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Dmitri R. Yakovlev

Publications and source records attributed to Dmitri R. Yakovlev.

53 records · Page 3Linked to original sources

Polarized emission of CdSe nanocrystals in magnetic field: the role of phonon-assisted recombination of the dark exciton

The recombination dynamics and spin polarization of excitons in CdSe nanocrystals synthesized in a glass matrix are investigated using polarized photoluminescence in high magnetic fields up to 30 Tesla. The dynamics are accelerated by increasing temperature and magnetic field, confirming the dark exciton nature of the low-temperature photoluminescence (PL). The circularly polarized PL in magnetic fields reveals several unusual appearances: (i) a spectral dependence of the polarization degree, (ii) its low saturation value, and (iii) a stronger intensity of the Zeeman component which is higher in energy. The latter feature is the most surprising being in contradiction with the thermal population of the exciton spin sublevels. The same contradiction was previously observed in the ensemble of wet-chemically synthesized CdSe nanocrystals, but was not understood. We present a theory which explains all the observed features and shows that the inverted ordering of the circular polarized PL maxima from the ensemble of nanocrystals is a result of competition between the zero phonon (ZPL) and one optical phonon (1PL) assisted emission of the dark excitons. The essential aspects of the theoretical model are different polarization properties of the dark exciton emission via ZPL and 1PL recombination channels and the inhomogeneous broadening of the PL spectrum from the ensemble of nanocrystals exceeding the optical phonon energy.

cond-mat.mes-hall↗

Optical second and third harmonic generation on excitons in ZnSe/BeTe quantum wells

Optical harmonic generation on excitons is found in ZnSe/BeTe quantum wells with type-II band alignment. Two experimental approaches with spectrally-broad femtosecond laser pulses and spectrally-narrow picosecond pulses are used for spectroscopic studies by means of second and third harmonic generation (SHG and THG). The SHG signal is symmetry-forbidden for light propagation along the structure's growth axis, which is the [001] crystal axis, but can be induced by an external magnetic field. The THG signal is detected at zero magnetic field and its intensity is field independent. A group theory analysis of SHG and THG rotational anisotropy diagrams allows us to identify the involved excitation mechanisms.

physics.optics↗

Optical harmonic generation on the exciton-polariton in ZnSe

We study optical harmonic generation on the 1S exciton-polariton in the semiconductor ZnSe. Intense and spectrally narrow exciton resonances are found in optical second (SHG), third (THG), and fourth (FHG) harmonic generation spectra. The resonances are shifted to higher energy by 3.2 meV from the exciton energy in the linear reflectivity spectrum. Additional resonances are observed in the THG and FHG spectra and assigned to combinations of incident and backscattered photons in the crystal. Rotational anisotropy diagrams are measured and further information on the origin of the optical harmonic generation and the involved exciton states is obtained by a symmetry analysis using group theory in combination with a microscopic consideration.

physics.optics↗

Magnon polaron formed by selectively coupled coherent magnon and phonon modes of a surface patterned ferromagnet

Strong coupling between two quanta of different excitations leads to the formation of a hybridized state which paves a way for exploiting new degrees of freedom to control phenomena with high efficiency and precision. A magnon polaron is the hybridized state of a phonon and a magnon, the elementary quanta of lattice vibrations and spin waves in a magnetically-ordered material. A magnon polaron can be formed at the intersection of the magnon and phonon dispersions, where their frequencies coincide. The observation of magnon polarons in the time domain has remained extremely challenging because the weak interaction of magnons and phonons and their short lifetimes jeopardize the strong coupling required for the formation of a hybridized state. Here, we overcome these limitations by spatial matching of magnons and phonons in a metallic ferromagnet with a nanoscale periodic surface pattern. The spatial overlap of the selected phonon and magnon modes formed in the periodic ferromagnetic structure results in a high coupling strength which, in combination with their long lifetimes allows us to find clear evidence of an optically excited magnon polaron. We show that the symmetries of the localized magnon and phonon states play a crucial role in the magnon polaron formation and its manifestation in the optically excited magnetic transients.

cond-mat.mtrl-sci↗

Second Harmonic Generation of cuprous oxide in magnetic fields

Recently Second Harmonic Generation (SHG) for the yellow exciton series in cuprous oxide has been demonstrated [J. Mund et al., Phys. Rev. B 98, 085203 (2018)]. Assuming perfect $O_{\mathrm{h}}$ symmetry, SHG is forbidden along certain high-symmetry axes. Perturbations can break this symmetry and forbidden transitions may become allowed. We investigate theoretically the effect of external magnetic fields on the yellow exciton lines of cuprous oxide. We identify two mechanisms by which an applied magnetic field can induce a second harmonic signal in a forbidden direction. First of all, a magnetic field by itself generally lifts the selection rules. In the Voigt configuration, an additional magneto-Stark electric field appears. This also induces certain SHG processes differing from those induced by the magnetic field alone. Complementary to the manuscript by A. Farenbruch et al. [Phys. Rev. B, submitted], we perform a full numerical diagonalization of the exciton Hamiltonian including the complex valence band structure. Numerical results are compared with experimental data.

