Spectra of the selective heat radiation of Yb2O3 under the laser thermal excitation

The dependence of the spectra of the near-IR and visible selective heat radiation (SHR) of the Yb₂O₃ polycrystals that are synthesized using the laser thermal method on the excitation intensity of the CW electric discharge CO₂ laser at the wavelength λ = 10.6 μm is experimentally studied. The SHR spectra are determined by the multiphonon excitation of the vibronic states of the ² F _5/2 term in the Yb³⁺ ions and the radiative transitions to the vibronic states of the ground term ² F _7/2.The laser heating of the polycrystals to the melting point causes the anomalous growth of the SHR spectral peaks in the wavelength range λ ≥ 1040 nm due to an increase in the intensity related to an increase in the probabilities of the radiative vibronic transitions owing to the thermal increase in the phonon density. The effective conversion of the thermal energy of the Yb₂O₃ polycrystals into the SHR indicate the significant role of the radiative cooling of surface.     

Nonlinear absorption properties of Co2+:MgAl2O4 crystal

The differential absorption spectra of Co²⁺: MgAl₂O₄ (MALO) crystal were studied with a picosecond pump-probe technique under excitation of the ⁴A₂→⁴T₁(⁴P) and ⁴A₂→⁴T₁(⁴F) transitions of the tetrahedral Co²⁺ ion. The difference spectra of stimulated emission (SE) and excited state absorption (ESA) were derived from the measured differential absorption spectra. The ⁴T₁(⁴P)→⁴A₂ SE band around 660 nm was observed. The ESA bands were assigned to the ⁴T₂→⁴T₁(⁴P) transition and to transitions from the thermally populated ²E(²G) excited state to doublet levels arising from the ²F free-ion level of the tetrahedrally coordinated Co²⁺ ion. Absorption saturation measurements were performed at 1.34 μm and 1.54 μm. Passive Q-switching of 1.34-μm Nd³⁺:YAlO₃ and 1.54-μm Er³⁺:glass lasers was realized using the Co²⁺:MALO crystal as saturable absorber. The Q-switched laser pulses of 38 ns (110 ns) in duration and up to 2.7 mJ (10 mJ) in energy at 1.54 μm (1.34 μm) were obtained. Received: 3 March 1999 / Revised version: 30 June 1999 / Published online: 30 November 1999     

Visible up-conversion and NIR luminescence studies of LiAl<Subscript>5</Subscript>O<Subscript>8</Subscript>:Er phosphor co-doped with Yb<Superscript>3+</Superscript> and Zn<Superscript>2+</Superscript>

The frequency up-conversion, an efficient laser emission and amplification in Er³⁺:LiAl₅O₈ phosphors co-doped with Yb³⁺ and Zn²⁺ phosphor powders in the 520–560, 640–680 nm regions and at ∼1.5 μm, respectively, have been reported. The emission corresponds to the ²H_11/2, ⁴S_3/2→⁴I_15/2, ⁴F_9/2→⁴I_15/2 and ⁴I_13/2→⁴I_15/2 transitions upon direct excitation into the intermediated ⁴I_11/2 level using ∼980 nm radiation from a CW laser. Possible mechanisms involved for the up-conversion processes based on the energy level matching scheme, the pump-power dependence and the dynamical behaviour have been discussed. The effect of the addition of Yb³⁺ and Zn²⁺ for the amplification in the 1.5 μm eye-safe telecommunication window has been elaborated and characterized in detail.     

