A5013851971- Spectroscopy and Quantum Chemical Studies
- Advanced Thermodynamics and Statistical Mechanics
- Quantum Information and Cryptography
- Photochemistry and Electron Transfer Studies
- Quantum, superfluid, helium dynamics
- Thermal Radiation and Cooling Technologies
- Quantum and electron transport phenomena
- Molecular Junctions and Nanostructures
- Photoreceptor and optogenetics research
- Quantum many-body systems
- Advanced Thermoelectric Materials and Devices
- Advanced NMR Techniques and Applications
- Spectroscopy and Laser Applications
- Quantum Computing Algorithms and Architecture
- Strong Light-Matter Interactions
- Advanced Chemical Physics Studies
- Laser-Plasma Interactions and Diagnostics
- TiO2 Photocatalysis and Solar Cells
- Thermal properties of materials
- Pancreatitis Pathology and Treatment
- Quantum Mechanics and Applications
- Diabetes Management and Research
- Porphyrin and Phthalocyanine Chemistry
- Diabetes Treatment and Management
- Infrastructure Maintenance and Monitoring
Stanford University
2018-2023
University of Toronto
2020-2023
Yale University
2017-2023
Consensus around an efficient second-line treatment option for type 2 diabetes (T2D) remains ambiguous. The availability of electronic medical records and insurance claims data, which capture routine practice, accessed via the Observational Health Data Sciences Informatics network presents opportunity to generate evidence effectiveness treatments.To identify drug classes among sulfonylureas, dipeptidyl peptidase 4 (DPP-4) inhibitors, thiazolidinediones are associated with reduced hemoglobin...
Understanding the effect of vibronic coupling on electron transfer (ET) rates is a challenge common to wide range applications, from electrochemical synthesis and catalysis biochemical reactions solar energy conversion. The Marcus-Jortner-Levich (MJL) theory offers model ET based simple analytic expression with few adjustable parameters. However, MJL equation in conjunction density functional (DFT) has yet be established as predictive first-principles methodology. A framework presented for...
Theoretical treatments of periodically driven quantum thermal machines (PD-QTMs) are largely focused on the limit-cycle stage operation characterized by a periodic state system. Yet, this regime is not immediately accessible for experimental verification. Here, we present general thermodynamic framework that handles performance PD-QTMs both before and during operation. It achieved observing periodicity may break down at ensemble average level, even in phase. With observation, using...
Whether the strong coupling to thermal baths can improve performance of quantum machines remains an open issue under active debate. Here we revisit operating with quasistatic Carnot cycle and aim unveil role in maximum efficiency. Our analysis builds upon definitions excess work heat derived from exact formulation first law thermodynamics for working substance, which captures non-Gibbsian equilibrium state that emerges at couplings during isothermal processes. These differ conventional ones...
In the case of quantum systems interacting with multiple environments, time-evolution reduced density matrix is described by Liouvillian. For a variety physical observables, long-time limit or steady state solution needed for computation desired observables. inverse design optimal control such systems, common approaches are based on brute-force search strategies. Here, we present novel methodology, automatic differentiation, capable differentiating respect to any parameter Our approach has...
The computation and interpretation of nonlinear vibrational spectroscopy is vital importance for understanding a wide range dynamical processes in molecular systems. Here, we introduce an approach to evaluate multi-time response functions terms double symmetrized Kubo transformed thermal correlation functions. Furthermore, extension ring polymer dynamics these transforms. Benchmark calculations show that the approximations are useful short times even operators, providing consistent...
The non-equilibrium stationary coherences that form in donor-acceptor systems are investigated to determine their relationship the efficiency of energy transfer a neighboring reaction center. It is found effects asymmetry dimer generally detrimental energy. Four types examined, arising from combinations localized trapping, delocalized (Forster) eigenstate dephasing, and site basis dephasing. In cases interplay between gap excited states environment shown give rise turnover effect under weak...
Matsubara dynamics has recently emerged as the most general form of a quantum-Boltzmann-conserving classical theory for calculation single-time correlation functions. Here, we present generalization evaluation multitime We first show that approximation can also be used to approximate two-time symmetrized double Kubo transformed function. By straightforward extension these ideas realm, obtained fully Although not practical method, due presence phase-term, this formulation represents benchmark...
Based on a recently developed generalization of Matsubara dynamics to the multi-time realm, we present formal derivation generalizations ring-polymer molecular dynamics, thermostatted (TRPMD), centroid (CMD), and mean-field dynamics. Additionally, analyze short-time accuracy each methodology. We find that for correlation functions linear operators, (T)RPMD is accurate up order t3, while CMD only correct t, indicating degradation in these methodologies with respect single-time counterparts....
We introduce a general method based on the operators of Dyson-Masleev transformation to map Hamiltonian an arbitrary model system into circuit Quantum Electrodynamics (cQED) processor. Furthermore, we modular approach programming cQED processor with components corresponding mapping Hamiltonian. The is illustrated as applied quantum dynamics simulations Fenna-Matthews-Olson (FMO) complex and spin-boson charge transfer. Beyond applications molecular Hamiltonians, provides implement any unitary...
