Stochastic Models for Non-Linear/Many-Body Dynamics in Molecular Semiconductors

分子半导体中非线性/多体动力学的随机模型

• 批准号: 2102506
• 负责人: Eric Bittner
• 金额: $ 45万
• 依托单位: University of Houston
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-06-01 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102506&HistoricalAwards=false
• 关键词: Stochastic; Models; Non; Linear; Many

Professor Eric Bittner of the University of Houston is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry. to model dark background dynamics that contribute to dephasing and spectral diffusion in complex semiconducting systems as revealed in coherent multi-dimensional spectroscopy. This work aims to facilitate the next significant breakthroughs in fundamental aspects of coherent non-linear spectroscopy as applied to condensed-matter physics, materials science, and ultimately, in quantum optoelectronic technologies in a broader context. The optimal choice of materials for such novel technologies relies on a profound understanding of correlated many-body dynamics as manifest in multi-dimensional spectral probes. This project develops key aspects of Quantum Leap by exploiting quantum entanglement of photons to unravel underpinning many-body correlations and hidden-layer dynamics.Spectroscopic line-shapes reveal a wealth of information concerning the underlying background dynamics a system is experiencing. In this project, Bittner proposes the use of quantum stochastic equations and Ito calculus to model dark background dynamics that contribute to dephasing and spectral diffusion in complex semiconducting systems as revealed in coherent multi-dimensional spectroscopy. Theoretical advances include the use of correlated noise and non-commutative noise to model the influence of various background environments on spectroscopic signals. Proposed applications of the work include exciton and bi-exciton dynamics in hybrid organic/inorganic layered semiconductors, semiconducting organic polymers, and DNA-wrapped Carbon nanorods. The work advances the notion that exciton dynamics can be cross-correlated via hidden-layer background processes. Bittner seeks to quantify these as manifest in 2D coherent non-linear spectroscopic signals. The work also advances the use of quantum entangled photons as a probe of many-body dynamics. Previous studies suggest that entanglement can be generated via indirect coupling of emitters to a common or correlated environment. Bittner will explore this idea with the goal developing novel quantum spectroscopies and/or generation of custom entanglements.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

休斯顿大学的Eric Bittner教授得到了化学系化学理论、模型和计算方法项目的支持。对在相干多维光谱学中揭示的复杂半导体系统中有助于退相和光谱扩散的暗背景动力学进行建模。这项工作旨在促进相干非线性光谱学在凝聚态物理、材料科学以及最终在更广泛的背景下应用于量子光电子技术的基本方面的下一个重大突破。对于这种新技术，材料的最佳选择依赖于对相关多体动力学的深刻理解，这在多维光谱探测器中可见一斑。这个项目通过利用光子的量子纠缠来揭示支撑多体关联和隐藏层动力学的基础，从而开发了量子跃迁的关键方面。光谱线形揭示了关于系统正在经历的潜在背景动力学的丰富信息。在这个项目中，Bittner建议使用量子随机方程和Ito微积分来模拟暗背景动力学，这些动力学有助于相干多维光谱中揭示的复杂半导体系统的退相和光谱扩散。理论上的进展包括使用相关噪声和非对易噪声来模拟各种背景环境对光谱信号的影响。这项工作的拟议应用包括有机/无机混合层状半导体、半导体有机聚合物和DNA包裹的碳纳米棒中的激子和双激子动力学。这项工作提出了激子动力学可以通过隐藏的背景过程相互关联的概念。Bittner试图量化这些在2D相干非线性光谱信号中的表现。这项工作还推进了量子纠缠光子作为多体动力学探测器的使用。以前的研究表明，纠缠可以通过发射体与公共或相关环境的间接耦合来产生。比特纳将探索这一想法，目标是开发新的量子光谱和/或产生定制纠缠。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Stochastic scattering theory for excitation-induced dephasing: Comparison to the Anderson–Kubo lineshape

激励引起相移的随机散射理论：与 Anderson-Kubo 线形的比较

• DOI: 10.1063/5.0026467
• 发表时间: 2020
• 期刊: The Journal of Chemical Physics
• 作者: Li, Hao;Srimath Kandada, Ajay Ram;Silva, Carlos;Bittner, Eric R.
• 通讯作者: Bittner, Eric R.

Stochastic exciton-scattering theory of optical line shapes: Renormalized many-body contributions

光线形状的随机激子散射理论：重正化多体贡献

• DOI: 10.1063/5.0095575
• 发表时间: 2022
• 期刊: The Journal of Chemical Physics
• 作者: Li, Hao;Shah, S. A.;Bittner, Eric R.;Piryatinski, Andrei;Silva-Acuña, Carlos
• 通讯作者: Silva-Acuña, Carlos

The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering

多体激子散射中随机过程的光学特征

• DOI: 10.1146/annurev-physchem-102822-100922
• 发表时间: 2023
• 期刊: Annual Review of Physical Chemistry
• 影响因子: 14.7
• 作者: Li, Hao;Shah, S.A.;Srimath Kandada, Ajay Ram;Silva, Carlos;Piryatinski, Andrei;Bittner, Eric R.
• 通讯作者: Bittner, Eric R.

Quantum Light Emission from Coupled Defect States in DNA-Functionalized Carbon Nanotubes

• DOI: 10.1021/acsnano.1c02709
• 发表时间: 2021-06-01
• 期刊: ACS NANO
• 影响因子: 17.1
• 作者: Zheng, Yu;Kim, Younghee;Htoon, Han
• 通讯作者: Htoon, Han