Anomalous dephasing of bosonic excitons interacting with phonons in the vicinity of the Bose-Einstein condensation

The dephasing and relaxation kinetics of bosonic excitons interacting with a thermal bath of acoustic phonons is studied after coherent pulse excitation. The kinetics of the induced excitonic polarization is calculated within Markovian equations both for subcritical and supercritical excitation with respect to a Bose-Einstein condensation (BEC). For excited densities n below the critical density , an exponential polarization decay is obtained, which is characterized by a dephasing rate . This dephasing rate due to phonon scattering shows a pronounced exciton-density dependence in the vicinity of the phase transition. It is well described by the power law that can be understood by linearization of the equations around the equilibrium solution. Above the critical density we get a non-exponential relaxation to the final condensate value p⁰ with that holds for all densities. Furthermore we include the full self-consistent Hartree-Fock-Bogoliubov (HFB) terms due to the exciton-exciton interaction and the kinetics of the anomalous functions . The collision terms are analyzed and an approximation is used which is consistent with the existence of BEC. The inclusion of the coherent exciton-exciton interaction does not change the dephasing laws. The anomalous function F_k exhibits a clear threshold behaviour at the critical density. Received 13 December 1999     

On the influence of two coexisting species of susceptibility-producing structures on the R21 relaxation rate

PurposeTissue microstructure can influence quantitative magnetic resonance imaging such as relaxation rate measurements. Consequently, relaxation rate mapping can provide useful information on tissue microstructure. In this work, the theory on relaxation mechanisms of the change of the relaxation rate ∆R₂^⁎ in the presence of spherical susceptibility sources in a spin bearing medium is validated in simulations and phantom experiments for the coexistence of two species of susceptibility sources.MethodsThe influence of coexisting spherical perturbers with magnetic susceptibilitys of different signs was evaluated in Monte Carlo simulations including diffusion effects in the surrounding medium. Simulations were compared with relaxometry measurements at 1.5 Tesla and at 3 Tesla. The phantoms used to validate the simulations were built from agarose gel containing calcium carbonate and tungsten carbide particles of different size and concentration.ResultsThe Monte Carlo simulations showed, that the change in relaxation rate only depends on the overall amount of susceptibility producing structures in the simulation volume and no difference was found, if mixtures of positive and negative particles were simulated. Phantom measurements within the static dephasing regime showed linear additivity of the effects from positive and negative susceptibility sources that were present within the same voxel.ConclusionsIn summary, both the simulations and the phantom measurements showed that changes in the relaxation rate ΔR₂^⁎ add up linearly for spherical particles with different susceptibilities within the same voxel if the conditions for the static dephasing regime are fulfilled. If particles with different susceptibilities have both different sizes and violate the conditions of the static dephasing regime, effects on relaxation rates might no longer be linear.     

Dephasing in the semiclassical limit is system-dependent

Dephasing in open quantum chaotic systems has been investigated in the limit of large system sizes to the Fermi wavelength ratio, L/λ_F 〉 1. The weak localization correction g ^wl to the conductance for a quantum dot coupled to (i) an external closed dot and (ii) a dephasing voltage probe is calculated in the semiclassical approximation. In addition to the universal algebraic suppression g ^wl ∝ (1 + τ_D/τ_?)^?1 with the dwell time τ_D through the cavity and the dephasing rate τ _? ^?1 , we find an exponential suppression of weak localization by a factor of ∝ exp[? $\tilde \tau $ /τ_?], where $\tilde \tau $ is the system-dependent parameter. In the dephasing probe model, $\tilde \tau $ coincides with the Ehrenfest time, $\tilde \tau $ ∝ ln[L/λ_F], for both perfectly and partially transparent dot-lead couplings. In contrast, when dephasing occurs due to the coupling to an external dot, $\tilde \tau $ ∝ ln[L/ξ] depends on the correlation length ξ of the coupling potential instead of λ_F.     

Hydrothermal synthesis of carbon- and reduced graphene oxide-supported CoMoO4 nanorods for supercapacitor

Hybrid CoMoO₄ nanorods with carbon (C) and graphene oxide (rGO) are successfully synthesized via one-step hydrothermal process. Hybrid α-CoMoO₄ nanorods have shown excellent electrochemical performances compared to pristine CoMoO₄ in alkaline electrolyte. Specifically, CoMoO₄/C nanorod exhibits a maximum specific capacitance of 451.6 F g^?1 at the current density of 1 A g^?1, whereas CoMoO₄/rGO shows high specific capacitance of 336.1 F g^?1 at the same current density. Both the hybrid nanorods show good rate capability even at high current density of 20 A g^?1 and long-term cyclic stability. The observed electrochemical features of the hybrid CoMoO₄ nanostructure could be attributed to the presence of highly conductive carbonaceous material on unique one-dimensional nanorod microstructure which enhances the electrical conductivity of the nanorods thereby allowing faster electrolyte ion diffusion during the redox process.     

