Observation of Wave-Packet Branching through an Engineered Conical Intersection

The topological θ-angle in gauge theories engenders a series of fundamental phenomena, including violations of charge-parity (CP) symmetry, dynamical topological transitions, and confinement-deconfinement transitions. At the same time, it poses major challenges for theoretical studies, as it implies a sign problem in numerical simulations. Analog quantum simulators open the promising prospect of treating quantum many-body systems with such topological terms, but, contrary to their digital counterparts, they have not yet demonstrated the capacity to control the θ-angle. Here, we demonstrate how a tunable topological θ-term can be added to a prototype theory with U(1) gauge symmetry, a discretized version of quantum electrodynamics in one spatial dimension. As we show, the model can be realized experimentally in a single-species Bose-Hubbard model in an optical superlattice with three different spatial periods, thus requiring only standard experimental resources. Through numerical calculations obtained from the time-dependent density-matrix renormalization group method and exact diagonalization, we benchmark the model system, and illustrate how salient effects due to the θ-term can be observed. These include charge confinement, the weakening of quantum many-body scarring, as well as the disappearance of Coleman’s phase transition due to explicit breaking of CP symmetry. This work opens the door towards studying the rich physics of topological gauge-theory terms in large-scale cold-atom quantum simulators.4 MoreReceived 15 April 2022Revised 19 September 2022Accepted 26 September 2022DOI:https://doi.org/10.1103/PRXQuantum.3.040316Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasColor confinementColor deconfinementConfinementQuantum simulationPhysical Systems1-dimensional systemsBose gasesTechniquesBose-Hubbard modelDensity matrix renormalization groupExact diagonalizationGauge symmetriesLattice gauge theoryPerturbation theoryAtomic, Molecular & OpticalCondensed Matter, Materials & Applied Physics

Photoinduced multi-mode quantum dynamics of pyrrole at the [formula omitted]– [formula omitted] conical intersections

Optimal control simulation is used to examine the control mechanisms in the photodissociation of phenol within a two-dimensional, three-electronic-state model with two conical intersections. This model has two channels for H-atom elimination, which correspond to the (2)pi and (2)sigma states of the phenoxyl radical. The optimal pulse that enhances (2)sigma dissociation initially generates a wave packet on the S(1) potential-energy surface of phenol. This wave packet is bifurcated at the S(2)-S(1) conical intersection into two components with opposite phases because of the geometric phase effect. The destructive interference caused by the geometric phase effect reduces the population around the S(1)-S(0) conical intersection, which in turn suppresses nonadiabatic transitions and thus enhances dissociation to the (2)sigma limit. The optimal pulse that enhances S(0) dissociation, on the other hand, creates a wave packet on the S(2) potential-energy surface of phenol via an intensity borrowing mechanism, thus avoiding geometric phase effects at the S(2)-S(1) conical intersection. This wave packet hits the S(1)-S(0) conical intersection directly, resulting in preferred dissociation to the (2)pi limit. The optimal pulse that initially prepares the wave packet on the S(1) potential-energy surface (PES) has a higher carrier frequency than the pulse that prepares the wave packet on the S(2) PES. This counterintuitive effect is explained by the energy-level structure and the S(2)-S(1) vibronic coupling mechanism.

The interplay between matter particles and gauge fields in physical spaces with nontrivial geometries can lead to novel topological quantum matter. However, detailed microscopic mechanisms are often obscure, and unconventional spaces are generally challenging to construct in solids. Highly controllable atomic systems can quantum simulate such physics, even those inaccessible in other platforms. Here, we realize a Bose-Einstein condensate (BEC) on a synthetic cylindrical surface subject to a net radial synthetic magnetic flux. We observe a symmetry-protected topological band structure emerging on this Hall cylinder but disappearing in the planar counterpart. BEC’s transport observed as Bloch oscillations in the band structure is analogous to traveling on a Möbius strip in the momentum space, revealing topological band crossings protected by a nonsymmorphic symmetry. We demonstrate that breaking this symmetry induces a topological transition manifested as gap opening at band crossings, and further manipulate the band structure and BEC’s transport by controlling the axial synthetic magnetic flux. Our work opens the door for using atomic quantum simulators to explore intriguing topological phenomena intrinsic in unconventional spaces.5 MoreReceived 10 August 2021Accepted 7 December 2021DOI:https://doi.org/10.1103/PRXQuantum.3.010316Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasBose-Einstein condensatesQuantum simulationSynthetic gauge fieldsPhysical SystemsUltracold gasesTechniquesAtom & ion coolingAtomic, Molecular & OpticalCondensed Matter, Materials & Applied Physics

