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Rui-Hua Xie

Publications and source records attributed to Rui-Hua Xie.

12 recordsLinked to original sources
arXiv2007

Theoretical analysis of dynamic chemical imaging with lasers using high-order harmonic generation

We report theoretical investigations of the tomographic procedure suggested by Itatani {\it et al.} [Nature, {\bf 432} 867 (2004)] for reconstructing highest occupied molecular orbitals (HOMO) using high-order harmonic generation (HHG). Using the limited range of harmonics from the plateau region, we found that under the most favorable assumptions, it is still very difficult to obtain accurate HOMO wavefunction, but the symmetry of the HOMO and the internuclear separation between the atoms can be accurately extracted, especially when lasers of longer wavelengths are used to generate the HHG. We also considered the possible removal or relaxation of the approximations used in the tomographic method in actual applications. We suggest that for chemical imaging, in the future it is better to use an iterative method to locate the positions of atoms in the molecule such that the resulting HHG best fits the macroscopic HHG data, rather than by the tomographic method.

physics.atom-ph↗
arXiv2005

A Simple Three-Parameter Model Potential For Diatomic Systems: From Weakly and Strongly Bound Molecules to Metastable Molecular Ions

Based on a simplest molecular orbital theory of H$_{2}^{+}$, a three-parameter model potential function is proposed to describe ground-state diatomic systems with closed-shell and/or S-type valence-shell constituents over a significantly wide range of internuclear distances. More than 200 weakly and strongly bound diatomics have been studied, including neutral and singly-charged diatomics (e.g., H$_{2}$, Li$_{2}$, LiH, Cd$_{2}$, Na$_{2}^{+}$, and RbH$^{-}$), long-range bound diatomics (e.g., NaAr, CdNe, He$_{2}$, CaHe, SrHe, and BaHe), metastable molecular dications (e.g., BeH$^{++}$, AlH$^{++}$, Mg$_{2}^{++}$, and LiBa$^{++}$), and molecular trications (e.g., YHe$^{+++}$ and ScHe$^{+++}$).

physics.chem-ph↗
arXiv2005

The Excitation of Extended Red Emission: New Constraints on its Carrier From HST Observations of NGC 7023

The carrier of the dust-associated photoluminescence process causing the extended red emission (ERE) in many dusty interstellar environments remains unidentified. Several competing models are more or less able to match the observed broad, unstructured ERE band. We now constrain the character of the ERE carrier further by determining the wavelengths of the radiation that initiates the ERE. Using the imaging capabilities of the Hubble Space Telescope, we have resolved the width of narrow ERE filaments appearing on the surfaces of externally illuminated molecular clouds in the bright reflection nebula NGC 7023 and compared them with the depth of penetration of radiation of known wavelengths into the same cloud surfaces. We identify photons with wavelengths shortward of 118 nm as the source of ERE initiation, not to be confused with ERE excitation, however. There are strong indications from the well-studied ERE in the Red Rectangle nebula and in the high-|b| Galactic cirrus that the photon flux with wavelengths shortward of 118 nm is too small to actually excite the observed ERE, even with 100% quantum efficiency. We conclude, therefore, that ERE excitation results from a two-step process. While none of the previously proposed ERE models can match these new constraints, we note that under interstellar conditions most polycyclic aromatic hydrocarbon (PAH) molecules are ionized to the di-cation stage by photons with E > 10.5 eV and that the electronic energy level structure of PAH di-cations is consistent with fluorescence in the wavelength band of the ERE. Therefore, PAH di-cations deserve further study as potential carriers of the ERE. (abridged)

astro-ph↗
arXiv2003

Tailorable acceptor ${\rm C}_{60-n}{\rm B}_{n}$ and donor ${\rm C}_{60-m}{\rm N}_{m}$ pairs for molecular electronics

