<p>The motions of a wavepacket in the two coupled potentials studied in this thesis can be classified into either bistable or astable motion according to the wavepacket interference at the curve crossing. Bistable motion, in which the wavepacket performs a coupled oscillation but remains in the same adiabatic and diabatic state, can exist both in bound-bound systems and bound-unbound ones with long time stability. Astable motion, in which the wavepacket at the curve crossing switches between the adiabatic and diabatic states and thus alternates between the two possible turning points in the unforked part of the motion, can only exist in bound-bound systems on a limited time scale. The motion of a wavepacket under bistable interference conditions exhibits all of the features expected if the wavepacket moved in a single anharmonic potential. The revival time can be predicted from the revival times in the corresponding diabatic and adiabatic potentials. The phenomenon was observed not only in model molecular systems but also in the system of the harmonically trapped ion pumped by an external laser field with standing wave spatial profile.</p><p>In order to study the bias effect of the detector on pump-probe rotational anisotropy measurements, in a specific direction the fluorescence polarization effect was removed by measuring the rovibrational wavepacket with the help of properly oriented polarizer placed in front of the detector. Our results show clearly the necessity to take polarization effects into account in ultrafast pump-probe rotational anisotropy measurements.</p>

The motions of a wavepacket in the two coupled potentials studied in this thesis can be classified into either bistable or astable motion according to the wavepacket interference at the curve crossing. Bistable motion, in which the wavepacket performs a coupled oscillation but remains in the same adiabatic and diabatic state, can exist both in bound-bound systems and bound-unbound ones with long time stability. Astable motion, in which the wavepacket at the curve crossing switches between the adiabatic and diabatic states and thus alternates between the two possible turning points in the unforked part of the motion, can only exist in bound-bound systems on a limited time scale. The motion of a wavepacket under bistable interference conditions exhibits all of the features expected if the wavepacket moved in a single anharmonic potential. The revival time can be predicted from the revival times in the corresponding diabatic and adiabatic potentials. The phenomenon was observed not only in model molecular systems but also in the system of the harmonically trapped ion pumped by an external laser field with standing wave spatial profile. In order to study the bias effect of the detector on pump-probe rotational anisotropy measurements, in a specific direction the fluorescence polarization effect was removed by measuring the rovibrational wavepacket with the help of properly oriented polarizer placed in front of the detector. Our results show clearly the necessity to take polarization effects into account in ultrafast pump-probe rotational anisotropy measurements.

Only very few molar polarizabilities are known with high accuracy; and when so, they are in general only known at a given wavelength. There is therefore a need to assess the molar polarizability with high accuracy of various gases, at different wavelengths. The molar polarizability of a gas is a measure of the susceptibility of a molecule to have its charge distribution affected by light. It is also the entity that relates the index of refraction to the (molar) density of a gas in Lorentz-Lorenz equation. Hence, for high precision measurements of the density of a gas, it is important to know the molar polarizability of the gas to high accuracy. In this work a GAMOR system has been used to determine the wavelength-dependent molar polarizability of Ar at 1550 nm.  However, a high accuracy assessment of the molar polarizability of a gas requires that the gas density is known with high accuracy. Since this is not trivial to assess, the molar polarizability of argon has been assessed in terms of that of nitrogen, which is assumed to be known with high accuracy. Hence, to minimise measurement errors, the measurement cavity was alternately filled with nitrogen and argon and the ratio between the signals provided by the GAMOR system represents the ratio of the molar polarizabilities of the two gases. It was found that the molar polarizability of argon was  0.94393(5) times that of nitrogen. Since the latter one has been assessed to 4.34828(3) x 10^-6  m^/mol, the molar polarizability of argon could be assessed to 4.10446(5) x 10^-6 m^3/mol.

In the last decades the scientific development has made it possible to produce pulses with durations below the femtosecond time scale (1 fs = 1015 s), reaching to attoseconds (1 as = 1018 s). This is the time scale of electronic motion inside atoms and molecules. One way to produce isolated attosecond pulses is through high harmonic generation in gases with intense few-cycle laser pulses. This process depends strongly on the electric field shape relative to the pulse envelope, which is characterized by the so called carrier-envelope phase (CEP).The goal of this master’s thesis is to measure and investigate the possibility to improve the CEP stability of sub-two-cycle laser pulses from the laser, Light Wave Synthesizer 20 (LWS-20). The first step of the master’s thesis was to modify a Labview program used to evaluate the CEP change to be able to reevaluate the already acquired raw data. The measurements are done with an f-to-2f interferometer, whichis a spectral interference device, which measures the CEP difference between two pulses. The CEP change of the laser system was measured at three positions: after the multi-pass amplifier of the laser front end (MP), after a hollow-core fiber (HCF), which is used for spectral broadening, and at the end of the laser system. The stability is determined as the RMS error (standard deviation) of the phase change overall shots in one sample (lower RMS is better stability). The measurements show an average stability of 160±20 mrad RMS after the MP, 280±31 mrad RMS after the HCF and 560±53 mrad RMS at the end of the system. The stability at the end of the system could be improved to 475±40 mrad RMS after a scan of the pump energy for one of the amplifier stages. The HCF appears to provide a lower limit in stability and influences it only if it is very good after the MP. The alignment of the HCF does also seem to influence the CEP stability and the best stability appears to coincide with maximum output energy. An acousto-optic modulator (Dazzler) has been used to manipulate the CEP change at the end of the system and can thereby compensate for long-term drifts, but the source of the CEP stability degradation at the end of the system should be further investigated.

