Strong Purcell enhancement at telecom wavelengths afforded by spinel Fe3O4 nanocrystals with size-tunable plasmonic properties.

Developments in the field of nanoplasmonics have the potential to advance applications from information processing and telecommunications to light-based sensing. Traditionally, nanoscale noble metals such as gold and silver have been used to achieve the targeted enhancements in light-matter interactions that result from the presence of localized surface plasmons (LSPs). However, interest has recently shifted to intrinsically doped semiconductor nanocrystals (NCs) for their ability to display LSP resonances (LSPRs) over a much broader spectral range, including the infrared (IR). Among semiconducting plasmonic NCs, spinel metal oxides (sp-MOs) are an emerging class of materials with distinct advantages in accessing the telecommunications bands in the IR and affording useful environmental stability. Here, we report the plasmonic properties of Fe3O4 sp-MO NCs, known previously only for their magnetic functionality, and demonstrate their ability to modify the light-emission properties of telecom-emitting quantum dots (QDs). We establish the synthetic conditions for tuning sp-MO NC size, composition and doping characteristics, resulting in unprecedented tunability of electronic behavior and plasmonic response over 450 nm. In particular, with diameter-dependent variations in free-electron concentration across the Fe3O4 NC series, we introduce a strong NC size dependency onto the optical response. In addition, our observation of plasmonics-enhanced decay rates from telecom-emitting QDs reveals Purcell enhancement factors for simple plasmonic-spacer-emitter sandwich structures up to 51-fold, which are comparable to values achieved previously only for emitters in the visible range coupled with conventional noble metal NCs.

Temperature-Induced Plasmon Excitations for the α-T3 Lattice in Perpendicular Magnetic Field.

We have investigated the α-T3 model in the presence of a mass term which opens a gap in the energy dispersive spectrum, as well as under a uniform perpendicular quantizing magnetic field. The gap opening mass term plays the role of Zeeman splitting at low magnetic fields for this pseudospin-1 system, and, as a consequence, we are able to compare physical properties of the the α-T3 model at low and high magnetic fields. Specifically, we explore the magnetoplasmon dispersion relation in these two extreme limits. Central to the calculation of these collective modes is the dielectric function which is determined by the polarizability of the system. This latter function is generated by transition energies between subband states, as well as the overlap of their wave functions.

Second-harmonic generation in nonlinear plasmonic lattices enhanced by quantum emitter gain medium.

We report on a theoretical study of second-harmonic generation (SHG) in plasmonic nanostructures interacting with two-level quantum emitters (QEs) under incoherent energy pump. We generalize the driven-dissipative Tavis-Cummings model by introducing the anharmonic surface plasmon-polariton (SPP) mode coupled to QEs and examine physical properties of corresponding SPP-QE polariton states. Our calculations of the SHG efficiency for strong QE-SPP coupling demonstrate orders of magnitude enhancement facilitated by the polariton gain. We further discuss time-domain numerical simulations of SHG in a square lattice comprising Ag nanopillars coupled to QEs utilizing a fully vectorial nonperturbative nonlinear hydrodynamic model for conduction electrons coupled to Maxwell-Bloch equations for QEs. The simulations support the idea of gain enhanced SHG and show orders of magnitude increase in the SHG efficiency as the QEs are tuned in resonance with the lattice plasmon mode and brought above the population inversion threshold by incoherent pumping. By varying pump frequency and tuning QEs to a localized plasmon mode, we demonstrate further enhancement of the SHG efficiency facilitated by strong local electric fields. The incident light polarization dependence of the SHG is examined and related to the symmetries of participating plasmon modes.

Magnetoplasmons for the α-T3 model with filled Landau levels.

Using the $\alpha-T_3$ model, we carried out analytical and numerical calculations for the static and dynamic polarization functions in the presence of a perpendicular magnetic field. The model involves a parameter $\alpha$ which is the ratio of the hopping strength from an atom at the center of a honeycomb lattice to one of the atoms on the hexagon to the hopping strength around its rim. Our results were employed to determine the longitudinal dielectric function and the magnetoplasmon dispersion relation. The magnetic field splits the continuous valence, conduction and at energy subband into discrete Landau levels which present significant effects on the polarization function and magnetoplasmon dispersion. This includes the fact that the energies of the Landau levels are valley dependent which leads to different behaviors of the polarization function as the hopping parameter $\alpha$ (or $\phi = tan^{-1}\alpha$) is reduced continuously toward zero. This essential critical behavior of the polarization function leads to a softening of a magnetoplasmon mode. We present results for a doped layer in the integer quantum Hall regime for fixed hopping parameter $\alpha$ and various magnetic fields as well as chosen magnetic field and different $\alpha$ in the random phase approximation.

