Experimental Investigation on Selective Excitation of Two-Pulse Coherent Anti-Stokes Raman Scattering

Selective excitation of coherent anti-Stokes Raman scattering from the benzene solution is achieved by adaptive pulse shaping based on genetic algorithm, and second harmonic generation frequency-resolved optical gating （SHG-FROG） technique is adopted to characterize the original and optimal laser pulses. The mechanism for two-pulse coherent mode-selective excitation of Raman scattering is experimentally investigated by modulating the pump pulse in the frequency domain, and it is indicated that two-pulse coherent mode-selective excitation of Raman scattering mainly depends on the effective frequency components of the pump pulse related to specific vibrational mode. The experimental results suggest that two-pulse CARS has good signal-to-background ratio and high sensitivity, and it has attractive potential applications in the complicated molecular system.     

New regime of fs-pulse stimulated Raman scattering

We present the results of experimental and theoretical studies of fs-pulse Raman-frequency conversion in gases in the regime of medium pumping with pulses shorter than the molecular vibrational period T_v. The spectral transformation of both intense excitation pulses and variably delayed injection pulses is analyzed as a function of laser parameters and gas pressure. For intense 40 fs pump pulses propagating in a SF₆-filled hollow waveguide, we observed a continuous (pressure-dependent) redshift of the carrier frequency, amounting to several thousand cm^у. By transmitting a weak injection pulse with a narrow spectrum through impulsively excited SF₆, we observed multiple Stokes and anti-Stokes lines of the injection radiation corresponding to scattering on the symmetric vibrational mode of SF₆. Since the pumping and scattering processes are decoupled in this delayed-pulse scheme, the effect of Kerr self-action on the injection field scattering was completely eliminated. Our physical model of the fs-pulse stimulated Raman scattering is in good quantitative agreement with the observed effects.     

红宝石能谱的理论研究

 本文用限制Hartree-Fock自洽场方法对红宝石进行了计算，得到了单电子分子轨道，在此基础上利用不可约张量方法求解红宝石价电子体系多体Schrodinger方程，得到了与实验相符的红宝石d－d跃迁能谱，标准误差为九百波数。进一步计算了在不同压力下红宝石d－d跃迁能谱。结果表明，能谱中R₁线（⁴A₁→²E）随压力增大产生红移，与实验定性一致。     

Observation of Quantum Beating from Two Coupled Parametric Six-Wave Mixing Signals in Rb

Two processes of coupled difference-frequency axially phase-matched parametric six-wave mixing are carried out in Rb vapour by two-photon excitation using fs laser pulses, and parametric six-wave mixing signals in the infrared and near infrared regime are detected. The infrared parametric six-wave mixing signals are up-converted into the visible spectral range by sum-frequency mixing with the pump laser in a LiIO₃ crystal. Moreover, quantum beating at 608cm^-1, corresponding to the 7s-5d energy difference in Rb, is observed from the sum-frequency signal at 495nm. As a result, we obtain modulated light signals in the visible, near infrared and infrared spectral ranges, and study the interference between 7s and 5d states of Rb.     

Dual-beam ablation of fused silica by multiwavelength excitation process using KrF excimer and F2 lasers

A new technique of dual-beam laser ablation of fused silica by multiwavelength excitation process using a 248-nm KrF excimer laser (ablation beam) coupled with a 157-nm F₂ laser (excitation beam) in dry nitrogen atmosphere is reported. The dual-beam laser ablation greatly reduced debris deposition and, thus, significantly improved the ablation quality compared with single-beam ablation of the KrF laser. High-quality ablation can be achieved at the delay times of KrF excimer laser irradiation shorter than 10 ns due to a large excited-state absorption. The ablation rate can reach up to 80 nm/pulse at the fluence of 4.0 J/cm² for the 248-nm laser and 60 mJ/cm² for the F₂ laser. The ablation threshold and effective absorption coefficient of KrF excimer laser are estimated to be 1.4 J/cm² and 1.2᎒⁵ cm^-1, respectively.     

