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Dielectric control of ultrafast carrier dynamics and transport in graphene
Authors:
Hai I. Wang,
Xiaoyu Jia,
Anand Nivedan,
Mischa Bonn,
Aron W. Cummings,
Alessandro Principi,
Klaas-Jan Tielrooij
Abstract:
Understanding the ultrafast dynamics of photoexcited charges in graphene is essential, as the microscopic mechanisms underlying these dynamics determine many of graphene's optical, optothermal, and optoelectronic properties. These are crucial properties for many functionalities and devices enabled by graphene, such as high-speed photodectors. Therefore, beyond scientific understanding, it is highl…
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Understanding the ultrafast dynamics of photoexcited charges in graphene is essential, as the microscopic mechanisms underlying these dynamics determine many of graphene's optical, optothermal, and optoelectronic properties. These are crucial properties for many functionalities and devices enabled by graphene, such as high-speed photodectors. Therefore, beyond scientific understanding, it is highly desirable to control ultrafast carrier dynamics for practical applications. Here, we establish this control by engineering the dielectric environment of graphene, thereby regulating both heating and cooling dynamics without altering the Fermi energy, optical power, or ambient temperature. By combining optical pump-terahertz probe experiments with theoretical calculations, we show that dielectric screening suppresses carrier-carrier interactions and slows the dynamics. In particular, reduced carrier-carrier scattering delays the formation of a quasi-equilibrium hot electron distribution, thus slowing carrier heating. It also slows carrier cooling because re-thermalization after optical-phonon emission depends on the same interactions. The enhanced screening further reduces the energy of electron-hole puddles, thereby increasing charge mobility and the Seebeck coefficient. This ability to externally control internal graphene dynamics and transport properties enables the optimization of device performance, such as the sensitivity of photodetectors for data communication and wireless communication applications.
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Submitted 31 March, 2026;
originally announced April 2026.
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Observation of a phonon bottleneck effect on the thermal depopulation from a photoexcited shallow defect in silicon
Authors:
Sergio Revuelta,
Hai I. Wang,
Mischa Bonn,
Enrique Canovas
Abstract:
We report the observation of a phonon bottleneck effect impacting the thermal depopulation of photoexcited shallow defects in high-resistivity silicon. Using time-resolved terahertz (THz) spectroscopy, near-band-gap excitation produces a pronounced temporal delay in photoconductivity, indicating that a fraction of photogenerated charge carriers is temporarily trapped immediately after excitation.…
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We report the observation of a phonon bottleneck effect impacting the thermal depopulation of photoexcited shallow defects in high-resistivity silicon. Using time-resolved terahertz (THz) spectroscopy, near-band-gap excitation produces a pronounced temporal delay in photoconductivity, indicating that a fraction of photogenerated charge carriers is temporarily trapped immediately after excitation. By analyzing the frequency-resolved complex photoconductivity as a function of pump-probe delay and photon energy, we attribute this delay to the presence of a localized shallow state situated approximately 40 meV from the band edge, which competes with silicon's indirect band-to-band absorption. The zero-order kinetic profile of the temporal delay, its invariance with respect to photon flux, and its temperature dependence collectively support the existence of a phonon bottleneck that hinders the thermal release of electrons from this shallow trap. this represents experimental evidence of a phonon bottleneck effect associated with the thermal activation of shallow traps in photoexcited silicon. These findings provide microscopic insight into carrier relaxation dynamics in silicon and highlight the significance of electron-phonon interactions in the ultrafast processes governing materials used in optoelectronic applications.
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Submitted 24 November, 2025;
originally announced November 2025.
