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Advanced Photonics Research

Active Modulation of Er3+ Emission Lifetime by VO2 Phase‐Change Thin Films

Boris Kalinic, Tiziana Cesca, Alessandro Lovo, Carlo Scian, Roberto Macaluso, Fabio Antonio Bovino, Roberto Li Voti, Concita Sibilia, Giovanni Mattei

Published Nov 14, 2023• 4 citations
Publisher

Abstract

The active modulation of optical response of quantum emitters at the nanoscale is of paramount importance to realize tunable light sources for nanophotonic devices. Herein, a thin film of phase‐change material (VO2) is coupled to a 20 nm‐thick silica layer embedding Er3+ ions, and it is demonstrated how the active tuning of the local density of optical states near the erbium emitters provided by the thermally induced semiconductor‐to‐metal transition of VO2 can be used to dynamically control the Er3+ emission lifetime at telecom wavelength (1.54 μm). A decay rate contrast of a factor 2 is obtained between high temperature (90 °C), when VO2 is metallic, and room temperature, when VO2 is semiconductor, in agreement with calculations performed with the classical dipole oscillator analytical model. A hysteretic behavior is observed by measuring the Er3+ lifetime as a function of the temperature, whose parameters are consistent with those of grazing incidence X‐ray diffraction and optical transmittance measurements. The fractions of Er3+ ions that couple with VO2 in each phase at the different temperatures are determined by the analysis of the temporal decays. The results make the investigated system an optimal candidate for the development of tunable photon sources at telecom wavelength.

