Influence of laser intensity on the double-resonance multiphoton ionization process of NO molecule

The analytic formula of the ionization efficiency in the process of double resonance enhanced multi-photon ionization （DREMPI） is derived from the dynamic rate equation about the interaction of photon and material. Based on this formula, the ionization efficiency and the laser power index versus laser intensity in the DREMPI process of NO molecule, via A2E and S2E intermediate resonant states, is numerically simulated. It is shown that the ionization efficiency of NO molecule increases with the laser intensity until getting saturation, while the laser power index decreases with the enhancement of the laser intensity and changes to zero at last. The variation of the laser power index with the laser intensity indicates that the ionization efficiency reaches saturation in the one, two, and three excitation steps respectively. It is also found that the narrower the laser pulse duration is, the higher becomes the laser intensity for saturation.     

Ellipticity-dependent ionization/dissociation of carbon dioxide in strong laser fields

Ionization and dissociation of linear triatomic molecules, carbon dioxide, are studied in 50-fs 800-nm strong laser fields using time-of-flight mass spectrometer. The yields of double charged ions CO2+2 and various fragment ions(CO+,O n+, and C n+(n = 1, 2)) are measured as a function of ellipticity of laser polarization in the intensity range from 5.0 ×1013W/cm2 to 6.0 × 1014W/cm2. The results demonstrate that non-sequential double ionization, which is induced by laser-driven electron recollision, dominates double ionization of CO2 in the strong IR laser field with intensity lower than2.0 × 1014W/cm2. The electron recollision could also have contribution in strong-field multiple ionization and formation of fragments of CO2 molecules. The present study indicates that the intensity and ellipticity dependence of ions yields can be used to probe the complex dynamics of strong-field ionization/dissociation of polyatomic molecules.     

Enhanced ionization of vibrational hot carbon disulfide molecules in strong femtosecond laser fields

By using a heated molecular beam in combination with a time-of-flight mass spectrometer, we experimentally study the ionization of vibrational-hot carbon disulfide(CS_2) molecules irradiated by a linearly polarized 800-nm 50-fs strong laser field. The ion yields are measured in a laser intensity range of 7.0 × 10~(12) W/cm~2–1.5 × 10~(14) W/cm~2 at different molecular temperatures of up to 1400 K. Enhanced ionization yield is observed for vibrationally excited CS_2 molecules.The results show that the enhancement decreases as the laser intensity increases, and exhibits non-monotonical dependence on the molecular temperature. According to the calculated potential energy curves of the neutral and ionic electronic states of CS_2, as well as the theoretical models of molecular strong-field ionization available in the literature, we discuss the mechanism of the enhanced ionization of vibrational-hot molecules. It is indicated that the enhanced ionization could be attributed to both the reduced ionization potential with vibrational excitation and the Frank–Condon factors between the neutral and ionic electronic states. Our study paves the way to understanding the effect of nuclear motion on the strongfield ionization of molecules, which would give a further insight into theoretical and experimental investigations on the interaction of polyatomic molecules with strong laser fields.     

Dynamics of Coulomb explosion of hydrogen clusters in a high-intensity femtosecond laser pulse

Using Bethe model, the dynamics of the ionization and Coulomb explosion of hydrogen clusters (0.5-5 nm) in high-intensity (1015 -1017 W/cm2) femtosecond laser pulses have been studied theoretically, and the dependence of energy of protons emitted from exploding clusters on cluster size and laser intensity has been investigated. It is found that the maximum proton energy increases exponentially with the cluster size, and the exponent is mainly determined by the laser intensity. For a given cluster size, the maximum proton energy increases with increasing laser intensity and gets saturation gradually. The calculation results are in agreement with the recent experimental observation.     

Effect of laser polarization on strong-field ionization andfragmentation of nitrous oxide molecules

Ionization of molecules in femtosecond laser fields is the most fundamental and important step of various strong-field physical processes. In this study, we experimentally investigate strong field ionization of linear N_2O molecules using a time-of-flight mass spectrometer in 800-nm laser fields. Yields of the parent ion and different fragment ions are measured as a function of laser intensity in the range of 2.0×10~(13) W/cm~2 to 3.6×10~(14) W/cm~2. We also investigate the dependence of strong field ionization and dissociation of N_2O on laser ellipticity and polarization direction. The significant role of laser induced electron re-collision in the formation of highly charged fragment ions is proved. The physical mechanism of strong field ionization and fragmentation is discussed, based on our experimental results.     

