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<p>Examples of molecular complexes acting as thermometers operating at room temperature in near infrared region are scarce, therefore this work showcases the anti-thermal quenching effect on neodymium(III) molecular thermometers working in biological windows within the physiological temperature range. A mononuclear complex, [Nd(L)(NO<sub>3</sub>)<sub>3</sub>] (<b>1Nd</b>), where L is a macrocyclic ligand, was synthesized and used as a precursor to develop two novel species: a dinuclear, [(Nd(L)(NO<sub>3</sub>))<sub>2</sub>(µ-BDC)](NO<sub>3</sub>)<sub>2</sub>·H<sub>2</sub>O (<b>2Nd</b>), linked by 1,4-benzenedicarboxylate (BDC), and a hexameric, [(Nd(L))(µ-BTC)(H<sub>2</sub>O)]<sub>6</sub>·35H<sub>2</sub>O (<b>6Nd</b>), linked with 1,3,5-benzenetricarboxylate (BTC). Thermometric properties were studied in the physiological temperature range (292-332 K), utilizing 804 nm laser excitation (first biological window) and monitoring emissions in the second biological window (908, 1065, and 1340 nm) associated with the <sup>4</sup>F<sub>3/2</sub> → <sup>4</sup>I<sub>9/2</sub>, <sup>4</sup>I<sub>11/2</sub>, <sup>4</sup>I<sub>13/2</sub> transitions, respectively. Among the complexes, the hexamer <b>6Nd</b> exhibited exceptional performance, with <i>S</i><sub><i>r</i></sub> of 2.4%K<sup>−1</sup> at 293 K, when luminescence intensity ratio (LIR) of two Stark components of the <sup>4</sup>F<sub>3/2</sub> → <sup>4</sup>I<sub>11/2</sub> emission was used, positioning it as a high-performance Nd<sup>III</sup>-based thermometer. All complexes displayed anti-thermal quenching behavior, surpassing the current molecular-based thermometers in the near-infrared region. Theoretical calculations using complete active space self consistent field (CASSCF) and Boltzmann population models between Kramers doublets of the <sup>4</sup>F<sub>3/2</sub> level were performed to rationalize the anti-thermal behavior.</p><p></p>

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Anti-thermal quenching in NdIII molecular near-infrared thermometers operating at physiological temperatures

  • 期刊论文

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  • 发表日期：

    2025年5月3日

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  • María José Maldonado,
  • Patricia Farías-Carreño,
  • Yolimar Gil,
  • Andrés Vega,
  • Ricardo Costa de Santana,
  • Daniel Aravena,
  • Carlos D. S. Brites,
  • Luís D. Carlos,
  • Albano N. Carneiro Neto,
  • Fiorenzo Vetrone,
  • Pablo Fuentealba

摘要

Examples of molecular complexes acting as thermometers operating at room temperature in near infrared region are scarce, therefore this work showcases the anti-thermal quenching effect on neodymium(III) molecular thermometers working in biological windows within the physiological temperature range. A mononuclear complex, [Nd(L)(NO3)3] (1Nd), where L is a macrocyclic ligand, was synthesized and used as a precursor to develop two novel species: a dinuclear, [(Nd(L)(NO3))2(µ-BDC)](NO3)2·H2O (2Nd), linked by 1,4-benzenedicarboxylate (BDC), and a hexameric, [(Nd(L))(µ-BTC)(H2O)]6·35H2O (6Nd), linked with 1,3,5-benzenetricarboxylate (BTC). Thermometric properties were studied in the physiological temperature range (292-332 K), utilizing 804 nm laser excitation (first biological window) and monitoring emissions in the second biological window (908, 1065, and 1340 nm) associated with the 4F3/2 → 4I9/2, 4I11/2, 4I13/2 transitions, respectively. Among the complexes, the hexamer 6Nd exhibited exceptional performance, with Sr of 2.4%K−1 at 293 K, when luminescence intensity ratio (LIR) of two Stark components of the 4F3/2 → 4I11/2 emission was used, positioning it as a high-performance NdIII-based thermometer. All complexes displayed anti-thermal quenching behavior, surpassing the current molecular-based thermometers in the near-infrared region. Theoretical calculations using complete active space self consistent field (CASSCF) and Boltzmann population models between Kramers doublets of the 4F3/2 level were performed to rationalize the anti-thermal behavior.