Two self-assembled photoanodes have been constructed by exploiting the unique optical and structural properties of aluminum(III) porphyrin (AlPor) in conjunction with TiO2 nanoparticles as an electron acceptor bis(p-anisole)aminopyridine (BAA–Py) donor. AlPor is bound to surface either: (i) a benzohydroxamic acid bridge, which hydroxamic acts anchor or (ii) direct covalent binding Al via ether bond. The open sixth coordination site center then used coordinate BAA–Py through Lewis acid–base...
The simulation of multidimensional vibrational spectroscopy condensed-phase systems including nuclear quantum effects is challenging since full quantum-mechanical calculations are still intractable for large comprising many degrees freedom. Here, we apply the recently developed double Kubo transform (DKT) methodology in combination with ring-polymer molecular dynamics (RPMD) evaluating multi-time correlation functions [K. A. Jung et al., J. Chem. Phys. 148, 244105 (2018)], providing a...
The nonequilibrium steady state (NESS) of a quantum network is central to host physical and biological scenarios. Examples include natural processes such as vision photosynthesis well technical devices photocells, both activated by incoherent light (e.g., sunlight) leading transport. Assessing time scales the relevant chemical in thus utmost interest our goal this paper. Here, completely general approach defining components NESS obtaining rates between these provided. Quantum effects are...
Time-resolved scattering experiments enable imaging of materials at the molecular scale with femtosecond time resolution. However, in disordered media they provide access to just one radial dimension thus limiting study orientational structure and dynamics. Here we introduce a rigorous practical theoretical framework for predicting interpreting combining optically induced anisotropy time-resolved scattering. Using impulsive nuclear Raman ultrafast x-ray chloroform simulations, demonstrate...
Electron transfer at electrode interfaces to molecules in solution or the surface plays a vital role numerous technological processes. However, treating these processes requires unified and accurate treatment of fermionic states their coupling molecule being oxidized reduced electrochemical and, turn, way molecular energy levels are modulated by bosonic nuclear modes solvent. Here we present physically transparent quasiclassical scheme treat electron presence vibrations using an...
Uncovering whether strong system-bath coupling can be an advantageous operation resource for energy conversion facilitate the development of efficient quantum heat engines (QHEs). Yet, a consensus on this ongoing debate is still lacking owing to challenges arising from treating couplings. Here we conclude optimal linear cyclic QHEs operated under small temperature difference by revealing detrimental role in their operations. We analytically demonstrate that both efficiency at maximum power...
Inverse design of a property that depends on the steady-state an open quantum system is commonly done by grid-search type methods. In this paper we present new methodology allows us to compute gradient with respect any parameter Hamiltonian using implicit differentiation theorem. As example, simulation spin-boson model where solution obtained Redfield theory.
The third-order response lies at the heart of simulating and interpreting nonlinear spectroscopies ranging from two dimensional infrared (2D-IR) to 2D electronic (2D-ES), sum frequency generation (2D-SFG). extra time dimensions in these provides access rich information on vibrational states present, coupling between them, resulting rates which they exchange energy that are obscured linear spectroscopy, particularly for condensed phase systems usually contain many overlapping features. While...
A strong light-matter interaction and the resulting polaritons provide a promising knob to control energy population transfer over long length scales. Yet, existing studies have been exclusively limited single-cavity scenario. Little is known about whether multiple cavities can facilitate new strategies. Here, we reveal that interplay of cavity-cavity coherence vibrational coupling induce stationary current between two identical, weakly coupled hybrid polaritonic systems at thermal...
Electron transfer at electrode interfaces to molecules in solution or the surface plays a vital role numerous technological processes. However, treating these processes requires unified and accurate treatment of fermionic states their coupling molecule being oxidized reduced electrochemical and, turn, way molecular energy levels are modulated by bosonic nuclear modes solvent. Here we present physically transparent quasiclassical scheme treat electron presence vibrations using an...
We introduce a general method based on the operators of Dyson-Masleev transformation to map Hamiltonian an arbitrary model system into circuit Quantum Electrodynamics (cQED) processor. Furthermore, we modular approach program cQED processor with components corresponding mapping Hamiltonian. The is illustrated as applied quantum dynamics simulations Fenna-Matthews-Olson (FMO) complex and spin-boson charge transfer. Beyond applications molecular Hamiltonians, provides implement any unitary...
Whether the strong coupling to thermal baths can improve performance of quantum machines remains an open issue under active debate. Here, we revisit operating with quasi-static Carnot cycle and aim unveil role in maximum efficiency. Our analysis builds upon definitions excess work heat derived from exact formulation first law thermodynamics for working substance, which captures non-Gibbsian equilibrium state that emerges at couplings during isothermal processes. These differ conventional...