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We present a new partially linearized mapping-based approach for approximating real-time quantum correlation functions in condensed-phase nonadiabatic systems, called spin-PLDM. Within a classical trajectory picture, partially linearized…

Chemical Physics · Physics 2021-02-03 J. R. Mannouch , J. O. Richardson

In the previous paper [J. R. Mannouch and J. O. Richardson, J.~Chem.~Phys.~xxx, xxxxx (xxxx)] we derived a new partially linearized mapping-based classical-trajectory technique, called spin-PLDM. This method describes the dynamics…

Chemical Physics · Physics 2021-02-03 J. R. Mannouch , J. O. Richardson

This paper focuses on developing a method to obtain an uncertain linear fractional transformation (LFT) system that adequately captures the dynamics of a nonlinear time-invariant system over some desired envelope. First, the nonlinear…

Systems and Control · Electrical Eng. & Systems 2023-05-02 Sourav Sinha , Devaprakash Muniraj , Mazen Farhood

We propose a trajectory-based quasiclassical method for approximating dynamics in condensed phase systems. Building upon the previously developed Optimized Mean Trajectory (OMT) approximation that has been used to compute linear and…

Chemical Physics · Physics 2024-08-23 Kritanjan Polley

We discuss theoretical approaches to nonlinear optical spectroscopy of molecular junctions. Optical response functions are derived in the form convenient for implementation of Green function techniques, and their expressions in terms of…

Mesoscale and Nanoscale Physics · Physics 2016-06-28 Yi Gao , Michael Galperin

Nonlinear spectroscopy employs a series of laser pulses to interrogate dynamics in large interacting many-body systems, and has become a highly successful method for experiments in chemical physics. Current quantum optical experiments…

Quantum Physics · Physics 2016-10-19 Frank Schlawin , Manuel Gessner , Shaul Mukamel , Andreas Buchleitner

Optical two-dimensional (2D) coherent spectroscopy excels in studying coupling and dynamics in complex systems. The dynamical information can be learned from lineshape analysis to extract the corresponding linewidth. However, it is usually…

Optics · Physics 2020-06-24 Srikanth Namuduri , Michael Titze , Shekhar Bhansali , Hebin Li

Spectroscopy is an indispensable tool in understanding the structures and dynamics of molecular systems. However computational modelling of spectroscopy is challenging due to the exponential scaling of computational complexity with system…

Quantum Physics · Physics 2021-06-22 Chee-Kong Lee , Chang-Yu Hsieh , Shengyu Zhang , Liang Shi

Two-dimensional electronic spectroscopy (2DES) provides a detailed picture of electronically nonadiabatic dynamics that can be interpreted with the aid of simulations. Here, we develop and contrast trajectory-based nonadiabatic dynamics…

We propose a trajectory-based method for simulating nonadiabatic dynamics in molecular systems with two coupled electronic states. Employing a quantum-mechanically exact mapping of the two-level problem to a spin-1/2 coherent state, we…

Chemical Physics · Physics 2020-03-03 Johan E. Runeson , Jeremy O. Richardson

We introduce a new algorithm to solve a regularized spatial-spectral image estimation problem. Our approach is based on the linearized alternating directions method of multipliers (LADMM), which is a variation of the popular ADMM algorithm.…

Signal Processing · Electrical Eng. & Systems 2025-02-25 Yunsong Liu , Debdut Mandal , Congyu Liao , Kawin Setsompop , Justin P. Haldar

Linear optical circuits with single-photon sources offer a promising platform for quantum chemistry and machine learning. However, current applications are all based on support vector machines or gradient-free optimization methods. This…

Quantum Physics · Physics 2024-12-10 Giovanni de Felice , Christopher Corlett

Nonlinear spectroscopy is a cornerstone of quantum science, providing unique access to multi-point correlations, quantum coherence, and couplings that are invisible to linear methods. However, classical simulation of these phenomena is…

Quantum Physics · Physics 2026-04-20 Long Xiong , Xiaoyang Wang , Xiaoxia Cai , Xiao Yuan

The mapping approach addresses the mismatch between the continuous nuclear phase space and discrete electronic states by creating an extended, fully continuous phase space using a set of harmonic oscillators to encode the populations and…

Chemical Physics · Physics 2019-09-30 Maximilian A. C. Saller , Aaron Kelly , Jeremy O. Richardson

We discuss the formulation of spin observables associated to a non-relativistic spinning particles in terms of grassmanian differential operators. We use as configuration space variables for the pseudo-classical description of this system…

High Energy Physics - Theory · Physics 2007-05-23 J. A. Lopez , J. Stephany

Optical computing systems provide an alternate hardware model which appears to be aligned with the demands of neural network workloads. However, the challenge of implementing energy efficient nonlinearities in optics -- a key requirement…

Optics · Physics 2025-08-04 N. Richardson , C. Bosch , R. P. Adams

The Feynman path integral formalism has inspired the development of memory-efficient and parallelizable classical algorithms for simulating quantum computers. We adapt this approach for the calculation of probability amplitudes of…

We present a theoretical approach to optical spectroscopy of open nonequilibrium systems, which generalizes traditional nonlinear optical spectroscopy tools by imposing charge and energy conservation at all levels of approximation. Both…

Mesoscale and Nanoscale Physics · Physics 2019-12-19 Shaul Mukamel , Michael Galperin

We recently derived a spin-mapping approach for treating the nonadiabatic dynamics of a two-level system in a classical environment [J. Chem. Phys. 151, 044119 (2019)] based on the well-known quantum equivalence between a two-level system…

Chemical Physics · Physics 2020-03-03 Johan E. Runeson , Jeremy O. Richardson

Exactly computing the full output distribution of linear optical circuits remains a challenge, as existing methods are either time-efficient but memory-intensive or memory-efficient but slow. Moreover, any realistic simulation must account…

Quantum Physics · Physics 2025-03-10 Timothée Goubault de Brugière , Nicolas Heurtel
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