Search

We propose to use wave function overlaps obtained from a quantum computer as inputs for the classical split-amplitude techniques, tailored and externally corrected coupled cluster, to achieve balanced treatment of static and dynamic correlation effects in molecular electronic structure simulations. By combining insights from statistical properties of matchgate shadows, which are used to measure quantum trial state overlaps, with classical correlation diagnostics, we can provide quantum resource estimates well into the classically no longer exactly solvable regime. We find that rather imperfect wave functions and remarkably low shot counts are sufficient to cure qualitative failures of plain coupled cluster singles doubles and to obtain chemically precise dynamic correlation energy corrections. We provide insights into which wave function preparation schemes have a chance of yielding quantum advantage, and we test our proposed method using overlaps measured on Google's Sycamore device.

We present the first hardware implementation of electrostatic interaction energies by using a trapped-ion quantum computer. As test system for our computation, we focus on the reduction of NO to N 2 O catalyzed by a nitric oxide reductase (NOR). The quantum computer is used to generate an approximate ground state within the NOR active space. To efficiently measure the necessary one-particle density matrices, we incorporate fermionic basis rotations into the quantum circuit without extending the circuit length, laying the groundwork for further efficient measurement routines using factorizations. Measurements in the computational basis are then used as inputs for computing the electrostatic interaction energies on a classical computer. Our experimental results strongly agree with classical noise-less simulations of the same circuits, finding electrostatic interaction energies within chemical accuracy despite hardware noise. This work shows that algorithms tailored to specific observables of interest, such as interaction energies, may require significantly fewer quantum resources than individual ground state energies would require in the straightforward supermolecular approach., Competing Interests: The authors declare the following competing financial interest(s): R.M.P., M.L., and P.J.O. own stock options in QC Ware Corp., (© 2024 The Authors. Published by American Chemical Society.)

Efficient representations of the Hamiltonian, such as double factorization, drastically reduce the circuit depth or the number of repetitions in error corrected and noisy intermediate-scale quantum (NISQ) algorithms for chemistry. We report a Lagrangian-based approach for evaluating relaxed one- and two-particle reduced density matrices from double factorized Hamiltonians, unlocking efficiency improvements in computing the nuclear gradient and related derivative properties. We demonstrate the accuracy and feasibility of our Lagrangian-based approach to recover all off-diagonal density matrix elements in classically simulated examples with up to 327 quantum and 18 470 total atoms in QM/MM simulations with modest-sized quantum active spaces. We show this in the context of the variational quantum eigensolver in case studies, such as transition state optimization, ab initio molecular dynamics simulation, and energy minimization of large molecular systems.

Results on the hardness of approximate sampling are seen as important stepping stones toward a convincing demonstration of the superior computational power of quantum devices. The most prominent suggestions for such experiments include boson sampling, instantaneous quantum polynomial time (IQP) circuit sampling, and universal random circuit sampling. A key challenge for any such demonstration is to certify the correct implementation. For all these examples, and in fact for all sufficiently flat distributions, we show that any noninteractive certification from classical samples and a description of the target distribution requires exponentially many uses of the device. Our proofs rely on the same property that is a central ingredient for the approximate hardness results, namely, that the sampling distributions, as random variables depending on the random unitaries defining the problem instances, have small second moments.

Under unitary time evolution, expectation values of physically reasonable observables often evolve towards the predictions of equilibrium statistical mechanics. The eigenstate thermalization hypothesis (ETH) states that this is also true already for individual energy eigenstates. Here we aim at elucidating the emergence of the ETH for observables that can realistically be measured due to their high degeneracy, such as local, extensive, or macroscopic observables. We bisect this problem into two parts, a condition on the relative overlaps and one on the relative phases between the eigenbases of the observable and Hamiltonian. We show that the relative overlaps are unbiased for highly degenerate observables and demonstrate that unless relative phases conspire to cumulative effects, this makes such observables verify the ETH. Through this we elucidate potential pathways towards proofs of thermalization.

We study correlations in fermionic lattice systems with long-range interactions in thermal equilibrium. We prove a bound on the correlation decay between anticommuting operators and generalize a long-range Lieb-Robinson-type bound. Our results show that in these systems of spatial dimension D with, not necessarily translation invariant, two-site interactions decaying algebraically with the distance with an exponent α≥2D, correlations between such operators decay at least algebraically to 0 with an exponent arbitrarily close to α at any nonzero temperature. Our bound is asymptotically tight, which we demonstrate by a high temperature expansion and by numerically analyzing density-density correlations in the one-dimensional quadratic (free, exactly solvable) Kitaev chain with long-range pairing.

