Humidity effect on ion behaviors of moisture-driven CO2 sorbents

Shi, Xiaoyang; Xiao, Hang; Liao, Xiangbiao; Armstrong, Mitchell R.; Chen, Xi; Lackner, Klaus S.

doi:10.1063/1.5027105

Cited by 30 publications

(22 citation statements)

References 38 publications

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“…As we will see in the following sections, the form of the Frenkel Hamiltonian allows us to easily map unitary qubit operations onto excitonic circuit geometries. As has been shown in previous studies, 31,32 the details of the molecular structure of the dyes, such as the disorder of the molecular system, can be encoded in the elements of the Hamiltonian. The parameters of the Frenkel Hamiltonian can also be determined from classical molecular dynamics together with semiempirical electronic structure calculations on the electronically excited molecular system.…”

Section: Frenkel Exciton Modelmentioning

confidence: 80%

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

Castellanos¹,

Dodin²,

Willard

2019

Preprint

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This manuscript presents a strategy for controlling the transformation of excitonic states through the design of circuits made up of coupled organic dye molecules. Specifically, we show how unitary transformation matrices can be mapped to the Hamiltonians of physical systems of dye molecules with specified geometric and chemical properties.The evolution of these systems over specific times encode the action of the unitary transformation. We identify the bounds on complexity of the transformations that can be represented by these circuits. We formalize this strategy and apply it to identify the excitonic circuits of the four universal quantum logic gates: NOT, Hadamard, π/8 and CNOT. We discuss the properties of these circuits and how their performance is expected to be influenced by the presence of environmental noise. We quantify the bounds on the spectroscopic properties of organic dye circuits under which single-qubit unitary transformations are possible.The elementary component of a quantum computer -a qubit -is a two-state quantum system. A qubit can be constructed from many different physical systems, including a pair of coupled organic dye molecules sharing a single electronic excitation (i.e., an exciton).Using this kind of qubit it is therefore possible, at least in principle, to develop quantum computing platforms that operate via the excited state dynamics of specifically designed excitonic circuits comprised of multiple dye molecules in precise geometric arrangements. In this manuscript, we introduce a general strategy for designing excitonic circuits for quantum computation. We apply this strategy to identify fundamental bounds on the computational complexity that these circuits can support and identify the physical requirements for performing universal quantum logic gate operations on one-and two-qubit systems. This study therefore sets the groundwork for enabling the development of programmable dye-based quantum computing platforms.Excitonic circuits are constructed by arranging the positions and orientations of dye molecules. The evolution of excitons within the circuit is determined by the intermolecular electronic coupling network and the electronic properties of the dyes. The electronic coupling between dye molecules is programmed by their intermolecular spacing and orientation. 1 Supermolecular support structures, such as proteins, 2,3 metal-organic frameworks, 4 and DNA nanostructures, 5,6 can be used to situate dye molecules with coupling networks that are designed to control certain aspects of exciton dynamics. The resulting dynamical control can be used to implement the state transformations required for quantum computation.Quantum computing offers several key advantages over traditional classical computing and is poised to make a transformative impact on certain areas of the information sciences, such as cryptography and molecular simulation. 7,8 However, despite enormous potential for broad technological impact, quantum computing presents unique implementation challenges that have thus f...

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Section: Frenkel Exciton Modelmentioning

confidence: 80%

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

Castellanos¹,

Dodin²,

Willard

2019

Preprint

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“…To investigate the diffusion behaviors of Cu ion on a-Ta 2 O 5 surface, again MD simulation can be employed as have done in a recent study of the moisture effect on the diffusion of ions in a novel CO 2 sorbent [18]. In the present study, however, the climbing-image nudged elastic band (CI-NEB) method [19] is employed using 2 × 2 × 1 k-points because realistic atomic structures of nanopores are difficult to obtain as mentioned in the next section.…”

Section: Theoretical Methodsmentioning

confidence: 99%

Moisture effect on the diffusion of Cu ions in Cu/Ta₂O₅/Pt and Cu/SiO₂/Pt resistance switches: a first-principles study

