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The downscaling of nonlinear optical devices is significantly hindered by the inherently weak nonlinearity in regular materials. Here, we report a giant third-harmonic generation discovered in epitaxial thin films of V-VI chalcogenide topological insulators. Using a tailored substrate and capping layer, a single reflection from a 13 nm film can produce a nonlinear conversion efficiency of nearly 0.01%, a performance that rivals micron-scale waveguides made from conventional materials or metasurfaces with far more complex structures. Such strong nonlinear optical emission, absent from the topologically trivial member in the same compound family, is found to be generated by the same bulk band characteristics that are responsible for producing the band inversion and the nontrivial topological ordering. This finding reveals the possibility of obtaining superior optical nonlinearity by examining the large pool of newly discovered topological materials with similar band characteristics.

Delafossites are promising candidates for photocatalysis applications because of their chemical stability and absorption in the solar region of the electromagnetic spectrum. For example, CuAlO2 has...

The rate equation associated with recombination dynamics of photoexcited charge carriers in Cu2O nanostructures shows Auger scattering occurs readily in smaller particles and that particle shape affects the onset of higher-order recombination mechanisms.

Solar-driven production of renewable energy (e.g., H2) has been investigated for decades. To date, the applications are limited by low efficiency due to rapid charge recombination (both radiative and nonradiative modes) and slow reaction rates. Tremendous efforts have been focused on reducing the radiative recombination and enhancing the interfacial charge transfer by engineering the geometric and electronic structure of the photocatalysts. However, fine-tuning of nonradiative recombination processes and optimization of target reaction paths still lack effective control. Here we show that minimizing the nonradiative relaxation and the adsorption energy of photogenerated surface-adsorbed hydrogen atoms are essential to achieve a longer lifetime of the charge carriers and a faster reaction rate, respectively. Such control results in a 16-fold enhancement in photocatalytic H2 evolution and a 15-fold increase in photocurrent of the crystalline g-C3N4 compared to that of the amorphous g-C3N4.

Aspects of the optoelectronic performance of thin-film ferromagnetic materials are evaluated for application in ultrafast devices. Dynamics of photocarriers and their associated spin polarization are measured using transient reflectivity (TR) measurements in cross linear and circular polarization configurations for La0.7Sr0.3MnO3 films with a range of thicknesses. Three spin-related recombination mechanisms have been observed for thicker films (thickness of d ≥ 20 nm) at different time regimes (τ), which are attributed to the electron–phonon recombination (τ 1 ns). Density functional theory (DFT+U) based first-principles calculations provide information about the nature of the optical transitions and their probabilities for the majority and the minority spin channels. These transitions are partly responsible for the aforementioned recombination mechanisms, identified through the compari...

We analyze four-wave-mixing experiments with three incident laser pulses performed on a semiconductor quantum well embedded in a microcavity. The coupling of the intracavity field and the exciton transition leads to exciton polaritons. The many-body hierarchy problem that arises due to the Coulomb interaction is treated by the dynamics-controlled truncation scheme, which leads to a set of Bloch equations that contain optical nonlinearities including biexcitonic many-body correlations and contributions beyond the coherent limit, which have not been thoroughly explored for a microcavity yet. A numerical solution of these Bloch equations is performed by projecting onto the 1s-exciton and biexciton states. We present the two-dimensional Fourier transform of the four-wave-mixing signal for different polarization directions of the incident pulses, which allows us to investigate the absorption and emission of the system and the couplings among the different resonances from the lower polariton, the upper polariton, and the biexciton. The numerical results are compared with measurements, in which a GaAs quantum well sample enclosed in distributed Bragg reflectors is investigated for four different polarization configurations, and we find a good agreement.

Non-equilibrium carrier transport and dynamics were investigated using AC photoconductivity in type-II quantum wells. Low carrier mobilities are observed in the system when the hot-carriers at the metastability time span.

Transient absorption captures dynamics of nanocubes, showing negative delay-time signals associated with perturbed free induction. This validates dielectric-resonance energy transfer between electromagnetic modes for light-harvesting applications.

Population/mixing-time-dependent two-dimensional coherent spectra are presented for exciton-polaritons in a microcavity. Theory based on dynamically-controlled truncation reveals coherent and incoherent contributions to the decay dynamics.

