Exact Quantum Research Articles

Toward a Correct Description of Initial Electronic Coherence in Nonadiabatic Dynamics Simulations.

The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat electronic coherence. However, the most popular and practical nonadiabatic molecular dynamics techniques, Tully's fewest-switches surface hopping and Ehrenfest mean-field dynamics, are unable to describe the dynamics proceeding from an initial electronic coherence. While such issues are not encountered with the analogous coupled-trajectory algorithms or numerically exact quantum dynamics methods, applying such techniques necessarily comes with a higher computational cost. Here we show that a correct description of initial electronic coherence can indeed be achieved using independent-trajectory methods derived from the semiclassical mapping formalism. The key is the introduction of an initial sampling over the electronic phase space and a means of incorporating phase interference between trajectories, both of which are naturally achieved when working within the semiclassical mapping framework.

Exact quantum dynamics for two-level systems with time-dependent driving

Abstract It is well known that the time-dependent Schrrödinger equation can only be solved exactly in very rare cases, even for two-level quantum systems. Thus, finding the exact quantum dynamics under a time-dependent Hamiltonian is not only fundamentally important in quantum physics but also facilitates active quantum manipulations for quantum information processing. In this work, we present a method for generating nearly infinite analytically assisted solutions to the Schrrödinger equation for a qubit under time-dependent driving. These analytically assisted solutions feature free parameters with only boundary restrictions, making them applicable in a variety of precise quantum manipulations. Due to the general form of the time-dependent Hamiltonian in our approach, it can be readily implemented in various experimental setups involving qubits. Consequently, our scheme offers new solutions to the Schrrödinger equation, providing an alternative analytical framework for precise control over qubits.

Extending Non-Perturbative Simulation Techniques for Open-Quantum Systems to Excited-State Proton Transfer and Ultrafast Non-Adiabatic Dynamics.

Excited state proton transfer is an ubiquitous phenomenon in biology and chemistry, spanning from the ultrafast reactions of photobases and acids to light-driven, enzymatic catalysis and photosynthesis. However, the simulation of such dynamics involves multiple challenges, since high-dimensional, out-of-equilibrium vibronic states play a crucial role, while a fully quantum description of the proton's dissipative, real-space dynamics is also required. In this work, we extend the powerful matrix product state approach to open quantum systems (TEDOPA) to study these demanding dynamics, and also more general nonadiabatic processes that can appear in complex photochemistry subject to strong laser driving. As an illustration, we initially consider an open model of a four-level electronic system interacting with hundreds of intramolecular vibrations that drive ultrafast excited state proton transfer, as well as an explicit photonic environment that allows us to directly monitor the resulting dual fluorescence in this system. We then demonstrate how to include a continuous "reaction coordinate" of the proton transfer that allows numerically exact simulations that can be understood, visualized and interpreted in the familiar language of diabatic and adiabatic dynamics on potential surfaces, while also retaining an exact quantum treatment of dissipation and driving effects that could be used to study diverse problems in ultrafast photochemistry.

Emergence of the Molecular Geometric Phase from Exact Electron-Nuclear Dynamics.

Geometric phases play a crucial role in diverse fields. In molecules, they appear when a reaction path encircles an intersection between adiabatic potential energy surfaces and the molecular wave function experiences quantum-mechanical interference effects. This intriguing effect, closely resembling the magnetic Aharonov-Bohm effect, crucially relies on the adiabatic description of the dynamics, and it is an open issue whether and how it persists in an exact quantum dynamical framework. Recent works suggest that the molecular geometric phase is an artifact of the adiabatic approximation, thereby challenging the entire concept. Here, building upon a recent investigation (Martinazzo, R.; Burghardt, I. Phys. Rev. Lett. 2024, 132, 243002), we address this issue using the exact factorization of the total wave function. We introduce instantaneous gauge-invariant phases separately for the electrons and nuclei and use them to monitor the phase difference between the trailing edges of a wavepacket encircling a conical intersection between adiabatic surfaces. The transition from the time-dependent open-path phase differences to the closed-path limit is examined, revealing how the phase differences in the electronic and nuclear subspaces compensate for each other upon path closure. In this way, we unambiguously demonstrate the role of the geometric phase in the interference process and shed light on its persistence beyond the adiabatic approximation.