Excitation energy transfer between Er3+ and Tm3+ in LiNbO3

Conclusions Nonradiative energy transfer between similar and different rare-earth ions in LiNbO₃ has been evidenced for the first time. The contribution of nonradiative energy transfer to the decay of the¹G₄ and³H₄ levels of thulium and the⁴S_3/2 and⁴I_13/2 levels of erbium is significant for activator concentrations of the order of several thousand ppm in LiNbO₃. The excitation of higher-lying levels of both activators is transferred faster in codoped crystal to the lowest luminescent levels, from which the luminescence in the 1–2-μm spectral region occurs. This accelerated relaxation is advantageous for broadband optical pumping since the contribution of radiative transitions competing with the³F₄−³H₆ laser transition of thulium is reduced. On the other hand, it appears that erbium ions will influence adversely the efficiency of a laser-diode-pumped LiNbO₃∶Er, Tm laser operating near 1.8 μm since the part of the³H₄ excitation transferred to erbium ions is emitted from the long-lived⁴I_11/2 level of Er³⁺. Furthermore, the⁴I_13/2 excitation is not transferred fully to thulium ions and is lost in⁴I_13/2−⁴I_15/2 emission. Lithium niobate singly doped with thulium is more promising since the cross-relaxation process that transfers the excitation from the³H₄ level to the³F₄ level appears to be efficient in this host. Published in Zhurnal Prikladnoi Spektroskopii, Vol. 62, No. 5, pp. 125–133, September–October, 1995.     

Spectroscopic characterisation of LaGaO3:Er3+ crystals

LaGaO₃ crystals doped with Er³⁺ ions were grown by the Czochralski method and their optical properties were examined. The Er³⁺ energy levels have been determined from the low-temperature absorption and emission spectra. The results of Judd–Ofelt analysis are presented and compared with experimental data. The emission cross sections are determined for the ⁴ I _13/2→⁴ I _15/2 (1.55 μm) and ⁴ I _11/2→⁴ I _13/2 (2.85 μm) transitions of erbium. Received: 6 December 1999 / Revised version: 10 February 2000 / Published online: 27 April 2000     

The Muonic Hydrogen Lamb Shift Experiment at PSI

A measurement of the 2S Lamb shift in muonic hydrogen (μ⁻p) is being prepared at the Paul Scherrer Institute (PSI). The goal of the experiment is to measure the energy difference ΔE(2⁵ P _3/2−2³ S _1/2) by laser spectroscopy (λ≈6μm) to a precision of 30 ppm and to deduce the root mean square (rms) proton charge radius with 10⁻³ relative accuracy, 20 times more precise than presently known. An important prerequisite to this experiment is the availability of long-lived μp_2S -atoms. A 2S-lifetime of ∼1 μs – sufficiently long to perform the laser experiment – at H₂ gas pressures of 1–2 hPa was deduced from recent measurements of the collisional 2S-quenching rate. A new low-energy negative muon beam yields an order of magnitude more muon stops in a small low-density gas volume than a conventional cloud muon beam. A stack of ultra-thin carbon foils is the key element of a fast detector for keV-muons. The development of a 2 keV X-ray detector and a 3-stage laser system providing 0.5 mJ laser pulses at 6 μm is on the way. This revised version was published online in August 2006 with corrections to the Cover Date.     

Site-selective spectroscopy of Er3+:Ti:LiNbO3 waveguides

Starting from previous investigations in LiNbO₃ bulk crystals, we studied the optical properties of Er³⁺ ions in Ti:LiNbO₃ channel waveguides and investigated the waveguide-specific lattice environment of the Er³⁺ ions (“sites”) caused by the doping method used and the presence of a large number of Ti⁴⁺ ions. For that purpose the method of combined excitation–emission spectroscopy was applied for the first time to waveguides at low temperatures. Comparing the spectroscopic results obtained for the green, red, and near-IR luminescence (λ≈550, ≈650 and ≈980 nm) under direct (450 nm), 2-step (980 nm), and 3-step (1.5 μm) laser excitation, we found several distinguishable Er³⁺ sites which in terms of energy levels and relative numbers are similar to those in bulk material, but exhibit significantly different up-conversion efficiencies and strongly inhomogeneously broadened transitions. Moreover, we were able to distinguish isolated and cluster Er³⁺ sites by their characteristic excitation and emission transition energies and studied the respective excitation/relaxation channels. The cluster sites are most efficient in the up-conversion process, especially under 3-step excitation. Using accepted microscopic models for Er³⁺ and Ti⁴⁺ incorporation into the LiNbO₃ crystal lattice, the site distribution and up-conversion mechanisms are elucidated and their consequences for laser applications in different spectral regions are discussed. Received: 16 November 2000 / Published online: 21 March 2001     

