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Joel D. Eaves

Publications and source records attributed to Joel D. Eaves.

13 recordsLinked to original sources

The Integral Decimation Method for Quantum Dynamics and Statistical Mechanics

The solutions to many problems in the mathematical, computational, and physical sciences often involve multidimensional integrals. A direct numerical evaluation of the integral incurs a computational cost that is exponential in the number of dimensions, a phenomenon called the curse of dimensionality. The problem is so substantial that one usually employs sampling methods, like Monte Carlo, to avoid integration altogether. Here, we derive and implement a quantum-inspired algorithm to decompose a multidimensional integrand into a product of matrix-valued functions -- a spectral tensor train -- changing the computational complexity of integration from exponential to polynomial. The algorithm constructs a spectral tensor train representation of the integrand by applying a sequence of quantum gates, where each gate corresponds to an interaction that involves increasingly more degrees of freedom in the action. Because it allows for the systematic elimination of small contributions to the integral through decimation, we call the method integral decimation. The functions in the spectral basis are analytically differentiable and integrable, and in applications to the partition function, integral decimation numerically factorizes an interacting system into a product of non-interacting ones. We illustrate integral decimation by evaluating the absolute free energy and entropy of a chiral XY model as a continuous function of temperature. We also compute the nonequilibrium time-dependent reduced density matrix of a quantum chain with between two and forty levels, each coupled to colored noise. When other methods provide numerical solutions to these models, they quantitatively agree with integral decimation. When conventional methods become intractable, integral decimation can be a powerful alternative.

cond-mat.stat-mech↗

Stochastic Path Compression for Spectral Tensor Networks on Cyclic Graphs

We develop a new approach to compress cyclic tensor networks called stochastic path compression (SPC) that uses an iterative importance sampling procedure to target edges with large bond-dimensions. Closed random walks in SPC form compression pathways that spatially localize large bond-dimensions in the tensor network. Analogous to the phase separation of two immiscible liquids, SPC separates the graph of bond-dimensions into spatially distinct high and low density regions. When combined with our integral decimation algorithm, SPC facilitates the accurate compression of cyclic tensor networks with continuous degrees of freedom. To benchmark and illustrate the methods, we compute the absolute thermodynamics of $q$-state clock models on two-dimensional square lattices and an XY model on a Watts-Strogatz graph, which is a small-world network with random connectivity between spins.

cond-mat.stat-mech↗

Accurate Numerical Simulations of Open Quantum Systems Using Spectral Tensor Trains

Decoherence between qubits is a major bottleneck in quantum computations. Decoherence results from intrinsic quantum and thermal fluctuations as well as noise in the external fields that perform the measurement and preparation processes. With prescribed colored noise spectra for intrinsic and extrinsic noise, we present a numerical method, Quantum Accelerated Stochastic Propagator Evaluation (Q-ASPEN), to solve the time-dependent noise-averaged reduced density matrix in the presence of intrinsic and extrinsic noise. Q-ASPEN is arbitrarily accurate and can be applied to provide estimates for the resources needed to error-correct quantum computations. We employ spectral tensor trains, which combine the advantages of tensor networks and pseudospectral methods, as a variational ansatz to the quantum relaxation problem and optimize the ansatz using methods typically used to train neural networks. The spectral tensor trains in Q-ASPEN make accurate calculations with tens of quantum levels feasible. We present benchmarks for Q-ASPEN on the spin-boson model in the presence of intrinsic noise and on a quantum chain of up to 32 sites in the presence of extrinsic noise. In our benchmark, the memory cost of Q-ASPEN scales linearly with the system size once the number of states is larger than the number of basis functions.

quant-ph↗

Direct Numerical Solutions to Stochastic Differential Equations with Multiplicative Noise

Inspired by path-integral solutions to the quantum relaxation problem, we develop a numerical method to solve classical stochastic differential equations with multiplicative noise that avoids averaging over trajectories. To test the method, we simulate the dynamics of a classical oscillator multiplicatively coupled to non-Markovian noise. When accelerated using tensor factorization techniques, it accurately estimates the transition into the bifurcation regime of the oscillator and outperforms trajectory-averaging simulations with a computational cost that is orders of magnitude lower.

cond-mat.stat-mech↗

Remembering the work of Phillip L. Geissler: A coda to his scientific trajectory

Phillip L. Geissler made important contributions to the statistical mechanics of biological polymers, heterogeneous materials, and chemical dynamics in aqueous environments. He devised analytical and computational methods that revealed the underlying organization of complex systems at the frontiers of biology, chemistry, and materials science. In this retrospective, we celebrate his work at these frontiers.

cond-mat.stat-mech↗

Efficient Photon Upconversion Enabled by Strong Coupling Between Organic Molecules and Quantum Dots

Hybrid structures formed between organic molecules and inorganic quantum dots can accomplish unique photophysical transformations by taking advantage of their disparate properties. The electronic coupling between these materials is typically weak, leading photoexcited charge carriers to spatially localize to a dot or a molecule at its surface. However, we show that by converting a chemical linker that covalently binds anthracene molecules to silicon quantum dots from a carbon-carbon single bond to a double bond, we access a strong-coupling regime where excited carriers spatially delocalize across both anthracene and silicon. By pushing the system to delocalize, we design a photon upconversion system with a higher efficiency (17.2%) and lower threshold intensity (0.5 W/cm^2) than that of a corresponding weakly-coupled system. Our results show that strong coupling between molecules and nanostructures achieved through targeted linking chemistry provides a new route for tailoring properties in materials for light-driven applications.

physics.chem-ph↗

Triplet-Pair Spin Signatures from Macroscopically Aligned Heteroacenes in an Oriented Single Crystal

