arXiv subjects

Marc Dvorak

Publications and source records attributed to Marc Dvorak.

14 recordsLinked to original sources

arXiv2026

A digitally controlled silicon quantum processing unit

Commercially-relevant quantum computers will require large numbers of high-performing qubits that can be manufactured, integrated, and controlled at scale. Silicon exchange-only (EO) qubits are a strong candidate modality due to their control-signal simplicity and compatibility with advanced semiconductor manufacturing, but questions remain around the achievability of sufficiently low noise and a scalable control and wiring solution. Here we introduce a quantum processing unit composed of a custom-designed cryogenic CMOS controller, a novel high-density superconducting ribbon cable, and a low-noise EO qubit device. The quantum chip features a three-rail array of 54 exchange-coupled quantum dots, configurable to host up to 18 EO qubits. We integrate and use these components to demonstrate qubit performance for both single-qubit and entangling operations that advances the EO state of the art by an order of magnitude. We further validate this system by implementing a distance-5 repetition code and a quantum error detecting code then make detailed comparisons with simulations. Our approach facilitates a utility-scale quantum computer with manageable operational and capital requirements.

quant-ph↗

arXiv2025

Roadmap on Advancements of the FHI-aims Software Package

Electronic-structure theory is the foundation of the description of materials including multiscale modeling of their properties and functions. Obviously, without sufficient accuracy at the base, reliable predictions are unlikely at any level that follows. The software package FHI-aims has proven to be a game changer for accurate free-energy calculations because of its scalability, numerical precision, and its efficient handling of density functional theory (DFT) with hybrid functionals and van der Waals interactions. It treats molecules, clusters, and extended systems (solids and liquids) on an equal footing. Besides DFT, FHI-aims also includes quantum-chemistry methods, descriptions for excited states and vibrations, and calculations of various types of transport. Recent advancements address the integration of FHI-aims into an increasing number of workflows and various artificial intelligence (AI) methods. This Roadmap describes the state-of-the-art of FHI-aims and advancements that are currently ongoing or planned.

cond-mat.mtrl-sci↗

arXiv2022

Protective Coating Interfaces for perovskite Solar Cell Materials: A first Principles Study

The protection of halide perovskites is important for the performance and stability of emergent perovskite-based optoelectronic technologies. In this work, we investigate the potential inorganic protective coating materials ZnO, SrZrO3, and ZrO2 for the CsPbI3perovskite. The optimal interface registries are identified with Bayesian optimization. We then use semi-local density-functional theory (DFT) to determine the atomic structure at the interfaces of each coating material with the clean CsI-terminated surface and three reconstructed surface models with added PbI2and CsI complexes. For the final structures, we explore the level alignment at the interface with hybrid DFT calculations. Our analysis of the level alignment at the coating-substrate interfaces reveals no detrimental mid-gap states, but substrate-dependent valence and conduction band offsets. While ZnO and SrZrO3act as insulators on CsPbI3, ZrO2 might be suitable as electron transport layer with the right interface engineering.

cond-mat.mtrl-sci↗

arXiv2021

Surface reconstruction of tetragonal methylammonium lead triiodide

We present a detailed first-principles analysis of the (001) surface of methylammonium lead triiodide (MAPbI3). With density-functional theory we investigate the atomic and electronic structure of the tetragonal (I4cm) phase of MAPbI3. We analysed surfaces models with MAI- (MAI-T) and PbI2-terminations(PbI2-T). For both terminations, we studied the clean-surface and a series of surface reconstructions. We find that the clean MAI-T model is more stable than its PbI2-T counterpart. For the MAI termination,reconstructions with added or removed units of nonpolar MAI and PbI2 are most stable. The corresponding band structures reveal surface states originating from the conduction band. Despite the presence of such additional surface states, our stable reconstructed surface models do not introduce new states within the band gap.

cond-mat.mtrl-sci↗

arXiv2021

Electronic Characterization of a Charge-Transfer Complex Monolayer on Graphene

Organic charge-transfer complexes (CTCs) formed by strong electron acceptor and strong electron donor molecules are known to exhibit exotic effects such as superconductivity and charge density waves. We present a low-temperature scanning tunneling microscopy and spectroscopy (LT-STM/STS) study of a two-dimensional (2D) monolayer CTC of tetrathiafulvalene (TTF) and fluorinated tetracyanoquinodimethane (F4TCNQ), self-assembled on the surface of oxygen-intercalated epitaxial graphene on Ir(111) (G/O/Ir(111)). We confirm the formation of the charge-transfer complex by dI/dV spectroscopy and direct imaging of the singly-occupied molecular orbitals. High-resolution spectroscopy reveals a gap at zero bias, suggesting the formation of a correlated ground state at low temperatures. These results point to the possibility to realize and study correlated ground states in charge-transfer complex monolayers on weakly interacting surfaces.