Ge Nanoparticles Encapsulated in Interconnected Hollow Carbon Boxes as Anodes for Sodium Ion and Lithium Ion Batteries with Enhanced Electrochemical Performance

A carbothermal reaction route to Ge nanoparticle homogeneously encapsulated hollow carbon boxes from NH₄H₃Ge₂O₆/resorcinol formaldehyde precursors is designed, using NH₄H₃Ge₂O₆ as a Ge precursor from commercial GeO₂ and NH₄OH. The Ge/C hybrid anode for sodium ion battery displays a higher Na⁺ storage capacity of 346 mA h g^?1 after 500 cycles at a current density of 100 mA h g^?1, almost approaching the theoretical capacity of Ge. Furthermore, Ge/C anode shows significantly improved electrochemical performance for Li⁺ storage, showing a higher initial Coulombic efficiency of 85.1% and a superior reversible capacity of 1336 mA h g^?1 at a high current density of 200 mA g^?1 after 150 cycles. An excellent rate capability with a capacity of 825 mA h g^?1 at a current density of 4.0 A g^?1 can be obtained based on Ge/C anodes. The enhanced electrochemical performance can be attributed to the unique microstructures of Ge/C hybrid anode. The internal void space of hollow carbon boxes can accommodate the volume expansion of Ge during lithiation or sodiation process, thus preserving the structural integrity of electrode material. The interconnected carbon shell can increase the electronic conductivity of the electrode, resulting in the high rate capability and cycling stability.     

Raman study of temperature and pressure effects on vibrational relaxation in liquid CHCl3 and CDCl3

The Raman line shapes of the ν₁(A ₁)C-H and C-D stretching fundamentals in liquid CHCl₃ and CDCl₃ have been measured as a function of pressure from 1 bar to 4·5 kbar within the temperature range 30°C to 90°C. Densities have also been determined under the same experimental conditions. The vibrational relaxation rates are obtained from the isotropic component of the Raman band and the experimental results can be summarized as follows: (i) as T increases at constant density the vibrational relaxation rate increases; (ii) at constant T, the increase in density produces an increase in the relaxation rate; (iii) an increase in temperature at constant pressure results in an increased relaxation rate. The above three cases hold for the CDCl₃ liquid, whereas only (ii) may be stated for the CHCl₃ liquid.

The experimental vibrational data are interpreted in terms of the Kubo stochastic line-shape theory and the collinear-isolated-binary-collision model proposed by Fischer and Laubereau. Application of the Kubo formalism shows that vibrational dephasing is the dominant relaxation mechanism and that the modulation is fast both in liquid CHCl₃ and CDCl₃.

Interpretation in terms of the binary collision dephasing model leads to the following results: (i) the pure dephasing mechanism seems to be the dominant broadening mechanism for the isotropic Raman line shapes studied; (ii) the calculated dephasing rates as a function of density and temperature show agreement with the experimental data. In these calculations the elastic collision times are obtained from the modified Enskog theory.     

Magnetic field dependent optical dephasing in LaF3:Er3+

Optical dephasing of the 5388 Å transition between the lowest Kramers doublets of the ⁴S_{$\text{3}\text{2}$} and ⁴I_{$\text{15}\text{2}$} multiplets of Er³⁺:LaF₃ has been studied by photon echo, optical phase switching and optical free induction decay. Er³⁺?¹⁹F hyperfine interactions produce dephasing which is two orders of magnitude faster than in previously studied non-Kramers systems, but at high field changes in the spin dynamics result in microsecond dephasing. For the lower Zeeman component of ⁴S_{$\text{3}\text{2}$}, T₂ (=6μs) is independent of H₀ whereas for the upper component the dephasing is rapid and strongly field dependent. This is quantitatively accounted for by spin lattice relaxation of the upper component of ⁴S_{$\text{3}\text{2}$}. Below 20 kG concentration and temperature dependent dephasing due to electron spin diffusion is observed.     