The photo-driven process of singlet fission generates coupled triplet pairs (TT) with fundamentally intriguing and potentially useful properties. The quintet 5TT0 sublevel is particularly interesting for quantum information because it is highly entangled, addressable with microwave pulses, and could be detected using optical techniques. Previous theoretical work on a model Hamiltonian and nonadiabatic transition theory, called the JDE model, has determined that this sublevel can be selectively populated if certain conditions are met. Among the most challenging, the molecules within the dimer undergoing singlet fission must have their principal magnetic axes parallel to one another and to an applied Zeeman field B0. Here, we present time-resolved paramagnetic resonance (TR-EPR) spectroscopy of a single crystal sample of a novel tetracenethiophene compound featuring arrays of dimers aligned in this manner, mounted so that the orientation of the field relative to the molecular axes could be controlled. The observed spin sublevel populations in the paired TT and unpaired (T+T) triplets are consistent with predictions from the JDE model, including preferential 5TT0 formation at z||B0, with one caveat - two 5TT spin sublevels have little to no population. This may be due to crossings between the 5TT and 3TT manifolds in the field range investigated by TR-EPR, consistent with the inter-triplet exchange energy determined by monitoring photoluminescence at varying magnetic fields.

physics.chem-ph↗

Entangled, Spin-polarized Excitons from Singlet Fission in a Rigid Dimer

Singlet fission, a process that splits a singlet exciton into a biexciton, has promise in quantum information. We report time-resolved electron paramagnetic resonance measurements on a molecule, TIPS-BP1$'$, designed to exhibit strongly state-selective relaxation to specific magnetic spin sublevels. The resulting optically pumped "spin polarization" is a nearly pure initial state from the ensemble. The long-lived spin coherences modulate the signal intrinsically, allowing a new measurement scheme that substantially removes noise and uncertainty in the magnetic resonance spectra. A nonadiabatic transition theory with a minimal number of spectroscopic parameters allows the quantitative assignment and interpretation of the spectra. The rigid, covalently bound dimer, TIPS-BP1$'$, supports persistent spin coherences at temperatures far higher than those used in conventional quantum hardware.

physics.chem-ph↗

Clock Transitions Guard Against Spin Decoherence in Singlet Fission

Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field, can substantially increase coherence times. We show how CTs can dampen intrinsic and extrinsic sources of quantum noise in molecules. Conical intersections between two periodic potentials form CTs in electron paramagnetic resonance experiments of the spin-polarized singlet fission photoproduct. We report on a pair of CTs for a two-chromophore molecule in terms of the Zeeman field strength, molecular orientation relative to the field, and molecular geometry.

physics.chem-ph↗

On the Nature of Trapped-Hole States in CdS Nanocrystals and the Mechanism of their Diffusion

Recent transient absorption experiments on CdS nanorods suggest that photoexcited holes rapidly trap to the surface of these particles and then undergo diffusion along the rod surface. In this paper, we present a semiperiodic DFT model for the CdS nanocrystal surface, analyze it, and comment on the nature of both the hole-trap states and the mechanism by which the holes diffuse. Hole states near the top of the valence band form an energetic near continuum with the bulk, and localize to the non-bonding sp$^3$ orbitals on surface sulfur atoms. After localization, the holes form nonadiabatic small polarons that move between the sulfur orbitals on the surface of the particle in a series of uncorrelated, incoherent, thermally-activated hops at room temperature. The surface-trapped holes are deeply in the weak-electronic coupling limit and, as a result, undergo slow diffusion.

physics.chem-ph↗

Atomistic Hydrodynamics and the Dynamical Hydrophobic Effect in Porous Graphene

Mirroring their role in electrical and optical physics, two-dimensional crystals are emerging as novel platforms for fluid separations and water desalination, which are hydrodynamic processes that occur in nanoscale environments. For numerical simulation to play a predictive and descriptive role, one must have theoretically sound methods that span orders of magnitude in physical scales, from the atomistic motions of particles inside the channels to the large-scale hydrodynamic gradients that drive transport. Here, we use constraint dynamics to derive a nonequilibrium molecular dynamics method for simulating steady-state mass flow of a fluid moving through the nanoscopic spaces of a porous solid. After validating our method on a model system, we use it to study the hydrophobic effect of water moving through pores of electrically doped single-layer graphene. The trend in permeability that we calculate does not follow the hydrophobicity of the membrane, but is instead governed by a crossover between two competing molecular transport mechanisms.

cond-mat.stat-mech↗

The Panic Model: Flocking with Minimal Cooperativity

We present a 2D lattice model of self-propelled spins that can only change direction upon collision with another spin. We show that even with ballistic motion and minimal cooperativity, these spins display robust flocking behavior at nearly all densities, forming long bands of stripes. The structural transition in this system can be characterized by an order parameter, and we demonstrate that if this parameter is studied as a dynamical variable rather than a steady-state observable, we can extract a detailed picture of how the flocking mechanism varies with density.

cond-mat.soft↗

Carrier Transport in Heterojunction Nanocrystals Under Strain

We present a theory for carrier transport in semiconducting nanoscale heterostructures that emphasizes the effects of strain at the interface between two different crystal structures. An exactly solvable model shows that the interface region, or junction, acts as a scattering potential that facilitates charge separation but also supports bound interfacial states. As a case study, we model a Type-II CdS/ZnSe heterostructure. After advancing a theory similar to that employed in model molecular conductance calculations, we calculate the electron and hole photocurrents and conductances, including non-linear effects, through the junction at steady-state.

cond-mat.mes-hall↗