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Quantum critical electro-optic and piezo-electric nonlinearities
Authors:
Christopher P. Anderson,
Giovanni Scuri,
Aaron Chan,
Sungjun Eun,
Alexander D. White,
Geun Ho Ahn,
Christine Jilly,
Amir Safavi-Naeini,
Kasper Van Gasse,
Lu Li,
Jelena Vučković
Abstract:
Electro-optics, the tuning of optical properties of materials with electric fields, is key to a multitude of quantum and classical photonics applications. However, a major obstacle preventing many emerging use cases is inefficient modulation in cryogenic environments, as traditional tuning mechanisms degrade at low temperatures. Guided by the connection between phase transitions and nonlinearity,…
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Electro-optics, the tuning of optical properties of materials with electric fields, is key to a multitude of quantum and classical photonics applications. However, a major obstacle preventing many emerging use cases is inefficient modulation in cryogenic environments, as traditional tuning mechanisms degrade at low temperatures. Guided by the connection between phase transitions and nonlinearity, we identify the quantum paraelectric perovskite SrTiO$_3$ (STO) as the strongest cryogenic electro-optic photonic material. As a result of the unique quantum paraelectric phase of STO, we demonstrate a dynamically tunable linear Pockels coefficient ($r_{33}$) exceeding 500 pm/V at $T=5$ K, and study its full temperature and bias dependence. We also measure an enhanced piezo-electric coefficient ($d_{33}$) above 90 pC/N. Both of these coefficients exceed all previously reported values for cryogenic materials, including lithium niobate ($r_{33}\approx24$ pm/V) and barium titanate ($r_{42}\approx170$ pm/V). Furthermore, by tuning STO towards \textit{quantum criticality} with oxygen isotope substitution we more than double the optical and piezo-electric nonlinearities, demonstrating a linear Pockels coefficient above 1100 pm/V. Our results probe the link between quantum phase transitions, dielectric susceptibility, and optical nonlinearities, unlocking opportunities in cryogenic optical and mechanical systems, and provide a framework for discovering new nonlinear materials.
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Submitted 25 February, 2025; v1 submitted 20 February, 2025;
originally announced February 2025.
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Microwave Spin Control of a Tin-Vacancy Qubit in Diamond
Authors:
Eric I. Rosenthal,
Christopher P. Anderson,
Hannah C. Kleidermacher,
Abigail J. Stein,
Hope Lee,
Jakob Grzesik,
Giovanni Scuri,
Alison E. Rugar,
Daniel Riedel,
Shahriar Aghaeimeibodi,
Geun Ho Ahn,
Kasper Van Gasse,
Jelena Vuckovic
Abstract:
The negatively charged tin-vacancy (SnV-) center in diamond is a promising solid-state qubit for applications in quantum networking due to its high quantum efficiency, strong zero phonon emission, and reduced sensitivity to electrical noise. The SnV- has a large spin-orbit coupling, which allows for long spin lifetimes at elevated temperatures, but unfortunately suppresses the magnetic dipole tran…
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The negatively charged tin-vacancy (SnV-) center in diamond is a promising solid-state qubit for applications in quantum networking due to its high quantum efficiency, strong zero phonon emission, and reduced sensitivity to electrical noise. The SnV- has a large spin-orbit coupling, which allows for long spin lifetimes at elevated temperatures, but unfortunately suppresses the magnetic dipole transitions desired for quantum control. Here, by use of a naturally strained center, we overcome this limitation and achieve high-fidelity microwave spin control. We demonstrate a pi-pulse fidelity of up to 99.51+/0.03%$ and a Hahn-echo coherence time of T2echo = 170.0+/-2.8 microseconds, both the highest yet reported for SnV- platform. This performance comes without compromise to optical stability, and is demonstrated at 1.7 Kelvin where ample cooling power is available to mitigate drive induced heating. These results pave the way for SnV- spins to be used as a building block for future quantum technologies.
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Submitted 30 August, 2023; v1 submitted 22 June, 2023;
originally announced June 2023.
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Suppressing Diffusion-Mediated Exciton Annihilation in 2D Semiconductors Using the Dielectric Environment
Authors:
Aaron J. Goodman,
Der-Hsien Lien,
Geun Ho Ahn,
Leo L. Spiegel,
Matin Amani,
Adam P. Willard,
Ali Javey,
William A. Tisdale
Abstract:
Atomically thin semiconductors such as monolayer MoS2 and WS2 exhibit nonlinear exciton-exciton annihilation at notably low excitation densities (below ~10 excitons/um2 in MoS2). Here, we show that the density threshold at which annihilation occurs can be tuned by changing the underlying substrate. When the supporting substrate is changed from SiO2 to Al2O3 or SrTiO3, the rate constant for second-…
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Atomically thin semiconductors such as monolayer MoS2 and WS2 exhibit nonlinear exciton-exciton annihilation at notably low excitation densities (below ~10 excitons/um2 in MoS2). Here, we show that the density threshold at which annihilation occurs can be tuned by changing the underlying substrate. When the supporting substrate is changed from SiO2 to Al2O3 or SrTiO3, the rate constant for second-order exciton-exciton annihilation, k_XX [cm2/s], is reduced by one or two orders of magnitude, respectively. Using transient photoluminescence microscopy, we measure the effective room-temperature exciton diffusion coefficient in chemical-treated MoS2 to be D = 0.06 +/- 0.01 cm2/s, corresponding to a diffusion length of LD = 350 nm for an exciton lifetime of τ = 20 ns, which is independent of the substrate. These results, together with numerical simulations, suggest that the effective exciton-exciton annihilation radius monotonically decreases with increasing refractive index of the underlying substrate. Exciton-exciton annihilation limits the overall efficiency of 2D semiconductor devices operating at high exciton densities; the ability to tune these interactions via the dielectric environment is an important step toward more efficient optoelectronic technologies featuring atomically thin materials.
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Submitted 2 November, 2018;
originally announced November 2018.
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Sr$_3$Ir$_2$O$_7$F$_2$: Topochemical conversion of a relativistic Mott state into a spin-orbit driven band insulator
Authors:
Christi Peterson,
Michael W. Swift,
Zach Porter,
Raphaele J. Clement,
Guang Wu,
G. H. Ahn,
S. J. Moon,
B. C. Chakoumakos,
Jacob P. C. Ruff,
Huibo Cao,
Chris Van de Walle,
Stephen D. Wilson
Abstract:
The topochemical transformation of single crystals of Sr$_3$Ir$_2$O$_7$ into Sr$_3$Ir$_2$O$_7$F$_2$ is reported via fluorine insertion. Characterization of the newly formed Sr$_3$Ir$_2$O$_7$F$_2$ phase shows a nearly complete oxidation of Ir$^{4+}$ cations into Ir$^{5+}$ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled J$_{eff}=1/2$ band into a nonmagnetic…
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The topochemical transformation of single crystals of Sr$_3$Ir$_2$O$_7$ into Sr$_3$Ir$_2$O$_7$F$_2$ is reported via fluorine insertion. Characterization of the newly formed Sr$_3$Ir$_2$O$_7$F$_2$ phase shows a nearly complete oxidation of Ir$^{4+}$ cations into Ir$^{5+}$ that in turn drives the system from an antiferromagnetic Mott insulator with a half-filled J$_{eff}=1/2$ band into a nonmagnetic $J=0$ band insulator. First principles calculations reveal a remarkably flat insertion energy that locally drives the fluorination process to completion. Band structure calculations support the formation of a band insulator whose charge gap relies on the strong spin-orbit coupling inherent to the Ir metal ions of this compound.
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Submitted 6 October, 2018;
originally announced October 2018.