Dynamics of Coulomb explosion of hydrogen clusters in a high-intensity femtosecond laser pulse

Using Bethe model, the dynamics of the ionization and Coulomb explosion of hydrogen clusters (0.5-5nm) in high-intensity (1015-1017 W/cm2) femtosecond laser pulses have been studied theoretically, and the dependence of energy of protons emitted from exploding clusters on cluster size and laser intensity has been investigated. It is found that the maximum proton energy increases exponentially with the cluster size, and the exponent is mainly determined by the laser intensity. For a given cluster size, the maximum proton energy increases with increasing laser intensity and gets saturation gradually. The calculation results are in agreement with the recent experimental observation.     

Ultraviolet laser ionization studies of 1-fluoronaphthalene clusters and density functional theory calculations

This paper studies supersonic jet-cooled 1-fluoronaphthalene(1FN) clusters by ultraviolet(UV) laser ionization at 281 nm in a time-of-flight mass spectrometer.The(1FN) + n(n=1-3) series cluster ions are observed where the signal intensity decreases with increasing cluster size.The effects of sample inlet pressures and ionization laser fluxes to mass spectral distribution are measured.Using density functional theory calculations,it obtains a planar geometric structure of 1FN dimer which is combined through two hydrogen bonds.The mass spectra indicate that the intensity of 1FN trimer is much weaker than that of 1FN dimer and this feature is attributed to the fact that the dimer may form the first "shell" in geometric structure while the larger clusters are generated based on this fundamental unit.     

Ionizations and fragmentations of benzene,methylbenzene, and chlorobenzene in strong IR and UV laser fields

Ionizations and fragmentations of benzene, methylbenzene, and chlorobenzene are studied in linearly polarized 50-fs,800-nm and 400-nm strong laser fields using a time-of-flight mass spectrometer. It is shown that at low laser intensity, the parent ions are dominant for any one of the molecules in an 800-nm strong laser field, while extensive fragmentation is observed in a 400-nm laser field, which can be understood by the resonant photon absorption of molecular cations. The ratio of the yield of the parent ion to the yield of the total ion for each molecule is measured as a function of laser intensity in a range from 1.0 × 1013W/cm2 to 4.0 × 1014W/cm2, in either the 800-nm or 400-nm laser field. The results show that the fragmentation of the aromatic molecules increases significantly as the laser intensity is increased. Possible mechanisms for fragmentation in strong laser fields are discussed. Finally, the saturation intensity of ionization of the titled molecules is also determined.     

Simultaneous measurement of SO2 and NO2 concentration using an optical fiber-based LP-DOAS system

SO2 and NO2 are the most important pollution in atmosphere.An optimized long path(LP)differential optical absorption spectroscopy(DOAS)system of high light intensity at an ultraviolet(UV)wavelength is proposed and used to measure the concentration of SO2 and NO2 simultaneously.In contrast to the traditional DOAS,the system adopted a Y-type optical fiber structure instead of a combination of mirrors in the telescope.The UV light intensity test shows that the light intensity of UV can arrive to above 80% of the max measuring range when the light path reaches 135 m,and the integral time of the spectrograph is only 15 ms.The system is proved to be efficacious through laboratory calibration.The maximum error of SO2 calibration is 4.19%,and is 5.22% for NO2.The error of the SO2 and NO2 mixture calibration is within 10%.Field measurement is implemented in a wastewater treatment plant in winter.The measurement light path is 738 m.The concentration of SO2 varies from 6μg/m^3(2.26 ppb)to 20μg/m^3(7.52 ppb),and the concentration of NO2varies from 100μg/m^3(53.2 ppb)to 200μg/m^3(106.4 ppb)approximately.The results are in accordance with the data from a monitoring station nearby in magnitude order and variation tendency mostly.     