Tailoring MoS2 Ultrathin Sheets Anchored on Graphene Flexible Supports for Superstable Lithium‐Ion Battery Anodes

2D MoS₂ has a significant capacity decay due to the stack of layers during the charge/discharge process, which has seriously restricted its practical application in lithium‐ion batteries. Herein, a simple preform‐in situ process to fabricate vertically grown MoS₂ nanosheets with 8–12 layers anchored on reduced graphene oxide (rGO) flexible supports is presented. As an anode in MoS₂/rGO//Li half‐cell, the MoS₂/rGO electrode shows a high initial coulomb efficiency (84.1%) and excellent capacity retention (84.7% after 100 cycles) at a current density of 100 mA g^?1. Moreover, the MoS₂/rGO electrode keeps capacity as high as 786 mAh g^?1 after 1000 cycles with minimum degradation of 54 µAh g^?1 cycle^?1 after being further tested at a high current density of 1000 mA g^?1. When evaluated in a MoS₂/rGO//LiCoO₂ full‐cell, it delivers an initial charge capacity of 153 mAh g^?1 at a current density of 100 mA g^?1 and achieves an energy density of 208 Wh kg^?1 under the power density of 220 W kg^?1.     

Hierarchical porous ZnMn<Subscript>2</Subscript>O<Subscript>4</Subscript> synthesized by the sucrose-assisted combustion method for high-rate supercapacitors

A simple sucrose-assisted combustion and subsequent high-temperature calcination route have been employed to prepare hierarchical porous ZnMn₂O₄ nanostructure. When used as an electrode for supercapacitor, the ZnMn₂O₄ electrode displays a high specific capacitance of 411.75 F g^?1 at a current density of 1 A g^?1, remarkable capacitance retention rate of 64.28 % at current density of 32 A g^?1 compared with 1 A g^?1, as well as excellent cycle stability (reversible capacity retention of 88.32 % after 4000 cycles). The outstanding electrochemical performances are mainly attributed to its hierarchical porous architecture, which provides large reaction surface area, fast ion and electron transfer, and good structure stability. All these impressive results demonstrate that ZnMn₂O₄ shows promise for its application in supercapacitors.     

Collective spontaneous emission of dye molecules and lasing

The threshold pump power density for lasing in dye solutions is found to depend on the photon energy of pumping radiation. An increase in the pumping photon energy can significantly lower the threshold pump power of dye lasers. For an ethanol solution of rhodamine 6G with a concentration of 4×10¹⁸ cm^?3, the threshold power density for pumping radiation with a wavelength of 532 nm is 20-fold higher than for pumping radiation with a wavelength of 347 nm. This phenomenon is associated with the competition of collective spontaneous emission, which can lead to the efficient deactivation of excited molecules in femtosecond times, and the dephasing of excited molecules due to the intramolecular nonradiative processes of absorbed-energy conversion. An increase in the dephasing rate with the increasing energy of exciting photons lowers the efficiency of collective spontaneous emission and increases the concentration of dephased excited molecules responsible for lasing.     

Synthesis and Spectroscopic Properties of Iron(H) Complex with Sterically Encumbered Thiolate Ligand: 2,4,6-Triphenylbenzenethiolate

Abstract

Novel iron(II) complex of 2,4,6-triphenylbenzenethiolate (tpbt) was synthesized by ligand exchange reaction of (Et₄N)2[Fe^II(S-t-Bu)₄] with tpbt-H. The complex shows absorption maxima at 277 nm (36500 M^?1cm^?1) and 367 nm (22800 M^?1 cm^?1), and Fe²⁺/Fe³⁺ redox potential at-0.78 V vs SCE in acetonitrile. While in tetrahydrofuran solution, the complex is found to be unstable and form a Fe(II) complex with low coordination number.     

Effect of pressure on the properties of DH diode lasers in AlxGa1-xAsySb1-y/GaSb system

Abstract

A helium pressure appparatus for diode laser studies up to 1.4 GPa at 77–300 K has been developed. DH lasers with Al_xGa_1-xAs_ySb_1-y active layers (x=0-0.05) lattice-matched to GaSb substrates have been investigated. It has been shown that in lasers with x,y=0 pressure dependences of the threshold current density (J_th) and the average electron lifetime at the threshold (τ) measured at 80 K depend strongly on the quadratic recombination of L^c ₆ electrons, the characteristic coefficient being 1.5×10^?11 cm³s^?1. The pressure-composition equivalence coefficient dx/dP=2.2×10^?10 Pa^?1 has been obtained for the lowest temperatures used.     

