A quantum dissipation theory is constructed with the system–bath interaction being treated rigorously at second-order cumulant level for both reduced dynamics and initial canonical boundary condition. The valid arbitrary bath correlation functions time-dependent external driving fields, satisfies correlated detailed-balance relation any temperatures. general formulation assumes a particularly simple form in driven Brownian oscillator systems which driving-dissipation effects can be accounted...

We propose an efficient method to propagate the hierarchical quantum master equations based on a reformulation of original formalism and incorporation filtering algorithm that automatically truncates hierarchy with preselected tolerance. The new is applied calculate electron transfer dynamics in spin-boson model absorption spectra excitonic dimmer. proposed significantly reduces number auxiliary density operators used equation approach thus provides way capable studying real time...

An exact quantum master equation formalism is constructed for the efficient evaluation of non-Markovian dissipation beyond weak system-bath interaction regime in presence time-dependent external field. A novel truncation scheme further proposed and compared with other approaches to close resulting hierarchically coupled equations motion. The interplay between strength, property, required level hierarchy also demonstrated aid simple spin-boson systems.

Padé approximant is exploited for an efficient sum-over-poles decomposition of Fermi and Bose functions. The resulting poles are all pure imaginary can therefore be used to define frequencies, in analogy with the celebrated Matsubara frequencies. proposed spectrum shown equivalent a truncated continued fraction. It converges significantly faster than other schemes such as expansion at temperatures. By introducing characteristic validity length measure approximant, we analyze convergence...

Padé spectrum decomposition is an optimal sum-over-poles expansion scheme of Fermi function and Bose [J. Hu, R. X. Xu, Y. J. Yan, Chem. Phys. 133, 101106 (2010)]10.1063/1.3484491. In this work, we report two additional members to family, from which the best among all methods could be chosen for different cases application. Methods are developed determining these three expansions at machine precision via simple algorithms. We exemplify applications present development with construction...

A nonperturbative theory is developed, aiming at an exact and efficient evaluation of a general quantum system interacting with arbitrary bath environment any temperature in the presence time-dependent external fields. An hierarchical equations motion formalism constructed on basis calculus-on-path-integral algorithm, via auxiliary influence generating functionals related to interaction correlation functions parametrization expansion form. The corresponding continued-fraction Green's for...

Accurate characterization of correlated electronic states, as well their evolution under external fields or in dissipative environment, is essentially important for understanding the properties strongly transition‐metal materials involving spin‐unpaired d f electrons. This paper reviews development and applications a numerical simulation program, Hierarchical Equations Motion QUantum Impurity with Correlated Kernel ( HEOM‐QUICK ), which allows an accurate universal quantum impurity systems....

In this Communication, we propose the time-domain Prony fitting decomposition (t-PFD) as an accurate and efficient exponential series method, applicable to arbitrary bath correlation functions. The resulting numerical efficiency of hierarchical equations motion (HEOM) formalism is greatly optimized, especially in low temperature regimes that would be inaccessible with other methods. For demonstration, calibrate present t-PFD against celebrated Padé spectrum followed by converged HEOM...

The hierarchical equations of motion (HEOM) method has become one the most popular methods for studies open quantum system. However, its applicability to systems at ultra-low temperatures is largely restrained by enormous computational cost, which caused numerous exponential functions required accurately characterize non-Markovian memory reservoir environment. To overcome this problem, a Fano spectrum decomposition (FSD) scheme been proposed recently [Cui et al., J. Chem. Phys. 151, 024110...

The Fano spectrum decomposition (FSD) scheme is proposed as an efficient and accurate sum-over-poles expansion of Fermi Bose functions at cryogenic temperatures. new method practically overcomes the discontinuity near zero temperature, which causes slow convergence in conventional schemes such state-of-the-art Padé (PSD). FSD fragments or function into a high-temperature reference low-temperature correction. While former efficiently decomposed via standard PSD, latter can be accurately...

