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Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics

Site‐dependent excited state absorption in Ce‐doped CaGa2S4 single crystal

Hisao Uchiki, Shinsaku Honma, Kunihiko Tanaka, Chiharu Hidaka, Takeo Takizawa

Published Jul 4, 2013• 2 citations

Abstract

Abstract Excited state absorption (ESA) by Ce3+ ions in the 5d1 lowest excited state in Ce‐doped CaGa2S4 single crystal was investigated by nanosecond two‐pulse pump‐CW probe spectroscopy. The first pump pulse of 425 nm excited the 4f ground state electron to the 5d1 first excited state and the second pump pulse of 589 nm was introduced at 13 ns after the first pump in order to selectively excite the 5d1 state. Transient intensity change of the CW probe of a diode laser of 780 nm was observed. Temporal behavior of photoluminescence intensity by the 5d1 to 4f state transition was also observed under excitation of the same two‐pulse pump. The experimental results can be explained by the model of site‐dependent excited state absorption. The photoluminescence is generated from the 5d1 states of Ce3+ at two sites with different decay time, whereas the excited state absorption takes place mainly from Ce3+ at one site as well as metastable Ce2+. The model predicts that optical gain by the 5d1 to 4f transition can be achieved by Ce3+ at the other site if the populations at both the 5d1 state of Ce3+ at the site resulting in ESA and Ce2+ can be bleached by simultaneous secondary optical pumping with an IR (e.g. Nd:YAG) laser. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

DOI: 10.1002/pssc.201200684

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Abstract Excited state absorption (ESA) by Ce3+ ions in the 5d1 lowest excited state in Ce‐doped CaGa2S4 single crystal was investigated by nanosecond two‐pulse pump‐CW probe spectroscopy. The first pump pulse of 425 nm excited the 4f ground state electron to the 5d1 first excited state and the second pump pulse of 589 nm was introduced at 13 ns after the first pump in order to selectively excite the 5d1 state. Transient intensity change of the CW probe of a diode laser of 780 nm was observed. Temporal behavior of photoluminescence intensity by the 5d1 to 4f state transition was also observed under excitation of the same two‐pulse pump. The experimental results can be explained by the model of site‐dependent excited state absorption. The photoluminescence is generated from the 5d1 states of Ce3+ at two sites with different decay time, whereas the excited state absorption takes place mainly from Ce3+ at one site as well as metastable Ce2+. The model predicts that optical gain by the 5d1 to 4f transition can be achieved by Ce3+ at the other site if the populations at both the 5d1 state of Ce3+ at the site resulting in ESA and Ce2+ can be bleached by simultaneous secondary optical pumping with an IR (e.g. Nd:YAG) laser. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Broad bandwidth 5d→4f transitions in Ce3+ have been considered for tunable laser action. In this letter, optical probe measurements of excited Ce3+ ions in Y3Al5O12 show that stimulated emission in the 550–610-nm region is not possible at 295 K because of excited-state absorption. Transient measurements demonstrate that part of this loss has ≈75-ns lifetime and is associated with absorption from the lowest 5d level; a longer-lifetime loss is also observed. The excited-state-absorption loss is reduced at lower temperatures.

Positive optical gain around 5 cm−1 (∼21 dB/cm) has been observed in Er3+-doped Ba2NaNb5O15 single crystal using a pump and probe experimental setup. High power laser pulses at 532 nm have been used as the pump source in order to strongly populate the S43/2(H211/2) levels of the Er3+ ions due to ground state absorption. Low signal beam cw laser radiation at 850 nm has been used as the probe beam to stimulate the emission associated with the S43/2(H211/2)→I413/2 electronic transition of the Er3+ ions. The process has been modelized as a four level system, and its population has been analyzed and simulated in order to study the gain dynamics. Optical amplification of the probe signal has been observed during the first 60 μs, which represents a good agreement between the measured lifetime of the S43/2(H211/2) levels and the reported simulation.