cond-mat.mes-hall↗

arXiv2021

Nonlocality, entropy creation, and entanglement in quantum many-body systems

We propose a reinterpretation and reformulation of the single-particle Green's function in nonrelativistic quantum many-body theory with an emphasis on normalization. By downfolding a correlation function covering all of Fock space into the observable portion, we derive a nonlocal Dyson equation which depends on an unknown downfolding frequency. The downfolding frequency is determined by solving the inverse problem so that the spectral function of the single-particle propagator is a Dirac-$δ$ function. Upon measurement, the system collapses stochastically onto one of these normalized solutions. This collapse has a nonlocal effect on the path the particle takes, in agreement with quantum entanglement. We postulate that the multiplicity of each quantized solution is directly related to the ensemble averaged spectrum and the entropy created by measurement of the particle. In the final part, we outline a new picture of dynamics in quantum many-body systems. As a function of the coupling strength, the multiplicity for collapse has a complicated form due to the shape of the quantization condition. This structure creates an entropic force from counting quantized solutions which is predominantly attractive but likely also has a narrow repulsive regime at weak coupling. Upon collapse, an internal spacetime forms between the two points in order to carry the information gained from the reduction of the probabilistic many-body state. The repeated creation of these spacetime bridges defines an internal spacetime with a complicated shape and history. We treat the quantum system as a finite informational resource that holds information about possible normalized outcomes, collapses the wave function to reset after encountering a conflict, and creates an internal spacetime to carry the information gained with every collapse.

cond-mat.str-el↗

arXiv2021

Particle conservation in the single-particle Green's function

We argue that the exact single-particle Green's function ($G$) in quantum many-body theory does not conserve particle number because the single-particle basis is incomplete. We conclude that the exact $G$ is not a probability amplitude and is not $Φ$-derivable in the Kadanoff-Baym sense. This sets up a number of inconsistencies involving normalization, the definition of $G$, interpretation of the spectral function, and $Φ$-derivability. Our result suggests that, in the most general case and in the most literal sense, $G$ is not suitable for computing particle addition/removal spectra.

cond-mat.str-el↗

arXiv2020

Atomic and electronic structure of cesium lead triiodide surfaces

The (001) surface of the emerging photovoltaic material cesium lead triiodide (CsPbI3 ) is studied. Using first-principles methods, we investigate the atomic and electronic structure of cubic (α) and orthorhombic (γ) CsPbI3 . For both phases, we find that CsI-termination is more stable than PbI2-termination. For the CsI-terminated surface, we then compute and analyse the surface phase diagram. We observe that surfaces with added or removed units of nonpolar CsI and PbI2 are most stable. The corresponding band structures reveal that the α phase exhibits surface states that derive from the conduction band. The surface reconstructions do not introduce new states in the band gap of CsPbI3, but for the α phase we find additional surface states at the conduction band edge.

cond-mat.mtrl-sci↗

arXiv2020

A balanced treatment of static and dynamic correlation in free- and Mg-porphyrin

We present an ab-initio dynamical configuration interaction (DCI) study of free- and Mg-porphyrin. DCI is a recently developed active space theory based on the Löwdin downfolding technique. In the active space, static correlation is described exactly with full configuration interaction. In the high energy, dynamically correlated subspace, we treat correlation at the quasiparticle level in the $GW$ approximation of Green's function theory. The final theory combines wave function and Green's function methods to give a balanced description of static and dynamic correlation. The theory and algorithm give a multireference treatment of ground and excited states for low computational cost. The four orbital Gouterman model of porphyrin offers an ideal active space in a large, correlated system to test the cost and accuracy of the embedding for large systems. Our parameter free, fully ab-initio DCI calculations in the minimal four-level active space agree well with both experiment and more expensive benchmark theories for the $Q_x$ and $Q_y$ transitions of free- and Mg-porphyrin. Studying the convergence of the excitation energies suggests that DCI correctly captures size extensive correlation effects, making it a promising active space theory for large, strongly-correlated systems.

