Probe Photon Energy Research Articles

Dynamically enhanced Autler–Townes splitting by orthogonal XUV fields

Abstract Based on numerical solutions of the time-dependent Schrödinger equation, we theoretically investigate the photoelectron spectrum of hydrogen atoms ionized by a pair of ultrashort, intense, and orthogonally polarized laser pulses with a relative time delay in a pump–probe configuration. The pump pulse resonantly excites electrons from the 1s and 2p levels, inducing Rabi oscillations. The resulting dynamically enhanced Autler–Townes (AT) splitting is observed in the photoelectron energy spectrum upon interaction with the second probe pulse. In contrast to the previous parallel-polarization scheme, the proposed orthogonal-polarization configuration enables the resolution of dynamically enhanced AT splitting over a considerably wider range of probe photon energies.

A coherent phonon-induced hidden quadrupolar ordered state in Ca2RuO4

Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic hidden states exhibiting higher multipolar ordering remain elusive owing to the challenge of directly manipulating and detecting them with light. Here we demonstrate a method to induce a dynamical transition from a thermally allowed to a thermally forbidden spin-orbit entangled quadrupolar ordered state in Ca2RuO4 by coherently exciting a phonon that is strongly coupled to the order parameter. Combining probe photon energy-resolved coherent phonon spectroscopy measurements with model Hamiltonian calculations, we show that the dynamical transition is manifested through anomalies in the temperature, pump excitation fluence, and probe photon energy dependence of the strongly coupled phonon. With this procedure, we introduce a general pathway to uncover hidden multipolar ordered states and to control their re-orientation on ultrashort timescales.

Time- and angle-resolved photoemission spectroscopy (TR-ARPES) of TMDC monolayers and bilayers.

Many unique properties in two-dimensional (2D) materials and their heterostructures rely on charge excitation, scattering, transfer, and relaxation dynamics across different points in the momentum space. Understanding these dynamics is crucial in both the fundamental study of 2D physics and their incorporation in optoelectronic and quantum devices. A direct method to probe charge carrier dynamics with momentum resolution is time- and angle-resolved photoemission spectroscopy (TR-ARPES). Such measurements have been challenging, since photoexcited carriers in many 2D monolayers reside at high crystal momenta, requiring probe photon energies in the extreme UV (EUV) regime. These challenges have been recently addressed by development of table-top pulsed EUV sources based on high harmonic generation, and the successful integration into a TR-ARPES and/or time-resolved momentum microscope. Such experiments will allow direct imaging of photoelectrons with superior time, energy, and crystal momentum resolution, with unique advantage over traditional optical measurements. Recently, TR-ARPES experiments of 2D transition metal dichalcogenide (TMDC) monolayers and bilayers have created unprecedented opportunities to reveal many intrinsic dynamics of 2D materials, such as bandgap renormalization, charge carrier scattering, relaxation, and wavefunction localization in moiré patterns. This perspective aims to give a short review of recent discoveries and discuss the challenges and opportunities of such techniques in the future.

A newly designed femtosecond KBe2BO3F2 device with pulse duration down to 55fs for time- and angle-resolved photoemission spectroscopy.

Developing a widely tunable vacuum ultraviolet (VUV) source with a sub-100fs pulse duration is critical for ultrafast pump-probe techniques such as time- and angle-resolved photoemission spectroscopy (TrARPES). While a tunable probe source with a photon energy of 5.3-7.0eV has been recently implemented for TrARPES by using a KBe2BO3F2 (KBBF) device, the time resolution of 280-320fs is still not ideal, which is mainly limited by the duration of the VUV probe pulse generated by the KBBF device. Here, by designing a new KBBF device, which is specially optimized for fs applications, an optimum pulse duration of 55fs is obtained after systematic diagnostics and optimization. More importantly, a high time resolution of 81-95fs is achieved for TrARPES measurements covering the probe photon energy range of 5.3-7.0eV, making it particularly useful for investigating the ultrafast dynamics of quantum materials. Our work extends the application of the KBBF device to ultrafast pump-probe techniques with the advantages of both a widely tunable VUV source and ultimate time resolution.

Population Inversion and Dirac Fermion Cooling in 3D Dirac Semimetal Cd3As2.

