Theoretical Investigation of Femtosecond-Resolved Photoelectron Spectrum of NaI Molecules

The time-resolved photoelectron spectra （TRPES） of NaI molecules are calculated by using the time-dependent wave packet method. Two different potential energy curves （adiabatic and diabatic） are adopted in the simulation. The third peak of the photoelectron spectra presented in the adiabatic calculation is induced by the reflection of the wave packet. The oscillating of the wave packet onto the diabatic energy curve is a decreasing process. The comparison of the photoelectron spectra between the two different calculations （adiabatic and diabatic） is presented.     

Theoretical Investigation of Femtosecond-Resolved Photoelectron Spectra of the Li2 Molecule

The time-dependent quantum wave packet method is used to investigate the dynamics for the Li2 molecule, and the time-resolved photoelectron spectra （TRPES） of the Li2 molecule are calculated. At the short delay time, the particular phenomenon of TRPES with four peaks is qualitatively interpreted in a dressed state picture by analyzing wave packet motion on light-induced potential （LIP）. The significant difference in the electronic structure of E1∑g^＋ between the inner and outer turning points has an impact on the TRPES. The control for the first excited state A1∑u^＋ of the initial wave packet is discussed.     

Probing Wave Packet Dynamics of I2- Anions with Pump--Probe Femtosecond Spectroscopy

The wave packet dynamics of I2^- anions is studied by using the time-dependent wave packet method. Two conclusions can be drawn from the calculations. First, the period of the total photoelectron signal oscillating with the propagation of delay time is about 750fs. Second, the photoionization of I2^- anions begin at the time 600 fs, and the time needed for the population of the electronic state of I2 neutral molecule to reach the maximum becomes shorter with the increasing delay time.     

Autler-Townes Splitting in Photoelectron Spectrum of Three-Level Li2 Molecule in Ultrashort Pulse Laser Fields

The Autler-Townes （AT） splitting in femtosecond photoelectron spectrum of three-level Li2 molecules is theoretically investigated using time-dependent quantum wave packet method. With proper femtosecond laser pulses, three peaks of the AT splitting can be observed in the photoelectron spectrum. The AT splitting stems from rapid Rabi oscillation caused by intense ultrashort laser pluses. The effects of laser parameters on the molecular ionization dynamics are also discussed.     

A Theoretical Study of Photoabsorption Cross Sections of Na^＋ 2

In the framework of quantum defect theory, we calculate photoabsorption cross sections of Na^＋ 2. Based on our calculations, there is an absorption window in the photoabsorption cross sections of Na^＋ 2. and more than one bump above the absorption window. The calculated photoabsorption cross sections provide an explanation for the abnormal bump in the experimental measurements of Hudson, which is a long-standing experimental puzzle.     

Theoretical Study of the Influence of Femtosecond Laser Wavelength on the Evolution of a Double-Minimum Electronic Excited State Wave Packet for NaRb

Employing the two-state model and the time-dependent wave packet method, the influence of femtosecond laser wavelength on the evolution of the double-minimum electronic excited state wave packet is numerically investigated. For different laser wavelengths, evolutions of the double-minimum electronic excited state wave packet with time and internuclear distance are different. One can control the evolution of the wave packet by varying the laser wavelength appropriately, which will benefit the light manipulation of atomic and molecular processes. Furthermore, study of the dynamics of the NaRb molecule may yield clues to creating an ultracold molecule.     

Frequency measurement of130Te2 resonances near 467 nm

Precision spectroscopy on molecular tellurium is performed by measuring the frequency difference between the observed lines and an eigenfrequency of a high-finesse cavity mode. The mode frequency is derived from a measurement of the cavity's free spectral range taking into account the cavity dispersion due to phase shifts in the dielectric mirror coatings. The experimental technique is based on dual frequency modulation and is applied to determine the transition wavenumbers of several lines in¹³⁰Te₂ near 467 nm with an uncertainty of 2 × 10^–8.     

A Theoretical Study of Super-Excited States of F2

In the framework of quantum defect theory, we study super-excited states of F2 molecules which can dissociate into F^＋ （^3P2,1,0） and F^-（^1 So） ion-pair. Based on our calculation, we present a vibrational resolved assignment of the high precision photofragment yield spectra for F^- from the F2 ion-pair production.     

