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Applied Physics Letters

Temperature dependent energy level shifts of nitrogen-vacancy centers in diamond

Xiu-Qi Chen, Chun‐Hua Dong, Fang‐Wen Sun, Chang‐Ling Zou, Jin‐Ming Cui, Z.-F. Han, Guang‐Can Guo

Published Oct 17, 2011• 193 citations
Publisher

Abstract

Magnetic resonance and fluorescence spectra of nitrogen-vacancy (NV) color centers ensemble in high purity diamond sample were measured, with temperature ranging from 5.6 K to 295 K. Both microwave and optical transition energies have similar nonlinear temperature dependent changes, which might mainly originate from the local thermal expansion. As the frequency shifts will reduce the fidelity of resonant quantum control, the present results demonstrate the necessity of taking temperature fluctuation into consideration. For temperature below 100 K, the transition energies show tendencies to be constant, which indicate higher stability and performance in applications with NV centers.

DOI
10.1063/1.3652910

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Magnetic resonance and fluorescence spectra of nitrogen-vacancy (NV) color centers ensemble in high purity diamond sample were measured, with temperature ranging from 5.6 K to 295 K. Both microwave and optical transition energies have similar nonlinear temperature dependent changes, which might mainly originate from the local thermal expansion. As the frequency shifts will reduce the fidelity of resonant quantum control, the present results demonstrate the necessity of taking temperature fluctuation into consideration. For temperature below 100 K, the transition energies show tendencies to be constant, which indicate higher stability and performance in applications with NV centers.
Laser-induced fluorescence quenching in nitrogen-vacancy (NV) centers in diamond is studied simultaneously with in situ measurements of the heating-induced shift of the electron spin resonance of NV centers in the presence of a microwave field. These experiments reveal a strong correlation between fluorescence suppression in NV centers and the rise of the local temperature inside the diamond crystal. This finding sheds light on quantum pathways behind stimulated fluorescence quenching in NV centers of diamond and may imply significant limitations on the applications of this effect as a method of superresolving imaging in biological systems.
We study the spectroscopy of an ensemble of negatively charged nitrogen-vacancy centers in diamond at high temperatures between room temperature and 700K under high vacuum conditions. Spin resonances are studied using optical detection of magnetic resonance (ODMR), and optical spectroscopy is employed to study radiative transitions. Upon increasing the temperature, the intensity of radiative decay in visible and infrared decreased. In addition, the ODMR resonance frequencies were decreased, and the phonon line emission shifted to higher wavelengths. Density functional theory calculation of the zero-field splitting parameter (D) revealed that thermal expansion is not enough to explain the shift in the ODMR frequencies. Fitting the measured intensity of photo-luminescence with the theoretical predictions of the Mott–Seitz model yields the value of 0.22eV for the energy barrier associated with nonradiative decay.
The ensemble of nitrogen-vacancy (NV) centers is widely used in quantum information transmission, high-precision magnetic field, and temperature sensing due to their advantages of long-lived state and the ability to be pumped by optical cycling. In this study, we investigate the zero-phonon line behavior of the two charge states of NV centers by measuring the photoluminescence of the NV center at 1.6 K-300 K. The results demonstrate a positional redshift, an increase in line width, and a decrease in fluorescence intensity for the ZPL of NV0 and NV- as the temperature increased. In the range of 10 K to 140 K, the peak shift with high concentrations of NV- revealed an anomaly of bandgap reforming. The peak position undergoes a blueshift and then a redshift as temperature increases. Furthermore, the transformation between NV0 and NV- with temperature changes has been obtained in diamonds with different nitrogen concentrations. This study explored the ZPL characteristics of NV centers in various temperatures, and the findings are significant for the development of high-resolution temperature sensing and high-precision magnetic field sensing in ensemble NV centers.
Diamond samples of defects with negative charged nitrogen-vacancy (NV) centers are promising solid state spin sensors suitable for quantum information processing, high sensitive measurements of magnetic, electric and thermal fields in nanoscale. The diamond defect with a NV center is unique for its robust temperature-dependent zero field splitting Dgs of the triplet ground state. This property enables optical readout of electron spin states through manipulation of the ground triplet state using microwave resonance with Dgs from 100 K to about 600 K. Thus, prohibiting Dgs from unwanted external thermal disturbances is crucial for an accurate measurement using diamond NV sensors. Our observation demonstrates the existence of a prominent microwave heating effect on the diamond samples of NV centers. The effect is inevitable to shift Dgs and cause measurement errors. The temperature increment caused by the effect monotonically depends on the power and the duration of microwave irradiation. The effect is obvious with the microwave irradiation in the continuous mode and some pulse sequence modes, but is neglectable for the quantum lock-in XY8-N method.
The spin dynamics of the negatively charged nitrogen-vacancy (NV⁻) centers in diamond are highly sensitive to quantum electromagnetic fluctuations arising from optical excitation, chemical interactions, and thermal processes. Here we investigated the optical and spin properties of ensembles of NV⁻ centers in diamond under continuous-wave (CW) and nanosecond pulsed laser excitation. Optical detection of magnetic resonance (ODMR) is employed to monitor laser induced shifts of the zero-field splitting parameter D under ambient and high-vacuum conditions. Increasing CW laser power results in a systematic downshift of the resonance frequency due to laser-induced heating. The effect is significantly enhanced under vacuum, where the shift in D reaches up to ~17 MHz, compared to ~5 MHz in air, emphasizing the role of environmental thermal dissipation. Under nanosecond pulsed excitation, increasing the pulse repetition rate similarly leads to resonance shifts and reduced ODMR contrast, consistent with cumulative thermal effects. Visible and infrared spectroscopy confirm power dependent modifications of NV emission. Time resolved photoluminescence measurements showed that the excited-state lifetime (~6 ns) remains nearly constant across the investigated excitation range, indicating that in this regime the dominant limitation is thermal loading of the spin resonance rather than a change in intrinsic radiative decay dynamics. These results provide a comprehensive characterization of thermal effects in high power optical excitation of NV ensembles and are directly relevant for high intensity NV-based sensing and spectroscopy, particularly in vacuum environments.
Abstract Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi-localized vibrational modes as well as ultrafast spectral diffusion on the picosecond timescale. The intrinsic, ensemble-averaged homogeneous linewidth is found to be in the tens of GHz range by extrapolating to zero temperature. We also observe a temperature-dependent Stark splitting of the excited state manifold, relevant to NV sensing protocols.