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Journal of Luminescence

Frequency-dependent dephasing of N-V centers in diamond

Eric van Oort, Max Glasbeek

Published Jul 1, 1992• 4 citations
Publisher
DOI
10.1016/0022-2313(92)90113-n

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Ultrafast photon echo spectroscopy of luminescent centers: NV:diamond and thulium(3+) yttrium aluminum oxygen(3).

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In the present work, ultrafast photon echo spectroscopy has been applied to investigate dephasing dynamics and excited state electronic structure of impurity N-V centers in diamond and Tm$\sp{3+}$-Tm$\sp{3+}$ centers. In the N-V center, quantum beat measurements revealed modulation frequencies of 0.63 $\pm$ 0.02 GHz, 1.650 $\pm$ 0.003 GHz, and 2.298 $\pm$ 0.006 GHz which furnished excited state spin-spin splittings directly for the first time. Wavelength dependent studies of dephasing times showed conclusively the existence of a larger splitting of 46 $\pm$ 2 cm$\sp{-1}$ in the excited E state. These results were found to be consistent with temperature dependent studies which reveal dephasing, near liquid-He temperatures, is dominated by a one-phonon direct dephasing process in the upper state with an activation energy of 68 $\pm$ 16 cm$\sp{-1}$ has a two-phonon Orbach contribution to dephasing in the lower state with an activation energy of 39 $\pm$ 5 cm$\sp{-1}.$ Experiments with circularly polarized light also revealed an interesting polarization selection rule originating from Zeeman coherence in the doublet E spin state of the $\sp3A$ ground state. A complete multi-electron model is presented which makes use of a previously undetected Jahn-Teller effect to explain all the observed excited state structure. An extension of these ultrafast techniques were applied to Tm$\sp{3+}$-Tm$\sp{3+}$ centers in YAlO$\sb3,$ permitting the first preliminary investigations of coherent dynamics on highly cooperative transitions. Dephasing times on the $\sp3F\sb4(\Gamma\sp2)$ $\to$ $\sp1G\sb4(\Gamma\sp1)$ excited state transitions were found to increase from 35 $\pm$ 2 ps to 61 $\pm$ 6 ps with decreasing intensity of a resonant auxiliary cw laser which populates this transition in a controllable fashion. Temperature dependence studies revealed dephasing on this cooperative transition was dominated by a direct process with an activation energy of 157 $\pm$ 16 cm$\sp{-1}$ at liquid-He temperatures. These results were consistent with expected dephasing rate dependence for interacting Tm$\sp{3+}$-Tm$\sp{3+}$ centers.

•Jan 1, 1993•0 citations
Here we investigate the temperature-dependent non-Markovian dynamics of the SiV^- center in diamond, focusing on the roles of low- and high-frequency quasi-localized phonon modes. Low-frequency phonons exhibit stronger electron-phonon coupling, leading to long-lived dephasing rate, while high-frequency phonons induce rapid attenuation of oscillatory dephasing rate facilitating a persistent memory effect. The non-Markovianity measure N_C shows memory effects persisting at low temperatures but diminishing at high temperatures due to enhanced damping. The temperature dependence of N_C follows a monotonic decay, from which a transition temperature T_NM=110 K is determined. These results highlight the interplay between phonon activation and damping in shaping quantum coherence, offering insights for optimizing solid-state quantum systems.
We report on the coherence properties of single photons from chromium-based color centers in diamond. We use field-correlation and spectral line-shape measurements to reveal the interplay between slow spectral wandering and fast dephasing mechanisms as a function of temperature. The zero-phonon transition frequency and its linewidth follow a power-law dependence on temperature, which is consistent with direct electron-phonon coupling and phonon-modulated Coulomb coupling to nearby impurities, which are the predominant fast dephasing mechanisms for these centers. Further, the observed reduction in the quantum yield for photon emission as a function of temperature suggests the opening of additional nonradiative channels through thermal activation to higher-energy states and indicates a near-unity quantum efficiency at 4 K.
In the present work, ultrafast photon echo spectroscopy has been applied to investigate dephasing dynamics and excited state electronic structure of impurity N-V centers in diamond and Tm$\sp{3+}$-Tm$\sp{3+}$ centers. In the N-V center, quantum beat measurements revealed modulation frequencies of 0.63 ±\pm± 0.02 GHz, 1.650 ±\pm± 0.003 GHz, and 2.298 ±\pm± 0.006 GHz which furnished excited state spin-spin splittings directly for the first time. Wavelength dependent studies of dephasing times showed conclusively the existence of a larger splitting of 46 ±\pm± 2 cm$\sp{-1}$ in the excited E state. These results were found to be consistent with temperature dependent studies which reveal dephasing, near liquid-He temperatures, is dominated by a one-phonon direct dephasing process in the upper state with an activation energy of 68 ±\pm± 16 cm$\sp{-1}$ has a two-phonon Orbach contribution to dephasing in the lower state with an activation energy of 39 ±\pm± 5 cm$\sp{-1}.$ Experiments with circularly polarized light also revealed an interesting polarization selection rule originating from Zeeman coherence in the doublet E spin state of the $\sp3A$ ground state. A complete multi-electron model is presented which makes use of a previously undetected Jahn-Teller effect to explain all the observed excited state structure. An extension of these ultrafast techniques were applied to Tm$\sp{3+}$-Tm$\sp{3+}$ centers in YAlO$\sb3,$ permitting the first preliminary investigations of coherent dynamics on highly cooperative transitions. Dephasing times on the $\sp3F\sb4(\Gamma\sp2)$ →\to→ $\sp1G\sb4(\Gamma\sp1)$ excited state transitions were found to increase from 35 ±\pm± 2 ps to 61 ±\pm± 6 ps with decreasing intensity of a resonant auxiliary cw laser which populates this transition in a controllable fashion. Temperature dependence studies revealed dephasing on this cooperative transition was dominated by a direct process with an activation energy of 157 ±\pm± 16 cm$\sp{-1}$ at liquid-He temperatures. These results were consistent with expected dephasing rate dependence for interacting Tm$\sp{3+}$-Tm$\sp{3+}$ centers.