Revealing the ultrafast dynamics of three-dimensional (3D) Dirac fermions is critical for both fundamental science and device applications. So far, how the cooling of 3D Dirac fermions differs from that of two-dimensional (2D) and whether there is population inversion are fundamental questions to be answered. Here we reveal the ultrafast dynamics of Dirac fermions in a model 3D Dirac semimetal Cd3As2 by time- and angle-resolved photoemission spectroscopy with a tunable probe photon energy. The energy- and momentum-resolved relaxation rate shows a linear dependence on the energy, suggesting Dirac fermion cooling through intraband relaxation. Moreover, a population inversion is reported based on the observation of accumulated photoexcited carriers in the conduction band with a lifetime of 3.0 ps. Our work provides direct experimental evidence for a long-lived population inversion in a 3D Dirac semimetal, which is in contrast to 2D graphene with a much shorter lifetime.

Ultrafast time- and angle-resolved photoemission spectroscopy with widely tunable probe photon energy of 5.3-7.0eV for investigating dynamics of three-dimensional materials.

Time- and angle-resolved photoemission spectroscopy (TrARPES) is a powerful technique for capturing the ultrafast dynamics of charge carriers and revealing photo-induced phase transitions in quantum materials. However, the lack of widely tunable probe photon energy, which is critical for accessing the dispersions at different out-of-plane momentum kz in TrARPES measurements, has hindered the ultrafast dynamics investigation of 3D quantum materials, such as Dirac or Weyl semimetals. Here, we report the development of a TrARPES system with a highly tunable probe photon energy from 5.3 to 7.0eV. The tunable probe photon energy is generated by the fourth harmonic generation of a tunable wavelength femtosecond laser source by combining a β-BaB2O4 crystal and a KBe2BO3F2 crystal. A high energy resolution of 29-48meV and time resolution of 280-320fs are demonstrated on 3D topological materials ZrTe5 and Sb2Te3. Our work opens up new opportunities for exploring ultrafast dynamics in 3D quantum materials.

Unmasking the cis-Stilbene Phantom State via Vacuum Ultraviolet Time-Resolved Photoelectron Spectroscopy and Ab Initio Multiple Spawning.

We present the first vacuum ultraviolet time-resolved photoelectron spectroscopy (VUV-TRPES) study of photoisomerization dynamics in the paradigmatic molecule cis-stilbene. A key reaction intermediate in its dynamics, known as the phantom state, has often been invoked but never directly detected in the gas phase. We report direct spectral signatures of the phantom state in isolated cis-stilbene, observed and characterized through a combination of VUV-TRPES and ab initio multiple spawning (AIMS) nonadiabatic dynamics simulations of the channel-resolved observable. The high VUV probe photon energy tracks the complete excited-state dynamics via multiple photoionization channels, from initial excitation to its return to the "hot" ground state. The TRPES was compared with AIMS simulations of the dynamics from initial excitation, to the phantom-state intermediate (an S1 minimum), through to the ultimate electronic decay to the ground state. This combination revealed the unique spectral signatures and time-dependent dynamics of the phantom-state intermediate, permitting us to report here its direct observation.

Disentangling the Temporal Dynamics of Nonthermal Electrons in Photoexcited Gold Nanostructures

AbstractThe study of nonthermal electrons, generated upon photoexcitation of plasmonic nanostructures, plays a key role in a variety of contexts, from photocatalysis and energy conversion to photodetection and nonlinear optics. Their ultrafast relaxation and subsequent release of energy to a low energy distribution of thermalized hot electrons has been the subject of a myriad of papers, mostly based on femtosecond transient absorption spectroscopy (FTAS). However, the FTAS signal stems from a complex interplay of different contributions arising from both nonthermal and thermal electrons, making the disentanglement of the two a very challenging task, so far accomplished only in terms of numerical simulations. Here a combined approach is introduced, based on a post‐processing of the FTAS measurements guided by a reduced semiclassical model, the so‐called extended two‐temperature model, which has allowed the purely nonthermal contribution to the pump‐probe experimental map recorded for 2D arrays of gold nanoellipsoids to be isolated. This approach displays the intimate correlation between electron energy and probe photon energy on the ultrafast time‐scale of electron thermalization. It also sheds new light on the ultrafast transient optical response of gold nanostructures, and will help the development of optimized plasmonic configurations for nonthermal electrons generation and harvesting.

