Guest-dependent T 2 of DAT triplets in D-MIL-53. a, Spin echo sequence used for T2 measurement. The intervals of microwave pulses and echo detection were varied. b, Plot of T2 obtained by the single-exponential fitting of the spin echo decay curves against the unit cell volume of MIL-53. Only the T2 obtained from the low field peaks where the effect of ESEEM was small is plotted. c, Spin echo decay curves after pulsed photoexcitation at 532 nm for empty (D-MIL-53⸧DAT) and guest-filled (D-MIL-53⸧[DAT+guest]) samples at room temperature. The decay curves of each sample at the magnetic field corresponding to the higher and lower EPR peaks (Fig. 3a) are shown at the top and bottom, respectively. Single-exponential fitting curves for each sample are also shown. Echo signals were not observed when the guest was h-Tol, EtOH, or AcNt.

Guest-dependent T 2 of DAT triplets in D-MIL-53. a, Spin echo sequence used for T2 measurement. The intervals of microwave pulses and echo detection were varied. b, Plot of T2 obtained by the single-exponential fitting of the spin echo decay curves against the unit cell volume of MIL-53. Only the T2 obtained from the low field peaks where the effect of ESEEM was small is plotted. c, Spin echo decay curves after pulsed photoexcitation at 532 nm for empty (D-MIL-53⸧DAT) and guest-filled (D-MIL-53⸧[DAT+guest]) samples at room temperature. The decay curves of each sample at the magnetic field corresponding to the higher and lower EPR peaks (Fig. 3a) are shown at the top and bottom, respectively. Single-exponential fitting curves for each sample are also shown. Echo signals were not observed when the guest was h-Tol, EtOH, or AcNt.

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Quantum sensing using molecular qubits is expected to provide excellent sensitivity due to the proximity of the sensor to the target analyte. However, many molecular qubits are used at cryogenic temperatures, and how to make molecular qubits respond to specific analytes remains unclear. Here, we propose a new quantum sensor design in which the cohe...

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Context 1
... coherence time (T 2 ). The coherence times (T2) of the photoexcited triplets of DAT in D-MIL-53 were measured by pulsed EPR at room temperature with a spin echo sequence varying the pulse intervals ( Fig. 2a). Measurements were taken at the magnetic field of the high-field and low-field peaks of the EPR spectra shown later, respectively, and both decay curves are shown (Fig. 2c). The decay of echo intensity was fitted with a single exponential function and T2 was obtained as the decay constant. While DAT shows electron spin echo envelope ...
Context 2
... The coherence times (T2) of the photoexcited triplets of DAT in D-MIL-53 were measured by pulsed EPR at room temperature with a spin echo sequence varying the pulse intervals ( Fig. 2a). Measurements were taken at the magnetic field of the high-field and low-field peaks of the EPR spectra shown later, respectively, and both decay curves are shown (Fig. 2c). The decay of echo intensity was fitted with a single exponential function and T2 was obtained as the decay constant. While DAT shows electron spin echo envelope modulation (ESEEM) due to hyperfine coupling with 1 H nuclei and 14 N nuclei at higher magnetic field, it does not affect the estimation of T2. The T2 values obtained at the ...
Context 3
... T2 value was plotted against the cell volume of MIL-53 ( Fig. 2b). With increasing cell volume, T2 shows a non-monotonic trend, becoming longer and then shorter. Triplet qubit and flexible MOF hybrids exhibit different coherence times for various guest molecules, enabling room-temperature quantum chemical sensing of neutral molecules that has not been reported previously. b, Plot of T2 obtained by ...
Context 4
... immediately absorbs water and forms a hydrated structure), DAT shows absorption peaks at 450, 480, and 515 nm derived from π-π* transitions. This is consistent with the absorption peaks of DAT molecularly dispersed in p-terphenyl and is clearly different from the red-shifted peaks of DAT in its aggregated solid state, as we previously reported 32 (Fig. S2). With the exception of BQ, where the guest itself shows absorption, no significant change in the absorption spectrum is observed when various guest molecules are introduced (Fig. S3). This indicates that the interaction between DAT and the guest molecules is small in the ground state and that DAT is not aggregated by the introduction ...

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Citations

... For the poten al of chemical quantum sensing, the interac ons between adsorbed guest molecules and qubits can be understood by es ma ng relaxa on me and hyperfine interac ons with electron spin resonance (ESR) measurements. 9,20 We have previously reported that MOFs consis ng of pyridylmodified 5,12-diazatetracene (DAT) ligands (DPyDAT) and Zn ions undergo charge separa on from the photo-excited DAT chromophore, and that the resul ng DAT radicals exhibit rela vely long coherence mes T 2 . 21,24 However, due to the instability of the MOF structure, the response of T 2 to various guest molecules could not be evaluated. ...
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Molecular electronic spin qubits are promising candidates for quantum information science applications because they can be reliably produced and engineered via chemical design. Embedding electronic spin qubits within two-dimensional polymers (2DPs) offers the possibility to systematically engineer inter-qubit interactions while maintaining long coherence times, both of which are prerequisites to their technological utility. Here, we introduce electronic spin qubits into a diamagnetic 2DP by n-doping naphthalene diimide subunits with varying amounts of CoCp2 and analyze their spin densities by quantitative electronic paramagnetic resonance spectroscopy. Low spin densities (e.g., 6.0 × 1012 spins mm-3) enable lengthy spin-lattice (T1) and spin-spin relaxation (T2) times across a range of temperatures, ranging from T1 values of 164 ms at 10 K to 30.2 μs at 296 K and T2 values of 2.36 μs at 10 K to 0.49 μs at 296 K for the lowest spin density sample examined. Higher spin densities and temperatures were both found to diminish T1 times, which we attribute to detrimental cross-relaxation from spin-spin dipolar interactions and spin-phonon coupling, respectively. Higher spin densities decreased T2 times and modulated the T2 temperature dependence. We attribute these differences to the competition between hyperfine and dipolar interactions for electron spin decoherence, with the dominant interaction transitioning from the former to the latter as spin density and temperature increase. Overall, this investigation demonstrates that dispersing electronic spin qubits within layered 2DPs enables chemical control of their inter-qubit interactions and spin decoherence times.