cond-mat.mtrl-sci↗

arXiv2019

The GW compendium: A practical guide to theoretical photoemission spectroscopy

The GW approximation in electronic structure theory has become a widespread tool for predicting electronic excitations in chemical compounds and materials. In the realm of theoretical spectroscopy, the GW method provides access to charged excitations as measured in direct or inverse photoemission spectroscopy. The number of GW calculations in the past two decades has exploded with increased computing power and modern codes. The success of GW can be attributed to many factors: favorable scaling with respect to system size, a formal interpretation for charged excitation energies, the importance of dynamical screening in real systems, and its practical combination with other theories. In this review, we provide an overview of these formal and practical considerations. We expand, in detail, on the choices presented to the scientist performing GW calculations for the first time. We also give an introduction to the many-body theory behind GW, a review of modern applications like molecules and surfaces, and a perspective on methods which go beyond conventional GW calculations. This review addresses chemists, physicists and material scientists with an interest in theoretical spectroscopy. It is intended for newcomers to GW calculations but can also serve as an alternative perspective for experts and an up-to-date source of computational techniques.

cond-mat.mtrl-sci↗

arXiv2019

A quantum embedding theory in the screened Coulomb interaction: Combining configuration interaction with GW/BSE

We present a new quantum embedding theory called dynamical configuration interaction (DCI) that combines wave function and Green's function theories. DCI captures static correlation in a correlated subspace with configuration interaction and couples to high-energy, dynamic correlation outside the subspace with many-body perturbation theory based on Green's functions. In the correlated subspace, we use a wave function description to avoid embedding the two-particle vertex, which greatly simplifies the frequency structure of the embedding. DCI takes the strengths of both theories to balance static and dynamic correlation in a single, fully ab-initio embedding concept. We show that treating high-energy correlation up to the $GW$ and Bethe-Salpeter equation level is sufficient even for challenging multi-reference problems. Our theory treats ground and excited states on equal footing, and we compute the dissociation curve of N$_2$, vertical excitation energies of N$_2$ and C$_2$, and the ionization spectrum of benzene in excellent agreement with high level quantum chemistry methods and experiment.

physics.chem-ph↗

arXiv2019

Observation of Coexistence of Yu-Shiba-Rusinov States and Spin-Flip Excitations

We investigate the spectral evolution in different metal phthalocyanine molecules on NbSe$_2$ surface using scanning tunnelling microscopy (STM) as a function of the coupling with the substrate. For manganese phthalocyanine (MnPc), we demonstrate a smooth spectral crossover from Yu-Shiba-Rusinov (YSR) bound states to spin-flip excitations. This has not been observed previously and it is in contrast to simple theoretical expectations. We corroborate the experimental findings using numerical renormalization group calculations. Our results provide fundamental new insight on the behavior of atomic scale magnetic/SC hybrid systems, which is important for e.g. engineered topological superconductors and spin logic devices.

cond-mat.mes-hall↗

arXiv2018

Dynamical configuration interaction: Quantum embedding that combines wave functions and Green's functions

We present the concept, derivation, and implementation of dynamical configuration interaction, a quantum embedding theory that combines Green's function methodology with the many-body wave function. In a strongly-correlated active space, we use full configuration interaction (CI) to describe static correlation exactly. We add energy dependent corrections to the CI Hamiltonian which, in principle, include all remaining correlation derived from the bath space surrounding the active space. Next, we replace the exact Hamiltonian in the bath with one of excitations defined over a correlated ground state. This transformation is naturally suited to the methodology of many-body Green's functions. In this space, we use a modified $GW$/Bethe-Salpeter equation procedure to calculate excitation energies. Combined with an estimate of the ground state energy in the bath, we can efficiently compute the energy dependent corrections, which correlate the full set of orbitals, for very low computational cost. We present dimer dissociation curves for H$_2$ and N$_2$ in good agreement with exact results. Additionally, excited states of N$_2$ and C$_2$ are in excellent agreement with benchmark theory and experiment. By combining the strengths of two disciplines, we achieve a balanced description of static and dynamic correlation in a fully ab-initio, systematically improvable framework.

physics.chem-ph↗

arXiv2017

Coupled Yu-Shiba-Rusinov states in molecular dimers on NbSe$_2$

Magnetic impurities have a dramatic effect on superconductivity by breaking the time-reversal symmetry and inducing so-called Yu-Shiba-Rusinov (YSR) low energy bound states within the superconducting gap. The spatial extent of YSR states is greatly enhanced in 2D systems, which should facilitate the formation of coupled states. Here, we observe YSR states on single cobalt phthalocyanine (CoPC) molecules on a 2D superconductor NbSe$_2$ using low-temperature scanning tunneling microscopy (STM) and spectroscopy (STS). We use STM lateral manipulation to create controlled CoPc dimers and demonstrate the formation of coupled YSR states. The experimental results are corroborated by theoretical analysis of the coupled states in lattice and continuum models. Our work forms an important step towards the realization of exotic topological states in designer magnetic lattices.

cond-mat.mes-hall↗