Pump Photon Energy Research Articles

Ultrafast dynamics of two-dimensional electron gas at Al2O3/SrTiO3 interface studied by surface terahertz spectroscopy.

Two-dimensional electron gas (2DEG) confined at the interface of SrTiO3-based heterostructure exhibits intriguing electronic and optoelectronic properties. In this work, we study the ultrafast dynamics of 2DEG at the Al2O3/SrTiO3 interface using surface-specific terahertz difference-frequency spectroscopy. Through proper polarization selection, we have resolved simultaneously the evolution of 2DEG confined in the quantum well and the surface potential after optical pump with different photon energies. The hot electrons excited from 2DEG with pump photon energy below the band gap relax to the ground state through two processes, a fast interfacial process associated with electron-electron and electron-phonon scattering on the order of tens of picoseconds and a slow surface-to-bulk transport on the order of hundreds of picoseconds. When the pump photon energy exceeds the bandgap, electrons are directly injected from the valence band to 2DEG at the interface and relax via electron-hole recombination in 3ps. The recorded dynamic change of interfacial potential provides the key information to identify the drift and diffusion of photocarriers at the interface. Our results broaden the horizon of investigation on the comprehension of complex oxide interfaces and their photonics capabilities.

Charge‐Transfer‐Mediated Exciton Dynamics in Van der Waals Antiferromagnet NiPS3

Abstract2D van der Waals antiferromagnets have emerged as excellent candidates for studying novel low‐dimensional magnetism. The recently discovered spin–orbit‐entangled excitonic bound state appearing below the Néel temperature of 150 K in 2D antiferromagnetic NiPS3 (the so‐called Zhang–Rice (ZR) exciton) has drawn considerable attention in terms of exploring the strong correlation of spins, orbitals, and charges in a localized many‐body state. However, the formation mechanism of ZR excitons remains unclear, and its ultrafast dynamics have yet to be fully explored. Here, utilizing broadband transient reflectivity spectroscopy, the strong correlation between the charge‐transfer state excitation and the dynamic evolution of ZR excitons is investigated. Through systematic tuning of the pumping photon energy across the charge‐transfer state in NiPS3, the results reveal a short radiative lifetime of tens of picoseconds and a long nonradiative lifetime of up to nanoseconds for ZR excitons following an ultrafast charge transfer of ≈2 ps from the charge‐transfer state. The findings provide evidence of charge‐transfer‐induced ZR excitonic states in NiPS3, where the intriguing phenomena of strongly coupled spins and charges can be explored.

Quantum‐Defect‐Minimized, Three‐Photon‐Pumped Ultralow‐Threshold Perovskite Excitonic Lasing

AbstractThree‐photon‐pumped (3PP) excitonic lasing in inorganic semiconductor quantum dots (QDs) is of particular importance for near‐infrared biophotonics and optical communications. However, the implementation of such lasers has been hindered severely by the required high pump thresholds. Here, 3PP excitonic lasing of all‐inorganic cesium lead bromide perovskite QDs (CsPbBr3 PQDs) embedded in a whispering‐gallery microcavity is demonstrated, and achieving a record low threshold of 3 mJ cm−2 by tuning the 3P pump energy in resonance with the S exciton state. Wavelength‐dispersive Z‐scan spectroscopy reveals that such reduced lasing threshold is attributed to the exciton resonance enhanced multiphoton absorption, which, as disclosed by the kinetics analysis of transient absorption spectroscopy (TAS), leads to the appearance of net gain at a pump fluence as low as 2.2 mJ cm−2, corresponding to an average S exciton population of 1.5. A microscopic model incorporating the quantum master equation reproduces the TAS results and provides the intrinsic parameters of biexciton relaxation for lasing. The 3PP resonant excitonic transition is the most favored multiphoton pumping process that minimizes quantum defect (6.8% of the pump photon energy) to realize optical gain at low threshold, marking a major step toward using all‐inorganic perovskite QDs for on‐chip integrated microlasers and multiphoton bioimaging.

