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1.
Nanoscale ; 11(31): 14540-14552, 2019 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-31364684

RESUMO

Strong coupling between plasmons in metal nanoparticles and single excitons in molecules or semiconductor nanomaterials has recently attracted considerable experimental effort for potential applications in quantum-mechanical and classical optical information processing and for fundamental studies of light-matter interaction. Here, we review the theory behind strong plasmon-exciton coupling and provide analytical expressions that can be used for fitting experimental data, particularly the commonly measured scattering spectra. We re-analyze published data using these expressions, providing a uniform method for evaluating and quantifying claims of strong coupling that avoids ambiguities in distinguishing between Rabi splitting and exciton-induced transparency (or Fano-like interference between plasmons and excitons).

2.
Sci Adv ; 5(7): eaav5931, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-31309142

RESUMO

Optical cavities can enhance and control light-matter interactions. This level of control has recently been extended to the nanoscale with single emitter strong coupling even at room temperature using plasmonic nanostructures. However, emitters in static geometries, limit the ability to tune the coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) with a nanocavity formed between a scanning plasmonic antenna tip and the substrate. By reversibly and dynamically addressing single quantum dots, we observe mode splitting up to 160 meV and anticrossing over a detuning range of ~100 meV, and with subnanometer precision over the deep subdiffraction-limited mode volume. Thus, TESC enables previously inaccessible control over emitter-nanocavity coupling and mode volume based on near-field microscopy. This opens pathways to induce, probe, and control single-emitter plasmon hybrid quantum states for applications from optoelectronics to quantum information science at room temperature.

3.
Proc Natl Acad Sci U S A ; 116(10): 4018-4024, 2019 03 05.
Artigo em Inglês | MEDLINE | ID: mdl-30765527

RESUMO

Optical trapping has been implemented in many areas of physics and biology as a noncontact sample manipulation technique to study the structure and dynamics of nano- and mesoscale objects. It provides a unique approach for manipulating microscopic objects without inducing undesired changes in structure. Combining optical trapping with hard X-ray microscopy techniques, such as coherent diffraction imaging and crystallography, provides a nonperturbing environment where electronic and structural dynamics of an individual particle in solution can be followed in situ. It was previously shown that optical trapping allows the manipulation of micrometer-sized objects for X-ray fluorescence imaging. However, questions remain over the ability of optical trapping to position objects for X-ray diffraction measurements, which have stringent requirements for angular stability. Our work demonstrates that dynamic holographic optical tweezers are capable of manipulating single micrometer-scale anisotropic particles in a microfluidic environment with the precision and stability required for X-ray Bragg diffraction experiments-thus functioning as an "optical goniometer." The methodology can be extended to a variety of X-ray experiments and the Bragg coherent diffractive imaging of individual particles in solution, as demonstrated here, will be markedly enhanced with the advent of brighter, coherent X-ray sources.


Assuntos
Técnicas Analíticas Microfluídicas , Pinças Ópticas , Tamanho da Partícula , Difração de Raios X
4.
Nano Lett ; 19(1): 277-282, 2019 01 09.
Artigo em Inglês | MEDLINE | ID: mdl-30539638

RESUMO

Modal gain coefficient is a key figure of merit for a laser material. Previously, net modal gain coefficients larger than a few thousand cm-1 were achieved in II-VI and III-V semiconductor gain media, but this required operation at cryogenic temperatures. In this work, using pump-fluence-dependent variable-stripe-length measurements, we show that colloidal CdSe nanoplatelets enable giant modal gain coefficients at room temperature up to 6600 cm-1 under pulsed optical excitation. Furthermore, we show that exceptional gain performance is common to the family of CdSe nanoplatelets, as shown by examining samples having different vertical thicknesses and lateral areas. Overall, colloidal II-VI nanoplatelets with superior optical gain properties are promising for a broad range of applications, including high-speed light amplification and loss compensation in plasmonic photonic circuits.

