DOI: 10.5061/dryad.3r2280gvm
title: Molecular quantum nanosensors functioning in living cells

description: Quantitatively mapping temperature within living cells is essential for
 understanding subcellular biophysical processes; however, existing
 intracellular quantum sensors such as nanodiamonds with nitrogen-vacancy
 centers, quantum dots and fluorescent proteins face limitations in
 material heterogeneity, cytotoxicity, and thermometric specificity. Here,
 we present molecular quantum nanosensors (MQNs) as a next-generation
 platform for intracellular quantum sensing. MQNs embed pentacene molecular
 spin qubits within para-terphenyl nanocrystals coated with Pluronic F127,
 yielding a coherent spin system with molecular-level uniformity and long
 spin coherence times under physiological conditions. By chemically
 suppressing hyperfine interactions, we enhance spectral resolution and
 demonstrate spatially resolved absolute temperature sensing inside the
 nuclei of living cells. MQNs thus offer a chemically tunable, biologically
 compatible platform for quantum-level detection of thermal and biochemical
 states of intracellular environments.
description: # Molecular quantum nanosensors functioning in living cells Experimental
 dataset for the manuscript entitled "Molecular Quantum Nanosensors
 Functioning in Living Cells". ## Description of the data and file
 structure The compressed archive is organized by figure number. Each
 folder contains the underlying data used to generate the corresponding
 figure panels in the manuscript and Supplementary Materials (Figs. 1–5 and
 Figs. S1–S16). Recommended structure: For T1 and T2 measurements,
 exponential fitting was applied for the estimation of relaxation time. For
 Rabi measurements cos fitting was applied for the estimation of Rabi
 frequency. Abbreviations (used across files): MQN200 / MQN500: molecular
 quantum nanosensors particle sizes 200nm / 500nm **Figure-by-figure data
 contents and variables** **Figure 1** — Schematics and extracellular
 ODMR/pulsed ODMR characterization * File: Fig1.xlsx * Sheet: Fig1D —
 Example CW-ODMR spectrum (extracellular). * Variables (as labeled in
 sheet): * Frequency [Hz]: microwave frequency (Hz). * photon counts [cps]:
 fluorescence photon count rate (cps). * Sheet: Fig1E — Summary values (one
 value per particle/measurement) grouped by sample type. * Variables: *
 200nm ND, 200nm MQN, 500nm ND, 500nm MQN: per-particle summary values
 (units as used in the sheet). * Sheet: Fig1E 200nm ND — CW-ODMR spectra
 used for the statistics (multiple particles). * Variables: * Frequency:
 microwave frequency axis (as labeled). * ODMR 1 … ODMR 10: ODMR spectra
 for each particle/measurement index. * Sheet: Fig1E 500nm ND — CW-ODMR
 spectra used for the statistics (multiple particles). * Variables: *
 Frequency: microwave frequency axis (as labeled). * ODMR 1 … ODMR 10: ODMR
 spectra for each particle/measurement index. * Sheet: Fig1E 200nm MQN —
 CW-ODMR spectra used for the statistics (multiple particles). * Variables:
 * Frequency: microwave frequency axis (as labeled). * ODMR 1 … ODMR 10:
 ODMR spectra for each particle/measurement index. * Sheet: Fig1E 500nm MQN
 — CW-ODMR spectra used for the statistics (multiple particles). *
 Variables: * Frequency: microwave frequency axis (as labeled). * ODMR 1 …
 ODMR 10: ODMR spectra for each particle/measurement index. * Sheet: Fig1I
 — Rabi oscillation trace with fit (extracellular). * Variables: * Pulse
 Length [sec]: microwave pulse length (s). * data: measured normalized
 contrast. * fit: cosine fit to the Rabi oscillation. * Sheet: Fig1J — T1
 relaxation decay with fit (extracellular). * Variables: * Relaxation Time
 [sec]: waiting time (s). * data: measured normalized contrast. * fit:
 exponential fit used to estimate T1. * Sheet: Fig1K — T2 (echo) decay with
 fit (extracellular). * Variables: * Free Evolution Time [sec]:
 free-evolution time (s). * data: measured normalized contrast. * fit:
 exponential fit used to estimate T2. **Figure 2** — MQNs functioning in
 living cells (imaging + in-cell ODMR) * File: Fig2.xlsx * Sheet: Fig.2I —
 In-cell CW-ODMR spectrum (example). * Variables: * Frequency [Hz]:
 microwave frequency (Hz). * odmr data: ODMR signal (as acquired). * Sheet:
 Fig.2J — In-cell Rabi oscillation with fit. * Variables: * tau [sec]:
 pulse length (s). * rabi data: measured normalized contrast. * rabi fit:
 cosine fit to the Rabi oscillation. * Sheet: Fig.2K — In-cell T1
 relaxation decay with fit. * Variables: * tau [sec]: relaxation time (s).
