Multiband emission from single β-NaYF_(4)(Yb,Er) nanoparticles at high excitation power densities and comparison to ensemble studies

Ensemble and single particle studies of the excitation power density (P)-dependent upconversion luminescence (UCL) of core and core-shell β-NaYF_(4):Yb,Er upconversion nanoparticles (UCNPs) doped with 20% Yb^(3+) and 1% or 3% Er^(^(3+)) performed over a P regime of 6 orders of magnitude reveal an increasing contribution of the emission from high energy Er^(3+) levels at P > 1 kW/cm^(2). This changes the overall emission color from initially green over yellow to white. While initially the green and with increasing P the red emission dominate in ensemble measurements at P < 1 kW/cm^(2), the increasing population of higher Er^(^(3+)) energy levels by multiphotonic processes at higher P in single particle studies results in a multitude of emission bands in the ultraviolet/visible/near infrared (UV/vis/NIR) accompanied by a decreased contribution of the red luminescence. Based upon a thorough analysis of the P-dependence of UCL, the emission bands activated at high P were grouped and assigned to 2–3, 3–4, and 4 photonic processes involving energy transfer (ET), excited-state absorption (ESA), cross-relaxation (CR), back energy transfer (BET), and non-radiative relaxation processes (nRP). This underlines the P-tunability of UCNP brightness and color and highlights the potential of P-dependent measurements for mechanistic studies required to manifest the population pathways of the different Er^(3+) levels.

Rock fragmentation mechanisms and an experimental study of drilling tools during high-frequency harmonic vibration

Resonance drilling is a new technology, still at the laboratory stage. It has great potential to improve rock fragmentation efficiency. We analyzed the amplitude-frequency characteristics of steady- state mechanical vibration excited by harmonic vibration in rocks and an apparatus was built to achieve high fi＇equency vibration of rock. The influence of rock drillability, rotary speed, excitation frequency, and other parameters on the rate of penetration （ROP） in resonance drilling was analyzed. The results show that the rock drillability decreased with an increase in excitation frequency. When drilling with a large size drill bit, the ROP increased with excitation frequency. The ROP reached a maximum value at the resonant frequency of the rock. Tile ROP of the bit increased linearly with rotary speed when no vibration was applied on the rock and increased approximately exponentially when harmonic vibration was applied. In addition, the resonant frequency of the rock was changing during the process of rock fi＇agmentation, so in order to achieve tile desired resonance of the rock, it is necessary to detemaine an appropriate hamlonic vibration excitation frequency.

Adiabatic Potential Energy Surfaces and Photodissociation Mechanisms for Highly Excited States of H_(2)O

Full-dimensional adiabatic potential energy surfaces of the electronic ground state X and nine excited states A,I,B,C,D,D',D'',E' and F of H_(2)O molecule are developed at the level of internally contracted multireference configuration interaction with the Davidson correction.The potential energy surfaces are fitted by using Gaussian process regression combining permutation invariant polynomials.With a large selected active space and extra diffuse basis set to describe these Rydberg states,the calculated vertical excited energies and equilibrium geometries are in good agreement with the previous theoretical and experimental values.Compared with the well-investigated photodissociation of the first three low-lying states,both theoretical and experimental studies on higher states are still limited.In this work,we focus on all the three channels of the highly excited state,which are directly involved in the vacuum ultraviolet photodissociation of water.In particular,some conical intersections of D-E',E'-F,A-I and I-C states are clearly illustrated for the first time based on the newly developed potential energy surfaces(PESs).The nonadiabatic dissociation pathways for these excited states are discussed in detail,which may shed light on the photodissociation mechanisms for these highly excited states.

Study of highly excited vibrational dynamics of HCP integrable system with dynamic potential methods

Highly excited vibrational dynamics of phosphaethyne(HCP)integrable system are investigated based on its dynamic potentials.Taking into consideration the 2:1 Fermi resonance between H–C–P bending vibrational mode and C–P stretching vibrational mode,it is found that the effects of H–C stretching vibrational mode on vibrational dynamic features of the HCP integrable system are significant and regularly vary with Polyad numbers(P number).The geometrical profiles of the dynamic potentials and the corresponding fixed points are sensitive to the variation of H–C stretching vibrational strength when P numbers are small,but are not sensitive when P numbers become larger and the corresponding threshold values become lower.The phase space trajectories of different energy levels in a designated dynamic potential(P=28)were studied and the results indicated that the dynamic potentials govern the various dynamic environments in which the vibrational states lie.Furthermore,action integrals of the energy levels contained in dynamic potential(P=28)were quantitatively analyzed and elucidated.It was determined that the dynamic environments could be identified by the numerical values of the action integrals of trajectories of phase space,which is equivalent with dynamic potentials.

AN SCF-CI STUDY OF HIGHLY EXCITED VIBRATIONAL STATES OF BENT TRIATOMIC MOLECULES AND ITS APPLICATION TO O_(3)

A self-consistent-field—configuration interaction(SCF-CI)procedure of studying highly excited vibrational states of bent triatomic molecules is suggested and its application to O_3 is investigated.