Robust finite-temperature many-body scarring on a quantum computer

Mechanisms for suppressing thermalization in disorder-free many-body systems, such as Hilbert space fragmentation and quantum many-body scars, have recently attracted much interest in foundations of quantum statistical physics and potential quantum information processing applications. However, their sensitivity to realistic effects such as finite temperature remains largely unexplored. Here, we have utilized IBM's Kolkata quantum processor to demonstrate an unexpected robustness of quantum many-body scars at finite temperatures when the system is prepared in a thermal Gibbs ensemble. We identify such robustness in the PXP model, which describes quantum many-body scars in experimental systems of Rydberg atom arrays and ultracold atoms in tilted Bose-Hubbard optical lattices. By contrast, other theoretical models which host exact quantum many-body scars are found to lack such robustness and their scarring properties quickly decay with temperature. Our study sheds light on the important differences between scarred models in terms of their algebraic structures, which impacts their resilience to finite temperature. Published by the American Physical Society 2024

Recovering the Original Simplicity: Succinct and Exact Quantum Algorithm for the Welded Tree Problem

Recovering the Original Simplicity: Succinct and Exact Quantum Algorithm for the Welded Tree Problem

Atomically Thin Two-Dimensional Kagome Flat Band on the Silicon Surface.

In condensed matter physics, the Kagome lattice and its inherent flat bands have attracted considerable attention for their prediction and observation to host a variety of exotic physical phenomena. Despite extensive efforts to fabricate thin films of Kagome materials aimed at modulating flat bands through electrostatic gating or strain manipulation, progress has been limited. Here, we report the observation of a d-orbital hybridized Kagome-derived flat band in Ag/Si(111) as revealed by angle-resolved photoemission spectroscopy. Our findings indicate that silver atoms on a silicon substrate form an unconventional distorted breathing Kagome structure, where a delicate balance in the hopping parameters of the in-plane d-orbitals leads to destructive interference, resulting in double flat bands. The exact quantum destructive interference mechanism that forms the flat band is uncovered in a rigorous manner that has not been described before. These results illuminate the potential for integrating metal-semiconductor interfaces on semiconductor surfaces into Kagome physics, particularly in exploring the flat bands of ideal 2D Kagome systems.

A stochastic Schrödinger equation and matrix product state approach to carrier transport in organic semiconductors with nonlocal electron-phonon interaction.

Evaluation of the charge transport property of organic semiconductors requires exact quantum dynamics simulation of large systems. We present a numerically nearly exact approach to investigate carrier transport dynamics in organic semiconductors by extending the non-Markovian stochastic Schrödinger equation with complex frequency modes to a forward-backward scheme and by solving it using the matrix product state (MPS) approach. By utilizing the forward-backward formalism for noise generation, the bath correlation function can be effectively treated as a temperature-independent imaginary part, enabling a more accurate decomposition with fewer complex frequency modes. Using this approach, we study the carrier transport and mobility in the one-dimensional Peierls model, where the nonlocal electron-phonon interaction is taken into account. The reliability of this approach was validated by comparing carrier diffusion motion with those obtained from the hierarchical equations of motion method across various parameter regimes of the phonon bath. The efficiency was demonstrated by the modest virtual bond dimensions of MPS and the low scaling of the computational time with the system size.

Decomposing Imaginary-Time Feynman Diagrams Using Separable Basis Functions: Anderson Impurity Model Strong-Coupling Expansion

