Biomedical subjects

Robin Santra

Publications and source records attributed to Robin Santra.

10 recordsLinked to original sources

PubMed2006

Role of many-electron dynamics in high harmonic generation.

High harmonic generation (HHG) in many-electron atoms is studied theoretically. The breakdown of the frozen-core single active electron approximation is demonstrated, as it predicts roughly the same radiation amplitude in all noble gases. This is in contradiction with experiments, where heavier noble gases are known to emit much stronger HHG radiation than lighter ones. This experimental behavior of the noble gases can be qualitatively reproduced when many-electron dynamics, within a simple approximation, is taken into account.

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PubMed2006

Three-step model for high-harmonic generation in many-electron systems.

The three-step model (TSM) of high-harmonic generation (HHG) is generalized to atomic and molecular many-electron systems. Using many-body perturbation theory, corrections to the standard TSM due to exchange and electron-electron correlations are derived. It is shown that canonical Hartree-Fock orbitals represent the most appropriate set of one-electron states for calculating the HHG spectrum. To zeroth order in many-body perturbation theory, a HHG experiment allows direct access, in general, to a combination of occupied Hartree-Fock orbitals rather than to the highest occupied molecular orbital by itself.

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PubMed2005

Ab initio configuration-interaction investigation of optical transitions in K+He and K+H2.

The potassium resonance line (4s-->4p) centered around 770 nm is a major contributor to the optical extinction in the atmospheres of certain classes of brown dwarfs and extrasolar giant planets. The resonance line is significantly broadened by collisions with He and H2, and an accurate calculation of the line profile is needed for astrophysical models of these objects. As a first step, we report an accurate ab initio study of the K+He and K+H2 potential-energy curves correlating to the K 4s and 4p atomic energy levels, together with the dipole moments governing the transitions between these potential-energy curves. The molecular calculations have been carried out using a multireference configuration-interaction method, with the molecular orbitals expanded in a large Gaussian basis set. The transition dipole moments show significant variation with the molecular geometry. Calculations for the K+H2 system have been carried out for a range of H2 orientations and internuclear separations, so that the effect of H2 rotation and vibration may be explicitly included in future calculations of the pressure-broadened line profiles.

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PubMed2005

Correlated complex independent particle potential for calculating electronic resonances.

We have formulated and applied an analytic continuation method for the recently formulated correlated independent particle potential [A. Beste and R. J. Bartlett J. Chem. Phys. 120, 8395 (2004)] derived from Fock space multireference coupled cluster theory. The technique developed is an advanced ab initio tool for calculating the properties of resonances in the low-energy electron-molecule collision problem. The proposed method quantitatively describes elastic electron-molecule scattering below the first electronically inelastic threshold. A complex absorbing potential is utilized to define the analytic continuation for the potential. A separate treatment of electron correlation and relaxation effects for the projectile-target system and the analytic continuation using the complex absorbing potential is possible, when an approximated form of the correlated complex independent particle potential is used. The method, which is referred to as complex absorbing potential-based correlated independent particle (CAP-CIP), is tested by application to the well-known (2)Pi(g) shape resonance of e-N(2) and the (2)B(2g) shape resonance of e-C(2)H(4) (ethylene) with highly satisfactory results.

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PubMed2005

Calculating molecular Rydberg states using the one-particle Green's function: application to HCO and C(NH2)3.

A simple but accurate and computationally efficient method for routine ab initio calculations of molecular Rydberg states is described. The method, which can be applied to Rydberg states associated with a nondegenerate ion core, consists in the self-consistent solution of an effective one-electron problem. First, the restricted Hartree-Fock problem of the ion core is solved. The orbital energies and certain two-electron Coulomb matrix elements with respect to the molecular orbital basis are then used to construct an energy-dependent many-body correction to the Hartree-Fock mean field. This correction is derived from the Dyson equation satisfied by the one-particle Green's function. The method is applied to calculate Rydberg potential-energy curves of HCO. The presented data confirm and extend recent large-scale multireference configuration-interaction calculations and help develop a detailed theoretical description of the astrophysically important dissociative recombination of a low-energy electron with HCO(+). As further illustration of the utility of the method, the first ab initio calculations of the excited states of an electron bound to the guanidinium cation [C(NH(2))(3)](+) are reported.

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PubMed2005

Analytically continued Fock space multireference coupled-cluster theory: application to the 2Pi(g) shape resonance in e-N2 scattering.

The technique of Fock space multireference coupled-cluster (FSMRCC) is applied for the first time to the correlated calculation of the energy and width of a shape resonance in an electron-molecule collision. The procedure is based upon combining a complex absorbing potential with FSMRCC theory. Accurate resonance parameters are obtained by solving a small non-Hermitian eigenvalue problem. The potential-energy curve of the (2)Pi(g) state of N2- is calculated using the FSMRCC and multireference configuration-interaction (MRCI) level of theories. Comparison with the single-determinant Hartree-Fock theory indicates that correlation effects are important in determining the behavior of the resonance state.

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PubMed2005

High-accuracy optical clock via three-level coherence in neutral bosonic 88Sr.

An optical atomic clock scheme is proposed that utilizes two lasers to establish coherent coupling between the 5s2 1S0 ground state of 88Sr and the first excited state, 5s5p 3P0. The coupling is mediated by the broad 5s5p 1P1 state, exploiting the phenomenon of electromagnetically induced transparency. The effective linewidth of the clock transition can be chosen at will by adjusting the laser intensity. By trapping the 88Sr atoms in an optical lattice, long interaction times with the two lasers are ensured; Doppler and recoil effects are eliminated. Based on a careful analysis of systematic errors, a clock accuracy of better than 2 x 10(-17) is expected.

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PubMed2003

Xenon clusters in intense VUV laser fields.

A simple model is developed that quantitatively describes intense interactions of a vacuum ultraviolet (VUV) laser pulse with a xenon cluster. We find good agreement with a recent experiment [Nature (London) 420, 482 (2002)]]. In particular, the large number of VUV photons absorbed per atom, at intensities significantly below 10(16) W/cm(2), is now understood.

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PubMed2003

Multichannel cold collisions between metastable Sr atoms.

We present a multichannel-scattering calculation of elastic and inelastic cold collisions between two low-field seeking, metastable 88Sr [(5s5p)3P2] atoms in the presence of an external magnetic field. The scattering physics is governed by strong anisotropic long-range interactions, which lead to pronounced coupling among the partial waves of relative motion. As a result, nonadiabatic transitions are shown to trigger a high rate of inelastic losses. At relatively high energies, T>100 microK, the total inelastic collision rate is comparable with the elastic rate. However, at lower collisional energy, the elastic rate decreases, and at T approximately 1 microK, it becomes substantially smaller than the inelastic rate. Our study suggests that magnetic trapping and evaporative cooling of 88Sr [(5s5p)3P2] atoms, as well as 40Ca [(4s4p)3P2], in low-field seeking states will prove difficult to achieve experimentally.

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PubMed2003

Coulombic energy transfer and triple ionization in clusters.

Using neon and its dimer as a specific example, it is shown that excited Auger decay channels that are electronically stable in the isolated monomer can relax in a cluster by electron emission. The decay mechanism, leading to the formation of a tricationic cluster, is based on an efficient energy-transfer process from the excited, dicationic monomer to a neighbor. The decay is ultrafast and expected to be relevant to numerous physical phenomena involving core holes in clusters and other forms of spatially extended atomic and molecular matter.

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