It was recently shown that the optical excitation of rare-earth ions produces a local change of the host matrix shape, attributed to a change of the rare-earth ion's electronic orbital geometry. In this work we investigate the consequences of this piezo-orbital backaction and show from a macroscopic model how it yields a disregarded ion-ion interaction mediated by mechanical strain. This interaction scales as1/r3, similarly to the other archetypal ion-ion interactions, namely electric and magnetic dipole-dipole interactions. We quantitatively assess and compare the magnitude of these three interactions from the angle of the instantaneous spectral diffusion mechanism, and re-examine the scientific literature in a range of rare-earth doped systems in the light of this generally underestimated contribution.
It was recently shown that the optical excitation of rare-earth ions produces a local change of the host matrix shape, attributed to a change of the rare-earth ion's electronic orbital geometry. In this work we investigate the consequences of this piezo-orbital backaction and show from a macroscopic model how it yields a disregarded ion-ion interaction mediated by mechanical strain. This interaction scales as1/r3, similarly to the other archetypal ion-ion interactions, namely electric and magnetic dipole-dipole interactions. We quantitatively assess and compare the magnitude of these three interactions from the angle of the instantaneous spectral diffusion mechanism, and re-examine the scientific literature in a range of rare-earth doped systems in the light of this generally underestimated contribution.
We consider a hybrid optomechanical system composed of an ensemble of identical rare earth ions embedded in a bulk crystal, and coupled to internal strain. We evidence the generation of a mechanical response within this hybrid system under resonant atomic excitation, which we find to be driven by two fundamental contributions: First, a conservative backaction force coined as piezo-orbital, coming along with the promotion of the atoms in their excited state. This effect is expected in all impurity-doped crystals and reflects the interaction between the ions' orbital shape and the crystal field of their host matrix. The second contribution corresponds to a dissipa-tive, photothermal backaction force associated with the non-radiative relaxation dynamics of the rare-earth ions. The two components are identified by means of a spatio-temporal mapping of the mechanically non-resonant op-tomechanical response in the bulk crystal. The optically resonant nature of the two effects and their fundamental connection to the internal atomic state dynamics are quantitatively confirmed.
Hybrid optomechanics can bridge the quantum and classical domains, to generally extend quantum principles to macroscopic scale. A milestone here would be observing the fundamental backaction force that occurs when a hybrid mechanical system is optically probed, which can be dominated by classical thermal effects. Using a large ensemble of rare-earth ions in a crystal plus time-resolved tomography, researchers see this backaction as a tiny distortion of the crystal's surface around a laser beam's spot, and unambiguously distinguish the photothermal contribution from that of the backaction. Thus rare-earth ions in crystals are confirmed as a promising platform for hybrid optomechanics.
Material strain has recently received growing attention as a complementary resource to control the energy levels of quantum emitters embedded inside a solid-state environment.Some rare-earth ion dopants provide an optical transition which simultaneously has a narrow linewidth and is highly sensitive to strain.In such systems, the technique of spectral hole burning, in which a transparent window is burned within the large inhomogeneous profile, allows one to benefit from the narrow features, which are also sensitive to strain, while working with large ensembles of ions.However, working with ensembles may give rise to inhomogeneous responses among different ions.We investigate experimentally how the shape of a narrow spectral hole is modified due to external mechanical strain, in particular, the hole broadening as a function of the geometry of the crystal sites and the crystalline axis along which the stress is applied.Studying these effects is essential in order to optimize the existing applications of rare-earth-doped crystals in fields which already profit from the more-well-established coherence properties of these dopants, such as frequency metrology and quantum information processing, or even suggest alternative applications of these materials, for example, as robust devices for force-sensing or highly sensitive accelerometers.
Material strain has recently received growing attention as a complementary resource to control the energy levels of quantum emitters embedded inside a solid-state environment. Some rare-earth ion dopants provide an optical transition which simultaneously has a narrow linewidth and is highly sensitive to strain. In such systems, the technique of spectral hole burning, in which a transparent window is burned within the large inhomogeneous profile, allows one to benefit from the narrow features, which are also sensitive to strain, while working with large ensembles of ions. However, working with ensembles may give rise to inhomogeneous responses among different ions. We investigate experimentally how the shape of a narrow spectral hole is modified due to external mechanical strain, in particular, the hole broadening as a function of the geometry of the crystal sites and the crystalline axis along which the stress is applied. Studying these effects is essential in order to optimize the existing applications of rare-earth-doped crystals in fields which already profit from the more-well-established coherence properties of these dopants, such as frequency metrology and quantum information processing, or even suggest alternative applications of these materials, for example, as robust devices for force-sensing or highly sensitive accelerometers.Received 24 December 2019Accepted 20 February 2020DOI:https://doi.org/10.1103/PhysRevResearch.2.013306Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasDopantsFine & hyperfine structureOptics & lasersStressPhysical SystemsRare-earth doped crystalsGeneral Physics
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,
By spectrally hole burning an inhomogeneously broadened ensemble of ions while applying a controlled perturbation, one can obtain spectral holes that are functionalized for maximum sensitivity to different perturbations. We propose to use such hole-burned structures for the dispersive optical interaction with rare-earth-ion dopants whose frequencies are sensitive to crystal strain due to the bending motion of a crystal cantilever. A quantitative analysis shows that good optical sensitivity to the bending motion is obtained if a magnetic-field gradient is applied across the crystal during hole burning and that the resulting optomechanical coupling strength is sufficient for observing quantum features such as zero-point vibrations.