Ronald Ulbricht

Ultrafast active control of localized surface plasmon resonances in silicon bowtie antennas.

Localized surface plasmon polaritons (LSPPs) provide an efficient means of achieving extreme light concentration. In recent years, their active control has become a major aspiration of plasmonic research. Here, we demonstrate direct control of semiconductor bowtie antennas, enabling active excitation of LSPPs, at terahertz (THz) frequencies. We modify the LSPPs by ultrafast optical modulation of the free carrier density in the plasmonic structure itself, allowing for active control of the semiconductor antennas on picosecond timescales. Moreover, this control enables the manipulation of the field intensity enhancements in ranges of four orders of magnitude.

Detection of deep-subwavelength dielectric layers at terahertz frequencies using semiconductor plasmonic resonators

Plasmonic bowtie antennas made of doped silicon can operate as plasmonic resonators at terahertz (THz) frequencies and provide large field enhancement close to their gap. We demonstrate both experimentally and theoretically that the field confinement close to the surface of the antenna enables the detection of ultrathin (100 nm) inorganic films, about 3750 times thinner than the free space wavelength. Based on model calculations, we conclude that the detection sensitivity and its variation with the thickness of the deposited layer are related to both the decay of the local THz field profile around the antenna and the local field enhancement in the gap of the bowtie antenna. This large field enhancement has the potential to improve the detection limits of plasmon-based biological and chemical sensors.

Assessing Charge Carrier Trapping in Silicon Nanowires Using Picosecond Conductivity Measurements

Free-standing semiconductor nanowires on bulk substrates are increasingly being explored as building blocks for novel optoelectronic devices such as tandem solar cells. Although carrier transport properties, such as mobility and trap densities, are essential for such applications, it has remained challenging to quantify these properties. Here, we report on a method that permits the direct, contact-free quantification of nanowire carrier diffusivity and trap densities in thin (∼25 nm wide) silicon nanowires-without any additional processing steps such as transfer of wires onto a substrate. The approach relies on the very different terahertz (THz) conductivity response of photoinjected carriers within the silicon nanowires from those in the silicon substrate. This allows quantifying both the picosecond dynamics and the efficiency of charge carrier transport from the silicon nanowires into the silicon substrate. Varying the excitation density allows for quantification of nanowire trap densities: for sufficiently low excitation fluences the diffusion process stalls because the majority of charge carriers become trapped at nanowire surface defects. Using a model that includes these effects, we determine both the diffusion constant and the nanowire trap density. The trap density is found to be orders of magnitude larger than the charge carrier density that would be generated by AM1.5 sunlight.

Loosening Quantum Confinement: Observation of Real Conductivity Caused by Hole Polarons in Semiconductor Nanocrystals Smaller than the Bohr Radius

We report on the gradual evolution of the conductivity of spherical CdTe nanocrystals of increasing size from the regime of strong quantum confinement with truly discrete energy levels to the regime of weak confinement with closely spaced hole states. We use the high-frequency (terahertz) real and imaginary conductivities of optically injected carriers in the nanocrystals to report on the degree of quantum confinement. For the smaller CdTe nanocrystals (3 nm < radius < 5 nm), the complex terahertz conductivity is purely imaginary. For nanocrystals with radii exceeding 5 nm, we observe the onset of real conductivity, which is attributed to the increasingly smaller separation between the hole states. Remarkably, this onset occurs for a nanocrystal radius significantly smaller than the bulk exciton Bohr radius a(B) ∼ 7 nm and cannot be explained by purely electronic transitions between hole states, as evidenced by tight-binding calculations. The real-valued conductivity observed in the larger nanocrystals can be explained by the emergence of mixed carrier-phonon, that is, polaron, states due to hole transitions that become resonant with, and couple strongly to, optical phonon modes for larger QDs. These polaron states possess larger oscillator strengths and broader absorption, and thereby give rise to enhanced real conductivity within the nanocrystals despite the confinement.

Elucidating gigahertz acoustic modulation of extraordinary optical transmission through a two-dimensional array of nano-holes

The ultrafast modulation of light transmitted by a metamaterial making up an extraordinary optical transmission geometry is investigated by means of optical pump-probe spectroscopy. Using a sample consisting of a lattice of square nano-holes in a gold film on a glass substrate, we monitor the high-frequency oscillations in the intensity of transmitted infrared light. A variety of gigahertz acoustic modes, involving the opening and shutting motion of the holes as well as the straining of the glass substrate below the holes, are revealed to be active in the optical modulation. Numerical simulations of the transient deformations and strain fields elucidate the nature of the vibrational modes contributing most strongly to the variations in optical transmission, and point to the hole-area modulation as the dominant effect. Potential applications include ultrafast acousto-optic modulators.

Gigahertz Optomechanical Modulation by Split-Ring-Resonator Nanophotonic Meta-Atom Arrays

Using polarization-resolved transient reflection spectroscopy, we investigate a metasurface consisting of coherently vibrating nanophotonic U-shaped split-ring meta-atoms that exhibit colocalized optical and mechanical resonances. With an array of these resonators formed of gold on glass, essentially miniature tuning forks, we monitor the visible-pump induced gigahertz oscillations in reflected infrared light intensity to probe the multimodal vibrational response. Numerical simulations of the associated transient deformations and strain fields elucidate the complex nanomechanical dynamics contributing to the ultrafast optical modulation and point to the role of acousto-plasmonic interactions through the opening and closing motion of the SRR gaps as the dominant effect. Applications include ultrafast acoustooptic modulator design and sensing.

THz plasmonic antennas: From metals to semiconductors

Plasmonic antennas at THz frequencies are promising candidates to enhance the sensitivity of THz detectors. The resonances of metallic and semiconductor antennas are compared. Experiments show the powerful advantage of semiconductors as a means for active control over the localized surface plasmons.

CHAPTER 11:Carrier Dynamics in Photovoltaic Structures and Materials Studied by Time-Resolved Terahertz Spectroscopy

Terahertz (THz) radiation, covering the frequency range from a few to about a hundred milli-electron volts (meV), is particularly sensitive to the response of charge motion in materials. Using a pump-probe scheme, time resolved terahertz spectroscopy (TRTS) allows, in a contact-free way, the study of charge carrier dynamics with ultrafast time resolution. In this chapter, we review how TRTS has been successfully employed for the characterization of photovoltaic materials and architectures. Particularly, we focus on TRTS studies that interrogate key processes occurring after photo-excitation in nano-structured semiconductor systems, including charge generation, separation and transport. Understanding the fundamental properties of charge carriers in these novel geometries is important for the development of future solar energy conversion technologies.