Room temperature persisting surface charge carriers driven by intense terahertz electric fields in a topological insulator Bi2Se3

Topologically protected surface current is highly promising for next-generation low-dissipation and disorder-tolerant quantum electronics and computing. Yet, electric transport from the co-existing bulk state dominates the responses of the Dirac surface state, especially at elevated temperatures relevant to technological applications. Here, we present an approach that convincingly showcases the generation, disentanglement, and precise control of enduring surface charge carriers on a topological insulator, Bi2Se3, with high bulk conductivity, all achieved at room temperature. By using pump–probe modulation spectroscopy under ultrabroadband driving tunable from 4 meV to 1.55 eV, we show the terahertz (THz) field-induced surface carriers by discovering their initial temporal responses dominant over high density trivial bulk carriers. Strikingly, the response of the induced surface carrier responses persists for more than ∼5 ps and is enhanced by reducing pump photon energy. The dynamics and lifetime of the distinct surface response manifest themselves as the enhanced THz pump-induced THz transmission, which directly correlates with the transient negative THz conductivity. Increasing the THz driving field reduces the induced surface carrier lifetime and identifies, particularly, an optimal pump field of Es ∼ 224 kV cm−1 for generating the dominant surface response relative to the bulk. This surface carrier dominant regime is suppressed by a joint effect of enhanced surface-bulk scattering and a more rapid saturation of surface excitation compared to the bulk that sets in above Es. The controllability of room temperature topologically surface carriers through pump photon energy offer compelling possibilities for extending this approach to other topological complex materials.

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

The optical Stark effect is a universal response of the electronic structure to incident light. In semiconductors, particularly nanomaterials, the optical Stark effect achieved with sub-band gap photons can drive large, narrowband, and potentially ultrafast changes in the absorption or reflection at the band gap through excitation of virtual excitons. Rapid optical modulation using the optical Stark effect is ultimately constrained, however, by the generation of long-lived excitons through multiphoton absorption. This work compares the modulation achievable using the optical Stark effect on CdSe nanoplatelets with several different pump photon energies, from the visible to mid-infrared. Despite expected lower efficiencies for spectrally-remote pump energies, infrared pump pulses can ultimately drive larger sub-picosecond optical Stark shifts of virtual excitons without creation of real excitons. The CdSe nanoplatelets show subpicosecond shifts of the lowest excitonic resonance of up to 22 meV, resulting in change in absorption as large as 0.32 OD (49% increase in transmission), with a long-lived offset from real excitons less than 1% of the peak signal.

Effects of initial three-dimensional electron energy distribution on terahertz Bloch oscillations in a biased semiconductor superlattice

We investigate how the initial three-dimensional energy distribution of electrons created by femtosecond pump pulses in a biased semiconductor superlattice affects terahertz Bloch oscillations, which imitate a step response to a bias electric field. The emitted terahertz waveforms are well reproduced from a damped oscillation current with capacitive nature, exhibiting shorter relaxation times and worse temporal resolutions for central pump photon energies that are outside the range of ordinary electron excitation into the conduction first miniband. This indicates that in-plane excess energy changes the relaxation time via scattering processes, while partial use of the pump pulse spectrum reduces the temporal resolution.

Quantum beat of heavy-hole and light-hole excitons originating from interband Stark-ladder transitions in a biased GaAs/AlAs superlattice

The letter reports the quantum beat of heavy-hole (HH) and light-hole (LH) excitons originating from interband Stark-ladder transitions in a GaAs/AlAs superlattice. Under the condition that the pump photon energy was well below the LH-related transition energy, only Bloch oscillation was observed. As the pump photon energy was increased, another oscillatory signal with a frequency of ∼6 THz was superimposed. The calculation considering related transitions indicates that the oscillation is due to the quantum beat of HH and LH excitons originating from the interband Stark-ladder transitions between the hole states and the electron state in the first-nearest-neighbor quantum wells.

Effects of Pump Photon Energy on Generation and Ultrafast Relaxation of Excitons and Charge Carriers in CdSe Nanoplatelets.