Nonperturbative signatures of nonlinear Compton scattering

The probabilities of various elementary laser - photon - electron/positron interactions display in selected phase space and parameter regions typical non-perturbative dependencies such as $\propto {\cal P} \exp\{- a E_{crit} /E\}$, where ${\cal P}$ is a pre-exponential factor, $E_{crit}$ denotes the critical Sauter-Schwinger field strength, and $E$ characterizes the (laser) field strength. While the Schwinger process with $a = a_S \equiv \pi$ and the non-linear Breit-Wheeler process in the tunneling regime with $a = a_{n \ell BW} \equiv 4 m / 3 \omega'$ (with $\omega'$ the probe photon energy and $m$ the electron/positron mass) are famous results, we point out here that also the non-linear Compton scattering exhibits a similar behavior when focusing on high harmonics. Using a suitable cut-off $c > 0$, the factor $a$ becomes $a = a_{n \ell C} \equiv \frac23 c m /(p_0 + \sqrt{p_0^2 -m^2)}$. This opens the avenue towards a new signature of the boiling point of the vacuum even for field strengths $E$ below $E_{crit}$ by employing a high electron beam-energy $p_0$ to counter balance the large ratio $E_{crit} / E$ by a small factor $a$ to achieve $E / a \to E_{crit}$. In the weak-field regime, the cut-off facilitates a threshold leading to multi-photon signatures showing up in the total cross section at sub-threshold energies.

Framework for analyzing the thermoreflectance spectra of metal thermal transducers with spectrally tunable time-domain thermoreflectance

The time-domain thermoreflectance (TDTR) technique has been widely used to measure thermal properties. The design and interpretation of the TDTR experiment rely on an in-depth understanding of the thermoreflectance signature for a given metal thermal transducer. Although the TDTR signals of several metal thermal transducers have been experimentally investigated, a practical framework bridging the electronic properties and the thermoreflectance characteristics of metal thermal transducers will be helpful for future studies. Compiling published results and our analysis and tests, in this work, we show a theoretical strategy to determine the thermallyinduced change of reflectance spectra with the electronic properties of metal transducers as the input. As a natural consequence of the proposed framework, we show that the optimal probe photon energy occurs near the interband transition threshold of the metal. To validate our approach, TDTR experiments are performed with Au and Cu as two representative metal thermal transducers in two temporal regimes when electrons and lattices have different temperatures (<10 ps) and reach thermal equilibrium (>10 ps), respectively. The experimental results show good agreement with the theory. The work fundamentally elucidates the thermally induced optical response of metal thermal transducers and also provides practical guidelines for choosing the appropriate probe photon energy to optimize the TDTR signal for a given metal thermal transducer, which is useful for broadening the adaptability of TDTR to various experimental conditions, materials, and new laser sources.

A study of two-photon florescence in metallic nanoshells

A theory of the two-photon florescence for a metallic nanoshell in the presence of quantum emitters has been developed. The metallic nanoshell is made of a metallic nanosphere as a core and a dielectric material as a shell. An ensemble of quantum emitters is deposited on the surface of the dielectric shell. A probe field is applied to study the two-photon process in the metallic nanoshell. Surface plasmon polaritons are created at the interface between the core and shell due to coupling between probe photons and surface plasmons present at the surface of the metallic nanosphere. The intensity of the surface plasmon polariton field is huge when the probe photon energy is in resonance with the polariton resonance energy. Induced electric dipoles are created in each quantum emitter due to the surface plasmon polariton field and the probe field. Dipoles in quantum emitters interact with each other via the dipole-dipole interaction. The dipole-dipole interaction is calculated using the many-body theory and mean field approximation. It is found that the dipole-dipole interaction has new term which is induced by the surface plasmon polariton field. An analytical expression of the two-photon florescence is derived in the presence the dipole-dipole interaction. Our theory predicts that the intensity of the two-photon florescence is enhanced in the presence of quantum emitters relative to the florescence of the metallic nanoshell in isolation. Physics behind the enhancement is the presence of the dipole-dipole interaction between the ensemble of quantum emitters. It is also found that as the concentration of quantum emitters increases, the dipole-dipole field also increases. This in turn, increases the two-photon florescence as function of the concentration. Finally, we have compared our theory with experiments of a metallic nanoshell which is made for Au nanosphere core and the SiO2 shell. The metallic nanoshell is surrounded by various concentrations of Cadmium-Selenium quantum dots as quantum emitters. A good agreement between theory and experiment is found.

