We present experimental and theoretical study of refractive index modification induced by femtosecond laser
pulses in photorefractive crystals. The single pulses with central wavelength of 800 nm, pulse duration of 150 fs,
and energy in the range of 6-130 nJ, tightly focused into the bulk of Fe-doped LiNbO3 and stoichiometric LiTaO3
crystals induce refractive index change of up to about 10-3 within the volume of about (2.0 x 2.0 x 8.0) μm3.
The photomodification is independent of the polarization orientation with respect to the crystalline c-axis. The
recorded region can be erased optically by a defocused low-intensity single pulse of the same laser. Recording
and erasure can be repeated at the same position many times without loss of quality. These findings demonstrate
the basic functionality of the ultrafast three-dimensional all-optical rewritable memory. Theoretically they are
interpreted by taking into account electron photogeneration and recombination as well as formation of a space-charge
field. The presented analysis indicates dominant role of photovoltaic effect for our experimental conditions,
and suggests methods for controlling various parameters of the photomodified regions.
Undoped and Mg-doped stoichiometric LiTaO3 with concentrations of 0.5, 0.7, and 1.0 mol % were grown by the double-crucible Czochralski method, and their photorefractive effect was investigated by measuring light-induced birefringence changes. Periodically poled Mg-doped stoichiometric lithium tantalate (PPMgSLT) were fabricated for QPM optical parametric oscillator, whose properties, including slope efficiency and threshold, were measured to investigate influence of photorefractive effect on optical parametric oscillator. The results showed that a concentration of 1 mol % MgO in the melt was enough to suppress photorefractive effect at tens of MW/cm2, and the OPO performance of PPMgSLT doped with 0.5 mol % MgO is only 6 % lower than that of PPMgSLT doped with 1 mol % MgO at room temperature, even though light-induced birefringence existed for the crystal doped with 0.5 mol % MgO.
Interband photorefractive gratings induced by deep ultraviolet light at λUV = 257 nm are investigated in pure and Mg-doped near-stoichiometric LiTaO3. By controlling the stoichiometry, the response time and dynamic range of the interband photorefractive effect can be very much improved. Measured time constants are in the
order of a few tens of milliseconds for UV light intensities of about 100 mW/cm2. Further, we report that Mg doping of near-stoichiometric LiTaO3 increases the grating response rate by a factor of 50 compared with the one in undoped crystals. In Mg-doped near-stoichiometric LiTaO3, quasi-fixing of holographic gratings with UV light and nondestructive readout in the visible has been observed. These quasi-fixed gratings are written in the deep traps of the crystal.
Computational study of nanosecond pulse laser radiation in periodically poled LiNbO3 and LiTaO3 crystals reveals the complex spacio-temporal evolution of the 1.064 μm fundamental harmonic (FH) and second harmonic (SH) energy fields with associated temperature fields, leading to the thermal dephasing and inhibition of second harmonic generation (SHG). The investigated range of the laser input power is W0=0.5-50 W (with the pulse energy Q0=0.01-1 mJ/pulse and repetition rate of 50 kHz). For input laser powers W0>10 W the FH and SH energy fields are found to strongly couple with non-uniform temperature field leading to significant thermal dephasing and SHG efficiency loss. Heat generation and temperature distributions also exhibit very significant non-uniformities along and across the laser beam, maximizing at the rear or inside the crystal, depending on the input power. Performed study shows the feasibility of the effective thermal control with temperature gradient along the crystal allowing one to maintain (i) the irradiated zone within the temperature tolerance range and (ii) high SHG efficiency under high input laser powers.
The growth characteristics and properties of large size SrAlF5 single crystals are described and compared with those of BaMgF4. Transmission spectra in the vacuum ultraviolet wavelength region indicate a high transparency of SrAlF5 (about 90% without considering surface reflection loses) down to 150 nm, on contrast to the optical loses observed for BaMgF4. The ferroelectric character of SrAlF5 is evidenced by the reversal of the spontaneous polarization in a hysteresis loop. The higher potential of SrAlF5 in comparison with BaMgF4 for the realization of all-solid-state lasers in the ultraviolet wavelength region by the quasi-phase matching (QPM) technique is pointed out. SrAlF5, besides a higher grade of transparency, shows a nonlinear effective coefficient similar to that of quartz and uniaxial nature, on contrast to the one order smaller nonlinear coefficient and biaxial character of BaMgF4. The refractive index of SrAlF5 from the ultraviolet to the near-infrared wavelength region is measured by the minimum deviation method. The Sellmeier and Cauchy coefficients are obtained from the fits to the curves of the ordinary and extraordinary refractive indices, and the grating period for the first order QPM is estimated as a function of the wavelength. The poling periodicity for 193 nm SHG from 386 nm is 4 micron-m.
