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Yuan-Chung Cheng

Publications and source records attributed to Yuan-Chung Cheng.

16 recordsLinked to original sources

Quantum Simulation of Dissipative Energy Transfer via Noisy Quantum Computer

We study whether dissipative energy-transfer dynamics can be simulated on noisy near-term quantum hardware by treating device noise as a calibrated resource rather than purely as an error source. Focusing on a biased exciton dimer, we encode the single-excitation manifold into a two-qubit subspace and implement the coherent dynamics through a shallow Trotterized propagator, while repeated noisy identity operations provide an effective dissipative channel. We benchmark the resulting short-time population dynamics against the hierarchical equations of motion (HEOM), which serves as a numerically accurate reference for the corresponding open-system model. On IBM quantum hardware, the calibrated noisy circuit reproduces a broad range of dissipative trajectories in the tested regime, and the fitted HEOM parameters exhibit an approximately linear dependence on the noisy-gate frequency. This empirical relation enables a practically useful interpolation strategy: once calibrated by a finite set of HEOM calculations, the noisy circuit can replace repeated HEOM fitting for intermediate parameter points within the same biased-dimer family. To extend the dynamics beyond the circuit-depth limit, we combine the short-time quantum data with the transfer tensor method (TTM). In simulator studies, TTM accurately extends the dynamics well beyond the directly simulated window, whereas on real hardware its performance is limited by the instability of coherence-sensitive initial states. Our results show that noisy few-qubit devices can act as calibrated phenomenological simulators of open-system dynamics and, within a restricted but experimentally relevant regime, can provide a practical surrogate for repeated HEOM-based modeling.

quant-ph

Accurate harmonic vibrational frequencies for diatomic molecules via quantum computing

During the noisy intermediate-scale quantum (NISQ) era, quantum computational approaches refined to overcome the challenge of limited quantum resources are highly valuable. However, the accuracy of the molecular properties predicted by most of the quantum computations nowadays is still far off (not within chemical accuracy) compared to their corresponding experimental data. Here, we propose a promising qubit-efficient quantum computational approach to calculate the harmonic vibrational frequencies of a large set of neutral closed-shell diatomic molecules with results in great agreement with their experimental data. To this end, we construct the accurate Hamiltonian using molecular orbitals, derived from density functional theory to account for the electron correlation and expanded in the Daubechies wavelet basis set to allow an accurate representation in real space grid points, where an optimized compact active space is further selected so that only a reduced small number of qubits is sufficient to yield an accurate result. To justify the approach, we benchmark the performance of the Hamiltonians spanned by the selected molecular orbitals by first transforming the molecular Hamiltonians into qubit Hamiltonians and then using the exact diagonalization method to calculate the results, regarded as the best results achievable by quantum computation. Furthermore, we show that the variational quantum circuit with the chemistry-inspired UCCSD ansatz can achieve the same accuracy as the exact diagonalization method except for systems whose Mayer bond order indices are larger than 2. For those systems, we demonstrate that the heuristic hardware-efficient RealAmplitudes ansatz, even with a shorter circuit depth, can provide a significant improvement over the UCCSD ansatz, verifying that the harmonic vibrational frequencies could be calculated accurately by quantum computation in the NISQ era.

quant-ph

The effect of static disorder on the center line slope in 2D electronic spectroscopy

Two-dimensional electronic spectroscopy (2DES) is a powerful tool for investigating the dynamics of complex systems. However, analyzing the resulting spectra can be challenging, and thus may require the use of theoretical modeling techniques. The center line slope (CLS) method is one of such approaches, which aims to extract the time correlation function (TCF) from 2DES with minimal error. Since static disorder is widely observed in complex systems, it may be interesting to ask whether the CLS approach still work in the presence of the static disorder. In this paper, the effect of the static disorder on the TCF obtained through the CLS method is investigated. It is found that the steady-state value of the CLS increases monotonically with respect to the static disorder, which suggests that the amplitude of the static disorder can be determined using the CLS in the long-time limit. Additionally, as the static disorder rises, the decay rate of the CLS first decreases to a certain value and remains at this value until the static disorder is sufficiently large. Afterward, the CLS begins to fluctuate significantly and thus results in obtaining the decay rate through the CLS method unreliable. Based on these discoveries, we propose a method to fix the error and obtain the TCF. Our findings may pave the way for obtaining reliable system-bath information by analyzing 2DES in the practical situations.

physics.optics

Accurate and Efficient Quantum Computations of Molecular Properties Using Daubechies Wavelet Molecular Orbitals: A Benchmark Study against Experimental Data

