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Negative Refraction in Rare-Earth Doped Crystals

Deniz D. Yavuz, N. R. Brewer, Zachary Noel Buckholtz, Zach J. Simmons

Published Jun 9, 2016• 0 citations
OpenAlex

Abstract

Abstract : In this project, our long-term goal is to demonstrate the first negative refraction in atomic systems. Although the concept of negative refraction remained an academic curiosity for a long time, it is now well-understood that negative refraction may have important and far-reaching practical implications. The key challenge in observing negative refraction in the optical region of the spectrum is the weakness of the magnetic response. Our central experimental result during this project has been the first observation of Rabi flopping of a magnetic dipole transition in the optical region of the spectrum. We have performed this experiment using the 7F0-5D1 transition of europium ions in a cryogenically cooled doped crystal. This is a major result; we have shown for the firs time that an electron can interact sufficiently strongly with the magnetic field of a light wave and coherently move between the levels. Another important result during this project was the proposal for a new type of materials that exhibit negative refraction. Because of these achievements, observing negative refraction and left-handed electromagnetic waves in atomic systems seem within reach for the first time.

Related papers

Negative refraction in terbium at ultraviolet frequencies

Zachary Noel Buckholtz, Deniz D. Yavuz

One of the key challenges in the development of negative index metamaterials is creating a sufficiently strong magnetic response in the material. Rare-earth ions can contain a strong optical magnetic response even in the ultraviolet region of the spectrum, which can be enhanced using magneto-electric cross-coupling. Using energies, transition strengths, and linewidths from atomic structure software, along with realistic inhomogeneous broadenings and densities in a solid, we simulate a negative index scheme using a terbium crystal at a wavelength of 282 nm.

Optics Letters•Aug 10, 2020•4 citations

The electromagnetically induced negative refractive index in the Er3+:YAlO3crystal

Chunxu Liu, Jisen Zhang, Junye Liu +1 more

We carried out the negative refractive index in the solid medium Er3+:YAlO3 crystal with a Λ-type four-level scheme proposed for atomic vapour by Thommen and Mandel, and Kastel (Phys. Rev. Lett. 2006 96 053601 and 2007 98 069301) based on quantum interference and electromagnetically induced transparency (EIT). The results show that the frequency band with the negative index is much wider (~1 MHz) than reported previously. Usually, Im[n] is always positive, corresponding to absorption, and the figure of merit (FOM, the ratio of real to imaginary, namely |Re[n]/Im[n]|) is only on the order of unity. We achieve FOM = |Re[n]/Im[n]| = 4.6. The corresponding negative Im[n] is related to the stimulated emission of 4I13/2 → 4I15/2 of the rare earth ion Er3+ under external electromagnetic fields. It is concluded that the rare earth ion doped material with abundant energy levels and various electric and magnetic transitions is an outstanding and practical candidate for the electromagnetically induced negative refractive index material.

Journal of Physics B Atomic Molecular and Optical Physics•Apr 21, 2009•12 citations

Selective Induced Magnetic Dichroism and Birefringence in a Left-Handed Medium

Haris Waleed Abbasi, Yasir Saeed, Nadia Boutabba +1 more

Birefringence and dichroism in atomic systems are active areas of research. Circular dichroism is typically observed in chiral atoms, molecules (such as DNA), and optically asymmetric materials. These phenomena enable polarization-based selectivity and high-precision measurements with applications in optical systems, biomedical diagnostics, and advanced photonics.Meanwhile, negative refractive index materials offer exotic applications in optics and photonics, including super-resolution imaging, invisibility cloaking, and sub-wavelength imaging. Here, we identify a novel route to achieving birefringence and dichroism in a left-handed system for the first time.We investigate the optical activity of an atomic left-handed medium, analyzing the interaction of left- and right-circularly polarized light with different atomic states while incorporating local field corrections. Notably, our results demonstrate simultaneous left-handedness for both polarization states. Furthermore, we find that electric birefringence and dichroism are significantly enhanced with increasing control field strength, while magnetic birefringence and dichroism can be fully controlled via strong laser coupling.These findings have promising implications for spintronics, image transmission in metamaterials, and the development of optical switches and high-speed data transmission devices, opening new avenues in quantum optics and photonics.