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity., 4 pages, 3 figures, 1 table

La0.7Sr0.3MnO3 is a strongly correlated complex oxide. There is limited information about La0.7Sr0.3MnO3 thin films’ transient reflectivity (TR), where differences in ultra-fast dynamics due to surface and interface effects are expected. By decreasing the film thickness, additional energy states emerge, providing extra relaxation channels. Due to the reduced absorption in thin films, observing the effects of these extra states in TR signal is challenging, especially in a hole doped system such as La0.7Sr0.3MnO3. Moreover, in lower thicknesses, sinusoidal behavior superimposed on the TR signal is not analyzable by Fourier transforms. Wavelet transforms are perfect tools to analyze these fast-vanishing oscillations.

Multidimensional coherent spectroscopy measures the third-order polarization response of a system to reveal microscopic electronic and many-body phenomena. Applied to semiconductor nanostructures, it can distinguish homogeneous and inhomogeneous broadening due to disorder or strain gradients, resolve coupling between transitions, and optically access transitions that are either non-radiating or outside the bandwidth of the pulses. Two tools often exploited in this versatile technique are (i) the ability to control the polarization of the excitation and emission and thus the optical selection rules, and (ii) the ability to capture the complex spectrum. Here, the polarization of pulses emerging from a multidimensional optical nonlinear spectrometer (MONSTR) and the resulting four-wave mixing emission are controlled automatically using variable retarders, such that multiple spectra are recorded during a single phase-stabilized scan. This improves the acquisition time by ~3x compared to running separate polarization scans. Importantly, only one phase ambiguity exists in the complex spectra across all sets of polarization states measured. This single ambiguity is resolved by comparing the initial spectrally resolved transient absorption to the complex four-wave mixing spectrum for collinear polarization and then applying it to all spectra. Here, the method is applied to a quantum well embedded in a semiconductor microcavity with an adjustable cavity-exciton detuning. The complex 2DCS spectra we report constitute the first measurements of detuning- and polarization-dependent exciton-polariton lineshape across the strong coupling regime.

CdGeP2 represents a broad class of nonlinear and optoelectronic materials whose growth can be improved through characterization by terahertz time-domain spectroscopy. We determine THz refraction, absorption, electron-phonon coupling, carrier mobility and scattering mechanisms.

We investigate temperature-dependent recombination mechanisms, decay times and AC photoconductivity of CdSiP2 nonlinear crystal using Time resolved terahertz spectroscopy. Carrier density and mobility are extracted by fitting photoconductivity with Drude-Smith model.

Photoexcited carrier relaxation dynamics were investigated using AC photoconductivity in type-II quantum wells. Meta stability of excited carriers were observed to arise due to electron-phonon interactions.

Multidimensional coherent spectra are presented for exciton-polaritons in a semiconductor microcavity at cryogenic temperatures as a function of mixing time. A decrease in vacuum Rabi splitting is observed along with spectral phase shifts.

For powder samples of CuAl1- x Fe x O2(x = 0, 0.01, 0.05, and 0.1), measured optical properties are compared with model simulations and phonon spectra are compared with simulations based on weighted dynamical matrix approach.

We demonstrate temperature-dependent refraction, absorption, electron-phonon coupling, AC conductivity and mobility in bulk chalcopyrite semiconductors using THz-TDs. The measured optical and electronic properties are significantly influenced by temperature that affects the underlying carrier scattering mechanism.

We apply Linear Prediction from Singular Value Decomposition (LPSVD) to two-dimensional complex optical data in the time-domain to generate spectra with advantages over discrete Fourier transformation (DFT). LPSVD is a non-iterative procedure that fits time-domain complex data to the sum of damped sinusoids, or Lorentzian peaks in the spectral domain. Because the fitting is linear, it is not necessary to give initial guess parameters as in nonlinear fits. Although LPSVD is a one-dimensional algorithm, it can be performed column-wise on two-dimensional data. The method has been extensively used in 2D NMR spectroscopy, where spectral peaks are typically nearly ideal Lorentzians, but to our knowledge has not been applied in the analogous optical technique, where peaks can be far from Lorentzian. We apply LPSVD to the analysis of zero, one, and two quantum electronic two-dimensional spectra from a semiconductor microcavity. The spectra consist of non-ideal, often overlapping peaks. We find that LPSVD achieves a very good fit even on non-ideal data. It reduces noise and eliminates discrete distortions inherent in the DFT. We also use it to isolate and analyze weak features of interest.