The excitation mechanism of rare-earth ions in silicon nanocrystals

A detailed investigation on the excitation mechanisms of rare-earth (RE) ions introduced in Si nanocrystals (nc) is reported. Silicon nanocrystals were produced by high-dose 80-keV Si implantation in thermally grown SiO₂ followed by 1100 °C annealing for 1 h. Subsequently some of the samples were implanted by 300-keV Er, Yb, Nd, or Tm at doses in the range 2×10¹²–3×10¹⁵ /cm². The energy was chosen in such a way to locate the RE ions at the same depth where nanocrystals are. Finally an annealing at 900 °C for 5 min was performed in order to eliminate the implantation damage. These samples show intense room-temperature luminescence due to internal 4f shell transitions within the RE ions. For instance, luminescence at 1.54 μm and 0.98 μm is observed in Er-doped nc, at 0.98 μm in Yb-doped nc, at 0.92 μm in nc and two lines at 0.78 μm and 1.65 μm in Tm-doped nc. Furthermore, these signals are much more intense than those observed when RE ions are introduced in pure SiO₂ in the absence of nanocrystals, demonstrating the important role of nanocrystals in efficiently exciting the REs. It is shown that the intense nc-related luminescence at around 0.85 μm decreases with increasing RE concentration and the energy is preferentially transferred from excitons in the nc to the RE ions which, subsequently, emit radiatively. The exact mechanism of energy transfer has been studied in detail by excitation spectroscopy measurements and time-resolved photoluminescence. On the basis of the obtained results a plausible phenomenological model for the energy transfer mechanism emerges. The pumping laser generates excitons within the Si nanocrystals. Excitons confined in the nc can either give their energy to an intrinsic luminescent center emitting at around 0.85 μm nor pass this energy to the RE 4f shell, thus exciting the ion. The shape of the luminescence spectra suggests that excited rare-earth ions are not incorporated within the nanocrystals and the energy is transferred at a distance while they are embedded within SiO₂. Rare-earth excitation can quantitatively be described by an effective cross section σ_eff taking into account all the intermediate steps leading to excitation. We have directly measured σ_eff for Er in Si nc obtaining a value of ≈2×10⁻¹⁷ cm². This value is much higher than the cross section for excitation through direct photon absorption (8×10⁻²¹ cm²) demonstrating that this process is extremely efficient. Furthermore, the non-radiative decay processes typically limiting rare-earth luminescence in Si (namely back-transfer and Auger) are demonstrated to be absent in Si nc further improving the overall efficiency of the process. These data are reported and their implications. Received: 9 April 1999 / Accepted: 10 April 1999 / Published online: 2 June 1999     

Investigation of the turbulent mixing of thin layers of materials of different density during the laser acceleration of flat multilayer targets in the Iskra-4 facility

The results of the first experiments devised to investigate the mixing of thin layers of Al and Au during the laser acceleration of flat three-layer targets of Si (5 μm), Al (2 μm), and Au (0.05–0.26 μm) by radiation converted to the second harmonic from the Iskra-4 iodine laser with an intensity of 4×10¹³−7×10¹³ W/cm² (τ _0.5∼1 ns), which acts on the Si side of the target. A method for detecting the occurrence of mixing is developed. It is established that under the experimental conditions the thickness of the mixing region is at least ∼0.15 μm. The results of a theoretical analysis of the evolution of the disturbances leading to mixing are presented. Zh. éksp. Teor. Fiz. 111, 882–888 (March 1997) Deceased.     

Self-pulsing dynamics of ytterbium-doped fiber laser with pump-bypassed cavity

In addition to efficient continuous wave laser action at 1.06 μm (⁴ F _3/2→⁴ I _11/2 transition), with a slope efficiency 30% and 30 mW pump power threshold, this work presents a throughout study of the spectroscopic, and thermo-optical properties of a 2.0 mol % Nd³⁺ doped fluoroindogallate glass. The characterization of the sample using the pump probe experimental technique indicated the presence of two broad excited state absorption bands from 0.94 to 1.05 μm (⁴ F _3/2→² D _3/2, ² G _9/2, ⁴ G _11/2, ² K _15/2) and from 1.16 to 1.42 μm (⁴ F _3/2→⁴ G _9/2, ⁴ G _7/2, ² K _13/2), found not to interfere with the stimulated emission at 1.06 μm, with a peak cross section value σ_SE = 2.55×10^-21 cm² and a full width at half maximum of 22 nm. Thermal lens measurements were performed to quantify the Auger upconversion parameter (γ=(1.26±0.09)×10^-16 cm³/s) and evaluate the thermal loading in the sample in comparison to other commercial glasses. PACS 181.05.Kf; 78.45.+h; 42.70.Hj     

