DNA-programmable assembly has been used to deliberately synthesize hundreds of different colloidal crystals spanning dozens of symmetries, but the complexity of the achieved structures has so far been limited to small unit cells. We assembled DNA-modified triangular bipyramids (~250-nanometer long edge, 177-nanometer short edge) into clathrate architectures. Electron microscopy images revealed that at least three different structures form as large single-domain architectures or as multidomain materials. Ordered assemblies, isostructural to clathrates, were identified with the help of molecular simulations and geometric analysis. These structures are the most sophisticated architectures made via programmable assembly, and their formation can be understood based on the shape of the nanoparticle building blocks and mode of DNA functionalization.

the radiation emitted by the room-temperature object is mainly in the LWIR region, with the peak wavelength of about 10 µm. [1] Because of these two properties, photodetectors operating in the LWIR range are of significant importance for the heat-seeking technologies, such as all-weather surveillance, night vision, and missile guidance. To detect such lowenergy radiation by photon detectors, commonly used photosensitive materials are narrow-bandgap semiconductors (e.g., HgCdTe) and quantum wells (e.g., GaAs/ InGaAs). [2,3] For these photodetectors, the dark current at room temperature usually is large, and thus a cryogenic cooling unit is indispensable, which certainly increases the size and weight of photon detectors. Therefore, to miniaturize the volume and weight of LWIR detectors, the development of high-performance uncooled photodetectors is vital. Thermal detectors are well known for their ultra-broadband spectral response from UV to far-infrared and even to terahertz at room temperature. The excellent ability of terahertz radiation (0.1-1 mm) to penetrate through nonconducting materials renders it particularly attractive for applications in tomographic inspection. [4,5] Thermal detectors are based on the measurement of temperature-dependent properties, such as the resistance for bolometers, the temperature-difference-driven voltage for photothermoelectric (PTE) detectors, and the spontaneous polarization for pyroelectric (PE) detectors. The photoresponse in PE detectors depends on the variation of the spontaneous polarization vector with temperature; therefore, an external chopper is needed when measuring the power of continuous-wave (CW) radiation. For bolometers, an external bias is required, which introduces the extra 1/f noise. The typical temperature-sensitive materials in commercial bolometers are vanadium oxide (VO x ) or amorphous silicon. The main advantage of VO x lies in that its temperature coefficient of resistance is high (≈4% K −1 ) while the resistivity remains low, which is beneficial to reduce the noise level. [6] Detailed comparisons among different kinds of photodetectors are listed in Table 1.PTE detectors are based on the photothermal conversion and thermoelectric effect. As schematically shown in Figure 1, after absorbing the photons on one side of PTE detector, a temperature difference (ΔT) is built up, which drives the directed diffusion of charge carriers from the hot end to the cold end, establishing an electric potential difference (ΔU). This process High-performance uncooled photodetectors operating in the long-wavelength infrared and terahertz regimes are highly demanded in the military and civilian fields. Photothermoelectric (PTE) detectors, which combine photothermal and thermoelectric conversion processes, can realize ultra-broadband photodetection without the requirement of a cooling unit and external bias. In the last few decades, the responsivity and speed of PTE-based photodetectors have made impressive progress with the discovery of novel thermoelectric materials and ...

The ability to precisely control nanocrystal (NC) shape and composition is useful in many fields, including catalysis and plasmonics. Seed-mediated strategies have proven effective for preparing a wide variety of structures, but a poor understanding of how to selectively grow corners, edges, and facets has limited the development of a general strategy to control structure evolution. Here, we report a universal synthetic strategy for directing the site-specific growth of anisotropic seeds to prepare a library of designer nanostructures. This strategy leverages nucleation energy barrier profiles and the chemical potential of the growth solution to control the site-specific growth of NCs into exotic shapes and compositions. This strategy can be used to not only control where growth occurs on anisotropic seeds but also control the exposed facets of the newly grown regions. NCs of many shapes are synthesized, including over 10 here-to-fore never reported NCs and, in principle, many others are possible.

