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We present several coupled-cluster calculations of ground and excited states of 4He and 16O employing methods from quantum chemistry. A comparison of coupled cluster results with the results of exact diagonalization of the hamiltonian in…

Extracting the Hamiltonian of interacting quantum-information processing systems is a keystone problem in the realization of complex phenomena and large-scale quantum computers. The remarkable growth of the field increasingly requires…

Quantum--Mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those…

Chemical Physics · Physics 2015-06-12 Michele Pavanello , Troy Van Voorhis , Lucas Visscher , Johannes Neugebauer

Excited states in single quantum dots (QDs) have been shown to be useful for spin state initialization and manipulation. For scalable quantum information processing it is necessary to have multiple spins interacting. Therefore, we present…

We introduce a unitary coupled-cluster (UCC) ansatz termed $k$-UpCCGSD that is based on a family of sparse generalized doubles (D) operators which provides an affordable and systematically improvable unitary coupled-cluster wavefunction…

Quantum Physics · Physics 2019-01-07 Joonho Lee , William J. Huggins , Martin Head-Gordon , K. Birgitta Whaley

We present an excited-state-specific coupled-cluster approach in which both the molecular orbitals and cluster amplitudes are optimized for an individual excited state. The theory is formulated via a pseudoprojection of the traditional…

Chemical Physics · Physics 2023-11-27 Harrison Tuckman , Eric Neuscamman

Quantum calculations are performed for an anion water cluster representing the first hydration shell of the solvated electron in solution. The absorption spectra from the ground state, the instant excited states and the relaxed excited…

Soft Condensed Matter · Physics 2009-11-11 P. O. J. Scherer , Sighart F. Fischer

Atomistic electronic structure calculations are performed to study the coherent inter-dot couplings of the electronic states in a single InGaAs quantum dot molecule. The experimentally observed excitonic spectrum [12] is quantitatively…

Mesoscale and Nanoscale Physics · Physics 2013-08-01 Muhammad Usman , Yui-Hong Matthias Tan , Hoon Ryu , Shaikh S. Ahmed , Hubert Krenner , Timothy B. Boykin , Gerhard Klimeck

Calculations of molecular spectral properties, like photodissociation rates and absorption bands, rely on knowledge of the excited state energies of the molecule of interest. Protocols based on the variational quantum eigensolver (VQE) are…

Quantum Physics · Physics 2021-10-19 Yordan S. Yordanov , Crispin H. W. Barnes , David R. M. Arvidsson-Shukur

The exploration of the root structure of coupled cluster equations holds both foundational and practical significance for computational quantum chemistry. This study provides insight into the intricate root structures of these non-linear…

Chemical Physics · Physics 2024-09-12 Svala Sverrisdóttir , Fabian M. Faulstich

The simulation of electronic properties is a pivotal issue in modern electronic structure theory, driving significant efforts over the past decades to develop protocols for computing energy derivatives. In this work, we address this problem…

Quantum computational chemistry has emerged as an important application of quantum computing. Hybrid quantum-classical computing methods, such as variational quantum eigensolvers (VQE), have been designed as promising solutions to quantum…

We evaluate the Sample-based Krylov Quantum Diagonalization (SKQD) algorithm on one- and two-dimensional Heisenberg models, including strongly correlated regimes in which the ground state is dense. Using problem-informed initial states and…

Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schr\"odinger equation that scales favorably for large systems is…

Chemical Physics · Physics 2023-01-19 Mike Entwistle , Zeno Schätzle , Paolo A. Erdman , Jan Hermann , Frank Noé

Variational quantum algorithms on bosonic quantum processors are an emerging paradigm for quantum chemistry calculations, exploiting the natural alignment between molecular structure and harmonic oscillator-based hardware. We introduce the…

Quantum Physics · Physics 2026-04-21 Marlon F. Jost , Sijia S. Dong

We propose and experimentally demonstrate sequential quantum computing (SQC), a paradigm that utilizes multiple homogeneous or heterogeneous quantum processors in hybrid classical-quantum workflows. In this manner, we are able to overcome…

We present high-precision quantum computing simulations of three-body atoms (He, H$^-$) and molecules (H$_2^+$, HD$^+$), the latter being studied beyond the Born-Oppenheimer approximation. The Non-Iterative Disentangled Unitary Coupled…

Quantum Physics · Physics 2025-10-22 Mohammad Haidar , Hugo D. Nogueira , J. -Ph. Karr

Elucidation of the mechanism for optical spin initialization of point defects in solids in the context of quantum applications requires an accurate description of the excited electronic states involved. While variational density functional…

Materials Science · Physics 2023-07-14 Aleksei V. Ivanov , Yorick L. A. Schmerwitz , Gianluca Levi , Hannes Jónsson

Initialization of a qubit in a pure state is a prerequisite for quantum computer operation. Qubits are commonly initialized by cooling to their ground states through passive thermalization or by using active reset protocols. To accurately…

Quantum Physics · Physics 2020-07-01 Anatoly Kulikov , Rohit Navarathna , Arkady Fedorov

We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting Square Gradient Minimization (SGM) approach only requires…

Chemical Physics · Physics 2020-03-11 Diptarka Hait , Martin Head-Gordon
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