Lasers excited by photodissociation: The thalliumiodide laser

This review is concerned with lasers excited by photodissociation of molecules. The principle of photolytic excitation is described and a number of existing lasers is presented. As an example the properties of the thallium laser such as spectral and temporal emission, achievable gain and efficiency are discussed in detail.     

Circular dichroism in radiative and nonradiative inelastic XUV scattering

Accepted: 6 March 1997     

The effect of an external magnetic field on the <Emphasis Type="Italic">L</Emphasis><Subscript>3</Subscript> subshell fluorescence yields and level widths for Ta,W, Tl,Th and U at 59.54 keV photons

The effect of an external magnetic field on the L₃ subshell fluorescence yields (ω₃ ) and level widths ($\Gamma_{L_3}$) for paramagnetic Ta, W, Tl, Th and U have been investigated using the 59.54 keV incident photon energy in the external magnetic field of intensities ±0.60 T. L₃ X-ray fluorescence cross sections ($\sigma_{L_3}^{X}$) have been measured for the same elements. The measured ω ₃, $\Gamma_{L_3} $ and $ \sigma_{L_3}^X$ values for B = 0 are in good agreement with the theoretical values. It was observed that the values of $\sigma_{L_3}^X$ and ω₃ with the applied magnitude of the magnetic field in both directions show a decreasing trend for paramagnetic Ta, W, Tl, Th and U. Furthermore, in the presence of an external magnetic field, the values of $\Gamma_{L_3}$ show an increasing trend for the same elements. The results show that the atomic parameters such as spectral linewidth, radiation rates, photoionization cross section and fluorescence yield can change when the irradiation is conducted in a magnetic field.     

Three-photon interference spectra in four-level atomic systems

We have considered the interference spectra that occur at the three-photon generated frequency arising from the interaction of three laser fields with a four-level atom, where two of the laser fields are on two-photon resonance with the three levels forming a “λ” scheme while the third laser operates between the second ground and the second excited state of the atom. At low intensities of all three laser fields, the overall intensity of the peak at the three-photon generated frequency, describing the spectrum of an electron in the second excited state, depends on the strength of the combined field of the two laser fields that are on two-photon resonance and it takes negative values. This indicates that light amplification without population inversion is likely to occur at the three-photon generated frequency. The combined field of the three laser fields induces multiphoton excitations near the three-photon generated frequency, whose peaks are characterized by linewidths which are much less than the natural linewidths of the atoms. These excitations describe absorption or stimulating emission processes depending on the values of the detunings of the laser fields. The derived results are graphically presented and discussed. Received: 24 January 2001 / Published online: 8 June 2001     

The second Born approximation in electron-helium scattering in a Nd-YAG laser field

The dynamics of laser-assisted elastic collisions in helium is studied using the second-order Born approximation. Detailed calculations of the scattering amplitudes are performed by using the Sturmian basis expansion. Differential cross sections for elastic scattering with the net absorption/emission of up to two photons are calculated for collision energies of 5 eV, 10 eV, and 20 eV. We discuss the influence of the low-energy electrons on the differential cross section (DCS) as a function of the scattering angle for selected choices of the laser frequency and the number of photons exchanged between the external field and electron-helium system.     

Spectroscopic studies of laser induced aluminum plasma using fundamental,second and third harmonics of a Nd:YAG laser

In the present work, we have studied the spatial evolution of the aluminum plasma produced by the fundamental (1064 nm), second (532 nm) and third (355 nm) harmonics of a Q-switched pulsed Nd:YAG laser. The experimentally observed line profiles of neutral aluminum have been used to extract the excitation temperature using Boltzmann plot method whereas the electron number density has been determined from the Stark broadened profiles. Besides we have studied the variation of excitation temperature and electron number density as a function of laser irradiance at atmospheric pressure. In addition, we have performed quantitative analysis of photon absorption and vapor ionization mechanism at three laser wavelengths and estimated the inverse bremsstrahlung (IB) absorption and photoionization (PI) coefficients. The validity of the assumption of local thermodynamic equilibrium is discussed in the light of the experimental results.     

