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Physical Review Letters

Revised Fine Splitting of Excitons in Diamond

R. Sauer, Hadwig Sternschulte, S. Wahl, K. Thonke, Thomas R. Anthony

Published May 1, 2000• 33 citations
Publisher

Abstract

We study low-strain synthetic high pressure, high temperature diamonds by cathodoluminescence and observe novel fine structure in the free exciton and the boron-bound exciton emission. The basic spectral structure is a doublet with DeltaE approximately 11 meV common to both exciton spectra. This resolves the previously found inequivalence of free exciton ( approximately 7 meV) and bound exciton ( approximately 12 meV) fine splitting. It is argued that for a spin-orbit interaction Delta(0) much smaller than the excitonic binding ( E(X) approximately 80 meV) and the excitonic localization ( E(loc) approximately 51 meV) at the boron acceptor, the orbital momentum and the spin of the particles constituting the electron-hole pair are recoupled to form spin singlet and triplet exciton states as the elementary excitations.

DOI
10.1103/physrevlett.84.4172

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We study low-strain synthetic high pressure, high temperature diamonds by cathodoluminescence and observe novel fine structure in the free exciton and the boron-bound exciton emission. The basic spectral structure is a doublet with DeltaE approximately 11 meV common to both exciton spectra. This resolves the previously found inequivalence of free exciton ( approximately 7 meV) and bound exciton ( approximately 12 meV) fine splitting. It is argued that for a spin-orbit interaction Delta(0) much smaller than the excitonic binding ( E(X) approximately 80 meV) and the excitonic localization ( E(loc) approximately 51 meV) at the boron acceptor, the orbital momentum and the spin of the particles constituting the electron-hole pair are recoupled to form spin singlet and triplet exciton states as the elementary excitations.
We observe exceptionally high diffusion of excitons in diamond using time-resolved photoluminescence imaging. The diffusivity is found to increase with decreasing temperature more rapidly than well-established predictions. The highest diffusion constant, $9.2\ifmmode\times\else\texttimes\fi{}{10}^{3}\phantom{\rule{0.28em}{0ex}}{\mathrm{cm}}^{2}/\text{s}$, measured for thermalized excitons is 150 times that recorded previously in diamond. We elucidate the momentum relaxation mechanisms determining transport: intraband and interband scattering by acoustic phonons in the exciton fine-structure levels. The enhanced diffusivity above 100 K is explained by a free-carrier contribution.
We have developed a new scheme for generating cold and high-density excitons in diamond by resonant excitation at the phonon-assisted absorption edge. Both the thermalization of excitons between fine-structure states and the effective temperature are examined with the tuning of the photon energy. The down-conversion rate for the excitons in the fine-structure states is found to be 3.5 ns independent of the photon energy, which means that the lowest-energy dark exciton can be created within a time scale comparable to its lifetime via the generation of a higher-energy bright exciton. With careful choice of excitation photon energy, we have achieved an electron-hole pair density of while maintaining the effective excitonic temperature below 15 K.
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.
The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T 0–T 1, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g (2)(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T 1→S→T 0 to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T 0) state sublevels can be obtained from the spectra and g (2)(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet 3 A-3 E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m S =0 sublevel of the excited 3 E state to the singlet 1 A state (~1 kHz) is much slower than the rates from the m S =±1 substates, while the rates of ISC transitions to different m S substates of the ground 3 A state are close to each other (~1 Hz). As a result, only the optical transition between m S =0 sublevels in the 3 A-3 E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g (2)(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T 0(m S )=0) transition and (ii) the S→T 0(m S =±1) transitions followed by the slow spin-lattice relaxation T 0(m S =±1)→T 0(m S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.
The emission intensity of diamond samples containing negatively charged nitrogen-vacancy centres are measured as a function of magnetic field along the ⟨111⟩ direction for various temperatures. At low temperatures the responses are sample and stress dependent and can be modelled in terms of the previous understanding of the 3 E excited state fine structure which is strain dependent. At room temperature the responses are largely sample and stress independent, and modelling involves invoking a strain independent excited state with a single zero field spin-level splitting of 1.42 GHz. The change in behaviour is attributed to a temperature dependent averaging process over the components of the excited state orbital doublet. It decouples orbit and spin and at high temperature the spin levels become independent of any orbit splitting. One significant implication of this averaging is that it simplifies the development of room temperature applications.
Silicon-vacancy (SiV) centers in diamond are promising systems for quantum information applications due to their bright single-photon emission and optically accessible spin states. Furthermore, SiV centers in low-strain diamond are insensitive to perturbations of the dielectric environment; i.e., they show very weak spectral diffusion. This property renders ensembles of SiV centers interesting for sensing applications. We here report on photoluminescence excitation (PLE) spectroscopy on an SiV ensemble in a low strain, chemical vapor deposition-grown high-quality diamond layer, where we measure the fine structure with high resolution and obtain the line widths and splittings of the SiV centers. We investigate the temperature dependence of the width and position of the fine structure peaks. Our measurements reveal line widths of about 10 GHz as compared to a lifetime limited width on the order of 0.1 GHz. This difference arises from the inhomogeneous broadening of the transitions caused by residual strain. To overcome inhomogeneous broadening we use spectral hole burning spectroscopy, which enables us to measure a nearly lifetime limited homogeneous line width of 279 MHz. Furthermore, we demonstrate evidence of coherent interaction in the system by driving a $\mathrm{\ensuremath{\Lambda}}$ scheme. Additional measurements on single emitters created by ion implantation confirm the homogeneous line widths seen in the spectral hole burning experiments and relate the ground-state splitting to the decoherence rate.