Although quantum computation (QC) is regarded as a promising numerical method for computational quantum chemistry, current applications of quantum-chemistry calculations on quantum computers are limited to small molecules. This limitation can be ascribed to technical problems in building and manipulating more qubits and the associated complicated operations of quantum gates in a quantum circuit when the size of the molecular system becomes large. As a result, reducing the number of required qubits is necessary to make QC practical. Currently, the minimal STO-3G basis set is commonly used in benchmark studies because it requires the minimum number of spin orbitals. Nonetheless, the accuracy of using STO-3G is generally low and thus cannot provide useful predictions. We propose to adopt Daubechies wavelet functions as an accurate and efficient method for QCs of molecular electronic properties. We demonstrate that a minimal basis set constructed from Daubechies wavelet basis can yield accurate results through a better description of the molecular Hamiltonian, while keeping the number of spin orbitals minimal. With the improved Hamiltonian through Daubechies wavelets, we calculate vibrational frequencies for H$_2$ and LiH using quantum-computing algorithm to show that the results are in excellent agreement with experimental data. As a result, we achieve quantum calculations in which accuracy is comparable with that of the full configuration interaction calculation using the cc-pVDZ basis set, whereas the computational cost is the same as that of a STO-3G calculation. Thus, our work provides a more efficient and accurate representation of the molecular Hamiltonian for efficient QCs of molecular systems, and for the first time demonstrates that predictions in agreement with experimental measurements are possible to be achieved with quantum resources available in near-term quantum computers.

quant-ph

Quantum sensing on magnetic field inspired by Avian compass

Magnetic measurement can be performed by various sensors, such as SQUID and Giant Magnetoresistance. This device can achieve high accuracy while losing efficiency and convenience. The model of biological magnetic sensing in avian proposes a radical pair response to the external field on the FLY results in regulating animal behaviour. Inspired by the radical pair system found in biological system, the effect of intra-radical coupling and the initial condition is studied in this simplified radical pair model as the quantum advantage results from entanglement and superposition are investigated in metrology. To identify the sensing benefit from the cooperation between the radical pairs, the inter-radical coupling is considered. We find the intra-radical coupling determines the sensing regime while the coupled radical pair system enables a new sensing scheme that provides a more general and flexible way for magnetic sensing in a broader range through a easier manipulation to the system.

quant-ph

Efficient Quantum Simulation of Open Quantum System Dynamics on Noisy Quantum Computers

Quantum simulation represents the most promising quantum application to demonstrate quantum advantage on near-term noisy intermediate-scale quantum (NISQ) computers, yet available quantum simulation algorithms are prone to errors and thus difficult to be realized. Herein, we propose a novel scheme to utilize intrinsic gate errors of NISQ devices to enable controllable simulation of open quantum system dynamics without ancillary qubits or explicit bath engineering, thus turning unwanted quantum noises into useful quantum resources. Specifically, we simulate energy transfer process in a photosynthetic dimer system on IBM-Q cloud. By employing designed decoherence-inducing gates, we show that quantum dissipative dynamics can be simulated efficiently across coherent-to-incoherent regimes with results comparable to those of the numerically-exact classical method. Moreover, we demonstrate a calibration routine that enables consistent and predictive simulations of open-quantum system dynamics in the intermediate coupling regime. This work provides a new direction for quantum advantage in the NISQ era.

quant-ph

Excitation Energies from Thermally-Assisted-Occupation Density Functional Theory: Theory and Computational Implementation

The time-dependent density functional theory (TDDFT) has been broadly used to investigate the excited-state properties of various molecular systems. However, the current TDDFT heavily relies on outcomes from the corresponding ground-state density functional theory (DFT) calculations which may be prone to errors due to the lack of proper treatment in the non-dynamical correlation effects. Recently, thermally-assisted-occupation density functional theory (TAO-DFT) [J.-D. Chai, \textit{J. Chem. Phys.} \textbf{136}, 154104 (2012)], a DFT with fractional orbital occupations, was proposed, explicitly incorporating the non-dynamical correlation effects in the ground-state calculations with low computational complexity. In this work, we develop time-dependent (TD) TAO-DFT, which is a time-dependent, linear-response theory for excited states within the framework of TAO-DFT. With tests on the excited states of H$_{2}$, the first triplet excited state ($1^3Σ_u^+$) was described well, with non-imaginary excitation energies. TDTAO-DFT also yields zero singlet-triplet gap in the dissociation limit, for the ground singlet ($1^1Σ_g^+$) and the first triplet state ($1^3Σ_u^+$). In addition, as compared to traditional TDDFT, the overall excited-state potential energy surfaces obtained from TDTAO-DFT are generally improved and better agree with results from the equation-of-motion coupled-cluster singles and doubles (EOM-CCSD).