We studied the initial nature and relaxation of photoexcited electronic states in CdSe nanoplatelets (NPLs). Ultrafast transient optical absorption (TA) measurements were combined with the theoretical analysis of the formation and decay of excitons, biexcitons, free charge carriers, and trions. In the latter, photons and excitons were treated as bosons and free charge carriers as fermions. The initial quantum yields of heavy-hole (HH) excitons, light-hole (LH) excitons, and charge carriers vary strongly with photon energy, while thermal relaxation occurs always within 1 ps. After that, the population of LH excitons is negligible due to relaxation to HH excitons or decay into free electrons and holes. Up to the highest average number of about four absorbed photons per NPL in our experiments, we found no signatures of the presence of biexcitons or larger complexes. Biexcitons were only observed due to the interaction of a probe-generated exciton with an exciton produced previously by the pump pulse. For higher pump photon energies, the initial presence of more free charge carriers leads to formation of trions by probe photons. On increasing the number of absorbed pump photons in an NPL, the yield of excitons becomes higher as compared to free charge carriers, since electron-hole recombination becomes more likely. In addition to a TA absorption feature at energy below the HH exciton peak, we also observed a TA signal at the high-energy side of this peak, which we attribute to formation of LH-HH biexcitons or trions consisting of a charge and LH exciton.

THz generation in GaSe crystals pumped with laser photon energy below and around the bandgap

We study optical rectification in GaSe by performing THz generation with femtosecond laser pulses whose wavelength is tuned from below to above the GaSe bandgap. As expected from a theory, we observed a first THz emission peak at 1.77 eV, where phase matching is realized. A second THz emission peak was recorded, when the pump photon energy reaches the crystal bandgap (2.205 eV). This can be attributed to a resonance of the GaSe nonlinearity. In crystals thinner than the coherence length, the bandgap peak is stronger than the phase-matched one.

Ultrafast signatures of spin and orbital order in antiferromagnetic α-Sr2CrO4

The antiferromagnetic Mott insulator α-Sr2CrO4 possesses multiple spin and orbital ordered phases, but their unique interplay is still relatively unexplored. Here, we used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in α-Sr2CrO4 through their non-equilibrium response to photoexcitation. By varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t2g orbitals and charge transfer-type transitions between oxygen 2p and Cr eg orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Néel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α-Sr2CrO4 and provide experimental evidence for the phase transition at TO, possibly related to antiferro-type orbital ordering.

Two-photon pumped exciton-polariton condensation

Two-photon absorption (TPA) allows accessing “dark” states of matter that are otherwise inaccessible to light, which serve as important building blocks for quantum information processing. In a semiconductor microcavity, TPA-driven condensation of strongly coupled light-matter exciton–polaritons can enable new solid-state quantum simulations of “dark” state-condensate interactions and was predicted to stimulate THz emission. Here, we report the first observation of two-photon-pumped polariton condensation, demonstrated by angle-resolved photoluminescence in a GaAs-based microcavity. TPA is evidenced in the quadratic emission dependence on pump power below and above the condensation threshold, and second-harmonic generation is ruled out by both this threshold behavior and by the emission peak energy showing no dependence on pump photon energy. Our results pave the way toward novel polariton-based sources and solid-state coherent control of collective quantum states with individual two-level systems.

Photon‐dressed biexciton‐mediated anomalous optical Stark effect in CsPbBr3 nanocrystals

Intense optical pumping below bandgap creates photon‐dressed states, which interact with and result in the shift of electronic levels, known as optical Stark effect (OSE). The OSE persists only for pump pulse duration implying the coherent response. Previous researches in semiconductors have shown that coherent OSE is evident only at cryogenic temperatures. Only recently lead halide perovskites (LHPs) were found to possess room temperature OSE. However, despite strong exciton–exciton interactions known in LHPs, OSE is described in non‐interacting framework that treats an exciton like isolated two‐level systems. The present work demonstrates anomalous OSE in interacting regime at room temperature in CsPbBr3 nanocrystals having exciton resonance (E0) at 2.40 eV using circularly polarized transient absorption spectroscopy. The results show that photon dressing for same pump–probe polarization (σ+σ+) lead to observation of blueshift of exciton resonance across all pump detuning energies (Ω = E0 − ħω; ħω is pump photon energy). On the contrary, under opposite pump–probe polarization (σ+σ−), the strong exciton−biexciton interaction leads to a coherent red shift and splitting of the exciton resonance as a function of the drive photon frequency. The hallmark observations under σ+σ− result from large biexciton binding energy of ~71 meV and exciton−biexciton transition dipole moment of ~25 Debye. Further, we demonstrate unusual crossover from linear to nonlinear dependence of the OSE as a function of the drive photon frequency. Our systematic study reveals crucial information on unexplored many body interacting regimes of coherent manipulation in LHPs, important for exotic quantum phase applications like quantum information processing and ultrafast switching.