Resonance Raman signature of intertube excitons in compositionally-defined carbon nanotube bundles.

Electronic interactions in low-dimensional nanomaterial heterostructures can lead to novel optical responses arising from exciton delocalization over the constituent materials. Similar phenomena have been suggested to arise between closely interacting semiconducting carbon nanotubes of identical structure. Such behavior in carbon nanotubes has potential to generate new exciton physics, impact exciton transport mechanisms in nanotube networks, and place nanotubes as one-dimensional models for such behaviors in systems of higher dimensionality. Here we use resonance Raman spectroscopy to probe intertube interactions in (6,5) chirality-enriched bundles. Raman excitation profiles for the radial breathing mode and G-mode display a previously unobserved sharp resonance feature. We show the feature is evidence for creation of intertube excitons and is identified as a Fano resonance arising from the interaction between intratube and intertube excitons. The universality of the model suggests that similar Raman excitation profile features may be observed for interlayer exciton resonances in 2D multilayered systems.

Plasmonic giant quantum dots: hybrid nanostructures for truly simultaneous optical imaging, photothermal effect and thermometry.

Hybrid semiconductor-metal nanoscale constructs are of both fundamental and practical interest. Semiconductor nanocrystals are active emitters of photons when stimulated optically, while the interaction of light with nanosized metal objects results in scattering and ohmic damping due to absorption. In a combined structure, the properties of both components can be realized together. At the same time, metal-semiconductor coupling may intervene to modify absorption and/or emission processes taking place in the semiconductor, resulting in a range of effects from photoluminescence quenching to enhancement. We show here that photostable 'giant' quantum dots when placed at the center of an ultrathin gold shell retain their key optical property of bright and blinking-free photoluminescence, while the metal shell imparts efficient photothermal transduction. The latter is despite the highly compact total particle size (40-60 nm "inorganic" diameter and <100 nm hydrodynamic diameter) and the very thin nature of the optically transparent Au shell. Importantly, the sensitivity of the quantum dot emission to local temperature provides a novel internal thermometer for recording temperature during infrared irradiation-induced photothermal heating.

Influence of exciton dimensionality on spectral diffusion of single-walled carbon nanotubes.

We study temporal evolution of photoluminescence (PL) spectra from individual single-walled carbon nanotubes (SWCNTs) at cryogenic and room temperatures. Sublinear and superlinear correlations between fluctuating PL spectral positions and line widths are observed at cryogenic and room temperatures, respectively. We develop a simple model to explain these two different spectral diffusion behaviors in the framework of quantum-confined Stark effect (QCSE) caused by surface charges trapped in the vicinity of SWCNTs. We show that the wave function properties of excitons, namely, localization at cryogenic temperature and delocalization at room temperature, play a critical role in defining sub- and superlinear correlations. Room temperature PL spectral positions and line widths of SWCNTs coupled to gold dimer nanoantennas on the other hand exhibit sublinear correlations, indicating that excitonic emission mainly originates from nanometer range regions and excitons appear to be localized. Our numerical simulations show that such apparent localization of excitons results from plasmonic confinement of excitation and an enhancement of decay rates in the gap of the dimer nanoantennas.

Effect of localized surface-plasmon mode on exciton transport and radiation emission in carbon nanotubes.

We report on a general theoretical approach to study exciton transport and emission in a single-walled carbon nanotube (SWNT) in the presence of a localized surface-plasmon (SP) mode within a metal nanoparticle interacting via near-field coupling. We derive a set of quantum mechanical equations of motion and approximate rate equations that account for the exciton, SP, and the environmental degrees of freedom. The material equations are complemented by an expression for the radiated power that depends on the exciton and SP populations and coherences, allowing for an examination of the angular distribution of the emitted radiation that would be measured in experiment. Numerical simulations for a (6,5) SWNT and cone-shaped Ag metal tip (MT) have been performed using this methodology. Comparison with physical parameters shows that the near-field interaction between the exciton-SP occurs in a weak coupling regime, with the diffusion processes being much faster than the exciton-SP population exchange. In such a case, the effect of the exciton population transfer to the MT with its subsequent dissipation (i.e., the Förster energy transfer) is to modify the exciton steady state distribution while reducing the equilibration time for excitons to reach a steady sate distribution. We find that the radiation distribution is dominated by SP emission for a SWNT-MT separation of a few tens of nanometers due to the fast SP emission rate, whereas the exciton-SP coherences can cause its rotation.

