Non-orthogonal State Research Articles

Quantum computing with time-travelling quantum gates

Quantum computing can solve problems that are difficult to solve in classical computing, expanding the range of problems that can be effectively computed within the allowable range of classical physical principles, and posing a challenge to the extended Church-Turing thesis in classical computing. Here, we discuss an interesting question: how to achieve more powerful computers by breaking through the limitations of physical principles, further enhancing the capabilities of quantum computers. To extend quantum computing, novel operations related to relativistic physics are a crucial candidate. Among them, the concept of closed time-like curve has aroused widespread interest, and it introduces the ability for time travel. Mathematically, quantum state along the closed time-like curve is determined through self-consistent equations, which has been demonstrated in simulations. Here, we consider a novel manipulation capability that allows quantum computing to achieve time-travelling quantum control gate. This is an intuitive extension of the graphical language of quantum circuits. Explaining quantum circuits as tensor networks, we first explain how to experimentally simulate the output of such a circuit in a system without time-travel capability. Then, we take an example to demonstrate an extended quantum algorithm that can efficiently solve SAT problems, indicating that with the involvement of time-travelling quantum gates, the computational complexity class P = NP. We also anticipate that the time-travelling quantum gates will play a facilitating role in accomplishing other quantum tasks, including achieving deterministic non-orthogonal quantum state discrimination, and quantum state cloning. Our results contribute to a more in-depth understanding of the relationship between computation and physical principles.

Leveling the Mountain Range of Excited-State Benchmarking through Multistate Density Functional Theory.

The performance of multistate density functional theory (MSDFT) with nonorthogonal state interaction (NOSI) is assessed for 100 vertical excitation energies against the theoretical best estimates extracted to the full configuration interaction accuracy on the database developed by Loos et al. in 2018 (Loos2018). Two optimization techniques, namely, block-localized excitation and target state optimization, are examined along with two ways of estimating the transition density functional (TDF) for the correlation energy of the Hamiltonian matrix density functional. The results from the two optimization methods are similar. It was found that MSDFT-NOSI using the spin-multiplet degeneracy constraint for the TDF of spin-coupling interaction, along with the M06-2X functional, yields a root-mean-square error (RMSE) of 0.22 eV, which performs noticeably better than time-dependent density functional theory (DFT) at an RMSE of 0.43 eV using the same functional and basis set on the Loos2018 database. In comparison with wave function theory, NOSI has smaller errors than CIS(D∞), LR-CC2, and ADC(3) all of which have an RMSE of 0.28 eV, but somewhat greater than STEOM-CCSD (RMSE of 0.14 eV) and LR-CCSD (RMSE of 0.11 eV) wave function methods. In comparison with Kohn-Sham (KS) DFT calculations, the multistate DFT approach has little double counting of correlation. Importantly, there is no noticeable difference in the performance of MSDFT-NOSI on the valence, Rydberg, singlet, triplet, and double-excitation states. Although the use of another hybrid functional PBE0 leads to a greater RMSE of 0.36 eV, the deviation is systematic with a linear regression slope of 0.994 against the results with M06-2X. The present benchmark reveals that density functional approximations developed for KS-DFT for the ground state with a noninteracting reference may be adopted in MSDFT calculations in which the state interaction is key.

Excimer Energies.

A multistate energy decomposition analysis (MS-EDA) method is introduced for excimers using density functional theory. Although EDA has been widely applied to intermolecular interactions in the ground state, few methods are currently available for excited-state complexes. Here, the total energy of an excimer state is separated into exciton excitation energy ΔEEx(|ΨX·ΨY⟩*), resulting from the state interaction between locally excited monomer states |ΨX*·ΨY⟩ and |ΨX·ΨY*⟩ , a superexchange stabilization energy ΔESE, originating from the mutual charge transfer between two monomers |ΨX+·ΨY⟩ and |ΨX-·ΨY+⟩ , and an orbital-and-configuration delocalization term ΔEOCD due to the expansion of configuration space and block-localized orbitals to the fully delocalized dimer system. Although there is no net charge transfer in symmetric excimer cases, the resonance of charge-transfer states is critical to stabilizing the excimer. The monomer localized excited and charge-transfer states are variationally optimized, forming a minimal active space for nonorthogonal state interaction (NOSI) calculations in multistate density functional theory to yield the intermediate states for energy analysis. The present MS-EDA method focuses on properties unique to excited states, providing insights into exciton coupling, superexchange and delocalization energies. MS-EDA is illustrated on the acetone and pentacene excimer systems; three configurations of the latter case are examined, including the optimized excimer, a stacked configuration of two pentacene molecules and the fishbone orientation. It is found that excited-state energy splitting is strongly dependent on the relative energies of the monomer excited states and the phase-matching of the monomer wave functions.

