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Vartkess A. Apkarian

Publications and source records attributed to Vartkess A. Apkarian.

2 recordsLinked to original sources

Photon momentum enabled light absorption in bulk silicon

Photons do not carry sufficient momentum to induce indirect optical transitions in semiconducting materials such as silicon, necessitating the assistance of lattice phonons to conserve momentum. Compared to direct bandgap semiconductors, this renders silicon a less attractive material for a wide variety of optoelectronic applications. In this work, we introduce an alternative strategy to fulfill the momentum-matching requirement in indirect optical transitions. We demonstrate that when confined to scales below ~3 nm, photons acquire sufficient momentum to allow electronic transitions at the band edge of Si without the assistance of a phonon. Confined photons allow simultaneous energy and momentum conservation in two-body photon-electron scattering; in effect, converting silicon into a direct bandgap semiconductor. We show that this less-explored concept of light-matter interaction leads to a marked increase in the absorptivity of Si from the UV to the near-IR. The strategy provides opportunities for more efficient use of indirect semiconductors in photovoltaics, energy conversion, light detection and emission.

physics.optics↗

Seeing the vibrational breathing of a single molecule through time-resolved coherent anti-Stokes Raman scattering

The motion of chemical bonds within molecules can be observed in real time, in the form of vibrational wavepackets prepared and interrogated through ultrafast nonlinear spectroscopy. Such nonlinear optical measurements are commonly performed on large ensembles of molecules, and as such, are limited to the extent that ensemble coherence can be maintained. Here, we describe vibrational wavepacket motion on single molecules, recorded through time-resolved, surface-enhanced, coherent anti-Stokes Raman scattering. The required sensitivity to detect the motion of a single molecule, under ambient conditions, is achieved by equipping the molecule with a dipolar nano-antenna (a gold dumbbell). In contrast with measurements in ensembles, the vibrational coherence on a single molecule does not dephase. It develops phase fluctuations with characteristic statistics. We present the time evolution of discretely sampled statistical states, and highlight the unique information content in the characteristic, early-time probability distribution function of the signal.

physics.chem-ph↗