立方氮化硼的振动光谱及反射光谱的研究

 将黑色、黄色、棕色三种小于50 μm立方氮化硼粉末为样品，研究了其红外光谱、拉曼光谱、反射光谱，结果表明：（1）样品的红外光谱中，1 818 cm^-1和1 548 cm^-1属于cBN的晶格本征振动，而立方氮化硼的晶格本征振动外的晶体缺陷吸收则发生在~800 cm^-1，1 580 cm^-1~1 740 cm^-1和大于2 400 cm^-1处。（2）拉曼光谱测试表明，在1 052 cm^-1和1 304 cm^-1附近出现的散射与cBN不具有反演中心及cBN具有立方结构这样的事实相一致，并且这种散射伴随着布里渊区中心声子的横向和纵向发射。144 cm^-1附近出现的散射，被认为是由于局部振荡模式的出现，在反斯托克斯区造成的信号，这与晶格中杂质缺陷有关。（3）依据得到的反射光谱，计算了cBN单晶禁带宽度，发现这三种cBN都具有大于金刚石的禁带宽度值，分别为：E_g(黑)=6.21 eV，E_g(黄)=5.73 eV，E_g(棕)=5.71 eV。     

Micromachining of quartz crystal with excimer lasers by laser-induced backside wet etching

We fabricated a well-defined pattern of lines and spaces on the surface of a quartz crystal plate (c-SiO₂) with micron-sized features, using laser-induced backside wet etching (LIBWE). The line patterns obtained using LIBWE showed a high aspect ratio of about 3. The etch rates of fused silica (a-SiO₂) ranged from 5 to 25 nm/pulse with KrF laser irradiation from 0.4-1.3 J/cm². Threshold fluences for a-SiO₂ and c-SiO₂ were 0.23 and 0.34 J/cm², respectively. The single-pulse etch depth was not affected by the repetition rates of laser pulses from 1-50 Hz.     

压力对GdoBr:Eu晶场参数的影响

 在室温下测量了GdoBr:Eu的常压和高压荧光谱，光谱范围在13 000~21 500 cm^-1之间，压力至12 GPa。由光谱数据得到了Eu³⁺晶场能级随压力的变化曲线。⁷F_0～5能级随压力的变化规律比较复杂，而⁵D_0~2各能均随压力的升高几乎线性地降低。在基态谱项⁷F的49个状态上进行了晶场拟合计算，所得常压下的5个非零晶场参数分别为：B₀²＝-1 124.0 cm^-1，B₀⁴＝-969.6 cm^-1，B₄⁴＝827.9 cm^-1，B₀⁶＝889.6 cm^-1，B₄⁶＝377.0 cm^-1。高压下的计算结果表明，B₀⁴、B₀⁶这两个晶场参数随压力的增加而增大，B₄⁶随压力的增加而减小，而B₀²、B₄⁴随压力的变化有些起伏。晶场强度在8 GPa以下随压力增加而减小，其后开始变强。     

High-speed etching of hexagonal GaN by laser ablation and successive chemical treatment

Photostimulated direct etching of GaN has been demonstrated with extremely high etching rate up to 135 nm/pulse. The process consists of laser irradiation and ex-situhydrochloric acid treatment. Not only deep etching but also a highly planarized surface are obtained by an increase in laser fluence and the number of pulses. Seven-pulse irradiation at 1 J/cm² decreases surface average roughness (R_a) to ~2 nm from ~10 nm of the untreated sample. No deep-level emission (450-600 nm) is detected in photoluminescence measurement on the samples irradiated with laser fluences as high as 3 J/cm².     

Diagnostics of laser-produced plume under carbon nanotube growth conditions

This paper presents diagnostic data obtained from the plume of a graphite composite target during carbon nanotube production by the double-pulse laser oven method. The in situ emission spectrum (300 to 650 nm) is recorded at different locations upstream of the target and at different delay times from the lasers (IR and green). Spectral features are identified as emissions from C₂ (Swan System: d³@_g-a³@_u) and C₃ (Comet Head System: A¹@_u-X¹D_u⁺). Experimental spectra are compared with computed spectra to estimate vibrational temperatures of excited state C₂ in the range of 2500 to 4000 K. The temporal evolution of the 510-nm band of C₂ is monitored for two target positions in various locations, which shows confinement of the plume in the inner tube and increase in plume velocity with temperature. The excitation spectra of C₂ are obtained by using a dye laser to pump the (0,1) transition of the Swan System and collecting the laser-induced fluorescence signal from C₂. These are used to obtain "ground-state" rotational and vibrational temperatures which are close to the oven temperature. Images of the plume are also collected and are compared with the spectral measurements.     

Growth of oriented Pb(ZrxTi1-x)O3 thin films on glass substrates by pulsed laser deposition

Oriented crystalline Pb(Zr_xTi_1-x)O₃ (x=0.53) (PZT) thin films were deposited on metallized glass substrates by pulsed laser deposition (1060-nm wavelength Nd:YAG laser light, 10-ns pulse duration, 10-Hz repetition rate, 0.35-J/pulse and 25-J/cm² laser fluence), from a commercial target at substrate temperatures in the range 380-400 °C. Thin films of 1-3 7m were grown on Au(111)/ Pt/NiCr/glass substrates with a rate of about 1 Å/pulse on an area of 1 cm². The deposited PZT films with perovskite structure were oriented along the (111) direction, as was revealed from X-ray diffraction spectra. Fourier transform infrared spectroscopy (FTIR) was performed on different PZT films so that their vibrational modes could be determined. Piezoelectric d₃₃ coefficients up to 30 pC/N were obtained on as-deposited films. Ferroelectric hysteresis loops at 100 Hz revealed a remanent polarization of 20 7C/cm² and a coercive field of 100 kV/cm.     

