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

Journal of Applied Physics

Upconversion as a discriminating tool in site-selective spectroscopy of the praseodymium ion in Y3Al5O12

G. Özen, Ottavio Forte, Baldassare Di Bartolo, John Collins

Published Jul 15, 2007• 16 citations
Publisher

Abstract

We exploit the upconversion process, utilizing it as a sensitive tool in site-selective spectroscopy of rare earth ion-doped solids. In the Y3Al5O12:Pr3+ praseodymium-doped yttrium aluminum garnet (YAG:Pr) crystals the Pr ions are situated in sites having slightly different environments. Under pulsed excitation into the D21 level, the upconverted emission from the P03 level of each Pr subsystem exhibits its unique, and easily identifiable, response to pulsed excitation, simplifying the process of selectively exciting ions in different sites. Using this technique, we have been able to identify three different sites in a sample of YAG with Pr concentration of 0.5%. We present the physical reasons for the sensitivity of this technique as an example of a useful approach to distinguish among atomic systems residing in slightly dissimilar environments.

DOI
10.1063/1.2753685

Related papers

Optical detection of a single rare-earth ion in a crystal

Roman L. Kolesov, Kangwei Xia, R. Reuter +5 more

Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr3+ ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr3+ ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications. The optical transitions that occur in rare-earth-doped crystals offer promise for quantum information storage and processing. Kolesovet al.report the optical detection of a single praseodymium ion residing in a crystal host by using an excited-state absorption process to enhance its fluorescence yield.

Nature Communications•Aug 28, 2012•279 citations

Hyperfine measurements of the D21 −3 H4 transition in Pr3+ : Yttrium aluminum garnet using photon echo

M. K. Kim, Ravinder Kachru

The hyperfine structure of the $^{1}\mathrm{D}_{2}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{H}}_{4}$ transition of ${\mathrm{Pr}}^{3+}$: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the $^{1}\mathrm{D}_{2}$ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of ${\mathrm{Pr}}^{3+}$ impurity ions in YAG is lowered to ${C}_{2}$ from the ${D}_{2}$ symmetry of ${\mathrm{Y}}^{3+}$ ions.

Physical review. B, Condensed matter•Aug 1, 1989•10 citations

Evaluation of critical distances for energy transfer between Pr3+ and Ce3+ in yttrium aluminium garnet

Peng Zeng, Xiantao Wei, Shaoshuai Zhou +2 more

A series of Pr3+/Ce3+ doped yttrium aluminium garnet (Y3Al5O12 or simply YAG) phosphors were synthesized to investigate the energy transfer between Pr3+ and Ce3+ for their potential application in a white light-emitting diode and quantum information storage and processing. The excitation and emission spectra of YAG:Pr3+/Ce3+ were measured and analyzed, and it revealed that the reabsorption between Pr3+ and Ce3+ was so weak that it can be ignored, and the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) did occur. By analyzing the excitation and the emission spectra, the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) was examined in detail with an original strategy deduced from fluorescence dynamics and the Dexter energy transfer theory, and the critical distances of energy transfer were derived to be 7.9 Å and 4.0 Å for Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2), respectively. The energy transfer rates of the two processes of various concentrations were discussed and evaluated. Furthermore, for the purpose of sensing a single Pr3+ state with a Ce3+ ion, the optimal distance of Ce3+ from Pr3+ was evaluated as 5.60 Å, where the probability of success reaches its maximum value of 78.66%, and meanwhile the probabilities were evaluated for a series of Y3+ sites in a YAG lattice. These results will be of valuable reference for achievement of the optimal energy transfer efficiency in Pr3+/Ce3+ doped YAG and other similar systems.

