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Senthil Kumar Kuppusamy

Publications and source records attributed to Senthil Kumar Kuppusamy.

5 recordsLinked to original sources

Controlled ion-ion interactions and cavity-enhanced emission of a coherent dinuclear Eu$^{3+}$ complex

Molecular rare-earth-ion complexes offer unique opportunities for quantum technologies by combining the intrinsic coherence properties of rare-earth ions with chemically tunable molecular environments. A crucial capability is the realization of multi-qubit architectures with defined qubit couplings to enable two-qubit quantum gates. Here, we investigate the optical coherence properties and excitation-induced interactions of two Eu$^{3+}$-based molecular complexes, comparing a mononuclear reference system with a dinuclear analogue in which two Eu$^{3+}$ ions are positioned at a well-defined intramolecular distance of about 7 Angstrom. Using cryogenic ensemble spectroscopy, including spectral hole burning, free-induction decay, and photon echo measurements at temperatures down to 100 mK, we demonstrate long optical coherence times $T_{2,\text{o}}$ of up to 9 $μ$s. As a key step toward scalable multi-qubit architectures, a control-target sequence was implemented to probe conditional ion-ion interactions, revealing a stronger interaction-induced dephasing in the dinuclear complex. Finally, we show the integration of the dinuclear complex into a fiber-based optical microcavity, and observe an 380-fold emission enhancement of the $\mathrm{}^5\mathrm{D}_0\rightarrow\mathrm{}^7\mathrm{F}_0$ transition. Together, these results position molecular rare-earth complexes as versatile and chemically tunable building blocks for scalable quantum technologies.

quant-ph

Photophysical properties of Eu3+ complexes approaching electronic contact to a metal surface

The application of rare-earth complexes in electrically driven light sources poses a series of challenges that require specific optimization of the molecular photophysical properties. Here, we present a report on films of three different Eu3+ complexes characterized in terms of emission spectra and fluorescence decay. We compare molecular complexes in powder form and sublimed films, in films on glass and on a metal surface, and in films of thicknesses down to less than 3 nm (< 3 ML), approaching electrical coupling. Our photoluminescence experiments supported by scanning tunneling microscopy of sub-monolayers indicate that Eu3+(trensal) complexes are less affected by sublimation and more stable on the metal surface than typical beta diketonate complexes, making them promising candidates for electroluminescence devices.

cond-mat.mes-hall

Femtosecond spin-state switching dynamics of spin-crossover molecules condensed in thin films

The photoinduced switching of Fe(II)-based spin-crossover complexes from singlet to quintet takes place at ultrafast time scales. This a priori spin-forbidden transition triggered numerous time-resolved experiments of solvated samples to elucidate the mechanism at play. The involved intermediate states remain uncertain. We apply ultrafast x-ray spectroscopy in molecular films as a method sensitive to spin, electronic, and nuclear degrees of freedom. Combining the progress in molecule synthesis and film growth with the opportunities at x-ray free-electron lasers, we analyze the transient evolution of the Fe L3 fine structure at room temperature. Our measurements and calculations indicate the involvement of an Fe triplet intermediate state. The high-spin state saturates at half of the available molecules, limited by molecule-molecule interaction within the film.

cond-mat.mes-hall

Optically detected nuclear magnetic resonance of coherent spins in a molecular complex

Nuclear magnetic resonance (NMR) is a powerful tool for applications ranging from chemical analysis to quantum information processing. Achieving optical initialization and detection of molecular nuclear spins promises new opportunities - including improved NMR signals at low magnetic field, sensitivity down to the single-molecule level, and full access to atomically precise molecular architectures for quantum technologies. In this study, we report optical readout of coherently controlled nuclear spins in a europium-based molecular crystal. By harnessing ultra-narrow optical transitions, we achieve optical initialization and detection of nuclear spin states. Through radio-frequency driving, we address two nuclear quadrupole resonances, characterized by narrow inhomogeneous linewidths and a distinct correlation with the optical transition frequency. We implement Rabi oscillations, spin echo and dynamical decoupling techniques, achieving nuclear spin quantum coherence with a lifetime of up to 2 ms. These results highlight the capabilities of optically detected NMR (ODNMR) and underscore the potential of molecular nuclear spins for quantum information processing.

quant-ph

Organic ferroelectric Croconic Acid: A concise survey from bulk single crystals to thin films

Owing to prospective energy-efficient and environmentally benign applications, organic ferroelectric materials are useful and necessary alternative to inorganic ferroelectrics. Although the first discovered ferroelectric, Rochelle salt, was a salt of an organic compound, organic ferroelectrics have not been as abundant as the inorganic ones. Further, the small polarization values in the organic systems discovered so far have been a demotivating factor for their applications. However, scientific interest and activities surrounding such materials, for the purpose of fundamental understanding and practical applications, have significantly risen lately, especially after the discovery of above-room-temperature ferroelectricity in croconic acid (4,5-dihydroxy-4-cyclopentene-1,2,3-trione, H2C5O5) crystals with polarization values rivalling those found in inorganic ferroelectrics. Its large polarization, organic nature, and vacuum sublimability make croconic acid an ideal candidate for non-toxic and lead-free device applications. In this review article, we survey the scientific activities carried out so far involving ferroelectricity in this novel material, paying equal attention to its bulk single crystal and thin film forms. While we discuss about the origin of ferroelectric order and the reversal of polarization in the bulk form, we also summarize the directions toward applications of the thin films.

cond-mat.mtrl-sci