Photon dressed electronic states in topological insulators: tunneling and conductance.

We have obtained analytic results for the surface states of three-dimensional topological insulators in the presence of circularly polarized light. This electron-photon interaction results in an energy gap as well as a novel energy dispersion of the dressed electron-photon states, different from both graphene and the standard two-dimensional electron gas (2DEG). Additionally, we made calculations of the ballistic conductance and Klein tunneling in both two- and three-dimensional topological insulators as well as investigating how these phenomena are affected in the presence of circularly polarized light. We have found a critical energy for an incoming particle, separating two substantially different types of tunneling.

Effects of nonlocal plasmons in gapped graphene micro-ribbon array and two-dimensional electron gas on near-field electromagnetic response in the deep subwavelength regime.

A self-consistent theory involving Maxwell's equations and a density-matrix linear-response theory is solved for an electromagnetically coupled doped graphene micro-ribbon array (GMRA) and a quantum well (QW) electron gas sitting at an interface between a half-space of air and another half-space of a doped semiconductor substrate, which supports a surface-plasmon mode in our system. The coupling between a spatially modulated total electromagnetic (EM) field and the electron dynamics in a Dirac-cone of a graphene ribbon, as well as the coupling of the far-field specular and near-field higher-order diffraction modes, are included in the derived electron optical-response function. Full analytical expressions are obtained with nonlocality for the optical-response functions of a two-dimensional electron gas and a graphene layer with an induced bandgap, and are employed in our numerical calculations beyond the long-wavelength limit (Drude model). Both the near-field transmissivity and reflectivity spectra, as well as their dependence on different configurations of our system and on the array period, ribbon width, graphene chemical potential of QW electron gas and bandgap in graphene, are studied. Moreover, the transmitted E-field intensity distribution is calculated to demonstrate its connection to the mixing of specular and diffraction modes of the total EM field. An externally tunable EM coupling among the surface, conventional electron-gas and massless graphene intraband plasmon excitations is discovered and explained. Furthermore, a comparison is made between the dependence of the graphene-plasmon energy on the ribbon's width and chemical potential in this paper and the recent experimental observation given by [Nat. Nanotechnol.6, 630-634 (2011)] for a GMRA in the terahertz-frequency range.

Anomalous photon-assisted tunneling in graphene.

We investigated the transmission of Dirac electrons through a potential barrier in the presence of circularly polarized light. An anomalous photon-assisted enhanced transmission is predicted and explained. It is demonstrated that the perfect transmission for nearly head-on collision in infinite graphene is suppressed in gapped dressed states of electrons, which is further accompanied by a shift of peaks as a function of the incident angle away from head-on collision. In addition, the perfect transmission is partially suppressed by a photon-induced gap in illuminated graphene. After the effect of rough edges of the potential barrier or impurity scattering is included, the perfect transmission with no potential barrier becomes completely suppressed and the energy range for the photon-assisted transmission is reduced at the same time.

Plasma excitations in graphene: their spectral intensity and temperature dependence in magnetic field.

In this paper, we calculated the dielectric function, the loss function, the magnetoplasmon dispersion relation and the temperature-induced transitions for graphene in a uniform perpendicular magnetic field B. The calculations were performed using the Peierls tight-binding model to obtain the energy band structure and the random-phase approximation to determine the collective plasma excitation spectrum. The single-particle and collective excitations have been precisely identified based on the resonant peaks in the loss function. The critical wave vector at which plasmon damping takes place is clearly established. This critical wave vector depends on the magnetic field strength as well as the levels between which the transition takes place. The temperature effects were also investigated. At finite temperature, there are plasma resonances induced by the Fermi distribution function. Whether such plasmons exist is mainly determined by the field strength, temperature, and momentum. The inelastic light scattering spectroscopies could be used to verify the magnetic field and temperature induced plasmons.

Graphene nanoribbons in criss-crossed electric and magnetic fields.

Graphene nanoribbons (GNRs) in mutually perpendicular electric and magnetic fields are shown to exhibit dramatic changes in their band structure and electron-transport properties. A strong electric field across the ribbon induces multiple chiral Dirac points, closing the semiconducting gap in armchair GNRs. A perpendicular magnetic field induces partially formed Landau levels as well as dispersive surface-bound states. Each of the applied fields on its own preserves the even symmetry E(k)=E(-k) of the sub-band dispersion. When applied together, they reverse the dispersion parity to be odd, which gives E(e,k)=-E(h,-k), and mix the electron and hole sub-bands within the energy range corresponding to the change in potential across the ribbon. This leads to oscillations of the ballistic conductance within this energy range. The broken time-reversal symmetry provides dichroism in the absorption of the circularly polarized light. As a consequence, one can observe electrically enhanced Faraday rotation, since the edges of the ribbon provide formation of the substantial density of states.