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Itinerant Orbital Hall Effect Mechanism Leading to Large Negative Orbital Torques from Light Metal Vanadium
Authors:
Nikhil Vijayan,
Durgesh Kumar,
Ao Du,
Mirco Sastges,
Lei Gao,
Zijie Xiao,
Dongwook Go,
José Omar Ledesma-Martin,
Hai I. Wang,
Daegeun Jo,
Peter M. Oppeneer,
Rahul Gupta,
Gerhard Jakob,
Sachin Krishnia,
Yuriy Mokrousov,
Mathias Kläui
Abstract:
The orbital Hall effect (OHE) has attracted significant attention for developing energy-efficient electronic devices. However, utilizing it in fast, low-power devices requires an enhanced understanding of underlying extrinsic and intrinsic contributions to OHE at timescales ranging from quasi-static to picoseconds. Here, we investigate OHE in light metal vanadium (V) using a combination of selecte…
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The orbital Hall effect (OHE) has attracted significant attention for developing energy-efficient electronic devices. However, utilizing it in fast, low-power devices requires an enhanced understanding of underlying extrinsic and intrinsic contributions to OHE at timescales ranging from quasi-static to picoseconds. Here, we investigate OHE in light metal vanadium (V) using a combination of selected measurement schemes, spanning the full frequency range. We observe a negative damping-like torque efficiency from V, opposite to conventional theoretical predictions, with a magnitude that depends on the adjacent ferromagnet, a dependence that indicates orbital effects. These results, with consistent torque efficiencies across all frequencies, corroborate a negative and intrinsic OHE in V with a large effective orbital Hall conductivity of $-(1.44 \pm 0.34)\,\frac{\hbar}{2e}\,\times 10^{5}\,Ω^{-1}\,\mathrm{m}^{-1}$ and a long orbital diffusion length of $(15.0 \pm 2.5)\,\mathrm{nm}$. To explain the observed OHE, we develop a theoretical model incorporating both local and itinerant circulation contributions to OHE. The model agrees excellently with the experimental results, demonstrating that itinerant contributions are essential for a complete physical understanding of intrinsic OHE. Our consistent experimental and theoretical data highlight the importance of itinerant contributions governing the fundamental understanding of intrinsic OHE and the large effects found open pathways for energy-efficient orbitronic devices.
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Submitted 17 December, 2025; v1 submitted 22 August, 2025;
originally announced August 2025.
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Temperature- and charge carrier density-dependent electronic response in methylammonium lead iodide
Authors:
Jiacheng Wang Jungmin Park,
Lei Gao,
Lucia Di Virgilio,
Sheng Qu,
Heejae Kim,
Hai I. Wang,
Li-Lin Wu,
Wen Zeng,
Mischa Bonn,
Zefeng Ren,
Jaco J. Geuchies
Abstract:
Understanding carrier dynamics in photoexcited metal-halide perovskites is key for optoelectronic devices such as solar cells (low carrier densities) and lasers (high carrier densities). Trapping processes at low carrier densities and many-body recombination at high densities can significantly alter the dynamics of photoexcited carriers. Combining optical-pump/THz probe and transient absorption sp…
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Understanding carrier dynamics in photoexcited metal-halide perovskites is key for optoelectronic devices such as solar cells (low carrier densities) and lasers (high carrier densities). Trapping processes at low carrier densities and many-body recombination at high densities can significantly alter the dynamics of photoexcited carriers. Combining optical-pump/THz probe and transient absorption spectroscopy we examine carrier responses over a wide density range (10^14-10^19 cm-3) and temperatures (78-315K) in the prototypical methylammonium lead iodide perovskite. At densities below ~10^15 cm-3 (room temperature, sunlight conditions), fast carrier trapping at shallow trap states occurs within a few picoseconds. As excited carrier densities increase, trapping saturates, and the carrier response stabilizes, lasting up to hundreds of picoseconds at densities around ~10^17 cm-3. Above 10^18 cm-3 a Mott transition sets in: overlapping polaron wavefunctions lead to ultrafast annihilation through an Auger recombination process occurring over a few picoseconds. We map out trap-dominated, direct recombination-dominated, and Mott-dominated density regimes from 78-315 K, ultimately enabling the construction of an electronic phase diagram. These findings clarify carrier behavior across operational conditions, aiding material optimization for optoelectronics operating in the low (e.g. photovoltaics) and high (e.g. laser) carrier density regimes.
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Submitted 24 May, 2025;
originally announced May 2025.
