Search Results (33)

We conducted a comprehensive study of the non-equilibrium dynamics of Cooper pair breaking, quasiparticle (QP) generation, and relaxation in niobium (Nb) cut from superconducting radio-frequency (SRF) cavities, as well as various Nb resonator films from transmon qubits. Using ultrafast pump–probe spectroscopy, we were able to isolate the superconducting coherence and pair-breaking responses. Our results reveal both similarities and notable differences in the temperature- and magnetic-field-dependent dynamics of the SRF cavity and thin-film resonator samples. Moreover, femtosecond-resolved QP generation and relaxation under an applied magnetic field reveals a clear correlation between non-equilibrium QPs and the quality factor of resonators fabricated by using different deposition methods, such as DC sputtering and high-power impulse magnetron sputtering. These findings highlight the pivotal influence of fabrication techniques on the coherence and performance of Nb-based quantum devices, which are vital for applications in superconducting qubits and high-energy superconducting radio-frequency applications. Full article

The ability to study chemical dynamics on ultrafast timescales has greatly advanced with the introduction of X-ray free electron lasers (XFELs) providing short pulses of intense X-rays tailored to probe atomic structure and electronic configuration. Fully exploiting the full potential of XFELs requires specialized experimental endstations along with the development of techniques and methods to successfully carry out experiments. The liquid jet endstation (LJE) at the Linac Coherent Light Source (LCLS) has been developed to study photochemistry and biochemistry in solution systems using a combination of X-ray solution scattering (XSS), X-ray absorption spectroscopy (XAS), and X-ray emission spectroscopy (XES). The pump–probe setup utilizes an optical laser to excite the sample, which is subsequently probed by a hard X-ray pulse to resolve structural and electronic dynamics at their intrinsic femtosecond timescales. The LJE ensures reliable sample delivery to the X-ray interaction point via various liquid jets, enabling rapid replenishment of thin samples with millimolar concentrations and low sample volumes at the 120 Hz repetition rate of the LCLS beam. This paper provides a detailed description of the LJE design and of the techniques it enables, with an emphasis on the diagnostics required for real-time monitoring of the liquid jet and on the spatiotemporal overlap methods used to optimize the signal. Additionally, various scientific examples are discussed, highlighting the versatility of the LJE. Full article

Photo-induced carrier dynamics were measured in the organic Dirac electron candidate $\alpha$-(BETS)${}_2$I${}_3$ to investigate why resistivity increases below $T_{\mathrm{MI}}$ = 50 K. We found a change in carrier dynamics due to an insulating gap formation below $T^{\prime }$ = 50 K. On the other hand, the relaxation time and polarization anisotropy of the observed dynamics differ from those in the charge-ordering (CO) state of the isostructural salt $\alpha$-(ET)${}_2$I${}_3$. Based on the difference, it can be concluded that the insulating phase has a different origin than the CO state. Full article

The photo-induced charge dynamics of textbook wide-bandgap semiconductor ZnO have been investigated on the picosecond time-scale. We performed optical Pump-THz Probe experiments in order to measure the dielectric constant of the material after high-fluence photo-excitation of charge carriers. The technique allows access to both carrier lifetime and scattering rates, and it provides direct access to the intrinsic dielectric function changes upon excitation. A complex dynamic is unveiled in the high-fluence pumping regime, where the relaxation time is in the hundreds of picoseconds range and increases with increasing Pump fluence, while the onset of photoconductivity takes place in a few picoseconds. The plasma frequency and the relaxation time dependence on the Pump fluence are discussed. Full article