The density and pressure of helium in bubbles in metals

Abstract

The energy shift of the He 1¹S₀?2¹P₁ transition, ΔE(n), can be used to determine the density, n, of He in bubbles in metals. A self-consistent band structure calculation for solid fcc He yields a linear relationship ΔE=C.n with C _th=22 × 10^?3 eV nm³. Systematic electron energy loss spectroscopy and transmission electron microscopy studies of He bubbles in Al for various He doses and temperatures result in C_exp=(24±8).10^?3 eV nm³ in agreement with theory. The analysis is consistent with the assumption that dislocation loop punching is the dominant bubble growth mechanism during high-dose room temperature implantation. The application to He bubbles in Ni indicates a maximum He density of n=0.2 × 10³ nm^?3 for which He should be solid at room temperature.     

Optical echo spectroscopy and phase relaxation of Nd3+ ions in CaF2 crystals

Accumulated photon echoes have been used to investigate the mechanisms of optical dephasing in CaF₂ crystals activated by Nd³⁺ ions. Tunable picosecond laser radiation, which permits the selective excitation of various Nd³⁺ optical centers in the ⁴ I _9/2→⁴ G _5/2, ² G _7/2 transition, is used. The optical phase relaxation times measured at temperatures from 9 to 50 K permit determination of the homogeneous widths of the transitions between the low-lying ⁴ I _9/2 Stark level and three excited ⁴ G _5/2, ² G _7/2 levels, and calculation of the constants of the inter-Stark relaxation transitions in the ground and excited multiplets for the rhombic N and M Nd³⁺ centers in CaF₂ crystals. An analysis of the temperature dependence of the homogeneous linewidth of the transitions between low-lying Stark levels of the ground and excited states shows that the mechanism of optical dephasing in the crystals investigated is described well by direct relaxation processes with resonant inter-Stark absorption of one phonon in the ground and excited states. At T=9 K, the homogeneous linewidth Γ_h in CaF₂ crystals is almost an order of magnitude smaller than Γ_h in disordered CaF₂-YF₃ crystals. This difference can be attributed to the significantly greater spectral phonon density of states in disordered crystals. Zh. éksp. Teor. Fiz. 113, 278–290 (January 1998)     

Low temperature electron transport in phosphorus-doped ZnO films grown on Si substrates

Low temperature magneto-transport properties and electron dephasing mechanisms of phosphorus-doped ZnO thin films grown on (1 1 1) Si substrates with Lu₂O₃ buffer layers using pulsed laser deposition were investigated in detail by quantum interference and weak localization theories under magnetic fields up to 10 T. The dephasing length follows the temperature dependence with an index p≈1.6 at higher temperatures indicating electron–electron interaction, yet becomes saturated at lower temperatures. Consistent with photoluminescence measurements and the multi-band simulation of the electron concentration, such behavior was associated with the dislocation densities obtained from x-ray diffraction and mobility fittings, where charged edge dislocations acting as inelastic Coulomb scattering centers were affirmed responsible for electron dephasing. Owing to the temperature independence of the dislocation density, the phosphorus-doped ZnO film maintained a Hall mobility of 4.5 cm² V⁻¹ s⁻¹ at 4 K.     

Hydrothermal Synthesis of Nickel Phosphate Nanorods for High‐Performance Flexible Asymmetric All‐Solid‐State Supercapacitors

Ni₂₀[(OH)₁₂(H₂O)₆][(HPO₄)₈(PO₄)₄]·12H₂O nanorods are successfully synthesized via a one‐pot hydrothermal reaction. A high‐performance flexible asymmetric all‐solid‐state supercapacitor based on the obtained Ni₂₀[(OH)₁₂(H₂O)₆][(HPO₄)₈(PO₄)₄]·12H₂O nanorods (positive electrode) and graphene nanosheets (negative electrode) is successfully assembled. It is the first report of this nanomaterial applied for all‐solid‐state supercapacitors. Interestingly, a maximum volumetric energy density of 0.446 mW h cm^?3 at a current density of 0.5 mA cm^?2 and a maximum power density of 44.1 mW cm^?3 at a current density of 6.0 mA cm^?2 are achieved by the as‐assembled device. What's more, the device also shows excellent mechanical flexibility and little capacitance change after over 5000 charge/discharge cycles at a current density of 0.5 mA cm^?2.     