Target State Optimized Density Functional Theory for Electronic Excited and Diabatic States.

A flexible self-consistent field method, called target state optimization (TSO), is presented for exploring electronic excited configurations and localized diabatic states. The key idea is to partition molecular orbitals into different subspaces according to the excitation or localization pattern for a target state. Because of the orbital-subspace constraint, orbitals belonging to different subspaces do not mix. Furthermore, the determinant wave function for such excited or diabatic configurations can be variationally optimized as a ground state procedure, unlike conventional ΔSCF methods, without the possibility of collapsing back to the ground state or other lower-energy configurations. The TSO method can be applied both in Hartree-Fock theory and in Kohn-Sham density functional theory (DFT). The density projection procedure and the working equations for implementing the TSO method are described along with several illustrative applications. For valence excited states of organic compounds, it was found that the computed excitation energies from TSO-DFT and time-dependent density functional theory (TD-DFT) are of similar quality with average errors of 0.5 and 0.4 eV, respectively. For core excitation, doubly excited states and charge-transfer states, the performance of TSO-DFT is clearly superior to that from conventional TD-DFT calculations. It is shown that variationally optimized charge-localized diabatic states can be defined using TSO-DFT in energy decomposition analysis to gain both qualitative and quantitative insights on intermolecular interactions. Alternatively, the variational diabatic states may be used in molecular dynamics simulation of charge transfer processes. The TSO method can also be used to define basis states in multistate density functional theory for excited states through nonorthogonal state interaction calculations. The software implementing TSO-DFT can be accessed from the authors.

Quantum Key Distribution Based on Orthogonal State Encoding

Quantum key distribution(QKD) is one of the most significant areas in quantum information theory. For nearly four decades, substantial QKD schemes are developed. In early years, the security of QKD protocols is depend on switching different bases, namely based on non-orthogonal state encoding. The most famous example is the BB84 protocol. Later, other techniques were developed for orthogonal state encoding. Examples of such protocols include the GV protocol and order-rearrangement protocols. In this paper, we present two QKD protocols based on orthogonal state encoding. One of them does not need to employ order-rearrangement techniques while the other needs to. We provide analyses for them, demonstrating that they are highly efficient when considering consumptions of both qubits and classical bits. Furthermore, the employment of maximally entangled states could be less than previous ones and so the measurement efficiency could be increased. We also modify the protocols for implementing in noisy channels by applying the testing state method.

Minimal Active Space: NOSCF and NOSI in Multistate Density Functional Theory.

In this Perspective, we introduce a minimal active space (MAS) for the lowest N eigenstates of a molecular system in the framework of multistate density functional theory (MSDFT), consisting of no more than N2 nonorthgonal Slater determinants. In comparison with some methods in wave function theory in which one seeks to expand the ever increasing size of an active space to approximate the wave functions, it is possible to have an upper bound in MSDFT because the auxiliary states in a MAS are used to represent the exact N-dimensional matrix density function D(r). Here, we partition the total Hamiltonian matrix functional into an orbital-dependent part, including multistate kinetic energy Tms and Coulomb-exchange energy EHx plus an external potential energy ∫dr v(r)D(r), and a correlation matrix density functional . The latter accounts for the part of correlation energy not explicitly included in the minimal active space. A major difference from Kohn-Sham DFT is that state interactions are necessary to represent the N-matrix density D(r) in MSDFT, rather than a noninteracting reference state for the scalar ground-state density ρo(r). Two computational approaches are highlighted. We first derive a set of nonorthogonal multistate self-consistent-field (NOSCF) equations for the variational optimization of . We introduce the multistate correlation potential, as the functional derivative of , which includes both correlation effects within the MAS and that from the correlation matrix functional. Alternatively, we describe a nonorthogonal state interaction (NOSI) procedure, in which the determinant functions are optimized separately. Both computational methods are useful for determining the exact eigenstate energies and for constructing variational diabatic states, provided that the universal correlation matrix functional is known. It is hoped that this discussion would stimulate developments of approximate multistate density functionals both for the ground and excited states.