DNA-programmable assembly has been used to prepare superlattices composed of octahedral and spherical nanoparticles, respectively. These superlattices have the same body-centered cubic lattice symmetry and macroscopic rhombic dodecahedron crystal habit but tunable lattice parameters by virtue of the DNA length, allowing one to study and determine the effect of nanoscale structure and lattice parameter on the light-matter interactions in the superlattices. Backscattering measurements and finite-difference time-domain simulations have been used to characterize these two classes of superlattices. Superlattices composed of octahedral nanoparticles exhibit polarization-dependent backscattering but via a trend that is opposite to that observed in the polarization dependence for analogous superlattices composed of spherical nanoparticles. Electrodynamics simulations show that this polarization dependence is mainly due to the anisotropy of the nanoparticles and is observed only if the octahedral nanoparticles are well-aligned within the superlattices. Both plasmonic and photonic modes are identified in such structures, both of which can be tuned by controlling the size and shape of the nanoparticle building blocks, the lattice parameters, and the overall size of the three-dimensional superlattices (without changing habit).

Halide perovskites have exceptional optoelectronic properties, but a poor understanding of the relationship between crystal dimensions, composition, and properties limits their use in integrated devices. We report a new multiplexed cantilever-free scanning probe method for synthesizing compositionally diverse and size-controlled halide perovskite nanocrystals spanning square centimeter areas. Single-particle photoluminescence studies reveal multiple independent emission modes due to defect-defined band edges with relative intensities that depend on crystal size at a fixed composition. Smaller particles, but ones with dimensions that exceed the quantum confinement regime, exhibit blue-shifted emission due to reabsorption of higher-energy modes. Six different halide perovskites have been synthesized, including a layered Ruddlesden-Popper phase, and the method has been used to prepare functional solar cells based on single nanocrystals. The ability to pattern arrays of multicolor light-emitting nanocrystals opens avenues toward the development of optoelectronic devices, including optical displays.

Photonic crystals have been widely studied due to their broad technological applications in lasers, sensors, optical telecommunications, and display devices. Typically, photonic crystals are periodic structures of touching dielectric materials with alternating high and low refractive indices, and to date, the variables of interest have focused primarily on crystal symmetry and the refractive indices of the constituent materials, primarily polymers and semiconductors. In contrast, finite difference time domain (FDTD) simulations suggest that plasmonic nanoparticle superlattices with spacer groups offer an alternative route to photonic crystals due to the controllable spacing of the nanoparticles and the high refractive index of the lattices, even far away from the plasmon frequency where losses are low. Herein, the stopband features of 13 Bravais lattices are characterized and compared, resulting in paradigm-shifting design principles for photonic crystals. Based on these design rules, a simple cubic structure with an ∼130-nm lattice parameter is predicted to have a broad photonic stopband, a property confirmed by synthesizing the structure via DNA programmable assembly and characterizing it by reflectance measurements. We show through simulation that a maximum reflectance of more than 0.99 can be achieved in these plasmonic photonic crystals by optimizing the nanoparticle composition and structural parameters.

Detailed phonon transport at Si/Ge interfaces is studied using the molecular dynamics wave-packet method. Three types of interfaces are investigated: A smooth interface, an interface with random roughness, and an interface with a regularly patterned roughness. The phonon transmissivity for each case is calculated as a function of phonon frequency, roughness characteristic length, and atomic structure. For a smooth interface, the transmissivities predicted by the MD simulations agree well with the acoustic mismatch model based on the continuum assumption. The rough interface simulation results indicate that random roughness is the source of incoherent phonon scattering and decreases the phonon transmission. Periodic structures such as the regularly patterned roughness employed in this paper cause strong phonon wave interference and may restore phonon transmission as the layer thickness increases.

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