| Elemental analysis, C₃₃H₆₁O₈Y | Calculated: C, 58.74; H, 9.11; found: C, 58.49; H, 8.17 |
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Suma Al-Hunaishi, Senthil Kumar Kuppusamy, Yisheng Lei, Idris Tlemsani, Burak Gurlek, Jordan L. Appleton, Sergei Lebedkin, Alexandre Tallaire, Mario Ruben, Philippe Goldner, Diana Serrano. “Robust optical coherence in a chemically tunable Eu(III) molecular crystal.” ChemRxiv (). https://doi.org/10.26434/chemrxiv.15007936/v1
Values presented only in diffraction patterns, Raman spectra, photoluminescence spectra, excitation spectra, photon-echo decays, or other plots or images were not transcribed. The supporting information is appended to the main paper
| Elemental analysis, C₄₅H₆₅EuN₂O₆ | Calculated: C, 61.28; H, 7.43; N, 3.18; found: C, 61.03; H, 7.43; N, 3.16 |
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| Single-crystal X-ray diffraction | Triclinic space group P1̅, Z = 2; the Eu(III) ion had an O₆N₂ eight-coordinate environment; the shortest crystallographic metal–metal separation was 9.27 Å |
| Photoluminescence, 10 K | The ⁵D₀→⁷F₂ transition accounted for 72.99 % of the total integrated emission; the 580 nm ⁵D₀→⁷F₀ transition had an oscillator strength of 1.27 × 10⁻⁸ |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.778 ± 0.005 ms |
| Emission-spectrum and photoluminescence-decay analysis, 10 K | R(I₀→₂/I₀→₁): 11.03; Ω₂: 19.19 × 10⁻²⁰ cm²; Ω₄: 9.18 × 10⁻²⁰ cm²; observed lifetime: 0.780 ms; radiative decay rate: 801.81 s⁻¹; non-radiative decay rate: 483.54 s⁻¹; intrinsic Eu(III) quantum efficiency: 62.38 % |
| Two-pulse photon echo, 1.4 K | Homogeneous linewidth: 80 ± 2 kHz; optical coherence time, T₂: 4.06 ± 0.06 µs |
| Three-pulse photon echo, 1.4 K, sudden-jump spectral-diffusion fit | Short-waiting-time homogeneous linewidth: 91 ± 2 kHz; spectral-diffusion amplitude: 72 ± 8 kHz; fluctuation rate: 56 ± 16 kHz |
| Temperature-dependent two-pulse photon echo, fitted data | Extrapolated zero-temperature linewidth: 45 ± 8 kHz; TLS-like coefficient: 28 ± 6 kHz K⁻¹; LFM coefficient: 102 ± 74 MHz; effective LFM frequency: 462 ± 56 GHz |
| X-band EPR, powder, 4 K | No sizeable paramagnetic impurity signal was detected; a weak feature near g ≈ 2.1 was compatible with a trace Cu(II)-like contribution close to the noise level and could not be quantified reliably |
| Elemental analysis, C₄₅H₇₃EuN₂O₆ | Calculated: C, 60.73; H, 8.27; N, 3.15; found: C, 60.74; H, 7.38; N, 3.14 |
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| PXRD, Lorentzian peak fits and Scherrer analysis, K = 0.9, λ = 154.060 pm | Apparent domain size: 111 ± 2 nm for the (010) reflection at 2θ = 7.8° and 108 ± 2 nm for the (012) reflection at 2θ = 9.4° |
| Raman spectroscopy, 633 nm excitation | The spectrum remained globally similar to that of [Eu(TMHD)₃(phen)], although selected vibrational bands were shifted |
| Photoluminescence, 10 K | The same main transitions as in [Eu(TMHD)₃(phen)] were observed |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.790 ± 0.006 ms |
| Two-pulse photon echo, 1.4 K | Homogeneous linewidth: 74.4 ± 0.4 kHz; optical coherence time, T₂: 4.28 ± 0.02 µs |
| Three-pulse photon echo, 1.4 K, sudden-jump spectral-diffusion fit | Short-waiting-time homogeneous linewidth: 87 ± 1 kHz; spectral-diffusion amplitude: 88 ± 5 kHz; fluctuation rate: 22 ± 2 kHz |
| Temperature-dependent two-pulse photon echo, fitted data | Extrapolated zero-temperature linewidth: 39 ± 3 kHz; TLS-like coefficient: 22 ± 2 kHz K⁻¹; LFM coefficient fixed at 100 MHz; effective LFM frequency: 489 ± 6 GHz |
| Elemental analysis, C₄₅H₆₅Eu₀.₅N₂O₆Y₀.₅ | Calculated: C, 63.55; H, 7.70; N, 3.29; found: C, 63.43; H, 7.21; N, 3.22 |
|---|---|