This text investigates THz-TDS signals in the time-frequency domain. Addi- tionally this text discusses the prospects of using time-frequency analysis to alleviate distortion in THz spectrographic characterizations induced by back- reflections in the free space electro optic sampling used in the THz time-domain spectroscopy detection scheme. THz time domain spectroscopy is a technique for characterization of materials in the terahertz regime. The THz regime offers interesting properties of materials such as strong phonon-photon interaction and resonances for vibration states of molecules. Three time-frequency representations are compared for the analysis of the time-domain signal, the short-time Fourier transform, the Wigner-Ville transform and the continuous wavelet transform. It is concluded that the Wigner-Ville transform is most suited for analysis of the spectral properties of a single pulse due to the Wigner-Ville transforms inherit high spectral resolution. The continuous wavelet transform is most suited for analysis of the time-domain signal since it has no cross-term interference as compared to the Wigner-Ville transform. By masking the continuous wavelet transform with a Lorentzian time-frequency mask the back-reflections are dampened and the resolution of the characterization is improved.

Potassium (K) is the main ash-forming element released from biomass during thermochemical conversion. A better understanding of K chemistry and monitoring of K species is needed to optimize combustion systems. Since K species are highly reactive and prevailing concentrations depend on the conversion conditions, accurate quantification requires in situ measurement techniques. Tunable diode laser absorption spectroscopy with a single-mode distributed feedback laser is used to probe the D1 transition of atomic potassium, K(g), at 769.9 nm. The large current tuning range of the diode laser (5 cm-1) enables monitoringthe wings of the absorption profile. Fitting to the acquired line shape wings is used as astrategy to enhance the dynamic range of the sensor and measure K(g) concentrations even under optically thick condition. A potassium-rich combustion environment is simulated by converting KOH salt in a premixed methane/air flat flame. Quantitative measurements of K(g) are made at 75 positions in the flame. This yields radial K(g) profiles at three different heightsin the plume above the KOH salt and an axial profile at the burner center. The acquired average K(g) concentrations are corrected for effective plume size, i.e. the absorption pathlength determined from the radial profiles. Knowledge of the K(g) distribution in flames can lead to a better understanding of K release and primary reaction kinetics.

In my thesis I describe the improvements of the Penning trap mass spectrometer SMILETRAP. The objective of these improvements have been to increase the reliability and the accuracy with which an atomic mass can be measured using highly charged ions. The improvements have been achieved by stabilizing both the electric and magnetic fields of the trap and by improving the technical performance of the trap system. As a result it has been possible to measure accurately the mass of several atoms ranging from hydrogen to mercury using charge states from 1+ to 52+. It was only possible to use the highest charge states after applying a successful cooling of these ions with Helium during the charge breeding. The technical improvements made a number of interesting accurate mass measurements possible. The measurements of the 3H, 3He, and 4He masses showed that the previously values were wrong. The mass difference between 3H and 3He which is the Q-value of the tritium beta decay has been determined to 18.588(3) keV. The Q-value of the double β-decay of 76Ge was measured at an accuracy of 50 eV. This value is indispensable for the evaluation the Heidelberg-Moscow experiment which aims at finding a possible neutrino-less decay which if present would be a violation of the standard model. The mass ratio of mCs/mp is used to determine the fine structure constant independent of QED calculations. The two decades old anomaly in the mass values of Hg was solved by the mass determination of 198Hg and 204Hg. The mass of 24Mg was measured at an uncertatinty of 0.6 ppb and will be used in the determination of the g-factor of a bound electron in a hydrogen like ions.

No description available.

Due to the unique combination of properties of high intensity and few optical cycle pulse duration, the ultrashort laser pulses have widespread applications in pump-probe spectroscopy and laser-plasma interaction. Correspondingly, it is critical to precisely measure the electric field in the temporal or spectral domain. Since there are no shorter pulses available to sample them in time, it is not easy to characterize few-cycle pulses. In this thesis, the temporal characterization methods including second harmonic generation (SHG) interferometric autocorrelation, single-shot SHG frequency-resolved optical gating (FROG) and chirp scan are used to measure the laser pulses at different positions in our laser system, the Light Wave Synthesizer-20. The SHG interferometric autocorrelation measured a 25.3 fs pulse duration after the kHz frontend laser with a 24.5 fs Fourier limit (FL). The FROG is tested by measuring seed pulses with a 6.5 fs FL providing 6.7 fs pulse duration with mostly flat phase. Then, this FROG apparatus is used to characterize the amplified pulses with a 4.5 fs FL after the whole laser system. The measured pulse duration is 4.5 fs reaching the FL. Similarly, the chirp scan is also used to measure the amplified pluses with a slightly different spectral phase, which retrieved a longer pulse duration of 5.2 fs. The second part of the thesis is focused on contrast improvement. The temporal intensity contrast is reduced in the amplification process leading to a deteriorated laser-plasma interaction. Contrast improvement based on the nonlinear elliptical polarization rotation (NER) technique in a hollow-core fiber (HCF) is implemented and its optimization is performed by using high extinction ratio polarizer, utilizing Ar gas and testing smaller polarization ellipticity (NER angle). The optimal condition is found to be 7° NER angle and 650 mbar Ar in the HCF. Under this optimal condition, sub-4 fs pulses with a smooth spectrum are generated with a power above 30 mW. The NER efficiency is higher than 50%. After amplification to 75 mJ energy with sub-5 fs duration the measured contrast improvement is 3 order of magnitude. In conclusion, the intense few-cycle pulses have been fully characterized by FROG and chirp-scan techniques. Furthermore, the NER method is promising to get cleaned pulses with higher than 3 order of magnitude contrast enhancement.

No description available.