Journal of Applied Physics•Sep 2, 2016•10 citations

Spin Hamiltonian characterization and refinement for Pr 3 + :YAlO 3 and Pr 3 + :Y 2 SiO 5

Marko Lovrić, Philipp Glasenapp, Dieter Suter

Rare-earth ions in dielectric crystals play an important role in high-resolution laser spectroscopy and are interesting candidates for storing quantum states of photons. We characterize the praseodymium hyperfine interaction of the ground-state (${}^{3}$H${}_{4}$) and one excited-state (${}^{1}$D${}_{2}$) for two important compounds: praseodymium doped in yttrium aluminum perovskite and praseodymium doped in yttrium orthosilicate. The spin Hamiltonian parameters are determined by numerical analysis of Raman-heterodyne spectra, which were collected for a range of static external magnetic field strengths and orientations. For Pr${}^{3+}$:YAlO${}_{3}$, we present a full analysis without restrictions for the Zeeman and quadrupole tensors, and our new characterization for Pr${}^{3+}$:Y${}_{2}$SiO${}_{5}$ resolves a controversy in the literature.

Physical Review B•Jan 24, 2012•24 citations

Spectroscopy properties of a single praseodymium ion in a crystal

Kangwei Xia, Roman Kolesov, Ya Wang +5 more

Abstract Addressing and coherent control of single atoms in solids, with both optical and nuclear spin degrees of freedom is of particularly interest for applications ranging from nanoscale sensing to quantum computing. Here, we performed the spectroscopy study of single praseodymium ions in an yttrium aluminum garnet crystal at cryogenic temperature. The single nuclear spin of individual praseodymium ions is detected through a background-free optical upconversion readout technique. Single ions show stable photoluminescence with spectrally resolved hyperfine splitting of the praseodymium ground state. Based on this measurement, optical Rabi and optically detected nuclear magnetic resonance measurements are performed to study their spin coherence properties. We find short the spin coherence times of praseodymium nuclear spins which we attribute to spin phonon coupling.

arXiv:1706.08736•New Journal of Physics•May 21, 2020•13 citations

Spectroscopy properties of a single praseodymium ion in a crystal

Kangwei Xia, Roman L. Kolesov, Ya Wang +5 more

AbstractAddressing and coherent control of single atoms in solids, with both optical and nuclear spin degrees of freedom is of particularly interest for applications ranging from nanoscale sensing to quantum computing. Here, we performed the spectroscopy study of single praseodymium ions in an yttrium aluminum garnet crystal at cryogenic temperature. The single nuclear spin of individual praseodymium ions is detected through a background-free optical upconversion readout technique. Single ions show stable photoluminescence with spectrally resolved hyperfine splitting of the praseodymium ground state. Based on this measurement, optical Rabi and optically detected nuclear magnetic resonance measurements are performed to study their spin coherence properties. We find short the spin coherence times of praseodymium nuclear spins which we attribute to spin phonon coupling.

