Diamondoid coating enables disruptive approach for chemical and magnetic imaging with 10 nm spatial resolution

Ishiwata, Hitoshi; Acremann, Yves; Schöll, A.; Rotenberg, Eli; Hellwig, Olav; Dobisz, Elizabeth A.; Doran, Andrew; Tkachenko, Boryslav A.; Fokin, Andrey A.; Schreiner, Peter R.; Dahl, Jeremy E. P.; Carlson, Robert M. K.; Melosh, Nick; Shen, Zhi‐Xun; Ohldag, Hendrik

doi:10.1063/1.4756893

Cited by 19 publications

(24 citation statements)

References 44 publications

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“…[1][2][3][4] Such systems are promising candidates for tuning of optical properties, [5][6][7] with a variety of applications ranging from molecular building blocks for optoelectronics to biocompatible, photostable biomarkers. [8][9][10][11][12][13][14][15] In particular, the observation of photoluminescence (PL) in reduced-dimensional semiconductor systems, which otherwise exhibit an indirect band gap, like Si and C (diamond), opens possibilities to tailor their optical properties and to interface with already existing technologies. [2][3][4] However, despite numerous studies, [2][3][4]16,17 the fundamental photophysical processes in such systems still are not fully understood.…”

Section: Introductionmentioning

confidence: 99%

Size and shape dependent photoluminescence and excited state decay rates of diamondoids

Richter

Wolter

Zimmermann

et al. 2014

Phys. Chem. Chem. Phys.

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We present photoluminescence spectra and excited state decay rates of a series of diamondoids, which represent molecular structural analogues to hydrogen-passivated bulk diamond. Specific isomers of the five smallest diamondoids (adamantane-pentamantane) have been brought into the gas phase and irradiated with synchrotron radiation. All investigated compounds show intrinsic photoluminescence in the ultraviolet spectral region. The emission spectra exhibit pronounced vibrational fine structure which is analyzed using quantum chemical calculations. We show that the geometrical relaxation of the first excited state of adamantane, exhibiting Rydberg character, leads to the loss of T d symmetry. The luminescence of adamantane is attributed to a transition from the delocalized first excited state into different vibrational modes of the electronic ground state. Similar geometrical changes of the excited state structure have also been identified in the other investigated diamondoids. The excited state decay rates show a clear dependence on the size of the diamondoid, but are independent of the particle geometry, further indicating a loss of particle symmetry upon electronic excitation.

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Section: Introductionmentioning

confidence: 99%

Size and shape dependent photoluminescence and excited state decay rates of diamondoids

Richter

Wolter

Zimmermann

et al. 2014

Phys. Chem. Chem. Phys.

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“…[140][141][142][143] These binding energies vary with diamondoid monolayer structure and thiol substitution position, consistent with different degrees of steric strain and electronic interaction with the substrate. [144][145][146] But the optical properties of the diamondoids are strongly affected due to a drastic change in the occupied states. 7).…”

Section: Diamondoids In Optical Devicesmentioning

confidence: 99%

Derivatization of diamondoids for functional applications

et al. 2015

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Diamondoids, a group of hydrocarbon cage molecules that resemble diamond lattice, are attracting increasing interest in the past decade. Their diamond-like structure warrants that diamondoids inherit the superior properties of diamond at nanoscale, including exceptional hardness and stiffness, high thermal stability, high chemical resistance, unique optical properties and fluorescence, and excellent biocompatibility. To effectively take advantage of the fascinating properties of diamondoids, they must be properly functionalized so that they can be covalently incorporated into the host systems or compatibly mixed with the hosts. Herein, the origin, synthesis, derivatization, and application of diamondoids are reviewed. In particular, how the derivatized diamondoids for various functional applications, including pharmaceuticals, polymers, fine chemicals, nanomaterials, and optical devices, are discussed. It is hoped that this review article can attract more interest in diamondoids, which in turn helps motivate the development of new synthesis and application of diamondoids and their derivatives so that this group of unique molecules can bring more benefits. Scheme 3 Bromination of adamantane under phase-transfer conditions.Scheme 4 Synthesis of 1,3,5,7-tetrabromoadamantane.Scheme 5 Preparation of 1-adamantanol by the ozonation of adamantane over silica gel.Scheme 6 Preparation of adamantyl amine.Scheme 7 Preparation of 1,3-adamantanedicarboxylic acid.

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“…This means that the materials system should be chosen to create a clear contrast with the features of interest appearing bright in the image, which in some circumstances can be done by an appropriate choice of substrate [17]. The contrast can also be modified by surface manipulation such as adsorption of molecules [59] or alkali metals [11].…”

Section: Xuv Imagingmentioning

confidence: 99%

Imaging Localized Surface Plasmons by Femtosecond to Attosecond Time‐Resolved Photoelectron Emission Microscopy – “ATTO‐PEEM”

Chew

Pearce

Scheffold

et al. 2014

Attosecond Nanophysics

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The direct detection of the spatiotemporal dynamics of nanolocalized optical near-fields on nanostructured metal surfaces, for example, imaging of localized surface plasmons (cf. Chapter 1) on rough or nanostructured metal films or the imaging of propagating surface plasmon polaritons at a vacuum-metal or metal-dielectric interface is a prerequisite to further control and optimize surface-plasmon based ultrafast nanooptics for future device development and applications [1][2][3][4].While free electrons in metals collectively respond to excitation from a light pulse, which is resonant to the surface plasmon frequency of the system, and squeeze and amplify the field intensity of the incoming plane light field into a subwavelength spatial volume, the typically broad frequency bandwidth of surface plasmon resonances supports an ultrafast response of these fields with rapid field changes on sub-femtosecond time scales [5].The sub-wavelength nanoscaled localization of optical fields in the vicinity of metal nanostructures and the ultrafast temporal evolution of such fields on a 0.1-100 fs time scale require the invention and development of new experimental methodologies, which combine nanometer (sub-optical) spatial resolution, sub-femtosecond temporal resolution, and optionally further nanospectroscopic information.Resolving the spatial distribution of such fields requires a microscopic technique with sub-optical spatial resolution, for example, in the 10-100 nm range. Scanning near-field optical microscopy (SNOM) techniques have been successfully applied with spatial resolutions of about ∼100 nm; however, the combination with ultrashort light pulses is still very difficult. Photoemission electron microscopy (PEEM) is a technique capable of resolving the spatial emission distribution of photoelectrons with an ultimate resolution of ∼10 nm.

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Diamondoid coating enables disruptive approach for chemical and magnetic imaging with 10 nm spatial resolution

Cited by 19 publications

References 44 publications

Size and shape dependent photoluminescence and excited state decay rates of diamondoids

Size and shape dependent photoluminescence and excited state decay rates of diamondoids

Derivatization of diamondoids for functional applications

Imaging Localized Surface Plasmons by Femtosecond to Attosecond Time‐Resolved Photoelectron Emission Microscopy – “ATTO‐PEEM”

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