Terahertz emission in tenuous gases irradiated by ultrashort laser pulses

Mechanism of terahertz (THz) pulse generation in gases irradiated by ultrashort laser pulses is investigated theoretically. Quasi-static transverse currents produced by laser field ionization of gases and the longitudinal modulation in formed plasmas are responsible for the THz emission at the electron plasma frequency, as demonstrated by particle-in-cell simulations including field ionization. The THz field amplitude scaling with the laser amplitude within a large range is also discussed.     

Terahertz emission in tenuous gases irradiated by ultrashort laser pulses

Mechanism of terahertz (THz) pulse generation in gases irradiated by ultrashort laser pulses is investigated theoretically. Quasi-static transverse currents produced by laser field ionization of gases and the longitudinal modulation in formed plasmas are responsible for the THz emission at the electron plasma frequency, as demonstrated by particle-in-cell simulations including field ionization. The THz field amplitude scaling with the laser amplitude within a large range is also discussed.     

Nonsequential double ionization of nonaligned diatomic molecules N2 and O2

Nonsequential double ionization (NSDI) processes of nonaligned diatomic molecules N2 and O2 are studied using the S-matrix theory. Our results show that the NSDI process significantly depends on the molecular symmetry and structure. The ratio of NSDI rate to single ionization rate as a function of the field intensity is obtained. It is found that N2 behaves closely with its companion atom Ar in the ratios over the entire intensity range, while O2 exhibits an obvious suppression effect, which is qualitatively consistent with the experiment.     

Photo-acoustic spectrum and detection of nitrogen dioxide

The photo-acoustic (PA) spectrum of nitrogen dioxide (NO2) in the range of 420- 520 nm with a Nd:YAG pumped optical parametric generator and amplifier as radiation source is presented. The spectrum has a characteristic of banded structure superimposed on continuum. The banded structure of the spectrum can be assigned to NO2 B2B1 ← X2A1 transition. While the continual one comes from the chaos states of the first excited state A2B2 and the high vibration levels of the ground state X2A1. The relationship of PA signal with buffer gas pressure and NO2 concentration is measured. The PA signal intensity increases with buffer gas pressure and almost is invariable when the buffer gas pressure is more than 3.00×104 Pa.The PA signal intensity has linearity with NO2 concentration. The detection limit is about 2×10-5 on the basis of SNR = 1, however lower value of the detection limit can be expected by improving the apparatus properties.     

Photo-acoustic spectrum and detection of nitrogen dioxide

The photo-acoustic (PA) spectrum of nitrogen dioxide (NO2) in the range of 420 - 520 nm with a Nd:YAG pumped optical parametric generator and amplifier as radiation source is presented. The spectrum has a characteristic of banded structure superimposed on continuum. The banded structure of the spectrum can be assigned to NO2 B2B1 ←X2A1 transition. While the continual one comes from the chaos states of the first excited state A2B2 and the high vibration levels of the ground state X2A1. The relationship of PA signal with buffer gas pressure and NO2 concentration is measured. The PA signal intensity increases with buffer gas pressure and almost is invariable when the buffer gas pressure is more than 3.00×104 Pa. The PA signal intensity has linearity with NO2 concentration. The detection limit is about 2×10-5 on the basis of SNR = 1, however lower value of the detection limit can be expected by improving the apparatus properties.     

Resonant gradient force on atom interacting with laser field

The gradient force, as a function of position and velocity, is derived for a two-level atom interacting with a standing-wave laser field. Basing on optical Bloch equations, the numerical solutions for the gradient force f⊥,n (n = 0,1, 2,3,4, …) pointing in the direction of the transverse of the laser beam are given. It is shown the higher order gradient force plays important role at strong intensity (G = 64), the contribution of them can not be neglected.     

