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In this paper, we present a new method for calculating linear absorption spectra for large molecular aggregates, called dyadic adaptive HOPS (DadHOPS). This method combines the adaptive HOPS (adHOPS) framework, which uses locality to…

The photoexcitation dynamics of molecular materials on the 10-100 nm length scale depend on complex interactions between the electronic and vibrational degrees of freedom, rendering exact calculations difficult or intractable. The adaptive…

Chemical Physics · Physics 2024-03-11 Brian Citty , Jacob K. Lynd , Tarun Gera , Leonel Varvelo , Doran I. G. B. Raccah

The simulation of spectroscopic observables for molecular aggregates with strong and structured coupling of electronic excitation to vibrational degrees of freedom is an important but challenging task. The hierarchy of pure states (HOPS)…

Quantum Physics · Physics 2022-04-13 Lipeng Chen , Doran I. G. Bennett , Alexander Eisfeld

We implement and apply time-dependent density matrix renormalization group (TD-DMRG) algorithms at zero and finite temperature to compute the linear absorption and fluorescence spectra of molecular aggregates. Our implementation is within a…

Chemical Physics · Physics 2019-07-30 Jiajun Ren , Zhigang Shuai , Garnet Kin-Lic Chan

Metal Organic Frameworks (MOFs) are promising materials to help mitigate the effects of global warming by selectively absorbing $\text{CO}_{2}$ for direct capture. Accurate quantum chemistry simulations are a useful tool to help select and…

The real-space density-functional perturbation theory (DFPT) for the computations of the response properties with respect to the atomic displacement and homogeneous electric field perturbation has been recently developed and implemented…

Computational Physics · Physics 2020-10-28 Honghui Shang , Wanzhen Liang , Yunquan Zhang , Jinlong Yang

In order to discern aggregation in solutions, we present a quantum mechanical analog of the photon statistics from fluorescent molecules diffusing through a focused beam. A generating functional is developed to fully describe the…

Biological Physics · Physics 2009-11-10 Hai-cang Ren , Noel L. Goddard , Gregoire Altan-Bonnet , Albert Libchaber

We describe a fast parallel iterative method for computing molecular absorption spectra within TDDFT linear response and using the LCAO method. We use a local basis of "dominant products" to parametrize the space of orbital products that…

Other Condensed Matter · Physics 2011-04-19 Peter Koval , Dietrich Foerster , Olivier Coulaud

An accurate treatment of electronic spectra in large systems with a technique such as time dependent density functional theory (TDDFT) is computationally challenging. Due to the Nyquist sampling theorem, direct real time simulations must be…

Materials Science · Physics 2024-01-17 Matthias Kick , Ezra Alexander , Anton Beiersdorfer , Troy Van Voorhis

Widely employed Near-Edge X-Ray Absorption Fine Structure (NEXAFS) spectroscopy probes a system by excitation of core electrons to unoccupied states. A variety of different methodologies are available to simulate corresponding spectra from…

Chemical Physics · Physics 2019-02-14 Georg S. Michelitsch , Karsten Reuter

Through temporal shaping of the excitation signal, the complex-frequency scattering zeros of a lossless structure can be accessed, enabling a storage-release mechanism referred to as coherent virtual absorption. Practical demonstrations of…

Event-based image sensors provide microsecond temporal resolution but lack spectral discrimination, whereas diffractive spectral imagers encode wavelength information at conventional frame rates. We introduce a fluorescence microscopy…

Optics · Physics 2026-03-20 Richard G. Baird , Boyden Myers , Erik M. Jorgensen , Rajesh Menon

With the emergence of Artificial Intelligence, numerical algorithms are moving towards more approximate approaches. For methods such as PCA or diffusion maps, it is necessary to compute eigenvalues of a large matrix, which may also be dense…

Numerical Analysis · Mathematics 2023-11-17 Keerthi Gaddameedi , Severin Reiz , Tobias Neckel , Hans-Joachim Bungartz

We briefly review the principles, mathematical bases, numerical shortcuts and applications of fast random walk (FRW) algorithms. This Monte Carlo technique allows one to simulate individual trajectories of diffusing particles in order to…

Computational Physics · Physics 2013-05-01 Denis Grebenkov

We present a scalable Bayesian framework for the analysis of confocal fluorescence spectroscopy data, addressing key limitations in traditional fluorescence correlation spectroscopy methods. Our framework captures molecular motion,…

Numerical Analysis · Mathematics 2024-11-07 Daniel McBride , Ioannis Sgouralis

We describe a new generation of algorithms capable of mapping the structure and conformations of macromolecules and their complexes from large ensembles of heterogeneous snapshots, and demonstrate the feasibility of determining both…

Biological Physics · Physics 2014-04-30 P. Schwander , R. Fung , A. Ourmazd

We presented an efficient algorithm, fast adaptive flat-histogram ensemble (FAFE), to estimate the density of states (DOS) and to enhance sampling in large systems. FAFE calculates the means of an arbitrary extensive variable $U$ in…

Statistical Mechanics · Physics 2008-11-13 Xin Zhou , Yi Jiang

We present an accurate and efficient finite-difference formulation and parallel implementation of Kohn-Sham Density (Operator) Functional Theory (DFT) for non periodic systems embedded in a bulk environment. Specifically, employing…

Computational Physics · Physics 2020-11-30 Swarnava Ghosh , Kaushik Bhattacharya

In fluorescence diffuse optical tomography (fDOT), the reconstruction of the fluorophore concentration inside the target body is usually carried out using a normalized Born approximation model where the measured fluorescent emission data is…

Computational Physics · Physics 2015-01-05 Meghdoot Mozumder , Tanja Tarvainen , Simon Arridge , Jari P. Kaipio , Cosimo d'Andrea , Ville Kolehmainen

Simulating a Gaussian process requires sampling from a high-dimensional Gaussian distribution, which scales cubically with the number of sample locations. Spectral methods address this challenge by exploiting the Fourier representation,…

Machine Learning · Statistics 2026-02-27 Arsalan Jawaid , Abdullah Karatas , Jörg Seewig
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