Markov logic networks (MLNs) reconcile two opposing schools in machine learning and artificial intelligence: causal networks, which account for uncertainty extremely well, and first-order logic, which allows for formal deduction. An MLN is essentially a first-order logic template to generate Markov networks. Inference in MLNs is probabilistic and it is often performed by approximate methods such as Markov chain Monte Carlo (MCMC) Gibbs sampling. An MLN has many regular, symmetric structures that can be exploited at both first-order level and in the generated Markov network. We analyze the graph structures that are produced by various lifting methods and investigate the extent to which quantum protocols can be used to speed up Gibbs sampling with state preparation and measurement schemes. We review different such approaches, discuss their advantages, theoretical limitations, and their appeal to implementations. We find that a straightforward application of a recent result yields exponential speedup compared to classical heuristics in approximate probabilistic inference, thereby demonstrating another example where advanced quantum resources can potentially prove useful in machine learning.

Exploiting quantum properties to outperform classical ways of information processing is an outstanding goal of modern physics. A promising route is quantum simulation, which aims at implementing relevant and computationally hard problems in controllable quantum systems. Here we demonstrate that in a trapped ion setup, with present day technology, it is possible to realize a spin model of the Mattis-type that exhibits spin glass phases. Our method produces the glassy behaviour without the need for any disorder potential, just by controlling the detuning of the spin-phonon coupling. Applying a transverse field, the system can be used to benchmark quantum annealing strategies which aim at reaching the ground state of the spin glass starting from the paramagnetic phase. In the vicinity of a phonon resonance, the problem maps onto number partitioning, and instances which are difficult to address classically can be implemented.

We review selected advances in the theoretical understanding of complex quantum many-body systems with regard to emergent notions of quantum statistical mechanics. We cover topics such as equilibration and thermalisation in pure state statistical mechanics, the eigenstate thermalisation hypothesis, the equivalence of ensembles, non-equilibration dynamics following global and local quenches as well as ramps. We also address initial state independence, absence of thermalisation, and many-body localisation. We elucidate the role played by key concepts for these phenomena, such as Lieb-Robinson bounds, entanglement growth, typicality arguments, quantum maximum entropy principles and the generalised Gibbs ensembles, and quantum (non-)integrability. We put emphasis on rigorous approaches and present the most important results in a unified language.

Quantum technologies promise a variety of exciting applications. Even though impressive progress has been achieved recently, a major bottleneck currently is the lack of practical certification techniques. The challenge consists of ensuring that classically intractable quantum devices perform as expected. Here we present an experimentally friendly and reliable certification tool for photonic quantum technologies: an efficient certification test for experimental preparations of multimode pure Gaussian states, pure non-Gaussian states generated by linear-optical circuits with Fock-basis states of constant boson number as inputs, and pure states generated from the latter class by post-selecting with Fock-basis measurements on ancillary modes. Only classical computing capabilities and homodyne or hetorodyne detection are required. Minimal assumptions are made on the noise or experimental capabilities of the preparation. The method constitutes a step forward in many-body quantum certification, which is ultimately about testing quantum mechanics at large scales.

In this work, we show how Gibbs or thermal states appear dynamically in closed quantum many-body systems, building on the program of dynamical typicality. We introduce a novel perturbation theorem for physically relevant weak system-bath couplings that is applicable even in the thermodynamic limit. We identify conditions under which thermalization happens and discuss the underlying physics. Based on these results, we also present a fully general quantum algorithm for preparing Gibbs states on a quantum computer with a certified runtime and error bound. This complements quantum Metropolis algorithms, which are expected to be efficient but have no known runtime estimates and only work for local Hamiltonians.

We establish a link between unitary relaxation dynamics after a quench in closed many-body systems and the entanglement in the energy eigenbasis. We find that even if reduced states equilibrate, they can have memory on the initial conditions even in certain models that are far from integrable. We show that in such situations the equilibrium states are still described by a maximum entropy or generalized Gibbs ensemble, regardless of whether a model is integrable or not, thereby contributing to a recent debate. In addition, we discuss individual aspects of the thermalization process, comment on the role of Anderson localization, and collect and compare different notions of integrability.

We investigate decoherence and equilibration in the experimentally relevant situation of weak coupling to an environment. We consider small subsystems of large closed quantum systems that evolve according to the von Neumann equation. Without approximations and without making any special assumptions on the form of the interaction we prove that, for almost all initial states and almost all times, the off-diagonal elements of the density matrix of the subsystem in the eigenbasis of its local Hamiltonian must be small whenever the energy difference of the corresponding eigenstates is larger than the interaction energy. This proves that decoherence with respect to the local energy eigenbasis is a natural property of weakly interacting quantum systems.

We study the dynamic properties of a model for wetting with two competing adsorbates on a planar substrate. The two species of particles have identical properties and repel each other. Starting with a flat interface one observes the formation of homogeneous droplets of the respective type separated by nonwet regions where the interface remains pinned. The wet phase is characterized by slow coarsening of competing droplets. Moreover, in 2+1 dimensions an additional line of continuous phase transition emerges in the bound phase, which separates an unordered phase from an ordered one. The symmetry under interchange of the particle types is spontaneously broken in this region and finite systems exhibit two metastable states, each dominated by one of the species. The critical properties of this transition are analyzed by numeric simulations.