Twisted Nonlinear Optics in Monolayer van der Waals Crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust...

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Published in:	ACS nano Vol. 19; no. 34; pp. 30919 - 30929
Main Authors:	Norden, Tenzin, Martinez, Luis M., Tarefder, Nehan, Kwock, Kevin W. C., McClintock, Luke M., Olsen, Nicholas, Holtzman, Luke N., Yeo, June Ho, Zhao, Liuyan, Zhu, Xiaoyang, Hone, James C., Yoo, Jinkyoung, Zhu, Jian-Xin, Schuck, P. James, Taylor, Antoinette J., Prasankumar, Rohit P., Kort-Kamp, Wilton J. M., Padmanabhan, Prashant
Format:	Journal Article
Language:	English
Published:	United States American Chemical Society 02.09.2025 American Chemical Society (ACS)
Subjects:	nonlinear optics two-dimensional semiconductors vortex beams difference frequency generation sum frequency generation orbital angular momentum four-wave mixing
ISSN:	1936-0851, 1936-086X, 1936-086X
Online Access:	Get full text
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Summary:	In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications in optical communications and quantum information science. Multibeam nonlinear optical processes, augmented by optical vortices, are essential in this context, providing robust access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting multipulse difference frequency, sum frequency, and four-wave mixing in monolayer quantum materials, we demonstrate their ability to independently control the orbital angular momentum and radial distribution of vortex light-fields in addition to their wavelength. Due to the atomically thin nature of the host crystal, this control spans a broad spectral bandwidth in a highly integrable platform that is unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds an innovative path for ultracompact and scalable hybrid nanophotonic technologies empowered by twisted nonlinear light–matter interactions in van der Waals nanomaterials.
Bibliography:	ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 National Nuclear Security Administration Gordon and Betty Moore Foundation Department of Energy National Nuclear Security Administration Laboratory Residency Graduate Fellowship Center for Integrated Nanotechnologies Alfred P. Sloan Foundation NA0003960 Division of Materials Research Los Alamos National Laboratory
ISSN:	1936-0851 1936-086X 1936-086X
DOI:	10.1021/acsnano.5c06908