 * T1 data: measured normalized contrast. * T1 fit: exponential fit used to
 estimate T1. * Sheet: Fig.2L — In-cell T2 (echo) decay with fit. *
 Variables: * tau [sec]: free-evolution time (s). * echo data: measured
 echo contrast. * echo fit: exponential fit used to estimate T2. **Figure
 3** — Absolute temperature measurement in living cells (dMQN thermometry)
 * File: Fig3.xlsx * Sheet: Fig.3A — Example dMQN CW-ODMR spectrum with
 peak fit. * Variables: * Frequency [Hz]: microwave frequency (Hz). * ODMR
 data: measured ODMR spectrum (after processing as used for the figure). *
 ODMR peak fit: fitted curve used to extract peak position. * Sheet: Fig.3A
 inset — ODMR spectrum with hyperfine-component fits (inset). * Variables:
 * Frequency [Hz]; ODMR data; ODMR peak fit; hyperfine fit 1; hyperfine fit
 2; ODMR spectrum from fit results. * Sheet: Fig3 B —
 Temperature-calibration replicates (block-form table). * Contents:
 repeated peak-frequency measurements grouped by temperature (°C) with
 adjacent average-frequency columns. * Variables (as labeled inside the
 table blocks): * Frequency [MHz]: extracted ODMR peak frequency for each
 replicate. * (adjacent column): average frequency for that temperature
 block (MHz). * Sheet: Fig3 C — Temperature-calibration summary table. *
 Variables (as labeled): * temp: temperature (°C). * Avg. Frequency [MHz]:
 average ODMR peak frequency (MHz). * Frequency [MHz] (per temperature
 columns): individual replicate peak frequencies (MHz). * Sheet: Fig.3D —
 Additional CW-ODMR spectrum with peak fit (as used in Fig. 3D). *
 Variables: Frequency [Hz]; ODMR data; ODMR peak fit. * Sheet: Fig3 E —
 Intracellular temperature-dependent peak-frequency replicates (block-form
 table). * Contents: repeated peak-frequency measurements grouped by
 temperature (°C) with adjacent average-frequency columns (as arranged in
 the sheet). * Variables: Frequency [MHz]; ODMR peak fit. * Sheet: Fig3 F —
 Intracellular temperature summary (temperature, average frequency, and
 replicate frequencies). * Variables (as labeled): * temperature:
 temperature (°C). * Average Frequency [MHz]: average ODMR peak frequency
 (MHz). * Frequency [MHz] (per temperature columns): individual replicate
 peak frequencies (MHz). * Sheet: Fig3 E F H I data — Underlying raw ODMR
 sweeps grouped by temperature/condition (block-form). * Variables (within
 each block, as labeled): Frequency [Hz]; CPS (counts per second). * Sheet:
 Fig3 G — Nanodiamond thermometry comparison summary (two temperature
 conditions). * Variables * temperature: temperature (°C). * Average
 Frequency [MHz]: average ODMR peak frequency (MHz). * Frequency [MHz] (per
 temperature columns). * Sheet: Fig3 G data — Underlying nanodiamond ODMR
 sweeps for Fig3G (block-form). * Variables (within each block, as
 labeled): Frequency [Hz]; CPS. * Sheet: Fig3 H — Medium temperature
 readings for two temperature conditions (columns labeled by temperature).
