Temperature Dependence of Photoluminescence Intensity and Spin Contrast in Nitrogen-Vacancy Centers

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Temperature Dependence of Photoluminescence Intensity and Spin Contrast in Nitrogen-Vacancy Centers

S. Ernst, P. J. Scheidegger, S. Diesch, L. Lorenzelli, and C. L. Degen

Phys. Rev. Lett. 131, 086903 – Published 24 August 2023

Abstract

We report on measurements of the photoluminescence properties of single nitrogen-vacancy centers in diamond at temperatures between 4 K and 300 K. We observe a strong reduction of the PL intensity and spin contrast between ca. 10 K and 100 K that recovers to high levels below and above. Further, we find a rich dependence on magnetic bias field and crystal strain. We develop a comprehensive model based on spin mixing and orbital hopping in the electronic excited state that quantitatively explains the observations. Beyond a more complete understanding of the excited-state dynamics, our work provides a novel approach for probing electron-phonon interactions and a predictive tool for optimizing experimental conditions for quantum applications.

Received 22 December 2022
Accepted 9 May 2023

DOI:https://doi.org/10.1103/PhysRevLett.131.086903

Physics Subject Headings (PhySH)

Color centers Magneto-optical spectra Point defects Single photon sources Spin-phonon coupling Temperature

Nitrogen vacancy centers in diamond

Optically detected magnetic resonance Photoluminescence Quantum master equation

Condensed Matter, Materials & Applied PhysicsAtomic, Molecular & Optical

Authors & Affiliations

S. Ernst ^1,*, P. J. Scheidegger ^1,*, S. Diesch ¹, L. Lorenzelli¹, and C. L. Degen ^1,2,†

¹Department of Physics, ETH Zurich, Otto Stern Weg 1, 8093 Zurich, Switzerland
²Quantum Center, ETH Zurich, 8093 Zurich, Switzerland

^*These authors contributed equally to this work.
^†degenc@ethz.ch

Temperature-Dependent Photophysics of Single NV Centers in Diamond

Jodok Happacher, Juanita Bocquel, Hossein T. Dinani, Märta A. Tschudin, Patrick Reiser, David A. Broadway, Jeronimo R. Maze, and Patrick Maletinsky

Phys. Rev. Lett. 131, 086904 (2023)

Modeling temperature-dependent population dynamics in the excited state of the nitrogen-vacancy center in diamond

S. Ernst, P. J. Scheidegger, S. Diesch, and C. L. Degen

Phys. Rev. B 108, 085203 (2023)

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Vol. 131, Iss. 8 — 25 August 2023

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Images

Figure 1
(a) Time-dependent PL traces during a laser pulse, measured on NV-2 initialized to the $| 0 ⟩$ (open circles) and $| - 1 ⟩$ (filled circles) states at low, intermediate and high temperature. The spin contrast is given by the relative difference between the two curves (pink shading). Solid lines are fits to the PL dynamics. (b) Spin contrast versus temperature for three NV centers measured on Setup A (empty markers) and Setup B (filled marker). Solid lines show corresponding simulations for NV-1 and NV-2. A bias field of 3 mT is applied.
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Figure 2
(a) Level diagram in the NV spin subspace $H_{spin}$ of the electronic ground ( ${}^{3}{A_{2}}$ ) and excited ( ${}^{3}E$ ) states, as well as the metastable ( ${}^{1}{A_{1}}$ , ${}^{1}E$ ) shelving states. The intersystem crossing (dotted line) is spin selective, favoring decay out of $| \pm 1 ⟩$ . In panels (a)–(c), solid arrows mark spin-conserving transitions, and curly arrows symbolize phonons. (b) Level diagram in the orbital subspace $H_{orbit}$ of the NV ES ( ${}^{3}E$ ). Two orbital branches ( $E_{x}$ , $E_{y}$ ) split under strain $δ_{⊥}$ . One- and two-phonon processes cause hopping between branches at temperature-dependent rates $k_{↓, 1 (2)}$ ( $k_{↑, 1 (2)}$ not shown). (c) Example of levels in the composite Hilbert space of orbit and spin $H_{orbit} \otimes H_{spin}$ . Eigenstates are superpositions of $| 0 ⟩$ and $| \pm ⟩ \propto (| + 1 ⟩ \pm | - 1 ⟩)$ . Spin-conserving, phonon-mediated transitions involving $| 0 ⟩$ are depicted by gray arrows. $ω_{x (y)}$ are the Larmor frequencies of involved spin transitions. (d) Hopping rates as a function of temperature. Inverse optical lifetime $T_{{}^{3}E}^{- 1}$ and Larmor frequencies (in MHz) are indicated by horizontal lines. For panels (c) and (d), we use $δ_{⊥} = 40 GHz$ in the direction of a carbon bond at low magnetic field, such that only two basis states mix significantly ( ${| ϵ |}^{2} = {| ε_{| y, 0 ⟩, | y, - ⟩} |}^{2} = 0.1$ [26]).
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Figure 3
(a) Simulation of the PL in dependence of the magnetic field and temperature. The PL is strongly reduced at avoided crossings of the excited-state (symbols) and the ground-state (103 mT) energy levels. The white dotted line marks the PL minimum; colored solid lines indicate the line cuts shown in panel (b). The simulation is based on parameters fitted to NV-1. (b) Experimental PL curves for NV-1 measured as a function of magnetic field and temperature. Solid lines are fits. (c),(d) Energy levels for the NV-1 ES at 300 K (c, time-averaged) and at 4 K (d). Symbols refer to panel (a). (e) Experimental spin contrast as a function of temperature for NV centers with different strain $δ_{⊥}$ . Measurements are taken at 3 mT (empty circles) and 200 mT (filled circles). Solid lines show the corresponding simulations.
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