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

arXiv:2203.09245 · ACS Nano

Deterministic Relation between Optical Polarization and Lattice Symmetry Revealed in Ion-Doped Single Microcrystals

Peng Li, Yaxin Guo, Ao Liu, Xin Yan Yue, Taoli Yuan, Jingping Zhu, Yanpeng Zhang, Feng Li

Published May 17, 2022• 36 citations
arXivHTMLPDF

Abstract

Rare-earth ion doped crystals are of great significance for microsensing and quantum information, while the ions in the crystals emit light with spontaneous partial polarization, which is, though believed to be originated from the crystal lattice structure, still lacking a deterministic explanation that can be tested with quantitative accuracy. We report experimental evidence showing the profound physical relation between the polarization degree of light emitted by the doped ion and the lattice symmetry by demonstrating, with high precision, that the lattice constant ratio c / a directly quantifies the macroscopic effective polar angle of the electric and magnetic dipoles, which essentially determines the linear polarization degree of the emission. Based on this result, we further propose a pure optical technology to identify the three-dimensional orientation of a rod-shaped single microcrystal using the polarization-resolved microspectroscopy. Our results, demonstrating the physical origin of light polarization in ion-doped crystals, allow work toward on-demand polarization control with crystallography and provide a versatile platform for polarization-based microscale sensing in dynamical systems.

DOI
10.1021/acsnano.2c02756

Related papers

Vectorial Symmetry Decoding with Single-Particle Precision via Room-Temperature Lanthanide Luminescence Polarimetry

Peng Li, Yaxin Guo, Yan, Yaoxu +10 more

Determining the local symmetry of luminescent centers in crystals is critical for understanding and controlling their optical transitions, yet current methods are limited by stringent experimental requirements and ambiguous symmetry assignments. Here, we develop a robust computational electromagnetics framework that directly connect the local symmetry and chirality of rare-earth-doped single crystals to the polarization states of their emitted light. This framework is experimentally validated through the precise determination of point and space group symmetries using high-resolution, polarization-resolved micro-photoluminescence (μ-PL) spectra. Unlike conventional approaches that usually rely on analyzing multiple transitions at cryogenic temperatures, our technique operates at room temperature, requires only a single optical transition, and enables accurate orientation of symmetry axes. This enables deterministic polarization control of nano-emitters by tailoring symmetry groups and selecting appropriate transition dipoles, eliminating the need for bulky or complex photonic structures. Additionally, we demonstrate the function of bio-sensing, via determining single particle orientations in complex cellular environments using minimal polarization measurements. These results pave the way for advances in energy transfer systems, ultra-bright rare-earth nanocrystals, nanophotonic materials, and real-time single-particle tracking in biological contexts.

arXiv:2501.07199•Jan 13, 2025•0 citations

Polarization Dynamics of Solid-State Quantum Emitters

Anand Kumar, Çağlar Samaner, Chanaprom Cholsuk +10 more

Quantum emitters in solid-state crystals have recently attracted a great deal of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single-photon sources to reveal the origin and temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.

ACS Nano•Feb 9, 2024•24 citations

Measuring the Magnetic Dipole Transition of Single Nanorods by Spectroscopy and Fourier Microscopy

Reinaldo Chacón, Aymeric Leray, Jeongmo Kim +6 more

Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the ${}^{5}{D}_{0}{\ensuremath{\rightarrow}}^{7}{F}_{1}$ transition dipole vector in individual ${\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}$ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of ${\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}$ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.

arXiv:2109.08574•Physical Review Applied•Nov 5, 2020•22 citations

Polarization Dynamics of Solid-State Quantum Emitters

Anand Kumar, Çağlar Samaner, Chanaprom Cholsuk +10 more

Quantum emitters in solid-state crystals have recently attracted a lot of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that play a crucial role in the applications, such as quantum computation that uses the indistinguishability of photons. However, the degree of single photon polarization is typically quantified using time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single photon sources to reveal the origin and the temporal evolution of dipole orientation in solid-state quantum emitters. The angle of excitation and emission dipoles relative to the crystal axes are determined experimentally and then calculated using density functional theory, which results in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics reveal a strongly modified linear polarization visibility that depends on the excited state decay time of individual excitation. This effect can be traced back potentially to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further be used to improve the performance of polarization-sensitive experiments, in particular that of quantum communication with single photon emitters.

