A simplified picture for Pi electrons in conjugated polymers : from PPP Hamiltonian to an effective molecular crystal approach

An excitonic method proper to study conjugated oligomers and polymers is described and its applicability tested on the ground state and first excited states of trans-polyacetylene, taken as a model. From the Pariser-Parr-Pople Hamiltonian, we derive an effective Hamiltonian based on a local description of the polymer in term of monomers; the relevant electronic configurations are build on a small number of pertinent local excitations. The intuitive and simple microscopic physical picture given by our model supplement recent results, such as the Rice and Garstein ones. Depending of the parameters, the linear absorption appears dominated by an intense excitonic peak.Comment: 41 Pages, 6 postscript figure

Evidence for Excimer Photoexcitations in an Ordered {\pi}-Conjugated Polymer Film

We report pressure-dependent transient picosecond and continuous-wave photomodulation studies of disordered and ordered films of 2-methoxy-5-(2-ethylhexyloxy) poly(para-phenylenevinylene). Photoinduced absorption (PA) bands in the disordered film exhibit very weak pressure dependence and are assigned to intrachain excitons and polarons. In contrast, the ordered film exhibits two additional transient PA bands in the midinfrared that blueshift dramatically with pressure. Based on high-order configuration interaction calculations we ascribe the PA bands in the ordered film to excimers. Our work brings insight to the exciton binding energy in ordered films versus disordered films and solutions. The reduced exciton binding energy in ordered films is due to new energy states appearing below the continuum band threshold of the single strand.Comment: 5.5 pages, 5 figure

Quantifying the contribution of pathways of nosocomial acquisition of COVID-19 in English hospitals

BACKGROUND: Despite evidence of the nosocomial transmission of novel coronavirus Severe Acute Respiratory Syndrome Coronavirus 2 (SARS-CoV-2) in hospitals worldwide, the contributions of the pathways of transmission are poorly quantified. METHODS: We analysed national records of hospital admissions and discharges, linked to data on SARS-CoV-2 testing, using an individual-based model that considers patient-to-patient, patient-to-healthcare worker (HCW), HCW-to-patient and HCW-to-HCW transmission. RESULTS: Between 1 March 2020 and 31 December 2020, SARS-CoV-2 infections that were classified as nosocomial were identified in 0.5% (0.34-0.74) of patients admitted to an acute National Health Service trust. We found that the most likely route of nosocomial transmission to patients was indirect transmission from other infected patients, e.g. through HCWs acting as vectors or contaminated fomites, followed by direct transmission between patients in the same bay. The risk of transmission to patients from HCWs over this time period is low, but can contribute significantly when the number of infected inpatients is low. Further, the risk of a HCW acquiring SARS-CoV-2 in hospital is approximately equal to that in the community, thereby doubling their overall risk of infection. The most likely route of transmission to HCWs is transmission from other infected HCWs. CONCLUSIONS: Current control strategies have successfully reduced the transmission of SARS-CoV-2 between patients and HCWs. In order to reduce the burden of nosocomial COVID-19 infections on health services, stricter measures should be enforced that would inhibit the spread of the virus between bays or wards in the hospital. There should also be a focus on inhibiting the spread of SARS-CoV-2 between HCWs. The findings have important implications for infection-control procedures in hospitals

Molecular crystal approach for pi-conjugated polymers: from PPP Hamiltonian to Holstein model for polaron states

Starting from the $\pi$-electron Pariser-Parr-Pople (PPP) Hamiltonian which includes both strong electron-phonon and electron-electron interactions, we propose some strongly correlated wave functions of increasing quality for the ground state of conjugated polymers. These wavefunctions are built by combining different finite sets of local configurations extended at most over two nearest-neighbour monomers. With this picture, the doped case with one additional particle is expressed in terms of quasi-particle. Thus, the polaron formation problem goes back to the study of a Holstein like model.Comment: 27 pages, 6 eps figs, Revtex; enlarged version. Submitted to Journal of Physics: Condensed Matte

Symmetry breaking and the random-phase approximation in small quantum dots

The random-phase approximation has been used to compute the properties of parabolic two-dimensional quantum dots beyond the mean-field approximation. Special emphasis is put on the ground state correlation energy, the symmetry restoration and the role of the spurious modes within the random-phase approximation. A systematics with the Coulombic interaction strength is presented for the 2-electron dot, while for the 6- and 12-electron dots selected cases are discussed. The validity of the random-phase approximation is assessed by comparison with available exact results.Comment: 9 pages, 4 embedded + 6 gif Figs. Published versio

