arXiv subjects

Kirill I. Bolotin

Publications and source records attributed to Kirill I. Bolotin.

At least 37 records · Page 2Linked to original sources

arXiv2021

Spin/valley coupled dynamics of electrons and holes at the ${\text{MoS}_{2}-\text{MoSe}_{2}}$ interface

The coupled spin and valley degrees of freedom in transition metal dichalcogenides (TMDs) are considered a promising platform for information processing. Here, we use a TMD heterostructure ${\text{MoS}_{2}-\text{MoSe}_{2}}$ to study optical pumping of spin/valley polarized carriers across the interface and to elucidate the mechanisms governing their subsequent relaxation. By applying time-resolved Kerr and reflectivity spectroscopies, we find that the photoexcited carriers conserve their spin for both tunneling directions across the interface. Following this, we measure dramatically different spin/valley depolarization rates for electrons and holes, $\sim 30\,{\text{ns}}^{-1}$ and $< 1\,{\text{ns}}^{-1}$, respectively and show that this difference relates to the disparity in the spin-orbit splitting in conduction and valence bands of TMDs. Our work provides insights into the spin/valley dynamics of free carriers unaffected by complex excitonic processes and establishes TMD heterostructures as generators of spin currents in spin/valleytronic devices.

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arXiv2021

Tunable graphene phononic crystal

In the field of phononics, periodic patterning controls vibrations and thereby the flow of heat and sound in matter. Bandgaps arising in such phononic crystals realize low-dissipation vibrational modes and enable applications towards mechanical qubits, efficient waveguides, and state-of-the-art sensing. Here, we combine phononics and two-dimensional materials and explore the possibility of manipulating phononic crystals via applied mechanical pressure. To this end, we fabricate the thinnest possible phononic crystal from monolayer graphene and simulate its vibrational properties. We find a bandgap in the MHz regime, within which we localize a defect mode with a small effective mass of 0.72 ag = 0.002 $m_{physical}$. Finally, we take advantage of graphene's flexibility and mechanically tune a finite size phononic crystal. Under electrostatic pressure up to 30 kPa, we observe an upshift in frequency of the entire phononic system by more than 350%. At the same time, the defect mode stays within the bandgap and remains localized, suggesting a high-quality, dynamically tunable mechanical system.

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arXiv2020

Ultrafast photocurrents in MoSe$_2$ probed by terahertz spectroscopy

We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe$_2$. We identify several distinct mechanisms producing THz radiation in response to an ultrashort ($30\,$fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscillations at about $23\,$THz in the emission from the BL sample. We attribute the oscillations to quantum beats between two excitonic states with energetic separation of $\sim100\,$meV.

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arXiv2020

In situ functionalization of graphene

While the basal plane of graphene is inert, defects in it are centers of chemical activity. An attractive application of such defects is towards controlled functionalization of graphene with foreign molecules. However, the interaction of the defects with reactive environment, such as ambient, decreases the efficiency of functionalization and makes it poorly controlled. Here, we report a novel approach to generate, monitor with time resolution, and functionalize the defects $\textit{in situ}$ without ever exposing them to the ambient. The defects are generated by an energetic Argon plasma and their properties are monitored using $\textit{in situ}$ Raman spectroscopy. We find that these defects are functional, very reactive, and strongly change their density from $\approx 1\cdot10^{13} cm^{-2}$ to $\approx 5\cdot10^{11} cm^{-2}$ upon exposure to air. We perform the proof of principle $\textit{in situ}$ functionalization by generating defects using the Argon plasma and functionalizing them $\textit{in situ}$ using Ammonia functional. The functionalization induces the n-doping with a carrier density up to $5\cdot10^{12} cm^{-2}$ in graphene and remains stable in ambient conditions.

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arXiv2020

Giant Tunable Mechanical Nonlinearity in Graphene-Silicon Nitride Hybrid Resonator

High quality factor mechanical resonators have shown great promise in developing classical or quantum technologies. Simultaneously, progress has been made in developing controlled mechanical nonlinearity. Here we combine these two directions of progress in a single platform consisting of coupled Silicon Nitride (SiNx) and graphene mechanical resonators. We show that nonlinear response can be induced on a large area SiNx resonator mode and can be efficiently controlled by coupling it to a gate-tunable, freely suspended graphene mode. The induced nonlinear response of the hybrid modes, as measured on the SiNx resonator surface is giant, with one of the highest measured Duffing constants. We observe a novel phononic frequency comb which we use as an alternate validation of the measured values, along with numerical simulations which are in overall agreement with measurements.