Experimental quantum state discrimination using the optimal fixed rate of inconclusive outcomes strategy

The problem of non-orthogonal state discrimination underlies crucial quantum information tasks, such as cryptography and computing protocols. Therefore, it is decisive to find optimal scenarios for discrimination among quantum states. We experimentally investigate the strategy for the optimal discrimination of two non-orthogonal states considering a fixed rate of inconclusive outcomes (FRIO). The main advantage of the FRIO strategy is to interpolate between unambiguous and minimum error discrimination by solely adjusting the rate of inconclusive outcomes. We present a versatile experimental scheme that performs the optimal FRIO measurement for any pair of generated non-orthogonal states with arbitrary a priori probabilities and any fixed rate of inconclusive outcomes. Considering different values of the free parameters in the FRIO protocol, we implement it upon qubit states encoded in the polarization mode of single photons generated in the spontaneous parametric down-conversion process. Moreover, we resort to a newfangled double-path Sagnac interferometer to perform a three-outcome non-projective measurement required for the discrimination task, showing excellent agreement with the theoretical prediction. This experiment provides a practical toolbox for a wide range of quantum state discrimination strategies using the FRIO scheme, which can significantly benefit quantum information applications and fundamental studies in quantum theory.

Quantum state discrimination in a PT -symmetric system

Nonorthogonal quantum state discrimination (QSD) plays an important role in quantum information and quantum communication. In addition, compared to Hermitian quantum systems, parity-time-($\mathcal{PT}$-)symmetric non-Hermitian quantum systems exhibit novel phenomena and have attracted considerable attention. Here, we experimentally demonstrate QSD in a $\mathcal{PT}$-symmetric system (i.e., $\mathcal{PT}$-symmetric QSD), by having quantum states evolve under a $\mathcal{PT}$-symmetric Hamiltonian in a lossy linear optical setup. We observe that two initially nonorthogonal states can rapidly evolve into orthogonal states, and the required evolution time can even be vanishing provided the matrix elements of the Hamiltonian become sufficiently large. We also observe that the cost of such a discrimination is a dissipation of quantum states into the environment. Furthermore, by comparing $\mathcal{PT}$-symmetric QSD with optimal strategies in Hermitian systems, we find that at the critical value, $\mathcal{PT}$-symmetric QSD is equivalent to the optimal unambiguous state discrimination in Hermitian systems. We also extend the $\mathcal{PT}$-symmetric QSD to the case of discriminating three nonorthogonal states. The QSD in a $\mathcal{PT}$-symmetric system opens a new door for quantum state discrimination, which has important applications in quantum computing, quantum cryptography, and quantum communication.

Deep-learning-assisted communication capacity enhancement by non-orthogonal state recognition of structured light.

In light of pending capacity crunch in information era, orbital-angular-momenta-carrying vortex beams are gaining traction thanks to enlarged transmission capability. However, high-order beams are confronted with fundamental limits of nontrivial divergence or distortion, which consequently intensifies research on new optical states like low-order fractional vortex beams. Here, we experimentally demonstrate an alternative mean to increase the capacity by simultaneously utilizing multiple non-orthogonal states of structured light, challenging a prevailing view of using orthogonal states as information carriers. Specifically, six categories of beams are jointly recognized with accuracy of >99% by harnessing an adapted deep neural network, thus providing the targeted wide bandwidth. We then manifest the efficiency by sending/receiving a grayscale image in 256-ary mode encoding and shift keying schemes, respectively. Moreover, the well-trained model is able to realize high fidelity recognition (accuracy >0.8) onto structured beams under unknown turbulence and restricted receiver aperture size. To gain insights of the framework, we further interpret the network by revealing the contributions of intensity signals from different positions. This work holds potential in intelligence-assisted large-capacity and secure communications, meeting ever growing demand of daily information bandwidth.