Many-body recombination in photoexcited insulating cuprates

We study the pump-probe response of three insulating cuprates and develop a model for its recombination kinetics. The dependence on time, fluence, and both pump and probe photon energies imply many-body recombination on femtosecond timescales, characterized by anomalously large trapping and Auger coefficients. The fluence dependence follows a universal form that includes a characteristic volume scale, which we associate with the holon-doublon excitation efficiency. This volume varies strongly with pump photon energy and peaks near twice the charge-transfer energy, suggesting that the variation is caused by carrier multiplication through impact ionization.

Femtosecond-time-resolved imaging of the dielectric function of ZnO in the visible to near-IR spectral range

We demonstrate micrometer-resolved imaging of the transient dielectric function of a c-ZnO thin film with femtosecond resolution in the visible to near-IR spectral range measured by pump-probe ellipsometry at five different probe photon-energies. The spatial profile of the real part of the dielectric function broadens drastically with increasing time delay, which we associate with the combined effect of carrier cooling and fast carrier transport with an effective diffusion coefficient of (1.1±0.1)×104 cm2/s. A ring structure is detected in the image after a few picoseconds, which can be explained by a random-walk model including ballistic transport due to the thermal gradient induced by the hot-phonon effect.

A time- and angle-resolved photoemission spectroscopy with probe photon energy up to 6.7 eV.

We present the development of a time- and angle-resolved photoemission spectroscopy based on a Yb-based femtosecond laser and a hemispherical electron analyzer. The energy of the pump photon is tunable between 1.4 and 1.9 eV, and the pulse duration is around 30 fs. We use a KBe2BO3F2 nonlinear optical crystal to generate probe pulses, of which the photon energy is up to 6.7 eV, and obtain an overall time resolution of 1 ps and energy resolution of 18 meV. In addition, β-BaB2O4 crystals are used to generate alternative probe pulses at 6.05 eV, giving an overall time resolution of 130 fs and energy resolution of 19 meV. We illustrate the performance of the system with representative data on several samples (Bi2Se3, YbCd2Sb2, and FeSe).

Unveiling the Stimulated Robust Carrier Lifetime of Surface‐Bound Excitons and Their Photoresponse in InSe

AbstractIn contrast to zero‐bandgap metallic graphene, the binary semiconducting compound, InSe, possesses a tunable bandgap. Herein, a range of particle sizes of β‐InSe from bulk to few‐layer nanosheets and quantum dots are carefully prepared. The size‐dependent bandgap variation and photon‐induced carrier dynamics of InSe are systemically investigated. In contrast to the normal size‐dependent carrier lifetime trend observed at 700 nm, anomalous size‐independent carrier decay is observed at 500 nm. Through time‐dependent density functional theory calculations, the normal carrier lifetimes at lower probe photon energies are attributed to in‐plane excitons, whereas the abnormal size‐independent carrier lifetimes at higher probe photon energies are found to be stimulated by surface‐bound excitons. In view of the robust surface exciton, this suggests that InSe may possess an outstanding optoelectronic performance in the shorter wavelength range. Through photoelectrochemical detection experiments, it is confirmed that InSe features a high photocurrent density and stability and, in particular, a more distinct photoresponse at short wavelengths than at longer ones. Comprehending and quantifying the role of the surface‐bound excitons in InSe across a broad range of semiconductor nanostructures and their fundamental properties may play an important role in understanding the physical properties of 2D III–VI compound materials.

