Ultrafast Photocurrent Research Articles

Optical control of ultrafast photocurrent in graphene

Optical control of ultrafast photocurrent in graphene

Femtosecond Drift Photocurrents Generated by an Inversely Designed Plasmonic Antenna.

Photocurrents play a crucial role in various applications, including light detection, photovoltaics, and THz radiation generation. Despite the abundance of methods and materials for converting light into electrical signals, the use of metals in this context has been relatively limited. Nanostructures supporting surface plasmons in metals offer precise light manipulation and induce light-driven electron motion. Through the inverse design optimization of a gold nanostructure, we demonstrate enhanced volumetric, unidirectional, intense, and ultrafast photocurrents via a magneto-optical process derived from the inverse Faraday effect. This is achieved through fine-tuning the amplitude, polarization, and gradients in the local light field. The virtually instantaneous process allows dynamic photocurrent modulation by varying optical pulse duration, potentially yielding nanosources of intense, ultrafast, planar magnetic fields and frequency-tunable THz emission. These findings open avenues for ultrafast magnetic material manipulation and hold promise for nanoscale THz spectroscopy.

Giant Photon‐Drag‐Induced Ultrafast Photocurrent in Diamond for Nonlinear Photonics

AbstractDiamond is emerging as an attractive third‐generation wide‐bandgap semiconductor for future on‐chip nonlinear photonics and quantum optics due to its unique thermal, optical, and mechanical properties. However, the light‐driven current under below‐band gap excitation from the second‐order nonlinear optical effect in diamond is still challenging. Herein, a giant second‐order nonlinear photocurrent is observed in the chemical vapor deposition (CVD) diamond by utilizing terahertz (THz) emission spectroscopy. This ultrafast photocurrent originates from the photon drag effect (PDE), during which the momentum transfer from the incident photons to the charge carriers at the rich grain boundaries of the CVD diamond after the exclusive subgap π–π* transition upon femtosecond laser excitation. Especially, the interplay between circular and linear PDE to the THz generation is clarified and distinguished under elliptically polarized light excitation. Furthermore, the picosecond ultrafast dynamics of these charge carriers are also verified by infrared spectroscopy. Owing to the giant photon‐drag‐induced ultrafast photocurrent, the CVD diamond presents the highest THz emission efficiency compared with the reported carbon allotropes, which expands the new functionality of diamond nonlinear photonics into on‐chip THz devices.

Chirality manipulation of ultrafast phase switches in a correlated CDW-Weyl semimetal

Light engineering of correlated states in topological materials provides a new avenue of achieving exotic topological phases inaccessible by conventional tuning methods. Here we demonstrate a light control of correlation gaps in a model charge-density-wave (CDW) and polaron insulator (TaSe4)2I recently predicted to be an axion insulator. Our ultrafast terahertz photocurrent spectroscopy reveals a two-step, non-thermal melting of polarons and electronic CDW gap via the fluence dependence of a longitudinal circular photogalvanic current. This helicity-dependent photocurrent reveals continuous ultrafast phase switches from the polaronic state to the CDW (axion) phase, and finally to a hidden Weyl phase as the pump fluence increases. Additional distinctive attributes aligning with the light-induced switches include: the mode-selective coupling of coherent phonons to the polaron and CDW modulation, and the emergence of a non-thermal chiral photocurrent above the pump threshold of CDW-related phonons. The demonstrated ultrafast chirality control of correlated topological states here holds large potentials for realizing axion electrodynamics and advancing quantum-computing applications.