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arXiv2020

Limits of funneling efficiency in non-uniformly strained 2D semiconductors

Photoexcited electron-hole pairs (excitons) in transition metal dichalcogenides (TMDC) experience an effective force when these materials are non-uniformly strained. In the case of strain produced by a sharp tip pressing at the center of a suspended TMDC membrane, the excitons are transported to the point of the highest strain at the center of the membrane. This effect, exciton funneling, can be used to increase photoconversion efficiency in TMDC, to explore exciton transport, and to study correlated states of excitons arising at their high densities. Here, we analyze the limits of funneling efficiency in realistic device geometries. The funneling efficiency in realistic monolayer TMDCs is found to be low, $ <5 \;\%$ both at room and low temperatures. This results from dominant diffusion at room temperature and short exciton lifetimes at low temperatures. On the other hand, in TMDC heterostructures with long exciton lifetimes the funneling efficiency reaches $\sim 50\;\%$ at room temperature, as the exciton density reaches thermal equilibrium in the funnel. Finally, we show that Auger recombination limits funneling efficiency for intense illumination sources.

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arXiv2020

Neutral and charged excitons interplay in non-uniformly strain-engineered WS$_2$

We investigate the response of excitons in two-dimensional semiconductors subjected to controlled non-uniform strain fields. In our approach to non-uniform strain-engineering, a WS$_2$ monolayer is suspended over a triangular hole. Large ($>2\;\%$), strongly non-uniform ($>0.28\;\%/μm$), and in-situ tunable strain is induced in the monolayer by pressurizing it with inert gas. We observe peak shifts and spectral shape changes in the photoluminescence spectra of strained WS$_2$. We interpret these changes as a signature of increased free electron density and resulting conversion of neutral excitons to trions in the region of high strain. Our result establishes non-uniform strain engineering as a novel and useful experimental `knob' for tuning optoelectronic properties of 2D semiconductors.

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arXiv2019

Intrinsic and Extrinsic Defect-related Excitons in TMDCs

We investigate an excitonic peak appearing in low-temperature photoluminescence of monolayer transition metal dichalcogenides (TMDCs), which is commonly associated with defects and disorder. First, to uncover the intrinsic origin of defect-related excitons, we study their dependence on gate voltage, excitation power, and temperature in a prototypical TMDC monolayer, $MoS_2$. We show that the entire range of behaviors of defect-related excitons can be understood in terms of a simple model, where neutral excitons are bound to ionized donor levels, likely related to sulphur vacancies, with a density of $7\cdot10^{11} cm^{-2}$. Second, to study the extrinsic origin of defect-related excitons, we controllably deposit oxygen molecules in-situ onto the surface of $MoS_2$ kept at cryogenic temperature. We find that in addition to trivial p-doping of $3\cdot10^{12} cm^{-2}$, oxygen affects the formation of defect-related excitons by functionalizing the vacancy. Combined, our results uncover the origin of defect-related excitons, suggest a simple and conclusive approach to track the functionalization of TMDCs, benchmark device quality, and pave the way towards exciton engineering in hybrid organic-inorganic TMDC devices.

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arXiv2019

Dynamics and efficient conversion of excitons to trions in non-uniformly strained monolayer WS$_2$

We investigate the transport of excitons and trions in monolayer semiconductor WS$_2$ subjected to controlled non-uniform mechanical strain. We actively control and tune the strain profiles with an AFM-based setup in which the monolayer is indented by an AFM tip. Optical spectroscopy is used to reveal the dynamics of the excited carriers. The non-uniform strain configuration locally changes the valence and conduction bands of WS$_2$, giving rise to effective forces attracting excitons and trions towards the point of maximum strain underneath the AFM tip. We observe large changes in the photoluminescence spectra of WS$_2$ under strain, which we interpret using a drift-diffusion model. We show that the transport of neutral excitons, a process that was previously thought to be efficient in non-uniformly strained 2D semiconductors and termed as "funneling", is negligible at room temperature in contrast to previous observations. Conversely, we discover that redistribution of free carriers under non-uniform strain profiles leads to highly efficient conversion of excitons to trions. Conversion efficiency reaches $\simeq 100\%$ even without electrical gating. Our results explain inconsistencies in previous experiments and pave the way towards new types of optoelectronic devices.