Two-photon-coincidence fluorescence spectra of cavity multipolaritons: novel signatures of multiexciton generation.

In a simulation study, we show that correlated two-dimensional frequency-resolved fluorescence spectra of a quantum dot in a microcavity provide a sensitive probe for the distribution of multiexcitons. Polariton couplings lead to a fine structure of Rabi multiplets that allow us to resolve otherwise overlapping features of the different multiexcitons. These may be used to probe multiexciton generation.

Manipulating stimulated coherent anti-Stokes Raman spectroscopy signals by broad-band and narrow-band pulses.

A transition-amplitude based representation of heterodyne detected coherent anti-Stokes Raman signals is used to separate them into a parametric component that involves no change in the material and dissipative processes associated with various transitions between states. Qualitatively different contributions from the two processes are predicted for the signal generated by an overlapping narrow (picosecond) and broad-band (femtosecond) pulse.

Photon entanglement signatures in difference-frequency-generation.

In response to quantum optical fields, pairs of molecules generate coherent nonlinear spectroscopy signals. Homodyne signals are given by sums over terms each being a product of Liouville space pathways of the pair of molecules times the corresponding optical field correlation function. For classical fields all field correlation functions may be factorized and become identical products of field amplitudes. The signal is then given by the absolute square of a susceptibility which in turn is a sum over pathways of a single molecule. The molecular pathways of different molecules in the pair are uncorrelated in this case (each path of a given molecule can be accompanied by any path of the other). However, entangled photons create an entanglement between the molecular pathways.We use the superoperator nonequlibrium Green's functions formalism to demonstrate the signatures of this pathway-entanglement in the difference frequency generation signal. Comparison is made with an analogous incoherent two-photon fluorescence signal.

Multidimensional pump-probe spectroscopy with entangled twin-photon states.

We show that entangled photons may be used in coherent multidimensional nonlinear spectroscopy to provide information on matter by scanning photon wave function parameters (entanglement time and delay of twin photons), rather than frequencies and time delays, as is commonly done with classical pulses. Signals are expressed and interpreted intuitively in terms of products of matter and field correlation functions using a diagrammatic close time path loop formalism which reveals the entangled quantum pathways of the fields and matter. The pump-probe signal measured when the pump and the probe are in a twin entangled state shows two-photon resonant contributions which scale linearly rather than quadratically with the incident beam intensity and reveal frequencies of off-resonant transitions. Two-dimensional spectrograms obtained by double Fourier transform of the signal with respect to the entanglement time and delay of the twins could provide detailed information on correlations among states and dynamical processes with high temporal resolution. The analogy with multidimensional time-domain optical techniques which use sequences of short classical pulses and pulse shaping algorithms is pointed out.

A unified description of sum frequency generation, parametric down conversion and two-photon fluorescence.

A superoperator non-equilibrium Green's function formalism is presented for computing nonlinear optical processes involving any combination of classical and quantum optical modes. Closed correlation-function expressions based on superoperator time-ordering are derived for the combined effects of causal response and non-causal spontaneous fluctuations. Coherent three wave mixing (sum frequency generation and parametric down conversion) involving one and two quantum optical modes, respectively, are compared with their incoherent counterparts: two-photon-induced fluorescence and two-photon-emitted fluorescence.

Nonlinear spectroscopy with entangled photons; manipulating quantum pathways of matter.

Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of incoming photons. Pathway-selectivity opens up new avenues for mapping photon into material entanglement. New material information, otherwise erased by interferences among pathways, is revealed.

Generalized Kramers-Heisenberg expressions for stimulated Raman scattering and two-photon absorption.

The frequency-domain pump-probe signal of a material system interacting with two quantum modes of the radiation field is recast in terms of products of scattering amplitudes (T matrix elements) rather than the third-order susceptibility Im chi((3)). The resulting expression offers a more intuitive physical picture for the optical process compared with the semiclassical approach which treats the radiation field as classical. It can be derived and interpreted using closed-time-path-loop diagrams which represent the joint state of the matter and the field for each contribution to the signal. The signal has two components representing stimulated Raman scattering omega(1) - omega(2) and two-photon absorption omega(1) + omega(2) two-photon resonances. Both are expressed as nonequi-librium steady-state photon and matter fluxes, as is common in the description of dissipative processes in open quantum systems.