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Cove-edged Chiral Graphene Nanoribbons with Chirality-Dependent Bandgap and Carrier Mobility
Authors:
K. Liu,
W. Zheng,
S. Osella,
Z. Qiu,
S. Böckmann,
W. Niu,
L. Meingast,
H. Komber,
S. Obermann,
R. Gillen,
M. Bonn,
M. R. Hansen,
J. Maultzsch,
H. I. Wang,
J. Ma,
X. Feng
Abstract:
Graphene nanoribbons (GNRs) have garnered significant interest due to their highly customizable physicochemical properties and potential utility in nanoelectronics. Besides controlling widths and edge structures, the inclusion of chirality in GNRs brings another dimension for fine-tuning their optoelectronic properties, but related studies remain elusive owing to the absence of feasible synthetic…
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Graphene nanoribbons (GNRs) have garnered significant interest due to their highly customizable physicochemical properties and potential utility in nanoelectronics. Besides controlling widths and edge structures, the inclusion of chirality in GNRs brings another dimension for fine-tuning their optoelectronic properties, but related studies remain elusive owing to the absence of feasible synthetic strategies. Here, we demonstrate a novel class of cove-edged chiral GNRs (CcGNRs) with a tunable chiral vector (n,m). Notably, the bandgap and effective mass of (n,2)- CcGNR show a distinct positive correlation with the increasing value of n, as indicated by theory. Within this GNR family, two representative members, namely, (4,2)- CcGNR and (6,2)-CcGNR, are successfully synthesized. Both CcGNRs exhibit prominently curved geometries arising from the incorporated [4]helicene motifs along their peripheries, as also evidenced by the single-crystal structures of the two respective model compounds (1 and 2). The chemical identities and optoelectronic properties of (4,2)- and (6,2)-CcGNRs are comprehensively investigated via a combination of IR, Raman, solid-state NMR, UV-vis, and THz spectroscopies as well as theoretical calculations. In line with theoretical expectation, the obtained (6,2)-CcGNR possesses a low optical bandgap of 1.37 eV along with charge carrier mobility of 8 cm2/Vs, whereas (4,2)-CcGNR exhibits a narrower bandgap of 1.26 eV with increased mobility of 14 cm2/Vs. This work opens up a new avenue to precisely engineer the bandgap and carrier mobility of GNRs by manipulating their chiral vector.
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Submitted 7 March, 2025; v1 submitted 18 February, 2025;
originally announced February 2025.
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Beyond the band edge: Unveiling high-mobility hot carriers in a two-dimensional conjugated coordination polymer
Authors:
Shuai Fu,
Xing Huang,
Guoquan Gao,
Petko St. Petkov,
Wenpei Gao,
Jianjun Zhang,
Lei Gao,
Heng Zhang,
Min Liu,
Mike Hambsch,
Wenjie Zhang,
Jiaxu Zhang,
Keming Li,
Ute Kaiser,
Stuart S. P. Parkin,
Stefan C. B. Mannsfeld,
Tong Zhu,
Hai I. Wang,
Zhiyong Wang,
Renhao Dong,
Xinliang Feng,
Mischa Bonn
Abstract:
Hot carriers, inheriting excess kinetic energy from high-energy photons, underpin numerous optoelectronic applications involving non-equilibrium transport processes. Current research on hot carriers has predominantly focused on inorganic materials, with little attention paid to organic-based systems due to their ultrafast energy relaxation and inefficient charge transport. Here, we overturn this p…
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Hot carriers, inheriting excess kinetic energy from high-energy photons, underpin numerous optoelectronic applications involving non-equilibrium transport processes. Current research on hot carriers has predominantly focused on inorganic materials, with little attention paid to organic-based systems due to their ultrafast energy relaxation and inefficient charge transport. Here, we overturn this paradigm by demonstrating highly mobile hot carriers in solution-processable, highly crystalline two-dimensional conjugated coordination polymer (2D c-CP) Cu3BHT (BHT = benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we unravel the microscopic charge transport landscape in Cu3BHT films following non-equilibrium photoexcitation across temporal, spatial, and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium transport regime, hot carriers achieve ultrahigh mobility of ~2,000 cm2 V-1 s-1, traversing grain boundaries up to 300 nm within a picosecond. In the quasi-equilibrium transport regime, free carriers exhibit Drude-type band-like transport with a remarkable mobility of ~400 cm2 V-1 s-1 and an intrinsic diffusion length exceeding 1 micrometer. These findings establish 2D c-CPs as versatile platforms for exploring high-mobility non-equilibrium transport, unlocking new opportunities for organic-based hot carrier applications.
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Submitted 15 January, 2025;
originally announced January 2025.