5.
Nat Commun ; 9(1): 4012, 2018 10 01.
Artigo em Inglês | MEDLINE | ID: mdl-30275446

RESUMO

Coherent coupling between plasmons and transition dipole moments in emitters can lead to two distinct spectral effects: vacuum Rabi splitting at strong coupling strengths, and induced transparency (also known as Fano interference) at intermediate coupling strengths. Achieving either strong or intermediate coupling between a single emitter and a localized plasmon resonance has the potential to enable single-photon nonlinearities and other extreme light-matter interactions, at room temperature and on the nanometer scale. Both effects produce two peaks in the spectrum of scattering from the plasmon resonance, and can thus be confused if scattering measurements alone are performed. Here we report measurements of scattering and photoluminescence from individual coupled plasmon-emitter systems that consist of a single colloidal quantum dot in the gap between a gold nanoparticle and a silver film. The measurements unambiguously demonstrate weak coupling (the Purcell effect), intermediate coupling (Fano interference), and strong coupling (Rabi splitting) at room temperature.

6.
Nanoscale ; 10(35): 16830-16838, 2018 Sep 13.
Artigo em Inglês | MEDLINE | ID: mdl-30167608

RESUMO

While gold nanorods (AuNRs) have found many applications due to their unique optical properties, a few challenges persist in their synthesis. Namely, it is often difficult to reproducibly synthesize AuNRs with specific and monodisperse sizes, especially at shorter aspect ratios. Here, we report a method of post-synthesis precise tailoring of AuNRs by etching with cysteamine. Cysteamine selectively etches AuNRs from their ends while preserving the initial rod shape and monodispersity, making this a viable means of obtaining highly monodisperse short AuNRs down to aspect ratio 2.3. Further, we explore the effect of this etching method on two types of silica-coated AuNRs: silica side-coated and silica end-coated AuNRs. We find that the etching process is cysteamine concentration-dependent and can lead to different degrees of sharpening of the silica-coated AuNRs, forming elongated tips. We also find that cysteamine behaves only as a ligand at concentrations above 200 mM, as no etching of the AuNRs is observed in this condition. Simulations show that excitation of plasmon resonances in these sharpened AuNRs produces local electric fields twice as strong as those produced by conventional AuNRs. Thus, cysteamine etching of AuNRs is shown to be an effective means of tailoring both the size and shape of AuNRs along with their corresponding optical properties. At the same time, the resulting cysteamine coating on the etched AuNRs displays terminal amino groups that allow for further functionalization of the nanorods.

7.
J Phys Chem Lett ; 9(8): 1900-1906, 2018 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-29589949

RESUMO

Colloidal semiconductor nanocrystals are commonly grown with a shell of a second semiconductor material to obtain desired physical properties, such as increased photoluminescence quantum yield. However, the growth of a lattice-mismatched shell results in strain within the nanocrystal, and this strain has the potential to produce crystalline defects. Here, we study CdSe/CdS core/shell nanorods as a model system to investigate the influence of core size and shape on the formation of stacking faults in the nanocrystal. Using a combination of high-angle annular dark-field scanning transmission electron microscopy and pair-distribution-function analysis of synchrotron X-ray scattering, we show that growth of the CdS shell on smaller, spherical CdSe cores results in relatively small strain and few stacking faults. By contrast, growth of the shell on larger, prolate spheroidal cores leads to significant strain in the CdS lattice, resulting in a high density of stacking faults.

8.
Nano Lett ; 17(11): 6900-6906, 2017 11 08.
Artigo em Inglês | MEDLINE | ID: mdl-28994296

RESUMO

Nonradiative Auger recombination limits the efficiency with which colloidal semiconductor nanocrystals can emit light when they are subjected to strong excitation, with important implications for the application of the nanocrystals in light-emitting diodes and lasers. This has motivated attempts to engineer the structure of the nanocrystals to minimize Auger rates. Here, we study Auger recombination rates in CdSe/CdS core/shell nanoplatelets, or colloidal quantum wells. Using time-resolved photoluminescence measurements, we show that the rate of biexcitonic Auger recombination has a nonmonotonic dependence on the shell thickness, initially decreasing, reaching a minimum for shells with thickness of 2-4 monolayers, and then increasing with further increases in the shell thickness. This nonmonotonic behavior has not been observed previously for biexcitonic recombination in quantum dots, most likely due to inhomogeneous broadening that is not present for the nanoplatelets.