Effect of diffusion on acoustic deformation potential characterization through coherent acoustic phonon dynamics

Ultrafast spectroscopy of coherent acoustic phonon (CAP) dynamics has recently been proposed as a method to characterize acoustic deformation potential (ADP), a key standard to quantify carrier--acoustic phonon coupling in semiconductors. In this Letter, we illustrate the importance of addressing the diffusion effect in ADP characterization by this method, using Ge as the demonstration system. It is found that the ADP mechanism and the thermoelastic effect have comparable contributions to CAP generation in Ge. Due to the different dependences on pump photon energies, the roles of these two mechanisms were assessed by varying pump wavelengths, based on which the ADP coupling constant of Ge was obtained. The analysis reveals that the carrier diffusion has a considerable impact on the shape of the CAP wave packet and must be processed cautiously for the ADP characterization for Ge.

Optimum excitation wavelength and photon energy threshold for spintronic terahertz emission from Fe/Pt bilayer

SummaryTerahertz emission from ferromagnetic/non-magnetic spintronic heterostructures had been demonstrated as pump wavelength-independent. We report, however, the pump wavelength dependence of terahertz emission from an optimized Fe/Pt spintronic bilayer on MgO substrate. Maximum terahertz generation per total pump power was observed in the 1200- to 1800-nm pump wavelength range, and a marked decrease in the terahertz emission efficiency beyond 2500 nm (pump photon energies <0.5 eV) suggests a ∼0.35-eV threshold pump photon energy for effective spintronic terahertz emission. The inferred threshold is supported by previous theoretical results on the onset energy of significant spin-filtering at the Fe-Pt interface, and confirmed by Fe/Pt electronic structure calculations in this present work. The results of terahertz time-domain emission spectroscopy show the sensitivity of spintronic terahertz emission to both the optical absorptance of the heterostructure and the energy-dependent spin transport, as dictated by the properties of the metallic thin films.

Photoinduced Polaron Formation in a Polymerized Electron-Acceptor Semiconductor.

Polymerized small molecular acceptor (PSMA) based all-polymer solar cells (all-PSC) have achieved power conversion efficiencies (PCE) over 16%, and the PSMA is considered to hold great promise for further improving the performance of all-PSC. Yet, in comparison with that of the polymer donor, the photophysics of a polymerized acceptor remains poorly understood. Herein, the excited state dynamics in a polymerized acceptor PZT810 was comprehensively investigated under various pump intensities and photon energies. The excess excitation energy was found to play a key role in excitons dissociation into free polarons for neat PSMA films, while free polarons cannot be generated from the polaron pairs in neat acceptor films. This work reveals an in-depth understanding of relaxation dynamics for PSMAs and that the underlying photophysical origin of PSMA can be mediated by excitation energies and intensities. These results would benefit the realization of the working mechanism for all-PSC and the designing of new PSMAs.

Large area stimulated emission luminescent solar concentrators modelled using detailed balance consistent rate equations.

Stimulated emission luminescent solar concentrators (SELSCs) have the potential to reduce escape cone losses in luminescent solar concentrators (LSCs). However, a functional SELSC is yet to be demonstrated. Previous numerical studies and detailed balance limits provide guidance, but they also contradict and likely overestimate performance and underestimate requirements. In this work, we introduce a rate-equation model with inversion requirements compatible with detailed balance limits and apply this model to the numerical modelling of window-sized SELSCs. We find that the optimal pump photon energy for both LSCs and SELSCs is 1.35 eV and the potential improvement of SELSCs over LSCs is found to be 19.3%. The efficiencies found are much lower than those specified in previous work due to the increase in Stokes shift required for a highly luminescent material. We also find that SELSCs are more attractive at higher matrix losses, that emission linewidths <0.05 eV are desirable, and that SELSC devices can potentially achieve performance equal to LSCs at low illumination levels and simultaneously exceed it by up to 16.5% at 1-sun illumination.

High-power quasi-CW diode-pumped 750-nm AlGaAs VECSEL emitting a peak power of 29.6 W and an average power of 8.5 W.