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The Effect of Charge Carrier Cooling on the Ultrafast Carrier Dynamics in Cs$_2$AgBiBr$_6$ Thin Films
Authors:
Huygen J. Jobsis,
Lei Gao,
Antti-Pekka M. Reponen,
Zachary A. VanOrman,
Rick P. P. P. M. Rijpers,
Hai I. Wang,
Sascha Feldmann,
Eline M. Hutter
Abstract:
Cs$_2$AgBiBr$_6$ shows promise for solution-processable optoelectronics, such as photovoltaics, photocatalysis and X-ray detection. However, various spectroscopic studies report rapid charge carrier mobility loss in the first picosecond after photoexcitation, limiting carrier collection efficiencies. The origin of this rapid mobility loss is still unclear. Here, we directly compare hot excitation…
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Cs$_2$AgBiBr$_6$ shows promise for solution-processable optoelectronics, such as photovoltaics, photocatalysis and X-ray detection. However, various spectroscopic studies report rapid charge carrier mobility loss in the first picosecond after photoexcitation, limiting carrier collection efficiencies. The origin of this rapid mobility loss is still unclear. Here, we directly compare hot excitation with excitation over the indirect fundamental bandgap, using transient absorption and THz spectroscopy on the same Cs$_2$AgBiBr$_6$ thin film sample. From transient absorption spectroscopy, we find that hot carriers cool towards the band-edges with a cooling rate of 0.58 ps$^{-1}$, which coincides with the observed mobility loss rate from THz spectroscopy. Hence, our study establishes a direct link between the hot carrier cooling and ultrafast mobility loss on the picosecond timescale.
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Submitted 19 December, 2024;
originally announced December 2024.
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Curved graphene nanoribbons derived from tetrahydropyrene-based polyphenylenes via one-pot K-region oxidation and Scholl cyclization
Authors:
Sebastian Obermann,
Wenhao Zheng,
Jason Melidonie,
Steffen Böckmann,
Silvio Osella,
Lenin Andrés Guerrero León,
Felix Hennersdorf,
David Beljonne,
Jan J. Weigand,
Mischa Bonn,
Michael Ryan Hansen,
Hai I. Wang,
Ji Ma,
Xinliang Feng
Abstract:
Precise synthesis of graphene nanoribbons (GNRs) is of great interest to chemists and materials scientists because of their unique opto-electronic properties and potential applications in carbon-based nanoelectronics and spintronics. In addition to the tunable edge structure and width, introducing curvature in GNRs is a powerful structural feature for their chemi-physical property modification. He…
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Precise synthesis of graphene nanoribbons (GNRs) is of great interest to chemists and materials scientists because of their unique opto-electronic properties and potential applications in carbon-based nanoelectronics and spintronics. In addition to the tunable edge structure and width, introducing curvature in GNRs is a powerful structural feature for their chemi-physical property modification. Here, we report an efficient solution synthesis of the first pyrene-based GNR (PyGNR) with curved geometry via one-pot K-region oxidation and Scholl cyclization of its corresponding well-soluble tetrahydropyrene-based polyphenylene precursor. The efficient A2B2-type Suzuki polymerization and subsequent Scholl reaction furnishes up to 35 nm long curved GNRs bearing cove- and armchair-edges. The construction of model compound, as a cutout of PyGNR, from a tetrahydropyrene-based oligophenylene precursor proves the concept and efficiency of the one-pot K-region oxidation and Scholl cyclization, which is clearly revealed by single crystal X-ray diffraction analysis. The structure and optical properties of PyGNR are investigated by Raman, FT-IR, solid-state NMR and UV-Vis analysis with the support of DFT calculations. PyGNR shows the absorption maximum at 680 nm, exhibiting a narrow optical bandgap of 1.4 eV, qualifying as a low-bandgap GNR. Moreover, THz spectroscopy on PyGNR estimates its macroscopic charge mobility of 3.6 cm2/Vs, outperforming other curved GNRs reported via conventional Scholl reaction.
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Submitted 10 October, 2024;
originally announced October 2024.