Isotope-selective femtosecond wave packet dynamics: The rare molecule

For the first time, the femtosecond real-time vibrational dynamics of the rare ^41,41K₂ isotope, excited to the electronic state, could be selectively studied by means of time-resolved three photon ionization. A vibrational period of fs is determined. Superimposed, a beat structure with a period of 20 ps is observed. A detailed Fourier analysis reveals a strong band of three lines centered around 65.5 cm^-1. A significant perturbation of the wave packet caused by spin-orbit coupling of the A and the crossing state is found. This perturbation is the reason for the fast dephasing of the initially generated wave packet within about 10 ps. The spectrogram of the real-time data shows total revivals of the wave packet at 20 ps and 40 ps. Fractional revivals are found for times around 10 ps and 30 ps. Due to high intensity effects a remarkable slightly broadened line at 90 cm^-1 appears and can be assigned to the wave packet propagation generated in the dimer's ground state by impulsive stimulated Raman scattering. Revivals of this ground state wave packet are found at 17ps and 34ps. A comparison with other isotopes of K₂ is given. Received: 9 February 1998 / Revised: 15 May 1998 / Accepted: 2 June 1998     

Vibrational Spectroscopy of the Borate Mineral Priceite—Implications for the Molecular Structure

ABSTRACT

Priceite is a calcium borate mineral and occurs as white crystals in the monoclinic pyramidal crystal system. We have used a combination of Raman spectroscopy with complimentary infrared spectroscopy and scanning electron microscopy with Energy-dispersive X-ray Spectroscopy (EDS) to study the mineral priceite. Chemical analysis shows a pure phase consisting of B and Ca only. Raman bands at 956, 974, 991, and 1019 cm^?1 are assigned to the BO stretching vibration of the B₁₀O₁₉ units. Raman bands at 1071, 1100, 1127, 1169, and 1211 cm^?1 are attributed to the BOH in-plane bending modes. The intense infrared band at 805 cm^?1 is assigned to the trigonal borate stretching modes. The Raman band at 674 cm^?1 together with bands at 689, 697, 736, and 602 cm^?1 are assigned to the trigonal and tetrahedral borate bending modes. Raman spectroscopy in the hydroxyl stretching region shows a series of bands with intense Raman band at 3555 cm^?1 with a distinct shoulder at 3568 cm^?1. Other bands in this spectral region are found at 3221, 3385, 3404, 3496, and 3510 cm^?1. All of these bands are assigned to water stretching vibrations. The observation of multiple bands supports the concept of water being in different molecular environments in the structure of priceite. The molecular structure of a natural priceite has been assessed using vibrational spectroscopy.     

Laser Induced Energy Transfer Studies in Polyatomic Mixtures: CH3F-NO2

Abstract

The internal kinetics of NO₂ as well as the kinetics of crossover between CH₃F and NO₃ were studied in mixtures of these polyatomics and rare gases.

Subsequent to excitation of the CH₃F to v ₃=1 by the P(20) line of a 9.6μ Q-switch CO₂ laser, fluorescence of NO₂ at 6.12μ from v ₃=1 was monitored.

The equilibration rate of the stretching modes in NO₂ was determined to be 46 ± 10 msec^?1 torr^?1 while the rate of stretches-bend equilibration was measured as 15 ± 3 msec^?1 torr^?1. The rate of crossover from excited CH₃F to NO₂ in high rare gas dilution was measured as 90 ± 20 msec^?1 torr^?1 and the reverse rate as 285 ± 60 msec^?1 torr^?1.

Comparison to other triatomic systems as well as other experiments with mixtures of polyatomics are made and implications of laser “photochemistry” of NO₂ reactions are discussed.     

The gas phase oxidation of HCOOH by Cl and NH2 radicals. Proton coupled electron transfer versus hydrogen atom transfer*

ABSTRACT

The reaction of formic acid (HCOOH) with chlorine atom and amidogen radical (NH₂) have been investigated using high level theoretical methods such BH&HLYP, MP2, QCISD, and CCSD(T) with the 6–311?+?G(2df,2p), aug-cc-pVTZ, aug-cc-pVQZ and extrapolation to CBS basis sets. The abstraction of the acidic and formyl hydrogen atoms of the acid by the two radicals has been considered, and the different reactions proceed either by a proton coupled electron transfer (pcet) and hydrogen atom transfer (hat) mechanisms. Our calculated rate constant at 298?K for the reaction with Cl is 1.14?×?10^?13?cm³?molecule^?1?s^?1 in good agreement with the experimental value 1.8?±?0.12/2.0?×?10^?13?cm³?molecule^?1?s^?1 and the reaction proceeds exclusively by abstraction of the formyl hydrogen atom, via hat mechanism, producing HOCO+ClH. The calculated rate constant, at 298?K, for the reaction with NH₂ is 1.71?×?10^?15?cm³?molecule^?1?s^?1, and the reaction goes through the abstraction of the acidic hydrogen atom, via a pcet mechanism, leading to the formation of HCOO+NH₃.