Atomic spectroscopy with squeezed light for sensitivity beyond the vacuum-state limit

A frequency tunable source of squeezed light has been developed which is suitable for a variety of spectroscopic applications. In initial experiments continuous tunability over a range of 2 GHz has been achieved with a directly observed nonclassical noise reduction of 6 dB relative to the vacuum-state limit in a balanced homodyne detector. A process of light-induced absorption in the nonlinear crystal has been identified as the principal loss mechanism which prevents the observation of yet larger degrees of squeezing. Although our source is potentially broadly tunable over the range of wavelengths from 840 to 970 nm, the current research centers on the performance at 852 nm for spectroscopy of the D ₂ line of atomic cesium. For frequency-modulated (FM) saturation spectroscopy in a vapor cell, an improvement of 3.1 dB in sensitivity relative to the usual quantum limit is demonstrated for the detection of Doppler-free resonances. When corrected for the thermal noise of the detector, the enhancement in signal-to-noise ratio brought by the squeezed field is 3.8 dB relative to the shot-noise limit set by the vacuum fluctuations of the probe field.     

Design and interpretation of laser pulses for the control of quantum systems

An extended theory of optimal control strategies for the design of feasible laser pulses is presented. The theoretical framework includes the control of population-transfer and expectation values. Selected studies for two-dimensional model systems providing aspects of uni- and bimolecular reactions are presented. Subsequent analysis of the obtained laser fields is performed to gain insight into the underlying reaction mechanisms. The effect of non-uniform spatial laser profiles and the orientation of the molecules versus the laser beam on controlling quantum dynamics is investigated with the main interest focussed on the achievable quantum yield and information on variable pathways stored in the laser field. Received: 10 November 1999 / Published online: 5 July 2000     

The effect of the homogeneous broadening on the propagation of the light pulses

The propagation of resonant pulses in a two-level homogeneously broadened atomic medium is analyzed. The pulses with the duration comparable with the atomic coherence relaxation time are considered. The effects of the long pulse area stabilization and destabilization are reported. The numerical simulation is performed.     

Two-step laser excitation of the highly excited even-parity states of atomic mercury

We report term energies and quantum defects of highly excited even-parity states of mercury in the 83 876–84 140 cm^-1 energy range, employing a two-step laser excitation scheme via the S₀↦6s6p³P₁ inter-combination transition. Two dye lasers, pumped by a common Nd:YAG laser, were frequency doubled by BBO crystals and used to record the spectra in conjunction with a thermionic diode ion detector. Our new observations include the much extended D₂ (22 ≤n ≤52) series and a few members of the S₁ (24 ≤n ≤30) Rydberg series. Members of the D₂ Rydberg series with such a high n value are reported for the first time. The relative intensities of the D₂ and S₁ transitions (m = 4, 5 and 6) of group II-B elements excited from the P₁ inter-combination states are also discussed.     

Nonlinear optics of chiral surface systems

Differential SHG signals from chiral surfaces are recorded using right and left circularly polarized incident light. We show that chiral information from the surface is conveyed through this SHG process. This study focuses on the model protein system, cytochrome c, adsorbed on various self-assembled mono- and bi-layers at the solid/liquid interface. SHG-CD signals are shown to be related to the oxidation state of the protein and are utilized to observe changes in this feature of the protein in situ at surfaces of varying chemical properties. Received: 20 September 1998 / Revised version: 9 December 1998     

A simple non-perturbative approach of atom ionisation by intense and ultra-short laser pulses

A simple theoretical approach based on Coulomb-Volkov states is introduced to predict ionisation of atoms by intense laser pulses in cases where the effective interaction time does not exceed one or two optical cycles [M. Nisoli et al., Opt. Lett. 22, 522 (1997)]. Under these conditions, the energy distributions of ejected electrons predicted by this non-perturbative approach are in very good agreement with “exact" results obtained by a full numerical treatment. The agreement is all the better that the principal quantum number of the initial state is high. For very strong fields, most electrons are ejected at an energy which is close to the classical kinetic energy that would be transferred to free electrons by the electromagnetic field during the pulse. The power of the present approach appears when keV. In this region, full numerical treatments become very lengthy and finally do not converge. However, the present Coulomb-Volkov theory still makes reliable predictions in very short computer times. Received 19 November 1999 and Received in final form 19 January 2000     

