Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Journal of Applied Physics

Autler–Townes effect of the photoexcited diamond nitrogen-vacancy center in its triplet ground state

Xing-Fei He, Peter Fisk, Neil B. Manson

Published Jul 1, 1992• 31 citations
Publisher

Abstract

The Autler–Townes effect in nuclear magnetic resonance (NMR) and electron paramagnetic resonance has been observed using recently developed Raman heterodyne techniques. The measurements were carried out on the nitrogen-vacancy color center in diamond, where the 3A↔3E optical transition was driven by a single mode dye laser at 638 nm while the magnetic transitions in the 3A ground state were driven by two rf fields. The measured splittings in the NMR lines were found to be in good agreement with theoretical predictions. Using the Autler–Townes effect, the magnitude of the dipole moments of the mI=0↔±1 (mS=0) transitions in the ground state was determined, and found to be the same. Comparison of this latter result with the NMR spectra shows that Raman heterodyne signal intensities are determined by population factors.

DOI
10.1063/1.352161

Related papers

Raman heterodyne detected magnetic resonance of the nitrogen-vacancy centre in diamond

Xing-Fei He

This thesis describes the Raman heterodyne detection of magnetic resonance in the ³A ground state of the nitrogen-vacancy C'-1· V) centre in diamond. The recently developed theory of Raman heterodyne spectroscopy was tested and compared with the spectra measured on the N-V centre. Among those results, the electron-nuclear double resonance (ENDOR), nuclear-nuclear double resonance (double NMR), Autler-Townes effect, coherence transfer and Zeeman quantum beat were observed for the first time using such techniques. Raman heterodyne techniques were also used to investigate the level anticrossing, hyperfine and nuclear quadrupole interactions, and spin relaxations of the N-V centre with high sensitivity and precision. This thesis is comprised of three parts. Part one includes Chapters 1 to 3, providing introductory accounts. Chapter l is an introduction to the N-V colour centre, which describes the defect configuration, the spin Hamiltonian and the calculations of energy levels and wave functions of the ³A ground state. Chapter 2 briefly describes the theory of Raman heterodyne spectroscopy - a coherent optical radio-frequency (RF) double resonance technique, in particular the Raman heterodyne signals at weak and intense RF fields. Chapter 3 deals with experimental details and techniques utilized in the studies. Part two consists of Chapters 4 and 5, where the Raman heterodyne theory is compared with experimental results. Chapter 4 presents the Raman heterodyne detected nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) lineshapes compared with theoretical results at various RF power levels, laser intensities and laser frequencies within the 6380A zero-phonon line. The double resonance spectra obtained by Raman heterodyne techniques are discussed in Chapter 5, where attention is paid to the analysis of their spectral profiles depending on the detection scheme. The application of Raman heterodyne techniques to the studies of magnetic resonance of the N-V centre is described in part three, consisting of Chapters 6 to 9. The EPR measurements are described in Chapter 6, which were used to study various interactions near the level anticrossing, in particular the spin alignment. The hyperfine and nuclear quadrupole interactions probed by the NMR, ENDOR and hole burning measurements are described in Chapter 7. From these measurements, the hyperfine and quadrupole parameters in the spin Hamiltonian were fully determined. Chapter 8 deals with the Autler-Townes effect in the NMR and EPR transitions. By measuring the Autler-Townes spittings, the magnitudes of matrix elements of the NMR transitions were examined and compared. Chapter 9 presents the coherent spin transient properties, including nutations, echoes, Zeeman beating and coherence transfer. The dephasing time and homogeneous linewidths of the NMR and EPR transitions were then determined from the echo measurements. Finally, the thesis is summarized in Chapter 10.