cond-mat.mes-hall↗

Single and double electron spin-flip Raman scattering in CdSe colloidal nanoplatelets

CdSe colloidal nanoplatelets are studied by spin-flip Raman scattering in magnetic fields up to 5 T. We find pronounced Raman lines shifted from the excitation laser energy by an electron Zeeman splitting. Their polarization selection rules correspond to those expected for scattering mediated by excitons interacting with resident electrons. Surprisingly, Raman signals shifted by twice the electron Zeeman splitting are also observed. The theoretical analysis and experimental dependencies show that the mechanism responsible for the double flip involves two resident electrons interacting with a photoexcited exciton. Effects related to various orientations of the nanoplatelets in the ensemble and different orientations of the magnetic field are analyzed.

cond-mat.mes-hall↗

Surface spin magnetism controls the polarized exciton emission from CdSe nanoplatelets

The surface of nominally diamagnetic colloidal CdSe nanoplatelets can demonstrate paramagnetism owing to the uncompensated spins of dangling bonds (DBSs). We reveal that by optical spectroscopy in high magnetic fields up to 15 Tesla using the exciton spin as probe of the surface magnetism. The strongly nonlinear magnetic field dependence of the circular polarization of the exciton emission is determined by the DBS and exciton spin polarization as well as by the spin-dependent recombination of dark excitons. The sign of the exciton-DBS exchange interaction can be adjusted by the nanoplatelet growth conditions.

cond-mat.mes-hall↗

Origin of Two Larmor Frequencies in the Coherent Spin Dynamics of Colloidal CdSe Quantum Dots Revealed by Controlled Charging

Coherent spin dynamics in colloidal CdSe quantum dots (QDs) typically show two spin components with different Larmor frequencies, whose origin is an open question. We exploit the photocharging approach to identify their origin and find that surface states play a key role in the appearance of the spin signals. By controlling the photocharging with electron or hole acceptors, we show that the specific spin component can be enhanced by the choice of acceptor type. In core/shell CdSe/ZnS QDs, the spin signals are significantly weaker. Our results exclude the neutral exciton as the spin origin and suggest that both Larmor frequencies are related to the coherent spin precession of electrons in photocharged QDs. The lower frequency is due to the electron confined in the middle of the QD, and the higher frequency to the electron additionally localized in the vicinity of the surface.

cond-mat.mes-hall↗

Coherent spin dynamics of electrons and holes in CsPbBr$_3$ perovskite crystals

The lead halide perovskites demonstrate huge potential for optoelectronic applications, high energy radiation detectors, light emitting devices and solar energy harvesting. Those materials exhibit strong spin-orbit coupling enabling efficient optical orientation of carrier spins in perovskite-based devices with performance controlled by a magnetic field. Perovskites are promising for spintronics due to substantial bulk and structure inversion asymmetry, however, their spin properties are not studied in detail. Here we show that elaborated time-resolved spectroscopy involving strong magnetic fields can be successfully used for perovskites. We perform a comprehensive study of high-quality CsPbBr$_3$ crystals by measuring the exciton and charge carrier $g$-factors, spin relaxation times and hyperfine interaction of carrier and nuclear spins by means of coherent spin dynamics. Owing to their "inverted" band structure, perovskites represent appealing model systems for semiconductor spintronics exploiting the valence band hole spins, while in conventional semiconductors the conduction band electrons are considered for spin functionality.

cond-mat.mtrl-sci↗

High-Resolution Second Harmonic Generation Spectroscopy with Femtosecond Laser Pulses on Excitons in Cu$_2$O

We present a novel spectroscopic technique for second harmonic generation (SHG) using femtosecond laser pulses at 30~kHz repetition rate, which nevertheless provides high spectral resolution limited only by the spectrometer. The potential of this method is demonstrated by applying it to the yellow exciton series of Cu$_2$O. Besides even parity states with $S-$ and $D-$ envelope, we also observe odd parity, $P-$ excitons with linewidths down to 100 $μ$eV, despite of the broad excitation laser spectrum with a full width at half maximum of 14~meV. The underlying light-matter interaction mechanisms of SHG are elaborated by a group theoretical analysis which allows us to determine the linear and circular polarization dependences, in good agreement with experiment.

physics.optics↗

Electron and hole g-factors and spin dynamics of negatively charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells

We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with increasing magnetic field from -0.4 to -0.7 is evaluated. Hole g-factors for two-dimensional structures are calculated for various hole confining potentials for cubic- and wurtzite lattice in CdSe core. These calculations are extended for various quantum dots and nanoplatelets based on II-VI semiconductors. We developed a magneto-optical technique for the quantitative evaluation of the nanoplatelets orientation in ensemble.

cond-mat.mes-hall↗

Addressing the exciton fine structure in colloidal nanocrystals: the case of CdSe nanoplatelets