We have investigated the dark decay mechanism by measuring dark decay time constants of two-color holograms recorded in undoped and slightly doped near-stoichiometric LiNbO3 and LiTaO3 crystals in the temperature range from 50 to 200 °C. All the samples in this work obey an Arrhenius-type dependence of time constant on absolute temperature, and yield nearly same activation energies of 1.08 eV. The results show that proton compensation mechanism dominated the dark decay process. Lifetimes of holograms at room temperature in LiTaO3 are one order of magnitude longer than that in LiNbO3 if having the same proton concentration.
Near-stoichiometric LiNbO3 crystals slightly doped with Mn from different Li concentrations in the melt were grown by the top seeded solution growth method. The light-induced (small polarons) absorption under UV illumination was probed using near-IR of 780 nm. The dark decay process shows a stretched-exponential behavior. The dependences of the light-induced absorption, the decay time constant, and the stretching factor on the pumping intensity were presented. The photovoltaic current intensity and the photoconductivity under UV illumination were measured by applying a DC field along the z-axis of the sample. The photoconductivity intensity showed superlinear dependence of intensity. The experimental results can be explained quantitatively by developing the two-center charge transport model with direct excitation and recombination between Mn and small polarons.
This paper reports the development and modelling of the reverse-proton-exchange process for the realization of high quality optical waveguides in MgO doped stoichiometric lithium tantalate, a promising nonlinear material due to its low coercive field and high damage threshold. Reverse-proton-exchange gives rise to a buried refractive index-profile providing significant advantages in terms of attenuation, insertion losses and overlap of the fields interacting through the nonlinear susceptibility. By characterizing several samples fabricated under different experimental conditions, we identified a fabrication procedure which is simpler than the conventional one used for lithium niobate: the annealing and reverse-exchange processes are indeed performed at the same temperature so that the diffusion of hydrogen ions towards the substrate during the reverse-exchange occurs in the same conditions as during the annealing. This results in very simple empirical laws relating the fabrication to the optical parameters. By such a modeling we defined fabrication parameters giving rise to a single-mode waveguide at l=1.55mm with good fiber mode-matching and high efficiency when used as a nonlinear device for telecom applications.
Two-color holography is an effective solution to the volatile readout problem in volume holographic data storage based on photorefractive materials. Popular materials for two-color holography are reduced doped and nondoped near-stoichiometric lithium niobate crystals. However, the lifetime at room temperature is from several weeks to several months depending on the reduction state of the material. Moreover, reductive treatment will degrade the nonvolatility of two-color holograms. The important issue for two-color holography is how to increase the lifetime. In this contribution, lifetimes of two-color nonvolatile holograms recorded in as-grown near-stoichiometric lithium niobate and tantalate crystals were compared by extrapolating the high-temperature data. The dark-decay time constants obey an Arrhenius dependence on absolute temperature and yield activity energy of 1.06 eV around in all measured crystals. Lifetimes of holograms in nondoped and slightly doped crystals depend on the proton concentration. Lifetimes of hologram in lithium tantalate are one order of magnitude longer than those in lithium niobate at the same proton concentration. The lifetime of two-color holograms in lithium tantalite is longer than 20 years.
Microscale to nanoscale ferroelectric domain engineering of a near-stoichiometric LiNbO3 crystal was investigated by using a scanning force microscope. The single crystal LiNbO3 was grown by the double-crucible Czochralski method with automatic powder supply system. The electric field required to inverse the polarization direction of the domain was about one-ninth of the filed for a conventional congruent LiNbO3. The near-stoichiometric LiNbO3 crystal fixed on metal substrate was polished to a thickness of approximately 5 μm. Polarization directions of the domains were locally inverted by applying voltages with a conductive cantilever of the scanning force microscope. Furthermore, the domain structure was patterned in the LiNbO3 samples, where the domains were inverted by scanning with the cantilever on the sample while applying voltages.