Proton transfer processes of organic molecules are key to charge transport and photoprotection in biological systems. Among them, excited-state intramolecular proton transfer (ESIPT) reactions are characterized by quick and efficient charge transfer within a molecule, resulting in ultrafast proton motions. The ESIPT-facilitated interconversion between two tautomers (PS and PA) comprising the tree fungal pigment Draconin Red in solution was investigated using a combination of targeted femtosecond transient absorption (fs-TA) and excited-state femtosecond stimulated Raman spectroscopy (ES-FSRS) measurements. Transient intensity (population and polarizability) and frequency (structural and cooling) dynamics of –COH rocking and –C=C, –C=O stretching modes following directed stimulation of each tautomer elucidate the excitation-dependent relaxation pathways, particularly the bidirectional ESIPT progression out of the Franck–Condon region to the lower-lying excited state, of the intrinsically heterogeneous chromophore in dichloromethane solvent. A characteristic overall excited-state PS-to-PA transition on the picosecond timescale leads to a unique “W”-shaped excited-state Raman intensity pattern due to dynamic resonance enhancement with the Raman pump–probe pulse pair. The ability to utilize quantum mechanics calculations in conjunction with steady-state electronic absorption and emission spectra to induce disparate excited-state populations in an inhomogeneous mixture of similar tautomers has broad implications for the modeling of potential energy surfaces and delineation of reaction mechanisms in naturally occurring chromophores. Such fundamental insights afforded by in-depth analysis of ultrafast spectroscopic datasets are also beneficial for future development of sustainable materials and optoelectronics. Full article

In this work, we investigate the relaxation processes of 2-thiouracil after UV photoexcitation to the S₂ state through the use of ultrafast, single-colour, pump-probe UV/UV spectroscopy. We place focus on investigating the appearance and subsequent decay signals of ionized fragments. We complement this with VUV-induced dissociative photoionisation studies collected at a synchrotron, allowing us to better understand and assign the ionisation channels involved in the appearance of the fragments. We find that all fragments appear when single photons with energy > 11 eV are used in the VUV experiments and hence appear through 3+ photon-order processes when 266 nm light is used. We also observe three major decays for the fragment ions: a sub-autocorrelation decay (i.e., sub-370 fs), a secondary ultrafast decay on the order of 300–400 fs, and a long decay on the order of 220 to 400 ps (all fragment dependent). These decays agree well with the previously established S₂ → S₁ → Triplet → Ground decay process. Results from the VUV study also suggest that some of the fragments may be created by dynamics occurring in the excited cationic state. Full article

By employing optical pump Terahertz (THz) probe spectroscopy, ultrafast photocarrier dynamics of a two-dimensional (2D) semiconductor, SnS₂ nanoflake film, has been investigated systematically at room temperature. The dynamics of photoexcitation is strongly related to the density of edge sites and defects in the SnS₂ nanoflakes, which is controllable by adjusting the height of vertically aligned SnS₂ during chemical vapor deposition growth. After photoexcitation at 400 nm, the transient THz photoconductivity response of the films can be well fitted with bi-exponential decay function. The fast and slow processes are shorter in the thinner film than in the thicker sample, and both components are independent on the pump fluence. Hereby, we propose that edge-site trapping as well as defect-assisted electron-hole recombination are responsible for the fast and slow decay progress, respectively. Our experimental results demonstrate that the edge sites and defects in SnS₂ nanoflakes play a dominant role in photocarrier relaxation, which is crucial in understanding the photoelectrochemical performance of SnS₂ nanoflakes. Full article

The development of novel coherent and brilliant sources, such as soft X-ray free electron laser (FEL) and high harmonic generation (HHG), enables new ultrafast analysis of the electronic and structural dynamics of a wide variety of materials. Soft X-ray FEL delivers high-brilliance beams with a short pulse duration, high spatial coherence and photon energy tunability. In comparison with FELs, HHG X-ray sources are characterized by a wide spectral bandwidth and few- to sub-femtosecond pulses. The approach will lead to the time-resolved reconstruction of molecular dynamics, shedding light on different photochemical pathways. The high peak brilliance of soft X-ray FELs facilitates investigations in a nonlinear regime, while the broader spectral bandwidth of the HHG sources may provide the simultaneous probing of multiple components. Significant technical breakthroughs in these novel sources are under way to improve brilliance, pulse duration, and to control spectral bandwidth, spot size, and energy resolution. Therefore, in the next few years, the new generation of soft X-ray sources combined with novel experimental techniques, new detectors, and computing capabilities will allow for the study of several extremely fast dynamics, such as vibronic dynamics. In the present review, we discuss recent developments in experiments, performed with soft X-ray FELs and HHG sources, operating near the carbon K-absorption edge, being a key atomic component in biosystems and soft materials. Different spectroscopy methods such as time-resolved pump-probe techniques, nonlinear spectroscopies and photoelectron spectroscopy studies have been addressed in an attempt to better understand fundamental physico-chemical processes. Full article

