Project description:Interparticle energy transfer offers great promise to a diverse range of applications ranging from artificial solar energy harvesting to nanoscale rulers in biology. Here, we assembled InP/ZnS core/shell quantum dot monolayers via the Langmuir-Blodgett technique and studied the effect of ZnS shell thickness on the excitonic energy transfer within these core/shell quantum dots. Three types of InP-based core/shell quantum dot Langmuir-Blodgett assemblies with different ZnS shell thicknesses were assembled. The structural and optical properties of colloidal quantum dots reveal the successful multiple ZnS shell growth, and atomic force microscopy studies show the smoothness of the assembled monolayers. Time-resolved photoluminescence (PL) and fluorescence lifetime imaging microscopy (FLIM) studies of the thick-shell QD monolayer reveal narrower lifetime distribution in comparison with the thin-shell QD monolayer. The interparticle excitonic energy transfer was studied by spectrally resolved PL traces, and higher energy transfer was observed for the thin-shell InP/1ZnS QD monolayer. Finally, we calculated the average exciton energy and indicated that the energy transfer induced exciton energy shift decreased significantly from 95 to 27 meV after multiple ZnS shell growth.
Project description:DNA nanotechnology has now enabled the self-assembly of almost any prescribed 3-dimensional nanoscale structure in large numbers and with high fidelity. These structures are also amenable to site-specific modification with a variety of small molecules ranging from drugs to reporter dyes. Beyond obvious application in biotechnology, such DNA structures are being pursued as programmable nanoscale optical breadboards where multiple different/identical fluorophores can be positioned with sub-nanometer resolution in a manner designed to allow them to engage in multistep excitonic energy-transfer (ET) via Förster resonance energy transfer (FRET) or other related processes. Not only is the ability to create such complex optical structures unique, more importantly, the ability to rapidly redesign and prototype almost all structural and optical analogues in a massively parallel format allows for deep insight into the underlying photophysical processes. Dynamic DNA structures further provide the unparalleled capability to reconfigure a DNA scaffold on the fly in situ and thus switch between ET pathways within a given assembly, actively change its properties, and even repeatedly toggle between two states such as on/off. Here, we review progress in developing these composite materials for potential applications that include artificial light harvesting, smart sensors, nanoactuators, optical barcoding, bioprobes, cryptography, computing, charge conversion, and theranostics to even new forms of optical data storage. Along with an introduction into the DNA scaffolding itself, the diverse fluorophores utilized in these structures, their incorporation chemistry, and the photophysical processes they are designed to exploit, we highlight the evolution of DNA architectures implemented in the pursuit of increased transfer efficiency and the key lessons about ET learned from each iteration. We also focus on recent and growing efforts to exploit DNA as a scaffold for assembling molecular dye aggregates that host delocalized excitons as a test bed for creating excitonic circuits and accessing other quantum-like optical phenomena. We conclude with an outlook on what is still required to transition these materials from a research pursuit to application specific prototypes and beyond.
Project description:Understanding the relationship between the structure of light-harvesting systems and their excitation energy transfer properties is of fundamental importance in many applications including the development of next generation photovoltaics. Natural light harvesting in photosynthesis shows remarkable excitation energy transfer properties, which suggests that pigment-protein complexes could serve as blueprints for the design of nature inspired devices. Mechanistic insights into energy transport dynamics can be gained by leveraging numerically involved propagation schemes such as the hierarchical equations of motion (HEOM). Solving these equations, however, is computationally costly due to the adverse scaling with the number of pigments. Therefore virtual high-throughput screening, which has become a powerful tool in material discovery, is less readily applicable for the search of novel excitonic devices. We propose the use of artificial neural networks to bypass the computational limitations of established techniques for exploring the structure-dynamics relation in excitonic systems. Once trained, our neural networks reduce computational costs by several orders of magnitudes. Our predicted transfer times and transfer efficiencies exhibit similar or even higher accuracies than frequently used approximate methods such as secular Redfield theory.
Project description:Quantum Zeno effect shows that frequent observations can slow down or even stop the unitary time evolution of an unstable quantum system. This effect can also be regarded as a physical consequence of the statistical indistinguishability of neighboring quantum states. The accessibility of quantum Zeno dynamics under unitary time evolution can be quantitatively estimated by quantum Zeno time in terms of Fisher information. In this work, we investigate the accessibility of quantum Zeno dynamics in quantum open systems by calculating noisy Fisher information when a trace preserving and completely positive map is assumed. We firstly study the consequences of non-Markovian noise on quantum Zeno effect and give the exact forms of the dissipative Fisher information and the quantum Zeno time. Then, for the operator-sum representation, an achievable upper bound of the quantum Zeno time is given with the help of the results in noisy quantum metrology. It is of significance that the noise reducing the accuracy in the entanglement-enhanced parameter estimation can conversely be favorable for the accessibility of quantum Zeno dynamics of entangled states.
