ABSTRACT
We report on a mode-mismatched thermal lens experiment performed to quantitatively evaluate thermal and electronic laser-induced lensing effects in ion-doped crystals Cr3+:LiSAF, Yb3+:KYW, and Yb3+:YAG. The large diameter of the probe beam resulted in a slow thermal effect (â¼dozens of milliseconds) two orders of magnitude larger than the electronic one, improving the discrimination of both competitive effects. All thermal and electronic parameters are obtained from transient signals modeled by an analytical equation, valid for small phase shifts in the absence of upconversion effects.
ABSTRACT
Erbium-doped yttrium aluminum garnet (Er3+:YAG) rods were inserted inside undoped tubes and grown into single-crystal fibers of a diameter of 300 µm using the laser-heated pedestal growth technique. Growth at various rates resulted in radially graded distributions of Er3+ dopant ions, as observed using laser-induced fluorescence imaging. Profiles of the refractive index were measured using cross-sectional reflectometry in a microscope. Dopant distributions and the corresponding index profiles were compared with thermal diffusion theory to determine the inter-diffusion coefficient of Y3+ and Er3+ ions at 2000°C, yielding an estimated value of D=(9.10±0.8)×10-11 m2/s. This work constitutes a step toward controlled growth of fibers with high thermal conductivities, low Brillouin gain, and waveguiding properties required for high-power optical amplifier and laser applications.
ABSTRACT
A new method of steering THz pulses radiated from a thin emitter excited by tilted optical pulse-fronts has been developed theoretically and validated in a proof-of-concept experiment. This steering technique is potentially efficient and rapid, and it should benefit from a THz-pulse energy that can scale with optical-beam size and magnitude. Conversely, the method employed for measuring the steered THz pulses is also capable of characterizing the pulse-front tilt of an optical beam.
ABSTRACT
The state mixings necessary to mediate three new optical nonlinearities are shown to arise simultaneously and automatically in a 2-level atom with an â = 0 ground state and an â = 1 excited state that undergoes a sequence of electric and magnetic dipole-allowed transitions. The treatment is based on an extension of dressed state theory that includes quantized electric and magnetic field interactions. Magneto-electric rectification, transverse magnetization, and second-harmonic generation are shown to constitute a family of nonlinear effects that can take place regardless of whether inversion is a symmetry of the initial unperturbed system or not. Interactions driven jointly by the optical electric and magnetic fields produce dynamic symmetry-breaking that accounts for the frequency, the intensity dependence, and the polarization of induced magnetization in prior experiments. This strong field quantum model explains not only how a driven 2-level system may develop nonlinear dipole moments that are forbidden between or within its stationary states, but it also broadens the class of materials suitable for optical energy conversion applications and magnetic field generation with light so as to include all transparent dielectrics.
ABSTRACT
A set of stilbene-substituted octasilicates [p-RStil(x)Ph(8-x)SiO(1.5)](8) (R = H, Me, MeO, Cl, NMe(2) and x = 5.3-8) and [o-MeStilSiO(1.5)](8) were prepared. Model compounds were also prepared including the corner and half cages: [p-MeStilSi(OEt)(3)], [p-Me(2)NStilSi(OSiMe(3))(3)], and [p-Me(2)NStilSi(O)(OSiMe)](4). These compounds were characterized by MALDI-TOF, TGA, FTIR, and (1)H NMR techniques. Their photophysical properties were characterized by UV-vis, two-photon absorption, and cathodoluminescence spectroscopy (on solid powders), including studies on the effects of solvent polarity and changes in concentration. These molecules are typically soluble, easily purified, and robust, showing T(d(5%)) > 400 degrees C in air. The full and partial cages all show UV-vis absorption spectra (in THF) identical to the spectrum of trans-stilbene, except for [o-MeStilSiO(1.5)](8), which exhibits an absorption spectrum blue-shifted from trans-stilbene. However, the partial cages show emissions that are red-shifted by approximately 20 nm, as found for stilbene-siloxane macrocycles, suggesting some interaction of the silicon center(s) with the stilbene pi* orbital in both the corner and half cages. In contrast, the emission spectra of the full cages show red-shifts of 60-100 nm. These large red-shifts are supported by density functional theoretical calculations and proposed to result from interactions of the stilbene pi* orbitals with a LUMO centered within the cage that has 4A(1) symmetry and involves contributions from all Si and oxygen atoms and the organic substituents. Given that this LUMO has 3-D symmetry, it appears that all of the stilbene units interact in the excited state, consistent with theoretical results, which show an increased red-shift with an increase in the functionalization of a