Nicolas Poilvert

Wavelet Scattering Regression of Quantum Chemical Energies

We introduce multiscale invariant dictionaries to estimate quantum chemical energies of organic molecules, from training databases. Molecular energies are invariant to isometric atomic displacements, and are Lipschitz continuous to molecular deformations. Similarly to density functional theory (DFT), the molecule is represented by an electronic density function. A multiscale invariant dictionary is calculated with wavelet scattering invariants. It cascades a first wavelet transform which separates scales, with a second wavelet transform which computes interactions across scales. Sparse scattering regressions give state of the art results over two databases of organic planar molecules. On these databases, the regression error is of the order of the error produced by DFT codes, but at a fraction of the computational cost.

Automated quantum conductance calculations using maximally-localised Wannier functions

A robust, user-friendly, and automated method to determine quantum conductance in quasi-one-dimensional systems is presented. The scheme relies upon an initial density-functional theory calculation in a specific geometry after which the ground-state eigenfunctions are transformed to a maximally-localised Wannier function (MLWF) basis. In this basis, our novel algorithms manipulate and partition the Hamiltonian for the calculation of coherent electronic transport properties within the Landauer-Buttiker formalism. Furthermore, we describe how short-ranged Hamiltonians in the MLWF basis can be combined to build model Hamiltonians of large (>10,000 atom) disordered systems without loss of accuracy. These automated algorithms have been implemented in the Wannier90 code (Mostofi et al., 2008) [1], which is interfaced to a number of electronic structure codes such as Quantum-ESPRESSO, Ablnit, Wien2k, SIESTA and FLEUR. We apply our methods to an Al atomic chain with a Na defect, an axially heterostructured Si/Ge nanowire and to a spin-polarised defect on a zigzag graphene nanoribbon

Switchable conductance in functionalized carbon nanotubes via reversible sidewall bond cleavage

We propose several covalent functionalizations for carbon nanotubes that display switchable on/off conductance in metallic tubes. The switching action is achieved by reversible control of bond-cleavage chemistry in [1 + 2] cycloadditions via the sp(3) ⇌ sp(2) rehybridization that it induces; this leads to remarkable changes of conductance even at very low degrees of functionalization. Reversible bond-cleavage chemistry is achieved by identifying addends that provide optimal compensation between the bond-preserving through-space π orbital interactions with the tube against the bond-breaking strain energy of the cyclopropane moiety. Several strategies for real-time control, based on redox or hydrolysis reactions, cis-trans isomerization or excited-state proton transfer are proposed. Such designer functional groups would allow for the first time direct control of the electrical properties of metallic carbon nanotubes, with extensive applications in nanoscale devices.

A silicon microwire under a three-dimensional anisotropic tensile stress

Three-dimensional tensile stress, or triaxial tensile stress, is difficult to achieve in a material. We present the investigation of an unusual three-dimensional anisotropic tensile stress field and its influence on the electronic properties of a single crystal silicon microwire. The microwire was created by laser heating an amorphous silicon wire deposited in a 1.7 μm silica glass capillary by high pressure chemical vapor deposition. Tensile strain arises due to the thermal expansion mismatch between silicon and silica. Synchrotron X-ray micro-beam Laue diffraction (μ-Laue) microscopy reveals that the three principal strain components are +0.47% (corresponding to a tensile stress of +0.7 GPa) along the fiber axis and nearly isotropic +0.02% (corresponding to a tensile stress of +0.3 GPa) in the cross-sectional plane. This effect was accompanied with a reduction of 30 meV in the band gap energy of silicon, as predicted by the density-functional theory calculations and in close agreement with energy-depend...