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arXiv:2204.11255 · Physical Review A

Influence of phonon harmonicity on spectrally pure resonant Stokes fields

Georgios Stoikos, Eduardo Granados

Published Aug 3, 2022• 3 citations
arXivHTMLPDF

Abstract

Due to their highly coherent emission, tunability, and compactness, integrated single-frequency diamond Raman lasers are interesting tools for applications in integrated quantum technology, high-resolution spectroscopy, or coherent optical communications. While the fundamental emission linewidth of these lasers can be Fourier limited, their thermo-optic characteristics lead to drifts in their carrier frequency, posing important challenges for applications requiring ultrastable emission. We propose here a method for measuring accurately the temperature-dependent index of refraction of diamond by employing standing Stokes waves produced in a monolithic Fabry-P\'erot diamond Raman resonator. Our approach takes into account the influence of temperature on the first-order phonon line and the average lattice phonon frequency under intense stimulated Raman scattering conditions. We further utilize this model to calculate the value of the average phonon frequency and then the temperature-dependent thermo-optic coefficient. The theory is accompanied by the demonstration of tunable Fourier-limited Stokes nanosecond pulses with a stabilized center frequency deviation of less than $4$ MHz.

DOI
10.1103/physreva.106.023504

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Due to their highly coherent emission, tunability, and compactness, integrated single-frequency diamond Raman lasers are interesting tools for applications in integrated quantum technology, high-resolution spectroscopy, or coherent optical communications. While the fundamental emission linewidth of these lasers can be Fourier limited, their thermo-optic characteristics lead to drifts in their carrier frequency, posing important challenges for applications requiring ultrastable emission. We propose here a method for measuring accurately the temperature-dependent index of refraction of diamond by employing standing Stokes waves produced in a monolithic Fabry-P'erot diamond Raman resonator. Our approach takes into account the influence of temperature on the first-order phonon line and the average lattice phonon frequency under intense stimulated Raman scattering conditions. We further utilize this model to calculate the value of the average phonon frequency and then the temperature-dependent thermo-optic coefficient. The theory is accompanied by the demonstration of tunable Fourier-limited Stokes nanosecond pulses with a stabilized center frequency deviation of less than 444 MHz.
Fourier-limited nanosecond pulses featuring narrow spectral bandwidths are required for applications in spectroscopy, sensing, and quantum optics. Here, we demonstrate a direct and simple route for the generation of single-frequency light relying on phonon-resonant Raman interactions within a monolithic diamond resonator. The technique enables the production of nearly Fourier-limited nanosecond optical pulses (15 ns), with an overall spectral bandwidth of down to 180 MHz, which is nearly two orders of magnitude narrower than the pump laser linewidth used (12 GHz). The power conversion efficiency was 47%, yielding a power spectral brightness enhancement of > 50 × compared to the pump. Our results pave the way to the integration of pulsed widely tunable, power scalable, narrow linewidth light sources into integrated photonic platforms. Furthermore, the device does not need elaborate mechanical feedback loops for cavity length or frequency stabilization, or any additional optical components.
Abstract Tunable single‐frequency lasers are the most prominent tool for high‐resolution spectroscopy, allowing for the study and exploitation of the electronic structure of atoms. A significant milestone relies on the demonstration of integrated laser technology for performing such a task. The device presented here is composed of a compact Fabry–Perot monolithic resonator capable of producing tunable and Fourier‐limited nanosecond pulses with a MHz‐class frequency stability without active cavity stabilization elements. It also has the remarkable capability of exploiting the Raman effect to funnel efficiently the broad spectrum of an input laser to a spectrally‐bright Stokes pulse at hard‐to‐access wavelength ranges. The targeted atom for the demonstrations is 152Sm, released as an atomic vapor in a hot cavity environment. Here, the Stokes field is tuned to a wavelength of 433.9 nm, while a crossed‐beams spectroscopy setup is used to minimize the Doppler broadened spectral features of the atoms. With this work, the suitability of integrated diamond Raman lasers as a high‐resolution in‐source spectroscopy tool is demonstrated, enabling many applications in atomic and nuclear physics. The integrated form‐factor and inherent simplicity makes such a laser an interesting prospect for quantum‐technology based sensing systems and related applications.
Tunable single-frequency lasers are essential for high-resolution spectroscopy and quantum technologies, yet achieving narrow-linewidth performance in compact, scalable systems across the UV-visible spectrum remains a key challenge. Recent work has revealed that Raman scattering in diamond can act as a natural spectral squeezer, where phonon dynamics help suppress frequency noise and concentrates optical power into a single, narrow spectral mode. Experiments at CERN and elsewhere have demonstrated linewidth compression by orders of magnitude, frequency-noise suppression exceeding 10³-10⁴, and pathways toward Schawlow–Townes-limited performance in CW regimes. These results establish Raman phonon damping as a universal mechanism for generating ultra-coherent, widely tunable lasers, opening new opportunities in quantum metrology, optical clocks, and high-resolution spectroscopy.
An experimental study of normal and stimulated Raman emission in diamond is presented, including measurements of linewidth, intensity, and angular distribution of radiation having a frequency shift of 1332.0 ${\mathrm{cm}}^{\ensuremath{-}1}$. The diamond crystal formed a Raman resonator; excitation was by a giant-pulse ruby laser. The dependence of normal Stokes emission on laser intensity and the threshold for oscillation were investigated. A value for the Raman gain ($g=6.9\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}3}$ ${\mathrm{cm}}^{\ensuremath{-}1}$ per MW/cm2{\mathrm{cm}}^{2}cm2) was calculated from the measured linewidth ($\ensuremath{\Delta}\ensuremath{\nu}=2.04$ ${\mathrm{cm}}^{\ensuremath{-}1}$) and cross section for scattering, and found to be in good agreement with a value determined from the threshold for oscillation. The angular distributions of anti-Stokes and Stokes emission and absorption for parallel and convergent laser light are also in good agreement with theory: The emission cone angles are strongly dependent on the angle of convergence of the incident light, and it is established that the preferred directions for emission are those making use of the most intense first-order Stokes radiation which is peaked in the forward direction within the Raman resonator.
Tunable single-frequency lasers are essential for high-resolution spectroscopy and quantum technologies, yet achieving narrow-linewidth performance in compact, scalable systems across the UV-visible spectrum remains a key challenge. Recent work has revealed that Raman scattering in diamond can act as a natural spectral squeezer, where phonon dynamics help suppress frequency noise and concentrates optical power into a single, narrow spectral mode. Experiments at CERN and elsewhere have demonstrated linewidth compression by orders of magnitude, frequency-noise suppression exceeding 10³-10⁴, and pathways toward Schawlow–Townes-limited performance in CW regimes. These results establish Raman phonon damping as a universal mechanism for generating ultra-coherent, widely tunable lasers, opening new opportunities in quantum metrology, optical clocks, and high-resolution spectroscopy.
Fourier-limited and tunable nanosecond pulses are essential for applications that rely on high-intensity interactions between light and atoms. These applications require precise and wide tunability across a large range of wavelengths (expanding from the UV to the near-IR). The vast interest in producing and integrating pulsed tunable narrow linewidth light is further fuelled by applications in quantum technology. The main challenge here is in the production of many (hundreds to thousands) individually tunable, narrow-band pulses simultaneously. Photonic integrated circuits (PICs) are expected to provide the scalability and simplicity required for these quantum technology-based sensing systems and applications, but there are still many obstacles to overcome. Among these are improvements in active materials, such as direct gain and laser output in the green-yellow spectral range.