•Jan 1, 2020•11 citations
We exploit the upconversion process, utilizing it as a sensitive tool in site-selective spectroscopy of rare earth ion-doped solids. In the Y3Al5O12:Pr3+ praseodymium-doped yttrium aluminum garnet (YAG:Pr) crystals the Pr ions are situated in sites having slightly different environments. Under pulsed excitation into the D21 level, the upconverted emission from the P03 level of each Pr subsystem exhibits its unique, and easily identifiable, response to pulsed excitation, simplifying the process of selectively exciting ions in different sites. Using this technique, we have been able to identify three different sites in a sample of YAG with Pr concentration of 0.5%. We present the physical reasons for the sensitivity of this technique as an example of a useful approach to distinguish among atomic systems residing in slightly dissimilar environments.
Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr3+ ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr3+ ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications. The optical transitions that occur in rare-earth-doped crystals offer promise for quantum information storage and processing. Kolesovet al.report the optical detection of a single praseodymium ion residing in a crystal host by using an excited-state absorption process to enhance its fluorescence yield.
The hyperfine structure of the 1D2^{1}\mathrm{D}_{2}1D2​${\mathrm{\ensuremath{-}}}^{3}$H4{\mathrm{H}}_{4}H4​ transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+: yttrium aluminum garnet (YAG) is studied using a photon echo modulation technique. The Fourier transform of modulation data gives hyperfine frequencies of the 1D2^{1}\mathrm{D}_{2}1D2​ state as 3.42 and 5.96 MHz. The photon echo modulation is a very sensitive function of the atomic environment, and we find that the site symmetry of Pr3+{\mathrm{Pr}}^{3+}Pr3+ impurity ions in YAG is lowered to C2{C}_{2}C2​ from the D2{D}_{2}D2​ symmetry of Y3+{\mathrm{Y}}^{3+}Y3+ ions.
A series of Pr3+/Ce3+ doped yttrium aluminium garnet (Y3Al5O12 or simply YAG) phosphors were synthesized to investigate the energy transfer between Pr3+ and Ce3+ for their potential application in a white light-emitting diode and quantum information storage and processing. The excitation and emission spectra of YAG:Pr3+/Ce3+ were measured and analyzed, and it revealed that the reabsorption between Pr3+ and Ce3+ was so weak that it can be ignored, and the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) did occur. By analyzing the excitation and the emission spectra, the energy transfer from Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2) was examined in detail with an original strategy deduced from fluorescence dynamics and the Dexter energy transfer theory, and the critical distances of energy transfer were derived to be 7.9 Å and 4.0 Å for Pr3+ (5d) to Ce3+ (5d) and Ce3+ (5d) to Pr3+ (1D2), respectively. The energy transfer rates of the two processes of various concentrations were discussed and evaluated. Furthermore, for the purpose of sensing a single Pr3+ state with a Ce3+ ion, the optimal distance of Ce3+ from Pr3+ was evaluated as 5.60 Å, where the probability of success reaches its maximum value of 78.66%, and meanwhile the probabilities were evaluated for a series of Y3+ sites in a YAG lattice. These results will be of valuable reference for achievement of the optimal energy transfer efficiency in Pr3+/Ce3+ doped YAG and other similar systems.
Rare-earth ions in dielectric crystals play an important role in high-resolution laser spectroscopy and are interesting candidates for storing quantum states of photons. We characterize the praseodymium hyperfine interaction of the ground-state (3{}^{3}3H4{}_{4}4​) and one excited-state (1{}^{1}1D2{}_{2}2​) for two important compounds: praseodymium doped in yttrium aluminum perovskite and praseodymium doped in yttrium orthosilicate. The spin Hamiltonian parameters are determined by numerical analysis of Raman-heterodyne spectra, which were collected for a range of static external magnetic field strengths and orientations. For Pr3+{}^{3+}3+:YAlO3{}_{3}3​, we present a full analysis without restrictions for the Zeeman and quadrupole tensors, and our new characterization for Pr3+{}^{3+}3+:Y2{}_{2}2​SiO5{}_{5}5​ resolves a controversy in the literature.
Abstract Addressing and coherent control of single atoms in solids, with both optical and nuclear spin degrees of freedom is of particularly interest for applications ranging from nanoscale sensing to quantum computing. Here, we performed the spectroscopy study of single praseodymium ions in an yttrium aluminum garnet crystal at cryogenic temperature. The single nuclear spin of individual praseodymium ions is detected through a background-free optical upconversion readout technique. Single ions show stable photoluminescence with spectrally resolved hyperfine splitting of the praseodymium ground state. Based on this measurement, optical Rabi and optically detected nuclear magnetic resonance measurements are performed to study their spin coherence properties. We find short the spin coherence times of praseodymium nuclear spins which we attribute to spin phonon coupling.
AbstractAddressing and coherent control of single atoms in solids, with both optical and nuclear spin degrees of freedom is of particularly interest for applications ranging from nanoscale sensing to quantum computing. Here, we performed the spectroscopy study of single praseodymium ions in an yttrium aluminum garnet crystal at cryogenic temperature. The single nuclear spin of individual praseodymium ions is detected through a background-free optical upconversion readout technique. Single ions show stable photoluminescence with spectrally resolved hyperfine splitting of the praseodymium ground state. Based on this measurement, optical Rabi and optically detected nuclear magnetic resonance measurements are performed to study their spin coherence properties. We find short the spin coherence times of praseodymium nuclear spins which we attribute to spin phonon coupling.