 * Variables: temperature (°C) per condition (as calculated from ODMR
 frequency). * Sheet: Fig3 I — Time-series of intracellular temperature
 estimates across multiple spots (with errors). * Variables: * time: time
 point/index (as labeled). * spot 1 … spot 4: temperature estimate per spot
 from ODMR spectrum (°C). * error/error.1 …: associated uncertainty from
 ODMR fit(°C). **Figure 4** — Absolute temperature sensing inside nuclei
 (organelle targeting/microinjection) * File: Fig4.xlsx * Sheet: Fig4 C —
 CW-ODMR sweep data used for panel C (no header row in sheet). * Variables:
 three columns as stored in the sheet (frequency/signal data as used for
 the figure). * Sheet: Fig4 D — Intranuclear spot temperatures over time
 (summary). * Variables: * (first column): time point (min; 10, 20, 60 as
 stored). * spot 1 / spot 2 / spot 3: temperature estimate (°C). * error:
 associated uncertainty (°C). * Sheet: Fig4 D data — Raw CW-ODMR sweeps for
 Fig4D grouped by time point and spot (block-form). * Variables (within
 each block, as labeled): Frequency [Hz]; CPS. * Sheet: Fig4 E —
 Cell-to-cell temperature distributions (summary; paired temp/error
 columns). * Variables (as labeled): temp; error (repeated across multiple
 spot columns). * Sheet: Fig4 E data — Raw CW-ODMR sweeps grouped by cell
 and spot (block-form). * Variables (within each block, as labeled):
 Frequency [Hz]; CPS. **Figure 5** — External spin detection (radicals) in
 cytoplasm and nucleus * File: Fig5.xlsx * Sheet: Fig5 B — Summary of
 fit-derived relaxation values vs TEMPOL concentration. * Variables: *
 10uM, 100uM, 1mM: per-replicate fit-derived values for each concentration
 (units as used in the sheet). * Sheet: Fig5 B data — Underlying decay
 traces for Fig5B (multiple replicates; block-form). * Variables (within
 each block, as labeled): tau [sec]; intensity. * Sheet: Fig5 C — Summary
 of fit-derived relaxation values including TEMPOL(−) control and TEMPOL
 conditions. * Variables: TEMPOL (−), 100uM, 1mM (per-replicate fit-derived
 values; units as used in sheet). * Sheet: Fig5 C data — Underlying decay
 traces for Fig5C (multiple replicates; block-form). * Variables (within
 each block, as labeled): tau [sec]; intensity. * Sheet: Fig5 E — Summary
 values before/after H2O2 treatment (paired columns). * Variables: Before
 H2O2; After H2O2 (per-replicate values; units as used in sheet). * Sheet:
 Fig5 E data — Underlying decay traces for Fig5E (block-form). * Variables
 (within each block, as labeled in sheet): tau [sec]; intensity. * Sheet:
 Fig5 F — Summary values before/after H2O2 treatment (paired columns). *
 Variables: Before H2O2; After H2O2 (per-replicate values; units as used in
 sheet). * Sheet: Fig5 F data — Underlying decay traces for Fig5F
 (block-form). * Variables (within each block, as labeled in sheet): tau
 [sec]; intensity. * Sheet: Fig5 H — Summary values before/after H2O2
 treatment (paired columns). * Variables: Before H2O2; After H2O2
 (per-replicate values; units as used in sheet). * Sheet: Fig5 H data —
 Underlying decay traces for Fig5H (block-form). * Variables (within each
 block, as labeled in sheet): tau [sec]; intensity. * Sheet: Fig5 I —
 Summary values before/after H2O2 treatment (paired columns). * Variables:
 Before H2O2; After H2O2 (per-replicate values; units as used in sheet). *
 Sheet: Fig5 I data — Underlying decay traces for Fig5I (block-form). *
 Variables (within each block, as labeled in sheet): tau [sec]; intensity.