physics.chem-ph

Exact and efficient quantum simulation of open quantum dynamics for various of Hamiltonians and spectral densities

Recently, we have theoretically proposed and experimentally demonstrated an exact and efficient quantum simulation of photosynthetic light harvesting in nuclear magnetic resonance (NMR), cf. B. X. Wang, \textit{et al.} npj Quantum Inf.~\textbf{4}, 52 (2018). In this paper, we apply this approach to simulate the open quantum dynamics in various photosynthetic systems with different Hamiltonians. By numerical simulations, we show that for Drude-Lorentz spectral density the dimerized geometries with strong couplings within the donor and acceptor clusters respectively exhibit significantly-improved efficiency. Based on the optimal geometry, we also demonstrate that the overall energy transfer can be further optimized when the energy gap between the donor and acceptor clusters matches the peak of the spectral density. Moreover, by exploring the quantum dynamics for different types of spectral densities, e.g. Ohmic, sub-Ohmic, and super-Ohmic spectral densities, we show that our approach can be generalized to effectively simulate open quantum dynamics for various Hamiltonians and spectral densities. Because $\log_{2}N$ qubits are required for quantum simulation of an $N$-dimensional quantum system, this quantum simulation approach can greatly reduce the computational complexity compared with popular numerically-exact methods.

quant-ph

Quantum simulation of photosynthetic energy transfer

Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry and material science, as it may offer valuable insights into efficient solar-energy harvesting. Recently, quantum coherent effects have been discovered in photosynthetic light harvesting, and their potential role on energy transfer has seen heated debate. Here, we perform an experimental quantum simulation of photosynthetic energy transfer using nuclear magnetic resonance (NMR). We show that an N- chromophore photosynthetic complex, with arbitrary structure and bath spectral density, can be effectively simulated by a system with log2 N qubits. The computational cost of simulating such a system with a theoretical tool, like the hierarchical equation of motion, which is exponential in N, can be potentially reduced to requiring a just polynomial number of qubits N using NMR quantum simulation. The benefits of performing such quantum simulation in NMR are even greater when the spectral density is complex, as in natural photosynthetic complexes. These findings may shed light on quantum coherence in energy transfer and help to provide design principles for efficient artificial light harvesting.

quant-ph

Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

The structure of Fenna-Matthews-Olson (FMO) light-harvesting complex has long been recognized as containing seven bacteriochlorophyll (BChl) molecules. Recently, an additional BChl molecule was discovered in the crystal structure of the FMO complex, which may serve as a link between baseplate and the remaining seven molecules. Here, we investigate excitation energy transfer (EET) process by simulating single-molecule pump-dump experiment in the eight-molecules complex. We adopt the coherent modified Redfield theory and non-Markovian quantum jump method to simulate EET dynamics. This scheme provides a practical approach of detecting the realistic EET pathway in BChl complexes with currently available experimental technology. And it may assist optimizing design of artificial light-harvesting devices.

physics.chem-ph

Using non-Markovian measures to evaluate quantum master equations for photosynthesis

When dealing with system-reservoir interactions in an open quantum system, such as a photosynthetic light-harvesting complex, approximations are usually made to obtain the dynamics of the system. One question immediately arises: how good are these approximations, and in what ways can we evaluate them? Here, we propose to use entanglement and a measure of non-Markovianity as benchmarks for the deviation of approximate methods from exact results. We apply two frequently-used perturbative but non-Markovian approximations to a photosynthetic dimer model and compare their results with that of the numerically-exact hierarchy equation of motion (HEOM). This enables us to explore both entanglement and non-Markovianity measures as means to reveal how the approximations either overestimate or underestimate memory effects and quantum coherence. In addition, we show that both the approximate and exact results suggest that non-Markonivity can, counter-intuitively, increase with temperature, and with the coupling to the environment.

quant-ph

An Efficient Quantum Jump Method for Coherent Energy Transfer Dynamics in Photosynthetic Systems under the Influence of Laser Fields