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Spontaneous Exciton Dissociation in Transition Metal Dichalcogenide Monolayers
Authors:
Taketo Handa,
Madisen A. Holbrook,
Nicholas Olsen,
Luke N. Holtzman,
Lucas Huber,
Hai I. Wang,
Mischa Bonn,
Katayun Barmak,
James C. Hone,
Abhay N. Pasupathy,
X. -Y. Zhu
Abstract:
Since the seminal work on MoS2 monolayers, photoexcitation in atomically-thin transition metal dichalcogenides (TMDCs) has been assumed to result in excitons with large binding energies (~ 200-600 meV). Because the exciton binding energies are order-of-magnitude larger than thermal energy at room temperature, it is puzzling that photocurrent and photovoltage generation have been observed in TMDC-b…
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Since the seminal work on MoS2 monolayers, photoexcitation in atomically-thin transition metal dichalcogenides (TMDCs) has been assumed to result in excitons with large binding energies (~ 200-600 meV). Because the exciton binding energies are order-of-magnitude larger than thermal energy at room temperature, it is puzzling that photocurrent and photovoltage generation have been observed in TMDC-based devices, even in monolayers with applied electric fields far below the threshold for exciton dissociation. Here, we show that the photoexcitation of TMDC monolayers results in a substantial population of free charges. Performing ultrafast terahertz (THz) spectroscopy on large-area, single crystal WS2, WSe2, and MoSe2 monolayers, we find that ~10% of excitons spontaneously dissociate into charge carriers with lifetimes exceeding 0.2 ns. Scanning tunnelling microscopy reveals that photo-carrier generation is intimately related to mid-gap defect states, likely via trap-mediated Auger scattering. Only in state-of-the-art quality monolayers14, with mid-gap trap densities as low as 10^9 cm^-2, does intrinsic exciton physics start to dominate the THz response. Our findings reveal that excitons or excitonic complexes are only the predominant quasiparticles in photo-excited TMDC monolayers at the limit of sufficiently low defect densities.
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Submitted 19 June, 2023;
originally announced June 2023.
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Harnessing van der Waals CrPS4 and Surface Oxides for non-monotonic pre-set field induced Exchange Bias in Fe3GeTe2
Authors:
Aravind Puthirath Balan,
Aditya Kumar,
Tanja Scholz,
Zhongchong Lin,
Aga Shahee,
Shuai Fu,
Thibaud Denneulin,
Joseph Vas,
Andras Kovacs,
Rafal E. Dunin-Borkowski,
Hai I. Wang,
Jinbo Yang,
Bettina Lotsch,
Ulrich Nowak,
Mathias Klaeui
Abstract:
Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that nat…
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Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that naturally oxidized vdW ferromagnetic Fe3GeTe2 exhibits exchange bias, attributed to the antiferromagnetic coupling of its ultrathin surface oxide layer (O-FGT) with the underlying unoxidized Fe3GeTe2. Anomalous Hall measurements are employed to scrutinize the exchange bias within the CrPS4/(O-FGT)/Fe3GeTe2 heterostructure. This analysis takes into account the contributions from both the perfectly uncompensated interfacial CrPS4 layer and the interfacial oxide layer. Intriguingly, a distinct and non-monotonic exchange bias trend is observed as a function of temperature below 140 K. The occurrence of exchange bias induced by a 'pre-set field' implies that the prevailing phase in the polycrystalline surface oxide is ferrimagnetic Fe3O4. Moreover, the exchange bias induced by the ferrimagnetic Fe3O4 is significantly modulated by the presence of the van der Waals antiferromagnetic CrPS4 layer, forming a heterostructure, along with additional iron oxide phases within the oxide layer. These findings underscore the intricate and complex nature of exchange bias in van der Waals heterostructures, highlighting their potential for tailored manipulation and control.
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Submitted 16 February, 2024; v1 submitted 23 March, 2023;
originally announced March 2023.