 **Supplementary Figures (S1–S16)** **Figure S1** — Confocal scan and ODMR
 measurement of p-terphenyl particles * File: FigS1.xlsx * Sheet: FigS1 B —
 CW-ODMR spectrum of p-terphenyl (TP-only control). * Variables (as labeled
 in sheet): * Frequency: microwave frequency. * ODMR signal: ODMR
 intensity/counts (as acquired). **Figure S2** — Statistical analysis of
 CW-ODMR contrast * File: FigS2.xlsx * Sheet: FigS2 — Summary table of
 CW-ODMR contrast values (one value per particle/spot). * Variables: *
 200nm ND, 200nm MQN, 500nm ND, 500nm MQN: CW-ODMR contrast (%) for each
 sample type. * Sheet: FigS2 200nm ND / FigS2 500nm ND / FigS2 200nm MQN /
 FigS2 500nm MQN — CW-ODMR spectra used for the statistics (multiple
 particles). * Variables: * Frequency: microwave frequency (as labeled). *
 ODMR 1 … ODMR 10: ODMR spectra (intensity/contrast) for each
 particle/measurement index. **Figure S3** — Statistical analysis of pulsed
 ODMR measurements (Rabi, T1, T2) * File: FigS3.xlsx * Panel A (Rabi) *
 Sheet: FigS3 A — Summary of fit-derived Rabi contrast (grouped by sample
 type). * Variables: 200nm ND, 200nm MQN, 500nm ND, 500nm MQN (Rabi
 contrast per particle/measurement). * Sheet: FigS3 A 200nm MQN / FigS3 A
 500nm MQN / FigS3 A 200nm ND / FigS3 A 500nm ND — Rabi oscillation traces
 (multiple particles). * Variables: * Pulse length: microwave pulse length
 (as labeled). * rabi 1 … rabi 10: normalized contrast vs pulse length. *
 Panel B (T1) * Sheet: FigS3 B — Summary of fit-derived T1 values (grouped
 by sample type). * Variables: 200nm ND, 200nm MQN, 500nm ND, 500nm MQN (T1
 per particle/measurement). * Sheet: FigS3 B 200nm MQN / FigS3 B 500nm MQN
 / FigS3 B 200nm ND / FigS3 B 500nm ND — T1 decay traces (multiple
 particles). * Variables: * Relaxation Time [sec]: evolution/wait time. *
 T1 1 … / T1 1 data 1 … : normalized contrast vs time (labels as in sheet).
 * Panel C (T2) * Sheet: FigS3 C — Summary of fit-derived T2 values
 (grouped by sample type). * Variables: 200nm ND, 200nm MQN, 500nm ND,
 500nm MQN (T2 per particle/measurement). * Sheet: FigS3 C 200nm MQN /
 FigS3 C 500nm MQN / FigS3 C 200nm ND / FigS3 C 500nm ND — T2 decay traces
 (multiple particles). * Variables: * Free Evolution Time [sec]:
 free-evolution time. * T2 1 … / T2 1 data 1 … : normalized contrast vs
 time (labels as in sheet). **Figure S6** — Photon-count time traces and
 Allan deviation (intracellular dMQN) * File: FigS6.xlsx * Sheet: FigS6 A —
 Fluorescence photon-count time trace. * Variables: * time [s]: time (s). *
 photon counts per second [cps]: photon count rate (cps). * Sheet: FigS6 B
 — Power spectral density (PSD) analysis of relative intensity
 fluctuations. * Variables: * frequency [Hz]: frequency (Hz). * PSD data
 [arb. Units/Hz]: PSD of measured data. * PSD total [arb. Units/Hz]: total
 PSD model/fit. * PSD white [arb. Units/Hz]: white-noise component. * PSD
 1/f [arb. Units/Hz]: 1/f noise component. **Figure S7** — Microwave-power
 dependence of intracellular Rabi * File: FigS7.xlsx * Sheet: FigS7 —
 Intracellular Rabi oscillations at different microwave powers with fit
 curves. * Variables: * Pulse Length [s]: pulse length (as labeled). *
 rabi35dbm [normalized contrast], 35dbm fit [normalized contrast]: data and
 fit at 35 dBm. * rabi30dbm [normalized contrast], 30dbm fit [normalized
 contrast]: data and fit at 30 dBm. **Figure S8** — MALDI-TOF-MS (MQN vs
 dMQN; deuteration quantification) * File: FigS8.xlsx * Sheet: Fig.S8 A
 H-MQN — MALDI spectrum for H-MQN. * Variables: m/z; intensity [a.u.]. *
 Sheet: Fig.S8 B D-MQN — MALDI spectrum for D-MQN. * Variables: m/z;
 intensity [a.u.]. **Figure S9** — Absolute temperature-related
 measurements under different solution conditions * File: FigS9.xlsx *
 Sheet: FigS9 — Per-particle ODMR peak frequency under different solution
 conditions (summary). * Variables: * Particle number: particle/spot index.