Our first-principles calculations demonstrate that ${\rm C}_{60-n}{\rm B}_{n}$ and ${\rm C}_{60-m}{\rm N}_{m}$ molecules can be engineered as the acceptors and donors, respectively, which are needed for molecular electronics, by properly controlling the number $n$ and $m$ of the substitutional dopants in ${\rm C}_{60}$. As an example, we show that acceptor ${\rm C}_{48}{\rm B}_{12}$ and donor ${\rm C}_{48}{\rm N}_{12}$ are promising components for molecular rectifiers, carbon nanotube-based $p$-type, $n$-type, $n$-$p$-$n$ and $p$-$n$-$p$ transistors and $p$-$n$ junctions.

cond-mat.mtrl-sci↗
arXiv2003

Structural, electronic and magnetic properties of heterofullerenes C48B12

Bonding, electric (hyper)polarizability, vibrational and magnetic properties of heterofullerene ${\rm C}_{48}{\rm B}_{12}$ are studied by first-principles calculations. Infrared- and Raman-active vibrational frequencies of ${\rm C}_{48}{\rm B}_{12}$ are assigned. Eight $^{13}$C and 2 $^{11}$B NMR spectral signals of ${\rm C}_{48}{\rm B}_{12}$ are characterized. The first-order hyperpolarizability in ${\rm C}_{48}{\rm B}_{12}$ is zero because of the inversion symmetry. The average second-order hyperpolarizability of ${\rm C}_{48}{\rm B}_{12}$ is about 180% larger than that of ${\rm C}_{60}$. Our results suggest that ${\rm C}_{48}{\rm B}_{12}$ is also a candidate for photonic and optical limiting applications because of the enhanced third-order optical nonlinearities.

cond-mat.mtrl-sci↗
arXiv2003

Generation of dipole squeezing in a two-mode system with entangled coherent states of a quantized electromagnetic field

Two-mode quantized electromagnetic fields can be entangled and admit a large number of coherent states. In this paper, we consider a two-mode system that consists of a two-level atom interacting with a two-mode quantized electromagnetic field, which is initially prepared in an entangled two-mode coherent state, via a nondegenerate two-photon process in a lossless cavity. We study the quantum fluctuations in the two-mode system and investigate in detail the effects of detuning, Stark shift and atomic coherence on atomic dipole squeezing (ADS). We show that ADS strongly depends on the atomic coherence. It is found that the stronger the correlations between the two modes are involved, the more the ADS could be generated. The detuning or Stark shift has a destructive effect on ADS, but the combined effect of the detuning and Stark shift may lead to a regular, periodical and strong ADS pattern.

cond-mat.mtrl-sci↗
arXiv2003

Generation of higher-order atomic dipole squeezing in a high-Q micromaser cavity: VIII. multi-photon interaction

In our preceding serial works, we have investigated the generation of higher-order atomic dipole squeezing (HOADS) in a high-Q micromaser cavity, discussing the effects of dynamic Stark shift, atomic damping, atomic coherence and nonlinear one-photon processes and different initial states (for example, correlated and uncorrelated states, superposition states, squeezed vacuum). In this paper, we continue to study HOADS in a high-Q micromaser cavity, but consider that the atom interacts with the optical field via a multi-photon transition process and that the initial atom is arbitrarily prepared. For a vacuum initial field, we demonstrate that HOADS cannot occur if the atom is initially prepared in a chaotic state and that a coherent atomic state generates less efficient and stable HOADS than an arbitrary one. It is found that large detuning may lead to enhanced and strong HOADS.

cond-mat.mtrl-sci↗
arXiv2003

Electronic, vibrational and magnetic properties of a novel C_{48}N_{12} aza-fullerene

We study the structural, electronic, vibrational and magnetic properties of a novel ${\rm C}_{48}{\rm N}_{12}$ aza-fullerene using density functional theory and restricted Hartree-Fock theory. Optimized geometries and total energy of this fullerene have been calculated. We find that for ${\rm C}_{48}{\rm N}_{12}$ the total ground state energy is about -67617 eV, the HOMO-LUMO gap is about 1.9 eV, five strong IR spectral lines are located at the vibrational frequencies, 461.5 ${\rm cm}^{-1}$, 568.4 ${\rm cm}^{-1}$, 579.3 ${\rm cm}^{-1}$, 1236.1 ${\rm cm}^{-1}$, 1338.9 ${\rm cm}^{-1}$, the Raman scattering activities and depolarization ratios are zero, and 10 NMR spectral signals are predicted. Calculations of diamagnetic shielding factor, static dipole polarizabilities and hyperpolarizabilities of ${\rm C}_{48}{\rm N}_{12}$ are performed and discussed.

