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Wide-field fluorescent nanodiamond spin measurements toward real-time large-area intracellular thermometry

MetadataDetails
Publication Date2021-02-19
JournalScientific Reports
AuthorsYushi Nishimura, Keisuke Oshimi, Yumi Umehara, Yuka Kumon, Kazu Miyaji
InstitutionsKeio University, Osaka City University
Citations47
AnalysisFull AI Review Included
  • Core Achievement: Validation of camera-based wide-field Optically Detected Magnetic Resonance (ODMR) using nanodiamonds (NDs) for real-time, large-area intracellular thermometry in living HeLa cells.
  • Sensitivity Comparison: Wide-field ODMR achieved temperature sensitivities (1.7-2.2 K/sqrt(Hz)) comparable to those obtained via traditional photon-counter-based confocal detection (2.1 K/sqrt(Hz)) under the same setup.
  • Artifact Management: The study identified and characterized critical artifacts specific to wide-field detection, including contrast degradation due to background fluorescence and frequency shift errors caused by camera pixel saturation (Full-Well Capacity, FWC).
  • Positional Robustness: Wide-field detection proved robust against ND z-positional variation (defocusing), but lateral drift required careful selection of the Region of Interest (ROI) to prevent noise and spectral distortion.
  • Technological Roadmap: The results provide realistic acquisition parameters necessary for integrating rapid, multi-point ODMR protocols into wide-field systems, paving the way for real-time, large-area thermal live-imaging in biological applications.
ParameterValueUnitContext
ND Particle Size100nmNDNV100nmHi10ml (AdĂĄmas Nanotechnologies)
NV Centers per ND~500-Estimated concentration per particle
Excitation Wavelength532nmContinuous-wave laser
Excitation Power Density~10W/cm2Typical optical excitation intensity
ODMR Frequency Range2.810 to 2.93GHzMicrowave sweep range
Microwave Power (Antenna)10 to 50mWEstimated power delivered to the linear antenna
Temperature Dependence (dD/dT)-74kHz/KZero-field splitting temperature coefficient
Wide-Field Sensitivity (in cells)1.7 to 2.2K/sqrt(Hz)Measured precision in living HeLa cells
Confocal Sensitivity (in cells)2.1K/sqrt(Hz)Measured precision in living HeLa cells
Camera TypeEMCCD (Evolve Delta)-Wide-field detection system
Camera FWC (Single Pixel)185,000e-Full-Well Capacity
Camera ADC Resolution16bitAnalog-to-Digital Converter
Wide-Field Exposure Time (Atexp)10msStandard measurement parameter
Wide-Field Accumulations (nacc)100-Accumulations per frequency step
Confocal Integration Time (Atpc)100msStandard measurement parameter
Dish Temperature Stability (Ta)±0.25KStability over 250 min using thermistor
Spatial Resolution (Confocal)0.24”mFWHM of fluorescence spot
Spatial Resolution (Wide-Field)0.55”mFWHM of fluorescence spot
  1. Hybrid Microscopy Setup: A single home-built microscope was configured to switch between confocal detection (using an APD gated by a bit pattern generator) and wide-field detection (using an EMCCD camera slaved to the generator).
  2. Sample Preparation and Environment Control: HeLa cells were labeled with 100 nm NDs and cultured in custom antenna-integrated glass dishes. Phenol red was removed from the medium to eliminate laser absorption and heating artifacts.
  3. Temperature Calibration and Control: Dish temperature (Ta) was precisely controlled using a stage-top incubator with PID feedback on foil heaters, calibrated against an external Pt100 thermistor (Ta = 5.51 + 0.814Ti).
  4. Wide-Field Data Acquisition: The EMCCD acquired 16-bit images (10 ms exposure) for both microwave ON (signal) and OFF (reference) states, accumulating 100 images per frequency step to form a 32-bit average image.
  5. Artifact Characterization: The relationship between camera photon counts (mG-1Iccd) and APD photon counts (R∆tpc) was established. Experiments were conducted to map the effects of pixel saturation (FWC limit: 185,000 e-) and positional drift (lateral and z-axis) on ODMR contrast and center frequency.
  6. Intracellular Thermometry: Wide-field ODMR spectra were measured from multiple NDs simultaneously within living HeLa cells across different dish temperatures (e.g., 35.5 °C and 33.7 °C).
  7. Spectral Analysis: ODMR spectra were generated by dividing signal images by reference images, and the center frequency shift (Δω) was determined by fitting the spectra with a Gaussian function to calculate the temperature change.
  • Quantum Sensing and Imaging: Advancing the development of scalable quantum sensors based on NV centers, moving beyond single-point measurements to parallel, large-area thermal and magnetic imaging.
  • Cellular and Subcellular Thermometry: Providing a tool for real-time monitoring of temperature gradients and thermogenesis within living cells, crucial for studying molecular mechanisms related to cell death (e.g., photothermal cancer therapy) and cellular signaling (e.g., thermotaxis).
  • High-Throughput Biological Screening: Enabling simultaneous temperature measurements across multiple cells or regions in a large field of view, accelerating research in drug discovery and physiological studies.
  • Microscope and Detector Technology: Driving the demand for specialized scientific cameras (e.g., sCMOS or EMCCD) with high FWC (greater than 185,000 e-), high bit depth (greater than 16-bit), and low noise to optimize wide-field quantum sensing performance.
  • Nanodiamond Material Science: Requiring the production of highly optimized NDs with high NV concentration, low background fluorescence, and robust functionalization for stable intracellular delivery and targeting of specific organelles (e.g., mitochondria, lysosomes).