9.
ACS Nano ; 11(9): 9360-9369, 2017 09 26.
Artigo em Inglês | MEDLINE | ID: mdl-28817767

RESUMO

Measurements of acoustic vibrations in nanoparticles provide an opportunity to study mechanical phenomena at nanometer length scales and picosecond time scales. Vibrations in noble-metal nanoparticles have attracted particular attention because they couple to plasmon resonances in the nanoparticles, leading to strong modulation of optical absorption and scattering. There are three mechanisms that transduce the mechanical oscillations into changes in the plasmon resonance: (1) changes in the nanoparticle geometry, (2) changes in electron density due to changes in the nanoparticle volume, and (3) changes in the interband transition energies due to compression/expansion of the nanoparticle (deformation potential). These mechanisms have been studied in the past to explain the origin of the experimental signals; however, a thorough quantitative connection between the coupling of phonon and plasmon modes has not yet been made, and the separate contribution of each coupling mechanism has not yet been quantified. Here, we present a numerical method to quantitatively determine the coupling between vibrational and plasmon modes in noble-metal nanoparticles of arbitrary geometries and apply it to silver and gold spheres, shells, rods, and cubes in the context of time-resolved measurements. We separately determine the parts of the optical response that are due to shape changes, changes in electron density, and changes in deformation potential. We further show that coupling is, in general, strongest when the regions of largest electric field (plasmon mode) and largest displacement (phonon mode) overlap. These results clarify reported experimental results and should help guide future experiments and potential applications.

10.
J Phys Chem Lett ; 8(15): 3607-3612, 2017 Aug 03.
Artigo em Inglês | MEDLINE | ID: mdl-28722415

RESUMO

Studies of the plasmon resonances in individual and coupled metal nanoparticles often involve imaging of the nanostructures of interest in an electron microscope. We show that this process can dramatically modify the optical spectra of coupled plasmonic nanoparticles, illustrated here with the case of gold nanorod-nanosphere dimers. The spectral changes are due to the thin, partially conductive carbonaceous layer that deposits onto the particles during imaging. These changes are particularly significant for coupled nanoparticles with subnanometer interparticle gaps but have largely been neglected in previous studies of such structures, including studies intended to probe quantum-mechanical effects in plasmon coupling. Accounting for the effects of the carbonaceous layer will lead to a more accurate understanding of such systems.

11.
Nat Commun ; 8(1): 143, 2017 07 26.
Artigo em Inglês | MEDLINE | ID: mdl-28747633

RESUMO

Colloidal semiconductor nanocrystals have emerged as promising active materials for solution-processable optoelectronic and light-emitting devices. In particular, the development of nanocrystal lasers is currently experiencing rapid progress. However, these lasers require large pump powers, and realizing an efficient low-power nanocrystal laser has remained a difficult challenge. Here, we demonstrate a nanolaser using colloidal nanocrystals that exhibits a threshold input power of less than 1 µW, a very low threshold for any laser using colloidal emitters. We use CdSe/CdS core-shell nanoplatelets, which are efficient nanocrystal emitters with the electronic structure of quantum wells, coupled to a photonic-crystal nanobeam cavity that attains high coupling efficiencies. The device achieves stable continuous-wave lasing at room temperature, which is essential for many photonic and optoelectronic applications. Our results show that colloidal nanocrystals are suitable for compact and efficient optoelectronic devices based on versatile and inexpensive solution-processable materials.Colloidal nanocrystals are a promising material for easy-to-fabricate nanolasers, but suffer from high threshold powers. Here, the authors combine colloidal quantum wells with a photonic-crystal cavity into a stable, continuous-wave room-temperature nanolaser with a threshold below one microwatt.