Previous studies have shown that hydrogen treatment leads to the formation of blue to black TiO_2, which exhibits photocatalytic activity different from that of white pristine TiO_2. However, the underlying mechanism remains poorly understood. Herein, density functional theory is combined with comprehensive analytical approaches such as X-ray absorption near edge structure spectroscopy and transient absorption spectroscopy to gain fundamental understanding of the correlation among the oxygen vacancy, electronic band structure, charge separation, charge carrier lifetime, reactive oxygen species (ROS) generation, and photocatalytic activity. The present work reveals that hydrogen treatment results in chemical reduction of TiO_2, inducing surface and subsurface oxygen vacancies, which create shallow and deep sub-band gap Ti(III) states below the conduction band. This leads to a blue color but limited enhancement of visible light photocatalytic activity up to 440 nm at the cost of reduced ultraviolet photocatalytic activity. The extended light absorption spectral range for reduced TiO_2 is ascribed to both the defect-to-conduction band transitions and the valence band-to-defect transitions. The photogenerated charge carriers from the defect states to the conduction band have lifetimes too short to drive photocatalysis. The Ti(III) deep and shallow trap states below the conduction band are also found to reduce the lifetime of photogenerated charge carriers under ultraviolet light irradiation. The ROS generated by the reduced TiO_2 are less than those generated by pristine TiO_2. Consequently, the reduced TiO_2 exhibits ultraviolet-responsive photocatalytic activity worse than that of pristine TiO_2. This report shows that increasing the light absorption spectral range of a semiconductor by doping or introduction of defects does not necessarily guarantee an increase in photocatalytic activity.

Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP

Aspects of the optoelectronic performance of thin-film ferromagnetic materials are evaluated for application in ultrafast devices. Dynamics of photocarriers and their associated spin polarization are measured using transient reflectivity (TR) measurements in cross linear and circular polarization configurations for La

Transient reflectivity (TR) measurements for La0.7Sr0.3MnO3 thin films indicate enhanced surface recombination of charge carriers for thinner films (d < 20 nm). Wavelet analysis of residual TR shows abrupt oscillatory modes with close energy ranges.

Automated, polarization-controlled 2D coherent spectroscopy is shown based on liquid-crystal variable retarders. Polarization-dependent rephasing spectra are recorded in a single scan, with absolute phase determined by a single auxiliary measurement.

Terahertz time-domain spectroscopy is employed to investigate temperature-dependent properties of bulk chalcopyrite crystals (CdGeP$_2$, ZnGeP$_2$ and CdSiP$_2$). The complex spectra provide the refraction and absorption as a function of temperature, from which electron-phonon coupling and average phonon energies are extracted and linked to the mechanics of the A- and B-site cations. Also, AC conductivity spectra provide carrier densities and electron scattering times, the temperature dependence of which is associated with unintentional shallow dopants. Temperature dependence of the scattering time is converted into carrier mobility and modeled with microscopic transport mechanisms such as polar optical phonon, acoustic phonons, deformation potential, ionized impurity and dislocation scattering. Hence, analysis links the THz optical and electronic properties to relate microscopic carrier transport and carrier-lattice interactions., Comment: 12 pages, 5 figures, journal submission preprint

Hot electrons established by the absorption of high-energy photons typically thermalize on a picosecond time scale in a semiconductor, dissipating energy via various phonon-mediated relaxation pathways. Here it is shown that a strong hot carrier distribution can be produced using a type-II quantum well structure. In such systems it is shown that the dominant hot carrier thermalization process is limited by the radiative recombination lifetime of electrons with reduced wavefunction overlap with holes. It is proposed that the subsequent reabsorption of acoustic and optical phonons is facilitated by a mismatch in phonon dispersions at the InAs-AlAsSb interface and serves to further stabilize hot electrons in this system. This lengthens the time scale for thermalization to nanoseconds and results in a hot electron distribution with a temperature of 490 K for a quantum well structure under steady-state illumination at room temperature.