Quasiclassical Trajectory Study of Collisional Energy Transfer between Highly Excited C_6F_6 and N_2 ,O_2 and Ground State C_6F_6

Quasiclassical trajectory calculation (QCT) is used frequently for studying collisional energy transfer between highly vibrationally excited molecules and bath gases. In this paper, the QCT of the energy transfer between highly vibrationally excited C6F6 and N2 ,O2 and ground state C6F6 were performed. The results indicate that highly vibrationally excited C6F6 transferred vibrational energy to vibrational distribution of N2, O2 and ground state C6F6, so they are V-V energy transfer. Especially it is mainly V-V resonance energy transfer between excited C6F6 and ground state C6F6, excited C6F6 transfers more vibrational energy to ground state C6F6 than to N2 and O2 . The values of QCT , -〈DEvib〉of excited C6F6 are smaller than those of experiments.

Experimental study of bound and autoionizing Rydberg states of the europium atom

An isolated-core-excitation （ICE） scheme and stepwise excitation are employed to study the highly excited states of the europium atom. The bound europium spectrum with odd parity in a region of 42400-43500 cm^-1 is measured, from which spectral information on 38 transitions, such as level position and relative intensity, can be deduced. Combined with information about excitation calibration and the error estimation process, the selection rules enable us to determine the possible values of total angular momentum J for the observed states. The autoionization spectra of atomic europium, belonging to the 4f^76pnl（l = 0, 2） configurations, are systematically investigated by using the three-step laser resonance ionization spectroscopy （RIS） approach. With the ICE scheme, all the experimental spectra of the autoionizing states have nearly symmetric profiles whose peak positions and widths can be easily obtained. A comparison between our results and those from the relevant literature shows that our work not only confirms many reported states, but also discovers 14 bound states and 16 autoionizing states.

Recent progress on garnet phosphor ceramics for high power solid-state lighting

As the fourth-generation light source,solid-state lighting has developed rapidly in the past 30 years due to its advantages of high efficiency and environmental protection.It is widely used in various scenes such as automobile headlights,projection displays,industrial production,and remote lighting.High-power,high-brightness white light-emitting diodes(LEDs)and laser diodes(LDs)technology put forward new requirements for the service stability of color conversion materials.Garnet phosphor ceramics have emerged with their unique advantages of withstanding high power excitation density and the flexibly tunable spectrum.In this article,the research progress of garnet based phosphor ceramics for high-power solid-state lighting was comprehensively reviewed.Firstly,the band gap and coordination environment regulations of luminescence centers of garnet phosphor were summarized.Secondly,the improvement of luminous efficacy via defects regulation was discussed.Thirdly,the relationship between the geometric design and the lighting performance was elucidated.Fourthly,the characterization methods of phosphor ceramics for laser lighting were introduced and illustrated.Finally,the development trend of garnet phosphor ceramics in solid state lighting and display was prospected.

Theoretical study of highly vibrational states of nonlinear triatomic molecules using Lie algebraic approach

The vibrational excitations of bent triatomic molecules are studied by using Lie algebra. The RMS error of fitting 30 spectroscopic data is 1.66 cm-1 for SO2. The results show that the expansion of a molecular algebraic Hamiltonian can well describe the experimental data. And the total vibrational levels can be calculated using this Hamiltonian. At the same time, the potential energy surface can also be obtained with the algebraic Hamiltonian.

The v-v energy transfer of highly vibrationally excited states (I)──Vibrational quenching of CO(v) by CO_2

The relaxation of the highly vibrationally excited CO (v=1-8) by CO\-2 is studied by time_resolved Fourier transform infrared emission spectroscopy (TR FTIR). 193 nm laser photolysis of the mixture of CHBr\-3 with O\-2 generates the highly vibrationally excited CO(v) molecules. TR FTIR records the intense infrared emission of CO(v→v-1). The vibrational populations of each level of CO(v) have been determined by the method of spectral simulation. Based on the evolution of the time resolved populations and the differential method, 8 energy transfer rate constants of CO(v=1-8) to CO 2 molecules are obtained: (5.7±0.1), (5.9±0.1), (5.2±0.2), (3.4±0.2), (2.4±0.3), (2.2±0.4), (2.0±0.4) and (1.8±0.6) (10 -14 cm 3·molecule -1·s -1), respectively. A two_channel energy transfer model can explain the feature of the quenching of CO(v) by CO 2. For the lower vibrational states of CO, the vibrational energy transfers preferentially to the υ\-3 mode of CO 2. For the higher levels, the major quenching channel changes to the vibrational energy exchange between CO(v→v-1) and the υ\-1 mode of CO 2.

The v-v energy transfer of highly vibrationally excitedstates (Ⅱ)──Vibrational quenching of CO(v) by H_2O

The vibrational energy transfer from highly vibrationally excited CO to H 2O molecules is studied by time-resolved Fourier transform infrared emission spectroscopy (TR FTIR). Following the 193 nm laser photolysis of CHBr 3 and O 2 the secondary reactions generate CO(v). The infrared emission of CO(v→v-1) is detected by TR FTIR. The excitation of H 2O molecules is not observed. By the method of the spectral simulation and the differential technique, 8 rate constants for CO(v)/H 2O system are obtained: (1.7±0.1), (3.4±0.2), (6.2±0.4), (8.0±1.0), (9.0±2.0), (12±3), (16±4) and (18±7) (10 -13cm 3·molecule -1·s -1). At least two reasons lead to the efficient energy transfer. One is the contributions of the rotational energy to the vibational energy defect and the other is the result of the complex collision. With the SSH and ab initio calculations, the quenching mechanism of CO(v) by H 2O is suggested.

What are Exciting in Laser Science

Recent advances in selected areas of laser science are briefly reviewed. They include laser technology, coherent control of quantum systems by lasers, X ray generation by ultrashort high intensity laser pulses, and laser spectroscopic studies of surface catalysis in real environment.