Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 153, Issue 4, Pages -Publisher
AMER INST PHYSICS
DOI: 10.1063/5.0013190
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Funding
- National Science Foundation [CHE-1553939]
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Ultrafast control of electron dynamics is essential for future innovations in nanoelectronics, catalysis, and molecular imaging. Recently, we developed a general scheme (Stark Control of Electrons at Interfaces or SCELI) to control electron dynamics at interfaces [A. J. Garzon-Ramirez and I. Franco, Phys. Rev. B 98, 121305 (2018)] that is based on using few-cycle lasers to open quantum tunneling channels for interfacial electron transfer. SCELI uses the Stark effect induced by non-resonant light to create transient resonances between a donor level in material B and an acceptor level in material A, resulting in B -> A electron transfer. Here, we show how SCELI can be employed to generate net charge transport in ABA heterojunctions without applying a bias voltage, a phenomenon known as laser-induced symmetry breaking. The magnitude and sign of such transport can be controlled by simply varying the time asymmetry of the laser pulse through manipulation of laser phases. In particular, we contrast symmetry breaking effects introduced by manipulation of the carrier envelope phase with those introduced by relative phase control in omega + 2 omega laser pulses. The omega + 2 omega pulse is seen to be far superior as such pulses exhibit a larger difference in field intensity for positive and negative amplitudes. The results exemplify the power of Stark-based strategies for controlling electrons using lasers.
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