Time-resolved Kerr-rotation microscopy explores the influence of optical doping on the persistent spin helix in a [001]-grown CdTe quantum well at cryogenic temperatures. Electron spin diffusion dynamics reveal a momentum-dependent effective magnetic field providing SU(2) spin-rotation symmetry, consistent with kinetic theory. The Dresselhaus and Rashba spin-orbit coupling parameters are extracted independently from rotating the spin helix with external magnetic fields applied parallel and perpendicular to the effective magnetic field. Most importantly, a non-uniform spatiotemporal precession pattern is observed. The kinetic theory framework of spin diffusion allows for modeling of this finding by incorporating the photocarrier density into the Rashba ($\alpha$) and the Dresselhaus ($\beta_3$) parameters. Corresponding calculations are further validated by an excitation-density dependent measurement. This work shows universality of the persistent spin helix by its observation in a II-VI compound and the ability to fine-tune it by optical doping., Comment: 5 pages, 4 figures, journal submission

In Forster resonance energy transfer (FRET), energy non-radiatively transfers from a blue-shifted emitter to a red-shifted absorber by dipole–dipole coupling. This study shows that plasmonics enables the opposite transfer direction, transferring the plasmonic energy towards the short-wavelength direction to induce charge separation in a semiconductor. Plasmon-induced resonance energy transfer (PIRET) differs from FRET because of the lack of a Stoke's shift, non-local absorption effects and a strong dependence on the plasmon's dephasing rate and dipole moment. PIRET non-radiatively transfers energy through an insulating spacer layer, which prevents interfacial charge recombination losses and dephasing of the plasmon from hot-electron transfer. The distance dependence of dipole–dipole coupling is mapped out for a range of detuning across the plasmon resonance. PIRET can efficiently harvest visible and near-infrared sunlight with energy below the semiconductor band edge to help overcome the constraints of band-edge energetics for single semiconductors in photoelectrochemical cells, photocatalysts and photovoltaics. Plasmon-induced resonance energy transfer is revealed and explored for solar energy harvesting from visible and near-infrared light.

Plasmonic metals can excite charge carriers in semiconductors through plasmon-induced resonance energy transfer (PIRET) and hot electron injection processes. Transient absorption spectroscopy reveals that the presence of plasmon-induced charge separation mechanisms in metal@TiO2 core–shell nanoparticles can be controlled by tailoring the spectral overlap and the physical contact between the metal and the semiconductor. In Ag@SiO2@TiO2 sandwich nanoparticles, the localized surface plasmon resonance band is overlapped with the absorption band edge of TiO2, enabling PIRET, while the SiO2 barrier prevents hot electron transfer. In Au@TiO2, hot electron injection occurs, but the lack of spectral overlap disables PIRET. In Ag@TiO2, both hot electron transfer and PIRET take place. In Au@SiO2@TiO2, photoconversion in TiO2 is not enhanced by the plasmon despite strong light absorption by Au.

Transient absorption spectroscopy is a powerful technique for understanding charge carrier dynamics and recombination pathways. Analyzing the results is not trivial due to nonexponential relaxation dynamics away from equilibrium, leading to a disparity in reported charge-transfer rates. An inversion analysis technique is presented that transforms transient signals back into their original rate equation. The technique is demonstrated on two CdSe/TiO2 heterostructures with different surface states. Auger recombination is identified at higher carrier densities and radiative recombination at lower carrier densities. The heterostructure with additional surface traps exhibits increased trap-state Auger recombination at high carrier densities and changes to radiative recombination at low carrier densities due to a Shockley–Read–Hall process. Carrier-dependent electron-transfer rates are determined and compared to common methods that only capture the magnitude of the charge transfer at specific carrier densities....