An Artificially Garnet Crystal Materials Using In Terahertz Waveguide

A hypothesis is brought forward that the materials with low propagation loss in both optical and microwave band may exhibit good performance in terahertz （THz） band because THz wave band interspaces those two wave bands. For the purpose-of exploring a kind of low-loss material for THz waveguide, Lu2.1Bi0.9Fe5O12（LuBiIG） garnet films are prepared by liquid phase epitaxy （LPE） method on a gadolinium gallium garnet （GGG） substrate from lead-free flux because of the good properties in both optical and microwave bands. In microwave band, the ferromagnetic resonance （FMR） linewidth of the film 2△H = 2.8-5.1Oe; in optical band, the optical absorption coefficient is 600cm^-1 at visible range and about 100-170cm^-1 when the wavelength is longer than 800nm. In THz range, our hypothesis is well confirmed by a THz-TDS measurement which shows that the absorbance of the film for THz wave is 0.05-0.3 cm 1 and the minimum value appears at 2.3 THz. This artificial ferromagnetic material holds a great promise for magnetic field tunable THz devices such as waveguide, modulator or switch.     

Polarized Micro-Raman Study of the Temperature-Induced Phase Transition In 0.67 Pb（Mg1/3Nb2/3）O3-0.33PbTiO3

Polarized Raman spectra of ferroelectric relaxor 0.67Pb（Mg1/3Nb2/3）O3-0.33PbTiO3 （0.67PMN-0.33PT） single crystal are systematically investigated in a wide temperature range from -196 to 600℃ by micro-Raman scattering technique. The results clearly reveal that there are two structural phase transitions in such composite ferroelectric relaxor： the rhombohedral-tetragonal （R- T） phase transition and the tetragonal-cubic （T- C） phase transition. The former occurs at about TR-T =34℃, corresponding to the vanishing of the soft A1 mode at 106cm^-1 recorded in the parallel polarization. The latter appears at about TT-C = 144℃, which can be verified with the vanishing of mode at 780cm^-1 measured in the crossed polarization.     

Atomic Diffusion in Cu/Si （111） and Cu/SiO2/Si （111） Systems by Neutral Cluster Beam Deposition

The Cu films are deposited on two kinds of p-type Si （111） substrates by ionized duster beam （ICB） technique. The interface reaction and atomic diffusion of Cu/Si （111） and Cu/SiO2/Si （111） systems are studied at different annealing temperatures by x-ray diffraction （XRD） and Rutherford backscattering spectrometry （RBS）. Some significant results are obtained： For the Cu/Si （111） samples prepared by neutral dusters, the interdiffusion of Cu and Si atoms occurs when annealed at 230℃. The diffusion coefficients of the samples annealed at 230℃ and 500℃ are 8.5 ×10^-15 cm^2.s^-1 and 3.0 ×10^-14 cm^2.s^-1, respectively. The formation of the copper-silicide phase is observed by XRD, and its intensity becomes stronger with the increase of annealing temperature. For the Cu/SiO2//Si （111） samples prepared by neutral dusters, the interdiffusion of Cu and Si atoms occurs and copper silicides are formed when annealed at 450℃. The diffusion coefficients of Cu in Si are calculated to be 6.0 ×10^-16 cm^2.s^-1 at 450℃, due to the fact that the existence of the SiO2 layer suppresses the interdiffusion of Cu and Si.     

Dielectronic Recombination of Sn^10＋ Ions and Related Satellite Spectra

Based on the multi-configuration Dirac-Fock method, theoretical calculations are carried out for the dielectronic recombination （DR） rate coefficients and the collision excitation rate coefficients of Sn^10＋ ions. It is found that the total DR rate coefficient has its maximum value between 10eV and 100eV and is greater than either the radiative recombination or three-body recombination rate coefficients （the number of free electrons per unit is 10^21 cm^3） for the ease of Te 〉 1 eV. Therefore, DR can strongly influence the ionization balance of laser produced multi-charged tin ions. The related dieleetronie satellite cannot be ignored at low temperature Te 〈 5 eV.     