High performance broadband photodetector in two-dimensional metal dichalcogenides mediated by topologically protected surface state

Carrier scattering in photodetectors employing 2D dichalcogenide as an absorber impedes carrier transport. As scattering at the interface between the semiconductor and the electrode restricts carrier transport, it is essential to develop alternative electrode materials to achieve high photoresponsivity. A carrier can effectively move through a topologically protected Dirac surface state without scattering: i.e., alternatives such as topological insulators (TI) containing the surface state can effectively reduce scattering at the interface between the semiconductor and the electrode. In this stucy, TI Bi2Se3 with a well-ordered interfacial structure was used as a carrier transport layer (CTL) to effectively employ the topological surface state (TSS) for improving WSe2 photoresponsivity. At 520 nm, the Bi2Se3 TI-CTL photodetector has a photoresponsivity of up to 11.47 AW−1, 100 times higher than the photodevice using only Au electrodes. The photoresponsivity and time-resolved photoluminescence as a function of thickness indicate that TSS contributes to improved carrier separation with high carrier transfer efficiency, thereby affecting photocurrent generation. The fast carrier transfer through TSS helps efficiently separate electron-hole pairs and suppress recombination at the interface, generating ultra-fast and high-efficiency photocurrents in the broadband region (450–1550 nm). Therefore, TSS based on carrier dynamics can lead to further applications of next-generation optoelectronic devices.

Probing the Formation of Dark Interlayer Excitons via Ultrafast Photocurrent.

Optically dark excitons determine a wide range of properties of photoexcited semiconductors yet are hard to access via conventional time-resolved spectroscopies. Here, we develop a time-resolved ultrafast photocurrent technique (trPC) to probe the formation dynamics of optically dark excitons. The nonlinear nature of the trPC makes it particularly sensitive to the formation of excitons occurring at the femtosecond time scale after the excitation. As a proof of principle, we extract the interlayer exciton formation time of 0.4 ps at 160 μJ/cm2 fluence in a MoS2/MoSe2 heterostructure and show that this time decreases with fluence. In addition, our approach provides access to the dynamics of carriers and their interlayer transport. Overall, our work establishes trPC as a technique to study dark excitons in various systems that are hard to probe by other approaches.

Layer‐controlled nonlinear terahertz valleytronics in two‐dimensional semimetal and semiconductor PtSe2

AbstractPlatinum diselenide () is a promising two‐dimensional (2D) material for the terahertz (THz) range as, unlike other transition metal dichalcogenides (TMDs), its bandgap can be uniquely tuned from a semiconductor in the near‐infrared to a semimetal with the number of atomic layers. This gives the material unique THz photonic properties that can be layer‐engineered. Here, we demonstrate that a controlled THz nonlinearity—tuned from monolayer to bulk —can be realized in wafer size polycrystalline through the generation of ultrafast photocurrents and the engineering of the bandstructure valleys. This is combined with the layer interaction with the substrate for a broken material centrosymmetry, permitting a second order nonlinearity. Further, we show layer dependent circular dichroism, where the sign of the ultrafast currents and hence the phase of the emitted THz pulse can be controlled through the excitation of different bandstructure valleys. In particular, we show that a semimetal has a strong dichroism that is absent in the monolayer and few layer semiconducting limit. The microscopic origins of this TMD bandstructure engineering are highlighted through detailed DFT simulations, and shows the circular dichroism can be controlled when becomes a semimetal and when the K‐valleys can be excited. As well as showing that is a promising material for THz generation through layer controlled optical nonlinearities, this work opens up a new class of circular dichroism materials beyond the monolayer limit that has been the case of traditional TMDs, and impacting a range of domains from THz valleytronics, THz spintronics to harmonic generation.image

Space-charge limited and ultrafast dynamics in graphene-based nano-gaps

We show that nano-gaps formed in graphene by utilizing a focused helium ion beam can act as ultrafast photoswitches. By temperature-dependent, time-integrated, and ultrafast photocurrent measurements, we demonstrate that the optoelectronic dynamics across such nano-gaps are dominated by a space-charge limited current in combination with the ultrafast dynamics of hot electrons. The demonstrated methodology allows the creation of ultrafast photoswitches with an amplification gain exceeding the ones as formed by pristine graphene.

Single-molecule photoelectron tunnelling spectroscopy.