Minimal Active Space for Diradicals Using Multistate Density Functional Theory.

This work explores the electronic structure as well as the reactivity of singlet diradicals, making use of multistate density functional theory (MSDFT). In particular, we show that a minimal active space of two electrons in two orbitals is adequate to treat the relative energies of the singlet and triplet adiabatic ground state as well as the first singlet excited state in many cases. This is plausible because dynamic correlation is included in the first place in the optimization of orbitals in each determinant state via block-localized Kohn–Sham density functional theory. In addition, molecular fragment, i.e., block-localized Kohn–Sham orbitals, are optimized separately for each determinant, providing a variational diabatic representation of valence bond-like states, which are subsequently used in nonorthogonal state interactions (NOSIs). The computational procedure and its performance are illustrated on some prototypical diradical species. It is shown that NOSI calculations in MSDFT can be used to model bond dissociation and hydrogen-atom transfer reactions, employing a minimal number of configuration state functions as the basis states. For p- and s-types of diradicals, the closed-shell diradicals are found to be more reactive than the open-shell ones due to a larger diabatic coupling with the final product state. Such a diabatic representation may be useful to define reaction coordinates for electron transfer, proton transfer and coupled electron and proton transfer reactions in condensed-phase simulations.

Modeling molecular J and H aggregates using multiple-Davydov D2 ansatz.

The linear absorption spectrum of J and H molecular aggregates is studied using the time-dependent Dirac-Frenkel variational principle (TDVP) with the multi-Davydov D2 (mD2) trial wavefunction (Ansatz). Both the electronic and vibrational molecular degrees of freedom (DOF) are considered. By inspecting and comparing the absorption spectrum of both open and closed chain aggregates over a range of electrostatic nearest neighbor coupling and temperature values, we find that the mD2 Ansatz is necessary for obtaining an accurate aggregate absorption spectrum in all parameter regimes considered, while the regular Davydov D2 Ansatz is not sufficient. Establishing a relationship between the model parameters and the depth of the mD2 Ansatz is the main focus of this study. Molecular aggregate wavepacket dynamics, during excitation by an external field, is also studied. We find the wavepacket to exhibit an out-of-phase oscillatory behavior along the coordinate and momentum axes and an overall wavepacket broadening, implying the electron-vibrational (vibronic) eigenstates of an aggregate to reside on non-parabolic energy surfaces.

Post-quantum software for distillation of non-orthogonal quantum states through binary frames

Quantum cryptography is a paradigm for the establishment of secret keys and data confidentiality, which represents an alternative in the quantum era because its security properties are based on the principles of quantum physics. Unfortunately, errors that occur during transmission and detection of quantum states have made it difficult to implement this technology globally. However, a new cryptographic key quantum distribution scheme based on non-orthogonal state pairs has recently been published which considerably outperforms known schemes. This article describes the fundamentals of this protocol which are represented as an algorithm and the pseudo-code of the most relevant functions of the system is shown; The current development of the software for the distillation of non-orthogonal quantum states by means of binary frames is presented, which demonstrates the transmission control, reconciliation and privacy amplification of the shared secret bits. Likewise, we present the results obtained from the computer system and its interpretation in relation to the efficiency of the protocol, which exceeds 50% channel error rates and a quadratic growth of the length of the secret key as a function of the number of double detection events. Objectives: Demonstrate the effectiveness of the non-orthogonal state distillation protocol through binary frames using the software developed. Methodology: For the development of this project, the following methodology has been carried out (see Figure 1). Contribution: The results of this software guide tests for quantum distillation in an experimental communications environment in order to provide a useful solution in the era of quantum information transmission and communication technologies.

