Cooperative dynamic polaronic picture of diamond color centers

Nat. Commun. 15, 7174 (2024) · DOI: 10.1038/s41467-024-51366-x

License: CC BY 4.0.

Abstract

Polarons can control carrier mobility and can also be used in the design of quantum devices. Although much effort has been directed into investigating the nature of polarons, observation of defect-related polarons is challenging due to electron-defect scattering. Here we explore the polaronic behavior of nitrogen-vacancy (NV) centers in a diamond crystal using an ultrafast pump-probe technique. A 10-fs optical pulse acts as a source of high electric field exceeding the dielectric breakdown threshold, in turn exerting a force on the NV charge distribution and polar optical phonons. The electronic and phononic responses are enhanced by an order of magnitude for a low density of NV centers, which we attribute to a combination of cooperative polaronic effects and scattering by defects. First-principles calculations support the presence of dipolar Fröhlich interaction via non-zero Born effective charges. Our findings provide insights into the physics of color centers in diamonds.

Figures

7 panels with data across 2 figures. Each panel page shows the plot, its columns and its files; each data.csv begins with a header naming the paper, the panel, the source, the license and the provenance route.

Fig. 1

• panel (a): Time-domain electro-optic signal $\Delta R_{\mathrm{EO}}/R_0$ ($\times 10^{-3}$) against time delay (fs) for the NI diamond and the NV diamond ($1\times10^{12}$ N$^{+}$ cm$^{-2}$), shaded to zero as printed. Times are 21 fs later than in the Source Data, as printed. The axis shows the first 900 fs of 8.6 ps. The structure and pump-probe inset is not drawn. data.csv
• panel (b): Fourier-transformed spectra of the signals in (a): FT intensity ($\times 10^{-3}$) against frequency (THz) for the NV diamond (red circles) and the NI diamond (blue squares, multiplied by 100 as printed), with the fits by the Debye model (dashed) and the Lorentz model (solid). The axis shows 0 to 50 THz; the spectra run to 456 THz. data.csv

Fig. 2

• panel (a): Time-domain electro-optic signals $\Delta R_{\mathrm{EO}}/R_0$ ($\times 10^{-6}$) against time delay (ps) for the NI diamond and the NV diamonds at four doses, each with its damped harmonic oscillator fit (black). As printed, the traces are offset vertically: NI by +49.26, $1\times10^{12}$ by $-50$, $5\times10^{12}$ by $-100$ and $2\times10^{13}$ by $-150$. data.csv
• panel (b): Dose dependence of the initial amplitude $A$ ($\times 10^{-6}$) against dose ($\times 10^{12}$ cm$^{-2}$): NI diamond (blue square) and NV diamonds (pink circles) with error bars, and dashed fits $\propto [\mathrm{N}^{+}]$ below $1\times10^{12}$ and $\propto 1/[\mathrm{N}^{+}]$ from $1\times10^{12}$ N$^{+}$ cm$^{-2}$. The $2\times10^{11}$ point is as printed; the Source Data value is higher. data.csv
• panel (c): Dose dependence of the decay time $\tau_{\mathrm{LO}}$ (ps) against dose ($\times 10^{12}$ cm$^{-2}$): NI diamond (blue square) and NV diamonds (pink circles); error bars are standard deviations. The grey line is drawn as printed. data.csv
• panel (d): Dose dependence of the LO phonon frequency $\Omega_{\mathrm{LO}}$ (THz) against dose ($\times 10^{12}$ cm$^{-2}$): NI diamond (blue square) and NV diamonds (pink circles); error bars are the frequency resolution. The grey line is drawn as printed. data.csv
• panel (e): Dose dependence of the initial phase $\psi$ (deg) against dose ($\times 10^{12}$ cm$^{-2}$): NI diamond (blue square) and NV diamonds (pink circles) with error bars, the dashed fits $\propto [\mathrm{N}^{+}]$ below $1\times10^{12}$ and $\propto 1/[\mathrm{N}^{+}]$ from $1\times10^{12}$ N$^{+}$ cm$^{-2}$, and dashed reference lines near $0^{\circ}$ and $90^{\circ}$. data.csv

Fig. 3

Illustrative figure, no extractable data. Shown in the paper PDF.

Fig. 4

Illustrative figure, no extractable data. Shown in the paper PDF.

Cite

Takuto Ichikawa, Junjie Guo, Paul Fons, Dwi Prananto, Toshu An, Muneaki Hase. Cooperative dynamic polaronic picture of diamond color centers. Nat. Commun. 15, 7174 (2024). https://doi.org/10.1038/s41467-024-51366-x

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