Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Applied Physics Letters

Measurement of excited-state-absorption loss for Ce3+ in Y3Al5O12 and implications for tunable 5d→4f rare-earth lasers

Ralph R. Jacobs, William F. Krupke, Marvin J. Weber

Published Sep 1, 1978• 203 citations
Publisher

Abstract

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.

DOI
10.1063/1.90395

Related papers

Excited-state absorption in Pr3+ : Y3 Al5 O12

Y. M. Cheung, Swapan Kumar Gayen

The optical-absorption transitions originating from the lowest 4f5d excited state of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{3}$${\mathrm{Al}}_{5}$${\mathrm{O}}_{12}$ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ ${\mathrm{cm}}^{2}$. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of ${\mathrm{Pr}}^{3+}$ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the $^{3}$${\mathit{P}}_{0}$ and $^{1}$${\mathit{D}}_{2}$ excited states of the 4${\mathit{f}}^{2}$ configuration of ${\mathrm{Pr}}^{3+}$ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ ${\mathrm{cm}}^{2}$ and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ ${\mathrm{cm}}^{2}$ for transitions from the $^{3}$${\mathit{P}}_{0}$ and $^{1}$${\mathit{D}}_{2}$ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.

Physical review. B, Condensed matter•Jun 1, 1994•50 citations

Optical-absorption and photoionization measurements from the excited states of Ce 3 + : Y 3 Al 5 O 12

D. S. Hamilton, Swapan Kumar Gayen, Gerald J. Pogatshnik +2 more

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.

Physical review. B, Condensed matter•May 1, 1989•143 citations

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

Hisao Uchiki, Shinsaku Honma, Kunihiko Tanaka +2 more

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)

Physica status solidi. C, Conferences and critical reviews/Physica status solidi. C, Current topics in solid state physics•Jul 4, 2013•2 citations

Suppression of excited-state absorption: A path to ultraviolet tunable solid-state lasers

Elena Kuznetsova, Roman L. Kolesov, Olga A. Kocharovskaya

A method of suppression of losses due to excited-state absorption (ESA) in laser crystals is proposed, based on the well-known phenomenon of electromagnetically induced transparency. Typical situations in which ESA prevents lasing are considered. Theoretical analysis shows that by using an additional driving laser field one can inhibit ESA and make lasing possible. On the basis of available spectroscopic information estimates for rare-earth-ion-doped laser materials are presented. They show the feasibility of obtaining optical gain at parity-allowed $4{f}^{n}\ensuremath{\leftrightarrow}4{f}^{n\ensuremath{-}1}5d$ transitions of rare-earth ions in the ultraviolet spectral region after suppression of ESA at an emission wavelength into the conduction band of a host material.

Physical Review A•Oct 4, 2004•17 citations

Two-Photon Excitations of Higher 5d States in Ce3+:CaF2

Swapan Kumar Gayen, Gerald J. Pogatshnik, D. S. Hamilton

The 4f-->5d near-ultraviolet transitions in Ce3+:CaF2 are dipole allowed in one-photon absorption (OPA) and first-order parity-forbidden for two-photon absorption (TPA). A relaxation of the parity selection rule due to odd crystal-field components has previously been observed1 in the TPA from the 4f ground state to the lowest 5d state. In this paper the TPA measurements are extended to include transitions to the higher 5d states.

International Conference on Luminescence - 1984•Jan 1, 1984•2 citations

Measurement of linewidths and permanent electric dipole moment change of the Ce 4 f -5d transition in Y2SiO5 for qubit readout scheme in rare-earth ion based quantum computing

Ying-yan, LiheZhen, JunXu +8 more

In this work the inhomogeneous (zero-phonon line) and homogeneous linewidths and the permanent electric dipole moment change (averaged value of all dipole orientations) for the Ce 4f -5d transition in Y2SiO5 were measured in order to investigate the possibility for using Ce as a sensor to detect the hyperfine state of a spatially close-lying Pr or Eu ion. The experiments were carried out on Ce doped or Ce-Pr co-doped single Y2SiO5 crystals. The homogeneous linewidth is essentially limited by the excited state lifetime. Based on the linewidth measurements, the oscillator strength, absorption cross section, and saturation intensity were calculated to be about 6.2(±1.7) × 10？7, 4.5(±1.3) × 10？19 m2, and 1.4(±0.4) × 107 W/m2, respectively. The difference in permanent dipole moment, μCe, between the ground and excited states of the Ce ion was measured as 9.6(±5.3) × 10？30 C m. These measurements indicate that Ce is a promising readout ion to probe a single-ion qubit state for the quantum computing scheme using rare-earth ions.