We present a deterministic algorithm for the efficient evaluation of imaginary-time diagrams based on the recently introduced discrete Lehmann representation (DLR) of imaginary-time Green’s functions. In addition to the efficient discretization of diagrammatic integrals afforded by its approximation properties, the DLR basis is separable in imaginary-time, allowing us to decompose diagrams into linear combinations of nested sequences of one-dimensional products and convolutions. Focusing on the strong-coupling bold-line expansion of generalized Anderson impurity models, we show that our strategy reduces the computational complexity of evaluating an Mth-order diagram at inverse temperature β and spectral width ωmax from O((βωmax)2M−1) for a direct quadrature to O(M(log(βωmax))M+1), with controllable high-order accuracy. We benchmark our algorithm using third-order expansions for multiband impurity problems with off-diagonal hybridization and spin-orbit coupling, presenting comparisons with exact diagonalization and quantum Monte Carlo approaches. In particular, we perform a self-consistent dynamical mean-field theory calculation for a three-band Hubbard model with strong spin-orbit coupling representing a minimal model of Ca2RuO4, demonstrating the promise of the method for modeling realistic strongly correlated multiband materials. For both strong and weak coupling expansions of low and intermediate order, in which diagrams can be enumerated, our method provides an efficient, straightforward, and robust blackbox evaluation procedure. In this sense, it fills a gap between diagrammatic approximations of the lowest order, which are simple and inexpensive but inaccurate, and those based on Monte Carlo sampling of high-order diagrams. Published by the American Physical Society 2024

Exact quantization conditions and full transseries structures for PT symmetric anharmonic oscillators

We study exact Wentzel–Kramers–Brillouin analysis (EWKB) for a PT symmetric quantum mechanics (QM) defined by the potential VPT(x)=ω2x2+gx2K(ix)ϵ with ω∈R≥0, g∈R>0 and K,ϵ∈N to clarify its perturbative/nonperturbative structure. In our analysis, we mainly consider the massless cases, i.e., ω=0, and derive the exact quantization conditions (QCs) for arbitrary (K,ϵ) including all perturbative/nonperturbative corrections. From the exact QCs, we clarify full transseries structure of the energy spectra with respect to the inverse energy level expansion, and then formulate the Gutzwiller trace formula, the spectral summation form, and the Euclidean path integral. For the massive cases, i.e., ω>0, we show the fact that, by requiring the existence of the solution of the exact QCs, the path of analytic continuation in EWKB is uniquely determined for a given N=2K+ϵ, and in consequence the exact QCs, the energy spectra, and the three formulas are all perturbative. Similarities to Hermitian QMs and resurgence are also discussed as additional remarks. Published by the American Physical Society 2024

Reconstructing the spatial structure of quantum correlations in materials

Quantum correlations are a fundamental property of quantum many-body states. Yet they remain experimentally elusive, hindering certification of genuine quantum behavior, especially in quantum materials. Here we show that the momentum-dependent dynamical susceptibility measured via inelastic neutron scattering enables the systematic reconstruction of a general family of quantum correlation functions, which express the degree of quantum coherence in the fluctuations of two spins at an arbitrary mutual distance. Using neutron scattering data for the compound KCuF3—a system of weakly coupled S=1/2 Heisenberg chains—and numerically exact quantum Monte Carlo data, we show that quantum correlations possess a radically different spatial structure with respect to conventional correlations. Indeed, they exhibit a different emergent length scale—the quantum coherence length—which is finite at any finite temperature (including when long-range magnetic order develops). Moreover, we show theoretically that coupled Heisenberg spin chains exhibit a form of quantum monogamy, with a trade-off between quantum correlations along and transverse to the spin chains. These results highlight real-space quantum correlators as an informative, model-independent means of probing the underlying quantum state of real quantum materials. Published by the American Physical Society 2024

Theory and quantum dynamics simulations of exciton-polariton motional narrowing.

The motional narrowing effect has been extensively studied for cavity exciton-polariton systems in recent decades both experimentally and theoretically, which is featured by (1) the subaverage behavior and (2) the asymmetric linewidths for the upper polariton and the lower polariton. However, a minimal theoretical model that is clear and adequate to address all these effects as well as the linewidth scaling relations remains missing. In this work, based on the single mode 1D Holstein-Tavis-Cummings (HTC) model, we studied the motional narrowing effect of the polariton linear absorption spectra via both semi-analytic derivations and numerically exact quantum dynamics simulations using the hierarchical equations of motion approach. The results reveal that under collective light-matter coupling between a cavity mode and N molecules, the polariton linewidth scales as 1/N under the slow limit, while scales as 1/N under the fast limit, due to the polaron decoupling effect. Furthermore, by varying the detunings, the polariton linewidths exhibit significant motional narrowing, covering both characters mentioned above. Our analytic linewidth expressions [Eqs. (34) and (35)] agree well with the numerical exact simulations in all the parameter regimes we explored. These results indicate that the physics of motional narrowing is adequately accounted for by the single-mode 1D HTC model. We envision that both the numerical results and the analytic polariton linewidths expression presented in this work will offer great theoretical value for providing a better understanding of the exciton-polariton motional narrowing based on the HTC model.

