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Mark I. Stockman

Publications and source records attributed to Mark I. Stockman.

At least 37 records · Page 2Linked to original sources

Ultrafast control of strong-field electron dynamics in solids

We review theoretical foundations and some recent progress related to the quest of controlling the motion of charge carriers with intense laser pulses and optical waveforms. The tools and techniques of attosecond science enable detailed investigations of a relatively unexplored regime of nondestructive strong-field effects. Such extremely nonlinear effects may be utilized to steer electron motion with precisely controlled optical fields and switch electric currents at a rate that is far beyond the capabilities of conventional electronics.

cond-mat.mes-hall↗

Spaser as Novel Versatile Biomedical Tool

Fluorescence imaging and spectroscopy remain the most powerful tools for visualization with chemical and immunological specificity of labeled biomolecules, viruses, cellular organelles, and living cells in complex biological backgrounds. However, a common drawback of fluorescence labels is that their brightness is limited by optical saturation and photobleaching. As an alternative, plasmonic metal nanoparticles are very promising as optical labels with no photobleaching and low optical saturation at realistic exciting intensities as was demonstrated in photoacoustic and photothermal sensing, imaging, and theranostics. However, plasmonic nanoparticles have wide absorption spectra and are not fluorescent, which limits their spectral selectivity and multimodal functionality, respectively. Here we demonstrate experimentally, both in vitro and in vivo, that spaser (surface plasmon amplification by stimulated emission of radiation) provides unprecedented efficiency as a versatile tool in biomedical research and applications. This is due to the unique combination of intense near-monochromatic stimulated emission and strongly enhanced absorption, free of optical saturation. Using soluble and biocompatible uranine dye as a gain medium surrounding the gold nanocore as a plasmonic resonator, we demonstrate unprecedented spaser stimulated emission intensity ("giant spasing") and a narrow spectral width (0.8 nm), which are more than ~380-fold and ~30-fold, respectively, better than in quantum dots as the best conventional fluorescent nanoprobes. At the same time, the plasmonic spaser nanocore served as excellent photoacoustic and photothermal contrast agents for imaging and nanobubble-based theranostics of cancer cells. This makes the spasers, arguably, the best multifunctional, super-contrast, low-toxicity optical probes in biomedical research, especially with single-pulse excitation.

cond-mat.mes-hall↗

Wannier-Stark states of graphene monolayer in strong electric field

We find theoretically energy spectrum of a graphene monolayer in a strong constant electric field using a tight-binding model. Within a single band, we find quantized equidistant energy levels (Wannier-Stark ladder), separated by the Bloch frequency. Singular interband coupling results in mixing of the states of different bands and anticrossing of corresponding levels, which is described analytically near Dirac points and is related to the Pancharatnam-Berry phase. The rate of interband tunneling, which is proportional to the anticrossing gaps in the spectrum, is only inversely proportional to the tunneling distance, in a sharp contrast to conventional solids where this dependence is exponential. This singularity will have major consequences for graphene behavior in strong ultrafast optical fields, in particular, leading to non-adiabaticity of electron excitation dynamics.

cond-mat.mes-hall↗

Strong-Field Perspective on High-Harmonic Radiation from Bulk Solids

Mechanisms of high-harmonic generation from crystals are described by treating the electric field of a laser as a quasi-static strong field. Under the quasi-static electric field, electrons in periodic potentials form dressed states, known as Wannier-Stark states. The energy differences between the dressed states determine the frequencies of the radiation. The radiation yield is determined by the magnitudes of the inter-band and intra-band current matrix elements between the dressed states. The generation of attosecond pulses from solids is predicted. Ramifications for strong-field physics are discussed.

physics.optics↗

Interaction of graphene monolayer with ultrashort laser pulse

We study the interaction of graphene with ultrashort few femtosecond long optical pulse. For such a short pulse, the electron dynamics is coherent and is described within the tight-binding model of graphene. The interaction of optical pulse with graphene is determined by strong wave vector dependence of the interband dipole matrix elements, which are singular at the Dirac points of graphene. The electron dynamics in optical pulse is highly irreversible with large residual population of the conduction band. The residual conduction band population as a function of the wave vector is nonuniform with a few localized spots of high conduction band population. The spots are located near the Dirac points and the number of spots depends on the pulse intensity. The optical pulse propagating through graphene layer generates finite transferred charge, which, as a function of pulse intensity, changes its sign. At small pulse intensity, the charge is transferred in the direction of the pulse maximum, while at large pulse intensity, the direction of the charge transfer is opposite to the direction of pulse maximum. This property opens unique possibility of controlling the direction of the charge transfer by variation of the pulse intensity.

cond-mat.mes-hall↗

Proposed Graphene Nanospaser

We show that graphene monolayer coupled to multi-quantum well system can form a graphene spaser, which is a coherent quantum generator of surface plasmons in graphene. The active element of graphene spaser is a multi-quantum well system with a design similar to the design of an active element of quantum cascade laser. Under realistic parameters of the multi-quantum well system, the spasing in graphene monolayer can be achieved at a finite doping of graphene and at a plasmon frequency, 0.15 eV, close to the typical frequency of intersubband transitions in multi-quantum well systems.