Dark resonance of Cs atoms velocity-selected in a thin cell

We carried out experimental and theoretical research on dark Raman resonances in the absorption of the probe monochromatic wave in a thin vapor cell, whose length is much less than the diameters of probe and coupling laser beams. In this case, only the slow atoms have enough time to settle down to the dark quantum state during a free flight between the end walls of the cell. As a result, a sub-Doppler structure is observed when one sweeps both the coupling and probe laser frequencies keeping the Raman resonance condition. Second harmonic lock-in detection is used to evaluate sharpness of the dark-resonance line. The cell-length dependence of the observed spectral profile is satisfactorily reproduced by the steady-state analysis of the density matrix in which the velocity-dependent transit time effect is taken into account.     

Observations and analysis of resonant laser ablation of GaAs

Laser ablation of solid GaAs samples has been studied using one tunable pulsed dye laser. At relatively low laser power, enhancements of up to several hundred times have been observed in the yield of resonantly ionised Ga using laser wavelengths corresponding to the atomic transition 4² P _1/2-4² D _3/2. The influences of laser power and target geometry, on the ion yield and spectral profile, are discussed. It is argued that the resonant excitation and ionisation processes occur in the gas phase of the atoms ablated from the sample surface, and the observed asymmetric spectral profile results from laser-induced collisional processes, e.g., optical collisions, under conditions of relatively high atomic density in the interaction region. Potential applications are foreseen for resonant laser ablation in trace analysis.     

Line width of an atom laser

We describe the measurement of the line width of an atom laser beam extracted from a Bose–Einstein condensate. Using a novel magnetic resonance imaging technique, we find that the energy width of the atom laser beam is Fourier-limited by the duration of the output-coupling process. Received: 25 July 2002 / Revised version: 28 October 2002 / Published online: 26 February 2003 RID="*" ID="*"Corresponding author. Fax: +41-1/633-1254, E-mail: koehl@iqe.phys.ethz.ch     

Kinetic energy and spatial width of ion clouds in paul traps

The ratio of the mean kinetic energy and the spatial width of ion clouds in Paul traps has been measured. The result is compared with predictions of various models that describe ion cloud dynamics in Paul traps.     

Coherent Control of Population Transfer in Li Atoms via Chirped Microwave Pulses

We demonstrate theoretically that Li atoms can be transferred to states of a lower principal quantum number by exposing them to a frequency chirped microwave pulse. The population transfer of Li atoms from the n = 75 state to n = 70 with more than 90% efficiency is achieved by means of the sequential single-photon △n = -1 transitions. The calculation fully utilizes all of the available orbital angular momentum l states for a given n, and the interference pattern and population evolution dynamics of individual l states are analyzed in detail. Using the time-dependent multilevel approach, we describe the process reasonably well as a sequence of adiabatic rapid passages.     

Energies and widths of triply excited states of lithiumlike oxygen and neon

Seven low-lying triply exited states of lithium-like oxygen and neon are calculated with the multichannel saddle-point and saddle-point complex-rotation methods. The term energies are given for these excited states, along with level shifts and partial Auger widths from dominant decay channels. The mass polarization effect and relativistic corrections are included. The radiative transition rates are also calculated. These results are compared with other theoretical data in the literature. Received: 25 May 1998 / Revised: 28 July 1998 / Accepted: 25 August 1998     

All-optical confinement of ultracold plasma with resonant ions

The solution of the problem of all-optical (nonmagnetic) confinement of ultracold electron-ion neutral plasma based on selective action on plasma ions with quantum transition J=1→J=0 of so-called rectified radiation forces in a strong nonmonochromatic light field is suggested. The presented scheme of the three-dimensional dissipative optical trap for plasma allows one to obtain long-lived ultracold plasma with controlled characteristics. The lifetime of the ultracold plasma in such a trap may exceed considerably (by orders of magnitude) the time of free plasma expansion and the lifetime in the (earlier proposed) optical molasses for the ultracold plasma.