Doping a semiconductor can extend the light absorption range, however, it usually introduces mid-gap states, reducing the charge carrier lifetime. This report shows that doping lanthanum dititinate (La2Ti2O7) with nitrogen extends the valence band edge by creating a continuum of dopant states, increasing the light absorption edge from 380 nm to 550 nm without adding mid-gap states. The dopant states are experimentally resolved in the excited state by correlating transient absorption spectroscopy with a supercontinuum probe and DFT prediction. The lack of mid-gap states is further confirmed by measuring the excited state lifetimes, which reveal the shifted band edge only increased carrier thermalization rates to the band edge and not interband charge recombination under both ultraviolet and visible excitation. Terahertz (time-domain) spectroscopy also reveals that the conduction mechanism remains unchanged after doping, suggesting the states are delocalized.

Antiferromagnets are an important class of ordered spin systems, common in spintronic applications and providing a testbed for studying magnetism. Recently, the injection of magnons – coherent spin waves – has been explored by broadband terahertz pulses in antoferromagnets, such as MnO. Here, terahertz time-domain spectroscopy is used to detect magnon resonances in MnF2, which is a model antiferromagnet with uniaxial anisotropy and a Neel temperature of 67 K. Temperature dependence of a one-magnon resonances is examined from 5 K to 70 K. The center frequency of the one-magnon is recorded below the Neel temperature and fit to a Brillouin function. It is found that the degree of correlation between neighboring spins is j = 1.1. Namely, a weak correlation and appropriately modeled by mean-field theory befitting this simple system. From low temperature to room temperature, a two-magnon resonance is observed to broaden and strengthen as the temperature increases. Two-magnon modes arise due to zone-edge magnons being stimulated with -k and +k momenta and do not require magnetic ordering. Over this same temperature range, THz transients are used to monitor the time-of flight through the crystal, the refractive index, the internal energy and the heat capacity. Overall these quantities decrease with decreasing temperature, with behavior that falls into three regimes: a thermal dominated region above the Neel temperature, a magnetic regime below the Neel temperature; and a hyperfine interaction region at temperatures below 6 K. The latter is the first direct observation of the hyperfine interaction using terahertz time-domain spectroscopy.

Electron spin transport and dynamics are investigated in a single, high-mobility, modulation-doped, GaAs quantum well using ultrafast two-color Kerr-rotation micro-spectroscopy, supported by qualitative kinetic theory simulations of spin diffusion and transport. Evolution of the spins is governed by the Dresselhaus bulk and Rashba structural inversion asymmetries, which manifest as an effective magnetic field that can be extracted directly from the experimental coherent spin precession. A spin precession length L-SOI is defined as one complete precession in the effective magnetic field. It is observed that application of (a) an out-of-plane electric field changes the spin decay time and L-SOI through the Rashba component of the spin-orbit coupling, (b) an in-plane magnetic field allows for extraction of the Dresselhaus and Rashba parameters, and (c) an in-plane electric field markedly modifies both the L-SOI and diffusion coefficient. While simulations reproduce the main features of the experiments, the latter results exceed the corresponding simulations and extend previous studies of drift-current-dependent spin-orbit interactions., Comment: 11 pages, 7 figures

This paper presents a sandwich-structured CdS-Au-TiO2 nanorod array as the photoanode in a photoelectrochemical cell (PEC) for hydrogen generation via splitting water. The gold nanoparticles sandwiched between the TiO2 nanorod and the CdS quantum dot (QD) layer play a dual role in enhancing the solar-to-chemical energy conversion efficiency. First, the Au nanoparticles serve as an electron relay, which facilitates the charge transfer between CdS and TiO2 when the CdS QDs are photoexcited by wavelengths shorter than 525 nm. Second, the Au nanoparticles act as a plasmonic photosensitizer, which enables the solar-to-hydrogen conversion at wavelengths longer than the band edge of CdS, extending the photoconversion wavelength from 525 to 725 nm. The dual role of Au leads to a photocurrent of 4.07 mA/cm(2) at 0 V (vs Ag|AgCl) under full solar spectrum irradiation and a maximum solar-to-chemical energy conversion efficiency of 2.8%. An inversion analysis is applied to the transient absorption spectroscopy data, tracking the transfer of electrons and holes in the heterostructure, relating the relaxation dynamics to the underlying coupled rate equation and revealing that trap-state Auger recombination is a dominant factor in interfacial charge transfer. It is found that addition of Au nanoparticles increases the charge-transfer lifetime, reduces the trap-state Auger rate, suppresses the long-time scale back transfer, and partially compensates the negative effects of the surface trap states. Finally, the plasmonic energy-transfer mechanism is identified as direct transfer of the plasmonic hot carriers, and the interfacial Schottky barrier height is shown to modulate the plasmonic hot electron transfer and back transfer. Transient absorption characterization of the charge transfer shows defect states cannot be ignored when designing QD-sensitized solar cells. This facile sandwich structure combines both the electrical and the optical functions of Au nanoparticles into a single structure, which has implications for the design of efficient solar-energy-harvesting devices.