The Zusman equation has been widely used to study the effect of solvent dynamics on electron transfer reactions. However, application this is limited by classical treatment nuclear degrees freedom. In paper, we revisit in framework exact hierarchical equations motion formalism, and show that a high temperature approximation theory equivalent describing dynamics. Thus formalism naturally extends include quantum at low temperatures. This new finding also inspired us rescale original...

Quantum simulation can beat current classical computers with minimally a few tens of qubits and will likely become the first practical use quantum computer. One promising application is to attack challenging chemistry problems. Here we report an experimental demonstration that small nuclear-magnetic-resonance (NMR) computer already able simulate dynamics prototype chemical reaction. The results agree well simulations. We conclude reaction not computable on feasible in near future.

Miniaturization and acceleration of synthetic chemistry are critically important for rapid property optimization in pharmaceutical, agrochemical, materials research development. However, most laboratories organic synthesis is still performed on a slow, sequential, material-consuming scale not validated multiple substrate combinations. Herein, we introduce fast touchless acoustic droplet ejection (ADE) technology into small-molecule to transfer building blocks by nL droplets scout newly...

Screening of large and diverse libraries is the 'bread butter' in first phase discovery novel drugs. However, maintenance periodic renewal high-quality compound collections pose considerable logistic, environmental monetary problems. Here, we exercise an alternative, 'on-the-fly' synthesis on a nanoscale highly automated fashion. For time, show feasibility library based 16 different chemistries parallel several 384-well plates using acoustic dispensing ejection (ADE) technology platform. In...

The Peltier effect, which is the reverse counterpart of Seebeck has been experimentally observed in nanojunctions. Despite its potential applications cooling nanoelectronic devices, achieving significant figures merit and power remain challenging. Here, we propose a novel approach to enable substantial by leveraging orbital-Kondo states formed through strong electron correlations. We demonstrate this showcasing heat current reduced local temperature serially connected two-impurity junction,...

Abstract Many‐body open quantum systems (OQSs) have a profound impact on various subdisciplines of physics, chemistry, and biology. Thus, the development computer program capable accurately, efficiently, versatilely simulating many‐body OQSs is highly desirable. In recent years, we focused advancement numerical algorithms based fermionic hierarchical equations motion (HEOM) theory. Being in‐principle exact, this approach allows for precise characterization correlations, non‐Markovian memory,...

Objective: The objective of this study was to explore the influence polymorphism protocadherin 9 ( PCDH9 ) gene and narcissistic personality trait (NPT) on risk major depressive disorder (MDD) in Chinese first-year university students. Methods: A 2-year cohort conducted among students who were enrolled 2018 from two universities Shandong Province, China. snapshot technique used detect genotypes (rs9540720). version Composite International Diagnostic Interview for MDD assessment. NPTs...

Metal-free diradicals based on polycyclic aromatic hydrocarbons are promising candidates for organic spintronics due to their stable magnetism and tunable spin coupling. However, distinguishing elucidating the origins of ferromagnetic antiferromagnetic interactions in these systems remain challenging. Here, we investigate

Hierarchical equations of motion theory for Drude dissipation is optimized, with a convenient convergence criterion proposed in advance numerical propagations. The theoretical construction on the basis Padé spectrum decomposition that has been qualified to be best sum-over-poles scheme quantum distribution function. resulting hierarchical dynamics under priori are exemplified benchmark spin-boson system, and also transient absorption related coherent two-dimensional spectroscopy model...

We present an optimized hierarchical equations of motion theory for quantum dissipation in multiple Brownian oscillators bath environment, followed by a mechanistic study on model donor-bridge-acceptor system. show that the optimal hierarchy construction, via memory-frequency decomposition any specified bath, is generally achievable through universal pre-screening search. The algorithm goes identifying candidates best be just some selected Padé spectrum based schemes, together with priori...

Several recent advancements for the hierarchical equations of motion (HEOM) approach are reported. First, we propose an a priori estimate optimal number basis functions reservoir memory decomposition. Second, make use sparsity auxiliary density operators (ADOs) and two ansatzs to screen out all intrinsic zero ADO elements. Third, new truncation scheme by utilizing time derivatives higher-tier ADOs. These novel techniques greatly reduce cost HEOM approach, thus enhance its efficiency...