A peak output power of 29.6 W and an average output power of 8.5 W at a wavelength of 750 nm were demonstrated in quasi-CW multi-mode operation using an AlGaAs-based vertical external-cavity surface-emitting laser (VECSEL) diode-pumped at a wavelength of 675 nm. The comparatively low bandgap of the barrier material that was tuned to the pump-photon energy allowed a good compromise between low heat generation due to the quantum defect and strong absorptance of the pump radiation. The limitations for the average output power came mainly from insufficient heat flow from the intra-cavity heat spreader to the heat sink. These results show the potential for power scaling of diode-pumped VECSELs and the importance of effective heat removal.

Ultrafast hot carrier transfer in WS2/graphene large area heterostructures

Charge transfer processes in two-dimensional van der Waals heterostructures enable upconversion of low energy photons and efficient charge carriers extraction. Here we use broadband ultrafast optical spectroscopy to track charge transfer dynamics in large-area 2D heterostructures made of epitaxial single-layer tungsten disulfide (WS2) grown by chemical vapour deposition on graphene. Selective carrier photoexcitation in graphene, with tunable near-infrared photon energies as low as 0.8 eV (i.e. lower than half of the optical bandgap of WS2), results in an almost instantaneous bleaching of the WS2 excitonic peaks in the visible range, due to the interlayer charge transfer process. We find that the charge transfer signal is strongly non-linear with the pump fluence and it becomes progressively more linear at increasing pump photon energies, while the interlayer photoinjection rate is constant in energy, reflecting the spectrally flat absorbance of graphene. We ascribe the interlayer charge transfer to a fast transfer of hot carriers, photogenerated in graphene, to the semiconducting layer. The measured sub-20-fs hot-carrier transfer sets the ultimate timescale for this process. Besides their fundamental interest, our results are technologically relevant because, given the capability of large-area deterministic growth of the heterostructure, they open up promising paths for novel 2D photodetectors, also potentially scalable to industrial platforms.

Role of primary and secondary processes in the ultrafast spin dynamics of nickel

The magnetic response of a ferromagnet after an ultrafast optical excitation can be connected to the underlying electronic dynamics either via primary excitation processes during the laser pulse or via secondary collision processes. In the latter case, the information on the details of the excitation is lost and, therefore, the electron dynamics can be described using quasi-equilibrium concepts. In this work, we study the effect of the pump photon energy on the ultrafast demagnetization dynamics in ferromagnetic nickel. We find that the magnetization dynamics for similar absorbed energies for a range of pump photon energies are almost identical and depend only on the absorbed energy. This is in stark contrast to characteristic differences in the optically excited electronic distributions, as calculated from the band structure. In addition, the measured fluence-dependent dynamics can be reproduced with a model based on local temperatures. These findings indicate that it is mainly secondary processes that are responsible for the observed demagnetization dynamics.

Probing ultrafast hot charge carrier migration in MoS2 embedded CdS nanorods.

Efficient utilization of hot charge carriers is of utmost benefit for a semiconductor-based optoelectronic device. Herein, a one-dimensional (1D)/two-dimensional (2D) heterojunction was fabricated in the form of CdS/MoS2 nanorod/nanosheet composite and migration of hot charge carriers was being investigated with the help of transient absorption (TA) spectroscopy. The band alignment was such that both the electrons and holes in the CdS region tend to migrate into the MoS2 region following photoexcitation. The composite system is composed of optical signatures of both CdS and MoS2, with the dominance of CdS nanorods. In addition, the TA signal of MoS2 is substantially enhanced in the heterosystem at the cost of the diminished CdS signal, confirming the migration of charge carrier population from CdS to MoS2. This migration phenomenon was dominated by the hot carrier transfer. The hot carriers in the high energy states of CdS are preferentially migrated into the MoS2 states rather than being cooled to the band edge. The hot carrier transfer time for a 400nm pump excitation was calculated to be 0.21ps. This is much faster than the band edge electron transfer process, occurring at 2.0ps time scale. We found that these migration processes are very much dependent on the applied pump photon energy. Higher energy pump photons are more efficient in the hot carrier transfer process and place these hot carriers in the higher energy states of MoS2, further extending charge carrier separation. This detailed spectroscopic investigation would help in the fabrication of better 1D/2D heterojunctions and advance the optoelectronic field.