Multiphonon Relaxation in Molecular Lanthanoid Luminescence

分子镧系元素发光中的多声子弛豫

基本信息

项目摘要

Non-radiative deactivation of excited levels in molecular compounds by the interaction of electronic states and vibrational overtones (= multiphonon relaxation, MR) is one of the most fundamental phenomena in the photophysics of light-emitting systems. One of the most interesting class of luminophores that are severely hampered by MR via anharmonic, high-energy oscillators are molecular lanthanoid complexes that emit in the near-infrared region of the spectrum (ca. 650-2000 nm). A detailed empirical and theoretical understanding of the intricacies determining MR in these species is still in its very infancy despite of the great technological potential of near-IR luminescence in areas like biomedical imaging or optical telecommunication. The current proposal aims at alleviating this situation by developing a comprehensive understanding of MR in molecular lanthanoid luminescence. The key enabling methodology for its realization is the organic synthesis of stereochemically well defined lanthanoid complexes which are systematically labeled with heavier isotopes (e.g. C-D instead of C-H). These tailor-made, isotopologic model systems allow the quantification of critical parameters for MR induced by typical structural motifs in the ligands. In particular, the project entails the determinations of the 3D complex structures in solution (paramagnetic 1H NMR), the non-radiative deactivation rates (time-resolved luminescence spectroscopy) and the vibrational overtone properties (near-IR absorption spectroscopy) of various coupled oscillator fragments, followed by integration of all empirical data under the known theoretical framework of the inductive-resonant mechanism of non-radiative transitions. The desired groundbreaking, unified understanding of MR for high-energy, anharmonic oscillators would go far beyond the current state-of-the-art and complement the well-known energy gap law for harmonic, low-energy oscillators in all areas of molecular photophysics.
由电子态和振动泛音相互作用引起的分子化合物激发态的非辐射失活(多声子弛豫,MR)是发光系统光物理中最基本的现象之一。最有趣的一类发光团是在光谱的近红外区域(约650-2000 nm)发射的分子类镧络合物,它通过非谐波高能振荡器受到MR的严重阻碍。尽管近红外发光在生物医学成像或光学通信等领域具有巨大的技术潜力,但对这些物种中确定MR的复杂性的详细经验和理论理解仍处于起步阶段。目前的建议旨在通过发展对分子镧系发光的MR的全面理解来缓解这种情况。实现这一目标的关键方法是有机合成立体化学定义明确的类镧配合物,这些配合物系统地标记为较重的同位素(例如C-D而不是C-H)。这些量身定制的同位素模型系统可以量化配体中典型结构基序诱导MR的关键参数。特别是,该项目需要确定溶液中的三维复杂结构(顺磁1H NMR),非辐射失活率(时间分辨发光光谱)和各种耦合振荡器片段的振动泛音特性(近红外吸收光谱),然后在已知的非辐射跃迁感应共振机制的理论框架下整合所有经验数据。对高能、非谐振子的磁共振的突破性的、统一的理解将远远超出目前最先进的水平,并补充分子光物理所有领域中众所周知的谐振、低能振子的能隙定律。

项目成果

期刊论文数量(6)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
专利数量(0)
Breakdown of the energy gap law in molecular lanthanoid luminescence: the smallest energy gap is not universally relevant for nonradiative deactivation.
  • DOI:
    10.1021/ic500017a
  • 发表时间:
    2014-03
  • 期刊:
  • 影响因子:
    4.6
  • 作者:
    Christine Doffek;Jessica Wahsner;Elisabeth Kreidt;Michael Seitz
  • 通讯作者:
    Christine Doffek;Jessica Wahsner;Elisabeth Kreidt;Michael Seitz
Deuterated Molecular Ruby with Record Luminescence Quantum Yield.
  • DOI:
    10.1002/anie.201711350
  • 发表时间:
    2018-01
  • 期刊:
  • 影响因子:
    0
  • 作者:
    Cui Wang;Sven Otto;Matthias Dorn;Elisabeth Kreidt;Jakob Lebon;L. Sršan;Patrick Di Martino‐Fumo;M. Gerhards;U. Resch‐Genger;Michael Seitz;K. Heinze
  • 通讯作者:
    Cui Wang;Sven Otto;Matthias Dorn;Elisabeth Kreidt;Jakob Lebon;L. Sršan;Patrick Di Martino‐Fumo;M. Gerhards;U. Resch‐Genger;Michael Seitz;K. Heinze
Nonradiative Deactivation of Lanthanoid Excited States by Inner-Sphere Carboxylates.
内层羧酸盐对镧系元素激发态的非辐射失活
  • DOI:
    10.1021/acs.inorgchem.5b01920
  • 发表时间:
    2015
  • 期刊:
  • 影响因子:
    4.6
  • 作者:
    J. Wahsner;M. Seitz
  • 通讯作者:
    M. Seitz
{{ item.title }}
{{ item.translation_title }}
  • DOI:
    {{ item.doi }}
  • 发表时间:
    {{ item.publish_year }}
  • 期刊:
  • 影响因子:
    {{ item.factor }}
  • 作者:
    {{ item.authors }}
  • 通讯作者:
    {{ item.author }}

