γ-LiAlO2上a面ZnO薄膜的光谱特性研究

利用激光脉冲沉积(PLD)技术在(302)γ-LiAlO₂衬底上成功生长了非极性的a面(1120)ZnO薄膜，光致发光谱(PL)带边发射峰半峰宽仅为115meV.研究了非极性ZnO薄膜光谱特性的面内各向异性，发现随着入射光偏振方向改变，在偏振透射光谱上，吸收边移动了20meV，这与A、B激子和C激子的能量差一致；而在拉曼光谱上，激发光偏振方向的改变导致E₂模式的强度发生明显改变.     

HD+离子在两个超短脉冲激光场作用下的解离几率分布

本文报告HD⁺离子在波长λ=306.7nm的三倍频超短脉冲弱光场E₃和不同延时的二倍频超短脉冲强光场E₂作用下解离几率分布的定量计算结果。E₃和E₂的脉冲宽度均为10fs.E₃先行,E₂延时取0、4、8、12、16、20、24、28fs.计算结果用三维图表出。图中看到,沿相对动量坐标有三个峰,分别位于动量2.1×10^-18、4.4×10^-18、5.8×10^-18g·cm/s处,依次称为1号峰、2号峰、3号峰,位置各是λ=306.7nm的单光子能量、双光子能量、三光子能量消耗于解离能之后离子碎片具有相对动量。据分析,1号峰来源于E₂场引起的受激发射作用。     

Ca掺杂的氧化铍纳米管吸附H2O和NH3的选择传感特

通过密度泛函计算, 借助NH₃和H₂O分子对未掺杂以及钙掺杂的BeO碳纳米管的结构和电传导性进行了研究. 结果发现,NH₃和H₂O分子可以吸附在纳米管侧壁的Be原子上,吸附能分别为约36.1和39.0 kcal/mol. 态密度分析显示BeO纳米管的电传导性在吸附后稍有变化. 对于NH₃和H₂O分子,纳米管表面的钙原子替换Be原子可使吸附能分别增加约7.4和14.7 kcal/mol. 与未掺杂纳米管不同的是,钙掺杂BeONT吸附NH₃和H₂O分子的电传导性更加敏感,且H₂O分子比NH₃分子更敏感.     

退火对He注入及随后208Pb27+辐照的Al2O3单晶PL谱的影响

利用高能离子研究了110 keV 的He⁺注入Al₂O₃单晶及随后230 MeV的²⁰⁸Pb²⁷⁺辐照并在不同温度条件下退火样品的光致发光的特性. 从测试结果可以清楚地看到在375 nm，390 nm，413 nm 和450 nm 出现了强烈的发光峰. 经过600 K退火2 h后测试结果显示，390 nm发光峰增强剧烈，而别的发光峰显示不明显. 在900 K退火条件下，390 nm的发光峰开始减弱相反在510 nm出现了较强的发光峰，到1100 K退火完毕后390 nm的发光峰完全消失，而510 nm的发光峰相对增强. 从辐照样品的FTIR谱中看到，波数在460—510 cm^-1间的吸收是振动模式，经过离子辐照后，吸收带展宽，随着辐照量的增大，Al₂O₃振动吸收峰消失，说明Al₂O₃振动模式被完全破坏. 1000—1300 cm^-1之间为Al-O-Al桥氧的伸缩振动模式，辐照后吸收带向高波数方向移动. 退火后的FTIR谱变化不大.     

非对称方势阱中的激子及其与声子的相互作用

采用类LLP(Lee-Low-Pines)变换和分数维变分法,在讨论有限深非对称方势阱Ga_1－xAl_xAs/ GaAs/Ga_0.7Al_0.3As的分数维基础上,计算了其中激子的基态能量以及声子对其影响,随着势阱宽度增加,激子能量先减小后增大,出现一个最小值.讨论了一侧势垒高度变化对分数维、激子基态能量的影响,并发现声子作用使得激子能量明显增大.另外,非对称方势阱中的激子结合能随阱宽的减小而增     

50MeV/u 12C离子实验靶区出射中子角分布实验测量

本文用氟和碳阈探测器对50MeV/u ¹²C离子引起的重离子反应实验靶区E_n>11MeV和E_n>20MeV中子的角分布进行了实验测量,结果显示出明显的前冲分布,较高能量的中子具有更强的前冲趋势.     

