Temperature-dependent excited state lifetimes of nitrogen vacancy centers in individual nanodiamonds

Abstract

Nitrogen vacancy (NV) centers are fluorescent defects widely employed for thermometry, most commonly via temperature-dependent shifts of their optically detected magnetic resonance. Recently, all-optical approaches based on temperature-dependent features of the NV center fluorescence spectrum have also gained traction. Excited state lifetime thermometry is an all-optical technique that has been implemented using other fluorophores but has not previously been demonstrated for NV centers in individual nanodiamonds (NDs). Here, we report temperature-dependent excited state lifetime measurements of NV centers in individual NDs between 300 K and 500 K. We measure a 32 ± 7.0% and 35 ± 8.3% average decrease in the excited state lifetimes of individual NDs on silicon and glass substrates, respectively, over this temperature range. A linear approximation applicable to nearly all measured NDs yields temperature coefficients of −2000 ± 240 ppm/K and −2600 ± 280 ppm/K for NDs on silicon and glass, respectively. In addition to all-optical operation, single-ND excited state lifetime thermometry offers ∼100 ns temporal resolution and utilizes time-correlated single photon counting measurements ideally suited to low emission intensities, a limiting factor for other NV center thermometry techniques above 700 K. We demonstrate that atomic force microscope nanomanipulation can position individual NDs at critical locations on a sample of interest, enabling single-point temperature measurements that combine ∼100 ns temporal resolution and ∼100 nm spatial resolution. This work also has broader implications for other single-ND excited state lifetime sensing applications, where care is required to avoid conflating changes in temperature and other environmental parameters.