Xiao

Watanabe

2019

Science and Technology of Advanced Materials

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are two of the most promising resistance switches. From experimental observations, it is speculated that the presence of H 2 O in the amorphous Ta 2 O 5 and SiO 2 (a-Ta 2 O 5 and a-SiO 2) facilitates the rate-limiting step during the switching process. This rate-limiting step is essentially the diffusion of Cu ions along the nanopores of the amorphous. To better understand this behavior and obtain a detailed examination of the atomic structures, a first-principles simulation was conducted. In addition, we investigate the diffusion behaviors of Cu ions in bare a-Ta 2 O 5 nanopore and in the one covered with H 2 O-together with those in a-SiO 2 nanopore. Our work reveals that Ta and Si atoms on the sidewalls of bare a-Ta 2 O 5 and a-SiO 2 nanopores are in the unsaturated (TaO 5) and saturated (SiO 4) forms, respectively. Consequently, H 2 O molecules are adsorbed on the nanopore sidewall strongly in the case of a-Ta 2 O 5, and weakly in a-SiO 2 , by forming O-Ta and H•••O bonds, respectively. This can explain the experimental observation that the desorption of H 2 O occurs only at high temperatures for a-Ta 2 O 5 films, while it is observed for a-SiO 2 even when the temperature is low. The calculated diffusion barrier of Cu ions in a-Ta 2 O 5 nanopores covered with H 2 O is about 0.43 eV, which is much lower than that without H 2 O (~1.40 eV). In view of the similar chemical environments of O and the adsorbed Cu ions in a-SiO 2 and a-Ta 2 O 5 nanopores, it is expected that the diffusion of Cu ions in a-SiO 2 nanopore without H 2 O is much more difficult than with H 2 O. This could be attributed to the strong and weak adsorption of Cu ions on the sidewall in the absence and presence of H 2 O, respectively, for both, a-Ta 2 O 5 and a-SiO 2. Our investigation provides a full atomic picture to understand the moisture effect on the diffusion of Cu ions in Cu/a-Ta 2 O 5 /Pt and Cu/a-SiO 2 /Pt resistance switches.

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“…Einige Feuchtigkeitswechsel‐Sorbenten sind stark basische Ionenaustauschharze ( ion exchange resins , IER) mit quartären Ammoniumionen (NR 4 + ), welche als starke Base agieren, analog zu Na + ‐Ionen in wässrigen Lösungen. Abbildung zeigt die chemische Struktur des Harzes. Die Kationen werden durch in der Matrix vorhandene Anionen ausgeglichen.…”

Section: Sorbenten Zur Gewinnung Von Co2 Aus Der Umgebungsluftunclassified

Sorbenten zur direkten Gewinnung von CO₂ aus der Umgebungsluft

et al. 2020

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Die Dringlichkeit, den durch Treibhausgasemissionen verursachten globalen Klimawandel anzugehen, wächst von Tag zu Tag. Insbesondere der Anstieg der atmosphärischen CO2‐Werte löst Alarm aus. Technologien zum Absorbieren von CO2 aus der Umgebungsluft, oder “Direct Air Capture” (DAC), haben kürzlich gezeigt, dass sie zu “negativen Kohlenstoffemissionen” beitragen können. Die jüngsten Fortschritte in der Oberflächenchemie und der Materialsynthese haben neue Generationen von CO2‐Sorptionsmitteln ermöglicht, die möglicherweise die Zukunft von DAC und seiner großangelegten Verwendung vorantreiben können. In diesem Aufsatz werden die wichtigsten Arten von Sorptionsmitteln zur Gewinnung von CO2 aus der Umgebungsluft beschrieben und nach Sorptionsmechanismen kategorisiert: Physisorption, Chemisorption und Feuchtigkeitswechsel‐Sorption.

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Humidity effect on ion behaviors of moisture-driven CO2 sorbents

Cited by 30 publications

References 38 publications

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

Moisture effect on the diffusion of Cu ions in Cu/Ta₂O₅/Pt and Cu/SiO₂/Pt resistance switches: a first-principles study

Sorbenten zur direkten Gewinnung von CO₂ aus der Umgebungsluft

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Humidity effect on ion behaviors of moisture-driven CO2 sorbents

Cited by 30 publications

References 38 publications

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

On the Design of Molecular Excitonic Circuits for Quantum Computing: The Universal Quantum Gates

Moisture effect on the diffusion of Cu ions in Cu/Ta2O5/Pt and Cu/SiO2/Pt resistance switches: a first-principles study

Sorbenten zur direkten Gewinnung von CO2 aus der Umgebungsluft

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Product

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Moisture effect on the diffusion of Cu ions in Cu/Ta₂O₅/Pt and Cu/SiO₂/Pt resistance switches: a first-principles study

Sorbenten zur direkten Gewinnung von CO₂ aus der Umgebungsluft