Related papers: Wavefunction Embedding for Molecular Polaritons
The Quantum-Electrodynamical Time-Dependent Density Functional Theory (QED-TDDFT) equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Applications for molecules in cavities…
Quantum electrodynamics coupled-cluster (QED-CC) theory is used to model vacuum-field-induced changes to ground-state properties of a series of sodium halide compounds (NaX, X = F, Cl, Br, I) strongly coupled to an optical cavity.…
Trying to export ab initio polaritonic chemistry onto emerging quantum computers raises fundamental questions. A central one is how to efficiently represent both fermionic and bosonic degrees of freedom on the same platform, in order to…
In the near future, material and drug design may be aided by quantum computer assisted simulations. These have the potential to target chemical systems intractable by the most powerful classical computers. However, the resources offered by…
The large number of degrees of freedom involved in polaritonic chemistry processes considerably restricts the systems that can be described by any ab initio approach, due to the resulting high computational cost. Semiclassical methods that…
Multireference systems are usually challenging to investigate using ab initio methods as they require an accurate description of static electron correlation. The urgency of developing similar approaches is even more pressing when molecules…
QCDFT is a multiscale modeling approach that can simulate multi-million atoms effectively via density functional theory (DFT). The method is based on the framework of quasicontinuum (QC) approach with DFT as its sole energetics formulation.…
The pair-coupled-cluster doubles (pCCD) method has emerged as a viable approach for quantum-chemical studies of strongly correlated systems. Despite its lower formal scaling (O(N$^4$)) compared to other versions of coupled cluster (CC)…
Perturbative approaches are methods to efficiently tackle many-body problems, offering both intuitive insights and analysis of correlation effects. However, their application to systems where light and matter are strongly coupled is…
Cavity quantum electrodynamics (QED) studies the interaction between a quantum emitter and a single radiation-field mode. When an atom is in strong coupling with a cavity mode1,2, it is possible to realize key quantum information processing…
It remains a prime question of how to describe the optical properties of large molecular clusters accurately. Quantum chemical methods capture essential electronic details but are infeasible for entire clusters, while optical simulations…
A unitary coupled-cluster (UCC) form for the wavefunction in the variational quantum eigensolver has been suggested as a systematic way to go beyond the mean-field approximation and include electron correlation in solving quantum chemistry…
We analyze the real-time electron-photon dynamics in long-range polariton-mediated energy transfer using a real-time quantum electrodynamics coupled cluster (RT-QED-CC) model, which allows for spatial and temporal visualization of transport…
Catalyzing reactions effectively by vacuum fluctuations of electromagnetic fields is a significant challenge within the realm of chemistry. Different from most studies based on vibrational strong coupling, we introduce an innovative…
Recent experiments have demonstrated that polariton formation provides a novel strategy for modifying local molecular processes when a large ensemble of molecules is confined within an optical cavity. Herein, a numerical strategy based on…
We analyse the coherent-state (CS) transformation in quantum electrodynamics coupled cluster (QED-CC) theory from the perspective of its non-vanishing commutator with the polaritonic cluster operator. Specifically, we show that a QED…
Achieving chemical accuracy for molecular simulations remains a central challenge in computational chemistry. Here, we present an embedded correlated wavefunction transfer learning (ECW-TL) framework for accurately simulating molecular…
We present an ab initio correlated approach to study molecules that interact strongly with quantum fields in an optical cavity. Quantum electrodynamics coupled cluster theory provides a non-perturbative description of cavity-induced effects…
Strong light-matter coupling enables hybrid states in which photonic and electronic degrees of freedom become correlated even in the ground state. While many-body effects in long-range dispersion interactions are known to reshape electronic…
Cavity quantum electrodynamics (cQED) harnesses light-matter interactions to produce nonclassical light states. However, a fundamental challenge lies in simultaneously achieving Purcell enhancement and tailored wavefront control within a…