Many-body systems of quantum interacting particles in which time-reversal symmetry is broken give rise to a variety of rich collective behaviors and are, therefore, a major target of research in modern physics. Quantum simulators can potentially be used to explore and understand such systems, which are often beyond the computational reach of classical simulation. Of these, platforms with universal quantum control can experimentally access a wide range of physical properties. However, simultaneously achieving strong programmable interactions, strong time-reversal symmetry breaking, and high-fidelity quantum control in a scalable manner is challenging. Here, we realize quantum simulations of interacting, time-reversal-broken quantum systems in a universal trapped-ion quantum processor. Using a recently proposed, scalable scheme, we implement time-reversal-breaking synthetic gauge fields, shown for the first time in a trapped-ion chain, along with unique coupling geometries, potentially extendable to simulation of multidimensional systems. Our high-fidelity single-site resolution in control and measurement, along with highly programmable interactions, allow us to perform full state tomography of a ground state showcasing persistent current and to observe dynamics of a time-reversal-broken system with nontrivial interactions. Our results open a path toward simulation of time-reversal-broken many-body systems with a wide range of features and coupling geometries.4 MoreReceived 4 July 2022Accepted 4 April 2023DOI:https://doi.org/10.1103/PhysRevX.13.021021Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasQuantum simulationQuantum verificationPhysical SystemsTrapped ionsAtomic, Molecular & OpticalQuantum Information

Conical intersection as a dynamic funnel in nonadiabatic transition dictates many important chemical reaction outputs such as reaction rates, yields, and energy disposals especially for chemical reactions taking place on electronically excited states. Therefore, the energetics and topology of conical intersections have been subjected to intensive theoretical and experimental studies for decades as these things are the keys to understanding and controlling nonadiabatic transitions which are ubiquitous in nature. In this article, we focus on πσ*-mediated photodissociation reactions of thiophenols and thioanisoles. Interestingly, for these chemical systems, the nonadiabatic transition probability can be precisely measured as a function of the excitation energy, giving a great opportunity for spectroscopic characterization of the multi-dimensional conical intersection seam that governs the nonadiabatic transition dynamics of polyatomic molecules. The passage of the reactive flux in the proximity of the conical intersection gives rise to dynamic resonances corresponding to dramatic state-specific increases of the nonadiabatic transition probability. Accordingly, it is found that the electronic and nuclear configurations of the reactive flux and their evolution, coupled to the conical intersection seam, are critical in nonadiabatic transition dynamics. Nonadiabaticity is found to be extremely sensitive to the conformational molecular structure, and this has been demonstrated in the photodissociation dynamics of the chemical derivatives of thiophenol. Intramolecular vibrational redistribution, which is nontrivial in surmounting the reaction barrier, is found to wash out state-specific dynamic resonances, implying the importance of the dynamic interplay between vibrational energy flow and nonadiabatic transition. The experimental results on conical intersection dynamics presented in this review provide many interesting and important issues to be pursued in the near future by both theoreticians and experimentalists.

Most experiments with ultracold atoms in optical lattices have contact interactions and therefore operate at high densities of around one atom per site to observe the effect of strong interactions. Strong ranged interactions can be generated via Rydberg dressing, which opens up the path to exploring the physics of few interacting particles. Rather than the unit cells of a crystal, the sites of the optical lattice can now be interpreted as discretized space. This allows the study of completely new types of problems in a familiar architecture. We investigate the possibility of realizing problems akin to those found in quantum chemistry, although with a different scaling law in the interactions. Through numerical simulation, we show that simple pseudoatoms and pseudomolecules could be prepared with high fidelity in state-of-the-art experiments.Received 12 December 2022Revised 7 February 2023Accepted 22 February 2023DOI:https://doi.org/10.1103/PRXQuantum.4.020301Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasCold gases in optical latticesQuantum simulationAtomic, Molecular & OpticalQuantum Information

We report on the spectra and dynamics of H3 near the conical intersection in its (2p)1E′ ground electronic manifold. The time-dependent wave packet approach and the double many-body expansion (DMBE) potential energy surface (PES) are employed for this purpose. We use Jacobi coordinates (R,r,γ) and employ the fast Fourier transform method for R and r, and the discrete variable representation method for γ, in conjunction with the split-operator formalism to describe the evolution of the wave packet (WP) in space and time, respectively. While the main focus of the present work is to explicitly reveal the effects of nonadiabatic coupling between the two sheets of the DMBE PES, companion calculations are also carried out to investigate the dynamics on the uncoupled upper and lower adiabatic sheets, both in two and three dimensions (for total angular momentum J=0). A set of pseudospectra is calculated by Fourier transforming the time autocorrelation function of suitably chosen Gaussian wave packets located initially at the minimum energy point of the seam of conical intersections. The eigenstates thus obtained are assigned by computing their eigenfunctions by spectral quantization. In the coupled states treatment the WP is propagated in the diabatic representation. The time dependence of the adiabatic populations is calculated by using suitable adiabatic projection operators. We find strong effects of nonadiabatic coupling on the discrete vibrational energy levels of the upper adiabatic sheet, which all change to quasibound states in the coupled manifold. The comparison of the decay dynamics of various levels of the upper adiabatic sheet indicates considerable mode specificity (their lifetimes typically vary between 3 and 6 fs). On the other hand, resonances are seen to be less pronounced near the conical intersection on the lower adiabatic sheet (when compared to those in the literature, obtained near the collinear saddle point region). The effect of nonadiabatic coupling on them is only minor. We also report preliminary results on the optical emission spectrum of H3 and compare them with the experimental findings.