•Jan 1, 1991•0 citations

Paramagnetic resonance of photoexcited N-Vdefects in diamond. I. Level anticrossing in the 3 Aground state

Xing-Fei He, Neil B. Manson, Peter Fisk

Raman-heterodyne-detected paramagnetic resonance has been used to study the level anticrossing in the $^{3}$A state of the N-V defect in diamond. The electron-paramagnetic-resonance (EPR) frequencies are well accounted for by a triplet-spin Hamiltonian. Comparison of the EPR spectra with the calculated transition dipole strengths indicates that optical pumping determines, to a large extent, the Raman-heterodyne-signal intensity. Spin alignment in the $^{3}$A ground state under optical pumping leads to the collapse of the EPR signal at the level anticrossing, where the population is equalized due to the mixing of the spin states. This is substantiated by transient nutation and spin-echo measurements, from which the dipole moment and dephasing time are examined. Laser detuning within the 638-nm zero-phonon line shows that the Raman signal is only detectable when the laser frequency is tuned to the low-energy part of the optical line.

Physical review. B, Condensed matter•Apr 1, 1993•88 citations

Raman heterodyne detection of electron paramagnetic resonance

Keith Holliday, X.-F. He, Peter Fisk +1 more

We report the detection of an electron paramagnetic resonance signal using Raman heterodyne spectroscopy, a rf -optical double-resonance technique. The signals are associated with the nitrogen-vacancy center in diamond, which has a spin-triplet ground state. A three-line spectrum associated with the nitrogen hyperfine structure is observed for various magnetic field strengths and crystal orientations.

Optics Letters•Apr 1, 1990•34 citations

Coherent population trapping in diamond N-V centers at zero magnetic field

Charles Santori, David A. Fattal, Sean M. Spillane +11 more

Coherent population trapping at zero magnetic field was observed for nitrogen-vacancy centers in diamond under optical excitation. This was measured as a reduction in photoluminescence when the detuning between two excitation lasers matched the 2.88 GHz crystal-field splitting of the color center ground states. This behavior is highly sensitive to strain, which modifies the excited states, and was unexpected following recent experiments demonstrating optical readout of single nitrogen-vacancy electron spins based on cycling transitions. These results demonstrate for the first time that three-level Lambda configurations suitable for proposed quantum information applications can be realized simultaneously for all four orientations of nitrogen-vacancy centers at zero magnetic field.

arXiv:cond-mat/0602573•Optics Express•Jan 1, 2006•107 citations

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

David A. Redman

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.

•Jan 1, 1991•0 citations

Raman-heterodyne-detected nonlinear susceptibility with an arbitrary radio-frequency field strength

Xing-Fei He, Peter Fisk, Neil B. Manson

Raman-heterodyne-detected complex nonlinear susceptibility has been measured and analyzed in detail with a radio-frequency field strength varying from weak to strong. The experiments were carried out on the nitrogen–vacancy color center in diamond involving both nuclear magnetic resonance and electron paramagnetic resonance transitions. The dispersive and the absorptive components of the nonlinear susceptibility are shown to have different saturation behaviors, and an anomalous-amplitude line shape arises where the dispersion component dominates in the response spectrum at high RF powers. The experimental results are found to be in good agreement with theoretical profiles, where no adjustable parameter is included in the calculation.