Cluster-assisted generation of multi-charged ions in nanosecond laser ionization of pulsed hydrogen sulfide beam at 1064 and 532nm

The multi-charged sulfur ions of S^q= (q\le 6) have been generated when hydrogen sulfide cluster beams are irradiated by a nanosecond laser of 1064 and 532,nm with an intensity of 10¹⁰\sim 10¹²W1\cdotcm^-2. S⁶⁺ is the dominant multi-charged species at 1064nm, while S⁴⁺, S³⁺ and S²⁺ ions are the main multi-charged species at 532nm. A three-step model (i.e., multiphoton ionization triggering, inverse bremsstrahlung heating, electron collision ionizing) is proposed to explain the generation of these multi-charged ions at the laser intensity stated above. The high ionization level of the clusters and the increasing charge state of the ion products with increasing laser wavelength are supposed mainly due to the rate-limiting step, i.e., electron heating by absorption energy from the laser field via inverse bremsstrahlung, which is proportional to \lambda ², \lambda being the laser wavelength.     

Simulation of cross-correlation method for temporal characterization of VUV free-electron-lasers

The cross-correlation method for temporal characterization is investigated using simulations of the two- color above threshold ionization （ATI） on He induced by a vacuum ultraviolet （VUV） free-electron laser （FEL） in the presence of an infrared （IR） field. Non-linear dependencies of the sideband structure pro- duced in the two-color ATI process are expressed as a function of IR laser intensity by considering the spatial distributions and temporal jitter of both lasers. The temporal properties of the FEL pulse can be characterized accurately using the cross-correlation method at a low IR laser intensity of ~3~101~ W/cm2 but with low cross-correlation signals. When the dynamic range of sidebands is increased to high IR intensity, the accuracy of the cross-correlation method becomes crucially dependent on the actual non- linear index. An approach of determining this index is proposed here to improve the accuracy of temporal characterizations.     

Double-Exponentially Decayed Photoionization in CREI Effect： Numerical Experiment on 3D H2^＋

On the platform of the 3D H2^＋ system, we perform a numerical simulation of its photoionization rate under excitation of weak to intense laser intensities with varying pulse durations and wavelengths. A novel method is proposed for calculating the photoionization rate： a double exponential decay of ionization probability is best suited for fitting this rate. Confirmation of the well-documented charge-resonance-enhanced ionization （CREI） effect at medium laser intensity and finding of ionization saturation at high light intensity corroborate the robustness of the suggested double-exponential decay process. Surveying the spatial and temporal variations of electron wavefunctions uncovers a mechanism for the double-exponentially decayed photoionization probability as onset of electron ionization along extra degree of freedom. Henceforth, the new method makes clear the origins of peak features in photoionization rate versus internuclear separation. It is believed that this multi-exponentially decayed ionization mechanism is applicable to systems with more degrees of motion.     

FLaser frequency stabilization and shifting by using modulation transfer spectroscopy

The stabilizing and shifting of laser frequency are very important for the interaction between the laser and atoms. The modulation transfer spectroscopy for the 87Rb atom with D2 line transition F = 2 →F＇ = 3 is used for stabilizing and shifting the frequency of the external cavity grating feedback diode laser. The resonant phase modulator with electro-optical effect is used to generate frequency sideband to lock the laser frequency. In the locking scheme, circularly polarized pump- and probe-beams are used. By optimizing the temperature of the vapor, the pump- and probe-beam intensity, the laser linewidth of 280 kHz is obtained. Furthermore, the magnetic field generated by a solenoid is added into the system. Therefore the system can achieve the frequency locking at any point in a range of hundreds of megahertz frequency shifting with very low power loss.     

Laser frequency stabilization and shifting by using modulation transfer spectroscopy

The stabilizing and shifting of laser frequency are very important for the interaction between the laser and atoms. The modulation transfer spectroscopy for the87 Rb atom with D2 line transition F = 2 → F = 3 is used for stabilizing and shifting the frequency of the external cavity grating feedback diode laser. The resonant phase modulator with electro–optical effect is used to generate frequency sideband to lock the laser frequency. In the locking scheme, circularly polarized pump- and probe-beams are used. By optimizing the temperature of the vapor, the pump- and probe-beam intensity, the laser linewidth of 280 kHz is obtained. Furthermore, the magnetic field generated by a solenoid is added into the system. Therefore the system can achieve the frequency locking at any point in a range of hundreds of megahertz frequency shifting with very low power loss.