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Transiently delocalized states enhance hole mobility in organic molecular semiconductors
Authors:
Samuele Giannini,
Lucia Di Virgilio,
Marco Bardini,
Julian Hausch,
Jaco Geuchies,
Wenhao Zheng,
Martina Volpi,
Jan Elsner,
Katharina Broch,
Yves H. Geerts,
Frank Schreiber,
Guillaume Schweicher,
Hai I. Wang,
Jochen Blumberger,
Mischa Bonn,
David Beljonne
Abstract:
There is compelling evidence that charge carriers in organic semiconductors (OSs) self-localize in nano-scale space because of dynamic disorder. Yet, some OSs, in particular recently emerged high-mobility organic molecular crystals, feature reduced mobility at increasing temperature, a hallmark for delocalized band transport. Here we present the temperature-dependent mobility in two record-mobilit…
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There is compelling evidence that charge carriers in organic semiconductors (OSs) self-localize in nano-scale space because of dynamic disorder. Yet, some OSs, in particular recently emerged high-mobility organic molecular crystals, feature reduced mobility at increasing temperature, a hallmark for delocalized band transport. Here we present the temperature-dependent mobility in two record-mobility OSs: DNTT (dinaphtho[2,3-b:2',3'-f]thieno[3,2-b]-thiophene), and its alkylated derivative, C8-DNTT-C8. By combining terahertz photoconductivity measurements with fully atomistic non-adiabatic molecular dynamics simulations, we show that while both crystals display a power-law decrease of the mobility (μ) with temperature (T, following: μ\propto T^(-n)), the exponent n differs substantially. Modelling provides n values in good agreement with experiments and reveals that the differences in the falloff parameter between the two chemically closely related semiconductors can be traced to the delocalization of the different states thermally accessible by charge carriers, which in turn depends on the specific electronic band structure of the two systems. The emerging picture is that of holes surfing on a dynamic manifold of vibrationally-dressed extended states with a temperature-dependent mobility that provides a sensitive fingerprint for the underlying density of states.
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Submitted 23 March, 2023;
originally announced March 2023.
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Probing Carrier Dynamics in sp$^{3}$-Functionalized Single-Walled Carbon Nanotubes with Time-Resolved Terahertz Spectroscopy
Authors:
Wenhao Zheng,
Nicolas F. Zorn,
Mischa Bonn,
Jana Zaumseil,
Hai I. Wang
Abstract:
The controlled introduction of covalent sp$^{3}$ defects into semiconducting single-walled carbon nanotubes (SWCNTs) gives rise to exciton localization and red-shifted near-infrared luminescence. The single-photon emission characteristics of these functionalized SWCNTs make them interesting candidates for electrically driven quantum light sources. However, the impact of sp$^{3}$ defects on the car…
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The controlled introduction of covalent sp$^{3}$ defects into semiconducting single-walled carbon nanotubes (SWCNTs) gives rise to exciton localization and red-shifted near-infrared luminescence. The single-photon emission characteristics of these functionalized SWCNTs make them interesting candidates for electrically driven quantum light sources. However, the impact of sp$^{3}$ defects on the carrier dynamics and charge transport in carbon nanotubes remains an open question. Here, we use ultrafast, time-resolved optical-pump terahertz-probe spectroscopy as a direct and quantitative technique to investigate the microscopic and temperature-dependent charge transport properties of pristine and functionalized (6,5) SWCNTs in dispersions and thin films. We find that sp$^{3}$ functionalization increases charge carrier scattering, thus reducing the intra-nanotube carrier mobility. In combination with electrical measurements of SWCNT network field-effect transistors, these data enable us to distinguish between contributions of intra-nanotube band transport, sp$^{3}$ defect scattering and inter-nanotube carrier hopping to the overall charge transport properties of nanotube networks.
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Submitted 20 June, 2022;
originally announced June 2022.
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Long-Lived Charge Separation Following Pump-Energy Dependent Ultrafast Charge Transfer in Graphene/WS$_2$ Heterostructures
Authors:
Shuai Fu,
Indy du Fossé,
Xiaoyu Jia,
Jingyin Xu,
Xiaoqing Yu,
Heng Zhang,
Wenhao Zheng,
Sven Krasel,
Zongping Chen,
Zhiming M. Wang,
Klaas-Jan Tielrooij,
Mischa Bonn,
Arjan J. Houtepen,
Hai I. Wang
Abstract:
Van der Waals heterostructures consisting of graphene and transition metal dichalcogenides (TMDCs) have recently shown great promise for high-performance optoelectronic applications. However, an in-depth understanding of the critical processes for device operation, namely interfacial charge transfer (CT) and recombination, has so far remained elusive. Here, we investigate these processes in graphe…
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Van der Waals heterostructures consisting of graphene and transition metal dichalcogenides (TMDCs) have recently shown great promise for high-performance optoelectronic applications. However, an in-depth understanding of the critical processes for device operation, namely interfacial charge transfer (CT) and recombination, has so far remained elusive. Here, we investigate these processes in graphene-WS$_2$ heterostructures, by complementarily probing the ultrafast terahertz photoconductivity in graphene and the transient absorption dynamics in WS$_2$ following photoexcitation. We find that CT across graphene-WS$_2$ interfaces occurs via photo-thermionic emission for sub-A-exciton excitation, and direct hole transfer from WS$_2$ to the valence band of graphene for above-A-exciton excitation. Remarkably, we observe that separated charges in the heterostructure following CT live extremely long: beyond 1 ns, in contrast to ~1 ps charge separation reported in previous studies. This leads to efficient photogating of graphene. These findings provide relevant insights to optimize further the performance of optoelectronic devices, in particular photodetection.