数据更新时间:{{ journalArticles.updateTime }}

{{ item.title }}
  • 作者:
    {{ item.author }}

数据更新时间:{{ monograph.updateTime }}

{{ item.title }}
  • 作者:
    {{ item.author }}

数据更新时间:{{ sciAawards.updateTime }}

{{ item.title }}
  • 作者:
    {{ item.author }}

数据更新时间:{{ conferencePapers.updateTime }}

{{ item.title }}
  • 作者:
    {{ item.author }}

数据更新时间:{{ patent.updateTime }}

Professor Dr. Michael Seitz其他文献

Professor Dr. Michael Seitz的其他文献

{{ item.title }}
{{ item.translation_title }}
  • DOI:
    {{ item.doi }}
  • 发表时间:
    {{ item.publish_year }}
  • 期刊:
  • 影响因子:
    {{ item.factor }}
  • 作者:
    {{ item.authors }}
  • 通讯作者:
    {{ item.author }}

{{ truncateString('Professor Dr. Michael Seitz', 18)}}的其他基金

Directed Energy Transfer in Luminescent Coordination Networks
发光协调网络中的定向能量转移
  • 批准号:
    316590317
  • 财政年份:
    2016
  • 资助金额:
    --
  • 项目类别:
    Priority Programmes
Multiphonon Relaxation in Molecular Lanthanoid Luminescence
分子镧系元素发光中的多声子弛豫
  • 批准号:
    256008545
  • 财政年份:
    2014
  • 资助金额:
    --
  • 项目类别:
    Heisenberg Fellowships
Universell vernetzbare Metallkomplex-Bausteine und ihre Anwendung
通用可联网金属复合积木及其应用
  • 批准号:
    94778992
  • 财政年份:
    2009
  • 资助金额:
    --
  • 项目类别:
    Independent Junior Research Groups
Chirale Lanthanoid-Komplexe in wäßriger Lösung - Hocheffiziente Sonden für Zirkular-polarisierte Lumineszenz
水溶液中的手性镧系元素配合物 - 用于圆偏振发光的高效探针
  • 批准号:
    5453370
  • 财政年份:
    2005
  • 资助金额:
    --
  • 项目类别:
    Research Fellowships

相似海外基金

Molecular Radiative and Relaxation Processes
分子辐射和弛豫过程
  • 批准号:
    2246379
  • 财政年份:
    2023
  • 资助金额:
    --
  • 项目类别:
    Continuing Grant
Local structure relaxation and non-equilibrium phase transition in dynamic facilitation of self-propelled complex molecular systems
自驱动复杂分子系统动态促进中的局部结构弛豫和非平衡相变
  • 批准号:
    23K03246
  • 财政年份:
    2023
  • 资助金额:
    --
  • 项目类别:
    Grant-in-Aid for Scientific Research (C)
Molecular Dynamics of Associative Polymers and Its Experimental Validation: Effect of Dissociation Equilibrium on Entanglement Relaxation Modes
缔合聚合物的分子动力学及其实验验证:解离平衡对缠结弛豫模式的影响
  • 批准号:
    21H01986
  • 财政年份:
    2021
  • 资助金额:
    --
  • 项目类别:
    Grant-in-Aid for Scientific Research (B)
Molecular Radiative and Relaxation Processes
分子辐射和弛豫过程
  • 批准号:
    1953045
  • 财政年份:
    2020
  • 资助金额:
    --
  • 项目类别:
    Continuing Grant
Fast Algorithm for Interface Relaxation and Efficient Computational Modeling of Molecular Binding and Unbinding
界面松弛的快速算法以及分子结合和解离的高效计算模型
  • 批准号:
    1913144
  • 财政年份:
    2019
  • 资助金额:
    --
  • 项目类别:
    Standard Grant
Ultrafast Dynamics of Ionic Liquids: Understanding of Molecular Level Aspects of Transition from Intermolecular Vibration to Structural Relaxation
离子液体的超快动力学:理解从分子间振动到结构弛豫转变的分子水平
  • 批准号:
    18J12979
  • 财政年份:
    2018
  • 资助金额:
    --
  • 项目类别:
    Grant-in-Aid for JSPS Fellows
Roles of molecular complex of IKs channel in plasma membrane depolarization - relaxation coupling in cardiac myocytes
IKs通道分子复合物在心肌细胞质膜去极化-弛豫耦合中的作用
  • 批准号:
    18K06683
  • 财政年份:
    2018
  • 资助金额:
    --
  • 项目类别:
    Grant-in-Aid for Scientific Research (C)
Dynamics of arrested relaxation in molecular ultracold plasmas
分子超冷等离子体中的阻滞弛豫动力学
  • 批准号:
    513032-2017
  • 财政年份:
    2017
  • 资助金额:
    --
  • 项目类别:
    University Undergraduate Student Research Awards
OP-Molecular Radiative and Relaxation Processes
OP-分子辐射和弛豫过程
  • 批准号:
    1663822
  • 财政年份:
    2017
  • 资助金额:
    --
  • 项目类别:
    Continuing Grant
Molecular Radiative and Relaxation Processes
分子辐射和弛豫过程
  • 批准号:
    1361516
  • 财政年份:
    2014
  • 资助金额:
    --
  • 项目类别:
    Continuing Grant
{{ showInfoDetail.title }}

作者:{{ showInfoDetail.author }}

知道了