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Physical review. B, Condensed matter

Electronic structure of the N-Vcenter in diamond: Experiments

Alan Lenef, Steven W. Brown, David A. Redman, Stephen Colby Rand, J.E. Shigley, Emmanuel Fritsch

Published May 15, 1996• 68 citations
Publisher

Abstract

Quantum-beat spectroscopy has been used to observe excited states of the N-V center in diamond. For the 1.945-eV optical transition, direct evidence is presented for the existence of GHz-scale fine structure, together with a much larger 46-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ level splitting in the E state. An interference effect observed in transient four-wave-mixing response is explained with a polarization selection rule involving Zeeman coherence among magnetic sublevels. Also, detailed dephasing measurements versus temperature and wavelength have identified the decay mechanisms operative among the various states. A comparison of these results with ab initio calculations of excited electronic structure and interactions based on several multielectron models supports the conclusion that the N-V center is a neutral, two-electron center governed by a strong Jahn-Teller effect and weak spin-spin interactions. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physrevb.53.13427

Related papers

Electronic structure of the nitrogen-vacancy color center in diamond.

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The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 $\pm$ 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 $\pm$ 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 $\pm$ 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.

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Spin dynamics and electronic states of N-Vcenters in diamond by EPR and four-wave-mixing spectroscopy

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A new phase-modulation technique for nonlinear laser spectroscopy is applied with a relative resolving power in the sub-Hz range to measure fundamental relaxation processes of the N-V center in diamond. Complementary EPR experiments versus temperature establish the spin character of the ground state in the absence of optical illumination and show that spin-lattice decay occurs via two-phonon processes involving the dominant vibrational mode. The combined results permit deduction of reliable fine-structure assignments for three states of the center and accurate values for zero-field intersystem crossing and spin-lattice relaxation rates from linewidths of individual resonances in the four-wave-mixing spectrum.

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Reply to “Comment on ‘Electronic structure of the N- V center in diamond: Theory’ ”

Alan Lenef, Stephen Colby Rand

We present insights into the electronic structure and relaxation of N-$V$ color centers in diamond which support the contention that Jahn-Teller effects may play a very significant role in the excited $E$ state. We also consider several opposing arguments, but show that the unusual relaxation behavior of the N-$V$ center can mask common signatures of the Jahn-Teller effect, and that it remains a strong candidate for the dominant interaction determining excited-state splittings.

Physical review. B, Condensed matter•Dec 15, 1997•14 citations

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.

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Dynamic Jahn-Teller Effect in the NV− Center in Diamond

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Electronic structure of the negatively charged silicon-vacancy center in diamond

Lachlan J. Rogers, Kay D. Jahnke, Marcus W. Doherty +8 more

The negatively charged silicon-vacancy (SiV${}^{\ensuremath{-}}$) center in diamond is a promising single-photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\ensuremath{\langle}111\ensuremath{\rangle}$ aligned split-vacancy structure with ${\mathrm{D}}_{3\mathrm{d}}$ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738-nm optical resonance.

arXiv:1310.3131•Physical Review B•Jun 2, 2014•227 citations
Quantum-beat spectroscopy has been used to observe excited states of the N-V center in diamond. For the 1.945-eV optical transition, direct evidence is presented for the existence of GHz-scale fine structure, together with a much larger 46-cm\ensuremath−1{\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}cm\ensuremath−1 level splitting in the E state. An interference effect observed in transient four-wave-mixing response is explained with a polarization selection rule involving Zeeman coherence among magnetic sublevels. Also, detailed dephasing measurements versus temperature and wavelength have identified the decay mechanisms operative among the various states. A comparison of these results with ab initio calculations of excited electronic structure and interactions based on several multielectron models supports the conclusion that the N-V center is a neutral, two-electron center governed by a strong Jahn-Teller effect and weak spin-spin interactions. \textcopyright{} 1996 The American Physical Society.
The nitrogen - vacancy (N-V) center is a point defect found in diamonds containing substitutional nitrogen impurities. It arises after exposure to ionizing radiation and subsequent thermal annealing. The physical structure of the center has previously been identified as a substitutional nitrogen atom located adjacent to a neutral carbon vacancy, but prior to this work knowledge of its electronic structure was very incomplete. The results presented here are intended to establish the energy level structure of the N-V center unambiguously, using nonlinear laser spectroscopy in concert with paramagnetic resonance experiments. A new technique which achieves sub-Hertz resolution in nearly degenerate four-wave mixing (NDFWM) and optical two-beam coupling experiments was applied to determine the decay rates of excited states in the N-V center. Laser-enhanced EPR experiments were performed to assign spin character to the ground state. Fluorescent emission of the center was used to determine excited state energies. In particular, these results resolve earlier conflicting reports of the N-V ground state structure and offer a picture of state energies and dynamics consistent with all observations to date. The principal results of this thesis may be summarized as follows. We show that the ground state of the center consists of a spin triplet ground state with a zero-field splitting of 2.88 GHz and a spin-lattice relaxation time of 1.170 ±\pm± 0.003 ms. The first parity-allowed transition occurs to a triplet excited state at 1.944 eV with a lifetime of 13.3 ±\pm± 0.2 ns. The first metastable singlet excited state is shown to have a lifetime of 265.3 ±\pm± 0.6 ms at room temperature and its temperature dependence measured between 77 and 295 K. Through low temperature studies the mechanism for ground state spin-lattice relaxation is determined to be a two-phonon process involving 63 meV optical phonons. Finally, the origin of satellite lines in the persistent hole-burning spectrum is tentatively explained using our picture of the energy level structure and used to infer a zero-field spin splitting in the excited triplet state of 0.6 GHz.
A new phase-modulation technique for nonlinear laser spectroscopy is applied with a relative resolving power in the sub-Hz range to measure fundamental relaxation processes of the N-V center in diamond. Complementary EPR experiments versus temperature establish the spin character of the ground state in the absence of optical illumination and show that spin-lattice decay occurs via two-phonon processes involving the dominant vibrational mode. The combined results permit deduction of reliable fine-structure assignments for three states of the center and accurate values for zero-field intersystem crossing and spin-lattice relaxation rates from linewidths of individual resonances in the four-wave-mixing spectrum.
We present insights into the electronic structure and relaxation of N-VVV color centers in diamond which support the contention that Jahn-Teller effects may play a very significant role in the excited EEE state. We also consider several opposing arguments, but show that the unusual relaxation behavior of the N-VVV center can mask common signatures of the Jahn-Teller effect, and that it remains a strong candidate for the dominant interaction determining excited-state splittings.
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.
The negatively charged nitrogen-vacancy (NV(-)) center in diamond is considered to be one of the most promising solid state systems for quantum information applications. Excited states of the NV(-) center play a center role in the proposed applications. Using a combination of first-principles calculations and vibronic interaction model analysis, we establish the presence of a dynamic Jahn-Teller effect in the (3)E excited state. The calculated temperature-dependent dephasing rate for the zero phonon line as well as the splitting of the first two vibronic states are in good agreement with experiment.
The negatively charged silicon-vacancy (SiV${}^{\ensuremath{-}}$) center in diamond is a promising single-photon source for quantum communications and information processing. However, the center's implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $\ensuremath{\langle}111\ensuremath{\rangle}$ aligned split-vacancy structure with D3d{\mathrm{D}}_{3\mathrm{d}}D3d​ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the center's 738-nm optical resonance.