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Submitted 6 August, 2020; v1 submitted 17 July, 2020;
originally announced July 2020.
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Experimental Observation of Strong Exciton Effects in Graphene Nanoribbons
Authors:
Alexander Tries,
Silvio Osella,
Pengfei Zhang,
Fugui Xu,
Mathias Kläui,
Yiyong Mai,
David Beljonne,
Hai I. Wang
Abstract:
Graphene nanoribbons (GNRs) with atomically precise width and edge structures are a promising class of nanomaterials for optoelectronics, thanks to their semiconducting nature and high mobility of charge carriers. Understanding the fundamental static optical properties and ultrafast dynamics of charge carrier generation in GNRs is essential for optoelectronic applications. Combining THz spectrosco…
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Graphene nanoribbons (GNRs) with atomically precise width and edge structures are a promising class of nanomaterials for optoelectronics, thanks to their semiconducting nature and high mobility of charge carriers. Understanding the fundamental static optical properties and ultrafast dynamics of charge carrier generation in GNRs is essential for optoelectronic applications. Combining THz spectroscopy and theoretical calculations, we report a strong exciton effect with binding energy up to 700 meV in liquid-phase-dispersed GNRs with a width of 1.7 nm and an optical bandgap of 1.6 eV, illustrating the intrinsically strong Coulomb interactions between photogenerated electrons and holes. By tracking the exciton dynamics, we reveal an ultrafast formation of excitons in GNRs with a long lifetime over 100 ps. Our results not only reveal fundamental aspects of excitons in GNRs (gigantic binding energy and ultrafast exciton formation etc.), but also highlight promising properties of GNRs for optoelectronic devices.
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Submitted 14 April, 2020; v1 submitted 11 November, 2019;
originally announced November 2019.
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The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies
Authors:
A. Tomadin,
S. M. Hornett,
H. I. Wang,
E. M. Alexeev,
A. Candini,
C. Coletti,
D. Turchinovich,
M. Klaeui,
M. Bonn,
F. H. L. Koppens,
E. Hendry,
M. Polini,
K. J. Tielrooij
Abstract:
For many of the envisioned optoelectronic applications of graphene it is crucial to understand the sub-picosecond carrier dynamics immediately following photoexcitation, as well as the effect on the electrical conductivity - the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations have be…
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For many of the envisioned optoelectronic applications of graphene it is crucial to understand the sub-picosecond carrier dynamics immediately following photoexcitation, as well as the effect on the electrical conductivity - the photoconductivity. Whereas these topics have been studied using various ultrafast experiments and theoretical approaches, controversial and incomplete explanations have been put forward concerning the sign of the photoconductivity, the occurrence and significance of the creation of additional electron-hole pairs, and, in particular, how the relevant processes depend on Fermi energy. Here, we present a unified and intuitive physical picture of the ultrafast carrier dynamics and the photoconductivity, combining optical pump - terahertz probe measurements on a gate-tunable graphene device, with numerical calculations using the Boltzmann equation. We distinguish two types of ultrafast photo-induced carrier heating processes: At low (equilibrium) Fermi energy ($E_{\rm F} \lesssim$ 0.1 eV for our experiments) broadening of the carrier distribution involves interband transitions - interband heating. At higher Fermi energy ($E_{\rm F} \gtrsim$ 0.15 eV) broadening of the carrier distribution involves intraband transitions - intraband heating. Under certain conditions, additional electron-hole pairs can be created (carrier multiplication) for low $E_{\rm F}$, and hot carriers (hot-carrier multiplication) for higher $E_{\rm F}$. The resultant photoconductivity is positive (negative) for low (high) $E_{\rm F}$, which originates from the effect of the heated carrier distributions on the screening of impurities, consistent with the DC conductivity being mostly due to impurity scattering. The importance of these insights is highlighted by a discussion of the implications for graphene photodetector applications.
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Submitted 7 December, 2017;
originally announced December 2017.