Er3+-doped sol–gel SnO2 for optical laser and amplifier applications

Erbium-doped tin dioxide (SnO₂:Er³⁺) was obtained by the sol–gel method. Spectroscopic properties of the SnO₂:Er³⁺ are analyzed from the Judd–Ofelt (JO) theory. The JO model has been applied to absorption intensities of Er³⁺ (4f¹¹) transitions to establish the so-called Judd–Ofelt intensity parameters: Ω₂, Ω₄, and Ω₆. With the weak spectroscopic quality factors Ω₄/Ω₆, we expect a relatively prominent infrared laser emission. The intensity parameters are used to determine the spontaneous emission probabilities of some relevant transitions, the branching ratios, and the radiative lifetimes of several excited states of Er³⁺. The emission cross section (1.31×10^-20 cm²) is evaluated at 1.54 μm and was found to be relatively high compared to that of erbium in other systems. Efficient green and red up-conversion luminescence were observed, at room temperature, using a 798-nm excitation wavelength. The green up-conversion emission is mainly due to the excited state absorption from ⁴ I _11/2, which populates the ⁴ F _3/2,5/2 states. The red up-conversion emission is due to the energy transfer process described by Er³⁺ (⁴I_13/2)+Er³⁺(⁴I_11/2)→Er³⁺(⁴F_9/2)+Er³⁺ (⁴ I _15/2) and the cross-relaxation process. The efficient visible up-conversion and infrared luminescence indicate that Er³⁺-doped sol–gel SnO₂ is a promising laser and amplifier material. PACS 71.20.Eh; 74.25.Gz; 78.55.-m     

Rearrangement of optical centers and stimulated radiation of Eu<Superscript>3+</Superscript> in polycrystalline huntite under optical and electron-beam excitation

Polycrystalline europium huntite EuAl₃(BO₃)₄ has been prepared by solid-phase synthesis. The spectral and kinetic characteristics of its luminescence under the excitation by a xenon lamp, single laser pulse, and electron beam have been studied. It has been established that the laser excitation of the polycrystalline samples in the ⁷ F ₀ →⁵ L ₆ transition of Eu³⁺ ions with the power density P ≥ 5 × 10⁷ W/cm² leads to the structure rearrangement of the optical centers, which is accompanied by an increase in the probability of the radiation transitions of the activator. The stimulated radiation of the main type of Eu³⁺ centers in the ⁵ D ₀→⁷ F ₁, ⁷ F ₂, and ⁷ F ₄ transitions has been obtained under the excitation by the electron beam with an energy of 200 keV and a duration of 2 ns.     

Luminescence detection of multiphoton ionization-fragmentation of the molecular CrO 4 2− anions adsorbed on the surface of dispersed SiO2

It is shown that luminescence detection of multiphoton ionization-fragmentation of the molecular CrO ₄ ²⁻ anions adsorbed on the surface of dispersed SiO₂ is possible under excitation with the fundamental frequency of a Nd:YAG pulsed laser (λ=1.064 μm). The structure and the process of formation of the adsorbed complexes under thermal activation of the surface and the nature of luminescence transitions in CrO ₄ ²⁻ anions are studied in detail. It is shown that luminescence is excited as a result of the recombination of photoelectrons and ionized chromate ions. Multiphoton ionization of the ions occurs under three-photon resonance conditions. The resonance level is an antibonding state of the adsorption complex formed with the participation of an oxygen vacancy on the SiO₂ surface. The dynamics of the multiphoton luminescence excitation process includes autoionization (stimulated by intercomplex electronic excitation) in superexcited states, fragmentation of chromate anions, and annealing of surface oxygen vacancies. The rate equations for three-photon-resonance multiphoton ionization are studied. The cross sections for two-and one-photon transitions on the nonresonance steps of multiphoton absorption are obtained. It is concluded that the nonlinear polarizability of the donor-acceptor adsorption bond in “chromate anion-oxygen vacancy” complexes is very important. Zh. éksp. Teor. Fiz. 111, 1748–1774 (May 1997)     

