Graphene nanostructures (GNs) including graphene nanoribbons and nanoflakes have attracted tremendous interest in the field of chemistry and materials science due to their fascinating electronic, optical and magnetic properties. Among them, zigzag-edged GNs (ZGNs) with precisely-tunable π-magnetism hold great potential for applications in spintronics and quantum devices. To improve the stability and processability of ZGNs, substitutional groups are often introduced to protect the reactive edges in organic synthesis, which renders the study of their intrinsic properties difficult. In contrast to the conventional wet-chemistry method, on-surface bottom-up synthesis presents a promising approach for the fabrication of both unsubstituted ZGNs and functionalized ZGNs with atomic precision via surface-catalyzed transformation of rationally-designed precursors. The structural and spin-polarized electronic properties of these ZGNs can then be characterized with sub-molecular resolution by means of scanning probe microscopy techniques. This review aims to highlight recent advances in the on-surface synthesis and characterization of a diversity of ZGNs with π-magnetism. We also discuss the important role of precursor design and reaction stimuli in the on-surface synthesis of ZGNs and their π-magnetism origin. Finally, we will highlight the existing challenges and future perspective surrounding the synthesis of novel open-shell ZGNs towards next-generation quantum technology.

The emergence of cylindrical vector beam (CVB) multiplexing has opened new avenues for high-capacity optical communication. Although several configurations have been developed to couple/separate CVBs, the CVB multiplexer/demultiplexer remains elusive due to lack of effective off-axis polarization control technologies. Here we report a straightforward approach to realize off-axis polarization control for CVB multiplexing/demultiplexing based on a metal–dielectric–metal metasurface. We show that the left- and right-handed circularly polarized (LHCP/RHCP) components of CVBs are independently modulated via spin-to-orbit interactions by the properly designed metasurface, and then simultaneously multiplexed and demultiplexed due to the reversibility of light path and the conservation of vector mode. We also show that the proposed multiplexers/demultiplexers are broadband (from 1310 to 1625 nm) and compatible with wavelength-division-multiplexing. As a proof of concept, we successfully demonstrate a four-channel CVB multiplexing communication, combining wavelength-division-multiplexing and polarization-division-multiplexing with a transmission rate of 1.56 Tbit/s and a bit-error-rate of 10⁻⁶ at the receive power of −21.6 dBm. This study paves the way for CVB multiplexing/demultiplexing and may benefit high-capacity CVB communication.

Optical logical operations demonstrate the key role of optical digital computing, which can perform general-purpose calculations and possess fast processing speed, low crosstalk, and high throughput. The logic states usually refer to linear momentums that are distinguished by intensity distributions, which blur the discrimination boundary and limit its sustainable applications. Here, we introduce orbital angular momentum (OAM) mode logical operations performed by optical diffractive neural networks (ODNNs). Using the OAM mode as a logic state not only can improve the parallel processing ability but also enhance the logic distinction and robustness of logical gates owing to the mode infinity and orthogonality. ODNN combining scalar diffraction theory and deep learning technology is designed to independently manipulate the mode and spatial position of multiple OAM modes, which allows for complex multilight modulation functions to respond to logic inputs. We show that few-layer ODNNs successfully implement the logical operations of AND, OR, NOT, NAND, and NOR in simulations. The logic units of XNOR and XOR are obtained by cascading the basic logical gates of AND, OR, and NOT, which can further constitute logical half-adder gates. Our demonstrations may provide a new avenue for optical logical operations and are expected to promote the practical application of optical digital computing.

Orbital angular momentum (OAM) mode multiplexing provides a new strategy for reconstructing multiple holograms, which is compatible with other physical dimensions involving wavelength and polarization to enlarge information capacity. Conventional OAM multiplexing holography usually relies on the independence of physical dimensions, and the deep holography involving spatial depth is always limited for the lack of spatiotemporal evolution modulation technologies. Herein, we introduce a depth-controllable imaging technology in OAM deep multiplexing holography via designing a prototype of five-layer optical diffractive neural network (ODNN). Since the optical propagation with dimensional-independent spatiotemporal evolution offers a unique linear modulation to light, it is possible to combine OAM modes with spatial depths to realize OAM deep multiplexing holography. Exploiting the multi-plane light conversion and in-situ optical propagation principles, we simultaneously modulate both the OAM mode and spatial depth of incident light via unitary transformation and linear modulations, where OAM modes are encoded independently for conversions among holograms. Results show that the ODNN realized light field conversion and evolution of five multiplexed OAM modes in deep multiplexing holography, where the mean square error and structural similarity index measure are 0.03 and 86%, respectively. Our demonstration explores a depth-controllable spatiotemporal evolution technology in OAM deep multiplexing holography, which is expected to promote the development of OAM mode-based optical holography and storage.