single corner to functionalization of all eight corners with stilbene. In the case of the Me(2)N- derivatives, this interaction is primarily a charge-transfer interaction, as witnessed by the influence of solvent polarity on the emission behavior. More importantly, the two-photon absorption behavior is 2-3 times greater on a per p-Me(2)Nstilbene basis for the full cage than for the corner or half cages. Similar observations were made for p-NH(2)stilbenevinyl(8)OS cages, where the greater conjugation lengths led to even greater red-shifts (120 nm) and two-photon absorption cross sections. Cathodoluminescence studies done on [p-MeStilSiO(1.5)](8) or [p-MeStilOS](8) powders exhibit essentially the same emissions as seen in solution at high dilution. Given that only the emissions are greatly red-shifted in these molecules, whereas the ground-state UV-vis absorptions are not changed from trans-stilbene, except for the ortho derivative, which is blue-shifted 10 nm. It appears that the interactions are only in the excited state. Theoretical results show that the HOMO and LUMO states are always the pi and pi* states on the stilbene, which show very weak shifts with increasing degrees of functionalization, consistent with the small changes in the UV-vis spectra. The band gap between the lowest unoccupied 4a1 symmetry core state localized inside the silsesquioxane cage and the highest occupied state (pi state on stilbene), however, is markedly decreased as the number of stilbene functional groups is increased. This is consistent with the significant red-shifts in the emission spectra. The results suggest that the emission occurs from the 4a1 state localized on the cage. Moreover, for the compounds [p-RStil(6-7)Ph(2-1)OS](8), the emissions are blue-shifted compared to those of the fully substituted compounds, suggesting the molecular symmetry is reduced (from cubic), thereby reducing the potential for 3-D delocalization and raising the energy of the LUMO. The implications are that these octafunctional molecules exhibit some form of 3-D interaction in the excited state that might permit their use as molecular transistors as well as for energy collection and dispersion as molecular antennas, for example, and for nonlinear optical applications.
ABSTRACT
Bistability is reported in sensitized Er3+ luminescence driven by an Yb3+ transition that previously revealed an Yb3+ luminescent instability. To our knowledge this is the first report of bistable energy transfer between different rare-earth ions.
ABSTRACT
We report electrically pumped, cw laser action near 405 nm from Nd(3+) -doped delta -alumina nanopowders. To our knowledge, this is the first report of stimulated emission from the high-lying F(2) -excited states, achieved through feedback from strong elastic scattering of light over transport path lengths shorter than half a wavelength.
ABSTRACT
A simple upconversion scheme utilizing 40-fs pulses is shown to permit high-contrast imaging of objects obscured by a highly scattering medium when no ballistic component is evident in the scattered light and imaging is performed with any portion of the scattered light pulse. We present a time-gated, inherently low-pass spatially filtered imaging method that minimizes signal-averaging requirements and greatly facilitates imaging under severe scattering (turbid) conditions.
ABSTRACT
Two-beam coupling measurements of an avalanche upconversion transition in concentrated Tm:LiYF (4) confirm that, despite the resonant nature of the excited-state optical interaction, the induced response is strongly dispersive. This surprising characteristic is shown to be a general feature of avalanche polarization, with an off-resonant process dominating the resonant response.
ABSTRACT
We describe continuous-wave mode locking and Q switching of an Er:LiYF(4) trio upconversion laser operating in the green spectral region.
ABSTRACT
We report trio upconversion laser action in Er:LiYF(4) with excitation at 1.55 microm resulting in cw emission at 0.55 microm to a temperature of 95 K and contrast its performance with earlier green erbium upconversion lasers.
ABSTRACT
Image retrieval based on degenerate four-wave mixing with a new nonlinear mechanism is demonstrated. An avalanche nonlinearity associated with induced excited-state absorption is exploited to furnish phase conjugation with threshold behavior and potential motion sensitivity. Population pulsations are reported at high intensities.
ABSTRACT
We report room-temperature operation of what we believe is the first continuous-wave laser that relies exclusively on cooperative upconversion by coupled ion pairs to achieve population inversion.
ABSTRACT
Laser action at 530 nm using H3 centers in diamond was observed with an efficiency of 13.5% at room temperature. Optical double-resonance experiments on N3 centers provided direct evidence for a (2)A metastable level. Its presence results in rapid decay of the excited (2)E state and low quantum efficiency as well as significant excited-state absorption in the N3 luminescence region.