We study the band-edge exciton fine structure and in particular its bright-dark splitting in colloidal semiconductor nanocrystals by four different optical methods based on fluorescence line narrowing and time-resolved measurements at various temperatures down to 2 K. We demonstrate that all these methods provide consistent splitting values and discuss their advances and limitations. Colloidal CdSe nanoplatelets with thicknesses of 3, 4 and 5 monolayers are chosen for experimental demonstrations. The bright-dark splitting of excitons varies from 3.2 to 6.0 meV and is inversely proportional to the nanoplatelet thickness. Good agreement between experimental and theoretically calculated size dependence of the bright-dark exciton slitting is achieved. The recombination rates of the bright and dark excitons and the bright to dark relaxation rate are measured by time-resolved techniques.

cond-mat.mes-hall↗

Picosecond control of quantum dot laser emission by coherent phonons

A picosecond acoustic pulse can be used to control the lasing emission from semiconductor nanostructures by shifting their electronic transitions. When the active medium, here an ensemble of (In,Ga)As quantum dots, is shifted into or out of resonance with the cavity mode, a large enhancement or suppression of the lasing emission can dynamically be achieved. Most interesting, even in the case when gain medium and cavity mode are in resonance, we observe an enhancement of the lasing due to shaking by coherent phonons. In order to understand the interactions of the non-linearly coupled photon-exciton-phonon subsystems, we develop a semiclassical model and find an excellent agreement between theory and experiment.

physics.optics↗

THz lattice vibrations for active plasmonics with light: Ultrafast optical response in gold/telluride hybrid plasmonic crystals

Excitation of coherent optical phonons in solids provides a pathway for ultrafast modulation of light on a sub-ps timescale. Here, we report on efficient 3.6 THz modulation of light reflected from hybrid metal/semiconductor plasmonic crystals caused by lattice vibrations in a few nm thick layer of elemental tellurium. We observe that surface plasmon polaritons contribute significantly to photoinduced formation of this thin layer at the interface between a telluride-based II-VI semiconductor, such as (Cd,Mg)Te or (Cd,Mn)Te, and a one-dimensional gold grating. The change in interface composition is monitored via the excitation and detection of coherent optical tellurium phonons of $A_1$ symmetry by femtosecond laser pulses in a pump-probe experiment. The patterning of a plasmonic grating onto the semiconductor enhances the transient signal which originates from the interface region. This allows monitoring the layer formation and observing the shift of the phonon frequency caused by confinement of the lattice vibrations in the nm-thick segregated layer. Efficient excitation and detection of coherent optical phonons by means of surface plasmon polaritons are evidenced by the dependence of the signal strength on polarization of pump and probe pulses and its spectral distribution.

cond-mat.mtrl-sci↗

Optical measurements of spin noise as a high resolution spectroscopic tool

The intrinsic fluctuations of electron spins in semiconductors and atomic vapors generate a small, randomly-varying "spin noise" that can be detected by sensitive optical methods such as Faraday rotation. Recent studies have demonstrated that the frequency, linewidth, and lineshape of this spin noise directly reveals dynamical spin properties such as dephasing times, relaxation mechanisms and g-factors without perturbing the spins away from equilibrium. Here we demonstrate that spin noise measurements using wavelength-tunable probe light forms the basis of a powerful and novel spectroscopic tool to provide unique information that is fundamentally inaccessible via conventional linear optics. In particular, the wavelength dependence of the detected spin noise power can reveal homogeneous linewidths buried within inhomogeneously-broadened optical spectra, and can resolve overlapping optical transitions belonging to different spin systems. These new possibilities are explored both theoretically and via experiments on spin systems in opposite limits of inhomogeneous broadening (alkali atom vapors and semiconductor quantum dots).

cond-mat.mes-hall↗

Modulation of a surface plasmon-polariton resonance by sub-terahertz diffracted coherent phonons

Coherent sub-THz phonons incident on a gold grating that is deposited on a dielectric substrate undergo diffraction and thereby induce an alteration of the surface plasmon-polariton resonance. This results in efficient high-frequency modulation (up to 110 GHz) of the structure's reflectivity for visible light in the vicinity of the plasmon-polariton resonance. High modulation efficiency is achieved by designing a periodic nanostructure which provides both plasmon-polariton and phonon resonances. Our theoretical analysis shows that the dynamical alteration of the plasmon-polariton resonance is governed by modulation of the slit widths within the grating at the frequencies of higher-order phonon resonances.

cond-mat.mtrl-sci↗

Manifestations of the hyperfine interaction between electron and nuclear spins in singly-charged (In,Ga)As/GaAs quantum dots

The nuclear spin fluctuations (NSF) as well as the dynamic nuclear polarization (DNP) and their effects on the electron spins in negatively charged (In,Ga)As/GaAs quantum dots have been studied by polarized pump-probe and photoluminescence spectroscopy techniques. The effective magnetic field of the NSF is about 30 mT at low excitation power. The NSF distribution becomes highly anisotropic at strong optical excitation by circularly polarized light with periodically alternating helicity. This phenomenon is attributed to a decrease of the nuclear spin entropy due to the hyperfine interaction with polarized electron spins. The DNP is limited to small values for intense, but short photoexcitation.

cond-mat.mes-hall↗