GaSb band-structure models for electron density determinations from Raman measurements.

We investigate the use of Raman spectroscopy to measure carrier concentrations in GaSb epilayers to aid in the development of this technique for the nondestructive characterization of transport properties in doped semiconductors. The carrier concentration is quantified by modeling the measured coupled optical phonon-free carrier plasmon mode spectra. We employ the Lindhard-Mermin optical susceptibility model with contributions from carriers in the two lowest GaSb conduction-band minima, the and minima.

Quantum thermodynamics of periodically driven polaritonic systems.

We investigate the energy distribution and quantum thermodynamics in periodically-driven polaritonic systems in the stationary state at room temperature. Specifically, we consider an exciton strongly coupled to a harmonic oscillator and quantify the energy reorganization between these two systems and their interaction as a function of coupling strength, driving force, and detuning. After deriving the quantum master equation for the polariton density matrix with weak environment interactions, we obtain the dissipative time propagator and the long-time evolution of an equilibrium initial state.

Strong Coupling in Infrared Plasmonic Cavities.

Controlling molecular spectroscopy and even chemical behavior in a cavity environment is a subject of intense experimental and theoretical interest. In Fabry-Pérot cavities, strong (radiation-matter) coupling phenomena without an intense radiation field often rely on the number of chromophore molecules collectively interacting with a cavity mode. For plasmonic cavities, the cavity field-matter coupling can be strong enough to manifest strong coupling involving even a single molecule.

Coupling, lifetimes, and "strong coupling" maps for single molecules at plasmonic interfaces.

The interaction between excited states of a molecule and excited states of a metal nanostructure (e.g., plasmons) leads to hybrid states with modified optical properties.

Metal adsorbate interactions and the convergence of density functional calculations.

The adsorption of metal atoms on nanostructures, such as graphene and nanotubes, plays an important role in catalysis, electronic doping, and tuning material properties. Quantum chemical calculations permit the investigation of this process to discover desirable interactions and obtain mechanistic insights into adsorbate behavior, of which the binding strength is a central quantity. Binding strengths, however, vary widely in the literature, even when using almost identical computational methods.

Optimal in situ electromechanical sensing of molecular species.

We investigate protocols for optimal molecular detection with electromechanical nanoscale sensors under ambient conditions. Our models are representative of suspended graphene nanoribbons, which due to their piezoelectric and electronic properties provide responsive and versatile sensors. In particular, we analytically account for the corrections in the electronic transmission function and signal-to-noise ratio originating in environmental perturbations, such as thermal fluctuations and solvation effects.

Extracting electron densities in -type GaAs from Raman spectra: Comparisons with Hall measurements.

We demonstrate quantitatively how values of electron densities in GaAs extracted from Raman spectra of two samples depend on models used to describe electric susceptibility and band structure. We, therefore, developed a theory that is valid for any temperature, doping level, and energy ratio proportional to =( + ) (where is the magnitude of wave vector, is Raman frequency, and is plasmon damping). We use a full Mermin-Lindhard description of Raman line shape and compare -type GaAs spectra obtained from epilayers with our simulated spectra.

Generalized Voigt broadening due to thermal fluctuations of electromechanical nanosensors and molecular electronic junctions.

Graphene and other 2D materials give a platform for electromechanical sensing of biomolecules in aqueous, room temperature environments. The electronic current changes in response to mechanical deflection, indicating the presence of forces due to interactions with, e.g.

Simultaneous weak measurement of non-commuting observables: a generalized Arthurs-Kelly protocol.

In contrast to a projective quantum measurement, in a weak measurement the system is only weakly perturbed while only partial information on the measured observable is obtained. A simultaneous measurement of non-commuting observables cannot be projective, however the strongest possible such measurement can be defined as providing their values at the smallest uncertainty limit. Starting with the Arthurs and Kelly (AK) protocol for such measurement of position and momentum, we derive a systematic extension to a corresponding weak measurement along three steps: First, a plausible form of the weak measurement operator analogous to the Gaussian Kraus operator, often used to model a weak measurement of a single observable, is obtained by projecting a naïve extension (valid for commuting observable) onto the corresponding Gabor space.

Pump-Probe Noise Spectroscopy of Molecular Junctions.

The slow response of electronic components in junctions limits the direct applicability of pump-probe type spectroscopy in assessing the intramolecular dynamics. Recently the possibility of getting information on a sub-picosecond time scale from dc current measurements was proposed. We revisit the idea of picosecond resolution by pump-probe spectroscopy from dc measurements and show that any intramolecular dynamics not directly related to charge transfer in the current direction is missed by current measurements.

Quantum thermodynamics: a nonequilibrium Green's function approach.

We establish the foundations of a nonequilibrium theory of quantum thermodynamics for noninteracting open quantum systems strongly coupled to their reservoirs within the framework of the nonequilibrium Green's functions. The energy of the system and its coupling to the reservoirs are controlled by a slow external time-dependent force treated to first order beyond the quasistatic limit. We derive the four basic laws of thermodynamics and characterize reversible transformations.

A non-equilibrium equation-of-motion approach to quantum transport utilizing projection operators.

We consider a projection operator approach to the non-equilibrium Green function equation-of-motion (PO-NEGF EOM) method. The technique resolves problems of arbitrariness in truncation of an infinite chain of EOMs and prevents violation of symmetry relations resulting from the truncation (equivalence of left- and right-sided EOMs is shown and symmetry with respect to interchange of Fermi or Bose operators before truncation is preserved). The approach, originally developed by Tserkovnikov (1999 Theor.

Interpreting single turnover catalysis measurements with constrained mean dwell times.

Observation of a chemical transformation at the single-molecule level yields a detailed view of kinetic pathways contributing to the averaged results obtained in a bulk measurement. Studies of a fluorogenic reaction catalyzed by gold nanoparticles have revealed heterogeneous reaction dynamics for these catalysts. Measurements on single nanoparticles yield binary trajectories with stochastic transitions between a dark state in which no product molecules are adsorbed and a fluorescent state in which one product molecule is present.