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Nonlinear optical spectrum of diamond at femtosecond regime

MetadataDetails
Publication Date2017-10-24
JournalScientific Reports
AuthorsJuliana M. P. Almeida, Charlie Oncebay, Jonathas P. Siqueira, Sérgio Ricardo Muniz, Leonardo De Boni
InstitutionsUniversidade de SĂŁo Paulo
Citations49
AnalysisFull AI Review Included

Technical Documentation and Analysis: Nonlinear Diamond Photonics

Section titled “Technical Documentation and Analysis: Nonlinear Diamond Photonics”

This document analyzes the research on the third-order nonlinear optical properties of CVD diamond at femtosecond regimes, crucial for advancing integrated quantum and nonlinear optics platforms. 6CCVD provides the specialized material specifications required to replicate and scale this highly technical research.

  • Core Achievement: First comprehensive measurement of the third-order nonlinear spectrum of diamond, spanning 0.83-4.77 eV (1500-260 nm), determining the two-photon absorption coefficient ($\beta$) and nonlinear refractive index (n2).
  • Material Focus: Experiments relied on high-purity, type-IIa Single Crystal Diamond (SCD) grown by Chemical Vapor Deposition (CVD), specifically requiring ultra-low nitrogen (N < 5 ppb) and nitrogen vacancy (NV < 0.03 ppb) concentrations.
  • Key Findings ($\beta$): The two-photon absorption coefficient ($\beta$) ranged from 0.07 to 0.23 cm/GW, increasing as photon energy approached the 5.54 eV bandgap.
  • Key Findings (n2): The nonlinear refractive index (n2) varied from zero to $1.7 \times 10^{-19}$ m2/W, exhibiting positive values characteristic of ultrafast electronic nonlinearity.
  • Ultrafast Response Confirmed: Optical Kerr Gate (OKG) measurements confirmed an instantaneous, pure electronic nonlinear response time of 130 fs, matching the laser pulse duration.
  • Dominant Mechanism: Results demonstrate that phonon-assisted two-photon absorption is the dominant mechanism determining the third-order nonlinear susceptibility dispersion in indirect bandgap diamond.
  • 6CCVD Value: 6CCVD specializes in delivering the ultra-high purity SCD plates (Ra < 1 nm) and custom dimensions necessary for high-fidelity replication and future device integration based on these fundamental findings.

The following table summarizes the critical material parameters and measured performance metrics extracted from the study, focusing on requirements for integrated photonics.

ParameterValueUnitContext
Material TypeType-IIa Single Crystal Diamond (SCD)N/ACVD grown, highest purity optical grade
Sample Dimensions$2 \times 2 \times 0.53$mmÂłSingle crystal plate used for Z-scan
Band Gap Energy ($E_{g}$)5.54eVFundamental material property of diamond
Nitrogen Impurities< 5 (usually < 1)ppbUltra-high purity requirement for optical studies
Nitrogen Vacancies (NV)< 0.03ppbLow NV concentration confirmed by fluorescence
Polishing Roughness (Ra)< 5nmOn the {100} face
Z-scan Wavelength Range1500 to 260nmCorresponds to 0.83-4.77 eV
Two-Photon Absorption ($\beta$) Range0.07 to 0.23cm/GWMeasured range as $E$ approached $E_{g}$
Nonlinear Refractive Index ($n_{2}$) Range0 to $1.7 \times 10^{-19}$m2/WMaximum observed positive value
Nonlinear Response Time130fsConfirmed by Optical Kerr Gate (OKG) measurements
Excitation RegimeFemtosecond (120-150 fs)Pulse DurationRequired to confirm pure electronic nonlinearity

The study successfully characterized the third-order nonlinear optical response of diamond using established ultrafast techniques tailored for wide spectral range analysis:

