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1 Nonlinear Vectorial Metasurface for Optical Encryption Yutao Tang, 1,2 Yuttana Intaravanne 3 , Junhong Deng, 1,2 King Fai Li, 1,2 Xianzhong Chen, 3,* and Guixin Li 1,2,† 1 Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055 China. 2 Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055 China. 3 SUPA, Institute of Photonics and Quantum Sciences, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, EH14 4AS, UK. * [email protected] [email protected] The unprecedented capability of metasurface in manipulation of light propagation has been extended to the nonlinear optical regime, enabling a plethora of applications for nonlinear optical security and encryption. One of the key issues in this area is how to arbitrarily control the vectorial polarization profile of nonlinear waves. Here we propose and experimentally demonstrate a nonlinear photonic metasurface that can generate a vectorial polarization profile for nonlinear imaging. The high-resolution grayscale image can be read out through a second harmonic generation (SHG) beam from an ultrathin nonlinear metasurface. The polarization of SHG waves can be locally manipulated by simply changing the orientation angle of the plasmonic meta-atoms. The grayscale image is revealed using a linear polarizer based on the Malus’s law. We believe that the rich polarization information based on nonlinear metasurfaces has significant potential for the applications in nonlinear optical image encryption, security, anti-counterfeiting, and so on.

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Page 1: Nonlinear Vectorial Metasurface for Optical Encryption · FIG. 1. Nonlinear vectorial metasurface for optical encryption. (a) Schematic illustration of a nonlinear optical process

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Nonlinear Vectorial Metasurface for Optical Encryption

Yutao Tang,1,2 Yuttana Intaravanne3, Junhong Deng,1,2 King Fai Li,1,2 Xianzhong Chen,3,* and Guixin Li1,2,†

1Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055 China.

2Shenzhen Institute for Quantum Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055 China.

3SUPA, Institute of Photonics and Quantum Sciences, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, EH14 4AS, UK.

*[email protected]

[email protected]

The unprecedented capability of metasurface in manipulation of light propagation has

been extended to the nonlinear optical regime, enabling a plethora of applications for

nonlinear optical security and encryption. One of the key issues in this area is how to

arbitrarily control the vectorial polarization profile of nonlinear waves. Here we

propose and experimentally demonstrate a nonlinear photonic metasurface that can

generate a vectorial polarization profile for nonlinear imaging. The high-resolution

grayscale image can be read out through a second harmonic generation (SHG) beam

from an ultrathin nonlinear metasurface. The polarization of SHG waves can be locally

manipulated by simply changing the orientation angle of the plasmonic meta-atoms.

The grayscale image is revealed using a linear polarizer based on the Malus’s law. We

believe that the rich polarization information based on nonlinear metasurfaces has

significant potential for the applications in nonlinear optical image encryption, security,

anti-counterfeiting, and so on.

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I. INTRODUCTION

Light, with its abundant degrees of freedom, has become the cornerstone of the

drastic development of information processing, optical communications, etc. The

degrees of freedom of light field that could be modulated include the amplitude, the

phase, the state of polarization and the orbital angular momentum (OAM), etc.

Recently, it was demonstrated that photonic metasurfaces, consisting of spatially

variant meta-atoms, provide unprecedented capability to tailor the various degrees of

freedom of light. To some extent, the metasurface based devices are more compact and

have more integrated functionalities than many conventional optical components [1,2].

Applications of metasurfaces such as planar lenses [3-5], retroreflector [6], metasurface

hologram [7-13], optical diffuser [14], polarimetry [15], augmented reality [16] and so

on have been successfully demonstrated. Among the family of working mechanisms,

phase control represents a powerful tool to manipulate the properties of light fields. In

the linear optical regime, both the propagation phase and the geometric Pancharatnam-

Berry phase (P-B phase) have been widely used for polarization encoded optical

holography [13] and generation of vectorial light beam via arbitrary spin-to-orbital

angular momentum conversion [17,18]. While the above phase control methods are

based on the elaborate engineering of the size and orientation of the meta-atoms, an

alternative way to manipulate the polarization of light can be achieved by controlling

both the displacements and orientations of two orthogonal identical meta-atoms [11].

