Nonlinear spectroscopy of antiferromagnetics

ijk and on their phase. One of the hexagonal manganites, YMnO₃ is chosen to demonstrate in detail the experimental methods for obtaining this information. The interference of different contributions is utilized to study domain topography. Received: 26 October 1998     

Topography of antiferromagnetic domains using second harmonic generation with an external reference

2 O₃, in which the time-invariant second-harmonic reference can be generated either intrinsically by the crystal or externally by use of the new technique, so that both methods may be compared. The technique is then used to visualize the domain structure of YMnO₃, an antiferromagnetic crystal which does not provide the time-invariant reference wave intrinsically. The experiments demonstrate the wide applicability of the method. Received: 13 June 1997     

Coupling of ferroelectric and antiferromagnetic order parameters in hexagonal RMnO3

Second-harmonic generation (SHG) is used as a probe for the coexisting ferroelectric and antiferromagnetic orders in hexagonal RMnO₃. SH contributions coupling to the electric and/or magnetic order parameters are identified on the basis of their spectral dependence and the symmetries of the corresponding order parameters. The SH signals from the ferroelectric and antiferromagnetic orders were employed to image the electric and magnetic domain structures separately. The transformation properties of electric and magnetic domains are discussed with respect to the transformation properties of the corresponding order parameters. An investigation of the mutual coupling between the coexisting electric and magnetic orders reveals apparently independent domain structures, which contradicts the symmetry and transformation properties of electric-dipole-induced SHG in this ferroelectromagnetic group of compounds. Apart from higher-order multipole contributions to SHG, interface contributions from clamped electric and magnetic domains can solve the contradiction. Received: 16 October 2001 / Published online: 24 April 2002     

Influence of optical-damage-resistant dopants on the nonlinear optical properties of lithium niobate

Using the chemical-bond method, nonlinear optical properties of lithium niobate containing different dopants are calculated. In crystals with stoichiometric composition the second order nonlinear susceptibility decreases approximately linearly with increasing dopant concentration. Among the dopants studied – Mg, Zn and In – this behaviour is most highly expressed for In doping. In contrast to that, congruently grown crystals show a different behaviour; only a weak dependence on the dopant concentration is found for, for example, Mg-doped material. Received: 24 October 2000 / Published online: 21 March 2001     

All-solid-state cw mode-locked picosecond KTiOAsO4 (KTA) optical parametric oscillator

4 (KTA) optical parametric oscillator (OPO) synchronously pumped by a cw diode-pumped mode-locked Nd:YVO₄ oscillator–amplifier system. The laser system (pumped by 84 W of cw 808-nm diode radiation) generates 7-ps-long pulses at 1.064 μm with a repetition rate of 83.4 MHz and an average power of 29 W. The OPO, synchronously pumped by the 1.064-μm laser pulses, consists of a 15-mm-long KTA crystal (cut for type II noncritical phase-matching) in a folded signal resonant linear resonator. The average powers of the 1.54-μm signal radiation and the 3.47-μm idler radiation are 14.6 W and 6.4 W, respectively. The total OPO output of 21 W corresponds to an internal efficiency of 75%. The experimental investigations include measurements of the OPO output power (and its dependence on the pump power, the transmission of the output coupler, and the resonator length) and of the pulse properties (such as pulse duration and spectral width). The measured results are in good agreement with the predictions of a numerical analysis based on a split-step Fourier method. Received: 4 May 1998     

Surface contribution versus bulk contribution in surface nonlinear optical spectroscopy

Received: 20 September 1998     

Second-harmonic spectroscopy of electronic structure of Si/SiO2 multiple quantum wells

Size effects in the resonant nonlinear optical response of amorphous Si/SiO₂ multiple quantum wells (MQW) are studied by second-harmonic generation (SHG) spectroscopy in a spectral interval of second-harmonic photon energies from 2.5 to 3.4 eV. The sensitivity of SHG spectroscopy to thickness-dependent electronic structure (sub-band energy position and density of states line shape) of MQW is demonstrated. A monotonic red shift of central energies of SHG resonances by 120 m eV upon increase of the well thickness from 2.5 to 10 ? is observed. This is interpreted as a size dependence of the position of singularities in the combined density of states for a 2D gas of electrons moving in an effective potential well. It is shown that, for agreement with experiment, the simplest (rectangular) shape of the well should be modified in order to take into account the lattice-potential distortion at the interfaces. Received: 16 October 2001 / Revised version: 16 April 2002 / Published online: 6 June 2002     