12.
Inorg Chem ; 55(21): 11522-11528, 2016 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-27775334

RESUMO

Noble metal nanoclusters (NCs) play a pivotal role in bridging the gap between molecules and quantum dots. Fundamental understanding of the evolution of the structural, optical, and electronic properties of these materials in various environments is of paramount importance for many applications. Using state-of-the-art spectroscopy, we provide the first decisive experimental evidence that the structural, electronic, and optical properties of Ag44(MNBA)30 NCs can now be tailored by controlling the chemical environment. Infrared and photoelectron spectroscopies clearly indicate that there is a dimerization between two adjacent ligands capping the NCs that takes place upon lowering the pH from 13 to 7.

13.
J Phys Chem Lett ; 6(6): 1032-6, 2015 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-26262865

RESUMO

Using time-resolved photoluminescence spectroscopy, we show that two-exciton Auger recombination dominates carrier recombination and cooling dynamics in CdSe nanoplatelets, or colloidal quantum wells. The electron-hole recombination rate depends only on the number of electron-hole pairs present in each nanoplatelet, and is consistent with a two-exciton recombination process over a wide range of exciton densities. The carrier relaxation rate within the conduction and valence bands also depends only on the number of electron-hole pairs present, apart from an initial rapid decay, and is consistent with the cooling rate being limited by reheating due to Auger recombination processes. These Auger-limited recombination and relaxation dynamics are qualitatively different from the carrier dynamics in either colloidal quantum dots or epitaxial quantum wells.

14.
Sci Rep ; 4: 6722, 2014 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-25342288

RESUMO

We demonstrate broadband non-resonant squeezing of terahertz (THz) waves through an isolated 2-nm-wide, 2-cm-long slit (aspect ratio of 10(7)), representing a maximum intensity enhancement factor of one million. Unlike resonant nanogap structures, a single, effectively infinitely-long slit passes incident electromagnetic waves with no cutoff, enhances the electric field within the gap with a broad 1/f spectral response, and eliminates interference effects due to finite sample boundaries and adjacent elements. To construct such a uniform, isolated slit that is much longer than the millimeter-scale spot of a THz beam, we use atomic layer lithography to pattern vertical nanogaps in a metal film over an entire 4-inch wafer. We observe an increasing field enhancement as the slit width decreases from 20 nm to 2 nm, in agreement with numerical calculations.

15.
Nano Lett ; 14(5): 2772-7, 2014 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-24773282

RESUMO

The use of colloidal semiconductor nanocrystals for optical amplification and lasing has been limited by the need for high input power densities. Here we show that colloidal nanoplatelets produce amplified spontaneous emission with thresholds as low as 6 µJ/cm(2) and gain as high as 600 cm(-1), both a significant improvement over colloidal nanocrystals; in addition, gain saturation occurs at pump fluences 2 orders of magnitude higher than the threshold. We attribute this exceptional performance to large optical cross-sections, slow Auger recombination rates, and narrow ensemble emission line widths.

16.
Nat Commun ; 4: 2361, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23999053

RESUMO

Squeezing light through nanometre-wide gaps in metals can lead to extreme field enhancements, nonlocal electromagnetic effects and light-induced electron tunnelling. This intriguing regime, however, has not been readily accessible to experimentalists because of the lack of reliable technology to fabricate uniform nanogaps with atomic-scale resolution and high throughput. Here we introduce a new patterning technology based on atomic layer deposition and simple adhesive-tape-based planarization. Using this method, we create vertically oriented gaps in opaque metal films along the entire contour of a millimetre-sized pattern, with gap widths as narrow as 9.9 Å, and pack 150,000 such devices on a 4-inch wafer. Electromagnetic waves pass exclusively through the nanogaps, enabling background-free transmission measurements. We observe resonant transmission of near-infrared waves through 1.1-nm-wide gaps (λ/1,295) and measure an effective refractive index of 17.8. We also observe resonant transmission of millimetre waves through 1.1-nm-wide gaps (λ/4,000,000) and infer an unprecedented field enhancement factor of 25,000.