Raman Investigation of Sodium Titanate Nanotubes under Hydrostatic Pressures up to 26.9GPa

High pressure behavior of sodium titanate nanotubes （Na2Ti2O5） is investigated by Raman spectroscopy in a diamond anvil cell （DAC） at room temperature. The two pressure-induced irreversible phase transitions are observed under the given pressure. One occurs at about 4.2 GPa accompanied with a new Raman peak emerging at 834 cm-1 which results from the lattice distortion of the Ti-O network in titanate nanotubes. It can be can be assigned to Ti-O lattice vibrations within lepidocrocite-type （H0.7Ti1.825V0.175O4＆#12539;H2O）TiO6 octahedral host layers with V being vacancy. The structure of the nanotubes transforms to orthorhombic lepidocrocite structure. Another amorphous phase transition occurs at 16.7 GPa. This phase transition is induced by the collapse of titanate nanotubes. All the Raman bands shift toward higher wavenumbers with a pressure dependence ranging from 1.58-5.6 cm-1/GPa.     

Spectral Hole-Burning of Eu^3＋：Y2SiO5 Crystal at 16 K

By using an Ar^＋ ion laser, a tunable Rh 6G dye laser （linewidth 0.5cm^-1） pumped by the second harmonic of a YAG：Nd laser and a Coherent 899-21 dye laser as light sources and using a monochromator, a phase-locking amplifier and a computer as the data detecting system, we detect the optical properties of Eu^3＋-doped Y2SiO5 crystal. Persistent ,spectral hole burning （PSHB） are observed in the Eu^3＋ ions spectral lines （^5 Do-T Fo transition） in the crystal at the temperature of 16K. For 15mW dye laser burning the crystal for 0.1 s spectral holes with hole width about 80 MHz both at 579.62nm and at 579.82nm are detected and the holes can remain for a long time, more than 10h.     

Large Storage Window in a-SiNx/nc-Si/a-SiNx Sandwiched Structure for Nanocrystalline Silicon Floating Gate Memory Application

An a-SiNx/nanocrystalline silicon [（nc-Si）/a-SiNx] sandwiched structure is fabricated in a plasma enhanced chemical vapour deposition （PECVD） system at low temperature （250℃）. The nc-Si layer is fabricated from a hydrogen-diluted silane mixture gas by using a layer-by-layer deposition technique. Atom force microscopy measurement shows that the density of nc-Si is about 2 ×10^11 cm^-2. By the pretreatment of plasma nitridation, low density of interface states and high-quality interface between the Si substrate and a-SiNs insulator layer are obtained. The density of interface state at the midgap is calculated to be 1 ×10^10 cm^-2eV^-1 from the quasistatic and high frequency C - V data. The charging and discharging property of nc-Si quantum dots is studied by capacitance-voltage （C- V） measurement at room temperature. An ultra-large hysteresis is observed in the C - V characteristics, which is attributed to storage of the electrons and holes into the nc-Si dots. The long-term charge-loss process is studied and ascribed to low density of interface states at SiNx/Si substrate.     

Ablation of transparent solids during self-limited deposition of diamond-like films from liquid hydrocarbons

A novel effect is studied of self-limitation of the diamond-like film thickness during laser irradiation of the interface of transparent substrates with liquid aromatic hydrocarbons. The interface is exposed through the transparent substrate to radiation of a copper vapor laser (wavelength of 510.6 nm, pulse duration of 20 ns). The thickness of diamond-like film increases linearly to 80-100 nm with the number of laser pulses and then saturates, while the substrate is ablated with nearly constant rate. This ablation rate depends on the thermal expansion coefficient of the substrate (glass, fused silica, sapphire, or CaF₂). The absorption of extinction coefficient of deposited films measured by ellipsometry is of order of 10⁴ cm^-1 and is sufficient to cause the significant heating of the interface. The ablation of the transparent substrates is due to their unequal thermal expansion compared to the diamond-like film having different thermal expansion coefficient. The measured ablation rates scale from 0.2 Å/pulse for glass to 4.5 Å/pulse for CaF₂. A 7m spatial resolution of the ablation process has been demonstrated for fused silica.     

Cubic boron nitride deposition on silicon substrates at room temperature by KrF excimer laser ablation of h-BN

A hexagonal-BN target was ablated by high-fluence (6 and 12 J/cm²) KrF excimer laser pulses in low-pressure (5 Pa) N₂ atmosphere, without any aid of ion bombardment and heating of the Si substrate. Investigations of the deposited films show that the cubic-BN phase was deposited. The film deposited at 6 J/cm² appears to contain a higher cubic phase content with respect to the one deposited at 12 J/cm².