Spectroscopic detection of single Pr3+ ions on the H-3(4)-D-1(2) transition

Rare earth ions in crystals exhibit narrow spectral features and hyperfine-split ground states with exceptionally long coherence times. These features make them ideal platforms for quantum information processing in the solid state. Recently, we reported on the first high-resolution spectroscopy of single ions in yttrium orthosilicate nanocrystals via the transition at a wavelength of 488 nm. Here we show that individual praseodymium ions can also be detected on the more commonly studied transition at 606 nm. In addition, we present the first measurements of the second-order autocorrelation function, fluorescence lifetime, and emission spectra of single ions in this system as well as their polarization dependencies on both transitions. Furthermore, we demonstrate that by a proper choice of the crystallite, one can obtain narrower spectral lines and, thus, resolve the hyperfine levels of the excited state. We expect our results to make single-ion spectroscopy accessible to a larger scientific community.Rare earth ions in crystals exhibit narrow spectral features and hyperfine-split ground states with exceptionally long coherence times. These features make them ideal platforms for quantum information processing in the solid state. Recently, we reported on the first high-resolution spectroscopy of single ions in yttrium orthosilicate nanocrystals via the transition at a wavelength of 488 nm. Here we show that individual praseodymium ions can also be detected on the more commonly studied transition at 606 nm. In addition, we present the first measurements of the second-order autocorrelation function, fluorescence lifetime, and emission spectra of single ions in this system as well as their polarization dependencies on both transitions. Furthermore, we demonstrate that by a proper choice of the crystallite, one can obtain narrower spectral lines and, thus, resolve the hyperfine levels of the excited state. We expect our results to make single-ion spectroscopy accessible to a larger scientific community.

arXiv:1504.00857New Journal of PhysicsAug 10, 201534 citations

Spectroscopy of single rare earth ions (Conference Presentation)

Vahid Sandoghdar

Recently, we showed the first high-resolution spectroscopy and manipulation of single Pr3+ ions in the solid state using rare-earth doped crystals. The special feature of these systems is access to the hyperfine splitting caused by the interaction of the 4f electrons and the nucleus, leading to sets of sublevels with exceptionally long coherence times at cryogenic temperatures, on the order of minutes and hours. This ground state splitting can serve as a lambda level scheme, a key ingredient for many prospective applications in quantum optics, in particular for qubit storage and manipulation. In this presentation, we discuss our latest results and future challenges in reducing spectral diffusion and line broadening down to the expected natural linewidth, prospects for the use of microcavities or plasmonic nano-antennas to enhance the photon yield, and schemes for on-chip integration.Recently, we showed the first high-resolution spectroscopy and manipulation of single Pr3+ ions in the solid state using rare-earth doped crystals. The special feature of these systems is access to the hyperfine splitting caused by the interaction of the 4f electrons and the nucleus, leading to sets of sublevels with exceptionally long coherence times at cryogenic temperatures, on the order of minutes and hours. This ground state splitting can serve as a lambda level scheme, a key ingredient for many prospective applications in quantum optics, in particular for qubit storage and manipulation. In this presentation, we discuss our latest results and future challenges in reducing spectral diffusion and line broadening down to the expected natural linewidth, prospects for the use of microcavities or plasmonic nano-antennas to enhance the photon yield, and schemes for on-chip integration.

Apr 28, 20170 citations

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.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 CommunicationsAug 28, 2012279 citations

Hole-burning techniques for isolation and study of individual hyperfine transitions in inhomogeneously broadened solids demonstrated in Pr3+:Y2SiO5

Mattias Nilsson, Lars Rippe, Stefan Kröll +2 more

Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ . Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in ${\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in ${\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.

arXiv:cond-mat/0408515Physical Review BDec 30, 2004201 citations

Hyperfine structure, optical dephasing, and spectral-hole lifetime of single-crystalline Pr3+:La2(WO4)3

O. Guillot-Noël, Philippe Goldner, Y. Le Du +4 more

Most of the experiments related to quantum information applications, involving rare-earth doped inorganic crystals, are performed on yttrium orthosilicate single crystals. The work presented here is motivated by the search of new compounds which can be used in the field of quantum computing and/or quantum storage. Relaxation times and hyperfine structure of the $^{3}H_{4}(0)\ensuremath{\rightarrow}^{1}D_{2}(0)$ transition in 1.4% ${\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ at $4\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground $^{3}H_{4}(0)$ and the excited $^{1}D_{2}(0)$ states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about $14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}$ . The fluorescence dynamics of the $^{1}D_{2}$ level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of $2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ . The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the ${\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ compound make this crystal an interesting host for quantum applications.Most of the experiments related to quantum information applications, involving rare-earth doped inorganic crystals, are performed on yttrium orthosilicate single crystals. The work presented here is motivated by the search of new compounds which can be used in the field of quantum computing and/or quantum storage. Relaxation times and hyperfine structure of the $^{3}H_{4}(0)\ensuremath{\rightarrow}^{1}D_{2}(0)$ transition in 1.4% ${\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ at $4\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground $^{3}H_{4}(0)$ and the excited $^{1}D_{2}(0)$ states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about $14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}$. The fluorescence dynamics of the $^{1}D_{2}$ level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of $2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$. The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the ${\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ compound make this crystal an interesting host for quantum applications.

Physical Review BMay 15, 200719 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.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:1706.08736New Journal of PhysicsMay 21, 202013 citations

{\mathrm{Pr}}^{3+}

{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}

. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in

{\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}

has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.

{\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}

4\phantom{\rule{0.3em}{0ex}}\mathrm{K}

have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground

^{3}H_{4}(0)

and the excited

^{1}D_{2}(0)

states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about

14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}

. The fluorescence dynamics of the

^{1}D_{2}

level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of

2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}

. The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the

{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}

compound make this crystal an interesting host for quantum applications.