Characterizing a configuration interaction excited state using natural transition geminals

We introduce natural transition geminals as a means to qualitatively understand a transition where double excitations are important. The first two $A_{1}$ singlet states of the CH cation are used as an initial example. We calculate these states with configuration interaction singles (CIS) and state-averaged Monte Carlo configuration interaction (SA-MCCI). For each method we compare the important natural transition geminals with the dominant natural transition orbitals. We then compare SA-MCCI and full configuration interaction (FCI) with regards to the natural transition geminals using the beryllium atom. We compare using the natural transition geminals with analyzing the important configurations in the CI expansion to give the dominant transition for the beryllium atom and the carbon dimer. Finally we calculate the natural transition geminals for two electronic excitations of formamide.Comment: 15 pages, 2 figures. Mol. Phys. (2013

Approaching exact hyperpolarizabilities via sum-over-states Monte Carlo configuration interaction

We propose using sum-over-states calculations with the compact wavefunctions of Monte Carlo configuration interaction to approach accurate values for higher-order dipole properties up to second hyperpolarizabilities in a controlled way. We apply the approach to small systems that can generally be compared with full configuration interaction (FCI) results. We consider hydrogen fluoride with a 6-31g basis and then look at results, including frequency dependent properties, in an aug-cc-pVDZ basis. We extend one calculation beyond FCI by using an aug-cc-pVTZ basis. The properties of an H$_{4}$ molecule with multireference character are calculated in an aug-cc-pVDZ basis. We then investigate this method on a strongly multireference system with a larger FCI space by modelling the properties of carbon monoxide with a stretched geometry. The behavior of the approach with increasing basis size is considered by calculating results for the neon atom using aug-cc-pVDZ to aug-cc-pVQZ. We finally test if the unusual change in polarizability between the first two states of molecular oxygen can be reproduced by this method in a 6-31g basis.Comment: 11 pages, 14 figure

Machine Learning Configuration Interaction

We propose the concept of machine learning configuration interaction (MLCI) whereby an artificial neural network is trained on-the-fly to predict important new configurations in an iterative selected configuration interaction procedure. We demonstrate that the neural network can discriminate between important and unimportant configurations, that it has not been trained on, much better than by chance. MLCI is then used to find compact wavefunctions for carbon monoxide at both stretched and equilibrium geometries. We also consider the multireference problem of the water molecule with elongated bonds. Results are contrasted with those from other ways of selecting configurations: first-order perturbation, random selection and Monte Carlo configuration interaction. Compared with these other serial calculations, this prototype MLCI is competitive in its accuracy, converges in significantly fewer iterations than the stochastic approaches, and requires less time for the higher-accuracy computations.Comment: This document is the unedited Author's version of a Submitted Work that was subsequently accepted for publication in The Journal of Chemical Theory and Computation, copyright American Chemical Society after peer review. To access the final edited and published work see https://pubs.acs.org/articlesonrequest/AOR-dANIFXJKzRAyR99E6hb

Applying Monte Carlo configuration interaction to transition metal dimers: exploring the balance between static and dynamic correlation

We calculate potential curves for transition metal dimers using Monte Carlo configuration interaction (MCCI). These results, and their associated spectroscopic values, are compared with experimental and computational studies. The multireference nature of the MCCI wavefunction is quantified and we estimate the important orbitals. We initially consider the ground state of the chromium dimer. Next we calculate potential curves for Sc$_{2}$ where we contrast the lowest triplet and quintet states. We look at the molybdenum dimer where we compare non-relativistic results with the partial inclusion of relativistic effects via effective core potentials, and report results for scandium nickel.Comment: 9 pages and 8 figure

Effects of wing leading-edge deflection on low-speed aerodynamic characteristics of a low-aspect-ratio highly swept arrow-wing configuration

Static force tests were conducted in the Langley V/STOL tunnel at a Reynolds number (based on the mean aerodynamic chord) of about 2.0 x 10 to the 6th power for an angle-of-attack range from about - 10 deg to 17 deg and angles of sideslip of 0 and + or - 5 deg. Limited flow visualization studies were also conducted in order to provide a qualitative assessment of leading-edge upwash characteristics

Results of recent NASA research on low-speed aerodynamic characteristics of supersonic cruise aircraft

The relatively low values of lift-curve slope produced by highly swept arrow wings, coupled with the low scrape angle of the fuselage, resulted in relatively low values of take-off and approach lift coefficients. Through the use of more efficient high-lift systems and the application of propulsive-lift concepts, it is possible to optimize the engine-airframe design for maximum range potential and also to provide good low-speed performance. Nose strakes provide significant improvements in directional stability characteristics and the use of a propulsive lateral control system provides a solution to problems associated with inherently low levels of lateral control

Monte Carlo configuration interaction applied to multipole moments, ionisation energies and electron affinities

The method of Monte Carlo configuration interaction (MCCI) [1,2] is applied to the calculation of multipole moments. We look at the ground and excited state dipole moments in carbon monoxide. We then consider the dipole of NO, the quadrupole of the nitrogen molecule and of BH. An octupole of methane is also calculated. We consider experimental geometries and also stretched bonds. We show that these non-variational quantities may be found to relatively good accuracy when compared with FCI results, yet using only a small fraction of the full configuration interaction space. MCCI results in the aug-cc-pVDZ basis are seen to generally have reasonably good agreement with experiment. We also investigate the performance of MCCI when applied to ionisation energies and electron affinities of atoms in an aug-cc-pVQZ basis. We compare the MCCI results with full configuration-interaction quantum Monte Carlo [3,4] and `exact' non-relativistic results [3,4]. We show that MCCI could be a useful alternative for the calculation of atomic ionisation energies however electron affinities appear much more challenging for MCCI. Due to the small magnitude of the electron affinities their percentage errors can be high, but with regards to absolute errors MCCI performs similarly for ionisation energies and electron affinities.Comment: 12 pages, 20 figure

Population Dynamics in the Penna Model

We build upon the recent steady-state Penna model solution, Phys.Rev.Lett. 89, 288103 (2002), to study the population dynamics within the Penna model. We show, that any perturbation to the population can be broken into a collection of modes each of which decay exponentially with its respective time constant. The long time behaviour of population is therefore likely to be dominated by the modes with the largest time constants. We confirm our analytical approach with simulation data.Comment: 6 figure

The X-ray Transient XTE J2012+381

We present optical and infrared observations of the soft X-ray transient (SXT) XTE J2012+381 and identify the optical counterpart with a faint red star heavily blended with a brighter foreground star. The fainter star is coincident with the radio counterpart and appears to show weak H alpha emission and to have faded between observations. The RXTE/ASM lightcurve of XTE J2012+381 is unusual for an SXT in that after an extended linear decay, it settled into a plateau state for about 40 days before undergoing a weak mini-outburst. We discuss the nature of the object and suggest similarities to long orbital period SXTs.Comment: 5 pages, 7 postscript figures included, uses mn.sty. Accepted for publication in MNRA