Absolute energy levels in nanodiamonds of different origins and surface chemistries

Daria Miliaieva; Aurelien Sokeng Djoumessi; Jan Čermák; Kateřina Kolářová; Maximilian Schaal; Felix Otto; Ekaterina Shagieva; Olexandr Romanyuk; Jiří Pangrác; Jaroslav Kuliček; Vojtech Nádaždy; Štěpán Stehlík; Alexander Kromka; Harald Hoppe; Bohuslav Rezek

doi:10.1039/D3NA00205E

Absolute energy levels in nanodiamonds of different origins and surface chemistries†

Daria Miliaieva,

*^ae Aurelien Sokeng Djoumessi,^bc Jan Čermák,^a Kateřina Kolářová,^a Maximilian Schaal,

^d Felix Otto,

^d Ekaterina Shagieva,^a Olexandr Romanyuk,^a Jiří Pangrác,^a Jaroslav Kuliček,^e Vojtech Nádaždy,^fg Štěpán Stehlík,^ah Alexander Kromka,

^a Harald Hoppe

^bc and Bohuslav Rezek

^e

Author affiliations

* Corresponding authors

^a Institute of Physics, Czech Academy of Sciences, Na Slovance 1999/2, 182 21 Prague 8, Czech Republic
E-mail: miliaieva@fzu.cz

^b Center for Energy and Environmental Chemistry Jena (CEEC Jena), Friedrich Schiller University Jena, Philosophenweg 7a, 07743 Jena, Germany

^c Laboratory of Organic and Macromolecular Chemistry (IOMC), Friedrich Schiller University Jena, Humboldstrasse 10, 07743 Jena, Germany

^d Institute of Solid State Physics, Friedrich Schiller University Jena, Helmholtzweg 5, 07743 Jena, Germany

^e Faculty of Electrical Engineering, Czech Technical University in Prague, 166 27 Prague, Czech Republic

^f Institute of Physics, Slovak Academy of Sciences, Dúbravská cesta 9, 845 11 Bratislava, Slovak Republic

^g Centre for Advanced Material Application, Slovak Academy of Sciences, Dúbravská cesta 9, 845 11 Bratislava, Slovak Republic

^h New Technologies – Research Centre, University of West Bohemia, Univerzitní 8, Pilsen, Czech Republic

Abstract

Nanodiamonds (NDs) are versatile, broadly available nanomaterials with a set of features highly attractive for applications from biology over energy harvesting to quantum technologies. Via synthesis and surface chemistry, NDs can be tuned from the sub-micron to the single-digit size, from conductive to insulating, from hydrophobic to hydrophilic, and from positively to negatively charged surface by simple annealing processes. Such ND diversity makes it difficult to understand and take advantage of their electronic properties. Here we present a systematic correlated study of structural and electronic properties of NDs with different origins and surface terminations. The absolute energy level diagrams are obtained by the combination of optical (UV-vis) and photoelectron (UPS) spectroscopies, Kelvin probe measurements, and energy-resolved electrochemical impedance spectroscopy (ER-EIS). The energy levels and density of states in the bandgap of NDs are correlated with the surface chemistry and structure characterized by FTIR and Raman spectroscopy. We show profound differences in energy band shifts (by up to 3 eV), Fermi level position (from p-type to n-type), electron affinity (from +0.5 eV to −2.2 eV), optical band gap (5.2 eV to 5.5 eV), band gap states (tail or mid-gap), and electrical conductivity depending on the high-pressure, high-temperature and detonation origin of NDs as well as on the effects of NDs' oxidation, hydrogenation, sp²/sp³ carbon phases and surface adsorbates. These data are fundamental for understanding and designing NDs' optoelectrochemical functional mechanisms in diverse application areas.

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Absolute energy levels in nanodiamonds of different origins and surface chemistries†

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