供电子能力对一类热活化延迟荧光分子反系间窜越速率的影响

本文基于第一性原理,研究了八个热活化延迟荧光分子的性质,揭示了基团供电子能力对分子几何构型、跃迁属性以及反系间窜越过程的影响.研究结果表明,对于咔唑和氧杂蒽酮组成的一类分子的最低三重激发态（T₁）而言,供体基团的二苯胺取代,几乎不会改变供体和受体之间的夹角,但却可以减小供体和受体间的键长.基团供电子能力越强,最高占据分子轨道（HOMO）和最低未占据分子轨道（LUMO）间的轨道重叠度越小,最低单重激发态S₁和T₁之间的能差（△E_S1-T1）越小.此外,供体基团上增加二苯胺能够增加HOMO的离域性,而且能够进一步地减小△E_S1-T1.通过计算S₁和T₁之间的旋轨耦合系数（H_so）,发现（<S₁|Ĥ_so|T₁>²）/（△E_S1-T1²）数值越大,反系间窜越速率越大.计算表明八个分子都可能是高效的热活化延迟荧光分子.本文提出了一条高效热活化延迟荧光分子的设计策略,即分离HOMO和LUMO的分布和增加HOMO的离域性能够有效地减小S₁-T₁能差.     

羟基碳纳米管吸附SF6放电分解组分的DFT计算

本文根据密度泛函理论(density functional theory , DFT), 采用MS分子动力学仿真软件对羟基修饰的单壁碳纳米管(SWNT-OH) 吸附SF₆局部放电分解的四种主要组分SOF₂, SO₂F₂, SO₂和CF₄进行了详细的理论计算, 通过分析气体分子和SWNT-OH的前线轨道, 吸附过程中吸附能、电荷转移量和电子态密度的情况, 以及吸附前后SWNT-OH能隙的变化, 评判了SWNT-OH对气体分子的敏感性和选择性, 给出了SWNT-OH是否可以制备气体传感器检测SF₆局部放电分解组分的理论依据.     

封装椭圆形C70的手性纳米管的理论表征

应用第一性原理计算,研究了椭圆形的C₇₀分子在碳纳米管中的可能取向．采用(14,7)单壁纳米管为原型材料,发现纳米管和C₇₀分子的弱化学相互作用是决定分子取向的决定因素．通过模拟扫描隧道显微镜图像和计算光学性质,发现封装的椭圆体C₇₀分子的局域电子结构敏感地依赖于分子取向     

甲醇在Pt (100)表面吸附与解离的第一性原理研究.

采用基于第一性原理的密度泛函理论结合周期模型方法对甲醇在Pt(100)完整表面的吸附与解离进行了研究. 通过比较不同吸附位置的吸附能与构型参数发现,表面top吸附位为最稳定吸附位,甲醇分子通过氧原子吸附于Pt(100)表面. 同时计算了甲醇分子在top吸附位可能的解离路径,发现在解离过程中OH键首先断裂的路径为最低能量路径. 分解生成的若干产物其吸附稳定性排序为CH₃O>CH₂OH>CH₃>CH₂O.     

Kinetics of radiation cooling of fullerenes

Emission from fullerene molecules excited by means of electron impact in crossed beams under conditions of single collisions between electrons and C₆₀ molecules in a kinetic energy range E _e from 25 to 100 eV was studied experimentally. Emission spectra in a wavelength range from 300 to 800 nm; the emission excitation functions and the temperature of emitting molecules as a function of E _e were measured with a resolution of 1.6–3.2 nm. The contribution to emission from ionized C ₆₀ ^+* molecules has been determined and data on the emissivity of the C ₆₀ ^+* ion have been obtained. It has been shown that the emission spectra can be well approximated with the spectral distribution of thermal emission from a black body (Planck’s formula), taking into account the lowering of emissivity for a small particle. The emission can be observed starting with electron energy of about 27 eV; the emission excitation function is of a nonresonant form, peaking at an energy of E _e ≈70 eV. As E _e is increased, the temperature of emitting particles rises and reaches its maximum value of 3100–3200 K at E _e ≈47 eV.     