cond-mat.mes-hall↗

Electric Spaser in the Extreme Quantum Limit

We consider theoretically the spaser excited electrically via a nanowire with ballistic quantum conductance. We show that in the extreme quantum regime, i.e., for a single conductance-quantum nanowire, the spaser with the core made of common plasmonic metals, such as silver and gold, is fundamentally possible. For ballistic nanowires with multiple-quanta or non-quantized conductance, the performance of the spaser is enhanced in comparison with the extreme quantum limit. The electrically-pumped spaser is promising as an optical source, nanoamplifier, and digital logic device for optoelectronic information processing with speed ~100 GHz to ~100 THz.

cond-mat.mes-hall↗

Metal nanofilm in strong ultrafast optical fields

We predict that a metal nanofilm subjected to an ultrashort (single oscillation) optical pulse of a high field amplitude $\sim 3 \mathrm{V/Å}$ at normal incidence undergoes an ultrafast (at subcycle times $\lesssim 1 \mathrm{fs}$) transition to a state resembling semimetal. Its reflectivity is greatly reduced, while the transmissivity and the optical field inside the metal are greatly increased. The temporal profiles of the optical fields are predicted to exhibit pronounced subcycle oscillations, which are attributed to the Bloch oscillations and formation of the Wannier-Stark ladder of electronic states. The reflected, transmitted, and inside-the-metal pulses have non-zero areas approaching half-cycle pulses. The effects predicted are promising for applications to nanoplasmonic modulators and field-effect transistors with petahertz bandwidth.

cond-mat.mes-hall↗

Ultrafast Dynamic Metallization of Dielectric Nanofilms by Strong Single-Cycle Optical Fields

We predict a dynamic metallization effect where an ultrafast (single-cycle) optical pulse with a field less or on the order of 1 V/Angstrom causes plasmonic metal-like behavior of a dielectric film with a few-nm thickness. This manifests itself in plasmonic oscillations of polarization and a significant population of the conduction band evolving on a femtosecond time scale. These phenomena are due a combination of both adiabatic (reversible) and diabatic (for practical purposes irreversible) pathways.

cond-mat.mes-hall↗

Spaser Action, Loss Compensation, and Stability in Plasmonic Systems with Gain

We demonstrate that the conditions of spaser generation and the full loss compensation in a resonant plasmonic-gain medium (metamaterial) are identical. Consequently, attempting the full compensation or overcompensation of losses by gain will lead to instability and a transition to a spaser state. This will limit (clamp) the inversion and lead to the limitation on the maximum loss compensation achievable. The criterion of the loss overcompensation, leading to the instability and spasing, is given in a analytical and universal (independent from system's geometry) form.

cond-mat.mes-hall↗

Metallization of Nanofilms in Strong Adiabatic Electric Fields

We introduce an effect of metallization of dielectric nanofilms by strong, adiabatically varying electric fields. The metallization causes optical properties of a dielectric film to become similar to those of a plasmonic metal (strong absorption and negative permittivity at low optical frequencies). The is a quantum effect, which is exponentially size-dependent, occurring at fields on the order of 0.1 V/A and pulse durations ranging from ~ 1 fs to ~ 10 ns for film thickness 3 to 10 nm.

cond-mat.mes-hall↗

Supplemental Material for Paper "Metallization of Nanofilms in Strong Adiabatic Electric Fields"

We introduce an effect of metallization of dielectric nanofilms by strong, adiabatically varying electric fields. The metallization causes optical properties of a dielectric film to become similar to those of a plasmonic metal (strong absorption and negative permittivity at low optical frequencies). The is a quantum effect, which is exponentially size-dependent, occurring at fields on the order of 0.1 V/A and pulse durations ranging from ~ 1 fs to ~ 10 ns for film thickness 3 to 10 nm.

cond-mat.mes-hall↗

Spaser as Nanoscale Quantum Generator and Ultrafast Amplifier

Nanoplasmonics has recently experienced explosive development with many novel ideas and dramatic achievements in both fundamentals and applications. The spaser has been predicted and observed experimentally as an active element -- generator of coherent local fields. Even greater progress will be achieved if the spaser could function as a ultrafast nanoamplifier -- an optical counterpart of the MOSFET (metal-oxide-semiconductor field-effect transistor). A formidable problem with this is that the spaser has the inherent feedback causing quantum generation of nanolocalized surface plasmons and saturation and consequent elimination of the net gain, making it unsuitable for amplification. We have overcome this inherent problem and shown that the spaser can perform functions of an ultrafast nanoamplifier in two modes: transient and bistable. On the basis of quantum density matrix (optical Bloch) equations we have shown that the spaser amplifies with gain greater than 50, the switching time less or on the order of 100 fs (potentially, 10 fs). This prospective spaser technology will further broaden both fundamental and applied horizons of nanoscience, in particular, enabling ultrafast microprocessors working at 10 to 100 THz clock speed. Other prospective applications are in ultrasensing, ultradense and ultrafast information storage, and biomedicine. The spasers are based on metals and, in contrast to semiconductors, are highly resistive to ionizing radiation, high temperatures, microwave radiation, and other adverse environments.