arXiv:2303.04732•Mar 8, 2023•4 citations

Symmetry considerations regarding light propagation and light polarization for coherent interactions with ions in crystals

Yiwen Sun, G. M. Wang, R. L. Cone +2 more

Spectroscopic studies and the efficiency of optical coherent transient devices can be adversely affected by interference arising from several distinct Rabi frequencies associated with crystallographically equivalent but orientationally inequivalent crystal sites. General symmetry principles have been used to find light field directions that guarantee both optimum single-Rabi-frequency interaction and the most efficient coherent transient generation in arbitrary crystals. This theoretical analysis has been applied experimentally to a wide range of rare earth crystals, many of which are important for technological applications. Site interference in optical nutation provides a simple illustration of this effect. Optimum single-Rabi-frequency nutation signal was obtained for the ${}^{3}{H}_{6}(1)$ to ${}^{3}{H}_{4}(1)$ transition of 0.1% ${\mathrm{Tm}}^{3+}:{\mathrm{Y}}_{3}{\mathrm{Al}}_{5}{\mathrm{O}}_{12}$ when the light $\stackrel{\ensuremath{\rightarrow}}{E}$ vector is along special crystal directions $〈111〉$ or $〈001〉.$ Quantitative comparison of nutation frequencies for light polarized along different directions allowed the determination of the optical transition dipole moment to be along $〈110〉$ for this transition. The transition dipole moment derived from the nutation signal agrees within 15% with that obtained from absorption experiments. Other applications of nutation measurements are discussed, including a procedure for determining site occupancy in crystals with crystallographically inequivalent sites.

Physical review. B, Condensed matter•Dec 15, 2000•71 citations

Investigations of spectral dynamics in rare earth ion doped crystals using high resolution laser techniques

Graf, Felix R.

Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,

•Jan 1, 1998•5 citations
Rare-earth ion doped crystals are of great significance for microsensing and quantum information, while the ions in the crystals emit light with spontaneous partial polarization, which is, though believed to be originated from the crystal lattice structure, still lacking a deterministic explanation that can be tested with quantitative accuracy. We report experimental evidence showing the profound physical relation between the polarization degree of light emitted by the doped ion and the lattice symmetry by demonstrating, with high precision, that the lattice constant ratio c / a directly quantifies the macroscopic effective polar angle of the electric and magnetic dipoles, which essentially determines the linear polarization degree of the emission. Based on this result, we further propose a pure optical technology to identify the three-dimensional orientation of a rod-shaped single microcrystal using the polarization-resolved microspectroscopy. Our results, demonstrating the physical origin of light polarization in ion-doped crystals, allow work toward on-demand polarization control with crystallography and provide a versatile platform for polarization-based microscale sensing in dynamical systems.
Determining the local symmetry of luminescent centers in crystals is critical for understanding and controlling their optical transitions, yet current methods are limited by stringent experimental requirements and ambiguous symmetry assignments. Here, we develop a robust computational electromagnetics framework that directly connect the local symmetry and chirality of rare-earth-doped single crystals to the polarization states of their emitted light. This framework is experimentally validated through the precise determination of point and space group symmetries using high-resolution, polarization-resolved micro-photoluminescence (μ-PL) spectra. Unlike conventional approaches that usually rely on analyzing multiple transitions at cryogenic temperatures, our technique operates at room temperature, requires only a single optical transition, and enables accurate orientation of symmetry axes. This enables deterministic polarization control of nano-emitters by tailoring symmetry groups and selecting appropriate transition dipoles, eliminating the need for bulky or complex photonic structures. Additionally, we demonstrate the function of bio-sensing, via determining single particle orientations in complex cellular environments using minimal polarization measurements. These results pave the way for advances in energy transfer systems, ultra-bright rare-earth nanocrystals, nanophotonic materials, and real-time single-particle tracking in biological contexts.
Quantum emitters in solid-state crystals have recently attracted a great deal of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that plays a crucial role in various applications, such as quantum computation, which uses the indistinguishability of photons. However, the degree of single-photon polarization is typically quantified using the time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single-photon sources to reveal the origin and temporal evolution of the dipole orientation in solid-state quantum emitters. The angles of the excitation and emission dipoles relative to the crystal axes were determined experimentally and then calculated using density functional theory, which resulted in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics revealed a strongly modified linear polarization visibility that depends on the excited-state decay time of the individual excitation. This effect can potentially be traced back to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further improve the performance of polarization-sensitive experiments, particularly that for quantum communication with single-photon emitters.
Rare-earth doped nanocrystals possess optical transitions with significant either electric or magnetic dipole characters. They are of considerable interest for understanding and engineering light-matter interactions at the nanoscale with numerous applications in nanophotonics. Here, we study the ${}^{5}{D}_{0}{\ensuremath{\rightarrow}}^{7}{F}_{1}$ transition dipole vector in individual NaYF4:Eu3+{\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}NaYF4​:Eu3+ nanorod crystals by Fourier and confocal microscopies. A single-crystal host matrix leads to narrow emission lines at room temperature that permit separation of the Stark sublevels resulting from the crystal-field splitting. We observe a fully magnetic transition and low variability of the transition dipole orientation over several single nanorods. We estimate the proportion of the dipole transitions for the Stark sublevels. We also determine an effective altitude of the rod with respect to the substrate. The narrow emission lines characteristic of NaYF4:Eu3+{\mathrm{NaYF}}_{4}:{\mathrm{Eu}}^{3+}NaYF4​:Eu3+ ensure well-defined electric or magnetic transitions, and are thus instrumental for probing locally their electromagnetic environment by standard confocal microscopy.
Quantum emitters in solid-state crystals have recently attracted a lot of attention due to their simple applicability in optical quantum technologies. The polarization of single photons generated by quantum emitters is one of the key parameters that play a crucial role in the applications, such as quantum computation that uses the indistinguishability of photons. However, the degree of single photon polarization is typically quantified using time-averaged photoluminescence intensity of single emitters, which provides limited information about the dipole properties in solids. In this work, we use single defects in hexagonal boron nitride and nanodiamond as efficient room-temperature single photon sources to reveal the origin and the temporal evolution of dipole orientation in solid-state quantum emitters. The angle of excitation and emission dipoles relative to the crystal axes are determined experimentally and then calculated using density functional theory, which results in characteristic angles for every specific defect that can be used as an efficient tool for defect identification and understanding their atomic structure. Moreover, the temporal polarization dynamics reveal a strongly modified linear polarization visibility that depends on the excited state decay time of individual excitation. This effect can be traced back potentially to the excitation of excess charges in the local crystal environment. Understanding such hidden time-dependent mechanisms can further be used to improve the performance of polarization-sensitive experiments, in particular that of quantum communication with single photon emitters.
Spectroscopic studies and the efficiency of optical coherent transient devices can be adversely affected by interference arising from several distinct Rabi frequencies associated with crystallographically equivalent but orientationally inequivalent crystal sites. General symmetry principles have been used to find light field directions that guarantee both optimum single-Rabi-frequency interaction and the most efficient coherent transient generation in arbitrary crystals. This theoretical analysis has been applied experimentally to a wide range of rare earth crystals, many of which are important for technological applications. Site interference in optical nutation provides a simple illustration of this effect. Optimum single-Rabi-frequency nutation signal was obtained for the 3H6(1){}^{3}{H}_{6}(1)3H6​(1) to 3H4(1){}^{3}{H}_{4}(1)3H4​(1) transition of 0.1% Tm3+:Y3Al5O12{\mathrm{Tm}}^{3+}:{\mathrm{Y}}_{3}{\mathrm{Al}}_{5}{\mathrm{O}}_{12}Tm3+:Y3​Al5​O12​ when the light $\stackrel{\ensuremath{\rightarrow}}{E}$ vector is along special crystal directions 〈111〉〈111〉〈111〉 or 〈001〉.〈001〉.〈001〉. Quantitative comparison of nutation frequencies for light polarized along different directions allowed the determination of the optical transition dipole moment to be along 〈110〉〈110〉〈110〉 for this transition. The transition dipole moment derived from the nutation signal agrees within 15% with that obtained from absorption experiments. Other applications of nutation measurements are discussed, including a procedure for determining site occupancy in crystals with crystallographically inequivalent sites.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,