Kenan Gundogdu

Two-Quantum 2D FT Electronic Spectroscopy of Biexcitons in GaAs Quantum Wells

Seeing Double Whereas electrons roam free in a metal, their motion in a semiconductor often correlates with that of the positively charged holes their excitation has left behind. Various spectroscopic techniques have quantified the energetics associated with such electron-hole pairs, termed excitons. However, the higher-order correlations that ensue from exciton-exciton interactions are harder to probe. Now, Stone et al. (p. 1169) have characterized the dynamics of such exciton pairs, or biexcitons, directly in a gallium arsenide quantum well structure using a sequence of four ultrashort optical pulses with precisely controlled mutual phase relationships. Controlling the phase and timing of four optical pulses enables measurement of correlations between the electronic semiconductor carriers. The motions of electrons in solids may be highly correlated by strong, long-range Coulomb interactions. Correlated electron-hole pairs (excitons) are accessed spectroscopically through their allowed single-quantum transitions, but higher-order correlations that may strongly influence electronic and optical properties have been far more elusive to study. Here we report direct observation of bound exciton pairs (biexcitons) that provide incisive signatures of four-body correlations among electrons and holes in gallium arsenide (GaAs) quantum wells. Four distinct, mutually coherent, ultrashort optical pulses were used to create coherent exciton states, transform these successively into coherent biexciton states and then new radiative exciton states, and finally to read out the radiated signals, yielding biexciton binding energies through a technique closely analogous to multiple-quantum two-dimensional Fourier transform (2D FT) nuclear magnetic resonance spectroscopy. A measured variation of the biexciton dephasing rate indicated still higher-order correlations.

Efficient Charge Transfer and Fine-Tuned Energy Level Alignment in a THF-Processed Fullerene-Free Organic Solar Cell with 11.3% Efficiency.

Fullerene-free organic solar cells show over 11% power conversion efficiency, processed by low toxic solvents. The applied donor and acceptor in the bulk heterojunction exhibit almost the same highest occupied molecular orbital level, yet exhibit very efficient charge creation.

Non-magnetic semiconductor spin transistor

We propose a spin transistor using only nonmagnetic materials that exploits the characteristics of bulk inversion asymmetry~BIA ! in ~110! symmetric quantum wells. We show that extremely large spin splittings due to BIA are possible in ~110! InAs/GaSb/AlSb heterostructures, which together with the enhanced spin decay times in ~110! quantum wells demonstrates the potential for exploitation of BIA effects in semiconductor spintronics devices. Spin injection and detection is achieved using spin-dependent resonant interband tunneling and spin transistor action is realized through control of the electron spin lifetime in an InAs lateral transport channel using an applied electric field ~Rashba effect !. This device may also be used as a spin valve, or a magnetic field sensor. ©2003 American Institute of Physics. @DOI: 10.1063/1.1609656 #

A near-infrared non-fullerene electron acceptor for high performance polymer solar cells

Low-bandgap polymers/molecules are an interesting family of semiconductor materials, and have enabled many recent exciting breakthroughs in the field of organic electronics, especially for organic photovoltaics (OPVs). Here, such a low-bandgap (1.43 eV) non-fullerene electron acceptor (BT-IC) bearing a fused 7-heterocyclic ring with absorption edge extending to the near-infrared (NIR) region was specially designed and synthesized. Benefitted from its NIR light harvesting, high performance OPVs were fabricated with medium bandgap polymers (J61 and J71) as donors, showing power conversion efficiencies of 9.6% with J61 and 10.5% with J71 along with extremely low energy loss (0.56 eV for J61 and 0.53 eV for J71). Interestingly, femtosecond transient absorption spectroscopy studies on both systems show that efficient charge generation was observed despite the fact that the highest occupied molecular orbital (HOMO)–HOMO offset (ΔEH) in the blends was as low as 0.10 eV, suggesting that such a small ΔEH is not a crucial limitation in realizing high performance of NIR non-fullerene based OPVs. Our results indicated that BT-IC is an interesting NIR non-fullerene acceptor with great potential application in tandem/multi-junction, semitransparent, and ternary blend solar cells.

Ultrafast electron capture into p-modulation-doped quantum dots

Electron and hole relaxation kinetics are studied in modulation-doped InAs quantum dots using femtosecond time-resolved photoluminescence experiments. We demonstrate that, as a result of doping, carrier relaxation from the barrier layers to the quantum dot ground states is strongly enhanced due to rapid electron–hole scattering involving the built-in carrier population. Results for p-doped quantum dots reveal a threefold decrease in the room-temperature electron relaxation time relative to corresponding undoped quantum dots. Our findings are promising for the development of high-speed, GaAs-based quantum dot lasers with modulation speeds in excess of 30GHz.Electron and hole relaxation kinetics are studied in modulation-doped InAs quantum dots using femtosecond time-resolved photoluminescence experiments. We demonstrate that, as a result of doping, carrier relaxation from the barrier layers to the quantum dot ground states is strongly enhanced due to rapid electron–hole scattering involving the built-in carrier population. Results for p-doped quantum dots reveal a threefold decrease in the room-temperature electron relaxation time relative to corresponding undoped quantum dots. Our findings are promising for the development of high-speed, GaAs-based quantum dot lasers with modulation speeds in excess of 30GHz.