Multiphoton Spectroscopy

Abstract

Absorption and cmission spectroscopies, which are widely utilized by chemists, can be classified as one–photon spectroscopy. A molecule is excited from its ground state of energy E₀ to thc excited state of E_e by the absorption of one photon of frequency given by the Bohr's condition (hω=E_e-E₀). The reverse transition is accompanied by the emission of one photon of the same frcquency. Therefore, the molecular state energies can be directly obtained by the photon encrgies absorbed or emitted. Infrared, microwave, electronic absorption, and emission spectroscopies belong to this category of one–photon spectroscopy.     

使用时间切片离子速度成像技术研究CF2Cl2光解动力学

本文使用时间切片离子速度成像技术结合共振增强多光子电离技术研究了CF₂Cl₂分子在235 nm附近的光解动力学. 通过测量CF₂Cl₂分子在235 nm附近单光子解离产生的氯原子影像,直接得到了解离产物的速度分布和角分布. 激发态氯原子的速度分布包含高动能组分和低动能组分,分别对应³Q₀电子态的直接解离和由于内转换引起的基态预解离. 基态氯原子的速度分布也包含高动能组分和低动能组分,分别对应³Q₀与¹Q₁电子态的预解离和由于内转换引起的基态预解离. 自由基解离通道被确认,二次解离通道和三体解离通道被排除.     

Effect of tube radius on the exohedral chemical functionalization of boron-nitride zigzag nanotubes with NH3

The interaction between zigzag BNNTs with chirality index n=3–10 and ammonia has been studied at the level of B3LYP/6-31G^?. Ammonia can be chemically adsorbed on (3,0) to (7,0) BNNTs and physically adsorbed on other studied BNNTs. From NBO analysis charge transfer occur from NH₃ to BNNTs and change in the natural electron configuration of B atom of BNNTs at adsorption site for the (3,0) and (4,0) BNNTs cases is larger than others. The DOS result show that after functionalization of BNNTs with NH₃ molecules electronic properties of tubes are largely preserved and can be viewed as some kind of harmless modification. Electronic analysis revealed that the interaction of zigzag BNNTs with ammonia is more electrostatic (ionic) in nature, rather than the sole covalent and electrostatic nature increased with increasing of tube diameter.     

抛物量子点中强耦合磁双极化子内部激发态性质

基于Lee-Low-Pines幺正变换,采用Pekar类型变分法研究了抛物量子点中强耦合磁双极化子的内部激发态性质,当考虑自旋和外磁场影响时,推导出二维量子点中强耦合磁双极化子基态的能量E0,声子平均数ˉN0以及第一激发态的能量E1,声子平均数ˉN1随量子点受限强度ω0,介电常数比η,电子-声子耦合强度α和磁场的回旋共振频率ωC的变化规律.结果表明,磁双极化子的基态能量E0和第一激发态能量E1由两电子的单粒子能量E E,两电子间库仑相互作用能E C,电子自旋与磁场相互作用能E s和电子-声子相互作用能E e-ph四部分组成;单粒子"轨道"运动与磁场相互作用导致了第一激发态能级E1分裂为E(1+1)1,E(1-1)1两条,而电子自旋-磁场相互作用的效应又使基态和第一激发态的各能级均产生了三条"精细结构";ˉN0和ˉN1随ω0,α和ωc的增加而增大,E e-ph的取值总是小于零,其绝对值随α,ω0和ωc的增加而增大;电子-声子相互作用的效应是束缚态磁双极化子形成的有力因素,而限定势和电子之间的库仑排斥能的存在不利于束缚态磁双极化子的形成;能量为E(1-1)1的磁双极化子要比能量为E(1+1)1的磁双极化子更容易且更稳定地处于束缚态.     

