vanishes. Furthermore, the peak can be re-established by altering the attachment points of the molecular leads to the naphthalene molecule. A breakdown of the individual terms contributing the relevant peak confirms that these results are in fact due to quantum interference effects. (C) 2004 Elsevier B.V. All rights reserved.

Liang, W. Z. ; Baer, R. ; Saravanan, C. ; Shao, Y. ; Bell, A. T. ; Head-Gordon, M. Fast methods for resumming matrix polynomials and Chebyshev matrix polynomials. J. Comput. Phys. 2004, 194, 575–587. liang2004fast.pdf
Kurzweil, Y. ; Baer, R. Time-dependent exchange-correlation current density functionals with memory. J. Chem. Phys. 2004, 121, 8731–8741.Abstract

Most present applications of time-dependent density functional theory use adiabatic functionals, i.e. the effective potential at time t is determined solely by the density at the same time. This paper discusses a method that aims to go beyond this approximation, by incorporating "memory" effects: the potential will depend not only on present behavior but also on the past. In order to ensure the derived potentials are causal, we formulate the action on the Keldysh contour for electrons in electromagnetic fields, from which we derive suitable Kohn-Sham equations. The exchange correlation action is now a functional of the electron density and velocity field. A specific action functional is constructed which is Galilean invariant and yields a causal vector potential term to the Kohn-Sham equations that incorporates causal memory effects. We show explicitly that the exchange-correlation Lorentz force is zero. The potential is consistent with known dynamical properties of the homogeneous electron gas (in the linear response limit).

Hawthorne, M. F. ; Zink, J. I. ; Skelton, J. M. ; Bayer, M. J. ; Liu, C. ; Livshits, E. ; Baer, R. ; Neuhauser, D. Electrical or Photocontrol of the Rotary Motion of a Metallacarborane. Science 2004, 303, 1849–1851.Abstract

Rotary motion around a molecular axis has been controlled by simple electron transfer processes and by photoexcitation. The basis of the motion is intramolecular rotation of a carborane cage ligand (7,8-dicarbollide) around a nickel axle. The Ni(III) metallacarborane structure is a transoid sandwich with two pairs of carbon vertices reflected through a center of symmetry, but that of the Ni(IV) species is cisoid. The interconversion of the two provides the basis for controlled, rotational, oscillatory motion. The energies of the Ni(III) and Ni(IV) species are calculated as a function of the rotation angle.

Hod, O. ; Baer, R. ; Rabani, E. Feasible nanometric magnetoresistance devices. The Journal of Physical Chemistry B 2004, 108, 14807–14810. hod2004.pdf
Kallush, S. ; Band, Y. B. ; Baer, R. Rotational Aspects of short-pulse population transfer in diatomic molecules. Chem. Phys. Lett. 2004, 392, 23.Abstract

A fully-selective population transfer scheme for diatomic molecules using short-duration (

Jacobi, S. ; Baer, R. The well-tempered auxiliary-field Monte Carlo. The Journal of chemical physics 2004, 120, 43–50.Abstract

The auxiliary-field Monte Carlo (AFMC) is a method for computing ground-state and excited-state energies and other properties of electrons in molecules. For a given basis set, AFMC is an approximation to full-configuration interaction and the accuracy is determined predominantly by an inverse temperature "\beta" parameter. A considerable amount of the dynamical correlation energy is recovered even at small values of \beta. Yet, nondynamical correlation energy is inefficiently treated by AFMC. This is because the statistical error grows with \beta, warranting increasing amount of Monte Carlo sampling. A recently introduced multideterminant variant of AFMC is studied, and the method can be tuned by balancing the sizes of the determinantal space and the \beta parameter with respect to a predefined target accuracy. The well tempered AFMC is considerably more efficient than a naive AFMC. We demonstrate the principles on dissociating hydrogen molecule and torsion of ethylene where we calculate the (unoptimized) torsional barrier and the vertical singlet-triplet

Collepardo-Guevara, R. ; Walter, D. ; Neuhauser, D. ; Baer, R. A Hückel study of the effect of a molecular resonance cavity on the quantum conductance of an alkene wire. Chem. Phys. Lett. 2004, 393, 367–371.Abstract

{We use Huckel theory to examine interference effects on conductance of a wire when a ‘lollypop’ side-chain is bonded to it, acting as a resonance cavity. A clear signature of interference is found at these ballistic conducting systems, stronger in small systems. Gating effects are enhanced by the presence of the loop, where the electronic wavefunctions can experience large changes in phase. Using an ‘interference index’

Baer, R. ; Seideman, T. ; Ilani, S. ; Neuhauser, D. Ab initio study of the alternating current impedance of a molecular junction. J. Chem. Phys. 2004, 120, 3387–3396.Abstract

The small-bias conductance of the C-6 molecule, stretched between two metallic leads, is studied using time-dependent density functional theory within the adiabatic local density approximation. The leads are modeled by jellium slabs, the electronic density and the current density are described on a grid, whereas the core electrons and the highly oscillating valence orbitals are approximated using standard norm-conserving pseudopotentials. The jellium leads are supplemented by a complex absorbing potential that serves to absorb charge reaching the edge of the electrodes and hence mimic irreversible flow into the macroscopic metal. The system is rapidly exposed to a ramp potential directed along the C-6 axis, which gives rise to the onset of charge and current oscillations. As time progresses, a fast redistribution of the molecular charge is observed, which translates into a direct current response. Accompanying the dc signal, alternating current fluctuations of charge and currents within the molecule and the metallic leads are observed. These form the complex impedance of the molecule and are especially strong at the plasmon frequency of the leads and the lowest excitation peak of C-6. We study the molecular conductance in two limits: the strong coupling limit, where the edge atoms of the chain are submerged in the jellium and the weak coupling case, where the carbon atoms and the leads do not overlap spatially. (C) 2004 American Institute of Physics.

