Picosecond time resolved luminescence change upon saturation

A new sensitive method is reported for the measurement of picosecond duration luminescence change upon saturation from photoexcited samples. Examples of 600 ps and 20 ps lifetimes are given.     

Picosecond spectroscopy of dye solutions

Using picosecond spectroscopy technique the rotational relaxation time of rhodamine 4C in solutions both in the ground and excited states is measured to be the same and equal to 250 ps.

While anti-Stokes exciting of non-substituted rhodamine ethanol solution by a single 530 nm picosecond pulse, the blue shift of the gain spectrum on 6 nm over 350 ps after excitation was observed, the process being explained by the orientational solvate relaxation.     

Picosecond spectroscopy of hydrogenated MBE-GaAs

Picosecond-resolved and steady-state photoluminescence at LHe temperature in low-energy ion-gun hydrogenated GaAs/GaAlAs heterostructures are reported. The exciton in the GaAs layer shows an increase in lifetime — up to a factor of 3 — for moderate hydrogenation, followed by a sharp decrease below the value for the untreated sample, for higher H doses. Luminescence efficiency shows a consistent behavior. Incorporation of H generates a strong D-A band falling 64 meV below the gap energy. The behavior for heavy hydrogenation indicates the formation of a new type of deep defect, not ascribed to surface damage, because of the protective GaAlAs layer, plus the fact that the excitonic emission of the latter shows no variation.     

Laser spectroscopy 8. Picosecond processes

Picosecond laser spectroscopy is a rapidly developing field, the applications of which extend to the adjacent subjects of chemistry and biology. Here, the various methods and areas of application are classified and compared. Some experiments and results are mentioned for illustration.     

Picosecond spectroscopy of intermolecular interactions in dye solutions

Some new experimental data on the time development of ultrashort superfluorescence (SF) in the dye solution are presented. The correlation between temporal behaviour change and the change of the spectral and spatial intensity distribution gives direct evidence of the important role of the selffocusing phenomenon in the formation of the ultrashort SF pulse synchronized with the pumping one. The oriental relaxation of solvent molecules in the dye solution not only influences the duration of the dye SF via the selffocusing mechanism but also causes a temporal change of spontaneous emission spectrum. At least two different relaxation times were found in the fluorescence spectrum of the dye in several polar solutions.     

Picosecond luminescence spectroscopy of highly excited GaAs

Time resolved luminescence of highly excited GaAs is studied using a streak camera. We observe the Mott transition from the electron-hole plasma to the excitonic state. This transition is smooth and does not show a phase separation. The plasmon sideband of the electron-hole plasma emission is identified.     

Picosecond infrared spectroscopy of molecules and semiconductors

Novel techniques for infrared spectroscopy on the picosecond time scale are presented. Ultrafast unimolecular reactions in organic molecules are studied by vibrational spectroscopy. The nonlinear infrared absorption of hot carriers in semiconductors is investigated.     

Picosecond spectroscopy of polaritons in anthracene crystals II. Luminescence

The low-temperature luminescence spectrum of anthracene crystals is investigated by applying simultaneous time and frequency resolution. The complicated kinetics of the emission in the polariton bottleneck region reflects directly the evolution and relaxation of the polariton distribution in the crystal. Three distinct relaxation stages are distinguished: (1) the ultrafast decay of initial vibronic excitations, mediated by optical phonons and resulting in a broad distribution of polaritons near the band bottom; (2) the formation of a narrow distribution of polaritons with a characteristic time of 30 ps, which is caused by scattering on acoustic phonons; (3) relaxation through the bottleneck region on a subnanosecond time scale. It is suggested that the polaritons immediately below the resonance frequency are responsible for the observed excitonic energy transfer in anthracene crystals.     

Unidirectional saturation spectroscopy,II

The general probe absorption coefficient derived in Part I is specialized to homogeneous- and inhomogeneous-broadening limits and illustrated as the dipole lifetime is increased from 0 to values comparable to the level lifetimes. This progression reveals the relation between pulsation dips of the short-dipole lifetime limit and the dynamic Stark effect in general. Interpretations of the coherent interactions involved are given in terms of modulator and Raman effects and of dressed atoms. The single-probe unidirectional pulsation dip is shown to be a special case of the grating dip in which the fringe spacing becomes infinite. Analogies with three-level systems are given in which both two and three-level cases are seen to obey an “equal-area theorem”, and to involve level crossing. Some comparison is made with corresponding spectroscopy in which spontaneous emission provides the probe radiation. Work performed as a Humboldt awardee in Germany. Work supported in part by the Space and Missiles Systems Organization, Los Angeles, California. Work supported by the Deutsche Forschungsgemeinschaft     

Laser Stark saturation spectroscopy in methyl alcohol

The method of Lamb dip spectroscopy in Stark tuned molecular gases is discussed and applied to the experimental assignment of methyl alcohol infrared transitions in the ₅ C–O stretch band. Theoretical expressions for Stark Lamb dip patterns are derived for P, Q and R-branch transitions. Stark tuning results and transition quantum number assignments are presented for several 10m transitions, along with measured values of resonant frequencies, absorption coefficients and pressure broadening coefficients.Work supported by the Army Research Office, Durham, and the National Science Foundation.     