Bose\u2013Einstein condensate soliton qubit states for metrological applications

We propose a novel platform for quantum metrology based on qubit states of two Bose–Einstein condensate solitons, optically manipulated, trapped in a double-well potential, and coupled through nonlinear Josephson effect. We describe steady-state solutions in different scenarios and perform a phase space analysis in the terms of population imbalance—phase difference variables to demonstrate macroscopic quantum self-trapping regimes. Schrödinger-cat states, maximally path-entangled (N00N) states, and macroscopic soliton qubits are predicted and exploited to distinguish the obtained macroscopic states in the framework of binary (non-orthogonal) state discrimination problem. For an arbitrary frequency estimation we have revealed these macroscopic soliton states have a scaling up to the Heisenberg and super-Heisenberg (SH) limits within linear and nonlinear metrology procedures, respectively. The examples and numerical evaluations illustrate experimental feasibility of estimation with SH accuracy of angular frequency between the ground and first excited macroscopic states of the condensate in the presence of moderate losses, which opens new perspectives for current frequency standard technologies.

A Novel Quantum Voting Scheme Based on BB84-State

BB84-state is the non-orthogonal single-photon state which has the advantage of easy implementation compared with the quantum multi-photon entanglement states. In this paper, based on BB84-state, by introducing a trusted third-party voting center, a quantum voting scheme is proposed. In this scheme, by performing corresponding unitary operation on BB84-state, all voters send their voting information to the tallyman Charlie, then Charlie counts all votes under the supervision of voting management center Bob, which ensures that the protocol can resist inside attacks. Moreover, by utilizing the decoy particles, our scheme can efficiently prevent outside attacks. Compared with other related quantum voting protocols, our protocol has higher qubit efficiency and fewer interactive times.

Theoretical Realization of a Two Qubit Quantum Controlled-NOT Logic Gate and a Single Qubit Quantum Hadamard Logic Gate in the Anti-Jaynes-Cummings Model

Quantum gates are fundamental in Quantum computing for their role in manipulating elementary information carriers referred to as quantum bits. In this paper, a theoretical scheme for realizing a quantum Hadamard and a quantum controlled-NOT logic gates operations in the anti-Jaynes-Cummings interaction process is provided. Standard Hadamard operation for a specified initial atomic state is achieved by setting a specific sum frequency and photon number in the normalized anti-Jaynes-Cummings qubit state transition operation with the interaction component of the anti-Jaynes-Cummings Hamiltonian generating the state transitions. The quantum controlled-NOT logic gate is realized when a single atomic qubit defined in a two-dimensional Hilbert space is the control qubit and two non-degenerate and orthogonal polarized cavities defined in a two-dimensional Hilbert space make the target qubit. With precise choice of interaction time in the anti-Jaynes-Cummings qubit state transition operations defined in the anti-Jaynes-Cummings sub-space spanned by normalized but non-orthogonal basic qubit state vectors, ideal unit probabilities of success in the quantum controlled-NOT operations is determined.

Generation of spin-adapted and spin-complete substitution operators for (high spin) open-shell coupled cluster of arbitrary order.

A rigorous generation of spin-adapted (spin-free) substitution operators for high spin (S = Sz) references of an arbitrary substitution order and spin quantum number S is presented. The generated operators lead to linearly independent but non-orthogonal configuration state functions (CSFs) when applied to the reference and span the complete spin space. To incorporate spin completeness, spectating substitutions (e.g., Êiv va) are introduced. The presented procedure utilizes Löwdin's projection operator method of spin eigenfunction generation to ensure spin completeness. The generated operators are explicitly checked for (i) their linear independence and (ii) their spin completeness for up to tenfold substitutions and up to a multiplicity of 2S + 1 = 11. A proof of concept implementation utilizing the generated operators in a coupled cluster (CC) calculation was successfully applied to the high spin states of the boron atom. The results show pure spin states and small effects on the correlation energy compared to spin orbital CC. A comparison to spin-adapted but spin-incomplete CC shows a significant spin-incompleteness error.

Entanglement of bipartite partly non-orthogonal -spin coherent states

We investigate the entanglement of a bipartite partly non-orthogonal state of the form through -spin coherent states by adopting the concurrence as a measure to quantify the degree of entanglement of the two-qubit system. After, we study the amount of entanglement of mixed states represented by a statistical mixture of partly non-orthogonal bipartite pure states. We also express the lower and upper bounds of the squared concurrence of mixed states in terms of the amplitudes of spin coherent states.