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arXiv2017

Hidden area and mechanical nonlinearities in freestanding graphene

We investigated the effect of out-of-plane crumpling on the mechanical response of graphene membranes. In our experiments, stress was applied to graphene membranes using pressurized gas while the strain state was monitored through two complementary techniques: interferometric profilometry and Raman spectroscopy. By comparing the data obtained through these two techniques, we determined the geometric hidden area which quantifies the crumpling strength. While the devices with hidden area $\sim0~\%$ obeyed linear mechanics with biaxial stiffness $428\pm10$ N/m, specimens with hidden area in the range $0.5-1.0~\%$ were found to obey an anomalous Hooke's law with an exponent $\sim0.1$.

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arXiv2017

Controlled dynamic screening of excitonic complexes in 2D semiconductors

We report a combined theoretical/experimental study of dynamic screening of excitons in media with frequency-dependent dielectric functions. We develop an analytical model showing that interparticle interactions in an exciton are screened in the range of frequencies from zero to the characteristic binding energy depending on the symmetries and transition energies of that exciton. The problem of the dynamic screening is then reduced to simply solving the Schrodinger equation with an effectively frequency-independent potential. Quantitative predictions of the model are experimentally verified using a test system: neutral, charged and defect-bound excitons in two-dimensional monolayer WS2, screened by metallic, liquid, and semiconducting environments. The screening-induced shifts of the excitonic peaks in photoluminescence spectra are in good agreement with our model.

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arXiv2016

Nonlinear optical conductivity of a generic two band systems, with application to doped and gapped graphene

We present a general formulation to calculate the dynamic optical conductivity, beyond the linear response regime, of any electronic system whose quasiparticle dispersion is described by a two band model. Our phenomenological model is based on the optical Bloch equations. In the steady state regime it yields an analytic solution for the population inversion and the interband coherence, which are nonlinear in the optical field intensity, including finite doping and temperature effects. We explicitly show that the optical nonlinearities are controlled by a single dimensionless parameter which is directly proportional to the incident field strength and inversely proportional to the optical frequency. This identification leads to a unified way to study the dynamical conductivity and the differential transmission spectrum across a wide range of optical frequencies, and optical field strength. We use our formalism to analytically calculate the nonlinear optical conductivity of doped and gapped graphene, deriving the well known universal ac conductivity of $σ_0={e^2}/4\hbar$ in the linear response regime of low optical intensities (or equivalently high frequencies) and non-linear deviations from it which appear at high laser intensities (or low frequencies) including the impact of finite doping and band-gap opening.

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arXiv2015

The Effect of Intrinsic Crumpling on the Mechanics of Free-Standing Graphene

Free-standing graphene is inherently crumpled in the out-of-plane direction due to dynamic flexural phonons and static wrinkling. We explore the consequences of this crumpling on the effective mechanical constants of graphene. We develop a sensitive experimental approach to probe stretching of graphene membranes under low applied stress at cryogenic to room temperatures. We find that the in-plane stiffness of graphene is between 20 and 100 N/m at room temperature, much smaller than 340 N/m (the value expected for flat graphene). Moreover, while the in-plane stiffness only increases moderately when the devices are cooled down to 10 K, it approaches 300 N/m when the aspect ratio of graphene membranes is increased. These results indicate that softening of graphene at temperatures less than 400 K is caused by static wrinkling, with only a small contribution due to flexural phonons. Together, these results explain the large variation in reported mechanical constants of graphene devices and paves the way towards controlling their mechanical properties.

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arXiv2015

Electrical control of near-field energy transfer between quantum dots and 2D semiconductors

We investigate near-field energy transfer between chemically synthesized quantum dots (QDs) and two-dimensional semiconductors. We fabricate devices in which electrostatically gated semiconducting monolayer molybdenum disulfide (MoS2) is placed atop a homogenous self-assembled layer of core-shell CdSSe QDs. We demonstrate efficient non-radiative Förster resonant energy transfer (FRET) from QDs into MoS2 and prove that modest gate-induced variation in the excitonic absorption of MoS2 lead to large (~500%) changes in the FRET rate. This, in turn, allows for up to ~75% electrical modulation of QD photoluminescence intensity. The hybrid QD/MoS2 devices operate within a small voltage range, allow for continuous modification of the QD photoluminescence intensity, and can be used for selective tuning of QDs emitting in the visible-IR range.