Exact-factorisation study of the photochemistry of phenol

We present an analysis of the performance of the coupled-trajectory schemes for nonadiabatic dynamics derived from the exact factorisation of the electron-nuclear wavefunction and implemented in the G-CTMQC code. These algorithms can be seen as variations of the standard Ehrenfest method and Tully surface hopping, which are based, however, on independent trajectories. The reported analysis aims to compare the coupled-trajectory and independent-trajectory schemes, and to benchmark the numerical results against exact quantum wavepacket dynamics. To this end, we employ an analytical molecular model with two nuclear degrees of freedom and three electronic states that allows us to describe the photo-induced hydrogen dissociation in phenol. The analysis focuses on different electronic and nuclear properties calculated along the nonadiabatic dynamics of phenol.

Chiral edge transport along domain walls in magnetic topological insulator nanoribbons

Quantum anomalous Hall insulators are topologically characterized by non-zero integer Chern numbers, the sign of which depends on the direction of the exchange field that breaks time-reversal symmetry. This feature allows the manipulation of the conducting chiral edge states present at the interface of two magnetic domains with opposite magnetization and opposite Chern numbers. Motivated by this broad understanding, the present study investigates the quantum transport properties of a magnetized Bi2Se3 topological insulator nanoribbon with a domain wall (DW) oriented either parallel or perpendicular to the transport direction. Employing an atomistic tight-binding model and a non-equilibrium Green’s function formalism, we calculate the quantum conductance and explore the nature of the edge states. We elucidate the conditions leading to exact conductance quantization and identify the origin of deviations from this behavior. Our analysis shows that although the conductance is quantized in the presence of the horizontal DW, the quantization is absent in the perpendicular DW case. Furthermore, the investigation of the spin character of the edge modes confirms that the conductance in the horizontal DW configuration is spin polarized. This finding underscores the potential of our system as a simple three dimensional spin-filter device.

Topological boundaries of representations and coideals

For a locally compact quantum group G, a (left) coideal is a (left) G-invariant von Neumann subalgebra of L∞(G). We introduce and analyze various generalizations of amenability and coamenability to coideals of discrete and compact quantum groups. We focus on a particular class of coideals found in the category of compact quantum groups, which are associated with a compact quasi-subgroup. This class includes all coideals of the quotient type. We also introduce the notion of a Furstenberg-Hamana boundary for representations of discrete quantum groups and use it to study amenability and coamenability properties of coideals. We then prove that a coideal of a compact quantum group that is associated with a compact quasi-subgroup is coamenable if and only if its codual coideal is G-injective. If G is a unimodular or an exact discrete quantum group, we can replace G-injectivity in the latter statement with the weaker condition of relative amenability. This result leads to a complete characterization of the unique trace property. Specifically, a unimodular discrete quantum group G has the unique trace property if and only if the action of G on its noncommutative Furstenberg boundary is faithful. We also demonstrated that if a unimodular discrete quantum group G is C⁎-simple then it has the unique trace property. These findings are the quantum analogs of the groundbreaking results of Breuillard, Kalantar, Kennedy, and Ozawa and they provide answers to questions posted by Kalantar, Kasprzak, Skalski, and Vergnioux.

Extending non-adiabatic rate theory to strong electronic couplings in the Marcus inverted regime

Electron transfer reactions play an essential role in many chemical and biological processes. Fermi’s golden rule (GR), which assumes that the coupling between electronic states is small, has formed the foundation of electron transfer rate theory; however, in short range electron/energy transfer reactions, this coupling can become very large, and, therefore, Fermi’s GR fails to make even qualitatively accurate rate predictions. In this paper, I present a simple modified GR theory to describe electron transfer in the Marcus inverted regime at arbitrarily large electronic coupling strengths. This theory is based on an optimal global rotation of the diabatic states, which makes it compatible with existing methods for calculating GR rates that can account for nuclear quantum effects with anharmonic potentials. Furthermore, the optimal GR (OGR) theory can also be combined with analytic theories for non-adiabatic rates, such as Marcus theory and Marcus–Levich–Jortner theory, offering clear physical insights into strong electronic coupling effects in non-adiabatic processes. OGR theory is also tested on a large set of spin-boson models and an anharmonic model against exact quantum dynamics calculations, where it performs well, correctly predicting rate turnover at large coupling strengths. Finally, an example application to a boron-dipyrromethane–anthracene photosensitizer reveals that strong coupling effects inhibit excited state charge recombination in this system, reducing the rate of this process by a factor of 4. Overall, OGR theory offers a new approach to calculating electron transfer rates at strong couplings, offering new physical insights into a range of non-adiabatic processes.