Baer, R. ; Neuhauser, D. ; Weiss, S. Enhanced absorption induced by a metallic nanoshell. Nano Lett. 2004, 4 85–88.Abstract

Nanoshells have been previously shown to have tunable absorption frequencies that are dependent on the ratio of their inner and outer radii. Inspired by this, we ask: can a nanoshell increase the absorption of a small core system embedded within it? A theoretical model is constructed to answer this question. A core, composed of a “jellium” ball of the density of gold is embedded within a jellium nanoshell of nanometric diameter. The shell plasmon frequency is tuned to the core absorption line. A calculation based the time-dependent density functional theory was performed showing a 10 fold increase in core excitation yield.

Baer, R. ; Neuhauser, D. Real-time linear response for time-dependent density-functional theory. J. Chem. Phys. 2004, 121, 9803–9807.Abstract

We present a linear-response approach for time-dependent density-functional theories using time-adiabatic functionals. The resulting theory can be performed both in the time and in the frequency domain. The derivation considers an impulsive perturbation after which the Kohn-Sham orbitals develop in time autonomously. The equation describing the evolution is not strictly linear in the wave function representation. Only after going into a symplectic real-spinor representation does the linearity make itself explicit. For performing the numerical integration of the resulting equations, yielding the linear response in time, we develop a modified Chebyshev expansion approach. The frequency domain is easily accessible as well by changing the coefficients of the Chebyshev polynomial, yielding the expansion of a formal symplectic Green's operator. (C) 2004 American Institute of Physics.

Baer, R. ; Siam, N. Real-time study of the adiabatic energy loss in an atomic collision with a metal cluster. The Journal of chemical physics 2004, 121, 6341–6345. baer2004d.pdf
Saravanan, C. ; Shao, Y. ; Baer, R. ; Ross, P. N. ; Head–Gordon, M. Sparse matrix multiplications for linear scaling electronic structure calculations in an atom-centered basis set using multiatom blocks. J. Comput. Chem. 2003, 24, 618–622. saravanan2003sparse.pdf
Lüchow, A. ; Neuhauser, D. ; Ka, J. ; Baer, R. ; Chen, J. ; Mandelshtam, V. A. Computing energy levels by inversion of imaginary-time cross-correlation functions. J. Phys. Chem. A 2003, 107, 7175–7180. luchow2003computing.pdf
Liu, C. ; Walter, D. ; Neuhauser, D. ; Baer, R. Molecular recognition and conductance in crown ethers. J. Am. Chem. Soc. 2003, 125, 13936–13937. liu2003.pdf
Neuhauser, D. ; Baer, R. ; Kosloff, R. Quantum soliton dynamics in vibrational chains: Comparison of fully correlated, mean field, and classical dynamics. J. Chem. Phys. 2003, 118, 5729–5735.Abstract

The dynamics of a chain of vibrational bonds which develop a classical solitary compression wave is simulated. A converged fully correlated quantum mechanical calculation is compared with a time dependent mean field approach (TDSCF) and with a classical simulation. The dynamics were all generated from the same Hamiltonian. The TDSCF and classical calculations show a fully developed solitary wave with the expected dependence of group velocity on amplitude. The full quantum calculations show a solitary-like wave which propagates for a while but then degrades. The robustness of the compression wave depends on the initial preparation. Evidence of partial recurrence of the wave has also been observed. (C) 2003 American Institute of Physics.

Neuhauser, D. ; Baer, R. A two-grid time-dependent formalism for the Maxwell equation. Journal of Theoretical & Computational Chemistry 2003, 2 537–546. neuhauser2003.pdf
Hod, O. ; Rabani, E. ; Baer, R. Carbon nanotube closed-ring structures. Phys. Rev. B 2003, 67, 195408.Abstract

We study the structure and stability of closed-ring carbon nanotubes using a theoretical model based on the Brenner-Tersoff potential. Many metastable structures can be produced. We focus on two methods of generating such structures. In the first, a ring is formed by geometric folding and is then relaxed into minimum energy using a minimizing algorithm. Short tubes do not stay closed. Yet tubes longer than 18 nm are kinetically stable. The other method starts from a straight carbon nanotube and folds it adiabatically into a closed-ring structure. The two methods give strikingly different structures. The structures of the second method are more stable and exhibit two buckles, independent of the nanotube length. This result is in strict contradiction to an elastic shell model. We analyze the results for the failure of the elastic model.

Baer, R. ; Neuhauser, D. Ab initio electrical conductance of a molecular wire. Int. J. Quantum Chem. 2003, 91, 524–532. baer2003c.pdf
Baer, R. ; Neuhauser, D. ; Zdanska, P. ; Moiseyev, N. Ionization and high-harmonic generation in aligned benzene by intense circularly polarized light. Phys. Rev. A 2003, 68, 043406. baer2003e.pdf