Intensities of hyperfine components in saturation spectroscopy

A theory is presented for the intensities of hyperfine components in saturation spectroscopy. We use a diagrammatic approach to nonlinear processes to derive closed-form formulas for the intensities of recoil doublets and of Doppler-generated level crossings. We discuss the influence of the terms introduced by hyperfine coherences in saturation spectroscopy. We also demonstrate spectroscopic stability when the hyperfine splittings are negligible. A catalog of simple formulas is given in view of applications to current spectroscopy and is illustrated by recent examples, including Doppler-free polarization spectroscopy. The extension to other sub-Doppler techniques such as two-photon Doppler-free spectroscopy is outlined.     

Observation of nonstationary effects in saturation spectroscopy

We have studied the nonstationary effects in saturated absorption spectroscopy of the ⁸⁷Rb D₂ line. Varying the size of the σ⁺ polarized pump laser beam, we observed saturated absorption spectra for the σ^± polarized probe beam. For equal polarizations of the pump and probe beams, we found that the resonance signal for the F_g = 1 → F_e = 2 line, and the crossover lines between F_g = 1 → F_e = 2 and F_g = 1 → F_e = 1 (and 0) lines increased to a greater extent than the others. This observation can be understood from the calculated time evolution of the populations of the ground-state sublevels by means of a rate equation model. We also compared experimental data for other conditions with the calculated results. We found good agreement between the calculated results and the data.     

Structure of water-in-oil microemulsions of AOT by infrared spectroscopy

Summary The structure of water in water/AOT/n-heptane reverse micelles has been studied as a function of the [H₂O]/[AOT] ratio (W) by using the absorption IR due to O−H stretching modes in the 3800–3000 cm⁻¹ range. The results show that the IR spectra can be expressed as a sum of contributions from bound- and bulk-like water. The fraction of water in the two ?regions? within the water pool was evaluated as a function ofW. The ?bound? water region seems to hold 3.5 water molecules (corresponding to 7 O−H oscillators) per AOT molecule and its formation is nearly complete atW>6. Paper presented at the I International Conference on Scaling Concepts and Complex Fluids, Copanello, Italy, July 4–8, 1994.     

Picosecond time-resolved X-ray absorption spectroscopy of ultrafast aluminum plasmas

We have used point-projection K-shell absorption spectroscopy to infer the ionization and recombination dynamics of transient aluminum plasmas. Two femtosecond beams of the 100 TW laser at the LULI facility were used to produce an aluminum plasma on a thin aluminum foil (83 or 50 nm), and a picosecond x-ray backlighter source. The short-pulse backlighter probed the aluminum plasma at different times by adjusting the delay between the two femtosecond driving beams. Absorption x-ray spectra at early times are characteristic of a dense and rather homogeneous plasma. Collisional-radiative atomic physics coupled with hydrodynamic simulations reproduce fairly well the measured average ionization as a function of time.     

Xenon saturation spectroscopy by diode laser

Summary Commercial diode lasers have emission wavelengths which overlap some absorption xenon lines. We have performed saturation spectroscopy of four lines, leaving from the first excited atomic configuration 5p ⁵6s, at 823.16 nm, at 828.01 nm, at 834.68 nm and at 820.63 nm, in a weak glow discharge of natural xenon. Natural xenon is a mixture of several isotopes, and the two even isotopes, Xe(129) (26% of relative abundance) and Xe(131) (21%), have a nuclear spin (1/2 and 3/2, respectively) that produces a hyperfine structure. The complex resulting spectra have been resolved and the results are compared with the available literature data. The authors of this paper have agreed to not receive the proofs for correction.     

Picosecond ultrasonics time resolved spectroscopy using a photonic crystal fiber

We present a broadband picosecond ultrasonics time resolved spectroscopy. Detection of picosecond coherent acoustic phonons using a wavelength continuum generation in a photonic crystal fiber (PCF) with femtosecond laser pulses is developed. Measurements are performed for selected wavelengths of a broad wavelength probe pulse within a bandwidth of 250 nm with an 825 nm center wavelength on two samples made of tungsten and of gallium arsenide.     

皮秒级时间分辨超快高能脉冲激光光谱

介绍了一种利用光电摄谱法和条纹管相结合测量ps级时间分辨超快高能脉冲激光光谱的方法。论述了条纹相机工作原理和平面衍射光栅的分光原理,分析指出利用介绍的装置,可以实现波长300 nm ～1 600 nm、脉宽＞2 ps超快高能脉冲激光的光谱测量。采用1 054 nm超快高能脉冲激光器,实验得到了条纹像,对条纹像进行数据处理后得到测量光谱曲线,通过能量标定后,得到了超快高能脉冲激光器实际光谱曲线,验证了ps级时间分辨超快高能脉冲激光光谱方法。讨论了系统中耦合透镜组对光谱测量和光纤色散角对条纹图像的影响,论述了ps级时间分辨超快高能脉冲激光光谱的作用。随着条纹管制造技术的飞速发展,该方法可用于fs级激光光谱的测量。