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arXiv2013

High-Field Electrical and Thermal Transport in Suspended Graphene

We study the intrinsic transport properties of suspended graphene devices at high fields (>1 V/um) and high temperatures (>1000 K). Across 15 samples, we find peak (average) saturation velocity of 3.6x10^7 cm/s (1.7x10^7 cm/s), and peak (average) thermal conductivity of 530 W/m/K (310 W/m/K), at 1000 K. The saturation velocity is 2-4 times and the thermal conductivity 10-17 times greater than in silicon at such elevated temperatures. However, the thermal conductivity shows a steeper decrease at high temperature than in graphite, consistent with stronger effects of second-order three-phonon scattering. Our analysis of sample-to-sample variation suggests the behavior of "cleaner" devices most closely approaches the intrinsic high-field properties of graphene. This study reveals key features of charge and heat flow in graphene up to device breakdown at ~2230 K in vacuum, highlighting remaining unknowns under extreme operating conditions.

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arXiv2013

Bandgap Engineering of Strained Monolayer and Bilayer MoS2

We report the influence of uniaxial tensile mechanical strain in the range 0-2.2% on the phonon spectra and bandstructures of monolayer and bilayer molybdenum disulfide (MoS2) two-dimensional crystals. First, we employ Raman spectroscopy to observe phonon softening with increased strain, breaking the degeneracy in the E' Raman mode of MoS2, and extract a Grüneisen parameter of ~1.06. Second, using photoluminescence spectroscopy we measure a decrease in the optical band gap of MoS2 that is roughly linear with strain, ~45 meV% strain for monolayer MoS2 and ~120 meV% strain for bilayer MoS2. Third, we observe a pronounced strain-induced decrease in the photoluminescence intensity of monolayer MoS2 that is indicative of the direct-to-indirect transition of the character of the optical band gap of this material at applied strain of ~1.5%, a value supported by first-principles calculations that include excitonic effects. These observations constitute the first demonstration of strain engineering the band structure in the emergent class of two-dimensional crystals, transition-metal dichalcogenides.

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arXiv2012

Probing charge scattering mechanisms in suspended graphene by varying its dielectric environment

Graphene with high carrier mobility μ is required both for graphene-based electronic devices and for the investigation of the fundamental properties of graphene's Dirac fermions. It is largely accepted that the mobility-limiting factor in graphene is the Coulomb scattering off of charged impurities that reside either on graphene or in the underlying substrate. This is true both for traditional graphene devices on SiO2 substrates and possibly for the recently reported high-mobility suspended and supported devices. An attractive approach to reduce such scattering is to place graphene in an environment with high static dielectric constant κ that would effectively screen the electric field due to the impurities. However, experiments so far report only a modest effect of high-κ environment on mobility. Here, we investigate the effect of the dielectric environment of graphene by studying electrical transport in multi-terminal graphene devices that are suspended in liquids with κ ranging from 1.9 to 33. For non-polar liquids (κ<5) we observe a rapid increase of μ with κ and report a record room-temperature mobility as large as ~60,000 cm2/Vs for graphene devices in anisole (κ=4.3), while in polar liquids (κ>18) we observe a drastic drop in mobility. We demonstrate that non-polar liquids enhance mobility by screening charged impurities adsorbed on graphene, while charged ions in polar liquids cause the observed mobility suppression. Furthermore, using molecular dynamics simulation we establish that scattering by out-of-plane flexural phonons, a dominant scattering mechanism in suspended graphene in vacuum at room temperature, is suppressed by the presence of liquids. We expect that our findings may provide avenues to control and reduce carrier scattering in future graphene-based electronic devices.

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arXiv2009

Observation of the Fractional Quantum Hall Effect in Graphene

When electrons are confined in two dimensions and subjected to strong magnetic fields, the Coulomb interactions between them become dominant and can lead to novel states of matter such as fractional quantum Hall liquids. In these liquids electrons linked to magnetic flux quanta form complex composite quasipartices, which are manifested in the quantization of the Hall conductivity as rational fractions of the conductance quantum. The recent experimental discovery of an anomalous integer quantum Hall effect in graphene has opened up a new avenue in the study of correlated 2D electronic systems, in which the interacting electron wavefunctions are those of massless chiral fermions. However, due to the prevailing disorder, graphene has thus far exhibited only weak signatures of correlated electron phenomena, despite concerted experimental efforts and intense theoretical interest. Here, we report the observation of the fractional quantum Hall effect in ultraclean suspended graphene, supporting the existence of strongly correlated electron states in the presence of a magnetic field. In addition, at low carrier density graphene becomes an insulator with an energy gap tunable by magnetic field. These newly discovered quantum states offer the opportunity to study a new state of matter of strongly correlated Dirac fermions in the presence of large magnetic fields.

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