Speech Encryption Algorithm Based on Nonorthogonal Quantum State with Hyperchaotic Keystreams

With the advancement in modern computational technologies like cloud computing, there has been tremendous growth in the field of data processing and encryption technologies. In this contest there is an increasing demand for successful storage of the data in the encrypted domain to avoid the possibility of data breach in shared networks. In this paper, a novel approach for speech encryption algorithm based on quantum chaotic system is designed. In the proposed method, classical bits of the speech samples are initially encoded in nonorthogonal quantum state by the secret polarizing angle. In the quantum domain, encoded speech samples are subjected to bit-flip operation according to the Controlled–NOT gate followed by Hadamard transform. Complete superposition of the quantum state in both Hadamard and standard basis is achieved through Hadamard transform. Control bits for C-NOT gate as well as Hadamard gate are generated with a modified Lu˙-hyperchaotic system. Secret nonorthogonal rotation angles and initial conditions of the hyperchaotic system are the keys used to ensure the security of the proposed algorithm. The computational complexity of the proposed algorithm has been analysed both in quantum domain and classical domain. Numerical simulation carried out based on the above principle showed that the proposed speech encryption algorithm has wider keyspace, higher key sensitivity and robust against various differential and statistical cryptographic attacks.

Stimulated transitions in resonant atom Majorana mixing

Massive neutrinos demand to ask whether they are Dirac or Majorana particles. Majorana neutrinos are an irrefutable proof of physics beyond the Standard Model. Neutrinoless double electron capture is not a process but a virtual ΔL = 2 mixing between a parent AZ atom and a daughter A(Z − 2) excited atom with two electron holes. As a mixing between two neutral atoms and the observable signal in terms of emitted two-hole X-rays, the strategy, experimental signature and background are different from neutrinoless double beta decay. The mixing is resonantly enhanced for almost degeneracy and, under these conditions, there is no irreducible background from the standard two-neutrino channel. We reconstruct the natural time history of a nominally stable parent atom since its production either by nature or in the laboratory. After the time periods of atom oscillations and the decay of the short-lived daughter atom, at observable times the relevant “stationary” states are the mixed metastable long-lived state and the non-orthogonal short-lived excited state, as well as the ground state of the daughter atom. We find that they have a natural population inversion which is most appropriate for exploiting the bosonic nature of the observed atomic transitions radiation. Among different observables of the atom Majorana mixing, we include the enhanced rate of stimulated X-ray emission from the long-lived metastable state by a high-intensity X-ray beam: a gain factor of 100 can be envisaged at current XFEL facilities. On the other hand, the historical population of the daughter atom ground state can be probed by exciting it with a current pulsed optical laser, showing the characteristic absorption lines: the whole population can be excited in a shorter time than typical pulse duration.

Analytic derivative couplings and first-principles exciton/phonon coupling constants for an ab initio Frenkel-Davydov exciton model: Theory, implementation, and application to compute triplet exciton mobility parameters for crystalline tetracene.

Recently, we introduced an ab initio version of the Frenkel-Davydov exciton model for computing excited-state properties of molecular crystals and aggregates. Within this model, supersystem excited states are approximated as linear combinations of excitations localized on molecular sites, and the electronic Hamiltonian is constructed and diagonalized in a direct-product basis of non-orthogonal configuration state functions computed for isolated fragments. Here, we derive and implement analytic derivative couplings for this model, including nuclear derivatives of the natural transition orbital and symmetric orthogonalization transformations that are part of the approximation. Nuclear derivatives of the exciton Hamiltonian's matrix elements, required in order to compute the nonadiabatic couplings, are equivalent to the "Holstein" and "Peierls" exciton/phonon couplings that are widely discussed in the context of model Hamiltonians for energy and charge transport in organic photovoltaics. As an example, we compute the couplings that modulate triplet exciton transport in crystalline tetracene, which is relevant in the context of carrier diffusion following singlet exciton fission.