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arXiv:1810.05265

Anti-Stokes excitation of solid-state quantum emitters for nanoscale thermometry

Toan Trong Tran, Blake Regan, Евгений Алексеевич Екимов, Zhao Mu, Yu Zhou, Weibo Gao, Prineha Narang, Alexander S. Solntsev, Milos Toth, Igor Aharonovich, Carlo Bradac

Published Oct 11, 2018• 0 citations
arXivHTMLPDF

Abstract

Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method employed to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems, and harness it towards the realization of practical nanoscale thermometry and sensing.

DOI
10.48550/arxiv.1810.05265

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Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light emitting diodes and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite Anti-Stokes process, where excitation is performed with lower energy photons. We report that the process is sufficiently efficient to excite even a single quantum system, namely the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method employed to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems, and harness it towards the realization of practical nanoscale thermometry and sensing.
Color centers in solids are the fundamental constituents of a plethora of applications such as lasers, light-emitting diodes, and sensors, as well as the foundation of advanced quantum information and communication technologies. Their photoluminescence properties are usually studied under Stokes excitation, in which the emitted photons are at a lower energy than the excitation ones. In this work, we explore the opposite anti-Stokes process, where excitation is performed with lower-energy photons. We report that the process is sufficiently efficient to excite even a single quantum system-namely, the germanium-vacancy center in diamond. Consequently, we leverage the temperature-dependent, phonon-assisted mechanism to realize an all-optical nanoscale thermometry scheme that outperforms any homologous optical method used to date. Our results frame a promising approach for exploring fundamental light-matter interactions in isolated quantum systems and harness it toward the realization of practical nanoscale thermometry and sensing.
Abstract Quantum emitters are widely used in quantum networks, quantum information processing, and quantum sensing due to their excellent optical properties. Compared with Stokes excitation, quantum emitters under anti-Stokes excitation exhibit better performance. In addition to laser cooling and nanoscale thermometry, anti-Stokes excitation can improve the coherence of single-photon sources for advanced quantum technologies. In this review, we follow the recent advances in phonon-assisted upconversion photoluminescence of quantum emitters and discuss the upconversion mechanisms, applications, and prospects for quantum emitters with anti-Stokes excitation.
Optically addressable solid-state color center spin qubits have become important platforms for quantum information processing, quantum networks and quantum sensing. The readout of color center spin states with optically detected magnetic resonance (ODMR) technology is traditionally based on Stokes excitation, where the energy of the exciting laser is higher than that of the emission photons. Here, we investigate an unconventional approach using anti-Stokes excitation to detect the ODMR signal of silicon vacancy defect spin in silicon carbide, where the exciting laser has lower energy than the emitted photons. Laser power, microwave power and temperature dependence of the anti-Stokes excited ODMR are systematically studied, in which the behavior of ODMR contrast and linewidth is shown to be similar to that of Stokes excitation. However, the ODMR contrast is several times that of the Stokes excitation. Coherent control of silicon vacancy spin under anti-Stokes excitation is then realized at room temperature. The spin coherence properties are the same as those of Stokes excitation, but with a signal contrast that is around three times greater. To illustrate the enhanced spin readout contrast under anti-Stokes excitation, we also provide a theoretical model. The experiments demonstrate that the current anti-Stokes excitation ODMR approach has promising applications in quantum information processing and quantum sensing.
The manipulation of the charge states of nitrogen-vacancy (NV) centers in diamond is a prerequisite for next-generation quantum sensing, communication, and computing. Here, we use phonon-assisted anti-Stokes excitation to realize the reversible conversion between the NV 0 and NV – states. In this case, we observe two decay processes of NV – centers with lifetimes as long as tens of seconds. By studying the kinetics of spectral structure evolution of NV – states, we find that the spectral structure of the NV – center is modulated by the charge state transition process under anti-Stokes excitation. We propose that the main reason is the local electric field generated by the ionization of the NV –, which changes the radiation environment of the color centers. Our results might provide an alternative method to control the charge states of nitrogen-vacancy centers.
Phonon-assisted anti-Stokes photoluminescence (ASPL) up-conversion lies at the heart of optical refrigeration in solids. The thermal energy contained in the lattice vibrations is taken away by the emitted anti-Stokes photons' ASPL process, resulting in laser cooling of solids. To date, net laser cooling of solids is limited in rare-earth (RE)-doped crystals, glasses, and direct band gap semiconductors. Searching more solid materials with efficient phonon-assisted photoluminescence up-conversion is important to enrich optical refrigeration research. Here, we demonstrate the phonon-assisted PL up-conversion process from the silicon vacancy (SiV) center in diamond for the first time by studying ASPL spectra for the dependence of temperature, laser power, and excitation energy. Although net cooling has not been observed, our results show that net laser cooling might be eventually achieved in diamond by improving the external quantum efficiency to higher than 95%. Our work provides a promising route to investigate the laser cooling effect in diamond.