Optical injection and detection of charge currents is an alternative to conventional transport and photoemission measurements, avoiding the necessity of invasive contact that may disturb the system being examined. This is a particular concern for analyzing the surface states of topological insulators. In this work one- and two-color sources of photocurrents are isolated and examined in epitaxial thin films of Bisub2/subSesub3/sub. We demonstrate that optical excitation and terahertz detection simultaneously captures one- and two-color photocurrent contributions, which has not been required for other material systems. A method is devised to extract the two components, and in doing so each can be related to surface or bulk excitations through symmetry. The separation of such photocurrents in topological insulators opens a new avenue for studying these materials by all-optical methods.

An experimental apparatus is described for multidimensional optical spectroscopy with fully automated polarization control, based on liquid crystal variable retarders. Polarization dependence of rephasing two-dimensional coherent spectra are measured in a single scan, with absolute phasing performed for all polarization configurations through a single automated auxiliary measurement at the beginning of the scan. A factor of three improvement in acquisition time is demonstrated, compared to the apparatus without automated polarization control. Results are presented for a GaAs quantum well sample and an InGaAs quantum well embedded in a microcavity.

Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP2, ZnGeP2 and CdSiP2. The emission is characterized using linear-polarized excitation from 0.8 eV to 1.55 eV (1550 nm – 800 nm). All three crystals are (110)-cut and polished to 0.5 mm, thinner than the coherence length across most of the excitation photon energy range, such that they all produce a bandwidth ~2.5 THz when excited with ~100 fs pulses. It is found that CdGeP2 produced the strongest emission at telecoms wavelengths, while CdSiP2 is generally the strongest source. Pump-intensity dependence provides the nonlinear coefficients for each crystal.

Applications of wavelet analysis in ultra-thin film transient reflectivity (TR) measurements have been investigated. Advantages of utilizing different localized wavelet bases, in position and time, have been addressed on the residual TR signals. Morse wavelets have been used to obtain information from the abrupt oscillatory modes in the signal, which are not distinguishable with conventional methods such as Fourier transforms. These abrupt oscillatory modes are caused by the surface, interface, or any short-lived oscillatory modes which are suppressed in the TR signal in ultra-thin films. It is demonstrated that by choosing different Morse wavelets, information regarding different oscillatory modes in the TR signal of a heterostructure thin film is achievable. Moreover, by performing wavelet analysis on multiferroic heterostructures, oscillatory modes with very close energy ranges are easily distinguishable. For illustration, residuals of the TR signals have been obtained by a pump-probe setup in reflectivity mode on La0.7Sr0.3MnO3/SrTiO3 and BaTiO3/La0.7Sr0.3MnO3/SrTiO3 samples, where sufficient signal to noise ratios have been achieved by taking multiple scans. The residual signals have been analyzed with Morse wavelets, and multiple oscillatory modes with close energy ranges have been observed and distinguished. This approach can isolate the location of various oscillatory modes at the surface, interface and in the bulk of the heterostructure sample.

The photocatalytic water oxidation activity of hematite (α-Fe2O3) has been greatly enhanced by incorporating hematite nanoparticles on the reduced graphene oxide (rGO) nanosheets. Photoelectrochemical measurement results show that coupling the hematite nanoparticles with the rGO greatly increases the photocurrent and reduces the charge recombination rate. Transient absorption spectroscopy and time-domain terahertz spectroscopy have provided the direct evidence that the photogenerated electrons have transferred as the mobile carriers from α-Fe2O3 to rGO, which enhances the charge separation and suppresses the charge recombination. This work has provided new insight into the mechanism of photocatalysis enhancement by reduced graphene oxide, which has implications in the design of semiconductor/graphene heterojunction photocatalysts.