Spin states of zigzag-edged Mobius graphene nanoribbons from first principles

Mobius graphene nanoribbons have only one edge topologically. How the magnetic structures, previously associated with the two edges of zigzag-edged flat nanoribbons or cyclic nanorings, would change for their Mobius counterparts is an intriguing question. Using spin-polarized density functional theory, we shed light on this question. We examine spin states of zigzag-edged Mobius graphene nanoribbons (ZMGNRs) with different widths and lengths. We find a triplet ground state for a Mobius cyclacene, while the corresponding two-edged cyclacene has an open-shell singlet ground state. For wider ZMGNRs, the total magnetization of the ground state is found to increase with the ribbon length. For example, a quintet ground state is found for a ZMGNR. Local magnetic moments on the edge carbon atoms form domains of majority and minor spins along the edge. Spins at the domain boundaries are found to be frustrated. Our findings show that the Mobius topology (i.e., only one edge) causes ZMGNRs to favor one spin over the other, leading to a ground state with non-zero total magnetization.Comment: 17 pages, 4 figure

Excited States of Ladder-type Poly-p-phenylene Oligomers

Ground state properties and excited states of ladder-type paraphenylene oligomers are calculated applying semiempirical methods for up to eleven phenylene rings. The results are in qualitative agreement with experimental data. A new scheme to interpret the excited states is developed which reveals the excitonic nature of the excited states. The electron-hole pair of the S1-state has a mean distance of approximately 4 Angstroem.Comment: 24 pages, 21 figure

Excited states of linear polyenes

We present density matrix renormalisation group calculations of the Pariser- Parr-Pople-Peierls model of linear polyenes within the adiabatic approximation. We calculate the vertical and relaxed transition energies, and relaxed geometries for various excitations on long chains. The triplet (3Bu+) and even- parity singlet (2Ag+) states have a 2-soliton and 4-soliton form, respectively, both with large relaxation energies. The dipole-allowed (1Bu-) state forms an exciton-polaron and has a very small relaxation energy. The relaxed energy of the 2Ag+ state lies below that of the 1Bu- state. We observe an attraction between the soliton-antisoliton pairs in the 2Ag+ state. The calculated excitation energies agree well with the observed values for polyene oligomers; the agreement with polyacetylene thin films is less good, and we comment on the possible sources of the discrepencies. The photoinduced absorption is interpreted. The spin-spin correlation function shows that the unpaired spins coincide with the geometrical soliton positions. We study the roles of electron-electron interactions and electron-lattice coupling in determining the excitation energies and soliton structures. The electronic interactions play the key role in determining the ground state dimerisation and the excited state transition energies.Comment: LaTeX, 15 pages, 9 figure

Formation and control of electron molecules in artificial atoms: Impurity and magnetic-field effects

Interelectron interactions and correlations in quantum dots can lead to spontaneous symmetry breaking of the self-consistent mean field resulting in formation of Wigner molecules. With the use of spin-and-space unrestricted Hartree-Fock (sS-UHF) calculations, such symmetry breaking is discussed for field-free conditions, as well as under the influence of an external magnetic field. Using as paradigms impurity-doped (as well as the limiting case of clean) two-electron quantum dots (which are analogs to helium-like atoms), it is shown that the interplay between the interelectron repulsion and the electronic zero-point kinetic energy leads, for a broad range of impurity parameters, to formation of a singlet ground-state electron molecule, reminiscent of the molecular picture of doubly-excited helium. Comparative analysis of the conditional probability distributions for the sS-UHF and the exact solutions for the ground state of two interacting electrons in a clean parabolic quantum dot reveals that both of them describe formation of an electron molecule with similar characteristics. The self-consistent field associated with the triplet excited state of the two-electron quantum dot (clean as well as impurity-doped) exhibits symmetry breaking of the Jahn-Teller type, similar to that underlying formation of nonspherical open-shell nuclei and metal clusters. Furthermore, impurity and/or magnetic-field effects can be used to achieve controlled manipulation of the formation and pinning of the discrete orientations of the Wigner molecules. Impurity effects are futher illustrated for the case of a quantum dot with more than two electrons.Comment: Latex/Revtex, 10 pages with 4 gif figures. Small changes to explain the difference between Wigner and Jahn-Teller electron molecules. A complete version of the paper with high quality figures inside the text is available at http://shale.physics.gatech.edu/~costas/qdhelium.html For related papers, see http://www.prism.gatech.edu/~ph274c