Spectroscopy and energy balance of the Nd<Subscript>2</Subscript>O<Subscript>3</Subscript> selective emission upon the laser thermal excitation

The laser thermal melting of powders is used to fabricate selective emitters (SEs) that represent Nd₂O₃ and Y₂O₃-Nd₂O₃ polycrystals on quartz holders. The SEs are stable under atmospheric conditions upon multiple heating by laser radiation up to the melting point. The spectral shape and integral intensity of the selective heat radiation (SHR) of the Nd₂O₃ microcrystalline powder and the Nd₂O₃ and Y₂O₃-Nd₂O₃ polycrystals are experimentally studied in the near-IR and visible spectral ranges versus the intensity of the laser thermal excitation at a wavelength of 10.6 μm in comparison with the absorption and luminescence spectra of the YAG:Nd³⁺ and YAlO₃:Nd³⁺ single crystals. The SHR spectra are determined by the vibronic transitions between the electronic states ² G _7/2-⁴F_3/2 ⁴I_11/2 and ⁴I_9/2 of the Nd³⁺ ions that are thermally excited due to the multiphonon transitions from the ground state. The energy balance of the SE laser thermal heating is experimentally investigated. The coefficient of the laser energy conversion to the Nd³⁺ SHR is measured, and the emissivity of the SEs that can be used for the study of the thermophotovoltaic generators and the optical excitation of the laser-active media in the near-IR spectral range is estimated.     

Thermal analysis of InP-based quantum cascade lasers for efficient heat dissipation

We have theoretically investigated the thermal characteristics of double-channel ridge–waveguide InGaAs/InAlAs/InP quantum cascade lasers (QCLs) using a two-dimensional heat dissipation model. The temperature distribution, heat flow, and thermal conductance (G _th) of QCLs were obtained through the thermal simulation. A thick electroplated Au around the laser ridges helps to improve the heat dissipation from devices, being good enough to substitute the buried heterostructure (BH) by InP regrowth for epilayer-up bonded lasers. The effects of the device geometry (i.e., ridge width and cavity length) on the G _th of QCLs were investigated. With 5 μm thick electroplated Au, the G _th is increased with the decrease of ridge width, indicating an improvement from G _th=177 W/K⋅cm² at W=40 μm to G _th=301 W/K⋅cm² at W=9 μm for 2 mm long lasers. For the 9 μm×2 mm epilayer-down bonded laser with 5 μm thick electroplated Au, the use of InP contact layer leads to a further improvement of 13% in G _th, and it was totally raised by 45% corresponding to 436 W/K⋅cm² compared to the epilayer-up bonded laser with InGaAs contact layer. It is found that the epilayer-down bonded 9 μm wide BH laser with InP contact layer leads to the highest G _th=449 W/K⋅cm². The theoretical results were also compared with available obtained experimentally data.     

Investigation of 13CH3OH methanol: new laser lines and assignments

We have reinvestigated ¹³CH₃OH as a source of far-infrared (FIR) laser emission using a CO₂ laser as a pumping source. Thirty new FIR laser lines in the range 36.5 μm to 202.6 μm were observed and characterized. Five of them have wavelengths between 36.5 and 75 μm and have sufficient intensity to be used in LMR spectroscopy. Using Fourier-transform spectroscopic data in the infrared (IR) and FIR regions we have determined the assignment for 10 FIR laser transitions and predict nine frequencies for laser lines which have yet to be observed. Received: 17 July 2000 / Published online: 6 December 2000     

650-nm laser emission under upconversion pumping at 1.064 μm in Tm<Superscript>+3</Superscript>: ZBLAN fiber laser

We report for the first time continuous wave (CW) red laser emission in Tm⁺³-doped ZBLAN fiber laser, operated at 650 nm (¹ G ₄ → ³ F ₄ transition of Tm⁺³). The excitation uses a three step upconversion scheme. The pump source is a Nd:YAG laser operated at 1.064 μm. A laser output power of CW 80 mW was obtained for 1.42 W of launched pump power. The slope efficiency with respect to launched pump power was measured to be 7.7%. The temporal behavior of the emitted laser is also addressed.     