Project description:The creation and manipulation of quantum superpositions is a fundamental goal for the development of materials with novel optoelectronic properties. In this letter, we report persistent (~80 fs lifetime) quantum coherence between the 1S and 1P excitonic states in zinc-blende colloidal CdSe quantum dots at room temperature, measured using Two-Dimensional Electronic Spectroscopy. We demonstrate that this quantum coherence manifests as an intradot phenomenon, the frequency of which depends on the size of the dot excited within the ensemble of QDs. We model the lifetime of the coherence and demonstrate that correlated interexcitonic fluctuations preserve relative phase between excitonic states. These observations suggest an avenue for engineering long-lived interexcitonic quantum coherence in colloidal quantum dots.
Project description:Designing quantum algorithms for simulating quantum systems has seen enormous progress, yet few studies have been done to develop quantum algorithms for open quantum dynamics despite its importance in modeling the system-environment interaction found in most realistic physical models. In this work we propose and demonstrate a general quantum algorithm to evolve open quantum dynamics on quantum computing devices. The Kraus operators governing the time evolution can be converted into unitary matrices with minimal dilation guaranteed by the Sz.-Nagy theorem. This allows the evolution of the initial state through unitary quantum gates, while using significantly less resource than required by the conventional Stinespring dilation. We demonstrate the algorithm on an amplitude damping channel using the IBM Qiskit quantum simulator and the IBM Q 5 Tenerife quantum device. The proposed algorithm does not require particular models of dynamics or decomposition of the quantum channel, and thus can be easily generalized to other open quantum dynamical models.
Project description:CdSe semiconductor nanocrystal quantum dots are assembled into nanowire-like arrays employing microtubule fibers as nanoscale molecular "scaffolds." Spectrally and time-resolved energy-transfer analysis is used to assess the assembly of the nanoparticles into the hybrid inorganic biomolecular structure. Specifically, we demonstrate that a comprehensive study of energy transfer between quantum dot pairs on the biotemplate and, alternatively, between quantum dots and molecular dyes embedded in the microtubule scaffold comprises a powerful spectroscopic tool for evaluating the assembly process. In addition to revealing the extent to which assembly has occurred, the approach allows determination of particle-to-particle (and particle-to-dye) distances within the biomediated array. Significantly, the characterization is realized in situ, without need for further sample workup or risk of disturbing the solution-phase constructs. Furthermore, we find that the assemblies prepared in this way exhibit efficient quantum dot-quantum dot and quantum dot-dye energy transfer that affords faster energy-transfer rates compared to densely packed quantum dot arrays on planar substrates and to small-molecule-mediated quantum dot-dye couples, respectively.
Project description:Quantum metrology studies the ultimate limit of precision in estimating a physical quantity if quantum strategies are exploited. Here we investigate the evolution of a two-level atom as a detector which interacts with a massless scalar field using the master equation approach for open quantum system. We employ local quantum estimation theory to estimate the Unruh temperature when probed by a uniformly accelerated detector in the Minkowski vacuum. In particular, we evaluate the Fisher information (FI) for population measurement, maximize its value over all possible detector preparations and evolution times, and compare its behavior with that of the quantum Fisher information (QFI). We find that the optimal precision of estimation is achieved when the detector evolves for a long enough time. Furthermore, we find that in this case the FI for population measurement is independent of initial preparations of the detector and is exactly equal to the QFI, which means that population measurement is optimal. This result demonstrates that the achievement of the ultimate bound of precision imposed by quantum mechanics is possible. Finally, we note that the same configuration is also available to the maximum of the QFI itself.
Project description:Exploring excitation energy transfer (EET) in light-harvesting complexes (LHCs) is essential for understanding the natural processes and design of highly-efficient photovoltaic devices. LHCs are open systems, where quantum effects may play a crucial role for almost perfect utilization of solar energy. Simulation of energy transfer with inclusion of quantum effects can be done within the framework of dissipative quantum dynamics (QD), which are computationally expensive. Thus, artificial intelligence (AI) offers itself as a tool for reducing the computational cost. Here we suggest AI-QD approach using AI to directly predict QD as a function of time and other parameters such as temperature, reorganization energy, etc., completely circumventing the need of recursive step-wise dynamics propagation in contrast to the traditional QD and alternative, recursive AI-based QD approaches. Our trajectory-learning AI-QD approach is able to predict the correct asymptotic behavior of QD at infinite time. We demonstrate AI-QD on seven-sites Fenna-Matthews-Olson (FMO) complex.
Project description:High-speed electrical control of nano-optoelectronic properties in two-dimensional semiconductors is a building block for the development of excitonic devices, allowing the seamless integration of nano-electronics and -photonics. Here, we demonstrate a high-speed electrical modulation of nanoscale exciton behaviors in a MoS2 monolayer at room temperature through a quantum tunneling nanoplasmonic cavity. Electrical control of tunneling electrons between Au tip and MoS2 monolayer facilitates the dynamic switching of neutral exciton- and trion-dominant states at the nanoscale. Through tip-induced spectroscopic analysis, we locally characterize the modified recombination dynamics, resulting in a significant change in the photoluminescence quantum yield. Furthermore, by obtaining a time-resolved second-order correlation function, we demonstrate that this electrically-driven nanoscale exciton-trion interconversion achieves a modulation frequency of up to 8 MHz. Our approach provides a versatile platform for dynamically manipulating nano-optoelectronic properties in the form of transformable excitonic quasiparticles, including valley polarization, recombination, and transport dynamics.