A simple method for surface and ultrathin film characterization

The method depends on monitoring variations of secondary electron emission as a function of changes in surface structure and composition. By measuring the crystal current i_cc and its variation with incident beam energy, E, surface changes can be measured rapidly and precisely. The principle of the method is already used qualitatively in secondary electron emission microscopy. If E is adjusted to give zero crystal current (E_zcc), and changes are followed from either variations in i_cc or E_zcc, then the measurements obtained during adorption are comparable to (but can be more precise than) those obtained from Auger spectroscopy. Results are presented for copper surfaces during cleaning cycles and during the adsorption of lead overlayers. Various applications can be envisaged, especially for rapid changes during segregation, diffusion or desorption.     

粉末LaOCl:Eu3+的5D1能级的无辐射跃迁几率

本文使用多次漫反射法测得粉末LaOCl:Eu的漫反射吸收谱,结合所测的LaOCl:Eu的激发光谱,直接得出5D1能级的无辐射量子效率,再由所测5D1能级寿命得出它的无辐射跃迁几率。另一方面,使用Ω参数法,即利用Ω参数计算5D1的辐射跃迁几率,然后由所测寿命值计算出无辐射跃迁几率,来验证第一种方法所得结果。两者结果接近,表明前一种方法是简便可行的。     

Vibrational symmetry classification and torsional tunneling splitting patterns in G6(EM), G12, and G36(EM) molecules

It is shown that the torsional splitting patterns in methanol-like molecules, with the excitation of small amplitude vibrational modes in the methyl group, are determined by mechanisms that can be formulated in an almost identical fashion to that for ethane-like molecules. This is achieved by treating ethane-like molecules by the internal axis method (IAM) and methanol-like molecules by the principal axis method (PAM) or rho-axis method (RAM). Using the extended molecular groups G₆(EM) or C_6v(M) for methanol and G₃₆(EM) for ethane, vibrations perpendicular to the internal rotation axis are conveniently described by modes of higher degeneracy (E for methanol and G_s for ethane) in the absence of coupling of top and frame. Head–tail coupling operators, except the cos-type barrier terms, lower the degeneracy, causing vibrational splittings. Coupled vibrational pairs with torsional splitting patterns that we call ‘regular’ (pure A₁, A₂ pairs for methanol and pure E_1d, E_2d pairs for ethane) or ‘inverted’ (pure B₁, B₂ pairs for methanol and pure E_1s, E_2s pairs for ethane) can be formed as limit cases. Actual splitting patterns occur between the above limits, and are basically determined by torsional Coriolis coupling, which can tune more or less to resonance pairs of uncoupled basis levels linked by specific head-tail coupling operators. The inversion of torsional splitting patterns, observed in perpendicular vibrational modes of the methyl group of methanol, can be predicted by these theoretical considerations. Similar considerations apply to molecules of G₁₂ symmetry.     

Bound exciton luminescence in GaP:Cu,O

Luminescence from Cu,O-diffused high-ohmic p-type GaP crystals exhibits hitherto unobserved complexity in the red spectral region (1.6−1.9 eV). The present investigation concerns the features of three different emission series, denoted by C, E₁ and E₂, simultaneously present in these crystals. From detailed measurements of emission and excitation spectra at different temperatures the properties of any of these emissions could be studied separately. The low-temperature spectra for the two line emission series E₁ (1.78−1.72 eV) and E₂ (1.67−1.62 eV) show strong resemblances to well-known properties of isoelectronic complexes such as, for example, Cd,O in GaP. The featureless broad C emission (1.81 eV) is probably of a similar physical origin as E₁ and E₂, so that all three emissions are believed to originate from excitons bound to different complexes involving Cu and possibly O. Further work to determine the chemical nature of these defects is suggested.     

Delayed ionisation of C70

A delayed ionisation experiment has been carried out on laser excited C₇₀ molecules. Ions and electrons are detected in coincidence to distinguish the ionisation of C₇₀ from that of C₆₈ molecules created by the dominant process, emission of C₂. From the time dependence of the C₇₀⁺ yield and the ratio to the C₆₈⁺ yield, we can deduce both the dissociation energy, E_d = 9.7 ±0.3 eV, and the pre–exponential factor, A_d = 1.7 ×10²⁰ s^-1, in the Arrhenius decay law for C₂ emission. The power of photon emission from neutral C₇₀ is also determined.