Photoelectron angular distributions of molecules in bichromatic laser fields of circular polarization

Photoelectron angular distributions (PADs) from above-threshold ionization of O₂ and N₂ molecules irradiated by a bichromatic laser field of circular polarization are studied. The bichromatic laser field is specially modulated such that it can be used to mimic a sequence of one-cycle laser pulses. The PADs are greatly affected by the molecular alignment, the symmetry of the initial electronic distribution, and the carrier-envelope phase of the laser pulses. Generally, the PADs do not show any symmetry, and become symmetric about an axis only when the symmetric axis of laser field coincides with the symmetric axis of molecules. This study shows that the few-cycle laser pulses can be used to steer the photoelectrons and perform the selective ionization of molecules.     

Control of the photodissociation of CsCl

A femtosecond UV laser pulse is used to resonantly excite CsCl molecules from the ionically bound ground state to the first excited repulsive state. The excitation leads to the dissociation of CsCl. After a certain time delay a visible (VIS) femtosecond laser pulse interrupts the dissociation process by resonantly de-exciting the molecule back to the ground state. According to the Tannor–Rice control scheme, the fraction of dissociated CsCl molecules is controlled by changing the delay time between the two fs laser pulses. The processes involved are investigated theoretically and experimentally. Based on the results, a self-learning system has been realized, which is able to control the dissociation without any a priori knowledge of the molecule. Received: 2 December 1999 / Published online: 24 July 2000     

Structural Deformation of CO22+ in Intense Femtosecond Laser Fields

The angular distributions of CO^＋ from the dissociation of CO2^2＋ and CO2^＋ in intense femtosecond laser fields （45 fs, about 5 × 10^15 W/cm^2） are studied at a laser wavelength of 800nm based on the time-of-flight mass spectra of CO^＋ fragment ions. The experimental results show that structural deformation occurs in the charge state of CO2^2＋ and the CO^＋ maintains linear geometrical structure.     

Spectroscopy of Te2 with modulation transfer: Reference lines for precision spectroscopy in Yb+ at 467 nm

Modulation-transfer spectroscopy is used to observe resonances in ¹³⁰Te₂ near 467 nm. A signal-to-noise ratio of 500 is obtained with 1 mW laser power and with a time constant of 10 ms; the lineshapes are investigated in detail for different demodulation phases. The signal can be used to servolock a blue dye ring laser at 467 nm on a ¹³⁰Te₂ resonance which serves as reference line for precision spectroscopy on single, trapped Yb⁺ ions at 467 nm.     

Improvement of Atomic-Layer-Deposited Al2O3/GaAs Interface Property by Sulfuration and NH3 Thermal Nitridation

Fermi level pinning at the interface between high-h gate dielectric and GaAs induced by unstable native oxides is a major obstacle for high performance GaAs-based metal-oxide-semiconductor （MOS） devices. We demonstrate the improved Al2O3/GaAs interracial characteristics by （NH4）2S immersion and NH3 thermal pretreatment prior to A1203 deposition. X-ray photoelectron spectroscopy （XPS） analysis confirms that sulfuration of GaAs surface by （NH4 ）2S solution can effectively reduce As-O bonds while Ga-O bonds and elemental As still exist at Al2O3 /GaAs interface. However, it is found that N incorporation during the further thermal nitridation on sulfurated GaAs can effectively suppress the native oxides and elemental As in the sequent deposition of Al2O3. Atomic force microscopy （AFM） shows that the further thermal nitridation on sulfurated GaAs surface can also improve the surface roughness.     

On the angular dependence of gaps in 1-D Si/SiO2 periodic structures

A multilayer of silicon and silicon dioxide was used to study the angular dependence of reflectance maxima originating from interference and bulk optical properties. Silicon dioxide has a lattice resonance in the infrared causing an interval of high reflectance for wavelengths around 9 μm. The multilayer was designed such that the interference maxima do not overlap/interact with the material related reflectance maximum. In this way the different angular behavior for the two types of reflectance maxima can be studied simultaneously. Experimental and calculated reflectance spectra for s- and p-polarized light for angles of incidence between 0° and 90° collected for every 5° are presented. The reflectance features caused by interference generally move to shorter wavelengths with increasing angle of incidence, and the materials related peak is widened for (s-polarized light) and excitation of the longitudinal modes was observed for p-polarized light.     