  1. Material Selection: A commercially sourced, high-purity, Type IIa SCD plate was used. The material purity (N < 5 ppb) and low defect concentration were confirmed via confocal fluorescence imaging.
  2. Laser System: Femtosecond pulses (150 fs, 775 nm, 1 kHz repetition rate) from a Ti:sapphire chirped pulse amplifier system were used to pump an Optical Parametric Amplifier (OPA). The OPA provided tunable 120 fs pulses from 2000 nm down to 260 nm.
  3. Z-Scan Technique: Open-aperture Z-scan measurements were conducted to determine the nonlinear absorption coefficient ($\beta$). Closed-aperture Z-scan measurements were used simultaneously (via a dual-arm setup) to determine the nonlinear refractive index ($n_{2}$).
  4. Nonlinear Absorption Detection: Two-Photon Absorption (2PA) was specifically detected only for photon energies $\ge$ 3.18 eV (390 nm), confirming its role as the dominant nonlinear absorption mechanism in this range.
  5. Optical Kerr Gate (OKG) Measurement: The time response of the nonlinearity was investigated using an OKG setup, employing strong pump and weak probe beams polarized at 45° relative angle. This confirmed the ultrafast (130 fs) pure electronic nature of the induced birefringence.

6CCVD is uniquely positioned to supply the advanced MPCVD diamond substrates required to not only reproduce this fundamental research but also scale these findings into next-generation integrated photonic and quantum devices.

To replicate and extend this research on third-order nonlinearities, researchers require ultra-high purity Single Crystal Diamond (SCD) with superior optical performance and structural integrity.

  • Material Recommendation: Optical Grade Single Crystal Diamond (SCD).
    • This material matches the high-purity, Type-IIa specifications used in the paper (low N, low NV centers), essential for minimizing competing absorption mechanisms (e.g., cascade absorption by free carriers) that can distort true 2PA measurements.
    • Bandgap Utilization: Given the measurements utilize photon energies near 4.77 eV (UV region), 6CCVD’s low-loss SCD ensures maximum transmission and minimized linear background absorption, vital for high signal-to-noise ratio in Z-scan setups.

The experimental findings lay the groundwork for integrated nonlinear optical platforms. 6CCVD offers extensive customization services required for device prototyping and fabrication.

Requirement from Paper/Future Integration6CCVD Custom CapabilityBenefit for Researchers
Purity & QualitySCD with Ra < 1 nm polishingExceeds the paper’s Ra < 5 nm specification, providing atomically smooth surfaces crucial for minimizing scattering loss in integrated waveguides and resonators.
Custom DimensionsPlates/wafers up to 125 mm (PCD); Substrates up to 10 mm thickEnables scalability from benchtop experiments (like the $2 \times 2 \times 0.53$ mmÂł sample) to inch-size integrated photonics wafers.
Precise Thickness ControlSCD thickness from 0.1 ”m up to 500 ”mCritical for optimizing light confinement and maximizing nonlinear interaction length in integrated diamond micro-resonators and waveguides.
Metalization for IntegrationIn-house capability for Au, Pt, Pd, Ti, W, CuSupports immediate post-growth processing for creating electrodes, ohmic contacts, or mirror layers necessary for high-speed quantum and nonlinear circuits (e.g., optical modulators or frequency conversion devices).

This research validates diamond’s ultrafast electronic response (130 fs) and high nonlinear coefficients, making it a powerful alternative to silicon for high-speed photonics.

  • 6CCVD’s in-house PhD team provides specialized engineering consultation to assist clients transitioning from fundamental material characterization to integrated device fabrication. We offer expert support in material selection, orientation, and doping levels (e.g., selecting optimal SCD crystal orientation, such as the {100} face used in this study, and managing Boron Doping Density for electro-optic modulation projects).
  • We specifically assist with material selection for similar Ultrafast Nonlinear Optics and Integrated Quantum Optics projects, ensuring material parameters (purity, defect control) are optimized for the intended application bandwidth and power regime.

For custom specifications or material consultation, visit 6ccvd.com or contact our engineering team directly. We offer global shipping via DDU (default) or DDP (upon request).