We present a non-Markovian quantum jump approach for simulating coherent energy transfer dynamics in molecular systems in the presence of laser fields. By combining a coherent modified Redfield theory (CMRT) and a non-Markovian quantum jump (NMQJ) method, this new approach inherits the broad-range validity from the CMRT and highly efficient propagation from the NMQJ. To implement NMQJ propagation of CMRT, we show that the CMRT master equation can be casted into a generalized Lindblad form. Moreover, we extend the NMQJ approach to treat time-dependent Hamiltonian, enabling the description of excitonic systems under coherent laser fields. As a benchmark of the validity of this new method, we show that the CMRT-NMQJ method accurately describes the energy transfer dynamics in a prototypical photosynthetic complex. Finally, we apply this new approach to simulate the quantum dynamics of a dimer system coherently excited to coupled single-excitation states under the influence of laser fields, which allows us to investigate the interplay between the photoexcitation process and ultrafast energy transfer dynamics in the system. We demonstrate that laser-field parameters significantly affect coherence dynamics of photoexcitations in excitonic systems, which indicates that the photoexcitation process must be explicitly considered in order to properly describe photon-induced dynamics in photosynthetic systems. This work should provide a valuable tool for efficient simulations of coherent control of energy flow in photosynthetic systems and artificial optoelectronic materials.

quant-ph

Clustered Geometries Exploiting Quantum Coherence Effects for Efficient Energy Transfer in Light Harvesting

Elucidating quantum coherence effects and geometrical factors for efficient energy transfer in photosynthesis has the potential to uncover non-classical design principles for advanced organic materials. We study energy transfer in a linear light-harvesting model to reveal that dimerized geometries with strong electronic coherences within donor and acceptor pairs exhibit significantly improved efficiency, which is in marked contrast to predictions of the classical Förster theory. We reveal that energy tuning due to coherent delocalization of photoexcitations is mainly responsible for the efficiency optimization. This coherence-assisted energy-tuning mechanism also explains the energetics and chlorophyll arrangements in the widely-studied Fenna-Matthews-Olson complex. We argue that a clustered network with rapid energy relaxation among donors and resonant energy transfer from donor to acceptor states provides a basic formula for constructing efficient light-harvesting systems, and the general principles revealed here can be generalized to larger systems and benefit future innovation of efficient molecular light-harvesting materials.

physics.bio-ph

Functional quantum biology in photosynthesis and magnetoreception

Is there a functional role for quantum mechanics or coherent quantum effects in biological processes? While this question is as old as quantum theory, only recently have measurements on biological systems on ultra-fast time-scales shed light on a possible answer. In this review we give an overview of the two main candidates for biological systems which may harness such functional quantum effects: photosynthesis and magnetoreception. We discuss some of the latest evidence both for and against room temperature quantum coherence, and consider whether there is truly a functional role for coherence in these biological mechanisms. Finally, we give a brief overview of some more speculative examples of functional quantum biology including the sense of smell, long-range quantum tunneling in proteins, biological photoreceptors, and the flow of ions across a cell membrane.

physics.bio-ph

Environmental correlation effects on excitation energy transfer in photosynthetic light harvesting

Several recent studies of energy transfer in photosynthetic light harvesting complexes have revealed a subtle interplay between coherent and decoherent dynamic contributions to the overall transfer efficiency in these open quantum systems. In this work we systematically investigate the impact of temporal and spatial correlations in environmental fluctuations on excitation transport in the Fenna-Matthews-Olson photosynthetic complex. We demonstrate that the exact nature of the correlations can have a large impact on the efficiency of light harvesting. In particular, we find that (i) spatial correlations can enhance coherences in the site basis while at the same time slowing transport, and (ii) the overall efficiency of transport is optimized at a finite temporal correlation that produces maximum overlap between the environmental power spectrum and the excitonic energy differences, which in turn results in enhanced driving of transitions between excitonic states.

quant-ph

Aging Continuous Time Random Walks

We investigate aging continuous time random walks (ACTRW), introduced by Monthus and Bouchaud [{\em J. Phys. A} {\bf 29}, 3847 (1996)]. Statistical behaviors of the displacement of the random walker ${\bf r}={\bf r}(t) - {\bf r}(0)$ in the time interval $(0,t)$ are obtained, after aging the random walk in the time interval $(-t_a,0)$. In ACTRW formalism, the Green function $P({\bf r}, t_a, t)$ depends on the age of the random walk $t_a$ and the forward time $t$. We derive a generalized Montroll--Weiss equation, which yields an exact expression for the Fourier double Laplace transform of the ACTRW Green function. Asymptotic long times $t_a$ and $t$ behaviors of the Green function are investigated in detail. In the limit of $t\gg t_a$, we recover the standard non-equilibrium CTRW behaviors, while the important regimes $t\ll t_a$ and $t \simeq t_a$ exhibit interesting aging effects. Convergence of the ACTRW results towards CTRW behavior, becomes extremely slow when the diffusion exponent becomes small. In the context of biased ACTRW, we investigate an aging Einstein relation. We briefly discuss aging in Scher-Montroll type of transport in disordered materials.

cond-mat.stat-mech