cond-mat.mes-hall↗

Giant Surface Plasmon Induced Drag Effect (SPIDEr) in Metal Nanowires

Here, for the first time we predict a giant surface plasmon-induced drag effect (SPIDEr), which exists under conditions of the extreme nanoplasmonic confinement. Under realistic conditions, in nanowires, this giant SPIDEr generates rectified THz potential differences up to 10 V and extremely strong electric fields up to 10^5-10^6 V/cm. The SPIDEr is an ultrafast effect whose bandwidth for nanometric wires is 20 THz. The giant SPIDEr opens up a new field of ultraintense THz nanooptics with wide potential applications in nanotechnology and nanoscience, including microelectronics,nanoplasmonics, and biomedicine.

cond-mat.mes-hall↗

Nanoconcentration of Terahertz Radiation in Plasmonic Waveguides

Recent years have seen an explosive research and development of nanoplasmonics in the visible and near-infrared (near-ir) frequency regions. One of the most fundamental effects in nanoplasmonics is nano-concentration of optical energy. Plasmonic nanofocusing has been predicted and experimentally achieved. It will be very beneficial for the fundamental science, engineering, environmental, and defense applications to be able to nano-concentrate terahertz radiation (frequency 1 - 10 THz or vacuum wavelength 300 - 30 microns). This will allow for the nanoscale spatial resolution for THz imaging and introduce the THz spectroscopy on the nanoscale, taking full advantage of the rich THz spectra and submicron to nanoscale structures of many engineering, physical, and biological objects of wide interest: electronic components (integrated circuits, etc.), bacteria, their spores, viruses, macromolecules, carbon clusters and nanotubes, etc. In this Letter we establish the principal limits for the nanoconcentration of the THz radiation in metal/dielectric waveguides and determine their optimum shapes required for this nanoconcentration We predict that the adiabatic compression of THz radiation from the initial spot size of light wavelength to the final size of R = 100 - 250 nm can be achieved with the THz radiation intensity increased by a factor of 10 to 250. This THz energy nanoconcentration will not only improve the spatial resolution and increase the signal/noise ratio for the THz imaging and spectroscopy, but in combination with the recently developed sources of powerful THz pulses will allow the observation of nonlinear THz effects and a carrying out a variety of nonlinear spectroscopies (such as two-dimensional spectroscopy), which are highly informative.

physics.optics↗

Nanoplasmonic Renormalization and Enhancement of Coulomb Interactions

Nanostructured plasmonic metal systems are known to enhance greatly variety of radiative and nonradiative optical processes, both linear and nonlinear, which are due to the interaction of an electron in a molecule or semiconductor with the enhanced local optical field of the surface plasmons. Principally different are numerous many-body phenomena that are due to the Coulomb interaction between charged particles: carriers (electrons and holes) and ions. These include carrier-carrier or carrier-ion scattering, energy and momentum transfer (including the drag effect), thermal equilibration, exciton formation, impact ionization, Auger effects, etc. It is not widely recognized that these and other many-body effects can also be modified and enhanced by the surface-plasmon local fields. A special but extremely important class of such many-body phenomena is constituted by chemical reactions at metal surfaces, including catalytic reactions. Here, we propose a general and powerful theory of the plasmonic enhancement of the many-body phenomena resulting in a closed expression for the surface plasmon-dressed Coulomb interaction. We illustrate this theory by computing this dressed interaction explicitly for an important example of metal-dielectric nanoshells, which exhibits a reach resonant behavior in both the magnitude and phase. This interaction is used to describe the nanoplasmonic-enhanced Foerster energy transfer between nanocrystal quantum dots in the proximity of a plasmonic nanoshell. Catalysis at nanostructured metal surfaces, nonlocal carrier scattering and surface-enhanced Raman scattering are discussed among other effects and applications where the nanoplasmonic renormalization of the Coulomb interaction may be of principal importance.

physics.optics↗

Toward Full Spatio-Temporal Control on the Nanoscale

We introduce an approach to implement full coherent control on nanometer length scales. It is based on spatio-temporal modulation of the surface plasmon polariton (SPP) fields at the thick edge of a nanowedge. The SPP wavepackets propagating toward the sharp edge of this nanowedge are compressed and adiabatically concentrated at a nanofocus, forming an ultrashort pulse of local fields. The one-dimensional spatial profile and temporal waveform of this pulse are completely coherently controlled.

physics.optics↗

Time-Reversal Coherent Control in Nanoplasmonics

We introduce an approach to determining the required waveforms to coherently control the optical energy localization in plasmonic nanosystems. This approach is based on the impulsive localized excitation of the nanosystem and time reversal of the generated far-zone field at a single point with one polarization. Despite strong interaction and significant dephasing and dissipation in metal plasmonic systems, and incompleteness of this time reversal, the proposed approach proves to be very efficient in controlling the nanoscale optical fields. Possible applications include nanoscale spectroscopy and photomodification, ultradense memory, and information processing on the nanoscale.

cond-mat.dis-nn↗