Holograms are recorded in near-stoichiometric LiNbO3 doped with 8 ppm of Mn by use of two-color holographic recording method, where an IR laser of 778 nm is used for writing and an UV laser of 350 nm is used for gating. Dependences of two-color sensitivity and M/# on gating and writing intensities are presented. Significant improvements of sensitivity, M/# and dark decay are obtained compared with reduced near-stoichiometric LiNbO3. To our knowledge, the measured two-color sensitivity of 0.21 cm/J with a gating intensity of 1.5 W/cm2 is the highest among the values reported so far, which is attributed to large light-induced absorption of small polarons. 50 plane-wave holograms are recorded by the conventional angle-multiplexing method.
Two-color recording is achieved in a Tb-doped near-stoichiometric LiNbO3 crystal of 3-mm thickness by use of extraordinary 778 nm information-carrying beams and ordinary 350 nm gating light. The dependences of key parameters, the two-color recording sensitivity and the dynamic range expressed by the saturated diffraction efficiency, on intensities of recording and gating beams are presented. The saturated diffraction efficiency increases with total writing intensity, and then reaches a saturated value of 56% at an intensity of 20W/cm2. The sensitivity increases linearly with gating intensity at low intensity, and then saturates with a value of 0.08 cm/J at a higher intensity than 1.6 W/cm2. The saturated sensitivity is much higher than the reported value in literature. This material shows very significant improvement on two-color holography performance. 50 plane-wave holograms are recorded by the angle-multiplexing method and an M/# of 1.13 is obtained.
We observed that newly developed near-stoichiometric LiNbO3 crystals doubly doped with Tb and Fe have three different types of energy levels: UV absorption centers just above the valence band, metastable shallow electron traps slightly below the conduction band, the deep traps located about 1.9 eV below the conduction band. Irradiation with UV light induced a stable absorption band extending from (lambda) equals 650 nm to the absorption edge, which is caused by the photoinduced charge transfer from UV-sensitive absorption centers to deep traps via the conduction band. The electron lifetimes at shallow and deep traps could be controlled by doping concentrations. Based on these favorable energy states, nonvolatile two-color holographic recording has been demonstrated by use of 852-nm recording beams and UV gating light. Quasi-nonvolatile one-color recording at 532 nm has also been demonstrated in these codoped crystals. Hologram recording from the UV-exposed, colored state revealed a much improved sensitivity in comparison to that from the uncolored state.
Doped stoichiometric LiNbO3 (SLN) crystals show more advantages over traditional congruent LiNbO3 (CLN). This paper is focused on the measurement of the holographic performances of doped SLN crystals, including the sensitivity, dynamic range, and angular selectivity. The principles and methods for the measurements are first described, with more attention paid to the measurement of erasure time constants. The results show that the SLN crystal co-doped with Ce and Mn has the largest dynamic range, owing to the extremely long erasure time constants even by the multiplexing method. The SLN crystal co-doped with Tb and Fe and reduced in rich nitrogen atmosphere has the fastest response time and highest sensitivity. The oxidized and as-grown SLN crystals co-doped with Tb and Fe exhibit photochromic effect under UV illumination. With UV pre-illumination these crystals have sensitivity competitive to the heavily Fe doped CLN. The measured selective angles for most of the SLN samples of proper optical quality agree well with the theoretical calculation.
We show that stoichiometric LiNbO3 crystal containing nonstoichiometric defects much less than congruent LiNbO3 exhibit some advantageous properties for the holographic data storage (HDS) applications. This was confirmed by the two-beam coupling experiment and digital hologram test. In order to interpret the high performance of stoichiometric LN, we compared some related parameters such as linear electro-optic constants, photoconductivity and photovoltaic constants between stoichiometric and congruent LN crystals. In all measurements, the stoichiometric crystals grown by the novel double crucible CZ method were found to be more excellent as HDS medium. This superiority was obvious at the geometry using the extraordinary polarization.
Some multi-component photorefractive crystals exhibit wide variations in their properties associated with the nonstoichiometry of the constituent cations. In order to grow single crystals with high quality and high homogeneity under nonstoichiometry control, a double crucible Czochralski method has been developed. In this method, the melt was divided into two parts by a double structure (two chamber system) crucible. The crystal was grown from the inner melt, and a powder with the same composition as the growing crystal was supplied to the outer melt. The powder was supplied continuously and smoothly at the rate of weight increase of the growing crystal. This rate was automatically controlled to match the weight increase of the growing crystals as monitored by a load cell. As an example, LiNbO3 single crystals with a composition close to stoichiometric were grown, and their photorefractive properties were compared with those of Nb-rich congruent LiNbO3 crystal. As the result, it turned out that the stoichiometric LN crystal exhibited higher efficiency and faster responsivity than the congruent crystal.
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