: Chiral inorganic nanostructures strongly interact with photons changing their polarization state. The resulting circularly polarized light emission (CPLE) has cross-disciplinary importance for a variety of chemical/biological processes and is essential for development of chiral photonics. However, the polarization effects are often complex and could be misinterpreted. CPLE in nanostructured media has multiple origins and several optical effects are typically convoluted into a single output. Analysing CPLE data obtained for nanoclusters, NPs, nanoassemblies, and nanocomposites from metals, chalcogenides, perovskite, and other nanostructures, we show that there are several distinct groups of nanomaterials for which CPLE is dominated either by circularly polarized luminescence (CPL) or circularly polarized scattering (CPS); there are also many nanomaterials for which they are comparable. We also show that (1) CPL and CPS contributions involve light-matter interactions at different structural levels; (2) contribution from CPS is especially strong for nanostructured microparticles, nanoassemblies and composites; and (3) engineering of materials with strongly polarized light emission requires synergistic implementation of CPL and CPS effects. These findings are expected to guide development of CPLE materials in a variety of technological fields, including 3D displays, information storage, biosensors, optical spintronics, and biological probes.
more »
« less
Optical Chirality Detection Using a Topological Insulator Transistor
Abstract Optical chirality is an effective means in screening molecules and their enantiomers in bioengineering, and recently has garnered attention as an implementation of qubits in quantum information processing. The conventional detection of circularly polarized light (CPL) is based on phase retardation and polarization separation using multiple optical components. An intrinsic solid‐state chirality detection device would be favorable for easier integration and implementation. Optical spin injection to the spin‐momentum‐locked topological surface states of topological insulators (TIs) by circularly polarized light leads to a directional DC photocurrent and hence possible circular polarization detection. However, this DC photocurrent is also accompanied by other photo‐responses. Here, a photodetection strategy using a TI transistor which senses CPL without the use of any additional components is demonstrated, it achieves a uniform response over the entire device with a sensitivity ≈5.6%. The Stokes parameters can also be extracted by arithmetic operation of photocurrents obtained with different bias and gate for a complete characterization of a polarized light beam. Therefore, this method enables chirality detection and Stokes parameter analysis using a single device. The proposed miniaturized intrinsic chirality detectors facilitate polarimetry sensing in applications from circular dichroism spectroscopy to biomedical diagnosis.
more »
« less
- Award ID(s):
- 1641101
- PAR ID:
- 10452999
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- Volume:
- 9
- Issue:
- 10
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Three-dimensional topological insulators have been demonstrated in recent years, which possess intriguing gapless, spin-polarized Dirac states with linear dispersion only on the surface. The spin polarization of the topological surface states is also locked to its momentum, which allows controlling motion of electrons using optical helicity, i.e., circularly polarized light. The electrical and thermal transport can also be significantly tuned by the helicity-control of surface state electrons. Here, we report studies of photo-thermoelectric effect of the topological surface states in Bi2Te2Se thin films with large tunability using varied gate voltages and optical helicity. The Seebeck coefficient can be altered by more than five times compared to the case without spin injection. This deep tuning is originated from the optical helicity-induced photocurrent which is shown to be enhanced, reduced, turned off, and even inverted due to the change of the accessed band structures by electrical gating. The helicity-selected topological surface state thus has a large effect on thermoelectric transport, demonstrating great opportunities for realizing helicity control of optoelectronic and thermal devices.more » « less
-
Abstract Chiral perovskite nanocrystals have emerged as an interesting chiral excitonic platform that combines both structural flexibility and superior optoelectronic properties. Despite several recent demonstrations of optical activity in various chiral perovskite nanocrystals, efficient circularly polarized luminescence (CPL) with tunable energies remains a challenge. The chirality imprinting mechanism as a function of perovskite nanocrystal dimensionality remains elusive. Here, atomically thin inorganic perovskite nanoplatelets (NPLs) are synthesized with precise control of layer thickness and are functionalized by chiral surface ligands, serving as a unique platform to probe the chirality transfer mechanism at the organic/perovskite interface. It is found that chirality is successfully imprinted into mono‐, bi‐, and tri‐layer inorganic perovskite NPLs, exhibiting tunable circular dichroism (CD) and CPL responses. However, chirality transfer decreases in thicker NPLs, resulting in decreased CD and CPL dissymmetry factors for thicker NPLs. Aided by large‐scale first‐principles calculations, it is proposed that chirality transfer is mainly mediated through a surface distortion rather than a hybridization of electronic states, giving rise to symmetry breaking in the perovskite lattice and spin‐split conduction bands. The findings described here provide an in‐depth understanding of chirality transfer and design principles for distorted‐surface perovskites for chiral photonic applications.more » « less
-
Abstract Plasmon‐mediated synthesis enables isotropic metal nanocrystal growth with linearly polarized light. This limits the effect of the polarization of incident light during synthesis, and thus restricts the structural chirality of nanocrystals produced with circularly polarized light (CPL). This study here demonstrates that surface engineering of initial achiral silver nanorods (AgNRs) can enhance the structural chirality of the resulting nanostructures produced with CPL. Specifically, the surface ligand hexadecyltrimethylammonium bromide (CTAB) stabilizes the lateral (100) facet‐terminated sides of achiral AgNRs and inhibits lateral growth. This surface engineering with achiral ligands results in increased dissymmetry of the nanostructures during the early stages of photo‐growth and leads to the formation of “hook” structures, where silver preferentially deposits near the tips of the nanorods. Upon further CPL illumination, these “hook” structures exhibit a significantly larger dissymmetry in the local electric field enhancement distribution compared to the initial achiral AgNRs. This highly dissymmetric electric field enhancement profile influences subsequent growth, resulting in AgNRs with enhanced structural chirality. Notably, the optical dissymmetry of these chiral nanostructures withg‐factor≈0.05 is an order of magnitude greater than that reported in previous studies conducted under similar chemical conditions but without surface engineering.more » « less
-
ABSTRACT Circular birefringence (CB) is defined as the difference in refractive index for opposite circular polarization states and has played a crucial role in the development of stereochemistry and the concept of chirality. It manifests experimentally as optical rotatory dispersion (ORD), that is, the wavelength‐dependent optical rotation of the plane of light polarization. However, most methods for probing ORD rely on analyzing transmitted light asymmetry at single wavelengths (usually the sodium D‐line at 589 nm) with linear polarizers, which cannot discern between unpolarized and circularly polarized light, limiting the apparatus to analyze a single phenomenon. Here we showcase the use of Stokes spectropolarimetry (SSP), a versatile and cost‐effective technique, to probe ORD of circularly birefringent materials. This technique allows complete analysis of the dispersive changes in polarization caused by anisotropic media, portraying a versatile experimental framework to study different types of optical anisotropies with a single spectropolarimeter. Here, aqueous solutions of chiral sucrose, fructose, and their mixtures are investigated. The ORD acquired verify that the optical rotation is proportional to the concentration of the chiral species and follows an inverse proportion with wavelength. As a case study, we show via SSP that ORD at 589 nm (D‐line of sodium) is in good agreement with literature (+63.5° ± 1.4° mL g−1 dm−1for sucrose and −83.7° ± 2.0° mL g−1 dm−1for fructose).more » « less
An official website of the United States government