DOI
10.1002/adpr.202300242

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The active modulation of optical response of quantum emitters at the nanoscale is of paramount importance to realize tunable light sources for nanophotonic devices. Herein, a thin film of phase‐change material (VO2) is coupled to a 20 nm‐thick silica layer embedding Er3+ ions, and it is demonstrated how the active tuning of the local density of optical states near the erbium emitters provided by the thermally induced semiconductor‐to‐metal transition of VO2 can be used to dynamically control the Er3+ emission lifetime at telecom wavelength (1.54 μm). A decay rate contrast of a factor 2 is obtained between high temperature (90 °C), when VO2 is metallic, and room temperature, when VO2 is semiconductor, in agreement with calculations performed with the classical dipole oscillator analytical model. A hysteretic behavior is observed by measuring the Er3+ lifetime as a function of the temperature, whose parameters are consistent with those of grazing incidence X‐ray diffraction and optical transmittance measurements. The fractions of Er3+ ions that couple with VO2 in each phase at the different temperatures are determined by the analysis of the temporal decays. The results make the investigated system an optimal candidate for the development of tunable photon sources at telecom wavelength.
We investigate the spontaneous emission of a two-level quantum emitter in the vicinity of a vanadium dioxide (VO2) thin film. By taking advantage of effective medium techniques to describe the dielectric constant of the VO2, we demonstrate that, in the near-field regime, the spontaneous emission rate of both electric and magnetic dipole emitters can be maximized at the insulator-to-metal phase transition temperature of the film. We find that VO2’s thermal hysteresis curve produces clear fingerprints in the emitter’s decay process, offering a new degree of freedom to dynamically control light emission at the nanoscale. We also find that the spontaneous emission rate is a non-monotonic function of the emitter transition wavelength, presenting a pronounced peak at infrared frequencies. Altogether, our results reveal that VO2 phase transition is a promising mechanism to achieve on-demand tuning of an emitter’s lifetime.
Modulation is a cornerstone of optical communication, and as such, governs the overall speed of data transmission. Currently, the two main strategies for modulating light are direct modulation of the excited emitter population (for example, using semiconductor lasers) and external optical modulation (for example, using Mach-Zehnder interferometers or ring resonators). However, recent advances in nanophotonics offer an alternative approach to control spontaneous emission through modifications to the local density of optical states. Here, by leveraging the phase-change of a vanadium dioxide nanolayer, we demonstrate broadband all-optical direct modulation of 1.5 μm emission from trivalent erbium ions more than three orders of magnitude faster than their excited state lifetime. This proof-of-concept demonstration shows how integration with phase-change materials can transform widespread phosphorescent materials into high-speed optical sources that can be integrated in monolithic nanoscale devices for both free-space and on-chip communication.
With their shielded 4f orbitals, rare-earth ions (REIs) offer optical and electron spin transitions with good coherence properties even when embedded in a host crystal matrix, highlighting their utility as promising quantum emitters and memories for quantum information processing. Among REIs, trivalent erbium (Er3+) uniquely has an optical transition in the telecom C-band, ideal for transmission over optical fibers, making it well suited for applications in quantum communication. The deployment of Er3+ emitters into a thin film TiO2 platform has been a promising step toward scalable integration; however, like many solid-state systems, the deterministic spatial placement of quantum emitters remains an open challenge. We investigate laser annealing as a means to locally tune the optical resonance of Er3+ emitters in TiO2 thin films on Si. Using both nanoscale x-ray diffraction measurements and cryogenic photoluminescence spectroscopy, we show that tightly focused below-gap laser annealing can induce anatase to rutile phase transitions in a nearly diffraction-limited area of the films and improve local crystallinity through grain growth. As a percentage of Er:TiO2 is converted to rutile, the Er3+ optical transition blueshifts by 13 nm. We explore the effects of changing laser annealing time and show that the amount of optically active Er:rutile increases linearly with laser power. We additionally demonstrate local phase conversion on microfabricated Si structures, which holds significance for quantum photonics.
Single quantum emitters embedded in solid-state hosts are an ideal platform for realizing quantum information processors and quantum network nodes. Among the currently investigated candidates, Er^{3+} ions are particularly appealing due to their 1.5 μm optical transition in the telecom band as well as their long spin coherence times. However, the long lifetimes of the excited state-generally in excess of 1 ms-along with the inhomogeneous broadening of the optical transition result in significant challenges. Photon emission rates are prohibitively small, and different emitters generally create photons with distinct spectra, thereby preventing multiphoton interference-a requirement for building large-scale, multinode quantum networks. Here we solve this challenge by demonstrating for the first time linear Stark tuning of the emission frequency of a single Er^{3+} ion. Our ions are embedded in a lithium niobate crystal and couple evanescently to a silicon nanophotonic crystal cavity that provides a strong increase of the measured decay rate. By applying an electric field along the crystal c axis, we achieve a Stark tuning greater than the ion's linewidth without changing the single-photon emission statistics of the ion. These results are a key step towards rare earth ion-based quantum networks.
We theoretically investigate the bistable spontaneous emission behavior of a single emitter in the vicinity of a hybrid V O 2 –Au nanoshell. The hybrid nanoshell is illuminated by a continuous wave pump laser. The incident beam generates heat through light absorption and causes the V O 2 to undergo a phase change from semiconductor to metallic mode. Our calculation shows that for certain values, over a range of incident laser intensity [ 0.25 ( G W / m 2 ) < I < 0.84 ( G W / m 2 )], at the resonance wavelength of the V O 2 (semiconductor)–Au nanoshell ( λ = 630 n m ), there is a reasonable bistable contrast for the two spontaneous emission rate values: the radiative and nonradiative decay rates. Our results provide important general guidelines for enabling platforms for optical switching sources and tunable sensors.
Atomic layer deposited (ALD) Y 2 O 3 thin films have been thoroughly investigated for optical or electronic applications. The coherent spectroscopy of lanthanide ions doped into this material has also recently attracted increasing interest in the field of quantum technologies for which they are considered promising candidates in quantum memories or as spin–photon interfaces. However, these most demanding applications require a deep control over the local positioning of the ions and their close environment in the crystalline matrix. This study focuses on the structural as well as optical properties of Eu 3+ and Er 3+ dopants in Y 2 O 3 using photoluminescence (PL), luminescence decay times, and inhomogeneous line width (Γ inh ) measurements within this particular context. While as-grown ALD films do not provide an ideal host for the emitters, we demonstrate that by optimizing the deposition conditions and using appropriate annealing post treatments narrow inhomogeneous lines can be obtained for the 7 F 0 ↔ 5 D 0 transition of Eu 3+ even for nanoscale films. Furthermore, about 1.5 ms lifetime has been measured for the infrared telecom transition of Er in ultrathin films (<10 nm), which is an order of magnitude higher than in nanoparticles of the same size. These results validate optimized rare-earth-doped ALD Y 2 O 3 films as a suitable platform for photonics applications where few-nanometer-thick films with well-localized emitters are mandatory. This approach provides the first building blocks toward the development of more complex devices for quantum sensing or hybrid structures coupled with other systems such as two-dimensional materials.