Nonlinear optical properties of (B3O7)5- and (B3O6)3- groups

3 O₅ (LBO) crystal has been studied by using the bond valence theory of complex crystals. Chemical bond parameters and linear and nonlinear optical (NLO) properties of each type of constituent chemical bonds are quantitatively determined. Because of the different crystal structure characteristics of LBO from those of β-BaB₂O₄ (BBO), the two anionic groups, (B₃O₇)^5- in LBO and (B₃O₆)^3- in BBO, play different roles in contributions to their own total NLO tensor coefficients of LBO and BBO, respectively. By comparison, we find that planar (B₃O₆)^3- groups are the ideal structure model, leading to little cancellation of contributions of each kind of bond in these groups, and this gives us a useful guide to design new NLO materials in the future. Received: 24 January 1997/Accepted: 27 March 1997     

Nonlinear optics for surface phase transitions

A general approach of second-harmonic generation (SHG) studies for surface phase transitions (PTs) is presented, with a thermodynamic classification of surface PTs and their relation to SHG parameters. The symmetry aspects of SHG near a surface PT are discussed, including issues connected with separation of surface and bulk contributions and the role of atomic and mesoscopic inhomogeneities. This approach is illustrated by applying it to two systems revealing a (near-) surface PT: single-crystalline SrTiO₃ near a bulk structural PT and single-crystalline Au in an electrochemical cell revealing an order–disorder and a reconstructive PT. Received: 15 January 2002 / Published online: 11 June 2002     

High-resolution magnetic imaging by local tunneling magnetoresistance

We give an overview over our recent efforts of high-resolution magnetic imaging using scanning tunneling microscopy with a ferromagnetic tip. Magnetic sensitivity is obtained on the basis of local tunneling magnetoresistance between a soft magnetic tip and the sample. The magnetisation of the tip is switched periodically with a small coil, leading to variations of the tunneling current due to the tunneling magnetoresistance effect. These variations are detected with a lock-in amplifier to separate spin-dependent parts from the topographic parts of the tunneling current such that the topography and the magnetic structure of the sample can be recorded simultaneously. Crucial for this method is to avoid mechanical vibrations of the tip, that may also lead to variations in the tunneling current. Exemplary studies of polycrystalline Ni and the closure domain pattern of Co(0001) are presented, showing high contrast at acquisition times as low as 3 ms/pixel and a lateral resolution of the order of 1 nm. Further it is demonstrated that besides topography and magnetisation, also local information about the magnetic susceptibility can be obtained. Received: 28 April 2000 / Accepted: 15 May 2000 / Published online: 7 March 2001     

Large magnetoresistance and field-induced transitions in Ni1-xS

Large magnetoresistance (MR) has been observed in Ni_{1- x} S (x=-0.02, -0.01, 0, 0.01, 0.02 and 0.03). The MR in a magnetic field of 4 T was found to be equal to 770% at 290 K for x=-0.02, 920% at 283 K for x=-0.01, 1530% at 268 K for x=0, 1040% at 230 K for x=0.01, 730% at 257 K for x=0.02 and 660% at 87 K for x=0.03. The large MR was found to be due to a magnetic field-induced magnetic and electrical transition from an antiferromagnetic (AFM) anomalous-metal phase to a paramagnetic (PM) metal phase. Received: 23 January 2001 / Accepted: 24 January 2001 / Published online: 27 June 2001     

Intracavity frequency mixing in pulsed optical parametric oscillators for the efficient generation of continuously tunable ultraviolet radiation

Received: 4 May 1998/Revised version: 8 July 1998     

Femtosecond ultraviolet pulses generated using noncollinear optical parametric amplification and sum frequency mixing

We demonstrate the generation of ultraviolet 33-fs pulses with a shot-to-shot energy fluctuation of less than 3% using sum frequency mixing of visible pulses of a noncollinear optical parametric amplifier with sub-40-fs pulses of a 1-kHz Ti:sapphire-amplified system. The pulses are transform-limited (ΔνΔτ=0.36) and tunable in the range from 315 nm to 355 nm with energy above 1 μJ (2.6 μJ at 330 nm). Received: 21 July 2000 / Published online: 8 November 2000     

Second-harmonic spectroscopy of Ge/Si(001) and Si1-xGex(001)/Si(001)

0.9 Ge_0.1(001)/Si(001) films with SH photon energies 3.1<2hν<3.5 eV near the bulk E₁ critical point of Si(001) or Si_0.9Ge_0.1(001). Ge was deposited on Si(001) by using atomic layer epitaxy cycles with GeH₄ or Ge₂H₆ deposition at 410 K followed by hydrogen desorption. As Ge coverage increased from 0 to 2 monolayers the SH signal increased uniformly by a factor of seven with no detectable shift in the silicon E₁ resonant peak position. SH signals from Si_0.9Ge_0.1(001)/Si(001) were also stronger than those from intrinsic Si(001). Hydrogen termination of the Si_0.9Ge_0.1(001) and Ge/Si(001) surfaces strongly quenched the SH signals, which is similar to the reported trend on H/Si(001). We attribute the stronger signals from Ge-containingsurfaces to the stronger SH polarizability of asymmetric Ge-Si and Ge-Ge dimers compared to Si-Si dimers. Hydrogen termination symmetrizes all dimers, thus quenching the SH polarizability of all of the surfaces investigated. Received: 13 October 1998 / Revised version: 18 January 1999     