An experimental study of saturable absorption and excited-state absorption (ESA) in several inorganic saturable absorbers, Cr/sup 4+/:YAG, Cr/sup 4+/:GGG, and Cr/sup 4+/:YSGG, is presented. We provide the theoretical background of absorption characteristics in saturable absorbers that exhibit ESA, with some new results: approximate analytical solutions are proposed for the optical transmission in the case of a slow absorber, and for various light intensity conditions of spatially or temporally Gaussian beams in fast and slow absorbers. Experimentally, partial bleaching of the first excited state itself could be observed in Cr/sup 4+/:YAG at /spl lambda/=1064 nm, yielding the higher excited-state lifetime as /spl tau/*=(0.55/spl plusmn/0.1) ns. The regular transmission bleaching curve was measured in Cr/sup 4+/:GGG, for the first time in this material, yielding /spl sigma//sub ga/=(58/spl plusmn/5)/spl times/10/sup -1/ cm/sup 2/, and /spl sigma/e/sub s/=(13/spl plusmn/2)/spl times/10/sup -19/ cm/sup 2/ at /spl lambda/=1064 nm, ESA spectra were measured for the three materials between /spl sim/700 and 900 nm. All three exhibit crossing between saturable absorption at longer wavelengths and inverse saturable absorption at shorter wavelengths.

The optical transitions in

{\mathrm{Ce}}^{3+}

:

{\mathrm{Y}}_{3}

{\mathrm{Al}}_{5}

{\mathrm{O}}_{12}

from the lowest 5d excited state of the

{\mathrm{Ce}}^{3+}

ion to the host conduction band have been investigated. Two spatially overlapped and time-sequenced laser pulses were used to observe directly the excited-state absorption (ESA) and the two-step photoionization of the cerium ions. The peak cross section of the ESA transition is (1.0\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$

{\mathrm{cm}}^{2}

at 700 nm. The ESA spectrum was measured from 600 to 880 nm and is used to construct an energy-level diagram for the

{\mathrm{Ce}}^{3+}

ions relative to the energy-band states of the

{\mathrm{Y}}_{3}

{\mathrm{Al}}_{5}

{\mathrm{O}}_{12}

host. The energy gap between the lowest relaxed 5d state and the conduction-band edge is estimated to be 10 000 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. Strong-probe saturation measurements indicate a slow and inefficient back-transfer of excitation to the cerium ions following the ESA. Photoconductivity measurements were used to confirm the two-step photoionization of the cerium ions.

The sub-Doppler absorption laser spectroscopy at 728 nm transition from the 5 D 5 / 2 state to the 6 F state of cesium with linewidth near 10 MHz is first experimentally performed with indirect pumping from the ground state 6 S 1 / 2 to the state 7 P 3 / 2 by a 455.5 nm diode laser. Using a 455.5 nm diode laser as an indirect pump laser, several excited states will be populated due to spontaneous decay from the 7 P state. We first implement the sub-Doppler absorption laser spectroscopy at 728 nm from the 5 D 5 / 2 state to the 6 F state when Cs atoms within thermal glass cell decay to the 5 D 5 / 2 state. Due to velocity transfer effect, the hyperfine structure of 5 D 5 / 2 shows a mixed and complicated pattern but very clear structure when the 455.5 nm pumping laser is counter-propagating (or co-propagating) with the 728 nm probing laser.

The optical absorption, temperature dependences of the luminescence intensity and decay time, and the transient absorption spectra of a Cr 4+ : Gd 2 SiO 5 crystal were determined by the picosecond excitation and probing method. An analysis of the results showed that the induced absorption observed in the 600–650 nm range was due to 3 T 2 ( 3 F ) → 3 T 1 ( 3 P ) transitions from the excited state. The lifetimes of the 3 T 2 ( 3 F ) and 3 T 1 ( 3 F ) levels were estimated to be 15 ns and 12 ps, respectively. The cross section for absorption from the first excited state at the wavelength of 616 nm was (1.1 ± 0.6)×10 -18 cm 2 and that for absorption from the ground state at λ = 540 nm was (2.2 ± 1.1)×10 -18 cm 2 .