David P. Tew
YOU?
Author Swipe
View article: Spin-free Generalised Normal Ordered Coupled Cluster
Spin-free Generalised Normal Ordered Coupled Cluster Open
We present a spin-free, size-extensive, and size-consistent coupled cluster method based on a generalised normal ordered exponential ansatz. This approach is a natural generalisation of single-reference coupled cluster theory for arbitrary…
View article: DLPNO-MP2 for Periodic Systems using Megacell Embedding
DLPNO-MP2 for Periodic Systems using Megacell Embedding Open
We present a domain-based local pair natural orbital Møller--Plesset second order perturbation theory (DLPNO-MP2) for periodic systems, working within an LCAO formalism within the Tubromole program package. This approach, Megacell-DLPNO-MP…
View article: Diagrammatic theory of the irreducible coupled-cluster self-energy
Diagrammatic theory of the irreducible coupled-cluster self-energy Open
Coupled-cluster and Green's function theories are highly successful in treating many-body electron correlation, and there has been significant interest in identifying and leveraging connections between them. Here we present a diagrammatic …
View article: Quantum Resource Assay for the Grid-Based Simulation of the Photodynamics of Pyrazine
Quantum Resource Assay for the Grid-Based Simulation of the Photodynamics of Pyrazine Open
We establish and analyse the performance and resource requirements of an end-to-end fault-tolerant quantum algorithm for computing the absorption spectrum and population dynamics of photoexcited pyrazine. The quantum circuit construction c…
View article: Spin coupling is all you need: Encoding strong electron correlation in molecules on quantum computers
Spin coupling is all you need: Encoding strong electron correlation in molecules on quantum computers Open
The performance of quantum algorithms for eigenvalue problems, such as computing Hamiltonian spectra, depends strongly on the overlap of the initial wave function and the target eigenvector. In a basis of Slater determinants, the represent…
View article: Wannier Function Localization Using Bloch Intrinsic Atomic Orbitals
Wannier Function Localization Using Bloch Intrinsic Atomic Orbitals Open
We extend the intrinsic atomic orbital (IAO) method for the localization of molecular orbitals to calculate well-localized generalized Wannier functions in crystals in the spirit of the Pipek-Mezey method. We furthermore present a one-shot…
View article: Wannier function localisation using Bloch intrinsic atomic orbitals
Wannier function localisation using Bloch intrinsic atomic orbitals Open
We extend the Intrinsic Atomic Orbital (IAO) method for localisation of molecular orbitals to calculate well-localised generalised Wannier functions in crystals using the Pipek--Mezey locality metric. We furthermore present a one-shot diab…
View article: Spin coupling is all you need: Encoding strong electron correlation in molecules on quantum computers
Spin coupling is all you need: Encoding strong electron correlation in molecules on quantum computers Open
The performance of quantum algorithms for eigenvalue problems, such as computing Hamiltonian spectra, depends strongly on the overlap of the initial wavefunction and the target eigenvector. In a basis of Slater determinants, the representa…
View article: Improved CPS and CBS Extrapolation of PNO-CCSD(T) Energies: The MOBH35 and ISOL24 Data Sets
Improved CPS and CBS Extrapolation of PNO-CCSD(T) Energies: The MOBH35 and ISOL24 Data Sets Open
Computation of heats of reaction of large molecules is now feasible using the domain-based pair natural orbital (PNO)-coupled-cluster singles, doubles, and perturbative triples [CCSD(T)] theory. However, to obtain agreement within 1 kcal/m…
View article: Multi-reference coupled cluster theory using the normal ordered exponential ansatz
Multi-reference coupled cluster theory using the normal ordered exponential ansatz Open
Properly spin-adapted coupled-cluster theory for general open-shell configurations remains an active area of research in electronic structure theory. In this contribution we examine Lindgren's normal-ordered exponential ansatz to correlate…
View article: Which model density is best in pair natural orbital local correlation theory?
Which model density is best in pair natural orbital local correlation theory? Open
Low-scaling electron correlation theory based on the pair natural orbital approximation, PNO-CCSD(T), has become a powerful computational tool. Motivated by the recent discovery of large errors for organometallic molecules, we assess the r…
View article: Spin-coupled molecular orbitals: chemical intuition meets quantum chemistry
Spin-coupled molecular orbitals: chemical intuition meets quantum chemistry Open
Molecular orbital theory is powerful both as a conceptual tool for understanding chemical bonding, and as a theoretical framework for ab initio quantum chemistry. Despite its undoubted success, MO theory has well documented shortcomings, m…
View article: Continuous-wave cavity ringdown for high-sensitivity polarimetry and magnetometry measurements
Continuous-wave cavity ringdown for high-sensitivity polarimetry and magnetometry measurements Open
We report the development of a novel variant of cavity ringdown polarimetry using a continuous-wave laser operating at 532 nm for highly precise chiroptical activity and magnetometry measurements. The key methodology of the apparatus relie…
View article: Continuous-Wave Cavity Ring-Down for High-Sensitivity Polarimetry and Magnetometry Measurements
Continuous-Wave Cavity Ring-Down for High-Sensitivity Polarimetry and Magnetometry Measurements Open
We report the development of a novel variant of cavity ring-down polarimetry using a continuous-wave laser operating at 532 nm for highly precise chiroptical activity and magnetometry measurements. The key methodology of the apparatus reli…
View article: Multi-reference coupled cluster theory using the normal ordered exponential ansatz
Multi-reference coupled cluster theory using the normal ordered exponential ansatz Open
We examine Lindgren's normal-ordered exponential ansatz to correlate specific spin states using spin-free excitation operators, with the aid of automatic equation generation software.