Such diatomic metasurface can be utilized to implement vectorial optical

holography [11]. In addition to the applications in optical holography, phase control

metasurface can be also used for high-resolution grayscale and multicolor

imaging [19,20].

Recently, the study of light-matter interaction on nonlinear optical metasurfaces

has attracted extensive interests [21-28]. Nonlinear optical processes such as

second [29-34], third [35-37] and high [38] harmonic generation, broadband optical

frequency mixer [39] have been extensively investigated by using both plasmonic and

dielectric metasurfaces. It is reported that the nonlinear optical susceptibility of the

meta-atoms strongly depends on the orders of the nonlinear process, the spin states of

fundamental wave (FW) and the local symmetry of the meta-atom [40]. Ascribed to the

effect of the nonlinear P-B phase, the method to continuously and locally tailor the

phase of nonlinear optical susceptibility was established recently [41], facilitating

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applications such as nonlinear holography [42,43], nonlinear spin-orbital interaction of

light [44], nonlinear metalens [45] and nonlinear image encryption [46] and so on.

Among all the above topics, the high-resolution nonlinear metasurface imaging has

great potential for information encoding and encryption. Previous effort has been

dedicated to the modulation of the intensity of nonlinear signal in real space by utilizing

the interference of SHG from two neighboring meta-atoms [46], however, the image

resolution is limited by the diatomic meta-molecule. Here we demonstrate a nonlinear

optical metasurface to locally manipulate the polarization states of the SHG wave and

encode a high-resolution image in the polarization profile accordingly [Fig. 1(a)]. Such

nonlinear image information could be revealed after filtering out the FW and converting

the vectorial polarization profile into intensity profile according to the Malus’s law. The

difference between the linear geometric metasurface and nonlinear geometric

metasurface provides a possible route to realize different polarization profiles for the

fundamental wave and the SHG wave, which can further improve the level of security

and encryption.

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FIG. 1. Nonlinear vectorial metasurface for optical encryption. (a) Schematic illustration of a nonlinear optical process to generate a polarization profile of the second harmonic generation (SHG) wave, by using a nonlinear photonic metasurface. A linear polarizer acts as an analyzer to convert the polarization profile into a grayscale image. (b) Metasurface unit cells with nonlinear gold meta-atoms. The unit cell is 500 nm × 500 nm and the length (L) and width (w) of each rectangular petal. The orientation parameter θ is varied to locally manipulate the polarization states of the SHG wave. (c) The generated SHG intensity is a squared cosine function of θ when the transmission axes of polarizer and analyzer are aligned horizontally. (d) The SHG intensities of θ = 0° and 30° meta-atoms behind a rotated analyzer, where α is the angle between the transmission axes of the analyzer and the horizontally aligned polarizer.

II. DESIGN PRINCIPLE OF THE NONLINEAR ENCRYPTION

METASURFACES

To encrypt image information into nonlinear optical devices, we utilize the

nonlinear plasmonic meta-atoms with three-fold rotational (C3) symmetry to construct

the nonlinear metasurface [Fig. 1(b)]. For a meta-atom with m-fold rotational

symmetry, when illuminated along its rotational axis by circularly polarized

fundamental waves, the allowed orders of the nonlinear harmonic generation are

restricted by the selection rule as 1n lm= ± . where l is an integer and the ‘+’ and ‘−’

signs indicate that the harmonic waves and the FWs possess the same and opposite spin

states [40,41]. Therefore, the C3 meta-atom can selectively produce SHG with opposite

handedness to that of the incident circularly polarized FW. More significantly, the

nonlinear polarizability of the meta-atoms can be continuously manipulated by varying

their orientations [Fig. 1(b), right panel]. As a result, a nonlinear geometric phase −3σθ

is simultaneously imparted to the SHG wave, where is the handedness of the

incident FW and θ is the angle by which the C3 meta-atom is rotated with respect to

the laboratory frame [40]. By using this characteristic we can encrypt an image

information into a polarization profile of the SHG waves.