cond-mat.mtrl-sci↗
arXiv2003

First-principles calculations of the structural, electronic, vibrational and magnetic properties of C_{60} and C_{48}N_{12}: a comparative study

In this work, we perform first-principles calculations of the structural, electronic, vibrational and magnetic properties of a novel ${\rm C}_{48}{\rm N}_{12}$ azafullerene. Full geometrical optimization shows that ${\rm C}_{48}{\rm N}_{12}$ is characterized by several distinguishing features: only one nitrogen atom per pentagon, two nitrogen atoms preferentially sitting in one hexagon, ${\rm S}_{6}$ symmetry, 6 unique nitrogen-carbon and 9 unique carbon-carbon bond lengths. The highest occupied molecular orbital of ${\rm C}_{48}{\rm N}_{12}$ is a doubly degenerate level of $a_{g}$ symmetry and its lowest unoccupied molecular orbital is a nondegenerate level of $a_{u}$ symmetry. Vibrational frequency analysis predicts that ${\rm C}_{48}{\rm N}_{12}$ has in total 116 vibrational modes: 58 infrared-active and 58 Raman-active modes. ${\rm C}_{48}{\rm N}_{12}$ is also characterized by 8 $^{13}{\rm C}$ and 2 $^{15}{\rm N}$ NMR spectral signals. Compared to ${\rm C}_{60}$, ${\rm C}_{48}{\rm N}_{12}$ shows an enhanced third-order optical nonlinearities which implies potential applications in optical limiting and photonics.

cond-mat.mtrl-sci↗
arXiv2003

Electron-Hole Correlations and Optical Excitonic Gaps in Quantum-Dot Quantum Wells: Tight-Binding Approach

Electron-hole correlation in quantum-dot quantum wells (QDQW's) is investigated by incorporating Coulomb and exchange interactions into an empirical tight-binding model. Sufficient electron and hole single-particle states close to the band edge are included in the configuration to achieve convergence of the first spin-singlet and triplet excitonic energies within a few meV. Coulomb shifts of about 100 meV and exchange splittings of about 1 meV are found for CdS/HgS/CdS QDQW's (4.7 nm CdS core diameter, 0.3 nm HgS well width and 0.3 nm to 1.5 nm CdS clad thickness) which have been characterized experimentally by Weller and co-workers [ D. Schooss, A. Mews, A. Eychmuller, H. Weller, Phys. Rev. B, 49, 17072 (1994)]. The optical excitonic gaps calculated for those QDQW's are in good agreement with the experiment.

cond-mat.mtrl-sci↗
arXiv2003

Raman scattering in C_{60} and C_{48}N_{12} aza-fullerene: First-principles study

We carry out large scale {\sl ab initio} calculations of Raman scattering activities and Raman-active frequencies (RAFs) in ${\rm C}_{48}{\rm N}_{12}$ aza-fullerene. The results are compared with those of ${\rm C}_{60}$. Twenty-nine non-degenerate polarized and 29 doubly-degenerate unpolarized RAFs are predicted for ${\rm C}_{48}{\rm N}_{12}$. The RAF of the strongest Raman signal in the low- and high-frequency regions and the lowest and highest RAFs for ${\rm C}_{48}{\rm N}_{12}$ are almost the same as those of ${\rm C}_{60}$. The study of ${\rm C}_{60}$ reveals the importance of electron correlations and the choice of basis sets in the {\sl ab initio} calculations. Our best calculated results for ${\rm C}_{60}$ with the B3LYP hybrid density functional theory are in excellent agreement with experiment and demonstrate the desirable efficiency and accuracy of this theory for obtaining quantitative information on the vibrational properties of these molecules.

cond-mat.mtrl-sci↗