Four-wave mixing of picosecond pulses in hollow fibers: expanding the possibilities of gas-phase analysis

Third-harmonic, difference-frequency, and sum-frequency generation processes in hollow fibers are experimentally studied with 30-ps pulses having an energy of several millijoules. The experimental dependence of the difference-frequency signal on the pressure of the gas filling the fiber agrees well with the results of calculations when the contribution of higher order waveguide modes is taken into consideration, thus indicating the importance of nonlinear-optical processes involving higher order waveguide modes of a hollow fiber. Hollow fibers are also shown to expand the possibilities of nonlinear-optical analysis of gases by allowing the generation of third-harmonic and sum-frequency signals, which vanish in the regime of tight focusing in a medium with normal dispersion. Received: 26 September 2000 / Revised version: 15 January 2001 / Published online: 30 March 2001     

Dispersion of second-order nonlinear optical coefficient

A simple, approximate relation between the dispersion of the second-order nonlinear optical (SNLO) coefficient and first-order susceptibility has been derived using the well-known results of density-matrix calculation of quantum-mechanical theory. A new tensor of SNLO coefficient has been defined, which retains symmetries when the input beams are in the spectral range of transparency while the generated beam can also be in the spectral range of absorption. The validity of the relation has been checked for three ferroelectric crystals, KTP, LiNbO₃ and KNbO₃, which are transparent in the visible and near infrared, and for two semiconductors, GaP and GaAs, which absorb in the visible. Contrary to Miller’s law, the presented relation is in good agreement with measurements. Received: 8 February 2001 / Revised version: 2 July 2001 / Published online: 10 October 2001     

Carrier-envelope offset phase control: A novel concept for absolute optical frequency measurement and ultrashort pulse generation

The shortest pulses periodically emitted directly from a mode-locked Ti:sapphire laser are approaching the two-optical-cycle range. In this region, the phase of the optical carrier with respect to the pulse envelope becomes important in nonlinear optical processes such as high-harmonic generation. Because there are no locking mechanisms between envelope and carrier inside a laser, their relative phase offset experiences random fluctuations. Here, we propose several novel methods to measure and to stabilize this carrier-envelope offset (CEO) phase with sub-femtosecond uncertainty. The stabilization methods are an important prerequisite for attosecond pulse generation schemes. Short and highly periodic pulses of a two-cycle laser correspond to an extremely wide frequency comb of equally spaced lines, which can be used for absolute frequency measurements. Using the proposed phase-measurement methods, it will be possible to phase-coherently link any unknown optical frequency within the comb spectrum to a primary microwave standard. Experimental studies using a sub-6-fs Ti:sapphire laser suggesting the feasibility of carrier-envelope phase control are presented. Received: 19 August 1999 / Published online: 8 September 1999     

Generation of 100 μJ pulses at 82.8 nm by frequency tripling of sub-picosecond KrF laser radiation

. Investigations of the efficient generation of powerful coherent radiation at 82.8 nm by frequency tripling of short-pulse KrF laser radiation are presented. Argon gas is selected as nonlinear medium due to the resonantly enhanced 3rd-order susceptibility χ⁽³⁾(-3ω,ω,ω,ω). Pulse energies of 100 μJ at 82.8 nm have been measured for a pump pulse energy of 14 mJ. An upscaling to more than 500 μJ is expected with available more powerful pump lasers. Features of this XUV source and possible applications are discussed. Received: 26 July 2002 / Published online: 15 November 2002 RID="*" ID="*"Corresponding author. Fax: +49-511/7622211, E-mail: reinhardt@iqo.uni-hannover.de     

Determining the spin polarization of surfaces by spin-polarized scanning tunneling spectroscopy

During the last few years, spin-polarized scanning tunneling microscopy and spectroscopy has been developed as a reliable tool to image surface magnetic domain structures of bulk materials as well as thin films and nanostructured systems. In principle, this technique also allows for the determination of the energy-resolved spin polarization of the sample P_S(E) with nanometer resolution, information which might play a crucial role in understanding systems like, for example, non-magnetic adatoms on magnetic surfaces. A main problem in quantifying P_S(E), however, arises from the fact that, in contrast to planar junctions, the tip–sample distance generally varies with the magnitude and direction of the surface magnetization, since the distance is controlled indirectly by the tunneling current that is itself spin-polarized. We employ a simple model of the tunneling process to investigate this issue and show that a normalization of the dI/dU spectra with the total conductance I/U is insufficient to correct for their distance dependence. Received: 2 September 2002 / Accepted: 2 September 2002 / Published online: 5 March 2003 RID="*" ID="*"Corresponding author. Fax: +49-40/42838-5311, E-mail: kubetzka@physnet.uni-hamburg.de