The spectral range of femtosecond time-resolved infrared spectroscopy is limited by the bandwidth of mid-IR pulses (100~400 cm⁻¹) generated from the combination of Ti:Sapphire amplifier, Optical Parametric Amplifier (OPA), and Difference Frequency Generation (DFG). To overcome this limitation, we implement a compact continuum mid-IR source producing ultrafast pulses that span the frequency range from 1000 to 4200 cm⁻¹ (from 10 to 2.4 μm), which utilize the mixing of fundamental, second-harmonic, and third-harmonic of 800 nm pulse in the air. After building an IR spectrometer with continuum IR and a monochromator, we found that the distortion of the measured IR spectrum originated from the contamination of higher-order diffraction. We used bandpass filters to eliminate the higher-order contributions and correct the measured IR spectrum. We further characterized the spectral properties of fundamental, second-harmonic, and third-harmonic fields after the plasmonic filamentation process, which helps to improve the efficiency of the continuum IR generation. Using the generated continuum IR pulses, we measured the IR absorption spectrum of a water–benzonitrile mixture, which was found to be consistent with the spectrum obtained with a commercial FT-IR spectrometer. The present work will be useful for the efficient generation of continuum IR pulses for IR pump-probe and two-dimensional IR spectroscopy experiments in the future. Full article

Two-dimensional (2D) tri-TMDCs carrier dynamics provide a platform for studying excitons through Ultrafast Pump-Probe Transient Absorption Spectroscopy. Here we studied the ZrTe₃ nanosheets (NTs) exciton dynamics by transient absorption (TA) spectrometer. We observed different carrier dynamics in the ZrTe₃ NTs sample at different pump powers and with many wavelengths in the transient absorption spectrometer. The shorter life decay constant is associated with electron-phonon relaxation. Similarly, the longer-life decay constant represents the long live process that is associated with charge separation. The interactions between carrier-phonons at nanoscale materials can be changed by phonons quantum confinements. The hot carrier lifetime determined the strength of carrier phonon interactions. The value of fast decay in the conduction band is due to carrier relaxation or the carrier gets trapped due to surface states or localized defects. The value of slow decay is due to the recombination of surface state and localized defects processes. The lifetime declines for long wavelengths as size decreases. Whereas, during short wavelength-independent decay, carrier characteristics have been observed. TA spectroscopy is employed to investigate insight information of the carrier’s dynamical processes such as carrier lifetime, cooling dynamics, carrier diffusion, and carrier excitations. The absorption enhanced along excitons density with the increase of pump power, which caused a greater number of carriers in the excited state than in the ground state. The TA signals consist of trap carriers and (electron-hole) constituents, which can be increased by TA changes that rely on photoexcitation and carrier properties. Full article

Bimetallic Au/Ag core–shell cuboid nanoparticles (NPs) exhibit a complex plasmonic response dominated by a dipolar longitudinal mode and higher-order transverse modes in the near-UV, which may be exploited for a range of applications. In this paper, we take advantage of the strong signature of these modes in the NP ultrafast transient optical response, measured by pump-probe transient absorption (TA) spectroscopy, to explore the NP vibrational landscape. The fast Fourier transform analysis of the TA dynamics reveals specific vibration modes in the frequency range 15–150 GHz, further studied by numerical simulations based on the finite element method. While bare Au nanorods exhibit extensional and breathing modes, the bimetallic NPs undergo more complex motions, involving the displacement of facets, edges and corners. The amplitude and frequency of these modes are shown to depend on the Ag shell thickness, as the silver load modifies the NP aspect ratio and mass. Moreover, the contributions of the vibrational modes to the experimental TA spectra are shown to vary with the probe laser wavelength at which the signal is monitored. Using the combined simulations of the NP elastic and optical properties, we elucidate this influence by analyzing the effect of the mechanisms involved in the acousto-plasmonic coupling. Full article