Three-dimensional electronic spectroscopy of excitons in GaAs quantum wells

We demonstrate three-dimensional (3D) electronic Fourier transform spectroscopy of GaAs quantum wells using four fully phase-coherent, noncollinear optical fields. Since the full complex signal field is measured as a function of all three time intervals, nearly every peak in the resulting 3D spectral solid arises from a distinguishable sequence of transitions represented by a single Feynman pathway. We use the 3D spectral peaks to separate two pathways involving weakly bound mixed biexcitons generated in different time orders. In the process, we reveal a peak that was previously obscured by a correlated but unbound exciton pair coherence. We also demonstrate a calibration procedure for the carrier frequency which yields biexciton binding energy values with high accuracy.

Invited Article: The coherent optical laser beam recombination technique (COLBERT) spectrometer: Coherent multidimensional spectroscopy made easier

We have developed an efficient spectrometer capable of performing a wide variety of coherent multidimensional measurements at optical wavelengths. The two major components of the largely automated device are a spatial beam shaper which controls the beam geometry and a spatiotemporal pulse shaper which controls the temporal waveform of the femtosecond pulse in each beam. We describe how to construct, calibrate, and operate the device, and we discuss its limitations. We use the exciton states of a semiconductor nanostructure as a working example. A series of complex multidimensional spectra-displayed in amplitude and real parts-reveals increasingly intricate correlations among the excitons.

Exciton valley relaxation in a single layer ofWS2measured by ultrafast spectroscopy

We measured the lifetime of optically created valley polarization in single layer WS2 using transient absorption spectroscopy. The electron valley relaxation is very short (< 1ps). However the hole valley lifetime is at least two orders of magnitude longer and exhibits a temperature dependence that cannot be explained by single carrier spin/valley relaxation mechanisms. Our theoretical analysis suggests that a collective contribution of two potential processes may explain the valley relaxation in single layer WS2. One process involves direct scattering of excitons from K to K ′ valleys with a spin flip-flop interaction. The other mechanism involves scattering through spin degenerate Γ valley. This second process is thermally activated with an Arrhenius behavior due to the energy barrier between Γ and K valleys. PACS numbers: 73.21.-b, 78.47.j-,71.35.-y 1 ar X iv :1 40 5. 51 41 v1 [ co nd -m at .m tr lsc i] 2 0 M ay 2 01 4

Excited-state dynamics and carrier capture in InGaAs/GaAs quantum dots

Subpicosecond time-resolved photoluminescence upconversion is used to measure the 12 K first-excited-state dynamics in large InGaAs/GaAs self-assembled quantum dots designed for 1.3 μm diode lasers. A comparison with the ground-state dynamics suggests that energy relaxation occurs in a cascade through the multiple discrete levels with an average interlevel relaxation time of ∼250 fs. Excited-state emission is observed from two distinct populations. Due to the ultrafast relaxation from the excited state to the ground state in dots containing only a single exciton, the excited-state emission is dominated by the fraction of dots that capture more than one electron–hole pair. In this case, state filling in the ground state blocks the ultrafast relaxation channel, thereby enhancing the excited-state emission. While state filling and a random capture process dictate the primary features of the excited-state emission, at low excitation levels we find that the rise time of emission from the excited state is influ...

Fundamental limits of exciton-exciton annihilation for light emission in transition metal dichalcogenide monolayers

We quantitatively evaluate the exciton-exciton annihilation (EEA) and its effect on light emission properties in monolayer TMDC materials, including WS2, MoS2, and WSe2. The EEA rate is found to be 0.3 cm2/s and 0.1 cm2/s for suspended WS2 and MoS2 monolayers, respectively, and subject to the influence from substrates, being 0.1 cm2/s and 0.05 cm2/s for the supported WS2 and MoS2 on sapphire substrates. It can substantially affect the luminescence efficiency of suspended monolayers even at an exciton concentration as low as 109 cm-2, but plays a milder role for supported monolayers due to the effect of the substrate. However, regardless the presence of substrates or not, the lasing threshold of the monolayer is always predominantly determined by the EEA, which is estimated to be 12-18 MW/cm2 if using 532 nm as the pumping wavelength.