Field-induced ionization and Coulomb explosion of nitrogen

Femtosecond-laser field-induced ionization and Coulomb explosion of diatomic nitrogen were systematically investigated using time-of-flight mass and photoelectron spectrometry. Both linearly and circularly polarized femtosecond laser pulses were used at intensities varying from 5×10¹³ to 2×10¹⁵ W/cm². Strong N₂ ⁺, N₂ ²⁺, N⁺, N²⁺ and N³⁺ ion signals were observed for horizontally polarized pulses. Moreover, signals from the atomic ions exhibited a double-peak structure. Suppression of ionization was observed for circularly polarized pulses, while for vertically polarized pulses, only N₂ ⁺ and N₂ ²⁺ ions were observed. The angular distributions of the ions were measured under zero-field conditions in the ionization zone. The atomic ions N⁺, N²⁺ and N³⁺ exhibited highly anisotropic distributions, with maxima along the laser polarization vector and zeroes normal to the laser polarization vector. In contrast to the atomic ions, N₂ ⁺ exhibited a strong isotropic angular distribution. These observations indicate that dynamic alignment is responsible for the observed anisotropic angular distribution of the atomic ions. The kinetic energy spectrum of the photoelectrons is featureless and broad, extending above the ponderomotive potential of the laser pulse. The angular distribution is markedly anisotropic, with a maximum along the laser polarization vector. These observations further support the notion that the field-ionization mechanism is dominant under our experimental conditions. Received: 29 January 2002 / Revised version: 15 March 2002 / Published online: 12 July 2002     

Optical Transmittance and Band Gap of Ferroelectric BaTi2O5 Bulk Glass

Optical transmittance and reflectance on ferroelectric BaTi₂O₅ glasses prepared recently by a containerless synthesis technique are measured at room temperature in the wavelength range 190-800nm. The fundamental absorption edge located around 340nm demonstrates the colourless and transparent character of the glass. The optical band gap of 3.32eV has been estimated. The tail of the optical absorption near the fundamental absorption edge is found to follow the Urbach rule. Our analysis of the experimental spectra supports an indirect allowed interband transition between the valence band formed by O-2p orbitals and the conduction band formed by Ti-3d orbitals.     

First-Principles Study of Electronic Structure of the Laves Phase ZrFe2

We perform the ab initio calculation for obtaining the density of states and magnetic properties of ZrFe2 Laves phase compound based on the method of augmented plane waves plus local orbital The results indicate that the ferromagnetic state is more stable than the paramagnetic one, but with a slightly larger volume. The 3d - 4d exchange interactions between Fe and Zr electrons lead to the antiparallel coupling for Fe 3d and Zr 4d states, which is responsible for the ferrimagnetic ordering of the compound. The resulting magnetic moment of about 1.98μB for Fe is spatially localized near the Fe site, while around Zr a small but extended negative spin states causes a moment of about -0.44 μB. Moreover, the resulting magnetic moments with the generalized gradient approximation are more consistent with experimental values than that of the local-spin density approximation.     

Resonant two-step photoionization of molecules: Effects of pulse sequence,pulse duration and delay time of two lasers on ionization probability and selectivity

Using rate equations the effect of different pulse sequences, pulse durations, and delay times of two lasers on ionization probability and selectivity in resonant two-step photoionization of molecules is investigated. The results demonstrate to what extent a given selectivity of the absorption or relaxation of the intermediate electronic, state is influenced by a special combination of these parameters.     

Above-Threshold Dissociation of HD+ in Femtosecond Laser Field

The above-threshold dissociation （ATD） of the HD＋ molecular ion in femtosecond laser field is investigated theoretically. The energy-dependent distribution of the dissociated fragments is calculated using an asymptoticflow expression in the momentum space. The calculations show that the ATD of HD＋ is sensitive to the initial vibrational level of ground electronic state. Multiphoton ATDs can be observed in the dissociation processes. The dynamics phenomena are interpreted by using the concept of light-dressed potential.     

An Efficient Pulsed CH3OH Terahertz Laser Pumped by a TEA CO2 Laser

An efficient pulsed CH3OH terahertz （THz） laser pumped by a TEA CO2 laser is investigated experimentally. To improve photon conversion efficiency and THz laser energy, two cavity configurations of the TEA CO2 laser, which is external and semi-external, are evaluated. The pump intensities are about 4.7 MW/cm2 and 1.2 MW/cm2, respectively. Higher pump intensity and more stable single lines are obtained in the external cavity. For the 3.8 J pump energy of the 9P（16） transition in the external cavity, the maximum terahertz output energy with 570.5 μm wavelength at 160 Pa is 431 μJ. With a 6 J energy pulse in terms of a semi-external cavity, a 353 μJ terahertz emission （570.5 μm） is produced. The corresponding photon conversion efficiencies are 1.36% and 0.705%, increasing by a factor of about 2.