Experimental mapping of transmission is essential for understanding and controlling charge transport through molecular devices and materials. Here we developed a single-molecule photoelectron tunnelling spectroscopy approach for mapping transmission beyond the HOMO-LUMO gap of the single diketopyrrolopyrrole molecule junction using an ultrafast-laser combined scanning tunnelling microscope-based break junction set-up at room temperature. Two resonant transport channels of ultrafast photocurrent are found by our photoelectron tunnelling spectroscopy, ranging from 1.31 eV to 1.77 eV, consistent with the LUMO + 1 and LUMO + 2 in the transmission spectrum obtained by density functional theory calculations. Moreover, we observed the modulation of resonant peaks by varying bias voltages, which demonstrates the ability to quantitatively characterize the effect of the electric field on frontier molecular orbitals. Our single-molecule photoelectron tunnelling spectroscopy offers an avenue that allows us to explore the nature of energy-dependent charge transport through single-molecule junctions.

Ultrafast Photocurrent Detection in Low‐Dimensional Materials

Photocurrent generation from photon absorption to electron collection involves various physical processes and reflects the whole life of excited charge carriers. The investigation of photocurrent enables the revelation of fundamental material properties and improvement of electronic device performance. Recently, with the development of ultrafast optics, the time‐resolved photocurrent (TRPC) technique is innovated as a photocurrent detection method with a time resolution down to subpicosecond, which allows exploring the ultrafast carrier dynamics and the photodetector intrinsic response highly efficiently. Herein, the advancement of TRPC studies in low‐dimensional materials is focused on. First, the TRPC technique is first introduced, including the setup composition and its measurement mechanism, and compared with the conventional transport‐based method to demonstrate its uniqueness. Then, the TRPC studies in various low‐dimensional materials including 2D graphene, transition metal dichalcogenides and black phosphorus, 1D nanowires, and 0D nanocrystals are discussed, where the originations of their ultrafast photocurrent are analyzed. Finally, an outlook is given on the research prospects of this powerful technique. The TRPC measurement is highlighted as a significant tool to analyze the ultrafast carrier dynamics in the generation of photocurrent and to instruct the structure design of a new generation of ultrafast photodetectors.

Semiconductor Characterization by Terahertz Excitation Spectroscopy.

Surfaces of semiconducting materials excited by femtosecond laser pulses emit electromagnetic waves in the terahertz (THz) frequency range, which by definition is the 0.1-10 THz region. The nature of terahertz radiation pulses is, in the majority of cases, explained by the appearance of ultrafast photocurrents. THz pulse duration is comparable with the photocarrier momentum relaxation time, thus such hot-carrier effects as the velocity overshoot, ballistic carrier motion, and optical carrier alignment must be taken into consideration when explaining experimental observations of terahertz emission. Novel commercially available tools such as optical parametric amplifiers that are capable of generating femtosecond optical pulses within a wide spectral range allow performing new unique experiments. By exciting semiconductor surfaces with various photon energies, it is possible to look into the ultrafast processes taking place at different electron energy levels of the investigated materials. The experimental technique known as the THz excitation spectroscopy (TES) can be used as a contactless method to study the band structure and investigate the ultrafast processes of various technologically important materials. A recent decade of investigations with the THz excitation spectroscopy method is reviewed in this article. TES experiments performed on the common bulk A3B5 compounds such as the wide-gap GaAs, and narrow-gap InAs and InSb, as well as Ge, Te, GaSe and other bulk semiconductors are reviewed. Finally, the results obtained by this non-contact technique on low-dimensional materials such as ultrathin mono-elemental Bi films, InAs, InGaAs, and GaAs nanowires are also presented.

