Abstract
We report selective trapping of chiral nanoparticles via vector Lissajous beams. Local optical chirality densities appear in these beams by properly choosing the values of two parameters (p,q) that determine the polarization vectors of light. For a particular set of parameter (p,q) = (2,1) which is found preferable for the selective trapping, the resulting vector beam has two dominant intensity spots with opposite chirality. In the transverse plane, one spot traps a chiral particle while the other one repels the same particle under appropriate conditions, which can be reversed for a particle of opposite chirality. Various chiral parameters and radii of a particle are considered for analyzing this selective trapping effect. The longitudinal forces that are found non-conservative are also discussed. The achieved functionality of identifying and separating different chiral particles may find applications in enantiomer separation and drug delivery in pharmaceutics.
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1. Introduction
Polarization is an intrinsic and fundamental vectorial feature of light. It plays a crucial role in designing novel optical fields and realizing exotic light-matter interactions. Different polarizations can be imparted to an optical field in a position-dependent configuration. The resulting so-called vector light, represented by the well-known cylindrical vector beams (CVBs), manifests unique properties in the application of optical manipulation [1–6], optical communication [7], optical microscopy [8,9], material processing [10,11], etc. These progresses have triggered increasing attention in recent years on tailoring the polarization of light.
Quite recently, a new type of CVBs, namely vector Lissajous beams (VLBs), was proposed [12]. Their transverse components have an angular relationship that is described by Lissajous curves. The polarization vectors of these VLBs are defined by two integer parameters (or orders) denoted as (p,q). Compared with traditional CVBs characterized by a single order p, the extra degree of freedom allows for engineering different types (real, imaginary, or complex) of electromagnetic field components. In particular, one can employ the imaginary part of the longitudinal component to control the local distribution of spin angular momentum [12]. Featured with circularly/elliptically-polarizations, traditional CVBs were found useful in the separation and selective trapping of chiral objects that have structures of opposite handedness (also called as enantiomers: S and R enantiomers are defined to stand for left- and right-handed chiral compounds, respectively [13]). Thus one may expect that VLBs, whose polarizations are more controllable, can offer additional functions in such light manipulations.
In this paper, we study the chiral properties of VLBs and their use in manipulating chiral particles. We find that VLBs can exhibit optical chirality for a certain combination of the beam parameters (p,q). Among these combinations, the VLB with (p,q) = (2,1) is found preferable for the separation of S and R enantiomers, as it has two well-separated intensity spots that carry strong chirality. The forces of this optical field exerting on particles with opposite chiral parameters have a relationship of odd and even parity in the transverse and longitudinal dimensions, respectively. The two light spots are capable of separately trapping particles of inverted chirality transversely while applying longitudinal forces of the same direction on these particles. Thus such optical beams may find applications in simultaneous identification and selective delivery of opposite enantiomer molecules.
2. Chiral vector Lissajous beams
To begin with, we consider the generation of VLBs via a high numerical aperture (NA) objective lens with a focal length f. Using the Richards-Wolf vectorial diffraction theory [14,15] and Bessel identities [1], the electric and magnetic components of an optical field in the vicinity of the focus have the expressions of
Optical fields having circular (elliptical) polarizations are often loosely called as chiral fields [17]. The chirality of light can be characterized by a conservative quantity of an electromagnetic field, namely optical chirality density (OCD), which was introduced to quantify the strength of the coupling between a field and chirality of an object [18]. In general, the OCD is expressed as [18,19]:
3. Optical force on dipolar chiral particles
3.1 Theoretical model
We consider that a dipolar chiral particle located in vacuum is illuminated by an optical beam. Within the small particle limit [20,21], the polarizability elements of this particle read [21–26]
The expression of the time-averaged optical force acting on a dipolar chiral particle can be expressed as [21,22,24–26,30]:
3.2 Results and discussion
In this section, we investigate the optomechanical behavior of a dipolar chiral particle having a spherical shape illuminated by a chiral VLB. In calculations, the parameters are set as: $P = \;200\;\textrm{mW}$ (beam power), ${r_s} = \;30\;\textrm{nm}$ (particle’s radius), ${\varepsilon _s} = \;2.0 + 0.1i$, and ${\mu _s} = \;1$. The chirality parameter of the particle has a plural form where the real and imaginary (also called as chiral absorption) parts correspond to rotatory power and circular dichroism, respectively [19]. The other parameters are the same with those used in Fig. 1. The VLB with $({p,q} )= ({2,1} )$ is under concern in the following analysis, since it is featured with a high OCD and the regions of inverted chirality densities have a large spacing, which are both beneficial to the separation of enantiomers having opposite handedness.