 * NaCl / TEMPOL / pH4 / BSA 10%: condition labels (as shown). * Frequency
 [MHz]: ODMR peak frequency (MHz) for each condition. * Sheet: FigS9 data —
 Raw ODMR sweeps grouped by condition. * Variables (within each condition
 block, as labeled): * Frequency [Hz]: microwave frequency (Hz). * CPS:
 fluorescence intensity (counts per second). **Figure S10** — Minimal
 detection analysis using CW-ODMR (Allan deviation-based) * File:
 FigS10.xlsx * Sheet: FigS10 — Allan deviation–based sensitivity summary. *
 Variables: * tau_s: averaging time τ (s). * delta_B_uT: minimal detectable
 magnetic field (µT). * fit tau ^-1/2: τ^(-1/2) fit/reference scaling (as
 labeled). * Sheet: FigS10 data — Underlying CW-ODMR time-series/sweeps
 used for Allan analysis. * Variables: * time_s: time (s). * sweep_index:
 sweep number. * freq_index: index of frequency point within each sweep. *
 freq_MHz: microwave frequency (MHz). * intensity [cps]: fluorescence
 intensity (cps). **Figure S11** — DLS size distribution (aqueous
 dispersion) * File: FigS11.xlsx * Sheet: FigS11 — DLS size distribution. *
 Variables: * Diameter [nm]: hydrodynamic diameter (nm). * Number percent
 [%]: number-weighted percentage (%). **Figure S12** — Characterization of
 MQNs (SEM, UV–Vis, transient absorption kinetics) Normalization was
 performed by normalizing each trace to its highest intensity. * File:
 FigS12.xlsx * Sheet: FigS12 C normalized — UV–Vis absorption spectra
 (normalized). * Variables: wavelength [nm]; 200nmMQN; 500nmMQN; Bulk
 p-doped p-terphenyl (normalized absorbance [a.u.]). * Sheet: FigS12 C
 unnormalized — UV–Vis absorption spectra (unnormalized). * Variables:
 wavelength [nm]; 200nmMQN; 500nmMQN; Bulk p-doped p-terphenyl (absorbance
 [a.u.]). * Sheet: FigS12 D normalized — Transient absorption kinetics
 (normalized). * Variables: Time / µs; 200MQN; 500MQN (signal [a.u.]). *
 Sheet: FigS12 D unnormalized — Transient absorption kinetics
 (unnormalized). * Variables: Time / µs; 200MQN; 500MQN (signal [a.u.]).
 **Figure S13** — Size distribution histogram derived from SEM images *
 File: FigS13.xlsx * Sheet: FigS13A — Particle diameters extracted from SEM
 analysis (dataset A). * Variables: Diameter [nm] (one entry per particle).
 * Sheet: FigS13B — Particle diameters extracted from SEM analysis (dataset
 B). * Variables: Diameter [nm] (one entry per particle). **Figure S14** —
 Fluorescence lifetime measurements Normalization was performed by
 normalizing each trace to its highest intensity. * File: FigS14.xlsx *
 Sheet: FigS14 normalized — Fluorescence lifetime decay traces
 (normalized). * Variables (paired columns per trace, as labeled): * Time
 [ns]: time (ns). * Fluorescence [a.u.]: fluorescence intensity (a.u.). *
 Sheet: FigS14 unnormalized — Fluorescence lifetime decay traces
 (unnormalized). * Variables: same structure/labels as above. **Figure
 S15** — Time-resolved ESR decay (MQN200) * File: FigS15.xlsx * Sheet:
 FigS15 A analyzed spectra — Field-swept spectrum used for panel A. *
 Variables (as labeled in sheet): * Magnetic field [mT]: magnetic field
 axis. * Ems. | Abs.: trESR signal intensity (a.u.). * Sheet: FigS15 A
 fitting — Fit curve corresponding to panel A. * Variables: * Magnetic
 field [mT]: magnetic field axis (same units as above). * Ems. | Abs.:
 fitted trESR spectrum (a.u.). * Sheet: FigS15 A trESR raw — Raw time
 traces acquired at multiple magnetic-field points (used to build panel A).
 * Variables: * time [s]: acquisition time (s). * …
 mT: raw trESR signal trace for each field point (column
 headers include the corresponding magnetic field in mT). * Sheet: FigS15 B
 — Time-domain trESR decay traces shown in panel B. * Variables: * Time
 [µs]: time axis (µs). * Neg. | Pos.: trESR signal for negative/positive
 field positions (a.u.). **Figure S16** — Nanodiamond ODMR peak fitting /
 D-value estimation (Lorentzian fit) * File: FigS16.xlsx * Sheet: FigS16 —
 ODMR spectrum and peak fitting components. * Variables: * Frequency [Hz]:
 microwave frequency (as labeled). * odmr data contrast [a.u.]: measured
 ODMR contrast. * peak fit 1 [a.u.], peak fit 2 [a.u.]: fitted peak
 components. * odmr spectrum from fits [a.u.]: reconstructed spectrum from
 fitted components.