We present a method based on the scattering T operator, and conservation of net real and reactive power, to provide physical bounds on any electromagnetic design objective that can be framed as a net radiative emission, scattering or absorption process. Application of this approach to plane-wave scattering from an arbitrarily shaped, compact body of homogeneous electric susceptibility χ is found to predictively quantify and differentiate the relative performance of dielectric and metallic materials across all optical length scales. When the size of a device is restricted to be much smaller than the wavelength (a subwavelength cavity, antenna, nanoparticle, etc.), the maximum cross-section enhancement that may be achieved via material structuring is found to be much weaker than prior predictions: the response of strong metals (Reχ≪0) exhibits a diluted (homogenized) effective medium scaling ∝χ/Imχ; below a threshold size inversely proportional to the index of refraction (consistent with the half-wavelength resonance condition), the maximum cross-section enhancement possible with dielectrics (Reχ>0) shows the same material dependence as Rayleigh scattering. In the limit of a bounding volume much larger than the wavelength in all dimensions, achievable scattering interactions asymptote to the geometric area, as predicted by ray optics. For representative metal and dielectric materials, geometries capable of scattering power from an incident plane wave within an order of magnitude (typically a factor of two) of the bound are discovered by inverse design. The basis of the method rests entirely on scattering theory and can thus likely be applied to acoustics, quantum mechanics, and other wave physics.Received 27 March 2020Revised 17 June 2020Accepted 10 July 2020DOI:https://doi.org/10.1103/PhysRevResearch.2.033172Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasElectromagnetismGeometrical & wave opticsLight propagation, transmission & absorptionMetamaterialsMie scatteringPhotonicsPlasmonicsScattering theoryAtomic, Molecular & OpticalGeneral Physics

Randomness is a defining element of mixing processes in nature and an essential ingredient to many protocols in quantum information. In this work, we investigate how much randomness is required to transform a given quantum state into another one. Specifically, we ask whether there is a gap between the power of a classical source of randomness compared to that of a quantum one. We provide a complete answer to these questions, by identifying provably optimal protocols for both classical and quantum sources of randomness, based on a dephasing construction. We find that in order to implement any noisy transition on a d-dimensional quantum system it is necessary and sufficient to have a quantum source of randomness of dimension d or a classical one of dimension d. Interestingly, coherences provided by quantum states in a source of randomness offer a quadratic advantage. The process we construct has the additional features to be robust and catalytic; i.e., the source of randomness can be reused. Building upon this formal framework, we illustrate that this dephasing construction can serve as a useful primitive in both equilibration and quantum information theory: We discuss applications describing the smallest measurement device, capturing the smallest equilibrating environment allowed by quantum mechanics, or forming the basis for a cryptographic private quantum channel. We complement the exact analysis with a discussion of approximate protocols based on quantum expanders deriving from discrete Weyl systems. This gives rise to equilibrating environments of remarkably small dimension. Our results highlight the curious feature of randomness that residual correlations and dimension can be traded against each other.Received 13 June 2018Revised 21 August 2018DOI:https://doi.org/10.1103/PhysRevX.8.041016Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasQuantum channelsQuantum correlations in quantum informationQuantum cryptographyQuantum quenchThermodynamicsQuantum InformationInterdisciplinary Physics

We derive a reduced model for the nonadiabatic quantum dynamics of an electronic wave packet moving through a conical intersection in the presence of strong vibrational damping. Starting from the dissipative two-state two-model model, we transform the tuning and the coupling mode to the bath. The resulting quantum two-state model with two highly structured environments is solved numerically exactly in the regime of strong vibrational damping. We find negative cross peaks in the ultrafast optical 2D spectra as clear signatures of the conical intersection. They arise from secondary excitations of the wave packet after having passed through the photophysical energy funnel. This feature is in agreement with recent transient absorption measurements of rhodopsin.