We first examine the transverse trapping of a dipolar chiral particle, whose chirality parameter is chosen as $\kappa = 0.5 + 0.1i$ (S enantiomer) as an example (other parameters will be discussed later). This large chirality parameter is frequently concerned in literatures, such as Refs. [25,34–38]. Figure 2(a) presents the calculated transverse force ${{\textbf F}_t}$ ($|{{{\textbf F}_t}} |= \sqrt {F_x^2 + F_y^2}$). The upper light spot, subject to left-handedness OCD, exerts relatively stronger forces on this particle, although the bottom light spot has the same intensity pattern. These strong forces are centripetal, thus allowing for a transverse trapping. In contrast, the bottom light spot, featured with right-handedness OCD, tends to push the S enantiomer away. To explore the physical origin of these optical forces, their contributions in ${F_y}$ are analyzed, as shown in Fig. 2(b). Apparently, the components excluding the gradient force ${F_g}$ almost do not make a contribution. For further analysis, the gradient force is decomposed into three parts: two achiral optical forces formulated as ${{\textbf F}_{ach1}} = {{{\textrm{Re}} ({{\alpha_{ee}}} )\nabla {{|{\textbf E} |}^2}} / 4}$ and ${{\textbf F}_{ach2}} = {{{\textrm{Re}} ({{\alpha_{mm}}} )\nabla {{|{\textbf B} |}^2}} / 4}$, and a chiral optical force ${{\textbf F}_{ch}} = {{ - {\mathop{\rm Im}\nolimits} ({{\alpha_{em}}} )\nabla {\mathop{\rm Im}\nolimits} ({{\textbf B} \cdot {{\textbf E}^ \ast }} )} / 2}$. Their distributions along the y-axis are presented in Fig. 2(c). ${F_{ch}}$ and ${F_{ach1}}$ exhibit a quite larger magnitude compared with ${F_{ach2}}$. In the region of $y > 0$ ($y < 0$), where the upper (bottom) light spot locates, the two main contributors in the gradient force tend to strengthen (contradict) each other. Furthermore, the parity of the gradient force is considered. For doing this, we start from the analysis of Eq. (8), and find the spherical wave functions satisfy the following relationships:
Next, we examine the selective trapping of enantiomers with other chirality parameters. To this end, the transverse trapping potential along the y-axis, defined as ${V_y} ={-} \int {{F_y}\; dy}$ [39], is calculated. Its distributions for different S enantiomers are presented in Figs. 3(a) and 3(b). The potential offered by the upper light spot is always a well, indicating a trapping effect. The trapping strength is more influenced by the real part of $\kappa$. In order to achieve a selective trapping for opposite enantiomers, the potential induced by the bottom light spot should be a barrier for an S enantiomer by considering the symmetry property (i.e., Eq. (14)) of the transverse force. This condition is yet not satisfied for all the chirality parameters. For instance, it is only met for ${\textrm{Re}} (\kappa )\ge 0.483$ and $- 0.192 \le {\mathop{\rm Im}\nolimits} (\kappa )\le 0.275$ in Fig. 3(a) and Fig. 3(b), respectively. Other more parameters meeting this condition are summarized in Fig. 3(c). They locate above the curve of ${\textrm{Re}} ({{\kappa_0}} )$ versus ${\mathop{\rm Im}\nolimits} ({{\kappa_0}} )$ (${\kappa _0}$ is hence defined as critical chiral parameter). In particular, as along as the value of ${\textrm{Re}} (\kappa )$ is sufficiently high (say, $\ge 0.945$), a selective trapping always exists regardless of the chiral absorption. For particles of other sizes, the value of ${\kappa _0}$ shows similar distributions [Fig. 3(c)].
Finally, we consider the longitudinal optical force ${F_z}$ of the VLB exerting on enantiomers. ${F_z}$ along the y-axis (x = 0) together with its contributions are displayed in Fig. 4(a) for an S enantiomer ($\kappa = 0.5 + 0.1i$). Pushing (${F_z} > 0$) and pulling (${F_z} < 0$) forces appear in the upper and bottom light spot, respectively. The longitudinal optical force is nearly not contributed by the gradient force ${F_g}$ and the alternating flow force ${F_f}$ [Fig. 4(a)]. This feature holds for the cases of other chirality parameters, as shown in Figs. 4(b) and 4(c). In this regard, we can safely write ${F_z}$ in the form of ${F_z} \cong {F_r} + {F_v} + {F_c} + {F_s}$ based on Eq. (9). Using the result in Eq. (12) together with the symmetry property [Eq. (13)] of the optical field, it is readily to obtain:
Thus, for opposite enantiomers that are assumed to be trapped transversely in different light spots, they experience longitudinal forces with the same direction and strength. This non-conserved force is helpful for the delivery of the chiral particles. Its strength is more sensitive to the imaginary part of the chirality parameter [Figs. 4(b) and 4(c)], which is contrary to the case of the transverse force. The sign of the longitudinal force is only determined by the sign of the chiral absorption [Fig. 4(c)].
4. Conclusion
In summary, we have investigated the chiral properties of VLBs in the manipulation of chiral particles. It is found that the OCD is not zero for certain relations of orders $({p,q} )$. We focus on a VLB whose chiral property is more beneficial to the separation of opposite enantiomers. For dipolar particles with opposite chiral parameters, the forces offered by this optical field have a relationship of odd and even parity in the transverse and longitudinal directions, respectively. The two spots of this optical beam can trap particles of inverted chirality transversely, while always exerting a force in the same direction longitudinally. Such a selective trapping effect is discussed for various chiral parameters and radii of dipolar particles. Our results may find potential applications in optical selection and separation of chiral particles at nanometer scales. More intriguing phenomena are expected by employing the VLBs to manipulate chiral particles in nontrivial media [40,41].
Funding
National Key Research and Development Program of China (2017YFA0303800); National Natural Science Foundation of China (12022404, 62075105, 91750204); 111 Project (B07013).
Disclosures
The authors declare that there are no conflicts of interest related to this article.
Data availability
Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.
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