Consider a horizontally polarized FW, its polarization state can be represented by

components as , where

and denote the components of the FW with left- and right-

circular polarizations, respectively, and ω is the angular frequency of the FW. After

passing through a nonlinear meta-atom, the polarization state of the SHG wave is given

by , the subscript 2ω

1σ = ±

FW LCP / 2 RCP / 2ω ω ω

= + TLCP [1 i] / 2ω

=

TRCP [1 i] / 2ω

= −

2 2 2SHG LCP exp(3i ) / 2 RCP exp( 3i ) / 2

ω ω ωθ θ= + −

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denotes the double frequency of the SHG wave, in other words, a phase difference

equals to 6θ is introduced between the two opposite spin components of the SHG wave,

corresponding to a 6θ rotation of the polarization vector in the equator of the Poincaré

sphere. Due to the two-to-one homomorphism between the physical SU(2) space of the

light beam and the topological SO(3) space of Poincaré sphere [47], such an equatorial

rotation corresponds to a 3θ rotation of the orientation angle of the linearly polarized

light. A linearly polarized FW along the horizontal direction can produce a transmitted

SHG wave with its polarization angle manipulated locally by the in-plane rotation of

nonlinear meta-atoms θ(x,y), and therefore encrypt a polarization profile.

To reveal the hidden information, we can filter out the FW by using a color filter

and then use a polarization analyzer to convert the polarization profile into an intensity

profile. According to the Malus’s law, when a polarized light beam passes through a

polarizer, the transmitted light intensity is , where α is the angle

between the polarization direction of light and the transmission axis of the polarizer.

The polarization direction of the SHG wave is rotated 3θ with respect to the horizontal

direction, and the insertion of a polarizer with horizontally aligned transmission axis

will lead to the intensity modulation, which is , as shown in

[Fig. 1(c)]. Therefore, the spatial intensity modulation I(x,y) after the linear analyzer

can reveal the distribution of the orientations of the meta-atoms θ(x,y), hence the

encoded image.

III. RESULTS AND DISCUSSION

Here we fabricate two nonlinear metasurfaces for polarization manipulation by

using standard electron beam lithography followed by a lift-off process (see

Supplemental Material [48] for details). The C3 gold meta-atoms sit on an indium tin

oxide (ITO) glass, with ITO thickness of ~20 nm. The width and the length of each arm

of the C3 meta-atom are 80 nm and 180 nm, respectively [Fig. 1(b)]. Each pixel is a

500 × 500 nm square cell with the C3 meta-atom at center. Two images comprising 201

× 201 pixels are eventually embedded into two small metasurfaces of 100 × 100μm

squares. One image is a grayscale bar which consisting 101 grayscale levels with a

linear intensity increase from the darkest to the brightest, while the other is an image of

a grayscale flower. The SEM and optical images of the fabricated metasurfaces are

shown in Figs. 2(a)-2(d).

2) (0)cos(I Iα α=

20) 3( cosI Iθ θ=

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We first measured the linear transmittances of the fabricated samples, as are shown

in Fig. 2(e). The transmittances are measured as the transmission axes of the polarizer

and the analyzer are parallel to each other, both horizontally aligned. The transmission

spectra of the two distinct samples are virtually identical to each other, proved that the

meta-atoms are isotropic when working in the linear mode. We also measured the

transmittance when the analyzer was perpendicular to the polarizer. The near to zero

transmittance clearly shows there is no polarization conversion for the incident light

(see Fig. S2 in Supplemental Material [48]). When working in the nonlinear mode, as

expected from the theoretical analysis, the metasurfaces exhibit strong dependencies on

the spin of the FW signal. As shown in Figs. 2(f)-2(g), under the illumination of a

circularly polarized (LCP or RCP) FW, the measured intensity of SHG wave with

opposite handedness are much larger than the same one. The measured SHG responses

of the grayscale bar sample also show maximum efficiency at fundamental wavelength

of 1225 nm, where we also measured the power dependence of the SHG signal, which

is presented in Fig. 2(h). The fitted slopes for both conversions of cross polarization

combination (LCP-RCP and RCP-LCP) are close to 2.0, which is the characteristic of

the nonlinear SHG process.