Journal of the Optical Society of America B•May 1, 1993•2 citations
The Autler–Townes effect in nuclear magnetic resonance (NMR) and electron paramagnetic resonance has been observed using recently developed Raman heterodyne techniques. The measurements were carried out on the nitrogen-vacancy color center in diamond, where the 3A↔3E optical transition was driven by a single mode dye laser at 638 nm while the magnetic transitions in the 3A ground state were driven by two rf fields. The measured splittings in the NMR lines were found to be in good agreement with theoretical predictions. Using the Autler–Townes effect, the magnitude of the dipole moments of the mI=0↔±1 (mS=0) transitions in the ground state was determined, and found to be the same. Comparison of this latter result with the NMR spectra shows that Raman heterodyne signal intensities are determined by population factors.
This thesis describes the Raman heterodyne detection of magnetic resonance in the ³A ground state of the nitrogen-vacancy C'-1· V) centre in diamond. The recently developed theory of Raman heterodyne spectroscopy was tested and compared with the spectra measured on the N-V centre. Among those results, the electron-nuclear double resonance (ENDOR), nuclear-nuclear double resonance (double NMR), Autler-Townes effect, coherence transfer and Zeeman quantum beat were observed for the first time using such techniques. Raman heterodyne techniques were also used to investigate the level anticrossing, hyperfine and nuclear quadrupole interactions, and spin relaxations of the N-V centre with high sensitivity and precision. This thesis is comprised of three parts. Part one includes Chapters 1 to 3, providing introductory accounts. Chapter l is an introduction to the N-V colour centre, which describes the defect configuration, the spin Hamiltonian and the calculations of energy levels and wave functions of the ³A ground state. Chapter 2 briefly describes the theory of Raman heterodyne spectroscopy - a coherent optical radio-frequency (RF) double resonance technique, in particular the Raman heterodyne signals at weak and intense RF fields. Chapter 3 deals with experimental details and techniques utilized in the studies. Part two consists of Chapters 4 and 5, where the Raman heterodyne theory is compared with experimental results. Chapter 4 presents the Raman heterodyne detected nuclear magnetic resonance (NMR) and electron paramagnetic resonance (EPR) lineshapes compared with theoretical results at various RF power levels, laser intensities and laser frequencies within the 6380A zero-phonon line. The double resonance spectra obtained by Raman heterodyne techniques are discussed in Chapter 5, where attention is paid to the analysis of their spectral profiles depending on the detection scheme. The application of Raman heterodyne techniques to the studies of magnetic resonance of the N-V centre is described in part three, consisting of Chapters 6 to 9. The EPR measurements are described in Chapter 6, which were used to study various interactions near the level anticrossing, in particular the spin alignment. The hyperfine and nuclear quadrupole interactions probed by the NMR, ENDOR and hole burning measurements are described in Chapter 7. From these measurements, the hyperfine and quadrupole parameters in the spin Hamiltonian were fully determined. Chapter 8 deals with the Autler-Townes effect in the NMR and EPR transitions. By measuring the Autler-Townes spittings, the magnitudes of matrix elements of the NMR transitions were examined and compared. Chapter 9 presents the coherent spin transient properties, including nutations, echoes, Zeeman beating and coherence transfer. The dephasing time and homogeneous linewidths of the NMR and EPR transitions were then determined from the echo measurements. Finally, the thesis is summarized in Chapter 10.
Raman-heterodyne-detected paramagnetic resonance has been used to study the level anticrossing in the 3^{3}3A state of the N-V defect in diamond. The electron-paramagnetic-resonance (EPR) frequencies are well accounted for by a triplet-spin Hamiltonian. Comparison of the EPR spectra with the calculated transition dipole strengths indicates that optical pumping determines, to a large extent, the Raman-heterodyne-signal intensity. Spin alignment in the 3^{3}3A ground state under optical pumping leads to the collapse of the EPR signal at the level anticrossing, where the population is equalized due to the mixing of the spin states. This is substantiated by transient nutation and spin-echo measurements, from which the dipole moment and dephasing time are examined. Laser detuning within the 638-nm zero-phonon line shows that the Raman signal is only detectable when the laser frequency is tuned to the low-energy part of the optical line.
Coherent population trapping at zero magnetic field was observed for nitrogen-vacancy centers in diamond under optical excitation. This was measured as a reduction in photoluminescence when the detuning between two excitation lasers matched the 2.88 GHz crystal-field splitting of the color center ground states. This behavior is highly sensitive to strain, which modifies the excited states, and was unexpected following recent experiments demonstrating optical readout of single nitrogen-vacancy electron spins based on cycling transitions. These results demonstrate for the first time that three-level Lambda configurations suitable for proposed quantum information applications can be realized simultaneously for all four orientations of nitrogen-vacancy centers at zero magnetic field.
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.
Raman-heterodyne-detected complex nonlinear susceptibility has been measured and analyzed in detail with a radio-frequency field strength varying from weak to strong. The experiments were carried out on the nitrogen–vacancy color center in diamond involving both nuclear magnetic resonance and electron paramagnetic resonance transitions. The dispersive and the absorptive components of the nonlinear susceptibility are shown to have different saturation behaviors, and an anomalous-amplitude line shape arises where the dispersion component dominates in the response spectrum at high RF powers. The experimental results are found to be in good agreement with theoretical profiles, where no adjustable parameter is included in the calculation.