View article: Which model density is best in pair natural orbital local correlation theory?
Which model density is best in pair natural orbital local correlation theory? Open
Low-scaling electron correlation theory based on the pair natural orbital approximation, PNO-CCSD(T), has become a powerful computational tool. Motivated by the recent discovery of large errors for organometallic molecules, we assess the r…
View article: Diagrammatic theory of the irreducible coupled-cluster self-energy
Diagrammatic theory of the irreducible coupled-cluster self-energy Open
Coupled-cluster and Green's function theories are highly successful in treating many-body electron correlation, and there has been significant interest in identifying and leveraging connections between them. Here we present a diagrammatic …
View article: Improved CPS and CBS Extrapolation of PNO-CCSD(T) Energies: The MOBH35 and ISOL24 Data Sets
Improved CPS and CBS Extrapolation of PNO-CCSD(T) Energies: The MOBH35 and ISOL24 Data Sets Open
Computation of heats of reaction of large molecules is now feasible using domain-based PNO-CCSD(T) theory. However, to obtain agreement within 1~kcal/mol of experiment, it is necessary to eliminate basis set incompleteness error, which com…
View article: Exact electronic states with shallow quantum circuits from global optimisation
Exact electronic states with shallow quantum circuits from global optimisation Open
Quantum computers promise to revolutionise molecular electronic simulations by overcoming the exponential memory scaling. While electronic wave functions can be represented using a product of fermionic unitary operators, the best ansatz fo…
View article: Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation"
Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation" Open
Numerical data and plotting scripts for regenerating figures in the article "Exact electronic states with shallow quantum circuits using global optimisation". See README for more details.
View article: TURBOMOLE: Today and Tomorrow
TURBOMOLE: Today and Tomorrow Open
TURBOMOLE is a highly optimized software suite for large-scale quantum-chemical and materials science simulations of molecules, clusters, extended systems, and periodic solids. TURBOMOLE uses Gaussian basis sets and has been designed with …
View article: A Regularized Second-Order Correlation Method from Green’s Function Theory
A Regularized Second-Order Correlation Method from Green’s Function Theory Open
[Image: see text] We present a scalable single-particle framework to treat electronic correlation in molecules and materials motivated by Green’s function theory. We derive a size-extensive Brillouin-Wigner perturbation theory from the sin…
View article: Grid-based methods for chemistry simulations on a quantum computer
Grid-based methods for chemistry simulations on a quantum computer Open
First-quantized, grid-based methods for chemistry modeling are a natural and elegant fit for quantum computers. However, it is infeasible to use today’s quantum prototypes to explore the power of this approach because it requires a substan…
View article: A regularized second-order correlation method from Green's function theory
A regularized second-order correlation method from Green's function theory Open
We present a scalable single-particle framework to treat electronic correlation in molecules and materials motivated by Green's function theory. We derive a size-extensive Brillouin-Wigner perturbation theory from the single-particle Green…
View article: Which Model Density is Best in Pair Natural Orbital Local Correlation Theory?
Which Model Density is Best in Pair Natural Orbital Local Correlation Theory? Open
View article: The microwave spectrum of the C2H2…AgI complex assigned and analysed using PGOPHER
The microwave spectrum of the C2H2…AgI complex assigned and analysed using PGOPHER Open
Rotational spectra of four isotopologues of C2H2…AgI have been recorded between 6.5 and 18.5 GHz by chirped-pulse Fourier transform microwave spectroscopy. The complex is generated through laser ablation of a silver target in the presence …
View article: Exact electronic states with shallow quantum circuits through global optimisation
Exact electronic states with shallow quantum circuits through global optimisation Open
Quantum computers promise to revolutionise electronic simulations by overcoming the exponential scaling of many-electron problems. While electronic wave functions can be represented using a product of fermionic unitary operators, shallow q…
View article: Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation"
Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation" Open
Numerical data and plotting scripts for regenerating figures in the pre-print "Exact electronic states with shallow quantum circuits using global optimisation". See README for more details.
View article: Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation"
Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation" Open
Numerical data and plotting scripts for regenerating figures in the article "Exact electronic states with shallow quantum circuits using global optimisation". See README for more details.
View article: Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation"
Research data supporting "Exact electronic states with shallow quantum circuits using global optimisation" Open
Numerical data and plotting scripts for regenerating figures in the article "Exact electronic states with shallow quantum circuits using global optimisation". See README for more details.