Nanostructured Ruddlesden–Popper-Layered Lead Bromide Perovskites with Stable and Selected Wavelength for Photodetection Applications

Success in photovoltaic power generation has raised a huge possibility in metal halide perovskites to exhibit excellent photodetection performance with the same physics of photocarrier generation, and their collection at terminal electrodes is employable with less defect-assisted carrier recombination loss. To test this, nanostructured Ruddlesden–Popper (RP)-layered perovskite series were synthesized based on a cyclic organic moiety and Br– halide, resulting in (CH)2(MA)n−1PbnBr3n+1 [where CH─2-(1-cyclohexenyl) ethylamine, MA─methylammonium, Br─bromine, and n = 1–4], to explore how best its mono-to-few layer (n) 2D and quasi 2D-structures can offer photodetection performance with maximum absorbance in the unexplored blue-to-green band gap RP perovskites with maximum stability. Thermogravimetric analysis revealed that the very stable nature of these RP perovskites is accompanied by a linear rise in the structural phase transition temperatures, which range from 270 °C (CH)2PbBr4 (n = 1) to 304 °C (CH)2(MA)3Pb4Br13. The RP perovskites (CH)2(MA)n−1PbnBr3n+1 (n = 1–4) demonstrated sharp exciton emission peaks from blue (∼408 nm) to green (∼528 nm). The X-ray diffraction results confirmed the highly crystalline nature of quasi-2D perovskite thin films. Layer-dependent photoluminescence studies exhibit strong room-temperature exciton photoluminescence and high carrier lifetime. The transient photocurrent measurements for (CH)2(MA)3Pb4Br13 (n = 4) RP perovskite thin films show nearly six times the bias voltage changed from 1 to 5 V at 405 nm laser light excitation. In addition, with respect to performance, the (CH)2(MA)3Pb4Br13 photodetector has shown the highest responsivity (67.2 mA/W), ultrafast transient photocurrent response (122 nA), and high EQE (20.6%) as compared to (CH)2(MA)2Pb3Br10 (n = 3) and (CH)2(MA)Pb2Br7 (n = 2) in ambient temperature.

Generation and Control of Ultrafast Circular Photon Drag Current in Multilayer PtSe2 Revealed Via Terahertz Emission

AbstractThe generation and control of ultrafast photocurrents on the surface of transition‐metal dichalcogenides (TMDs) are essential for the development of advanced optoelectronic devices. A detailed understanding of the mechanism of ultrafast photocurrent generation is primarily needed to design functional devices. Here, it is reported that ultrafast photocurrents in multilayer PtSe2 are induced by the photon drag effect with high conversion efficiency. Particularly, under circularly polarized laser excitation, anisotropic in‐plane photon drag currents are generated, leading to the elliptically polarized terahertz (THz) radiation directly controlled by the helicity of the pump beam. Furthermore, a new model called “THz emission by the circular ac Hall effect” (TECacHE) is proposed to unveil the carrier transport process. It is observed that the origins of elliptically polarized THz emission controlled by helicity involve the pure circular photon drag current and the retardation induced by the Lorentz force. Besides, ultrafast ternary encoding is proposed and demonstrated by polarized THz emission. The results not only provide a new contactless detection model to study surface ultrafast photocurrents but also afford a fundamental investigation of the circular photon drag current in layered TMDs for THz telecommunication devices.

Femtosecond Thermal and Nonthermal Hot Electron Tunneling Inside a Photoexcited Tunnel Junction.

Efficient operation of electronic nanodevices at ultrafast speeds requires understanding and control of the currents generated by femtosecond bursts of light. Ultrafast laser-induced currents in metallic nanojunctions can originate from photoassisted hot electron tunneling or lightwave-induced tunneling. Both processes can drive localized photocurrents inside a scanning tunneling microscope (STM) on femto- to attosecond time scales, enabling ultrafast STM with atomic spatial resolution. Femtosecond laser excitation of a metallic nanojunction, however, also leads to the formation of a transient thermalized electron distribution, but the tunneling of thermalized hot electrons on time scales faster than electron–lattice equilibration is not well understood. Here, we investigate ultrafast electronic heating and transient thermionic tunneling inside a metallic photoexcited tunnel junction and its role in the generation of ultrafast photocurrents in STM. Phase-resolved sampling of broadband terahertz (THz) pulses via the THz-field-induced modulation of ultrafast photocurrents allows us to probe the electronic temperature evolution inside the STM tip and to observe the competition between instantaneous and delayed tunneling due to nonthermal and thermal hot electron distributions in real time. Our results reveal the pronounced nonthermal character of photoinduced hot electron tunneling and provide a detailed microscopic understanding of hot electron dynamics inside a laser-excited tunnel junction.