17.
ACS Nano ; 7(10): 8794-800, 2013 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-24041038

RESUMO

Understanding whether noble-metal nanostructures can be trapped optically and under what conditions will enable a range of applications that exploit their plasmonic properties. However, there are several nontrivial issues that first need to be resolved. A major one is that metal particles experience strong radiation pressure in optical beams, while stable optical trapping requires an attractive force greater than this radiation pressure. Therefore, it has generally been considered impossible to obtain sufficiently strong gradient forces using single-beam optical tweezers to trap relatively large metal nanostructures in three dimensions. Here we demonstrate that a single, tightly focused laser beam with a wavelength of 800 nm can achieve three-dimensional optical trapping of individual gold (Au) nanowires with lengths over 2 µm. Nanowires can be trapped by the beam at one of their ends, in which case they undergo significant angular fluctuations due to Brownian motion of the untrapped end. They can also be trapped close to their midpoints, in which case they are oriented approximately perpendicular to the light polarization direction. The behavior is markedly different from that of Ag nanowires with similar length and diameter, which cannot be trapped in three dimensions by a single focused Gaussian beam. Our results, including electrodynamics simulations that help to explain our experimental findings, suggest that the conventional wisdom, which holds that larger metal particles cannot be trapped, needs to be replaced with an understanding based on the details of plasmon resonances in the particles.

18.
ACS Nano ; 7(2): 1790-802, 2013 Feb 26.
Artigo em Inglês | MEDLINE | ID: mdl-23363451

RESUMO

We demonstrate assembly of spheroidal Ag nanoparticle clusters, chains and arrays induced by optical binding. Particles with diameters of 40 nm formed ordered clusters and chains in aqueous solution when illuminated by shaped optical fields with a wavelength of 800 nm; specifically, close-packed clusters were formed in cylindrically symmetric optical traps, and linear chains were formed in line traps. We developed a coupled-dipole model to calculate the optical forces between an arbitrary number of particles and successfully predicted the experimentally observed particle separations and arrangements as well as their dependence on the polarization of the incident light. This demonstrates that the interaction between these small Ag particles and light is well described by approximating the particles as point dipoles, showing that these experiments extend optical binding into the Rayleigh regime. For larger Ag nanoparticles, with diameters of approximately 100 nm, the optical-binding forces become comparable to the largest gradient forces in the optical trap, and the particles can arrange themselves into regular arrays or synthetic photonic lattices. Finally, we discuss the differences between our experimental observations and the point dipole theory and suggest factors that prevent the Ag nanoparticles from aggregating as expected from the theory.

19.
Phys Rev Lett ; 111(24): 244502, 2013 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-24483667

RESUMO

Newtonian fluid mechanics, in which the shear stress is proportional to the strain rate, is synonymous with the flow of simple liquids such as water. We report the measurement and theoretical verification of non-Newtonian, viscoelastic flow phenomena produced by the high-frequency (20 GHz) vibration of gold nanoparticles immersed in water-glycerol mixtures. The observed viscoelasticity is not due to molecular confinement, but is a bulk continuum effect arising from the short time scale of vibration. This represents the first direct mechanical measurement of the intrinsic viscoelastic properties of simple bulk liquids, and opens a new paradigm for understanding extremely high frequency fluid mechanics, nanoscale sensing technologies, and biophysical processes.

20.
Nano Lett ; 12(12): 6158-63, 2012 Dec 12.
Artigo em Inglês | MEDLINE | ID: mdl-23137014

RESUMO

It has recently become possible to chemically synthesize atomically flat semiconductor nanoplatelets with monolayer-precision control over the platelet thickness. It has been suggested that these platelets are quantum wells; that is, carriers in these platelets are confined in one dimension but are free to move in the other two dimensions. Here, we report time-resolved photoluminescence and transient-absorption measurements of carrier relaxation that confirm the quantum-well nature of these nanomaterials. Excitation of the nanoplatelets by an intense laser pulse results in the formation of a high-temperature carrier population that cools back down to ambient temperature on the time scale of several picoseconds. The rapid carrier cooling indicates that the platelets are well-suited for optoelectronic applications such as lasers and modulators.

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