Vanadium pentoxide can undergo a reversible phase transition by heating above 260 °C; its non-thermal phase transition, as well as ultrafast dynamical processes, is still not known. Here, femtosecond laser-induced phase transition properties in V₂O₅ thin films were first explored using femtosecond time-resolved pump–probe spectroscopy. The results show that the phase transient processes occur on a 10⁻¹⁵–10⁻¹³ temporal scale. The phase transition and recovery properties are dependent on both the substrates and pump laser energy densities. We propose the oxygen vacancies theory to explain the results, and we provide valuable insights into V₂O₅ films for potential applications. Full article

Cu₃N with a cubic crystal structure is obtained in this paper by the sputtering of Cu under N₂ followed by annealing under NH₃: H₂ at 400 °C, after which it was doped with iodine at room temperature resulting into p-type Cu₃N with hole densities between 10¹⁶ and 10¹⁷ cm⁻³. The Cu₃N exhibited distinct maxima in differential transmission at ~2.01 eV and 1.87 eV as shown by ultrafast pump-probe spectroscopy, corresponding to the M and R direct energy band gaps in excellent agreement with density functional theory calculations, suggesting that the band gap is clean and free of mid-gap states. The Cu₃N was gradually converted into optically transparent γ-CuI that had a hole density of 4 × 10¹⁷ cm⁻³, mobility of 12 cm²/Vs and room temperature photoluminescence at 3.1 eV corresponding to its direct energy band gap. We describe the fabrication and properties of γ-CuI/TiO₂/Cu₃N and γ-CuI/Cu₃N p-n heterojunctions that exhibited rectifying current-voltage characteristics, but no photogenerated current attributed to indirect recombination via shallow states in Cu₃N and/or deep states in the γ-CuI consistent with the short (ps) lifetimes of the photoexcited electrons-holes determined from transient absorption–transmission spectroscopy. Full article

Chemical and physical processes in molecules can be controlled through the manipulation of quantum interferences between rotational, vibrational, and electronic degrees of freedom. Most of the past efforts have been focused on the control of nuclear dynamics. Even though electronic coherence and its coupling to nuclear degrees of freedom may profoundly affect the outcome of these processes, electron dynamics have received less attention. Proper investigation of electron dynamics in materials demands ultrafast sources in the visible, ultraviolet (UV), and extreme ultraviolet (XUV) spectral region. For this purpose, a few-cycle deep-UV and XUV beamlines have been constructed for studying ultrafast electron dynamics in molecules. To ensure the required high temporal resolution on the attosecond time scale, vibration isolation from environmental mechanical noise and active stabilization have been implemented to achieve attosecond timing control between pump and probe pulses with excellent stability. This is achieved with an actively phase-stabilized double-layer Mach-Zehnder interferometer system capable of continuous time-delay scans over a range of 200 fs with a root-mean-square timing jitter of only 13 as over a few seconds and ~80 as of peak-to-peak drift over several hours. Full article

We developed a single-shot coherent X-ray imaging instrument at the hard X-ray beamline of the Pohang Accelerator Laboratory X-ray Free Electron Laser (PAL-XFEL). This experimental platform was established to conduct a variety of XFEL experiments, including coherent diffraction imaging (CDI), X-ray photon correlation spectroscopy (XPCS), and coherent X-ray scattering (CXS). Based on the forward-scattering geometry, this instrument utilizes a fixed-target method for sample delivery. It is well optimized for single-shot-based experiments in which one expects to observe the ultrafast phenomena of nanoparticles at picosecond temporal and nanometer spatial resolutions. In this paper, we introduce a single-shot coherent X-ray imaging instrument and report pump–probe coherent diffraction imaging (PPCDI) of Ag nanoparticles as an example of its applications. Full article