Group IV THz large area emitter based on GeSn alloy.

THz photoconductive emitters based on III-V materials have demonstrated excellent THz radiation properties, enabling many unique applications. However, the incompatibility with the complementary-metal-oxide-semiconductor (CMOS) foundry fabrication process and the challenging growth condition hampers THz photoconductive emitters from large-scale production. To address this limitation, we proposed the GeSn alloy as the photoconductive material candidate through the CMOS-compatible epitaxy instrument. The GeSn photoconductor features a 518 cm2/V-s mobility and a 7187 cm-1 absorption coefficient at the wavelength of 1560 nm, resulting in sufficiently ultrafast photocurrent generation for THz radiation. As a result, the GeSn THz emitter provides over a bandwidth of 2 THz and a 40 dB signal-to-noise ratio, which shows its potential in realizing mass-producible, cost-effective THz integrated systems with CMOS technology.

(Invited) Controlling Interlayer Stacking Configuration to Optimize Exciton Extraction Pathways in Van Der Waals Materials

Employing ultrafast microscopy methods, we demonstrate how tuning the interlayer coupling by twisting stacking orientations results in different metastable electronic states like Moiré excitons in twisted bilayer graphene (tBLG) and bound triplet pairs (TT) in molecular crystals. Considering first tBLG, we show how stacking-angle tunable absorption resonances form a strongly-bound exciton state due to the interlayer orbitals' symmetric rehybridization. Using two-photon photoluminescence and intraband-transient absorption (TA) microscopies, we have imaged the photoemission and exciton dynamics from single-grains of tBLG. After resonant excitation, our results suggest the formation of strongly bound (up to 690 meV), metastable interlayer exciton states.[1] Our observation of resonant PL emission from twisted bilayer graphene materials is best explained by the theoretically predicted coexistence of strongly bound interlayer excitons and metallic graphene continuum states to form Moiré excitons.Unlike stacked graphene, semiconducting 2D transition metal dichalcogenides (TMDCs) have diffuse interlayer d-orbital overlap. To enhance interlayer electronic coupling in TMDCs, we apply an interlayer-directed E-field, inducing electron-hole dissociation as shown in Fig. 1b. Time-resolved photocurrents show that stacked WSe2 devices shown in Fig. 1a can have both IQE >50% and fast (<60 ps) picosecond electron escape times. Our ultrafast photocurrent rates kinetics give the same E-field-dependent electronic escape and dissociation rates seen from ultrafast optical TA microscopy.[2] To rationalize these fast electronic escape rates, we show the ratio of the electronic rates accurately predicts the actual WSe2 device photocurrent generation efficiency. Lastly, we will show how certain intermolecular twist angle packings of athraditiophene molecular crystals make electron-multiplication by singlet fission of TT states favorable. Singlet fission dynamics are indicated in Fig. 1c by the matching singlet (blue) vs. rising triplet dynamics (red) obtained when the probe polarization aligned along the crystal charge-transfer axis. However, other intermolecular packing angles (at 90o) instead localize and trap excitons as excimers, preventing singlet fission.[3] These interlayer stacked systems collectively demonstrate how remarkably different interlayer electronic states evolve from relatively small changes in interlayer twist angles in van der Waals stacked materials and molecular singlet fission materials.