| PXRD, Lorentzian peak fits and Scherrer analysis, K = 0.9, λ = 154.060 pm | Apparent domain size: 95 ± 1 nm for the (010) reflection at 2θ = 7.8° and 114 ± 4 nm for the (012) reflection at 2θ = 9.4° |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.773 ± 0.004 ms |
| Three-pulse photon echo, 1.4 K | No data of sufficient quality over a broad enough waiting-time range were obtained for reliable analysis |
| Elemental analysis, C₄₅H₆₅Eu₀.₂₅N₂O₆Y₀.₇₅ | Calculated: C, 64.75; H, 7.85; N, 3.36; found: C, 64.26; H, 7.81; N, 3.35 |
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| PXRD, Lorentzian peak fits and Scherrer analysis, K = 0.9, λ = 154.060 pm | Apparent domain size: 108 ± 2 nm for the (010) reflection at 2θ = 7.8° and 108 ± 2 nm for the (012) reflection at 2θ = 9.4° |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.769 ± 0.005 ms |
| Three-pulse photon echo, 1.4 K, sudden-jump spectral-diffusion fit | Short-waiting-time homogeneous linewidth: 112 ± 3 kHz; spectral-diffusion amplitude: greater than 500 kHz, reported as a lower bound; fluctuation rate: 4.6 ± 0.7 kHz |
| Elemental analysis, C₄₅H₆₅Eu₀.₁N₂O₆Y₀.₉ | Calculated: C, 65.5; H, 7.94; N, 3.39; found: C, 65.61; H, 7.99; N, 3.39 |
|---|---|
| PXRD, Lorentzian peak fits and Scherrer analysis, K = 0.9, λ = 154.060 pm | Apparent domain size: 91 ± 1 nm for the (010) reflection at 2θ = 7.8° and 96 ± 1 nm for the (012) reflection at 2θ = 9.4° |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.787 ± 0.006 ms |
| Three-pulse photon echo, 1.4 K, sudden-jump spectral-diffusion fit | Short-waiting-time homogeneous linewidth: 63 ± 1 kHz; spectral-diffusion amplitude: 220 ± 21 kHz; fluctuation rate: 5 ± 1 kHz |
| Temperature-dependent two-pulse photon echo, fitted data | Extrapolated zero-temperature linewidth: 46 ± 5 kHz; TLS-like coefficient: 7 ± 3 kHz K⁻¹; LFM coefficient fixed at 100 MHz; effective LFM frequency: 446 ± 5 GHz |
| Elemental analysis, C₄₅H₆₅Eu₀.₀₅N₂O₆Y₀.₉₅ | Calculated: C, 65.75; H, 7.97; N, 3.41; found: C, 65.70; H, 7.99; N, 3.38 |
|---|---|
| PXRD, Lorentzian peak fits and Scherrer analysis, K = 0.9, λ = 154.060 pm | Apparent domain size: 97 ± 1 nm for the (010) reflection at 2θ = 7.8° and 93 ± 2 nm for the (012) reflection at 2θ = 9.4° |
| Photoluminescence decay, 10 K, single-exponential fit | Lifetime: 0.801 ± 0.004 ms |
| Three-pulse photon echo, 1.4 K, sudden-jump spectral-diffusion fit | Short-waiting-time homogeneous linewidth: 99 ± 4 kHz; spectral-diffusion amplitude: 121 ± 25 kHz; fluctuation rate: 30 ± 10 kHz |
| Elemental analysis, C₄₅H₆₅N₂O₆Y | Calculated: C, 66.00; H, 8.00; N, 3.42; found: C, 65.76; H, 7.6; N, 3.33 |
|---|---|
| X-band EPR, powder, 4 K | No sizeable paramagnetic impurity signal was detected; a weak feature near g ≈ 2.1 was compatible with a trace Cu(II)-like contribution close to the noise level and could not be quantified reliably |
| PXRD | The diffraction profiles were globally preserved across the series |
|---|---|
| Raman spectroscopy, 633 nm excitation | The main Raman features were preserved across the dilution series; sample-dependent relative-intensity changes were observed, including in the approximately 1650 cm⁻¹ region |
| Low-frequency Raman spectroscopy, 633 nm excitation | The main spectral features remained broadly similar, while sample-to-sample relative-intensity changes were observed; at approximately 15 K, the main room-temperature bands of the 100 % Eu and 100 % Eu–D samples generally split into patterns of sharp peaks with linewidths comparable to the approximately 2 cm⁻¹ spectral resolution |
| Photoluminescence, approximately 10 K | The same overall emission profile was observed across the concentration range; emission was dominated by the ⁵D₀→⁷F₂ transition around 612 nm |