Surface science using coupled cluster theory via local Wannier functions and in-RPA-embedding: the case of water on graphitic carbon nitride

<div> <div>A shortcoming of presently available fragment-based methods is that electron correlation (if included) is described at the level of individual electrons, resulting in many redundant evaluations of the electronic relaxations associated with any given fluctuation. A generalized variant of coupled-cluster (CC) theory is described, wherein the degrees of freedom are fluctuations of fragments between internally correlated states. The effects of intra-fragment correlation on the inter-fragment interaction is pre-computed and permanently folded into the effective Hamiltonian. This article provides a high-level description of the CC variant, establishing some useful notation, and it demonstrates the advantage of the proposed paradigm numerically on model systems. A companion article shows that the electronic Hamiltonian of real systems may always be cast in the form demanded. This framework opens a promising path to build finely tunable systematically improvable methods to capture precise properties of systems interacting with a large number of other systems. </div> </div>

Download Full-text

Excitonic Coupled-cluster Theory: Part I, General Formalism

10.26434/chemrxiv.5330773.v1 ◽

2017 ◽

Author(s):

Yuhong Liu ◽

Anthony Dutoi

Keyword(s):

Electron Correlation ◽

Degrees Of Freedom ◽

Model Systems ◽

Coupled Cluster ◽

Effective Hamiltonian ◽

Coupled Cluster Theory ◽

Cluster Theory ◽

Companion Article ◽

High Level ◽

Fragment Interaction

<div> <div>A shortcoming of presently available fragment-based methods is that electron correlation (if included) is described at the level of individual electrons, resulting in many redundant evaluations of the electronic relaxations associated with any given fluctuation. A generalized variant of coupled-cluster (CC) theory is described, wherein the degrees of freedom are fluctuations of fragments between internally correlated states. The effects of intra-fragment correlation on the inter-fragment interaction is pre-computed and permanently folded into the effective Hamiltonian. This article provides a high-level description of the CC variant, establishing some useful notation, and it demonstrates the advantage of the proposed paradigm numerically on model systems. A companion article shows that the electronic Hamiltonian of real systems may always be cast in the form demanded. This framework opens a promising path to build finely tunable systematically improvable methods to capture precise properties of systems interacting with a large number of other systems. </div> </div>

Download Full-text

Two Dimensional Nanosheet of Graphitic Carbon Nitride and Graphene: An Efficient Spin Filter With Robust Negative Differential Resistance Action

SSRN Electronic Journal ◽

10.2139/ssrn.3526726 ◽

2020 ◽

Author(s):

Rinki Bhowmick ◽

Vishal Kashyap ◽

Yachna Raj ◽

Sabyasachi Sen

Keyword(s):

Negative Differential Resistance ◽

Carbon Nitride ◽

Differential Resistance ◽

Graphitic Carbon ◽

Graphitic Carbon Nitride ◽

Two Dimensional ◽

Spin Filter

Download Full-text

Metal Doped-C3N4/Fe2O4: Efficient and Versatile Heterogenous Catalysts for Organic Transformations

Current Organic Chemistry ◽

10.2174/1385272823666190709113758 ◽

2019 ◽

Vol 23 (12) ◽

pp. 1284-1306

Author(s):

Vijai K. Rai ◽

Fooleswar Verma ◽

Suhasini Mahata ◽

Smita R. Bhardiya ◽

Manorama Singh ◽

...

Keyword(s):

Ring Opening ◽

Carbon Nitride ◽

Addition Reaction ◽

High Surface ◽

Graphitic Carbon ◽

Graphitic Carbon Nitride ◽

Organic Transformations ◽

Reduction Reactions ◽

Activation Reaction ◽

Metal Doped

The polymeric graphitic carbon nitride (g-C3N4) has been one of the interesting earth abundant elements. Though g-C3N4 finds application as a photocatalyst, its photocatalytic behaviour is limited because of low efficiency, mainly due to rapid charge recombination. To overcome this problem, several strategies have been developed including doping of metal/non-metal in the cavity of g-C3N4. Moreover, the CoFe2O4 NPs have been used in many organic transformations because of its high surface area and easy separation due to its magnetic nature. This review describes the role of cobalt ferrite as magnetic nanoparticles and metal-doped carbon nitride as efficient heterogeneous catalysts for new carbon-carbon and carbon-hetero atom bond formation followed by heterocyclization. Reactions which involved new catalysts for selective activation of readily available substrates has been reported herein. Since nanoparticles enhance the reactivity of catalyst due to higher catalytic area, they have been employed in various reactions such as addition reaction, C-H activation reaction, coupling reaction, cyclo-addition reaction, multi-component reaction, ring-opening reaction, oxidation reaction and reduction reactions etc. The driving force for choosing this topic is based-on huge number of good publications including different types of spinels/metal doped-/graphitic carbon nitride reported in the literature and due to interest of synthetic community in recent years. This review certainly will represent the present status in organic transformation and for exploring further their catalytic efficiency to new organic transformations involving C-H activation reaction through coupling, cyclo-addition, multi-component, ring-opening, oxidation and reduction reactions.

Download Full-text