We present a quantum algorithm for the dynamical simulation of time-dependent Hamiltonians. Our method involves expanding the interaction-picture Hamiltonian as a sum of generalized permutations, which leads to an integral-free Dyson series of the time-evolution operator. Under this representation, we perform a quantum simulation for the time-evolution operator by means of the linear combination of unitaries technique. We optimize the time steps of the evolution based on the Hamiltonian’s dynamical characteristics, leading to a gate count that scales with an L<sup>1</sup>-norm-like scaling with respect only to the norm of the interaction Hamiltonian, rather than that of the total Hamiltonian. We demonstrate that the cost of the algorithm is independent of the Hamiltonian’s frequencies, implying its advantage for systems with highly oscillating components, and for time-decaying systems the cost does not scale with the total evolution time asymptotically. In addition, our algorithm retains the near optimal log (1/ϵ)/loglog(1/ϵ) scaling with simulation error ϵ.

[This paper is part of the Focused Collection on Upper Division Physics Courses.] Compared with introductory physics, relatively little is known about the development of expertise in advanced physics courses, especially in the case of quantum mechanics. Here, we describe a framework for understanding the patterns of student reasoning difficulties and how students develop expertise in quantum mechanics. The framework posits that the challenges many students face in developing expertise in quantum mechanics are analogous to the challenges introductory students face in developing expertise in introductory classical mechanics. This framework incorporates both the effects of diversity in upper-level students’ prior preparation, goals, and motivation in general (i.e., the facts that even in upper-level courses, students may be inadequately prepared, have unclear goals, and have insufficient motivation to excel) as well as the “paradigm shift” from classical mechanics to quantum mechanics. The framework is based on empirical investigations demonstrating that the patterns of reasoning, problem-solving, and self-monitoring difficulties in quantum mechanics bear a striking resemblance to those found in introductory classical mechanics. Examples from research in quantum mechanics and introductory classical mechanics are discussed to illustrate how the patterns of difficulties are analogous as students learn to unpack the respective principles and grasp the formalism in each knowledge domain during the development of expertise. Embracing such a framework and contemplating the parallels between the difficulties in these two knowledge domains can enable researchers to leverage the extensive literature for introductory physics education research to guide the design of teaching and learning tools for helping students develop expertise in quantum mechanics.Received 29 September 2014DOI:https://doi.org/10.1103/PhysRevSTPER.11.020119This article is available under the terms of the Creative Commons Attribution 3.0 License. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical Society

The ultrafast nonadiabatic dynamics of a two-electronic-state four-vibrational-mode conical intersection coupled to a finite bath with up to 20 harmonic oscillators has been investigated by employing the multiple Davydov D2 ansatz. It is demonstrated, using the multi-configuration time-dependent Hartree method as a benchmark, that this approach provides an efficient and robust description of the internal conversion process at multimode conical intersections. Thanks to the Gaussian nature of the Davydov ansatz, it allows for numerically accurate simulations of time-dependent diabatic and (for the first time for a 24-mode system) adiabatic populations of the electronic states and reduced probability densities of the tuning and coupling modes. The obtained adiabatic populations and wave packets can be used as benchmarks for the testing of various simulation methods, in particular, surface-hopping methods.

The ground-, (1)(pipi*)-, and (3)(pipi*)-state potential-energy surfaces of 1,2-cyclononadiene and isomeric C(9)H(14) species, as well as 1-methyl-1,2-cyclononadiene and isomeric C(10)H(16) species were all mapped using CASSCF and the 6-31G(d) basis set. Theoretical results were found to be in good agreement with the available experimental observations for both 1,2-cyclononadiene and 1-methyl-1,2-cyclononadiene isomerization reactions under singlet and triplet direct or sensitized irradiation. Extremely efficient decay occurs from the first singlet excited state to the ground state through at least three different conical intersections (surface crossings). The first of these crossing points is accessed by a one-bond ring closure. From this conical intersection point (CI-A or CI-C), some possible subsequent ground-state reaction paths have been identified: 1) intramolecular C--H bond insertion to form the bicyclic photoproduct and 2) intramolecular C--H bond insertion to form tricyclic photoproducts. An excited state [1,3]-sigmatropic shift leads to the second conical intersection (CI-B or CI-E), which can give a three-bond cyclononyne species. Besides these, in the singlet photochemical reactions of 1-methyl-1,2-cyclononadiene, excited-state, one allenic C--H bond insertion leads to a third conical intersection (CI-D). Possible ground-state reaction pathways from this structure lead to the formation of a diene photoproduct or to transannular insertion photoproducts. Moreover, in the case of triplet 1,2-cyclononadiene and 1-methyl-1,2-cyclononadiene photoisomerization reactions, both chemical reactions will adopt a 1,3-biradical (T(1)/S(0)-1, T(1)/S(0)-2, and T(1)/S(0)-3), which may undergo intersystem crossings leading to the formation of tricyclic or bicyclic photoproducts. The results obtained allow a number of predictions to be made.