•Jul 22, 2025•0 citations

Negative refractive index in doped semiconductors via electromagnetically induced mixed-parity transitions

Adil‐Gerai Kussow, Alkim Akyurtlu

The existing Quantum Optics- based models of negative refractive index in atomic-vapor medium (e.g. Ne, Na) require unrealistically strong magnetic response of atoms combined with high atomic density. In contrast to these gas-based models, our approach explores solid-state n-type semiconductor with well-defined hydrogen-like donor atomic states within the band gap. Based on methods of Quantum Optics, we have found that optically transparent indium oxide is negative refractive index material if doped with tin and zinc (In 2-x Sn x/2 Zn x/2 O 3 (zinc-doped ITO)). The desirable negative refractive index effect is due to coherent coupling an electric dipole transition with magnetic transition with proper detunings of the probe and support laser beams (A.-G. Kussow and A. Akyurtlu, Int. J. Mod. Physics (2010)). The calculations demonstrate the feasibility of the effect at ~ 10 THz with extremely high figure of merit FOM >> 10.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Aug 19, 2010•1 citation

Spectroscopic study of rare earth ions in antiferromagnets

Masaya Hiraishi

Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.

•May 14, 2025•0 citations

Quantum memory development and new slow light applications in rare-earth-ion-doped crystals

Qian Li

When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.