Laser induced breakdown spectroscopy of germane plasma induced by IR CO2 pulsed laser

Laser-induced breakdown spectroscopy (LIBS) in germane (GeH₄), initially at room temperature and pressures ranging from 2 to 10 kPa, was studied using a high-power transverse excitation atmospheric (TEA) CO₂ laser (λ=10.653 μm, τ _FWHM=64 ns and power densities ranging from 0.28 to 5.52 GW cm⁻²). The strong emission spectrum of the generated plasma is mainly due to electronic relaxation of excited Ge, H and ionic fragments Ge⁺, Ge²⁺ and Ge³⁺. The weak emission is due to molecular bands of H₂. Excitation temperatures of 8100±300 K and 23,500±2500 K were estimated by Ge atomic and Ge⁺ singly ionized lines, respectively. Electron number densities of the order of (0.7–6.2)×10¹⁷ cm⁻³ were deduced from the Stark broadening of several atomic Ge lines. The characteristics of the spectral emission intensities from different species have been investigated as functions of the germane pressure and laser irradiance. Optical breakdown threshold intensities in germane at 10.653 μm have been determined. The mechanism of initiation of the laser-induced plasma in germane has been analyzed.     

Efficient tunable laser operation of diode- pumped Yb,Tm:KY(WO4)2 around 1.9 μm

A new laser medium – Yb,Tm:KY(WO₄)₂ – for diode pumped solid state laser applications operating around 1.9 to 2.0 μm has been investigated and the main laser characteristics are presented. Diode pumping at 981 nm and around 805 nm was realised. For 981-nm pumping, the excitation occurs into Yb³⁺ ions followed by an energy transfer to Tm³⁺ions. A slope efficiency of 19% was realised. For pumping around 805 nm, the excitation occurs directly into the Tm³⁺ ions. Here a maximum slope efficiency of 52%, an optical efficiency of 40%, and output powers of more than 1 W were realised. Using a birefringent quartz plate as an intracavity tuning element, the tunability of the Yb,Tm:KY(WO₄)₂ laser in the spectral range of 1.85–2.0 μm has been demonstrated. The possibility of laser operation in a microchip cavity configuration for this material has also been shown. Received: 12 March 2002 / Revised version: 20 May 2002 / Published online: 25 September 2002 RID="*" ID="*"Corresponding author. Fax: +49-531/592-4116, E-mail: stefan.kueck@ptb.de     

Structural changes induced on strontium barium niobate glass by femtosecond laser irradiation

Localized modification of the optical properties of erbium doped strontium barium niobate (SBN) glass has been performed using femtosecond laser irradiation. The samples, with composition SrO–BaO–Nb₂O₅–B₂O₅ and doped with 5%mol of Er³⁺, were fabricated using a melt-quenching method. The samples were irradiated with different number of pulses per spot (1–50 pulses) at two different laser fluences (2.6 and 5.6 J/cm²) by using an fs laser amplifier operating at 800 nm and generating pulses with a duration of 120 fs. Micro-luminescent microscopy, using an Ar⁺ laser as excitation source, has been used to analyze the modifications of the luminescent properties of the sample upon fs laser exposure. The emissions of the Er³⁺: ⁴I_11/2→⁴I_15/2 and ⁴I_13/2→⁴I_15/2 transitions allow appreciating the structural modifications caused by femtosecond laser exposure. The lifetimes of the levels involved in these transitions were measured inside and outside the laser irradiated region. These measurements have been compared with those obtained in bulk glass ceramic sample, which is obtained from the glass precursor by a thermal treatment in order to estimate the optimal conditions to produce nanocrystals in a localized region by ultrafast laser irradiation.