FIG. 2. Vectorial metasurfaces and the measured optical properties. Scanning electron microscopy (SEM) images of the metasurfaces for encoding (a) a grayscale bar and (b) an image of a flower. (c) and (d) are corresponding optical microscope images of the bar and flower metasurfaces. (e) Measured linear transmission spectra of the two samples in the near infrared regime. The transmission axes of the polarizer and the analyzer are parallel to each other, both horizontally aligned. (f) Measured nonlinear SHG intensity of the grayscale bar sample as the fundamental wavelength varies. Four spin polarization combinations are recorded to reveal the cross-polarization conversion property of the metasurface. The maximum SHG intensity is observed at 1225 nm. (g)

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Nonlinear response of the metasurface for the encoded flower. Strongest SHG response is found at 1250 nm. (h) Power dependencies of the SHG intensity of the flower metasurface.

To reveal the image hiding in the SHG signal of the nonlinear metasurface, we use

a pair of linear polarizers as polarizer and analyzer to retrieve the image encoded in the

SHG waves, in addition to a color filter to filter out the FW. The experimental setup is

shown in Fig. 3(a). We observe the SHG polarization profile at the pumping wavelength

of 1225 nm, under the pumping power of 15 mW. Fig. 3(b) shows the measured images

collected with varied orientations of the transmission axis of the analyzer while fixing

the polarizer with horizontally aligned transmission axis. The figure also includes the

simulated results of the corresponding scenarios (see simulation method in

Supplemental Material [48]). While the simulation results assume homogeneous

illumination of the fundamental wave, the laser beam illuminated at the metasurface in

experiments possesses a Gaussian intensity profile. As a result, the intensity variations

are most obvious at the center of each measured images when the analyzer is rotated,

while in the marginal parts of the images (especially in the four corners), only slight

variations are observed. In all measured images, we can consistently observe a range of

brightness from the brightest to the darkest, and the positions of the brightest and the

darkest lines are changing as expected in the simulated results. Such a position shift is

most pronounced when the transmission axes of the polarizer and the analyzer are

changed from mutually parallel to orthogonal configurations [α= 0° and 90° in

Fig. 3(b), respectively], as the brightest line in the center changes to the darkest line,

although the FW is the strongest at center. Therefore, our observation successfully

proved the encoding capability of the nonlinear metasurface, indicating that the

predesigned local orientation profile of the nonlinear meta-atoms can effectively impart

a polarization profile into the SHG wave.

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FIG. 3. Schematic of experimental setup and nonlinear optical results of the grayscale bar metasurface. a) Optical setup. P: linear polarizer; L: lens; Obj: objective lens; CF: color filter (short pass filter); CCD: camera. b) Simulated and experimental results for the SHG intensity profiles of the grayscale bar metasurface. Pumping wavelength is at 1225 nm. The analyzer is rotated counterclockwise while the transmission axis of the polarizer is fixed along the horizontal direction. α is the angle between the transmission axes of the polarizer and the analyzer.