•Jan 1, 2018•0 citations
Abstract : In this project, our long-term goal is to demonstrate the first negative refraction in atomic systems. Although the concept of negative refraction remained an academic curiosity for a long time, it is now well-understood that negative refraction may have important and far-reaching practical implications. The key challenge in observing negative refraction in the optical region of the spectrum is the weakness of the magnetic response. Our central experimental result during this project has been the first observation of Rabi flopping of a magnetic dipole transition in the optical region of the spectrum. We have performed this experiment using the 7F0-5D1 transition of europium ions in a cryogenically cooled doped crystal. This is a major result; we have shown for the firs time that an electron can interact sufficiently strongly with the magnetic field of a light wave and coherently move between the levels. Another important result during this project was the proposal for a new type of materials that exhibit negative refraction. Because of these achievements, observing negative refraction and left-handed electromagnetic waves in atomic systems seem within reach for the first time.
One of the key challenges in the development of negative index metamaterials is creating a sufficiently strong magnetic response in the material. Rare-earth ions can contain a strong optical magnetic response even in the ultraviolet region of the spectrum, which can be enhanced using magneto-electric cross-coupling. Using energies, transition strengths, and linewidths from atomic structure software, along with realistic inhomogeneous broadenings and densities in a solid, we simulate a negative index scheme using a terbium crystal at a wavelength of 282 nm.
We carried out the negative refractive index in the solid medium Er3+:YAlO3 crystal with a Λ-type four-level scheme proposed for atomic vapour by Thommen and Mandel, and Kastel (Phys. Rev. Lett. 2006 96 053601 and 2007 98 069301) based on quantum interference and electromagnetically induced transparency (EIT). The results show that the frequency band with the negative index is much wider (~1 MHz) than reported previously. Usually, Im[n] is always positive, corresponding to absorption, and the figure of merit (FOM, the ratio of real to imaginary, namely |Re[n]/Im[n]|) is only on the order of unity. We achieve FOM = |Re[n]/Im[n]| = 4.6. The corresponding negative Im[n] is related to the stimulated emission of 4I13/2 → 4I15/2 of the rare earth ion Er3+ under external electromagnetic fields. It is concluded that the rare earth ion doped material with abundant energy levels and various electric and magnetic transitions is an outstanding and practical candidate for the electromagnetically induced negative refractive index material.
Birefringence and dichroism in atomic systems are active areas of research. Circular dichroism is typically observed in chiral atoms, molecules (such as DNA), and optically asymmetric materials. These phenomena enable polarization-based selectivity and high-precision measurements with applications in optical systems, biomedical diagnostics, and advanced photonics.Meanwhile, negative refractive index materials offer exotic applications in optics and photonics, including super-resolution imaging, invisibility cloaking, and sub-wavelength imaging. Here, we identify a novel route to achieving birefringence and dichroism in a left-handed system for the first time.We investigate the optical activity of an atomic left-handed medium, analyzing the interaction of left- and right-circularly polarized light with different atomic states while incorporating local field corrections. Notably, our results demonstrate simultaneous left-handedness for both polarization states. Furthermore, we find that electric birefringence and dichroism are significantly enhanced with increasing control field strength, while magnetic birefringence and dichroism can be fully controlled via strong laser coupling.These findings have promising implications for spintronics, image transmission in metamaterials, and the development of optical switches and high-speed data transmission devices, opening new avenues in quantum optics and photonics.
The existing Quantum Optics- based models of negative refractive index in atomic-vapor medium (e.g. Ne, Na) require unrealistically strong magnetic response of atoms combined with high atomic density. In contrast to these gas-based models, our approach explores solid-state n-type semiconductor with well-defined hydrogen-like donor atomic states within the band gap. Based on methods of Quantum Optics, we have found that optically transparent indium oxide is negative refractive index material if doped with tin and zinc (In 2-x Sn x/2 Zn x/2 O 3 (zinc-doped ITO)). The desirable negative refractive index effect is due to coherent coupling an electric dipole transition with magnetic transition with proper detunings of the probe and support laser beams (A.-G. Kussow and A. Akyurtlu, Int. J. Mod. Physics (2010)). The calculations demonstrate the feasibility of the effect at ~ 10 THz with extremely high figure of merit FOM >> 10.
Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.
When doped into solid state transparent crystals, rare-earth ions can have optically excited states with milliseconds coherence time and up to six hours coherence time for hyperfine levels after being cooled down to liquid helium temperature. This long coherence property makes them unique as solid state material and attractive for quantum information applications.The rare-earth ions have narrow homogeneous linewidths on the order of ~ kHz. When doped into a crystal, the lattice structure is slightly distorted due to the size mismatch between the dopant and the host ions, resulting in slight differences in the local crystal fields at the dopant sites. Therefore, the resonance frequencies of the rare-earth ions are shifted relatively, resulting in an inhomogeneously broadened absorption profile, typically on the order of a few GHz. This provides the possibility of addressing each group of ions individually and engineering the absorption profile for different purposes by optical pumping using a narrow linewidth laser, and makes rare-earth-ion-doped crystals suitable for ensemble based quantum memories.Quantum memories are vital components for developing longdistance quantum communication. Part of this thesis project focused on making quantum memories with high efficiency and long storage time, especially using materials with low optical depth. To achieve this goal, a low finesse, unsymmetrical cavity was employed and experiments were carried out at (or close to) the impedance matched condition. Atomic frequency comb (AFC) protocol proposed for such an inhomogeneously broadened system was used to store coherent light for a certain time. 56% overall efficiency was achieved, and the main limiting factor for reaching even higher efficiency was the inefficient coupling between incoming light and the cavity mode. Other possible loss mechanisms were analyzed as well.Long-time, on-demand, quantum memory experiments were conducted with the help of two efficient radio-frequency rephasing pulses. Storage time was extended from microseconds to milliseconds after compensating (most of) the residual earth magnetic field in the lab. The opportunities and challenges of combing the cavity assistant quantum memory and the long time, on demand quantum memory were analyzed and possible solutions were proposed. Another part of the thesis project involves slow light-based applications in rare-earth-ion-doped crystals. The strong slow light effect at the presence a spectral hole is due to the fact that the light interacts with the absorbing ions outside the spectral hole off-resonantly, and most of the light energy is stored inside the ions as a polarization. For example, with a group velocity of 300 km/s, 99.9% of the pulse energy is stored in the ions when the pulse propagates inside the crystal. The slower the light propagates, the more energy is stored inside the medium. Based on this, a frequency shifter that is capable of shifting the light frequency of ± 4 MHz was demonstrated, and frequency shift up to GHz was proposed. Group velocity control by a factor of 20 and pulse compression in time by a factor of 2 were also demonstrated. The frequency shift and group velocity of the light are solely controlled by the external electric field, which makes them ideal for weak light situation. The unique property of such a frequency shifter and group velocity controller is that they could be made to accept light from an arbitrary incoming angle and polarization, for example, scattered light.