Real-time dynamics of the Schwinger model as an open quantum system with Neural Density Operators

Ab-initio simulations of multiple heavy quarks propagating in a Quark-Gluon Plasma are computationally difficult to perform due to the large dimension of the space of density matrices. This work develops machine learning algorithms to overcome this difficulty by approximating exact quantum states with neural network parametrisations, specifically Neural Density Operators. As a proof of principle demonstration in a QCD-like theory, the approach is applied to solve the Lindblad master equation in the 1 + 1d lattice Schwinger Model as an open quantum system. Neural Density Operators enable the study of in-medium dynamics on large lattice volumes, where multiple-string interactions and their effects on string-breaking and recombination phenomena can be studied. Thermal properties of the system at equilibrium can also be probed with these methods by variationally constructing the steady state of the Lindblad master equation. Scaling of this approach with system size is studied, and numerical demonstrations on up to 32 spatial lattice sites and with up to 3 interacting strings are performed.

Giant caloric effects in spin-chain materials

The giant electro- and elastocaloric effects in spin-chain materials are predicted. The theory is based on the exact quantum mechanical solution of the problem. It is shown that the giant jumps in the entropy and the temperature caused by the caloric effect are weakly affected by the initial temperature. The effect can be used for the cooling of new quantum devices (like systems of qubits in quantum computers). On the other hand, since large changes are predicted in the narrow neighborhood of the critical point, the predicted effect can be used in ultrasensitive electric and stress sensors for modern microelectronics. Published by the American Physical Society 2024

Detailed Complementary Consistency: Wave Function Tells Particle How to Hop, Particle Tells Wave Function How to Collapse.

In mixed quantum-classical dynamics, the quantum subsystem can have both wave function and particle-like descriptions. However, they may yield inconsistent results for the expectation value of the same physical quantity. We here propose a novel detailed complementary consistency (DCC) method based on the principle of detailed internal consistency. Namely, the wave function along each trajectory tells the particle how to hop, while the particle tells the wave function how to collapse based on active states in the trajectory ensemble. As benchmarked in a diverse array of representative models with localized nonadiabatic couplings, DCC not only achieves fully consistent results (i.e., identical populations calculated based on wave functions and active states) but also closely reproduces the exact quantum results. Due to the high performance, our new DCC method has great potential to give a consistent and accurate mixed quantum-classical description of general nonadiabatic dynamics after further development.

Near-Optimal Performance of Quantum Error Correction Codes.

The Knill-Laflamme conditions distinguish exact quantum error correction codes, and they have played a critical role in the discovery of state-of-the-art codes. However, the family of exact codes is a very restrictive one and does not necessarily contain the best-performing codes. Therefore, it is desirable to develop a generalized and quantitative performance metric. In this Letter, we derive the near-optimal channel fidelity, a concise and optimization-free metric for arbitrary codes and noise. The metric provides a narrow two-sided bound to the optimal code performance, and it can be evaluated with exactly the same input required by the Knill-Laflamme conditions. We demonstrate the numerical advantage of the near-optimal channel fidelity through multiple qubit code and oscillator code examples. Compared to conventional optimization-based approaches, the reduced computational cost enables us to simulate systems with previously inaccessible sizes, such as oscillators encoding hundreds of average excitations. Moreover, we analytically derive the near-optimal performance for the thermodynamic code and the Gottesman-Kitaev-Preskill code. In particular, the Gottesman-Kitaev-Preskill code's performance under excitation loss improves monotonically with its energy and converges to an asymptotic limit at infinite energy, which is distinct from other oscillator codes.