Ultrafast nonlinear transparency driven at a telecom wavelength in an organic semiconductor system

Ultrafast laser-induced transparency is demonstrated using femtosecond (fs) pump-probe experiments in the organic P3HT:PCBM (donor:acceptor) blend structure. For above band gap pumping, ultrafast transient signals strongly depend on the probe photon energy. Most intriguingly, for below band gap pumping at 0.95 eV, or 1.3 µm at a telecom wavelength, a huge transmission increase up to 30% only during the laser pulse ∼100 fs is observed as a pump-driven, quasi-instantaneous suppression of absorption for the high photon-energy energy probe beam. We attribute the observed laser-driven transparency to dynamic Franz-Keldysh effect, at least one order of magnitude stronger compared to the multiphoton nonlinearities. Our results may be used for development of low-cost, beyond 100 Gbit/s optical switching devices.

Time- and angle-resolved photoemission spectroscopy of solids in the extreme ultraviolet at 500 kHz repetition rate.

Time- and angle-resolved photoemission spectroscopy (trARPES) employing a 500 kHz extreme-ultraviolet light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification, and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than 1011 photons/s on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynamics in occupied and normally unoccupied (excited) states in the entire Brillouin zone and with a temporal system response function below 40 fs.

Observation of Small Polaron and Acoustic Phonon Coupling in Ultrathin La0.7Sr0.3MnO3/SrTiO3 Structures

Understanding the underlying physics of interactions among various quasi‐particles is a fundamental issue for the application of spintronics and photonics. Here the observation of a coupling between the small polarons in the nanoscale ultrathin La0.7Sr0.3MnO3 (LSMO) films and the acoustic phonons in the SrTiO3 (STO) substrate using ultrafast pump–probe spectroscopy has been reported. According to the temperature‐ and wavelength‐dependent measurements, the amplitudes of the acoustic phonons are suppressed by tuning the small polarons absorption. This shows a coupled relationship between the acoustic phonons and the small polarons. At the probe photon energy of 1.55 eV where the polaron absorption is dominant, the acoustic phonons become unobservable. Furthermore, by performing the pump fluence dependent measurements on the LSMO films with different thicknesses, smaller acoustic phonon amplitudes are found in the thinner film with stronger small polaron binding energy. Such a coupled nature can be utilized to manipulate the small polarons using the acoustic phonons or vice versa, which is of great importance in device applications of colossal magnetoresistance materials.

Dynamics of electron attachment and photodissociation in iodide-uracil-water clusters via time-resolved photoelectron imaging.

The dynamics of low energy electron attachment to monohydrated uracil are investigated using time-resolved photoelectron imaging to excite and probe iodide-uracil-water (I-·U·H2O) clusters. Upon photoexcitation of I-·U·H2O at 4.38 eV, near the measured cluster vertical detachment energy of 4.40 eV ± 0.05 eV, formation of both the dipole bound (DB) anion and valence bound (VB) anion of I-·U·H2O is observed and characterized using a probe photon energy of 1.58 eV. The measured binding energies for both anions are larger than those of the non-hydrated iodide-uracil (I-·U) counterparts, indicating that the presence of water stabilizes the transient negative ions. The VB anion exhibits a somewhat delayed 400 fs rise when compared to I-·U, suggesting that partial conversion of the DB anion to form the VB anion at early times is promoted by the water molecule. At a higher probe photon energy, 3.14 eV, I- re-formation is measured to be the major photodissociation channel. This product exhibits a bi-exponential rise; it is likely that the fast component arises from DB anion decay by internal conversion to the anion ground state followed by dissociation to I-, and the slow component arises from internal conversion of the VB anion.

Ultrafast Electron–Phonon Coupling at Metal-Dielectric Interface

ABSTRACTEnergy transfer from photo-excited electrons in a metal thin film to the dielectric substrate is important for understanding the ultrafast heat transfer process across the two materials. Substantial research has been conducted to investigate heat transfer in a metal-dielectric structure. In this work, a two-temperature model in metal was used to analyze the interface electron and dielectric substrate coupling. An improved temperature and wavelength-dependent Drude–Lorentz model was implemented to interpret the signals obtained in optical measurements. Ultrafast pump-and-probe measurements on Au-Si samples were carried out, where the probe photon energy was chosen to be close to the interband transition threshold of gold to minimize the influence of non-equilibrium electrons on the optical response and maximize the thermal modulation to the optical reflectance. Electron-substrate interface thermal conductance at different pump laser fluences was obtained, and was found to increase with the interface temperature.