Bias-free terahertz generation from a silicon-compatible photoconductive emitter operating at telecommunication wavelengths

We present a telecommunication-compatible bias-free photoconductive terahertz emitter composed of a bilayer InAs structure directly grown on a high-resistivity silicon substrate. The bilayer InAs structure includes p+-doped and undoped InAs layers, inducing a strong built-in electric field that enables terahertz generation without requiring any external bias voltage. A large-area plasmonic nanoantenna array is used to enhance and confine optical generation inside the photoconductive region with the highest built-in electric field, leading to the generation of a strong ultrafast photocurrent and broadband terahertz radiation. Thanks to a higher terahertz transmission through the silicon substrate and a shorter carrier lifetime in the InAs layers grown on silicon, higher signal-to-noise ratios are achieved at high terahertz frequencies compared with previously demonstrated bias-free terahertz emitters realized on GaAs. In addition to compatibility with silicon integrated optoelectronic platforms, the presented bias-free photoconductive emitter provides more than a 6 THz radiation bandwidth with more than 100 dB dynamic range when used in a terahertz time-domain spectroscopy system.

Generating and Capturing Secondary Hot Carriers in Monolayer Tungsten Dichalcogenides.

It remains challenging to capture and investigate the drift dynamics of primary hot carriers because of their ultrashort lifetime (∼200 fs). Here we report a new mechanism for secondary hot carrier (∼25 ps) generation in monolayer transition metal dichalcogenides such as WS2 and WSe2, triggered by the Auger recombination of trions and biexcitons. Using ultrafast photocurrent spectroscopy, we measured and characterized the photocurrent stemming from the Auger recombination of trions and biexcitons in WS2 and WSe2. A mobility of 0.24 cm2 V-1 s-1 and a drift length of ∼3.8 nm were found for the secondary hot carriers in WS2. By leveraging interactions between exciton complexes, we envision a new mechanism for generating and controlling hot carriers, which could lead to efficient devices in photophysics, photochemistry, and photosynthesis.

Manipulating Picosecond Photoresponse in van der Waals Heterostructure Photodetectors

AbstractSelf‐powered ultrafast 2D photodetectors have demonstrated great potential in imaging, sensing, and communication. Understanding the intrinsic ultrafast charge carrier generation and separation processes is essential for achieving high‐performance devices. However, probing and manipulating the ultrafast photoresponse is limited either by the temporal resolution of the conventional methods or the required sophisticated device configurations. Here, van der Waals heterostructure photodetectors are constructed based on MoS2/WSe2 p–n and n–n junctions and manipulate the picosecond photoresponse by combining photovoltaic (PV) and photothermoelectric (PTE) effects. Taking time‐resolved photocurrent (TRPC) measurements, a TRPC peak at zero time delay is observed with decay time down to 4 ps in the n–n junction device, in contrast to the TRPC dip in the p–n junction and pure WSe2 devices, indicating an opposite current polarity between PV and PTE. More importantly, with an ultrafast photocurrent modulation, a transition from a TRPC peak to a TRPC dip is realized, and detailed carrier transport dynamics are analyzed. This study provides a deeper understanding of the ultrafast photocurrent generation mechanism in van der Waals heterostructures and offers a new perspective in instruction for designing more efficient self‐powered photodetectors.

Coherent injection photocurrent in bismuth sulfide film induced by one-plus-two photon absorption quantum interference.

Quantum interference (QuI) effect is a powerful method to generate and control the ultrafast photocurrent in semiconductors. We utilize two-color pulsed light excitation in bismuth sulfide (Bi2S3) film to induce the photocurrent through the QuI effect. Experimentally, the photocurrent is indirectly monitored using a standard terahertz (THz) time-domain spectroscopic system. Due to the QuI, an asymmetric photon injection occurs in Bi2S3 film, resulting in coherent injection current and subsequently THz wave generation. Our results on the pump pulse energy dependence of the THz electric field suggests that the THz wave generation process follows the third-order nonlinear optical process.