•May 30, 2013•0 citations
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.
The optical-absorption transitions originating from the lowest 4f5d excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ have been studied. The experimental arrangement uses a 7-ns 266-nm light pulse to populate the lowest 4f5d state, and a spatially overlapped, time-sequenced pulse from a frequency-tunable dye laser to induce transitions from that excited state. The excited-state-absorption (ESA) spectrum covering the 900--300-nm probe wavelength range is characterized by two broad peaks centered at 700 and 350 nm on a slowly rising background. The peak ESA cross section at 355 nm is (1\ifmmode\pm\else\textpm\fi{}0.1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}17}$ cm2{\mathrm{cm}}^{2}cm2. The position, shape, and strength of the spectrum suggest that the terminal states of the ESA transitions are the second 4f5d state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ and the conduction band of the host lattice. The ESA measurements have been extended to transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states of the 4f2{\mathit{f}}^{2}f2 configuration of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as well. The ESA cross sections at a probe wavelength of 532 nm are (8\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 and (5.7\ifmmode\pm\else\textpm\fi{}0.6)\ifmmode\times\else\texttimes\fi{}${10}^{\mathrm{\ensuremath{-}}19}$ cm2{\mathrm{cm}}^{2}cm2 for transitions from the 3^{3}3P0{\mathit{P}}_{0}P0​ and 1^{1}1D2{\mathit{D}}_{2}D2​ excited states, respectively. The terminal state of ESA transitions from these two levels is the lowest 4f5d state. The strong ESA completely inhibits the potential laser action based on emission from these states in this crystal.
The optical transitions in Ce3+{\mathrm{Ce}}^{3+}Ce3+:Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ from the lowest 5d excited state of the Ce3+{\mathrm{Ce}}^{3+}Ce3+ 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{}${10}^{\mathrm{\ensuremath{-}}17}$ cm2{\mathrm{cm}}^{2}cm2 at 700 nm. The ESA spectrum was measured from 600 to 880 nm and is used to construct an energy-level diagram for the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions relative to the energy-band states of the Y3{\mathrm{Y}}_{3}Y3​Al5{\mathrm{Al}}_{5}Al5​O12{\mathrm{O}}_{12}O12​ 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.
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)
A method of suppression of losses due to excited-state absorption (ESA) in laser crystals is proposed, based on the well-known phenomenon of electromagnetically induced transparency. Typical situations in which ESA prevents lasing are considered. Theoretical analysis shows that by using an additional driving laser field one can inhibit ESA and make lasing possible. On the basis of available spectroscopic information estimates for rare-earth-ion-doped laser materials are presented. They show the feasibility of obtaining optical gain at parity-allowed $4{f}^{n}\ensuremath{\leftrightarrow}4{f}^{n\ensuremath{-}1}5d$ transitions of rare-earth ions in the ultraviolet spectral region after suppression of ESA at an emission wavelength into the conduction band of a host material.
In this work the inhomogeneous (zero-phonon line) and homogeneous linewidths and the permanent electric dipole moment change (averaged value of all dipole orientations) for the Ce 4f -5d transition in Y2SiO5 were measured in order to investigate the possibility for using Ce as a sensor to detect the hyperfine state of a spatially close-lying Pr or Eu ion. The experiments were carried out on Ce doped or Ce-Pr co-doped single Y2SiO5 crystals. The homogeneous linewidth is essentially limited by the excited state lifetime. Based on the linewidth measurements, the oscillator strength, absorption cross section, and saturation intensity were calculated to be about 6.2(±1.7) × 10？7, 4.5(±1.3) × 10？19 m2, and 1.4(±0.4) × 107 W/m2, respectively. The difference in permanent dipole moment, μCe, between the ground and excited states of the Ce ion was measured as 9.6(±5.3) × 10？30 C m. These measurements indicate that Ce is a promising readout ion to probe a single-ion qubit state for the quantum computing scheme using rare-earth ions.