To demonstrate the polarization encoding capability of the nonlinear metasurface

more vividly, we designed the second metasurface and encoded an image of a flower

into it. We also measured the revealed intensity profile converted from the vectorial

polarization profile of the SHG wave. The experimental setup is the same as the one

used to measure the grayscale bar sample, but the pumping wavelength is set as 1250

nm for the maximum nonlinear response [as indicated in Fig. 2(e)]. The simulated and

measured results are presented in Fig. 4, where varied analyzer orientations are set to

reflect the polarization profile of the SHG beam. The image revealed by transmission

axes parallel aligned setup (α= 0°) shows clearly view of a flower, with exact

configuration of five petals as the design target, and fine grayscale change from the

flower petal centers to the corners. Although the small water droplet on one of the

flower petals can’t be clearly distinguished from the measured image, the overall

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display quality of the image is quite impressive. The slight difference should be

attributed to the fabrication imperfection. On the other side, the measured images under

different configurations of the analyzer varied in a way consistent with the simulated

results. When the transmission axis of the analyzer is rotated from the parallel direction

of the polarizer to the orthogonal direction, the bright pixels of the image become dark

and vice versa, therefore an operation of image reversion can be easily achieved by

changing the orientation of the transmission axis of the analyzer. Actually, any pair of

images obtained after orthogonally orientated analyzer are complementary to each

other. For example, images obtained in α=0° and α=90°, or α=30° and α=

120° configurations, are mutually inverted from each other. This complementary

characteristic of the image pairs also indicates the superior polarization encoding

capability of the nonlinear metasurface. As the complementary characteristic of the

nonlinear image indicate, the summed image intensity should be homogenous, i.e. no

intensity modulation of SHG waves from the nonlinear metasurface. The measured

SHG image without an analyzer is shown in the last column of Fig. 4, from which we

can find that only slight intensity variation as predicted by the theory.

FIG. 4. Nonlinear vectorial metasurface for encoding a flower into the polarization profile of the SHG wave. The measurement setup is same as that in Fig. 3(a). The pumping wavelength is at 1250 nm. The last column shows the results when the analyzer [P2 in Fig. 3(a)] is absent in the experimental setup.

IV. CONCLUSION

To realize nonlinear responses, the complex phase-matching process and optically

large samples are typically required due to the inherent weak nonlinear response in

natural materials. Nonlinear metasurfaces have provided unprecedented capability to

produce similar effects with much smaller footprints, which can keep pace with

continued miniaturization of nonlinear devices and the daunting increase in the volume

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of the integrated nonlinear systems. Nonlinear metasurface paradigm is very promising

and can efficiently generate nonlinear polarization topology by engineering artificial

materials with predesigned polarization profile. The manipulation of light polarization

at subwavelength resolution via metasurfaces has been extended to the nonlinear optical

regime, enabling the applications of this technique for nonlinear optical security and

encryption, which are impossible or very difficult to realize with conventional methods.

Such nonlinear image information could be revealed after filtering out the FW and

converting the vectorial polarization profile into the intensity profile according to an

elegant rule (Malus’s law).

In this work, we utilized the spin-dependent nonlinear phase control metasurface

to manipulate the polarization profile of the second harmonic generation wave. A one-

to-one correspondence between the desired relative phase difference of the two spin

components of the SHG signal wave and the local orientation configuration of the

nonlinear meta-atoms can be built. With such an encoding process, one can effectively

control the polarization states of the SHG wave in the transverse plane. Using a linear

polarizer we can simply convert the polarization profile into an intensity profile, which

is easier for people to observe. Our demonstration of the polarization controlled

nonlinear metasurface provide a novel way for image encryption in nonlinear optical

process, which may have important applications for security of optical information.

ACKNOWLEDGEMENTS

G. L. is supported by the National Natural Science Foundation of China

(11774145), the Guangdong Provincial Innovation and Entrepreneurship Project

(2017ZT07C071), the Applied Science and Technology Project of Guangdong Science

and Technology Department (2017B090918001) and the Natural Science Foundation

of Shenzhen Municipal Science and Technology Innovation Commission

(JCYJ20170412153113701). X. C. acknowledge the support from Engineering and

Physical Sciences Research Council of the United Kingdom (Grant Ref:

EP/P029892/1). Y.T., Y.I. and J.D. contributed equally to this work.

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linear transmittances, and the simulation method of the SHG intensity profiles

under varies experimental configurations.